(Ted M. Knowlton, Chair) Proceedings of International

PROGRAM
International Conference on Circulating Fluidized Beds and

Fluidization Technology - CFB-10
May 1 - 5, 2011
Sunriver Resort
Sunriver, Oregon, USA
Conference Chair
Ted M. Knowlton
Particulate Solid Research, Inc, USA
Sunday, May 1, 2011
One-Day Seminar on Fluidization
8:00 - 8:30 am Registration

8:30 - 10:15 am Hydrodynamics (J. Grace)
10:15 - 10:30 am Coffee Break
10:30 - 11:15 am Scaling and Scale-Up (T. Knowlton)
11:15 - 12:00 am Cyclone Design and Operation (T. Knowlton)
12:00 - 1:00 pm LUNCH
1:00 - 1:45 pm Standpipes/Non-Mechanical Valves (T. Knowlton)
1:45 - 2:30 pm Heat Transfer (J. Grace)
2:30 - 2:45 pm Coffee Break
2:45 - 4:15 pm Reactors and Combustors (J. Werther)
4:15 - 4:45 pm Question-and-Answer Period with Instructors
4:45 pm Adjourn
Conference Registration
2:00 - 6:00 pm
Activity Program Meeting
5:30 - 6:30 pm
Reception/Dinner
6:30 - 9:30 pm
Special Poster Session/Social Hour

9:30 pm - 11:00 pm
Monday, May 2, 2011
7 - 8:15 am BREAKFAST
8:15 - 8:30 am CONFERENCE OPENING
PLENARY SESSION
Chairman: R. Cocco
8:30 - 9:30 am P-1: Reflections on Mathematical Models and Simulation of Gas-Particle Flows
Sankaran Sundaresan, Princeton University
9:30 - 9:40 am COFFEE BREAK
SESSION 1 SESSION 2
Solids Flow and Circulation Novel Fluidized Bed Processes
Co-Chairs: Co-Chairs:
J. Zhu P. Basu
U. Muschelknautz Y. Cheng
1-1: Gas Tracer Study in a Non- 2-1: Process Decoupling of Plasma

9:40 - 9:54 am Mechanical L-Valve Enhanced Synthesis of Chlorinated
Polyvinyl Chloride (CPVC) Particles in
M.M.Yazdanpanah, A. Hoteit, A. Forret a Circulating Fluidized Bed
Thierry Gauthier
IFP Energies Nouvelles W. Lu, T. Cao, Y. Cheng
Arnaud Delabarre Tsinghua University, China
Université Henri Poincaré, France
1-2: Investigation on the Hydrodynamic 2-2 Manufacture of Granular

9:54 - 10:08 am Properties in the External Loop of a Polysilicon from Trichlorosilane in an
Circulating Fluidized Bed with a Loop Internally Circulating Fluidized Bed
Seal Reactor
X. Yao, T. Wang, H. Yang, H. Zhang, Q. Liu C. Wang, T. Wang, Z. Wang
J. Lv Tsinghua University, China
Tsinghua University, China
1-3: Hydrodynamics of a Dual Fluidized 2-3 High-Flux Triple Bed Circulating

10:08 - 10:22 am Bed System Which has Internal Mixing Fluidized Bed (TBCFB) Gasifier for
Channels Between CFB and BFB Exergy Recuperative IGCC/IGFC
Reactor
C. Fushimi, G. Guan, M. Ishizuka
U. Lee, I. Choi, W. Yang, Y. Kim, Y. Nakamura, A. Tsutsumi
Y. Choi The University of Tokyo, Japan
Korea Institute of Industrial Technology Y. Suzuki, National Institute of Industrial
J. Song - SeenTec Co., Ltd. Science, Japan
Korea E.W.C. Lim, Y. Cheng, C-H. Wang
National University of Singapore, Singapore
Monday, May 2, 2011 (continued)
1-4: Particle Flow in L-Valves 2-4: Bio-Gasoline from Jatropha Oil:

10:22 - 10:36 am New Applications for the FCC- Process
D. Subbarao
University Teknologi PETRONAS, Malaysia A. Weinert, A. Reichold, P. Bielansky
C. Schonberger, B. Schumi
Vienna University of Technology
Austria
1-5: A Generalized Flow Diagram for 2-5 Waste Wood Gasification:

11:00 - 11:14 am Fluid-Solid Vertical Transport Distribution of Nitrogen, Sulphur and
Chlorine in a Dual Fluidised Bed Steam
X. Bi Gasifier
University of British Columbia, Canada
V. Wilk, C. Aichernig, H. Hofbauer
Vienna University of Technology, Austria
1-6: Cold Model Investigations of a 2-6: Removal of Nitrate from Water
11:14 - 11:28 am High Temperature Looping Process in a Using Fluidized Bed Ion Exchange
Dual Circulating Fluidized Bed System Column
A.R. Bidwe, C. Hawthorne, A. Charitos, M.A.M. Ammar Arab Beddai, V.V. Basava Rao
Dominguez, H. Dieter, A. Schuster, G. Osmania University
Scheffknecht India
University of Stuttgart, Germany
1-7: Hydrodynamics of a Loop Seal 2-7: A Pyrolysis Pilot Unit Integrated to

11:28 - 11:42 am Operated in a Circulating Fluidized a Circulating Fluidized Bed Boiler -
Bed: Influence of the Operating Experiences from a Pilot Project
Parameters on Gas and Solid Flow
Patterns J. Autio, J. Lehto, Metso Power Oy
P. Jokela, UPM
R. Solimene, R. Chirone J. Alin, Fortum
Istituto di Recerche sulla Combustione - CNR A. Oasmaa, Y. Solantausta, VTT
P. Bareschino Finland
Universita degli Studi del Sannio
P. Salatino
Universita degli Studi di Napoli Federico II
Italy
1-8: Effects of Particle Properties on 2-8: Production of Gasoline and
11:42 - 11:56 am Cluster Characteristics in a 2-D CFB Gaseous Olefins by Catalytic Cracking
Riser of Pyrolysis Oil
J. Xu and J. Zhu P. Bielansky, A. Reichhold, A. Weinert
University of Western Ontario, Canada Vienna University of Technology
Austria
1-9: Flow Field in a Novel Short 2-9: Energetic Optimization of the
11:56 - 12:10 pm Residence Time Gas-Solid Separator Lignin Pyrolysis for the Production of
Aromatic Hydrocarbons
M. Liu, C. Zhou, C. Lu, Z. Wang
China University of Petroleum M. Franck, B. Lorenz, E-U. Hartge,
China S. Heinrich, J. Werther
Hamburg University of Technology, Germany
1-10: Cold Model Study on 2-10: Studies on Propane

12:10 - 12:24 pm Interconnected Fluidized Bed Reactors Dehydrogenation to Propylene in a
for Multi-Generation Systems and Gas-Solid-Sold Fluidized Bed Reactor
Chemical Looping Processes
Y. Chu, T. Wu, Y. Li, Z. Nawaz, T. Wang
G.A. Ryabov, O.M. Folomeyev, D.A. Sankin, F. Wei
K.V.Khaneyev, All-Russian Thermal Tsinghua University, China
Engineering Institute, Russia
12:30 - 2:00 pm LUNCH
2:00 - 5:30 pm FREE TIME
SESSION 3 SESSION 4
Mathematical Modeling I Chemical Looping
N. Mostoufi E.-U. Hartge
F. Johnsson R. Gupta
3-1: A Modeling Study of Gas 4-1: The Development of a Novel

5:30 - 5:44 pm Streaming in a Deep Fluidized Bed of Cu-Mn Oxygen Carrier for the Chemical
Geldart A Particles Looping Gasification of Biomass
S. Karimipour, T. Pugsley M. Aghabararnejad, J. Chaouki, G.S. Patience
University of Saskatchewan Ecole Polytechnique de Montreal
Canada Canada
3-2: Effects of Gas Velocity and Solid 4-2:CO2 Looping Cycle for CO2
5:44 - 5:58 pm Hold-Up on the Sub-Grid Behavior of Separation
Riser Flows
T. Shimizu, H. T. Takahashi, Narisawa, L. Li, H.
C.C. Milioli, F. E. Milioli Kim
University of São Paulo, Brazil Niigata University
Japan
3-3: Numerical Simulations of a 4-3: Fluid Dynamic Effects of Ring-Type

5:58 - 6:12 pm Circulating Fluidized Bed with a Square Internals in a Dual Circulating Fluidized
Cross-Section Bed System
T. Li, S. Pannala, C. Guenther D.C. Guio Perez, K. Marx, T. Proell
National Energy Technology Laboratory H. Hofbauer
S. Pannala Vienna University of Technology
Oak Ridge Institute for Science and Education, Austria
USA
3-4: High-Resolution Simulations of 4-4: Design Requirements for

6:12 - 6:26 pm Gas-Solids Jet Penetration Into a High- Pressurized Chemical Looping
Density Riser Flow Reforming
T. Li, C. Guenther K. Marx, T. Proell, H. Hofbauer
National Energy Technology Laboratory, USA Vienna Institute of Technology
Austria
3-5: Simulation of Particle-Gas Flow in 4-5: The Influence of Carbon Stripper

6:26 - 6:40 pm a Cyclone Using URANS Efficiency on CO2 Capture Rate in a
Chemical-Looping Combustion
A. Karvinen, H. Ahlstedt, Tampere University of Process for Solid Fuels
Technology
M. Palonen, Metso Power Oy M. Kramp, A. Thon, E-U. Hartge, S. Heinrich
Finland J. Werther
Hamburg University of Technology
Germany
3-6: Evaluation of a Lagrangian 4-6: Study of Calcination-Carbonation

6:40 - 6:54 pm Discrete Phase Modeling Approach for of Calcium Carbonate in Different
Application to Industrial Scale Bubbling Fluidizing Mediums for Chemical
Fluidized Beds Looping Gasification in Circulating
Fluidized Beds
S. Cloete, S.T. Johansen, M. Braun, S. Amini,
SINTEF Materials and Chemistry, Norway B. Acharya, A. Dutta, P. Basu
M. Braun, B. Popoff Dalhousie University
Ansys, Germany Canada
3-7: Effect of Wall Boundary Conditions 4-7: Understanding Standpipe

6:54 - 7:08 pm and Mesh Refinement on Numerical Hydrodynamics Using Electrical
Simulation of Pressurized Dense Capacitance Tomography
Fluidized Bed for Polymerization
C. Qui, R. Joachim
Reactor Industrial Tomography Systems, USA
P. Fede, O. Simonin, R. Ansart, H. Neau S.B.R. Karri
Universite de Toulouse, France Particulate Solid Research, Inc., USA
I. Ghouila
INEOS, France
3-8 Fluidized Bed Membrane Reactor 4-8: A Practical Model for a Dense-Bed
7:08 - 7:22 pm for Steam Reforming of Higher Countercurrent FCC Regenerator
Hydrocarbons: Model Sensitivity
Y. Zhang, C. Lu
M.A. Rakib, J.R. Grace, C.J, Lim China University of Petroleum
University of British Columbia, China
Canada
7:30 - 9:15 pm DINNER
POSTER SESSION and SOCIAL HOUR

9:15 - 11:00 pm for Papers Presented in Sessions 1, 2, 3 and 4
Tuesday, May 3, 2011
7 - 8:30 am Breakfast
PLENARY SESSION 2
Chairman: J. Werther
8:30 - 9:30 am P-2: Electrostatic Phenomena in Fluidized Systems: Present Status of

Understanding, and Research Needs
Xiaotao Bi, University of British Columbia
SESSION 5 SESSION 6
Dynamics of Gas-Solids Flow Combustion and Gasification
J. Grace W. Nowak
B. Formisani A. Luckos
5-1: Design Criteria of Uniflow 6-1: Experimental Study on the Effects

9:40 - 9:54 am Cyclones for the Separation of Solid of Gas Permeation Through Flat
Particles from Gases Membranes on the Hydrodynamics in
Fluidized Beds
U. Muschelknautz, P. Pattis, M. Reinalter,
M. Kraxner J.F. de Jong, M. van Sint Annaland,
MCI Management Center Innsbruck J.A.M. Kuipers, Eindhoven University of
Austria Technology, The Netherlands
5-2: Erosion in Second Stage Cyclones: 6-2: Experimental Study on Reforming

9:54 - 10:08 am Effects of Cyclone Length and Outlet Activity and Oxygen Transfer of Fe-
Gas Velocity Olivine in a Dual Circulating Fluidized
Bed System
S.B. Reddy Karri, R. Cocco and T.M. Knowlton
Particulate Solid Research, Inc., USA S. Koppatz, T. Proell, C. Pfeifer, H. Hofbauer
Vienna University of Technology, Austria
5-3: Correlation of the Minimum 6-3: Study of Recarbonation in

10:08 - 10:22 am Spouting Velocity for the Design of Circulating Fluidized Bed Combustion
Open-Sided Draft Tube Conical
Spouted Beds for the Treatment of Fine I. Hyytiainen, H. Lemmetyinen, Tampere
Materials University of Technology
A. Mahlamaki, M. Palonen, M. Varonen, Metso
M. Olazar, H. Altzibar, G. Lopez, I. Estiati, Power Oy
J. Bilbao, University of the Basque Country Finland
Spain
5-4: Hydrodynamics of Conical Spouted 6-4: Coal Ignition Temperature in
10:22 - 10:36 am Beds with High Density Particles Oxygen-Enriched CFB Boiler
S. Sari, D. Zaglanmis, M. Koksal, Hacettepe J. Chao, H. Yang, J. Lu, H. Zhang, Q. Liu
University Y. Wu
A. Polat, Middle East Technical University, Tsinghua University
Turkey China
Tuesday, May 3, 2011 (continued)
5-5: Experiments and Modeling of 6-5: Co-Combustion of Various

11:00 - 11:14 am Micro-Jet Assisted Fluidization of Biowastes with a High-Sulfur Turkish
Nanopowder Lignite in a Circulating Fluidized Bed
Combustor with Air Staging
J.R. van Ommen, N. Loojie, Delft University of
Technology, The Netherlands A. Atimtay, M. Vario, Middle East Technical
D.M. King, A. Weimer, S. Johnson, University University, Turkey
of Colorado, USA H. Olgun, U. Kayahan, B. Bay, A. Unlu,
R. Pfeffer, University of Arizona, USA TUBITAK-MRC Energy Institute, Turkey
B.G.M. van Wachem, Imperial College London, M. C. Celebi, H. Atakul, Istanbul Technical
U.K. University, Turkey
G. Bardakcioglu, M. Ozcan, GAMA Power
Systems Engineering and Contracting, Turkey
5-6: Effect of Gas Bypassing in Deep 6-6: Oxy-Combustion of Different Coals

11:14 - 11:28 am Beds on Cyclone Dipleg Operation in a Circulating Fluidized Bed
A.S. Issangya, S.B. Reddy Karri, T.M. M. Kosowska-Golachowska, K. Klos, T. Musial,
Knowlton, R. Cocco Czestochowa University of Technology, Poland
Particulate Solid Research, Inc., USA A. Luckos, Sasol Technology, South Africa
5-7: Fluidization Behavior in a Gas- 6-7: Effects of Secondary Air Injection

11:28 - 11:42 am Solid Fluidized Bed with Thermally Upon the Fluidization Characteristics
Induced Inter-Particle Forces of the Lower Stage in a Two-Stage,
Variable-Area Fluidized Bed Riser
J. Shabanian, F. Fotovat, J. Bouffard, J.
Chaouki, Ecole Polytechnique de Montreal, E.K. Johnson, S.L. Rowan, West Virginia
Canada University, USA
5-8: Particle to Gas Heat Transfer in a 6-8: Gas-Solids Hydrodynamics in a

11:42 - 11:56 am Circulating Fluidized Bed Riser CFB with 6 Cyclones and a Pant Leg
Y.T. Makkawi, Aston University, U.K. L. Cheng, X. Zhou, C. Wang, Z. Wang, Z. Luo,
K. Cen, L, Nie, C. Wu, Q, Zhou
Zhejiang University, China
5-9: Fast Pyrolysis Process 6-9: The Research of CFB Boiler

11:56 - 12:10 pm Intensification: Study of the Gas Phase Operation for Oxygen Enhanced Dried
Residence Time Distribution and Lignite Combustion
Backmixing in a Downer Reactor
W. Muskala, J. Krzywanski, T. Czakiert,
M. Huard, F. Berruti, C. Briens, The University W. Nowak, Czestochowa University of
of Western Ontario, Canada Technology, Poland
12:30 - 2:00 pm LUNCH
2:00 - 3:40 pm WORKSHOP A

Panel Discussion on Energy
Chairman: D. Keairns
WORKSHOP B WORKSHOP C WORKSHOP D

3:45 - 5:20 pm Chemical Looping Instrumentation for Fluid PSRI/NETL Challenge
Chairman: L. S. Fan Particle Systems Problem
Chairman. J. R. van Ommen Co-Chairs:
L. Shadle
R. Cocco
SESSION 7 SESSION 8
Mathematical Modeling II Industrial Operation of Fluidized Beds
J. Li P. Gauville
H. Arastoopour J. de Jong
7-1: DEM-CFD Modeling of a Bubbling 8-1: Commissioning of a 0.8 MWth
5:30 - 5:44 pm Fluidized Bed and a Wurster Coater CFBC for Oxy-Fuel Combustion
L. Fries, S. Antonyuk, S. Heinrich, S. Palzer L, Jia, Y. Tan, D. McCalden, Y. Wu, I He
Hamburg University of Technology R. Symonds, E.J. Anthony
Germany Canmet ENERGY
Canada
7-2: Elutriation from Fluidized Beds: 8-2: High Sulfur Lignite Fired Large
5:44 - 5:58 pm Comparison Between Experimental CFB Boilers-Design and Operating
Measurements and 3D Simulation Experience
Results
M. Lakshminarasimhan, B Ravikumar, A.
R. Ansart, H. Neau, O. Simonin, IMFT Lawrence, M. Muthukrishnan,
P. Accart, A. de Ryck, CNRS Bharat Heavy Electrical Limited, India
Universite de Toulouse, France
7-3: Fluidized Bed Gasification of Mixed 8-3: Research on Heat Transfer Inside
5:58 - 6:12 pm Plastic Wastes: A Material and a the Furnace of Large Scale CFB Boilers
Substance Flow Analysis
R. Zhang, H. Yang, H. Zhang, Q. Liu, J. Lu
M.L. Mastellone, U. Arena Y. Wu, Tsinghua University, China
Second University of Naples, Italy
7-4: Circulating Fluidized Bed 8-4: Design and Operation of Biomass

6:12 - 6:26 pm Combustion-Build-Up and Validation of Circulating Fluidized Bed Boiler with
a Three-Dimensional Model High Steam Parameter
M. Palonen, V. Yla-Outinen, Metso Power Oy, S. Li, S. Bao, Q. Lu, D. Wang, H. Teng
J. Laine, Tampere University of Technology Chinese Academy of Sciences
Finland Y. Peng, Z. Liu, B. Hong
D. Pallares, A. Larsson, F. Johnsson Changsha Boiler Plant Co., Ltd.
Chalmers University of Technology China
Sweden
7-5: 3D CFD Simulation of Combustion 8-5: Operating Experience and Latest

6:26 - 6:40 pm in a 150 MWe Circulating Fluidized Bed Developments of Alstom Power's 300
Boiler MWe Class CFB Boilers
N. Zhang, B. Lu, W. Wang, J. Li, Chinese B. Wilhelm, P. Gauville, I. Abdulally, C. Enault
Academy of Sciences, China Alstom Power, France
7-6: Comparison Between 8-6: UOP FCC Innovations Developed

6:40 - 6:56 pm Measurements and Numerical Using Sophisticated Engineering Tools
Simulation of Particle Flow and
Combustion at the Duisburg CFBC L. Wolschlag, K. Couch
Plant UOP LLC
USA
M. Weng, Aixprocess,
J. Plackmeyer, Consulting Engineer
Germany
7-7: Hydrodynamics of a Cluster 8-7: Co-Gasification of Biomass and

6:56 - 7:10 pm Descending at the Wall of a CFB Riser - Coal in an 8MW Dual Fluidized Bed
Numerical Study Steam Gasifier
S. Vashisth, J. Grace C. Pfeifer, I. Aigner, H. Hofbauer
University of British Columbia Vienna University of Technology
Canada Austria
7-8: Characteristics of the Solid Volume 8-8: Coal and Biomass Co-Gasification
7:10 - 7:24 pm Fraction Fluctuations in a CFB in a Circulating Fluidized Bed Reactor
S. Kallio, J. Peltola, V. Taivassalo A. Czaplicki, M. Sciazko
VTT Technical Research Centre of Finland Institute for Chemical Processing of Coal
Finland Poland
7:30 - 9:15 pm DINNER
9:15 - 11:00 pm POSTER SESSION and SOCIAL HOUR

for Papers Presented in Sessions 5, 6, 7 and 8
Wednesday, May 4, 2011
PLENARY SESSION 3
Chairman: L. S. Fan
8:30 - 9:30 am P-3: Evolution of FCC Technology-Past, Present and Future and the
Challenges of Operating a High-Temperature CFB System
Ye Mon Chen, Shell Global Services
PLENARY SESSION 4
Chairman: L. S. Fan
9:30 - 10:30 am P-4: Putting Structure Into Fluidized Beds - From Concept to
Industrial Applications
Fei Wei, Tsinghua University
SESSION 9 SESSION 10
Particle Dynamics HT/HP Research
C. Pfeifer K. Wirth
R. Karri S. Moffatt
9-1: Sulfur Uptake by Limestone-Based 10-1: The Variation of the Bubble Phase
11:00 - 11:14 am Sorbent Particles in CFBC: The Properties of a FCC Fluidized Bed at
Influence of Attrition/Fragmentation on High Temperature
Sorbent Inventory and Particle Size
Distribution R. Girimonte, B. Formisani
University of Calabria, Italy
F. Montagnaro, P. Salatino, F. Scala,
M. Urciuolo
Universita degli Studi di Napoli Federico II, Italy
9-2: Study of Standpipe and Loop Seal 10-2: A Study of Solids and Gas Mixing
11:14 - 11:28 am Behavior in a Circulating Fluidized Bed in a Partitioned Fluidized Bed
for Geldart B Particles
J-H. Moon, Y-J. Seo, S. Kang, S-Y. Lee,
A.R. Bidwe, A. Charitos, H. Dieter, A. Wei, M. Y-C. Park, H-J. Ryu, G-T. Jin
Zieba, G. Scheffknecht Korea Institute of Energy Research, Korea
University of Stuttgart, Germany
9-3: Observation of Flow Regime 10-3: Effect of Temperature Field on the

11:28 - 11:42 am Transition in a CFB Riser Using an LDV Coal Devolatilization in a Millisecond
Downer Reactor
P. Yue, J. Mei, L. Shadle
National Energy Technology Laboratory, USA B. Yan, L. Zhang, Y. Jin, Y. Cheng
Wednesday, May 4, 2011 (continued)
9-4: Bench-Scale Investigation of 10-4: Effect of Bed Temperature, Fuel

11:42 - 11:56 am Limestone Size Evolution in a Fluidized Density and Particle Size on
Bed Combustor Hydrodynamic Parameters of 10 MW
Fluidized Bed Combustion Power Plant
X. Yao, N. Hu, H. Yang Using Riser Waste
J.H. Chiu, P. Gauville, S.G. Kang R..I. Singh Jassar
Alstom Power Inc., USA Guru Nanak Dev Engineering College
S.K. Mohapatra
Thapar University, India
9-5: Catalyst Attrition in the CFB Riser 10-5: Transient Temperature and Char
11:56 - 12:10 am Conversion Profiles in Wood During
A. Thon, M. Kramp, E-U. Hartge, S. Heinrich, Devolatilization in a Fluidized Bed
J. Werther Combustor
Germany D.R. Sudhakar, A.K. Kolar
Indian Institute of Technology Madras
India
9-6: The Relationship Between
12:10 - 12:24 am Fluidization Velocity and Segregation in
Two-Component Fluidized Beds: A
Preliminary Analysis
B. Formisani, R. Girimonte, V. Vivacqua
University of Calabria, Italy
12:30 - 2:00 pm LUNCH
2:00 - 5:30 pm FREE TIME
SESSION 11 SESSION 12
Mathematical Modeling III Measurement Techniques
R. Cocco J. R. van Ommen
T. Shimizu M. Palonen
11-1: Comparison of Entrainment Rate 12-1: Time-Resolved X-Ray

5:30 - 5:44 pm in Acrylonitrile Reactors Using Plant Tomography of a Fluidized Bed of
Data and CFD Simulations Geldart A Particles
S. Moffatt, S. Ramchandran\ R. Mudde, Q. Ricoux, E. Wagner,
Ascend Performance Materials J.R. van Ommen
P. Zhao, K. Williams Delft University of Technology
CPFD-Software, LLC The Netherlands
11-2: Critical Evaluation of Euler-Euler 12-2: A New Approach for Modeling of
5:44 - 5:58 pm and Euler-Lagrangian Modelling a Fluidized Bed by CFD-DEM
Strategies in a 2-D Gas Fluidized Bed
S. Karimi, H. Chizari, N. Mostoufi,
F. Hernandez-Jimenez, A. Acosta-Iborra R. Sotudeh-Gharebagh
University Carlos III Madrid University of Tehran
Spain Iran
J.R. Third, C.R. Muller
ETH Zurich
Switzerland
11-3: Particle-Fluid Flow Simulation of 12-3: Characterization of Fluidization
5:58 - 6:12 pm an FCC Regenerator and Mixing of Binary Mixtures
Containing Biomass at Low Velocities
S. Clark Through Analyzing Local Pressure
CPFD Software Fluctuations
USA
F. Fotovat, J. Shabanian, J. Chaouki,
J. Bergthorson
Ecole Polytechnique de Montreal, Canada
11-4: CFD Simulation of CO2 Sorption 12-4: ECVT Imaging of 3-D Flow
6:12 - 6:26 pm in a Circulating Fluidized Bed Using Structures and Solids Concentration
Deactivation Kinetic Model Distributions in a Riser and a Bend of a
Gas-Solid Circulating Fluidized Bed
E. Abbasi, H. Arastoopour
Illinois Institute of Technology F. Wang, Q. Marashdeh, L-S. Fan
USA The Ohio State University, USA
11-5: CFD Modeling of Fluidized Bed 12-5: Description of Pressure

6:26 - 6:40 pm Reactor for the Synthesis of Dimethyl Fluctuations in a Circulating Fluidized
Ether Bed by Statistical Analysis
R. Kalluri, N. Akunuri, A. Jamal, R. Gupta R. Coetzer, A. Mostert, A. Luckos
RTI International Sasol Technology, South Africa
USA
11-6: DEM Study of Fluidized Bed 12-6: Dynamics of Gas-Solids Fluidized

6:40 - 6:54 pm Dynamics During Particle Coating in a Beds Through Pressure Fluctuations:
Spouted Bed Apparatus A Brief Examination of Methods of
Analysis
S. Antonyuk, S. Heinrich, A. Ershova
Hamburg University of Technology S. Sasic, F. Johnsson
Germany Chalmers University, Sweden
M-O. Coppens
Renssalaer Polytechnic Institute, USA
J. van der Shaaf, Eindhoven University of
Technology, The Netherlands
S. Gheorghiu, Center for Complexity Studies
Romania
J. R. van Ommen, Delft University of
Technology, The Netherlands
12-7: Dynamic Characteristics of

6:54 - 7:08 pm Bubbling and Turbulent Fluidization
Using a Hurst Analysis Technique
H. Azizpour, N. Mostoufi, R. Zarghami
R. Sotudeh-Gharebagh
University of Tehran, Iran
7:30 – 10:30 pm CONFERENCE DINNER at the High Desert Museum
10:45 - 11:45 pm POSTER SESSION and SOCIAL HOUR

for Papers Presented in Sessions 9, 10, 11 and 12
Thursday, May 5, 2011
8:30 am END OF CONFERENCE

REFLECTIONS ON MATHEMATICAL MODELS AND
SIMULATION OF GAS-PARTICLE FLOWS
Sankaran Sundaresan
Department of Chemical & Biological Engineering
Princeton University
Princeton, New Jersey 08544 USA
ABSTRACT
Examples of complex flow characteristics observed in circulating fluidized beds and

turbulent fluidized beds are presented. Different gas-particle modeling and simulation
approaches that are being pursued to probe these flow characteristics are
summarized. Major advances that are likely to emerge within the next decade are
discussed.
1. INTRODUCTION
Circulating fluidized beds (CFBs) and turbulent fluidized beds (TFBs) are applied
widely in chemical process and energy conversion industries (1). They have been in
use in fluid catalytic cracking of gas oil for nearly seven decades, and for lesser
duration in many other processes; new processes, such as synthesis of olefins from
methanol (2), coal and biomass gasification (3), and CO2 capture by solid sorbents
(4, 5), are under development at the present time. Although the long history of use
has led to a wealth of design and operational experience with these systems,
confidence to design and build commercial plants without significant levels of pilot
scale testing at various intermediate scales is still lacking. This is due to an
incomplete understanding of the origin and nature of the inherently complex flow
structures observed in these devices, and uncertainties as to how they would change
upon scale-up. Advanced experimental characterization and rigorous modeling
studies are being pursued to unravel the complexities of these flows in both pilot and
commercial scale systems. This article presents briefly the author’s perspective on
the current status of modeling these flows and the advances that can be expected to
emerge in the near future.
Section 2 outlines a few illustrative examples of intriguing behavior of CFBs and

TFBs, and what one would like to model and understand. This is followed by a brief
discussion of why modeling them is difficult. Section 3 attempts to explain why
effective fluid-particle drag force model is a critical element in accurate and yet
affordable simulations. Section 4 is devoted to advances being made in different
modeling approaches. Section 5 touches very briefly on role of gas turbulence.
Section 6 outlines some additional data that can benefit modeling efforts. Section 7
provides an outlook of what advances in modeling and simulations can be expected
in the next 5-10 years.
1
2. SOME FLOW CHARACTERISTICS TO UNDERSTAND AND MODEL
In its simplest form, a CFB consists of a riser tube where particles are transported up
by co-flowing gas, a device to separate the gas and particles at the top, a standpipe
to return the particles to the bottom of the riser and a suitable valve to control the
delivery of the particles to the bottom of the riser. The volume fraction of particles in
the riser is generally small enough that the particles interact with each other primarily
through collisions, while in standpipes it is usually high enough that stress
transmission can occur through collisions as well as sustained frictional contact
between the particles and between the particles and the wall. More elaborate CFBs
would include additional devices such as fluidized beds (e.g., FCC regenerator),
leading to more complex flow loops for the particles. Let us briefly review a few flow
characteristics that one would like to be able to understand and model.
a) In tall CFBs, operating at near atmospheric pressures, the gas pressure can
increase appreciably from the top of the standpipe to the bottom resulting in
loss of gas volume through compression; to compensate for the adverse
effect of this compression, aeration gas is added at a number of elevations
along the standpipe. At low aeration levels, stick-slip flow is often observed in
the standpipe. Increasing the aeration level enables smoother flow and
improved solids circulation rate. However, beyond some threshold aeration
level, the flow becomes unstable and the circulation rate becomes very
erratic, which is unacceptable (6). How does the onset of this instability
depend on the manner in which aeration is administered and the scale of the
CFB?
b) The flow characteristics in the riser are complex even under stable operating
conditions. Risers typically operate in the so-called fast-fluidization regime
where there is a denser bottom region, transitioning to a more dilute flow at
the top. Furthermore, the time-averaged particle volume fraction and gas and
particle mass fluxes manifest significant lateral variations; particle volume
fractions generally tend to be high near the riser walls where the mass flux of
particles is frequently negative (i.e. downflow) even though the cross-
sectionally averaged mass flux of particles is positive (7). The particles tend
to drag the gas downward in the wall region, and so there can be significant
internal recirculation of both particles and gas in the riser. At very high gas
velocities, the downflow disappears and one can even get a higher mass flux
of particles at the wall region than the core (8). How well can we capture
these trends in models and how confident are we in predicting the flow
pattern changes that will come about upon scale-up, flow rates or
modifications to the flow device?
c) Since risers are often used to carry out (catalytic or non-catalytic) chemical
reactions involving the gas and particles, one can anticipate that these
persistent macro-scale non-uniformities would affect the effective contact
between particles and the gas, and hence the conversion and selectivities.
How well can we model these effects and propose design choices to
maximize conversion and/or selectivity?
d) Gas by-passing is a common concern in the operation of turbulent fluidized
beds and the beds are extensively baffled to mitigate this problem. Deep
beds operating at low (say, near-atmospheric) pressures are particularly
2
susceptible to local defluidization and gulf-streaming (9). Can we capture
such flows in models and simulations, and predict how they will change upon
scale-up and process modifications (such as the introduction of baffles)?
When such inhomogeneous flows arise in chemical reactors, they can affect
conversions and selectivities; they can also lead to reactant breakthrough to
the top of the bed and cause unwanted freeboard reactions. For example, in
FCC regenerators, oxygen breakthrough causes CO combustion in the
freeboard leading to high temperatures that favor NOx formation (10). Can
such problems be detected in simulations in a reliable manner?
e) Cyclones play vital functions in CFBs in capturing and returning the particles
and minimizing particle emissions. The mass loading of particles in the
stream entering the cyclones varies appreciably from stage to stage. The
separation efficiency of cyclones is determined by the competition between
the swirling flow which aids particle separation and turbulent dispersion which
results in re-entrainment of particles into the gas (11, 12). Mass loading of
particles affects both the strength of the swirl and turbulent intensity (13-15);
how well can we model and simulate these effects?
f) In some processes carried out in CFBs and TFBs, liquid is intentionally
injected (16) either as a reactant or for coating purposes. In such systems,
one can readily expect that in some regions of the bed (e.g., close to where
the liquid is injected), the particles will be coated with a liquid and this can
lead to agglomeration of the particles. These agglomerates are likely to
induce local defluidization and cause secondary flow structures in the CFBs
and TFBs (17). How well do we understand these secondary flow structures
and their effects on conversions and selectivities (or coating uniformity)?
The above list, though incomplete, illustrates some characteristics that one would
like to understand and model with confidence, so that the models can then be used
as tools to test design options for new plants as well modifications to existing units.
More specifically, the models should help us understand the macroscale flow
behavior and allow us to perform computational experiments exploring means of
manipulating the flow to maximize a desired set of objectives, such as conversion,
selectivity and operational stability.
What makes modeling difficult? One can readily list a number of reasons, a few of
which are described below.
a) Circulating fluidized beds typically consist of a number of devices, as

mentioned above, and regions with widely different particle volume fractions
are encountered in the flow loop. As a result, the manner in which stress is
transmitted through the particles changes significantly from location to
location. For example, such stress transmission occurs predominantly by
collisions in the riser, while in the standpipe and slide (or “L”) valves stresses
transmitted through enduring contact become important. As the overall
performance involves a complex interaction of various devices in the
circulation loop, a good model should account for the effect of stress
transmission through particles via collisions as well as enduring contact.
b) Meso-scale structures form as a result of the instability of two-phase fluidized
flow when the particle volume fraction becomes too small to support
sustained force chains (18); the point at which this occurs depends on
particle roughness, size (which affects the importance of cohesion) and
3
shape. These meso-scale structures take the form of bubble-like voids at high
mean particle volume fractions (approximately greater than 0.40) and clusters
and streamers at low mean particle volume fractions (approximately less than
0.25) (19). In the intermediate region, a turbulent state exists where the
meso-scale structure changes rapidly between bubble-like voids and clusters
and streamers. These structures are generally difficult to resolve in
computations; yet, they affect the gas-particle interactions (such as the
effective fluid-particle drag, the heat and mass transfer rates, and the stress
transmission in the particle and fluid phases).
c) The particles invariably have a distribution of sizes that evolve naturally
through attrition, or develop because of reactions occurring in the fluidized
beds. Accounting for the particle size distribution (PSD) is critical to predict
accurately the rate of elutriation from turbulent fluidized beds, cyclone
efficiency, etc.
3. THE FLUID-PARTICLE DRAG
It is easy to understand that one must include gravity (which pulls the particles to the
bottom of any device), pressure gradient (which establishes motion of the gas
relative to the particles) and fluid-particle drag (which is the principal means by which
particles can be suspended against gravity) in any model to capture the flow of
fluidized suspensions. The accuracy with which the fluid-particle drag can be
determined is critically important in modeling of fluidized suspension flows. A number
of empirical constitutive models for the fluid-particle drag in homogeneous
suspensions of uniformly sized spherical particles are available in the literature (20);
a prominent example is the widely used correlation due to Wen & Yu (21). A practical
difficulty comes about when we apply such correlations developed for (nearly)
homogeneous suspensions to flows of fluidized gas-particle mixtures.
As noted earlier, fluidized suspensions readily form inhomogeneities that span a

wide range of length and time scales. As a result of these inhomogeneities, flows in
turbulent fluidized beds and risers are invariably multi-dimensional. Furthermore,
when the particles and the gas move around from one location to another in a
device, inertia should be included in the models. Inertia – especially, the particle
phase inertia – is important to capture the formation of flow inhomogeneities such as
bubbles, clusters and streamers. As a result of the multi-dimensionality and inclusion
of inertia, the models are invariably solved numerically on suitable spatial grids (more
on solution methods later). Such computations resolve the flow at scales larger than
the grid resolution, but not those occurring at a sub-grid scale. Using extremely fine
grid resolution to resolve all the flow structures is often not practical.
The challenge in accounting for the effective drag force accurately can be illustrated
as follows. Consider a zero-dimensional (0D) model for a turbulent fluidized bed, i.e.
the entire bed is simulated using a single numerical grid cell. Such a 0D model
ignores all the flow structures present in the bed and reduces to a force balance over
a uniformly fluidized bed. If drag force correlations intended for homogeneous
suspensions are employed, one readily concludes that the superficial gas velocity
must remain well below the terminal settling velocity (vt) of the particles in the bed;
however, this is almost never the case and most turbulent fluidized beds operate at
velocities in excess of vt. This difference is primarily due to the fact that the
inhomogeneities, which were not resolved in this 0D analysis, result in a decrease in
4
the fluid-particle drag and it has not been properly accounted for in the analysis. To
capture the particle volume fraction in the bed correctly using such a 0D model, one
must modify the drag force correlation to reflect the effects of unresolved flow
inhomogeneities. If one analyzes the same system as an unsteady flow problem
using several numerical grid cells, then some of the flow inhomogeneities will be
resolved, and so the modification to the drag force correlation will now be different;
as the number of grids increases, the required modification to the drag force
correlation decreases. Knowing what inhomogeneous flow structures have not been
resolved and how one should account for their effects on the effective fluid-particle
interaction (drag) force is a challenge. This issue has been addressed in the
literature. O’Brien & Syamlal (22) and Heynderickx et al. (23) corrected the drag
coefficient at very low particle volume fractions to account for the consequence of
clustering. McKeen & Pugsley (24) used an apparent cluster size in an effective drag
coefficient closure. Li and coworkers (25) deduced corrections to the drag coefficient
using an Energy Minimization Multi-Scale approach. Filtered models, where the
effects of sub-filter scale inhomogeneities on the drag force are modeled by
introducing a filter size dependent drag law, are being developed (26, 27);
Parmentier et al. (27) have presented an additional advance where the filter size
dependent drag force is dynamically corrected in simulation of filtered model
simulations. The development of these filtered models is still in the early stage, and
many more validation studies are needed to test and refine these models.
All the modifications to the drag law that have been described in the literature,
which are intended to correct for unresolved structures, are for uniformly sized
particles. Drag laws for homogeneous suspensions of particles having a distribution
of sizes are described in the literature (28); however, little has been published in the
literature on modifying these drag force correlations to correct for unresolved
structures.
4. FORM OF THE MODEL FOR GAS-PARTICLE FLOWS
The above discussion touched upon numerical computations without making specific
reference to the form of the models for gas-particle flows. All the models for gas-
particle flows solve the Eulerian form of the continuity and momentum balance
equations for the gas phase on a fixed spatial grid, and so the unresolved structures
discussed above are obviously relevant. When solving for the particle phase, there
are multiple options.
4.1. Eulerian treatment of the particle phase(s)
In two-fluid models, Eulerian continuity and momentum balance equations are

formulated for the particle phase as well, and are solved using the same grids (as for
the gas phase). This approach (also referred to as the Eulerian-Eulerian model) has
a long history of development and analysis. When multiple types of particles are
present, they can be generalized as multi-fluid models, where each particle type is
treated as a separate phase, interacting with all the other phases.
Two-fluid models have served well in our quest to understand the underlying
mechanisms leading to inhomogeneous structures. For example, one can readily find
the solution of two-fluid model equations corresponding to the state of uniform
fluidization analytically, and examine its linear stability to pinpoint the origin of
5
instability leading to bubble-like voids in dense suspensions, as well as clusters and
streamers in dilute suspensions (19, 29, 30), and the characteristic length and time
scales associated with the dominant instability mode. It has also helped advance
simple qualitative arguments explaining why particles segregate towards the walls in
riser flows (31).
The two-fluid model equation for the particle phase allows for stress transmission
through the particle phase. Over the past three decades, researchers have adapted
the kinetic theory of dense gases and developed constitutive models for the rheology
of assemblies of monodisperse, spherical and inelastic particles interacting through
binary collisions (32, 33). Such models, generally referred to as kinetic theory of
granular materials, require solution of an additional scalar equation for the kinetic
energy per unit mass associated with the fluctuating motion of the particles relative to
the local average velocity of the particle phase (a.k.a. granular temperature); the
particle phase stress is then expressed in terms of local particle volume fraction,
granular temperature and local rate of deformation of the particle phase.
The kinetic theory models have also been generalized for mixtures of different types
of particles (32-37). These multi-fluid models can take one of two forms:
(a) Separate continuity, momentum and granular energy balance equations are
formulated for each particle phase, and solved. In this approach, if there are
N different particle phases, one has to solve (N+1) continuity equations,
d(N+1) momentum balances (where d denotes the number of spatial
dimensions involved in the problem) and N granular energy balance
equations (34, 35).
(b) Continuity equations are formulated for the N different particle species, along
with a single momentum balance equation and a single granular energy
balance equation for the particle mixture; these are supplemented by
algebraic models for the granular temperatures of the different particle
species and the “diffusive” flux of each particle species relative to the mixture
flow. In this approach, one has to solve (N+1) continuity equations 2d
momentum balances, one granular energy balance equation, along with a set
of algebraic equations to determine the diffusive fluxes (36, 37).
A recent study comparing these two approaches found that both approaches yield
similar predictions for binary particle mixtures, with the latter approach requiring less
computational time (38); the advantage is likely to be more significant when the
number of particle species increases.
While the kinetic theory has given us a good handle on particle phase stress
resulting from particle streaming and collisions, models for stress in the dense,
quasi-static flow regime where the particles make enduring contacts with multiple
neighbors and stress is transmitted largely through force chains are by and large
phenomenological (39-41).
Distribution of particle sizes is handled in the Eulerian modeling approach in several

different ways. In one approach, the particles are divided into a number of cuts, each
representing a size range and each cut is treated as a separate particle phase. Multi-
fluid models are solved to determine the flow behavior. In the other approach –
discrete quadrature method-of moment – the actual PSD is replaced by a sum of
6
delta functions placed at judiciously selected particle sizes (quadrature nodes); these
quadrature nodes are allowed to change temporally and spatially to capture
agglomeration and break-up, change in size by chemical reactions, etc. (42). The
number of different particle phases that are needed to capture the effect of PSD will
clearly depend on the nature of the PSD; studies addressing how the predictions
change as more and more particle phases are used to approximate a given PSD are
beginning to appear in the literature (43).
The development of software platforms for solving multi-fluid models has progressed
appreciably over the past two decades. The open-domain code MFIX developed at
NETL (22) and commercial software (e.g., ANSYS Fluent®) are widely used by
many research groups around the world to study reacting multiphase flows. Many
research groups also employ in-house codes to solve such models (e.g., Neptune in
the research group of Olivier Simonin).
Application of multi-fluid models to simulate gas-particle flows does raise questions

and also poses a number of challenges. Let us consider the two-fluid model where
the all the particles are treated as a single particle phase and examine the issues:
a) A basic question that one can raise concerns the validity of treatment of the
particle phase via a continuum model. In writing such a model, it is presumed
that the particles interact with each other rapidly, thus endowing the particle
phase with a pressure and a viscosity. In normal fluids, we are able to do this
for low Mach number flows as there is a clear separation of scales between
the random motion of the molecules that gives rise to pressure and viscosity,
and the mean velocity of the fluid phase. It is not at all obvious that such a
separation of scales exists for the particle phase in most gas-particle flows
where the particles interact via binary collisions. In such situations, the low
order moments of the particle velocity distribution function - namely, mass,
momentum and fluctuation energy - which are evolved through the particle
phase continuity, momentum and granular energy balance equations - may
not adequately define the full flow problem.
b) High resolution simulations of gas-particle flows via two-fluid models yield fine
structures at length scales as small as 10 particle diameters, and it is argued
by some that these fine structures are not real features of gas-particle flows
and that it is manifestation of the inadequacy of the continuum treatment of
particle phase in the two-fluid model.
c) The existence of such fine structure raises the issue on the required grid
resolution. Resolving all the fine structures contained in the two-fluid model
equations requires numerical computations using extremely fine grids. These
are simply unaffordable. This necessitates development of filtered two-fluid
models where the fine structures are smoothed out and their effects on the
resolved flow are modeled. While some progress has been made on the
hydrodynamic aspect of filtered two-fluid models, corresponding thermal
energy and species balance equations have not yet been developed and
validated.
d) Handling PSD using multi-fluid models, especially when the PSD is changing
due to reactions, break-up, etc., remains a challenge.
e) Three-dimensional simulations using two-fluid models of large process units
remain expensive (unless one uses filtered models that permit coarse grids);
multi-fluid models increase the computational cost significantly.
7
f) Boundary conditions for multi-fluid models at solid surfaces are still primitive.
g) The continuum hydrodynamic model for the particle phase is obtained by
taking the low-order moments of the Boltzmann equation for the particle
distribution functions; such an approach usually emphasizes dominant
aspects of flow. In some engineering applications, one would like to
understand relatively rare events (such as formation of hard particle
agglomerates in fluid cokers); two-fluid models are not useful for such
inquiries.
4.2. Lagrangian treatment of the particle phase(s)
Here one formulates and solves Newton’s equations for the motion of particles. Also,
the particles are not restricted to be on an Eulerian mesh (e.g., the one used to solve
for the gas phase variables). The fluid velocity and pressure gradient at the particle
locations, required to solve the particle momentum balance, are readily obtained
from the Eulerian (fluid phase) mesh via interpolation. Similarly, the force on the fluid
due to the particles can readily be mapped to the Eulerian mesh from the particle
locations. Such Lagrangian treatment offers several advantages, while also placing
some limitations, as discussed below.
At very low volume fractions where inter-particle collisions are rare and unimportant,
one can formally ignore collisions and employ a point-particle approximation. Such
an approach is used extensively in the literature in studies on particle-turbulence
interactions. In the context of CFBs, it is employed in (secondary and tertiary)
cyclones. Typically 1-50 million point particles can be tracked in practical simulations
and so it is possible to follow all the particles in modestly sized devices only at
extremely low particle volume fractions.
4.2.1. Parcel-based approach
To circumvent this limitation on the number of particles that can be simulated,

parcels of point particles are simulated. Here each test particle being tracked
represents a large number of particles having the same characteristics as the test
particle (e.g., see Andrews and O’Rourke (44), or Pantakar and Joseph (45). Such a
parcel based approach can appreciably expand the range particle volume fractions
that can be handled.
The approach using parcels of point particles must be modified when the particle
volume fraction becomes sufficiently large that interactions between particles via
collisions, sustained force chains, cohesion, etc. become important. In the multi-
phase particle-in-cell (MP-PIC) method, the interaction of other particles with a test
particle (parcel) is modeled by a force on the test particle that is proportional to the
prevailing particle phase volume fraction gradient at the location of the test particle
(46-49). Clearly, even though one tracks point particles, it is recognized that each
particle has a finite volume; the particle phase volume fraction and its gradient at the
location of the test particle affects both the fluid-particle drag and the effective force
due to the interaction between particles.
Conceptually, the parcel-based MP-PIC method and the multi-fluid model are
equivalent; this has been illustrated recently by direct comparison of the two
approaches on a model flow problem (50). Nevertheless, there are clear differences
8
in the advantages offered by the two approaches. As noted earlier, the two-fluid
model approach is readily amenable to stability and simple macroscopic analyses,
which have been useful to develop better understanding of the competing forces
leading to complex flow structures. The MP-PIC approach always requires a
numerical solution and is not well-suited for simple mathematical analyses. On the
other hand, the parcel-based MP-PIC approach does have major attractions:
a) Particle size distribution is much more easily handled than in multi-fluid

models.
b) In dilute flows where the interaction of particles with bounding surfaces
occurs mainly by collisions, boundary conditions are easily implemented.
c) Changing particle properties and size are easily handled.
d) As a large number of parcels are tracked, there is a possibility that rare
events can be detected and analyzed.
The parcel-based MP-PIC approach [available commercially, CPFD®] has indeed

rapidly emerged as very powerful and is being used more and more in industries.
Preliminary versions of this approach are available in MFIX as well. It is now being
offered as an option in Fluent® as well. In the opinion of this author, parcel-based
MP-PIC method will likely emerge over the next decade as a preferred approach for
reasons mentioned above. At the same time, it should be noted that this approach
has not been tested as extensively as the two-fluid models. There are relatively few
interrogations of the properties of solutions obtained by this approach; for example,
studies investigating the influence of grid resolution on the solutions for various
classes of flow problems – fluidized beds, risers, etc. – are needed. A limited
investigation (50) performed recently shows that at fine grid resolution the parcel
based approach yields similar microstructure as the two-fluid model, and so it
appears that MP-PIC simulation of flows in large devices using coarse grids will need
filtered fluid-particle drag force models (and possibly modifications to the effective
particle interaction force as well) – as in the case of multi-fluid models. If this is
indeed the case, and if so, what filtered fluid-particle drag force model is appropriate
for the parcel-based approach, are not clearly understood at the present time.
It would also be useful to perform more simulations of classical problems to gain

better understanding of the parcel-based approach itself, as well as the underlying
flow physics. One example would be simulations of fluidization in a vertical pipe over
a wide range of gas velocities and particle fluxes, thus generating a map of average
pressure gradient vs. gas velocity at different particle mass fluxes. The general
character of such phase diagrams are well known experimentally: choking,
multiplicity of states and carrying capacity of the gas have been widely studied
experimentally (51, 52). Demonstrating that such complex phase diagrams can be
robustly captured would greatly increase the confidence of the method in the minds
of the users, than simply testing the method against a few operating conditions.
4.2.2. Discrete Element Method (DEM) for spherical particles
One can, in principle, circumvent the need to postulate a phenomenological model

for the force on a test particle due to interactions with other particles (in the parcel
approach) by directly simulating all the finitely sized particles in a region and their
interaction via collisions and enduring contacts. Though these simulations may allow
9
for arbitrarily shaped particles, let us focus first on spherical particles, which have
been studied the most using granular/molecular dynamics. In assemblies at low
particle volume fraction, where the particles interact largely through binary collisions,
grains are conveniently modeled as hard particles that experience instantaneous
collisions, which are detected using an event-based algorithm. At high volume
fractions, where particles tend to make enduring contact, DEM is the preferred
approach, where the particles are modeled as soft spheres that can overlap slightly
and exert both normal and tangential forces on each other (53). DEM simulations,
however, are computationally expensive. In the early 1990’s, DEM simulations were
limited to about 103 particles (54, 55); simulations of millions of soft-sphere particles
are now feasible using CPUs with higher clock frequency, as well as computer
clusters. Also, significant improvements in commercial (e.g. PFC3D (56)), as well as
open-source (e.g., LAMMPS (57)) software make DEM simulations more common.
Recent applications of DEM-based simulations of particle flows also include a
coupling to computational fluid dynamics (CFD) of the fluid phase, e.g., cyclone
separators under high mass loads (58), or the DEM-CFD model recently proposed
for fluidized bed reactors including heat, and mass transfer, as well as chemical
reactions (59). Computations using Graphic Processing Units (GPUs) have become
fashionable after software to use these powerful co-processors was published (60).
Tailored applications focusing on single-GPU computations have been developed,
enabling a roughly 100-fold speed-up compared to conventional single-CPU
calculations (61, 62). Thus, the application of DEM-CFD models is poised to grow
rapidly in the years ahead.
DEM is also widely used as a tool to study rheological behavior of dense particle
assemblies (63-65). However, most of these studies have been only for spherical
particles. Also, these simulations tend to use simple interaction models (e.g., the
linear spring-dashpot model of Cundall and Strack (66)). A comprehensive overview
of more sophisticated contact force models, e.g. accounting for rolling and twisting
resistance between particles, is given by Luding (67). Rarely do all details of these
sophisticated contact forces and torques significantly impact granular flow behavior
in most of industrial applications of interest; instead, the effect of particle shape has a
more severe impact on the static and dynamic features of a granular assembly (53).
4.2.3. DEM for non-spherical particles
The effect of particle shape on flow behavior is currently an active area of research –
both from an experimental, as well as modeling point of view. Campbell (68)
investigated the flow of prolate spheroidal particles and their effect on granular flow
transition; he found that force chain formation, and consequently the stresses in a
quasi-static flow situation, depend strongly on particle shape. A specialized algorithm
for cylindrical objects has recently been published by Kodam et al. (69, 70). In this
latter work the particles are described as true cylinders (as opposed to spherical
particles glued together). Also, Kodam et al. provided experimental verification of
their approach, as well as a comparison of their simulation with a glued-sphere
approach. DEM simulation of non-spherical particles requires significantly more
computational resources than a similar simulation of spherical particles. Although
various strategies to approximate the true shape of particles exist, they currently
cannot compete with the accuracy and details of particle interaction force modeling
available for spherical particles. This point is even true for specialized algorithms,
e.g., the one used by Kodam et al. (70), as the latter did not include rolling or twisting
10
resistance. Thus, there will be always a compromise between particle shape, contact
force modeling, as well as time and resources available for the simulation.
While the effect of shape on dry granular flow without interaction with the gas phase
has been summarized recently (53), there is much less published on fluidized
suspensions; more studies would be useful to fully expose the role of particle shape
on fluidization. Recently, Liu et al. (71) measured lower fluidization velocities of non-
spherical particles compared to sphere packings. Hilton et al. (72) simulated non-
spherical Geldart group D particles using a DEM-CFD approach. Rosendahl and
Mando (73) recently reviewed the status of models for non-spherical particle motion
in gas-solid flows, and highlighted the importance of the alignment of particles with
turbulent vortices. The effect of particle shape on fluidization is likely to be a concern
in fluidized beds used to gasify biomass, where degassing of the particles may also
alter the effective fluid-particle drag considerably.
4.2.4. More on parcel-based methods
Even with advances in computational power, DEM simulations will remain prohibitive
for large process devices. Therefore, a parcel-based approach will remain the
method of choice for large scale problems. As noted earlier, in the parcel-based MP-
PIC method the particle interaction force is modeled through an empirical particle
pressure, while in DEM simulations they are resolved. Researchers have examined if
the parcel-based method could be configured in a way that the need for empirical
pressure model can be eliminated. Sakai et al. (74) as well as Mohktar et al. (75)
assume that the parcel is represented by a sphere with a volume equivalent to the
sum of the volumes of the particles making up the parcel. This requires contact
detection between parcels, and hence is computationally more expensive than the
parcel-based MP-PIC approach discussed earlier. A primitive form of such contact
detection has been already used in the work of Patankar and Joseph (45). Bierwisch
et al. (76) have shown recently that a parcel-approach with contact detection, when
using appropriately scaled interaction parameters, yields simulation results
independent of the number of particles making up the parcel. In this approach, one
would be performing DEM simulations of the pseudo-particles representing the
parcels, where the characteristics of these pseudo-particles are chosen (based on
dimensional analysis) such that important features of the flow remain equivalent to
the flow of the original particles. Specifically, they show that it is possible to obtain
stresses in the quasi-static regime and parcel velocities in all regimes of granular
flow, that are independent of the scaling of the system. Analogous scaling can be
identified for a linear spring-dashpot model as well (77), whereby properly scaling the
spring stiffness, the damping coefficient, as well as cohesive forces, a parcel-based
approach can be made to yield the same quasi-static flow behavior, stresses, and
particle velocities as the original particle system; however, the parcel-based
approach with contact detection overestimates the stresses in the inertial regime (78)
where stresses are primarily transmitted through collisions and so a correction is
needed.
In their latest work, O’Rourke and Snider (46) propose a method to relax the parcel
velocities to their local mean value which can be adapted to the parcel-based
approach with contact detection to obtain the same particle phase pressure as in the
original system of particles (Radl et al. (77) ). Thus, it seems possible to have a
discrete particle method based on parcels that can closely approximate the stresses
in the original system of particles across different flow regimes. In the opinion of the
11
author, this approach holds promise for simulations of flows in standpipes, hoppers,
spouted beds, dense phase pneumatic conveying, etc.
5. ROLE OF GAS TURBULENCES IN CFBs AND TFBs
In turbulent and fast fluidized beds, where the mass loading of particles is often one
or more orders of magnitude larger than that of the gas, gas turbulence has only a
secondary effect on the flow in most of the regions (in the opinion of this author). Its
effect is more likely to be localized in regions where the particle volume fraction is
low (for example, in cyclones where turbulent dispersion of particles lead to loss of
separation efficiency) and at the interface separating dense and dilute region where
it plays an important role in entrainment of particles into the dilute stream (for
example, particle pickup by turbulent eddies in pneumatic conveying, and
entrainment of particles into jets). Adequate resolution of gas-phase turbulent
fluctuations (e.g., via Large Eddy Simulations, or Direct Numerical Simulations) in
industrial-scale devices and jets, especially at high particle volume fractions, does
not seem feasible for the foreseeable future. We will continue to rely on sub-grid
models for the role of gas turbulence in inducing fluctuations in the particle phase.
Such models can readily be included in the granular energy equation of the two-fluid
model and in parcel-based models (79, 80). This seems adequate for modeling gas-
phase stresses in CFB applications, where the mass loading (i.e., the ratio of particle
mass flux to gas mass flux) is relatively high.
6. MODEL VERIFICATION AND VALIDATION
It is clear from the discussion above that a variety of different models are being
applied to study gas-particle flows, and simulations are based on discretized
versions of these models. It is important that the models and the simulators based on
these models be subjected to careful verification as well as validation with
experimental data. What constitutes verification and what is validation have been
discussed in some detail by Grace (81).
Verification is an essential first step and it can take several different forms depending
on the model being tested:
a) It is important to demonstrate that simulators based on any model be compared

(if possible) with analytically obtainable results for some test problems, even if
the problems are highly idealized. For example, in two-fluid models for gas-
particle flows, the growth rate of instability modes (starting from a uniformly
fluidized state) can be determined readily through linear stability analysis;
verifying whether numerical codes can reproduce the analytical results (and if so
at what grid resolution and time steps) is a natural test of the fidelity of the code
[for example, see ref. (30)].
b) When parcel-based model simulations with collision tracking are formulated, it is
important to verify that they yield the expected trends in predictions as one
changes parcel size [For example, see ref. (77)].
c) When a filtered two-fluid model is developed by coarse-graining some (say,
kinetic theory based) two-fluid model equations, one should verify that
simulations of the filtered model yield the same coarse flow structures as the
underlying two-fluid model (82).
12
d) Models invariably involve approximations; frequently different models tend to
capture different aspects of physics more accurately. Yet, there must be
situations where the different models agree with each other reasonably well; and
so, it makes eminent sense to compare predictions of various models. Such
predictions fall in the category of verification and not validation. For example,
demonstration that two-fluid model and a parcel-based model yield nearly the
same results in simulations of a highly idealized flow problem (50) is a useful
verification step as it enhances the credibility, establishes equivalence between
models and exposes how ideas from one approach can be adapted for the other.
Comparison of CFD-DEM and multi-fluid models is also in the same spirit.
e) Comparison of the simulation results obtained at different grid resolutions is also
an important verification step. Although this is indeed done in most published
articles in an empirical manner (i.e. presenting results obtained at different grid
resolutions for one or two test simulations), concrete guidelines on grid
resolutions needed to get grid-size independent results are generally not
available, with a recent study by Parmentier et al. (27) being a welcome
exception. As a result even when grid size independence is demonstrated and
the simulation is validated against experimental data in a pilot scale unit, practical
challenges regarding grid resolution requirements when applying that simulation
approach to large scale devices are not fully appreciated. Good verification
studies should strive to bring forward simulation issues at different scales.
Even though most of the simulation studies solve the unsteady equations governing
the flow, attempts to validate have invariably focused on time-averaged flow
characteristics such as axial pressure profile and lateral variation of particle volume
fraction and mass flux. Indeed, these quantities arise naturally as the most important
ones. Since the flows manifest persistent fluctuations, comparing the power spectra
of fluctuations between the models and experiments makes eminent sense (of which
differential pressure is the easiest to measure). Since the extent of contact between
the gas and the particles is intimately linked to gas dispersion characteristics, they
are also important metrics. The challenge problems issued as a part of this CFB-10
conference do indeed focus on validation of models with experimental data on these
quantities.
A large number of early studies compared time-averaged results obtained from 2D

simulations with experimental data; with increasing computing power, more and
more 3D simulations are being done. As one would expect, there are quantitative
differences between the results obtained with 2D and 3D simulations, and so true
validation does require 3D simulations. However, 3D simulations are very expensive
and so demonstrating grid independence of solutions is often prohibitive; in the
opinion of this author, it is not at all obvious if some of the published simulation
results are truly grid independent. This point is particularly clear from the simulation
study of turbulent fluidized beds by Parmentier et al. (27) who estimated the grid size
needed for nearly grid independent solution of standard two-fluid models used by
most researchers; such resolution is often not feasible in commercial scale devices.
Based on a recent study (50) comparing the two-fluid model and a parcel based
approach, it appears that the grid resolution requirement for the latter approach is
also similar. Given this concern (as to whether the computed results are truly grid
independent), there is a lingering doubt as to whether favorable comparison of model
predictions with experimental data is really indicative of successful validation or a
coincidence for the chosen grid resolution. Researchers engaged in simulations
13
certainly understand the need to seek grid independent results, and so the above
comment is not intended as a criticism; instead, it is presented as a practical
limitation imposed by the size of the problem that one can simulate within the
available resources. As clearly demonstrated by Parmentier et al. (27), the grid
resolution needed to get a grid-independent solution changes appreciably with
particle size. Therefore, experimental data on riser flows and turbulent fluidized beds
for particles of different sizes would be valuable. The challenge problem (#3)
discussed in this conference considers riser flow data for 59 m (group A) and 802
m (group B) particles. It would be useful to generate riser flow results for several
intermediate sizes as well. The challenge problems include turbulent fluidized bed
data for a single particle size (~75-80 m, with different fines contents); data for
somewhat larger particles would be useful as well.
Even if a particular model is validated successfully using pilot scale data (at a certain
grid resolution), is there a basis for trusting the simulation results on commercial
scale device performance obtained using this model and necessarily coarser grids?
This question has been repeatedly posed to the author of this article by researchers
in industries (who use the simulation tools to evaluate performance of commercial
scale devices). A major concern in scale-up from pilot scale to commercial scale has
always been whether the flow characteristics would change qualitatively upon
scaleup and lead to serious shortfall in performance. With this in mind, it is
suggested that one should compare simulation results obtained at different scales
with experimental data. For example, the current challenge problem (#3) considers
data obtained in a 30 cm diameter riser; researchers will continue to use these data
for many years to further refine their models and simulators. (The data from earlier
challenge problems continue to be used for validation studies even today.) It would
be useful to collect analogous data on a larger scale unit (say 75 cm diameter riser)
for future challenge problems, so that one can evaluate how well the various models
and simulation approaches capture both sets of data (30 and 75 cm).
A great deal of current research is aimed at incorporating PSD into models and
simulations. To better understand the role of PSD and also validate these models, it
would be useful to have data for different PSDs (particularly for group B particles in
the size range of commercial interest).
Risers tend to operate in the fast fluidization regime, where (sometimes) there is a
dense phase at the bottom transitioning to a dilute phase at higher elevations.
Phase diagrams for riser flows suggest that nearly the same combination of riser gas
velocity and particle mass flux can yield different pressure drops across the riser
depending on the height of the dense region at the bottom. In such situations it is
more sensible to specify one of the fluxes and the pressure gradient and calculate
the other flux as an output. Most simulators do not perform such computations and
part of the reason for poor validation may be due to this. This suggests that it would
be useful to have (at least skeletal) performance data at different riser gas velocities
(while fixing the solids flux) and generating results akin to the phase diagram
mentioned in section 4.2.1). One would then ask how well models and simulations
capture a continuous spectrum of operating conditions – this can help assess if the
departure between models and experiments is qualitative or quantitative.
14
In the not too distant future, simulations of the entire CFB loop will become common.
It would be of interest to develop good data sets on standpipe operation for models
to compare against. The standpipe plays a critical role in stable operation of the CFB
loop. Plant operators often seek to increase circulation rate (which is usually tied to
productivity of the unit) by improving aeration. Unacceptable failure of the standpipe
upon excessive aeration is of practical concern and models and simulations can play
a valuable role in understanding this problem and identifying means of improving
performance without causing instability. Good data to validate simulations of
standpipe flow will help improve confidence in simulations of the full CFB loop.
7. FORWARD LOOK
Within the next 5-10 years, significant advances can be expected in simulation of
CFBs and TFBs, because of improved computer resources, as well as better
modeling approaches. Three-dimensional simulations of full CFB loops will become
more common, and these will pave the way for better understanding of global
phenomena such as loop instability. Instead of performing simulations at a small
number of operating conditions (in individual units such as risers), researchers will
map out model predictions over a range of conditions and examine the robustness of
trends and quantify uncertainties in the simulation results.
At a more fundamental level, coarse-grained drag laws for polydisperse systems will
emerge along with better understanding of how they should be constructed for the
different simulation approaches (multi-fluid models vs. parcel based method). Parcel
based methods (with and without collision detection) will likely emerge as the more
preferred approach, and it will be studied in greater detail by academic researchers
as well, leading to further improvements in the method.
Although not discussed in this article, better understanding of models that one would
use for wet systems (such as fluid cokers) where the particles can form
agglomerates will also emerge (83). These, in conjunction with flow simulators, will
lead to better understanding of secondary flows in such devices. Recent
experimental findings, as well as small-scale simulations are a promising starting
point to refine our understanding of liquid transport in fluidized beds (84, 85).
ACKNOWLEDGEMENTS
The author gratefully acknowledges the help of Stefan Radl, William Holloway and
Sebastian Chialvo in the preparation of this article. Ted Knowlton’s critique of an
initial draft of this manuscript is much appreciated.
REFERENCES
1. Grace, J.; Bi, H., Introduction to circulating fluidized beds. In Circulating

fluidized beds, J.R. Grace, A. A. A., and T. M. Knowlton Ed. Chapman & Hall:
London, 1997.
2. Soundararajan, S.; Dalai, A. K.; Berruti, F., Modeling of methanol to olefins
(mto) process in a circulating fluidized bed reactor. Fuel 2001, 80, (8), 1187-
1197.
3. Delgado, J.; Aznar, M. P.; Corella, J., Biomass gasification with steam in
fluidized bed: Effectiveness of cao, mgo, and cao-mgo for hot raw gas
15
cleaning. Industrial & Engineering Chemistry Research 1997, 36, (5), 1535-
1543.
4. Chalermsinsuwan, B.; Piumsomboon, D.; Gidaspow, D., A computational fluid
dynamics design of a carbon dioxide sorption circulating fluidized bed. AIChE
Journal 2010, 56, 2805-2824.
5. Yi, C.; Jo, S.; Seo, Y.; Lee, J.; Ryu, C., Continuous operation of the
potassium-based dry sorbent co2 capture process with two fluidized-bed
reactors. Int. J. Greenhouse Gas Control 2007, 1, 31-36.
6. Srivastava, A.; Agrawal, K.; Sundaresan, S.; Karri, S. B. R.; Knowlton, T. M.,
Dynamics of gas-particle flow in circulating fluidized beds. Powder
Technology 1998, 100, (2-3), 173-182.
7. Bader, R.; Findlay, J.; Knowlton, T. M. In International circulating fluidized
bed conference, Gas/solid flow patterns on a 30.5 cm diameter circulating
fluidized beds, Compiegne, France, 1988; Compiegne, France, 1988.
8. Karri, S. B. R.; Knowlton, T. M. In Circulating fluidized bed technology vii,
Wall solids upflow and downflow regimes in risers for group A particles,
Ottowa, 2002; J.R. Grace, J.-X. Z., H de Lasa, Ed. Canadian Society of
Chemical Engineering: Ottowa, 2002.
9. Karri, S. B. R.; Issangya, A.; Knowlton, T. M. In Fluidization xi, Gas bypassing
in deep fluidized beds, Naples, Italy, 2004; Engineering Conferences
International: Naples, Italy, 2004.
10. Schwartz, M.; Lee, J., Reactive cfd simulation of an fcc regenerator. Asia-
Pacific Journal of Chemical Engineering 2007, 2, 347-354.
11. Hoffman, A.; Arends, H.; Sie, H., An experimental investigation elucidating
the nature of the effect of solids loading on cyclone performance. Filtration
and Separation 1991, 28, 188-193.
12. Muschelknautz, E.; Brunner, K., Experiments with cyclones. Chemie
Ingenieur Technik 1967, 531.
13. Lewnard, J.; Herb, B.; Tsao, T.; Zenz, J. In Effect of design and operating
parameters on cyclone performance for circulating fluidized bed boilers,
Fourth International Conference on Circulating Fluidized Beds, 1993; 1993;
pp 636-641.
14. Pirker, S.; Kahrimanovic, D.; Aichinger, G., Modeling mass loading effects in
industrial cyclones by a combined eulerian-lagrangian approach. Acta
Mechanica 2009, 204, (3-4), 203-216.
15. Tuzla, K.; Chen, J., Performance of a cyclone under high solids loadings.
AIChE Symp. Ser. 1992, 289, 130-136.
16. Gray, M. R., Fundamentals of bitumen coking processes analogous to
granulations: A critical review. Canadian Journal of Chemical Engineering
2002, 80, (3), 393-401.
17. Briens, C.; McDougall, S.; Chan, E., On-line detection of bed fluidity in a
fluidized bed coker. Powder Technology 2003, 138, (2-3), 160-168.
18. Loezos, P. N.; Costamagna, P.; Sundaresan, S., The role of contact stresses
and wall friction on fluidization. Chemical Engineering Science 2002, 57, (24),
5123-5141.
19. Glasser, B. J.; Sundaresan, S.; Kevrekidis, I. G., From bubbles to clusters in
fluidized beds. Physical Review Letters 1998, 81, (9), 1849-1852.
20. Li, J.; Kuipers, J. A. M., Gas-particle interactions in dense gas-fluidized beds.
Chemical Engineering Science 2003, 58, (3-6), 711-718.
21. Wen, Y.; Yu, Y., Mechanics of fluidization. Chem. Eng. Prog. Symp. Ser.
1966, 62, 100.
16
22. Syamlal, M.; Rogers, W.; O'Brien, T., Mfix documentation and theory guide.
In 1993; Vol. DOE/METC-94/1004.
23. Heynderickx, G. J.; Das, A. K.; De Wilde, J.; Marin, G. B., Effect of clustering
on gas-solid drag in dilute two-phase flow. Industrial & Engineering Chemistry
Research 2004, 43, (16), 4635-4646.
24. McKeen, T.; Pugsley, T., Simulation and experimental validation of a freely
bubbling bed of fcc catalyst. Powder Technology 2003, 129, (1-3), 139-152.
25. Li, J. H.; Cheng, C. L.; Zhang, Z. D.; Yuan, J.; Nemet, A.; Fett, F. N., The
emms model - its application, development and updated concepts. Chemical
Engineering Science 1999, 54, (22), 5409-5425.
26. Igci, Y.; Andrews, A. T.; Sundaresan, S.; Pannala, S.; O'Brien, T., Filtered
two-fluid models for fluidized gas-particle suspensions. Aiche Journal 2008,
54, (6), 1431-1448.
27. Parmentier, J.; Simonin, O.; Delsart, O., A functional subgrid drift velocity
model for filtered drag prediction in dense fluidized bed. AIChE Journal 2011,
(accepted for publication).
28. Van der Hoef, M. A.; Beetstra, R.; Kuipers, J. A. M., Lattice-boltzmann
simulations of low-reynolds-number flow past mono- and bidisperse arrays of
spheres: Results for the permeability and drag force. Journal of Fluid
Mechanics 2005, 528, 233-254.
29. Glasser, B. J.; Kevrekidis, I. G.; Sundaresan, S., Fully developed travelling
wave solutions and bubble formation in fluidized beds. Journal of Fluid
Mechanics 1997, 334, 157-188.
30. Glasser, B. J.; Kevrekidis, I. G.; Sundaresan, S., One- and two-dimensional
travelling wave solutions in gas-fluidized beds. Journal of Fluid Mechanics
1996, 306, 183-221.
31. Dasgupta, S.; Jackson, R.; Sundaresan, S., Turbulent gas-particle flow in
vertical risers. Aiche Journal 1994, 40, (2), 215-228.
32. Gidaspow, D., Multiphase flow and fluidization: Continuum and kinetic theory
descriptions. Academic Press: Oxford, 1994.
33. Gidaspow, D.; Jiradilok, V., The multiphase approach to fluidization and
green energy technologies. Nova Science Publishers: New York, 2009.
34. Valiveti, P.; Koch, D. L., The inhomogeneous structure of a bidisperse
sedimenting gas-solid suspension. Physics of Fluids 1999, 11, (11), 3283-
3305.
35. Iddir, H.; Arastoopour, H., Modeling of multitype particle flow using the kinetic
theory approach. Aiche Journal 2005, 51, (6), 1620-1632.
36. Garzo, V.; Dufty, J. W.; Hrenya, C. M., Enskog theory for polydisperse
granular mixtures. I. Navier-stokes order transport. Physical Review E 2007,
76, (3), 27.
37. Garzo, V.; Hrenya, C. M.; Dufty, J. W., Enskog theory for polydisperse
granular mixtures. Ii. Sonine polynomial approximation. Physical Review E
2007, 76, (3), 20.
38. Holloway, W.; Benyahia, S.; Hrenya, C. M.; Sundaresan, S., Meso-scale
structures of bidisperse mixtures of particles fluidized by a gas. Chem. Eng.
Sci. 2011, (in revision).
39. Rao, K.; Nott, P., An introduction to granular flow. Cambridge University
Press: New York, 2008.
40. Jackson, R., Dynamics of fluidized particles. Cambridge University Press:
New York, 2000.
17
41. Johnson, P. C.; Nott, P.; Jackson, R., Frictional collisional equations of
motion for particulate flows and their application to chutes. Journal of Fluid
Mechanics 1990, 210, 501-535.
42. Fan, R.; Marchisio, D. L.; Fox, R. O., Application of the direct quadrature
method of moments to polydisperse gas-solid fluidized beds. Powder
Technology 2004, 139, (1), 7-20.
43. Fan, R.; Fox, R. O., Segregation in polydisperse fluidized beds: Validation of
a multi-fluid model. Chemical Engineering Science 2008, 63, (1), 272-285.
44. Andrews, M. J.; Orourke, P. J., The multiphase particle-in-cell (mp-pic)
method for dense particulate flows. International Journal of Multiphase Flow
1996, 22, (2), 379-402.
45. Patankar, N. A.; Joseph, D. D., Modeling and numerical simulation of
particulate flows by the eulerian-lagrangian approach. International Journal of
Multiphase Flow 2001, 27, (10), 1659-1684.
46. O'Rourke, P. J.; Snider, D. M., An improved collision damping time for mp-pic
calculations of dense particle flows with applications to polydisperse
sedimenting beds and colliding particle jets. Chemical Engineering Science
65, (22), 6014-6028.
47. Snider, D. M., Three fundamental granular flow experiments and cpfd
predictions. Powder Technology 2007, 176, (1), 36-46.
48. Snider, D. M., An incompressible three-dimensional multiphase particle-in-cell
model for dense particle flows. Journal of Computational Physics 2001, 170,
(2), 523-549.
49. O'Rourke, P. J.; Zhao, P.; Snider, D., A model for collisional exchange in
gas/liquid/solid fluidized beds. Chemical Engineering Science 2009, 64, (8),
1784-1797.
50. Benyahia, S.; Sundaresan, S., Do we need sub-grid scale corrections for both
continuum and discrete gas-particle flow models. Powder Technology 2010,
(under review).
51. Wirth, K., Axial pressure profile in circulating fluidized beds. Chemical
Engineering Technology 1988, 11, 11-17.
52. Wirth, K., Fluid mechanics of circulating fluidized beds. Chemical Engineering
Technology 1991, 14, 29-38.
53. Cleary, P. W., Industrial particle flow modelling using discrete element
method. Engineering Computations 2009, 26, (6), 698-743.
54. Tsuji, Y.; Tanaka, T.; Ishida, T., Lagrangian numerical-simulation of plug flow
of cohesionless particles in a horizontal pope. Powder Technology 1992, 71,
239-250.
55. Tsuji, Y.; Tanaka, T.; Ishida, T., Discrete particle simulation of 2-dimensional
fluidized bed. Powder Technology 1993, 77, 79-87.
56. Inc, I. I. Pfc3d 4.0.184.
57. Plimpton, S., Fast parallel algorithms for short-range molecular-dynamics.
Journal of Computational Physics 1995, 117, (1), 1-19.
58. Chu, K. W.; Wang, B.; Xu, D. L.; Chen, Y. X.; Yu, A. B., Cfd-dem simulation
of the gas-solid flow in a cyclone separator. Chemical Engineering Science
66, (5), 834-847.
59. Geng, Y. M.; Che, D. F., An extended dem-cfd model for char combustion in
a bubbling fluidized bed combustor of inert sand. Chemical Engineering
Science 66, (2), 207-219.
60. Nvidia Nvidia cuda programming guide, 2.3.1; nVIDIA Corporation Santa
Clara, California, U.S., 2009.
18
61. Radeke, C. A.; Glasser, B. J.; Khinast, J. G., Large-scale powder mixer
simulations using massively parallel gpu architectures. Chemical Engineering
Science 65, (24), 6435-6442.
62. Radeke, C.; Radl, S.; Khinast, J. G. In Granular flows - showing size effects
by using high-performance simulations on gpus, Melbourne, Australia, 2009,
CSIRO Australia: Melbourne, Australia.
63. Aarons, L. R.; Sun, J.; Sundaresan, S., Unsteady shear of dense assemblies
of cohesive granular materials under constant volume conditions. Industrial &
Engineering Chemistry Research 49, (11), 5153-5165.
64. Forterre, Y.; Pouliquen, O., Flows of dense granular media. Annual Review of
Fluid Mechanics 2008, 40, 1-24.
65. Aarons, L.; Sundaresan, S., Shear flow of assemblies of cohesive granular
materials under constant applied normal stress. Powder Technology 2008,
183, (3), 340-355.
66. Cundall, P. A.; Strack, O. D. L., Discrete numerical-model for granular
assemblies. Geotechnique 1979, 29, (1), 47-65.
67. Luding, S., Cohesive, frictional powders: Contact models for tension.
Granular Matter 2008, 10, (4), 235-246.
68. Campbell, C., Elastic granular flows of ellipsoidal particle Physics of Fluids
2011, 23, 013306.
69. Kodam, M.; Bharadwaj, R.; Curtis, J.; Hancock, B.; Wassgren, C., Cylindrical
object contact detection for use in discrete element method simulations, part
ii-experimental validation. Chemical Engineering Science 65, (22), 5863-
5871.
70. Kodam, M.; Bharadwaj, R.; Curtis, J.; Hancock, B.; Wassgren, C., Cylindrical
object contact detection for use in discrete element method simulations. Part i
- contact detection algorithms. Chemical Engineering Science 65, (22), 5852-
5862.
71. Liu, B. Q.; Zhang, X. H.; Wang, L. G.; Hong, H., Fluidization of non-spherical
particles: Sphericity, zingg factor and other fluidization parameters.
Particuology 2008, 6, (2), 125-129.
72. Hilton, J. E.; Mason, L. R.; Cleary, P. W., Dynamics of gas-solid fluidised
beds with non-spherical particle geometry. Chemical Engineering Science 65,
(5), 1584-1596.
73. Rosendahl, L.; Mando, M. In Status and challenges of modeling non-
spherical particle motion at high reynolds numbers, Halle, Germany, 2010,
12th ERCOFTAC Workshop on Two-Phase Flow Predictions Halle,
Germany.
74. Sakai, M.; Koshizuka, S., Large-scale discrete element modeling in
pneumatic conveying. Chemical Engineering Science 2009, 64, (3), 533-539.
75. Mokhtar, M.; Kuwagi, K.; Takami, T.; Hirano, H.; Horio, M., Validation of the
similar particle assembly (spa) model for the fluidization of geldart's group a
and d particles. AIChE Journal 2011, (accepted).
76. Bierwisch, C.; Kraft, T.; Riedel, H.; Moseler, M., Three-dimensional discrete
element models for the granular statics and dynamics of powders in cavity
filling. Journal of the Mechanics and Physics of Solids 2009, 57, (1), 10-31.
77. Radl, S.; Radeke, C.; Khinast, J.; Sundaresan, S. In 8th international
conference on cfd in oil & gas, metallurgical and process industries, Parcel-
Based Approach for the Simulation of Gas-Particle Flows, Trondheim,
Norway 2011, 2011; Trondheim, Norway 2011.
19
78. Benyahia, S.; Galvin, J. E., Estimation of numerical errors related to some
basic assumptions in discrete particle methods. Industrial & Engineering
Chemistry Research 49, (21), 10588-10605.
79. Simonin, O., Two-fluid model approach for turbulent reactive two-phase
flows. In Summer school on numerical modeling and prediction of dispersed
two-phase flows, Meserburg, Germany, 1995.
80. Lain, S.; Sommerfeld, M., Euler/lagrange computations of pneumatic
conveying in a horizontal channel with different wall roughness. Powder
Technology 2008, 184, 76-88.
81. Grace, J.; Taghipour, F., Verification and validation of cfd models and
dynamic similarity for fluidized beds. Powder Technology 2004, 139, 99-110.
82. Igci, Y.; Sundaresan, S., Verification of filtered two-fluid models for gas-
particle flows in risers. AIChE Journal 2011, (to appear).
83. Weber, S.; Briens, C.; Berruti, F.; Chan, E.; Gray, M., Stability of
agglomerates made from fluid coke at ambient temperature. Powder
Technology (accepted for publication)
84. Donahue, C. M.; Hrenya, C. M.; Davis, R. H., Stoke's cradle: Newton's cradle
with liquid coating. Physical Review Letters 105 (3), 034501-1-034501-4.
85. Kantak, A. A.; Hrenya, C. M.; Davis, R. H., Initial rates of aggregation for
dilute, granular flows of wet particles. Physics of Fluids 2009, 21, (2),
0233101.
20
ELECTROSTATIC PHENOMENA IN FLUIDIZATION SYSTEMS:
CURRENT STATUS OF UNDERSTANDING AND FUTURE
RESEARCH NEEDS
Xiaotao T. Bi
Fluidization Research Centre, Department of Chemical and Biological Engineering
The University of British Columbia, Vancouver, BC, Canada
ABSTRACT
Electrostatic charging of dielectric powders in gas-solids fluidized beds has received

increased attention in recent years, due to its impact on particle agglomeration,
dispersion and reactor fouling in polymerization and pharmaceutical processes, and
charging and coating uniformity in powder coating processes. This paper provides a
critical review on the measurement techniques for characterizing powder charging,
distribution of charged powders and the factors influencing the powder electrification
in gas-solids fluidization systems.
INTRODUCTION
The electrification phenomenon in fluidized beds was first observed in late 1950s,
and particle charging has been considered as one of the key factors causing particle
agglomeration and reactor wall fouling in gas-solids fluidized beds dealing with fine
dielectric powders [1]. Electrostatic forces induced by the charges carried by
particles can also change the hydrodynamics of gas-solid fluidized beds. Despite
these negative effects of electrostatic charging, the mechanisms of charge
generation and dissipation are still poorly understood because of the lack of accurate
measurement techniques for determining particle charge distributions inside the
fluidized beds and the lack of applicable theories for charge separation between
similar dielectric materials.
Due to the non-homogeneous flow structure in gas-solids fluidized beds, the electric
forces between adjacent particles cannot be considered as isotropic in the region
close to the gas bubbles. Similarly the electric field of the charged particle bed
cannot be treated as a homogeneous medium. Instead, heterogeneous flow
structure at the bubble scale has to be considered in order to properly characterize
the electrostatic forces and fields associated with charged particles.
The reactor performance is impacted by electrostatics as reflected by the particle

agglomeration, particle segregation, wall fouling and non-uniform temperature
distribution. A proper understanding of charge generation and dissipation
mechanisms at the particle scale or even the molecular scale coupled with the
distribution of charged particles at the bubble scale is required to properly predict the
impact of electrostatic charges on the reactor hydrodynamics and to develop
effective tools for mitigating electrostatic charges.
Electrostatic phenomena in industrial fluidized bed polymerization reactors and the

mitigation strategies were reviewed comprehensively by Hendrickson [1], while the
triboelectric charging of dielectric powders was recently reviewed by Matsusaka et
al. [2]. This paper attempts to provide a critical review on measurement techniques,
charge generation and spatial distribution in fluidized beds, and the factors
determining the degree of particle electrification in gas-solids fluidized beds.
MEASUREMENTS OF STATIC CHARGES IN FLUIDIZED BEDS
Various techniques have been used to quantify the electrification phenomenon and
to measure particle charge density in gas-solids flow systems. The most commonly
used method is to capture certain amount of charged particles into a Faraday cup so
that the charge density of particles (Q/m) can be obtained. Some methods measure
the current or the electric potential from the metal surface of an electrostatic probe
either in direct contact with the bed particles (ball probes, collision probes or
capacitance probes) or exposed to the electrical field induced by the pass-by
particles (induction probes). Particle charge density can also be deduced by
analyzing the trajectory of a charged particle subject to an electric or electromagnetic
field. Table 1 summarizes the techniques used to measure electrification in gas-
solids fluidized beds.
Direct Methods: Measurements of Charge Density by Faraday Cup and Particle

Trajectory Tracking
The sign and density of charges on each particle will provide crucial information on
the degree of particle charging and the magnitude of electrostatic forces acting on
individual particles. Charged particles in the fluidized bed can be removed by a
sampling tube or a scooper, then poured into a Faraday cage, as illustrated in Figure
1. Such a sampling method has been applied to measure the particle charge density
in the dense bed region [3, 4, 5, 6, 7] and the freeboard region [8] of bubbling/
slugging fluidized beds or CFB risers [9, 10]. Such a method can be made localized
by taking samples from different locations of the fluidized bed [5].
Since particles with size distributions have been commonly used in the fluidized bed,
it will be important to know the differential charging of particles of different sizes in
the bed. To determine the charge density on removed particle samples of different
sizes from the fluidized bed, multi-compartment Faraday cup systems were used
which separated particles of different charge densities into several Faraday cups
arranged either horizontally [11] or vertically [6], as shown in Figure 2.
Table 1. Electrostatics measurement techniques for gas-solids fluidized beds.
Researchers Bed Particles Probe Signal
Ciborowski and Wlodarski Bubbling Sand, polystyrol, Ball probe Potential
(1962) [12] vinyl polyacetate
Boland et al., (1969) [13]; Bubbling Glass beads Induction probe Potential
Boland and Geldart (1971)
[14]
Bafrnec and Bena (1971) Bubbling Glass beads Ball probe Potential
[15]
Tardos and Pfeffer (1980) Bubbling Porcelain Faraday cup; Q/m;
[3] Ball probe Current
Fasso et al. (1982) [8] Bubbling Glass beads Faraday cup Q/m
Wolny and Opalinski Bubbling Polystyrene Faraday cup Q/m
(1983) [16] (Single particle
sampling)
Fujino et al. (1985) [4] Bubbling Glass bead, Ball probe; Potential;
Neobead, PMMA Faraday cup Q/m
Gajewski (1985) [17] Bubbling Polyethylene Multi ring probes Current
Rojo et al. (1986) [18] Bubbling Glass bead Ball probe Potential
Wolny and Kazmierczak Bubbling Polystyrene Tracking of particle Q/m
(1989) [19] trajectory
Gidaspow et al. (1986) Bubbling Coal Ball probe Current
[25]
Guardiola et al. (1992; Bubbling Glass beads, Ball probe Potential
1996) [20,21] steel
Napier (1994) [22] Bubbling Glass beads, Ball probe; Q/m
sugar Field meter (No details)
Jiang et al. (1994) [9] Riser FCC, Faraday cup Q/m
Polyethylene
Coronella and Deng Riser Sand Electrostatic field Potential
(1997) [23] meter
Mountain et al. (2001) [24] Bubbling Polymers Faraday cup Q/m
Tucholski and Colver Riser Glass beads Faraday cup; Q/m
(1998) [10] Ball probe; Probe current;
Metal wall Wall current.
Ali et al. (1998; 1999) [11, Bubbling Polyamide Faraday cup Q/m
5]; Zhao et al. (2003) [6]
Servais and Bernot (2000) Bubbling Polyethylene Ball probe Potential
[26]
Park et al. (2002a, 2002b) Single Glass beads Ball probe Current
[27,28] bubble
Revel et al. (2003) [7] Slugging Polyethylene Faraday cup Q/m
Murtomaa et al. (2003) Bubbling Glass beads, Multi-scan Potential &
[29] lactose, cellulose Induction ring Q/m
probe
Yao et al. (2002) [30] Bubbling Glass beads Ball probe Current
Mehrani et al. (2005; Bubbling Glass beads, Faraday cup (in- Q/m
2007) [31, 32] Polyethylene situ)
Chen et al. (2006, 2007) Bubbling Glass beads Multi induction Current & Q/m
[33, 34, 35] probes distribution
Demirbas et al. (2008) Bubbling Glass beads Multi Induction Charge
[36] probes
Wang et al. (2008) [37] Bubbling Polyethylene Multi ball probes Potential
Moughrabiah et al. (2009) Bubbling Polyethylene, Multi ball probes Current
[38]; Liu et al. (2010) [39] (P, T) glass beads distribution
Sowinski et al. (2009, Bubbling Polyethylene Faraday cup Q/m
2010) [40, 41]
Omar et al. (2010) [42] Bubbling Polyethylene Faraday cup (in- Transient Q/m
situ)
Powder in
FB
Faraday Cup
Grounded Cup
Electrometer
Faraday cup
+ + ++
Electrometer + ++++
Insulation
Figure 1. Schematic of a Faraday cup charge density measurement system.
Fluidized bed
Plug
Powders
Metal sampling
tube 1
2
3
4
Vertical array of
Faraday cup sensors 5
6
7
(a) (b)
Figure 2. (a) Horizontal and (b) vertical multi-compartment Faraday cups [6, 11].
The charge density of individual particles in the fluidized bed can also be measured
using the single particle sampling method [16] or the single particle trajectory method
[19]. For single particle sampling, a small vacuum sampling tube (0.5 mm in
diameter) is inserted into the bed to remove single polystyrene particles (~ 1 mm in
diameter) into a Faraday cup so that the charge density of individual particles can be
directly obtained. The particle trajectory method is a non-contact measurement
method by which two parallel metal plates are installed in the freeboard region of a
transparent fluidized bed. When single particles are ejected into the space between
the parallel plate by a single gas nozzle located inside the dense bed right beneath
the space of the parallel plates, the trajectory of single particle movement was
captured by a high speed video camera which enabled the determination of the
charge density of individual particles by analyzing the trajectory of the particles
subjected to an electrical field. The accuracy of this method will be impacted by the
interference of the electric field imposed by the charged column walls and the bed
particles unless the space between the parallel plates are well isolated.
The Faraday cup method can provide the charge density directly, but the
measurement accuracy is affected by the additional charging or discharging of
samples during the sampling process due to the contact of sampled powders with
the sampling tube or device. A novel in-situ Faraday cup fluidized bed method was
developed by Mehrani et al., [31, 32] to measure the charge density of entrained fine
powders from an electrically isolated copper fluidized bed, which serves as a
Faraday cup. As shown in Figure 3, when charged fine particles are elutriated from
the fluidized, an equal but opposite charge will be registered by the electrometer
connected to the isolated copper fluidized bed. To monitor the change of charge
density of entrained fine powders with time, the entrained particles can be captured
into a bag filter and weighed by a sensitive balance so that the transient charge
density of the entrained fines can be obtained [42]. On the other hand, improvement
has been made in minimizing the additional electric charging by discharging bed
materials directly into a Faraday cup installed beneath a fluidized bed using a quick-
open distributor for the measurement of the average charge density of bed materials
at the end of each fluidization test [40, 41], as shown in Figure 4.
C o pp e r p ip e
G a s o ut
C op p er c yc lon e
T ef lo n
P le x ig las s
s ea le d c ha m b er
Fine s
In n er c o pp e r c olle c te d
c olum n In a c up
S ca le
O u ter c op p er
c olum n
D at a ac qu is itio n
E le ct ro m et e r by c om pu te r
T ef lo n
F lu id iz a tio n g a s
Figure 3. A Faraday cup fluidized bed unit for transient charge measurement of
entrained fines [31, 42].
Figure 4. A novel fluidized bed unit with a quick-opening distributor for measurement
of powder charging [40, 41].
Indirect Methods: Measurements of Current and Voltage Potential by

Electrostatic Probes
When particles in the fluidized bed are charged, no matter whether the reactor wall is
grounded or not, an electric field will be created in the fluidized bed. By placing a
metal probe inside the fluidized bed with the probe connected to an electrometer, a
potential against a grounded reference probe (either the reactor wall, the metal
distributor or another metal probe) will be registered by the electrometer, as
illustrated in Figure 5. The magnitude of the potential against a grounded metal wall
or distributor generally increases with fluidization time, and reached a final steady
state value, Vs, after a few minutes to an hour, see Figure 5. The final potential is
thus believed to reflect the degree of electrification of fluidized particles at steady
state when the equilibrium between charging and discharging is reached.
An equivalent electric circuit could be used to relate the final potential to the charge
behaviour in the fluidized bed [4]. As illustrated in Figure 5 the charged bed particles
can be treated as a condenser which captures charges generated in the fluidized
bed. The total electrical resistivity of the whole system consists of three parts: bed
resistivity accounting for current flow from the bed to the probe, the leakage
resistance from the reactor wall and the internal resistance of the electrometer. The
final potential is thus related to the resistances by:
I 0 Rbed Rwall Rm
Vs  I 0 Rt 
Rbed Rwall  Rbed Rm  Rwall Rm
The final potential between the probe and the grounded metal distributor can also be
analyzed using a capacitance model, with the final potential being related to the
charge in the capacitor by,
4H
Vs  Q
 f Dc D p
where H is the vertical distance between the probe and the distributor, Dc is the
diameter of the distributor and Dp is the diameter of the electrostatic probe. The final
potential is then seen to be influenced by the dielectric properties of the bed
particles, which depend on the bed voidage, relative humidity etc.
Im
Q/m E Rbed C Rwall Rm
FB
V  V s (1  e  t /  )
Potential
Electrometer
Vs
Potential probe
Time
Figure 5. A typical electrostatic potential probe, its equivalent circuit and measured
signals.
The other type of electrostatic probes is the collision type current probes, or so-
called ball probes. The probe is installed in the fluidized bed and connected to a
resistor, with the current measured by an electrometer, see Figure 6. Different from
the potential probe which treats the fluidized bed as a charged continuum medium,
the current ball probe receives charges both transferred from particles colliding with
the probe surface and induced when the particles pass by the probe [3, 27]. For a
single bubble passing a current probe in a two-dimensional fluidized bed, Park et al.
[27] and Chen et al. [43] proposed a combined charge transfer and induction model
to interpret the recorded transient current signal. The net current change is related to
the charge transfer from particle-probe collisions while the fluctuations are induced
by the passing bubble. Chen et al. [44] further demonstrated that the charge density
of the particles in the dense phase surrounding the bubble could be obtained by
fitting the model to the measured current signals from a single bubble, for given
particle electrical properties and a uniformly charged dense phase.
To eliminate probe interference with the motion in the bed and charge transfer due to
collisions between particles and the probe, shielded induction probes have also been
used to characterize the electrification of fluidized beds. Boland and Geldart [14]
embedded an induction probe onto the Plexiglas wall of a 2-D column, and
registered the dynamic response of the probe to the passage of a single injected gas
bubble into a fluidized bed of glass ballotini particles. They speculated for the first
time that the static electrification is generated by the motion of particles around the
gas bubble, particularly in the region of the wake. Single or double ring induction
probes have been commonly used to measure particle velocities in pneumatic
conveying lines based on probe calibration and cross-correlation of signals from two
rings separated by a given distance [45-47] by assuming a uniform particle flow in
the pneumatic conveying lines.
Figure 6. A typical collision current probe installed in a 2-D column [27].
Chen et al. [33-35] used multi-induction probes aligned horizontally to measure the
charge distribution around rising gas bubbles in a two-dimensional Plexiglas column.
Using four induction probes placed flush with the outer surface of the column,
signals received from the four probes are shown in Figure 7(a), and used in
conjunction with the bubble position captured by a synchronized digital camera to
reconstruct the charge density distribution around rising gas bubbles in gas-solids
fluidized beds. Figure 7(b) shows the reconstruction results for the induced charges
shown in Figure 7(a). It can be seen that the charge inside the air bubble is almost
zero, and the charge density increases gradually toward the dense phase region
outside the bubble, with the sign of charges in the dense phase remote from the
bubble being negative. There is a more negatively charged wake, confirming the
postulation based on measurements with a single collision probe [23, 43, 44]. The
charge density outside the bubble in the dense phase was approximately –3.6x10-7
C/kg and the charge in the wake was about–6.8 x10-7 C/kg.
Murtomaa et al. [29] used a multi-scan induction ring probe to measure the induced
potential at different bed height by moving the ring probe vertically. The average
particle charge density of the bed under steady state was obtained by signal
reconstruction, with the assumption of a uniform charge density on homogeneously
distributed particles. As will be discussed later, the non-uniform charge density
distribution in the fluidized bed will make this technique difficult to be used for
fluidized beds without a priori charge distribution information.
The disadvantage of induction probes is that the signals received by those probes
can be interfered by electric fields induced by charged column walls, especially for
non-conductive walls such as Plexiglas.
1200 inside bubble
1000
Induced charge, pC
800
600
probe 4
400
line: measured
200 probe 1 scatter: reconstructed
0
probe 2 probe 3
100 50 0 -50 -100
Distance from the center of the bubble, mm
(a)
80 3
charge density, pC/mm
60 -2.0
-1.7
40
-1.5
20
bubble -1.2
-0.90
probe 1 probe 2 probe 3 probe 4
-0.63
z, mm
0
-0.35
-0.075
-20
0
-40
-60
-80
0 10 20 30 40
x, mm
(b)
Figure 7. (a) Measured induced charge signals and simulated induced charge
signals based on reconstructed charge distribution and (b) reconstructed charge
distributions (Hmf = 0.7 m, DB=0.08 m, UB=0.45 m/s, dp=565 μm, ρp=2500 kg/m3,
Qair=1.78 m3/s ) [34].
CHARGE GENERATION AND DISTRIBUTION IN FLUIDIZED BEDS
Charge Generation and Bipolar Charging
Tribo-electrification between dissimilar materials can be characterized by the surface

work function, defined as the work/energy needed to pull an electron away from the
surface of a material. In general, metal has a lower work function, thus easier to loss
electrons when contact with other materials. Work function also closely correlates
with the dielectric constant of the material, higher for materials with a higher
dielectric constant. When two dissimilar materials are in contact, electrons will flow
from the surface of lower work function to that of a higher work function. Thus, in
contact with a neutral metal surface, a neutral dielectric particle will extract electrons
from the metal surface. On separation, the dielectric particle becomes negatively
charged. When a charged particle contacts with a metal surface, however, the net
charge exchange will depend on the pre-charge level, collision speed and the
collision angle etc. As reviewed in Matsusaka et al. [2], extensive work has been
reported on the effect of particle pre-charge level, surface pre-charge level, collision
angle and collision speed on the degree of charge transfer and separation. The
charge generated by colliding a dielectric particle with a metal surface generally
increases with the collision speed and is at the maximum for a head-on collision with
the surface. In fluidized beds of dielectric particles, particles are expected to be
charged via collision with the reactor walls, either grounded metal wall or poorly
conductive plastic walls.
Most studies on electrostatic charging of fluidized beds assumed a single polarity of

bed materials before 1990s, although bipolar charging was identified as early as in
1950 [48, 49]. Based on the measurement of the charge density of individual
particles, it was found that for glass beads of narrow size distributions, particles are
approximately evenly divided between positively and negatively charged although
the net charge is close to zero. Charging particles through a vibrating chute and then
falling them through air between parallel vertical electrode plates to separate
particles into eight groups using 8 Faraday pales aligned horizontally beneath the
electrode plates with each unit connected to an electrometer, Turner and
Balasubramanian [49] confirmed that both positive and negative charges could arise
on particle surfaces for three narrowly sized glass bead samples, 45-53 m, 63-75
m and 75-90 m. Cartwright et al. [50] tested polyethylene (PE) powders in a
pneumatic conveying system and showed that fine PE powders were charged
negatively and coarse powders charged positively. Similar to the tests of Turner and
Balasubramanian [49], the ratio of the positively and negatively charged powders
strongly depended on the relative humidity, suggesting that the moisture on the
particle surface might play an important role during the charging process. Similar
bipolar charging phenomenon was also reported by Singh and Hearn [51] and
Mazumder et al. [52, 53] for PVC and tonner powders based on the measured
charges on individual particles in samples of size distributions using a microprobe
system and an electric single particle aerodynamic relaxation time (E-SPART)
analyzer, respectively.
The first direct evidence of bipolar charging in fluidized beds was given in the paper
by Wolny and Kazmierczak [19] who measured the charge density of individual
particles using a particle trajectory tracking technique installed in the freeboard of the
fluidized bed and reported a probability distribution of charge density, although his
results were not noticed until now.
Ali et al. [11] used a horizontal array Faraday cup system (see Figure 2) to measure
the charge density of particles charged differently whereby a small sample of
charged powders removed from a fluidized bed by a scooper was poured from a
height and separation occurred between the majority and the minority particles of
opposite charges. The degree of separation is a function of charges on the individual
particles and the height at which the sample is poured. Bipolar charging of the fine
and coarse fluidized particles was identified in which the fine particles are charged
negatively, while coarse particles are charged positively for two polymer samples
tested, while the third polymer sample showed the opposite charge signs. Further
tests by Zhao et al. [6] using a vertical array Faraday cup system confirmed the
bipolar charging behaviour for three polymer powders, all showing negatively
charged fines. Mehrani et al. [32] measured the charge density of fines entrained
from a copper fluidized bed of glass beads and polyethylene powders. Bipolar
charging was identified with fines charged positively for all glass beads samples, but
negatively charged fines for polyethylene resin powders at both zero and 60%
relative humidity. Further study of Omar et al. [42] using polyethylene resins of
different grades from different manufacturers showed consistent results of negatively
charged fines. The addition of different fines to the polyethylene powder [32] also
showed a strong dependence of the charge level and signs on the relative humidity
of the fluidizing gas. The fine Larostat 519 powder was negatively charged at dry
nitrogen, but positively charged at 60% relative humidity. The opposite signs reversal
phenomenon was observed for fine catalyst powder and silver-coated glass beads.
The identification and confirmation of bipolar charging changed the perception of a

uniformly charged fluidized bed of particles of singular polarity, and thus opened the
door for examining the charge distribution inside the fluidized beds.
Charge Distribution
Ali et al. [5] studied the charge distribution in fluidized beds of polymer powders with
the samples removed from different locations of the fluidized bed by a scooper and
poured into a Faraday cup. Their results showed that the charge density inside the
bed was quite uniform, except in the near wall region where some fine powders
deposited onto the walls. The wall deposit was further analyzed on its mean size
and the charge density. It was found that the wall deposit was positively charged in
the dense bed region, with the charge density increased with increasing the distance
from the distributor [Figure 8(a)]. Above the bed surface, however, the deposit
reversed the polarity to negative. In the region where the charge density crosses
zero, there was no deposit on the wall. The maximum charge density of the deposit
somehow corresponded to the maximum field potential for a uniformly charged bed
[Figure 8(b)]. Also, the mean particle size in the deposit of the dense bed was
generally larger than that in the freeboard region [Figure 8(c)].
Recently, Sowinski et al. [40, 41] carried out similar tests in a novel fluidized bed unit
in which the entrained fine powders were captured into a Faraday cup to have the
charge density measured, and the charge density of the bed material, polyethylene
powders, was measured by dropping the bed particles into a Faraday cup located
beneath the gas distributor right after the fluidizing gas was cut off. The fine powders
deposited on the column wall was visually inspected and sampled to have the
charge density and the particle size distribution determined. Their results showed
that the entrained fines were highly positively charged, while the bed materials were
negatively charged. The particles deposited on the wall were overall highly
negatively charged, with most deposit residing in the dense bed region, and minor
deposit above the bed surface. Again there was a clean wall region between the
dense bed and the freeboard region. Their results are in general consistent with Ali
et al. [5], although the deposits at different region were not examined.
Figure 8. Axial distribution of (a) charge density of wall deposit, (b) field intensity of
charged bed and (c) volume mean particle size of wall deposit. [5].
Gajewski [17] measured the axial profiles of the average electrostatic current from
multiple isolated copper rings embedded inside a glass fluidized bed with
polypropylene powders as the bed material. Positive current was measured in the
bottom dense bed region, and negative current was found in the upper bed and
freeboard region, showing a reversal of current flow in the system. Moughrabiah et
al. [38] and Liu et al. [39] also measured the axial distribution of electrostatic current
from 8 ball probes located at both the axis and near the wall of the fluidized bed
using polyethylene powders. The average currents from those probes were found to
be always negative in the lower dense bed region, and positive in the upper and the
freeboard region, confirming the current sign reversal phenomenon in the bed.
Rojo et al. [18], Servais and Bernot [26] and Wang et al. [37] measured the axial
distribution of electrical potentials using potential probes immersed in the fluidized
bed. Wang et al. [37] showed that negative potentials always presented in the lower
dense bed region, and positive potentials in the upper bed and freeboard region,
appearing to be consistent with the reported current distribution.
The new experimental evidence on non-uniform distribution of bipolarly charged

powders inside the fluidized beds and the likely induction charging of bed particles
from the highly charged wall deposit [5] revealed the complexity of the particle
charging and accumulation mechanisms in the fluidized bed. All bulk measurement
techniques relying on the assumption of uniform spatial charge distribution would not
be able to capture the local characteristics of the charging phenomenon. Localized
measurements using sampling tubes in conjunction with cascaded Faraday cups or
small current probes and localized current induction tomography in combination with
advanced signal analysis and reconstruction methods may provide the opportunity to
improve our understanding of local charging behaviour of fluidized beds.
FACTORS INFLUENCING POWDER CHARGING
Tardos and Pfeffer [3] and Fujino et al. [4] found that the particle charge density was
not sensitive to the superficial gas velocity. Revel et al. [7], however, showed that
the charge density increased with increasing the superficial gas velocity using
polyethylene powders. Note that all those tests were conducted in bubbling fluidized
beds. In circulating fluidized risers, both Jiang et al. [9] and Tucholski and Colver [10]
showed that the particle charge density was insensitive to the solids circulation rate
and the superficial gas velocity. One likely explanation is that the increase in gas
velocity and particle circulation rate promotes both charge generation and dissipation
via particle-wall collisions, with the net change remaining unchanged.
Fujino et al. [4] showed that the relative humidity has little impact on the particle
charge density in bubbling fluidized beds. Tardos and Pfeffer [3] showed that the
charge density in the bed with a humid gas (RH=36-42%) was almost 50% lower
than that at lower humidity (RH=21-25%). Wolny and Kazmierczak [19] also showed
that the charge density of a 0.475 mm diameter polystyrene bubbling bed decreased
substantially when the relative humidity increased from 30% to 70%. In a charge
dissipation test carried out in a packed bed separately, they also demonstrated that
the charge dissipation rate at 70% relative humidity was much higher than at 30%
relative humidity. The increase in relative humidity was also found to be effective in
reducing the particle charge density in circulating fluidized risers [9]. It is also noted
that the reduction in average current and final potential measured by static probes
has been reported in all tests in the literature, supporting the effectiveness of relative
humidity in lowering the particle charge density. In general, such a reduction in bed
charge level at high humidities can be attributed to the increased surface
conductivity of moisture-coated particles [13]. Also, the increase in the humidity of
the fluidizing gas may also lower the resistivity and the break-down potential of the
gases, helping the dissipation of particle surface charges.
Antistatic agents have been used in the industry for powder charge mitigation. Wolny
and Opalinski [16] reported that the addition of 0.1% fine powders of either
conductive (active coal and TiO2) or insulating materials (pigment A-extra) was
effective in reducing the buildup of particle charge density in a fluidized bed of ~1
mm polystyrene particles. Wolny and Kazmierczak [19] later reported that the
addition of fine aluminium and NaCl powders to a bubbling fluidized bed of
polystyrene beads significantly reduced the charge density. It was also observed that
all NaCl particles in the bed were negatively charged and that all polystyrene
particles were coated with NaCl fines. The effectiveness of fine powders, no matter
conductive or not, has also been reported in many studies based on reduced current
and potential from electrostatic probes [15, 20, 28].
Servais and Bernot [26] examined the effect of antistatic powders (Larostat 519) on
both the axial and radial electrical potential profiles in a fluidized bed of polyethylene
and polypropylene powders using a potential probe. The results showed that both
the axial and radial electric potential profiles were significantly modified in the
presence of antistatic powders. The signs of the potential could even be flipped with
the addition of antistatic powders. They also showed that the potential increased
with increasing the fines content in polyethylene samples, inferring that higher
charges were generated for powders containing more fines, as evidenced by more
fines sticking to the column wall. Their results suggest that the addition of fine
powders may not only change the bed particle charge density but also altered the
spatial distributions of bipolarly changed particles in the fluidized bed.
One possible explanation is the lubrication of the fine powders as “spacers” attached
to bed particles so that charge dissipation by particle-to-particle contact is enhanced
due to the increased particle contacts. The difference between antistatic powders
and fine powders is still unclear and requires further investigation in the future.
Particle size distribution may also influence the electrostatic behaviour of powders
because of the bipolar charging between fine and coarse particles and the effect of
the addition of fines on the reduction of charge buildup. The implication is that a
proper design of particle size and size distribution may potentially reduce
electrostatic charge generation and build-up in fluidized beds.
FUTURE RESEARCH NEEDS
Understanding the impact of electrostatic charging of particles on gas-solids fluidized

bed reactor performances related to particle agglomeration and reactor fouling
requires the exploration of electrostatic charge generation and dissipation
mechanisms and segregation patterns of charged particles, which, in turn, relies on
the development of reliable and accurate measurement techniques. Advanced
techniques which can provide transient local particle charge density as well as
charge density distribution across a spectrum of particle sizes of the fluidized
particles will enable researchers to improve the understanding of the bipolar
charging behaviour and segregation of particles of different sizes and charge
polarities in the fluidized bed. Resolution of charged particle distribution surrounding
gas bubbles in the bubbling beds and particle clusters or particle streamers in the
annulus region of risers may provide key information for unlocking particle charging
and segregation mechanisms in fluidization systems.
ACKNOWLEDGEMENT
I am grateful to final supports from NSERC, Mitsubishi Chemicals, Japan Polychem,

Nova Chemicals, Chevron-Philip Chemicals and contributions from John Grace,
Alissa Park, Poupak Mehrani, Li Yao, Aihua Chen, Flip van Willigen, Kwang-Seok
Choi, Wajeeh Moughrabiah, Zhengliang Liu, Amy Yang and Muammar Omar.
NOTATION
DB = bubble diameter, m Dc = diameter of gas distributor, m

Dp = diameter of electrostatic probe, m dp = mean particle diameter, μm
H = vertical distance between probe and distributor, m
Hmf = packed bed height, m I = electric current, A
m = particle mass, kg Q = electrostatic charges, C
Q/m = particle charge density, C/kg Qair = fluidizing air flow rate, m3/s
RH = relative humidity of gases Rbed = Electric resistance of bed, 
Rm = External electric resistance,  Rwall = Electric resistance of wall, 
UB = bubble rise velocity, m V = voltage potential, V
Vs = steady state voltage potential, V X = horizontal coordinate, m
z = vertical coordinate, m f = dielectric constant
ρp = particle density, kg/m3
REFERENCES
1. Hendrickson, G., Electrostatics and gas phase fluidized bed polymerization

reactor wall sheeting, Chem. Eng. Sci., 61, 1041 – 1064, 2006.
2. Matsusaka, S., H. Maruyama, T. Matsuyama and M. Ghadiri, Triboelectric
charging of powders: A review. Chem. Eng. Sci., 65, 5781–5807, 2010.
3. Tardos, G., and R. Pfeffer, A method to measure electrostatic charge on a
granule in a fluidized bed. Chem. Eng. Comm., 4, 665-671, 1980.
4. Fujino, M., S. Ogata and H. Shinohara, The electric potential distribution profile in
a naturally charged fluidized bed and its effects. Int. Chem. Eng., 25(1), 149-159,
1985.
5. Ali, F.S., I.I. Inculet and A. Tedoldi, Charging of polymer powder inside a metallic
fluidized bed. J. Electrostatics, 45, 199-211, 1999.
6. Zhao, H., G.S.P. Castle, I.I. Inculet, and A.G. Bailey (2003). Bipolar charging of
poly-disperse polymer powders in fluidized beds. IEEE Transactions Industry
Applications, 39, 612-618.
7. Revel, J., C. Gatumela, J.A. Dodds and J. Taillet, Generation of static electricity
during fluidisation of polyethylene and its elimination by air ionisation. Powder
Technol., 135– 136, 192– 200, 2003.
8. Fasso, L., B.T. Chao and S.L. Soo, Measurement of electrostatic charges and
concentration of particles in the freeboard of a fluidized bed. Powder Technol.,
33, 211-221, 1982.
9. Jiang, P.J., J.P. Zhang and L.S. Fan, Electrostatic charge effects on the local
solids distribution in the upper dilute region of circulating fluidized beds, CFB??
10. Tucholski, D. and G.M. Colver, Charging of glass powder in a circulating fluidized
bed, IEEE Trans. Ind. Applica. 1906-1912,1998.
11. Ali, F.S., M.A. Ali, R.A. Ali and I.I. Inculet, Minority charge separation in falling
particles with bipolar charge. J. Electrostatics, 45, 139-155, 1998.
12. Ciborowski, J. and A. Vlodarski, On electrostatic effects in fluidized beds. Chem.
Eng. Sci., 17, 23-32, 1962.
13. Boland, D., Q.A.W. Al-Salim and D. Geldart, Static electrification in fluidised
beds, Chem. Eng. Sci., 24, 1389-1390, 1969.
14. Boland, D. and D. Geldart. Electrostatic charging in gas fluidized beds. Powder
Technol., 5, 289-297, 1971/2.
15. Bafrnec, M. and J. Bena, Quantitative data on the lowering of electrostatic
charge in a fluidized bed. Chem. Eng. Sci., 27, 1177-1181, 1972.
16. Wolny, A. and L. Opalinski, Electric charge neutralization by addition of fines to a
fluidized bed composed of coarse dielectric particles. J. Electrostatics, 14, 279-
289, 1983.
17. Gajewski, A., Investigation of the electrification of polypropylene particles during
the fluidization process. J. Electrostatics, 17, 289–298, 1985.
18. Rojo, V., J. Guardiola and A. Vian, A capacitor model to interpret the electric
behaviour of fluidized beds. Influence of apparatus geometry. Chem. Eng. Sci.,
41, 2171-2181, 1986.
19. Wolny, A. and W. Kazmierczak, Triboelectrification in fluidized bed of
polystyrene. Chem. Eng. Sci., 44, 2607-2610, 1989.
20. Guardiola, J., G. Ramos and A. Romero, Electrostatic behaviour in binary
dielectric/conductor fluidized beds. Powder Technol., 73, 11-19, 1992.
21. Guardiola, J., V. Rojo and G. Ramos, Influence of particle size, fluidization
velocity and relative humidity on fluidized bed electrostatics. J. Electrostatics, 37,
1-20, 1996.
22. Napier, D.H., Generation of static electricity in a fluidized bed and in powder
conveying. Proc. 2nd World Congress Particle Technology, 1994.
23. Coronella, C.J. and J.X. Deng, Electrostatic effects in cold-model circulating
fluidized beds, 1997.
24. Mountain, J.R., M.K. Mazumder, R.A. Sims, D.L. Wankum, T. Chasser and P.H.
Pettit, Triboelectric charging of polymer powders in fluidization and transport
processes, IEEE Transactions on Industry Applications, 37(3), 778-784, 2001.
25. Gidaspow, D., D. Wasan, S. Saxena, Y.T. Shih, R. Gupta, A. Mukherjee,
Electrostatic desulfurization of coal in fluidized beds and conveyors, AIChE
Symp. Ser. 83 (255), 74–85, 1986.
26. Servais, T. and C. Bernot, Measurement of electrostatic effects in a fluidized bed
reactor. First European Conference on the Reaction Engineering of Polyolefins,
Lyons, July 3–6, 2000.
27. Park, A., H.T. Bi, J.R. Grace and A.H. Chen, “Modeling electrostatic charge
transfer in gas-solids fluidized beds,” J. Electrostatics, 55, 135-168, 2002a.
28. Park, A., H.T. Bi and J.R. Grace, “Reduction of electrostatic charges in fluidized
beds,” Chem. Eng. Sci., 57, 153-162, 2002b.
29. Murtomaa, M., E. Räsänen, J. Rantanen, A. Bailey, E. Laine, J. Mannermaa, J.
Yliruusi, Electrostatic measurements on a miniaturized fluidized bed, J.
Electrostatics. 57, 91-106, 2003.
30. Yao, L., H.T. Bi and A.H. Park, “Electrostatic charges in freely bubbling fluidized
beds with dielectric particles,” J. of Electrostatics, 56, 183-197, 2002.
31. Mehrani, P., H.T. Bi, and J.R. Grace (2005). Electrostatic charge generation in
gas-solid fluidized beds. J. Electrostatics., 63, 165-173.
32. Mehrani, P., X.T. Bi and J.R. Grace, Electrostatic behavior of different fines
added to a Faraday cup fluidized bed, J. Electrostatics, 65, 1–10, 2007.
33. Chen, A.H., H.T. Bi and J.R. Grace, Effects of Probe Numbers and Arrangement
on the Measurement of Charge Distributions around a Rising Bubble in a Two-
Dimensional Fluidized Bed, Chem. Eng. Sci., 61, 6499-6510, 2006a.
34. Chen, A.H., F. Kleijn van Willigen, H.T. Bi, J.R. Grace, R. van Ommen,
Measurement of charge distribution around a single rising bubble in a two-
dimensional fluidized bed, AIChE J., 52, 174-184, 2006b.
35. Chen, A.H., H.T. Bi and J.R. Grace, Charge distribution around a rising bubble in
a two-dimensional fluidized bed by signal reconstruction, Powder Technology,
177, 113-124, 2007.
36. Demirbas, B., J. Nijenhuis, C.U. Yurteri and J.R. van Ommen, Towards
Monitoring Electrostatics in Gas–Solid Fluidized Beds, Can. J. Chem. Eng., 86,
493-505, 2008.
37. Wang, F., J.D. Wang and Y.R. Yang, Distribution of Electrostatic Potential in a
Gas-Solid Fluidized Bed and Measurement of Bed Level. Ind. Eng. Chem. Res.,
47, 9517–9526, 2008.
38. Moughrabiah, W., J.R. Grace and X.T. Bi, Effect of pressure and temperature on
electrostatics in fluid beds of PE particles, Ind. & Eng. Chem., 48, 320-325, 2009.
39. Liu, Z.L., X.T. Bi, J.R. Grace, Electrostatic charging behaviour of dielectric
particles in a pressurized gas-solid fluidized bed. J. Electrostatics, 68, 321-327,
2010.
40. Sowinski, A., Salama, F., Merhani, P., New technique for electrostatic charge
measurement in gas–solid fluidized beds. Journal of Electrostatics 67, 568–573,
2009.
41. Sowinski, A., L. Miller, P. Mehrani, Investigation of electrostatic charge
distribution in gas–solid fluidized beds. Chem. Eng. Sci., 65, 2771–2781, 2010.
42. Omar, M., K.C. Choi, X.T. Bi, J.R. Grace, Effect of particle size and residence
time on charging behaviour of fine polymer powders in fluidized beds.
Fluidization XIII, Korea, 2010.
43. Chen, A.H., H.T. Bi and J.R. Grace, “Effect of charge distribution around bubbles
on charge induction and transfer to a ball probe in gas-solid fluidized beds,” J. of
Electrostatics, 58, 91-115, 2003a.
44. Chen, A.H., H.T. Bi and J.R. Grace, “Specific charges of particles in fluidized
beds,” Powder Technology, 133, 237-276, 2003b.
45. Yan, Y., B. Byrne, S. Woodhead and J. Coulthard, Velocity measurement of
pneumatically conveyed solids using electrodynamic sensors. Meas. Sci.
Technol., 6, 515-537, 1995.
46. Ma, J. and Y. Yan, Design and evaluation of electrostatic sensors for the
measurement of velocity of pneumatically conveyed solids. Flow Measurement
and Instrumentation. 11, 195-204, 2000.
47. Armour-Chelu, D.I. and S.R. Woodhead, Comparison of the electric charging
properties of particulate materials in gas-solids flows in pipelines. J.
Electrostatics, 56, 87-101, 2002.
48. Kunkel, W.B., The static electrification of dust particles on dispersion into a
cloud. J. Appl. Phys., 21, 820-832, 1950.
49. Turner, G.A. and M. Balasubramanian, The frequency distribution of electrical
charges on glass beads, J. Electrostatics, 2, 85-89, 1976.
50. Cartwright, P., S. Singh, A.G. Bailey and L.J. Rose, Electrostatic charging
characteristics of polyethylene powder during pneumatic conveying. IEEE Trans.
Industry Applicat., IA-21 (2), 541-546, 1985.
51. Singh, S. and G.L. Hearn, Development and application of an electrostatic
microprobe. J. Electrostatics, 16, 353-361, 1985.
52. Mazumder, M.K., R.E. Ware, T. Yokoyama, B.J. Rubin and D. Kamp,
Measurement of particle and electrostatic charge distributions on tonners using
E-SPART analyzer, IEEE Trans. Industry Applicat., 27(4), 611-619, 1991.
53. Mazumder, M.K., S. Banerjee, R.E.Ware, C. Mu, N. Kaya and C.C. Huang,
Characterization of tribocharging properties of powder paint, IEEE Trans.
Industry Applicant, 30(2), 365-369, 1994.
EVOLUTION OF FCC – PAST PRESENT AND FUTURE – AND
THE CHALLENGES OF OPERATING A HIGH-TEMPERATURE
CFB SYSTEM
Ye-Mon Chen
Shell Global Solutions (US) Inc.
ABSTRACT
The fluid catalytic cracking (FCC) process is one of the most important circulating
fluidized bed processes. Although the FCC process has been in commercial operation
for over 60 years, the technology continues to evolve in order to meet new challenges,
which include processing more difficult feedstock and meeting more stringent
environmental regulations. This paper presents selected snap-shots of a few challenges
(high temperature erosion, corrosion and emission control) that the FCC process faces
today and the new challenges yet to come in the near future.
INTRODUCTION
The fluid catalytic cracking (FCC) process is one of the most important circulating
fluidized bed processes, with more than 400 units in operation worldwide today. The
FCC unit is the primary conversion unit in a refinery, which converts, or cracks, low value
heavy ends of crude oil into a variety of higher-value, light products, such as gasoline
and LPG. The unit consists of a reactor and a regenerator, as shown in Figure 1.
Figure 1: A typical FCCU configuration
Historically, the FCC unit and its downstream units, such as the alkylation unit, supply
about 50% of the gasoline supply in the US. Although FCC is a mature process
commercially deployed for over 60 years, the technology continues to evolve because of
following unique capabilities:
 The FCC process is the only continuous catalytic process in the refinery
business, which can adjust or replace catalyst on the run without a shutdown,
 The FCC catalyst is relatively robust to handle a wide variety of feedstock, and
 The FCC process can be operated over a wide range of conditions.
The focus of this paper is NOT on the historical evolution [1, 2, 3, 4] of FCC technology.
Instead, the paper focuses on selected snap-shots of issues, such as high temperature
erosion, corrosion and emission control, that exemplify the challenges that the FCC
process faces today and the new challenges in the future.
EXAMPLES OF CHALLENGES THAT FCC FACES TODAY
It might sound strange at first that keeping Examples of Today’s Challenges

an FCC unit running, without having the
unit `fall apart unexpectedly, is in fact the 1. Cyclone reliability
biggest challenge today for a process that
has been around for over 60 years. To put A. Erosion
this in the right perspective, the average B. Corrosion
run length between two scheduled
2. Emission Control – NOx reduction
maintenance shutdowns for an FCC unit
was about 2 years in the 1970’s/80’s,
whereas the current average run length is now being stretched to between 4 to 5 years.
Considering the fact that an FCC unit, on average, circulates about 50 tons of catalyst
per minute between the reactor and the regenerator; keeping an FCC unit running
continuously for 4 or 5 years means that the equipment will experience the traffic of over
100 million tons of catalyst without falling apart, which is by no means a small task. On
the other hand, the incentive of stretching the FCC run length is also enormous because
the average costs of an FCC maintenance shutdown is on the order of 10’s of millions of
dollars.
Cyclone Reliability
The FCC unit relies on reactor and regenerator cyclones to keep the catalyst within the
unit while circulating catalyst between the two vessels. Two recent industry surveys
reveal the pervasive problems of cyclones used in FCC operation today. Table 1
summarizes the survey results from Grace Davison as presented at their 2002 Dublin
FCC conference. The results indicate that catalyst losses from cyclones were the
number 1 problem in FCC operation, identified by the participants of the meeting. The
2006 Solomon survey (Figure 2) again revealed that FCC cyclone reliability was the
number 1 limitation of FCC unit run length today, with more than 41% of unscheduled
shutdowns of FCC units in US caused by cyclone problems. Two common cyclone
problems that challenge FCC units today, high-temperature cyclone erosion and
corrosion will now be discussed.
Cyclone Reliability – Erosion Problem
Problem Statement
One major contributor to unscheduled FCC unit shutdowns is unexpected cyclone failure
due to high temperature erosion. Figures 3a and 3b show two examples of high
temperature cyclone erosion problems. Figure 3a shows a cyclone which was eroded
through, from inside out, with holes on the cyclone body. Figure 3b shows multiple
cyclones that had severe erosion into the cyclone diplegs such that several diplegs were
cut off and fell to the bottom of the vessel.
Table 1: Grace Davison 2002 Survey
2006 Solomon FCC Survey

Events Determining TAR Timing
(Outside of Planned Maintenance)
Rx Cyclones
Regen Cyclones
Rx Refractory
Rg Refractory
12% 13% Rotating Equipment
Slide Valves
14% Regulatory
Other
3%
2%
28%
12%
16%
Figure 2: 2006 Solomon Survey Chart

(a)
(b)
Figure 3. FCC cyclone damage a) Inside out erosion; b) Diplegs cut off due to erosion
What is Happening in the Cyclone?
The most pervasive problem is high temperature erosion in the secondary cyclone,
particularly in the lower cone and in the transition to the dipleg, which is the focus of the
study.
There is a fundamental difference between erosion patterns in first and second stage
FCC cyclones. Highly-loaded first stage cyclones normally experience little to no cone
erosion, whereas the lightly-loaded second stage cyclones can have severe cone
erosion. This seems to be counter-intuitive at first. However, the key difference in
erosion pattern lies in the differences in the solids flow patterns and vortex formation, as
shown in Figure 4. Due to high solids loading and low gas velocity in a typical FCC
primary cyclone, the gravitational force plays a key role; as a result, the solids appear to
drop (or fall) rapidly down into the cyclone cone and dipleg, as shown in the figure on the
left side of Figure 4, taking only one to two full turns before exiting the cyclone bottom.
The vortex length in the highly-loaded primary cyclone is much shorter because the high
solids loading dampens the formation of a robust vortex. Therefore, the vortex does not
“whip” the solids at a high velocity around the cone in the primary cyclone.
In a typical FCC second stage cyclone, the solids loading is approximately 1/1000 to
1/10,000 of the loading in the first stage cyclone. Due to the light solids loading and high
gas velocity, the vortex is relatively long, energetic and, more importantly, moving
asymmetrically about its axis. As the swirling solids in the outer vortex approach the
cone in a second stage cyclone, the long, rapidly-rotating vortex accelerates the solids
stream and causes it to intensify its rotation (i.e., the solids spin faster similar to the
motion of a figure skater pulling inwards).
Figure 4: Schematic Depiction of First and Second-Stage Cyclone Operation
The outer vortex in a second-stage cyclone typically takes from four to six turns before
exiting the bottom cone, as shown in the figure on the right in Figure 4, and the spinning
continues into the top portion of the dipleg below the cone. The concentrated solids
stream rotates at a high velocity, and the unstable, continuous movement of the vortex
causes the significant erosion observed in the cone and the top of the dipleg of second-
stage cyclones.
Solution to the Cyclone Erosion Problem
Most FCC units in US rely on cyclone vendors to provide cyclones for FCC applications,
which will be categorized as “conventional cyclones” in this paper. Shell Global
Solutions, on the other hand, has developed a cyclone technology, which is different
from conventional cyclone in that it uses a vortex stabilizer.
Particulate Solids Research, Inc. (PSRI), an independent, industrial consortium, recently

studied and benchmarked different FCC cyclone technologies [5], since high
temperature cyclone erosion and cyclone reliability were highlighted as the major
concerns of FCC operation for companies in recent surveys. The PSRI cyclone test
program was structured to benchmark three different possible solutions to mitigate the
damaging erosion occurring in FCC second-stage cyclones:
1. Increasing cyclone length (L/D) of a conventional cyclone

2. Increasing the angle of the cone of a conventional cyclone
3. Adding a vortex stabilizer to a conventional cyclone
Air was used as the conveying gas in the test unit. The solids used were equilibrium
FCC catalyst with a median (Dp50) particle size of approximately 75 µm. The fines
(material <44 µm) concentration in the catalyst was approximately 8 wt.%. The particle
density of the catalyst was 1488 kg/m3. Loadings to the second stage cyclone were
varied between 0.001 to 0.16 kg/m3.
Multiple coatings of drywall joint compound were added to the inside of the cyclone
before each test. The amount of erosion occurring in the cyclone was measured by the
weight loss of the drywall compound occurring over a certain period of time.
Effect of Increased Cyclone Length
The study found that the erosion took place primarily in the bottom 1/3 of the cone of a
secondary conventional cyclone. A photograph illustrating this effect is shown in Figure
5. This figure shows that the drywall coating was completely eroded from the bottom 1/3
of the cone, whereas the remaining drywall was mostly intact.
Cyclone lengths were increased by increasing the length of the conventional cyclone
barrel with L/Ds of 3.1, 4.1 and 5.1. In these tests, the inlet gas velocity to the cyclone
was 19.8 m/s and the outlet gas velocity was 26.8 m/s.
The results of the testing to determine the effect of cyclone length are shown in Figure 6.
As can be seen, the erosion rate decreased with increasing cyclone length. The
measured erosion rate at an L/D of 5.1 was about seventy percent (70%) of the erosion
rate of the cyclone with an L/D of 3.1.
Barrel erosion rates were also measured in the tests and were found to be much lower
than the erosion rates in the cone at the test conditions, as also shown in Figure 6. The
measured barrel erosion ranged between 85 to 105 g/h, which is approximately fifteen
percent (15%) of the cone erosion rate for the cyclone with an L/D of 3.1, and
approximately twenty percent (20%) for the cyclone with an L/D of 5.1.
Effect of a Longer Cone Conventional Cyclone
The effect of a longer cone of a conventional cyclone on cyclone cone erosion was
tested by adding a longer cone so that the cone angle from the horizontal increased
from 79 to 84º. This increased the cone length from 0.8 m to 1.7 m. When comparing
the two cone configurations, the overall length of the cyclone was held constant.
As shown in Figure 7, the longer cone had a higher erosion rate at lower gas velocities
than the shorter cone (but longer barrel). However, the erosion rate became
approximately equal to the erosion rate of the shorter cone at the highest gas velocity.
The trend of the two curves was exactly opposite. For the short cone, the erosion rate
increased with gas velocity, whereas for the longer cone the erosion rate decreased with
increasing gas velocity. For an outlet gas velocity of approximately 26.8 m/s, the
erosion rate for the short cone was approximately 800 g/h, while the erosion rate for the
longer cone was approximately 1800 g/h—a factor of 2.25. However, even at the
highest gas velocities, which are outside typical operating conditions of the secondary
cyclones, the longer cone did not have a significant advantage over the shorter cone in
regard to cone erosion
Figure 5: Photograph of Erosion of Drywall Joint Compound in the Cone of a Second Stage
Cyclone
The Effect of Adding a Vortex Stabilizer to a Conventional Cyclone
To determine the effect of adding a vortex stabilizer to a conventional cyclone on cone

erosion, a flat-disk vortex stabilizer was added to the cyclone, approximately 1/3 of the
cone length up from its bottom to simulate the improved cyclone technology.
The effect of adding the vortex stabilizer disk to a conventional cyclone, simulating the
improved cyclone technology, on cone erosion is shown in Figure 8 for cyclones with an
L/D of 3.1. It was found that cone erosion for a cyclone with the vortex stabilizer was
significantly lower than that for a conventional cyclone without a vortex stabilizer. Cone
erosion increased linearly with increasing gas velocity for a conventional cyclone without
a vortex stabilizer. However, cone erosion of a cyclone with a vortex stabilizer decreased
slightly with increasing gas outlet velocity. The decrease in erosion is counter-intuitive at
first; however, this can be explained by the fact that the vortex diameter is smaller when
the diameter of the outlet tube is decreased to increase the gas outlet velocity. This
increases the distance between the vortex and the cone wall, which then reduces the
centrifugal force (and, therefore, the solids velocity) on the solids rotating in the cone.
This reduction in force on the solids would explain the decrease of cone erosion vs. gas
outlet velocity for a cyclone with the vortex stabilizer as shown in Figures 8.
Figure 6: The Effect of Second-Stage Cyclone L/D on Cone Erosion and
Barrel Erosion
Figure 7: The Effect of Cone Length on Second-Stage Cyclone Cone Erosion

Ugo , m/s
0 20 40 60
3000
w/o disk
00 w/ disk - -
2500
2000
1500
1000
500
Cone Ero sion Rat e, g /h
0
0 50 100 150 200
Ugo , ft/s
Material: FCC Eq. Catalyst Inlet Type: Tangential

Ugi: 65 ft/s (19.8 m/s) L/D b: 3 3
Cyclone Size: 17 -in (43 cm) Li: 14 grains/ft 3
Figure 8: The Effect of Gas Outlet Velocity on Second-Stage Cyclone Cone Erosion for
Cyclones With and Without a Flat-Plate Vortex Stabilizer (Cyclone L/D = 3.1)
For the shorter cyclone, the cone erosion rate was approximately 2100 g/h for the
conventional cyclone without a vortex stabilizer at a gas velocity in the outlet tube of
15.2 m/s. The corresponding cone erosion rate for the cyclone with a vortex stabilizer at
the same gas velocity was about 1400 g/h. The cone erosion rate with the vortex
stabilizer was about 67% of the cone erosion for the cyclone without the vortex
stabilizer. However, at an outlet gas velocity closer to actual practice (~ 46 m/s), the
cone erosion rate for a cyclone with the vortex stabilizer was only about 600 g/h. The
corresponding cone erosion rate for the conventional cyclone without the vortex
stabilizer was about 2900 g/h. This is a factor of about 5.
For the cyclone with an L/D of 5.1, the overall cone erosion rates were lower. This was
to be expected because the tests with a longer cyclone described above gave lower
cone erosion rates than shorter cyclones. As with the shorter cyclone, the trend lines of
cone erosion rate vs. outlet gas velocity were linear. Similarly, the curve for the
conventional cyclone erosion without a vortex stabilizer increased with increasing gas
velocity, and the curve for the cyclone erosion with the vortex stabilizer decreased
slightly with increasing gas velocity. However, as with the shorter cyclone, the cyclone
with the vortex stabilizer was found to have much lower erosion rates than the
conventional cyclone without the vortex stabilizer. Comparing the cone erosion rates at
an outlet gas velocity of 46 m/s, the conventional cyclone without a vortex stabilizer had
a cone erosion rate of approximately 1200 g/h, while the cyclone with the vortex
stabilizer had a cone erosion rate of about 240 g/h. This is a factor of approximately
five, which is similar to what was found for the shorter cyclone.
Why does the vortex stabilizer decrease cone erosion? It appears that the stabilizer
prevents the vortex from "whipping" the solids around at high velocities below the
stabilizer in the region where high cone erosion rates are experienced for a conventional
cyclone. Below the stabilizer, the high-velocity central vortex does not really exist.
Therefore, this reduction of spinning solid velocity in the outer vortex leads to significant
reduction in erosion. A comparison of the cone erosion rates for various second-stage
cyclone configurations is given in Table 2.
Table 2: Comparison of cone erosion rates for different cyclone configurations
Erosion Cone
Velocity Velocity
L/D Reduction Erosion
Inlet, m/s Outlet, m/s
(-) Factor Rate, g/h
Short Cyclone 3.1 19.8 46 Base 2850

Long Cyclone 5.1 19.8 46 >2 1200
Long Cone 5.1 19.8 46 >2 1200
Vortex Stabilizer 3.1 19.8 46 >4 650
Vortex Stabilizer 5.1 19.8 46 >11 240
Drywall joint compound was also added to the disk to see if the upper surface of the
vortex stabilizer would be eroded by the vortex. However, essentially no erosion was
measured on the upper surface of the disk. No erosion was found on the supporting
rods as well.
Commercial Bench-Marking
In the 1980’s, Shell had over 30 FCC units within the system, mostly with Conventional
Cyclones, which were found to be the number one cause of all FCC unscheduled
shutdowns.
Shell made a conscious decision in developing improved cyclone technology, using the
vortex stabilizer, and started the implementation of the technology in the early 90’s.
Figure 9 shows the result of how this improved cyclone technology reduced overall FCC
unscheduled down time in Shell refineries. Using 1992 data as the base line, Figure 9
shows that the improved cyclone technology, with the vortex stabilizer, reduced the total
unit down time of all FCC units in Shell system by a factor of 10.
Cyclone Reliability – Corrosion Problem
Problem Statement
In recent years, several FCC units have encountered unscheduled shutdowns due to
high temperature corrosion failure of the cyclone refractory system. These refractory
systems failed unexpectedly in some cases within only 4 to 5 years. Figure 10 (a) [6]
shows examples of a failed refractory system which resulted in sheets of refractory
peeling off from the walls of the regenerator cyclones. Figure 10 (b) shows that the fallen
refractory sheets were caught above the primary cyclone termination device.
Total Severity of Cyclone Problems

100%
Severity(Incl. nearmisses)[Numberof
90%
Events* Duration] 1992=100%
80%
70%
60%
50%
40%
30%
20%
10%
0%
1992 1993 1994 1995 1996 1997 1998 1999
Figure 9: Severity of cyclone related issues in Shell FCCUs
Regenerator Hexmesh Corrosion
Figure 10. (a) Failed refractory, in sheets, due to Hex Mesh corrosion [6]; (b): fallen refract sheets
caught above the primary cyclone termination device
Figure 10: Hex Mesh Refractory Structure
What is Happening to the Cyclone Refractory System?
The FCC regenerator cyclones are typically made of SS 304H material for high
temperature (~ 1400 ºF) operation. In order to protect cyclones from high temperature
erosion damage, as discussed previously, the regenerator cyclone internal surface is
commonly lined with SS 304H hex mesh, approximately 2.5 cm deep which is welded on
to the cyclone interior and packed with refractory within the hex mesh. The structure of
the hex mesh/refractory looks like a honeycomb, as shown in Figure 11. The refractory
is a concrete-like material which has high resistance to erosion.
Historically, the hex mesh/refractory system has served the FCC industry well in
providing protection against high temperature erosion. However, a series of unexpected
failures of the hex mesh/refractory system, due to corrosion of the SS304H hexmesh,
has surfaced very recently as reported by a number of operating companies as well as
FCC licensors [6, 7]. As shown in Table 3 and based on current known information, a
common pattern involves the application of a “calcium-rich” refractory in the regenerator
section of FCC units and failure appears to be related to a corrosion mechanism that
attacks the SS304H hex mesh support system for this refractory. It is more prevalent in
complete combustion mode (full burn).
Table 3: Summary of refractory analysis [7]
Refractory Analysis – Sample Summary

Effect of exposure to process conditions
Reported Refractory Instalation SO2 Level

Refinery Location S Na Volatiles
Type Date (ppm)
Dipleg - 1st stage
Refinery X Ca-rich binder 2005 2500 1.80 0.41 2.55
cyclone
Bad Refinery Y Ca-rich binder Regen Primary Cyclone 1.34 0.21 1.38
Refinery Z Ca-rich binder primary cyclone 1997 - - -
Refinery U Ca-rich binder 1.43 0.62 1.43
Refinery X Ca-rich binder Regen cyclone 2002 (original) 2500 1.69 0.27 2.89
Refinery T Ca-rich binder Regen Cyclone 2002 900 0.01 0.716 0.33
Good phos-bonded Regen Cyclone Dipleg 900 0.07 0.11 0.27
Refinery H
? Regen Cyclone 0.16 0.11 0.4
Refinery Y phos-bonded flue gas expansion joint 1.12 0.07 5.66
• Both Ca-rich binder and phos-bonded materials appear to absorb sulfur from the process gas
• No clear relation between S, Na and volatile content and “good/bad” rating
124 UOP - CONFIDENTIAL
Although there are some minor variations, this particular type of corrosion has very
specific patterns that are strikingly similar from all reported failures:
 The attack of the 304H SS hex mesh was identified primarily as

sulfidation/oxidation corrosion of the metal support structure.
 The corrosion occurs preferentially on the underside of the hexmesh metal lining
where it is welded to the base steel, such as at the cyclone wall, whereas little
corrosion is observed on the process side of the hexmesh lining where it is
exposed to the bulk of flue gas, as shown in Figures 12 and 13
 The corrosion on the process side is mild oxidation with a well protected Cr-O
layer, shown in Figure 14. The corrosion on the underside is a combination of
oxidation, sulfidation and carburization where Cr in SS304H no longer forms a
tight formation of Cr-O protection layer.
 The hexmesh/refractory detached from the wall in sheets, as shown in Figure
10, due to weakening of the corroded hexmesh.
 The corrosion can be very aggressive. Some units reported that newly installed
regenerator cyclones could have total refractory system failure within 4 years.
Figure 11: Refractory on process side vs. underside of the hex mesh lining
Corrosion Characterization
General Trends
Process
Side
Tab
• Process gas itself does not appear corrosive.

- Conditions are different within/behind refractory.
• Accelerated corrosion seemingly always associated
with carburization of base metal.
120 UOP - CONFIDENTIAL
Figure 12: Assessment of general trends in refractory corrosion characterization [7]

Regenerator Hexmesh Corrosion
• SEM/EDS analysis of a corroded hexmesh ligament
– Exposed side – oxidation
– Creviced region – carburization
– Underside – carburization & sulfidation/oxidation
Q&A Session
2010 Cat Cracker Seminar
Figure 13: Possible corrosion mechanism: Process side vs. Underside [6]
Possible Solutions
The root cause of the high temperature corrosion to the refractory metal support
structure is currently being discussed in the FCC industry. Several teams in the industry
are actively working on the problem. The common belief is that the hexmesh on the
underside is under a sub-environment that is more reducing than the bulk flue gas (more
oxidizing), and hence more prone to sulfidation and carburization. However, the exact
mechanism of how local reducing, sub-environment is formed is still being debated.
Possible solutions are a work in progress at the moment.
Emission Control – NOx Reduction
Problem Statement
The FCC regenerator is a major NOX emission source from the US refineries. Several
existing technologies are available to reduce NOX emissions from an FCC regenerator,
which include SCR, or selective catalytic reduction. Even though SCR is quite effective,
it has several issues:
 It is quite expensive, on the order of 10’s of millions of dollars, and even more so,
on the order of hundred million dollars, when the CO boiler needs to be replaced
due to the increase of back pressure caused by the catalyst bed of SCR.
 It requires a higher a residual flue gas temperature. Unless a second stage heat
recovery system is included (which means additional cost), the unit loses energy
efficiency
There is a potential cost-effective solution to this challenge.

What is Happening Inside the Regenerator?
Most of the NOX emissions from FCC units comes from nitrogen in the feed. The
contribution of direct oxidation of N2 to NOX is negligible, particularly for full combustion
FCC regenerators. For partial combustion regenerators, the contribution of direct
oxidation of N2 to NOX is relatively small if low-NOX burner technology is applied in the
CO boiler/incinerator.
A recent study [8] shows that about 50% of the nitrogen in the feed exits the FCC unit on
the reactor side and the remaining 50% of nitrogen in the feed exits as coke on the
spent catalyst sent to the regenerator. Of the 50% of the feed nitrogen exiting from the
reactor, about 10% of the feed nitrogen ends up as ammonia, which is collected in sour
water, and the other 40% of the feed nitrogen ends up in various streams of the reactor
liquid products.
This section focuses on the remaining 50% of the feed nitrogen, which enters the
regenerator in the form of coke on the spent catalyst. As the spent catalyst is
regenerated and coke is burned off in the regenerator, the nitrogen species on the coke
are released into the flue gas. Recent studies [8, 9] further show that only a small
fraction, less than 10%, of the feed nitrogen on coke is released in the form of NO X
emissions in the flue gas. The majority, or more than 40%, of the feed nitrogen on coke
is initially released in the form of NOX or other intermediates, but is eventually converted
in-situ to N2 in the regenerator.
The recent study [9] of batch regeneration of spent FCC catalyst with oxygen and helium
reveals a close interaction between the combustion of carbon and the release of
nitrogen in the coke. Figure 15 shows the concentrations of CO, CO2, and O2 in the flue
gas as a function of time as coke on the catalyst is burned off in the batch regeneration
experiment. The amount of coke on catalyst was not directly measured, but Figure 15
implies that coke on catalyst was removed continuously, converted to CO/CO 2, and
became negligible after 26 minutes as both CO and CO2 concentrations fell to negligible
levels. For the first 9 minutes, the O2 concentration remained low and the CO
concentration was higher than CO2, indicating a reduction environment in this period of
the batch regeneration. As O2 broke through the unit around the 10-minute mark and its
concentration continued to rise afterwards, coinciding with sharp drop of CO
concentration and rise of CO2, the batch regeneration shifted gradually from a reduction
environment to an oxidation environment.
Figure 16 shows the concentrations of NO, HCN, and N2 in the flue gas as a function of
time as coke nitrogen is released in the same batch regeneration experiment. Note that
most of the coke nitrogen was released as N2, which peaked around the 13.5-minute
mark at about 200 ppm, under a reducing or a slightly oxidizing environment. A fraction
of the coke nitrogen was released as HCN, which peaked around the 10.5-minute mark
at 35 ppm, under the same environment. Note that the NO concentration was below 20
ppm for the first 14 minutes under a reducing or a slightly oxidizing environment when
both coke on catalyst and CO were present. The NO X level increased sharply afterward,
and peaked around the 18-minute mark at 190 ppm when the CO concentration fell
sharply and the O2 concentration increased beyond 1%, as shown in Figure 15.
Figure 14: CO, CO2 and O2 in the Flue Gas as a Function of Time [9]
Figure 15: NO, HCN and N2 in the Flue Gas as a Function of Time [9]
The proposed reaction kinetics [9] for the release of coke nitrogen in the FCC catalyst
regeneration process involves initial volatilization of coke nitrogen as HCN, which could
be hydrolyzed to another intermediate, NH3. Both intermediates, HCN and NH3, can be
oxidized to NO, which can be reduced by the presence of CO or/and coke on catalyst to
N2.
Solution to the NOx Emission Problem
The FCC regenerator design has a direct impact on the effectiveness of in-situ reduction
of NOX to N2, and hence reduction of the final NOX emissions in the flue gas. The new
Shell Global Solutions’ low NOX regenerator technology [10] involves an improved
process consisting of the strategic design of catalyst and air distributions, as shown in
Figure 17, which enables the unit to operate in both full and partial combustion modes
with low NOX emission.
As shown in Figure 17, the regenerator system 1 includes a single regenerator vessel 10
having an upper end 12 and a lower end 14. The regenerator vessel 10 includes a
dilute phase catalyst zone 16 above and a dense phase catalyst zone 18 below with a
transition surface 20 between the two. The dense phase catalyst zone 18 further
includes a high velocity central region 22, located in the central portion 26 of the dense
phase catalyst zone 18, and a low velocity annular region 24, located in the annular
portion 28 of the dense phase catalyst zone 18. It is a significant aspect of the new
regenerator technology that the high velocity central region 22 and the low velocity
annular region 24 are formed within the dense phase catalyst zone 18, without the use
of a structural element such as a vertical baffle or a partition. The two fluidization
regions are instead formed within the dense phase catalyst zone 18 by the introduction
into the dense phase catalyst zone 18 of more than one fluidization gas stream, each of
which is directed and controlled in such a manner as to cause the formation of multiple
fluidization regions. Introduced into the central portion 26 of the dense phase catalyst
zone 18 is a high velocity fluidization gas stream that passes through the fluidization gas
distribution ring 32 near the bottom of the regenerator vessel 10. Introduced into the
annular portion 28 of the dense phase catalyst zone 18 is a low velocity fluidization gas
stream that passes through the fluidization gas distribution ring 38 located within the
annular portion 28 near the bottom of the regenerator vessel 10.
The controlled introduction of the various fluidization gas streams at the different
fluidization gas flow rates along with the directed introduction of the fluidization gas
streams to desired locations induces a desired circulation of the FCC catalyst within the
dense phase catalyst zone 18, as depicted in Figure 17 by the bold arrows 40 that show
the general direction and circulation of the FCC catalyst within the dense phase catalyst
zone 18. As shown by the bold arrows 40, catalyst particles in the high velocity central
region move in a generally upward direction, and catalyst particles in the low velocity
annular region move in a generally downward direction. Catalyst from the bottom end
42 of the low velocity annular region 24 flows into the high velocity central region 22 and
most of catalyst from the top end 44 of the high velocity central region 22 flows into the
low velocity annular region 24, thereby forming the catalyst circulation within the dense
phase catalyst zone 18.
Figure 16: A Schematic Diagram of the Low NOX Regenerator System
The regenerator system 1 further includes the introduction of spent catalytic cracking
catalyst into the high velocity central region 22 through conduit 50, which can be a riser
or a standpipe. Connected to the end of conduit 50 is a spent catalyst distributor 52 that
introduces spent FCC catalyst into the high velocity central region 22 in a generally
horizontal direction and mixes with catalyst circulating from the bottom end 42 of the low
velocity annular region 24. The regenerated catalyst is removed from the low velocity
annular region 24 by way of conduit 54, which removes regenerated catalyst from the
annular portion 28 of the dense phase catalyst zone 18.
One advantage of the new regenerator system is that the induced catalyst circulation
pattern distributes partially regenerated spent catalyst to the proximity of the surface 20,
which results in reducing NOx emissions from the regenerator. Another advantage of the
new regenerator system is that the location and the spent catalyst distributor design
induce intimate mixing between catalyst and transport air, thus preventing transport air
or entrained hydrocarbon from breaking through the dense bed, and resulting in reduced
afterburn.
Commercial Experience
The new low NOX regenerator technology was implemented as an integrated part of a
recent major FCC revamp, as presented in the case study below [10].
The original FCC unit was a large side-by-side unit with a regenerator diameter > 15 m,
as shown to the left in Figure 18. The scope of the revamp, as shown to the right in
Figure 18, included:
 A new stripper,
 Catalyst Circulation Enhancement Technology (CCET) [4] at the stripper outlet,
 A new, larger air blower,
 Additional pairs of regenerator cyclones for handling higher air flow, and
 The low NOX regenerator technology, consisting of a new spent catalyst
distributor, new regenerator outlets with CCET, new air distributors, and the
controlled system.
The unit performance was measured before and after the revamp. Key performance
improvements were observed:
The unit was able to operate in both full and partial combustion modes with low NO X
emission after the revamp. Figure 19 shows the NO X level in partial combustion mode
under 4 different air distribution conditions. As shown in the figure, NO X emission is the
lowest with Case D, with 40 ppm @ CO concentration of 2.4%. The unit can reach NO X
level lower than 40 ppm under either lower CO concentration or full combustion mode
with O2 concentration < 1% (not shown in the figure); however, partial combustion with
CO concentration in the range of 2 to 3.5% is the preferred mode of operation because
of its capability to increase the unit feed rate.
Figure 17: Scope of the FCC Revamp in the Case Study

Stack NOx versus Rgn OH CO
100
90
80
70
60
NOx @ 0% O2, ppm
50
40
30
20
10
0
1.5 2.0 2.5 3.0 3.5 4.0 4.5
CO, pct
Case A Case B Case C Case D
Figure 18: NOx emission in partial combustion under four cases of air distribution
What the Future of FCC Might Look Like
Shifts of Product Demands and Feedstock
Historically, the FCC unit and its downstream units provide the majority of gasoline
supply in the world. However, the landscape of the demand from FCC products is
shifting and is region-specific as shown in Figure 20.
The demand for propylene from FCC products has increased, and in some regions, the
light olefins have become the premier products from FCC. In addition, in many regions
the demand for diesel outpaces the demand for gasoline.
Figure 21 shows the demand shift in the US. The motor gasoline demand has reached a
plateau and the long term projection is a decreasing demand trend. One the other hand,
demand for gasoil and diesel is increasing. This shift from motor gasoline to gasoil/diesel
follows a similar pattern as was seen in Europe 10 years ago. In parallel, the demand for
propylene in the US is also growing so rapidly that the traditional source for propylene -
steam cracking - cannot keep up with the demand. From the available technologies to
bridge the gap, FCC is by far the best.
Figure 19: Current market demands of FCC products
Figure 20: Road transport fuel demand trends in the United States
Given these demand shifts, the refining industry needs a redefinition of the FCC process
to enable the following process objectives to be satisfied:
 Lower gasoline yield;
 Higher LCO yield, with better product quality characteristics (lower density and
higher cetane number);
 Higher propylene yield;
 Flexibility to switch seamlessly between these different production modes and
conventional FCC operation depending on the market demand.
There are several new FCC process technologies available that address these expected
shifts in market demands. One of them is the Shell MILOS process [11, 12], or Middle
Distillates and Lower Olefins Selective process.
A relative new direction of FCC is to co-process bio-liquid feedstock. The FCC unit is the
single largest contributor, accounting for 30 to 50%, to the overall CO2 footprint of a
refinery. Beside the benefit of a potential, inexpensive, alternative feedstock, processing
bio-liquid feedstock has the added benefit of a tax credit in a region where CO2
emissions are regulated. Processing bio-feedstock presents totally different challenges,
yet to come, in FCC operation such as extremely high oxygen content in the feedstock.
MILOS – Process Background
Recycling cat-cracked gasoline to the bottom of the riser (where the temperature is
typically in the range of 1250-1320 ºF) has been widely practiced in the refining industry
with the objective of increasing propylene yields. This has the desired effect of producing
more propylene, but with significant penalties of producing large amounts of coke, dry
gas, butylenes, LCO+ and it would produce little iso-butane. To confirm this,
experiments were conducted in which light and heavy cat cracked gasoline were
recycled in the Shell Global Solutions large FCC riser pilot plant.
The most favorable condition for the production of propylene was found when light CC
gasoline was injected below the VGO feed such that the residence time for cracking
pure light CC gasoline was approximately 0.5 to 1 second prior to the VGO injection
point. However, it had a large impact on VGO conversion, which dropped at constant
coke rate. As a result the net LCO+ flow rate at riser exit increased significantly. Such
large increases in LCO+ material were also observed in all other tests. Additionally,
injecting light CC gasoline with or above the VGO feed yielded a net decrease in
propylene yields due to quenching in that section of the riser reactor. For heavy
gasoline, the results were even more disappointing in all cases. The flaw of this option is
that it is impossible to achieve optimal conditions for both feeds (both the recycled
gasoline and the VGO) in one single riser.
Figure 21: MILOS concept
MILOS Process Concept
The MILOS concept, shown in Figure 22, consists of adding a separate riser to the FCC
unit, in which gasoline or other suitable streams are cracked under process conditions
tailored specifically to maximize propylene yields, to maintain or increase the iso-butane
yield (which is desirable for the alkylation unit) without producing excessive amounts of
dry gas, coke and butylenes. The ideal temperature is relatively low (1050-1150 ºF) in
order to minimize thermal reactions. At temperatures lower than these, high gasoline
conversions cannot be easily obtained. The catalyst used is the same as in a
conventional cat cracker with ZSM-5 added to boost the propylene yield. Typical yields
obtained by cracking catalyst cracked gasoline in a MILOS riser are 15.5 %wt propylene,
7.5 %wt dry gas and 5%wt iso-butane.
Case Study – Diesel Mode
A case study focusing on diesel-mode implementation is presented to demonstrate one

aspect of implementing MILOS in existing FCC units.
The base-case is a Shell Global Solutions’ designed long residue CCU, processing feed
with a Conradson Carbon content of 3.2%wt. Shell’s rigorous heat-balanced Catalytic
Cracking Process model was used. This model was tuned to the actual operating
conditions of the specific FCC unit, including realistic unit constraints and feed
properties.
The base-case (Case #1) represents the average operating conditions and average feed
properties of the unit over the recent years. Besides this case, the following cases were
explored:
 Cases #2 and #3: the maximum diesel and the maximum propylene cases based on
the conventional FCC-unit without the addition of a separate MILOS riser
 Case #4: a MILOS riser is added to the FCC unit to achieve maximum diesel and
propylene
 Case #5: a sensitivity case with the same MILOS-FCC unit, maximizing propylene
only.
The results of the case studies are presented in Table 4.

The comparison between the base case FCCU (Case #1) versus the diesel mode FCCU
(Case #2) or propylene mode FCCU (Case #3) is straightforward. If we operate the unit
in diesel mode (Case #2), the LCO yield is boosted by more than 3%wt (Table 4) and
the cetane index is increased by 5 points. However, propylene yield suffers a reduction
of 1.2%wt. Valuable LPG (total C3s and C4s) also suffers a reduction of 3.5%wt. On the
other hand, if we operate the unit in propylene mode (Case #3), the propylene yield is
boosted by 3%wt, and the LPG (total C3s and C4s) is also increased by 9%wt. (The
increase in butylenes Cases #3, 4 and 5 is a direct result of ZSM-5 addition). However,
the cetane index of LCO suffers a big hit of about 6 points reduction. LCO yield is slightly
reduced by 1%wt.
The situation above is a typical dilemma faced by FCC that is supplying a diesel and
propylene driven market. The diesel mode and propylene mode represent the opposite
extreme ends of operation and depending on market forces, the operator swings from
one mode to the other. Some operators might choose to operate in the middle of the two
modes and not make either maximum propylene or maximum diesel in terms of quantity
and quality. However, after revamp with MILOS, the operator can produce more
propylene than the standalone FCC propylene mode and more LCO than the standalone
FCC diesel mode, with even a higher cetane index, all achieved at the same time (Case
4 in Table 4).
Table 4: Diesel revamp case study results
Cas e number #1 #2 #3 #4 #5
FCC on ly FCC onl y FCC Di esel mo de FCC Pro pyle ne mode

Case Base
Di esel mod e Prop ylen e mode + MILOS + MIL OS
Existing FC C re vamp Existing FCC re vamp

Typ ical o pera ti ng Existin g unit op erated Exi sti ng u nit o pe ra te d with a ddi ti on o f wi th a ddi ti on o f
co ndi ti ons in
Case d escrip ti on to pro duce ma ximum to prod uce maxi mu m MIL OS tech nology. MIL OS tech nol ogy.
rece nt ye ars
LCO p ropyl en e FCC i s o per ati ng in FCC i s o pera ti ng in
diesel mod e p rop yl en e mo de
Fre sh fe ed rate to FCC riser t/d 100 00 10 000 10 000 10 000 1 000 0
Recycl e of ligh t cat crack gaso lin e to MILOS t/d N/A N/A N/A 2 50 0 25 00
o
FCC riser ou tlet temp erature C Base -19 +5 -30 +5
ZSM-5 a dditive in catal yst in ventory % wt 0 0 10 10 10
LCO Ce tane Index - 2 5.9 31 .0 24.9 3 3.3 2 4.8
Ove rall yie ld
C2 mi nus % wt 4.3 3.2 4.4 4.7 6.3
Ethyle ne %wt 1.1 0.8 1.2 1.9 2.4
Total C 3 % wt 8.2 6.3 12.2 1 3.7 1 7.1
Propylene %wt 5.2 4.0 8.2 9.8 1 1.9
Prop ane % wt 3.1 2.3 4.0 4.0 5.1
Total C4 %wt 1 0.2 8.6 13.7 1 6.0 1 7.8
i-Bu ta ne % wt 3.2 2.8 3.8 5.5 5.6
n-Bu ta ne % wt 1.2 0.9 1.5 1.7 2.0
Total C4 Ole fins % wt 5.8 4.9 8.4 8.9 1 0.2
i-Bu tylene s % wt 1.3 1.1 2.9 2.9 3.5
Li gh t cat cra ck gasol in e (C5 - 142 de gC ) % wt 3 4.7 32 .8 30.3 1 4.4 1 6.1
He avy cat crack g asolin e ( 142 - 22 1 d eg C) % wt 1 1.2 12 .4 9.4 1 2.0 1 0.8
LCO (221 - 370 degC) %wt 1 5.8 18 .9 14.7 1 9.3 1 5.2
HC O (3 70 - 4 25 de gC) % wt 3.4 4.4 3.4 4.5 3.5
SO (4 25 d egC+) % wt 4.5 6.7 4.4 7.5 4.5
Co ke % wt 7.6 6.8 7.5 7.9 8.8
Gas oline /C ycle Oil ratio wt 2.9 2.4 2.7 1.4 1.8
It is clear from the results above that a revamp with MILOS (Case #4) on a conventional
FCC unit brings the benefits of maximising propylene make, maximising LCO make and
increasing LCO Cetane quality, all at the same time. This is achieved by allowing the
FCC to operate in diesel mode to achieve the desired high LCO yield and high LCO
Cetane. Directing the cooler MILOS spent cat (cooler relative to regen temperature) to
the FCC riser also plays an important role in improving the LCO yield and quality. On the
other hand, the MILOS riser is focusing on maximising propylene by cracking recycled
light cat-cracked gasoline.
With the same FCC and MILOS unit, we have studied a sensitivity case to see if the
propylene make can be boosted further. In this study, the conventional FCCU is
operated towards maximum propylene make instead of operated in the diesel mode
(Table 4).
It is clear that with this MILOS-FCC configuration (Case #5), the propylene yield can be
further boosted if the operator is ready to accept the same level of LCO yield and quality
as they are getting during the conventional FCC propylene mode operation. The
propylene yield can be increased to almost 1.5 times compared to the standalone FCC
propylene mode operation.
MILOS vs. other process technologies
The MILOS process has significant advantages compared to technologies licensed by

Shell’s competitors (Tables 5 and 6). Most importantly, the operational flexibility offered
by MILOS is a key advantage. As MILOS is integrated in an FCCU, it can even be
reverted on the run to regular FCC operation if this is required. DCC and PetroFCC do
not have this flexibility. A DCC/PetroFCC implementation requires many more significant
changes to an existing FCC unit.
Overall, the revamp of a conventional FCC unit to a Diesel MILOS-FCC is a very

attractive option to refiners, especially for those units located in Europe or other regions
where both diesel and propylene demand are expected to grow rapidly. The operating
flexibility provided by MILOS helps set a refinery up for long term success with changing
market environments.
CONCLUSIONS
The FCC process is one of the most important circulating fluidized bed processes.
Through a few examples, some current challenges of high temperature erosion,
corrosion and NOx emission in operating a high temperature CFB process like FCC
have been highlighted.
Although the FCC process has been in commercial operation for over 60 years, the
technology continues to evolve. A new FCC technology, MILOS, for producing more
light olefins and diesel in light of the market demand shift has been proposed and the
new trend of co-processing bio-feedstock has been discussed. These new applications
will present new challenges to the operation of FCC.
Table 5: Typical features of MILOS relative to Deep Catalytic Cracking technology
Table 6: Typical features of MILOS relative to PetroFCC technology

REFERENCES
1. Fluid Catalytic Cracking hits 50 year mark on the run, A.D. Reichle, OGJ, May
18, 1992, P. 41.
2. Evolutionary design changes mark FCC process, J. R. Murphy, OGJ, May 18,
1992, P. 49.
3. FCC is far from being a mature technology, A.A. Avidan, OGJ, May 18, 1992, P.
59.
4. “Fluid Catalytic Cracking”, in Handbook for fluidization and fluid-particle systems,
Y. Chen, Wen-Ching Yang, ed. (2003)
5. “Keeping FCC units on track, winning the operation race with an innovative
cyclone technology”, Y. Chen, et al, 2010 NPRA meeting
6. 2010 NPRA FCC seminar
7. 2010 NPRA Q&A
8. Rosser, F.S., et al, “ Integrated view to understanding the FCC NOx puzzle “,
2004 AIChE Annual meeting.
9. Stevenson, S. A. et al., “Model of NOx emission from laboratory regeneration of
spent fluid catalytic cracking catalyst”, Ind. Eng. Chem. Research, 2005, 44,
2966-2974.
10. Y. Chen and D. Brosten “A New Technology for Reducing NO X Emission from
FCC Regenerators”, 2008 NPRA meeting
11. W. Mo, F. H. H. Khouw and G. A. Hadjigeorge, US2006/0231461A1 – “Method
and Apparatus for making a Middle Distillate Product and Lower Olefins from a
Hydrocarbon Feedstock”; US2006/0178546A1; US2006/0191820A1.
12. M. Nieskens, “MILOS – Shell’s ultimate flexible FCC technology in delivering
diesel/propylene”, NPRA Annual Meeting, AM-08-54, March 9-11, 2008.
PUTTING STRUCTURES INTO FLUIDIZED BEDS - FROM
CONCEPT TO INDUSTRIAL APPLICATIONS
Qiang Zhang, Weizhong Qian, Guohua Luo, Yao Wang, Fei Wei*
Beijing Key Laboratory of Green Chemical Reaction Engineering and Technology,
Department of Chemical Engineering, Tsinghua University, Beijing 100084, China
Corresponding author. Fax: +86-10-62772051; E-mail: wf-dce@tsinghua.edu.cn
ABSTRACT
Structures of particles, particle agglomerates, distributors, and internals have
significantly influence on hydrodynamics and transfer behaviors of the dense
gas-solid fluidized bed. For nanomaterial production, the particle surface and their
agglomerated structures directly influence the fluidization behaviors; while for coal to
chemical process, the distributors, internals play an important role in regime transient,
and hydrodynamics. Carbon nanotubes mass production, coal to chemicals process.
and fuel production were employed as examples to describe the concept of putting
structures into fluidized bed, and then to put these structures into industrial
applications.
The asymmetric surface of solids plays a very important role in material functions,
such as its reactivity, catalytic performance, adsorption, and transfer behaviors,
which were rapidly developed with the growth of nanotechnology and information
technology. Recently, nano-structured granular materials, which are consisted of
various flakes, tubes, and rods, possess unique mechanical, electrical, optical,
electrochemical, and thermal properties. Novel advanced functional nanomaterials
for energy conversion and storage, environmental, catalysis, materials engineering,
biology, drug, sensors, devices, information technology are highly concerned. Those
particles usually belong to group C particles according Geldart classification, which
were extremely fine powders and therefore the most cohesive particles. The
fluidization of Group C particles was difficult to achieve, which may require the
application of some external forces, such as mechanical agitation. Recently, with the
fast development of nanotechnology, nanomaterials with tunable structures and
extraordinary properties were widely investigated.
In fluidized bed, the particles become fluid-like dense flow. Thus, the heat transfer
between fluid and solid phase is over thousand times of that on porous catalysts,
which is an important step for high-efficiency solid processing. For fluidization
1
behavior, the symmetric spherical particles and cylinder fluidized beds always the
first and simplest choice. While for the academic researches and industrial
applications, it is quite important to let materials or catalysts well fluidize, and to
control their fluidized states as well as transfer behaviors. Structured internals in a
fluidized bed reactor have significantly influences on regime transition. Recently, they
were also widely used in a fluid catalytic cracking (FCC) stripper. To get high yield of
intermediate products, plug flow fluidized bed with high efficient heat transfer were
highly required. Structured distributors and internals can also play an important role
in control of the backmixing and heat transfer of the fluidized bed. When the fluidized
bed reactor is coupled with special structures for various functions, excellent heat
and mass transfer properties as well as the multifunctional properties were provided
by the particles. This significantly enlarges fluidized bed reactor applications for
chemical or material production, or even device manufacture. When putting those
structures into fluidized bed, a series of scientific questions were proposed: 1) Can
those structures be smoothly fluidized? 2) Can we use fluidized bed to produce
structures in large scale? 3) Can we use structure to improve the efficiency of
fluidized bed process?
To answer these questions, we briefly review our recent progress on putting

structures into fluidized bed reactor, and demonstrate several examples in mass
production of carbon nanotubes (CNTs), high efficient catalytic reaction for coal to
chemicals and particle sensors for detection of fluidization state.
FLUIDIZATION SCIENCE: NANOPARTICLE AGGLOMERATION AND ITS

FLUIDIZATION
Nanomaterials with morphological features on the nanoscale (smaller than 100 nm in

at least one dimension) have become the focus of science because of many
interesting properties that make them attractive for various applications. Interactive
forces between nanosized particles significantly increase with decreasing particle
size, so nanoparticles coalesce easier than micron-sized particles. The properties of
the primary particles determine the properties of the agglomerates that control the
behavior of the two-phase flow in a fluidized bed. For instance, as shown in Fig. 1,
the SiO2 aerogels with a size distribution of 7 to 16 nm form agglomerates, called
multi-stage agglomerates (MSA), by several steps with different bonding
mechanisms.[2] The cohesive force between nanoparticles and the gravity force on
the agglomerates are effectively diminished by the porous MSA structure, thus, even
with a fairly high bed expansion, these SiO2 agglomerates still form bubbleless
fluidized beds that have a texture much closer to the particulate fluidization of a
liquid–solids system and which obeys the Richardson–Zaki relation, as opposed to
the aggregative bubbling regime in many gas–solids systems. In the region of Ug =
2
0.01–0.08 m/s, the average hydrodynamic diameters of the fluidized complex
agglomerates are 230–331 μm. The structure of the agglomerates as well as their
size, apparent weight and the interactive forces between them significantly influence
the hydrodynamic behavior of agglomerating fluidization.
Except nanoparticles, 1D nanomaterials, such as CNTs which consist of graphene

sheet wrapped around to form cylindrical tubes, were selected as model to
demonstrate their fluidization behavior. The dependences of bed expansion and
pressure drop on gas velocity in a CNT nano-agglomerate fluidize bed is shown in
Fig. 2.[3] A smooth and highly expanded fluidization was achieved, but a strong
hysteresis exists in the CNT fluidization curve. On the defluidization branch, similar to
Geldart-A particles, particulate fluidization, ABF, turbulent, and fast fluidizations can
be successively observed. However, Uc and Use of the CNTs were relatively lower
than that of Geldart-A particles, due to the weak interaction among the CNT
agglomerates and their highly porous structure. This indicated that good fluidization
behavior can be achieved only with strong turbulence of the fluidized bed, because of
strong interaction between agglomerated CNTs.
4
Increasing gas velocity
Decreasing gas velocity
3
H/H0
Umb=0.038 Uc=0.11 Ut=0.205
1 U =0.017
0.0 mf
0.1 0.2
Ug (m/s)
Fig. 1. Nanoparticle agglomeration Fig. 2. Dependence of bed expansion

behavior on Geldart classification. and pressure drop on gas velocity in a
CNT nano-agglomerate fluidized bed.[3]
Fig. 3. (a) Design of prototype PMS. (b) A PMS prototype.[4]
3
To identify a particle trace in a fluidized bed, an intelligent particle spy capable of
detecting, transferring, and storing data, is proposed under the name of Particle
Measurement Sensor (PMS) (Fig. 3).[4] The mobile PMS can be appended to the
measurement system to sense movement information, including acceleration,
velocity, distance between particles, and so on. A prototype 60-mm-dia PMS was
tested and served as a particle spy in a fluidized bed delivering the in situ
acceleration information it detects. With increasing superficial gas velocity in the
fluidized bed, the acceleration felt by PMS was observed to increase. The variance of
the signals, which reflect the fluctuation, increased at first and then reached a
maximum at the gas velocity (Uc), which marks the transition from bubbling to
turbulent fluidization. The probability density distribution peak can be divided into the
emulsion phase peak and the bubble phase peak. The average acceleration of
emulsion and bubble phase increased, while the variance of both phases reached a
maximum at Uc, at the same time. However, the difference between the variances of
two phases reached the maximum at Uc. The solids mixing behavior of nanoparticle
in a fluidized bed were also investigated.[5] The axial and radial solids dispersion
coefficients of nanoparticles were two orders of magnitude lower than those in fluid
catalytic cracking (FCC) catalyst systems. The axial solids dispersion coefficient
increased with increasing superficial gas velocities, and ranged between 9.1×10−4
and 2.6×10−3 m2/s. There was a step increase in the axial solids dispersion
coefficient between the particulate fluidization regime and bubbling and turbulent
fluidization regimes. As the superficial gas velocity increased, the radial solids
dispersion coefficient increased gradually, from 1.2×10−4 to 4.5×10−4 m2/s. The much
smaller Da and Dr, compared to regular fluidized systems, is mainly due to the
reduced density difference between the fluidized particles and fluidizing medium.
PARTICULOGICAL DESIGN: NANOSTRUCTURE PRODUCTION IN A

FLUIDIZED BED
The fluidization technique has been an efficient route for materials production.
However, how to produce tunable nanostuctured materials in a fluidized bed is still an
open area. We selected CNTs as a typical advanced nanostructured materials to
describe their mass production via fluidization bed chemical vapor deposition
(CVD).[1, 6] CNTs possess extremely high tensile strength, high modulus, large aspect
ratio, low density, good chemical and environmental stability, and high thermal and
electrical conductivity. It is a new type of carbon nanomaterials with high
performance that are in demand for different potential applications, including both the
large-volume applications (such as supercapacitor or battery electrodes, battery
electronic additives, conductive, high-strength composites, etc.) and limited-volume
applications (such as electronic devices, etc). Recently, CNTs have been used as
fillers in advanced battery electronic additives, supercapacitor or battery electrodes,
4
and light high-strength composites at a scale of hundreds of tons. Mass production of
CNTs with desired structure at a low cost is the first step.
Fig. 4. The pilot plant facility for MWCNT production.[1]
Among various ways to synthesis CNTs, the CVD method has the advantages of mild
operation, low cost, and controllable process, and is the most promising method for
the mass production of CNTs. In CVD methods, the carbon source is deposited with
the assistance of a catalyst at temperatures lower than 1200 oC. Tubular CNTs are
deposited at the catalyst site. Fe, Co, Ni particles, always show high activity for CNT
growth. With sustainable growth of CNTs, the as-grown tubes will cluster into
agglomerated or aligned CNTs. The CNT aggregates were nanocarbon products in
which CNTs are randomly entangled with each other, while the CNT arrays were
nanocarbon products in which CNTs are nearly parallel to each other.
The agglomerated CNTs are 3-dimensional network structure composed with large
amounts of CNTs. They are very easy to be synthesized for the reason that CNTs are
5
prone to entangle with each
other during the growth on
powder catalysts.[7] If the wall
number of CNTs decreased
and became
double/single-walled, then the
as-obtained CNTs will be very
flexible. S/DWCNTs were
confined grown in the porous
catalyst.[8] S/DWCNT growth
needs not only a good
dispersion of the active metal
components on the catalyst
support and a suitable large
BET surface area, but also a
proper catalyst structure.
Layered double hydroxides
(LDHs), also known as
hydrotalcite-like materials,
which are a class of
two-dimensional Fig. 5. CNT-array double helices grown on
nanostructured anionic clays Fe/Mg/Al LDH flakes. a) As-obtained Fe/Mg/Al
whose structure is based on LDH flakes; b) a large number of CNT-array
brucite (Mg(OH)2)-like layers, double helices; c) dextrorotatory CNT-array
can be used as a novel double helices grown on LDH flakes; d,e)
catalysts for SWCNT growth calcined LDH flakes and middle section of (c);
with a huge BET surface area
of 1289 m2/g.[9] Based on catalyst concept design, multiphase flow of CNTs, and
process scale up rules, A pilot plant for producing high quality and purity MWCNTs
was designed (Fig. 4).[1] Based on the fluidized bed technologies developed, we
realized a commercial production of MWCNTs with a capacity of 560 tons per year,
and SWNCTs with a capacity of 8 tons per year in the middle of 2009.
The aligned structures of CNTs were always obtained via a bottom-up self-assemble
process during thermal/floating CVD. The synchronous growth of a CNT forest
induced by stress was found.[10] Based on CNT growth and agglomeration
mechanism, various effective strategies for VACNT mass production have been
proposed. It is commonly reported that aligned CNTs can be synthesized on a flat
surface. However, the surface area of the flat substrate is often limited and its
mobility is poor. Only 1 g/h VACNT arrays can be obtained with flat silica as substrate.
If a substrate with a larger surface area is used, such as spheres, more VACNT
6
arrays can be produced. We have recently large scale synthesized VACNT arrays on
spheres,[11] quartz fibers[12] and flakes.[13] Left or right handed CNT arrays were
twisted into a double helix on a LDH flake through a self-organization process during
growth by chemical vapor deposition (Fig. 5).[13a] The wall number and diameter of
CNT in the double helix can be tuned by chemical precursor mediated process. [13b] To
avoid the damage caused by the collisions among CNT arrays during the transport or
fluidization process, a strategy of intercalating VACNTs into layered compounds and
directly constructing a layered hybrid nanocomposite composed of alternate CNT
films and inorganic sheets was proposed (Fig. 6).[14] This is a successful way for the
mass production of VACNT arrays in a fluidized bed reactor. A 3.0 kg/hr VACNT array
productivity was realized in a fluidized bed reactor with a diameter 500 mm. [15] The
CNTs in the as-grown arrays were with good alignment, and can be easily purified by
facile acid treatment.
Fig. 6. Illustration of the formation of hybrid composites by intercalating vertically

aligned CNT films into layered inorganic compounds, showing stacked layers in the
original vermiculite (left panel), catalyst particles adhering to the surface of the layers
after impregnation (middle), and aligned CNTs between the layers after the CNT
growth process (right); d) SEM image showing an enlarged view of a single interlayer
with aligned CNTs and an interlayer distance of 20mm. e) SEM image showing CNT
growth on both sides of a vermiculite layer. f) Transmission electron microscopy
image of a multiwalled CNT.
7
For the horizontally aligned CNT formation, the gas flow, which makes the CNTs
grow in a way similar with a flying kite, is efficient for super long (20 cm) CNT growth
at a fast rate (80-90 μm/s).[16] The growth rate of CNT is very high, and the weight
space velocity can reach 108 gCNT/gcath, which is millions of times of that of
agglomerated CNTs on porous catalyst. The synthesis of HACNTs on movable or
free substrates in a fluidized bed to obtain long CNTs is still an important issue.
Based on particuological concept design, the agglomerated CNTs and aligned CNTs
have been successfully mass produced in ton scale via fluidized bed process, and
are available in the market. This will greatly promote the bulk applications of CNTs,
and provide a sustainable route for the development of the novel advanced
materials.
INDUSTRIAL APPLICATION: MULTI-FUNCTIONAL STRUCTURE FOR

ADVANCED CATALYTICAL FLUIDIZATION TECHNIQUE
The last level of structure in fluidized bed is in macro-scale of fluidized bed, such as
the distributors, internals or bluffs in a fluidized bed reactor. Chemical looping
concept for high efficient fossil fuel conversion by a family of configurations with
different reactors or regions of fluidized bed have also been explored. [17] Many
applications of internals in fluidized bed have been employed for acrylonitrile, aniline,
vinyl acetate and vinyl chloride monomer synthesis,[18] and fluid menthol to propylene.
The influence of internals on hydrodynamics and mixing in fluidized bed and related
reactor performance will also be presented.
Due to the worldwide crude oil shortage and the rapidly increasing demands for light
olefins, the methanol to olefins (MTO) process and dimethyl ether to olefins (DTO)
process were selected as the alternative ways for the production of light olefins.
Because of the strongly exothermicity of MTO/DTO reactions and fast deactivation of
SAPO-34 zeolite catalyst, a fluidized bed was the preferred reactor for industrial
application.[20] Consequently, the MTO/DTO catalysts needed to be prepared for
facile fluidization. Herein, a hierarchical SAPO-34 zeolite with high crystallinity and
excellent hydrothermal stability was directly synthesized in the nanoscale confined
environment provided by the natural layered material kaolin (Fig. 7). [19] The
hierarchical sample showed a much higher conversion than the conventional zeolite.
The overall olefin selectivity was as much as 96.7%, which was 4–7% higher than
that of the conventional zeolite. The presence of the mesopore structure shortened
the diffusion path, thus, the primary products could easily diffuse out of the zeolites
and secondary reactions were avoided. Therefore, higher propylene selectivity and
overall olefin selectivity were obtained. This expected to be a facile and economically
8
feasible way to prepare more effective catalyst for fluidized MTO/DTO process. A
fluidized bed methanol to propylene (FMTP) industrial technology was developed.
The industrial practice of fluidized bed for FMTP process at Huainan with a 470 hours
of continuous operation at full capacity were carried out, and high yield of propylene
was reached (Fig. 7c).
Fig. 7. a) As synthesized hierarchical SAPO-34 zeolite; b)DME conversions and

overall olefin selectivities (Conversion on hierarchical (■) and conventional (□)
SAPO-34; selectivity on hierarchical (▲) and conventional (Δ) SAPO-34.[19] c)
300kT/a multistage fluidized bed FMTP unit
Polyvinylchloride (PVC) is second largest general plastics in the world, the very low
space velocity makes gas-phase catalytic hydro-chlorination of C2H2 on
HgCl2/activated carbon (AC) catalyst only can be carried out in packed bed at high
conversion. However, if a multistage fluidized bed (MSFB) is applied into this process,
a high conversion of C2H2 at 130-140 °C at a high space velocity of C2H2, while
maintaining high selectivity to vinyl chloride monomer (VCM), could be obtained by
efficiently inhibiting the back-mixing of gases between stages. The new catalyst with
a coconut-shell-type AC as the support shows much higher mechanical strength for
stable fluidization with a proper pore structure for the dispersion of HgCl2 and a high
thermal stability, as compared to a catalyst with coal-based AC as the support in
9
conventional packed bed reactors. The catalyst lifetime estimated by simulation and
a rapid sublimation experiment fits in well with the data from the pilot plant test.
These results suggest that the combination of a MSFB and the new catalyst
described here is a novel technology for producing VCM on a large scale at low cost.
The scale-up of MSFB through a series of small hot model, 3000 ton/a pilot-plant and
100 kT/a industrial plant was demonstrated and reactor modeling of the scale up of
the MSFB was carried out, as shown in Fig. 8.
Fig. 8. Top: Internal structured fluidized bed reaction; Bottom: Multistage fluidized
bed reactor for VCM production scale-up process: Left: small hot model test unit;
Middle: 3 kT/a pilot plant; Right: 100kT/a multistage fluidized bed CVM unit
The flow structure of gas-solid can significantly regulated the flow directions. The
gas-solid downward flow (downer) reactor can reduce axial gas and solids
backmixing by 30 times in comparison with upward flow riser reactor. Downer is
therefore acknowledged as a novel multiphase flow reactor with great potential in
high-severity operated processes, such as the short contact time reactions with the
intermediates as the desired products.[21] Compared with the riser reactor with the
same feeds and catalysts, the LPG and propylene yield increased by 8.15 and 4.30
wt%, respectively. The gasoline octane number likewise reached 94.8 with 28 wt%
olefin content. However, dry gas is significantly suppressed, and the coke has little
10
change in yield even with the increased catalyst to oil ratio. With some gasoline
recycling, the LPG and propylene yield increased by 11.45 and 5.06 wt %,
respectively. The olefin content in gasoline significantly decreased to 22 wt %; the
high octane number (95.4) is maintained. The computational fluid dynamics (CFD)
coupled with a 6-lump kinetic model is also applied to simulate the FCC process for
the industrial trials. The yield of propylene and butylene and the temperature profile
along the axis direction demonstrated consistency between the simulation results
and the experimental data. The axial solid mixing mechanisms in gas-solids
cocurrent upflow and downflow circulating fluidized bed systems revealed that
among the many influencing factors, flow direction has the most profound influence
on the axial solids mixing. When the flow is in the direction of gravity (downflow in the
downer), axial solids dispersion is very small and the flow pattern approaches plug
flow; when the flow is against gravity (upflow in the riser), axial solids dispersion is
significantly larger and the flow pattern deviates significantly from plug flow. Solid
mixing is found to be mainly due to the dispersion of dispersed particles in the
downer; however, in the riser, both the dispersion of dispersed particles and particle
clusters were co-existed in the riser.. In both the riser and the downer, the dispersion
of the dispersed particles is very small, indicating that dispersed particles pass
through the system in a near plug flow pattern. Dispersion due to particle clusters in
the riser, on the other hand, is very significant, contributing to the large axial solids
backmixing and the bimodal solids residence time distribution in the riser.
CONCLUSIONS
Development of fluidization technique has spanned several decades, attesting to the

importance of this technique in chemical engineering, thermal engineering, and
metallurgy. When nanostructured granular materials were used for fluidization, some
kinds of nanoparticles (such as SiO2, carbon nanotubes) are agglomerated into
multi-stage agglomerates for stable fluidization. The structure of the agglomerates as
well as their size, apparent weight and the interactive forces between them
significantly influence the hydrodynamic behavior of agglomerating fluidization. The
concept of a particle spy was tested in the form of an encapsulated prototype PMS
was proposed to in situ detect the phase structure of fluidized bed. The axial and
radial solids dispersion coefficients were both two orders of magnitude lower than
those in FCC systems. Based on the scientific understanding of nanomaterials
fluidization, the fluidization process was successfully employed for nanomaterial
(both agglomerated and aligned CNT) production. Multi-functional nanostructures,
such as hierarchical SAPO-34 zeolite, were employed as advanced catlaysts for
catalytic fluidized bed route for methanol to olefin process. Novel fluidized bed
reactor, such as the novel riser-downer coupling reactor for the FCC process and a
two-stage fluidized-bed for gas-phase catalytic hydrochlorination of acetylene, were
11
also proposed. More efforts should be pain on new scientific challenges for
nanomaterials fluidization and novel industrial process for nanomaterial production
and (nano)structure enhanced fluidization technology for advanced materials, novel
chemical production, and energy conversion.
REFERENCES
1. F. Wei, et al., Powder Technol 2008, 183, 10-20.

2. Y. Wang, et al., Powder Technol 2002, 124, 152-159.
3. H. Yu, et al., AIChE J 2006, 52, 4110-4123.
4. Q. Zhang, et al., Particuology 2009, 7, 175-182.
5. a) C. Huang, et al., Powder Technol 2006, 161, 48-52; b) C. Huang, et al.,
Powder Technol 2008, 182, 334-341.
6. Y. Wang, et al., Chem Phys Lett 2002, 364, 568-572.
7. Y. Hao, et al., Carbon 2003, 41, 2855-2863.
8. Y. Liu, et al., Carbon 2008, 46, 1860-1868.
9. a) M. Q. Zhao, et al., Carbon 2010, 48, 3260-3270; b) M. Q. Zhao, et al., Adv
Funct Mater 2010, 20, 677-685.
10. a) Q. Zhang, et al., J Phys Chem C 2007, 111, 14638-14643; b) J. Q. Huang, et
al., Nanotechnology 2008, 19, 435602; c) J. Q. Huang, et al., Nanoscale 2010,
2, 1401-1404.
11. Q. Zhang, et al., Carbon 2008, 46, 1152-1158.
12. a) Q. Zhang, et al., Mater Chem Phys 2008, 107, 317-321; b) K. Zhou, et al.,
Nanoscale Res Lett 2010, 5, 1555-1560.
13. a) Q. Zhang, et al., Angew Chem Int Ed 2010, 49, 3642-3645; b) M. Q. Zhao, et
al., J Am Chem Soc 2010, 132, 14739-14741.
14. Q. Zhang, et al., Adv Mater 2009, 21, 2876-2880.
15. a) Q. Zhang, et al., Carbon 2009, 47, 2600-2610; b) Q. Zhang, et al., Carbon
2010, 48, 1196-1209.
16. a) Q. Wen, et al., Adv Mater 2010, 22, 1867-1871; b) Q. Wen, et al., Chem
Mater 2010, 22, 1294-1296.
17. L. S. Fan, Chemical Looping Technology for Fossil Energy Conversions, John
Wiley, 2010.
18. X. B. Wei, et al., Ind Eng Chem Res 2009, 48, 128-133.
19. J. Zhu, et al., Chem Commun 2009, 3282-3284.
20. H. Q. Zhou, et al., Appl Catal A-gen 2008, 348, 135-141.
21. a) R. S. Deng, et al., Ind Eng Chem Res 2005, 44, 1446-1453; b) H. Liu, et al.,
Ind Eng Chem Res 2005, 44, 733-741; c) F. Liu, et al., Ind Eng Chem Res 2008,
47, 8582-8587; d) Y. Cheng, et al., Powder Technol 2008, 183, 364-384.
12
A MODELING STUDY OF GAS STREAMING IN A DEEP FLUIDIZED
BED OF GELDART GROUP A PARTICLES
Shayan Karimipour, Todd Pugsley1
Department of Chemical Engineering, The University of Saskatchewan,
57 Campus Drive, Saskatoon, SK, Canada S7N 5A9
1
Corresponding author (todd.pugsley@usask.ca),
Tel.: (+1-306) 966-4761, Fax: (+1-306) 966-5205
ABSTRACT
Gas streaming has been modeled in a deep fluidized bed of 5 m depth and 0.3 m inside
diameter. The model results suggest that the lower pressure drop of the stream zone compared
to the remainder of the bed is the reason for severe streaming flow in deep beds. The effects of
different parameters such as bed depth, gas velocity and particle size on the severity of the
streaming flow are also evaluated with the model.
INTRODUCTION
Several studies in the past decade have demonstrated that in sufficiently deep fluidized beds
(i.e. beds approaching a depth of 1 m or greater) of Geldart Group A particles (1), gas
bypassing may occur by increasing the superficial gas velocity (2-6). When this phenomenon
occurs, the fluidizing gas bypasses the bed in the form of streams of gas, leaving a large
fraction of the bed unfluidized or poorly fluidized. The concept of gas streaming was first
reported in the literature by Wells (2). He performed several experiments in large scale units
with up to 2.5 m diameter and 5 m bed depth and observed streaming flow under conditions that
were expected to lead to operation in the bubbling regime. He attributed the streaming
phenomenon to gas compression, caused by the pressure head of the deep solids bed over the
distributor.
Karri et al. (3) investigated the formation of streaming flow in a column of 0.3 m inner diameter
and 4.9 m height. They found that for all combinations of operating conditions investigated, the
addition of a sufficient amount of fines to the bed of Geldart Group A particles was able to delay
the streaming. In another work, Issangya et al. (4) used several pressure transducers mounted
at various radial positions to detect the presence of streaming flow.
Recently, Karimipour and Pugsley (5) have performed a systematic study on the streaming flow
in deep beds of FCC particles. They discussed the effects of streaming flow on the pressure
fluctuations time series measured in the fluidized bed for different combinations of bed depth,
gas velocity, particle size, and distributor design. They concluded that streaming flow does not
appear suddenly, but emerges gradually in the bed by increasing the bed depth. They found
that although changing parameters such as superficial gas velocity and/or fines content can
1
reduce the severity of the streaming flow, streaming is the dominant phase for deep fluidized
beds operating at gas velocities where a fully bubbling bed regime would normally be
anticipated.
The only mathematical model to predict the onset of gas streaming is that of Wells (2). Wells (2)
concluded that when the ratio of the density at minimum fluidization to the density of the
emulsion phase becomes less than a critical value for a given bed depth, streaming occurs. The
model of Wells (2) was tremendously valuable for improving the understanding of streaming, but
it was not a direct function of operating conditions such as bed depth and gas velocity. The
objective of the present work is to develop a simple phenomenological model for the streaming
flow and to use the model to evaluate the effect of bed depth, gas velocity, and particle size.
MODEL DEVELOPMENT
Based on our finding from a separate experimental campaign (e.g. 5), the deep fluidized bed is
divided into two adjacent regions in which the smaller region is occupied by the stream flow and
the other region is assumed to be at minimum fluidization conditions. It is assumed that by
increasing the superficial velocity the gas in excess of that required for minimum fluidization is
directed into the stream zone. Also based on our experimental observations, the cross section
of the gas stream is assumed to be circular and its diameter to be less than one fourth of the
bed diameter. The stream therefore forms a vertical cylinder of constant diameter along the
fluidized bed. A small lateral zone above the distributor is reported to be better fluidized (2) and
gas and particles from other parts of the distributor find their way towards the stream and move
upward through the stream. As such, particles can be assumed to move upward only in the
stream and after discharging at the surface of the bed slowly return to the bottom through the
non-streaming region.
Similar to the acceleration zone of a circulating fluidized bed riser (6, 7), the stream can be
modeled by a force balance over a single particle inside the stream:
2
dυ p 1 ⎛u ⎞
ρ pV p = ρ g ⎜ st − υ p ⎟ Ap CD − ( ρ p − ρ g )V p g (1)
dt 2 ⎜⎝ ε g ⎟
⎠
Assuming the particles as spheres of constant diameter, and incorporating Eq. 2 from the
derivative theory, the force balance equation can be re-written as Eq. 3:
dυ p dυ p
=υp (2)
dt dz
2
dυ p 3ρ g CD ⎛ ust ⎞ g
= ⎜⎜ − υ p ⎟⎟ − (ρ p − ρg ) (3)
dz 4d p ρ pυ p ⎝ ε g ⎠ ρ pυ p
We have estimated the drag coefficient, CD, in Eq. 3 based on the correlation of Mostoufi and
Chaouki (8). The porosity in these equations is calculated from the solids mass balance
equation as follows:
Gp = ρ p (1 − ε g )υ p (4)
The initial value of the particle velocity at the bottom of the stream is obtained from the solids
mass balance. Thus, Eq. 3 will be solved subject to the following initial condition:
Gp
υp = (5)
z =0 ρ p (1 − ε mf )
2
Once the axial profile of particle velocity in the stream is determined from Eq. 3, the
corresponding solids holdup can be calculated from
ε p = 1− ε g (6)
The axial profile of the pressure drop along the stream can be determined from the momentum
balance over the stream. The momentum balance could be expressed as follows:
dp ⎛ dp ⎞ ⎛ dp ⎞ ⎛ dp ⎞
= ⎜ ⎟ +⎜ ⎟ +⎜ ⎟ (7)
dz ⎝ dz ⎠ head ⎝ dz ⎠ acceleration ⎝ dz ⎠ friction
where
⎛ dp ⎞
⎜ ⎟ = ρ pε p g + ρ g ε g g (8)
⎝ dz ⎠ head
⎛ dp ⎞ dυ p u d ⎛ ust ⎞
⎜ ⎟ = ρ pε pυ p + ρ g ε g st ⎜ ⎟⎟ (9)
⎝ dz ⎠ acceleration dz ε g dz ⎜⎝ ε g ⎠
The pressure drop caused by friction includes two sources, i.e., gas-wall and particle-wall
frictions:
⎛ dp ⎞ ⎛ dp ⎞ ⎛ dp ⎞
⎜ ⎟ =⎜ ⎟ +⎜ ⎟ (10)
⎝ dz ⎠ friction ⎝ dz ⎠ gas − wall ⎝ dz ⎠ particl − wall
These pressure losses are defined by the Fanning equation as
⎛ dp ⎞ 1 ust2
⎜ ⎟ = f ρ (11)
⎝ dz ⎠ gas − wall
g
2d st
g
εg
⎛ dp ⎞ 1
⎜ ⎟ = fp ρ pε pυ p2 (12)
⎝ dz ⎠ particle − wall 2d st
Since gas-wall and particle-wall frictions form a minor portion of the overall pressure drop, type
of the friction factor does not have a major effect on the results. Here, the gas-wall friction
factor, fg, has been calculated from the Blasius formula (9)
0.316
fp = , Reg ≤ 105 (13)
Reg0.25
and the particle-wall friction factor has been estimated using the correlation of Kanno and Saito
(10)
0.057
fp = ( gd st )
1/ 2
(14)
2υ p
The wall in our case corresponds to the “wall” of the cylindrical stream in the bed. In order to
solve these equations, the solid circulation rate (Gp) is needed as an input. Since the system is
not a real circulating fluidized bed, a pseudo-circulating rate may be calculated from the
correlations proposed for the internally circulating fluidized bed. An internally circulating fluidized
bed resembles the current case in that both of the systems involve flow of gas and solids
between a fluidized bed at minimum fluidization conditions and a dilute bed (a riser in an
internally circulating fluidized bed and a stream in the current case). The net rate of the particle
exchange between two zones along the fluidized bed is considered to be trivial. The correlation
of Jeon et al. (11) has been used for this purpose:
0.795
⎛u ⎞
0.728
⎛ dp ⎞
ΔPor = 5.327 × 10 ⎜ st 3
⎟⎟ ⎜ ⎟ (15)
⎜u
⎝ mf ⎠ ⎝ d or ⎠
3
Sor
Gp = Cdis 2 ρ p (1 − ε mf )ΔPor (16)
Sst
In the above equations, the orifice refers to that point at the bottom of the bed that allows for the
exchange of gas and particles between the stream and non-streaming zones.
For the pressure drop through the none-streaming zone which is considered to be at minimum
fluidization conditions, the pressure drop is assumed to be due to the mass of the particle bed:
dp
= ρ p g (1 − ε mf ) (17)
dz
RESULTS AND DISCUSSIONS
The model predictions of pressure drop along the fluidized bed for a bed depth of 5 m are
provided in Fig. 1. As can be seen in the figure, the model predicts a lower pressure drop
immediately above the distributor for the non-stream zone compared to the case of the stream
zone. Therefore, streams do not form in this region. However, the stream pressure drop
decreases dramatically with increasing distance from the distributor, which makes the streams a
preferable pathway for the gas. The higher pressure drop of the stream immediately above the
distributor is due to the much higher flow of gas and particles in the stream compared to the
non-stream zone. Similar trend of pressure drop has been reported for the bottom of FCC risers
(7, 8). As illustrated in the figure, as the upper surface of the bed is approached, the difference
between the pressure drop of the streaming and non-streaming zones decreases. The result of
this would be that preferential flow of gas through the stream would be diminished, allowing gas
to diffuse into other parts of the bed and provide more uniform fluidization at upper regions. This
is consistent with visual observations from experiments, which showed improved fluidization at
the upper regions of the bed.
5 Non-Stream Zone
Stream Zone
Axial Position (m)
0
0 5000 10000 15000 20000 25000 30000 35000
Pressure Drop (Pa)
Figure 1. Axial profile of the pressure drop in the fluidized bed, Bed depth = 5 m, Superficial gas
velocity = 0.2 m/s, Particle diameter = 84 microns
4
Effect of Bed Depth
Fig. 2 illustrates the differences between the pressure drops of stream and non-stream
pathways at the bottom of the fluidized bed for different bed depths. As can be seen, the
difference in the pressure drops of the two zones, which is considered to be the motivation for
the formation and stability of the streams, increases with increasing bed depth. Experimentally
we found that the onset of streaming flow occurred gradually in the fluidized bed as bed depth
was increased. According to the model results, this can be attributed to the gradual increase of
the difference in pressure drop between the streaming and non-streaming zones. This
difference is probably low enough in shallow beds that the gas is able to fluidize all of the cross
section and prevents the formation or permanence of streaming flow.
Effect of Gas Velocity
Fig. 3 provides the axial profile of the pressure drop in the fluidized bed for different superficial
gas velocities. As Fig. 3 illustrates, two changes occur in the fluidized bed by increasing the gas
velocity. Firstly, the difference between the pressure drops of the streaming and non-streaming
zones decreases and secondly, the region expands above the distributor where streaming is not
preferred or present. The positive influence of increasing the gas velocity on diminishing the
streaming flow has been emphasized in all of the previous experimental works in the literature
(2-6). As the figure indicates, at gas velocities higher than 1 m/s streaming flow is not preferred
anywhere in the fluidized bed and uniform fluidization would be possible throughout the bed.
20000
of Stream and Non-Stream zones at the
Difference between the pressure drop
16000
bottom of the bed (Pa)
12000
8000
4000
0
0 1 2 3 4 5 6
Bed Depth (m)
Figure 2. Difference between the pressure drop of Stream and Non-Stream zones at the bottom
of the bed for different bed depths, Superficial gas velocity = 0.2 m/s, Particle diameter = 84
microns
5
6
Non-Stream Zone
5 Stream Zone, U0 = 0.2 (m/s)
Axial Position (m) Stream Zone, U0 = 0.4 (m/s)
4 Stream Zone, U0 = 0.6 (m/s)
Stream Zone, U0 = 0.8 (m/s)
3 Stream Zone, U0 = 1 (m/s)
Stream Zone, U0 = 1.2 (m/s)
0
0 10000 20000 30000 40000 50000
Pressure Drop (Pa)
Figure 3. Axial profile of the pressure drop in the fluidized bed for different superficial gas
velocities, Bed depth = 5 m, Particle diameter = 84 microns
Effect of Particle Size
Fig. 4 illustrates the axial profile of the pressure drop in the fluidized bed for different particle
sizes and a constant particle density of 1400 kg/m3. As can be seen, the pressure drop in the
stream increases by increasing the particle size. Thus, its preference as an alternative pathway
with lower pressure drop for gas decreases gradually. According to the literature, streaming flow
has only been reported for Geldart Group A particles; it does not appear to exist for coarser
Geldart B particles (2-6). Thus, as the model predicts, the fluidized bed of these particles display
uniform fluidization. The results show that the model is able to predict this directional effect of
increasing particle size.
Effect of Stream Size
The effect of the size of stream zone (i.e. stream diameter) on the axial profile of pressure drop
has also been investigated (results not shown due to space constraints). Our model predicts
that decreasing the stream size from 1/4 to 1/8 of the bed diameter reduces the preference of
streaming as an alternative pathway for gas flow.
CONCLUSIONS
In the present work, gas streaming flow has been modeled in a deep fluidized bed of 5 m bed
depth and 0.3 m diameter. The trend of the model predictions have been qualitatively compared
and validated with the experimental findings. The model is based on the assumption that the
stream already exists in the bed. The initiation of streaming flow has been discussed in our
previous work (6). According to that work, the potential for streaming always exists in a fluidized
bed. The results of the present work suggest that what causes a severe streaming flow with
increasing bed depth is probably the gradual increase of the difference between pressure drop
of two zones: that smaller portion of the bed where streaming becomes preferred and the
remainder of the bed at minimum fluidization. Our model results show that increasing the bed
6
depth favors the streaming flow, while increasing the gas velocity increases the uniformity of the
bed and decreases the streaming severity. Streaming flow was found to be less severe for
larger particle sizes. All of these findings are in conformity with experimental investigations
reported previously in the literature.
6
Non-Stream Zone
Stream Zone, Particle Ave. Diam. = 42 microns
5
Axial Position (m)

4
0
0 5000 10000 15000 20000 25000 30000 35000
Pressure Drop (Pa)
Figure 4. Axial profile of the pressure drop in the fluidized bed for different particle sizes, Bed
depth = 5 m, Superficial gas velocity = 0.2 m/s
NOTATION
Ap cross-sectional area of particle (m2)

Ar Archimedes number ( d 3p ρ g ( ρ p − ρ g ) g / μ 2 )
Cdis gas discharge coefficient
CD effective drag coefficient
dp particle diameter (m)
dst stream diameter (m)
D fluidized bed diameter (m)
f drag coefficient correction factor
fp solid-wall friction factor
fg gas-wall friction factor
g acceleration of gravity (m/s2)
Gp solids flux (kg/m2s)
p pressure (Pa)
∆Por orifice pressure drop (Pa)
Reg gas Reynolds number (D U0 ρg/μg)
Sor orifices cross sectional area (m2)
Sst stream cross sectional area (m2)
t time (s)
umf minimum fluidization velocity (m/s)
ust gas velocity in stream (m/s)
vp particle velocity (m/s)
7
Vp particle volume (m3)
z fluidized bed height above distributor (m)
Greek Letters
εg gas voidage
εp gas voidage
εmf voidage at minimum fluidization
ρg gas density (kg/m3)
ρp particle density (kg/m3)
μ gas viscosity (Pa∙s)
REFERENCES
[1] D. Geldart, Types of gas fluidization, Powder Technology 7 (1973) 285-292

[2] J. Wells, Streaming flow in large scale fluidization, Paper presented at the AIChE annual
meeting, Particle Technology Forum, Reno, Nevada, USA, 2001.
[3] S. B. R. Karri, A. S. Issangya, M. Knowlton, Gas bypassing in deep fluidized beds, In
Fluidization XI, U. Arena, R. Chirone, M. Miccio, P. Salatino, eds., Ischia (Naples), Italy, 9-14
May 2004.
[4] A. Issangya, T. Knowlton, S. B. R. Karri, Detection of gas bypassing due to jet streaming in
deep fluidized beds of group A particles, In Fluidization XII, F. Berruti, X. Bi, T. Pugsley, eds.,
Vancouver, British Columbia, Canada, 13-17 May 2007.
[5] S. Karimipour, T. Pugsley, Study of gas streaming in a deep fluidized bed containing Geldart’
Group A particles, Chemical Engineering Science 65 (2010)
3508–3517.
[6] T. S. Pugsley, F. Berruti A predictive hydrodynamic model for circulating fluidized bed risers,
Powder Technology 89 (1996) 57-69
[7] Sh. Karimipour, N. Mostoufi, R. Sotudeh-Gharebagh, Modeling the hydrodynamics of
downers by cluster-based approach, Ind. Eng. Chem. Res. 45 (2006) 7204-7209
[8] N. Mostoufi, J. Chaouki, Prediction of effective drag coefficient in fluidized beds, Chemical
Engineering Science 54 (1999) 851-858
[9] R. W. Fox, A. T. McDonald, P. J. Pritchard, Introduction to fluid mechanics, 6th ed.; Wiley:
New York, 2003
[10] H. Kanno, S. Saito, Pneumatic conveying of solid through straight pipes, J. Chem. Eng.
Jpn. 2 (1969) 211-217
[11] J. H. Jeon, S. D. Kima, S. J. Kim, Y. Kang, Solid circulation and gas bypassing
characteristics in a square internally circulating fluidized bed with draft tube, Chemical
Engineering and Processing 47 (2008) 2351-2360
8
EFFECTS OF PARTICLE PROPERTIES ON CLUSTER
CHARACTERISTICS IN A 2-D CFB RISER
Jing Xu and Jesse Zhu*

Particle Technology Research Centre, Department of Chemical & Biochemical Engineering,
The University of Western Ontario, London, Ontario, Canada N6A 5B9
*Corresponding author. Tel.: +1 519 661 3807; fax: +1 519 850 2441; email address: jzhu@uwo.ca (J. Zhu)
ABSTRACT
The characteristic of particle clusters was studied in a 2-D circulating fluidized bed
riser by using a digital image system and optical fiber probes. A new parameter,
cluster number fraction, was proposed to characterize the clusters. The results
indicated the smaller and lighter particles have higher potential to aggregate, while
the effects of particle sphericity were less significant than those of particle density
and size.
INTRODUCTION
The analysis of the micro structure of the gas-solid two phases is considered
complex and remains unclear. The micro flow structure is usually identified as the
behavior of clusters, which are defined as dense clouds of particles having
significantly more particles per unit volume than the surrounding dilute regions (1).
Since the particles in CFB tend to aggregate and form clusters, which flow quite
differently from a single particle, the gas-solid flow in CFBs is often characterized by
the existence of particle aggregates or clusters (1, 2).
Most of the researchers (1-5) used the visualization technique and intrusive probe to
obtain the micro flow behaviors. However, the visualization technique they used was
restricted to dilute flow. In addition, almost all of the former studies appear to conduct
the investigation within one type of particles, and very few references can be found
clarifying the effects of particle properties on the cluster characteristics. Since
previous studies (6, 7) have revealed that a strong dependence of the particle
properties on the solids concentration and particle velocity, the particle properties,
including particle density, size and sphericity may play an non-negligible role in
affecting the cluster properties. In this study, various types of particles with typical
different density, size or sphericity were taken into consideration. Moreover, very few
studies have been carried out to investigate the cluster properties by combining the
visualization with intrusive probes. In this study, we applied high-speed video camera
and optic fiber probes in a 2-D circulating fluidized bed, to connect the two different
measurements and make both function better. This study also realized the
visualization technique to be effectively used under high solids concentration (Gs is
up to 200 kg/m2s).
EXPERIMENTAL APPARATUS
All experiments were carried out in a rectangular circulating fluidized bed which is
illustrated schematically in Figure 1. The riser is a rectangular column with 7.6 m
height and 19 mm × 114 mm (0.75 in × 4.5 in) cross-section.
The visualization system was self-designed and set up. To eliminate the entrance
and exit effects, the system was mounted focusing on the upper fully developed
region, where Z = 5m. The system consists of a light source, a high-speed video
camera and programs for digital image analysis (Figure 2). The speed of the high-
speed video camera is up to 16,000 fps. A MATLAB program was used to allow the
images to be analyzed frame by frame. The probe chosen to measure the local
solids concentration in this study was optical fiber probe, which is capable of
measuring the solids concentration with a reliable pre-calibration (1, 8, 9). The solids
concentrations were measured at 9 lateral positions and 6 axial levels along the
entire riser. The instantaneous solids concentration was analyzed by a self-
developed FORTRAN program which introduces sensitivity analysis to identify the
clusters from solid concentration signals.
Images Face Wall

Monitor Diffuser
Panel
Video Camera
Images
Analysis Lamp
CFB Riser Side Wall
Figure 1 Circulating fluidized bed unit and Figure 2 Sketch of Visualization system
schematic of riser cross section
The properties of the particles used in this study are listed in Table 1. The materials
were selected in order to investigate the effects of particle size, density and
sphericity, respectively. In this study, the solids concentration measurement was
conducted under the operating conditions of Ug = 3 ~ 8 m/s, and Gs = 50 ~ 200
kg/m2·s. The high-speed videos were recorded simultaneously under the
corresponding operating conditions at 2000 fps.
Table 1 Properties of particles used
Particles FCC Glassbeads #1 Glassbeads #2 Glassbeads #3 Sand

Particle Sauter mean
67 76 134 288 138
diameter, μm
Particle density, 1877 2453 2403 2498 2467
3
kg/m
3
Bulk density, kg/m 1125 1434 1421 1475 1453
Sphericity, - 0.95 ~1 ~1 ~1 0.65~0.75
Particle terminal
0.26 0.42 1.19 3.73 N/A
velocity, m/s
RESULTS AND DISCUSSION
Observation and Description of Clusters

Generally, the solids flowing in the riser were observed to distribute dense in wall
regions and dilute in the center. The particles were moving faster in the column
center and slower towards the wall. Nearly no appearance of solids buildup or falling-
down was observed on either of the face walls.
Cluster Forms
Figure 3 shows an image sequence with a solid cluster moving upwards in the center
region of the riser. The frames (window size of 46.6 mm × 13.5 mm) were taken at a
recording rate of 2000 fps and an exposure time of 500 μs. The movement and
development of the cluster can be recognized as the darker structure which is
visualized directly within the observed area. The sequence of images clearly show
that a U-shape cluster is formed with a round nose facing downward and a core on
the “nose tip”, where it is much darker than the peripheral area. Initially, the cluster is
moving as a longish core with blurred boundary. Continuously, the core is stretched
to be longer and crotched. Since the cluster is moving slower, the dispersed particles
passing by are blocked and adhere to the cluster. Therefore, the U-shape outline is
clearer and the core is darker and bigger with the aggregating of particles. In this
study, the U-shape cluster is the most common form of clusters observed in the riser
center.
As observed, the clusters exist as U-shape, longish strand and other cluster
structures. The pictures of the clusters shown in Figure 4 are for different particles
under several typical operating conditions. As mentioned above, the U-shape is the
most common structure viewed in the riser center. Some of them have a core with
particular high solids concentration at the nose tip, while the others don’t. The
opening of the U-shape cluster faces upward or downward with a size range from 5
cm to 30 cm, most are smaller than 20 cm. The longish strand cluster is the cluster
form also often observed in the core region of the riser. The size of the strand cluster
is approximately 10 mm in width and 10 cm to 50 cm in length. The motion of this
form of cluster is slower than other particles in the vicinity. Occasionally, some
clusters in small size (1-2 cm), and in shapes of circle, short stripe (as shown in
Figure 4(c)) or crescent are observed. They are always seen to flow as fast as the
adjacent non-aggregative region. In addition, the shape of these types of clusters is
nearly constant during the motion in the observation window. Besides the forms of
individual clusters aforementioned, clusters in different structures may adhere
together to form floc-like clusters. The most common combination seen is between
the U-shape and the strand clusters, typically shown in Figure 4(d), (e) and (f).
Figure 3 Sequence of 12 images taken in the core region with a U-shape cluster
(a) (b) (c) (d) (e) (f)

Figure 4 Cluster structures observed in the riser center under different operating conditions: (a)
Glassbead #3, Gs = 100 kg/m2·s, Ug = 5 m/s; (b) Glassbead #3, Gs = 100 kg/m2·s, Ug = 8 m/s; (c) Sand,
Gs = 100 kg/m2·s, Ug = 5 m/s; (d) Glassbead #1, Gs = 100 kg/m2·s, Ug = 5 m/s; (e) Glassbead #1, Gs =
150 kg/m2·s, Ug = 5 m/s; (f) FCC, Gs = 100 kg/m2·s, Ug = 5 m/s
Effects of Particle Properties on Cluster Forms

Five different types of particles were employed in this study. The effects of particle
density, size and sphericity on the clusters behaviors were compared. All the images
in Figure 4 are in the size of 256 pixel ×880 pixel with a scale of 1.99×10 -4 m/pixel. In
Figure 4(a) and (b), Glassbead #3 with a mean size of 288 μm is seen to form
clusters typically in U or strand shape and with a large cluster size. The Sand
particles having particle diameter 134 μm and approximate 0.7 sphericity are
observed to have the flow structure indistinguishable from the Glassbead #3, while
small size clusters can be found occasionally. With further decreasing of particle size
to 76 μm for Glassbead #1, the form of clusters turns to be more complicated and
interconnective. It is seen that the clusters are smaller in size than that of the larger
particles, and tend to connect together with each other. Therefore, the individual
cluster is difficult to be identified in small size particle flow. Compared with the flow of
Glassbead #1 (2453 kg/m3), the structure of clusters is more intricate and irregular
when lighter FCC particles (1877 kg/m3) were used, as shown in Figure 4(f). The
area with darker color, which is occupied by the clusters, is obviously larger than the
area in lighter color. In other words, - a great amount of particles are seen moving in
aggregating form and few particles are left to move individually. The size and form of
individual cluster is unlikely to be identified since the interconnection among the
highly populated clusters is very intense. The observation indicates that the smaller
and the lighter particles have higher potential to aggregate than the larger and
heavier particles, whereas, the effect of particle sphericity cannot be distinguished
here.
Characterizing Clusters with Optical Fiber Probe

To identify clusters with reflective probes applied, a set of criterion must be satisfied.
Based on the previous studies, it is suggested that (3, 10): (1) the solids
concentration inside the cluster must be n-times the standard deviation of the
sampled signal over the local time-mean solids concentration; (2) the number of
consecutive samples above the critical solids concentration, Ns, must be set to
determine the minimum time interval for the perturbation caused by a cluster; (3) the
sampling volume must be greater than one to two orders of particle diameter.
Furthermore, it is found in this study that the sampling frequency of solids
concentration signal is another sensitive criterion to establish the cluster properties.
The sampling frequency in this study is placed very high, at 100 kHz, which allowed
high sensitivity to the solids concentration.
1.0
Ns = 30
FCC, y/Y = 0
Ug = 5.5 m/s FCC, y/Y = 0.5
0.8
Gs = 100 kg/m s
2 FCC, y/Y = 0.98
Large size cluster fraction
GB #1, y/Y = 0
GB #2, y/Y = 0
0.6 GB #3, y/Y = 0
Sand, y/Y = 0
0.4
0.2
0.0
0 50 100 150 200 250 300 350 400
Ns
Figure 5 Cluster number fraction vs. Ns
Subjecting to the difference of sampling frequency among various studies, the

optimal values for both n and Ns are required to be determined individually. The
sensitivity analysis, firstly introduced by Manyele et al. (3), is adopted in this study to
optimize the value for n. Consequently, n=2 is finalized as optimal critical solids
concentration. Then, such method is further improved to identify Ns. A new
parameter, cluster number fraction, Flc, is proposed for the first time to characterize
clusters. Flc is defined as Flc  Nlc N c , where Nc is the total number of perturbations
with the solids concentration higher than the critical value over the time series
studied; while Nlc is the number of perturbations with Ns consecutive samples above
the critical solids concentration. Considering the cluster number fraction as a sample
parameter for the sensitivity analysis, an increase/decrease of Ns would lower/raise
the fraction of clusters with existence time longer than Ns sampling time interval.
Some of the perturbations of solids concentration are very small and with short time
intervals, therefore, they are classified as part of the dispersed particulate phase.
Since such small perturbations are numerous, there tends to be a decrease of Flc
with the increase of Ns. As shown in Figure 5, there is a sharp change at Ns = 30,
which is the critical value that demarcates the particulate phase and the clusters. In
addition, single critical Ns is also applicable to different types of particles and multiple
lateral positions under specific operating condition.
Cluster Number Fraction (Flc)

It is found that Flc can not only be used to determine the optimal value for Ns, but also
characterizes the effects of particle properties on the aggregates. Since Ns is the
number of consecutive samples, with a sampling frequency, it can be easily
transfromed to the minimum time interval, Tc, set for the perturbation caused by a
cluster.
Since the clusters are irregular in shape and vary both laterally and axially within a
riser, the accurate definition of the cluster size is impossible. Therefore, the vertical
length is usually used to identify the size of clusters. Since the time interval of the
solids concentration perturbation measured by the optical fiber probe represents the
traveling time of a cluster passing through a probe tip, it is feasible to calculate the
cluster vertical length with dvl  Vc  Tc , where Vc is the vertical velocity of cluster
(11). With the evaluation of the cluster velocity, it is possible to obtain the size of
clusters in the riser. To some extent, the cluster number fraction reflects the
distribution of cluster size.
Figure 6 plots Flc against minimum time interval to elucidate the cluster
characteristics of different particles. Figure 6(a) interprets the fractions of cluster
number at different lateral positions. The Flc at the riser center region (y/Y = 0),
middle region (y/Y = 0.5) and wall region (y/Y =0.98) are seen decrease with the
increase of minimum time interval. In other words, with increasing Tc set for a cluster,
the number of clusters with the transit time longer than the criterion decreases. It can
also be seen that the decreasing curves of y/Y =0 and y/Y = 0.5 are almost
overlapping and cross approximately at Tc = 1.1×10-3 µs. Below this value, the cluster
number fraction at y/Y =0 is larger than that at y/Y = 0.5, while smaller when beyond
the point. The curve for the wall region with y/Y = 0.98 is obviously above the other
two, meaning that the population of clusters in the wall region is larger than that in
the center or middle region. Due to the wall friction, the particle velocity is low on the
wall, which increases the tendency of forming clusters and the probability of
existence for clusters.
Figure 6(b) compares Flc of particles with different mean size. It is found that under
identical Tc, the Flc of smaller size particles is greater than that of larger particles. It
shows that the finer particles are prone to aggregate and incline to form clusters. It is
agreed well with the observations in the section 3.2. The finer particles (GB #1 or
FCC particles) were seen to form numerous clusters interconnecting with each other,
while only several huge size clusters were observed occasionally in the coarse
particles (GB #3 or Sand).
1.0 1.0
(a) (b)
Ug = 5.5 m/s
0.8 0.8 2
Gs = 100 kg/m s
Large size cluster fraction, Flc

Z = 5.33 m
0.6 0.6
FCC, y/Y = 0 GB #1 (dp = 76m), y/Y = 0

FCC, y/Y = 0.5 GB #2 (dp = 138m), y/Y = 0
0.4 0.4
FCC, y/Y = 0.98
GB #3 (dp = 288m), y/Y =0
0.2 0.2
-3
Tc=1.110 s
0.0 0.0
0.0 0.5 1.0 1.5 2.0 2.5 3.0 3.5 4.0 0.0 0.5 1.0 1.5 2.0 2.5 3.0 3.5 4.0
1.0 1.0
-3
(c) -3
Tc=0.4510 s
(d)
Tc=0.5510 s
0.8 0.8
Large size cluster fraction, Flc
0.6 0.6
0.4
3
FCC (p = 1877kg/m ), y/Y = 0 0.4
GB #2 ( s  1), y/Y = 0
3 Sand ( s 0.7), y/Y = 0
GB #1 (p = 2453kg/m ), y/Y = 0
0.2 0.2
0.0 0.0
0.0 0.5 1.0 1.5 2.0 2.5 3.0 3.5 4.0 0.0 0.5 1.0 1.5 2.0 2.5 3.0 3.5 4.0

Minimum time interval, T c, ( s) 
Minimum time interval, T c, ( s)
Figure 6 Cluster number fraction for different particles.
For the particles with different density, the curves of Flc against Tc cross
approximately at Tc = 0.55×10-3 µs, as the dotted line shown in Figure 6(c). Under the
given small time criterion, the fraction of clusters number for FCC particles is larger
than that of GB#1. With the increase of Tc, the clusters for heavier particles (GB #1)
are greater in fraction than for lighter particles (FCC) when Tc passes over the
marked dotted line. It indicates that the lighter particles tend to form smaller clusters
than the heavier particles. It is matched with the observations by high-speed films in
section 3.2.
The curves for particles with different sphericities are also observed in Figure 6(d)
when Tc = 0.45×10-3 µs. Same interpretation can also be applied to the different
sphericities particles: the more spherical particles incline to aggregate larger size
clusters than the irregular particles when Tc is beyond the value of the intersection
point. Below the marked line, the two curves are nearly overlapping, indicating that
the clusters fraction in each cut for both types of particles are almost the same. In
other words, the sphericity of particles has only minor effects on the small size
clusters but more obvious effects on the larger size clusters.
CONCLUSION
The particle aggregation characteristics were studied in a narrow rectangular CFB

riser with a 19 mm × 114 mm cross-section and a 7.6m length. The study was
conducted by operating FCC, glassbeads and sand particles under various operating
conditions. Forms of clusters were observed by employing a visualization system
with a high-speed video camera. The lighter and smaller particles tended to
aggregate and form interconnected clusters, while the effects of particle sphericity on
the form of clusters are less evident. The aggregation characteristics were also
studied with the optical fiber probe. A new parameter, the cluster number fraction,
was originally defined. The results obtained by analyzing the instantaneous solids
concentration agreed well with the observations and also indicate that the low
particle density and small particle size contribute to form clusters. It shows that the
particle sphericity plays a limited role in affecting the particle aggregation.
NOTATION
dp Sauter mean diameter of particle, m dvl Cluster vertical length, m

Flc Cluster number fraction Gs Solids circulation rate, kg/m2·s
Tc Minimum time interval for cluster, s Ug Superficial gas velocity, m/s
Vc Cluster vertical velocity, m/s Y Half of riser width, m
y Lateral coordinates Nlc Number of clusters
Nc Number of perturbations higher Ns Number of consecutive samples
than critical solids concentration above critical solids concentration
Z Height from riser bottom, m ρp Density of particle, kg/m3
Φs Particle sphericity
REFERENCES
1. Bi, H.T., J.X. Zhu, Y. Jin, and Z.Q. Yu. Forms of particle aggregations in CFBs. in
Proceedings of the Sixth Chinese Conference on Fluidization. 1993. Wuhan,
China.
2. Soong, C.H., K. Tuzla, and J.C. Chen. Experimental determination of cluster size
and velocity in circulating fluidized bed. in Fluidization VIII. 1995. New York:
Engineering Foundation.
3. Manyele, S.V., J.H. Pärssinen, and J.-X. Zhu, Characterizing particle aggregates
in a high-density and high-flux CFB riser. Chemical Engineering Journal, 2002. 88:
p. 151-161.
4. Li, H., Y. Xia, Y. Tung, and M. Kwauk, Micro-visualization fo clusters in a fast
fluidized bed. Powder Technology, 1991. 66: p. 231-235.
5. Hatano, H. and N. Kido, Microscope visualization of solid particles in circulating
fluidized beds. Powder Technology, 1994. 78: p. 115-119.
6. Mastellone, M.L., U. Arena, The effect of particle size and density on solids
distribution along the riser of a circulating fluidized bed. Chemical Engineering
Science, 1999. 54: p. 5383-5391.
7. Xu, J. and J. Zhu, Effects of particle properties on flow structure in a rectangular
circulating fluidized bed: solids concentration distribution and flow development.
Submitted to Chemical Engineering Science, 2011.
8. Zhang, H., P.M. Johnston, J.-X. Zhu, H.I. de Lasa, and M.A. Bergougnou, A novel
calibration procedure for a fiber optic solids concentration probe. Powder
Technology, 1998. 100: p. 260-272.
9. Liu, J., J.R. Grace, and X. Bi, Novel multifunctional optical-fiber probe I:
Development and validation. AIChE Journal, 2003. 49: p. 1405-1420.
10.Soong, C.H., K. Tuzla, and J.C. Chen. Identification of particle clusters in
circulating fluidized bed. in Circulating Fluidized Bed Technology IV. 1994. New
York: AIChE.
11.Li, H., Q. Zhu, H. Liu, and Y. Zhou, The cluster size distribution and motion
behavior in a fast fluidized bed. Powder Technology, 1995. 84: p. 241-246.
OXY-COMBUSTION OF DIFFERENT COALS IN A CIRCULATING
FLUIDIZED BED
Monika Kosowska-Golachowska1, Adam Luckos2, Konrad Klos1, Tomasz Musial1

1
Czestochowa University of Technology
Institute of Thermal Machinery
Armii Krajowej 19C, 42-201 Czestochowa, Poland
e-mail: kosowska@kkt.pcz.czest.pl
2
Sasol Technology R&D
1 Klasie Havenga Road, Sasolburg
PO Box 1, Sasolburg 1947, South Africa
e-mail: adam.luckos@sasol.com
ABSTRACT
Combustion of three Polish and one South African bituminous coal particles in air
versus O2/CO2 mixtures with oxygen concentrations in the range from 21% to 60%
vol. was conducted at temperature of 850°C in a 12 kW bench-scale CFB
combustor. Combustion in air was proceeded at ~50˚C higher centre temperatures
and was slightly shorter in time compared to combustion in O2/CO2 mixture with
21% vol. O2. Larger heat capacity of CO2 compared to that of N2 also retards the
ignition of volatiles in O2/CO2 mixtures with 21% O2. However, when the
concentration of oxygen in O2/CO2 mixtures is larger than 30%, the ignition time
decreases and surface and centre temperatures increase significantly with
increasing O2 content.
INTRODUCTION
Nowadays, greenhouse gases emissions from coal-fired systems, particularly CO2,

become more and more important. Oxy-fuel combustion is one of the promising
options for power generation with carbon dioxide capture. This technology can
reduce significantly emissions of NOx and improve the thermal efficiency of the
combustion process through the reduction of flue gas volume. In the oxy-fuel
combustion, coal particles are burnt in a mixture of pure oxygen and recycled flue
gas. Because nitrogen is eliminated from the oxidizing gas, the flue gas leaving the
combustion chamber is highly enriched in CO2 which means that the combustion
process takes place in an O2/CO2 environment. Partial recycling of flue gas helps to
control the flame temperature in the combustion chamber. Extensive studies in both
pilot-plant and lab scales have pointed out the pronounced influence of gas
composition (air versus O2/CO2) on coal combustion performance. The heat transfer
and temperature distribution in a furnace are greatly affected by the large specific
heat capacity of CO2. Coal ignition is delayed in O2/CO2 in comparison to in O2/N2
with the same O2 concentration. To match the flame/particle temperature in air,
a large amount of O2 in CO2, typically around 30%, is required. Coal conversion rate,
char properties, and reactivity are also affected by the replacement of air with an
O2/CO2 mixture, Zhang et al. (1). Buhre et al. (2) and Toftegaard et al. (3)
summarized the literature on oxy-fuel combustion of pulverized coal and discussed
a number of operational concerns, including ignition, heat transfer, environmental
issues and flame stability. Oxy-fuel combustion has now been well studied for
pulverized coal combustion, but to date has received relatively little attention for oxy-
fuel circulating fluidized bed combustion (CFBC), Jia et al. (4). Work in this field has
been conducted by: Foster Wheeler Energia Oy and VTT (5), ALSTOM (6),
CANMET (4) and Czestochowa University of Technology (7).
In the present work, oxy-fuel CFB combustion tests were conducted in a 12-kW
bench-scale CFB combustor. The main objective of this study is to investigate the
combustion behaviour of three Polish and one South African bituminous coal
particles, in air and O2/CO2 mixtures, in terms of particle temperature profiles,
ignition time, devolatilization time and the total combustion time.
EXPERIMENTAL
Oxy-CFB Combustor
Oxy-fuel combustion tests were conducted in a 12-kW bench-scale CFB combustor

shown schematically in Figure 1. The bench-scale CFBC consists of a combustion
chamber (1), a cyclone (2) a downcomer (3) and a loop seal (4). The electrically-
heated rectangular combustion chamber (riser), 680×75×35 mm, is the main
component of the unit. The front wall of the riser is made of transparent quartz
through which the combustion process can be directly observed.
Fig. 1. Schematic diagram of the experimental apparatus for oxy-CFB combustion

1-combustion chamber, 2-cyclone, 3-downcomer, 4-loop seal, 5-coal particle, 6-insulation, 7-drain
valve, 8-preheater, 9-card, 10-computer, 11-temperature measurement and control system, 12-gas
cylinders, 13-air compressor, 14-pressure regulators, 15-rotameters, 16-valves, 17-mixer, 18-gas
analyser, 19-ventilation duct, T1–T3-S-type thermocouples
Particles of silica sand between 100 and 400 μm, with d50=210 μm (d50, median
sand particles diameter, represents the size at which 50%, of the sand particles, by
weight, are smaller than the specified diameter), constitute the inert bed (see Figure
2 for the particle size distribution). Total mass of circulating solids is 0.3 kg. The
gases to make up gas mixtures are supplied from cylinders (12) to a mixer (17) and
then transferred via a preheater (8) directly into the combustion chamber. Flow rates
of gases are controlled by valves (16) and measured by rotameters (15). During
combustion tests, the superficial gas velocity was kept at a constant level
of about 5 m/s. The temperature was held at 850°C by means of microprocessor
thermoregulators (11). S-type thermocouples (T1–T3) measured the temperature at
three different levels inside the combustion chamber with an accuracy of ±2°C.
A single coal particle (5) was introduced into the combustion chamber and
positioned stationary in the bed. To measure the temperatures in the centre and at
the surface of the coal particle a special stand was constructed. It provides a
support for two S-type thermocouples. The tip of the first thermocouple was located
inside the particle, while the second thermocouple measured the surface
temperature and served as a basket in which the coal particle was places. The
thermocouples were connected via a card (9) to a computer (10) in order to record
the temperature measurements. Ignition time and devolatilization time were
measured by stopwatch with an accuracy of 0.1s. The intraparticle temperature, the
surface temperature, ignition time and devolatilization time were measured
simultaneously.
The experiments were carried out in air (base case) and mixtures of O2/CO2 with
oxygen concentrations in the range from 21% to 60% vol. Video and digital cameras
were used to record the progress of combustion.
a) b)
100
90
Cumulative mass fraction, %
80
70
60
50
40
30 d50 = 210 μm
20 ρs = 2620 kg/m3
10
0
0 100 200 300 400 500 600 700
dp, μm
Fig. 2. The bed material (silica sand): a) particle size distribution, b) SEM picture
Coals Tested
Particles of three Polish and one South African bituminous coal were used in this
study. Table 1 shows proximate, ultimate and petrographic analyses of these coals.
Spherical 10-mm particles were produced from coal lumps through mechanical
grinding.
Table 1. Proximate, ultimate and petrographic analyses of the coals tested
A B C D
Coal
Polish Polish Polish South African
Proximate analysis (%, air-dried basis)
Volatile Matter 30.9 30.9 28.9 23.7
Moisture 2.7 4.3 10.1 3.8
Ash 2.4 8.2 11.1 25.0
Fixed carbon 64.0 56.6 49.9 47.5
Calorific value (HHV), MJ/kg 32.38 31.31 24.66 22.44
Ultimate analysis (%, dry, ash-free basis)
Carbon 83.73 82.97 75.94 81.90
Hydrogen 4.59 5.14 4.59 3.44
Nitrogen 1.34 1.28 1.48 2.44
Sulphur 0.33 0.68 2,17 2.71
Oxygen (by difference) 10.01 9.93 15.82 9.51
Petrographic analysis, %
Vitrinite 52 88 59 14
Liptinite 9 2 12 0
Inertinite 39 6 21 68
Mineral matter 0 4 8 18
Results of proximate and petrographic analyses (Table 1) reveal that ash and
inertinite (maceral that is less reactive than vitrinite) contents in the South African
are much higher than those in Polish coals. Therefore, it can be expected that the
combustion behaviour of these coals may differ significantly. Thus, the main
objective of our study was to investigate the combustion behaviour of these coals, in
air and O2/CO2 mixtures, in terms of particle temperature profiles, ignition time,
devolatilization time and the total combustion time.
Figure 3 shows temperatures measured at the surface and in the centre of C and D
coal particles burned at 850˚C in air and in O2/CO2 mixture with 21% vol. O2. In both
cases, after an initial delay, the centre temperature exceeds the surface temperature
and stays approximately 100˚C during the course of combustion. Lower surface
temperatures can be explained by intensive heat transfer between burning coal
particles and bed material. Combustion in air proceeded at ~50˚C higher centre
temperatures and was slightly shorter in time compared to combustion in O 2/CO2
mixture with 21% vol. O2.
a) coal C b) coal D
1400 1400
1200 1200
Temperature, C
Temperature, C
1000 1000
800 800
600 600
air - surface air - surface
400 400
air - centre air - centre
200 21%O2 + 79%CO2 - surface 21%O2 + 79%CO2 - surface
200
21%O2 + 79%CO2 - centre 21%O2 + 79%CO2 - centre
0 0
0 200 400 600 800 1000 1200 1400 0 200 400 600 800 1000 1200 1400
Time, s Time, s
Fig. 3. Temperature profiles for coal C (a) and coal D (b) combusted in CFB in air
and 21%O2+79%CO2
As expected, the total combustion time, in both air and O2/CO2 mixture, for coal D
was much longer (~90%) than that for more reactive coal C.
Figure 4 illustrates the effect of oxygen content in O2/CO2 mixtures on surface and
centre temperatures measured for coals C and D. For both coals the trends are
similar; these temperatures increase significantly with increasing O2 concentration.
In the case of coal D, the maximum difference between the centre and surface
temperatures is larger than for coal C.
a) coal C b) coal D
1400 1400
1200 1200
1000 1000
Temperature, C
Temperature, C
800 800
600 600
30%O2 + 70%CO2 - surface 30%O2 + 70%CO2 - surface

400 400
200 60%O2 + 40%CO2 - surface 200 60%O2 + 40%CO2 - surface

0 0
0 100 200 300 400 500 0 100 200 300 400 500 600 700 800 900 1000
Time, s Time, s
Fig. 4. Temperature profiles for coal C (a) and coal D (b) particles combusted
in CFB in various mixtures of O2/CO2
Figure 5 shows the effect of gas composition on the ignition time of volatiles. Ignition
time was characterized by the time required to achieve a visible flame. Larger heat
capacity of CO2 compared to that of N2 retards the ignition of volatiles in O2/CO2
mixtures with 21% O2. However, when the concentration of oxygen in O2/CO2
mixtures is larger than 30%, the ignition time decreases with increasing O2 content.
The trends are consistent with those found in the literature, Toftegaard et al. (3) and
Molina and Shaddix (8).
30
Air
21%O2 + 79%CO2
25 30%O2 + 70%CO2 24
40%O2 + 60%CO2
50%O2 + 50%CO2 19
Ignition time, s
20 60%O2 + 40%CO2
16
15 13
11 11
10
10 9 9
8
7
6 6 6
5 5 5
5 4 4 4
3 3
2
1
0
Coal A Coal B Coal C Coal D
Fig. 5. Ignition time for bituminous coal particles combusted in various atmospheres
The influence of oxygen concentration in O2/CO2 mixtures on the devolatilization

time is shown in Figure 6. Devolatilization time was the duration of the visible flame
(from ignition of volatile matter to the end of combustion of volatile matter). The
devolatilization time decreases with increasing O2 concentration for coals A, B and
C and increases for coal D. Different devolatilization behaviour in the case of coal D
can be associated with differences in its internal structure (porosity and pore size)
and lower reactivity.
65
Coal A
60 Coal B
Devolatilization time, s
55 Coal C
Coal D
50
45
40
35
30
25
10 20 30 40 50 60 70
Oxygen concentration, %vol
Fig. 6. Devolatilization time for coal particles combusted in mixtures of O2/CO2
Figure 7 shows the influence of O2 concentration in O2/CO2 mixtures on the total

combustion time. For all coals tested the total combustion time decreases with
increasing oxygen concentration. The largest combustion times have been recorded
for coal D. They are approximately 100% higher compared to those for coal C.
Figure 8 shows images of A coal particle at different stages of combustion.
1500
Coal A
1300 Coal B
Total combustion time, s
Coal C
1100
Coal D
900
700
500
300
100
10 20 30 40 50 60 70
Oxygen concentration, %vol
Fig. 7. Total combustion time for coal particles combusted in mixtures of O2/CO2
CONCLUSIONS
Oxy-fuel tests were conducted for 10-mm three Polish and one South African
bituminous coal particles in a 12 kW bench-scale CFB combustor at temperature of
850°C. The experiments were carried out in air (base case) and mixtures of O2/CO2
with oxygen concentrations in the range from 21% to 60% vol. Results of proximate
and petrographic analyses reveal that ash and inertinite (maceral that is less
reactive than vitrinite) contents in the South African are much higher than those in
Polish coals. Therefore the combustion behaviour of these coals was different in air
and O2/CO2 mixtures. Combustion in air proceeded at ~50˚C higher centre
temperatures and was slightly shorter in time compared to combustion in O 2/CO2
mixture with 21% vol. O2. As expected, the total combustion time, in both air and
O2/CO2 mixture, for South African coal was much longer (~90%) than that for more
reactive Polish coal C. Larger heat capacity of CO2 compared to that of N2 also
retards the ignition of volatiles in O2/CO2 mixtures with 21% O2. These trends are
consistent with those found in the literature. However, when the concentration of
oxygen in O2/CO2 mixtures is larger than 30%, the ignition time decreases with
increasing O2 content. Surface and centre temperatures increase significantly with
increasing O2 concentration. The devolatilization time decreases with increasing O2
concentration for Polish coals A, B and C and increases for South African coal D.
Different devolatilization behaviour in the case of coal D can be associated with
differences in its internal structure (porosity and pore size) and lower reactivity. The
total combustion time decreases with increasing oxygen concentration for all coals
tested.
air 21%O2 + 79%CO2 40%O2 + 60%CO2 60%O2 + 40%CO2

Heating and drying
Ignition of volatile matter
Combustion of volatile matter
Combustion of char
Fig. 8. Visualisation of A coal particle in CFBC in air and O2/CO2 mixtures

This paper included fundamental research and it is only the first step in studying and
modeling of the oxy-fuel combustion process. The next step will be combustion of
a portion of coal not only single coal particles. It will allow us to answer a question
how a specific coal influences operation of oxy-CFB combustor like temperature
profile in combustion chamber, real particles distribution of fluidized bed
(fragmentation and erosion processes) and emission of pollutants. Next research
will also answer a question how much oxygen in mixture of O2/CO2 is needed to
have similar conditions like in the air combustion. Concentration of oxygen in
O2/CO2 mixture will differ for various types of coal. It is very important for design and
operation of oxy-fuel CFB units.
ACKNOWLEDGMENT
This work was supported by the Polish Ministry of Science and Higher Education
from sources for science in the years 2009-2010 under Research Project
No. N N513 396336. The support is gratefully acknowledged.
NOTATION
dp – particle diameter, μm
d50 – median particle diameter, μm
ρ – density, kg/m3
REFERENCES
1. Zhang L., Binner E., Chen L., Qiao Y., Li C.Z., Bhattacharya S., Ninomiya Y.:
Experimental Investigation of the Combustion of Bituminous Coal in Air and
O2/CO2 Mixtures: 1. Particle Imaging of the Combustion of Coal and Char.
Energy Fuels 24, p.4803-4811, 2010.
2. Buhre B.J.P., Elliott L.K., Sheng C.D., Gupta R.P., Wall T.F.: Oxy-fuel
combustion technology for coal-fired power generation. Progress in Energy and
Combustion Science 31, p.283-307, 2005.
3. Toftegaard M.B., Brix J., Jensen P.A., Glarborg P., Jensen A.D.: Oxy-fuel
combustion of solid fuels. Progr. in En. and Comb. Scien 36, p.581-625, 2010.
4. Jia L., Tan Y., Anthony E.J.: Emissions of SO2 and NOx during Oxy-Fuel CFB
Combustion Tests in a Mini-Circulating Fluidized Bed Combustion Reactor.
Energy Fuels 24, p.910-915, 2010.
5. Kuivalainen R., Eriksson T., Hotta A., Sacristan A.S.B., Jubitero J.M.,
Ballesteros J.C., Lupion M., Cortes V., Anthony B., Jia L., McCalden D., Tan Y.,
He I., Wu Y., Symonds R.: Development and Demonstration of Oxy-fuel CFB
Technology. Proc. of the 35th International Technical Conference on Clean Coal
& Fuel Systems, Florida, USA, 2010.
6. Fiveland W.: Advanced Combustion Technology: Oxy-Firing to Enable CO2
Capture. 2nd Workshop Intern. Oxy-Combustion Res. Network, USA, 2007.
7. Czakiert T., Sztekler K., Karski S., Markiewicz D., Nowak W.: Oxy-fuel
circulating fluidized bed combustion in a small pilot-scale test rig. Fuel
Processing Technology 91, p.1617-1623, 2010.
8. Molina A., Shaddix C.R.: Ignition and devolatilization of pulverized bituminous
coal particles during oxygen/carbon dioxide coal combustion. Proc. Combust.
Inst. 31(2), p.1905-12, 2007.
FLUIDIZED BED MEMBRANE REACTOR FOR STEAM REFORMING
OF HIGHER HYDROCARBONS: MODEL SENSITIVITY
M.A. Rakib*, J.R. Grace and C.J. Lim
University of British Columbia, Vancouver, Canada V6T 1Z3
* Corresponding author (rakibche@gmail.com),
currently with SABIC T&I, Riyadh 11551, Saudi Arabia
ABSTRACT
A fluidized bed membrane reactor (FBMR) was built and operated at temperatures
<600°C to reform higher hydrocarbons like propane and heptane. A two-phase
reactor model is utilized to simulate the FBMR with hydrogen withdrawn from both
phases. The superficial gas velocities in the reactor change because of variations in
molar flow due to reaction and hydrogen withdrawal through the membranes, as well
as variations in temperature, pressure and cross-sectional area. Sensitivity studies
show that the FBMR performance is primarily controlled by chemical equilibrium and
hydrogen permeation through the membranes, while being insensitive to errors in
accurately characterizing the chemical kinetics and hydrodynamics.
INTRODUCTION
The increasing demand for hydrogen as an industrial commodity and future energy
carrier has intensified research on alternative methods of hydrogen production.
Steam reforming is the favoured process for making hydrogen (1). Natural gas is the
most widely used feedstock due to its widespread availability. Liquid hydrocarbon
feedstocks like naphtha and LPG can be used when natural gas is not available.
Higher hydrocarbons like LPG, naphtha, kerosene and diesel are preferable for
making hydrogen in mobile applications. In addition, feedstock flexibility is desirable
for refineries, which often have seasonal surpluses of some of these hydrocarbons.
The main reactions for steam reforming of higher hydrocarbons are (1):
CnHm + nH2O D nCO + (n + m/2)H2 DH°298 = 499 kJ/mol (for n = 3) (1)
CH4 + H2O D CO + 3 H2 DH°298 = 206 kJ/mol (2)
CO + H2O D CO2 + H2 DH°298 = - 41 kJ/mol (3)
CH4 + 2H2O D CO2 + 4H2 DH°298 = 165 kJ/mol (4)
The yield of hydrogen is limited by the reversibility of reactions (2)-(4). In general,
reaction (1) is irreversible for higher hydrocarbons, but methane appears in the
reaction mixture due to the reversibility of reactions (2) and (4). In traditional steam
reformers, this is overcome by operating at high temperatures. However, elevated
temperatures lead to limited pressure ratings of the containment material, catalyst
sintering, and high steam-to carbon ratios to minimize catalyst deactivation.
A fluidized bed membrane reactor (FBMR) for steam reforming of natural gas is a
potential low-temperature alternative to achieve high hydrogen yields by continuous
shifting of equilibrium in the forward direction (2-4). An FBMR has been shown to be
flexible; able to process different alkane hydrocarbons (CnHm) as the feedstock (5,6),
leading to complete conversion of the hydrocarbons to produce maximum hydrogen:
CnHm + 2nH2O ® nCO2 + (2n + m/2)H2 (5)
EXPERIMENTAL SETUP
Steam reforming was conducted in a pressure vessel designed to withstand 10 bars
gauge at a maximum temperature of 621°C. The dense catalyst bed is contained in
a rectangular channel, 1.88 x 10-3 m2 and height of 1.87 m, with an extended circular
cross-section, 4.26 x 10-3 m2, above this. Figure 1 portrays the FBMR pressure
vessel. Vertical membrane panels (231.8 mm x 73.0 mm x 6.4 mm), with 25 µm
thick Pd77Ag23 membrane foils bonded on either side, divide the rectangular channel
into two equal sections. Six membrane panels could be inserted from alternate
sides, supported on rectangular flange covers, and passed through vertical slits on
the reactor wall. Consecutive membrane panels were separated by a vertical
distance of 22 mm. There is a horizontal gap of 5 mm between the reactor wall and
the unsupported end of the membrane panel. To evaluate the effects of the
hydrogen withdrawal through the membranes, the reactor was also operated with no
membrane panels, one membrane panel (fifth panel from the bottom), and six
membrane panels, with dimensionally identical stainless steel dummy plates
replacing the active membrane panels to keep the reactor internal geometry
identical wherever the latter were not installed.
The static bed height for all runs was 1.7 m.
The FBMR was operated under different operating
conditions with a feed of steam mixed with
methane, propane or heptane, with varying steam-
to-carbon molar ratios. Experimental details are
available elsewhere (5,6). The operating
conditions for the runs compared with the
simulations of this paper are given in Table 1.
The reactor was heated by internal cable heaters
along the height of the dense catalyst bed at all
four corners of the rectangular channel, in addition
to external band heaters in the semi-circular
spaces between the successive side openings for
inserting and supporting membrane panels. The
small scale of the reactor, and heat losses,
especially close to the flanges, made the
temperature profiles strongly dependent on the
heater distribution.
Table 1: Experimental conditions for steam

reforming of propane
Feed Propane, Steam
Steam-to-carbon molar ratio 5.0
Average temperature 500°C
Reactor pressure 600 kPa abs Figure 1: Fluidized bed membrane
Permeate pressure 25 kPa abs reactor showing six membranes for
Total feed rate 0.614 mols/min removal of pure hydrogen.
Commercial naphtha steam reforming catalyst particles, RK-212, of mean diameter

from Haldor Topsoe A/S were crushed and sieved to a mean diameter of 179 µm.
2
REACTOR MODEL
The FBMR was modeled as two phases in parallel: a high-density dense phase,
containing most of the particles, and a low-density bubble phase including a small
number of particles, with the solids volume fraction assumed to be:
fb = 0.001e b (6)
The minimum fluidization velocity was estimated from the correlation of Grace (7).
Model assumptions are:
(1) Steady state conditions.
(2) Ideal gas law.
(3) Catalyst temperature equal to local gas temperature. The axial variation in
temperature is the same in each phase and follows the measured profile.
(4) Catalyst internal mass transfer resistance ignored.
(5) The membranes are infinitely selective, i.e. only H2 passes through them.
(6) Catalyst deactivation is neglected.
(7) The gas in both the dense and bubble phases are assumed to be in plug flow.
(8) Visible bubble flow = flow in excess of that at minimum fluidization.
For each phase, the mole balance equation has four components:
(a) Reaction terms: The reactions are given by equations (1) – (4), with rate
equations as listed in an earlier paper (8).
(b) Interphase diffusional mass transfer: The interphase mass transfer coefficient
is estimated by the correlation of Sit & Grace (9), with the effective diffusivity of
gas components based on the average composition of the bubble and the
dense phases, using the correlation of Wilke (10). The bubble size is estimated
based on Darton’s equation (11).
(c) Hydrogen permeation: The immersed membrane panels withdraw hydrogen
from both phases, with the hydrogen flux governed by Sieverts’ equation (12):
P æ - EH 2 ö
QH 2 ,j = AP M 0 exp çç
δH 2
(
÷ PH ,j - PH ,m
÷
) (7)
è RT ø
2 2
(d) Interphase convection to maintain with the two-phase theory of fluidization. For
this, at a given height, the flow required in the dense phase is written as:
Qd , req = U mf A(1 - e b ) (8)
Hence, the volumetric bulk convective terms can be written as:
NC NC
R.T R.T
when
P
å Fi ,d > Qd ,req , Qd ®b =
i =1 P
åF
i =1
i,d - Qd ,req , Qb®d = 0 (9)
NC NC
R.T R.T
when
P
å Fi ,d £ Qd ,req , Qb®d = Qd ,req -
i =1 P
åF
i =1
i,d , Qd ®b = 0 (10)
This way of maintaining the flow in the dense phase is consistent with CFD
predictions for small particles (13).
Thus, the mole balance equation for the separation side can be written as:
dFH 2, p
dL
(
= a e b Qm H ,b + (1 - e b )Qm H , d
2 2
) (11)
where α, (≤1), the overall permeation effectiveness factor, is an adjustable parameter
to fit the simulated hydrogen permeation yields to the experimental results.
3
For the ith species in Bubble Phase:
NR
dFi, b
åg ij R j,b + kiq abe b A(Ci, d - Ci,b ) - ae b Qmi,b -
dQbd dQdb
= fb r p A Ci , b + Ci , d
dh j =1
dh dh
with i = C7H16, C3H8, CH4, H2O, CO, CO2, and H2 (12)
th
A similar mole balance is written for the i species in the dense phase. The flux of
all components other than hydrogen through the membranes is zero.
To predict the reactor offgas composition, it is also necessary to account for catalytic
reaction in the freeboard. An amount of catalyst equivalent to 0.8 mm of static bed
depth was assumed to be distributed uniformly in the freeboard region, based on
least squares error minimization with respect to the experimental concentrations of
methane, CO2, and H2 in the reformer off-gas for all of the experimental runs. The
freeboard was then modeled as a single-phase dilute suspension, with
dFi , fb NR
= f fb r p Aå g ij R j , fb (13)
dh fb j =1
The following quantities are calculated to assess the reactor performance:

molar flow of pure H2 extracted via membranes
Permeate hydrogen yield = (14)
molar flow of hydrocarbon in feed stream
Total hydrogen yield =
molar flow of pure H2 extracted via membranes + molar flow of H2 in retentate stream
(15)
molar flow of hydrocarbon in feed stream
total molar flow of CO and CO in retentate stream
Carbon oxides yield = 2 (16)
molar flow of carbon (in hydrocarbon) in feed stream
molar flow of methane in retentate stream
Methane yield = (17)
molar flow of carbon (in hydrocarbon) in feed stream

Temperature profiles for the experiments, greatly affected by the heater
arrangement, are shown in each plot below. The model was used (8) to simulate
previous experimental results (5,6), and good agreement was achieved with α as the
only adjustable parameter. Fitting of experimental data to the model for hydrogen
permeation through the membranes gave a = 0.248 as a correction to a membrane
permeation equation provided by the suppliers of the membrane panels. The decline
in permeation flux relative to that in tests in a permeation test rig without particles
was likely due to formation of a thin coating of catalyst fines on the membrane foils.
Figure 2 plots the superficial gas velocities for propane steam reforming with six
membrane panels. Four factors caused the variations in superficial velocity:
(1) Intermittent abrupt variations of the superficial gas velocity due to changes in
cross-sectional area in the spaces between adjacent membrane panels.
(2) The superficial gas velocity is affected by the temperature variations.
(3) The steam reforming reactions lead to a net increase in molar flow. This
caused steep increases in U near the FBMR entrance, where propane
conversion is completed. Subsequent methanation (reverse reactions from
equations (2) and (4)) can result in the opposite trend.
4
(4) Superficial velocity also varies owing to hydrogen removal via the membranes.
570
Temp. (oC)
Local 520
470
420
Superficial Gas
Velocity (m/s)
0.08
0.06
0.00 0.25 0.50 0.75 1.00 1.25 1.50 1.75
Height above Distributor (m)
Figure 2: Gas superficial velocities for propane steam reforming.
The sensitivity of the reactor model was tested (8) to understand the relative
importance of the various phenomena inside the FBMR, as well as the effect of
uncertainties in estimating parameters in the model. The bulk mass transfer was
found to be negligible compared to the other three components of the mole balance
equations. Similar observations apply to steam methane reforming in an FBMR (14).
The kinetic rate constants for all reactions included were first varied upwards and
downwards by a factor of 10 compared with those based on the literature values.
Some variations in performance occurred near the reactor entrance, affected mainly
by the propane steam reforming kinetics. However, over most of the height, there
was very little difference in the local yields of methane, carbon oxides or hydrogen.
To test the importance of hydrodynamics and interphase mass transfer, Figure 3
shows the reactor performance with the interphase mass transfer coefficient
increased and decreased a factor of 10 relative to those from the Sit and Grace (9)
correlation. The higher coefficient results in almost immediate transfer of propane
from the bubbles to the dense phase, whereas, slower mass transfer retains more
propane in the bubbles, delaying its conversion, Since methane is an intermediate
component, it appears more slowly in the reactor, and its overall conversion is also
delayed. With delayed transfer of hydrogen from the dense phase, where it is
produced, to the bubble phase, where negligible hydrogen is produced, the net
removal of hydrogen via membranes is reduced.
While the effects of tenfold upward and downward changes in the interphase mass
transfer coefficient are discernible, these effects are not very significant. Hence,
interphase mass transfer, while not a negligible factor, plays a secondary role with
respect to overall reaction. Since the bed hydrodynamics mostly enter the model
through the interphase mass transfer, one may also conclude that accurate portrayal
of bed hydrodynamics is of secondary importance for this process and for the
operating conditions investigated.
To explore the effect of permeation capacity variation of the membranes, the
membrane permeation effectiveness factor was set at a = 0.15, 0.248 ( fitted value),
and 0.35. As shown by Figure 4, the FBMR performance depends strongly on the
hydrogen permeation through the membranes.
5
570
Temp. ( o C)
520
Local
470
570
C)
420
o
520
Local
0.9
Temp. (
470
Carbon Oxides
0.7 420
Yield
0.5 0.1 x Mass Transfer

0.9
1 x Mass Transfer
0.3 10 x Mass Transfer
0.7
Carbon Oxides
0.7
Yield
0.1 x Mass Transfer 0.5 a = 0.15
0.5 1 x Mass Transfer a = 0.2484
Methane Yield
10 x Mass Transfer 0.3 a = 0.35

0.3 0.7
a = 0.15
0.1
0.5 a = 0.2484
a = 0.35
Methane Yield
1.00
0.3
Propane Conversion
0.75
0.50 0.1 x Mass Transfer 0.1

1 x Mass Transfer
0.25 10 x Mass Transfer
7
Yield
0.00
2
7 5
Yield 2
Permeate H
5 3 a = 0.15
Permeate H
3 0.1 x Mass Transfer a = 0.2484

1 x Mass Transfer 1 a = 0.35
1 10 x Mass Transfer 10
10
8
8
Yield
Yield
6
6
2
2
4
a = 0.15
Total H
Total H
4 0.1 x Mass Transfer

1 x Mass Transfer 2 a = 0.2484
2
10 x Mass Transfer
a = 0.35
0 0
0.0 0.5 1.0 1.5 2.0 2.5 0.0 0.5 1.0 1.5 2.0 2.5
Height above Distributor (m) Height above Distributor (m)
Figure 3: FBMR performance with variations Figure 4: FBMR performance with variations
in interphase mass transfer coefficient in permeation effectiveness factor.
CONCLUSIONS
A fluidized bed membrane reactor is modeled to simulate its performance for
producing hydrogen from propane. Model sensitivity studies show that the chemical
kinetics are fast enough at all temperatures tested for their role to be insignificant in
determining the FBMR performance. The interphase diffusional mass transfer rate is
somewhat more significant in affecting reactor performance, but again plays a
secondary role. From these results, it is evident that the FBMR performance is
primarily controlled by chemical equilibrium and by the rate of hydrogen permeation
through the membranes. Hence the model is sensitive to accurately characterizing
6
the chemical equilibrium and hydrogen permeation, but insensitive to the chemical
kinetics, interphase mass transfer and hydrodynamics, at least for the temperature
range of interest (450-550°C).
ACKNOWLEDGEMENT
Financial support from the Canada Foundation for Innovation and the Natural
Sciences and Engineering Research Council of Canada (NSERC) is gratefully
acknowledged. M.A.R. thanks NSERC for a two-year doctoral scholarship.
NOTATION
ab Specific surface area of gas bubbles (m2/m3)
A Cross-sectional area of bed (m2)
AP Membrane permeation area per unit length of membrane (m2/m)
C i ,b Molar concentration of species i in bubble phase (mol/m3)
C i ,d Molar concentration of species i in dense phase (mol/m3)
E H2 Activation energy for permeation (J/mol)
Fi ,b Molar flow rate of species i in bubble phase (mol/s)
Fi,d Molar flow rate of species i in dense phase (mol/s)
Fi , fb Molar flow rate of species i in freeboard (mol/s)
h Vertical coordinate measured from distributor (m)
h fb Vertical co-ordinate from dense catalyst bed surface (m)
k iq Interphase mass transfer component for species i (m/s)
m, n Stoichiometric constants (-)
NC, NR Number of components, reactions (-)
P Pressure (Pa)
Pi Partial pressure of species i (bar)
PH 2 ,b , PH 2 ,d Partial pressure of hydrogen in bubble, dense phase (atm)
PH 2 , p Partial pressure of hydrogen on permeate side (atm)
PM 0 Pre-exponential factor for permeation (mole/(m.min.atm0.5))
Qbd Cross-flow from bubble to dense phase per unit length (m3/(m.s))
Qdb Cross-flow from dense to bubble phase per unit length (m3/(m.s))
Qd ,req Flow requirement for dense phase to prevent de-fluidization (m3/s)
Qmi ,j Membrane permeation rate of species i for j phase (mol/(m.s))
R Universal gas constant (J/mol/K)
Rj Rate of jth reaction (mol/kg catalyst/s)
U Superficial gas velocity (m/s)
dH 2
Thickness of hydrogen selective membranes (m)
eb Volume fraction of catalyst bed occupied by bubble phase (-)
fb , f d Bed volume fraction occupied by particles in bubble, dense phase (-)
f fb Volume fraction of freeboard occupied by solid particles (-)
7
g ij Stoichiometric coefficient of component i in j th reaction
rp Density of catalyst particles (kg/m3)
DH Heat of reaction (kJ/mol)
Subscripts
b, d Bubble, dense phase
fb Freeboard
i Species i
in At reactor inlet
j Reaction j
m Membrane side
j Phase j
REFERENCES
1. Rostrup-Nielsen, J., Catalytic steam reforming. In Catalysis Science and
Technology, Andersen, J.R.; Boudart, M., Eds. Springer-Verlag: 1984; pp 1-117
2. Adris, A.M.; Lim, C.J.; Grace, J.R., The fluidized bed membrane reactor
system: A pilot scale experimental study. Chem. Eng. Sci. 1994, 49, 5833-5843.
3. Boyd, T.; Grace, J.; Lim, C.J.; Adris, A.M., Hydrogen from an internally
circulating fluidized bed membrane reactor. Int. J. Chem. React. Eng. 2005, 3, A58.
4. Patil, C.S.; Annaland, M.V.S.; Kuipers, J.A.M., Fluidised bed membrane
reactor for ultrapure hydrogen production via methane steam reforming:
Experimental demonstration and model validation. Chem. Eng. Sci. 2007, 62, 2989-
3007.
5. Rakib, M.A.; Grace, J.R.; Lim, C.J.; Elnashaie, S.S.E.H., Steam reforming of
heptane in a fluidized bed membrane reactor. J. Power Sources 2010, 195, 5749-
5760.
6. Rakib, M.A.; Grace, J.R.; Lim, C.J.; Elnashaie, S.S.E.H.; Ghiasi, B., Steam
reforming of propane in a fluidized bed membrane reactor for hydrogen production.
Int. J. Hydrogen Energy 2010, 35, 6276-6290.
7. Grace, J.R., Fluidized-bed hydrodynamics. In Handbook of Multiphase
Systems, Hetsroni, G., Ed. Hemisphere: Washington, 1982; pp 8-5 - 8-64.
8. Rakib, M.A.; Grace, J.R.; Lim, C.J.; Elnashaie, S.S.E.H., Modeling of a
fluidized bed membrane reactor for hydrogen production by steam reforming of
hydrocarbons. Ind. Eng. Chem. Res., 2011, In Press.
9. Sit, S.P.; Grace, J.R., Effect of bubble interaction on interphase mass transfer
in gas fluidized beds. Chem. Eng. Sci. 1981, 36, 327-335.
10. Wilke, C. R., Diffusion properties of multicomponent gases. Chem. Eng. Prog.
1950, 46, 95-104.
11. Darton, R.C.; Lanauze, R.D.; Davidson, J.F.; Harrison, D., Bubble growth due
to coalescence in fluidized-beds. Trans. IChemE 1977, 55, 274-280.
12. Sieverts, A.; Zapf, G., The solubility of deuterium and hydrogen in solid
palladium. Zeitschrift für Physikalische Chemie 1935, 174, 359-364.
13. Li, T.W.; Mahecha-Botero, A.; Grace, J.R., Computational fluid dynamic
investigation of change of volumetric flow in fluidized bed reactors. Ind. Eng. Chem.
Res. 2010, 49, 6780-6789.
14. Adris, A.M.; Lim, C.J.; Grace, J.R., The fluidized-bed membrane reactor for
steam methane reforming: Model verification and parametric study. Chem. Eng. Sci.
1997, 52, 1609-1622.
8
CRITICAL EVALUATION OF EULER-EULER AND EULER-
LAGRANGIAN MODELLING STRATEGIES IN A 2-D GAS
FLUIDIZED BED
F. Hernández-Jiméneza, J.R. Thirdb, A. Acosta-Iborraa, C.R. Müllerb

a
Universidad Carlos III of Madrid, Department of Thermal and Fluid Engineering, ISE
research group. Av. de la Universidad, 30, 28911, Leganés, Madrid, Spain .
b
ETH Zürich, Institute of Energy Technology, Laboratory of Energy Science and
Engineering, Leonhardstrasse 27, 8092 Zürich, Switzerland.
Abstract
Two-phase granular systems are commonly encountered in industry, and fluidized
beds are particularly important due to their excellent heat and mass transfer
characteristics. Here, we critically evaluate the differences between two modelling
strategies, Euler-Euler and Euler-Lagrangian models. Euler-Euler simulations were
performed using MFIX and an in-house code was used for Euler-Lagrangian
simulations. A 2D bed of width, height and transverse thickness of respectively, 0.2
m, 0.5 m and 0.01 m, served as a test case. The settled bed height was H 0 = 0.2 m.
Particles of density ρ = 1000 kg/m³ and diameter dp = 1.2 mm were fluidized with air.
The drag-law proposed by Benyahia et al. (10) was used in both models.
Comparison between the simulation results was based on both instantaneous and
time-averaged properties. A particular focus of this study was the influence of the
coefficients of restitution and friction on the simulation results.
INTRODUCTION
Fluidized beds have various applications in industry, such as fluid catalytic cracking
(FCC), gasification and combustion of coal, and Fischer−Tropsch synthesis (Kunii
and Levenspiel (1)). Despite the fact that fluidized beds have been used in industry
since the 1920s and good progress has been made in numerical simulations using
two-fluid (Gidaspow (2)) or discrete element models (Tsuji et al. (3)), some aspects
of fluidized bed hydrodynamics, such as bubble splitting, are still far from fully
understood.
Numerical modelling of fluidized beds has advanced significantly over the last two
decades, the most popular modelling approaches being the Euler-Euler and Euler-
Lagrangian models. The Euler-Lagrangian approach combines an Eulerian
description of the fluid-phase with a Lagrangian particle simulation, in which the
trajectory of each particle is calculated based on Newton's second Law. The gas-
solids interaction is computed through semi-empirical closure models (Deen et al.
(4)). Although very promising, the Euler-Lagrangian approach is very
computationally expensive and is, therefore, currently unable to simulate the large
number of particles encountered in medium- or large-scale fluidized beds. In the
Euler-Euler approach (Gidaspow (2), Wachem and Almstedt (5)) the particulates
and the fluid phase are treated as inter-penetrating continua (two-fluid model). As in
the case of the Euler-Lagrangian approach, two-fluid simulations of fluidized beds
require closure relationships for the gas-solids interaction. However, since the
particle motion is not modelled in detail, the two-fluid model also requires closure
relationships for the particle-particle interactions. These closure relationships may
be empirical in nature or may be derived from theoretical relations that are linked to
the kinetic theory of granular gases (Gidaspow (2)).
The aim of this work is to compare the Euler-Euler and Euler-Lagrangian

approaches for a specific test case, consisting of a two-dimensional (2D) gas
fluidized bed. In addition, the effect of parameters such as the inter-particle and
particle-wall coefficients of friction, and the coefficient of restitution, will be studied
for both models.
DEM APPROACH
A Discrete Element Model (DEM) has been constructed based on the work of Tsuji
et al (3), which combines the discrete element model of Cundall and Strack (6) to
simulate the particulate phase, with the volume-averaged Navier-Stokes equations
for the fluid phase, as derived by Anderson and Jackson (7). For each particle, the
linear and angular momenta are governed by Newton’s second law:
d vs V p ds
mp =−V p ∇ p  vg− vs  F c Ip =Tp
dt 1− g  dt
 s , V p , vg ,  , F c , Tp and I p are the mass, linear and angular
where m p , vs , 
velocities of the particle, the particle volume, the velocity of the gas phase, the inter-
phase momentum exchange coefficient, the force and torque resulting from the
collision of the particles, and the moment of inertia of the particle, respectively. To
model the collision between contacting particles the soft-sphere approach was used,
in which the particles are allowed to overlap by a small amount, δ. For the fluid the
volume-averaged continuity and Navier-Stokes equations are given by Anderson
and Jackson (7):
∂ g  g
∇ · g g vg =0
∂t
∂ g  g vg
∇ · g g vg ²=− g ∇ p−∇ · g  g − F p g  g 
g
∂t
here,  g is the viscous stress tensor and F p is the rate of exchange of
momentum between the particulate and the fluid phases. The fluid was assumed to
be Newtonian. The rate of momentum exchange between the particulate and fluid
phases was calculated by adding up the fluid forces acting on the N p individual
particles in a fluid cell of volume V cell :
Np
Vp
∑  vg− vs 
n=1
F p=
V cell 1−g 
TWO-FLUID MODEL APPROACH
The two-fluid model, based on the conservation equations of mass, momentum and
granular temperature, was solved using the MFIX code (Multifluid Flow with
Interphase eXchanges) (Syamlal et al (8), Benyahia et al (9)). The kinetic theory of
granular gases was used for the closure of the solids pressure stress terms. The
governing equations can be summarized as follows.
Mass conservation of the gas (g) and solid (s) phases:
∂ g  g ∂ s s
∇ · g g vg =0 ∇ · s  s vs =0
∂t ∂t
Momentum conservation of the gas and solids phases:
∂ g  g vg
∇ · g g vg =−g ∇ p∇ ·  g  g  g  g −K gs  vg −vs 
∂t
∂ g  g vg
∇ · s  s vs =−s ∇ p−∇ p s∇ ·  s s  s g  K gs  vg −vs 
∂t
where  g , s ,  g ,  s , vg , vg correspond to gas and solids volume fraction, gas and
solids density and gas and solids velocity respectively, p is pressure,  g , s the
stress tensors for gas and solids respectively,  g is the acceleration due to the
gravity and K gs is the gas-solids momentum exchange coefficient.
The balance equation for the granular temperature, Θ, is given by:

3 ∂
   ∇ · s s vs =− p s I  s :∇ vs ∇ · k  ∇ −−3K gs 
2 ∂t s s
where − p s I s : ∇ vs is the generation of Θ by the solids stress tensor,
∇ ·k  ∇  is the diffusion of Θ energy,  is the collisional dissipation of
energy and 3K gs  is the transfer of kinetic energy between phases. A second
order accurate scheme (Superbee) was used to discretize the convective derivatives
in the balance equations.
NUMERICAL SIMULATIONS
The gas-fluidized bed studied was of 0.2 m width, 0.01 m transverse thickness and
0.5 m height, filled with spherical particles of density ρ = 1000 kg/m³ and diameter d p
= 1.2 mm. The static bed height was H0 = 0.2 m and the gas inlet velocity was U =
0.6 m/s, corresponding to U/Umf = 2 . Several cases were studied to evaluate the
effect of the properties of the particles and walls. Table 1 summarizes the cases
studied in this work. The parameters that are varied are the inter-particle and
particle-wall coefficients of friction, and the restitution coefficient. Case 1 is taken to
be the base case incorporating commonly used parameters. The inlet has been
modelled as a homogeneous velocity inlet and the outlet as a constant pressure
outlet for both models. The computational domain for the two-fluid model simulations
comprised 57 × 141 × 8 cells in the x- (width), y- (height) and z- (thickness)
directions, respectively. This creates a mesh with a 3.5 mm cell size, which is below
10 particle diameters and ensures grid-independent results. A partial slip boundary
condition was applied at the walls of the fluidized bed, with a partial slip coefficient of
Ф=0.6. The fluid computational domain for the DEM model comprised 58 × 148 × 3
cells in the x-, y- and z- directions. The fluidized bed contained 265650 particles.
Interactions between particles are modelled using a damped Hertzian spring with an
E-modulus of 1.2×106 N/m2. Both models use the drag law proposed by Benyahia
et al. (10). For the time-averaged results, 40 seconds are employed for the Euler-
Euler model and 28 seconds for the Euler-Lagrangian model.
Model Parameter Case 1 Case 2 Case 3 Case 4
Restitution coefficient 0.9 0.9 0.9 0.5
Two-fluid Coefficient of friction between particles 0.57 0.1 0.57 0.57

model
Walls boundary conditions Partial Partial Free Partial
slip slip slip slip
Restitution coefficient 0.9 0.9 0.9 0.5
DEM Coefficient of friction between particles 0.57 0.1 0.57 0.57
Friction between particles and walls 0.57 0.1 0 0.57

Table 1: Simulation parameters for the two-fluid and DEM simulations.
RESULTS DISCUSSION
Figure 1 shows instantaneous snapshots of the solids volume fraction for case 1
simulated using the two models. Both snapshots were taken after the transient
fluidization that occurs during start-up. The snapshots show the characteristic
pattern of 2-D beds: small and narrow bubbles appearing in the bottom of the bed,
and bigger and less numerous circular bubbles reaching the bed surface. Here
bubbles are located where the solids volume fraction reaches a value close to zero.
The solids volume fractions presented have been averaged over the entire bed
thickness.
Figure 1. Instantaneous snapshot of the bed showing αs: a) two-fluid model; b)

DEM.
Figures 2 and 3 show the solids volume fraction averaged over the width and
thickness of the bed, as a function of time, for the two fluid model and DEM
respectively. Both models show the creation of small, slow-moving bubbles close to
the distributor and the coalescence and eruption of faster bubbles at distances
around y = 0.1 m above the distributor.
Figure 4a and 4b show the power spectra obtained from the data presented in
Figures 2 and 3 at two different heights, y = 0.005 m (close the distributor) and y =
0.217 m (close to the top of the bed). For both models the maxima in the power
spectra occur at higher frequencies at y = 0.005 m than at y = 0.217 m. This is
expected because bubbles coalesce as they rise through the bed, leading to a
reduction in the number of bubbles that cross a horizontal section.
It should be noted, however, that the frequency depicted in Figure 4 is a 'bubble
coherence frequency' because several bubbles may cross a horizontal section at
any instant of time. Therefore, the frequencies of Figure 4 cannot be interpreted as a
single bubble frequency unless the size of the bubble is comparable to the bed
width, i.e. near the bed surface. The bubble coherence frequency near the
distributor defines the principal frequency of bubble formation. This frequency of
bubble formation is qualitatively similar in both models, namely ~ 6 Hz. The principal
frequencies at y = 0.217 m, i.e. the frequency of bubble eruption, are also similar for
both simulation strategies. In particular, Figure 4 shows that the peak of the power
spectrum at y = 0.217 m occurs at ~ 2.5 Hz, which is in agreement with the bed
oscillation frequency due to bubble eruption given by Baskakov et al. (11),
f = g/ H o /=2.23 Hz .
s
Figure 2. XZ-averaged αs, two-fluid model. Case 1.

s
Figure 3. XZ-averaged αs, DEM. Case 1.
The average solids volume fraction in an x-z plane located at y = 0.22 m is shown in
Figure 5 for the two fluid model and DEM. This y position is close to the freeboard of
the bed. Figure 5a reveals that the amplitude of the fluctuations in the solids volume
fraction is smaller in the two-fluid simulations when compared with the DEM results.
This is expected since the two-fluid approach tends to smear the distinction between
the bubble and particulate phase. For the DEM a sharper, and more realistic,
transition between the bubble and particulate phase is modeled.
Figure 5b plots the dominant frequencies, extracted as the peak-frequency from the
power spectra, as a function of vertical position, y. In both simulation strategies, the
profiles of peak-frequencies are in good agreement. In particular, high frequencies
(around 6 Hz) are observed near the distributor and there is a transition zone in 0.05
m < y < 0.1 m. Near the freeboard both simulations show a region where the
frequency stabilizes due to big bubbles passing at a frequency around 2.5Hz.
Figures 2 and 3 reinforce this observation: both figures indicate a large number of
slow-moving bubbles close to the distributor and a smaller number of faster bubbles
after the transition zone.
Figure 4. Power spectra of XZ-averaged αs, a) two-fluid model, b) DEM. y = 0.005 m

(solid line); y = 0.217 m (dash line). Case 1.
Figure 5. a) XZ-averaged αs at a height of 0.22 m b) Vertical profile of peak

frequency for XZ-averaged αs: two-fluid model (solid line); DEM (dash line). Case 1.
The effect of the wall friction is demonstrated in Figures 6a and 6b. Here, the solids
velocity and solids volume fraction, averaged with respect to time and transversal
thickness, are presented at a height y = 0.01 m for both simulation strategies. In
case 1, both models predict very similar magnitudes for the solids velocity, however
the bed hydrodynamics are substantially different. In the two-fluid model there are
two preferential bubble paths at a distance of ~ 0.05 m away from the lateral walls
(Figure 6b). On the other hand in the DEM there is only one path in the middle of the
bed. For case 3, which employs a free slip condition at the walls, the time-averaged
velocities within the bed are an order of magnitude greater than those obtained for
case 1. Furthermore, there are substantial discrepancies between the two-fluid and
DEM results obtained for case 3: the two-fluid model predicts velocities that are
approximately twice those predicted by the DEM and also predicts higher solids
volume fractions, i.e. smaller bed expansion.
Finally, Figure 7 compares the solids velocity in both models for cases 1, 2 and 4.
For the two-fluid model only small changes in the profile of the solids velocity can be
observed for the case that the coefficients of friction and restitution are reduced.
However, for the DEM the coefficient of friction plays an important role. Reducing
the coefficient of friction in the DEM from 0.57 to 0.1 leads to a substantial increase
in the time-averaged solids velocities, as seen in Figure 7b. Furthermore, it is
observed that for the two-fluid model reducing the coefficient of restitution decreases
the gradient along x-direction in the solids velocity profile; only very small variations
were observed in the DEM results.
Figure 6. Time averaged values of a) solids vertical velocity and b) αs at a height of

0.1 m: two-fluid model case 1 (solid line); DEM case 1 (dash line); two-fluid model
case 3 (dot line); DEM case 3 (dash-dot line).
Figure 7. Time averaged values of solids vertical velocity at a height of 0.1 m, a)

two-fluid model b) DEM: case 1 (solid line); case 2 (dash line); case 4 (dot line).
CONCLUSIONS
DEM and two-fluid model simulations of 2D bubbling fluidized beds have been
compared in this work. For the base case, in which the coefficient of friction was set
to 0.57, both simulation strategies yield time-averaged velocities with similar
magnitudes, however the agreement of the characteristics of the velocity profiles is
disappointing, especially for the case using zero friction for the particle-wall contact.
The two-fluid model predicts that the highest velocities within the bed are located at
a distance of ~ 0.05 m away from the side wall, whereas the DEM predicts that the
highest velocities are located at the centre of the bed. For both simulation
techniques, the time-averaged solids volume fractions show minima that are
coincident with the maxima in the velocity profiles. This is consistent with the
hypothesis that bubbles preferentially pass through these locations.
The behaviour of bubbles has been examined by averaging the solids volume
fraction over horizontal cross sections of the bed. Both the two-fluid and DEM
simulations predict a coherence bubble frequency of 6 Hz close to the distributor
and a frequency of 2.5 Hz close to the surface of the bed.
Furthermore, the influence of the coefficients of friction and restitution on the

simulation results has been investigated. The time-averaged solids velocity and
solids volume fraction profiles suggest that, within the range examined here, the
behaviour of the bed, using two-fluid and DEM models, is relatively insensitive to the
particle-particle coefficient of friction and, for the DEM results, to the coefficient of
restitution. However, setting the particle-wall coefficient of friction to zero was found
to have a pronounced effect on the particle motion within the bed. Under these
conditions both models were found to give time-averaged solids velocities an order
of magnitude larger than those predicted for simulations with particle-wall friction.
Nevertheless, further work is required to establish the causes of the discrepancies
between the DEM and two-fluid models highlighted here.
Acknowledgement
This work has been co-funded by the Spanish Government (Project DPI2009
-10518) and the Autonomous Community of Madrid (Project S2009/ENE-1660).
References
1. D. Kunii, O. Levenspiel, Fluidization Engineering: Butterworth-Heinemann:
Newton, MA, 1991.
2. D. Gidaspow, Multiphase flow and Fluidization: Continuum and kinetic theory
descriptions; Academic Press: San Diego, CA. 1994.
3. Y. Tsuji, T. Kawaguchi, T. Yanaka, Discrete particle simulations of 2-dimensional
fluidized-beds. Powder tech. 77 (1993) 79-87.
4. N.G. Deen M. van Sint Annaland, M.A. van der Hoef, J.A.M. Kuipers, Review of
discrete particle modelling of fluidized beds. Chem. Eng. Sci. 62 (2007) 28-44.
5. B.G.M. van Wachem, A.E. Almstedt, Methods for multiphase computational fluid
dynamics. Chem. Eng J. 96 (2003) 81-98.
6. P.A. Cundall, C.D.L. Strack, A discrete numerical-model for granular assemblies.
Geotechnique 29 (1979) 47-65.
7. T.B Anderson, R. Jackson, A fluid mechanical description of fluidized beds. Ind.
Eng. Chem. Fund 6 (1967) 527-539.
8. M. Syamlal, W. Rogers, T.J. O'Brien, MFIX Documentation: Theory guide, U.S.
department of Energy (DOE), Morgantown Energy Technology Center, Morgantown,
West Virginia, 1993.
9. S. Benyahia, M. Syamlal, T.J. O'Brien, Summary of MFIX equations 2005-4,
2007.
10. S. Benyahia, M. Syamlal, T.J. O'Brien, Extension of Hill-Koch-Ladd drag
correlation over all ranges of Reynolds number and solids volume fraction. Powder
Tech. 162 (2006) 166-174.
11. A. P. Baskakov, V. G. Tuponogov, N. F. Filippovski. A study of pressure
fluctuations in a bubbling fluidized bed. Powder Tech. 45 (1986) 113-117.
DESCRIPTION OF PRESSURE FLUCTUATIONS IN A
CIRCULATING FLUIDIZED BED BY STATISTICAL ANALYSIS
Roelof L.J. Coetzer, Andre Mostert and Adam Luckos
Sasol Technology, Research and Development
1 Klasie Havenga Road, Sasolburg, 1947 South Africa
ABSTRACT
In this paper we evaluate different methods for statistically analyzing the variability in
pressure fluctuations measured at three locations in an 80-mm-ID, 5-m-tall CFB model
operated with natural rutile particles and air at ambient conditions. The methods
evaluated are the Shannon entropy, Fischer information matrix together with kernel
density estimation, and an estimation of the magnitude of the pressure amplitudes. The
accuracy of the different methods is estimated by the bootstrap method. We illustrate
how informative statistics from these methods can be used to quantify the effect of the
process variables on fluidization at different bed locations. Depending on the interest of
the experimenter, the method and statistic can be selected which explains fluidization
operation most accurately.
INTRODUCTION
The continuous monitoring of gas-solid fluidized-bed reactors is an important issue in

the industrial practice because of the complex dynamical behaviour characterizing
these systems. Failures and difficulties experienced in the operation of fluidized-bed
reactors are usually attributed to an un-sufficient understanding of the physics of gas-
solid fluidization (1). In particular, our knowledge on systems with irregularly shaped
particles with wide size distributions operated at higher gas velocities (in the turbulent
regime and in the fast fluidization regime), elevated temperatures and pressures is still
relatively poor.
In the last three decades, several techniques have been developed to describe the
dynamic phenomena that take place within the bed. Among these techniques, the
pressure fluctuation measurements are the most popular owing to their low costs and
direct relation to the bed dynamics (2). Pressure measurements sampled at frequencies
20–1000 Hz can be used to describe important fluidized-bed characteristics such as the
quality of fluidization, size and frequency of bubbles, transition from bubbling to
turbulent regime and minimum fluidization velocity.
In our previous studies, several important process parameters such as critical
velocities, distributions of solid concentration and pressure fluctuations were measured
in a CFB cold model (3–6). The variability in the pressure fluctuations were previously
evaluated by using the standard deviation and the coefficient of variation (7). In this
paper, we extend the analysis of the data by applying Shannon entropy and Fisher
information matrix (8). Our analysis should establish the relationship between two
entities, (1) process variables, and (2) pressure fluctuations at different levels in the
riser. This relationship will provide a basis for controlling the operation of a CFB reactor.
TEST APPARATUS AND PROCEDURE
Measurements of pressure fluctuations were carried out in the riser of the 80-mm, 5-m
tall CFB cold model made of transparent PVC. Data acquisition units recorded the
signals (sampled at 200 Hz) from three pressure transducers located at the bottom (0.2
m above the distributor), in the middle (at 2.46 m), and at the top of the riser (at 4.47
m). All tests were conducted with air at ambient conditions. At each stable condition
signals were collected over a period 40 s, an interval producing 8192 (i.e. 213) pressure
readings. The solid material used was natural rutile (TiO2). Its particles fall into group B
of Geldart’s classification. They are sub-rounded, fine (80–165 µm) and dense (4085
kg/m3). A more detailed description of the apparatus and test procedure can be found in
an earlier paper on the subject (4).
RESULTS
The concentration of solids in the riser adopts a ‘C’ shape, which becomes less
pronounced as the solid-circulation rate, Gs, at a given superficial fluidizing velocity, U,
decreases (4–6). Concomitant with the decrease is a shift in solids concentration at
each point in the riser to lower values, and move to greater solids concentrations at the
top of the riser than at the bottom. A higher suspension density at the top of the riser—a
consequence of the rebounding of particles from the plate closing the top of the riser—
is a phenomenon that is well known in small-scale (<0.2 m) CFB units (9−12). In tests at
a comparatively low U (3.5 m/s), higher solids concentrations span the top half of the
riser (~2.5 m). The suspension density decreases gradually from the top of the riser. At
higher fluidizing velocities (U=4.9 and 7.4 m/s) higher solids concentrations are
confined to a shorter length of the riser (≤1 m), and the profile is much steeper. As Jin
and co-workers showed (13), higher superficial gas velocities increase the velocity of
upwardly moving particles, which increases the exchange of momentum between
particles moving in opposite directions. As the influence of upwardly moving particles
grows stronger (at high gas velocities), the region of momentum exchange shortens. A
shortening of the region of higher suspension densities would accompany this change.
Pressures in the riser fluctuate over a range of about 1.2 kPa. The patterns of
fluctuations along the length of the riser are similar and synchronized (6). Pressure
fluctuations are irregular, and their peak intensities vary. The distribution of pressure at
each tap is skewed towards higher values; fluctuations are more pronounced above the
mean than below it. Expressing the amplitude of fluctuations over a scanned interval by
the standard deviation of pressure readings, one can readily see that (7):
• The average amplitude of pressure fluctuations increases with increasing Gs and U.
• The average amplitude of fluctuations is largest at the top of the column; the
amplitudes of fluctuations at the middle and bottom of the column are similar—yet
the solids concentration is similar at the top and bottom, and different from that in
the middle.
• There is an exception to this pattern at high superficial gas velocities. The
measurements may be problematic as solids flow bordered on being unstable.
Figure 1 depicts the pressure fluctuations (normalized with respect to the mean
pressure) in the middle of the riser at U=3.57 m/s and Gs=11.52 kg/m2·s. It can be
observed that pressure fluctuates in a fairly narrow band about zero.
Figure 2 shows the pressure fluctuations in the middle of the riser at U=3.57 m/s and
Gs=19.24 kg/m2·s. It is immediately evident that pressure fluctuates significantly more
about zero for the higher Gs of 19.24 kg/m2·s compared with the lower Gs of 11.52
kg/m2·s depicted in Fig. 1. Specifically, the variability in the pressure fluctuations is
significantly higher for Gs=19.24 kg/m2·s compared with Gs=11.52 kg/m2·s.
800 800
600 600
400 400
Pressure, Pa
Pressure, Pa
200 200
0 0
-200 -200
-400 -400
-600 -600
-800 -800
0 5 10 15 20 25 30 35 40 0 10 20 30 40
Time, s Time, s
Fig. 1. Pressure fluctuations (normalized) Fig. 2. Pressure fluctuations (normalized)

in the middle of the riser at U=3.57 m/s in the middle of the riser at U=3.57 m/s
and Gs=11.52 kg/m2·s and Gs=19.24 kg/m2·s
However, the statement of “significantly higher” variability should be substantiated and

statistically quantified. Therefore, statistical methods need to be applied to quantify the
difference in variability. This becomes even more relevant when more than two reactor
conditions are being evaluated at different values. In the study, three different
superficial gas velocities and three different solids fluxes were evaluated for differences
in pressure fluctuations along the riser.
STATISTICAL METHODOLOGY
The superficial gas velocity and solids flux are referred to as the reactor variables.
Three values or conditions for each reactor variable were tested and the pressure
fluctuations recorded. The pressure fluctuations will be evaluated in terms of its
variability at the different reactor conditions (see Table 1). Note that pressure
fluctuations were measured at three different positions in the fluidized bed i.e. at the
bottom, middle and top of the riser.
The standard deviation has been used in a previous study by the authors for quantifying
the variability of pressure fluctuations (7). In this paper, we introduce the Shannon
entropy, HX, and Fisher information matrix, IX, as methods for evaluating the variability
of pressure fluctuations.
Table 1. Experimental conditions
Condition U, m/s Gs, kg/m2·s
1 3.57 11.52
2 3.57 14.78
3 3.57 19.24
4 4.17 17.79
5 4.17 21.75
6 4.17 26.76
7 4.78 29.65
8 4.78 34.17
The Shannon entropy is a well-known tool for investigating the degree of disorder in
dynamical systems. The Shannon entropy will be high if the degree of disorder in the
system is high. Let x = ( x1 , x 2 , K, x N ) T denote the sample of pressure fluctuations. The
¯
Shannon entropy (differential entropy) is given by the following formula (8):
∞ (1)
H X = − ∫ f ( x) log f ( x) dx
−∞
where f (x) is the probability density function (PDF) of x.

The Fisher information is a tool that can be used to accurately describe the behavior of
dynamic systems and to characterize the complex signals generated by these systems
(8). The Fisher information is defined as follows:
∞ (2)
∂
2
 dx
I X = − ∫ f ( x) 
−∞
∂x  f ( x)
In this paper we approximate the PDF with the kernel density estimation technique.
Specifically, the PDF is approximated by:
1 N  x − si  (3)
fˆN ( x, λ ) = ∑ K
λN i =1  λ 

where si is the i-th pressure measurement, K is the kernel function and λ is the chosen
bandwidth (14). A popular choice for the kernel is the Epanechnikov kernel given by:
3 (4)
 (1 − u 2 ) if u ∈ [−1,1]
K (u ) =  4
 0 if u ∉ [ −1,1]
The kernel, K(u), in eq. (4) is a continuous non-negative and symmetric function
∞
satisfying ∫
−∞
K (u )du = 1 . The bandwidth, λ, is estimated by minimizing the integrated
mean squared error (IMSE):
∫ ( f ( x) − fˆ )
∞
2
IMSE (λ ) = N ( x, λ ) dx (5)
−∞
Faraway and Jhun (14) proposed the estimation of the optimal λ with the bootstrap. As
an example, Fig. 3 illustrates the estimation of the PDFs for the different conditions of U
and Gs in Table 1 at the bottom of the reactor.
Fig. 3. PDF estimations for conditions 1 and 2 in Table 1 at the bottom of the reactor
STATISTICAL RESULTS
Figure 4 shows the relationship between the calculated Shannon entropy, HX, and the
U/Gs ratio for all conditions. The HX increases with an increase in U and Gs. Several
observations can be made from this figure; first, there is a significant drop in the entropy
with an increase in the U/Gs ratio for all locations in the reactor. Second, there exists a
significant difference between the entropy at the top of the reactor compared to that at
the middle and bottom of the reactor. Therefore, there is significantly less variation or
chaotic behavior of the fluidization process at the top of the reactor compared to the
middle and bottom of the reactor.
Figure 5 shows the relationship between the IX and the U/Gs ratio. Similar trends to the
HX are observed for the IX; IX decreases for an increase in the U/Gs ratio. Again, the IX
illustrates that there is significantly less variation at the top of the reactor compared to
the middle and bottom of the reactor.
7.0 0
top
middle
6.5 bottom -2
4
IX×10
Hx
6.0 -4
top
5.5 -6
middle
bottom
5.0 -8
0.10 0.15 0.20 0.25 0.30 0.35 0.10 0.15 0.20 0.25 0.30 0.35
3 3
U/Gs, m /kg U/Gs, m /kg
Fig. 4. Shannon entropy, HX, as a function Fig. 5. Fischer information, IX, as a

of U/Gs function of U/Gs
250 Comparing with previous work (7), Fig. 6
top
middle
shows the relationship between the
200 bottom standard deviation, σ, and U/Gs. Trends
are similar to the HX and the IX; the σ
σ, Pa
150
decreases with an increase in U/Gs.
Again, σ illustrates that there is
100
significantly less variation in the
fluidization process at the top of the
50
0.10 0.15 0.20 0.25 0.30 0.35 reactor compared to the middle and
3
U/Gs, m /kg bottom sections of the reactor.
Fig. 6. Standard deviation, σ, as a function
of U/Gs The differences in the measures of
variability, i.e. HX, IX, σ (also referred to
as responses) between the locations in the reactor, as well as the relationship with
U/Gs, can be quantified by constructing a statistical model to predict the measure of
variability as a function of the location and U/Gs (15). Specifically, the linear model is of
the form:
yi = τ i z i + βx (6)
where yi is the response variable for the i-th point or height in the reactor where the
pressure measurements were made, i.e. top, middle or bottom, respectively; τi is the
effect of the i-th location in the reactor on the response, and zi is the dummy variable
indicating the location in the reactor, i.e. zi = 1 for the i-th location and zero otherwise. In
Eq. (6) x is the U/Gs ratio, and τi (i=1, 2, 3) and β are parameters to be estimated from
the least squares minimization.
Table 2. Parameters for linear models describing HX, IX and σ

Measure Location Regression information
Intercept, τ Slope, β Standard error p-value

IX bottom 0.00032 -0.00216 0.00007 0.0001
middle 0.00031
top 0.00005
HX bottom 7.447 -4.873 0.13 0.0001
middle 7.403
top 6.803
σ bottom 293.62 -594.74 20.05 0.0001
middle 288.09
top 211.44
Table 2 shows the results of fitting the Eq. (6) to the three measures of variability, HX, IX
and σ. The standard error of the model, i.e. the square root of the sum of squares of
errors divided by the number of observations minus 2, is very small for each model
(note the standard error of the model is in the same units as the response). The p-value
indicates the significance of the model, i.e. a p-value smaller than 0.05 indicates a 95%
confidence in the relationship between the variables and the measure of variability.
Clearly, all three models in Table 2 are highly significant.
7.0 2
bottom bottom
middle middle
top top
0
6.5
-2
4
IX ×10
HX
6.0
-4
5.5
-6
5.0 -8
0.10 0.15 0.20 0.25 0.30 0.35 0.10 0.15 0.20 0.25 0.30 0.35
3 3
U/Gs, m /kg U/Gs, m /kg
Fig. 7. Predicted entropy, HX, as a function Fig. 8. Predicted Fischer information, IX, as
of U/Gs a function of U/Gs
250 Equation (6), with the parameters in
bottom
Table 2, can be used to predict the
middle
200 top
measures of variability for a given U/Gs
150 and location in the reactor. As an
σ, Pa
illustration, Fig. 7 shows the predicted

100
entropy, HX, as a function of U/Gs and
50 the location in the reactor. The 95%
confidence bands are also indicated for
0
0.10 0.15 0.20 0.25 0.30 0.35 each model. The 95% confidence band
U/G , m /kg s
3
indicates the area about the regression
Fig. 9. Predicted standard deviation, σ, as a model that captures the true relationship
function of U/Gs with 95% confidence. Note the
significant difference between the
relationship at the top of the reactor to the relationship at the bottom and middle of the
reactor. Figures 8 and 9 show the predicted Fischer information, IX, and the standard
deviation, σ, respectively as a function of U/Gs and the location in the reactor. Similar
trends to the entropy are observed.
CONCLUSIONS
The Shannon entropy analysis and Fisher information matrix analysis of pressure
fluctuations are promising techniques to study the dynamics of gas-solid flow in
fluidized beds. In this study, effects of two operating variables namely the superficial
gas velocity, U, and solids circulation flux, Gs, on the Shannon entropy and Fisher
information at different bed locations were determined. Both HX and IX follow the same
trend; they decrease with increasing U/Gs. This result suggests that the fluidization
process in CFBs with lower solids concentrations can be less chaotic than that in CFBs
with high solids concentrations. The analysis also shows less variation at the top of the
riser compared to its middle and bottom sections.
Simple linear statistical models have been developed to quantify the relationships
between the measures of variability and U/Gs. The standard errors for these models are
very small indicating that they are highly significant. The results confirm that both
techniques can be use as tools to understand the complex dynamic behavior of gas-
solid flows in CFBs.
ACKNOWLEDEMENT
Experimental data utilized in this paper were collected in the CFB cold model at Mintek.
NOTATION
Gs – solids flux, kg/m2·s U – gas velocity, m/s

HX – Shannon entropy x – pressure vector
IX – Fisher information β – parameter in Eq. (6)
K(u) – kernel function λ – band width
N – number of pressure measurements σ – standard deviation
REFERENCES
1. M. Hartman, O. Trnka and K. Svoboda (2009). Ind. Eng. Chem. Res. 48: 6830.
2. L. de Martin, J. Villa Briongos, J.M. Aragon and M.C. Palancar (2010). Chem. Eng.
Sci. 65: 4055.
3. A. Luckos and P. den Hoed (2004). Ind. Eng. Chem. Res. 43: 5645.
4. A. Luckos and P. den Hoed (2005). In K. Cen (ed.) Circulating Fluidized Bed
Technology VIII: 231–238. International Academic Publishers, Beijing.
5. A. Luckos and P. den Hoed (2005). In A. Luckos and P. Smit (eds.) IFSA 2005,
Industrial Fluidization South Africa: 345–355. SAIMM, Johannesburg.
6. A. Luckos, Q.G. Reynolds and P. den Hoed (2007). In X. Bi, F. Berruti and T.
Pugsley (eds) Fluidization XII: 145–152. ECI, New York.
7. R.L.J. Coetzer, A. Luckos and P. den Hoed (2008). In T. Hadley and P. Smit (eds.)
IFSA 2008, Industrial Fluidization South Africa: 428-444. SAIMM, Johannesburg.
8. L. Telesca, R. Caggiano, V. Lapenna, M. Lovallo, S. Trippetta and M. Macchiato
(2008). Physica A 1: 6.
9. U. Lackermeier and J. Werther (2002). Chem. Eng. Process. 41: 771.
10. C.M.H. Brereton and J.R. Grace (1993). In A.A. Avidan (ed.) Circulating Fluidized
Bed Technology IV: 137–144. AIChE, New York.
11. Q.-Y. Zheng and H. Zhang (1995). In Fluidization VIII, Preprint, Vol. 2: 657–664.
Progep, Toulouse, France.
12. T. Pugsley, D. LaPointe, B. Hirschberg and J. Werther (1997). Can. J. Chem. Eng.
75: 1001.
13. Y. Jin, Z. Yu, C. Qi and D.-R. Bai (1988). In M. Kwauk and D. Kunii (eds.)
Fluidization’ 88 Science and Technology: 165–173. Science Press, Beijing.
14. J.J. Faraway and M. Jhun (1990). J. American Statistical Association 85: 1119.
15. D.C. Montgomery (2001). Design and analysis of experiments. John Wiley & Sons,
Inc.
TIME-RESOLVED X-RAY TOMOGRAPHY OF A
FLUIDIZED BED OF GELDART A PARTICLES
R.F. Muddea , Q. Ricouxb , E.C. Wagnera and J.R. van Ommenb
a
Kramers Laboratorium voor Fysische Technologie (r.f.mudde@tudelft.nl)
b
Department of Chemical Engineering
Delft University of Technology
Pr.Bernhardlaan 6, 2628 BW Delft, The Netherlands.
ABSTRACT
This paper discusses the influence of fines on the size of bubbles moving through a 23 cm
ID fluidized bed of Geldart A particles imaged with an X-ray Tomographic Scanner. In earlier
work [1], the bubble distribution in a fluidized bed of Geldart B particles was shown. The
current study using Geldart A particles is more challenging to the reconstruction algorithm,
since there are more bubbles, and they are smaller in size. We study the influence of adding
fines (i.e. particles ≤ 45 micron) to the system. When adding a mass fraction of fines of 24%,
we find a decrease of the average bubble of 40% of the size for the original powder, in line with
earlier results from pressure probes and optical probes [2]. We find that the entire distribution
of the bubble sizes shifts to smaller values.
INTRODUCTION
Many catalyzed gas reactions are performed in fluidized beds. The small particle size in combi-
nation with the low pressure drop are favorable for several applications. For higher gas through
puts, part of the gas will flow through the fluidized bed in the form of void or bubbles. Although
these bubbles are important when it comes to mixing of the powder, they have negative effects
on the conversion as not all gas is now always in contact with the catalytic material. As shown
in [2], a reduction of the bubble size by 40% may lead to an increase in conversion by 50%.
Various papers have discussed the possibilities of reducing the bubble size. For instance, in
[3] different gas injection strategies were employed. In the same article, the authors used elec-
trical fields to influence the interparticle forces. In both cases a reduction of the bubble size
was observed. The addition of fines is another possibility to improve the conversion [4], [5].
Beetstra et al. ([2]) reported experiments on the influence of fines on the fluidization behaviour
of porous alumina particles. They added up to 50% fines to their powder and find, from pres-
sure fluctuation analysis, a decrease of the average bubbles size with increasing mass fraction
of fines. However, for the lower superficial gase velocities they investigated an increase was
observed. Nevertheless, the trend was clear: for higher superficial gas velocities the average
bubble size decreased monotonically with increasing mass fraction fines. From video images
taken in a pseudo 2D bed, the authors found a clear shift in the bubble size distribution: for the
higher gas velocities the entire distribution moved to smaller values with a smaller standard
deviation (in absolute values).
In the present paper, we report experiments using our three source fast X-rays tomographic
scanner and a 23cm fluidized bed. Tomographic systems have the advantage of being non-
intrusive, while at the same time giving bubble properties such as size and shape. A few dif-
ferent tomographic techniques are in use, such as Electrical Capacitance Tomography (ECT,
[6], [7]) and nuclear densitometry. ECT has the advantage of being fast and relatively cheap.
However, its spatial resolution is problematic due to the soft nature of the electric fields used.
The trajectory of the field lines is influenced by the gas-solid distribution, leading to a more
cumbersome reconstruction ([8]). On the other hand, γ and X-rays are hard fields that, in prin-
1
ciple provide a better spatial resolution. They are, however, costly and due to inherent noise
usually slow ([9], [10], [11], [12]). Recently, the time resolution of X-ray tomographic scanners
has been considerably improved ([13], [14], [15], [16]).
We study the bubble size distribution of a Geldart A powder to which in steps a certain mass
fraction of fines (particle size smaller than 45µm) is added. We reconstruct individual bubbles
and measure their size. At the same time, we obtained the bubble frequency, by counting the
number of bubbles passing the measuring plane in a given time interval.
EXPERIMENTAL SETUP
A 23cm inner-diameter perspex tube (wall thickness 5mm, height 71cm) is partially filled with
powder. As the base case, the column is filled with alumina particles (mean particle size = 146
µm; particle density 1300 kg/m3 ). These particles form a Geldart A powder close to the border
of the A-B line. The minimum fluidization velocity is 0.008m/s. Additionally, different amounts
of fines (also alumina) have been added during the experiments creating powders with a mass
fraction of 0%, 8%, 16% and 24% of fines. The total amount of particles in the bed was kept
at 14.5 kg, which gives a packed bed height of 40cm. The particle size distributions are given
in table 1; the minimum fluidization velocity for each powder in table 2.
cumm. fraction (%) 10 25 50 75 90 mean

base material (µm) 104 121 143 169 195 146
fines (µm) 19.3 26.0 33.7 42.1 50.3 34.0
Table 1: Particle size distribution.
fraction fines (%) 0 8 16 24

Umf (cm/s) 0.8 0.6 0.4 0.12
Table 2: Minimum fluidization velocity for the powders investigated.
Air (room temperature) is used as fluidization gas. It is either supplied via a wind box to the
bed through a porous plate (sintered bronze, pore size 30 to 70µm, plate thickness 7mm), or
via a single capillary (diameter 3.7mm) inserted in the bottom part of the bed. In the former
case, the wind box is filled with 2mm glass beads to generate an as even as possible air flow
into the bed. In the latter case the bed is not gassed through the porous plate: all air comes
out of the capillary. On top of the bed an expanded section is placed (diameter 44cm, height
79cm) acting as a free board. The air leaving the set up first passed a filter before being vented
to the surroundings. A schematic of the fluidized bed with the densitometer is given in Fig.1.
upper & lower
detector array 3
fluidized
bed X-ray
upper
source 1
detector
array
X-ray
source 2
fluidized bed
X-ray
source 1
ay r
upp ector
lower
or lowe
1
det
er arra
detector
arr
det per &
&
array
low y 2
ect
up
er
X-ray
source 3
Figure 1: Schematic of the X-ray scanner. Left: side view showing for clarity only one source
with its two detector arrays, right: top view.
2
The X-ray sources are placed at 120◦ around the fluidized bed. Each source generates a fan
beam that is detected by two sets of 32 sensors placed opposite of the source. By using 2 sets,
two measuring planes are formed located at 34.1cm and 36.0cm above the distributor plate,
resp. The distance between the planes is 1.9cm. Comparing the raw signals allows estimation
of the velocity of passing bubbles and from that the bubble size in the vertical direction. The
distance from the X-ray-target to the center of the fluidized bed is 68.5cm, from the X-ray target
to the detectors is 138.6cm. The fluidized bed is placed on a table that can be moved up and
down in the vertical direction. This way we can adjust the height of the measuring plane in the
column.
The X-ray sources used are manufactured by Yxlon International GmbH. The maximum X-ray
energy is 150keV. We operate the sources at a low energy flux with a tube current less than
1mA. The detectors all consist of a CdWO4 scintillation crystal optically coupled to a PIN photo
diode. They are manufactured by Hamamatsu (type: S 1337 - 1010BR). Their crystal size is
10mm*10mm*10mm. A plastic casing in the form of an arc holds two horizontal arrays of 32
detectors. The curvature of the array is such that the distance to the focal point of the source
is equal for all detectors. The data are collected simultaneously at a sampling frequency of
2500Hz, both for the upper and lower ring of detectors. The measured data are read out using
a 12 bit ADC-card. The entire process is controlled via a workstation that sends out the trigger
signals to the sources and reads out the detectors.
TOMOGRAPHIC RECONSTRUCTION
Measuring Principle
Each detector measures the attenuation of the X-rays in a thin cone. In the reconstruction this
is treated as a thin line. If such a line of mono-energetic γ- or X-rays is transmitted through a
closed system containing a particle-gas two-phase mixture, the number of photons registered
per second, R, follows from the Lambert-Beer law:
R = R0 exp [− ((1 − α)µp + αµg ) d] (1)

where R0 is the number of photons registered per second when the system is in vacuum;
µp and µg denote the linear absorption coefficient of the particle and gas phase; α is the
volume fraction of the gas phase; d is the inner diameter of the system. It should be noted that
the attenuation characteristics of the fluidized bed wall is incorporated in R0 . X-ray sources
generate a wide spectrum of X-ray energies. The attenuation coefficients, µp and µg , are
functions of the photon energy E. Therefore, a two-point calibration is inadequate, as the
absorption of the photons of lower energy is much faster. In order to deal with this, we have
calibrated all detector individually by placing various amounts of packed powder in between a
source and its detectors. The amount of packed powder is put inside the column to ensure
that the calibration encompasses the effects of the walls of the column. Furthermore, the
calibration includes a completely empty and a completely filled bed. These two calibration
points provide the upper and lower limit of the signal. We fitted a smooth function of the form
Acal + Bcal · exp (−x/Ccal ) to the data, with x the distance traveled by the beam through the
powder phase. For every detector, an individual curve is obtained, see [13].
Reconstruction
We use an Algebraic Reconstruction Technique. Although significantly slower than e.g. Linear
Back Projection, algebraic methods offer more flexibility in terms of limited data sets and are
more appropriate for the CT configuration system under consideration here. Detailed accounts
of reconstruction techniques can be found in [17], [18] or [19].
We use the calibration curve to convert the measured line-averaged attenuation into a line
averaged solids fraction. We will reconstruct the solids fraction α(x, y) in a pixel representation
of the cross-section of the fluidized bed. Here, we use a square pixel array of 55*55 pixels. The
cross-section of the fluidized bed exactly fits in this square. All pixels outside the circle have a
3
solids fraction of zero. For a given ray, traveling through the object, the total solids fraction on
the line, pi , referred to as ray sum, can be estimated as
X
N
p̃i = Wik αk (2)
k=1
with αk the pixel-based value of the solids fraction distribution and Wik the weighing factor
for pixel k for the ith ray through the object. We use a linear weighing matrix W . Hence, the
weighing factor Wik is the length of ray i through pixel k.
To reconstruct the image we need to solve the unknown pixel-averaged solids fraction αk
from eq.(2) for M different rays on N pixels. As the number of independent measurements
is only 3*30=90 and the number of unknown pixels is easily 1000 or more, the problem is
ill-posed. Moreover, there will be measuring noise in the data. The Algebraic Reconstruction
Techniques (ART, see e.g. [17]) are designed to minimize the mismatch between the data p~
and W · α ~ . They are iterative methods that solves p~ = W · α ~ . We use the Simultaneous
Algebraic Reconstruction Technique (SART) [20]. Instead of sequentially updating the pixels
on a ray-by-ray basis, SART simultaneously applies to a pixel the average of the corrections
generated by all rays. This offers a reduction in the amplitude of the salt and pepper noise
that is usually present in ART. However, it goes at the expense of the computation time. Still,
pepper and salt noise will be present in the images. This can be reduced by using a so-called
one-step-late algorithm (see [21]). We invoked an algorithm based on the median root function
(suggested first by [22]). It effectively removes pepper and salt noise, but keeps the edges of
larger objects sharp enough, see e.g. Mudde et al. [13] for full details about the reconstruction
algorithm.
X-ray sources are inherently noisy. This noise corrupts accurate reconstruction of the images
of the bubbles as they are cut out by the measuring plane. Therefore, we have averaged the
data first over a period of 10 data points and moved in steps of 10 time steps through the data
series for each new reconstruction. This obviously reduces the time resolution of the images
from 2500 frames per second to 250 frames per second. For the reconstructions a square
pixel array of 55*55 pixels is used. The fluidized bed just fits in this square. Each pixel has a
size of 4.188mm. Pixels outside the cross-sectional area of the fluidized bed are during the
reconstruction set to zero. Fig.2 shows a quasi-3D reconstruction of the bubbling bed. The
reconstructed images (at a frame rate of 250Hz) are stacked vertically. Note that the data are
gathered in one plane: the vertical axis in the figure is time rather than the vertical coordi-
nate (the two horizontal axis are in pixels; the unit for the vertical axis is 4ms). Note that the
rectangular box shown in Fig.2 does not coincide with the outer dimensions of the fluidized
bed, which is cylindrical in shape: a horizontal cross-section of the fluidized bed is a circle
that exactly fits in a horizontal cut through Fig.2. Bubble travelling along the wall region of the
fluidized bed, therefore look like moving internal through this box. However, they actually tough
the wall of the bed.
It is noted here, that with the X-ray scanner and the reconstruction algorithm used we can
confidently detect bubbles with a diameter of 2.5cm and above. Smaller bubbles can still be
detected, but not with the same accuracy as the bigger ones. The influence of noise and
small misalignments as well as the uncertainty in the calibration data put a lower limit to the
diameter of the bubbles. To estimate the accuracy of small bubbles we performed a test on
static phantoms. For this, we filled the bed with the Geldart A powder and places hollow
cylinders of various diameters in the bed. In the measuring planes these cylinders should be
visible as circular voids. As this is a steady state experiment there is no motion blurring and the
measured data should yield the best possible reconstructions. For a cylinder with a diameter
of 1.28cm, i.e. an area of 1.29cm2 , we reconstruct an area of 1.03cm2 , thus a diameter of
only 1.14cm. if we put in more cylinders at the same time, reconstruction of the smaller ones
4
Figure 2: Reconstructed images stacked to form a quasi 3D image of the bubbles in the bed.
The rectangular box does not show the wall of the fluidized bed, but is the stacking of the
square reconstruction grid used.
becomes more problematic: occasionally ghost images of non-existing small cylinders show
up. This is caused by noise in the data and by slight misalignment of the detectors. Note, that
the value of each pixel is between 0 (fully packed) and 1 (no particles in pixel). To find the edge
of teh bubbles, we used a threshold value of 0.5.
Gas Jet Experiments

Two types of experiments are performed. In the first one all air is sparged via a single capillary.
This way a bubble train is generated. This has the advantage that we know a priori that only one
bubble a time will be present in the reconstructed planes, making interpretation of the recon-
structed solids distribution straight forward. The bubble diameter is obtained from the recon-
structed images by taking the image in which a bubble shows its maximum area for each indi-
vidual bubble. From that we estimate the bubble size according to Db = xmax −xmin +y 2
max −ymin
.
Here, xmax , xmin denote the maximum, respectively minimum x-coordinate of all pixels com-
prising the bubble cross-sectional area, in the x-direction of the reconstruction grid. Similarly,
ymax , ymin denote those in the y-direction. Subsequently, this bubble diameter is converted
to centimeters using the known column diameter (23cm) and the number of grid points per
direction (i.e. 55).
Experiments are run at two different gas velocities: Ujet = 46.5 cm/s and 93cm/s, i.e. a super-
ficial velocity of 1.20cm/s and 2.41cm/s, resp. The averaged bubble size is computed from 10
different runs, each of 5 seconds data collecting and separated by 15 minutes between two
subsequent runs. In total at least 140 bubbles are detected and used to compute the average
bubble size. The effect of the mass fraction of fines is shown in Fig.3(a). It is clear from the
data that the bubble size significantly decreases when increasing the mass fraction fines. From
the measurements, we also obtain the bubble frequency, i.e. the number of bubbles passing
the measuring plane per unit time, see Fig.3(b) where we show the bubble frequency for the
high velocity jet case. The bubble frequency increases when increasing the mass fraction of
fines. However, in the case of jet gassing, the increase of the frequency is only 30% for the
lower gas velocity and 50% for the higher gas velocity case. Fig.3(a) shows a decrease of
40% of the mean bubble diameter. Consequently, based on the mean size, the bubble volume
is only 22% of the bubble volume at 0% fines. Hence, the visible bubble rate, calculated as
5
φb = fb Vb , decreases to 28% of the visible bubble rate without the addition of fines for the
lower gas inlet velocity and to 33% for the higher gas velocity used in the experiments. Appar-
ently, considerably more gas is moving through the powder phase when introducing fines in
the system. It should, however, be noted here that the bed is not fully fluidized; a considerably
amount of the dense phase is in the packed state.
5
10
jet, 93cm/s 4
8 p, 10cm/s
Db jet, 46.5cm/s fb
p, 10cm/s 3
6 p, 6cm/s
(cm) (Hz)
4 2
jet, 93cm/s
2 1
0 5 10 15 20 25 0 5 10 15 20 25
mass fraction fines (%) mass fraction fines (%)
(a) Evolution of the bubble size as a function of the (b) Relative bubble size as a function of the mass
mass fraction fines: squares for the jet, black square fraction fines. Filled squares: jet Ujet = 93 cm/s,
Ujet = 93 cm/s, open square for Ujet = 46.5 cm/s; filled circles porous pate: Usup = 10 cm/s.
circles for the porous plate (denote by p), grey circle
for Usup = 10 cm/s, open circle for Usup = 6 cm/s.
Figure 3: Average bubble size and bubble frequency.
Fig.4 shows the bubble size distribution for Ujet = 46.5 cm/s for the original powder (0% fines)
and for the 24% mass fraction fines case. Clearly the entire distribution has shifted to smaller
values. Similar findings have been reported for a pseudo 2D bed, based on video images by
[2]. For both cases shown in Fig.4 the standard deviation of the distribution is about 1.5 cm.
0.4
24%
0%
fraction (-)
0.3
0.2
0.1
0
1 2 3 4 5 6 7 8 9 10 11 12
bubble size (cm)
Figure 4: Bubble size distribution for two cases (Ujet = 46.5 cm/s): black bars 0% fines, white
bars 24% fines.
Uniform Gassing
Similar experiments as described in the previous section have been performed using the
porous plate as gas distributor. Although we tried to get the gas distribution as uniform as
possible of the cross-section of the distributor of the plate, we observed that there was a slight
tilt in the spatial bubble distribution. In Fig.3(a) also the average bubble size for gassing via the
porous plate is shown as a function of the mass fraction fines for two superficial gas velocities,
Usup = 6.0 cm/s, 10.0 cm/s resp. Again, a clear decrease in bubble size is found. In this case
the bubble size drops to only 60% of the original one. The values found are in reasonable
6
agreement with the Darton et al. equation [23], which predicts 5.7 and 4.5 cm diameter, re-
spectively. However, the Darton et al. equation predict a slight increase in bubble diameter
with increasing fines fraction (since the mimimum fluidization velocity is decreasing), while we
find a strong decrease in bubble diameter. Fig.3(b) shows the increase in bubble frequency.
For these conditions the increase in bubble frequency is much higher than for the jet-case.
Consequently, the visible bubble rate drops less than in the jet experiments, but the drop is
more relevant in this case, since the dense phase is fully fluidized at all fines fractions. At the
highest mass fraction of fines (24%) the relative visible bubble rate is only 76% of that without
fines. Clearly, a larger fraction of the gas flows through the particle phase when introducing
fines. This is very important for catalyzed gas phase reactions, in which this will lead to higher
conversions and often to higher selectivities.
CONCLUSIONS
In this paper, we used our fast X-ray tomographic scanner to investigate the influence on the
bubble size when adding fines to a Geldart A powder (alumina, average particle size 146.4
µm; close to the B-border). We performed two experiments. In the first one, all gas is sparged
through a single capillary, mounted in the bottom of the bed, into the powder. In the second
one, the gas is introduced via a porous plate over the entire bottom of the fluidized bed. In both
case the mass fraction of fines added was 8, 16 and 24%. We find a clear decrease in the bub-
ble size and an increase in the bubble frequency. The average bubble size may decrease to
only 60% of the mean bubble size without adding fines. The increase of the bubble frequency
is insufficient to make up for this volume decrease and we conclude from the measurements
that more gas flows through the powder mass when fines are present.
Our data agree with those reported by [2] based on pressure analysis and optical probes.
The advantage of the X-ray scanner over pressure sensing is a more direct assessment of
the bubble properties. Compared to the optical probe, the X-ray technique is, obviously, non-
intrusive. Moreover, with the tomographic reconstruction the entire bubble is imaged, whereas
the optical probe can only measure the chord length, which needs to be converted back, via a
probabilistic approach, into the bubble size distribution. We can conclude that, due to its mea-
suring speed, the X-ray tomographic scanner is a welcome new technique to experimentally
study bubbling fluidized beds.
NOTATION
Acal , Bcal , Ccal calibration coefficient
Db estimated bubble diameter m
d path length of beam through material m
fb bubble frequency −1
pi total solids fraction on X-ray beam (ray sum) -

R photon count rate s−1
R0 photon count rate in vacuum s−1
Ujet gas velocity through capillary m/s
Usup superficial gas velocity m/s
Vb bubble volume m3
v velocity m/s
Wik weighing matrix -
x path length of beam through powder phase m
x, y Cartesian coordinates in measuring plane m
α gas volume fraction -
∆t time interval s
φb visible bubble rate m/s3
µg linear absorption coefficient of gas m−1
µp linear absorption coefficient of particle m−1
7
REFERENCES
1. Mudde, R.F., Time-resolved X-ray tomography of a fluidized bed, Powder Techn., 199,
55-59 (2010).
2. Beetstra, R., Nijenhuis, J., Ellis, N. and Van Ommen, J.R., The influence of the particle size
distribution on fluidized bed hydrodynamics using high-throughput experimentation, AIChE J.,
55 (8), 2013-2023.
3. van Ommen, J.R., Nijenhuis, J., van den Bleek, C.M. and Coppens, M.O., Four ways to
introduce structure in fluidized bed reactors, Ind. & Eng. Chem. Res., 46, 4236-4244 (2007).
4. Yates, J.G. and Newton, D., Fine particle effects in a fluidized-bed reactor, Chem. Eng.
Sci., 41, 801-806 (1986).
5. Sun, G. and Grace, J.R., The effect of particle size distribution on the performance of a
catalytic fluidized bed reactor, Chem. Eng. Sci., 45, 2187-2194 (1990).
6. Beck, M. S., Dyakowski, T., and Williams, R. A., Process tomography - the state of the art,
Trans. Inst. Meas. and Control, 20(4), 163-177 (1998).
7. Warsito, W. and Fan, L.-S., Dynamics of spiral bubble plume motion in the entrance region
of bubble columns and three-phase fluidized beds using 3D ECT, Chem. Eng. Sci., 60, 6073-
6084 (2005).
8. Van Ommen, J.R. and Mudde, R.F., Measuring the Gas-Solids Distribution in Fluidized
Beds - A Review, Int. J. Chem. Reactor Eng., 6, Article no. R3 (2008).
9. Duduković, M.P., Opaque Multiphase Reactors: Experimentation, Modeling and Trou-
bleshooting, Oil & Gas Sci. Techn., 55 (2), 135-158 (2000).
10. Kumar, S.B., Moslemian, D. and Dudukovic, M.P., A γ-ray tomographic scanner for imag-
ing voidage distribution in two-phase flow systems, Flow Meas. Instr., 6 (1), 61-73 (1995).
11. Kumar, S.B., Moslemian, D. and Dudukovic, M.P., Gas holdup measurements in bubble
columns using computed tomography, AIChE J., 43, 1414-1425 (1997).
12. Mudde, R.F., Harteveld, W.K., Van den Akker, H.E.A., Van der Hagen, T.H.J.J. and Van
Dam, H., Gamma radiation densitometry for studying the dynamics of fluidized beds, Chem.
Eng. Sci., 54, 2047-2054 (1999).
13. Mudde, R.F., Alles, J. and Van der Hagen, T.H.J.J., Feasibility study of a time-resolving
X-ray tomographic system, Meas. Sci. & Techn., 19, 085501 (2008).
14. Mudde, R.F., Bubbles in a fluidized bed: a fast X-ray scanner, AIChE J., online: 29 Nov.
(2010).
15. Bieberle, M. and Hampel, U., Evaluation of a limited angle scanned electron beam x-ray
CT approach for two-phase pipe flows, Meas. Sci. Technol., 17, 2057-2065 (2006).
16. Bieberle, M., Fischer, F., Schleicher, E., Hampel, U., Koch, D., Aktay, K.S.D.C., Menz, H.-
J. and H.-G. Mayer, Ultrafast limited-angle-type x-ray tomography, Appl. Phys. Lett., 91 (12),
123516 (2007).
17. Brooks, R. A. and DiChiro, G., Principles of computer assisted tomography (CAT) in
radiographic and radioscopic imaging, Phys. Med. Biol., 21, 689-732 (1976).
18. Herman, G. T., Image reconstruction from projections - the fundamentals of computerized
tomography, Academic Press, 1980.
19. Kak, M. and Slaney, M., Principles of computerized tomographic imaging, IEEE Press,
New York, 1988.
20. Andersen, A. H. and Kak, A. C., Simultaneous algebraic reconstruction technique (SART):
a superior implementation of the ART algorithm, Ultrasonic Imaging, 6, 81-94 (1984).
21. Green, P. J., Bayesian reconstruction from emission tomography data using a modified
EM algorithm, IEEE Trans. on Med. Imag., 9, 84-93 (1990).
22. Alenius, S. and Ruotsalainen, U., Bayesian Image reconstruction for emission tomography
based on median root prior, Eur. J. of Nucl. Med., 24, 258-265 (1997).
23. Darton, R.C., La Nauze R.D., Davidson, J.F. and Harrison, D., Bubble growth due to
coalescence in fluidised beds, Trans. I. Chem. E., 55, 274-280 (1977).
8
ENERGETIC OPTIMIZATION OF THE LIGNIN PYROLYSIS FOR
THE PRODUCTION OF AROMATIC HYDROCARBONS
Miika Franck, Ernst-Ulrich Hartge, Stefan Heinrich, Bea Lorenz, Joachim Werther
Institute of Solids Process Engineering and Particle Technology
Hamburg University of Technology, Hamburg, Germany
ABSTRACT
The energy supply of the endothermic lignin pyrolysis process in a circulating
fluidized bed is to be achieved by recirculation of bed material, which is heated by
combustion of the by-products char and permanent gases in a separate combustor.
The feasibility of this concept is examined by the investigation of the yield of the by-
products in pyrolysis experiments, char combustion kinetics, the pyrolysis energy
demand and the combustion energy of the char and the non-condensable gases. It
is shown that the integrated pyrolysis-combustion process is feasible and even
produces an energy surplus of 4 MJ/kg raw lignin, which can be used in the
downstream processing of pyrolysis products.
INTRODUCTION
As a waste material in the bioethanol production and the celluloses industry lignin is
a source for aromatic hydrocarbons. It is built up from three-dimensionally
connected phenylpropane units, which upon thermal degradation are a rich source
for phenolic compounds for synthesis of chemicals (1) to (3).
One of the most promising concepts for the thermal decomposition of lignin is to use
a circulating fluidised bed (CFB) reactor for pyrolysis. The benefits of the use of a
CFB system are the short residence time of the pyrolysis vapours (the desired
product) and a high heating rate of the lignin, which are necessary to prevent further
degradation reactions and to achieve a high yield of liquid product. By-products of
the endothermic pyrolysis are non-condensable gases and char (4).
The aim of the present project is to optimize the endothermic pyrolysis process
energetically by integrating the combustion of the by-products into the solids
circulation loop of the CFB, by means of a bubbling fluidized bed. Furthermore, as
char components have been reported to catalyze secondary reactions of the
products to form lighter compounds (1, 5 and 6), the effect of catalysis shall be
minimized by the integrated combustion of the char.
EXPERIMENTAL
To determine the design parameters for an integrated pyrolysis-combustion system,
experiments in a CFB pyrolysis reactor (Figure 1) with riser diameter of 80 mm and
a height of 1700 mm have been carried out at different operating conditions (Table
1). The lignin was pneumatically fed into the reactor through a nozzle with 6 mm
diameter at a velocity of 40 m/s. The superficial velocity directly above the distributor
plate u0,b is given in Table 1 as well as u0,t which is the superficial velocity at the riser
top, which includes the lignin conveying N2 as well as the pyrolysis gas and the
steam from vaporization of the lignin humidity. The solids flux in the riser could not
be measured. The composition of the non-condensable, permanent gas has been
monitored continuously throughout the experiments. The bed material (BM) as well
as the material from the secondary cyclone (2C) have been collected after each test.
The material properties, i.e. composition, particle morphology, particle size
distribution and particle density were analyzed.
These properties
have been used to
2C
determine the char
combustion kinetics in
a laboratory-size
1C
Electrostatic
fluidized bed reactor.
precipitator
At the temperatures
Scrubber
Demister
700, 750, 800, 850
Pyrolysis reactor
and 900°C the

samples of the
materials with known
mass mS and carbon
content γC were
injected batchwise
into the reactor. The
gas composition of
the flue gas was
monitored and used
to calculate the
conversion Xchar(t). Figure 1: Experimental pyrolysis plant (80 mm riser diameter)
Moreover, the gross calorific values of the gas and the char together with their yields
were compared with the required heat for pyrolysis. The latter was estimated by a
simultaneous differential scanning calorimetry – thermogravimetric analysis (DSC-
TGA) experiment of lignin. In the experiment two lignin samples were heated in an
argon environment at a heating rate of 10 K/min in a thermal analysis apparatus,
type NETZSCH STA F1 Jupiter between room temperature and 900°C. The gross
calorific value of the char was determined by experiments with an adiabatic
calorimeter.
Table 1: Pyrolysis conditions

Exp. Lignin Fluidisation by steam Gas velocity at Pyrolysis
No. Feed rate uN2 H2O u0,b riser top u0,t temperature
kg/h m/s kg/h m/s m/s °C
1 2.76 40 24 5 5.7 650
2 2.57 40 24 5 5.7 600
THEORY
Due to the nature of the bed material particles, i.e. the char layer on the quartz sand,
the shrinking particle model (7) is modified, so that the particle shrinks upon
combustion until the inert sand core is reached. The modified model is subsequently
derived and called shrinking particle inert-core model.
Shrinking Particle Inert Core-Model

The shrinking of a particle can be described as follows:
dR
− ρ char = kCOn 2 (1)
dt
Therein ρchar is the density of the char, RP the mean radius of the char laden particle
at the entrance of the fluidized bed combustor, k the reaction rate constant, C O 2 the
mean oxygen concentration in the whole bed during the reaction, t the time and n
the reaction order. With the burnout time t = τ and the radius of the quartz sand core
R = RQS, the integration gives
ρchar ⋅ ( RP − RQS )
τ= (2)
kCOn 2
Analogously for an arbitrary time t < τ :
ρchar ⋅ ( RP − R)
t= (3)
kCOn 2
Dividing Eq. (3) by Eq. (2) results in
t  R 
= K1 ⋅ 1 −  (4)
τ  RP 
( )
with K 1 = 1 / 1 − RQS / RP . For a particle with inert core the conversion Xchar can be
expressed as
4
volume unreacted char 3
π R3 − RQS
3
( )
1 − X char =
total char volume
=
4
= K 2 ⋅ R 3 − RQS
3
( ) (5)
3
π RP3 − RQS
3
( )
(
with K 2 = 1 / RP3 − RQS
3
)
. Solving Eq. (5) for R and replacing R by the result in Eq. (4)
with subsequent differentiation results in
2
3R K 2  1 − X char  RQS  
3 3
3
dX char
= P
⋅ + 
dt τ K1  R 3P K 2  RP  
  (6)
2
2
3R K 2 ⋅ kC n  1− X R  
3 3
⋅  3 char +  QS  
P O2
=
ρchar  R P K 2  RP  
 
It should be noted that with RQS = 0 the equation reduces to the shrinking particle
formulation, that can be found in (7). The radius of the inert quartz sand core RQS is
calculated by the difference RQS = RP − d .
RESULTS
Pyrolysis Conditions and Solids Properties

For the determination of combustion kinetics it is necessary, that the composition of
the solid fuel (proximate and ultimate analysis), its density and morphology as well
as particle size distribution are known. The proximate as well as ultimate analysis for
the bed material (BM) and the material collected by the secondary cyclone (2C) are
listed, in Table 2. The difference of the inert and the ash fraction is equal to the sand
Table 2: Proximate and ultimate analysis as well as gross calorific value of solid
materials used for experiments
Sample composition (wt.-%)
Sample Proximate analysis Ultimate analysis HHV
Vola-
Water CFix Inert Ash C H N S O
tiles MJ/kg
Lignin 5.3 66.0 27.5 1.2 1.2 58.8 5.3 0.4 1.7 27.3 25.2
BM Exp. 1 0.7 1.5 6.9 90.9 12.1 9.3 0.3 0.0 0.3 0.0 29.0
2C Exp. 1 1.1 1.9 11.1 85.9 12.1 16.8 0.4 0.0 0.3 0.0 29.7
BM Exp. 2 0.8 1.4 7.3 90.5 7.2 8.2 0.3 0.0 0.2 0.0 30.2
2C Exp. 2 1.0 2.1 9.9 87.0 7.2 10.6 0.3 0.0 0.3 0.8 28.6
Reference state: raw except HHV: inert free; Water content of lignin at 60°C (due to
reactions at temperatures above 66°C)
fraction in the sample. The ash contents of the bed material as well as the
secondary cyclone material have been calculated by the ash content of the lignin
divided by the char yield YC. Latter is calculated by dividing the integral char mass
after an experiment by the integral of the fed raw lignin mass during the experiment:
mbed material after exp. + m2C material after exp. − mbed material before exp.
YC = (7)
mlignin fed during exp.
100
Cumulative mass in %
80
60
40
20 2C Exp. 2
QS F36
BM Exp. 2
0
0 100 200 300 400
Particle diameter in µm
Figure 2: SEM of the surface structure of Figure 3: Exemplarily particle size

a bed material particle’s coating fracture, distribution of BM and 2C of Exp 2 in
scale bar is 10 µm comparison with quartz sand
A SEM image of the bed material after pyrolysis experiment is shown in Figure 2.
On the picture a sand particle coated with a char layer can be recognized, with part
of the char layer broken apart. The particle size distribution of the secondary cyclone
material (2C) is bimodal, while Table 3: Sauter mean diameter DS, char layer
the distributions of the quartz thickness d and densities ρQS of the quartz sand
sand and the bed material (BM) and ρP of the bed material and the corresponding
are monomodal (Figure 3). This ρchar of the char
is due to the fragments of the DS d ρQS/ ρP ρchar
Sample 3
char coating shells, which are µm µm g/cm g/cm3
mainly found in the secondary Quartz sand 39.2 -- 2.63 --
cyclone material. The char BM Exp. 1 78.8 9.0 2.50 0.81
density ρchar was calculated 2C Exp. 1 35.8 -- -- --
from the composition of the bed BM Exp. 2 129.5 15.5 2.50 1.03
material and the densities of 2C Exp. 2 45.0 -- -- --
bed material and quartz sand. The average char layer thickness d has been
calculated, using the assumption of spherical particles.
These calculations have been validated by dimensioning of char layer fragments in

several SEM images (0.6 to 18.1 µm). The results are listed in Table 3.
Combustion Kinetics
The conversion of the char Xchar at an arbitrary time t is defined as the conversion of
carbon at that time. Therefore, the measured carbon content in the flue gas,
integrated over the time, is divided by the initial carbon mass of the sample:
mC (t ) in CO 2
X char = (8)
mS ⋅ γ C
1 Temperature in °C
900 850 800 750 700
-4
0.8
ln(k) with k in kg/(m s (mol / l) )
n
BM Exp. 2: n = 0.5
-4.5 ln(k) = -914.06/T - 3.443 BM Exp. 1: n = 0.5
0.6
Xchar
R2 = 0.5443 ln(k) = -1157.8/T - 3.9193

2
2
R = 0.7833
0.4 -5
2C Exp. 2: n = 0.5
SPIC-model ln(k) = -1143.2/T - 3.9937
0.2 Experimental data -5.5 R2 = 0.8871 2C Exp. 1: n = 0.5
ln(k) = -1028.4/T - 4.8865
2
Shifted SPIC-model R = 0.9816
0
0 10 20 30 40 -6
0.852406 0.890353 0.931836 0.977374 1.02759
t in s 1000/T in K
-1
Figure 4: Conversion of a BM Exp. 1 sample Figure 5: Arrhenius-plot of the analysed

in a combustion experiment at 850°C and materials
the correlative Shrinking Particle Inert Core
kinetic model conversion
The measured values Xchar(t) were fitted by the Shrinking Particle Inert Core-model
(Eq. (6)) with the fitting parameters k and n. An example of both curves for
BM Exp. 1 is given in Figure 4. Other than predicted by the Shrinking Particle Inert
Core-model, the slope of the conversion-curve is not maximal at the beginning and
also much smaller at higher reaction times than expected. Because of the
experimental setup, which comprises a quite long duct between the reactor and the
online gas measurement as well as a gas filter, dispersion effects cause the
deviation. This was checked by the introduction of a known square pulse to the
reactor. The pulse response needed about 8 s to reach the pulse amplitude and the
decay took about 16 s. These durations approximately relate to the response and
decay times in Figure 4. Therefore, the conversion curve computed by the Shrinking
Particle Inert Core-model was shifted by 8 s (Figure 4).
The resulting Arrhenius-plots for the four tested materials are shown in Figure 5 in
the temperature interval of 700 to 900°C with the obtained values for n and k.
Energy Balance
To establish an energy balance for the pyrolysis system with integrated by-product
combustion, the total heat release of the by-products related to the fed raw lignin
mass and the mass specific heat demand for lignin pyrolysis are specified below.
The combustion of the by-products shall take place at 850°C. Heat losses and
auxiliary energy demand, e.g. for feeding of lignin and preheating of the fluidisation
gas, have not been considered.
Pyrolysis Energy Requirement

The results of the thermal analysis of lignin are shown in Figure 6. It is very probable
that the first mass loss step belongs to the loss of moisture, whereas the other steps
are caused by devolatilization and pyrolytic cracking of the sample.
requirement q in MJ/kg raw lignin
100 1.2 2.5

DSC
2
0.8
Pyrolysis energy
80
DSC in W/g
1.5
TG in %
0.4
1
60
0 0.5
TG
0
40 -0.4 0 200 400 600 800 1000
0 200 400 600 800 Temperature in °C
Temperature in °C
Figure 6: Thermal analysis of lignin (DSC Figure 7: Approx. pyrolysis energy

and TGA) requirement per kg raw lignin
According to the mass loss endothermic or exothermic effects can be seen in the
DSC curve. The enthalpy of the single effects is difficult to determine, because the
effects interfere with each other. In the temperature interval of 200°C to 350°C it can
not be differentiated between endothermic or exothermic behaviour. To calculate the
energy demand for the pyrolysis the integral of the DSC signal qɺ is used (Eq. (9)).
T t
1
q= ⋅ ∫ qɺ dT = ∫ qɺ dt (9)
β T0 t0
The results are shown in Figure 7. The specific heat is related to the initial mass of
raw lignin. For the pyrolysis at a temperature of 650°C a mean value of about
1300 kJ/kg of raw lignin for the energy demand can be calculated.
Energy Supply
The yield of permanent gases, which contribute to a heat release upon combustion
(CO, CO2, H2, C1-C4 as CH4) rises with rising temperature. This result coincides with
the observations of Wei et al. (8), Scott and Piskorz (9), Zheng (10) and Di Blasi
(11). As with rising temperature secondary cracking reactions are favoured, the
more complex char and liquid molecules are converted to gases. Our
measurements have shown, that the composition of the permanent gas mixture
does not change considerably. This trend can also be found for the total heat
release by the combustion of permanent gas per mass of raw lignin fed to the
pyrolysis. The results are shown in Figure 8.
7 5
in MJ / kg raw lignin
4
Total heat release

in MJ/kg raw lignin
Total heat release
5
3
4
3 2
2
1
1 12 kg/h Steam BM Exp. 1 & 2
24 kg/h Steam 2C Exp. 1 & 2
0 0
600 650 700 750 800 600 625 650
Pyrolysis temperature in °C Pyrolysis temperature in °C
Figure 8: Total heat release of permanent Figure 9: Total heat release of char
gas combustion per kg raw lignin combustion per kg raw lignin
(combustion at 850°C) (combustion at 850°C)
On the other hand, because of secondary reactions as explained above, the yield of
char decreases with rising temperature, while the gross calorific value does not
change significantly (see Table 2). Therefore, the lignin specific total heat release of
char combustion decreases with rising temperature. This can be seen in Figure 9
and is in good agreement with the above cited literature.
At a pyrolysis temperature of 650°C, the energy demand for lignin pyrolysis is about
1500 kJ/kgL. The combustion of the by-products at this temperature releases about
3000 kJ/kgL for the permanent gases and 2500 kJ/kgL for the char. In the integrated
pyrolysis-combustion process this gives an energy surplus of 4000 kJ/kgL.
SUMMARY AND CONCLUSIONS

To couple a pyrolysis CFB reactor with an integrated combustion of the pyrolysis by-
products, char properties, combustion kinetics and the energy balance have been
investigated.
The quartz sand particles, which make up the bed material, are coated with char.
Therefore, a model for combustion kinetics has been derived, which accounts for the
fact that only a char layer with certain thickness is combusted. For the investigated
materials, the combustion kinetics have been determined by combustion
experiments in a laboratory scale fluidized bed. The combustion kinetics model does
fit the experimental data well.
The energy demand for lignin pyrolysis has been estimated by differential scanning
calorimetry. Pyrolysis experiments in a CFB reactor (80 mm diameter) were carried
out to identify the lignin specific energy in the by-products. At the pyrolysis
temperature of 650°C the combustion of permanent gases and char generates an
energy surplus of 4000 kJ/kgL. The surplus can be used for preheating the
fluidization gases and balancing the heat losses.
The obtained data is currently used to design a circulating fluidized bed pyrolysis
reactor with integrated fluidized bed combustor.
ACKNOWLEDGEMENT
This work has been carried out within the framework of the cluster Biorefinery2021,
funded by the German Federal Ministry of Research and Technology (FKZ
0315559A). The responsibility for the content of this work lies with the authors.
NOTATION
C Concentration β Heating rate K/min
d Char layer thickness µm γ Mass fraction --
DS Sauter mean diameter µm υ Temperature °C
n
k Reaction rate constant kg/(m²s(mol/l) ) ρ Density kg/m³
K Constant -- τ Burnout time s
m Mass kg
n Reaction order -- Subscripts
q Mass specific energy kJ/kg char Char
qɺ Mass specific heat flux W/kg C Carbon
R Radius µm L raw Lignin
t time s P Particle
T Temperature K QS Quartz sand
X Conversion -- S Sample, Sauter
Y Yield --
REFERENCES
(1) Amen-Chen C., Pakdel H., Roy C. (2001), Bioresource Technology 79, 3,
277–299.
(2) Bridgwater A. V., Meier D., Radlein D. (1999), Organic Geochemistry 30, 12,
1479–1493.
(3) Bridgwater A. V. (2003), Chemical Engineering Journal 91, 2-3, 87–102.
(4) Basu P. (2010) Biomass gasification and pyrolysis, Elsevier/AP. Amsterdam
(5) Park H., Park Y., Dong J., Jeon J., Kim S., Kim J. et al. (2009), Fuel
Processing Technology 90, 2, 186–195.
(6) Asadullah M., Anisur Rahman M., Mohsin Ali M., Abdul Motin M., Borhanus
Sultan M., Robiul Alam M., Sahedur Rahman M. (2008), Bioresource
Technology 99, 1, 44–50.
(7) Levenspiel O. (1999) Chemical reaction engineering, Wiley. Hoboken, NJ.
(8) Wei L. G., Xu S. P., Zhang L., Zhang H. G., Liu C. H., Zhu H., Liu S. Q.
(2006), Fuel Processing Technology 87, 10, 863–871.
(9) Scott D. S., Piskorz J. (1982), Canadian Journal of Chemical Engineering 60,
5, 666–674.
(10) Zheng J. L. (2007), Journal of Analytical and Applied Pyrolysis 80, 1, 30–35.
(11) Di Blasi C. (2009), Progress in energy and combustion science 35, 2, 121–
140.
THE INFLUENCE OF CARBON STRIPPER EFFICIENCY ON CO2-CAPTURE
RATE IN A CHEMICAL-LOOPING COMBUSTION PROCESS FOR SOLID
FUELS
Marvin Kramp, Andreas Thon, Ernst-Ulrich Hartge, Stefan Heinrich, Joachim Werther
Denickestrasse 15
21073 Hamburg, Germany
ABSTRACT
In the present work a Chemical-Looping Combustion process for solid fuels is simulated
on the 100 MW th scale. The coal is gasified inside the fuel reactor by recirculated CO2
and H2O. A carbon stripper downstream of the fuel reactor is used to reduce the
carryover of char from the fuel to the air reactor. The influence of the carbon stripper on
the CO2 capture rate is investigated. The results demonstrate the significance of the
carbon stripper in this process.
INTRODUCTION
Chemical-Looping Combustion (CLC) is an interesting variant for the inherent

separation of carbon dioxide inside a power generation process. It has recently
attracted much attention by numerous research groups (e.g. 1-4). Most research
focuses on the realization of CLC in two interconnected fluidized bed reactors. In
between these two reactors solids are circulated which transport chemically bound
oxygen taken up from the air inside the air reactor to the so called fuel reactor. The
oxygen carrier (OC) particles provide the fossil fuel (e.g. natural gas or coal) with
oxygen and will themselves be reduced. Reduced oxygen carrier particles are then
cycled back towards the air reactor for re-oxidation. CLC has the advantage that the
carbon dioxide of the off-gas will not be diluted by nitrogen. After condensation of water,
almost pure carbon dioxide can be obtained and transported to its designated storage
location.
If solid fuels are to be used in CLC, the complexity increases compared to gaseous
fuels. A scheme for a solid fuels CLC process is shown in Figure 1. The direct reaction
between the solid carbon and the oxygen bound to the solid oxygen carrier particles will
not proceed at a significant rate. Thus the solid carbon has to be gasified. In CLC it is
self-evident to recycle the fuel reactor off-gases consisting of H2O and CO2 to use them
as gasifying agents. During carbon gasification H2 and CO will be produced. The OC
particles will oxidize these intermediate products further towards H2O and CO2.
Gasification is a rather slow process compared to the reaction of CO and H2 with the
OC (5) and thus sufficient residence time of the coal particles in the fuel reactor must be
provided. On the other hand to yield a sufficient
flow of oxygen for fuel oxidation a rather large
circulation flow of OC particles is needed. The
solids flow leaving the fuel reactor consists of a
mixture of unreacted char particles, ash and
oxygen carrier particles. The char particles must
not enter the air reactor since they would combust
with the air-oxygen present. The formed CO2 would
not be captured and thus decrease the CO2 capture
rate of the plant. To reduce the amount of carbon
slip towards the air reactor a carbon stripper can be
used. The OC particles and the char particles can
be separated according to their terminal settling
velocity.
The aim of this investigation is to investigate how Figure 1: Scheme of a CLC

the CO2 capture rate is influenced by the carbon process for solid fuels
stripper.
THEORY
Char Gasification
In CLC both CO2 and H2O can be used for gasification of the coal char. It is repeatedly
reported in literature that steam gasification proceeds at a higher rate than carbon
dioxide gasification (e.g. 6). The net gasification reactions are shown in the following
equations:
C + β ⋅ H 2O → β ⋅ H 2 + ( 2 − β ) ⋅ CO + ( β − 1) ⋅ CO2 (1)
C + CO2 → 2CO (2)
The factor β in equation (1) was introduced by Matsui et al. (7) and summarizes the
following two reactions:
C + H 2O → CO + H 2 (3)
C + 2 H 2O → CO2 + 2 H 2 (4)
For this investigation β is set to 1.2 according to (7). A set of kinetic equations was
chosen that describes the gasification of coal char by CO2 and H2O (7,8).
Fuel Reactor Model
The fuel reactor is a bubbling fluidized bed, where the solid phase is assumed to be
ideally mixed. It was stated above that the fuel reactor should be fluidized by its own re-
circulated off-gas. Therefore the gas composition at steady-state is the same at the inlet
and the outlet of the fuel reactor. Accordingly the fuel reactor can be described
reasonably well by continuous stirred tank reactor characteristics. A corresponding
model has been set up that is able to handle multiple reactions and considers changes
in volume flow due to reaction. The release of volatiles is assumed to occur
instantaneously upon fuel introduction in the reactor. The composition of the volatiles is
calculated according to the model of Jensen (9). The model has been slightly modified
in order to neglect the formation of nitrous oxides and the sulfur content of the fuel. All
fuel nitrogen is therefore released as gaseous nitrogen. It is assumed that the particle
size distribution (PSD) of the char does not change during the initial devolatilization
process. During gasification a size reduction of the char particles is considered. It is
assumed that shrinkage is a process of external surface reaction:
dR m
= −k s   (5)
dt s
The PSD of the char at the exit of the fuel reactor is then calculated according to
Levenspiel (10). The reaction of volatiles and the gasification products with oxygen
carrier particles is usually much faster than the gasification of char. Accordingly the
concentrations of the aforementioned gases in the fuel reactor are set to zero due to
their reaction with oxygen carrier particles.
Carbon Stripper Model
The carbon stripper is simulated as a classifier. The grade efficiency is described by the
Rogers expression (11), which has been adapted for usage with settling velocities
instead of particle diameters and to neglect bypass of fines:
1
G ( ut ,i ) =  3
, (6)
 ut ,i 
α ⋅1−  
u  


 ut ,50 


1 +  t ,50  ⋅ e
 ut ,i 
with the grade efficiency G(ut,i ), defined as the ratio of mass fraction of the particle
settling velocity interval i in the coarse product and the mass fraction of the same
interval in the feed. The parameter ut,50 designates the cut terminal velocity (50 %-value
of the grade efficiency curve) and ut,i is the terminal settling velocity of the particles in
size interval i. The sharpness of the separation is defined by α, which can vary between
0.3 (diffuse separation) and 6.6 (analysis-sharp separation). A more common
description of the separation sharpness is (12):
ut ,25
χ= , (7)
ut ,75
where ut,25 and ut,75 are the terminal velocities that belong to the values of the grade
efficiency curve at G(ut,i) = 0.25 and 0.75, respectively. An ideal separation would have a
value of χ = 1 (usual technical sharpness: 0.3 < χ < 0.6, technically sharp: 0.6 < χ < 0.8,
analysis sharp: 0.8 < χ < 0.9 according to 12). Reactions are not considered in the
carbon stripper.
Simulation Environment
The simulations have been carried out in SolidSim (13), a steady-state flowsheet
simulation environment for solids processes.
Test Case
The flowsheet of the test case is

shown in Figure 2. To prevent unburnt
char from entering the air reactor a
carbon stripper (sifter) is located
downstream of the fuel reactor. This
device separates the mixture of OC
and char by differences in settling
velocity. It is desired to facilitate this
separation as much as possible. Coal
particles will naturally decrease in size
during combustion and therefore it is
chosen to grind the coal fine and have
larger oxygen carrier particles in
comparison. This strategy is reflected
by the flowsheet. The stream of fine
particles leaving the carbon stripper is
reintroduced to the fuel reactor while Figure 2: Simulated flowsheet of the CLC
process for solid fuels.
the OC rich stream of coarse particles
is transported to the air reactor. The
feed denoted by OC-refill is necessary to ensure that the target circulation flow of OC
particles can be reached during the iterative solution procedure.
As fuel a Columbian anthracite coal from the El Cerrejon mine has been selected.
Proximate and ultimate analysis results are shown in Table 1 and Table 2.
Table 1: proximate analysis results of coal ‘El Cerrejon’ (14)
LHV [MJ/kg] (waf) Water [wt.-%] (raw) Ash [wt.-%] (wf) Volatiles [wt.-%] (waf)
31.98 15.39 10.3 41.9
Table 2: ultimate analysis results of coal ‘El Cerrejon’ (14)
C [wt.-%] (waf) H [wt.-%] (waf) O [wt.-%] (waf) N [wt.-%] (waf) S [wt.-%] (waf)
81.0 6.01 10.70 1.50 0.79
El Cerrejon coal char has an apparent density of 1500 kg/m³ (14). The total flow of coal
should represent a fuel input of 100 MW th at complete combustion. Dividing the coal
feed into separate flows 1.528 kg/s char, 0.536 kg/s H2O, 0.780 kg/s CH4, 0.567 kg/s
CO, 0.126 kg/s N2 and 0.036 kg/s CO2 are fed to the fuel reactor (sulfur content is
neglected). The fate of the ash is not tracked in this investigation. The initial PSD of the
coal is the same as a state of the art coal mill for pulverized coal boilers delivers (15).
A copper based OC was selected 1
that consists of 10 wt.-% of active char
cumulative mass, -
CuO. The inert phase is Puralox 0.8
NWa155 from Sasol, Germany,
0.6
which is a porous aluminum oxide oxygen carrier
of medium size and a possible 0.4
inert support for impregnation
(16,17). Since the particle size 0.2
distribution of synthetic OC
prepared by impregnation is 0
defined by the support particles, 0 200 400 600 800
the particle size distribution of the dp, µm
Puralox (measured by laser
diffraction) was chosen for the OC Figure 3: Particle size distributions of char (dots)
particles of this investigation. The and oxygen carrier particles (empty squares).
apparent density is taken to be 1
1800 kg/m³ for the oxidized state. char
cumulative mass, -
The particle size distributions of 0.8

char and OC are shown in Figure
0.6
3. It can be observed, that there is
a certain overlap of the two 0.4
distributions. The difference in
particle density is not very large, 0.2
thus the settling velocity oxygen carrier
distributions of the two solids in 0
Figure 4 shows a similar overlap. 0 0.5 1 1.5 2
Figure 4 shows only a small part terminal settling velocity, m/s
of the distribution of OC particles.
At 8 m/s the distribution Figure 4: Settling velocity distributions of char
approaches finally the value 1. The (dots) and oxygen carrier particles (empty squares)
settling velocity distributions are with marked area of overlap at fuel reactor
calculated for fuel reactor conditions.
conditions. According to Figure 4
the cut separation velocity should be chosen between 0.2 m/s and 1.0 m/s.
Fuel reactor operation is carried out at 900°C and the solids entering the fuel reactor
have a residence time of 240 s (18,19). For fluidization and gasification a mixture of
steam and carbon dioxide is fed to the fuel reactor. The CO2 fraction is assumed as
74 % by weight which would correspond to complete gasification of the char. For the re-
oxidation of the OC particles a global excess air ratio of 1.2 is assumed. The circulation
mass flow of OC particles is 650 kg/s.
Simulation results
Simulation results are compared on CO2 capture rate (CCR) basis:

CO2 flow from fuel reactor
CCR = (8)
total CO 2 flow based on fuel input
The CCR is decreased by CO2 leaving the process through the air reactor. This is the
case, when char is transported to the air reactor where it will combust with air oxygen.
In order to minimize the flow of char from the fuel reactor to the air reactor a sifter /
carbon stripper was introduced in-between both reactors (Figure 2). The carbon stripper
divides the mixed solids flow into a flow of fines and coarse. Because of the
aforementioned overlap of the settling velocity distributions the separation of the two
types of solids will never return two pure streams of only one species. It is possible
though to minimize the flow of char within the stream of coarse particles flowing to the
air reactor. This can be achieved by the choice of a high cut velocity. Figure 5 shows
the result of a variation of the cut velocity in terms of char flow in the coarse flow for a
separation sharpness of α = 0.84
which corresponds to χ = 0.5. The 1.6 3000
flow of char in the coarse flow
char flow in coarse, kg/s
solid flow to sifter, kg/s

from the carbon stripper
decreases with increasing cut 1.2
2000
velocity. Increasing the cut
velocity does though also 0.8
increase the flow of OC particles
in the flow of fines that is returned 1000
to the fuel reactor. If this flow 0.4
increases, the carbon stripper will
have to handle a larger flow of 0.0 0
mixed solids. This can generally 0 1 2 3
only be achieved by a larger unit. cut velocity ut,50, m/s
In Figure 5 the flow entering the Figure 5: Char flow towards the air reactor in
carbon stripper unit is shown on dependence of the cut terminal settling velocity and
the secondary axis. For 3 m/s for the corresponding total flow of solids entering the
instance it can be observed that sifter unit (χ = 0.5).
the flow entering the sifter unit 1
reaches approximately 2500 kg/s
CO2 Capture Rate, -
χ =0.8, finer char

which is 3.8 times the flow of OC 0.8
particles circulating between the χ =0.8
reactors. 0.6
χ =0.5
0.4
The aforementioned results are without carbon stripper
shown in Figure 6 in terms of CO2 0.2
capture rate for χ = 0.5 and
χ = 0.8 (corresponding to α = 0.84 0
and α = 3, respectively). The 0 1 2 3
lower boundary indicated by the cut velocity ut,50 ,m/s
dashed line represents the case Figure 6: CO2 capture rate in dependency of the cut
of the CLC process without a terminal settling velocity for χ = 0.5 and χ = 0.8.
sifter. In this case a CCR of 0.36 Additionally the value of CCR is shown for a CLC
is achieved, which corresponds to process without a carbon stripper. The influence of
the reaction of volatiles with the initial char particle size distribution is shown for
oxygen carrier particles and the χ = 0.8 and 1.5 m/s cut velocity.
fraction of char that can be gasified in a single pass through the fuel reactor. Linking the
results shown in Figure 6 with those of Figure 5 it can be observed that corresponding
to the decreased flow of char towards the air reactor at higher cut velocities the CCR
increases at higher cut velocities. For a χ = 0.5 (usual technical sharpness) the CCR is
significantly lower than for χ = 0.8, which represents a technically sharp separation. The
maximum CCR for χ = 0.8 is 0.74. This value is still rather low but higher CCRs are
possible in an optimized process. For instance smaller particle sizes for the coal would
facilitate the separation from the oxygen carrier particles in the sifter. In Figure 6 the
result of a single simulation at χ = 0.8 and 1.5 m/s cut velocity with finer coal
(dp,63 = 50 µm) is additionally shown. This simulation reaches a CCR of 0.83. This value
is still not satisfactory but there is still room for improvements. In general there are two
ways to improve the CCR. First the carbon stripper can be improved and second the
char conversion in the fuel reactor can be increased. This can be achieved in various
ways and the first one was already mentioned above, a further simplification of the
separation of char and OC. Other options are:
• Increased residence time of the solids in the fuel reactor
• Higher temperatures in the fuel reactor
• Elevated steam content in the gasification gas
• Usage of special oxygen carriers that release gaseous oxygen in the fuel reactor
Finally, there is a certain spread in the literature concerning char gasification rates with
H2O and CO2. The chosen gasification kinetics are a rather conservative choice
compared to Ye et al. (6) which differ up to one order of magnitude.
CONCLUSIONS
The influence of the carbon stripper on the CO2 capture rate of a Chemical-Looping
Combustion process for solid fuels was investigated. It can be concluded that the
carbon stripper is an important unit operation in a CLC process for solid fuels. Higher
cut velocities lead to a decreased slip of char towards the air reactor. This increases the
carbon capture rate but on the other hand also increases the load on the carbon
stripper. The simulations show rather low CCRs for the chosen process setup and
operation. Yet, it is possible to achieve higher CCRs either by improvements regarding
the carbon stripper or by increasing the char conversion in the fuel reactor.
ACKNOWLEDGEMENT
The present work is part of a joint research project of the Institute of Combustion and
Power Plant Technology of the University of Stuttgart, the Institute of Energy Systems
of the Hamburg University of Technology and the Institute of Solids Process
Engineering and Particle Technology of the Hamburg University of Technology. This
project received financial support of the German Federal Ministry of Economics and
Technology (FKZ 0327844B / CLOCK) with additional funding from BASF SE, EnBW
Kraftwerke AG, E.ON Energie AG, Hitachi-Power Europe GmbH, RWE Power AG and
Vattenfall Europe Generation AG. The responsibility for the content of this report lies
with the authors.
NOTATION
G Separation grade efficiency,- β Split factor for CO / CO2

production in H2O gasification, -
ks Shrinkage rate, m s-1 χ Separation sharpness, -
R Particle radius, m CCR CO2 capture rate, -
t Time, s CLC Chemical-Looping Combustion
ut,i Terminal settling velocity of OC Oxygen carrier
particles in class i, m s-1
α Separation sharpness PSD Particle size distribution
(Rogers),-
REFERENCES
1. Jerndal E., Mattisson T., Thijs I., Snijkers F., Lyngfelt A. (2010), Int. J. Greenh.
Gas Con. 4, 1, 23–35.
2. Gayán P., Forero C. R., Diego L. F. de, Abad A., García-Labiano F., Adánez J.
(2010), Int. J. Greenh. Gas Con. 4, 1, 13–22.
3. Xiao R., Song Q., Song M., Lu Z., Zhang S., Shen L. (2010), Combust. Flame
157, 6, 1140–1153.
4. Hossain M. M., Lasa H. I. de (2008), Chem. Eng. Sci. 63, 4433–4451.
5. Berguerand N., Lyngfelt A. (2008), Int. J. Greenh. Gas Con. 2, 2, 169–179.
6. Ye D. P., Agnew J. B., Zhang D. K. (1998), Fuel 77, 11, 1209–1219.
7. Matsui I., Kunii D., Furusawa T. (1985), J. Chem. Eng. Jpn. 18, 2, 105–113.
8. Matsui I., Kunii D., Furusawa T. (1987), Ind Eng. Chem. Res. 26, 1, 91–95.
9. Jensen A. (1996), Nitrogen Chemistry in Fluidized Bed Combustion of Coal. Ph.D.
thesis. Technical University of Denmark. Lyngby, Denmark.
10. Levenspiel O. (1989), The chemical reactor omnibook, OSU Book Stores.
Corvallis, Or.
11. Rogers R. S. C. (1982), Powder Technol. 31, 1, 135–137.
12. Rumpf H. (1990), Particle technology, Chapman and Hall. London.
13. SolidSim Engineering GmbH (2010), SolidSim. Version 1.2.
http://www.solidsim.com/.
14. Ratschow L. (2009), Three-Dimensional Simulation of Temperature Distributions
in Large-Scale Circulating Fluidized Bed Combustors. Ph.D. thesis. Hamburg
University of Technology. Hamburg, Germany.
15. Baumeister W., Bischoff W., Pannen H. (2002), VGB PowerTech 82, 9, 54–60.
16. Adánez J., Gayán P., Celaya J., Diego L. F. de, García-Labiano F., Abad A.
(2006), Ind Eng. Chem. Res. 45, 625–645.
17. Diego L. F. de, Gayán P., García-Labiano F., Celaya J., Abad A., Adánez J.
(2005), Energ. Fuel. 19, 1850–1856.
18. Markström P., Berguerand N., Lyngfelt A. (2010), Chem. Eng. Sci. 65, 18, 5055–
5066.
19. Leion H., Mattisson T., Lyngfelt A. (2008), Int. J. Greenh. Gas Con. 2, 2, 180–193.
CATALYST ATTRITION IN THE CFB RISER
Andreas Thon, Marvin Kramp, Ernst-Ulrich Hartge, Stefan Heinrich, Joachim Werther,
Denickestrasse 15
21073 Hamburg, Germany
ABSTRACT
Catalyst attrition in the CFB riser was experimentally investigated in a pilot scale CFB
system consisting of a 400 mm diameter riser with a height of 15 m, a return leg and a
two-stage cyclone separation. The catalyst loss of the CFB system was measured. In
order to discern between attrition occurring in the cyclones and in the riser the system
was simulated by a population balance approach which takes the separation efficiency
of the cyclone system into account. On the basis of the experimental investigation an
empirical correlation for catalyst attrition in the CFB riser has been developed which
accounts for the influence of the gas velocity and the catalyst mass in the riser.
INTRODUCTION
Attrition plays a major role in fluidized bed processes where catalyst particles are used,
e.g. in the Fluid Catalytic Cracking (FCC) process. In this process the fluidization of the
catalyst inside and the transport between the reactors together with the gas solid
separation in the solids recovery system (e.g. cyclones) causes a considerable
mechanical stress on the catalyst material. This stress leads to particle attrition. In the
process a number of attrition sources can be identified. Usually, the gas jets issuing
from the gas distributor into the fluidized bed, the bubble motion in the fluidized bed and
the cyclones are regarded as the most relevant attrition sources (1). Under normal
operating conditions the attrition in a fluidized bed process occurs as surface abrasion,
which means that asperities and edges are removed from the surface of particles (2).
The primary consequence of attrition is the production of fine particles which can not be
kept in the process by the solid recovery system. Thus, attrition leads to a loss of
valuable catalyst material (3). Catalyst attrition is therefore a major issue and efforts
have to be made to produce sufficiently attrition resistant catalyst in order to reduce the
costs for make-up catalyst (4). Furthermore, the prediction of the catalyst loss in a
fluidized bed process is an important issue for process design.
Many works deal with the experimental investigation of the attrition sources in a fludized
bed process e.g. in the cyclone (5), jet-induced attrition (6) and bubble-induced attrition
(7)). At Hamburg University of Technology test procedures were established to
characterize the material’s attrition propensity under mechanical stress conditions in an
isolated cyclone and in a bubbling fluidized bed with and without submerged gas jets.
/
Based on the experimental investigations of each attrition source in isolation, attrition
models have been developed. An overview of various attrition tests is given in (3).
Unlike the before mentioned attrition sources, practically no experimental investigation
regarding the attrition occurring in a circulating fluidized bed (CFB) riser can be found in
the open literature. The difficulty in the experimental investigation of attrition in the CFB
riser is that it can not be continuously operated in isolation. This is, because the catalyst
which is entrained from the riser with the gas, has to be separated from the gas and
returned to the bottom of the riser for continuous operation. Hence, the catalyst loss
and changes in the particle size distribution (PSD) in a CFB system will originate from
the combination of attrition occurring in the riser and attrition occurring in the cyclone
and will be affected by the separation efficiency of the cyclone.
The present work now focuses on the experimental investigation of the attrition
occurring in the CFB riser.
THEORY
In this study the attrition occurring in the CFB riser and in the cyclone are considered.
The jet-induced attrition occurring above the gas distributor is neglected, because a
bubble cap gas distributor with low gas exit velocities is installed in the pilot scale CFB
system. Furthermore, the attrition in the return leg is neglected. The catalyst attrition
occurring in the cyclone is simulated according to the model developed by
Reppenhagen (5). The rate of attrition rc,i in the particle size class dp,c,i occurring in the
cyclone is given by
2
ɺ attr,c,i
m uc,in
rc ,i = = Cc ⋅ dp,c,i
mɺ c,in,i µc (1)
with ṁattr,c,i the mass flow of fines generated by attrition in the particle size class i, ṁc,in,i
the catalyst mass flow entering the cyclone, Cc is the size-independent attrition rate
constant, dp,c,i the particle size, uc,in is the gas velocity at the cyclone inlet and µc is the
solids loading of the incoming gas flow,
mɺc
µc =
ρc ⋅ uc ⋅ Ac (2)
where ρc is the density of the inflowing gas and Ac is the inlet cross-sectional area of the
cyclone.
In contrast to the attrition in the cyclone no specific attrition model for attrition occurring
in the CFB is available in the open literature. However, the attrition due to bubble
motion in fluidized beds was intensively investigated by various authors. For example
Merrick and Highley (7) and Ray et al. (8) found that the bubble-induced attrition rate rb,
which is the mass flow of attrition generated fines in the bubbling fluidized bed ṁattr,b
related to the bed material mass mb is given by
ɺ attr,b
m
rb = = Cb ⋅ (u − umf )
mb (3)
/
with Cb the attrition rate constant for bubble induced attrition, u the superficial gas
velocity in the fluidized bed and umf the minimum fluidization velocity.
The experimental investigations of the bubble induced attrition, cited above, were
carried out at excess gas velocities (u-umf) below 2.16 m/s (7) and 1.1 m/s (8),
respectively. Hence, the application to attrition occurring in a CFB riser, which is
operated at much higher gas velocities, means a significant extrapolation. However, as
a first approach it is assumed here that the same general relationship describes the rate
of attrition occurring in the riser rr,
ɺ attr,r
m
rr = = Cr ⋅ (u − umf )
mr (4)
with ṁattr,r the mass of attrition generated fines in the CFB riser, mr the mass of catalyst
in the riser as indicated by the pressure drop, u the gas velocity in the riser Cr the
attrition rate constant for attrition occurring in the CFB riser.
Attrition rates rc and rr cannot be measured individually in the CFB loop. What is
measured is the overflow of the cyclone which is leaving the system. In order to get
access to rr the population balance for the whole system has to be solved. Therefore,
the flowsheeting software SolidSim (9) is used. In SolidSim the system is simulated by
connecting unit models for the cyclones and the CFB riser. The CFB riser is modelled
by a fluidized bed module developed by Püttmann (10). It accounts for the
hydrodynamic as well as the attrition induced changes in the particle size distribution.
Based on the population balance modelling approach developed by Werther and Hartge
(e.g. 11) the effect of attrition on the PSD in the system is calculated. The attrition
process generates fines, which are added to the smallest size class i = 1. Moreover, the
mother particles shrink due to surface abrasion, which leads to a mass transfer from the
size class i to i-1.
1
cumulative mass Q3, -
EXPERIMENTAL
0.8
Material 0.6
In this study equilibrated cracking catalyst 0.4
(FCC) was used which has been used for 0.2
long time in the industrial process. The
0
particle size distribution, shown in Fig. 1,
has developed from a feed material as result 0 50 100 150 200 250 300
of solids separation and attrition processes. particle diameter, µm
The mean diameter dp50 of the catalyst was Figure 1. Particle size distribution of the
85 µm. catalyst
Attrition test in an isolated cyclone

The material specific attrition constant Cc for attrition occurring in the cyclone was
measured for the FCC catalyst in an isolated cyclone on the lab scale. The diameter of
the cyclone was 90 mm. The tests were conducted under ambient conditions with air for
gas velocities at the cyclone inlet between 10 and 20 m/s and solids loadings at the
/
cyclone inlet between 1 and 2 kg/kg. Detailed information about the test procedure can
be found in (12).
CATALYST LOSS IN THE CFB SYSTEM
The CFB system shown in Fig. 2 was used

for the experimental investigation of catalyst
attrition occurring in the CFB riser. The riser
has a height of 15.6 m and an inner diameter
(ID) of 0.4 m. A bubble cap gas distributor is
installed. The experiments were conducted
under ambient conditions with air as fluidizing
gas in the riser and syphon. The cross-
sectional average gas velocity in the riser was
varied between 3 and 5 m/s and the catalyst
mass in the riser between 30 and 110 kg. The
catalyst entrained from the riser with the gas
is separated by a primary and a secondary
cyclone with diameters of 1 m and 0.8 m,
respectively. According to the cyclone’s
separation efficiency some catalyst leaves the
secondary cyclone with the gas through the
overflow and is then collected in a
subsequent bag filter. The latter catalyst is
not returned to the process and therefore
designated here as catalyst loss. The Figure 2. Pilot scale CFB system
recovered catalyst is recycled via a syphon to
the riser. In the return leg the circulation
rate is measured. Therefore, a section
of the downcomer is separately
supported and decoupled from the
system by compensators. In this section
a butterfly valve is installed. The
circulation rate can be determined by
measuring the weight change of the
section with time after the butterfly valve
is closed.
Figure 3. Measurement system
The CFB system’s catalyst loss is
assessed by measuring a side stream which is withdrawn in a section between the
secondary cyclone’s overflow and the bag filter. The measurement system used is
shown in Fig. 3. The side steam is withdrawn via a suction probe. In the tests two
different probes, one with a diameter of 6 mm and the second with a diameter of
20 mm, were used. The catalyst entrained by the withdrawn gas is subsequently
separated by a filter. The catalyst mass flow is determined by differential measurement
of the filter weight per measurement time. The volume flow through the probe is
controlled manually by valves and a rotameter. It is adjusted such that the gas velocity
/
in the probe is the same as the average gas velocity in the measurement section of the
pipe. The measurement setup allows the measurement at different radial positions to
investigate the solids concentration profile.
Material specific cyclone attrition rate constant

In an isolated cyclone the catalyst loss ṁc,loss, i.e. the catalyst which is entrained with
the gas in the cyclone overflow, is measured for multiple passes of the catalyst through
the cyclone. Under steady-state conditions it is assumed that the measured ṁc,loss is
equal to the mass flow of fines generated by attrition inside the cyclone and the attrition
rate rc is given by
ɺ c,loss
m u2
rc = = Cc ⋅ c,in ⋅ dp,c,mean
mɺ c,in µc (5)
with the mean particle size dp,c,mean defined as
n
dp,c,mean = ∑ dp,c,i ⋅ q3,i ∆dp,c,i
i =1
(6)
q3 denotes the mass density distribution of the particles entering the cyclone. The mean
particle size is calculated with the PSD measured for the FCC catalyst.
In Fig. 4 the attrition rate rc against the passes through the cyclone is shown for two
tests at different operating conditions. The results illustrate that the attrition rates
measured for the first passes through the cyclone are higher than for the following. This
can be explained by fines which are present in the feed material and are sifted off in the
first passes through the cyclone. Thereafter the attrition rate decreases to a stationary
value, the so called steady state attrition rate indicated by the dashed lines in Fig. 4.
The steady state attrition rate measured for each operating condition plotted against the
product of dp,c,mean·uc,in²·µc-0.5 is shown in Fig. 5. According to the attrition model equ. (1)
the slope of the straight line represents the material specific steady state attrition rate
constant Cc, which is 8.8·10-4 s²/m³ in this case.
steady state attrition rate
6 u=10 m/s µ=1 kg/kg 4.0

attrition rate rc,10 kg/kg
5 u=20 m/s µ=1 kg/kg 3.5

3.0
rc , 10 kg/kg
-5
4 2.5
3 2.0
-5
1.5
2
1.0
1 0.5
0 0.0
0 5 10 15 20 0 0.01 0.02 0.03 0.04
0.5
number of passes trough the cyclone dp,c,mean·uc,in²/µc , m³/s²
Figure 4. Attrition rates rc measured over Figure 5. Steady state attrition rates versus
15 passes through the cyclone for two the operating conditions according to the
different operating conditions attrition model in equ. (1)
/
Attrition test in the CFB system
The CFB system was operated over 200 h under different operating conditions. For
each measurement condition the plant was filled with a predetermined mass of solids
(8-200 kg). Then the plant was run for two hours in order to elutriate the fines of the
initial inventory. After this time the cyclone loss contains only solids generated by
attrition, i.e. the fines attrited from the solids and the particles which have shrunk by
attrition. This is a quasi-steady state. A real steady state would require addition of fresh
bed material compensating the loss. Since the measurements show that the catalyst
loss during one hour is less than 0.05 % of the bed material this latter effect was
neglected.
The catalyst mass flow in the side stream of the cyclone is measured using the
measurement setup shown in Fig. 3. Under each operating condition the measurement
was repeated more than four times. In order to isolate the attrition effect in the riser it
must be considered that the measured catalyst loss results from several mechanisms,
i.e. attrition occurring in the cyclones, attrition in the riser, particle shrinkage and the
separation in the cyclones. The difficulty is that the latter mechanisms are influenced by
the catalyst’s particle size distribution and concurrently affect the catalyst’s PSD
themselves. Hence, the CFB system has to be simulated in consideration of the
catalyst’s PSD.
70 u = 3 m/s
cross sectional average
In Fig. 6 the cross sectional average 60 u = 4 m/s

mass flow Gs , kg/m²s
u = 5 m/s
catalyst mass flow in the riser Gs measured 50
for the three different gas velocities versus 40
the catalyst mass in the riser is shown. 30
Obviously, the circulation rate increases 20
with increasing gas velocity and catalyst
10
mass in the riser. The Gs values measured
0
under different operating conditions vary
from 15 and 60 kg/m²s. 0 20 40 60 80 100 120
catalyst mass
Figure 6. Influence in thecatalyst
of the riser, kg mass
Simulation
and gas velocity u on the cross sectional
The simulation flowsheet representing the average solid mass flow in the riser Gs
pilot scale CFB system is shown in Fig. 7.
The process is simulated based on the catalyst properties (i.e. PSD and attrition
characteristics), the operating conditions and the geometry of the CFB system.
Unlike the attrition constant Cc the constant for attrition occurring in the riser Cr (c.f.
equ. (4)) is unknown. Hence, this parameter is fitted to all measurements using the
simulation. The material specific attrition constant Cr is found to be 3.2·10-8 1/m.
Compared to the attrition rate constants for FCC catalysts measured previously in a
stationary fluidized bed Cb = 0.45·10-8 1/m and Cb = 1.37·10-8 1/m (12) the attrition rate
constant Cr is higher.
The exemplary result for the simulation conducted with a catalyst mass in the riser of
89 kg and a superficial gas velocity in the riser of 4 m/s are also shown in Fig. 7. The
/
results display that attrition in the riser is ṁattr,c2 = 0.23 g/h
responsible for a major part of the catalyst loss. ṁattr,c1 = 14.7 g/h 61.6 g/h
The rate of attrition occurring in the riser rr,
operated at a superficial gas velocity of 4 m/s is
1.1 % of the catalyst inventory in the riser per day.
The influence of the catalyst mass in the riser on

the catalyst loss rate was experimentally
investigated. Additionally, simulation runs with
varying catalyst mass in the riser are conducted. A ṁattr,r = 45 g/h
comparison between the measured and simulated
catalyst loss rate is shown Fig. 8. The catalyst loss
rate increases with increasing catalyst mass in the
riser. The influence of the gas velocity in the riser
on the catalyst loss rate is shown in Fig. 9. The gas
velocity has a significant influence on the catalyst 61.6 g/h
loss rate in the CFB system, with increasing gas
velocity in the riser the catalyst loss increases. The Figure 7. SolidSim flowsheet
results indicate that with the approach for attrition in representing the CFB system with
the CFB riser, equ. (4), a satisfactory description of simulation results for mr = 89 kg
all measured values is possible. and u = 4 m/s
CONCLUSION
The catalyst loss of a pilot scale CFB system was measured. The influence of the
catalyst inventory in the riser and the gas velocity in the riser was investigated. Based
on a population balance approach the attrition in the CFB system was simulated. The
simulation considered the attrition occurring in the cyclone and in the CFB riser in the
mode of pure abrasion. As a first approximation the mass produced by attrition in the
riser was assumed to be linear proportional to the excess gas velocity (u-umf) and the
solids mass mr in the riser, respectively. The attrition constant for attrition occurring in
the CFB riser was then fitted to the measured values using the simulation. The
45 6 mm probe 100
40 20 mm probe measurement
catalyst loss rate, g/h
simulation 80 simulation
35
catalyst loss rate, g/h
30
60
25
20 40
15
10 20
5
0 0
0 20 40 60 80 100 120 0 1 2 3 4 5 6
catalyst mass in the riser, kg gas velocity in the riser, m/s
Figure 8. Influence of the catalyst mass in Figure 9. Influence of the gas velocity in
the riser on the catalyst loss rate for u = the riser on the catalyst loss rate for mr =
3 m/s 50 kg
/
comparison of the simulation results and the measured catalyst loss rates for varying
solids mass in the riser and gas velocities indicates that the simulation predicts the
tendencies without significant deviations. Additionally, the simulation allows the
investigation of the individual attrition sources.
NOTATION
Ac cross-sectional cyclone inlet area, m² q3 mass density distribution, 1/m

Cb bubble induced attrition constant, 1/m r attrition rate, rc, - ; rb and rr, 1/s
Cc constant for attrition occurring in the uc,in gas velocity in the cyclone inlet,
cyclone, s²/m³ m/s
Cr constant for attrition occurring in the umf minimum fluidization velocity, m/s
CFB riser, 1/m
dp particle diameter, m µc solids loading of the gas, kg/kg
Gs average cross sectional solids mass ρc gas density at the cyclone inlet,
flow in the riser, kg/m²s kg/m³
ṁ mass flow, kg/s CFB circulating fluidized bed
m mass, kg PSD carticle size distribution
REFERENCES
1. Pell M. (1990), Gas fluidization, Elsevier. Amsterdam.

2. Werther J. (2008), Fluidized-Bed Reactors. In: Handbook of Heterogenous
Catalysis, Ertl G.; Knözinger H.; Schüth F.; Weitkamp J. (eds.), Wiley-VCH Verlag
Weinheim.
3. Werther J., Reppenhagen J. (2003), Attrition. In: Handbook of Fluidization and
Fluid-Particle Systems, Yang W. C. (ed.), Marcel Dekker, New York.
4. Contractor R. M., Bergna H. E., Chowdhry U., Sleight A. W. (1989), Attrition
resistant catalysts for fluidized bed systems. In: Fluidization VI, Grace J. R.;
Shemilt L. W.; Bergougnou M. A. (eds.), New York: Engineering Foundation .
5. Reppenhagen J., Werther J. (2000), Powder Technol. 113, 55–69.
6. Werther J., Xi W. (1993), Powder Technol. 76, 39–46.
7. Merrick D., Highley J. (1974), AIChE Symp. Ser. 70, 137, 367–378.
8. Ray Y. C., Jiang T. S., Wen C. Y. (1987), Powder Technol. 49, 193–206.
9. SolidSim Engineering GmbH (2010), SolidSim. Version 1.2.
http://www.solidsim.com/.
10. Püttmann A., Hartge E. -U, Werther J. (2008), Modeling of Fluidized Bed Riser-
Regenerator Systems. In: Circulating Fluidized Bed Technology IX, Werther J.;
Nowak W.; Wirth K-E; Hartge E. -U (eds.), TuTech Innovation GmbH, Hamburg.
11. Werther J., Hartge E. -U (2004), Powder Technol. 148, 113–122.
12. Thon A., Werther J. (2010), Appl. Catal. A-Gen 376, 1-2, 56–65.
/
EFFECTS OF GAS VELOCITY AND SOLID HOLD-UP
ON THE SUB-GRID BEHAVIOR OF RISER FLOWS
Christian Costa Milioli 1 and Fernando Eduardo Milioli 2
University of São Paulo, School of Engineering of São Carlos, Dept. of Mech. Engng.,
Av. Trabalhador São-carlense, 400, 13566-590, São Carlos, SP, Brazil.
1
ccosta@sc.usp.br; 2 milioli@sc.usp.br
ABSTRACT
Two-fluid highly resolved sub-grid simulations (SGS) of riser flows were developed
under realistic gas velocities and solid hold-ups, for a solid phase derived from high
Stokes number particles. The results showed that both gas velocity and solid hold-up
considerably affect the effective hydrodynamics of the solid phase.
INTRODUCTION
Large scale simulations (LSS) with two-fluid models are expected, in time, to provide
accurate predictions of real scale riser flows. One related aspect requiring attention is
the proposition of sub-grid closures for solid phases. Along this last decade some
researchers have been trying to draw those closures from sub-grid scale simulations
(SGS) with two-fluid models. Among the relevant works on that matter are those of
Sundaresan (1), Agrawal et al. (2), Andrews IV et al. (3), van der Hoef et al. (4) and
Igci et al. (5). Those works take advantage of the fact that, regarding solid phases,
highly resolved simulations are feasible in computational domains that are large
enough to fit LSS numerical cells. Under suitable grid refinements a single SGS step
can directly provide closures for LSS of real riser flows. The micro-scale description
of the solid phase that is required in SGS is brought from the kinetic theory of
granular flows (KTGF) (6,7,8,9). The common SGS computational experiment is
performed in small periodic domains which are thought to repeat themselves
throughout the whole volume of a riser. As periodic boundaries are applied an
additional gas phase pressure gradient is introduced in the gravitational direction to
account for the flow driving force. Such additional term is chosen to exactly match the
gravity acting on the average gas-solid mixture, so that the simulations give rise to
low velocity gas-solid flows. In spite of that, the clustering mechanism that prevails is
believed to be relevant to rapid gas-solid flows (10,11).
In a recent work by Benyahia (12), a filtered drag model derived from the sub-grid
data of Igci et al. (5) was applied to the LSS of a riser flow. The author’s comparison
of predictions against experiment showed considerable discrepancies, indicating that
SGS under periodic boundaries requires enhancement. The present article is an
attempt to contribute to the discussion on that matter by performing SGS under riser
realistic conditions of gas velocity and solid hold-up. It is proposed, differently from all
the previous work, to apply an additional gas phase pressure gradient in excess of
that required to match the gravity acting on the local gas-solid mixture. In this case
1
the flow becomes accelerated and instantaneous field predictions are found through
a range of gas velocities. While those predictions at any particular mesh point should
not be regarded as significant in view of the instability of the flow, the domain
average results, on the other hand, are thought to be quite representative.
Simulations were developed for a range of domain average solid volume fractions,
and results were analyzed in a range of gas phase axial velocities typical of riser
flows. The effect of those parameters were evaluated over the flow topology, the
average slip velocity, the effective stresses of the solid phase, and the effective drag.
A solid phase was considered which is derived from a high Stokes number particulate
typical of circulating fluidized bed combustors and gasifiers.
MATHEMATICAL MODELLING
Multiphase flow two-fluid models stand on the major hypothesis of continuum for all
of the phases, no matter fluid or particulate. The phases are treated as
inter-penetrating dispersed continua in thermodynamic equilibrium. The theory of
two-fluid models has been developed by many researchers. Some classical
references on this matter are due to Gidaspow (9), Anderson and Jackson (13), Ishii
(14), Drew (15), Enwald et al. (16), among many others. The hydrodynamic two-fluid
models comprise a basic set of average mass and momentum conservative
equations plus closure laws for stress tensors, viscosities, pressures and drag.
The present two-fluid model is formulated to perform SGS, which remains LSS alike
regarding the gas phase, but is required to become highly resolved regarding the
solid phase so that all the scales of clusters are captured. In this way, the gas phase
would require closures at both the micro and the meso-scales. Literature shows that
under high Stokes numbers, which is the present case, the turbulence of the fluid
phase has little effect over the solid (2,17). As the concern in the present analysis is
the behavior of the solid phase, no turbulence model is applied for the gas phase.
The micro-scale closure for the solid phase is established by applying the kinetic
theory of granular flows (KTGF), where solid phase micro-scale properties are
derived as a function of a granular temperature determined from a pseudo thermal
energy balance. In this work, for the sake of simplicity, the algebraic approach of
Syamlal et al. (18) is applied, where the pseudo thermal energy is assumed to be
locally generated by viscous stress and dissipated by inelastic collisions. Table 1
presents the sub-grid scale hydrodynamic formulation that was applied, where the
gas phase continuity and momentum equations come from Favre averaging over the
respective filtered equations. Periodic conditions are applied at entrance and exit, i.e.
in the horizontal boundaries normal to the vertical gravitational direction. An additional
gas phase pressure gradient is enforced in that direction to account for the flow
driving force. Free slip is applied in all of the vertical boundaries. Agrawal et al. (2)
showed that the application of either free slip, partial slip, or periodic conditions to
vertical boundaries gives rise to the same flow topology. In the present work the
simpler free slip condition was applied. Solid phase’s effective stresses and effective
drag are determined from the SGS predictions by applying the relations in Table 2. The
effective stress tensor is derived by Favre averaging over the filtered solid phase
momentum equation. As a filter size is applied that exactly fits the sub-grid domain, the
filtered parameters become equal to their volume averages. Following literature (4,5)
the filtered drag force was expressed as a function of an effective drag coefficient and
the filtered slip velocity, thereby providing a relation for the effective drag coefficient.
2
Table 1. Sub-grid scale hydrodynamic formulation of the two-fluid model.
—————————————————————————————————————
∂
∂t
( ) (
ρ g α g + ∇ ⋅ ρ g α g u~ g = 0 )
∂
( ρs α s ) + ∇ ⋅ ( ρs α su s ) = 0
∂t
∂
∂t
( ) ( ~
) ( ~
ρ g α g u~ g + ∇ ⋅ ρ g α g u~ g u~ g = − α g ∇ Pg + ψ∇ Pg* + ∇ ⋅ α g τ~g − τ ge + ρ g α g g + M gI ) [ ( )]
∂
∂t
(
( ρs α su s ) + ∇ ⋅ ( ρs α su su s ) = − α s ∇P~g + ψ∇Pg* + ∇Ps + ∇ ⋅ (τ s ) + α s ρs g + M sI )
α g + αs = 1
∇Pg* = (ρs α s + ρ g α g ) g
τ~g = µ g [∇u~ + (∇u~ ) ] − µ (∇ ⋅u~ )I

g g
T 2
3 g g
= µ [∇u + (∇u ) ] + (λ − µ ) (∇ ⋅ u ) I
T 2
τs s s s s 3 s s
1 1
4 Θ 4 Θ 2
λs = αs2 ρs d p g 0 (1 + e ) 
2
µs = α s2 ρs d p g 0 (1 + e )  (Gidaspow, 9)
5 π 3 π
s ,max − 2.5 α
   
α
g 0 = 1 −  s  
(Lun and Savage, 19)
  α s ,max  
 
Ps = ρ s α s Θ[1 + 2(1 + e )g 0 α s ] (Gidaspow, 9)
1 − K1 α s tr (Ds ) + K12tr 2 (Ds ) α s2 + 4 K 4 α s K 2 tr 2 (Ds ) + 2 K 3 tr Ds2 [ ( )]

(Syamlal et al., 18)
Θ 2 =
2α s K 4
Ds =
1
2
[∇u s + (∇u s )T ] K1 = 2(1 + e )ρs g 0 K2 =
4d p ρs (1 + e ) α s g 0
3 π
−
2
3
K3
d p ρs 
K3 = 
π
[1 + 0.4(1 + e )(3e − 1) αs g 0 ] + 8αs g 0 (1 + e) 

K4 =
12 1 − e 2 ρs g 0 ( )
2  3(3 − e ) 5 π  dp π
~
M sI = − M gI = − β u s − u~ g ( )
α s2 µ g ρ g α s u~ g − u s
β = 150 + 1.75 for αs > 0.2 (Ergun, 20; Gidaspow, 9)
αg d pφp (
2
)d pφ p ( )
~
3
β = C Ds
ρg αsα g u g − u s
αg
− 2.65
( )
for α s ≤ 0.2 (Wen and Yu, 21; Gidaspow, 9)
4
d pφ p ( )
 24  0 ,687 
 R e  1 + 0.15 R e p  for

R e p < 1000
u~ g − u s d p ρ g α g
 p
C Ds = Rep = (Rowe, 22)
 µg
0.44 for R e p ≥ 1000
—————————————————————————————————————
3
SIMULATIONS
The simulations were performed for a solid phase derived form a high Stokes number
monodisperse particulate typical of low density risers (520 µm diameter, 2620 kg/m3
density), and for solid phase average volume fractions of 0.015, 0.03, 0.05, 0.07 and
0.09. Accelerating flows were generated and the results were analysed for increasing
gas velocities from about 3 to about 9 m/s. A 2x2 cm wide and 8 cm tall vertical
hexahedral domain was considered, applying a 1x1x1 mm uniform hexahedral
numerical mesh. The flow entered the domain through the bottom and exited at the top.
The density and viscosity of the gas phase were, respectively, 1.1614 kg/m3 and 1.82 x
10-5 N.s/m2. A solid phase volume fraction at maximum packing of 0.38 was applied
following Gidaspow and Ettehadieh (23), and a restitution coefficient of 0.9 was taken
following Agrawal et al. (2).
Table 2. Solid phase’s effective stresses and effective drag.

—————————————————————————————————————
 α su s ⋅ α su s 
τ se = ρ s α s ( u~
 α s u su s αu αu  
s u s − u su s ) = ρ s α s 
~ ~  − s s⋅ s s  = ρs  α su su s −
 
 αs αs αs   αs 
 
( ~
β us − u g )
M sI = − β (u s − u~ g ) = − β (u s − u~ g ) M sI = − βe u s − u~ g βe =
u s − u~ g
—————————————————————————————————————
The driving force factor ( ψ ) was set to 1.5. This value allowed the simulations to go
along a suitable range of gas axial velocities in a reasonable computing time. Initial
conditions for the accelerating runs were obtained by running previous simulations
applying ψ = 1 , departing from uniform quiescent suspensions with fixed uniform solid
volume fractions. A time step of 5x10-5 s was applied which is suitable for solid phase
highly resolved simulations. The lower characteristic time scale of clusters of the order
of 10-2 s (24). Also, for the present 520 µm particulate size the smaller clusters on the
flow are expected not to be larger than 5.2 mm (following 2). Therefore, regarding the
solid phase, both the spatial and temporal meshes which were applied are suitable for
highly resolved simulations. The convergence criterion for the numerical procedure
was a rms of 1x10-5. The simulations were carried out using the software Cfx (25).
RESULTS
The effects of the domain average solid volume fraction and gas phase axial velocity
over the flow effective hydrodynamics were evaluated. The greyscale plots of solid
phase fraction in Figure 1 show that the topology of the flow considerably changes by
changing the concerning parameters. By increasing the average solid fraction, for a
particular gas velocity, larger clusters are formed. By increasing the gas velocity, for a
particular average solid fraction, the clusters become stretched in the axial direction.
Figure 2 shows plots of the effective stresses of the solid phase. Even though the
results are very scattered, it is possible to observe that higher solid fractions give rise
to higher stresses. The effective shear stresses seem not to change with gas velocity,
while the normal stresses show considerable variations (e.g. drawn line in Fig. 2 (b)).
4
0.015 0.05 0.09 0.015 0.05 0.09 0.015 0.05 0.09
∼ 3 m/s ∼ 6 m/s ∼ 9 m/s
0 > 0.25
Figure 1. Solid volume fraction in an axial section of the domain for αs = 0.015,
0.05, 0.09, and v g ≅ 3, 6, 9 m/s.
(a) (b)
|τxy,se|, |τxz,se|, |τyz,se| (N/m )
|τxx,se|, |τyy,se|, |τzz,se| (N/m )

2
10
1
1E-3 0.1
1E-6 1E-3
3 4 5 6 7 8 9 3 4 5 6 7 8 9
< vg > m/s < vg > (m/s)
Figure 2. Effective shear (a) and normal (b) stresses of the solid phase as a function of
v g , for αs = 0.015 (S); 0.03 (z); 0.05 (Â); 0.07 (U) and 0.09 ({).
Figure 3 shows the behavior of the slip velocity and the effective drag coefficient. As
seen, the higher the solid fraction, the lower the slip velocity, and the higher the
effective drag coefficient. Both the parameters resulted little affected by the gas
velocity, except for the slip velocity at higher solid fractions, where an oscillating
behavior is also observed. This is possibly due to the formation of larger clusters in
comparison to the size of the domain (see Fig. 1). Those oscillations are expected to
disappear at sufficiently enlarged domains, that would always hold a considerable
number of clusters throughout the whole range of gas velocities in an accelerating run.
This issue, of course, requires verification.
Figure 4 brings some of the predictions compared to empirical data of Luo (26). This
author performed experiments in a riser column with the same conditions applied in
the current simulations. From the measurements, Luo determined effective shear
stresses and effective drag coefficients for various average solid fractions. A few of
those solid fractions, for a gas velocity close to 5 m/s, fall in the ranges considered in
5
the present simulations. As seen in Figure 4, Luo’s results for those cases compare
reasonably well with the present predictions, which is fine considering that Luo’s
results apply to regions close to the column wall, while the predictions are volume
averaged over a free slip walls domain.
(a) (b)
1000
5.0
< vg - vs > (m/s)
750
βe (kg/m s)
4.5
3
4.0 500
3.5 250
3.0
0
5 6 7 8 9 5 6 7 8 9
< vg > (m/s) < vg > (m/s)
Figure 3. Slip velocity (a) and effective drag coefficient (b) as a function of v g , for
αs = 0.015 (S); 0.03 (z); 0.05 (Â); 0.07 (U) and 0.09 ({).
(a) (b)
900
|τxy,se|, |τxz,se|, |τyz,se| (N/m )
2
1
600
βe (kg/m s)
3
0.01
300
1E-4 0
0.00 0.02 0.04 0.06 0.08 0.10 0.00 0.02 0.04 0.06 0.08 0.10
< αs > < as >
Figure 4. Effective shear stresses of the solid phase (a) and the effective drag
coefficient (b) as a function of αs , for v g ≅ 5 m/s; (X) empirical, Luo (26).
CONCLUSION
Two-fluid SGS was developed to investigate the sub-grid behavior of riser flows for a
solid phase derived from a high Stokes number monodisperse particulate.
Accelerated flow simulations were performed for a range of average solid fractions
and gas velocities typical of risers. The effects of those parameters over the flow
topology, the effective hydrodynamics of the solid phase and the effective drag were
analyzed. The effects of both the gas velocity and the solid hold-up were found to be
significant. A comparison was made of predictions against a few empirical data, and
a reasonable agreement was found.
6
ACKNOWLEDGEMENTS
This work was supported by The State of São Paulo Research Foundation (FAPESP),
The National Council for Scientific and Technological Development (CNPq), and The
Coordination for the Improvement of Higher Level Personnel (CAPES).
NOTATION
CD drag coefficient (nd) P pressure (Nm-2)

dp particle diameter (m) ∇P* additional pressure gradient (Nm-3)
D strain rate tensor (s-1) Re p particle Reynolds number (nd)
e restitution coefficient (nd) t time (s)
g gravity acceleration (ms-2) u velocity vector (ms-1)
g0 radial distribution function (nd) u , v, w Cartesian velocities (ms-1)
I unit tensor (nd) V SGS domain volume (m3)
M interface drag force (Nm-3) x , y, z Cartesian coordinates (m)
Greek letters
α volume fraction (nd) ρ density (kgm-3)
β friction coefficient (kgm-3s-1) τ viscous stress tensor (Nm-2)
Θ granular temperature (m2s-2) τe effective stress tensor (Nm-2)
λ bulk viscosity (Nsm-2) φp particle sphericity (nd)
µ dynamic viscosity (Nsm-2) ψ driving force factor (nd)
Subscripts
e meso-scale or effective max maximum
g gas phase s solid phase
I interface x , y, z Cartesian directions
Others
LSS filtered (resolved)
~ ~ αf
Favre average, f =
α
∫ f dV
1
... volume average, f =
V V
REFERENCES
1. Sundaresan, S. Modeling the hydrodynamics of multiphase flow reactors: current

status and challenges. AIChE J. Vol. 46-6, pp. 1102-1105 (2000).
2. Agrawal, K., Loezos, P. N., Syamlal, M. and Sundaresan, S. The role of
meso-scale structures in rapid gas-solid flows. J. Fluid Mech. Vol. 445, pp.
151-185 (2001).
3. Andrews IV, A. T., Loezos, P. N. and Sundaresan, S. Coarse-grid simulation of
gas-particle flows in vertical risers. Ind. Eng. Chem. Res. Vol. 44-16, pp.
6022-6037 (2005).
4. van der Hoef, M. A., Ye, M., van Sint Annaland, M., Andrews IV, A. T.,
Sundaresan, S. and Kuipers, J. A. M., Multiscale modeling of gas-fluidized beds,
Adv. Chem. Eng. Vol. 31, pp. 65-149 (2006).
5. Igci, Y., Andrews IV, A. T., Sundaresan, S., Pannala, S. and O’Brien, T. Filtered
two-fluid models for fluidized gas-particle suspensions. AIChE J. Vol. 54-6, pp.
7
1431-1448 (2008).
6. Bagnold, R. A. Experiments on a gravity-free dispersion of large solid spheres in
a Newtonian fluid under shear. Proc. R. Soc. Vol. A225, pp. 49-63 (1954).
7. Jenkins, J. T. and Savage, S. B. A Theory for the rapid flow of identical, smooth,
nearly elastic spherical particles. J. Fluid Mech. Vol. 130, pp. 187-202 (1983).
8. Lun, C. K. K., Savage, S. B., Jeffrey, D. J. and Chepurniy, N. Kinetic theories for
granular flows: inelastic particles in Couette flow and singly inelastic particles in a
general flow field. J. Fluid Mech. Vol. 140, pp. 223-256 (1984).
9. Gidaspow, D. Multiphase flow and fluidization. San Diego. Academic Press
(1994).
10. Goldhirsch, I., Tan, M. -L. and Zanetti, G. A molecular dynamical study of granular
fluids I: the unforced granular gas in two dimensions. J. Sci. Comput. Vol. 8-1, pp.
1-40 (1993).
11. Tan, M. -L. and Goldhirsch, I. Intercluster interactions in rapid granular shear
flows. Phys. Fluids Vol. 9-4, pp. 856-869 (1997).
12. Benyahia, S., On the effect of subgrid drag closures, Ind. Eng. Chem. Res., Vol.
49, pp. 5122-5131 (2010).
13. Anderson, T. B. and Jackson, R. Fluid mechanical description of fluidized beds.
Equations of motion. Ind. Eng. Chem. Fund. Vol. 6, pp. 527-539 (1967).
14. Ishii, M. Thermo-fluid dynamic theory of two-phase flow. Paris. Eyrolles (1975).
15. Drew, D. A. Averaged field equations for two-phase media. Stud. Appl. Math. Vol.
1-2, pp.133-136 (1971).
16. Enwald, H., Peirano, E. and Almstedt, A. -E. Eulerian two-phase flow theory
applied to fluidization. Int. J. Multiphase Flow. Vol. 22, pp. 21-66 (1996).
17. Fede, P. and Simonin, O. Numerical study of the subgrid fluid turbulence effects
on the statistics of heavy colliding particles. Phys. Fluids Vol. 48, pp. 045103
(2006).
18. Syamlal, M, Rogers, W. and O´Brien, T. MFIX documentation theory guide. West
Virginia. U.S. Department of Energy (1993).
19. Lun, C. K. K. and Savage, S. B. The effects of the impact velocity dependent
coefficient of restitution on stresses developed by sheared granular materials.
Acta Mech. Vol. 63, pp. 15-44 (1986).
20. Ergun, S. Fluid flow through packed columns. Chem. Eng. Prog. Vol. 48-2, pp.
89-94 (1952).
21. Wen, C. Y. and Yu, Y. U. Mechanics of fluidization. Chem. Eng. Prog. S. Ser. Vol.
62, pp. 100-111 (1966).
22. Rowe, P. N. Drag forces in a hydraulic model of a fluidized bed. Part II. Trans. Inst.
Chem Eng. Vol. 39, pp. 175-180 (1961).
23. Gidaspow, D. and Ettehadieh, B. Fluidization in two-dimensional beds with a jet.
Part II. Hydrodynamic modeling. Ind. Eng. Chem. Fund. Vol. 22, pp. 193-201
(1983).
24. Sharma, A. K., Tuzla, K., Matsen, J. and Chen, J. C. Parametric effects of particle
size and gas velocity on cluster characteristics in fast fluidized beds. Powder
Technol. Vol. 111, pp. 114-122 (2000).
25. Cfx, Discretization and solution theory. In Solver theory manual. Release 10.
Waterloo. Ansys Canada (2005).
26. Luo, K. M., Experimental gas-solid vertical transport, PhD Thesis, Illinois Institute
of Technology, Chicago, Illinois, (1987).
8
A GENERALIZED FLOW REGIME DIAGRAM FOR FLUID-
SOLID VERTICAL TRANSPORT
Xiaotao T. Bi
Fluidization Research Centre
Department of Chemical and Biological Engineering
The University of British Columbia, Vancouver, Canada
ABSTRACT
An ideal generalized flow regime diagram was proposed for fluid-solids vertical
transport systems with no bottom and top restrictions. Such an ideal flow regime
diagram was further extended to shed light onto the understanding of the flow
regimes and instabilities encountered in bottom- restricted bubbling and circulating
fluidized bed systems.
INTRODUCTION
Flow patterns and flow regimes in gas-solids two-phase fluidization and vertical flow
systems have attracted a great attention in the multiphase research community since
the 1940s. A number of flow regime maps have been proposed to distinguish
different unique flow patterns. Although it has been commonly agreed that there
exist distinct flow patterns in gas-solids fluidized beds and vertical transport lines,
such as the bubbling and slugging fluidization and dilute phase transport based on
extensive research from 1940s to 1960s. Controversies still exist on the existence of
turbulent fluidization, which was first proposed in late 1960s, fast fluidization, which
was first proposed in late 1970s. The transition from pneumatic conveying to fast
fluidization or dense suspension upflow is still not well defined, as reflected in the
debates on the definition of choking in Fludization X in Beijing and CFB-7 in Naragra
Falls. Further work on this topic is warranted in order to develop a generalized flow
regime diagram for the flow pattern identification. In this work, attempt was made to
elucidate the flow patterns in free or non-restricted gas-solids vertical flow systems in
hope that such an analysis will shed some light on the understanding of the bottom-
restricted fluidized bed systems and the dense suspension upflow system in which
the solids feeding system is coupled with the flow in the riser.
FLOW PATTERNS IN FREE GAS-SOLIDS VERTICAL FLOW SYSTEMS
In gas-solids vertical flow systems with gas flowing upward, particles can travel up or
down, giving rise to two possible flow modes: co-current upflow and counter-current
flow. The termination of counter-current flow occurs when solids can no longer fall
downward (i.e. at the flooding point) and the gas-solids co-current upflow ceases
when the gas velocity is lower than particle terminal settling velocity.
If we feed solids from the middle section into a vertical tube with open top and
bottom in which gas is flowing from bottom to top, both co-current upward flow in the
upper section above the feeding point and counter-current flow in the lower section
below the feeding point are possible depending on the gas velocity and the solids
feeding rate. At a gas velocity lower than the particle terminal velocity, all feed
particles will fall downward at a low feed rate, forming a counter-current flow in the
lower section of the tube and a single-phase gas flow in the upper section, as shown
in Figure 1. However, with the increase in solids feed rate, flooding will be reached
when particles discharge rate from the bottom end of the tube becomes smaller than
the solids feed rate. As a result, solids start to build up upward into the upper
section, forming a dense fluidized bed in the upper section. This flooding
phenomenon is in analogy to the flooding in gas-liquid counter-flow systems.
1400
II V
1200
Solids feed rate, kg/m2s
1000
Saturation
800
IV
600
400
Flooding
I
200
Ut Use
III
0
0 2 4 6 8 10 12
Superficial gas velocity, m/s
Figure 1. A flow regime diagram for non-restricted vertical transport lines. FCC
particles in ambient air: mean particle size, 60 μm; particle density, 1800 kg/m3.
Let us now consider the case when the gas velocity in the tube is higher than the
particle terminal settling velocity. At a low solids feed rate all fed particles are carried
upward giving a co-current upward flow in the upper section, and a single-phase gas
flow in the lower section, shown in Figure 1. When the solids feed rate is increased
to such an extent that the solids feed rate exceeds the saturation particle carrying
capacity of the gas, excess amount of particles will fall downward and leave the tube
from the bottom, forming a counter-current flow in the lower section as well as a co-
current upward flow in the upper section. If the solids feed rate is further increased to
such an extent that the downflowing particle rate exceeds the flooding rate which
corresponds to the maximum discharge rate from the bottom end of the column, a
dense suspension starts to build up above the solids feed point, forming a co-current
dense suspension upflow in the upper section and a flooded counter-current flow in
the lower section.
A flow regime diagram for a given vertical tube, gas and particle properties can be
constructed based on the flooding velocity and the gas velocity corresponding to the
saturation carrying capacity, estimated from two correlations:
Equation (1) from Papa and Zenz [1], which was modified from the Sherwood
equation originally developed to predict flooding in packed towers, is selected to
predict flooding point:
2/3
⎡ U g ⎛ ρ g ⎞1 / 2 ⎤
2/3
1 ⎛G /ρ ⎞
1/ 3
⎛ 1 ⎞
⎢ ⎜⎜ ⎟⎟ ⎥ + 1/ 3 ⎜ s p ⎟ =⎜ ⎟ (1)
⎢⎣ gD ⎝ ρ D ⎠ ⎥⎦ 2 ⎜⎝ gD ⎟⎠ ⎝ 2 tan θ ⎠
where Ug is the superficial gas velocity, Gs is the solids flux, D the column diameter,
θ is the angle of internal friction and is typically around 70 degrees for round-shaped
particles.
Equation (2) developed by Bi and Fan [2] based on experimental data in CFB risers
is selected to predict the saturation carrying capacity:
U CA / gd p = 21.6 Ar 0.105 (Gs / ρ gU CA ) 0.542 (2)
Figure 1 shows such a flow regime diagram for a gas-solids vertical transport line
with an upward gas flow. It is seen that there exist five unique flow regimes in the
tube, as summarized in Table 1.
Table 1. Flow regimes and corresponding flow patters in a vertical tube with open
ends.
Regime Ug Gs Upper section Lower section
I <Ut <Gs,f Single-phase gas Dilute counter flow
flow
II <Ut >Gs,f Dense co-current Dense counter flow
flow
*
III >Ut <Gs Dilute co-current Single-phase gas
flow flow
IV >Ut Gs*<Gs<(Gs*+Gs,f) Dilute co-current Dilute counter flow
flow
V >Ut >Gs*+Gs,f Dense co-current Dense counter flow
flow
FLOW PATTERNS IN BOTTOM-RESTRICTED CIRCULATING FLUIDIZED BED

SYSTEMS
If the bottom of the tube is restrained by a distributor to prevent particles from

escaping from the bottom of the system, a circulating fluidized bed forms as shown
in Figure 2(b). Thus, two types of flow systems can be distinguished, with the free
system corresponding to transport operation as shown in Figure 2(a), while the
bottom-restricted system corresponds to (circulating) fluidized bed operation as
indicated in Figure 2(b). A circulating fluidized bed can be operated in either a co-
current upward flow (pneumatic transport) mode or fast fluidization mode, depending
on the gas velocity and solids circulation rate. It can be visualized that the flow
pattern in the bottom-restricted CFB riser should be identical to the upper section
above the solids feeding point of a free pneumatic vertical transfer line when the
solids feeding/circulating rate is lower than the saturation carrying capacity of the
gas. When the solids feeding rate is higher than the saturation carrying capacity, a
dense bed forms at the bottom of the riser and develops upward with further
increase in the solids feeding rate under steady state operation. The global flow
patterns in the riser then resembles the “fast fluidization” as commonly accepted in
the literature, with a dense region in the lower section and a dilute region in the
upper section of the riser.
Gs
Gs
Ug Ug
(a) Free system (b) Bottom-restricted
Figure 2. Illustration of (a) free vertical transport system and (b) bottom-restricted
CFB system.
A dense fluidized bed is typically operated at the saturation carrying capacity point,
with entrainment rate equal to the saturation carrying capacity. The transition from
bubbling to turbulent fluidization would thus be better defined by the flow pattern
difference in the dense fluidization region. As generally agreed, such a transition
corresponds to the balance between bubble coalescence and splitting, as reflected
by the maximum pressure fluctuations in the dense bed, denoted by transition
velocity Uc. The transition from turbulent fluidization to fast fluidization has still not
been well defined. Some considered a critical velocity, Use, corresponding to the
onset of significant particle entrainment as the transition form turbulent to fast
fluidization [3, 4]. This critical velocity can be considered as a hindered or apparent
terminal settling velocity of bed particles, reflecting the existence of particle clusters
or agglomerates in the dense fluidized beds for Group A and fine Group B particles.
For Group D particles, Use is essentially the same as the terminal settling velocity of
single particles. Others proposed a transport velocity, Utr, beyond which the sharp
change of vertical pressure drop gradient with increasing solids circulation rate
disappears to quantify the transition from turbulent to fast fluidization [5]. An
examination of pressure gradient profiles reveals that Utr varies with height. Utr may
indicate a transition of axial voidage profiles in the riser [6]. Below this velocity, a
distinct interface exists between the top-dilute and bottom-dense regions. Beyond
this velocity, the interface becomes relatively diffuse. For Group A powders, another
transition velocity, Uk, defined as the level-off point in pressure fluctuations with
further increase in gas velocity, was proposed in early years to represent the
disappearance of bubbles in the fluidized bed [5]. Such a transition velocity was not
consistently identified in later studies because of the strong influence of solids return
system design [4, 7]. Quantitatively, reported Uk values were found to be very close
to the critical velocity Use [6], suggesting some linkage between the breakdown of
bubbles in the dense bed and the onset of significant entrainment of particles from
the dense fluidized bed. If the transition from turbulent fluidization to fast fluidization
is considered as corresponding to the flow pattern changes in the dense fluidized
beds, e.g. the disappearance of regular shaped bubbles or voids, then such a
transition can be demarcated by either Uk or Use. On the other hand, if such a
transition is considered as the disappearance of a distinct dense-dilute interface
around the upper bed surface, then Utr can be used to demarcate such a transition.
Quantitatively, Utr appears to be slightly higher than Use and Uk, but generally around
1 to 2 m/s for Group A powders.
Once substantial solids entrainment occurs at a gas velocity well above the transport
velocity, the flow pattern in the CFB riser now depends on not only the superficial
gas velocity but also the solids feeding rate, with the standpipe being coupled with
the riser to establish a circulation loop. As a result, the circulation rate in the CFB
system is now also influenced by the solids inventories due to the global pressure
balance over the whole solids circulation loop [8]. Such a pressure balance
becomes a key in understanding the “choking” phenomenon defined as the critical
condition when the CFB riser terminates its stable operation, either because of the
gas blower limitation to support a dense flow in the riser or the insufficient pressure
head buildup in the standpipe to feed particles from the standpipe side into the riser
due to a lower solids inventory [9], see Figure 3. For an ideal system with no
“slugging” in the riser flow, there is no reason that prevents the riser to be operated
at a full dense suspension flow at high solids circulation rates when the limitations
from the gas blower and the standpipe solids return line are eliminated. The riser can
thus be operated in a “dense suspension upflow” regime [10], similar to those
identified in Figure 1.
Decreasing superficial gas velocity (Gs = constant)
Choking
UCC transitions CFB
Severe slugging
FFB
Blower/standpipe UCB Turbulent VCA Core-annular Vmp Homogenous

limitation flow dilute-flow dilute-flow
Bubbly/slug Vc
flow Non-choking CFB Circulating Fluidized Beds
Fast
systems
fluidization FFB Fast Fluidized Beds
Figure 3. Flow patterns and termination of stable operation in a bottom-restricted

CFB system.
FLOW REGIME MAPS FOR BOTTOM-RESTRICTED CIRCULATING FLUIDIZED
BEDS
The first attempt concerning the gas-solids co-current upward flow appears to be
made by Zenz [11] with the pressure drop over a unit length (dP/dz) plotted versus
the superficial gas velocity (Figure 4). He tried to develop a unified flow diagram
combining experimental findings from traditional low velocity fluidized beds and
pneumatic transport lines. The co-current gas-solids flow region in the diagram
spans the flow regimes encountered in the circulating fluidized beds with the lower
limit set by the “choking” velocity. The lower velocity fluidization is divided into a
"dense phase" fluidization (likely to correspond to the bubbling fluidization) and
"turbulent" fluidization (may be the same as the slugging/turbulent fluidization used
nowadays) regions. The missing linkage between the lower velocity fluidization and
the co-current upflow was attributed to “choking”. Such a regime diagram has been
further extended to incorporate more sub-regions for the co-current upflow [12],
including at least the homogeneous dispersed flow, core-annulus flow and fast
fluidization. Since the pressure gradient (dP/dz) is proportional to the solids fraction
if the friction and acceleration/deceleration are neglected, one can alternatively plot
solids fraction [13] or bed voidage [3, 14] versus the superficial gas velocity (U) or
the normalized superficial gas velocity (U/vt).
"Quiescent" Fluidization
De n
"Turbulent" Fluidization
d
se P
Be
has
e
ed
Fix
Slugging or Choking
w
Velocity W3
lo
ol t
sF
-S en
Log(dP/dz)
as rr
id
G ocu
C
Slug Flow W2
be
Tu
W1
ty
mp
W3
nE
Countercurrent
ni
Gas-Solids Flow
tio
W2
ric
sF
Ga
W1
ut
Log(Ug )
Figure 4. Flow regime diagram of Zenz (1949) for both free and bottom-restricted
vertical transport lines. W is the solid flux rate and ut is the terminal velocity.
Another group of diagrams plots solids circulation rate (Gs) or solids loading ratio
[Gs/(ρgU)] versus the superficial gas velocity or normalized superficial gas velocity,
with one typical diagram shown in Figure 5. It is seen that the flow patterns in CFB
riser could be divided into the dilute phase flow, refluxing flow, fast fluidization and,
ideally, turbulent and bubbly flow regimes if the severe slugging and blower and
standpipe limitations are absent.
14
rt
anspo
Tr Uc
Ump 10
10 as e
12 Homogeneous Flow
te-Ph
Use Dilu Flow
t
UCA ulen
Turb
10
low
la rF 11
low
nnu ly F
bb
Ug /u t
A
re- u
8 Co B
V*
low
dF
0.1-1
6 10
Umf
Be
Fast Fluidization
ed
UCC
ck
4
Pa
-2
Ut
0.01
10
BD boundary
AB boundary
Approximate
Typical AC
2
Inoperable
0 -3 boundary
0.00 0.05 0.10 0.15 0.20 0.25 0.30 10
0.001 2
1 3 10
10 30 100
10 300
1/3
Gs/ρp, m/s Ar
Figure 5. Flow regime diagram for co-current Figure 6. An ideal flow regime map
upward bottom-restricted CFB risers [12]. for both fluidized beds and co-current
upflow risers [12]. V* is the relative
velocity between the superficial gas
and particle velocities.
Grace [15] incorporated the typical operation regions of pneumatic transport lines
and fast fluidized beds into a phase diagram plotted with the dimensionless
superficial gas velocity versus the dimensionless particle diameter. The typical
operation region for bubbling fluidized beds and the spouted beds are also identified
in this diagram. Bi and Grace [12] extended this diagram by plotting the
dimensionless relative velocity between the gas and particles against the
dimensionless particle diameter, see Figure 6. Such a diagram is thus believed to
be able to identify the ideal flow regimes without the solids circulation rate Gs
provided in the diagram by assuming that the flow pattern will be primarily
determined by the relative motion between the gas and particles in co-current upflow
systems.
To summarize, each diagram has its particular use and advantages. Those
developed by Grace [15] and others mostly apply to dense fluidized beds with limited
solids entrainment/circulation. The other two types of diagrams developed for vertical
upflow in the riser, on the other hand, can provide detail quantitative boundaries
between flow regimes for each riser-particle-gas system. The one developed by Bi
and Grace [12] attempted to extend the Grace [15] diagram to the vertical co-current
upflow riser system, without considering the limitations from the blower/standpipe.
Therefore, the severe slugging, blower and standpipe limitations are not captured in
almost all of these ideal phase diagrams, but can be identified by using appropriate
analyses and approaches as demonstrated in [8] for specific CFB systems.
CONCLUSION
A flow regime diagram for the non-restricted vertical transport lines includes at least
5 different flow patterns in the riser below and above the solids feeding level, with
flooding limiting the maximum solids downflow through the lower section and
saturation carrying capacity limiting the upward solids flow rate. In a bottom-
restricted CFB riser, the same flow patterns exist in the upper section, except that
there are now no particles leaving the riser from the bottom of the riser. The
coupling of the riser and the standpipe makes the maximum solids circulation rate
now being determined by the pressure balance over the whole CFB loop and the
capability of the standpipe and the gas blower to withstand pressure fluctuations
induced by severe slugging in the riser for slugging systems.
REFERENCES
1. Papa, G.; Zenz, F. A. Optimize performance of fluidized-bed reactors. Chem.

Eng. Prog. 1995, 91(4), 32.
2. Bi HT, Fan LS. Regime transitions in gas-solid circulating fluidized beds. Paper
#101e, AIChE Annual Meeting, Los Angeles, Nov. 17-22, 1991.
3. Li Y, Kwauk M. The dynamics of fast fluidization. In: Grace JR, Matsen JM, eds.
Fluidization. New York: Plenum, 1980, pp.537-544.
4. Bi HT, Grace JR, Zhu JX. Regime transitions affecting gas-solids suspensions
and fluidized beds. Chem Eng Res Des 73:154-161, 1995.
5. Yerushalmi J, Cankurt NT. Further studies of the regimes of fluidization. Powder
Technol 24:187-205, 1979.
6. Bi, H.T., Transition from turbulent to fast fluidization, Chem. Eng. Comm., 189,
942-958, 2002.
7. Rhodes, M.J. and D. Geldart, Transition to turbulence? Fluidization V, K.
Ostergaard and A. Sorensen eds., Science Foundation, New York, pp.281-288,
1986.
8. Bi HT, Zhu JX. Static instability analysis of circulating fluidized beds and the
concept of high-density risers. AIChE J 39:1272-1280, 1993.
9. Bi HT, Grace JR, Zhu JX. On types of choking in pneumatic systems. Int J
Multiphase Flow 19:1077-1092, 1993.
10. Grace JR, Issangya AS, Bai DR, Bi HT, Zhu JX. Situating the high-density
circulating fluidized beds. AIChE J 45:2108-2116, 1999.
11. Zenz FA. Two-phase fluidized-solid flow. Ind Eng Chem 41:2801-2806, 1949.
12. Bi HT, Grace JR. Flow regime maps for gas-solids fluidization and upward
transport. Int J Multiphase Flow, 21:1229-1236, 1995.
13. Squires, A.M., M. Kwauk and A.A. Avidan, Fluid beds: at last, challenging two
entrenched practices, Science, 230, 1329-1337, 1985.
14. Avidan, A.A. and J. Yerushalmi, Bed expansion in high velocity fluidization,
Powder Technol., 32, 223-232, 1982.
15. Grace JR. Contacting modes and behaviour classification of gas-solid and other
two-phase suspensions. Can J Chem Eng 64:353-363, 1986.
GAS-SOLIDS HYDRODYNAMICS IN A CFB WITH 6 CYCLONES
AND A PANT LEG
Leming Cheng a, Xinglong Zhou a, Chao Wang a, Qinhui Wang a, Zhongyang Luoa,
Kefa Cen a, Li Nie b Chaogang Wu b, Qi Zhou b
a
State Key Laboratory of Clean Energy Utilization, Zhejiang University, Hangzhou
310027, China
b
Dongfang Boiler Group Co., Ltd. Chengdu 611731, China
ABSTRACT
Solids volume fraction and particle velocity profiles were measured with a fiber
optical probe in a cold circulating fluidized bed test rig with 6 parallel cyclones and a
pant leg. Results in the pant leg zone, main bed zone and exit zone of the furnace
are reported. The work also includes the influences of superficial gas velocity,
secondary air rate and static bed height on the gas-solids hydrodynamics.
INTRODUCTION
Circulating fluidized beds (CFBs) are commercially employed in a number of

gas–solids contacting processes such as fluid catalytic cracking, fossil fuel
combustion and gasification (1). Knowledge of the gas-solids hydrodynamics is the
key to understanding and predicting chemical interactions between gas and particles,
heat transfer performance and erosion in the furnace (2).
The majority of previous experimental studies of solid flux profiles have been carried
out in CFBs with single furnaces (3-5). In single furnace, a typical core-annulus flow
pattern has been observed by many researchers in laboratory and industrial scale
units (5-7). However, the structure of a CFB furnace is becoming more and more
complex during scale-up, especially in recent development of a 600MW CFB boiler.
Large-scale CFB furnaces have new characteristics, i.e. multiple outlets, pant legs
and internal walls. Few studies have been conducted and reported on lateral solids
flow in the riser with a pant leg structure. Therefore, further study on the gas-solids
hydrodynamics in a large-scale CFB furnace is required to provide more
understanding of the flow structure.
In this study, solids volume fraction and particle velocity profiles in a CFB with 6
cyclones and a pant leg furnace were investigated by using a fiber optical probe
(FOP). The work focused on three zones in the furnace, the lower pant leg zone, the
main bed zone and the exit zone of the furnace. Effects of superficial gas velocity,
secondary air rate and static bed height on the solids volume fraction and particle
velocity distributions were examined. This was a part of the work conducted to
develop the 600MW CFB boiler.
EXPERIMENTAL
The experiments were done in the CFB cold model system shown in Fig. 1. The test
rig was scaled down from a 600 MW CFB boiler (8) following the scaling law
proposed by Glicksman et al (9). The riser had a height of 5.5 m and the bottom
section of the riser looks like a pair of pants (pant leg structure). The internal walls of
the pant leg were 1 m high. Above 1 m from the gas distributors, the riser had a
cross-sectional area of 0.422 × 0.727 m2. 6 parallel cyclones were located
asymmetrically on the left and right walls of the riser (Fig. 2). Circulating loops were
formed with the pant leg riser, 6 cyclones, 6 standpipes and 6 loopseals. Most of the
apparatus was made of Plexiglas for convenient observation. The measurements
were conducted at atmospheric pressure and ambient temperature.
Fig. 1. Experimental CFB cold test rig Fig. 2. Layout of the 6 parallel cyclones
During operation, the solids fluidization in the individual pant legs was controlled by
independent primary air flow. Bed pressures in the two pant legs were kept in
balance by a pressure control unit (PCU).
The Fiber optical probe (FOP) method (10-12) was used to measure the solids
volume fraction and the particle velocity in the riser. The probe measurement system
(PV6D) was composed of an optical fiber probe, a control system, an A/D converter
and a data acquisition system. It was calibrated before the measurements were
made (13).
The FOP measurements were taken at seven different height levels (level 1: 0.25,
level 2: 0.65, level 3: 1, level 4: 1.45, level 5: 2.55, level 6:3.65 and level 7: 5.25 m)
above the air distributors as shown in Fig. 1. At locations from level 1 to level 6, the
fiber optic probe was traversed from the left wall to the right wall. It was traversed
from the front wall to the rear wall at level 7, as shown in Fig. 2. It should be noted
that a positive value for the particle velocity means the particle moves upward in the
riser at levels 1 ~ 6 and flows toward the cyclones at level 7.
Glass beads with a density of 2364 kg/m3 and an average particle diameter of 0.114
mm were used as bed materials. The effects of superficial gas velocity (u0),
secondary air rate (RSA) and static bed height (Hs) on the solids volume fraction and
particle velocity profiles were studied in the experiments. The bed material properties
and the operational parameters of the boiler and model are shown in Table 1.
Table 1. Bed material properties and operational parameters

Parameter Unit Boiler Model
Temperature, Tb °C 900 50
3
Gas density, ρg kg/m 0.301 1.093
2
Gas viscosity, Vs m /s 1.55E-04 1.80E-05
Mean particle diameter of, dp mm 0.400 0.114
Density of particle, ρs kg/m3 2000 2364
Superficial gas velocity, u0 m/s - 1.7
Minimum fluidization velocity, umf m/s 0.050 0.016
2
Solid flux, Gs kg/m s - 6.00
Solids volume fraction and particle velocity profiles in the pant leg, main bed
and exit zone
Fig. 3 shows the solids volume fraction (εs) and particle velocity (up) profiles at level 2
(within the pant leg section, 0.65 m above the gas distributors) for u0 = 1.7 m/s, RSA =
10 % and Hs = 500 mm. Corresponding results for the left and right pant leg show
similar distributions of εs and up although the particles in the two pant leg furnaces are
fluidized independently. The solids volume fraction increased near the walls since it
requires less energy for the bubbles to pass through the center of the bed (14).
Particle velocity decreased near the walls, and a negative axial solids velocity
appeared near the wall.
Lateral profiles of εs and up at level 3 (top- section of the pant leg, 1 m above the gas
distributors) at the same conditions of Fig. 3 are shown in Fig. 4. A W-shaped
distribution of the solids volume fraction and an M-shaped distribution of the particle
velocity are seen in Fig. 4. Solid boundary layers exist near the side walls and the
internal walls of the pant leg. The solids volume fraction in the boundary layer is
higher than in the core zone. The maximum solids volume fraction in the boundary
layer near the internal walls was even higher than in the boundary layer near the side
walls. It was found that the downflow of particles in the boundary layers had different
downflow velocities at different locations. The downflow particles near the enclosure
walls had higher velocities (1.5 ~ 2 m/s) than that near the pant leg internal walls
(below 1 m/s).
Fig. 3. Profiles of εs and up at level 2 Fig. 4. Profiles of εs and up at level 3
The above results on εs and up profiles in Fig. 3 and Fig. 4 give a general picture of
the gas-solids flow pattern in the pant leg zone. Within the pant leg zone, two
core-annulus flow structures are formed independently. These two cores are merged
into one core at the top of the pant legs and then a W-shaped profile of solids volume
fraction and an M-shaped profile of particle velocity are formed.
Above the pant leg section, the riser is a single furnace. Fig. 5 shows εs and up
profiles at level 4 (1.45 m above the air distributors) and shows a transitional flow
pattern from the two core-annulus structures to a traditional core-annulus structure.
The particle velocity profile has completely transitioned, but the solids volume
fraction profile still is higher in the center of the furnace.
Fig. 6 shows εs and up profiles of a traditional core-annulus flow structure in the upper
dilute section of the riser (at level 5, 2.55 m above the air distributors). The boundary
layer thickness is defined as the distance from the wall to the position of zero particle
velocity, i.e. the position separating the particle upflow in the bed core and the
particle downflow near the wall (7). From the areas marked out by the dotted lines in
Figs 4 to 6, the boundary layer thickness is about 5 to 15 mm which decreases
slightly with the height of the riser. This is in agreement with results from literature (6).
Inside the core zone, the εs and up profiles are both flat with an average εs of
approximately 0.017 and an average up of about 1 m/s. The particles in the boundary
layer have a downflow velocity which varies from 0.7 to 1.5 m/s depending on
location. The downflow velocity reaches a lower value of about 0.7 m/s near the wall.
This suggests a momentum transfer between the falling film and the wall, which is
likely to depend on the properties of the wall surface (surface roughness of wall,
inclination of surfaces from the vertical direction, etc.). The resulting solids volume
fraction and particle velocity distributions are similar to measurements reported by
Zhang et al. (7) .
Fig. 5. Profiles of εs and up at level 4 Fig. 6. Profiles of εs and up at level 5
The εs and up distributions at the exit section presented in Fig. 7 were measured at
level 7 (near the horizontal ducts, 5.25 m above the air distributors). Due to the
complicated structure of the exit section and the asymmetric layout of the cyclones,
solids volume fraction and particle velocity were not evenly distributed across the
furnace. Of the three outlets indicated by the dotted lines in Fig. 7, a slightly higher
particle velocity and a lower solids volume fraction were measured for the middle
outlet (outlet B).
Effect of superficial gas velocity, secondary air rate and static bed height
The evolution of the εs and up profiles as a function of superficial gas velocity (u0) is
shown in Fig. 8. The results were measured at level 5 for a secondary air rate of 10
% and a static bed height of 500 mm. The solids volume fraction in the core zone
increased with increasing superficial gas velocity. When u0 increases more particles
are entrained into the upper section of the riser. However, the superficial gas velocity
did not show a significant impact on solids volume fraction in the boundary layer.
Moreover, in spite of increasing superficial gas velocity, it did not have a significant
effect on particle velocity.
Fig. 9 shows εs and up profiles at a constant superficial gas velocity (u0 = 1.70 m/s)
and static bed height (Hs = 500 mm) but at different secondary air rates (RSA). It can
be seen that at level 6, the solids volume fractions in both the core zone and the
boundary layer decrease when secondary air rate increases from 10 % to 20 %. The
difference in the solids volume fraction is most likely, because of the barrier effect of
the secondary air (15). The particle velocity in the core decreases when RSA
increases due to the reduction in the acceleration of the particles due to primary air
(16).
Fig. 7. Profiles of εs and up at level 7 Fig. 8. Profiles of εs and up for different u0
Fig. 9. Profiles of εs and up for different Fig. 10. Profiles of εs and up for different
Rsa at level 6 Hs at level 6
Fig. 10 shows εs and up profiles at level 6 in the furnace for different static bed heights
(Hs = 400 and 500 mm). The solid volume fractions in both the core zone and the
boundary layer when Hs = 500 mm were higher than that for a lower Hs. This is
reasonable because a higher Hs results in a higher average solids volume fraction in
the whole furnace. Comparing the up profiles in Fig. 10, it can be seen that up in the
core zone increases slightly with Hs while no clear influence is observed in the
boundary layer.
CONCLUSIONS
The results of the investigation show that within the pant leg section, two
core-annulus flow structures are formed independently. These two cores are merged
into one core above the pant leg section and the solids flow pattern makes a
transition to a traditional core-annulus structure. The boundary layer thickness is
about 5 to 20 mm which decreases slightly with riser height. The particles in the
boundary layer have a downflow velocity which varies from 0.7 to 1.5 m/s. Due to the
asymmetric layout of the three riser outlets on each side wall, a higher particle
velocity and a lower solids volume fraction were observed in the middle outlet.
The solids volume fraction in the upper section of the riser increases with superficial
gas velocity and static bed height but decreases with secondary air rate. Particle
velocity in the core zone of the upper riser section increases with static bed height
and decreases with secondary air rate. There was no significant influence of bed
height on particle velocity in the boundary layer.
ACKNOWLEDGEMENT
The authors are grateful for financial support of the National Key Technologies R & D
Program of China (No. 2006BAA03B02-08, 2006BAA03B01-09).
NOTATION
dp: Mean diameter of particle [mm] u0: Superficial gas velocity [m/s]
2
Gs: Solid flux [kg/m s] umf: Minimum fluidization velocity [m/s]
H: Height of the riser [m] up: Particle velocity [m/s]
Hs: Static bed height [mm] Vs: Gas viscosity [m2/s]
D: Depth of the riser’s cross-section [m] εs: Solids volume fraction [-]
X: Radial position from left wall [m] ρs: Solids density [kg/m3]
RSA: Secondary air rate [%] ρg: Gas density [kg/m3]
Tb: Bed temperature [°C]
REFERENCES
1. Cheng LM, Chen B, Liu N, Luo ZY, Cen KF. Effect of characteristic of sorbents on
their sulfur capture capability at a fluidized bed condition. Fuel 2004: 83:
925-932.
2. Basu P. Combustion of coal in circulating fluidized-bed boilers: a review.
Chemical Engineering Science 1999: 54: 5547-5557.
3. Ye S, Qi XB, Zhu J. Direct Measurements of Instantaneous Solid Flux in a
Circulating Fluidized Bed Riser using a Novel Multifunctional Optical Fiber Probe.
Chem Eng Technol 2009: 32: 580-589.
4. Malcus S, Cruz E, Rowe C, Pugsley TS. Radial solid mass flux profiles in a
high-suspension density circulating fluidized bed. Powder Technology 2002: 125:
5-9.
5. Salvaterra A, Geldart D, Ocone R. Solid flux in a circulating fluidized bed riser.
Chem Eng Res Des 2005: 83: 24-29.
6. Kim SW, Kirbas G, Bi HT, Lim CJ, Grace JR. Flow structure and thickness of
annular downflow layer in a circulating fluidized bed riser. Powder Technology
2004: 142: 48-58.
7. Zhang WN, Johnsson F, Leckner B. Fluid-Dynamic Boundary-Layers in CFB
Boilers. Chemical Engineering Science 1995: 50: 201-210.
8. Li Y, Nie L, Hu XK, Yue GX, Li WK, Wu YX, Lu JF, Che DF. Structure and
performance of a 600MWe supercritical CFB boiler with water cooled panels. In:
20th International Conference on Fluidized Bed Combustion. Xian, China, 2009:
132-136.
9. Glicksman LR, Hyre M, Woloshun K. Simplified Scaling Relationships for
Fluidized-Beds. Powder Technology 1993: 77: 177-199.
10. Li SH, Yang HR, Zhang H, Yang S, Lu JF, Yue GX. Measurements of solid
concentration and particle velocity distributions near the wall of a cyclone. Chem
Eng J 2009: 150: 168-173.
11. Werther J. Measurement techniques in fluidized beds. Powder Technology 1999:
102: 15-36.
12. Zhu JX, Li GZ, Qin SZ, Li FY, Zhang H, Yang YL. Direct measurements of
particle velocities in gas-solids suspension flow using a novel five-fiber optical
probe. Powder Technology 2001: 115: 184-192.
13. Zhang H, Johnston PM, Zhu JX, de Lasa HI, Bergougnou MA. A novel calibration
procedure for a fiber optic solids concentration probe. Powder Technology 1998:
100: 260-272.
14. Guo QJ, Werther J. Flow behaviors in a circulating fluidized bed with various
bubble cap distributors. Ind Eng Chem Res 2004: 43: 1756-1764.
15. Koksal M, Hamdullahpur F. Gas mixing in circulating fluidized beds with
secondary air injection. Chem Eng Res Des 2004: 82: 979-992.
16. Ersoy LE, Golriz MR, Koksal M, Hamdullahpur F. Circulating fluidized bed
hydrodynamics with air staging: an experimental study. Powder Technology
2004: 145: 25-33.
PRODUCTION OF GASOLINE AND GASEOUS OLEFINS:
CATALYTIC CO-CRACKING OF PYROLYSIS OIL
RESIDUE
P. Bielansky, A. Reichhold, A. Weinert
Vienna University of Technology, Institute of Chemical Engineering
A 1060 Vienna, Getreidemarkt 9/166-3
ABSTRACT
Co-processing of biomass in petroleum refineries is a promising approach for biofuel
production. In this work fluid catalytic cracking of residue from a co-pyrolysis with
sawdust and VGO (1:2) was investigated. The pyrolysis oil residue with a boiling
range bigger than 350 °C was mixed in different ratios with VGO and could be
processed successfully up to 20 m%. Crack gas amounts increased while gasoline
and total fuel yields decreased compared to VGO cracking. The gasoline obtained
has a high octane number and is oxygen free.
INTRODUCTION
For the last decades crude oil was the most important raw material for the
production of transport fuels. This leads to several problems like the dependence on
politically unstable countries and the emission of huge amounts of fossil CO2. Many
scientists see a correlation between global warming and the increase in CO2
concentration in the atmosphere (1). As a consequence new ways to substitute
fossil fuels by renewable fuels have been investigated in the last years. Currently
the production of so called first generation biofuels like bio ethanol and biodiesel can
be considered as state-of-the-art technologies with considerable production
capacities worldwide (2, 3). A disadvantage is that these fuels are derived from
agricultural products which lead to a food vs. fuel dilemma (4).
Second generation biofuels made of lignocellulosic biomass from forestry as well as

agricultural and industrial waste are not in competition with food. Gasification with
downstream Fischer Tropsch synthesis has been investigated extensively (5-7).
However, high investment costs lead to high fuel prices. In contrast, co-processing
biomass with FCC-plants in existing crude oil refineries requires only little additional
investments. Due to the very large scale the conversion process is highly efficient
and existing downstream facilities for product upgrading can be used (8).
The suitability of the FCC-process for vegetable oils and used cooking oils has been
shown by several researchers with promising results (9-11). The use of
lignocellulosic feed requires prior liquefaction. Bio oil obtained from flash pyrolysis is
an interesting possibility for co-processing. Due to high oxygen and water content it
is not miscible with VGO and needs upgrading associated with additional costs (12).
Alternatively, bio oil can be in situ upgraded by introducing catalysts during pyrolysis
(8).
In literature some experimental results with different pyrolysis oils as FCC feedstock
can be found. All show the tendency to high coke formation and reactor plugging if
they are processed in high concentrations (8, 12).
A new approach is co-pyrolysis. VGO is heated up in a stirred tank reactor and

biomass is added. Released inorganic substances from biomass decomposition act
catalytically. Thereby a part of the VGO is cracked mainly to diesel as well as
gasoline and gases. These products leave the reactor. In this paper the suitability of
a co-pyrolysis residue (boiling range 350°C plus) in admixtures with VGO in an
FCC-plant is investigated.
EXPERIMENTAL
Small scale pilot plant
An FCC plant consists of the two main parts: reactor (usually constructed as riser),
and regenerator. All experiments were conducted in a fully continuous FCC pilot
plant at Vienna University of Technology. An internal circulating fluidized bed was
used which means that regenerator and reactor are arranged concentrically in one
apparatus. In Figure 1 a scheme of the apparatus and the periphery is shown, Table
1 comprises some benchmark data.
To chimney
Gas
Natural Gas
Product
Gas-sampling tube for GC-analysis
N2
Air Cat-cooler
Gas meter
M
M Condensate Diaphragm pump
Feed
Barrel 50l
Flue gas
M M
Heated and Gear pump Gas cooler
stirred beaker Gas analyzer
Figure 1: Scheme of the FCC pilot plant and periphery

Feed is dosed by a gear- or a peristaltic pump and preheated in a tubular oven to a
temperature barely under boiling temperature (approximately 280–320 °C) and
enters the apparatus at the bottom of the riser. Due to the contact with the hot
catalyst it evaporates instantaneously resulting in a strong upwards expansion.
Thereby catalyst is sucked into the riser and pneumatically transported to the top. All
cracking reactions as well as coke formation and deposition on the catalyst surface
occur in the riser within a mean residence time of approximately 0.9 s. At the particle
separator catalyst and products are separated. The product gas leaves the
apparatus at the top. Due to the large difference in diameter from the riser to the
upper part of the apparatus the fluidization velocity decreases under transportation
velocity. Thus, the catalyst flows down the return flow tube and enters the
regenerator through a nitrogen fluidized siphon which acts as a gas barrier. In the
regenerator coke is burned with air whereby the catalyst is regenerated. Emerging
flue gas leaves the reactor laterally. The heat generated is required for the
endothermic cracking reactions. It is transported via the hot bed material as well as
direct heat transfer to the riser. Feedstocks which yield more coke, and thus to a
high catalyst temperature in the regenerator, require a cooler in the bottom part to
adjust the riser temperature.
Table 1: Benchmark data of the FCC pilot plant

Height 2.5 m Riser temperature 550 - 600°C
Riser length 2.022 m Regenerator temperature 590 - 650°C
Riser diameter 0.0205 m Feed flow 1 - 3 l/h
Regenerator diameter 0.18 m Riser residence time ca. 0 9 s
Catalyst Commertial E-Kat Fluidization bottom 1.5 Nl/min
Shape selective zeolite Fluidization syphon 8 Nl/min
Catalyst mass 9 - 11 kg Fluidization regenerator 29 Nl/min
Catalyst spectrum 20 - 200 μm Fluidization velocity 16 vmf
Pressure Ambient Flue gas oxygen 1 - 2 vol%
Sufficient siphon fluidization is required in order to maintain circulation. Interrupting

this fluidization results in a breakdown of the circulation. As a result the level in the
return flow tube increases while it decreases in the regenerator. Pressure measured
at the bottom of the reactor decreases proportionately with the bed height whereby
the circulation rate can be calculated during operation.
The product gas is burned in a flare. For analyses purposes a branch current is
sucked off before the flare by a diaphragm pump and condensed in three intensive
coolers. The incondensable crack gas flows through a gas sampling tube and a gas
meter and is then combusted with the rest of the product. The regenerator flue gas
is determined by a gas analyzer.
Analysis
Gaseous and liquid products were analyzed separately with two gas
chromatographs.
The gas chromatograph used for crack gas analysis consists of two capillary
columns and two detectors. Hydrocarbons are detected by a flame ionization
detector (FID), nitrogen and carbon dioxide are detected by a thermal conductivity
detector (TCD). Liquid products were analyzed conducting a simulated distillation
(SimDist) using a gas chromatograph with a capillary column and an FID.
Additionally a PIONA analysis was conducted to obtain detailed information of the

product composition and quality. RON and MON were calculated out of these
results.
Feedstock and Catalyst
The experiments were conducted with different mixtures of VGO and residue from a
co-pyrolysis from VGO and lignocellulosic biomass. Both feeds were provided by the
OMV AG. VGO is the top product of the vacuum distillation with a boiling range
between 350 and 650°C. It consists mainly of paraffins, naphtenes und aromatics. A
low sulfur content to obtain long catalyst lifetime is achieved by hydro treating
(Figure 2). The co-pyrolysis was conducted in a batch stirred tank reactor under
atmospheric pressure. VGO was heated to approximately 350 °C and 33 m%
biomass (sawdust) was added. The lignocelluloses started to decompose
immediately to gaseous and liquid products, coke, and inorganic compounds. These
inorganic substances (mainly salts) act catalytically and enable cracking of a part of
the VGO. All substances with a boiling range below reactor temperature (mainly
diesel with a cetane number of approximately 40 as well as gasoline, gases, and
water) leave the reactor. The remaining residue and coke are separated by a
centrifuge. According to C14 analysis the residue contains a certain amount of
biomass derived substances. Only small amounts of the oxygen from the biomass
remain in the residue. Table 2 shows the elementary analysis. Detailed analyses of
the co-pyrolysis residue are confidential and cannot be published. In this paper the
suitability of this residue (boiling range 350°C plus) in admixtures with VGO in an
FCC-plant is investigated.
Table 2: Composition of the co-pyrolysis

residue
Nitrogen 0.3 [m%]

Carbon 84.7 [m%]
Hydrogen 11.1 [m%]
Sulfur <0.1 [m%]
Oxygen 1.8 [m%]
Ash 1.576 [m%]
Water <0.1 [m%]
Figure 2: The main components of
VGO
The commercial FCC equilibrium catalyst E-Space from the company Grace
Davison was used. It is an acidic spray dried REUSY-catalyst which is partially
coated with ZSM-5-zeolite crystals. It was already in use at the OMV refinery in
Schwechat and extracted during the process from the FCC-plant. Thus there was no
need to steam it to obtain a certain conversion level.
Definitions and calculations
For product characterization a lump model was used (Table 3). Gaseous and liquid
fractions were separated by condensation. Water and liquid organic products can be
easily separated by phase separation. The liquid organic phase was divided
furthermore according to the boiling range in gasoline, light cycle oil (LCO) and
residue. In order to determine the coke lump the flue gas was analyzed by a gas
analyzer for O2 (paramagnetic measurement method) as well as CO and CO2
(infrared measurement method). The amount of coke is calculated out of these
values.
Table 3: The six Lump Model

Fraction Lump Composition, Boiling range Analysis method
Gas Fraction Crack gas C1-C4 GC
Liquid fraction Gasoline <215°C SimDist
LCO 215 - 320°C SimDist
Residue >320°C SimDist
Water Gravimetric
Solid fraction Coke Flue gas composition
The total fuel yield X is defined as:
mCrack gas + mGasoline

TFY =
mFeed
RESULTS
Experiments lasted about six hours each in steady state operation. Three sample
periods of 15 minutes were made per run and analyses values were averaged. The
riser temperature was set to 550 °C.
15
80 LCO
Residue
70
10
Amount [m%]
Amount [m%]
Total fuel yield

60
Crack gas
50 Gasoline
5
40
30
0
0 5 10 15 20 0 5 10 15 20
Amount co-pyrolysis residue [m%] Amount co-pyrolysis residue [m%]
Figure 3: Influence of co-pyrolysis Figure 4: Influence of co-pyrolysis

amount on total fuel yield, crack gas, amount on light cycle oil and residue
and gasoline
Figure 3 depicts the total fuel yield. It decreases from approximately 82.5 m% for
VGO to 77.5 m% with 20 m% admixture of pyrolysis residue. The gasoline yield
decreases significantly from approximately 52 m% to 39 m% with a pyrolysis residue
content of 17.5 m% and increases to 40 m% with 20 m% pyrolysis residue. Crack
gas rises clearly from 31 m% to a maximum of 38 m% between 10 and 17.5 m%
pyrolysis residue addition and decreases slightly to 37.5 m% at a 20 m% admixture.
LCO increases slightly with a maximum at 17.5 m% pyrolysis residue addition.
Approximately 4 m% residue is formed with a clearly higher value at 20 m%
pyrolysis residue admixture (Figure 4).
15
8
10
Amount [m%]
Coke [m%]
Ethene
6 Propene
5
4
0
0 5 10 15 20 0 5 10 15 20
Amount co-pyrolysis residue [m%] Amount co-pyrolysis residue [m%]
Figure 5: Influence of co-pyrolysis Figure 6: Influence of co-pyrolysis

amount on coke amount on ethene and propene
Coke amounts increase strongly with higher pyrolysis residue ratios with a maximum
at 17.5 m% addition (Figure 5). Ethene and propene increase with increasing
pyrolysis residue admixture. This is mainly caused by higher crack gas yield,
concentration of gas components stays roughly constant (Figure 6).
The C/O ratio for experiments with pyrolysis residue addition was higher than for
VGO experiments (Figure 7). Figure 8 shows the gasoline composition for three
samples with different pyrolysis residue amounts in the feedstock. Naphtenes and
iso-paraffins concentrations are less with admixtures, more aromatics are formed.
N-paraffins and olefins stay roughly constant.
60
0 m% Pyrolysis residue
50 10 m% Pyrolysis residue
30 20 m% Pyrolysis residue
40
Amount [m%]
25
30
C/O Ratio [-]
20
20
15 10
10 0
0 5 10 15 20 es ins ins ins ins ins tics
hten araff araff Olef i-Olefn-OleAf roma
Amount co-pyrolysis residue [m%] Nap i-P n-PCyclic
Figure 7: Influence of co-pyrolysis Figure 8: Gasoline composition with

amount on the catalyst/oil ratio different amounts of co-pyrolysis
residue
Table 4 depicts some gasoline characteristics. Research octane numbers (RON) are
generally at a high level with bigger values for experiments with pyrolysis residue
addition. Motor octane numbers (MON) show an opposite trend. Benzene (like
aromatics in general) increases at higher pyrolysis residue ratios. The caloric value
for all samples is at a similar level. Gasoline from feedstock with addition contains
less hydrogen. Further on, density and thus average molecular weight are slightly
higher.
Table 4: Gasoline characteristics

Amount pyrolysis oil 0 10 20 [m%]
RON 101.8 104.4 103.2 [-]
MON 90.5 89.5 88.2 [-]
Benzene 0.99 1.64 1.56 [m%]
Caloric value 42.85 42.19 42.28 [MJ/kg]
C:H Ratio 0.57:1 0.62:1 0.61:1 [-]
Density 763.5 791.2 788.0 [kg/m³]
Average molecular weight 104.2 106.3 106.4 [g/mol]
CONCLUSIONS
Admixtures of VGO and co-pyrolysis residue up to 20 m% could be converted
successfully in a fully continuous FCC pilot plant for several hours in steady state
operation. No major adaption was necessary. Higher pyrolysis residue contents led
to more crack gas and less gasoline, resulting in a decrease in total fuel yield. The
product quality was very high with RON clearly over 100 and MON around 90. Due
to the chemical similarity (the product is oxygen free) it can substitute regular
gasoline in any percentage without limitation.
VGO experiments could be conducted without catalyst cooling in the regenerator

bottom. Due to the bigger coke yield with pyrolysis oil admixtures the regenerator
temperature increases and cooling was necessary to reach the required riser
temperature. The VGO experiments showed a decrease in temperature from riser
bottom to the top. Experiments with pyrolysis oil admixtures had a different trend
due to relatively low catalyst temperature in the bottom part. This led to higher
reaction temperature in the upper part of the riser thus promoting secondary
cracking. Higher C/O-ratios for experiments with pyrolysis oil addition also supported
secondary cracking. These two process parameters may have enhanced gas
formation.
For admixtures with more than 20 m% pyrolysis oil no stable operation point could
be found. The feed tended to strong coking in the feed inlet area after a few minutes
of operation. As a result the riser clogged and circulation collapsed.
One of the big advantages of the presented technology is the possibility of co-
processing in existing petroleum refineries. The large scale of these facilities leads
to high efficiency in the conversion and product upgrading process. Additionally,
considerable amounts of propene and ethene are formed which can be used to
produce polymers out of renewable sources.
ACKNOLEDGEMENT
This work was supported by OMV AG.
REFERENCES
1 IPCC, Climate Change 2007 - The Physical Science Basis: Working Group I,
Contribution to the Fourth Assessment Report of the IPCC, Cambridge,
University Press, (2007)
2 EU, Panorama of Energy – Energy Statistics to Support EU Policies and
Solutions, (2007)
3 IEA, Biofuels for Transport – An International Perspective, 2004
4 R. Rathmann, A. Szklo, R. Schaeffer, Land use competition for production of food
and liquid biofuels: An analysis of the arguments in the current debate,
Renewable Energy 35 (2010) 14–22
5 M.J.A. Tijmensen et al., Exploration of the possibilities for production of Fischer-
Tropsch liquids and power via biomass gasification, Biomass and Bioenergy 23
(2002) 129–152
6 T. Takeshita, K. Yamaji, Important roles of Fischer-Tropsch synfuels in the global
energy future, Energy Policy 36 (2008) 2773–2784
7 S. Fürnsinn et al., Diesel aus Holz – die Fischer- Tropsch Synthese als
zukunftsweisende Technologie zur Gewinnung flüssiger Brennstoffe aus
Biomasse, 4, Internationale Energiewirtschaftstagung an der TU-Wien, 2005
8 A.A. Lappas, S. Bezergianni, I.A. Vasalos, Production of biofuels via co-
processing in conventional refining processes, Catalysis Today 145 (2008) 55–
62
9 R.O. Idem, S.P.R. Katikaneni, N.N. Bakhshi, Catalytic conversion of canola oil to
fuels and chemicals: roles of catalyst acidity, basicity and shape selectivity on
product distribution, Fuel Processing Technology 51 (1997) 101–125
10 T.L. Chew, S. Bhatia, Catalytic processes towards the production of biofuels in a
palm oil and oil palm biomass-based biorefinery, Bioresource Technology 99
(2008) 7911–7922
11 P. Bielansky, A. Reichhold, C. Schönberger, Catalytic cracking of rapeseed oil to
high octane gasoline and olefins, Chemical Engineering and Processing 49
(2010) 873–880
12 G. Fogassy, Biomass derived feedstock co-processing with vacuum gas oil for
second-generation fuel production in FCC units, Applied Catalysis B:
Environmental 96 (2010) 476–485
COMMISSIONING OF A 0.8 MWTH CFBC FOR OXY-FUEL
COMBUSTION
L. Jia, Y. Tan, D. McCalden, Y. Wu, I. He, R. Symonds and E.J. Anthony
CanmetENERGY, 1 Haanel Drive, Ottawa, ON, Canada, K1A 1M1
ABSTRACT
Oxy-fuel fluidized bed combustion (FBC) is a new technology being developed for
power production from carbonaceous fuels while producing a nearly pure steam of
CO2 ready for sequestration or storage. Unlike oxy-fuel pulverized fuel combustion
technology, oxy-fuel FBC offers the opportunity to use poor quality coals,
hydrocarbon residues and a range of other materials including biomass. In Canada,
pitches, tars and bottoms, in particular, are available in large quantities in western
Canada, and this technology offers an opportunity to deal with many of these waste
feedstocks in an environmentally benign manner. In addition, oxy-fuel circulating
FBC (CFBC) can be fired at lower flue gas recycle ratio, offering potentially smaller
plants for any given power output, and can capture sulphur in situ.
CanmetENERGY has been operating a 75 kW oxy-fuel CFBC since 2006 with full
flue gas recycle. Initial results were very encouraging and in order to further study
oxy-fuel FBC technology, a 0.8 MW th CFBC unit has been retrofitted for oxy-fuel
research. The facility is used to emulate commercial oxy-fuel CFBC performance.
The modifications included adding oxygen supply, flue gas recycle train, airtight fly
ash discharge, flue gas compressor for baghouse pulsing and system purge, etc., as
well as upgrading the control and instrumentation for oxy-firing. The most major
challenge has been to properly seal the entire CFBC unit to prevent air ingress.
Fuels fired during the commissioning phase included bituminous coal and petroleum
coke from the US, and lignite from Saskatchewan. Combustion under oxy-fuel
conditions has proved to be very stable and the transition from air firing mode to oxy-
fuel firing mode and vice versa were quick and presented little operational difficulties.
This work has demonstrated that the retrofitted oxy-fuel CFBC can produce a stream
of flue gas containing 80% to 90% CO2. The NOx emissions were significantly lower
compared to air firing in CFBC with the same fuel. SO2 capture was in the range of
70% to 75%, but limestone utilization is lower than in air-firing mode, and research is
on-going to better understand sulphation under oxy-firing conditions.
INTRODUCTION
Anthropogenic CO2 production is primarily driven by fossil fuel combustion. To
reduce greenhouse gas emissions from fossil fuel combustion in the electric utility
industry, CO2 capture and storage (CCS) appears to be among the most promising
methods (1). Oxy-fuel pulverized coal combustion technology had been studied for
many years (1, 2, 3). The commissioning of a 30 MW th oxy-fuel demonstration plant
at Schwarze Pumpe in Germany by Vattenfall is an important milestone for the
development of pulverized fuel (PF) oxy-fuel technology. The Schwarze Pumpe oxy-
fuel plant has been running initial tests since mid 2008 (4).
Oxy-fuel circulating fluidized bed combustion (CFBC) is a relatively new technology

compared with oxy-fuel PF combustion, but has several advantages. It can be fired
at lower flue gas recycle ratio; it can capture sulphur in situ; and can co-fire biomass.
CanmetENERGY-Ottawa has been working on this technology since 2006, using a
75 kW th CFBC facility with full flue gas recycle and has obtained very positive results
(5, 6). Eriksson et al. (7) have also reported on their initial oxy-fuel CFBC results in
2007 using a similar facility to that at CanmetENERGY and their results also confirm
the same advantages with the technology. At this point the technology is receiving
attention in Canada (5, 6), Finland (7), Poland (8), China (9), USA (10) and Spain,
where a 20 MW th demonstration oxy-fuel CFBC plant is being built (11), among other
countries.
In order to advance studies in this area, a 0.8 MW th CFBC unit at CanmetENERGY

has been retrofitted for oxy-fuel research. The facility is used to simulate commercial
oxy-fuel CFBC performance. The modifications included adding oxygen supply, flue
gas recycle train, airtight fly ash discharge, flue gas compressor for baghouse
pulsing and system purge, etc., as well as upgrading the control and instrumentation
for oxy-firing. This paper describes the pilot oxy-fuel CFBC plant and initial results
obtained during the commissioning of the unit.
CanmentENERGY’s 0.8 MWth OXY-FUEL CFBC

The 0.8 MW th pilot-scale CFBC research facility at CanmetENERGY was built in the
1990s to generate a database useful for the design and process optimization of full-
scale units, study emissions of pollutants and predict the combustion performance of
feed stocks. The main components of the facility comprise the refractory-lined
combustor and cyclone, an inclined L-valve, four retractable bayonet-type cooling
tubes, flue gas cooler, baghouse, fuel and sorbent feed system, stack and air supply
system. The combustor has an inside diameter of 0.406 m and an internal height of
6.5 m. The CFBC has comprehensive instrumentation, control and data acquisition
systems and is also equipped with an 0.5 MW start-up burner fired with natural gas
to preheat the unit as well as to provide an additional heat source if needed.
Modifications to the pilot-scale CFBC began in 2007 for oxy-fuel CFBC research.
Oxygen supply and flue gas recycle were installed, and much work related to
preventing leakage throughout the entire plant has been undertaken. The oxy-fuel
CFBC is shown schematically in Fig. 1. Components shown in red are the existing
parts, and components shown in blue are the new additions. The primary fluidizing
gas, secondary gas and loop gas are all supplied from the main gas header. The
supply pressure of the main gas header is typically maintained at 55 kPag.
Secondary gas may be introduced into the combustor at up to 5 different locations
along the height of the combustor. The positions of these inlets are at 765 mm,
1549 mm, 2159 mm, 2769 mm and 4521 mm above the distributor.
Figure 1. CanmetENERGY 0.8 MW th oxy-fuel CFBC research facility
The recycled flue gas is controlled using a Tuthill Competitor GT series tri-lobe
blower capable of delivering up to 800 kg/h of recycled flue gas through the main air
header at a discharge pressure of 55 kPa. The flow, temperature and header
pressure of recycled flue gas are measured and logged. Oxygen is added to the
main header after the loop seal gas header. Oxidant level in the gas header can be
brought up to 29% oxygen (vol. wet basis). Oxidant level in the main air header is
measured with a Siemens Oxymat 61. The Oxymat 61 measures oxygen using the
paramagnetic alternating pressure method. Both the primary and secondary gases
have the same oxidant level at the present time. A planned upgrade will see a
second oxygen train installed, allowing the primary and secondary fluidizing gases to
be operated at different oxygen levels if desired.
Oxygen for the enrichment of the recycled flue gas is provided from a Linde-supplied
1500 US gal. bulk liquid oxygen tank. The oxygen is vaporized and brought to the
pilot facility at 50 psig. The maximum design flow of oxygen using this system is 220
kg/h. Isolation between the air system and recycle gas system is achieved using two
pneumatically actuated proportionate slide gate valves.
The fuel feeding system is comprised of a fuel storage bin, vibratory bin dispenser
and belt-type gravimetric weigh feeder. The maximum feed rate of the weigh feeder
is 342 kg/h with a 20:1 turndown ratio.
The sorbent feeding system has a similar arrangement as the fuel system.
Maximum sorbent feed rate is 64.8 kg/h.
The combustor is equipped with four bayonet cooling tubes that can be inserted or
raised during operation. Each bayonet tube is 7160 mm in length and is fabricated
with a 30 mm schedule 40 outer tube and a 16 mm 18 BWG inner tube (both
304SS). The bayonet tubes were designed for a total heat duty of 546 kW with a
water flow rate of 217 L/min.
Fly ash removal is accomplished with a negative pressure fabric filter dust collector
with a pulse jet bag cleaning system. The dust collector uses Nomex bags with
maximum temperature rating of 200C. The design gas volume is 0.59 Am3/s with a
normal operation inlet temperature of 177ºC and a dust loading of 48-79 g/Am3.
Ports are available for solid and gas sampling from the combustor. In addition,
CanmetENERGY has the equipment and trained staff for stack sampling of volatile
organic compounds (VOCs) and isokinetic sampling for semi-volatile organic
compounds (SVOCs), metals and polyaromatic hydrocarbons (PAHs) using US EPA
or Environment Canada standard sampling techniques.
Under air firing conditions, the pressure balance point is usually at the furnace exit.
Under oxy-fuel mode, the combustor is run under slightly positive pressure to
prevent air ingress. Some typical operating parameter ranges are shown in Table 1.
Table 1. Range of operating conditions

Input Range
Combustion temperature up to 980ºC
Heat input up to 0.8 MW th
Excess O2 2-10%
Ca/S molar ratio 0-3
Primary air 30-100%
Secondary air 0-70%
Loop seal air 1-5%
Superficial velocity 2-7 m/s
O2 in primary gas up to 29%
O2 in secondary gas up to 29%
Table 2. Fuel analysis, wt% (as analyzed)

Petroleum coke Anthracite
Proximate analysis
Moisture 0.63 8.3
Ash 0.48 30.7
Volatile 10.17 6.4
Fixed carbon 88.72
Ultimate analysis
Carbon 86.84 54.6
Hydrogen 3.42 1.7
Nitrogen 1.48 0.9
Sulphur 5.61 1.0
Oxygen (diff) 1.59 2.8
LHV, MJ/kg 32.46 19.89
COMMISSIONING TESTS
Bituminous coal, lignite, petroleum coke and anthracite were all used in the
commissioning tests. Table 2 gives analysis of some of the fuels. Limestone was
not used in the first several tests since the primary goal was to first obtain the
desired CO2 levels in the flue gas. In later tests, Calpo limestone (98.6% CaCO3)
from Canada was used.
The first several tests under oxy-fuel mode revealed that transition from air firing to
oxy-fuel firing was quick and smooth. The transition took less than 30 min to
complete. Combustion under oxy-fuel mode was stable. Transition from oxy-fuel to
air firing mode was faster. No operational difficulties were encountered. However,
CO2 concentrations in the flue gas were only about 50-60% in these initial tests.
Repeated efforts were made to seal the flue gas recycle train and all components
which are under negative pressure during oxy-fuel operation (baghouse, flue gas
cooler, etc.). It was a very difficult task. Once the system was properly sealed, CO2
concentration in the flue gas reached ~85%+ consistently in the following tests.
Figures 2 and 3 show the first successful oxy-fuel test in the 0.8 MW th CFBC unit
firing Pine Bend coke. CO2 concentration remained at ~90% for the entire duration
of the oxy-fuel firing period. Temperature distribution along the axis of the
combustor was similar to that of air firing with the same fuel. Figure 2 shows the
transition from air to oxy-fuel firing was completed in about 30 min, and the transition
from oxy-fuel to air firing was very fast indeed. Figure 3 shows the concentrations of
SO2 and CO. Note the SO2 concentration was over the range of the SO2 analyzer
(1.5%) during oxy-fuel firing conditions. Later a new analyzer with a much higher
range was purchased and installed. CO concentration was about the same for both
air firing and oxy-fuel firing periods. The increase of CO at time 16+ h was
apparently caused by the decrease of oxygen concentration as shown in Fig. 2.
100
90 CO2
80 O2
70
Concentration, %
60
50
40
30
20
10
0
10 11 12 13 14 15 16 17 18
time, hour
Figure 2. Oxy-fuel combustion of Pine Bend coke. Note the transition from air firing
to oxy-fuel mode in about 30 min.
14000
SO2
12000 CO
10000
Concentration, ppm
8000
6000
4000
2000
0
10 11 12 13 14 15 16 17 18
time, hour
Figure 3. SO2 and CO concentrations during oxy-fuel combustion of Pine Bend coke.
As the commissioning process progressed, a full week test using anthracite with
limestone addition was carried out. Figure 4 shows CO2 and O2 concentrations for
the entire duration of the test.
100
90
CO2
80
O2
70
60
CO 2, %
50
40
30
20
10
0
0.5 1 1.5 2 2.5 3 3.5 4 4.5
Time , day
Figure 4. Oxy-fuel CFBC combustion of anthracite.
Results shown in Fig. 4 and Table 3 demonstrate that the retrofitted 0.8 MW th oxy-
fuel CFBC unit was reliable. It was extremely stable during operation. This test
proved it can be run continuously for long periods of time under oxy-fuel CFBC
conditions to generate useful data for industrial purposes. It should be noted that
since the pilot CFBC does not have an ash cooler (external or integrated) in the
return loop, the recycle ratio was higher, at 70.7%. Fuel nitrogen to NO was low,
1.13% under oxy-fuel conditions. However, it is in line with our earlier results on the
much smaller 10 cm (75 kW th) oxy-fuel mini-CFBC plant (5, 6). Sulphur capture was
poorer than would be expected based on experience with air firing. This poor
performance may also have been exacerbated by the fact that the limestone used
was too fine. It is of interest that Scala and Salatino (12) also noted a lower degree
of sulphation in batch tests carried out in a 40 mm ID oxy-fired bubbling bed reactor,
which they relate to the well known phenomenon that direct sulphation is slower than
indirect sulphation until conversions reach a level around 30-40% (13). However, a
complicating factor is that all comparative evidence for this difference has been
developed using TGA and differential reactors using dry gas mixtures (14).
However, while it is recognized that direct sulphation is influenced by water (15), the
assumption that indirect sulphation is not itself strongly influenced by water is not
well founded (16). Therefore, while sulphation in oxy-fuel FBC systems needs further
study, the evidence for the superiority of conversions achieved by direct sulphation,
for longer sulphation periods is not supported by these results, and needs to be
reassessed with tests carried out with water levels typical of combustion (10-20%).
Table 3. Oxy-fuel CFBC combustion of anthracite at nominal temperature of 900C

Anthracite
Average freeboard temperature, C 905.5 ± 37
Fuel, kg/h 96.5 ± 1.4
Limestone, kg/h 9.5 ± 1
Oxygen, kg/h 138.7 ± 4
Nominal Ca/S 3
O2, % 3.85 ± 0.55
CO2, % 86.9 ± 0.6
CO, ppm 1143 ± 300
SO2, ppm 2628 ± 592
NO, ppm 108.4 ± 14
Superficial velocity in riser, m/s 5.9±0.4

Recycle ratio, % 70.7 ± 5
Sulphur capture, % 43.8 ± 4
Fuel N to NO, % 1.13 ± 0.1
CONCLUSIONS
A 0.8 MW th pilot-scale CFBC unit at CanmetENERGY had been successfully
retrofitted for oxy-fuel CFBC research. The unit can fire a wide range of fuels
including coal, petroleum coke and lignite. The operation of oxy-fuel CFBC was
stable and reliable. Transition from air firing to oxy-fuel firing was fast and smooth.
CO2 concentrations in the flue gas reached 85%+ during the entire oxy-fuel firing
period. NO emissions were extremely low with only 1.13% fuel nitrogen converted to
NO. Sulphur capture was poorer in the initial series of commissioning tests. Part of
the reason may have been that the limestone used was too fine.
REFERENCES
1. Buhre, B.J.P., Elliot, L.K., Sheng, C.D, Gupta, R.P., Wall T.F., Oxy-fuel
Combustion Technology for Coal-Fired Power Generation, Progress in Energy and
Combustion Science 31 (2005) 283-307.
2. Wall, T., Liu, Y., Spero, C., Elliott, L., Khare, S., Rathnam, R., et al., An overview
on oxyfuel coal combustion--State of the art research and technology development,
Chemical Engineering Research and Design 87 (2009) 1003-1016.
3. Toftegaard, M.B., Brix, J., Jensen, P.A., Glarborg, P., Jensen, A.D., Oxyfuel
combustion of solid fuels, Progress in Energy and Combustion Science 36 (2010)
581-625.
4. Vattenfall CCS Newsletter, http://www.vattenfall.com/en/ccs/pilot-plant.htm
5. Jia, L., Tan, Y., Anthony, E.J., Emissions of SO2 and NOx during Oxy-Fuel CFB
Combustion Tests in a Mini-Circulating Fluidized Bed Combustion Reactor, Energy &
Fuels 24 (2009) 910-915.
6. Jia, L., Tan, Y., Wang, C., Anthony, E.J., Experimental Study of Oxyfuel
Combustion and Sulfur Capture in a Mini-CFBC, Energy & Fuels 21 (2007) 3160-
3164.
7. Eriksson, T., Sippu, O., Hotta, A., Myohanen, K., Hyppanen, T., Pikkarainend, T.,
Oxy-fuel CFB Boiler as a Route to Near Zero CO2 Emission Coal Firing, Power
Generation Europe, Madrid, Spain, June 26-28, 2007.
8. Czakiert, T., Bis, Z., Muskala, W., Nowak, W., Fuel conversion from oxy-fuel
combustion in a circulating fluidized bed, Fuel Processing Technology 87 (2006)
531-538.
9. Fang, M., Yang, L., Mao, Y., Luo, Z., Cen, K., Experimental Study on O2/CO2
Combustion in a CFB Test Facility, 2007 International Conference on Coal Science
and Technology, Nottingham, United Kingdom, August 28-31, 2007.
10. Victor, R., Bonaquist, D., Shah, M., Hack, H., Wagner, D., Leathers, D., Kulig, S.,
The Jamestown Oxy-Coal Project, Power-Gen International 2008, Orlando, Florida,
December 2-4, 2008.
11. http://www.fwc.com/publications/pdf/PowerNews_Q42007.pdf
12. Scala, F., Salatino, P., Flue Gas Desulfurization under Simulated Oxyfiring
Fluidized Bed Combustion Conditions: The Influence of Limestone Attrition and
Fragmentation, Chemical Engineering Science 65 (2010) 556-561.
13. Chen, C., Zhao, C., Liu, S., Wang, C., Direct Sulfation of Limestone Based on
Oxy-Fuel Combustion Technology, Environmental Engineering Science 26 (2008)
1481-1487.
14. Hu, G., Dam-Johansen, K., Wedel, S., Hansen, J.P., Review of the Direct
Sulphation Reaction of Limestone, Progress in Energy and Combustion Science 32
(2006) 386-407.
15. Hu, G., Dam-Johansen, K., Wedel, S., Hansen, J.P. Direct Sulfation of
Limestone, AIChE Journal 53 (2007) 948-960.
16. Wang, C., Jia, L., Tan, Y., Anthony, E.J., The Effect of Water on Sulphation of
Limestone, Fuel 89 (2010) 2628-2632.
A NEW APPROACH FOR MODELING OF A FLUIDIZED BED
BY CFD-DEM
S. Karimi1, H. Chizari2, N. Mostoufi*1, R. Sotudeh-Gharebagh1

1
Process Design and Simulation Research Center, Department of Chemical
Engineering, Universityof Tehran, P.O. Box 11155/4563, Tehran, Iran
2
Department of Mechanical Engineering, Universityof Tehran, Tehran, Iran
* Corresponding author, Tel.: (+98-21)6696-7797, Fax: (+98-21)6646-1024,
E mail: mostoufi@ut.ac.ir
ABSTRACT
Numerical studies of 3D cylindrical fluidized bed by means of combined
computational fluid dynamics (CFD) and discrete element method (DEM) were
carried out. For motion of particles, Newton's second law and 3D compressible
Navier-Stokes equations in generalized curvilinear coordinates in its conservative
form were used. Navier-Stokes equations were solved with high order compact finite
difference scheme by fully implicit flux decomposition method. Non-reflecting
boundary conditions (NRBC) were used for the outflow boundary. The convergence
of this method, especially at high Reynolds number, is significantly better than the
SIMPLE method.
INTRODUCTION
Gas-solid fluidized beds have been widely utilized as reactors in the chemical and
petrochemical industries. Successful design and operation of fluidized bed reactors
requires proper prediction of the performance of reactor. Whereas experiment
studies in these systems are quite tedious and expensive, recently modeling of
fluidized bed reactors has been extensively used to study these systems.
Mathematical models for modeling fluidized bed reactors can be grouped into two
main categories: Eulerian-Eulerian (EE) and Lagrangian-Eulerian (LE) .In the EE
model, both particles and gas phase are considered as a continuum phase (1, 2, 3
4). Recently, many researchers (5, 6) have adopted the LE model, which is also
called discrete element method (DEM), for modeling the phenomena in particle-fluid
systems. Using this model, trajectories of individual particles can be traced by
solving Newton's second law for each particle while the flow of gas, which is treated
as a continuum phase, is described by Navier-Stokes equation.
Finite volume method is usually used to solve the Navier-Stokes equation. The
SIMPLE method with staggered grid is suitable for solving Navier-Stokes equation.
However, using this method of solution for problems with high Reynolds number is
typically unstable. Furthermore, implementing the high order SIMPLE method is so
difficult in comparison with finite difference schemes. One of the finite difference
methods that can be used for high Reynolds flow is the flux decomposition method.
In this method, convective fluxes are decomposed based on eigenvalues which
results in a better agreement with the physical properties of the fluid, especially at
high Reynolds numbers.
1
Although the LE approach is more appropriate to study the hydrodynamics of
fluidized beds. This model requires large computational resources for large scale
𝐿
systems ( > 4.4𝑅𝑒1/6 must be chosen to prevent wave reflection). In recent years,
𝐷
non-reflecting boundary conditions (NRBC) were used by some researchers (7, 8) to
mitigate wave reflection problems. The concept of NRBC was proposed by
Thompson (9) where the idea of specifying the boundary conditions according to the
inward and outward propagating waves was introduced. Thompson showing that
wave reflections, and therefore, can be used as a fictitious boundary. By using this
boundary condition, computational domain and computational time for solving
Navier-Stokes equation is decreased. The amount of time saving depends on the
gas inlet velocity. As the gas inlet velocity increases the free domain which is
required for particles motion increase and therefore the effect of NRBS reduces. But
using NRBS almost half the computational time decreases.
In the present work, a CFD-DEM technique was used to investigate the

hydrodynamics of a 3D cylindrical fluidized bed. Newton's second law and 3D
compressible Navier-Stokes equation in generalized curvilinear coordinates in
conservative form was solved for particle and gas phase respectively. In spite of
previous studies that usually used SIMPLE method for solving Navier-Stokes
equations, these equations were solved with high order compact finite difference
scheme by fully implicit flux decomposition method. Using curvilinear coordinates,
the physical domain was changed from cylindrical to semi-Cartesian coordinates in
computational domain. Furthermore, NRBC was used for outflow boundary to reduce
computation time. Hydrodynamics of the bed was investigated and the results were
in good agreement with the expected behavior of gas and solids in the fluidized bed.
Governing equations
Equation of motion
In the present work, the flow of sphere particles in a 3D cylindrical fluidized bed was
investigated. Newton’s second law was applied to each particle. The translational
and rotational motion of the particles can be described by following equations (10):
𝑘𝑖
𝑑𝑉𝑖
𝑚𝑖 = = 𝑓𝑓,𝑖 + ��𝑓𝑐,𝑖𝑗 + 𝑓𝑑,𝑖𝑗 � + 𝑓𝑔,𝑖 (1)
𝑑𝑡
𝑗=1
𝑘𝑖
𝑑𝜔𝑖
𝐼𝑖 = � 𝑇𝑖,𝑗 (2)
𝑑𝑡
𝑗=1
Soft sphere method (11) was used for simulation Inter-particle and particle-wall
U U
contact forces.
For the gas phase, three-dimensional compressible Navier-Stokes equations in

generalized curvilinear coordinates (𝜉, 𝜂, 𝜁 )were written in conservative form:
𝜕𝜀𝑄 𝜕(𝐸 − 𝐸𝑣 ) 𝜕(𝐹 − 𝐹𝑣 ) 𝜕(𝐺 − 𝐺𝑣 ) (3)
+ + + =𝑃
𝜕𝑡 𝜕𝜉 𝜕𝜂 𝜕𝜁
2
𝜌 𝜌𝑈𝜀 𝜌𝑉𝜀
𝜌𝑢 𝜌𝑈𝑢𝜀 + 𝑃𝜉𝑥 𝜌𝑉𝑢𝜀 + 𝑃𝜂𝑥
1⎛ ⎞ 1⎛ ⎞ 1⎛ ⎞
𝑄 = ⎜ 𝜌𝑣 ⎟ 𝐸= ⎜ 𝜌𝑈𝑣𝜀 + 𝑃𝜉𝑦 ⎟ 𝐹= ⎜ 𝜌𝑉𝑣𝜀 + 𝑃𝜂𝑦 ⎟
𝐽 𝜌𝑤 𝐽 𝐽 𝜌𝑉𝑤𝜀 + 𝑃𝜂𝑧
𝜌𝑈𝑤𝜀 + 𝑃𝜉𝑧
⎝ 𝐸𝑡 ⎠ ⎝𝑈(𝐸𝑡 + 𝑃)𝜀 + 𝑈𝑃 𝑃 (1 − 𝜀 )⎠ ⎝𝑉 (𝐸𝑡 + 𝑃)𝜀 + 𝑉𝑃 𝑃(1 − 𝜀 )⎠
𝜌𝑊𝜀 0
𝜌𝑊𝑢𝜀 + 𝑃𝜁𝑥 𝜀�𝜏 𝑥𝑥 𝜉𝑥 + 𝜏 𝑥𝑦 𝜉𝑦 + 𝜏𝑥𝑧 𝜉𝑧 �
1⎛ ⎞ 1⎛ ⎞
𝐺= ⎜ 𝜌𝑊𝑣𝜀 + 𝑃𝜁𝑦 ⎟ 𝐸𝑣 = ⎜ 𝜀�𝜏 𝑦𝑥 𝜉𝑥 + 𝜏 𝑦𝑦 𝜉𝑦 + 𝜏 𝑦𝑧 𝜉𝑧 � ⎟
𝐽 𝐽⎜ ⎟
𝜌𝑊𝑤𝜀 + 𝑃𝜁𝑧 𝜀�𝜏𝑧𝑥 𝜉𝑥 + 𝜏𝑧𝑦 𝜉𝑦 + 𝜏𝑧𝑧 𝜉𝑧 �
⎝𝑊 (𝐸𝑡 + 𝑃)𝜀 + 𝑊𝑃 𝑃 (1 − 𝜀 )⎠ ⎝ 𝑄𝑥 𝜉𝑥 + 𝑄𝑦 𝜉𝑦 + 𝑄𝑧 𝜉𝑧 ⎠
0 0
𝜀�𝜏𝑥𝑥 𝜂𝑥 + 𝜏𝑥𝑦 𝜂𝑦 + 𝜏𝑥𝑧 𝜂𝑧 � 𝜀�𝜏𝑥𝑥 𝜁𝑥 + 𝜏𝑥𝑦 𝜁𝑦 + 𝜏𝑥𝑧 𝜁𝑧 �
1⎛ ⎞ 1⎛ ⎞
𝐹𝑣 = ⎜ 𝜀�𝜏 𝜂
𝑦𝑥 𝑥 + 𝜏 𝜂
𝑦𝑦 𝑦 + 𝜏 𝜂
𝑦𝑧 𝑧 �⎟ 𝐺𝑣 = ⎜ 𝜀�𝜏 𝜁
𝑦𝑥 𝑥 + 𝜏 𝜁
𝑦𝑦 𝑦 + 𝜏 𝜁
𝑦𝑧 𝑧 ⎟� (4)
𝐽⎜ ⎟ 𝐽⎜ ⎟
𝜀�𝜏𝑧𝑥 𝜂𝑥 + 𝜏𝑧𝑦 𝜂𝑦 + 𝜏𝑧𝑧 𝜂𝑧 � 𝜀�𝜏𝑧𝑥 𝜁𝑥 + 𝜏𝑧𝑦 𝜁𝑦 + 𝜏𝑧𝑧 𝜁𝑧 �
⎝ 𝑄𝑥 𝜂𝑥 + 𝑄𝑦 𝜂𝑦 + 𝑄𝑧 𝜂𝑧 ⎠ ⎝ 𝑄𝑥 𝜁𝑥 + 𝑄𝑦 𝜁𝑦 + 𝑄𝑧 𝜁𝑧 ⎠
0
𝑆1 𝐹𝜉
1⎛ 𝑆1 𝐹𝜂
⎞ 𝐿∞ 𝐿∞
𝑃= ⎜ ⎜ ⎟
⎟ , 𝑆1 = 2 , 𝑆2 = ,
𝐽 𝑆1 𝐹𝜁 𝜌∞ 𝑈∞ 𝜌∞ 𝑈∞3
⎝𝑆2 �𝐹𝜉 𝑈𝑃 + 𝐹𝜂 𝑉𝑃 + 𝐹𝜁 𝑊𝑃 � + 𝑆2 𝑄𝑃 ⎠
The contra-variant velocity components 𝑈, 𝑉, and 𝑊 are defined as:

𝑈 = 𝑢𝜉𝑥 + 𝑣𝜉𝑦 + 𝑤𝜉𝑧 , 𝑉 = 𝑢𝜂𝑥 + 𝑣𝜂𝑦 + 𝑤𝜂𝑧 , 𝑊 = 𝑢𝜁𝑥 + 𝑣𝜁𝑦 + 𝑤𝜁𝑧 , (5)
Other equations used in Navier-Stokes equations are introduced as follow:

𝑄𝑥 = −𝑞𝑥 + 𝜀�𝑢𝜏𝑥𝑥 + 𝑣𝜏𝑥𝑦 + 𝑤𝜏𝑥𝑧 �
�𝑄𝑦 = −𝑞𝑦 + 𝜀�𝑢𝜏𝑦𝑥 + 𝑣𝜏𝑦𝑦 + 𝑤𝜏𝑦𝑧 � (6)
𝑄𝑧 = −𝑞𝑧 + 𝜀�𝑢𝜏𝑧𝑥 + 𝑣𝜏𝑧𝑦 + 𝑤𝜏𝑧𝑧 �
1 𝑁𝑢 × 𝑘�
𝑄𝑃 = � ℎ(4𝜋𝑟𝑃2 )�𝑇𝑃 − 𝑇�� , 𝑇� = 𝑇 × 𝑇∞ , ℎ= , 𝑘� = 𝑘 × 𝑘∞ , (7)
𝑉𝑐𝑒𝑙𝑙 2𝑟𝑃
𝐹𝑥 𝜉𝑥 + 𝐹𝑦 𝜉𝑦 + 𝐹𝑧 𝜉𝑧 𝐹𝑥 𝜂𝑥 + 𝐹𝑦 𝜂𝑦 + 𝐹𝑧 𝜂𝑧 𝐹𝑥 𝜁𝑥 + 𝐹𝑦 𝜁𝑦 + 𝐹𝑧 𝜁𝑧
𝐹𝜉 = , 𝐹𝜂 = 𝐹𝜁 =
(8)
�𝜉𝑥2 + 𝜉𝑦2 + 𝜉𝑧2 �𝜂𝑥2 + 𝜂𝑦2 + 𝜂𝑧2 �𝜁𝑥2 + 𝜁𝑦2 + 𝜁𝑧2
𝜇 𝜕𝑢𝑖 𝜕𝑢𝑗 2 𝜕𝑢𝑘 𝑘𝑒𝑓𝑓 𝜕𝑇
𝜏𝑖𝑗 = �� + � − 𝛿𝑖𝑗 �, 𝑞𝑖 = − 2 (9)
𝑅𝑒 𝜕𝑥𝑗 𝜕𝑥𝑖 3 𝜕𝑥𝑘 𝑅𝑒𝑀𝑟 𝑃𝑟(𝛾 − 1) 𝜕𝑥𝑖
𝑘�𝜀 + 𝑘�𝑃 (1 − 𝜀 )
𝑘𝑒𝑓𝑓 = (10)
𝑘∞
For solving Navier-Stokes equations with flux decomposition method, first the
Jacobean matrices must be evaluated:
𝜕𝐸𝑖 𝜕𝐹𝑖 𝜕𝐺𝑖
𝐴𝑖𝑗 = , 𝐵𝑖𝑗 = , 𝐶𝑖𝑗 = (11)
𝜕𝑄𝑗 𝜕𝑄𝑗 𝜕𝑄𝑗
3
By considering𝑄 𝑛+1 = 𝑄𝑝 + 𝛿𝑄𝑝 Navier-Stokes equations are changed to:
𝑛+1 �
𝜕𝑄 𝑛+1 𝑛+1
𝜕𝜀 𝑛+1 𝜕𝐴 𝑝 𝜕𝐵 𝑝 𝜕𝐶 𝑝
𝜀 � +𝑄 � � + 𝛿𝑄 + 𝛿𝑄 + 𝛿𝑄
𝜕𝑡 𝜕𝑡 𝜕𝜉 𝜕𝜂 𝜕𝜁
(12)
𝜕𝐸𝑣 𝜕𝐹𝑣 𝜕𝐺𝑣 𝑛 𝜕𝐸 𝜕𝐹 𝜕𝐺 𝑛
= 𝑃𝑛 + � + + � −� + + �
𝜕𝜉 𝜕𝜂 𝜕𝜁 𝜕𝜉 𝜕𝜂 𝜕𝜁
The Jacobean matrices are decomposed using eigenvalues (𝜆):

1
𝐴 = 𝐴+ + 𝐴− 𝐴± = (𝐴 ± 𝜆𝐼) (13)
2
𝜕𝐴+ 𝜕𝐴−
= 𝐴+ +
𝑖,𝑗,𝑘 − 𝐴𝑖−1,𝑗,𝑘 , = 𝐴− −
𝑖+1,𝑗,𝑘 − 𝐴𝑖,𝑗,𝑘 (14)
𝜕𝜉 𝜕𝜉
Finally, flow field obtain by solving following equation:

2∆𝑡 𝜕𝐴 𝜕𝐵 𝜕𝐶
�𝐼 + 𝑛+1 𝑛 𝑛−1
� + + �� 𝛿𝑄𝑝 = 𝑅𝑖𝑚𝑝
6𝜀 − 4𝜀 + 𝜀 𝜕𝜉 𝜕𝜂 𝜕𝜁
𝜀 𝑛+1 (3𝑄𝑝 − 4𝑄𝑛 + 𝑄𝑛−1 ) + 𝑄𝑝 (3𝜀 𝑛+1 − 4𝜀 𝑛 + 𝜀 𝑛−1 )
𝑅𝑖𝑚𝑝 = −
6𝜀 𝑛+1 − 4𝜀 𝑛 + 𝜀 𝑛−1
2∆𝑡 𝜕(𝐸 − 𝐸𝑣 ) 𝜕(𝐹 − 𝐹𝑣 ) 𝜕(𝐺 − 𝐺𝑣 ) (15)
− 𝑛+1 � + + �
6𝜀 − 4𝜀 𝑛 + 𝜀 𝑛−1 𝜕𝜉 𝜕𝜂 𝜕𝜁
2∆𝑡
+ 𝑛+1 𝑃
6𝜀 − 4𝜀 𝑛 + 𝜀 𝑛−1
NON-REFLECTING BOUNDARY CONDITIONS

If 𝑄 is the conservative variable,𝑞 is the primitive variable and 𝑀 is the conversion
matrix as below:
1 0 0 0 0
𝑢 𝜌 0 0 0 𝜌
⎛ ⎞ 𝑢
𝜕𝑄 𝑣 0 𝜌 0 0
𝑀= =⎜ ⎟ ⎛𝑣⎞
𝜕𝑞 ⎜ 𝑤 0 0 𝜌 0 ⎟, 𝑞 = (16)
𝑤
1 2 1 ⎝𝑃⎠
(𝑢 + 𝑣 2 + 𝑤 2 ) 𝜌𝑢 𝜌𝑣 𝜌𝑤
⎝2 𝛾 − 1⎠
NRBC in the 𝜉-direction in conservative form can be written as

𝜕𝑄 𝜕𝑞 𝜕𝑞
+ 𝐷𝑖 + 𝑀𝑏� + 𝑀𝑐̿ = 𝐽𝑅𝑣 (17)
𝜕𝑡 𝜕𝜂 𝜕𝜁
where
𝑉 𝜌𝜂𝑥 𝜌𝜂𝑦 𝜌𝜂𝑧 0 𝑊 𝜌𝜁𝑥 𝜌𝜁𝑦 𝜌𝜁𝑧 0
𝜂𝑥 ⎛0 𝜁𝑥 ⎞
⎛0 𝑉 0 0 ⎞ 𝑊 0 0
⎜ 𝜌 ⎟ ⎜ 𝜌⎟
⎜ 𝜂𝑦 ⎟ ⎜ 𝜁𝑦 ⎟
𝑏� = ⎜ 0 0 𝑉 0 ⎟ , 𝑐̿ = ⎜ 0 0 𝑊 0 (18)
𝜌 𝜌⎟
⎜ 𝜂𝑧 ⎟ ⎜ ⎟
⎜0 0 0 𝑉 ⎟ 𝜁𝑧
⎜0 0 0 𝑊 ⎟
𝜌 𝜌
⎝0 𝛾𝑃𝜂𝑥 𝛾𝑃𝜂𝑦 𝛾𝑃𝜂𝑧 𝑉⎠ ⎝0 𝛾𝑃𝜁𝑥 𝛾𝑃𝜁𝑦 𝛾𝑃𝜁𝑧 𝑊⎠
4
𝑑1
𝐷1 𝑢𝑑1 + 𝜌𝑑2
⎛ ⎞
⎛𝐷2 ⎞ ⎜ 𝑣𝑑1 + 𝜌𝑑3 ⎟
𝐷
𝐷 = 𝑀𝑑 = ⎜ 3 ⎟ = ⎜ ⎟ (19)
⎜ 𝑤𝑑1 + 𝜌𝑑4 ⎟
𝐷4
1 2 𝑑5
⎝𝐷5 ⎠ 2 2
(𝑢 + 𝑣 + 𝑤 )𝑑1 + 𝜌𝑢𝑑2 + 𝜌𝑣𝑑3 + 𝜌𝑤𝑑4 +
⎝2 𝛾 − 1⎠
𝜌
𝜉̃𝑥 𝐿1 + 𝜉̃𝑦 𝐿2 + 𝜉̃𝑧 𝐿3 + (𝐿 4 + 𝐿 5 )
⎛ √2𝑐 ⎞
⎜ 𝜉̃𝑥
𝑑1 −𝜉̃𝑧 𝐿2 + 𝜉̃𝑦 𝐿3 + (𝐿4 − 𝐿5 ) ⎟
⎜ √2 ⎟
𝑑 ⎜ ⎟
⎛ 2⎞ 𝜉̃𝑦
𝑑 = 𝑃𝐿 = ⎜𝑑3 ⎟ = ⎜ ̃ ̃
𝜉𝑧 𝐿1 − 𝜉𝑥 𝐿3 + (𝐿4 − 𝐿5 ) ⎟ (20)
𝑑4 ⎜ √2 ⎟
⎜ ̃
𝜉𝑧 ⎟
⎝𝑑5 ⎠ ⎜
−𝜉̃𝑦 𝐿1 + 𝜉̃𝑥 𝐿2 + (𝐿4 − 𝐿5 ) ⎟
⎜ √2 ⎟
𝜌𝑐
(𝐿 4 + 𝐿 5 )
⎝ √2 ⎠
𝜕𝜌 𝜕𝑣 𝜕𝑤 𝜉̃𝑥 𝜕𝑃
𝑈 �𝜉̃𝑥 + 𝜉̃𝑧 − 𝜉̃𝑦 − �
⎛ 𝜕𝜉 𝜕𝜉 𝜕𝜉 𝑐 2 𝜕𝜉 ⎞
⎜ 𝜕𝜌 𝜕𝑢 𝜕𝑤 𝜉̃𝑦 𝜕𝑃 ⎟
⎜ 𝑈 �𝜉̃𝑦 − 𝜉̃𝑧 + 𝜉̃𝑥 − 2 � ⎟
𝐿1 𝜕𝜉 𝜕𝜉 𝜕𝜉 𝑐 𝜕𝜉
⎜ ⎟
⎛𝐿 2 ⎞ ⎜ 𝜕𝜌 𝜕𝑢 𝜕𝑣 𝜉̃𝑧 𝜕𝑃 ⎟
𝐿 = ⎜𝐿 3 ⎟ = ⎜ 𝑈 �𝜉̃𝑧 + 𝜉̃𝑦 − 𝜉̃𝑥 − 2 � ⎟ (21)
𝜕𝜉 𝜕𝜉 𝜕𝜉 𝑐 𝜕𝜉
𝐿4 ⎜ ⎟
̃ ̃ ̃
⎝𝐿5 ⎠ ⎜ (𝑈 + 𝐶 ) � 𝜉𝑥 𝜕𝑢 + 𝜉𝑦 𝜕𝑣 + 𝜉𝑧 𝜕𝑤 + 1 𝜕𝑃� ⎟
⎜ √2 𝜕𝜉 √2 𝜕𝜉 √2 𝜕𝜉 √2𝜌𝑐 𝜕𝜉 ⎟
⎜ ⎟
𝜉̃𝑥 𝜕𝑢 𝜉̃𝑦 𝜕𝑣 𝜉̃𝑧 𝜕𝑤 1 𝜕𝑃
(𝑈 − 𝐶 ) �− − − + �
⎝ √2 𝜕𝜉 √2 𝜕𝜉 √2 𝜕𝜉 √2𝜌𝑐 𝜕𝜉 ⎠

In this numerical study, a cylindrical fluidized bed with 7.5 cm diameter and 50 cm
height, filled with 10000 particles was considered. The diameter and density of
particles were 2 mm and 1100 kg/m3, respectively. A jet of gas was introduced into
the bed via a central hole with jet velocity of 8 m/s (u~5umf).
Fig. 1 shows snapshots of particles positions in the bed. As can be seen in this
figure, particles that are at the center of the bed accelerate very fast and move
vertically in the bed. The initial acceleration of the particles is so high that they travel
almost 50 cm in the bed. This high acceleration is due to the high vertical drag force
exerted on particles due to high gas velocity in the central area of the bed. However,
particles in the annulus of this area do not move very noticeably in the vertical
direction. This is mainly due to the low gas velocity in this region. The gas velocity in
this region is low for two reasons. First, the gas is not introduced into the bed from
near the walls. Second, wall effects induce a velocity boundary layer in which the
gas velocity is low near the wall.
5
t= 0.1s t= 0.3s t=1s
Fig.1. Snapshot of particle motion
Over time by particles movement from distributor, the void fraction in that region
increase and the gas velocity decrees. Void fraction increasing in distributor center
is more than the distributor corner. So reduction in the gas velocity in the distributor
center holes is more than distributor corners. The gas velocity affects particles
motion that caused to occurring two peaks in particles motion. If the simulation has
been permitted to continue for a longer time, the transient state of the bed would
have been vanished and a better solid flow pattern would have been obtained. Since
the time required for the calculation is very high (around 1 month), this results has
not been obtained yet.
Fig. 2 shows velocity vector and density contour of the gas in the bed. The bed is
divided into four sections that are perpendicular to each other to able to show the
behavior of the flow field in 3D cylindrical bed. However, this figure shows only two
sections of the bed.
For low Mach number flows, changes in density are low, but as it can be seen in
these figures, with upcoming the particles the density of fluid before them increases.
Moreover, the velocity vectors in center of the cylinder are high. This flow pattern is
in accordance with a gas flow pattern in a cylinder with boundary layer. According to
the continuity relation, while the gas velocity increases, the density of gas
decreases. This result shows that the presented model and the implemented method
can predict compressibility behavior of the gas very well.
6
t = 0.1s t = 0.3 s t=1s
Fig.2.velocity vectors and density contour of gas
CONCLUSIONS
A combination of CFD and DEM was used to study the behavior of the high velocity
fluidized bed reactor. The conservative form of Navier-Stocks equations in
curvilinear coordinate was derived and used to obtain flow field of the gas in the bed.
As described before, flux decomposition method is more compatible with high
Reynolds numbers and high order solving methods than SIMPLE method; therefore
in this work flux decomposition method was used for modeling high Reynolds
fluidized bed. It must be emphasized that solving high order Navier-Stokes equations
caused to seeing the physical behavior of the bed much better.
NOTATION
d amount of wave for each primitive Navier-Stokes equation

D amount of wave for each conservative Navier-Stokes equations
E inviscid flux vector (𝜉 direction)
Ev viscous flux vector (𝜉 direction)
fc contact force, N
fd Damping force, N
ff particle-fluid interaction force, N
fg acceleration force, N
F inviscid flux vector (𝜂 direction)
7
Fv viscous flux vector (𝜂 direction)
G inviscid flux vector (𝜁 direction)
Gv viscous flux vector (𝜁 direction)
I moment of inertia, kg m2
J Jacobian of the coordinate transformation,
L amount of each characteristic wave
M conversion matrix
q vector of primitive variables
Q vector of conservative variables
U contra-variant velocity(x direction), m s-1
V contra-variant velocity(y direction) , m s-1
W contra-variant velocity(z direction) , m s-1
REFERENCES
1. D. Gidaspow, Y. C. Seo, B. Ettehadieh, Hydrodynamics of fluidization:
Experimental and theoretical bubble sizes in a two-dimensional bed with a jet,
Chemical Engineering Communication, 22,253-272, 1983.
2. J. A. M. Kuipers, K. J. vanDuin, F. P. H. van Beckum, W. P. M. van Swaaij,
Computer simulation of the hydrodynamics of a two-dimensional gas-fluidized
bed, Computer and Chemical Engineering, 17(8), 839-858,1993.
3. C. Guenther and M. Syamlal, The effect of numerical diffusion on simulation of
isolated bubbles in a gas-solid fluidized bed, Powder Technology,116, 142-154,
2001.
4. F. Gevrin, O. Masbernat, O. Simonin, Granular pressure and particle velocity
fluctuations prediction in liquid fluidized bed, Chemical Engineering Science, 63,
2450-2464, 2008.
5. H. P. Zhu, Z.Y. Zhou, R. Y. Yang, A. B. Yu, Discrete particle simulation of
particulate systems: a review of major application and findings, Chemical
Engineering Science, 63(23), 5728-5770, 2008.
6. M. Ye, M. A. van der Hoef, J. A. M. Kuipers, A numerical study of fluidization
behavior of Geldart A particles using a discrete particle model, Powder
Technology, 139, 129, 2003.
7. L. H. Jiang, Shan, C. Liu, M. Visbal, Non-Reflecting Boundary Conditions For
DNS in Curvilinear Coordinates, International Conference, Rutgers, New Jersey,
June 7-9.1999.
8. T. J. Poinsot, and S. K. Lele, Boundary Conditions for Direct Simulations of
Compressible Viscous Floes, Journal of Computational Physics, 101, 104-129,
1992.
9. K. W. Thompson, Time-Dependent Boundary Conditions for Hyperbolic Systems
II, Journal of Computational Physics, 89, 439-461, 1990.
10. B.H. Xu and A. B. Yu, Numerical simulation of the gas-solid flow in a fluidized
bed by combining discrete particle method with computational fluid dynamics,
Chemical Engineering Science, 52 (16), 2785-2809,1997.
11. P. A. Cundall and O. D. L. Strack, A discrete numerical model for granular
assemblies, Geotechnique, 29, 47-65, 1979.
8
THE RESEARCH OF CFB BOILER OPERATION
FOR OXYGEN-ENHANCED DRIED LIGNITE COMBUSTION
Waldemar Muskala, Jaroslaw Krzywanski, Tomasz Czakiert, Wojciech Nowak

Czestochowa University of Technology, Faculty of Environmental Protection
and Engineering
Dabrowskiego 73, 42-200 Czestochowa, Poland, tel./fax: +48 343250933
ABSTRACT
The paper presents the research of CFB boiler operation for oxygen-enhanced dried
lignite combustion. The combustion in oxygen-enhanced conditions generally leads
to reducing the emissions of CO and NOx and N2O due to reduced volume of flue
gas. The maximum oxygen content for oxygen-enhanced combustion in O2/N2
conditions should not exceed 60%, however, the maximum drying extent of fuel
should not be higher than 50% of the initial moisture content in an examined lignite.
INTRODUCTION
The technology of coal combustion in circulating fluidized bed (CFB) boilers and its
chemical and process engineering may be ranked among the technologies referred
to as clean combustion technologies including reduced emission of pollutants. Such
technologies are crucial as the most favorable conditions for the combustion of solid
fuels in oxygen-enhanced conditions appears to be the circulating fluidized bed. This
technology brings about a number of advantages such as reducing the pollutants
emission, increasing the effectiveness of CO2 separation from the flue gas owing to
higher CO2 content, decreasing the flue gas volume. The technical knowledge of an
operation of circulating fluidized bed boilers is still insufficient within the modeling
and simulation of the processes of combustion in such boilers. However, as this new
technology has been developing rapidly one may expect a lot of additional data from
experiments to appear concerning the operation of CFB boilers under such
conditions. The theoretical computations which have been carried out provide the
results that satisfactorily simulate the boiler operation parameters and some of those
parameters were possible to be determined during the operation of a real facility.
ASSUMPTIONS FOR THE MATHEMATICAL MODEL OF FUEL COMBUSTION IN

OXYGEN-ENHANCED CONDITIONS
The model consists of several sub-models which enables the description of crucial
processes associated with combustion of solid fuels under circulating fluidized bed
conditions. The model considers hydrodynamics of bed material, fuel devolatilization
stage, volatiles and char combustion, flue gas desulfurization as well as heat and
mass transfer. The core of the model was based on the fluidized bed coal
combustion model (1, 2). The structure was developed by adding additional data
from experiments on the combustion in oxygen-enhanced conditions (3-5). This
paper presents some computations and validations performed for an existing 670 t/h
CFB boiler operated at nominal load. The computing data refer to the boiler
operation taking into account the initial drying extent of fuel before it was fed to the
combustion chamber. The combustion is assumed to occur in oxygen enhanced
conditions within the range of 21-100% under O2/N2 and O2/CO2 conditions. The
simulation computations were carried out assuming the constant heat flux within fuel
fed to the boiler containing initially 43% of the moisture content and in the dried fuel
the moisture content being 30%, 20% and 10% respectively. Table 1. presents the
properties and fluxes of fuel in the CFB boiler depending on the drying extent of fuel.
Table 1. The properties of fuel depending on the drying extent of fuel

The flux of coal
Moisture [%] Carbon (c) [%] LHV [kJ/kg]
[kg/s]
43.5 28 10991.2 63.0
30 34.7 14214.7 48.7
20 39.6 16602.5 41.7
10 44.6 18990.3 36.5
Two different simulations of the boiler operation as well as the assumptions for the
mathematical model of fuel combustion in oxygen-enhanced conditions were
thoroughly analyzed in the passage referring to modeling of solid fuels combustion
under oxygen-enhanced conditions in circulating fluidized bed boiler (5). The
sorbent was also fed to the boiler. The sorbent volume is ms = 2.02 kg/s. The
simulation computations for two different boiler operations are presented taking into
account variations in the oxygen contents in the mixtures during coal combustion in
oxygen-enhanced conditions. The overall results are calculated using Runge-Kutta-
IV type Equation. After entering input data, determining the initial conditions and
convergence conditions, the computations of bed hydrodynamics and chemical
reactions are carried out. Distribution and concentrations of solids and gaseous
components concentrations in the whole volume of combustion chamber are
established on the basis of solids and gas balances. The physicochemical
properties of fuel are the average properties of lignite from the Turow Coal Mine,
combusted in fluidized- bed boilers in the Turow Power Plant in Poland. The
fluidizing reacting gases were O2/CO2 and O2/N2 mixtures with increased oxygen
content (zo2) The primary gas to the secondary gas ratio was 60/40 and the
secondary gas was supplied onto two levels: 0.75 and 1.25 m above the grid. In
order to retain the regime of the circulating fluidized bed with the variable oxygen
content in a supplied gas mixture, the modification of the overall dimensions of
combustion chamber is necessary. In a presented model, only one of the three
characteristic chamber dimensions , i.e. the chamber depth, was subjected to
changes that ranged from 9.9 m for zo2= 21% to 2.1 m for zo2 = 100%, which
corresponded to the reduction of the chamber volume to 33,6% of its initial volume.
It allows maintaining a constant gas velocity in the whole volume of combustion
chamber at a level of w=5.4 m/s.
COMPUTATION RESULTS AND THEIR ANALYSIS
The computational model served for the simulation and assessment of the
concentration in dry flue gas (Fig. 1 - 2) and (Fig. 3 - 4) their volume flux of CO, CO2
NO and N2O as a function of oxygen content in the inlet gas at the exit of the
combustion chamber during combustion. The obtained results presented in (Fig. 1)
show that the increase of the oxygen content leads to an increasing carbon dioxide
content from 15 % with 21 % of oxygen content in O 2/N2 mixture to about 98 %
during the oxy-combustion, whereas the CO content decreases (within 3 to 0,8 ppm)
thus reaching almost zero value. Similar results were reported by other researchers
(6) Decline in the moisture content (W r) of combusted fuel from 43% to 10 % causes
a slight increase of about 2-5 % of CO2 and CO contents in dry flue gas.
16 3,0
14
2,5
12
2,0
10
zCO [ppm]
zCO2 [%]
8
21 % O2 1,5
6
1,0
4 CO2
CO 0,5
2
0 0,0
5 15 25 35 45
Wr [%]
120 1,60
1,40
100
1,20
80
1,00
zCO [ppm]
zCO2 [%]
60 0,80
CO2
100 % O2 0,60
40 CO
0,40
20
0,20
0 0,00
5 15 25 35 45
Wr [%]
Fig.1. CO and CO2 concentration in dry flue gas as a function of moisture content in
fuel for different oxygen content in the inlet gas of O2/N2
Reduction of NOx and N2O concentration (Fig. 2) occurs as the moisture content in
the inlet gas decreases. For NOx the reduction is about 30%, from the value of about
110-140 ppm to 90-100 ppm regardless of the oxygen content in the mixtures of
O2/N2. Reduction of N2O concentration of about twice (that is from about 8 - 10 ppm
to 4 - 5 ppm) is noticed. Decline in moisture content in flue gas results in slight
increase of CO concentration in combustion chamber, which promote NOX
reduction.
Fig. 3 and Fig.4. show the comparison of CO2, CO, NO and NO2 flux in dry
flue gas as a function of oxygen content in the inlet gas for oxygen-enhanced
combustion in O2/N2 conditions. The CO2 and CO flux little depends on the drying
extent of solid fuel and its values are as follows: for CO2 from 1,3 to about 1,8
kmol/s and for CO within the range of 2,5 10-5 - 1,5 10-6 kmol/s. However, CO2 flux
increases whereas CO flux declines as a result of oxygen content increase in O2/N2
mixtures.
Fig.2. NO and N2O concentration in dry flue gas as a function of moisture content in
fuel for different oxygen content in the inlet gas of O2/N2
Decline of NOx and N2O flux (Fig.4) of about 40 % was found as a result of
decreasing moisture content in fuel from 43 to 10 %. Decline of N2O and NOx flux
with O2 content in an inlet gas occurs as oxygen concentration in O2/N2 mixtures
increases. The general conclusion could be drawn that the combustion in oxygen-
enhanced conditions leads to reducing the pollutants emission of NOx and N2O
which makes it possible to obtain the required reduced emission of pollutants and no
additional technologies need to be implemented. As it is in the case of oxygen
enhanced combustion in O2/N2 conditions, the CO2 and CO concentrations are
regardless of the drying extent of fuel. The concentration of CO 2 is estimated at
about 95-98%. The CO concentration increases as the moisture content in
combusted fuel decreases and they range within 1-3 ppm. Decline on average of
about 30 % of NO and N2O with O2 content in an inlet gas was also found, which
could be explained by the effect of increasing CO concentration in dry flue gas.
Fig.3. CO2 and CO flux in dry flue gas as a function of moisture content in fuel for
different oxygen content in the inlet gas of O2/N2
CO2 and CO fluxes little depend on the drying extent of fuel and they range
within: for CO2:: 9,0 – 1,6 kmol/s, for CO: 2,8 10-5 – 1,6 10-6 kmol/s, higher
concentrations is noticed when there is a decline of oxygen contents in O2/CO2
mixtures. Similarly as it is in case of O2/N2, there is a decline of NOx and N2O
concentrations in O2/CO2 conditions as well as decline of moisture content of about
40%. Besides increase in oxygen concentration from 21% to 100 % for oxygen-
enhanced combustion in O2/CO2 conditions results in NOx and N2O 4-times
reduction. As it was in the case for oxygen-enhanced combustion in O2/N2
conditions, it may be supposed that combustion of initially dried fuels in oxygen-
enhanced conditions could lead to reducing pollutants emissions of NOx and N2O.
1,6E-03 7,0E-05 6,0E-04 4,0E-05
1,4E-03 6,0E-05 3,5E-05

5,0E-04
1,2E-03 3,0E-05
5,0E-05
4,0E-04
nN2O [kmol/s]
nN2O [kmol/s]
nNO [kmol/s]
nNO [kmol/s]
1,0E-03 2,5E-05
4,0E-05
8,0E-04 3,0E-04 2,0E-05
3,0E-05
6,0E-04 1,5E-05
21 % O2 2,0E-04
NO 2,0E-05
4,0E-04 40 % O2 NO 1,0E-05
N2O 1,0E-05 1,0E-04
2,0E-04 N2O 5,0E-06
0,0E+00 0,0E+00 0,0E+00 0,0E+00
5 15 25 35 45 5 15 25 35 45
Wr [%]
Wr [%]
4,00E-04 3,0E-05
3,5E-04 2,5E-05
3,50E-04
2,5E-05 3,0E-04
3,00E-04 2,0E-05
2,0E-05 2,5E-04
nN2O [kmol/s]
nNO [kmol/s]
2,50E-04
nN2O [kmol/s]
nNO [kmol/s]
1,5E-05
2,00E-04 1,5E-05 2,0E-04
1,50E-04 1,5E-04
1,0E-05 1,0E-05
1,00E-04 NO
60 % O2 1,0E-04 NO
N2O 5,0E-06
5,00E-05 80 % O2 5,0E-06
5,0E-05 N2
0,00E+00 0,0E+00 O
5 15 25 35 45 0,0E+00 0,0E+00
0 10 20 30 40 50
Wr [%]
Wr [%]
3,0E-04 2,5E-05
2,5E-04
2,0E-05
2,0E-04
nN2O [kmol/s]
nNO [kmol/s]
1,5E-05
1,5E-04
NO 1,0E-05
1,0E-04
N2O
5,0E-05
100 % O2 5,0E-06
0,0E+00 0,0E+00
5 15 Wr25[%] 35 45
Fig.4. NO and N2O flux in dry flue gas as a function of moisture content in fuel for
different oxygen content in the inlet gas of O2/N2
The extent of fuel drying largely influences the overall flue gas flux which is shown in
Fig.5 for oxygen-enhanced combustion with various moisture contents in fuel
combusted under O2/N2 and O2/CO2 conditions and various fraction of oxygen.
There is a decline of about 15-20% of wet gas concentration as the moisture content
declines from 43 to 10 %. The increase of oxygen content both in O 2/N2 and O2/CO2
mixtures results in 4-times reduction of pollutant emissions. On the one hand it may
reduce chimney loss due to the reduction of flue gases in a volume, however, it may
also result in limiting the heat transfer in combustion chamber, which may make
difficult to keep the temperature to 1173 K required in CFB boilers.
Fig.5. Flux of wet flue gas as a function of moisture content in fuel for different
oxygen content in the inlet gas of O2/N2
Combustion in an oxygen-enhanced conditions leads to an increase in the adiabatic

temperature. The variations in the heat duty are the result of the changes in the
temperature distribution in the combustion chamber. The variable temperature
distribution, in turn, results from an increase in the adiabatic temperature, which is
mainly caused by the reduction of the flue gas volume with the increase in the
oxygen content of the gas supplied to combustion. Slight increase of CO2 flux and
decrease in CO flux during combustion in oxygen-enhanced conditions prove higher
efficiency of the process under these conditions. Maximum oxygen content in O2/N2
and O2/CO2 mixtures should not be higher than 60 %, however, the maximum drying
extent of fuel should not exceed 50 % of the initial moisture content, which means
the value of 20 - 25 % for the examined brown coal.
SUMMARY AND CONCLUSIONS
The research of CFB boiler operation for oxygen-enhanced dried lignite

combustion under O2/N2 and O2/CO2 conditions allow the following general
conclusion to be drawn:
The CO2 concentration in dry flue gas little depends on the drying extent of fuel
but depends on the oxygen content in mixtures of O2/N2 and O2/CO2 and its
concentration ranges within 15 - 96 % depending on the increasing oxygen content.
The CO2 flux little depends on the drying extent of fuel in the mixture of O2/N2,
however, it declines about six times as oxygen content in the mixture O 2/CO2
increases.
Decrease in CO concentration in dry flue gas is close to zero (about 1 - 5 ppm)
for oxygen-enhanced combustion in O2/N2 and O2/CO2 conditions, however, it
slightly increases as the decline of the initial moisture content is noticed.
Slight increase in CO flux (about 10%) for oxygen enhanced combustion in
O2/N2 and O2/CO2 conditions is noticed as the moisture content decreases,
however, there is a significant decline of CO flux of about one degree as the oxygen
content increases.
Decrease in NO concentration in dry flue gas of about 30 % for oxygen
enhanced combustion in O2/N2 and O2/CO2 conditions is noticed as the initial
moisture content declines.
Decrease in NO flux of about 40 % for oxygen-enhanced combustion in O2/N2
and O2/CO2 conditions is noticed as the initial moisture content declines.
N2O concentration in dry flue gas decreases about twice for oxygen enhanced
combustion in O2/N2 and O2/CO2 conditions as the initial moisture content declines.
Decrease of N2O flux on average of about 40 % for oxygen-enhanced
combustion in O2/N2 and O2/CO2 conditions is noticed as the initial moisture content
declines.
The analysis of operation of a circulating fluidized bed boiler show that
combustion in oxygen-enhanced conditions cause an increase in the adiabatic
temperature. The variation in the heat duty is the result of the changes in the
temperature distribution in the combustion chamber. It mainly refers to membrane
walls of the combustion chamber, superheaters SH I and SH II and heat exchangers
located in the 2nd pass.
Coal combustion in oxygen-enhanced conditions causes an increase of heat
transfer between fluidized bed, membrane-walls and superheaters. That increase in
the heat transfer is the result of the changes in the temperature distribution in the
combustion chamber.
The research show that the maximum oxygen content for oxygen enhanced
combustion in O2/N2 and O2/CO2 conditions should not be higher than 60 %,
however, the maximum drying extent of fuel should not exceed 50 % of initial
moisture content, which means the 20-25 % for the examined coal.
NOTATION
ni – i-th gas component flux, kmol s-1
ngas – wet flue gas flux, kmol s-1
w – superficial gas velocity, m s-1,
Wr – moisture content, %
zi – concentration of i-th gas component, %, ppm
REFERENCES
[1] Muskała W., Krzywański J., Sekret R, Nowak W. Model research of coal
combustion in circulating fluidized bed boilers. Chemical and Process Engineering
2008; 29:473-492.
[2] Krzywanski J., Czakiert T., Muskala W., Sekret R., Nowak W., Modeling of Solid
Fuels Combustion in Oxygen-Enriched Atmosphere in Circulating Fluidized Bed
Boiler – Part I. The mathematical model of fuel combustion in oxygen-enriched CFB
environment, Fuel Processing Technology, 2010, Vol. 91, pp. 290-295.
[3] Klajny T., Krzywański J., Nowak W. Mechanism and Kinetics of coal combustion
in oxygen enhanced conditions. 6th International Symposium on Coal Combustion ,
Wuhan, China, 1-4 December 2007: 148-153.
[4] Nowak W., Klajny T., Krzywański J., Czakiert T., Mechanism of Coal Combustion
in Oxygen Enhanced Conditions, Procedings of the 20th International Symposium on
Chemical Reaction Engineering, Kyoto 7-10.09.2008, Book of Abstracts, p.410- 411.
[5] Klajny T., Krzywański J., Nowak W., Mechanism and kinetics of biomass
combustion in oxygen enhanced conditions, XX-th International Symposium on
combustion processes, Pultusk, Poland, September 3-5, 2007.
[6] Hu, Y., Naito, S., Kobayashi, N., Hasatani, M., 2000. CO2, NOX and SO2
emissions from the combustion of coal with high oxygen concentration gases. Fuel.
79, 1925-1932
COLD FLOW MODEL STUDY ON INTERCONNECTED
FLUIDIZED BED REACTORS FOR MULTI-GENERATION
SYSTEMS AND CHEMICAL LOOPING PROCESSES
G. A. Ryabov*, O. M. Folomeyev, D. A. Sankin, K. V. Khaneyev

All-Russian Thermal Engineering Institute, 14/23 Avtozavodskaya St., Moscow,
Russia, Phone (495) 675-3239, Fax (495) 234-7427,
e-mail: georgy.ryabov@gmail.com, vti@vti.ru
ABSTRACT
Interconnected fluidized bed reactors (DCFB) were implemented in multi-generation

systems (pyrolysis FB reactor and CFB boiler), chemical looping combustion (CLC)
systems (double metal oxides or carbonate oxide reactors) and three reactor
chemical looping gasification processes. The presented data focus on the solids
circulation rate and on pressure profiles of the DCFB depended on selected
operating parameters such as fluidization gas flow rate, loop seal fluidization, and
solids inventory. Most work was devoted to studying standpipe and valve operation.
INTRODUCTION
The important feature of the DCFB concept is the inherent stabilization of solids
hold-up obtained by the direct hydraulic link between the two CFB systems, i.e. the
loop seal connection in the bottom region of the risers. Only the air reactor
entrainment is responsible for the global solids circulation between the reactors,
while the fuel reactor operation can be optimized. The hydrodynamics of
interconnected reactor systems and loop seal (standpipe and non-mechanical
valves) are very important in that optimization.
Modern multi-generation technologies can be subdivided into three categories:

- Multi-generation systems based on complete coal gasification, used by Shell Co.;
- Multi-generation systems based on partial coal gasification (combination of coal
combustion and gasification);
- Multi-generation systems based on pyrolysis of coal.
Multi-generation systems based on pyrolysis of coal include many of configurations.

An example is the shale processing units in the USSR. The resulting technology
was implemented in industrial units. Two high-capacity units of this type (UTT –
3000, 139 tons of shale per hour each) were erected at in the Estonian thermal
power plants and they with still show good performance. VTI has an agreement on
scientific cooperation with the Institute for Thermal Power Engineering, Zhejiang
University in this field. In studies carried out by Zhejiang University (1), (2)) data
were received from their tests on a 1 MW pilot plant. The first results showed that a
pilot unit can produce gas with a heating value of about 12 to 14 MJ/m3 with a 5 to 6
% tar content at 500 to 600 оС in the fluidized bed (FB). It was established that
solids circulation is a critical parameter for stable plant operation. The investigation
was financed by the Russian Ministry of Science and Education as a part of a China
– Russia scientific cooperation project.
Another aim of the investigation of the interconnected FB and CFB reactors is to

study the hydrodynamics of the CLC (double metal oxides or carbonate oxides
reactors) and the three reactor chemical looping gasification processes (3) and (4).
RESULTS
It is important for interconnected units containing CFBs to provide a stable

circulation rate between reactors as well as an efficient solids separation. Such a
study has been connected in VTI`s experimental unit shown in Fig. 1. This unit
consists of a CFB reactor and a transportation reactor (TR) that are interconnected
with pneumatic valves and
standpipes to a FB reactor.
The system consists of three
interconnected fluidized bed
reactors: The CFB (0.2*0.3 m
cross section, 5 m height),
the FB reactor (0.4*0.4 m
cross section, 1.6 m height)
and the transport reactor (0.1
m diameter, 4.8 m height).
Standpipes and J or L valves
connected the FB reactor and
the bottom parts of the CFB
and transport reactors with
the cyclones of the CFB and
transport reactors.
The CFB reactor consisted of

a vertical column 5.4 m high,
made of 9 sections 600 mm
high each with a 300*200 mm
cross-section. The upper
section was connected to the
cyclone inlet. The cyclone
outlet was removable and Fig. 1 –Drawing of the VTI cold model of
was located 50 mm away interconnected reactors
from the cyclone central axis.
The cyclone cone was
connected to a standpipe, consisting of 3 sections, each of 100*100 mm cross-
section. The lower section of the standpipe was connected to a pneumatic valve.
The design of the valve allowed solids to flow in different directions. Part of the flow
could be directed back to the bottom part of the CFB reactor, and the other flow to
the FB reactor. The transportation reactor consisted of a vertical column 5.4 m high,
made of 3 sections of 100 mm diameter and each were 1600 mm high. The reactor
and standpipes were equipped with taps to measure pressure along their heights.
The FB reactor consisted of a vertical vessel with a square (400*400 mm) cross-
section and 1500 mm in height. There was a nozzle grid at its bottom for distributing
the air. The reactor was subdivided into two equal 200*400 mm sections by a
partition. Solids were discharged from the FB reactor through pipes equipped with a
pneumatic L-valve. The L-valve connected the bottom of the first section of the FB
reactor to the bottom part of the transportation reactor. In the first section of the FB
reactor, air flowed counter-currently to the flow of solids. In the second section flow
ws co-current. In the second section, solids were discharged through the top part of
the section, and then fell into the CFB reactor. The VTI aerodynamic test unit has
been described in other references (5) and (6). Local mass flows were measured
with isokinetic S-type probes, and local heat exchange with gauges while heating.
Also mini-turbine flowmeters and differential concentration-measurement gauges
were employed.
Based on these tests it was established that:

- pressure profiles and vertical solid concentrations in the CFB and FB reactors are
depended on gas velocity and solids loading;
-pressure drops in the unit
depended on operating
parameters and on design
features of the units and
return legs.
VTI studies carried out on

a similar unit showed that
particle size determined
the value of the
dimensionless criteria (Аr,
Re, Fr), used for
hydrodynamic and heat
exchange calculations. It
was established that the
change in average particle
size with respect to unit
width or diameter was
insignificant. The studies
were basically directed to
calculate the circulating
mass flow rate in the
external circuit (Gr), as it
is the critical operational Fig. 2 – Typical solid circulation rate as function of
parameter for the velocity and inventory
ireactors. The solid flow
rate increased with gas velocity in the CFB unit and with unit inventory. This
relationship is shown in Fig. 2. This relationship was obtained at stable unit
operation when unit load increases were possible. Stable system performance was
made possible with good loop seal operation. A separated solids return system is
necessary for reliable operation of the CFB unit. Usually a return system consists of
a vertical standpipe, pneumatic valve and a short return leg back to the furnace. It is
important to choose the right dimensions (diameters and height) of the standpipes
and have them operate in the correct fluidization regime. Observation of the solids
motion in the standpipe indicated that in the bottom part was in dense phase flow,
but it was in dilute phase flow at the top. During several tests with sand (at a low bed
level in the standpipe and a large mass of sand in the unit) a pulsating regime was
established with bubble generation and gas overshoot to the upper part of the
standpipe. The amplitude of the standpipe solids level oscillations reached 1 m with
a frequency of 0.1 Hz. The limiting significant pulsation case could be estimated
using Equation (1):
⎛ ΔP ⎞
⎜ ⎟ ⋅ Hs ≈ Hv ⋅ (1− εv ) ⋅ ρp ⋅ g + ΔРft + ΔРc (1)
⎝ L ⎠mf
At normal conditions the pressure drop in the upper part of the loop seal
H v ⋅ (1 − ε v ) ⋅ ρ p ⋅ g was equal to or exceeded the pressure drop at the bottom part
of the furnace ΔРfb=ΔРf-ΔРft, so this guaranteed zero furnace gas overshoot into the
valve or the standpipe. The limiting bed level in the standpipe was estimated using
Equation (2):
ΔР f + ΔРc
(Н s )lim = (2)
⎛ ΔР ⎞
⎜ ⎟
⎝ L ⎠ mf
In the tests, the limiting bed level in the standpipe ranged from 0.15 to 0.5 m. This
increased with increasing bed mass and increasing particle size. For an industrial
CFB boiler this limiting value was about 2-3 m. It was suggested (7) to increase the
standpipe height to double its normal height. Fig. 3 shows the dependence of
standpipe bed level with constant aeration. Small changes in aeration to the
standpipe caused a significant bed level change in the standpipe (Fig. 3a), but the
aeration to the valve had little affection on the standpipe bed level (Fig. 3b).
1 – full cross-section bed material reduced speed Wms=0,013 m/s; 2 – Wms=0,02

m/s; 3 – Wms=0,05 m/s; 4 – Wms=0,1 m/s; 5 – Wms=0,15 m/s
Fig. 3 – Standpipe bed level dependence of aeration to the standpipe (a) and to the
valve (b)
Thus, parameters shown in Fig. 3 are critical for return system regulation. The best
operational mode is with continuous light aeration to the standpipe and regulating
the aeration to the valve.
A master curve of standpipe bed height (Нs/H0) relative to aeration velocity (Wsv/Wmf)
is shown in Fig. 4. Solids inventory in the unit (riser + return system), gas flow rate in
the riser and in the solids upflow section of the loop seal were constant, as aeration
to the standpipe was varied. A similar curve was given by (8), which says that the
minimum bed height
level was obtained
when the air velocity
is about 5 Wmf. If the
velocity was less
than 4 Wmf there
was an increase in
the height of the
solids level in the
standpipe. If the air
velocity was greater
than 6 Wmf, then the
steandpipe height
increased with
increases in gas
velocity. At low
velocities – there
was a dense
bubbling downflow
mode and at high
velocities air
bubbles moved 1 –Knowlton data (8), 2 – VTI experimental data
upwards to the Fig. 4 – Relative standpipe bed material height level
cyclone. Our data dependence of relative air velocity in the standpipe
show that the
cyclone efficiency decreased when that occurred. From the data in Fig. 4 it is clear
that it was necessary to maintain the bed level in the standpipe so that it did not
exceed 0.4 of its height with simultaneous limitation of aeration to the standpipe at la
value of 3-6 Wmf. Within the recommended regime, the solids flow rate reached
1800 t/h⋅m2 (there was no opportunity to reach higher values because of cyclone
overload). It is recommended a velocity of 0.1 m/s be used for standpipe diameter
calculations.
In the normal operating mode of the ash return system, a dense flow occurs in the
bottom part of the standpipe. In this case, the Ergan Equation pressure gradient will
be equal to:
ΔP 150 ⋅ μ g ⎛1− ε ⎞ 1,75 ⋅ ρ g ⎛1− ε
2
⎞
= ⋅⎜ ⎟ ⋅ VR + ⋅⎜ ⎟ ⋅ VR ⋅ / VR / (3),
L (ϕ ⋅ d )2 ⎝ ε ⎠ ϕ ⋅d ⎝ ε ⎠
A linear dependence of voidage on relative velocity was suggested by Knowlton (8):
VR ⋅ ε mf
ε = ε v + (ε mf − ε v ) ⋅ (4)
Wmf
Relative bed velocity is equal to:
Gp Qg
VR = Wp −Wg = − (5)
ρ p ⋅ (1 − ε ) ⋅ Fs ρg ⋅ ε ⋅ Fs
From Equations (3), (4) and (5) voidage as a function of pressure gradient Δ P in
L
the standpipe can be calculated as:
ΔP 2
⎛1− ε ⎞
2
L ⎛ 1 − ε mf ⎞ (6)
⎜ ⎟ ⋅ (ε − ε v ) = ⋅⎜ ⎟ ⋅ ( ε mf − ε v )
⎝ ε ⎠ ⎛ Δ P ⎞ ⎜ ε ⎟
⎜ ⎟ ⎝ mf ⎠
⎝ L ⎠ mf
The standpipe voidage dependence on relative gas velocity (Wg/Wmf) is represented

in Fig. 5a. Standpipe voidage increased with increasing of the aeration, but was still
less than the voidage a minimum fluidization. A comparison of the relative particle
velocity from Equation (5) and form the observed solids velocity (Fig. 5b) shows that
the calculated relative velocity was lower than the observed velocity in most cases.
This indicates that gas flowed down with the bed material. In the pulsation regime,
the relative velocity was much higher than the observed velocity, indicating that the
gas was flowing up the standpipe.
1-particle velocity in standpipe Wms=0,06 m/s; 2 – Wms=0,1 m/s, 3 - Wms=0,13 m/s

Fig. 5 – Relative air velocity dependence of standpipe voidage (a); Particle velocity
in the standpipe dependence of its relative velocity (b)
Thus, calculations confirmed the experimental data from the unit and indicate that
this method can be used to design industrial units.
CONCLUSIONS
The studies on solids circulation and solids return systems of interconnected

reactors found:
- pressure profile and vertical solids concentrations in interconnected FB and

CFB reactors were typical for reactors of this type, and depended on gas
velocity and bed mass;
- the axial pressure profile depends on the fluidization velocity and the design
features of unit`s structure and return system;
- the recirculating solids flow rate between interconnected FB and CFB reactors
depends on gas velocity and solids inventory in the CFB reactor, on high-
efficiency cyclones and sufficient capacity of the return system for a certain
particle size;
- the solids return system (standpipe and pneumatic valve) must have a reserve
capacity and be able to regulate aeration to the standpipe and to the upflow part
of the valve. Otherwise, the recirculation solids flow rate is determined by the
operational mode of the valve.
ACKNOWLEDGEMENT
Financial support of this work by the Federal Agency of Science and Innovation is
gratefully acknowledged.
NOTATION
Gc – solid circulation rate

Ho – standpipe height
Hs – bed height in the standpipe
Hv – height of the upper part of the valve
M – unit inventory
ΔPft – pressure differential at the top of the furnace
ΔP c – cyclone pressure drop
ΔPfb – pressure differential at the bottom part of the furnace
ΔPf – pressure differential in the furnace
u – gas velocity in the riser
ρp – particle density
εv – vibrated bed porosity (≈ 0.37)
εu – voidage in the upper part of the valve
Wmf – velocity at minimum fluidization
Wms – particle velocity in the standpipe (downflow particle velocity)
φ – shape coefficient (ϕ ≈ 0.73)
VR – relative particle velocity
ε – voidage
εmf – minimum voidage
Gp – solids flow rate
Qg – flow rate of gas
Fs – cross-section of the standpipe
Wg – relative gas velocity
Wsv – standpipe fluidization air velocity
⎛ ΔP ⎞
⎜ ⎟ - pressure gradient in the standpipe at minimum fluidization parameters
⎝ L ⎠ mf
ΔP
- pressure gradient
L
(H S )lim - limiting bed level in the standpipe
d - average particle diameter
REFERENCES
1. M. Fang, Q. Wang , C. Yu, Z. Shi, Z. Luo, K. Cen, Development of Gas

Steam and Power Multi-Generation System, Proc. of 18th Int. Conf. on
FBC, May 22-25, 2005, Toronto, Ontario, Canada.
2. M. Fang, J. Cen, Q. Wang, K. Cen,. Z. Cao, X. Zhang, J. Shu, X. Rao, G. Dong,
J. Wang, Y. Wang, Study on Coal Combustion and Pyrolysis Gas Tar and Steam
Polygeneration System, Proc. of 9th Int. Conf. on CFB, May, 2008, Hamburg,
Germany.
3. A. Lyngfelt, M. Johansson, T. Mattisson, Chemical looping combustion – Status of
development, Proc. of CFB 9, May 13-16, Hamburg, Germany, pp 39-53
4. T. Proll, K. Rupanovits, P. Kolbitsch, J. Bolhar-Nordenkampf, H. Hofbauer, Cold
Flow Model Study on a Dual Circulating Fluidized Bed (DCFB) System for Chemical
Looping Processes, Proc. of CFB-9, Germany, Hamburg, May 2008.
5. O. M. Folomeyev, S. N. Truhachev, G. A. Ryabov, Hydrodynamics and heat
exchange study of overbed area functional in the CFB units, “Teploenergetica”
№10, 2000., pgs 27-32.
6. G. A. Ryabov, O. M. Folomeyev, D. A. Shaposhnik, Solid separation in upper
part of CFB riser, Proc. of the 8-th Int. Conf. on CFB, Hangzgou, China, May 10-13,
2005.
7. Chong I.O., O'Dea D.P., Leung L.S. at el. Design of standpipe and non-
mechanical V-valves for a circulating fluidized bed. 3-rd Int. Conf. on CFB
Technology, Pergamon Press, 1988.
8. Knowlton T.M. Non-mechanical solid feed and recycle devices circulating
fluidized beds. 3-rd Int. Conf. on CFB Technology, Pergamon Press, 1988.
FLOW RATE OF SOLIDS IN L-VALVES
Duvvuri Subbarao
Department of Chemical Engineering,
Universiti Teknologi PETRONAS, Tronoh 31750, Malaysia
ABSTRACT
Movement of solids in a L-valve by fluid drag due to external aeration is opposed by

frictional resistance at the wall/non-moving solids. Model equations developed for the
threshold aeration rate and solids flow rate as a function of aeration rate compare
well with the literature data.
INTRODUCTION
Transport of solids into and out of process equipment is of critical importance for
smooth continuous operation of process units handling particulates such as
circulating fluidized beds. Non-mechanical valves such as L-valve (L–shaped pipe)
are widely used to control solid flow by fluid drag. Solids discharging from a cyclone
at a pressure PS flow and accumulate as packed bed of height HU in the vertical
standpipe of a L-valve as the drainage at the bottom is arrested by the presence of a
horizontal pipe of length HD. External aeration to the bottom section of the stand pipe
at a pressure P1 control solids flow through the horizontal pipe into the riser at
pressure PR. Pioneering work reported by Knowlton and Hirsan (1) on the
characteristics of L-valves has excited further investigations (2 - 8) to explore the
effect of particle properties and geometry of the valve on the particle flow rate W as a
function of gas flow rate Q. It is to be noted that in industrial units PS > P1 >PR while
in laboratory research units PS = PR = P2. Some of the empirical correlations
proposed to relate solid flux to gas velocity are summarized in Table 1.
Table 1: Correlations reported in the literature for sold flux through L-Valve
Reference Correlation
Geldart and Jones (2) Gs u
= 3354 − 2965
Dt u mf
Smolders and Baeyens (6) 2
Gs ⎛ u ⎞ 0 .6
= 79600⎜ ⎟ Dp
Dt ⎜u ⎟
⎝ mf ⎠
Daous , Al-Zahrani (10) Gs u
= 1.08 − 5450
Dt Dp
Chan et l.(12) 8.9
Gs ⎡ ⎛ u ⎞⎤
= 0.0002 ⎢ln⎜ ⎟⎥
Dt ⎢⎣ ⎜⎝ D p ⎟⎠⎥⎦
Yang and Knowlton (9) presented a model to estimate solid flow rate in a L-
valve assuming no slip between flowing gas and particles; the net gas flow was
assumed to include external aeration introduced along with the gas flowing through
the solids in the standpipe; they adopted the equation of Jones and Davidson (10)
(developed for particle discharge through an orifice from fluidized beds) for solids
flow rate through an active flow area which increased with L-valve pressure drop;
however, the correlation proposed by them reflects the universally observed need of
a threshold aeration rate to initiate flow of solids. Daos and Al-Zahrani (11) and Tong
and Zheng (12) considered gas-particle slip velocity to be described by Ergun’s
equation for flow through packed beds. Tong and Zheng (12) considered mechanics
of particulate media flow in modeling gas and particle flows in a L-valve; they noted
that external aeration rate can split into two streams – one flowing out horizontally
through the bend and the other through the vertical stand pipe – depending on the
relative resistance in each section for gas flow.
Asymmetry in the introduction of gas flow and two phase flow through a three
dimensional 90o bend in a L-valve makes particle flow visualization difficult. In an
interesting piece of effort, Chan et al. (13) investigated particle motion by positron
emission particle tracking technique to identify particle flow structure and observed
solid flow to be stable for u/umf less than 6. They observed that maximum solid flow
rate in a hopper fed laboratory L-valve is limited by the hopper discharge pipe
diameter. Agarwal (14) investigated particle flow structure in a 2-dimensional L-valve
made of 0.6 cm thick Perspex sheets with a cross sectional size of (13.8 cm x 2 cm).
Effect of standpipe height (i150 to 100 cm), length of horizontal section (i30 to 50
cm) and particle size on solid discharge rate as a function of aeration rate were
investigated. A typical solid flow trajectories are shown in Fig 1. For gas flow rates
below threshold aeration, solids were stagnant; at and around the threshold aeration
rate first movement of solids was observed near the 900 bend at the upper edge of
the L-valve; coordinates of points farthest from Y-axis upto which solids velocity is
zero (y) were noted for each (x) coordinate; these points were plotted as shown in
Fig. 1.
cms
Zone of Zone of
Stagnant Solid flow
Solids
cms
Fig.1 Solid flow trajectories in a 2-D L-valve (Agarwal(14))

At an aeration rate of 422 cc/s with a low solid flow rate of 10 kg/hr, particles
movement was restricted to a rather narrow region very near the inside of 900 turn
and along the top edge of the horizontal section over a stagnant layer; at the exit,
particles rolled out over the slope dictated by angle of repose; cross sectional area of
particle down flow in the stand pipe increased with distance away from the 90o bend.
At 750 Kg/hr, the stagnant region decreased in size and at 1700 Kg/hr it decreased
further but still a substantial portion of the particles in the bend remained stagnant.
Similar solid flow profiles were observed at different aeration point locations with the
other particles.
A simple equation for solid flow rate as a function of the affecting parameters is
needed for rational design of L-valves. In the present work, an attempt is made to
develop equations for a L-valve operating with PS = PR = P2 considering that a
threshold aeration rate is needed to initiate solid flow and solids flow rate increases
with fluid drag on particles while their movement is resisted by the drag due to wall /
stationary particles on moving solids.
THE MODEL
The aeration rate Q provided to a stand alone L-valve containing particles in the
standpipe and horizontal pipe in a packed bed form gets split into an up flow stream
QU (through the standpipe) and downflow stream QD (through the horizontal pipe)
depending on their relative packed bed resistance for gas flow. At a threshold
aeration rate QTh, solids flow rate is initiated through a “small throat” at upper wall 90o
bend of the horizontal pipe as the gas drag force overcomes the friction between
particles to wall/particles to push the particles to the edge where they roll over by
gravity. Particles in the standpipe descend by gravity to the extent of solid flow
through the horizontal section. As the particles descend in a section of the standpipe
against the up flow aeration rate of QU, the gas to particle relative velocity in that
section will be at the incipient fluidization condition as the bed voidage is around 0.5.
The “small throat” diameter needs to be greater than 5xDp to 10xDp to overcome
arching tendency. Further increase in external aeration through the L-valve increases
the gas drag force on particles to increase solid flow rate and throat area near 90o
bend near the upper wall. Due to the gas-particle slip velocity and increased sold flow
rate, most of the external aeration ends up in the down flow stream assisting solid
flow rate. Together, the solid flow rate depends on aeration rate Q above the
threshold aeration rate QTh, standpipe diameter D, height of the standpipe above the
aeration point HU, length of downstream solid flow path HD through which solids flow
out, particle diameter Dp, particle density !p, gas density !g and gas viscosity .
Based on this hypothesis, equations are developed in the following sections.
Model for Threshold Aeration Rate QTh:
Threshold aeration rate is the aeration rate at which the drag by gas can just
overcome the friction between particles and particles/wall to let the solids flow along
with the gas. Aeration flow introduced into the standpipe at a pressure P1 gets split
into upward flow through the standpipe and downward/horizontal flow through the
horizontal section depending on the resistance in each section. As both sections are
filled with particles in a packed bed form, assuming laminar flow and exit pressure P2
to be same, from Ergun’s equation, the upflow and downflow components can be
expressed as
πDt2 ε3 D p2 (P1 − P2 )
QU = 1
4 150 ( 1 − ε )2 μHU
πDt2 ε3 D p2 (P1 − P2 )
QD = 2
4 150 ( 1 − ε )2 μH D
From ratio of these two flows
QU H D
= 3
QD H U
and the two components add upto the aeration rate Q
QU + QD = Q 4
From equations 3 and 4, flow in the horizontal section can be obtained as
⎛ H ⎞
Q D ⎜⎜1 + D ⎟⎟ = Q 5
⎝ HU ⎠
From equations 2 and 5
πDt2 D p2 (P1 − P2 ) ⎛ H U + H D
ε3 ⎞
Q= ⎜⎜ ⎟⎟ 6
4 150 ( 1 − ε ) 2 μH D ⎝ HU ⎠
At the point of particle flow initiation, particles flow through a critical throat area
(fU (Dt2/4)). Relative velocity between gas and particles in the moving section of the
standpipe will be around umf. Hence, pressure drop for gas upflow in that section can
be expressed as
P1 − P2 = H U (ρ p − ρ g )(1 − ε )g 7
With this approximation, threshold gas velocity can be obtained as
πDt2 D p2 (ρ p − ρ g )g (H U + H D )
ε3
QTh = fU
4 150 ( 1 − ε ) μ HD 8
= fU
πDt2
umf
( HU + H D )
= fU X
4 HD
with X defined as
πDt2 HU + H D
X = u mf 9
4 HD
Threshold Aeration Model Validation:
Experimental observations on QTh reported in the literature are compared with
parameter X, defined by equation 9 in Fig. 2. The correlation is reasonably good and
an average value for the factor fU at the initiation of particle flow is estimated to be
0.07.
πDt2 HU + H D
QTh = 0.07 umf 10
4 HD
350
300
250
QTh, mL/s
200 Knowlton
Arena
150
Geldart
100 Zheng
QTh=0.07 X
50
0
0 1000 2000 3000 4000 5000 6000
Parameter X
Fig.2 Correlation of data on threshold aeration rate reported in literature with

parameter X (Eq.9)
Model for Particle Flow Rate:
Let the interstitial gas velocity be u and solids velocity be v in the horizontal pipe
through which solids flow out of L-valve. The flow of solids due to fluid drag is
resisted by the friction at the non moving particles/pipe walls.
πD 2 H D 6(1 − ε ) πD p2 v2
Np FD = c Dm ρ g (u − v )2 = f πDH D ρ p (1 − ε )ε
4 πD p 3
4 2 11
Fluid drag on particles = Friction at the wall
For aeration rates Q greater than the threshold QTh, area (D2/4) of solid flow
increases with gas flow upto (Dt2/4) where the solid flow rate will be Wmax.
W D 2 − DTh2 D2
= ≈ 12
Wmax Dt2 Dt2
Assuming laminar flow conditions, the drag coefficient and friction factor can be taken
as
μg μb
c Dm ∝ ; f ∝ 13
D p ρ g (u − v ) Dρ b v
Rearranging equations 11 with 12 and 13
⎛ k μ b D p ⎞⎟
2
u ⎜
= 1+ v 14
⎜ 1 − ε μ D2 ⎟
⎝ g ⎠
where k is a constant. Combining equation 14 with 12
ρ p (1 − ε ) ⎛ D2 W ⎞
(Q − QTh ) = ⎜⎜1 + kv p2 max ⎟⎟W 15
ε ⎝ Dt W ⎠
where kv is a constant incorporating gas viscosity, moving bed viscosity, bed
voidage, k and other constants.
Yang and Knowlton (8) suggested that maximum flow rate of solids may be
estimated using the equations proposed by Jones and Davidson (10) developed for
particle discharge rate from fluidized beds through an orifice
Wmax = 0.56 ρ p (1 − ε )g 0.5 H U0.5 ( Dt − D p ) 2 16
However, particles move as a packed bed in a section of the horizontal pipe. Hence,
maximum flow rate of solids may be dictated by the diameter of the horizontal pipe
and may be estimated by the equation of Beverloo et al. (15) given as
Wmax = 0.58ρ p (1 − ε )g 0.5 ( D t − 1.5D p ) 2.5 17
Validation of the Model for Particle Flow Rate:
Data of Knowlton and coworkers (1), Zeng et al. (4) and Arena et al. (7) on solid flow
rate as function of aeration rate are compared with the present model equation 15 in
Fig.3 with and kv assigned values of 0.4 and 2640. Table 2 summarizes the details
of the properties of the experimental systems. The estimates of maximum solid flow
rate by the equation 16 of Jones and Davidson (10) and equation 17 of Beverloo et
al.(15) are included in Table 2. Experimentally observed maximum solid flow rates
are in the range suggested by the Beverloo equation.
Table 2. Details of the systems used for the evaluation of the equation 15
Reference D HS HD Dp !p Wmax. g/s
cm cm cm cm g/cm3 Eq.16 Eq.17
Knowlton 1, (1) 7.62 854 45.72 0.02609 2.611 38820 3798
Knowlton 2, (1) 5.08 854 45.72 0.02609 2.611 17253 1378
Knowlton 3, (1) 7.62 854 45.72 0.02609 2.611 38820 3798
Zheng, (4) 4.7 295 32.6 0.0605 1.392 4629 605
Arena 1, (7) 2.7 270 31.7 0.0073 2.55 2678 277
Arena 2, (7) 2.7 270 31.7 0.0156 2.55 2678 277
Arena 3, (7) 2.7 270 31.7 0.0341 2.55 2678 277
Arena 4, (7) 2.7 270 31.7 0.017 4.46 4683 485
10000
W(1+[kvDp2Wmax)/(Dt2W)], g/s
1000
Knowlton 1
Knowlton 2
Knowlton 3
100
Zheng
Arena 1
Arena 2
10 Arena 3
Arena 4
Parity line
1
1 10 100 1000 10000
(Q‐QTh)!p((1‐ε)/ε), g/s
Fig.3. Comparison of equation 15 with the literature data.

Data of Knowlton and coworkers (1) Zeng et al. (4) and Arena et al.(7) are
resasonably well represnted by the equation 15 as shown in Fig.3.. Using equations
15 and 17, maximum solid flow rate and corresponding maximum aeration rate Qmax
upto which the L-valve can be operated can be estimated.
CONCLUSIONS
1). A model for solid flow rate in a stand alone L-valve as a function of external
aeration rate is developed considering that a minimum threshold aeration rate QTh is
necessary to initiate solids flow rate in L-valves.
2). Threshold aeration rate increases with increase in L-valve diameter and
particle minimum fluidization velocity. The model equation 10 gives a reasonable
description to the experimental observations reported in the literature as shown in
Fig.2.
3). Equation 15 with kv assigned a value of 2640 could correlate the data of
Knowlton and coworkers (1), Zeng et al. (4) and Arena et al. (7) on solid flow rate as
a function of external aeration rate as shown in Fig.3.
ρ p (1 − ε ) ⎛ D p2 Wmax ⎞
(Q − QTh ) = ⎜1 + 2640 2
⎜
⎟W
⎟
18
ε ⎝ Dt W ⎠
ACKNOWLEDGEMENT
The author is thankful to University Teknologi PETRONAS for the encouragement

and support for carrying out this work.
NOTATION
cDm Gas-particle drag coefficient

D Diameter of throat through which solids flow (cm)
Dp Diameter of particles (cm)
Dt L-valve diameter (cm)
f Friction factor for flow of solids
fU Fraction of standpipe particles set in motion
g Acceleration due to gravity (cm/s2)
Gs Particle mass flux, (kg/m2/s)
HD Length of down flow section (cm)
HU Height of upflow section (cm)
Hs Standpipe height (cm)
P1 Aeration point pressure (g/cm/s2)
P2 Discharge point pressure (g/cm/s2)
Q Aeration flow rate (cm3/s)
QD Downward aeration flow through Horizontal section (cm3/s)
QTh Threshold Aeration Rate (cm3/s)
Qu Upward aeration flow through standpipe (cm3/s)
u’, v’ Actual gas and particle velocities (cm/s)
u Superficial gas velocity (cm/s)
umf Minimum fluidization air velocity (cm/s)
W Solids flow rate (gm/s)
Wmax Maximum solid flow Rate (gm/s)
Greek Symbols
Bed voidage
,!g Gas density (g/cm3)
!b !P Density of moving bed, Particle (g/cm3)
Gas viscosity (g/cm/sec)
b Viscosity of moving bed (g/cm/sec)
REFERENCES
1. T. M. Knowlton, I. Hirsan, L-valves characterized for solids flow, Hydrocarbon

process, 3(1978) 149-156
2. D. Geldart, P. Jones, The behavior of the L-valves with granular powders,
Powder Technol, 67 (1991) 163-174.
3. M.Ozawa, S.Tobita, T Mii, Y.Tomoyasu, T.Takebayashi, K Suziki, Flow
pattern and flow behaviour of solid particles in L-valve, CFB Technology III,
(Eds) P.Basu, M. Horio and M.Hasatani, Pergamon, Oxford (1991), 615-620.
4. Q.Zheng, Z.Ma, A.B.Wang, Experimental study of the flow pattern and flow
behaviour of gas-solid two phase flow in L-valve, in:A.A.Avidan, (ed). CFB
Technology IV, Hidden Valley, USA (1993) 246-252
5. M. Rhodes, H. Cheng, Operation of an L-Valve in a circulating bed of fine
solids, in:A.A.Avidan, (ed). CFB Technology IV, Hidden Valley, USA (1993)
240-245.
6. K.Smolders and J.Baeyens, “ The operation of L-Valves to control standpipe
flow” Advanced Powder Technology, vol. 6 (1995) 163-176
7. U. Arena, A. Cammarota, “L-valve behavior with solids of different size and
density”, Powder Technol, 98 (1998) 231-240.
8. W.Yang, T. M. Knowlton, L-valve equations, Powder Technol, 77 (1993) 49-
54
9. T. M. Knowlton, “Standpipes and return systems”, in: J.R.Grace, A.A.Avidan
and T.M.Knowlton (Eds.), Circulating Fluidized Beds, Chap 7, Blackie
Academic & Professional, an imprint of Chapman & Hall, London, 1997, 214-
260.
10. D.R.M. Jones, J.F. Davidson, The flow of particles from a fluidized bed
through an orifice, Rheologica Acta 4 (1965) 180– 192.
11. M. A. Daous, A. A. Al-Zahrani, “Modeling solids and gas flow through an L-
valve”, Powder Technol, 99 (1998) 86-89.
12. H. Tong, Q. Zheng, “Hydrodynamic modeling of the L-valve”, Powder
Technol, 129 (2003) 8-14.
13. C.W.Chan, Jonathan Seville, Xianfeng Fan, Jan Baeyens, “Particle motion in
L-valve as observed by positron emission particle tracking”, Powder
Technology 193 (2009) 137-149.
14. Amit Agarwal, “Solid flow in a 2 D Lvalve”, M.Tech Thesis IIT Delhi (2004).
15. W.A. Beverloo, H.A.Leniger, J, van de Velde, The flow of granular solids
through orifices, Chem.Eng.Sci., 15 (1961)260-269.
PROCESS DECOUPLING OF PLASMA ENHANCED
SYNTHESIS OF CHLORINATED POLYVINYL CHLORIDE
(CPVC) PARTICLES IN A CIRCULATING FLUIDIZED BED
Wei Lu, Tengfei Cao, Yi Cheng*

Department of Chemical Engineering, Beijing Key Laboratory of Green Chemical
Reaction Engineering and Technology, Tsinghua University
Beijing 100084, P.R. China
PH: +86-10-62794468; FAX: +86-10-62772051; e-mail: yicheng@tsinghua.edu.cn
ABSTRACT
Plasma enhanced synthesis of CPVC particles in a gas-solid plasma circulating

fluidized bed reactor (PCFBR) is proposed as a novel CPVC synthesizing method.
The chlorination process is decoupled into a fast initiation step in a plasma riser and
a slow chlorination process in the accompanying bed. The CPVC product has good
properties in terms of chlorine content and microstructure.
INTRODUCTION
Chlorinated polyvinyl chloride (CPVC) is produced by chlorination of polyvinyl

chloride (PVC) particles. In recent years, CPVC has received much attention as a
kind of high-performance thermoplastic which gives better performance in heat
stability, mechanical properties and flame retardant ability because of the increase of
polarity compared with PVC. Therefore, CPVC can be widely used in hot and cold
water pipes, industrial liquid handling and other commercial applications (1).
For the rapid development of the chlor-alkali industry in China, a large amount of
excess chlorine has caused a serious problem, i.e., how to balance the noxious
chlorine gas or the chlorine ion as in HCl from a sustainability viewpoint. PVC is a
major solution to this problem, CPVC provides a further valuable route to immobilize
chlorine. By further chlorinating the PVC particles to CPVC, more chlorine gas can
be fixed into the solid products. It is known that the chlorine content of PVC is about
56.7 wt%. Most commercial CPVC resins have a chlorine content ranging from 63
wt% to 69 wt%, and even to 74 wt% by special treatments. For example, about 400
kg of chlorine is consumed by chlorinating 1,000 kg of PVC to CPVC with a 69 wt%
chlorine content. Accordingly, the CPVC industry not only consumes the excess
chlorine, but also converts PVC into another high-value material.
Among the reported approaches to synthesizing CPVC, the aqueous suspension

method is the main production technology at the commercial scale (2-3). However, a
gas-solid method is acknowledged as a cleaner process, considering the ease to
control and to separate the CPVC products from waste gases, etc. The main
challenge of this method is to improve the gas-solid contact efficiency and find an
effective initiator. In general the approach is carried out in fluidized beds, utilizing UV
light as the initiator. But, the UV light is too easily shielded by PVC particles and the
capability of initiation is weakened.
So, finding a more effective and cleaner initiator for the gas-solid chlorination method
is of great importance. It is reported that the typical mechanism of PVC chlorination is
a series of free radical reactions (4). It was proposed that cold plasma could be an
effective initiator instead of UV. Cold plasma can be comprised of many kinds of ions,
radicals, UV light, etc. Researchers have shown that cold plasma can be widely
applied in the surface treatment of polymer materials (5-6). The mechanism
showed that plasma could activate the surface of polymers and reactive gas
simultaneously. However, the chlorine absorbed on the surface of a PVC particle
must migrate into the core of the particle to chlorinate the bulk of the particle,
which is assumed to be a slow diffusion-like process (7). Therefore, the
chlorination process can be decoupled into two steps: the first step is the initiation of
chlorination by plasma, and the second step is the chlorine diffusion from the surface
to the inside of particles in a chlorine atmosphere. In this work, we proposed a novel
CPVC synthesizing method in the Plasma Circulating Fluidized Bed Reactor
(PCFBR).
EXPERIMENTS
First, a fixed-bed DBD reactor was employed to examine the feasibility of the CPVC
synthesizing method. PVC particles were chlorinated with/without plasma at 100 C.
During chlorination, the plasma power source was turned on for 1 minute and then
turned off for 10 minutes to simulate the process decoupling method. The power
density of the plasma was 8.1 W/cm3 at atmospheric pressure, and the working
frequency was 13.8 KHz.
A PCFBR was designed to synthesize CPVC as shown in Figure 1. The riser was
assembled by two 0.5 m long straight coaxial quartz tubes with a gap of 4 mm, and
the thickness of quartz tubes was ~2 mm. An iron bar was inserted into the inner tube
as one electrode while some copper was wound outside the outer tube as the other.
One electrode was connected to the DBD power source (CTP-2000K, Nanjing
Suman Electronics Co., Ltd), the other electrode was grounded. The plasma was
generated by means of double–dielectric barrier discharge method inside the gap of
two tubes. The accompanying bed was made of quartz, the same as the riser. The
particle circulation rate was controlled by the flow rate of carrier gas. The chlorine
gas had a purity of 99.999%, and the other gases including Ar and N2 had a purity of
99.9%. The waste gas from the reaction unit was treated by an alkali solution.
Waste gas Alkali

Solution
Electrodes
Plasma
generator
MFC
Cl2
Thermostat Ar
Cl2
N2
Figure 1 Schematic drawing of the plasma circulating fluidized bed reactor (PCFBR)
Approximately 70 g of PVC particles (SG-5 provided by Xinjiang Tianye Co. Ltd.) with
~150 m diameter were added to the accompanying bed. The whole apparatus was
purged with N2 gas in order to exhaust the oxygen in the system and fluidize the
particles. The accompanying bed was heated up from room temperature to 70 oC,
and then the reactant gas, e.g., the mixture of chlorine and N2, was injected into the
accompanying bed from the bottom nozzle. The gas flows were fixed at 1 SLM Cl2
and 1 SLM N2. At the same time, a mixture of chlorine and Ar was injected into the
riser from the bottom nozzle with two different flow rates of 0.3/2.0 SLM and 0/2.5
SLM. The Cl2/Ar plasma was generated inside the gap between the two tubes by the
DBD method. The power density and frequency were 1.02 W/cm3, 12.7 KHz
(Cl2/Ar=0.3/2.0) and 1.24 W/cm3, 13.6 KHz (Cl2/Ar=0/2.5, respectively). The particle
circulation rate in both situations was ~0.2 g/s. After treating particles at 70 C for 20
minutes, the temperature was raised to 100 C for 40 minutes. After that, the particles
were chlorinated for different times. At the end of the experiments, the plasma
generator, chlorine flow and heating apparatus were turned off but N2 and Ar were
kept flowing for several minutes to purge the remaining chlorine in the apparatus and
that absorbed on the particles. Then the particles were exposed in the fume hood for
a day or more so that chlorine gas volatilized thoroughly.
The CPVC products were characterized by several methods. The chlorine content
was analyzed by oxygen combustion and electrification method. Each product was
characterized for at least 3 times to get an average and the error was found to be
less than 0.5%. The distribution of chlorine in CPVC particles was measured by SEM
and EDS (JSM-6460LA and EDS were made by the Oxford Instrument Company).
The microstructure of CPVC products was characterized by Raman spectrum
analysis (RM2000 made in Renishaw, UK.). In the measurements, the laser was
Ar-514, with 20X objective lens, 5 m diameter of facula, 4.7 mw and 30 s scanning
time.
Chlorination of PVC particles without a plasma initiator was carried out in the first
series of experiments in the fixed bed reactor. The chlorine content of the CPVC
particles rose to 69.7 wt% after 12 hours (see Figure 2). It proved that the
chlorination process could take place by heating PVC particles at high temperature
without any other initiator. However, it is not an effective method due to the low
reaction rate. Then an atmospheric pressure DBD plasma was employed as the
initiator in the second experimental series. It can be clearly seen that the chlorination
process was accelerated significantly by the cold plasma and the chlorine content
rose to 67 wt% in only 3 h. Considering that the working time of plasma was only 5
min/h under the intermittent operation, this proved that plasma was an efficient
initiator in PVC chlorination.
72
the ratio of Ar/Cl2=2.5/0,
66 3
1.24 W/cm , 13.6KHz
Chlorine content /wt%
68
Chlorine Content /%
the ratio of Ar/Cl2=2.0/0.3,

3
63 1.02 W/cm , 12.7KHz
64
o 60
60 Heated PVC particles at 100 C
for chlorination
o
CPVC at 100 C with
56 plasma as initiator 57
0 1 2 3 4 5
0 3 6 9 12 15
Chlorination time /h Chlorination Time /h
Figure 2 Chlorination curves of PVC Figure 3 The chlorine content of CPVC

particles with/without plasma as the by mass as a function of reaction time
initiator at 100 C in PCFBR
The results obtained from fixed-bed DBD reactor proved that the cold plasma was
able to initiate the chlorination effectively. At the same time, the method of process
decoupling was feasible and could be operated in a CFB reactor. That was, PVC
particles were treated fast in the riser by cold plasma and the chlorination was
initiated, then the chlorine slowly diffused into the core of the particles in the
accompanying bed with a relatively long residence time. Particles were circulated in
the PCFBR several times to be chlorinated sufficiently. The following discussion is
based on the experiments in the PCFBR.
The chlorine content of CPVC is shown as a function of reaction time in Figure 3.

One series of the results shows the chlorine content increasing up to 65.0% when
pure Ar was used as the carrier gas with plasma in the riser. These results revealed
that PVC can be chlorinated in the PCFBR. The total residence time of particles in
the plasma zone was only about 22.2 s during the 4-hr experiments. In fact, with
appropriate optimization of the PCFBR operation, a successful single-run of the
chlorination process would be ~1.5 hr, or even much less.
Figure 3 also indicates that under the same power input of plasma, the composition
of carrier gas in the riser is very important, because it provides the atmosphere in
which plasma is generated, and the reactive species are different in different
plasmas. So it is possible to adjust the property of plasma by changing the ratio of
Cl2/Ar. At the same time, the mechanism of chlorination is changed. For example,
chlorination can occur in the riser when Cl2 is introduced, which is different from the
case of pure Ar as carrier gas. It was noticed that the chlorine content increases
linearly as a function of reaction time in Figure 3 for the case of Cl2/Ar=2.0/0.3. This
might indicate that when introducing chlorine gas with Ar to generate plasma, not
only are the PVC particles activated, but also the surface of the PVC particles is
chlorinated rapidly in the plasma zone. However, the chlorine content increased
slowly when the chlorination time was lengthened. Another fact is that the
discharging of Cl/Ar plasma was weaker than pure Ar plasma so that the initiation
effect became weaker. Obviously, work is required for a deep understanding of the
complex mechanism and for guiding this optimization of the process design.
CPVC characterization
SEM and EDS can give a semi-quantitative result by comparing two samples under
the same conditions. The chlorine content shown in Figure 4 is the mass fraction of
chlorine. The total amount of chlorine and carbon elements (hydrogen is not included
because EDS cannot discern light elements). So this value is larger than the actual
chlorine content of CPVC. Considering that the analysis error of the instrument is
less than 5 %, in principle, the results of EDS shown in Figure 4 indicate that the
CPVC synthesized in this work has a much higher chlorine content than PVC raw
material. In addition, the scanning area was the interior of the CPVC particles, which
proved that chlorination occurred inside the PVC particles, not only on the surface.
Figure 4 Chlorine distribution in the particle of plasma synthesized CPVC (left), and
PVC raw material (right)
The microstructure of CPVC was analyzed by Raman spectral analysis. In Figure 5,

five kinds of CPVCs were analyzed, including four samples of CPVC synthesized
using PCFBR with Ar plasma as the initiator and one sample of commercial CPVC
using the aqueous suspension method. The PVC SG-5 raw material was also
analyzed for comparison. In the spectra, the characteristic peak of CPVC is at
300-500 cm-1.
25000
20000
Intensity
15000 Commercial CPVC
PECFB 4h
10000 PECFB 3h
PECFB 2h
5000 PECFB 1h
PVC SG-5
0
0 750 1500 2250 3000 3750
-1
Wavenumber cm
Figure 5 Raman spectra of PVC or CPVCs

In the chlorination process, the increase of the amount of -CCl- can be seen clearly.
At the same time, there is essentially no -C=C- group in all of the samples, which has
a signal at 1650 cm-1. This proves that almost all the CPVC samples have a fine
microstructure. But with it is still evident that there is a very weak -C=C- signal in the
spectrum of an every CPVC sample and no signal in the spectrum of PVC, which
reveals the influence of Elimination-Addition mechanism. To sum-up, it was shown
that chlorination occurred in the bulk of the PVC particles and that the microstructure
of plasma synthesized CPVC was comparative to the commercial product by the
Raman analysis.
CONCLUSION
In this article, a novel CPVC synthesizing method was proposed that employed
plasma as the initiator and which operated in a circulating fluidized bed. The
chlorination process consisted of two steps: a fast initiation step and a slow
chlorination process. In the chlorination process, the residence time of particles in the
plasma zone was only about 22 seconds in the total 4-h reaction time, which
indicated that plasma had high initiation efficiency. In the experiments so far, the
chlorine content of CPVC product reached 65.0%. Characterizations by SEM and
Raman spectrum show that the bulk of the particles were chlorinated. Moreover, the
particle product had a uniform chlorine distribution inside the particles and a fine
microstructure. The objective of this work was to propose a novel CPVC production
method with preliminary demonstration of feasibility. This would also open a specific,
potential area for CFB applications. Still, there is lots of work to do in the future, for
example, to investigate the operational performances of PCFBR, plasma-related
design and optimization, influence of PVC particle properties on the chlorination
process, etc.
ACKNOWLEDGEMENT
Financial support from the National Science and Technology Key Supporting Project
(No.2009BAC64B09) and the Program for New Century Excellent Talents in
University are acknowledged.
REFERENCES
1. Liu, H., and Zhang, X.M. (2008). “Review on chlorinated polyvinyl chloride.”
Polyvinyl Chloride, 36 (11), 9.
2. Alan, O. J., and Robert, V. G., Process for chlorination of PVC in water without
use of swelling agents: US, 4412898 [P], 1983
3. Wakabayashi, T., Kobayashi, Y., and Tujii, I., Process for the proparation of
chlorinated polyvinyl chloride resin: US, 3534013 [P], 1970
4. Lukas, R., Svetly, J., and Kolinsky, M. (1981). “Structure of chlorinated poly (vinyl
chloride) X. Conclusions on the chlorination mechanisms.” Journal of Polymer
Science: Polymer Chemistry Edition, 19, 295.
5. Arpagaus, C., Sonnenfeld, A., and Von Rohr, P. R., (2005). “A downer reactor for
short-time plasma surface modification of polymer powders.” Chemical Engineer
Technology, 28 (1), 87.
6. Arpagaus, C., Rossi, A., and Von Rohr, P. R., (2005). “Short-time plasma surface
modification of HDPE powder in a plasma downer reactor – process, wettability
improvement and ageing effects.” Applied Surface Science, 252, 1581.
7. Wachi, S., Morikawa, H., and Inoue, H. (1988). “Conversion distribution in
diffusion-governed chlorination of poly (vinyl chloride).” AICHE Journal, 34 (10),
1683.
A PRACTICAL MODEL FOR A DENSE-BED
COUNTERCURRENT FCC REGENERATOR
Yongmin Zhang, Chunxi Lu
State Key Laboratory of Heavy Oil Processing, China University of Petroleum, Beijing,
102249, P. R. China
Abstract
In this study, a new practical countercurrent regenerator model for in-situ FCC
operation optimization was proposed. A three-zone-and-two-phase gas model and a
new two-CSTR-with-interchange model were used to give better descriptions on the
gas and solids flow patterns, addressing the region-dependent mass transfer rates
and the freeboard effect on catalyst regeneration. The model coupled mass and heat
balances, hydrodynamics and reaction kinetics. The modeled results are in
reasonable agreement with the commercial data from an industrial FCC regenerator
under both partial and full CO combustion modes.
INTRODUCTION
A regenerator is an indispensable part of a FCC unit, acting as a fluidized-bed reactor

to burn the coke deposited in the spent catalyst and recover its cracking activity. An
ideal FCC regenerator requires very low levels of carbon content in regenerated
catalyst (CCR) (0.05~0.1 wt%) with minimized air consumption and maximized coke
burning intensity (CBI) (usually defined as weight of coke burned for a given catalyst
inventory and a given period). A practical regenerator model based on sound
understanding of its intrinsic hydrodynamics, mixing and reaction kinetics is
undoubtedly valuable to optimization of its design and operation.
There have been several published studies on modeling dense-bed FCC

regenerators (1-7). However, they all failed to describe the gas and solids flow
patterns properly in the three zones (grid zone, dense-bed zone and freeboard zone)
of a regenerator simultaneously, resulting in modeled results divergent largely from
experimental facts and low reliability and predictability. Some of them (1-5) used the
simple Orcutt fluidized-bed model (8) to model gas flow in the dense bed, which
falsely modeled the reactant gas concentration in the emulsion phase to be a
constant level. Otherwise, only Lu (5) and De Lasa et al. (7) considered the large
amount of particles entrained in the freeboard and the associated reactions. However,
Lu (5) improperly modeled the solid flow in the freeboard with a
multiple-CSTR-in-series model, which over-predicted the freeboard reaction. The
freeboard model of De Lasa et al. (7) was a particle-trajectory based model, which
was too complex to use in engineering practice.
The goal of this study is to establish a modified model for a countercurrent

regenerator. This model has a modified hydrodynamic model that provides better
-1-
descriptions for gas and solid flows in both dense bed and freeboard. Otherwise, its
structure still remains simple enough to be a practical engineering tool.
MODEL SCHEME
y O , out u2 At2
2
free-
freeboard
board CCf
Fs,df Fs,df
y O , z=H u1At1 dense bed
Fs0
2 f
K be
bubble emulsion
void dense bed
CCd
jet kj emulsion
y O , z=0 u1At1
2
Fs0
(a) (b)
Fig. 1 Gas and solid flow patterns in the countercurrent FCC regenerator model: (a) gas flow pattern; (b)
solid flow pattern
A countercurrent regenerator is usually the preferred choice in a FCC unit for its better
performance, where catalysts are usually injected to the top of its dense bed by a
specially designed catalyst distributor, and withdrawn through the bed bottom. Figure
1 illustrates the hydrodynamic models describing the gas and solid flow patterns in
this study. For the gas flow in the dense bed, a simple two-phase bubbling-bed model
proposed by Chavarie and Grace (9) is used. This is a two-phase model with a
“stagnant” emulsion phase, i.e. gas in the emulsion phase coming only from mass
transfer from the bubble phase and without axial dispersion. Different from the Orcutt
model (8), there is an axial gradient for the reactant gas concentration in the emulsion
phase in agreement with experimental facts. Axially, two zones were partitioned in the
dense bed to address the different gas transfer rates between emulsion and voids in
the bubbling zone and jets in the jet zone. In the freeboard, the gas phase becomes a
continuous phase, where interphase mass transfer becomes less important than in
the dense bed. Gas flows in the jets, voids and freeboard were all modeled as plug
flow without back-mixing. For an irreversible first order reaction A  B with negligible
volume change, mole balances on A in the bubble phase and emulsion phase yield,
respectively,
dC Ab (1)
u0 + kbeab db (C Ab - C Ae ) + kr f sbC Ab = 0 ,
dz
kbeabdb (C Ae - C Ab ) = kr fseC Ae . (2)
-2-
For the solids flow, a two-CSTR-with-interchange model shown in Fig. 1(b) was
adopted. A distinct difference in this model lies in its different
d t2
manipulation on solid flow in the freeboard. In a typical
fluidized bed, particles in the freeboard come mainly from
bubble eruptions on the bed surface. Particle concentration
freeboard
and upward flux decrease exponentially with increasing
distance from the bed surface. Only a negligibly small
fraction of particle leaves from the freeboard top and is
Fs0 C Cs
CHs u1At1 QH O
captured by cyclones. This demonstrates that most solid 2
inventory in freeboard exists within a small-height zone near d t1

the bed surface, i.e. the so called splash zone. In this zone,
violent mixing due to strong gas flow turbulence and large bubbling
zone
solids exchange rate between the dense bed and the
freeboard can be expected. Therefore, solids flow in jet zone
freeboard was modeled as a separate CSTR reactor with F s0 CCr
u1At1
solid exchange with the dense bed in this model. Physically,
Fig. 2 Geometry model for
freeboard in this model is to provide particles with additional
an FCC regenerator with
time to burn coke with negligible interphase mass transfer
an expanded freeboard
resistance.
Other simplifications are assumed to facilitate the modeling. First, the hydrogen
content of the coke is assumed to combust instantly near the bed surface due to the
much higher combustion rate of hydrogen (usually an order faster than carbon
combustion) (10). Second, the structure of the FCC regenerator is simplified as
showed in Fig. 2. The bottom bed section is always assumed to have the same height
as the dense bed, Hf, whereas the expanded top section is assumed to be a cylinder
of diameter dt2 and height Ht-Hf.
MODEL SETUP
Kinetic Model
Due to the simplification for hydrogen combustion, only carbon combustion needs to
be considered in this model. Carbon combustion can be described by
. 2b +1 æ b ö÷ æ 1 ö÷ (3)
C+ O2  çç ÷ CO2 + çç ÷ CO
2 (b +1) ç ÷
è b +1ø èç b +1ø÷
where  is the ratio of CO2 to CO released.  is affected by many factors including
catalyst type, feedstock, temperature, contents of oxygen and CO promoter etc. In
this model,  is simply determined as the ratio of CO2 and CO concentrations in the
flue gas of the modeled regenerator. This also simplifies the complex homogeneous
and heterogeneous CO combustion procedures in actual conditions. The carbon
combustion rate is estimated by (11)
-3-
æ 1.422´105 ö÷
kC = 2.967 exp çç- ÷. (4)
çè RT ø÷÷
Hydrodynamics Model
Two important parameters in the grid zone, jet length and jet diameter, are
determined by Lu‘s correlations (5).
 p d p 0.273  g uor d or 0.654 uor2 0.408 , (5)
Lj  141.85d or ( ) ( ) ( )
 g d or g gd or
uor2 0.332 . (6)

D j  0.388d or ( )
gd or
The average bed density is also determined based on the measured industrial data
as expressed by Eqs. (7) and (8). The derivative in Eq. (8) is derived from a
correlation of Cai et al. (12)
¶rB (7)
rB =rB,exp + (u1 - u1e )
¶u1
¶rB ¶ éêërp (1- e)ùúû 3n (rp - rB,exp )

= =- (8)
¶u1 ¶u1 u1
The dense bed height and the axial particle concentration profile are determined
based on Zhang et al. (13), which considered the solid mass balance of the whole
regenerator. The solid fraction in the freeboard is expressed as
fs =f s* + ( f s0 -fs* ) exp (-azf ) , (9)
where fs* is the saturated solids fraction, determined by measured cyclone inlet
concentration in this study, fs0 is the initial solid fraction at the bed surface and
determined by
0.3  u1  umf 1   mf  At1 . (10)
fs0 
At2ub
Here, ub is void rise velocity determined by the ratio of superficial gas velocity and
bubble fraction in the dense bed, i.e. u1/　b; the exponent coefficient 　is determined
by 0.7/u2 according to Zhang et al. (13). Based on mass balance in the regenerator,
H t  Hf
B H f At1  p At2  fs dzf  M s , (11)
0
the dense bed height Hf can be determined.
Gas transfer coefficient between jet and emulsion is estimated by Lu’s correlation (7),
-0.504 0.068
æ d u r ÷öæ u 2 ÷ö æ Lj ö÷
0.905
æ ö
k j = 0.48 ççç or or g,j ÷÷ççç or ÷÷ çç ÷÷ çç d or uor rg,j ÷÷ . (12)
çç u ÷÷
èç Lj ÷øèç gLj ÷ø çè d
or ø
÷ è g,j ø
-4-
Bubble-emulsion gas transfer coefficient is estimated by De Groot’ s correlation (14),
u1 , (13)
K be = kbe ab =
0.67 H f0.5 d t10.25
which omits the need to know the average bubble size, a very difficult parameter to
estimate in large-scale industrial fluidized beds.
Mass and Heat Balances
To determine the profiles of gas components, carbon content in the catalyst and
temperature in the regenerator, the oxygen balance, carbon balance and heat
balance are needed in the model. Due to page limit here, these procedures are only
briefly introduced in the following text.
During the regeneration process, changes of gas compositions, carbon content and
temperature are interrelated. Their values need to be solved together. Oxygen
balance in the dense bed is based on Chavarie and Grace (14) with consideration of
different mass transfer rates in the grid and bubbling zones. In the freeboard,
interphase mass transfer is neglected, with reaction kinetics as the controlling factor.
With oxygen concentration, concentrations of CO2 and CO are readily known
according to the reaction formula shown in Eq. (3). The profile of carbon content is
determined according to the solids
raw data
flow model and the consumption of
oxygen. In this model, the carbon data initialization
contents in the dense bed and
Td0 Tf0
freeboard are constant due to the
completely mixed assumption. With hydrodynamics
higher mass transfer rate, the carbon
CCd0 CCf0
content in the freeboard is a little
lower than in the dense bed. The gas component balance
heat balance needs to consider the carbon balance
heat input from combustion of carbon
CCd0 ≠ CCd1
and hydrogen, heat to heat up the CCf0 ≠ CCf1
CCd1 CCf1
influent air and spent catalyst, heat heat balance
loss to atmosphere from the outside
Td0 ≠ Td1
shell, and heat removed from catalyst Td1 Tf1 T ≠T f0 f1
coolers. output
Solving Algorithm Fig. 3 Flow chart of model program
This model is programmed in Matlab language using a modularized scheme and

solved by an iterative method as shown in Fig. 3. There are seven modules and two
iteration loops. To establish a model for optimizing the operation of a specified FCC
regenerator, a calibration procedure is required to determine key unit-dependent
parameters based on existing industrial data. Then, basic operating data can be
-5-
changed to see their effects on the performance of the regenerator and to determine
optimized operating parameters.
MODEL VALIDATIONS AND DISCUSSION

Table 1 A comparison of the modeled results and industrial data
Items Partial mode Full mode
Catalyst inventory, ton 185 160
Superficial gas velocity in the dense bed, m/s 0.85 0.93
Superficial gas velocity in the freeboard, m/s 0.48 0.52
Items for comparison Model Exp. Model Exp.
Bed height of dense bed, m 7.91 8.05
3
Bed density, kg/m 278 276 221 220
3
Freeboard density, kg/m 10.9 12 14.9 14
Dense bed temperature, °C 660 662 689 690
Freeboard temperature, °C 669 670 696 699
Carbon content of the spent catalyst, (wt) % 1.49 1.74
Carbon content of the regenerated catalyst, (wt) % 0.18 0.15 0.038 0.05
CBI, kg/(h.ton (cat.)) 102.1 105.7 112.8 106.7
O2 0.89 0.8 3.31 3.1
Components of flue gas (dry), v% CO 1.61 1.6 0.31 0.3
CO2 16.88 16.8 15.8 15.4
Industrial data from a FCC unit in Luoyang Petrochemical Corporation, Sinopec were
used to compare with the modeled results. This FCC unit has a coaxial
reactor-regenerator layout, processing 1.4 million tons of atmospheric residue per
year. A single-stage countercurrent regenerator is used to regenerate the spent
catalyst. The regenerator was first operated in the full CO combustion mode with a
CO promoter. Later, in order to increase the processing capacity and decrease the
main air flow rate, the regenerator was revamped to partial CO combustion mode with
reduced air flow rate and without CO promoter. An advantage of this model is that
only one fitting parameter, i.e. the interchanging solids flux between the dense bed
and the freeboard, Fs,df, is used, which was determined based on the difference of
temperature in the dense bed and freeboard. With a same Fs,df, both regeneration
modes are modeled. The modeled results are compared with industrial data in Table 1.
The main modeled hydrodynamic and performance results are in reasonable
agreement with the industrial data, demonstrating the feasibility of this model.
With this model, the axial profiles of voidage, temperature, gas components and
carbon content can be predicted, as shown in Fig. 4 for a typical partial CO
combustion mode. It can be seen that most of the solids inventory in the freeboard is
-6-
concentrated within a ~2 m high from the bed surface, where solids mixing is vigorous
and a large solids exchange flux exists between the dense bed and freeboard.
Therefore, there is only a small temperature increase in the freeboard, as seen in Fig.
4(b). Due to the different mass transfer rates, oxygen concentration decreases much
sharply in the grid zone than in the bubbling zone. In the grid zone, the difference of
oxygen concentration in the emulsion and dilute phases is much lower than in the
bubbling zone. Due to higher mass transfer rate, carbon burns more efficiently in the
freeboard, as indicated by the lower carbon content shown in Fig. 4 (d).
1.2 700
T
1.1  680
Temperature, C
dense bed
o
Voidage, -
1.0 660
0.9 640
dense bed freeboard
freeboard
0.8 620
0.7 600
0 5 10 15 20 0 5 10 15 20
Height, m Height, m
(a) (b)
20 0.20
16 dense bed yCO2 CC

Carbon content, w%
0.18
Mole content, %
12 yH2O
0.16
8
yb,O2
dense bed
0.14 freeboard
4 freeboard
ye,O2 yCO
0 0.12
0 5 10 15 20 0 5 10 15 20
Height, m Height, m
(c) (d)
Fig. 4 Predicted profiles of (a) voidage, (b) temperature, (c) gas composition, and (d) carbon
content under partial CO combustion mode
CONCLUSION
In this study, a modified countercurrent FCC regenerator model is proposed based on
modified gas and solids flow patterns. The gas flow pattern in dense bed employs the
“two-phase bubbling bed model” proposed by Chavarie and Grace (8), which can
predict gas concentration profiles in better agreement with experimental facts. The
modification in solids flow patterns focuses on the solids flow in freeboard, which was
modeled as another CSTR exchanging solid with the dense bed. The model was
applied to an industrial FCC regenerator operated under both full and partial CO
-7-
combustion modes with agreeable modeled results obtainable with industrial data for
both modes.
NOTATION
At bed area, m2  coefficient, 1/m
C gas concentration, - b interphase area per volume of
CC carbon content, - bubble, m2/m3
d diameter, m  CO2/CO, -
dt bed diameters, m b bubble fraction, -
fs solid volume fraction, - ε void fraction, -
Fs,df interchange solid rate, kg/m2.s  density, kg/m3;
kbe bubble-emulsion mass transfer Subscripts
coefficient, m/s b bubble/bed
Kbe bubble-emulsion mass transfer e emulsion
coefficient, 1/s d dense bed
kj jet-emulsion mass transfer s solid
coefficient, kg/m2.s f freeboard
kf reaction constant, 1/s g gas
R gas law constant, kj/(kmol.K) j jet
T temperature, K mf minimum fluidization
Hf dense bed height, m p particle
Lj jet length, m or orifice
M mass, kg 0 initial
u superficial gas velocity, m/s 1(2) dense bed (freeboard)
y concentration, - * saturated
z height, m
REFERENCES
1. Ford, F. D., Reinmen, R. C., Vasalos, I. A., and Fahrig, R. J., 1977. Chem. Eng. Prog. 73 (4): 92.
2. De Lasa, H. I., Errazu, A, Barreiro, E. And Solioz, S., 1981. Can. J. Chem. Eng. 59: 549-553.
3. Faltsi-Saravelou, O., Vasalos, I. A. And Dimogiorgas, G., 1991. Comp. Chem. Eng. 15: 647-656.
4. Filho, R. M., Batista, L. M. F. L. and Fusco, M., 1996. Chem. Eng. Sci. 51: 1807-1816.
5. Lu, C., 1996. Doctoral dissertation, China University of Petroleum, Beijing, China. (in Chinese)
6. Lee L. S., Yu, S. W., Cheng, C. T. and Pan, W. Y., 1989. Chem. Eng. J. 40: 71-82.
7. De Lasa, H. I. and Grace, J. R. 1979. AIChE J. 25: 984-991.
8. Orcutt, J. C., Davidson, J. F. and Pigford, R. L., 1962. Chem. Eng. Prog. Symp. Ser. 58: 1–15.
9. Chavarie, C. and Grace, J. R., 1975. Ind. Eng. Chem. Fundam. 14: 75-91.
10. Wang, G., Lin S., and Yang G., 1986. Ind. Eng. Chem. Proc. Des. Dev. 25: 626.
11. Dong, X. and Hao, X., 2006. Petroleum Refinery Engineering. 36 (6): 7-9. (in Chinese)
12. Cai, P., Jin, Y., Yu, Z. Q., and Wang, Z. W., 1990. AIChE. J. 36: 955-956.
13. Zhang Y. M., Lu C. X., Shi M. X., 2008. Chem. Eng. Tech. 31, 1735-1742.
-8-
INVESTIGATION ON THE HYDRODYNAMIC PROPERTIES IN
THE EXTERNAL LOOP OF CIRCULATING FLUIDIZED BED
WITH A LOOP SEAL
Xuan Yao, Tao Wang, Hairui Yang, Hai Zhang, Qing Liu, Junfu Lv, Guangxi Yue
Key laboratory for Thermal Science and Power Engineering of ministry of Education,
Tsinghua University, Haidian District, Beijing 100084, China
T: 86-1-62773384; F:86-10-62781743;E:yhr@tsinghua.edu.cn
ABSTRACT
The pressure balance and mass balance are influenced by the characteristics of
different components in the loop of a circulating fluidized bed (CFB). Experiments
were conducted in a 4.3 m high cold laboratory CFB test rig with a loop seal. With a
fixed bed inventory and superficial gas velocity, the pressure drop of the loop seal
decreased with increasing aeration, thus causing an increase in the solid circulation
flux (Gs). Correspondingly, the pressure drop in the riser became higher with
increasing Gs; the pressure drop of the cyclone had a non-linear relationship with
Gs, and the transition point was determined in the experiment. Using the laser fiber
and gas tracer method, hydrodynamic characteristics in the standpipe were directly
measured. It was found that the pressure gradient, voidage, and solid height in the
standpipe were affected by the pressure balance in the whole loop. By adjusting the
gas flow rate and direction in the standpipe, the gas-solid slip velocity and pressure
gradient changed correspondingly. Therefore, the standpipe could maintain the
pressure balance and realize self-equilibrium of the loop by absorbing the pressure
drop variations of other parts in the system.
INTRODUCTION
Circulating fluidized bed (CFB)normally consists of the riser, cyclone, standpipe and
solid recycling valve. The standpipe and recycling valve can overcome the high
pressure difference and recycle particles collected by cyclone to the bottom of the
riser. The standpipe often has the function to prevent gas bypassing.
Non-mechanical valves, such as loop seal, L valve, are commonly used in industrial
CFB boilers as they can work under the harsh conditions of high temperature and
pressure. The solid circulating flux is commonly controlled by changing the aeration
rate in the valves.
Though a number of studies have been conducted on gas-solid flow in the riser and
cyclone [1-5], there are few studies on the hydrodynamic properties in the external
loop of CFB system, especially for the influence of riser operation conditions on the
performance of the recycle valve and standpipe. Basu [1] built a model to describe
the CFB external loop pressure drop and analyzed the influence of aeration rate,
1
riser velocity and Gs on the standpipe pressure gradient. However, the gas flow
direction and vodiage in the standpipe were not measured directly. Monazam[2]
studied the influence of bed inventory, riser velocity and aeration rate on GS and
confirmed that the performance of the loop seal and standpipe can’t be studied
ignoring the influence of other components in the whole system.
Standpipe is a special part of the CFB system. It has the function to absorb the
pressure variation of other components in the system and the gas bypassing can be
prevented by designing the standpipe correctly. However, there is very little
literatures on the performance of the standpipe in the CFB system. The flow state in
the standpipe is still in controversy and there is little evidence to validate the
different viewpoints [1,6].
In this paper, experiments was conduced in a 4.5 m high CFB test rig with a loop
seal to study the influence of operating conditions on the performance of
hydrodynamic properties in the external loop, including the loop seal and standpipe.
Laser fiber and gas tracer methods were applied to measure the flow behavior in the
standpipe directly, including the voidage and gas
flow direction.
EXPERIMENTAL
Experimental test rig
Experiments were conducted in a CFB cold test rig

as shown in Fig.1. The rig consisted of a distributor,
a riser, a cyclone, a standpipe and a loop seal. The
riser had a cross-section area of 0.1x0.1 m2 and a
height of 4.5m. The cyclone was of high separation
efficiency. The standpipe had a height of 3.0m and
a diameter of 0.08m and connected the riser with a
loop seal [7]. The dimension of the loop seal was
shown in Fig.2. 20 pressure taps were installed at
different heights along the solid circulation loop to
measure the pressure drop online. The fluidizing
gas rate and loop seal aeration rate, Q, were
measured by gas flow meters. Two methods were
used to measure the solids circulation flux, GS. One
was based on the time for the recirculating solids to
accumulate to a certain height in the standpipe
after a sudden close of a butterfly valve installed in
the standpipe. The other method used a
self-designed measuring device placed under the Fig. 1 Schematic diagram of
experimental test rig
2
cyclone. All experiments were carried out at ambient temperature and atmospheric
pressure. The bed material was quartz sand, its physical properties are listed in
Table 1.
Table 1 Physical properties of the bed material

Real Bulk Minimum Minimum Sauter
Size range
density voidage voidage fluidization velocity diameter
2625 kg/m3 0.50 0.58 0.09 m/s 200-500μm 360μm
Flow behavior measurement in the standpipe and loop seal
To study the gas flow behavior in the

standpipe, high purity CO2 gas was used
as the tracer. As shown in Fig. 2, CO2
was injected into the system at Point A,
and CO2 concentration at Tap 1, 2 and 3
were simultaneously measured by a CO2
detecting system with 3 channels, each
equipped with a sampling probe, a CO2
sensor (GSS-C20) and a vacuum pump.
A laser fiber was used to measure the
solid volumetric fraction at Taps 2 and 3.
Signals from the CO2 sensors and laser
Fig. 2 Measurement system of flow
fiber were recorded online through a
behavior in loop seal and standpipe
data acquisition system.
In the first test, it found that CO2 concentrations at different locations in the same
cross section were nearly the same, so the gas and solids in the standpipe were
regarded as well mixed horizontally. Shown in Fig.2, in the control volume enclosed
by the dot lines and solid walls, the gas balance can be expressed as following
equations when CO2 is injected with a certain volumetric flow rate q at Point A.
According to Eqn.1and 2, QV and QH can be calculated with known Q, q, C1 and C3.
QV + QH = Q + q (1)
QV × C3 + QH × C1 = q (2)
DISCUSSION
Riser pressure drop
The solid circulation flux GS of the system has significant influence on the mass
balance in the CFB reactor, and directly determines the performance of the system.
As shown in Fig. 3, GS increases with the aeration rate, Q, in the loop seal. After Q
increases to a critical value, GS no long changes with aeration rate and maintains at
3
the maximum rate about 45kg/m2s.
GS can be estimated by the particle suspension density in the upper region of the
riser. GS = ρ s(1 − ε ) (uriser − ut) .Therefore, GS can be used characterize the
suspension density in the upper riser. Fig. 4 shows the solids hold up distribution in
the riser at Uriser=5.0 m/s. With increasing Gs, particles hold up in the riser becomes
denser. Former studies have shown that, with increasing Gs at a certain riser
fluidizing velocity, the flow in the riser will transition from dilute phase pneumatic
conveying to the fast fluidization state [8]. In the fast fluidized bed, the voidage in the
dense zone and upper dilute zone are held stably, while the height of dense zone
ascends gradually and the voidage in the transition zone increases.
50
2
Gs=15.7 Kg/m s ,△P=515 Pa
4 2
40 Gs=27.7 Kg/m s ,△P=950 Pa
bubbling 2
Gs=38.1 Kg/m s ,△P=1500 Pa
transintion point 2
Gs=39.8 Kg/m s ,△P=2542 Pa
Riser hieght (m)
3
30 2
Gs (kg/m s)
Gs=45.6 Kg/m s ,△P=3670 Pa

2
2
Gs=45.7 Kg/m s ,△P=5020 Pa
20 2
Uriser=5.0 m/s
10 1
0
5.0 5.5 6.0 6.5 7.0 7.5 8.0 0
0.00 0.05 0.10 0.15 0.20 0.25 0.30
3
Areation rate (m /h) Solid hold up 1-ε
Fig. 3 Variation of GS with Q of loop seal Fig. 4 solid hold up distribution in riser
The pressure drop of the riser △Pr is approximately equal to solids gravity pressure
drop, which is determined by solids inventory in the riser. Fig. 5 shows the
relationship of △Pr and Gs. △Pr and Gs represent proportional relationship, but after
the △Pr is larger than 3.0KPa, Gs maintains at about 45kg/m3s. According to Figs 4
and 5, when Gs reaches the critical value 45kg/m2s, solid hold up of upper and
bottom region of the riser remains unchanged. The increase of solids inventory in
the riser only causes height of dense phase zone increase. Overall solids hold up
distribution fit the S type curve of fast fluidization, and the saturated carrying rate
under 5.0m/s in the paper is about 45 kg./m2s.
Cyclone characteristic
The pressure drop or resistance of the cyclone △Pcyc has a square relationship with
the entering gas velocity. However, △Pcyc is also influenced by solids concentration
CS. CS is defined as the solids mass in one cubic meter of fluidizing gas. It can be
calculated with GS by CS = GS AS / (Ar uriser).
In this paper, besides the traditional steady method, a transient method is used to
4
study the characteristic of the cyclone pressure drop. At a specific Uriser, after a
steady state with a large Gs was maintained for a few minutes, the loop seal
aeration was suddenly cut off, the bed inventory was then elutriated out of the riser
and accumulated in the standpipe. The flow regimes in the riser changed from fast
fluidization to dilute convey regime with decreasing Gs, until the riser was empty of
particles. This method is simple and has better reproducibility than traditional steady
method.
Fig. 6 shows the characteristic of the cyclone at different Uriser. The comparison
between the steady method and transient method further verifies the reliability of the
transient method.
1000
6000
steady transient
Uriser method method
5000 800 6.0 m/s
5.0 m/s
4000 4.0 m/s
△Pcyc (Pa)
600
△ Pr (Pa)
3000
2000 400
1000
200
0
0 10 20 30 40 50 0 1 2 3 4 5
3
2
Gs (kg/m s) Cs(kg/m )
Fig. 5 Variations of △Pr with Gs Fig. 6 character of cyclone △Pcyc
Flow behavior of loop seal and standpipe
It’s generally believed that all the aeration gas passes through the loop seal into the
riser. However, industrial operation has verified that the gas-bypassing phenomenon
in standpipe can’t be ignored. As shown in Fig. 7, the actual gas flow rate across the
loop seal is not equal to the aeration rate. With a small aeration rate,Q, QH through
the loop seal is close to the aeration rate, account for more than 95% percent of Q.
However, with increasing Q, more gas goes up through the standpipe, QH/Q rapidly
decreases.
A loop seal can be divided into a horizontal part and a vertical part based on its
physical structure, as shown in Fig.2. The gas-solid flow in the horizontal part
belongs to the transport state, the resistance of which is mainly caused by the
friction among particles and the wall. With increasing aeration rate, the pressure
drop of the horizontal section (P17-P18) increases due to higher GS. The flow in the
vertical section is in the bubbling bed regime. With higher aeration rate, as QH/Q
decrease, the ejecting height of particle decreases rapidly due to less QH. This
results in the reduction of △Plsl, as shown in Fig. 7.
5
Therefore, the loop seal characteristics are closely related to the flow state in the
120 120
Voidage ε △P/L (kPa/m) Height (cm)

Gas flow ratio (%)
110 QH/Q 80
solid height
100
40
90
12
0
80 standpipe pressure
70 8 gradient
60 4
2000
50
loopseal 0
voidage
1500 0.56
△P (Pa)
0.52
1000
vertical 0.3 Usl
500 hozirontal Ug
U (m/s)
0.2
Us
0 0.1
5.0 5.5 6.0 6.5 7.0 7.5
Areation rate (m /h)
3 0.0
5.0 5.5 6.0 6.5 7.0 7.5
Areation rate (m 3/h)
Fig. 7 the performance of loop seal
Fig. 8 flow behavior of standpipe
(Uriser=5.0 m/s)
(Uriser=5.0 m/s)
standpipe, which affects the actual gas passing through the loop seal. In this paper,
the pressure drop gradient, voidage and gas flow were directly measured.
As shown in Fig. 8, when Gs increases with increasing aeration rate, Q, at fixed Uriser
and bed inventory, IV, the mass of solid and thereby solid height in the standpipe
decrease because more solids accumulate in the riser. At the same time, the
pressure gradient in the standpipe increases. This is a special feature of transient
packed bed flow [9], which is related to the pressure gradient and gas-solid slip
velocity USl. According to the experimental measurement of voidage by laser fiber
and gas flow rate measured by gas tracer, the slip velocity USl can be calculated by
the equation USl=GS/ρp(1-ε)+Ug/ε[9]. With increasing aeration rate, particle velocity,
US, increases due to higher GS. At the same time, the upward gas flow rate in the
standpipe, QV, also increases. Therefore, the slip velocity will increase with
increasing aeration rate. Although the solid height decreases, the solid seal can
provide a pressure head because of the increasing pressure gradient and slip
velocity USl. With increasing aeration rate, the upward gas flow, QV, keeps on
increasing and the voidage gradually approaches to the minimum fluidization
voidage. With very high aeration rates, upward flowing bubbles can be visually
observed and the flow reaches the bubbling state.
Pressure balance of the CFB external loop
As shown in Fig. 9, at fixed riser fluidizing velocity, more bed material accumulates
in the riser with increasing aeration rate. As a result, △Pr increases. At the same
6
time, both the pressure drop gradient
and total pressure drop, △Psp, in the 6000
standpipe increase. Under stable
operation condition, the pressure 5000
balance of the CFB system can be

4000
expressed as △Pr + △Plsl + △Pcyc = △Psp
△Pr (Pa)
△Psp. Whenever pressure drop of 3000
any other parts changes, the pressure
gradient △P/L and Usl in the standpipe 2000 △Plsl △Pr
change correspondingly to rebalance
the system. Therefore, the standpipe 1000
△Pcyc
has the ability to keep pressure
0
balance in the CFB by adjusting inner 5.0 5.5 6.0 6.5 7.0 7.5
3
flow behavior. Its characteristic is Areation Rate (m /h)
greatly affected by the operation
Fig. 9 Variations of pressure drops around
conditions of the riser and other parts,
the CFB loop
and should be studied in the external
loop of CFB system [10].
CONCLUSION
The flow behavior of a CFB external loop, including loop seal and standpipe is
schematically studied in this paper. It found that with a fixed bed inventory and
fluidizing velocity, the pressure drop of the riser increases with solid circulation flux
because more particles accumulate in the riser. When Gs reach a critical value,
solids suspension distribution can be described by the S type curve of the fast
fluidization. The pressure drop of a cyclone depends on the riser gas velocity and
solids concentration. The cyclone pressure drop first decreases and then increases
with suspension solid concentration. The actual gas flow ratio QH/Q through the loop
seal decreases with increasing aeration rate, while the upward flow gas rate in the
standpipe increases.
Voidage in the standpipe increases and the flow state gradually transitions to the
minimum fluidizing state from packed bed flow. The flow behavior in the standpipe
adjusts to conditions in the whole CFB system. The standpipe maintains the
pressure balance by changing the slip velocity and pressure gradient to provide the
required pressure head with lower solids height.
Because the CFB system used in this paper is an inventory constrained system, the
results, especially for the transition points, may be different under different bed
inventories. At same time, the solids properties also have an influence on the results.
These factors will be studied in the future studies.
7
ACKNOWLEDGMENT
Financial support of this work by High Technology R&D (863) (2009AA05Z302) is

acknowledged.
NOTATION
Ar section area of riser, m2 As section area of standpipe, m2
CS solids concentration, kg/m3 GS solid circulation flux, kg/m2s
IV system bed inventory, kg Q loop seal aeration, m3/h
QH gas flow cross loop seal, m3/h QV gas flow cross standpipe, m3/h
q gas tracer(CO2) flow rate,m3/h Ug superficial gas velocity m/s
Uriser riser fluidizing velocity, m/s USl gas –solid slip velocity m/s
US actual particle velocity m/s Ut actual solid velocity m/s
ρs particle density kg/m3 ε voidage
P0~P19 Number of pressure taps △Pcyc pressure drop of cyclone,
P13-P14, Pa
△Plsl pressure drop of loop seal, △Pr pressure drop of riser,P0-P13,
P17-P19 Pa Pa
△Psp pressure drop of standpipe, △Psp/L pressure drop gradient,
P17-P14,Pa (P16-P15)/0.1, Pa /m
REFERENCES
1. Basu P; Cheng L. An analysis of loop seal operations in a circulating fluidized

bed. Chemical Engineering Research and Design,2000,78(7) :991-998
2. Monazam E R; Shadle L J ,et al. Impact of the circulating fluidized bed riser on
the performance of a loopseal non-mechanical valve. Industrial & Engineering
Chemistry Research,2007,46(6):1843-1850
3. Wang Qing,Sun Jian. A overall fluid flow process dynamic model of circulating
loop for CFB boiler. Proceedings of the CSEE,1999,19(12):31-35
4. Hu Nan,Wang Wei,et al. Study on gas-solid s flow properties in the 38 m/54 m
riser of circulating fluidized bed. Proceedings of the CSEE,2009,29(26):7-12
5. Lim K S, Zhu Jinxu, et al. Hydrodynamics of gas-solid fluidization. International
Journal Multiphase Flow, 1995,21(1):141-193
6. Kim, S. W; Kim, S. D. Effects of particle properties on solids recycle in loop-seal
of a circulating fluidized bed, Powder Technology, 2002,124(1) :76-84.
7. Yao, X; Yang, Set al; Experiment study of solids circulating rate's effect on the
pressure loop in circulating fluidized bed. Proceeding of CSEE. 2010, 30(20), 1-6
8. Yerushalmi J, Cankurt N T．Further studies of the regimes of fluidization.
Powder Technology,1979, 24(2): 187-205
9. Ergun S. Fluid flow through packed columns. Chemical Engineering
Progress,1952, 48 (2): 89-94.
10. Yang, S; Yang, H. R et al. Impact of operating conditions on the performance of
the external loop in a CFB reactor. Chemical Engineering and Processing: Process
Intensification. 2009, 48(4), 921-926.
8
COAL IGNITION TEMPERATURE IN AN OXYGEN-ENRICHED
CFB BOILER
Junnan Chao, Hairui Yang, Junfu Lv, Hai Zhang, Qing Liu, Yuxin Wu
Key Laboratory for Thermal Science and Power Engineering of Ministry of Education
Department of Thermal Engineering, Tsinghua University, Beijing, 100084, China
ABSTRACT
The oxygen-enriched Circulating fluidized bed (CFB) combustion technology is a

new method to reduce CO2 emissions. The coal ignition temperature, TiF, in an
oxygen-enriched CFB boiler is an important parameter for designing the startup
burner and for choosing the operating strategy during the startup process. The
combustion of five types of coal under four different atmospheres (air, O2 27 %, O2
40%, O2 53%, CO2 as balance gas) was measured in a laboratory scale fluidized bed
(FB) with an under-bed preheat system. Using thermocouples and a Gas Analyzer,
the changes in bed temperature and the concentration of the different components,
such as O2, CO2 and CO, in flue gas were directly measured to determine TiF. It was
found that TiF decreased with increasing O2 concentration. The differences between
the ignition temperatures determined in air and with 27 % O2 were not significant. At
lower bed temperatures, for two coal types with higher volatiles, a two stage-ignition
for volatiles and char was observed under a high O2 concentration. The time delay
between the two stages decreased and finally merged into one with increasing bed
temperature. Similar results were obtained in air. The coal with the higher volatile
content had a lower ignition temperature in an oxygen-enriched CFB. Comparison of
the ignition temperatures obtained by different methods and the feed temperatures in
industrial CFB boilers showd that the measured result in a fluidized bed can be used
as a reference for oxygen-enriched CFB boilers.
INTRODUCTION
As one of the “green house” gases, CO2 was considered as the one of the main reasons
for causing climate changes. Oxygen-enriched combustion in a PC boiler is considered
one potential technology to reduce CO2 emissions. Many researchers have focused on
this area. By recycling the flue gas, the CO2 concentration in the exhaust gas can reach
more than 90%, which is convenient for the application of Carbon Capture and Storage
(CCS) technology.
An oxygen-enriched CFB is superior to a traditional CFB, Yuru Mao et al (1), and is

being studied as a new technology to reduce CO2 emissions by more and more
researchers. Recycling of the flue gas increases the contact of the SO2 and
desulphurization sorbent, which decreases the conversion rate of the
SO2 ,Zhongyang Luo et al,(2).The emissions of NOX is much lower because of the
‘time gap’ in the formation of nitrogen species and the lack of thermal NOx,Omasz
Czakiert et al,(3). However, there are still many promblems to be solved for
oxygen-enriched CFB, such as the coal ignition temperature and coal combustion
characteristics in the CFB boiler. The Coal ignition temperature in CFB boilers, Ti,
defined as the lowest bed temperature required for stable coal combustion, is an
important parameter for burner design and automatic control during the startup
process. When the coal is fed into a furnace at a temperature lower than Ti, the coal
will not burn and the furnace temperature will decrease even more. Once the fuel
concentration and temperature in the furnace reach critical conditions, the mixture
will flash and the furnace temperature will suddenly increase, which leads to
overheating. Feeding the coal in the furnace at temperatures higher than Ti is safer
but consumes time and oil. The coal ignition temperature is influenced by the type of
the reactor, the way of heating and particle size in the conventional CFB boiler, Hairui
YANG et al,(4).The ignition characteristics of the coal can be described by an ignition
index, which is defined as:
ΔT
Fi =
(t1 + t2 )
where ΔT is the difference between the initial furnace temperature and the
maximum temperature, t1 is the time to reach the lowest temperature, and t2 is the
time to reach the maximum temperature, Hairui YANG et al,(4).
In this work, ignition temperatures of five different types of coal under four different
atmospheres (air, O2 27 %, O2 40%, O2 53%, CO2 as balance gas) were measured in
a laboratory scale bubbling fluidized bed (FB) with an under-bed preheat system. By
using thermocouples and a Gas Analyzer, bed temperature, O2 concentration and Fi
were obtained to determine the factors influencing the coal ignition temperature and
the combustion characteristics.
EXPERIMENTAL SETUP
The ignition temperature was measured in a laboratory-scale fluidized bed reactor

with an inner diameter of 65 mm, which was heated with an under-bed preheat
system. The sketch of the experimental setup is shown in Figure 1.
Quartz sand was used as bed material. The size of the bed particles was in the range
of 0.275mm-0.3mm.The height of the bed was 40mm. CO2 and O2 were mainly used
as the component gases in this experiment to obtain three kinds of inlet gases with
different concentration of O2. The component gases were supplied by gas cylinders.
The simulated gas flowed through the pre-heater directly into the FB. The superficial
gas velocity in the combustion chamber was about three times Umf. Since the
operating conditions greatly influence the coal ignition characteristics, standard
operating conditions as a baseline were specified in Table 1.
Fig.1. Schematic drawing of the experimental setup
Table 1 The standard conditions of coal particle ignition tests

Bed
Fluidized Coal particles Bed Bed
U/ Umf. material
gas (g) material height(mm)
size(µm)
O2/ CO2 3 2.0 Quartz sand 40 275-300
Table 2 Proximate analyses of different coals

proximate analyses [wt%] LHV,ar
No. Coal Type
Mt Vad Fc ad Aad (MJ/kg)
1 Long Yan 4.72 4.30 58.02 32.96 19.07
2 Lu An 2.12 10.31 61.03 26.54 25.05
3 Fu Gu 3.96 30.19 44.31 21.53 22.58
4 Yan Zhou 0.00 35.51 55.67 8.82 21.38
5 Xiao Long Tan 9.88 49.07 36.10 4.95 12.43
Table 3 Ultimate analyses of different coals

No. Coal Type Cad Had Oad Nad Sad
1 Long Yan 52.30 1.04 0.83 0.71 1.12
2 Lu An 62.13 2.67 7.33 1.18 0.15
3 Fu Gu 56.58 3.61 14.28 1.12 0.42
4 Yan Zhou 55.38 2.04 6.42 1.12 0.50
5 Xiao Long Tan 36.72 1.87 12.59 1.01 1.66
Five different types of coal were used as fuel. Tables 2 and 3 list the proximate and
ultimate analyses of each fuel. The size of the coal sample was in the size rang of
1-2mm and the mass in each batch experiment was about 2g. The temperature of
the dense bed was measured by thermocouples during the experiment. A Gas
Analyzer was used to measure the changing of concentration of different
components.
Procedure
1. After the furnace was electrically heated to the selected furnace temperature, Tb,
the coal particles were injected into the furnace.
2. The furnace temperature was then recorded by the data acquisition system.
Ignition of the coal particles was evaluated by observing the flame and sparks
through a mirror. If the coal particles ignited, the furnace temperature was reduced to
a lower temperature Ti+1 and steps 1 and 2 were repeated until the coal particles did
not ignite.
3. If the coal particles did not ignite, TiF, was assumed to be half way between Ti and
Ti-1 and the process was repeated. The process was terminated when |Ti - Ti-1
|<5℃.Then Ti was considered as the ignition temperature.
Influence of furnace temperature on TiF
Figure 2 shows the bed temperature history curves of coal type 2 with different initial
bed temperatures at an oxygen concentration of 52.7 %(CO2 balance).
140 1.0
52.7%
120 O2 52.7%
40.7%
CO2 balance 0.8
100 o
27.8%
1: 585 C air
80 o
2: 583 C
FI, C/s
ΔΤ, C
0.6
o
o
60 3: 570 C
o
o
4: 561 C
40 o 0.4
5: 553 C
20 o
6: 509 C
0 0.2
-20
1 10 100 1000 400 450 500 550 600 650
o
t, s T, C
Fig.2. Bed temperature difference vs. time
Fig.3. Fi of coal 2 vs. temperature
(coal 2, O2 52%, CO2 balance)
Obviously, the combustion characteristics of the same coal type were different even if
the initial bed temperature, Tb, changes within a narrow range. The ignition index
increased with increasing Tb, as shown in Figure 3, which was the same as the result
obtained with air [Yang 2005]. This means the coal particle is easy to ignite at higher
Tb. The initial bed temperature directly influences the heating rate of the particles, the
volatile release rate, and the combustion kinetics. There is a point of the index when
Tb reaches ignition temperature, which means when Tb is over the ignition
temperature the reaction goes faster than it does below this temperature. Results
obtained from different coal types had the same tendency.
Influence of volatile content on TiF

Figures 4 and 5 show a comparison of the temperature history curves of char and
coal at 785℃, O2 20.9%, CO2 balance condition with coal types 1 and 5. For these
conditions coal types 1 and 2 with low volatile contents had a higher ignition index
than their char with the same mass. However, for the same conditions, for coal types
3, 4 and 5 with high volatile contents, the results were opposite. For a high furnace
temperature, a small volatile content in the coal would encourage the ignition, yet
large content would inhibit the ignition.
100 100
o
o
Tb=784 C 1: char
80 80
1: char Tb=785 C O2 20.9% 2: coal
2: coal O2 20.9% CO2 balance
60
60 CO2 balance 1
40
40
ΔΤ, C
ΔΤ, C
o
2 2
20
20
1
0
0
-20
-20
1 10 100 1000 1 10 100 1000
t, s t, s
Fig.4. Bed temperature difference vs. time Fig.5. Bed temperature difference vs. time
(coal 1,785℃, O220.9% , CO2 balance,2.0g) (coal 5,785℃, O220.9% , CO2 balance,2.0g)
Volatiles release from the coal particles immediately after the coals were injected into
the furnace, which increases the porosity at the surface and inside the coal particles.
Increased porosity of the particle enhances oxygen diffusion and increases the
reactivity of char. Therefore, for coals with a high volatile content, TiF is lower.
However, at a higher Tb, rapid volatile releases and combustion results in increasing
local temperature, this causes the local reactant gases to increase in volume
increasing too, which decreases the oxygen concentration. For coal with a high
volatile content, the positive influence caused by increasing contact area is
restrained by the negative influence caused by the volatiles, so, at higher furnace
temperatures, the influence of volatile content is not as significant as at a lower Tb,
and even can have the opposite effect.
Influence of oxygen concentration on TiF
The tests results show that the ignition index increases with increasing oxygen
concentration for all types of coal, as shown in Figure 2. With a high initial
temperature, this tendency is more obvious. The combustion rate of the coal particles
in a fluidized bed boiler is usually controlled by the chemical kinetics and the species
diffusion. However, it is controlled most by chemical kinetics when the furnace
temperature is low (under 500℃).
When the oxygen concentration of the fluidizing media was 27%, the ignition curves
were similar with the results obtained in air, which implies that the increase of the
oxygen concentration from 20.9% to 27% did not improve the ignition process.
Because of the replacement of N2 with CO2, the combustion reaction process was
inhibited by the high concentration of CO2.
Two stage-ignition
Fig.6.Two stage ignition vs. time, coal 4 Fig.7.Two stage ignition vs. time, coal 4
(O2=27.8%) (O2=40%)
Two stage-ignition was observed in the tests with some high volatile coal types with a
certain range of initial bed temperatures and oxygen concentrations, as shown in
Figures 6 and 7. The volatiles released and were ignited after the coal particles were
injected into the furnace, and then the char began to burn. This “two stage-ignition”
became more conspicuous with increasing oxygen concentration, and the two stages
would move closer when furnace temperature was increased. The two stages would
merge when the initial bed temperature was high enough, because of the high
chemical kinetics of char.
However, two stage-ignition was not found in the tests with coal 5 which had the
highest volatile content. It was observed that the combustible content in the volatiles
of coal 5 was much lower than that of coals 3 and 4 by using a mass spectrograph.
This means the reactivity of the volatiles of coal 5 is not high enough to reach the first
stage.Therefore,the ignition process is influenced not only by the volatile content, but
also the combustible content in the volatiles.
Comparison
Figure 8 shows a comparison of the ignition temperatures obtained in

laboratory-scale FB in air condition and oxygen-enriched condition, and the actual
feed temperatures in CFB boilers of China. The actual feed temperatures in CFB
boilers for bituminous coal and brown coal are similar with the ignition temperatures
obtained in the laboratory-scale FB in air. However, for coal types with low volatile
content and high ash content, such as anthracite, the feed temperatures are much
higher than the ignition temperatures because the operators normally choose relative
high feed temperatures for safe operation. The oxygen enriched technology is
capable of decreasing the coal ignition temperature in compared with air, so it can
save more oil during the ignition stage.
CFB plants in
750
China
52% O2+CO2
40% O2+CO2
27% O2 +CO2
Ti，oC
600 Air
450
0 15 30 45 60
Vdaf,%
Fig.8.Comparison of ignition temperature and actual feed temperatures in CFB.
CONCLUSION
The ignition temperatures and combustion characteristics of five different types of

coal were determined in a laboratory-scale FB with a preheat system. Similar with
the results obtained in air, coals with high volatiles had lower ignition temperatures in
an oxygen-enriched CFB. TiF decreased with increasing O2 concentration. The
difference between the ignition temperatures determined in air and 27% O2 were not
significant. Two-stage ignition appeared in the ignition process of some high volatile
content coals in a range of oxygen concentrations and initial temperatures. This was
also influenced by the combustible content in the volatiles.
ACKNOWLEDGMENT
Financial support of this work by High Technology R&D (863) (2009AA05Z302,

2007AA05Z303) are grateful acknowledged.
NOTATION
U— fluidizing air velocity, m/s Umf—minimum fluidizing air velocity, m/s

Tb—bed temperature, ℃ TiF—coal ignition temperature in FB, ℃
Vdaf—volatile content as base of dry free
of ash,%
REFERENCES
1. Yuru Mao, Mengxiang Fang, Zhongyang Luo, et al. Experimental research on

Coal/ char combustion in O2/ CO2 mixed atmosphere. Proceedings of International
Conference on Energy and the Environment ,China , (2003).
2. Luo Zhong yang , Mao Yuru, WU Xue cheng et al ,Test study on and analysis of
burning behavior for coal under atmosphere of O2/ CO2.,Thermal power generation,
33 ,(2004)
3. T Czakiert,Z.Bis,W Muskala,et al.Fluidized bed combustion in oxygen-enriched
conditions,.The 19th inter-national Conference on Fluidized Bed Combustion.(2006.)
4. Hairui Yang,Lei Xue,Yuanxiong Guo et al,The ignition characteristic in CFB boiler,
Journal of Combustion Science and Technology,11,(2005)
5. C.S. Zhao, L.B. Duan, X.P. Chen, C. Liang, Latest Evolution of Oxy-fuel
Combustion Technology in Circulation Fluidized Bed, 20th International Conference
on Fluidized Bed Combustion,(2009)
EFFECT OF TEMPERATURE FIELD ON COAL
DEVOLATILIZATION IN A MILLISECOND DOWNER REACTOR
Binhang Yan, Li Zhang, Yong Jin, Yi Cheng *

Department of Chemical Engineering, Beijing Key Laboratory of Green Chemical
Reaction Engineering and Technology, Tsinghua University
Beijing 100084, P.R. China
PH: +86-10-62794468; FAX: +86-10-62772051; e-mail: yicheng@tsinghua.edu.cn
ABSTRACT
A comprehensive CFD-DPM model was established to describe coal pyrolysis in

millisecond downer reactors under high temperatures. The model predictions
revealed the fact that the reactor performance is dominated by the design of the
temperature field to guarantee fast, sufficient heating of coal particles in milliseconds.
INTRODUCTION
Coal pyrolysis to acetylene in thermal plasma provides a direct route to make

chemicals from coal resources (1-3). Since the coal pyrolysis process is
accommodated in a multiphase downer reactor operated under extreme conditions
(e.g., an ultra-high temperature greater than 3000 K), multiple physical and chemical
processes are completed in milliseconds of contact time, where the rapid heating and
release of volatile matter in coal particles play the dominant role in the overall reactor
performance. It has been acknowledged that thermal energy is the driving force for
coal devolatilization. Therefore, the reactor design is actually directed to the
appropriate design of the temperature field inside the reactor to guarantee sufficiently,
fast heating of coal particles in milliseconds.
A comprehensive computational fluid dynamics model with a discrete phase model

(CFD-DPM) was developed to understand the complex gas-particle reaction
behavior in the coal pyrolysis millisecond process. The model incorporated
particle-scale physics such as heat conduction inside solid materials, diffusion of
released volatile gases (4), coal devolatilization, and the tar cracking reaction (5-6).
The chemical percolation devolatilization (CPD) model (7-9) was applied to describe
the devolatilization behavior of rapidly heated coal based on the physical and
chemical transformations of the coal structure. The predictions by the CFD-DPM
method were validated by comparing the predicted volume fractions of the main
species and light gas yields with the experimental data under a set of typical
operating conditions from the 5-MW coal pyrolysis plasma reactor (10). The results
showed that the heating histories and the devolatilization of particles with the same
diameter were mainly determined by the surrounding temperature field. That is to say,
different heating histories experienced by the particle led to different heating rates as
well as the heating time of the particles, and different yields of light gases.
For further illustration of the effect of the temperature field on the heating histories of
particles and coal devolatilization, different reactor designs were modeled using
CFD-DPM. The same energy input to the downer reactor was assumed by fixing the
pre-defined enthalpy streams of gases, the heat input through the reactor wall, and
the coal feeding conditions. The results showed that coal particles exhibited different
devolatilization performance when experiencing different temperature histories.
Accordingly, reactor optimization can be determined with the guidance of the above
simulation.
MODEL DESCRIPTION
The comprehensive CFD-DPM model includes the k-ε turbulence model for gaseous
turbulent flow with heat and mass transfer, the mixture fraction approach with the
probability density function (PDF) method of modeling the interaction of turbulence
and chemistry, the chemical equilibrium model for high temperature gas-phase
chemical reactions, the discrete phase model (DPM) for momentum, heat and mass
transfer between gas and particles and sub-models for the devolatilization of coal
particles.
Figure 1 Heat, mass and momentum transfer Figure 2 Schematic of a coal particle with
between the discrete and continuous phases heating gas
The numerical simulations of gas-particle flows follow the Eulerian-Lagrangian

approach, as shown in Figure 1. The fluid phase is treated as a continuum by solving
the Navier-Stokes equations, while the particle is considered as the dispersed phase,
solved by tracking a large number of particles through the calculated flow field. As
the trajectory of each particle is computed, the momentum, mass and energy
exchange between the particles and the continuous phase is added to the source
term of the discretization equations for the gas continuum (see Chen and Cheng
(11)).
In addition, the heat transfer model inside a particle (as shown in Figure 2) is
established based on the conduction equation with consideration of the heat of
pyrolysis and the heat conduction in solid materials:
( ρcp )eff ∂T∂(tr , t ) = r12 ∂∂r ⎛⎜ λeff r 2 ∂T∂(rr , t ) ⎞⎟ − Δr H ⋅ γ vol (r , t ) (1)

⎝ ⎠
where
( ρ c p ) = ερvol c p,vol + (1 − ε ) ρ pc p,p
eff
(2)
λeff = ελvol + (1 − ε ) λp (3)
In these equations, T(r,t) represents the local temperature at any radial position r and
time t, ε is the porosity of particle; ρp and ρvol are the densities of the solid material
and the volatile phases, respectively; cp,p and cp,vol are the specific heat capacities of
the solid material and volatile phases, respectively; λeff is the effective local thermal
conductivity; λp and λvol represent the thermal conductivities of the solid material and
volatile phases, respectively; ΔrH is the heat of pyrolysis; and γvol(r,t) denotes the rate
of devolatilization (kg/m3·s).The boundary conditions of Eq. (1) are given as:
⎧ ∂T ⎛ δ ⎞
2
⎪ 4π R λeff
⎪
2
∂r ⎝ 2 ⎠
(
= 4π ⎜ R + m ⎟ h (Tg − Tw )θ + σε p (4π R 2 ) Tg4 − Tw4 )
r =R
⎨ (4)
⎪ ∂T =0
⎪ ∂r
⎩ r =0
where R is the radius of the coal particle, Tw is the temperature at the surface of the
coal particle, Tg is the local temperature of the continuous phase, σ is the
Stefan-Boltzmann constant, εp is the black-body radiation coefficient for the
pulverized coal, δm is the thickness of the gas film around the coal particle (estimated
to be 2R at a relative small Reynolds number in this study), h is the gas-particle heat
transfer coefficient, and θ is a factor related to the effect of volatiles’ release on heat
conduction. The gas-particle heat transfer coefficient was calculated from the Nusselt
number, Nu = hδm/λm, where λm is the thermal conductivity of the gas film. The factor
θ reported by Spalding (12) was adopted in this study,
B cp,g ⎛ dmvol ⎞
θ= , B = (5)
eB − 1 2π dp λm ⎜⎝ dt ⎟⎠
where cp,g represents the gas specific heat capacity, dp is the particle diameter, and
dmvol/dt denotes the formation rate of volatiles from coal (kg/s).
The CPD model was employed to describe the devolatilization of coal particles,
where the fractional change in the coal mass as a function of time was divided into
light gases, tar precursor fragments and char. The tar cracked through the following
assumed paths:
light gases ←⎯⎯ k1
Tar ⎯⎯→
k2
soot (6)
The mechanism utilizes the Arrhenius equation which is defined as:
ki = Ai exp ( −Ei / RT ) i = 1,2 (7)
The values of the kinetic parameters were obtained from the work of Ma (5) and
Brown (6).
The solution of the complex model described above was implemented using the
commercial software FLUENT with self-developed user-defined functions (UDFs).
Model validation
Figure 3 shows a schematic drawing of the 5-MW plasma downer reactor for coal
pyrolysis, which was composed of the V-shaped plasma torch, the mixing zone, the
reaction zone and the quench and separator.
Yield of product (wt %, daf)

80 80
Prediction
Volume fraction (%)
60 Experiment 60
40 40
20 20
0 0
C 2H 2 CO CH 4 H 2 gases
ht
Lg
i
Figure 3 Schematic drawing of the Figure 4 Comparison of predictions with the

5-MW plasma downer reactor experimental data of the 5-MW reactor
The predicted volume fractions of the main species and the yield of light gases using
this practical geometry are plotted in Figure 4, together with typical experimental data.
The predictions and the actual performance of the 5-MW pilot reactor are based on
typical operating conditions (10). It can be seen from Figure 4 that the model
predictions agreed well with the experimental data. Therefore, the comprehensive
CFD-DPM model is qualified for describing the complex devolatilization process in
the reactor under the extreme environmental conditions such as ultrahigh
temperatures and the milliseconds reaction time. Meanwhile, the simulations can
help to optimize the operating conditions and improve reactor performance.
Reaction process of coal particles
Figure 5 shows the variations of the particle temperature and yields of light gases
with particle residence time in the 5-MW downer reactor, together with the
temperature of the heating gas around the particle trajectories. The unique structure
of V-shaped torch causes the uniform temperature distribution and the corresponding
uniform velocity field in the reactor. Therefore, Coal particles with a diameter of 50
μm injected from different positions experience different heating histories, which
result in different devolatilization performances. It can be shown that the effect of the
surrounding temperature field on the particle heating history and devolatiliation
performance is significant.
Average temperature (K)

Yield of product (wt%, daf)

40 40 40
2000 2000 2000
30 30 30
1500 1500 1500
20 20 20
1000 Heating gas 1000 Heating gas 1000 Heating gas
Particle 10 Particle 10 Particle 10
500 500 Light gases 500
Light gases Light gases
0 0 0
0 1 2 3 4 0 1 2 3 4 0 1 2 3 4
Residence time (ms) Residence time (ms) Residence time (ms)
Figure 5 Reaction process of a single representative particle in the 5-MW downer reactor
Effect of the specified temperature field
For further illustration of the effect of temperature field on the particle heating history
and devolatilization performance, variations of the particle temperature and
devolatilization versus the particle residence time under different specified
temperature fields are plotted in Figure 6. It is assumed that coal particles with a
diameter of 50 μm passed through the preset temperature field and the temperature
of the heating gas was not impacted by the discrete particles.
When the particle residence time is long enough to ensure that the temperature of
the particle is close to that of the heating gas, a higher surrounding temperature
would lead to a faster heating rate, and therefore a better devolatilization
performance. The devolatilization is almost competed once the particle reaches its
peak temperature. After that, thermal energy is no longer the main driving force for
the coal devolatilization process. Therefore, in order to get a better devolatilization
performance and a higher energy utilization efficiency, the thermal energy should be
used for maintaining a high temperature field to make sure the coal particle is heated
to a higher temperature.
When the surrounding temperature field is fixed, the particle heating histories and
yields of light gases are observed to be very sensitive to changes in the heat up time,
as shown in Figure 7. The optimal residence time in the high temperature zone
should be more than 2 ms under this situation. When the heat up time is less than 1
ms, the thermal energy stored in the high temperature heating gas was not used
effectively to achieve satisfactory reactor performance.


2000 40 2000 40 2000 40
30 30 30
1500 1500 1500
20 20 20
1000 Heating gas 1000 Heating gas 1000 Heating gas
500 500 500
Light gases Light gases Light gases
0 0 0
0 2 4 6 8 0 2 4 6 8 0 2 4 6 8
Figure 6 Effect of temperature field on particle heating history and devolatilization

performance


2000 40 2000 40 2000 40
1500 30 1500 30 1500 30
20 20 20
1000 1000 1000
Heating gas Heating gas Heating gas
500 500 500
Light gases Light gases Light gases
0 0 0
0 1 2 3 0 1 2 3 4 0 2 4 6
Figure 7 Effect of heating time on the particle heating history and devolatilization
performance
Effect of reactor design
The reactor design is actually directed to the temperature

Wall-1
design of the temperature field inside the reactor, Wall-2 2600
2400
Wall-3
as shown in Figure 8. Three kinds of energy input 2200
Wall-4 2000
designs are carried out to investigate the Wall-5 1800
1600
influences of reactor design on the particle 1400
Wall-6 1200
heating history and the yield of light gases. The 1000
800
feed conditions to the downer reactors are fixed 600
400
and the same amount of energy is exerted into the
different specified reactor wall, Figure 8 Temperature field of
i) Case I: all the energy is inputted to the different reactors
reactor only through wall-2;
ii) Case II: all the energy is inputted to the reactor through wall-2 and wall-3 evenly;
iii) Case III: all the energy is inputted to the reactor through wall-2, wall-3, wall-4
and wal-5 evenly;
The temperature of wall-1 is fixed at 300K and the ones of other walls are fixed at
1600 K for all cases. The input energy density of each reactor design is: Case I,
1.4e6 W/m2; Case II, 7e5 W/m2; Case III, 3.5e5 W/m2. It is shown in Figure 8 that
different reactor designs cause different temperature fields, which leads to a different
devolatilization performance. Too concentrated an energy input (e.g., Case I) leads
to a shorter heat up time as well as a lower peak temperature of the coal particle. As
a result, a poor devolztilization performance is obtained. The appropriate energy
input density is achieved when both a high temperature field and enough heat up
time occurs, which leads to the higher yield of light gases, as shown in Figure 9.


2500 50 2500 50 2500 50
2000 40 2000 40 2000 40

30 30 30
1500 1500 1500
Heating gas 20 Heating gas 20 Heating gas 20
1000 1000 1000
500 Light gas 500 Light gas 500 Light gas
0 0 0
0 3 6 9 12 0 3 6 9 12 0 3 6 9 12 15
Case I Case II Case III
Figure 9 Effect of reactor design on the particle heating history and devolatilization
performance
The temperature field can be designed by altering the operating conditions. In order
to get a better devolatilization performance, special attention must be paid to the
design of the high-temperature heat source and the gas-particle mixing efficiency to
ensure that the coal particles can be heated up rapidly have sufficient time in the high
temperature zone.
CONCLUSION
A comprehensive CFD-DPM model was established to describe coal devolatilization

in millisecond downer reactors with successful validation using experimental data.
This model was further employed to explore the effect of temperature field on the
particle heating history and devolatilization performance. The results indicate that the
coal particles exhibit different devolatilization performances when experiencing
different designed temperature histories. Faster heat up rates, higher gas
temperatures and longer residence times lead to a better devolatilization
performance. With the guidance of these simulations, the reactor design and
operating conditions can be selected to obtain the best temperature field and
excellent gas-particle mixing efficiency in order to achieve a better reactor
performance.
ACKNOWLEDGEMENT
Financial supports from National 863 Project of China under the grants of no.
2009AA044701, National Natural Science Foundation of China (NSFC) under the
grants of no. 20976091 and no. 20990223, and Xinjiang Tianye Corporation are
acknowledged.
REFERENCES
1. Bond, R. L., Ladner, W. R., Mcconnell, G. I. T., and Galbraith, I. F. (1963). “Production
of Acetylene from Coal, Using a Plasma Jet.” Nature, 200(491), 1313-1314.
2. Nicholso, R., and Littlewo, K. (1972). “Plasma Pyrolysis of Coal.” Nature, 236(5347),
397-400.
3. Fauchais, P., Bourdin, E., Aubreton, J., and Amouroux, J. (1980). “Plasma Chemistry
and Its Applications to The Synthesis of Acetylene from Hydrocarbons and Coal.” Int.
Chem. Eng, 20(2), 289-305.
4. Shuang, Y., Wu, C. N., Yan, B. H., and Cheng, Y. (2010). “Heat Transfer inside
Particles and Devolatilization for Coal Pyrolysis to Acetylene at Ultrahigh
Temperatures.” Energy & Fuels, 24(5), 2991-2998.
5. Ma, J. (1996). “Soot Formation and Soot Secondary Reactions During Coal Pyrolysis.”
PhD thesis, Brigham Young University, Utah, USA.
6. Brown, A. L. (1997). “Modeling Soot in Pulverized Coal Flames.” MSc thesis, Brigham
Young University, Utah, USA.
7. Grant, D. M., Pugmire, R. J., Fletcher, T. H., and Kerstein, A. R. (1989). “Chemical
Model of Coal Devolatilization Using Percolation Lattice Statistics.” Energy & Fuels,
3(2), 175-186.
8. Fletcher, T. H., Kerstein, A. R., Pugmire, R. J., and Grant, D. M. (1990). “Chemical
Percolation Model for Devolatilization. 2. Temperature and Heating Rate Effects on
Product Yields.” Energy & Fuels, 4(1), 54-60.
9. Fletcher, T. H., Kerstein, A. R., Pugmire, R. J., Solum, M. S., and Grant, D. M. (1992).
“Chemical Percolation Model for Devolatilization. 3. Direct Use of C-13 Nmr Data to
Predict Effects of Coal Type.” Energy & Fuels, 6(4), 414-431.
10. Yan, B.H., Wu, C.N., Jin, Y., & Cheng, Y. (2010, May). “CFD simulation of the
reacting flow process of coal pyrolysis to acetylene in hydrogen plasma downer
reactors.” In S.D. Kim, Y. Kang, J.K. Lee, & Seo, Y.C. (Eds.), Fluidization XIII (p.725),
Engineering Conferences International, Gyeong-ju, Korea.
11. Chen, J. Q., and Cheng, Y. (2009). “Process Development and Reactor Analysis of
Coal Pyrolysis to Acetylene in Hydrogen Plasma Reactor.” J. Chem. Eng. JPN, 42,
s103-s110.
12. Spalding, D. B. (1955). “Some Fundamentals of Combustion.” Butterworths Scientific
Publications: London.
NUMERICAL SIMULATIONS OF A CIRCULATING FLUIDIZED
BED WITH A SQUARE CROSS-SECTION
Tingwen Li1,2, Sreekanth Pannala3, Chris Guenther2
1. URS Corporation, Morgantown, WV 26505, U.S.A.
2. National Energy Technology Laboratory, Morgantown, WV 26505, U.S.A.
3. Oak Ridge National Laboratory, Oak Ridge, TN 37831, U.S.A.
ABSTRACT
In this study, both 2D and 3D numerical simulations of a well-documented circulating

fluidized bed with a square cross-section were conducted. With some assumptions, a
series of 2D simulations was first carried out to study the influence of grid resolution,
initial flow field, and boundary condition on the flow hydrodynamics. It was found that
2D simulations under-predicted the solids inventory even with the finest grid
(10-particle-diameter grid size). On the other hand, a 3D simulation with relatively
coarse grid was found in better agreement with the experimental data. Differences
between 2D and 3D simulations were briefly discussed.
INTRODUCTION
Circulating fluidized beds (CFBs) have been widely utilized in a variety of industrial
applications including coal combustion, gasification, fluid catalytic cracking, etc. To
accomplish successful and reliable design and operation of CFBs, numerous
investigations pertaining to different hydrodynamic aspects of CFBs have been
undertaken over the past few decades e.g. (1, 2). Among various research tools,
computational fluid dynamics (CFD) is playing an increasingly important role in
studying the complex flow hydrodynamics in CFBs. Numerical simulation of
gas-solids flow in CFBs, usually with two-fluid model (TFM) based on kinetic theory of
granular flow, requires a very fine mesh (typically 10~100 particle diameters), and
consequently, very small time steps (typically 0.1~1.0 milliseconds). However, due to
the high computational cost of multiphase flow simulations of usually very long CFBs,
such a high resolution simulation is prohibitive.
An appropriate simplification of the computational domain is necessary to achieve a

good balance between speed and accuracy of the CFB simulations. Axi-symmetric
assumption of the flow was employed mainly in the steady flow simulations as this
assumption is likely to result in unphysical accumulation of particles along the axis in
unsteady simulations (1). Alternatively, most unsteady numerical studies were carried
out with a two-dimensional flow assumption in which a cut plane along the axis of a
cylindrical column was simulated. Two-dimensional flow assumption is a rough
assumption of the flow in a cylindrical column as the transient riser flow has significant
angular movements despite its wide applications in the literature and successes in
predicting certain flow hydrodynamics, for example, the core-annular pattern in riser
flows. Undoubtedly, a 2D numerical simulation is not able to accurately account for
the 3D effects resulting from geometry and operation. In addition, comparing ratios of
wall area to column volume, 2D simulations inherently under-estimate the wall effects
that are usually important in lab-scale riser flows. Hence, it is necessary to quantify
the differences between 2D and 3D simulations in order to conduct efficient numerical
1
modeling.
In this study, the gas-solids flow in a well-documented circulating fluidized bed of

square cross-section has been simulated. The influences of initial conditions and grid
resolution on 2D simulations were investigated mainly with respect to solids loading to
seek a way to accelerate numerical modeling. After that, a 3D numerical simulation
was conducted to evaluate the differences between 2D and 3D simulations.
NUMERICAL SIMULATION
Numerical Model
An open source software, Multiphase Flow with Interphase eXchanges (MFIX), was
used to conduct the numerical simulations. In MFIX, a multi-fluid, Eulerian-Eulerian
approach, with each phase treated as an interpenetrating continuum, was employed.
Mass and momentum conservation equations were solved for the gas and solid
(particulate) phases, with appropriate closure relations (3). Constitutive relations
derived based on the granular kinetic theory were used for the solid phase. More
information on MFIX as well as detailed documentation on the hydrodynamic model
equations can be found in (4).
Simulation Setup
A cold-model CFB riser of 146×146 mm square cross-section and total height of 9.14
m was simulated. Sand of mean diameter 213 µm, particle density 2640 kg/m3 and
loosely packed bed void fraction of 0.43 was used as the bed material. In this study, a
superficial gas velocity of 5.5 m/s and a solids circulating flux of 40 kg/m2s were
simulated. Detailed information on the experimental setup and measurements on void
fraction and solids velocity profiles were
provided in the literature (5, 6).
In this study, both 2D and 3D simulations

as schematically shown in Figure 1 were
conducted. The simple geometry of
square riser was discretized by Cartesian
grid with uniform grid size in each
direction. Uniform inflow boundary
conditions were imposed at the bottom
gas distributor and the solids side inlet and
a constant pressure at the outlet was
imposed. A partial slip wall boundary
condition was applied for the solids phase
and a no-slip wall boundary condition was
used for the gas phase.
A series of 2D simulations is first

presented to evaluate the effects of grid
resolution and initial flow condition. This is Figure 1. Schematic plots of 2D and 3D
followed by the 3D simulation and the simulations.
2
differences between 2D and 3D numerical simulations are briefly discussed. Finally,
comparisons between numerical results and experimental data are presented.
Grid Resolution
Different grid resolutions of 15×456, 30×456, 30×912, 60×912, 60×1824 and

60×3648 were tested in the 2D simulations. The finest grid resolution (dy≈dz≈2.5 mm)
corresponds to 12-particle-diameter grid size which is very close to the
10-particle-diameter criterion for grid independence in gas-solids flow simulations (1,
7). The simulation has been typically performed for 100 seconds of real-time for most
grid resolutions reported here. The solids inventory inside the system was monitored
in form of the overall solids holdup to characterize the flow development as shown in
Figure 2. It can be seen from the plot that solids loading decreases with time and
finally reaches a near-stationary value indicating the fully developed state. The grid
resolution affects the history of solids loading inside the riser at the initial stage but
has no significant influence on the solids inventory after reaching the fully developed
state except for the coarsest grid. Compared to an estimation of solids holdup, which
is greater than 0.08, based on the experimental measurements of cross-sectional
void fraction (5), the current 2D simulations substantially under-predict the solids
inventory. It seems that the under-prediction cannot be overcome by decreasing grid
size even to 10-particle-diameter, at least for the current case. Similar finding was
reported by Lu et al. (8) in their 2D simulations of CFB riser with FCC particles
although the grid sizes in their study were greatly larger than 10-particle-diameter.
Consistent to their study, refinement of grid does affect the predicted transient flow
behavior for example the spatial distribution of solids. The transient flow fields
suggest that a finer grid tends to predict higher gradient of concentration and lower
void fraction in the clusters.
Figure 2. Temporal variation of the overall solids holdup predicted by the 2D

simulations with different grid resolutions.
Initial Condition
For the cases shown above, a uniform solids concentration of 0.15 was assumed
throughout the domain as the initial flow condition. It is expected that the initial flow
condition has no influence on the final results when the flow is fully developed.
However, it is still meaningful to evaluate if different initial conditions affect the
duration for the flow to fully develop so that the computation time can be shortened.
For this purpose, two additional cases with initial conditions of a partial filled packed
3
bed with the same loading (solids holdup of 0.15) and a uniform solids concentration
of 0.05 were conducted. Figure 3 presents the temporal variation of the overall solids
holdup for cases with different initial conditions. As expected, the initial condition does
not affect the solid inventory when the flow is fully developed. However, it does affect
the time needed to reach the stationary state. These simulations indicate that it is
helpful to set the solids loading closer to that at the developed state to decrease the
simulation time and accelerate convergence through the initial transients. For real
process simulations, this is possible since the solids inventory can be roughly
estimated based upon the overall pressure drop.
Figure 3. Temporal variation of the overall solids holdup for the cases with different
initial flow conditions (grid resolution: 30×456).
Inflow Condition
The yz plane cutting along the side inlet and outlet was simulated in the 2D
simulations. Constant solids feed rate at the side inlet was set based on the whole
column cross-sectional solids flux reported in experiments. An alternate way was also
evaluated to set the solids inflow rate based on the solids flux at the side inlet along
the intersection of the yz plane. With this method, the solids circulating rate was
higher than that based on the riser cross-section. For example, the resulting
cross-sectional solids flux of 51 kg/m2s was 25% higher than that of 40 kg/m2s
reported experimentally. As shown in Figure 4, the solids holdup at the fully
developed state increases with the solids circulating rate. However, this adjustment of
inflow condition in the 2D simulations cannot overcome the significant
under-prediction of solids loading.
Figure 4. Time variations of the overall solids holdup for cases with different solids
inflow rates based on column solids flux and side inlet flux (grid resolution: 30×456).
4
3D Simulation
A case with grid resolution of 30×30×456 is conducted for which 150 seconds
simulation was completed to address the differences between 2D and 3D simulations.
Temporal variation of the overall solids holdup predicted by both 2D and 3D
simulations with comparable grid sizes is presented in Figure 5. There is a substantial
difference between 2D and 3D simulations with respect to the solids loading.
Differences in 2D and 3D simulations for both cylindrical and rectangular fluidized
beds operated in bubbling, slugging, and turbulent fluidization regimes have been
systematically discussed by Xie et al. (9, 10). Their results demonstrated that a 2D
Cartesian simulation can be used to successfully study a bubbling fluidization regime
close to Umf (minimum fluidization velocity) but needs extra caution for modeling other
fluidization regimes with higher gas velocity. The substantial differences presented
here indicate that 3D simulation should be used for modeling CFBs. Of course, this
inevitably leads to an extremely large number of computational cells for a
grid-independent simulation. Due to the prohibitively expensive computational cost,
not many 3D unsteady simulations of CFB riser flows were reported. To overcome
high computational cost, a coarse grid three-dimensional numerical simulation with
appropriate sub-grid closure models is necessary, which has been addressed by
many researchers, e.g. (8, 11). Nevertheless, 2D simulations might be used as an
effective tool to conduct qualitative study.
Figure 5. Time variations of the overall solids holdup predicted by 2D (30×456) and
3D (30×30×456) simulations.
Due to the computational cost of 3D simulation, no sensitivity study on the grid

resolution and initial conditions was conducted so far. However, in future it might be
helpful to conduct sensitivity studies on grid resolution, wall boundary conditions, and
other physical and operational parameters in 3D unsteady simulations.
Comparison with Experimental Data
Figure 6 presents axial profiles of mean void fraction at different lateral positions
predicted by the current numerical simulations when the flow is fully developed as
well as the experimental data measured by a fiber optic probe (5). General profiles of
low void fraction at the bottom of the riser and gradually increasing towards the top
are predicted by the 3D simulation. However, the trend is not correctly predicted by
the 2D simulation and the void fraction is substantially over-predicted almost
everywhere. The results clearly indicate that 3D effects in a CFB riser are important in
5
the case studied and assuming 2D flow can lead to under-prediction of solids
inventory. Under-prediction of solids inventory with a fixed solids mass flux or
over-prediction of solids flux with a fixed solids inventory has often been reported in
the literature for 2D numerical simulations of CFB riser flows with fine FCC particles
by using traditional inter-phase drag correlations. It is usually attributed to the
unresolved meso-structure or clustering phenomena by insufficient grid resolution.
The current results likely suggest that the three-dimensional effect is another reason
for the discrepancies owing to the inherent differences between 2D and 3D
simulations as stated before.
Figure 6. Axial profiles of mean voidage at different lateral positions.
Lateral profiles of mean void fraction at two heights are shown in Figure 7. Again,
results of the 3D simulation shows better agreement with the experimental data than
the 2D simulation. Offset of the void fraction maxima from the axis of the column is
predicted. The asymmetric lateral distribution of void fraction caused by the side exit
is reasonably captured. By examining the cross-sectional distribution of void fraction
and solids velocity, a core-annulus flow structure is observed for this riser of square
cross-section similar to risers of circular cross-section. Different lateral profiles of the
mean vertical solids velocity at z=5.13 m above the distributor predicted by the
numerical simulations are also compared to the experimental data in Figure 8.
Numerical predictions are consistent with the experimental measurements, with most
particles traveling downwards close to wall and upwards in the central region except
that the rising velocity in the core region is under-predicted. Overall, the 3D numerical
simulation shows reasonably good agreement with the experimental data.
Although the 3D simulation produces much improved results, there are some
discrepancies in void fraction and velocity profiles between simulation and
experiment. For example, good agreement is obtained for the axial voidage profiles
near the wall, but relatively poor agreement is predicted along the central axis. One
possible reason can be the coarse nature of the grid (much larger than the
6
10-particle-diameter thumb-rule for grid independence) and probably a sub-grid
correction for the inter-phase drag is needed to account for clusters. Another possible
reason is the simplification of solids inlet and outlet configurations. For instance, the
effect of solid side inlet cannot be accurately modeled by the simple uniform inflow
condition upon entering the system. Fluctuations in solids concentration and velocity
at the inlet have been predicted by numerical simulations with a short L-valve (12).
While, the simplification of the horizontal duct connecting the riser exit to cyclone into
a simple pressure outlet is not capable of predicting the solids accumulation in the
duct and its influence on the riser flow observed in the experiments. Closer
agreement with the experimental data is expected if more accurate inlet and outlet
conditions are assigned for the simulations.
Figure 7. Lateral profiles of mean voidage at z=7.06, 8.98 m and x=0 cm.
Figure 8. Lateral profiles of mean solids velocity at z=5.13 m.
CONCLUSIONS
In this study, both 2D and 3D numerical simulations of a well-documented circulating

fluidized bed of square cross-section were conducted. Effects of grid resolution and
initial flow condition were studied in 2D simulations. It was found that the time needed
by numerical simulations to reach the stationary state can be reduced by carefully
choosing the initial bed loading. However, it was demonstrated that the 2D
simulations under-predicted the solids inventory even with very high grid resolution
(~10-particle-diameter grid size). A 3D simulation predicted a considerably higher
solids inventory compared to the 2D simulation. Profiles of void fraction and solids
7
velocity predicted by the 3D simulation were in reasonable agreement with the
experimental data. Clearly, three-dimensional simulations are required to accurately
represent a circulating fluidized bed system, at least for the system simulated. With
this in mind, some conclusions obtained through 2D simulations might need further
verification in 3D simulations.
ACKNOWLEDGMENT
This research was sponsored by the Fossil Energy, U.S. Department of Energy. The
work was partly performed at the Oak Ridge National Laboratory, which is managed
by UT-Battelle, LLC under Contract No. DE-AC05-00OR22725. The authors thank
Drs. Sofiane Benyahia, Tom O’Brien, and Madhava Syamlal at National Energy
Technology Laboratory. This research was also supported in part by an appointment
to the National Energy Technology Laboratory Research Participation Program,
sponsored by the U.S. Department of Energy and administrated by the Oak Ridge
Institute for Science and Education.
REFERENCES
1. Guenther, C.; Syamlal, M.; Shadle, L.; Ludlow, C. A numerical investigation of
an industrial scale gas-solids CFB, Proceedings of the 7th International
Conference on Circulating Fluidized Beds, Falls, Ontario, Canada, 2002.
2. De Wilde, J., G.B. Marin, and G.J. Heynderickx. The effects of abrupt T-outlets in
a riser: 3D simulation using the kinetic theory of granular flow. Chemical
Engineering Science 2003, 58: 877-885.
3. Syamlal, M., W. Rogers, and T. J. O'Brien. MFIX documentation: Theory guide.
Morgantown, West Virginia, U.S. Department of Energy (DOE), Morgantown
Energy Technology Center, 1993.
4. Benyahia, S., M. Syamlal, and T.J. O'Brien. Summary of MFIX Equations 2005-4.
2007.
5. Zhou, J., J.R. Grace, S. Qin, C.M.H. Brereton, C.J. Lim, and J. Zhu, Voidage
profiles in a circulating fluidized bed of square cross-section, Chemical
Engineering Science, 1994, 49: 3217-3226.
6. Zhou, J., J. R. Grace, C. J. Lim, and C. M. H. Brereton, Particle velocity profiles in
a circulating fluidized bed riser of square cross-section, Chemical Engineering
Science, 1995, 50: 237-244.
7. Andrews, A. T., P. N. Loezos, and S. Sundaresan. Coarse-grid simulation of
gas-particle flows in vertical risers. Industrial & Engineering Chemistry Research,
2005, 44(16): 6022-6037.
8. Lu, B., W. Wang, and J. Li, Searching for a mesh-independent sub-grid model for
CFD simulation of gas-solid riser flows. Chemical Engineering Science, 2009, 64:
3437-3447.
9. Xie N, Battaglia F, Pannala S. Effects of using two- versus three-dimensional
computational modeling of fluidized beds: Part I, hydrodynamics. Powder
Technology, 2008; 182:1-13.
10. Xie N, Battaglia F, Pannala S. Effects of using two- versus three-dimensional
computational modeling of fluidized beds: Part II, budget analysis. Powder
Technology, 2008; 182:14-24.
11. Igci, Y., A. T. Andrews, S. Sundaresan, S. Pannala, and T. O'Brien, Filtered
tow-fluid models for fluidized gas-particle suspensions. AIChE Journal, 2008, 54:
1431-1448.
12. Li, T., J. Dietiker, and M. Shahnam, Numerical modeling of NETL challenge
problem 3. Poster at CFB10, Oregon, USA, May 1-5, 2011.
8
HIGH-RESOLUTION SIMULATIONS OF GAS-SOLIDS JET
PENETRATION INTO A HIGH DENSITY RISER FLOW
Tingwen Li1,2, Chris Guenther1
1. National Energy Technology Laboratory, Morgantown, WV 26505, U.S.A.
2. URS Corporation, Morgantown, WV 26505, U.S.A.
ABSTRACT
High-resolution simulations of a gas-solids jet in a 0.3 m diameter and 15.9 m tall

circulating fluidized bed (CFB) riser were conducted with the open source
software-MFIX. In the numerical simulations, both gas and solids injected through a
1.6 cm diameter radial-directed tube 4.3 m above the bottom distributor were tracked
as tracers, which enable the analysis of the characteristics of a two-phase jet. Two
jetting gas velocities of 16.6 and 37.2 m/s were studied with the other operating
conditions fixed. Reasonable flow hydrodynamics with respect to overall pressure
drop, voidage, and solids velocity distributions were predicted. Due to the different
dynamic responses of gas and particles to the crossflow, a significant separation of
gas and solids within the jet region was predicted for both cases. In addition, the jet
characteristics based on tracer concentration and tracer mass fraction profiles at
different downstream levels are discussed. Overall, the numerical predictions
compare favorably to the experimental measurements made at NETL.
INTRODUCTION
Gasification is a process converting carbonaceous materials, such as coal, biomass,

and waste to syngas, a mixture of CO and H2 and other gases, which can be used for
the production of liquid fuels and chemicals or for power generation. Recently, gasifier
designs based on circulating fluidized bed-type technology have drawn attention from
both academia and industries (1), as circulating fluidized beds (CFBs) possess a
number of unique features that make them more attractive than other systems in
energy industries.
In gasification processes, the fuel particles with high energy density are usually
injected into the gasifier as gas-solids jets. It is thus of great practical importance to
understand the manner in which fuel particles disperse and mix with the bed material
upon entering the system. Only limited studies on particle-laden jets in fluidized beds
can be found in the open literature. Glicksman et al. (2) studied the mixing
characteristics of horizontally injected particles in a one-quarter scale model of a
pressurized bubbling fluidized bed combustor using a thermal tracer technique.
Shadle et al. (3) studied the jet penetration of a gas-solids jet into a circulating
fluidized bed riser by tracking phosphorescent particles illuminated immediately prior
to injection. Wang et al. (4) reported the dynamic phenomena of horizontal gas and
gas/solid mixture jets in a bubbling fluidized bed with an electrical capacitance volume
tomography (ECVT) technique. Recently, a challenge problem was generated by
NETL in collaboration with PSRI, in which experimental measurements of a
gas-solids jet into a riser flow will be reported for validation of mathematical models
(5). However, the aforementioned knowledge is far from enough to fully understand
the flow behavior of particle-laden jets in a gas-solids flow system.
1
In this study, CFD was employed to study the gas-solids jet penetration into a high
density circulating fluidized bed riser flow (3). A gas-solids jet in a pilot-scale riser was
simulated with the open-source Multiphase Flow with Interphase eXchanges (MFIX)
code at https://mfix.netl.doe.gov. The general hydrodynamics of riser flow predicted
by the numerical simulations were first compared against the available experimental
data. Jet behaviors were studied through the numerical simulations and separation of
jetting gas and particles was observed. Parameters characterizing the solids
penetration were evaluated at different levels above the jet injection and comparison
with the experimental data was reported.
NUMERICAL MODELING
In this study, the MFIX code was used to carry out the numerical simulations. MFIX is
a multi-fluid, Eulerian-Eulerian code, with each phase treated as an interpenetrating
continuum. Mass and momentum conservation equations are solved for the gas and
solid (particulate) phases, with appropriate closure relations (6). The governing
equations for the solid phase are closed by the kinetic granular theory Constitutive
relations derived based on the kinetic theory for the solid phase stress tensor are
used. More information on the code as well as detailed documentation can be found
at the MFIX website.
The pilot-scale cold flow circulating fluidized

system available at NETL with 0.305 m
diameter 15.9 tall is schematically shown in
Figure 1. To simplify the simulation, only the
riser section indicated in Figure 1 was
simulated. The solids enter the riser from a
side port 0.23 m in diameter and 0.27 m
above the gas distributor. Solids exit the
riser through a 0.20 m side port about 1.2 m
below the top of the riser. A gas-solids jet
was introduced through a small tube of 1.59
cm diameter at 4.3 m above the bottom
distributor in the same azmuthal direction as
the bulk solids feed to the riser. Gas and
particles injected through the jet were
treated as species in the gas and solid
phases, respectively. Transport equations
were solved for the mass fraction of each
species. The high density polyethylene
(HDPE) beads with an averaged diameter of
750 microns and a density of 863 kg/m3 used
in the experiments were simulated. The
material properties and operating conditions
based on the experiments conducted at
NETL were used in the simulation, as
summarized in Table 1. Two cases with low Figure 1. Schematic of NETL CFB with
and high jet gas velocities of 16.6 and 37.2 the gas-solids jet injection (Adapted
m/s, respectively, were simulated. from (3))
2
Table 1. Material properties and operating conditions.
High-resolution 3D numerical Property Value
simulations of the riser flow Particle diameter (µm) 750
were performed. A cuboid Solid density (kg/m3) 863
domain was discretized with Interparticle restitution coefficient - 0.8
a uniform grid size of 7.5 mm Particle-wall restitution coefficient 0.7
except at the jet injection Packed bed voidage - 0.346
level where the grid was Angle of internal friction (deg)_ 30
slightly refined. The current Superficial gas velocity (m/s) 7.62
gird is believed to be fine Solids circulation rate (kg/s) 11.34
enough according to Gas viscosity (Pa.s) 1.8E-5
10-particle-diameter criterion Jet inlet diameter (cm) 1.59
for grid independence in
Voidage at jet inlet (-) 0.97
gas-solids simulations (7, 8).
Jet gas velocity (m/s) 16.6, 37.2
To represent the cylindrical
Jet solids velocity (m/s) 6.93, 15.5
geometry of the riser, some
Temperature (K) 298
cells were blocked so that a
stair-step surface was used Pressure at top exit (Pa) 101325
to represent the column Pressure at bottom (Pa) 118000
boundary. A total of 3 million Gas molecular weight (kg/kmol) 28.8
computational cells was used. To better resolve the transient flow behavior of riser
flow and gas-solid jet, a second order Superbee discretization scheme was employed
for all equations (9). The computation was conducted on a high performance
computing (HPC) system with 192 Xeon quad-core CPU running at 2.83 GHz. More
information on the numerical modeling was provided in (10).
The following boundary conditions were applied in the numerical simulations. At the
bottom distributor, a uniform gas inflow was specified, with no particles entering the
domain. While for the side solids inlet and the gas-solids jet inlet, constant inflow
conditions were assumed. At the top abrupt exit, a constant pressure was used and
particles were free to leave the system. At the wall, a no-slip boundary condition was
adopted for both gas and solid phases for simplicity and it is believed to be
appropriate for the stair-step boundary surface used in the current study.
Approximately, a real time simulation of 25 seconds was completed for each case.
Numerical results in the last 5 seconds were recorded at a frequency of 20 Hz for
post-processing with the first 20 seconds simulation excluded to avoid the startup
effect of such a large system. The flow was confirmed to be fully developed after 15
seconds by monitoring the overall pressure drop across the entire riser. The
numerical results were visualized by an open-source, multi-platform data analysis and
visualization application–Paraview.
General hydrodynamics of the riser flow were compared to the experimental

measurements first to validate the numerical models. Figure 2 presents the
comparison between numerical simulation and experimental data on the axial
pressure gradient. The experimental data shown in the figure are average of 12
duplicated runs and the error bar indicated the standard deviation. Reasonable
agreement between simulation and experiment was obtained though the pressure
gradient was slightly over-predicted presumably because of the no-slip wall boundary
condition and possibly due to the compressive nature of the superbee discretization
3
scheme used in the simulations (7). From the axial pressure gradient profile, it can be
observed that the apparent solids holdup first decreases with increasing height at the
lower region (0-5 m) and remains fairly constant in the middle region (5-10 m) and
then, increases with height at the upper region of the riser (10-15 m). This profile is
consistent with the experimental measurements and the effects of solids side inlet
and abrupt exit were reasonably predicted (11). In addition, comparison with the
experimental data on the solid velocity was made and reasonable agreement
between simulation and experiment was obtained (10).
Figure 2. Axial profiles of pressure gradient for the case with low jet velocity (error bar
indicates the standard deviation of 12 experimental data sets of duplicated runs).
In the numerical simulations, gas and particles injected through the jet were tracked
as species in the gas and solid phases, respectively. Transport equations were
solved for the mass fraction of each species. The tracer concentrations, ε g ,tr and
ε p ,tr , thus can be determined through
ε g ,tr = ε g X g ,tr (1)
ε p ,tr = ε p X p ,tr (2)
where ε g and ε p are volume fractions of gas and solid phases, and X g ,tr and
X p ,tr are species mass fraction of tracer gas and particles, respectively.
Distributions of gas and solid tracers were calculated and the behavior of gas-solids
jet was studied by analyzing the transient results. Snapshots of voidage, tracer
concentrations close to the jet injection in the lengthwise cross-section are shown in
Figure 3. Clusters phenomenon, prominent near the wall, can be clearly observed
from the voidage distribution in Figure 3(a). The gas-solids jet penetrates into the riser
flow and bends upward because of the crossflow. It was also found that the jet was
very unstable due to the strong interactions between the jet and the
non-homogeneous riser flow. The clusters in the dense riser flow played the most
important role in the interaction. Occasionally, the large falling clusters close to the
wall dragged the jet downward.
It is seen from the distributions of solid and gas tracer concentration in Figure 3 that
the jetting particles with high momentum travel deeper into the crossflow and
4
separate from the jetting gas flow. This is caused by the different dynamic responses
of gas and particles to the crossflow. The separation of gas and solids from the jet
flow was also observed when the mean tracer concentrations were examined for both
low and high jet velocities. Hence, the penetration depths, which determine the length
of the effective interaction zone of the jet and crossflow, are different for the jetting
gas and particles. The gas-solids separation suggests that both jetting gas and
particles need to be tracked in order to study the gas-solids jet behavior. In some
gasifier processes, the air-coal mixture is expected to undergo combustion reactions
to supplement the heat needed by endothermic gasification reactions and provide
rapid release of volatile matter. Under such circumstances, the separation of coal
particles from the air jet not only limits the desired combustion but also leads to a cool
region of oxygen-rich gas. The cool oxygen-rich gas flow propagates upwards and
might cause un-wanted combustion of the devolitization and gasification product
gases. Hence, the separation of gas and solids should be taken into account in
design and operation when they are injected together into the reactor crossflow (9).
The depth of tracer particles penetrating into the crossflow increases slightly at higher
levels. It is difficult to define the jet boundary due to fast mixing of the jetting gas and
solids with the riser flow. Here, the analyses were focused on the penetration of tracer
particles into the cross-flow. The penetration depth of tracer gas can be studied in a
similar way.
Figure 3. Snapshots of (a) voidage, (b) volume fraction of tracer particles, and (c)
volume fraction of tracer gas in the length-wise cross-section for the case with a jet
velocity of 37.2 m/s.
In the experiments, the solids particles were exposed to UV light before injection into
the riser in form of gas-solids jet (3). The phosphorescent glow from the tracer solids
was then detected by photo sensors at different radial positions along the jet direction
5
within the riser 15 and 30 cm above the injection level. Relative concentration
distribution of the jetting particles could be obtained through voltage signals of the
photo detector probe. Each set of average radial voltage signals was normalized by
dividing by the maximum voltage measured for that radial profile. Normalized
concentration profiles of the phosphorescent particles ranged between 0 and 1 were
then obtained by data fitting. The distance from the jet wall to the maximum peak and
the width of the profile at half of the peak value were reported to characterize the
jet-behavior as schematically shown in Figure 4.
Figure 4. Schematic of experimental measurements on jet characteristics.
It was expected that the voltage signal from the photo sensor is proportional to the
local concentration of the tracer particles. However, the light intensity of the glowing
particles detected by the probe was also affected by the presence of opaque bulk
particles which might block the light from glowing tracer particles. Hence, the
concentration profile measured through this technique was an unknown combination
of the absolute tracer concentration and the relative concentration of tracer in the
solid phase. Without knowing the exact contributions of both concentrations to the
final signal, it is necessary to compare the jet behaviors determined through the
absolute and relative concentration profiles, which is straightforward in the numerical
simulations. For this purpose, profiles of the tracer particles concentration, ε p ,tr , and
the tracer particles mass fraction in the solid phase, X p ,tr , at different downstream
levels are plotted against the radial distance from the wall in Figure 5 for the case with
a jet velocity of 37 m/s. Regardless of the magnitude, similar shape of profiles are
predicted with a single peak corresponding to the jet position. However, it is seen that
the locations of peak are slightly different. From both profiles, the radial location of
peak and half-height width can be determined as summarized in Tables 2 and 3 for
cases with low and high jet velocities. The experimental measurements are listed for
comparison. The radial peak locations based on the absolute tracer concentration
profiles are higher than those based on the relative concentration profiles. While the
half-height widths based on the absolute concentration are lower than those based on
the relative concentration. The difference can be very significant, especially for the
high jet velocity. From a practical point of view, the absolute tracer concentration
should be used as it characterizes the distribution of the jetting particles in the riser.
On the other hand, it is important to make sure the numerical simulations and the
experimental measurements are equivalent in order to interpret experimental finding
and validate numerical models. In Figure 5, obvious differences between these
profiles can be observed near the wall. The high tracer concentration is resulted from
6
the strong solids backmixing and the dense solids flow close to the wall.
(a) 15 cm above injection (b) 30 cm above injection
2.5 2
mass fraction concentration
concentration 0.04 mass fraction
0.04
Concentration (x10 -3)
Concentration (x10 -3)

2
1.5
Mass fraction
Mass fraction
0.03
0.03
1.5
1
0.02 0.02
1
0.5
0.01 0.5 0.01
0 0
0 0.05 0.1 0.15 0.2 0.25 0.3 0 0.05 0.1 0.15 0.2 0.25 0.3
Radial distance (m) Radial distance (m)
Figure 5. Radial profiles of tracer particle mass fraction in the solid phase and tracer
particle concentration at (a)15 and (b) 30 cm above jet inlet for high jet velocity.
Table 2. Jet characteristics at 15 and 30 cm above injection for low jet velocity.
15 cm above injection peak location (cm) half-height width (cm)
Relative concentration 6 5.4
Absolute concentration 6.2 5.2
Experiment (3) 8 13
Relative concentration 6.4 6.7
Experiment (3) 8 15
Table 3. Jet characteristics at 15 and 30 cm above injection for high jet velocity.
Relative concentration 10.8 7
Experiment (3) 13 18
Relative concentration 12.3 9.1
Absolute concentration 15 7.2
Experiment (3) 14 17
Generally, the current numerical predictions compare favorably to the experimental

measurements. However, the half-height width is greatly under-predicted in the
simulations. The main reason might be the unstable gas-solids flow through the feed
nozzle. In the experiments, the solids concentration and gas and solids velocities
subject to strong fluctuations, which tend to increase the lateral fluctuations of jet
movement, leading to a wide concentration profile with low peak value. This was not
considered in the current numerical simulations where a stable jet inflow with constant
velocity and solids concentration was assumed.
CONCLUSIONS
High resolution numerical simulations were conducted to study the gas-solids jet
penetration into a high density riser flow. General flow hydrodynamics of a pilot-scale
riser were predicted and behaviors of a gas-solids jet were studied. The gas-solids jet
7
was found to be very unstable because of the strong interactions between the jet and
the non-homogeneous riser flow. There existed a significant separation of the jetting
gas and solids when they entered the crossflow. Since experimental measurements
of the absolute tracer concentration was difficult to obtain, the jet characteristics
based on the radial profiles of absolute tracer concentration and relative
concentration to the solids phase were compared against the experimental data.
Generally, reasonable agreement between numerical simulations and experimental
measurements on the gas-solid jet characteristics were obtained.
ACKNOWLEDGMENTS
The authors would like to thank Drs. Lawrence Shadle, Christopher Ludlow, and
James Spenik for providing detailed experimental data and useful discussions. This
research was supported in part by an appointment to the National Energy Technology
Laboratory Research Participation Program, sponsored by the U.S. Department of
Energy and administrated by the Oak Ridge Institute for Science and Education.
NOTATION
X g ,tr mass fraction of tracer gas X p ,tr mass fraction of tracer particles
ε g volume fraction of gas ε p volume fraction of particles
ε g ,tr concentration of tracer gas ε p ,tr concentration of tracer particles
REFERENCES
1. Higman, C., and M. van der Burgt. Gasification, Gulf publishing, 2003.
2. Glicksman, L., E. Carr, and P. Noymer. Particle injection and mixing experiments
in a one-quarter scale model bubbling fluidized bed. Powder Technology, 2008,
180(3):284-288.
3. Shadle, L., J.C. Ludlow, J. Spenik, S. Seachman, and C. Guenther, Jet
penetration into a riser operated in dense suspension upflow: Experimental and
model comparisons. Circulating Fluidized Bed IX, Tutech Innovation, Hamburg,
2008.
4. Wang, F., Z. Yu, Q. Marashdeh, and L.S. Fan. Horizontal gas and gas/solid jet
penetration in a gas-solid fluidized bed. Chemical Engineering Science, 2010,
65(11):3394-3408.
5. NETL/PSRI Challenge Problem 3. URL: mfix.netl.doe.gov/challenge/index.php
6. Syamlal, M., W. Rogers, and T.J. O’Brien. MFIX documentation: Theory guide.
U.S. Department of Energy (DOE), 1993.
7. Guenther, C., M. Syamlal, L. Shadle, C. Ludlow. A numerical investigation of an
industrial scale gas-solids CFB, Circulating Fluidized Bed VII, 2002.
8. Andrews, A.T., P. N. Loezos, and S. Sundaresan. Coarse-grid simulation of
gas-particle flows in vertical risers. Industrial & Engineering Chemistry Research,
2005, 44(16):6022-6037.
9. Li, T., M. Syamlal, C. Guenther, A. Gel, and S. Pannala, High resolution
simulations of coal jets in a gasifier, Industrial & Engineering Chemistry Research,
2010, 49(21):10767–10779.
10. Li, T., and C. Guenther, A CFD study of gas-solids jet in a CFB riser flow, AIChE
Journal, 2011, (in review).
11. Mei, J. S., E. R. Monazam, and L. J. Shadle. Flow regime study of a light material
in an industrial scale cold flow circulating fluidized bed. Journal of Energy
Resources Technology-Transactions of the ASME, 2006, 128(2):129-134.
8
CFD MODELING OF FLUIDIZED-BED REACTOR FOR THE
SYNTHESIS OF DIMETHYL ETHER
Ranjeeth Kalluri, Nandita Akunuri, Aqil Jamal, and Raghubir Gupta
RTI International, P.O. Box 12194, Research Triangle Park, NC 27709 -
2194, USA
ABSTRACT
The syngas-to-DME reaction is highly exothermic, and the catalyst temperature

window is very narrow. The fluidized-bed reactor is, therefore, an ideal choice to
carry out these reactions. RTI is developing a circulating fluidized bed design for
DME synthesis. This paper discusses a two-phase CFD model and optimization of
the solids circulation rate.
INTRODUCTION
In recent years, dimethyl ether (DME) has been generating broad interest as a
promising alternative transportation fuel with great potential impact on society. DME
is also a key chemical intermediate in the production of several petrochemicals such
as dimethyl sulfate, synthetic gasoline, polymer-grade ethylene and propylene, and
acetonitrile, a solvent used in the battery industry. Production of DME worldwide has
increased from 30,000 tonnes/yr in 2000 to 545,000 tonnes/yr in 2006, and is
expected to continue to rise over the next decade, due to the planned construction of
multiple DME production facilities, especially in Asia(1). The conventional production
of DME utilizes carbon monoxide (CO) from syngas. The recent recognition of DME
synthesis from carbon dioxide (CO2) as a potential means to mitigate global CO2
emissions has further added to the growing interest in DME research.
Commercially, DME is produced in a two-step process, where syngas is first

converted to methanol, and the methanol produced is dehydrated to DME. This
process mainly involves the following three reactions:
Methanol synthesis reaction: CO  2H2  CH3OH H  98.744kJ / mol (1)

Water gas shift reaction: CO  H2O  CO2  H2 H  21.255kJ / mol (2)
Methanol dehydration reaction: 2CH3OH  CH3OCH3  H2O H  40.9kJ / mol (3)
Reactions (1) and (2) are catalyzed by a methanol synthesis catalyst (Cu/ZnO/Al2O3)
and reaction (3) is catalyzed by an acid catalyst. All the above three reactions are
reversible and exothermic, which results in a narrow catalyst operating temperature
window. Combining the above reactions so that they occur simultaneously allows
inhibiting products from one equilibrium reaction to be consumed in another, creating
a strong driving force for the production of DME(2). The methanol produced in
1
reaction (1) is consumed by reaction (3), and the water (H2O) formed in reaction (3)
is consumed in reaction (2), thereby driving reaction (3), and producing additional
hydrogen (H2) required for the methanol production (reaction (1)). The net reaction
for the direct syngas-to-DME process can be given as:
Overall Reaction: 3CO  3H2  CH3OCH3  CO2 H  256.615kJ / mol (4)
Numerous commercial DME production processes are available from companies

such as Haldor Topsoe, Lurgi, Mitsubishi Gas Chemical, etc. However, most of these
designs are two-step processes that are extensions of existing methanol synthesis
facilities, and are not optimized for the production of DME. Recent developments for
direct syngas-to-DME (single-stage) production include the use of slurry phase
reactors such as that employed by JFE Holdings, Inc., Japan (3). Although the slurry-
phase reactor provides improved conversion efficiency due to efficient removal of the
heat generated by reactions (1) - (3), the product recovery at typical operating
conditions requires cryogenic separation (< 213 K).
An alternative reactor design for direct DME synthesis is a fluidized-bed reactor. Lu

et al. (4) have demonstrated experimentally that the per-pass CO conversion can be
significantly improved using two-phase fluidized-bed reactors compared to slurry
reactors. These authors have also shown the DME selectivity to be notably higher in
fluidized-bed reactors compared to slurry reactors. Fluidized-bed reactors offer
higher gas-solid mass transfer rates, which lead to higher DME yields compared to
slurry reactors. Dynamic mixing of particles in a fluidized-bed also eliminates hot spot
formation. Elimination of hot spots is critical for an extended catalyst life time (5), as
the catalyst rapidly deactivates at higher temperatures (> 570 K). Further, at higher
temperatures the equilibrium does not favor a high DME yield. These catalyst
deactivation and equilibrium restrictions lead to a narrow catalyst operating
temperature window.
Effective temperature control in a

fluidized-bed reactor can be achieved
by circulating boiler feed water
through internal coils within the
reactor. The major challenge for this
internal cooling scheme is the design
of the reactor internals, which provide
maximum heat recovery. To overcome
these limitations, RTI is exploring a
circulating fluidized-bed (CFB) reactor
design with an external solids-cooler.
In this approach, the catalyst is
circulated between the fluidized-bed
reactor and an external solids-cooler,
where the solids act as a heat
transport medium to carry heat out of
the reactor, thereby allowing for
control of the reactor temperature. A
schematic of this process is shown in
Figure 1: Schematic of the CFB design Figure 1. This process ensures high
2
heat transfer rates and applicability of commercial solid cooling systems typically
used in fluid catalytic cracking (FCC) processes.
In this paper, a computational fluid dynamics (CFD) model for simulating the two
phase (gas-solid) fluidized-bed DME synthesis process was developed using Fluent
12.1. The model developed was first validated with the experimental fluidized-bed
results obtained by Lu et al. (4). This validated model was then used to study the
benefits of a CFB reactor with external solids cooling for DME synthesis, and to
optimize the solids circulation rate for maximizing CO conversion and DME yields.
This CFD model can be further used for design and scale-up of the proposed CFB
reactor for DME production.
CFD MODEL
The two different fluidized-bed geometries (described in detail in the next section)
considered in this study were modeled using 2-D axisymmetric models using Ansys
Fluent 12.1. The Eulerian-Eulerian approach has been used to model the fluid-solid
flow dynamics. This model considers both the primary and the secondary (dispersed)
phases to be interpenetrating continua. The equations considered (6) in the model
are summarized below.
The generalized continuity equation can be written as (i= g or s):
  i i 
    i i vi   0 (5)
t
The momentum balance equations for gas and solid phases can be written as (i, k =
g or s):
  i  i vi 
 .( i i vi vi )  i i g   i P  . i   (vk  vi ) (6)
t
The generalized energy conservation equation for the gas and solid phases is:
 ( i  i H i ) (7)
 .( i i ui H i )  (ki Ti )  hki (Tk  Ti )
t
For the solid phase, the random granular motion resulting from particle collision is
described by the following transport equation:
3  (  s s )  (8)
 (  s s vs )   ( Ps I   s ) : vs  .( s )    gs
2  t 
where the first term on the right hand side is the generation of energy by the solid
stress tensor, the second term denotes the diffusion of energy, the third term
represents the collisional dissipation of energy, and the fourth term represents the
energy exchange between the solid and the gas phase.
The generalized conservation equation for the various species in the gas phase is:
3

t
  g  gYg , j      g  g vgYg , j   . g J g , j  R j (9)
The rate expressions and parameters from Lu et al. (7) were used to model the
reactions involved in the DME synthesis process. The activity of the catalyst was
assumed to remain constant, with no deactivation occurring with time. The rate
expressions used for the three individual reactions (1) - (3), are:
k1KCO  pCO pH3/22  pM / ( pH0.52 K P01 

r1  (10)
1  K CO  
pCO  KCO2 pCO2  pH0.52  KW / K H0.52 pW 
  
r2   
k2 KCO2  pCO pW  pCO2 pH 2 / K P03 
  (11)
  
1  KCO pCO  KCO2 pCO2  pH 2  KW / K H0.5 pW 

0.5
2  
k3  pM   pD pW / K P02  
0.5

 
 (12)
r3 
M  p D pW / K P2 
0.5 2
1  K 0 

 

As will be further discussed in the next section, these kinetic rate expressions were
validated against experimental data reported by Lu et al. (4). While the methanol
synthesis catalysts used in both these studies (4 and 7) were similar (Cu-ZnO-Al2O3),
the methanol dehydration catalyst was different, -alumina by Lu et al. (4) and
HZSM-5 by Lu et al. (7). In view of this difference in the methanol dehydration
catalyst used, kinetic constant k3 was varied to enable a better fit of the CFD model
with the experimental results, while all the other rate and equilibrium constants used
in the above rate expressions were left unchanged from those published by Lu et al.
(7). An order-of-magnitude-lower value for the pre-exponential factor for k3,
compared to that reported by Lu et al. (7), yielded a better fit of the CFD data with
the experimental results, and hence it was used for this entire study. For the purpose
of this study, the CO conversion and DME selectivity was defined as:
( NCO )in  ( NCO )out (13)

X CO 
( NCO )in
2 N DME (14)
SDME 
2 N DME  N MeOH
M DME
PDME  (15)
M cat
CFD SIMULATIONS AND RESULTS
Validation of the CFD Model
As described above, the CFD model was first validated with the experimental CO
conversion results obtained by Lu et al. (4). The reactor geometry and operating
conditions used in this published experimental study are summarized in Table 1.
Also shown in the table are the assumed catalyst thermal properties (conductivity
and specific heat), which correspond to the alumina (catalyst support). A particle
4
sphericity of 0.8 was assumed in this
study to account for the particle Table 1: Operating conditions and parameters
surface roughness. The experimental Reactor diameter (m) 0.026
study by Lu et al. was conducted over Reactor length (m) 2.0
a pressure range of 2 MPa to 4 MPa Bed height at min. fluidization (m) 1.0
and a H2/CO ratio of 0.8 to 2.1. A fixed Inlet & wall temperatures (K) 533
gas space velocity of 3000 ml/g cat/h Packed bed voidage 0.428
(STP) was used in all these Catalyst particle diameter (μm) 150
experimental tests. Catalyst sphericity 0.8
Catalyst density (kg/m3) 1983
Transient CFD cases representing Catalyst specific heat (J/kg K) 880
each of these experiments were Catalyst thermal conductivity (W/m.K) 35
simulated. An isothermal wall boundary
condition (533 K) was used in all these 0.6 0.2
CO mole fraction
simulations to simulate the DME mole fraction
experimental conditions. Each of the 0.5
Gas vol. flow rate (m /h)

H mole fraction
Component mole fraction

2
simulations was run for at least three Gas Vol. flow 0.15
0.4
(gas) residence times, so as to obtain
steady state outputs. The output
0.3 0.1
composition and flow rate were
monitored and plotted. Figure 2 shows 0.2
the typical outlet mole fractions and
3
0.05
flow rate variations with flow time as 0.1
predicted by the CFD simulation. The
outlet gas composition and flow rate 0 0
typically approached relatively constant 0 20 40 60 80
values in about one (gas) residence Time (s)
time from startup. Other process Figure 2: Outlet stream composition and flow
variables such as temperature and rate variation with time (P=3 MPa, H2/CO=1.0,
pressure also showed similar T=533 K, and SV=3000 ml/gcat/h)
stabilization patterns. To eliminate the
effect of small fluctuations present in
0.7
these output flow variables, time- CO mole fraction
averaged (10 s) values were used in DME mole fraction
0.6
Component mole fraction
H2 mole fraction
assessing the steady-state
performance of the reactor. 0.5 Solids volume fraction
0.4
Figure 3 shows the axial profiles of
solids volume fraction, and mole 0.3
fractions of CO, H2, and DME for the
0.2
case of inlet H2/CO ratio of 1.0 and 3
MPa reactor pressure. For these 0.1
conditions, the bed expanded to about
1.40 m in height. The solids fraction 0
increased gradually along the length of 0 0.5 1 1.5 2
the reactor, as the gas volume (molar) Reactor height (m)
flow decreased due to the reactions.
The concentrations of CO and H2 Figure 3: Profile plots of component
compositions and solid volume fractions at t=70
decreased, as they were consumed by
s (P=3 MPa, H2/CO=1.0, T=533 K, and
the reactions, and methanol and DME SV=3000 ml/gcat/h)
concentrations increased along the
5
length of the reactor. Similar patterns were seen for the other reactor pressures and
H2/CO ratios studied. The maximum temperature rise in any of these cases was less
than 5 K, due to the isothermal wall boundary conditions and small reactor diameter
used. The mole fraction of water (not shown in the figure) remained low (< 0.01)
throughout the reactor, as the water gas shift reaction consumed most of the water
generated by the methanol synthesis and methanol dehydration reactions.
Figure 4 and Figure 5 show a comparison of CFD and experimental (4) results of CO
conversion as a function of inlet gas composition and pressure, respectively. The CO
conversion values are in good agreement with the experimental results for the entire
range of pressure and H2/CO ratios reported by Lu et al. (4). The figures also show
DME selectivity and productivity for various inlet conditions. For the same gas space
velocity, increase in H2/CO ratio led to higher CO conversion (Figure 4), as the
methanol synthesis reaction has higher (order) dependence on H2 partial pressure
(1.5) than on CO partial pressure (1.0). Also, an increase in pressure led to higher
conversions and DME productivities (Figure 5), due to higher reactant partial
pressures and effective gas residence times in the reactor. The DME selectivity
decreased with increasing conversions, as the increasing DME concentrations
deterred the methanol dehydration (equilibrium) reaction.
100 0.5 100 0.5
80 0.4 80 0.4
P
(%)
P
(%)
DME
DME
60 0.3 60 0.3
DME
DME
(g/g cat/h)
(g/g cat/h)
or S
or S
40 0.2 40 0.2
CO
CO
X (Lu et. al.)

X
X (Lu et. al.)

X
CO
CO
X (CFD) X (CFD)
CO
20 CO 0.1 20 0.1
S (CFD) S (CFD)
DME DME
P (CFD) P (CFD)
DME DME
0 0 0 0
0.5 1 1.5 2 2.5 1 2 3 4 5 6
H2/CO ratio
Pressure (MPa)
Figure 4: Effect of feed composition on Figure 5: Effect of pressure on

simulation and experimental results simulation and experimental results
(P=3 MPa, T=533 K, and SV=3000 (H2/CO=1.0, T=533 K, and SV=3000
ml/gcat/h) ml/gcat/h)
Circulating Fluidized-bed Optimization
Lu et al. (4) demonstrated through experimental results that the optimum reactor
temperature for maximizing CO conversion and DME yield lies in the range of 550 K
to 570 K, for an inlet gas pressure of 3 MPa and H2/CO ratio of 1.0. The kinetics of
methanol synthesis are limiting at lower temperatures, whereas the equilibrium
restricts CO conversion at higher temperature. This leads to a narrow temperature
window for optimal reactor operation and hence makes the ability to attain precise
temperature control in the reactor critical. As described previously, in this study,
benefits of using a CFB reactor with an external solids cooling loop (Figure 1) for
effective temperature control in the DME synthesis process were explored.
6
A series of CFD simulations were conducted using the above validated CFD model
on a modified fluidized-bed geometry to optimize the solids circulation rates for
maximizing CO conversion and DME yield. The circulating fluidized-bed geometry
used for this study had a length of 4.0 m and a diameter of 0.026 m. In these
simulations, feed gas and catalyst particles entered the reactor at 533 K and 3 MPa.
The feed gas flow rate was fixed at 90 SLPM, and the solids/gas ratio entering the
reactor was varied between 10 and 30, by changing the solids mass flow rate
entering the reactor. The reactor wall boundary condition in these simulations was
set to the adiabatic (no heat flux) condition. All the exothermic heat released from the
reactions was carried out of the reactor exclusively by the catalyst particles and
product gases exiting the reactor. The catalyst, thereby, served dual functions –
reaction rate promoter as well as heat transport medium. Further, the hot solids
exiting the reactor were assumed to be separated and cooled to 533 K, before being
recirculated to the reactor.
1 610
Figure 6 shows the effect of inlet
solids/gas mass ratio on CFB reactor
performance. For maximum CO
Outlet Temperature (K)
0.9 X 600
CO conversion, the optimum solids/gas ratio
(%)
S
0.8 DME 590 appears to be around 20. As expected,
DME
Outlet Temp with increase in solids/gas mass ratio, the

0.7 580 outlet temperature decreased significantly,
or S
as the increasing solids flow absorbs more

CO
0.6 570 heat. The optimum solids/gas ratio (=20)

X
for CO conversion also corresponds with

0.5 560
the outlet temperature of 565 K, which is in
0.4 550
the optimum reactor operating
0 5 10 15 20 25 30 35 40 temperature range suggested by Lu et al.
(4). A lower (<20) solid/gas ratio leads to
Solids/gas mass ratio
excess reactor temperature, resulting in
Figure 6: Effect of inlet solids/gas mass ratio equilibrium limitations, whereas a higher
on performance of CFB reactor for DME (>20) solid/gas ratio leads to low reactor
production (Inlet conditions: P=3 MPa, temperatures and kinetic limitations.
T=533 K. and H2/CO=1.0)
CONCLUSIONS
The CFD model developed in this study was successfully validated with experimental
DME synthesis fluidized-bed results from the literature. It was further used to
demonstrate the benefits of using a CFB reactor with external solids-cooler to control
the bed temperature. The model predicted an optimal solids/gas ratio for highest CO
conversion and/or DME yield to be about 20 for the catalyst (kinetics) used in this
study. In this concept, the catalyst particles act as a heat sink to carry heat out of the
reactor, apart from catalyzing the DME synthesis reactions. The kinetic model used
in this analysis was validated using literature data. Further validation of the CFD
model using our own experimental data is under way.
7
NOTATION
g acceleration due to gravity vi mean velocity of the phase (m/s)

(m/s2)
XCO conversion of CO, dimensionless
hsg heat transfer coefficient Greek Letters
(W/m2.K)
 drag coefficient (kg/m3.s)
H enthalpy (J/kg)
Jg,j diffusion flux (kg/m2s)  dense phase voidage,
k rxn rate constant (units vary) dimensionless
K reaction equilibrium constant s energy diffusion coefficient
Mcat mass of catalyst in reactor (g)  density, kg/m3
MDME DME outlet mass flow rate (g/h)  stress tensor (bar)
NCO molar flow rate of CO (mol/s) gs energy exchange between gas
NDME molar flow rate of DME (mol/s) and solid phase
NMeOH molar flow rate of CH3OH(mol/s)  granular temperature
p partial pressure of species „j‟  dissipation of fluctuating energy
P pressure (bar) (W/m3)
PDME productivity of DME (g/g(cat)/h) Subscripts
SDME selectivity of DME in products, i gas or solid phase
dimensionless k interacting phase
T temperature (K) j species „j‟
r reaction rate, mol/gcat/s g gas phase
Rj rate of production of species „j‟ s solid phase
REFERENCES
1. Reuters. (2008). “China domestic production of dimethyl ether is expected to

reach 4.36 million tons in 2008.” [cited 2009 Aug. 26]; Available from:
http://www.reuters.com/article/pressRelease/idUS140041+08-Aug-
2008+BW20080808
2. Wang, Z., Wang, J., Diao, J., and Jin, Y. (2001). "The synergy effect of process
coupling for dimethyl ether." Chem. Eng. Tech., 24, 507-511.
3. Bourg, H. M. (2006). "Future Prospective of DME." 23rd World Gas Conference,
Amsterdam.
4. Lu, W., Teng, L., and Xiao, W. (2004). “Simulation and experiment study of
dimethyl ether synthesis from syngas in a fluidized-bed reactor.” Chem. Eng.
Sci., 59, 5455-5464.
5. Cooper, M., (2010). “Direct synthesis of dimethyl ether from syngas using a novel
fluidizable catalyst.” Internal R & D Report, RTI International, Durham, NC.
6. Ansys Inc. “Ansys Fluent Theory Guide - Ansys Fluent 12.0.”
7. Lu, W.Z., Teng, L.H., and Xiao, W.D. (2003). “Theoretical analysis of fluidized-
bed reactor for dimethyl ether synthesis from syngas.” Intl. J. of Chem. Reactor
Eng., 1, S2.
8
CFD SIMULATION OF CO2 SORPTION IN A CIRCULATING
FLUIDIZED BED USING THE DEACTIVATION KINETIC MODEL
Emadoddin Abbasi and Hamid Arastoopour

Department of Chemical and Biological Engineering, Wanger Institute for Sustainable
Energy Research (WISER), Illinois Institute of Technology, Chicago, IL 60616
ABSTRACT
The Computational Fluid Dynamics (CFD) approach was used to simulate sorption of
CO2 using solid sorbents in the riser section of a circulating fluidized bed. The
simulation results were compared with the experimental data of Korea Institute for
Energy Research (KIER) for continuous CO2 sorption using potassium carbonate in
a circulating fluidized bed system.
INTRODUCTION
Coal-based power plants generate more than 50 percent of the today’s United States
electric power (1). This means coal will continue to play a significant role in electricity
generation for the foreseeable future. Therefore, the global emission of CO2 and its
impact on climate change will continue to increase. Separation and sequestration of
CO2 has been investigated by many researchers during the past decade including
pre-combustion CO2 separation (gasification), oxyfuel combustion, and post-
combustion CO2 separation. Post-combustion CO2 separation, which includes
chemical and physical sorption of CO2 from flue gases, is a challenging process due
to the low pressure and low concentration of CO2 in flue gas which requires high
volumetric flow rates of flue gas to be processed. In addition, these processes
generally use sorbents to capture the CO2 and these sorbents need to be
regenerated and used continuously in the process. The regeneration of sorbents is
an energy demanding process that reduces the overall efficiency of the power plant.
Therefore, developing more efficient and economically feasible processes for CO2
removal has been one of our goals in recent years. Based on National Energy
Technology Laboratory’s 2009 report (1), the goal for energy consumption of novel
sorbents should be one third of energy consumption for today’s commercially
available sorbents, which are basically amine-based liquid sorbents.
Recent studies have shown that alkali-metal-based solids could be a promising
sorbent for efficient and cost-effective CO2 removal from combustion gases (2, 3, 4).
Ryu and coworkers (3) studied sodium- and potassium-based sorbents and
concluded that they possess excellent features like superior attrition resistance, high
CO2 sorption capacity, and high bulk density. Afterward, their group (5,6) at Korea
Institute for Energy Research (KIER) used a potassium-based solid sorbent to
1
perform two sets of experiments in a 2 Nm3/hr and a 100 Nm3/hr facility for CO2
capture from flue gas. They found that using a circulating fluidized bed (CFB)
ensures the continuous CO2 removal process from dilute flue gases at laboratory
and bench scales.
To scale up this CFB process, a state-of-the-art design tool based on CFD simulation
is needed. However, to this point, few detailed simulations of this process have been
conducted (7, 8) that can capture qualitatively the behavior of the system.
In this study, we used experimental data provided by KIER (5) to validate our CFD
simulation for the CO2 capture process in the riser part of a circulating fluidized
bed using a potassium-based solid sorbent.
EXPERIMENT USED FOR SIMULATION

For our simulation we used the experiments of Yi et al. (5), which includes a
circulating fluidized bed consisting of a riser as carbonator and a bubbling fluidized
bed as regenerator. Figure 1 shows the schematic of CO2 sorption using a circulating
fluidized bed system.
CO2 free gas CO2 + H2O Flue gas containing CO2, H2O, and N2
enters the carbonator and reacts with fresh
(regenerated) solid sorbent containing 35%
Carbonator Regenerator
K2CO3 as shown below:
CO2 + H2O + K2CO3 2KHCO3 + Heat
CO2-free gas exits from the top of the riser

while reacted sorbents go back to the
regenerator to react with steam according
to the following reaction:
2KHCO3 CO2 + H2O + K2CO3 – Heat
A very slender 2.5 cm ID and 6 m height
Flue gas Regenerative
Fluidization Gas riser, with an expanded 3.5 cm ID mixing
zone at the first 0.6 m of the bottom of the
Figure 1. Schematic of CO2 riser as the carbonator and a 10 cm ID and
sorption process in a CFB 1.28 m height bubbling bed as the
regenerator reactor, were used. In this
study, our focus has been on the simulation
of the riser and the carbonation process.
The operating condition is atmospheric pressure and 80o C in the riser. The flue gas
inlet velocity was 2 m/s with 12% CO2 (dry basis) and 12.3% H2O composition. The
solid circulating rate was controlled using a solid valve and was set to 21 kg/m2.s as
the baseline operating condition.
The potassium-based Sorb KX35 sorbent has a bulk density of 1100 kg/m3 and
particle density of 2394 kg/m3 with average particle size of 98 µm. The attrition index
(AI) of this sorbent has been reported as 0.1% at 10 std l/min (3).
Differential pressure was measured at four different elevations along the riser. In
addition, CO2 concentration at the riser outlet was monitored continuously.
2
NUMERICAL MODELING
The CFD simulation of this work is based on a two-dimensional Eulerian-Eulerian
approach in combination with the kinetic theory of granular flow (9, 10). To convert
the real geometry to a reduced two-dimensional domain, the solid mass flux was
kept constant as the basis for calculation.
The assumptions of our numerical simulation include the isothermal condition for the
process, and consider the gas phase as an ideal gas and the particles in the solid
phase to be of uniform and constant size and density. Fluent 6.3 code was used to
solve a set of governing equations including:
Mass conservation
∂ •
For gas phase: (ε g ρ g ) + ∇.(ε g ρ g v g ) = m g
∂t
∂ •
For solid phase: (ε s ρ s ) + ∇.(ε s ρ s v s ) = m s
∂t
Momentum conservation
For gas phase:
∂
(ε g ρ g v g ) + ∇.(ε g ρ g v g v g ) = −ε g ∇P + ∇.τ g + ε g ρ g g − β gs (v g − v s )
∂t
For solid phase:
∂
(ε s ρ s v s ) + ∇.(ε s ρ s v s v s ) = −ε s ∇P + ∇.τ s + ε s ρ s g + β gs (v g − v s )
∂t
Species conservation
∂
For gas phase: (ε g ρ g y i ) + ∇.(ε g ρ g v g y i ) = R j i=1, 2, 3
∂t
∂
For solid phase: (ε s ρ s y i ) + ∇.(ε s ρ s v s y i ) = R j i=1, 2, 3
∂t
And conservation of solid phase fluctuating energy:
3 ∂
[ (ε s ρ sθ ) + ∇.(ε s ρ sθ )v s ] = ( −∇p s I + τ s ) : ∇v s + ∇.(κ s ∇θ ) − γ s
2 ∂t
Where κ s and γ s are conductivity of fluctuating energy and collisional dissipation of
solid fluctuating energy, respectively.
For the gas-solid inter-phase exchange coefficient β gs there are different correlations
available in the literature. Garg et al. (7) showed that using an EMMS-based model
as proposed by Li et al. (11) gives better results compared to the drag model
proposed by Gidaspow (12). Nikolopoulos et al. (13) showed that the EMMS model
increased the accuracy of the simulation at the lower part of the riser, resulted in
better prediction for solid concentration and pressure distribution, and was able to
account for heterogeneous solid structures and cluster formation in the riser.
3
The EMMS-based drag model has been used in this study as follows:
3 (1 − ε g )ε g
ρ g u g − u s C D 0 ω (ε g ) ε g > 0.74
4 dp
(1 − ε g ) 2 µ g (1 − ε g ) ρ g u g − u s
β sg = 150 2
+ 1.75 ε g ≤ 0.74
εgdp dp
Where , ω (ε g ) is called the heterogeneity factor and is defined as
0.0214
− 0.5760 + 0.74 < ε g ≤ 0.82
4(ε g − 0.7463) 2 + 0.0044
ω (ε g ) = 0.0038
− 0.0101 + 0.82 < ε g ≤ 0.97
4(ε g − 0.7789) 2 + 0.0040
− 31.8295 + 32.8295ε g ε g > 0.97

And
24 0.687
CD0 = (1 + 0.15 Re p ) for Rep<1000
Re p
C D 0 = 0.44 for Rep>1000
In addition, k − ε turbulent model has been used to take care of turbulent

fluctuations of the gas-solid mixture.
Initially, there was no solid in the riser and the concentration of CO2 was zero as well.
The summary of the boundary conditions is shown in Table 1.
A second order discretization scheme was used to discretize the governing equation
throughout the domain including 34x1200 uniform rectangular cells. In order to check
the grid independence of the solution, the computations were also performed using
two other coarser grids. The comparison between the calculated pressure drop using
34x1200 and 17x600 uniform grids showed an insignificant difference in the
calculated pressure drop along the riser.
REACTION KINETIC MODEL

There is very little information available on the kinetics of the carbonation reaction of
K2CO3 in the literatures. Onischak and Gidaspow (14) have proposed a first order
homogenous reaction kinetic model which is dependent only on CO2 concentration
and is independent of sorbent and H2O concentration. Recently, Park et al. (15)
investigated different kinetic models including a Homogenous Model (HM), Shrinking
Core Model (SCM), and Deactivation Model (DM). They concluded that the
Deactivation Model explains fixed bed reactor experimental data better than the
other two above-mentioned models.
Garg et al. (7) used the proposed HM to simulate a similar process. Although their
simulation was able to capture the CO2 concentration at the outlet of the riser, the
simulation results were approximately three times more sensitive to the changes in
4
gas flow rate than observed in their experiments. It seems that the independence of
the reaction model to gas velocity is one of the issues of HM.
The Deactivation Model (DM) proposed by Park et al. includes gas volumetric flow
rate in the kinetic model. The concept of this model is based on analogy between
deactivation of catalyst particles by coke formation and deactivation of sorbent
particles by carbonation.
Table 1. Summary of Boundary Conditions for Baseline Operating Condition
Solid inlet Gas inlet Outlet Wall
2
Solid mass flux = 21 kg/m s Gas velocity= 2 m/s No slip
condition for
gas phase
Solid volume fraction = 0.6

P = 1 atm
Solid volume fraction= 0 Partial slip
Carrier gas mass condition for
flux = 0.05 kg/m s
2 solid phase
Mass fraction K2CO3 = 0.35 Mass fraction CO2 = 0.1

Mass fraction KHCO3 = 0 Mass fraction H2O = 0.15
Mass fraction Inert = 0.65 Mass fraction N2 = 0.75
IN the deactivation Model, the effect of the formation of a product layer on the
surface of sorbent particles (which results in an additional diffusion resistance and
reduction in available active surface area) is lumped into a reducing activation factor
with an exponentially deactivation rate.
R = k CCO2 a
Where a is activity of the sorbent and defined as:
[1 − exp(τ .k s (1 − exp(− k d t )))]
a = exp[ exp(− k d t )]
1 − exp(− k d t )
τ , called surface time, is defined as the ratio of available pore surface to the
volumetric flow rate of flue gas. ks= 2.44x10-3m/s and kd = 1.42x10-4/s are surface
reaction constant and deactivation constant, respectively. (15)
RESULTS
The simulation results for CO2 removal percentage and sensitivity analysis of the
model to the changes in gas flow rate and pressure drop along the riser are
presented in this section. Simulations ran for 200 seconds of the processing time
and, as it takes about 90 seconds for the solid inventory in the riser to become
stable, the first 100 seconds of the simulations were not considered in the calculation
of the time averaged results. Our results are being compared with the experimental
data of KIER provided by Yi et al. (5).
5
Figure 2 shows the simulated axial profile of time averaged CO2 mass fraction and
CO2 removal percentage at the different elevations in the riser at the baseline
Time averaged CO2 removal percentage %

0.1 60
operating condition.
The CO2 removal
Time averaged CO2 mass fraction
0.09 50 percentage at the

outlet of the riser is
0.08 40 58%, which is very
close to the
0.07 30 reported 54%
removal in the
0.06 20
experimental data.
0.05 10 In addition, the axial
profile of the time
0.04 0 averaged CO2 mass
0 1 2 3 4 5 6
Riser Height (m) fraction showed that
around 60% of CO2
Figure 2. Simulated time averaged CO2 mass fraction and removal takes place
CO2 removal percentage in the first 0.6 m of
rise (mixing zone),
which is due to the higher solid concentration and solid circulation in this region.
Furthermore, the effect of gas flow rate on the percentage of CO2 removal has been
investigated. The results showed that the increasing inlet gas flow rate (inlet gas
velocity) decreases the CO2 removal percentage, which is in-line with the
experimental data. The higher gas flow rate means shorter residence time, which
results in reduction of surface time, τ , in DM and, in turn, increases the deactivation
factor and decreases the CO2 removal (see Figure 3). Moreover, our model was able
to capture the sensitivity of the CO2 removal process to the gas flow rate much better
than Garg et al. (7) who used the homogeneous reaction model. Sensitivity of CO2
removal to the changes in the solid circulation rate was also investigated. As was
expected, increasing the solid circulation rate resulted in increased CO2 removal
percentage. Similar to the
Table 2. Differential Pressure at Different Elevations experimental data and the
simulation of Garg et al. (7),
Differential Pressure Differential Pressure the results of our simulation
(mm H2O) (mm H2O)
were also sensitive to the
KIER Experiments Simulation variations in the solid
Yi et al (5) circulation rate. However,
due to some inconsistencies
DP1 100 107 in the reported data by Yi et
al. (5), no comparison with
DP2 200-500 335 their data was made in this
study.
DP3 100-210 270 Table 2 shows the
comparison between the
DP4 70 67 pressure drop predicted
using our simulation with the
experimental results of Yi et al. (5) at 4 different elevations of 0.52 m, 2.27 m, 4.07
m, and 5.87 m which are referred to as DP1, DP2, DP3, and DP4, respectively. Our
simulation closely predicted the pressure drop over the DP1, DP2, and DP4 sections
6
and over predicts the
70 Baseline pressure drop over the
operation DP3 section. This could
CO2 Removal %
60 condition be due to a couple of
reasons. First, in the 20
50 hours of pressure drop
40 profiles reported by
KIER, there is a sudden
30 reduction over the DP2
KIER and DP3 sections at
20 Simulation
Garg et al around the 11th hour of
10 operation that remains
1 1.5 2 2.5 3 3.5 up to the end of the
experiment. This
Inlet Gas Velocity (m/s)
reduction in pressure
Figure 3. Effect of inlet gas velocity on CO2 removal drop is apparently due to
percentage an undisclosed change
in the operating condition
that cannot be implemented in our simulation. The second possible reason could be
due to the inaccuracy of the EMMS drag model in predicting a wide range of solid
phase concentration and heterogeneities.
CONCLUSION
A 2-D Eulerian-Eulerian CFD simulation based on kinetic theory of granular flow in
combination with deactivation kinetic model has been used to simulate the KIER
experiments for CO2 sorption in a circulating fluidized bed using solid sorbent. The
simulation was able to predict CO2 removal percentage at the riser outlet at different
gas flow rate in good agreement with experimental data. Our simulation was also
able to predict the pressure drop in the riser and dependency of the CO2 conversion
to gas flow rate in line with the KIER experimental data.
NOTATION
a Activation coefficient (-) yi Species i mass fraction
C D0 Drag coefficient (-) γs Collisional dissipation of solid
fluctuating energy (kg/s-m3)
dp Particle diameter (m) κs Conductivity of solid fluctuating
energy (kg/m-s)
kd Deactivation rate constant (1/s) θ Granular temperature (m2/s2)
ks Surface reaction constant (m/s) β gs Inter-phase drag coefficient
(kg/s-m3)
• Inter-phase mass transfer (kg/m3-s) ρi Density of phase i (kg/m3)
m
Rj Heterogeneous reaction rate (kg/m3-s) τi Stress tensor of phase i (Pa)
ui Superficial velocity of phase i (m/s) εi Volume fraction of phase i (-)

vi Local velocity of phase i (m/s) τ Surface time (s/m)
7
REFERENCES
1. DOE/NETL Advanced Carbon Dioxide Capture R&D Program: Technology Update,
2009, http://www.netl.doe.gov/technologies/coalpower/ewr/index.html
2. Hayashi, H., Taniuchi, J., Furuyashiki, N., Sugiyama, S., Hirano, S., Shigemoto, N.
and Nonaka, T., “Efficient Recovery of Carbon Dioxide from Flue Gases of Coal-Fired
Power Plants by Cyclic Fixed-Bed Operations over K2CO3-on-Carbon”, Ind. Eng. Chem.
Res., 37, 185-191, 1998
3. Ryu, C.K, Lee, J.B., Eom, T.H., Oh, J.M., Yi, C.K,”Development of Na and K-Based
Sorbents for CO2 Capture from Flue Gas”, FOURTH ANNUAL CONFERENCE ON
CARBON CAPTURE AND SEQUESTRATION DOE/NETL, May 2-5, 2005
4. Lee, S.C., Chae, H.J., Lee, S.J., Park, Y.H., Ryu, C.K, Yi, C, K., Kim. J.C., “Novel
regenerable potassium-based dry sorbents for CO2 capture at low temperatures” Journal
of Molecular Catalysis B: Enzymatic 56, 179–184, 2009
5. Yi, C., K., Jo, S., J., Seo, Y., Lee, J., B., Ryu, C. K., “Continuous operation of the
potassium-based dry sorbent CO2 capture process with two fluidized-bed reactors”,
International journal of greenhouse gas control, 1, 31-36, 2007
6. Park, Y., C., Jo, S., J., Ryu, C., K., Yi, C., K.,” Long-Term Operation of Carbon Dioxide
Capture System from a Real Coal-Fired Flue Gas Using Dry Regenerable Potassium-
Based Sorbents” Energy Procedia 1, 1235–1239, 2009
7. Garg, R., Shahnam, M. and Huckaby, E. D., “Continuum simulations of CO2 capture
by dry regenerable Potassium based sorbents”, 7th International Conference on
Multiphase Flow, ICMF 2010, Tampa, FL, May 30 – June 4, 2010
8. Chalermsinsuwan, B., Piumsomboon, P., Gidaspow, D., “A Computational Fluid
Dynamics Design of a Carbon Dioxide Sorption Circulating Fluidized Bed”, AIChE
Journal, Vol. 56, No. 11, 2010
9. Arastoopour, H., “Numerical simulation and experimental analysis of gas/solid flow
systems: 1999 Flour-Daniel Plenary Lecture” Powder Technology, 119, 59-67, 2001
10. Benyahia, S., Arastoopour, H., Knowlton, T.M., Massah, H., “Simulation of particle
and gas flow behavior in the riser section of a circulating fluidized bed using the kinetic
theory approach for the particulate phase”, Powder Technology, 112, 24-33, 2000
11. Yang, N., Wang, W., GE, W., Wang, L., Li, J., “ Simulation of Heterogeneous
Structure in a Circulating Fluidized Bed Riser by Combining the Two-Fluid Model with the
EMMS Approach”, Ind. Eng. Chem. Res., 43, 5548-5561, 2004
12. Gidaspow, D., “Multiphase flow and fluidization”, Academic Press, 1994
13. Nikolopoulos, A., Atsonios, K., Nikolopoulos, N., Grammelis, P., Kakaras, E., “An
advanced EMMS scheme for the prediction of drag coefficient under a 1.2MWth CFBC
isothermal flow—Part II: Numerical implementation”, Chem. Eng. Science 65, 4089–
4099, 2010
14. Onischak M, Gidaspow D., “Kinetics of the reaction of CO2 with solid K2CO3”, 73rd
National AIChE Meeting, Minneapolis, USA, 1972.
15. Park, S.W, Sung, D. H., Choi, B.S., Lee, J.W., and Kumazawa, H., “Carbonation
Kinetics of Potassium Carbonate by Carbon Dioxide”, J. Ind. Eng. Chem. Vol 12, No. 4,
522-530, 2006
8
RESEARCH ON HEAT TRANSFER INSIDE THE FURNACE OF
LARGE SCALE CFB BOILERS
Ruiqing Zhang, Hairui Yang, Hai Zhang, Qing Liu, Junfu Lu, Yuxin Wu
ABSTRACT
Field tests in one unit of 135MWe and two units of 300MWe commercial Circulating
Fluidized bed (CFB) boilers (A&B) with different structures were carried out. The
influence of operating conditions on the thermal boundary layer, local heat transfer
coefficient and peripheral distribution of heat transfer coefficient were studied. It was
found that, in the 135MWe and 300MWe-A CFB furnace, the thickness of the thermal
boundary layer was almost constant, about 100mm, and independent of the height
above the distributor and the boiler load. The local heat transfer coefficient increased
with increasing load as well as the coal feeding rate and air volume in both the
135MWe and 300MWe-A CFB boilers.
The boiler structure and heating surface layout had a great influence on the
distribution of the heat transfer coefficient in the large-scale CFB boilers. In both the
135MWe furnace and the 300MWe-B CFB boilers, the heat transfer coefficient was
lower in the center than near the corner due to higher suspension density in the
corner. In the 300MWe-B CFB with heating surfaces in the furnace, because of the
uneven layout of the heating surface and the mal-distribution of gas-solid flow
caused by the asymmetric arrangement of cyclones, heat transfer coefficients tended
to be higher in the middle part than at the walls.
INTRODUCTION
The distribution of the heat flux and the heat transfer coefficient inside a circulating
fluidized bed (CFB) boiler, which is related to the arrangement of heating surfaces, is
of great significance to the design and operation of the boiler. Many studies on heat
transfer in CFB boilers have been conducted (Glicksman (1); Wirth (2); Andersson
and Leckner (3); Basu and Nag (4)) and the results showed that the heating transfer
coefficient from bed to heating surface was affected by the solids suspension density,
particle size and bed temperature. Pagliuso, et al. (5) found that the profile of the
heat transfer coefficient along the riser correlated well with that of the solid
suspension density. They also found that the heat transfer coefficient increased with
the increasing particle size, which became more obvious for smaller particles and
higher suspension density. Breitholtz and Leckner (6) presented a correlation
between heat transfer coefficient and suspension density based on measurements in
six CFB boilers ranging from 12 to 300 MWth. In addition, with increasing bed
temperature, Tb, thermal conductivity and radiation heat transfer of the gas increased
accordingly, which lead to an increase of the heat transfer coefficient. This was
confirmed by the test of Jestin, et al. (7) in a 125MWe CFB boiler and the experiment
of Jeon, et al. (8).
Many studies on gas-solid flow and heat transfer in CFB boilers were carried out in
laboratory scale CFB combustors, which differ from industrial ones because of
smaller height to diameter ratios. Zhang, et al. (9) and Noymer, et al. (10) found the
height to diameter ratio of a riser has a significant impact on the gas-solid flow inside
the furnace. Besides, considering the difference in temperature, particle size
distribution and suspension density between laboratory scale CFB combustors and
industrial ones, previous test results may not totally represent those found in
industrial CFB boilers. At the same time, the heat transfer coefficient is also affected
by boiler load, which was proven by Zhang et al. (11).
Therefore, it is necessary to measure the distribution of the heat transfer coefficient
inside an industrial CFB boiler for proper design and arrangement of heating
surfaces. In recent years, large-scale CFB boilers have been developed, however,
only a few test results on heat transfer in large-scale CFB boilers have been
published. To compare and analyze heat transfer characteristics in different
large-scale CFB boilers, field tests in one unit of 135MWe CFB boiler and two units of
300MWe CFB boilers with different structures were conducted. The influence of
boiler load on the local heat transfer coefficient and thermal boundary layer
distribution were studied in this work.
EXPERIMENTAL
The tests were carried out in a 135MWe CFB boiler and two 300MWe CFB boilers,
which are all reheat, natural circulation boilers. The 135MWe CFB boiler has single
furnace with height of 38m from distributor to the roof and with a cross section of
6.6m×13.1m. Two refractory-lined cyclones were used as the gas solid separators.
Lean coal was burnt during the experimental test. Two 300MWe CFB boilers,
referred to as A and B respectively, have different furnace structures. Boiler A has a
pants leg furnace structure with height of 36m and a cross section of 14.8m×12.6m.
Four cyclones are arranged on both sides of the furnace. A higher bed temperature
(890℃) was adopted for coal with a low volatile content to improve combustion
efficiency. The boiler was operated with a high solids circulation rate. Boiler B has a
single furnace with height of 40m from the distributor to the roof, and a cross section
of 8.4m×28.2m. There were two water cooled wing walls hung in the furnace. Three
steam-cooled cyclones are used as gas solid separators.
Local heat transfer coefficient (a), heat flux (b), the peripheral distribution of the heat
transfer coefficient (c), the temperature profile near the wall (d) and the vertical
distribution of the solid suspension density along the furnace height at different loads
(e) were measured respectively.
The local heat transfer coefficient, K, was measured by a water-cooled conductive
heat flux meter designed by Tsinghua University, shown in Fig.1. According to the
heat conduction law, the local heat transfer coefficient can be calculated from the
axial temperature gradient inside the probe-defined as heat flux method (HFM).
The heat flux, q, was calculated based on the temperature difference measured with
thermocouples installed in the fin-tube (shown in Fig.2) with a two-dimensional finite
element calculation method (FEM), which has been investigated by many
researchers (Andersson and Leckner (12); Zhang, et al. (13); Wang, et al. (14);
Zhang et al. (15)). The heat flux profile was obtained by arranging a number of
measuring points peripherally at different heights along the furnace. The relationship
between the heat transfer coefficient and the heat flux can be expressed as:
q=K△T
The temperature difference, △T, was determined by the difference between the
furnace temperature and the stream temperature at each point. The former can be
gained from the temperature distribution at certain boiler height. The stream
temperature inside the tube is the saturated water temperature under drum pressure.
So, the heat transfer coefficient can be derived from equation above by knowing the
heat flux q and the temperature difference △T.
The temperature profile near the wall was measured with a multi-thermocouple probe,
shown in Fig. 3. Pressure sensors were placed at different level to monitor the
vertical profile of the suspension density along the furnace height.
Measurements (a)~(e) were all conducted in the 135MWe CFB boiler while
measurements (a), (d), (e) were performed in the 300MWe-A CFB boiler and
measurements (b), (c), (e) performed in the 300MWe-B CFB boiler.
Figure 1. Heat flux meter
combustor chamber
2
3 Insulation
Figure 2. Thermal couple distribution on Figure 3. Temperature

tube surface measurement probe
RESULT AND DISCUSSION
Thermal boundary layer
Fig.4 shows the temperature profiles near the wall in the 135MWe CFB boiler at full
load. Measurement points were located at three different heights. Fig.5 shows
temperature profiles near the wall in the 300MWe-A CFB boiler at full load.
Measurement points 1-4 were symmetrically located 3m below the cyclones, with 1
and 2 on the rear wall and 3 and 4 on the front wall. Point 5 was located 3m above
the distributor, where the bed temperatures were lower than those measured at 1-4.
The temperature profiles remained similar at different boiler loads. It was found that
furnace temperatures increased significantly in the region near the wall, about
100mm, and then become almost constant, at a temperature considered to be the
furnace core temperature. The thickness of the thermal boundary layer was defined
as the distance to the tube wall where the temperature was 90% of the core
temperature. Figs.4 and 5 show that the thicknesses of the thermal boundary layers
measured in both boilers were about 100mm and were independent of the boiler load
and furnace height. This was consistent with the study of Wang et al. (16).
Local heat transfer coefficient
Fig.6 shows the measured local heat transfer coefficient in the 135 MWe CFB boiler.
Heat transfer coefficients increase with increasing load and decrease with increasing
height, which agrees well with previous work (Zhang, et al. (11)). When the boiler
load increases, the coal feeding rate, gas velocity and air volume increase
correspondingly, resulting in a higher particle velocity that results in more particles
participating in contacting the water wall per unit area. As a result, the heat transfer
coefficient increases. The solid suspension density gradually decreases in the
furnace from the distributor to the roof. Therefore, the heat transfer coefficients
decrease with the height for a constant boiler load.
1000 1000
900 900
800 800
Temperature (oC)
Temperature (oC)
700 700
mearsuring point-1
600 600 mearsuring point-2
14m mearsuring point-3
500 500 mearsuring point-4
22.2m
26m mearsuring point-5
400 400
300 300
0 200 400 600 800 1000 0 40 80 120 160 200
Distance from fin (mm) Distance from fin (mm)
Figure 4. Temperature profile (135MWe) Figure 5. Temperature profile (300MWe-A)
160
Heat Transfer Coefficient (W/(m2.K))
Output 85MWe
Output 100MWe
Output 135MWe
120
80
40
12 16 20 24 28
Furnace Height From Distributor (m)
Figure 6. Local heat transfer coefficient (135MWe)

Table 1．Local heat transfer coefficient at measurement point-4 (300MWe-A)
Furnace Local heat transfer
Measurement Boiler load
temperature coefficient
point o
MWe C W/(m2K)
260 908 161
4
300 915 183
The measurement of the local heat transfer coefficients at point 1-4 in 300MWe-A
boiler verified the conclusions above. Typical results are listed in Table 1. The heat
transfer coefficient at point 4 increased from 161 W/(m2K) to 183 W/(m2K) when the
boiler load was increased to 300MWe from 260MWe. Though the effect of height on
the heat transfer coefficient is not proved directly, it is reasonable to assume that the
coefficient would decrease with increasing height because the suspension density
decreases with height.
Peripheral distribution of the heat transfer coefficient
The peripheral distribution of the heat flux at different levels, from which the heat
transfer coefficient distribution can be derived, was indirectly measured in the 135
MWe and 300 MWe-B boiler by the finite element method discussed above.
In the test of the 135MWe CFB boiler, measuring points were arranged in the left
front wall and the front left side wall at heights of 12m, 18.5m, and 23m above the
distributor. The bed temperature was about 882~894℃, the water temperature was
about 353~354℃, the superficial gas velocity was about 5.78~5.86m/s, the tube
dimension was 60×5mm and the tube pitch was 90 mm. Fig. 7 shows the heat
transfer coefficient distribution over half of the front wall and the left side wall at
different height levels. Consistent with the result by HFM, the heat transfer
coefficients by FEM also decreased with the increasing height. In the cross section,
the heat flux and the heat transfer coefficient were lower in the center than in the
corner on both the front wall and the side wall.
190 190
23.0m 23.0m
185 185 18.5m
18.5m
12.0m 12.0m
180 180
175 175
170 170
165 165
160 160
0.0 0.1 0.2 0.3 0.4 0.5 0.0 0.1 0.2 0.3 0.4 0.5
Dimensionless Distance to the Center of the Side Wall Dimensionless Distance to the Center of the Front Wall
(a) (b)
Figure 7. Peripheral distribution of heat transfer coefficient on side wall

and front wall (135MWe)
In the 300MWe-B boiler, the measuring points were arranged in the left half of the
rear wall and the back half of the left side wall at heights of 13m (L1), 19m (L2), 25m
(L3), 30m (L4), and 35m (L5). In particular, the entire rear wall and left side wall at L1
were fitted with measuring points. The water temperature was about 358.6~359.3℃,
the superficial gas velocity was about 3.6~3.9m/s, the water tube dimension was
57×6.5mm and the tube pitch is 87mm. As the heat transfer at different heights was
similar, results in L1 were set as an example for the analysis. The heat flux and the
heat transfer coefficient distribution along the rear wall are shown in Figs.8 and 9
respectively. It is seen that, the heat fluxes between the wing walls appear to be
higher than between the side wall and the wing wall. Also, heat fluxes on the left side
are higher than on the right side. For the correlation of the coefficient and heat flux by
calculation, the heat transfer coefficient prolife trend was similar trend to the pattern
of the heat flux profile.
In actual operation, it is found that the solids mix well in the dense zone at the bottom
of the furnace. In the upper furnace, the two wing walls divide the furnace into three
parts, marked as left, middle and right. Three cyclones were also arranged
asymmetrically. Therefore, the gas-solid flows in these three regions were relatively
independent, which prevents solids in upper furnace from experiencing good lateral
mixing. Furthermore, the layout of the heating surfaces was not uniform. A1 is the
heating surface area in the left or right section, A2 is the heating surface area in the
middle section. Calculating from the heating surface structure, A2/A1 is about 0.91,
which means less heating surface is placed in the middle part compared with that in
left or right part. As a result, the temperature between the wing walls tends to be
higher than that between the side wall and the wing wall. This can explain the
temperature non-uniformity. The uneven layout of the heating surface is the essential
reason for the uneven heat flux distribution.
120 200
between side and wing wall between side and wing wall
between wing walls between wing walls
160
90
Heat Flux KW/m2
120
60
80
30
40 left side wall right side wall
left side wall right side wall
0 0
0.0 0.2 0.4 0.6 0.8 1.0 0.0 0.2 0.4 0.6 0.8 1.0
Dimensionless Distance from Left to Dimensionless Distance from Left to
Right Side Wall Right Side Wall
Figure 8. Peripheral distribution of Figure 9. Peripheral distribution of heat

heat flux in the whole rear wall transfer coefficient in the whole rear
(300MWe-B) wall(300MWe-B)
It is clear that the heat flux and heat transfer coefficient have a close relationship with
suspension density and bed temperature. The peripheral distribution of the bed
temperature, shown in Fig.10, gives good agreement with that of heat flux with the
fact that bed temperature in center section was greater. Also, the temperature on the
left side seems to be lower than that of right side, contrary to the heat flux distribution.
This is supported by the result that the section has a greater suspension density than
right, as derived from the pressure profile during the experiment. It is the combined
effects of the suspension density and the bed temperature, that result in the heat flux
and heat transfer coefficient characteristics presented above.
1000
between side and wing wall
between wing walls
960
Furnace Temperature oC
920
880
left side wall right side wall

840
800
0.0 0.2 0.4 0.6 0.8 1.0
Dimensionless Distance from Left to Right Side Wall
Figure 10. Temperature distribution in the furnace (300MWe-B)

In Fig.9 the heat transfer coefficient was found to increase near the corner formed by
the rear wall and either side wall or the wing wall, which is consistent with what was
found in the 135MWe boiler. It can be inferred that in large-scale CFB boilers, a
corner effect does exist, causing the heat flux and the heat transfer coefficient near
the corner to increase compared to the central area. Considering the relationship
between the heat transfer coefficient and the suspension density, the suspension
density in this area is likely to be higher, which is also indicated by the fact that tube
erosion near the corner is greater than the central area in CFB boilers.
CONCLUSIONS
Field measurements mainly on heat transfer performance has been carried out in a
135 MWe CFB boiler and two 300 MWe CFB boilers with different configurations. It
was found that:
1. The thickness of the thermal boundary layer is about 100mm and remains
constant with height above with distributor and with boiler load.
2. The local heat transfer coefficient decreases with increasing furnace height and
with decreasing boiler load.
3. The heat flux and the heat transfer coefficient have an uneven distribution in
large-scale CFB boilers. Near the corner formed by rear wall with the side wall
and wing wall, the heat flux and heat transfer coefficient is higher than that in the
central area. In a 300 MWe CFB boiler with two wing walls arranged unevenly
inside the furnace, heat flux and heat transfer coefficient tend to be higher in
middle section than in the left or the right section at a particular level.
ACKNOWLEDGMENT
Financial support of this work by High Technology R&D (863) (2009AA05Z302,
2007AA05Z303) are grateful acknowledged
NOTATION
A1 heating surface area of the left or right part in 300 MWe-B, m2
A2 heating surface area of the intermediate part in 300 MWe-B, m2
K heat transfer coefficient, W/(m2K)
q heat flux, W/m2
△T temperature difference, K
Abbreviations
CFB Circulating Fluidized bed
FEM Finite element method
HFM Heat flux method
REFERENCES
1. Glicksman, L. R., “Circulating Fluidized Bed Heat Transfer”, in “Circulating
Fluidized Bed Technology II”, P. Basu and J. F. Large, Eds., Pergamon Press,
Oxford (1988), pp13-29.
2. Wirth, K. E., “Prediction of Heat Transfer” in “Circulating Fluidized Beds” in
“Circulating Fluidized Bed Technology IV”, A. A. Avidian, Eds, (1994), pp291-296.
3. Andersson, B. A. and Leckner, B., “Local Lateral Distribution of Heat Transfer on
Tube Surface of Membrane Walls in CFB Boilers”, in “Circulating Fluidized Beds”
in “Circulating Fluidized Bed Technology IV”, A. A. Avidian, Eds, (1994),
pp311-315.
4. Basu, P., and Nag, P. K., “A Review on Heat Transfer to Walls of a Circulating
Fluidized Bed Furnace”, Chemical Engineering Science 1, 1-26 (1996).
5. Pagliuso, J. D., Lombardi, G., Godstein, L., et al, “Experiments on the local heat
transfer characteristics of a circulating fluidized bed”, Experimental Thermal and
Fluid Science 20(3-4), 170-179 (2000).
6. Breitholtz, C and Leckner, B, “Wall average heat transfer in CFB boilers”, Powder
Technology 120(1-2), 41-48 (2001).
7. Jestin, L., Meyer, P., Schmitt, C., et al, “Heat transfer in a 125 MWe CFB boiler”,
Proceedings of the Engineering Foundation Conference, Australia (1992).
8. Jeon, J. H., Kim, S. D., Kim, S. J. and Kang Y., “combustion and heat transfer
characteristics in a square internally circulating fluidized bed combustor with draft
tube”, Fuel 87 , 3710–3713 (2008).
9. Zhang, W., Johnsson, F., Leckner, B., “Fluid-dynamic boundary layers in CFB
boilers”. Chemical Engineering Science 50(2), 201-210 (1995).
10. Noymer, P. D., Hyre, M. R., Clicksman, L. R., et al, “The effect of bed diameter on
near-wall hydrodynamics in scale-model circulating fluidized beds”, International
Journal of Heat and Mass Transfer 43(19), 641-3649 (2000).
11. Zhang, M., Xiao, P., Lu, H. A. and Jiang, M. H., “Experimental Investigation on
Heat Transfer Coefficient of CFB Boiler in Gaoba Power Plant”, Thermal Power
Generation 4, 35-37 (2002) (in Chinese).
12. Andersson, B A, Leckner, B, “Experimental Methods of Estimating Heat Transfer
in Circulating Fluidized Bed”, Int. J. Heat Mass Transfer 35, 3353-3362 (1992).
13. Zhang, H., Lu, J. F., Yang, H. R., et al., “Heat Transfer Measurements inside the
Furnace of a 135MWe CFB Boiler”, Proceedings of the 8th International
Conference on Circulating Fluidized Beds Technology. Hangzhou, pp254-260
(2005).
14. Wang, Y., Lu, J. F., Yang, H. R., et al., “Measurement of Heat Transfer in a 465t/h
Circulating Fluidized Bed Boiler”, Proceeding of the18th International Fluidized
Bed Combustion Conference, May 2005, Toronto Canada, No.96 (2005).
15. Zhang, P., Lu, J. F., Yang, H. R., et al., “The heat transfer coefficient distribution in
a 300MWe CFB boiler”, Proceeding of the 20th International Fluidized Bed
Combustion Conference, Xi’an, China, pp167-171 (2009).
16. Wang, J., Zhao, X., Wang, Y., et al, “Thermal boundary layer in the CFB boiler
riser”, China P articuology 4 (3-4), 131-135 (2006).
MANUFACTURE OF GRANULAR POLYSILICON FROM
TRICHLOROSILANE IN AN INTERNALLY CIRCULATING
FLUIDIZED BED REACTOR
Chenjing Wang, Tiefeng Wang, Zhanwen Wang
Beijing Key Laboratory of Green Reaction Engineering and Technology
Department of Chemical Engineering, Tsinghua University, Beijing 100084, China
T: 86-10-62797490; F: 86-10-62772051; E: wangtf@mail.tsinghua.edu.cn
ABSTRACT
A lab scale internally circulating fluidized bed (ICFB) with a centrally located draft
tube was designed to make polysilicon from trichlorosilane. Experimental results and
evaluations showed that particle circulation could carry enough heat for reaction and
effectively decrease wall deposition. Well grown granular polysilicon was obtained in
a stable fluidization state and particle circulation rate.
INTRODUCTION
Solar grade silicon is in ever-increasing demand due to the rapid development of the
photovoltaic (PV) industry (1). One challenge the PV industry is currently facing is the
development of cheap solar grade silicon feedstock (2). The traditional method for
producing high purity polysilicon is the Siemens process that uses the decomposition
of trichlorosilane (SiHCl3 or TCS) on a high purity silicon rod in a bell-jar reactor.
However, the cost of polysilicon made by this method (30-45 $·kg-1) is too high for the
PV industry (3,4). Therefore, several manufacturers have developed other new
production technologies for solar grade polysilicon (5), which could be divided into
two categories. The metallurgical routes produce solar grade silicon directly from
metallurgical grade silicon by a purification process. The chemical routes are based
on different reactor types such as a tubular reactor and fluidized bed reactor for the
decomposition of a silicon-containing gas.
The technology that makes polysilicon by decomposing a silicon-containing gas in a

fluidized bed reactor is considered to be the most attractive alternative to the
conventional bell-jar process (6). This technology produces polysilicon in the form of
silicon granules instead of the traditional silicon rods (7). The purity level of the
granular materials produced is slightly lower than that produced with the Siemens
process, but it meets the requirement of the PV industry. The feasibility and
operating costs have been estimated in a pilot scale reactor by Wacker-Chemie, who
showed that the energy consumption of polysilicon from the fluidized bed process
1

can be decreased to below half that of the Siemens process. The low energy
consumption advantage would be more pronounced in large scale reactors.
The chemical vapor deposition (CVD) reaction of polysilicon from SiHCl3 is a highly
endothermic reaction and is sensitive to operating temperature. In a traditional
fluidized bed reactor, deposition on the inner reactor wall is significant. This
phenomenon will limit the life time of the reactor and cause problems due to the
different thermal expansion coefficients of silicon and quartz. One effective way to
limit wall deposition is the design of a novel reactor with an appropriate heating
method. This is the most important issue in future demonstration of making
polysilicon in a fluidized bed reactor.
In this work, a type of internally circulating fluidized bed (ICFB) with a novel gas
distributor was developed for producing high purity polycrystalline silicon. The ICFB
consisted of a downcomer with low gas velocity and a riser with high gas velocity.
The separate aeration of gas for the riser and downcomer provides a more flexible
operation.
EXPERIMENTAL
In order to determine optimized reaction conditions such as temperature, molar ratio

of H2 to SiHCl3 and superficial gas velocity, a lab scale bubbling fluidized bed reactor
(I.D.=0.025 m, H=0.6 m) was designed for producing granular polysilicon from SiHCl3.
The schematic diagram of the experimental apparatus is given in Figure 1. The
fluidized bed reactor was made of quartz and heated by a resistance furnace outside
the reactor. Liquid SiHCl3 was vaporized and mixed with H2 in a specially designed
heated mixer, and the gas mixture was fed into the reactor through a gas distributor
at the bottom of the reactor. The fluidized bed had an expanded head of 0.08 m I.D.
to reduce particle entrainment. The gas distributor was placed below the heated zone
to avoid plugging that would occur if there was silicon deposition on it. At the
beginning of the experiment, the fluidized bed reactor was loaded with silicon
particles. The incipient fluidization velocity, Umf, was calculated with the following
empirical correlation (8):
de2 ( ρp - ρ )g
Umf =
1650μ
The cold flow experiments were first carried out in an ICFB reactor (I.D.=0.12 m,
H=0.80 m) made of Plexiglas to determine the appropriate superficial gas velocity in
the real CVD reaction. A Schematic of the ICFB is shown in Figure 2. The draft tube
(I.D.=0.07 m, H=0.25 m) with 24 orifices of 0.01 m in diameter was fixed in the
bottom of the reactor. For gas supply to the reactor, two separate tubular gas
2

distributors were used: one was in the annular downcomer with 12 orifices, and the
other was in the central riser with 24 orifices. All the orifices were 2 mm in diameter.
An expanded section (I.D.=0.25 m, H=0.4 m) was installed in the top of the reactor to
reduce particle entrainment. The bed was loaded with silicon beads (dp=300 μm,
ρp=2.71 kg·m-3, Umf=0.051 m·s-1) at the beginning of the experiment.
The real CVD reactor for making polysilicon from SiHCl3 on granular silicon is the
same in structure as the cold flow reactor. It was made of quartz and heated by a
resistance furnace outside the reactor.
Figure 1. Schematic of experimental apparatus Figure 2. Schematic of cold

flow ICFB
The product gas contained SiHCl3, SiCl4, SiH2Cl2 and HCl. The molar fractions of
these species were determined by GC analysis using an empirical molar calibration
ratio. The main reactions were
SiHCl3 +H2 → Si+3HCl (1)
4SiHCl3 → Si+3SiCl4 +2H2 (2)
SiHCl3 +H2 → SiH2Cl2 +HCl (3)
The conversion of SiHCl3 (X), the yield of silicon (Y) and the selectivity to silicon (S,
which was defined as the molar ratio of the produced silicon to the converted SiHCl3)
calculated from the molar fractions of silicon-containing products and HCl. The
microstructure of the polysilicon deposited on the surface of seed particles was
investigated by scanning electron microscopy (SEM, JEOL-7410). The particle size
distribution of the silicon particles was obtained using Image-Pro Plus software by
analysis of high-resolution digital photos of the silicon particles.
3

The CVD in Bubbling Fluidized Bed Reactor
The preparation of polysilicon from SiHCl3 was studied in a bubbling fluidized bed
reactor under a wide range of reaction conditions in previous research with small size
silicon particles (dp=300 μm). The effects of temperature (T), molar ratio of H2 to
SiHCl3, superficial gas velocity (Ug) and particle seed loading were investigated. The
temperature and molar ratio of H2 to SiHCl3 have notable effects on the reaction. The
conversion was more sensitive to temperature below 900 oC. The optimized
operating conditions were determined to be 950~1050oC for temperature, 4:1~6:1 for
the molar ratio of H2 to SiHCl3, and 2.5~4.5 for fluidization number (Ug/Umf). The
deposition reaction occurred by heterogeneous deposition to produce polysilicon,
and this avoided the generation of fines which would occur in silane pyrolysis by
homogeneous deposition (9).
In this work, larger diameter granular silicon (dp=742 μm) was used to make
polysilicon, the molar ratio of H2 to SiHCl3 was 5 and the fluidization number was 4.5.
Well grown polysilicon product was obtained in the optimized operating conditions.
The influence of different temperatures (Figure 3) is the same as was found with the
deposition reaction with smaller size silicon particles (dp=300 μm). The average
particle was about 912 μm after CVD reaction. The total reaction time was about 8 h.
The growth rate was evaluated to be 10 μm/h, which was consistent with previous
experience.
70
X 40
60 Before CVD
Y
S
Size Distribution, %
50 30 After CVD
X, Y or S, %
40
20
30
20 10
10
0
0
750 800 850 900 950 1000 1050 400 600 800 1000 1200
o
T, C dp, μm
Figure 3. Conversion of SiHCl3 (X), Figure 4. Particle size distribution of

yield (Y), and selectivity (S) of Si silicon before and after CVD reaction
(molar ratio of H2 to SiHCl3 is 5) (dp, seed =742 μm, dp, product =912 μm)
Figure 5 shows the digital photos of the granular silicon before and after the CVD
reaction. It shows that compared with the seed silicon particles, the surface of silicon
4

granules become bright after the CVD reaction. The cross-sectional microstructure of
the silicon particle after reaction is shown in Figure 6. It shows the clear interface
between the deposited polysilicon and seed silicon particle after the CVD reaction.
The growth thickness was about 80μm, which was consistent with the average
diameter change analyzed by particle diameter size statistics.
Figure 5. Digital photos of granular Figure 6. Cross-sectional microstructure

silicon before and after CVD of granular silicon after CVD
Cold Flow Experiments in ICFB
A big problem in the manufacture of granular polysilicon from SiHCl3 in a fluidized

bed reactor is the deposition of silicon on the inner reactor wall. The ICFB reactor
has a centrally located draft tube to form separate heating and reaction zones in the
fluidized bed reactor. In this work, the interior of the draft tube was used as the
reaction zone and the exterior was the heating zone. The difference in superficial gas
velocity was the driving force for particle internal circulation between the heating
zone and reaction zone. In the ICFB, another important issue was to guarantee the
quantity of heat carried by the high temperature granular silicon for the CVD reaction.
One aim of the cold flow experiments was to estimate whether the particle solid
circulation rate was enough to supply heat for the reaction zone, the other was to
investigate whether the gas bypassing between the two zones was small enough to
reduce the wall deposition of silicon in the heating zone.
The same optimized operating conditions (T=1000 oC, H2:SiHCl3=5:1, fluidization

number=4.5) in the reaction zone were used to estimate the minimum solid
circulation rate in the ICFB. The conversion of SiHCl3 (X) at 1000 oC was about 63%
and the selectivity to Si (S) was about 45%. According to the optimized operating
conditions, the inlet amount of SiHCl3 was 0.008 mol·s-1. In consideration of the
reaction selectivity, the needed reaction heat was about 40.16 kJ·mol-1 SiHCl3. The
sensible heat of feed H2 and SiHCl3 from 25 oC to 1000 oC was about 192.35 kJ·mol-1
5

SiHCl3. So the total heat needed was 1.74 kJ·s-1. The heat capacity of silicon
granules at 1000 oC was 27.52 kJ·mol-1·K-1. Assuming that the temperature
difference between the heating zone and reaction zone was 25 oC, the needed
minimum solid circulation rate was 0.071 kg·s-1. Taking into account the
cross-sectional area of the heating zone, the needed minimum solid circulation rate
per unit area, Gs,min, was about 10 kg·m-2·s-1. The cold flow experiments show that
when UD/Umf>1.8 and UR/Umf>4.5, the solid circulation rate per unit area Gs (Figure 7)
could satisfy the heat demand. Heat supply could also be increased with a larger
heating zone or a larger temperature difference between the two zones. For example,
if the temperature difference between the heating zone and reaction zone was 50 oC,
Gs,min was about 5 kg·m-2·s-1.
30 80
UD/Umf
1.1
24 60
1.8
γDR and γRD, %
2.5
-1
Gs, kg·m ·s
18 UD/Umf=2.2
-2
40
γDR
γRD
12 o
25 C
Gs,min 20
6 o
50 C
Gs,min
0
4.5 6.0 7.5 9.0 10.5 4 5 6 7 8 9 10
UR/Umf UR /Umf
Figure 7. Effect of superficial gas Figure 8. Effect of superficial gas

velocity in downcomer (UD) and riser (UR) velocity in riser (UR) on gas bypassing
on solid circulation flux (GS) fraction γRD and γDR
The purpose of designing the ICFB reactor was to restrict wall deposition of
polysilicon during CVD reaction and prevent detrimental destruction of the reactor. In
the ICFB reactor, the circulating solid particles were transported upwards in the
reaction zone and moved downwards in the heating zone, providing heat transfer
between the two zones. At the same time, gas bypassed between the heating zone
and reaction zone occurred and should be investigated. In the cold flow experiments,
the amount of reaction gas SiHCl3 and the H2 bypassing from the reaction zone to
heating zone (γRD) was slight, while the amount of H2 bypassing from the heating
zone to reaction zone (γDR) was more notable. For example, when the fluidization
number of the two zones (UD/Umf and UR/Umf) was 2.2 and 7.0, the gas bypassing
fraction γDR was 60% and γRD was 4% respectively. According to the molar ratio of H2
to SiHCl3 (5) and a ratio of the reaction zone area and heating zone area (1:2), the
molar ratio of H2 to SiHCl3 after gas bypassing was 7 and 40. So the molar fraction of
SiHCl3 in heating zone was less than one-fifth of the molar fraction in the reaction
zone. According to the kinetics of CVD in the SiHCl3-H2 system (10,11), the reaction
6

is one-order reaction to the concentration of SiHCl3, so the deposition rate in the
heating zone is less than one-fifth of the reaction zone.
The CVD Reaction in ICFB
On the basis of the optimized operating conditions in the conventional fluidized bed
reactor and cold flow experimental results, tests to manufacture granular polysilicon
from SiHCl3 were carried out in an ICFB reactor of 0.12 m I.D.. Well grown polysilicon
product was obtained with a stable operation and depressed wall deposition.
CONCLUSIONS
1. Well grown granular polysilicon product was obtained with optimized operating
conditions in a bubbling fluidized bed reactor of 0.025 m I.D.. Compared with the
seed silicon particles, the silicon granules surface became bright and showed a
clear interface between the fresh polysilicon and the seed silicon particle after the
CVD reaction. The growth rate on the silicon particle surface was about 10 μm/h.
2. The effect of superficial gas velocity was investigated in cold flow experiments in
an ICFB reactor. When UD/Umf>1.8 and UR/Umf>4.5, the solid circulation flux Gs
(10 kg·m-2·s-1) could satisfy the heat supply needed. The heat transferred could
be increased with a larger heating zone or a larger temperature difference
between the heating zone and reaction zone. Analysis of the gas bypassing
showed that the ICFB reactor could effectively decreased the wall deposition.
3. Well grown polysilicon product was also obtained in an ICFB reactor of 0.12 m
I.D. with stable operation and depressed wall deposition at the optimized
operating conditions.
ACKNOWLEDGMENT
The authors gratefully acknowledge the financial support by the Beijing New Star
Project on Science & Technology of China under Grant No. 2009B35.
NOTATION
de equivalent diameter, m
dp diameter of particles, μm
g gravitational acceleration, m·s-2
Gs solid circulation rate, kg·m-2·s-1
H height of reactor, m
S selectivity to silicon, %
T temperature, oC
7

UD superficial gas velocity in downcomer, m·s-1
Ug superficial gas velocity, m·s-1
Umf incipient fluidization velocity, m·s-1
UR superficial gas velocity in riser, m·s-1
X conversion of SiHCl3, %
Y yield of silicon, %
γDR gas bypassing fraction from the downcomer to the riser
γRD gas bypassing fraction from the riser to the downcomer
μ viscosity, Pa·s
ρ density of gas, kg·m-3
ρp density of particles, kg·m-3
REFERENCES
1. Hesse, K.; Schindbeck, E.; Freiheit, H. C. Challenges of solar silicon production.

The 9th Silicon for the Chemical and Solar Industry, Norway, 2008.
2. Sarti, D.; Einhaus, R. Silicon feedstock for the multi-crystalline photovoltaic
industry. Sol. Energ. Mat. Sol. C 2002, 72, 27.
3. Woditsch, P.; Koch, W. Solar grade silicon feedstock supply for PV industry. Sol.
Energ. Mat. Sol. C 2002, 72, 11.
4. Odden, J. O.; Halvorsen, G.; Rong, H. M.; Gløckner, R. Comparison of energy
consumption in different production processes for solar grade silicon. The 9th
Silicon for the Chemical and Solar Industry, Norway, 2008.
5. Braga, A. F. B.; Moreira, S. P.; Zampoeri, P. R.; Bacchin, J. M. G.; Mei, P. R.
New processes for the production of solar-grade polycrystalline silicon: a review.
Sol. Energ. Mat. Sol. C 2008, 92, 418.
6. Weidhaus, D.; Schindlbeck, E. Trichlorosilane based silicon feedstock for the
photovoltaic industry. The 7th Silicon for the Chemical and Solar Industry,
Norway, 2004.
7. Müller, A.; Ghosh, M.; Sonnenschein, R.; Woditsch, P. Silicon for photovoltaic
applications. Mat. Sci. Eng. B 2006, 134, 257.
8. Jiang, W. J.; Dai, Y. Y.; Gu, H. J. Principles of Chemical Engineering. Tsinghua
University Press. 2003, 203.
9. Wang, C. J.; Wang, T. F.; Wang, Z. W. Manufacture of granular polysilicon from
trichlorosilane in a fluidized bed reactor. Ind. Eng. Chem. Res. 2010, submitted.
10. Hitoshi, H.; Takatoshi, N.; Masanori, M.; Masatake, K.; Manabu, S.; Kikuo, O.
Model on transport phenomena and epitaxial growth of silicon thin film in
SiHCI3-H2 system under atmospheric pressure. J. Cryst. Growth 1996, 169, 61.
11. Hitoshi, H.; Yasuaki, A.; Shoji, A.; Toru, O.; Qu, W. F.; Manabu, S.; Kikuo, O.
Chemical process of silicon epitaxial growth in a SiHCl3-H2 system. J. Cryst.
Growth 1999, 207, 77.
8

SIMULATION OF PARTICLE-GAS FLOW
IN CYCLONE USING URANS
Aku Karvinen and Hannu Ahlstedt
Tampere University of Technology
PO Box 589, FI-33101 Tampere, Finland
Marko Palonen
Metso Power Oy
PO Box 109, FI-33101 Tampere, Finland
ABSTRACT
Particle-gas flow in a cyclone separator used in a circulating fluidized-bed boiler is

simulated using computational fluid dynamics software Fluent 6.2.36 and an Unsteady
Reynolds-Averaged Navier-Stokes (URANS) method. A Lagrangian method is used
for particle simulation and a one-way coupling between particles and gas is assumed.
The effect of the turbulence model is studied using several turbulence models. Only
the Reynolds stress model gives a physically reasonable flow field without adjusting
parameters unknown beforehand.
INTRODUCTION
Cyclone separators (Fig. 1) occur in many industries, z

e.g. in oil and gas industry, power generation, incin- outlet
eration plants, cement plants, coking plants and the
food industry. Compared to the other methods for
particle removal from gases the main advantages of inlet
cyclone separators are: low capital investment and
maintenance costs, applicability under extreme pro- y x
cessing conditions, no moving parts, and robustness.
According to (1), the first studies of the cyclone flow

were undertaken in 1930-1950 (2) and (3). The first
CFD (computational fluid dynamics) simulations were
undertaken in the 80’s (4). In the 21st century, CFD Figure 1: Cyclone separator.
simulations have been made for example by Derksen Domain and coordinate sys-
(5) and by Wang (6). A more extensive review can be tem used in this study.
found in (7) and (1).
CASE STUDIED
The schematic of the case studied and the coordinate system used is given in Fig. 1.
The flow gas is hot air. The cyclone body Reynolds number based on an average inlet
velocity and the cyclone diameter (7) is Re = 634,000.
METHODS AND MODELS
The Reynolds-averaged Navier-Stokes equations (RANS) for incompressible flow are

∂ui
= 0, (1)
∂xi
∂ui ∂u 1 ∂p ∂ 2 ui ∂ ′ ′
+ uj i = − +ν + −ui uj , (2)
∂t ∂xj ρ ∂xi ∂xj ∂xj ∂xj
where the overbar denotes time averaging, and the prime denotes the fluctuating com-
ponent. In the k-ε models and the k-ω models, the Boussinesq hypothesis is used in
which the Reynolds stresses, −ui′ uj′ , are calculated from

′ ′ 2 1 ∂ui ∂uj
−ui uj = 2νt Sij − kδij , Sij = + . (3)
3 2 ∂xj ∂xi
In the standard k-ε model (8), the turbulence kinetic energy and its dissipation rate
are obtained from the modeled transport equations, which are as follows:

∂k ∂k ∂ νt ∂k
+ uj = ν+ + νt S 2 − ε, (4)
∂t ∂xj ∂xj σk ∂xj

∂ε ∂ε ∂ νt ∂ε ε ε2
+ uj = ν+ + C1ε νt S 2 − C2ε , (5)
∂t ∂xj ∂xj σε ∂xj k k
p
where S ≡ 2Sij Sij . The turbulent viscosity is computed from νt = Cµ k 2 /ε. Model
constants used have the following values: Cµ = 0.09, C1ε = 1.44, C2ε = 1.92, σk = 1.0,
and σε = 1.3.
The transport equations for k and ε in the RNG k-ε model (9) are

∂k ∂k ∂ ∂k
+ uj = αk νt + νt S 2 − ε, (6)
∂t ∂xj ∂xj ∂xj

∂ε ∂ε ∂ ∂ε ε ε2 Cµ η 3 (1 − η/η0 ) ε2
+ uj = αε νt + C1ε νt S 2 − C2ε − , (7)
∂t ∂xj ∂xj ∂xj k k 1 + βη 3 k
where η ≡ Sk/ε, η0 = 4.38, β = 0.012, and νt is obtained in a similar way as in
the standard k-ε model. The model constants are: Cµ = 0.0845, C1ε = 1.42, and
C2ε = 1.68.
The RNG k-ε model in Fluent provides an option to account for the effects of the swirl
in the mean flow by modifying the turbulent viscosity appropriately:

k
νt,modified = νt f αs , Ω, , (8)
ε
where Ω is a swirl number evaluated within Fluent and αs is a swirl constant that
assumes different values depending on whether the flow is swirl-dominated or mildly
swirling. The exact function for describing this dependency is not revealed in (10).
The transport equations for k and ε in the realizable k-ε model (11), (10) are

∂k ∂k ∂ νt ∂k
+ uj = ν+ + νt S 2 − ε, (9)

∂ε ∂ε ∂ νt ∂ε ε2
+ uj = ν+ + C1ε Sε − C2ε √ , (10)
∂t ∂xj ∂xj σε ∂xj k + νε
where C1ε is now a variable. The turbulent viscosity is obtained in a similar way as
in the standard k-ε model, but Cµ is no longer constant. The model constants are:
C2ε = 1.9, σk = 1.0, and σε = 1.2.
In the standard k-ω model (12), the turbulence kinetic energy, k, and the specific
dissipation rate, ω, are obtained from the following transport equations:

∂k ∂k ∂ νt ∂k
+ uj = ν+ + νt S 2 − β∞
∗
fβ ∗ kω, (11)

∂ε ∂ω ∂ νt ∂ω ω
+ uj = ν+ + νt S 2 − βi fβ ω 2 , (12)
∂t ∂xj ∂xj σω ∂xj k
and the turbulent viscosity is obtained from νt = k/ω. The model constants are: βi =
∗ = 0.09, σ = 2.0, and σ = 2.0.
0.072, β∞ k ω
The SST k-ω model (13) has a form similar to that of the standard k-ω model. The
transport equations are given as follows

∂k ∂k ∂ νt ∂k
+ uj = ν+ + min(νt S 2 , 10ρβ∞
∗
kω) − β∞∗
kω, (13)

∂ε ∂ω ∂ νt ∂ω
+ uj = ν+ + S 2 − βi ω 2 + Dω , (14)
∂t ∂xj ∂xj σω ∂xj
where βi = F1 βi,1 + (1 − F1 )βi,2 and σk and σω are calculated in a similar way. The
turbulent viscosity νt = (k/ω)/ max[1, SF2 /(a1 ω)]. The model constants are: a1 = 0.31,
β∞∗ = 0.09, β
i,1 = 0.075, βi,2 = 0.0828, σk ,1 = 1.176, σω,1 = 2.0, σk ,2 = 1.0, and
σω,2 = 1.168.
In the Reynolds stress model (RSM), there are the exact transport equations for the
transport of Reynolds stresses, −ui′ uj′ (14):
∂ ∂
∂ui′ uj′ ∂ ′ ′
∂ ′ ′ ′ p′ ′ ′ ′ ′
+ uk ui uj = − uuu + δkj ui + δik uj + ν ui uj
∂t ∂xk ∂xk i j k ρ ∂xk ∂xk
| {z }
Dijt
!
∂uj ∂ui p′ ∂ui′ ∂uj′ ∂ui′ ∂uj′
− ui′ uk′ + uj′ uk′ + + − 2ν , (15)
∂xk ∂xk ρ ∂xj ∂xi ∂xk ∂xk
| {z } | {z }
ε ij
φij
where Dijt , φij , and εij are modeled, see (10) for more details. The model constants
are: C1 = 1.8, C2 = 0.60, C1ε = 1.44, C2ε = 1.92, Cµ = 0.9, σk = 1.0, and σε = 1.3.
Calculation Procedure and Computational Grid
All the calculations are performed using commercial software Fluent 6.3.26 (10). All
terms in all equations are discretized in space using second-order central differencing,
apart from the convection term, which is discretized using a second-order upwind
scheme. Pressure-velocity coupling is achieved using the PISO algorithm.
Time integration is done using a first order implicit method and adaptive time stepping
where the first time step is very small (∆t0 = 10−6 s) and next time steps are chosen as
follows: If the solution has not converged after seven iterations, then ∆tnew = 0.9∆told ,
otherwise, ∆tnew = 1.1∆told .
The simulation is initiated using a steady state solver. After several thousand itera-
tions, the simulation is continued by running an unsteady solver and run until the flow
becomes statistically steady (30 s). After that, simulation is continued until statistically
stable data is gathered (30 s → 60 s).
The computational grid consists exclusively of hexahedral cells (Fig. 2). Four different
grid resolutions have been used such that the total number of control volumes used
is 72,978, 260,808, 785,819 or 1,802,564. All grids are constructed so that the grid is
finer for the wall-adjacent cells of all no-slip walls of the cyclone.
(a) In inlet and (b) In middle of cyclone barrel in

cyclone walls. positive quadrant.
Figure 2: Grid 785,819.
GRID INDEPENDENCY TEST
The grid independency test shows that velocity profiles of the RSM in the middle of the
cyclone barrel do not change significantly when the grid is made finer than 785,819
cells (Fig. 3). A grid of 785,819 cells is therefore used exclusively in the turbulence
model comparison. A dimensionless wall unit y + in a cyclone barrel is in an acceptable
range (within the log-law layer) when a 785,819 grid is used (Fig. 3(d)).
2.0 8
Grid 72,978 Grid 72,978
Grid 260,808 Grid 260,808
Grid 785,819 Grid 785,819
6
1.5 Grid 1,802,564 Grid 1,802,564
4
u/velinlet
v /velinlet
1.0
2
0.5
0
0 −2
0 0.2 0.4 0.6 0.8 1.0 0 0.2 0.4 0.6 0.8 1.0
y /R y /R
(a) Radial mean velocity in middle of cyclone (b) Tangential mean velocity in middle of
barrel. cyclone barrel.
Grid 72,978
3 Grid 260,808
Grid 785,819
Grid 1,802,564
2.5 75 75
2
w /velinlet
2.0 100
100 75
75 inlet
1 125
1.5
z/R
100
1.0
0 150
0.5
0.0 125 5
−1
0 0.2 0.4 0.6 0.8 1.0 −5 −4 −3 12 −2 −1 0 1
y /R t/R
(c) Axial mean velocity in middle of cyclone (d) Dimensionless wall unit y + in cyclone barrel looked
barrel. inside out. Grid 785,819.
Figure 3: Grid independency test.
TURBULENCE MODEL COMPARISON
Several papers, e.g. (7) and (1), show that there is rigid body rotation in the core of the
cyclone and almost friction free flow in the outer part of the cyclone. Tangential velocity
profiles complying with these assumptions are shown in Fig. 4(b) by the dashed lines
(constants are adjusted according to the results of the RSM).
Because of the highly anisotropic turbulence caused by the high curvature of the
streamlines and the high swirl intensity, two equation models cannot predict the flow
field correctly – they predict almost rigid body rotation in the whole flow field. Only the
RSM gives a physically reasonable flow field.
The RNG k-ε model with swirl modification implemented in Fluent gives usable results,
but the modification contains an adjustable parameter which was unknown before the
simulations. The default value of the parameter is αs = 0.07, which turns out to be too
small, as can be seen in Fig. 4(b). This makes the modification difficult to use.
2.5 10
Std. k -ε
RNG k -ε (αs = 0) 8
2.0 RNG k -ε (αs = 0.07)
RNG k -ε (αs = 0.35) 6
Real. k -ε
1.5 Std. k -ω
4 Std. k -ε
u/velinlet
v /velinlet
SST k -ω
RSM RNG k -ε (αs = 0)
1.0 2 RNG k -ε (αs = 0.07)
RNG k -ε (αs = 0.35)
0 Real. k -ε
0.5
Std. k -ω
−2 SST k -ω
0 RSM
−4 v = C1 y + D1
v = C2 /y + D2
−0.5 −6
0 0.2 0.4 0.6 0.8 1.0 0 0.2 0.4 0.6 0.8 1.0
y /R y /R
(a) Radial mean velocity. (b) Tangential mean velocity.

7
Std. k -ε
6 RNG k -ε (αs = 0)
RNG k -ε (αs = 0.07)
5 RNG k -ε (αs = 0.35)
Real. k -ε
4 Std. k -ω
w /velinlet
SST k -ω
3 RSM
2
−1
−2
0 0.2 0.4 0.6 0.8 1.0
y /R
(c) Axial mean velocity.
Figure 4: Turbulence model comparison.
PARTICLE TRAJECTORY SIMULATION
Because the only turbulence model that gives a reasonable flow field without any ad-
justable parameter is the RSM, particle trajectory simulation is only done using that
model. Particles of different size are released from the bed and the particle trajectories
are calculated assuming one-way coupling (particles do not affect the flow field). The
mean flow field is used and no turbulence effects on particles are taken into account.
The collision chart in the cyclone barrel is shown in the Fig. 5(a). The collision area of
the largest particle corresponds well with the largest measured erosion (Fig. 5(b)).
2.5 2.5
2.0 2.0
inlet inlet
1.5 1.5
z/R
z/R
d < 50 µm
1.0 d = 50 ... 100 µm 1.0
d = 100 ... 150 µm
0.5 d = 150 ... 200 µm 0.5
d > 200 µm
0.0 0.0
−5 −4 −3 −2 −1 0 1 −5 −4 −3 −2 −1 0 1
t/R t/R
(a) Simulated collision chart. RSM. (b) Measured erosion in target zone. Darkest gray
denotes largest erosion.
Figure 5: Simulated collision chart and measured erosion.

CONCLUSIONS
An extensive grid independency test is achieved using the Reynolds stress model
(RSM). The number of the cells in grids varies between 72,978 and 1,802,564. The
grid independency test shows that a grid consisting of about 800,000 cells gives ac-
ceptable results.
An effect of the turbulence model is studied using six different turbulence models. Be-
cause of the highly anisotropic turbulence caused by the high curvature of the stream-
lines and the high swirl intensity, two equation models cannot predict the flow field
correctly. Only the RSM gives a physically reasonable flow field. Also the RNG k-ε
model with a swirl modification implemented in Fluent gives usable results, but the
modification contains an adjustable parameter which was unknown before the simu-
lations. When the RSM is used, the collision area of the largest particle corresponds
well with the largest measured erosion.
ACKNOWLEDGMENT
The authors gratefully acknowledge the support from Metso Power Oy and from The
Finnish Graduate School in Computational Fluid Dynamics.
NOTATION
Cµ , C1 , C2 , C1ε , C2ε model constant in turbulence models

Dijt turbulent diffusive transport tensor in RSM
Dω cross-diffusion term in RNG k-ε model
F1 , F2 blending functions in SST k-ω model
Pij stress production tensor in RSM
R radius of cyclone barrel
Re cyclone body Reynolds number
S mean rate-of-strain tensor
d particle diameter
fβ ∗ , fβ auxiliary functions in standard k-ω model
k turbulent kinetic energy
p mean pressure
t time, tangential coordinate
∆t0 , ∆told , ∆tnew first, old and new time steps
u, v , w mean velocity components
velinlet average mean velocity in beginning of inlet
y+ dimensionless wall unit
Ω mean rate-of-rotation, characteristic swirl number
αk , αε inverse effective Prandtl numbers
αs swirl constant in RNG k-ε model
βi , β∞ ∗ ,β ,β model constants in turbulence models
i,1 i,2
δ Kronecker delta
ε dissipation rate of turbulent kinetic energy
εij dissipation tensor in RSM
ν, νt molecular and turbulent kinematic viscosity
νt,modified modified turbulent kinematic viscosity
φij pressure-strain tensor in RSM
ρ density
σk , σε , σω , σk ,1 , σk ,2 , σω,1 , σω,2 model constants in turbulence models
σk , σω auxiliary functions in SST k-ω model
REFERENCES
1. C. Cortés and A. Gil. Modeling the gas and particle flow inside cyclone separa-
tors. Progress in Energy and Combustion Science, 33(5):409–452, 2007.
2. R. M. C. K. Alexander. Fundamentals of cyclone design and operation. Proceed-
ings of the Australasian Institute of Mining and Metallurgy, 152:208–228, 1949.
3. A. J. Linden. Investigation into cyclone dust collectors. Proceedings of the Insti-
tution of Mechanical Engineers, 160:233–251, 1949.
4. F. Boysan, W. H. Ayers, and J. Swithenbank. A fundamental mathematical mod-
elling approach to cyclone design. Transactions of the American Institute of
Chemical Engineers, 60:222–230, 1982.
5. J. J. Derksen, S. Sundaresan, and H. E. A. van den Akker. Simulation of mass-
loading effects in gas-solid cyclone separators. Powder Technology, 163:59–68,
2006.
6. B. Wang, D. L. Xu, K. W. Chu, and A. B. Yu. Numerical study of gas-solid flow in
a cyclone separator. Applied Mathematical Modelling, 30:1326–1342, 2006.
7. A. C. Hoffmann and L. E. Stein. Gas Cyclones and Swirl Tubes: Principles,
Design and Operation. Springer, Berlin, 2002.
8. B. E. Launder and D. B. Spalding. Lectures in Mathematical Models of Turbu-
lence. Academic Press, London, 1972.
9. V. Yakhot and S. A. Orszag. Renormalization group analysis of turbulence. Phys-
ical Review Letters, 57:1722–1724, 1986.
10. Fluent Inc. FLUENT 6.3 User’s Guide. Lebanon, 2006.
11. T.-H. Shih, W. W. Liou, A Shabbir, Z. Yang, and J. Zhu. A new k-ε eddy viscosity
model for high Reynolds number turbulent flows. Computers and Fluids, 24:227–
238, 1995.
12. D. C. Wilcox. Turbulence Modeling for CFD. DCW Industries, Inc., La Canada,
California, second edition, 1998.
13. F. R. Menter. Two-equation eddy-viscosity turbulence models for engineering
applications. AIAA Journal, 32:1598–1605, 1994.
14. M. M. Gibson and B. E. Launder. Ground effects on pressure fluctuations in the
atmospheric boundary layer. Journal of Fluid Mechanics, 86:491–511, 1978.
A STUDY OF STANDPIPE AND LOOP SEAL BEHAVIOR
IN A CIRCULATING FLUIDIZED BED FOR GELDART B
PARTICLES
Ajay R. Bidwe, Alexander Charitos, Heiko Dieter, An Wei, Mariusz Zieba,
Günter Scheffknecht
Institute of Combustion and Power Plant Technology (IFK), University of Stuttgart,
Pfaffenwaldring 23, 70569, Stuttgart, Germany.
Email: bidwe@ifk.uni-stuttgart.de
ABSTRACT
The loop seal aeration effect on the supply side has been studied through small
scale CFB experimentation. Parameters affected include inventory allocation and
entrainment. The gas velocity in the standpipe is influenced by loop seal aeration
and riser velocity. Variation in slugging behavior above and below solid downflow
velocity of 0.025 m/s is analyzed and discussed here.
INTRODUCTION
Circulating fluidized bed (CFB) technology is used in

various applications including combustion of solid
fuels for electricity production (1). Recently, it has
been applied in the field of solid looping cycles
aiming at CO2 capture, such as calcium looping (2),
and chemical looping combustion (3). For
combustors standalone CFB’s are used, while for
solid looping cycles dual fluidized bed (DFB) systems
are utilized. In both cases the standpipe-loop seal
arrangement is an important component. A typical
standalone CFB consists of a riser, cyclone and
standpipe-loop seal arrangement, shown in Fig. 1.
The loop seal acts as a solid pumping device from
the low pressure cyclone to the high pressure riser
and ensures that riser gas does not take the short cut Figure 1- Stand alone CFB
through the cyclone. In comparison, DFB systems
consist commonly of two CFBs or a CFB and a BFB, depending on the facility
purpose (2). In this case the role of a loop seal is to transfer solids from the low
pressure cyclone of one reactor to a high or low pressure point of the other reactor,
while disallowing gases from one reactor to enter the other. In both cases,
standpipe-loop seal operation is indispensible. Solid downflow, within the standpipe
and loop seal occurs in three modes as explained by Knowlton (4). Moving bed
mode, bubbling fluidized mode are possible below the level of the particle bed, Lst.
Above this level solid flow occurs in dilute mode. A bubbling or moving bed

standpipe is common
c in CFB appliccations
andd is consideered to be sttable. Howe ever, in
sma all scale faacilities, slu
ugging mayy occur
as a result of small scale sta andpipe
diameter and is threatening to operrational
stability. The lo
oop seal itself consistss of two
secctions, the supply sections annd the
recycle section, as show wn in Fig. 2. The
suppply section n is fed with a particle flow
m the riser cyclone. This flow pro
from oceeds
thro
ough the slits and the e recycle section
s
bacck to the riiser or, in the case of o DFB
sysstems, to thee other reacctor.
Forr above me entioned DF FB processses the Figure 2- Sta andpipe and d loop seal
loop seal is ann important part but gasses used in loop seal aeration
a couuld be a souurce
of dilution
d for product
p gasses. Thereffore optimiz zing the loop p seal desig gn is imporrtant
for these proccesses. Con nsiderationss for standppipe, loop seal design and operattion,
to which
w this paper
p aimss to contribu ute to, are summarize ed below: (i) the loop seal
s
aerration effectt on solid in
nventory, risser entrainm
ment (ii) thee split of this aeration flow
f
between the loop seal supply and d recycle chamber
c (iii) hydrodyynamic stab bility
thro
ough avoid dance of slugging ope eration in the
t standpipe. In norrmal loop seal s
opeeration both h sections ofo the loopp seal are fluidized.
f However to investigate the
aerration split systematica
s ally it was decided
d to aerate
a onlyy in the supply section. By
doing this the effect of loop seal aeration only in the su upply sectio on can alsoo be
inve
estigated.
TES
ST FACILIT
TY AND EX
XPERIMENT
TAL PROCE
EDURE
Thee test facilityy consists ofo a CFB syystem, as Table 1 :D Dimensions of CFB
shoown in Fig g. 1 and iss constructted from Riser
tran
nsparent plexi-glass. The dimen nsions of Riser diam meter [[mm] 70
the CFB are shown
s able 1. The aeration
in Ta Riser heig ght [[m] 4
nozzzles, locate ed only in th he supply section
s of Standpipe e H / Dia [[m] 1/0
0.03
the loop seal are insertted sidewayys at an Loop sea al
anggle of 45°, too prevent particles
p cloggging the Height [[mm] 2000
gass nozzles. TheT fluidiza
ation gas iss air and Supply Le ength [[mm] 35
parrticles are Illmenite min neral particle
es with a Recycle Length
L [[mm] 50
parrticle size diistribution of
o 100-200 µmµ and a Width [[mm] 35
mean particle size of 14 43 µm. The e particle Weir height [[mm] 1500
dennsity ( ) iss 4400 kg/m m³ and the e Geldart
Slit opening [[mm] 30
classsification of
o particles is class B (5). The
is calculatted, as shown in (1), to o be equal 0.029 m/s. Pressure transducers are
mounted at va arious locations of the CFB system. Rotame eters are ussed to meassure
the air supply to the riserr and loop seal.
s The faacility is fille
ed with a knnown total solid
s
inve
entory (TSI). The parameters varied are the loop l seal ae eration ( ) in wide raange
of 0.003 to 0.2 28 m/s and d riser velo
ocity 3 to 5 m/s. The entrainmen nt is measu ured
thro
ough stoppiing loop seal aeration and measu uring the acccumulation n of the particle
bedd height with h the standpipe for a given period of time.

Loop seal aeration flow path determination
The data evaluation procedure is based on Basu & Cheng (7) and has been applied
for every steady state. Goal of the analysis, presented in steps, is to define the gas
flow path through the loop seal.
(i) Calculation of the standpipe slip velocity
The slip velocity ( ), expresses the relative velocity between gas and solid within
Δ 150 1 1.75 1
∆ | | | | (1)
the standpipe and is calculated through Eq.1. The pressure drop through the
standpipe ( and the particle bed height ( ) have been measured for every
Δ
steady state, thus defining also the pressure gradient .The ∆ is measured
from the bottom of the loop seal to the bottom of the cyclone. Althought the areas of
Δ
standpipe and loop seal vary, but for simplification the is assumed to be
constant and further calculations of gas and solid velocity are based on the area of
standpipe. The voidage (ε) value, for packed bed column found to be equal to 0.48
and at minimum fluidizing conditions (εmf) is found to be 0.54. However the exact
voidage while standpipe operation is difficult to estimate. Therefore an average
voidage of 0.51 is considered for calculation. Eq.1 has been applied only when the
fluidization regime in the standpipe was moving bed. The situations in which this
standpipe showed bubbling or slugging mode of fluidization are not considered in
the calculations. The sphericity of the particles ( ) has been taken as 0.75 from
voidage-sphericity graphs in (6).
(ii) Calculation of the real solid downflow and gas velocity

The real solid downflow velocity ( ) and gas velocity ( ) is calculated through Eq.
(2) and Eq. (3). The and are positive in the downwards direction. The is
defined through measurement of the riser entrainment, based on the standpipe
cross-section ( ). The real standpipe gas velocity ( ) is subsequently calculated
through Eq. 3, which is the definition of the slip velocity. The superficial gas velocity
( ) in the standpipe is calculated from the voidage.
(2) (3)
1
(iii) Calculation of loop seal aeration split

The flow travelling through the particle column in the standpipe ( ) is given by
Eq.4. If ( ) is positive than the loop seal aeration flow is split between the loop seal
supply chamber-standpipe and the recycle chamber-riser. This split is quantified with
the ratio of Eq.5 and is defined as the fraction of total volumetric flow of the loop seal
aeration ( ) entering supply side ( ) or the recycle side ( ) of the loop seal. The
aeration split in the supply section is calculated using Eq.5 and the recycle side
given by Eq.6. If the is negative, the gas flow from the cyclone is carried

wnwards wiith the particles. This carried
dow c gas from the particles entters the recycle
cha
amber ( ) in
i addition to
t the loop seal
s aeratio
on ( ).
A = A (4) (5
5)
1 (6
6)
Pre
essure bala
ance
The
e pressure balance
b for the system
m of Fig.1 is given by Eq
q.7 (7) (9).
∆ ∆ ∆ ∆ (7
7)
The
e pressure drop
d terms of Eq.7 are
e depicted in
n Fig.1.
RESULTS AND DISCUSS

SION
Thee effect of th
he loop sea
al aeration in y section is examined, with respec
n the supply ct to
the parameterss below.
Ris
ser pressurre drop
Fig.3 shows thhe effect off the loop

sea
al aeration on
o the riserr pressure
dro
op. The lo oop seal becomes
functional whe
en > 2. Itts velocity
( ) is calculated based on the
tota
al area of o the lo oop seal
inclluding supply and recycle
chaamber given in Table 1.
Increasing lo oop seal aeration
deccreases thee standpipe e particle
bedd height ( ) and incrreases its
pre
essure dro op ( ). This is
expplainable du
ue to the increase of
Δ
, as expected
e fro
om Eq.1.
Forr constantt riser superficial
s Figure 3-- Effect off loop sea al aeration on
velo ncrease of loop seal standpipe height, pressure
ocity, the in p drop and riser
r
aerration causses an inccrease in pressure drop d
rise
er pressure drop ( ). This
is a result of mass
m transffer from thee standpipe, noticed ass a decreasse of standppipe
heigght ( ), to the riser. A similar observation is reportted by Cha aritos et al (2).
How wever, mosst of the rise
er inventoryy is located in the botto
om part the
erefore slope of
incrrease of is bigger than that
t of the standpipe pressure drop ( ), this
follo
ows the preessure balan nce as per Eq.7.
Ris
ser entrain
nment The riser entra ed against the loop seal
ainment ( ) is plotte s
aerration ratio in Fiig.4. For bo
oth riser ve
elocities rea
alized during
g experime
ents,
incrreasing loo
op seal aeration resultts in an inc
crease of until a maximum
m is

ached (5)((7)(8). Thiss can be
rea
expplained since increassing loop
seaal aeration n results in an
incrrease of as shown in
Fig. 3. For a riser velocity ( ) of
3.6 m/s the maximumm is equal
to 23.5 kg/m2s at a lo oop seal
aerration ratio of 3.6
6. For the
higher of 4.3
4 m/s the maximum
m
is equual to 288.7 kg/m2s
occcurring at of 6.6
6. Further
aerration reducces the slightly. A
nummber of works, e.g. (7) and (9),
do not predicct a reduction of
with
h loop seall aeration. However,
Leee et al. (10) has reported such Figure 4- Effect of loo op seal aera ation on rise
er
behhavior in a seal
s pot for Geldart A entrainmeent at two
o velocities. TSI -2.9 kgg.
parrticles. In this work the decrease
of beyond its maximum m coincidess and may be b attributedd to the apppearance off the
sluggging in the e standpipee. Finally, foor a given value, in
ncreasing riser velocity y
results in a hig
gher valu
ue, as reporrted in many
y works, e.g
g. (2).
Gas
s velocity through
t the standpip
pe
Fig.5 and Fig

g.6 depict the effect of the loo
op seal aeration ratio
o ( ) on the
perficial gass velocity in
sup i the stan ndpipe ( ) and the aeration
a sp
plit respectively
deffined in Eq.5, at riser velocity
v of 3.6 and 4.3 3 m/s. The superficial gas velocitty is
calcculated as a product ofo the real gas velocitty ( ) and the voidag ge (ε) showwn in
Eq..4. The voiddage considdered for ca alculation is 0.51. As se
een in Fig.5
5 an increas
se of
results in an increasee of for the
t riser ve elocity ( ) of
o 3.6 m/s almost linea arly.
Forr higher rise
er velocity of
o 4.3 m/s and loop sea
al aeration ratios
r <5
5.6, is in
n the
range of -0.02
2 m/s. The gas flow in
n the standp
pipe is movving downw
wards, when n
and
d the aeration split values
v are negative. For the loower off 3.6 m/s, this
phe
enomenon isi encounteered for a smaller range,
r nam
mely when < 2.6. For a
give
en value, the iss higher at a of 3.6 m/s
m in comp
parison to a of 4.3 m/s.
m
Theese observa ations can be explained based on o the high her valuees, resulting in
higher values (see Eq q.3), occurring at a of 4.3 m/s in comparisson to a 3.6
m/ss, as shownn in Fig. 4. This
T is base
ed on that higher
h . Higher
H va
alues result in a
higher resistannce for gass up flow in the standppipe. Howevver, when the ratiio is
incrreased enoough, then the t and
d aeration split
s become positive, thus indicaating
that the gas flo
ow in the sttandpipe is upwards. Itt can be observed thatt the downw ward
have a limittation, i.e. -0
0.03 m/s. Basu
B and Buutler(8) have
e the similar conclusion
n.

The aeration split increases with
increase in and is calculated from -
8% to +6%. Up to 6% of the aeration
gas is entering the standpipe. This
concludes that remaining 94-100% of
the aeration gas is entering the recycle
chamber. In case of negative
additional gas is entering the recycle
side of the loop seal. If the calculated
aeration in the recycle side is in the
range of 2-6 and enough to keep
the recycle side of the loop seal
fluidized. Therefore the loop seal
Figure 5 – Effect of loop seal aeration on worked well even without the aeration in
gas velocity in standpipe ( ) at different the recycle chamber.
riser velocities (TSI =2.9 kg)
The deviation bars in Fig.5 and Fig.6
show the influence of voidage in the
calculations of and aeration split. The
lower deviation shows the value at a
voidage of 0.48 and the upper deviation
shows the value of voidage 0.54 close
to . As observed the voidage can
affect the results significantly. As
discussed earlier, the assumption of a
Δ
constant , despite the two different
standpipe cross-sections, holds true to a
limited extent. Therefore, to find out the
exact gas flow pattern would implicate
the use of tracer gases. Johansson et al
Figure 6 – Effect of loop seal aeration on (3) reported aeration split values of 2 to
the aeration split 7 % using tracer gases. In that work, for
a separate downcomer of the same
facility values of -0.05 m/s to + 0.1 m/s were recorded. Hence the results
reported in this section are comparable with the data of (3).
Slugging in the standpipe
Fig.5 and Fig.6 show that the increasing loop seal aeration increases the gas
velocity in the standpipe. At low or negative gas velocities the standpipe was in
moving bed mode. With increasing aeration in the loop seal a stage is reached when
bubbles start to appear in the standpipe. The bubbles could be equivalent to a
standpipe diameter in such small standpipe used in this study. This situation is
commonly referred as slugging, common phenomenon for such small scale units.
Two types of slugging have been described by Wen (5). Type A- Round nose
slugging and Type B - Flat nose slugging. The Type A is similar to normal bubbling
bed where bubbles rise up in fluidized bed. The difference compared to bubbling
bed is that a gas slug is nearly equal to the standpipe diameter. Typical Type B

sluggging is shhown in Figg.7 where gas slug completely
c
occcupies the cross
c sectio
on and lift th
he solid chu
unk above
it. The
T solid do ownward motion is only possible by raining
dow wn as solid streamers or when the e chunk getts broken.
The e Type B slugging occurs ma ainly with cohesive
parrticles and is not a suittable modee for the sta
andpipe to
ope erate becauuse sometimmes the chu unks may be e lifted up
to the cyclone and cau use frequen nt operationnal break
dow wns.
Succh Type B slugging occcurred durring the experiments

at riser velocities of 3.6 and 4.3 m/s m and ha as caused
reduction in thhe entrainm ment rate (see Fig.4). Typically
Typ
pe B sluggin ng occurred d at > 0..03 m/s whiile Type A
or bubbling occurred
o at < 0.02
25. Sometim mes both
type
es occurre ed simultaneously, i.e. Type B in the
standpipe and Type A in the t loop seal supply side where
cross section is
i larger thaan standpipe e. This clea
arly shows
the influence of solid velocity on th he Type of slugging.
This fact can be explain ned as folloows: Increa asing loop
seaal aeration increases
i th
he gas veloocity in the standpipe
andd at lower solid
s velocitty ( <0.0225 m/s), thee particles Figure 7- Slugging g in
standpipee
bedd is expand dable and allows
a smoo oth bubble travel. At
higher solid veelocities ( >0.03 m/s) the particle es tend to flow
f closely packed, att the
samme time inccreasing ga as velocity in the stan ndpipe tries to expand d the bed. This
T
couunter acting
g behavior of o gas and solid leads s to the Typ pe B slugging depicted in
Fig.7. Since Tyype B is common to co ohesive parrticles, thuss at higher d
down flow solid
s
velo
ocity the pa
articles exhibit cohesivee nature.
In certain
c appplications likke calcium looping (2), the prefe erred fluidizzation mode e in
standpipe is bubbling to prevent
p the calcium pa
articles from
m sticking toogether (1). For
larg
ge scale faccilities such
h slugging may
m not be relevent. However
H in small facilitties,
for certain coonditions Tyype A slug gging is unnavoidable. The abovve results give g
sugggestions how to prevvent the sta andpipe from operating in the Tyype B slugg ging
mode. To avoid d Type B slugging it is suggested that in the standpippe is kept lo
ower
than 0.025 m/ss. Which ca an be achieeved either by reducing the riser entrainmen nt or
by increasing the
t standpip pe area .
CO
ONCLUSION
NS
Thee standpipe e-loop seal behavior in small scale e CFB is sttudied throuugh variation of
the loop seal aeration
a of the
t supply chamber
c us
sing Ilmenitte particles. The standppipe
gass velocity and aerationn split in the
e standpipee increases with increa asing loop seal
s
aerration. Increeasing the downflow solid veloc city decreasses the ga as velocity and
f a given loop seal aeration.
aerration split for a Ann incrementt in the loop p seal aera
ation
incrreases the riser u to a limit and then
up n decreases due to sslugging in the
standpipe. The e standpipe
e slugged ea asily due to
o its small diameter.
d Hoowever at solid
s
velo
ocities up to 0.025 m/sm Round nose slugg ging occurrred while a at higher solid
s
velo
ocity i.e. ab
bove 0.03 m/s
m Flat nose e slugging occurred.
o F a stable CFB opera
For ation
Flat nose slugg ging should
d be avoided d.

ACKNOWLEDGEMENTS
This work is part of the ongoing CAL-MOD Project which is funded in part by the
RFCS Research Program of the European Commission (RFCR-CT-2010-00013).
NOTATIONS
m² Standpipe area m/s Real gas velocity in the

standpipe
m Particle diameter m/s Gas velocity in loop seal
kg/m2s riser circulation rate m/s Slip velocity
Δpi mbar, Pa Pressure drop in a m/s Real solid velocity in the
given CFB section i standpipe
m/s Riser superficial m/s Minimum fluidization velocity
velocity
m/s Superficial gas velocity m³/s, Volumetric flow rate
in standpipe
Greek symbols
ε Voidage ρg kg/m³ Gas density
µ Pa.s Gas viscosity ρs kg/m³ Particle density
Sphericity
Abbreviations
CFB Circulating fluidized bed St Standpipe
DFB Dual fluidized bed TSI Total solid inventory
LS Loop seal
REFERENCES
1. Basu P., (2006)''Combustion and Gasification in fluidized beds''.Taylor & Francis Group.
2. Charitos A. Hawthorne C., Bidwe A.R., Korovesis L., Schuster A. and Scheffknecht G.
(2010), ''Hydrodynamic analysis of a 10 kWth Calcium Looping Dual Fluidized Bed for
post-combustion CO2 capture'', Powder technology, 200(3), 117–127.
3. Johansson E., Lyngfelt A., Mattisson T. and Johnsson F. (2003), ''Gas leakage
measurements in a cold model of an interconnected bed for chemical looping
combustion.'' Powder Technology, 134(3), 210-217.
4. Knowlton T.M. Handbook of fluidization and fluid particle systems, Chapter 21,
Standpipes and Nonmechanical valves. Taylor and Francis group LLC.
5. Wen-Ching Yang. Handbook of fluidization and fluid particle systems, Chapter 3,
Bubbling fluidized beds, Taylor and Francis group LLC
6. Kunni D. and Levenspiel O.,(1991), Fluidization engineering, A Butterworth-Heinemann
7. Basu P. and Cheng L., (2000), ''An analysis of loop seal operations in a circulating
fluidized bed.'', Chemical Engineering Research and Design, 78(7), 991-998.
8. Basu P. and Butler J., (2009),''Studies on the operation of loop seal in ciruculating
fludized bed boilers.'', Applied energy, 86(9),1723-1731.
9. Kim S.W., Namkung W. and Kim S.D. (1999), ''Solid flow characteristics in loop seal of
circulating fludized bed.'', Korean J. of chemical eng., 16(1), 82-88
10. Lee H.S., Lee Y., Park S.S., Chae H.J. Jeon S.Y and Lee D.H. (2010), ''Hydrodynamic
characteristics of cold-bed circulating fluidized beds for methanol to olefins process.'',
Korean J. of chemical eng., 27(4), 1328-1332

EFFECT OF BED TEMPERATURE, FUEL DENSITY AND
PARTICLE SIZE ON HYDRODYNAMIC PARAMETERS OF A 10
MW FLUIDIZED BED COMBUSTION POWER PLANT USING
RICE WASTE
Ravi Inder Singh1 and S.K.Mohapatra2
1
Assistant Professor, Dept. of Mechanical Engineering, Guru Nanak Dev Engineering
College, Ludhiana, Punjab, India
2
Prof and Head, Mechanical Engineering Department, Thapar University, Patiala, Punjab,
India
*
Corresponding Author (Email: ravis021@ yahoo.com )
ABSTRACT
The design and operation of boilers using rice waste present a number of challenges. The
overall capacity and efficiency of the boiler are strongly dependent on the fuel, and the
supplier has to be able to guarantee the capacity and efficiency within the whole range of the
fuel mixture being burned. It is well known that the exit gas composition is strongly dependent
on the fuel. Bed temperature, fuel density and particle size significantly affect the
hydrodynamic properties of a fluidized bed combustor. The effect of bed temperature, fuel
density, particle size on exit gas composition and other hydrodynamic parameters of 10 MW
power plant is discussed in this paper, and a heat balance sheet for the 10 MW fluidized bed
boiler based on rice waste is prepared. Heat release in the fluidized bed region is also
calculated and the efficiency of fluidized bed boiler is found.
1.0 INTRODUCTION
Energy consumption in the world in the form of petroleum-based fuels has increased several
fold during the last 20 years. Fast depleting stocks of fossil fuel and steep increases in their
prices may lead to an energy crisis in the future. With declining reserves and fluctuating
prices of fossil fuels, the search for an alternative renewable raw material to replace
petroleum has intensified. Rice waste is an agro residue which is found in regions where the
demand for energy exists. Rice waste is primarily comprised of rice straw, rice husk and rice
bran. Fluidized bed combustion a technology, which produces energy efficiently with a wide
range of fuels, at low temperature and at isothermal conditions. Due to these reasons a
number of commercial fluidized bed power plants of 10-20 MW capacities based on rice
husk/rice straw have been installed in the last two decades for power generation.
Rice husk and rice straw are the waste materials which are incinerated in a fluidized bed
combustor (FBC) in Punjab (India) and adjoining areas. Due to high collection costs, feeding
problems and agglomeration problems, the rice straw is not incinerated in most commercial
fluidized bed combustors in its present form. Rice husk can be easily bought from commercial
rice mill owners, and is the main fuel used in commercial atmospheric fluidized bed
combustors based on rice husk/rice straw. A three-phase mathematical model for exit gas
composition and solid population balance (2) (4) for shrinking particles in an atmospheric
bubbling fluidized bed combustor using rice-husk was developed in previous studies. The
main aim of this paper is to study the effects of fuel density, bed temperature and particle size
on hydrodynamic features of the plant and to calculate the various heat transfer effedcts in
the 10 MW power plant situated at Jalkheri, Patiala, Punjab, India. Figure 1.1 shows the
schematic diagram of the boiler, and Figure 1.2 shows the layout of the biomass based plant
at Jalkheri for which the study and model were developed.
Ravi Inder singh et al. (1) conducted a study of an atmospheric bubbling fluidized bed
combustor for a 10 MW power plant based on rice husk. In his paper an environmental
assessment, an exit gas composition model, an agglomeration problem and a model for a
solids population balance for the 10 MW power plant at Jalkheri, Punjab, India using rice
husk is discussed. Goo al (2) studied the effects of temperature and particle size on minimum
fluidization and transport velocities in a dual fluidized bed. They found that the minimum
fluidization velocity decreased with temperature due to the increase of gas viscosity. The
transport velocity increased with increasing temperature. They proposed correlations in terms
of Reynolds and Archimedes numbers.
Figure 1.1 Schematic diagram of Boiler Figure 1.2: Schematic diagram of 10 MW

Jalkheri power plant
2.0 MODEL FORMULATION
A mathematical model was developed to calculate the exit gas composition and solids
population balance for a 10 MW FBC power plant suitable for biomass particularly rice husk.
The model was validated by collecting data from the 10 MW commercial FBC plant based on
biomass (1). The model was based on the three-phase theory of fluidization and single film
theory of carbon combustion. It was based on the assumption that essentially the C + O2 =
CO2 reaction is taking place in the combustor. It was assumed that the fluidized bed consists
of a number of stages and the height of each stage was equivalent to the average bubble
diameter. Each stage consisted of the bubble, cloud, and emulsion phases. Bubbles were
solids free and gas in bubbles were in plug flow, bubbles and the cloud-wake rise at the same
velocity. In each stage the emulsion and cloud-wake phases were back mixed. The voidage
in both these phases were the same at incipient condition. The assumption that combustion
does not involve a change in number of moles and that char and volatiles burn at the same
rate throughout the bed was assumed. The main features of these models were physical
chemical processes occurring in a fluidized bed combustor based on rice husk, oxygen mass
balance for exit gas composition and a solid population balance. The details of the models
can be obtained from references (1) and (3). A brief description of model is given below.
Oxygen balance around stage ‘n’ for the bubble phase
Oxygen in by convection-Oxygen out by convection -Oxygen transfer to cloud-wake = 0

It is represented symbolically as;
(2.1)
Zn
U bC b n −1
− U bC b − ( K
n
) εb
bc b ∫ ( C b − C cw ) d Z
n
Z n −1
Oxygen balance around stage ‘n’ for bubble-cloud wake phase
‫׀‬Oxygen in by convection ‫׀ – ׀‬Oxygen coming from bubble phase by transfer ‫ ׀ – ׀‬Oxygen

going out from cloud –wake to emulsion by transfer ‫׀ – ׀‬Oxygen out from cloud-wake by
convection ‫ ׀ – ׀‬Oxygen consumed in cloud-wake phase‫ = ׀‬0
Symbolically, this can be represented as:
Zn
U cw C cw n −1
+ ( K bc ) b ε b ∫ ( C b − C cw ) dZ + K ce C e − (U cw + K cw + K ce ) C cw
n n n
(2.2)
Z n −1
Where
K ce = ( K ce )b ε b ΔZ K cw = ( K )( f cw )(ε b )( ΔZ ) and ΔZ = Z n − Z n −1 = Db (2.3)
,
Oxygen balance around stage ‘n’ for the emulsion phase
‫׀‬Oxygen in by convection‫׀ – ׀‬Oxygen out by convection ‫ ׀‬+ ‫׀‬Oxygen transfer from cloud-
wake phase ‫׀ = ׀‬Oxygen consumed by Combustion reaction ‫׀‬
Symbolically, this can be represented as:
U mf Ce + ( K ce )(Ccw ) − (U mf + K e + K ce )Ce = 0
n −1 n n
(2.4)
Where K e = K [1 − ε b (1 + f cw )]ΔZ and K ce = ( K ce )ε b ΔZ (2.5)
The the oxygen balance over a height (dZ) in the bubble phase is written as:
U b Cb − U b (Cb + dCb ) − ( K bc )b ε b (Cb − Ccwn ) dZ = 0 (2.6)
Rearranging and integrating the above equation, we get
Cb − Ccwn = (Cbn−1 − Ccwn ) exp[{−( K bc )b ε b ( Z − Z n −1 )}/ U b ] (2.7)
At the bottom of the bed (n=0), the concentration of oxygen fed to each phase is the same as
that of the incoming feed oxygen. Hence, the boundary conditions are:
At n=0, Cbn = Ccwn = Cen = C0 (2.8)
Equations 2.1-2.7, together with the boundary conditions in equation 2.8, make up a
complete mathematical description of the system. Details could be referred from (1) and (3).
The average gas composition leaving the nth stage, i.e at the top of the bed is:
Oxygen Cavg = (U b Cb + U cw Ccw + U mf Ce ) / U 0
n n n
(2.12)
Carbon dioxide CO2 = C0 − C avg (2.13)
Nitrogen N 2 = (0.79 / 22, 400)(273 / Tb ) + [ XN (1 − XW )] / 28.U 0 . At (2.14)
3.0 HEAT BALANCE CALCULATIONS IN 10 MW PLANT
The amount of heat entering the bed and various losses have been calculated. Finally
thermal efficiency is calculated and the results shown in Table 4.3 and Figure 4.14.
3.1 Heat added to fluidized bed combustor

Qha= mass of fuel * Calorific value of rice waste (3.1)
3.2 Heat lost to flue gases: The flue gases contain dry products of combustion as well as the
steam generated due to combustion of hydrogen in the fuel.
Qfg = mg * Cpg * (Tg – Ta ) (3.2)
3.3. Heat carried away by the steam from flue gases
Qsg = ms1 (hs1 – hf1) (3.3)
3.4 Heat lost due to incomplete combustion
Heat lost due to incomplete combustion (6) of carbon per kg of fuel
Qic= [CO × C / CO2 + CO] × 23680 KJ/kg of fuel (3.4)
3.5 Heat lost due to unburnt fuel
Qub = mf1× C.V (3.5)
3.6 Convention and Radiation losses
The loss of heat due to convection and radiation losses
Qcr= Heat released per kg of fuel – (Qg + Qs + Qic + Qub) (3.6)
3.7 Equivalent evaporation (me) = ma * (h – hf1) / hfg (3.7)
3.8 Boiler efficiency
ηb = ma * ( h – hf1 ) / C.V (3.8)
3.9 Average Heat transfer Coefficient
The overall bed heat transfer coefficient is given by
hα = Heat Transfer flux / A. ∆t (3.9)
More details could be found in the work of (6).
4.0 RESULTS AND DISCUSSIONS
The input data required for the exit gas model and solid population model (1) was taken from
a 10 MW FBC plant at Jalkheri (Jalkheri Power Pvt. Limited, Fatehgarh Sahib, Punjab, India).
The plant uses the rice husk (80%) and rice straw (20%) as feed stock. The average size of
rice husk particle ranges from 0.25 to 0.625 cm. At one time the size of the rice husk particles
was uniform. Bed temperature ranged from 925 K to 1125 K. The density of fuel varied from
0.09 to 1.2 g/cm3 as fuel consists of rice husk and rice straw. The proximate and ultimate
analyses of rice husk were done at different times and the result of one such sample is given
in Table 4.1. The results of these analysis, along with the other physical-chemical parameters
taken from plant were the input parameters to the model in Section 3.0 and (1). Fuel density,
Table 4.1 Proximate and ultimate analysis of rice waste sample
Proximate analysis Ultimate analysis
(Rice husk) (Rice husk)
Volatile 58.03 C 38.9
Fixed Carbon 16.65 H 5.1
Ash 17.82 S 0.12
Moisture 7.5 O 37.9
N 2.17
Table 4.2 Physico chemical parameters of Plant
Type of fuel used (at Rice husk and rice Area of fluidized bed 391000 cm2
time of study) straw
Feed rate of fuel 3200 g/s Type of distributor Nozzle type tuyre
Feed rate of water 11110 g/s Total no. of holes in 22500
distributor
Air flow rate 20 × 106 cm3/s Specific fuel consumption 1300 g of fuel /unit
generation
Rate of steam 10830 g/s Bed Voidage 0.48
generation
Main steam 400oC Bed height at minimum 48 cm
temperature fluidization
Combustion efficiency 82% (Designed Boiler capacity 50 T/hr equivalent
Value) to 13888.88 kg/s
Figure 4.1 Composition of oxygen and carbon dioxide in flue gas vs. fuel density
Figure 4.2, 4.3 and 4.4 Minimum fluidization velocity, bubble diameter and expanded bed
height vs. fuel density
Figure 4.5, 4.6 and 4.7 Minimum fluidization velocity, bubble diameter and shrinkage rate vs.
Particle size
Figure 4.8 Carbon utilization efficiency Figure 4.9, 4.10 Shrinkage rate and diameter of
Vs. Bed temperature bubble vs. Bed temperature
Figures 4.11 and 4.12 Expanded bed height and the composition of oxygen and carbon
dioxide in the flue gas vs. Bed Temperature
bed temperature and particle size are the important parameters which decide the various
hydrodynamic properties of FBCs. The output of both models resulted in hydrodynamic
parameters, exit gas composition, carbon utilization efficiency etc. of the FBC situated at
Jalkheri. The data given in table 4.2 were used to prepare the heat balance sheet for the
Jalkheri boiler, and to calculate the actual thermal efficiency of the boiler at the time of
operation. The variation of oxygen and carbon dioxide in the flue gas with fuel density is
shown in Figure 4.1. The model values closely match the actual plant data. The value of
carbon dioxide increases and oxygen decreases. It is due to the fact that the combustion of
dense fuel is more proper than less dense fuel. The oxygen supplied to the dense fuel is
more than less dense fuel. The trend of Umf is shown in Figure 4.2. Umf increases with
increasing density and is directly proportional to fuel density.
The trend of bubble diameter with fuel density is shown in Figure 4.3. Bubble diameter
decreased with increasing fuel density because the bubble diameter is dependent on the
difference between superficial velocity and Umf. As Umf increases, it causes the bubble
diameter to decrease. The trend of expanded bed height with fuel density is shown in Figure
4.4 The expanded bed height increases is due to increase of bubble diameter.
The trend of minimum fluidization velocity with particle size is shown in Figure 4.5. It
increases with increasing particle diameter. The bubble diameter and shrinkage rate with
particle diameter are shown in Figure 4.6 4.7. Both decrease with increasing particle diameter
as these are inversely proportional to particle diameter and due to the fact that Umf increases
as particle size increases causing the increase of bubble diameter. Carbon utilization
efficiency increases with increasing particle diameter because large particles stay in the
fluidized bed longer than smaller particles.
Figure 4.13 Variation of percentage of gases in flue gas with moisture
Shrinkage rate, bubble diameter and expanded bed height with bed temperature are shown
in Figures 4.9, 4.10 and 4.11. Bubble diameter is dependent on Umf which is further
dependent on gas viscosity. Gas viscosity decreases with increasing bed temperature. This
causes the minimum fluidization velocity to decrease which further increases the bubble
diameter. Bubble diameter causes the expanded bed height to increase. Bed temperature
causes reaction rates to increase which causes the shrinkage rate to increase.
Table 4.3 Heat balance sheet of Jalkheri Power Plant
Notation Description Calculated Notation Description Calculated

Value Value
Qha Heat added to fluidized 48 MJ Qub Heat lost due to 0.125 MJ
bed un burnt fuel
Qfg Heat lost to flue gases 0.62 MJ Qcr Convention , 13.31 MJ
Radiation and
other losses
Qsg Heat gained by steam 33.93 MJ me Equivalent 4.697 kg/kg
evaporation of fuel
Qic Heat lost due to 0.015 MJ ηb Calculated 70.68 %
incomplete combustion value
The variation of oxygen and carbon dioxide in flue gas with bed temperature is shown in
Figure 4.12. The model values are completely in accordance with plant results as shown in
the figure. Carbon dioxide increases up to 975 K and thereafter decreases. After 975 K the
problem of agglomeration predominates and that causes non-uniform combustion in the
fluidized bed, which causes the carbon dioxide values to decrease and oxygen to increase.
The moisture in rice husk varies throughout the year. The effect of moisture on oxygen
concentration and carbon dioxide emitted from the FBC is shown in Figure 4.13. The
percentage of carbon dioxide increases with increasing moisture content and the percentage
of oxygen decreases with increasing moisture content in the rice husk particles. Fuel with
different moisture contents is checked and model predictions are within satisfying limits. The
actual plant data noted at different moisture percentage of rice husk particles are shown in
Figure 4.13. The variation of actual plant data is in accordance with the model values. It was
described by Ganesh et al. (6) that in order to achieve complete conversion of carbon it is
desirable to maintain a low temperature during pyrolysis and/or partial combustion of rice
husk, followed by steam gasification. The increase in moisture content in fuel causes the
plant bed temperature to decrease. Bed temperature decreases because more heat is
needed to convert moisture from fuel into the vapor form since a phase change takes place.
Therefore, the latent heat required to change the phase is greater which causes bed
temperature to decrease. Due to the lower bed temperature, complete carbon conversion
occurs and causes to increased carbon dioxide concentration as shown in Figure 4.13
Figure 4.14 Heat Balance Chart

The heat balance boiler sheet is described in Table 4.3 and Figure 4.14. This was calculated
with data collected from the plant as shown in Table 4.2 and from steam tables. The
calculations were performed assuming the calorific value of rice waste is 15 MJ/kg. The total
heat input to the fluidized bed boiler is 48 MJ for a mass rate of fuel entering in the combustor
of 3200 g/s. From the total heat entering, 33.93 MJ of heat has been used in raising the
steam. Remaining heat is gone in the losses mentioned in figure 4.14 and table 4.3. Major
portion of heat loss around 13.31 MJ is gone in radiation, convection and other losses. The
other losses are like leakage of steam etc. The actual boiler efficiency calculated at plant is
found to be 70.68 % which is quite lower than the designed value. It is because of various
losses present which need to be controlled. It is also found that some refractory plates which
are used to prevent radiation losses are in damaged condition. Mass of equivalent
evaporation of steam is found to be 4.697 kg/kg of fuel burnt. The average heat transfer
2
coefficient is found to be 1101.7 W/m .K in bed region.
5.0 CONCLUSIONS
The above study conducted with respect to incineration of rice waste in an FBC leads to the
following conclusions.
1. The CO2 percentage in the flue gas increased from 11 to 15.62 and the oxygen
percentage from 10.9 to 6.4 with increases in fuel density from 0.09 to 0.12 g/cm2,
respectively.
2. Umf increased from 21.64 to 28.05 cm/s, bubble diameter decreased from 20.2 to 19.65
cm/s, expanded bed height decreased from 84.7 to 82.9 cm with increases in fuel density
from 0.09 to 0.12 g/cm2, respectively.
3. Umf increased from 9.44 to 43.6 cm/s, bubble diameter decreased from 21.6 to 18.8 cm,
shrinkage rate decreased from 0.0462 to 0.0325 cm/s and carbon utilization efficiency
increased from 96.8 to 98.75 with increases in particle size from 0.25 to 0.6 cm.
4. The shrinkage rate increased from 0.0256 to 0.0383 cm/s, bubble diameter from 19 to
20.83 cm and expanded bed height increased from 80.93 to 86.8 cm with increases in bed
temperature from 925 to 1100 K. The maximum value of carbon dioxide in the flue gas was
12.55 percent and the minimum value of oxygen in the flue gas was 8.3 percent.
5. Increasing the moisture percentage in the fuel from 6.5 to 12.5 decreased the oxygen
percentage from 7.3 to 6.2 in the flue gas and there was an increase in the percentage of
carbon dioxide from 13.4 to 14.8 in the flue gas.
6. The actual boiler efficiency was 70.68% which is quite low, The majority of the heat losses
were from radiation and convection. The average heat transfer coefficient was found to
2
1101.7 W/m .K in the bed region.
ACKNOWLEDGEMENT
The authors are thankful to the management and Er. S.Bandopadhya of Jalkheri Power
Private Limited for providing the information and data required for the study.
NOTATION
Ub = Velocity of gas through bubble phase, cm/s

Ucw = Velocity of gas through cloud wake phase, cm/s
Ucwn-1 = Velocity of gas through (n-1)th stage of cloud wake phase, cm/s
Ucwn = Velocity of gas through nth stage of cloud wake phase, cm/s
Ug = Gas velocity, cm/s
(Kce)b = Gas interchange co-efficient from cloud wake to emulsion phase, s-1
(Kbc)b = Gas interchange co-efficient from bubble to cloud wake phase, s -1,
Z = Bed height ,cm,
Umf = Minimum fluidization velocity/emulsion phase gas velocity, cm/s,
Uo = Superficial gas velocity, cm/s ,
Ucwn = Velocity of gas through nth stage of cloud wake phase, cm/s,
Cbn = nth stage oxygen concentration in the bubble phase, g-mol /cm3 ,
Ccwn = nth stage oxygen concentration in the cloud wake phase, g-mol /cm3 ,
fcw = Fraction of cloud wake phase in the bed,
εb = Volume fraction of bubbles in the bed. For detailed notations refer (1) and (3).
7.0 REFERENCES
[1] Singh Ravi Inder, Mohapatra S.K. ,Gangacharyulu D.,2008, “ Energy Conservation and
Management, Elsevier, Vol 49 No.11, pp 3086-3103.
[2] J. H. Goo, M. W. Seo, S. D. Kim, B. H. Song, “Effects of temperature and particle size on
minimum fluidization and transport velocities in a dual fluidized bed”, 2009, Proceeding of the
20th International conference on fluidized bed combustion, Springer.
[3] Singh Ravi Inder Singh, “Study of performance of an atmospheric bubbling fluidized bed
combustor using rice waste”, PhD Thesis, 2010, Thapar university, Patiala, Punjab.
[4] Kunni Daizo, Levenspiel Octave. Fluidization engineering. USA: Butterworth–Heinemann;
1991.
[5] Rajput R.K, “Thermal Engineering” Laxmi Publications (P) Ltd. Delhi, ISBN 81-7008-834-
8.
[6] Ganesh A, Grover P D and Ramachandra P V I, 1992, “Combustion and gasification
characteristics of rice husk”, Fuel, 71, 889-894.
DYNAMIC CHARACTERISTICS OF BUBBLING AND
TURBULENT FLUIDIZATION USING A HURST ANALYSIS
TECHNIQUE
H. Azizpour, N. Mostoufi*, R. Zarghami, R. Sotudeh-Gharebagh
Multiphase Systems Research Lab, School of Chemical Engineering, College of
Engineering, University of Tehran, P.O. Box 11155/4563, Tehran, Iran
*
Corresponding author, Tel.: (+98-21)6696-7797, Fax: (+98-21)6646-1024,
E mail: mostoufi@ut.ac.ir
ABSTRACT
A non-intrusive vibration monitoring technique was used to study the flow behavior in
a fluidized bed. This technique has several advantages compared to other
techniques, such as pressure probes and optical fiber probes which may influence
the measurement because they are intrusive. Experiments were conducted in a 15
cm diameter by 2 m tall fluidized bed using 470 micron sand particles. Auto
correlation functions, mutual information function and Hurst exponent analyses were
used to analyze the fluidized bed hydrodynamics near the transition point from
bubbling to turbulent fluidization regime. These methods were able to detect the
regime transition point using vibration signals.
INTRODUCTION
Fluidization is a process in which solid particles become suspended and fluidized at

threshold gas or liquid velocity (minimum fluidization velocity), and the bed adopts
fluid-like characteristics. Today, due to their many advantages, fluidized beds have
industrial applications in many areas, e.g. oil, petrochemical, mineral, biochemical,
pharmaceutical, food processing. The proper functioning of fluid bed reactors
requires suitable means of measuring and monitoring the bed hydrodynamics.
Various techniques have been used to measure signals in fluidized beds. Pressure
probes and fiber optic probes are widely used techniques but they have a
shortcoming of being intrusive. This work utilized a novel non-intrusive method that
measures vibrations in fluidized beds. The most common methods for characterizing
time dependent signals from fluidized beds are time, frequency domain and state
space analyses. Time domain approaches include observation of the time sequence
of the measured signal, standard deviation analysis and analysis of other statistical
moments like skewness, kurtosis and flatness (1-5).
Autocorrelation and mutual information functions are more frequently used in

nonlinear state space analysis to determine time delay of reconstructed attractor (6-
8). Hurst exponent analysis was developed for the first time by Hurst (9) to
distinguish completely random time series from correlated time series. Hurst
exponent was used by Fan et al. (10), Franca et al. (11), Drahos et al. (12), Cabrejos
et al. (13), Briens et al. (14), Karamavruc and Clark (15) to assess the hydrodynamic
status of the fluidized bed. Fast Fourier transform and wavelet transform are also the
mathematical tools used to analyze the pressure fluctuations in fluidized bed, which
express the behavior of a time series in the frequency domain.
1
In the present investigation, auto correlation functions, mutual information function
and Hurst exponent analysis were applied to analyze vibration signals of a gas-solid
fluidized bed and identify the hydrodynamics of the bed.
EXPERIMENTS
The experiment setup is schematically shown in Fig. 1. The experiments were

carried out in a gas-solid fluidized bed made of Plexiglas of 15 cm inner diameter (D)
and 2 m height (L). The gas distributor was a perforated plate containing 435 holes
with 7 mm triangle pitch. Air was supplied by a compressor and its flow rate was
measured by an orifice meter. A cyclone was placed at the column exit to return the
entrained solids back to the bed. Sand particles with mean size of 470µm and
particle density of 2600 kg/m3 were used in the experiments. The system was
electrically grounded to decrease electrostatics effect.
The experiments were carried out a static bed height of 22.5 cm. The same DJB
accelerometer with a cutoff frequency of 25.6 kHz and sensitivity of 100 mV/ms-2 was
used to measure vibration fluctuations signals.
These measuring probes were mounted on the column 10 cm above the distributor
plate by means of a magnet to minimize sudden shakes. To prevent wave
interference and losing information, the sampling frequency of vibration signals was
set to 25.6 kHz. All the measurements were repeated three times to ensure accuracy
and reproducibility of signals.
Figure 1. Schematic of the experimental fluidized bed set-up
METHOD OF ANALYSIS
R/S Analysis
Rescaled range analysis (R/S analysis) was first introduced by Hurst (9) for studying
long-term memory of a time series. Mandelbrot (16) showed that the R/S analysis is
a more helpful tool in detecting long range dependence compared to more
2
conventional analysis like autocorrelation analysis and spectral analysis. In this
method, first cumulative deviation from the mean of the time series x(i) in time
window n is calculated:
N
x (i ) = ∑ ( x (i ) − x n ) (1)
i =1
where
1 n
xn = ∑ x(i )
n i =1
(2)
Then, the range function R(n) is determined as maximum and minimum difference of
time series x(i) in each time interval n:
R (n ) = max ( x (i, n )) − min ( x (i, n )) 1 ≤ i < n (3)
Rescaled range function is obtained by dividing R(n) by the standard deviation S(n):
R R (n )
=
S S (n )
(4)
where the standard deviation S(n) is:
1 n
S (n ) = ∑ (x(i ) − xn ) (5)
n i =1
It has been found that, for some time series, the dependence of R/S on the number
of data points follows an empirical power law described as (10):
(R S ) ∝ n
n
H
(6)
where H is the Hurst exponent and varies between 0 and 1. The Hurst exponent is
equal to 0.5 for stochastic (e.g., white noise) series, less than 0.5 for rough anti-
correlated series and greater than 0.5 for positively correlated series known as
persistence.
For the persistent data set, if the trend or behavior in the data set is increasing or
decreasing over a certain unit interval of time, it would have a tendency to persist in
increase or decrease over such an interval. Hurst exponent can be estimated by
linear regression of ln(R/S) versus ln(n).
Autocorrelation function
The autocorrelation function (ACF) from the mathematics compares linear

dependence of two time series separated by delay and is defined as (7-8):
3
∑ [x (i ) − x ][x (i + τ ) − x ]
N −τ
ACF = i =1
(7)
∑ [x (i ) − x ]
N −τ
2
i =1
where
1 N
x= ∑ x(i )
N i =1
(8)
The time delay for the attractor reconstruction is then taken at a specific threshold
value of ACF where ACF is equaled to one half or zero or the first inflection point of
that.
Mutual information
While the autocorrelation function measures the linear dependence of two variables,
Fraser and Swinney (6) suggested using the mutual information I(τ) function to
determine when the values of x(i) and x(i+τ) are independent enough of each other
to be useful as coordinates in a time delay vector, but not so independent as to have
no connection which each other at all. The mutual information of the attractor
reconstruction co-ordinates is defined as:
N − ( d −1)τ
⎡ P(x(i ), x(i + τ ),", x(i + (d − 1)τ )) ⎤
I (τ ) = ∑ P(x(i), x(i + τ ),", x(i + (d −1)τ )) log⎢ P(x(i ))P(x(i + τ ))...P(x(i + (d − 1)τ ))⎥ (9)
i =1 ⎣ ⎦
where P(x(i)) refers to the individual probability of the time series variable.
In general, the time delay provided by the I(τ) criteria is normally smaller than that
calculated by the ACF(τ) and provides appropriate characteristic time scales for the
motion. As mentioned above, I(τ) presents a kind of nonlinear correlation concept,
while the ACF(τ) provides an optimum linear correlation criterion.
Fig. 2 shows the Hurst diagram of the vibration signal which is measured at 10 cm
above the distributor for particles size of 470 µm, initial aspect ratio L/D of 1.5 and
different gas velocities. According to the figure, the fluidized bed has multifractal
behaviour with three different Hurst exponents. For example, consider the graph
related to the gas velocity equal to 1.0 m/s, it can be seen that for small values of n
(time lag), the Hurst exponent is 0.8451, which is much larger than 0.5, indicating a
highly persistent dynamic feature of the fluidized bed. On the other hand, Hurst
exponent is 0.494 for larger values of n, which is less than 0.5, indicates a highly
antipersistent dynamic feature of the fluidized bed. In general, as stated by
Karamavruc and Clark (15), bubble motions correspond to higher Hurst exponents
than particle motions do. It can be concluded that while Hurst exponent at small
values of n or smaller fractal dimension represents the dynamic feature of macro
structures, Hurst exponent at larger values of n or larger fractal dimension represents
the dynamic feature of finer structures.
4
The Hurst exponent value of macro structures initially rises with increasing the gas
velocity and then declines with further increasing of the gas velocity. This change in
the trend of the Hurst exponent can be related to the regime transition of the fluidized
bed. Increase in the Hurst exponent of the macro structures can be related to the
growth of the bubble size due to the gas velocity increase in the bubbling regime.
However, further increase in the gas velocity in the turbulent regime results in the
decrease of the Hurst exponent because of the breakdown of large bubbles to voids
and small bubbles. (Transition velocity from bubbling to turbulent regime was
calculated equal to U=1.23 m/s by Bi and Grace Correlation).
As pointed out by Fan et al. (17), the reciprocal of the break point in the Hurst profile
is similar to the dominant frequency of the bed. As shown in Fig. 2, the break point
occurs at n equal to 47 points which is equal to a time interval of about 0.00077 (s),
this presents an equivalent dominant frequency of about 1396 Hz which is close to
the value estimated from the power spectrum analysis of the bed vibration signal at
the same conditions (9).
Figure 2. Hurst exponent diagram of the vibration signal measuring in tap height 10 cm above
the distributor at different superficial gas velocity, particles size 470 µm, and L/D=1.5
The autocorrelation function ACF(τ) and the mutual information profile I(τ) of the
vibration signal which is measured at 10 cm above the distributor, for particles
size of 470 µm, initial aspect ratio L/D of 1.5 and different gas velocities is
illustrated in Fig. 3. For U=1.0 m/s, the first pass of the autocorrelation function
from one half and the time delay at which the ACF becomes zero occur at 2 and
9, respectively. The first minimum of the mutual information occurs at a delay
time of 26. As can be seen in this figure, these points initially occur at higher
values of time delay with increasing the gas velocity, on further increase of the
gas velocity results that these points occur at lower time delay. This trend can be
related to the regime transition of the fluidized bed. The growth of the bubble size
by increasing the gas velocity in the bubbling regime means that the behavior of
the system tends to a periodic system. In periodic systems, the first pass of the
5
autocorrelation function from one half and the time delay at which it becomes
zero, and also the first minimum of the mutual information occurs at a higher
delay time in comparison with stochastic systems. When the turbulent regime is
reached by the further increase of gas velocity, time delays were found to occur
at lower point time delays than for the bubbling regime. This shows that the
systems tends to tends to a stochastic system because of the breakdown of large
bubbles to voids and small bubbles.
Figure 3. The autocorrelation function and mutual information profile against delay time for
vibration
CONCLUSIONS
Two different Hurst exponents were identified from the vibration signals measured in
the fluid bed suggesting that the fluidized bed had a multifractal behavior. Higher
Hurst exponent is corresponded to macro structure in the bed, e. g. motion of large
bubbles. The reciprocal of the break point in Hurst profile is similar to the main
frequency of the bed. The value of the larger Hurst exponents increased with
increasing gas velocity and was highest at the bubbling-to-turbulent regime transition
point. The transition velocity was about 1.2 m/s, and system shows the highest
periodical behavior in this point.
The autocorrelation and the mutual information functions were also used to
determine the turbulent transition point from the accelerometer data. The fluidized
bed system at transition point from bubbling to turbulent, the first pass of the
autocorrelation function from one half and the time delay at which it becomes zero,
and also the first minimum of the mutual information occurs at a higher delay time in
comparison with stochastic systems, and the values of time delays were highest at
the bubbling-to-turbulent transition gas velocity. These findings were similar to those
of the Hurst exponent analysis.
NOTATION
ACF autocorrelation function

d embedding dimension
6
D Bed diameter
fs sampling frequency, Hz
H Hurst exponent
I mutual information
L bed height; number of windows
N total number samples
P individual probability
R Rescaled Range function
S standard deviation
t time, s
x vibration signal (m/s2)
Greek symbols
τ Embedding time delay
τ1 Embedding time delay related to ACF=0.5
τ2 Embedding time delay related to ACF=0.0
τ3 Embedding time delay related to minimum mutual information
REFERENCES
1. G. S. Lee, S. D. Kim, Pressure fluctuations in turbulent fluidized beds, J. Chem.

Eng. Japan, 28, 515, 1988.
2. F. Johnsson, R. C. Zijerveldb, J. C. Schoutenb, C. M. van den Bleek, B. Leckner,
Characterization of fluidization regimes by time-series analysis of pressure
fluctuations, Int.J. Multiphase Flow, 26, 663, 2000.
3. H. T. Bi, J. R. Grace, K. S. Lim, Transition from bubbling to turbulent fluidization,
Ind. Chem. Res. Dev., 34, 4003-4008, 1995.
4. D. Bai, E. Shibuya, N. Nakagawa, and K. Kato, Fractal characteristics of gas-
solids flow in a circulating fluidized bed, Powder Technol, 90, 205, 1997.
5. R. Zarghami, Conditional Monitoring of Fluidization Quality in Fluidized Beds,
Ph.D. Dissertation, University of Tehran, 2009.
6. A. Fraser and H. Swinney, Independent coordinates for strange attractors from
mutual information, Phys. Rev. A, 33, 1134-1140, 1986.
7. H. Kantz, T. Schreiber, Ed., Nonlinear time series analysis. Cambridge University
Press, 2002.
8. P. S. Addison, Fractals and Chaos: An Illustrated Course. IOP Publishing Ltd.,
2005.
9. Hurst, H. E., Long-term storage capacity of reservoirs, Trans. Am. Soc. Civ. Eng.,
116, 770, 1951.
10. L. T. Fan, D. Neogi, M. Yashima, R. Nassar, Stochastic analysis of a three-phase
fluidized bed: Fractal Approach, AIChE J., 36, 1529, 1990.
11. F. Franca, M. Acikgoz, R. T. Lahey, and A. Clausse, The use of fractal techniques
for flow regime identification, Int. J. Multiphase Flow, 17, 545, 1991.
12. J. Drahos, F. Bradka, M. Puncochar, Fractal behaviour of pressure fluctuations in
a bubble column, Chem. Eng. Sci., 47, 4069, 1992.
13. F. J. Cabrejos and G. E. Klinzing, Characterization of dilute flows using the
rescaled range analysis, Powder Technol, 84, 139, 1995.
14. C. L. Briens, L. A. Briens, J. Hay, C. Hudson, A. Margaritis, Hurst’s analysis to
detect minimum fluidization and gas maldistribution in fluidized beds, AIChE
J., 43, 1904, 1997
7
15. A. I. Karamavruc and N. N. Clark, A fractal approach for interpretation of local
instantaneous temperature signals around a horizontal heat transfer tube in a
bubbling fluidized bed, Powder Technol, 90, 235, 1997.
16. B. Mandelbrot, the Fractal Geometry of Nature. Freeman, San Francisco, 1982.
17. L. T. Fan, Y. Kang, D. Neogi, M. Yashima, Fractal analysis of fluidized particle
behavior in liquid-solid fluidized beds, AIChE J., 39, 513, 1993.
8
CORRELATION OF THE MINIMUM SPOUTING VELOCITY FOR
THE DESIGN OF OPEN-SIDED DRAFT TUBE CONICAL
SPOUTED BEDS FOR THE TREATMENT OF FINE MATERIALS
M. Olazar, H. Altzibar, G. Lopez, I. Estiati, J. Bilbao

University of the Basque Country, Dept. Chemical Engineering, P.O. Box 644-
E48080 Bilbao, Spain.
ABSTRACT - The hydrodynamics of conical spouted beds provided with open-sided

draft tubes have been studied for the treatment of fine particles. A correlation has
been proposed for the calculation of the minimum spouting velocity as a function of
dimensionless moduli that take into account the geometric factors of the contactor
and the draft tube, particle characteristics and operating conditions.
INTRODUCTION
The spouted bed regime is an alternative contact method to fixed and fluidized
beds. The conventional spouted bed contactor is a cylindrical contactor which has a
conical base. This conventional spouted bed has limitations for operation with deep
beds and solids that are coarse, sticky and have a wide size distribution.
Different modifications of the original spouted bed (cylindrical with conical base) are
proposed in the literature with the aim of improving its performance. These
modifications mainly concern the geometry of the contactor and/or the gas inlet to
the bed. Given the advanced knowledge of their hydrodynamics and applications,
the spouted beds of rectangular section, also with rectangular gas inlet (Freitas and
Dogan (1), Dogan et al (2)), the conical spouted beds (Olazar et al (3,4,5), San José
et al (6), Povrenovic et al (7), Al-Jabari et al (8), Bi et al (9)), and the spout-fluid
beds (Nagarkatti and Chaterjee (10), Sutanto et al (11), Zhao et al (12), Passos and
Mujumdar (13), Ye et al (14,15)), which combine the advantages of the spouted bed
and of the bubbling fluidized bed, are worth mentioning.
Spouted beds with fully conical geometry combine the features of the cylindrical
spouted beds (such as the capacity for handling coarse particles, small pressure
drop, cyclic movement of the particles and so on) with those inherent to their
geometry, such as stable operation in a wide range of gas flow-rates (Olazar et al
(3,16), San José et al (6)). This versatility in the gas flow-rate allows handling
particles of irregular texture, fine particles and those with a wide size distribution and
sticky solids, whose treatment is difficult using other gas-solid contact regimes
(Olazar et al (5,17,18), Bilbao et al (19)). Moreover, operation can be carried out
with short gas residence times (as low as milliseconds) in the dilute spouted bed
(Olazar et al (20,21)).
A crucial parameter that limits scaling up of spouted beds is the ratio between the
gas inlet diameter and particle diameter. In fact, the inlet diameter should be smaller
than 20-30 times the average particle diameter in order to achieve spouting status.
The use of a draft tube is the usual solution to this problem. Nevertheless, solid
circulation, particle cycle time, gas distribution and so on, are governed by the
space between the bottom of the bed and the draft-tube, Moreover, minimum
spouting velocity and operation pressure drop depend also on the type of draft tube
used.
A study has been carried out in this paper on the hydrodynamics of conical spouted
beds with open-sided draft tubes. The main aim is to obtain a correlation for the
determination of the minimum spouting velocity when fine particles are used. In a
previous paper (Altzibar et al. (22)), correlations have been determined for the
design of conical spouted beds provided with non-porous draft tubes, and their
performance has been compared with that of an open-sided draft tube. A detailed
study is carried out in this paper using open-sided draft tubes of different diameter
and aperture ratio in order to establish a reliable correlation for the design of conical
spouted beds provided with this type of tube.
EXPERIMENTAL
The experimental unit used is described in previous papers and allows for operating
with contactors of different geometry (Olazar et al (3,4), San José et al (6), Altzibar
et al. (22)). The blower supplies a maximum air flow-rate of 300 m3 h-1 at a pressure
of 1500 mm of water column. The flow-rate is measured by means of two mass flow-
meters in the ranges 50-300 m3 h-1 and 0-100 m3 h-1, both being controlled by
computer. The blower supplies a constant flow-rate and the first mass flow-meter
controls the air flow that enters the contactor (in the range 50-300 m3 h-1) by acting
on a motor valve that reroutes the remaining air to the outside. When the flow
required is lower than 50 m3 h-1, it crosses the first mass flow meter and is regulated
by the second one placed in series, which also acts on another motor valve that
regulates the desired flow-rate. The accuracy of this control is 0.5% of the measured
flow-rate.
The measurement of the bed pressure drop is sent to a differential pressure

transducer (Siemens Teleperm), which quantifies these measurements within the 0-
100% range. This transducer sends the 4-20 mA signal to a data logger (Alhborn
Almeno 2290-8), which is connected to a computer where the data are registered
and processed by means of the software AMR-Control. This software also registers
and processes the air velocity data, which allows for the acquisition of continuous
curves of pressure drop vs. air velocity.
There are three different zones in the conical spouted bed with draft tube, namely,
spout, annulus and fountain. Figure 1 shows these different zones.
Three conical contactors made of polymethyl methacrylate have been used. Figure
2 shows the geometric factors of these contactors. The dimensions of these
contactors are: column diameter, Dc, 0.36 m; contactor angle, γ, 28, 36 and 45º;
height of the conical section, Hc, 0.60, 0.45 and 0.36 m; gas inlet diameter, D0, 0.03,
0.04, 0.05 and 0.06 m. The stagnant bed heights used are, H0, 0.14, 0.20, 0.25 and
0.30 m.
Figure 1. Zones in the conical spouted bed with draft tube.
Figure 2. Geometric factors Figure 3. Scheme of the

of the conical contactors. open-sided draft tube.
Furthermore, three open-sided draft tubes have been used. The scheme and
geometric factors of the open-sided draft tube are shown in Figure 3. These tubes
are of different aperture ratios with three slots. The widths of the faces on the open-
sided tubes, ωH, are 0.025, 0.018 and 0.010 m, which mean 57, 65 and 78% of open
area (aperture ratio) in the tubes. The diameters of the tubes, DT, are 0.04 and 0.05
m. Moreover, the total length of the open-sided tubes is 0.50 m, which means they
stand about 0.20 m above the bed surface. This length has been chosen according
to previous experimentation in which lower and denser fountains were observed
when the tube end was above the bed surface. In fact, the height above the bed
must be at least 2/3 of the stagnant bed height.
Runs have been carried out by combining all these contactor and draft tubes
variables.
The material used is building sand. Figure 4 shows the particle size distribution
obtained by sieving (ISO 3310).
Figure 4. Particle size distribution of the sand.
The average particle size (reciprocal mean diameter) has been calculated by means
of the expression:
dp =1 [∑ (x i d pi )] (1)
The average size of the sand obtained using eq.(1) is 0.71 mm and the density of
the sand is 2358 kg m-3.
In addition, different fractions of this material have also been used in order to
establish a more reliable correlation. The mean diameters of these fractions are 0.4
and 0.9 mm, respectively.
In order to illustrate the general characteristics of pressure drop evolution in the bed
with air velocity, the results for two different systems are shown in Figure 5 as an
example. The operating conditions are the same for the two systems and only the
value of the width of the faces (ωH) is varied.
Figure 5 shows for the two systems that, at first, as air velocity is increased,
pressure drop increases to a maximum value. Subsequent to the maximum value, a
further increase in air velocity gives way to the fountain and pressure drop
decreases. In order to define more precisely the minimum spouting velocity, air
velocity is then decreased and the values of operating pressure drop are monitored.
A very pronounced hysteresis is noticed, which is due to the fact that peak pressure
drop is much higher than operating pressure drop and, furthermore, a much higher
velocity than the minimum one is required to break the bed and open the spout.
Figure 5 shows that the values of minimum spouting velocity, operating pressure
drop and peak pressure drop are highly dependent on the system configuration. As
observed, the values of the minimum spouting velocity, operating pressure drop and
peak pressure drop increase as the width of the faces is decreased (or as aperture
ratio is increased).
14000
ΔPM WH=2.5 cm; Increasing air velocity
12000 WH=2.5 cm; Decreasing air velocity
Pressure drop (Pa)
WH=1 cm; Increasing air velocity

10000 WH=1 cm; Decreasing air velocity
ΔPM
8000
6000
4000 ΔPS
ΔPS
2000
ums
ums
0
0 5 10 15 20
Air velocity (m/s)
Figure 5. Evolution of the bed pressure drop with air velocity for different values of
the widths of the faces (ωH) when non-porous draft tubes are used.
Experimental conditions: γ=36º; D0=0.04 m; H0=0.25 m, DT=0.042 m.
These higher values are due to the higher solid-cross flow from the annulus into the
spout along the whole length of the spout. Moreover, it is clearly observed that the
solid flow rate increases with the aperture ratio.
From these plots, the minimum spouting velocity has been determined for a wide
range of systems.
In order to ascertain the influence of the different factors on the minimum spouting
velocity, an analysis of variance (ANOVA) of the data obtained following a design of
experiments has been carried out by means of a standard statistical program (SPSS
13.0).
The results show that the parameters of greater influence on the minimum spouting
velocity, ordered by their significance, are the contactor angle (γ), gas inlet diameter
(D0) and width of the faces on the open-sided tubes (ωH), respectively.
The quantitative influence of the variables may be observed by plotting the different
responses vs. factors. Figure 6 shows the change in minimum spouting velocity
caused by the factors of greater influence (contactor angle, a; gas inlet diameter, b;
width of the faces, c).
Figure 6a shows that the minimum spouting velocity goes through a minimum with
contactor angle. Thus, it decreases as contactor angle is increased from 28 to 36
degrees and then increases with this factor. Regarding the gas inlet diameter
(Figure 6b), an increase in this factor (D0) gives way to a sharp decrease in the
minimum spouting velocity. The same happens when the width of the faces is
increased (Figure 6c), but in a much less pronounced way.
Figure 6. Influence of the contactor angle, the gas inlet diameter and the width
of the faces on the minimum spouting velocity.
Based on dimensional and statistical analysis, a hydrodynamic correlation for the

calculation of the minimum spouting velocity in open-sided draft tube conical
spouted beds has been determined as a function of dimensionless moduli that take
into account the geometric factors of the contactor and the draft tube, particle
characteristics and operating conditions. The hydrodynamic correlation previously
obtained by our research group for conical spouted beds without draft tubes (Olazar
et al. (3)) has been taken as a starting point, and a dimensionless modulus related
to the aperture ratio of open-sided draft tubes has been introduced. The correlation
determined is the following:
1.68 −0.57 0.32
⎛D ⎞ ⎡ ⎛ γ ⎞⎤ ⎛A ⎞
(Re0 )ms = 0.126 ⋅ Ar ⋅ ⎜⎜ b ⎟⎟
0.5
⋅ ⎢ tan⎜ ⎟⎥ ⋅ ⎜⎜ 0 ⎟⎟ (2)
⎝ D0 ⎠ ⎣ ⎝ 2 ⎠⎦ ⎝ AT ⎠
This equation is valid for calculating the minimum spouting velocity of stable beds in
conical spouted beds with open-sided draft tubes (regression coefficient r2= 0.87,
and maximum relative error below 8%) in the range of contactor geometries and
operating conditions studied.
CONCLUSIONS
The hydrodynamic study of conical spouted beds provided with open-sided draft
tubes have been carried out operating with fine particles. The evolution of bed
pressure drop with air velocity has been studied in a wide range of conditions.
A very pronounced hysteresis, much higher than in conventional conical spouted

beds, is obtained in the evolution of pressure drop with air velocity.
Hydrodynamics of conical spouted beds with open-sided draft tube is influenced by

the geometric factors of the contactor and draft tube, and operating conditions.
The parameters of greater influence on the minimum spouting velocity are the
contactor angle, the gas inlet diameter and the width of the faces.
The value of the minimum spouting velocity increases as the width of the faces of
the tube and the gas inlet diameter are decreased.
Based on a wide range of experimental results and taken as a reference the
hydrodynamic correlation previously obtained for plain conical spouted beds, a new
correlation has been proposed for predicting the minimum spouting velocity in open-
sided draft tube conical spouted beds.
ACKNOWLEDGMENT
This work was carried out with the financial support of the Ministry of Science and
Technology of the Spanish Government (Project CTQ2007-61167) and of the
Ministry of Industry of the Basque Government (Project IE08-241).
NOTATION
A0 [m2] external area of the tube, empty

AT [m2] external area of the tube, full
Ar [-] Archimedes number, gdp3ρ(ρs-ρ)μ-2
dp [mm] average particle diameter
dpi [mm] average particle diameter of i fraction
Dc [m] column diameter
Do [m] gas inlet diameter
DT [m] draft-tube diameter
g [m s-2] acceleration of gravity
Hc [m] height of the conical section
Ho [m] stagnant bed height
LT [m] length of the tube
(Re0)ms[-] Reynolds number of minimum spouting, per unit area of inlet
section, ρumsdpμ-1
ums [m s-1] minimum spouting velocity at the inlet orifice
γ [deg] included angle of the cone
ΔPS [Pa] operating pressure drop
ΔPM [Pa] peak pressure drop
μ [kg m-1s-1] viscosity of the gas
ωH [m] width of the face of the tube
ρ [kg m-3] density of the gas
ρb [kg m-3] bed density
ρs [kg m-3] density of the particle
REFERENCES
1. Freitas, L. A. P.; Dogan, O. M.; Lim, C. J.; Grace, J. R.; Luo, B. Hydrodynamics
and Stability of Slot-Rectangular Spouted Beds. Part I: Thin Bed. Chem. Eng.
Comm, vol. 181, 243-258, 2000.
2. Dogan, O. M.; Freitas, L. A. P.; Lim, C. J.; Grace, J. R.; Luo, B. Hydrodynamics
and Stability of Slot-Rectangular Spouted Beds. Part II: Increasing Bed Thickness.
Chem. Eng. Comm, vol. 181, 225-242, 2000.
3. Olazar, M.; San José, M. J.; Aguayo, A. T.; Arandes, J. M.; Bilbao, J. Stable
Operation Conditions for Gas-Solid Contact Regimes in Conical Spouted Beds. Ind.
Eng. Chem. Res., vol. 31, 1784-1791, 1992.
4. Olazar, M.; San José, M. J.; Aguayo, A. T.; Arandes, J. M.; Bilbao, J. Pressure
Drop in Conical Spouted Beds. Chem. Eng. J., vol. 51, 53-60, 1993.
5. Olazar, M.; San José, M. J.; Llamosas, R.; Bilbao, J. Hydrodynamics of Sawdust
and Mixtures of Wood Residues in Conical Spouted Beds. Ind. Eng. Chem. Res.,
vol. 33, 993-1000, 1994.
6. San José, M. J.; Olazar, M.; Aguayo, A. T.; Arandes, J. M.; Bilbao, J. Expansion
of Spouted Beds in Conical Contactors. Chem. Eng. J., vol. 51, 45-52, 1993.
7. Povrenovic, D. S.; Hadzismajlovic, Dz. E.; Grbavcic, Z. B.; Vucovic, D. V.;
Littman, H. Minimum Fluid Flowrate, Pressure Drop and Stability of a Conical
Spouted Bed. Can. J. Chem. Eng., vol. 70, 216-222, 1992.
8. Al-Jabari, M.; Van de Ven, T. G. M.; Weber, M. E. Liquid Spouting of Pulp Fibers
in a Conical Vessel. Can. J. Chem. Eng., vol. 74, 867-875, 1996.
9. Bi, H. T.; Macchi, A.; Chaouki, J.; Legros, R. Minimum Spouting Velocity of
Conical Spouted Beds. Can. J. Chem. Eng., vol. 75, 460-465, 1997.
10. Nagarkatti, A.; Chaterjee, A. Pressure and Flow Characteristics of a Gas Phase
Spout-Fluid Bed and the Minimum Spout-Fluid Condition. Can. J. Chem. Eng., vol.
52, 185-195, 1974.
11. Sutanto, W.; Epstein, N.; Grace, J. R. Hydrodynamics of Spout-Fluid Beds.
Powder Technol., vol. 44, 205-212, 1985.
12. Zhao, J.; Lim, C. J.; Grace, J. R. Flow Regimes and Combustion Behaviour in
Coal-Burning Spouted and Spout-Fluid Beds. Chem. Eng. Sci., vol. 42, 2865-2875,
1987.
13. Passos, M. L.; Mujumdar, A. S. Spouted and Spout-Fluidized Beds for Grain
Drying. Drying Technol., vol. 7, 663-697, 1989.
14. Ye, B.; Lim, C. J.; Grace, J. R. Hydrodynamics of Spouted and Spout-Fluidized
Beds at High Temperatures. Can. J. Chem. Eng., vol. 70, 840-847, 1992.
15. Ye, B.; Lim, C. J.; Grace, J. R. Spouted Bed and Spout-Fluid Bed Behaviour in a
Column of Diameter 0.91 m. Can. J. Chem. Eng., vol. 70, 848-857, 1992.
16. Olazar, M.; San José, M. J.; Aguado, R.; Gaisán, B.; Bilbao, J. Bed Voidage in
Conical Sawdust Beds in the Transition Regime between Spouting and Jet
Spouting. Ind. Eng. Chem. Res., vol. 38, 4120-4122, 1999.
17. Olazar, M.; San José, M. J.; Cepeda, E.; Ortiz de Latierro, R.; Bilbao, J.
Hydrodynamics of Fine Solids in Conical Spouted Beds. In Fluidization VIII; Large,
J. F., Laguerie, C., Eds.; Engineering Foundation: New York; pp. 196-201, 1996.
18. Olazar, M.; San José, M. J.; Peñas, F. J.; Bilbao, J. Segregation in Conical
Spouted Beds with Binary and Tertiary Mixtures of Equidensity Spherical Particles.
Ind. Eng. Chem. Res., vol. 33, 1838-1844, 1994b.
19. Bilbao, J.; Olazar, M.; Romero, A.; Arandes, J. M. Design and Operation of a Jet
Spouted Bed Reactor with Continuous Catalyst Feed in the Benzyl Alcohol
Polymerization. Ind. Eng. Chem. Res., vol. 26, 1297-1304, 1987.
20. Olazar, M.; San José, M. J.; Peñas, F. J.; Aguayo, A. T.; Arandes, J. M.; Bilbao,
J. A Model for Gas Flow in Jet Spouted Beds. Can. J. Chem. Eng., vol. 71, 189-194,
1993b.
21. Olazar, M.; Arandes, J. M.; Zabala, G.; Aguayo, A. T.; Bilbao, J. Design and
Operation of a Catalytic Polymerization Reactor in a Dilute Spouted Bed Regime.
Ind. Eng. Chem. Res., vol. 36, 1637-1643, 1997.
22. Altzibar, H.; Lopez, G.; Aguado, R.; Alvarez, S.; San José, M.J.; Olazar, M.
Hydrodynamics of Conical Spouted Beds Using Different Types of Internal Devices.
Chem. Eng. Technol., vol. 32, 463-469, 2009.
WASTE WOOD GASIFICATION: DISTRIBUTION OF
NITROGEN, SULPHUR AND CHLORINE IN A DUAL
FLUIDISED BED STEAM GASIFIER
V. Wilk 1 , C. Aichernig 3 and H. Hofbauer 2

1
Bioenergy2020+ GmbH, Wienerstraße 49, 7540 Güssing, Austria,
veronika.wilk@bioenergy2020.eu, + 43 1 58801 17313
2
Vienna University of Technology, Institute of Chemical Engineering,
Austria
3
Repotec Umwelttechnik GmbH, Austria
Abstract
Waste wood was gasified in a dual fluidised bed gasifier in order to investigate the
behaviour of waste fuels in this technology. The distribution of nitrogen, sulphur and
chlorine between the gasifier and combustor of the dual bed system was studied to
identify the requirements for gas cleaning devices. The gasification system is
suitable for the use of waste wood. A slight adaption of the gas cleaning equipment
was necessary compared to gasification of natural woody biomass.
INTRODUCTION
In order to address the challenge of climate change and global warming the
European Union agreed on the binding target to supply 20% of energy from
renewable sources by 2020 (1). Solid biomass is an important renewable energy
carrier, and it is going to play a major role in the future.
Steam gasification converts solid biomass into a high quality producer gas.
Electricity and heat can be produced in an efficient way from this producer gas; it is
also suitable for chemical synthesis of fuels and chemicals. At the Vienna University
of Technology (VUT) the dual fluidised bed steam gasifier has been developed. The
process was demonstrated in Guessing (Austria) in an 8 MWth gasification plant,
that has operated successfully since 2002. In the meantime further plants are in
operation or currently under construction. In all cases wood chips from natural
sources are used as the feedstock.
The scope of this work is to investigate the suitability of waste wood for the
gasification system described above. The use of waste wood in biomass gasifiers
can increase the feedstock flexibility of the gasifier and could also offer some
economic advantages. Furthermore, gasification is also an interesting approach for
thermal waste wood treatment in general.
1
There are different types of waste wood according to precise quality standards.
Slabs, logs or chippings, bark, fibreboards and surface treated wood are suitable for
biomass combustion plants. Those plants use biomass from forestry as standard
fuel. In Austria there are several power plants, where waste wood is combusted,
among them the biomass plant in Timelkam and St. Veit an der Glan. The boilers
are circulating fluidised beds (2), (3). However, contaminated wood, such as coal tar
oil treated wood or wood-polymer-composites containing halogens, is not suitable
for those plants and has to be treated in waste incineration plants.
Waste wood is already used in gasification processes at an industrial scale. In the

autothermal gasifier in Lahti (Finland) waste wood is part of the feedstock mix (4). In
the Amer power plant in the Netherlands 150.000 t/a of demolition wood are
gasified. In both plants producer gas is combusted in a coal fired power station (5).
The gasifiers are circulating fluidised beds with air as the gasification agent. Air
gasification yields nitrogen-diluted producer gas with a low calorific value.
THE DUAL FLUIDISED BED GASIFIER
The dual fluidised bed gasifier is an allothermal gasifier, where gasification and
combustion take place in spatially divided reactors. The principle is shown in Figure
1. The gasification reactor is fluidised with steam and a bubbling fluidised bed is
formed. The residual ungasified char is transported into the combustion reactor
together with the circulating bed material and is combusted with air. Combustion
takes place in a highly expanded fast fluidised bed. Heat is delivered back to the
gasifier by the bed material to satisfy the endothermic gasification reactions.
producer gas
(CH4, CO, H2, CO2, H2O) flue gas
heat
gasification combustion
biomass auxiliary
fuel
steam circulation air
(bed material, char)
Figure 1: Principle of the dual fluidised bed gasifier
This gasification process has been demonstrated successfully in Guessing (Austria).

Due to steam gasification the producer gas is virtually free of nitrogen. It is
characterised by a high hydrogen content (>40%) and an average heating value of
12-14 MJ/m³ (stp) of dry gas. Producer gas is converted into electrical power in an
internal combustion engine. Heat occurring in the process is fed into the local district
heating system (6). This technology is about to be commercialised. Four new plants
in the range of 10-20 MW are currently being built or are in the start-up phase.
The 100kW pilot plant
At the Vienna University of Technology a 100 kW pilot plant was installed. It is a

prototype of the Guessing gasifier, and has been used for the design of the
Guessing gasifier and is now used to further develop the dual fluidised bed gasifier.
In Figure 2 the pilot plant is schematically illustrated.
2
Figure 2: 100 kW dual fluidised bed pilot plant for steam gasification
Superheated steam for gasification is produced in an electrically heated steam

generator. The gasification reactor and the combustion zone are connected by loop
seals. In order to promote transport of solids and to prevent leakage the loop seals
are also fluidised with steam. In the combustion reactor heat is generated as
residual char is combusted with air. At the bottom of the combustor primary air is
injected and a dense fluidised bed is formed in the bottom region. Light fuel oil is
used as auxiliary fuel; it is also added there. The temperature in the gasifier is
controlled by the amount of oil inserted. Usually the temperature difference between
the gasification zone and the combustor is about 70 to 100°C depending mainly on
the water content of the fuel and the circulation rate. Secondary air is injected at a
higher level to transport particles to the top of the riser. Hot bed material is
transported back into the gasification reactor. In this gasification process olivine is
used as the bed material. It has been proven that olivine has good mechanical
stability and shows moderate tar cracking activity (7).
After leaving the gasifier the producer gas is cooled in an oil-cooled heat exchanger
to temperatures around 250°C and is sampled for gas analysis. Producer gas and
flue gas are mixed and combusted in an afterburning chamber with air. A cyclone
removes particles before passing to the stack.
Measurement equipment
During the experiments, producer gas and flue gas properties are measured. The
main producer gas compounds are analysed by a Rosemount NGA2000 device.
The range of measurement is 0 to 100% for CH4, CO, H2, and CO2 and 0 to 25% for
O2. A gas chromatograph (Syntech Spectras GC 955) is employed for the online-
measurement of N2, C2H4, C2H6 and C3H8.
An impinger bottle method for tar measurement has been developed at VUT. It is
similar to the conventional tar protocol, but has been adapted for producer gas from
steam gasification. Toluene is employed as a tar absorbent. Dust, entrained char,
3
water and tar content can be analysed from one sample. Further description of the
tar measurement is available in (8). NH3, HCl and H2S are also measured by the
impinger bottle method. The ammonia content is determined by dissolution in H2SO4
with a molar concentration of 0.05. Ammonium sulphate is formed and detected by
ion chromatography. The concentration of HCl is analysed by dissolution in H2O2 in
impinger bottles. Chlorine is measured by ion chromatography. For the
measurement of H2S impinger bottles filled with 35%-KOH are used. H2S is detected
by potentiometric titration.
In the flue gas stream the CO, CO2 and O2 content is measured by a Rosemount
NGA2000 device. The range of measurement is 0 to 100% for CO and CO2 and 0 to
25% for O2. For the assessment of NO and SO2 a Rosemount NGA2000 MLT4
device is used, which allows online measurement. The HCl concentration in the flue
gas stream is determined by impinger bottles filled with H2O2. Chlorine is measured
by ion chromatography.
FEEDSTOCK CHARACTERISATION
Two different types of waste wood have been gasified in the pilot plant at VUT.
Waste wood A has been provided by a manufacturer of windows and doors. It
contains pieces of coated chipboards, fibreboards, surface treated wood and
cardboard. It is in the form of chips with particle sizes in the range of 10 to 30 mm
with a considerably high amount of fine particles. Waste wood B mainly consists of
shredded furniture in the form of chips and fibres ranging from 10 to 40 mm. The
content of fine particles is higher than in waste wood A. Table 1 gives an overview at
the elementary analyses.
Table 1: Composition of wood pellets, waste wood A and waste wood B
wood pellets A B
water content % 6.11 6.73 15.49
volatile matter %, dry 86.45 81.39 74.82
ash content %, dry 0.29 1.56 7.90
carbon %, dry 50.23 48.31 48.71
hydrogen %, dry 6.04 5.51 4.78
oxygen %, dry 43.67 43.64 36.41
nitrogen %, dry 0.05 2.49 1.99
sulphur %, dry 0.005 0.03 0.08
chlorine %, dry 0.003 0.02 0.13
net calorific value kJ/kg 18 753 18 420 17 719
Soft wood pellets are the standard feedstock for the pilot plant, as they are
standardised fuel with defined water content and heating value. A significant ash
content has been measured in waste wood B. Therefore, there is less volatile matter
in this sample. The water content is also markedly higher in waste wood B. Soft
wood pellets contain virtually no nitrogen, sulphur and chlorine. Noxious gases are
formed from these elements. Waste wood A contains 2.49% of nitrogen, which is
present in adhesives and coatings. The nitrogen content of waste wood B is in a
comparable range. The chlorine and sulphur content in waste wood B exceeds the
sample of waste wood A.
4
GASIFICATION EXPERIMENTS
During all experiments the main operating conditions of the gasifier are kept
constant in order to achieve similar reaction conditions and comparable results. The
fuel input is about 100 kW. The characteristic temperature in the gasifier is 850°C in
all experiments. The steam-to-carbon ratio, which is determined by fluidisation
settings and water content of the feedstock, is in the range of 1.8 to 1.9. For one
experiment stable gasification of feedstock lasts an average for 6 to 8 h.
During gasification of waste wood B more light fuel oil was required to maintain the
temperature in the gasification reactor. Due to the high water content more energy is
consumed to evaporate the water in the feedstock, which results in a greater
requirement of auxiliary fuel.
In Figure 3 the main producer gas compounds are illustrated. All experiments yield a
similar gas composition, which is typical for steam gasification of woody biomass.
Gasification of waste wood decreases the hydrogen content, but increases CO and
C2H4 yield. Because of the higher nitrogen content in waste wood, a significant
concentration of ammonia has been detected. H2S and HCl content increases with
increase of sulphur and chlorine in the feedstock.
Figure 3: Producer gas composition in vol% referred to dry gas
Table 2: Solid impurities and tar in producer gas
wood pellets A B
dust content g/Nm³, db 8.3 18.8 >>
char content g/Nm³, db 37.7 31.8 >>
GC/MS tars g/Nm³, db 5.5 12.4 >>
gravimetric tars g/Nm³, db 1.8 7.8 >>
Table 2 gives an overview of the solids and tars in the producer gas. Gravimetric
tars are weighed after evaporation of the solvent. A GCMS device is used to
measure the content of many different tar species. As lighter hydrocarbons
(especially indene and naphthalene) disappear during evaporation and not all higher
hydrocarbons are analysed by GC/MS, the measuring range overlaps. The content
of tars and inorganic dust increases significantly, when waste wood is gasified.
Waste wood B contains high amounts of fine particles and ash, which are found in
5
the producer gas. The particle content of producer gas from waste wood B is so
high, that it is not possible to take a sample for tar measurement. Thus, there is no
quantitative information on tar, dust and char for the time being.
DISTRIBUTION OF POLLUTANTS IN THE DUAL FLUIDISED BED GASIFIER
Due to the spatial separation of the gasification and combustion reactors, two gas
streams, producer gas and flue gas, are generated. Volume flows of producer gas
and flue gas are calculated with IPSEpro, an equation-oriented steady state
simulation software. Due to measurements the mass and energy balances form an
over-determinated equation system, which is solved by the Method of Least
Squares. More details about this procedure can be found in (9). Flow rates of the
equilibrated solution represent the basis for balancing trace elements like N, S
and Cl.
Balance of nitrogen
Figure 4 shows the distribution of the main nitrogen compounds in the pilot plant
during the gasification of waste wood. There is N2 in air injected into the combustion
zone and N2 to flush the hopper. Output streams are NH3 and N2 in the producer
gas, and N2 and NO in the flue gas. In the illustration N2 in combustion air, in the
hopper flush and flue gas is omitted, because it does not react. The balance shows
that the vast majority of nitrogen (ca. 90%) is present in the producer gas in the form
of NH3 (waste wood A = 3.4 vol%, waste wood B = 2.7 vol%). Only a small portion of
fuel nitrogen is transported to the combustion section with the char. There it is
oxidised, NO averages 190 ppm (waste wood A) and 110 ppm (waste wood B).
During gasification also other nitrogen compounds such as HCN can be formed;
they have not been analysed yet.
Figure 4: Distribution of nitrogen (left: waste wood A, right: waste wood B)
Balance of sulphur
As sketched in Figure 5, input streams containing sulphur are fuel and light fuel oil.
Figure 5: Distribution of sulphur (left: waste wood A, right: waste wood B)
6
In the producer gas concentrations of 210 ppm (waste wood A) and 570 ppm (waste
wood B) were measured. A small amount of sulphur sticks to ash. In the pilot plant,
producer gas and flue gas are mixed and combusted, then particles are separated in
a cyclone. Thus, producer gas ash and flue gas ash are analysed as a mixture.
When waste wood A is gasified, the SO2 concentration in the flue gas is below the
detection limit. Flue gas of waste wood B contains on average 5 ppm of SO2. Other
sulphur compounds that can be formed during gasification have not been analysed
yet.
Balance of chlorine
Fuel is the only source of chlorine in the gasification process (Figure 6). Minor
contents of HCl are measured in the producer gas, 35 ppm for waste wood A and
70 ppm for waste wood B. The majority of chlorine is bound to ash particles (more
than 90%). HCl in the flue gas was below the detection limit in all experiments.
Other chlorine compounds that might occur have not been determined yet.
Figure 6: Distribution of chlorine (left: waste wood A, right: waste wood B)
GAS CLEANING
The distribution of pollutants in producer gas and flue gas is an important basis for
adaption of the gas cleaning system for use of waste wood. The balance of
pollutants shows that nitrogen and sulphur are mainly present in producer gas and
chlorine is mainly found in ash.
At the demonstration plant in Guessing, producer gas cleaning consists of the

following devices: a precoated bag house filter to remove particles and an organic
scrubber to precipitate tars. That is sufficient for gasification of wood chips from the
forest. If the system has to be adapted to waste wood, some changes will be
necessary. The majority of chlorine is bound to particles, which are removed in the
bag house filter. It has been shown that the precoat material, which is injected at the
Güssing plant prior to the fabric filter, captures chlorine too (10). Thus, no additional
effort might be necessary for chlorine. In the scrubber water in the producer gas is
condensed. If the scrubber is operated at a low pH value, ammonia will be dissolved
in water and will also be precipitated (11). Depending on the concentration of H2S in
the producer gas and legal requirements an additional scrubber for sulphur might be
necessary. Only traces of pollutants are present in flue gas in the pilot plant. As a
first assessment, no adaption of the flue gas cleaning equipment (consisting only of
a bag house filter) is necessary.
7
CONCLUSION
Gasification experiments with two different types of waste wood have been carried
out in the pilot plant at the Vienna University of Technology. From these
experiments it can be concluded that the dual fluidised bed system is suitable for the
gasification of waste wood. The majority of pollutants is present in the producer gas.
Thus gas cleaning equipment in the producer gas line has to be adapted according
to the higher concentration of pollutants in the waste fuels.
ACKNOWLEDGEMENT
We want to thank the team of the Notified Testing Laboratory for Combustion
Systems at VUT for their support. Many thanks to EnergieAG Oberösterreich for
providing the waste wood samples. Bioenergy2020+ is funded within the Austrian
COMET program managed by the Austria Research Promoting Agency FFG. The
financial support of the funding association FFG and the company partners Magna,
Repotec and BKG is gratefully acknowledged.
REFERENCES
1. Directive 2009/28/EC of the European Parliament and of the Council of 23 April

2009 on the promotion of the use of energy from renewable sources
2. M. Bolhàr-Nordenkampf, I. Tschanun, S. Kaiser: Two new biomass fired FBC-
plants with a high fuel flexibility, Proceedings of Power Generation Industry
Conference and Exhibition, Spain (2007).
3. http://www.hsenergie.eu/pdf/Prospekt%20BioCOM_080411_%20englisch_k.pdf
downloaded on 7th October 2010, 04:00pm.
4. D. Granatstein: Case study on Lahden Lampovoima Gasification Project
Kymijarvi power station, Lahti. IEA Bioenergy Agreement Task 36 (2002).
5. M. Spanjers, W. Willeboer: Biomass Gasification for Power Generation –
Essent’s own developments, Proceedings of International Conference on
Polygeneration Strategies, Germany (2010).
6. H. Hofbauer, R. Rauch, G. Löffler, S. Kaiser, E. Fercher, H. Tremmel: Six years
experience with the FICFB gasification process, Proceedings of the 12th
European Biomass Conference, Italy (2002) p982-985.
7. R. Rauch, C. Pfeifer, K. Bosch, H. Hofbauer, D. Swierczynski, C. Courson, A.
Kiennemann: Comparison of different olivines for biomass steam gasification.
Proceedings of the Conference for Science in Thermal and Chemical Biomass
Conversion, Canada, vol. 1, (2004) p799-809.
8. U. Wolfesberger, I. Aigner, H. Hofbauer: Tar content and composition in
producer gas of fluidized bed gasification of wood - influence of temperature
and pressure, Environmental Progress & Sustainable Energy (2009) p372-379.
9. T. Pröll, H. Hofbauer: H2 rich syngas by selective CO2 removal from biomass
gasification in a dual fluidized bed system - Process modelling approach, Fuel
Processing Technology, vol. 89/11 (2008) p1207-1217.
10. I. Siefert: Stickstoff-, Chlor- und Schwefelbilanzen über das Biomasse- Block-
Heiz- Kraftwerk Güssing, PhD Thesis, Vienna University of Technology (2004).
11. T. Pröll, H. Hofbauer: Removal of NH3 from Biomass Gasification Producer Gas
by Water Condensing in an Organic Solvent Scrubber. Industrial & Engineering
Chemistry Research, 44 (2005), p1576-1584.
8
COLD MODEL INVESTIGATIONS OF A HIGH
TEMPERATURE LOOPING PROCESS IN A DUAL
CIRCULATING FLUIDIZED BED SYSTEM
Ajay R. Bidwe, Miguel A.M. Dominguez, Craig Hawthorne, Heiko Dieter, Alexander
Charitos, Anja Schuster, Günter Scheffknecht
Institute of Combustion and Power plant technology (IFK), University of Stuttgart,
Pfaffenwaldring 23, 70569, Stuttgart, Germany.
Email: bidwe@ifk.uni-stuttgart.de
ABSTRACT
The Calcium Looping process is a promising post-combustion CO2 capture

technology. A 200 kWth Dual Circulating Fluidized Bed has been built at IFK,
University of Stuttgart. Tests were carried out on a hydrodynamically scaled cold
model. Operating parameters have been varied, while the suitability of the 200 kWth
design has been proven.
INTRODUCTION
It is now evident that the

anthropogenic CO2 emissions are
causing serious global warming.
Coal and natural gas based power
plants are the major source of CO2
emissions and cause nearly 30 % of
global CO2 emissions (1). Various
pre- and post-combustion CO2
capture options are currently under
investigation. One of the attractive
options is the Calcium Looping
(CaL) process which can be Figure 1- Scheme of Calcium Looping process
integrated with the existing power
plants (2). The CaL process has the advantage of low efficiency penalties of
4 to 6% (3) and can be economical compared to other suggested methods (3). The
basic reaction of the Calcium Looping Process is given in Eq. 1.
CaO(s) + CO2 (g) ↔ CaCO3(s) (1)
A schematic of the CaL process is shown in Fig. 1. This process was first suggested
by Shimizu et al. (4). It consists of the carbonator and the regenerator for the CO2
capture and the sorbent regeneration, respectively. The CO2 rich flue gases are fed
into carbonator where CO2 reacts with CaO to form CaCO3 at 600-700°C. As a
result a CO2 lean gas can is released from the carbonator. The formed CaCO3 is
transferred to the regenerator where at >900 °C CO2 is released again. The sorbent
(CaO) is regenerated by the reverse reaction of Eq. 1. Since the regeneration step
requires energy to heat up and support the endothermic reaction at 900°C; an
oxyfuel combustion is conducted in the regenerator. The exit stream of the
regenerator is CO2 rich, and after compression can be stored geologically (2). The
most suitable reactors are the dual fluidized bed reactors (DFB) and the process has
been successfully demonstrated in various DFB facilities (5)(6). Blamey et al. (2)
reviewed the CaL process as matured enough for a stage of pilot scale
demonstration.
200 kWth Pilot Plant at IFK, University of Stuttgart
At IFK, University of Stuttgart, to

realize the application of CaL
process at pilot scale a dual
circulating fluidized bed (DCFB)
with a capacity of 200 kWth has
been installed (7). The schematic
is shown in Fig. 2, where the
carbonator and the regenerator
are circulating fluidized beds
(CFB) and are connected together
by cone valves for the solid
looping between the reactors. In
previous studies at IFK, CFB
reactors as carbonator were found
to be kinetically more effective
than the bubbling fluidized bed
(BFB) (5)(6). In the regenerator the
heat is generated by the
combustion of fuels. A CFB is
commercially well proven for its
ability as a combustor (8).
Therefore the regenerator is also
Figure 2 - Schematic of DCFB pilot plant and cold selected as a CFB. The Cone
model for CO2 capture using CaO as sorbent and valve is a mechanical valve which
important pressure drops considered in pressure is used also in commercial CFB
balance boilers for transporting material to
the external heat exchangers (9).
Charitos et al. (5) used the cone valve to control the solid looping rate between two
fluidized beds effectively. The cone valve offers the control and variation of the
looping rate independent of the fluidization velocities in the reactors and thus allows
a high flexibility in operation.
The twin cone valve coupled DCFB system at IFK is a new process concept. In
order to support the design of the pilot plant, a scaled cold flow model has been built
and operated under conditions scaled to the real conditions in the pilot plant. The
aim of this paper is summarized as follows a) Prove the hydrodynamic feasibility of
this novel DCFB concept shown in Fig. 2 b) Testing of the cold model and
operational boundary conditions. c) Investigate the effect of important operational
parameters on the operation of the DCFB and find out the optimum way to control
the solid looping rates. The operational parameters are stated in Table 1. The test
will show if the required riser inventories, entrainment rates and solid looping rates
can be met in the pilot plant.
DCFB Cold Model Description
As shown in Fig. 2 the pilot plant consists of two CFBs namely the carbonator and
the regenerator. Table 1 shows the important dimensions of the carbonator and the
regenerator. A detailed description of the 200 kWth pilot plant can be found in (7).
Each CFB has its own internal circulating system comprising of riser - cyclone –
standpipe – loop seal - return leg - riser. Both CFBs reactors are connected by the
cone valves which are placed at the bottom of the loop seals on the supply side of
the standpipes. The discharge of each cone valve is directed to the other reactor.
The cold model, shown in Fig. 2 is geometrically scaled in the ratio of 1:2.5. This
ratio is also maintained for other components of the fluidized bed, i.e. standpipes,
loop seals, etc. The cold model presented in this study is based on the scaling laws
developed by Glicksmann (10). The complete set of equations is given in Eq. 2.
u o2 ρ s u o L1 G s Δp riser (2)
, , , , , , φ , PSD
gL ρ g u mf L2 ρ s u o ρ s gDriser
Basic operational values of the cold model derived from the application of the above
mentioned scaling laws are listed in Table 1. The particles were chosen in order to
match the density ratio of Eq. 1 for the carbonator. The required particle density for
these experiments is 5440 kg/m³. Iron oxide (Fe3O4) particles with a particle density
of 5170 kg/m³ have been chosen. The particle size distribution (PSD) was 100 to
200 µm with a mean size of 166 µm. This PSD at cold flow scale corresponds to a
PSD of about 300-500 µm for the conditions in the pilot plant. Moreover, the gas
density in the regenerator is different than in the carbonator due to different gas
composition and higher temperatures. The gas density of the regenerator is thus
adjusted by using a mixture of CO2 and air, whereas the carbonator is operated on
air. The operational parameters considered in this study are the riser velocity, the
total solid inventory and cone valve opening. While parameters such as riser
pressure drop ( ), riser inventory ( ), entrainment rate ( ) and cone valve
flow rate ( ) are obtained as experimental results. The experimental results from
the cold model are extrapolated to the pilot plant scale using the ratios shown in
Table 1. These ratios are derived from Eq. 2. For example the pressure term in Eq. 2
for the hot pilot and cold model can be matched and 0.87 is obtained
from geometric ratio and particle densities of the hot plant and cold model.
Experimental Procedure
Since the regeneration of the sorbent will be conducted with high O2/CO2 ratios in
the real process, oxidant staging is necessary in order to avoid temperature hot
spots in the hot facility. Moreover oxidant staging will improve the combustion
quality. Therefore, the pilot plant regenerator will have different axial velocity
profiles. For the cold model experiments, a combined velocity rise due to air staging
and gas release is simulated and the scaled velocity is applied with three air stages.
The air in both risers is supplied by a blower and the gas flow rates are measured by
the rotameters. Pressure drop measurements are recorded in different positions at
the cold model using pressure transducers and a data acquisition system. During
the experiment the following parameters are varied: carbonator velocity (u0 Ca),
regenerator velocity (u0 Re), regenerator air staging ratio, total solid inventory (TSI)
and cone valve openings (Acv Ca, Acv Re). Both riser circulation rates are determined
by stopping the loop seal aeration and measuring the time required to achieve a
specific increase of the solid level in the standpipe. Cone valve flow rates are
measured by diverting the cone valve flow into sampling ports, situated below the
cone valves. Flow diversion is done for a specific time and the sample is
subsequently weighed.
Table 1 – Basic values of cold model and 200 kWth Calcium looping DCFB pilot plant
Carbonator Regenerator Ratio

Parameter Unit Pilot Cold Pilot Cold
plant model plant model
m 0.23 0.092 0.17 0.069 2.5
m 10 4 10 4 2.5
°C 650-700 20 850-900 20
kg/m³ 1800 5170 1800 5170
kg/m³ 0.39 1.18 0.44 1.26
m/s 4-6 2.5-4 4-6 2.5-4 1.58
mbar 100 115 60-80 69-92 0.87
kg/m²s 5-25 10-45 10-40 15-70 0.55
Gcv kg/h 500-1200 500-1200
kg 30-50 5.52-9.05 5.43
Pressure Balance
As seen in Fig. 2 there are two clear distinct pressure balance loops for each CFB,
i.e. riser-cyclone-standpipe-loop seal-riser-loop-return leg. The pressure balance for
this loop can be described as follows in Eq. 3 and Eq. 4. This is similar to what has
found in other works on CFB loop (11)(12).
∆ ∆ ∆ ∆ (3)
∆ ∆ ∆ ∆ (4)
∆ and ∆ are the pressure drops in the riser above the return leg of
the loop seal. The pressure drop between the distributor and the return leg entrance
(∆ and ∆ ) does not take part in the pressure balance. The total
pressure drop in the riser is the sum of ∆ and ∆ .
However, in the present DCFB system, there exists another loop linking carbonator
and regenerator similar to Eq. 3 and Eq. 4. The pressure balance for this loop can
be described as follows in Eq. 5 and Eq. 6.
∆ ∆ ∆ ∆ (5)
∆ ∆ ∆ ∆ (6)
The absolute pressure at the exit and standpipe pressure drop ∆ of one
CFB equals the sum of the cone valve pressure drop ∆ , riser top ∆ , cyclone
pressure drop ∆ and absolute exit pressure of the other CFB . Eq. 7 is the
cone valve characteristic equation deduced from Charitos et al. (12). It shows the
relation between flow rate and pressure drop across the valve and its opening.
∆ (7)
In order to ensure mass flow through the cone valve, the pressure at the bottom of
the standpipe should be sufficiently high to overcome the pressure in the other
reactor. It is very important that both cone valves deliver equal amounts of mass in
order to provide a hydrodynamic steady state for the entire solid looping process.
Hydrodynamics of Single Loop Carbonator
Fig. 3 shows the effect of the superficial velocity on the riser inventory. During the
tests only the carbonator has been operated and the total solid inventory (TSI) kept
constant. The total riser inventory clearly decreases with increasing superficial
velocity. This fact is a result of the pressure balance, since a raise in velocity
increases the mass in the riser top region of the riser as shown in Fig. 3 and thus
taking part in the pressure balance. To balance this increased pressure drop
∆ the standpipe should create enough ∆ according to Eq. 2. This is
accomplished by adjusting the required mass from the riser bottom to the standpipe.
The decrease of inventory in the riser bottom is a proof of this.
The inventory carried by the

riser is determined to 8.5 kg
at 2 m/s which corresponds
to 46.1 kg for the pilot plant
extrapolated by scaling ratios
(see Table 1). This amount is
within the inventory range
required in the pilot plant.
Moreover Fig. 3 shows an
increase of circulation rate
(measured after the
cyclone). This results from
the velocity increase in the
carbonator and shows that
the circulation rates are
Figure 3 - Effect of carbonator velocity on inventory and
circulation rates. directly related to the
velocity. The circulation rate
varies from 6.6 to 26.1 kg/m²s and corresponds to 3.64 to 14.38 kg/m²s or 545 to
2150 kg/h extrapolated to the pilot plant using scaling ratios in Table 1. Furthermore,
the circulation rate should be higher than cone valve flow rate. The cone
valve flow rates required in the pilot plant are in the range of 500 to 1200 kg/h, thus
circulation rates projections from carbonator are satisfactory.
Coupled DCFB Behaviour
The most important aspect of the cold model investigations was to prove the
feasibility of a DCFB system interconnected with two cone valves. The pressure
balance as explained earlier shows that reactors, connected with two cone valves
are hydrodynamically linked. Therefore, single parameters affecting the pressure
balance will influence the hydrodynamics of both reactors. For the operation of a
coupled DCFB system, the effect of parameter variations, such as riser velocities,
solid inventory, cone valve openings and its effect on the cone valve flow rate as
well as riser hydrodynamics were studied. For a given set of riser velocities, the total
solid inventory, the cone valve opening, the cone valve flow rate and the riser
pressure drops were always adjusted according to the pressure balance
established. The mass flow rates at both cone valves were equal. Variations of the
riser velocity or the solid inventory have effect on the cone valve mass flow rates.
The inventory transfer between both reactors achieves a stable point with a stable
pressure balance and flow conditions. This behaviour can be seen in Fig. 6 and 7.
The most reliable way to control the flow rates is to change the opening of the cone
valves. In the experiments of Fig. 4 the u0 in both risers and TSI in the system was
kept constant and only Acv in both CFB was varied. With increasing cone valve
opening the flow rate increased. The cone valves used in this study were
geometrically identical and flow rates measured had little deviation as observed in
Fig. 4.

Figure 4 - Variation of cone valve flow with Figure 5 - Cone valve characteristics
opening
Cone Valve Characterization
In Fig. 5 the variation of cone valve flow rate is shown with the product of area of
the cone valve and square root of the pressure drop across the valve. A linear curve
with a satisfactory fit could be observed. The final equation of the cone valve mass
flow is given in Eq. 8. The deduced empirical Eq. 8 is according to equations found
in the literature (13), where the solid flow through mechanical valves is a function of
the opening area and square root of the pressure drop across the valve.
GCV = 0.0261ACV ΔpCV
0.5
+ 26.479 (8)
Regenerator Hydrodynamics at Different Air Staging Ratios
In Fig. 6 and Fig. 7 the effect of air staging in the regenerator on the operational
conditions in the coupled DCFB system is presented. During these experiments, the
conditions in the carbonator, the total solid inventory (TSI) and the cone valve
openings (Acv) were kept constant. The total volumetric flow rate (VFR) in the
regenerator was kept constant at 50 m³/h therefore final u0 Re is equal to 3.7 m/s. The
required VFR in the regenerator is divided into primary air (PA), secondary air (SA)
and tertiary air (TA) as shown in Fig. 2. Fig. 6 shows that with increasing PA, the
regenerator pressure drop decreases from 73 to 34 mbar and at the same time
the carbonator pressure drop increases from 61 to 70 mbar giving an indication
that the bed inventory is transferred from the regenerator to the carbonator. The
raise in the carbonator pressure drop is lower compared to the regenerator

Figure 6 - Effect of air staging in Figure 7 - Effect of air staging on

regenerator on inventory distribution in circulation rates and cone valve flow
DCFB system (Regenerator)
pressure drop because of the larger diameter of the carbonator. From the
present results it becomes obvious that the pressure balances in the coupled DCFB
system play an important role. More primary air shifts more mass towards the upper
region of regenerator. This increases the regenerator standpipe pressure
according to Eq. 4 and Eq. 5 increases. An increase of primary air has a major
effect on the solid flow rate in the regenerator as seen in Fig. 7 and is the main
driving force for the change of circulation rate in the regenerator. The amount of
primary air can also increase the cone valve flow rate rates as given in Eq. 6,
but due to transfer of inventory and changes of pressure values this increase is
limited.
CONCLUSIONS
The scaled cold model investigations of the proposed DCFB system at IFK,
University Stuttgart have been performed. The coupling of two CFB reactors,
interconnected with two cone valves is possible. The flow rate between the beds can
be controlled by the two cone valves and has a characteristic equation. The
pressure balance plays an important role for the inventory distribution and cone
valve flow rate. The cold model was investigated within the required design range,
corresponding to the planned pilot plant. By means of this investigation, the design
of the planned 200 kWth pilot plant was approved.
ACKNOWLEDGEMENTS
We thank EnBW Kraftwerke AG for the funding of this research project.
NOTATION
Acv mm2 area of cone valve T °C temperature

D m diameter u0 i m/s superficial velocity of
riser i
g m/s2 gravitational acceleration umf m/s minimum fluidization
velocity
kg/h cone valve flow rate W kg solid inventory
kg/m2s riser circulation rate Δpi mbar pressure drop in i
L m dimension of a component ρg kg/m³ gas density
Ø [-] sphericity of particles ρs kg/m³ particle density
Abbreviations
CFB Circulating fluidized bed PSD Particle size distribution
CV Cone valve SA Secondary air
DCFB Dual circulating fluidized bed Stp Standpipe
DFB Dual fluidized bed TA Tertiary air
LS Loop seal TSI Total solid inventory
PA Primary air VFR Volumetric flow rate
Subscripts component i
Ca carbonator
Re regenerator
top Part of riser above return leg from loop seal till exit.
bot Part of riser between distributor and loop seal return leg inlet.
REFERENCES
1. Mondol J.B., McIlveen-Wrighta D., Rezvania S., Ye Huanga and Hewitt N., (2009),
“Techno-economic evaluation of advanced IGCC lignite coal fuelled power plantsnext
term with CO2 capture”, Fuel, 88 (12), 2495-2506.
2. Blamey J., Anthony E.J., Wang J., Fennell P.S., (2010), ''The calcium looping cycle for
large-scale CO2 capture'', Progress in Energy and Combustion Science, 36 (2), 260-279.
3. Hawthorne C., Trossmann M., Galindo Cifre P., Schuster A. and Scheffknecht G. (2009),
''Simulation of the carbonate looping power cycle'', Energy Procedia, 1, 1387-1394.
4. Shimizu T., Hirama T., Hosoda H. and Kitano K. A., (1999), ’’Twin fluid-bed reactor for
removal of CO2 from combustion processes'', Chemical Engineering Research and
Design, 77 (1), 62- 68.
5. Charitos A., Hawthorne C., Bidwe A.R., Sivalingam S., Schuster A., Spliethoff H. and
Scheffknecht G., (2010), ''Parametric investigation of the calcium looping process for CO2
capture in a 10 kWth dual fluidized bed.'', Int. J. of greenhouse gas control, 4 (5), 776-784.
6. Rodriguez N., Alonso M., Abanades J.C., Charitos C., Hawthorne C., Scheffknecht G., Lu
D.Y. and Anthony E.J., (2010), “Comparison of experimental results from three dual
fluidized bed test facilities capturing CO2 with CaO”, In proceeding: GHGT-10 Amsterdam
(19-23 Sep 2010).
7. Hawthorne C., Dieter H., Bidwe A., Schuster A., Scheffknecht G., Unterberger S. and Käß
M., (2010), “CO2 capture with CaO in a 200 kWth dual fluidized bed pilot plant”, In
proceeding: GHGT-10 Amsterdam (19-23 Sep 2010).
8. Basu P., (2006), ''Combustion and Gasification in Fluidized Beds”. Taylor & Francis
Group.
9. Wang Q., Luo Z., Fang M., Ni M. and Cen K., (2003), ''Development of a new external
heat exchanger for a circulating fluidized bed boiler'', Chemical Engineering and
Processing, 42 (4), 327-335.
10. Glicksman L.R., (1993), ''Simplified scaling relationships for fluidized bed'.', Powder
Technology, 77 (2), 177-199.
11. Basu P. and Cheng L.,(2000), ''An analysis of loop seal operations in a circulating
fluidized bed”. Chemical Engineering Research and Design, 78 (7), 991-998.
12.Charitos A. Hawthorne C., Bidwe A.R., Korovesis L., Schuster A. and Scheffknecht G.
(2010), ''Hydrodynamic analysis of a 10 kWth calcium looping dual fluidized bed for post-
combustion CO2 capture'', Powder Technology, 200 (3), 117–127.
13. Davidson. J.F and Jones D.R.M. (1965), ''The flow of particles from a fludized bed
through an orifice'', Rheologica Acta 4, 180-192.
HIGH SULPHUR LIGNITE FIRED LARGE CFB BOILERS:
DESIGN & OPERATING EXPERIENCE
M.Lakshminarasimhan, B.Ravikumar, A.Lawrence, M.Muthukrishnan

Building 79, Bharat Heavy Electrical Limited, Trichy, Tamil Nadu, India 620014
phone:+91 431 2574049 e-mail: mlsimhan@bheltry.co.in
INTRODUCTION
One of the measures of the prosperity of a nation is per capita consumption of

electricity. In developing countries like India the gap between supply and demand is
strongly increasing. The demand for all forms of energy is expected to increase
substantially in the foreseeable future and is forecasted to double by 2020.
Although coal would continue to be a major energy source in India due to its
availability, lignite is fast emerging as an alternate source of fuel for electricity
generation. In India the total lignite potential is 4177 million tonnes. The varieties
found in India (Gujarat & Rajasthan region) have moderate to high sulphur (1 to 15
%wt dry ash free) content. It has become economically necessary to use this lignite
for power generation in view of spurt in energy demand while caring for the
environment (by controlling the SO2 emission).
CFB boilers with their in-furnace SO2 capturing capability perfectly suit these
demands and are very attractive while their utilization in comparison with pulverized
fuel boilers would require very expensive add-on flue gas conditioning systems. The
CFB boiler technology designed by BHEL (see Notation list for acronyms) has been
successfully demonstrated for utilities at the 2x125 MWe power project at Surat.
Based on the excellent performance of the units at SLPP, BHEL has bagged order
for 2x125 MWe CFB power plant for RVUNL at Giral, Rajasthan and 1x75 MWe
CFB power plant for GEB, at Kutch, Gujarat. The plant at Giral is now operating
after overcoming unique challenges for firing >15%daf sulphur lignite (one of highest
sulphur-content fuel used in CFB utility-scale units).
This paper provides an overview of the CFB process, its advantages, the
development of CFB technology, and the experience gained from these units in
particular attention to lignite fired units of 125 MWe capacities. The teething
problems experienced during initial operation and their resolution form part of this
paper. With the experience gained at Giral, firing high-sulphur lignite, BHEL is
uniquely placed among CFB boiler manufacturers to meet market requirement of
using such demanding fuels for power generation. The successful operation of the
boiler after surmounting the issues is bound to stimulate utility users to adopt CFB
technology for their proposed projects for such challenging fuels also. Many other
large capacity BHEL CFB boilers (firing range of fuel: from Indonesian coal, lignite
with high/medium sulphur to petroleum coke) are under various stages of
commissioning and will be in operation in another few months.
ROLE OF LIGNITE IN THERMAL POWER PROJECTS IN INDIA
With growing energy consumption, India is looking at utilizing its potential energy
resource in economically and environmentally sustainable manner. The coal
1
varieties found in India are of high ash content, heating values, and sulphur content.
This requires substantial refinement of conventional pulverised fuel combustion
technology by BHEL to suit Indian conditions. The focus has now shifted to utilizing
low-grade lignite varieties with typically high moisture and ash levels with wide
variation in sulphur content. The lignite in India is concentrated geographically to
three states - Tamil Nadu, Rajasthan and Gujarat. The total resource estimated is
around 39 billion tons with proven resource of 4.2 billion tons
Table 1. Lignite resources

State Potential Proven
million tons million tons
Tamil Nadu 31327 2831
Rajasthan 4485 561
Gujarat 2663 785
Puduchery 417 0
Jammu & Kashmir 28 0
Kerala 10 0
West Bengal 1 0
Total 38931 4177
As per the latest indication, share of lignite based thermal projects is bound to
receive an impetus and therefore requires careful selection of combustion
technology. The lignites found at the three major states have different composition
and their own unique behavior. The level of sulphur, ash and moisture, key
parameters for any boiler design, shows remarkable variation among the regions.
This view has been further strengthened by the operating experience of the CFB
power plants designed by BHEL for these fuels
Table 2. Lignite – Key parameters influencing CFB design

Parameter Gujarat Rajasthan Tamil Nadu
HHV(MJ/kg) 11-13 12-16 10-11
Sulphur (%wt) 1.0-4.0 <6.0 <1.0
Moisture(%wt) <42 <40 <55
Ash (%wt) <19 <20 <14
BHEL’S EXPERIENCE IN CFB BOILER
BHEL has developed bubbling fluidized bed technology in response to the national
need to utilize low-calorific fuels in an environmentally sustainable way as early as in
1977. As fluidized bed technology was maturing, BHEL established a test facility in
1991 and good progress has been made in basic understanding of the CFB
technology. In response to the customer’s requirements and with a view to introduce
this technology quickly, BHEL tied up with LURGI LENTJES BABCOCK (LLB) as
collaboration partner in the year 1993. In 1995, BHEL was able scale-up to 175 t/hr
boiler (scale of 30 in thermal heat input terms). The first CFB utility boiler was
introduced in India in the year 1999 after securing an order for 2x125MWe CFB
boiler (scaling by a factor of 3), which was the largest CFB boiler in the country till
recently. The collaboration agreement period with LLB ended by the year 2003. The
successful application of this technology resulted in installation of similar units at
Giral & Barsingsar in Rajasthan, designed and supplied by BHEL, and a repeated
2
order at Surat Gujarat. BHEL further scaled up the CFB unit size by securing an
order for 250MWe units at Neyveli, Tamilnadu.
The first unit of 175t/hr for a paper plant has given a reliability of over 98% till date
while firing a variety of fuels ranging from imported Indonesian coal to Indian coals.
The CFB unit at Surat has also given excellent operating results with the availability
being over 90% and the plant load factor of 85%.
BHEL has recently focused its efforts to diversify into the international market and
secured the first export order in Indonesia for a 120 t/hr boiler in 2007, which is in
successful operation firing low-ash, high-moisture Indonesian coal with unburnt
carbon levels in fly ash of less than 2%. A recent order for a 135 MWe CFB power
plant of the Xstrata group for their prestigious Koniambo Nickel project at New
Caledonia demonstrates the capability of the BHEL CFB boiler in meeting the strict
environmental norms required by the project.
Figure 1. BHEL’s experience in CFB design.
ADVANTAGE OF BHEL’S CFB BOILER
The flue gas flow rate from a unit varies depending on the fuel characteristics,
predominantly its moisture and ash contents. A controlled portion of the solids
sliding down the return leg to the seal pot is diverted via the cone valve (a
mechanical ash-flow control valve) to the FBHEs, while the remaining solids are
returned directly to the combustor at the same temperature. By adjusting the cone
valve opening, the solids flow to the FBHE can be varied, thereby maintaining the
heat absorbed in the combustor constant and consequently its temperature and
combustion conditions for different fuels and loads.
In the absence of the FBHE this variation of the heat absorption in the primary loop
(Combustor, Cyclone and Recycle System) due to variations in fuel quality or load
can be achieved only by:
3
(a) Varying bed density (by altering the primary to secondary air ratio and/or bed
inventory), which becomes operationally difficult;
(b) Varying combustor temperature; or
(c) Varying excess air.
The above variations alter the combustion performance and reduce the boiler
efficiency, and therefore BHEL CFB boiler design for lignite utilizes external fluidized
bed heat exchangers (FBHE) to maintain combustor and steam temperatures. This
provides excellent operational flexibility while maintaining optimum process
conditions. FBHE also provides a unique option of achieving the rated reheat
temperature down to even 50 % of MCR without any attemperation by only
controlling the solids flow through the FBHE containing the reheater coils. This has
enabled operators to handle boiler turndown operation smoothly without undue
concern regarding combustor temperatures.
HIGH SULPHUR LIGNITE CFB BOILER DESIGN
The fuel and steam design parameters of the 125 MWe CFBC units are elaborated
in Table 3.
Table 3. CFB boiler steam parameters
Parameters Units Design Parameters Units Value

Main Steam Proximate Analysis (as fired)
Flow kg/s 112.5 Moisture %wt 40.0
Pressure bar 134.6 Ash %wt 15.0
Temperature °C 540 Volatile matter %wt 20.0
Reheat Steam Fixed carbon (by diff) %wt 25.0
Flow kg/s 93.3 High Heating Value MJ/kg 12.56
Outlet Pressure bar 33.2 Ultimate Analysis (dry ash free)
Outlet Temperature °C 540 Carbon %wt 66.9
Feed Water Hydrogen %wt 4.9
Temperature °C 236.8 Sulphur %wt 13.3
Nitrogen %wt 0.9
Oxygen %wt 14.0
Solid System (Fuel, Bed Material, Limestone & Ash System)
The pre-crushed lignite is withdrawn from the bunkers by two variable speed
extraction drag-link chain conveyors and fed into the seal pot through self-cleaning
type of rotary valves and slide gates, which shut off the fuel feed system from the
combustor in case of an emergency. The system has two parallel trains both of
which need to be operated for optimal fuel combustion. Inert material such as bed
ash or sized sand, required for initial start-up, is fed to the combustor directly by
gravity through a rotary valve. Sized limestone stored in silos is discharged through
variable speed rotary valves at a required rate based on the SO2 content in the flue
gas and is fed by gravity to the seal pot.
Ash is removed from four different locations in the system. Coarse bed ash from the
lower combustor, bed ash from the FBHE, fly ash from the collection hoppers below
4
the convective pass and air heater sections, and fly ash from the electrostatic
precipitator. In order to maintain an appropriate solids inventory in the combustor,
bed ash is continuously extracted from the lower combustor and FBHE through ash
discharge devices cooled in fluidized bed ash coolers.
Air and Gas System
Combustion air is supplied to the combustor by two main streams. Two fans supply
primary air after being heated in a tubular heater. The air is introduced through a
wind box and grate assembly located at the bottom of the lower (refractory lined)
section of the combustor. Similarly two fans supply secondary air, which after being
heated in a tubular air heater is admitted into the lower combustor region by means
of multiple ports located on the walls. Fluidizing air for FBHEs, seal pots, ash
coolers and purge & seal air also form part of the combustion air. Flue gas leaves
the combustor and passes through the cyclones, convective pass, tubular air
heaters, and electrostatic precipitators. Two centrifugal-type induced draft fans
ensure near atmospheric pressure at the outlet of the cyclones. The convective back
pass consists of horizontal superheater, reheater and economizer surfaces with
tubular air heaters for additional heat recovery.
Start-up System
The start-up system consists of two independent start-up burners supplied with air
from the secondary air fans arranged on the sidewalls of the combustor. They are
used for preheating the combustor system and the ash inventory to the ignition
temperature of fuel oil. Fuel oil lances (six units) are then used to further heat up the
ash inventory to the ignition temperature of main fuel - lignite.
Steam-Water Circuits
Feed water enters the in-line horizontal economizer tubes located in the convective
back pass. The steam drum receives sub-cooled water from the economizer and
feeds the evaporators. The evaporative surfaces of the boiler consist of the
combustor water walls, the FBHE water walls and a tube bundle in the FBHE. A
system of down-comers, distribution supply pipes and headers and relief tubes
ensure adequate flow through the evaporator circuits. Drum internals separate and
purify the saturated steam before it feeds the steam-cooled hanger tubes and the
enclosure of the convective pass. The steam is further heated in the superheater
stage I (a horizontal in-line tube bundle) located above the economizer in the
convective pass. After a first stage attemperation the steam flows to the second
stage superheater, which is arranged in two parts in the FBHEs. The second stage
attemperation is arranged between second stage superheater and the final
superheater. The final superheater is the first heat transfer surface in the back pass
and is an in-line horizontal tube bundle.
Cold reheat steam enters the first stage reheater located in the FBHE. The final
reheater stage is located in the convective pass after the final superheater and
before the economizer. Reheat steam temperature is primarily controlled by the
FBHE cone valve, that controls the ash flow through the FBHE containing the
reheater. A spray type attemperator located between two stages of reheater is used
as a secondary control. Refer to Fig. 2 for the arrangement of the boiler surfaces.
5
Figure 2. Arrangement of heat transfer surfaces of boiler
3 1 Bunker
2 Combustor
4 3 Back pass
5 4 Final superheater
1 5 Final Reheater
6
2 6 Low temperature
superheater
8 7 Economiser
8Tubular Air heater
7 9 Fluidized Ash Cooler
ISSUES FACED WHILE FIRING HIGH SULPHUR LIGNITE
Standpipe Blockage
There were three occurrences of unit stoppage due to ash hold-up in the cyclone at
very low loads of about 20 MW and one suspected hold-up at about 70 MW load.
Analysis & Improvements Carried Out
Ash samples and boiler operating conditions were collected. The chemical
compositions of the lignite, limestone and cyclone ash were analyzed. One critical
factor noticed early during cyclone choking was low combustor temperature
(<750ºC) and excessively high limestone addition due to non functional SO 2
measurement equipment.
The phenomenon of recarbonation of calcined limestone not reacted with sulphur

dioxide was suspected as a primary cause for the loose bonding of material at the
cyclone standpipe leading to blockage of the cyclone. This was also reflected in the
analysis by the presence of free lime. The following steps were taken up to relieve
the situation:
a) Limestone feed size was checked continuously with more sampling;
b) Limestone feeder size was optimized by blanking some of its pockets;
c) The operation procedure was revised to maintain higher combustor
temperatures before start of limestone addition;
d) Incorporation of automatic pincing air arrangements at the junction of
cyclone and standpipe to disturb the agglomeration.
It was found from samples that the limestone size was much finer than
recommended. This also resulted in high throughput during low loads because SO 2
measurement was not available to control the volumetric feeder of the limestone. It
should be noted that these incidents occurred during boiler commissioning and initial
stabilization period.
6
Results
After incorporation of the changes in the operation procedure and the pincing air
arrangements, the issue stands resolved. The timing of pincing air has been
subsequently reduced, as it was found that the temperature regime (stable free lime)
is one of key parameter in avoiding the situation of blockage. Figure 3 shows
specific recommendations on avoiding the recarbonation-prone regime for limestone
addition. The curve denotes the limit of equilibrium of calcium compounds. On the
left-hand side of the curve CaCO3 is stable. On the right-hand side CaO is stable.
CaO is abundant if excess limestone is added to the furnace. When the temperature
is reduced into the critical range indicated in the figure recarbonization may take
place, creating a rather sticky carbonate that may cause agglomerates or deposits
on tubes.
Figure 3. Recarbonation prone zone (reference 4).
Back Pass Tube Fouling
Heavy and rapid deposit build-up on the flue gas side of the heat transfer tubes has
been experienced in the back pass of the boiler. Deposit buildup seems most severe
at the low temperature superheater tube bank. Also growth of ash deposit in final-
stage reheater tube bank is observed during the initial period of operation. This
deposit increases the gas-side pressure drop and in turn operation of the ID fans
with high current, causing boiler trips.
Analysis & Improvements carried out
The issue of deposits cropped up during loading the boiler after sorting out the
cyclone blockage problem when the limestone feed rate was increased to maintain
the SO2 emission within limits. The same phenomenon as with the cyclone was
suspected as initiator also for this issue. In order to ascertain the root cause,
samples were taken by an exposure probe in the back-pass tube location to collect
short-term ash deposits, as long term exposure converts calcium carbonate to
calcium sulphate. The results of the detailed study clearly points to recarbonation of
free lime followed by slow sulphation of the deposit as the primary mechanism of
fouling. Improvements in the soot blowing mechanism along with an increase in its
frequency have helped in overcoming the fouling issue.
7
Results
After implementation of high pressure soot blowers (See Fig. 4) along with a
fluidization arrangement for smooth evacuation of the ash falling onto the hoppers,
full load operation with limestone addition to ensure sulphur capture of more than
98% (vs. 97% design) was achieved.
Figure 4 Before Soot Blowing After Soot Blowing
CONCLUSION
CFB technology has emerged as a reliable and cost-effective process for

environmentally friendly power generation. Besides eliminating the need for add-on
equipment for control of emission at a huge cost, the process also accepts wide
variation in fuel quality, eliminates the need for pulverizer, minimizes oil requirement,
and avoids slagging. The issues with regard to utilizing high sulphur fuel have been
understood and changes to overcome the same have been presented.
The CFB technology has been successfully demonstrated for utilities at the 2x125
MWe power project at Surat. Based on the excellent performance of the units at
SLPP, BHEL has bagged order for 2x250MWe CFBC boilers for Neyveli Lignite
Corporation, Neyveli, a 1x125MWe CFB Power plant for RRVUNL at GIRAL,
Rajasthan, and a 1x75MWe CFB Power plant for GEB, at Kutch, Gujarat. They are
under various stages of commissioning. These projects are bound to stimulate utility
users to adopt CFB technology for their proposed projects.
NOTATIONS
CFB - circulating fluidized bed, BHEL -Bharat Heavy Electricals Limited, RRVUNL –
Rajasthan Rajya Utpadan Nigam Limited, GEB- Gujarat Electricity Board, SLPP –
Surat Lignite Power Plant, FBHE – Fluidized Bed Heat Exchanger, MCR –
Maximum continuous rating.
REFERENCES
1. Joint Internal BHEL Analysis report with B. Leckner (2007), Chalmers

University, Sweden.
2. M. Hupa, Investigation into backpass fouling, Åbo Akademy, Finland.
Investigation for BHEL (2010).
3. E. J. Anthony, R. E. Talbot, L. Jia, and D. L. Granatstein, Agglomeration and
fouling in three industrial petroleum coke-fired CFBC boilers due to
carbonation and sulfation, Energy & Fuels (2000) 14, 1021–1027.
4. Prabir Basu, Combustion and Gasification in Fluidised beds, CRC eqn 5.7
8
CHARACTERISTICS OF THE SOLID VOLUME FRACTION
FLUCTUATIONS IN A CFB
Sirpa Kallio, Juho Peltola, Veikko Taivassalo

VTT Technical Research Centre of Finland
P.O.Box 1000, FI-02044 VTT, Finland
ABSTRACT
In the paper, the fluctuation characteristics of the solids volume fraction in a CFB are
evaluated from measurements and Eulerian-Eulerian CFD simulations. In both cases,
similarly large fluctuations are observed in the intermediate voidage range whereas dense
and dilute suspension regions are more uniform, as expected. The frequency distributions of
solids volume fraction are classified to represent three different suspension density regimes:
dilute, dense and intermediate “bimodal” regimes.
INTRODUCTION
Gas-solid flow in a CFB is governed by strong fluctuations in the local solid volume fraction
s. In addition to the hydrodynamics of a CFB process, heat transfer, the distribution of
reagents and the chemical reactions are also strongly affected by the distribution of s.
Hence accurate information on the solids distribution is vital for modelling any CFB process.
Bai & al. (1) and Issangaya et al. (2) analysed temporal variations in s from measurements
and Wang (3) from high-resolution simulations. These studies considered Geldart A
particles in a narrow geometry. In the present study, the fluctuation characteristics of the
solid volume fraction for Geldart B particles in a slightly wider geometry were evaluated from
results of Eulerian-Eulerian CFD simulations and from measurements.
EXPERIMENTS
The solids volume fraction was determined for experiments conducted in a 2D CFB unit at
Åbo Akademi University (Guldén, (4)). The height of the riser was 3 m and the width 0.4 m.
The distance between the riser walls was 0.015 m which renders the bed pseudo-two-
dimensional. The effect of wall friction on the solids is largest at the riser bottom. In the
upper dilute regions, flow patterns tend to become three-dimensional. The width 0.015 m is
thus a compromise selected to reduce these phenomena. The air distributor consisted of 8
equally spaced air nozzles. Solids exit the riser from the top end and they are separated in a
simple separation box from which particles fall through the downcomer into a loop seal
consisting of two fluidized 0.1 m wide sections. Experiments were carried out with different
particle sizes, solids loads and fluidization velocities. In the present paper, a summary of the
experimental findings related to the variation in the solids volume fraction is presented.
In the experiments, a dense vigorously fluctuating bottom region was observed with the
highest particle concentration near the side walls. Above the bottom zone, the suspension
travelled mainly upwards in a form of clusters and a more dilute suspension between the
clusters. At the side walls, the particles fell down either as clusters or as a thin, more
continuous wall layer.
Figure 1 illustrates the flow structure in the bottom section (height 0.03-0.34 m above the air
distributor) and in a section higher up (height 1.14-1.45 m). A denser wall region with falling
clusters can be recognized at both heights. The images show clusters and strands
everywhere in the bed. The widths of the narrowest strands observed were approximately 2
mm. At the higher elevation, the solid concentration inside the clusters was significantly
lower than in the clusters of the bottom region.
Figure 1. Images from two experiments, from the left: at the bottom for superficial gas
velocity U0=2.75 m/s, at the bottom for U0=3.5 m/s, at 1.14-1.45 m height for U0=2.75 m/s,
and at 1.14-1.45 m height for U0=3.5 m/s. Particle diameter is 0.256 mm.
The behaviour of the particles in the CFB unit at these two heights was recorded with a
digital video camera that has the image resolution of 720x576 pixels. For each case, a 30 s
section of the video was analyzed to estimate the average solids volume fractions and the
characteristics of the fluctuations in the chosen locations. The local instantaneous solid
volume fraction s was estimated based on a comparison between the local instantaneous
grey scale values of the video image with the reference values corresponding to an empty
bed and to a packed bed. The same method was used e.g. in Grasa & Abanades (5).
Before determining local solids volume fractions, the grey scale values were smoothed with
a 3x3 pixel Gaussian filter. The used pixel filter corresponds to 1.7 mm scale in the
experimental device.
In Figure 2, the lateral spatial distribution of the average solids volume fraction is plotted at
three heights in the bottom bed region and at 1.14-1.45 m height. The average particle size
in this case is 0.256 mm, fluidization velocity 2.75 m/s and the solids loading in the riser 120
kg/m 3. According to Figure 2, a thick wall layer is formed on both side walls at both heights.
Figure 2. Experimental lateral profiles of the average solids volume fraction at three heights
in the bottom bed region (left) and at 1.2-1.4 m height. Particle diameter is 0.256 mm and
fluidization velocity 2.75 m/s.
A more detailed analysis of the volume fraction fluctuations can be done by examining the
distribution of the instantaneous solids volume fraction. This analysis can be used to identify
different flow regimes and to explain observed behaviour. The probability distributions of the
instantaneous solids volume fraction are presented in Figure 3 for two heights. In the dilute
area at 1.24 m height, the local solids volume fraction is always in the dilute range, whereas
in the bottom zone it varies more and a bimodal distribution is typical. At the walls in the
bottom bed, dense suspension regions dominate.
Figure 3. The histograms of the solids volume fraction at 1.24 m height (top) and at 0.1 m
height (below). Lateral location varies from x=0.20 m (middle of the riser) to x =0.38 m (0.02
m from the right wall) (x goes from left to right, cf. Figure 2). Particle diameter is 0.256 mm
and fluidization velocity 2.75 m/s.
The standard deviation of the volume fraction
( s s )2 (1)
describes the level of time-averaged fluctuation in the solids volume fraction as an easily
comparable number. Hence, if the minimum and maximum values of the variable are
known, the highest value of the standard deviation it can reach is determined by the mean
value. For the solids volume fraction in a granular flow, the theoretical maximum standard
deviation is
, max f( s ) s s ,max s , (2)
where the s , max is the packing limit for the solid particles. The theoretical maximum
standard deviation tends to zero at the dense and dilute limits and has a maximum of
s , max 2 at s s , max 2 .
In Figure 4, the standard deviation of the volume fraction, calculated from the same
experiment as illustrated in Figure 2, is plotted at the same three heights in the bottom bed
region and at 1.14-1.45 m height. In the bottom bed region, the fluctuations in the solids
volume fraction are smallest close to the wall while the highest values are observed at the
edge of the wall layer. Higher up in the riser the pattern is completely different. The biggest
fluctuations are observed on the walls, while in the centre section the fluctuations are
relatively small.
Figure 4. Experimental lateral profiles of standard deviation of the solids volume fraction at
three heights in the bottom bed region. Bed mass on the riser side is 1.94 kg, particle
diameter 0.256 mm, and fluidization velocity 2.75 m/s.
Wang (3) plotted the standard deviation as a function of the local average solids volume
fraction. In the dilute and dense regions, the fluctuations were clearly smaller than in the
intermediate suspension density range. The shape of the curves was observed to be close
to parabolic which can be expected because of the relationship of the mean and the
standard deviation definition, Equation (1). A similar analysis of the experimental data is
carried out here. Since the lateral position and the distance to the walls could also play a
role in the fluctuation characteristics of the suspension, the wall region data (less than 0.02
m from the walls) were considered separately. Due to the experimental arrangement, solids
volume fraction could not be measured in points where the distance to the wall was below 2-
4 mm. The effect of the lateral location on the relationship between average and s is
shown in Figure 5 for three cases.
a) b) c)
Figure 5. The effect of the lateral location on the relationship between average and
average s in the bottom section in the experiments. U0 =2.75 m/s. Particle diameter: a) and
b) 0.44 mm and c) 0.256 mm. Total solids mass in a) and c) 3260 g, and in b) 1940 g.
A high value of the standard deviation indicates extensive clustering and separation into
dense and dilute suspension flows. Figure 5 indicates that both the bed mass and the
average particle size affect the clustering of the suspension. A smaller bed mass and a
smaller particle size both reduce the maximum value of the standard deviation, indicating
that the suspension has become more homogeneous in the experiments. Another reason
for the lower measured standard deviations with the smaller particles is the finer cluster
structures they produce. These can be partially filtered out by the Gaussian filter used for
smoothing the images.
CFD SIMULATIONS
Simulation models
The experiments conducted in the 2D CFB were simulated with the models based on the
kinetic theory of granular flow available in the Fluent 6.3.26 CFD software (6). In addition,
wider fictitious geometries were simulated for comparison. The continuity and momentum
equations used in the transient simulations can be summarized for phase q (gas phase
denoted by g and solid phase by s) as follows:
q qm q u
qm q , k
=0 (3)
t xk
M
q qm u q ,i q qm u q , k u q ,i p q q ,ik q q ,ik pq
= q qs
t xk xi xk xk xi (4)
( 1)
q qm gi ( 1) qs
K gs u g ,i u s ,i
where t is time, x is spatial coordinate, volume fraction, density, u velocity, p gas phase
pressure, ps solids pressure, g gravitational acceleration, K drag coefficient, qs Kronecker
M
delta, the laminar stress, and the local scale turbulent stress.
The granular temperature was obtained from a partial differential equation using the Syamlal
et al. (6) model for the granular conductivity. The solid phase granular viscosity was
calculated from the model by Syamlal et al. (7). The solids bulk viscosity and solids pressure
were calculated from the formulas by Lun et al. (8) ( s , max =0.63). The k- turbulence model
producing the local scale turbulent stress was the version modified for multiphase flows
(“dispersed turbulence model”, Fluent (6)). At the walls, the partial slip model of Johnson
and Jackson (9) was used for the solids with the specularity coefficient equal to 0.001 and
the free slip boundary condition was used for the gas. For the gas-particle interaction, a
combination of the Wen & Yu (10) (at the voidage above 0.8) and Ergun (11) equations was
used. The frictional solids stresses were calculated from the model of Schaeffer (12). The
first-order discretization for time stepping and the second-order spatial discretization were
employed. The time step in the simulation was 0.2 ms. Air inflow velocity at the bottom was
described by a function that reproduces the orifice locations.
Analysis of the fluctuation of solids volume fraction
The results were analysed and plotted in the same way as the experimental data in Figure
5. In Figure 6, results from two simulations with different particle sizes are depicted. In
addition to the difference in particle size, the simulations differ in terms of the mesh
spacings used in the simulations. For the larger 0.385 mm particles, the mesh spacing was
6.25 mm, whereas in the case of the small 0.256 mm particles, the bottom section (< 0.7 m)
of the riser was simulated with a finer mesh with a 3.12 mm spacing. As in the experiments,
in dense and very dilute flow regions in the simulations, the fluctuations in the solids volume
fraction are small whereas in the intermediate suspension density range fluctuations are
large due to the strong clustering tendency of gas-solids suspensions.
The results from the two simulations look similar. The highest values in the standard
deviation are located very close to the volume fraction of 0.315, predicted by Equation (2),
and consistent with the experiments. In both the simulation cases, fluctuations are reduced
close to the walls. Similar reduction was also seen in the experiments, but there the
observed wall effect was smaller (Figure 5) since no measurement data could be obtained
from the near-wall region (less than 2-4 mm from the side walls). The highest value of is
smaller in the case of the larger particles. This is opposite to what was observed in the
experiments where smaller particles produced a more uniform suspension. In the
simulations, the difference in the obtained can also be a result of the differences in the
mesh spacings as indicated by the results for the case of a varying mesh spacing in Figure
6. The coarser mesh used in the simulation with larger particles does not resolve the finest
clusters and this could produce a more uniform suspension in the simulation. This effect of
the mesh on was confirmed by conducting simulations in coarser meshes. In the future,
simulations in finer meshes should be conducted to evaluate effects of the particle size.
Figure 6. Average fluctuation in the solids volume fraction as a function of the average
solids volume fraction plotted for different regions in simulations of 2D CFB experiments
with fluidization velocity 3.15 m/s and particle size 0.385 mm (top) and fluidization velocity
2.75 m/s and particle size 0.256 mm (below). 'Walls' refers to a 0.015 m wide layer at the
side walls. 'Centre' refers to the whole domain without the 0.05 m high bottom section, the
0.015 m wide wall sections, and a 0.05 m high section at the top exit.
The same analysis of the temporal distribution of the solids volume fraction carried out with
the experimental results (Figure 3) was also repeated with the simulation data. Figures 7
and 8 show the probability distribution of the solids volume fraction and its logarithm in the
core region and close to the walls for a few monitoring points. The points represent different
suspension regimes.
Figure 7. Probability distributions of solids volume fraction (left) and logarithm of the solids
volume fraction (right) in the riser core region at different heights in a CFD simulation.
Fluidization velocity 3.15 m/s and particle size 0.385 mm
Figure 8. Probability distributions solids volume fraction (left) and logarithm of the solids
volume fraction (right) close to the riser side wall (at x=0) at different heights in a CFD
simulation. Fluidization velocity 3.15 m/s and particle size 0.385 mm.
Examining probability distributions for a number of points, three distinct types of probability
distributions can be defined and used to identify three different suspension density regimes.
Firstly, for lower time-averaged volume fractions than 0.01, no volume fraction values close
to the packing limit occur and the mode of the volume fraction distributions is very close to
zero. In this case, the probability distributions of log( s) resemble the normal distribution. In
this “dilute” suspension regime, the volume fraction fluctuations are not affected by the
packing limit.
Secondly, at average solids volume fractions above 0.03 and below 0.3, there are
distributions that have distinct modes at very low volume fractions and right at the packing
limit. The distributions of the log( s) consist of a dilute sub-distribution resembling the
normal distribution and a sharp peak at the packing limit (Figures 7 and 8). As the average
solids volume fraction increases, the dilute mode moves toward the packing limit mode and
the packing limit peak grows until the modes merge. In this “bimodal” suspension regime,
the formation of densely packed clusters significantly affects the flow behaviour. The
standard deviation of the solids volume fraction increases as the mean value increases and
reaches its peak values just before the two modes merge.
Thirdly, in the “dense” suspension regime the average solids volume fraction is above 0.35
and there is only one mode in the volume fraction probability distribution: the peak at the
packing limit. As the mean solids volume fraction increases, the distribution narrows towards
the packing limit reducing the volume fraction fluctuations.
CONCLUSIONS
In the paper, the variation of the solids volume fraction in measurements and simulations of
a 2D CFB was analysed. Both the measured and simulated results showed very similar
characteristics. In dense and very dilute flow regions, the fluctuations in the solids volume
fraction are small whereas in the intermediate suspension density range fluctuations are
large due to the strong clustering tendency in gas-solids suspensions. The probability
distribution of the temporal solids volume fraction is characterized by different shapes for the
dilute, bimodal and dense suspensions.
ACKNOWLEDGMENT
The authors gratefully acknowledge the financial support of Tekes, VTT Technical Research
Centre of Finland, Fortum Oyj, Foster Wheeler Energia Oy, Neste Oil Oyj and Metso Power
Oy.
NOTATION
g gravitational acceleration [m/s2] Subscripts

Kgs momentum exchange coefficient [kg/s2m3] f gas phase
p pressure [N/m2] q phase index
t time [s] s solid phase
u,u velocity [m/s] x,y,z rectangular coordinates
U0 superficial velocity [m/s]
Other symbols and operators
volume fraction [-]
Kronecker delta gradient operator
material density [kg/m3] x time average of x
standard deviation
stress tensor [N/m2]
REFERENCES
1. Bai, D., Issangya, A.S., Grace, J.R., Ind. Eng. Chem. Res. 38 (1999) 803-811.
2. Issangya, A.S., Grace, J.R., Bai, D., Zhu, J., Powder Technology 111 (2000) 104-113.
3. Wang, J., Chemical Engineering Science, 63 (2008) 3341-3347.
4. Guldén, M. Pilotmodell av en circulerande fluidiserad bädd, Masters thesis (in Swedish),
Åbo Akademi Univ., Heat Engineering Lab., Turku, Finland, 2008.
5. Grasa G. and Abanades J.C., Powder Technology, Vol. 114 (2001) 125-128.
6. Fluent Inc., Fluent 6.3 Users manual (2006).
7. Syamlal, M., Rogers, W., and O'Brien T. J. MFIX Documentation: Volume 1, Theory
Guide. National Technical Information Service, Springfield, VA, DOE/METC-9411004,
NTIS/DE9400087 (1993). (Referenced by Fluent (6)).
8. Lun, C. K. K., Savage, S. B., Jeffrey, D. J., Chepurniy, N. J. Fluid Mech., Vol. 140 (1984)
223-256. (Referenced by Fluent (6)).
9. Johnson, P.C., Jackson, R. J. Fluid Mech., Vol. 176 (1987) 67-93.
10. Wen, C.Y., Yu, Y.H., Chemical Engineering Progress Symposium Series, Vol. 66
(1966) No. 62, pp. 100-111.
11. Ergun, S., Chemical Engineering Progress, 48 (1952) 89-94.
12. Schaeffer, D. G. J. Diff. Eq., Vol. 66 (1987) 19-50. (Referenced by Fluent (6)).
COAL AND BIOMASS CO-GASIFICATION IN A CIRCULATING
FLUIDIZED BED REACTOR
Andrzej Czaplicki, Marek Sciazko
Institute for Chemical Processing of Coal, 1 Zamkowa St. 41-803 Zabrze, Poland
ABSTRACT
Co-gasification tests of subbituminous coal with biomass were performed. A rape

straw blended with coal was used in a mass ratios of coal/biomass of 25%, 50% and
75%. The gasification process was conducted in a circulating fluid bed reactor at
atmospheric pressure with air and steam addition was applied to the reaction. The
addition of biomass to coal resulted in a higher conversion to gas and increased the
gas calorific value due to higher content of carbon oxide.
INTRODUCTION
Co-gasification of biomass with coal can contribute to a reduction of CO2 emissions

and may reduce the dependence on fossil fuels [Valero and Uson (1), Kezhong et al
(2)]. The high reactivity of biomass and its high volatile matter content suggests that
some synergetic effects can be expected in a simultaneous thermo-chemical
treatment of biomass and coal [Fermoso (3)].
Co-gasification of coal and biomass has been extensively studied in different scales,
reactors and conditions [McKendry (4), Andre et al (5), Aznar et al (6), Pinto et al
(7), Kurkela et al (8), de Jong et al (9), Brown et al (10), Chmielniak and Sciazko
(11), Kumabe et al (12)]. Gasification of coal and biomass in a circulating fluid bed
offers a number of advantages. However, the most important is stabilization of bed
inventory due to lower reactivity of the coal char [Collot et al (13)]. As a result of
decomposition three products are obtained: gas, coal tar and a solid product – char
[Velez et al (14)]. The degree of decomposition of the fuels used and the efficiency
of the process depend mainly on the temperature of gasification. Typically the
process is carried out in the temperature range of 800 to 1000 °C. The main
difference is manifested in the yield of products depending on the coal/biomass
ratio.
TEST RIG DESCRIPTION
The testing facility used for the study of solid fuels gasification was aimed at
obtaining two basic products: char and process gas. The main components of the
plant were: a circulating fluidised bed reactor, a system for raw material preparation,
char separation from a hot process gas, a process gas cooling and cleaning, and a
combustion chamber for process gas utilization.
The gasification reactor consists of two sections: the lower, composed of two
inverted cones connected by a cylindrical section of 0.38 m I.D., and the upper part
– a riser of 0.14 m I.D. The total length of the riser was 4.41 m. The reactor
operation depends on a gas phase velocity and on a solid phase concentration. The
bottom section operates as a turbulent or a bubbling fluidised bed. These
hydrodynamic conditions enable high values of heat/mass transfer coefficients and
good mixing of blended fuels in the bed to be achieved.
A proper blends of coal and biomass after drying were delivered to the test facility in
containers. The plant configuration and instrumentation enabled studying the
gasification processes over a wide range of temperatures, using air and steam as
gasification agents. The process diagram of the plant is shown in Figure 1.
Figure 1. Test rig for coal - biomass co-gasification
The temperature and pressure distributions were measured throughout the system
and air, steam and process gas flow rates were recorded for a mass balance
evaluation. Coal, biomass and char mass flow rates were determined by averaging
measured mass of the solids fed or received over the testing time.
TESTING METHODOLOGY
Six tests were performed to gasify coal (Run 1), biomass (Runs 5 and 6) and coal –
biomass mixtures (Runs 2 - 4). A hammer mill and a drum dryer-mixer were used to
prepare homogenous raw materials and their mixtures. Tests were started once the
plant had been checked and the raw material prepared. The reaction system was
heated to the desired temperature by burning a butane - propane mixture. The
feeding of coal was started when the temperature in the gasification zone reached
about 650°C. Having initiated the process of gasification, the burner of the start-up
combustion chamber was shut off. Once a stable temperature in the gasification
zone was achieved at the level of about 800°C the start-up material was replaced
with the proper fuel and the assumed process parameters were achieved. The test
was started after stabilisation of process conditions. On average, one test run was
carried out over 4 h.
PROPERTIES OF FUELS USED
The composition of the raw materials gasified is given in Table 1.
Table 1. Raw material composition in the gasification tests

Raw material composition, w/w %
Test No.
Wieczorek coal Rape straw
Run 1 100 0
Run 2 75 25
Run 3 50 50
Run 4 25 75
Run 5 0 100
Run 6 0 100
Properties of Wieczorek coal and rape straw are given in Table 2.
Table 2. Physicochemical properties of Wieczorek coal and of rape straw*)

Property Wieczorek coal Rape straw
Proximate analysis, w/w %
Moisture content 3.9 6.1
Ash content 9.9 4.3
Volatile content 30.6 73.8
Ultimate analysis, w/w %
Total sulphur content 0.6 0.1
Total carbon content 72.4 45.1
Hydrogen content 4.2 5.2
Nitrogen content 1.1 0.4
Chlorine content 0.28 0.31
Fluorine content <0.01 <0.01
Net calorific value, MJ/kg 28.4 15.4
)
* air dry basis
The characteristic temperatures of Wieczorek coal and rape straw ash fusibility are
given in Table 3.
Table 3. Characteristic temperatures of Wieczorek coal and rape straw ash
under oxidative conditions
Characteristic temperature, °C Wieczorek coal Rape straw
Sintering point 1100 900

Softening point 1200 1380
Melting point 1220 1530
Flow point 1280 1540
The partice size analysis of the Wieczorek coal and of rape straw are given in Table 4.
Table 4. Particle size analysis of Wieczorek coal and of rape straw

Particle size, Content, %
mm Wieczorek coal Rape straw
>3.15 6.8 3.8
3.15-2.0 14.3 11.0
2.0-1.0 22.9 32.5
1.0-0.5 17.4 29.9
0.5-0.2 15.5 16.7
<0.2 23.1 6.1
Total 100.0 100.0
PROCESS DATA
Basic process parameters of gasification tests are presented in Table 5.
Table 5. Process parameters of gasification tests

Test No. Run 1 Run 2 Run 3 Run 4 Run 5 Run 6
Temperatures
o Gasification
TR02, C 940 981 910 966 899 812
zone
Outlet from
TR03, °C 957 937 990 1094 1021 944
the reactor
TR04, °C Riser 921 865 925 897 912 836
TR05, °C Expander 866 825 805 743 793 795
Downstream
TR06, °C 742 705 658 560 655 720
the cyclone
Air to the
TR10, °C 80 63 56 58 60 61
reactor
TR11, °C Steam 137 152 100 101 149 154
Flow rates
3 Air to the
FR01, m /h 115.2 117.5 90.4 85.6 94.7 92.1
reactor
Air to the
3
FR02, m /h combustion 20.5 24.2 20.02 18.9 19.3 18.9
chamber
Steam to the
FR12, kg/h 11.0 0.3 0.3 0.8 2.8 0.0
reactor
Table 5 (continued)
Test No. Run 1 Run 2 Run 3 Run 4 Run 5 Run 6

Process gas
3 downstream
FR041, m /h 167.0 159.0 133.0 125.0 157.0 163.0
the cyclones
battery
Pressures
Gasification
PR02, kPa 6.1 6.3 6.6 9.3 8.7 9.4
zone
Outlet from
PR03, kPa 1.8 2.3 1.9 2.1 4.0 5.0
the reactor
PR04, kPa Riser 2.0 2.4 2.0 2.2 4.1 5.7
Output of the screw-conveyor feeder
Feeder
VR01, % 26.3 42.9 35.6 44.3 61.7 80,6
revolutions
Coal/biomass flow rate,
112,0 83.5 82.7 70.8 97.0 116.0
kg/h
ANALYSIS OF RESULTS
Mass balances for the gasification tests were made and were found to agree within
a relative error not higher than ±3%. The fuel conversion efficiency in a particular
test is presented in Fig. 2. It was calculated as feedstock quantity converted to gas
divided by the total solid fuels fed to the reactor expressed in w/w %.
Figure 2. Fuel conversion efficiency versus feed composition (TG - gasification

temperature)
The fuel conversion efficiency increased with increasing rape straw content in the
gasified mixture (which ranged from 48% for coal to 81% for rape straw). The
highest increase in the fuel conversion efficiency was observed at rape straw
contents in the mixture of 75% to 100%. A decrease of straw gasification
temperature by around 90°C resulted in the decrease of its conversion efficiency by
about 2%. The output data for process gas and char are shown in Fig. 3. The
highest yield of gas (2.4 kg/kg) was obtained for the mixture containing 75% coal
and 25% rape straw. The lowest yield (1.71 kg/kg) was for pure rape straw gasified
at 812°C. The char yield systematically decreased with increasing rape straw
content in the mixture. A decrease in straw gasification temperature by around 90°C
resulted in a slight (by 0.2 kg/kg) increase in char yield.
Figure 3. Process gas and char yields
Figure 4. Main combustible component content in the process gas

Hydrogen, carbon oxide, methane and ethane contents in the process gases
obtained from the tests are presented in Fig. 4. The content of carbon oxide,
methane and ethane show an increasing trend with an increase in the rape straw
content in the gasified mixtures. The hydrogen content reached a minimum (4.90%)
for the mixture containing 50% of Wieczorek coal and rape straw.
The content of the condensable organic matter (tar) in the process gases (presented
in Fig. 5) increased with increasing content of the rape straw in the mixtures and
ranged from 6 g/Nm3 for pure Wieczorek coal to 12.6 g/Nm3 for pure rape straw.
Depending on process parameters the HHV of process gas ranged from 4 to 7
MJ/m3 (Fig. 6).
Figure 5. Yield of condensable organic matter
Figure 6. Process gas high heating value

CONCLUSIONS
The mass balances for the gasification tests had relative error smaller than 3%. The
fuel conversion efficiency (feedstock quantity converted to gas divided by the total
solid fuels fed to the reactor) increased as long as the rape straw content increased
in the gasified blend. A drop in gasification temperature with rape straw by 90oC
caused the drop in its conversion efficiency by 2%. The addition of biomass to coal
resulted in a higher conversion to gas and increased the gas calorific value due to
higher content of carbon oxide.
REFERENCES
1. A. Valero, S. Uson. Oxy-co-gasification of coal and biomass in an integrated

gasification combine cycle (IGCC) power plant. Energy 31 (2006), 1643-1655.
2. l. Kezhong, Z. Rong, B. Jicheng. Experimental study on syngas production
by co-gasification of coal and biomass in a fluidized bed. International journal
of hydrogen energy 35 (2010) 2722-2726.
3. J. Fermoso, B. Arias, M.V. Gil, M.G. Plaza, C. Pevida, J.J. Pis, F. Rubiera.
Co-gasification of different rank coals with biomass and petroleum coke in a
high-pressure reactor for H2-rich gas production. Bioresource Technology,
101, (2010), 3230-3235.
4. P. McKendry. Energy production from biomass (part 3): gasification
technologies. Bioresource Technology, 83, (2002), 55-63.
5. R.N. Andre, F. Pinto, C. Franco, M. Dias, I. Gulyurtlu, M.A.A. Matos, I.
Cabrita. Fluidised bed co-gasification of coal and olive oil industry wastes.
Fuel 84 (2005) 1635-1644.
6. M.P. Aznar, M.A. Caballero, J.A. Sancho, E. Frances. Plastic waste
elimination by co-gasification with coal and biomass in fluidized bed with air
in pilot plant. Fuel Processing Technology 87 (2006) 409-420.
7. F. Pinto, F. Franco, R.N. Andre, M. Miranda, I. Gulyurtlu, I. Cabrita. Coga-
sification study of biomass mixed with plastic wastes. Fuel 81 (2002) 291-297.
8. E. Kurkela, J. Laatikainen, P. Stahlberg. Clean coal technology programme.
Paper C9, vol. III. University of Sttuttgart: 1995. p. 1-20.
9. W. de Jong, J. Andries, K.R.G. Hein. Coal/biomass co-gasification in a
pressurised fluidised bed reactor. Renewable Energy 16 (1999) 110-1113.
10. R.C. Brown, Q. Liu, G. Norton. Catalytic effects observed during the co-
gasification of coal and switchgrass. Biomass Bioenergy 18 (2000) 499-506.
11. T. Chmielniak, M. Sciazko. Co-gasification of biomass and coal for methanol
synthesis. Applied Energy 74 (2003) 393-403.
12. K. Kumabe, T. Hanaoka, S. Fujimoto, T. Minowa, K. Sakanishi. Cogasifyca-
tion of woody biomass and coal with air and steam. Fuel 86 (2007) 684-689.
13. A.-G. Collot, Y. Zhuo, D.R. Dugwell, R. Kandiyoti. Co-pyrolysis and co-
gasification of coal and biomass in bench-scale fixed-bed and fluidised bed
reactors. Fuel 78 (1999) 667-679.
14. J. F. Velez, F. Chejne, C.F. Valdes, E.J. Emery, C.A. Londono. Co-
gasification of Colombian coal and biomass in fluidized bed: An experimental
study. Fuel 88 (2009) 424-430.
A PYROLYSIS PILOT UNIT INTEGRATED TO A CIRCULATING
FLUIDIZED BED BOILER - EXPERIENCES FROM A PILOT PROJECT
J. Autioa,*, J. Lehtoa, A. Oasmaad, Y. Solantaustad, P. Jokelab, J. Alinc

a
Metso Power, Kelloportinkatu 1 D, PO Box 109, FI-33101 Tampere, Finland
b
UPM, Eteläesplanadi 2, PO Box 380, FI-00101 Helsinki, Finland
c
Fortum, Keilaniementie 1, Espoo, PO Box 100, 00048 Fortum, Finland
d
VTT, Biologinkuja 5, PO Box 1000, FI-02044 VTT, Finland
ABSTRACT
A novel integrated pyrolysis pilot plant has been built in Tampere, Finland by Metso,
in co-operation with UPM, Fortum and VTT. A 7 tons of bio-oil per day (2 MW fuel
input) fast pyrolysis unit has been integrated with Metso’s 4 MW th CFB pilot boiler.
Test runs of bio-oil production have been carried out during 2009-2010. More than
80 tons of bio-oil has been produced and utilization tests have been started in
district heating burner applications.
INTRODUCTION
Bio-oils from plant residues are an alternative to fossil fuels. The industrial
feedstocks forest residues, forest industry residues, and some agricultural residues
such as straw can be used. It has been estimated that these residues offer a
considerable, potential source for conversion. The use of bio-oil (bio crude, fast
pyrolysis oil, flash pyrolysis oil, pyrolysis liquid) as a fuel oil in industrial kilns,
boilers, diesel engines, and gas turbines has been tested. Further use in the
production of chemicals and feedstock for synthesis gas production (and the further
production of transportation fuels and C1-chemicals) is also being developed. Bio-oil
has also been upgraded on a small scale, to transportation fuel fractions. However,
at the moment bio-oil is only used commercially in the food flavoring industry (1).
Once produced, bio-oils can be shipped, stored and utilized much like conventional
liquid fuels, if their specific fuel properties are taken into account. As experienced in
test use over the years, bio-oil qualities have varied considerably. However, once
larger scale observations are available, the specific properties of bio-oils will be
better understood and proper utilization procedures developed.
Introducing a new fuel, for example bio-oil, into the markets, will not be easy. Bio-oil
is different to conventional liquid fuels and many challenges remain. In view of such
difficulties, a stepwise market introduction is proposed: bio-oil would first replace fuel
oil in boilers, where its properties would not prove prohibitive. An example of such a
chain has been presented earlier (2). Once the entire chain from biomass to fast
pyrolysis plants to heat utilization has been proven, other applications may be
demonstrated.
There is general awareness of the current competition for good quality biomasses
for use as fuel. Biomass is especially popular in power production, with market
incentives in place in many EU countries to produce green electricity. Power plants
will remain large users of wood fuels, since, for example, modern fluidized-bed
boilers can use several types of biomass. To compete on the markets, bio-oil
production must provide a higher payoff for the investor than the current
alternatives.
The bio-oil production potential of the European pulp and paper industry has been
analyzed by Sipilä et al (3). Their findings show that the European pulp and paper
industry alone has the potential to build up to 50 pyrolyzers integrated with fluidized-
bed boilers. In the short-term, the bio-oil market lies in fuel oil and natural gas
replacement in lime kilns and boilers. The challenge is to develop and demonstrate
a technical and economic concept for these applications.
Metso, UPM, and Fortum have agreed on a joint venture forming part of a more
extensive development program focusing on the development of pyrolysis
technology and its introduction on the market. This joint venture, which targets the
promotion and advancement of research on an integrated bio-oil concept, involves
expertise in the implementation of this concept across the entire value and
production chain. Metso is in charge of delivering the related technology. UPM, a
raw material supplier, plant operator and user of the final product, and Fortum, plant
operator and user of the final product, complete the value chain. VTT (Technical
Research Centre of Finland) is a research partner in the work.
INTEGRATED PYROLYSIS PILOT
Metso has built the world’s first integrated pyrolysis pilot plant in Finland in co-
operation with UPM, and VTT. A 7 tons of bio-oil per day (2 MW fuel) fast pyrolysis
unit has been integrated with Metso’s 4 MW th circulating fluidized bed pilot boiler,
located at Metso’s R&D Center in Tampere. This project is also partly funded by
TEKES, the Finnish Funding Agency for Technology and Innovation. The joint
venture was begun in 2007 (Fortum joined in August 2009), the pilot plant was
finalized in early 2009, and hot commissioning took place during the spring and
summer of 2009.
The hot sand of a fluidized bed boiler offers a considerable opportunity to integrate
the pyrolysis and combustion processes. A fluidized bed boiler acts as a heat source
for pyrolysis, in addition to which it can easily combust the coke and uncondensed
gases produced during the pyrolysis process, into electricity and heat. In this way,
high efficiency can be achieved also for pyrolyzed fuel. In addition, when integrated
with a fluidized bed boiler, pyrolysis represents a cost efficient way of producing bio-
oil, which can be used to replace fossil oils. Considerable savings can be achieved
in operating costs and the price of the investment in both new boiler projects and
retrofit solutions. Industrial, fluidized bed boilers are very large in size, totaling
several hundreds of megawatts at their largest, for which reason even large
pyrolyzers can be integrated. The operation of the entire integrated plant can be
optimized through efficient and intelligent automation. It may be possible to produce
electricity, heat and bio-oil at the same boiler plant in the future.
The process is illustrated in Figure 1. Hot solids from the pilot boiler are led into an
entrained flow reactor, in which solids (sand and char) are separated from the gas
stream and returned to the boiler circulation loop. The formed pyrolysis gases are
condensed in a 2-stage scrubber and condenser system. The remaining non-
condensable gases are recycled to the reactor as fluidization medium, while surplus
NCG’s are led to the boiler through a lance. Product oil from the condensing stage is
led to an intermediate storage tank.
Figure 1. Pyrolysis pilot unit flowsheet
First results from bio-oil production have been encouraging. During the first season
of test runs, more than 80 tons of bio-oil has been produced. The integrated concept
has been verified as a reliable and flexible technology for the production of bio-oil.
Compared to stand-alone pyrolysis unit with a non-optimal small boiler for
combustion of pyrolysis by-products (char and pyrolysis gases), the integrated
concept is easy and smooth to operate. For pyrolysis having a steady and smooth
flow of input energy (i.e. boiler sand) to pyrolysis is a considerable advantage from
the operator point of view.
The integration of pyrolysis and combustion processes has been successful.

Pyrolysis process can be started, operated and shut down without compromising
boiler process. The controllability of the integrated concept has also been good. One
of the critical features of pyrolysis is the ability to maintain constant reactor
temperature during operation. An example of the controllability of the integrated
concept is shown in Figure 2. Since pyrolysis reactor is integrated directly to the
boiler, there is an interest to find out how potential boiler temperature variations
effect pyrolysis temperature. Boiler temperature disturbances are seen in Figure 2. It
may be seen that pyrolysis temperature control handles rapid changes of boiler
sand temperature smoothly.
850 550
825 525
Boiler bed temperature, °C
Pyrolysis temperature, °C
800 500
775 475
Boiler sand
Reactor
750 450
5.11.09 11:00 5.11.09 17:00 5.11.09 23:00 6.11.09 5:00
Date & Time
Figure 2. An example of pyrolysis reactor temperature control
Solids contents in bio-oil have been below 0.2 wt-% using pine as feedstock without
any additional solids removal stage. Removal of solids from extractive-rich (forest
residues) bio-oils is challenging and needs further development. A continuous
centrifuge has been used successfully (Figure 3), other methods will also be
developed.
0,2
IN OUT
Solids, wt%
0,1
0,0
Figure 3. Solids removal by on-line centrifuge, average solids reduction 40 wt% from
two measurements
QUALITY CONTROL
A quality control chain will be developed for the whole chain from biomass selection
to oil use. Feedstock drying down to 8 – 10 wt-% moisture content is monitored with
on-line moisture analyzer. The ground and dried feedstock is then analyzed for fuel
oil properties. The amounts of volatiles and/or ash give indication on pyrolysis
organic yields (Figure 4).
75
70
65
Organic yield wt%
60
55 PDU
Pilot pine 1
50 Pilot pine 2
45 Pilot pine 3
Pilot FR1
40 Pilot FR 2
35
70 75 80 85 90
Volatiles wt%
Figure 4. Yield of organic liquids in biomass pyrolysis as a function of feedstock

volatile matter, wt % based on dry feed
During pyrolysis, water and solids content in the product liquid will be followed on-
line. Due to the novelty of the product medium, pyrolysis oil, analysis was first
restricted to laboratory analysis and automatic on-line analyzers, like on-line Karl-
Fischer titration. These provide accurate results from samples, but take time and, in
the long run, are expensive due to reactant consumption and labor costs. Advances
were made in measurement technology for in-line measurement of bio-oil moisture,
one of the key properties that are continuously monitored, when Metso’s microwave-
based analyzers (MCA) were successfully tested. Microwave technology is widely
used in e.g. pulp & paper industry for pulp consistency measurements. The in-line
analyzer provided a fast response time and consistent results (Figure 5) during the
tests and is a good candidate for commercialization. In Figure 5 it can be seen that
the MCA (green line) followed quite well the laboratory water content analyses (red
□) and KF on-line water analyses (blue ◊). First the seed oil (older oil in condensers)
was replaced which can be seen as a decrease in water content. Then the water
content balanced to about 26 wt-%. Due to change of feedstock batch into a wetter
one, the moisture content started to increase. Around 30 – 35 wt-% water content,
inhomogeneous oil is produced and water contents vary until they balance again.
40
35
Moisture, wt%
KF
30
OLKF
MCA
25
20
16.3.10 12:00 18.3.10 0:00 19.3.10 12:00 21.3.10 0:00
Date & Time
Figure 5. MCA for in-line water content, results from the pilot plant
Particle sizing will be carried out using an on-line particle measurement system
developed by Pixact Ltd. Measurement will be based on the high-magnification
imaging of particles flowing through the measurement cell and an on-line image
analysis procedure. Furthermore, a special algorithm will be used to detect particles
in the images. In addition to size measurement, other properties such as shape
parameters can also be analyzed. VTT compared the results with a commercial
particle counter and a good correlation was obtained. These methods yield
reproducible results, but the data is qualitative and intended to register sudden
changes in solids concentrations. The results also correlated well with the actual
change in solids.
BIO-OIL COMBUSTION
UPM’s focus is on using bio-oil as a substitute for both light and heavy fuel oil in
heating and combined heat and power plants. Fortum is focusing on replacing heavy
fuel oil. Their previous combustion tests in 2002 - 2003 (2) showed promising results
in relation to combustion on a small scale (below 1 MW). Oilon has developed two
model burners for bio-oils.
Bio-oil was combusted in Fortum's 1,5 MW district heating plant in Masala, Finland.
Existing burner was changed to a new bio-oil burner, which is actually a modified
heavy fuel oil burner. Total amount of bio-oil combusted in spring 2010 was about
20 tons. One main focus area was overall functionality of bio-oil receiving, storing
and pumping system. Receiving system and oil tank were located outside the
building. System worked well despite the outside temperature which varied from -20
°C from +10 °C during test period.
Another focus was in burner function. As a result, good reliability and satisfactory
turn-down-ratio of 1:3 were gained. Flue gas emissions were close to those of heavy
fuel oil - with 4 % O2 CO emissions ranged from 0 to 10 ppm, and NOx from 300 to
400 ppm. Organic compounds were under 5 mg/m3n and particulate emission in
range of 150 - 200 mg/m3n.
A new test run in Fortum's district heating plant will be carried out in autumn 2010.
After demonstrating the replacement of heavy fuel oil use the focus of UPM will be in
light fuel oil replacement.
Based on the experiences, bio-oil is technically suitable for replacing heavy fuel oil
in district heating plants. Emissions (CO, NOx, particulate) were close to heavy fuel
oil. No significant odors were released in the neighborhood.
SUMMARY
A novel integrated pyrolysis pilot plant has been built to Finland by Metso, in co-
operation with UPM, Fortum and VTT. A 2 MW fuel (7 t oil/d) fast pyrolysis unit has
been integrated with Metso’s 4 MW th circulating fluidized bed boiler, located at
Metso’s R&D Center in Tampere, Finland.
Test runs of bio-oil production from forest residue chips and sawdust have been
carried out during 2009-2010. More than 80 tons of bio-oil has been produced and
utilization tests have been started in burner applications.
Quality control methods have been developed and hence water can be followed in-
line. On-line solids measurement is under testing.
The integration of the pyrolysis and combustion processes has been successful, and
the controllability of the integrated concept has been excellent.
ACKNOWLEDGEMENTS
At Metso Heikki Ikonen, Markku Toots, Antti Kaura and Jani Laine are
acknowledged. At VTT Sampo Ratinen, Pekka Saarimäki, Jaana Korhonen, Sirpa
Lehtinen, Anssi Källi, and Jouko Kukkonen are acknowledged.
NOTATION
FR = Forest residue
KF = Karl-Fischer laboratory titration
OLKF = On-line Karl-Fischer analyzer
MCA = Metso in-line analyzer
REFERENCES
(1) http://www.redarrowusa.com/redarrow.html
(2) Gust, S. (1997). Combustion of Pyrolysis Liquids. In: Biomass Gasification
and Pyrolysis, State of the Art and Future Prospects, Kaltschmitt, M.,
Bridgwater, A., (eds), CPL Press, Newbury, UK.
(3) Sipilä, E., Vasara, P., Sipilä, K., Solantausta, Y. (2007). Feasibility and
Market Potential of Pyrolysis Oils in the European Pulp and Paper Industry.
15th European Biomass Conference & Exhibition. Berlin, Germany, 7 - 11
May, 2007. ETA-WIP
HIGH-FLUX TRIPLE BED CIRCULATING FLUIDIZED BED
(TBCFB) GASIFIER FOR EXERGY RECUPERATIVE IGCC/IGFC
Chihiro Fushimi1*, Guoqing Guan1,2, Masanori Ishizuka1, Yu Nakamura1,

Atsushi Tsutsumi1, Yoshizo Suzuki3, Eldin Wee Chuan Lim4, Yongpan Cheng4,
Chi-Hwa Wang4
1
Collaborative Research Center for Energy Engineering, Institute of Industrial
Science, The University of Tokyo, 4-6-1 Komaba, Meguro, Tokyo, 153-8505,
Japan
2
NJRISE, Hirosaki University, Japan
3
Clean Gas Group, National Institute of Advanced Industrial Science and
Technology, 16-1 Onogawa, Tsukuba, Ibaraki 305-8569, Japan
4
Department of Chemical and Biomolecular Engineering, National University of
Singapore, 4 Engineering Drive 4, Singapore 117576
* fushimi@iis.u-tokyo.ac.jp, Tel: +81-3-5452-6293 Fax: +81-3-5452-6728
Abstract
The flow behavior of silica sand, of average particle size 128 μm, was investigated
using a large-scale triple-bed combined circulating fluidized bed (TBCFB) cold model,
which was composed of a 0.1 m I.D. ×16.6 m tall riser, a solids distributor, a 0.1m I.D.
× 6.5 m long downer, a gas-solids separator, a 0.75 m × 0.27 m × 3.4 m bubbling
fluidized bed and a 0.158 m I.D. × 5.0 m tall gas-sealing bed (GSB) with a high solids
mass flux. The main focus of this study is to determine effect of riser secondary air
injection on solids mass flux (Gs) and solid holdup. Gs slightly increased by
secondary air injection when the riser gas velocity (Ugr) was less than 10 m/s. This
was caused by the increase in the pressure difference between the GSB and the
riser. Secondary air injection had little influence on the solid holdup in the riser. The
mixing between silica sand and coal particles was investigated for two different coal
feeding arrangements by coupling Computational Fluid Dynamics (CFD) with the
Discrete Element Method (DEM). The results show a tangential arrangement
provided better mixing than a normal arrangement except near the entrance.
INTRODUCTION
Coal utilization is one of the major contributors of anthropogenic CO2 and pollutants
emission. Clean Coal Technology (CCT) has been under development to find ways
for more efficient utilization of coal. So far, Integrated coal Gasification Combined
Cycle (IGCC) and Integrated coal Gasification Fuel-cell Combined cycle (IGFC) have
been developed to increase the thermal efficiency of coal-fired power plants.
For improvement of the thermal efficiency of coal-fired IGCC/IGFC, an advanced

IGCC (A-IGCC) or advanced IGFC (A-IGFC) system with exergy recuperation was
proposed (1,2). In this system, the waste heat from a gas turbine or solid oxide fuel
cell is recuperated as a heat source for steam gasification of coal to reduce the
partial combustion of coal. Because the reaction temperature for gasification is
expected to be 700-900 °C, which is not suitable for conventional entrained bed
gasifiers, a novel triple-bed combined circulating fluidized bed (TBCFB) gasifier was
proposed (3-5). The TBCFB is composed of a downer pyrolyzer, a bubbling fluidized
bed (BFB) char gasifier, and a riser partial combustor of unreacted char. The heat
generated in the riser partial combustor is supplied to the downer pyrolyzer for the
endothermic reaction by using a heat media such as silica sand (3-5). According to
the mass and energy balance calculation for the system (2,6), the solids mass flux
(Gs) of the heat media should be 511 to 684 kg/(m2•s), which is much higher than in a
conventional CFB (7-10) to make the A-IGCC/IGFC system feasible.
Besides the requirement for a high solids flux of the heat media, the mixing behavior
between the heat media and reactant, i.e. silica sand and coal, is also critical. Since
the residence time of the solid particles in the downer is usually quite short, the heat
carried by the silica sand needs to be effectively transferred to the coal for pyrolysis.
In this study, a preliminary investigation was carried out to study the mixing behavior
between sand and coal particles by numerical simulation.
In our previous study (5), we set up a large-scale TBCFB gasifier cold model and
investigated flow behavior of the sand particles. The maximum obtained Gs was over
400 kg/(m2•s) when the riser gas velocity (Ugr) was 12 m/s, and the average solid
holdup in the bottom dense region of 0.110 to 0.122 at Gs=377 to 410 kg/(m2•s) was
achieved by installing a gas-sealing bed (GSB) between the riser and BFB. However,
it was observed that some amount of air passed from the riser bottom to the GSB
bottom when the riser gas velocity was high. Thus, in this study, some amount of
riser gas was injected in the second nozzle 1.9 m above the riser bottom and the
influence of the secondary air on Gs and solids holdup was investigated.
EXPERIMENT AND SIMULATION
Experimental
Figure 1 shows a schematic image of the
large scale TBCFB cold model, which is
composed of a riser (0.1 m I.D. × 16.6 m),
a solid distributor for downer, a downer
(0.1 m I.D. × 6.5 m), a gas-solid separator
and a BFB (0.75 × 0.27 × 3.4 m3). Sand
particles with a density of 2600 kg/m3 and
an arithmetic average particle size of 128
μm (minimum fluidization velocity was
0.0074 m/s) were used as bed material. To
increase the driving force to transport a
large amount of particles from the BFB Figure 1 Experimental apparatus (5)
into the riser bottom, a gas-sealing solids
bed (0.158 m I.D. × 5.0 m) was installed. The sand particles overflowed from the BFB
were transported to the GSB through an inclined tube. The sand particles were
fluidized by air in the GSB and transported to the riser bottom. The bed height in the
GSB was 4.0 m. At the top of the riser, the solids passed through a smooth elbow into
cyclone 1 for gas-solids separation, and some small solids were collected by
cyclones 2 and 3, and returned to the dipleg of cyclone 1. At the top of the downer,
the solids were redistributed by a solids distributor with 13 vertically positioned brass
tubes with a diameter of 19 mm using an air assist. The air was introduced into the
downer at the entrance of the downer and the solids and air flowed downwardly. At
the end of the downer, the solids were separated from the air by a separator and
passed to the BFB. The solids entrained by the gas were collected by a cyclone and
returned to the BFB. For the seal between the downer and the BFB, a seal tube (0.15
m I.D. × 1.0 m long) was inserted into the BFB. In this study, the superficial gas
velocity of the riser was changed in two ways: i) the air was fed from the bottom of
the riser at a volumetric rate to give 6 to 12 m/s in the riser without secondary air
injection, ii) the air fed from the bottom of the riser was fixed at volumetric rate to give
6 m/s in the riser and secondary air was fed at the nozzles located 1.9 m above the
riser bottom at a volumetric rate to give 0 to 6 m/s in the riser. The superficial gas
velocity in the GSB and BFB were fixed at 0.10 and 0.025 m/s, respectively. Static
pressures were measured at 47 pressure taps around the unit using differential
pressure sensors (Keyence Corp., AP48). The output signals from the sensors were
acquired at a sampling frequency of 100 Hz via a data logger (CONTEC,
AIO-163202FX) and a laptop computer. Solids mass flux (Gs) was measured by
closing a butterfly valve below the cyclone 1 and measuring the time to accumulate
given amounts of particles. This was determined from the mean value after 10
measurements at a steady state.
Simulation
The commercially available CFD code
FLUENT (Ansys, Inc) and a Discrete
Element Method (DEM) based code
EDEM (DEM-Solutions Ltd) were used to
(a) Normal (b) Tangential
study the dynamics of coal and sand
Figure 2 Arrangements of 4 nozzles
particles in the downer. The air flow was
for coal feeding
solved by FLUENT using an Eulerian
approach, and particle motion was computed by EDEM using a Lagrangian approach.
At every time step the two methods were coupled such that interactions between gas
and solid particles were handled rigorously. Due to CPU and memory limitations,
simulations were carried out for sand particles 4 mm in diameter and coal particles 6
mm in diameter in a downer of 2 m in length. The other geometrical dimensions were
the same as those in the experimental setup.
The basic equations for air flow in the downer are the continuity and momentum
equations (11)
  
    u   0
t (1)
  u 
    uu   p  2u   g  S (2)
t
where  is the air volume fraction, g is the gravity force vector, S is the momentum
sink and the coupling between the gas and solid phases is achieved through the
calculation of the momentum sink of the drag force that arises due to the slip velocity
between the phases. The momentum sink S is calculated by: S 

F D
, where
V
V is the volume of a CFD mesh cell, and FD is the summation of the drag force
exerted on the fluid in the mesh cell. The free stream drag model adopted was
FD  0.5CD  A v v
(3)
where the drag coefficient CD depends on the Reynolds number (11)
 d pvr (4)
Re p 

 24
 Re Re p  0.5
 p

CD  24 1.0  0.15 Re0.687
p  / Rep 0.5  Re p  1000
 (5)
 0.44 Re p  1000

The sand particles were fed into the downer through 13 tubes in the distributor, and
two nozzle arrangements were designed to feed coal into the downer, as shown in
Fig.2. The four feeding nozzles were all horizontal. One arrangement was that all the
four nozzles were normal to the downer, and the other arrangement was that all four
nozzles were tangential to the downer. The uniform inlet velocity for the nozzle was
20 m/s, the standard k ~  turbulent model was adopted.

Effect of secondary air injection on
Gs
Figures 3 and 4 show the solids mass
flux (Gs) and the pressure difference
between the GSB and riser bottom as a
function of riser gas velocity (Ugr),
respectively. Note that Ugr was defined
as the sum of air fed from the riser
bottom and the secondary injection
nozzle divided by the cross section of Figure 3 Relationship between riser gas
the riser. When no secondary air was velocity (Ugr) and solid mass flux (Gs)
injected, Gs monotonically increased
with the increase in Ugr. The maximum Gs obtained was 433 kg/(m2•s) at Ugr =12 m/s.
When secondary air was injected, Gs peaked at 451 kg/(m2•s) at Ugr =10 m/s (i.e. 6
m/s was fed from the bottom and 4 m/s was fed from the nozzle). Further increases
in Ugr decreased Gs. Compared with
the results without secondary air
injection, the Gs was slightly larger at
Ugr ≤ 10 m/s. However, the influence
of secondary air injection was not
significant at velocities Ugr ≥ 11 m/s.
It can be seen in Figure 4 the
pressure difference between the
GSB and riser bottom, which is a Figure 4 Relationship between riser gas
major driving force to transport solids velocity and pressure difference between
to riser, became larger when GSB bottom and riser bottom
secondary air injection was used.
Thus, it can be said secondary air injection is an effective way to increase Gs when
the total Ugr is not high.
Effect of secondary air injection on solids holdup along riser

The influence of secondary air injection on riser solids holdup was also studied.
Figure 5 shows the apparent solids holdups (εs) along riser calculated by the
following equation;
16
ΔP/ΔH=ρpεsg (6)
2nd 2 m/s (total 8 m/s)
where ΔP [Pa], ΔH [m], ρp [kg/m3], εs [-] and g 14
[m/s2] mean pressure difference, the distance 12 2nd 0 m/s (total 6 m/s)
Height from riser bottom [ m ]

between the two sensors, particle density, solids 10 2nd 0 m/s (total 10 m/s)
holdup and the gravitational acceleration, 8
respectively. The open and closed symbols 6
represent the results with and without secondary 4
air injection, respectively. εs decreased sharply at 2
the bottom part of the riser (Hr < 5 m) and 0
gradually decreased at the middle and top of the 0 0.05 0.1

Solids holdup [ - ]
0.15 0.2 0.25
riser (Hr ≥ 5 m). The solids holdup decreased in Figure 5 Solids holdup along riser
the riser as Ugr increased. When Ugr was 10-12
m/s, the εs was almost constant (around 0.02) at Hr ≥ 5 m. The results indicate the
formation of dense phase at Hr < 5 m and lean phase at Hr ≥ 5 m. By comparing the
results with and without secondary air injection at each Ugr, a slight increase in εs was
observed at bottom dense part (Hr < 5 m). However, no significant difference of εs
was observed at middle and top part (Hr ≥ 5 m). This indicated that secondary air
injection did not significantly increase solids holdup along riser.
Simulation results
Figure 6 shows the mixing behavior
between sand particles (dark) and coal
particles (light). It can be seen that near
the entrance, the tangential arrangement
resulted in a poorer mixing performance
than the normal arrangement. This is
because in the normal arrangement, (a) Normal (b) Tangential
strong collisions between the normally Figure 6 Mixing behaviors for the
injected coal particles and the falling two types of nozzle arrangements
sand particles occurred. In contrast, in the tangential arrangement, the coal particles
had a tendency to move spirally along the walls of the downer while most of the sand
particles moved downwards along the center of downer. This resulted in less mixing
between the coal and sand particles in the latter case. But downstream, the sand and
coal particles are distributed more uniformly in the radial direction when the
tangential arrangement was used than when the normal arrangement was used,
which means the tangential arrangement gave better mixing than the normal
arrangement downstream of the feeder.
The mixing of coal and sand particles depends on several parameters, such as
particle diameters, inlet velocity, downer diameter and solids mass flux. A sensitivity
analysis of these parameters on the mixing is still under study. Also, the mixing
content will be quantified and a suitable mixing index will be developed.
CONCLUSIONS
1) Secondary air injection slightly increases solid mass flux (Gs) at a riser gas velocity
≤ 9 m/s. This is thought to due to the increase in the pressure difference between the
GSB and the riser bottom, which is the main driving force to transport solids.
2) The injection of secondary air does not affect solids holdup along riser.
3) The tangential arrangement of nozzles for feeding coal particles into the downer
provided better mixing between coal and sand particles except near the entrance.
ACKNOWLEDGEMENT
This study was supported by the New Energy and Industrial Technology
Development Organization (NEDO), Japan and the Economic Development Board
Singapore under grant number R261-501-003-414 (Minerals, Metals and Materials
Technology Center, National University of Singapore)
REFERENCES
1) A. Tsutsumi, Advanced IGCC/IGFC using exergy recuperation technology, Clean
Coal Technol. J. (in Japanese) 11 (2004) 17-22.
2) J.-i. Hayashi, S. Hosokai, N. Sonoyama, Gasification of low-rank solid fuels with
thermochemical energy recuperation for hydrogen production, Trans. IChem E: Part
B 84, (2006) 409-419.
3) G. Guan, C. Fushimi, M. Ikeda, Y. Nakamura, A. Tsutsumi, T. Suda, M. Ishizuka, H.
Hatano, S. Matsuda, Y. Suzuki, Flow behaviors in a high solid flux circulating fluidized
bed composed of a riser, a downer and a bubbling fluidized bed, Fluidization XIII
407-414 (2010)
4) G. Guan, C. Fushimi, A. Tsutsumi, Prediction of flow behavior of the riser in a novel
high solids flux circulating fluidized beds for steam gasification of coal or biomass,
Chem. Eng. J. 164 (2010) 221-229.
5) C. Fushimi, G. Guan, Y. Nakamura, M. Ishizuka, A. Tsutsumi, S. Matsuda, H.
Hatano, Y. Suzuki, Hydrodynamic characteristics of a large-scale triple-bed
combined circulating fluidized bed, Powder Technol. (accepted)
6) X.T. Bi, X. Liu, High density and high solids flux CFB risers for steam gasification
of solids fuels, Fuel Process. Technol. 91 (2010) 915-920.
7) X. Liu, X. Cui, G. Sun, F. Sun, T. Suda, G. Xu, High solid-flux concurrent conveying
flow-realized by coupling a moving bed to the bottom section of a riser, Ind. Eng.
Chem. Res. 47 (2008) 9703-9708.
8) X. Liu, X. Cui, G. Sun, T. Suda, M. Narukawa, Y. Liu, G. Sun, G. Xu, Buildup of high
solids flux conveying flow by coupling a moving bed to the riser bottom, AIChE J. 55
(2009) 2477-2481.
9) X.-B. Qi, J. Zhu, X. Huang, A new correlation for predicting solids concentration in
the fully developed zone of circulating fluidized bed risers, Powder Technol. 188
(2008) 64-72.
10) X. Wang, B. Jin, W. Zhong, M. Zhang, Y. Huang, F. Duan, Flow behaviors in a
high-flux circulating fluidized bed, Int. J. Chem. Reac. Eng. 6 (2008) A79.
11) User Guide, EDEM-CFD coupling module for FLUENT, (2010).
HYDRODYNAMICS OF CONICAL SPOUTED BEDS WITH HIGH
DENSITY PARTICLES
Salih Sari1, Aylin Polat2, Dogukan Zaglanmis1, Gorkem Kulah2,*, Murat Koksal3,*
1
Dept. of Nuclear Eng., Hacettepe University, Beytepe, 06800, Ankara, Turkey
2
Dept. of Chemical Eng., Middle East Technical University, 06531, Ankara, Turkey
3
Dept. of Mechanical Eng., Hacettepe University, Beytepe, 06800, Ankara, Turkey
*
Corresponding authors: gorkemk@metu.edu.tr, koksalm@hacettepe.edu.tr
ABSTRACT
An extensive experimental investigation of conical spouted beds with high density

particles were carried out by measuring bed pressure drop, particle velocity and
solids hold-up in a 15 cm ID conical spouted bed at three different cone angles (30°,
45°, 60°) with Yttria-stabilized zirconia (YSZ) particles (ρp = 6050 kg/m3). The results
show that the minimum external spouting velocity increases with cone angle, particle
diameter and static bed height. The bed is characterized by two regions: upward
moving particles with high slip in the spout and slowly downward moving particles at
loosely packed conditions in the annulus.
INTRODUCTION
Due to its unique solids circulation characteristics and excellent gas-particle contact,
spouted beds have wide range of applications in many industrial processes like
drying, granulation and particle coating. One of the particle coating applications of
the spouted beds is the chemical vapor deposition (CVD) coating of uranium dioxide
kernels with pyrolytic carbon and silicon carbide to produce spherical fuel elements
(known also as TRISO type fuel element) for high temperature gas cooled reactors
(HTR) (1). HTR is an advanced reactor technology (still under development)
recognized for its inherent safety, high fuel utilization and high efficiency in electricity
generation with cogeneration possibilities. Currently, the fuel production for the
prototypes of HTR technology is realized in small scale spouted bed coaters with
limited capacity. Once the full scale reactors are in operation, there will be a huge
need for large scale fuel coaters with mass production capability. To design, scale
up and manufacture spouted bed coaters operating with heavy particles, it is of
fundamental importance to have a detailed understanding of the hydrodynamics of
the system. Although there are a considerable number of hydrodynamic studies
published in the literature, a very limited number of these have been conducted in
spouted beds operating with heavy particles (ρp > 2500 kg/m3) typically encountered
in CVD coating of nuclear fuels.
To the authors' knowledge, the most comprehensive study on the hydrodynamic

behavior of spouted beds with high density particles is a Ph.D. dissertation from the
University of Tennessee (2). In this work, the minimum spouting velocity, time-
averaged and dynamic pressure drops, time-averaged fountain height and gas
velocity profiles were measured in a 5 cm ID conical spouted bed at different cone
angles (45°,60°,75°) operating with Yttria-stabilized zirconia (YSZ) particles (ZrO2,
also known as zirconia) having a particle density of 6050 kg/m3. Effects of the static
bed height and particle size on measurements were investigated and new
correlations for minimum spouting velocity, time-average pressure drop and fountain
height based on the experimental data were developed. An unpublished final project
report by a group of University Tennessee researchers is also available in the open
literature (3). In this report, Zhou’s (2) work has been further extended with bed
pressure drop, pressure fluctuations and fountain height measurements carried out
with alumina particles in a 5 cm ID spouted bed for the aim of developing
hydrodynamic scaling relationships.
On the computational side, Pannala et al. (4) performed a 2-D Eulerian-Eulerian

simulation of a 5 cm ID spouted bed with zirconia particles using MFIX (Multiphase
Flow with Interphase Exchanges) code. Centerline axial velocity and Fourier spectra
of pressure fluctuations were compared with corresponding experimental data. Their
simulations revealed an interesting dynamic behavior - occurrence of regular
spontaneous pulsations of gas and particle flow in the spout - which was also
observed by Zhou (2).
All of the aforementioned studies were performed in a 5 cm ID, conical spouted bed.
However, to have a comprehensive understanding of the hydrodynamics of CVD
fuel coaters for HTR reactors, further investigations need to be carried in larger inner
diameter spouted beds. In addition, complete characterization of the hydrodynamics
should also involve the determination of voidage and solids velocity inside the
system. Therefore, the objective of this study was to investigate the hydrodynamic
characteristics of spouted bed nuclear fuel coaters at cold bed conditions. To
achieve this objective, experiments were performed in a 15 cm ID conical spouted
bed at different static bed heights and cone angles (30°, 45°, 60°) with zirconia
particles (dp = 0.5, 1 mm; ρp = 6050 kg/m3) to simulate the particle properties in hot
bed conditions. Bed pressure drop and its fluctuations were measured to determine
the minimum external spouting velocity. Local instantaneous particle velocities and
solids hold-ups were also measured by an optical fiber probe to better understand
the gas-solid dynamics in the spouted bed.
EXPERIMENTAL SET-UP
The experimental study was carried out in three full circular conical spouted beds
made of Polyoxymethylene (also known as Delrin) which is an excellent
thermoplastic that can withstand the continuous impact of hard zirconia particles
without significant erosion. A schematic diagram of the units is given in Fig. 1 and
their geometric parameters and operating conditions are presented in Table 1.
Spherical Yttria-stabilized zirconia (YSZ) particles (dp = 0.5, 1 mm; ρp = 6050 kg/m3)
were used to simulate the particle properties in hot bed conditions and compressed
air at ambient temperature was used as the spouting gas. The total pressure drop
across the spouted bed was measured by a differential pressure transducer (Omega
PX142-005D5V) connected to the bed internal wall at the base of the conical
section. The other line of the transducer was open to atmosphere. The data was fed
to a computer by a high speed data acquisition board (National Instruments PCI-
6280) and processed using LabVIEW version 8. The sampling was performed at a
frequency of 1 kHz for 20 seconds. Each measurement was repeated for three times
and the corresponding averages are reported. To eliminate the possible effects of
the initial packing status on the measurements, following the approach proposed by
Wang (5), the spouted beds were operated for 1 hour prior to each experimental
run.
Figure 1. Geometric sketch of conical spouted beds.
Table 1. Geometric parameters of the spouted beds and experimental operating

conditions.
Data Sets γ d p (mm) Di (mm) Do (mm) Dc (mm) Hc (mm) Hb (mm)

1 0.5 100
60 25 15 150 108
2 1 100
3 0.5 100
4 45 1 25 15 150 151 100
5 1 140
6 0.5 100
7 1 100
8 30 1 25 15 150 233 140
9 1 180
10 1 220
A multi-fiber optical probe, PV-6, developed by the Institute of Process Engineering,

Chinese Academy of Sciences, was used to measure simultaneously local
instantaneous particle velocities and solids volume concentrations. The probe
consists of two bundles of optical fibers. Inside each bundle, there are alternating
arrays of light emitting and receiving fibers. The fibers have a uniform diameter of 15
μm. Light was projected into multiphase suspension through the emitting fibers. The
backscattered light from the particles were transmitted by the receiving fibers to two
photomultipliers, one for each bundle, and was converted to voltage signal. The
signals were digitized by the high speed data acquisition board and processed by
using LabVIEW version 8. If the flow structure does not change between these two
bundles and the particles move in the same direction, the two signals would be
identical, but separated by a time delay, τ. This time delay, which was obtained by
cross-correlating the two signals, was used to calculate the axial particle velocity in
Eq. (1):
L
Up = e (1)
τ
where Le is the effective distance between the two bundles. In this study, Le was
determined to be 2.11 mm through the calibration studies performed with rotating
disks with different designs and rotating disks with particles glued. Since the particle
velocity changed significantly in different radial locations of the spouted bed, the
sampling frequency and time had to be varied correspondingly. For each
measurement, a total of 180,000-500,000 data were collected through each bundle
with a sampling frequency of 1-100 kHz. During the particle velocity measurements,
particles may reverse directions, or a flow structure travelling non-vertically passing
one bundle may not be detected by the second one, causing the cross-correlation
coefficients to be low or indeterminate. Such uncorrelatable or poorly correlated data
need to be eliminated. In this study, following the approach proposed by Kirbas et al.
(6), in order for the results to be acceptable, the correlation coefficients were
required to exceed 0.7, and individual calculated velocities were required to differ by
no more than 3 standard deviations from the average.
The optical fiber probe was capable of simultaneously measuring solids

concentration together with particle velocity. The same data used in the calculation
of particle velocity was integrated over time and by utilizing a calibration equation,
solid hold ups were calculated. Before experiments, the probe was calibrated by
using original+black colored zirconium particle mixtures. For this purpose, different
concentration mixtures were prepared by combining known masses of original
zirconium particles and black color painted zirconium particles. Since the painted
zirconium particles were black and therefore absorbed most visible light, it was
assumed that they behaved as voids, while only original particles reflected light. The
calibration was performed in a system similar to the one described in (7). Using
different concentration mixtures, solids hold ups were simulated. A linear
relationship was observed between the voltage and solids hold-up.
Local instantaneous particle velocities and solids hold ups were measured at
several radial positions and three heights in the spouted bed with a cone angle, γ, of
45° operating at 1.25 Ums.

Bed Pressure Drop Measurements
Effects of ascending and descending inlet gas velocity, static bed height, particle
diameter and cone angle on bed pressure drop were investigated in this study.
Besides, the inlet gas velocity at which the external spouting begins (denoted by
Ums) at each case were visually determined and indicated on relevant pressure drop
figures with corresponding arrows.
The effect of the ascending and descending inlet gas velocity, Uo, on the bed
pressure drop in the bed is shown in Fig. 2 (Data set 4 in Table 1). The inlet gas
velocity, Uo, is simply the superficial gas velocity based on Do. The descending
velocity case does not show a steep peak as in the case of ascending velocity
although the average pressure drop after the external spouting begins is the same.
Furthermore, the external spouting is observed at the exact same velocity for both
cases. The peak observed for the ascending velocity case is attributed to resistance
that needs to be overcome as the internal spout first forms at the bottom of the bed.
Fig. 3 shows the effect of the cone angle on the bed pressure drop (Data sets 2, 4
and 7 in Table 1). The figure shows that the minimum external spouting velocity
increases as the cone angle increases. As the bed wall becomes more horizontal
with increasing cone angle, it becomes more difficult to move particles downward
near the wall and in turn a higher velocity is needed to create a spout at the center
and establish a circulation pattern typically observed in spouted beds. The same
trend is also obtained for the inlet gas velocity at which the pressure peak is
observed. Hence, the pressure drop curve shifts to the left as the cone angle
increases. Increasing the cone angle also decreases the average bed pressure drop
after the external spouting since the weight of the particles is carried more and more
by the wall.
Fig. 4 shows the effect of particle diameter on the bed pressure drop (Data sets 1
and 2 in Table 1). The minimum external spouting velocity increases with particle
diameter. The effect of the static bed height on the bed pressure drop is shown in
Fig. 5 (Data sets 7, 8, 9, 10 in Table 1). The bed pressure drop increases with static
bed height. Both trends observed in Figs. 4 and 5 are consistent with literature.
Fig. 6 shows a complete picture of the effect of the static bed height and cone angle
on the minimum external spouting velocity. The minimum external spouting velocity
increases linearly with static bed height for all cone angles tested in this work.
Radial Particle Velocity and Solids Hold Up Measurements
The local particle velocities and solids-hold-ups measured in the spouted bed with a
cone angle of 45° operating at Uo = 56.3 m/s (1.25Ums) with a bed pressure drop of
3054 Pa are illustrated in Figure 7 (Data set 5 in Table 1).
As depicted in this figure, the spouted bed is made up of two distinct regions: spout
and annulus. A high velocity gas (56.3 m/s) enters the bed and the particles are
carried up in the spout. It is interesting to note that at z = 42 mm, the local particle
velocity at the axis is around 2.5 m/s indicating a large slip between gas and
particles. In the annulus, the particles falling down from the fountain move slowly
downwards with particle velocities of approximately -0.003 m/s. The particle velocity
at any axial location decreases from its maximum value at the axis to zero at the
spout-annulus interface. When the evolution of spout diameter is monitored, it is
observed that at the two axial locations above the entrance, the spout has a
diameter of approximately 17 mm which is close to the value of the inlet diameter of
the spouted bed (Do = 15 mm). The spout then starts widening up and its diameter
becomes approximately 21 mm at the highest measurement level (z = 120 mm).
When the solids hold up profiles are examined it is observed that in the spout solids
hold up is much lower compared to the annulus where particles are in close contact
with each other and the solids fraction is uniform and almost equal to the loosely
packed solids hold up at all levels. The solids hold up increases sharply at the
interface between the spout and the annular zones.
γ=60⁰
Ascending 5000 γ=45⁰
5000 Descending 4500 γ=30⁰
Bed Pressure Drop (Pa)

4500 Ums,30⁰
Ums,45⁰ 4000 Ums,45⁰

4000
3500 Ums,60⁰
3500
3000
3000
2500 2500
2000 2000
1500 1500
1000 1000
500 500
0 0
0 10 20 30 40 50 60 70 80 90 0 10 20 30 40 50 60 70 80 90
Inlet Air Velocity (m/s) Inlet Air Velocity (m/s)
Figure 2. Effect of ascending and descending inlet gas velocity on Figure 3. Effect of cone angle on the bed pressure drop.
the bed pressure drop.
18000 Hb=100 mm
5000 dp=1 mm 16000 Hb=140 mm

4500 dp=0.5 mm 14000 Hb=180 mm

4000 Ums,1mm Hb=220 mm
12000
3500 Ums,0.5 mm 10000
3000
2500 8000
2000 6000
1500 4000
1000 2000
500 0
0
0 10 20 30 40 50 60 70 80 90
0 10 20 30 40 50 60 70 80 90 Inlet Air Velocity (m/s)
Inlet Air Velocity (m/s)
Figure 5. Effect of the static bed height on the bed pressure
Figure 4. Effect of the particle diameter on the bed pressure drop. drop.
60
Min. Ext. Spouting Velocity

γ=30⁰, dp=1 mm
50 γ=45⁰, dp=1 mm
γ=60⁰, dp=1 mm
γ=30⁰, dp=0.5 mm
40 γ=45⁰, dp=0.5 mm
γ=60⁰, dp=0.5 mm
(m/s) 30
20
10
0
0 20 40 60 80 100 120 140 160 180
Static Bed Height (mm)
Figure 6. Effect of the static bed height on the minimum external spouting velocity.
3.0
2.5 z=42 mm
z=82 mm
2.0
Particle Velocity
z=120 mm
1.5
(m/s)
1.0
0.5
0.0
-0.5 0 10 20 30 40 50 60
-1.0
0.6
0.5
Solids Hold-up
0.4
0.3
0.2
0.1
0.0
0 10 20 30 40 50 60
r (mm)
Figure 7. Radial profiles of local time-mean particle velocities and solids hold-up
at different axial locations.
CONCLUSIONS
The purpose of this study was to understand the hydrodynamic characteristics of
spouted bed nuclear fuel coaters. Experiments were performed in a 15 cm ID
conical spouted bed at different static bed heights and cone angles (30°, 45°, 60°)
with zirconia particles (dp = 0.5, 1 mm; ρp = 6050 kg/m3) to simulate the particle
properties in hot bed conditions. Bed pressure drop, local instantaneous particle
velocities and solids hold-ups were measured. The main conclusions are
summarized below:
• The minimum external spouting velocity increases with cone angle, particle
diameter and static bed height.
• The average bed pressure drop decreases with cone angle.
• A very large slip is obtained between gas and particle velocities in the spout
region. The spout widens with height. At the axis, the particle velocity decreases
from 2.5 m/s to 1.6 m/s, whereas the solids hold up increases from 0.08 to 0.20
with height.
• The solids hold up increases sharply at the interface between the spout and the
annular zones. The annulus is characterized by slowly downward moving
particles with velocities of approximately -0.003 m/s at almost loosely packed
conditions.
ACKNOWLEDGEMENT
This work was carried out with the financial support of the Scientific and
Technological Research Council of Turkey (Project No: MAG 108M435).
NOTATION
γ Angle of the conical section, degree
ρp Particle density, kg/m3
τ Delay time between two signals from two light receivers, sec
dp Particle diameter, mm
Di ,Do ,Dc Diameter of the bed bottom, gas inlet, column, respectively, mm
Hc ,Hb Height of the conical section, static bed, respectively, mm
Le Effective distance between two bundles of optical fibers, mm
r Radial distance from the bed axis, mm
Ums ,Up ,Uo Min. external spouting velocity, particle velocity, inlet gas velocity, m/s
z Axial location, mm
REFERENCES
1. Vahlas, C., Caussat, B., Serp, P., Angelopoulos, G.N., “Principles and
applications of CVD powder technology”, Material Science and Engineering, 53,
1-72, (2006).
2. Zhou, J., “Characterizing and modeling the hydrodynamics of shallow spouted
beds”, Ph.D. dissertation, University of Tennessee, Knoxville, (2008).
3. Bruns, D., Counce, M. “Ambient laboratory coater for advanced gas reactor fuel
development”, Final Technical Report, Office of Scientific and Technical
Information, US Department of Energy, retrieved from
http://www.osti.gov/bridge/servlets/purl/981929-H1FgNA/981929.pdf, (2010).
4. Pannala, S., Daw, C.S., Finney, C.E.A., Boyalakuntla, D., Syamlal, M., O’Brien,
T.J., “Simulating dynamics of spouted-bed nuclear fuel coaters”, Chemical Vapor
Deposition, 13, 481-490, (2007).
5. Wang, Z., “Experimental Studies and CFD Simulations of Conical Spouted Bed
Hydrodynamics”, Ph.D. Thesis, University of British Columbia, (2006).
6. Kirbas G., Kim S.W., Bi H.T., Lim C.J., Grace J. "Radial distribution of local
concentration-weighted particle velocities in high-density circulating fluidized
beds", Proc. Fluidization XII, Canada, 71-78 (2007).
7. Kirbas, G., “Solids motion and mixing in high-density circulating fluidized beds”,
Ph.D. Thesis, Department of Chemical and Biological Engineering, University of
British Columbia, Vancouver, Canada, (2004).
CIRCULATING FLUIDIZED BED COMBUSTION – BUILD-UP
AND VALIDATION OF A THREE-DIMENSIONAL MODEL
Marko Palonena, David Pallarèsb, Ville Ylä-Outinena, Anton Larssonb,

Jukka Lainec, Filip Johnssonb
a
Metso Power Oy, Lentokentänkatu 11, P.O. Box 109, FI-33101 Tampere, Finland
b
Chalmers University of Technology, S-41296 Göteborg, Sweden
c
Tampere University of Technology, P.O. Box 589, FI-33101 Tampere, Finland
ABSTRACT
This paper presents the validated simulation of a full-scale circulating fluidized bed
boiler as obtained via a comprehensive three-dimensional CFB process model. The
model is utilized in boiler design and scale-up as well as to study and optimize boiler
performance. Feedstock characterization tests, which are also presented, are used
to provide data for those parts of the process where up-to-date modeling is not fully
reliable, thus enabling the model to provide accurate results.
The overall model and its sub-models have been validated against data from
numerous experiments ranging from characterization tests at laboratory scale to
measurements in a 550 MWth CFB boiler. The paper exemplifies comparisons
between model results and experimental data, showing generally good agreement.
INTRODUCTION
Circulating fluidized bed combustion (CFBC) is a technology where combustion

takes place within a gas-solid suspension. CFBC offers many benefits over other
combustion technologies, among these fuel flexibility and relatively low emission
levels.
There is a need for comprehensive modeling of CFBC in order to support design

and scale-up of boilers. Despite the availability in the literature of sub-models for
specific phenomena in fluidized bed combustion, the need for an overall CFBC
model has been addressed by only a few works, the most relevant being the model
provided by Hyppänen et al. (1), Hannes (2), and Lücke (3).
Metso and Chalmers University of Technology have together developed a

comprehensive three-dimensional CFB process model (4, 5), which is an essential
part of the knowledge process for Metso CFB combustion technology (see Fig. 1).
The CFB process model is utilized in the boiler design process and scale-up as well
as to study and optimize boiler performance. Among the concrete applications are
evaluation of circulation material behavior and flow rates, assessment of combustion
characteristics, dimensioning of heat transfer surfaces, and optimization of the air
and fuel feeds. The model, also widely used in planning and post-processing in
experimental research campaigns, is capable of establishing the boundary
conditions for other calculation tools, such as water circulation, corrosion, and
emission models.
Fig. 1: Knowledge process of the Metso CFB combustion technology
Experimental data in large quantities have been used to verify the sub-models as
well as the overall model. The experimental research consisted of:
- Laboratory-scale characterization tests - Metso 4 MWth CFB
- Small-scale FB tube reactors - Chalmers 12 MWth CFB
- VTT Jyväskylä 100 kWth CFB - Full-scale CFB boilers up to 550 MWth
CFB PROCESS MODEL
The CFB process model is a combination of different validated submodels available

in literature (6-11) each focusing one key phenomenon in the CFB process. These
submodels contain as little empirical content as possible and are linked into an
overall model by exchanging data according to the overview shown in Fig. 2. The
input data need by the overall model is summarized in geometry of the unit,
operational conditions (gas and solids injections, pressure drop over the furnace and
waterwall temperature) and solids (including fuel) properties. As seen, some of the
submodels use experimental input data from feedstock characterization tests
(detailed below). Such tests are used instead of submodels where these would not
be reliable enough. The model starts with a transient modeling of the fluid dynamics
which accounts for the external actions taken to control the bed inventory
(i.e. discharge of bed material and addition of makeup material) and the attrition of
the solids, as detailed in (6). It is important to note that the solids inventory is
modeled and monitored over the whole circulating loop including also the cyclones,
downcomers and particle seals. These elements can contain significant fractions of
the total solids inventory in form of finer solids than those found in the furnace. To
account for the solids populating the return leg, a pressure balance over the
circulating loop has to be closed, as well explained in (8). From this, the steady-state
solids inventory in the unit is determined
and can be used as input for the
calculation of the steady-state fluid
dynamics describing both the gas and
solids flows as detailed in (7) and (8)
respectively. For this, the solids in the
furnace freeboard are divided into
superimposing (ballistic) cluster and
(core- annulus) disperse phases, each
characterized by a decay constant, as
detailed in (8). The gas flow is
described according to the potential
flow theory. The fluctuating nature of its
mixing originates from the bubble flow
in the dense bed and can be described
through the formulation of a series of
quasi-steady state pressure balances in
the dense bed, as given in detail in (7).
It is well known that fuel particles
undergo varying mixing behaviors as
they convert, due to the gradual
decreases of size and density. Thus, a
transient representation of the fuel
mixing in order to account for the
different mixing pattern of fresh fuel and
fuel close to burn-out is needed. This is
Fig. 2: Overall model structure done in combination with a fuel particle
conversion model, as described in (9).
The conversion fate of a batch of fresh fuel is modeled on a time-resolved basis,
and the solution obtained is then recalculated into a sum of continuously fed batches
yielding the solution corresponding to the continuous feeding case. Finally, heat
transfer is modeled by separating convection and radiation mechanisms and using
individual heat transfer coefficients for convection and radiation, see (10), instead of
a lumped coefficient accounting for both mechanisms (as usually is the case in
works facing the modeling of the heat transfer in CFB units). This separate
treatment of convection and radiation sets a basis for accurate descriptions of each
mechanism (e.g. shadowing factors due to gas-solids suspension, internal heat
exchanging surfaces such as division walls and wing walls, varying suspension
emissivity and local convection peaks in furnace). A very first origin of this overall
model is found in an EU-funded project (11).
FEEDSTOCK CHARACTERIZATION
Conventional laboratory analyses are a starting point for basic balance calculations,
but, in addition, more detailed information is needed for modeling purposes. Feed
material characteristics, including the fuel fragmentation and attrition characteristics
of solids generating the circulation material, must be taken into account because of
their significant influence – in combination with boiler design and the operation
parameters – on the CFB process.
Attrition of Solids
As a result of the strong influence of the particulate phase in the heat and mass
transfer of in-furnace processes in CFB boilers, characterization of the solids
inventory is a crucial element in modeling. Attrition of different feed solid fractions
and their capability to generate circulation material, along with cyclone separation
efficiency, have a direct effect on the performance of a CFB boiler.
The experimental characterization of the attrition pattern for feed materials is carried
out in a small bench-scale setup wherein the solids sample undergoes attrition for a
set amount of time. The result for a certain fuel ash is illustrated in Fig. 3, which
shows the cumulative mass size distribution of the fuel ash after different attrition
times expressed as a fraction of the total test time.
The duration of the test is in the range of hours, and the test is developed to provide
data used in the modeling of solids inventory as described in Reference 6. After
proper processing, the test result data describes which fraction of each size range
will be reduced by attrition to finer size grades in a certain time.
Production of fine material is found to be faster at the beginning of the test, which is
a typical finding for experimental investigations of attrition (12). The evolution of the
amount of solids having a particle size smaller than 400 µm and its fitted power law
function are presented in Fig. 3.
Fig. 3: Results from attrition testing for fuel ash
Rate of Fuel Conversion
The fuel conversion sub-model applied in the CFB process model is based on the
formulation originally developed by Palchonok (13) and improved by Thunman (14)
and Larsson (15). Fig. 4 schematizes the fluidized bed tube reactor developed to
validate the fuel conversion model. Full combustion is ensured by the secondary
gas, and fuel conversion is obtained from the time-resolved oxygen concentration in
gases exiting the reactor (Fig. 4).
In comparison of the model and measurement results, it becomes obvious that the
test method’s contribution to the dynamics of the oxygen measurement must be
accounted for. This is done by convolving the model’s output with a convolution
model designed for the test reactor used. The convolution model comprises three
factors affecting the result:
1) Release and combustion of volatiles
2) The duration of the gas transportation and the mixing effects along the
reactor before the gas is detected by the oxygen sensor
3) The contribution of the analyzer response time, which is described by the
analyzer time constant analyzer time constant
10
8
Model + Convolution
O2 fraction (vol-%)
Measurement
6
0
0 50 100 150 200 250
time(s)
a) Schematic of the FB tube reactor b) Dynamic O2 concentration during test
Fig. 4: Fuel reactivity test
Fuel Fragmentation
Fragmentation is the phenomenon by which fuel particles break into smaller ones
during their conversion. There are several types of fuel particle comminution:
primary, secondary, percolative fragmentation and attrition, which are involved in
different stages of combustion. Primary fragmentation occurs in the first stages of
combustion (particle heating, drying, and devolatilization) and is caused by intense
thermal shock and local internal overpressures when a fuel particle is fed into a
fluidized bed. Comprehensive research has been conducted on the fuel
comminution phenomenon from coals and low volatile fuels (16) to waste fuels (17).
However, the experimental methods used in these works are too laborious to be
adopted as routine procedure in the fuel characterization process.
A fragmentation test method based on fuel particle image analysis has been
developed. The fuel particle under analysis is placed in a furnace where the
radiative heat transfer to the particle is adjusted to be equivalent to the total heat
transfer in a fluidized bed environment. From a sequence of tests, the fragmentation
probability, time of fragmentation, and number and size of fragments can be
determined. This test method characterizes only primary fragmentation.
Figure 5 illustrates the particle recognition by digital image analysis of a fragmented

fuel particle and exemplifies with test results the change in particle size due to
fragmentation.
a) Optical
O image analysis of a fragmented
f fu
uel b)
b Average parrticle size afterr the test vs. in
nitial
partticle particle
p size
Fig. 5: Fuel fragmentation
n test results
FULL-SCALE CFB FIELD

D TESTS AND
A MODEL VALIDAT
TION
Tests were
w carried
d out in a 350
3 MWth C CFB boiler with
w
two cycllones comb busting petrroleum cokke. Both a sides
view of the boiler and
a the main measure ement locations
are showwn in Fig. 6.6 In total, 32 measurrement portts in
the furna
ace were us sed for mea asurement o of the main gas
components, temp peratures, and
a ures. Intensive
pressu
samplingg of feed materials, circulation material, and
ashes was
w conductted during th he campaig gn.
After seetting of thhe input da ata (geome etry, opera
ation
condition
ns, and solids propertie es – including results from
f
characteerization teests), the case can n be prop perly
modeled d. The calc culation meesh normally consists s of
50,000––300,000 he exahedral cells
c for moodeling of full-
scale CFFB units.
Even th hough the model con ntains the least poss sible
empiricaal content, some sub b-models a are based on
experimental corre elations. For example, parame eters
g heat tran
affecting nsfer, air an nd fuel fee
ed penetrattion,
dispersioon, and mixing of ga ases and fu uel have been
b
adjustedd to achiev ve satisfacctory agreement with the
measure ed data. These parame eters have been valida ated
against several exp periments, with
w differe ent boiler siz
zes,
Fig. 6: Boiler unit and main fuel mixttures, and lo
oad levels.
meaasurement locations
Temmperature and
a main gas
g concen ntration profiles were measured simultaneously
from
m 10 locatioons with sp
pecially desiigned probe es and a multi-channe el gas analy
yzer.
Measured and d modeled horizontal
h emperature and O2 pro
te ofiles above
e secondaryy air
leve
el are show wn in Fig. 7 (where results
r from
m wall layerrs are omittted). As se
een,
agrreement is satisfactoryy for both comparisons
c s, although the model overestima ates
O2 concentratiion in locattion close too the wall layers. Thiss is a conseequence off the
(no
on-accounte ed in the model)
m diffusion of volatile matter and charr from the wall
laye
ers to the co
ore region.
10
8
Temperature (K)
1000
O2 (vol-%)
6
4
500
2
0 0
5 5
0 0
x, (m) -4 x, (m) -4
-5 0 -2
-5 0 -2
4 2 y, (m) 4 2 y, (m)
a) Modeled and measured temperature b) Modeled and measured O2 concentration
Fig. 7: Furnace horizontal profiles above secondary air level
The vertical pressure profile in the furnace was measured by differential pressure
transmitters and is presented in Fig. 8 together with corresponding modeled data,
showing a very good agreement. Fig. 9 presents the modeled and measured
cumulative mass size distribution of furnace bottom ash. As observed, the model
predicts the presence of a significant mass fraction of particles finer than 100 μm in
the bottom ash. The reasons for this disagreement are most likely 1) the perfect
vertical mixing in the dense bed assumed in the modeling and 2) not accounting in
the model for the size segregation effect in the bottom ash cooler (where a
significant part of the finest particles are entrained back to the riser).
Fig. 8: Modeled and measured vertical Fig. 9: Modeled and measured bottom ash
pressure profile and solids density profile particle size distribution
CONCLUSIONS
Key features and validation of a new comprehensive model of CFB combustion are
presented. The model is formed by a combination of semi-empirical models
describing key phenomena in the CFB combustion process. The validated overall
model aims at being a tool for boiler design and scale-up as well as to study and
optimize boiler performance.
Accurate characterization of feed materials plays a critical role in the modeling. The
main feedstock characterization tests used in combination with the model are
described and examples are given.
NOTATION
dp particle diameter
REFERENCES
1. Hyppänen, T., Lee, Y. Y., and Rainio, A. (1991). A three-dimensional model for
circulating fluidized bed boilers. Proceedings of the 11th International
Conference on FBC.
2. Hannes, J. (1996). Mathematical modelling of circulating fluidized bed
combustion. City-Print Verlag GmbH.
3. Lücke, K. (2003). On the influence of mixing on the performance of large-scale
atmospheric circulating fluidized bed combustors. PhD thesis, Hamburg-Harburg
Technical University.
4. Pallarès, D. (2008). Fluidized bed combustion – modeling and mixing. PhD
thesis, Chalmers University of Technology, Gothenburg.
5. Pallarès, D., Johnsson, F., and Palonen, M. (2008). A comprehensive model of
CFB combustion. 9th International Conference on Circulating Fluidized Beds.
6. Pallarès, D., Johnsson, F., and Palonen, M. (2010). Modeling of the solids
inventory in CFB boilers. 13th International Conference on Fluidization.
7. Pallarès, D. and Johnsson, F. (2009). Dynamical modeling of the gas phase in
fluidized bed combustion – accounting for fluctuations. Proceedings of the 20th
International Conference on Fluidized Bed Combustion.
8. Pallarès, D. and Johnsson, F. (2006). Macroscopic modelling of fluid dynamics
in large-scale circulating fluidized beds. Progress in Energy and Combustion
Science, 32 (5–6), pp. 539–569.
9. Pallarès, D. and Johnsson, F. (2008). Modeling of fuel mixing in fluidized bed
combustors. Chemical Engineering Science, 63 (23), pp. 5663–5671.
10. Pallarès, D., Johnsson, F., and Palonen, M. (2011). Modeling and validation of
the heat transfer in the furnace of large-scale CFB boilers. Proceedings of the
10th International Conference on Circulating Fluidized Beds.
11. Zhang, W. et al. (2000). Final report of EU project JOR3CT980306.
12. Klett, C., Hartge, E.-U., and Werther, J. (2005). Time-dependent behavior of the
ash particle size distribution in a circulating fluidized bed system. Proceedings of
the Combustion Institute, 30 (2005), pp. 2947–2954.
13. Palchonok, G. (1998). Heat and mass transfer to a single particle in fluidized
bed. PhD thesis, Chalmers University of Technology, Gothenburg.
14. Thunman, H. (2001). Principles and models of solid fuel combustion. PhD thesis,
Chalmers University of Technology, Gothenburg.
15. Larsson, A., Pallarès, D., Neves, D., Seemann, M., and Thunman, H. (2010).
Zero-dimensional modeling of indirect fluidized bed gasification. 13th
International Conference on Fluidization.
16. Chirone, R., Massimilla, L., and Salatino, P. (1991). Comminution of carbons in
fluidized bed combustion. Progress in Energy and Combustion Science, 17 (4),
pp. 297–326.
17. Arena, U., Cammarota, A., and Mastellone, M. (1998). The phenomenology of
comminution in the fluidized bed combustion of packaging-derived fuels. Fuel,
77 (11), pp. 1185–1193.
EVALUATION OF A LAGRANGIAN DISCRETE PHASE
MODELING APPROACH FOR APPLICATION TO INDUSTRIAL
SCALE BUBBLING FLUIDIZED BEDS
S. Cloete†, S.T. Johansen†, M. Braun*, B. Popoff*, S. Amini†
† Flow
Technology research group, SINTEF Materials and Chemistry,
Richard Birkelands Vei 3, 7034 Trondheim, Norway
Shahriar.Amini@sintef.no
*Ansys Germany GmbH, Birkenweg 14a, D-64295 Darmstadt, Germany
ABSTRACT
Industrial scale bubbling fluidized bed simulations were carried out within the Kinetic
Theory of Granular Flows (KTGF). The KTGF was applied within two different
modelling frameworks, the traditional Two Fluid Model (TFM) and a new approach in
the form of the Dense Discrete Phase Model (DDPM), in order to identify any
differences in performance. Only the DDPM was able to attain fully grid independent
results for industrial scale 2D simulations. In fact, the performance was sufficiently
good to enable the completion of reasonably affordable full 3D simulations. These
simulations revealed some differences between 2D and 3D, but the global system
behaviour remained relatively similar. Comparisons to experimental pressure drop
data for both 2D and 3D simulations were acceptable.
INTRODUCTION
Grid independence behaviour of fluidized bed simulations depends primarily on the
resolution of meso-scale particle structures in the computational domain. In bubbling
beds these structures are realized as bubbles, while risers typically display the
formation of particle clusters. Within industrial scale fluidized bed systems, the
length scales on which these clusters occur generally requires a mesh size which is
too small to be realistically simulated with present computational capacities.
In order to address this challenge, substantial research effort has been invested into
filtered or ‘coarse graining’ approaches (1-5). These methods aim to model the
effects of particle structures so that they do not have to be directly resolved on a
very fine grid. The filtered approach holds great promise for industrial application
and has a solid fundamental basis, but after a decade of study is still said to be in its
infancy when reviewed for the highly sensitive Geldart A particle class (6). In order
to arrive at a complete predictive model for industrial reactors, these closures will
have to be extended to poly-dispersed particle systems and additional closures will
have to be formulated for reaction kinetics. It is therefore reasoned that it will be
many years before a sufficiently generic and reliable set of sub-grid closures will be
developed.
The alternative to the filtered approach is fully resolving all the particle structures on
a sufficiently fine computational grid. When using this approach, no modelling is
needed in addition to the standard Kinetic Theory of Granular Flows (KTGF). Using
the traditional Two Fluid Model (TFM), grid independent results cannot be attained
for industrial reactors, but an alternative modelling formulation, known as the Dense
Discrete Phase Model (DDPM), has been shown to display much improved grid
independence behaviour (7). This modelling approach will now be evaluated in an
industrial scale bubbling bed reactor without any sub-grid closures incorporated in
order to assess the degree to which it can improve grid independence behaviour.
1
SIMULATIONS
Model equations
Simulations will be carried out both with the TFM and the DDPM in order to compare
their grid independence behaviour. A summary of the TFM model equations for this
approach can be found in Taghipour et al. (8). The most important closure relations
employed was the modelling of the drag and solids viscosity according to Syamlal et
al. (9), the frictional viscosity according to Schaeffer (10), the solids pressure
according to Lun et al. (11) and the radial distribution function according to Ogawa
et al. (12). The granular temperature equation was only solved in its algebraic form,
thereby neglecting the contributions of convection and diffusion.
Due to its novelty, a more complete description of the DDPM will be provided here.
The DDPM is based on the standard Discrete Phase Modelling (DPM) approach
where parcels of particles are tracked through the domain in a Lagrangian
framework according to Newton’s laws of motion. In its standard form, the DPM
does not account for the volume fraction of the discrete phase particles. The DDPM
formulation (13) overcomes this limitation by solving a set of conservation equations
for multiple phases (generalized form written below for phase p).
∂ 
(α ρ p ) + ∇ (α=
p p p) ∑ ( m − m pq )
n phases
ρυ (1)
∂t
p qp
q =1
∂     
(α ρ pυ p ) + ∇ (α p ρ pυ pυ p ) = −α p ∇p + ∇ ⋅ α p µ p ( ∇υ p + υ pT )  +
∂t
p

∑ ( K (υ )
    
− υ p ) + m qpυ qp − m pqυ pq +
n phases
αpρpg + F + qp q (2)
q =1
 
K DPM (υ DPM − υ p ) + S DPM ,explicit
The conservation equations are not solved for the particulate phase, but the
appropriate volume fraction or velocity values are taken directly from the particle
field.
The particle equation of motion is solved for each particle in the form:

g (ρp − ρ )

dυ p −1    
= ∇p + FD (υ − υ p ) + + F + Finteraction (3)
dt ρp ρp
The right hand side terms represent the pressure force, drag force, gravitational
force, any additional force and the particle-particle interaction force. The drag force
is calculated as in equation (4) with the drag coefficient modelled according to
Syamlal et al. (9).
18µ CD Re p −1
FD = (4) =
Finteraction ∇p p (5)
ρ pd 2
p
24 α pρp
2
The interaction force is estimated from the solids pressure gradient according to
equation (5). This is a simple but fast model for the major physical effect. It does not
have the highest possible accuracy but favours efficiency, in particular when
compared to DEM like approaches. A major limitation of this formulation is that the
particle interaction force does not contain any viscous contribution. The resistance
to strain caused by the modelled shear viscosity is therefore not included. In the
dense fluidized bed system simulated here, this viscous force could be of significant
importance and its negligence is expected to create a more free-flowing bed than
might be expected.
The granular temperature used in the KTGF is calculated in its algebraic form from
the ordinary differential equation below:
3∂  

2  ∂t
( α p ρ p Θ )  = τ p : ∇υ p + γ Θ + φ pq (6)

Here, the right hand side terms represent the generation of fluctuating energy by the
solids stress tensor, the collisional dissipation of fluctuating energy (11) and the
energy exchange between the fluctuating particles and any additional phases (14).
The solids stress tensor in equation (6) is written as follows:
 2  
τ p = − p p I + 2 µ p S +  λ p − µ p  ⋅ ∇υ p I (7)
 3 
Here, the solids pressure and the bulk viscosity is calculated according to Lun et al.
(11) and the shear viscosity according to Syamlal et al. (9). Within these
formulations, the radial distribution function is calculated according to Ogawa et al.
(12).
Computational Domain
Simulations will be compared to pressure drop data collected from an industrial
fluidized bed reactor as reported by Gobin et al. (15). The cylindrical reactor was 5
m in diameter and 30 m in height. It was found, however, that only 15 m of height
needs to be included in the domain for the flow scenarios investigated in this study.
Both 2D and 3D simulations were conducted. The 2D simulations were carried out
on a planar domain, 5 m in width and 15 m in height, while the 3D simulations were
carried out in a cylindrical domain, 5 m in diameter and 15 m in height. Both
domains were meshed with constant sized square (2D) or cubic (3D) structured cells
according to the simulation run in question.
Material properties
The particles used in the experiments were poly-disperse with a mean diameter of
1.3 mm and a density of 850 kg/m3, characterizing them as Geldart D particles (16).
The fluidization gas was pressurized hydrocarbons with a density of 20 kg/m3 and a
dynamic viscosity of 1.5e-5 Pa.s (15).
Boundary Conditions
The bottom boundary of the domain was designated as a constant velocity inlet (0.5
m/s) to simulate a perfect plate distributor as the gas inlet. The top boundary was
designated as a pressure outlet. Side boundaries were designated as walls with a
3
specularity coefficient of 0.01 to describe a low friction wall in the framework of the
Johnson and Jackson (17) boundary condition.
Solver settings
The commercial CFD package, FLUENT 12.1 was used as the flow solver in this
study. The phase-coupled SIMPLE algorithm (18) was selected for pressure-velocity
coupling. All remaining equations were discretized using the QUICK scheme (19).
1st order implicit temporal discretization was used.
Operation and data extraction

Each simulation domain was initialized with a zero value for all flow variables. A
region of solids at a volume fraction of 0.35 was subsequently patched into the
bottom 8 m of the reactor as specified in Gobin et al. (15). For the DDPM, the
particle parcels were injected in the first 0.1 s of the simulation from all of the
internal surfaces of the mesh. This was done in such a way that the each cell in the
lower 8 m of the reactor would, on average, contain 10 particle parcels.
Following the patching and injection, the simulation was run until a quasi-steady
state was reached. This was identified by a monitor on the solids velocity. Once the
quasi-steady state was attained, the sampling of time statistics was activated in
order to get time-averaged axial pressure profiles for each simulation. Time statistics
were collected for a minimum of 30 s real time which was tested to be
representative of the time-averaged system behaviour.

As is often the case in industrial reactors, experimental values of pressure drop can
only be estimated from the available data (15). Only two pressure measurements
were available in the 5 m ID reactor, one at a height of 3.5 m and the other at a
height of 6.5 m. The pressure drop between them was experimentally measured to
be between 9 and 11 kPa. An average of 10 kPa will be taken. Some more detailed
pressure drop measurements were made in a pilot scale unit scaled to one third of
the industrial one. These measurements confirmed a virtually linear pressure drop
profile along the height of the pilot scale reactor. Under the assumption that the
pressure drop profile in the industrial scale reactor is linear as well, a linear pressure
drop of 10000/(6.5-3.5)=3333 Pa/m can be deduced. The total pressure drop over
the reactor can be estimated from the weight of the solids that has to be fluidized as
23348 Pa. An estimated linear pressure profile can therefore be specified with a
gradient of 3333 Pa/m and a y-intercept of 23348. Numerical simulations will be
compared against this experimental estimation.
The first set of simulations was carried out in 2D on grids spanning from 4 cm to 16
cm. In the domain simulated, this translated to cell counts between 2930 and 46875.
The simulation results attained with the TFM and the DDPM are given in Figure 1.
4
Figure 1: Pressure drop profiles for the 2D simulations with the TFM (left) and
the DDPM (right) for various mesh sizes from 4 cm to 16 cm.
It is clear that both modelling approaches provide adequate fits to the estimated
experimental data. The important finding for this study, however, is that the DDPM
seems to retain grid independent behaviour throughout with all the grids investigated
while the TFM never reaches complete grid independence. Grid independent results
for the DDPM with the 16 cm grid implies that reliable results in an industrial reactor
can be attained within an industrial reactor with only 2930 cells in 2D. This
simulation required about 1 hour of processing time on a single processor, which, in
terms of CFD standards, is very fast.
In comparison to the TFM, where grid independence might be attained on a 4 cm

grid, the DDPM solved on a 16 cm grid would require 16 times less cells in 2D and
can be run at a 4 times greater timestep. On a fixed grid, the DDPM is currently
about 3 times slower than the TFM, but even with this taken into account, the DDPM
can provide grid independent results more than 20 times faster than the TFM.
The reason for the good grid independence behaviour displayed by the DDPM is
similar to the conclusions drawn in Cloete et al. (7) – the Lagrangian particle
tracking provides for a much more accurate representation of the volume fraction
field. The volume fraction field tracked by the TFM on coarse grids is subject to
substantial numerical diffusion and the large volume fraction gradients cannot be
resolved accurately. Instantaneous plots of the volume fraction are displayed in
Figure 2 as illustration of this point.
Figure 2 shows very clear differences between the volume fraction fields resolved by
the TFM and the DDPM. In the DDPM, there is a very clear separation between the
bubble and emulsion phases on all the grids investigated, while the TFM does not
resolve clear bubbles even on the finest grid investigated. When looking at the
DDPM, it is clear that some of the flow detail is lost on the coarser grids, but Figure
1 shows that the global system behaviour is preserved, at least from a
hydrodynamic point of view. The degree to which this will be true for reaction kinetic
simulations is a subject for future study.
5
Figure 2: Instantaneous volume fraction profiles for the TFM (top) and the
DDPM (bottom). The mesh is coarsened from left to right from 4 cm to 16 cm.
Figure 3: Pressure drop profiles for 3D Figure 4: Comparison between the

simulations carried out with the DDPM solids volume fraction profiles
for various mesh sizes from 4 cm to 16 returned by the DDPM for the 2D and
cm. 3D cases with an 8 cm grid.
6
Following the good grid independence shown by the DDPM on coarse grids, some
3D simulations were also completed for grids of 8 cm and larger. The pressure
profiles in Figure 3 show that the 3D simulations also display very satisfactory grid
independence behaviour. Comparison to experimental data also shows acceptable
agreement, even though a possible under-prediction of bed expansion is observed.
In comparison to 2D simulations, the 3D runs also seem closer to reality in that they
display a more linear pressure drop trend.
Figure 3 seems to indicate that 2D simulations can adequately predict global system
behaviour in comparison to 3D at significantly reduced computational costs. When
looking at the solids volume fraction profiles (Figure 4), however, significant
differences between the 2D and 3D representations are observed. It is clear that the
3D simulations display much smaller bubbles than their 2D counterparts, especially
towards the upper regions of the bed. The large voidage at the top of the 2D bed
would explain the reduction in the pressure gradient towards the surface.
This pronounced difference between particle structure representation in 2D and 3D

implies that 2D simulations of 3D industrial beds should be interpreted with caution.
The similarity in pressure drop and bed height does suggest that the global system
behaviour is preserved even in 2D, but the local transport phenomena in the bed
seem to be significantly different. The system seems to be very forgiving towards
these differences in terms of global hydrodynamic behaviour, but is likely to be less
so when reaction kinetics are eventually incorporated.
CONCLUSIONS
Industrial scale bubbling fluidized bed simulations were carried out using the
traditional Two Fluid Model (TFM) and a new approach known as the Dense
Discrete Phase Model (DDPM). The DDPM showed substantially better grid
independence behaviour than the TFM. 2D simulations showed that results could be
attained at least 20 times faster with the DDPM than with the TFM.
Grid independence results with the DDPM were so encouraging that even
reasonably affordable 3D simulations could be completed. Comparisons to
experimental pressure drop data also proved to be acceptable. It was shown that
differences exist between the axial pressure profiles for 2D and 3D cases, but these
differences are not as large as might be expected. The local volume fraction
distribution through the respective domains did show substantial differences,
however, with the 2D simulations showing the formation of much larger bubbles than
their 3D counterparts. These differences seem to have only a minor influence on
global parameters such as pressure drop and bed height, but should be further
investigated in more detailed studies.
ACKNOWLEGMENT
The authors would like to acknowledge the financial support of the Research
Council of Norway under the Flow@CLC grant. Futhermore, the authors
acknowledge the use of the supercomputing facilities at the Norwegian University of
Science and Technology.
NOTATION
Regular symbols Greek letters
C Coefficient α Volume fraction
d Diameter (m) φ Rate of energy exchange (W/m3)
7
F Force (1/s) γΘ Energy dissipation rate (W/m3)
 Force vector per unit volume µ
F Viscosity (Pa.s)
(N/m3)

g Gravity vector (m/s2) Θ Granular temperature (m2/s2)
I Identity tensor ρ Density (kg/m3)
K Interphase exchange coefficient τ Stress-strain tensor

m Mass transfer rate (kg/s/m3) υ Velocity vector (m/s)
p Pressure (Pa) ∇ Gradient (1/m)
Re Reynolds number Subscripts
S Source term (kg/m2s2) D Drag
t Time (s) p Phase p or Particle/Solids
q Phase q
T Transpose
REFERENCES
1. Agrawal K, Loezos PN, Syamlal M, Sundaresan S. Journal of Fluid
Mechanics. 2001;445:151-85.
2. Wang J, Ge W, Li J. Chemical Engineering Science. 2008;63(6):1553-71.
3. Igci Y, Andrews AT, Sundaresan S, Pannala S, O'Brien T. AIChE Journal.
2008;54(6):1431-48.
4. Benyahia S. Industrial and Engineering Chemistry Research. 2010;49:5122-
31.
5. Andrews AT, Loezos PN, Sundaresan S. Industrial and Engineering
Chemistry Research. 2005;44(16):6022-37.
6. Wang J. Industrial & Engineering Chemistry Research. 2009;48(12):5567-77.
7. Cloete S, Johansen ST, Braun M, Popoff B, Amini S. 7th International
Conference on Multiphase Flow; 2010; Tampa, FL USA; 2010.
8. Taghipour F, Ellis N, Wong C. Chemical Engineering Science.
2005;60(24):6857-67.
9. Syamlal M, Rogers W, O'Brien TJ. Springfield: National Technical
Information Service 1993.
10. Schaeffer DG. Journal of Differential Equations. 1987;66:19-50.
11. Lun CKK, Savage SB, Jeffrey DJ, Chepurniy N. Journal of Fluid Mechanics.
1984;140:223-56.
12. Ogawa SU, A.; Oshima, N. Journal of Applied Mathematics and Physics.
1980;31:483.
13. Popoff B, Braun M. A Lagrangian Approach to Dense Particulate Flows. 6th
International Conference on Multiphase Flow. Leipzig, Germany 2007.
14. Gidaspow D, Bezburuah R, Ding J. Hydrodynamics of Circulating Fluidized
Beds, Kinetic Theory Approach. 7th Engineering Foundation Conference on
Fluidization 1992:75-82.
15. Gobin A, Neau H, Simonin O, Llinas J, Reiling V, Selo J. International journal
for numerical methods in fluids. 2003;43(10-11):1199.
16. Geldart D. Powder Technology. 1973;7(5):285-92.
17. Johnson PC, Jackson R. Journal of Fluid Mechanics. 1987;176:67-93.
18. Patankar S. Hemisphere Publishing Corporation 1980.
19. Leonard BP, Mokhtari S. NASA TM 1-2568 (ICOMP-90-12); 1990; NASA
Lewis Research Center; 1990.
8
HYDRODYNAMICS OF DUAL FLUIDIZED BED SYSTEMS WITH
INTERNAL MIXING CHANNELS BETWEEN CIRCULATING
AND BUBBLING FLUIDIZED BED REACTORS
Uendo Lee*†, Insoo Choi*, Jaehun Song **, Won Yang*, Youngdoo Kim*, and
Youngtai Choi*
* Korea Institute of Industrial Technology, Cheonan, Korea
**SeenTec Co., Ltd., Changwon, Korea
†Tel: +82-41-589-8574; Fax: +82-41-589-8323; Email: uendol@kitech.re.kr
ABSTRACT
We have examined a dual fluidized bed (DFB) system having internal mixing
channels between the circulating fluidized bed (CFB) and bubbling fluidized bed
(BFB) reactors. The bed material of the CFB reactor was supplied to the gasifier both
by an external circulation loop, comprising a riser, cyclone, and standpipe, and an
internal circulation loop that was implemented by making openings between the CFB
and BFB reactors. The hydrodynamics and mixing characteristics of the system were
investigated using a cold model test. Simple openings work very well for DFB
systems, and internal mixing can be realized while maintaining stable external
circulations.
INTRODUCTION
Gasifiers are systems that are essentially used to convert carbonaceous materials
such as coal or petroleum into product gases such as carbon monoxide and
hydrogen by reacting the raw materials at high temperatures using controlled
amounts of oxygen and/or steam. Three representative types of gasifiers are widely
used today—fixed bed, entrained flow, and fluidized bed. Among them a dual
fluidized bed (DFB) gasifiers is an advanced type. The DFB produces medium
heating value gas because the product gas is inherently separated from the
combustion gas that is necessary for providing heat for the endothermic gasification
reaction (1-2). In this system, the gasifier is separated from the combustor, and the
bed material is used as a heat and mass carrier between the two reactors. The
product gases from DFB gasifiers have been used for many applications such as
power generation, co-combustion with a conventional fuel, and catalytic synthesis to
obtain bio-Fischer-Tropsch (FT) diesel, dimethylester (DME), and synthetic natural
gas (SNG), respectively (3-4).
After Prof. D. Kunii proposed this system in 1975, various types of DFB gasification
systems have been developed; they are summarized in the review paper of Corella
et al. (5). Although the system is useful for generating medium heating value gases,
the operation of DFB systems is more difficult than that of the other systems because
it has two reactors that are sensitive to the mass and heat balance (6-8). Further,
loop seals are typically placed between the two reactors, and their function is to
reroute the solids for stable operations and to separate the product and combustion
gases; the loop seals complicate the process and makes it difficult to operate.
In our study, we have developed a novel DFB gasification system. Instead of having
a loop seal between the gasifier and combustor, we have created openings between
the two reactors, which enable the movements of the gases and solids. Overall, the
solids and gases flow from the gasifier to the combustor, but local internal mixing can
occur between the two reactors near the opening; such mixing enhances the heat
and mass transfers. In addition, by removing the loop seal, the entire system
becomes simpler and easier to operate.
COLD FLOW MODEL
Figure 1 shows the schematic diagram of the cold flow model as well as the external
and internal circulation loops. The external loop comprises a riser, cyclone, and
standpipe, while the internal loop was implemented by adding openings between the
reactors that are closely connected to each other. The hydrodynamics of the system
and the mixing characteristics of the system were expected to be significantly
affected by the openings. Under some conditions, internal mixing occurs near the
opening, and it helps to heat up the gasification zone along with the hot bed material
of the external circulation.
Fig. 1 Schematic diagram of novel dual fluidized bed (DFB) gasification system
In this system, the synthetic gas (syngas) from the gasifier flows directly to the CFB
combustor. When the syngas is injected into the hot combustion gas, the tar in the
syngas is thermally cracked and steam reforming occurs automatically with the
steam of the combustion gas. Moreover, the heating value of the product gas is low
because of mixing with the combustion gas. Some syngas loss occurs due to
combustion but additional syngas production from the tar cracking can be expected
to compensate the loss. Moreover, to decrease the syngas loss, the injection point of
the syngas should be kept far from the main combustion zone; however, such a
positioning is not considered here. In this paper, we have focused on the function of
the openings between the CFB and BFB reactors. As a result of the reduction in the
number of loop seals, this design minimizes any need for controlling the system
operations and even helps to maintain more uniform gasifier temperatures by
realizing simultaneous heating both by external and internal circulations of the hot
bed material.
EXPERIMENTAL CONDITIONS
In this study, the hydrodynamics and pressure balances of the system were
investigated in terms of the opening size and location and the number of openings.
The experimental conditions are summarized in Table 1. We changed the opening
sizes and locations by using partition plates. Three different cases have been tested,
as shown in Table 1. The opening height H0 is the length from the bottom of the
reactor to the starting position of the opening.
Table 1 Experimental conditions

Ugr Ug Opening height
Item Opening size (m × m)
(m/s) (Umf) HO (m)
CASE
0.833 1.2 0.05×0.05 0.10×0.05 0.16×0.05 0.345
1
CASE
0.833 1.2 0.16 × 0.05 0.245 0.295 0.345
2
Dual openings HO(m)
CASE
0.833 1.2 Bottom Upper Bottom Upper
3
0.16×0.05 0.16×0.05 0.245 0.445
EFFECT OF OPENING SIZE
In order to determine the effects of the opening size, experiments were conducted
with three different opening sizes (L × H: 5 cm × 5 cm, 10 cm × 5 cm, and 16 cm × 5
cm); all other conditions were identical for each case. In this experiment, the opening
is located above the free surface of the bed. Figure 2 shows the solid circulation rate
(Gs) for each case. Gs is dependent on the amount of solid from the gasifier and the
riser velocity. For identical riser velocities, Gs of the smallest opening is larger than
that of the other cases. In all cases, Gs increased as the gasifier velocity increased,
and the effect of gas velocity became more significant as the opening size
decreased.
18
HO = 0.345 m
Ugr = 0.833 m/s
16
Opening size (0.05 m x 0.05 m)
Opening size (0.10 m x 0.05 m)
Gs(kg/m Xsec) 14 Opening size (0.16 m x 0.05 m)
12
2
10
6
0.075 0.080 0.085 0.090 0.095
Ug(m/sec)
Fig. 2 Solid circulation rates with different opening sizes and gasifier velocities (single
opening)
0.7 0.7
Opening size is fixed (0.05mX0.05m) Opening size is fixed(0.16mX0.05m)
R-10 R-10
HO is fixed (0.345m) HO is fixed(0.345m)
0.6 Ugr(0.833m/sec) 0.6 R-9
R-9 Ugr(0.833m/sec)
Ug(1.2Umf) Ug(1.2Umf)
R-8 R-8
0.5 0.5
R-7 R-7
R-6 R-6
H (m )
H (m )
0.4 G-35 0.4

R-5 G-35 Opening
R-5 Opening
R-4 R-4
0.3 0.3
R-3 R-3
G-20 G-20
R-2
0.2 R-2 0.2
R-1 R-1
0.1 0.1
G-5
G-5
0.0 0.0
0.0 0.5 1.0 1.5 2.0 2.5 3.0 3.5 4.0 0.0 0.5 1.0 1.5 2.0 2.5 3.0 3.5 4.0
∆ p (kPa) ∆ p(kPa)
Fig. 3 Effects of different opening sizes: (a) 0.05 m × 0.05 m (b) 0.16 m × 0.05 m)
Figure 3 shows the pressure drop profile of the riser and gasifier for different opening
sizes. When the opening size is small (Fig. 3(a)), the gasifier pressure is always
greater than the riser pressure; this implies that the solid and gas flow in one
direction from the gasifier to the riser. In the case of such small openings, Gs is
higher than in the case of large openings if the riser velocity is sufficient to transport
the solid in the upward direction. In the case of large openings (Fig. 3(b)), the
pressures of the gasifier and riser become identical, and this implies that a mutual
exchange of the solid and gas occurs through the openings. This large opening leads
to internal mixing between the two reactors and leads to a decrease in the amount of
solid that flows into the external loop in the riser.
EFFECT OF OPENING LOCATION
In order to investigate the effects of the opening location, openings were created at
three different positions: H0 = 0.245, 0.295, and 0.345 m. Figure 4 shows the solid
circulation rate as a function of the riser velocity for different opening locations. When
the opening location was lower, the solid circulation rate was higher because the
gasifier pressure increases when the opening location becomes closer to the reactor
bottom.
EFFECT OF NUMBER OF OPENINGS
In order to investigate the influence of the number of openings, two openings were
installed between the gasifier and riser. The lower opening was located under the
bed (H0 = 0.245 m) while the upper opening was installed above the bed (H0 = 0.445
m). The opening size was fixed as 0.16 m × 0.05 m. In the case of such a dual
opening, internal mixing between the two reactors was observed. In the lower
opening, the solid flows from the gasifier to the riser, while in the upper opening, the
solid flows from the riser to the gasifier. Figure 5 shows the pressures of the riser and
gasifier near the two openings. The pressure of the gasifier is larger than that of the
riser in the lower opening, while the pressures for the two reactors are identical near
the upper opening. In the case of the dual opening, a vigorous internal circulation
occurred through the upper opening while the external circulation was maintained.
Obviously, this simultaneous solid circulation assists in heating the bed material more
uniformly in the gasifier.
12
Opening size (0.16m x 0.05m) is fixed.
Ug = 1.2Umf
10
HO = 0.245 m
8 HO = 0.295 m
HO = 0.345 m
Gs(kg/m Xsec)
6
2
0
0.65 0.70 0.75 0.80 0.85
Ugr(m/sec)
Fig. 4 Solid circulation rate with different opening locations

0.7
Ugr(0.833m/s) and Ug(1.2Umf) are fixed
R-10 HO(0.245m,0.445m) is fixed
0.6 Bottom opening: 0.16mX0.05m
R-9
Upper opening: 0.16mX0.05m
R-8
0.5
R-7 Upper opening
R-6
H(m)
0.4 R-5
G-35
R-4
0.3
R-3 Lower opening
G-20
R-2
0.2
R-1
0.1
Riser G-5
Gasifier
0.0
0 1 2 3 4
∆ p(kPa)
Fig. 5 Pressure of the gasifier and riser with dual openings
CONCLUSIONS
The hydrodynamics of a DFB system having openings between the CFB and BFB
reactors were investigated. These openings function as a replacement for the loop
seal and have identical functions. The effects of the sizes, numbers, and locations of
the openings were examined, and the characteristics of the solid and gas
movements through the openings were observed. For single openings, internal
mixing occurs when the opening size is large and is located over the bed. For dual
openings, vivid internal circulations were observed. In this manner, we have
demonstrated that simple openings work very well for the DFB system, and internal
mixing can be realized using the openings while simultaneously maintaining stable
external circulations of the bed material.
ACKNOWLEDGEMENT
The authors are grateful to MKE for providing funding via ” Development of Syngas
Production/Utilization System Through Large-scale (CFB)Circulating Fluidized Bed
Biomass Gasifier” project. The authors also would like to acknowledge the extensive
contributions of Prof. Bo G Leckner.
NOTATION
GS: solid circulation rate [kg/m2s]

H: height [m]
L: length [m]
W: width [m]
△P: pressure drop [kPa]
Uo : Superficial gas velocity [m/s]
Ugr: gas velocity in riser [m/s]
Ug: gas velocity in gasifier [m/s]
Umf: minimum fluidization velocity [m/s]
HO : Opening height from the distributor [m]
REFERENCES
1. Boerrigter, H., Den Uil, H., Calis, H., “Green Diesel from Biomass via
Fischer-Tropsch synthesis: New Insights in Gas Cleaning and Process Design”,
Pyrolysis and Gasification of Biomass and Waste, Strasbourg (2002)
2. Sung, YK, Song, JH, Bang, BR, Yu, TU, Lee, UD, "A hydrodynamic characteristic
of a dual fluidized bed gasification" 20th International Conference on Fluidized Bed
Combustion. Xian, China (May , 2009)
3. Tijmensen, M., Faaij, A., Hamelinck C. and Hardeveld, M., “Exploration of the
possibilities for production of Fischer Tropsch liquids and power via biomass
gasification”, Biomass and Bioenergy 23, pp.129-152, (2002)
4. Song, JH, Sung, YK, YU, TU, Choi, YT., Lee, UD, “Optimization of Biomass
Gasification Process for F-T Biodiesel Synthesis,“ 20th International Conference
on Fluidized Bed Combustion. Xian, China (May, 2009)
5. Corella, J, Toledo, J. M. Molina. G, "A Review on Dual Fluidized Bed Biomass
Gasifiers, Ind. Eng. Chem, 46, pp.6831-6839, (2007)
6. Guanwen Xu, Takhiro Murakmi, Yoshiaki Matsuzawa, and Hidehisa Tani, “The
Superior Technical Choice for Dual Fluidized Bed Gasification”, Industrial &
Engineering Chemistry Research, 45, pp.2281-2286 (2006)
7. Song, JH, Sung, YK, Choi, IH, Jeong HJ, Yu, TU, Lee, UD, "Steam gasifiaction of
woody biomass in a fluidized bed for F-T Synthesis", 34th Clear Water Conference,
Clearwater, Florida, USA (June, 2009)
8. Jansawang, W., Klimanek, A., and Gupta, A., “Enhanced yield of hydrogen from
wastes using high temperature steam gasification”, Journal of Energy Resources
Technology, Transactions of the ASME 128 (3), pp. 179-185 (2006)
BIO-GASOLINE FROM JATROPHA OIL:
NEW APPLICATIONS FOR THE FCC-PROCESS
by Alexander Weinert 1, 2 , Alexander Reichhold 1 , Peter Bielansky 1 ,

Christoph Schönberger 1 , Bettina Schumi 1
1
Getreidemarkt 9/166, 1060 Vienna, Austria
2
alexander.weinert@tuwien.ac.at
ABSTRACT
Jatropha curcas L. is a very drought-resistant plant, and jatropha oil can be ex-
tracted from its seeds. Whilst not suitable for human consumption, we found that it is
a promising feedstock for producing (bio)-gasoline. The oil was cracked in an inter-
nally circulating FCC-reactor using a Grace Davison Ultima® catalyst. The total con-
version was around 65%, with ca. 40% gasoline and ca. 25% crack gas (exact num-
bers varied with reactor temperature). The gasoline has a RON > 95 and oxy-
gen < 0.3% m. The crack-gas consisted of ca. 35% propylene, ca. 13% 1-butene
and ca. 6% ethylene.
THE FEEDSTOCK
Jatropha curcas L. (JCL) belongs to the family Euphorbiaceae. Jatropha originated
in Mexico, Central America and northern South America, but today it grows in many
tropical and subtropical countries. In 2008, the worldwide area under cultivation was
900,000 hectares, with Asia (85%), Africa (13%) and South America (2%) being the
main producing areas. Estimations suggest that the area of cultivation will increase
to a total of 13,000,000 hectares by 2015 (1).
The Plant
Jatropha curcas grows as small tree or bush, with a maximum height of 5-7 m. Its
life expectancy is 50 years and the crop yield increases with age. Under normal
conditions jatropha seeds are only harvested once a year, but when watered suffi-
ciently or when grown in humid regions, the fruits ripen throughout the entire year
(2). As JCL is a tropical to semi-arid climate well-adapted succulent, it can survive
three consecutive years of drought by dropping its leaves (3).
Jatropha plants grown from seed develop a strong tap root (up to 5 m long) that can
help stabilize the soil and prevent landslides. If propagated vegetatively by cuttings,
JCL forms a dense root carpet that can prevent erosion and accumulate humus (4).
Jatropha curcas grows on a wide variety of soils, except clay-rich soil. Accordingly,
well-drained sandy soils with good aeration are preferred (5). Jatropha has very low
nutrient requirements, but for optimal crop yield fertilization is necessary (6).
Because its leaves are inedible to animals, jatropha is often used as a hedge plant
to protect fields from animals. Because of a greater interest in non-fossil sources for
fuel, there is an increase in large-scale plantations (1).
The Oil
The most valuable product of JCL is jatropha oil. The quantity of seeds harvested,
the oil content in the seeds and thus the total oil yield vary greatly with the climatic
region and cultivation conditions. With optimal watering conditions (ca. 1200 mm
precipitation per year) and a high soil fertility of around 6000 kg/ha/a, seed can be
harvested (7).
There are two main ways to obtain the oil: mechanical and solvent extraction. Up to
60% of the total oil can be obtained by using a manually operated oil press. If the
press is motorized, jatropha seeds can yield up to 75% oil (8). A more efficient way
of obtaining the oil is solvent extraction: when using organic solvents (hexane is
most frequently used) practically 100% can be extracted, whereas with water-based
solvents these values vary from 65% to 100% (depending on temperature and pH-
value, amongst others). Since solvent extraction is energetically more demanding, it
is only economically practical on a larger scale (4).
Jatropha oil mainly consists of fatty acids. We determined the exact composition by
transesterification followed by GC-analysis (according to EN ISO 5509:2000). The
oil was found to contain high amounts of unsaturated fatty acids (76.8%) and 23.2%
saturated fatty acids. The details are shown in Figure 1.
Palmitic Acid
14,2% 9,0% 40,4% 36,4% Stearic Acid
Oleic Acid
Linolic Acid
0% 20% 40% 60% 80% 100%
Figure 1: Fatty acid composition of the jatropha oil analyzed
Jatropha oil is unsuitable for human consumption as it contains relatively high

amounts of phorbolic esters and lecithins (2). Therefore, unlike conventional biofuel
feedstocks (i.e. corn or palm oil), it is not part of the food vs. fuel dilemma.
EXPERIMENTAL SETUP
The Pilot Plant
A continuously working fluid catalytic cracking (FCC)-pilot plant (see Figure 2) was
used for the experiments. The different areas in the plant consist of the feed pre-
heater, the riser (where the catalyst comes into contact with the feed and where the
cracking takes place), the regenerator (where the spent catalyst is regenerated) and
the product gas condensation area. All sections are kept under an inert gas atmos-
phere (nitrogen), except for the regenerator (this needs oxygen to burn off the coke)
(9).
The plant has an internal circulating design, thus the riser is inside the regenerator.
This is a major difference from most other FCC-plants, which have external circula-
tion. The main advantages of internal vs. external circulation are:
 compact design
 simplified architecture (i.e. no slide valve for catalyst recirculation or cyclones
needed)
 desired heat coupling regenerator (exothermic combustion of coke) – riser (endo-
thermic crack-reaction)
The feed pre-heater is an electrically heated tubular oven. The oil is heated to
300°C. The length of the oven (9 m) helps to level out any peaks in flow rate and
thus assures a constant transport of the feed into the reactor.
Inside the reactor, the pre-heated oil
comes into contact with the hot cata-
lyst. This leads to vaporization of the
oil. The gaseous feed-molecules can
then react with the catalyst particles.
The cracking reactions produce many
gaseous molecules, which in turn are
responsible for the increase in volume.
This effect causes an upward move-
ment inside the riser. The flow created
conveys the catalyst upwards to the
particle separator that diverts the cata-
lyst-flow to the regenerator. The prod-
uct gas, on the other hand, leaves the
reactor and is transported to the prod-
uct gas condensation area, from
where samples are taken for analysis.
The spent catalyst circulates internally
to the regenerator. Since this area of
the reactor is fluidized with air, a si-
phon (fluidized with nitrogen) is used
to strip the catalyst and prevent the air
from entering the product gas side.
The siphon also enables us to meas-
ure the catalyst circulation rate: when
the siphon fluidization is turned off, no
further spent catalyst can enter the
regenerator. As some of the catalyst is
still being transported through the ris-
er, the level of catalyst in the regene-
rator drops. This is measured as a
Figure 2: Schematic of the used FCC pilot plant drop in pressure, which is converted
into the catalyst circulation rate.
The regenerator is a stationary fluidized bed. Air is used as a fluidizing agent in or-
der to burn off the coke that becomes deposited on the catalyst during the cracking
reaction. The average residence time in the regenerator is around 10 minutes.
The bottom section is also built with a fluidization system. Like the siphon, this is
used to strip the catalyst coming in from the regenerator and to prevent the catalyst
flow from stopping.
The Catalyst
A standard zeolite FCC-catalyst was used for cracking of the oil. The catalyst was
an equilibrium catalyst (e-cat) by Grace Davison (E-Ultima®). For more details,
please see Table 1 below.
Table 1: Specifications of the catalyst used
Name of catalyst Grace Davison E-Ultima®

Type of catalyst shape-selective zeolite
Particle size range 20 – 200 µm
Mean particle size 75 µm
ANALYSIS
There were three main components that needed to be analyzed: the flue gas, the
gaseous product and the liquid product. Figure 3 shows a schematic of the sampling
and analytics.
Figure 3: Schematic of the sampling and analytics and assignment to the product lumps
A side-stream of the product gas was sucked away for 15 minutes. The hot gas was
run through coolers (first and second stage at 4°C and a third cooler at -20°C) and
partially condensed. The still gaseous fraction was collected in a gas-sampling bulb
and analyzed immediately. The liquid fraction was stored in a glass bottle for subse-
quent phase separation.
Gaseous Phase
The gaseous phase mainly contained crack gas: olefins (propylene, 1-butene and
ethylene) and paraffins (linear and iso-paraffins). Another part contained uncon-
densed paraffins (mainly C5 and C6). This group was added to the gasoline lump
(see Figure 3).
Other components in the gas were CO and CO2, both of which are only formed in
the presence of oxygen contained in the biomass.
Liquid Phase
The liquid phase was separated into an aqueous and an organic phase. The water
formed contained most of the oxygen from the biomass. The rest was found as CO
or CO2 (see the section above). This left the organic phase (gasoline, LCO and resi-
due) practically free from oxygen compounds (total oxygen < 0.3% m.).
The resulting boiling range of the organic phase was measured by a SimDist so that
the contents of the gasoline in the product could be determined.
Flue Gas
The flue gas provides information about the coke formed during cracking. It was
analyzed online with two Rosemount® NDIR-gas analyzers. The detected compo-
nents were CO, CO2 and O2. The amount and composition of the coke formed was
determined from this data.
RESULTS
First, experiments with varying riser temperatures were conducted. Each data point
is an averaged from three single values in order to improve statistical significance.
Figure 4 shows the influence of varying riser temperature (averaged along the
height of the riser) on the valuable products of gasoline, crack gas and CO. The total
fuel yield (TFY) shown was defined as shown in (1) below:
(1)
With increasing temperature in the reactor, there was a tendency for smaller mole-
cules to form in the cracking process; this led to an increased production of gasoline
(+3% / 100 K) and gas (+9% / 100 K). This was mainly at the expense of light cycle
oil (LCO) and residue (-11% / 100 K), and coke, to a lesser extent (-2% / 100 K)
(see Figure 5).
The formation of the oxygen-containing products CO (in Figure 4), CO2 and H2O
(both in Figure 5) was barely influenced by the increasing average riser tempera-
ture. There was no change in CO2 yield or a redistribution between CO
(-1% / 100 K) and water (+1% / 100 K).
Further experiments were carried out in order to compare jatropha oil with vacuum
gas oil (VGO, the regular feed for FCC units). These were performed at a mean riser
temperature of 550°C, which corresponds to the average FCC operating conditions
in refineries.
90% Total Fuel Yield 25% LCO & Residue
Gasoline Water
Percentage feedbased [% m.]

80%
Crack Gas Coke
70% CO 20%
CO2
60%
15%
50%
40%
10%
30%
20% 5%
10%
0% 0%
500 550 600 500 550 600
Average riser temperature [°C] Average riser temperature [°C]
Figure 4: Influence of riser temperature on the Figure 5: Influence of riser temperature on the
formation of gasoline, crack gas and CO formation of LCO & residue, water, coke and CO2
Figure 6 shows the products of jatropha oil compared to VGO when used as feeds-
tock. Jatropha oil yielded less gasoline (-9%) and crack gas (-6%) per kilogram feed
than vacuum gas oil. This was mainly due to the formation of water (+11%) and CO2
(+1%). The oxygen contained in the triglyceride converted into these components.
60% 14%
12%
50% VGO VGO

50% Jatropha oil 12% Jatropha oil
41%
40% 10%
9%
32%
30% 8%
26%
20% 6% 5%
14%15% 4%
11% 4% 3%
10% 6% 3%
4% 0% 0%1% 2%
2% 1%
0%
0%
Figure 6: Products lumps of jatropha oil as feed Figure 7: Olefins contained in the crack gas of
compared to VGO (at 550°C riser temperature) jatropha oil as feed compared to VGO (at 550°C)
Figure 7 depicts the olefin contents of the crack gas. Compared to VGO, the jatro-
pha oil showed a similar distribution of the olefins. The composition of crack gas was
about the same for both feeds. The decrease shown above was due to the afore-
mentioned formation of water (and the subsequent reduction in gas yields).
Figure 8 shows the results of a PIONA analysis: paraffins, iso-paraffins, olefins,
naphthenes and aromatics. It was performed using two-dimensional GC-analysis
(GC × GC).
Jatropha oil produced fewer aromat-
60% ics (-6%) and iso-paraffins (-7%). The
Percentage of gasoline [% m.]
VGO 51% increase in paraffins (+11%) and

50% Jatropha Oil 45%
naphthens (+2%) compensated for
40% this.
30% 26% 26% Table 2 compares the gasoline prop-
erties with the current legal specifica-
20% 13%15% tions. The research octane number
10% 8% 6% 8% (RON) and the motor octane number
2% (MON) were comparable to regular
0% FCC gasoline (from VGO). This was
mainly due to the very high amounts
of aromatics and i-paraffins still
present.
The gasoline from the jatropha oil
Figure 8: PIONA results of gasoline produced contained virtually no lead. The sulfur
contents was also considerably lower
than with regular FCC gasoline from VGO. As mentioned before, almost all of the
oxygen contained in the biomass was removed: only 0.3% was found in the liquid
product.
Table 2: Comparison of gasoline properties with current legal specifications
Property Unit Legal Legal Jatropha Common

min max gasoline FCC-gasoline
RON - 95 95 91 – 96
MON - 85 81 78 – 84
Density kg/m³ 720.0 775.0 801.1
Pb-contents mg/L 5 < 0.1
S-contents mg/kg 10 2 100 – 2000
O-contents % m. 2.7 0.3
ACKNOWLEDGEMENT
This work was funded by OMV Holding.
NOTATION
CO Carbon monoxide
FCC Fluid catalytic cracking
GC Gas chromatography
JCL Jatropha curcas L., botanical name of the jatropha plant
LCO Light cycle oil
MON Motor octane number
PIONA Acronym for paraffins, iso-paraffins, olefins, naphthenes, aromatics
RON Research octane number
TFY Total fuel yield
VGO Vacuum gas oil
REFERENCES
1. The Global Exchange for Social Investment LLP. (GEXSI LLP) (2008). Global
Market Study on Jatropha. London/Berlin.
2. Achten W.M.J., Verchot L., Franken Y.J., Mathijs E., Singh V.P., Aerts R., Muys
B. (2008). Jatropha bio-diesel production and use. Biomass and Bioenergy,
32(12), 1063-1084.
3. Macintyre, B. (2007). Poison plant could help to cure the planet. The Times, UK
(28.07.2007).
4. Achten, W.M.J., Mathijs E., Verchot L., Singh V.P., Aerts R., Muys B. (2007).
Jatropha biodiesel fueling sustainability? Biofuels, Bioproducts and Biorefining,
1(4), 283-291.
5. Heller, J. (1996). Jatropha curcas L. Promoting the conservation and use of
underutilized and neglected crops. PhD thesis, Institute of Plant Genetic and
Crop Plant Research, Gatersleben, Germany, and International Plant Genetic
Resource Institute, Rome, Italy.
6. Foidl, N., Foidl G., Sanchez M., Mittelbach M., Hackel S. (1996). Jatropha cur-
cas L. as a source for the production of biofuel in Nicaragua. Bioresource Tech-
nology, 58(1), 77-82.
7. FACT Foundation (2010). The Jatropha Handbook – From Cultivation to Appli-
cation. Fact Foundation, Eindhoven, Netherlands.
8. Jongschaap, R.E.E., Corré, W.J., Bindraban, P.S., Brandenburg, W.A. (2007).
Claims and Facts on Jatropha curcas L. Global Jatropha curcas evaluation,
breeding and propagation programme. Plant Research International B.V., Wa-
geningen, Netherlands, 158.
9. Reichhold, Al., Hofbauer, H. (1996). Internally Circulating Fluidized Bed as a
Reaction/ Regeneration System for Catalytic Cracking. in: 5th International Con-
ference on Circulating Fluidized Beds, Proceedings, Beijing, China.
STUDY OF RECARBONATION IN CIRCULATING FLUIDIZED
BED COMBUSTION
Irina Hyytiäinen, Anna Mahlamäki, Marko Palonen, and Mikko Varonen
Metso Power Oy, Lentokentänkatu 11, P. O. Box 109, 33101 Tampere, Finland
Helge Lemmetyinen
Tampere University of Technology, Korkeakoulukatu 10, P. O. Box 541, 33101
Tampere, Finland
ABSTRACT
Oxy-fuel circulating fluidized bed combustion (CFBC) can use calcium based sorbents,
primarily limestone, for the in-situ capture of much of the sulfur dioxide in the fuel.
Under oxy-fuel CFBC conditions, the CO2 content is usually high, and at high
combustor temperatures sulfur capture can occur in two steps, calcination and then
sulfation. The typical Ca utilization ratio in oxy-fuel CFBCs is less than half. When
temperature is below the calcination temperature while remaining exposed to a high
CO2 environment, recarbonation of unused CaO may occur. This reaction between
calcium oxide and carbon dioxide has the potential to create serious operational
problems and boiler maintenance issues. The main purposes of this study were to
design a test method to study recarbonation of limestone under oxy-firing fluidized bed
conditions using a test reactor and to carry out test runs using this method. The test
runs were carried out in a test reactor at Metso Power Research and Development
Center in Tampere, Finland.
The results show that the recarbonation and calcination reactions are limited by
thermodynamic equilibrium, while the partial pressure of CO2 and the temperature also
play important roles. The effects of N2 and O2 are not significant during the fast reaction
period, but become more pronounced during the slow, diffusion-controlled reaction
stage. Repeatability of the test method was good.
INTRODUCTION
Carbon-dioxide capture and storage (CCS) offers the potential for major reduction in
carbon dioxide emissions from fossil fuel based power generation. Oxygen enriched
combustion has been identified as one of the main CCS technology options. The main
design parameter in oxy-firing is to burn fossil fuel in a mixture of oxygen instead of air
and recycled flue gas, which contain mostly CO2. (Eriksson et al. (1), Zhao et al. (2))
Oxy-fuel circulating fluidized bed combustion (CFBC) can use solid sorbents, primarily
limestone, for in-situ capture of much of the sulfur dioxide in the fuel. Under oxy-fuel
CFB combustion conditions, the CO2 content is higher than 70%, and at high combustor
temperatures sulfur capture can occur in two steps. First, the limestone is expected to
decompose to CaO, and calcination (I) and subsequent reaction between CaO and SO2
will lead to the formation of solid CaSO4, sulfation (II).
Calcination: CaCO3(s) + heat CaO(s) + CO2(g) (I)
Sulfation: CaO(s) + SO2(g) + 1/2O2(g) CaSO4(s) + heat (II)
Recarbonation: CaO(s) + CO2(g) CaCO3(s) + heat (III)

Calcination will proceed only if the partial pressure of the CO2 in the gas above the
limestone is less than the equilibrium partial pressure of carbon dioxide, at the
calcination temperature. For each partial pressure of CO2 there is a corresponding
temperature, known as the equilibrium calcination temperature. Figure 1 plots five of the
expressions for dissociation pressures and corresponding equilibrium calcination
temperatures listed in the literature.
Figure 1. Dissociation pressures and corresponding equilibrium calcination temperatures. (Basu

et al. (3), Baker (4), FACT-database (5), CRC Handbook (6), Nskala et al.(7))
The typical Ca utilization ratio during sulfation in CFBCs is about 30–45%. Therefore,
the CaO content in CFBC fly ash and bed ash is generally high. When CFBC ash cools
while remaining exposed to a high CO2 environment, recarbonation (III) of unused CaO
deposited on cool surfaces may occur. (Wang et al. (8)) Recarbonation is the reverse
reaction to calcination, and it occurs below calcination temperatures. This phenomenon
has the potential to create serious operational problems and boiler maintenance issues.
There are relatively few findings on oxy-fuel fluidized bed combustion published in the
open literature, especially studies on recarbonation. However, there are a few studies in
which the recarbonation was carried out mainly in TGA. The main purposes of this
study were to design a test method to study recarbonation of limestone under oxy-firing
fluidized bed conditions using a test reactor and to carry out test runs using this
method.
EXPERIMENTAL SET-UP AND PROCEDURE
The experimental tests were carried out in a vertical tube reactor with an internal
diameter of 4.9 cm. The test reactor simulates a fluidized bed furnace where a
limestone sample is fluidized in a sand bed using inlet gas. In this experimental study,
the reactor was supplied with CO2 and O2 in an N2 balance. The pure gases are mixed
before entering the reactor inlet. The gases flow through a perforated grid at the bottom
of the reactor up to the top of the reactor. The fine particles in the flue gas are
separated and captured by a cyclone. The sand and limestone can be fed in batches
from the top of the reactor. The hot bed material can be removed by an ejector from
above the tube reactor. Also the cyclone can be emptied. The flue gas flows through
gas analyzers to the stack. The test equipment used in this study is illustrated in Figure
2.
Figure 2. Diagram of testing equipment.
The test reactor is fully automated and computer-controlled. Its temperature is

controlled by electric heaters with a combined heat input of 10.4kW. Electrical heaters
encircle the reactor. The heaters can maintain the bed region at a maximum
temperature of 850°C. The temperature at many different points along the tube reactor
(at different heights from the grid) can be measured with thermocouples. The walls of
the reactor are insulated with thermo wool to avoid heat loss. The pressure differences
can be controlled by pressure control valves, and pressure differences in the reactor
tube and at the grid plate are measured. The pressure difference between the reactor
tube and atmospheric pressure is also measured. Mass flow meters are utilized to
obtain the desired inlet volume flow rates (ln/min). The concentrations of CO2 and O2 in
the gas leaving the bed were measured continuously, using gas analyzers. The
evolution of gas concentrations in the outlet gas and the temperature and pressure
differences were continuously monitored and recorded at intervals of one second.
Table 1. Chemical compositions of Piney
Creek limestone.
Table 2. Experimental conditions.
Element wt-% Element wt-%
CaO 51.6 K2O 0.13 Temperature (°C) 650, 750, 850
SiO2 3.1 Na2O 0.02 XCO2 (vol-%) 10,40,60,90
TiO2 0.04 MnO 0.053 XO2 (vol-%) 4, 10
Al2O3 0.69 P2O5 0.067 XN2 (vol-%) 0,6,36,56,86
Fe2O3 1.4 S-Eltra 0.1
MgO 0.55 H.h. 950°C 41.7
The limestone used in this study was Piney Creek (PC) limestone from the USA; its
chemical composition is shown in Table 1. The limestone samples were prepared
before the experiments. All experiments followed the same procedure. First, the
limestone was sieved to a size fraction of 500–710µm, which was considered to be
appropriate for the fluidized-bed system. Another reason for sieving was to remove all
the small particles and to obtain a coarse enough batch, because if the particles are too
small they may escape with the flue gas. After sieving, 20 g of limestone was calcined
in a furnace at 900°C (30 minutes) under air. The tube reactor was operated in oxy-fuel
combustion mode under atmospheric conditions. In each run, 130 g of sand at a size of
0.1–0.5mm was loaded from the top of the reactor to form a fluidized bed. A constant
fluidization velocity of 0.3m/s was maintained throughout the tests. Each test run was
initiated by loading a calcined and weighed batch of limestone onto the hot sand bed,
which had been heated to the required temperature and was simultaneously fluidized
by a gas mixture containing the desired content of CO2 and O2 in an N2 balance. The
CaO conversion was calculated according to the amount of CO2 which had reacted
during the test run. The calcination was studied by using 20 g of fresh and unprepared
Piney Creek limestone as the sample instead of the calcined sample. Table 2 shows
the experimental conditions during the series of experiments.
To estimate the composition of the samples (calcined limestones) it is necessary to

determine the free lime (CaO) contents. After calcination and before each recarbonation
test, the calcined sample was weighed to measure mass loss during the calcination
process, and thereby the extent of the calcination. The total weight loss of the sample
after calcination should be due to the weight of the CO2 lost through the CaCO3
decomposition. The total molar content of CaO in the calcined sample was calculated
from this weight loss. Respectively, the conversion of CaO to CaCO3 during the
recarbonation test in the tube reactor was calculated according to the amount of CO2
reacted during the test run, while conversion of calcium oxide was calculated on a
molar basis.
The first 320 seconds of reaction were taken into consideration, as this period was
ascertained to be sufficient to achieve the maximum reaction rate and therefore bring
the reaction into the slower (diffusion-limited) reaction regime.
Effect of CO2 content
Conversions of CaO vs. time for different CO2 contents at three different temperatures
are presented in Figures 3 (a)–(c). There were four different CO2 contents and 4% of O2
in N2 atmosphere. As can be seen in Figure 3 (a), high CO2 plays a particularly
important role in the recarbonation of CaO. The figure shows that the conversions of
CaO are close to each other except for conversion in high (90%) CO2 content. The
higher content of CO2 corresponds to the increased conversion of CaO. CO2 and CaO
are both reactants and the higher content of CO2 leads to the adding shift of the
reaction toward the product side (CaCO3), which compensates for the imposed change
in the conditions.
(a) 650°C (b) 750°C
(c) 850°C
Figure 3. Conversion of CaO at temperature of (a) 650°C, (b) 750°C, and (c) 850°C. 10–90%
CO2, 4% O2 in N2 atmosphere.
Figure 3 (b) shows that in the recarbonation results obtained at a temperature of 750°C,
the conversion at 90% CO2 is highest while the difference in the CaO conversion
between 60% CO2 and 40% CO2 is not significant. Several observations can be made
for conversion at 10% CO2. First, the low concentration of CO2 leads to the low
conversion of CaO. Second, as can be seen in Figure 1, this test point overlaps the
equilibrium curve, and such a test point position causes a drop in the conversion of
CaO.
The recarbonation of CaO at 850°C is shown in Figure 3 (c). The conversion of CaO at
90% CO2 is over 1. This is impossible and must represent a measuring error. The
conversion of CaO at 40% CO2 is close to zero, because at this point the pressure of
CO2 is close to the dissociation pressure. At 10% CO2, conversion of CaO is negative
because the partial pressure of CO2 is below the dissociation pressure at this point.
Under these conditions, the reverse reaction to recarbonation, i.e calcination, takes
place.
Effect of temperature
Figures 4 (a)–(d) show the recarbonation results obtained for a CO2 content of 10–90%,
4% O2 in an N2 balance. The effect of temperature on recarbonation was studied and
was found to have a strong effect on the conversion of CaO. Recarbonation is
exothermic, which means that the forward reaction is favored by lower temperatures.
Nevertheless, experiments show that higher temperatures lead to higher conversions of
CaO.
(a) 90% CO2 (b) 60% CO2
(c) 40% CO2 (d) 10% CO2
Figure 4. Conversion of CaO at (a) 90% CO2, (b) 60% CO2, (c) 40% CO2, and (d) 10% CO2.
The conversion of CaO decreases rapidly as the temperature approaches the

equilibrium temperature, as shown in Figure 4 (b) at 850°C, (c) at 850°C and (d) at
750°C. When the temperature is above the equilibrium temperature, the conversion of
CaO is negative, as shown in Figure 4 (c) at 850°C.
Effect of N2 and O2
The effect of temperature on the reaction between CaO and CO2 in a mixture of 90%
CO2 and 10% O2 without N2 is shown in Figure 5, curves (b), (d), and (f). It seems that
the higher temperature corresponds to the increased conversion of CaO. This is the
same observation as that made for the tests at 90% CO2, 4% O2 in an N2 balance, and
three different temperatures, as presented in Figure 4 (a).
Figure 5. Conversion of CaO at a mixture of 90% CO2 and 10 % O2 at (b) 850°C, (d) 750°C, and
(f) 650°C. Conversion of CaO at a mixture of 90% CO2, 4% O2 and 6% N2 at (a) 850°C, (c)
750°C, and (e) 650°C.
Figure 5 presents in parallel the curves of CaO conversion with and without N2 and with
different O2 content. Figure 5, curves (c) and (d) at 750°C and curves (e) and (f) at
650°C show that the conversions of CaO at the same temperature (650°C and 750°C)
with and without N2 (with 4% and 10% O2) during the fast reaction period are similar.
The slight differences between the runs become more prominent during the slow,
diffusion-controlled reaction stage, when conversion of CaO at 90% CO2, 4% of O2 in
an N2 balance becomes greater than the conversion of CaO at 90% CO2 and 10% O2.
As can be seen in Figure 5, curves (a) and (b) at 850°C, there is difference between the
conversions of CaO, probably due to an error in measurement of curve (a).
Repeatability
To verify the oxy-fuel firing results, repeat tests were conducted with calcined samples.
Repeatability is assessed through the variation in measurements taken under the same
conditions. The test conditions were identical in both tests, but they were carried out on
different days. It seems that the consumption rates of CaO were close to each other for
the tests and repeat tests. In summary, it can be said that the repeatability of this test
method is good.
CaCO3 feeding – calcination
The conversion of CaCO3 at 850°C is presented in Figure 6. Here, the conversion of

CaCO3 is the molar ratio of the reacted CaCO3 in relation to the initial content of CaCO3
in the sample.
Figure 6. Conversion of CaCO3 at temperature of 850°C. 10–90% CO2, 4% O2 in an N2 balance.
As can be seen in Figure 6, the highest conversion of CaCO3 is at 10% CO2. The
conversion of CaCO3 at 40% CO2 is low, and at 60% CO2 near to zero. This is because
the partial pressures of CO2 at these test points are close to the dissociation pressure of
CO2. The conversion of CaCO3 at 90% CO2 is negative, because the partial pressure of
CO2 at this point is above the dissociation pressure of CO2. This means that the
recarbonation takes place at these conditions and the equilibrium is on the reactant
(CaCO3) side.
CONCLUSIONS
The experimental tests on recarbonation were carried out in a test reactor, which
simulates oxy-firing fluidized bed conditions. The extent of recarbonation was
determined using the differences in the concentrations of CO2 in the flue gas during the
tests.
The conversion of CaO showed that recarbonation occurred easily at conditions, where
the values for the CO2 concentration was noticeable higher than the equilibrium CO2
concentration at the reference bed temperature under certain conditions. Observations
during the experiments show that the conversion of CaO is also sensitive to
temperature, the conversion of CaO being significantly higher at high temperatures than
at low temperatures, when the temperature is above the equilibrium temperature. The
experiments show that the conversion of CaO decreases rapidly as the temperature
approaches the equilibrium temperature. When the temperature is below the equilibrium
temperature, the conversion of CaO is negative, and under these conditions the reverse
reaction to recarbonation (calcination) takes place. Calcination was examined by using
fresh limestone as the sample instead of the calcined sample. The highest conversion
of CaCO3 was when the CO2 content was low, whereas when the CO2 content was
high, recarbonation took place instead of calcination. The conversions of CaO with and
without N2 (with 4% and 10% O2) during the fast reaction period are similar. The small
differences between the runs are pronounced during the slow, diffusion-controlled
reaction stage. The experimental data show that repeatability for this test method is
good.
The study of recarbonation will continue in a 4 MW oxy-fuel CFB pilot-scale unit during
several weeks in the fall of 2010. The bigger test equipment makes it possible to study
the effects of many important parameters, e.g. moisture, temperature and Ca/S ratio, on
recarbonation.
REFERENCES
1. Eriksson, T., Sippu, O., Hotta, A., Fan, Z., Myöhänen, K., Hyppänen, T.,
Pikkarainen, T. 2007. Oxyfuel CFB boilers as a route to near zero CO2 emissions
coal firing. Power Gen, Europe.
2. Zhao, C.S., Duan, L.B., Chen, X.P., Liang, C. 2009. Latest evolution of oxy-fuel
combustion technology in circulating fluidized bed. 20th International Conference on
Fluidized Bed Combustion. Xian City, China.
3. Basu, P. 2006. Combustion and gasification in fluidized beds. CRC Press. Taylor &
Francis Group. pp. 143.
4. Baker, E.H. 1962. The calcium oxide-carbon dioxide system in the pressure range
1–300 atmospheres. Journal of the Chemistry Society 70, pp. 464–470.
5. FACT-database. Bale, C.W., Pelton, A.D., Thompson, W.T. CRCT École
Polytechnique de Montréal, Quebec, Canada.
6. CRC Handbook of Chemistry and Physics. 70th edition. 1989–1990. Editor-in-Chief:
Weast, R.C., Editor: Lide, D.R., Associate Editors: Astle, M.J. and Beyer, W.H.
CRC Press, Inc. Boca Raton, Florida. F-72.
7. Nskala, N., Liljedahl, G.N., Turek, D.G. 2007. Commercialization development of
oxygen fired CFB for greenhouse gas control. Volume I Pilot scale testing and
design study of an existing CFB retrofit to oxygen firing and CO2 capture. Final
report submitted by Alstom Power Inc.
8. Wang, C., Jia, L., Tan, Y., Anthony, E.J. 2008. Carbonation of fly ash in oxy-fuel
CFB combustion. Fuel 87, pp. 1108–1114.
EXPERIMENTS AND MODELLING OF MICRO-JET ASSISTED
FLUIDIZATION OF NANOPOWDER
J. Ruud van Ommen1, David M. King2, Samantha Johnson2, Niels Looije1,

Alan W. Weimer2, Robert Pfeffer3, Berend G.M. van Wachem4
1
Department of Chemical Engineering, Delft University of Technology
Julianalaan 136, 2628 BL Delft, The Netherlands
T: +3115 278 2133; F: +3115 278 5006; E: j.r.vanommen@tudelft.nl
2
Department of Chemical and Biological Engineering, University of Colorado
Boulder, CO 80309-0424, USA; alan.weimer@colorado.edu
3
Department of Chemical Engineering, Arizona State University
Tempe, AZ 85287, USA; robert.pfeffer@asu.edu
4
Department of Mechanical Engineering, Imperial College London
London SW7 2AZ, United Kingdom; B.van-wachem@imperial.ac.uk
ABSTRACT
The fluidization of nanoparticle agglomerates can be largely improved by using

downward pointing micronozzles, creating a high-velocity jet, as experimentally
shown. By discrete particle simulations – treating the agglomerates as single
particles – we show that the microjet strongly reduces the amount of gas in voids.
INTRODUCTION
In recent years, the fluidization behaviour of nanoparticles has been receiving

increased attention. It poses challenging scientific questions, but also has practical
applications. For example, through atomic layer deposition it is possible to provide
individual nanoparticles with an ultrathin coating. Weimer and co-workers
demonstrated this technique for a wide variety of materials (1,2,3); recently van
Ommen and co-workers showed that it is possible to carry out the process at
atmospheric pressure (4). Although it sounds counterintuitive that nanoparticles
could be fluidized, it is possible since they form agglomerates. Primary particles with
sizes ranges from 7 to 500 nm typically form agglomerates from about 100 to 700
μm (5). These agglomerates are so dilute they are often assumed to have a fractal
nature, thus making the coating of individual nanoparticles possible. Moreover, they
are dynamic in nature, meaning that each agglomerate continually sheds a
significant fraction of its composition, while simultaneously adding material from
other agglomerates. Over the past decade, several researchers have made efforts
to model the formation and fluidization of nanoparticle agglomerates (see, e.g.,
6,7,8,9). Because of the large cohesive forces, fluidization aids are often needed to
obtain proper fluidization of nanoparticles. Several ways have been proposed, such
as vibration, sound wave pulsation, and the use of AC electric fields (10). Recently,
Quevedo et al. (11) proposed the use of microjets as an alternative. They showed
that the fluidization behaviour of nanoparticle agglomerates is greatly enhanced by
adding a secondary flow in the form of a high-velocity jet produced by one or more
micronozzles pointing vertically downward toward the distributor. The micronozzles
produced a jet with high velocity (up to near sonic velocities), breaking up large
nanoagglomerates, preventing channelling, curtailing bubbling, and promoting liquid-
like fluidization. In addition, they claimed that microjet-assisted nanofluidization was
also found to improve solids motion and prevent powder packing in an internal, is
easily scaled-up, and can mix and blend different species of nanoparticles on the
nanoscale. They proposed that microjets improve the fluidization by increasing the
turbulence and inducing high shear forces, which lead to agglomerate breakage. In
this paper, we aim at achieving a further elucidation of the mechanisms through
which a microjet enhances nanoparticle fluidization using experiments and
modelling.
APPROACH
Experimental
Experiments are carried out in a glass column with a diameter of 26 mm, equipped
with a porous stainless steel distributor plate and a conical freeboard section to
minimize particle elutriation. A HEPA filter and water bubbler at the outlet of the
freeboard ensured that no nanoparticles were released to the environment. The
entire system was kept inside of a fume hood to protect operators.
The bed material consists of microfine TiO2 (Evonik Aeroxide P-25) with a primary
particle diameter 25 nm, which tend to form soft agglomerates. In all experiments
except those explicitly mentioned, the powders were sieved to have a diameter
between 70 and 180 µm. This enabled comparison between the jetted and unjetted
systems, as unsieved powders in the unjetted bed would segregate by size and only
a portion of the bed would expand. However, some experiments were completed
with unsieved powders to show the magnitude of the effect of the microjet.
The bed is fluidized at atmospheric pressure and room temperature with nitrogen at
superficial gas velocities ranging from 0 to 0.12 m/s. The bed was fluidized with a
downward pointing tube (2mm diameter) inserted at the axis of the column; at the
end of the tube a micro-nozzle has been attached with an internal diameter of 254
μm. Through the nozzle, we apply a nitrogen flow that is 30% of the base flow
through the distributor.
Modelling
For the modeling of particles and fluids, different approaches and models exist,
depending on the scale and region of interest. In this research, the interaction
between the fluid and the particle agglomerates is of interest. Therefore, a CFD-
DEM (Eulerian-Lagrangian) model was chosen. In this model, the fluid is
represented as a continuous medium. Since agglomerates typically consist of
billions of nanoparticles, it is not possible to model each individual nanoparticle.
Instead, we model the agglomerates as spheres with a typical density and diameter
that has been found experimentally in previous studies (7,9). For simplicity, we
assumed all agglomerates to have the same size, and we did not include the
breakage of agglomerates. Although we realize that this is a rough approximation,
we think this approach is a good first step to obtain insight in the forces that are
exerted on the nanoparticle agglomerates. We intend to extend the model to include
agglomerate breakage in the near future. The program that was used is MultiFlow
(12). Gas-agglomerate interactions (drag force) are calculated by the Wen and Yu
correlation (13). Agglomerate-agglomerate interactions are calculated using the soft-
sphere approach. This type of modeling enables multiple collisions, which occur
frequently in a dense fluidized bed. When agglomerates collide, they will have a
reversible deformation, leading to a repulsive force between the agglomerates. The
elastic deformation is approximated by allowing a small overlap, and a repulsive
force model is based upon the magnitude of the overlap. The model is based upon
the pioneering work of Mindlin and Deresiewicz (14) and Tsuji et al. (15). Model
details and implementation can de found in Hemph et al. (16). To properly model
cohesive particles, the interparticle forces are calculated by van der Waals forces
according to Hamaker (17). This force is inversely proportional to the square of the
interparticle distance and is characterized by the Hamaker constant which has
typical values of 10-19 J. The agglomerate motion is calculated by integrating
Newton's law of motion and the fluid is modeled by approximating the Navier-Stokes
equations in a finite volume discretized framework.
Table 1: Agglomerate parameters Table 2: System settings
Property Value Property Value
Model type Lagrangian Steps per collision 36
Diameter 260 μm Time step hydrodynamics 1·10-4 s
Density 30 kg/m3 Gravitation constant 10 m/s2
Youngs modulus 1.0 GPa X-dimension 30·10-3 m
Coef. of restitution 0.90 Y-dimension 4.0·10-3 m
Poisson ratio 0.25 Z-dimension 100·10-3 m
Coef. Of Friction 0.35 Superficial gas velocity 2.0·10-2 m/s
Number of agglom. 260,000
The most important properties of the agglomerates are shown in Table 1. A value of
1.0 GPa is used for the Young modulus. The minimum fluidization velocity for these
agglomerates was calculated to be 0.6 mm/s, using the Wen and Yu correlation
(13). Note, however, that the Wen and Yu correlation has not been validated for
particles (agglomerates) with such a low density. The properties of the walls with
respect to collision are equal to the agglomerates' properties. The fluid is air at
ambient conditions with a temperature of 298.15 K and a pressure of 1·105 Pa. The
density of air is 1.21 kg/m3 and the viscosity 1.52·10-5 Pa· s.
The other simulation settings are given in Table 2. The time steps for the particle
phase in the model are determined by the collisions. Each collision is calculated in
36 steps and depending on the collision properties, such as velocities and masses,
a time step is calculated. The jet tip is positioned in the centre of the horizontal
cross-section at 100·10-3 m above the distributor; the jet is pointing downward. The
mesh is refined around the microjet. We carried out two different simulations: a base
case with a superficial gas velocity of 2.0·10-2 m/s and the jet turned off, and a
second simulation with a superficial gas velocity of 1.4·10-2 m/s through the
distributor and a gas velocity of 18 m/s through the jet. The horizontal cross-section
of the jet is 200 μm x 200 μm. The total amount of gas provided to the bed is equal
for the two cases.
Experiments
Before carrying out the micro-jet experiments, we have investigated the effect of
isopropanol as a fluidization aid on the fluidization of nanopowders and heating and
sieving as pre-processing techniques. Isopropanol is hypothesized to suppress the
electrostatic forces. It also is useful in hydrating the system for de-aeration tests, so
it was important to see the effect. This was completed by a bubbler system, where
nitrogen, the fluidization gas, would flow through isopropanol, loading the nitrogen
with isopropanol solely through the vapour pressure of the isopropanol.
Subsequently, the bed heights of beds fluidized would be recorded with and without
isopropanol. Bed collapse experiments were also carried out to determine if the
isopropanol affected the distribution of gasses between the dense and bubble
phases. However, the effect of adding isopropanol is apparent from bed collapse
tests (not shown here): isopropanol leads to a slower de-aeration of the bed.
Isopropanol is hypothesized to suppress the electrostatic forces between particles,
but not to contribute to liquid bridging as long as it is in the vapour form. This effect
would allow almost all of the nanoagglomerates to participate in the fluidization
(rather than sticking to the wall or distributor), and lead to smaller bubbles, since
powders would not aggregate due to electrostatics.
Sieved & heated, IPA

2.5
Normalized Height [-]
Sieved, IPA
2
1.5 Unsieved, IPA
1
Unsieved, no IPA
0.5
0
0 0.02 0.04 0.06 0.08 0.1
Superficial Velocity [m/s]
Figure 1. The effect of sieving, heating, and adding isopropanol (IPA) on the
normalized bed height for the case without a microjet.
Figure 2. The powder in the bottom of the bed before and after processing with the
microjet.
Figure 2 shows the stark contrast in the unjetted and jetted beds, as indicated by
bed height. The jet (internal diameter 254 µm) was operated at 30% of the base
flow. For the case without the jet we found a minimum fluidization velocity of 3.2
cm/s; the jet reduced the minimum fluidization velocity to 2.0 cm/s. This implies that
less gas is required to fluidize the bed with a higher void fraction. Another important
aspect is the amount of gas that is in the bubble and dense phases. The goal is to
minimize the amount of gas in the bubble phase, especially if the fluidization gas is a
reactant. Measurements of the percentages in each phase can be done using bed
collapse test. In case of the jetted bed (both with sieved and unsieved material), we
found an even slower bed collapse that for normal fluidization with isopropanol
added. The bed collapse data indicates that the fraction of gas in the dense phase
increases from 0.55 (no jet, no isopropanol) and 0.75 (no jet, with isopropanol) to
(a) (b)
Figure 3. The powder in the bottom of the bed (a) before and (b) after processing
with the microjet. While in (a) agglomerates are clearly visible, no agglomerates can
be seen in (b).
0.85-0.90 with the jet turned on and isopropanol added. This is likely due to the fact
that the jet breaks up the agglomerates and diminishes the stratification. This can be
seen in Figure 3. In the left-hand picture, the visible, millimetre-sized aggregates can
be seen congregating in the bottom of the reactor. This formation hinders fluidization
by encouraging channelling. The right-hand picture was taken after the bed was
fluidized for ten minutes with the microjet turned on. This picture shows a much
more homogeneous bed with no visible aggregates. Our results indicate that with
the microjet no prior sieving of the bed material is needed, making it an industrially
advantageous technique.
Simulations
With the simulations, it is not possible to mimic the experimental set-up completely:
the amounts of nanoparticles agglomerates would become too large (>>106) to keep
the computational times within reasonable limits. Therefore, we decided to study a
pseudo 2D geometry. The depth is limited (4 mm), but large enough in term of
agglomerate diameters (>10 times the agglomerate diameter). For the simulations,
the ratio of the microjet cross-section (200 μm x 200 μm) compared to the bed
cross-section (30 mm x 4 mm) is much larger than in the experimental setup (3.3 x
10-4 versus 1.6 x 10-5). In order to keep the volumetric flow rate through the jet in the
optimum range (10-30% of the total volumetric flow rate (11)), we used a much
lower jet velocity in the simulations (18 m/s). In spite of these differences between
the experimental setup and the simulations, we still expect to obtain qualitative
insight in the mechanisms in which the jet enhances the fluidization of nanoparticle
agglomerates. The simulations have been run for a period of 1 s of real time.
Although this is a very short time, it gives us a first impression of the hydrodynamics.
Longer simulations are currently being carried out.
(a) (b)
Figure 4. Snapshots of the voidage as a function of the Hamaker constant,

respectively A = 0, 10-21 and 10-19 J, in the bed for (a) the jet turned off and (b) the jet
turned on. The snapshots are taken 1 s after the start of the simulation.
We show the results in colour contour plots of a vertical cross section through the
middle of the fluidized bed. Figure 4 shows the voidage distribution over the bed,
with the jet turned off (a) and on (b). The figure clearly shows that there is a strong
bubble formation in the case with the jet turned off, while the functioning jet leads to
a much more homogeneous bed. Figure 4(b) does not show a large bed expansion.
This means that the high jet velocity itself does not cause the large bed expansion,
but rather causes the agglomerate breakage due to the action of the jet, and its
impact on agglomerate-agglomerate collision frequency and force. Since these
simulations assume a constant agglomerate size (i.e. agglomerate breakage is not
considered), no bed height increase is observed. These results are well in line with
results we reported earlier (18).
We also varied the interparticle forces during the simulations. The left-hand-side
contour plots in Figs. 4(a) and (b) are the voidage distributions without interparticle
forces. The middle and right-hand-side plots in Figs. 4(a) and 4(b) show the voidage
for non-zero Hamaker constants, yielding low (A=10-23 J) and normal (A=10-21 J)
magnitudes of interparticle forces. The value of the Hamaker constant seems to
have little influence; even for the absence of interparticle forces (A=0 J) a very
similar voidage profile is observed. The results show that the inclusion of the
microjet leads to a more even distribution of the particles over the bed (i.e., absence
of large voids), irrespective of the presence and magnitude of interparticle forces.
Preliminary results from both experiments and simulations (not shown in this paper)
indicate that the jet just penetrates a few cm in to the bed. This means that in
deeper beds than currently investigated, it is best to position the jet relatively close
to the bottom, as most large agglomerates will be present in the bottom zone.
CONCLUSIONS
Experiments have shown that the fluidization behaviour of nanoparticle

agglomerates is greatly enhanced by adding a secondary flow in the form of a high-
velocity jet produced by a micronozzle pointing vertically downward toward the
distributor. We found that the microjet increases the bed expansion and the amount
of gas in the dense phase, which can be explained by a reduction in agglomerate
size. Discrete particle simulations were performed using a pseudo 2D geometry, in
which the agglomerates were mimicked by single particles and agglomerate
breakage was not taken into account. These simulations showed that the microjet
lead to a reduction of the amount of gas in voids, and a more homogeneous nature
of the bed. This agrees well with the experimental findings.
NOTATION
A Hamaker constant [J]

REFERENCES
1. Hakim, L. F., Blackson, J., George, S. M., Weimer, A. W. (2005), ‘Nanocoating

individual silica nanoparticles by atomic layer deposition in a fluidized bed
reactor’, Chem. Vap. Deposition 11, 420-425.
2. King, D.M., Johnson, S.I., Li, J., Du, X., Liang, X., Weimer, A.W. (2009),
‘Atomic layer deposition of quantum-confined ZnO nanostructures’,
Nanotechnology 20, 195401.
3. Liang, X., King, D.M., Li, P., George, S.M., Weimer, A.W. (2009), ‘Nanocoating
hybrid polymer films on large quantities of cohesive nanoparticles by molecular
layer deposition ’, AIChE J. 55, 1030-1039.
4. Beetstra, R., Lafont, U., Nijenhuis, J., Kelder, E.M., van Ommen, J.R. (2009),
‘Particle coating by Atomic Layer Deposition: protection of cathode material for
Li-ion batteries against degradation’, Chem. Vap. Deposition 15, 227 - 233.
5. Zhu, D., Yu, Q., Dave, R.N., Pfeffer, R. (2005), ‘Gas Fluidization
Characteristics of Nanoparticle Agglomerates’, AIChE J. 51, 426-439.
6. Chaouki, J., Chavarie, C. Klvana, D., Pajonk, G. (1985), ‘Effect of interparticle
forces on the hydrodynamic behaviour of fluidized aerogels’, Powder Technol.
43, 117-125.
7. Yao, W., Guangsheng, G., Fei, W., Wu, J. (2002), ‘Fluidization and
agglomerate structure of SiO2 nanoparticles’, Powder Technol. 124, 152–159.
8. Jung, J. and D. Gidaspow (2002), ‘Fluidization of nano-size particles’, J.
Nanopart. Res. 4, 483-497.
9. Hakim, L.F., Portman, J.L., Casper, M.D., Weimer, A.W. (2005), ‘Aggregation
behavior of nanoparticles in fluidized beds’, Powder Technol. 160, 149-160.
10. Lepek, D., Valverde, J.M., Pfeffer, R., Dave, R.J. (2010), ‘Enhanced
nanofluidization by alternating electric fields’, AIChE J. 56, 54-65.
11. Quevedo, J.A., Omosebi, A., Pfeffer, R. (2010), ‘Fluidization enhancement of
agglomerates of metal oxide nanopowders by microjets’, AIChE J. 56, 1456-
1468.
12. van Wachem, B.G.M. (2008) MultiFlow - A fully coupled solver for multiphase
flows, www.multiflow.org
13. Wen, C., Yu, Y. (1966), ‘Mechanics of fluidization’, Chemical engineering
programming symposium 62, 100-110.
14. Mindlin, R., Deresiewicz, H. (1953), ‘Elastic spheres in contact under varying
oblique forces’, J. Appl. Mech. 20, 327-344
15. Tsuji, Y., Kawaguchi, T., Tanaka, T. (1993), ‘Discrete particle simulation of
two-dimensional fluidized bed’, Powder Technol. 77, 79-87
16. Hemph, R., van Wachem, B., and Almstedt, A.-E. (2006), ‘Distinct element
modeling of hopper flows comparison and validation of models and
parameters’, In: Proc. Fifth World Congress on Particle Technology, Orlando,
Florida.
17. Hamaker, H.C. (1937), ‘The London-van der Waals attraction between
spherical particles’, Phyisica IV, 10, 1-15
18. van Ommen, J.R., King, D.M., Weimer, A.W., Pfeffer, R., van Wachem (2010),
‘Experiments and Modeling of Micro-jet Assisted Fluidization of Nanoparticles’,
in: Kim, S.D., Kang, Y., Lee, J.K., Seo, Y.C. (Eds), Proceedings of the 13th
International Conference on Fluidization, pp. 479-486, Engineering
Conferences International, New York.
EFFECTS OF SECONDARY AIR INJECTION UPON THE
FLUIDIZATION CHARACTERISTICS OF THE LOWER STAGE
IN A TWO-STAGE, VARIABLE-AREA FLUIDIZED BED RISER
Eric K. Johnson and Steven L. Rowan

West Virginia University, Morgantown, WV
ABSTRACT
A transparent scale model of a two-stage fluidized bed coal dryer with a small
diameter lower stage and a large diameter upper stage, separated by a conical
transition zone with secondary air injection ports, has been constructed to study the
effects of secondary air injection upon the fluidization characteristics of the lower
riser stage. The superficial velocity of the lower stage of the riser was held constant
within the turbulent fluidization regime while the superficial gas velocity in the upper
riser stage was varied by changing the volumetric flow rates of air introduced
between the upper and lower riser stages. Through examination of time series
pressure data via standard deviation, autocorrelation, spectral density plots and
visual observation of dense bed height, it becomes apparent that secondary air
injection has a dominant effect upon the fluidization characteristics below the
injection location, leading to a transition from a dense to a dilute bed.
INTRODUCTION
While not commonly used for commercial drying of fine coal particles, many other
industries have utilized fluidized beds for the drying of granular materials such as
grains, fertilizers and chemicals [1,2,3,4]. Fluidized beds possess many advantages
over more conventional drying techniques, among these advantages are: better
temperature control, more uniform temperature distribution, higher thermal efficiency
and intensity of drying, better gas-particle contact and less degradation of the
particles. Unfortunately, there are also disadvantages associated with fluidized bed
drying. These disadvantages include high pressure drops, non-uniform moisture
content in the product (when operated in continuous mode) and the inability to adapt
to counter-current operations [5,6,7,8].
While not commonly utilized in commercial coal drying applications, there has been
some research conducted to study aspects of fluidized bed drying of coal. Diamond
[7] concluded in a study to determine the effects of temperature and particle size on
the fluidized bed drying of northern Ireland lignite coal that drying rates increased as
air temperatures increases, as well as when particle sizes decreased. Calban et al
[5] obtained similar results while studying the drying characteristics of Turkish lignite
in a batch bubbling fluidized bed. In addition to temperature and particle size
considerations, Calban et al [5] determined that the velocity of the drying air had no
significant effect on drying rates. In another study, Calban [6] investigated the effects
of bed height and initial moisture concentration on drying rates of Turkish lignite.
Rowan [9] examined the performance of a two-stage, variable area fluidized bed
dryer with secondary air injection.
Commonly used in pulverized coal boilers, secondary air injection in fluidized beds
typically consists of splitting the fluidizing gas supply and introducing it into the
fluidized bed riser at multiple bed height locations. Ersoy et al [10] examined the
hydrodynamics of a circulating fluidized bed with secondary air injection, finding that
secondary air injection led to an increase in solids holdup in the zone below the
injection height for both radial and tangential injection modes. Above the secondary
air injection location, it was found that only tangential injection led to an increase in
solids holdup. It was also found that using a higher ratio of secondary air to primary
air (into the bottom distributor) also led to higher solids holdup values. Ersoy et al
[10] also looked at the effects of secondary air injection on the axial particle velocities
and noted a decrease in the primary zone below the injection location and an
increase in the secondary zone above. Chen et al [11] examined the effects of
secondary air injection on the distribution of solids concentration and proposed a
correlation between the secondary air penetration distance and the velocity of
secondary air.
In each of the previous studies, the fluidized beds used were of constant cross-
sectional area, and the given superficial gas velocities were calculated by combining
the flow rates of air into the bottom bed distributor as well as the secondary air. The
current study utilizes a novel two-stage, variable area geometry, as described in the
following section. In addition, the objective of the current study was to maintain a
constant superficial gas velocity in the lower riser stage, UL, while increasing the
superficial gas velocity in the upper riser stage, UU, by increasing the amounts of
secondary air injection. In this way, it was possible to characterize the effects of
secondary air injection on the fluidization characteristics below the secondary
injection location.
EXPERIMENTAL SETUP
The fluidized bed system shown in Figure 1 is a scale model of a larger system
designed to be a warm air dryer of fine coal particles. The model riser is constructed
primarily of transparent acrylic sections to allow for visual observation during
operation. The lower stage has an inside diameter of 2.29 inches and a height of
approximately 55.625 inches, the upper riser stage has an inside diameter of 4.0
inches and a height of 36.75 inches. The system also contains an air distributor at
the bottom of the lower stage, and a second conical distributor located between the
lower and upper riser stages. Both distributor plates are designed so that air is
injected radially into the riser. In addition, the lower distributor has another air inlet
that forms a vertical jet along the centerline of the riser. The air supply for both of the
distributors and the bottom jet is supplied by a compressor and are individually
controlled via rotameters.
Sand with a specific gravity of 2.65 and particle sizes ranging between 150 and 500
microns are supplied at a constant feed rate into a pneumatic transport line and enter
the bottom of the fluidized bed riser through the bottom air jet. Particle-laden air
exits the riser through an exit port in the upper riser stage and enters a cyclone,
which separates the sand from the exhaust gases. The sand is then collected in a
solids collection bin attached to the bottom cyclone exit and the air leaving the
cyclone is passed through a water filtration drum to trap any sand not separated out
by the cyclone.
Omega Engineering PX35k1- series pressure transducers are located along the
height of the riser. Three are located within the lower riser stage; they are located at
the bottom, middle and top, respectively. Another is located at the bottom of the
upper riser stage, and the final is located just below the exit port at the top of the
upper riser stage. Each of the pressure transducers measure absolute pressures in
units of psia at a sample rate of 100 samples per second and the resulting signal
was recorded for later analysis via an Omega Engineering OMB-DAQ-300 usb data
acquisition system.
Figure 1: System diagram
For this series of testing, the superficial gas velocity in the lower stage of the
fluidized bed riser (UL) was maintained at a constant 2.36 m/s, which was
determined to be within the turbulent fluidization regime by prior fluidization regime
mapping. The superficial gas velocity within the upper stage of the riser (UU) was
then varied from 1.42 m/s to 3.35 m/s by the addition of secondary air injection at the
transition between the two stages. Table 1 shows all of the test conditions.
Table 1: Test point upper and lower riser stage superficial velocities
Test # 1 2 3 4 5 6 7
UL (m/s) 2.36 2.36 2.36 2.36 2.36 2.36 2.36
UU (m/s) 1.42 1.74 2.06 2.38 2.70 3.02 3.35
Figures 2 and 3 show the effects of increasing levels of secondary air injection
upon the standard deviations of pressures in the lower and upper riser stages.
Similar trends can be seen in both figures. Each exhibits an initial increase in the
magnitude of standard deviation as the pressure fluctuations increase. This increase
is then followed by a subsequent decrease and then leveling out in the values of
standard deviation. The peak at UL = 2.36 m/s and UU = 1.74 suggests that both
riser stages are undergoing transition to turbulent fluidization at those operating
conditions. The curves in both figures, with the exception of the Lbottom location
(Figure 1a), exhibit a transition to fast fluidization when the amount of secondary air
injection leads to approximate superficial velocity matching between the two riser
stages (i.e. UL = 2.36 m/s and UU = 2.38 m/s).
In addition, as can be seen in Figure 2, the relative magnitudes of the standard

deviation decreases with increasing height within the lower riser stage, and the
Lbottom location exhibits a more gradual transition to core-annular flow than seen at
the Lmid and Ltop locations. This suggests that the effects of secondary air injection
occur first close to the area of injection and propagate progressively lower down the
riser with increasing amounts of secondary air injected, as denoted by increasing
values of upper riser stage superficial velocity, UU.
Figure 2: Lower riser stage standard deviation of pressure (a) Lbottom (b) Lmid (c) Ltop pressure
transducer locations.
Figure 3: Upper riser stage standard deviation of pressure (a) Ubottom (b) Utop pressure transducer
locations.
The effects of increases levels of secondary injection upon the fluidization

characteristics within the lower stage of the two-stage fluidized bed can also be seen
when examining the autocorrelation and spectral density plots shown in Figures 4
and 5. Due to space considerations, only data for the Lbottom pressure transducer
location are presented here.
Figure 4 shows the effects of increasing amounts of secondary air injection upon the
autocorrelation function of the Lbottom pressure transducer data. The
autocorrelation curves in lots a-c show evidence of very little periodicity in the
fluctuations of pressure. Plots d-g exhibit a higher frequency of extremely low
magnitude oscillations about zero and are assumed to primarily represent signal
noise in the instrumentation system due to a lack of bubble formation within the riser
as it transitions from a dense bed to a dilute fluidization regime.
Figure 4: Autocorrelation of Lbottom pressure: UL = 2.36 m/s, UU = (a) 1.42 m/s (b) 1.74 m/s (c) 2.06
m/s (d) 2.38 m/s (e) 2.70 m/s (f) 3.02 m/s (g) 3.35 m/s.
Perhaps the most obvious indicator of the effects of secondary air injection upon the
fluidization characteristics of the lower riser stage of the two-stage fluidized bed is
the spectral density plots, as shown in Figure 5. For levels of secondary air injection
resulting in upper riser superficial velocities UU ≤ UL=2.36 m/s, the frequency of
pressure fluctuations are concentrated within a range of frequencies between 0 and
2.5 Hz. In addition, the magnitude of power associated within these frequencies
increases as UU approaches the value of UL. As the magnitude of UU increases
beyond UL, there is a resulting widening of the range over which the pressure
fluctuation frequencies are spread. In addition, there is a general shift towards
higher frequency ranges and the amount of power associated with each frequency
becomes several orders of magnitude less than seen with lower amounts of
secondary air injection.
Figure 5: Spectral density of Lbottom pressure: UL = 2.36 m/s, UU = (a) 1.42 m/s (b) 1.74 m/s (c) 2.06
m/s (d) 2.38 m/s (e) 2.70 m/s (f) 3.02 m/s (g) 3.35 m/s.
Figure 6 shows the effects of increasing levels of secondary air injection (reflected by
increasing upper riser stage superficial velocity UU) upon the height of the visually
observed interface between the dense turbulent bed and dilute fast fluidization in the
lower riser stage. In the figure, the area above the curve exhibited visual indications
of fast fluidization (or core annular flow), while the region below the curve appeared
to be in a state of turbulent fluidization. As UU increased, the height of the dense
turbulent bed within the lower riser stage was observed to decrease. This supports
the conclusion from examining Figure 2 that increasing levels of secondary air
injection results in transition to fast fluidization progressively lower with the lower
riser stage.
Figure 6: Effects of upper riser stage superficial gas velocity on normalized height of interface between
dense bed and dilute regions of lower riser stage.
CONCLUSIONS
A transparent scale model of a two-stage, variable area fluidized bed was

constructed in order to study the effects of secondary air injection when introduced
above a lower riser stage operating within the turbulent fluidization regime. It was
discovered that increasing levels of secondary air injection eventually leads to a
transition from a dense bed turbulent regime to a dilute bed fast fluidization regime
below the level of secondary air injection. It is assumed that this occurs because the
solids carrying capacity above the secondary air injection point increases with
increasing levels of secondary air, limiting the recirculation of solids particles from
the upper riser stage back into the lower riser stage. This assumption is supported
by visual observation of greater amounts of solid material being pneumatically
conveyed out of the upper riser stage while operating at higher upper riser stage
superficial velocities.
ACKNOWLEDGEMENT
The authors would like to thank the National Research Center for Coal & Energy
(NRCCE), as well as the Center for Advanced Separation Technologies (CAST) for
their support and funding of this research effort.
NOTATION
UL lower riser stage superficial gas velocity

UU upper riser Stage superficial gas velocity
HI height of turbulent/fast fluidization regime interface
HLRH height of lower riser stage
Lbottom Pressure transducer, located 2 inches above bottom air distributor
Lmid Pressure transducer, located 27.5 inches above bottom air distributor
Ltop Pressure transducer, located 53 inches above bottom air distributor
Ubottom Pressure transducer, located 62 inches above bottom air distributor
Utop Pressure transducer, located 92 inches above bottom air distributor
REFERENCES
1. Balasubramanian, N., Srinivasakannan, C. Drying of granular materials in
circulating fluidized beds. Advanced Powder Technology, 18 (2007), 135-
142.
2. Jumah, R.Y., Mujumdar, A.S., Raghavan, G.S.V. Batch drying kinetics of
corn in a novel rotating jet spouted bed. The Canadian Journal of
Chemical Engineering, 74 (1996), 479-486.
3. Kannan, C.S., and Subramanian, N.B. Some drying aspects of multistage
fluidized beds. Chemical Engineering Technology, 21 (1998), 961-966.
4. Tatemoto, Y., Mawatari, Y., Sugita, K., Noda, K., Komatsu, N. Drying
characteristics of porous materials in a fluidized bed under reduced
pressure. Drying Technology, 23 (2005), 1257-1272.
5. Calban, T. and Ersahan, H. Drying of a Turkish lignite in a batch fluidized
bed. Energy Sources, 25 (2003), 1129-1135.
6. Calban, T. The effects of bed height and initial moisture concentration on
drying lignite in a batch fluidized bed. Energy Sources, 28 (2006), 479-
485.
7. Diamond, N.C., Magee, T.R.A., McKay, G. The effect of temperature and
particle size on the fluid bed drying of northern Ireland lignite. Fuel, 69
(1990), 189-193.
8. Nonhebel, M.A., Moss, A.A.H. Drying of solids in the Chemical Industry.
Butterworth & Co. Publishers, 1971.
9. Rowan, S. Analysis and Scaling of a Two-Stage Fluidized Bed for Drying
of Fine Coal Particles Using Shannon Entropy, Thermodynamic Exergy
and Statistical Methods. Doctoral Dissertation, West Virginia University,
Morgantown, WV, 2010.
10. Ersoy, L.E., Golriz, M.R., Koksal, M., Hamdullahpur, F. Circulating
fluidized bed hydrodynamics with air staging: an experimental study.
Powder Technology, 145 (2004), 25-33.
11. Chen, J., Lu, X., Liu, H. and Liu, J. The effect of solid concentration on the
secondary air-jetting penetration in a bubbling fluidized bed. Poweder
Technology, 185 (2008), 164-169.
EXPERIMENTAL STUDY ON REFORMING ACTIVITY AND
OXYGEN TRANSFER OF FE-OLIVINE IN A DUAL
CIRCULATING FLUIDISED BED SYSTEM
Stefan Koppatz, Tobias Proell, Christoph Pfeifer, Hermann Hofbauer
Institute of Chemical Engineering,
Vienna University of Technology, A-1060 Vienna, Austria
e-mail: stefan.koppatz@tuwien.ac.at
ABSTRACT
Fe-olivine was investigated in a dual circulating fluidised bed reactor system with
focus on hydrocarbon reforming activity and effects of oxygen transfer. H2, CO2, CH4
and 1-methylnaphthalene were fed as a surrogate gas mixture to the reforming part.
Oxygen transport was developed by solids circulation. Tar decomposition was
marginally affected by partial oxidation. The overall degree of tar decomposition was
found to be in the range of 70 to 80%.
INTRODUCTION
Biomass gasification is a suitable option for syngas generation and is the only
renewable carbon source for partial substitution of fossil fuels. Fluidised bed
processing is a common technology for the conversion of solid fuels into product gas
and therefore is the pre-process for direct use (heat and power supply) or for further
conversion processes into synthetic natural gas, liquid fuels or other chemicals. The
catalytic approach to biomass gasification, related to the reforming of hydrocarbons
(tars), is widely considered and under investigation by several groups (i.e.
Kiennemann et al., Corella et al. or Simell et al.) and is specified within this section.
Generally, catalysts can be grouped into natural or synthetic materials.
Comprehensive reviews on catalysts in biomass gasification are given by Dayton (1)
and Yung et al. (2).Natural olivine is often applied as bed material in fluidised bed
gasification. Several investigations have been performed focusing the catalytic
properties of olivine in terms of reforming of hydrocarbons or the gasification of
biomass. Comprehensive investigations have been published by Devi et al. (3), Abu
el Rub et al. (4), Kuhn et al. (5), Constantinou et al. (6), Rapagna et al. (7) or Rauch
et al. (8). Generally, the studies outline that olivine acts as a catalyst. It is assumed
that the catalytic property is associated with pre-treatment and iron content of the
particle surface. Thus, it is supposed that iron is responsible for the catalytic activity.
Pecho et al. (9) studied olivine and emphasised the oxygen transfer capability and
reforming activity by means of toluene. Beyond these applications, iron is usually
applied as a catalyst in the chemical industry (Fischer-Tropsch synthesis, ammonia
synthesis). However, the latter studies were carried out at lab-scale and
non-application oriented facilities. Thus, predictive or general statements with regard
to industrial application are rather limited. The present study focused on the
investigation of iron-supported olivine (Fe-olivine) to elucidate the effect of iron in
terms of tar reforming. Further, it is aimed to apply Fe-olivine as an in-bed catalyst,
for fluidised bed biomass steam gasification, as the iron material is considered to be
active for tar reforming. The investigations were carried out at a dual circulating
fluidised bed reactor system with 120 kW fuel power to consider application-oriented
aspects. A previous experimental study with natural olivine in terms of hydrocarbon
reforming activity and oxygen transfer was carried out by Koppatz et al. (10).
EXPERIMENTALS
Natural olivine (silicate tetrahedra with iron and magnesium) was used as the carrier
material for synthesis of the iron catalyst. The natural olivine (Mg1-x,Fex)2SiO4
(x ~ 8 wt.-%) was provided by Magnolithe GmbH (Austria). Thermal pre-treatment of
the raw material was carried out by the manufacturer in order to dry the water of
crystallization. Through the pre-treatment process, the bulk material passes through
a rotary kiln for approximately 4 h at 1600°C. Thus, sintering of the material was
further caused by the high temperature treatment. The Fe-olivine was developed by
the University of Strasbourg (Laboratoire des Matériaux, Surfaces et Procedés pour
la Catalyse). The material was synthesised with 10 wt.% at a large scale by wet
impregnation with iron nitrate solution. Drying of water excess (at 100°C) and
calcination (at 1000°C) of the material were carried out. Thus, the final global iron
content was at about 20 wt.% considering that the major part of the iron was
available at the particle surface. Preparation and characterisation of Fe-olivine has
been detailed by Virginie et al. (11). Moreover, Virginie et al. (12) studied Fe-olivine
as a catalyst for toluene steam reforming (at a micro-reactor scale) and found high
toluene conversion (95%). The study assumed that metallic iron was responsible for
the high conversion rates, since catalyst reduction with H2 was carried out as the
pre-treatment step.
Fig. 1. Particle size distribution Fig. 2. Sketch of the dual circulating

fluidised bed reactor system
Further, natural olivine is a non-porous material with a BET surface area of
< 0.5 m²g-1 is reported Devi et al. (3), but has due to its hardness of 6.5 – 7.0 on the
Mohs scale a high attrition resistance. Besides mechanical stability, high availability
at low cost makes the olivine advantageous for fluidised bed applications. The
cumulative size distribution of the applied Fe-olivine particles is depicted in Fig. 1.
According to the Geldart particle classification, the applied Fe-olivine is classified as
Geldart group B. The DCFB pilot rig consists of two interconnected circulating
fluidised bed reactors, named the fuel reactor (FR) and the air reactor (AR), allowing
continuous circulating of solid material between the reactors. A sketch of the reactor
system with dimensional information is displayed in Fig. 2. The pilot rig (nominal fuel
power of 120 kW) was developed for chemical looping combustion or chemical
looping reforming processes for gaseous fuels with a focus on scalability to large
scale application, whereas the circulating solids act as an oxygen carrier or reforming
catalyst. Further, sensitive heat transfer between the reactors is enabled by the
circulating bed material. The AR is designed as a fast fluidisation regime and the FR
for a turbulent fluidisation regime. Mixing of the gas phases is avoided by steam or
nitrogen fluidised loop seals. Downstream of each reactor, gas and solids are
separated in cyclone separators. After solid separation, the gas streams pass a
common post combustion chamber equipped with a support burner for complete
combustion. The exhaust gas stream is cooled down, cleaned in a bag filter and sent
to the chimney. The pilot rig and further auxiliary units are detailed by Kolbitsch et al.
(13) or Pröll et al. (14). For determination of fuel reactor exhaust gas concentrations,
a Rosemount NGA 2000 is used and, additionally, an online gas chromatograph
(Syntech Spectras GC 955) allows for cross-checking of carbon species and
determination of the N2 content for evaluation of possible gas leakages from the air
reactor to the fuel reactor. The air reactor exhaust stream is analysed using a
Rosemount NGA 2000. Tar measurement was carried out to determine the tar
concentration and tar conversion, respectively. The tar measurement method is
based on the tar protocol given by Neeft et al. (15). Further details are given by
Pfeifer (16). The combustion of propane in the AR serves as the heat source to cover
the heat demand in the FR whose global reaction is endothermic. Generally, the
gaseous species in the FR undergo CO-shift and reforming reactions,
Reactions (a) – (c).
CO + H2O ←⎯ ⎯→
Cat . CO2 + H2 ΔHR,850°C = -33.6 kJ/mol (a)
CxHy + xH2O ⎯⎯→ ⎯
Cat . xCO + (x+y/2)H2 ΔHR,850°C > 0 (b)
CxHy + CO2 ⎯⎯→ ⎯
Cat . 2xCO + (y/2)H2 ΔHR,850°C > 0 (c)
H2 + Fe2O3 ⎯
⎯→ H2O + 2FeO (d)
CO + Fe2O3 ⎯
⎯→ CO2 + 2FeO (e)
CxHy + Fe2O3 ⎯
⎯→ xCO2 + ½y H2O + (4x+y) 2FeO (f)
2FeO + ½ O2 ←
⎯→ Fe2O3 (g)
In parallel to the gas-gas reactions, CO, H2 or CxHy may be oxidised through partial
oxygen input by the oxygen carrier, Reactions (d) – (f). The oxidation-reduction
chemistry of iron is lumped into the formal expression FeO (FeII) and Fe2O3 (FeIII),
Reaction (g). The air reactor was fuelled with propane (C3H8) and air. A surrogate gas
mixture of H2 (52 vol.%), CO2 (40 vol.%) and CH4 (8 vol.%) was fed into the FR. The
surrogate gas mixture is related to product gas derived by steam gasification of
biomass, assuming that CO and H2O are formed in the FR, Reaction (a).
1-Methylnaphthalene (1-MN) was added as a tar model
compound to the FR gas feed. Thus, a strong reducing
atmosphere developed in the FR. The AR was
alternately operated at stoichiometric air/fuel ratios (λAR)
> 1 and < 1, resulting in O2 or CO excess in the AR
exhaust gas. Fig. 3 displays the experimental matrix.

Fig. 3. Experimental matrix
Fluid Dynamic Characteristics
Fig. 4 displays the pressure profile of the reactor system, which was about the same
for all the operation points. Due to the application of coarse particles compared to the
conventional particle size for circulating fluidised risers and the design particle size of
the DCFB reactor system, the exponential decay of pressure in the air reactor was
less developed. The pressure profiles (AR and FR) indicate the decrease of solid
concentration and the increase of voidage with reactor height, respectively. A low
solid circulation developed in the AR. For the FR, a high solid concentration was
found in the bottom region and the upper part was lean in solids. Fig. 5 highlights the
mapping of the fluidisation regime according to the map suggested by Bi and Grace
(17). The AR was operated slightly above the terminal velocity with superficial gas
velocity of ~ 4.5 m/s. A bubbling fluidised bed developed in the FR with a U/Umf ratio
(superficial velocity/minimum fluidisation velocity) of 7 – 8 at a superficial gas velocity
of ~ 3.5 m/s.
Fig. 4. Pressure profile in the reactor Fig. 5. Fluidisation regime of FR and AR

system according to Bi and Grace (17)
Reaction and Conversion Behaviour
The mean residence time in the FR amounted to ~ 3 s. Further, the FR operated at a

mean gas hourly space velocity (GHSV) of ~ 1350 h-1. The FR exhaust gas
composition for OP1 to OP4 is highlighted in Fig. 6.
Fig. 6. FR exhaust gas composition, mean Fig. 7. Mapping of oxygen transport and gas
values and standard deviation of conversion (logarithmic deviation from
measurement CO-shift equilibrium)
Due to nitrogen fluidisation of the loop seals and argon flushing of the pressure
measurements, the FR exhaust gas stream was diluted by about 25 vol.%db. OP1
was taken as the benchmark point and was characterised by highly developed
oxygen transfer. The restricted oxygen transport which developed in OP2 (AR
operation with CO excess) resulted in a considerably different exhaust gas
composition compared to OP1, see Fig. 6. CO and H2 were partially oxidised towards
CO2 and H2O. Compared to OP1, the CO content increased to about 45% and the H2
content increased to about 41% during OP2. The shift in CO, CO2 and H2 indicates
partial oxygen transfer with selectivity towards the oxidation of CO and H2. The
content in CH4 was marginally influenced. Tar feed (13.3 g/Nm³) was performed
within OP3 at λAR > 1. The feed of the tar compound (C11H10) caused a shift in gas
composition, since the total input in carbon and hydrogen increased. Based on OP1,
the content of H2, CO and CH4 increased. The content in CO2 decreased, since the
relative amount of oxygen was lowered by the hydrocarbon feed. However, the gas
composition was further affected by the overall reaction behaviour and the solids.
Limited oxygen transfer developed in OP4 (AR operation with CO excess). Hence,
the partial oxidation of CO and H2 was disabled. Thus, the relative contents in CO2,
CO and H2 shifted. Evaluation of process data using a data reconciliation method for
fulfilment of mass and energy balances was carried out, Bolhàr-Nordenkampf et al.
(18). Thus, the oxygen transfer in the reactor system is specified. Further, the
logarithmic deviation from CO-shift equilibrium was determined to rate the gas
conversion, Eq. (1).
⎡ ∏ pi ⎤
1000
pδ eq ( p i , T ) = log 10 ⎢⎢ i ⎥
Eq. (1) K P ,CO −shift = −1.6164 + 1.7632 ⋅ Eq. (2)
K P (T ) ⎥ T [K]
⎢⎣ ⎥⎦
The actually measured gas phase partial pressure of the species i is expressed as pi.
Kp is the equilibrium constant calculated from pure substance thermodynamic data as
a function of temperature, according to Eq. (2), derived by (19). Oxygen transfer and
deviation from CO-shift equilibrium are highlighted in Fig. 7. In each case (OP3 and
OP4), three tar samples were taken. Thus, in contrast to OP1 and OP2, three values
for oxygen transfer and pδeq are given for OP3 and OP4. Thus, the values
correspond to the tar sampling time. Generally, the oxygen transfer was lowered in
the case of CO excess in the AR. However, the oxygen transfer was not completely
inhibited. The total solid inventory ha a certain quantity of oxygen available, which
was present in different iron oxidation states and was released with advancing
operation. Despite the substoichiometric oxygen supply (CO excess in the AR
exhaust gas), oxidation of iron might occur, but at lower quantities. Furthermore, the
oxygen transfer capacity decreased, since particle attrition minimised the total solid
inventory. It is generally found that (Fig. 7):
oxygen transfer (during OP2) was reduced to about 30% compared to OP1
similar reduction comparing OP3 and OP4, but at lower quantities
Fig. 8. Tar feed and tar measurement FR
The CO-shift was close to equilibrium for OP1 and OP2 (Fig. 7), but showed minor
values above zero. Hence, the actual state of the exhaust gas composition was
slightly on the side of the products, Reaction (a). Lower oxygen transport (OP2)
resulted in a shift towards the equilibrium state. Thus, the oxidation caused by
oxygen transfer dominated the product side of the CO-shift reaction (CO2 content
increased). Considerable deviation in CO-equilibrium was found for the operation
points with tar feed. The shift from the equilibrium state proceeded towards the
product side (CO2 and H2), (pδeq.~ 0.25, deviation of about 75%). The results of tar
measurement (three measurements per operation point) are summarised in Fig. 8.
The graph depicts the amount (logarithmic scale) of tar compound feed (1-MN), the
residual tar content in the FR exhaust gas (according to GC/MS and gravimetric
method) and the content of 1-MN (unconverted part) in the FR exhaust gas. The tar
feed ranged from 13.3 to 13.9 g/Nm³, due to fluctuation of the pumping system. 1-MN
was converted to about 99%, since residual contents of 1-MN below 0.1 g/Nm³db
were measured. Certain hydrocarbons were subject to re-combination. Thus, heavy
tars (GC/MS undetectable) were formed. The mean gravimetric tar content for OP3
was about 1.6 g/Nm³db. A lower content of about 1.3 g/Nm³db was found for OP4 with
a decreasing tendency during the operation point. The amount of GC/MS detectable
tars ranged from 3.5 to 4.0 g/Nm³db. Hence, the conversion amounted to roughly 73%.
The major part (~94 wt.%) of the GC/MS detectable tars was naphthalene (C8H10).
The minor part (~6 wt.%) consisted of intermediate products of decomposition
(1H-indene, 1-benzothiophene, acenaphthylene and 2-methylnaphthalene).
CONCLUSION
The investigation focused on the reforming activity (tar conversion) and influence of
partial oxygen transfer. A surrogate gas mixture with 1-Methylnaphthalene as a
model tar compound (related to the product gas derived by biomass steam
gasification) was exposed to the catalytically active material Fe-olivine. Thus, the
performance was studied under ash, chlorine and sulphur-free conditions. It was
found that the catalyst acted as an oxygen carrier. It was assumed that FeIII (hematite)
was reduced to FeII (wustite) in the FR. However, Fe3O4 (magnetite) might occur as
part of the reduction-oxidation chemistry. The oxygen transfer to the fuel reactor was
influenced by modification of the air reactor operation (O2 or CO excess in the air
reactor exhaust gas). Complete prevention of oxygen transfer was not achieved,
since the total solid inventory possessed a certain quantity of oxygen which was
bound as iron oxides and was not entirely reduced during the operation time. Further,
iron oxidation occurred unavoidably to a certain quantity, due to contact of the solids
with the oxygen-containing fluidisation agent (propane and air). However, it was
found that CO and H2 were oxidised towards CO2 and H2O, respectively. The
oxidation selectivity was highly developed towards CO and H2, since it was found
that tar reduction was marginally influenced by partial oxidation. The 1-MN was
decomposed to 99 wt.%. However, full hydrocarbon decomposition was not achieved,
since further hydrocarbons were generated by recombination. The tar conversion
based on GC/MS measurement was approximately 73%, containing mostly
naphthalene. Naphthalene is a representative of aromatic ring hydrocarbons and is
therefore difficult to open due to the bonds of the aromatic rings. Hence, the catalyst
activity was classified in the medium to high range. It is suggested that the iron did
not act as a CH4 reforming catalyst, but CH4 was a product of tar conversion. The
overall hydrocarbon reforming capacity of Fe-olivine might be influenced by the
occurring iron state at the particle, since it has been reported by Nordgreen et al. (20)
and Virginie et al. (12) that metallic iron is obviously active in reforming and cracking.
Thus, a further activity upgrade is might be achieved (i.e. long term behaviour).
Moreover, the Fe-olivine catalyst featured the CO-shift equilibrium. This aspect is
corroborated by the findings of Rhodes et al. (21), who reported that iron oxide is a
catalyst for CO-shift.
ACKNOWLEDGMENTS
The authors gratefully acknowledge the financial support granted by the European
Commission, Contract No. 211517 (www.uniqueproject.eu). We sincerely thank the
Notified Testing Laboratory at Vienna University of Technology for their support.
Christoph Varga and Klemens Marx are gratefully acknowledged for their support.
NOTATION
AR air reactor pδeq. logarithmic deviation from equilibrium

FR fuel reactor λ stoichiometric air/fuel ratio
1-MN 1-Methylnaphthalene Kp equilibrium constant
U superficial velocity, [m/s] pi partial pressure of gas species i
Umf minimum fluidisation Use superficial velocity at border between
velocity, [m/s] turbulent and fast fluidisation, [m/s]
Ut terminal velocity, [m/s] Uc superficial velocity at border between
bubbling and turbulent regime, [m/s]
REFERENCES
1. Dayton, D. A. Report NREL/TP-510-32815; National Renewable Energy

Laboratory (NREL) Technical Report: Golden, CO, (2002).
2. Yung, M. M.; Jablonski, W. S.; Magrini-Bair, K. A. Energy & Fuels (2009), 23,
pp. 1874–1887.
3. Devi, L., PhD Thesis, Technical University of Eindhoven, Netherlands, (2005).
4. Abu El-Rub, Z.; Bramer, E. A.; Brem, G. Ind. Eng. Chem. Res. (2004), 43, pp.
6911–6919.
5. Kuhn, J. N.; Zhao, Z.; Felix, L. G.; et al. Applied Catalysis B: Environmental,
(2008), 81, pp. 14 – 26.
6. Constantinou, D. A.; Fierro, J. L. G.; Efstathiou, A. M. Applied Catalysis B:
Environmental, (2010), 95, pp. 255–269.
7. Rapagna, S.; Jand, N.; Kiennemann, A.; Foscolo, P. U. Biomass and
Bioenergy, (2000), 19, pp. 187-197.
8. Rauch, R.; Pfeifer, C.; Bosch, K.; Hofbauer, H.; Świerczyński, D.; Courson, C.;
Kiennemann, A. Science in Thermal and Chemical Biomass Conversion
Conference, Victoria, BC, Aug 3rd−Sept 2nd, (2004).
9. Pecho, J.; Schildhauer, T.; Sturzenegger, M.; et al. Chemical Engineering
Science, (2008), 63, pp. 2465–2476.
10. Koppatz, S., Proell, T., Pfeifer, C., Hofbauer, H. Proceedings of the
Fluidization XIII Conference, May 16-21, (2010), Gyeong-ju, Korea, ISBN:
978-0-918902-57-3, pp. 901-908.
11. Virginie, M.; Courson, C.; Niznansky, D.; Chaoui, N.; Kiennemann, A. Applied
Catalysis B: Environmental, (2010), 101, pp. 90–100.
12. Virginie, M.; Courson, C.; Kiennemann, A. Comptes Rendus Chimie, (2010),
13, pp. 1319 – 1325.
13. Kolbitsch, P.; Pröll, T.; Bolhàr-Nordenkampf, J.; Hofbauer, H. Chem. Eng.
Technol. (2009), 32, pp. 398-403.
14. Pröll, T.; Kolbitsch, P.; Bolhàr-Nordenkampf J.; Hofbauer, H. AIChE Journal,
(2009) 55 (12), pp. 3255-3266.
15. Neeft, J. P. A.; Knoef, H. A. M.; Zielke, U. et al. “Guideline for Sampling an
Analysis of Tar and Particles in Biomass Producer Gas, Version 3.1; Energy
project EEN5-1999-00507 (Tar protocol)” (1999).
16. Pfeifer, C., PhD-Thesis, Vienna University of Technology (2004).
17. Bi, H. T.; Grace, J. R. Int. Journal of Multiphase Flow, (1995, 21, 1229-1236.
18. Bolhàr-Nordenkampf, J., Pröll, T., Kolbitsch, P., Hofbauer, H., Chem Eng
Technol. (2009), 32, pp. 410–417.
19. HSC Chemistry 6.1. Chemical reaction and eq. software, thermochem.
database and simulation module; oututec research Oy, Pori, Finland, 2008.
20. Nordgreen, T.; Liliedahl, T.; Sjöström, K. Energy & Fuels, American Chemical
Society, (2006), 20, pp. 890-895.
21. Rhodes, C.; Hutchings, G. J.; Ward, A. M. Catalysis Today, (1995), 23, pp.
43–58.
FAST PYROLYSIS PROCESS INTENSIFICATION: STUDY OF
THE GAS PHASE RESIDENCE TIME DISTRIBUTION AND
BACKMIXING IN A DOWNER REACTOR
Martin Huard, Franco Berruti and Cedric Briens

Institute for Chemicals and Fuels from Alternative Resources (ICFAR)
The University of Western Ontario
22312 Wonderland Road North, N0M 2A0, Ilderton, Ontario, Canada
ABSTRACT
A downer reactor was developed at ICFAR to maximize the liquid yield of pyrolysis in
the conversion of biomass and heavy oil feedstock. An experimental study using hot
wire anemometers was performed to measure the residence time distribution of the
gas phase in the reactor and around the gas-solids separator. Some gas backmixing
was observed around the gas-solids separator, which decreased with increasing
distance between the separator and the gas outlet.
INTRODUCTION
The Institute for Chemicals and Fuels from Alternative Resources (ICFAR) is
developing and testing reactor technology for the conversion of biomass and heavy
oil feedstocks to useful bio-oil, bio-char, syngas, and other valuable chemical
products via pyrolysis. Among the various biomass conversion processes developed
at ICFAR, a downer reactor was designed and manufactured for the pyrolysis of
biomass and heavy oil feedstocks to maximize the liquid yield. The downer
configuration was selected over other reactor types for careful control of thermal
cracking reactions and gas-solid contact times. To achieve these goals, a novel gas-
solids separator was developed and tested (1,2) specifically for the downer to quickly
and efficiently separate heat-bearing sand particles from product vapors. The
purpose of this study is to ensure that the separator does not introduce excessive
gas backmixing, which would degrade the downer performance.
Several gas phase RTD studies have previously been performed in circulating
fluidized bed (CFB) riser reactors (3,4,5,6). Most authors reported significant gas
backmixing in the riser and increased backmixing with increasing solids flux.
However, only Brust and Wirth (7) measured gas backmixing in a downer reactor
and found that backmixing was reduced at high gas velocities. Hence, in the present
study, the gas residence time distribution (RTD) and backmixing in the downer
reactor and around the gas-solids separator were investigated in the absence of
solids. A simple hot wire anemometry technique was developed to measure the
concentration of helium tracer in the model downer and around the gas-solids
separator. Some initial results of the study are presented to demonstrate the
applicability of hot wires in measuring the gas phase RTD.
BACKGROUND
Knowledge of the RTD in a reactor may be obtained by measuring the concentration

of a tracer in the reactor as time proceeds. Thin filament hot wire anemometers were
used in this study to detect the presence of helium tracer in air. These sensors detect
differences in the heat transfer characteristics of gas flow over the thin electrified
resistive film or filament. Heat generated by the resistive element must be dissipated
by the flowing gas, which results in decreased detector resistance or voltage. For
fluid flow past a resistive element, the heat balance for the hot wire is given by
⁄ = ℎ
− , (1)
where Vw is the voltage applied to the detector, Rw is the resistance of the detector,
hw is the heat transfer coefficient between the detector and the surrounding fluid, Aws
is the heat transfer surface area of the detector, Tw is the temperature at the surface
of the detector, and Tg is the gas temperature.
Variation in gas composition as the gas flows over the hot wire is detected in the
constant-voltage mode as a change in the probe resistance Rw. For most hot wire
filaments, the resistance is linearly related to the probe temperature in the form
= ∆ + , (2)
where ∆T = Tw - Tg and m and b are empirical coefficients of resistivity specific to the

filament material. Substituting Equation (2) in (1) and solving for ∆T gives
. (3)
Changes to ∆T in Equation (3) are due only to changes in hw and possibly to Vw if not
operated in constant-voltage mode. The hot wire may be treated as a smooth
cylinder, so that hw can be determined by the Churchill-Bernstein correlation (8) for
external cross-flow over a cylinder. For known gas properties, extreme values of Rw
may be calculated for pure carrier gas flow and for pure tracer. Measured values of
Rw between these extreme values represent mixtures of carrier and tracer, and the
concentration of tracer CHe may be inferred by interpolating in a theoretical curve of
Rw for different gas mixture properties.
The time-dependent input and output tracer concentration signals cin(t) and cout(t) are
related to the RTD function e(t) by the convolution integral:
! !
= ∗ = "! − = "! − , (4)
where t refers to the time domain and t1 is a shift of one of the functions relative to
the other in the time domain. In the present study, cin and cout were measured and
e(t) was unknown; hence, deconvolution was used to obtain the RTD function
between any two given concentration signals. A fast Fourier transform algorithm was
used to convert measured concentration signals to the frequency domain, where
deconvolution is simplest. After obtaining the RTD in the frequency domain, the
inverse Fourier transform was used to convert the RTD e(t) back to the time domain.
MATERIALS & METHOD
A model downer similar to the one used by Huard et al. (1) and Huard (2)
constructed of transparent acrylic was used to perform cold flow gas phase RTD
experiments as shown in Figure 1. The downer had an internal diameter of 6.99 cm
and a total height of 133.5 cm. The cone deflector was attached to an adjustable rod
to change the distance LS between the gas outlet and the cone rim from -1.40 cm to
6.99 cm. Values of LS < 0 indicated that the cone rim was below the gas outlet.
Figure 1 – Sketch of Experimental Model Downer
Compressed air was used as the carrier gas in the downer. Three calibrated sharp-
edged orifice nozzles with diameters of 0.20 cm, 0.22 cm, and 0.31 cm were used to
control the mass flowrate of air in the downer. The range of superficial gas velocities
Ug in the downer was 0.30 m/s to 1.27 m/s for the present study. A tracer injection
line was installed upstream of the downer as depicted in Figure 2. As shown in
Figure 2, air was permitted to flow into the downer inlet either through the tracer gas
injection line or the air bypass line.
Before injection, solenoid valves on the injection line were opened and the bypass
line was closed. Helium was then permitted to flow through the open injection line
and into the downer for about one minute to flush the injection line. Both solenoid
valves were then closed to trap tracer in the line. Next, the air bypass line was
opened with a slight restriction in the line for strong preferential flow to the injection
line during injection. Data logging was then initiated on the data acquisition system.
Finally, the tracer injection was performed by opening sequentially the solenoid
valves at the inlet and outlet of the injection line, respectively. The inlet valve was
first opened to equilibrate the pressure between the flowing air and the trapped
helium, while the outlet valve was opened about two seconds later to flush the
injection line with air and inject the helium pulse into the downer.
Figure 2 – Schematic Diagram of Experimental Apparatus
Three hot wire anemometers (Probes 1 to 3) were used to measure the

concentration of helium, whose approximate locations in the downer are shown in
Figure 2. Probe 1 was installed 5.1 cm below the downer inlet to measure the
incoming helium concentration signal. Probe 2 was located 16.5 cm above the gas
outlet just upstream of the gas-solids separator, and Probe 3 was located 47.0 cm
downstream of the entrance to the gas outlet. These detection points allowed
measurement of the RTD through the entire downer and across the gas-solids
separator. A 6.0 VDC regulated power supply was used to power each probe circuit,
which were operated in a mode similar to constant-voltage mode. This allowed for a
very simple electronic setup but slightly sacrificed probe sensitivity compared to
other standard operation modes. Each detector was connected in a Wheatstone
bridge circuit to increase the sensitivity of the detectors.
RESULTS & DISCUSSION
Effect of Gas Velocity
Gas phase RTD measurements were performed in the absence of solids to gain
insight into potential gas backmixing in the reactor and around the gas-solids
separator. The gas velocity Ug and separation length LS/D were adjusted to
understand their respective effects on the RTD in the downer. The effect of gas
velocity was investigated for the range of gas velocities Ug = 0.30 m/s to 1.27 m/s.
This range corresponded to average residence times of 3.9 s to 0.92 s between the
downer inlet and the gas outlet, and to residence times of 5.0 s to 1.2 s when also
including the reactor volume below the gas outlet. Hence, the gas outlet was an open
boundary through which the flow could penetrate.
Figures 3(a) and 3(b) show typical normalized helium concentration CHe curves
measured at Probes 1, 2, and 3 and the corresponding RTD curves for Ug = 1.05 m/s
and LS/D = 0. Concentration measurements were acquired at 500 Hz. Huard (2)
showed that maximum particle removal efficiency in the separator occurred at LS/D =
0 for the operating conditions expected in the actual pyrolysis process in the downer
reactor. Hence, this condition was of particular focus in the present study.
Figure 3 – Measured downer concentration signals and corresponding RTD curves

for Ug = 1.05 m/s and LS/D = 0
The RTDs shown in Figure 3(b), obtained by deconvolution of the concentration

signals, indicated some spreading and potential bypassing of the initial helium pulse
in the downer upstream of the gas-solids separator. This was indicated by a bimodal
RTD curve e1-2 (i.e. RTD between Probes 1 and 2) in Figure 3(b). A small secondary
peak was also observed in curve e2-3 as shown in Figure 3(b), which indicated some
backmixing around the gas-solids separator. Although future introduction of solids
would likely increase backmixing in the reactor, these initial results confirmed the
possibility to operate the downer close to the plug flow regime.
The severity of backmixing was gauged by analyzing the average residence time and
variance of the measured RTDs. Figure 4 shows the actual average residence time
and variance of the measured RTD curves for the range of tested gas velocities. As
shown in Figure 4(a), the measured residence times in the downer before the
separator were reasonably close to the nominal values calculated by dividing the
reactor volume by the volume flowrate, which confirmed near plug flow and use of
the deconvolution technique. Based on the RTD variance curves shown in Figure
4(b), the gas-solids separator was the major contributor to RTD spreading for all
tested gas velocities. This result indicated very little RTD spreading and backmixing
in the downer before the separator.
Another important indicator of reactor performance was the effective gas penetration
length LP. This indicator represented how far the gas “effectively” flowed past the gas
outlet based on the measured residence time compared to the nominal residence
time between the inlet and the gas outlet. In other words, measured residence times
longer than the nominal values gave LP > 0, indicating gas flow below the outlet.
Measured residence times shorter than the nominal values gave LP < 0, indicating
either no gas flow past the outlet or bypassing. The effect of gas velocity on LP is
shown in Figure 4(c). The results show that gas did not penetrate past the gas outlet
for velocities Ug ≤ 0.79 m/s, which corresponded to short durations in the gas-solids
separator. Long penetration lengths past the outlet were observed for gas velocities
Ug ≥ 1.05 m/s. Penetration past the gas outlet did not necessarily correspond to
backmixing, but the relative duration in the separator was much longer for LP > 0.
This result also indicated that future use of stripping gas below the gas outlet would
likely decrease the penetration length and separation time.
Figure 4 – Effect of Gas Velocity on Average Residence Time, Variance, and

Effective Penetration Length
Effect of Separation Length
The effect of separation length on the residence time, variance, and penetration
length in the downer was investigated over the range of LS/D = -0.2 to LS/D = 1.0.
The gas velocity was set at Ug = 1.27 m/s to represent the actual pyrolysis process
operating conditions. As shown in Figure 5(a), a modest increase in the residence
time with decreasing separation length was observed for 0 ≤ LS/D ≤ 1.0.
Considering also the gas-particle separation efficiency, which increased with
decreasing separation length to a maximum at LS/D = 0 for similar operating
conditions (2), the present results suggest that there may be a trade-off between
separation efficiency, residence time, and backmixing for optimum process
performance in the downer. However, for LS/D = -0.2, an enormous increase in the
residence time, variance, and penetration length was observed. This indicated very
significant backmixing below the gas outlet and gas flow reaching the solids outlet.
Hence, this operating condition must be avoided to achieve plug flow in the reactor
and to avoid pyrolysis product vapor degradation.
Figure 5 – Effect of Separation Length on Residence Time, Variance, and
Penetration Length
CONCLUSION
A simple hot wire anemometry technique was developed and used successfully to
measure the gas phase RTD in a downer reactor. The measured RTD curves show
near plug flow behavior in the downer for most tested operating conditions. Some
gas backmixing was observed around the gas-solids separator at high gas velocity
and for very short separation lengths. The most severe backmixing occurred for LS/D
= -0.2. The best operating conditions for near plug flow in the reactor were Ug = 1.27
m/s and for separation lengths LS/D ≥ 0.
NOTATION
Aws Hot wire heat transfer surface area [m2]
b Empirical coefficient of electrical resistivity [Ω]
CHe Normalized concentration of helium [-]
cin(t) Input tracer concentration [kg/m3]
cout(t) Output tracer concentration [kg/m3]
D Downer internal diameter [cm]
Dw Hot wire diameter [mm]

E(s) Residence time distribution function in the frequency domain [-]
e(t) Residence time distribution function in the time domain [-]
hw Heat transfer coefficient between the hot wire and the surrounding
fluid [W/m2K]
LS Vertical distance between gas outlet and cone deflector rim [cm]
m Empirical coefficient of electrical resistivity [Ω/K]
Rw Hot wire probe resistance [Ω]
s Frequency domain [s-1]
Tw Hot wire surface temperature [K]
Tg Ambient gas temperature [K]
t Time [s]
Ug Superficial gas velocity [m/s]
Vw Voltage applied to hot wire [V]
σ2 Variance [s2]
τavg Average residence time [s]
REFERENCES
1. Huard, M., Briens, C., Berruti, F. (2010) Experimental study of a novel fast gas-
solid separator for pyrolysis reactors. Int. J. Chem. Reactor Eng. 8, A134.
2. Huard, M. (2009) An investigation of a novel gas-solid separator for downer
reactors. M.E.Sc. Thesis. The University of Western Ontario, London, Ontario,
Canada.
3. Gauthier, T., Andreux, R., Verstraete, J., Roux, R., & Ross, J. (2005) Industrial
development and operation of an efficient riser separation system for FCC
units. Int. J. Chem. Reactor Eng. 3.
4. Smolders, K., & Baeyens, J. (2000) Residence time distribution of the gas
phase in dilute phase circulating fluidized beds. Powder Hand. Proc. 12(3),
265-269.
5. Dry, R. J., & White, C. C. (1989) Gas residence-time characteristics in a high-
velocity circulating fluidised bed of FCC catalyst. Powder Technol. 58(1), 17-
23.
6. Gauthier, T. (1991) Étude de la separation rapide dans un cyclone a co-
courant. Thèse de Doctorat. L’Université de Paris VI, Paris, France.
7. Brust, H., Wirth, K.-E. (2004) Residence time behavior of gas in a downer
reactor. . Ind. Eng. Chem. Res. 43(18), 5796-5801.
8. Churchill, S.W., Bernstein, M. (1977) A correlation for forced convection from
gases and liquids to a circular cylinder in cross flow. J. Heat Transfer, Trans.
ASME. 94, 300-306.
DEM-CFD MODELING OF A TOP-SPRAY FLUIDIZED BED
GRANULATOR AND A WURSTER-COATER
Lennart Fries1, Sergiy Antonyuk1, Stefan Heinrich1 and Stefan Palzer²
1
Institute of Solids Process Engineering and Particle Technology,
Denickestr. 15, 21073 Hamburg, Germany
T:+49-40-42878 2143; F:+49-40-42878-2678; E: lennart.fries@tuhh.de
² Nestlé Product Technology Centre York,

Haxby Road, York YO91 1XY, United Kingdom
ABSTRACT
Coupled DEM-CFD simulations were performed to study the fluid and particle dynamics
of a fluidized bed granulator on the micro-scale. In a first study, wetting of the particles
is estimated based on the residence time distribution inside a conical spray zone. The
effect of the geometry of the apparatus on the homogeneity of wetting is analyzed in
order to understand the performance and specificity of different granulator
configurations. For a small simulation system, heat and mass transfer laws were
resolved to calculate the moisture content of the individual particles An effective
modelling tool for design of a fluidized bed spray granulator is obtained.
INTRODUCTION
Fluidized bed spray granulation plays an important role in the manufacturing of powder
granules in the food and pharmaceutical industries as it allows producing dust-free and
free-flowing particles.
Liquid binder is sprayed into a bed of solids to achieve granule growth. A homogeneous
distribution of the spray liquid is a prerequisite for uniform growth, whereas local
overwetting leads to the formation of particle clusters. The moisture distribution in the
apparatus is a key parameter affecting both particle size and structure of the product
[1]. The fluid bed granulation process is controlled by many parameters which can
influence size and structure of the product. Since so far the choice of operating
conditions and the design of the equipment geometry have been made empirically, the
actual influence of the fundamental mechanisms in the process is not well understood.
To describe the process in detail on the scale of individual particles, the Discrete-
Element-Method (DEM) offers large potential. As each particle is tracked individually,
the method allows a complete representation of the particle-particle and particle-wall
interactions and their influence on the process dynamics.
MATHEMATICAL MODEL
The motion of each particle i in the system is calculated using Newton's second law:
Vi β g − p
mi
dv i
= −Vi ∇p + (u g − v i ) + mi g + Fc,i + FA,i (1)
dt 1− ε
The forces on the right hand side of Eq. 1 are respectively due to pressure gradient,
drag, gravity and contact forces (i.e. due to collisions). The interphase momentum
transfer coefficient βg-p is modeled by combining the Ergun equation [2] for dense
regimes (gas volume fraction ε < 0.8) and the correlation by Wen&Yu [3] for dilute
regimes (ε ≥ 0.8). The gas is considered as continuous phase. The geometry of the
apparatus is discretized in mesh cells and the flow profile is calculated using volume-
averaged Navier-Stokes equations.
∂
(ερ g ) + ∇(ερ g u g ) = 0 (2)
∂t
∂
(ερ g u g ) + ∇(ερ g u g u g ) = −ε ∇p g − ∇(ε τ g ) − S p + ερ g g (3)
∂t
Due to momentum exchange and the reduced free gas volume the particles influence
the velocity profile of the gas phase. This effect is accounted for by adding a sink term
Sp to the momentum balance, which closes the two-way-coupling. Forces between the
gas and particle phase are of opposite direction and equal magnitude. The flow around
particles is not fully resolved, as the size of the fluid mesh cells is 2-10 times larger than
the particle diameter.
Contact forces between particles are calculated according to a contact model (Eq. 4)
based on the theory developed by Hertz [4] for the normal impact. A no-slip
approximation of the model by Mindlin and Deresiewicz [5] is applied for the tangential
component of the contact force, as proposed by Tsuji et al. [6]. According to the
Hertzian theory [4], the relation between the elastic deformation and the displacement is
nonlinear, due to the elliptical pressure distribution in the circular contact area
Fc ,n = −k n ⋅ δ n ⋅ n ab − η n v ab,n
3
2
(4)
For the tangential component of the contact force Ft an equation analogue to Eq. 4 is
used [6]. Energy dissipation is included in the model using coefficient of restitution,
which is defined as the ratio of the square root of the elastic strain energy Ekin,r released
during the restitution to the impact energy, i.e the initial kinetic energy Ekin [7]:
E kin ,r vr
en = = (5)
E kin v
The coefficient of restitution can be determined experimentally with a free-fall tester.
Model of the spray zone
The spray injection is represented in the form of a conical zone starting from the nozzle
tip, where the suspension is injected. All particles inside the spray zone are wetted. As
a first approximation, the wetting intensity is supposed to be homogeneous in the entire
spray zone. By integrating over the particle trajectories, their residence time inside the
spray zone is obtained, which allows estimating their moisture content.
In a second step, the model of the spray is refined by taking into account the distance
between particle and nozzle tip and the local solids volume fraction. Particles in the
spray zone are assigned to discrete levels (see Fig. 1).
Fig. 1. Discretization scheme of the spray Fig. 2. Heat and enthalpy streams on the
zone. particle surface.
Starting from the nozzle tip at level j = 1, the suspension is deposited on the particles
according to the ratio of the projected area of the particle to the total area of level j,
according to Eq. 6. Suspension that is not deposited on level j is passed to level j+1.
A ,i
M& susp ,i = M& susp
j
⋅ pp
j
(6)
Alevel
j +1
 ∑ App ,i 
M& susp = M& susp
j
⋅  1 − j 
(7)
 Alevel 
Suspension, which has not been deposited until the last level of the nozzle is supposed
to leave the system as overspray.
Modeling of heat and mass transfer
By applying heat and mass transfer laws, the moisture content and temperature of each
individual particle can be calculated. It is assumed that suspension deposited on a
particle spreads on its surface and forms a film with constant thickness Lfilm of 0.1 mm.
Penetration into pores and wetting of the particle core are neglected. Deposition and
evaporation of liquid influence the size of the wetted area Afilm. If the entire particle
surface is wet, it will not absorb further suspension. The enthalpy and heat streams
considered in this model are shown schematically in Fig. 2. The liquid film interacts with
the particle and the gas phase, which is expressed through the enthalpy balance:
dH film
= H& susp + Q& pf − H& vap + Q& af (8)
dt
Evaporation of liquid will change the mass of the film. The evaporation rate depends on
the mass transfer coefficient β, which is a function of the relative velocity between
particle and fluid. The vapor mass flow from a particle surface is calculated:
M& vap = β ⋅ A film ⋅ (Ysat − Ya )
(9)
Heat transfer between the gas phase and the liquid film is described with the help of
& = α ⋅ A ⋅ (ϑ − ϑ )
Q af af film a film (10)
For dry zones on the particle surface the heat exchange between the particle and gas
phase is described using
Q& = α ⋅ (A − A ) ⋅ (ϑ − ϑ )
ap ap p film a p
(11)
The current contribution does not include particle growth or agglomeration.
SIMULATION CONDITIONS
In order to describe the mechanical behavior of the material (spherical γ-Al2O3 granules
loaded with solid) the input parameters for the contact model were determined
experimentally. By image analysis, the impact and rebound velocity as well as the
rebound angle and the rotational speed of the particle were determined. According to
results by Antonyuk et al. [7], a constant coefficient of restitution of 0.8 for γ-Al2O3
granules was used in the simulations. See Table 1 for all parameters of the model.
Table 1: Overview on simulation parameters.

Parameter Value Parameter Value
Fluidization vel. annulus 4 m/s = 3.7·umf Poisson ratio 0.25
Fluidization vel. Wurster 11 m/s = 10·umf Static friction coeff. 0.1
Fluidization vel. top-spray 5.5 m/s = 5.1·umf DEM time step 2·10-6 s
Nozzle injection rate 7 m³/h CFD time step 2·10-4 s
Fluidization air flow rate 600 m³/h Air temperature 75 °C
Wurster gap distance 15 mm = 5·dp Particle heat capacity 900 J /kgK
Normal rest. coefficient 0.8 Suspension spray rate 5·10-5 kg/s
Shear modulus 1·108 Pa Liquid film thickness 0.1 mm
For two different granulator configurations the residence time distribution of the particles
inside the spray zone was analyzed. As shown in Fig. 4a, the injection nozzle can be
positioned above the bubbling fluidized bed (top spray). Another common configuration
is the Wurster-coater [8], where a cylindrical draft tube is inserted vertically into the
granulator, as shown in Fig. 4b. Combined with a bottom-spray injection nozzle, the
Wurster geometry induces a circulating movement of the particles. The draft tube
physically separates the wetting zone at the center from the drying zone in the annulus.
Simulations were performed with 45,000 spherical particles and a particle diameter of
3 mm, which corresponds to a batch size of 0.95 kg at a particle density of 1500 kg/m³.
The geometry of the GF5-insert used in the simulations was supplied by Glatt
Ingenieurtechnik GmbH, Germany. The outer dimensions of the top-spray granulator
are identical to those of the Wurster-coater. The same fluidization air flow rate and
nozzle injection rate is used in both configurations. While the top-spray granulator has a
homogeneous distributor plate with constant porosity, the bottom plate of the Wurster
coater consists of 2 segments with different porosity. With the help of pressure drop
correlations the flow rate in both segments of a Glatt GF3 insert was approximated. The
nozzle injection rate in the simulations was set according to the used experimental
device (Schlick type 970).
a) b)
Fig. 4: Configurations of a fluidized bed granulator: (a) top-spray, (b) Wurster-coater.
For a precise investigation of particle wetting and drying in a top-spray granulator, the
calculation of heat and mass transfer was coupled with the DEM-CFD simulation. Due
to the higher numerical effort, a small system with 10,000 particles was analyzed,
where the particle properties were identical to those given in the previous section. The
simulation allows monitoring the moisture content and temperature of each individual
particle. Based on the gas flow profile obtained from the CFD model, local heat and
mass transfer coefficients are calculated.
SIMULATION RESULTS
The particle and fluid dynamics of both granulator configurations have been studied. In
the Wurster-coater the particles move at high velocity inside the draft tube. A relatively
low injection depth of the spray nozzle of approximately 45 mm was found. Obviously,
the momentum of the jet is quickly transferred to the particles. In the top-spray
granulator the average gas velocity is lower than in the Wurster configuration. A
stagnant zone can be seen above the counter current injection nozzle.
Residence time distribution
For the Wurster-coater configuration, the residence time of the particles inside the spray
zone is primarily determined by the upflow velocity of gas and particles in the draft tube.
Once a stable circulating regime is established, the particles are transported through
the spray zone at constantly high velocity (driven by the spout), which corresponds to a
well-defined residence time and homogeneous wetting of the particles. For the given
process conditions the residence time distribution obtained after 5 s simulation time is
shown in Fig. 5. A clear peak at 22 ms for particles which have passed once through
the spray zone and smaller peaks at multiples of this period are found. If the simulation
is continued, the distribution will continuously shift to the right with time.
For the top spray configuration a different picture is obtained (see Fig. 6). Since there is
no directed flow profile as in the Wurster-coater, the particle trajectories are randomly
influenced by the high number of individual collisions in the fluidized bed. This leads to
a wide residence time distribution of the particles in the spray zone, which corresponds
to inhomogeneous wetting. Some particles spent up to 5 % of the simulation time inside
the spray zone, whereas 30 % were not wetted at all.
a) b)
simulation time t = 2.5 s simulation time t = 2.5 s
4000 simulation time t = 5.0 s 4000 simulation time t = 5.0 s
number of particles N (-)
number of particles N (-)

3000 3000
2000 2000
1000 1000
0 0
0.00 0.04 0.08 0.12 0.16 0.20 0.00 0.04 0.08 0.12 0.16 0.20
residence time (s) residence time (s)
Fig. 5: Residence time distribution in the Fig. 6: Residence time distribution in the
spray zone for the Wurster-coater. spray zone for the top-spray granulator.
Simulations including heat and mass transfer
Temperature and moisture content of the individual particles as well as temperature and
humidity profiles of the gas phase in the apparatus can be calculated.
Initially all 10,000 particles are dry. Following the continuous liquid injection, more and
more particles are wetted. Accordingly, the peak in Fig. 7 is shifted to the right with
time. Due to inhomogeneous wetting, the particle moisture distribution gets broader.
After 30 s simulation time the wetting/drying equilibrium is reached.
gwater / kg dry air
10.2
10.1
10.0
30
20 20
10
5 10 15
Time [s] 0 0
height [cm]
Fig. 7: Particle moisture distribution. Fig. 8: Humidity profile of the gas phase.
In Fig. 8, the humidity of the gas phase is presented as a function of the height of the
granulator and time. Due to evaporation, the humidity increases steeply with the height
of the apparatus and slowly with time.
EXPERIMENTAL RESULTS
Experimentally the effect of different granulator configurations on the agglomeration

behavior of spray dried glucose syrup in a fluidized bed (Glatt GCPG 3.1) was studied.
The geometry of the fluidization chamber is the same in both cases, only the position of
the nozzle was varied and the draft tube was inserted for the bottom spray case. Pure
water was injected as binder and all operating conditions were kept constant.
While a narrow particle size distribution of the agglomerates is obtained with the
Wurster-coater, the size distribution of the product from the top spray granulator is
much broader. In the top spray granulator more oversize agglomerates are built. The
experimental results of the particle size distribution (Fig. 9) correspond very well with
the residence time distributions of the particles in the spray zone found in the numerical
simulations (Figs. 5 and 6).
0,0035
The simulations showed that
0,0030 the top spray configuration had
an inhomogeneous residence
d / 1/µm
0,0025 time of the particles in the

20% water (wb), liquid flow rate
density distribution q3 (a)
30g/min; bottom spray + Wurster spray zone indicating

0,0020 tube
unfavorable wetting.
0,0015 This is reflected by the broad
size distribution of the
0,0010 produced agglomerates. The
20% water (wb), liquid flow rate
30g/min; top spray Wurster-coater had a narrow
0,0005
residence time distribution,
0,0000 which matches well with the
0 500 1000 1500 2000 shape of the particle size
particle diameter d
a / µm
distribution of the agglome-
Fig. 9. Comparison of the agglomerate size distribution rates.
obtained in two different granulator configurations.
CONCLUSIONS
For two different granulator configurations the homogeneity of the liquid distribution
among the particle phase was investigated numerically on the scale of individual
particles with the help of coupled DEM-CFD simulations. The residence time distribution
of the particles in a conical spray zone at the tip of the injection nozzle allows estimating
their moisture content. The results show that the Wurster-granulator is characterized by
a narrow residence time distribution, whereas the top spray configuration leads to a
wide residence time distribution. The positive effect of a Wurster tube on the distribution
of the spray liquid seen in the DEM-CFD simulations was approved by agglomeration
experiments. Coupled with heat and mass transfer relations, the DEM-CFD model
allows the direct calculation of the temperature and moisture content of the individual
particles and the gas phase in a fluid bed granulator.
ACKNOWLEDGEMENT
We would like to thank Nestec S.A. for the financial support and Dr.-Ing. Michael Jacob
from Glatt Ingenieurtechnik GmbH, Weimar for the supply of geometry data.
NOTATION
A area m² n normal unit vector -

e coefficient of restitution - p pressure Pa
Ekin kinetic energy J Q heat stream W
F force N Sp momentum sink term N m -³
g gravitation m s-2 t time s
H enthalpy J u gas velocity m s-1
k stiffness N m-1 v particle velocity m s-1
m mass kg V volume m³
Ṁ mass flow kg s-1 Y gas moisture content -
α heat transfer coeff. Wm-2K-1 ε porosity -

β mass transfer coeff. m s-1 η damping coefficient Nsm-1
βg-p momentum transfer coeff. kgm-3s-1 ρ density kg m-3
δ displacement (overlap) m τ gas phase stress tensor Pa
REFERENCES
[1] Palzer, S.: Influence of material properties on the agglomeration of water-soluble

amorphous particles. Powder Technology 189 (2), 2009, 318-326.
[2] Ergun, S.: Fluid flow through packed columns. Chemical Engineering Progress 48,
1952, 89–94.
[3] Wen, Y.C. Yu, Y.H.: Mechanics of Fluidization. Chemical Engineering Progress
Symposium Series, 62, 100-111.[4] Hertz, H. Über die Berührung fester elastischer
Körper. Journal für die Reine und Angewandte Mathematik 92, 1882, pp. 156-171.
[5] Mindlin, R.D., Deresiewicz, H.: Elastic spheres in contact under varying oblique
forces. Transactions of ASME, Ser. E. J. of applied Mechanics 20, 1953, pp. 327-344.
[6] Tsuji, Y., Tanaka, T., Ishida, T.: Lagrangian numerical simulation of plug flow of
cohesionless particles in a horizontal pipe. Powder Technology 71, 1992, pp. 239-250.
[7] Antonyuk, S., Heinrich, S., Tomas, J., Deen, N.G., van Buijtenen, M.S. and J.A.M.
Kuipers: Energy absorption during compression and impact of dry elastic-plastic
spherical granules. Granular Matter 12 (1), 2010, pp. 15-47.
[8] Wurster, D. E.: Particle Coating Process. U.S. Pat. No. 3253944, May 31, 1966.
DESIGN REQUIREMENTS FOR
PRESSURIZED CHEMICAL LOOPING REFORMING
K. Marx, T. Pröll and H. Hofbauer
Vienna University of Technology, Institute of Chemical Engineering,
A-1060 Vienna, Austria
ABSTRACT
A key issue in chemical looping reforming is to operate the process under

pressurized conditions. Applicability of dual fluidized bed systems, currently used in
atmospheric chemical looping processes, is affected by pressure. Critical design
issues were studied and experimentally verified by cold flow model experiments. It
turns out that it is important to achieve sufficient global solids circulation and to keep
the pressure difference between the reactors low enough for proper operation of the
loop seals.
INTRODUCTION
Hydrogen is an important raw material for production of basic chemicals, in oil

refining, and many other industrial applications. Although naturally occurring, most
of the hydrogen used is produced from fossil raw materials (1). Catalytic steam
reforming of hydrocarbons is currently the cheapest way to produce hydrogen and
accounts for more than 90% of the world’s hydrogen production. In such systems
heat transfer is a key issue to improve the process performance (2).
H2, CO,
Chemical looping combustion (CLC) recently attracted N2, (O2) (CO2, H2O)
interest as a carbon capture technology. A variant of
the process is chemical looping reforming (CLR)
where less oxygen than required for complete MeOa
combustion is supplied. In chemical looping two Air Fuel
separate reaction zones, an air reactor (AR) and a fuel Reactor Reactor
(AR) MeOa-1 (FR)
reactor (FR) are available. A metallic solid is kept in
circulation between the reactors, usually called
oxygen carrier (OC). The solids are used to transport air/fuel ratio < 1
oxygen and heat and, especially in CLR, also act as a
Air Fuel
reforming catalyst. While in CLC full conversion of the
fuel is intended, a syngas is produced in CLR. Fig. 1 Chemical looping
reforming principle
The CLC process has been intensively studied over the recent years (3-4). Many
different oxygen carrier materials have been tested (3-5) and the technology has
been demonstrated for more than 1000h (6) and at scales of up to 150kW (7). Dual
fluidized bed (DFB) systems have been applied to the process claiming to fit the
requirements of chemical looping the best (8-9).
Nickel based oxygen carriers are beneficial in CLR because of their high catalytic
activity towards methane steam reforming. Promising results have been obtained
with such oxygen carriers at atmospheric conditions (10-11). Thermodynamic
equilibrium has been reached and no coke formation has been observed even at
very low steam to carbon ratios in the FR feed. Pröll et.al. (11) addressed the main
advantages of CLR compared to catalytic steam reforming to be:
• Heat required in the reactions is supplied inherently, no external heating is

needed, thus no heat transfer limitations are expected.
• Less steam is required.
• Fewer concerns with respect to sulfur contaminants (12).
A key issue in CLR is to operate the process at pressurized conditions (PCLR). Dual
fluidized bed systems have never been applied to pressurized systems.
Considerable operational limitations occurring from reactor pressure difference and
solids throughput are expected. In this study limitations occurring from pressure
were addressed and critical design issues in PCLR were identified. Cold flow model
tests at conditions corresponding to pressurized conditions were carried out in an
atmospheric dual circulating fluidized bed system.
CHEMICAL REACTIONS
The main reaction occurring in the air reactor is the oxidation of the oxygen carrier
which is in case of a nickel based oxygen carrier:
1
𝑁𝑖 + 𝑂2 ⇌ 𝑁𝑖𝑂 ∆𝐻𝑅900°𝐶 = −234.6 𝑘𝐽⁄𝑚𝑜𝑙 ( reac. 1)
2
The situation inside the fuel reactor is governed by many reactions taking place in
parallel or consecutively. The most relevant catalytic activated gas-phase reactions
are the steam reforming and CO-shift reactions. Which, for methane will be:
𝐶𝐻4 + 𝐻2 𝑂 ⇌ 𝐶𝑂 + 3𝐻2 ∆𝐻𝑅900°𝐶 = 225.6 𝑘𝐽⁄𝑚𝑜𝑙 ( reac. 2)
900°𝐶 ( reac. 3)
𝐶𝑂 + 𝐻2 𝑂 ⇌ 𝐶𝑂2 + 𝐻2 ∆𝐻𝑅 = −33.1 𝑘𝐽⁄𝑚𝑜𝑙
The heat needed is supplied either by oxidation of reforming products or fuel with
the metal oxide, or by the circulating solids transporting heat from the AR to the FR.
𝐶𝐻4 + 𝑁𝑖𝑂 ⇌ 𝐶𝑂 + 2𝐻2 + 𝑁𝑖 ∆𝐻𝑅900°𝐶 = 211.6 𝑘𝐽⁄𝑚𝑜𝑙 ( reac. 4)
𝐶𝑂 + 𝑁𝑖𝑂 ⇌ 𝐶𝑂2 + 𝑁𝑖 900°𝐶 ( reac. 5)
∆𝐻𝑅 = −47.2 𝑘𝐽⁄𝑚𝑜𝑙
𝐻2 + 𝑁𝑖𝑂 ⇌ 𝐻2 𝑂 + 𝑁𝑖 ∆𝐻𝑅900°𝐶 = −14.0 𝑘𝐽⁄𝑚𝑜𝑙 ( reac. 6)
Practically, in CLR just enough air will be supplied to the AR to keep the desired
operating temperature. The oxygen transport can be varied without influencing the
global heat balance if a fraction of the fuel is fed to the AR. In this way the oxygen
transport can be theoretically reduced to zero. From the principle of Le Chatelier it is
evident that in equilibrium the methane content decreases with increasing
temperature and higher steam ratios, and the methane content increases with
pressure. Thus to improve the methane conversion high temperatures, high excess
steam and low pressure are favorable. Compared to conventional catalytic methane
steam reforming methane breakthrough at increased pressure can be avoided by
increasing the FR temperature in PCLR.
CHALLENGES AT INCREASED PRESSURE
With increasing pressure, the gas density increases while the solids properties
remain unchanged. This means that, for a certain gas mass flow rate, either the riser
cross section or the superficial gas velocity will decrease with increasing pressure,
both resulting in lower solids entrainment rates. The main challenges with respect to
pressurized chemical looping reforming therefore are:
• The higher gas-solids reaction intensity.

• The fluidizing velocities must be kept within reasonable limits.
• The increased solids flux.
• Proper sealing between the reactors by the loop seals.
AR off-gas recycling is necessary to product gas

limit the solids throughput per cross
section area in the AR as depicted in
MeOa
Fig. 2. The power demand of the
recycle blower is expected to be low AR MeO FR
because of the low compression a-1
pressure ratio. Anyhow, the recycle htx.

gas stream has to be kept low to
reduce the energy penalty from gas re- blower fuel at
heating. This requires optimization of pressure
the ratio of solids circulation rate
relative to gas velocity in the AR riser.
to heat rcovery
The loop seals have to be designed ambient air
considering dynamic backpressure Fig. 2 Proposed PCLR arrangement.
changes from the two exhaust lines. Therefore,
deep loop seals which can handle significant level
changes are required. In addition an active control
setup of the backpressure is necessary for proper
operation of the system.
EXPERIMENTAL
An existing dual circulating fluidized bed cold flow

model (CFM) erected to study the dual circulating
fluidized bed (DCFB) concept for chemical looping
at atmospheric conditions (13) was modified and
operated at conditions simulating pressurized
conditions. A schematic drawing of the cold flow
model is shown in Fig. 3. The system includes two
risers, the air reactor and the fuel reactor, and
three loop seals, the upper-, lower-, and internal
loop seal. The CFM is a model of the existing hot
120 kW chemical looping pilot unit at Vienna
University of Technology at a scale of 1:3. It is
built of transparent acrylic glass allowing visual
observation of the fluid dynamic pattern. 23
pressure probes were placed and connected to a
personal-computer assisted measurement
equipment. Solids circulation rates are measured
by stopping the loop seal fluidization and
measuring the rate of solids accumulation inside Fig. 3 Sketch of the DCFB CFM
the appropriate downcomer. More specific details with pressure measure-
about the cold flow model can be found elsewhere ment ports indicated by
(13). dots.
The Glicksman criteria (14) Table 1 Characteristic design parameters of the
are a set of dimensionless system
numbers which are used to Hot unit CFM
Unit
maintain hydrodynamic ARH FRH ARC FRC
similarity in the cold flow Type of gas air syngas air air -
model and the Reactor inner
50 51 50 54 mm
corresponding hot unit. diameter
The necessity of gas-solids Superficial gas 6 3 5.75 9 m/s
density ratio similarity velocity
requires very light weight Operation 10 10 1.013 1.013 bar(a)
particles to simulate pressure
pressurized conditions in Operation 1000 900 25 25 °C
the atmospheric CFM temperature
fluidized with air. For good Particle Ni/NiO
agreement with the definition 40wt% NiO Polystyrene -
60wt% NiAl2O4
Glicksman criterion
Particle mean
polystyrene particles were 120 110 μm
diameter
used with a density of
Particle
1050 kg/m³ and a Sauter 3250 1050 kg/m³
density
mean diameter of 110 µm.
Spericity 0.99 0.99 -
To avoid buildup of
electrostatic forces ATMER 163, an anti-static agent, was added. The dimensions of
the hot unit are subjected to detailed mass and energy balance investigations of a
150 kW methane input pilot PCLR unit operated at 10 bar(a) pressure where
equilibrium of the reactions is reached theoretically. The dimensions and important
parameters of the hot unit as well as the corresponding cold flow model are
summarized in Table 1. For the given CFM geometry only the air reactor agrees well
with similarity rules, shown in Table 2. Considering that the FR flow regime has a
minor effect on the global system loop (13) the cold flow model can be used for
investigating the behavior of the global solids loop with little error.
Table 2 Comparison of dimensionless groups

Hot unit Cold unit Hot/Cold
Parameter Definition
ARH FRH ARC FRC AR FR
𝑑𝑝 ∙ 𝑈0 ∙ 𝜌𝑔 ∙ 𝜓
Rep 39.3 15.5 40.4 63.2 0.97 0.24
𝜂𝑔
𝜌𝑔 ∙ �𝜌𝑝 − 𝜌𝑔 � ∙ 𝑑𝑝 3 ∙ 𝑔
Ar 65.3 7.6 48.1 48.1 1.35 0.16
𝜂𝑔 2
𝑈0 2 4 4 4 4
Fr 3.0∙10 7.5∙10 3.0∙10 7.5∙10 1 1
𝑔 ∙ 𝑑𝑝
density 𝜌𝑝
𝜌𝑔 1265.8 2355.3 903.9 903.8 1.4 2.6
ratio
diameter 𝐷
416.7 425 454.5 490.9 0.92 0.87
ratio 𝑑𝑝
spericity 𝜓 0.99 0.99 0.99 0.99 1 1
Observed pressure profiles
The pressure profile of fluidized beds can be used to identify design problems and to
determine the solids distribution within the system. A typical pressure profile of the
CFM in operation is shown in Fig. 4. The 1600
low density of the particles used caused AR cylone
that the observed overall pressures are 1400
relatively low in the range of 15 mbar. AR
The solids distribution curve of a typical 1200
circulating fluidized bed has a lower FR cyclone
dense region and a lean upper section. 1000 AR downcomer
Height in mm
Derived from momentum balance it is
evident that in steady-state conditions the 800
decay of the pressure profile indicates the
ULS
solids inside the volume. Thus, typically a 600
FR downcomer
pressure profile in a CFB unit has a
shape of high pressure gradients at the 400
ILS
lower and low gradients at the upper
section. On the other hand in dilute phase 200 FR LLS
or pneumatic transport regime the solids
are equally distributed over the riser 0
height indicated by a nearly constant 0 5 10 15
pressure decay along height. The
pressure profile of the FR shows the Pressure in mbar(g)
typical shape of a CFB while the profile in Fig. 4 Typical pressure profile of the
the AR had a shape similar to the one of CFM with 0.5 kg total inventory
a pneumatic conveyor. This occurs and at following fluidization rates
because of the relatively low gas velocity in Nm³/h: AR 25/FR 5/LLS 0.5
in the FR and the high gas velocity and ULS 0.6/ILS 0.2
low solids inventory in the AR. In the DCFB concept three loop seals are needed.
Proper operating loop seals show a pressure drop in solids flow direction indicating
movement of solids and appropriate gas sealing. Operation stability of loop seals
towards pressure fluctuations between the loop seal inlet and outlet can be obtained
by increasing the pressure at the bottom of the loop seal. In the DCFB concept the
lower and upper loop seal are directly exposed to fluctuations and differences of
pressure between the two fluidized beds. For that reason deeper loop seals will
improve the operation stability of the system.
Impact of gas velocity
To study the effect of the AR fluidization the gas volumetric flow to the AR was
varied at constant FR and loop seal fluidization. Pressure profiles are shown in
Fig. 5. With increasing gas flow rate to the AR it was observed that the overall
pressure profiles were shifted towards a higher pressure which was caused by
increased back pressure from the filter bag and cyclone. It was also observed that
although the pressure profile of the AR was affected by gas velocity in the AR the
FR profile itself remained nearly unchanged. Inaccurate pressure probe placement
was detected at the bottom of the AR showing a discrepancy from the expected
pressure profile. Rearrangement of the probe has to be considered in further
investigations.
Results of solids circulation rate measurement are depicted in Fig. 6. At low flow
rates of 20 to 30 Nm3/h in the AR an increasing solids flux was observed while at
high fluidization velocities the solids flux decreased. This is in contrast to the
expected behavior that the solids circulation rate increases with fluidization rate.
One reason for this seems to be that 1600 AR20/FR5
the increasing back pressure from the AR30/FR5
filter bag with AR fluidization rate is 1400
AR40/FR5
affecting the actual solids inventory in
the AR. It might also be that due to
1200
the fact that the fluidization nozzles of
the AR are inclined downwards (Fig.
3) the dynamic pressure of the gas 1000
Height in mm
flow increases the back pressure at
the outlet side of the lower loop seal, 800
thus inhibiting solids flow. Fig. 6 also
shows that the AR fluidization rate 600
has only a minor effect on the FR
internal solids circulation rate which is 400
in agreement with the observed
pressure profiles and previous
200
investigations (13).
Impact of reactor outlet pressure 0

difference 0 5 10 15 20 25
Pressure in mbar(g)
To study the effect of reactor outlet
pressure difference the FR Fig. 5 Influence of AR fluidization on the
backpressure was changed by closing pressure profile at a total solids
or opening a valve placed after the inventory of 0.5 kg and following
dip tube of the FR cyclone. The CFM fluidization rates in Nm³/h: FR 5/
results are shown in Fig. 7. It was ULS 0.5/LLS 0.5/ILS 0.2
found that with increasing pressure difference the AR solids entrainment rate
increased nearly linearly with the pressure difference while the FR internal
15 20
Solids entrainment flux in kg/m²s
Solids enrtainment flux in kg/m²s
15
10
AR 10 AR
FR FR
5
5
0 0
20 30 40 0 1 2 3 4
AR fludization rate in Nm3/h Pressure difference in mbar(g)
Fig. 6 Influence of the AR fluidization Fig. 7 Influence of the riser outlet

on the solids circulation relative pressure difference on the
to reactor cross-section at a solids circulation relative to
total inventory of 0.5kg and the riser cross-section at a total
following fluidization rates in inventory of 0.5kg and the
Nm³/h: FR 5/ULS 0.5/LLS 0.5/ following fluidization rates in
ILS 0.2 Nm³/h: AR 25/FR 5/ULS 0.5 /
LLS 0.5/ILS 0.2
circulation rate remained unaffected. This can be explained by the increased driving
force for particle movement through the lower loop seal which is governed in the
DCFB concept by the solids inside the riser of the fuel reactor and the back pressure
from the fuel reactor exhaust line. It is important to note that when the pressure
difference between the risers is increased too far, solids accumulation in the
downcomer of the AR cyclone can lead to loop seal blockage by occurrence of a
slugging fluidized bed regime in the downcomer. On the other hand also emptying of
the upper loop seal can occur at inversed pressure differences. Generally, in
pressurized conditions, small relative backpressure changes can cause significant
changes in solids circulation and possibly lead to failure of loop seal operation. Deep
loop seals better resisting pressure difference fluctuations between loop seal inlet
and outlet can be part of a solution. In addition it seems that an automatic
backpressure control setup is inevitable for pressurized operation of a DCFB.
CONCLUSIONS
The chemical looping reforming process for autothermal steam reforming has shown
great potential at atmospheric conditions. To minimize the compression work
needed a key issue is to operate the process under pressurized conditions.
Pressurization influences the process from the chemical-, as well as from the
hydrodynamic point of view. Because of increased gas density the reactor cross
section area decreases resulting in increased gas-solids reaction intensity. To avoid
occurrence of critical solids flux values in the AR riser recycling of parts of the AR
off-gas is needed. This recycling gas stream should be kept low to decrease the
energy penalty from re-heating the recycle-gas. This has to be considered when
aiming for high process temperatures to improve the methane conversion.
Possible problems occurring at pressurized operation were indentified in a dual

circulating fluidized bed cold flow model. Proper operation of the loop seals placed
between the two risers requires controlling the pressure difference between the
reactors. High solids throughput and high pressure differences might lead to loop
seal feeding tube blockage or emptying of the loop seal. A pressurized system will
therefore be characterized by loop seals larger in both cross section and depth. It
was also found that increasing the back pressure of the FR increases the global
solids circulation rate which might be used to control the solids circulation rate
between the air reactor and the fuel reactor.
NOTATION
AR Air reactor CFB Circulating fluidized bed

CFM Cold flow model CLC Chemical looping
combustion
CLR Chemical looping reforming D Bed diameter, mm
DCFB Dual circulating fluidized bed DFB Dual fluidized bed
dp Particle mean Sauter FR Fuel reactor
diameter, µm
g Gravitation constant, m/s² htx Heat exchanger
ILS Internal loop seal LLS Lower loop seal
MeO Metal oxide OC Oxygen carrier
PCLR Pressurized chemical looping U0 Superficial gas velocity, m/s
reforming
ULS Upper loop seal ΔHR900°C Reaction enthalpy at 900°C,
kJ/mol
ηg Gas viscosity, Pa·s ρg Gas density, kg/m³
ρp Particle density, kg/m³ Ψ Sphericity, -
REFERENCES
1. Bellona Report 6:02. Bellona Foundation 2002.
2. Dybkjaer I.: Fuel Processing Technology 42 (April 1995) 85-107.
3. Lyngfelt A., Johansson M., Mattisson T., CFB Technology IX. Hamburg,
Germany: TuTech; 2008.
4. Hossain M.M., de Lasa HI., Chem. Eng. Sci. 63 (2008) 4433-4451.
5. Johansson M., Mattisson T., Rydén M., Lyngfelt A., International Seminar on
Carbon Sequestration and Climate Change, Rio de Janeiro, October 2006.
6. Linderholm C., Mattisson T., Lyngfelt A., Fuel 88 (2009) 2083-2096.
7. Kolbitsch P., Pröll T., Bolhàr-Nordenkampf J., Hofbauer H., Proceedings of the
9th International Conference on Greenhouse Gas Control Technologies
(GHGT-9), Washington DC., November 2008.
8. Lynfelt A., Leckner B., Mattisson T., Chem. Eng. Sci. 56 (2001) 3101-3113.
9. Kolbitsch P., Bolhàr-Nordenkampf J., Pröll T., Hofbauer H., Chem. Eng. Sci 32
(3) (2009) 398-403.
10. Rydén M., Lyngfelt A., Mattisson T., Energy & Fuels 22 (2008) 2585-2597.
11. Pröll T., Bolhàr-Nordenkampf J., Kolbitsch P., Marx K., Hofbauer H.,
Proceedings of the 2009 AIChE Spring National Meeting and 5th Global
Congress on Process Safety, Tampa, FL, April 26-30, 2009.
12. de Diego LF., Gayán P., Adánez J., Abad A., Dueso C., Ind. Eng. Chem. Res.
48 (2009) 2499-508.
13. Pröll T., Rupanovits K., Kolbitsch P., Bolhàr-Nordenkampf J., Hofbauer H.,
Chem. Eng. Technol. 32 (2009) 418-424.
14. L. R. Glicksman, Chem. Eng. Sci. 39 (1984) 1373-1379.

FLUID DYNAMIC EFFECTS OF RING-TYPE INTERNALS IN A
DUAL CIRCULATING FLUIDIZED BED SYSTEM
D. C. Guío-Pérez, K. Marx, T. Pröll and H. Hofbauer
Vienna University of Technology, Institute of Chemical Engineering, Getreidemarkt 9 / 166,
A-1060 Vienna, Austria
ABSTRACT
Intensified gas-solids contact in the fuel reactor of chemical looping combustion systems can
be a key issue for achieving the necessary gas-phase conversion rates. Wedge-shaped rings
were designed and installed in the fuel reactor of a cold flow model for fluid dynamic testing.
These internals are meant to reduce the typical radial and axial solids concentration non-
uniformity. It is shown, that more solids are present in the upper regions of the riser when in-
ternals are used. Additionally, increase of the solids elutriation rate from the riser was found.
INTRODUCTION
Dual Circulating Fluidized Bed System
The general idea of dual fluidized bed (DFB) reactor

systems is to expose two different gas streams to a
circulating stream of solids transporting chemical
species and often also heat. The use of loop seals
avoids direct contact between the two main gas
streams. Chemical looping processes in particular
require high gas–solid interaction and sufficient con-
tact time in both reactors.
The unit (Figure 1) has been designed as dual circu-

lating fluidized bed system with the solids elutriated
from a primary circulating fluidized bed reactor (air
reactor, AR) separated in a cyclone and fed to a
secondary CFB reactor (fuel reactor, FR) passing
first through a loop seal (upper loop seal, ULS). The
particles from the fuel reactor are fed back into the Figure 1: Sketch of the 120kW DCFB pilot unit.
fuel reactor itself after separation in a second
cyclone provided with a loop seal too (internal loop seal, ILS). The global solids circuit is closed
via a loop seal in the lower part of the reactors (lower loop seal, LLS) that constitutes a hydrau-
lic communication of the reactor inventories.
In this design, only the air reactor entrainment is responsible for the global solids circulation
between the two reactors, while the fuel reactor can be optimized in order to reach maximum
fuel conversion. An excellent gas-solids contact is especially required in the fuel reactor to
prevent undesirable presence of unconverted fuel in flue gas (1) (2).
Application of Internals
Introduction of internals has been studied for decades in slow velocity fluidized beds, several
types of internals are reported in literature already; rings, perforated plates, tubes, etcetera, an
initial classification of internals and their effects was done by Harrison and Grace (3). Whereas,
for circulating fluidized beds (CFB) some pioneering efforts have been completed (summaries
can be found in Lim et al. 1995 (4) and Zhu et al. 1997 (5)).
The principal objective of internals installation is the improvement of gas-solids contact; it has
been indicated that walls with baffles reduce the typical radial solids concentration non-
uniformities by removing the particles flowing down near the wall (annulus region) and bringing
them to the core, where reaction by contact with the gas is possible. They can likely also mi-
nimize solids back-mixing along the riser while preserving overall solids inventory. Even a se-
ries of baffles might divide a fluidized column in a multilayer fast fluidized bed that alternates
dense and dilute zones.
Above all, wall baffles in the form of flat rings have been of special interest when it comes to
internals in CFB and their effects on the gas-solids flow characteristics were well described by
Bu and Zhu in (6). They also concluded that elimination of sharp edges in the baffles would be
practical to reduce erosion. Likewise, the observed accumulation of particles in the corner
formed between flat rings and the wall, particularly important at low velocities and small open-
ing percentage of the ring, can be avoided by using wedged profile rings.
Optimal sizing of the baffles has been found to be decisive since they can affect the pressure
drop, on one hand, by scraping the down-flowing solids at the wall and deflecting them into the
core region where they can be quickly entrained upwards, and on the other hand, by creating
extra resistance to the gas-solids up-flowing stream. “When the rings are only in the annulus
region, the first mechanism would dominate, but when the rings extend into the core region,
the second mechanism would become more and more significant” (6).
For this particular dual circulating fluidized bed system, given that, the global circulation rate is
governed by the primary reactor fluidization and that the secondary reactor (where the inter-
nals need to be installed) is a counter-current reactor, effect of the rings introduction must be
seen from an additional point of view. It is, the internals not only intensify the contact between
the phases and promote a denser core, but also prolong the time needed for the particles to
reach the bottom of the reactor and hence increase their availability for reaction in this section
of the system. Additionally, it is important to notice that the investigated unit represents a sys-
tem of freely circulating CFBs where the total inventory is con-
stant and the solids fluxes in the risers result as a consequence
of inner fluid dynamics.
Rings Design
The rings were designed with a wedge shape section and an

aperture ratio of 60% (Figure 2). The wedge form of the rings
can likely be applied in refractory-lined hot systems and have
the advantages of reducing the impact of erosion and of elimi-
nating any dead area above the internal. This shape is ex-
pected to influence the flow structure of particles and gas by
both, promoting the change of direction in particles flow and by
creating a narrowed length for the flow of gas.
Figure 2: Rings (measures in mm).
EXPERIMENTAL The present study was carried out in a cold flow model pre-
viously designed and built for the fluid dynamic analysis of a
Cold Model 120 kW chemical looping pilot rig for gaseous fuels. The
model is a 3:1 scale of the hot unit and was dimensioned
P13 based on data of the hot facility and according to Glicksman
criteria (7); these principles allow the transformation of the
P14 results from the model to the pilot plant conditions. A basic
fluid dynamic description of the system was previously car-
ried out, in which influence of main parameters, namely
fluidization velocities and inventory, were characterized (8).
Figure 3 presents the configuration of the experimental rig.

P2
The most important parameters are listed for both, hot and
cold units in Table 1. Compressed air was used as the flui-
P3
dization agent for all fluidization points. The air flows were
P12 regulated by means of several rotameters and fed to the
different fluidization points, namely, primary and secondary
P4
air injection of both, air and fuel reactors, as well as upper,
P5 lower and internal loop seals. Bronze powder, with a mean
diameter of 64 μm was selected as the bed material. Elu-
triated particles from each reactor are separated by inde-
P19 P6 pendent cyclones and each stream passes through a filter
P1
/18 before leaving the unit.
P15 P7
Parameter Dimension ARH FRH ARC FRC
P8 ηG Pa s
. .
4.7 10
-5 .
4.1 10
-5 .
1.79 10
-5 .
1.79 10
-5
P9 ρG .
kg m
-3
0.316 0.288 1.22 1.22
. -1
U ms 7.32 2.08 4.25 1.21
P10
ρP .
kg m
-3
3200 3200 8730 8730
P16 dP µm 161 161 64 64
Φ - 0.99 0.99 1.00 1.00
P23/24
P17 P11 D mm 150 159 50 54
Table 1: Main fluid dynamic parameters in hot (H) and cold (C) units.
P22 P21
Three identical rings (Figure 2) were inserted in the second-
ary reactor of the cold flow model at the positions indicated in
Figure 3: Sketch of the cold flow model Figure 3. Different operating conditions were tested in order
including rings. to determine the effect of the internals on pressure profiles of
the system as well as on global and internal solids circulation rates.
Pressure was recorded at 9 positions along the height of the secondary reactor. Circulation
rates were calculated based on the accumulation velocities of particles measured in each of
the downcomers after interruption of fluidization gas flow in the corresponding loop seal; ULS
for global circulation rate and ILS for internal circulation rate.
Inherent Pressure Drop of the Unit with Rings
Pressure along the empty unit was measured under several aeration velocities. Pressure pro
files are presented in Figure 4. The pressure 1.2
drop expected to appear in the places were Fuel Reactor
rings were installed, was very slight or even 1
nonexistent. This supports the statement that

0.8
for the type of rings and the aeration velocities
Internals
Height [m]
used here, the influence of the rings on the location
0.6
pressure profiles due to extra resistance to the
up-flowing gas stream might be low.
0.4
5
Effect of Internals on Pressure Profiles 10
0.2 15
Figure 5 presents a comparison of pressure 20
25
profiles for the unit with and without internals at 0
standard operating conditions, 30Nm³/h in AR 0 10 20 30
Pressure [mbar]
and 10Nm³/h in FR. This profile is especially
interesting since it exhibits a comparable total Figure 4: Pressure profile of FR with no bed material
pressure drop in FR with and without rings. 3
for variation of fluidization between 5 and 25Nm /h.
Here it can be seen that pressure profiles of
AR are hardly altered after installation of rings. In the FR, a notable increment in pressure is
seen for the profiles with rings, particularly in the lower part of the column; while in the top,
pressures appear to be very similar for both profiles. It can be said then, that for a similar total
pressure drop along the FR (which would also mean, similar total particles hold up), pressure
drop, and hence particles, are redistributed upwards in the column.
A relatively larger pressure drop is observed across ring positions than along the length be-
tween them, the effect is more important as lower is the ring located, it is, as more concen-
trated is the bed. Since, no important pressure drop was found to be caused by the presence
of the rings themselves (Figure 4), this pressure drop would be then due to accumulation of
particles visually observed in the regions right above the rings. This tendency has been also
found by Jiang et al. 1991 (9) and Zhu et al. 1997 (5). The observation that the pressure drop
occurs across the ring while solids density is high above it, could be explained by the obvious
1.6 1.6
1.4 1.4
1.2 1.2
Air Reactor Fuel Reactor
1 1 Internals
location
Height [m]
Height [m]
0.8 0.8
0.6 0.6
0.4 0.4
0.2 0.2
0 0
-10 0 10 20 30 40 -10 0 10 20 30 40
Pressure relative to pressure at AR top [mbar] Pressure relative to pressure at FR top [mbar]
3 3
Figure 5: Pressure profiles for operation at 10Nm /h in FR and 30Nm /h in AR; with (solid line) and without (dotted
3 3 3
line) rings. 4kg inventory, 1.0 Nm /h fluidization in LLS, 1.0Nm /h fluidization ULS and 0.6Nm /h fluidization in ILS.
acceleration of the solids in the area of the ring. The acceleration phenomena cause a deviation
of the pressure profile and solids concentration in the vicinity of the internals. Zhu et al 1997 (5)
described a detailed flow structure around the internals as follows: “particles have the tendency
to form a relatively dense region above the rings under high solids circulation rates, the hold-up of
this relatively dense region increases with the solid circulation rate and decreases with the dis-
tance from the ring, this hold-up region is besides, denser at lower gas velocities. The tendency
to form a dense region depends also on the open area, a wider ring with relative smaller open
area provides, more “protected” space for the solids to form a dense region”.
Experiments in the modified model were performed varying systematically AR and FR fluidiza-
tion gas flow rates. Figure 6 shows pressure profiles of the unit with and without rings for a
fluidization gas rate of 30Nm³/h in AR and variation of fluidization rate in FR. In general, some
effects of variation of FR fluidization gas flow rate on the pressure of the unit are preserved
whether the rings are installed or not; namely:
− Pressure profile of FR is erected as the fluidization gas flow is increased, since higher flui-
dization velocities carry higher amounts of particles to upper sections of the reactor.
− Neither the pressure in AR nor in LLS undergo important modifications due changes in FR
fluidization gas flow as long as the latter is kept in lower values. Strong fluidization in FR
(see profile for 15Nm³/h) leads to accumulation of particles in ILS-downcomer and conse-
quent decrease of pressure in LLS as well as in both reactors. The effect is intensified if
the AR fluidization velocity in reduced (Figure 7).
1.6 1.6
1.4 1.4
1.2 1.2
Air Reactor Fuel Reactor
1 1 Internals
Height [m]
Height [m]
location
0.8 0.8
7 7
0.6 0.6
10 10
15 15
0.4 7 0.4 7
10 10
0.2 15 0.2 15
0 0
-10 0 10 20 30 40 -10 0 10 20 30 40
80 40 80
Internal Loop Seal
Pressure [mbar]
Pressure [mbar]
Pressure [mbar]
60 30 60
40 20 40
20 10 20
Lower Loop Seal Upper Loop Seal
0 0 0
P11 P21 P22 P17 P12 P19 P18 P6 P10 P24 P23 P1
3 3
Figure 6: Pressure profiles for operation at 30Nm /h constant in AR and variation between 7 and 15Nm /h in FR. 4kg
3 3 3
inventory, 1.0Nm /h in LLS,1.0Nm /h in ULS and 0.6Nm /h in ILS. With rings: solid lines, without rings: dotted lines.
− Pressures of ULS and ILS are increased with the increment of FR fluidization gas flow, in
the first case, as a consequence of the increased pressure in the discharge branch, and in
the second due to increment of elutriation from FR.
However, the increase of pressure in FR due to the presence of rings has an interesting influ-
ence on the ILS, since a higher pressure difference needs to be overcome. Especially at low
FR fluidization gas low rates (with very low circulation rates), ILS does not reach a desirable
operation state, and for high FR fluidization gas flow rates, where enough circulation occurs,
pressures in ILS are higher for the unit with rings. Pressure profiles prove as well, the incre-
ment of total pressure difference in the FR for every set of conditions, caused by the installa-
tion of rings; which indicates a general increment of hold up in this reactor.
Figure 7 presents a comparison of pressure profiles for the unit with and without rings at
20Nm³/h in AR and variation of FR fluidization velocity. Comparing with Figure 6, where the
AR fluidization gas flow and thus the solids circulation between AR and FR was higher; it can
be seen that even preserving the tendencies valid for the unit without rings with changes in AR
fluidization velocity (it is, redistribution of pressure drop in the AR riser and increment of pres-
sure in ULS), the presence of the rings makes the FR more sensitive to changes in the AR
fluidization gas rate. In Figure 8, pressure profiles for different inventories are shown for the unit
with internals, the expected increments in pressure drop due to increased inventory are ob-
served in both reactors.
1.6 1.6
1.4 1.4
1.2 1.2
Fuel Reactor
Air Reactor
1 1 Internals
Height [m]
Height [m]
location
0.8 0.8
0.6 7 0.6 7
10 10
0.4 15 15
0.4
7 7
10 10
0.2 15 0.2 15
0 0
-10 0 10 20 30 40 -10 0 10 20 30 40
80 40 60
Upper Loop Seal Internal Loop Seal
50
Pressure [mbar]
Pressure [mbar]
Pressure [mbar]
60 30
40
40 20 30
20
20 10
10
Lower Loop Seal
0 0 0
P11 P21 P22 P17 P12 P19 P18 P6 P10 P24 P23 P1
3 3
Figure 7: Pressure profiles for operation at 20Nm /h constant in AR and variation between 7 and 15Nm /h in FR. 4kg
3 3 3
inventory, 1.0 Nm /h in LLS, 1.0Nm /h in ULS and 0.6Nm /h in ILS. With rings: solid lines, without rings: dotted lines.
1.6 1.6
1.4 1.4
1.2 1.2
Fuel Reactor
Air Reactor
1 1 Internals
Height [m]
Height [m]
location
0.8 0.8
0.6 0.6
0.4 0.4
0.2 0.2
0 0
-10 0 10 20 30 40 -10 0 10 20 30 40
Pressure relative to pressure at FR top [mbar] Pressure relative to pressure at FR top [mbar]
80 40 60
Upper Loop Seal 50 Internal Loop Seal
Pressure [mbar]
Pressure [mbar]
Pressure [mbar]
60 30
40
40 20 30
20
20 10
10
Lower Loop Seal
0 0 0
P11 P21 P22 P17 P12 P19 P18 P6 P10 P24 P23 P1
3 3
Figure 8: Pressure profiles operation (with rings) at 10Nm /h in FR and 30Nm /h in AR for variation of inventory
3 3 3
between 3kg (dotted line) and 4kg (solid line). 1.0 Nm /h in LLS, 1.0Nm /h in ULS and 0.6Nm /h in ILS.
Effect of Internals on Circulation Rates
Given the increased pressures in both ULS and ILS after installation of rings, global and inter-
nal circulation rates are expected to be raised. This can be confirmed in Figure 9, the incre-
ments are proportional to the fluidization rates, it is, larger differences appear for higher fluidiza-
tion gas flow rates. However, at 15Nm3/h of fluidization gas flow in FR, the increase of the in-
ternal circulation rate and the accumulation of material in FR-downcomer reduce dramatically
the concentration of particles in the rest of the system (as already seen in the profiles) and
120 120 120
100 100 100

Circulation rate [kg/m²s]
80 80 80
60 60 60
AR 10Nm³/h AR 20Nm³/h AR 30Nm³/h
40 40 40
20 20 20
0 0 0
0 5 10 15 20 0 5 10 15 20 0 5 10 15 20
FR Nm3/h FR Nm3/h FR Nm3/h
Figure 9: Global circ. rate (triangles ∆) and internal circ. rate (circles Ο) with variation of FR fluidization for different values of AR
fluidization. Comparison between operation with (solid markers) and without (empty markers) rings in FR. 4kg total inventory.
hence the global circulation rate. The balance between global and internal circulation rates
should be thus better considered in the unit with internals. It must be additionally indicated that
at stronger fluidization rate in FR, high elutriation was observed.
CONCLUSION
The designed rings with wedge-shaped section installed in the secondary reactor of a DCFB
cold flow model were found to be effective on increasing the inventory in this section and im-
proving the contact between solid and gas phases by reducing the typical radial solids concen-
tration non-uniformities. After comparison of pressure profiles and circulation rates between the
unit with and without rings it can be affirmed that the pressure in the FR has been increased
and redistributed after installation of rings; total pressure drop is also increased, meaning an
increment in total hold up in this reactor. Particularly high pressure drops are observed across
the sections were rings were installed, which can be attributed to the reacceleration of particles
in these segments after the bed material is scrapped from the wall and directed to the core
zone by effect of the rings. Slightly higher internal circulation rate as well as the corresponding
pressure increase in ILS was observed in the unit with rings. Additionally, the influence of the
aperture ratio of rings will be studied in further work.
ACKNOWLEDGEMENT
Financial support from the Austrian Government’s climate and energy research program, or-
ganized by the Austrian Research Promotion Agency (FFG), contract No.8219511 Gvolution,
is gratefully acknowledged.
NOTATION
AR Air Reactor Fr Froude Number, [-] ULS Upper Loop Seal
. -2
Ar Archimedes Number, [-] g grav. acceleration, [m s ] V 3. -1
normal vol. flow, [Nm s ]
D inner riser diameter, [m] ILS Internal Loop Seal
Φ mean sphericity of part., [-]
dP mean particle diameter, [m] LLS Lower Loop Seal .
DCFB dual circulating fluidized bed ReP particle Reynolds N., [-] η dynamic viscosity, [Pa s]
. -3
FR Fuel Reactor U
. -1
superficial gas velocity,[m s ] ρ density, [kg m ]
REFERENCES
1. Pröll T., Kolbitsch, P., Bolhàr-Nordenkampf, J., Hofbauer, H. A novel DCFB system for chemical
looping processes. AIChE J. Vol.55, N.12, 3255-3266. 2009.
2. Kolbitsch, P., Pröll T., Bolhàr-Nordenkampf, J., Hofbauer, H. Design of a Chemical Looping Com-
bustor using a DCFB Reactor System. Chem. Eng. Technol. 32, No.3, 398–403. 2009.
3. Harrison, D. and Grace, J.R. Fluidized bed with internal baffles. In: J.F. Davidson and D. Harrison,
Editors, Fluidization, Academic Press, London. pp. 599–626. 1971.
4. Lim, K.S. Zhu, J.X., Grace, J.R. Hidrodynamics of gas-solid fluidization. Int.J. Multiphase Flow.
Vol.21, Suppl., 141-193. 1995.
5. Zhu, J-X. Salah, M. Zhou, Y. Radial and axial voidage distributions in CFB with ring-type internals.
J. Chem. Eng. Jpn. Vol.30, N.5, 928-937. 1997.
6. Bu J., Zhu J-X. Influence of ring type internals on axial pressure distribution in CFB. Can. J. Chem.
Eng., Vol. 77, 26-34. 1999.
7. Glicksman, L. Scaling relationships for fluidized beds. Chem. Eng. Sci. 39, 1373-79. 1984.
8. Pröll T., Rupanovits K., Kolbitsch P., Bolhàr-Nordenkamf J., Hofbauer H. Cold flow model study on
a DCFB system for chemical looping processes. Chem. Eng. Technol., 32, No.3, 418-424. 2009.
9. Jiang, PJ., Bi, H.T., Jean, R.H. and Fan, L.S. Baffle effects on performance of catalytic CFB reac-
tor. AIChE J. 37, 1392-1400. 1991.
OPERATING EXPERIENCE AND LATEST DEVELOPMENTS
OF
ALSTOM POWER‘S 300 MWe CLASS CFB BOILERS.
Bruce Wilhelm1, Pierre Gauvillé2, Iqbal Abdulally1, Christian Enault2

1
Alstom Power R&D Execution, 175 Addison Road, P.O. Box 500, Windsor, CT 06095, USA
2
Alstom Power CFB Product Line, 12 Rue Jean Bart, 91300 Massy, FRANCE
ABSTRACT
Fuel flexibility combined with low emissions, particularly with high sulphur fuels, are
the key drivers for installing a Circulating Fluidised Bed (CFB) Boiler. Taking into
account the global drive for more efficient and clean combustion, and the
development of CFB combustion and emission reduction technologies accordingly,
worldwide applications for CFB Boilers are increasing.
Accordingly, Alstom Power continues the evolutionary development of its CFB Boiler
portfolio, based on the experience gained with operating units. This paper focuses
on Alstom Power’s 300 MWe Class CFB Boiler products.
East Kentucky Power Cooperative's (EKPC) Spurlock unit 4 is one of the large
Alstom’s 300 MWe CFB boilers in operation since 2009. This unit is a duplicate of
EKPC’s Gilbert #3 CFB boiler unit, which was also supplied by Alstom. The lessons
learned from the Gilbert #3 unit were applied to the Spurlock #4 unit, which has
resulted in high availability and smooth operation to date. The performance and
operation of the Flash Dryer Absorber system and SNCR for NOx removal, which
are an integral part of the CFB unit where stringent emission control is a
requirement, are also discussed.
Low NOx emissions were achieved by the low temperature combustion and by the
use of the selective non-catalytic reduction (SNCR) system developed and tested by
Alstom at the EKPC Spurlock station, leading to 20% reduction of the ammonia
consumption. A 98% SO2 removal rate was achieved with limestone injection into
the furnace. The proprietary Flash Dryer Absorber (NID™) system developed and
tested by Alstom has helped to improve overall O&M by reducing the limestone
consumption by around 25%.
Finally, the paper introduces the latest 300 MWe Class CFB Boiler product, built on
the well proven features of the operating units, which has been developed to further
enhance fuel flexibility and clean combustion on a cost-effective basis.
INTRODUCTION
The latest 268 MWe (net) boiler, named Spurlock #4, is the fourth generating unit at
East Kentucky Power Cooperative’s (EKPC) Spurlock Station near Maysville,
Kentucky (KY), USA. It is located alongside Gilbert #3, as well as two pulverized
coal units, 300 MWe and 500 MWe, that were built over 25 years ago. It burns a
variety of coals primarily supplied by Kentucky mines and reached commercial
operation in 2009.
Low SO2 emissions is achieved by sulfation of limestone sorbent in the CFB and by
additional sulfation of unreacted sorbent in the NID™, a proprietary flash dryer
absorber (FDA) system located downstream of the CFB. This permits low SO2
emissions (245 mg/Nm3, 98% removal). Very low NOx emissions ( 85 mg/Nm3) are
enabled by the low combustion temperatures of the CFB and by the use of
proprietary selective non-catalytic reduction (SNCR). The latter employs the
addition of anhydrous ammonia and extended residence times at low temperature to
further reduce NOx within the boiler.
CFB BOILER DESCRIPTION
The CFB is a natural circulation boiler consisting of a single grate furnace; three
recycle cyclones and two Fluidized Bed Heat Exchanges (FBHEs) in the hot loop.
Some superheater and evaporator panels are provided in the furnace to attain the
total duty required in the hot loop. The finishing superheater and reheater are
located in the FBHEs. A portion of the solids from the recycle loop are passed
through the FBHEs in a controlled manner in order to maintain the duty and,
therefore, the final reheat and superheat steam temperatures. With this approach,
the plant heat rate is minimized by not using spray water to control the final reheat
temperature and only a minimum amount of spray to control the final steam
temperature.
A Just-In-Time (JIT™) limestone system

is provided for sorbent injection into the Coal Silos
CFB for 90+% reduction of SO2 within the Cyclones Furnace
furnace. The JIT™ system utilizes two Backpass

Limestone
Silo
100% capacity Raymond™ Roller Mills

operating with a pressurized Primary Air
system to directly transport the limestone NIDTM/Fabric Filter
to the furnace. Airheater
FBHE
A Selective Non Catalytic Reduction FBAC

JIT
(SNCR) system is provided that optimally System
discharges ammonia reagent into the Figure 1: Model of the Gilbert 3 and
inlet and outlet of the cyclone in order to Spurlock #4 Boiler Island
control the NOx emission to the permitted
levels.
The flue gas leaving the cyclones is passed through a convection backpass
consisting of the primary reheater and superheater and economizer surface. Final
heat recovery is done by Alstom’s tri-sector Air Preheater. The flue gas leaving the
Air Preheater is directed to a NIDTM and baghouse for final SO2 and particulate
control.
The solids inventory is controlled by removing bottom ash via two Fluidized Bed Ash
Coolers (FBACs) consisting of water cooled surface.
FUEL FLEXIBILITY
Coal Firing: Being situated on the Ohio River and adjacent to CSX rail lines, EKPC
is able to choose fuels from a number of sources. The use of a CFB boiler
enhances fuel flexibility by being able to fire a wide range of fuels. Table 1 shows
the range of fuels used in the design of the Gilbert #3 and Spurlock #4 units.
The use of a CFB boiler also allows EKPC to burn this wide fuel range while
maintaining low emissions rates as called for in the permits. The coals are High
Volatile Bituminous coals as per ASTM classification which can produce up to 12000
mg/Nm3 uncontrolled SO2. The permitted emissions for the Spurlock #4 Unit are
well below the New Source Performance Standards (Table 2)
Table 1: Coal Fuels Ultimate Analysis
Fuel analysis (%) on weight Design fuel Pine Branch Pittsburgh 8 Range for all
basis Fuel Fired
Carbon 53.48 61.67 70.84 47.79 – 71.48
Hydrogen 4.40 2.40 3.87 2.40 – 4.56
Oxygen 7.21 5.03 3.95 3.79 – 10.11
Nitrogen 0.90 1.33 1.41 0.72 – 1.41
Sulfur 4.50 1.50 4.00 1.21 – 5.56
Ash 20.00 20.00 8.00 6.30 – 30.00
Moisture 9.51 8.07 7.85 7.24 – 17.46
Higher Heating Value Btu/lb 10,400 10,215 12,502 9,154 – 12,710
(Kcal/kg) (5800) (5600) (7000) (5100 – 7000)
Table 2: Comparative Emissions Levels
Spurlock #4 Emissions Spurlock #4 New Source

Lb/mmBtu Permitted Performance
( mg/Nm3, 6% o2 dry gas) Emissions Standards
NOx 0.07 (85) 0.60 (740)
SO2 0.2 (245)or 98+% 1.2 (1500)
reduction
Particulate PM10 0.015 (20) 0.03 (35)
Biomass and Opportunity Fuel firing: In addition to the coals specified, the unit is
also designed to burn biomass and approximately five million tires per year. Having
the widest possible fuel choices allows EKPC to continuously supply power to their
customers at the lowest possible rates. EKPC CFB units to date have co-fired
biomass up to 45 MWth and Tire Derived Fuel (TDF) up to 135 MWth (20% of firing
capacity). Table 3 shows the analysis of these alternative fuels.
Table 3: Alternative Fuels Ultimate Analysis
Fuel analysis (%) on weight Switchgrass TDF Wood chips

basis
Carbon 46.38 78.35 24.5
Hydrogen 5.56 6.62 3.00
Oxygen 40.20 1.22 22.00
Nitrogen 0.24 0.22 -
Sulfur 0.05 1.15 -
Ash 2.53 11.74 0.5
Moisture 5.04 0.7 50.0
Chlorine 0.049 - -
Higher Heating Value Btu/lb 7,764 14,950 4,730

(Kcal/kg) (2300) (4350) (2600)
Biomass and opportunity fuels are fired into the unit as and when they are available.
No impact on operation, performance and emissions were observed at these rates
of firing.
These fuels were fired without additional equipment. The raw limestone storage and
conveying system to the JITTM system was used to add the biomass. When feeding
the biomass, the conveyor system leaving the limestone storage discharges the
biomass onto the conveyor belt carrying prepared coal to the common tripper. The
biomass is introduced at a predetermined ratio via the limestone system while the
prepared coal is loaded onto the coal bunkers. So, the biomass is blended with the
coal and introduced to the CFB furnace via the normal feed system. If the raw
limestone make-up is required the control system switch to the usual mode so as to
feed separately the raw limestone bins.
EMISSIONS CONTROL
With a CFB boiler, combustion takes usually place in the range 850 – 900°C, which
results in a lower NOx emission compared to the higher combustion temperature
associated with PC boilers. SO2 emission can also be reduced by injecting
limestone into the furnace. The limestone is calcined in the boiler to become lime
that subsequently reacts with SO2 released in the combustion process to form
gypsum, a very stable inert compound. This is then removed from the CFB unit
either with the bottom or the fly ash.
To control emissions further, the Gilbert #3 and Spurlock #4 boilers include
additional methods of SNCR technology for NOx control and the recently developed
Alstom NID™ system for advanced SO2 emissions control.
In the SNCR process ammonia gas is injected into the flue gas stream where it
thermally reduces the NOx in the flue gas to form nitrogen (N2) and water vapor.
The anhydrous ammonia is injected in the CFB’s gas ducting via a novel proprietary
grid, providing excellent mixing and dispersion of the reagent.
The NID™ system uses the fly ash produced in the boiler that contains unused lime
as the reagent. The fly ash collected in the baghouse is hydrated slightly and then
re-entrained in the flue gas stream. The hydrated lime then reacts with any SO2
present in the flue gas. In order to maintain the permitted SO2 emission, the overall
removal rate for the Spurlock #4 CFB with the NID™ system is greater in operation
than 95% over the complete range of fuels.
NOx REDUCTION FROM GILBERT #3 TO SPURLOCK #4
The operation of Gilbert #3 unit has highlighted a difference of bed temperature

between the right side and the left side of the furnace. The deviation in the bed
temperature led to a hotter area resulting in higher NOx formation in comparison with
the opposite side. On Spurlock #4 unit additional evaporative panel was added to
the left side for keeping a bed temperature uniformly low.
After over a year in commercial operation, EKPC has reported that the addition of
the evaporative panel has in effect lowered the bed temperatures on the left side of
the unit by an average of 10°C and has met its intended performance of reducing
the formation of NOx.
The second effort was focused on the SNCR’s efficiency by improving the quality of
ammonia injection into the flue gas.
Alstom’s original SNCR

employed three to four wall
lances in the cyclone outlet and
inlet duct (Figure 2). Through
testing it was determined that
the standard CFB industry
approach of injecting ammonia
reagent to the gas stream was SNCR Lances
ineffective because of the
following reasons:
Cyclone Outlet Hood Side and Plan View
Figure 2: Original SNCR Lance Configuration

1-The gas distribution was uneven over the duct section
2-The NOx concentration was uneven over the duct section
3-The lances were not as effective in distributing the ammonia as required to
address the non-uniformity as indicated in 1 and 2 above.
This leads to the innovation of the
new SNCR grid system.
The new grid system has multiple

lances that spans across the duct
from side-to-side (Figure 3). Each
half of these lances receive
Location of Improved SNCR System
reagent with a supply line that
can be controlled independently.
Each lance has evenly distributed
nozzles to ensure even Cyclone Outlet Hood Side and Plan View
distribution of reagent from each
section of the lance. Figure 3: New Alstom SNCR Grid System
This arrangement gives the ability to distribute the reagent between cyclone and
with each cyclone duct to match the NOx concentration in the flue gas streams
entering and leaving each of the cyclones thereby optimizing the SNCR system
resulting in lower NOx emission, ammonia consumption and slip.
Both EKPC and Alstom have been actively improving NOx control with the objective
of reducing both ammonia consumptions and NOx emission. To this end, several
optimization tests and modification of the SNCR were done on both Gilbert #3 and
Spurlock #4 as follows:
1) 2005 – SNCR optimization with original system on Gilbert #3 unit

2) 2006 – Modification of SNCR system to change original lance system to a
ammonia grid distributions system
3) 2007 – Optimization testing on Gilbert # 3 unit
4) 2008 – Addition of evaporative panel on Spurlock unit #4
5) 2009 – SNCR optimization test on Spurlock #4
6) 2009 – Emissions optimization test on Spurlock #4 unit
7) 2010 – Emissions optimization test on Spurlock #4 unit
During the optimization test all emission gas constituents (SO2, NOx, CO and O2)
were measured. The measurements were completed either at the outlet duct of the
economizer or the outlet duct of the each of the three cyclones. On the cyclone
outlet duct the gas was sampled at three points before and after the new SNCR grid
system .
The cyclone outlet measurements gave a better indication of the gas composition
leaving each of the three furnace sections associated with a given cyclone.
The tests showed that there was an uneven distribution of emission during the
various test campaigns. The main changes were as follows:
1) Side-to-side biasing of fuel
2) Side-to-side biasing of Secondary air
3) Deeper staging of combustion air. That is, decrease in primary/secondary air
ratio.
These changes, together with the use of the new SNCR distribution grid resulted in
the lowering in-furnace and final NOx, ammonia consumption by greater than 20%
while maintaining ammonia slip to less than 2 ppm.
SO2 REMOVAL RATE
The NIDTM system provided on this unit was of the first generation for a large-scale
unit. There were several upgrades made to eliminate problems encountered during
initial operation.
However, the NIDTM system has helped to improve overall O&M cost by reducing
the overall limestone consumption by as much as 27%. This reduction in limestone
rate has secondary benefits as follows:
o 0.8% increase in boiler efficiency

o 2.6% decrease in CO2 emission
o 16% decrease in ash flow
o A few percent decrease in ammonia consumption.
PATH FORWARD
Based on overall experience on large scale CFBs, Alstom is developing a common

product platform of standardized equipment based on various popular size units
such as 100, 150, 300 MWe. The 300 MW-class CFB product has been developed
and is currently offered by Alstom.
The 300 MW-class CFB is a natural Limestone bin

circulation boiler consisting of a
single grate furnace with
evaporative, final reheat and
superheat panels and three steam
cooled recycle cyclones to attain the
total duty required in the hot loop. By
locating the finishing superheater Coal silos
and reheater in the furnace, a proper
blend of radiant and convection heat
duty is maintained at all loads. This
ensures that a steady and high final JITTM
steam and reheat steam
temperature are maintained through
out the control load range.
Rotary ash
Figure 4: 300 MW-Class CFB Standard Boiler
Arrangement
A reheat steam bypass system is provided around the convection surface in the
backpass in order to control the final reheat temperature without the use of spray
water. With this approach, the plant heat rate is minimized by not using spray water
to control the final reheat temperature and only a minimum amount of spray to
control the final steam temperature.
Alstom’s Just-In-Time (JIT™) limestone system is provided for sorbent injection into
the CFB for 90+% reduction of SO2. The system provides sorbent to the front and
back of the furnace.
Alstom’s proprietary Selective Non Catalytic Reduction (SNCR) system consisting of

injection grids is provided that is capable of discharging aqueous or anhydrous
ammonia reagent evenly to the inlet and outlet of the cyclone in order to control the
NOx emission with high reduction levels to the permitted levels while maintaining
acceptably low ammonia slip.
The flue gas leaving the cyclones is passed through a conventional convection
backpass consisting of the primary reheater and superheater and economizer
surface. Final heat recovery is done by a tri-sector Air Preheater. The flue gas
leaving the Air Preheater is directed to a NIDTM and baghouse for final SO2 and
particulate control.
The solids inventory is controlled by removing bottom ash Rotary Ash Coolers
(RACs). This eliminates the issues encountered when firing fuels with large
quantities of ash as rocks or agglomerates that may form in the furnace.
CONCLUSION
EKPC Spurlock #4 300MWe Power Plant is one of the cleanest burning coal fired
power plants and demonstrated the flexibility of the CFB technology by burning
different kinds of biomass as well as tires. The development of the SNCR
distribution grid resulted in the reduction of ammonia consumption around 20%
while keeping the ammonia slip below 2 ppm. The reactivation of free lime included
in the fly ash by using the Flash Dryer Absorber ( NIDTM) enabled the EKPC power
plant to reduce the limestone consumption by around 25%.
The experience learned from the Gilbert #3 contract execution, commissioning and
operation was applied to the Spurlock #4 unit, which has resulted in 94% availability
after the first year of commercial operation.
Finally, an excellent relationship with EPKC enabled Alstom to develop and improve
the integrated CFB solution with FDA and SNCR as an available clean coal
technology to make coal generation a vital and environmentally responsible means
of power generation in the United States.
Going forward, all design enhancements derived from this cooperation have been
implemented into the current large-scale designs such as the 300 MW-class CFB
standard boiler offered by Alstom.
OBSERVATION OF FLOW REGIME TRANSITION IN A CFB
RISER USING AN LDV
Paul C. Yue, Joseph S. Mei, Lawrence J. Shadle
National Energy Technology Laboratory
U. S. Department of Energy
3610 Collins Ferry Road
Morgantown, West Virginia 26507-0880
Abstract
The solids flow in a circulating fluidized bed (CFB) riser is often described to have a
core-annular structure. For a given superficial gas velocity, at the initial introduction
of solids into a riser a flow structure of dilute upflow regime exists. Continuing to
increase the solids flow in the riser transitions the flow structure to the core-annular
flow regime. However, with further increase of solids flow a condition is reached,
depending on the superficial gas velocity, where all the solids across the riser cross
section flow upwards, even those at the wall. When the solids flux, solids fraction and
gas velocity are relatively high, such a condition is described as the dense phase
suspense upflow (DSU) regime.
In this paper we report our observations of these flow regime transitions by using a
laser Doppler velocimeter (LDV) to monitor the upward and downward particle flow
velocities at and near the riser wall of the National Energy Technology Laboratory’s
30.4 centimeters diameter CFB cold flow model. The particles were high density
polyethylene (PPE) spheres with a Sauter mean diameter of 861 micron and a
density of 800 kg/m3. Three superficial gas velocities of 6.55 m/s, 10.67 m/s and
13.72 m/s were used in this study. For the case of superficial gas velocity 6.55 m/s,
the experimental data show that the transition from dilute upflow to core-annular flow
occurred when the solids flux was about 7 kg/m2-s and the transition from core-
annular flow to dense suspension upflow was about 147 kg/m2-s. As the superficial
gas velocity was increased to 10.67 m/s the corresponding flow regime transitions
were at 34 kg/m2-s and 205 kg/m2-s, respectively. For the case of superficial gas
velocity of 13.72 m/s the data showed no distinct transition of flow regimes. The
particles were all upflow for the range of solids fluxes from 10 kg/m2-s to 286 kg/m2-
s.
INTRODUCTION
The fluidization condition in a circulating fluidized bed (CFB) is classified as lean-

phase fluidization. Within this lean-phase fluidization, two flow regimes exist, the
dilute phase upflow regime and the fast fluidization regime (1). The dilute phase
upflow regime is characterized by a homogeneous flow structure. The fast
fluidization regime is characterized by a heterogeneous flow structure and has higher
slip velocity between the gas and solids than that in the dilute phase transport
regime. In a typical fast fluidized bed, there often exists particle agglomerates or
clusters moving up and down especially along the riser wall. This leads to a core-
annulus flow structure. The formation of clusters is an important and necessary
feature, but by itself is not an adequate condition for a fast fluidized bed (2). In a
core-annulus flow structure, the center or core region consists of a mostly dilute
phase of upward-flowing gas and particles surrounded by an annular region of
descending particles (3). This flow structure is the basis of various CFB models [1].
However, there exists a third flow regime, the dense suspension upflow (DSU), first
pointed out by Grace (4). The solids hold-up in his flow regime is typically in the 10%
to 20% range and the superficial gas velocities on the order of 6-10 m/s with very
high solids net circulation rates, 300-1000 kg/m2-s. Another feature in DSU is the
relative lack of particle downflow. Hence, measuring particle velocities at the wall
over different solids fluxes should provide the necessary information to identify and
discriminate the transitions between these three flow regimes.
We have observed that during

the introduction of solids into
the riser at the initial stage of
operation of a CFB, the solids
flow at the upper section of the
riser is homogeneous, i.e. in the
dilute upflow regime. Upon
increasing the solids flux,
clusters begin to appear and the
flow structure eventually
transitions into the fast
fluidization regime. Monazam
and Shadle (5) have developed
a transient method to identify
the transition velocities to
identify when riser operations
are in slugging, fast fluidized or
core-annular regimes making
the case that many of the riser’s
dynamic responses are
dependent only upon the gas
velocities and solid properties,
but independent of the solids
flux. Note that this analysis
does not distinguish between
risers operating with different
solids holdups, such as being
above and below the saturated
carrying capacity (6). Thus, it is
of interest to explore the
Figure 1. Schematic of National Energy Technology behavior of particles near the
Laboratory’s cold flow circulating fluidized bed. wall at an axial location that is
normally in the fully developed
region of the riser. Basu (2) has stated that there is a lack of a clear picture of the
transition to and from fast fluidization. This is interpreted to include transitions due to
both the gas velocity and solids flux.
We conducted particle velocity measurements with a laser Doppler velocimeter
(LDV) system. By using the axial down-flow velocity component (one can also use
the upflow component), we were able to identify the flow regime transitions from the
velocity counts. The solids hold up in these flow transitions were compared with the
apparent solids fraction profiles based on the differential pressure measurements
along the vertical axis of the riser.
FLOW REGIME TRANSITION MEASUREMENTS
The measurements were conducted at the National Energy Technology Laboratory’s

cold flow CFB model illustrated in Figure 1. The riser has a height of 15 meters and
a diameter of 30.4 centimeters. It has been described in detail elsewhere (5-8). The
particles were high density polyethylene (PPE) spheres with a Sauter mean diameter
of 861 micron and a density of 800 kg/m3. Three superficial gas velocities of 6.55
m/s, 10.67 m/s and 13.72 m/s were used in this study. The classical or lower
transport velocity was 4.3 m/s for this material while the upper transport velocity was
found to be 6.3 m/s (5). Thus, all of these tests were conducted in dilute, core
annular, or dense suspension upflow conditions.
The LDV was used to monitor the particle flow in the axial direction. The probe
volume of the LDV was positioned at 9.3 meters above the centerline of the solids
entry port. This location is the upper part of the middle region of the riser (9). The
riser wall in this section is of optical quality acrylic material. The approach was to
obtain the upflow and downflow
velocity counts rather than
velocities in the space close to
the inside wall of the riser. We
set the transceiver of the LDV
on a manually operated
translation platform. A digital
meter with a resolution of 0.01
mm is attached to the driving
screw. In order to ensure the
LDV probe volume is at the riser
Figure 2. LDV in CFB riser wall velocity readings with wall, we initially positioned it
only air circulating taken at the wall, P0. inside the acrylic wall of the
riser. With the CFB running on
air only, the vibrations induced
on the structure by the air flow
was sufficient to generate
detectible velocity signals on the
LDV, shown in Figure 2.
Monitoring these signals while
advancing the probe volume of
the LDV through the wall, the "at
wall" position was determined
accurately when these noise
velocity signals disappeared.
Figure 3. LDV at CFB riser wall velocity readings Figure 3 is an example when
with only air circulating within the riser at P0 + 6.8 such a condition was reached.
The few particles detected over
the 30 second period were probably particles entrained from the CFB wall.
Since the condition of a flow regime is defined by the axial component of the particle
velocity we used the downflow velocity counts in our analysis. It would be equally
valid to use the upflow velocity counts.
y g
80
Flow Regimes Transition at
Superficial Gas Velocity Ug =
6.55 m/s
Velocity Count Ch. 1
60
This superficial gas velocity was
chosen to be consistent with
40 previous CFB operation conditions
to provide experimental data for
model validation study. Figure 4
shows that a typical velocity
20
distribution containing broadly
two to three velocity groups.
The flow direction convention
0 used by the instrument is such
-21 -14 -7 0 7 that positive velocities indicate
Velocity Ch. 1 (m/sec) downflow direction and negative
for upflow direction. Hence, in
Figure 4 the negative velocities
Figure 4. An example of LDV particle velocity are particle upflow velocities in
histogram taking measurement at CFB riser wall, the CFB riser and the positive
Ug=6.58 m/s. Ms=2,665 kg/hr. velocities are downflow particle
velocities.
With reference to the velocity

histogram, notice that the high
velocity group has velocities
more than twice the superficial
gas velocity used. It has been
reported that some particles in a
riser may have velocities much
higher than the gas velocity [10].
However, because of their
relatively low count, most of the
data sets showed that they
Figure 5. Percentage of downflow velocity counts comprised less than 10% of the
at height 9.36 m versus solids flux for Ug=6.55 m/s. total velocity counts; we have not
included them in our analyses.
We expressed the down flow
velocity counts, respectively, as a percentage of the total velocity count, excluding
the high velocity group. In Figure 5 we plotted the downflow velocity count in
percentage of the total velocity count (both upflow and downflow) against particle flux
derived from mass flow rate measured by a spiral device (6). However, for particle
flux greater than 100 kg/m2-s we observed that the downflow velocity count
percentage decreased as the particle mass flux increased. This indicates a shift in
the particle flow direction towards the dense suspension upflow condition.
We compared this observation

based on the velocity count
analyses with the solids fraction
profiles for two flow conditions,
one in the dilute upflow and one in
dense suspension upflow as
shown in Figure 6. For low solids
flux condition (the red curve) the
apparent solids fraction at the 9 to
10 meter level shows a value of
much less than 10% indicating the
bed is in the dilute transport
Figure 6. Solid fraction profiles along the axis of regime which is also indicated in
CFB riser at Ug=6.55 m/s for a low and a high solids Figure 5, showing low downflow
flux conditions corresponding to the dilute and the velocity count percentage. On the
dense suspensions upflow regime. other hand, for the high flux case
the solids fraction profile (the blue
curve in Figure 6) indicates a
solids fraction of higher than 10%
exists at the 9 to 10 meters level
agreeing with that indicated in
Figure 5.
Flow Regime Transition at

superficial velocities of 10.67
m/s and 13.72 m/s
Figure 7. Percentage of downflow velocity counts
at height 9.36 m versus solids flux for Ug=10.67 Similar measurements were made
m/s. at higher superficial gas velocities.
The purpose is to see how, if any,
the superficial gas velocities
would affect the flow regimes
transition. It is obvious that at
higher superficial gas velocity,
because of the dilution effect, one
would expect the transition would
require higher solids flux.
For the case of superficial gas

velocity of 10.67 m/s the downflow
velocity counts are plotted in
Figure 7 as in Figure 5. However,
Figure 8. Solids fraction profiles along the axis of it seems that the transition from
CFB riser at Ug=10.67 m/s and a low and a high dilute transport regime to core-
solids flux conditions. annular flow regime was not
clearly observed. The overall
downflow velocity count
percentage is low throughout this solids flux range indicating that high percentage of
the particles were being carried upwards by the higher carrier gas velocity. The
decrease in downflow as solids flux is increased suggests that the flow structure is
approaching the dense suspension upflow (DSU) regime. The data show that at
high gas velocities (for both low and high solids fluxes) there can be no net downflow
at the wall. These data also suggest that dilute phase flow may transition to DSU
regime without going through the core annular flow regime. However, more
experimental data will be needed to verify this trend. Figure 8 show the apparent
solids fraction profiles. As the data suggested, at riser gas velocity of 10.67 m/s and
at solids flux of 205 kg/m2-s, the average solids fraction was still less than 10%.
The corresponding downflow

velocity count percentage plot
and the apparent solids fraction
profile plot for the superficial gas
velocity of 13.72 m/s are shown
in Figures 9 and 10, respectively.
Figure 9 shows that there is no
apparent flow regime transition
detected. The apparent solids
fraction profile, Figure 10, also
indicates low solids hold-up in the
riser at the sample location
Figure 9. Peercentage of downflow velocity counts showing the diluting effect.
at height 9.36 m versus solids flux for Ug=13.72 Indeed, at these high gas
m/s. velocities it may require much
higher solids flux to the riser to
achieve dense suspension
upflow.
CONCLUSIONS
We have shown that it Herman

Yue
<hermanyue76@gmail.com> is
possible by monitoring either the
downflow or upflow velocity
counts measured by an LDV
system at the riser wall to
demarcate the transitions of flow
regimes. These transition
Figure 10. Solids fraction profiles along the axis of
CFB riser at Ug=13.72 m/s and a low and a high measurements were supported
solids flux conditions. by apparent solids fractions
obtained from differential
pressure measurements at the corresponding sampling region of the riser. At higher
riser gas velocity, the flow regime transition from dilute phase flow may directly
transit to DSU flow regime without going through the core annular flow regime. This
solids flow behavior may be attributed to the higher percentage of particles are being
transported out of the riser through the high gas velocity. However, more
experimental data will be needed to verify this trend.
NOTATION
Ms Mass circulation rate, kg/hr

Ug superficial gas velocity, m/s
REFERENCES
1. Fan, L-S and Zhu, C., Principles of Gas-Solid flows, Cambridge University Press,
1998, p.448.
2. Basu, P., Combustion and Gasification in Fluidized Beds, Taylor & Francis
Group, 2006, p. 36.
3. Lints, M. C., and Glicksman, I. R., The Structure of Particle Clusters Near the
Wall of a Circulating Fluidized Bed, in Fluid-Particle Processes. Fundamentals
and Applications, Weimer, A. W., Chen, J. C., Fan, Liang-Shih, and Yang, W-C
(Eds), AIChE Symposium Series No 296, Vol. 89, 1993.
4. Grace, J.R., Reflections on Turbulent Fluidization and dense suspension upflow,
Powder Technology, 113 (2000), 242-248.
5. Monazam, E.R. and Shadle, L.J., Method and Prediction to Determine
Transitional Velocities in a CFB’s Riser, Ind. Eng. Chem. Res., 2011, 50 (4), pp
1921–1927.
6. Ludlow, C., Lawson L. O. and Shadle, L. J., Proc. Cir. Fluid. Bed Tech. VII
(Grace, J.R., J., and de Lasa, H. (Eds.)), Can., Soc, Chem. Eng. Ottawa, 2002,
pp, 513-520.
7. Monazam, E., Shadle, L. J., and Lawson, L., A Transient Method for
Determination of Saturation Carrying Capacity. Powder Technology, 121 (2005),
205-212.
8. Mei, J. S., Shadle, L J., Yue, P. C., and Monazam,E. R., 12th International
Fluidization, Vancouver, Canada, 2007, p. 63.
9. Mei, J S., Lee, G. T. Seachman,S. M., Ludlow, J. C., and Shadle, J. L.,
Proceedings of the 9th International Conference on Circulating Fluidized Beds,
Hamburg, Germany, 2008, p. 177.
10. Bierl, T. W., Gaido, L. J., McIver, A. E. and McGovern, Jr., J. J., Studies in
Support of
Recirculating Bed Reactors for the Process of Coal, Final Report, Carnegie-
Mellon University, Department of Energy Contract No. EX-C-76-01- 2449,1980.
THE DEVELOPMENT OF A NOVEL Cu-Mn OXYGEN CARRIER
FOR THE CHEMICAL LOOPING GASIFICATION OF BIOMASS
Milad Aghabararnejad, Jamal Chaouki*, Gregory S. Patience
Department of Chemical Engineering, Ecole Polytechnique de Montreal, C.P. 6078,
succ. Centre-Ville, Montreal, Que. H3C 3A7, Canada
* Corresponding author: Tel.: +1-514-340-4711 X 4034; fax: +1-514-340-4159.

E-mail address: jamal.chaouki@polymtl.ca
ABSTRACT
Circulating fluidized bed technology applied to combustion processes in which oxygen
and fuel are fed into separate reactors is referred to as Chemical Looping Combustion.
Typically, oxygen reacts with a reduced metal (-oxide), then it is transferred to a second
vessel where the metal oxide is reduced by a hydrocarbon. In chemical looping
gasification, a fuel is contacted indirectly by oxygen and/or steam again with a metal
oxide shuttling between two vessels reducing the contact between fuel and air. In this
case, a concentrated stream of syngas exits the fuel reactor undiluted by nitrogen. The
objective of this study is to develop a solids substrate capable of releasing oxygen in
the fuel reactor. A bimetallic Cu-Mn oxygen carrier was synthesized by incipient
wetness impregnation at ambient conditions over Al2O3. Copper-based oxygen carriers
have superior oxygen transfer capacity and environmental and economical
characteristics compared to nickel, iron and cobalt, but the operating temperatures are
limited due to the low melting point of the metallic copper. Adding manganese to copper
minimizes the formation of copper aluminate. Moreover, it inhibits copper agglomeration
and carbon deposition. The developed oxygen carriers were characterized by BET,
XRD and SEM analyzers. Also, oxygen transfer capacities of particles were tested
using thermo gravimetric analysis (TGA). Results indicate that Cu-Mn is a superior
carrier, which is suitable for the separation of oxygen in a chemical looping process.
Also, adding manganese to copper allows working at high temperatures and improves
the reactivity of copper.
INTRODUCTION
Energy-efficient practices are becoming more and more necessary as energy prices
continue to rise and the impact of climate change emerges. Institutions that adopt
measures to reduce energy and its associated greenhouse gas emissions will obtain
financial, environmental, and social benefits. New opportunities for biomass energy are
developing as environmental and economic concerns encourage governments,
industries, and consumers to explore alternatives to fossil fuels.
Combustion and gasification are two processes, which convert hydrocarbons to energy.
Gasification has some advantages over combustion, such as higher efficiency, treating
with a lower volume of gas and low emission of toxic gases. Gasification also makes it
possible to have synthesis fuels, which can be used for transportation. However, an
1
oxygen separation unit is needed before each gasification process, which can raise the
capital and variable costs of the process. A chemical looping process is a relatively new
technology for combustion and gasification processes. Figure 1 shows a schematic of a
chemical looping combustion process.
Figure 1: Chemical looping combustion
Chemical looping combustion consists of two reactors. On the right side is the fuel
reactor, where oxygen from a metal oxide (MyOx) reacts with fuel according to the
following reaction:
(2n+m)MyOx + CnH2m → (2n+m) MyOx-1 + mH2O + nCO2
On the left side is the air reactor, where an oxidation reaction occurs between reduced
metal oxide (MyOx-1) and air:
MyOx-1 + 1/2O2 → MyOx
Consequently, CO2 is separated from water by condensing the product stream. Both
reactors should operate as circulating fluidized beds in order to supply the circulation of
oxygen carrier between the two beds. It has been reported that chemical looping
combustion is the most economical way to capture CO2 compared to post capture and
oxyfuel processes (1). Besides combustion, chemical looping is a suitable technology
for gasification. It can provide the oxygen needed for gasification reactions. In this way
a pure syngas can be obtained.
Mattison and Lyngfelt found that some oxide systems of the transition metals, Fe, Cu,
Co, Ni and Mn could be used as oxygen carriers (2). Some researchers (3-5) reported
that nickel is the best oxygen carrier in terms of reactivity, although there are
thermodynamic restrictions in the presence of CO and H2 (6). Hossain et al. (7-9)
observed that carbon deposition is a major problem in dealing with nickel carriers.
In addition to nickel, copper deserves serious consideration due to its high reactivity
and low cost. De Diego et al. (10) developed Cu-based oxygen carriers by mechanical
2
mixing, co-precipitation, and impregnation methods. They analysed the behaviour of
CuO in a thermogravimetric analyser. Their results showed that carriers prepared by
impregnation exhibited excellent chemical stability without sustainable decay of the
mechanical strength in multicycle testing. Copper suffers from agglomeration due to its
low melting point. Researchers have tried to improve the properties of copper by using
promoters. Adanez et al. (6) prepared a nickel-copper oxygen carrier using the dry
impregnation method. They showed that CuO is used for the reduction reaction before
NiO. In addition, it was observed that NiO stabilized the CuO and allowed working at
950οC.
Pure manganese oxide is expected to release oxygen at 900οC, but there are
thermodynamic limitations for the reoxidation of these materials at low oxygen
concentration levels in the air reactor at elevated temperatures (11). Recently,
Moghtaderi (12) studied the separation of oxygen from air in a chemical looping process
and demonstrated that a 1:1 mixture of Mn/Co metal oxide systems has more
favourable redox characteristics than its parent materials.
Considering the different properties of individual Mn- and Cu-based oxygen carriers, the
objective of this work was to use manganese as a promoter for the copper oxygen
carrier. It is claimed that manganese can enhance the thermal stability of copper as well
as its reactivity.
EXPERIMENTS
Oxygen Carrier Preparation
The incipient wetness impregnation method was used for catalyst preparation. In the
following order a specific amount of nitrate hydrate salt of the desired metal was mixed
with distilled water. All salt should be dissolved in water. Then, activated alumina was
added gradually as a binder to the nitrate solution until it makes a paste. The entire
amount of water solution should be adsorbed by the pores of the binder. Drying, which
is the next step, was performed at 140οC for 12 hours. Finally, prepared powders were
calcined at 850οC for 5 hours in air atmosphere. In each impregnation step a specific
amount of active phase settles on the support. Impregnation steps should be repeated
in order to reach the desired concentration of the active phase. Stirring can be done at
higher temperatures in order to increase the solubility of salt in water and,
consequently, increase the amount of settling of the active phase on the binder during
each impregnation step. Copper, manganese, nickel, and cobalt have been used as the
active phase and activated alumina as the binder. Also, in the case of the bimetallic
oxygen carrier 50-50% of each metal has been used. Table 1 shows the amount of
loading of the active phase versus impregnation steps:
3
Table 1. Loading of active phase versus impregnation step
%Metal loading
Impregnation Step ௪௘௜௚௛௧ ௢௙ ௠௘௧௔௟
(௪௘௜௚௛௧ ௢௙ ௠௘௧௔௟ା௪௘௜௚௛௧ ௢௙ ௦௨௣௣௢௥௧ ∗ 100)
1 10.8
2 18.6
3 24.6
CHARACTERIZATION
Several techniques have been used to characterize the prepared oxygen carriers. A
laser diffraction apparatus has been used to determine the particle size distribution of
powders. The surface area of the oxygen carrier was measured by BET. The
identification of the crystalline phases of the oxygen carrier was carried out using
powder X-ray diffraction (XRD) analysis in an X-ray diffractometer using Cu-Kα
radiation. Changes in morphology were determined in a scanning electron microscope
(SEM). Table 2 shows the physical properties and the crystalline phases of the oxygen
carrier.
Table 2. Properties of prepared oxygen carriers

Particle Surface Density
Sample 2
XRD phases (fresh)
size(µm) area (m /g) (kg/m3)
Cu 109 67.49 2346 CuO, Cu2O, CuAl2O4, Al2O3
Cu-Co 127 45.92 2383 CuO, CoO, CuAl2O4, Al2O3
2437 CuO, Cu2O, NiO, CuAl2O4, NiAl2O4,

Cu-Ni 140 61.25
Al2O3
2135 CuO, Cu2O, MnO, Mn3O4, MnAl2O4,

Cu-Mn 102 58.99
Al2O3
The reactivity of the oxygen carrier was determined using a thermogravimetric analyzer.
For the reactivity test 20 mg of sample were exposed to alternating reduction and
oxidation cycles. The particles were well spread out in the platinum basket (5 mm in
diameter and 1 mm in height) forming a single layer, thus avoiding the inter-particle
mass transfer resistance. Air (20 ml/min STP) was used as the oxidizing agent and
nitrogen (20 ml/min STP) was used as carrying gas during the reduction step. The
experiments were carried out at 800οC and atmospheric pressure. Usually, the reactivity
of the oxygen carrier will reach a constant value after the second cycle. However, the
reactivity data related to the fifth cycle has been chosen for comparison purposes.
4
The purpose of this study was to separate oxygen from air using a chemical looping
process. The main step for commercializing the process is to develop an oxygen carrier
with superior reactivity and stability properties. Besides having high reactivity during
oxidation and reduction reactions, an oxygen carrier should have sufficient thermal and
mechanical stability and be environmentally friendly and inexpensive.
Copper is one of the candidates for the oxygen carrier in the chemical looping process.
Its high reactivity, low cost, and friendly environmental properties make it one of the
best materials, like metal oxide. However, copper suffers from agglomeration due to its
low melting point (1083οC). In chemical looping processes, the oxygen carrier must
pass around one hundred thousand cycles through circulating fluidized beds. As a
result, agglomeration can be a huge problem. For this reason, it is suggested to use a
bimetallic Cu-Mn oxygen carrier. It has been shown that besides increasing the
agglomeration resistance, manganese can enhance the oxygen transport capacity of
copper oxide. During calcination, which is one of the catalyst preparation steps, a solid-
solid reaction takes place between copper oxide and alumina as the binder. During this
reaction CuAl2O4 forms, which has a higher oxidation temperature compared to CuO.
Consequently, it is trying to avoid the reaction between copper and alumina. During
XRD experiments, it was investigated whether adding manganese can decrease the
amount of copper aluminate, because between copper and manganese, the latter has a
higher tendency to react with alumina. Thus, CuO remains as the active phase. The
oxidation and reduction reactions are:
Cu+1/2O2→CuO
CuO→Cu+1/2O2
Figure 1 shows SEM micrographs for Cu and Cu-Mn oxygen carriers before and after
20 oxidation-reduction cycles. It is evident that copper particles stick together at 800ο C
because of agglomeration. By adding manganese, copper particles can withstand
higher temperatures without agglomerating.
5
Figure 2. SEM micrograph of fresh and after 20 cycles tests in TGA of samples Cu, Cu-Mn
Particle diameter will increase because of agglomeration and it can cause de-
fluidization of the bed. Figure 3 compares the reactivity of various oxygen carriers,
which were prepared in this study.
Figure 3: Oxidation and reduction activity of different carriers
Cu-Mn has a high oxygen transport capacity as well as high oxidation and reduction
rates compared to other carriers. Figure 4 shows the effect of a number of oxidation-
reduction cycles on the reactivity of the Cu and Cu-Mn oxygen carrier.
Figure 4. Reactivity versus number of cycles (left) Cu (right) Cu-Mn
6
In the case of pure copper, its reactivity will decrease as it is cycled and especially from
the first to second cycle due to agglomeration and the formation of copper aluminate.
Manganese can stabilize the reactivity of copper as can be seen in Figure 4(b).
CONCLUSION
Biomass as a renewable source of energy has been the focus of much interest in recent
years. Gasification technology is very effective in terms of conversion of biomass,
environmental aspects, efficiency, etc. However, the gasification process has some
challenges, such as oxygen separation. In the present study, a chemical looping
process was proposed for the separation of oxygen from air using a novel oxygen
carrier. To achieve this, a Cu-Mn oxygen carrier was prepared via the incipient wetness
impregnation method. The performance of the oxygen carrier to separate oxygen from
air was tested in a thermogravimetric analyzer. Results showed that manganese can
enhance the properties of copper. By increasing the agglomeration temperature of
copper, it can withstand high temperatures. Also, adding manganese decreases the
possibility of forming copper aluminate during the calcination process resulting in
improved reactivity.
REFERENCES
1. Moghtaderi, B., Wall, T., An overview of chemical looping combustion as a
potential clean coal technology, in Coal 21 conference. 2007: Crowne Plaza Hunter
Valley.
2. Mattisson, T., Lyngfelt, A., Capture of CO2 using chemical-looping combustion,
in First Biennial Meeting of the Scandinavian-Nordic Section of the Combustion
Institute. 2001: Göteborg, Sweden. p. 163-168.
3. Gayán, P., Dueso, C., Abad, A., Adanez, J., F. de Diego, L., García-Labiano, F.,
NiO/Al2O3 oxygen carriers for chemical-looping combustion prepared by
impregnation and deposition-precipitation methods. Fuel, 2009. 88(6): p. 1016-1023.
4. Mattisson, T., A. Järdnäs, and A. Lyngfelt, Reactivity of Some Metal Oxides
Supported on Alumina with Alternating Methane and OxygenApplication for
Chemical-Looping Combustion. Energy & Fuels, 2003. 17(3): p. 643-651.
5. Mattisson, T., M. Johansson, and A. Lyngfelt, The use of NiO as an oxygen
carrier in chemical-looping combustion. Fuel, 2006. 85(5-6): p. 736-747.
6. Adanez, J., García-Labiano, F., F. de Diego, L., Gayán, P., Celaya, J., Abad, A.,
Nickel-copper oxygen carriers to reach zero CO and H-2 emissions in chemical-
looping combustion. Industrial & Engineering Chemistry Research, 2006. 45(8): p.
2617-2625.
7. Hossain, M., Fluidized bed chemical-looping combustion: Development of a
bimetallic oxygen carrier and kinetic modeling. 2007, The University of Western
Ontario (Canada): Canada. p. 178.
8. Hossain, M.M. and H.I. De Lasa. Reduction kinetics of CoO-NiO/AI2O3 oxygen
carrier for chemical-looping combustion. in 2006 AIChE Annual Meeting, November
12, 2006 - November 17, 2006. 2006. San Francisco, CA, United states: American
Institute of Chemical Engineers.
9. Hossain, M.M. and H.I. de Lasa, Reactivity and stability of Co-Ni/Al2O3 oxygen
carrier in multicycle CLC. AIChE Journal, 2007. 53(7): p. 1817-1829.
7
10. de Diego, L. F., Garcı́a-Labiano, F., Adánez , J., Gayán, P., Abad, A., M.
,
Corbella, B., Marıá Palacios J., Development of Cu-based oxygen carriers for
chemical-looping combustion. Fuel, 2004. 83(13): p. 1749-1757.
11. Shulman, A., Cleverstam, E., Mattisson, T., Lyngfelt, A., Manganese/Iron,
Manganese/Nickel, and Manganese/Silicon Oxides Used in Chemical-Looping With
Oxygen Uncoupling (CLOU) for Combustion of Methane. Energy & Fuels, 2009.
23(10): p. 5269-5275.
12. Moghtaderi, B., Application of Chemical Looping Concept for Air Separation at
High Temperatures. Energy & Fuels, 2009. 24(1): p. 190-198.
8
FLOW FIELD IN A NOVEL SHORT RESIDENCE TIME
GAS-SOLID SEPARATOR
Mengxi Liu, Chan Zhou, Chunxi Lu, Zhuan Wang
State Key Laboratory of Heavy Oil Processing
Faculty of Chemical Engineering, China University of Petroleum, Beijing,
Changping, Beijing, P.R.China, 102249
T: 0-8610-89733803; F: 0-8610-89733803; E: mengxi.liu@yahoo.com
ABSTRACT
The gas flow field in a short residence time separator was investigated. The
tangential velocity in the separator housing increases with increasing angle to the
positive x axis, and decreases with increasing radial position. A swirl of opposite
direction to the main current in the separator housing occurs in the gas outlet.
INTRODUCTION
Gas-particle separators play a key role in a gas-solid fluidized bed by effectively

collecting and recycling particles. Over the years, collection efficiency and pressure
drop have been considered as the most important characteristics of a gas-particle
separator (1-3). However, more concerns should be made when a separator is
employed in a specific industrial process in which the reaction time is elaborately
controlled, such as in the fluid catalytic cracking (FCC) process. Preferably, catalytic
cracking reactions only occur in the riser reactor, which usually takes 1 to 5 s (4).
Further contact of the highly active cracking catalysts and the cracked hydrocarbon
vapor in the separator and the dilute phase is harmful, causing unwanted side
reactions and byproducts (5-6). The catalysts are separated from the vapor at the
end of the riser reactor, and the post riser reactor residence time is critically restricted.
This is defined as the time the cracked hydrocarbon product remains in the
separators and the dilute phase. A conventional scheme consists of multiple stage
separators, usually a riser termination device and a cyclone. It provides high
efficiency gas-solid separation, but allows a long and uncontrolled hydrocarbon
post-riser residence time of 15-45 s in the separators and the reactor dilute phase,
which significantly exceeds the time required by catalytic cracking reactions (4).
Work associated with reducing post-riser residence time has been rare, mainly
focused on the reduction in residence time in the separators and in the reactor dilute
phase.
Gas-solid separators can be roughly categorized into centrifugal separators and

inertial separators. A common and traditional centrifugal separator is the cyclone,
which provides high separation efficiency, but allows relatively long contact time of
gas and particles. Typical inertial separators are T-type ballistic riser terminators,
which offer rough separation efficiency of approximately 60%. Recently, some novel
short residence time separators (SRTS) have been proposed. Donsí et al (7)
presented a horizontally placed inertial riser terminator with a U-bend channel.
Pictures and video show a particle-rich layer occurring within the first 60° of the
separator circumference, indicating a rough separation of the gas-particle
suspension. With increasing inlet gas velocity, the collection efficiency approximately
remains constant (nearly 100%) for the high mass flow rate ranging from 260 to 340
kg/m2·s, but significantly decreases for the low mass flow rate less than 90 kg/m2·s.
The retention time of the separation is only 4 ms. Andreus et al (4) presented a
horizontal short contact time separator. In the separator, the gas-particle is
centrifuged in a half-turn elbow, with particles moving downwards through the dipleg
and gas exiting from a gas outlet horizontally located on the center of the separator
head. Results show that the particle collection efficiency increases with increasing
inlet solid loading and reaches an asymptotic value close to 95%. Variation of the
back pressure exerted on the outlet of the dipleg has a slight influence on the particle
collection efficiency, but a significant effect on the gas collection efficiency. A modified
cyclone model was employed for prediction of the particle collection efficiency.
Letzsch et al (5) and Joseph et al (6) proposed a novel separator called a rams horn,
which combines centrifugal with inertial separations. The ram horn separator
contains an upward flowing suspension inlet, a downward flowing solids outlet, a
horizontally flowing gas outlet and a semi-circular separator area. The gas outlet
extends through the separator housing and contains a horizontally disposed gas
opening. Gas-solid suspension enters the SRTS vertically upwards and is then
centrifuged in a half-turn elbow. Particles segregate at the concave wall of the
separator housing and move vertically downward from the solid outlet, while the gas
is withdrawn through gas openings on the gas outlet. The ram horn separator
provides a number of significant potential advantages: small size, simple
configuration, high collection efficiency, low pressure drop and short gas residence
time. This work evaluates a novel ram horn-type short residence time separator with
multiple gas openings uniformly disposed on the gas outlet.
MODEL DESCRIPTION
Mathematic Models
The flow field in a SRTS is characterized by a strongly swirling flow and anisotropic
turbulence. The k-ε model, algebraic stress model (ASM) and Reynolds stress model
(RSM) have been commonly employed in flow field simulation, but the RSM provides
a more precise estimation on the strongly swirling flow and anisotropic turbulence (1).
The governing equations of the continuous phase can be written as
∂ ∂ ∂ ∂φ
(ρφ ) + (ρu j φ ) = (Γ φ ) + Sφ (1)
∂t ∂x j ∂x j ∂x j
where φ is a universal variable, Гφ is the transport coefficient, Sφ is the source item.
The expression of φ, Гφ and Sφ in different equations is listed in Table 1, where
σk=0.82 and σε=1. The inlet boundary was set as the uniform velocity inlet, and the
turbulence quantities were also uniformly imposed on the inlet by using the
correlations: kin=3/2(uinI)2, and εin=Cμ0.75k1.5/l, where I = 0.05, Cμ=0.09, l =0.07 DH, and
DH = 0.108 m. The boundary condition at the gas outlet was based on the fully
developed flow assumption where the gradients of all variables in the flowing
direction were taken to be zero. No-slip conditions were assumed at the wall.
Table 1 Governing equations of the CFD model
Equations φ Γφ Sφ
Continuty equation 1 0 0
μ∂u j
∂( )
∂p ∂xi ∂( ρui' u 'j )
Momentum equation ui μ − + + ρg i −
∂xi ∂x j ∂x j
Turbulence dissipation equation ε μ + μt / σε ε(cε1Pii / 2 − cε 2 ρε ) / k
Reynolds stress equation ui' u 'j μ+ μ /σ Pij + εij + φij
t k
Geometric Model
The inlet gas velocity is set as 16.12 m/s. The schematic diagram and structured
mesh of the SRTS is shown in Fig. 1. It is seen that the SRTS contains a
semi-circular separator housing which is connected with an inlet of upward flowing
gas-solid suspension and a downward flowing solid outlet or dipleg. A 156 mm ID gas
outlet is horizontally and centrally located, extending through the separator housing
and paralleling the base of the separator and the inner concave surface of the
separator housing. Several horizontal gas openings are disposed uniformly around
the gas outlet. The width of the inlet and outlet is 68 mm and 73 mm, respectively.
The radius of the concave surface and the width of the separator housing is 157.5
mm and 268 mm. Coordinate directions of x, y, z are illuminated in Fig.1.
(a)
(b)
Fig.1 Schematic diagram and structured mesh of the SRTS
Model Validation
In order to validate the CFD simulation method described above, the predicted
results were compared with available experimental data obtained in a cold model
SRTS having the same size. Fig.2 shows that data from both methods are close,
indicating validation of the established CFD models.
40
35
30
25
ut(m/s)
20
15
10
experiment
5 simulation
0
0.60 0.65 0.70 0.75 0.80 0.85
r/R
Fig. 2 Comparison of results from experiment and simulation
Flow Field in Separator Housing
Fig.3 gives the velocity vectors on the vertical plane of z =100 mm of SRTS. In the
range of 0º< A < 180º, the gas velocity is always higher than the inlet gas velocity,
indicating a greater gas flow rate in the SRTS. As shown in Fig. 1, the gas flow in the
SRTS can be categorized into two types: gas flow entering the gas outlet through the
gas openings and gas flow circulating in the separator housing. The latter
significantly increases the gas flow rate in the separator housing, leading to a greater
gas velocity than in the inlet. Moreover, the gas velocity in the bottom region, the
space between the gas outlet and the base, is large, mainly arising from the
decrease of the cross-sectional area.
Fig.3 Velocity vectors on the plane of z =100 mm

The tangential gas velocity governs the centrifugal force and the particle collection.
Fig. 4 shows the variation of tangential gas velocity as a function of dimensionless
radial position and A, the angle to the positive x axial as shown in Fig. 1. It is seen
that the tangential gas velocity decreases with increasing radial position, with the
maximum near the outer surface of the gas outlet and the minimum at the vicinity of
the inner concave surface of the separator housing. The tangential gas velocity also
varies along the circumference. As shown in Fig. 4, the tangential velocity decreases
as A increases, arising from the decrease of the gas flow rate and leading to
decreasing centrifugal force.
36 A = 0°
34 A = 45°
A = 90°
32 A = 135°
30 A = 180°
ut, m/s
28
26
24
22
20
0.5 0.6 0.7 0.8 0.9 1.0
r/R
Fig. 4 Variation of tangential gas velocity as a function of radial position and A
8
10
A = 0° 6
8 A = 45° 4
6 A = 90° 2
A = 135° 0
uz, m/s
4
ur, m/s
A = 180° -2
2 -4 A = 0°
-6 A = 45°
0 -8 A = 90°
A = 135°
-2 -10 A = 180°
-12
0.5 0.6 0.7 0.8 0.9 1.0 0.5 0.6 0.7 0.8 0.9 1.0
r/R r/R
(a) radial gas velocity (b) axial velocity component
Fig. 5 Variation of radial and axial velocity components as a function of radial position
and A
Fig. 5 presents the variation of radial and axial velocity components as a function of
radial position and A. In this work, the radial velocity in the direction opposite to the
centrifugal force is defined to be positive. It is seen that the radial velocity decreases
with increasing A within the first 45º of the separator circumference, while it is
approximately zero when A is greater than 45º. The axial velocity does not show a
regular variation, except that it is negative at the vicinity of the gas outlet (r/R=0.495),
probably influenced by the gas flow in the gas outlet which also has a negative axial
velocity.
Flow Field in the Bottom Region
As discussed before, gas not only enters the gas outlet through the gas openings,
but also circulates in the separator housing. The variation of the cross-sectional area
of the bottom region governs the circulation gas flow rate and influences the pressure
drop of the SRTS, while the former significantly increases the gas flow rate in the
SRTS and affects the particle collection efficiency. Fig. 6 shows the tangential gas
velocity in the bottom region. When gas passes through the bottom region, the
tangential velocity increases first, reaches the maximum when x is close to 0, and
then decreases. This is dominated by the variation of the cross-sectional area of the
bottom region, with a contraction for x<0 and an enlargement for x>0 (Fig. 1). Fig. 6
shows that the tangential velocity also changes with the distance to the gas outlet.
The closer to the gas outlet, the higher the tangential velocity. This is similar to the
variation of the tangential velocity for 0º<A<180º.
35
30
25
ut, m/s
20 y = -92mm
y = -102mm
y = -112mm
15
y = -122mm
10
-0.06 -0.04 -0.02 0.00 0.02 0.04 0.06
x, m
Fig. 6 Variation of the tangential velocity in the bottom region
Fig.7 (a) presents the profile of the radial velocity in the bottom region. It is seen that
the radial velocity increases with increasing x, with consistently negative values for
x<0, which is probably caused by inertial force, and positive velocity for x > 0.
Moreover, the radial velocity increases with height. The axial velocity seems to be
almost constant along the x axis, Fig.7(b).
6 y = -92mm 6
4 y = -102mm 4
2 y = -112mm
2
y = -122mm
0 0
ur, m/s
-2
uz , m/s
-2
-4
-4 y = -92mm
-6 y = -102mm
-8 -6
y = -112mm
-10 -8 y = -122mm
-0.06 -0.04 -0.02 0.00 0.02 0.04 0.06 -10
-0.06 -0.04 -0.02 0.00 0.02 0.04 0.06
x, m x, m
(a) (b)
Fig. 7 Variation of the radial and axial velocities in the bottom region
Flow Field in the Gas Outlet
Fig. 8 presents the tangential velocity variation in the gas outlet. It is seen that the
tangential velocity is consistently negative, indicating a clockwise swirling flow
occurring in the gas outlet. Gas openings were initially made with slanting edges.
These slanting edges lead to a sharp turn when the gas-particle suspension enters
the gas openings. In this way, particles are separated by inertial force. The tangential
velocities are close to each other for different A, signifying that every gas opening on
the gas outlet gets approximately the same gas flow rate. Moreover, the tangential
velocity is very small for r/R close to zero, mainly caused by the eddy at the center of
the gas outlet.
The axial gas velocity at different cross sections of the gas outlet is shown in Fig. 9. It
is seen that the axial velocity near the wall of the gas outlet is greater than that at the
center. There is a big difference in the axial velocity between the cross sections of
z=100 mm and 200 mm, signifying a spiral motion in the gas outlet. Moreover, the
evolution of the axial velocity along the radial direction at the cross-section of z=600
mm is more fluent than that of z=100 mm and 200 mm, signifying a fully developed
flow near the exit of the gas outlet.
0
A = 45°
-5 A = 135°
A = 225°
A = 315°
-10
ut , m/s
-15
-20
-25
0.0 0.2 0.4 0.6 0.8 1.0

r/R
Fig. 8 Tangential velocity in the gas outlet
5 z = -100 mm
z = -200 mm
z = -600 mm
0
-5
uz, m/s
-10
-15
-20
0.1 0.2 0.3 0.4 0.5 0.6 0.7 0.8 0.9 1.0
r/R
Fig. 9 Axial velocity at different cross-sections of gas outlet
CONCLUSION
The flow field in a novel ram horn-type short residence time separator (SRTS) was
investigated by CFD simulation. The gas flow rate in the SRTS is significantly greater
than the feed flow rate. The tangential velocity in the separator housing increases
with the increase of the angle to the positive x axis, and decreases with increasing
radial position. The radial velocity is positive at the vicinity of A=0º, but approximately
equals zero in the remaining regions. Influenced by the gas flow in the gas outlet, the
axial velocity is negative at the vicinity of the gas outlet (r/R=0.495). In the bottom
region, the tangential velocity is governed by the cross-sectional area of the region.
The radial velocity increases with increasing x, being negative for x<0 and positive
for x>0. Because of the slanting edges of the gas openings, the gas passing through
the gas openings in the reverse direction, and a swirl in the opposite swirling
direction to the main flow in the separator housing occurs in the gas outlet.
NOTATION
A angle of the gas opening to positive x axis, º

DH hydrodynamic diameter, m
k turbulent kinetic energy
I turbulence intensity
Sφ source item of equation (1)
ur radial velocity, m/s
ut tangential velocity, m/s
uz axial velocity, m/s
x x axis as shown in Fig.1
Greek letters
φ universal variable, -
Гφ transport coefficient,-
ρ density, kg/m3
μ viscosity, Pa.s
σ k, Prandtl number of turbulent kinetic energy k
σε, Prandtl number of turbulent dissipation rate ε
ε turbulent dissipation rate, m2/s3
REFERENCES
1. G. Wan, G. Sun, X. Xue, M. Shi. Solids concentration simulation of different size

particles in a cyclone separator. Powder Technol., 183 (2008), 94-104.
2. L. Shi, D.J. Bayless. Comparison of boundary conditions for predicting the
collection efficiency of cyclones. Powder Technol., 173 (2007), 29-37.
3. F. Kaya, I. Karagoz. Numerical investigation of performance characteristics of a
cyclone prolonged with a dipleg. Chem. Eng. J. 151 (2009), 39-45.
4. R. Andreux, G. Ferschneider, M. Hémati, O. Simonin. Experimental study of a
fast gas-particle separator. Chem. Eng. Res. and Des. 85(6) (2007), 808-814.
5. W. S. Letzsch, G. Earl. Short residence time cracking apparatus and process.
U.S. Patent 5, 662, 868, Sep. 2, 1997
6. J.L. Ross, Jr., C.S. Caty, C.J. Horecky. Apparatus for separating fluidized
cracking catalysts from hydrocabon vapor. U.S. Patent 5, 259, 855. Nov. 9, 1993.
7. G. Donsì, L.S. Osséo, M. Schenato. Experimental characterization of a short
retention time gas-solid separator. Powder Technol., 85 (1995), 11-17.
CO-GASIFICATION OF BIOMASS AND COAL IN AN 8 MW
DUAL FLUIDIZED BED STEAM GASIFIER
Christoph Pfeifer, Isabella Aigner, Hermann Hofbauer

Getreidemarkt 9/166, A-1060 Vienna, Austria
ABSTRACT
Gasification of biomass is an attractive technology for combined heat and power

production. Co-gasification of biomass and coal was tested in an 8 MW dual
fluidized bed steam gasifier with coal ratios up to 22% on an energy basis.
Hydrogen levels in the producer gas increased with the addition of coal as well as
ammonia, hydrogen sulfide and tars. Addition of coal to the system stabilized the
process and improved gas quality.
INTRODUCTION
Coal as a substitute for oil is nothing new. During the oil crises in the 1970s and up
until the middle of the 1980s, coal was already being used as a substitute for oil (1).
But in these days, not only was an oil substitute required but also a way to minimize
the carbon dioxide emissions, which many countries agreed to in the Kyoto protocol.
Since carbon dioxide emissions from biomass are perceived as being neutral (1),
and since coal is a fuel with a high availability (especially in politically stable
countries) and is less expensive than oil, the gasification of mixtures of these two oil
alternatives is a natural consequence. The availability of biomass fluctuates mostly
with the season (2), hence the idea of gasifying miscellaneous mixtures in one plant
looks economically advantageous. Generally, co-firing is the use of different fuels at
the same time for combustion or gasification. For example, biomass is co-fired in
existing coal plants with fuels that cannot be burned alone because of the low
energy content (such as sewage sludge), and it could be burned together with
natural gas to give a good performance. In industrial coal-fired power plants co-firing
is often used to add a green fingerprint without any loss in efficiency and with only
minor changes to plant settings. Therefore, only low percentages of the other fuels
are usually used. Co-combustion of biomass with coal is a matter of intensive
research for different applications and several comprehensive studies exist on this
topic (3-11). Different types of reactors can be used such as fixed bed, fluidized bed,
dual fluidized bed and entrained flow reactors. Co-firing can be accomplished via
three different modifications, which are direct, indirect and parallel co-firing. The first
two are favorable since for indirect co-firing a separate gasification unit is required.
Direct co-firing uses blends of both fuels, and for parallel co-firing the fuels are fed
into separate boilers to produce steam. Different kinds of fuels have been
investigated, such as agricultural residues together with coal (12). Moreover, the use
of energy plants such as Cynara (13) and sewage sludge (14) are options for the co-
firing of biomass feedstocks together with coal. Recently, the co-gasification of
biomass and coal has attracted more interest due to the environmental benefits
such as reduced sulfur and nitrogen emissions when adding biomass to the fuel for
systems designed for coal. Moreover, CO2 emissions can also be reduced. Several
reports about co-gasification are available (15-19). However, only a small amount of
literature is available for tests with different ratios of biomass and coal (2,20-21).
Within this work the suitability of coal for the dual fluidized bed gasification process
was tested in a commercially operated 8 MW plant in Güssing, Austria. In order to
guarantee a positive test run at the plant, test runs at the 100 kW scale were
previously undertaken (22-23). These tests showed that blend ratios of 0 to 100%
were possible. Thus, the goal of the tests described in this paper was to verify the
findings from the pilot scale to the large scale. Due to the limitations (see the
Results section) of existing plants, the maximum possible coal ratio was 22% in
terms of energy. However, the general aim was to demonstrate the fuel flexibility of
the dual fluidized bed process.
EXPERIMENTAL
Producer gas Figure 1 shows the

(CH4, CO, H2, CO2, H2O) Flue gas
principles behind the dual
Heat fluidized bed steam
gasification process and
Gasification Combustion Figure 3 shows a schematic
(~ 850 °C) (~ 920 °C) of the process. The biomass
Additional
Biomass fuel enters a bubbling fluidized
Circulation bed gasifier where drying,
(bed material, thermal degasification, and
Steam char coal) Air
partially heterogeneous char
gasification take place at
Figure 1: Principles behind the dual fluidized bed gasifier
bed temperatures of about
850-900 °C. The residual
biomass char leaves the gasifier together with the bed material through an inclined,
steam fluidized chute, towards the combustion reactor. The combustion reactor is
used to heat up the bed material and is designed as a highly expanded fluidized bed
(riser). Air is used as a fluidization agent in the riser. After particle separation from
the flue gas in a cyclone, the hot bed material flows back to the gasifier via a loop
seal. Both connections, between the loop seal and the chute, are fluidized with
steam, which effectively prevents gas leakage between the gasification and
combustion zones and also allows high solid throughput. The temperature difference
between the combustion and the gasification reactors is determined by the energy
needed for gasification as well as the circulation rate of the bed material. The
system is inherently auto-stabilizing since a decrease in the gasification temperature
leads to higher amounts of residual char, which results in more fuel for the
combustion reactor. This, in turn, transports more energy into the gasification zone
and thereby stabilizes the temperature. In practical operations, the gasification
temperature can be influenced by the addition of fuel (e.g. recycled producer gas,
sawdust, etc.) into the combustion reactor. The pressure in both gasification and
combustion reactors is close to atmospheric conditions.
The process yields two separate gas streams at high temperatures: a high quality
producer gas and a conventional flue gas. The producer gas is generally
characterized by a relatively low content of condensable higher hydrocarbons (2-
10 g/m³ of so called tars, heavier than toluene), low N2 (< 1 vol%db), and a high H2
content of 35-40 vol%db. For practical use, Olivine, a natural mineral, has been
proven to be a suitable bed material with enough resistance to attrition and
moderate tar cracking activity.
A combined heat and power plant in Güssing, Austria
The demonstration plant in Güssing was developed based on the results gathered
from a 100 kWFuel input pilot plant at Vienna University of Technology. The fuel power
of the demonstration plant is 8 MWFuel input, the electrical output is 2 MW and the
thermal output 4.5 MW. A simplified flow sheet is shown in Figure 2. More than
42,000 hours of combined heat and power (CHP) operation has been achieved
since it was commissioned in 2002. Wood chips from the forestry are used as fuel.
The producer gas is cooled and cleaned by a two-stage cleaning system. A water
cooled heat exchanger reduces the temperature from 850-900 °C to about 160-
180 °C. The first stage of the cleaning system is a fabric filter to separate the
particles and some of the tar from the product gas. These particles are returned to
the combustion zone of the gasifier. In the second stage, the gas is liberated from
the tar by a scrubber. At the same time, the product gas is cooled down to about
40 °C, which is necessary for the gas engine. The spent scrubber liquid saturated
with tar and condensate is vaporized and fed into the combustion zone of the
gasifier for thermal disposal. If the gas engine is not in operation the entire amount
of producer gas can be burned in the boiler to produce heat. The sensible heat of
the engine´s flue gas is used to produce district heat, and the flue gas from the
combustion zone is used for preheating air and superheating steam, as well for
delivering heat to the district heating grid.
Figure 2: Simplified flow sheet of the combined heat and power plant in Güssing, Austria
Analysis
The components CH4, H2, CO, and CO2, as well as O2, were measured by a
Rosemount NGA 2000. The components N2, C2H4, C2H6, and C3H8 were measured
via an online gas chromatograph. Minor contaminants (H2S, NH3) and tar were
measured between the producer gas filter and the scrubber. The tars were sampled
isokinetically with washing bottles with toluene as the absorption liquid and
gravimetric as well as GC/MS tars were determined. For the ammonia
measurement, gas was sampled in a similar way to the tar measurements, using
washing bottles. The solvent used in this procedure was diluted sulfuric acid at a
temperature of about 2 °C. Hydrogen sulfide was again sampled first using washing
bottles filled with an aqueous potassium hydroxide solution at a temperature of
about 2 °C. Subsequently, the H2S values were determined by potentiometry. The
flue gas was measured with a Rosemount NGA 2000 (CO, CO2, O2, and NO).
Sulfure dioxide (SO2) was measured by potentiometry after sampling with washing
bottles with an aqueous potassium hydroxide solution as the absorption liquid at a
temperature of about 2 °C. Details about the measurement methods can be found
elsewhere (22).
RESULTS
Throughout the whole test campaign all of the main parameters were kept constant;
where this was not possible it will be mentioned in the following discussion. The bed
pressure in the gasification section was adjusted to 120 mbar, the steam-to-fuel ratio
to 0.67 kgsteam/kgdry fuel (which corresponded to 1.35 kgsteam/kgcarbon) and the
gasification temperature was 870 °C by default. A schematic of the gasification
reactor and a regime map of the gas/solid contact are given in Figure 3 and Figure
4, respectively. A comprehensive description of the gas/solid contact in a fluidized
bed reactor was previously given (24-25).
Figure 3: Process schematic of the dual fluidized bed Figure 4: Regime map of the dual fluidized
gasifier in Güssing, Austria bed gasifier in Güssing, Austria (25)
It can be seen that the regime in the gasification section of the reactor is a bubbling
bed, whereas the combustion section lies in the fast fluidization section. The
operational area is determined by the fact that producer gas is produced in the bed
over the height and in the combustion section air is introduced at three different
levels. The superficial gas velocity in the riser after the secondary inlet ranges from
10 to 13 m/s, whereas superficial gas velocities of 1.8 to 3 m/s occur in the
gasification zone. The minimum fluidization velocity Umf for both reactors (product
gas at 850 °C and flue gas at 920 °C) varied from 0.11 to 0.13 m/s, and the terminal
velocity Ut was in the range of 4.6 to 5.3 m/s.
Untreated wood chips from the forestry were used (mainly hard wood) as a standard
fuel for the plant. Polish hard coal was added at ratios of 12, 18, and 22% on an
energy basis. The proximate and ultimate analyses of the fuels are listed in Table 1.
Each operation point was applied for at least one day in order to obtain reliable
figures. It should be mentioned that due to an accumulation of coal in the system the
gasification temperature slightly increased at the operation point with 22% of coal.
However, at the pilot scale it was possible to operate the gasifier even with 100% of
coal, whereas the load had to be reduced due to the low reaction rate of coal at
these temperatures (23).
Polish hard coal Wood chips

Dry basis As received Dry basis As received
Water content - 6.11 - 27.7
Ash content 2.89 2.76 1.0 0.94
C 82.17 78.43 48.82 46.06
H [mass %] 4.57 4.36 5.87 5.54
N 1.66 1.58 0.15 0.14
O 8.08 12.27 44.16 47.32
S 0.14 0.13 0.005 0.003
Volatile matter [mass %] 34.68 33.1 84.02 79.27
Fixed carbon [mass%] 65.32 62.35 15.98 15.08
LHV [MJ/kg] 31.6 30.1 18.2 17.0
Table 1: Proximate and ultimate analyses of the fuels
Figure 5 shows the main producer gas components and Figure 6 shows the higher
hydrocarbons as well as the lower heating value LHV vs. the coal ratio. Hydrogen,
carbon monoxide and methane slightly increased whereas carbon dioxide
decreased. Surprisingly, the opposite trend was found for carbon monoxide in the
pilot plant (fluidization 2010). Ethane (C2H6) and propane (C3H8), showed no
significant trend, whereas ethene (C2H4) seemed to decrease slightly, which
corresponds to the findings at the pilot scale (100 kWFuel input) (22). Moreover, the
amount of char transported with the bed material to the combustion zone increased
due to the lower reaction rate of coal in comparison to the biomass. Hence, more
thermal energy bound in char was available in the combustion part of the facility and
less additional fuel needed to be burned in the combustor. This is in fact the
limitation for the coal ratio at the existing plant since the gas burners are cooled by
the gas and the volume flow cannot be reduced under a certain limit. Generally, the
dual fluidized bed gasifier can also handle 100% coal as fuel (22-23), whereas due
to the lower reaction rate of coal in comparison to biomass the load had to be
removed. Another option would be to increase the residence time of the char
fraction in the gasification section to increase the conversion rate by changing the
geometry and/or the bed material circulation rate. In summary, the process was
stabilized since pressure fluctuations due to the devolatilization of the biomass were
reduced. As described above, two different tar measurements were taken via
GC/MS as well as gravimetrically. Three samples were taken daily between the
producer gas filter and the scrubber (see Figure 2). With an increase in the coal ratio
the gravimetric tar and the GC/MS tar increased significantly, as shown in Figure 7.
The same trends, although less distinctive, were found at the pilot scale. Figure 8
shows the nitrogen and sulfur mass flows into the gasifier via the fuel versus the
applied coal ratio. The mass flows of nitrogen released as NH3 and sulfur released
as H2S with the producer gas are displayed. Linear trends were measured for both
impurities. Nearly all sulfur ended up in the producer gas as H2S, whereas only
about 50% of the nitrogen inlet flow was transferred to ammonia. This correlation
was previously found for the dual fluidized bed steam gasification technology (26).
50 5 15
LHV
H2
40 4
Lower heating value [MJ/Nm³]
Gas composition [vol %dry]
Gas composition [vol %dry]
10
30 3
C2H4
CO
20 CO2 2
5
10 CH4 1
C3H8
C2H6
0 0 0
0 5 10 15 20 25 0 5 10 15 20 25
Coal ratio [energy %] Coal ratio [energy %]
Figure 5: Main producer gas components vs. Figure 6: Higher hydrocarbons and lower heating
coal ratio value vs. coal ratio
5 12 1)
Tar GC/MS released as NH3 Nin
2)
released as H2S
10
4
Tar content [g/Nm³ dry]
8
Mass flow [kg/h]
3 Tar grav
6
Nout1)
2
4
1 Sin
2
Sout2)
0 0
0 5 10 15 20 25 0 5 10 15 20 25
Coal ratio [energy %] Coal ratio [energy %]
Figure 7: Gravimetric and GC/MS tars in the Figure 8: Nitrogen and sulfur mass flows in/out
producer gas vs. coal ratio vs. coal ratio
CONCLUSIONS
The experiments showed that coal can be added to the biomass as fuel for the dual
fluidized bed steam gasification process. The gas composition shifted to higher
hydrogen and carbon monoxide contents, which increased the lower heating value
of the gas. Thus, the H2/CO ratio can be adjusted to the needs of the applied
utilization route (e.g. synthetic natural gas synthesis). The addition of up to 22% coal
on an energy basis could be applied without major operational problems. During co-
gasification the process was stabilized due to the lower reaction rate of coal as well
as to the reduced level of devolatilization. Tar levels in the producer gas slightly
increased. Ammonia and hydrogen sulfide linearly increased with the addition of
coal due to the higher nitrogen and sulfur contents in coal in comparison to biomass.
Generally, the dual fluidized bed system offers excellent fuel flexibility for use in
advanced power cycles as well as in future liquid/gaseous fuel production systems.
ACKNOWLEDGEMENTS
The authors want to acknowledge the financial support of the European Commission
since this work was carried out under the EU Project Flexgas (CONTRACT N°
RFCR-CT-2007-00005) and under the EU Project Fecundus (CONTRACT N°
RFCR-CT-2010-00009). Moreover, the authors would like to express their thanks to
the team members of the ´Testing Laboratory for Combustion Systems´ at Vienna
University of Technology for the measurements as well as their support in analytical
concerns.
NOTATION
Umf minimum fluidization velocity, m/s

Ut terminal velocity, m/s
REFERENCES
1. Prins, M.J., Ptasinski, K.J., Janssen, F.J.J.G. From Coal to biomass gasification:
Comparison of thermodynamic efficiency. Energy, 2007, 1248-1259
2. André, R.N., Pinto, F., Franco, C., Dias, M., Gulyurtlu, M., Matos, M.A.A.,
Cabrita, I. Fluidised bed co-gasification of coal and olive oil industry wastes.
Fuel, 2005, 84(12-13):1635-1644
3. Baxter, L. Biomass-coal co-combustion: opportunity for affordable renewable
energy. Fuel, 2005, 84(10), 1295-1302
4. Dai, J., Sokhansanj, S., Grace, J.R., Bi, X., Lim, C.J., Melin, S. Overview and
some issues related to co-firing biomass and coal. Canadian Journal of
Chemical Engineering, 2008, 86(3), 367-386
5. Gajewski, W., Kijo-Kleczkowska, A. Co-combustion of coal and biomass in the
fluidized bed. Archives of Thermodynamics, 2007, 28(4), 63-68
6. Huang, Y., D. McIlveen-Wright, S., Rezvania, Y.D., Wang, N.H., Williams, B.C.
Biomass Co-Firing in a Pressurized Fluidized Bed Combustion (PFBC)
Combined Cycle Power Plant: A Techno-Environmental Assessment Based on
Computational Simulations, Fuel Processing Technology 87, 2006, 927-934
7. Hupa, M. Interaction of fuels in co-firing in FBC. Fuel, 2005, 84(10), 1312-1319
8. Leckner, B. Co-firing of wastes and biofuels with coal. Proceedings of the
International Symposium on Coal Combustion, 5th, Nanjing, China, Nov. 23-26,
2003
9. Nevalainen, H., Jegoroff, M., Saastamoinen, J., Tourunen, A., Jantti, T.,
Kettunen, A., Johnsson, F., Niklasson, F. Firing of Coal and Biomass and Their
Mixtures in 50 kW and 12 MW Circulating Fluidized Beds-Phenomenon Study
and Comparison of Scales. Fuel, 2007, 86, 2043-2051
10. Sami, M., Annamalai, K., Wooldridge, M. Co-firing of coal and biomass fuel
blends. Progress in Energy and Combustion Science, 2001, 27(2), 171-214
11. Zulfiqar, M., Moghtaderi, B., Wall, T.F. Flow Properties of Biomass and Coal
Blends. Fuel Process. Technol., 2006, 87, 281-288
12. Ghani, W.A.W.A.K., Alias, A.B., Savory, R.M., Cliffe, K.R. Co-combustion of
agricultural residues with coal in a fluidised bed combustor. Waste Management,
2009, 29(2), 767-773
13. Aho, M., Gil, A., Taipale, R., Vainikka, P., Vesala. H., A pilot-scale reside deposit
study of co-ring cynara with two coals in a fluidised bed. Fuel, 2008, 87(1), 58-69
14. Leckner, B., Amand, L. E., Lüucke, K., Werther, J.. Gaseous emissions from co-
combustion of sewage sludge and coal/wood in a fluidized bed. Fuel, 2004,
83(4-5), 477-486
15. Beenackers, A.A.C.M., Maniatis, K. Gasification technologies for heat and power
from biomass. Biomass Gasification and Pyrolysis: State of the Art and Future
Prospects, [Conference], Stuttgart, Apr. 9-11, (1997), 24-52
16. Chmielniak, T., Sciazko, M. Co-Gasification of Biomass and Coal for Methanol
Synthesis. Applied Energy, 2003, 74, 393-403
17. Hernandez, J.J., Aranda-Almansa, G., Serrano, C. Co-Gasification of Biomass
Wastes and Coal-Coke Blends in an Entrained Flow Gasifier: An Experimental
Study. Energy & Fuels, 2009, 24(4), 2479-2488
18. Kurkela, E. Recent results and plans concerning co-gasification of biomass and
coal - an overview. Biomass for Energy and the Environment, Proceedings of
the European Bioenergy Conference, 9th, Copenhagen, June 24-27, (1996),
164-169
19. McLendon, T.R., Lui, A.P., Pineault, R.L., Beer, S.K., Richardson, S. W. High-
Pressure Co-Gasification of Coal and Biomass in a Fluidized Bed. Biomass and
Bioenergy, 2004, 26, 377-388
20. Kumabe, K., Hanaoka, T., Fujimoto, S., Minowa, T., Sakanishi, K. Co-
gasification of woody biomass and coal with air and steam. Fuel, 2007, 86, 684-
689
21. Li, K., Zhang, R., Bi, J. Experimental study on syngas production by co-
gasification of coal and biomass in a fluidized bed. International Journal of
Hydrogen Energy, 2010, 35(7), 2722-2726
22. Aigner, I., Pfeifer, C., Hofbauer, H. Co-Gasification of Coal and Wood in a Dual
Fluidized Bed Gasifier, submitted to Fuel, April 2010
23. Aigner, I., Pfeifer, C., Hofbauer, H. Co-Gasification of Coal and Wood in a Dual
Fluidized Bed Gasifier: Variation of Fluidization Conditions and Load Ratio.
Proceedings of the Fluidization XIII Conference, May 16-21, 2010, Gyeong-ju,
Korea, ISBN: 978-0-918902-57-3, pp. 527-534
24. Grace J.R. Contacting Modes and Behaviour Classification of Gas-Solid and
Other Two-Phase Suspensions. The Canadian Journal of Chemical Engineering,
1986, 353-363
25. Kunii D., Levenspiel, O. Circulating fluidized-bed reactors, Chemical Engineering
Science, 1997, 52(15), 2471-2482
26. Siefert, I.G. Stickstoff-, Chlor- und Schwefelbilanzen über das Biomasse - Block
- Heiz - Kraftwerk Güssing. Vienna: PhD thesis, Vienna University of
Technology, 2004
GAS TRACER STUDY IN A NON MECHANICAL L-VALVE
Mohammad-Mahdi Yazdanpanah1, Ali Hoteit1, Ann Forret1*,Thierry Gauthier1,

Arnaud Delebarre2
1
IFP Énergies nouvelles, Rond-point échangeur de Solaize- 69360 Solaize, France
*T: + 33 (0)4 37 70 20 00; F: +33 (0)4 37 70 20 08; E: Ann.forret@ifpen.fr
2
ESSTIN, Université Henri Poincaré, Nancy, France
ABSTRACT
A gas tracer (Helium) was used to study solid and gas flow in an L-valve. Effect
of solid flow rate and pressure drop variation on the quantity of gas in the
vertical section of the L-valve is presented. Results were then used to calculate
the voidage of the moving solid bed in the L-valve vertical section.
INTRODUCTION
The control of solid flow rate is an important element in many different solid
circulating fluidized bed processes. The solid circulation control could be best
achieved through use of the mechanical valves as in some mature catalytic process
like FCC (1). However, use of the mechanical valves is more complex and limited in
high temperature processes (>800°C) due to the material selection and resistance
problem. Chemical Looping Combustion (CLC) is an example of this kind. CLC is a
promising novel combustion technology involving inherent separation of the CO2 (2).
An oxygen carrier, mostly a metal oxide, transports oxygen from the air reactor to
the fuel reactor while circulating between them. The solid transport rate controls the
extent of reaction conversion in each reactor while controlling the energy balance in
the system. The control of particles circulation rate is hence one of the most
important factors in the CLC system.
The non-mechanical valves are a category of solid flow control devices employing
no mechanically moving part (3). Accordingly, they can be easily adapted to high
temperature conditions such as CLC. An external gas injection is used to control
solid flow rate in these valves. L-valve is one of the possible choices for CLC
process among different existing non-mechanical valves. It is simple in design, easy
to operate, effective in solid flow control and requires minimum maintenance (4;5).
Various studies on the L-valve behavior have been published to date (3;5-9). These
studies mostly illustrate the effect of operating and geometrical parameters on the
solid flow rate actuated in the L-valve and the corresponding pressure drop (3;6-8).
The flow in the horizontal section of the L-valve is an important subject in these
studies. Three flow patterns have been distinguished in horizontal flow based on the
aeration rate including: fast moving stream flow, dune-ripple flow, and dune-slug
flow (5;7;9).
The solid flow in vertical section of the L-valve (standpipe) is in downwards

cocurrent or counter current solid and gas flow. The particles flow in the dense
phase mode due to the gravity force. The pressure drop in this section is developed
through the relative movement of gas and solid (3). As solids are not fluidized,
change in the relative solid–gas velocity can change the pressure drop across the
solid bed. Ergun equation (10) modified for slip velocities is used to calculate the
pressure drop in the standpipe of the L-valve (3;7;11). Gas-solid flow in a standpipe
can be largely divided into non-fluidized and fluidized flows. The non-fluidized bed
flows are divided into the packed bed and the transitional packed bed flows by slip
velocity (12). The slip velocity (vsl) is defined as the interstitial gas velocity (vg) minus
the solid interstitial velocity (vs) with downwards solid velocity as positive direction.
Packed bed flow occurs when the interstitial slip velocity is positive and gas
pressure is higher at the top of the standpipe than at the bottom. The bed porosity is
believed to remain constant regardless of vsl value in this case (12). The transitional
packed bed flow occurs when vsl is negative, and the gas pressure at the bottom of
the standpipe is higher than that at the top (13). Different correlations have been
developed to estimate the voidage of the solid bed in a standpipes. Some of the
existing correlations in the literature are listed in Table 1.
Table 1: Correlations of solid bed voidage in a standpipe/ downcomer ( sp).

Correlation Condition Reference
(ε mf − ε s ) linear relation between Knowlton T. M.
ε SP = ε s + v sl
v mf gas velocity and voidage and Hirsan I. (3)
1−εs
ε SP = 1 −
R Yagi (14)
U Uo
− 0.6 Sand particles
R = 3 . 1( d p ρ s ) 0 .5
for < 0 .0168 dp (503, 232, 90) µm
Ut Ut 3
−0.6 s(2818,2730,2365)kg/m
U U U
R = 23.94( d p ρ s ) 0.3 for > 0.0168 o
Ut Ut Ut
− 0 . 054
ε sp = 0 . 6953
Cd Cd
=
Ar Geldart group A
C ds Cds 18 Re s + 2.7 Re s 1.687 Alumina/Hydrated Li et al. (15)
,
d pρg Qsp ε sp alumina/ FCC catalyst
Re s = ± + νs dp (34.11,46.66, 54) µm
µg A 1 − ε sp
s (2770.4, 2037.4,
1760.9) kg/m3
−0.2
ε sp Cd Cd Ar Sand particles
= 2.25 = Chan C. W. et
D 0.4
Cds Cds 18 Re s + 2.7 Re s 1.687 dp (95) µm, s (2260)
, al. (16)
kg/m3
EXPERIMENTAL SETUP
IFP EN and TOTAL are collaborating on an R&D project on CLC. A novel CLC
design based on the interconnected bubbling fluidized beds was developed at IFP
EN to build a 10 kW th pilot plant. The main concern was to insure an independent
solid flow control, and to achieve minimum gas leakages between the air reactor
and the fuel reactor. A cold prototype was constructed with identical geometrical
dimensions as the hot 10 kW th CLC prototype. The system is schematically
illustrated in Figure 1. Detailed explanation of the system and function of each
section can be find elsewhere (17).
Helium was used to trace the gas flow in different L-valve sections. Helium flow rate
was controlled by means of a He
rotameters at fixed pressures fed detection
from a bottle with 99.99% Helium
purity. A ProtecTM Helium Sniffer
Leak Detector was used as the
Helium measurement device. It is
capable of detecting He sucked in
the device though a sniffer line by
means of a mass spectrometer. The
Helium injection and detection points
are illustrated in Figure 1. Silica
sand was used as the solid in the
current study. The properties of
particles are listed in Table 2.
He
Table 2: Properties of sand Injection
particles used in this study.
Property Value DR1 0.1 m
3 Section I
s (kg/m ) 2650 HR1 1.0 m
ds (µm) 321 Dlv 0.017 m
Hlv 1.27m
d50 (µm) 334 Section II LH 0.14 m
Umf (m/s) 0.068 HL 2.15 m
mf 0.514
s (free settled) 0.46 Figure 1: The scheme of the CLC cold flow
st (tapped) 0.40 prototype. Different Helium injection and
(sphericity) 0.76 detection positions are indicated in the
figure.
GAS TRACING IN THE L-VALVE
The gas and solid flow in two main sections of L-valve were experimentally
investigated. The first section is the vertical part above the external gas injection
point. Second section is the vertical section below external gas injection point
together with elbow and horizontal pipe of the L-valve, (Figure 1). Tracer gas
(Helium) was injected into the fluidization gas of the reactor with low concentration
of 0.33 vol. %. Low inlet concentration of tracer gas was used to ensure that the
tracer gas does not modify significantly properties of the fluidization gas (air). Helium
was then detected in the cyclone gas exit (Figure 1).
Pressure drop in the standpipe ( Pv) is a variable parameter that adjusts to match
the pressure balance across the solid circulation loop. Change of Pv will in turn
change the quantity of gas passing through this section. Series of tests were
conducted where the gas flow rate in the vertical section of the L-valve was
measured for different pressure drops across the element. A unique feature of the
current CLC installation is the possibility to adjust Pv through variation of the
pressure drop across the reactor ( PR) by change of the solid height in the reactor.
This permits control of pressure drop across the standpipe independently from the
L-valve external aeration.
The measurements were conducted during the steady state solid circulation for
different bed height in the reactor with constant external aeration rate in the L-valve
(Qlv). The superficial velocity of the gas and pressure drop in the vertical section of
the L-valve are illustrated in Figure 2. Increase in PR causes the Pv to reduce
from +60 mbar to –30 mbar. The gas flow changes based on the pressure drop
across the standpipe. Two zones can be distinguished for gas flow in the standpipe
(Uv). In the case of high pressure drops in the standpipe, gas flows upwards in the
standpipe and no Helium was detected in the gas exit of the cyclone (Cyc1 in Figure
1). As the pressure drop reduces below a critical value, gas starts flowing
downwards in the standpipe and progressively increases as the pressure drop
reduces further in the standpipe.
The variation of the interstitial velocities in the standpipe is illustrated in Figure 3 for
the same tests series above. In the case of negative pressure drop, the slip velocity
is positive and the gas velocity is higher than the solid velocity. As the pressure drop
in the reactor increases, slip velocity reduces progressively to zero (the solid and the
gas have the same velocity). At higher reactor pressure drops, the slip velocity
becomes negative. In this case, the particles flow faster than the gas. Finally, the
relative velocity increases more than the solid velocity in value, which means the
gas flows upward in the standpipe in the opposite direction of the solids flow.
80 0.03 0.08
Zone I Zone II Vsl
60 0.06 Vs
Vg
40 0.02 0.04
Pv (mbar)
Uv (m/s)
V (m/s)
20 0.02
0 0.01 0.00
-20 -0.02
-40 0.00 -0.04

0 20 40 60 80 100 -40 -20 0 20 40 60
DPR (mbar) DPv (mbar)
Figure 2: The effect of the reactor Figure 3: The change of the interstitial
pressure drop on the pressure drop and velocities in the standpipe due to the
the gas flow in the vertical section of the change of the standpipe pressure drop
L-valve with Ulv = 0.2 m/s. with Ulv = 0.2 m/s and Gs = 35 - 64
kg/m².s (equivalent to variation of Vs).
The variation of the gas flow through the vertical section of the L-valve changes the
total gas flow around the bend of the L-valve. The solid flow rate in the L-valve is
controlled by the gas flow rate through the bend of the L-valve (QH) (3). Therefore,
the solid flow actuated in the L-valve will be affected due to the variation of the gas
flow in the L-valve(UV). This phenomenon is shown in Figure 3 where increase of
Pv from -30 to 33 mbar reduces solid velocity from 0.042 to 0.026 m/s equivalent to
solid flux variation of 64 to 43 kg/m².s.
The internal and the external L-valve air flow rates versus the solid flux in the L-
valve are presented in Figure 4 for two test series. In the first series, the solid flow
rate was controlled by the variation of the external L-valve aeration (Ulv). As
expected, increase in Ulv increases solid flux. Moreover, the gas flow rate in the
standpipe increases as solids entrain more gases downwards in the standpipe. Gas
flow rate in the horizontal section of the L-valve which is sum of Ulv and Uv increases
in the same order.
0.10
HR=cte: UH Ulv UH'
The external L-valve aeration (Ulv'), 0.4
Qlv=cte: Ulv' Uv Uv' 0.08
was kept constant in the second
series of experiments presented in 0.3
0.06
U (m/s)
the Figure 4. The standpipe gas
U (m/s)
0.2
flow rate was then varied by 0.04
adjusting the pressure drop across 0.1 0.02
the standpipe through changes in
the reactor pressure drop. 0.0 0.00
Accordingly, for a constant external 0 50 100 150 200
aeration, horizontal gas flow rate in Gs (kg/m².s)
the L-valve increases as Uv' Figure 4: The variation of the solid flux versus
increases. This demonstrate that the measured gas flow velocity in the L-valve
for a constant external aeration of for two experimental series: the change in
the L-valve, the solid flow rate can external L-valve aeration with the fixed solid
be varied through variation of the height (♦, , ) and the variation of the
Uv imposed by change of pressure pressure drop in the standpipe with fixed
drop across the standpipe. external aeration ( , , ).
Therefore, the solid flow rate
actuated in the L-valve is not only a function of the external aeration but also
pressure drop across the L-valve. Knowlton (3;4;18) has explained this phenomenon
being due to the fact that the solid flow rate in the L-valve is controlled by the
quantity of the gas flowing around the bed of the L-valve (QH). This theory is well
illustrated in the Figure 4 where the QH curve lays on the same line for both of the
experimental series. Standpipe gas flow variation is steeper in case of pressure drop
change compared to the external aeration change for unit change of the solid flux.
This is due to the fact that Qv must compensate required QH variation for a unit
change of solid flux while external aeration is constant.
These results illustrate that a desired solid flow rate in the L-valve can be achieved
by different configurations of the external aeration and the gas flow in the standpipe.
This is of particular interest in case of CLC process where the gas flow out of the
reactor is considered as a leakage and is desired to be minimized. Therefore, a
proper control of pressure drop across the system together with appropriate external
aeration helps to optimize this gas leakage out of the reactor.
VOIDAGE OF THE MOVING SOLID BED

The experimentally measured pressure drop, gas flow rate and solid flow rate values
were used to calculate the average voidage of the moving solid bed ( sp) based on
the Ergun equation. As discussed before, the current installation permits to control
the pressure drop across the standpipe independently from Qlv. Using this feature,
the voidage of the solid bed was measured for two non-fluidized solid flows regimes
(Figure 5). The packed bed solid flow regime was reached when the pressure drop
across the standpipe was negative, corresponding to positive slip velocities (see
Figure 3). This corresponds to Zone II illustrated in Figure 5. The slip velocity is
positive in this regime, as gas downward flow is faster than solids velocity (see
Figure 3). The resulting moving bed voidage in this case is constant and
corresponds roughly to the tapped bed voidage. In other words, gas flow pushes to
pack moving solids tighter together in this regime. Transition packed bed solid flow
attained by imposing positive pressure
60%
drop in the standpipe. Slip velocities was
Zone II
negative in this region (see Figure 3). In Zone I (Vsl <0)
mf (Vsl >0)
this case, reactor pressure drop was 50%
kept constant and solid flow and
(%)
pressure drop variation was adjusted s
through changes of Qlv. Resulting 40%
variation of average voidage is illustrated vmf

in Figure 5, Zone I. Slip velocity is 30%
negative in this region, meaning that -0.15 -0.10 -0.05 0.00 0.05
solid particles have higher velocity than Vsl (m/s)
gas. As slip velocity increases in value, Figure 5: The experimental results of
voidage of solid bed expends from the variation of the average voidage of
tapped bed voidage toward bed voidage moving solid bed in the standpipe of the
at the minimum fluidization condition. L-valve.
The correlations listed in the Table 1 80% Yagi
were then compared with experimental
results in Figure 6. Linear correlation 60%
Li et al.
proposed by Knowlton and Hirsan (3)
(%)
results in closest prediction. Correlation 40% Knowlton
of Li et al. (15) and Chan et al. (16) give

20% Chan et al.
a good estimate of the voidage variation
trend, they however over/under 0%
estimates the voidage values. The 0.00 0.04 0.08 0.12
significant difference observed in some -Vsl (m/s)
cases is mostly due to different operating Figure 6: The experimental results of
conditions in this test and developed variation of the voidage of the moving
correlations. solid bed in the standpipe of the L-valve
compared with the literature
L-VALVE LIMITING OPERATION correlations.
The L-valve operation is reported to be limited due to different limiting conditions
including: fluidization of vertical arm (3), limit of solid flow rate into the L-valve (8), or
unstable operation of the inclined section of the L-valve (19) (in case of hybrid
standpipe as in the current configuration). However, these limits depend on the
pressure drop across the standpipe of the L-valve which is a dependent variable
parameter. Accordingly, the upper operation limit of the L-valve can be adjusted
depending upon the operating conditions.
A test was carried out to investigate continuous operation of the L-valve in the
limiting condition. External gas flow rate was set to a high value of 0.416 m/s. The
resulting pressure drop variation and gas flow in the standpipe is illustrated in Figure
7. An oscillatory behavior of the pressure drop and gas the flow was observed in the
system. Moreover, height of the moving bed in the standpipe was also behaving in
an oscillatory mode. Once the L-valve was opened, solid height started to gradually
decrease while pressure drop was increasing across the standpipe. The solid height
finally got to a minimum level where it started to raise again. The solid height then
increased till it reached the top of the L-valve where the solid height started to
decrease again. This unsteady phenomenon repeated itself in an oscillatory mode
as illustrated in Figure 7. 80 0.08
PR Pv PL
PH Uv
When a very high gas flow rate is
60 0.06
injected into the L-valve, a very
DP (mbar)
high solid flow rate is actuated in
Uv (m/s)
40 0.04
the L-valve exit (W s) higher than
solid flow into the L-valve (W in).
20 0.02
The solid height in the standpipe
(Hs) then reduces, resulting in
increase of the pressure drop per 0 0
0 100 200 300 400 500
unit height of the standpipe t (s)
( P/Hs). Consequently, the
downward gas flow rate in the Figure 7: Oscillatory operation of L-valve in
standpipe (Uv) reduces gradually, limiting condition of Ulv = 0.416 m/s.
get to zero and finally gas flows upwards in the standpipe. Accordingly, UH reduces,
resulting in reduction of solid flow rate actuated in the L-valve. The solid inventory in
the reactor then increases. Consequently, pressure drop in the reactor increases,
resulting in reduction of the total pressure drop in the standpipe. As the solid flow
rate reduces, W in exceeds W out and standpipe starts to fill. As the solid height in the
standpipe increases, P/Hs reduces. Therefore, more gas passes downwards, and
the solid flow rate increases gradually. This continues until solid height gets its
maximum once standpipe is filled with the solid and again W out exceeds Win. Once
more, the same cycle starts to repeat again. At the same time, the second L-valve
(lv2 in Figure 1) was operating normally with an average solid flow rate equal to that
of the first L-valve (lv1) which was operating in an unstable manner. The stable
operation of the second L-valve was due to proper adjustment of the external
aeration and the pressure drop along the standpipe. The external air flow velocity
was set to 0.381 m/s (compared to 0.416 m/s in the lv1) and the pressure drop in
the reactor was slightly higher in the reactor R2 compared to R1. This illustrates
importance of proper selection of the operating conditions in high solid flow rate
operations to avoid possible instable instabilities. This is of particular interest in the
CLC process where a high solid circulation rate is desired between two reactors to
transfer the required oxygen for combustion.
CONCLUSION
The results of experimental study of an L-valve in a chemical looping combustion
cold prototype was presented in this work. Helium was used as gas tracer to
experimentally measure quantity of gas flow in the different sections of the L-valve.
Gas flow rate in the vertical section of the L-valve increased by increasing solid flow
rate or by decreasing pressure drop across the vertical section of the L-valve.
Experimental results were then used to calculate the average voidage of the moving
solid bed in the vertical arm of the L-valve. Voidage variation in two regimes of
packed bed flow and transitional packed bed flow were presented. Finally,
oscillatory operation of L-valve in the limiting condition was presented in terms of
gas and solid flow and pressure drop.
NOTATION
Gs: solid flux, kg/m².s. Vg: interstitial gas flow rate, m/s.
Hs: Height of solid bed in the standpipe, m. Vs: interstitial solid velocity, m/s.
Qlv: The external L-valve aeration, Nm3/h. PR: pressure drop in the reactor,
Ulv: external aeration flow velocity calculated mbar.
based on the L-valve area, m/s. Pv: pressure drop in he vertical arm
UH: gas flow velocity in the horizontal section of the L-valve, mbar.
of the L-valve, m/s. s: voidage of free settled solid bed.
Uv: gas flow velocity in the vertical section of sp: voidage of solid bed in the
the L-valve, m/s. standpipe.
Vsl: gas-solid slip velocity, m/s. st: voidage of tapped solid bed.
REFERENCES
1. Gauthier T., Bayle J., Leroy P. FCC: Fluidization Phenomena and Technologies. Oil
& Gas Science and Technology - Rev IFP 2000;55(2):187.
2. Lyngfelt A., Leckner Bo, Mattisson T. A Fuidized-bed combustion process with
inherent CO2 separation; application of chemical-looping combustion. Chemical
Engineering Science 2001;56:3101.
3. Solids Flow Control using a Nonmechanical L-valve. Ninth Synthetic Pipeline Gas
Symposium; Chicago, illinois. 1997.
4. Knowlton T.M. Feeding and Discharge of Solids Using Nonmechanical Valves.
Institute of Gas Technology . 1988. Chicago, Illionois, Institute of Gas Technology.
5. Yang Wen-Ching, Knowlton Ted M. L-valve equations. Powder Technology
1993;77:49.
6. Chan CW, Seville J, Fan X, Baeyens J. Particle motion in L-valve as observed by
positron emission particle tracking. Powder Technology 2009;193(2):137.
7. Geldart D., Jones P. The behaviour of L-valve with granular solids. Powder
Technology 1991;67:163.
8. Smolders K, Baeyens J. The Operation of L-valve to Control Standpipe Flow.
Advaced Powder technology 1995;6(03):163.
9. Yang TY, Leu LP. Multi-resolution analysis of wavelet transform on pressure
fluctuations in an L-valve. International Journal of Multiphase Flow 2008;34(6):567.
10. Ergun S. Fluid flow through packed columns. Chemical Engineering Process
1952;48(2):89.
11. Smolders K, Baeyens J. The Operation of L-valve to Control Standpipe Flow.
Advaced Powder technology 1995;6(03):163.
12. Kojabashian C. Properties of dense-phase fluidized solids in vertical downflow
Massachusetts Inst. of Technology; 1958.
13. Zhang J.Y., Rudolph V. Transitional Packed Bed Flow in Standpipes. Can J of Chem
Eng , 1991;69:1242.
14. Yagi S. Chemical Machinery, Japon 1952;16:307.
15. Li Y., Lu Y., Wang F., Han K., Mi W., Chen X. et al. Behavior of gas-solid flow in the
downcomer of a circulating fluidized bed with a V-valve. Powder Technology
1997;91:11.
16. Chan C.W., Seville J., Fan X., Baeyens J. Solid particle motion in a standpipe as
observed by Positron Emission Particle Tracking. Powder Technology 2009;194(1-
2):58.
17. Yazdanpanah M.M., Hoteit A., Forret A., Delebarre A., Gauthier T. Experimental
Investigations on a Novel Chemical Looping Combustion Configuration. OGST -
Revue d'IFP Energies nouvelles 2010.
18. Wet and Dry Limestone Feeding Using an L-valve. Sixth International Conference on
Fluidized Bed Combustion; Atlanta, Georgia. 1980.
19. Knowlton T.M. Standpipes and Nonmechanical Valves. In: Yang W-C, editor.
Handbook of Fluidization and Fluid-Particle Systems. NEW YORK: MARCEL
DEKKER, INC; 2003. p. 576.
3D CFD SIMULATION OF COMBUSTION
IN A 150 MWe CIRCULATING FLUIDIZED BED BOILER
Nan Zhang, Bona Lu, Wei Wang, Jinghai Li

State Key Laboratory of Multiphase Complex Systems, Institute of Process
Engineering, Chinese Academy of Sciences, Beijing 100190, China
ABSTRACT
Eulerian granular multiphase model with meso-scale modeling of drag coefficient and
mass transfer coefficient, based on the energy minimization multi-scale (EMMS)
model, was presented to simulate a 150 MWe CFB boiler. The three-dimensional
(3D), full-loop, time-dependent simulation results were presented in terms of the
profiles of pressure, solids volume fraction and solids vertical velocity, the
distributions of carbon and oxygen, as well as the temperature. The EMMS-based
sub-grid modeling allows using coarse grid with proven accuracy, and hence it is
suitable for simulation of such large-scale industrial reactors.
INTRODUCTION
The gas-solid flow, heat /mass transfer and chemical reactions in Circulating
Fluidized Bed (CFB) reactors are inherently coupled with spatio-temporal multi-scale
structures, and featured with non-linear non-equilibrium behavior (1). For such a
multi-phase complex system, it is inadequate to reproduce the real physical process
by refining the grid in the conventional Two-Fluid Model (TFM), thus calling for
establishing meso-scale models (2).
The present study firstly presents a 3D full-loop simulation for a 150 MWe CFB boiler,
showing the powerful capability of the sub-grid EMMS model in predicting the
hydrodynamics in a CFB. Then, a reduced EMMS/mass model is incorporated into
the mass conservation equations for combustion species, and a 3D combustion
simulation is realized for the furnace part.
MODEL DESCRIPTION AND SIMULATION SETTING
Governing equations
The Eulerian granular model in Fluent®6.3.26 was used to study the flow behavior in
the full-loop of the boiler, in which the stress of the solid phase was described with
the kinetic theory of granular flow; the drag coefficient correlation was corrected with
consideration of particle clusters, which was detailed in (3) and would not be stressed
here. By neglecting of energy due to viscous dissipation, compression or expansion
and interfacial flow, the internal energy balances and the conservation equations of
chemical species in gas and solid phase were used to study the combustion in the
furnace. As a first step to combustion simulation, only the main reaction of carbon
react with oxygen to carbon dioxide was considered here. The volatile combustion
and moisture release was considered in the heat balance through a UDF which filled
the gap between the low heating value of the coal and the reaction heat as carbon
was combusted completely, and the value was added averagely on the solids phase
in the lower section (h <= 6m) of the furnace. The volatile and moisture was
neglected in the mass balance equation, as they are less than 2% compared with the
total air input, detailed in (4).
Geometry and mesh
The 150 MWe CFB boiler was designed by Harbin Boiler Co. Ltd. and installed in
Guangdong, China. The main cross section of the furnace is a rectangle of 15.32 ×
7.22 m2; the chamber height is 36.5 m; detailed information can be found in (3).
The geometry and surface mesh of the whole loop of the solids material was shown
in Fig. 1. As can be seen from the figure, most of the boiler was meshed with
hexahedron, others meshed with polyhedron, all with size scale of 0.1 m. For
convenience, the primary air and the loop-seal aeration were assumed in plug flow
from their bottoms. To balance the solid inventory in the boiler, the solids exiting from
the cyclone outlets, which was about 6%(mass fraction) of the circulating solids
during the simulation, were returned via the coal-feed inlets. The origin point is set at
the center of the primary inlet at the bottom of the furnace; the x-axis is along the
front-to-back wall direction (width direction); the y-axis is along the side-to-side wall
direction (depth direction), and the z-axis is against the gravity direction.
Simulation settings
For full-loop hydrodynamic simulation, the boiler was considered operated at the
design temperature of 917℃ and atmospheric pressure, thus the physical properties
of the gas was considered as a const, while for combustion simulation in the furnace,
the mixing laws of the gas mixture were summarized in Table 1. The boundary and
initial conditions of the hydrodynamic simulation and the combustion simulation are
listed in Table 2 and Table 3 separately.
Fig. 1. Geometry and surface mesh of the whole loop of the 150 MWe CFB boiler.
Table 1. Mixing laws of the gas mixture

Property Unit Mixing law Equation
Density (kg/m )3 Incompressible ideal gas ρ = pop RT ∑ (Yi MWi )
law i
Specific Heat (J/kg·k) Mixing law c p = ∑ Yi c p ,i

Capacity i
Thermal (w/m·k) mass weighted mixing law k = ∑ Yi ki

Conductivity i
Viscosity (kg/m·s) mass weighted mixing law μ = ∑ Yi μi

i
Mass Diffusion (m2/s) Dilute Approximation

Di ,m
Table 2. Boundary and initial conditions of hydrodynamic simulation in full-loop of the boiler
Boundary and Initial Gas Phase Solid Phase
Conditions Flow rate Area Velocity
2
(kg/s) (m ) (m/s)
Primary air inlet 94.16 50.88 6.32 0
Secondary air Inlet 53.21 0.92 198.01 0
Slag-cooler inlet 8.00 0.75 36.32 0
Loop-seal inlet 2.32 8.02 0.99 0
Coal-feed inlet 12.48 1.16 36.70 UDF
Initial solid packing height 2.5 m
Cyclone Outlet 101325 Pa
Wall No-slip Partial slip
Table 3. Boundary and initial conditions of combustion simulation in the furnace

Boundary and Initial Gas Phase Solid Phase
Conditions Temperature Velocity Temperature Velocity
(K) (m/s) (K) (m/s)
Primary air inlet 500.15 2.662 1190 0
Secondary air Inlet 500.15 83.397 1190 0
Slag-cooler inlet 293.15 9.018 1190 0
Loop-seal inlet 293.15 0.245 1190 0
Coal feed inlet 293.15 15.458 1190 0.013+returned
Initial solid packing height 1.5 m
Cyclone Outlet 101325 Pa
Wall No-slip Partial slip
HYDRODYNAMIC FLOW IN THE FULL-LOOP
Fig. 2(a) shows the simulated pressure balance in the boiler: pressure gradient is
large at the bottom and comparatively small at the top in the furnace, while the
largest gradient occurs at the return legs. Fig. 2(b) shows that the general trends of
the simulated data were comparable with experimental data. Fig. 3 and Fig. 4 show
profiles of solids volume fraction and solids vertical velocity at different heights,
respectively. Fig. 3(a) shows the so-called core-annulus structure, i.e. a denser
solids concentration near the wall than in the center. Fig. 3(b) shows that solids
concentration profiles along the depth direction are flatter than those along the width
direction. Fig. 4(a) shows falling clusters near the walls while rising particles in the
center. Fig. 4(b) shows two maximum rising velocities not far from the walls, which
may be affected by the secondary air inlets at the side walls.
(a) (b)
Fig. 2. Pressure distribution: (a): in the whole loop (b): compared with experimental
data in the furnace (simulation data were taken from the center line of the furnace).
Fig. 3. Solids volume fraction at different heights in the boiler.
Fig. 4. Solids vertical velocity at different heights in the boiler.
COMBUSTION IN THE FURNACE PART
Fig. 5 shows the simulated temperature in the furnace, which is low at the bottom
because of the injected cold air and is high at the top because of combustion energy
released. Fig. 6 and Fig. 7 show snapshots of simulated carbon concentration and
oxygen concentration with several slices in different directions, respectively. Fig. 6(a)
and Fig. 6 (b) Show that carbon concentration is large at the bottom and small at the
top, Fig. 6(b) and Fig. 6 (c) show that carbon concentration reaches local maximum
near the solids return ports and causes non-uniform in the bottom of the furnace, and
this local non-uniform caused by local ports will decrease along the height because
of combustion and dispersion. Fig. 7(a) shows that oxygen concentration is large at
the bottom and is small at the top because of combustion. Fig. 7(b) shows that the
injected secondary air causes local maximum of oxygen concentration, while the
maximum oxygen is not at the center line of the furnace but there are two maximum
near the center line, which is caused by the fact that the injection does not reach the
center of the furnace, this phenomenon was also reported by Myöhänen et al. (5). Fig.
7(c) shows that the injected secondary air leads to non-uniform oxygen concentration
at the bottom and this non-uniformity decreases along the height but still exists at the
top of the furnace.
Fig. 5. Temperature profile in the furnace.
(a) (b) (c)
Fig. 6. Simulated carbon concentration distributions with vertical slices (a): side-to-side
slice ，(b): front-to-back slices and (c): horizontal slices.
(a) (b) (c)
Fig. 7. Simulated oxygen concentration distributions with vertical slices (a): side-to-side
slice ，(b): front-to-back slices and (c): horizontal slices.
CONCLUSIONS
Simulation results show the capability of the current model, with emphasis on the
EMMS-corrected drag coefficient, in predicting the two-phase flow behavior. The
reduced multi-scale mass transfer model and the drag coefficient correction based
on the EMMS model were coupled to realize combustion simulation in the furnace. It
is an extension to our experience on virtual experimentation to investigate the
combustion within an industrial reactor.
ACKNOWLEDGMENT
The authors are grateful to Professor Junfu Lu of Tsinghua University for providing
the blueprint of the boiler. The financial supports from NSFC under Grant No.
20821092, MOST under Nos. 2007AA050302-03 and 2008BAF33B01, and CAS
under No. KGCX2-YW-222 are also gratefully acknowledged.
NOTATION
cp specific heat capacity, J/kg·k

D mass diffusion coefficient, m2/s
k thermal conductivity, w/m·k
p pressure, Pa
R gas constant, 8.314 J / mol·K
MW molecular weight, kg/mol
T temperature, K or ℃
V velocity, m/s
x coordinate, m
y coordinate, m
Y mass fraction, dimensionless
z coordinate, m
Greek letters
ε volume fraction, dimensionless
μ viscosity, kg/(m·s)
ρ density, kg/m3
Subscripts
s solid phase
i species
REFERENCES
1. J. Li, M. Kwauk, Particle-fluid two-phase flow: The energy-minimization multi-scale method.

Beijing: Metallurgical Industry Press, 1994.
2. B. Lu, W. Wang, J. Li, Searching for a mesh-independent sub-grid model for CFD
simulation of gas-solid riser flows. Chemical Engineering Science 2009, 64 (15),
3437-3447.
3. N. Zhang, B. Lu, W. Wang, J. Li, 3D CFD simulation of hydrodynamics of a 150 MWe
circulating fluidized bed boiler. Chemical Engineering Journal 2010, 162 (2), 821-828.
4. N. Zhang, B. Lu, W. Wang, J. Li, 3D CFD simulation of combustion in a 150 MWe circulating
fluidized bed boiler. To be submitted.
5. K. Myöhänen, T. Hyppänen, M. Loschkin, Converting Measurement Data to Process
Knowledge by Using Three-Dimensional CFB Furnace Model, in: K. Cen (Eds.),
Circulating Fluidized Bed Technology VIII - Proceedings of the Eighth International
Conference on Circulating Fluidized Beds, International Academic Publishers, World
Publishing Corp., Hangzhou, 2005, pp. 306-312.
HYDRODYNAMICS OF A LOOP-SEAL OPERATED IN A
CIRCULATING FLUIDIZED BED: INFLUENCE OF THE
OPERATING CONDITIONS ON GAS AND SOLID FLOW
PATTERNS
Roberto Solimene1, Riccardo Chirone1, Piero Bareschino3, Piero Salatino2
1
Istituto di Ricerche sulla Combustione – CNR
2
Dipartimento di Ingegneria Chimica - Università degli studi di Napoli Federico II
Piazzale Tecchio, 80 80125 Napoli Italy
3
Dipartimento di Ingegneria – Università degli Studi del Sannio
Piazza Roma, 21 82100 Benevento Italy
T: +390817682237; F: +390815936936; E: solimene@irc.cnr.it
ABSTRACT
Hydrodynamic features of a loop-seal operated as solids re-injection device in a lab-

scale cold CFB apparatus are studied. Gas flow patterns are characterized by
means of gas tracing experiments with continuous injection of CO2 in the loop-seal
chambers. Solids flow patterns are characterized by impulsive injection of dye-
coloured particles into the supply chamber, followed by particle tracking.
INTRODUCTION
The dual fluidized bed technology has recently risen to renewed interest for process
applications whenever distinct reactive environments (e.g. oxidative/reducing,
temperature and/or pressure looping) need to be established while sharing a solid
stream which acts as reactant or thermal carrier. Exploitation of the dual fluidized
bed concept is currently being explored in fields like: i) CO2 capture in coal-fired
generating stations and cement kilns (1)); ii) chemical-looping combustion (2-3); iii)
biomass pyrolysis and gasification (4). The dual loop system presents, however,
some criticalities that are mostly related to the effective control of solids recirculation
between the beds and to the establishment of leak-tight operation of the beds with
respect to the gaseous streams. These criticalities involve both design and
operational variables of the plant which determine the hydrodynamic behaviour of
different plant components (5-6). Several types of non-mechanical valves (L-valve,
J-valve, seal pot and loop-seal) are commonly used in CFBs and DIFBs to control
the mass flow rate of solids or to seal gaseous streams. Despite empirical or semi-
empirical criteria for correct loop-seal design have been laid (7-15), thorough
characterization of loop-seal hydrodynamics, especially under large solid throughput
conditions, is still lacking. In the present study the hydrodynamics of a loop-seal is
investigated. The seal is operated as solids re-injection device between a 40 mm ID
downcomer and a 102 mm ID riser in a lab-scale cold CFB apparatus. The
experimental procedure includes time-resolved measurements of gas pressure at
several locations along the CFB loop and in the loop-seal and of solids mass flux
along the riser. The gas flow patterns are characterized according to tracing
methods based on continuous CO2 injection at the bottom of the loop-seal
chambers. Solids flow patterns are characterized by impulsive injection of dye-
coloured particles into the supply chamber, followed by particle tracking by means of
a video camera interfaced to a computer. The characterization of the gas and solids
flow patterns is carried out under a broad range of operating conditions
by varying: i) the gas superficial velocity in the riser; ii) the fluidization
velocity in the loop seal; iii) the throughput of circulating bed solids in
the loop seal. Results are presented and discussed with an emphasis
on the establishment of gas cross-flow between the loop seal chambers
and its relevance to effective solids recirculation and gas “leakage”.
EXPERIMENTAL
Apparatus
The lab-scale cold model CFB (Figure 1) consisted of a riser, a
cyclone, a solids reservoir, a standpipe and a loop seal. The Plexiglas
riser, 0.102 m ID and 5.6 m high, was equipped with a gas distributor
consisting of several stainless steel nets layered one on the other up to
2 mm thickness, characterized by low-pressure drop. An high-efficiency
cyclone, 0.09 m and 0.32 m high, was installed at riser outlet. The
solids return line consisted of the solids reservoir, 180 mm ID 0.40 m
high, a 40 mm standpipe and a loop seal. The supply and recycle
chambers of the loop seal have a square cross section (50mm side),
height of 300 and 250 mm, respectively, and separate wind-boxes. The
gap at the bottom of the two chambers is about 50 mm. The CFB loop
was equipped with 21 pressure taps at different locations. The overall
solids mass flux was determined by closing for a pre-set time a butterfly
valve located along the standpipe and measuring the solids mass
accumulated upstream the valve.
Diagnostics
High-precision piezo-resistive gas pressure transducers have been
adopted to measure the gas pressure along the CFB loop. An on-line
gas sampling carried out by means of a probe connected to a CO2 gas
analyzer (ABB advance optima Uras 14) was optimized to investigate
the gas flow in the loop seal. All signals coming from the instruments
were logged on a data acquisition unit consisting of a PC equipped with
a data acquisition board. A high-speed, highly light-sensitive mega-
pixel CMOS camera interfaced to a computer and controlled with an
image processing software has been adopted for particle tracking in the
loop seal chambers.
Materials and Operating Conditions

Table 1 reports the properties of quartz adopted for the tests. Fluidizing
gas was technical air at room temperature. Gaseous CO2 from
cylinders and black glass (500 μm) beads were used as gas and solids
tracer, respectively. Solids inventory was 3.5 kg. Gas superficial
velocity in the riser Ug,r ranged between 2.1 and 4.4 m/s. The minimum
value of Ug,r was always larger than the terminal velocity (Ut) of the
granular solid. Air was injected at the bottom of the loop-seal so that
gas superficial velocity in loop-seal chambers (Ug,ls) results to be 1, 1.5 Fig. 1:
and 2 times Umf. Solids mass circulation fluxes in the riser Gs ranged Experimental
apparatus.
between 2 and 11 kg/(s m2). Voidage (ε) Table 1 - Properties of the granular solids
along the riser was calculated by Material Quartz
Sauter mean diameter (dp), μm 253
processing the pressure drops, ΔP,
Size range, μm 100-400
measured at successive pressure taps
Particle density (ρs), kg/m3 2300
located at distance Δz according to the Incipient fluidization velocity (Umf)(1), m/s 0.047
relationship ΔP=ρsg(1-ε)Δz, where g is the Terminal velocity (Ut)(1), m/s 1.77
acceleration due to gravity. (1)
calculated
Procedure
Bed Hydrodynamics: Steady state operation of the CFB loop has been investigated
at a pre-set fluidization velocity in the riser and in the loop seal. The steady state
condition has been recognized by continuous monitoring of the gas pressure along
the loop and by step-wise measurement of the mass flow rate. Once the steady
state condition was reached, the gas pressure signal was acquired for about 5
minutes. The experiments have been characterized in terms of fluidization velocity
both in the riser and in the loop seal.
Gas and Solids Tracing in the Loop Seal: Some experiments have been carried out
to investigate the gas and solids flow patterns in the loop seal at Ug,r= 2.85m/s.
Once the steady state operation of the CFB loop was reached at a pre-set Ug,ls, a
batch of solids tracer (50g) was injected along the standpipe. The tracing particles
fell down in the loop seal and their motion has been recorded by the video camera
at 125 fps for 30s. The experiments has been repeated for three times and they
have characterized in terms of Ug,ls. An ad-hoc procedure of image analysis has
been developed to follow the trajectories of the tracing particles. In the same
operating conditions, gas tracing has been carried out by continuous feeding of a
gas fluidizing stream with a pre-set CO2 concentration (in the range of 10-20%v) in
the supply and in the recycle chamber, alternatively. The CO2 concentration has
been measured at the bottom and the top of beds of the loop seal. The obtained
data have been analyzed to achieve the gas flow distribution in the loop seal.
Hydrodynamics of the Riser and of the Loop Seal: Figure 2 reports relative
pressures measured at different pressure taps located around the CFB loop during
runs operated at Ug,r=2.85m/s. The gas superficial velocity in the loop seal Ug,ls was
varied in the range Umf≤Ug,ls≤2Umf. Analysis of the pressure loop indicates that the
pressure gradient at the bottom of the riser (i.e. at levels above the distributor up to
0.1m) increases as Ug,ls is increased. The pressure gradient in the recycle chamber
of the loop seal remains constant at a value consistent with the bulk density of the
bed material under bubbling fluidization conditions at any Ug,ls. The pressure
gradient in the supply chamber increases from a minimum at Ug,ls=Umf to approach
values corresponding to the bulk density of a fully fluidized bubbling bed as Ug,ls is
increased. Figure 3 reports the solids mass flux in the riser as well as the pressure
drop and the height of the bed of solids, respectively, in the recycle and in the
supply chamber of the loop-seal. Data points correspond to the three experimental
conditions reported in Figure 2. As Ug,ls is increased the following features can be
recognized: i) the solid mass flux remains substantially constant; ii) the pressure
drop in the recycle chamber slightly decreases; ii) the pressure drop in the supply
chamber undergoes a pronounced increase whereas the bed height decreases as
Ug,ls increases from Umf to 1.5Umf, both
600
remaining nearly constant at values larger
Ug,ls=Umf; GS=4.75 kg/(s m2)
than Umf. Altogether, the fluidization 2
Ug,ls=2Umf; GS=4.15 kg/(s m )
velocity in the loop seal exerts a moderate Ug,ls=1.5Umf; GS=3.47 kg/(s m2)
influence on riser hydrodynamics,
whereas loop seal hydrodynamics is 500
affected to a larger extent. As Ug,ls was

increased from Umf to 1.5Umf, the bed
material present in the supply chamber
becomes fully fluidized, consistently with 400
the change of pressure drop and gradient

reported in Figures 2 and 3.
Height, cm
When the supply chamber is fluidized, a 300
fraction of the solids present in this
chamber is transferred to the riser, and
the loading of solids at the bottom of the
200
10
A Ug,r = 2.85 m/s
8
GS, kg/(s m2)
6
100
0
0 0 10 20 30 40 50 60
30 Pressure, mbar
28
B
Fig. 2: Pressure loop for different Ug,ls/Umf
26 ratio;Ug,r = 2.85 m/s.
24 riser is increased. This feature is reflected
ΔPls, mbar
22 by the change of bed height in the supply

20 chamber and of the pressure gradient at the
18 bottom of the riser. Figure 4 reports the
16
Recycle chamber
Supply chamber
solids mass flux in the riser and the bulk
14 density (ρ) of the bed at the bottom of the
55 riser as a function of the fluidization velocity
50
C Recycle chamber (Ug,r) for different values of the ratio Ug,ls/Umf
Supply chamber
45
in the loop seal. The following features can
be recognized: i) Gs increases almost
40
linearly with Ug,r; ii) Gs is barely influenced
H, cm
35 by Ug,ls/Umf, except for Ug,ls=Umf and for high

30 values of Ug,r; iii) ρ is also barely influenced
25
by Ug,ls/Umf except for Ug,ls=Umf, when the
values of ρ recorded are smaller regardless
20
0.8 1.0 1.2 1.4 1.6 1.8 2.0 2.2 of Ug,r; iv) ρ remains substantially constant
U /U
g,ls mf at a value of about 140kg/m3 for Ug,r>3m/s,
Fig. 3: Solids mass flux (A) pressure drops (B) it increases as the fluidization velocity in the
and bed height (C) in the loop-seal chambers riser is decreased at Ug,r<3m/s; v) for values
as a function of Ug,ls/Umf ratio. Ug,r=2.85m/s.
of Ug,r<3m/s, as the terminal velocity of
bed particles is approached, a dense 12
Ug,ls/Umf = 1.0
bed is established at the bottom of the Ug,ls/Umf = 1.5 A
10
riser with values of ρ in the order of Ug,ls/Umf = 2.0
800-1000kg/m3. It can concluded that 8
GS, kg/(s m2)

loop seal operation in the CFB loop
6
becomes fully effective when the
supply chamber, and not only the 4
recycle chamber, becomes fully
fluidized. This condition requires the 2
gas superficial velocity in the loop seal 0

to exceed Umf. 1200
g,ls mf U /U = 1.0
Analysis of Solids Flow Patterns in
1000 B Ug,ls/Umf = 1.5
Ug,ls/Umf = 2.0
the Loop Seal: Loop seal 800
hydrodynamics has been also 3
ρ, kg/m
investigated by inspection of the gas 600
and solids flow patterns in the loop 400

seal chambers as Ug,ls has been
changed. Figure 5 shows the trajectory 200
and the time-resolved components (VX,
0
VY) of the instantaneous velocity of 1.5 2.0 2.5 3.0 3.5 4.0 4.5
three tracer particles. Trajectories were Ug, m/s
reconstructed by frame-by-frame
analysis of videorecordings taken Fig. 4: Solids mass flux (A) and bottom bulk density
(B) as a function of Ug,r for different Ug,ls/Umf ratio.
during system operation at Ug,ls equal
to Umf and 1.5Umf, with a riser gas superficial velocity set at Ug,r=2.85m/s. Images
acquired for Ug,ls=2Umf could not be analyzed as the stochastic motion of the
particles typical of a bubbling fluidized bed prevented to follow a single particle along
the test. Trajectories are mapped in Figure 5 assuming as origin of the reference
axes the bottom-left corner of the supply chamber, taking x positive along the
direction pointing toward the riser and y positive along the direction opposed to
gravity. The tracer particles were selected as they were at the top of the supply
chamber: one at the center and the other two near the external wall and the
separation wall (vertical solid line) with the recycle chamber, respectively. The tracer
particles were then followed frame by frame during their motion toward and beyond
the gap between the loop seal chambers. At Ug,ls=Umf, the following features can be
recognized: i) the streamlines followed by the tracer particles in the supply chamber
converge toward the top of the gap between the chambers; ii) a significant part of
the supply chamber bottom appears stagnant (below the dashed line); iii) a limited
part of the gap between the two loop seal chambers is characterized by flow of bed
solids; iv) the velocity component along the x axis (VX) is substantially similar for all
the tracer particles and constant with time (about 1.5 mm/s), but it increases
significantly as they approach the gap between the two chambers; v) the velocity
component along the y axis (VY) is similar for all the tracer particles and decreases
as they approach the gap between the two chambers; vi) the tracer particle initially
close to the supply chamber axis presents the largest value of VY; vii) VY is negative
and positive in the supply and recycle chamber, respectively. Increasing Ug,ls
(Ug,ls=1.5Umf), it can be recognized that: i) convergence of the trajectories followed
by the tracer particles in the supply chamber takes place at a later stage close to the
upper part of the gap Ug,ls=1Umf Ug,ls=1.5Umf
between the two 900 left
900
left
chambers; ii) the stagnant 800 center
right
center
800 right
region at supply chamber
bottom is less extended 700 700
than that observed at
Ug,ls=Umf; iii) the fractional 600 600
area of the gap between

the two chambers where 500 500
Y, a.u.
Y, a.u.
solids flow takes place to
a significant extent, is 400 400
expanded; iv) VX is initially

negligible for all the 300 300
tracing particles except

200 200
when they approach the
gap; v) VY is similar for all 100 100
the tracer particles and
constant with time (about 0 0
12.5 mm/s) in the supply 0 100 200 300 400 500 600 700 800
X, a.u.
0 100 200 300 400 500 600 700 800
X, a.u.
chamber; it becomes
80 140
left V 120 left V X

X
positive and increases 60 center V

right V
X 100
80
center V
right V
X
with time in the recycle

X X
VX, mm/s
VX, mm/s
40 60
chamber; vi) the tracer 20

40
20
particle initially located 0
close to the external wall 0 -20
-40
impinges the stagnant -20

30
-60
200
region and stops there. In 20

left V Y
150
left V Y
center V center V
the range Umf<Ug,ls<1.5Umf 10 right V Y
Y
100 right V Y
Y
the bed solids motion in

VY, mm/s
VY, mm/s
0 50
the supply chamber can -10 0
be accurately described -20 -50
by streamlines being the -30 -100
random effect due to -40

0 2 4 6
-150
0 1 2 3 4 5 6
bubble motion negligible, time, s time, s

Fig. 5: Loop seal solids flow patterns: trajectory and time-resolved
whereas at Ug,ls=2Umf, the instantaneous velocity of three tracing particles as a function of Ug,ls.
stagnant region
disappears and bubbling fluidization conditions established throughout the bed.
Analysis of gas flow patterns in the loop seal from gas tracing experiments:
Figure 6 shows a schematic sketch of the gas flow pattern in the loop seal during
gas tracing experiments. Two separate gas streams of equal flow rates are fed to
the bottom of the supply (QSCin) and recycle (QRCin) chambers of the loop seal,
characterized by different CO2 concentrations xSCin and xRCin, respectively.
Experiments have been carried out at a pre-set inlet concentration both in the supply
and recycle chamber and in the same operating conditions of bed solids tracing
(Ug,r=2.85m/s, Ug,ls=Umf, 1.5Umf, 2Umf). The gas cross-flow between the two
chambers has been represented by two streams: one (QRCbypass) directed from the
recycle chamber toward the supply chamber, the other (QSCbypass) in the opposite
direction. It has been assumed that the by-pass stream CO2 concentration is that of
the inlet gas flow rate at the corresponding chamber. From the known values of
QSCin, QRCin, xSCin, xRCin and the measured values of the CO2 out out
QSC, xSC
concentration (xSCout, xRCout) at the outlet, it is possible to
calculate all the other gas flow rates (QRCbypass, QSCbypass, QSCout
and QRCout) on the basis of global material balance and on a
balance on CO2. Figure 7 shows xSCin, xRCin, xSCout and xRCout as
a function of Ug,ls during gas tracing experiments in both loop
seal chambers. It can be recognized that: i) xSCout is nearby to out
QRC, xRC
out
xSCin both when a pre-set CO2 concentration is fed to the supply

chamber (supply chamber gas tracing) and when only air is
used as fluidizing gas (recycle chamber gas tracing); ii) xRCout P17 P20
shows departures from xRCin: it is smaller than the inlet pre-set
CO2 concentration when gas tracing occurs in the recycle
chamber and it is larger than air CO2 concentration when gas bypass
QRC
tracer is fed to the supply chamber. On the basis of the data
reported and on the material balances, the calculated QRCbypass P18
QSC
bypass
P19
is negligible (in order of 0.01m3/h), whereas QSCbypass does not

significantly depend on Ug,ls and it is about 0.2m3/h. Taking into
account that the minimum fluidization gas flow rate is about
0.45m3/h for a single chamber, QSCbypass represents a significant
fraction of the effective gas superficial velocity in the supply
chamber. The fluidization condition in the supply chamber can
be approximately based on the following simplified relationship: in
QSC, xSC
in in
QRC, xRC
in
Gs Ar ε mf Fig. 6: Schematic
U geff,ls ≥ U mf − (1) sketch of the gas flow
Als ρ s (1 − ε mf ) pattern in the loop seal.
where Ug,lseff, ρs, εmf, Ar, Als are the effective gas superficial velocity, bed solids
density, bed voidage at incipient fluidization, cross sections of the riser and of the
supply chambers, respectively. Equation (1) expresses the net gas superficial
velocity established in the emulsion phase of the bed in the supply chamber when
the downflow of bed solids is taken into account. This value could be negative for
low values of Umf or large values of Gs. It is worth noting that a negative value of
Ug,lseff is not per se undesirable from the standpoint of an effective recirculation of
solids, but it is extremely important when “leakage” of gas from the supply chamber
to the recycle chamber must be
0.25
inlet CO concentration 2
required by process constraint.
air CO concentration 2 This is the case, for instance,
out
supply chamber gas tracing: x
0.20
supply chamber gas tracing: x
when the loop seal is part of a
RC
SC
out
CO2 molar fraction, -
recycle chamber gas tracing: x dual interconnected fluidized

RC
out
bed-system with distinct reactive

out
recycle chamber gas tracing : x SC
0.15
environments. The relationship
0.10
(1) is satisfied in all the
experimental conditions tested,
except for those carried out at
0.05
Ug,ls=Umf. Under this condition,
the supply chamber of the loop
0.00 seal is largely unfluidized,
1.0 1.2 1.4 1.6 1.8 2.0
consistently with the pressure
U/Umf
drop data and with the analysis of
Fig. 7: Inlet and outlet CO2 concentrations in the loop seal bed solids tracing.
chambers as a function of Ug,ls during gas tracing
experiments.
CONCLUSIONS
The hydrodynamics of a loop-seal operated as solids re-injection device in a lab-

scale cold CFB apparatus was characterized by a combination of methods, including
solids and gas tracing. For a given riser gas superficial velocity, the loop seal
fluidization velocity exerts a limited influence on riser hydrodynamics, but
significantly modifies the gas and solids flow patterns in the loop-seal. As the loop
seal is kept at gas superficial velocities just beyond incipient fluidization, the supply
chamber is only partly fluidized and an extended stagnant zone is observed at its
bottom. As fluidization becomes more vigorous, stagnant zone extension is reduced
and more solids are transferred to the riser. Analysis of solids and gas tracing tests
highlights the role of solids downflow in the supply chamber and of gas cross-flow
from the supply to the recycle chamber on the fluidization patterns. An approximate
criterion is given for the onset of gas “leakage” between the two loop seal sections,
relevant to loop seal applications in dual interconnected fluidized beds.
NOTATION
Alp
2
loop seal cross section [m ] VX horizontal velocity of tracing particle [m/s]
Ar
2
riser cross section [m ] VY vertical velocity of tracing particle [m/s]
in
xRC recycle chamber inlet CO2 molar fraction
dp particle size [μm]
2 [gmol/gmol]
g acceleration due to gravity [m/s ] out
2 xRC recycle chamber outlet CO2 molar fraction
Gs solids mass flux [kg/m s]
[gmol/gmol]
P gas pressure [Pa] in
bypass 3 xSC supply chamber inlet CO2 molar fraction
QRC recycle chamber by-pass flow rate [m /s]
in 3 [gmol/gmol]
QRC recycle chamber inlet flow rate [m /s] out
out 3 xSC supply chamber outlet CO2 molar fraction
QRC recycle chamber outlet flow rate [m /s]
bypass 3 [gmol/gmol]
QSC supply chamber by-pass flow rate [m /s]
in 3 X horizontal coordinate of tracing particle
QSC supply chamber inlet flow rate [m /s]
out 3 [a.u.]
QSC supply chamber outlet flow rate [m /s]
Y vertical coordinate of tracing particle, [a.u.]
Ug,ls loop seal gas superficial velocity [m/s]
eff z riser axial coordinate [m]
Ug,ls effective loop seal gas superficial velocity
[m/s] ε gas voidage [-]
Ug,r riser gas superficial velocity [m/s] εmf minimum fluidization gas voidage [-]
3
Umf minimum fluidization velocity [m/s] ρ bulk density at riser bottom [kg/m ]
3
Ut particle terminal velocity [m/s] ρs particle density [kg/m ]
REFERENCES
1. Hughes, R. W., Lu, D. Y., Anthony, E. J., Macchi, A. (2005) Fuel Process. Technol.,
86, 1523.
2. Kronberger, B., Lyngfelt, A., Löffler, G., Hofbauer, H. (2005) Ind. Eng. Chem. Res., 44,
546.
3. Hossain, M. M., de Lasa, H. I. (2008). Chem. Eng. Sci., 63, 4433.
4. Pfeifer, C., Proll, T., Punchner, B., Hofbauer, H. (2007) Fluidisation XII (Bi, X., Berruti,
F., Pugsley, T., (Eds.)), Engineering Foundation New York, pp. 889.
5. Kaiser, S., Löffler, G., Bosch, K., Hofbauer, H. (2003). Chem. Eng. Sci., 58, 4215.
6. Bai, D., Issangya, A. S., Zhu, J.-X., Grace, J. R. (1997) Ind. Eng. Chem. Res., 36,
3898.
7. Cheng, L., Basu, P., Cen, K. (1998). Trans. Inst. Chem. Eng., 76, 761.
8. Cheng, L., Basu, P., (2000). Powder Tech., 103, 203.
9. Basu, P., Cheng, L., (2000). Trans. Inst. Chem. Eng., 78, 991.
10. Botsio, E., Basu, P. (2005) Can. J. Chem. Eng., 83, 554.
11. Kim, S. W., Namkung, W., Kim, S. D. (1999). Korean J. Chem. Eng., 16(1), 82.
12. Kim, S. W., Namkung, W., Kim, S. D. (1999). Chem. Eng. Technol., 24, 843.
13. Kim, S. W., Kim, S. D., Lee, D. H. (2002). Ind. Eng. Chem. Res., 41, 4949.
14. Kim, S. W., Kim, S. D. (2002). Powder Tech., 124, 76.
15. Basu, P., Buttler, J. (2009). Applied Energy, 86, 1723.
SULPHUR UPTAKE BY LIMESTONE-BASED SORBENT
PARTICLES IN CFBC: THE INFLUENCE OF
ATTRITION/FRAGMENTATION ON SORBENT INVENTORY
AND PARTICLE SIZE DISTRIBUTION
Fabio Montagnaro#, Piero Salatino*, Fabrizio Scala§, Massimo Urciuolo§
#
Dipartimento di Chimica, Università degli Studi di Napoli Federico II,
Complesso Universitario del Monte di Sant’Angelo, 80126 Naples (Italy)
*
Dipartimento di Ingegneria Chimica, Università degli Studi di Napoli Federico II,
§
Istituto di Ricerche sulla Combustione, Consiglio Nazionale delle Ricerche,
Piazzale Vincenzo Tecchio 80, 80125 Naples (Italy)
ABSTRACT
This paper presents a population balance model aiming at the prediction of sorbent
inventory and particle size distribution establishing at steady state in the bed of an
air-blown CFBC fuelled with a sulphur-bearing solid fuel. The core of the model is
represented by population balance equations on sorbent particles which embody
terms expressing the extent/rate of sorbent attrition/fragmentation. The effect of the
progress of sulphation on attrition and fragmentation is taken into account by
selection of appropriate constitutive equations. Model results are presented and
discussed with the aim of clarifying the influence of particle attrition/fragmentation on
sorbent inventory and particle size distribution, partitioning of sorbent between fly
and bottom ash, sulphur capture efficiency. A sensitivity analysis is carried out with
reference to relevant operational parameters of the combustor.
INTRODUCTION
Substantial changes in the particle size distribution of limestone-based SO2 sorbents

can be brought about by particle attrition/fragmentation in fluidized bed combustors.
The mutual interference between chemical reactions (calcination and dehydration,
sulphation) and attrition/fragmentation of limestone has been largely disclosed (1-
16). It has been shown that primary fragmentation occurs immediately after the
injection of sorbent particles in the hot bed, as a consequence of thermal stresses
and internal overpressures due to release of gas (CO2 following calcination of raw
sorbent, steam following dehydration of spent/reactivated sorbent). Primary
fragmentation takes place in the dense bed/splashing region of FBC reactors,
resulting in the generation of coarse and fine fragments. Further breakage occurs as
a consequence of mechanical stresses experienced by the particles during their
lifetime in the reactor. Attrition by abrasion is related to the occurrence of surface
wear as the emulsion phase of the FB is sheared by the passage of bubbles, and
generates fine fragments that are quickly elutriated. Secondary fragmentation
gives rise to coarse and fine fragments, and may onset as a result of high-velocity
impacts of sorbent particles against targets (bed material, reactor walls/internals);
these impacts are likely experienced by the particles in the jetting region of FBC.
The exit region of the riser and the cyclone are other potential locations of impact
damage of sorbent particles in a CFBC reactor. The main features of
attrition/fragmentation mechanisms are summarized in Table 1 and a conceptual
framework for analyzing the effects of particle sulphation/attrition/fragmentation on
the fate of sorbents is represented in Figure 1a, where the simplification of lumping
sorbent particles into coarse and fine and the population of sorbent particles (of
different age and sulphation degree) into lime and sulphated limestone components
has been adopted. In this work a population balance model is presented, which aims
at predicting the sorbent inventory and particle size distribution, the partitioning of
sorbent between fly and bottom ash and the sulphur capture efficiency during steady
operation of an air-blown CFBC. The influence of attrition/fragmentation on the main
output parameters is assessed.
Table 1
Main features of attrition/fragmentation mechanisms.
Mechanism Caused by… Location: Generation of…
Primary fragmentation thermal/ dense bed/ coarse/fine
(decrepitation) mechanical stresses splashing zone fragments
Attrition by abrasion rubbing of dense bed fine
(surface wear) bed solids fragments
Secondary fragmentation collisions jetting region + coarse/fine
(impact fragmentation) against targets riser exit/cyclone fragments
ei
(b) gi
cyclone
riser
standpipe
EHE
&i
m
bottom bed
Wi
bi
Fig. 1. (a) Particle sulphation/attrition/fragmentation network for the assessment of

the fate of sorbents; (b) Schematic representation of CFBC loop with the indication
of relevant sorbent fluxes.
MODEL
A schematic representation of the CFBC loop with the indication of relevant sorbent
fluxes is reported in Figure 1b. Population balance equations can be written on the
sorbent present at steady state in the combustor. Calcination and primary
fragmentation are assumed to occur almost instantaneously so that the inventory of
the raw limestone can be neglected. Each particle in the population is characterized
by two variables: the particle size (d) and the sulphation degree (XS). A simplified
version of the population balance is hereby developed based on the assumption that
the sorbent can be lumped into two classes as far as XS is concerned: the
unconverted lime (L) and the sulphated limestone (SL). Accordingly, the population
balance in the d-XS domain simplifies yielding two 1-D equations in the d-domain.
Upon discretization of the domain and referring to the i-th particle size bin, equations
concerning the L and SL components read, respectively (cf. Notation):
Ri +1,L Wi +1,L n W j,L Ri,L Wi,L
& P0 (di )∆d +
m + ∑ k a,LU Pa,L (di )∆d = + ei,L + ai,L + bi,L + kCSO 2 Wi,L (1)
∆d j =i +1 dj ∆d
kCSO2 Wi,L Ri+1,SL Wi +1,SL n Wj,SL
[(1 − X S,i )MWL + X S,iMWSL ] + + ∑ k a,SLU Pa,SL (di )∆d =
MWL ∆d j=i +1 dj
(2)
Ri,SL Wi,SL
= + ei,SL + ai,SL + bi,SL
∆d
In Eq. (1), at LHS three inlet terms can be found, namely i) a term related to the
feeding; ii) a term related to continuous particle shrinkage, where:
R = k aU / 3 (3)
and iii) a term under summation, which takes into account particles formerly
belonging to coarser particle size bins that fall into the i-th size bin due to
attrition/fragmentation. At RHS, five outlet terms can be found, namely:
i) a term related to continuous particle shrinkage;
ii) a term related to sorbent loss by elutriation at the cyclone:
ei,L = [1 − η(di )]gi,L (4)
where gi,L is computed as a function of Wi,L according to (17) and the cyclone
collection efficiency is expressed as (cf. (18)):
η(di ) = 1/[1 + (dcut / di )c ] for di<120 µm, otherwise η=1 (5)
iii) a term related to attrition/fragmentation, where:
ai,L = k a,LUWi,L / di (6)
iv) a term related to the bed drain where, according to the hypothesis of perfect
mixing of bed material in the bottom bed, it is:
bi,L / b = W i,L / W (7)
v) a term related to the transfer from the L to the SL phase, driven by the
sulphation kinetics.
Eq. (2) can be written taking into account that, for particles sulphated according to a
core-shell pattern, it is:
shell 3
X S,i = X S [di − (di − 2δ)3 ] / di3 (8)
shell
for di>2δ, otherwise X S,i = X S . In particular, it has been discussed (19,20) that
sorbent sulphation in FBC takes place in two subsequent stages (Figure 2): stage I,
associated with the initial build-up of a sulphate-rich particle shell, and stage II,
associated with attrition-enhanced sulphation promoted by continuous attrition of
sulphated material. Accordingly, the SO2 capture efficiency can be calculated as:
cap n
inlet
ηdes = FSO / FSO = [kCSO 2 ∑ ( Wi,L X S,i ) / MWL ] /[m
& /(MWLrCa / S )] (9)
2 2
i =1
where the contribution to SO2 capture given by stage II is assumed negligible, based
on preliminary model computations. Finally, the SO2 concentration is calculated as:
C SO 2 = Cinlet
SO
(1 − ηdes ) (10)
2
Fig. 2. Outline of sulphation regimes. Stage I: build-up of the sulphated layer of
thickness δ up to a maximum local sulphation degree in the sulphated shell; Stage
II: attrition-enhanced sulphation regime.
Evaluation of Model Parameters
The model was solved in MATLABTM environment, assuming typical values for the
input parameters as reported in Table 2. In particular, the total bed inventory in the
riser per unit cross-sectional area has been set at 800 kg m-2, a typical figure based
on admissible pressure drops across the riser in practical operation of CFBC. Based
on realistic sorbent feeding rates and fuel ash content, it is further assumed that the
total bed inventory consists of W=250 kg m-2 of sorbent (either L or SL) and 550 kg
m-2 of fuel ash. Furthermore, P0 was expressed as a log-normal distribution
extending to the particle size range 5-2000 µm, with a mean particle size of 110 µm,
about 28% of particles finer than 100 µm and about 4% of particles coarser than
1000 µm. The size distribution of attrited fines Pa was expressed as an exponential
function for both L and SL:
Pa,L (di ) = Pa,SL (di ) = (1/ d) exp( −di / d) (11)
with d =35 µm. Attrition/fragmentation was considered to be active for particles
coarser than 50 µm, while for finer particles its contribution was supposed to be
negligible (ka,L=ka,SL=0). Moreover, the values of ka,L and ka,SL take into account both
attrition by surface wear (3) and impact fragmentation (10). This latter contribution
was calculated by estimating the fractional mass of fragments formed upon multiple
particle impacts in the jetting region of a typical full-scale CFBC. The entrainment
rate of sorbent particles into the jets, required to calculate the frequency and kinetic
energy of impacts, has been estimated according to Massimilla (21). Finally, attrition
in the cyclone has been neglected.
Table 2
Main input parameters of the model.
m& 0.013 kg m-2 s-1 c 4
ka,L 5×10-9 k 10-6 ppm-1 s-1
ka,SL 10-9 shell
XS 0.55
U 2.5 m s-1 δ 50 µm
W 250 kg m-2 rCa/S 2.5
dcut 10 µm Cinlet 2000 ppm
SO 2
Model Results
The influence of attrition on the combustor’s performance has been assessed by

comparing results obtained from computations performed neglecting attrition (i.e.,
ka=0 for both L and SL) with those in which attrition was considered. Results of
computations for the no-attrition case are reported in Figure 3 and Table 3. Figure
3a shows the probability density functions (PDF) of particle sizes, whereas the
distribution is reported as cumulative undersize in Figure 3b. A noticeable shift
toward coarser particles can be observed for material reporting to bottom ashes as
compared with the lime feeding. The PDF peak is located at 120 µm, particles finer
than 50 µm are hardly found and only 7% of particles mass is finer than 100 µm. On
the other hand, the PDF peak is located at 65 µm in the population reporting to the
fly ash: particles coarser than 120 µm are not present, 95% of particles mass is finer
than 100 µm and the mean Sauter diameter is 48 µm. These values are critically
dependent on cyclone efficiency characteristics. Values reported in Table 3 show
that sorbent reporting to fly ashes accounts for 21% of the total sorbent ashes even
without attrition, due to the presence of elutriable fines in the sorbent feeding. The
inventory of lime (W L) is 22 kg m-2, corresponding to 8.8% of the total sorbent
inventory. Sulphur capture corresponds to ηdes=0.78 when attrition is neglected.
0.015 1.1
(a) (b)
lime feed 1.0 lime feed
−]
cumulative PSD, mass basis [−
bottom ashes bottom ashes

µm ]
0.9
-1
(b-stream) (b-stream)
PDF of particle sizes [µ
fly ashes 0.8 fly ashes

0.010 (e-stream) (e-stream)
0.7
0.6
0.5
0.4
0.005
0.3
0.2
0.1
0.000 0.0
1 10 100 1000 10000 1 10 100 1000 10000
µm]
particle diameter [µ µm]
particle diameter [µ
Fig. 3. Model results without attrition: (a) Probability density functions (PDF) of
particle sizes for lime feed, bottom and fly ashes; (b) Cumulative particle size
distributions (PSD) for lime feed, bottom and fly ashes.
Table 3
Selected output parameters of the model.
f WL WSL dS for ηdes
-2 -2
[-] [kg m ] [kg m ] fly ashes [µm] [-]
Without attrition 0.21 22 228 48 0.78
With attrition 0.38 18 232 34 0.74
With attrition (ka,L*3) 0.43 13 237 31 0.68
Model results considering the effect of attrition are reported in Figure 4 and Table 3.
Plots in Figure 4 display the same general features of those corresponding to the
no-attrition case. However it can be recognized that attrition/fragmentation induce a
pronounced shift of the curves toward finer particle sizes. The PDF peaks are
located at 115 µm and 55 µm for bottom and fly ashes, respectively. The fractional
mass of sorbent finer than 100 µm is 8% and 97% for bottom and fly ashes,
respectively. The mean Sauter diameter of sorbent reporting to fly ashes is dS=34
µm. As expected, consideration of attrition brings about an increase of the fractional
mass of sorbent reporting to the fly ash (f raises to 0.38) and a decrease of W L (18
kg m-2, that is 7.2% of the total sorbent inventory). Correspondingly, W SL increases
due to the fact that attrition of L particles determines finer L-particle sizes and, in
turn, a better Ca exploitation for SO2 capture (cf. Eq. (8)). It is noteworthy that this
feature does not imply an improvement in ηdes, which decreases from 78% to 74%.
This finding should be related to the competing effects of the better Ca exploitation
in fine particles, on the one hand, and of the larger amount of material which is lost
at the cyclone, on the other, when attrition/fragmentation are at work. Under the
operating conditions selected in this work, the negative effect associated with fine
sorbent loss at the cyclone overweighs the positive effect of a more extensive
degree of calcium exploitation, resulting into a worse SO2 abatement efficiency.
0.015 1.1
(a) (b)
lime feed 1.0 lime feed
−]
cumulative PSD, mass basis [−
bottom ashes bottom ashes

µm ]
0.9
-1
(b-stream) (b-stream)
PDF of particle sizes [µ
fly ashes 0.8 fly ashes

0.010 (e-stream) (e-stream)
0.7
0.6
0.5
0.4
0.005
0.3
0.2
0.1
0.000 0.0
1 10 100 1000 10000 1 10 100 1000 10000
µm]
particle diameter [µ µm]
particle diameter [µ
Fig. 4. Model results with attrition: (a) Probability density functions (PDF) of particle
sizes for lime feed, bottom and fly ashes; (b) Cumulative particle size distributions
(PSD) for lime feed, bottom and fly ashes.
A sensitivity analysis has been carried out with reference to the

attrition/fragmentation constant for L particles (ka,L). In fact, while the value assumed
for ka,SL (cf. Table 2) is to be considered as an upper limit for typical sorbents and
operating conditions, the higher comminution susceptibility of L particles makes it
possible to consider ka,L-values also greater than the one reported in Table 2. Thus,
Table 3 lists the main results obtained when, holding all the other operating
conditions/parameters, ka,L was increased by a factor of 3, 5, 8 or 10. The model
sensitivity was appreciable: as expected, enhanced attrition gives rise to increased
f-values (up to 53%), decreased W L-values (down to 8 kg m-2) and decreased dS-
values for fly ashes (down to 28 µm). The overall detrimental influence that
attrition/fragmentation do have on ηdes is again highlighted: ηdes is as low as 54%
when ka,L was 10-times increased.
CONCLUSIVE REMARKS
The influence of particle attrition/fragmentation on sorbent inventory and particle

size distribution in air-blown circulating fluidized bed combustors was carefully
investigated by solving a population balance model able to take into account attrition
and fragmentation phenomena, generation of fly and bottom ashes, kinetic aspects
related to the SO2 capture by lime-based sorbent particles. With reference to a
base-case in which attrition was deliberately neglected, it was clearly shown that the
presence of attrition ends up into increased fly ash amounts having finer mean
particle sizes and decreased lime inventories in the bottom bed. Interestingly, the
desulphurization ability of the system decreased since the effect related to the
greater amount of material lost at the cyclone seemed to overweigh the effect
related to a better calcium exploitation for SO2 capture when finer particles are
considered. The sensitivity of the model with reference to attrition/fragmentation
constants appeared to be noticeable. Altogether, model computations confirmed the
relevance of attrition and fragmentation to the performance of circulating fluidized
bed combustors.
NOTATION
-2 -1
a attrition rate [kg m s ]
-2 -1
b overall mass rate of sorbent bed drain [kg m s ]
c exponent appearing in Eq. (5) [-]
C SO2 SO2 concentration [ppm]
Cinlet
SO
SO2 inlet concentration [ppm]
2
∆d particle diameter interval [m]

δ thickness of the sulphated shell [m]
d particle diameter [m]
d mean diameter of attrited fragments [m]
dcut cyclone cut diameter [m]
dS mean Sauter diameter [m]
η cyclone collection efficiency [-]
ηdes SO2 abatement efficiency [-]
-2 -1
e overall mass rate of sorbent lost by elutriation [kg m s ]
f ratio e/(e+b) [-]
cap -2 -1
FSO molar rate of SO2 captured by the sorbent [kgmol m s ]
2
inlet -2 -1
FSO molar rate of SO2 at the inlet [kgmol m s ]
2
-2 -1
g overall net mass rate along the riser of sorbent material [kg m s ]
-1 -1
k sulphation kinetic constant [ppm s ]
ka attrition/fragmentation constant [-]
& -2 -1
m overall mass feed rate of lime particles [kg m s ]
-1
MW molecular weight [kg kgmol ]
-1
P0 particle size distribution of lime after primary fragmentation [m ]
-1
Pa particle size distribution of attrited fragments [m ]
-1
R rate of particle shrinkage due to attrition/fragmentation [m s ]
rCa/S calcium to sulphur inlet molar ratio [-]
-1
U gas superficial velocity in the primary region of the riser [m s ]
-2
W overall mass of sorbent in the bottom bed [kg m ]
XS sulphation degree [-]
shell
XS sulphation degree in the sulphated shell [-]
Subscripts: i, j, n are referred to particles in the i-th, j-th, last (coarsest) size bin; L is referred to lime
particles; SL is referred to sulphated limestone particles.
REFERENCES
[1]. Chandran RR, Duqum JN. Attrition characteristics relevant for fluidized bed combustion. In:
Grace JR, Shemilt LW, Bergougnou MA, editors. Fluidization VI, New York: Engineering Foundation;
1989, pp. 571-80.
[2]. Couturier MF, Karidio I, Steward FR. Study on the rate of breakage of various Canadian
limestones in a circulating transport reactor. In: Avidan AA, editor. Circulating Fluidized Bed Technology
IV, New York: American Institution of Chemical Engineers; 1993, pp. 672-8.
[3]. Scala F, Cammarota A, Chirone R, Salatino P. Comminution of limestone during batch fluidized-
bed calcination and sulfation. AIChE J 1997;43:363-73.
[4]. Di Benedetto A, Salatino P. Modelling attrition of limestone during calcination and sulfation in a
fluidized bed reactor. Powder Technol 1998;95:119-28.
[5]. Scala F, Salatino P, Boerefijn R, Ghadiri M. Attrition of sorbents during fluidized bed calcination
and sulphation. Powder Technol 2000;107:153-67.
[6]. Montagnaro F, Salatino P, Scala F. The influence of sorbent properties and reaction temperature
on sorbent attrition, sulfur uptake, and particle sulfation pattern during fluidized-bed desulfurization.
Combust Sci Technol 2002;174:151-69.
[7]. Werther J, Reppenhagen J. Attrition. In: Yang WC, editor. Handbook of Fluidization and Fluid-
Particle Systems, New York: Dekker; 2003, pp. 201-37.
[8]. Chen Z, Lim J, Grace JR. Study of limestone particle impact attrition. Chem Eng Sci
2007;62:867-77.
[9]. Saastamoinen JJ, Shimizu T. Attrition-enhanced sulfur capture by limestone particles in fluidized
beds. Ind Eng Chem Res 2007;46:1079-90.
[10]. Scala F, Montagnaro F, Salatino P. Attrition of limestone by impact loading in fluidized beds.
Energy Fuels 2007;21:2566-72.
[11]. Montagnaro F, Salatino P, Scala F, Chirone R. An assessment of water and steam reactivation
of a fluidized bed spent sorbent for enhanced SO2 capture. Powder Technol 2008;180:129-34.
[12]. Scala F, Montagnaro F, Salatino P. Sulphation of limestones in a fluidized bed combustor: the
relationship between particle attrition and microstructure. Can J Chem Eng 2008;86:347-55.
[13]. Shimizu T, Saastamoinen J. Optimization of limestone feed size of a pressurized fluidized bed
th
combustor. In: Yue G, Zhang H, Zhao C, Luo Z, editors. Proceedings of the 20 International Conference
on Fluidized Bed Combustion, Xi’an; 2009, pp. 1028-34.
[14]. Montagnaro F, Salatino P, Scala F. The influence of temperature on limestone sulfation and
attrition under fluidized bed combustion conditions. Exp Therm Fluid Sci 2010;34:352-8.
[15]. Montagnaro F, Salatino P, Santoro L, Scala F. The influence of reactivation by hydration of spent
SO2 sorbents on their impact fragmentation in fluidized bed combustors. Chem Eng J 2010;162:1067-74.
[16]. Yao X, Zhang H, Yang H, Liu Q, Wang J, Yue G. An experimental study on the primary
fragmentation and attrition of limestones in a fluidized bed. Fuel Process Technol 2010;91:1119-24.
[17]. Wirth KE. Fluid mechanics of circulating fluidized beds. Chem Eng Technol 1991;14:29-38.
[18]. Redemann K, Hartge EU, Werther J. A particle population balancing model for a circulating
fluidized bed combustion system. Powder Technol 2009;191:78-90.
[19]. Shimizu T, Peglow M, Sakuno S, Misawa N, Suzuki N, Ueda H, et al. Effect of attrition on SO2
capture by limestone under pressurized fluidized bed combustion conditions-Comparison between a
mathematical model of SO2 capture by single limestone particle under attrition condition and SO2 capture
in a large-scale PFBC. Chem Eng Sci 2001;56:6719-28.
[20]. Scala F, Salatino P. Limestone attrition under simulated oxyfiring fluidized-bed combustion
conditions. Chem Eng Technol 2009;32:380-5.
[21]. Massimilla L. Gas jets in fluidized beds. In: Davidson JF, Clift R, Harrison D, editors. Fluidization
II, London: Academic Press; 1985, pp. 133-72.
CaO LOOPING CYCLE FOR CO2 SEPARATION
Tadaaki Shimizu*1, Takayuki Takahashi2, Hiroko Narisawa1, Yasuyuki Murakami2,
Liuyun Li 1, and Heejoon Kim1
1
Department of Chemistry and Chemical Engineering, Niigata University
2
Graduate School of Science and Technology, Niigata University
*: corresponding author
2-8050 Ikarashi, Niigata, 950-2181, Japan, tshimizu@eng.niigata-u.ac.jp
ABSTRACT
A dual fluidized bed process using CaO-based solid sorbent is considered to be a

promising technology to separate CO2 from flue gas with low energy penalty. As
reactor for CaO-looping cycle, both bubbling fluidized bed and “fast” fluidized bed are
available, thus four possible combinations, (bubbling or fast absorber)x(bubbling or
fast regenerator), are conceivable for this process. In this work, the authors discuss
favorable combination of reactor type from viewpoints of heat removal from
carbonation reactor and on energy penalty associated with dilution of pure oxygen by
CO2 in the regenerator. As conclusion, suitable combination was found to be
bubbling bed absorber and fast regenerator. Design of bench-scale experimental
apparatus of the present system was also carried out. Bubbling bed absorber was
designed to achieve 86 % CO2 removal efficiency from flue gas. Preliminary
operating results of solid circulation at room temperature are also presented.
INTRODUCTION
It is well known that the concentration of CO2 in the atmosphere has been increasing
and the greenhouse effect (global warming) is anticipated. Fossil fuel combustion
such as coal-fired power plant is one of the major sources of CO2. An approach to
reduce CO2 emission into the atmosphere is the separation of CO2 from flue gas of
conventional air-blown combustion system followed by CO2 storage in the ground.
Attempts have been made to separate CO2 from flue gas using absorption by amine
solution (1) and adsorption by solids such as zeolite (2). Another way is to burn fuel
using pure oxygen, which is separated from air in advance, to make the flue gas pure
CO2 (1). For combustion using O2, pure O2 is usually diluted with recycled CO2 to
control the temperature in the combustion chamber. CaO-looping cycle has been
developed as a CO2 separation process with low energy penalty (3); CaO particles
capture CO2 from flue gas in one reactor (absorber) and produced CaCO3 is
decomposed to CaO in another reactor (regenerator) by supplying heat through fuel
combustion in O2/CO2 atmosphere,.
Since CaO-looping process needs continuous solid transportation between absorber

and regenerator, fluidized bed solid circulation system is considered to be suitable for
reactor system. There are two types of fluidized beds which can be used as reactor,
bubbling fluidized bed and “fast” fluidized bed. In the fast fluidized bed, all of the
particles are entrained to the top of the reactor in high-velocity gas stream. In
literature, different combinations of reactor type have been employed not only for
experiments but also for simulation of reactors; bubbling bed absorber (3, 4, 5), fast
bed absorber (6, 7, 8, 9), bubbling regenerator (9), and fast bed regenerator (4, 5, 7,
8). Both bubbling bed and fast bed can be used to capture CO2 in the absorber if
sufficient gas-to-solid contact time is to be given. However, for put this concept into
practice, one must take account of heat removal from the exothermic reaction in the
absorber to maintain bed temperature. In general, reactor size is determined not only
by reaction rate but also installation of heat transfer surface. Thus the design of heat
transfer surface is necessary.
The objective of the present work is to discuss suitable combination of reactor type
for the CaO-looping process. Design of heat transfer surface was conducted for both
fast fluidized bed absorber and bubbling bed absorber. Then design of a bench-scale
experimental apparatus was then carried out based on the selection of reactor type.
Also preliminary experiments were carried out to measure solid circulation rate in the
system under a room temperature condition.
REACTOR DESIGN AND SELECTION OF REACTOR TYPE
Absorber Design
First, material and heat balances of CaO-looping process were calculated. Fig.1
shows an example of material balance and heat balance of this process of total gross
electricity output of 350 MW. In order to avoid hot-spot formation within the
regenerator, in which coal particles are burned in high O2 concentration atmosphere,
fed O2 (pure) was assumed to be diluted by CO2 at a ratio of CO2/O2=1. From the
material balance, feed rates of gases were calculated to design horizontal cross
sectional area of absorber and regenerator. Fig.2 shows enthalpy-temperature
diagram of heat source and heat sink for secondary steam cycle denoted as
“Steam2” in Fig.1-b. The heat from the absorber and sensible heat of CO2 stream
from regenerator is assumed to produce subcritical steam as a separated steam
cycle from existing steam cycle of air-blown combustor (denoted as “Steam1”). From
the heat removal requirement and temperature difference between steam and heat
source, the required heat transfer surface area was calculated.
Heat transfer design in a fast bed absorber was carried. Heat transfer coefficient of
reactor wall (h [W/m2K]) is empirically given as a function of suspension density (susp
[kg/m3]) as (10, 11):
h = asusp0.5 (a = 30 - 40) (1)
h = 58susp0.36. (2)
Both equations give similar results. When susp is assumed to be 55 kg/m3, h is
estimated to be 260 (eq.1) – 245 (eq.2) W/m2K. At this suspension density, total
pressure drop across a fast bed riser of a height of 50 m is 27 kPa, which is nearly
the same as that of bubbling bed absorber, thus an advantage of fast bed, lower
pressure drop, is lost under the present suspension density condition. Also it should
be mentioned that this suspension density of 55 kg/m3 is far higher than solid loading
in the gas at the exit of the absorber: the solid loading in the gas at the exit should be
1.2 kg/m3 to attain solid/gas material flow ratio shown in Fig.1. A measure to enhance
internal solid circulation in the riser is thus required. Therefore, this suspension
density of 55 kg/m3 is considered to be maximum conceivable value.
CO2 0.17 CO2 2.85 Flue gas 39 CO2 32
O2 0.23 O2 0.06 Steam1 89 Steam2 134
N2 5.16 N2 0.03 CaO
H2O 0.46 H2O 0.41 Steam2 CaCO3 HR
286 273 144
Absorber Regenerator
CaO 7.60 (T=873K) (T=1223K)
ΔHR CaO Loss
Absorber CaCO3 0.84 Regenerator 144 393 7
(T=873K) (T=1223K)
CaO 8.44
Steam1 62
CO2 1.02 Fuel 436
O2 0.23 Coal 13.1 Steam1 Gas 0
N2 5.16 O2 1.09 263
H2O 0.46 CO2 1.09 Main
combustor
Main Unit: Loss
(air-blown)
combustor Coal: [kg/s] 7
(air-blown) Unit: [MW]
Others: [kmol/s]
Steam1: Primary cycle
Coal 14.5 Fuel 483 Steam2: Secondary cycle
Air 6.53 Air 0 ΔHR: Heat of reaction
(a)Material flow (b) Heat flow
Fig.1 An example of material and heat balance of a CaO-looping cycle of total gross
electricity output of 350 MW with dilution of pure O2 by CO2 at CO2/O2=1.
1400 A B C
Heat transfer surface design in a fast bed 1200
Temperature [K].
B1 B2 B3 B4
was conducted assuming a bed-to-wall
1000
heat transfer coefficient of h = 250 W/m2K.
The overall heat transfer resistance is the 800
sum of heat transfer resistances, i.e., 600
tube-to-steam/water heat transfer 400
resistance, conductive resistance in tube WH Ev SH RH SH
wall, and bed-to-wall heat transfer 200
resistance. Thus the overall heat transfer 0 100 200 300 400
Enthalpy rate [MW]
coefficient was calculated separately in
Fig.2 Enthalpy-temperature diagram of
water preheater, evaporator, reheater,
heat source and secondary steam cycle
and superheater regioms (Table 1). The
denoted as “Steam2” in Fig.1-b. (Dash
detail of calculation is available
line: Heat source; Solid line: Heat sink; A,
elsewhere (3). In order to avoid erosion of
C: sensible heat of CO2; B: heat
heat transfer surface, flat panel heat
recovery in absorber; WH: water
transfer exchangers are employed in fast
preheat; EV: evaporation; SH:
beds when heat transfer surfaces are to
superheat; RH: reheat).
be installed in addition to reactor wall.
Fig.3 shows an example of estimated plant size and heat transfer panel requirement
for the case of fast bed absorber combined with fast bed regenerator. The cross
sectional area of absorber is determined by gas flow rate and superficial gas velocity.
In this work, a superficial gas velocity of 6 m/s was assumed. Cross sectional area of
absorber was 2.25 times of that of regenerator. This proportion is similar to the
design by Ströhle (8) which gave an absorber/regenerator ratio of 2.6. To install heat
transfer panels, rectangular horizontal cross section of 11 m x 7 m was assumed.
The reactor wall is used as water prehater. To attain required evaporation, reactor
height of 50 m was found to be required. For evaporator, reheater, and superheater,
flat panel heat transfer surfaces of 40 m in height and 7 m in width are assumed.
Since both sides of flat panel can be used for heat transfer, a heat transfer surface
area of 560 m2 is available for one panel. Total 13 panels were calculated to be
required, in which two panels are for evaporator, seven for reheater, and four for
supereheater, respectively. Installing such large number of heat transfer panels in a
fast bed is considered to be not easy. Therefore, the idea of employing fast bed for
absorber is abandoned in this work.
Cy clon es
Cyc lon e Cyclone
HT p an els
2 E vap.
7 R eheat.
4 S u per h .
50 m φ 6.6 m
M em b r an e
φ 6 .6 m
wall f or w at er
pr eh eatin g
26 m 13 m
Ab sor ber Ab sor ber

Regenerator Reg en erator
11m 7m
Side view Fron t view
Abs or ber Abs or ber
Side v iew F ron t view Fig.4 Estimated plant size and heat
Fig.3 Estimated plant size and heat transfer panel requirement for the
transfer panel requirement for the case of case of bubbling fluidized bed
fast bed absorber combined with fast bed absorber combined with fast bed
regenerator for total gross electricity regenerator for total gross electricity
output of 350 MW. output of 350 MW.
Table 1 Estimation of required heat transfer surface area for heat removal from fast
bed absorber assuming bed-to-wall heat transfer coefficient of 250 W/m2K
Heat recovery Overall heat transfer Heat transfer
rate [MW] coefficient [W/m2K] area [m2]
Water preheater 111 183 1753
Evaporator 72 218 1369
Reheater 68 101 3874
Superheater 36 85 2302
Bubbling fluidized bed absorber has already been designed in the authors’ previous
work (3). The cross sectional area was given by the volume flow rate and superficial
gas velocity (assumed to be 1 m/s to suppress elutriation of solids). The bed height
to install heat transfer tubes had been calculated to be 2.4 m and this height was
higher than the bed height to capture CO2. As shown in Fig. 4, considerably large
cross sectional area is required because of low gas velocity. Stacked bed design
may be required to reduce the plant size. Nevertheless, bubbling fluidized bed is
considered to be suitable for absorber because the density of heat transfer surface
can be higher than that of fast bed absorber.
Regenerator Design
Regenerator should be basically adiabatic to suppress heat loss, thus one important
operating parameter is dilution of fed oxygen by recycled CO2 in order to prevent
hot-spot formation. As shown in Fig.5, dilution by CO2 decreases net efficiency
through increase power consumption of air separation unit (ASU) because CO2
carries sensible heat away from the reactor and more fuel combustion is necessary
with increasing CO2 recycle. To reduce the risk of hot-spot formation at low recycle
ratio of CO2, fast bed is considered to be advantageous because of vigorous solid
mixing near the reactor inlet.
40 0.12
BENCH SCALE REACTOR DESIGN
35
ASU power / gross output [-].

0.1
Net efficiency [%] (HHV).

Design parameters and reactor size 30
0.08
25
As discussed above, one advantageous 20 0.06
combination of reactor type for
CaO-looping cycle is bubbling bed 15
(a) 0.04
absorber and fast bed regenerator. A 10
Net efficiency
bench scale experimental apparatus is 5 ASU power consumption
0.02
designed based on this combination.
0 0
Material flow was calculated assuming
0 0.5 1 1.5 2
that oxygen is diluted with the same
CO2 recycle/O2 feed [mol/mol]
amount of CO2. Table 2 shows the
design parameters. For the absorber, a Fig.5 Estimation of the change in net
bubbling bed of 93 mm in I.D. is efficiency and ASU power consumption
adopted. For the regenerator, a fast bed with dilution of O2 by recycled CO2 at
of 22 mm in I.D. is adopted. The design ambient temperature.
size of sorbent particle is 0.3 mm,
whose minimum fluidizing velocity at 873 K and terminal velocity at 1273 K are 0.026
m/s and 1.48 m/s in each atmosphere, respectively. Thus fluidization in absorber and
transportation of particles in regenerator are expected to be attained. The design
parameters such as the ratio of the cross sectional area of two reactors and gas
velocities are different from that of large scale plant (Fig. 4) because of the height
limitation of bench-scale unit. Nevertheless this reactor is expected to attain
necessary CO2 recovery and solid circulation as discussed later. The material flow
rates are determined by scaling down the material flow shown Fig.1-a.
Table 2 Design parameters of CaO-looping bench scale plant

Absorber
ID Gas feed rate Gas velocity Inlet gas composition [%] Temperature
[mm] [mol/s] [m/s] CO2 H2O O2 N2 [K]
93 0.0213 0.226 14.8 6.7 3.3 75.2 873
Regenerator
ID Gas feed rate Gas velocity Coal feed Temperature
O2 CO2 Bottom Top rate
[mm] [mol/s] [mol/s] [m/s] [m/s] [g/s] [K]
22 0.0034 0.0034 1.79 2.75 0.041 1273
Solid circulation
CaO/Captured CO2 CaO circulation rate Solid circulation/Gas flow rate in riser
[mol/mol] [g/s] [kg/kg]
10 1.47 3.2
Estimation of CO2 capture efficiency in absorber
In order to design the bed height of absorber, CO2 capture efficiency was estimated
using Kunii-Levenspiel model. The detail of the model is described elsewhere (3).
The reaction of CaO with CO2 is characterized by maximum utilization of CaO (D)
and rate constant (kR); change in CaO conversion (X) with time is given as follows:
3 -1 -1
dX/dt = kR(D - X). (3) kR=25[m kmol s ]
16
The maximum utilization of CaO is known to
14 D=0.17
decrease after repeating carbonation –
Averaged CO2
12
calcination cycles (3, 12). After a number of
conc. [%]
10
carbonation – calcination cycles, maximum
8
conversion finally decreased to 0.17 (12). Thus
6
D=0.17 was assumed. Reaction rate constant
4
of kR =25 m3/kmol.s was assumed based on the
2
author’s previous work (3). The gas velocity is
0
given in Table 2. The calculation result is shown
in Fig.6. A CO2 removal efficiency of 86% was 0 0.1 0.2 0.3
Bed height [m]
calculated to be attained when a bed height of Fig.6 Estimated CO2 capture in
0.30 m and bubble diameter of 4 cm was bubbling fluidized bed operated
assumed. Thus the present experimental under a condition shown in
apparatus is expected to be suitable for CO2 Table 2 assuming a bubble
capture experiments. diameter of 4 cm.
PRELIMINARY OPERATION RESULTS OF BENCH SCALE REACTOR
A bench-scale reactor of CaO-looping cycle was constructed and operated at room

temperature. The objective of the cold-experiments was to confirm whether required
solid circulation rate could be attained. Schematic diagram of the experimental
apparatus is shown in Fig.7. The experimental apparatus consisted of riser reactor
(22 mm in I.D. and 1.93 m in height) and bubbling fluidized bed reactor (93 mm in
I.D.), both of which were made of stainless steel. The gas exit at the top of the riser is
connected to a cyclone in which particles were separated from the gas then the
captured particles were transported to the bubbling fluidized bed by gravity. Particles
in the bubbling fluidized bed were drained from an overflow tube. The fluidizing bed
height (i.e. height of overflow tube) was 0.30 m above gas distributor. The particles
flowed through a standpipe whose bottom is connected to a loopseal. The particles
from the loopseal were fed into the bottom of the riser. The bed material was quartz
sand of average size of 0.15 mm. Under the present cold model experiments, gas
velocities were 1.75 m/s, 0.050 m/s, and 0.067 m/s in the riser, in the bubbling bed,
and in the loopseal, respectively.
In order to measure the solid circulation rate, the standpipe was equipped with three
thermocouples at an interval of 10 cm and with a tracer injection system from the top.
As tracer, heated bed material was employed. A batch of tracer was injected from the
top of the standpipe. The change in temperature with time after tracer injection was
continuously measured. When the tracer particles passed the location of the
thermocouple, a peak of the temperature was observed (Fig.8). From the time lag (tD)
of the peaks and the distance between two thermocouples (L), the descending
velocity (UD) of solids in the standpipe is given as:
UD=L/tD. (4)
By assuming that the solids in the standpipe forms moving bed without bubbles and
the solid density in the standpipe is identical to the bulk density of the solids (b), the
solid circulation rate (Gs) is given as a product of descending velocity, bulk density,
and cross sectional are of loopseal (As) as follows:
Gs  As  bU D . (5)
Fig.9 shows the solid circulation rate that attained at a pressure drop across the riser
of about 3 kPa. Solid circulation rate under the present condition was 3 – 4 g/s, which
is considered to sufficient for CO2 capture experiments in the present test apparatus
(Table 2). The present measurement method can be applied for hot experiments. For
hot experiments, cold limestone particles can be used as tracer because circulating
particles from the bubbling bed absorber are sufficiently hot (about 873 K) and the
temperature decrease due to tracer can be easily detected.
Top - 10cm below top
Cyclone 10 - 20 cm below top
Sand
Heater Estimated from riser pressure drop
5
Solid circulation rate [g/s] 4

Absorber
(BFB) ΔP 3
Regenerator
Air (Fast FB) 2
Stand
T pipe
T 1
T
0
Loopseal
0 1 2 3 4
Pressure drop across riser [kPa]
Air Fig.9 Comparison between solid
Air circulation rate measured by tracer
Fig.7 Bench-scale fluidized bed solid injection into the standpipe and
circulation system for cold experiments. estimation from riser pressure drop.
45 10
Pressure drop across riser [kPa]
tD tD
40
Temperature [ C]
o
35
1
30
25
Top Top - 10cm
Top - 20cm
20 0.1
0 20 40 60
0 20 40 60 80
Time after tracer injection [s] Time after stopping solid circulation [s]
Fig.8 Typical temperature change in Fig.10 Decrease in pressure drop
standpipe at different vertical position across riser after stopping solid
after injecting a batch of hot sand circulation.
(tracer) into the standpipe.
Another approach to measure the solid circulation rate is to measure the pressure
drop across the riser ( PR ) after stopping solid circulation by stopping gas feed into
the loopseal. As shown in Fig.10, the pressure drop across the riser decreased with
time (t) according to the first-order equation after stopping solid circulation as:
ln PR   ln PR ,0   kt (6)
where k is first-order decay constant. This relationship indicates that the decreasing
rate of pressure drop across the riser is proportional to the pressure drop itself. By
neglecting pressure drop due to gas flow, the pressure drop across the riser is given
by total amount of solid in the riser (Ws), cross sectional area of riser (AR) and
acceleration of gravity (g). Thus the entrainment rate of solids is given as:
dPR g dWs
  kPR . (7)
dt AR dt
Under constant pressure drop condition, solid circulating rate is thus given as:
dWs kPR AR
Gs    kWs  . (8)
dt g
As shown in Fig.9, solid circulation rate measured by tracer injection into the
standpipe agreed well with that estimated by eq.8. Therefore, the solid circulation
rate can be monitored by measuring the pressure drop across the riser.
CONCLUSION
Conceptual design of a CaO-looping cycle was carried out. To recover heat from
absorber, bubbling fluidized bed is considered to be more suitable than fast bed.
Experimental apparatus is designed and CO2 capture efficiency in the absorber was
estimated. Solid circulation rate was measured under a cold model condition and
required solid circulation rate was attained.
REFERENCES
(1) Noguchi, Y., Nakayama, S., Kiga, T., Utada, O., Makino, H.,
Karyoku-Genshiryoku-Hatsuden (The Thermal and Nuclear Power, in Japanese),
Vol.44, pp.412 – 419, 1993
(2) Naka, H., Shibagaki, T., Takatsuka, T., Kajiyama, R., Hirohama, S., Karyoku-
Genshiryoku- Hatsuden (The Thermal and Nuclear Power, in Japanese), Vol.44,
pp.816 – 821, 1993
(3) Shimizu, T., Hirama, T., Hosoda, H., Kitano, K., Inagaki, M., Tejima, K., Trans
IChemE Part A (Chem. Eng. Res. Des.), Vol.77, pp.62-68, 1999
(4) Romeo, M., Energy Procedia, Vol.1, pp.1099 - 1106, 2009
(5) Hughes, R.W., Lu, D.Y., Anthony, E.J., Macchi, A., Fuel Processing Technol.,
Vol.86, pp.1523-1531, 2005
(6) Ströhle, J., Lasheras, A., Galloy, A., Epple, B., Chem. Eng. Technol., Vol.32, No.3,
pp.435 – 442, 2009
(7) Abanades, J.C., Alonso, M., Rodriguez, N., Gonzalez, B., Grasa, G., Mrillo, R.,
Energy Procedia, Vol.1, pp.1147- 1154, 2009
(8) Ströhle, J., Galloy, A., Epple, B., Energy Procedia, Vol.1, pp.1313-1320, 2009
(9) Charitos, A., Hawthorne, C., Bidwe, A.R., Korovesis, L., Schuster, A.,
Scheffknecht, G., Powder Technol., Vol.200, pp.117 – 127, 2010
(10) Andersson, B.A., B.Leckner, Int. J. Heat Mass Transf., Vol.35, pp.3353-3362,
1992
(11) Andersson, B.A., Powder Technol., Vol.87, pp.239-248, 1996
(12) Abanades, J.C., Chem. Eng. J., Vol.90, pp.303-306, 2002
ECVT IMAGING OF 3-D FLOW STRUCTURES AND SOLIDS
CONCENTRATION DISTRIBUTIONS IN A RISER AND A BEND
OF A GAS-SOLID CIRCULATING FLUIDIZED BED
Fei Wang, Qussai Marashdeh and Liang-Shih Fan*
William G. Lowrie Department of Chemical and Biomolecular Engineering
The Ohio State University
140 West 19th Avenue, Columbus, Ohio 43210, USA
*To whom correspondence should be addressed (fan@chbmeng.ohio-state.edu)
ABSTRACT
Experimental studies using electrical capacitance volume tomography (ECVT) are

conducted to examine gas-solid flows in a riser and a bend of a 0.05 m (2 in) ID gas-
solid circulating fluidized bed (CFB) system. The quantitative measurements using
ECVT are made that illustrate a three-dimensional symmetric core-annulus structure
in the riser and a non-centro-symmetric core-annulus structure in the bend. Results
on the volume solids holdup distributions in the riser and in the bend at various
operating conditions are also obtained.
INTRUDUCTION
Gas-solid flows have been employed extensively in industrial operations (Kunii and
Levenspiel (1), Fan and Zhu (2)). Bent vessels are commonly used in solids handling
systems such as an exit of a riser in a gas-solid circulating fluidize bed (CFB) and
elbows to change the solids transport direction in solids pneumatic conveying. The
details of the gas-solid flow behaviors in such bends as well as in straight vessels
are of great importance for the design of the CFB reactors and pneumatic conveying
systems. Due to the lack of advanced imaging technologies in the past,
visualizations of on-line three-dimensional gas-solid flow patterns and measurements
of volumetric solids holdup in straight vessels and bends were rarely reported.
Currently, there are two main methods of measurement, intrusive and non-intrusive
techniques, applied to gas-solid flows. Classification of these methods is predicated
by the mechanism by which measurement signals are acquired. For intrusive
techniques, the measurement sensor, such as a capacitance probe (Lanneau (3),
Geldart and Kelsey (4)), optical fiber probe (Yasui and Johanson (5), Cui and
Chaouki (6)), endoscopic probe (Peters et al. (7), Du et al. (8)) or pressure
transducer probes (Kang et al. (9), Geldart and Xie (10)), requires direct contact with
the flow media to record a measurement. This intrusive nature may potentially
disturb the physical flow behavior. Conversely, non-intrusive techniques are based
on remote acquisition of the measurement signals from sensors mounted away from
the flow and avoiding interference with the internal of a multiphase flow system. Non-
intrusive techniques are widely applied for the measurements of gas-solid flows. In
this regard, electrical capacitance volume tomography (ECVT) has emerged as a
practical technology for realistic measurements without interfering with the flow
(Warsito et al. (11), Marashdeh et al. (12), Wang et al. (13, 14, 15)). ECVT has
provided the means for imaging gas-solid flows in complex geometries due to the
flexibility of its sensors (Marashdeh et al. (12), Wang et al. (13, 15)).
In this study, an advanced ECVT sensor system is designed for imaging gas-solid
flows in complex geometries. Two developed sensors are used for imaging real-time
three-dimensional gas-solid flows in a riser and a 90o bend at the exit region of a
CFB. The flow structures in the riser and the bend are analyzed based on
quantitative ECVT images. The volumetric solids holdup in the riser and the bend in
the CFB are obtained for various superficial gas velocities and solids fluxes.
EXPERIMENTAL SETUP
Figure 1 is a schematic diagram of the gas-solid circulating fluidized bed. The CFB
unit, made of Plexiglas, consists of a 0.05 m ID riser with a height of 2.6 m, a porous
distributor, a 90o bend, a cyclone system, a standpipe/downer and an L-shape non-
mechanical valve. The FCC particles (Geldart group A) with a mean diameter of 60
µm and a particle density of 1400 kg/m3 and air are used as the fluidized particles
and fluidizing gas. A porous plate with a pore size of 20 µm and a fractional free area
of 60% is used as the distributor of the CFB riser. The gas flow rate in the riser is
controlled by a flowmeter in the main gas line. Another flowmeter is used to control
the aeration gas flow rate at the bottom of the downer to provide different solids flux
in the CFB. A bend sensor and a cylindrical sensor are mounted at the exit region
and in riser in the CFB, respectively. Figure 2 is a photo of the real gas-solid
circulating fluidized bed mounted with the ECVT bend sensor and the cylindrical
sensor.
Gas outlet
Cyclone ECVT sensor II
Riser
Downer
ECVT sensor I
Gas
Distributor
Gas
Figure 1. Schematic diagram of the gas-solid circulating fluidized bed mounted with
ECVT sensors.
Figure 2. Photo of the real gas-solid circulating fluidized bed mounted with ECVT
bend sensors at the Ohio State University.
In an ECVT, a volume image of different phases in the test domain is reconstructed

based on utilizing nonlinear distributions of electric field lines. An ECVT system
consists of three basic components: (1) a capacitance sensor, (2) a data acquisition
system, and (3) a computer system for reconstruction and viewing. Figure 3 is a
schematic diagram of the ECVT system incorporating the three components. The
capacitance sensor is made of a number of capacitance electrodes, ne , distributed
around the peripheral of the domain of interest. Additionally, there are
ne ( ne − 1) / 2 combinations of independent capacitance measurements between all
pairs of electrode. The ECVT image reconstruction employed here is based on an
optimization reconstruction technique called the neural network multi-criterion
optimization image reconstruction technique (NN-MOIRT) (Warsito and Fan (16)).
The technique has also been extended to reconstruct volume images from 3D
capacitance sensors (Warsito et al. (11)). This extension increased the accuracy of
reconstructed images.
Recent developments have focused on the ECVT sensor design with 3D features for
detecting capacitance variations due to permittivity perturbations in the imaging
volume. For imaging complex geometries using ECVT, sensor design is the main
element of the imaging system to define the volume under interrogation. In this work,
two ECVT sensors are designed to image flows in the riser and the transition region
in the right-angle bend. The design of the cylindrical sensor is aimed at establishing
an electrically varied field around the riser by arranging 12 electrodes in three layers
as depicted in Figure 4 (a). The capacitance measurements are obtained between
the plates at each layer and between plates in different layers of the cylindrical
sensor to image the flow in the riser. The design of the bend sensor is also aimed at
establishing an electrically varied field at and around the corner of the bend by
arranging 12 electrodes in two layers perpendicular to each other as depicted in
Figure 4 (b). While the plates at each layer image the flow entering and exiting the
bend, it is the interaction between plates in both layers that most reveals the flow
dynamics in the region where the flow changes direction. The ECVT sensor design is
developed intuitively and confirmed by computer simulation (Marashdeh et al., 2008).
Simulations in this case confirmed the sensitivity distribution is focused at and
around the bend corner. The acquisition frequency is 80 Hz and the reconstruction
resolution is 20 × 20 × 20 for the three-dimensional reconstructed images of all tests.
Volume fraction as measured by ECVT is in the range of 2-5% of total volume. The
accuracy varies within this range depending on the flow structure and particles used
in flow. The assessment for the accuracy of ECVT images of a flow in a bend is
based on previous assessments of ECVT imaging accuracy in straight sections.
Figure 3. Schematic diagram of the ECVT system.
(a) (b)
Figure 4. Configuration of the ECVT sensors: (a) cylindrical sensor; (b) bend sensor.
Solids Holdup Distribution in the Riser
The cylindrical sensor is used for imaging real-time three-dimensional gas-solid flows
in the riser of the CFB. The volumetric solids holdup distribution in the sensor section
of the riser at varying superficial gas velocity and solids flux is obtained. The
instantaneous three-dimensional dynamic gas-solid flow structures in the riser are
analyzed based on quantitative ECVT images. Figure 5 shows the time-averaged
solids holdup distribution in the test region of the riser with superficial gas velocity, Ug,
from 0.97 m/s to 1.94 m/s and a solids flux, Gs, of 21.6 kg/m2s within 10 seconds.
The sub-image on the left in each image is the solids concentration distribution in the
X-Z (X, Y: two horizontal directions; Z: direction of the axis of the riser) whereas the
right sub-image represents the solids concentration distribution at the top, middle,
and bottom cross-sectional planes of the test region of the riser. Figure 6 shows the
time-averaged volume solids holdup in the riser at Gs=21.6 kg/m2s. The experimental
results indicate that the averaged volume solids holdup decreases with Ug. A
symmetric core-annulus structure with a low solids holdup in the core area and a
high solids holdup in the annulus area in the riser is observed. The thickness of the
annulus and solids holdup in the annulus near the wall decrease with Ug.
Figure 5. Time-averaged solids holdup distribution in the riser at Gs=21.6 kg/m2s: (a)
Ug=0.97 m/s; (b) Ug=1.16 m/s; (c) Ug=1.36 m/s; (d) Ug=1.55 m/s; (e) Ug=1.75 m/s; (f)
Ug=1.94 m/s.
0.3
Solids Holdup
0.2
0.1
0
0.5 1 1.5 2 2.5
U g (m/s)
Figure 6. Time-averaged solids volume holdup in the riser at Gs=21.6 kg/m2s.
Solids Holdup Distribution in the Bend
The bend-sensor is used for imaging real-time three-dimensional gas-solid flows at

the exit region of the CFB riser. The volumetric solids holdup distribution in the exit
region of the CFB riser at varying superficial gas velocity and solids flux is probed.
The three-dimensional solids holdup distributions in the bend of the riser are
illustrated by slices in the volume image cut through the bend vertically and
horizontally. The configurations of the vertical and horizontal slices are given in
Figure 7. Figure 8 shows the solids holdup distribution in the bend of the riser with Ug
of 1.36 m/s and Gs of 21.2 kg/m2s. The images indicate that a core-annulus flow
structure is formed both in the vertical and horizontal parts of the bend. The solids
holdup in the core region is relatively low compared to that in the annulus region. The
annulus structure is non-centro-symmetric in the horizontal part of the bend (Grace,
et al. (17)). The asymmetry of the solids volume fraction in the bend is due to the exit
at one side and the tortuosity of the flow path at entrance of the cyclone. The solids
holdup in the annulus near the top wall area in the bend is higher than that in other
locations of the annulus. The asymmetry is due to the following reasons: (1) back
mixing and reflection of solids from the upper wall of the horizontal duct; (2) solids in
the bend are difficult to entrain with the gas flow due to an abrupt turn of the gas
stream in the bend; (3) a zone with low gas velocities at the upper corner of the bend
is formed. The images also indicate that a solids “dune” is formed, at the bottom of
the horizontal section of the bend. The sedimentation of solids in the horizontal duct
is due to: (1) the velocity of the main gas stream is not high enough to carry all the
solids horizontally to the cyclone, and thus the sedimentation of solids occurs; (2)
after an abrupt turn in the bend, the gas moves towards the top of the horizontal duct
in the bend, which forms a zone with relatively low gas flow rate at the bottom of the
horizontal duct. Figure 9 shows the solids holdup distribution in the bend of the riser
with Ug of 1.16 m/s and Gs of 21.2 kg/m2s. The comparison between Figures 8 and 9
indicates that the solids holdup near the top wall area in the bend increases with the
superficial gas velocity. More solids move to the outside wall area from the main
stream in the bend due to high solids velocity at high superficial gas velocity. Figure
10 shows the time-averaged volume solids holdup in the bend at a superficial gas
velocity of 1.16 m/s. The experimental results indicate that the time-averaged volume
solids holdup near the top wall area increases with solids flux. More solids are
separated to the outside of the bend from the main stream of the gas-solid flow at
high solids flux in the CFB.
(a) (b)
Figure 7. Configuration of the slices for the plots of the tomographic images in the
bend: (a) vertical slices; (b) horizontal slices.
(a) (b)
Figure 8. Solids holdup distribution in the bend of the CFB riser at Ug=1.36 m/s and
Gs=21.2 kg/m2s: (a) vertical slices; (b) horizontal slices.
(a) (b)
Figure 9. Solids holdup distribution in the bend of the CFB riser at Ug=1.16 m/s and
Gs=21.2 kg/m2s: (a) vertical slices; (b) horizontal slices.
0.08
0.07
εs
0.06
0.05
18 20 22
2
G s (kg/m s)
Figure 10. Time-averaged volume solids holdup at the top wall region at the start of
the horizontal duct of the bend at Ug=1.16 m/s.
CONCLUSIONS
An advanced ECVT sensor system is designed for real-time, three-dimensional

imaging of gas-solid flows in a riser and a 90o bend at the exit region of a CFB. The
instantaneous 3-D dynamic gas-solid flow structures in the riser and the bend are
analyzed based on quantitative ECVT images. A symmetric core-annulus structure in
the riser is observed. It is found that the thickness of the annulus and solids holdup in
the annulus near the wall of the riser decrease with Ug. A core-annulus flow structure
is formed both in the vertical and horizontal parts of the bend. The annulus structure
is non-centro-symmetric in the horizontal part of the bend. The solids holdup in the
annulus near the top wall area in the bend is higher than that in other locations of the
annulus. A solids “dune” is observed by ECVT at the bottom of the horizontal duct of
the bend. The solids holdup at the top wall region in the bend increases with the
superficial gas velocity. The time-averaged volume solids holdup near the top wall
area increases with the solids flux.
ACKNOWLEDGEMENTS
The support of the US Department of Energy DOE/NETL under Grant # DE-

NT0005654 and Tech4Imaging is greatly appreciated. The CFB design adopted in
this work is similar to the one employed by Professor Lynn Gladden’s research group
at University of Cambridge, with whom collaborative research efforts on tomography
techniques are in progress. The assistance of Mr. Paul Green and Mr. Leigh Evrard
in the fabrication of the circulating fluidized bed, Mr. Mustafa Mergaye in the
fabrication of the sensor, and Mr. Samuel Bayham and Mr. Aining Wang in the
operation of the circulating fluidized bed is gratefully acknowledged.
NOTATION
Gs solids flux (kg/m2s)

ne number of capacitance electrodes
Ug superficial gas velocity (m/s)
Greek letters
εs solids holdup
REFERENCES
1. Kunii, D. & Levenspiel, O. Fluidization engineering, second ed. Butterworth-

Heinemann, Boston (1991)
2. Fan, L.-S. & Zhu, C. Principles of Gas-Solid Flows. Cambridge University
Press, Cambridge (1998)
3. Lanneau, K. P. Gas-solids contacting in fluidized beds. Transactions of the
Institution of Chemical Engineers, 38(3), 125-43 (1960)
4. Geldart, D. & Kelsey, J. R. The use of capacitance probes in gas fluidised
beds. Powder Technol., 6(1), 45 – 50 (1972)
5. Yasui, G. & Johanson, L. N. Characteristics of gas pockets in fluidized beds.
Am. Inst. Chem. Engrs J., 4, 445 – 452 (1958)
6. Cui, H. & Chaouki, J. Effects of temperature on local two-phase flow structure
in bubbling and turbulent fluidized beds of FCC particles. Chem. Eng. Sci.,
59(16), 3413-3422 (2004)
7. Peters, M. H.; Fan, L.-S.; and Sweeney, T. L. Study of particle ejections in the
freeboard region of a fluidized bed with an image carrying probe. Chem. Eng.
Sci., 38(3), 481-485 (1983)
8. Du, B.; Warsito, W.; and Fan, L.-S. ECT Studies of the Choking Phenomenon
in a Gas–Solid Circulating Fluidized Bed. AIChE Journal, 50(7) 1386 – 1406
(2004)
9. Kang, W. K.; Sutherland, J. P.; and Osberg, G. L. Pressure fluctuations in a
fluidized bed with and without screen cylindrical packings. Ind. & Eng. Chem.
Fund., 6(4), 499-504 (1967)
10. Geldart, D. & Xie, H. Y. The use of pressure probes in fluidized beds of group
A powders. Fluid. VII, Proc. Eng. Found. Conf. Fluid. 749-756 (1992)
11. Warsito, W.; Marashdeh, Q.; Fan, L.-S. Electrical Capacitance Volume
Tomography (ECVT). IEEE Sens. J., 7, 525-535 (2007)
12. Marashdeh, Q.; Fan, L.-S.; Du, B.; Warsito, W. Electrical Capacitance
Tomography-A Perspective. Ind. Eng. Chem. Res., 47, 3708-3719 (2008)
13. Wang, F.; Marashdeh, Q.; Fan, L.-S.; Williams, R. A. Electrical capacitance,
electrical resistance, and position emission tomography techniques and their
applications in multi-phase flow systems, in: Li, J. H.(Ed.), Advances in
Chemical Engineering Vol. 37: Characterization of flow, particles, and
interfaces. Academic Press, Amsterdam, 179-222 (2009)
14. Wang, F.; Yu, Z.; Marashdeh, Q.; Fan, L. -S. Horizontal Gas and Gas/Solid
Jet Penetration in a Gas-Solid Fluidized Bed, Chemical Engineering Science,
In Press (2010), doi:10.1016/j.ces.2010.02.036
15. Wang, F.; Marashdeh, Q.; Fan, L.-S.; Warsito, W., Electrical Capacitance
Volume Tomography: Design and Applications. Sensors, 10, 1890-1917
(2010)
16. Warsito, W. & Fan, L.-S. Neural network based multi-criterion optimization
image reconstruction technique for imaging two- and three-phase flow
systems using electrical capacitance tomography. Meas. Sci. Technol., 12,
2198–2210 (2001)
17. Grace, J. R.; Bi, X. T.; Golriz, M. Circulating Fluidized Beds in: Yang, W.-C.
(Ed.), Handbook of Fluidization and Fluid-Particle Systems. Marcel Dekker,
Inc. New York, NY, 485-544 (2003)
THE RELATIONSHIP BETWEEN FLUIDIZATION VELOCITY
AND SEGREGATION IN TWO-COMPONENT FLUIDIZED
BEDS: A PRELIMINARY ANALYSIS
Brunello Formisani, Rossella Girimonte and Vincenzino Vivacqua

Dipartimento di Ingegneria Chimica e dei Materiali, Università della Calabria,
I 87030 Arcavacata di Rende (Cosenza), Italy
ABSTRACT
Experiments are presented that provide the initial and final fluidization velocity of
binary mixtures at varying composition. Introducing just one parameter to account
for their segregation level, the theoretical equations of the two characteristic
velocities are derived. These equations are then employed to predict the
concentration profile obtained by slowly defluidizing the bed down to the fixed state.
INTRODUCTION
In many industrial processes in which fluidized beds are employed (combustion and
gasification of coal and biomass, polymerization, etc.), solids of various kinds are
simultaneously subjected to fluidization. During the process, gas-solid and
solid-solid interaction determines the tendency of system components to segregate
or mix up so as to give place to a characteristic axial concentration profile.
Segregation phenomena may lead, in some cases, to strong inhomogeneities or
even to partial defluidization of the bed with detrimental effects on process
performance.
In spite of the huge number of experimental studies published in the last three
decades, even for mixtures of only two components the relationship between
fluidization regime and level of segregation is still poorly understood, so that no
reliable quantitative theory of segregating fluidization is, to date, available. Attempts
made to refer the state of mixing of a binary bed to the characteristics of its
fluidization regime have led to a few relationships, mostly empirical. To this regard, a
well-known equation is that proposed by Nienow et al. (1), valid for two-density
mixtures and flotsam-rich systems, which expresses the variation with the
fluidization velocity of a component mixing index defined by the authors as the ratio
between the jetsam concentration in the upper region of the bed and its overall
value. Modified versions of this equation, meant to extend its validity to two-size
mixtures and to improve its accuracy, were proposed by Rice and Brainovich (2),
Peeler and Huang (3) and Wu and Baeyens (4). All these works make use of the
“minimum fluidization velocity of the mixture” umf and correlate the degree of bed
mixing to the “excess gas velocity” u−u mf. However, the concept of umf, taken from
the theory of monosolid fluidization, has no meaning when applied to the suspension
process of a binary bed, because of the gradual nature of the phenomenon (5,6).
This paper, instead, develops a novel approach, based on definition of the “initial”
and “final fluidization velocity” of the binary mixture. As shown by previous studies
(5-8), in a ∆p versus u diagram uif is determined where the pressure drop first
deviates from the fixed bed curve, uff where it attains its final value. Introduction of
these two characteristic velocities is suggested by the actual phenomenology of the
fluidization process, analysed in detail elsewhere (5,6). The mechanism of binary
fluidization is here summarized in Fig.1.
Fig.1 - Fluidization mechanism of a homogeneous bed of two solids.
THEORY
Any bed of two solids homogeneously mixed (Fig.1a) achieves suspension

gradually, while the axial distribution of its components changes along with the
increase of the fluidizing gas velocity. The process begins at uif, whose calculation
can be accomplished by a fully predictive equation devised in a previous stage of
the research (5,6):
180 µ g u if (1 − ε mf ,m )
2
d av2 ε mf
3
[ ]
= (ρ f − ρ g )x f 0 + (ρ j − ρ g )(1 − x f 0 ) (1 − ε mf ,m )g (1)
,m
In it, dav is the Sauter mean diameter, calculated from
1 x f 0 1− x f 0
= + (2)
d av df dj
while the value of bed voidage is drawn from the experimental curve of εmf,m versus
xf.
At any operating velocity intermediate to uif and uff the axial distribution of mixture
components is approximately that sketched in Fig.1b. The bed consists of a top
flotsam layer, a middle jetsam stratum and a residual homogeneous portion whose
heights are indicated as hf ,hj and hm, respectively. As the flotsam layer results
fluidized since the beginning of its buildup at uif, a force balance between the total
drag force and the buoyant weight in the remaining two layers provides the following
expression relating uff (Fig.1c) to the properties of the two solids, the mixture
voidage and the level of segregation corresponding to the height hm of the static
mixed layer:
u ff =
[(ρ f − ρ g )x f 0 hm + (ρ j − ρ g )(1 − x f 0 )h0 g ] (3)
 (1 − ε mf ,m ) (1 − ε mf , j ) 
180 µ g  3 + ( − )( − )
(
 ε mf ,m d av
2
hm
) (
ε mf3 , j d 2j
h0
) hm 1 x f 0

In order to make eqn (3) deterministic, it is necessary to fix the value of the
parameter hm. In the absence of a fundamental theory, the following correlation has
been devised for hm,ff, that is at the final fluidization velocity, capable to give
accurate predictions (9):
(1 − ε ) ε 3
x f 0 (1 − x f 0 )
hm , ff
=k
mf , m mf , j
(4)
h0 (1 − ε ) ε mf , j
3
mf , m
Eqn (4) relates the height of the residual homogeneous layer to mixture composition
and to the gain in drag force effectiveness provided by the void condition typical of
the mixed state. In it, k is a best fit parameter which does not depend on
composition.
For a two-density mixture, assuming the invariance of voidage with composition, uff
calculated from eqn (3) turns out to be equal to the velocity obtained by substituting
in eqn (1) the value of the flotsam fraction in the system made of the jetsam and the
mixed layer, of height hj and hm respectively:
x f 0 (hm , ff h0 )
x fb = (5)
x f 0 (hm , ff h0 ) + 1 − x f 0
The correspondence between the value of uif evaluated at xfb and that of uff
calculated at the overall concentration xf0, exact for density segregating beds, is well
approximated also for two-size systems.
Given that uff does not depend on the initial state of mixing of the two solids (5), xfb
may be also considered as the concentration of the first thin layer that settles down
during the defluidizing procedure; eqn (5) can hence be regarded as a phase
equilibrium relationship, where h0/hm,ff=α plays a role analogous to that of the
relative volatility in gas-liquid equilibrium, in a way that:
α ⋅ x fb
xf0 = (6)
α ⋅ x fb + (1 − x fb )
When a packed portion of the bed is still present and the defluidization front has
reached the height z, the average flotsam fraction in the overlying fluidized region is:
∫ (1 − ε )x
H
mf f dz
yf = z
(7)
∫ (1 − ε )dz
H
mf
z
ӯ f can now be linked to xf, i.e. the flotsam fraction of the thin layer which settles
down by slightly decreasing the gas flow rate; the way to relate these two variables
is suggested by eqn (6): xf0 is substituted with ӯ and xf with xfb, so that
α ⋅ xf
yf = (8)
α ⋅ x f + (1 − x f )
Under the assumption of constant voidage (H=h0),

a simplification that introduces a negligible error:
[ ]
x f dz = −d (h0 − z ) ⋅ y f = −(h0 − z )d y f + y f dz (9)
Introducing the dimensionless height Z=z/h0 and

considering that
Fig. 2 - Sketch of the

d yf dx f dy f
defluidization process. = (10)
dZ dZ dx f
eqn (9) gives rise to the first order differential equation:
dx f 1 yf − xf
= (11)
dZ (1 − Z ) ∂ y f ∂x f
From eqn (7) it is then obtained:
1 (x f + α )(1 − x f )2
dx f
=
dZ (1 − Z ) α 2 −1 [ ] (12)
Once integrated with the condition Z=0, xf=xfb, eqn (12) allows calculating the axial
profile of xf as:
α
 1 − x f   1 − x fb  α −1  αx f + 1 − x f   αx fb + 1 − x fb 
Z = 1 −        
 x fb   1 − x f
(13)
 x f    1− x 
      fb 
EXPERIMENTAL
All the experiments of this study were carried out in a transparent fluidization column
of 10 cm ID, equipped with a plastic porous distributor 4 mm thick. The pressure
drop across the column was measured by means of a U-tube water manometer
connected to a tap located 1 mm above the distributor plane. Bed heights were
evaluated by averaging the values read on three graduated scales put at 120°C
around the column wall, and then used for determining bed void fractions.
The concentration profiles were obtained by gently drawing the solids from the top
of the column by means of a vacuum device, in horizontal layers of particles
generally 2 cm thick (or 1 cm thick, when a higher resolution was needed). Each of
these layers was then sieved to measure the mass fraction of either solid
component by weighing. Concentration values were then referred to the average
height of the relevant layers and used to trace the respective profiles in function of
height.
Measurements involved mixtures of various spherical solids, closely sieved. The
properties of each cut are reported in Table 1, together with those of the mixtures
investigated. In all the experiments the aspect ratio h0/D of the fixed bed was 1.7.
Tab.1 – Properties of the experimental solids and mixtures
Density Sieve size Sauter mean diameter

Solid
[g/cm3] [µm] [µm]
500-710 593
Glass ballotini (GB) 2.48 450-600 499
150-180 172
Ceramics 3.76 500-710 605
Type ρj/ρf dj/df εmf k

Mixture
[-] [-] [-] [-]
Density-segregating CE605-GB593 1.52 1.02 0.405 0.39
Size-segregating GB499-GB172 1 2.90 See Fig.1 0.18
VALIDATION
As a major difference with the case of two-density mixtures, the binary beds in which
a significant difference of component diameters is present exhibit a voidage which
varies with their composition (6,7). Thus, for the system CE605-GB593 εmf,m can be
assumed as practically constant with xf, and an average values of 0.405 was used.
As regards instead the mixture GB499-GB172, εmf,m varies with xf according to the
experimental curve of Fig.2.
0.5
εmf,m [ - ]
0.4
0.3
0.0 0.2 0.4 0.6 0.8 1.0
xf , [ - ]
Fig.2 - Voidage of the homogeneous mixtures GB499-GB172 at varying

composition.
In Fig. 3 are shown the velocity diagrams of the two systems investigated. Model
curves for uif are generated by the theoretical eqn (1), wheras uff is predicted from
eqns (3) and (4), using the values of k reported in Table 1. The errors do not exceed
10% for both the density- and the size-segregating mixture.
60 40
50
GB499-GB172
30
uif uff
u if , u ff , [ cm/s ]
u if , u ff , [ cm/s ]
40
30 20
CE605-GB593
20
uif uff 10
10
0 0
0 0.2 0.4 0.6 0.8 1 0 0.2 0.4 0.6 0.8 1
xf , [ - ] xf , [ - ]
Fig.3 - Fluidization velocity diagrams of the homogeneous mixtures CE605-GB593

(density-segregating) and GB499-GB172 (size-segregating).
CE605-GB593 GB499-GB172
1 1
xf0=0.1 xf0=0.2
0.8 0.8
xf0=0.4
0.6 0.6 xf0=0.5
Z, [-]
Z, [-]
0.4 0.4
0.2 xf0=0.9 0.2 xf0=0.8
0 0
0 0.2 0.4 0.6 0.8 1 0 0.2 0.4 0.6 0.8 1
xf, [-] xf, [-]
Fig.4 - Concentration profile of the fixed bed obtained by a slow defluidizing

procedure at varying flotsam total concentration for the mixtures CE605-GB593 and
GB499-GB172.
By introducing into eqn (4) the values of k used to correlate the velocity data, it is
possible to calculate hm,ff at a given overall concentration and, thanks to eqn (6), the
corresponding value of xfb. Finally, the concentration profile of the fixed bed obtained
after slow defluidization of the mixture is found by eqn (12). Model curves and
experimental points are compared in Figs 4 for the two different types of mixtures
under examination, over the whole field of system composition.
Although the agreement is not always satisfactory from the quantitative point of
view, the model seems capable to reproduce the general trend of the component
composition profiles. While confirming the potentiality of the approach followed,
these preliminary results encourage the effort of addressing segregating
phenomena occurring in multisolid systems in the light of the fundamental theory of
fluidization.
CONCLUSIONS
Results relevant to mixtures subjected to segregation by difference of either density

or size between their components show that a unique theory based on fundamental
analysis proves capable to relate the progress of fluidization to the extent of
segregation.
The model equations proposed in this paper successfully reproduce the effects of
segregation by means of a parameter whose determination can be carried out with
minimal experimental effort, by a single fluidization experiment.
In the prediction of the final fluidization velocity of a two-solid mixture, an important
role is played by the fact that the force balance is applied to a realistic picture, even
when some evident simplifications are introduced. The difference uff-uif, i.e. the width
of the fluidization velocity interval of the binary bed, seems related to the
concentration profile obtained from its slow defluidization down to the fixed state.
NOTATION
A column cross section [cm2] z axial coordinate [cm]

D column bed diameter [cm] Z dimensionless height z/h0 [-]
d particle diameter [µm]
dav Sauter mean diameter (eqn.4) εmf minimum fluidization voidage [-]
[µm] ε0 fixed bed voidage [-]
g gravity acceleration [cm/s2] µg gas viscosity [g/cm s]
H total bed height [cm] ρ solid density [g/cm3]
h0 height of the fixed bed [cm] ρg gas density [g/cm3]
k best-fit parameter (eqn. 17) [-]
uif, uff initial, final fluidization velocity
[cm/s] Subscripts
umf minimum fluidization velocity
[cm/s] f,j of the flotsam, jetsam
xf solid fraction of flotsam [-] component (or layer)
xf0 overall solid fraction of flotsam m of the homogeneous mixture
[-] ff at the final fluidization
ӯ average flotsam fraction of the conditions.
fluidized portion of the bed [-]
REFERENCES
1) Nienow, A.W., Rowe, P.N. and Cheung, L.Y.L. (1978). A quantitative analysis of
the mixing of two segregating powders of different density in a gas-fluidized bed,
Powder Technol., 20, 89–97.
2) Rice, R.W. and Brainnovich, Jr J.F. (1986). Mixing/segregation in two- and
three-dimensional fluidized beds: binary systems of equidensity spherical
particles, A.I.Ch.E J., 32, 7–16.
3) Peeler, J.P.K. and Huang, J.R. (1989). Segregation of wide size range particle
mixtures in fluidized beds, Chem. Eng. Sci., 44, 1113–1119.
4) Wu, S. Y. and Baeyens, J. (1998). Segregation by size difference in gas
fluidized beds, Powder Technol., 98, 139-150.
5) Formisani, B., Girimonte, R. and Longo, T. (2009). The fluidization process of
binary mixtures of solids: Development of the approach based on the fluidization
velocity interval, Powder Technol., 185, 97-108.
6) Formisani, B., Girimonte, R. and Longo, T. (2008). The fluidization pattern of
density-segregating binary mixtures. Chem. Eng. Res. Des., 86, 344-348.
7) Chen, J. L.-P. and Keairns, D. L. (1975). Particle segregation in a fluidized bed,
Can. J. Chem. Eng., 53, 395-402.
8) Vaid, R. P. and Sen Gupta P. (1978). Minimum fluidization velocities in beds of
mixed solids, Can. J. Chem. Eng., 56, 292-296.
9) Formisani, B., Girimonte, R. and Vivacqua, V. (2010). Fluidization of mixtures of
two solids differing in density or size, AIChE J., (in press, DOI:
10.1002/aic.12450).
THE VARIATION OF THE BUBBLE PHASE PROPERTIES
OF A FCC CATALYST FLUIDIZED BED
AT HIGH TEMPERATURE
Rossella Girimonte and Brunello Formisani

Dipartimento di Ingegneria Chimica e dei Materiali, Università della Calabria,
I 87036 Arcavacata di Rende (Cosenza), Italy
T: +39-0984-496689; F: +39-0984-496655; E: rossella.girimonte@unical.it
ABSTRACT
Some important characteristics of the bubbling regime, relevant to a cut of FCC

catalyst with an average size of 110 µm were investigated at 100, 400 and 700 °C.
This was achieved by imploying data of bed collapse tests as well as images of the
bubble eruption at the free surface of the bed by varying fluidization velocities and
bed aspect ratios. The results show that a smoother regime of fluidization is
observed at superambient temperature.
INTRODUCTION
Industrial fluidized bed units are often operated in the bubbling regime at high
temperatures, like in the case of catalytic reactors, combustors or gasifiers. In spite
of that, current descriptions of their hydrodynamics are still widely based on the
results of investigations carried out at room conditions.
Very little is known, therefore, on the specific relationship that links operating
temperature and general properties of the bubbling regime of a fluidized bed, a lack
of information also connected to the difficulty of producing experimental data by
affordable diagnostic techniques. A noticeable uncertainty exists, for instance, on
the nature and the behaviour of the bubble phase at elevated temperatures, as
bubbles flow across a particulate phase whose properties are definitely influenced
by temperature, T.
Literature studies have reported so far some contradictory results, possibly due to
the frequent use of intrusive techniques or to the adoption of indirect measurements.
With beds of Geldart B particles in the temperature range 20-300°C, Geldart and
Kapoor (1) observed that the diameter of bubbles, measured at their eruption,
decreased by 15-25%. Sitthiphong et al. (2) reported opposite results for beds of
larger particles. Stubington et al. (3), who used a three-dimensional resistivity probe,
determined bubble sizes in a coal bed at temperatures ranging from 20 to 1000°C:
the equivalent sphere diameter exhibited a 5-15% reduction as T was raised from
ambient level to about 300°C. Sishtla et al. (4 ) used pressure probes to determine
bubble frequency, velocity and size in fluidized beds of solids of various particle size
(100-400 µm) and density (1.25-2.56 g/cm3) at temperatures up to 980°C. They
reported that the average pierced length of bubbles, as well as their frequency and
velocity, did not change with T.
Hatate et al. (5), who analysed the behaviour of cuts of sand in the range
75-521 µm, found that the effect of temperature on the properties of the bubble
phase was significant only for fine particles. With coarser solids, instead, the
dependence of the equivalent bubble diameter on variables such as bed height and
excess gas velocity did not differ from that observed at ambient conditions. Llop et
al. (6) investigated the influence of temperature on bubble hold-up in beds of
particles of Geldart’s groups B and D. With the former type of solids, the bubble
fraction was found to diminish as T increased, whereas an opposite trend was
obtained with D particles.
Contradictory results were obtained by Cui and Chaouki (7), whose measurements
were carried out by an optical fiber probe immersed in the fluidized bed. They
reported that both the frequency of the cycle and the ratio of the dilute/dense phase
duration were enhanced by high temperature, with the consequent increase of
bubble frequency and size. On this basis, their questionable conclusion was that at
elevated temperatures the fluidization behaviour of a solid like FCC catalyst, which
belongs to Geldart's group A, becomes that typical of B particles.
Given the relative inconsistency of the few studies that have tried to characterize the
bubble regime at high temperature, the main aim of the present study is that of
providing some clear result by non-invasive measurements based on image
analysis.
EXPERIMENTAL
The present investigation addresses the influence of temperature on the overall

properties of the bubble phase as well as on some characteristic of the individual
bubbles erupting at the free surface of the bed. Bed collapse tests and
video-recording of bubble eruption at the free surface of the bed were carried out in
a transparent column (ID=90mm). In either case, image analysis procedures were
used. Both techniques were applied at different values of fluidization velocity, bed
aspect ratio and temperature.
Each collapse test provides a diagram of bed height versus time capable of
describing the bed deaeration process that follows the instantaneous interruption of
gas feed. From it, several parameters are determined: the dense phase voidage εd,
the average velocity ud of the gas flowing through it, the volumetric bubble fraction δ
(otherwise termed "bubble hold-up"), and the average gas velocity in the bubble
phase, ub.
At the same operating conditions, images of the upflowing bubbles as they reach the
free surface of the fluidized bed, were recorded and processed to determine the
bubble frequency fb, and the distribution of their diameters at eruption; from these
data, the average bubble diameter db,av was also evaluated.
The present investigation was focused on a specific system, i.e. a cut of FCC
catalyst fluidized by air. Solid density was 1600 kg/m3; the average particle diameter
was 110 µm and fines were practically absent (F22=0 and F45=0.02). The estimated
value of particle sphericity, equal to 0.99, was assumed as that capable to give the
best fit of data of minimum fluidization velocity at ambient conditions. This
assumption was confirmed by SEM analysis, that showed that the catalyst particles
were substantially spherical. The experiments were carried out at 100, 400 and 700
°C. The fluidization velocity was set equal to 1.6, 2.1, 2.7, 3.2, 4.2 and 5.3 cm/s, with
corresponding values of the excess velocity equal to 1.1, 1.6, 2.1, 2.7, 3.7 and 4.8
cm/s respectively. Given that the minimum fluidization velocity is nearly independent
of temperature, the same is true for u-umf in the field 100-700°C. At each
experimental temperature, the bed aspect ratio H0/D of the particle bed was fixed at
values of 3, 3.8 and 4.6.
500
H0/D=4.6 H0/D=4.6 H0/D=4.6
400
H0/D=3.8 H0/D=3.8 H0/D=3.8
H , [mm]
300 H0/D=3 H0/D=3 H0/D=3
FCC 110 µm FCC 110 µm FCC 110 µm

T=100°C u-u mf=4.8 cm/s T=400°C u-u mf=4.8 cm/s T=700°C u-u mf=4.8 cm/s
200
0 1 2 3 4 0 1 2 3 4 0 1 2 3 4
t , [s] t , [s] t , [s]
Figure 1. FCC catalyst collapse curves at varying H0/D and T; u-umf=4.8 cm/s.
RESULTS
Bed collapse experiments show that the expansion of the dense phase of the
fluidized bed past incipient fluidization is independent of bed height (see Fig. 1) and
that at relatively high gas velocity (above 4 cm/s) the dense phase properties
become insensitive to further increases of the fluidization velocity (see Figs 2 and 3).
0.7
T=400°C umb,e=umb,s T=700°C
T=100°C
0.6
umb,e ε
umb,e
ε
ε , εd ,[-]
0.5
ε
εd
εd
0.4
εd umb,s
umf
umf u umf
mb,s
0.3
0 2 4 6 8 0 2 4 6 8 0 2 4 6 8
u , [cm/s] u , [cm/s] u , [cm/s]
Figure 2. FCC catalyst fluidization maps at varying temperature.

As illustrated by the fluidization maps in Fig. 2, at T=100 and 400°C the transition to
the bubbling regime occurs with a contraction of the dense phase voidage whereas
at 700°C the high level of voidage attained by the dense phase of the bed becomes
stable. After the commencement of bubbling the properties of the particulate phase
apparently depend only on operating temperature and their trends of variation are
different from those of the corresponding minimum fluidization parameters (see
Fig. 3): the dense phase voidage εd is constantly higher than εmf and the interstitial
gas flows at a velocity ud higher than umf.
0.6 2.5
u-umf=2.7 cm/s u-umf=2.7 cm/s FCC 110 µm
u-umf=3.7 cm/s u-umf=3.7 cm/s
2
0.5
u d , [cm/s]
1.5
εd , [-]
1
0.4
0.5
εmf FCC 110 µm
umf
0.3 0
0 200 400 600 800 0 200 400 600 800
T , [°C ] T , [°C ]
Figure 3. Dense phase properties at varying temperature.
These results confirm that with solids of Geldart’s Group A, application of the
two-phase theory to the behaviour of the fluidized bed should account for the fact
that the actual excess gas velocity u-ud is significantly different from u-umf. Thus,
running experiments at constant u-umf corresponds to working with u-ud that
increases with T. The dense phase porosity is constantly higher than that of the bed
at incipient fluidization, but the properties of the particle emulsion noticeably change
over 400°C, a thermal level past which any further growth of εd is accompanied by
the progressive diminution of the gas velocity through the emulsion phase. As this
should cause a remarkable increase of the excess gas flowing in the form of
bubbles, it is expected that the bubble phase characteristics vary accordingly.
To this regard, Fig. 4 illustrates the variation of the hold-up of bubbles as function of
the excess velocity at different values of temperature and of the bed aspect ratio
H0/D. The volume fraction of bubbles strongly increases over 400°C. Over this
temperature thermally induced interparticle forces are likely to be much stronger, as
shown by the corresponding fluidization map of Fig. 2 where εd is much higher than
at lower T. The increase of interparticle cohesion may thus be thought to stabilize
the dense phase structure, so that the same excess gas is converted into a more
abundant bubbly flow.
As for the effect of changing the bed aspect ratio, its increase is associated to a
reduction of the volumetric extension of the bubble phase. As this occurs without the
excess flow rate being varied, increasing the bed height appears to give place to a
different partition of the total gas flow rate into the two phases.
0.1 0.1
100 °C FCC 110 µm H0/D FCC 110 µm
400 °C H0/D=4.6 3.0 T=400°C
0.08 700 °C 0.08 3.8
4.6
0.06 0.06
δ, [-]
δ, [-]
0.04 0.04
0.02 0.02
0 0
0 2 4 6 8 10 0 2 4 6 8 10
(u-u d ) , [cm/s] (u-u d ) , [cm/s]
Figure 4. Bubble hold-up versus excess gas velocity at varying T and H0/D.
Measurements of the average velocity of the bubble phase confirm that temperature
has an influence on this parameter: the velocity reduction observed at high T (see
Fig. 5) indicates that the flow section of bubbles becomes larger (consistently with
the correspondent growth of δ). Similarly, the increase of ub at large values of H0/D
is coherent with the parallel decrease of bubble hold-up already shown in Fig. 4.
300 300
FCC 110 µm FCC 110 µm
H0/D=4.6 u-umf=4.8 cm/s
200 200
u b , [cm/s]
u b , [cm/s]
100 u-umf=1.6 cm/s 100

H0/D
u-umf=2.7 cm/s 3.0
u-umf=3.7 cm/s 3.8
u-umf=4.8 cm/s 4.6
0 0
0 200 400 600 800 0 200 400 600 800
T , [°C ] T , [°C ]
Figure 5. Average bubble phase velocity in function of temperature.
In order to confirm this hypothesis, the images of bubbles erupting at the free
surface of the bed were recorded. It has to be mentioned that the analysis could not
be conducted at all the operating velocities employed for running the collapse
experiments, due to the excessive turbulence encountered at high velocities.
Observations are thus limited to the lower bound of the velocity field, namely to
values of u=1.6 and 2.1 cm/s (i.e. u-umf=1.1 and 1.6 cm/s, respectively). The
eruption diameters were calculated by converting the surface limited by bubble
perimeter into that of an equivalent circle and the diagrams of their distribution
reconstructed at varying operating conditions.
100
H0/D=3.0 u-umf=1.6 cm/s H0/D=3.8 u-umf=1.6 cm/s H0/D=4.6 u-umf=1.6 cm/s
80
T °C T °C T °C
100 100 100
60 400 400 400
Nb , [%]
700 700 700

40
20
0
0 1 2 3 4 5 6 7 0 1 2 3 4 5 6 7 0 1 2 3 4 5 6 7
d b , [cm] d b , [cm] d b , [cm]
Figure 6. Distribution of bubble eruption diameters at varying H0/D and T.
This procedure allows stating that the distribution of bubble diameters depends on
the bed aspect ratio as well as on temperature (see Fig. 6), a result consistent with
those previously provided by the bed collapse experiments. The two series relevant
to different superficial velocity appears quite similar, then only data for
u-umf=1.6 cm/s are shown. At any temperature level increasing the bed height has
no significant influence on the amplitude of bubble size distribution but causes the
increase of the average diameter of the bubbles, possibly due to the enhanced role
played by coalescence.
At any given bed height, on the other hand, raising the process temperature lowers
both limits of the bubble size distribution while also their average diameter is
reduced. Such effects constitute an indirect confirmation of the fact that high
temperature changes the nature of the dense phase of the bed, making bubbles flow
through a medium characterized by an increasingly cohesive behaviour.
6 8
FCC 110 µm FCC 110 µm
6
4
db,av , [cm]
fb , [1/s]
2
H0/D 2 H0/D
3.0 3.0
3.8 3.8
4.6 4.6
0 0
0 200 400 600 800 0 200 400 600 800
T , [°C ] T , [°C ]
Figure 7. Average bubble diameter and bubble frequency in function of T.
The two plots of Fig. 7 show the variation with T of the properties of the bubbles that
flow across the bed, at a fixed value of the excess velocity. It is observed that their
average diameter reduces as much as the operating temperature is raised while
their frequency of eruption accordingly increases; these seem two clear findings in a
field where literature results are few and rather controversial.
Altogether the results presented so far clearly indicate that temperature plays a key
role in determining the characteristics of the bubbling regime in that it changes the
properties of the two phases of the fluidized system.
CONCLUSIONS
Measurements conducted in a fluidized bed of FCC catalyst operating at high

temperature show that temperature influences the quality of bubbling. The results
provided by the bed collapse technique indicate that bubble hold-up increases in
response to the temperature increase as a consequence of the decrease in the gas
velocity through the dense phase. Connected to that is the fact that the average gas
velocity in the bubble phase decreases with T, while bubble diameters, as
determined by image analysis at their eruption, become smaller. Such phenomena,
more easily recognizable over 400°C and influenced also by bed height, are
associated to the tendency of the dense phase of the bed to become increasingly
cohesive due to thermally induced interparticles forces (7, 8).
On the whole, the different quality of the bubbling regime at high temperature, with a
larger number of smaller bubbles travelling across a more permeable particulate
phase, makes clear that substantial corrections have to be introduced in modelling
the performance of fluidized bed reactors characterized by significant thermal
effects.
ACKNOWLEDGEMENT
This work was financially supported by the University of Calabria.
NOTATION
db Bubble eruption diameter, cm

db,av Average bubble eruption diameter, cm
fb Bubble frequency, -
F22 Fine fraction under 22 µm, -
F45 Fine fraction under 45 µm, -
H Fluidized bed height, mm
H0 Static bed height, mm
D Column diameter, mm
H0/D Bed aspect ratio, -
Nb Bubble fraction, %
t Time, s
T Temperature, °C
u Superficial velocity, cm/s
ub Bubble phase velocity [=(u-ud)/δ], cm/s
ud Emulsion phase velocity, cm/s
umb,e Maximum velocity of homogeneous expansion, cm/s
umb,s Minimum velocity of a stable bubbling regime, cm/s
umf Minimum fluidization velocity, cm/s
δ Bubble hold-up, -
ε Bed voidage, -
εd Emulsion phase voidage,-
εmf Minimum fluidization voidage, -
REFERENCES
(1) Geldart, D. and Kapoor, D.S., 1976, Bubble sizes in a fluidized bed at elevated
temperatures, Chem. Eng. Sci. 31, 842-843.
(2) Sitthiphong, N., George, A.H. and Bushnell, D., 1981, Bubble eruption diameter
in a fluidized bed of large particles at elevated temperatures, Chem. Eng. Sci.
36, 1259-1260.
(3) Stubington, J.F., Barrett, D. and Lowry, G., 1984, Bubble size measurements
and correlation in a fluidised bed at high temperatures, Chem. Eng. Res. Dev.
62, 173-178.
(4) Sishtla, C., Chan, I. and Knowlton, T., 1986, The effect of temperature on
bubble parameters in gas-fluidized beds, Fluidization V, Eds. K. Ostergaard and
A. Sorensen, 127-134.
(5) Hatate, Y., Ijichi, K., Uemura, Y., Migita, M. and King, D.F., 1990, Effect of bed
temperature on bubble size and bubble rising velocity in a semi-cylindrical
slugging fluidized bed, J. Chem. Eng. Japan 23, 765-767.
(6) Llop, M.F., Casal, J. and Arnaldos, J., 2000, Expansion of gas-solid fluidized
beds at pressure and high temperature, Powder Technol. 107, 212-225.
(7) Cui, H. and Chaouki, J., 2004, Effects of temperature on local two-phase flow
structure in bubbling and turbulent fluidized beds of FCC particles, Chem. Eng.
Sci. 59, 3413-3422.
(8) Formisani, B., Girimonte, R. and Pataro, G., 2002, The influence of operating
temperature on the dense phase properties of bubbling fluidized beds of solids,
Powder Technol. 125, 28-38.
CHARACTERIZATION OF THE FLUIDIZATION AND MIXING OF
BINARY MIXTURES CONTAINING BIOMASS AT LOW GAS
VELOCITIES
Farzam Fotovat1,Jaber Shabanian1,Jamal Chaouki1,and Jeffrey Bergthorson2
1
Department of Chemical Engineering, École Polytechnique, Montréal, QC, Canada
2
Department of Mechanical Engineering, McGill University, Montréal, QC, Canada
ABSTRACT
To judge qualitatively the effect of biomass properties on its fluidizability and mixing
tendency with sand particles at low fluidization velocities, local pressure gradients in
the top and bottom of the bed were compared for all investigated systems. It was
found that changing the mass fraction and the size of biomass impacted the onset of
bubbling and the size of bubbles across the bed, which, in turn, affected the
mixing/segregation of the bed content.
INTRODUCTION
Biomass, living and recently dead biological material, is known as one of the highly
potential renewable sources of energy. Biomass materials stand as the third energy
resource after oil and coal due to their abundance and rapid replenishment.
Producing energy from biomass results in the mitigation of greenhouse gas
emissions making biomass an outstanding substitution for fossil fuels. Nowadays, a
variety of thermo-chemical processes, e.g., combustion, gasification, and pyrolysis,
are being developed worldwide to convert biomass to energy and added-value fuels
(1). Due to the unique advantages of fluidized beds, they are widely used as the
heart of nearly all of the above-mentioned processes. Nevertheless, fluidization of
biomass particles alone is a problematic or even impossible task due to their peculiar
sizes, densities, and shapes. The most widespread solution for this problem is
adding inert materials, such as sand particles commonly used in regular fluidized
beds. Highly different properties of biomass and bed material particles, in terms of
hydrodynamics, result in some shortcomings, e.g., segregation, which negatively
affects fluidization performance. In spite of the noticeably different characteristics of
mixing and segregation in the biomass-sand mixture from that of a common binary
mixture, a few studies have been devoted to examine the mixing dynamics of
systems, including biomass particles (2-4). On the other hand, the scarcity of
phenomenological studies on the mixing/segregation behavior of biomass particles
hinders the industry from applying general solutions for biomass fluidization.
1
In general, the difference between the density, size, and/or shape of components of
fluidizing solids causes segregation and, as a consequence, particles of each
component tend to accumulate at the top (flotsam) or bottom (jetsam) of the bed.
Early investigations addressed mainly segregation patterns in binary mixtures of
particles of equal size but with different densities. More recent studies have been
carried out on the equal density and different size systems. Only a few works have
considered mixing and segregation phenomena in systems dealing with particles
differing in both size and density; however, such systems have a vast application not
only in biomass processing, but also in pharmaceutical and chemical industries (5).
To understand the phenomena underlying segregation in mixtures dealing with
biomass, the main objective of the present work is devoted to scrutinizing the binary
fluidization behavior of relatively light biomass and dense sand particles at
comparatively low superficial gas velocities, namely, around the limit required for
complete fluidization. In particular, the analysis of the mixing/segregation trend of
binary mixtures consisting of biomass particles with two different sizes and/or mass
fractions has been attempted on the basis of mechanisms governing the
mixing/segregation in binary mixtures of granular solids.
EXPERIMENTAL
Apparatus
The experiments were conducted in a cold conventional fluidized bed consisting of a

Plexiglas fluidization column 1.5 m high and 0.152 m in diameter. A perforated plate
containing holes 1 mm in diameter and arranged in a triangular pitch was used as a
distributor. Three graduated scales spaced at 120◦ around the column wall were
used to determine the bed height. The dynamic pressure fluctuations were monitored
along the bed via a couple of pressure transducers mounted flush with the wall of the
bed. One of the pressure transducers was used to register the pressure fluctuations
of the whole bed (PT1). The local pressure signals corresponding to the low and high
levels of the bed were obtained by two pairs of differential pressure transducers,
namely PT2 and PT3, respectively. The position and configuration of all pressure
transducers has been shown in Figure 1. The pressure data were acquired at a
sampling frequency of 400 Hz for 180 seconds through a 16 bit A/D data acquisition
board with the help of the Labview 9.0.1® program. The pressure signals were low-
pass filtered at 100 Hz to remove the signal noises. This frequency is sufficiently
higher than the frequency of typical phenomena taking place at low velocities (1-10
Hz), thus it seems unlikely to affect the signal fluctuations.
Materials
Biomass particles were provided from birch cylindrical rods with two different
diameters cut into identical lengths of tiny particles. The bed material used had a
continuous normal size distribution ranging from 100 to 1000 µm. Table 1 reports
more details of all materials used in this investigation.
2
Figure 1. Schematic diagram of experimental setup.
Table 1. Properties of materials used

Material Shape dp(mm) hp(mm) ρp(kg/m3) ρb(kg/m3) ε (-)
Sand Spherical 0.381 - 2865 1632 0.43
Biomass 1 Cylindrical 3.175 6.350 670 331.5 0.50
Biomass 2 Cylindrical 6.350 6.350 670 332 0.50
Procedure
To investigate the effect of the cross section size and mass fraction of biomass
particles four different mixtures of bed material and biomass, whose properties are
mentioned in Table 2, were studied. In each experiment, the height of the static bed
was set at 225 mm (H/D=1.5). To gain insight into the fluidization behavior of the bed
material used in the mixtures, the sand alone was fluidized first under the same
conditions as the other experiments. In an attempt to make the he mixing state of the
systems uniform before starting the experiments
experiments, the binary mixture was vigorously
fluidized for about 15 min. Experiments were conducted at ambient pressure and
temperature. Starting from the fixed bed state, the superficial gas velocity was quasi
quasi-
steadily increased until it reached the desired value. Then, the bed was slowly
defluidized until it returned to a fixed state.
Table 2. P
Properties of binary mixtures investigated
System Biomass Sand Biomass Wt.% of Vol.% of
type mass (kg) mass (kg) biomass biomass
System 1 Biomass 1 5.363 0.282 5 20.58
System 2 Biomass 2 5.364 0.282 5 20.55
System 3 Biomass 1 4.365 0.485 10 35.36
System 4 Biomass 2 4.367 0.484 10 35.33
3
Analysis Methods
Processing the time-series signals reflecting the pressure fluctuations in the different
vertical positions of the bed was the main method used to characterize the
fluidization and mixing of particles. In this regard, the time-averaged value of all
72000 data collected during each run was considered as the static pressure of the
relevant section. Moreover, signals were analyzed dynamically in time and frequency
domains. In terms of statistical analysis in the time domain, the mean amplitude or
standard deviation (σ) of the fluctuation signals over the bed has an intense
interrelation with mean bubble size. The standard deviation of pressure data is
calculated as follows (6):

=

− (1)
where N is the number of data points at the intended time interval and is the
average of recorded Pi s.
The most common method for identifying the fluidization status at different velocities
is studying the whole bed pressure drop as a function of superficial gas velocity. This
method is not, however, sufficient to distinguish the phenomenological differences
between the fluidization behavior of mixture components and, despite the diversities
existing between the systems investigated in the present work, their overall pressure
drops versus gas velocity show more or less a similar trend during fluidization and
defluidization, correspondingly.
As observed, the bed pressure drop increases initially in the fixed bed mode. It is
well known that for the ideally mono-sized and homogenous particle systems
transition from fixed to fluidized state takes place at a specific gas velocity known as
minimum fluidization velocity (Umf). Realistically speaking, Umf is determined by
finding the superficial gas velocity, which corresponds to the intersection of the
pressure drop line of the fixed bed with that for the fluidization state. Unlike the
monodispersed systems, for the binary solids mixtures the transition from fixed to
fully fluidized occurs gradually at a gas velocity interval beginning with initial
fluidization velocity (Uif) and ending at complete fluidization velocity (Ucf). Uif is
located at the point where ∆P first deviates from the fixed bed curve. In relation to
Umf of sand alone, the values of Uif of investigated binary systems were slightly
lower. This is due to the difference between the packing extent and bulk densities of
sand alone and sand mixtures containing biomass.
For the systems investigated, particles might stay in a bubble-free fluidization regime
during the transition from initial to complete fluidization mode. In other words,
deviation from the fixed bed state did not necessarily result in the immediate
formation of bubbles. The occurrence of such phenomenon is the first departure of
the fluidization behavior of binary mixtures whose components differ in density from
that of uniform particles (7).
4
A further increase in the gas velocity brought about the appearance of bubbles in the
bed. It should be noted that before bubbles became large enough to move upward
along the entire height of the bed, bubbling might take place just occasionally and
locally at the bed depending on the mixture properties. The velocity corresponding to
the onset of bubbling across the entire bed is defined as the initial bubbling velocity
(Uib). In the present work, Uib was considered as the velocity at which a sudden jump
was observed in the dominant frequency of the signal representing the pressure
fluctuations of the whole bed (PT1 signal). It is noteworthy that Uib is always located
between Uif and Ucf.
Ucf is defined as the velocity beyond which no considerable change in the total bed
pressure drop can be observed. Indeed, the essence of the Ucf is the same as that of
Umf defined for the fluidization of homogeneous particles; however determination of
Ucf is not as straightforward as the aforementioned method used for finding the Umf of
monodispersed particle systems.
In spite of the similar features of whole bed pressure drop for systems containing
different sizes and/or amounts of biomass particles, pressure drop profiles of low
(PT2) and high (PT3) levels are meaningfully different for the investigated systems.
As shown in Figure 2, the discrepancy between up and down pressure drops of the
bed in systems 1 and 2 is lower than those of systems 3 and 4, signifying the inferior
segregation propensity of sand and biomass particles in systems having less
biomass mass fraction. Notably, it seems that biomass particles with a small cross
section (system 3) are subject to an intensified segregation at a very low superficial
gas velocity compared to biomass particles having a larger cross section (system 4).
Comparing the local pressure drops of systems composed of the same biomass
particle but differing in the mass fraction of components (systems 1 & 3 or 2 & 4)
reveals that the change of the biomass mass fraction considerably changes the
behavior of the systems at low gas velocities. For example, increasing the biomass
content of the mixture could result in a delay in the formation of bubbles in the bed.
As a result, the bed content stayed in a bubble-free mode at a range of very low gas
velocities. Local segregation was extremely severe in this bubble-free fluidization
regime due to the percolation effect.
Upon the emergence of bubbles in the bed, sand particles moving with the bubble
wake can penetrate to the top flotsam-rich layer and partially offset the segregation.
Accordingly, as seen in the curves denoting system 3, the difference between up and
down pressure drops decreases sharply. A progressive increase of the gas velocity
brings about the formation of bubbles at lower layers of the bed content. Thus, one
can consider a downwardly moving front for the bubbling fluidization regime whose
movement is significantly slower for system 3 in comparison with system 1.
On the other hand, comparing the standard deviations of systems 1 & 3 or 2 &4 at
corresponding velocities (Figure 3) verifies that the increase of biomass
concentration in the mixture leads to a decrease of pressure fluctuation amplitude
(standard deviation, σ, Eq. (1)). Since the standard deviation of pressure fluctuations
as a function of gas velocity correlates with the bubble diameter (6), it can be
concluded that the size of bubbles decreases when the portion of biomass particles
increases in the bed. Therefore, it is not surprising that the ‘well mixing’ of the bed
inventory caused chiefly by strong and energetic bubbles is achieved at the higher
gas velocities.
5
16
Pressure gradient,
System 1
12
kPa/m 8
4 Top
Bottom
0
0 0.05 0.1 0.15 0.2 0.25 0.3 0.35 0.4
U, m/s
16
System 2
Pressure gradient,
12
kPa/m
8
4 Top
Bottom
0
0 0.05 0.1 0.15 0.2 0.25 0.3 0.35 0.4
U, m/s
16
Pressure gradient,
System 3
12
kPa/m
8
4 Top
Bottom
0
0 0.05 0.1 0.15 0.2 0.25 0.3 0.35 0.4
U, m/s
16
System 4
Pressure gradient,
12
kPa/m
8
4 Top
Bottom
0
0 0.05 0.1 0.15 0.2 0.25 0.3 0.35 0.4
U, m/s
Figure 2. Bottom and top pressure drop gradients of systems investigated at
increasing values of the superficial gas velocity (Top and bottom curves obtained via
time-averaging the pressure fluctuations recorded by PT2 and PT3, respectively.)
6
0.6 0.6
σ (PT1), kPa
σ (PT1), kPa 0.4 0.4
0.2 0.2
System 1 System 2
0 System3 System 4
0
0.15 0.2 0.25 0.3 0.35 0.4 0.15 0.2 0.25 0.3 0.35 0.4
U, m/s U, m/s
Figure 3. Comparison of standard deviation of signals representing the global
pressure fluctuation in systems differing in mass fraction of biomass (σ PT1)
The analysis of pressure signals shows that the bubble-free transient condition
persists only at a short range of low gas velocities for system 4. Since the number of
biomass particles in this case is about ¼ of those in system 3 (because both of these
systems contain 10% wt. biomass but the cross section of biomass particles is four
times bigger in system 4), the particle packing is less loose. Therefore, in relation to
large biomass particles, remarkable multiplicity of small biomass significantly
intensifies segregation in the early stages of fluidization; however, this condition can
improve easily in favor of mixing by the bubbles passing through the bed. The effect
of a higher number of biomass particles can be seen during the defluidization of
systems. For example, as seen in Figure 4, the larger discrepancy between top and
bottom pressure drop profiles in system 3 with respect to those of system 4
(especially at the transition zone from fluidized to fixed state) expresses the higher
sensitivity of system 3 to a gradual decrease of gas velocity. In other words, for
system 3 biomass particles possess greater potential to be segregated from sand
during the defluidization. Consequently, the system falls into the fixed bed state
earlier.
16
gradient, kPa/m
System 3
12
Pressure
8
4 Top
0 Bottom
0 0.1 0.2 0.3 0.4
U, m/s
16
gradient, kPa/m
System 4
12
Pressure
8
4 Top
0 Bottom
0 0.1 0.2 0.3 0.4

U, m/s
Figure 4. Bottom and top pressure drop gradients of systems 3 and 4 at decreasing
values of the superficial gas velocity
7
CONCLUSION
To investigate the effect of biomass properties on its fluidization behavior in the

presence of bed material, four mixtures of woody biomass and sand particles
differing in biomass size and mass fraction were investigated. The applied
characterization method was measuring the global and local pressure drops of the
bed by means of pressure transducers mounted along the bed. The intensity of
segregation in different systems was analyzed by comparing the time-averaged
amplitude of signals representing pressure fluctuations at the top and bottom of the
bed. Through comparing the profiles of local pressure drops for the mixtures
investigated, it can be concluded that since varying the mass fraction of biomass
particles changes the distribution of inlet gas between the bubble and emulsion
phases, it can considerably affect the mixing/segregation extent, particularly, at low
gas velocities. Besides, it seems that for a given mass fraction of biomass, the
number of biomass particles can influence the sensitivity of mixtures towards
mixing/segregation at least for the range of gas velocities studied.
REFRENCES
1. Khan, A., De Jong, W., Jansens, P.J. and Spliethoff, H., 2009. Biomass
combustion in fluidized bed boilers: Potential problems and remedies. Fuel
Processing Technology 90 (1), 21-50.
2. Zhang, Y., Jin, B., Zhong, W., 2008. Fluidization, mixing and segregation of a
biomass-sand mixture in a fluidized bed. International Journal of Chemical
Reactor Engineering 6, A88.
3. Zhang, Y., Jin, B., Zhong, W., 2009. Characterization of fluidization
andsegregation of biomass particles by combining image processing and
pressurefluctuations analysis. International Journal of Chemical Reactor
Engineering 7,A81.
4. Zhang, Y., Jin, B., Zhong, W., 2009. Experimental investigation on mixing and
segregation behavior of biomass particle in fluidized bed. Chemical
Engineering and Processing 48, 745-754.
5. Joseph, G. G., Leboreiro, J., Hrenya, C. M., Stevens, A. R., 2007.
Experimental segregation profiles in bubbling gas-fluidized beds. AIChE
Journal 53 (11), 2804-2813.
6. Johnson, F., Zijerveld, R. C., Schouten, J. C., Van Den Bleek, C. M., Leckner,
B., 2000. Characterization of fluidization regime by time series analysis of
pressure fluctuation. Int. J. Multiphase Flow 26, 663–715.
7. Olivieri, G., Marzocchella, A., and Salatino, P., 2004. Segregation of fluidized
binary mixtures of granular solids. AIChE Journal 50 (12), 3095-3106.
8
STUDIES ON PROPANE DEHYDROGENATION TO
PROPYLENE IN A GAS-SOLID-SOLID FLUIDIZED BED
REACTOR
Yue Chu, Tongwei Wu, Yunxin Li, Zeeshan Nawaz, Yao Wang, and Fei Wei
Beijing Key Labrotary of Green Chemical Reaction Engineering & Technology
(FLOTU), Department of Chemical Engineering, Tsinghua University, Beijing 100084,
China
ABSTRACT
Platinum and tin deposited on mixed support of SAPO-34 and alumina oxide at
certain proportion constitute a new catalyst of good catalytic performance. The
catalyst was tested in a Gas-Solid-Solid fluidized bed reactor. Cold model experiment
was carried on to obtain fluidization curves and characteristic velocities. Reaction
results in the GSS-FBR showed that propylene yield was improved by 5 % compared
with that in micro fixed bed reactor.
INTRODUCTION
Light alkenes such as propylene are indispensable raw material in numerous

(petro)chemical applications. To comply with the development of downstream
industries, propylene demand has been growing quickly (1). On-purpose propylene
production technologies such as direct propane dehydrogenation (PDH) have been
focused on as one of major process to make up the shortfall of propylene supply left
by catalytic and steam cracking of naphtha in which propylene is called a by-product
(2, 3, 4).
Nowadays, chromia-alumina catalysts and platinum based catalysts are used in

commercial dehydrogenation plants. In the late 1980s, Catofin technology applying
chromia-alumina catalyst was commercialized by ABB Lummus (6). Then during the
1990s, UOP (Universal Oil Products, USA) developed Oleflex process. In Oleflex
process, Pt-Sn/Al2O3 catalyst was used (7). The effect of support has been
discussed by many researchers. Traditional catalysts with Al 2O3 support had
problems in application especially of stability and selectivity. As a result a variety of
catalysts in which Pt-Sn was supported on various supports like SiO2, Y-zeolite, Beta,
SBA-15, MgAl(O), ZSM-5 were studied in an effort to find an optimum catalyst (5, 8, 9,
10). In our work, a kind of silicoaluminophosphate zeolite called SAPO-34 is chosen
as catalyst support which is a microporous sieve with chabasite-like structure. This
zeolite has good thermal stability and is inherently resistant toward hydrothermal
treatment (5), making it possible for support of the propane direct dehydrogenation
catalyst.
As a highly endothermic reaction, direct dehydrogenation process is suitable to be

operated in a fluid bed reactor which offers a lot of advantages such as high rate of
mass and heat transfer and solids mobility. The mobility of catalyst particles gives the
deactivate catalyst a chance to be regenerated. In PDH process, because of the high
temperature and olefins product, coke deposited rate is high resulting in deactivation
of the catalyst. In Circulating Fluidized Bed, catalysts can move into the regenerator
continuously making sure of the continuous operation.
While the particle attrition rate in a fluidized bed is much faster than fixed bed reactor,
to save the noble metal Pt of the PDH catalysts, an idea of binary particles fluidized
bed reactor (Gas-Solid-Solid fluidization, GSS) is proposed (11). In our previous work,
mechanical attrition behavior in binary fluidization was examined. The negligible
attrition of large particles in the experiment indicated that GSS fluidized reactor was
applicable for platinum based catalytic process (12).
This paper presents some experimental results from a study of Pt-Sn catalysts
supported on SAPO-34 and specially pelletized supports making up of SAPO-34
zeolite and alumina oxide binder. Effect of the improvement in catalyst supports on
catalytic activity is tested in a micro fixed bed reactor. And then in a cold model,
fluidization characteristics of pelletized catalysts are studied. Finally, the process is
operated in a lab-scale Gas-Solid-Solid fluidized bed reactor.
EXPERIMENTAL SECTION
Catalyst Preparation
Three kinds of supports were used in this article to compare their activity in propane
direct dehydrogenation. Besides pure SAPO-34 zeolite, γ-Al2O3 and their mixture
were also used. The specially pelletized support made up of SAPO-34 and Al2O3 at
certain proportion was produced by a manufactory named Hui er green chemical
technology corporation, Beijing.The Pt-Sn based catalyst was prepared by
sequential impregnation method (5). For the three kinds of catalysts made with
different supports, metallic composition was the same by 0.5, 1.0 wt % of Pt, Sn.
Catalytic Tests in a Micro Fixed Bed Reactor
The catalytic tests of different catalysts were performed using a micro fixed-bed plug
flow reactor working at atmospheric pressure. The reactor was a 8 mm i.d. and 240
mm long quartz tube placed inside an electrical furnace. Mass flow controllers were
used to adjust the amount of inlet gas. The product analysis was accomplished by an
online gas chromatograph. The deposited coke content in the catalyst sample was
analyzed by thermal gravimetric analysis (TGA) using Netzsch STA 409.
Catalytic Tests in a Gas-Solid-Solid Fluidized Bed Reactor
Cold model fluidization experiment

To be used in the Gas-Solid-Solid fluidized bed reactor, prepared catalysts were
pelletized to coarse particles with diameter of 590~840μm (20~30 mesh). SiO2
particles of average diameter 87.76μm that had similar physical properties with FCC
catalyst were used as small particles. The fluidization characteristics of that system
were studied in a cold model Perspex equipment with dimensions of diameter 5 cm
and height 100 cm. Pure nitrogen was used as fluidization medium.
Reactive fluidization experiment
Figure 1 shows a scheme of the P

P
Gas-Solid-Solid fluidized bed reactor used 1
7
in this work. The fluidized bed reactor was

4
a steel tube with inner diameter 50 mm and 6
2
height 600 mm. Inside the tube several fins
5
were added in order to enlarge the heat
50 1- Fluidized bed
transfer area and improve the fluidization 2- Disengager
10 3- Gas distributor
state. 4- Condenser
5- Sampling
600
T6 6- Filter
Typically 50 g pelletized Pt-Sn based T5 7- Catalyst inlet
T4 8- Reactant inlet
catalyst and 100 g small particles were 1 T3 9- Discharge
3 T2
catalyst
charged in the fluidized bed reactor. T1 10- Fin
8
Preheated propane and hydrogen, T1-T6:
9 Thermocouples
sometimes including inert fluidization P1: Manometer
medium nitrogen, were let into the reactor
from the bottom. The flow rate of hydrogen Figure 1 Scheme of the reactive
changed as to keep the reactant ratio fluidized bed reactor
H2/C3H8 0.25.
Influence of Supports on Catalyst Performance

Figure 2 shows the experimental result of different catalysts in a micro fixed-bed
reactor. It can be drawn that using SAPO-34 as support can largely improve
propylene selectivity as has been mentioned in our previous work (5). By adding
Al2O3 into SAPO-34 at a certain proportion as binder, the specially pelletized catalyst
made a great improvement in both propane conversion and propylene selectivity.
The coke deposited catalysts were analyzed by TGA to measure the amount of coke
produced during five hours’ reaction. The calculated data was listed in Table 1. By
comparing the coke selectivity of Pt-Sn/SAPO-34 and Pt-Sn/mixed supports, it’s
clear that coke selectivity decreased significantly through specially pelletization of the
support. The low rate of coke deposition is one of the reasons why catalysts’ activity
and stability improved by using the specially pelletized support.
Figure 3 shows the different curves of TGA results of coke deposited catalysts after
five hours’ reaction. The position of peaks which was in accordance with literatures (5,
13) showed that coke deposited on the catalyst was of different forms. The peak at
450oC shows coke deposit on Al2O3 support while the peak at 630oC represents coke
deposit on SAPO-34 support. In the mixed carriers, two kinds of coke existed
simultaneously.
40 100
35
Propylene Selectivity (%)
Propane Conversion (%)
95
30
25 Pt-Sn/SAPO-34 90
Pt-Sn/mixed supporter
Pt-Sn/Al2O3
20 Pt-Sn/SAPO-34
85 Pt-Sn/mixed supporter
15 Pt-Sn/Al2O3
10 80
0 1 2 3 4 5 0 1 2 3 4 5
Time (hr) Time (hr)
Figure 2 Evolution of catalyst performance with time in micro fixed bed reactor.
T=863K; WHSV=2.8 h-1; mcatalyst=200mg; QC3H8=5.5 ml/min; QH2=0.25 QC3H8 .
Table 1 The amount of coke formed after five hours’ on-stream and selectivity for
coke of the three kinds of catalyst calculated from TGA results
Catalyst C, wt% S coke, %
Pt-Sn / SAPO-34 7.68 4.11
Pt-Sn / mixed support 10.73 2.98
Pt-Sn / Al2O3 5.3 2.90
Pt-Sn / mixed support* 8.25 1.06
* This catalyst was tested in the GSS-FBR.
Fluidization Properties of Binary Mixtures in the GSS-FBR
To determine the proper range of operating parameters, experiments in a cold model

of same diameter to the hot model reactor were done using 50 g pelletized Pt-Sn
based catalyst and 50 g SiO 2 particles. Figure 4 shows the fluidization curve and the
calculated minimum fluidization velocity is 0.035 m/s.
Fluidization of binary particles with significhant difference had been studied decades
of years and several formulas to calculate U mf had been described. In this work a
semi-empirical formula presented by Noda was chosen to calculate the minimum
fluidization velocity (14). Calculative process was as follows:
Calculation of the average density and diameter of the mixture:

1  f p 1 f p
  ;  
m  f p dm m d f  f dpp
Calculation of Umf with the following equation:
Ar  A Re 2mf  B Re mf
In which,
d m3  (  m   ) g d umf
Ar  ; Re mf 
2 
0.196 0.296
 dp f   dp f 
A  36.2   ; B  1397   , if d p / d f  3
 d f p   d f p 
   
By using formula listed above, the Umf of our fluidization system can be calculated
and its value was 0.041 m/s. There were some difference between the experimental
result and the calculated result. This had something to do with the wide diameter
distribution of the large particles as well as the limitation of applicable range of the
formula.
0.002 350
0.000 300
-0.002
Pressure drop (Pa)

250
-0.004
dm (g)
200
-0.006
-0.008 150
-0.010 100
Pt-Sn/SAPO-34
-0.012 Pt-Sn/mixed supporter
50
Pt-Sn/Al2O3
-0.014 umf
100 200 300 400 500 600 700 800 900 0
0.00 0.02 0.04 0.06
Temperature (oC) Superficial velocity (m/s)
Figure 3 TGA results of coke deposited Figure 4 Cold model fluidization result of
catalysts the binary mixture
Reactive Fluidization Experiment
Figure 5 shows the evolution of propane conversion and propylene selectivity with
time in the micro fixed bed reactor and in the Gas-solid-solid fluidized bed reactor.
The experiments used the same specially pelletized catalysts and were run under the
same temperature, weight hourly space velocity of propane and H2/C3H8 ratio that
had been optimized in micro fixed bed reactor previously (15). It can be seen that
propane conversion was more stable in the fluidized bed reactor compared to the
fixed bed reactor. After six hours’ reaction, the remaining conversion was about 60 %
of the initial in fixed bed reactor while in fluidized bed reactor that percentage was
about 95 %. For selectivity of propylene, in both reactors, trend of two curves was
identical that in the initial period a significant increase existed and finally a stable
state of higher than 96 % can be achieved. In the GSS-FBR, though the growth
speed of selectivity was slower, high selectivity of 97 % remained steady in the later
4 hours. Propylene yield was improved by 5 % in the GSS-FBR than the fixed bed
reactor.
This improvement in propylene yield profits from the high value of heat transfer
coefficient in the fluidized bed reactor. Due to uniform bed temperature in the reactor,
the selectivity of coke deposition and byproduct like methane and ethylene resulting
form propane cracking would decrease. The value of coke deposited on catalyst after
five hours’ reaction in the GSS-FBR was measured by TGA and listed in Table 1.
Coke selectivity was found to be much lower than that of the same catalyst tested in
fixed bed reactor.
40 100
Micro fixed bed reactor
Propane Conversion (%)
Propylene Selectivity (%)

Fluidized bed reactor
35 90
30 80
70
25 Micro fixed bed reactor
Fluidized bed reactor
60
20
0 1 2 3 4 5 6 7 8 0 1 2 3 4 5 6 7 8 9
Time (hr) Time (hr)
Figure 5 Comparison of catalytic performance in fixed bed reactor and fluidized bed
reactor.T=863K; WHSV=5.6 h-1; In micro fixed bed reactor: mcatalyst=100mg ;
QC3H8=4.75 ml/min; QH2=0.25 QC3H8. In fluidized bed reactor: m catalyst = 50 g; QC3H8 =
2.38 L /min; QH2 = 0.25 QC3H8.
CONCLUSION
Pt-Sn based catalysts were tested in a micro fixed bed reactor and the specially
pelletized catalyst of higher conversion, better stability and lower coke selectivity
than others was chosen to be tried in the Gas-solid-solid fluidized bed reactor. Cold
model experiment was run to study the fluidization characteristics of binary particles
mixture with significant size difference obtaining fluidization curves and minimum
fluidization velocity. Finally, using the chosen catalyst as big particle and inert
substance SiO2 as small particle, propane dehydrogenation reaction was tried in a
fluidized bed reactor. Stable propane conversion and high propylene selectivity were
achieved. The reaction result in the GSS-FBR indicated that this design of fluidized
bed reactor was practicable for PDH process.
NOTATION
GSS-FBR: Gas-solid-solid fluidized bed reactor

TGA: Thermal gravimetric analysis
WHSV: Weight hourly space velocity, h-1
Umf: Minimum fluidization velocity, m/s
ρm: Density of mixed particles, kg/m3
dm: Diameter of mixed particles, m
ωf: Mass fraction of fine particle,
ωp: Mass fraction of large particle
ρf: Density of fine particle, kg/m3
ρp: Density of large particle, kg/m3
df: Diameter of fine particle, m
dp: Diameter of large particle, m
ρ’: Density of gas, kg/m3
μ: Viscosity of gas, Pa•S
g: Acceleration due to gravity, m/s2
REFERENCES
1. Wang G, Xu CM, Gao JS. FUEL PROCESSING TECHNOLOGY. 2008, 89(9),

864-873
2. L. Bednarova, C.E. Lyman, E. Rytter, A. Holmen. Journal of Catalysis. 2002,
211(2), 335-346
3. Odd A. Bariås, Anders Holmen, Edd A. Blekkan. Journal of Catalysis. 1996,
158(1), 1-12
4. Toshio Waku, Joseph A. Biscardi, Enrique Iglesia. Journal of Catalysis. 2004,
222(2), 481-492
5. Zeeshan Nawaz, Xiaoping Tang, Qiang Zhang, Dezheng Wang, Wei Fei.
Catalysis Communications. 2009, 10(14),1925-1930
6. Won, Wangyun, Lee, Kwang Soon, Lee, Seokho, Jung, Chansul. COMPUTERS
& CHEMICAL ENGINEERING. 2010, 34(4), 508-517
7. M. M. Bhasin, J. H. McCain, B. V. Vora, T. Imai, P. R. Pujadó.Applied Catalysis A:
General. 2001, 221(1-2), 397-419
8. M. Santhosh Kumar, Anders Holmen, De Chen. Microporous and Mesoporous
Materials. 2009, 126(1-2), 152-158
9. Linyang Bai, Yuming Zhou, Yiwei Zhang, Hui Liu, Xiaoli Sheng, Yongzheng Duan.
Catalysis Communications. 2009, 10(15), 2013-2017
10. D. Akporiaye, S. F. Jensen, U. Olsbye, F. Rohr, E. Rytter, M. Rønnekleiv, A. I.
Spjelkavik. Ind. Eng. Chem. Res. 2001, 40(22), 4741-4748
11. Shuiyuan Huang, Zhanwen Wang, Yong Jin. Chemical Engineering Science.
1999, 54(13-14), 2067-2075
12. Zeeshan Nawaz, Yue Chu, Wei Yang, Xiaoping Tang, Yao Wang, Fei Wei. Ind.
Eng. Chem. Res. 2010, 49(10), 4614-4619
13. Júlio C. Afonso, Donato A. G. Aranda, Martin Schmal, Roger Frety. Fuel
Processing Technology. 1997, 50(1), 35-48
14. K. Noda, S. Uchida, T. Makino, H. Kamo. Powder Technology. 1986, 46(2-3),
149-154
15. Zeeshan Nawaz, Xiaoping Tang, Yao Wang, Fei Wei. Ind. Eng. Chem. Res. 2010,
49(3), 1274-1280
DESIGN AND OPERATION OF BIOMASS CIRCULATING
FLUIDIZED BED BOILERS WITH HIGH STEAM PARAMETERS
Shiyuan Li, Shaolin Bao, Qinggang Lu, Dongyu Wang, Haipeng Teng
Institute of Engineering Thermophysics, Chinese Academy of Sciences, Beijing,
100190, China E-mail: lishiyuan@iet.cn
Yicheng Peng, Zhibin Liu, Bo Hong
Changsha Boiler Plant Co., Ltd., Changsha, 410114, China
ABSTRACT
Two circulating fluidized bed(CFB) boilers with capacity of 12 MWe and 25 MWe,
respectively, with biomass as fuel, adopting the basic technology independently
developed by Institute of Engineering Thermophysics (IET), Chinese Academy of
Sciences, have been in commercial operation since March 2010 in China. This paper
focuses on the design principles, the design specifications and operating results of
the two CFB boilers.
INTRODUCTION
Power demand has been mostly met by consuming fossil fuels for a long time in
China. However, fossil fuels are limited and results in severe air pollution. Due to the
increasing environmental concerns, especially on greenhouse gas emissions related
to the use of fossil fuels, new solutions to limit the greenhouse gas are continuously
sought. The available alternative energy sources are hydro, solar and wind etc. In
order to mitigate greenhouse emissions, biomass is the only carbon-based
sustainable option, which is potentially CO2-neutral and a renewable energy source.
At present, biomass has been converted into heat and electricity on a large scale
most often by combustion. Over the past five years, more than 20 commercial
biomass boilers have been put into operation in China. These boilers are all for 100%
biomass combustion because the government has a policy of providing a subsidy for
this kind of combustion. Most are grate boilers with electrical capacity from 6 MWe to
25 MWe. Recently, since the CFB combustion technology develops quickly in China,
circulating fluidized beds which can be used for a broad variety of biomass inputs
have been gradually accepted by the Chinese market. Furthermore, the cost of
fluidized beds is also its strength compared with other combustion technologies for
biomass fuels. In recent years, some biomass CFB boilers have been put into
operation for power generation with the capacities from 6 MWe to 25 MWe and at the
highest steam parameters of 9.8 MPa and 540 oC. However, to some extent the
technology of biomass CFB boilers is still immature and in the demonstration phase
in China.
1
This paper reports two CFB boilers with capacity of 12 MWe and 25 MWe,
respectively, for 100% biomass as fuel using basic technology independently
developed by Institute of Engineering Thermophysics (IET), Chinese Academy of
Sciences. The paper focuses on the design principles applied to the two boilers and
presents commercial operation results.
DESIGN PRINCIPLES OF BIOMASS CFB BOILERS
Generally, compared with coal, biomass has more oxygen, more chlorine and
potassium, less carbon, aluminum, iron, titanium and sulfur, and sometimes more
calcium. Some special elements in biomass should deserve special attention
because the existence of them will be the reason for designing different type boilers
from those for coal. The most important element in biomass is potassium, which may
form a low melting point ash during combustion in a CFB boiler. The low melting point
ash constituents can induce the formation of agglomerates in a CFB boiler, in
addition to deposition and corrosion. Accumulation of the agglomerates composed of
sand and ash particles bound by fused and glassy materials may lead to
defluidization and unscheduled shutdown of a plant (1, 2). The other important
element is chlorine with regard to its behavior for related problems in different
combustors. Chlorine found in high quantities in certain kinds of biomass, such as
straw, may affect a boiler’s operation since it can cause serious corrosion. The high
chlorine and alkali content of some biomass fuels can lead to severe damage of
combustion units. The greatest concern is high temperature corrosion of the
superheater by chlorine on the tube surface. Therefore, agglomeration, deposition
and corrosion should all be concerned in the biomass CFB boilers design. To
biomass CFB boilers, the IET’s design has the features as the follow:
z Relatively low temperatures at the combustion chambers, the cyclones and the
loop seals, approximately 780 oC to 880 oC, which will be different to different
kinds of biomass;
z To adopt the final stage superheater panels at the tops of the combustion
chambers in order to reduce corrosion. There is no deposition on these tubes
due to the movement of bed material particles;
z Kaolin or other minerals are used as bed material or added to the bed to avoid
agglomeration of bed material;
z Relatively low gas velocities in the back passes to reduce deposition.
The bulk density of the most biomass fuels, especially agricultural origin, is much
lower than that of coals (3). Many disadvantages of biomass fuels, for example,
2
relatively low heating values per unit volume, difficulty of feeding control, requirement
of huge storage vessels and expensive transportation, are due to the very low bulk
densities The energy density resulting from the bulk density and the net calorific
values influences the process control of the fuel supply system. Densification is a
good process to overcome these disadvantages. However, it is expensive and some
project owners would not like to accept the extra cost to the fuel pretreatment.
Nevertheless, herbaceous biomass should be densified before being fed into a
biomass CFB boiler. For woody biomass, suitable pretreatment for sizing is
necessary to meet the CFB facilities requirements.
Biomass fuels show higher combustion reactivity due to their high volatile content
and highly reactive char, but have much lower carbon and high oxygen contents
which are responsible for their lower heating values. The moisture content of
biomass can vary in a wide range from 10% to 60% in different seasons in a year.
High moisture contents would cause ignition and agglomeration issues and reduce
the combustion temperature, which in turn hinder the combustion of the reaction
products and consequently affects the quality of combustion. Therefore, larger
dimensions are required to guarantee the normal operation of the boiler for biomass
fuel with high moisture content which generates more flue gas.
Most biomass fuels have low inherent ash contents. However, some materials are
produced from the process because soil is incorporated into the fuel. Although dirt
increases the ash content, it is still difficult to form good bed material circulation
without adding external bed material during the operation of a CFB boiler. Therefore,
adding kaolin or other minerals during operation is necessary for a biomass CFB
boiler, which also can control the agglomeration of bed material at the same time.
12 MWe BIOMASS CFB BOILER
Design Specification of the 12 MWe Biomass CFB Boiler
Biomass fuels for the boiler are mainly sawdust, wood chips and bamboo. The
ultimate and proximate analyses of the fuel for the boiler design are listed in Table 1,
the biomass boiler arrangement is shown in Figure 1, the main design parameters
are given in Table 2.
3
Table 1 Composition of biomass
For the 12 MWe Boiler For the 25 MWe Boiler

sawdust bamboo wood corn stalk cotton stalk
Proximate analysis
Moisture (wt% as received) 48.57 30.4 42.1 9.0 10.5
Ash (wt% as dry) 3.67 4.02 0.74 22.28 11.79
Fixed carbon (wt% as dry) 17.85 — — 15.60 18.74
Volatile (wt% as dry) 78.48 53.36 47.55 62.12 69.47
Ultimate analysis (wt% as dry)
C 49.41 48.19 51.19 38.47 44.03
H 5.76 5.01 6.10 4.70 5.23
N 0.63 0.66 0.16 1.11 0.94
O 40.43 42.03 41.73 33.27 37.88
S 0.08 0.05 0.02 0.16 0.14
Cl 0.07 — — 0.515 0.226
Heating value (MJ/kg, as received)
LHV 9.48 11.70 10.03 14.10 16.43
Figure 1 The 12 MWe biomass CFB boiler arrangement
In Figure 1, there are three sets of horizontal double screw feeders conveying the
biomass to the bottom of the furnace. Two adiabatic cyclone separators with a
4
diameter of 3.0 m with water-cooled diplegs are placed between the rear wall of the
furnace and the back pass. Two non-mechanical loop seals are located below the
two separators. There are two water wall panels and three final-stage superheater
panels close to the front wall in the furnace. In the back pass, a middle-stage
superheater, a primary superheater, an economizer and an air preheater are
arranged along the flow direction of flue gas. Only one stage of spray desuperheater
is arranged at the outlet of the middle-stage superheater in the superheater system.
Operation Results
The boiler is at Changguang electricity generation plant in Changxing county of

Zhejiang province, China. Commercial operation of the biomass CFB boiler started in
March 2010. After a successful 72-hours trial run, the plant was handed over to the
owner. The performance test of the boiler was conducted in August 2010.
The design of the biomass CFB boiler was confirmed during commissioning and
subsequent commercial operation. The main commercial operating results of the
biomass CFB boiler are shown in Table 2. All gas emission values are far below the
guaranteed limits.
Table 2 Main design values and operating results of the 12 MWe biomass CFB boiler
Item Unit Design Values Operating results

Nominal steam capacity t/h 75 75.18
o
Steam temperature C 485 481.3
Steam pressure MPa 5.3 5.3
o
Feed water temperature C 150 149
o
Flue gas exit temperature C 138 142
o
Preheated air temperature C 180 180
Guaranteed boiler efficiency % 89.37 90.75
o
Furnace temperature C 810 800
o
Outlet of furnace temperature C — 730
3
NOx emission (O2=6%) mg/Nm 200 66
3
SO2 emission (O2=6%) mg/Nm 200 4
Unburnt carbon contents of recirculation ash, fly ash and bottom ash were 0.49%,
3.47% and 1.35%, respectively. The size distributions of recirculation ash and fly ash
are shown in Figure 2 and Figure 3. The size of the recirculation ash is widely
distributed from 10 μm to 450 μm with a 50% cut size of 135 μm, and the size of the
fly ash ranges from 0.5 μm to 120 μm with a 50% cut size of 40 μm.
5
Figure 2 Size distribution of recirculation ash Figure 3 Size distribution of fly ash
However, the moisture content of the biomass fuel often reached 40%~45% in
summer. The high moisture content and the non-uniformity feeding of biomass fuel
affected the boiler load greatly. In addition, some problems occurred in the biomass
fuel feeding system, which resulted in the break age of the fuel supply. The fuel
feeding system has now been improved.
25 MWe BIOMASS CFB BOILER
Design Specification of the 25 MWe Biomass CFB Boiler
The Main design parameters of the 25 MWe (130 t/h) boiler are given in Table 3. The
biomass fuel for this project were mainly corn stalk and cotton stalk pellets, the
ultimate and proximate analyses for boiler design are listed in Table 1, the boiler
arrangement is shown in Figure 4.
Table 3 Main design parameters of the 25 MW CFB Biomass Boiler
Item Unit Value

Nominal steam capacity t/h 130
o
Steam temperature C 540
Steam pressure MPa 9.81
o
Feed water temperature C 215
o
Flue gas exit temperature C 150
o
Preheated air temperature C 220
Guaranteed boiler efficiency % 89
o
Average furnace temperature C 818
3
NOx emission limit mg/Nm 200
3
SO2 emission limit mg/Nm 200
6
Figure 4 The 25 MWe biomass CFB boiler arrangement
In Figure 4, there are four sets of horizontal double screw feeders conveying the
biomass pellets to the bottom of the furnace. Two adiabatic cyclone separators with a
diameter of 4.0 m with water-cooled diplegs are placed between the rear wall of the
furnace and the back pass. Two non-mechanical loop seals are located below the
two separators. There are four water wall panels, three final-stage superheater
panels and three middle-stage superheater panels close to the front wall in the
furnace. In the back pass, a primary superheater, an economizer and an air
preheater are arranged along the flow direction of flue gas. Two stages of spray
desuperheater are arranged at the outlet of the primary and middle-stage
superheater separately in the superheater system.
Operation Results
The 25 MWe demonstration biomass plant is located in Guantao county of Hebei

province, China. Commissioning of the plant started in October 2010. In January
2011, the plant met all guaranteed targets in the performance test.
CONCLUSIONS
The 100% of IET CFB biomass boiler technology is capable of combusting a broad
7
range of different biomass fuels, including wood biomass and other agriculture
biomass. Furthermore, the technology ensures high steam parameters and enables
biomass fired power plants to obtain high efficiencies with emissions far below the
limits. So far, the 25 MWe demonstration power plant has been the biggest 100%
biomass fired CFB power plant in China, which is an important milestone.
REFERENCES
1. W. G. Lin, K. D. Johansen, F. Frandsen. Agglomeration in bio-fuel fluidized bed

combustors. Chemical Engineering Journal. 2003, 96: 171-185.
2. S. Y. Li, L.L. Shang, H. P. Teng, Q. G. Lu. A model for Agglomeration in Bio-fuel
Fired Fluidized Bed. Journal of Thermal Science. 2010, 19(5): 451-458.
3. A. Khan, W. de Jong, P. J. Jansens, H. Spliethoff. Biomass combustion in
fluidized bed boiler: Potential problems and remedies. Fuel Processing
Technology. 2009, 90 (1): 21-50.
8
DYNAMICS OF GAS-SOLID FLUIDIZED BEDS THROUGH
PRESSURE FLUCTUATIONS: A BRIEF EXAMINATION OF
METHODS OF ANALYSIS
Srdjan Sasic1, Marc-Olivier Coppens2, John van der Schaaf3, Stefan Gheorghiu4,
Filip Johnsson5, J. Ruud van Ommen6
1
Chalmers Univ. of Technology, Dept. of Applied Mechanics, Göteborg, Sweden
2
Rensselaer Polytechnic Inst., Isermann Dept. of Chem. and Biol. Eng., Troy, NY,
USA
3
Eindhoven Univ. of Technology, Lab. of Chem. React. Eng. the Netherlands
4
Center for Complexity Studies, Bucharest 061942, Romania
5
Chalmers Univ. of Technology, Dept. of Energy and Environ. Göteborg, Sweden
6
Delft Univ. of Technology, Dept. of Chem. Eng., 2628 BL Delft, the Netherlands
ABSTRACT
This paper revisits and critically examines a number of methods used for analysis of
in-bed pressure signals recorded in gas-solid fluidized beds. The goal is to obtain
information on the time scales of dominant phenomena present in the pressure time
series of four fluidization regimes. It is demonstrated that the average cycle time
represents an effective alternative to spectral analysis. In addition, we give evidence
that the average cycle time yields equivalent information as some of the advanced
methods of non-linear analysis (e.g. the Kolmogorov entropy). Finally, by using
wavelets and wavelet packets, we show how to obtain an accurate time localization
of the different frequency components present in the pressure signal.
INTRODUCTION
The dynamics of gas-solid fluidized beds are often characterized by investigating

pressure fluctuations. A pressure measurement system is robust, cheap and non-
intrusive, thus avoiding distortion of the flow around the point of measurement. In
addition, pressure is easily measured, even in industrial conditions. The in-bed
pressure fluctuations are predominantly related to bubble motion within the bed, but
a more comprehensive explanation on the origin of the fluctuation has already been
debated for a long time (e.g. Kage et al., (1); van der Schaaf et al., (2); Bi (3)). The
pressure signal has an intrinsically non-local nature, and due to this fact, the
interpretation of pressure measurements is far more complicated than of a more
local measurement, such as local solids concentration measurements using optical
probes. An important aspect of any interpretation is to evaluate available techniques
of signal analysis, related to their ability to describe the dynamics of the bed. In
general, the techniques can be grouped into three categories: (1) time domain
methods, (2) frequency domain methods, and (3) state space methods. It is not
feasible to analyse in this work all methods regularly used in the literature for the
analysis of fluidized-bed pressure signals; a broader review has recently been
published (4). In the current paper, our aim is to demonstrate how to most
conveniently gain fundamental information on the dynamics of fluidized beds (e.g.,
the main time scales) by using some of the commonly employed methods of signal
analysis. Furthermore, we will critically evaluate these techniques nowadays
frequently used and show that often some very advanced methods do not give more
insight into the system behaviour than do some considerably simpler ones. We will
carry out the analysis by looking into data sets for four fluidization regimes
investigated by Johnsson et al. (5). In summary, our goal is, by calculating the main
time scales present in the signals, to provide important recommendations on the
suitability of the use of the methods examined.
EXPERIMENTS
The data sets applied here are the same as those used in Johnsson et al. (5). In
brief, the experiments were carried out in a CFB unit operated under ambient
conditions. The riser has a cross-section of 0.12 × 0.7 m and a total height of 8.5 m.
The bed material was silica sand with an average particle size of 0.32 mm and a
particle density of 2600 kg/m3, i.e., Group B particles. In the riser, pressure
fluctuations were measured at 0.2 m above the air distributor through a 50 mm long
and 4 mm ID steel tube with a fine mesh net at the side facing the fluidized bed;
these probe dimensions in combination with the transducer minimize the distortion
of the pressure signal (van Ommen et al., 6). The pressure is measured “single
ended”: the fluctuations are recorded and the signals were low-pass filtered at the
Nyquist frequency. The sampling frequency was 400 Hz in all cases, with
33 minutes of total sampling time. The four fluidization regimes identified are: the
multiple bubble regime, the single bubble regime, the exploding bubble regime and
the transport regime. To obtain the multiple bubble regime, a distributor with a
higher pressure drop was used (Johnsson et al., (5)). Note that, although the names
of the identified regimes are not standard in the fluidization community, we have
nevertheless used them in this work, in accordance with (5). The main conditions
are presented in Table 1.
Table 1. Operating conditions for the four pressure time-series used in this paper
Regime condition Multiple Single Exploding Transport
bubble bubble bubble conditions
gas velocity [m/s] 0.6 0.6 2.2 4.1
solids mass flux [kg m-2 s-1] 0 0 ~1 25
bottom bed height [m] 0.40 0.37 0.30 -
bottom bed voidage [-] 0.51 0.50 0.58 0.80*
bottom bed pressure drop 4 960 4 730 3 310 1 120*
[Pa]
distributor pressure drop 4 200 660 3 090 13 700
[Pa]
*No bottom bed present, values given over the lower 20 cm of the columns
THEORY
As indicated above, this paper is not a full review on all the methods employed in
the literature when analyzing pressure signals in fluidized beds. Alternatively, we
have chosen here to discuss only the techniques that are either a most
straightforward choice when looking at time scales of the governing phenomena
existing in a signal, or are at present extensively used (perhaps sometimes without
justification, as we will show here).
The most common way to look at the time scales of a signal is to analyze the power
spectrum (frequency domain analysis) and a brief explanation of the procedure is
given here. Since the conclusions obtained by the spectral analysis may not be so
clear in the case of non-periodic or non-smooth signals, an alternative in the form of
the average cycle time or wavelets may be a suitable option. Finally, if we assume
that a pressure signal from fluidized beds is non-linear in nature, it is of interest to
characterize its unpredictability (i.e. the loss of information per unit of time).
Accordingly, a concise description of those methods is given in this section.
Spectral Analysis
Fourier spectral analysis often aims at obtaining the dominant frequencies present in
time series and assigning them to various physical phenomena (1). In the present
paper we will use the Welch’s method (7), where the variance is reduced by
estimating the power spectra as an average of several sub-spectra. The number of
sub-spectra is chosen to obtain a satisfactory trade-off between frequency resolution
and variance. Therefore, the signal treated is divided into time segments and an
estimate of the power spectrum of each segment is obtained. An important feature
of the spectral analysis is that the energy of the signal is conserved in the frequency
domain. Hence, summation of the power spectra over the range of interest yields
the total energy of the signal in a given frequency range.
Average Cycle Time
A suitable alternative to spectral analysis is to look at the average cycle time of the
signal. The method belongs to the time domain analysis. It is calculated as two
times the pressure signal duration divided by the number of times the pressure
signal crosses its average value (e.g. 8). The technique can be sensitive to the
presence of noise in the data, but when a low-pass filtering of the signal is applied,
the average cycle time yields useful information. A change in the trend of the
average cycle time typically indicates a regime change.
Wavelets
Wavelets allow for the representation of a signal simultaneously in time and in

frequency. In fluidization, wavelets are used to characterize the heterogeneous
nature of fluidization, and for the study of short-time or transient phenomena. Since
fluidization is a multiscale phenomenon, signals measured in fluidized beds typically
contain components on at least three frequency scales: the high-frequency scale
associated to particle motion, the medium-frequency scale related to particle
clusters, and low-frequency scale related to voids. We use here the discrete version
of the wavelet transform, which is based on a pair of digital filters. The latter
decompose the signal into a low frequency component A1 called the
“approximation”, and a high frequency component D1 called the “detail”. The
operation is then repeated using the approximation A1 as the input signal. By doing
this operation recursively up to a desired level N, one obtains a hierarchical
multiresolution representation of a signal f (Mallat, 9), such that each detail Dk
contains frequency information in a range around fs/2k, where fs is the sampling
frequency, and k is an integer. The inverse wavelet transform allows for
reconstruction of a signal without loss of information.
Entropy
Fluid dynamics in fluidized beds are governed equations of motion with a non-linear
nature. It is then not surprising that numerous results have appeared so far in the
literature from applying non-linear analysis to describe various aspects of
performance of fluidized beds, such as behaviour of bubbles and information on flow
regimes. The methods applied are based on the construction of an attractor
representing the dynamic evolution of the system in the state space, defined as a
multi-dimensional space containing all the variables governing the system. An
attractor is a clearly identified structure in the state-space domain, and probably the
most commonly applied method for its characterization is the Kolmogorov entropy
(also called correlation entropy or just entropy). The latter is a measure of
predictability of a system: it expresses the sensitivity to small changes in the initial
conditions. Linear systems have an entropy of zero and are predictable at infinitum,
whereas random systems have an infinite entropy and are thus unpredictable.
Analysis in the frequency domain most often aims at characterizing fluidization

regimes by finding the dominant frequency at which bubbles pass through the bed.
10 Fig. 1 shows power
10
spectra of pressure
10
8 fluctuations for the four
regimes as obtained by
the Welch method. The
PSD(Pa2/Hz)
6
10
low frequency region is
10
4 dominated by large
structures (bubble flow),
10
2
single bubble
and, at higher frequencies,
multiple bubble finer structures are
exploding bubble
10
0
transport conditions represented. The relation
between the two regions is
-2
10 -2 -1 0 1 2 3
still not clear, but it is often
10 10 10 10 10 10
Frequency (Hz) argued (5) that the fine
structures are not primarily
Figure 1: Power spectra of the four regimes treated in
governed by the bubble
this work.
flow. As for the analysis of
the time scales of the signals, it is obvious that valuable information can be obtained
from spectral analysis (e.g. the existence of the dominant frequency in the regimes
studied). However, applying power spectral analysis to strongly non-periodic or non-
smooth signals, such as those recorded in fluidized beds, may not always turn
beneficial. In such a case, it is useful to look at alternatives in the time domain. As
mentioned above, an easy-to-calculate characteristic is the average cycle time.
Figure 2 shows the average cycle time as the function of the gas velocity. It can be
shown that, at least within the non-circulating fluidization regimes, the average cycle
time is in effect
0.8 independent of gas
Circ. conditions Transport
velocity, solid particles
0.7
with dense conditions inventory and particle size.
For the time series applied
Aveage cycle time [-]
0.6 bottom bed
0.5 here, this would imply that

the regime change, most
0.4
likely from bubbling to
0.3 turbulent fluidization, takes
0.2 Non-circulating
place at a gas velocity
conditions around 0.88 m/s.
0.1
0 If we want to obtain a more

0 1 2 3 4
detailed picture, we can 5 6
Superficial gas velocity [m/s]
plot the cycle time
Figure 2: The average cycle times as a function of the distribution instead of just
fluidization velocity. The error bars give the standard calculating the average
deviation. The dashed vertical lines give the cycle time. Since fluidized-
boundaries between the different regimes. The large bed pressure signals are
squares indicate, from left to right, the values for the typically non-periodic
selected data sets for the single bubble, exploding signals, and in the same
bubble and transport conditions, respectively. time contain information at
multiple time scales, it may
be a good idea to use wavelets in the analysis. In this work, we have decomposed
the signals up to the 9th level, using the discrete version of the Meyer wavelet,
implemented in the Matlab Wavelet Toolbox. For every level k of the decomposition,
a reconstruction has been computed using only the detail coefficients DK. The
0 variance of the reconstruction
10 is then proportional to the
power of the signal in that
particular frequency window.
The resulting spectrum (Fig.
-2
10 3) shows that the peaks at
low frequencies, as well as
% Power
power-law tails at higher

frequencies, are nicely
-4 recovered.
10 single
multiple However, with wavelets it can
exploding be difficult to interpret the
transport results when the studied
-6
10 phenomenon does not reside
A9 D9 D8 D7 D6 D5 D4 D3 D2 D1 exactly into one of the
frequency bands of the
Figure 3: Representation of the wavelet power
wavelet decomposition. In
spectrum of the four signals. The x-axis
such a case, wavelet packets
corresponds to frequency, increasing from left to
may be used. With the latter,
right.
instead of decomposing only
the approximation Ai at stage i, both Ai and Di are passed through the low- and high-
pass filters, thus producing four components: an approximation of the
approximation, a detail of the approximation, an approximation of the detail and a
detail of the detail. As an example, Fig.4 shows the results for the exploding bubble
regime, with the logarithm of the coefficients plotted. Even with this representation,
6000 it is not straightforward
Pressure [Pa]
to see a clear separation

in frequency between
0
different components of
-4000 the signal. The
1 2 3 4 5
time [s] frequencies seem to be
Frequency [Hz]
mixed together, and we

153
may even conclude that
103
the broader bands of an
52.6
ordinary wavelet
1.4
1 2 3 4 5 analysis do a better job
Figure 4: Logarithm of the wavelet packets coefficients of separating them.
for the exploding bubble regime. Alternatively, if we
choose to present the
reconstructions of the signals from the coefficients plotted, we are in a position to
recover the total time resolution. Fig. 5 exemplifies the result of the latter procedure,
again for the exploding bubble regime.
6000
pressure [Pa]
The procedure may be

0
summarized as follows: we
set all but one of the
-4000
0.5 1 1.5 2 2.5 3 3.5 4 4.5 5 coefficients of the terminal
time [s] nodes to zero. Then, the
frequency [Hz]
187 signal is reconstructed from

109
just the coefficients of that
terminal node. It is now
31
1 2 3 4 5 3 3.5 4 4.5 5
feasible to recognize the
various components as
Figure 5: Reconstruction of the original signal from shadows in the figure.
the wavelet packets coefficients for the exploding
bubble regime.
Finally, we will assess non-linear analysis (also called chaos analysis or state space
analysis) in relation to the results obtained so far. State space analysis of pressure
data in fluidized beds has been extensively used since the second half on the
1990s. In that period, the Kolmogorov entropy has been often used to characterize
fluidized bed-hydrodynamics. For example, Schouten et al. (10) have suggested that
the Kolmogorov entropy is proportional to the number of bubbles per unit of time,
and to a bubble impact factor, defined in (10) as the ratio of the diameter of a bubble
and that of a fluidized bed. This conclusion is more valid if the signal is recorded in
the upper part of a riser, since these fluctuations reflect the local bubble behaviour
more that if the signal is measured in the bottom of the bed. However, there is a
potential problem when obtaining the Kolmogorov entropy. Namely, the entropy
should be independent of the length scale at which it is calculated, if the latter is
chosen small enough. Such a scaling region is very difficult, if possible, to find. This
statement then implies that the entropy analysis does not prove that fluidized beds
indeed exhibit low-dimensional chaotic behaviour. Furthermore, we will show on the
data sets used in the present paper that there is a strong correlation between the
Kolmogorov entropy calculated at a specific length scale and the average cycle
6 30 frequency (the inverse of the
5.5 average cycle time), see Fig.
25 6. Note that similar
Average cycle frequency [s]
Kolmogorov entropy [bits/s]

5
4.5 conclusions have already
20
4 been suggested by Johnsson
3.5 15 et al. (5) and van der Schaaf
3 et al. (11). If we plot the
2.5
10 entropy versus the average
2
5
cycle frequency (Fig. 7), we
1.5 see that the two are in fact
1 0 linearly proportional. It can be
0 1 2 3 4 5 6 demonstrated that the
Superficial gas velocity [m/s] proportionality constant is
Figure 6: The maximum likelihood entropy and the directly related to the shape
average cycle frequency as functions of the gas of the power spectrum. Since
velocity. The squares indicate the four data sets; the average cycle frequency
the other markers represent the additional and the power spectrum are
measurements at intermediate gas velocities. more easily correlated to
physical phenomena, these
characteristics should be
preferred over the
Kolmogorov entropy (or any
similar feature from the state
space analysis, such as the
correlation dimension). The
latter conclusion is further
supported by the fact that the
average frequency is not
dependent on calculation
parameters, whereas the
Kolmogorov entropy clearly
is. Since the application of
Figure 7: The maximum likelihood entropy versus non-linear analysis is typically
the average cycle frequency for the four regimes more complicated, we
investigated in the paper. recommend its use only if it
yields information that is not
obtainable by linear analysis, such as an early detection of non-stationarities in
fluidized bed behaviour (12).
CONCLUSIONS
When pressure is recorded in a gas-solid fluidized bed, the obtained signal can yield
significant information on the bed dynamics. The interpretation of signals is,
however, not always straightforward. In this paper, we have revisited some of the
most commonly used methods of analysis of the pressure time series. The work is
not meant as a complete review paper. Instead, we have chosen to go through the
techniques frequently used to obtain information on main time scales of the
dominant phenomena present in the bed. We have shown that the cycle time and its
distribution provide useful information on the dynamics of the bed. As such, they
represent an easy-to-calculate alternative to frequency analysis. The latter, in
general, provides essential information, but may be problematic when non-periodic
and non-smooth signals are investigated.
To provide information on time localization of particular frequency components in a

signal, we have carried out the analysis using wavelets and wavelet packets. We
have seen that the main features of the spectral analysis are adequately reproduced
by wavelet analysis. We have used wavelet packets to obtain an unambiguous
separation in frequency between different components of the signals.
Finally, we have shown that the information given by the Kolmogorov entropy is
entirely equivalent to that of the average cycle frequency, obtained by linear
methods of analysis.
REFERENCES
1. Kage, H., Iwasaki, N., Yamaguchi, H., Matsuno, Y., 1991. Frequency analysis of pressure
fluctuation in fluidized bed plenum. J. Chem. Eng. Jpn. 24, 76-81.
2. van der Schaaf, J., Schouten, J.C., van den Bleek, C.M., 1998. Origin, propagation and
attenuation of pressure waves in gas-solid fluidized beds. Powder Technol. 95, 220-233.
3. Bi, H.T., 2007. A critical review of the complex pressure fluctuation phenomenon in gas-
solids fluidized beds. Chem. Eng. Sci. 62, 3473-3493.
4. van Ommen, J.R., Sasic, S., van der Schaaf, J., Gheorghiu, S., Johnsson, F., Coppens,
M.O., 2010, Time series analysis of pressure fluctuations in gas-solid fluidized beds – a
review, in press, Int. J. of Multiphase Flow, dx.doi.org/10.1016/j.ijmultiphaseflow.2010.12.007
5. Johnsson, F., Zijerveld, R.C., Schouten, J.C., van den Bleek, C.M., Leckner, B., 2000.
Characterization of fluidization regimes by time-series analysis of pressure fluctuations. Int.
J. Multiphase Flow 26, 663-715.
6. van Ommen, J.R., Schouten, J.C., vander Stappen, M.L.M., van den Bleek, C.M., 1999.
Response characteristics of probe-transducer systems for pressure measurements in gas-
solid fluidized beds: How to prevent pitfalls in dynamic pressure measurements. Powder
Technol. 106, 199-218.
7. Welch, P.D., 1967. The use of fast Fourier transform for the estimation of power spectra: a
method based on the averaging over short, modified periodograms. IEEE Transactions
Audio Electroacoustics AU-15, 70-73.
8. Briens, L.A., Briens, C.L., 2002. Cycle detection and characterization in chemical
engineering. AIChE J. 48, 970-980.
9. Mallat, S., A wavelet tour of signal processing. Academic Press, London, (1999) ISBN 0-
12-466605-1.
10. Schouten, J.C., vander Stappen, MLM, van den Bleek, CM., 2000, Scale-up of fluidized
bed hydrodynamics. Chem. Eng. Science 51, 1991-2000.
11. van der Schaaf, J.,van Ommen, J.R., Takens, F., Schouten, J.C., van den Bleek, C.M.,
2004. Similarity between chaos analysis and frequency analysis of pressure fluctuations in
fluidized beds. Chem. Eng. science 59, 1829-1840.
12. van Ommen, J.R., Coppens, M. O., van den Bleek, C.M., Schouten, J.C., 2000. Early
warning of agglomeration in fluidized beds by attractor comparison, AIChE J., 46, 2183
2197.
A STUDY OF SOLID AND GAS MIXING
IN A PARTITIONED FLUIDIZED BED
Jong-Ho Moon, Young-Ju Seo, Solim Kang, Seung-Yong Lee,
Young-Cheol Park, Ho-Jung Ryu, and Gyoung-Tae Jin
Korea Institute of Energy Research, Greenhouse Gas Research Center
71-2 Jang-dong, Yuseong-gu, Daejon 305-343, Korea
T: +82-42-860-3676. F: +82-42-860-3134. E: gtjin@kier.re.kr
ABSTRACT
A partitioned fluidized bed gasifier has been developed for improving coal
gasification performance. The basic concept is to divide a fluidized bed into two
parts, a gasifier and a combustor, by a partition. Char is burnt in the combustor and
generated heat is supplied to the gasifier by solid mixing. Therefore, solid mixing
should be maximized whereas gas mixing between syngas and the combusted gas
should be minimized. In this study, gas and solid mixing behaviors were verified in
cold model acrylic beds. For monitoring solid mixing behavior, transient temperature
trends in the beds were analyzed. A heat source and a heat sink were installed in
each bed. Dozens of thermocouples were used to monitor temperature distribution.
INTRODUCTION
Since the world recoverable oil resources will be depleted within the next few
decades, a search for alternatives to oil is an urgent task. In the post-oil era, coal
technologies are of great interest as a practical alternative to oil, due to their cost,
availability and versatility. However coal causes 40% of global CO2 emissions. CO2
is considered as a representative green-house gas and increased levels of CO 2 with
other green-house gases in the atmosphere contribute to global warming. To sum up,
mankind will have to use coal, but at the same time restrain CO 2 emissions.
Therefore, clean coal technologies should be developed.
The solid residence time depends on solids feed rate in a fluidized bed. In a dual
bed system, the solid residence time depends on the sum of the solid feed rates and
solid circulation rates. If the heat requirement is increased, it is necessary to
increase the solid circulation rates. This shortens the residence time of solids and
reduces the solid conversion. To overcome this, a “partitioned fluidized bed” concept
for low rank coal gasification has been developed (figure 1). The upper part of the
bed is blocked by a partition, but the lower part of the partition is open to connect the
two beds. Endothermic reactions (coal gasification) and exothermic reactions (coal
combustion) occur simultaneously in a gasifier and combustor. For coal gasification,
a high temperature of over 900oC is needed. Most of the heat is generated by coal
combustion. Therefore, the generated heat should be supplied from a combustor to
a gasifier using the bed materials.
In this study, cold model experiments in a “partitioned fluidized bed (transparent

acrylic bed)” were executed at atmospheric conditions to understand solid and gas
mixing behavior. N2, CO2 and compressed air were introduced as fluidizing gases
into each partitioned fluidized bed. For the gas mixing experiments, glass beads with
an average diameter of 150 microns and particle density of 2.5 g/cm3 were used. As
can be seen in figure 2(a), CO2 and N2 were introduced into each distributor in the
bed. Outlet gas flow rates and concentrations for each bed were analyzed by gas
flow meters and FT-IR respectively. The gas exchange ratios between the reactors
were then calculated. For the solid mixing experiments, 1000-micron polypropylene
particles with a density of 0.883 g/cm3 were continuously fed into the reactor. As a
fluidizing gas, compressed air was introduced into each bed. For improving solid
mixing, newly developed distributors and plenums were installed. The objectives of
this study were to understand gas and solid mixing characteristics and to quantify
the solid flux between the reactors under various operating conditions.
Figure 1. Schematic diagrams of coal gasifiers:

conventional, dual, and partitioned fluidized bed gasifiers
EXPERIMENTAL
Experimental Method (1): Gas Mixing
For gas mixing experiments, CO2 and N2 were introduced into each distributor.
Experimental procedure was (Figure 3): step 1. Initially, introduce N2 into each
partitioned bed (L, C, R) to fluidize the solids, step 2. Switch N2 to CO2 in the center
bed by using a 3-way valve, step 3. Measure flow rates and concentrations. Outlet
gas flow rates and concentrations of each fluidized bed were analyzed by gas flow
meters and IR respectively. Then, the gas exchange rates between the reactors
were calculated.
Mixed Gases
Center
PP
Right L C R
GB
N2 CO2 N2
(a) Configuration (b) Diagram (c) Photo
Figure 2. Schematic diagram of a partitioned fluidized bed: (a) Cold model
configuration, (b) Diagram, and (c) Apparatus for cold mode run
N2 N2 N 2 N2 N2 N 2 Mixed Gases
N 2 N 2 N2 N2 CO2 N2 N2 CO2 N2
Step 1 Step 2 Step 3
Figure 3. Experimental procedure for gas mixing evaluation
At first, CO2 and N2 compositions and flow rates at the inlet and the outlet of each
bed were measured and/or calculated respectively. Then, they were substituted into
the following equations;
VC  yC ,CO2
X RC  (1)
FR  xR , CO2
VR  yR , N 2
X CR  (2)
FC  xC , N 2
Where, XRC (Eq. 1) is the gas exchange ratio from the right side bed to the center
bed and the XCR (Eq. 2) is the gas exchange in the opposite direction. F and V are
inlet and outlet flow rates respectively. Small x and y are inlet and outlet mole
fractions respectively. Subscripts R and C mean left and center beds.
Experimental Method (2): Solid Mixing
For the solid mixing experiments, the 1000-micron polypropylene particles with a
density of 0.883 g/cm3 were continuously fed into the left bed (L). Mixed solid
particles were withdrawn from the center bed (C) and the right bed (R) (figure 4). As
a fluidizing gas, compressed air was introduced into each partitioned fluidized bed
by controlling input flow rates. Outlet gas flow rates of each fluidized bed were
measured by gas flow meters. Withdrawn mixed solid particles (GB/PP) were
separated by sieves. The solid particle distributions were measured by weighing the
separated particles.
O utput
GB PP PP (solid)
Air Air Air Air Air Air Air Air A ir

Step 1 Step 2 Step 3
Figure 4. Experimental procedure of solid mixing at a three partitioned fluidized bed
gasifier.
Center and right side solid discharge ratio could be controlled by the fluidizing gas
velocity in each side bed. The discharge percentage of center was mainly affected
by the ratio of UC (input fluidizing velocity at center bed) to UR (right bed). As can be
seen in figure 5, solid mixing in a three partitioned fluidized bed can be considered
the same as in a CSTR.
 CSTR w/o Reaction  Partitioned-FB

N2 N2 N2
Input Output Input Output

(liquid) (liquid) (solid) (solid)
N2 N2 N2
0
Perfect-Mixing Well-Mixing
Figure 5. Analogy between a CSTR and a Partitioned fluidized bed.
Gas Exchange Experiments
The effect of gas velocity on gas mixing is shown in figures 6 and 7. In this
experiment, the gas velocity of each reactor was same.
100 100
99
CO2
80 98
N2
97
Mole Fraction [%]
Mole Fraction [%]
60 96
40 4
3 CO2
20 2
N2
1
0 0
0 20 40 60 80 100 0 20 40 60 80 100
Time [sec] Time [sec]
(a) Center Bed (b) Right Bed

Figure 6. Transient gas mixing behavior (UL=UC=UR=2Umf): (a) Center Bed and (b)
Right bed
The left side, center and right side gas velocities were 2, 3, and 4 times the
minimum fluidizing velocity (Umf). Figure 6 shows transient gas mixing behavior for
the center and right beds. It reached a steady state within 80 sec. After reaching
steady state, CO2 mol% in the center bed was 93.5% (XCR=0.032) and N2 mol% in
the right bed was 97.0% (XRC=0.0.032). This means that the effect of gas mixing in
the partitioned fluidized bed was very small. Increasing the gas velocity from 2.0 to
4.0 Umf, caused the gas exchange rates from the center to left(XCL) and right(XCR) to
decrease while the gas flows from the left and right to center (X LC and XRC)
increased.
At the same gas velocity in each bed (figure. 7 (a)), the gas exchange ratios, from
center to right and from right to center, had similar values. At higher flow rates, gas
mixing was slightly enhanced. At a low gas velocity condition in the center (figure.
7(b)), XCR was far higher than XRC. The exchanged CO2 amount from center to right
decreased, whereas the exchanged N2 amount from right to center increased. XRC
was not affected by the center flow rate. At low flow rates in right and left beds
(figure 7 (c)), the exchanged CO2 amount from the C to R bed linearly increased,
while the exchanged N2 amount from the right to center bed decreased. That means
the flow from the side to the center became dominant. XCR was not affected by flow
rate in the center bed.
10
(a)
Gas Exchange Ratio [ - ]
XRC
8 XCR
2
2 3 4
UC / Umf [ - ]
12
(b)
XRC
10
XCR
2
2 3 4
Uc / Umf [ - ]
8
(c)
6
XRC
5 XCR
4
2
2 3 4
Uc / Umf [ - ]
Figure 7. The effect of flow rate on gas mixing (exchange ratio):
(a) case1 (UL = UC = UR), (b) case2 (UL = UR = 4Umf), and (c) case3 (UL = UR = 2Umf)
Solid Mixing Experiments
Figure 8 shows analogies between a CSTR and a partitioned fluidized bed. CSTR
behaviors are based on perfect mixing. That is, as soon as reactants are introduced
into a reactor, mixing and reaction occurs immediately. For no reaction, a CSTR is a
perfect mixer. Similarly, if solids are well mixed in a three-partitioned fluidized bed,
the solid concentration in each partitioned bed will be the same. Figure 8(a) shows a
comparison between calculated CSTR behavior and experimental data from a
partitioned fluidized bed. The calculated line is CSTR behavior and the squares are
experimental data from a partitioned fluidized bed, where the x-axis is time and the
y-axis is PP (polypropylene) concentration in the mixtures.
The second figure indicates PP concentration dispersion between the center and
right beds. The x-axis is PP concentration in the center bed and the y-axis is that in
the right bed. The diagonal line shows the case when the PP concentration in the
center and right beds are exactly same, i.e. CSTR behavior. The squares are the
experimental data.
1.0
1.0(a)
(b)
0.8 0.8
C/C0, PP Content [w/w]
PP content at R [ - ]
0.6 0.6
0.4
0.4
0.2 Center Column

Right Column 0.2
CSTR Behavior Exp.
0.0 CSTR
0.0
0 1 2 3 4 0.0 0.2 0.4 0.6 0.8 1.0
Residence Time [ - ] PP content at C [ - ]
Figure 8. Experimental vs. theoretical results of solid mixing behavior

(UL = UC = UR = 2Umf):
(a) Comparison between CSTR and partitioned fluidized bed, and
(b) Particle distribution at the partitioned bed fluidized bed
Temperature Trend
As can be seen from the above results, the solid mixing behavior in a three
partitioned bed is analogous to liquid mixing behavior in a CSTR. These results were
be confirmed by analyzing temperature distribution. Dozens of thermocouples were
added to the beds for monitoring temperature distribution. (See Figure. 9) For
improving solid mixing, newly-developed distributor systems were installed.
For monitoring solid mixing behavior, transient temperature trends in the beds were
analyzed. A heat source (right bed) and a heat sink (left bed) were installed in each
bed at a height of 55 cm. Dozens of thermocouples were equipped for monitoring
temperature distribution. Figure 10 shows the transient temperature trend at the
heat source (combustor) and the heat sink (gasifier). Initially, fluidizing air was not
introduced into the beds. Therefore, the temperatures at the heat source and the
heat sink could be kept constant at 24℃ and 19℃, respectively. After introducing
fluidizing air (UL = UR = 2Umf) into the beds, generated heat was transferred from the
right bed (heat source) to the left bed (heat sink). Temperatures at all positions
reached steady state within 50 seconds. This means that the solids (or temperature)
can be dispersed well in spite of a partition in the bed.
Figure 9. Cold mode partitioned bed for analyzing temperature distribution.
25
Heat Source (55 cm)

24 Heat Sink (55 cm)
23
Temperature [ C]
o
22
21
20
19
18
-10 0 10 20 30 40 50 60
Time [sec]
Figure 10. Transient temperature trend in a partitioned fluidized bed (UL = UR =
2Umf); temperature at heat source (white circles) and heat sink (black diamonds)
CONCLUSIONS
Gas and solid mixing experiments in partitioned fluidized beds were conducted. Gas
mixing between the partitioned fluidized beds can be minimized by controlling the
gas velocity in the beds.
The center and right side solid discharge ratio can be controlled by the fluidizing gas
velocity in each side bed. The discharge percentage in the center bed is mainly
affected by the ratio of UC to UR. Solid mixing in partitioned fluidized beds can be
considered well mixed as in a CSTR.
ACKNOWLEDGMENT
This work was supported by Energy Efficiency and Resources R&D program
(2009T100100675) under SK Innovation Co., Ltd. and the Ministry of Knowledge
Economy, Republic of Korea
NOTATIONS
F inlet mass flow rates respectively (g s-1)

r rate of reaction (g cm-3 s-1)
t time (s)
U gas velocity (cm s-1)
V outlet mass flow rates (g s-1)
XCR gas exchange ratio from the center to the right side (-)
x inlet mole fraction (-)
y outlet mole fraction (-)
Subscripts
L, C, R left, center and right respectively

mf minimum fluidization conditions
REFERENCES
1. Murakami, T., Xu, G. Suda, T. and Matsuzawa, Y. Tani, H., Fujimori, T. (2007).
“Some process fundamentals of biomass gasification in dual fluidized bed”, Fuel,
86, 244–255
2. Du, B., Fan, L-S., Wei, F. and Warsito, W. (2002). “Gas and solid mixing in a
turbulent fluidized bed“, AIChE J., 48(9), 1896-1910
3. G.T. Jin et al., ISOPE2010, Beijing, China (2010)
4. G.T. Jin et al., FLUIDIZATION XIII, Gyeong-ju, Korea (2010)
EXPERIMENTAL STUDY ON THE EFFECTS OF GAS
PERMEATION THROUGH FLAT MEMBRANES ON THE
HYDRODYNAMICS IN FLUIDIZED BEDS
J.F. de Jong, M. van Sint Annaland, J.A.M. Kuipers
Multiphase Reactors Group, Department of Chemical Engineering and Chemistry,

Eindhoven University of Technology, P.O. Box 513, 5600 MB Eindhoven, the
Netherlands. E-mail: m.v.sintannaland@tue.nl, URL: http://www.chem.tue.nl/smr, T:
+31(0)402472241, F: +31(0)402475833
ABSTRACT
In this work, the effects of gas permeation through flat membranes on the
hydrodynamics in a pseudo-2D membrane-assisted gas-solid fluidized bed have
been investigated experimentally. A combination of the non-invasive Particle Image
Velocimetry (PIV) and Digital Image Analysis (DIA) was employed to simultaneously
investigate emulsion phase and bubble phase properties in great detail. Counter-
intuitively, addition of secondary gas via the membranes, that constituted the
confining walls of a gas-solid suspension at conditions close to incipient fluidization,
did not result in a larger, but in a smaller bubble diameter, while gas extraction on
the other hand, resulted in a larger equivalent bubble diameter, although in this case
the effect was less pronounced. This could be explained by changes in the larger
scale particle circulation patterns due to gas extraction and addition via the
membranes: gas extraction leads to densely packed zones near the membranes,
forcing bubbles through the center of the bed, where they become elongated and
increase in size. Gas addition, on the other hand, totally inverts the particle
circulation compared to a fluidized bed without membranes, splitting up bubbles in
the center and forcing them towards the membranes, thus decreasing the bubble
size.
INTRODUCTION
Fluidized bed membrane reactors combine the excellent separation properties of

membranes with the advantages of fluidized beds. Moreover, the utilization of
membranes enables to overcome reaction equilibrium limitations, thus resulting in
higher reactant conversions and product yields. These clear advantages have led to
an increasing number of applications of fluidized bed membrane reactors being
proposed, for both product removal (e.g. hydrogen with palladium membranes) and
reactant dosing (mostly oxygen) via membranes (Adris et al. (1); Mleczko et al. (2);
Grace et al. (3); Gallucci et al. (4)). Despite the current developments, however,
detailed understanding of the effect of the presence and permeation of gas through
membranes immersed in a fluidized bed is lacking. The majority of current research
relies on experimentally acquired data in experimental setups designed to provide a
proof-of-concept and on phenomenological models, which often make use of ad-hoc
empirical correlations that neglect the influence of internals.
Al-Sherehy et al. (5) investigated distributed feed and concluded that oxygen
distribution is beneficial in expanding the range of reactant feed compositions
beyond those normally allowed by safety constraints, while the selectivity was
increased. Deshmukh et al. (6) confirmed these findings and, moreover, made great
advances with respect to the effect of the presence of – and permeation through –
the membranes on the extent of gas back mixing and the bubble-to-emulsion phase
mass transfer rate. With ultrasound gas tracer experiments, they showed that due to
the presence of membranes, but particularly due to gas permeation through the
membranes, the macro-scale solids circulation was strongly reduced, resulting in a
near plug-flow behavior for the gas phase. They also found smaller average bubble
diameters for higher permeation ratios relative to the total gas flow. Christensen et
al. (7) confirmed that such systems indeed lead to a decrease in bubble size and
bubble hold-up, and therefore to an increase in the total number of bubbles.
This paper aims to advance the fundamental understanding by investigating

experimentally the effect of a change in gas flow rate inside a fluidized bed
membrane reactor, where gas is added or extracted through the side-walls of the
fluidized bed. Therefore, we focus specifically on bubble formation/annihilation close
to the membranes, bubble size distribution and particle mixing as a function of the
gas permeation ratio, i.e. the ratio of gas added/extracted relative to the total feed.
After a description of the experimental setup and the procedures used for data post-
processing, we discuss and compare the PIV/DIA results for cases of gas extraction
and gas addition.
EXPERIMENTAL SETUP
A pseudo-2D setup 30cm in width, 1.5cm in depth and 1m in height has been
constructed. For the front of the bed a glass plate is used, for the back an anodized
aluminum plate to provide good contrast between emulsion phase and background.
The distributor is a porous plate with a mean pore size of 40 μm. At both sides of the
fluidized bed, up to a height of 30cm above the distributor, gas can be added to or
extracted from the fluidized bed through a 10 μm porous plate. For all experiments,
glass beads with a particle size distribution of 400-600 μm and a density of 2500
kg/m3 (Geldart B) have been used. Air has been used as a fluidization agent. The
Figure 1: Process flow diagram of the experimental setup

process flow diagram is given in Figure 1. The minimum fluidization velocity Umf was
determined to be 0.25 m/s by slowly decreasing the fluidization velocity. All
experiments reported here have been performed with a total gas feed corresponding
to 2.6.U/Umf (see Table 1). A lower velocity would significantly de-fluidize the bed
during gas extraction experiments, while a much higher gas velocity is not possible
with the current setup. The number of images has been determined to be sufficient
for obtaining reliable time-averaged results; the error in the vector plots presented in
this paper is below 6%. The error in the equivalent bubble diameter depends on the
number of bubbles detected at a certain height in the bed, and ranges from <1% at
a height of 2.5 cm to 3% at a height of 45 cm.
PIV/DIA Procedure
PIV is a non-intrusive optical technique based on the comparison of two images

recorded with a very small time delay (here 0.82-1.98 ms) with a high speed CCD
camera. It divides every image into interrogation zones (here 32x32 pixels were
used), and uses a special cross-correlation on two consecutive images to obtain an
average displacement of the particles in that interrogation zone. These PIV image
pairs were post-processed using the commercial software package DaVis.
DIA is an image post-processing algorithm, that discriminates bubble and emulsion

phase based on the pixel intensity. Prior to the actual bubble detection, the
algorithm corrects for the camera lens effect, inhomogeneous lighting and shadow
effects near the walls. For every measurement series at least 10 random images
were inspected visually, to ensure that the script is functioning correctly. Only by
using the combination of PIV and DIA, it is possible to determine the time-averaged
emulsion phase velocity profiles from the obtained instantaneous particle velocity
profiles and correct for particle raining through the bubbles to avoid under-estimation
of the particle fluxes in the centre of the bed (Laverman et al. (8)).
Table 1: Measurement series

Measurement Background gas Total membrane Number of
name flow / velocity flow / velocity images
[-] [%] [m/s] [%] [m/s] For DIA [-] For PIV [-]
Reference 100 0.65 0 0 2700 2160
100% + 20% 100 0.65 +20 + 0.065 2700 2160
100% + 40% 100 0.65 +40 + 0.130 2700 2160
100% - 20% 100 0.65 -20 - 0.065 1350 2160
100% - 40% 100 0.65 -40 - 0.130 1350 2160
RESULTS & DISCUSSION
The discussion on the experimental results on the effect of gas permeation on the
hydrodynamics of the fluidized bed is started by first focusing on the solids
circulation patterns, followed by the bubble properties.
Emulsion Phase Circulation Patterns
The time averaged solids circulation pattern and the time-averaged lateral profile of
the axial emulsion phase velocity at different heights in the bed is shown in Figure 2.
In the reference series without secondary gas extraction or addition, the
characteristic pattern for fluidized beds with an upwards directed solids flow through
Figure 2: Time-averaged particle movement and time-averaged lateral profile of the
axial emulsion phase velocity for different heights in the fluidized bed with (a) 40%
gas extraction, (b) 20% gas extraction, (c) the reference series with no gas
addition/extraction, (d) 20% gas addition and (e) 40% gas addition.
the core and a downward solids flow along the walls of the fluidized bed can be
clearly discerned. This well-known solids circulation pattern is also clearly visible in
the lateral profiles of the axial emulsion phase velocity at different heights: a broad
region in which particles move upwards in the center of the fluidized bed, and near
the walls a small region where the particles move downwards. It is interesting to
notice the local minimum in the axial emulsion phase velocity in the centre at 10 cm
above the bottom distributor plate, corresponding to the well-known average bubble
trajectories from the walls towards the centre in the lower sections of the fluidized
bed (see also Laverman et al. (8)).
When comparing the cases with gas extraction to the reference case, a striking
difference is the stagnant regions near the membranes in case of gas extraction. It
is already appearing in the 100%-20% case, but becomes even more pronounced
when 40% of the background fluidization gas is extracted. These stagnant zones
have two consequences: the first consequence is that the bed height is reduced,
implying a smaller number of bubbles or smaller bubbles inside the fluidized bed.
Secondly, the velocity plot shows that the peak of upward moving solids has
become steeper, while the downward directed ‘peak’ for the downward moving
solids has become less pronounced and has shifted somewhat towards the center
of the bed. The reason for these phenomena is that the stagnant zones near the
membranes leave less space for bubbles to rise and for particles to re-circulate to
the bottom of the bed, resulting in narrower vortices in the solids circulation.
In contrast to gas extraction, gas addition via the membranes has an even more
distinctive effect on the particle circulation pattern: gas addition inverts the
circulation pattern. This phenomenon shows that there is a competition between the
background gas velocity and the additional gas entering via the membranes to drag
the particles along. Already in the 100%+20% series this phenomenon starts to
become apparent, but is even more pronounced for the 100%+40% series. Usually
particles would move downwards near the walls. However, due to the gas addition,
particles near the wall (in the first 30 cm) are dragged upwards instead, causing the
particles to move downwards in the center of the bed. This phenomenon is also
illustrated by the lowest three lateral profiles of the axial emulsion phase velocity
profiles; the upwards directed peak is now near the wall, while the velocity in the
center of the bed is slightly negative. Above the membrane (above 30 cm), the
particles are pushed towards the center, and continue their way as usual: upwards
via the center and downwards via the sides. This division in a part with membrane
and a part without membrane results in four vortices inside the fluidized bed, each
one rotating differently than its neighbor.
The findings described above can be schematically summarized as depicted in

Figure 3. In all cases, the magnitude of the effects depends on the background
fluidization velocity and amount of gas extraction or gas addition. It can be expected
that the change in particle behavior has a pronounced effect on the bubble
properties and bubble size distribution, which is discussed next.
Figure 3: Illustration of the particle circulation patterns for (a) gas extraction, (b) the
reference and (c) gas addition.
Bubble Properties
Firstly, the obtained experimental results were validated by comparison with

literature; both the equivalent bubble diameter, as well as the bubble rise velocity
compared well to the corresponding literature correlations (not shown here).
Subsequently, the equivalent bubble diameter as a function of the axial position in
the fluidized bed is shown in Figure 4.a. In the lower part of the fluidized bed, the
bubbles remain approximately the same size, irrespective of the amount of gas
extraction or addition. Only from a height of approximately 20 cm, a difference
becomes apparent. However, unlike what would be expected intuitively, extracting
gas leads to larger bubbles, while adding gas results in smaller bubbles.
Figure 4: Effect of gas extraction and addition on (a) equivalent bubble diameter as
a function of the bed height, (b) average number of bubbles per frame as a function
of the bed height, (c) average bubble diameter as a function of the lateral position
and (d) bubble hold-up as function of the bed height.
In particular the experimental series in which gas is added via the membranes
deviate substantially from the reference case above a height of 30 cm. Note that the
largest bubbles for the cases of gas extraction appear at 40 cm height, the ones for
the reference case at about 46 cm, and the bubbles for the cases with gas addition
appear even at 52 cm height, reflecting the difference in fluidized bed height.
Figure 4.b shows a slight difference in the average number of bubbles present in
every frame. For gas addition, it can be concluded that there are more bubbles
(Figure 4.b) with a smaller diameter (see Figure 4.a). For gas extraction, the number
of bubbles is decreased, but they have a larger equivalent diameter. However, the
difference in the number of bubbles is less important in comparison with the
difference in bubble diameter. The bubble rise velocity as a function of the
equivalent bubble diameter (not shown here) is quite similar for all cases. The
graphs of the lateral profile of the equivalent bubble diameter and the axial profile of
the bubble hold-up (Figure 4.c and 4.d) provide more insight into the bubble
behavior. There is a significant difference in the average lateral position of the
bubbles. The reference case shows an almost parabolic distribution, as expected,
because bubbles are formed over the entire width of the fluidized bed and move
towards the center due to bubble coalescence. The 100%-20% and 100%-40%
series show a similar distribution, although bubbles are situated more in the center
(which is in line with the conclusions drawn from Figure 2). The 100%+20% and
100%+40% series reveal a very different bubble distribution: in these cases the
large bubbles are situated much closer to the walls. In the center, a significant
decrease in bubble diameter is visible, indicating that the movement of the bubbles
is reversed, i.e. while bubbles are rising and growing, they are moving away from
the center and towards the membranes. This is in line with the particle movement
seen in Figure 3.
Not only the location, but also the bubble volume is different or these cases. The
series with gas extraction show a slightly larger bubble volume, although this
difference is very small. However, the series with gas addition reveal that – in
particular in the top section of the bed – the bubble volume is much smaller
compared to the reference case. Now the question remains why for the 100%+20
and 100%+40 series, both the average bubble diameter as well as the average
bubble volume are lower than the reference case. This phenomenon is caused by a
combination of particle movement and bubble detection: large gas voids near the
walls are likely to be part of the freeboard of the fluidized bed, and are therefore no
longer defined as bubbles. This is caused by particles near the freeboard that are –
in contrast to the reference case – moving away from the wall toward the center of
the fluidized bed, and as a consequence, there are much fewer large bubbles
surrounded by emulsion phase. The effect of gas extraction and gas addition on the
bubble behavior is schematically depicted in Figure 5.
Figure 5: Illustration of the bubble size distribution and movement for (a) gas
extraction, (b) the reference and (c) gas addition.
CONCLUSIONS
A pseudo-2D experimental fluidized bed setup with membranes (porous plates) at

both the left and right side has been constructed to investigate the effect of gas
extraction or gas addition on the emulsion and bubble phase behavior in detail. A
combination of Particle Image Velocimetry (PIV) and Digital Image Analysis (DIA)
was employed.
The experimental results revealed that gas addition via the membranes counter-
intuitively leads to significantly smaller bubbles, whereas gas extraction slightly
increases the bubble size. During gas addition, the bubble size in the top of the bed
decreased to 60% of the original bubble size. During gas extraction, a small
increase in bubble size was found (an increase in bubble size of 10% and 20% was
observed relative to the reference case for 20% and 40% gas extraction
respectively). The explanation was found in the lateral bubble distribution and
particle circulation patterns. During gas addition, the bubbles are split up and
distributed towards both membranes. The particle circulation therefore inverts, and
particles move upwards with the bubbles via the sides, and downward through the
center of the bed. During gas extraction, on the other hand, stagnant zones near the
membranes emerge. These zones force upwards moving bubbles and particles, as
well as downwards moving particles towards the center of the fluidized bed, which
results in bubbles that are vertically stretched and therefore slightly larger than in the
reference case. The experimental findings have shown a large effect of gas
extraction or addition on the fluidized bed hydrodynamics, which should be properly
taken into account in the optimization and design of membrane-assisted fluidized
bed reactors.
It would be interesting to validate the conclusions from this work in 3D systems, but
these systems require different measuring techniques. In the near future, we will
compare the obtained results to numerical simulations with a Euler-Euler model.
Furthermore, the hydrodynamics in a fluidized bed with a membrane configuration
consisting of horizontal membrane tubes instead of vertical membranes will be
investigated both numerically as well as experimentally in order to derive improved
design rules for future fluidized bed membrane reactors.
ACKNOWLEDGEMENT
We gratefully acknowledge SenterNovem, the agency for sustainability and

innovation within the Dutch Ministry of Economic Affairs, for its financial support of
this project.
NOTATION
U gas velocity [m/s]

Umf minimum fluidization velocity [m/s]
REFERENCES
1. Adris, A.M., Elnashaie, S.S.E.H., and Hughes, R., 1991. A Fluidized-Bed Membrane
Reactor for the Steam Reforming of Methane. Canadian Journal of Chemical Engineering
69, 1061-1070
2. Mleczko, L., Ostrowski, T., and Wurzel, T., 1996. A fluidised-bed membrane reactor for
the catalytic partial oxidation of methane to synthesis gas. Chemical Engineering Science
51, 3187-3192
3. Grace, J., Elnashaie, S.S.E.H., and Lim, C.J., 2005. Hydrogen production in fluidized
beds with in-situ membranes. International Journal of Chemical Reactor Engineering 3,
4. Gallucci, F., Annaland, M.V., and Kuipers, J.A.M., 2009. Autothermal reforming of
methane with integrated CO2 capture in novel fluidized bed membrane reactors. Asia-
Pacific Journal of Chemical Engineering 4, 334-344
5. Al-Sherehy, F., Grace, J.R., and Adris, A.E.M., 2005. The influence of distributed reactant
injection along the height of a fluidized bed reactor. Chemical Engineering Science 60,
7121-7130
6. Deshmukh, S.A.R.K., Annaland, M.V., and Kuipers, J.A.M., 2007. Gas back-mixing
studies in membrane assisted bubbling fluidized beds. Chemical Engineering Science 62,
4095-4111
7. Christensen, D., Vervloet, D., Nijenhuis, J., van Wachem, B.G.M., van Ommen, J.R., and
Coppens, M.O., 2008. Insights in distributed secondary gas injection in a bubbling
fluidized bed via discrete particle simulations. Powder Technology 183, 454-466
8. Laverman, J.A., Roghair, I., Annaland, M.V., and Kuipers, H., 2008. Investigation into the
hydrodynamics of gas-solid fluidized beds using particle image velocimetry coupled with
digital image analysis. Canadian Journal of Chemical Engineering 86, 523-535
UOP FCC INNOVATIONS DEVELOPED USING SOPHISTICATED ENGINEERING
TOOLS
Lisa M. Wolschlag and Keith A. Couch

UOP LLC, a Honeywell Company
Des Plaines, Illinois, USA
INTRODUCTION
Fluid Catalytic Cracking (FCC) technology has been a part of the petroleum industry since the
1940’s. Yet, despite being a very mature technology, continued development is vital, especially
as many refiners move their FCC operations from fuels production to higher value products.
Advanced diagnostic and design tools are accelerating process developments and have
resulted in several innovations.
Through the development and commercialization of world record scale FCC units, technical
discoveries have emerged, which have provided opportunities for improvements across all units,
independent of size. Through the development and use of sophisticated engineering tools such
as Computational Fluid Dynamic (CFD) modeling, combined with radioactive tracer and
tomography, physical inspection reports and commercial yield analysis, new technological
innovations can be delivered more confidently, faster and with reduced risk.
This paper will highlight advancements in regenerator technology for higher capacity through
existing assets, emissions reduction and feed distribution systems for large diameter risers. It
will showcase how UOP is using and validating innovative tools to both improve existing FCC
designs and move an aged technology towards true growth opportunities.
DUAL RADIUS FEED DISTRIBUTORS
As refiners look to capitalize on economies of scale, design throughputs of FCC units have
reached record levels. At this scale, opportunities have emerged from the background noise of
the data to improve FCC technology. Through pushing multiple constraints to design limits,
yields and conversion deviated from benchmark performance with gasoline selectivity lower,
conversion lower and dry gas higher than benchmark performance. To get more out of the
existing asset, an intensive program was undertaken to achieve benchmark performance.
The riser for a particular FCC Unit has an inner diameter (ID) of 2 meters (6.6 feet) at the point
of feed injection, which expands to 2.7 meters (9 feet) immediately above. The feed is injected
into the riser through a set of circumferentially positioned distributors. The combination of low
1
conversion and high dry gas yield seems counter-intuitive given traditional FCC operations. A
hypothesis was raised that the large riser diameter might be preventing the feed from
adequately distributing across the full cross-sectional area of the riser. To help test this
hypothesis, a CFD model of the riser was created to analyze the fluid dynamics of the system.
The results of the model supported the theory that raw oil feed would only penetrate the riser a
finite distance thus creating a vapor annulus, and that much of the catalyst flowing up the riser
would form a high density core.
Based on CFD results, a tomographic analysis (gamma scan) of the riser was completed. The
scan results confirmed the CFD model prediction, as illustrated in Fig. 1.
Figure 1. CFD Prediction and Gamma Scan of 2 meter (6.6 foot) ID Riser
Actual Riser
CFD Prediction Gamma Scan
0.9
0.8
0.7
0.6
0.5
0.4
0.3
27-30
0.2 24-27
0.1 21-24
18-21
0
15-18
-0.1 12-15
-0.2 9-12
6-9
-0.3
3-6
-0.4
0-3
-0.5
-0.6
-0.7
-0.8
-0.9
-0.9
-0.8
-0.7
-0.6
-0.5
-0.4
-0.3
-0.2
-0.1
0.1
0.2
0.3
0.4
0.5
0.6
0.7
0.8
0.9
0
lb/ft3
Radioactive tracer work was also completed on the 2 meter (6.6 foot) ID riser. Irradiated
Krypton-79 gas was injected into the riser base. Detectors were positioned along the riser length
and reactor to measure the tracer as it moved through the system. The results indicated that the
time of flight of the krypton gas from one detector to another did not provide a sharp response
peak. Rather, there was an early peak followed by a secondary peak and a high degree of
skewness (Fig. 2).
A mathematical evaluation was performed to determine what type of continuous stirred tank
reactor (CSTR) response would be needed to emulate the measured data. To accurately
reproduce the field data plot, required a composite plot combining the 100, 40 and 15 CSTR
responses (Fig. 2).
Unit performance, CFD modeling, tracer and tomography tests, and mathematical analysis all
indicated the same pathology: that the feed was not adequately accessing the full cross-
sectional area of the riser leading to the presence of a high density core of catalyst and a low
2
Figure 2. Mathematical Composite
14 Mar 2007 Gas Injection

1000
Early Peak Centroid 77.18s
Feed Plug t-res = 1.32s
800 Velocity 9.3 m/s Riser Ex Top – Avg
Flow Core?
40 – CSTR Response
Response
Composite
600 100 – CSTR Response
15 – CSTR Response
400 Late Peak

Wall Holdup?
200
0
0.0 1.0 2.0 3.0 4.0 5.0 6.0 7.0
Seconds
density annulus which caused low conversion and high dry gas and coke make. One solution to
this problem would be to install two, smaller diameter risers to match more conventional FCC
sizes. However, installing dual risers, even with a new construction is substantially more
expensive. For an FCC Unit of 200,000 barrels per stream day (BPSD), the estimated cost
difference between a single, large-radius riser and a pair of smaller risers was estimated to cost
$60 million, in 1998 US Dollars.
UOP has developed a substantially lower cost solution with implementation of dual radius feed
distributors (Fig. 3). This design helps ensure optimal feed distribution across the entire riser,
while avoiding adjacent spray impact that could cause undesirable spray interference.
Another CFD model that now incorporated the dual radius feed distributors was created. Fig. 4
shows catalyst density profiles of an axial slice of the riser, both with and without dual radius
feed distributors. The riser on the left side without the dual radius feed distributors show the high
density core of catalyst, the CFD model with the dual radius feed distributors indicates that the
dense core of catalyst is effectively eliminated.
The dual radius feed distributors were installed on an FCC Unit designed with a 2.4 meter (8
foot) diameter riser. The unit was commissioned in May 2009. Results indicate that dry gas
yield, conversion and gasoline selectivity are all within expectations. The riser’s gamma scans
3
Figure 3. Dual Radius Feed Distributors Schematic
indicate that the high density core of catalyst was effectively eliminated. The catalyst density
profile of the riser at approximately 1 pipe diameter above the point of dual radius feed injection
indicates that core annular flow has been achieved with a very evenly distributed catalyst
density profile (Fig. 5). Additional tomography scans were completed at varying feed ratios, to
optimize the distribution of oil and steam across the riser.
SPENT CATALYST DISTRIBUTOR
PROBLEM
The Engineering tools and associated skills used to solve the previous problems on very large
FCC Units can be used on FCC Units of all sizes and types, to support operating and reliability
needs of individual refiners. In one example, an 80,000 BPSD FCC Unit with a bubbling bed
regenerator exhibited a regenerator cyclone outlet temperature differential of 56°C (100°F) from
one side of the regenerator to the other. This afterburn differential resulted in a localized hot
spot that limited the throughput of the unit against a main air blower constraint. The regenerator
was an older design that employed a gull wing spent catalyst distributor design. Catalyst
maldistribution in the regenerator causes fuel rich areas in the dense phase with localized hot
spots directly above in the dilute phase. Hot spots can be completely invisible within a unit
depending on where the TI instrumentation is placed in relation to the spent catalyst inlet.
4
Figure 4. CFD Models of the Riser Catalyst Profiles with and without Dual Radius Feed
Distributors
Dual Radius
Feed
Distribution
Eliminates
Dense Core
lb/ft3
Figure 5. Gamma Scan of 2.4 meter (8 Foot) ID Riser with Dual Radius Feed Distributors
Design Ratio
5
To validate the temperature data, catalyst tracer work was completed on the regenerator to
evaluate the flow distribution in the unit. With ideal distribution, a radar plot of the detector
signals would show perfect symmetry. The actual unit data showed that the catalyst was heavily
skewed to one side, which was not a surprise (Fig. 6).
Figure 6. Catalyst Tracer Results for Bubbling Bed Regenerator with Gull Wing Design
Cyclone 10 14%
Cyclone 1
12%
Cyclone 9 10%
8%
6% Cyclone 2
4%
2%
0%
Cyclone 3
Cyclone 7
Cyclone 4
Cyclone 6
Cyclone 5
SOLUTION
The typical spent catalyst distributor installed in a bubbling bed regenerator of this vintage was
the gull wing design with an external lift riser. A schematic of this distributor is shown in Fig. 7.
Air maldistribution in this type of regenerator design results from two sources. First, the external
riser lift air discharges vertically out of the disengager, resulting in an oxygen rich environment
in the dilute phase. Second, the high localized catalyst density and resultant hydraulic head
causes preferential flow of combustion air to the opposite side of the regenerator.
To achieve a more even catalyst density and uniform coke distribution, the piped spent catalyst
distributor was developed (Fig. 7). The piped distributor was designed to radially distribute both
the lift air and spent catalyst across the regenerator bed through a set of side arms. The size
and orientation of the distributor arms were designed in an iterative process with CFD modeling
to ensure as even catalyst and air distribution as possible within the back pressure limitations of
the existing lift air blower.
CFD models of the gull wing distributor and the piped spent catalyst distributor were created to
predict the catalyst distribution, gas flow paths and bed density profiles in the bubbling bed
regenerator. With the gull wing distributor, the catalyst was concentrated in the center of the
6
bed. With the piped spent catalyst distributor, the catalyst distribution was much more uniform
throughout the bed (Fig. 8).
Figure 7. Gull Wing and Piped Spent Catalyst Distributors
Gull Wing Piped Spent

Distributor Catalyst
Distributor
RESULTS
The piped spent catalyst distributor was commissioned in December 2006. Post-revamp tracer
tests were conducted on the regenerator to evaluate the results of the design. The actual
catalyst distribution is very close to the ideal distribution (Fig. 9).
Operational data also indicates a significant improvement in the regenerator performance. The
dilute phase temperature differential was reduced from 56°C (100°F) pre-revamp to about 8°C
(15°F) following the implementation of the pipe spent catalyst distributor. As a result, the refiner
was able to lower the excess oxygen level in the flue gas from a pre-revamp minimum of 2
mol% to a post-revamp 1 mol%, enabling a higher capacity through existing assets and saving
on utility consumption.
7
Figure 8. CFD Model of the Catalyst Densities in a Regenerator with Gull Wing and Piped
Spent Catalyst Distributors
Gull Wing Piped Distributor
Figure 9. Catalyst Tracer Results for Bubbling Bed Regenerator with Piped Spent Catalyst
Distributor
14.00%
12.00%
10.00%
8.00%
6.00%
4.00%
2.00%
0.00%
NOTATION
t-res residence time
8
REMOVAL OF NITRATE FROM WATER USING A FLUIDIZED
BED ION EXCHANGE COLUMN
Ammar Arab Beddai and V.V.Basava Rao
Universaity College of Technology,
Osmania University
Hyderabad-500 007
Email: ammararab77@yahoo.com
Email: drbasavarao@yahoo.com
ABSTRACT
Experimental and theoretical studies were carried out to investigate the performance of
a fluidized bed ion exchange system to remove nitrate. The exchange of nitrate on
strong anion exchange resin (TULSION A-27) was studied in the flow rate range of 2 to
7 L/h. Nitrate removal was done at five conditions of the expanded bed height (Z). The
results showed that the experimental data can be fitted to Richardson and Zaki
equation, and the comparison between the experimental and calculated terminal
velocities showed low relative error.
INTRODUCTION
Increased levels of nitrate in ground water have made many wells unsuitable as
sources for drinking water. Nitrate is so toxic, especially to pregnant women and infants,
that the USEPA (United States Environmental Protection Agency) standard of 10 mg
NO3—N/L or less in drinking water was established for human health [Taekyung et al
(1); Kavita et al (2); Lucija et al (3)]. Ion exchange is a chemical treatment process used
to remove unwanted ionic species from wastewater [M. Matosic et al (4); Robert Kunin
(5); Ammar Arab (6)].
Solid-liquid fluidized beds (SLFB) are used in industry for hydrometallurgical operations,
catalytic cracking, chromatographic separation, ion exchange, adsorption, crystallization
and sedimentation, etc [Prakash and Jyeshtharaj (7); Srikuma et al (8)]. However, the
packed bed ion exchange process has some disadvantages such as high pressure drop
and bed clogging. These disadvantages can be eliminated if the packed bed is replaced
by a fluidized bed [Shyh-Jye and Wen-Jang (9); Hideaki et al (10); Seung-Jai et al (11)].
The purpose of this study was to investigate nitrate removal in a liquid-solid fluidized
bed ion-exchange system. The effects of operating parameters including liquid flow rate
and height of the bed on the removal rate of nitrate were studied. The experimental
data of voidage versus superficial velocity were successfully correlated using the
Richardson-Zaki Equation.
1
THEORY OF FLUIDIZED BED
Minimum fluidization velocity
The minimum fluidization velocity can be obtained using the Ergun Equation by sitting
the pressure drop equal to the pressure required to suspend the bed or the weight of
the bed divided by the cross sectional area [McCabe et al (12); Vassilis et al (13)]:
150m u 1- e 1.75r u 2fm 1 u rd
fm fm
+ = g (r p - r ) (1) and Re fm =
fm p
(2)
F d
2
s
2
p e 3
fm F s d p e 3fm m
Estimation of bed voidage (ε)
Bed voidage was obtained by substitution of data into the following equation [Mohsen et
al (14)]:
é Vpù é Vp ù é mp ù
e = ê1 - ú = ê1 - ú = ê1 - ú (3)
ë V L û ë A T .H û ëê r p . A T .H úû
Bed expansion characteristics
Before processing with feedstock, determination of the bed expansion characteristics

was necessary. It was decided to use the well-known Richardson–Zaki Equation
[Mohsen et al (14)]:
U
= e n
(4 )
U t
1- e
The expanded bed height is [Inglezakis and Poulopoulos (15)]: Z f =Z (5)
1- e f
The average bed voidage can be estimated from Eq. (3) or the following equation:
Z
e f = 1 - (1 - e ) (6)
Zf
Where ε0=0.41 is the packed-bed voidage. Values of the Richardson–Zaki coefficients

n, and the apparent terminal velocities of the particles Ut were calculated from linear
regression of plots of ln(U) versus ln(ε). For the particles which had a mean diameter of
750 μm, the apparent terminal velocities of the particles Ut were calculated from Allen’s
equation, Eq. (7). For adsorbents with an approximate mean particle size of 200 μm
one can calculate Ut using Stokes’ law. Ut Stokes is given by Eq. (8) [Mohsen et al
(14)].
d p (r p - r )g g (r - r )d 2
U t = 0.27 Re t0.4 (7 ) U t - stokes =

p p
(8)
r 18m
2
Where (n) is the index which depends on the particle size and sedimentation velocity.
The expansion index (n) was calculated by following equations [Yong-Hong et al (16)]:
n = 4.65 Re t < 0.2
n = 4.4 Re - 0 .03
0.2 < Re t < 1
t (9)
n = 4.4 Re t- 0.1 1 < Re t < 500
n = 2. 4 500 < Re t
The expansion behavior can also be estimated from empirical considerations.

Hartmann obtained a good fit of their experimental data for n using Eq. (10) [Mohsen et
al (14)].
5.09 + 0.2309 Re t0.877
n = (10)
1 + 0.104 Re t0.877
The model of Shiller and Naumann is commonly used for the prediction of terminal
velocity of a spherical particle [M.H.Shahavi et al (17)]:
G a = 18 Re t + 2.7 Re1t .687 3.6 < G a < 10 5 (11)
Where the Grashof number is given by the following equation:
r (r p - r )gd 3
Ga =
p
(12)
m 2
The fluidization behavior of particles is based on the Gallileo number [Vassilis et al

(13)]:
r p g (r p - r )d 3
Ga =
p
(13)
m 2
From Ga the terminal velocity Reynolds number can be calculated for different column
and particle diameters:
-1 -1
é 23 0. 6 ù é dpù
Re t = ê + 0 .5 ú ê
1 + 2.35 ú (14)
ë Ga Ga û ë dc û
The expansion index was estimated from Ga:

5 .1 - n
= 0.016Ga 0.67
(15)
n - 2 .4
For the relatively large particles (of several millimeters) in water, the equation proposed
by Lewis, Gilliland, and Bauer can be used to calculate bed [voidage Inglezakis and
Poulopoulos (15)]:
1/ m
éu ù
e f =ê s ú e (16 )
ëê u fm úû
3
The exponent m is a function of the particle Reynolds number based on the minimum
fluidization velocity. It can be estimated by the following correlation:
m = 4.21 Re -fm0.0804 (17 )
The value of m is between 4.2 and 4.5 for 0.1<Refm<1 and between 2.5 and 4.2 for
1<Refm<1000.
Pavlov (1979) gave a simpler equation for εf based on the Archimedes number:
0.21
æ 18 Re p + 0.3 Re 2p ö d 3p r ( r - r )g
e f =ç
ç
÷
÷
(18) Where Ar =
p
(19)
è Ar ø m 2
MATERIALS AND METHODS
Resin Material
The ion-exchange resin employed was the OH-1 type TULSION A-27 which was a
strong base anion exchange resin. TULSION A-27 (OH-1) was obtained from the
Thermax Company. The particles are in the shape of almost perfect spheres with an
average diameter 0.7 mm (700 µm) and a wet density of 1.08 g/mL. The capacity of the
resin was measured from the breakthrough curve of the OH-/NO-3 exchange
experiments. The total exchange capacity was about 1.2 meq/ml of resin.
Fluidized Bed System
The overall experimental apparatus is depicted in Figure 1. The column was filled with
resin and washed with distilled water. Experiments were carried out in a glass column
having 1 cm diameter and 100 cm high. To obtain the hydroxide, the resins were
regenerated in downflow with four bed volumes of 4% NaOH solution and washed with
distilled water. The temperature was maintained at 31 ± 1 oC. As the fluidized bed
showed a quiescent behavior, the height of the bed could be determined visually.
6
1
7
2 5
3 4
Figure 1. Experimental system: (1) NaNO3,(2) H2O,(3) NaOH ,(4) pump,

(5) rotameter, (6)column, (7)resin, and (8)effluent.
4
CHEMICAL ANALYSIS
Nitrates were measured by a UV-Vis spectrophotometer. The absorbance was

measured at 220 nm and a second reading was taken at 275 nm. This allowed
correction for the interference due to dissolved organic matter. The difference between
the two absorbance measurements was then calculated by the formula [Andre (18)]:
Abs220 - 2*(Abs275) (20)
The effect of Reynolds number on fluidization voidage is presented in Figure 2. Values

of the Richardson-Zaki coefficients n, and the apparent terminal velocity of the particle
were calculated from linear regression of the plots of log (U) versus log(ε), and the
results are shown in Figure (3). The parameters correlated are listed in Table 1. An
experimental value of n=3.0007 was obtained. The theoretical values of n were
calculated by Equations 9, 10, and 15. A comparison of results showed a good
agreement between the experimental and theoretical values of n and Ut. This
comparison showed the operation of bed agreed with theory. The diffusion of nitrate ion
with a resin particle at height 2 cm was slower than that at 3, 6, and 10 cm in the bed.
1
0.8
εf 0.6
0.4
0.2
0
0 5 Rep 10 15
Figure 2. Effect of Rep on fluidized bed
voidage (εf)
y = 3.0007x + 0.3349 0.2

R2 = 0.9759 0.1
0 log εf
-0.2 -0.15 -0.1 -0.05 -0.1 0
-0.2
log u
Figure 3. Richardson-zaki correlation between flow
velocity and bed voidage for determination of n and Ut
5
Table 1. Experimental and theoretical values of Ut and n.
Ut (cm/s) n
Experimental Eq. (7) Experimental Eq. (9) Eq. (10) Eq. (15)
2.162 2.16 3.0007 3.261 3.4 2.68
Figure (4) shows a comparison of the voidage estimated by various models at different
particle Reynolds numbers. Figure (5) shows the experimental breakthrough curves at
various bed heights.
0.8 EXP.
Eq. (16)
Eq.(18)
0.6
εf Eq. (10)
Eq. (15)
0.4
Eq. (9)
0.2
0
0 5 10 15
Rep
Figure 4. Comparison of overall voidage
estimation models with experimental data
1.2
1 10 cm
C/C0 2 cm
0.8 3 cm
6 cm
0.6
0.4
0.2
0
0 20 40 60 80 100
Time (min)
Figure 5. Breakthrough curves of NO3 ions in the fluidized bed
at different bed heights Z and a constant flow rate of 2 L/h
6
CONCLUSIONS
An experimental study of NO3 removal from water by using a fluidized bed was carried
out, and the following conclusion were made:
1- The Richardson and Zaki model showed a good fit with the experimental data,
and can be use for voidage estimation.
2- Results of a fluidized bed operation using an ion exchange resin indicate that
nitrate removal was improved significantly by increasing the bed height.
ACKNOWLEDGEMENT
The authors wish to acknowledge a research grant-in-aid from the Osmania

University, Hyderabad, India.
NOTATION
Abs absorbance measurements

Ar Archimedes number
AT area of the cross-section of the column (m2)
C concentration (mol/m3)
Co initial concentration (mol/m3)
dp particle diameter (m)
g gravity (m2/s)
Ga Gallileo number
Ga Grashof number
H bed height (m)
mp mass of particles (kg)
Refm minimum fluidization Reynolds number
Rep particle Reynolds number
Ret terminal velocity Reynolds number
ufm minimum fluidization velocity (m/s)
us superficial fluid velocity (m/s)
U fluid velocity (m/s)
Ut terminal fluid velocity (m/s)
VL liquid volume (m3)
Vp particle volume (m3)
Z bed height (m)
Zf bed height at fluidization (m)
ε bed voidage
εf voidage at fluidization.
εfm voidage at minimum fluidization
µ dynamic viscosity of the fluid (Kg/m.s)
ρ density of the fluid (kg/m3)
ρp density of the particles (Kg/m3)
Фs the spherity of the particle
7
REFRENCES
1-Taekyung Yoon, Zang HoShon, Gangchoon Lee, Byunghyun Moon, Byeongil Noh
and Nakchang Sung, Korean J. Chem. Eng., 18(2), 170-177 (2001).
2-Kavita Batheja, A.K. Sinha and Gita Seth, Asian J. Exp. Sci., Vol. 23, No. 1, 2009; 61-
66.
3-Lucija Foglar, Laszlo Sipos, Nenad Bolf, World J Microbiol Biotechnol (2007)
23:1595-1603.
4-M. Matosic, Mijatovic, and E. Hodzic, Chem. Biochem. Eng. Q. 14 (4) 141-146 (2000).
5-Robert Kunin, “ Ion Exchange Resins”, Rohm and hass company, Philadelphia,
Pennsylvania, 1958.
6-Ammar Arab Beddai, “Water treatment of Cooling Towers Blowdown from Dissolved
salts”, M.Sc. Thesis, Baghdad University, 2002.
7-Prakash V. Chavan and Jyeshtharaj B. Joshi, Ind. Eng. Chem. Res., Vol. 47, No. 21,
8458-8470, 2008.
8-Srikuma V. Murli, Prakash V. Chavan and Jyeshtharaj B. Joshi, Ind. Eng. Chem.
Res., Vol. 46, No. 6, 1836-1842, 2007.
9-Shyh-Jye Hwang and Wen-Jang Lu, Ind. Eng. Chem. Res., Vol. 34, No. 4, 1434-
1439, 2008.
10-Hideaki Tokuyama, Susumu Nii, Fumio Kawaizumi, and Katsuroku Takahashi,
Ind. Eng. Chem. Res., Vol. 41, 3447-3453, 2002.
11-Seung-Jai Kim, Kyung-Ran Hwang,Sung-YongCho and Hee Moon, Korean J.
chem.. Eng., 16(5), 664-669, (1999).
12-McCabe, Smith, and Harriot, Unit Operation of Chemical Engineering, 1993.
13-Vassilis J. Inglezakis, Marinos Stylianou, Maria Loizidou, International Journal of
Chemical Reactor Engineering, Vol. 8, 1-17, 2010.
14-Mohsen Jahanshahi, Ghasem Najafpour, Melika Ebrahimpour, Solmaz Hajizadeh,
and Mohammad H. Shahavi, Phys. Status Solidi C, 1-8 (2009).
15-V.J.Inglezakis and S.G. Poulopoulos, Adsorption, Ion Exchange and Catalysis
Design of Operations and Environmental Applications, 2006.
16-Yong-Hong Liu, Yan-Ling He, Shu-Cheng Yang, and Chun-Jiang An, Water SA, Vol.
32, No. 4, 555-560, October 2006.
17-M.H.Shahavi, G.D. Najafpour, and M.Jahanshahi, African Journal of Biotechnology,
Vol. 7(23), pp. 4336-4344, 3 December 2008.
18-Andre D. Eaton, Leonore S. Clesceri, Eugene W. Rice and Arnold E. Greenberg,”
Standared Methods for the Examination of Water and Wastewater”, American Public
Health Association (APHA), American Water Works Association (AWWA) & Water
Environment Federation (WEF), 2005.
8
PARTICLE-FLUID FLOW SIMULATION OF AN FCC
REGENERATOR
Sam Clark
CPFD Software, LLC
10899 Montgomery Blvd. NE, Suite A
Albuquerque, NM 87111
sam@cpfd-software.com
ABSTRACT
A particle-fluid flow simulation of a commercial-scale fluidized catalytic cracking unit

has been conducted. The simulation was full-scale, three-dimensional, and with
complex internal geometries. The focus of the computational model was to predict
wear on internal structures. The geometry of the particle feed pipe was found to
cause asymmetric flow of high-speed gas which led to significant wear.
INTRODUCTION
A particle-fluid flow simulation of a commercial-scale fluidized catalytic cracking

(FCC) unit has been conducted using CPFD's Barracuda software. Barracuda is
based on a multi-phase particle-in-cell (MP-PIC) implementation of computational
particle fluid dynamics (CPFD), which uses an Eulerian scheme for the fluid field and
a Lagrangian scheme for the particles. For the sake of brevity, the current paper
does not go into the numerical details of the CPFD method, and the reader
interested in such details is directed instead to Andrews and O’Rourke (1) and
Snider (2).
The regenerator simulation was full-scale, three-dimensional, and with complex

internal geometries. The geometry was generic, i.e. the simulation was not of any
actual operating FCC unit. Though chemistry can be included in Barracuda models,
as shown by Snider and Banerjee (3) and Snider, Clark, and O’Rourke (4), the
current simulation was isothermal, and did not include chemical reaction
calculations. The hydrodynamic behavior was of primary interest, so thermal and
chemical effects were neglected.
The simulation was run to quasi-steady state operating conditions, and both transient
and time-average data were collected. The results of the simulation included
prediction of fluidization characteristics, wear on internal structures due to particle
impact, and entrainment of solids into cyclones. It was found that an asymmetric
feed pipe geometry was the reason for the extreme wear observed on specific
internal structures.
GEOMETRY AND OPERATING CONDITIONS
The physical configuration and operating conditions of the FCC regenerator in the
current simulation were chosen to be generically representative of what might be
found in industry. Fig. 1 shows the geometry of the regenerator, which was a
cylindrical vessel with domed bottom and top, a diameter of 15.2 m (50 ft), and an
overall height of 29.0 m (95 ft). The bottom portion of the vessel was equipped with
three gas distribution rings to provide fluidizing gas. Twelve primary-secondary
cyclone pairs were positioned in the top portion of the vessel, and each cyclone had
a dipleg extending down to return entrained particles to the fluidized bed. The
regenerator was also equipped with a single standpipe, which in an operating system
would allow particles to be discharged back to the FCC reactor.
Figure 1: Geometry and boundary conditions for the FCC regenerator
The geometry of the FCC catalyst particle feed pipe was of particular interest in the
current simulation. The horizontal pipe led to an upwardly curved “J-bend”, which
transitioned to a vertical riser section. This type of “J-bend” configuration is
necessary for reactor-regenerator configurations where the units are side-by-side,
and the FCC catalyst particles must be transported horizontally from the reactor to
the regenerator. In other reactor system designs, the reactor might be positioned
directly above the regenerator, and a “J-bend” would not be necessary.
Particles exiting the vertical riser section of the feed pipe impacted a flat plate
positioned above the pipe outlet. This plate was used as a crude termination device
for the purposes of the current simulation. In operating FCC regenerators, more
sophisticated termination devices are used. These more complex designs attempt to
distribute particles more evenly into the fluidized bed, which leads to better
regeneration of the catalyst. For the purposes of the current generic geometry, it was
not necessary to use a more sophisticated termination device.
As approximations of typical operating conditions, the values shown in Table 1 were

used in the current simulation.
Table 1: FCC operating conditions

Parameter Value
Freeboard pressure 203 kPa (2 atm)
Temperature (isothermal) 994 K (1330 °F)
FCC catalyst particle density 1,425 kg/m3 (89 lb/ft3)
FCC catalyst d50 particle diameter 78 microns
Initial bed catalyst particle mass 70,000 kg (77 tons)
Superficial velocity in fluidized bed 0.42 m/s (1.4 ft/s)
SIMULATION SETUP
Computational Grid and Particles
The first step of the simulation process was the definition of a computational grid.
The computational cells defined by the grid are used to solve the fluid transport
equations, the results of which are strongly coupled with particle momentum
equations. A finer grid gives higher fidelity in the computational solution, but requires
a longer calculation time. Barracuda uses a regular rectangular grid. The grid used
for the current simulation had computational cells with side-lengths ranging from 15
to 46 cm (6 to 18 inches) throughout most of the domain. The computational grid
contained 270,000 real cells.
In a large commercial vessel such as the regenerator currently under consideration,

there could be on the order of 1015 individual particles in the system. With current
computers, it is not feasible to model the detailed motion of this many individual
particles in a simulation. Barracuda uses so-called computational particles, which
allows for useful engineering results in reasonable solution times. Each
computational particle represents a group of real particles that share physical
properties such as material, radius, and density. The number of computational
particles used the simulation affects the accuracy of the results. As with the grid,
using more computational particles gives more accuracy, but also requires longer
run-times. In the current simulation, about 1.8 million computational particles were
used.
Initial and Boundary Conditions
Barracuda solves for the motion of particles and fluid by solving conservation
equations for all computational cells and particles in the simulation (2). The initial
conditions provide a starting point for all calculations, while the boundary conditions
(BCs) specify where fluids and particles are entering or leaving the system. Fig. 1
shows the regenerator geometry with BC definitions. The initial condition for the
simulation was specified such that the regenerator was filled to a target level with
FCC catalyst particles at rest. The fluid, air, was also at rest. The pressure and
temperature of the system were set to match the desired operating conditions.
Flow BCs that brought in only gas were defined for the fluidizing air rings. Flow BCs
that brought in both gas and particles were defined at the bottoms of the primary
cyclone diplegs and at the FCC catalyst particle feed at the end of the feed pipe.
Pressure BCs were defined at the inlet horns of the primary cyclones and at the
bottom of the standpipe. Particles were allowed to exit at all pressure BCs, and the
overall system mass was maintained at a constant value by using a particle feed
controller, which adjusted the flow rate of particles at the cyclone diplegs as needed
to maintain a constant system mass.
Wear Due to Particle Impact
Estimating the expected wear on internal structures was an important goal of the
simulation, so the Barracuda wear model was used. The wear model calculates the
cumulative wear due to impact of particles on all wall surfaces in the simulation.
Research has shown that the damage to a surface from particle impacts is
dependent on factors such as particle mass, velocity, and angle of incidence (5). In
the Barracuda wear model, when a particle hits a wall, the wear due to this impact is
calculated based on the particle mass, velocity, and angle of incidence. The user has
control over the dependence on each of these factors, and the appropriate values for
each are material-specific. For example, FCC catalyst particles impacting bare metal
would have different values for the calculation parameters than FCC catalyst
particles impacting refractory. For the current simulation, the particle mass, m, and
velocity, u, terms contributed to the calculated wear as m1.5 and u3.5.
RESULTS
The simulation was set up to collect various types of data, including transient
pressure at specific locations, time-averaged gas and particle mass fluxes, and
particle residence times for FCC catalyst particles entering through the feed pipe.
Many aspects of the system could be examined based on the available data, but this
study was focused specifically on two related behaviors shown by the simulation:
flow of particles and gas around the “J-bend” in the feed pipe, and high wear on
internal cyclone diplegs in one half of the regenerator.
Transporting FCC catalyst particles horizontally is necessary in situations where the

reactor and regenerator vessels sit side-by-side. In the current simulation, the FCC
catalyst particles being fed to the regenerator traveled through the “J-bend” and then
vertically through a riser section before discharging into the regenerator. Ideally,
particles should be dispersed uniformly into the fluidized bed. However, the “J-bend”
geometry causes the particles to pack against the far wall of the bend, which in turn
favors high gas flow rates on the inside portion of the curved section. Figs. 2 and 3
show thin-slice views of particles and gas traveling through the feed pipe. The
particles are colored by speed, with faster moving particles having darker colors. The
gas vectors have their lengths scaled based on gas velocity and are colored with
darker vectors representing higher gas velocity.
The particles which pack up on the far wall of the “J-bend” tend to be low-speed, and
gas prefers to avoid the higher solids concentration region, leading to a high-speed
condition along the inner portion of the curved pipe. The high-velocity gas continues
up the vertical riser section, and exits the feed pipe on the inner-curve side.
Figure 2: Particles colored by speed in the feed pipe
Figure 3: Vectors of gas velocity in the feed pipe

Fig. 4 shows isovolumes of regions where the time-averaged gas velocity is greater
than 5 m/s. The tendency of the high-speed gas to stay on the inner-side of the
curved pipe is shown by the large isovolume structure emanating from the same side
of the feed pipe outlet. Other regions of high fluid velocity include the standpipe area
and the inlet horn areas for the primary cyclones. All of these locations are high flux
regions, and the relatively small open areas compared with the overall cross-
sectional area of the regenerator lead to high gas velocities.
Figure 4: Isovolmues of regions with gas velocity higher than 5 m/s
The high gas velocity on the inner side of the inlet pipe propagates through the
fluidized bed, and the effect is significant on the wear calculated for the cyclone
diplegs on that side of the regenerator. Fig. 5 shows regions where more and
stronger particle impacts occurred. These regions are the most likely to incur
damage from wear due to particles hitting the internal structures of the regenerator.
CONCLUSIONS
The FCC regenerator simulation provided insight into the flow behavior of gas and
solids through the “J-bend” in the feeding pipe. The asymmetric flow of high-speed
gas into the fluidized bed penetrated into the freeboard, and was found to be
responsible for high wear on cyclone diplegs on one particular side of the
regenerator. If this were an operating unit, it would be difficult to identify the
asymmetric flow behavior through typical pressure taps or thermocouples. If the
cyclone diplegs were damaged sufficiently, an emergency shutdown might be
required, which would be very costly. This simulation shows that CPFD modeling can
be applied to large commercial fluid-particle systems to solve performance issues.
Figure 5: Isovolumes of regions with high predicted wear due to particle impact
REFERENCES
1. Andrews, M. J., and O'Rourke, P. J., 1996. The multiphase particle-in-cell (MP-
PIC) method for dense particle flow. Int. J. Multiphase Flow 22, 379-402.
2. Snider, D. M., 2001, An Incompressible three dimensional multiphase particle-in-

cell model for dense particle flows. Journal of Computational Physics 170, 523-
549.
3. Snider, D. M., Banerjee, S., 2009, Heterogeneous gas chemistry in the CPFD
Eulerian–Lagrangian numerical scheme (ozone decomposition). Powder
Technology, http://dx.doi.org/10.1016/j.powtec.2009.04.023
4. Snider, D. M., Clark, S. M., and O’Rourke, P.J., 2011, Eulerian-Lagrangian

method for three dimensional thermal reacting flow with application to coal
gasifiers. Chemical Engineering Science,
http://dx.doi.org/10.1016/j.ces.2010.12.042
5. Mills, D., and Mason, J.S., 1979. Evaluating the conveying capacity and service
life of pipe bends in pneumatic conveying systems. Journal of Powder & Bulk
Solids Technology, 3 (1979) 2; 13-20.
PARTICLE TO GAS HEAT TRANSFER IN A CIRCULATING
FLUIDIZED BED (CFB) RISER
Yassir T. Makkawi
European Bioenergy Research Institute (EBRI), School of Engineering and Applied
Science, Aston University, Birmingham B4 7ET, United Kingdom
T: +44 (0)121 204 3398; E: y.makkawi@aston.ac.uk
ABSTRACT
The main objective of this study was to measure the heat transfer from particle to gas in
a dilute CFB riser (   0.8 ) and to derive a predictive equation for the local particle-gas
heat transfer coefficient. This coefficient was found to be a strong function of the
particle velocity, concentration and length of the heat transfer section. Accordingly, a
new correlation in terms of these parameters is proposed.
INTRODUCTION
Studies on heat transfer in a Circulating Fluidized Bed (CFB) have been mainly focused
on two characteristic heat exchange mechanisms (i) exchange between the wall to gas
or particle (ii) exchange between the gas to particle. While considerable amount of
research has been conducted on the first mechanism, which is relevant to fluidized bed
boilers, limited attention has been paid to the second mechanism. Particle to gas heat
transfer is of particular interest in CFB thermo-chemical processes, such as biomass
thermal conversion and the new emerging technology of chemical looping. In biomass
gasification/pyrolysis, circulating hot particles, such as sand and char, are used to drive
the thermochemical conversion of fresh biomass feed via particle-gas heat exchange.
While in chemical looping, hot metal particles are circulated between two reactors as a
mean for carrying oxygen. This process is also relevant to drying and catalytic reactions.
MOTIVATION OF THIS STUDY
Review of the published literature on heat transfer in dilute-phase suspension, such as

in a CFB riser, indicate considerable uncertainties with respect to heat transfer
coefficient. Table 1 shows two of the most widely used correlations and two recently
developed ones. The literature contain a fairly large number of studies, using the
correlations of Ranz and Marshall (1) and Gunn (2), in the simulation of particle-gas
heat transfer in a CFB, e.g. Xie et al. (3) and Watanabe and Otaka (4).
We recently carried out a numerical simulation, Fluent code (5), to investigate the
particle-gas heat transfer in dense suspension (bubbling bed) and dilute suspension
(CFB riser). Using Gunn’s correlation, the latter case has shown poor agreement with
experimental measurements, while excellent agreement has been noticed for the case
of dense suspension as shown in Fig. 1. The same was observed when applying Ranz
1
and Marshall correlation (1). It should be noted that, in both cases, the hydrodynamics
were in good agreement with the experimental measurement (not shown here).
Table 1. Particle-gas heat transfer correlations

Correlation Author Range
10< Re <104
(a) Nu  2  0.6 Re Pr 0.5
p
0.33
Ranz & Marshall (1)
Pr  0.7
(b)    
Nu  7  10  5 2 1  0.7 Re 0p.2 Pr 0.33  1.33  2.4  1.2 2 Re 0p.7 Pr 0.33
Gunn (2) 0.3<  <1.0
'' 5.3365
7
(c)
Nu  8.295 10 Re p Fm1.3863 Fe 5.0530 Rajan et al. (6) dilute phase
'' 2.7624
4
(d)
Nu  1.336 10 Re p Fm0.6792 Fe 1.8344 Rajan et al. (6) dense phase
Figure 1. Simulation and experiment results of suspension temperature in (a) bubbling bed with
initial cold bed fluidized by hot air and (b) CFB with hot particles inlet and cold fluidizing air.
Rajan et al. (6) recently developed a new correlations for particle-gas heat transfer
coefficient in a vertical pneumatic conveyer operating at low particle to gas flow ratio in
the range of Fm  1.0 . The reported correlations, given in Eq. (c) and Eq. (d) in Table 1,
were derived from data collected at the inlet and exit of the conveyers, thus
representing the overall average performance across the whole conveyer height. The
coefficients were categorized to dilute and dense flow regimes, however the authors did
not give clear cut boundaries between what they call “dense” and “dilute”.
In this study, the main objective was to carry out localized measurements in a CFB riser
operated at low suspension density within the range of   0.8 , this corresponds to a
particle-gas flow ratios of 0.5  Fm  10 . The data was then used to derive a simple
correlation for particle-gas heat transfer coefficient.
2
EXPERIMENTAL
Set-up and Procedure
Fig. 2 shows a schematic diagram of the circulating

fluidized bed, which mainly comprises a 163 cm height
and 5.2 cm diameter riser, connected to a primary and
secondary cyclones and a particle feeding/receiving tank.
The fluidizing air flow rate was measured by two
rotameter, giving a maximum flow rate of 1300 lit/min.
The average suspension temperature and pressure along
the riser were measured by eight thermocouples and
pressure transducers. Two electric heating elements,
wrapped around the particle feeding tank, were used for
heating the particles up to a maximum temperature of 100
ºC. The riser, downer and particle tank were all thermally
insulated to minimize heat losses. Glass beads and sand
in the range of 235 m to 700m were used as the bed
material. The experiment starts by loading the feeding
tank with around 10 kgs of particles. The particles are
then heated to the desired temperature using the electric
heater at a selected set point. At fluidization, the pressure
and temperature of the suspension along the riser
Figure 2. Circulating fluidized bed
were logged at the rate of 1 Hz. The particle mass flow
rate was determined by relating the particle mass to collecting time. To ensure
comprehensive data, a total of 48 different combinations of operating conditions were
considered.
Data Analysis Method
If we assume uniform cross-sectional particle and gas distribution and negligible

downfall of particles at the wall, then local heat transfer coefficients along the riser can
be estimated by dividing the riser to a number of axial segments. Fig. 3 shows a
schematic representation of this method. The heat transfer in each section was
calculated using the measured gas/particle flow rate and temperatures at the end of
each section such that:
q  mg C p , g (Tg ,i 1  Tg ,i )  ms C p , s (Ts ,i 1  Ts ,i ) (1)
The average void fraction (  ) for each bed section of length ( z ) was determined from
pressure drop measurement ( P ) such that,
P
  1
 s   g gz (2)
3
With the available information on temperature and pressure variations along various
sections of the riser, the local particle-gas heat transfer coefficient was determined by
relating the localized heat transfer ( q ) to the particle surface area ( As ) and the
temperature difference between the two phases ( T ) as follows:
q Tg (out) Ts (out)
h (3)
As T
The particles surface area was related to the estimated void
fraction, such that,
Tg (i+1) Ts (i+1)
6(1   )
As  Ac z (4)
ds Section (i)
 z
where Ac is the riser cross-sectional area and d s is the
particle diameter. The heat transfer driving force ( T ) was
given in terms of the log mean temperature as follows: Tg (i) Ts (i)
(Tg ,i  Ts ,i )  (Tg ,i 1  Ts ,i 1 )
T  (5) Ts (in)
log[(Tg ,i  Ts ,i ) (Tg ,i 1  Ts ,i 1 )] ms
In obtaining the particle temperature, we start by assuming Tg (in), mg

that the measured temperature along the riser represents Figure 3. Data analysis method
the suspension temperature or bed temperature (gas
and particle mixture). Hence, this can be expressed
as volume-weighted average temperature:
Tmix  (1   )Ts  Tg (6)
The exit air temperature in each section is obtained
from Eq. 6 as follows:
Tmix ,i 1  (1   i 1 )Ts ,i 1
Tg ,i 1  (7)
(1   i 1 )
Equating both sides of Eq. 1, the exit particle
temperature in each section is given by:
mg C p ,s
Ts ,i 1  Ts ,i  (Tg ,i 1  Tg ,i ) (8)
ms C p , g
Taking   mg C p , g mg C p , g , and substituting Eq. 7
into Eq. 8, gives
Figure 4. Gas and particle
Ts ,i 1 
1
 i   (1   i )

Ts ,i i   (Tmix ,i 1  Tg ,i i )  (9) temperature along the CFB riser.
Inlet particle temp=70 oC, inlet gas
temp=18 oC
4
Variation of Temperature, Pressure and Particle Concentration
Examples of the variations in the temperature, pressure and particle concentration

along the CFB riser are shown in Figs. 4 and 5. These figures typically demonstrate the
great complexity and vast variations in the hydrodynamics and heat transfer in such
system. The temperature profiles shown in Fig. 4 indicate steep variations at the bottom
part of the riser, within the range of ~40 cm above the particle entrance (thermal
entrance length). It is interesting to note that both phases are at thermal equilibrium at
the height of ~140 cm, just few centimeters below the riser exist. However, for higher
particle temperature and particle loading, thermal equilibrium at exit was never reached.
This is expected for such a relatively short riser. The pressure and particle volume
fraction along the riser are shown in Fig. 5. Similarly, the variations are steep at the
dense bottom zone. It is also interesting to note the significant entrance effect on
particle concentration near the particle feeding point (10 cm from bottom). This is of
significant important since most of the heat transfer takes place in this region.
Figure 5. Pressure and particle concentration variations along the riser for glass beads of 700
m diameter at two different operating conditions.
Particle-Gas Heat Transfer Coefficient
Particle-gas heat transfer coefficient in a dilute CFB is believed to be dominated by

particle/gas axial convection. This behavior is rather different than what is observed in
CFB boilers and combustors, where the process is controlled by radial convection and
conduction between the bed and wall. Therefore, in terms of operating conditions, we
are interested in establishing relations between the local heat transfer coefficient and
particle/gas axial velocities and particle concentration.
5
For the range of operating conditions
considered in this study the particle-gas heat
transfer coefficient was found to fall within the
range of 0.1-350. Fig. 6 shows an example of
the variations in heat transfer along the riser.
As expected, rapid heat transfer takes place at
the bottom region, which then decreases
towards the top. The thermal entrance length
increases with increasing the particle to gas
flow ratio. Fig. 7 show the local heat transfer
coefficient as function of the particle
concentration and axial velocity for data
collected from different sections of the riser and
at all range of operating conditions considered.
The cross-sectional local average particle
concentration was obtained from pressure drop
measurements (Eq.2) and the average local Figure 6. particle-gas heat transfer as
particle axial velocity was obtained from function of riser height. Inlet particle
particle mass flux measurement such that: temp=70 oC, inlet gas temp= 18 oC
Gs
us  (10)
(1   )  s
In Fig. 7a, it is observed that the heat transfer coefficient decreases with increasing
particle concentration. This is exactly opposite to CFB wall-bed heat transfer, where the
heat transfer coefficient is directly proportional to particle concentration, mainly due to
the dominated radial conduction and convection through the dense wall layer. In dilute
CFB, the heat transfer mechanism is rather different, dominated by axial convections.
As the particle concentration decreases, gas-particle convection diminishes, but at the
Figure 7. Local heat transfer coefficient as function of particle concentration and velocity
6
same time the gas convection component becomes important. This is consistent with
the observation reported by Rajan et al. (6) and Bandrowski et al. (7), where it is was
shown that the heat transfer coefficient decreases with increasing particle concentration
within the limit of   0.95 . In Fig. 7b the local heat transfer coefficient is observed to
consistently increase with increasing the axial particle velocity.
PROPOSED CORRELATION FOR HEAT TRANSFER COEFFICIENT
The analysis shown in section 4.2 suggests that the local particle-gas heat transfer
coefficient in the CFB riser can be best correlated with particle velocity, concentration
and length of the heat transfer section. Hence, dimensional analysis leads to the
following function:
 (1   ) z 
h  f Re 'p ,  (11)
 ds 
'
where the Reynolds number, Re p , is
expressed in terms of the particle
velocity (i.e.   g u s d s  g ). Using
regression analysis, the following
proposed correlation for heat transfer
coefficient is obtained:
0.924
 (1   ) z 
h  8.4(Re ) ' 0.871
p  
 ds  (12)
Figure 8. Correlation for heat transfer coefficient
This relation is valid for   0.8 and
0.1  Re 'p  200 . Fig. 8 shows the
measured heat transfer coefficient
for all range of operating conditions
considered in the study against the
values obtained from Eq. 12.
Comparison of the measured heat

transfer coefficient and values
obtained from literature correlations
given in Table 1 is shown in Fig. 9.
Generally, the data is scattered;
however, Rajan correlation for dense
phase (Eq. d) appear to give the
closest match with our experimental
Figure 9. Proposed heat transfer coefficient
measurements. The other two
7
correlations, of Gunn (Eq. b) and Rajan for dilute phase (Eq. c), considerably deviates
from our measurements. Results from Eq. (a) are omitted as it gives almost the same
values as that from Gunn correlation.
CONCLUSION
Particle-gas heat transfer coefficient in a dilute CFB riser (   0.8 ) has been found to
be a strong function of the particle axial velocity, concentration and length of the heat
transfer section. A new correlation equation, in terms of these three parameters has
been developed. The present experimental data for particle-gas heat transfer coefficient
has also been compared with selected correlations from the literature. Work is in
progress to extend this correlation to higher temperatures and to incorporate it in Fluent
CFD code for the simulation of a CFB gasifier.
ACKNOWLEDGEMENT
The author acknowledges the help of Mr. Joseph Eke in the experimental runs.
NOTATION
Ac cross-sectional area of the riser (m2) Re’p Reynolds number, =gusds/g
As surface are of particles (m2) Re’’p Reynolds number, =gUds/g
Cp specific heat capacity (J kg-1 K-1) T temperature (oC)
ds particle diameter (m) u velocity (m s-1)
Fe Fedorov number,=ds[4gg2(s/g-1)/3g2]0.3 (-) U superficial gas velocity (m/s)
Fm particle to gas flow ratio (-) z length of heat transfer section (m)
Gs Particle flux (kg m-3 s)  Greek symbols
h particle-gas heat transfer coefficient ( W m-2 K)  density (kg m-3)
m mass flow (kg/s)  void fraction (-)
Nu Nusselt number, =hds/kg (-) 
P pressure (N m-2)  Subscripts
Pr Parndtl number, =Cp/kg (-) g gas
Q heat transfer (W) s particle
REFERENCES
1. Ranz, W. E. Marshall, W. R. (1952). Evaporation from drops, Chem. Eng. Prog. 48 (Part I)
(1952) 141–146.
2. Gunn, D. J. (1978). Transfer of Heat or Mass to Particles in Fixed and Fluidised Beds. Int. J.
Heat Mass Transfer, 21, 467-476.
3. Xie, D., Bowen, B. D., Grace, J. R., Lim, C. J. (2004). Two-dimensional model of heat
transfer in circulating fluidized beds. Part I: Model development and validation, Int. J. of Heat
and Mass Transfer 46 (2003) 2179–2191
4. Watanabe, H. Otaka, M. (2006). Numerical simulation of coal gasification in entrained flow
coal gasifier, Fuel 85, 1935–1943
5. Fluent 6.3, 1996. Fluent 6.3 Users Guide. Lebanon, NH, 1996, Ansys Inc.
6. Rajan, K. S., Dhasandhan, K., Srivastava, S.N., Pitchumani, B. (2008). Studies on gas–solid
heat transfer during pneumatic conveying, Int. J. of Heat and Mass Transfer 51, 2801–2813.
7. Bandrowski, J., Kaczmarzyk, G. (1976). Gas-to-particle heat transfer in vertical pneumatic
conveying of granular materials, Chem. Eng. Sci., 1303–1310.
8
DEM STUDY OF FLUIDIZED BED DYNAMICS DURING PARTICLE
COATING IN A SPOUTED BED APPARATUS
Sergiy Antonyuk, Stefan Heinrich, Anastasia Ershova

Institute of Solids Process Engineering and Particle Technology, Hamburg
University of Technology, Denickestrasse 15, 21073 Hamburg, Germany
T: +49-40-42878-2748; F: +49-40-42878-2678; E: antonyuk@tu-harburg.de
ABSTRACT
A novel process for coating of spherical aerogel particles in a spouted bed is
suggested. Using Discrete Element Method the influence of the density and
restitution coefficient of experimentally coated aerogels on the fluidized bed
dynamics in the developed apparatus was described.
INTRODUCTION
The aerogels are nanoporous materials which show extremely low density, high
surface area and excellent insulation properties. However, the limitation of aerogels
in a number of applications is their open-pore structure, allowing the penetration of
liquids therein. Their structure might be destroyed by contact with water because of
capillary forces which are higher than the strength (Antonyuk et al. (1)). This
drawback could be overcome by coating of aerogels with a polymeric protection
material. In this work the aerogel particles were coated in a spouted bed apparatus.
This technology offers the fluidization of small and light or very large particles, which
can be non-spherical or sticky with a broad size distribution, Mörl et al. (2).
One objective of this work was to produce the coated aerogel particles with good
structural properties. In order to optimize the coating process parameters the
particle and fluid dynamics of spouted bed apparatus was investigated by Discrete
Element Method (DEM) which is coupled with CFD.
EXPERIMENTAL
Experimental Slit-shaped Spouted Fluidized Bed
1
3
process
chamber 2
7 4
6
2 Process air
5
h
Nozzle
air
Coating fluid
Fig. 1 Experimental spouted bed apparatus for the coating of aerogels (left) and its
fluidization chamber (middle and right).
To perform the coating of the aerogels an experimental spouted bed apparatus was
built, Fig. 1, which allows an operation under batch conditions. The pilot plant has a
cylindrical chamber, Item 1, which is connected through a conic part with a prismatic
fluidization chamber, Item 2, with two horizontal gas inlets (slots) for adjustable gas
supply. The velocity of the inlet air can be varied changing the height of these slots
h. The air flow produced from blower, Item 3, can be heated up to 100 °C in a 500 W
heater, Item 4. The solution or melt prepared in the vessel, Item 5, was transported
in a coated hose using a peristaltic pump, Item 6, and injected in the fluidized bed
using a two-component nozzle 7. The nozzle was heated up to temperature of
injecting fluid. A fabric filter, Item 8, separates small particles from the exhaust gas.
The air temperatures before, after and inside the bed (chamber 2), the temperatures
of the liquid and nozzle and pressure drop were measured.
Materials for the Coating Experiments

Fig. 2 shows nearly spherical silica aerogels produced
by supercritical extraction of a gel-oil emulsion
(Alnaief&Smirnova (3)). The particles with the size
ranging from 100 µm to few millimetres and the mean
density of 190 kg/m³ were coated with Eudragit® 200 μm
(solution with 25.8 vol-% of the solid material) which
provides a pH sensitive release of the drugs. Fig. 2 SEM of produced
silica aerogel particles.
Parameter and Results of the Coating Experiments
During the first experiments the high shrinking of aerogels was observed. The
droplets of Eudragit solution destroyed the particle surface of aerogel and their size
decreased (Antonyuk et al. (1)). The Eudragit layer showed many cracks (Fig. 3).
Hence, to avert the breaking of the particles the coating with two materials was
carried out. Firstly the PEG 2000 was sprayed in the apparatus forming a protection
layer on the aerogel. Thereafter the Eudragit® was injected (Fig. 4). The different
process parameters were varied during coating experiments and their optimal
values were obtained, which are summarised in Table 1.
Table 1. Process parameters of the coating.
Parameter PEG 2000 Eudragit® L
process air mass flow in m3/h 25-40 25-40
bed temperature in °C 45 21
mass flow of the coating fluid in g/min 20 10
temperature of the coating fluid in °C 95 25
flow rate of the nozzle air in l/min 15-20 15-20
temperature of the nozzle in °C 80 30
Mechanical Properties of the Aerogels
The mechanical properties characterize the product quality. They are also important
parameters in the calculated here DEM model (Antonyuk et al. (4)). The stiffness
and breakage properties of aerogel were measured by compression tests (Antonyuk
et al. (1)) and presented in Table 2 for the different sizes (uncoated particles with d50
= 0.7 mm and two fractions of coated particles with d50 = 0.8 mm and 3.71 mm with
layer thickness of approximately 50 µm).
Eudragit-Aerogel layer
Aerogel microstructure
10 µm 100 nm
100 µm
Fig. 3 Aerogel particle coated in spouted bed apparatus with Eudragit® L solutions
(left) and the cross section area of the layer (middle and right).
Eudragit®
layer
protection
layer
10 µm
50 µm
Fig. 4 Cross section area of a silica aerogel particle coated with two layers.
Table 2 Mechanical characteristics of aerogels.
Diameter in mm Breakage force in N Strength in kPa Stiffness in N/mm
0.70 ± 0.14 0.37 ± 0.2 970 ± 0.50 10.3 ± 2.0
0.80 ± 0.12 0.33 ± 0.1 650 ± 460 10.0 ± 3.0
3.71 ± 0.40 0.61 ± 0.2 60 ± 30 3.0 ± 0.6
The aerogels with Eudragit shell show smaller strength in comparison with the
uncoated particles. The decreasing of the strength occurs due to damaging of the
particle surface by contact with Eudragit®. No significant influence of the shell on the
particle stiffness was obtained. With the increasing of the particle size (from 0.8 to
3.7 mm) the strength and stiffness decrease.
The impact and rebound behaviour of aerogels before (d50 = 1.5 mm) and after
coating (d50 = 1.7 mm) was analyzed with the help of a free fall set-up (Antonyuk et
al. (8)). The normal coefficients of restitution (euncoated = 0.6±0.13 and ecoated =
0.4±0.16) were measured at the impact velocity range of 1 m/s. They are input
parameters for the DEM model, which will be described in the next paragraph.
MODELLING OF PARTICLE AND FLUID DYNAMICS
DPM Model
A discrete particle model (DPM) was employed to study the particle and fluid
dynamics of spout bed apparatus used for the coating of aerogel. The DPM is a
coupling of the discrete element method (DEM), which describes the motion of every
individual element, and the computational fluid dynamics (CFD), which calculates
the gas phase (van Buijtenen et al. (5), Fries et al. (6)). The motion of each particle i
can completely be described using Newton's and Euler's laws:
r
r Vi β g − p r r r m r
mi
dv i
dt
= −Vi ∇p +
1− ε
( g i ) i + ∑ Fc, j ,i ,
u − v + m g (1)
j =1
r
d ωi
l r
Ii
dt
= ∑M
j =1
i, j . (2)
The force balance on the right side of Eq. (1) consists of the force due to pressure
gradient, drag, gravity and contact forces by a particle-particle and particle-wall
collision, respectively. Ii and ωi in Eq. (2) are the moment of inertia and angular
velocity for particle i. Mi,j are the moments generated from tangential contact forces
acting on the particle i. The interphase momentum transfer coefficient βg-p is
modelled by combining the Ergun equation (1952) for dense regimes (ε ≤ 0.8) and
the correlation proposed by Wen&Yu (1966) for more dilute regimes (ε > 0.8).
Contact forces between particles are calculated according to a viscoelastic contact

model based on the Kelvin-Voigt law with a constant restitution coefficient (Cundall
and Strack (7)). The normal and tangential contact forces are defined as follows:
r r
Fc(,ijn ) = (kc ,ij ,n ⋅ sij ,n + ηij ,n ⋅ s&ij ,n ) ⋅ nij , (3)
r
r ( ij ) (kc ,ij , s ⋅ sija, s + ηij , s ⋅ s&ij , s ) ⋅ tij
Fc , s = min r , (4)
( μij ⋅ Fc(,ijn ) ) ⋅ tij
where kc,ij,n and kc,ij,s are the contact stiffness in normal and shear direction, μij is the
dynamic friction coefficient. The overlap in normal and shear direction is sij,n and sij,s.
ηi,j,n and ηi,j,s are the normal and shear damping given as:
⎡ ⎛ π ⎞⎤
η = 4m* ⋅ kc / ⎢1 + ⎜ ⎟⎥ . (5)
⎣ ⎝ ln e ⎠ ⎦
m* is equivalent mass of contact partners. kc is the contact stiffness. The coefficient
of restitution, e, describes the energy dissipation during impact and can be found as
a ratio of rebound velocity to impact velocity of the particle, Antonyuk et al. (8).
The hydrodynamics of the gas phase considered as continuum is calculated using

volume-averaged Navier-Stokes equations (6)-(7).
∂
∂t
(ερ g ) + ∇ (ερ g ug ) = 0 , (6)
∂
∂t
(ερ g u g ) + ∇ (ερ g u g u g ) = −ε ∇pg − ∇ (ε τ g ) − S p + ερ g g . (7)
Simulations were performed using the commercial simulators EDEM and Fluent.
Simulation Parameters
The geometry of fluidization chamber (2 in Fig. 1) is discretized in mesh cells
(Fig. 5). The mesh consists of 76.725 tet/hybrid cells with an interval size of 0.008
and minimum volume of 4 mm3. The air with the temperature of 25 °C, density of
1.18 kg/m3 and kinematic viscosity of 15.7·10-6 m2/s was calculated. To describe the
effects of turbulent fluctuations of velocities on the pressure drop of the empty
apparatus a k-ε model (with the turbulence intensity of 5%) was applied for the
calculation which showed good results for the spout beds in CFD simulations of
Gryczka et al. (9). The parameters of the DEM model are given in Table 3.
Table 3 Properties of the particles in DEM model.
Parameter uncoated coated
diameter in µm 800 820
3
density in kg/m 190 300
stiffness in N/mm 10 10
shear modulus in MPa 6.25 6.25
restitution coefficient 0.6 0.4
friction coefficient 0.8 0.8
rolling friction coefficient 0.01 0.01 Gas inlet
number of the particles 150.000 150.000 Fig. 5 Mesh of CFD simulation.
The DPM simulations were performed for the dry uncoated aerogel particles and
compared with the case of coated particles. The coated particles are significantly
heavier than dry uncoated aerogel. Moreover, with the wetting the energy adsorption
during impact increases that results in the decreasing the coefficient of restitution
(Antonyuk et al. (10)).
SIMULATION RESULTS
First simulations were performed for the empty apparatus without the solid particles.
The inlet velocity of the gas was varied in the range of 1-2 m/s. The calculated
pressure drop increases with increasing inlet velocity (Fig. 6). The calculated
pressure drop predicted well with the experimental measurements that were carried
out for the full spout bed apparatus included its cylindrical chamber (Fig. 7).
Therefore the predicted values of the pressure drop are smaller than experimental
obtained pressure drops. The gas velocity reaches its maximum in the narrow
vertical inlet splits (Fig. 8). This velocity in these zones increases linearly with
increasing the inlet velocity (Fig. 6).
200 15
200
pressure
Experiment
pressure drop [Pa]
velocity
pressure drop [ Pa]
max. velcity [m/s]
150 150
10 CFD
100 100
5
50 50
0
0 0
0 20 40 60
0 1 2 3 3
inlet velocity in m/s volume flow [m /h]
Fig. 6 Calculated pressure drop and Fig. 7 Comparison of the calculated
maximum gas velocity in the empty pressure drop depending on the
apparatus versus the inlet gas velocity. volume flow of the inlet gas.
Fig. 8 shows the time-averaged flow profiles. The flow starts with a relatively high
velocity at the bottom and becomes wider and slower with the height. Due to
turbulence, two vortices are arisen that generate the secondary flow moving from
the top to down in the near-wall region.
On top of the T-shaped bottom a stagnant air region takes place. The movement
and drying of the particles will be reduced in this area. The particles can sink on the
bottom, as shown in Fig. 9 (DPM simulation, after real fluidization time of 1.1 s).
During coating experiments that leads to sticking of the particles in this region. To
overcome this problem, the nozzle can be placed above this zone and the T-shaped
element must be produced as knee-shaped.
Fig. 10 shows the instantaneous particle positions in the apparatus. As expected the
maximum particle velocity is reached in the spout region. Here the inlet gas
accelerates the particles and picks up nearly vertically according to primary flow.
The gas velocity is decreased gradual over the apparatus height and leads to
decreasing the particle velocity. The particles deviate from vertical air flow and
moves downward along the walls. The maximum bed height depends on the gas
velocity, particle mass and restitution coefficient. With increasing of the particle
mass, the necessary bed height decreases. The Fig. 11 compares the calculated
bed heights.
stagnant particles in
zone sagnant
zone
Fig. 8 The plot of time-averaged fluid Fig. 9 The particle deposition on the
velocities in the empty apparatus at the inlet middle profile in the stagnant zone
velocity of 2 m/s. of the gas (see Fig. 8).
300
3
ρ = 190 kg/m
Maximum bed height in mm
200
.
y 100
x ρ = 300 kg/m
3
z 0
0.2 0.6 1 1.4
Time t in s
Fig. 10 Instantaneous particle positions and Fig. 11 Influence the particle
velocity distributions inside the spout bed density on the maximum bed height
apparatus (particle density = 190 kg/m3, inlet in the spout bed apparatus (inlet
gas velocity = 1.3 m/s). gas velocity = 1.3 m/s).
The wet coated aerogel particles showed a lower translation and rotation velocities
in comparison with dry and light aerogels (Table 4). Therefore, during the coating
process, the inlet gas flow and the velocity must be increased in order to keep
constant particle dynamics and to avoid sticking and agglomeration. The obtained
distributions of the average particle velocity and impact velocity in spouted bed can
be described with a lognormal distribution function, as it shown in Fig. 12. The
average particle-particle impact velocity (Fig. 12 right) is about 7 times smaller than
the absolute particle velocity at the same simulation time. The mean impact velocity
by particle-wall impact is at the average 15 % higher than that by impact of particles.
Table 4 Time-averaged motion parameters.

parameter uncoated particles coated particles
maximum bed height in mm 165 130
mean/maximum particle velocity in m/s 0.36/1.62 0.28/1.20
average particle rotation in 1/s 275 226
1 3 1 30
0.8
P(v)
0.8
p(v imp) [1/(m/s)]

p (v) [1/(m/s)]
2 20
P(v imp) [-]
0.6 impact velostiy:

P (v) [-]
0.6
p(v) P(vp-p)
_V P(vp-w)
p-w
0.4 0.4
1 p(vp-p)
_V p(v
p-wp-w) 10
0.2 0.2
0 0 0 0
0 0.5 1 1.5 0 0.1 0.2 0.3 0.4
velocity [m/s] impact velocity v imp [m/s]
Fig. 12 Distribution function P and its density p for: (left) average absolute particle
velocity and (right) relative impact velocity in the spout bed apparatus. (particle
density of 300 kg/m3; p-p - particle-particle impacts, p-w - particle-wall impacts).
6
2000 Fc,n,breakage = 310 ± 100 mN
Collision rate [1/s].
Impact force in mN
1500 ρ = 300 kg/m

3
4
Fc,n,max
1000
2
500
3
ρ = 190 kg/m
0
Fc,t,max
0
0.3 0.6 0.9 1.2 1.5
0.2 0.6 1 1.4
Time t in s Time t in s
Fig. 13 (left) Collision rate of the particles during the fluidization time, (right) maximal
values of the normal and tangential impact forces (particle density of 300 kg/m3).
Fig. 13 shows the calculated particle-particle collision rates. The fluidized bed of
wetted particles shows smaller height and porosity and so higher collision rates than
for dry aerogels. The particle collides with another particle almost ten times more
frequently than with a wall. The calculated forces acting on the particles during
collisions in the bed (Fig. 13 right) are significantly smaller than breakage range of
the aerogels (Table 2). This confirms the experimental fact that no breakage occurs
during fluidization of aerogels. The small magnitude of the force can be explained by
relative small particle impact velocities in the presented apparatus (Fig. 12).
CONCLUSIONS
The process of coating silica aerogels with pH sensitive polymers was performed
successfully in the experimental spouted bed apparatus. To produce a closed
Eudragit® layer and to avert the shrinking and breakage of the aerogel the particles
can be coated with PEG 2000 as protection material.
The DPM simulations showed a high gas velocity in the bottom part of the apparatus
and its gradual decrease over the apparatus. The increasing mass and energy
dissipation at the contact during the coating decreases the bed height, particle
velocities and increases the collisions rate. The average impact velocity in spouted
bed can be described with a lognormal distribution function. No breakage of the
aerogels was obtained because the impact forces acting in the fluidized bed are
significantly smaller than the measured breakage force of aerogel particles.
REFERENCES
1. Antonyuk, S., Heinrich,S., Alnaief, M. and I. Smirnova: Application of a novel

spouted bed process for the drying and coating of silica aerogel microspheres for
advanced drug delivery, 17th International Drying Symposium, Magdeburg, 2010.
2. Mörl, L., Heinrich, S., Peglow, M., The Macro Scale I: Processing for Granulation,
in Handbook of Powder Technology, Vol. 11, Elsevier Science, (2005), 21-188.
3. Alnaief, M., Smirnova I.: In situ production of spherical aerogel microparticles, J.
of Supercritical Fluids 55 (2010) 3, 1118-1123.
4. Antonyuk, S., Palis, S., Heinrich, S.: Breakage behaviour of agglomerates and
crystals by static loading and impact, Powder Technology 206 (2011) 88-98.
5. van Buijtenen, M.S., Deen, N.G., Heinrich, S., Antonyuk, S. and J.A.M. Kuipers: A
discrete element study of wet particle-particle interaction during granulation in a
spout fluidized bed, Can. J. Chem. Eng., (2009), Vol. 9999, 1-10.
6. Fries L., Antonyuk, S., Heinrich, S., Palzer, S.: DEM-CFD modelling of a fluidized
bed spray granulator, Chemical Engineering Science (2011), in Press.
7. Cundall, P.A., Strack, O.D.L., A discrete numerical model for granular assemblies.
Geotechnique 29 (1979), 47-65.
8. Antonyuk, S., Heinrich, S., Tomas, J., Deen, N.G., van Buijtenen, M.S. and J.A.M.
Kuipers: Energy absorption during compression and impact of dry elastic-plastic
spherical granules, Granular Matter 12 (2010) (1), 15-47.
9. Gryczka, O., Heinrich, S., Deen, N. van Sint Annaland, M., Kuipers, J.A.M. and L.
Mörl: CFD-modeling of a prismatic spouted bed with two adjustable gas inlets, Can.
J. Chem. Eng. 87 ( 2009), 318-328.
10. Antonyuk, S., Heinrich, S., Deen, N.G. and J.A.M. Kuipers: Influence of liquid
layers on energy absorption during particle impact, Particuology 7 (2009), 245-259.
FLUIDIZED BED GASIFICATION OF MIXED PLASTIC
WASTES: A MATERIAL AND A SUBSTANCE
FLOW ANALYSIS
Maria Laura Mastellone*,** and Umberto Arena*,**
*
Department of Environmental Sciences - Second University of Naples, Via A.
Vivaldi, 43 - 81100 Caserta, ITALY
**
AMRA s.c. a r.l., Via Nuova Agnano, 11 - 80125 Napoli, ITALY
ABSTRACT
Gasification as a reliable and convenient waste-to-energy process for the

economic analysis of mixed-plastic waste (MPW) was investigated. To this end a
pilot scale bubbling fluidized bed air gasifier was fired with two commercially
available MPWs to obtain syngas composition and characterization of the bed
material, cyclone collected fines and purge material from the scrubber. These
results were then processed by means of Material and Substance Flow Analyses
to evaluate the main process performance parameters for the two MPWs tested.
INTRODUCTION
Pervasive use of plastics as packaging materials makes this the most important
fraction of municipal solid waste to be considered to reach a gradually larger
intensity of separate collection (6). The sorting process of this fraction after a
household separate collection generally produces a high percentage of residues,
together with some completely recyclable streams and a not negligible fraction of
a non homogeneous plastic scrap, called mixed plastic waste (MPW). This latter
stream contains several types of plastic polymers that often are together with a
not negligible amount of ferrous and non-ferrous metals. Due to its heterogeneity
MPW can be utilized to substitute virgin materials only for a limited number of
goods. On the other hand, its high calorific value makes thermal treatment an
environmental sustainable and economic attractive alternative (9,1).
The study investigates the possibility to utilize the gasification as a reliable and
convenient waste-to-energy process for the economic valorisation of mixed-
plastic waste. To this end a pilot scale bubbling fluidized bed air gasifier, having a
thermal capacity of 500kJ/s, was fired with two commercially available MPWs.
The results have been combined with an environmental assessment tool, the
Material Flow Analysis, which is named Substance Flow Analysis when it is
referred to a specific chemical. MFA/SFA is a systematic assessment of the flows
and stocks of materials and elements within a system defined in space and time.
It connects the sources, the pathways, and the intermediate and final sinks of
each species in a specific process (7). In this study MFA/SFA was applied to a
system boundary that includes the BFB gasifier and the cleaning system for ash
separation (cyclone and wet scrubber). The BFB gasifier was further divided into
two sections: the first corresponds to the dense bed and splashing zone; the
second to the freeboard.
THE PILOT SCALE FLUIDIZED BED GASIFIER
The utilized pilot scale BFB gasifier has the characteristics schematically listed in
Table 1. An olivine - a magnesium-iron silicate, (Mg,Fe2)SiO4 - was selected as
material for the fluidized bed on the basis of results of previous investigations
carried out on the same pilot-scale BFBG [Arena et al., 2010a] that indicated
olivine as an interesting candidate to act as a bed catalyst for the tar cracking
reactions in waste-derived fuel gasification, even taking into account its low cost
and excellent resistance to attrition in the fluidized bed reactor. The main
characteristics of the utilized olivine are reported in Table 2.
Table 1. Main design and operating features of the pilot scale bubbling fluidized
bed gasifier.
ID: 0.381m; total height: 5.90m;
Geometrical parameters
reactive zone height: 4.64m
Feedstock capacity 100 kg/h
Typical bed amount 145 kg
over-bed air-cooled screw
Feeding system
feeder
Bed temperatures 700-950°C
Fluidizing velocities 0.3 –1m/s
Flue gas treatments cyclone, scrubber, flare
Table 2. Characteristics of the olivine particles utilized as bed material in the pilot
scale bubbling fluidized bed gasifier.
Mineral Mg-Fe silicate
Chemical composition, %
SiO2 39-42
MgO 48-50
Fe2O3 8-10.5
CaO <0.4
K2O -
TiO2 -
Al2O3
Cr2O3 0.8
Mg3O4
LOI (loss of ignition) 0.20
Size range, μm 200 ÷ 400
Sauter mean diameter, μm 298
Particle density, kg/m3 2900
In the reported experiments, air was used as reducing agent and always injected
at the bed bottom while the fuel was fed by means of an over-bed feeding
system. The fluidizing air stream was heated up to 450°C by a two electric
heaters before entering the reactor. The fuel and blast flow rates were mutually
adjusted so that, at the fixed fluidizing velocity, the desired equivalence ratio ER
was obtained (where ER is defined as the ratio between the oxygen content of air
supply and that required for the stoichiometric complete combustion of the fuel
effectively fed to the reactor). The cylindrical BFB reactor was heated up to the
reaction temperature by the sensible heat of pre-heated blast gases and by a set
of three external electrical furnaces. The gas generated in the reactor was sent to
a high efficiency cyclone and then to a wet scrubber (for the removal of tars,
residual fly ash and acid gases) and finally incinerated by a safety flare. An
accurate description of the plant and of experimental procedures is provided
elsewhere (3). Here it is sufficient to highlight that gas composition was on-line
measured upstream and downstream of the syngas conditioning section as well
as at the reactor height corresponding to the end of splash zone. The diagnostic
apparatus utilizes IR analyzers for the main syngas components (carbon
monoxide and dioxide, hydrogen, methane) and two micro-gas-chromatographs
equipped with different columns for the detection of light and heavy hydrocarbons
as well as of carbon monoxide and dioxide, hydrogen, nitrogen and water.
EXPERIMENTAL RESULTS
The plant was fed with one of the two mixed plastic wastes taken in
consideration, both obtained as by-products of the sorting process of end-of-use
plastic packaging from separate collection (Table 3). The first, named GS3, is a
mixture of recycled polyolefins obtained from plastic packaging for food and
beverages by means of sorting and washing treatments. The second, named
SRA, is a mixture of several plastic wastes obtained from separate collection of
packagings made of plastic as well as ferrous and non-ferrous metals, as
resulting after an intensive treatment aimed to produce a fuel that can meet even
high quality standards, as those of metallurgical industry.
Table 3. Chemical characterization of the two MPWs utilized in the study.

Mixed Plastic Wastes GS3 SRA
Ultimate analysis, % wb
C (min-max) 84.4 (84.3-84.8) 79.5 (75.9-83.1)
H (min-max) 14.0 (13.5-14.2) 13.1 (12.8-13.4)
N (min-max) 0 0.2 (0.15-0.25)
S (min-max) 0 0.1 (0.08-0.12)
Moisture (min-max) 0.3 0.7 (0.6 – 0.8)
Ash (min-max) 1.3 1.9 (1.4 – 2.4)
O (by difference) 0 4.5
HHVa, MJ/kgfuel,db 46.0 43.4 (41.8-45.0)
b
LHV , MJ/kgfuel,ar 42.9 40.2 (38.6-41.8)
Size (diameter and height), mm 7, 1 irregular
3
Bulk density, kg/m 460 310
a) evaluated by means of relationship proposed by Channiwala and Parikh (2002).b) evaluated by
the HHV on dry basis by taking into account the latent heats of vaporization of fuel moisture and
water obtained as product of hydrogen combustion;wb= weight basis; db=dry basis; ar=as received.
The pilot scale BFBG was operated with the mixed plastic wastes in a bed of
olivine particles fluidized at a velocity of 0.7m/s, at a bed temperature of about
850°C, preheated air of about 450°C and an equivalence ratio of 0.27. The
performances of the BFBG were measured and recorded only when the chemical
composition of the produced syngas and the temperature profile along the reactor
reached steady-state conditions. The experimental activity provided the complete
chemical composition of gas stream at two levels of BFB gasifier (2m above the
air distributor and at the reactor exit) together with those of streams leaving the
cyclone and the wet scrubber system. These latter data, (Table 4), have been
elaborated and used for the substance flow analysis of carbon, hydrogen, iron,
magnesium and other elements and for the feedstock energy flow analysis (5).
THE MFA/SFA ANALYSIS
Figures 1-3 report the quantified flow diagrams resulting by the MFA/SFA applied
to the above cited sections of the bubbling bed gasifier (dense bed + splashing
zone and freeboard zone) and of the cleaning system (cyclone for ash separation
+wet scrubber for gas cleaning) of the pilot scale gasification system, when
operated with the two MPWs.
Figure 1. Layers of total mass balances (kg/h) throughout the pilot scale
gasifier, for test with GS3 (left) and SRA (right)mixed plastic waste fuels.
The layer of total mass flow rate is reported in Figure 1. The input flows to the
BFBG unit are the stream of plastic fuel and that of air used as oxidizing agent
and fluidizing gas. The output flow stream from the dense bed and splashing
zone is that of the obtained syngas, which still contains heavy hydrocarbons and
entrained fines. This stream is visualized in Figs. 1-3 as two different arrows, one
indicating the syngas, i.e. the mixture of N2, CO, H2 and CnHm with n<6, the other
indicating the contaminants, mainly heavy hydrocarbons and entrained fine
particles. The output from this first section moves throughout the freeboard and
then to the cyclone for dust abatement and to the wet scrubber for removal of tars
and inorganic compounds. Along these paths both chemical and physical
reactions occurred so that the mass flow and composition of each stream were
modified (Figs. 1-3).
By looking at Figure 1 it is evident the different process performances obtained

with the mixture of polyolefin plastic waste (GS3) and with the other mixed-plastic
waste (SRA). The analysis of the results of the test with GS3 in a bed of olivine
indicates a great performance, with the almost complete absence of tar (Fig. 1), a
consequently high value of the specific syngas conversion efficiency
(122.2/(28.5+97.6)=0.97) and a high concentrations of molecular hydrogen and
carbon monoxide in the syngas (Table 4). Specific studies about the role of
olivine as a tar removal catalyst during the gasification of polyolefin plastic wastes
[Arena et al., 2009; 2010a] indicated that magnesium and iron, both largely
present in the olivine particles, activate the endothermic decomposition reactions
of hydrocarbon fragments that are the first precursors of tar formation. The very
low tar concentrations are always coupled with low concentrations of methane
(less than 3%), ethane, ethylene, acetylene, propylene or, in other words, with
high extension of the cracking and dehydrogenation reactions (10).
Table 4. Operating conditions and performance parameters of the pilot scale
BFBG operated with the SRA fuel under two values of equivalence ratio.
Mixed Plastic Wastes GS3 SRA
Operating Conditions
ER (equivalence ratio), - 0.27 0.27
AF (air/fuel ratio), kgair/kgfuel 3.95 3.59
Output Process Data
Temperature of fluidized bed,°C 830 890
Qsyngas,m3N/kgfuel 5.82 3.75
LHVsyngas, kJ/m3N 6850 6430
Specific energy, kWh/kgfuel 11.1 6.7
CGE (cold gas efficiency), - 0.83 0.77
Syngas composition (downstream of cyclone and scrubber)
N2, % 46.25 65.11
CO2, % 1.50 9.80
CO, % 21.07 5.34
H2, % 28.18 8.58
CH4, % 2.31 7.30
C2H4 + C2H6+ C2H2 + C3H6, % 0.55 3.76
The analysis of the results for the SRA fuel indicates that syngas has very low
concentrations of H2 and CO and larger concentrations of CH4 and C3Hm together
with a higher content of tar (11.4/(25.1+97.6)=0.093) and a correspondingly lower
specific syngas yield (111.2/(25.1+97.6)=0.91): this suggests that the catalytic
action of olivine is not present. Moreover, the role of the freeboard section
appears negligible since the decreasing of heavy hydrocarbons and elutriated
fines fraction between the exit of dense bed and splashing zone and the reactor
exit is very low (3.5%).
Figure 2 reports the results of the mass balances applied to the carbon element,
i.e. the carbon layer of SFA, for both MPWs. It provides the carbon conversion
efficiency CCE, defined as the ratio between the mass flow rate of the carbon
present in the syngas as CO, CO2, CH4 and light hydrocarbons (until C5Hm) and
the mass flow rate of the carbon that enters the reactor with the fuel.
In the case of the GS3, the CCE increases from the value of 0.77 at the exit of
the splashing zone to 0.81 and 0.83 related to the freeboard and cleaning system
exit, respectively. These values confirm that the largest part of fuel conversion
into syngas occurs in the dense bed and splashing zone, which is characterized
by an intense turbulence of gas phase and by the effect of heterogeneous and/or
catalytic reactions (dehydrogenation and carbonization).
Analogous calculations can be made for the SRA test (right side of Fig. 2). In this
case, the CCE does not vary between the three measurement points and remains
almost equal to 0.76. This different behaviour is confirmed by the value of carbon
accumulated in the bed (that is almost zero) as well as by that of carbon fines
elutriation rate (that is negligible). The absence of carbon fines along the
freeboard can affect the type of reactions occurring in this region: oxygen is
absent and heterogeneous reactions cannot occur, so that the only expected
reactions are those of recombination of reactive molecules that can lead to an
increasing of heavy hydrocarbons (tar).
Figure 2. Layers of total carbon balances (kg/h) throughout the pilot scale
The graph on the left side highlights the completely different behaviour of the
GS3 waste. The carbonization was so present, and strong, that an accumulation
of carbon on the bed particles surface was present: the stock of 145kg of bed
particles was progressively incremented (3.7kg/h) as a result of opposite effects
of elutriation losses and carbon accumulation. The fines collected at the cyclone
in the run with GS3 were mainly produced by the attrition between the bed
particles and the carbon layer deposited on their surface. They contained
quantity of iron larger than that entering the reactor with the fuel (4): this means
that part of the elemental iron of olivine, linked with the carbon by coordination
complexes, was then detached from the particle by mechanical attrition and
entrained out of the reactor in the syngas.
This behaviour allowed that, in the test with GS3, less than 6% of the fuel carbon
was used to produce tar precursors while, in that with SRA where this mechanism
was inactive, the 24% of the fuel carbon was transformed into heavy compounds
in the dense bed+splashing zone. These considerations can be repeated and
further supported by analyzing the hydrogen layer (Fig. 3).
In the test with GS3 the hydrogen conversion into syngas moved from 0.82 to
0.89 and to 1, i.e. the dehydrogenation of the fuel was completed. All the fuel
hydrogen was transferred into syngas as H2 and light hydrocarbons. No hydrogen
was present as tar compounds and as carbon fines. This result was due to the
completion of carbonization/dehydrogenation reactions that largely occurred in
the dense bed and partly occurred in the freeboard and in the cyclone, thank to
the contact between the carbon fines (that contained metal active particles
absorbed over and inside its surface) and heavy hydrocarbons not yet converted
into small molecules in the dense bed+splashing zone. The dehydrogenation was
Figure 3. Layers of total hydrogen balances (kg/h) throughout the pilot scale
due to the increasing of aromatization until to the complete hydrogen abstraction

from heavy hydrocarbons and PAHs.
The hydrogen flow analysis of SRA test shows, again, a different behaviour (Fig.
3). In this case, the increasing of hydrogen conversion into syngas components
moved from 0.74 to 0.75 and to 0.77. The values are, as with CCE, very close to
each other, and the final value was very far from the total conversion obtained
with GS3. This result was due to the absence of any heterogeneous reactions in
the dense bed as well as in the other zones of gasifier: the carbon accumulation
rate was almost zero and, as a consequence, the carbon elutriation rate too.
CONCLUSIONS
The industrial application of plastics-to-energy gasifiers was investigated. The

process performances of two mixed-plastic wastes, gasified in a pilot scale
bubbling fluidized reactor having a bed of olivine have been evaluated.
Experimental measurements taken at different points inside and downstream of
the gasifier, combined with mass balances and material and substance flow
analyses, indicated the MPW that offers the higher performance and reliability. In
particular, SRA, a MPW obtained from a separate multi-material collection
(plastics+ferrous+non-ferrous packaging) processed by an intense treatment,
presently designed to be utilized in the metallurgic industry, appeared convenient
for a gasification-based, plastics-to-energy plant only if a downstream recovery
and valorization of tar stream is provided. On the contrary, GS3, a more
homogeneous MPW, mainly made of polyolefin plastics with a substantial
absence of ferrous or non-ferrous packaging, and just processed by means of a
shredding and washing treatment gave the best performance.
During the gasification of SRA, the catalytic effect of olivine particles appeared
absent or limited: carbonization was practically absent and the produced tar was
captured by the wet scrubber so determining a not negligible environmental
burden and a remarkable energetic loss and, then, a relevant economic cost. It is
likely that the catalytic support to the cracking and isomerization was always
active (the heavier fragments are broken and a number of unsatured
hydrocarbons with two or three carbon atoms are formed) but the catalytic
enhancement of the dehydrogenation and carbonization determined by active
sites of iron was absent (the hydrogen content remains low and the tar formation
was not inhibited).
During the gasification of GS3, the catalytic effect of olivine particles was so
strong that no tars were detected downstream of the cleaning section and the
endothermic reactions of carbonization clearly reduces the bed temperature. The
negative aspect of this mechanism is that an amount of carbon continuously
accumulates in the bed, indicating the necessity of an overflow of exhausted
olivine particles and a corresponding make-up of fresh particles. Exhausted
olivine could be regenerated by burning the carbon layer covering the external
surface (2).
ACKNOWLEDGEMENTS
The study was carried out with the financial support of CONAI (Italian National
Consortium for Packaging). Authors are indebted to to Mr. Donato Santoro for all
the chemical analyses related to the experimental activity.
REFERENCES
1. Arena U. and M.L. Mastellone (2006) Fluidized Bed Pyrolysis of Plastic

Wastes. Chapt. 16 in Feedstock Recycling and Pyrolysis of Waste Plastics, J.
Scheirs and W. Kaminsky (Eds). J. Wiley&Sons Ltd, ISBN: 0-470-02152-7, pp.
435-474
2. Arena U, L. Zaccariello, M.L. Mastellone (2008) Gasification of a plastic waste
in a fluidized bed of olivine. Proc. of CFB9 - 9th Int. Conf. on Circulating Fluidized
Beds. J. Werther, W. Nowak, K.-E. Wirth and E.-U. Hartge /eds.), ISBN 978-3-
930400-57-7, p. 691-696
3. Arena U., L. Zaccariello, M.L. Mastellone (2009) Tar Removal During the
Fluidized Bed Gasification of Plastic Waste. Waste Management, 29:783-791
4. Arena U., L. Zaccariello, M.L. Mastellone (2010a). Fluidized Bed Gasification
of Waste-Derived Fuels. Waste Management, 30:1212-1219
5. Arena U., F. Di Gregorio, L. Zaccariello and M.L. Mastellone (2010b) Fluidized
bed gasification of biomass: a substance flow analysis, in Fluidization XIII,
S.Done Kim, Y. Kang, J.Keun Lee and Y. ChilSeo (Eds), Engineering
Conferences International, ISBN 978-0-918902-57-3, pp. 805-812
6. Brandrup J., M. Bittner, W. Michaeli and G. Menges (Eds.) (1996). Recycling
and recovery of plastics, New York, NY: Hanser Publ
7. Brunner P.H. and V. Rechberger (2004) Practical Handbook of Material Flow
Analysis. CRC Press LLC, Boca Raton (FL)
8. Channiwala S.A and P.P. Parikh (2002). A unified correlation for estimating
HHV of solid, liquid and gaseous fuels, Fuel, 81:1051-1063
9. Hermann C., F.J. Schwager, K.J. Whiting (2001).Pyrolysis & Gasification of
Waste.A Worldwide Technology & Business Review. 2nd Edition. Juniper
Consultancy Services Ltd
10. Mastellone M.L. and U. Arena (2008). Olivine as a Tar Removal Catalyst
During Fluidized Bed Gasification of Plastic Waste. AIChE Journal, 54/6: 1656-
1667
EFFECT OF GAS BYPASSING IN DEEP BEDS ON CYCLONE
DIPLEG OPERATION
A. S. Issangya, S. B. Reddy Karri, Ted M. Knowlton and Ray Cocco
Particulate Solid Research, Inc., 4201 W 36th Street, Suite 200, Chicago, USA
ABSTRACT
Cyclone diplegs play a major role in the functioning of fluidized beds. Previous
studies have shown that at certain operating conditions there can be severe gas
bypassing (also referred to as jet streaming) of gas in deep beds of Geldart Group A
materials which leaves significant portions of the fluid bed defluidized. If cyclone
diplegs are immersed in these defluidized regions, solids discharge from the dipleg
may be hindered, which can lead to the flooding of the dipleg and the cyclone. This
could result in high solids losses from the fluidized bed. Tests were conducted to
demonstrate that cyclone diplegs can flood when discharging into a bed with gas
bypassing. Tests were also conducted to determine how gas bypassing affects the
operation of cyclone diplegs that have a splash plate or a trickle valve. These tests
were conducted in a 1.52-m-diameter semicircular column equipped with a Plexiglas
faceplate to allow visual observation.
INTRODUCTION
Cyclone diplegs are pipes attached to the conical bottom of cyclones that return the
collected solids back into the system. Cyclones are widely used in catalytic
processing units where diplegs are used to return collected catalyst particles back to
fluidized beds. Diplegs can discharge solids above a fluid bed (suspended diplegs)
or directly into the fluid bed (submerged diplegs). During start-up, the fluidizing gas
preferentially flows up the dipleg of a second-stage cyclone until a solids level in the
dipleg is established to seal it. First-stage cyclone diplegs generally have enough
solids flow through them to allow a seal to be established in spite of the initial
upward gas flow in the dipleg, and sealing devices at the dipleg exit of first stage
cyclones are typically not necessary. Splash plates, placed a short distance below
the dipleg, are often been used with first stage diplegs to try to prevent gas from
entering the dipleg. The solids flow rate in second stage cyclones is generally too
small to establish a seal unless a device such as a trickle valve is attached to the
dipleg end to prevent gas from flowing up the dipleg.
Despite the wide use of cyclones and diplegs in fluidized beds, there are only a few
dipleg studies in the open literature. Bristow and Shingles (1) identified four
operating modes of trickle valves in diplegs: trickling, dumping, trickling/dumping,
and flooding. Flooding occurs if the solids flow into the dipleg is greater than the
solids being discharged from the dipleg causing the dipleg to fill with solids and
back-up into the cyclone. A blowing mode can also occur in some cyclone diplegs
(2) where the pressure inside the cyclone can be greater than at the end of the
dipleg.
Geldart et al. (3) found that a considerable amount of the cyclone inlet gas can be
dragged downwards by the solids if the dipleg is operating in streaming flow. Dries
and Bouma (4) proposed five modes of flow in a cyclone dipleg; (a) stick-slip flow
when the solids in the dipleg were in packed bed condition, (b) transition flow mode
in which the dipleg had a dense fluidized region on top of a packed bed region, (c)
unstable flow at low solids fluxes, and (d & e) at higher solids fluxes, a wholly dilute
phase flow or a dipleg flow with a dilute region on top of a dense fluidized region.
Wang et al (5, 6) measured axial pressure and radial solids volume fractions and
particle velocity profiles in cyclone diplegs and the amount of gas flowing down the
dipleg. The formation of a dense phase in a dipleg was found to significantly
decrease the amount of gas downflow.
Karri and Knowlton (2) found for FCC catalyst that aeration substantially increased
the amount of solids flow through both immersed and nonimmersed trickle valves
and that the solids flux through the dipleg was not a function of the flapper weight
when aeration was used. The best aeration locations for a trickle valve were found to
be just above the mitered bend and at the midpoint of the mitered section. It was
also found that cyclone gas was dragged down the dipleg into the bed by the fast
moving solids when the solids flux exceeded about 100 kg/ s-m2.
One factor that is missing in submerged dipleg studies is how solids discharge from
a dipleg is affected by the quality of fluidization at the point of discharge. Studies
(Wells, 7; Knowlton, 8; Karri et al., 9; Issangya et al., 10, 11; Karimipour and
Pugsley, 12) have shown that deep beds of Geldart Group A materials can have
defluidized regions caused by gas bypassing. Most of the fluidizing gas was
observed to preferentially flow up near the column wall in a single or a number of
high velocity streams of bubbles. Gas bypassing was attributed to decreased
voidage and permeability of the emulsion phase due to the compression of gas in
the emulsion phase caused by the pressure head developed in deep beds.
Bolthrunis (13) found that severe gas maldistribution occurring in a large fluid bed
reactor could be prevented by installing baffles.
If cyclone diplegs are located in the poorly fluidized region of a gas bypassing bed,
solids discharge from the dipleg will likely be hindered, which can lead to the flooding
of the dipleg and the cyclone. Defluidization can also result from poorly designed or
defective gas distributors. This paper discusses tests conducted to determine if
cyclone diplegs with and with no exit attachments will flood because of gas
bypassing in the fluid bed.
EXPERIMENTAL
Tests were conducted in a 1.52-m-diameter, 5.2 m tall semicircular fluidized bed that
had a Plexiglas faceplate (Figure 1). The unit had three, 41-cm-diameter, tangential
inlet internal first stage cyclones (Figure 2). The left and the right hand side cyclones
had 15-cm-diameter fully round diplegs that discharged solids into the bed 25 cm
away from the faceplate. The middle cyclone had the test dipleg which was
transparent and semicircular and was attached to the flat faceplate to enable visual
observation of solids flow through it. Air exiting the three primary cyclones entered a
51-cm-diameter second stage cyclone and then passed into a third stage cyclone of
the same diameter before entering the exhaust header. The third stage cyclone
dipleg returned solids to the second-stage cyclone dipleg via an automatic L-valve
and the combined flow was returned to the column by another automatic L-valve.
The operation of the middle cyclone dipleg was studied for various solids fluxes
through the dipleg, and with and without dipleg aeration. In order to have a wide
range of solids fluxes through the test dipleg, diplegs of two sizes, 7.6 and 20 cm
diameters, were tested. The solids flux was also varied by changing the bed
superficial gas velocity. The solids flux through each dipleg was calculated from the
measured fluid bed entrainment rate at a given superficial gas velocity by assuming
that the loading was split equally among the three cyclones.
At superficial bed velocity of 0.9 m/s, the solids fluxes in the 15-cm-diameter round
dipleg and the 20-cm-diameter semicircular dipleg were 85 and 96 kg/s-m2,
respectively. These values are within the high solids flux range of commercial
second stage diplegs which are normally operated at fluxes much less than 100
kg/s-m2. The solids flux in the 7.6-cm-dia. semicircular dipleg was 684 kg/s-m2 at the
same gas velocity in the bed. This was within the range of the solids fluxes in
commercial first stage cyclone diplegs which are typically 350 to 750 kg/s-m2.
The Plexiglas faceplate allowed visual observation of the quality of fluidization in the
bed and of the flow of solids and bubbles in the diplegs. Digital videos of the dipleg
flow were made at selected operating conditions. Differential pressure (∆P)
fluctuations were measured across bed axial lengths of 60 cm at five locations
around the circumference of the unit. The ∆P fluctuation data offered another way of
assessing if there was gas bypassing in the bed. Locations near the gas bypass
stream have been found (Issangya et al. (3)) to have significantly higher ∆P
fluctuations than the rest of the bed.
The middle cyclone dipleg was tested having (a) no exit terminations (b) a trickle
valve and (c) a splash plate (Figure 3). The two 15-cm-diameter interior cyclone
diplegs had no exit attachments. The splash plate tests were conducted with the 7.6-
cm-diameter dipleg where high solids fluxes, typical of those in primary cyclone
diplegs, could be achieved. An 8.9-cm-diameter semicircular steel splash plate was
placed 8.9 cm below the dipleg end. The distance of the splash plate from the dipleg
end was calculated such that the solids discharge area was twice the area of the
open end of the dipleg, a criterion often used in industry.
The trickle valve tests were conducted with the 20-cm-diameter dipleg. The trickle
valve was made from a 15-cm-diameter pipe whose opening was inclined 4 degrees
from the vertical. The trickle valve flapper plate was attached to the pipe by loose
hanger rings.
The cyclone diplegs were operated both without and with dipleg aeration. The dipleg
aeration was equivalent to a gas velocity of 0.03 m/s in the dipleg. The aeration for
the diplegs with no exit terminations and the one with a splash plate were located
2.54 cm above the open end. Aeration was supplied to the dipleg with a trickle valve
15.2 cm above the bend and at the midpoint of the underside of the inclined part of
the trickle valve as recommended by Karri and Knowlton (4).
Tests were conducted with two static bed heights: 1.52 m, referenced to the air
distributor, to obtain strong gas bypassing in the bed, and 1.07 m to obtain a
uniformly fluidized bed. The test material was a 2.5% fines (<44 μm) FCC catalyst
with a median particle diameter (dp50) of 85 microns and particle density of 1488
kg/m3. The particle size distribution is given in Figure 4.
Gas bypassing in the semicircular unit occurred in the form of two gas bypass
streams located near the corners where the flat faceplate met the semicircular
column. The two streams occasionally moved toward the center of the faceplate or
moved inward and around the unit along the wall. Because the shell of the column
was made of steel, the motion of the gas bypass stream was only detected from the
∆P fluctuation signals. It was possible to visually observe solids and bubble flow in
and around the test cyclone located at the center of the faceplate. Results presented
in this study are visual observations of the bed fluidization behavior, and of whether
flooding was occurring in the test cyclone dipleg.
Effect on Straight Diplegs With no Exit Attachments
Table 1 shows the results for the 20-cm-diameter semicircular cyclone dipleg with no
exit attachment. The fluid bed unit was operated at superficial gas velocities of 0.15
to 0.9 m/s and the static bed height was 1.52 m. The solids flux in the dipleg ranged
from 0.24 kg/s-m2 at a bed velocity of 0.15 m/s to 96 kg/s-m2 at a bed velocity of 0.9
m/s. With or without dipleg aeration, the dipleg operated well without flooding at all
gas velocities. Gas bypassing was present for all gas velocities except at 0.9 m/s
where it was significantly reduced because of the high superficial gas velocity.
Occasionally, a relatively stagnant dense (but not packed) region formed around the
dipleg exit region. This dense region was frequently broken by bubbles rising directly
up from the air distributor or by the gas bypass streams that at times moved to the
middle of the faceplate. Bubbles rose through the dipleg, but their frequency
decreased as the solids flux through the dipleg increased.
Table 1. Dipleg operation: 20-cm-diameter semicircular dipleg (no exit attachment)
Ug Dipleg Solids Flux Gas DIPLEG 2 OPERATION

m/s kg/s-m2 Bypassing in
Diplegs Dipleg 2 the Fluid No Dipleg With Dipleg
1 and 3 (D = 20 cm) Bed? Aeration Aeration
0.15 0.20 0.24 YES GOOD GOOD
0.30 1.61 1.95 YES GOOD GOOD
0.46 6.35 6.84 YES GOOD GOOD
0.61 17.1 19.0 YES GOOD GOOD
0.76 36.6 41.0 YES GOOD GOOD
0.91 85.4 96.2 WEAK GOOD GOOD
Table 2 shows the results for the 7.6-cm-diameter semicircular dipleg with no exit
termination for a static bed height of 1.52 m. With no dipleg aeration, the dipleg
functioned well for all solids fluxes up to 88 kg/s-m2. The dipleg flooded for solids
fluxes of 103, 137 and 293 kg/s-m2. At a solids flux of 684 kg/s-m2 solids bridging
occurred in the upper part of the dipleg where there the semicircular dipleg joined
the round tube. The solids then accumulated and overflowed into the cyclone. When
dipleg aeration was present, the dipleg functioned without flooding at all the solids
fluxes except at 684 kg/s-m2 when bridging occurred. Bubbles were able to rise
through the dipleg for solids fluxes up to about 220 kg/s-m2. The dipleg functioned
properly for the 1.07 m static bed tests with or without dipleg aeration except for the
highest solids flux that led to dipleg bridging.
Table 2. Dipleg operation: 7.6-cm-diameter semicircular dipleg (no exit attachment)
Ug Dipleg 2 Gas DIPLEG 2 OPERATION

m/s (D = 7.6 cm) Bypassing in
Solids Flux the Fluid No Dipleg With Dipleg
kg/s-m2 Bed? Aeration Aeration
0.15 1.46 YES GOOD GOOD
0.61 136.7 YES FLOODED GOOD
0.91 683.5 NO/WEAK BRIDGED BRIDGED
Effect on Diplegs Fitted With a Splash Plate
Table 3 gives the results for the 7.6-cm-diameter semicircular dipleg fitted with a
splash plate and with and with no dipleg aeration. With no aeration, the dipleg
functioned well for solid fluxes of 13 and 49 kg/s-m2 but flooded at solid fluxes of 78,
107 and 137 kg/s-m2. When dipleg aeration was turned on, the dipleg was able to
function well at solid fluxes of 107 and 137 kg/s-m2. Flooding occurred for solid
fluxes of 200 and 459 kg/s-m2 and the dipleg bridged when the solid flux was
increased to 684 kg/s-m2 as was the case was for the straight dipleg discussed
above. The dipleg did not flood for tests that were conducted with a static bed height
of 1.07 m where no or very weak gas bypassing was occurring. Comparing the
dipleg with no attachment with the dipleg with a splash plate under gas bypassing
conditions, it appears that with no dipleg aeration a straight open cyclone dipleg
worked just as well as the one with a splash plate. However, when there was dipleg
aeration the dipleg with a splash plate flooded at a lower solids flux of 200 kg/s-m2,
compared to the straight dipleg which did not flood at Gs = 293 kg/s-m2.
Effect on Diplegs Fitted With a Trickle Valve
Table 4 presents results for the 20-cm-diameter semicircular dipleg fitted with a
trickle valve and with and with no dipleg aeration for a 1.52 m static bed. With no
dipleg aeration, the dipleg worked well for solids fluxes of 0.24, 1.92 and 6.83 kg/s-
m2 which corresponded to gas velocities in the bed of 0.15, 1.0 and 0.46 m/s,
respectively. The dipleg flooded when the solids flux was raised to 19 kg/s-m2
corresponding to a bed superficial velocity of 0.6 m/s, but functioned well when the
superficial gas velocity was increased to 0.76 m/s. At a superficial gas velocity of
0.76 m/s, the dipleg solids flux was 41 kg/s-m2. It seemed that more air was able to
leak from the bed and enter the dipleg at a superficial gas velocity of 0.76 m/s than
at a superficial gas velocity of 0.6 m/s, and this amount of air was sufficient to aerate
the dipleg and allow the dipleg to operate without flooding. At a superficial gas
velocity of 0.9 m/s, for a solid flux of 96 kg/s-m2, the dipleg at first flooded but then
recovered and continued to function well. Apparently, enough air was able to leak
through the trickle valve and reaerate the flooded dipleg. The dipleg flooded at solid
fluxes of 130 and 205 kg/s-m2. These solids fluxes corresponded to superficial gas
velocities of 1.0 and 1.1 m/s, respectively. It appeared that even with the higher air
leakage from the bed, the solids flux was too high for the dipleg to function without
an external supply of aeration. For tests performed with dipleg aeration on the dipleg
functioned without flooding at all solids fluxes tested, up to 205 kg/s-m2.
Table 3. Dipleg operation: 7.6-cm-diameter semicircular dipleg with a splash plate

m/s (D = 7.6 cm) Bypassing in
Solids Flux kg/s- the Fluid No Dipleg With Dipleg
m2 Bed? Aeration Aeration
0.69 200.2 YES GOOD FLOODED
0.84 458.9 YES GOOD FLOODED
0.91 683.5 NO/WEAK GOOD BRIDGED
Table 4. Dipleg operation: 20-cm-diameter semicircular dipleg with a trickle valve

m/s (D = 20 cm) Bypassing
Solids Flux in the Fluid No Dipleg With Dipleg
kg/s-m2 Bed? Aeration Aeration
0.91 96.2 WEAK FLOODED THEN GOOD
RECOVERED
0.98 130.3 NO FLOODED GOOD
1.07 204.6 NO FLOODED GOOD
CONCLUSION
Diplegs immersed in poorly fluidized zones caused by gas bypassing can flood and
cause solids to back up into the cyclone causing excessive solids losses. The
occurrence of flooding was a function of dipleg solids flux and the presence or
absence of a dipleg exit attachment. As found in other studies, dipleg aeration
significantly increased the operating range of the dipleg solids flux before flooding
would occur. Diplegs with no exit attachments functioned well at all conditions tested
if they had dipleg aeration. With no dipleg aeration, diplegs with no exit attachments
flooded at solids fluxes of 137 kg/s-m2 and above. With no dipleg aeration, the dipleg
fitted with a splash plate flooded at solids fluxes of 78 kg/s-m2 and above. The
addition of dipleg aeration extended the mass flux operating window of the dipleg.
With aeration, the dipleg fitted with a trickle valve functioned well for all conditions
tested, up to 205 kg/s-m2. With no dipleg aeration, the dipleg flooded if the solids flux
exceeded 98 kg/s-m2.
REFERENCES
1. T. C. Bristow and T. Shingles (1989), Cyclone dipleg and trickle valve operation,
in Fluidization VI, J. R. Grace, L. W. Shemilt, M. A. Begougnou, eds., Engineering
Foundation, 161 – 168
2. Reddy Karri, S. B. and T. M. Knowlton (2004), The effect of aeration on the
operation of cyclone diplegs fitted with trickle valves, Ind. Eng. Chem. Res., 43 (18),
5783 - 5789
3. D. Geldart, N. Broodryk and A. Kerdoncuff (1993), Studies on the flow of solids
down cyclone diplegs, Powder Technol., 76, 175 – 183
4. H. W. A. Dries and J. H. Bouma (1997), Down flow of class A powder in cyclone
diplegs, in Proceeding of 5th Int. Conf on Circulating Fluidized Beds, 585 – 590
5. S. J. Wang, D. Geldart, M. S. Beck and T. Dyakowski (2000), A behaviour of a
catalyst flowing down in a dipleg, Chem. Eng. J., 77, 51 – 56
6. J. Wang, J. H. Bouma and H. Dries (2000), An experimental study of cyclone
dipleg flow in fluidized catalytic cracking, Powder Technol., 112, 221 – 228
7. J. Wells, Streaming flow in large scale fluidization, Paper presented at the AIChE
Annual Meeting, Reno, Nevada, 2001
8. T. M. Knowlton (2001), Video presented at Fluidization IX, Beijing, China.
9. S. B. R. Karri, A. S. Issangya and T. M. Knowlton, (2004), Gas bypassing in deep
fluidized beds, in Fluidization XI, U. Arena, R. Chirone, M. Miccio, P. Salatini, eds.,
Naples, Italy
10. A. S. Issangya, S. B. Reddy Karri and T. M. Knowlton (2008), Effect of baffles
on jet streaming in deep fluidized beds of Group A particles, in Circulating Fluidized
Bed Technology IX, Hamburg, Germany
11. A. S. Issangya, S. B. Reddy Karri and T. M. Knowlton (2009), Effects of imposed
solids flux and pressure on gas bypassing in deep beds of Group A materials (2009),
in Fluidization XIII, S. D. Kim, Y. Kang, J. K. Lee, Y. C. Seo (eds.) Engineering
Conference International, NY
12. S. Karimipour and T. Pugsley (2010), Study of gas streaming in deep fluidized
bed containing Geldart’s Group A particles, Che. Eng. Sci., 65, 3508 – 3517
13. C. O. Bolthrunis, M. Hagan and W. Mukaddam (2010), Spinning straw into gold:
Turning academic papers into commercial fluidized bed reactor designs, in
Fluidization XIII, S. D. Kim, Y. Kang, J. K. Lee, Y. C. Seo (eds.) Engineering
Conference International, NY
Baghouse P
DP
Internal
Cyclones
D = 41 cm DP
51-cm-Dia.
Cyclones
Dipleg
Total DP
DP
DP Across
Fluctuations 15.2 cm
DIPLEGS
1.52-m-Dia, 5.2 m Tall AERATION
30°
Semi-Circular
Column with Three
41-cm-Dia. 10.2-cm-Dia.
Internal Cyclones Semicircular
191 cm
FLUIDIZING Sparger
AIR
7.6-cm-Dia
Pipes Manifold
79 cm
Fluidizing
Air
Figure 1. Side View of the Test Unit Figure 2. Front View of the Test Unit
Semicircular Semicircular
25.4 mm
Dipleg With a Dipleg With a Particle Diameter, micron
Thick
Splash Plate Trickle Valve
Cumulative Volume Percent Less Than
Faceplate 0 20 40 60 80 100 120 140 160 180 200

38 mm Radius 12
100
25.4 mm 12.7 mm
Thick Wall Thickness 10 Percent Volume Fraction
Faceplate 80
102 mm FCC Catalyst
Radius 8
dp50: 84 μm
60 Fines: 2.5% < 44 μm
6
15 cm-Dia
Aeration Round Pipe 40
Aeration 4
Steel Plate 20 2
89-mm-Dia.
Semicircular Aeration
Splash Plate 0 0
Trickle Valve 0 20 40 60 80 100 120 140 160 180 200
89 mm
o Particle Diameter, micron
4
Figure 3. Schematic Drawing of Diplegs with a Figure 4. Particle Size Distribution of

Splash Plate and a Trickle Valve Material Used
FLUIDIZATION BEHAVIOR IN A GAS-SOLID FLUIDIZED BED
WITH THERMALLY INDUCED INTER-PARTICLE FORCES
Jaber Shabanian, Farzam Fotovat, Jonathan Bouffard, Jamal Chaouki
Department of Chemical Engineering, Ecole Polytechnique de Montreal, Montreal,
Quebec, Canada

Corresponding author: Tel.: +1-514-340-4711 X 4034; fax: +1-514-340-4159.
E-mail address: jamal.chaouki@polymtl.ca.
ABSTRACT
In this work, a new approach for increasing and controlling inter-particle forces (IPFs)
was applied. This method used a spherical inert particle coated with a polymer
material having a low glass transition temperature. Since IPFs depend on the
temperature of the coated particles, they can be easily controlled by the temperature
of the inlet air. For this reason, the temperature of the system was varied uniformly
near the glass transition temperature of the polymer, between 20 – 40oC, to
investigate the effect of IPFs on fluidization behavior at low and high gas velocities.
INTRODUCTION
Particle size, shape, roughness and density as well as inter-particle forces (IPFs) are
among the most important parameters affecting the flow dynamics of powder
materials. In regard to the significance of IPFs, for instance, there is no doubt that
IPFs dominate the fluidization behavior of Geldart Group C particles, which leads to
a completely different behavior compared to the other groups of Geldart’s
classification with low or no IPFs.
Investigations into the influence of IPFs on the behavior of a gas-solid fluidized bed
have been carried out using different methods. Most importantly, however,
controlling the level of IPFs to have a uniform cohesion throughout the particulate
media is not an easy task. Methods that have been used include the following:
increasing the amount of Van der Waals forces by decreasing the mean size of
particles (1); increasing the amount of capillary forces by the addition of a cohesive
agent into the bed (2); creation of a magnetic field around the bed (3) or raising the
bed temperature to a high value (4).
Each of these methods has specific difficulties in practice. For the first method it is
very difficult to control particle shape and surface roughness. Due to these
difficulties, the use of Van der Waals forces to study the effect of IPFs on fluidization
characteristics is a complex procedure. By increasing the size of particles, the
hydrodynamic forces become dominant compared to the IPFs. For larger particles,
an increase in IPFs must be induced by the addition of a cohesive agent into the
particulate system. One of the most popular methods to conduct this technique is by
the presence of wet capillary bonds created by an interstitial liquid between the
particles. The problem with this approach is that it is challenging to have a uniform
distribution of the agent throughout the whole bed, which leads to force anisotropy
1

inside the particulate system (5). The other problem with this approach is that it
restricts the fluidization study at low superficial gas velocities. To employ the third
method an expensive set-up is needed to generate a magnetic field with the help of
a costly electromagnetic coil system. The other problem of this approach is that the
ferromagnetic particles attract themselves when they are parallel to the magnetic
field and repel each other when they are perpendicular, which, consequently, causes
anisotropic attraction/repulsion in the bulk materials (6). For the last method, the first
problem is that it is costly to have an apparatus operating at high temperatures.
Secondly, the lack of proper measurement techniques at high temperatures is the
other difficulty with this strategy (7).
In this work, a novel approach is proposed to induce IPFs inside a particulate media.
It involves large particles that are not significantly influenced by the Van der Walls
forces and other colloidal interactions. This technique uses a copolymer of
PMMA/PEA (Poly Methyl MethAcrylate/Poly Ethyl Acrylate) contained in a polymer
suspension called Eudragit NE30D. The copolymer, which is characterized by a low
glass transition temperature, around 9oC, is coated on inert particles by an
atomization process. By changing the ambient temperature to which the coated
particles are exposed, the polymer adhesion/friction parameters and Young Modulus
are modified in a way that the observed cohesive IPFs between the particles are
changed significantly. Accordingly, the cohesion between particles can be adjusted
by temperature in a stable and reproducible manner. The advantage of this method
is that it does not necessitate the addition of any liquid phase, which has to be
uniformly distributed into the particulate system. Besides, it allows the fluidization
study to be carried out at both low and high superficial gas velocities. In contrast to
the magnetic interactions, the forces are not dominant in only one direction, but are
located at each contact between the particles. Thus, there is no force anisotropy
present except if the temperature is not uniform in the system. The last priority of this
technique is that it can be conducted at low temperatures and IPFs are changed in a
completely controlled manner by merely a small increment in the system
temperature.
METHODOLOGY
Particle Coating Process
The experimental work necessitates having inert particles as base particles, which
can accept the copolymer of PMMA/PEA as the coating. A 450-720μm cut of
spherical sugar beads (dp=580μm, =1575 kg/m3), which lie in Geldart Group B
particles, were chosen as inert particles in this work.
Sugar beads were coated by an atomization process with a polymer suspension in
water and dried simultaneously to obtain a uniform coating on the particle surface. It
was achieved in a spheronizer, which allowed the introduction of air under the
rotating disc located inside the bowl. Table 1 presents operating parameters
associated with the coating process of the particles. Heated air, which was passed
through an electrical heater before entering the processing chamber, was used for
adjusting the temperature to the desired operating setpoint and also for concurrent
drying of the particles. The temperature was controlled with the help of a controller
coupled with an infrared cell, which measured the surface temperature of the
particles. In addition, a thermocouple located under the spheronizer disc allowed for
measuring the air entrance temperature. The air flow rate was adjusted to the
2

desired value with the help of a rotameter. The coating solution (Water 0.21 kg;
PMMA/PEA 0.086 kg; Nonoxynol100 0.004 kg) was added by atomization onto the
particles with a Schlick 970 series two-substance atomizer. The atomizer was fed
with the solution by a peristaltic pump with a flow rate approximately equal to 1 g/min
and compressed air, which allowed the formation of fine droplets. The atomizer gun
was arranged in such a manner that the tip of the nozzle was placed at
approximately 4 cm from the torus surface to avoid coating losses on the parts of the
equipment. The characteristics of the final product are summarized in Table 2.
Table 1. Spheronizer’s Operating Parameters Table 2. Final Particles Coating Characteristics
Disc rotational rate (rpm) 230 Materials Quantity
Air flow rate (cfm) 25 Spherical sugar beads 3.0 (kg)
Air temperature (oC) 30 PMMA/PEA 0.10 (kg)
Solution flow rate (g/min) 1 Mass percentage of coating 3.4 %
Atomization pressure (bar) 2 Coating layer thickness ~ 5
Experimental Set-up and Procedure for Fluidization Study
The experimental set-up used for the fluidization study consisted of a fluidization
column, which was constructed with a transparent Plexiglas tube with 0.152 m I.D.
and 1.5 m in height. Dried and filtered air was introduced into the bed through a
perforated plate as the distributor. It contained holes 1 mm in diameter arranged in a
triangular pitch.
Air was heated with the help of an electrical heater before entering the fluidizing
column. Accordingly, it was used to adjust the temperature of the bed to a desired
value. Temperature was controlled by means of a PI controller driven by a
thermocouple constantly immersed in the bed. A thermocouple located at the
windbox allowed measuring the air entrance temperature. Furthermore, the air flow
rate was controlled with a calibrated rotameter, which gave rise to a maximum
superficial gas velocity of 0.75 m/s in the bed. In this regard, different superficial gas
velocities were used for each system and temperature tested, covering both the
fixed bed state and bubbling regime.
To investigate the effect of IPFs on the fluidization behavior, two systems were
studied, uncoated sugar beads and coated sugar beads. Experiments of uncoated
sugar beads were carried out at 20oC while the ones for coated sugar beads were
conducted at different operating temperatures, 20oC, 30oC and 40oC. Hereafter, for
simplicity, we name these systems with their different operating conditions in
abbreviated form, SB, CSB20, CSB30 and CSB40, which stand for uncoated sugar
beads at 20oC and coated sugar beads at 20oC, 30oC and 40oC, respectively. All
experiments were performed at atmospheric pressure. It is worth noting that
variations in the air density and viscosity in the 20oC to 40oC temperature range are
6% and 5%, respectively, which are fairly negligible compared to the amount of
variation of cohesion, which rises from the new technique for the same temperature
range. Moreover, the same amount of material was poured into the bed for both
systems, which resulted in an initial bed height of approximately 20 cm at ambient
conditions.
The pressure drop across the bed was measured using a differential pressure
transducer. It was mounted flush with the wall of the bed through 15 micron inline
filters and measuring ports. In addition, a local measurement technique was
employed to investigate the influence of IPFs on the hydrodynamics of a gas-solid
fluidized bed. To study the dynamic local flow structure a parallel optical fiber probe
3

was employed to measure the instantaneous local bed voidage. The probe was
located 16 cm in height above the distributor and at the bed center for all the
experiments. This axial position for the probe ensured it was far away from the
turbulent effects of the distributor. For every temperature tested, the optical fiber
probe was calibrated according to the linear interpolation between the read voltage
of the air alone ( = 1) and the read voltage of the fixed bed.
Analysis Methods
The ratio between the measured and calculated pressure drop across the bed,
∆ /∆ , was used to highlight changes in the fluidization behavior of the coated
sugar beads with increasing temperature.
Analysis of local bed voidage can effectively provide much information about the
dynamics of the fluidized beds, which results in a better understanding about the
flow behavior in the fluidized bed (8). In this regard, the dynamic local two-phase
flow structure was analyzed for beds of different amounts of IPFs at each superficial
gas velocity. Instantaneous local bed voidage was at first scrutinized to have a
closer picture on gas and solids interaction in the bed for different operating
conditions. The time-averaged local bed voidage at the same measurement position
was also used to indicate the influence of IPFs on the local flow structure. The
probability density function of the local voidage from to 1 was analyzed to
quantitatively explain the gas-solid distribution of emulsion and dilute phases and its
dependence on the IPFs. According to Cui et al. (9), this is allowed for investigating
the dynamic behavior of the dilute and dense phases.
First and foremost, it was necessary to confirm that the new methodology for the
increment of cohesive IPFs can work properly after a slight increase in the system
temperature. It was verified in the spheronizer where coated particles were
prepared. To execute it, a required amount of inert particles with pharmaceutical
excipients was first produced and, subsequently, coated with a 30 layer of the
copolymer. Figure 1 shows the modification of the particulate system with
temperature. It can be easily demonstrated that by progressively increasing the
temperature, the surface of the particulate media, which was characterized by a
smooth profile with no observable deviations or clusters relative to the mean position
of the interface at 27oC, was gradually changed. It started to create apparent clusters
at 36oC, which became more obvious at 39oC, followed by the appearance of
significant structure modification at 40oC, the presence of a secondary particle flow
structure at the top of the main particle bed at 41oC and, finally, the moving of the
particle bed in mass at 43oC.
The most common approach for the overall identification of the fluidization status at
different velocities is studying the whole bed pressure drop as a function of
superficial gas velocity. The ∆ /∆ ratio can be used as a first indication of the
effect of IPFs on fluidization behaviour (10). Figure 2 shows that by increasing IPFs,
the degree of overshooting in the “fluidization” curve increases, which is
accompanied by the increment of minimum fluidization velocity (Umf). For the case of
CSB40, IPFs considerably influenced the bed’s behavior and caused the presence
of a mass of particles, which lifted as a plug rather than fluidizing. This effect is
shown in Figure 2.
4

27 oC 36 oC 39 oC
o
40 C 41 oC 43 oC
Figure 1. Modification of the particulate system with temperature in spheronizer.
1.6
Table 3. Variation of Fixed Bed Height
1.4
with IPFs
1.2
ΔPm / ΔPc
1.0 Fixed bed height (cm)

0.8
SB SB 20.3
0.6 CSB20
0.4 CSB30 CSB20 20.5
CSB40
0.2 ΔPc = Mg/A CSB30 21.4
0.0
0.0 0.1 0.2 0.3 0.4 0.5 0.6 CSB40 23
Ug (m/s)
Figure 2. Effect of IPFs on normalized pressure
drop profile in fluidization path.
Furthermore, a decrement of the measured/theoretical pressure drop ratio from unity

when the bed is fluidized shows the growth of the degree of cohesiveness of the bed
(1, 10). As can be found in Figure 2, for CSB20 the ∆ /∆ ratio is similar to SB,
while a decrement in the ratio is fairly observable for CSB30. For CSB40 fluidization
was not attained due to paramount effect of cohesive IPFs. These results show that
enhancement of IPFs can cause the behavior of the bed to change from Group B to
Group A and even Group C powders.
Formisani et al. (11) noted that voidage of the loosely settled bed of particles of
Groups A and B increases with temperature. They attributed these findings to the
increment of IPFs with temperature. Table 3 reports the variation of fixed bed height
with IPFs in this study. It reveals that the fixed bed height and, correspondingly, the
fixed bed voidage increase with IPFs. This result affirms Formisani et al. (11) and
indicates that a bed with higher IPFs can hold more gas in the fixed state.
The variations of local bed voidage with time reflect the interaction between gas and
solids phases, which can influence the mass and heat transfer rates in the fluidized
beds and, consequently, can affect the overall reaction rate in fluidized reactors (12).
Figures 3 – 6 show the evolution of instantaneous local bed voidage with superficial
gas velocity and IPFs for SB and CSB40. As can be found in these figures the
portion of the dilute phase increases with increasing gas velocity for both cases.
Therefore, the fluidizing air prefers to pass through the bed as a bubble phase.
However, it seems that IPFs have the opposite influence on local bed behavior. It
can be seen from Figures 3 – 6 that by increasing IPFs, the optical probe spends
5

more time in the emulsion phase rather than the dilute phase, which means that the
portion of the emulsion phase increases by the enhancement of IPFs. As a result,
the tendency of gas to pass the bed in the emulsion phase increases. It is worth
noting that the CSB40 has a higher saturated emulsion value ( ) compared to SB,
which is a subsequent consequence of holding more gas in the fixed bed state.
Moreover, a bed of higher IPFs has a dilute phase with a maximum voidage value
lower than unity, while in the case of SB there are some temporal signals of bed
voidage equal to unity, which are indications of pure bubbles. This can be referred to
the presence of more solid in the dilute phase for the particulate bed of enhanced
cohesive IPFs.
1.0 1.0
0.9
Local voidage ε (-)

0.9
0.8 0.8
0.7
0.7
0.6
0.6
0.5 εmf
εmf 0.5
0 2 4 6 8 10 0 2 4 6 8 10
Τime (s) Τime (s)

Figure 3. Signal of instantaneous local bed Figure 4. Signal of instantaneous local bed
voidage for SB (Ug = 0.41 m/s). voidage for CSB40 (Ug = 0.41 m/s).
1.0 1.0
0.9
0.9
0.8
0.8
0.7
0.7
0.6
0.6
0.5 εmf
εmf
0.5
0 2 4 6 8 10 0 2 4 6 8 10
Τime (s) Τime (s)
Figure 5. Signal of instantaneous local bed Figure 6. Signal of instantaneous local bed
voidage for SB (Ug = 0.74 m/s). voidage for CSB40 (Ug = 0.74 m/s).
The time-averaged local bed voidage was further investigated to give valuable
information about the effect of IPFs on the hydrodynamics of a gas-solid fluidized
bed. As it is illustrated in Figure 7 the time-averaged local bed voidage increases
with superficial gas velocity for particulate beds with different amounts of IPFs.
Moreover, for each superficial gas velocity tested in the bubbling regime the time
average local bed voidage decreases with increasing IPFs. This implies that the two-
phase flow structure at constant superficial gas velocity varies with a greater extent
for beds with higher IPFs.
Analysis of the probability density function of dynamic local voidage demonstrates
that for each superficial gas velocity tested, the probability of the dense phase and
dilute phase increases and decreases, respectively by increasing IPFs (Figures 8-
10). These findings indicate that the probability of the flow structure with higher
voidage is reduced and the whole flow structure becomes less dilute when IPFs are
enhanced. In addition, it can be found that at a given fluidizing gas throughput, with
6

enhancing IPFs, more gas enters into the emulsion phase and dilutes it rather than
passing into the bubble phase and increasing its fraction. Therefore, it can be
inferred that the behavior of the particulate bed shifts from Group B into Group A by
increasing IPFs in the bed.
Probability density function (%)

0.80
40 Ug = 0.41 m/s
0.75 Ug = 0.55 m/s
Ug = 0.74 m/s
0.70 30
0.65
20
0.60
SB
10
0.55 CSB30
CSB40
0.50 0ε
0.3 0.4 0.5 0.6 0.7 0.8 mf 0.5 0.6 0.7 0.8 0.9 1.0
Ug (m/s) Local voidage ε (-)
Figure 7. Variation of the average local voidage Figure 8. Probability density function of the local
with IPFs and superficial gas velocity. voidage of dynamic flow structure for SB.

40 Ug = 0.41 m/s 40 Ug = 0.41 m/s
Ug = 0.55 m/s Ug = 0.55 m/s
Ug = 0.74 m/s Ug = 0.74 m/s
30 30
20 20
10 10
0 εmf 0
0.5 0.6 0.7 0.8 0.9 1.0 0.5 εmf 0.6 0.7 0.8 0.9 1.0
Local voidage ε (-) Local voidage ε (-)
Figure 9. Probability density function of the local Figure 10. Probability density function of the local
voidage of dynamic flow structure for CSB30. voidage of dynamic flow structure for CSB40.
Overall, the experimental results of this work are in good agreement with those for
Yates and Newton (13) and Rowes et al. (14), who found that increasing the fines (<
45 ) content results in an increase in interstitial gas flow. In the range of IPFs
studied in this work, which defluidization phenomenon was not encountered within,
the presence of more gas in the fixed bed state and emulsion phase is an indication
of the improvement of gas/solid contact in the bed of Group B powders.
CONCLUSION
This work introduces a new and different approach to study the effect of IPFs on the
fluidization behavior of the gas-solid fluidized bed. It was shown that by controlling
the temperature of the particulate system of inert particles coated with a layer of a
PMMA/PEA copolymer, the degree of cohesiveness of the bed can be easily
changed in a selective manner. Interesting aspects of this approach for increment of
IPFs are working at low bed temperatures, controlling the level of cohesiveness by
merely controlling the bed temperature and facilitating the investigation of the
influence of IPFs on fluidization characteristics from low to high superficial gas
velocities.
Experimental results obtained by local and global measurement techniques show
that increment of IPFs can significantly affect the dynamic local flow structure and
overall behavior of the gas-solid fluidized bed. Dictating higher amounts of IPFs into
7

the bed causes higher fixed bed voidage and minimum fluidization velocity. Similarly,
there is a significant influence of IPFs on the bed behavior in the bubbling fluidization
regime. The results obtained in the range of IPFs studied in this work imply that at a
given throughput of the fluidizing gas, the relative tendency of gas flowing in the
emulsion phase increases with IPFs, which has a positive effect on enhancing
chemical conversion in the case of the active catalyst. According to experimental
results, it can be concluded that by increasing IPFs the fluidization behavior of the
particulate bed can shift from Group B to Group A or even Group C powders.
NOTATION
A bed cross-section area (m2) ∆ measured pressure drop (N/m2)

dp mean particle diameter (μm)
M bed weight (kg) Greek Letters
Umf minimum fluidization velocity (m/s) local voidage (-)
Ug superficial gas velocity (m/s) minimum fluidization voidage (-)
∆ Mg/A (N/m2) particle density (kg/m3)
REFERENCES
1. Geldart, D., Harnby, N. and Wong, A.C., Fluidization of cohesive powders. Powder
Technology, 1984. 37(1): p. 25-37.
2. Seville, J.P.K. and Clift, R., The effect of thin liquid layers on fluidisation characteristics.
Powder Technology, 1984. 37(1): p. 117-129.
3. Rhodes, M.J., Wang, X.S., Forsyth, A.J., Gan, K.S. and Phadtajaphan, S., Use of a
magnetic fluidized bed in studying Geldart Group B to A transition. Chemical Engineering
Science, 2001. 56(18): p. 5429-5436.
4. Lettieri, P., Yates, J.G. and Newton, D., The influence of interparticle forces on the
fluidization behaviour of some industrial materials at high temperature. Powder
Technology, 2000. 110(1-2): p. 117-127.
5. Fraysse, N., Thomé, H. and Petit, L., Humidity effects on the stability of a sandpile. The
European Physical Journal B - Condensed Matter and Complex Systems, 1999. 11(4): p.
615-619.
6. Lumay, G. and Vandewalle, N., Controlled flow of smart powders. Physical Review E,
2008. 78(6): p. 061302.
7. Cui, H. and Chaouki, J., Effects of temperature on local two-phase flow structure in
bubbling and turbulent fluidized beds of FCC particles. Chemical Engineering Science,
2004. 59(16): p. 3413-3422.
8. Zhu, H., Zhu, J., Li, G. and Li, F., Detailed measuremnets of flow structure inside a dense
gas-solids fluidized bed. Powder Technology, 2008. 180(3): p. 339-349.
9. Cui, H., Mostoufi, N. and Chaouki, J., Characterization of dynamic gas-solid distribution
in fluidized beds. Chemical Engineering Journal, 2000. 114(1-3): p. 133-143.
10. Bruni, G., Lettieri, P., Newton, D. and Barletta, D., An investigation of the effect of the
interparticle forces on the fluidization behaviour of fine powders linked with rheological
studies. Chemical Engineering Science, 2007. 62(1-2): p. 387-396.
11. Formisani, B., Girimonte, R. and Mancuso, L., Analysis of the fluidization process of
particle beds at high temperature. Chemical Engineering Science, 1998. 53(5): p. 951-
961.
12. Mostoufi, N. and Chaouki, J., Local solid mixing in gas-solid fluidized beds. Powder
Technology, 2001. 114(2): p. 23-31.
13. Yates, J.G., and Newton, D., Fine particle effects in a fluidized-bed reactor. Chemical
Engineering Sceince, 1986. 41(4): p. 801-806.
14. Rowe, P.N., Santoro, L., and Yates, J.G., The division of gas between bubble and
interestitial phases in fluidized beds of fine powders. Chemical Engineering Sceince,
1978. 33(1): p. 133-140.
8

CO-COMBUSTION OF HAZELNUT SHELLS WITH A HIGH-
SULFUR TURKISH LIGNITE IN A CIRCULATING FLUIDIZED
BED COMBUSTOR WITH AIR STAGING
Aysel T. Atimtaya*, Hayati Olgunb, Murat Varola, Mustafa Can Çelebic, Hüsnü
Ataküld, Ufuk Kayahanb, Berrin Bayb, Alper Ünlüb, Gerçek Bardakçıoğlue, Murat
Özcane
a
Middle East Technical University, Dept. of Environ. Eng., 06531 Ankara, Turkey
b
TUBITAK-MRC, Energy Institute, P.O.Box 21, Gebze 41470, Kocaeli, Turkey
c
Istanbul Technical University, Energy Institute, Maslak 34469, Istanbul, Turkey
d
Istanbul Technical University, Dept. of Chem. Eng., Maslak 34469, Istanbul, Turkey
e
GAMA Power Systems Engineering and Contracting, Inc., 06520 Ankara, Turkey
ABSTRACT
In this study, a high-S lignite coal was burned with hazelnut shells in a laboratory
scale circulating fluidized bed with secondary air injection. The results showed that
emissions can be reduced with the addition of secondary air. The objective of the
study was to maximize combustion performance, minimize the emissions, and to
see the effect of various amounts of secondary air injection on emissions.
INTRODUCTION
Combustion of mixtures of different fuels, particularly biomass materials with coal, in
a fluidized bed combustor is a promising application to produce cleaner energy as
well as to dispose waste products of biomass resources. In addition to this,
combustion of biomass materials as a supplementary fuel for coal-fired power plants
has an advantage of saving money for the fuel cost. Moreover, co-combustion of
biomass with coal is also an effective way to reduce CO2 emissions (1). Annual
amount of hazelnut shells in Turkey is 566,437 tons and the corresponding total
heating value is 8,745,790 GJ (2). This waste can be used in energy production.
Youssef, et al. (3) conducted the combustion of four different kinds of biomass in a
circulating fluidized bed with 145 mm inner diameter and 2 m height. Different
excess air ratios were utilized in experiments. Desroches-Ducarne, et al. (4)
investigated the emissions of NO, N2O, HCl, SO2 and CO during co-combustion of
coal and municipal refuse mixtures in a circulating fluidized bed boiler. Cliffe and
Patumsawad (5) studied the co-combustion of olive cake with coal. They used
fluidized bed combustor to research the feasibility of using olive cake as an energy
source. Armesto, et al. (6) investigated the co-combustion of coal and olive oil
industry residues in fluidized bed. Two different Spanish coals, lignite and anthracite
were used for the study. Topal, et al. (7) investigated the olive cake combustion in a
CFBC. They used a small scale circulating fluidized bed of 125 mm diameter and
1800 mm height. The results obtained from this combustor were used to compare
them with that of coal combustion. Permchart and Kouprianov (8) made an
experimental study about the combustion of three different biomass sources in a
single fluidized bed combustor (FBC). Atimtay and Topal (9) studied the co-
combustion of olive cake with lignite coal in a CFB. Experiments were conducted in
the same bed used in the previous work by Topal, et al. (7). In all of these studies, it
was found that all biomass materials are good candidates to be used as
supplementary fuels to various coals, especially lignite coals. However, combustion
and co-combustion of hazelnut shells were not studied before.
MATERIALS AND METHODS
A laboratory scale CFBC system was used for small scale tests before going into
pilot scale studies of 0.75 MWth. The thermal capacity of the laboratory scale CFBC
was 30 kW as shown in Fig.1. The experimental setup consists of a riser, a down
comer, a fuel feeding system, electrical heaters, and two cyclones. The lab-scale
combustor column (riser) has an inside diameter of 108 mm and a height of 6 m. It
consists of 8 modules. Six electrical heaters are used along the combustor column
in order to heat the system during the start-up period. The effect of staged air
injection on the emissions from several ports along the column has been studied.
The temperature of the riser column was kept at 850 oC during the combustion
experiments. Combustion tests were carried out with Orhaneli lignite coal as the
main fuel. Hazelnut shells were used as the auxiliary fuel (biomass). The fuel
particles were between 1-2 mm. The proximate and ultimate analyses of fuels are
presented in Table 1. During the experiments, CO, SO2, NO, and O2 emissions were
continuously measured with the ABB/AO2000 flue gas analyzer. Calibration of the
flue gas analyzer was done with certified calibration gases. Figure 1 shows the
experimental system. The measurements were also checked with GASMET DX-
4000 Flue Gas Analyzer. All emission concentrations measured are expressed on
6% oxygen basis.
Figure 1. Schematic view of laboratory scale experimental system

Table 1. Characteristics of fuels
Orhaneli Lignite Hazelnut shell
Proximate Analysis Ash, wt % 23.09 1.52

(wet basis)
Volatile Matter, wt % 34.40 64.73
Fixed Carbon, wt % 20.18 21.78
Moisture, wt % 22.33 11.97
Lower Heating Value, kJ/kg 11,829 18,933
Higher Heating Value, kJ/kg 12,962 20,326
Ultimate Analysis (dry C, wt % 41.48 56.34
basis)
H, wt % 2.37 5.35
N, wt % 0.54 0.51
O, wt % 24.12 36.06
S (Total), % 1.76 0.01
Ash, wt % 29.73 1.73

Combustion Experiments
Temperature Distribution: The temperature profiles along the combustor with and
without secondary air injection (SAR) was between 790-850°C. During the
experiments, the total amount of air given to the system was held constant. The ratio
of secondary air to total air was changed. The increase in the SAR causes a
temperature increase in the dense phase and the maximum temperature was
observed at about 240 mm above the distributor plate due to better combustion of
volatiles. Later on, as the height increases a decrease in the temperature is
observed due to cooling effect of secondary air. Throughout the experiments
secondary air was fed to the 3rd, 4th 5th and 6th modules.
Emissions: All the emission data presented in this section were taken for the dense
phase temperature of 85050°C. Fig. 2 demonstrates the CO emissions resulting
from the fuel mixture of Orhaneli Lignite (OL) and Hazelnut Shells (HS) for three
different ratios, namely 90 wt% OL-10 wt% HS, 70 wt% OL-30 wt% HS and 50 wt%
OL-50 wt% HS. In Fig. 2, CO emissions vs. SAR are plotted for different places at
which the secondary air is injected. As it is seen from Fig. 2a, 2b and 2c, CO
emissions do not suddenly decrease as the secondary air is introduced. Instead, CO
emissions increase up to a certain point as the secondary air is introduced for case
(a) and (c). The reason for increasing CO concentration might be the Boudouard
reaction where char is reacted with CO2 to give CO (10). It was observed that after
the secondary to total air ratio exceeds 20%, CO emissions display a decreasing
trend. Highest CO concentrations are observed for the case where the secondary air
is injected at a height of 400 mm from the distributor for case (a), and at a height of
220 mm from the distributor for case (c). In both cases SAR value was 20%.
a b
Figure 2: CO emissions with different secondary air ratios: (a) 90% by wt. OL -10%
by wt. HS with primary air, (b) 70% by wt. OL -30% by wt. HS with primary air,
(c) 50% by wt. OL -50% by wt. HS with primary air
a b
Figure 3: CO, NO, N2O emissions with different secondary air ratios, when staged
air is introduced 139 cm above the distributor plate: (a) 90 wt% OL-10wt% HS,
(b) 70 wt% OL-30 wt% HS, (c) 50 wt% OL-50 wt% HS
Fig.3 shows the CO, NO and N2O emissions resulting from co-combustion of
various ratios of OL and HS. NO emissions followed a decreasing trend for all SAR
values. As it was shown in Fig. 2a and 2c before, CO concentrations increased until
SAR value of 20% and then decreased. It was reported in the literature before that
CO has an important role in NO reduction (7, 8). Besides, NO emissions slightly
dropped for all SAR values. The reason might be the cooling effect of secondary air
injection after some values of SAR.
Fig. 3a shows CO emissions having a declining trend for different mixtures with SAR
after a certain SAR value. It was thought that this may be due to lower volatile
matter (VM) content of the hazelnut shells (64.7%) as compared to other biomasses.
As the fuel particles are introduced into the combustor, VM in the fuel immediately
volatilizes and the medium becomes oxygen deficient. Therefore, some incomplete
combustion products like CO can form. When secondary air is injected, this helps
the combustion to be better. Since the VM content of the hazelnut shells is not very
high, the secondary air injection becomes effective starting with small SAR values.
Another point to notice is that as the HS content in the fuel mixture increases, CO
emissions also increases. As in the case of 90% coal-10% HS, CO concentration
was maximum 300 mg/Nm3, but with the hazelnut shell in the mixture increases to
50%, CO concentration went up to 800-1100 mg/Nm3.
Figs. 4, 5 and 6 show the change of NO, N2O and NO2 emissions with height above
the distributor plate for 10%, 30% and 50% HS addition to Orhaneli lignite,
respectively. In each case, secondary air ratios of 10%, 20% and 30% are tried. In
all of these figures, one can see that NO2 concentration is almost zero. N2O
concentration is small and NO concentration is the most prominent among these
three. As can be seen in Fig.4a, NO concentration starts at 330 mg/Nm3 in the
second module and decreases with height along the combustor. The same trend is
observed in the other figures. However, as SAR increases from 10 to 30%, NO
concentration decreases down to 200-250 mg/Nm3. The reason might be the cooling
effect of secondary air injection.
In Fig.5, a similar trend is observed for NO concentration where in this case 30% HS
is mixed in the fuel mixture. NO concentrations are around 200-250 mg/Nm3. In
these cases SAR is 10% and 20%. However, when SAR is increased to 30%, NO
concentration increases along the height of the combustor and goes up to 350
mg/Nm3. This behaviour could not be explained.
In Fig.6, again a similar trend is observed for NO concentration where in this case
50% HS is mixed in the fuel mixture. NO concentrations decrease slightly along the
combustor height. The concentrations are around 200-250 mg/Nm3. Then with the
increase of SAR to 30%, the concentration drops to 150 mg/Nm3. These decreases
are thought to happen due to dilution effect with increasing SAR. N2O and NO2
concentrations stay almost the same, with very slight changes as SAR increases.
a b
Figure 4: Change of NO, N2O and NO2 emissions with height above the distributor
plate for 90 wt% OL-10 wt% HS: a) SAR 10%, b) SAR 20%, c) SAR 30%
a b
plate for 70 wt% OL-30 wt% HS : a) SAR 10%, b) SAR 20%, c) SAR 30%
a
b
plate for 50 wt% OL-50 wt% HS : a) SAR 10%, b) SAR 20%, c) SAR 30%
Combustion Efficiency
Combustion efficiency is calculated according to the Equations (1) to (4). The results
of unburnt carbon analysis are given in Table 2. It is clear that, the unburnt carbon is
negligible both in the bottom and in the fly ash for all runs. Carbon loss during the
combustion is mainly originated from CO formation.
Table 2: Unburnt C analysis results
Bottom LCO Lbottom Lfly η

Ash Fly Ash Fuel Mixture % % % %
0 0 90 % wt. OL-10 % wt. HS 2.70 - - 97.30
0.043 0.182 70 % wt. OL-30 % wt. HS 1.55 0.02 0.05 98.38
0 0.384 50 % wt. OL-50 % wt. HS 0.92 - 0.05 99.03
LCO = CO ppm, measured * V fluegas, measured * HL_CO / HL_fuel / 10,000 (1)

Lbottom = Ashbottom * Cbottom * HL_Char / Mf / HL_fuel * 100 (2)
Lfly= Ashfly* Cfly* H L_Char / Mf / HL_fuel * 100 (3)
η = 100 - (LCO + Lbottom + Lfly) (4)
where LCO is the percentage of the total carbon loss due to CO formation; Lbottom is
the percentage of the total carbon loss in the bottom ash; Lfly is the percentage of the
total carbon loss in the fly ash; and η is the total combustion efficiency. As can be
seen from the table, the combustion efficiency for all mixtures are found to be
greater than 97.3%.
CONCLUSION
The results of this study have shown that the co-combustion of lignite coal with
hazelnut shells in a CFBC can be performed with minimum emissions. With the
injection of secondary air into the combustor, CO emission trends were found to be
different for SAR< 20% and SAR> 20%. CO presence in the emissions helped the
NO reduction. Further tests with several combinations of sorbent addition with air
staging will be carried out to obtain the optimum emission performance for future
work.
ACKNOWLEDGEMENT
The financial support provided by the Turkish Scientific and Technical Research Council
(TUBITAK) under the project code of TUBITAK-KAMAG-105G023 is greatly appreciated.
NOTATION
SAR: secondary air ratio LCO: combustion loss due to CO emission
(secondary air/total air) measured in stack gas
η: combustion efficiency (%) HL_CO: Lower heating value of CO
Lfly: combustion loss due to (∆Hc 0, Heat of combustion), 12.63 MJ/Nm3
unburnt C contained in fly ash CO (Perry, 2007)
HL_Char: Lower heating value of char
Lbottom: combustion loss due to
(∆Hc 0, Heat of combustion), 32.79 MJ/kg
unburnt C contained in bottom ash char (Perry, 2007)
HL_fuel: Lower heating value of the fuel used
REFERENCES
1 Hupa M., “Interaction of Fuels in Co-Firing in FBC”, Fuel, 2005, 84, 1312-1319.
2 Biosynergy Workshop 17-18 April 2008, Petten.
3 Youssef M.A., Wahid S., Mohamed M.A., Askalany A.A., “Experimental Study on
Egyptian Biomass Combustion in Circulating Fluidized Bed
4 Desroches-Ducarne E., Eric M., Gerard M., Lucien D., “Co-combustion of Coal and
Municipal Solid Waste in a Circulating Fluidized Bed”, Fuel, 1998, 77, 1311-1315.
5 Cliffe K.R., Patumsawad S., “Co-combustion of Waste From Olive Oil Production With
Coal in a Fluidised Bed”, Waste Management, 2001, 21, 49-53.
6 Armesto L., Bahillo A., Cabanillas A., Veijonen K., Otero J., Plumed A., Salvador A., “Co-
combustion of Coal and Olive Oil Industry Residues in Fluidized Bed”, Fuel, 2003, 82,
993-1000.
7 Topal H., Atimtay T.A., Durmaz A., “Olive Cake Combustion in a Circulating Fluidized
Bed”, Fuel, 2003, 82, 1049-1056.
8 Permchart W., Kouprianov V.I., ”Emission Performance and Combustion Efficiency of a
Conical Fluidized Bed Combustor Firing Various Biomass Fuels”, Bioresource
Technology, 2004, 92, 83-91.
9 Atimtay A. T., Topal H., “Co-combustion of Olive Cake With Lignite Coal in a Circulating
Fluidized bed”, Fuel, 2004, 83, 859-867.
10 Xie J, Yang X, Zhang L, Ding T., Song W.,Lin W., “Emissions of SO2, NO and N2O in a
circulating fluidized bed combustor during co-firing coal and biomass”, Journal of
Environmental Sciences, 2007, 19, 109-116.
11 Gungor A., “Simulation of NOx emission in circulating fluidized bed burning low
grade fuels”, Energy and Fuels, 2009, 23, 2475-2481.
12 Adanez J., Diego L.F., Gayan P., Cabanillas A., “Modeling of Sulfur Retention in
Circulating Fluidized Bed Combustors”, Fuel, 1996, 75 (3), 262-270.
COMPARISON BETWEEN MEASUREMENTS AND NU
MERICAL SIMULATION OF PARTICLE FLOW AND
COMBUSTION AT THE DUISBURG CFBC PLANT
M. Weng1), J. Plackmeyer2)
1)
aixprocess GmbH, Aachen (Germany)
2)
Consulting Engineer, Bergisch-Gladbach (Germany)
ABSTRACT
The article presents the 3-dimensional numerical simulation of combustion and
particle flow as an efficient engineering tool for analysis and optimization of fluidized
bed combustion chambers. The comparison with measurements that were carried
out within a European Research Project and with operational experience shows very
good agreement and provides recommendations for future optimization.
SCOPE OF THE STUDY

After retrofitting the Duisburg CFB combustion chamber with elongated heat ex
changer modules, the plant showed a significant increase in local wear and corro
sion. The reason was supposed to be a locally reducing atmosphere from high CO
concentrations. In order to verify this hypothesis and to develop adequate optimiza
tion measures, a comprehensive simulation study was performed. For this plant,
measurements are available concerning local solids volume fraction and temperat
ure, Wischniewski et al. (1). Hence, the Duisburg CFBC appears to be adequate to
prove the capability of numerical simulation in large scale fluidized bed combustors.
Figure 1: Duisburg CFBC design
1
Fig. 1 shows the combustor design with inlet and recycle ports, integrated heat ex
changer modules and the exit to subsequent cyclones. For the simulation study, the
primary air is assumed to have a uniform profile at the distributor due to high nozzle
pressure head. Secondary air is injected via 4 inlet nozzles with a velocity of appr.
80 m/s. In operation with 100% coal, solid fuel enters through 2 discrete ports loc
ated on one side of the combustion chamber. In secondary fuel co-firing operation,
coal-substituting matter is injected through 2 inlets located on the opposite side.
SIMULATION METHOD
Numerical Simulation in Fluidized Beds and Dense Particle Flows
Many different fluidized bed simulation studies have been reported historically. How
ever, most or all of these studies reveal significant simplifications according to local
discretization, coupling between particle and gas phase or the computation of com
bustion phenomena. The commercial software code Barracuda® employs a different
approach based on the Computational Particle Fluid Dynamics (CPFD®) method,
Snider (2). It overcomes the shortcoming traditionally seen in CFD fluidized bed sim
ulations. This is done by a bi-directional coupling between the discrete motion of
Lagrangian particles and the continous gas phase for which the Navier-Stokes
equations are solved. The simulation is strictly transient, thus accounting for the in
herently fluctuating character of flows with high solid volume fractions.
In the lower part of a CFB the flow is dense with local solid volume fractions > 10%.
In this regime, the two-phase flow is governed by particle-particle interactions. Typ
ically the fuel is injected into this region, so the proper computation of solids mixing
and jet penetration is crucial for the prediction of process characteristics. The simu
lation method considers the particle interactions by integrating the discrete particle
properties in each computational cell, hence forming a particle stress tensor for
which a transport equation is computed within the Eulerian frame of reference. The
result of this solution is then mapped back onto the respective position of each
single particle. This hybrid particle interaction model then solves the particle equa
tion of motion by balancing drag, pressure gradient, volume forces and an additional
expression for particle normal stress representing multiple particle interactions.
A characteristic feature of the Barracuda® software is that particles displace the sur
rounding continuous phase (see Fig. 2). As a consequence, the Eulerian phase
computational domain is a highly complex transient 3-dimensional space, thus en
abling the realistic representation of large scale fluctuations in dense particle flows.
particle
fluid
particles displace the fluid
Figure 2: CPFD Barracuda method for the continuous phase region
For reacting flows, the continuous phase momentum transport equations and
particle motion are coupled with scalar equations for energy and gas phase species
(O2, N2, H2O, CO, CO2, …). The set of equations is completed by closure terms for
2
homogeneous and heterogeneous reactions. The respective reaction rates are com
puted at each location and time step.
The resulting variable sequences provide a deep insight into the complex structure
of dense particle flows. Time- and space-averaging of instantaneous values enables
quantitative studies and form the base for comparison with measurements. Never
theless, all information about variable fluctuations is preserved.
Modeling of Coal and Secondary Fuel Combustion

In the present simulation study, two fuel compositions were considered. Tables 1
and 2 show the short analysis of coal and Meat-and-Bone-Meal (MBM) as a typical
secondary fuel (SF).
Table 1: coal composition

Component weight- %
Moisture 14 -16
total carbon 75-80
Ash 8-10
Volatiles 40-43
Table 2: composition meat-and-bone meal (MBM)

Component weight- %
Moisture 4
total carbon 42
ash 21
volatiles 66
Table 3: stoichiometric equations for the reduced combustion mechanism

Steam gasification C(s) + H2O ↔ CO + H2
CO2 gasification C(s) + CO2 ↔ 2CO
Combustion λC(s) + O2 → 2(λ-1)CO + (2-λ)CO2
Water gas shift CO + H2O ↔ CO2 + H2
Volatile combustion CxHyOz + αO2 → βCO2 + γH2
CO combustion 2CO + O2 → 2CO2
Each solid fuel is represented by its specific particle size distribution (milled coal d50
= 320 micron, MBM d50 = 450 micron). The loss of particle matter due to reaction is
considered by a shrinking particle model. At the beginning of the calculation, the ash
content is initialized with a typical mass of bed ash and an initial particle size distri
bution with 220 micron mean diameter). The homogeneous and heterogeneous fuel
reactions are represented by a reduced mechanism (see Table 3).
3
The equilibrium reactions are split into single equations for forward and backward
reactions. All kinetic reactions rates are taken from approved references, Syamlal
and Bisset, Yoon et al., Bustamante et al. [3-5]. Simplifying the complex heat and
mass transfer in partially porous particles, moisture and volatile fuel contents are as
sumed as gaseous inlet streams. The model error is considered to be small since
drying and volatiles evaporation are very fast at fluidized bed conditions with relat
ively small fuel particles. For the presented study, the coal and secondary fuel com
bustion system was modeled in the Barracuda code for the first time.
COMPARISON BETWEEN SIMULATION AND MEASUREMENTS

With a sophisticated experimental setup, local solid phase volume fractions, gas-
phase temperatures, pressure profiles and concentrations were taken in the inner
region of the Duisburg plant. The objective of the study was to investigate the influ
ence of secondary fuel co-firing on emissions and solid phase inventory. The opera
tional data used as a base for simulation boundary condition definition are slightly
different from the load case during the measurement campaign. The exact operation
conditions could not be reconstructed with total agreement according to SF compos
ition and position of injection. However, the comparison between different load
cases with and without co-firing of SF is assumed to sufficiently represent the overall
plant characteristic in order to evaluate the simulation quality.
The operation conditions were 100% load each. In the first case, 100% coal is used,
for the co-firing case 25% of the heating value is substituted by MBM which enters
via 2 ports opposite from the coal injection.
Figure 3: local solid phase volume fraction for 100% coal combustion and co-firing
conditions: comparison between simulation and measurements
Fig. 3 shows profiles of the local solid phase volume fraction vs. height above the
primary air distributor. Measurement positions are within the inner chamber region
without the influence of the dense near-wall particle wall carpet. Position “Front” is
the coal injection side, “back” is opposite in the lateral direction. The heat exchanger
modules are located between the measurement positions 17 m and 27 m. In the
simulation, virtual sensors were installed at respective positions within the computa
tional domain and values were time-averaged to receive statistically sound values.
Simulation and measurements are in good agreement and show the strong volume
fraction decay in the region 8 m to 13 m above the air distributor. Above secondary
air injection, the volume fractions decrease slightly up to the cyclone entrance.
Again in good agreement is the tendency towards a higher solid content in the co-fir
4
ing case. The maldistribution between front and back side is given correctly, too. Re
garding the difficult measurement conditions and the model simplifications, even the
absolute values are in remarkable agreement.
Fig. 4 shows the temperature profiles in the combustor. The absolute discrepancy
between local measured and simulated values is small, only the front side temperat
ure below the heat exchanger being 35° lower compared to the measured value.
Again, the profile trends between front and back side and load cases with and
without co-firing are given correctly.
Figure 4: local gas phase temperature for 100% coal combustion and co-firing con
ditions; comparison between simulation and measurement
The corresponding profiles show that a considerable fraction of the overall combus
tion takes place in a region higher than 15 m above the distributor and that the burn-
out is not finalised in the heat exchanger zone. Mean temperature difference
between front and back side is 30 – 50°C. This discrepancy decreases for co-firing
conditions with SF feeding on the back side. Furthermore the profiles show coincid
ently the lack of lateral mixing throughout the whole combustion chamber.
SIMULATION RESULTS AND OPERATIONAL EXPERIENCE

The internal circulation of solid matter within the combustion chamber plays an im
portant role for the overall solids inventory and its residence time distribution. The in
ternally recycled solids form a dense layer that flows downwards in a near-wall re
gion. For the 100% coal case, fig. 5 gives the time-averaged particle velocities on
the left hand side and the solids volume fraction on the right. The penetration depth
of the secondary air injected with 80 m/s is below 1.5 m which is remarkably low.
The reason is a high momentum stream due to the relatively dense particle flow that
is further accelerated by gas-phase mass and heat sources from the combustion re
actions. The dense particle wall film can be clearly seen. The mean downward velo
city is 2 m/s which is in good agreement with observations from similar plants.
The upward flow in the combustion region has an average velocity of 15 m/s and
stretches out up to the heat exchanger. The vector plot of instantaneous gas velocit
ies in Fig. 6 demonstrates the high fluctuations with maximum velocities above
25 m/s. The effect of high mean velocity combined with large amplitude fluctuations
on wear can be seen in Fig. 7. Barracuda explicitly calculates the wear effect from
an integration of particle velocity and impact angle from each particle that hits the
wall. Although this value is qualitative, it provides useful information about the posi
tion of maximum wear in a plant. Fig. 7 shows the wear at the heat exchanger plates
5
as a comparison of the outer (left picture) and a centre position (right picture). The
predicted region of maximum wear above the coal injection is in excellent agree
ment with operational experience.
volume
vel [m/s] fraction [-]
15.0 0.5
0.0 0.0
Figure 5: time-averaged particle velocity vectors and solid volume fraction at the
combustion chamber centre plane; coal is injected from the right hand side
vel [m/s]
25.0
0.0
t - 2s t t + 2s
Figure 6: Instantaneous particle velocities in a plane of the coal inlet (coal injection
from the right)
In addition to mechanical wear, the heat exchanger region experiences a chemical

impact from a locally reducing atmosphere. Fig. 8 shows the time-averaged oxygen
mole fraction in the centre plane for 100% coal firing (left) and 25% MBM co-firing
(right). The oxygen maldistribution is clearly to be seen. Due to the lack of lateral
mixing, nearly the complete fuel stream including the volatiles remains on the coal
injection side leading to incomplete burnout and local lack of oxygen. Secondary air
injected from the opposite side is not sufficient for mixing and does not reach the
zone of high fuel content. The oxygen-poor streak stretches out into the cyclone in
6
let. The cyclone high turbulence intensities will then induce mixing and reaction of
the fuel- and oxygen-rich streaks, respectively. This tendency is underlined by oper
ational experience. Temperatures of 950° to 1050°C are observed in the cyclone
and in the transfer duct to the subsequent heat exchangers.
Figure 7: qualitative wear prediction
Figure 8: comparison of time-averaged oxygen mole fractions for 100% coal firing
(left) and 25% MBM co-firing (right)
MBM injection on the coal-opposite side leads to a slight equalization in oxygen con
centration. There still exists a region with lower oxygen concentration in the center
due to the low secondary air penetration depths and the poor lateral mixing. Here,
the simulation reveals further optimization potential according to the position of sec
ondary air injection. Above the MBM injection port there is a zone with oxygen con
7
centration near zero. This is due to the high MBM volatiles content and the resulting
oxygen consumption. The volatiles combustion rate decreases and restarts above
the secondary air nozzle. To displace the combustion zone and use the complete
height of the combustion chamber, the simulation indicates a relocation of the back
side secondary air nozzle in the downward direction (about 3-4 m).
CONCLUSIONS
The advanced particle flow and reaction simulation of the Duisburg CFBC shows
very good agreement with local in-situ measurements and additional operational ex
periences. The tendencies of characteristic parameters such as local solids volume
fraction and temperatures are predicted correctly, the identification of wear-intensive
regions is reliable. The high resolution in time and space enables detailed analysis
of the plant characteristics and remarkably enhances the understanding of the com
plex coupled flow and reaction behaviour. The high information density including fre
quency and amplitude of fluctuations which are characteristic for dense particle
flows underlines the relevance of advanced simulation tools for plant optimization.
Analogous to well-established simulations of pulverized-coal combustion plants with
conventional CFD methods, now by means of the Barracuda method the effect of
fuel scenarios and geometric modifications on emissions, wear and local heat im
pact can be reliably predicted for fluidized bed applications.
NOTATION
CFB circulating fluidized bed
d50 particle mean diameter
MBM meat and bone meal
SF secondary fuel
REFERENCES
[1] Wischnewski, R. , Werther, J. and Heidenhof, N. (2006): Synergy effects of
co-combustion of biomass and sewage sludge with coal in the CFB-combustor of
Stadtwerke Duisburg AG. VGB Power Tech, 86(12), pp 63-70, 2006
[2] Snider, D. M., 2001, An Incompressible three dimensional multiphase
particle-in-cell model for dense particle flows. Journal of Computational Physics 170,
523-549
[3] Syamlal, M., Bissett, L.A., 1992, METC Gasifier Advanced Simulation
(MGAS) Model, DOE/METC--92/4108, DE92 001111
[4] Yoon, H., Wei, J. And Denn, M.M., 1978, A Model for Moving-Bed Coal Gasi
fication Reactors. AIChE Journal 24, 5
[5] Bustamante, F., Enick, R. M., Cugini, A., Killmeyer, R. P., Howard, B. H.,
Rothenberger, K. S., Ciocco, M. V., Morreale, B. D., Chattopadhyay, S. and Shi, S.
(2004), High-temperature kinetics of the homogeneous reverse water–gas shift re
action. AIChE Journal, 50: 1028–1041
8
COMPARISON OF ENTRAINMENT RATE IN ACRYLONITRILE
REACTORS USING PLANT DATA AND CFD SIMULATIONS
S. Moffatt1, S. Ramchandran1, P. Zhao2, and K. Williams2

1
Ascend Performance Materials, LLC, PO Box 711,FM 2917,Alvin, TX 77512
2
CPFD Software, LLC,10899 Montgomery Blvd. Suite B,Albuquerque, NM 87111
ABSTRACT
Accurate entrainment rates are important in fluidized bed reactors for several reasons, including
determination of cyclone loadings and efficiencies, sizing of diplegs, and inputs to population
balance models. Entrainment correlations exist in the literature and from other sources to predict
entrainment rates from fluidized beds, but they can vary by orders of magnitude. In addition,
many correlations do not take into account effects of internals which are present in many types of
industrial reactors. A study was undertaken to better understand entrainment rates from Sohio-
type acrylonitrile fluidized bed reactors containing catalyst classified as a Geldart type A powder.
As part of this study, full scale CFD models were developed using the Barracuda® computational
particle fluid dynamics (CPFD®) software and validated with the help of data collected from
multiple plant reactors. These models compared two different sizes of industrial-scale reactors
and included all major internals including cooling coils, cyclones, cyclone diplegs and gas
spargers.
Data on the pressure profile and actual entrainment rate to the cyclones generated by the
Barracuda models were compared to the measured pressure data and derived entrainment rate
in the plant reactors. The results showed good agreement. Additionally, evaluation of using the
slip factor in the model to compare the particle volume fraction in the freeboard to the actual
entrainment rate was done to determine if this technique could be used in the plant setting. The
slip factor as calculated by Barracuda was between 1.55-1.95 which is similar to other values in
the literature.
INTRODUCTION
Barracuda® CPFD model pressure profiles and entrainment rates were compared to plant reactor
data from two different diameter Acrylonitrile reactors. In the industrial setting, accurate
entrainment rates are important in fluidized bed reactors for several reasons, including
determination of cyclone loadings and efficiencies, sizing of diplegs, and inputs to population
balance models. Entrainment correlations exist in the literature and from other sources to predict
entrainment rates from fluidized beds, but they can vary by orders of magnitude. In addition,
many correlations do not take into account effects of internals which are present in many
industrial reactors. In contrast, a full-scale Barracuda model can take into account effects of
particle size distribution and effects of internals and reactor walls. In addition to the direct
Barracuda model predictions, the idea of using a slip factor applied to actual plant reactor
pressure measurements in the upper freeboard near the cyclone inlets was explored within the
model. This technique may provide a simplified way to more directly estimate entrainment rates
in industrial reactors.
REACTOR SYSTEM
The two reactors studied were Sohio-type Acrylonitrile reactors, as illustrated in Figure 1. These
reactors are described by Kunii and Levenspiel (1) as having a uniform air feed through a bottom
distributor and an upper distributor where ammonia and propylene are fed. The Sohio reactors
have numerous vertical coolant coils that circulate water and produce steam from the highly
exothermic reaction. Internal cyclones collect the catalyst from the effluent gas and return it to
the bottom of the reactor.
Product Gas
Table 1. Operating and Model Conditions
Catalyst dp 50, 50-65

microns
Fines Content, < 44 10-35
microns
Particle Density, 1400-2000
Coolant Water Steam
kg/m3
Reactor Diameter, m 3.6 (small),
9 (large)
Operating Pressure, 100-200
kPa
NH3, C3H6
Operating 425-490
Temperature, °C
Distributor
Distributor
Air
Figure 1. Sohio-type Acrylonitrile Reactor,

Modified from Kunii and Levenspiel (1)
Pressure profiles were taken with local digital pressure gauges. Due to the limited nozzle
locations on the reactor vessels, the pressure profile was limited to approximately ten locations
along the reactor height. The pressures were taken at points approximately 1 foot from the wall
of the reactor vessels using internal piping.
NUMERICAL MODEL (CPFD)
The three-dimensional gas-solids flow inside the two Acrylonitrile reactors operating in the
turbulent fluidization mode was numerically simulated using the commercial Barracuda software
package. The Barracuda software is an advanced math-physics based numerical tool built on the
technology of the computational particle-fluid dynamics (CPFD) developed by CPFD Software.
The software's numerical methodology uses a direct element method where solids are modeled
using the Lagrangian method as discrete particles with proper size and density distributions, and
the fluid is modeled as a continuum solved on a fixed grid using the Eulerian method. The actual
solids particles numbering in the order of 1015 to 1018 are typically modeled with 1 to 5 million
numerical particles, each of which groups the physical particles with the same properties (size,
density, etc) as a single entity. Each of the numerical particles is explicitly tracked and calculated
for its position and motion in the Lagrangian scheme. Solutions of the fluid dynamics and solids
motion and their interaction are fully coupled. The software has been extensively validated
against available theoretical and experimental data, and it is efficient in simulating large
commercial scale fluidization units.
The reactor simulations included all major internals including cyclones, diplegs, cooling coils and
support beams and gas spargers in the numerical model. Figure 2(a) shows the larger reactor
loaded with solids particles. The reactor model was discretized with approximately 200,000 cells.
A quarter of the gridded model cutting through the center lines is shown in Figure 2(b). The
geometry of the smaller reactor was similar with fewer cyclones and coils.
The simulation conditions are typical operation conditions of Acrylonitrile reactors. Since
fluidization behavior of the bed was the focus of the study, chemical reactions and thermal
dynamics and heat transfer were not considered. The fluid, a gas mixture of air and
hydrocarbons, had a superficial gas velocity of approximately 0.6 m/s. The reactor was initially
loaded with solids particles at near close-pack volume fraction. The flow boundary conditions
included fluidizing gas entering the bed uniformly through the bottom of the reactor and through
the gas sparger at a higher elevation inside the reactor, pressure boundary conditions at the
cyclone inlets where gas and solids flow exit the system, and solids returned to the bed through
the bottom of the primary and secondary diplegs. The rate of solids returned to the bed from the
diplegs matched approximately the rate of solids entrainment through the cyclones so the bed
inventory was maintained almost constant during the simulation. The variation of bed inventory is
within 1~2%. A typical simulation was approximately 200 s of real-time operation; about 100s to
reach quasi-steady state and an additional 100 s is run to obtain average properties such as the
particle volume fraction, the pressure and gas and solids velocities.
Two simulations were performed on different reactor sizes both with a superficial gas velocity of
about 0.6 m/s.
(a) (b)
Figure 2. One of the Two Acrylonitrile Reactors Simulated. (a) The Whole Reactor with Solids
Particles Being Fluidized at the Early Stage of the Simulation. (b) Gridded Model.
Pressure vs. Elevation
Pressure vs. elevation as well as density vs. elevation were measured in the plant and computed
by the Barracuda model and were compared in Figures 3-4. The key parameters of the
Barracuda models and the plant reactor were chosen to be as close as possible for a good
comparison. They are shown on a relative basis to the maximum elevation and pressure. In
addition, calculated points corresponding to the relative top pressure accounting only for the
weight of the bed as well as the relative top pressure using the bed weight and correcting for an
average 6% reduction in cross-sectional area due to the reactor internals are shown for
comparison..
From Figures 3, the Barracuda pressure vs. height shows a more gradual decrease in pressure
than the plant data. The model shows reasonably good agreement with the pressure survey data
over the entire reactor height. A force balance check showed that the pressure drop calculated
by the Barracuda model matched the bed weight within 5%.
Figure 4 shows the pressure profile of the 3.6-meter diameter reactor compared to the pressure
profiled predicted by the Barracuda model. In this case, the pressure profile matched the shape
of the plant data closely up to about 40% of the reactor bed height. The top point of the plant
reactor survey shows about 2% difference from the Barracuda model. While the overall inventory
in the model matched the plant within 5%, the pressure deviation may be due to de-fluidized
catalyst in the plant reactor and catalyst below the bottom pressure tap that is not contributing to
the overall pressure drop.
1.00
0.90
ΔP used for entrainment rate
estimate
0.80
0.70
Relative Height, h/H
Barracuda Average
0.60 Plant Reactor Static Data
Top Pressure Using Bed Weight Only
Top Pressure Using Bed Weight and 6% Area Reduction for Internals
0.50
0.40
0.30
0.20
0.10
0.00
0.90 0.91 0.92 0.93 0.94 0.95 0.96 0.97 0.98 0.99 1.00
Absolute Pressure Relative to Maximum Pressure
Figure 3. Pressure Profile Comparison in the 9-m Diameter Reactor

1.00
0.90 ΔP used for entrainment rate

estimate
0.80
0.70
Relative Height, h/H
0.60 Barracuda Average

Plant Reactor Static Data
Top Pressure Using Bed Weight Only
0.50 Top Pressure Using Bed Weight and 6% Area Reduction for Internals
0.40
0.30
0.20
0.10
0.00
0.93 0.94 0.95 0.96 0.97 0.98 0.99 1.00
Absolute Pressure Relative to Maximum Pressure
Figure 4. Pressure Profile Comparison in the 3.6-m Diameter Reactor
Entrainment Rate Comparisons

One of the key parameters desired from the pressure survey and the Barracuda models was an
estimate of the entrainment rate of solids to the cyclones. While the upper limit of the
entrainment can be calculated from the upper-most bed density, the actual entrainment to the
cyclones would be lower. A question posed during this study was if a slip factor could be applied
to the upper-most bed density to better estimate the entrainment rate and cyclone loading. The
slip factor, as defined by Patience, et.al. (2), is the ratio of the gas velocity to the particle velocity.
In parallel, the Barracuda model offered a way to not only apply this concept within the model, but
to also directly compare to the actual entrainment with the model itself.
ψ = Uo/(εavgVp) (1)
The average particle velocity is calculated from Eq. (2) and the voidage from Eq. (3) assuming
pressure drop is only due to the hydrostatic head of the solids:
Vp = Gs/[ρp(1- εavg)] (2)
εavg = 1- dP/(ρpgdz) (3)
The slip factor defined by Eq. (1) was directly calculated from the Barracuda simulation. Figure 5
shows the slip factor for both reactor diameters at various elevations over the equivalent range
between the top two pressure taps in the plant reactors. The slip factor was 1.47 to 2.97 over this
elevation range. The 9-m reactor average slip factor was higher than the 3.6-m reactor which
was also reflected in the higher predicted entrainment rate shown in Table 3. The arithmetic
average slip factor around 2 indicated that on average the particle velocity was less than half of
the fluid velocity (note that the average void fraction was around 0.97). Due to the difference in
the particle and fluid velocities, the actual entrainment rate was much less than that calculated
under the assumption that the particle and fluid flow to the cyclone together at the same velocity.
The Barracuda simulation predictions match well with data from Patience, et. al. where the slip
factor in the fully developed region of CFB risers from various data sources was calculated as
approaching 2. The entrainment flux (Gs) from the acrylonitrile reactors was calculated from
Equations 1 to 3 using the average Barracuda model calculated slip factor applied to the top most
differential pressure measurement under the operating conditions present.
1.00
0.95
9-m Average Slip Factor = 2.44

3.6-m Average Slip Factor = 1.83
0.90
Relative Height (h/H)
0.85 3.6-m Diameter Barracuda Model

9-m Diameter Barracuda Model
0.80
0.75
0.70
0 0.5 1 1.5 2 2.5 3 3.5
Calculated Slip Factor (Model)
Figure 5. Slip factor calculated by Barracuda at elevations between the top two plant reactor
pressure taps
The Barracuda model results and the method described above applied to the plant reactor data
are compared to several other literature entrainment rate correlations in Table 3. A 5% higher
superficial gas velocity was used in the entrainment rate correlations due to the internal blockage
inside the reactor around the transport disengagement height (TDH). Evaluating the Barracuda
model results in the same manner as the plant data, the average slip factor shown in Figure 5 for
each reactor diameter was applied to the pressure drop over height (DP/L) data from the plant to
estimate the actual entrainment rate. By using this method, the Barracuda model results include
both the actual solids slip and any solids moving down the reactor walls, diplegs, or other
structures. Therefore, the Barracuda predicted slip may be reasonably applied to the plant
reactor data. Using this same slip factor on the plant DP/L data, the 9-m diameter reactor
entrainment at a superficial gas velocity of 0.6 m/s is about 50% of the Barracuda model
prediction. The 3.6-m diameter reactor entrainment rate predicted using this method was about
65% of the Barracuda model prediction. A separate independent method of measuring cyclone
loading in the plant reactor was reasonably close to these entrainment rate predictions. Ideally,
the top two pressure taps would be closer together and closer to the cyclone inlet.
Overall the Barracuda model was as good as or better than most literature correlations. Reasons
for the deviation could include the lack of inter-particle forces (clustering) in the Barracuda model
vs. the expectation that these are present in the plant reactors, or drag model and bed-expansion
differences. Schildermans and Baeyens (3) attempted to correlate entrainment rates Sohio-type
Acrylonitrile reactors using a combination of entrainment rate correlations. Using a 3.5-m
diameter reactor, they calculated entrainment fluxes of 0.23-0.91 kg/s m2, which are much lower
than those calculated in this study. Possible reasons for the higher estimated fluxes from the
plant reactor data compared to Schildermans and Bayeyens or FCC systems include less
clumping due to different catalyst systems, higher fines content, and that the real slip factors
could be higher than predicted by Barracuda.
Table 3. Entrainment Flux Comparison to Selected Correlations at Uo = 0.6 m/s

kg /s m2
3.6-m plant reactor pressure data with 1.83 slip factor applied 11.9
3.6-m Barracuda Model Actual Entrainment 18.6
9-m plant reactor pressure data with 2.44 slip factor applied 7.81
9-m Barracuda Model Actual Entrainment 15.5
PSRI Correlation (4) 2.9
Tasirin and Geldart (4) 1.8
Zenz, et al. Procedure (5) 22.5
Kato, et al. (6) 7.3
Wen and Hashinger (7) 0.4
Geldart et al. (8) 5.9
Merrick and Highley (9) 35.0
Zenz and Weil (10) 1.7
Sciazko (11) 5.6
Interestingly, Abrahamsen and Geldart (12) showed no impact of bed diameter on entrainment
rate, and Wen and Chen (13) indicate directionally that the elutriation rate is expected to be
higher for larger diameter vessels. Their work contrasts with this study in which both the plant
and Barracuda models show decreasing entrainment flux with increasing column diameter. In the
case of the plant reactor data, the smaller diameter plant reactor had a higher fines content which
may have dominated this difference.
CONCLUSIONS
Barracuda CPFD models showed reasonable fit of pressure vs. height compared to Sohio-type
Acrylonitrile reactors of 3.6- and 9-m diameter. Slip factors were calculated over the range of the
top two pressure taps of the plant reactors and were used to estimate entrainment rates within
10-50% of the Barracuda model predicted entrainment rates. The Barracuda model slip factor
approached 1.55 for the 3.6-m diameter reactor and 1.95 for the 9-m diameter reactor. The
Barracuda model fit the 3.6-m diameter reactor data better than the 9-m diameter data. Overall,
using the calculated slip factor from the Barracuda models applied to the density above TDH or
the Barracuda model directly to estimate entrainment rates from large diameter industrial reactors
appears to be a reasonable approach.
ACKNOWLEDGEMENTS
The authors would like to acknowledge the contributions of the plant personnel at Ascend
Performance Materials, LLC including Bart Propst, Stephen Pope, Brian Manis, and Dean Murphy
for collecting the data and helping with the analysis. In addition, we would like to acknowledge
Ted Knowlton from PSRI and Todd Pugsley from University of Saskatchewan for their input on
entrainment rate considerations as well as comments from Mayank Kashyap of Ascend
Performance Materials.
NOTATION
dp 50 = Mass Mean Particle Diameter

H = Total Reactor Height
h = Local Reactor Height
ψ = Slip Factor
Uo = Superficial Gas Velocity
εavg = Average Void Fraction
Vp = Particle Velocity
Gs = Solids Flux (mass/area-time)
ρp = Particle Density
g = Gravitational Constant
P = Pressure
z = Vertical Coordinate
dP/dz = Pressure Gradient
REFERENCES
1. Kunii, D., and O. Levenspiel, Fluidization Engineering, 2nd Ed., Butterworth-Heinmann,

Boston,1991, pp. 31-32.
2. Patience, G.S., J. Chaouki, F. Berruti, and R. Wong, Powder Technology, 72 (1992) 31-37.
3. Schildermans, I., and J. Baeyens, The Carry-over of Catalyst from Large Fluidized Bed Gas-
catalytic Reactors, Powder Handling and Processing, Vol. 14, No. 4, (2002) 246-251.
4. PSRI Fluidization Seminar, February 20-23, 2006, Sugarland, TX.
5. Tasirin, S.M., and D. Geldart, Powder Technology, 95 (1998) 240-247.
6. Kato, K., T. Tajima, M. Mao, and H. Iwamoto, In: Kwauk M, Kunii D, Zheng J, Hasatani M, eds.
Fluidization ’85 – Science and Technology, Elsevier, Amsterdam, 1985, pp. 134-147.
7. Wen, C.Y., and R.F. Hashinger, AIChE J., 6 (1960) 220-226.
8. Geldart, D., J. Cullinan, S. Gilvray, and D.J. Pope, Trans. Inst. Chem. Eng., 57 (1979) 269-275.
9. Merrick, D. and J. Highley, AIChE Symposium Ser., 70 (1974), 366-378.
10. Zenz, F.A. and N.A. Weil, AIChE J, 4, (1958) 472.
11. M. Sciazko, Powder Technol., 66 (1991) 33-39.
12. Abrahamsen, A.R., and D. Geldart, Powder Technology, 26 (1980) 47-55.
13. Wen, C. Y., and L.H. Chen, AIChE Journal, 28 (1982) 117-128.
EFFECT OF WALL BOUNDARY CONDITIONS AND MESH
REFINEMENT ON NUMERICAL SIMULATION OF
PRESSURIZED DENSE FLUIDIZED BED FOR
POLYMERIZATION REACTOR
P. Fede1,2, O. Simonin1,2, R. Ansart1,2, H. Neau1,2 and I. Ghouila3
1
Université de Toulouse; INPT, UPS ; IMFT ; 31400 Toulouse, France
e-mail : fede@imft.fr
2
CNRS; Institut de Mécanique des Fluides de Toulouse ; 31400 Toulouse, France
3
INEOS; Innovene; CTL/PRO Ecopolis Lavéra, 13117, Lavéra, France
ABSTRACT
The effect of the mesh refinement and the solid phase boundary condition are
investigated for numerical simulation of dense pressurized fluidized bed. Two
fluidized beds have been considered: a laboratory-scale device and a pilot-scale
facility. A relation is proposed to scale-up the numerical simulation and preserving
the spatial resolution accuracy. As expected the boundary condition of the solid
phase modifies the behaviour of the fluidized bed. Compared to free-slip wall
boundary condition, a no-slip condition improves the numerical predictions with
respect to available experimental data.
INTRODUCTION
Pressurized gas-solid fluidized beds are used in a wide range of industrial
applications such as coal combustion, catalytic polymerization, uranium fluoration or
biomass pyrolysis. The numerical modelling of such industrial fluidized beds is
challenging because many complex phenomena take place (particle-turbulence
interaction, particle-particle and particle-wall collision, heat and mass transfers) and
the large-scale geometry of the industrial facilities. The development of numerical
modelling of fluidized bed hydrodynamic started about two decades ago. Nowadays
it is possible to perform 3D realistic simulations of industrial configurations by using
unsteady Eulerian reactive multi-fluid approach. Numerical simulations of industrial
and pilot-reactor were carried out with such an approach showing a good agreement
with the qualitative knowledge of the process (bed height, pressure drop, local mass
flux). However the size of industrial reactor and the computer resources imposed too
coarse meshes. Recent studies have emphasized the role of the spatial resolution
on the prediction of the fluidized bed behaviour (Agrawal et al (1); Igci et al (2);
Parmentier et al (3-4)). Also it has been shown that for dilute (Benyahia et al (5))
and dense (Fede et al (6)) gas-solid flow the boundary condition of the solid phase
may modify the structure of the flow. According to Fede et al (6), in dense fluidized
bed, the no-slip wall boundary improves the prediction of the radial profile of mean
vertical particle velocity compared to the results predicted by using a free-slip wall
boundary condition.
In the present study, 3D numerical simulations of dense pressurized fluidized beds

have been carried out using an Eulerian n-fluid modelling approach for fluid-particle
turbulent polydispersed flows developed and implemented by IMFT (Institut de
Mécanique des Fluides de Toulouse) in the NEPTUNE CFD V1.07@Tlse version.
Table. 1. Mesh characteristics for laboratory- and pilot-scale reactors.
NEPTUNE CFD is a multiphase flow software developed in the framework of the

NEPTUNE project, financially supported by CEA (Commissariat à l’Energie
Atomique), EDF (Electricité de France), IRSN (Institut de Radioprotection et de
Sûreté Nucléaire) and AREVA-NP.
The multiphase Eulerian approach is derived from a joint fluid-particle PDF equation
allowing to derive the transport equations for the particle velocity’s moment (Simonin
(7)). In the proposed modelling approach, separate mean transport equations
(mass, momentum, and fluctuating kinetic energy) are solved for each phase and
coupled through inter-phase transfer terms. The drag law is modified according to
Gobin et al (8). The collisional particle stress tensor is derived in the frame of the
kinetic theory of granular media (Boëlle et al (9)). The turbulence modelling is
achieved by the standard k−ε model extended to the multiphase flows (i.e.
accounting for additional source terms due to the inter-phase interactions). For the
dispersed phase, a coupled transport equation system is solved on particle
fluctuating kinetic energy and fluid-particle fluctuating velocity covariance (Simonin
(7)).
In the present paper, we analyze the effect of the solid wall boundary conditions and
mesh size for several fluidized bed systems: first a laboratory-scale bed (0.9m of
height) and a pilot-scale bed (9m of height). The numerical simulation of an
industrial-scale bed (34m of height) is discussed and the results will be shown at the
conference.
GEOMETRY, MESH AND SCALING

The numerical simulations were carried out for several isothermal reactors: first a
laboratory-scale reactor with a diameter of 0.077m and an height of 1.7m, second a
pilot-scale device with a diameter of 0.74m and a height about 9 meters. For the
comparison, simulations were carried out for an industrial-scale polymer reactor has
a diameter of 5m and a height of 34m.
In the last few years, the sensitivity of the numerical simulation with respect to the
mesh has been investigated. Agrawal et al (1) showed that a very fine mesh
(typically with a cell size of the order of a few particle diameters) permits to capture
some meso-scale structures. These structures have a strong influence on the
hydrodynamic of the fluidized bed especially on the bed height, on the vertical solid
mass flux and the mixing process. Recent studies (Heynderickx et al (10); Igci et al
(2)) pointed out the role of the drag force in the formation of the meso-scales. These
studies were made by a priori analysis of mesh-independent numerical simulation.
Fig. 1. Sketches of the reactor. From the left to the right: the laboratory-scale
reactor, the pilot-scale reactor and the large industrial facilities.
Parmentier et al (3) have shown that the error related to the mesh can be scaled.
Indeed, for similar operating conditions and particle properties, considering a
numerical simulation of a dense fluidized bed of diameter Dr with a cell size of ∆, the
~
required mesh for a larger reactor of diameter Dr and conserving the error due to
the mesh is given by:
~ ~
∆ = ∆ Dr / Dr (1)
The meshes have been constructed using O-grid technique in order to have nearly
uniform cells in a horizontal section ( dx ≈ dy ). The Table 1, giving the main
characteristics of the meshes for the laboratory- and pilot-scale reactors, shows that
the cell size dx is nearly in accordance with Equation (1) when passing from the
laboratory-scale to the pilot-scale reactors.
The numerical simulations are performed in two steps. First the column of the
fluidized bed is filled of solid. The solid volume fraction is uniformly distributed and
determined in order to fit the solid mass of the experiment. Then a transitory phase,
corresponding to the destabilization of the bed, is computed during 20 seconds (the
2 2
1.5 1.5
1 1
0.5 0.5
Wp / Vf
Wp / Vf
0 0
-0.5 -0.5
Experimental data Experimental data
WBC: no-slip ; standard mesh WBC: no-slip ; standard mesh
-1 WBC: free-slip ; standard mesh -1 WBC: free-slip ; standard mesh
WBC: no-slip ; refined mesh WBC: no-slip ; refined mesh
WBC: free-slip ; refined mesh WBC: free-slip ; refined mesh
-1.5 -1.5
0 0.2 0.4 0.6 0.8 1 0 0.2 0.4 0.6 0.8 1
r / Rp r / Rp
Fig. 2. Laboratory-scale: radial profile of the mean vertical particle velocity

normalized by the fluidization velocity (Vf). The operating pressure is P=12bar and
the fluidization velocity Vf=0.32m/s. On the left-panel the data has been extracted
at z=0.75×Dr and the right panel z=1.7×Dr.
time step is approximately 10-3s). In a second step, the time-averaged statistics are
computed during 80s in order to obtain converged statistics.
LABORATORY-SCALE DEVICE
The experimental investigation of dense fluidized bed is a trickiest challenge.
Because of the medium opacity, the experimental data are commonly reduced to
pressure drop at the wall or local solid mass flux. However, recently a novel
technique has been developed called Positron Emission Particle Tracking allowing
to access to the local properties of the solid flow. This non-invasive technique
consists of tracking a single particle (up to now it is possible to have multiple particle
tracking) and using specific algorithm to reconstruct the Lagrangian trajectory of the
particle inside the fluidized bed. This technique has been successfully employed to
investigate the hydrodynamic of dense fluidized bed (Link et al (11); Fede et al (6)).
The drawback of the PEPT method is that the entire reactor has to be equipped of
sensor. Then, the using of PEPT to investigate an industrial reactor is still quite
complicated. However the PEPT can be used on a laboratory-scale fluidized bed.
Such experimental works are crucial to improve the knowledge on the local
mechanisms taking place in a fluidized bed. This is also relevant to assess a
modelling approach and closure laws used in Euler-Euler models.
Fede et al (6) made an analysis of experimental data obtained by PEPT. On the

radial profiles of the time-averaged mean vertical particle velocity they observed that
in the near-wall region the solid velocity is nearly equal to zero. It suggests that a
no-slip wall boundary condition for the solid phase is more suitable than a free-slip
condition. However, a no-slip boundary condition for the mean particle velocity and
zero flux for the particle fluctuating kinetic energy are very questionable but could
represent elastic bouncing on the wall with an isotropic angle distribution. Such a
situation could correspond to spherical particles bouncing on very rough wall or to
Fig. 3. Pilot-scale: streamtraces of the time-averaged simulated particle velocity.
Left panel: free-slip wall boundary condition for solid phase, right-panel: no-slip
boundary condition. The operating pressure is P=12 bar and the fluidization
velocity Vf=0.32m/s.
very irregular particles bouncing on a smooth wall (Konan et al (12)). However the
experimental observations have shown a downward solid flux at the wall. Then one
may emphasize that wall boundary condition for the mean solid velocity is between
the free-slip and the no-slip condition.
The Figure 2 shows the radial profile of the time-averaged mean vertical particle
velocity using the two meshes and both boundary condition. The operating pressure
is 12bar and the fluidization velocity 32cm/s and the particles are Geldart’s B type.
As shown by Figure 3 such a dense pressurized fluidized bed exhibits a peculiar
hydrodynamic with a 3-dimensional recirculating loop. The figure shows that the
modification of the wall boundary condition for the mean particle velocity changes
the topology of the flow. The free-slip condition leads to a one-loop system whereas
a no-slip boundary condition to a two counter-rotating recirculating loop. The
recirculating loop is clearly shown by the radial profiles in Figure 2. Indeed, we
observe an upward mean vertical particle velocity at the bed centre (r = 0) and in the
near-wall region a downward particle velocity. We observe that the mesh refinement
does not have a significant effect on the time-averaged mean particle vertical
velocity. In contrast, the Figure 3 shows that the no-slip wall boundary condition
gives the same trend than the experimental data. In particular, the slope break
appearing close to wall is well predicted even if the position of the slope break is not
correct. Similar trends have been observed with the same particles but differing in
terms of fluidization velocity and operating gas density.
Fig. 4. Pilot-scale: radial profile of the time-averaged mean vertical gas (left) and
solid (right) velocity normalized by the fluidization velocity. The radial profile is
extracted at z=3.2×Dr.
PILOT-SCALE FACILITY
The pilot-scale reactor investigation is particularly important because the operating
conditions are very close to the ones in industrial process. In addition, the flow
simulation conditions of such a device are well controlled (in terms of temperature,
velocity of fluidisation, particle properties) and experimental data are available
(pressure drops, temperature, gas composition).
Fede et al (13) performed numerical simulations of such a polymerization pilot

reactor located at INEOS Lavéra (France). As for the laboratory-scale they found a
large recirculating loop. The Figure 4 shows the radial profile of the time-averaged
mean vertical gas and solid velocity in the pilot-scale fluidized bed. We observe that
the structure of the flow is similar to the one observed in the laboratory-scale
reactor. Namely, we notice a large upward particle velocity at the reactor centre (up
to 4 times the fluidisation velocity) and a downward particle velocity near the wall.
This typical profile indicates the presence of the recirculating loop. The figure 4
shows that the profile of the gas velocity profile has the same shape than the profile
of the particle velocity. In such a fluidized bed, the near-wall region is characterized
by large downward solid mass flux. Then, the particles drag the gas in their motion
leading to negative vertical gas velocity. The modification of the wall-boundary
condition for the solid phase clearly modifies this effect. Indeed, Figure 4 exhibits a
strong reduction of the downward particle velocity at the wall and consequently a
reduction of the downward gas velocity. The mass conservation leads to decrease
the particle velocity at the reactor centre.
The vertical mean pressure distribution is shown by Figure 5. The pressure

distribution exhibits a slope break corresponding to the top of the fluidized bed. With
the free-slip wall boundary condition the pressure distribution inside the fluidized bed
is found slightly bended whereas a no-slip condition gives linear profiles. This effect
may be explained by the recirculating loop identified in such a fluidized bed. Indeed,
the free-slip boundary condition should lead to a too large rotating motion of the
Fig. 5. Vertical mean gas pressure distribution measured at the wall in pilot-scale
reactor.
recirculating loop. Then, the gas and the particles are accelerated at the centre of
the bed modifying the pressure distribution. The mesh refinement does not
significantly modify the pressure distribution even if the top of the fluidized bed is
slightly decreased with the mesh refinement. It was expected because the particles
correspond to Geldart’s B particle type. For such kind of particles the sensitivity of
the numerical solution with the mesh is less important than for Geldart’s A particles.
INDUSTRIAL-SCALE FACILITY
In the two previous sections, we have briefly described the hydrodynamic of
isothermal laboratory-scale and pilot-scale device. For the considered operating
points and powder properties, Equation (1) gives the required mesh size to ensure a
good spatial resolution. If we apply such a scaling-rule, the mesh for the industrial-
scale configuration requires about 4,000,000 cells. Nowadays such a numerical
simulation is realizable using High Parallel Computing. In particular the parallel
efficiency of NEPTUNE CFD has been demonstrated up to 1,024 CPU (Neau et al
(14)). Such an industrial-scale numerical simulation is currently running and the
results will be presented.
CONCLUSION
Numerical simulations of pressurized dense fluidized bed for polymerization have
been carried out and compared with experimental data for laboratory-scale and pilot
scale. The effect of boundary conditions on the solid phase has been investigated
and the results show that the prediction of the gas pressure vertical distribution is
improved with a no-slip boundary condition for the mean solid velocity.
ACKNOWLEDGMENT
This work was granted access to the HPC resources of CINES under the allocation
2010-026012 made by GENCI (Grand Equipement National de Calcul Intensif) and
by CALMIP under the project P0111.
NOTATION
Dr diameter of the reactor Wg mean vertical gas velocity
Hr height of the reactor Wp mean vertical solid velocity
Vf operating fluidization velocity P gas pressure
REFERENCES
(1) Agrawal, K., Loezos, P., Syamlal, M., and Sundaresan, S. (2001). “The role of
mesoscale structures in rapid gas-solid flows”, J. Fluid Mech., 445, 151–185.
(2) Igci, Y., Andrews IV, A. T., Sundaresan, S., Pannala, S., and O’Brien, T. (2008).
“Filtered two-fluid models for fluidized gas-particle suspensions”, AIChE Journal, 54,
1431–1448.
(3) Parmentier, J.-F., Simonin, O., and Delsart, O. (2008). “A numerical study of
fluidization behavior of Geldart B, A/B and A particles using an Eulerian multifluid
modeling approach”, Proc. of the 9th Int. Conference on Circulating Fluidized Beds,
Circulating Fluidized Bed Technology IX. 331–336.
(4) Parmentier, J.-F., Simonin, O., and Delsart, O. “A functional subgrid drift velocity
model for filtered drag prediction in dense fluidized bed”, Submitted to AIChE
Journal.
(5) Benyahia, S., Syamlal, M., and O’Brien, T. J. (2005). “Evaluation of boundary
conditions used to model dilute, turbulent gas/solids flows in a pipe”, Powder
Technology, 156, 62 – 72.
(6) Fede, P., Moula, G., Ingram, A., Dumas, T., and Simonin, O. (2009). “3D
numerical simulation and PEPT experimental investigation of pressurized gas-solid
fluidized bed hydrodynamic”, Proceedings of ASME 2009 Fluids Engineering
Division Summer Meeting, ASME.
(7) Simonin, O. (1996). “Combustion and turbulence in two-phase flows”. Lecture
Series 1996-02, Von Karman Institute for Fluid Dynamics.
(8) Gobin, A., Neau, H., Simonin, O., Llinas, J. R., Reiling, V., and Sélo, J. L. (2003).
“Fluid dynamic numerical simulation of a gas phase polymerisation reactor”,
International Journal for Numerical Methods in Fluids, 43, 1199–1220.
(9) Boëlle, A., Balzer, G., and Simonin, O. (1995). “Second-order prediction of the
particlephase stress tensor of inelastic spheres in simple shear dense suspensions”,
in Gas-Particle Flows, Vol. 228, ASME FED. 9 – 18.
(10) Heynderickx, G. J., Das, A. K., Wilde, J. D., and Marin, G. B. (2004). “Effect of
clustering on gas-solid drag in dilute two-phase flow”, Ind. Eng. Chem. Res., 43,
4635–4646.
(11) Link, J. M., Deen, N. G., Kuipers, J. A. M., Fan, X., Ingram, A., Parker, D. J.,
Wood, J., and Seville, J. P. K. (2008). “PEPT and discrete particle simulation study
of spout-fluid bed regimes”, AIChE Journal, 54(5), 1189–1202.
(12) Konan, N., Kannengieser, O., and Simonin, O. (2009). “Stochastic modeling of
the multiple rebound effects for particle-rough wall collisions”, International Journal
of Multiphase Flow, 35(10), 933 – 945.
(13) Fede, P., Neau, H., Simonin, O., and Ghouila, I. (2010). “3D unsteady
numerical simulation of the hydrodynamic of a gas phase polymerization pilot
reactor”, 7th International Conference on Multiphase Flow, ICMF 2010, Tampa, FL.
(14)Neau, H., Laviéville, J., and Simonin, O. (2010). “Neptune CFD high parallel
computing performances for particle-laden reactive flows”, 7th International
Conference on Multiphase Flow, ICMF 2010, Tampa, FL, May 30 - June 4.
ELUTRIATION FROM FLUIDIZED BEDS: COMPARISON BETWEEN
EXPERIMENTAL MEASUREMENTS AND 3D SIMULATION RESULTS
Renaud Ansart1 2 , Hervé Neau 1 2 , Philippe Accart3 4

Alain de Ryck3 4 and Olivier Simonin1 2
1 Université de Toulouse; INPT, UPS; IMFT ; F-31400 Toulouse, France
2 CNRS; Institut de Mécanique des Fluides de Toulouse; F-31400 Toulouse, France
3 Université de Toulouse; Mines Albi; RAPSODEE; F-81013 Albi, France
4 CNRS, Centre RAPSODEE, Campus Jarlard, F-81013 Albi, France
ansart@imft.fr, simonin@imft.fr
ABSTRACT
This paper presents comparisons between experimental measurements and unsteady three-
dimensional numerical simulations performed by an unstructured parallelized CFD multiphase
flow code of elutriation and transport of mono-dispersed glass beads type B and A/B in a
fluidized bed. These comparisons show a satisfactory agreement between experimental mea-
surements and numerical predictions. The numerical results also show a strong dependence
on the mesh size, especially for fine particles. A model accounting for influences of meso-
scales structures on overall bed hydrodynamics, which are not resolved by coarse mesh simu-
lations, is applied. Results obtained with the model show improvements for the dense fluidized
bed and even for a transport step.
INTRODUCTION
Gas-solid fluidized beds are used in a wide range of industrial applications such as
coal combustion, catalytic polymerization and uranium fluoridation. Many of the flu-
idized bed industrial processes involve poly-dispersed powder and even multi-species
of powders. In bubbling fluidized bed combustion and catalytic cracking, elutriation is a
major cause of inefficiency, while it could be highly desirable in specific case. Whether
the intention is to minimize or to promote elutriation, the involved phenomena must be
properly known if the process has to be efficiently controlled.
Numerical simulation is becoming an efficient approach to study the separation and
entrainment processes observed in an industrial fluidized bed. In the literature, there
is a lack of experimental data to validate CFD simulations of these phenomena. Thus,
a joint experimental and numerical project between RAPSODEE Centre and IMFT
was initiated. The object of this paper is to present comparisons between three-
dimensional numerical simulation predictions and experimental data of particle gas
pressure drop and entrainment in a fluidized bed.
Particle properties Fine Coarse
Solid mass (kg) 2.5 2.5
Density (kg/m3 ) 2470 2470
Diameter d50 (µm) 84 213
Span= d90d−d
50
10
0.38 0.414
−1
Vt (m · s ) 0.41 1.51
Umf (m · s−1 ) 5 · 10−3 36 · 10−3
Fig. 1: Experimental set up. Table. 1: Powder properties.
EXPERIMENTAL SET UP
The column in the laboratory experimental set up was 10 cm in diameter and 59 cm
high (Fig. 1) and was fitted with a conical outlet. The column material was stainless
steel to avoid electrostatic charge (Ansart et al. (1)). The bronze distributor had a
pressure drop of 6 kPa at a superficial gas velocity of 0.18 m · s−1 . Fluidizing air was
supplied by a Brooks smart mass flow meter and controllers 5853S with an accuracy
of ±0.7 % of the rate and ±0.2 % of full scale (2.32 m · s−1 ).
The process was divided into two parts: the first allowed the fluidization of particles
by a homogeneous superficial gas velocity (Vf 1 < Vt ), in order to obtain a bubbling
fluidized bed regime. According to a linear ramp-up of 5 s during the second part, the
fluidization velocity was increased to entrain the particles (Vf 2 > Vt ). The particles
entrained were collected through a vessel at the outlet of a cyclone. The mass of
particles collected was continuously weighed during the process with a resolution time
of 1 s and an accuracy of 0.01 g. Pressure variations along the pipe were monitored
by severals sensors located every 1.5 cm. Honeywell DC pressure instrumentation
was used with an accuracy of ±0.25 % of full scale. The resolution time was 0.1 s.
The measurement of gas pressure on the wall was made through an 8 mm diameter
opening with a filter.
The powder was glass beads with properties described in Table 1. For 2.5 kg of solid
mass, the bed at rest in the column is approximatively 21 cm. Two particle sizes called
fine (Geldart type A/B) and coarse (Geldart type B) were used. The mean diameters
of powder were determined using a Mastersizer 2000 with 1.5 bar of dispersion. The
bulk material was sieved to ensure an almost mono-dispersed distribution. The ter-
minal settling velocity Vt of the particle was calculated by the expression of the drag
coefficient, Equation (5). According to Remf , an estimation of minimum fluidization
velocity Umf was computed using the expression recommended by Wen and Yu:
ρg (ρp − ρg )d3p g 0.5 Remf µg

Remf = (33.72 + 0.0408 ) − 33.7 Umf = . (1)
µ2g ρp dp
MATHEMATICAL MODEL
Simulations were carried out using an Eulerian n-fluid modeling approach for poly-
dispersed fluid-particle flows implemented in the NEPTUNE CFD software which was
developed and implemented by IMFT (Institut de Mécanique des Fluides de Toulouse).
This software is a multiphase flow code developed in the framework of the NEP-
TUNE project, financially supported by CEA (Commissariat à l’Énergie Atomique),
EDF (Électricité de France), IRSN (Institut de Radioprotection et de Sûreté Nucéaire)
and AREVA.
In the proposed modeling approach, the mean transport equations (mass, momentum
and fluctuant kinetic energy) are solved for each phase and coupled through inter-
phase transfer terms. These equations are derived by phase ensemble averaging
weighted by the gas density for the continuous phase and by using kinetic theory of
granular flows supplemented by fluid and turbulence effects for the dispersed phase
(Balzer et al. (2), Gobin et al. (3)). In the following development, subscript k = g, refers
to the gas phase and k = p refers to the particle phase. The mass balance equation
is:
∂ ∂
αk ρk + αk ρk Uk,i = 0, (2)
∂t ∂xi
where αk is the k th phase volume fraction, ρk the density and Uk,i the ith component of
the velocity. In equation (2), the right-hand-side is equal to zero without mass transfer.
The mean momentum transport equation for the phase k is written:

∂Uk,i ∂Uk,i ∂Pg ∂
−αk ρk u0k,i u0k,j + Θp,ij ,

αk ρk + Uk,j = −αk + αk ρk gi + Ik,i +
∂t ∂xj ∂xi ∂xj
(3)
where u0k,i is the fluctuating part of the instantaneous velocity of phase k, Pg is the
mean gas pressure, gi the ith component of the gravity acceleration and Ik,i the mean
gas particle interphase momentum transfer without the mean gas pressure contribu-
tion. Finally, Θk,ij is for k = g the molecular viscous tensor and for k = p the collisional
particle stress tensor. Due to the large particle to gas density ratio, only the drag force
was assumed to be acting on the particles. Hence, the mean gas-particle interphase
momentum transfer can be written:
Vr,i 1 3 ρg h|vr |i
Ip,i = −Ig,i = −αp ρp F
with F
= Cd,WY . (4)
τgp τgp 4 ρp dp
with Cd,WY given by Wen & Yu’s correlation:

(
24
−1.7 ρg h|vr |idp
Rep 1 + 0.15Re0.687
p αg Rep < 1000 Rep = αg µg
Cd,W Y = −1.7
(5)
0.44 αg Rep ≥ 1000
The mean relative velocity Vr,i between gas and particle is expressed in terms of the
mean gas velocity, mean particle velocity and drift velocity. In equation (3), the col-
lisional particle stress tensor is derived in the frame of the kinetic theory of granular
media (Boelle et al. (4)).
For the gas turbulence, a standard k − ε model extended to the multiphase flows
accounting for additional source terms due to the interfacial interactions was used.
For the dispersed phase, a coupled transport equation system is solved on particle
fluctuating kinetic energy and fluid-particle fluctuating velocity covariance (qp2 − qf p ).
In this paper, the influence of mesh size on the numerical predictions was studied.
The mesh size required to fully resolve all of the fine-scale structures decreased as
a function of the mean particle relaxation timescale (Parmentier et al. (5)). Because
of limited computational resources, a filtered approach can be used to model the drag
term accurately (Agrawal (6)). In the framework of a filtered approach for gas-solid
flows, Parmentier et al. (7) proposed that the filtered drag can be modeled by:

αp ρp αp ρp
F
Vr,i = F
(δij + h(αp )Kij f (∆∗G )) Ver,j , (6)
τgp τegp
where Ver,j = is the resolved relative velocity. Kij = δij Kh + δi3 δj3 (Kv − Kh ), the model
coefficient is the same in x and y direction (Kh and Kv are determined by a dynamic
√
adjustment performed by a second filter). h(αp ) = − u (1 − u)2 (1 − 1.88 u + 5.16 u2 ),
where u = αp /αm et αm = 0.64 is the maximum compacting. The forms of the h and
f functions are derived from a highly-resolved simulation of mono-dispersed gas-solid
flow. The function f is modeled as the following equation:
∆∗G 2 ∆G
f (∆∗G ) = with ∆∗G = √ . (7)
a2 + ∆∗G 2 τpSt gL
where a = 0.084, ∆∗G is a dimensionless mesh size, ∆G the cube root of the cell
volume, L the bed diameter and τpst stokes relaxation time.
NUMERICAL PARAMETERS
To study the influence of mesh refinement, we used three 3D meshes based on O-
grid technique were used. The reference mesh contained 428 451 hexahedra with
approximately ∆x = ∆y = ∆z = 3.7 mm. The mesh was uniformly refined by a
factor of 1.5 which consisted of 1 477 060 cells. The coarse mesh was made up
of 123 816 cells constructed from the reference mesh by coarsening by a factor of
1.5. The numerical simulations were performed on parallel computers with 8 cores for
the coarse mesh, 64 cores for the reference mesh and 128 cores for the fine mesh,
because of mesh size and physical time needed (Neau et al. (8)).
At the bottom (z = 0), the fluidization grid was an inlet for the gas, with an imposed
superficial velocity corresponding to the fluidization velocity vf , and a wall for the par-
ticles. At the top of the fluidized bed, a free outlet for both the gas and the particles
was defined. The wall-type boundary condition was friction for the gas and a no-slip
for the particle. Fede et al. (9) have shown that the gas pressure drop predictions are
improved with a no-slip boundary condition for the mean particle velocity and zero-flux
condition for the mean particle agitation q2p .

First of all, a comparison between the numerical predictions for the coarse particles
and the experimental results was obtained. Then, the same comparison was carried
30 100
90
25
80
Mass of particles collected (%)

Measurements 70 Exp. data
20
Coarse mesh Coarse Mesh
Height (cm)
60
Reference mesh Reference Mesh
15 50
40
10
30
20
5
10
0 0
0 500 1000 1500 2000 2500 3000 50 100 150 200 250 300
P−PO (Pa) Time (s)
(a) Wall distribution of the mean gas pressure. (b) Mass of particles collected.
Fig. 2: Comparison between experimental data and numerical simulation predictions

for coarse particles. In the left plot the data were obtained during the bubbling step
Vf 1 = 2.5 Umf and in the right plot during the entrainment step Vf 2 = 1.03 Vt .
out for the results of fine particles. In the experiments, the particle phase was slightly
poly-dispersed (span ≈ 0.4). However, the numerical simulations were carried out with
a monodisperse particle distribution having a median diameter equal to d50 .
Coarse particles
Gas pressure drop along the wall during the bubbling phase and the mass of particles
collected obtained by numerical predictions, for the coarse and reference mesh sizes,
were compared with the experimental measurements. To study the wall gas pressure
drop during the bubbling step, the numerical simulations were carried out as follows: at
t = 0 the fluidized bed was filled up with a uniform solid mass fraction according to the
experimental solid mass. A transitory step takes place for t ∈ [0 s, 20 s] corresponding
to the destabilization of the fluidized bed. Then, the statistics were computed for t ∈
[20 s, 60 s] insuring a statistical convergence.
As Fig. 2 shows, the mesh refinement had no effect on the bed expansion or the mass
of particles entrained for the coarse particles (type B). The coarse mesh was sufficient
to predict bed dynamics, and no further mesh refinement was needed. Moreover, a
very good agreement between numerical predictions of the wall gas pressure drop
and the experimental data during the bubbling step (Vf 1 = 2.5 Umf ), Fig. 2(a), was
obtained. Above the bed particles, the gradient of gas pressure was equal is negligible
for the numerical results and for the experimental measurements. Inside the bed, both
distributions were linear. The numerical results predicted the same bed height as the
experimental data.
Fig. 2(b) shows the evolution of the mass of particles collected during the entrainment
step (Vf 2 = 1.03 Vt ). A good agreement between the experimental measurements of
the mass flow rate of coarse particles and the numerical results was obtained. Indeed,
at the start of the entrainment process the flux of particles was slightly overestimated,
and during the following progress of the process the numerical predictions of the flux
were very close to the measurements.
30 30
Measurement data Measurement data
Coarse mesh Coarse mesh + sub grid
25 25
Reference mesh Reference mesh + sub grid
Fine mesh Fine mesh + sub grid
20 20
Height (cm)
Height (cm)
15 15
10 10
5 5
0 0
0 500 1000 1500 2000 2500 3000 0 500 1000 1500 2000 2500 3000
P−PO (Pa) P−PO (Pa)
(a) Effect of mesh size. (b) Effect of sub-grid model for drag force.
Fig. 3: Comparison between experimental data and numerical simulation predictions

of wall mean gas pressure for fine particles during the bubbling step. Vf 1 = 5 Umf .
Fine particles
For fine particles, the numerical simulations were performed on three mesh sizes. Fig.
3(a) shows the wall distribution of time averaged gas pressure, during the bubbling
step (Vf 1 = 5 Umf ), for the experimental measurements and for the numerical pre-
dictions. As shown, mesh refinement had a strong effect on the numerical results for
the fine particles. For the coarse and reference mesh sizes, the bed expansion was
overestimated. Only, the fine mesh case was able to predict a similar wall gas pres-
sure as the experimental measurements, and to correctly estimate the bed height. The
structures of the gas-particle fluidized bed were not able to be resolved by the coarse
and reference mesh simulations and they had a drastic influence on the macroscopic
flow. To account for the effect of unresolved structures on the macroscopic behavior in
the coarse and reference mesh sizes, the sub-grid model described before was used
to model the effective drag term.
The Fig. 3(b) shows that the wall gas pressure drop predictions are greatly improved
by using the sub-grid model. With the sub-grid model, the bed height was almost
independent of the mesh size. A satisfactory agreement was obtained between the
numerical predictions (fine grid and large grid with sub-grid model) and experimental
measurements of the bed height, Table 2. The mean bed height was defined as the
height where the gas pressure distribution slope was modified.
The Fig. 4 shows the mass of fine particles collected during the entrainment step
(Vf 2 = 1.53 Vt ). In the bubbling phase, mesh refinement had a strong effect on the
mass flow rate of particles entrained. Comparisons with the fine mesh simulation
results showed that the coarse and reference mesh simulations overestimated the
mass flow rate of the particles entrained. With the sub-grid model, the numerical
simulations were approaching to the experimental measurements.
100
90
80 Bed height
Mass of particles collected (%)
70
(cm)
60
Coarse mesh 27
50
Reference mesh 26.2
40 Exp mean data Fine mesh 24.1
30
Coarse mesh Coarse mesh + sub-grid 24.5
Reference mesh
20 Fine mesh Reference mesh + sub-grid 24.2
10
Coarse mesh +sub grid
Fine mesh + sub-grid 23.6
Reference mesh +sub grid
0
Exp. data 24.2
50 100 150 200 250 300 350 400 450 500
Time (s)
Table. 2: Time-averaged bed height.
Fig. 4: Mass of fine particles collected dur-
ing the entrainment step. Vf 2 = 1.53 Vt .
The simulation for the reference mesh with sub-grid model appeared to give similar
results as with the simulation of fine mesh but with less expensive computational re-
sources. As for the coarse particles, the flux of particles at the start of the process
was slightly overestimated, and was similar to the experimental measurements for the
following test duration.
CONCLUSION
An experimental test unit was designed and built to study particle separation and en-
trainment in a fluidized bed by measuring the gas pressure along the column and
the mass of particles leaving the column. A three dimensional, unsteady numerical
predictions was carried out with the unstructured parallelized CFD multiphase flow
NEPTUNE CFD were compared with experimental measurements.
Comparisons were obtained for two types of particles (B and A/B). The numerical pre-
dictions for type A/B have strong dependency on the mesh size. To account for the
effect of unresolved structures on the macroscopic behavior for coarse grid simula-
tions, a sub-grid model was used to model the drag term. Accordingly, the numerical
results were greatly improved and were in good agreement with the fine grid simula-
tion. Coarse numerical simulations with the sub-grid model were hugely much less
expensive from the point of view of the computational resources. The numerical pre-
dictions of the bed height and of the entrainment rate were in good agreement with
experimental measurements. The next step of this study is to focus on the elutriation
of a mixture of fine and coarse particles.
ACKNOWLEDGMENTS
This work was granted access to the HPC resources of CINES under the allocation
2010-026012 made by GENCI (Grand Equipement National de Calcul Intensif) and
CALMIP (Centre de Calcul Midi-Pyrénées) under the allocation P0111.
NOTATION
Cd,W Y Wen ’n Yu drag coefficient Vr relative velocity
dp particle diameter Vt terminal settling velocity
g gravitational constant u0k,i fluctuating velocity of phase k
Pg mean gas pressure αk volume fraction of phase k
qp2 mean particle agitation ∆∗G dimensionless mesh size
Rep particle Reynolds number ∆G cube root of the cell volume
Uk,i mean velocity of phase k µg gas viscosity
Umf minimum fluidization velocity ρk density of phase
Vf superficial gas velocity F
τgp mean gas-particle relaxation timescale
REFERENCES
1. Ansart, R., Neau, H., Accart, P., de Ryck, A. and Simonin, O. (2010). “Separation
and Taking Off in a Fluidized Bed: Comparison between Experimental Measurements
and Three-dimensional Simulation Results”, Proceedings of 7th International Confer-
ence on Multiphase Flows, Florida USA.
2. Balzer, G. and Boelle, A. and Simonin, O. (1995). “Eulerian Gas-Solid Flow Mod-
elling of Dense Fluidized Bed”, FLUIDIZATION VIII, Proc. International Symposium of
the Engineering Foundation, J.F. Large and C. Laguérie (Editors).
3. Gobin, A., Neau, H., Simonin, O., Llinas, J.R. and Reiling, V. and Sélo, J.L. (2003).
“Fluid Dynamic Numerical Simulation of a Gas Phase Polymerization Reactor”, Int. J.
for Num. Methods in Fluids, 43, 1199-1220.
4. Boelle, A., Balzer, G. and Simonin, O. (1995). “Second-order prediction of the pre-
diction of the particle-phase stress tensor of inelastic spheres in simple shear dense
suspensions”, In Gas-Particle flows, Vol. 228, ASME FED. 9-18.
5. Parmentier, J.F., Simonin, O. and Delsart O. (2008). “A numerical study of fluidiza-
tion behavior of Geldart B, A/B and A particles using an eulerian multifluid modeling
approach”, 9th International Conference on circulating fluidized beds. Hamburg, Ger-
many.
6. Agrawal, K., Loezos, P., Syamlal, M. and Sundaresan, S. (2001). “The Role of
Mesoscales Structures in Rapid Gas-solid Flows”, J. Fluid Mech., 445, 151-185.
7. Parmentier, J.F., Simonin, O. and Delsart O. (2010). “A functional subgrid drift ve-
locity model for filtered drag prediction in dense fluidized bed”, Submitted to AIChE
Journal.
8. Neau, H., Laviéville, J. and Simonin, O. (2010). “NEPTUNE CFD high parallel com-
puting performances for particle laden reactive flows”, Proceeding 7th International
Conference on Multiphase Flows, Florida USA.
9. Fede, P., Moula, G., Ingram, T. and Simonin, O. (2009). “3D numerical simulation
and pept experimental investigation of pressurized gas-solid fluidized bed hydrody-
namic”, Proceedings of ASME 2009 Fluids Engineering Division Summer Meeting.
ASME.
EROSION IN SECOND STAGE CYCLONES: EFFECTS OF
CYCLONE LENGTH AND OUTLET GAS VELOCITY
S. B. Reddy Karri*, Ray Cocco and Ted M. Knowlton
Particulate Solid Research, Inc.
4201 W. 36th Street, Chicago, IL 60632, USA
ABSTRACT
Severe erosion in the lower cone and in the upper dipleg of second stage cyclones
have been observed in commercial cyclones. The main objective of this study is to
shed light on the mechanism by which this erosion takes place, and how different
design and operating parameters affect the erosion. Experimental data on how
parameters such as the cyclone length-to diameter ratio (L/D), inlet solids loading
and gas outlet velocity affect second stage cyclone erosion are presented. The
outlet gas velocity was varied by changing the size of the vortex tube diameter. The
effect of a vortex stabilizer on cyclone cone erosion is also discussed.
INTRODUCTION
Petroleum refineries have increased their focus on improving unit reliability, and
reducing operational and maintenance costs. Because their cyclones have high
efficiencies, fluidized catalytic cracking unit (FCCU) process operators are now
concerned with longer campaign durations, and would like to improve cyclone
reliability. The 2008 NPRA survey and other surveys (1,2) revealed that FCCU
cyclone reliability (3,4) was a major concern for refineries. The most pervasive
problem is erosion in secondary cyclones in the lower cone and upper dipleg, which
is the focus of this study.
There is a fundamental difference between first and second stage FCC cyclones in
regard to erosion patterns. Highly-loaded first stage cyclones normally experience
no cone erosion, whereas lightly-loaded second stage cyclones can have severe
cone erosion. This seems to be counter-intuitive, but can be explained by the
differences in the solids flow patterns and vortex lengths, as shown in Figure 1.
Due to the high solids loading and the low gas inlet velocity in a typical FCCU
primary cyclone, gravitational force plays a key role. As a result, the solids appear to
fall rapidly down into the cyclone cone and dipleg, as shown in Fig. 1, taking only one
to two full turns before exiting the cyclone. The vortex length in a highly-loaded
Primary Cyclone Secondary Cyclone
(High Loading) (Low Loading)
Inner Vortex
Longer , Energetic,
Inner Vortex
Solids Flow Path

(Outer Vortex) Many More Turns on
Tighter Radius: Spins
Faster – Hence More
Potential for Erosion
Figure 1. Schematic Depiction of First and Second-Stage Cyclone Operation
primary cyclone is much shorter, because the high solids loading dampens the
formation of a long vortex. Therefore, the vortex does not “whip” the solids at a high
velocity around the cone as in a primary cyclone.
In a typical second stage cyclone, the solids loading is approximately 1/1000 to

1/10,000 of the loading in the first stage cyclone. Due to the light solids loading and
high gas velocity, the inner vortex is relatively long and energetic. As the swirling
solids in the outer vortex approach the cone in a second stage cyclone, the long,
rapidly-rotating vortex accelerates the solids stream and causes it to intensify its
rotation because of the conservation of angular momentum. The solids in a second-
stage cyclone typically take four to seven turns before exiting the bottom cone, and
the spinning continues into the top portion of the dipleg below the cone. Most of
those spins are located in the lower part of the cone and in the upper dipleg where
the small diameters result in high angular velocities. The rapidly-rotating solids
stream coupled with the unstable, continuous movement of the vortex causes
significant erosion in the cone and at the top of the dipleg of second-stage cyclones.
EXPERIMENTAL
The testing was structured to benchmark three possible solutions to mitigate the
erosion occurring in second-stage cyclones: 1) increasing cyclone length-to-diameter
ratio (L/D), 2) increasing the angle of the cone, and 3) adding a vortex stabilizer.
The cyclone test facility used in the study is shown in Fig. 2. It consisted of a 0.91-
m-diameter fluidized bed, a 0.2-m-diameter standpipe approximately 17 m in length;
a slide valve to control the solids flow rate around the unit; a 0.2-m-diameter riser
approximately 21 m tall; a 0.48-m-diameter first stage cyclone; and the 0.43-m-
diameter second stage cyclone.
2
Air was used as the conveying gas in
the test unit. The solids used were
17 18
16 15
2nd Stage Cyclone
14R equilibrium FCC catalyst with a median
1st Stage Cyclone
(dp,50) particle size of 75 m. The fines
(material < 44 microns) concentration
Diverter Valve 20-cm Riser
in the catalyst was approximately 8
13R wt.%. The particle density of the
catalyst was 1490 kg/m3. Loadings to
the second stage cyclone were varied
12R
between 0.001 to 0.21 kg/m3. The
secondary cyclone was constructed
Automatic L-Valve modularly for easy change of
0.91-m -Bed dimensions. A schematic drawing of
the second stage cyclone is shown in
11R
Fig. 3 for several different barrel

Receiving Tank
on Load Cells
20-cm Standpipe
lengths. Multiple coatings of drywall
10R
joint compound were added to the
inside of the cyclone before each test.
The amount of erosion occurring in the
Figure 2. Schematic Drawing of cyclone was measured by the weight
Cyclone Erosion Test Unit loss of the drywall compound occurring
over a certain period of time.
1"
44
[10.80]
7° 7° 7°
1'-5" 1'-5" 1'-5"

[43.18] [43.18] [43.18]
9"
9" [22.86] 1'-9" 1'-9" 1'-9"
[22.86] [53.34] [53.34] [53.34]
6"
[15.41]
1'-5" 1'-5"
1"
2'-84 [43.18] [43.18]
[81.92]
1'-5"
1"
2'-84 [43.13]
4" [81.92]
[10.16]
1"
2'-84
4" [81.92]
[10.16] 79°
4"
L/Db = 3.1 L/Db = 4.1 L/Db = 5.1

Figure 3. Schematic Drawing of Different Cyclone L/D's [cm]
Effect of Increased Cyclone L/D
3
The study found that the erosion took place
primarily in the bottom 1/3 of the cone of
the secondary cyclone”. A photograph
illustrating this effect is shown in Fig. 4.
This figure shows that the drywall coating
was completely eroded from the bottom
1/3 of the cone, whereas the remaining
drywall was mostly intact.
Cyclone lengths were increased by

increasing the length of the cyclone barrel
to give length-to-diameter (L/D) ratios of
3.1, 4.1 and 5.1. In these tests, the inlet
gas velocity to the cyclone was 19.8 m/s
and the outlet gas velocity was 27 m/s.
The results of the testing to determine the
effect of cyclone L/D is shown in Fig. 5.
As can be seen, the erosion rate
Figure 4. Photograph of Erosion of decreased with increasing cyclone L/D.
Drywall Joint Compound in the The measured erosion rate at an L/D of 5.1
Cone of a Second-Stage Cyclone was about 70% of the erosion rate of the
cyclone with an L/D of 3.1.
Barrel erosion
800
rates were also Material: FCC Eq. Catalyst
measured in the Ugi: 19.8 m/s
700
Ugo: 27 m/s
tests and were Cyclone Size: 43-cm
600
found to be much h
/ Inlet Type: Tangential
g
lower than the ,
s 500 Li : 0.011 kg/m3
erosion rates in e
t L/Db:
a 400
the cone (Fig. 5). R
n
3.1
Measured barrel o
i
s 300 4.1
erosion rates ro 5.1
E 200
ranged between
85 to 105 g/h, 100
which was about
0
15% of the cone
Cone Barrel
erosion rate for
the cyclone with
an L/D of 3.1, and
about 20% for a Figure 5. The Effect of Second-Stage Cyclone L/D on Cone
cyclone with an Erosion and Barrel Erosion
L/D of 5.1.
Effect of Cone Length
The effect of cone length on cyclone cone erosion was tested by adding a longer
cone so that the cone angle from the horizontal increased from 79 to 84º. This
increased the cone length from 0.82 to 1.68 m. When comparing the two cone
configurations, the overall length of the cyclone was held constant.
4
As shown in Fig. 6, the cyclone with the longer cone had a higher erosion rate at low
outlet gas velocities than the cyclone with the shorter cone but longer barrel.
However, the erosion rate became approximately equal to the erosion rate of the
shorter cone at the highest outlet gas velocity. The trend of the two curves was
exactly opposite. For the cyclone with the shorter cone, the erosion rate increased
with gas velocity, whereas for the longer cone the erosion rate decreased with gas
velocity. For an outlet gas velocity of approximately 27 m/s, the erosion rate for the
short cone cyclone Ugo, m/s
was approximately 0 10 20 30 40 50 60
800 g/h, while the 2500
Cone Erosion Rate, g/h

erosion rate for the
long cone cyclone 2000
was approximately
1500 Longer Cone
1800 g/h, a factor of
2.25. However, 1000
shorter cone
Material: FCC Eq. Catalyst
even at the highest Ugi: 19.8 m/s
outlet gas velocities, 500 Cyclone Size: 43-cm
which were outside Inlet Type: Tangential
Li : 0.032 kg/m3; L/Db: 5.1
typical operating 0
0 50 100 150 200
outlet velocities of Ugo, ft/s
secondary cyclones,
the longer cone did Figure 6. The Effect of Cone Length on Second-Stage
not have a Cyclone Cone Erosion
significant
advantage over the shorter cone in regard to cone erosion
Vortex Stabilizers
To determine the effect of adding a vortex stabilizer on cone erosion, a flat-disk

vortex stabilizer was added in the
cyclone cone, approximately 1/3
1" Stabilizer
of the cone length from its 74
Disk
bottom, at the top of the region in [18.42]
which the cone erosion was most
1"
significant. A photograph of the 102 79°
disk is shown in Fig. 7. [26.78]
4"
The location of the vortex [10.16]
stabilizer was selected to be at
the top of the high-erosion section
of the cone. It was thought that
adding the vortex stabilizer 1/3 of
the cone height from the bottom
of the cone would prevent high-
velocity spinning solids in that
region and reduce erosion. The No Erosion
purpose of the flat plate (or the
vortex stabilizer) was to stabilize Three Supports
the central vortex. It was
expected that the influence of the Figure 7. Photographs and Schematic
vortex would end at the plate, and Drawing of the Vortex Stabilizer and Supports
5
the number and intensity of the solids spirals below the plate would be reduced.
The effect of adding the vortex stabilizer disk on cyclone cone erosion is shown in
Figs. 8 and 9 for cyclones with L/Ds of 3.1 and 5.1, respectively. It was found that
cone erosion for a cyclone with a vortex stabilizer was significantly lower than that for
a cyclone without a vortex stabilizer. Cone erosion was found to increase linearly
with increasing gas velocity for a cyclone without a vortex stabilizer. However, cone
erosion in a cyclone with a vortex stabilizer decreased slightly with increasing gas
outlet velocity. The decrease in erosion is counter-intuitive. However, this can be
explained by the fact that the vortex diameter is smaller when the diameter of the
outlet tube is decreased. This
increases the distance between 0 20
Ugo, m/s
40 60
the vortex and the cone wall, 3500
Cone Erosion Rate, g/h

which then reduces the 3000
w/o disk
centrifugal force (and, therefore, w/ disk

2500
the solids velocity) on the solids Material: FCC Eq. Catalyst
rotating in the cone. The 2000 Ugi: 19.8 m/s
Cyclone Size: 43-cm
reduction in force on the solids 1500 Inlet Type: Tangential
appears to explain the decrease 1000
Li : 0.032 kg/m3; L/Db: 3.1
of cone erosion vs. gas outlet
500
velocity for a cyclone with a
vortex stabilizer (Figs. 8 and 9). 0
0 50 100 150 200
Ugo, ft/s
For the shorter cyclone, the
cone erosion rate was Figure 8. The Effect of Gas Outlet Velocity on
approximately 2100 g/h for the
Second-Stage Cyclone Cone Erosion for
cyclone without a vortex Cyclones With and Without a Flat-Plate Vortex
stabilizer at an outlet gas
Stabilizer Ugo, m/s
velocity of 15.2 m/s. The 0 10 20 30 40 50 60
corresponding cone erosion 1600
rate for the cyclone with a Material: FCC Eq. Catalyst
C o n e E ro si o n R a te , g / h
1400
Ugi: 19.8 m/s
vortex stabilizer at the same 1200 Cyclone Size: 43-cm
outlet gas velocity was about 1000
Inlet Type: Tangential
Li : 0.032 kg/m3; L/Db: 5.1
1400 g/h. The cone erosion 800
rate with the vortex stabilizer 600
was about 67% of the cone 400
w/o disk
erosion rate for the cyclone 200

w/ disk
without the vortex stabilizer. 0

However, at an outlet gas 0 50 100
Ugo, ft/s
150 200
velocity (45.7 m/s) closer to

actual practice, the cone Figure 9. The Effect of Gas Outlet Velocity on
erosion rate for a cyclone with Second-Stage Cyclone Cone Erosion Rate for
the vortex stabilizer was only Cyclones With and Without a Flat-Plate Vortex
about 600 g/h. The Stabilizer
corresponding cone erosion
rate for a conventional cyclone without a vortex stabilizer was about 2900 g/h. This
was a factor of about 4.8.
For the cyclone with an L/D of 5.1, the overall cone erosion rates were lower. This
was expected because the tests with the longer cyclone described above gave lower
cone erosion rates than shorter cyclones. As with the shorter cyclone, the trendlines
6
of cone erosion rate vs. outlet gas velocity were linear. Similarly, the curve for the
conventional cyclone erosion rate without a vortex stabilizer increased with
increasing gas velocity, and the curve for the cyclone erosion rate with the vortex
stabilizer decreased slightly with increasing gas velocity. However, as with the
shorter cyclone, the cyclone with the vortex stabilizer was found to have much lower
erosion rates than the conventional cyclone without the vortex stabilizer. Comparing
the cone erosion rates at an outlet gas velocity of 45.7 m/s, the conventional cyclone
without a vortex stabilizer had a cone erosion rate of approximately 1200 g/h, while
the cyclone with the vortex stabilizer had a cone erosion rate of about 240 g/h. This
is a factor of approximately 5 - similar to what was found for the shorter cyclone.
Why does the vortex stabilizer decrease cone erosion? It appears that the stabilizer
prevents the vortex from "whipping" the solids around at high velocities below the
stabilizer in the region where high cone erosion rates are experienced for a cyclone
without a vortex stabilizer. Below the stabilizer, the high-velocity central vortex does
not really exist. Therefore, this reduction in the spinning solids velocity at the wall
leads to a significant reduction in erosion. A comparison of the cone erosion rates
for various second-stage cyclone configurations is given in Table 2.
Drywall joint compound was also added to the disk to see if the upper surface of the
vortex stabilizer would erode. However, essentially no erosion was measured on the
upper surface of the disk, and no erosion was found on the supporting rods.
Shell Experience with Vortex Stabilizers
In the 1980’s, Shell had over 30 FCC units, mostly with cyclones without vortex
stabilizers, which were found to be the number one cause of all FCC unscheduled
shutdowns. Shell started using the vortex stabilizer (5) in the early 90’s. Fig. 11
shows the result of how the vortex stabilizer reduced overall FCC unscheduled down
time.
Table 2. Comparison of cone erosion rates for different cyclone configurations

Erosion Cone
Velocity Velocity
L/D Reduction Erosion
Inlet, m/s Outlet, m/s
(-) Factor Rate, g/h
Short Cyclone 3.1 19.8 45.7 Base 2850

Long Cyclone 5.1 19.8 45.7 >2 1200
Long Cone 5.1 19.8 45.7 >2 1200
Vortex Stabilizer 3.1 19.8 45.7 >4 650
Vortex Stabilizer 5.1 19.8 45.7 >11 240
Using 1992 data as the base line, Fig. 11 shows that cyclones with the vortex
stabilizer reduced the total unit down time of all FCC units in the Shell system by a
factor of 10 over a period of 8 years.
7
Total Severity of Cyclone Problems
100%
Severity (Incl. near misses) [Number of
90%
Events * Duration] 1992 = 100%
80%
70%
60%
50%
40%
30%
20%
10%
0%
1992 1993 1994 1995 1996 1997 1998 1999
Figure 10. Cyclone Severity vs. Time
CONCLUSIONS
Second stage cyclone cone erosion is a pervasive problem in FCCU operation,
which can be significantly improved by incorporating the use of a vortex stabilizer.
Vortex stabilizers were more effective in reducing second stage cyclone cone
erosion than increasing cyclone barrel or cone length.
REFERENCES
1. Solomon Associates LLC , 2006 Solomon FCC Events Determining TAR Timing
Survey, 2006
2. Grace Davison Survey, FCC Conference in Dublin, California, USA, 2002
3. Zenz, F.A., Cyclone Separators, in Manual on Disposal of Refinery Wastes
Volume on Atmospheric Emissions, Chapter 11, American Petroleum Institute,
Pub. No. 931, Washington, D.C. (1975).
4. Tenney, Ed., FCC Cyclone Problems And How They Can Be Overcome With
Current Designs, Presented at the Grace-Davison FCC Technology Conference,
Toledo, Spain (1992).
5. Chen, Y., Karri, S.B.R., Knowlton, T.M., Winning in the Downturn: How to
Improve FCC Unit Reliability and Reduce Costs via Improved Cyclone
Technology, NPRA Meeting, Phoenix, AZ (2010).
6. Sexton, J., Karri, S.B.R., Knowlton, T.M., “What is Happening Above Your
Fluidized Bed?” Tools to Maximize FCC Unit Reliability and Turnaround Cycles,
NPRA Meeting, Phoenix, AZ (2010).
8
STUDY OF CALCINATION-CARBONATION OF CALCIUM CARBONATE
IN DIFFERENT FLUIDIZING MEDIUMS FOR CHEMICAL LOOPING
GASIFICATION IN CIRCULATING FLUIDIZED BEDS
Bishnu Acharya*, Animesh Dutta** and Prabir Basu

**Department of Mechanical Engineering, Dalhousie University, Halifax, Nova Scotia,
B3J 1Z1 Canada**School of Engineering, University of Guelph, Guelph, ON, N1G
2W1, Canada
ABSTRACT
Chemical looping gasification (CLG) of biomass in a circulating fluidized bed is an
excellent option for production of separate streams of hydrogen rich and carbon
dioxide rich gases. This process uses H2O (steam) instead of air or oxygen for
gasification, and thereby produces high value nitrogen free product gas. An
important feature of this process is in-process removal of carbon dioxide from the
reaction site by CaO. This allows the reaction to move towards higher yield of
hydrogen. Circulating fluidized bed (CFB) provides an ideal reactor configuration for
such a looping reaction. A CFB based CLG unit operates somewhat similar to the
FCC reactor except that the bubbling bed in the loopseal serves as the gasifier
where calcined limestone absorbs carbon dioxide forming calcium carbonate. The
riser works as the regenerator of CaCO3, the CO2 sorbent. Thus, the sorbent
particles move back and forth between the riser calciner and loopseal carbonizer. To
study this process closely and to determine how well the sorbent retains its reactivity
through such a cyclical process, an experiment was carried out in a Quartz wool
matrix reactor (QWM), which closely simulates the highly expanded ambience of a
fast-fluidized bed. An empirical relation was developed for the conversion of calcium
carbonate (CaCO3) as a function of temperature and residence time. A simple
reaction kinetic model for calcination in presence of N2, CO2 and H2O has been
developed and compared. Loss in effectiveness of the sorbent has been studied and
another empirical relation was developed for the estimation of extent of carbonation
with the number of cycle.
INTRODUCTION
Chemical looping gasification (CLG) is an innovative approach for production of

hydrogen-rich gas with in-process capture and regeneration of carbon dioxide. It
consists of two fluidized bed reactors, one operating as a gasifier in bubbling bed
mode, and another as a regenerator in fast fluidized bed regime, together forming a
circulating fluidized bed reactor. Calcium oxide (CaO) is used as the sorbent in the
gasifier. It absorbs the carbon dioxide produced during gasification and is
subsequently regenerated in the regenerator. Thus, from the gasifier a CO 2 free
hydrogen-rich gas is obtained while from the regenerator, a relatively pure stream of
carbon dioxide is produced that can be taken directly for sequestration or other value
added use thus avoiding the cost and efficiency penalty for post capture. The main
focus of this paper will be on the study of regeneration behaviour of calcium
carbonate.
The calcination reaction (CaCO3 = CaO + CO2 +183 kJ/mol) is highly endothermic in
nature. Also its capacity for regeneration of CaO depends on the fluidizing medium in
the fast fluidized bed. The fluidizing medium in the riser for the study was chosen to
1
be carbon dioxide because the CFB riser is to use a part of the CO 2 produced
(Acharya et al, 2009). The partial pressure of carbon dioxide in this case will naturally
be very high, and it might be above the equilibrium pressure of CO2 for calcination.
Therefore, one would expect a very low regeneration of the sorbent, CaO. This
necessitates an alternative medium that could not be air due to potential nitrogen-
dilution of the product gas from the nitrogen in air. So, steam is identified as the next
best and yet inexpensive fluidizing medium.
The main objective of this research is to determine the level of regeneration with
nitrogen (N2), carbon dioxide (CO2) and steam (H2O) as the fluidizing medium and
compare them. Ideally the work should be done in a fast-fluidized bed, but it is
extremely difficult to follow the calcination process while the particles are constantly
moving around the CFB loop. Standard Thermo Gravimetric (TGA) test is more
representative of a fixed bed than of a fast bed reactor. Fast bed reactor is
characterized by it is highly expanded bed, where reacting particles are widely apart.
For this reason experiments were done in the quartz wool matrix reactor developed
by Wu and Basu (1993), where particles were dispersed on a quartz wool matrix with
a voidage similar to that of a fast bed. The gas velocity was adjusted to represent the
gas-solid slip velocity in a fast bed. Thus, this closely simulates the reaction in the
riser of a CFB. A reaction kinetic model was developed for calcination in three
different mediums. The comparisons of different medium were made on the basis of
activation energy and the reaction rate constant. The results obtained could provide
a basis for the choice of fluidizing medium for the regenerator in a chemical looping
gasification system. In a CFB-CLG reactor the sorbent will continuously move back
and forth between the gasifier and the regenerator undergoing calcination and
carbonation. So, the calcination-carbonation cycle was studied to identify the loss in
activity of sorbent over different cycle. This will help to identify the requirement of
fresh sorbent into the system.
EXPERIMENTAL SETUP
The quartz wool matrix reactor comprises a stainless steel reactor of 50 mm internal
diameter heated externally by electric heaters (Fig 1). A precision electronic balance
sits at the top of the reactor. Temperature was measured at three different locations
of the reactor with K type thermocouple. Data from the balance, thermocouple and all
flow meters were recorded by a data acquisition system. Reactor was heated to the
desired temperature and then the gas was supplied from the bottom of the reactor.
Flow of gas, (or gas mixtures) going into the reactor was measured by electronic
regulating type flow meters. A measured weight of calcium carbonate of size 45
micron was sprinkled over and inside the quartz wool that was placed inside a wire
basket suspended on the balance. The particle size was deliberately chosen small to
reduce the mass transfer effect as well as to make sure that the particle size was
significantly smaller than the reactor size. Once the system was stabilized and a
constant temperature in the reactor was noted, the basket with quartz wool and
calcium carbonate was lowered into the reactor. The change in mass of the sample
was measured continuously. After allowing the reaction (calcination and carbonation)
for 30 minutes it was taken out, cooled and was weighted.
2
After calcination for 30 min, the sample was moved out into a cooler ambient to
quench the calcination reaction. Thereafter, the medium in the QWM was changed to
carbon dioxide and the temperature of reactor was reduced to 650oC. Once the
temperature drops to 650oC, the previously calcined sample was lowered into the
reactor, and was left there for another 30 min for carbonation. Thus the sample
undergoes alternative calcination and carbonation. It is repeated for 5 cycles of
calcination and carbonation.
The calcination reaction (CaCO3 = CaO + CO2) was studied at four temperatures:
800oC, 900oC, 950oC and 1000oC for each of the three media, CO2, H2O and N2. The
carbonation reaction (CaO + CO2 = CaCO3) in a biomass gasifier generally takes
place at a relatively lower temperature in a CLG. So, in QWM reactor, the
carbonation was studied at 650oC with CO2 alone. Experiments in CO2 alone ensure
that complete conversion of calcium oxide. Any loss in conversion over consecutive
cycle could occur due to sintering of the particle.
Figure 1: Schematic of QWM experimental setup

To examine the kinetics of calcination as well as to compare the rate for three media
a first order reaction kinetic model was used.
dX (1- X)(Peq - PCO2 )

=K (1)
dt Peq
(Stanmore and Gilot, 2005)

Where, K = intrinsic rate constant (s-1), X = conversion (-), Peq = equilibrium
decomposition pressure (atm), PCO2 = partial pressure of CO2 (atm), ko = reaction
rate constant (s-1), Ea = activation energy (kJ/mol), R = universal gas constant
3
(kJ/mol K), T = temperature (K), Wo = initial weight of calcium carbonate (gm), Wt =
weight of calcium carbonate after time t (gm).
Effect of Temperature and Residence Time on Calcination
Table 1 shows the results of calcination at different temperatures in presence of

three different media. A conversion greater than 99% was obtained at 900oC in a N2
environment in 12.5 min. The same level of conversion was obtained in a shorter
time if the temperature increased to 950oC. In CO2 environment this conversion at
900oC was only 72.89%. Even at 1000oC the maximum conversion was 92.95% in
30 min. A higher partial pressure of CO2, close to the equilibrium decomposition
pressure would inhibit the calcination reaction. Therefore at such high CO 2 partial
pressure the conversion is much lower even at very high temperatures. With steam,
complete conversion was obtained in shorter residence time of 10 min at a
temperature of 1000oC.
Table 1: Calcination obtained during calcination under three different mediums
N2 CO2 H2O
Temperature Conversion Time Conversion Time Conversion Time
(oC) (%) (mins) (%) (mins) (%) (mins)
600 8.78 30
700 52.29 30 73.22 30
800 96.32 25.50 7.58 30 96.94 30
900 99.39 12.5 20 30 100 25
950 99.31 10 72.89 30 100 19.16
1000 100 10 92.95 30 100 10
Supply of N2 and steam quickly removes carbon dioxide from the system, thus
lowering its partial pressure resulting in higher conversion. However, steam offers
higher conversion than N2. At 700oC, 73.22% conversion was obtained which was
28% more than that obtained with N2 at the same temperature. Steam seems to
have a catalytic effect that lowers the equilibrium decomposition temperature for
calcination reaction to occur, thus conversion has been complete even at very low
temperature. Wang and Thompson (1995) found that the surface adsorption of H2O
molecules weakens the CaO-CO2 bond resulting in enhanced calcination rates. Iyer
et al (2005) attributed this phenomenon to higher gas-solid heat transfer properties of
steam. Therefore the calcination obtained was much higher with steam.
The calcination with steam can occur at a lower temperature, but it needs longer
residence time. As shown in Fig 6, it will take a long time to achieve full conversion
with CO2 as medium, while it takes 10 min with N2 and 19 min with steam at 950oC.
Therefore, to study the combined effect of temperature and residence time, a linear
regression model was developed.
The fractional conversion of CaCO3, X is expressed empirically as a function of
temperature θ and time τ.
4
For H2O:
X = -1627 + 1.68 θ +46.1 τ – 0.0416 θ τ [R2 = 88.8%] (2)
For CO2:
X = -359 + 0.446 θ [R2 = 79.3%] (3)
For N2:
X = 186 – 0.126 θ – 14.6 τ + 0.0188 θ τ [R2 = 99.1%] (4)
Here, θ = Temperature (oC), τ = time (min) and X = conversion of CaCO3 (%).
From Table 1 it is apparent that the conversion of CaCO3 in presence of H2O
reduces with reduction in temperature, but there was a sharp order of magnitude
drop in conversion when the temperature drops from 700oC to 600oC. Reasons for
this large reduction below 700oC could not be explained at this time.
Figure 2: Calcination obtained with time at T = 950oC for three different media
Kinetics of Calcination
The intrinsic rate constant (Eq. 1) for calcination was calculated at each temperature
and by the use of the Arrhenius plot; the activation energy was determined. The
activation energy and the reaction rate constant for the calcination reaction occurring
in presence of three media is shown in Table 2.
Table 2: Kinetics of calcination under three different media
N2 CO2 H2O
Ea (kJ/mol) 257.78 180.56 248.62
ko (1/s) 4.82x1010 2.12 x106 3.63 x1010
5
Figure 3: Arrehenius plot for calcination done in presence of three medium
Fig 3 shows the comparison of reaction kinetics in presence of different media. it
suggests that the kinetic rate in presence of steam is closer to that in presence of
nitrogen. On the other hand for CO2 the kinetics rates are significantly lower.
Calcination and Carbonation Reaction Cycle
In a chemical looping system, the sorbent (CaO) undergoes through number of
calcination-carbonation cycle and with each cycle its performance decrease. This
could occur due to sintering and deposition of tar/char on sorbent particles. The
change in percentage of CaO in the sorbent particle during calcination-carbonation
cycle is plotted against time in Fig 4. Calcination occured in presence of N2, CO2 or
H2O while carbonation in CO2.
Figure 4: Calcination-carbonation cycle
6
Figure 5: Calcination and carbonation conversion obtained at the end of each cycle
Fig 5 shows the total conversion obtained at end of each calcination and carbonation
cycle studied. Calcination in presence of steam and N2 shows nearly complete
conversion at the first cycle studied and then drops slightly for latter cycles. In
presence of CO2, the conversion was only partial even for the first cycle and drops
quickly in the subsequent cycle.
The carbonation study shows that irrespective of the medium used for calcination,
the ability of the sorbent CaO to capture carbon dioixde decreases with number of
cycle. Stanmore and Gilot (2005) inferred that in high temperature calcination, the
calcium particles sinters leading to decrease in porosity and surface area
compounded by the pore closure due to carbonation (due to difference in molar
volume of CaO and CaCO3) resulting in loss of conversion. Thus to quantify this loss
in ability of the sorbent to capture CO2, an emperical relation was developed
between the conversion, XCaO obtained and the number of cycle, N.
XCaO = - 18.63 ln (N) + 62.598 (5)
Using this relation one can estimate the frequency at which the fresh sorbent needs
to be charged into a CFB based chemical looping gasifer. Limitation of this emperical
relation is that it only includes the effect of high temperature sintering phenomenon
but does not include other effects that may influence in a commercial chemical
looping gasification system. The deposition of tar and carbon on the sorbent are
examples of such inhibiting factors. These can only be studied in the real chemical
looping gasification system.
CONCLUSION
The study on calcination of CaCO3 in presence of different media shows that the
calcination shown in presence of H2O is similar to that in N2. The kinetic of
calcination in N2 and H2O are much higher than that for CO2. Compared to other
media steam offer higher conversion at a relatively low temperature. Thus steam
reduces the energy requirement of calcination, which may partially offset the energy
required to produce the additional steam.
7
Figure 6: Conversion obtained during carbonation with number of cycles
Considering this and the potential dilution of the product gas with N2, steam could be
the best medium in the riser in a chemical looping gasification system. However one
can expect a lower conversion in a large chemical looping CFB system than that
obtained in the present bench scale study. Therefore, a study on calcination-
carbonation looping cycle in a pilot lab scale chemical looping gasification plant is
underway.
ACKNOWLEDGEMENT
The authors thank Natural Science Engineering Council financial support to the first
author. It also thanks Greenfield Research Incorporated for financial support and use
of the QWM reactor for this study.
REFERENCES
1. Wu, S. and Basu, P, 1993. Surface reaction rates of coarse bituminous char
particles in the temperature range 600 to 1340K. Fuel 72, 1429-1433
2. Acharya B, Dutta A, Basu P, 2009. “Chemical-Looping Gasification of Biomass for
Hydrogen-Enriched Gas Production with In-Process Carbon Dioxide Capture”,
Energy Fuels, 23, 5077–5083.
3. Y. Wang, W.J. Thomson, 1995. “The effects of steam and carbon dioxide on
calcite decomposition using dynamic X-ray diffraction”, Chem. Eng. Sci. 50, 1373–
1382.
4. M, Gupta H, Wong D, and Fan L.S., 2005. Enhanced Hydrogen Production
Integrated with CO2 Separation in a Single-Stage Reactor”, DOE annual progress
report DE-FC26-03NT41853
5. Stanmore.B.R and Gilot P, 2005. “Review-calcination and carbonation of
limestone during thermal cycling for CO2 sequestration”, Fuel Processing
Technology 86 (2005) 1707– 1743
8
BENCH-SCALE INVESTIGATION OF LIMESTONE SIZE
EVOLUTION IN A FLUIDIZED BED COMBUSTOR
Xuan Yao 1, Nan Hu 1, Hairui Yang 1*, John H. Chiu2, Pierre Gauville2,
and Shin G. Kang2
1
2
Boiler Combustion Systems, Alstom Power Inc., Windsor, CT, 06095 U.S.A.
ABSTRACT
The influence of temperature, heating rate and chemical reaction on fragmentation

and attrition of limestone in a fluidized bed (FB) was investigated. The intensity of
fragmentation and attrition was measured in the same apparatus but at different
fluidizing velocities and fluidizing media. It was found that the heating rate has a
positive effect on fragmentation for the tested limestones. The effect of bed
temperature on limestone fragmentation was inconclusive. The influence of
chemical reaction on the fragmentation seems to be complicated; CO2 release due to
calcination would prompt fragmentation while the sulfation would increase the gas
diffusion resistance and depresses the fragmentation intensity. On the other hand,
the CaSO3/CaSO4 layer was found to be attrition-resistant leading to small attrition
rates. Attrition rate constant showed to decay exponentially with time and
approaching a constant for all limestone particles. Particle sizes between 200-400 m
have larger attrition rate constant than coarse ones perhaps due to their large specific
surface area.
INTRODUCTION
Limestone is commonly used as a desulfurization sorbent in fluidized bed and

circulating fluidized bed (CFB) boilers to reduce SO2 emissions. After limestone is
added to the furnace, substantial changes in the sorbent particle size distribution,
namely comminution, can be caused by limestone fragmentation and attrition [1-7].
Based on previous studies, fragmentation is often classified into primary and
secondary steps [6]. The primary fragmentation refers to the generation of
fragments, either coarse or fine, immediately after the injection of limestone particles
into the hot furnace [4, 6, 8, 9]. This process often occurs in the dense bed or in the
splashing zone of either FB or CFB combustors. The secondary fragmentation
refers to the generation of fragments mostly from high-velocity collisions against bed
material or reactor walls and internals. Attrition refers to the generation of fine
particles by abrasion and depends upon the resistance of the bed particles to surface
wear. Size evolution caused by fragmentation and attrition is strongly coupled with
the calcinations and sulfation processes as well as the overall mass balance in the
CFB system. Thus, factors impacting fragmentation and attrition play important
roles in the boiler performance.
Previous studies have investigated the impact of limestone type and size
[2,4,7,10-13], fluidizing gas velocity [6,8,9] and temperature [7,14] on fragmentation.
For a CFB boiler, scholars also found that fragmentation is influenced by the solids
circulation rate [2,3,8] and by the inventory of inert bed material [13-14], etc.
However, an investigation on the effect of chemical reaction, especially sulfation, on
1
limestone fragmentation is an issue of practical significance. In addition, the impact
of particle size, temperature and heating rate on fragmentation remains a
controversial topic in the literature [7,14]. Therefore, the aim of this work was to
conduct a systematic study of limestone fragmentation and attrition in the FB reactor
in order to further explore some of these factors.
A set of experiments on the primary fragmentation and attrition of two different

limestones was conducted in this study. The effects of heating rate, temperature
and initial particle size of the limestone were studied. Different fluidizing media (air,
SO2, CO2) were used in the experiment to study the influence of calcination and
sulfation on fragmentation and attrition behavior. The jet effect near the distributor
was not studied.
EXPERIMENTAL
The bench-scaled fluidized bed reactor used in this study was described in detail
previously [15]. The reactor was a round tube made of silica glass, with an inner
diameter of 54 mm and height of 800 mm. The reactor was electrically heated and
the main section could be maintained at a desired temperature with a deviation of
±5oC. An air distributor (a porous plate type) was placed near the middle of the
reactor. The section below the distributor was used to preheat the fluidizing gases.
During the fragmentation experiments, inert bed material, i.e., quartz sand (90-125
m) was pre-laid on the air distributor. The limestone was then added in batch mode
(20 g), with a particular initial size cut, and mixed with the quartz sand. The initial
static height of the bed material was kept at about 40 mm for all tests.
A rather low, superficial gas velocity, Ug, was set for the tests at about 0.1-0.2 m/s, at
a reactor temperature of 850oC, to minimize the attrition and secondary fragmentation.
Thus, all of the fragments formed could be attributed to the primary fragmentation.
After the limestone was added into the reactor for a prescribed time interval, all of the
materials, including limestone fragments and bed material, were aspirated out and
collected by a solids collection system. The bed material was then separated from
the collected mixture by a sieve shaker, and the particle size distribution (PSD) of the
residual fragments was obtained by sieving and weighing. The mass of the
fragments in the size range of the inert bed material (90-125 m) was estimated by
measuring the weight loss during calcination in a muffle furnace.
As in a previous study [16], the coefficient of average particle size variation, Fd, was
used to characterize the degree of particle size change, which can be expressed as
Fd = df/do, where df is the average Sauter diameter of new PSD and do is the average
Sauter diameter of the particles in the original sample. For purposes of discussion,
another parameter called the fragmentation intensity coefficient (FIC), defined as FIC
= 1 - Fd, was introduced to describe the intensity of fragmentation. The FIC can vary
between zero (no change in particle size) and near unity (denoting a substantial
decrease in particle size).
To measure the attrition rate by abrasion, a relatively high Ug (e.g., Ug 0.5 m/s) was
used such that fines with a diameter less than 80 m, generated by attrition, could be
elutriated and then collected by the solids collection system. Before the adding of
the testing sample, a certain amount of bed material of quartz sand (~160 g, 250-300
m) was pre-loaded in the reactor. The quartz sand was abrasion resistant and
2
remained in the reactor under the selected Ug. The bed was put into operation with
a preset Ug and bed temperature for a prescribed period until it was steady. The
testing sample, with a mass of 50 g, was then added to the bed. At 10 minute
intervals, the attrition rate, Rs, was obtained [1] by weighing the fine particles collected
in the cyclone with a total sampling time of about one minute duration. From these
data, the attrition rate constant, Ka, was calculated. The experiment was continued
until the attrition rate became steady. In this study, the influence of chemical reaction
was also evaluated by changing the fluidizing media. Limestone was first calcined in
the FB for 10 minutes under an air atmosphere; and then different mixtures of CO2
and SO2 were subsequently used to study the influence of sulfation.
Two kinds of limestone (types A and B) were studied. The CaCO3 and MgCO3
compositions measured by x-ray diffraction are listed in Table 1. Each limestone was
classified into 3 size groups of 200-400 m, 400-600 m, and 600-800 m in order to
study the effects of the initial particle size.
Table 1. The composition of the limestone samples (% in mass)

Sample Ca Mg CaCO3 MgCO3 Other
A 39.4048 - 98.51 - 1.49
B 38.5512 0.7811 96.38 2.73 0.89

0.5
Effect of Limestone Type and Original Size 0.45
Limesteone A
Limesteone B
0.4
Figure 1 shows the FIC of both limestone types 0.35
at a temperature of 850ºC under an air 0.3
atmosphere in the FB furnace. A higher FIC
FIC
0.25
value represents a higher fragmentation intensity 0.2
and a smaller average particle size produced. 0.15

0.1
For both limestone types, the enhanced
0.05
fragmentation of the tests with a larger initial 0
particle size classification is apparent. 200-400 400-600 600-800
However, a previous experimental study [15] origin particle size, m
indicates that the effect of particle size on Figure 1. Fragmentation intensity coefficient
fragmentation is not always the same, and depends (FIC) of limestones A and B under air
on the limestone type. The micro-structure of the atmosphere in FB (850°C)
particles could be very different for different limestone samples and could cause
significant differences in fragmentation and attrition [8]. In this study, it is believed
that the impact of the particle micro-structure, combined with other effects such as
heating rate, could be the reason for the ambiguous effect of initial particle size. This
phenomenon should be studied in more detail in future research.
Effect of Temperature on Fragmentation
In order to study the influence of temperature on the fragmentation of limestone, a

test was conducted under different temperatures (850 and 900ºC) in the FB reactor.
Figure 2 and Figure 3 show the changes in the cumulative particle size distributions of
limestone A with different initial sizes. The data appears to indicate, albeit not
conclusively, that the average particle size dS increases with temperature except
3
sizes between 400-500 m. Other study [14] showed that high temperature enhances
the attrition of particles but lessens the primary fragmentation. The author explained
that enhancement of CO2 release at high temperature is not strong enough to prompt
increased fragmentation in the bed. More studies are necessary in the future.
1 1
limestone limestone
0.9 0.9
FB-850 (ds=336 m)
0.8 FB-850 (ds=418 m)

FB-900 (ds=356 m) 0.8
FB-900 (ds=474 m)

Cumulative mass (%)
0.7 0.7
Cumulative mass,%

0.6 0.6
0.5 0.5
0.4 0.4
0.3 0.3
0.2 0.2
0.1 0.1
0 0
0 100 200 300 400 500 600 0 100 200 300 400 500 600 700 800
particle size( m) particle size( m)
Figure 2. Effect of temperature on the PSD Figure 3. Effect of temperature on the PSD
of fragmentation product (A, 400-600 m) of fragmentation product (A, 600-800 m)
Effect of Heating Rate on Primary Fragmentation
In order to simulate the effect of heating rate on the primary fragmentation of

limestone, various experimental conditions were used. In Figures 4 and 5, FB refers
to the baseline operational condition, C refers to the calcination of limestone in the
reactor without inert bed material (silica sand), and FB-H refers to the introduction of a
higher limestone weight (50g) to decrease the heating rate in the FB.
1 1
limestone limestone
0.9 C 0.9 C
0.8 FB 0.8 FB
FB-H FB-H
Cumulative mass (%)
Cumulative mass (%)
0.7 0.7
0.6 0.6
0.5 0.5
0.4 0.4
0.3 0.3
0.2 0.2
0.1 0.1
0 0
0 100 200 300 400 500 600 0 100 200 300 400 500 600
particle size( m) particle size( m)
Figure 4 Effect of heating rate on the PSD Figure 5 Effect of heating rate on the PSD
of fragmentation product (A. 400-600 µm) of fragmentation product (B. 400-600 µm)
As shown in Figures 4 and 5, compared with the initial limestone particle size, lime
calcined under FB condition is much finer than that of lime PSD obtained under the ‘C’
experimental condition. Under the ‘C’ experimental condition, where no inert bed
material was used, the thermal heating rate was mainly caused by radiation from the
wall and convection of high temperature gas, which induced a smaller heating rate
than that provided by silica sand bed. Therefore, the heating rate could enhance the
fragmentation of the limestone, especially for limestone B. The relative contribution
of the higher heating rate on fragmentation, provided by the silica sand particles, is
difficult to quantify, because it is coupled with the mixing-induced attrition caused by
4
the purely mechanical stresses of the sand particles on the limestone.
The comparison between the PSDs from the FB and FB-H conditions also illustrates
the promotion of thermo-mechanical and chemical effects by the heating rate on the
primary fragmentation intensity. Limestone is calcined into lime in the furnace
(endothermic process) and at the same time experiences thermal stresses as it is
heated up. The time required for complete fragmentation is about 4 to 6 minutes
longer for the larger sample weight (FB-H). But the effect of such a small difference
on attrition and particle size evolution is probably negligible. Because the output of
the electrical furnace is constant, less limestone sample means a higher heating rate.
In general, an improved heating rate can enhance calcination and prompt primary
fragmentation. Therefore, as shown in Figures 4 and 5, the fragmentation product
size of FB-H is less than that of FB condition.
Effect of Fluidizing Media on Fragmentation
The product gas from industrial CFB boilers is composed of CO2, SO2, NOX, etc.
These gas species may have a great impact on limestone fragmentation in the boilers.
Previous studies have found that the existence of a high CO2 concentration will
suppress the calcination and fragmentation of limestone [9,15,16]. SO2, calcined lime
absorbs SO2 to form CaSO3/CaSO4, which may also suppress fragmentation.
0.5 0.5
A-air B-air
0.45 0.45
A-800ppmSO2 B-800ppmSO2
0.4 A-2000ppmSO2 0.4 B-2000ppmSO2
0.35 0.35
FIC
FIC
0.3 0.3
0.25 0.25
0.2 0.2
0.15 0.15
0.1 0.1
0.05 0.05
0 0
200-400 400-600 600-800 200-400 400-600 600-800
limestone particle size(µm) limestone particle size(µm)
Figure 6 Fragmentation intensity of limestone A Figure 7 Fragmentation intensity of limestone B
with SO2 atmosphere with SO2 atmosphere
Figures 6 and 7 show FIC values of two kinds of limestone under different
atmospheres at a reactor temperature (850°C). It’s obvious that the SO2
suppressed the fragmentation of both kinds of limestone under the conditions used in
this study, at least for the larger particle sizes
Both limestone types have the largest fragmentation intensity under an air
atmosphere. The possible reason may be that fresh lime on the surface of the
particle reacted with SO2 and produced a harder, attrition-resistant layer of
CaSO3/CaSO4 product over the particle surface and may hinder the CO2 release.
Figure 8a shows CO2 concentration variation during the fragmentation process under
different fluidizing media. The release of CO2 is faster with air initially as comparing
to the SO2 atmosphere. But with the uncertainty of reading in low value the trend
seems reversed later. Figure 8b shows the accumulated CO2 released (normalizing
to 100%). As shown for the same percent of calcinations completed, fluidizing media
with air requires less time than that with SO2 case. This seems to confirm the
5
suppressing effect of the SO2 on CO2 release. On the other hand, the variation of SO2
concentration has no obvious impact on the FIC of limestone with short time duration.
The sulfation reaction of CaO and SO2, as a relatively long duration process, will take
hours to complete. Therefore, during the short time of primary fragmentation, the
variation of SO2 concentration from 800 ppm to 2000 ppm may have no appreciable
effect on the thickness of the layer and subsequently on the FIC.
Accumulative CO2 Concentration

12 100
90
CO2 concentration (%)
10 80 2000ppm SO2
800 ppm SO2
8 70 air
60
(%)
6 50
2000ppm SO2
40
4 800ppm SO2 30
2 Air 20
10
0 0
0 2 4 6 8 10 12 14 16 0 2 4 6 8 10 12 14 16
Time [min] Time (min)
Figure 8a CO2 concentration variation during Figure 8b Normalized CO2 concentration accumulated
fragmentation process (A, 400-600mm) during fragmentation process (A, 400-600mm)
Generally, three mechanisms are attributed to the

1
limestone fragmentation: thermal stress at high limestone
0.9
temperature, high internal pressure caused by FB
0.8 2000ppmSO2
organics or water evaporation and the CO2 release 2000ppmSO2+15%CO2
0.7
during calcination [5]. Calcination is a chemical
Cumulative mass
0.6
reaction process that will produce CO2 and lime 0.5
(CaO). At a certain temperature, calcination 0.4
reaction occurs only if the partial pressure of CO2 in 0.3
the environment is lower than the CO2 pressure at 0.2
chemical equilibrium [9,18]. The existence of 0.1
high CO2 concentration in the environment will 0
suppress the calcination reaction [16]. As shown in 0 100 200 300 400
particle size( m)
500 600
Figure 9, fragmentation was suppressed under an

Figure 9 PSD of fragmentation
atmosphere of 15% CO2+2000 ppm SO2, as evidenced product ( A, 400-600 µm)
by the fact that the size change of limestone was insignificant.
The results further confirmed the contribution of the 1
calcination reaction to the fragmentation of 0.9
limestone
limestone. 0.8
Fragmentation(ds=336 m)
Attrition (ds=313 m)
0.7
Effect of the Sulfation on Attrition of Limestone
Cumulative mass
0.6
0.5
The degree of (secondary) fragmentation that can 0.4
be attributed to sulphation processes other than 0.3
calcinations and rapid gas release is trivial. Thus, 0.2
comminution of lime and its sulphate products is 0.1
mainly attributed to attrition by abrasion [6]. 0
Attrition by abrasion generates fine particles that are 0 100 200 300 400 500 600
particle size( m)
quickly elutriated by the high fluidizing gas velocity Figure 10. PSD comparisons of attrition
and collected by the cyclone at the outlet of furnace. and fragmentation product (A, 400-600µm)
The average size of the product remaining in the
6
reactor after the attrition process is finer than with the primary fragmentation product,
except for particle 450 m as shown in Figure 10. In this study, the attrition process
lasted for about 150 minutes at a temperature of 850°C and a fluidizing velocity of 0.5
m/s in the FB reactor.
Figure 11 shows the change of Ka for limestone A with three initial particle sizes. Ka is
found to decay exponentially with time, and then approaches a constant (K ).
Regardless of the initial value of Ka for limestone, finer limestone samples less than
400 m eventually have a higher K . The attrition rate constant of K for particles
larger than 400 m shows small difference. Finer particles have a larger specific
surface area for the same inventory and may experience more abrasion.
1.2E-04 2.5E-05
200-400 m Air
1.0E-04 2.0E-05
400-600 m 800ppmSO2
8.0E-05 600-800 m 2000ppmSO2

1.5E-05
K (m-1)
Ka(m-1)
6.0E-05
1.0E-05
4.0E-05
5.0E-06
2.0E-05
0.0E+00 0.0E+00
0 20 40 60 80 100 200-400 400-600 600-800
time (min) limestone particle size( m)
Figure 11. Change of attrition rate constant of Figure 12. Attrition rate constant K
limestone A (air atmosphere) of limestone A
The influence of sulfation on the attrition of limestone and its products was shown in
Figure 12 for limestone sample A. After the limestone was calcined in the FB for ten
minutes under an air atmosphere, the fluidizing gas was switched to a mixture of air
and SO2. The attrition rate of the sample under an SO2 atmosphere was found to
exhibit a trend that was similar to that under an air atmosphere in size effect up to a
factor of 2. Similar to other studies [6,8], the higher SO2 concentration produces lower
K due to more attrition resistant.
CONCLUSION
Two limestone samples were selected and tested in a bench-scale bubbling fluidized
bed reactor under various conditions to study the limestone fragmentation and
attrition. Experimental results confirmed that fragmentation and attrition could be
significantly affected by limestone type, initial size, heating rate, fluidizing media, and
temperature. The average size of the particles decreased during the fragmentation
process. The heating rate and mechanical collision in the FB have been found to
enhance the fragmentation, while the temperature seems to have negative effect on
fragmentation. Sulfation reactions suppress the fragmentation of limestone due to
the gas diffusion resistance of the CaSO3/CaSO4 layer. The layer of CaSO3/CaSO4
surface is attrition resistant. The sulfation reaction leads to a smaller attrition rate of
limestone products under an SO2 atmosphere than under an air atmosphere.
ACKNOWLEDGEMENT
Financial support of this work by Alstom is gratefully acknowledged.
7
NOTATION
Ug gas superficial velocity in tube, ms-1 Ra attrition rate, kgs-1

-1
Ka attrition rate constant, m K final attrition rate constant, m-1
do average Sauter mean diameter of the original PSD, µm
df average Sauter mean diameter of the new PSD, µm
REFERENCES
1. D. Merrick, J. Highley, Particle size reduction and elutriation in a fluidized bed

process, AIChE Symposium Series, 137 (1974) 366-378.
2. R. Chandran, J. Duqum, Attrition characteristics relevant for fluidized-bed
combustion, in: J. Grace, L. Shemile, M. Bergougnou (Eds.), Fluidization VI,
3. M. Couturier, I. Karidio, F. Steward, Study on the rate of breakage of various
Canadian limestones in a circulating transport reactor, in: A. Avidan (Eds.),
Circulating Fluidized Bed Technology IV, 1993, pp.672-680.
4. I. Karidio, Sulfation and breakage characterization of various Canadian
limestones, University of New Brunswick, Canada, PhD Thesis, 1994
5. N. Hu, A.W. Scaroni, Fragmentation of Calcium-based Sorbents under High
Heating Rate, Short Residence Time Conditions, Fuel, 74 (1995) 374-382.
6. F. Scala, A. Cammarota, R. Chirone, et al., Comminution of limestone during
batch fluidized-bed calcination and sulfation, AIChE Journal, 43 (1997) 363–73.
7. A. Benedetto, P. Salatino P. Modelling attrition of limestone during calcination
and sulfation in a fluidized bed reactor, Powder Technology, 95 (1998) 119–28.
8. F. Scala, P. Bareschino, R. Boerefijn, et al., Attrition of sorbents during fluidized
bed calcination and sulfation, Powder Technology, 107 (2000) 153-167.
9. F. Scala, F. Montagnaro, P. Salatino, Sulfation of Limestones in a Fluidized Bed
Combustor: The Relationship between Particle Attrition and Microstructure,
Canadian Journal of Chemical Engineering, 86 (2008) 347-355.
10. J .Wang, S. Li and H. Yang, et al., Study of the Explosive Cracking and Wear
Characteristics of Limestone, Journal of Engineering for Thermal Energy &
Power, 21 (2006) 366-369 (In Chinese).
11. F. Scala, P. Salatino, The Influence of Sorbent Properties and Reaction
Conditions on Attrition of Limestone by Impact Load in Fluidized Beds, The
Proceedings of the 20th FBC Conference, Xi’an China, 2009, 486-491.
12. F. Montagnaro, P. Salatino, F. Scala, M. Urciuolo, Sorbent Inventory and Particle
Size Distribution in Air-blown Circulating Fluidized Bed Combustors: The
influence of Particle Attrition and Fragmentation, The Proceedings of the 20th
FBC Conference, Xi’an China, 2009, 696-671.
13. F. Scala, F. Montagnaro, P. Salatino, Attrition of Limestone by Impact Loading in
Fluidized Beds, Energy and Fuels, 21 (2007) 2566–2572.
14. F. Montagnaro, P. Salatino, F. Scala. The influence of temperature on limestone
sulfation and attrition under fluidized bed combustion conditions, Experimental
Thermal and Fluid Science, 34 (2010) 352–358.
15. Xuan Y, Hai. Zhang, Hairui Yang, et al. An experimental study on the primary
fragmentation and attrition of limestones in a fluidized bed, Fuel Processing
Technology, 91 (2010) 1119–1124.
16. G. Hu, Kim Dam-Johansen, Stig Wedel, et al., Review of the direct sulfation
reaction of limestone, Progress in Energy and Combustion Science, 32 (2006)
386-407.
8
HYDRODYNAMICS OF A CLUSTER DESCENDING AT THE
WALL OF A CFB RISER: NUMERICAL STUDY
Subhashini Vashisth and John R. Grace
Department of Chemical and Biological Engineering,
University of British Columbia, 2360 East Mall, Vancouver, Canada V6T 1Z3
ABSTRACT
The incompressible hydrodynamics of a single parabolic cluster descending at
the wall of a CFB riser was numerically simulated using a 2-D Eulerian-Granular
model and a segregated time-dependent unsteady solver. Numerical predictions
of the velocity of descent and the evolution of cluster shape are in reasonable
agreement with experimental results available in the literature.
INTRODUCTION
Clustering of particles is an important feature observed in CFB risers. Grace and

Tuot (1) showed that vertical flow of homogeneous particle suspensions is
unstable, causing the particles to gather in ‘clusters’, ‘strands’ or ‘packets’, mostly
falling down along the riser wall (2,3). The frequent formation, descent and
dissolution of clusters causes axial dispersion of particles and gas, thereby
having a negative impact on the performance of CFB catalytic and gas-solid
reactions. Clustering also strongly influences particle holdup and pressure drop
(4). In order to understand cluster dynamics, several researchers (e.g. 5, 6) have
measured the velocity of descent of particle clusters near the wall of CFB risers.
Except for very large risers, the descent velocities have almost always been
found to be between 0.3 to 2.0 m/s, despite wide variations in operating
conditions. Experimental investigations have also been reported on flow
characterization of clusters (7, 8, 9), cluster porosity, cluster occurrence
frequency, as well as cluster residence time and size (10, 11, 12). Despite
significant advances in the visualization of flow, there is no clear definition of
cluster shape. Yerushalmi (13) adopted the terms “streamers”, “strands” and
“ribbons”. Rhodes et al. (14) described clusters as `swarms or `strands,
depending on their shape and the operating conditions. Elliptical or ellipsoidal
frontal shapes were observed by Lim et al. (6). Similarly, rounded-bottom
assemblies descending near the riser wall were captured by the infrared images
of Noymer and Glicksman (11). Even though the clusters are far from spherical in
shape, some researchers (e.g. 15) have approximated clusters as spheres in
order to simplify the analysis of gas flow around clusters.
Considering possible shapes of clusters, it seems reasonable from the existing

information to assume aerodynamic bluff bodies. In the present work we have
attempted to investigate a single cluster which, based on the experimental
observations of Zhou et al. (5), is initially parabolic in shape. The leading edge of
the descending cluster is assumed to be similar to that of a large liquid drop (6).
A two-dimensional computational fluid dynamic model employing the Eulerian-
granular model is used to simulate the behaviour of clusters. Numerical
simulations based on the commercial CFD code solver, Ansys-Fluent 12.1, were
carried out and are compared with the experimental results of Zhou et al. (5) and
Lim et al. (6).
EULERIAN-GRANULAR GAS-SOLID FLOW MODEL
The gas-solid two-phase incompressible flow is modeled in an Eulerian-Granular

framework, with the Syamlal-O’Brien (16) drag model employed for interphase
momentum exchange. The solid phase stress was computed from the kinetic
theory of granular flow. A laminar viscous model was assumed. External forces,
lift and virtual mass forces were neglected. For the sake of brevity, the model
equations are not presented here. Instead, the complete set of governing
equations may be obtained from the manuals of Ansys-Fluent 12.1 (17). Table 1
specifies the granular parameters for the riser flow simulations. The value of the
granular temperature was adopted from the literature (17, 18). Its value was kept
constant as the core region of the riser was very dilute compared to the cluster.
Hence, random fluctuations were neglected. Incorporation of an appropriate
turbulence model and effect of varying the granular temperature will be
considered in future work.
MODEL SET-UP AND NUMERICAL SOLUTION PROCEDURE
The CFB riser geometry and grid were created using Ansys-Workbench 12.1.
The primary objective of the present work was to simulate the descent of an
initially parabolic-shaped cluster of width Dc in a two-dimensional calculation
region. Key parameters are listed in Table 2. Air and particles are fed into the
riser from the bottom at a specified superficial gas velocity and at a given mass
flux, respectively. Both particles and air leave the riser at the top. Initially, the
riser was completely filled with air, and then the solids were introduced. At t = 0 s,
the cluster was initiated. QUICK and second-order upwind differences were used
to discretize the continuity and momentum equations respectively, whereas time
was second-order implicitly discretized. The Phase-Coupled SIMPLE algorithm
was used for pressure-velocity coupling. Each case was simulated for 1.5 s. The
velocity of descent of each cluster was calculated as a mass-weighted-average
velocity over all of the particles which initially belonged to the cluster, i.e.
 n   n 
U cl =  ∑ ε pi ρ pU pi  /  ∑ ε pi ρ p 
 i =1   i =1 
Boundary Conditions:
Uniform-velocity inlet conditions were imposed:
Ug,y =Ug; Ug,x = 0 ; Up,y =Up; Up,x = 0
At the outlet: ∂U g , y / ∂y = ∂U g , x / ∂y = 0
No slip was imposed on the gas velocity at both side walls: Ug = 0
Transient simulations with a time step of 0.0001 s were carried out based on the
governing equations and boundary conditions until steady state was obtained. In
order to accurately account for the motion of clusters at the wall, refined grid
spacing was used near the wall. Sensitivity to the grid spacing and time step
were checked in the initial numerical experiments. The numerical computations
were confirmed to be converged by checking the time-averaged mass residual
(<10−4) at different planes along the height of the riser. Simulation experiments
were performed for 25 x 80 (width x height), 36 x 100 and 60 x 200 mesh
resolutions and compared with the experimental results of Zhou et al. (5). This
comparison showed that the 36 x 100 grid (with a time step of 0.0001 s) was able
to provide mesh-independent results, as shown in Figure 1. This mesh was then
adopted for further parametric studies.
Experimental investigations of particle velocity profiles and motion of clusters

near the wall of a 146 mm x 146 mm square by 9.14 m tall riser conducted by
Zhou et al. (5) and Lim et al. (6) were compared with the CFD predictions. As
can be seen from Figure 1, the air and particle velocity distributions were
predicted reasonably well.
The particles inside the riser are not uniformly distributed, despite the imposed
uniformity at the inlet. The clusters are characterised by local high particle
concentration. The predicted spatial-temporal structure of clusters depends on
the local velocities and concentrations of both gas and solids. Figure 2 shows
predicted contours of particle volume fraction at various times for Ug = 5.5 m/s
and Gs = 20 kg/m2.s. A section of the riser is shown with a cluster at the wall. At
t = 0.05 s, the volume fraction at the core of the cluster is 0.335, decreasing to
0.035 on its outer surface, and further to 0.029 at the centre of the riser. The
cluster is predicted to descend along the wall of the riser and to deform under the
influence of gravity and drag due to the upward flow of gas and solids. After t =
0.4 s, the outer surface of the cluster is pulled upwards, while the core maintains
a drop-like elongated shape. The cluster is predicted to become more and more
dilute with time as it expands, but it still keeps itself intact as a cluster, in practice
probably influenced by inter-particle forces (20). The influence of frictional forces
was neglected in this study. At t = 0.7 s, a petal-like shape was observed, after
which the cluster starts to recede to a parabolic-drop shape, before detaching
from the wall at t ≈ 0.8 s. Similar shape evolution was predicted for other gas
velocities and solid mass fractions.
The descent velocities of clusters for different gas velocities and solid mass
fluxes are plotted in Figure 3 as a function of time. These velocities are predicted
to be in the range of 0.1 to 2 m/s, in accordance with experimental values (e.g. 5,
6). The cluster velocity increases with time as the cluster descends from rest,
before detaching from the wall. Increasing either the superficial air velocity or the
solid mass flux in the upward direction increases the drag resistance on the
descending cluster, thereby reducing its velocity of descent. Moreover, clusters
are predicted to detach earlier with increasing upward suspension velocities and
solids fluxes.
The predicted particle concentration profiles at and near the left wall as a function
of time in Figure 4 show higher particle concentration near the wall, falling as the
centre of the riser is approached. Similar observations were reported by Manyele
et al. (12) and Li Huilin et al. (21). The present model correctly predicts the trend
of particle concentrations. As time progresses, their concentration drops from
0.48 at t = 0 s to 0.054 at t = 0.7 s, while descending from a cluster mid-point
coordinate, z, of 0.9 m to z = 0.2 m, respectively. It is evident that considerable
dilution of the cluster is predicted to take place. Note that the present model
does not take inter-particle forces into account, which may in practice help to
keep clusters intact (20). The change in cluster voidage did not greatly affect the
evolution of cluster shape.
Figures 5(a) and (b) show average lateral distributions of gas and particle
velocities at various times. The particle motion closely follows the upward-flowing
carrier gas in the centre, but, near the left wall, particles were observed to
descend. Hence, both graphs can be divided into two regions: (a) Region I,
distance from left wall < 0.05 m (presence of cluster at wall) and, (b) Region II,
distance from left wall > 0.05 m (towards the center of the riser). It was observed
that with increasing time, the velocity profiles for both gas and solids approach
symmetry at the centre.
Figure 6 shows the lateral variation of cluster width for Ug = 5.5 m/s and varying
solids flux. Initially centered at height, z = 0.9 m above the inlet, clusters at the
wall were considered with an initial width of 30 mm. As a cluster descends along
the wall, its maximum width progressively increases and reaches nearly 120 mm
at z = 0.2 m. Beyond this point, the cluster detaches from the wall and is large
enough to either fall down or be entrained by the incoming gas. Similar
monotonically increasing cluster dimensions were observed for different inlet
solid mass fluxes. Mostoufi and Chaouki (22) and Li Huilin et al. (21) found a
similar trend from their experimental and numerical investigations, respectively.
Figure 7 shows the cluster velocity of descent as a function of initial cluster width.
Simulations were first carried out for widths of 22.2, 26.6, 28.1, 30.0 and 35.6
mm. Both the experimental data (6) and CFD predictions were observed to
fluctuate. Interestingly, the predicted data followed a similar trend to the
experimental results. When further simulations were conducted for widths of
19.9, 21.0, 23.4 and 31.9 mm, the model captured the experimental trend
reasonably well. It is recommended that further investigations be carried out to
understand the reasons for the fluctuations.
Figures 8(a) and (b) plot the velocity of descent of a cluster as a function of
superficial gas velocity and solid mass flux rate. As the gas velocity and solid flux
increase, there is little variation in the predicted descent velocity of the clusters.
However, descending clusters experience some drag resistance owing to the
rapid upward suspension flow, and hence a small decrease in cluster descending
velocity is observed. Similar observations were made by Zhou et al. (5), Lim et
al. (6) and Noymer (23).
NOTATION
Dc width of the cluster [mm]

dp particle diameter [µm]
Gs solid mass flux [kg/m2.s]
Ucl cluster descent velocity [m/s]
Ug gas superficial velocity [m/s]
Up particle velocity [m/s]
t time [s]
z height of the riser [m]
ε solid volume fraction [-]
ρ density [kg/m3]
CONCLUSIONS
A gas-solid Eulerian-Granular CFD model was developed to predict the motion of

initially parabolic-drop-shaped clusters at the wall of a CFB riser. The predicted
velocity of cluster descent is in reasonable agreement with experimental data of
Zhou et al. (6) and Lim et al. (7). Clusters are predicted to distort while
descending, from parabolic to drop-shape to petal and back to parabolic, before
detaching from the wall. They also increase in size and become more dilute as
they accelerate from rest while descending. The present model can be refined in
the future by incorporating such additional features as frictional forces, turbulence
and interactions between multiple clusters.
REFERENCES
[1] Grace, J.R. and Tuot, J.A., 1979. A theory for cluster formation in vertically
conveyed suspension of intermediate density Trans. Int. Chem. Eng., 57, 49–
54.
[2] Yerushalmi, R.G.J., Cankurt, N.T., Geldart, D., Liss, B., 1978. Flow regimes
in vertical gas– solid contact systems, AIChE Symp. 74, 1–13.
[3] Chen, C.J., 1999. Experiments that address phenomenological issues in fast
fluidization, Chem. Eng. Sci. 54, 5529–5539.
[4] Guenther, C. and R. Breault, R., 2007. Wavelet Analysis to Characterize.
Cluster Dynamics in a Circulating Fluidized Beds, Powder Technol., 2007;
173, 163–173.
[5] Zhou, J., Grace, J.R., Lim, C.J., Brereton, C.M.H., 1995. Particle velocity
profiles in a circulating fluidized red riser of square cross-section, Chem.
Eng. Sci., 50 (2), 237-244, 1995.
[6] Lim, K.S., Zhou, J., Finley, C., Grace, J.R., Lim, C. J., & Brereton, C. M. H.,
1997. Cluster descending velocity at the wall of circulating fluidized bed
risers. Proceedings of the fifth international conference on circulating
fluidized beds. Beijing, People’s Republic of China.
[7] Horio, M. and Kuroki, H., 1994. Three-dimensional flow visualization of dilutely
dispersed solids in bubbling and circulating fluidized beds, Chem. Eng. Sci.
49, 2413–2421.
[8] Soong,C.H., Tuzla,K., Chen, J.C., 1995. Experimental determination of
clusters size and velocity in circulating fluidized beds, in: J.F. Large, C.
Laguerie (Eds.), Fluidization VIII, AIChE, New York, pp. 219–227.
[9] Sharma, A.K., Tuzla, K., Matsen, J., Chen, J.C., 2000. Parametric effects of
particle size and gas velocity on cluster characteristics in fast fluidized beds,
Powder Technol. 111, 114–122.
[10] Moortel, V.D., Azario,E., Santini, R., Tadrist, L.1998. Experimental analysis
of the gas particle flow in a circulating fluidized bed using a phase Doppler
particle analyzer, Chem. Eng. Sci. 53, 1883–1899.
[11] Noymer, P.D., Glicksman, L.R., 1998. Cluster motion and particle-convective
heat transfer at the wall of a circulating fluidized bed, Int. J. Heat Mass
Transfer 41, 147–158.
[12] Manyele, S.V., Parssinen, J.H., Zhu, J.X., 2002. Characterizing particle
aggregates in a high-density and high-flux CFB riser, Chem. Eng. J. 88, 151–
161.
[13] Yerushalmi, R.G.J., Turner, D.H., Squires, A.M., 1976. Ind. Eng. Chem.
Process Des. Dev., 15, 47–53.
[14] Rhodes, M., Mineo, H., & Hirama, T., 1992. Particle motion at the wall of a
circulating fluidized bed. Powder Technology, 70, 207-214.
[15] Shuyan, W., Guodong, L., Yanbo, W., Juhui, C., Yongjian, L., Lixin, W.,
2010. Numerical investigation of gas-particle cluster convective heat transfer
in circulating fluidized beds, Int. J. Heat and Mass Transfer, 53, 3102 -2110.
[16] Syamlal, M., Rogers, W., O’Brien, T.J., 1993. MFIX Documentation: Theory
Guide. National Technical Information Service, vol. 1. Springfield, VA,
DOE/METC-9411004, NTIS/DE9400087.
[17] Ansys-Fluent 12.1 Users Guide, Fluent Inc., Lebanon, NH, 2009.
[18] Kuipers, J. A. M., Prins,W., Van Swaaij, W. P. M., 1992. Numerical
calculation of wall-to-bed heat transfer coefficients in gas-fluidized beds,
AIChE J., 38 (7), 1079 – 1091.
[19] Lun, C.K.K., Savage, S.B., Jeffrey, D.J., Chepurniy, N., 1984. Kinetic
theories for granular flow: inelastic particle in Couette flow and slightly
inelastic particles in a general flow field. Journal of Fluid Mechanics 140,
223–256.
[20] Shaffer, F., Gopalan, B., Breault, R., Cocco, R., Hays,R., Karri, R.,
Knowlton, T. A., New View of Riser Flow Fields using High Speed Particle
Imaging, NETL Multiphase Flow Workshop May 4-6, 2010.
[21] Huilin, L., Qiaoqun, S., Yurong, H., Yongli, S., Ding, J., Xiang, L., 2005.
Numerical study of particle cluster flow in risers with cluster-based approach.
Chem. Eng. Sci. 60, 6757-6767.
[22] Mostoufi, N., Chaouki, J., 2004. Flow structure of the solids in gas–solid
fluidized beds. Chem. Eng. Sci. 59, 4217 – 4227.
[23] Noymer, P. D., 1997. Heat transfer by particle convection at the wall of a
circulating fluidized bed. Ph.D. thesis, Massachusetts Institute of Technology,
Cambridge, MA.
Table 1. Kinetic model specifications
Granular temperature, m2/s2 10-5 [17,18]

Granular viscosity, kg/m. s Syamlal-O’Brien (16)
Granular bulk viscosity, kg/m. s Lun et al. (19)
Frictional viscosity, kg/m. s None
Solids pressure , Pa Lun etal. (19)
Radial distribution correction factor for Lun etal. (19)
inter-particle collisions)
Elasticity modulus, Pa Derived (17)
Packing limit, [-] 0.6
Table 2. Parameters used in the CFD simulations
Parameter Value(s)
Height of riser computational domain, m 8, 1.0
Width of riser, m 0.146 and 0.285
Particle diameter, dp, µm 213
Width of cluster, Dc, mm 19.1, 21, 22.2, 23.4, 26.6,
28.1, 30.2, 31.9 and 35.6
Density of particles, ρp, kg/m3 2640
Inlet solids mass flux, Gs, kg/m2.s 10, 20, 30, 40 and 60
Superficial gas velocity, Ug, m/s 4.5, 5.5, 6, 7 and 8
Particle-particle coefficient of restitution, [-] 0.95
Volume fraction of particles in cluster, [-] 0.48 (base case)
0.0
Gs = 20 kg/m2.s Zhou et al. (1995) Gs = 40 kg/m2.s Zhou et al. (1995) Gs = 40 kg/m2.s Zhou et al. (1995)
-0.4 25 x 80
Ug = 5.5 m/s 25 x 80 Ug = 5.5 m/s 25 x 80 Ug = 7 m/s
30 x 100 30 x 100 30 x 100
-0.8 60 x 200
60 x 200 60 x 200
Particle velocity [m/s]
-1.2
-1.6
-2.0
-2.4
-2.8
-3.2
0.00 0.04 0.08 0.12 0.00 0.04 0.08 0.12 0.00 0.04 0.08 0.12
Distance from left wall [m] Distance from left wall [m] Distance from left wall [m]
(a) (b) (c)
Figure 1. Grid independent test: Lateral profiles of particle velocities for Dcl = 30 mm, dp = 213 µm,
z= 6.2 m, t = 5.2 s]
0.029
0.035
0.007
0.02
0.335 0.011
0.218
0.144
0.478
z = 0. 88 m z = 0. 7 m z = 0. 6 m
z = 0. 9 m
(a) t = 0 s (b) t = 0.05 s ( c) t = 0.3 s (d) t = 0.4 s
0.005 0.003
0.004
0.008
0.024
0.034
0.106 0.025
z = 0. 5 m z = 0. 3 m z = 0. 25 m z = 0. 2 m
(e) t = 0.5 s (f) t = 0.7 s (g) t = 0.75 s (h) t = 0.8 s

2
Figure 2. Volume fraction of particles at instantaneous time, Gs = 10 kg/m .s; Ug = 5.5 m/s; Dcl = 30 mm
Gs = 20 Kg/m2.s
0.5 Ug = 5.5 m/s
2.0
Dcl = 30 mm
Particle volume fraction [-]
0.4 t=0s
1.5 t = 0.05 s
t = 0.1 s
0.3 t = 0.2 s
Ucl [m/s]
t = 0.3 s
1.0
t = 0.4 s
0.2 t = 0.5 s
t = 0.6 s
0.5 Gs (kg/m2.s) Ug (m/s) t = 0.7 s
10 5.5 0.1
60 5.5
20 8
0.0 0.0
0.0 0.1 0.2 0.3 0.4 0.5 0.6 0.7 0.8 0.00 0.01 0.02 0.03 0.04 0.05 0.06
Time [s]
Distance from the left wall [m]
Figure 3. Descent velocity of cluster Figure 4. Lateral profile of particle
versus time with varying Ug and Gs concentration at and near left wall
4.0
8 3.5
7 3.0
2.5
6 2.0
Particle velocity [m/s]

Air Velocity [m/s]
1.5
5
1.0
4 0.5
0.0
3
-0.5
2 -1.0
Gs= 10 kg/m2.s t = 0.05 s Gs= 10 kg/m2.s t = 0.05 s
t = 0.4 s -1.5
1 t = 0.4 s
Ug = 5.5 m/s t = 0.7 s -2.0 Ug = 5.5 m/s t = 0.7 s
0 -2.5
0.00 0.05 0.10 0.15 0.20 0.25 0.00 0.05 0.10 0.15 0.20 0.25
Distance from left wall [m] Distance from left wall [m]
(a) (b)
Figure 5. Lateral distributions of (a) Gas velocity and, (b) Particle velocity at z = 0.5 m, Dcl = 30 mm
1.0 1.6
Ug = 5.5 m/s Gs = 40 kg/m2.s
0.9 Lim et al. (1997)
Gs = 30 kg/m2.s 1.4 Predicted
0.8 Gs = 20 kg/m2.s
0.7 1.2
Height [m]
0.6
Ucl [m/s]
0.5
1.0
0.4
0.8
0.3
0.2 0.6
0.1
20 40 60 80 100 120 140 16 20 24 28 32 36
Maximum width of cluster [mm] Maximum width of cluster, Dcl [mm]
Figure 7. Comparison of predicted cluster

Figure 6. Variation of maximum width of cluster descent velocity with experimental data of Lim
versus height of riser et al. (1997) including 15% error bars,
2
Gs = 10 kg/m .s, Ug = 5.5 m/s.
1.12
1.1 Ug = 5.5 m/s; Dcl = 30 mm
1.10
1.08
1.0
Ucl [m/s]
Ucl [m/s]
1.06
1.04
0.9
1.02
2
Gs=20 kg/m .s ; Dcl = 30 mm
1.00
0.8
4.0 4.5 5.0 5.5 6.0 6.5 7.0 7.5 8.0 8.5 10 20 30 40 50 60
Gas Velocity, Ug [m/s] Solid mass fraction, Gs [kg/m2.s]
(a) (b)
Figure 8. Variation of cluster velocity as a function of (a) Gas velocity and, (b) Solid mass flux at
z = 0.5 m
DESIGN CRITERIA OF UNIFLOW CYCLONES FOR THE
SEPARATION OF SOLID PARTICLES FROM GASES
Ulrich Muschelknautz, Paul Pattis, Michael Reinalter, Michael Kraxner
MCI Management Center Innsbruck
Egger-Lienz-Str. 120, A-6020 Innsbruck, AUSTRIA
ABSTRACT
The main advantages of uniflow cyclones compared to standard reverse flow

cyclones are their compact design and their capability of being easily integrated into
pipelines. Experiments show that a 0.2m-diameter horizontal uniflow cyclone re-
moves 88.6% of 2 g/m3 of fine mineral powder (d10=3 m, d50=20 m) from 1000 m3/h
air at a pressure loss of 2510 Pa (0.364 psi).
INTRODUCTION
Uniflow cyclones for the separation of

particles from gases have solids and
gas passing through them in only one
direction, Fig. 1, left. At the pipe
entrance a rotational flow is generated
by curved blades. Subsequently the
particles are moved towards the pipe
wall due to the centrifugal force. At the
end of the separation chamber the
particles are discharged through an
opening in the wall. The clean gas
leaves the separator through a central
gas outlet pipe. The main difference to
the standard reverse flow cyclone Fig, 1. Uniflow cyclone (left) and standard
(Fig. 1, right) is, that in a uniflow reverse flow cyclone (right).
cyclone the gas flow does not reverse.
This property leads to several essential advantages of uniflow cyclones compared to
standard reverse flow cyclones:
Easy installation into pipelines
Much smaller volume (diameter and length) needed for cleaning a given gas
volume flow rate at a given pressure loss, i.e. at a given energy consumption
Short residence time of the gas
1
Applications of uniflow cyclones are amongst others
dust removal from gases on compact space
pre-separation of particles from process gases in order to vastly increase the
operation time of subsequent filters
combustion and melting processes in metallurgy (Weng (1))
short-contact time reaction processes (Gauthier et al. (2, 3))
Approved design criteria as well as calculation models for uniflow cyclones, which
are valid for a wide range of applications, are missing up to now. Progress has been
made for a few special applications:
Baluev and Troyankin (4, 5) studied uniflow cyclones for application to combustion
chambers. On the basis of experiments they developed design criteria as well as
calculation formulas for the tangential velocity and the pressure loss.
Gauthier et al. (2, 3) extensively investigated uniflow cyclones for separating catalyst
particles from the process gas of carbon hydrogen cracking. Tests with uniflow
cyclones (diameter DC = 0.05 m) at high solids loadings (above 1wt. solids /wt. gas)
and with glass beads (Sauter diameter of 29 m) showed, that excellent collection
efficiencies require short separator lengths LC/DC of approximately 1.5 and a proper
design below the gas outlet. They showed the strong influence of air humidity on the
separation efficiency.
Experiments of Zhang et al. (6) with horizontal uniflow cyclones (diameter 0.168 m)
at very low crude gas particle concentrations of a few mg/m3 showed that particles
of 10 m can be separated by an efficiency of 90%. Muschelknautz (7) derived
design criteria for vertical uniflow cyclones (diameter 0.292 m) with very low
pressure loss below 2 mbar for collecting coarse particles. Weng (1) developed a
uniform calculation method for the pressure loss of different uniflow cyclone types
(diameter 0.19 m), based on measurements of the gas flow patterns with Laser
Doppler Velocimetry (LDV) and CFD simulations.
Also calculation models for uniflow cyclones have been published (Brunazzi and
Paglianti (8), Tan (9, 10)). Applying these models on measurements at MCI showed
good agreement with the measured overall separation efficiencies. However the
calculated fractional efficiency curves deviated from the measured ones (11).
MCI intends to develop design fundamentals of uniflow cyclones for a wide range of
industrial applications. Extensive studies have been performed at test facilities for
vertical (diameter 0.3m) and horizontal uniflow cyclones (diameters 0.3m and 0.2m).
For vertical cyclones several design parameters have been studied, such as the gas
volume flow rate, the particle size distribution of the feed, the geometries of swirl
vane inserts and of the vortex finder by Würtl (12), and the feed material (steel,
sand, food powders, wolfram, molybdenum and others) by Leitner (13). Foidl (14)
achieved a pressure recovery of 43% by installing swirl vane inserts in the gas
outlet.
Open questions remaining from those investigations were: 1) how re-entrainment of
particles from the dust bunker back into the clean gas can be minimized and 2) how
the geometry of the swirl generator can be improved. Those problems were
investigated at a test facility for horizontal uniflow cyclones (Pattis (15), Reinalter
(16)).
2
EXPERIMENTAL SET UP
Fig. 2 shows the test facility for cyclones with an inner diameter of DC = 192 mm.
Fig. 2. Scheme of the test plant. 1. Injector (1.1 pressurized air), 2.Vibrating feeder (2.1
Potentiometer for mass flow control), 3. Swirl generator, 4. Dust bunker, 5. Filter, 6. Orifice
measuring the gas flow rate, 7. Sound absorber, 8. Compensator, 9. Radial fan.
The solid particles are fed into the gas flow by a hopper, a vibrating feeder (2) and
an injector (1). The gas streams first through a 2 m long inlet pipe in order to
uniformly distribute the gas velocity as well as the particle concentration over the
pipe cross section before entering the cyclone. To allow visual observations the inlet
pipe, the cyclone body and the particle collection chamber are made from Plexiglas.
As test dusts, limestone powders with two different particle size distributions have
been chosen: Carolith 20-R with d10 = 3 m and d50 = 20 m as well as Carolith 0-
0,2 with d10 = 5 m and d50 = 65 m.
The collection efficiency has been determined from the mass of the collected partic-
les mCollected and the mass of the feed mFeed.The fractional efficiency was calculated
from the particle size distributions of the feed Q3,Feed and of the fines Q3,Fines. The
latter has been measured in-line on probes by isokinetic sampling 4 m after the
entrance of the gas outlet. At this position the former swirling flow has already been
transformed into a pure axial flow by a flow straightener and the diameter has been
widened onto 300 mm. Probes at 5 positions distributed over the cross section have
been taken. Q3,Feed has been measured off-line on a probe taken from the hopper.
The cyclone pressure loss p has been measured as the difference of the static
pressures p1 at a position 0.2 m before the swirl generator, and p3 at 1.4 m (i.e. 12
pipe diameters) after the entrance of the gas outlet with diameter 117 mm (Fig. 2).
All tests presented here were performed with a gas flow rate of 1000 m3/h (
30 m 3 /h ) and a solids concentration in the crude gas of 2g/m3 ( 0.08 g/m 3 ).
The variations during one test are shown in brackets. Every test was performed at
least twice. All tests showed that, for a given set of cyclone-geometry and operation
data, the measured separation efficiencies, , deviated from the mean value by a
maximum of 0.5% . In all tests a feed mass of 250 g was used. During all tests the
air humidity was between 25 and 35%, and the temperature between 12 and 18°C.
3
RESULTS
Three uniflow cyclone types have been investigated:

Type 1: Swirl vane inserts (SVI), ring slot for solids discharge (15, 16)
Type 2A: Swirl vane inserts (SVI), window for solids discharge (16)
Type 2B: Spiral (SP) as swirl generator, window for solids discharge (15)
Two swirl vane inserts have been tested: SVI-30° with a vane angle of 30° and SVI-
50° with a vane angle of 50°, measured between the vane line at the core and
normal to the cyclone axis. The vortex finder diameter DVF was in all cases 117mm.
Uniflow cyclone type 1: Swirl vane inserts and ring slot for solids discharge
The swirl generator consists of 6 curved vanes arranged around a cylindrical core,
the solids discharge opening is a ring slot, see Fig. 3.
Fig. 3. Uniflow cyclone with ring-slot shaped solids discharge opening.
Maximum separation efficiencies achieved by this device were:

SVI-30°: = 87.9% at p = 4125 Pa (0.598 psi) for LC/DC = 1, LVF = 0 mm.
SVI-50°: = 82.0% at p = 1860 Pa (0.270 psi) for LC/DC = 1, LVF = 0 mm.
For optimum separation efficiencies a short separator length, LC, between the end of
the swirl generator and the beginning of the discharge opening is required, Fig. 4.
Fig. 4. Performance data of Uniflow Cyclone type 1 as a function of separator length LC

(Carolith 20-R, LVF=0mm).
4
The vortex finder length, LVF, crucially influences the collection efficiency. The
optimum length is LVF=0 mm, see Fig. 4. Sticking the vortex tube into the separation
chamber up to 100 mm (positive values of LVF, see Fig. 3) leads to a small decrease
of by 2%. If LVF<0, then separation passes first a local minimum at LVF=-200mm
and breaks down for LVF<-600mm. The pressure loss depends only weakly on LVF.
Fig. 5. Performance data of Uniflow Cyclone type 1 as a function of vortex finder length LVF
for swirl generator SVI-30° (Carolith 20-R, Lc/Dc = 7).
The collection efficiency depends strongly on the feed’s particle size distribution:
Carolith 20-R (d10 = 3 m, d50 = 20 m) Carolith 0-0.2 (d10 = 5 m , d50 = 65 m)
% 86.7 94.1
p Pa 3651 3420
Table 1: Separation efficiency and pressure loss for different particle size distributions of the
feed (Uniflow Cyclone with SVI-30°, LC/DC = 7, LVF = 150 mm).
Uniflow cyclone type 2: Window for solids discharge
This uniflow cyclone type has a window for the solids discharge in connection with a
rectangular box as dust bunker, similar to that investigated by Zhang (6). Two
variants of this cyclone type have been tested: Variant 2A with swirl vane inserts
(Fig. 6, left) and variant 2B with a spiral (Fig. 6, right) as a swirl generator.
Fig. 6 Uniflow cyclone with window-shaped opening for solids discharge (LB = length of
bunker). Left: Variant 2A with swirl vane inserts (16), right: Variant 2B with spiral (15).
5
The spiral inlet of variant 2B, called SP-40°, is a single vane assembled as a spiral
around a core, with a vane angle of 40° at the spiral core against the normal to the
cyclone axis.
Maximum values for the separation efficiency of variant 2A (without core) were
- SVI-30°: = 90.0 %, p = 4050 Pa (0.587 psi) for LC/DC=4.6, LVF = 400 mm
- SVI-50°: = 82.9 %, p = 1782 Pa (0.258 psi) for LC/DC=3.6, LVF = 400 mm
Best values for the separation efficiencies of variant 2B were
- SP-40°: = 88.6 %, p = 2510 Pa (0.364 psi) for LC/DC=3.6, LVF = 400 mm
If in variant 2A (LVF=400mm) a core is installed, which elongates the swirl vane in-
serts core up to the vortex finder, the separation efficiency decreases with
increasing core length by up to 2%. At a core length of 1000 mm the separation
efficiency for Carolith 20-R decreases to 87.5%, but also the pressure loss
decreases to 3250 Pa.
The separator length LC (see Fig. 6) should again not be too large. The best
performances are obtained for LC/DC = 3 to 5, cf. Fig. 7.
Fig. 7. Performance data of Uniflow Cyclone type 2A (left) and type 2B (right) as a function
of separator length LC for swirl generators SVI-30° and SVI-50° (both types with Carolith 20-
R, LVF = 400 mm, without core).
The vortex finder length LVF (see Fig. 6) has its optimum value at 400 mm (Fig. 8).
Fig. 8. Performance data of Uniflow Cyclone type 2A as a function of vortex finder length L VF
for swirl generator SVI-30° (Carolith 20-R, core length 1000 mm).
6
Influence of the particle size distribution of feed on the cyclone performance:
Carolith 20-R (d10 = 3 m, d50 = 20 m) Carolith 0-0.2 (d10 = 5 m , d50 = 65 m)
% 88.6 96.0
p Pa 2510 2425
Table 2: Cyclone performance of Uniflow Cyclone type 2B, LC/DC = 3.6, LVF = 400 mm.
Fig. 9 shows the fractional separation efficiency F of the uniflow cyclone variant 2B.
The minimum of F may be explained as the result of particle agglomeration.
Fig. 9. Fractional separation efficiency of Uniflow Cyclone type 2B (Lc/Dc =3.6, Carolith 20-R,
= 88.6%, p = 2510 Pa). Dashed curves: Cumulative fractions undersize of feed and fines
(Measurements by Laser Diffraction).
CONCLUSIONS
Compared to standard cyclones, uniflow cyclones are able to clean a given gas
particle flow using a much more compact cyclone body. A spiral as swirl generator
needs much less pressure loss than swirl vane inserts, for the same collection
efficiency. Future studies will be focused on the influence of the solids loading.
ACKNOWLEDGMENT
Financial support from MCI is gratefully acknowledged.
NOTATION
d Particle size ( m)
d50 Particle diameter for 50% cumulative fraction undersize ( m)
d10 Particle diameter for 10% cumulative fraction undersize ( m)
DC Diameter of cyclone (mm)
DVF Diameter of vortex finder (mm)
7
LC Length of separation chamber (mm)
LVF Length of vortex finder (mm)
mcollected Mass of collected particles (g)
mfeed Mass of feed (g)
mfines Mass of fines (g)
Q3,Feed Cumulative volume fraction undersize of feed (%)
Q3,Fines Cumulative volume fraction undersize of fines (%)
Greek:
p Pressure loss (Pa)
Total separation efficiency (%)
F Fractional separation efficiency (%)
REFERENCES
1. Weng M. Experimentelle und numerische Untersuchung von Gleichstrom-

zyklonen. Dissertation, RWTH Aachen University, 2002.
2. Gauthier T.A., Briens C.I., Bergougnou M.A., Galtier P. Uniflow cyclone
efficiency study. Powder Technol. 62, 217-225, 1990.
3. Gauthier T.A., Briens C.I., Crousle O, Galtier P, Bergougnou M.A. Study of
the gas circulation patterns in a uniflow cyclone. Can. J. Chem. Eng. 70, 209-
215, 1992
4. Baluev E. D. and Troyankin Y. V. The effect of design parameters on the
aerodynamics of cyclone chambers. Teploenergetika 14, 67-71, 1967.
5. Troyankin Y. V. and Baluev E. D. The aerodynamic resistance and efficiency
of a cyclone chamber. Teploenergetika 16, 29–32, 1969.
6. Zhang Y., Wang X., Riskowski G.L., Christianson L.L., Ford S.E. Particle
separation efficiency of a uniflow deduster with different types of dust.
Transactions of ASHRAE, 1999.
7. Muschelknautz U. Separation of coarse particles: New Separator with low
pressure drop. Proceedings of CFB-7-Conference, Niagara Falls, 2002.
8. Brunazzi E., Paglianti A. Simplified Design of Axial-Flow Cyclone Mist
Eliminators. AIChE Journal, Vol 49, No. 1, 41-51, 2003.
9. Tan Z. Mechanisms of Particle Separation in an Aerodynamic Air Cleaner.
Department of Agricultural and Biological Engineering, University of Illinois at
Urbana-Champaign, Illinois, 2004.
10. Tan Z. An analytical model for the fractional efficiency of a uniflow cyclone
with tangential inlet. Powder Technology 183, 147-151, 2008.
11. Krimbacher T. Evaluierung von Gleichstromzyklon-Rechenmodellen anhand
von Messdaten. Bachelor Thesis, MCI Innsbruck, 2010.
12. Würtl R. Experimental investigation of uniflow cyclone performance, Diploma
Thesis. MCI Innsbruck, 2007.
13. Leitner A. Einfluss der Staubart auf den Trenngrad eines Gleichstrom-
zyklons. Diploma Thesis, MCI Innsbruck, 2009.
14. Foidl S. Entwicklung von Leitapparaten zur Druckverlustminimierung in
Gleichstromzyklonen. Diploma Thesis, MCI Innsbruck, 2007.
15. Pattis P. Entwicklung eines Gleichstromzyklons mit gezielter Strähnen-
führung. Master Thesis, MCI Innsbruck, 2010.
16. Reinalter M. Minimierung des Partikelwiedereintrages in den Reingasstrom
von Gleichstromzyklonen. Master Thesis, MCI Innsbruck, 2010.
8
UNDERSTANDING STANDPIPE HYDRODYNAMICS USING
ELECTRICAL CAPACITANCE TOMOGRAPHY
Changhua Qui1, Robert Joachim, S.B1. Reddy Karri2,3

1Industrial
Tomography Systems
39 Deangate, Manchester, UK M32BA
2Particulate
Solid Research, Inc.
4201 W 36th Street, Suite 200
Chicago, IL, USA 60632
3Corresponding author (reddy.karri@psrichicago.com)
Tel.: +1 773 523 7227 Fax: +1 773 299 1007
ABSTRACT
Standpipes are often the bottleneck in a circulating fluidized bed processes.

Understanding the pressure build and dissipation in a standpipe is critical in
designing and operating a standpipe that can meet production needs. However, this
critical component of a circulating fluidized bed (CFB) is often neglected in the
design process which usually results in an underperforming unit operation. In an
effort to better design new standpipe and to better optimize existing ones, electrical
capacitance tomography (ECT) was evaluated in a 7-inch (18-cm) diameter
standpipe to understand the gas-solid hydrodynamics in a standpipe with respect to
circulation rates and aeration strategies.
INTRODUCTION
Standpipes are the pressure balance in a circulating fluidized beds. It is the

pressure build and dissipation in a standpipe that determined the maximum
circulation rate or solids flux in a circulating fluidized bed (CFB). How a standpipe is
aerate determined the level of pressure build that can be obtained. For Geldart
Group A powders, uniform aeration is recommended. For Geldart Group B powders,
only aeration near the slide valve is recommended [1]. Even the level of aeration
should be considered as an important operating parameter [2]. Too much, and the
bubbles can defeat any possible pressure build and too little makes the aeration
ineffective.
Yet, how aeration enhances the standpipe pressure build is unclear. Does the
aeration provide a reduction in friction at the wall or does the gas penetration deep
into the standpipe and keeps the solids fluidized or perhaps both? To better
understand how aeration effects solids hydrodynamics in a standpipe, electrical
capacitance tomography (ECT) was installed on an 7-inch (18-cm) diameter
standpipe of circulating fluidized bed cold-flow unit.
EXPERIMENTAL
Standpipe
Tests were conducted in a 8-inch (20-cm) diameter circulating fluidized bed equipped
with a 8-inch (20-cm) diameter standpipe and a 7-inch (18-cm) diameter spool piece
for the ECT electrodes, as shown in Figure 1. The riser was 22-m tall and
terminated with an elbow with an r/D of 1.5 to a 48-cm diameter primary cyclone, a
secondary cyclone, and diplegs to route the solids collected by the cyclones into the
3-ft (0.9-m) diameter fluidized storage hopper. A 20-cm diameter by 16.8-m tall
standpipe returns the solids back to the riser. A 7-inch (18-cm) diameter spool piece
was incorporated into the riser near the slide valve to accommodate the ECT
system. A diverter valve in the first-stage cyclone dipleg allows solids to be diverted
into a collection hopper on load cells so that the solids flow rate can be measured.
The facility operated at ambient temperature and pressure. It can operate at gas
velocities of up to 70 ft/s (21.3 m/s) and at solids fluxes in the riser of 200 lb/s-ft2
(980 kg/s-m2). The unit was filled with equilibrium FCC catalyst powder having a
particle density of 1500 lb/ft3 and median particle size of 72 microns.
Figure 1: Schematic and picture of 8-inch (20-cm) diameter CFB with 7-inch (18-cm)
diameter spool piece for ECT system.
Two trials were conducted, the first test was to establish optimal measurement
parameters; the second was to observe and evaluate the ECT system over a test
matrix of 16 fluidized beds flowing process conditions. These conditions are
presented in Table 1.
Table 1: Experimental design for ECT evaluation in a 7-inch (18-cm) diameter
standpipe.
Solids Flux Aeration Rate
Test Aeration Injection Points
Case
lb/ft2-sec kg/m2-sec SCFH SCMH
1 0 0 30 0.850 All
2 0 0 50 1.416 All
3 5 24 25 0.708 All
4 5 24 20 0.566 All
5 10 49 15 0.425 All
6 28 137 20 0.566 All
All but Increasing Qg from 20-200

7 28 137 20 0.566
@ #9,#10
8 60 294 30 0.850 All
9 50 245 35 0.991 All
All but Qg @ #9 increasing from 40

10 50 245 40 1.133
to 200
11 76 372 35 0.991 All
All but Increasing Qg from 35 up to

12 76 372 35 0.991
200 @ #7,#9
13 115 563 35 0.991 All
All but Increasing Qg from 35 up to

14 115 563 35 0.991
200 @ #7
15 115 563 200 5.664 All
All but decreasing the Qg from 200

16 115 563 200 5.664
down to 40@ #7
Electrical Capacitance Tomography
The tests were performed using an ITS m3000c Electrical Capacitance Tomography
system (ECT). The instrument operates by taking measurements from the multiple
electrodes arranged around a pipe to obtain information on the material(s) within the
pipe by dielectric imaging.
The ITS capacitance sensor was 7-inch (18-cm) internal diameter with 12
electrodes, the PSRI fluidized bed circulation pipe at either side (top and bottom)
was 8-inch (20-cm) diameter. It driven by an m3000c system, - which applies a
voltage to an electrode and measures voltages between this and all other
electrodes. Measurements are repeated rapidly (in approx. 20 ms) until all
combinations have been measured for a single frame of data. Overall, 66
capacitance measurements points are taken per frame. These are combined using
proprietary software to provide a cross-sectional map of the capacitance distribution
through the pipeline. Including on line image processing data is presented at 12 Hz.
The measurements are very sensitive (measuring capacitances in order of pico-

Farads). To ensure data is collected properly high and low thresholds must be taken
with homogeneous material in the sensor. After a number of tests (calibrations), it
was determined that the optimal threshold settings were: the low reference with the
gas filled into the sensor and high reference with the fully packed FCC catalytic
power filled with the sensor during the real time trial tests.
Figure 2: ECT scans for a standpipe at rest with uniform aeration and the slide
valve fully closed (Test Case 1).
Figure 3: ECT scans for a standpipe at a solids flux of 76 lb/ft2-sec (385 kg/m2-
sec) with 35 SCFH (0.991 SCMH) uniform aeration and the slide valve at the 0.5-
inch (1.25-cm) opening position (Test Case 3).
Figure 4: ECT scans for a standpipe at a solids flux of 115 lb/ft2-sec (563 kg/m2-
sec) with 200 SCFH (5.7 SCMH) uniform aeration and the slide valve at the 1.9-
inch (4.8-cm) opening position (Test Case 15).
Figure 2 shows the results of the ECT scan for a 7-inch (18-cm) diameter riser at a
zero solids flux (slide valve was fully closed) with 25 SCFH (0.71 SCMH) uniform
aeration, which corresponds to Test Case 1. Under these conditions, the standpipe
behaved more like a bubbling fluidized bed. The ECT scans started with the startup
of the aeration. The images are plotted on a 32 x 32 grid with 820 pixels within the
circular geometry of the sensor. The lower image of Figure 2, shows 3D
tomographic images in a ‘stack’ of 400 images. This represents a time period of 32
seconds and allows temporal flow features to be observed over this time period. The
ECT scans revealed the expected behavior for a bubbling fluidized bed. Gas
bubbles were clearly resolved in the center of the standpipe with respect to time.
Figure 3 shows the ECT scans for an operating standpipe at a solids flux of 76 lb/ft2-
sec (385 kg/m2-sec) with 35 SCFH (0.991 SCMH) uniform aeration, which
corresponds to Test Case 11. For the results shown in Figure 3, the ECT scans
started with the startup of the standpipe and the aeration. During the next 30
seconds, gas from the aeration ports appeared to from a core-annulus profile with
low concentrations of solids in the center of the standpipe.8
This was an expected profile determined by the ECT scans. The slide valve position
for this test case had only 0.5-inch (1.25-cm) opening and was the limiting factor for
the solids circulation rate. The amount of aeration far exceeded that needed to
enhance the standpipe flow. This resulted in the generation large pockets of gas
flowing up the standpipe.
Opening the slide valve such that it no longer limited the flow, changed the gas-solid
distribution completely, as shown in Figure 4. With the slide valve opened to the 1.9-
inch (4.8-cm) position, solids fluxes increased to 115 lb/ft2-sec (563 lb/m2-sec). As
shown in Figure 4, the aeration gas quickly migrated to the wall, even with the
aeration increased to 200 SCFH (5.7 SCMH).
Thus, it appears that at low solids flow rates in standpipes, bubbles have enough
momentum to push the solids to the wall and generate a core-annulus profile. At
Figure 5: ECT scans for a standpipe at a starting solids flux of 115 lb/ft2-sec (563
kg/m2-sec) with 35 to 200 SCFH (1 to 5.7 SCMH) bottom aeration (Top - Test Case
14) and 200 to 40 SCFH (5.7 to 1.1 SCMH) bottom aeration (Bottom - Test Case
16)and the slide valve at the 1.9-inch (4.8-cm) opening position.
high solids flows, the solids momentum restricts the gas to the walls. In this mode, it
is suspected that the gas may act as a lubricant against the solids shear stress and
friction at the wall and thereby further enhance the standpipe flow and pressure
build. These results are consistent with earlier ECT studies done in a 3-inch (4.6-cm)
diameter standpipe [2]. In addition, PETP studies in a 1-inch and 3-inch (2.5-cm and
4.5-cm) diameter standpipe by Chan et. al. [3] that with good standpipe operation,
the solids flow seemed to dominate the center of the riser as well. They also noted
that velocity distribution of solids is asymmetrical within the standpipes cross-section
with a faster motion away from the aeration point but a slower motion closer to the
aeration point.
Where the aeration comes into the standpipe is equally important. For Geldart
Group A powders, uniform aeration is recommended where as for Geldart Group B
powders, only aeration near the slide valve is recommended [1]. As shown in Figure
5, increasing gas flow from 35 to 200 SCFH (1 to 5.7 SCMH) in only one aeration
port at the bottom of the standpipe resulted in flow instabilities in the standpipe
aeration despite that similar, relatively high levels of aeration were deemed useful for
Test Case 15 shown in Figure 3 for uniform aeartion. Stability was regained when
the aeration was lowered to 40 SCFH (1.1 SCMH). The contrast between the ECT
scanned images between Figures 4 and 5 suggest that for Geldart Group A powders,
too much aeration in one location could lead to a core-annulus profile with low solids
concentration in the center of the riser, indicative of unstable standpipe flow.
CONCLUSIONS
ECT imaging of standpipes appeared to generate expected results and highlighted

the role aeration has on standpipe behavior. Too much aeration or aeration in the
wrong position can lead to the gas migrating to the center of the standpipe and
impede solids circulation rates, and standpipe pressure builds. Well positioned
aeration and the correct levels results in the gas migrating to the wall region and
perhaps reduce solids stress and friction at the wall, which enhances the solids
circulation rates.
REFERENCES
1. Knowlton, T.M.. “Standpipes and return systems” in Fluidization Solids Handling and
Processing (Yang, W-C, ed.) Noyes Publications, NJ (1999) pp. 435-486
2. Srivastava, A., Agrawal, K., Sundaresan, S., Karri, S.B.R., Knowlton, T.M., Dynamics of
gas-particle flow in circulating fluidized beds. Powder Technology, 100 (1998) pp. 173-182.
3. Chan, C.W, Seville, J., Fan X., Baeyens, J., Solid particle motion in a standpipe as
observed by Positron Emission Particle Tracking. Powder Technology 194 (2009) pp.
58-66.

(Ted M. Knowlton, Chair) Proceedings of International

Uploaded by

Copyright:

Available Formats

You might also like

(Ted M. Knowlton, Chair) Proceedings of International

Uploaded by

Document Information

Original Title

Copyright

Available Formats

Share this document

Share or Embed Document

Sharing Options

Did you find this document useful?

Is this content inappropriate?

Copyright:

Available Formats

(Ted M. Knowlton, Chair) Proceedings of International

Uploaded by

Copyright:

Available Formats

PROGRAM

International Conference on Circulating Fluidized Beds and

One-Day Seminar on Fluidization

8:00 - 8:30 am Registration

Activity Program Meeting

Special Poster Session/Social Hour

9:30 - 9:40 am COFFEE BREAK

1-1: Gas Tracer Study in a Non- 2-1: Process Decoupling of Plasma

1-2: Investigation on the Hydrodynamic 2-2 Manufacture of Granular

1-3: Hydrodynamics of a Dual Fluidized 2-3 High-Flux Triple Bed Circulating

1-4: Particle Flow in L-Valves 2-4: Bio-Gasoline from Jatropha Oil:

10:36 - 11:00 am COFFEE BREAK

1-5: A Generalized Flow Diagram for 2-5 Waste Wood Gasification:

1-7: Hydrodynamics of a Loop Seal 2-7: A Pyrolysis Pilot Unit Integrated to

1-10: Cold Model Study on 2-10: Studies on Propane

12:30 - 2:00 pm LUNCH

2:00 - 5:30 pm FREE TIME

3-1: A Modeling Study of Gas 4-1: The Development of a Novel

3-3: Numerical Simulations of a 4-3: Fluid Dynamic Effects of Ring-Type

3-4: High-Resolution Simulations of 4-4: Design Requirements for

3-5: Simulation of Particle-Gas Flow in 4-5: The Influence of Carbon Stripper

3-6: Evaluation of a Lagrangian 4-6: Study of Calcination-Carbonation

3-7: Effect of Wall Boundary Conditions 4-7: Understanding Standpipe

7:30 - 9:15 pm DINNER

POSTER SESSION and SOCIAL HOUR

8:30 - 9:30 am P-2: Electrostatic Phenomena in Fluidized Systems: Present Status of

9:30 - 9:40 am COFFEE BREAK

5-1: Design Criteria of Uniflow 6-1: Experimental Study on the Effects

5-2: Erosion in Second Stage Cyclones: 6-2: Experimental Study on Reforming

5-3: Correlation of the Minimum 6-3: Study of Recarbonation in

10:36 - 11:00 am COFFEE BREAK

5-5: Experiments and Modeling of 6-5: Co-Combustion of Various

5-6: Effect of Gas Bypassing in Deep 6-6: Oxy-Combustion of Different Coals

5-7: Fluidization Behavior in a Gas- 6-7: Effects of Secondary Air Injection

5-8: Particle to Gas Heat Transfer in a 6-8: Gas-Solids Hydrodynamics in a

5-9: Fast Pyrolysis Process 6-9: The Research of CFB Boiler

12:30 - 2:00 pm LUNCH

2:00 - 3:40 pm WORKSHOP A

WORKSHOP B WORKSHOP C WORKSHOP D

7-4: Circulating Fluidized Bed 8-4: Design and Operation of Biomass

7-5: 3D CFD Simulation of Combustion 8-5: Operating Experience and Latest

7-6: Comparison Between 8-6: UOP FCC Innovations Developed

7-7: Hydrodynamics of a Cluster 8-7: Co-Gasification of Biomass and

7:30 - 9:15 pm DINNER

9:15 - 11:00 pm POSTER SESSION and SOCIAL HOUR

10:30 - 11:00 am COFFEE BREAK

9-3: Observation of Flow Regime 10-3: Effect of Temperature Field on the

9-4: Bench-Scale Investigation of 10-4: Effect of Bed Temperature, Fuel

12:30 - 2:00 pm LUNCH

2:00 - 5:30 pm FREE TIME

11-1: Comparison of Entrainment Rate 12-1: Time-Resolved X-Ray

11-5: CFD Modeling of Fluidized Bed 12-5: Description of Pressure

11-6: DEM Study of Fluidized Bed 12-6: Dynamics of Gas-Solids Fluidized

12-7: Dynamic Characteristics of

7:30 – 10:30 pm CONFERENCE DINNER at the High Desert Museum

10:45 - 11:45 pm POSTER SESSION and SOCIAL HOUR

Thursday, May 5, 2011

8:30 am END OF CONFERENCE