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Dynamic Model of Calcium Looping Carbonator Using Alternating Bubbling Beds With Gas Switching
Dynamic Model of Calcium Looping Carbonator Using Alternating Bubbling Beds With Gas Switching
Fuel
journal homepage: www.elsevier.com/locate/fuel
h i g h l i g h t s
a r t i c l e i n f o a b s t r a c t
Article history: Carbon capture and storage (CCS) has been globally gaining popularity as a viable greenhouse gases mit-
Received 29 September 2016 igation strategy throughout the last decade. Calcium looping (CaL) is an emerging technology to capture
Received in revised form 16 June 2017 carbon dioxide from flue gases of fossil fueled power plants exploiting the reversible gas-solid reaction
Accepted 12 July 2017
between the carbon dioxide (CO2) and calcium oxide (CaO) to form calcium carbonate (CaCO3) in a flu-
idized bed. In this paper, the concept of calcium looping application using alternating fluidized beds is
explored as well as a proposed scheme to allow smooth gas switching between reactors using an inter-
Keywords:
mediate third reactor. The latter scheme enables energy saving as well. A dynamic model of a bubbling
Carbon capture
Global warming
bed carbonator, the key reactor in the capture process, is presented. The model incorporates both hydro-
Calcium looping dynamics and chemical kinetics to provide more reliable predictions. The model has been validated with
Fluidized bed experimental results obtained at combustion lab, Mansoura University, Egypt using an atmospheric flu-
idized bed reactor of 10.5 cm inner diameter. The key parameters have been investigated to check for sys-
tem sensitivity. Bed temperature has a non-monotonic effect on CO2 capture efficiency. Maximum CO2
capture efficiency was found to occur around a temperature of 675 °C. Capture efficiency increases with
either decreasing fluidization velocity or increasing bed particle size due to enhanced mass transfer and
increased residence time. These findings almost accord with published data. Also, the average CO2 cap-
ture efficiency was found to increase with increasing static bed height up to a certain limit. Further
increase in bed height doesn’t considerably affect the capture efficiency. The proposed model can be used
as a design tool that would enable the optimization and commercialization of calcium looping.
Ó 2017 Elsevier Ltd. All rights reserved.
http://dx.doi.org/10.1016/j.fuel.2017.07.049
0016-2361/Ó 2017 Elsevier Ltd. All rights reserved.
S. Emad et al. / Fuel 208 (2017) 522–534 523
Nomenclature
the CO2 emissions from polluting the atmosphere. It begins with (900–950 °C respectively, allowing for efficient heat recovery in
the capture of CO2 from fossil fuel combustion or industrial pro- process heating or steam cycle of a power generation system.
cesses. Next, the captured CO2 is compressed and transported via Moreover, CaL can be integrated with cement manufacturing so
ships or pipelines. Finally it is stored in suitable geological forma- that a near zero-waste process can be achieved [5,6].
tions. An overview of different CCS technologies can be found in Hirama et al. [7] patented separation of carbon dioxide from
[3,4]. However, the most critical step in the CCS chain that deter- gases containing it by contacting the gas mixture with metal based
mine the feasibility of a certain technique is the capture step [2]. oxides (e.g. calcium oxide) to form metal carbonate. The metal
One of the promising technologies that has shown some poten- oxide is then regenerated at higher temperatures in a second con-
tial advantages in terms of net efficiency and cost of CO2 avoided tacting zone where heat is supplied. The application of CaL as a
on both lab and pilot scale is carbon dioxide capture by absorp- post-combustion CO2 capture process with dual fluidized bed
tion/regeneration process with calcium oxide, known as calcium was then proposed and applied by Shimizu et al. [8]. Since then,
looping as shown in Fig. 1. Both the carbonation and calcination a lot of research has been done to further analyze and develop
reactions are carried out at high temperatures (600–700 °C and the process [5,9,10]. Moreover, several projects have been estab-
lished to assess its feasibility on both lab and pilot scales [11–14].
Fig. 2 shows two different dual fluidized bed configurations that
can be used in the calcium looping process where heat is supplied
in the calciner by oxyfuel combustion. Most research works have
focused on interconnected fluidized beds with solids circulation
between carbonator and calciner, Fig. 2(a). However, this configu-
ration has three main drawbacks.
First, it requires using circulating fluidized bed with relatively
high inlet gas velocities which increases attrition and diminishes
the possibility of reusing sorbent particles in subsequent cycles.
Second, solids exiting the carbonator may include unreacted cal-
cium oxide particles and solids exiting the calciner may include
calcium carbonate particles which affects the capture efficiency.
Third, plugging can occur in solid circulation lines between the
Fig. 1. Calcium looping process. two reactors. In order to solve these problems, the present work
524 S. Emad et al. / Fuel 208 (2017) 522–534
38000
700 log10 Peq ðatmÞ ¼ 7:079 ð2Þ
4:574 T
600
This heterogeneous carbonation reaction takes place in two
500
sequential stages. First, an initial fast stage controlled by chemical
400 kinetics at reaction surface. The formation of the product layer
300 starts to prevent the unreacted core from contacting the reacting
gas. Then comes a much slower stage controlled by diffusion of
200
gas through the product layer of calcium carbonate. In most indus-
100 trial applications, the diffusion stage is commonly neglected and
0 calcium oxide is considered to reach its maximum conversion at
0 50 100 150 200 the end of the kinetically controlled stage.
Time(s)
The thickness of the product layer formed on the free surface of
Fig. 4. Cooling of reactor B. CaO is an important parameter to indicate the end of the fast reac-
tion stage. Also, the formation and growth of solid product affects
(4) Oxygen is fed to reactor C so that O2 is preheated and fed to the porous structure decreasing the available surface area for reac-
reactor A (with fuel) to continue calcination while reactor C tion. Many researchers investigated the average value for the crit-
cools down to 650 °C. Then, steps 1–4 are repeated with ical CaCO3 product layer thickness [17]. The theory of a critical
reactors A and B are interchanged. product layer thickness has been used extensively to study the
maximum obtainable conversion during carbonation reaction
A simplified mathematical analysis of step 2 is given in [18,19]. However, these studies lack the important effects of oper-
Appendix A. For the base case (discussed later), it is found that step ating temperature on chemical kinetics. They consider that operat-
2 continues about 2 min (Fig. 4) corresponding to 13% average con- ing temperature only determines the equilibrium partial pressure
version of calcium oxide particles in reactor C. Oxygen preheating of carbon dioxide. However, experiments indicate greater role for
during this time has been found to save fuel consumption required temperature in the reaction scenario [20].
for calcination by 2.24%. As stated above, only the fast reaction period is considered for
most practical applications. It is controlled by chemical kinetics.
The grain model for porous solids [21] is adopted here to model
3. Carbonator model description
the gas-solid reaction between CO2 and CaO.
The reaction rate for a gas-solid reaction is usually defined as a
The following assumptions are adopted throughout the follow-
specific reaction rate R, where;
ing model derivation;
dX
1- There are two main phases in the bed: emulsion and bub- R¼ ð3Þ
dtð1 XÞ
bles. Bubbles are free of particles. Clouds and wakes are con-
sidered part of the emulsion. When the reaction is under kinetic control, the specific rate can
2- Gas streams passing through the emulsion, bubble phase, be further expressed in power law form [22];
and freeboard follow a plug-flow regime. R ¼ 56ks ðPCO2 PCO2 ;eq Þn S ð4Þ
3- One-dimensional model, i.e. variations of gas concentrations
occur only in the vertical or axial z direction. Assuming that reaction takes place uniformly on spherical
4- Homogeneous composition of solid particles throughout the grains, the following equation can be used,
bed is assumed. This is justifiable because of the high circu- 3
lation rate in the bed. r
1X ¼ ð5Þ
5- Uniform temperature distribution is assumed throughout r0
the bed due to the higher heat capacities of proposed config- Combining Eqs. (3)-(5) would result in
uration, due to higher bulk solid densities.
6- Thermal equilibrium between flue gases and bed particles dX 5
¼ 56ks S0 ðP CO2 PCO2 ;eq Þn ð1 XÞ3 ð6Þ
takes place in less than 1 cm. So, reaction almost takes place dt
at constant temperature. Sun et al. [22] reported a first-order reaction changing to zero-
7- Heat generation is found to increase gases temperature by order dependence when the CO2 partial pressure exceeded 10 kPa.
175 °C. Hence, carbonator temperature is kept approxi- The kinetic constant can be evaluated using Arrhenius equation;
mately constant via introducing flue gases at a temperature
lower than the predetermined carbonation temperature by E
ks ¼ k0 exp ð7Þ
175 °C. Heat generation compensate for this difference. R:T
Kinetic parameters (k0 and E) are obtained from experimental
3.1. Kinetic model measurements and values reported by Sun et al. [22] are adopted
here.
Carbon capture in carbonator takes place through the exother- Barker [23] reported that the carbonation reaction, presented
mic reaction of calcium oxide with carbon dioxide as follows: by Eq. (1), is far from reversible in practice. The sorption capacity
in the fast reaction stage decreases rapidly with increasing the
CaO þ CO2 ! CaCO3 DH0r ¼ 179:2 kJ=mol ð1Þ
number of calcination–carbonation cycles. Grasa and Abanades
The carbonation reaction is a non-catalytic gas-solid reaction [24] proposed a semi-empirical expression, Eq. (8) to express the
and there exists an equilibrium partial pressure of carbon dioxide sorbent capacity after a large number of complete cycles (up to
526 S. Emad et al. / Fuel 208 (2017) 522–534
500). It is valid for different sorbents and for a wide range of oper- 3.2.3.3. Bed expansion. The fraction of bubble phase in the fluidized
ating conditions. bed (d) is proportional to the fluidization velocity of inlet gas. For
intermediate bubbles, the following expression has been proposed
1
X max;N ¼ þ Xr ð8Þ by Abanades et al. [29]:
1
ð1X r Þ
þkN
u0 umf
d¼ 5umf ub emf
ð16Þ
where k and Xr represent the deactivation constant and the ub þ 4
residual conversion, respectively. It is observed that values of
k ¼ 0:52 and X r ¼ 0:075 fit well with a wide range of sorbents Also, expanded bed height is related to Bubble fraction by Eq.
and conditions [24]. (17)
Hmf
3.2. Hydrodynamic model Heb ¼ ð17Þ
1d
Calcium oxide particles used in practice fall well in the Geldart It can be concluded from Eqs. (12)–(14), (16), and (17), that an
B category. Kunii-Levenspiel model for bubbling bed is widely iterative solution (Fig. 5) is required to evaluate the expanded bed
accepted for its simplicity and reliable results [15]. A bubbling flu- height, bubble size and velocity, and bubble fraction of the flu-
idized bed consists mainly of two phases, bubbles and emulsion. idized bed [30].
Bubbles are lean phase free of solid particles, while emulsion is a
dense phase where solid particles are assumed to be uniformly 3.3. Reactor model
distributed.
Species conservation is applied on both phases of fluidized bed
3.2.1. Minimum fluidization reactor. Assuming no accumulation of gas in control volume, the
The minimum fluidization velocity, umf , may be calculated using rate of outflow should equal the summation of rate of inflow, rate
the following expression [25]; of mass transfer to the control volume and rate of generation by
chemical reaction, Fig. 6.
qg dp umf qffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffi
ffi
Rep;mf ¼ ¼ C 21 þ C 2 Ar C 1 ð9Þ
l o For Emulsion phase, the conservation equation for carbon diox-
ide can be written as follows,
d3p qg ðqs qg Þg
where: Ar ¼ l2
dC e
C 1 and C 2 are constants with values of 27.2 and 0.0408, respec- Ce þ Dz Ae umf ¼ C e Ae umf þ K be ½C b C e Ab Dz
tively as suggested by Grace [26]. dz
Broadhurst and Becker [27] proposed a correlation to estimate RCO2 Ae Dz emf ð18Þ
bed porosity at minimum fluidization conditions, emf , where;
0:021
qg
emf ¼ 0:586/0:72 Ar0:029 ð10Þ
qs
3.2.3.2. Bubble rise velocity. For Bubbles in bubbling bed, the rise
velocity is given by the following equation:
ub ¼ ½u0 umf þ ubr ð13Þ
where ubr is the rise velocity of a single bubble estimated using
the expression reported by Kunii-Levenspiel [15] as follows,
0:5
ubr ¼ 0:711½gdb ð14Þ
The effective superficial gas velocity through the bubble phase
can be defined from the gas balance in a cross section of the bed
where;
u0 ð1 dÞumf
ub ¼ ð15Þ
d Fig. 5. Iterative calculation of hydrodynamic parameters.
S. Emad et al. / Fuel 208 (2017) 522–534 527
dC e K be d emf
¼ ½C b C e RCO2 ð19Þ
dz umf 1 d umf
The last term in Eq. (19) (RCO2 ) is the rate of consumption of CO2
due to chemical reaction and is given by Eq. (20)
" #
mol 1 dNCO2 1 emf qs dX
RCO2 ¼ ¼ ð20Þ
m3gas :s V g dt emf MW s dt
dC b K be
¼ ½C b C e ð22Þ
dz ub
Although time is not a variable in Eq. (22), this equation is also
time-dependent as the CO2 concentration in emulsion phase
depends on reactivity of sorbent, Eq. (21), which varies with time
as stated above.
The average conversion (or conversion ratio), X av g , of sorbent at
any time can be calculated using this following expression:
Z
MW s t 1 xCO2;in
X av g ¼ Q gas;in C CO2;in C CO2;out dt ð23Þ
Ws 0 1 xCO2;out
This should be calculated at the end of each time step and used
to calculate RCO2 ns the following time step.
A common performance parameter used in applications of car-
bon dioxide capture is called CO2 capture efficiency, gcapture . It is
defined as the ratio between the number of moles of captured
CO2 to the number of moles of CO2 entering the carbonator.
obtained values of dX dt
is within acceptable tolerance,
calculations are approved and performance parameters are 4
evaluated. However, if this difference is larger than toler-
ance, time step is reduced and calculations have to be 2
repeated. Note that, if the difference is considerably smaller
than tolerance, solution proceeds with an increased time 0
step to save calculation time.
0 0.1 0.2 0.3 0.4 0.5
4- Steps 1-to-3 are repeated till the end of simulation time Height (m)
span. (b) t = 30 minutes
The apparatus used in this work is a bubbling fluidized-bed Fig. 8. Axial profiles of CO2 mole fraction at different times (T = 650 °C, u0 = 0.8 m/s).
6
16
4
limiting error as ±0.4% of the temperature. A temperature con-
2
troller is used to maintain the bed temperature within the preset 0 1000 2000 3000 4000
temperature range by switching on or switching off the electric
Time (s)
heaters based on the bed-thermocouple signal. Measurement of
gases concentrations has been carried out using KANE455 gas ana- Fig. 10. CO2 exit mole fraction vs. time (T = 650 °C, u0 = 0.8 m/s).
lyzer. The measurement accuracy is ±0.3% for CO2.
The sorbent used is a limestone coming from Jabal al-Tair in
Minya, Egypt. The chemical composition of the used limestone is 80
reported in Table 1. The limestone has a density of 2560 kg/m3
CO 2 capture efficiency (%)
70
and particle size of 0.425–0.600 mm. The corresponding minimum
fluidization velocities are 0.19 m/s and 0.1 m/s at 27 °C and 650 °C 60
bed temperature, respectively.
50
The technique pursued to perform an experimental test may be
described in the following. The fluidization air is preheated before 40
it is delivered through the distributor plate to the bed. Feeding of
air continues until the bed temperature reaches the calcination 30
Model
temperature, 950 °C using electric heaters. During the calcination 20
process CaCO3 converts to CaO by losing CO2 according to the Experiment
reaction, 10
Table 1
Chemical composition of the sorbent (wt%).
80 90
60
70
50
40 60
30 Model at
50
Model
20 Model at
Experiment
40 Model at
10
Experiment at
0 30
0 1000 2000 3000 4000 550 600 650 700 750
Time (s) Temperature (°C)
Fig. 12. Sorbent conversion ratio vs. time (T = 650 °C, u0 = 0.8 m/s). Fig. 14. Average CO2 capture efficiency vs. bed temperature.
attributed to the greater molar volume of the product CaCO3 the reaction (Eq. (6)). From 550 °C to 675 °C, the chemical kinetic
(36.9 cm3/g) compared to that of the reactant CaO (16.9 cm3/g). term is dominant leading to an increase in average efficiency and
Layers of CaCO3 are building up that impede the diffusion of CO2 after that the increasing equilibrium concentration becomes more
inside the particles. For this reason the complete carbonation of dominant resulting in a decrease in average efficiency. An opti-
the particle couldn’t be possible. mum temperature of 675 °C has also been reported by Mostafavi
Comparisons between experimental results and model predic- et al. [33]
tions given in Figs. 10–12 indicate satisfying. Fig. 14 also indicates that decreasing fluidization velocity moves
Parametric studies have been conducted to assess influences of the peak slightly to the left. As fluidization velocity decreases, the
operating parameters on carbonator behavior by evaluating gas molecules have increased residence time in the bed (i.e. have
capture efficiency at different bed temperatures, fluidization veloc- more time to react with solid sorbent) which reduces the effect
ities, particle sizes, and static bed height. of decreased reaction rate at lower temperatures.
Fig. 13 shows the model results at different temperatures from Different fluidization velocities have been tested (from 0.4 to
550 °C to 700 °C. The average capture efficiency versus bed tem- 1.2 m/s) to investigate the effect of hydrodynamics on the reactor,
perature is shown in Fig. 14 along with experimental results. The Fig. 15. It can be observed from Fig. 16 that the average efficiency
maximum average capture efficiency is found to occur around a increases with decreasing the fluidizing velocity due to increased
bed temperature of 675 °C. To understand the existence of such residence time and enhanced mass transfer from bubbles to emul-
an optimum bed temperature, we need to keep in mind that oper- sion. Meanwhile, Kunii and Levenspiel [15] stated that bubbling
ating temperature has two opposing effects. The positive effect is bed starts to switch to slugging when dbm =dbed > 0:6. At a fluidiza-
that increasing temperature enhances the chemical kinetics of tion velocity of 0.4, dbm =dbed 0:36, while at a velocity of 1.2 the
the carbonation reaction (Eq. (7)) and the negative effect is that ratio 0.93 indicating that slugging takes place resulting in poor
increasing temperature also increases the equilibrium concentra- mass transfer.
tion and partial pressure of carbon dioxide which slows down However it should be noted that for the same amount of CO2,
decreasing fluidization velocity would require larger system (e.g.
16
T= 550 Exp. at 550 20
CO2 exit mole fraction (%)
16
T= 675
14
10 T= 700
12
8
10
6 8
6
4
4
2
2
0 0
0 500 1000 1500 2000 2500 3000 3500 4000 0 1000 2000 3000 4000 5000 6000
Time (s) Time (s)
Fig. 13. CO2 exit mole fraction vs. time at different bed temperatures (u0 = 0.8 m/s). Fig. 15. CO2 exit mole fraction at different fluidization velocities (T = 650 °C).
S. Emad et al. / Fuel 208 (2017) 522–534 531
85 100
Model
14 22
H = 0.05 m Hs= 0.15 m
s
CO 2 exit mole fraction (%)
0 2
0 1000 2000 3000 4000 5000 6000 0 3000 6000 9000 12000 15000 18000
Time (s) Time (s)
Fig. 17. CO2 exit mole fraction at different particles sizes (T = 650 °C, u0 = 0.8 m/s). Fig. 19. CO2 Exit mole fraction at different bed heights (T = 650 °C, u0 = 0.8 m/s).
532 S. Emad et al. / Fuel 208 (2017) 522–534
A dynamic model has been presented to evaluate carbon diox- mf LHV gcomb ¼ ms C ps ðT calc T carb Þ þ ms DHr
ide capture using the carbonation reaction between calcium oxide þ mf C pf ðT calc T amb Þ
(from lime) and carbon dioxide. It describes carbonator perfor- þ mf ð1 þ AFÞ C pg ðT calc T gi Þ
mance at different conditions. The model makes a coupling
between hydrodynamics and kinetics to give more realistic ½ms C ps ðT calc T carb Þ þ ms DHr
insights. It can be used to make design choices such as bed sizing mf ¼
ðLHV gcomb C pf ðT calc T amb Þ ð1 þ AFÞ C pg ðT calc T gi ÞÞ
and determine optimum operating conditions that maximize the
capture efficiency. Carbonator model can be integrated with the Without Oxygen preheating;
whole plant simulations to predict thermal efficiency penalties of
the carbon capture process. T gi ¼ T amb ffi 300 K
A novel scheme is proposed to allow smooth gas switching With Oxygen preheating;
between reactors using an intermediate third small reactor. The
"Z Z #
later scheme serves in energy saving as well. The scheme can save 1 t¼t preheat t¼t final
about 2.24% of fuel consumption necessary for calcination process T gi ¼ T preheat dt þ T amb dt
time t¼0 t¼t preheat
by preheating the oxygen required for combustion.
S. Emad et al. / Fuel 208 (2017) 522–534 533
Table 2
Switching time, average CO2 capture efficiency and average sorbent conversion at selected cases (For all; dbed ¼ 10:5 cm;dp ¼ 500 lm and T ¼ 675
C).
dt in 1 xCO2out ijggc.2013.07.014.
! [14] Charitos A, Rodríguez N, Hawthorne C, Alonso M, Zieba M, Arias B, et al.
1 xCO2 Experimental validation of the calcium looping CO2 capture process with two
¼ Q gasin C CO2 C CO2out in
ðB4Þ circulating fluidized bed carbonator reactors. Ind Eng Chem Res
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CBO9781107415324.004.
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