(Edited by Jorge Welti-Chanes, Jorge F. Velez-Rui (BookFi) PDF

Transport Phenomena
in Food Processing
© 2003 by CRC Press LLC

Library of Congress Cataloging-in-Publication Data
Transport phenomena in food processing / edited by Jorge Welti-Chanes, Jorge F. Vélez-Ruiz,

Gustavo V. Barbosa-Cánovas
p. cm.— (Food preservation technology series)
Includes bibliographical references and index.
ISBN 1-56676-993-0 (alk. paper)
1. Food—Effect of heat on. 2. Food industry and trade. I. Welti-Chanes, Jorge. II. Vélez-
Ruiz, Jorge F. III. Barbosa-Cánovas, Gustavo V. IV. Series.
TP371.2.T73 2002
664—dc21 2002073736
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Series Preface
Transport phenomena is one of food process engineering’s most important pillars,
and this new addition to the CRC Food Preservation Technology Series offers a
sound combination of the fundamental and applied aspects of this classic engineering
topic. Transport Phenomena in Food Processing plays an important role in the series
because it offers the tools for quantifying many important operations, classic or
novel, using state-of-the-art calculation approaches.
I am particularly impressed with the analytical depth of the chapters and the
wide spectrum of covered topics. For me, this is a very inspiring book that hopefully
will become a key reference. This book is also important because it is the first in
the CRC series to cover fundamental aspects of food processing. In short, I anticipate
that this book will be in good company with upcoming books in the series on other
fundamental aspects of food preservation.

Preface
The latest applications of new and improved traditional food preservation processes
have generated the need for increased knowledge of the phenomenological and
engineering principles that are the basis of the correct application of factors that
produce stability and maintain the quality of transformed and processed products.
This need for knowledge has given the field of food engineering a new identity at
both the research and industrial levels. Understanding the transport phenomena that
govern the engineering analysis and design of food preservation processes is a key
element in improving processing conditions and the employment of energy resources,
and to increasing the quality of the product.
This book presents the state of the art in the transport phenomena area as applied
to food preservation and transformation. It is divided into four sections containing
a total of 33 chapters, each written by prestigious scientists from institutions and
universities around the world. The first section reviews the fundamental concepts of
mass, heat, and momentum transfer, while the remaining three sections discuss
specific applications for a large variety of processes and products where the pre-
dominant transfer phenomenon is mass or heat, or processes employing more than
one transport mechanism.
The mass transfer section focuses on phenomena controlling osmotic dehy-
dration and hot-air drying processes. However, the themes related to water transfer
in superficial films placed on foods, and pre-evaporation, ultrasound, and spinning
cone columns are also included. The seven chapters that constitute the heat transfer
section study the effects of product shape and process equipment on the phenome-
non’s efficiency. The chapters in the last section deal with the study of the combination
of two or three transfer phenomena in frying, sterilization, and drying processes.
We trust this book on transport phenomena will make a meaningful contribution
in facilitating the understanding, design, and implementation of food processing unit
operations that will result in the production of safer, higher quality, and more
convenient foods.
Jorge Welti-Chanes
Jorge Vélez-Ruiz

About the Editors
Jorge Welti-Chanes is a Professor in the Departments of Chemical and Food
Engineering and of Chemistry and Biology at the Universidad de las Americas–
Puebla in Mexico. He earned his B.S. degree in Biochemical Engineering and his
M.S. in Food Engineering from the ITESM, Mexico and his Ph.D. from the
Universidad de Valencia, Spain. Dr. Welti-Chanes was president of the International
Association of Engineering and Food and is a member of the editorial boards of five
international journals. He is the author and co-author of more than 80 scientific
papers and the editor of five books with the food technology, water activity, drying,
emerging technologies, and minimal processing areas.
Dr. Jorge F. Vélez-Ruiz was born in Puebla City, Mexico. He received a B.S.
in Biochemical Engineering in 1977 and an M.S. in Food Science in 1981, both from
the Instituto Tecnológico y de Estudios Superiores de Monterrey (ITESM), Mexico,
and a Ph.D. in Food Engineering from Washington State University, Pullman in
1993. He began his professional career working in the food industry and in 1979
joined the Food Science Department, ITESM. Since 1980, he has been with the
Department of Chemical and Food Engineering, University of the Américas, Puebla
(UDLA,P), serving as chairman from 1987 to 1990. In 1990, he was recognized as
Food Engineering Researcher by the National System of Researchers in Mexico and
in 1999 was named titular professor.
Dr. Vélez-Ruiz’s research activities are focused on rheology of foods; dairy
products and milk processing; evaporation and dehydration of fluid foods; osmotic
concentration of fruits; heat and mass transfer through the frying process; and
physical properties of foods. He is the author of approximately 45 scientific publi-
cations in international journals, more than 90 presentations at national and inter-
national professional meetings, and three book chapters, and he is an editor of three
food science and engineering journals.
Gustavo V. Barbosa-Cánovas earned his B.S. in Mechanical Engineering at the
University of Uruguay and his M.S. and Ph.D. in Food Engineering at the University
of Massachusetts–Amherst. He then worked as an Assistant Professor at the
University of Puerto Rico from 1985–1990. Next, he went to Washington State
University (WSU), where he is now a Professor of Food Engineering and Director
of the Center for Nonthermal Processing of Food (CNPF). His current research areas
are nonthermal processing of foods, physical properties of foods, and food powder
technology.

Acknowledgments
The editors would like to acknowledge each one of the researchers who kindly
agreed to participate in this project with their contributions.
The support of the Universidad de las Américas, Puebla, of Washington State
University, and of Texas Christian University is also acknowledged.
For the manuscript’s revision and correction process, the editors counted on the
valuable work of M.S. Reyna León and M.S. Daniela Bermúdez, who were supported
by Ing. Luz del Carmen López, to help the complete book. We express our gratitude
to them.

Contributors
A.G. Abdul-Ghani P.M. Azoubel
Food Science and Process Engineering Faculdade de Engenharia de
Group Alimentos
Department of Chemical and Materials UNICAMP
Engineering Campinas, São Paulo, Brazil
The University of Auckland
Auckland, New Zealand E. Azuara-Nieto
Instituto de Ciencias Básicas
E.A.A. Adell Universidad Veracruzana
Departamento de Engenharia Química Xalapa, Veracruz, México
e Alimentos
Escola de Engenharia Mauá M.O. Balaban
Instituto Mauá de Tecnologia — Praça Food Science and Human Nutrition
Mauá University of Florida
São Paulo, Brazil Gainesville, Florida
S.M. Alzamora
J. Barat
Departamento de Industrias
Department of Food Technology
Facultad de Ciencias Exactas y
Universidad Politécnica de Valencia
Naturales
Valencia, Spain
Universidad de Buenos Aires
Buenos Aires, Argentina
G.V. Barbosa-Cánovas
A. Andrés Department of Biological Systems
Department of Food Technology Engineering
Universidad Politécnica de Valencia Washington State University
Valencia, Spain Pullman, Washington
A. Angersbach A.F. Baroni

Department of Food Biotechnology and Departamento de Engenharia Química
Food Process Engineering e Alimentos
Berlin University of Technology Escola de Engenharia Mauá
Berlin, Germany Instituto Mauá de Tecnologia — Praça
Mauá
J. Arul São Paulo, Brazil
Department of Food Science and
Nutrition and Horticulture Research F.H. Barron
Center Department of Packaging Science
Laval University Clemson University
Sainte-Foy, Quebec, Canada Clemson, South Carolina

J. Benedito M.S. Chinnan
Food Technology Department Center for Food Safety and Quality
Universidad Politécnica de Valencia Enhancement
Valencia, Spain Department of Food Science and
Technology
C.I. Beristain-Guevara University of Georgia, Griffin
Instituto de Ciencias Básicas Campus
Universidad Veracruzana Griffin, Georgia
Xalapa, Veracruz, México
A. Chiralt
J.M. Bunn
Department of Packaging Science
Clemson University
Valencia, Spain
Clemson, South Carolina
J. Cárcel P. Coronel
Department of Food Technology Department of Food Science
Universidad Politécnica de Valencia North Carolina State University
Valencia, Spain Raleigh, North Carolina
F. Castaigne
J.G. Crespo
Department of Food Science and
Department of Chemistry
Nutrition and Horticulture Research
Faculdade de Ciências e Tecnología
Center
Universidade Nova de Lisboa
Laval University
Caparica, Portugal
Sainte-Foy, Quebec, Canada
M.A. Castro S.L. Cuppett

Departamento de Ciencias Biológicas Department of Food Science and
Facultad de Ciencias Exactas y Technology
Naturales University of Nebraska-Lincoln
Universidad de Buenos Aires Lincoln, Nebraska
Buenos Aires, Argentina
F. Erdoǧdu
K.V. Chau
Department of Food Engineering
Biological and Agricultural Engineering
University of Mersin
University of Florida
Ciftlikkoy, Mersin, Turkey
Gainesville, Florida
X.D. Chen M.M. Farid

Food Science and Process Engineering Food Science and Process Engineering
Group Group
Department of Chemical and Materials Department of Chemical and Materials
Engineering Engineering
The University of Auckland The University of Auckland
Auckland, New Zealand Auckland, New Zealand

H. Feng J.A. Hernández-Pérez
Department of Biological Systems Joint Research Unit Food Process
Engineering Engineering
Washington State University Cemagref, ENSIA, INAPG, INRA
Pullman, Washington Massy, France
P. Fito
B. Heyd
Joint Research Unit Food Process
Engineering
Valencia, Spain
Cemagref, ENSIA, INAPG, INRA
Massy, France
A.L. Gabas
Departamento de Engenharia de
Alimentos M.V. Karwe
Universidade Estadual de Campinas Department of Food Science
Campinas, São Paulo, Brazil Rutgers University
New Brunswick, New Jersey
M.A. Garcia-Alvarado
Departamento de Ingeniería Química y
D. Knorr
Bioquímica
Department of Food Biotechnology and
Instituto Tecnológico de Veracruz
Food Process Engineering
Veracruz, México
Berlin University of Technology
Berlin, Germany
C. González-Martínez
Universidad Politécnica de Valencia H. Krishnamurthy
Valencia, Spain Department of Food Science and
Agricultural Chemistry
S. Grabowski McGill University, Macdonald
Food Research and Development Campus
Centre Ste. Anne de Bellevue, Quebec,
Agriculture and Agri-Food Canada Canada
St. Hyacinthe, Quebec, Canada
R. León-Cruz
G.F. Gutiérrez-López
Departamento de Ingeniería Química y
Departamento de Graduados e
Alimentos
Investigación en Alimentos
Universidad de las Américas-Puebla
Escuela Nacional de Ciencias
Santa Catarina Mártir
Biológicas — I.P.N.
Cholula, Puebla, México
México, México
F. Hamouz M. Marcotte
Department of Nutritional Science and Food Research and Development
Dietetics Centre
University of Nebraska-Lincoln Agriculture and Agri-Food Canada
Lincoln, Nebraska St. Hyacinthe, Quebec, Canada

J. Martínez-Monzó K. Niranjan
Department of Food Technology School of Food Biosciences
Universidad Politécnica de Valencia The University of Reading
Valencia, Spain Reading, Berkshire, U.K.
F.C. Menegalli N. Nitin

Departamento de Engenharia de Department of Food Science
Alimentos Rutgers University
Universidade Estadual de Campinas New Brunswick, New Jersey
Campinas, São Paulo, Brazil
R. Olivas-Vargas
M.R. Menezes Advanced Materials Research Center
Departamento de Engenharia de Complejo Industrial Chihuahua
Alimentos Chihuahua, México
Universidade Estadual de Campinas
Campinas, São Paulo, Brazil E. Ortega-Rivas
Graduate Program in Food Science and
Technology
F.J. Molina-Corral
University of Chihuahua
Graduate Program in Food Science and
Chihuahua, México
Technology
University of Chihuahua
Chihuahua, México K.S. Pannu
Food Process Engineering
Delta
H. Mújica-Paz British Columbia, Canada
Facultad de Ciencias Químicas
Universidad Autónoma de Chihuahua
A. Pérez-Hernández
Chihuahua, México
Advanced Materials Research Center
Complejo Industrial Chihuahua
A. Mulet Chihuahua, México
Food Technology Department
Universidad Politécnica de Valencia D.L. Pyle
Valencia, Spain School of Food Biosciences
The University of Reading
F.E.X. Murr Reading, Berkshire, U.K.
Faculdade de Engenharia de Alimentos-
UNICAMP H.S. Ramaswamy
Campinas, São Paulo, Brazil Department of Food Science and
Agricultural Chemistry
A. Nieto McGill University, Macdonald Campus
Departamento de Industrias Ste. Anne de Bellevue, Quebec, Canada
Facultad de Ciencias Exactas y
Naturales A.L. Raoult-Wack
Universidad de Buenos Aires CIRAD, Agri-Food Program
Buenos Aires, Argentina Montpellier, France

N.K. Rastogi S. Simal
Department of Food Engineering Chemistry Department
Central Food Technological Research Universitat de les Illes Balears
Institute Palma de Mallorca, Spain
Mysore, India
R.P. Singh
E.P. Ribeiro Department of Biological and
Departamento de Engenharia Química Agricultural Engineering
e Alimentos University of California, Davis
Escola de Engenharia Mauá Davis, California
Instituto Mauá de Tecnologia—Praça
Mauá M.E. Sosa-Morales
São Paulo, Brazil Chemical Engineering and Food
Engineering Department
C. Rosselló Universidad de las Américas-Puebla
Chemistry Department Santa Catarina Mártir, Cholula
Universitat de les Illes Balears Puebla, México
Palma de Mallorca, Spain
J. Tang
S.S. Sablani
Department of Biological Systems
Department of Bioresource and
Engineering
Agricultural Engineering
Washington State University
Sultan Qaboos University
Pullman, Washington
Muscat Sultanate of Oman
J. Telis-Romero
K.P. Sandeep
Departamento de Engenharia e
Department of Food Science
Tecnologia de Alimentos
North Carolina State University
Universidade Estadual Paulista
Raleigh, North Carolina
São José do Rio Preto, São Paulo,
T. Schäfer Brazil
Department of Chemistry-CQFB
Faculdade de Ciências e Tecnología R.F. Testin
Universidade Nova de Lisboa Department of Packaging Science
Caparica, Portugal Clemson University
M. Schnepf
Department of Nutritional Science and G. Trystram
Dietetics Joint Research Unit Food Process
University of Nebraska-Lincoln Engineering
Lincoln, Nebraska Cemagref, ENSIA, INAPG, INRA
Massy, France
D.R. Sepúlveda
Department of Biological Systems A. Valdez-Fragoso
Engineering Facultad de Ciencias Químicas
Washington State University Universidad Autónoma de Chihuahua
Pullman, Washington Chihuahua, México

M.E. Vargas-Ugalde J. Welti-Chanes
Departamento de Ingeniería y Departamento de Ingeniería Química y
Tecnología Alimentos
Facultad de Estudios Superiores Universidad de las Américas-Puebla
Cuautitlán Santa Catarina Mártir, Cholula
Izcalli, Edo. de México, México Puebla, México
School of Food Biosciences
The University of Reading
S. Wichchukit
Reading, Berkshire, U.K.
Department of Biological and
Departamento de Graduados e
Agricultural Engineering
Investigación en Alimentos
University of California, Davis
Escuela Nacional de Ciencias
Davis, California
Biológicas - I.P.N.
México, México
J.L. Wiles
J.F. Vélez-Ruiz Department of Packaging Science
Chemical Engineering and Food Clemson University
Engineering Department Clemson, South Carolina
Universidad de las Américas-Puebla
Santa Catarina Mártir, Cholula Y. Wu
Puebla, México Department of Research and
Development
P.J. Vergano The Wright Group
Department of Packaging Science Crowley, Louisiana
Clemson University
M.R. Zareifard
O. Vitrac Department of Food Science and
INRA - Food Packaging Unit Agricultural Chemistry
Centre de Recherches Agronomiques McGill University, Macdonald Campus
Reims, France Ste. Anne de Bellevue, Quebec, Canada
C.L. Weller S.E. Zorrilla

Industrial Agricultural Products Center Instituto de Desarrollo Tecnológico para
and la Industria Química (INTEC)
Department of Biological/Systems Consejo Nacional de Investigaciones
Engineering Científicas y Técnicas
University of Nebraska-Lincoln Universidad Nacional del Litoral
Lincoln, Nebraska Santa Fe, Argentina

Table of Contents
Part I Fundamental Concepts
1 Fundamentals of Mass Transport
J. Welti-Chanes, H. Mújica-Paz, A. Valdez-Fragoso, and R. León-Cruz
2 Heat Transfer in Food Products
D.R. Sepúlveda and G.V. Barbosa-Cánovas
3 Introductory Aspects of Momentum Transfer Phenomena
J.F. Vélez-Ruiz
Part II Mass Transfer

4 Structural Effects of Blanching and Osmotic Dehydration
Pretreatments on Air Drying Kinetics of Fruit Tissues
S.M. Alzamora, A. Nieto, and M.A. Castro
5 Pretreatment Efficiency in Osmotic Dehydration of Cranberries
S. Grabowski and M. Marcotte
6 Mass Transfer Description of the Osmodehydration of Apple Slabs
E. Azuara-Nieto, G.F. Gutiérrez-López, and C.I. Beristain-Guevara
7 Combined Effect of High Hydrostatic Pressure Pretreatment
and Osmotic Stress on Mass Transfer during Osmotic Dehydration
N.K. Rastogi, A. Angersbach, and D. Knorr
8 Hydrodynamic Mechanisms in Plant Tissues during Mass
Transport Operations
P. Fito, A. Chiralt, J. Martínez-Monzó, and J. Barat
9 Effect of Pretreatment on the Drying Kinetics of Cherry Tomato
(Lycopersicon esculentum var. cerasiforme)
P.M. Azoubel and F.E.X. Murr
10 Determination of Concentration-Dependent Effective Moisture
Diffusivity of Plums Based on Shrinkage Kinetics
A.L. Gabas, F.C. Menegalli, and J. Telis-Romero
11 Modeling Dehydration Kinetics and Reconstitution Properties
of Dried Jalapeño Pepper
R. Olivas-Vargas, F.J. Molina-Corral, A. Pérez-Hernández,
and E. Ortega-Rivas
12 Application of an Artificial Neural Network for Moisture Transfer
Prediction Considering Shrinkage during Drying of Foodstuffs
J.A. Hernández-Pérez, M.A. García-Alvarado, G. Trystram,
and B. Heyd

13 Modeling of Prato Cheese Salting: Fickian and Neural
Network Approaches
A.F. Baroni, M.R. Menezes, E.A.A. Adell, and E.P. Ribeiro
14 Influence of Vacuum Pressure on Salt Transport during Brining
of Pressed Curd
A. Chiralt, P. Fito, C. González-Martínez, and A. Andrés
15 Effects of Water Concentration and Water Vapor Pressure on the
Water Vapor Permeability and Diffusion of Chitosan Films
J.L. Wiles, P.J. Vergano, F.H. Barron, J.M. Bunn, and R.F. Testin
16 Water Vapor Permeability, Water Solubility, and Microstructure
of Emulsified Starch–Alginate–Fatty Acid Composite Films
Y. Wu, C.L. Weller, F. Hamouz, S.L. Cuppett, and M. Schnepf
17 Mass Transport Phenomena during the Recovery of Volatile
Compounds by Pervaporation
T. Schäfer and J.G. Crespo
18 Ultrasonic Mass Transfer Enhancement in Food Processing
A. Mulet, J. Cárcel, J. Benedito, C. Rosselló, and S. Simal
19 Mass Transfer and Residence Time Studies in Spinning
Cone Columns
M.E. Vargas-Ugalde, K. Niranjan, D.L. Pyle, and G.F. Gutiérrez-López
Part III Heat Transfer

20 Transport Phenomena during Double-Sided Cooking of Meat Patties
S.E. Zorrilla, S. Wichchukit, and R.P. Singh
21 Thermal Processing of Particulate Foods by Steam Injection.
Part 1. Heating Rate Index for Diced Vegetables
K.S. Pannu, F. Castaigne, and J. Arul
22 Thermal Processing of Particulate Foods by Steam Injection.
Part 2. Convective Surface Heat Transfer Coefficient for Steam
23 Modeling of Heat Conduction in Elliptical Cross Sections
(Oval Shapes) Using Numerical Finite Difference Models
F. Erdoğdu, M.O. Balaban, and K.V. Chau
24 Heat Transfer Coefficient for Model Cookies in a Turbulent Multiple
Jet Impingement System
N. Nitin and M.V. Karwe
25 Flow Dynamics and Heat Transfer in Helical Heat Exchangers
P. Coronel and K.P. Sandeep
26 Relating Food Frying to Daily Oil Abuse. Part 1. Determination
of Surface Heat Transfer Coefficients with Metal Balls
K.S. Pannu and M.S. Chinnan

Part IV Combined Transfer Phenomena
27 Relating Food Frying to Daily Oil Abuse. Part 2. A Practical
Approach for Evaluating Product Moisture Loss, Oil Uptake,
and Heat Transfer
28 Heat and Mass Transfer during the Frying Process of Donuts
J.F. Vélez-Ruiz and M.E. Sosa-Morales
29 Influence of Liquid Water Transport on Heat and Mass Transfer
during Deep-Fat Frying
O. Vitrac, A.L. Raoult-Wack, and G. Trystram
30 Numerical Simulation of Transient Two-Dimensional Profiles
of Temperature, Concentration, and Flow of Liquid Food
in a Can during Sterilization
A.G. Abdul-Ghani, M.M. Farid, and X.D. Chen
31 Heating Behavior of Canned Liquid/Particle Mixtures during
End-over-End Agitation Processing
S.S. Sablani, H.S. Ramaswamy, and H. Krishnamurthy
32 Dimensionless Correlations for Forced Convection Heat Transfer
to Spherical Particles under Tube-Flow Heating Conditions
H.S. Ramaswamy and M.R. Zareifard
33 Heat and Mass Transfer Modeling in Microwave and Spouted
Bed Combined Drying of Particulate Food Products
H. Feng and J. Tang

Part I
Fundamental Concepts

Fundamentals of Mass
1 Transport
J. Welti-Chanes, H. Mújica-Paz,
A. Valdez-Fragoso, and R. León-Cruz
CONTENTS
1.1 Introduction
1.2 Mass Transfer Variables
1.2.1 Concentration
1.2.2 Velocity
1.2.3 Flux
1.2.4 Flux Relations for Binary Systems
1.3 Mass Transfer by Diffusion
1.3.1 Steady State Diffusion
1.3.2 Molecular Diffusion in Gases, Liquids, and Solids
1.3.2.1 Molecular Diffusion in Gases
1.3.2.2 Molecular Diffusion in Liquids
1.3.2.3 Molecular Diffusion in Solids
1.3.3 Unsteady State Diffusion
1.3.3.1 Solutions of Fundamental Equations
1.4 Mass Transfer by Convection
1.4.1 Film Theory and Mass Transfer Coefficient
1.4.2 Two-Film Theory and Mass Transfer Coefficient
1.4.3 Dimensionless Numbers for Mass Transfer
1.4.4 Transport Analogies
1.4.5 Mass Transfer Coefficients and Correlations
1.4.6 Mass Transfer Units
Nomenclature
References
1.1 INTRODUCTION
Mass transfer can be defined as the migration of a substance through a mixture under
the influence of a concentration gradient in order to reach chemical equilibrium.
Biochemical and chemical engineering operations, such as absorption, humidifi-
cation, distillation, crystallization, and aeration, involve mass transfer principles.

In food processing, mass transfer phenomena are present in freeze-drying, osmotic
dehydration, salting or desalting, curing and pickling, extraction, smoking, baking,
frying, drying of foods, membrane separations, and the transmission of water vapor,
gases, or contaminants across a packaging film. Food stability and the preservation
of food quality are also affected by mass transfer of environmental components that
can affect the rate of reactions. Among the components involved in these mass transfer
processes are water, sugars, salt, oils, proteins, acids, flavor and aroma substances,
oxygen, carbon dioxide, residual monomers or polymer additives, and toxins or car-
cinogens produced by microorganisms. Furthermore, mass transfer phenomena are
important in the scale-up of processes to pilot- or commercial-scale plants and in the
control and optimization of the processes.
This chapter presents the basic principles of mass transfer. First, the variables
that occur in mass transfer are reviewed. Then the mechanisms of mass transfer,
diffusion and convection are discussed. Analogies among momentum, heat, and
mass transfer are described; convective mass transfer coefficients and correlations
are derived by analogy with convective heat transfer. Finally, the concept of transfer
units is presented.
1.2 MASS TRANSFER VARIABLES

Mass transfer processes involve concentration, velocity, and flux variables, which
are defined and related by a set of basic equations (White, 1988).
1.2.1 CONCENTRATION
The concentration of a mixture and its components may be expressed in terms of
3
mass and mol. In terms of mass, the mass concentration of the mixture (ρ, kg/m ),
3
the mass concentration of a component i (ρi, kg/m ), and the mass fraction of
component i (wi) are given by:
ρ= m/V (1.1)
ρi = m i / V (1.2)
w i = m i / m = ρi / ρ (1.3)
where m and mi are the mass flux of the mixture and component i, respectively.
3
The bulk molar concentration (C, kg mol/m ), the molar concentration of com-
3
ponent i (Ci, kg mol/m ), and the mole fraction of component i (xi) are defined by:
C = n/V (1.4)
Ci = n i / V (1.5)
x i = n i / n = Ci / C (1.6)
where n and ni are the mol of the mixture and component i, respectively.

According to the previous definitions, it can be easily shown that:
n n
m= ∑
i =1
m i and ρ = ∑ρ
i =1
i (1.7)
n n
n= ∑
i =1
n i and C = ∑C
i =1
i (1.8)
n n
w= ∑
i =1
w i = 1 and x = ∑x =1
i =1
i (1.9)
where xi is the mole fraction of component i, and ρi and Ci are related through the
molecular weight of constituent i (Mi, kg/kg mol):
ρi = M i C i (1.10)
1.2.2 VELOCITY
In mass transfer phenomena, the velocity of a bulk mixture and of its components
can be measured with respect to fixed coordinates. In addition, the velocity of the
components can also be measured relative to the bulk velocity. Figure 1.1 illustrates
these velocities in a binary system of components A and B in the z direction.
fixed coordinate
vB – v = diffusion velocity of B = UB
vB
v= wA vA + wB vB
vA
z
vA – v = diffusion velocity of A = UA
FIGURE 1.1 Scheme of individual and bulk velocities of a binary mixture.

The mass bulk velocity of the mixture (v, m/sec) relative to fixed coordinates is
defined as:
n n n
ρi
∑ ∑ ∑ ρv
mi
v= wi vi = v = (1.11)
i =1 i =1
m i i =1
i
where vi is the velocity of component i with respect to stationary coordinates.

In a similar manner, a molar bulk velocity ( V, m/sec) measured relative to
stationary coordinates can be defined as:
n n n
∑x V = ∑ ∑ CV
ni Ci
V= i i V = i (1.12)
i =1 i =1
n i i =1
The velocity of the constituent i relative to the bulk velocity of the mixture is:
u i = vi − v (1.13)
Ui = Vi − V (1.14)
where ui (m/sec) and Ui (m/sec) are the mass and molar diffusion velocities, respectively.
1.2.3 FLUX
2 2
The mass bulk flux (n, kg/m sec) and the molar bulk flux ( N , kg mol/m sec) of a
mixture relative to fixed coordinates are:
n
n = ρv = ∑ρ v
i =1
i i (1.15)
N = CV = ∑C V
i =1
i i (1.16)
The flux of the components of a mixture can also be expressed relative either
to fixed coordinates or to the bulk average velocity. The flux of the component i
relative to stationary coordinates is:
n i = ρi v i (1.17)
N i = Ci Vi (1.18)
The diffusion fluxes of the constituents i of the mixture with respect to the
2 2
average bulk velocity are ji (kg/m sec) for the mass flux and Ji (kg mol/m sec) for
the molar flux.
ji = ρi u i = ρi ( vi − v) (1.19)
J i = C i U i = C i (V i − V) (1.20)

The use of concentration, velocities, and fluxes in mass or molar terms is subject
to preferences and convenience. Nevertheless, concentration and flux expressed
in molar units and average molar velocity are preferred. In discussing the funda-
mentals of mass transfer, systems are frequently assumed as a two-component mixture
to facilitate the understanding of multi-component systems found in engineering
applications.
1.2.4 FLUX RELATIONS FOR BINARY SYSTEMS

For a binary mixture of components A and B, Equations (1.18) and (1.20) become:
N A = CA VA (1.21)
J A = C A U A = C A (V A − V) (1.22)
Substituting V from Equation (1.12) into Equation (1.22),
CA
J A = CA V A − CA V = CA VA − (C A V A + C B V B ) (1.23)
C
Since N A = C A V A and N B = C B V B , for component A, Equation (1.23) becomes:
CA
NA = JA + (N A + N B ) (1.24)
C
A similar mathematical derivation gives for component B:
CB
NB = JB + (N A + N B ) (1.25)
C
Equations (1.24) and (1.25) show that the absolute molar flux (NΑ or NB) results
from a concentration gradient contribution or a molar diffusion flux (JA or JB) and
a convective contribution ( C A V or C B V). The molar diffusion flux is described by
Fick’s law, which for component A is written as:
dC A
J A = − D AB (1.26)
dz
where DAB is the diffusion coefficient of A through B and dCA/dz is the change of
the concentration A with respect to the position z.
In terms of mass, the mass fluxes for components A and B are, respectively:
ρA
n A = jA + (nA + nB ) (1.27)
ρ˜
nB
n B = jB + (n + n B ) (1.28)
ρ̃ A

Two important simple cases can be considered in Equation (1.24):
1. Diffusion of A through stagnant B, NB = 0
JA D dC A
NA = = − AB (1.29)
1 − xA 1 − x A dz
2. Equimolar counter-diffusion NA + NB = 0,
dC A
N A = J A = − D AB (1.30)
dz
where xA is the mole fraction of component A in the case of dilute systems xA <<
1, and Equations (1.29) and (1.30) become the same.
1.3 MASS TRANSFER BY DIFFUSION

Mass transfer by diffusion is the transport of molecules caused by a random molec-
ular motion in a region in which a composition gradient exists.
1.3.1 STEADY STATE DIFFUSION

Steady state diffusion, in which the concentration does not change with time at any
position, is described by Fick’s first law.
∂Ci
J i = − Dim (1.31)
∂z
2
where Ji is the molar diffusion flux of component i (kg mol/sec m ) in the z direction
3
(m), Ci is the concentration of component i (kg mol/m ), and Dim is the diffusion
2
coefficient of i with respect to the mixture (m /sec). This equation is widely used
in problems related to the processing and preservation of foods.
The mass flux (ji) of the component i is expressed as:
∂ρi
ji = − Dim (1.32)
∂z
2 3 2
where the units of ji, ρi, and Dim are, respectively, kg/sec m , kg/m , and m /sec.
1.3.2 MOLECULAR DIFFUSION IN GASES, LIQUIDS, AND SOLIDS

Theoretical and empirical correlations for estimating the binary diffusion coefficient
DAB in gases, liquids, and solids are described in this section.

1.3.2.1 Molecular Diffusion in Gases
The diffusion coefficient of component A through B (DAB) may be estimated for

pressures below 20 atm from the formula:
(1 / M A + 1 / M B )1/ 2
D AB = 0.001858T 3/ 2 (1.33)
Pσ 2ABΩ D
where P is the absolute pressure (atm), T is the absolute temperature (K), σAB is the
collision diameter (°A), ΩD is the collision integral for molecular diffusion, and MA
and MB are the molecular weights of A and B, respectively (Sherwood et al., 1975).
1.3.2.2 Molecular Diffusion in Liquids
The diffusivity of a solute A in a dilute solution B (DAB) can be predicted by the

following equation (Treybal, 1981):
T
D AB = 7.4 × 10 −8 (ϕ BM B )1/ 2 (1.34)
µ BVA0.6
where ϕB, µB, and MB are an association parameter, the viscosity (centipoises), and
the molecular weight of solvent B, respectively, T is the absolute temperature (K),
3
and VA is the molal volume of A (cm /g mol).
1.3.2.3 Molecular Diffusion in Solids
The diffusion of gases and liquids through porous solid materials may occur by a
combination of Fick diffusion and Knudsen diffusion.
If the pores are large, the mass transfer within the gas or liquid contained in the
pores will be by Fick diffusion. Nevertheless, the diffusivity in the solid is reduced
below what it would be in a fluid, due to the tortuous nature of the path that a
molecule must travel to advance a given distance in the solid and to the restricted
free cross-sectional area (Sherwood et al., 1975). In such a case, the flux must be
described in terms of an “effective” diffusion coefficient, defined as:
ε
Deff = D (1.35)
τ AB
where DAB is the diffusion coefficient in a binary system, τ is the tortuosity, and ε is
the fractional void space. Values of ε, τ, and Deff must be determined experimentally.
Therefore, when the system is a porous solid that has interconnected voids that
affect the diffusion, for a binary system the molar flow is:
ε dC
N A = − D AB A (1.36)
τ dz

Knudsen diffusion occurs when the pores are small and their size approaches
the mean free path of the gas molecule. A gas molecule now collides predominantly
with the walls of the pores rather than with other molecules. The Knudsen diffusion
coefficient (DK), derived from the kinetic theory of gases (Welty et al., 1984), is
given by the expression:
19400ε 2 T
DK = (1.37)
τS′ ρ M
where ρ is the density of the solid material, M is the molecular weight of the diffusing
gas, and T is the temperature (K).
The molar flux for gas and liquids through a porous solid can be described in
terms of DK by:
(C A1 − C A 2 ) (p − pA2 )
N A = DK = D K A1 (1.38)
z RTz
where CA1 and CA2 are the bulk concentrations in the gas and liquid phases, respectively,
and pA1 and pA2 are the partial pressures of the gas and liquid phases, respectively.
When Fick and Knudsen diffusions are important, the effective diffusion coef-
ficient is defined by:
1 1 1
= + (1.39)
Deff D AB D K
which applies for equimolar counter-diffusion.

Diffusion in liquids is important in separation operations such as liquid–liquid
extraction and distillation. Typical examples of diffusion of fluids through solids are
water vapor transport in the drying of porous foods, the diffusion of a gas through
a polymer film used in the packaging of foods, and separation processes through a
membrane, such as reverse osmosis and ultrafiltration.
1.3.3 UNSTEADY STATE DIFFUSION

The unsteady state diffusion, in which the local concentration change with time is
described in one dimension for slab shape and constant DAB, is shown by Fick’s
second law:
∂C A d 2CA
= D AB (1.40)
∂t dz 2
Analogous equations can be written for diffusion in spherical or cylindrical
shapes and two or three dimensions. These equations are used to find the concen-
tration of a solute as a function of time and position and are mainly applicable to
diffusion in solids and to limited situations in fluids. The analysis of unsteady state
systems, however, is frequently simplified to a one-directional flow.

1.3.3.1 Solutions of Fundamental Equations
Solutions to unsteady state diffusion equations can be obtained by analytical, numer-

ical, and graphical methods. Analytical solutions for one-dimensional diffusion in
an infinite slab, an infinite cylinder, and a sphere have been found by assuming a
constant diffusion coefficient given appropriate boundary conditions (Crank, 1975):
1. Infinite slab:
n =∞
C − C∞  D(2n + 1)2 π 2 t 
∑ 2n− + 1 cos  2n 2+δ1
4 ( 1)n ( )πx 
= exp −  (1.41)
C0 − C∞ π n=0
  4δ 2 
2. Infinite cylinder:
n =∞
C − C∞
∑ b J (b , r) exp(−Db t)
2 J0 (bn , r)
= 2
(1.42)
C0 − C∞ R n =1 n 1 n
n
3. Sphere:
n =∞
C − C∞ (−1)n +1 1 sin nπr  exp Dn 2 π 2 t 
∑
2R
=   (1.43)
C0 − C∞ π n r  R   R
2

n =1
where Co and C are the molar concentration at time t = 0 and t = ∞, respectively.

When properties become dependent upon position or concentration, the solutions
become more complicated. In this case, numerical techniques can be used, since they
are more appropriate for complex and real problems. Among the numerical methods
are finite difference and finite element analysis. The finite difference method is based
on the approximation of the difference of a derivative at a point. This analysis is often
limited to cases where the body has a simple geometry. The finite element method
of analysis overcomes this problem; its basic concept is that any continuous quantity,
such as a concentration, can be approximated by a discrete model composed of a set
of piecewise continuous functions defined over a finite number of domains.
For unsteady state heat conduction problems in solids, solutions have been
presented for simple geometries subject to a given set of boundary and initial
conditions. These solutions are presented in charts in terms of dimensionless ratios
and can be translated directly to analogous problems of unsteady state diffusion,
allowing the application of heat transfer results to solve mass diffusion problems.
The ordinate of these charts represents the fraction of the unaccomplished change
2
[(c1 – c)/(c1 – c0)] and the abscissa the relative time [DABt /x1 ]. These charts and
their physical significance, use, and application are presented in several books (Welty
et al., 1984; Geankoplis, 1993). Table 1.1 summarizes the correspondence between
variables for unsteady heat and molecular diffusion.

TABLE 1.1
Relation between Mass and Heat Transfer Variables for Unsteady State
Mass Transfer
Heat Transfer K=1 K≠1
Y, Unaccomplished change T1 − T c1 − c (c1 / K ) − c

T1 − T0 c1 − c 0 (c1 / K ) − c 0
X, Relative time αt D AB t D AB t
x12 x12 x12
m, Relative resistance k D AB D AB
hx1 k m x1 Kk m x1
n, Relative position x x x
x1 x1 x1
Note: T0 and c0 = temperature and concentration at time t = 0, respectively; T1 and c1 = temperature

and concentration at the position of interest; x 1 = distance from the midpoint to the position of
interest; m = ratio of the convective mass transfer resistance to the internal molecular resistance to
the mass transfer; K = cLi/ci, where cLi = bulk fluid concentration and ci = concentration in the fluid
adjacent to the solid surface.
Source: Adapted from Welty, J.R., Wicks, C.E., and Wilson, R.E., Momentum, Heat, and Mass
Transfer, John Wiley & Sons, New York, 1984 and Geankoplis, C.J., Transport Processes and Unit
Operations, 3rd ed., Prentice-Hall, London, 1993. With permission.
1.4 MASS TRANSFER BY CONVECTION

Convective mass transport, which occurs in liquids and gases, results from bulk
motion of the fluid imposed by external forces (forced convection) or occurring
naturally, due to the concentration difference or density variations (free convection).
The free or forced character is determined by the nature of the motion of the fluid,
which may be either laminar or turbulent. In laminar flow, the mechanism is the
same as in a stationary medium, and the transfer occurs by diffusion. In turbulent
flow, mass transfer is affected by the irregular motion of small volumes of the fluid.
1.4.1 FILM THEORY AND MASS TRANSFER COEFFICIENT

Convective mass transfer problems in turbulent flow are not always amenable to
analytical methods of solution. Consequently, they are usually approached with the
aid of coefficients and empirical relationships. Among several models proposed for
a better understanding of mass transfer under turbulent regime, we find the model
built around the film theory. In this theory the interfacial region is treated as a
hypothetical stagnant film of thickness x, called the boundary layer, and it is assumed
that all the concentration changes occur in this layer (Figure 1.2) (Welty et al., 1984).

stagnant film
solid
CA1
bulk fluid
CA2
x
FIGURE 1.2 Fluid-solid interfacial region: z
the film theory.
Thus, the molar flux and the concentration profile of species A (JA) are found from
D AB
JA = (C A1 − C A 2 ) = − k m (C A1 − C A 2 ) (1.44)
x
where DAB/z is the mass transfer coefficient, km, CA1, and CA2 are the bulk concen-
trations in the fluid and solid phase, respectively, and
z(C A1 − C A 2 )
C A = C A1 − (1.45)
x
Similarly, the corresponding expression for mass flux is:
jA = k ρ (ρA1 − ρA 2 ) (1.46)
where CA is the concentration of the components A, and ρA1 and ρA2 are the mass
concentration of the fluid and solid, respectively.
2
The mass transfer coefficient kC or kρ has units of velocity (m /sec). It can be
determined either from experimental data and empirical formulas derived from them
or with the aid of methods of similitude theory. A rough estimation of km can be
attained by assuming km = D/x, provided the effective film thickness and the diffusion
coefficient are known (Sherwood, 1974).
1.4.2 TWO-FILM THEORY AND MASS TRANSFER COEFFICIENT

Mass transfer from a gas and/or a liquid to another fluid is a common engineering
problem. For interphase transfer, it is convenient to use an overall mass transfer
coefficient, the interpretation of which is achieved with the aid of the two-film theory.
Figure 1.3 schematically shows the transfer of component A from the gas phase to

gas phase liquid phase
interface
x1 x2
CA1
CA1i
CA2i
CA2
layer layer
CA 2
C*A 2 = mCA1 C*A1 =
m
FIGURE 1.3 Mass transfer at a gas liquid interphase: the two-film theory.
the liquid phase. The two-film theory assumes that the resistance to mass transfer
lies in each adjacent phase to the interphase and that no resistance is offered to the
transfer of the solute across the interphase (Welty et al., 1984).
At steady state, the fluxes in gas and liquid (J1) phases must be equal:
J1 = k mG (C A1 − C A1i ) = k mL − (C A 2 i − C A 2 ) (1.47)
where kmG and kmL are the mass transfer coefficients in the gas and liquid phases,
respectively, CA1i and CA2i are the concentrations of component A at the interface,
and CA1 and CA2 are the bulk concentrations in the gas and liquid phases, respectively.
Since the concentrations at the interphase are not easily measurable, it is con-
venient to calculate an overall mass transfer coefficient based on an overall potential
gradient between the bulk compositions. The overall driving force is not, however,
CA1 – CA2, since at the interphase discontinuity of the concentrations exists, and the
solubility in the liquid is not necessarily the same as in the gas. Moreover, the film
thickness x1 and x2 and the diffusivity of the solute may be different in the two phases.
The solubility relationship that governs the equilibrium concentration between
phases is of the form:
CG = mC L (1.48)
where m is the solubility constant between the two phases, and CG and CL are the
concentrations of the gas and liquid, respectively.

Thus, the flux in terms of the total potential gradient in the gas phase is:
 C 
J = K mG (C A1 − C*A1 ) = K mG C A1 − A 2 (1.49)
 m 
*
where CA2/m = C A1, which is the concentration in the gas phase that would exist in
equilibrium with CA2, the concentration of species A in the liquid.
A similar equation can be obtained for the overall coefficient if the driving force
is based on the concentration in the liquid phase:
J = K mL (C*A1 − C A 2 ) = K mL ( mC A1 − C A 2 ) (1.50)
where mCA1 is the concentration in the liquid that would exist in equilibrium with
*
C A1. KmG and KmL represent the overall mass transfer coefficient based on the gas
phase and the liquid concentration driving force.
Coefficients KmG and KmL are related to the individual mass transfer coefficients
and the equilibrium constant m of a gas–liquid (kmG) or vapor–liquid (kmL) system
as follows:
1 1 m
= + (1.51)
K mG k mG k mL
1 1 1
= + (1.52)
K mL mk mG k mL
These last two equations show the relationship among the coefficients for the
individual phases and the overall transfer coefficients, expressed as a global resis-
tance (1/KmG or 1/KmL) to the transfer of the diffusing component. In studying
performance separation processes, it is important to determine which individual
resistance is the limiting factor.
1.4.3 DIMENSIONLESS NUMBERS FOR MASS TRANSFER

Mass transfer coefficients are expected to vary with hydrodynamic conditions and
with geometrical and physical properties of the fluid. These variables are collected
into the so-called dimensionless numbers. Dimensionless numbers that arise in mass
transfer modeling and scale-up studies are presented in Table 1.2.
For mass transport, the Biot number is defined by the equation Bi = kmd/D. The
Biot number compares the resistance to mass transfer at the surface of a solid to the
resistance inside the solid. High Biot numbers can be obtained by increasing the mass
transfer coefficient. For instance, in solids drying, the higher the value of Bi, the
faster the drying proceeds; hence, the air humidity increases rapidly.
2
The Fick number, Fi = Dt/d , is a nondimensional time parameter. It is important
in studying unsteady state diffusion mass transfer in several simple shapes with
certain restrictive boundary conditions (Gekas, 1992).

TABLE 1.2
Dimensionless Numbers Related to Mass Transfer
Dimensionless
Number Equation Physical Meaning
Mass transfer across the

k md
Biot Bi = boundary/mass transfer within
D
the solid
Dt Dimensionless time in the
Fick Fi =
d2 unsteady state regime
Graetz ReSc Mass transfer in laminar flow
gd 3β∆Tρ2
Grashof Gr = Buoyancy forces/viscous forces
ν
α
Lewis Le = Heat diffusivity/mass diffusivity
D
vd
Peclet Pe = Convection/diffusion
D
vd
Reynolds Re = Inertial force/viscous force
ν
ν Momentum diffusivity/mass
Schmidt Sc =
D diffusivity
k md Measure of boundary layer
Sherwood Sh =
D thickness
km Wall mass transfer/mass transfer
Stanton St =
v by convection
The Graetz number is defined as the product of the Reynolds and Schmidt
numbers. It includes the effects of forced and free convection.
The Grashof number is a measure of free convection, which will be enhanced
by buoyancy forces (ρ) and decreased by viscous forces (ν). The Grashof number
is found in correlations of free convection mass transfer.
The Lewis number, Le = α/D, is the ratio of heat to mass diffusivity. It plays
an important role in processes where simultaneous convective transfer of energy and
mass occurs.
The Peclet number, defined as Pe = vd/D, is the ratio of bulk mass transport to
diffusive mass transport.
The Reynolds number, Re = vd/ν, characterizes the nature of the motion of a
flowing gas or liquid, and is interpreted as the ratio of inertial forces to the viscous
forces in the flow. When the Re value is below a certain critical value, the flow is
laminar; when it is larger, the flow is turbulent.
In the Schmidt number, Sc = ν/D, the two molecular transport coefficients (ν
and D) are the physical properties of the medium in which the transfer of mass takes
place. The Schmidt number, which represents the ratio of momentum to mass
diffusivities, is of great importance in convective mass transfer (Welty et al., 1984).

The Sherwood number is defined as Sh = kmd/D, where km is the mass transfer
coefficient, d is a characteristic length dimension, and D is the diffusion coefficient.
The Sherwood number is a convenient parameter for the analysis of transfer pro-
cesses occurring in a stationary medium in laminar flow. In the case of purely
molecular transfer, the Sherwood number is highly dependent on the geometrical
shape of the body.
The Stanton number is interpreted as the ratio of the mass-transfer coefficient
(km) to the flow velocity (v). It represents a measure of the mass flux in the direction
transverse to that of the mean flow. The Stanton number is used more conveniently
in turbulent flow.
The dimensionless numbers Sc, Sh, and Le will be encountered in the analysis
of convective mass transfer correlations.
1.4.4 TRANSPORT ANALOGIES

The basic laws governing the flux of momentum, heat, and mass transport due to
molecular motion or vibration have the form:
µ d d
τ= (ρv) = v (ρv) (1.53)
ρ dz dz
k d d
q=− (ρC p T) = −α (ρC p T) (1.54)
ρC p dz dz
dC
Ji = −D (1.55)
dz
All three processes are quite different from one another at a molecular level.
However, certain analogies exist among them. In effect, molecular diffusivities
kinematic viscosity (ν), thermal diffusivity (α), and diffusion (D) have the same
2
dimensions (L /t). Also, in Fick’s law, the molar flux varies with the gradient in mol
per volume; in the rewritten Fourier’s law, the energy flux is proportional to the
gradient of energy per volume (ρCpT); and the momentum flux, given by the rewritten
Newton’s law, varies with the gradient of the momentum per volume (ρv) (Cussler,
1984). These analogies are shown in Table 1.3.
The corresponding equations for momentum, heat and mass flux in convective
motion are:
τ = f  ρv2  =   (ρv − 0)
1 fv
(1.56)
2   2
h
q = h∆T = ∆(ρC p T) (1.57)
ρC p
N i = k m ∆Ci (1.58)

TABLE 1.3
Analogies among Momentum, Heat, and Mass Transfer
Analogous Form
Momentum Transfer Heat Transfer Mass Transfer
Variable ρv ρC p T C
(momentum/volume) (energy/volume) (mol/volume)
Molecular diffusivity ν α D
(kinematic viscosity) (thermal diffusivity) (diffusion coefficient)
Transfer coefficient f h km
(friction factor) (heat transfer coefficient) (mass transfer
coefficient)
Dimensionless ν ν
number Pr = Sc =
α D
h / ρC p km
St = St =
v v
α
Le =
D
where the transfer coefficient fv/2 is like h/ρCp and k. Note that the driving forces in
the momentum, heat, and mass flux are volume concentrations: (ρv − 0) is expressed
in momentum per volume, ∆(ρC p T) in energy per volume, and ∆Ci in mol per volume
(Table 1.3).
Since the molecular diffusivities have the same dimensions, a ratio of any of
two of these leads to dimensionless numbers: Pr number for heat transfer, Sc and
Le numbers for mass transfer. Likewise, the ratio transfer coefficients to the flow
velocity lead to an [St] number for heat transfer and an [St] number for mass transfer
(Tables 1.2 and 1.3).
A useful and simple analogy relating all three types of transport simultaneously
is the Chilton–Colburn analogy, which is written as
k m 2/3 h / ρC p 2/3 f
Sc = Pr = (1.59)
v v 2
The group
k m 2/3
Sc
v
is called the jD factor for mass transfer, and
h / ρC p
Pr 2 / 3 = St Pr 2 / 3
v
defines the jH factor for heat transfer.

The Chilton–Colburn analogy agrees well with a wide range of experimental
data for flow and geometries of different types in forced convection systems. There-
fore, when an engineer is concerned with the calculation of heat and mass transfer
coefficients, the analogies are of great utility. In this way, when heat transfer and
mass transfer occur by the same mechanism, the results of experiments on heat
transfer may be used to calculate diffusion processes, or vice versa. Also, information
obtained from a small-scale model can be used to scale up the process, or information
obtained with one substance can be extended to another substance. In very particular
cases, Pr = Sc = 1, which means that ν = α = D, and heat and mass transfer
measurements may be used to predict momentum transfer or vice versa (Sherwood
et al., 1975; Treybal, 1981).
1.4.5 MASS TRANSFER COEFFICIENTS AND CORRELATIONS

Although the analogy concept is useful in predicting mass transfer coefficients, in
certain turbulent situations correlations based on experimental observations are
required. A few typical correlations for mass transfer in a variety of geometries and
flow conditions are given in Table 1.4 (Treybal, 1981).
TABLE 1.4
Typical Mass Transfer Correlations
Situation Equation Remarks
Round tubes Sh = 0.023 Re 0.83 Sc 0.44 Used for turbulent flow

1/ 3
Used for laminar flow in a circular
Sh = 1.67 Re Sc
d
x  pipe
Flat plates Sh = 0.664 Re1/ 2 Sc1/ 3 Transfer begins at leading edge
Sh = 0.332 Re 1/ 2
Sc 1/ 3 Used for laminar flow over a plate
Used for evaporation drops in spray
Evaporation drops Sh = 2 + 0.6Sc1/ 3 Re1/ 2 drying
1/ 4
 d 4 ( P / V)  ν
1/ 3 Used in mixing liquid solutions; P/V
Stirred drops Sh = 0.13   D  is important in scale-up
 ρν
3

1/ 2 1/ 3
Solid spheres Sh = 2 + 0.6  
dv ν Used for forced convection
ν  D 
 d 3 [ ∆ρ]g 
1/ 4 1/ 3
Sh = 2 + 0.6  ν Used for natural convection
  D 
 ρν 
2
Bubbles Sh = 2 + 0.31(Gr )1/ 3 (Sc)1/ 2 Used for rising bubbles, d > 2.5 mm
Sh = 0.42 + (Gr ) (Sc) 1/ 3 1/ 2 Used for rising bubbles, d < 2.5 mm
k Used in actual or hypothetical

Membranes =1
dD membranes
Packed bed of Re f (particle diameter and superficial
jD = 1.17 Re −0.415
pellets velocity in the bed)

1.4.6 MASS TRANSFER UNITS
The number of transfer units is another approach in the application of pilot plant
results to the design of mass transfer equipment, such as cooling towers, packed
columns, extractors, or driers.
This method can be illustrated in the determination of the height of a drier (Z),
which is obtained as the product:
Z = HTU C NTU D (1.60)
where HTUc is the height of a transfer unit and NTUD is the number of mass transfer
units given by:
C2
∫ C −C
dC
NTU D = (1.61)
i b
C1
Subscripts 1 and 2 refer to inlet and outlet values. The integral is evaluated from
considerations of bulk (b) and interphase (i) conditions at any cross-section of the
drier, absorption tower, etc., the former being determined by mass balances and the
latter by equilibrium data.
The height of a transfer unit is given by:
G
HTU = (1.62)
k m aA tρg
where km is the mass transfer coefficient, a is a specific area, At is a cross-sectional

area of the drier, ρg is the density of the gas phase, and G is the gas flow rate.
In practice, it is found that HTU is a property of the type of drier and the material
being dried but is independent of size and operating conditions. Therefore, HTU
can be calculated from pilot plant experiments in which the height of the drier and
the number of transfer units are known. Thus, the design of a similar drier can be
obtained by scaling up the pilot plant results.
Here again, the Colburn analogy is of great utility. From the arguments used in
the section about transfer analogies, a similar expression for the Colburn analogy
has been proposed (Le Goff, 1980):
NTU DSc2 / 3 NTU H Pr 2 / 3

= = NEU (1.63)
LfD LfH
where the quantity NEU is the number of energy units, and the Le Goff number
(Lf) represents the deviation of the Colburn analogy from unity, the Lf number being
in the range 1–0.02.

Equations for NTUH and NEU are similar to Equation (1.58) for NTUD:
T2
∫ T −T
dT
NTU H = (1.64)
i b
T1
P1 − P2
NEU = (1.65)
ρv2
The number of transfer units is a basic parameter that appears frequently in the
design of heat and mass exchangers (Van den Bulck et al., 1985; Khodaparast, 1992;
Treybal, 1981).
NOMENCLATURE
2 2
a Specific area; cm or m
2
At Cross-sectional area of drier; m
bn Roots of Bessel function
3
C, c Molar concentration; kg mol/m
* 3
C Molar concentration at equilibrium; kg mol/m
Cp Specific heat capacity; kJ/kg K
d Characteristic dimension of a solid body; m or cm
2 2
D Diffusion coefficient; m /sec or cm /sec
f Friction factor; dimensionless
2
g Acceleration constant for gravity, m/sec
2
G Flow rate; kg/m sec
2
h Heat transfer coefficient; W/m K
HTUD Height of a mass transfer unit, m
j The mass flux of the mixture with respect to the average bulk velocity;
2
kg/m sec
J Molar diffusion flux of the mixture with respect to the average bulk velocity;
2
kg mol/m sec
Jo Bessel function of first kind and order zero
J1 Bessel function of first kind and order one
2
km Mass transfer coefficient; m /sec
k Thermal conductivity; W/m K
Km Overall mass transfer coefficient based on the gas system concentration
driving force
K Partition coefficient; dimensionless
m Mass of the mixture; kg in Equation (1.1)
m Solubility constant between the two phases in Equation (1.48)
2
m Mass flux of the mixture relative to fixed coordinates, kg/m sec in Equation
(1.11)
M Molecular weight; kg/kg mol
n Mole of the mixture; kg mol in Equation (1.4)
n Relative position in Equations (1.7) and (1.12)

n Mass bulk flux of the mixture relative to stationary coordinates, kg
2
mol/m sec
2
N Molar bulk flux of the mixture relative to fixed coordinates; kg mol/m sec
NEU Number of energy units
NTUD Number of mass transfer units
p Partial pressure; atm
P Pressure; atm
q Heat flow rate; W
r Radial coordinate
R Radius; cm or m in Equations (1.42) and (1.43)
R Gas constant; joules/g mol K in Equation (1.38)
S′ Shape factor
T Temperature; K
t Time; sec
u Mass diffusion velocity of the system relative to the mass bulk velocity; m/sec
U Molar diffusion velocity of the system relative to the molar bulk velocity; m/sec
v Mass bulk velocity of the mixture relative to stationary coordinates; m/sec
3
V Volume of the mixture, m in Equation (1.1)
3
V Molal volume of the system; m /kg mol in Equation (1.34)
V Molar bulk velocity measured with respect to fixed coordinates; m/sec
w Mass fraction of the mixture
x Rectangular coordinate
x Mole fraction of the mixture in Equation (1.29)
X Dimensionless time
z Rectangular coordinate
Z Height of a drier; m
GREEK SYMBOLS
2
α Thermal diffusivity; cm /sec
β Coefficient of thermal expansion; 1/K
δ Thickness of a hypothetical stagnant film; cm or m
ε Porosity
µ Viscosity; centipoises
2
ν Kinematic viscosity; m /sec
3
ρ Mass concentration of the mixture or fluid density; kg/m
σAB Collision diameter; °A
τ Tortuosity
ΩD Collision integral for molecular diffusion; dimensionless
ϕ Association parameter
REFERENCES
Crank, J., The Mathematics of Diffusion, 2nd ed., Oxford University Press, London, 1975.
Cussler, E.L., How we make mass transfer seem difficult, Chem. Eng. Educ., 18(3), 124–127,
149–152, 1984.

Geankoplis, C.J., Transport Processes and Unit Operations, 3rd ed., Prentice-Hall., London,
1993.
Gekas, V., Transport Phenomena of Foods and Biological Material, CRC Press, Boca Raton,
FL, 1992.
Khodaparast, K.A., Predict the number of transfer units for cooling towers, Chem. Eng.
Progress, 4, 67–68, 1992.
Le Goff, P., Performance energétique des echangeurs de matière et de chaleur: interprétation
energétique des analogies de Reynolds et de Colburn, Chem. Eng. J., 20, 197–209, 1980.
Sherwood, T.K., A review of the development of mass transfer theory, Chem. Eng. Educ., 3,
204–213, 1974.
Sherwood, T.K., Pigford, R.L., and Wilke, C.R., Mass Transfer, McGraw-Hill Kogakusha,
Ltd., Tokyo, 1975.
Treybal, R.E., Mass Transfer Operations, 3rd ed., McGraw-Hill International Editions, 1981.
Van den Bulck, E., Mitchell, J.W., and Klein, S.A., Design theory for rotary heat and mass
exchangers II. Effectiveness number of transfer units method for rotary heat and mass
exchangers, Int. J. Heat Mass Transfer, 28(8), 1587–1595, 1985.
Welty, J.R, Wicks, C.E., and Wilson, R.E., Momentum, Heat and Mass Transfer, 3rd ed, John
Wiley & Sons, New York, 1984.
White, F.M., Heat and Mass Transfer, Addison-Wesley, Reading, MA, 1988.

Heat Transfer in Food
2 Products
D.R. Sepúlveda and G.V. Barbosa-Cánovas
CONTENTS
2.1 Introduction
2.2 General Background
2.2.1 Thermal Properties of Foods
2.2.1.1 Specific Heat
2.2.1.2 Thermal Conductivity .
2.2.1.3 Thermal Diffusivity
2.2.1.4 Surface Heat Transfer Coefficient
2.2.2 Heat Transfer by Conduction
2.2.2.1 Steady State
2.2.2.2 Nonsteady State
2.2.3 Heat Transfer by Convection
2.2.3.1 Natural Convection
2.2.3.2 Forced Convection
2.2.4 Heat Transfer by Radiation
2.3 Conclusions
References
2.1 INTRODUCTION
Heating and cooling are common activities in food processing. Several operations
involving heating of raw foods are performed for different purposes, such as reduc-
tion of the microbial population, inactivation of enzymes, reduction of the amount
of water, modification of the functionality of certain compounds, and of course,
cooking. On the other hand, heat is removed from foods to reduce the rate of its
deteriorative chemical and enzymatic reactions and to inhibit microbial growth,
extending shelf life by cooling and freezing. Heat transfer plays a central role in all
of these operations; therefore, food engineers need to understand it in order to achieve
better control and avoid under- or over-processing, which often results in detrimental
effects on food characteristics. In practice, heat transfer to or from foods can be
attained either by indirect or direct methods. Indirect methods involve the use of
heat exchangers that isolate the product from the medium used as a source or sink

TABLE 2.1
Examples of Direct and Indirect Heating and Chilling
Heating Chilling
Direct Frying, boiling, baking, and grilling solid Fluidized bed individual quick freezing
foods (IQF)
Indirect Fluid food pasteurization; canned products Fluid food cooling; ice production
sterilization
of heat. Direct methods allow contact between the food and the heating/cooling
medium. Examples of these methods can be found in Table 2.1.
Indirect heating methods use gases and vapors, such as steam or air, and liquids,
such as water or organic compounds, as a source of thermal energy. Chilling by

indirect methods involves the use of coolant gases, such as ammonia or Suva , or
the use of coolant liquids, such as water or ethylene glycol. Direct heating can be
attained by means of hot air, oil, infrared energy, and dielectric or microwave
methods, among others. Direct chilling can be achieved by the use of cold air or by
the application of the Peltier effect.
2.2 GENERAL BACKGROUND

The first step in understanding heat transfer is to define what heat is and how it diffuses
through a single body or is transferred from one body to another. Heat is a nonme-
chanical form of energy transferred between regions of different temperature. Heat
transfer, therefore, is a natural energy transfer process in which energy tends to travel
from a hotter point to a colder point in order to reach an equilibrium temperature.
Now that we know that the temperature gradient is the driving force in heat
transfer processes, and therefore that if a temperature difference exists, energy
transference will occur, a couple of questions arise. How fast will this energy transfer
process occur? How will the energy diffuse through foods? The answers to these
questions are not easy. Great efforts have been made to try to answer these questions,
and several models have been developed to describe heat transfer behavior in dif-
ferent systems under different conditions.
The heat transfer mode governing the process is defined by the physical state of
the bodies and their relative position. If a heat gradient exists between two solid
bodies in contact, the heat transfer will proceed by conduction. If the same gradient
exists between two fluids, or between a fluid and a solid, the energy will be transferred
by convection. Finally, any body with a temperature above absolute zero will radiate
energy in the form of electromagnetic waves transferring heat by radiation. Besides
the physical state or relative position, other physical properties of the bodies involved
in these processes influence the heat transfer rate. Characteristics such as form, size,
structure, thermal conductivity, specific heat, density, and viscosity, among others,
are of paramount importance in the definition of the behavior of a system.
Early developments in the study of heat transfer in the chemical engineering
field assumed controlled situations dealing with well-defined substances with fixed

physical characteristics and clearly defined heat transfer modes. However, actual
situations in food engineering involve more than one mode of heat transfer simul-
taneously, and frequently some of the physical characteristics of food, such as
density, form, or viscosity, change as heat modifies the chemical structure, affecting
the food’s thermal behavior. Furthermore, foods usually have neither regular form
nor homogeneous or isotropic behavior. Finally, some particular features of food
being heated, such as nonuniform evaporation of water, crust formation, or closing
or opening of pores, are of such complexity that they make the modeling of this
process difficult or impracticable. Nevertheless, some of these drawbacks have been
overcome, and the modeling of several specific practical situations is possible, mainly
due to the development of knowledge of empirical relations that properly suit these
specific processes. Present-day analytical techniques, such as the finite element
method, allow for the modeling of situations characterized by nonuniform thermal
properties that change with time, temperature, and location, so that great develop-
ments can be expected in the modeling of heat transfer processes in foods.
The objective of this chapter is not to describe all of these specific models, but to
introduce the reader to a practical approach to the study of heat transfer in foods. Classic
models constructed over assumptions of homogeneity and isotropy will be introduced
in order to provide a basic knowledge that will enable the modeling of simple systems
and the understanding of more elaborate and specific models. Now we will focus on
some of the most important engineering properties of foods and how they can be
measured or calculated in order to use them in further modeling of heat transfer processes.
2.2.1 THERMAL PROPERTIES OF FOODS

As stated before, the modeling of heat transfer processes is dependent on some of
the physical properties of the foods involved. As mathematical techniques become
more elaborate, a higher accuracy is needed in the measurement or calculation of
properties such as specific heat, thermal conductivity, thermal diffusivity, and surface
heat transfer coefficient. These properties will be discussed below.
2.2.1.1 Specific Heat
Specific heat (Cp) is an exclusive property of every substance, and it is defined as

the amount of energy needed to increase the temperature of one kilogram of matter
by one degree Celsius; therefore, its units are J/kg°C. This property is not dependent
upon temperature or mechanical structure (e.g., density). It has been found that a
strong correlation exists between a food’s composition and its specific heat. Derived
from the definition of specific heat, the amount of heat Q required to increase the
temperature of a body with mass m from an initial temperature T1 to a final tem-
perature T2 is:
Q = m Cp (T2 – T1) (2.1)
In order to determine the Cp value for a specific substance or food, differential
scanning calorimetry (DSC) is used. Comprehensive data have been gathered, and
tables containing Cp values for many products are available in the literature (Amer-
ican Society of Heating, Refrigerating and Air-Conditioning Engineers, Inc., 1985).

However, as the water content and composition of foods have been found to affect
the Cp value, the data presented in the literature are bound to specific water contents
and formulations, thus reducing their usefulness. For a more practical way to find
the Cp value, several empirical mathematical expressions have been developed.
These expressions can vary from product to product and sometimes even from author
to author. Some of these expressions are based only on the water content, having
the form Cp = C1 + C2W, where W stands for water content and the constants are
defined depending on the situation and product. Examples of these expressions are:
Cp = 0.837 + 3.349W Siebel, 1982 (2.2)
Cp = 1.382 + 2.805W Dominguez et al., 1974 (2.3)
Cp = 1.470 + 2.720W Lamb, 1976 (2.4)
More complex expressions including other food components besides water have
been developed, and some examples are shown below.
Cp = 2.309Xf + 1.256Xs + 4.187W Charm, 1971 (2.5)
Cp = 1.424Xc + 1.549Xp + 1.675Xf + 0.837Xa + 4.187W

Heldman and Singh, 1981 (2.6)
where Xc stands for mass fraction of carbohydrates, Xp for proteins, Xf for fat, Xa
for ash, and W for water. Generic expressions for mixtures are also available:
Cp = ∑ (C Cp )
i
i i Choi and Okos, 1986a (2.7)
where Ci is the mass concentration of each constituent i and Cpi its corresponding Cp.
2.2.1.2 Thermal Conductivity
Thermal conductivity (k) is a characteristic that tells us how effective a material is

as a heat conductor. As stated in Fourier’s law for heat conduction, this constant is
a proportionality factor needed for calculations of heat conduction transfer processes.
This physical property can be directly measured from a food material using a
thermocouple and a heater, as described in detail by Mohsenin (1980). The suited
units for this property are W/m°C. Some data have been gathered and can be found
in the literature (American Society of Heating, Refrigerating and Air-Conditioning
Engineers, Inc., 1985). Thermal conductivity of foods depends mainly on the com-
position of the food, but factors such as fiber orientation and void spaces have an
influence on the heat flow paths through food; therefore, it is important to describe
the bulk condition in addition to the composition when reporting a k value. As in
the case of specific heat, some empirical expressions to calculate thermal conduc-
tivity values for different foods have been developed. Some examples are:
For fruits and vegetables:
k = 0.148 + 0.493W Sweat, 1974 (2.8)
where W is the mass fraction of water.

For sucrose solutions, fruit juices and milk:
−3 2
k = 1.73 × 10 (326.8 + 1.0412T – 0.00337T )(0.44 + 0.54W) Riedel, 1949
(2.9)
where T is temperature expressed in degrees Celsius.
Other applicable more general expressions for mixtures are of the type:
k= ∑ (k X )
i
i
v
i (2.10)
th v
where ki is the thermal conductivity of the i component and Xi its volume fraction.
When heat is flowing through wrappings or compound layer materials, a total thermal
conductivity coefficient is needed. This expression can be calculated if the individual
thermal conductivity coefficients are known.
For heat flowing parallel to two layers, the total thermal conductivity coefficient
is given by
kT = k1 (1 – c) + k2c Hallstrom et al., 1988 (2.11)
where c is the volume fraction of material two. On the other hand, if the heat flow
is perpendicular to the material’s layer orientation:
k1k 2
kT = Hallstrom et al., 1988 (2.12)
ck1 + (1 − c)k 2
In the case of material mixtures with random size and orientation particles, the
value for the total thermal conductivity value will be found between the value for
parallel flow and the value for perpendicular flow. For mixtures of more than two
components, the same method is followed, taking two materials at a time.
2.2.1.3 Thermal Diffusivity
Thermal diffusivity (α) is a compounded thermal property of materials and is

calculated from the values found for thermal conductivity, specific heat, and density
of a particular product.
k
α= (2.13)
Cpρ
where k is thermal conductivity, Cp specific heat, and ρ mass density. This thermo-
physical property links conductivity of the materials with their ability to store heat,
thereby showing how heat will diffuse throughout the materials when heated. The units
2
for thermal diffusivity are m /sec. Although the recommended method to determine
thermal diffusivity is a calculation based on experimentally measured values of
thermal conductivity, specific heat, and density, other heat diffusivity measurement
methods have been developed (Choi and Okos, 1983). Expressions based on water
content and temperature of foods have also been developed. Some examples are:
–8 –10
α = 5.7363 × 10 W + 2.8 × 10 T Martens, 1980 (2.14)

where W is the mass fraction of water and T is the temperature expressed in degrees
Kelvin, and
–8
α = 8.8 × 10 (1 – W) + α wW Dickerson, 1969 (2.15)
where α w is the thermal diffusivity of water at the studied temperature.
As in the cases of other properties, the thermal diffusivity of mixtures can be
calculated with a general expression:
α= ∑ (α X )
i
i i Choi and Okos, 1986b (2.16)
th
where αi is the thermal diffusivity of the i component and Xi its mass fraction. As
thermal diffusivity can be calculated from other thermal properties, data are not
frequently found in the literature.
2.2.1.4 Surface Heat Transfer Coefficient
The heat transfer coefficient (h) is not a property of materials themselves, but rather
a property of convective heat transfer systems involving a solid surface and a fluid.
This coefficient is used as a proportionality factor in Newton’s law of cooling,
adjusting for the characteristics of the system under study.
To define the value of this factor, it is necessary to characterize the convective
medium and the surface involved in the convective heat transfer process. Some of
the characteristics involved in the calculation of the heat transfer coefficient are the
fluid’s velocity, viscosity, density, thermal conductivity, and specific heat. The form
and surface texture of the solid involved are also important. As can be determined
from a dimensional analysis of Newton’s cooling law, the units for the heat transfer
2
coefficient are W/m °C. Since the heat transfer coefficient is a property of the system
rather than of the material, its measurement is difficult, and several empirical expres-
sions have been developed to overcome this problem. Some of these expressions
will be reviewed below in the section dealing with heat transfer by convection.
A compilation of surface heat transfer coefficient data and empirical expressions
to calculate this coefficient can be found in the 1985 edition of the ASHRAE
Handbook of Fundamentals. Further information regarding measurement of the heat
transfer coefficient can be found in the literature (Arce and Sweat, 1980).
Now that we have shown methods for determining the most relevant thermal
properties of foods, we will find out how to use them to model heat transfer processes.
The particulars of the different heat transfer modes will be dealt with in the following
sections.
2.2.2 HEAT TRANSFER BY CONDUCTION

Heat transfer in solids or highly viscous materials takes place by conduction. In this
mode, energy is transferred among particles touching each other with no movement
of material. As a solid material is heated on one of its faces, a gradient is established
between the hot face and the opposite cooler face. This gradient is the driving force
promoting the heat flow from one face to the other. As heat penetrates the body,

the interior temperature changes from point to point and across time. This period of
time is known as the unsteady state period. Later, when heat has traveled all the
way across the body and equilibrium in temperatures has been reached, the interior
temperature of each point will remain the same with respect to time and will only
depend on its relative position inside the body. At this moment, the steady state
transfer regime has been reached, and the body is working as a heat conductor with
a determined heat flux going through it.
Thus, the study of heat conduction can be divided into two main areas: the study
of heat conduction in the steady state and the study of heat conduction in the
nonsteady state.
2.2.2.1 Steady State
The study of heat conduction in the steady state is useful in modeling the perfor-
mance of insulators, heat exchangers, and other equipment used to transfer heat from
one point to another, such as containers, pans, and walls. In these, the initial varia-
tions in internal temperature dependent on time have settled, and the temperature
profile inside the material is stationary. The important issue here is to determine the
amount of heat a particular material of a given thickness will allow to flow through it.
This mechanism can be modeled using Fourier’s law for heat conduction
(Equation 2.17), which establishes that the heat flux Qx transmitted through a solid
in the direction x is inversely proportional to the thickness x and directly proportional
to both the perpendicular transmission area A and to the temperature difference
between its two opposite faces ∆T. The proportionality constant needed by this model
is the thermal conductivity (k), one of the physical characteristics previously
described. In some materials, thermal conductivity may vary with temperature. In
these situations, the value corresponding to the average temperature should be used.
∂T(x)
Q x = − kA (2.17)
∂x
The negative sign represents the heat flow from the hottest to the coolest surface,
thereby rendering a positive value for the heat flux. As can be seen, this equation
describes heat flow only in one direction. For a complete mathematical description, we
would need to write similar equations for the other two directions in a three-dimensional
system and to integrate over the entire volume. However, most steady state processing
applications involve heat conduction in only one direction, as when heat flows across
walls or heat exchangers. For practical purposes, these materials can be considered as
infinite slabs, so we do not need to be concerned with a general mathematical solution.
A∆T
Qx = − k (2.18)
x
Equation (2.18) is the integrated form of Fourier’s law for unidirectional steady
state heat conduction over a path of constant cross-sectional area in a parallelepiped.
It can be used directly to calculate the heat flux through a body. Besides heat flowing
through flat surfaces, another common situation in food engineering is the use of

cylindrical containers or pipes; therefore, an expression for Fourier’s law on cylindrical
surfaces is necessary. That expression is shown in Equation (2.19),
A lm ∆T
Qx = − k (2.19)
x
where all the terms stand for the same characteristics as in the previous expression
except for Alm, which in this case is the logarithmic mean of the inner and outer areas:
A1 − A 2
A lm = (2.20)
ln 1 A 
A
 2
Another common situation is the presence of compounded walls. The introduc-

tion of the concept of thermal resistance can be of help when studying heat conduc-
tion in this kind of system. If thermal resistance R is defined as the ratio of the
thickness x over the area A and thermal conductivity k,
x
R= (2.21)
kA
Fourier’s law takes a form identical to Ohm’s law for electric current flow, and all
mathematical manipulations can be performed as in electrical calculations.
∆V
I= (2.22)
R
∆T
Q= (2.23)
R
Here, the flow of electric current I is directly proportional to the voltage differ-
ence ∆V and inversely proportional to the electric resistance R. In the same way,
the heat flow Q is directly proportional to the temperature difference ∆T and inversely
proportional to the thermal resistance R. This analogy shows that in the case of
several different layers placed in series (normal heat flow), the overall temperature
difference is the sum of the individual temperature differences, and the same Q flows
through all the resistances. Therefore, the total thermal resistance is simply the sum
of the individual resistances.
On the other hand, when there is parallel heat flow through several layers, the
analogy indicates that we have a parallel system. Therefore, the total Q is the sum
of the Qx through the individual resistances, and the temperature differences for the
individual resistances are all the same and equal to the overall temperature difference.
In this case, the reciprocal of the total thermal resistance is equal to the sum of the
reciprocals of the individual resistances. The use of these analogies allows us to
predict heat transfer in compound systems.
2.2.2.2 Nonsteady State
The study of heat conduction in the nonsteady state is pertinent when calculating
processes in which the focus is to heat or cool a body instead of using it as a heat
conduction medium. Such processes include freezing, cooking, and thermal sterilization

of foods. In these cases, the main concern is to find out how long it will take the
coldest/hottest point in the body to reach the desired temperature. Moreover, the
study of this phenomenon allows us to determine the time needed to process foods at
a desired temperature or the temperature at a determined point at a given time. In
nonsteady state heat transfer processes in which more than one heat transfer mode
applies, conduction usually governs the process, as it is the slowest heat transfer mode.
It is important to consider that heat conduction in foods is frequently a three-
dimensional phenomenon, as the food has finite dimensions and sometimes is
immersed in the heat transfer medium, with heat being transferred through all its
surfaces (as in oven baking or deep fat frying). Fourier’s second law of heat transfer
for three-dimensional nonsteady state heat conduction states that:
∂T  ∂2 T ∂2 T ∂2 T 
= α 2 + 2 + 2  (2.24)
∂t  ∂x ∂y ∂z 
where T stands for temperature, t for time, x, y, and z for the distance on the x, y
and z axes, respectively, and α for thermal diffusivity, which is a physical character-
istic of the materials, as previously discussed. To arrive at the analytical solution to
this complex expression can be difficult or impracticable. However, the analysis of
some practical situations may be simplified through a couple of useful assumptions.
The first assumption supposes that we are dealing with a semi-infinite body, also
known as a thick solid. This semi-infinite body is defined as one with infinite width,
length, and depth. If a body with these characteristics is immersed in the heating
medium, we can assume that heat will be transferred just from the surface toward
the interior, following a straight trajectory to the center; therefore, Fourier’s law can
be transformed into:
∂T ∂2 T
=α 2 (2.25)
∂t ∂x
where the x-axis corresponds to any one of the dimensions on a parallelepiped or
to the radius on a sphere-like body. The solution to Equation (2.25) becomes simpler
now and may be obtained by applying the boundary conditions, which are:
T0 Initial temperature of the body at time 0

Tm Heating medium temperature acquired at the surface when immersed in
the fluid.
The solution takes the form of Equation (2.26), where the temperature T at any
point x, measured from the surface, can be determined using a dimensionless tem-
perature ratio:
2
hx  h
Tm − T  x  +   αt
 k   x  h αt 
= erf   +e
k
 erf  +  (2.26)
Tm − T0  4αt   4αt  k 
where erf is the Gauss’ error function, which can be obtained from Table 2.2, and k
is the thermal conductivity.

TABLE 2.2
Gauss’ Error Function
η η)
erf (η η η)
erf (η η η)
erf (η
0.00 0.00000 0.68 0.66278 1.80 0.98909

0.04 0.45110 0.72 0.69143 1.90 0.99279
0.08 0.09008 0.76 0.71754 2.00 0.99532
0.12 0.13476 0.80 0.74210 2.10 0.99702
0.16 0.17901 0.84 0.76514 2.20 0.99814
0.20 0.22270 0.88 0.78669 2.30 0.99886
0.24 0.25670 0.92 0.80677 2.40 0.99931
0.28 0.30788 0.96 0.82542 2.50 0.99959
0.32 0.34913 1.00 0.84270 2.60 0.99976
0.36 0.38933 1.10 0.88020 2.70 0.99987
0.40 0.42839 1.20 0.91031 2.80 0.99993
0.44 0.46622 1.30 0.93401 2.90 0.99996
0.48 0.50275 1.40 0.95228 3.00 0.99998
0.52 0.53790 1.50 0.96610 3.20 0.999994
0.56 0.57162 1.60 0.97635 3.40 0.999998
0.60 0.60386 1.70 0.98379 3.60 1.000000
0.64 0.63459
Since, in this case, the heat is transferred from a fluid to a solid surface, the
surface heat transfer coefficient h is incorporated into the solution. For situations
where the heat transfer between the fluid and the solid proceeds very efficiently, that
is, if h is infinite, the solid surface takes the medium temperature instantaneously,
and Equation (2.26) can be simplified to:
Tm − T  x 
= erf   (2.27)
Tm − T0  4αt 
Now that we know how to handle semi-infinite bodies, a problem arises. The
definition of a semi-infinite body describes a body with infinite dimensions, which
in reality is not a possible situation. When can a body be considered as a semi-infinite
body for practical purposes? The concept of a semi-infinite body in practice is better
related to the system’s behavior than to the body dimensions. The surface heat
transfer coefficient, along with the thermal conductivity, plays a fundamental role
in determining whether a body will exhibit a thick body response. If a finite body
of a given thickness is studied in the early steps of heat penetration, it will exhibit
a semi-infinite body response as heat has only flowed from the outside to the center;
therefore, the ratio of thickness to time plays an important role as well. Schneider
(1973) found a critical Fourier number to define when a body ceases to exhibit a
thick body response:
–0.3
Focritical = 0.00756 Bi + 0.02 for 0.001 ≤ Bi ≥ 1000 (2.28)

The Fourier and Biot numbers are:
αt
Fo = (2.29)
( L )2
hL
Bi = (2.30)
k
where L is half the thickness of the body and t is the time the body has been exposed
to the conditions studied. If the actual Fourier number exceeds the critical value,
the body can no longer be considered to be a semi-infinite body, and a different
approach must be taken.
Another possible approximation used to solve practical problems regarding heat
conduction in a nonsteady state involves the assumption of infinite bodies with
simple geometry. Again, the concept of an infinite body is just theoretical, as in
practice no such bodies occur and, therefore, a practical definition is needed. An
infinite body is a body in which two of its dimensions are much larger than the third.
In this situation, it can be expected that heat will reach the center of the body first
traveling the shortest way; that is, following the axis corresponding to the thinner
dimension. Heat transfer through the remaining axes becomes negligible. This
assumption applies to infinite slabs with thickness 2xo and infinite longitude and
width, infinite cylinders with radius r and infinite length, and spheres.
Analytical solutions for this kind of problem can be developed using dimension-
less ratios. Expressions for temperature Y and position n are:
Tm − T
Y= (2.31)
Tm − T0
x
n= (2.32)
x0
where Tm is the temperature of the cooling or heating fluid surrounding the solid,
T0 is the initial temperature of the body, T is the temperature at a point x, x0 is the
distance from the center or midplane to the surface, depending on the body’s shape,
and x is the distance from the center or midplane to the selected point. Time and
thermal diffusivity are introduced using Fourier module τ, while surface heat transfer
coefficient and thermal conductivity are both included using the Biot module in m:
αt
τ = Fo = (2.33)
x 20
1 k
m= = (2.34)
Bi hx 0
Modifying Equation (2.25), we obtain:
∂T ∂2 Y
=α 2 (2.35)
∂t ∂n

which is the dimensionless form for Fourier’s second law. Applying boundary con-
ditions, Equation (2.35) can be analytically solved by partial derivatives for different
situations. However, the analytical solutions for an infinite slab, an infinite cylinder,
and a sphere have already been developed and can be found in graphic form as
shown in Figures 2.1, 2.2, and 2.3.
Using these figures, it is possible to find the Y value for a given set of conditions.
First, the correct group of lines is chosen based on the calculated m value. Next,
one of the lines is picked depending on the n value. Finally, by finding the intersection
between the selected line and the calculated Fourier modulus τ, the proper Y value
will be determined. Once the Y value is obtained, only a simple substitution from
Equation (2.31) is needed.
A deviation from the assumption of an infinite body is apparent in several cases
where the ratio of length or width to thickness is not too large. In these cases, the
application of Newman’s rule can be of help. Newman demonstrated that for a finite
solid body being heated or cooled, the internal variation of temperature as a function
of time and position could be stated as:
Y = YxYyYz (2.36)
1
m=∞
m=6 x x
0
m
=2
m
=2
n = 1.0
0.8
m
0.6
=
1
0.1 0.4
m
0.2
=
0.0
1
m=
0.5
m=
Y
0.5
n = 1.0
0.8
m=
0.6
m=
0.4
0.2
0
n = 1.0 0.0
0.01 0.8
0.6
0.4
0.2
n = 0.8 0.0
0.6
0.4
0.2
0.0
m=0
n=1
0.001
0 0.5 1 1.5 2 2.5 3 3.5
τ = (Fo)
FIGURE 2.1 Dimensionless temperature chart for an infinite cylinder.

1 m=∞
x x?
m=6 x?
m= n = 1.0
2 0.8
0.6
m= 0.4
2 0.2
0.0
0.1
m
=
1
m
n = 1.0
=
0.8
1
0.6
0.4
Y 0.2
0.0
m
=0
.5
m
=0
.5
0.01 m=
m=
0
n = 1.0
0
0.8
0.6
0.4
0.2
0.0
n = 0.8
m=0 0.6
n=1 0.4
0.2
0.0
0.001
0 1 2 3 4 5 6
τ = (Fo)
FIGURE 2.2 Dimensionless temperature chart for an infinite slab.
where Y is the dimensionless temperature defined in Equation (2.31), and values Yx,
Yy and Yz are the dimensionless temperature values with respect to the x, y, and z axes,
respectively, which can be obtained from Figures 2.1, 2.2, and 2.3. Newman’s rule
can be applied in the calculation of heat transfer processes on finite parallelepipeds
and cylinders, as it can be understood that a finite body results from the conjunction
of three infinite bodies.
2.2.3 HEAT TRANSFER BY CONVECTION

Heat transfer within a fluid will occur by convection. In this heat transfer mode,
energy flows as a result of bulk movement of the fluid due to a temperature gradient.
The molecules in the fluid will move due to density changes and will interact with
each other at different points of the fluid, exchanging energy. Since the efficiency
of this process depends on the extent of mixing within the fluid, flow characteristics
are as important as thermal properties in determining heat flow rate. Most processing
applications of heat transfer by convection involve steady state heat transfer from a
solid surface to a fluid in contact with it or vice versa. Heat transfer is defined as
the rate of heat flowing through the interface between the fluid and the solid. The
amount of energy flowing through this interface is proportional to the temperature
gradient and to the interchange surface. This relationship is defined by Equation (2.37),

1
m=∞
x x
m= 0
6
m
=
2
m
0.1 =
2
m=
m=
n = 1.0
1
0.8
1
m=
0.6
Y
m=
0.4
0.5
n = 1.0 0.2
0.5 0.8 0.0
n = 1.0 0.6
0.8 0.4
m=0
0.6 0.2
m=0
0.4 0.0
0.2
0.0
0.01
n = 0.8
0.6
0.4
0.2
0.0
m=0
n=1
0.001
0 0.5 1 1.5 2 2.5 3 3.5
τ = (Fo)
FIGURE 2.3 Dimensionless temperature chart for a sphere.
known as Newton’s law of cooling:

Q = hA ∆T (2.37)
where Q corresponds to heat flux, A to the interchange area, ∆T to the difference
between the fluid and solid temperatures, and h to the proportionality coefficient,
known as the heat transfer coefficient.
Bulk molecular motion can be induced by differences in the fluid’s temperature
at different points within it, developing a buoyant force. This process is known as
natural convection. The coefficient of thermal expansion of a fluid (β) is the main
property governing natural convection. Without the existence of gravity and thermal
expansion, natural convection would not be possible. Mixing efficiency in natural
convection depends on the temperature gradient. A small temperature difference
between the fluid and solid in contact will promote weak currents with a low heat
transfer coefficient. On the other hand, when a fluid is forced to flow past a surface
by mechanical means such as a pump or a fan, higher velocities are obtained and
strong currents are induced regardless of natural convection. High heat transfer
coefficients can be reached due to more efficient mixing. This regime is known as
forced convection. In practice, forced convection is the most used convective heat
transfer mode, as greater heat transfer can be accomplished and better control of the
system can be easily established.

As stated by Newton’s cooling law, heat flux is proportional to the contact area
and temperature gradient, both easily measurable. However, several problems arise
when determining the proportionality constant h. This constant depends on several
factors, including the fluid’s properties such as viscosity, density, specific heat, and
thermal conductivity; the nature of the flow (i.e., its velocity, natural or forced
convection, streamline or turbulent flow); and other physical characteristics of the
system such as size and shape. In practice, exact derivation of heat transfer coeffi-
cients from the basic fluid flow and heat conduction equations is not possible, and
the use of empirical correlations is needed. These empirical correlations, which have
been developed from a theoretical basis and experimental observations, are expressed
in dimensionless numbers, allowing us to apply these generic expressions to different
fluids and systems.
A basic general dimensionless expression that connects the heat transfer coef-
ficient to particular characteristics of fluids and systems has been proposed. This
expression states that the Nusselt number Nu is proportional to the product of the
Reynolds (Re), Prandtl (Pr), and Grashof (Gr) numbers, as shown in Equation (2.38):
Nu = φ [(Re)(Pr)(Gr)] (2.38)
The Nusselt number is a dimensionless form for the heat transfer coefficient.
The other factors involved in this ratio are the thermal conductivity of the fluid k
and the characteristic dimension of the system d, which is the diameter for a round
pipe or the length for a flat surface.
hd
Nu = (2.39)
k
The Reynolds number introduces information about the fluid characteristics and
flow regime. It can be considered as the ratio of macroscopic flow to internal friction.
When this ratio exceeds a certain value, the inertial force predominates, converting
flow from a laminar form into a turbulent one. This number involves the characteristic
dimension d, and the fluid’s properties density ρ, viscosity η, and velocity v. For
physical properties such as viscosity or density that vary with temperature, the value
at the arithmetic mean temperature between the inlet and outlet points will be used.
ρvd
Re = (2.40)
η
The Prandtl ratio deals only with physical properties of the fluid and behaves
as a physical constant. This expression involves specific heat Cp, viscosity η, and
thermal conductivity k.
Cpη
Pr = (2.41)
k
Finally, the Grashof number represents the ratio of buoyancy to internal friction.
This quantity involves the characteristic dimension of the system d, the acceleration

due to gravity g, the thermal expansion coefficient β, the density of the fluid ρ, the
viscosity η, and the temperature difference between a surface and the fluid ∆T:
β g ∆T d 3ρ2
Gr = (2.42)
η2
As can be seen, all the process variables included in these dimensionless ratios,
with the exception of h, can be measured; therefore, a heat transfer coefficient value
for a given set of conditions can be calculated using Equation (2.38). However, a
difficulty remains, as the exact proportionality factor has not been stated. This exact
proportionality factor varies from situation to situation, and empirical values have
been found for several specific situations, as a general expression is not possible.
Equation (2.38) can be further modified into two generic expressions. From simple
examination of the meaning of each of the dimensionless ratios, it is apparent that
when dealing with natural convection, the buoyancy effect governs the process, and
the importance of the Reynolds number subsides under the importance of the Grashof
number, leading to:
Nu = φ [(Pr)(Gr)] (2.43)
On the other hand, Equation (2.38) can be practically modified for forced convec-
tion as the Reynolds number turns out to be more important than the Grashof number
under this flow regime; hence:
Nu = φ [(Pr)(Re)] (2.44)
Now we will review some empirical expressions developed for particular, though
frequent, situations. More information about expressions regarding heat transfer by
convection in different situations is found extensively throughout the specialized
literature.
2.2.3.1 Natural Convection
The most common expression used for natural convection in Newtonian fluids is:
a
Nu = K [(Pr)(Gr)] (2.45)
where values for constants K and a in some specific situations are given in Table 2.3.
2.2.3.2 Forced Convection
The relationship most commonly used for turbulent flow inside tubes is known as
the Dittus–Boelter equation:
0.8 n
Nu = 0.023 (Re) (Pr) (2.46)
where n = 0.4 for a fluid being heated or n = 0.3 for a fluid being cooled. This
4
expression is valid for Re > 10 and 0.7 < Pr < 160.

TABLE 2.3
Values of K and a for Equation (2.45)
Configuration (Pr)(Gr) K a
4
Vertical surfaces <10 1.36 1/5
4 9
L = vertical dimension 0.9 m 10 . < (Pr)(Gr) < 10 0.59 1/4
9
>10 0.13 1/3
–5
Horizontal cylinder <10 0.49 0
–5 –3
L = diameter 0.2 m 10 < (Pr)(Gr) < 10 0.71 1/25
–3
10 < (Pr)(Gr)r < 1 1.09 1/10
–4
1 < (Pr)(Gr) < 10 1.09 1/5
–4 9
10 < (Pr)(Gr) < 10 0.53 1/4
9
>10 0.13 1/3
5 7
Horizontal flat surfaces 10 < (Pr)(Gr) < 2 × 10 (FU) 0.54 1/4
7 10
2 × 10 < (Pr)(Gr) < 3 × 10 (FU) 0.14 1/3
5 10
3 × 10 < (Pr)(Gr) < 3 × 10 (FD) 0.27 1/4
Note: FU = Facing upward; FD = Facing downward.
Data from Heldman, D.R., and Singh, R.P., Food Process Engineering, 2nd ed., AVI, Westport, CT, 1981.
For liquid flowing inside tubes in a laminar flow (Re < 2100), a suitable equation
is
1 0.14
 d  3 η 
Nu = 1.86 (Pr)(Re)    (2.47)
  L    ηW 
where d/L is the diameter/length ratio and η/ηW is the ratio of the bulk viscosity to
the viscosity at the wall.
The equation used for a liquid flowing in turbulent flow outside a solid body is
0.52 0.3
Nu = [0.35 + 0.47(Re) ] (Pr) (2.48)
and the equation for a liquid flowing in laminar flow (Re < 200) outside a solid
body is
0.43 0.3
Nu = 0.86(Re) (Pr) (2.49)
2.2.4 HEAT TRANSFER BY RADIATION

Heat radiation is another way to dissipate energy. Any body with a temperature
above absolute zero emits electromagnetic radiation. The wavelength of this radiation
varies as a function of the body temperature. The higher the temperature, the more

energetic the radiation; therefore, the smaller the wavelength. Heat radiation does
not need a material in which to propagate and can travel through a vacuum. Addi-
tionally, heat transfer by radiation does not require a temperature gradient to proceed
and therefore occurs constantly throughout nature. However, for practical purposes,
use of heat transfer by radiation in food engineering is limited to the use of infrared
radiation, dielectric heating, and microwave heating.
Use of infrared radiation implies the use of electromagnetic radiation with
wavelengths between visible light and radio waves (0.76–1000 µm). Often, the infra-
red source has a high temperature (500–3000°C), and heat transfer by convection
is also taking place and cannot be ignored unless the process occurs under vacuum,
as in the case of freeze drying. Examples where heat transfer by infrared radiation
is present are grilling and the use of electrical resistances. As penetration of this
kind of radiation is poor, the heating effect of infrared radiation has an impact only
on the surface of the body, and heat transfer through the body proceeds by conduction
or convection. Although infrared radiation is almost always present in heat transfer
processes, generally its effect is not as important as the effect of convection, and its
contribution has already been taken into account by the empirical equations used to
model heat transfer by convection.
Dielectric heating such as microwave or radio frequency heating is generally
used when large objects need to be quickly and uniformly heated. The principle
underlying the operation of these methods lies in the ability of some wavelengths
to induce vibration in some dipolar molecules such as water, producing intermolec-
ular friction and thereby increasing the temperature. Using these methods, food
products are heated volumetrically, that is, at all points at the same time. The
frequencies used for radio frequency heating are in the range of 10 to 100 MHz,
while the frequencies used for microwave heating are a little higher, normally 915
to 2450 MHz.
The dielectric heating methods described above involve the “instantaneous”
generation of heat within the product. Conduction and convection take command of
the heat transfer process after heat has been generated. The study of heating processes
such as microwave heating, radio frequency heating, and ohmic heating is beyond
the scope of this chapter, and no further details will be discussed here.
2.3 CONCLUSIONS
The modeling of heat transfer in foods is a difficult task. Often, two or even three
heat transfer modes proceed in a system at the same time. Some thermal properties
of foods can vary with changes in temperature, and further problems arise because
food is seldom regular in shape or homogeneous. However, some assumptions and
empirical relations allow the development of practical models that describe certain
processes with sufficient precision. Nowadays, some efforts are being made to apply
finite element method to take into account the changing properties of foods and to
better model complex food heating or cooling processes. Most empirical heat transfer
models applicable to foods are highly specific, and general analytical models are
seldom encountered.

REFERENCES
American Society of Heating, Refrigerating and Air-Conditioning Engineers, Inc., ASHRAE
Handbook of Fundamentals, American Society of Heating, Refrigerating and Air-
Conditioning Engineers, Inc., Atlanta, 1985.
Arce, J.A. and Sweat, V.E., Survey of lashed heat transfer coefficients encountered in food
refrigeration processes, ASHRAE Trans., 86(2), 235–260, 1980.
Charm, S.E., Fundamentals of Food Engineering, AVI, Westport, CT, 1971.
Choi, Y. and Okos, M.R., The thermal properties of tomato juice concentrates, Trans. ASAE,
26, 305–311, 1983.
Choi, Y. and Okos, M.R., Effects of temperature and composition on the thermal properties
of foods, in Food Engineering and Process Applications, vol. 1, Maguer L. and Jelen,
P., Eds., Elsevier, New York, 1986a.
Choi, Y. and Okos, M.R., Thermal properties of liquid foods: review, in Physical and Chemical
Properties of Foods, Okos, M.R., Ed., American Society of Agricultural Engineers,
St. Joseph, MI, 1986b.
Dickerson, R.W., Thermal properties of foods, in The Freezing Preservation of Foods, vol.
2, 4th ed., Tressler, D.K., Van Arsdel, W.B., and Copley, M.J., Eds., AVI, Westport,
CT, 1969.
Dominguez, M., De Elvira, C., and Fuster, C., Influence of air velocity and temperature on
the two-stage cooling of perishable large-sized products, Annexe Bressanone, Bull.
IT Regrig., Annexe 83–90, 1974.
Hallstrom, B., Skjoldebrand, C., and Tragardh, C., Heat Transfer and Food Products, Elsevier,
New York, 1988.
Heldman, D.R. and Singh, R.P., Food Process Engineering, 2nd ed. AVI, Westport, CT, 1981.
Lamb, J., Influence of water on the thermal properties of foods, Chem. Ind., 24, 1046–1048, 1976.
Martens, T., Mathematical model of heat processing in flat containers, in Operaciones Uni-
tarias en la Ingenieria de Alimentos, Ibarz, A. and Barbosa-Canovas, G., Eds.,
Technomic Publishing Company, Lancaster, PA, p. 317.
Mohsenin, N.N., Thermal Properties of Foods and Agricultural Materials, Gordon and Breach
Science Publishers, Inc., New York, 1980.
Riedel, V.L., Wärme leitfähigkeitsmessungen an Zuckerlösungen, Frucht säften und Milch,
Chem. Ing. Technik., 21, 340, 1949.
Schneider, P.J., Conduction, in Handbook of Heat Transfer, Rohsenow, W.M. and Hartnett,
J.P., Eds., McGraw-Hill, New York, 1973.
Siebel, J.E., Specific heat of various products, Ice Refrigeration, 2, 256–257, 1982.
Sweat, V.E., Experimental values of thermal conductivity of selected fruits and vegetables,
J. Food Science, 39, 1080, 1974.

Introductory Aspects
3 of Momentum Transfer
Phenomena
J.F. Vélez-Ruiz
CONTENTS
3.1 Introduction
3.2 Momentum Transfer Variables
3.2.1 Flux of Momentum
3.2.2 Mass Conservation
3.2.3 Energy Balance
3.3 Laminar and Turbulent Flow
3.3.1 Laminar Flow
3.3.2 Turbulent Flow
3.3.3 Transportation of Fluids
3.4 Rheological Properties of Foods
3.4.1 Rheology
3.4.2 Rheological Models
3.4.3 Temperature and Concentration Variables
3.5 Simultaneous Transfer Phenomena
3.6 Final Remarks
Nomenclature
References
3.1 INTRODUCTION
Momentum transfer is a physical phenomenon present in almost any process of the
food industry; often the heat and/or mass transfer phenomena occur in association
with flow, and it is difficult to imagine a unit operation without moving streams.
This phenomenon necessarily involves a convection mechanism between molecules
or groups of molecules, or the momentum gradient would be null. In other words,
momentum transfer is characterized by the tendency toward equilibrium.
When momentum transfer is analyzed in the food fluid field, some particular
considerations should be taken into account. Foodstuffs are biological materials
consumed by humans and animals for nutritional purposes; in order to process the

final food products, the raw food material must be transformed to achieve the proper
and desirable properties, providing a diversity of satisfactory factors.
A food may be considered a multi-component mixture in which carbohy-
drates, lipids, proteins, and water are the macro constituents, and minerals and
vitamins, among others, are the micro components. The type of component, its
concentration, and its specific characteristics play important roles in the structure and
engineering properties of each food product, particularly in fluid motion. Food
materials are influenced by many aspects such as variety, time of harvesting, ripeness
stage, handling during transport, and of course, by process treatments. The non-
Newtonian behavior of many food fluids makes transfer momentum a complicated
phenomenon.
To explain transfer phenomena, a rigorous mathematical approach leads to differ-
ential equations that often are too difficult to be solved analytically, especially when
a transient instead of a steady state condition is involved; furthermore, the presence
of many molecules or groups of molecules in natural or forced convection complicates
analytical solution. For this reason, empirical and numerical methods have been devel-
oped to reach faster, more practical, and useful solutions.
In food processing, the utilized raw materials are exposed to process conditions
that transform, to a minor or major degree, the food’s native state. Differences in
concentration, mechanical force, pressure, temperature, and/or velocity, which act as
driving forces of the three transport phenomena, importantly affect the food product’s
characteristics. Thus, mathematical and/or engineering modeling favors the predict-
ability of those transport phenomena, particularly of momentum transfer, in order to
control food quality and to produce a well specified end product.
The fundamentals and applications of momentum transfer are themes widely
covered by many authors. Therefore, the main purpose of this chapter is to present
the basic principles and main process variables involved in momentum transfer
phenomena. Two major fluid motions are introduced: laminar and turbulent flows.
Rheological properties and simultaneous transfer phenomena are commented on
briefly, and finally, some general comments are given.
3.2 MOMENTUM TRANSFER VARIABLES

The momentum of a fluid may be defined as the product of its mass and velocity at
a given point; hence, changes in velocity per unit mass can result in momentum
transport. Therefore, momentum transfer or fluid motion depends upon the interre-
lation of three fundamental variables: mass, velocity, and time (Bennet and Myers,
1983; Fahien, 1983).
3.2.1 FLUX OF MOMENTUM

Considering that the velocity is a vector and the velocity gradient is a second-order
tensor, the corresponding moment flux or shear stress is also a second-order tensor,

which for an incompressible fluid is given by the following equation (Brodkey and
Hershey, 1988):
τ = − µ[∇v + (∇v)T ] (3.1)
Equation (3.1) shows that the stress tensor (τ) is a function of the shear rate
T
tensor (∇v) and its transpose (∇v) .
Velocity, a vector quantity, has three components, and any of these can vary in
three directions. Since Equation (3.1) must be homogeneous, the stress tensor (ττ)
must be a second-order tensor:
 τ xx τ xy τ xz 
 
τ =  τ yx τ yy τ yz  (3.2)
 
 
 τ zx τ zy τ zz 
This stress tensor has a complicated physical interpretation due to the fact that it
is utilized both as a momentum flux and as a shear stress. The application/interpretation
of this stress tensor, or force imposed on a unit of surface area, for a given material
is conducted as a function of the specific conditions controlling a physical situation;
for instance, in a steady simple shear flow the number of components of the stress
tensor is reduced to five (Rao, 1999; Steffe, 1992).
Because the complete analysis of momentum transfer is too complicated, the
solution for each particular physical situation has been studied and solved by many
researchers, using both simple and complex analytical methods (Gekas, 1992;
Toledo, 1991). And even though the solution for many practical situations has been
developed, many physical phenomenon problems involving food fluids remain to be
solved. Furthermore, whatever the physical problem, the elementary variables are
dimensions of the system, involved forces, particular properties of the process
material, shear and normal stresses, time, and velocities, among the most important.
Most of these variables are combined in those driving force balances known as
dimensionless numbers, in which the variable’s participation depends on the physical
phenomenon. Table 3.1 includes the common dimensionless numbers related to
momentum transfer of Newtonian fluids; the list could be extended if non-Newtonian
behavior were considered (Bennet and Myers, 1983; Fahien, 1983; Welty et al.,
1976; Vélez-Ruiz, 2001).
3.2.2 MASS CONSERVATION

Sometimes it is not necessary to formulate a complete force balance in the solution of
a new flow problem; instead, it is more practical to start with the equations of mass
conservation, momentum balance, and mechanical energy conservation, also known as
equations of change (Bird et al., 1960).

TABLE 3.1
Momentum Transfer Dimensionless Numbers
Variables Relationship Involved Forces Name Symbol
2
Density, drag force, surface area, velocity FD/ρv A Drag force/inertial force Drag coefficient CD
2
Density, pressure, velocity P/ρv Pressure force/inertial force Euler Eu
2
Density, stress, velocity τ/ρv Wall shear force /inertial force Friction factor f
2
Characteristic dimension, gravity, velocity v /dg Inertial force /gravity force Froude Fr
3 5
Agitator speed, diameter, density, power P/ρN D Power/inertial force Power Po
3
Agitator speed, diameter, volumetric flow Q/ND Flow force /inertial force Pumping P
Characteristic dimension, density, velocity, vdρ/µ Inertial force /viscous force Reynolds Re
viscosity
2
Characteristic dimension, density, velocity, stress v dρ/σ Kinetic energy force/surface force Weber We
Same variables, including rheological properties Generalized Hedstrom (GHe) and Reynolds (GRe), Hedstrom (He), and Plasticity (Pl) numbers
The developed mass conservation over a stationary volume element generates
the equation of continuity:
∂ρ  ∂ ∂ ∂ 
= − ρv x + ρv y + ρvz  = −(∇ ⋅ ρv) (3.3)
∂t  ∂x ∂y ∂z 
This equation describes the density rate of change resulting from the changes
in the mass velocity vector (ρv) at a given point, the right hand term being the point
product of ρv.
The equation of motion for a volume element at a fixed point, even though it is
complicated for the x, y, and z directions, takes a single vector expression form
(Bird et al., 1960; Liu and Masliyah, 1998):
∂
ρv = −[∇ ⋅ ρvv] − ∇P − [∇τ] + ρg (3.4)
∂t
in which the different mathematical terms represent the contributions to the momen-
tum balance:
∂
ρv = rate of momentum increase
∂t
[∇ ⋅ ρvv] = rate of momentum gained by convection
∇P = pressure force on the element
∇τ = rate of momentum gained by viscous transfer
ρg = gravitation force
For an incompressible Newtonian fluid, the x-component of the Navier–Stokes
equations for the three components of the velocity vector for x, y, z coordinates
appears as (Molerus, 1997):
 ∂v ∂v ∂v ∂v  ∂P  ∂2 v ∂2 vx ∂2 vx 
ρ x + v x x + v y x + vz x  = − + µ 2x + + 2  (3.5)
 ∂t ∂x ∂y ∂z  ∂x  ∂x ∂y 2 ∂z 
3.2.3 ENERGY BALANCE

Similarly, the mechanical energy balance can be applied to a stationary volume
element through which the fluid flows, generating the corresponding equation with
several terms:
∂  1 2
ρv = − ∇ ⋅ ρv 2 v − (∇ ⋅ Pv) − P( −∇ ⋅ v) − (∇ ⋅ [τ ⋅ v]) − ( − τ: ∇v) + ρ(v ⋅ g)
1

∂t 2   2 
(3.6)
In which the meaning of each term is:
∂  1 2
ρv , rate of increase in the kinetic energy
∂t  2 
 ∇ ⋅ ρv 2 v , net rate of input of kinetic energy due to bulk flow
1
 2 

(∇ ⋅ Pv), rate of work done by surrounding pressure
P( −∇ ⋅ v), rate of reversible conversion to internal energy
(∇ ⋅ [τ ⋅ v]), rate of work done by viscous forces
( − τ: ∇v), rate of irreversible conversion to internal energy
ρ(v ⋅ g), rate of work done by gravity force
As may be noted, the three preceding relationships were obtained in rectangular

coordinates; thus, if the flow problem involves curvilinear coordinates, the cylindrical
or spherical corresponding equations should be applied. Additionally, the specific
characteristics of the physical system and its properties will have to be considered.
3.3 LAMINAR AND TURBULENT FLOW

Among the many types of flow developed by fluids, laminar and turbulent flows are
very important and commonly found, no matter what the specific physical situation.
Several geometries, such as cylinder, coil, cube, helix, oven, parallel plates, shell
and tubes, tube, and vessels containing food fluids are frequently utilized in food
process operations.
It can be observed from Table 3.1 that the ratio of the inertial variables to the
viscous force (Re) is determinant in the presence of streamline or turbulent flow;
therefore, the rheological nature of the food plays an outstanding role in flow
definition. From a practical viewpoint, the type of flow may be established with the
evaluation of the Reynolds number for Newtonians, whereas for non-Newtonian
behavior the Generalized Reynolds and the critical Generalized Reynolds numbers
should be computed.
3.3.1 LAMINAR FLOW

Of the several geometries involved in food processing, tube flow is the most impor-
tant due to easy pipe manufacturing and a very high rate of handled volume to
amount of construction material. In it, the shear stress and the velocity profile are
functions of the rheological behavior. The corresponding equations are introduced
next and are extremely useful for most food fluid systems:
For shear stress:
r( ∆P )
τ rz = (3.7)
2L
For the velocity distribution, the type of fluid implies different relationships:
1. In the case of a Newtonian fluid:
1  ∆P  2
vx =    (R − r 2 )
 2   2µL 
(3.8)

2. In cases of non-Newtonian behavior:
a. Power law model:
( 1n)
vx = 
n   ∆P   R( n +1 n ) − r ( n +1 n )  (3.9)
 n + 1  2 KL   
b. Herschel–Bulkley model (when R0 ≤ r ≤ R):
  1 
 1 
 n +1
  n +1
 H 
vx =
2L ( τ − τ )  H 
−  r∆P − τ   (3.10)
 1  1n  w 0  2L 0

∆P + 1 K H  
 nH  H  
c. Bingham plastic model (when R0 ≤ r ≤ R):
 ∆P R 2 − r 2 − τ R − r 
vx =
1
µP
(
 4 L )
0( )

(3.11)
Similar equations can be developed or have been obtained for other geometries.
For the aforementioned equations, four assumptions were considered:
1. Steady flow
2. Constant rheological properties and density
3. No entrance or exit effects
4. Prevalence of laminar flow
Even though most industrial process flows are turbulent, food materials may be
the exception during transport due to their non-Newtonian nature.
3.3.2 TURBULENT FLOW

There are many considerations and equations for flows under turbulent conditions;
in this type of flow, the average and the instantaneous/point velocity are normally
different as a consequence of the velocity fluctuation for a given volume element of
fluid. Several approaches, such as the Boussinesq theory, Prandtl mixing length,
analogies between the transport phenomena, and film and penetration theories,
among others, have been proposed for the modeling of turbulence (Brodkey and
Hershey, 1988).
The mathematical relationships for velocity distribution, when turbulent flow is
present, are known as “universal velocity distribution” equations. They are valid
inside channels and smooth tubes in which the flow has been fully developed, with
most of the boundary layer arising from Prandtl’s theory:

+
For the wall region or viscous sublayer, y ≤ 5:
v+ = y+ (3.12)
+
For the buffer or generation zone, 5 < y < 30:
v + = 5.0 ln y + − 3.05 (3.13)

+
For the turbulent zone, y ≥ 30:
v + = 2.5 ln y + + 5.5 (3.14)
These velocity profiles, also known as the law of the wall, have been verified
experimentally for Newtonian fluids with very good results, but such is not the case
for non-Newtonian fluids, in which some differences have been observed.
Both groups of velocity equations, for viscous and turbulent flows, may be used
in the involved unit operation not only for velocity profiles mass and volumetric
flows, but also for computation of residence time, design parameters, and dimensions
inside process units. Furthermore, temperature distribution, heat transfer area, and
concentration profiles in heat exchangers or in mass transfer related equipment may
be obtained with incorporation of momentum transfer considerations.
3.3.3 TRANSPORTATION OF FLUIDS

As previously mentioned, there are process conditions involving different geome-
tries, but the cylindrical shape is the most commonly encountered flow situation.
Also, it is the most studied in relation to momentum phenomena and related topics,
such as pump needs, pressure losses, and friction factors through pipe systems.
Accurate prediction of pressure drop/flow relationships for non-Newtonian fluids in
ducts is consequently of great importance.
Additionally, when fluid flows through fittings (bends, elbows, entrances, expan-
sions, reductions, and valves), the flow patterns become more complex than those
in a straight tube and are characterized by altered velocity distributions and the
presence of centrifugal forces and secondary flows (Das et al., 1991).
In the unit operation of fluid foods’ transportation, there is a lack of information
for non-Newtonian materials. Some studies related to the prediction of friction factors,
pressure losses, and power consumption evaluations as part of the mechanical energy
have been completed. Bernoulli’s equation (Equation 3.15), in which the input of
mechanical energy is conserved through the output for uncompressible, isothermal,
and steady flow in one direction, is the fundamental mathematical model for the
aforementioned evaluations.
v12 P Zg v22 P Zg
+ 1 + 1 + ηp Wp = + 2 + 2 + Ef (3.15)
2α1g c ρ gc 2α 2 g c ρ gc
Some advances for non-Newtonian behavior, particularly those related to the

correction factor for the kinetic energy, friction factor, and related coefficients have

been made recently; they are summarized in Table 3.2 for both Newtonian and non-
Newtonian fluids. There are many proposed explicit and implicit equations for
Newtonian fluids as a function of Reynolds number and relative roughness that were
not included in Table 3.2, and although some contributions have been proposed to
characterize non-Newtonian food fluid transportation, it remains a complex flow and
an incompletely understood phenomenon.
3.4 RHEOLOGICAL PROPERTIES OF FOODS

3.4.1 RHEOLOGY
Rheology, defined as the science of flow and deformation of material, is a funda-
mental interdisciplinary science that has been gaining increasing importance in the
field of foods. According to Rao (1986), Steffe (1992), Kokini (1992) and Vélez-
Ruiz (1996), among other authors, there are numerous topics of interest to the food
industry related to rheological behavior, such as:
1. Process engineering applications involved in equipment and process

design
2. Development of new products or reformulation of existing products
3. Quality control of intermediate and final products
4. Correlation with sensory evaluation
5. Understanding of food structure
Rheology can be used to characterize not only flow behavior of foods and other
materials, but also structural characteristics. The knowledge of flow food properties,
such as consistency, pourability, thickness, viscoelasticity, viscosity, and yield
stress, contributes substantially to facilitating transport and commercial processing,
as well as to promoting consumer acceptance. Insight into structural arrangement
helps to predict the behavior or stability of a given material with storage, change
in humidity and/or temperature, and handling (Motyka, 1996). Consequently, basic
rheological information on materials is important not only to engineers, but also
to food scientists, processors, and others who may utilize this information and find
new applications.
Many foods are neither solid nor liquid, but exist in an intermediate state of
aggregation known as semiliquid or semisolid. As a consequence of the complex
nature and lack of precise boundaries between solids/semisolids and liquids/semi-
liquids, many foods may exhibit more than one rheological behavior depending on
their specific characteristics and the measuring conditions used during the physical
characterization. Due to the complex composition and particular structure of foods,
the approaches for characterizing a food’s rheological behavior may be classified
into five methods: empirical, phenomenological (including fundamental and imita-
tive), linear viscoelastic, nonlinear viscoelastic, and micro-rheological. In the case
of foods, empirical and phenomenological approaches have been predominant in
studies associated with flow properties (Rao, 1992; Vélez-Ruiz and Barbosa-
Cánovas, 1997b). With respect to viscoelastic nature, the approaches mainly include

TABLE 3.2
α) Friction Factors (F) and Related Coefficient (K) for Newtonian and Non-newtonian Fluids
Kinetic Energy Factor (α
Factor Regimen Considerations References
Kinetic Energy Correction Factor

α = 0.5 Laminar Newtonian fluids, Re ≤ 2100 Charm (1971)
(2n + 1)(5n + 3)
α= Laminar Power law fluids, and evaluation of GRec Heldman (1975)
3(3n + 1) 2 Ibarz et al. (1996)
1
α= Laminar Bingham plastic fluids, and evaluation of Skelland (1967)
τ0
2− GRec Ibarz et al. (1996)
τw
[(1 + 3n + 2 n 2 + 2 n 2 C + 2 nC + 2 n 2 C 2 )3 (2 + 3n )(3 + 5n )(3 + 4 n )]
α=
[[(1 + 2 n) (1 + 3n ) ][18 + n(105 + 66 C) + n (243 + 306C + 85C 2 ) + n 3 (279 + 522C + 350C 2 ) + n 4 (159 + 390C + 477C 2 ) + n 5 (36 + 108C + 216C 2 )]]
2 2 2
Laminar Herschel-Bulkley fluids, and evaluation of Osorio and Steffe (1984)

GRec Ibarz et al. (1996)
ln(2α ) = 0.168C − 1.062 nC − 0.954 n 0.5 − 0.115 C 0.5 + 0.831 For 0.06 ≤ n ≤ 0.38 Briggs and Steffe (1995)
ln(2α ) = 0.849C + 0.296 nC − 0.600 n 0.5
− 0.602C 0.5
+ 0.733 For 0.38 ≤ n ≤ 1.60 Briggs and Steffe (1995)
4c (3 + c)(3 + 2c)
4
α= ≈ 1.0 Turbulent Newtonian fluids, c:6 − 10 depending of Re Ibarz et al. (1996)
(1 + c) 3 (1 + 2c) 3
0.5 < α < 1.0 Laminar and turbulent Values obtained as a function of Re Foust et al. (1980)
Friction factor
16 64
fF = ;f = Laminar Newtonian fluids, fD = 4 fF Foust el al. (1980)
Re D Re
16
fF = Laminar flow Power law Fluids, GRe instead of Re Ibarz et al. (1996)
G Re
1 f He (He) 4
= F − + Laminar flow Implicit equation for Bingham plastic fluids Ibarz et al. (1996)
Re B 16 6(Re B )2 3fF3 (Re B )8
16
fF = Laminar flow Herschel-Bulkley fluids, GRe and GHe Garcia and Steffe (1986)
ψGR ε need to be considered
n
 (1 − C)2 2C(1 − C) C 2 
ψ = (3n + 1) n (1 − C)1+ n  + +
 3n + 1 2n + 1 n + 1 
1  1.255 1 ε 8
= −4 log  +  Turbulent flow Newtonians, Re: 4000 − 10 Levenspiel (1993)
(fF )1/ 2  Re( f F )1/ 2
3.7 D 
1  5.62 ε
= −2 log  0.9 + 0.27  Turbulent flow Newtonians, rough pipes Levenspiel (1993)
( 4 fF )1/ 2  Re D
log G Re ff(1− n / 2 ) − 1.2 

1 4 0.4
= Turbulent flow Power law fluids, GRe: 2900-36000 Dodge and Metzner (1959)
(fF )1/ 2 n 0.75  n 
1
= 2.27 log(1 − C) + 2.27 log[Re B f F0.5 ] − 1.15 Implicit equation for Bingham fluids Ibarz et al. (1996)
( 4 f F ) 1/ 2
fF from figures Laminar and Turbulent flow Values obtained as a function of GRe and Garcia and Steffe (1986)
GHe for n = 0.2 and 0.5
Friction Loss Coefficients

k from graphical representations Different fittings Values obtained as a function D and Foust et al. (1980)
equivalent length. Newtonians
−0.896
k = 191 G Re 90° short radius elbow Laminar flow of power law fluids Steffe et al. (1984)
−0.504
k = 29.4 G Re Tee, line to branch Laminar flow of power law fluids Steffe et al. (1984)
−0.492
k = 30.3 G Re Fully open three-way plug valve Laminar flow of power law fluids Steffe et al. (1984)
fundamental and linear. Most food systems are considered to be linear viscoelastic
materials at small strains.
Any of the available commercial instruments that allow objective characterizations
are appropriate for measuring the rheological properties and identifying the rheological
behavior of food materials. The accuracy of these rheometers has been improved due
to the incorporation of modern mechanical devices and microcomputer technology.
3.4.2 RHEOLOGICAL MODELS

The relationship between applied stress and resulting strain shown by any food
material can be expressed either empirically or in terms of a rheological equation
of state, also known as a rheological model. There exists a particular approach in
which the rheological behavior of a material is analyzed on a simplified deforma-
tion called single shear or uniaxial deformation. This approach is the basis for
many rheological measurement techniques and permits the analysis of many food
materials.
Fluid, solid, and viscoelastic behaviors have been observed in food products.
Juices, milk, vegetable oils, and water behave as Newtonian fluids; but dressings,
fruit concentrates, ketchup, and yogurt behave as non-Newtonian. Gels, meat emul-
sions, and some types of cheese have been characterized as solids with elastic
behavior. Other food products such as ice cream, mayonnaise, and whipped cream
have been characterized by their viscoelastic nature.
Among the many mathematical relationships proposed to characterize the rheo-
logical nature of liquid materials, four models are particularly useful for describing
the behavior of fluid foods. One is Newton’s model for Newtonians, expressing the
concept of viscosity, and the other three (Power Law, Bingham Plastic and Herschel
and Bulkley models) are for non-Newtonian behavior; the corresponding equations are:
Newtonian model τ = µγ˙ (3.16)
Power law model τ = K( γ˙ )n (3.17)
Bingham model τ = τ 0 + ηP γ˙ (3.18)
Herschel–Bulkley model τ = τ 0 + K( γ˙ )n (3.19)
Many other more complex or more specific models have been proposed for
different fluid materials. Consequently, these models are utilized for particular prod-
ucts. Some of them are included in Table 3.3.
In addition, if time is considered as another variable, the fluids may show a
thixotropic or a rheopectic behavior. Thixotropy refers to a reversible decrease in
apparent viscosity with time at constant shear rate. This is generally due to a
reversible change in structure of the material with time under shear, with a limiting
viscosity ultimately being approached. Rheopexy is, in essence, the reverse of thix-
otropy; that is, it represents an increase of apparent viscosity with time at a constant

TABLE 3.3
Additional Rheological Models for Time-Independent Fluids
Model Application Reference
Casson τ 0.5 = τ 00.5 + K( γ˙ ) 0.5 Chocolate, fruit dispersions Casson, 1959

and products
n
 1

Vocadlo τ =  ( τ 0 ) n + Kγ˙  Fruit and puree concentrates Parzonka and
  Vocadlo, 1968
Modified Casson τ 0.5 = τ 00.5 + K( γ˙ ) n Concentrated orange juice Mizrahi and Berk,
1972
Generalized H-B τ n1 = τ 0n1 + K( γ˙ ) n 2 Food fluids Ofoli et al., 1987
⋅
Power Series γ = K1τ + K 2 τ + K 3 τ ...
3 5
Food fluids Whorlow, 1992
⋅
τ = K1 γ + K 2 ( γ˙ ) + K 3 ( γ˙ ) ...
3 5
shear rate. To model thixotropic and rheopectic behavior, several models have been
developed. The model expressed by Equation (20) is a modification proposed by
[Mason et al. (1987)] to another previously established model (Barbosa-Cánovas
et al., 1993).
  t 
 Σb i exp −  
 λi  
τ = K( γ˙ )n 1 + ( b 0 t( γ˙ ) − 1) (3.20)
 Σb i 
 
 
Sometimes the rheological behavior of foods depends on the experimental con-

ditions; for example, evaporated milk has been characterized as Newtonian by
Fernández-Martín (1972), Bloore and Boag (1981), and Wayne and Shoemaker
(1988), and as a non-Newtonian fluid by Randhahn (1973) and Schmidt et al. (1980),
and during its flow has shown thixotropic behavior (Ibarz et al., 1987). Also, sweet-
ened condensed milk has been characterized as non-Newtonian by Alvarez De Felipe
et al. (1991), as a thixotropic fluid by Higgs and Norrington (1971), and as a vis-
coelastic material by Patil and Patel (1992). The same material may even develop
different flow behaviors depending on the applied range of shear rate or shear stress.
A viscoelastic material may show either linear or nonlinear behavior. A linear
viscoelastic material has properties that are dependent upon time alone and not upon
the magnitude of the stress that is applied to the material. Nonlinear viscoelastic
materials exhibit mechanical properties that are a function of time and the magnitude
of stress used. To express the viscoelasticity of a linear food material, mechanical
models incorporating two basic elements have been utilized. These elements are the
elastic spring, which represents the instantaneous elastic nature, and the dashpot,
which expresses the pure viscous flow. These two elements when in a series constitute
a Maxwell body, and when parallel, a Kelvin–Voigt body (Vélez-Ruiz, 1996).

3.4.3 TEMPERATURE AND CONCENTRATION VARIABLES
The influence of temperature on the viscosity of Newtonian and the consistency
coefficient of non-Newtonian fluid foods is commonly expressed in terms of an
Arrhenius type equation (Equation 3.21). Furthermore, the effects of both variables,
concentration and temperature at a given shear rate range, can be combined in terms
of single relationships (Vélez-Ruiz and Barbosa-Cánovas, 1997a). Fernández-Martín
(1972) and Bloore and Boag (1981) have proposed a polynomial relationship (Equation
3.22) to fit the viscosity of concentrated milk (considered a Newtonian fluid) as a
function of total solids and temperature, which also has been fitted to other food
fluids.
 Ea 
η, µ a , K = A 0 exp (3.21)
 RT 
2 2 2 2
log η = A0 + A1t + A2t + (B0 + B1t + B2t )S + (C0 + C1t + C2t )S (3.22)
Vitali and Rao (1984) used an exponential relationship to model the apparent
viscosity of concentrated orange juice influenced by temperature and concentration:
B
η = φ (T, C) = KT,C exp (Ea/RT)⋅C (3.23)
Reddy and Datta (1994) employed a combined exponential potential function-

ality to relate the consistency coefficient, absolute temperature, and concentration:
X
K = B1 exp (C2/T) 1.25 (3.24)
Generally, the effect of concentration and temperatures on rheological behavior

has been expressed by power and/or exponential equations for different types of
food fluids (Vélez-Ruiz and Barbosa-Cánovas, 1997a).
3.5 SIMULTANEOUS TRANSFER PHENOMENA

Industrial equipment often involves simultaneous transfer phenomena, hence flow
effects must be considered when designing and evaluating heating/cooling processes
and mass transfer operations. The velocity profile of any phase will depend on the
rheological properties of the food fluid, used geometries, and other specific factors,
such as the solids loading, particle diameter, and density differences in the case of
solids–food liquids, and density differences and interface in the case of oil–water
and gas non-Newtonian liquid mixtures. Other important factors should be consid-
ered, including temperature and thermal properties for heat transfer operations and
concentration and density for mass transfer processes.

Since non-Newtonian fluids are often very viscous, most thermal treatment
methods assume the flow of foods in tubular ducts as a laminar regime. Thus, the
process calculations need to be very accurate in order to avoid under- or overprocess-
ing; in most cases the Arrhenius relationship has been used to describe the effect of
temperature on the rheological behavior of non-Newtonian food fluids. To take account
of the rheological behavior, Pereira et al. (1989), for instance, considered the rheolog-
ical parameters as part of the Generalized Reynolds (Equation 3.25), Generalized
Prandtl (Equation 3.26), and Generalized Grashoff (Equation 3.27) numbers and the
“viscosity correction term” (Kb/Kw), in a double tube heat exchanger modeling for
laminar flow:
8v 2 − n D n ρ
G Re = n (3.25)
3n + 1
2 n K
 n 
  3n + 1 n n −1 
Cp   n 
K 2 
G Pr =  1− n n −1
 (3.26)
k t  4v D 
 
gβρ2 D3∆T
G Gr = 2 (3.27)
  3n + 1 n 
 K 
 n  
1− n n −1
 4v R 
 
Flow properties are also closely related to those unit operations involving heat
transfer phenomena. Cooling, heating, pasteurization, sterilization, and evaporation
are the most common heat transfer operations utilized in food processing, and
whatever the main purpose, heat transfer implies flow of food fluids inside the
exchanger, mostly with non-Newtonian behavior. Since the flow profile controls
mixing and thermal–times effects in the heat equipment, it is essential to know how
flow regime influences the heat transfer phenomenon.
On the other hand, there are mass transfer operations in which food fluids are
handled and flow behavior will affect the operation performance importantly. There-
fore, engineers who work with air and spray drying, fermentation processes, membrane
separations, and vacuum drying should consider the flow properties of the fluid mate-
rials. Other unit operations, such as extraction, frying, leaching, and osmotic dehydra-
tion, have less dependency on rheological properties. Table 3.4 presents a summary
of studies in which the heat and mass transfer operations have been related to momen-
tum transfer, such as rheological properties or velocity profiles.

TABLE 3.4
Examples of Heat and Mass Transfer Operations Related to Rheological
Properties of Food Fluids
Application/Fluids Purpose Important Remarks Reference
Continuous Modeling continuous Understanding the effect Gauriguata

a
sterilization/Bingham sterilization for a NN of temperature on the et al., 1979
plastic fluids fluid rheology is necessary for
good sterilization process
Thin film Simulation of fruit Evaporation regimes were Stankiewics
evaporation/water juices evaporation related to flow and Rao, 1988
and sugar solutions
Double tube heat Predicting heat Correlations were Pereira et al.,
exchanger/guar gum exchange during developed for a non- 1989
b
and CMC solutions laminar flow Newtonian fluid
c d
UHT process/starch Evaluations of the h for particles heated in Awuah et al.,
e
solutions and water particle/fluid interface N fluids were 20% 1993
convective heat higher than in NN fluids
transfer coefficient
d
Aseptic Determination of fluid h was significantly Bhamidipati and
treatment/particles in convective heat affected by fluid Singh, 1995
CMC solutions transfer coefficient viscosity
Scraped surface Effect of heat transfer on Figures of velocity Wang et al.,
heat/NN fluids flow profiles and profiles for three NN 1999
numerical simulation fluids
Spray drying/power Prediction of drop An equation for drop Weberschinke
law liquid diameter; theoretical diameter of NN fluids and Filková,
deprivation was developed 1982
Drum drying/power Film thickness of drying Thickness of the film was Daud, 1989
law fluids material for a drum equated as a function of
dryer; theoretical velocity ratio of cylinders
approach and flow behavior index
Spray drying/soy Effect of viscosity on The viscosity must be Hayashi, 1996
protein milk drying rates of soy controlled for good ato-
protein milk mization and milk quality
a
NN = non-Newtonian
b
CMC = carboxy methylcellulose
c
UHT = ultra high temperature
d
h = convective heat transfer coefficient
e
N = Newtonian
3.6 FINAL REMARKS

This chapter is an overall review of an extensive topic in which many aspects of the
complex phenomena remain unknown. Therefore, the main momentum transfer
parameters and variables have been only briefly commented upon. In process design,
momentum transfer is most likely present; thus, some simple or complex approach

must be taken into consideration, not only with respect to the flow nature, but also
with respect to heat and mass transfer, as well as biochemical reactions. Rheological
behavior has some impact on all unit operations involving food liquids.
Nowadays, several computer programs have been developed to solve various
transport equations, and they are commercially available. Furthermore, continuous
advances in computer capacity in terms of computational speed, disposability, and
memory will enable application of rigorous analytical models to specific momentum
transfer problems. Also, the utilization of modern instrumental techniques, such as
nuclear magnetic resonance and magnetic resonance imaging, will contribute to the
experimental approach for measuring velocity profiles and rheological behavior of
non-Newtonian fluids, including fluid/particle mixtures, and therefore to a better
understanding of the momentum phenomenon.
NOMENCLATURE
2
A Surface area or transfer area (L )
A0, Ai Constants model
b0, bi Constants model
B, B0, Bi Constants model
c Constant value (with a magnitude between 6 and 10)
C Constant ratio (τ0/τw) (dimensionless); solids content (ºBx)
C0 , Ci Constants model
CD Drag coefficient (dimensionless)
Cp Fluid specific heat (E/MT)
d Characteristic dimension (L)
D Tube diameter (L)
Ea Activation energy (E/Mol)
Ef Friction losses energy (FL/M)
Eu Euler number (dimensionless)
f Friction factor (dimensionless)
fD Darcy’s friction factor (dimensionless)
fF Fanning’s friction factor (dimensionless)
FD Drag force (F)
Fr Froude number (dimensionless)
2
g Gravitational constant (L/t )
2
g Vector representing the acceleration due to a gravitational field (L/t )
GGr Generalized Grashoff number (dimensionless)
GHe Generalized Hedstrom number (dimensionless)
GPr Generalized Prandl number (dimensionless)
GRe Generalized Reynolds number (dimensionless)
GRec Critical generalized Reynolds number (dimensionless)
He Hedstrom number (dimensionless)
k Friction loss coefficient
kt Thermal conductivity (E/LtT)
K Consistency coefficient, or model constant for rheological relationships
n 2
(Ft /L )

K1, K2, K3 Constants model
L Pipe length (L)
n Flow behavior index or in general, power law exponent (dimensionless)
np Pump efficiency
N Agitator speed or rotational velocity (rev/t)
2
P Pressure (F/L ) or power (FL/t)
Pl Plasticity number (dimensionless)
Po Power number (dimensionless)
3
Q Volumetric flow (L /t)
r Radial coordinate (L)
R Pipe inner radius (L); universal gas constant (Equation 21) (E/MolT)
R0 Plug radius (L)
Re Reynolds number (dimensionless)
S Solids content (%)
t Time; temperature (°C)
∆T Temperature difference (Tw – Tbav)
T Absolute temperature (K)
Tbav Bulk average fluid temperature (T)
Tw Wall temperature (T)
v Flow velocity vector (L/t); v is the magnitude of v, which is composed
of vx, vy, and vz; velocity components in directions x, y, z
+
v Time averaged velocity (dimensionless)
∇v Shear rate tensor (1/t)
T
(∇v) Transpose of the shear rate tensor (1/t)
We Weber number (dimensionless)
X Milk concentration (% w/w)
+
y Time averaged distance, distance from the wall (dimensionless)
Z Vertical position (L)
GREEK SYMBOLS
α Kinetic energy correction factor (dimensionless)
β Thermal expansion coefficient (1/T)
3
ρ Fluid density (Μ/L )
ε Relative roughness (dimensionless)
γ Shear rate (1/t) (dimensionless)
λi Time constant (t)
Ψ Constant for NN friction factor
σ Surface force (F/L)
2
τ Shear stress tensor or momentum flux (F/L ) which is composed of τxy , τyz,
etc., the components of the shear stress tensor
2
τ0 Yield stress (F/L )
2
τrz Shear stress (F/L )
2
τw Shear stress at wall (F/L )
2
µ, η Viscosity coefficient or absolute viscosity (Ft/L or M/Lt)

2
µa Apparent viscosity (Ft/L or M/Lt)
2
µp, ηp Plastic viscosity (Ft/L or M/Lt)
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Part II
Mass Transfer

Structural Effects
4 of Blanching and
Osmotic Dehydration
Pretreatments on Air
Drying Kinetics of
Fruit Tissues
S.M. Alzamora, A. Nieto, and M.A. Castro
CONTENTS
4.1 Introduction
4.2 Materials and Methods
4.2.1 Experiment
4.2.2 Moisture Diffusivity Calculation
4.3 Results
4.3.1 Effect of Blanching
4.3.2 Effect of Osmotic Treatment
4.4 Conclusions
Nomenclature
References
4.1 INTRODUCTION
Typical commercial fruit processing currently involves predrying treatments aimed at
either quality improvement of the final product or improved drying kinetics (Lewicki,
1998). The most popular pretreatments are blanching and sugar or salt osmotic dehy-
dration. Blanching prior to drying is sometimes performed to inactivate enzymes that
adversely affect product quality, denature cell membranes to reduce drying times,
remove intercellular air, and/or reduce microbial load. Osmotic pretreatment results
in substantial dewatering; it has also been reported to prevent excessive shrinkage of
the tissue undergoing drying and to improve rehydration of dry material.
Literature results pertaining to the drying behavior of fruit and vegetable tissues
as affected by blanching and the osmotic process are apparently contradictory, as

reviewed by Alvarez et al. (1995). For example, moisture diffusivity of water in sugar
beet root plates, carrot cubes, and potato slices was reported to decrease because of
the uptake of sugar and/or salt. In contrast, sucrose osmotic treatment did not affect
the dehydration rate of pineapple. Blanching increased the rate of drying of sugar beet
and carrot, decreased the moisture transport rate in potato, and had only a small effect
on avocado dehydration behavior.
This dissimilarity can be ascribed to the intricate simultaneous heat and mass
transfer drying process and to the wide variation in physical and structural properties
among vegetables and fruits. A schematic view of the various transfer mechanisms
that can be present during drying of fruit tissues is presented in Figure 4.1a. A significant
(a)
Molecular diffusion
CONDUCTION Capillary motion
Knudsen flow
Vapor diffusion in pores
CONVECTION Liquid diffusion
Evaporation - condensation
(b)
tt
cwp
tt
st
cl = chloroplast; cw = cell wall; cwp: the cell wall pathway; g = Golgi; is =

intercellular space; nu = nucleolus; n = nucleus; ml = middle lamella; pl =
plasmodesmata; pm = plasmalemma; rer = rough endoplasmic reticulum; st: the
symplastic; tt: the transmembrane transport; v = vacuole
FIGURE 4.1 (a) Major mechanisms during drying of parenchymatous fruit tissue. (b) Pos-
sible pathways for water transport in a parenchymatous fruit cell (courtesy of Dr. Ancíbor).

number of mechanisms for moisture transport within porous foods has been proposed,
including molecular diffusion, capillary motion, liquid diffusion through solid pores,
Knudsen flow, vapor diffusion in air-filled pores, and hydrodynamic flow, none of
them prevailing throughout the whole drying process (Zogzas et al., 1996). Usually, a
series, parallel, and/or series–parallel combination of the aforementioned mechanisms
contributes to the total flow, and the relative contributions show product and drying
system specificity as well as drying time dependence.
Structural heterogeneity of biological materials, such as fruit, brings an additional
complexity to the water migration in a porous solid system.As Figure 4.1b shows, cellular
tissues are multiphase systems (i.e., vacuole, cytoplasm, tonoplast and plasmalemma
membranes, cell wall, intercellular spaces), and water can migrate out of cells in three
possible ways: transmembrane transport (through tonoplast and plasmalemma mem-
brane boundaries), symplastic transport (via cytoplasmic strands or plasmodesmatas),
or cell wall pathway (the apoplastic way), this last being the preferred pathway for
small nonionic species such as water (Molz and Ikenberry, 1974; Tyree, 1970).
Because of this complexity, the macroscopic (also called the “black box”) approach
to quantifying the transport of water during the first falling rate period of air drying
commonly involves the determination of an empirical single experimental effective
water diffusivity (Deff). This parameter, obtained by applying Fick’s second law for
species diffusion in a single phase, takes into account the internal porosity and the
tortuosity of the sample, but it also lumps together the deformation of the fruit matrix,
the volume changes, the composition and structure of the fruit, the material–water
interactions, and the multiphase water transport (Zogzas et al., 1996; Achanta and
Okos, 1996). Hence, Deff is an empirical parameter useful as a quick engineering design
tool but without physical significance.
A phenomenological understanding of the dehydration kinetics and the effect of
pretreatments, however, requires, among others, a microscopic analysis to address the
structural and ultrastructural changes produced at the cellular level and their potential
influence on drying rates and quality of the final products. Food structure is a process
variable usually neglected in engineering design and transport kinetics analysis. But
cell wall resistance to water flux, as well as membrane integrity, are modified to different
degrees due to the predrying treatments, depending on the type of fruit considered.
In this chapter, ultra-, micro- and macrostructural effects of blanching and osmotic
dehydration (atmospheric or in vacuum) pretreatments on the moisture transport rate
during the first falling rate period of air drying of fruits are illustrated. Drying behavior
of strawberry, mango, and apple is discussed under the following headings: shrinkage
of fruit piece, porosity, sugar content, cell membrane integrity, and cell wall architecture.
4.2 MATERIALS AND METHODS

4.2.1 EXPERIMENT
The experimental process has been well described by Alvarez et al. (1995) and Nieto
et al. (1998, 2001). Briefly, apples (Malus pumila, Granny Smith cv.; ≅85–88% w/w
moisture content, wet basis) and mangoes (Mangifera indica Linn, Keitt var.; ≅85–
88% w/w moisture content, wet basis) were hand peeled and cut into an infinite plate

shape (dimensions at the end of the pretreatment ≅4 × 4 × 0.4 cm). Strawberries (Pájaro
or Tioga Leico var.; ≅86% w/w moisture content, wet basis) were washed, decapped
by hand, and selected to obtain samples of uniform size and maturity.
For steam blanching, apple and mango plates were exposed to steam for 1 min
at atmospheric pressure and then cooled in water at 5°C. Whole strawberries were
exposed to steam for 3 min and cooled in similar conditions.
For osmotic dehydration at atmospheric pressure, samples were immersed into
different glucose aqueous solutions with (mango and apple) or without (strawberry)
forced convection at 25°C until the desired final water activity (aw) value was reached
(≅3 h for mango and apple and 48 h for strawberry). For vacuum glucose impregnation,
fruit samples were immersed in a 59.0% w/w glucose aqueous solution (aw = 0.84) at
25°C, and a pressure equal to 60 mmHg was applied to the system for 10 min. After
the vacuum treatment, the system was placed at atmospheric pressure for 10 min; the
final aw value reached by fruits was 0.97.
After osmosis, fruit samples were drained and dried at 60°C (mango and apple)
or 55°C (strawberry) with air at high constant velocity (about 15 m/sec) to eliminate
or minimize external resistance to moisture loss.
4.2.2 MOISTURE DIFFUSIVITY CALCULATION

The Deff value was obtained by applying Fick’s second law for species diffusion in
a single phase, with boundary conditions of internal resistance controlling and
uniform initial moisture content, integrated over the volume of the slab (apple,
mango) or sphere (strawberry) (Luikov, 1968). The Deff values for spheres were
affected by a shape factor to take into account that strawberries are ellipsoids (Becker,
1959; Aguerre et al., 1987).
Uniform internal fruit temperature was assumed due to the low Biot number for
heat transfer usually found for conventional air drying of fruits (Alzamora et al.,
1979). Negligible external heat transfer effects were also considered.
Assuming diffusion in an isotropic medium, constant diffusion coefficient, and
isothermal process, and using the moisture concentration converted to moisture
content on a dry basis, Fick’s second law for one-dimensional unsteady diffusion is
given as:
∂m  ∂2 m C ∂m 
= Deff  2 +  (4.1)
∂t  ∂x x ∂x 
where x is the spatial coordinate, C is a constant (0 for infinite plate; 2 for sphere),
and Deff is the effective moisture diffusivity.
For uniform moisture distribution (assuming no constant drying period takes
place) and internal control to mass transfer, initial and boundary conditions are:
m(x, 0) = m0 at t = 0 (4.2)
m(xS, t) = me at x = xS (at the surface) (4.3)
m(0, t) = finite at x = 0 (at the center) (4.4)

Solutions for the different geometrical configurations can be expressed as:
∞
m − me  2 π D eff t

∑
2
8 1
= exp  − ( 2 n + 1) 2 
(4.5)
m0 − me π2 n =1
(2 n + 1) 2
 4 l0 
for a slab, where l0 is the half-thickness of the slab;

∞
m − me  D t
m0 − me
= ∑ n 6π
n =1
2 2
exp − n 2 π 2 eff2 
 Re 
(4.6)
for a sphere, where Re is the radius.

For long drying times, only the first term of Equations (4.5) and (4.6) is significant,
and the values of Deff may be estimated from the linear relationship m − me/m0 −
me vs. time on semilogarithmic coordinates.
Strawberries were assumed to be ellipsoids, having three characteristic diameters
(2 rM1 ≅ 2 rM 2 ≤ 2 rM ). For bodies having an ellipsoid shape, the Fourier number may
be extended to (Aguerre et al., 1987; Becker, 1959):
Deff t
F0 = 2 (4.7)
 Vp 
3 S 
 p
where Vp is the volume and Sp is the surface of the body. Generally, the equivalent
spherical radius (Re) is used as the characteristic length.
Deff t
F0′ = (4.8)
R 2e
where Re = 3(VS/SS), and SS and VS are the surface area and the volume of the
sphere, respectively. If VS = VP = V, the relationship between F0 and F0′ is given by
2
Deff t Deff t  Sp  Deff t F0′
F0 = 2 = 2   = Ψ2 R2 = Ψ2 (4.9)
 V  V  S S e
3 S  3 S 
 p  S
where Ψ is defined as SS/Sp, and SS is the surface area of a sphere of volume equal
to that of the fruit with surface area Sp, which is assumed to be an ellipsoid. The
2
intrinsic diffusivity Deff is given by Ψ D′eff. Ψ is the shape factor of a solid, commonly
known as the sphericity (Becker, 1959). The diffusion coefficient calculated from
2
Equation (4.6) is D′eff, and it must be corrected by the factor Ψ when the product
shape can be assumed as an ellipsoid:
Expressing the surface area of an ellipsoid as
 rm R m 
Sp = 2 π rm2 + 2 π sin −1 e (4.10)
 e 

and calculating the eccentricity, e, as (Aguerre et al., 1987):
e = 1 − ( rm / R m )2 (4.11)
the shape factor results in:
SS 4 π R 2e
Ψ= = (4.12)
Sp r R 
2 π rm2 + 2 π m m sin −1 e
 e 
4.3 RESULTS
4.3.1 EFFECT OF BLANCHING
Table 4.1 summarizes the main structural features that may be produced by fruit scalding
(Ilker and Szczesniak, 1990; Alzamora et al., 1997). Depending on the preponderant
phenomenon/a, drying rates of blanched tissues could be decreased or increased com-
pared to the moisture transport rate for the fresh fruit.
The photomicrographs in Figure 4.2 compare the structures of the fruits with
and without blanching. All raw fruits (Figure 4.2A, C, F, G) exhibited parenchyma-
tous cells containing intact membranes, cytoplasm, and organelles and had intact
cell walls without degradation, disruption, or dissolution. The plasma and tonoplast
membranes were closely associated with the cell wall, and the middle lamella was
clearly seen cementing adjacent cells. On the contrary, in the three blanched fruits
(Figure 4.2B, D, E, H, I), plasmalemma and tonoplast were disrupted, and numerous
vesicles of the cytoplasm had been formed.
In blanched strawberry, the electronic density of the cell wall was much lower
than that of fresh fruit walls (Figure 4.2B). The middle lamella practically disappeared,
and microfibrils appeared distorted. Reduction in fruit volume was small (<10%)
(Alvarez et al., 1995).
In mango, heated cell walls exhibited disorganized microfibrils and longitudinal
striations with zones of high and low electron density (Figure 4.2I). Protoplasm appeared
TABLE 4.1
Major Reported Structural Phenomena Due to Blanching in Connection
with Water Transport Rate During Drying of Fruit Tissues (from
Various Sources)
Disruption of cell membranes and increased permeability to water as well as loss of solubles to the
surrounding medium and/or redistribution of solubles within the material during drying
Shrinkage of tissues due to contraction of some biopolymers and/or displacement of occluded air
Loosening of the hemicellulose–cellulose and the pectin networks due to cleavage and solubilization
of polymers, increasing the cell wall porosity and decreasing cellular adhesion along the middle
lamella
2+
Crosslinking of pectic polysaccharides by Ca and by ester linkages (facilitated by deesterification
of pectin chains due to activation of pectin methylesterase)
Starch gelatinization and protein insolubilization

FIGURE 4.2 Parenchyma tissue from strawberry, apple, and mango as affected by vapor blanch-
ing. A,B: strawberry. A: fresh control. Cell wall with a nitid middle lamella and a very tightly
packed pattern of microfibrils mainly toward the margin. B: blanched. Less densely stained
wall. C–E: apple. C: fresh control. Intact membranes close to cell walls and conspicuous
middle lamella. D, E: blanched. Disrupted membranes and densely stained wall with some
striations; formation of vesicles. F–I: mango. F,G: fresh control. Polygonal cells closely
aligned to one another, with grouped starch granules and protein–carbohydrate slime; cell
walls with good electron density. H, I: blanched. Dense protoplasm due to gelatinization of
starch and thermal denaturation of slime. Rounded cells, disorganized microfibrils and lon-
gitudinal striations. A–E, G, I: TEM micrographs; F, H: LM micrographs. Scale: A, B, G, I:
0.5 µm; C–E: 1 µm; F, H: 100 µm. cw: cell wall; p: plasmalemma; T: tonoplast; ML: middle
lamella; s: starch granule; sl: slime; ve: vesicle.

dense probably due to gelatinization of starch and thermal denaturation of the protein–
carbohydrate slime typical of the fruit (Figure 4.2H). Blanching also produced a slight
volume shrinkage (≅10%) and decreased intercell contact (Nieto et al., 2001).
Cell walls of blanched apple showed good optical density, only slightly lower than
that of raw apples. Striations with zones of high and low electron density were observed
but were less pronounced compared with those in heated mango. Separation of adjacent
cells caused by dissolution of the middle lamella was not observed (micrographs not
shown). Shrinkage of apples due to blanching was approximately 23%, a value very
similar to the reported porosity of the fruit (air spaces comprise 20–30% of flesh tissue
volume) (Nieto et al., 1998).
These alterations in the ultrastructure and microstructure of heated apple, mango,
and strawberry tissues might explain, at least partially, the drying behavior (Figure 4.3).
For strawberry, blanching would enhance Deff value due to:
1. The elimination of the cell membrane’s resistance to water diffusion
2. A decrease in the resistance of the cell walls to water flux
In apple, the effect of blanching on Deff could be ascribed to the increase in density
of apples due to air exhaustion and the slight contraction of tissues, all phenomena
predominating over the slight modification of cell wall resistance to water flux and/or
the decreased transmembrane transport resistance due to membrane disruption.
The decrease of Deff in mango could be attributed to:
1. The slight increase in density due to the cell collapse
2. The alteration of cellular contents (gelatinization of starch and denatur-
ation of slimes)
Both of these phenomena are more noticeable than the low ultrastructural dam-
age of the cell wall and the disruption of membranes that would facilitate water flow.
2.50E-05
2.00E-05
Deff(cm2/s)
1.50E-05
1.00E-05
5.00E-06
0.00E+00
apple strawberry mango
control; steam blanched
FIGURE 4.3 Experimental Deff values for the first falling rate period of air drying of raw and
blanched fruits (drying temperature: 60°C for mango and apple; 55°C for Pájaro var. strawberrry).

4.3.2 EFFECT OF OSMOTIC TREATMENT
Drying rate can be also affected by various structural modifications produced in the
fruit tissue by osmotic treatments (Table 4.2) (Alzamora et al., 1997).
A general aspect of the drying curves of mango and apple as affected by glucose
dipping at atmospheric pressure or in vacuum to reach aw 0.97 is seen in Figure 4.4.
m (g H2O / g DM)
10
9 (a)
8
0
0 100 200 300 400 500 600
2 2
t / lo (min / cm )
_
m (g H2O / g DM)
6
(b)
5
0
0 100 200 300 400 500 600
t / lo2 (min / cm2)
control (raw) ; x blanched; * osmotically dehydrated to aw 0.97 (atmospheric);

osmotically dehydrated to aw 0.97 (in vacuum).
FIGURE 4.4 Effect of blanching and glucose osmotic dehydration on drying curves of (a) apple
and (b) mango at 60°C.

TABLE 4.2
Major Reported Structural Phenomena Due to Osmotic Dehydration
in Connection with Water Transport Rate during Drying of Fruit Tissues
(Various Sources)
Collapse of the tissue due to water removal
Loss/redistribution of native sugars and solutes due to decompartmentation and/or passive transport
through membranes; uptake of osmotic solute(s)
Alteration of cell wall ultrastructure due to (a) leakage of soluble pectins to the osmotic medium that
reduces the cohesiveness of the polysaccharide matrix and/or (b) specific interactions among
solute(s) and cell wall components that modify to different degrees the strength of the walls as well
as the porosity of the pectin matrix
Starch gelatinization
Stabilization of three-dimensional structure of proteins
Plasmolysis and/or disruption of tonoplast and plasmalemma
Osmotic treatment appreciably reduced the moisture content of the fruits. No con-
stant drying period was observed at any of the conditions studied. For both fruits,
experimental Deff values decreased as the glucose concentration of the impregnation
solution increased, that is, as aw of the slabs decreased (Figure 4.5).
When glucose impregnation was performed under vacuum, the Deff value was
similar to that of the atmospheric treated slab with the same aw (0.97) for mango, but
vacuum impregnated apple exhibited a Deff value much lower than that corresponding
to apple impregnated at atmospheric pressure with aw 0.97 and similar to the Deff value
of the atmospheric impregnated fruit with aw 0.93.
Shrinkage of mango and apple tissues before drying depended on the pretreatment
(Figure 4.5). The percentage volume reduction shown by atmospheric osmotically
dehydrated mango or apple to aw 0.97 was similar to that exhibited by blanched
tissues (≅10% and ≅23%, respectively), while treatments in glucose solutions with
aw 0.95 or 0.93 resulted in a more severe volume change (≅40–43%). Vacuum treated
samples showed a greater shrinkage compared with the atmospheric impregnated
fruit with the same aw (19 vs. 10% for mango and 37 vs. 24% for apple).
Sugar composition of mango and apple tissues was significantly influenced by the
osmotic process (Table 4.3). Sugar exchange during osmosis (glucose gain and loss of
“natural” sugars, fructose and glucose) resulted in modified sugar profiles of the final
products. Glucose content of mango and apple tissues impregnated at atmospheric
pressure increased with the increasing glucose concentration of the solution. Vacuum
glucose impregnated mango showed a lower uptake of glucose and a lower loss of
“natural” sugars than the slabs impregnated at atmospheric pressure with aw 0.97, while
the glucose content of the vacuum treated apple was 35% greater than that of atmo-
spheric impregnated slabs with the same aw.
Light microscopy observations of atmospheric glucose impregnated apples to reach
aw 0.97 showed original arrangements of cells rather well maintained (micrographs not
shown). Cells looked rounded but well defined, with plasmalemma separated from the
wall. Examinations with transmission electron microscopy (TEM) indicated electronic

50
40
30
Sv,%
20
10
0
apple mango
2.50E-05
2.00E-05
Deff(cm2/s)
1.50E-05
1.00E-05
5.00E-06
0.00E+00
apple strawberry mango
control; osmotically dehydrated, atmospheric pressure, aw 0.97;

osmotically dehydrated, vacuum, aw 0.97; osmotically dehydrated, atmospheric
pressure, aw 0.95; osmotically dehydrated, atmospheric pressure, aw 0.93
FIGURE 4.5 Experimental Deff values and volume shrinkage (Sv, %) for osmotically dehy-
drated apple, mango, and strawberry (Tioga Leico, var.).
dense cell walls and a network of microfibrils and a pectic matrix very similar to those
of the fresh fruit (Figure 4.6C). When impregnation was made in vacuum, more
rounded cells were observed in light microscopy (LM) (micrographs not shown), with
some spaces between cells, but the degree of cell-to-cell contact did not decrease. Cell
walls appeared with a very pronounced staining, exhibiting a very densely packed
fibrillar material (Figure 4.6D).
Original arrangements of cells were also maintained in atmospheric glucose
impregnated mango tissues with aw 0.97 or 0.93. Tonoplast and plasmalemma appeared

TABLE 4.3
Sugar Content (% W/W) of Glucose Impregnated Mango and Apple Slabs
Mango Apple
Pretreatment Fructose Glucose Sucrose Fructose Glucose Sucrose
At Atmospheric Pressure
Control 3.6 ± 0.1 2.3 ± 0.1 4.3 ± 0.1 5.6 ± 0.1 4.1 ± 0.1 2.6 ± 0.1
Immersed in aqueous glucose solution of

aw 0.97 2.3 ± 0.1 17.6 ± 0.3 1.8 ± 0.01 3.8 ± 0.1 12.6 ± 0.3 1.5 ± 0.1
aw 0.95 — — — 4.0 ± 0.1 20.9 ± 0.1 2.4 ± 0.1
aw 0.93 2.6 ± 0.1 35.7 ± 0.9 1.9 ± 0.2 3.8 ± 0.1 27.4 ± 0.9 1.3 ± 0.2
In Vacuum
Control 3.6 ± 0.1 2.3 ± 0.1 4.3 ± 0.1 7.2 ± 0.1 3.7 ± 0.1 2.5 ± 0.2
Vacuum impregnated with glucose solution of

aw 0.84 (final fruit 2.9 ± 0.1 6.9 ± 0.1 3.8 ± 0.2 7.0 ± 0.1 16.5 ± 0.3 1.5 ± 0.2
aw = 0.97)
intact, and cellular contents were plasmolyzed; this effect was very pronounced at aw
0.93. Due to plasmolysis, starch granules were localized near the center of the cells
(micrographs not shown). As seen in TEM (Figure 4.6A), fibrillar material appeared
darkly stained and tightly packed, and the middle lamella, either cementing adjacent
cells or lining the walls at the intercellular spaces (micrographs not shown), exhibited
high electron density.
Mango tissues impregnated under vacuum (aw 0.97) also showed a cell assembly
similar to that of the control and cytoplasm plasmolysis. In some zones, disrupted
membranes were observed. Ultrastructure observations indicated densely stained cell
walls with clear reticulate pattern and a nitid middle lamella (Figure 4.6B).
On the contrary, the optical density of cell walls of osmotically dehydrated
strawberries was lower than the optical density of fresh strawberry cell wall. The
middle lamella partially disappeared, and distortion of miofibrils occurred (micro-
graphs not shown), indicating degradation of the hemicellulose polysaccharides
present in the cell wall, breakdown of pectins, and changes in the “crystallinity” of
cellulose.
The many changes in ultrastructure, microstructure, and composition induced
by predrying osmosis could affect drying behavior in many ways. In mango and
apple, cell walls of glucose-impregnated tissues were not modified (hence, neither
were the wall transport properties of the wall) to a great extent compared with the
control. But shrinkage and glucose uptake during the impregnation step would
increase the overall water transport resistance. The magnitude of the increase would
be dependent on the degree of cell collapse and sugar incorporation.
In strawberry, glucose infusion would cause no effect on drying rate due to two
counter-blanching effects: increased water transport resistance due to solute uptake

FIGURE 4.6 Ultrastructure (TEM) of parenchyma tissue of mango and apple as affected by
osmotic dehydration. A, B: mango; C, D: apple. A: immersed in glucose solution of aw 0.97.
Densely stained wall and plasmolyzed cytoplasm; intermixed microfibrillar pattern; conspic-
uous middle lamella. B: vacuum impregnated, aw 0.97. Interrupted membranes; visible middle
lamella; moderate electronic density of the walls. C: immersed in glucose solution of aw 0.97.
Miofibrillar disorganization but moderately electron dense wall. D: vacuum impregnated, aw
0.97. Walls darkly stained; very densely packed fibrillar material; broken membranes with
formation of vesicles. Scale: A, D: 500 nm; B, C: 1 µm.
and the reduction of the cell wall resistance due to degradation/solubilization of

polysaccharides of the cell wall.
4.4 CONCLUSIONS
There is a close relation between drying kinetics and structural modifications under-
gone by fruits under blanching and osmotic dehydration pretreatments. Resistance
of fruit tissues to water flux could be decreased by disruption of membranes and
degradation/solubilization of the cell wall matrix, while drying rate would be
adversely influenced by cell collapse, solute(s) gain, starch gelatinization, and protein
denaturation.

NOMENCLATURE
l0 Half-thickness of the slab (cm)
Re Sphere radius (cm)
F0 Fourier number
DM Dry matter (g)
aw Water activity
m Average moisture content, dry basis (kg water/kg dry matter)
mo Initial moisture content, dry basis (kg water/kg dry matter)
m Moisture content, dry basis (kg water/kg dry matter)
me Moisture content in equilibrium with the surrounding temperature and humidity
conditions, dry basis (kg water/kg dry matter)
2
Deff Effective moisture diffusivity in the solid (cm /sec)
x Characteristic dimension (cm)
Ψ Shape factor of a solid, adimensional
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research needs and opportunities, Drying Technol., 14, 1329–1368, 1996.
Aguerre, R.J., Gabitto, J.F., and Chirife, J., Shape factors for the analysis of diffusion in air
drying of grains, Int. J. Food Sci. Technol., 22, 701–705, 1987.
Alzamora, S.M., Chirife, J., and Viollaz, P.E., A simplified model for predicting the temper-
atures of foods during air dehydration, J. Food Technol., 14, 369–380, 1979.
Alzamora, S.M, Gerschenson, L.N., Vidales, S.L., and Nieto, A., Structural changes in min-
imal processing of fruits: some effects of blanching and sugar impregnation, in Food
Engineering 2000, Fito, P., Ortega-Rodríguez, E., and Barbosa-Cánovas, G.V., Eds,
Chapman and Hall, New York, 1997.
Alvarez, C.A., Aguerre, R., Gómez, R., Vidales, S., Alzamora, S.M., and Gerschenson, L.N.,
Air dehydration of strawberries: effects of blanching and osmotic pretreatments on
the kinetics of moisture transport, J. Food Eng., 25, 167–178, 1995.
Becker, H.A., A study of diffusion in solids of arbitrary shape, with application to the drying
of the wheat kernel, J. Appl. Polym. Sci., 1, 212–216, 1959.
Ilker, R. and Szczesniak, A.S., Structural and chemical bases for texture of plant foodstuffs,
J. Texture Stud., 21, 1–36, 1990.
Lewicki, P.P., Effect of pre-drying treatment, drying and rehydration on plant tissue properties:
a review, Int. J. Food Prop., 1, 1–22, 1998.
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Nieto, A., Salvatori, D., Castro, M.A., and Alzamora, S.M., Air drying behavior of apples as
affected by blanching and glucose impregnation, J. Food Eng., 36, 63–79, 1998.
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thermodynamics of irreversible processes, J. Theor. Biol., 26, 181–214, 1970.
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in foodstuffs, Drying Technol., 14, 2225–2253, 1996.

Pretreatment Efficiency
5 in Osmotic Dehydration
of Cranberries
S. Grabowski and M. Marcotte
CONTENTS
5.1 Introduction
5.2 Experimental Procedure
5.2.1 Osmotic Dehydration
5.2.2 Pretreatment Techniques
5.3 Results and Discussion
5.3.1 Selection of the Best Pretreatment
5.3.1.1 Coefficient of Pretreatment Efficiency
5.3.1.2 Taste Acceptability
5.3.2 Simple Diffussivity Model for Cut Cranberries
5.4 Conclusions
Nomenclature
Acknowledgments
References
5.1 INTRODUCTION
Dehydration of small fruits, such as grapes, blueberries, cranberries, cherries, and
gooseberries, is restricted by the fruit outer surface (cuticle), which plays a major
role in the control of transpiration, and in protecting the fruit against weather
inclemencies or attacks from insects and parasites (Mazliak, 1970; Somogyi and
Luh, 1986; Somogyi et al., 1996). This cuticle, if it has not been damaged, has little
permeability to moisture (Suarez et al., 1984). It includes two classes of compounds:
natural waxes and cutin. The waxes contain a particular kind of lipid, which is an
ester of high molecular weight, resulting from the combination of a fatty acid with
a long chain monoalcohol. With the exception of the wax esters, natural fruit waxes
contain a mixture of hydrocarbons (paraffins and olefins), fatty acids (normal,
hydroxylated, and ethylenic), ketones, alcohols, and aldehydes. All of these com-
pounds have high molecular weights and similar physical properties, especially
insolubility in water and a melting point between 40 and 100°C. Ursolic acid is

widespread on the surface of apples, cranberries, pears, and prunes, among other
fruits. This acid is very difficult to dissolve from the fruit skin. For example, at 15°C
one part of this acid dissolves in 88 parts of methanol, in 178 parts of ethanol (or in
35 parts of boiling ethanol), or in 140 parts of ether and is soluble in glacial acetic
acid and 2% alcoholic NaOH (Mercks Index, 1983). The second layer of the fruit skin
(cutin) is poorly soluble in most organic solvents, as the chains of constituents are
firmly fixed by cross-polymerization in the membrane (Mazliak, 1970).
In practice, many different pretreatment techniques before fruit dehydration have
been developed and applied. Saravacos and Charm (1962) divided fruits and vegetables
into three general groups: those with a homogenous structure (carrot, blanched potato,
garlic); those with a porous structure (apples, peaches, pears); and those possessing a
surface skin (grapes, cranberries, cherries, gooseberries, etc.). The fruits from the third
group need special pretreatments, as drying without pretreatment is not practical and
requires a long time and much energy. The authors also specified conditions for the
proper surface agent selection. The agent should be nontoxic, water soluble or easily
dispersible, relatively low in molecular weight, and inexpensive.
Detailed outlines of the California pretreatment practices for sun drying of fruits
were presented by Heid and Joslyn (1967). Short (3–30 sec) hot or cold lye dip
(0.25–1% of lye in water) is the most typical pretreatment for prunes, grapes, apricots,
peaches, and nectarines. Most recently, a review of predrying treatment techniques
and their effects on drying and rehydration of plant tissues was presented by Lewicki
(1998). The author divided all pretreatments into two main groups: chemical (inorganic
and organic) and nonchemical (heating, blanching, freezing, etc.). According to the
author, the main beneficial effects of pretreatment included reduced drying time,
denaturation or inactivation of surface enzymes, removal of intracellular air, soften-
ing of the texture, and increased rehydration rate. According to Kostaropoulus and
Saravacos (1995), Grabowski et al. (1994), and Masi and Riva (1988), the drying time
of surface pretreated grapes (immersed in ethyl oleate, etc.) was reduced by about
half. Venkatachalapathy and Raghavan (1997) found a positive effect using a combi-
nation of ethyl oleate (3%) and NaOH (0.5%) for microwave drying of strawberries.
However, the convective drying rate of the strawberries was improved by only about
10% as a result of this pretreatment. In another study, surfactant pretreatment of basil
leaves increased the drying rate by a factor of 14 (Rocha et al., 1993).
In light of the above, the main objective of this study was to compare the effect
of some of the most typical surface pretreatment techniques on osmotic dehydration
and sugar infusion of cranberries. Some of the techniques tested in this study were
theoretical rather than practical. They were selected based on knowledge of the
characteristics of ursolic acid, the main component of the cranberry skin waxes.
5.2 EXPERIMENTAL PROCEDURE

5.2.1 OSMOTIC DEHYDRATION
The experimental procedure enabled measurement of two important parameters of
osmotic dehydration: water loss (WL) and mass reduction (MR). The third parameter
of the process, solid gain (SG), which is mainly the infusion of sugar into the fruit

structure, is the difference between the water loss and the mass reduction, as shown
in Equations (1–3). All three parameters were calculated on the basis of 100 g of
initial mass of fresh (control) or surface pretreated fruits:
MR = 100 – M2 (5.1)
WL = 100 × b1 – M2 × b2 (5.2)
SG = WL – MR (5.3)
Small scale laboratory equipment (Figure 5.1) was used to perform osmotic dehy-
dration tests for fresh whole (control) and pretreated cranberries. Five vertical cylin-
drical columns of 250 ml each (5.08 cm diameter, 12.7 cm high) were connected in
parallel to a positive displacement pump (Speed-trol, Sterling Electric Inc., New
York) with a variable flow rate (1–20 l/min). Using control valves, the syrup flow
rate was adjusted to be equal and constant through each column during the entire
process (1 l/min for each column). Sucrose syrup at 67.5°Brix (commercially called
liquid sugar) was recirculated from a tank (30 l) equipped with a heating jacket,
through the test columns filled with cranberries, and back to the tank. Heating of
the syrup in the tank was controlled to obtain a constant temperature at the inlet of
the columns of 50 ± 2°C. The actual mass of the samples and the moisture content
were determined after removing the samples one by one from the columns after a
given period of time. All tests were performed at least in triplicate.
The moisture content in the cranberry samples was determined using a standard
procedure by drying the samples in a vacuum oven at 70°C for 6 h (AOAC, 1984).
The sugar content of the cranberry samples was determined using a high pressure
4 2
1
3
Steam
Condensate
FIGURE 5.1 Laboratory osmotic dehydration unit: (1) osmotic syrup tank; (2) mixer; (3) variable
speed pump; (4) flow regulating valves; (5) dehydration columns filled with cranberry samples
(250 ml each).

liquid chromatography (HPLC) after grinding a defined quantity in distilled water
(Marcotte and LeMaguer, 1991, 1992). The sugar concentration of the syrup was
assumed to be constant during the process, as the mass of syrup circulating into the
system was approximately 40 times more than the mass of cranberries in the col-
umns. At the beginning and end of each run, the concentration of sugar in the syrup
was measured (refractometer, Minolta Co., Ltd., Osaka, Japan) and adjusted to
67.5°Brix, if necessary.
5.2.2 PRETREATMENT TECHNIQUES

Frozen cranberries (Vaccinium macrocarpon) of Stevens or Early Black varieties
were purchased from a local cranberry farm and stored in a cold room (−4°C) until
use. Each time, five samples of cranberries (about 100 g each) were thawed to +4°C
and pretreated using one of the 13 procedures presented in Table 5.1. Among
pretreatments, NaOH (2%) in 95% ethanol (pretreatment No. 4) and pectinase
(pretreatment No. 5) have a theoretical rather than practical importance. These were
included in the pretreatment list because of the solubility characteristics of ursolic
acid (Mercks Index, 1983). Ethyl oleate, ethanol, NaOH, and enzyme (pectinase)
applied in the pretreatment were supplied by Sigma-Aldrich Chemical Co. (Milwaukee,
WI) and sodium oleate by J.T. Baker (Philipsburg, NJ).
TABLE 5.1
Characteristics of the Pretreatment Techniques Applied and Experimental
Values of Coefficients of Pretreatment Efficiency (ζζDEH for Moisture
Removal and ζINF for Sugar Infusion)
Pretr. Conc. Time Temp
No. Type Description (% mass) (min) (ºC) ζDEH ζINF
1. CH Ethyl oleate 3 3 20 2.8 2.45

2. CH Sodium oleate 3 3 20 2.6 2.3
3. CH NaOH in water 0.5 3 20 3.15 3.1
4. CH NaOH in ethanol (95%) 2 3 20 2.7 2.0
5. CH Pectinase 0.3 10 20 1.1 1.1
6. T Steaming — 3 100 5.7 5.05
7. T Boiling water — 3 100 5.6 4.5
8. M Cut into halves — — 20 6.1 5.1
a
9. M Perforating — — 20 3.5 2.5
10. CO Ethyl oleate: hot dip 3 3 100 5.6 4.9
11. CO Sodium oleate: hot dip 3 3 100 5.5 4.7
12. CO NaOH in water: hot dip 0.5 3 100 5.8 4.95
13. CO Ethyl oleate + NaOH: hot dip 3 + 0.5 3 100 6.3 5.4
Note: CH, chemical; T, thermal; M, mechanical; CO, combined (chemical + thermal).

a
10 small holes (1 mm diameter) per berry.

5.3 RESULTS AND DISCUSSION
5.3.1 SELECTION OF THE BEST PRETREATMENT
Pretreatment techniques applied before osmotic dehydration of cranberries were
evaluated for their effect on cranberry moisture reduction and sugar infusion. The
faster osmotic dehydration and sugar infusion were achieved, the better the
pretreatment effect obtained. Two specific measurements of pretreatment efficiency
were determined:
1. Coefficient of pretreatment efficiency (ζ)
2. Taste acceptability of the cranberries after 5 h of osmotic process
5.3.1.1 Coefficient of Pretreatment Efficiency
Weitz et al. (1989) defined the coefficient of pretreatment efficiency as:

ζ = τN/τP (5.4)
where τN and τP are the process times to reach an assumed dehydration (or infusion)
level in the food, without (N) and with (P) a given type of pretreatment, respectively.
Normally, unless atypical changes in the food structure arise, a coefficient of pre-
treatment efficiency higher or equal to 1 (ζ ≥ 1) is found. Table 5.1 presents experi-
mental results of different pretreatment tests. A final moisture content of 50% (w.b.)
and a mass reduction of 18% were assumed. Figure 5.2 shows data of dehydration
kinetics of pretreated cranberries.
The best result was achieved by combining chemical and thermal methods (pre-
treatment No.13 [NaOH and ethyl oleate in boiling water]: ζDEH = 6.3 and ζINF = 5.4).
Similar results were obtained for cranberries cut into halves (ζDEH = 6.1 and ζINF = 5.1)
8
MOISTURE CONTENT, X, dry basis
Halves
7
Steamed
6
Sodium oleate
5
Ethyl oleate
4
3 Pectinase
2 Untreated
1
0 12 24 36
Thousands
PROCESSING TIME, sec
FIGURE 5.2 Effect of different pretreatments on cranberry dehydration kinetics.

and other combinations of chemical and thermal pretreatments (pretreatments No. 10,
11, 12). The main problem associated with the combined pretreatments was the high
sensitivity of the process to even small differences in initial temperature, size, and
variety of tested cranberries. The range of effective pretreatment times for these
techniques (pretreatments No. 10–13) and other thermal methods (pretreatments No. 6
and 7) was very narrow.
Overprocessing of berries resulted in the destruction of texture, while underpro-
cessing was an insufficient pretreatment effect. Thus, based on the results presented
in Table 5.1, cutting cranberries into halves was found to be the most practical pre-
treatment before osmotic dehydration of cranberries. For cranberries cut into halves,
approximately 30% of the total surface was exposed to an effective mass transfer
(dehydration and infusion), and the rest of the surface (approximately 70%) was
covered by the skin with a mass transfer resistant to the layer of wax.
5.3.1.2 Taste Acceptability
A panel of 10 untrained testers evaluated the taste of cranberries pretreated with 13

different techniques and then subjected to 5 h osmotic dehydration in a sugar syrup
of 67.5° Brix at 50°C. An evaluation scale of 0–100 points was applied (0 = totally
rejected; 100 = maximum preference). Figure 5.3 shows the average values. The lowest
values were given to all chemically pretreated cranberries, medium to thermal and
combined (chemical and thermal), and the highest to cranberries cut into halves.
According to comments of the testers, each of the chemical or thermal pretreatments
100
90
80
TASTE ACCEPTABILITY, %
CHEMICAL
70 MECHANICAL
THERMAL
60
COMBINED
50
40
30
20
10
0
1 2 3 4 5 6 7 8 9 10 11 12 13
PRETREATMENT TYPE (Number)
FIGURE 5.3 Results of taste panel acceptability evaluation. The numbers of the pretreatments
refer to Table 5.1.

caused some specific changes in the taste or texture of the berries. Thus, the mechanical
cutting of cranberries into halves was the most effective pretreatment tested. The other
mechanical pretreatment, perforating the skin, was not successful, probably because
a very low proportion of the skin was opened to the osmotic syrup. If it were possible
to obtain a high enough number of perforations (or surface area opened by perfo-
ration), for example, 20–30% or more, this technique could also be practical.
5.3.2 SIMPLE DIFFUSSIVITY MODEL FOR CUT CRANBERRIES

After selection of the most effective pretreatment technique, attention was given to
the mathematical description of the mass transfer between cut cranberries and the
osmotic syrup. It is obvious that water and sucrose are mainly transferred through
the cut surface of the berries, with only a small proportion being transferred through
the uncut surface covered by the skin. Therefore, the entire mass transfer is the sum
of two quantities: one related to the cut surface of the berry, and the second to the
unaffected surface. Introducing a surface ratio parameter (α), which is the ratio of
the cut surface area divided by total surface of the cut cranberry,
α = Fopen by cut/Ftotal (5.5)
and introducing different moisture (or infused sugar) effective diffusivity for the cut
(Deff cut) and the uncut (Deff uncut) surface, the following simplified model of mass
exchange between cut cranberry and osmotic syrup is proposed:
Deff = αDeff cut + (1 – α)Deff uncut (5.6)
To verify this model, a special set of tests was performed. Cranberries of uniform
size were cut into halves and additionally from both sides, to achieve approximately
50% of open surface. Samples of uncut cranberries (reference: α = 0), cranberries
cut into halves (30% open surface: α = 0.3), and cranberries cut from both sides
(for 50% of open surface: α = 0.5) were placed into the osmotic dehydration unit
(Figure 5.1). The osmotic dehydration and infusion treatment was performed in a
sucrose syrup of 67.5° Brix at 50°C.
Figure 5.4 shows examples of the dehydration kinetics. Figure 5.5 shows examples
of sugar infusion kinetics of cut and uncut cranberries. At first, no significant differ-
ences in osmotic process of either variety of cranberries were observed. As predicted,
the water content of cranberries cut to 50% of open surface (α = 0.5) was reduced at
a higher rate than that of those cut into halves (α = 0.3). The dehydration time of
uncut or whole cranberries was many times longer than for cut cranberries. For the
sugar infusion, a similar situation was observed (Figure 5.5).
Based on Fick’s second law of unsteady state mass diffusion (Crank, 1975), and
assuming a spherical geometry and a uniform initial temperature and concentration
distribution inside the berry, an effective coefficient of diffusion (Deff) was calculated
from the following equations (Crank, 1975; Nsonzi and Ramaswamy, 1997):
2 2 2
WR = 6/π exp(–Deffπ τ/a ) (5.7)
2 2
Deff = Ba /π (5.8)

7
WATER CONTENT, X, dry basis

6
4 Untreated Halves "Early Black"
3 Halves Cut (50% open

"Stevens" surface)
2
0
0 10 20 30 40
Thousands
FIGURE 5.4 Kinetics of moisture removal (osmotic dehydration) from samples of cut and
uncut (reference) cranberries.
0.4
Untreated (whole)
SUGAR CONTENT (S), kg dry basis
Halves "Stevens"
Halves "Early black"
kg
Cut (to 50% open)

0.3
0.2
0.1
0
0 5 10 15 20
Thousands
FIGURE 5.5 Kinetics of sugar infusion into uncut (reference) and cut cranberries.

where τ is the process time; a is a characteristic dimension of the cranberry, and B
is the slope of the kinetic curves ln(WR) or ln(SI) against time (t). Figure 5.6 shows
the moisture reduction, and Figure 5.7 shows the sugar infusion.
2
Based on the statistical analysis (R = 0.91 − 0.96), effective diffusion coefficient
values were found to obey the following equations:
-1
-2
ln(WR)
Untreated
-3
Halves "Stevens"
-4
Halves "Early Black"
-5 Cut (50% open surface)
-6
0 7200 14400 21600
FIGURE 5.6 Calculation of the effective moisture diffusivity for moisture reduction of
cranberries.
0
ln(SI)
-2
-4
Untreated (whole)
Halves "Stevens"
Halves "Early black"
Cut (to 50% open)
-6
0 7200 14400 21600
FIGURE 5.7 Calculation of the effective diffusivity for sugar infusion into cranberries.

For water loss (osmotic dehydration):
–9 –11
Deff = 2.38 10 α + 1.7 10 (1 − α) (5.9)
For sugar gain (infusion):
–9 –11
Deff = 10 α + 1.65 10 (1 − α) (5.10)
Equations (5.9) and (5.10) show that the effective diffusion coefficient for the cut
area of a cranberry is around 100 times higher than that of the uncut surface of the
berry. The values of effective diffusivity for dehydration and infusion varied with
process temperature and concentration of the osmotic syrup. In this work, both
parameters were kept constant to study the clear effect of pretreatment techniques.
For cranberries cut into halves (30% of open surface or α = 0.3), average effective
–10 2 –10 2
mass diffusivities of about 7 × 10 m /sec and 3.1 × 10 m /sec were obtained
for dehydration and sugar infusion, respectively. In osmotic dehydration literature,
similar values have been reported (Rastogi and Raghavarao, 1997; Kaymak and
Kincal, 1994; Marcotte and LeMaguer, 1992; Lewicki et al., 1984). Lower values
–10 2 –10 2
of Deff, i.e., 2–5 × 10 m /sec for dehydration and 0.2–2 × 10 m /sec for infusion,
were determined by Nsonzi and Rawaswamy (1997) for blueberries that were
untreated before the osmotic process.
To validate our mathematical model, shown in Equation (5.6), a special osmotic
dehydration test for cranberries cut from one side to obtain 15% of open surface (α =
–10 2
0.15) was performed. Experimental values of mass diffusivity of 4 × 10 m /sec for
–10 2
dehydration and 1.9 × 10 m /sec for sugar infusion were obtained. These values
–10 2
compared well with values calculated from Equations (5.9) and (5.10) (3.7 × 10 m /sec
–10 2
for dehydration and 1.64 × 10 m /sec for sugar infusion). Therefore, this simple model
can be applied to other fruits and vegetables cut before the next steps of processing.
5.4 CONCLUSIONS
From the point of view of efficiency and taste acceptability, the best practical
pretreatment of cranberries before osmotic dehydration and infusion was to cut
the berries into halves. Taking into account the ratio of the open surface from
cutting to the total surface of cut cranberries, a simple proportional model for the
effective moisture loss and sugar gain diffusivities was proposed. Within the range
of experimental data, effective diffusion coefficients for moisture loss and sugar gain
were approximately 100 times higher for the cut surface than for the uncut cranberries.
The model was validated experimentally by comparing theoretical values to experi-
mental data generated for berries with 15% of open surface. This model could be
applied to other fruits and vegetables that are cut before other processing operations.
NOMENCLATURE
a Characteristic dimension of cranberry, m
–1
B Slope of the kinetic curves (absolute value from Equation 5.8), s

b Cranberry moisture content, w.b.
2
Deff Effective coefficient of diffusion, m /sec
2
F Surface of the single berry, m
MR Mass reduction, g/100 g of initial mass
S Sugar content, kg/kg dry basis
SG Solid gain, g/100 g of initial mass
SI Dimensionless sugar intake: (S – SEQ)/(S1 − SEQ)
WL Water loss, g/100 g of initial mass
WR Dimensionless water reduction: (X – XEQ)/(X1 – XEQ)
X Moisture content, kg/kg dry basis
α Surface ratio: open by cut to total
τ Process time, sec
ζ Coefficient of pretreatment efficiency (Equation 5.4)
SUBSCRIPTS
1, 2 Initial and final, respectively
DEH Dehydration
EQ Equilibrium
INF Infusion of sugar
N, P Without pretreatment and pretreated, respectively
ACKNOWLEDGMENTS
Financial support from the Office of Energy Research and Development of Canada
(Program PERD) is gratefully acknowledged. Special thanks go to Francois Brunet
for the HPLC sugar tests.
REFERENCES
AOAC, Official Methods of Analysis, 14th ed., Association of Official Analytical Chemists,
Washington, DC, 1984.
Crank, J., The Mathematics of Diffusion, Clarendon Press, Oxford, 1975, pp. 89–103.
Grabowski, S., Mujumdar, A.S., Ramaswamy, H.S., and Strumillo, C., Osmo-convective
drying of grapes, Drying Technol., 12, 1211–1219, 1994.
Heid, J.L. and Joslyn, M.A., Fundamentals of Food Processing Operations, AVI, Westport,
CT, 1967, p. 510.
Kaymak, F. and Kincal, N.S., Apparent diffusivities of reducing sugars in potato strips
blanched in water, Int. J. Food Sci. Technol., 29, 63–70, 1994.
Kostaropoulos, A.E. and Saravacos, G.D., Microwave pre-treatment for sun-dried raisins,
J. Food Sci., 60, 344–347, 1995.
Lewicki, P., Effect of pre-drying treatment, drying and rehydration of plant tissue properties:
a review, Int. J. Food Prop., 1, 1–22, 1998.
Lewicki, P., Lenart, A., and Turska, D., Diffusive mass transfer in potato tissue during osmotic
dehydration, Food Technol. Nutr. — Annals of Warsaw SGGW-AR, 16, 25–32, 1984.

Marcotte, M. and LeMaguer, M., Repartition of water in plant tissues subjected to osmotic
processes, J. Food Process Eng., 13, 297–320, 1991.
Marcotte, M. and LeMaguer, M., Mass transfer in cellular tissues. Part II: Computer simula-
tions vs. experimental data, J. Food Eng., 17, 177–199, 1992.
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Food Materials, Bruin, S., Ed., Elsevier, Amsterdam, 1988, pp. 203–214.
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Academic Press, New York, 1970, pp. 209–221.
Mercks Index, An Encyclopedia of Chemicals, Drugs, and Biologicals, Mercks & Co., Inc.,
Rahway, NJ, 1983, pp. 1413–1414.
Nsonzi, F., and Ramaswamy, H.S., Osmotic dehydration kinetics of blueberries, Drying
Technol., 15, 705–723, 1997.
Rastogi, N.K. and Raghavarao, K.S., Water and solute diffusion coefficient of carrot as a
function of temperature and concentration during osmotic dehydration, J. Food Eng.,
34, 429–440, 1997.
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on drying rate and color retention of basil (Ocimum basilicum), Lebensm.-Wiss.
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Saravacos, G.D. and Charm, S.E., Effect of surface active agents on the dehydration of fruits
and vegetables, Food Technol., 16, 91–93, 1962.
Somogyi, L.P. and Luh, B.S., Dehydration of foodstuffs, in Commercial Fruit Processing,
2nd ed., Woodroof, J.G. and Luh, B.S., Eds., AVI, Westport, CT, 1986, pp. 353–405.
Somogyi, L.P., Ramaswamy, H.S., and Hui, Y.H., Processing Fruits: Science and Technology—
Biology, Principles and Applications, Technomic, Lancaster, PA, 1996, pp. 14–24
and 185–220.
Suarez, C., Loncin, M., and Chrife, J., A preliminary study of the ethyl oleate dipping treatment
on drying rate of grain corn, J. Food Sci., 49, 236–238, 1984.
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drying of strawberries, Proceedings of the Annual Conference of the Canadian Society
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pp. 215–224.
Weitz, D.A., Lara, M.A., Piacentini, R.D., and Feldman, S., Dipping treatment effects on
simulated prune solar drying, Can, Inst. Food Sci. Technol. J., 22, 133–136, 1989.

Mass Transfer
6 Description of the
Osmodehydration
of Apple Slabs
E. Azuara-Nieto, G.F. Gutiérrez-López,
and C.I. Beristain-Guevara
CONTENTS
6.1 Introduction
6.2 Theoretical Frame
6.4 Results
6.4.1 Mathematical Modeling
6.5 Discussion
6.6 Conclusions
Nomenclature
Acknowledgments
References
6.1 INTRODUCTION
Over the past few years, a number of reports related to mass transfer during osmotic
dehydration (OD) have appeared in the technical literature. However, a full under-
standing of the mechanisms involved in the simultaneous countercurrent mass flows
has not been reached.
Transport phenomena during OD depend on the diffusion coefficient and on the
driving force for water and solutes. By manipulating processing factors affecting
these parameters, it is possible to reach different levels of dehydration or impreg-
nation of the material under treatment. A common property of foodstuffs subjected to
osmotic dehydration is the formation of a layer of high solute concentration on the
product surface. Osmotically dehydrated gels and plant tissues in sucrose solutions
display a solute impregnation localized on a superficial layer 2–3 mm from the surface.
Solute layer formation plays a role in mass transfer control during osmotic dehydration,

enhancing water loss and reducing both solute uptake and losses of soluble solids
from the foodstuff as ascorbic acid and fructose (Vial et al., 1991; Saurel et al.,
1994). Additionally, the presence of the solute layer may have an effect on product
behavior during storage or further dehydration (Karathanos et al., 1995). Only a
limited number of reports suggest the existence of three stages during the osmotic
dehydration process (Toupin et al., 1989; Le Maguer and Yao, 1995). Among these,
the model proposed by Le Maguer and Yao is the only one that attempts to explain
the mass transfer in each stage. These authors were able to model the operation
closely to the behavior of the real tissue by employing thermodynamic concepts for
irreversible processes. However, the main drawbacks of the model were the vast
number of biophysical properties that have to be known for a given foodstuff and
the need to develop a numerical solution of the equations.
The purpose of this work was to develop a kinetic model based on shrinking
core theory (Levenspiel, 1976), in order to describe the osmotic dehydration stages
of apples and to obtain information about the mass transfer mechanisms along the
process.
6.2 THEORETICAL FRAME

Variability of raw materials is one of the most important sources of error when
collecting mass transfer data during osmodehydration. Agricultural practices, variety
of the product, and level of maturity, among other factors, affect composition and
physical–chemical properties of fruits and vegetables. The complex heterogeneous
structure of natural tissues makes it difficult to study and understand countercurrent
mass transfer mechanisms arising during this operation.
Nobel (1983) claimed that cell tissues may be considered as individual cells within
a continuous cell wall with porous matrixes forming channels through which water
flows. Individual cells containing over 90% water act as springs that supply water to
the channels. These cells are separated from the cell wall by a cellular membrane.
This organ allows water flow and also may function as a solids barrier depending
on the nature of the solids. The space occupied by cells is called intracellular volume
and the free space is called extracellular volume.
When tissues are put into contact with the osmotic solution, solids enter the
extracellular volume. Penetration of solids induces a difference in the chemical poten-
tial of water on both sides of the cellular membranes, and water leaves the intracellular
volume, reaching the osmotic solution before passing this extracellular volume. The
amount of water leaving the system is proportional to the mass of solids entering the
tissue. During osmodehydration, the volume of water flowing out of the system is
much higher than the entering volume of solids. Driving forces are maintained due to
this difference in flows, and shrinkage of the tissue also arises as a consequence.
Pseudodiffusion has frequently been used to model osmotic dehydration. A het-
erogeneous material is assumed to be homogeneous to allow the usage of the second
degree diffusion equation for nonsteady conditions and thus to find an approximate
solution for the evaluation of transferred mass. An effective diffusion coefficient is
introduced to allow for the resistance due to the effects of the cell membrane and
shrinkage of tissues.

Stahl and Loncin (1979) used a one-dimensional equation to model mass transfer
in potatoes with and without peel. These authors found that the diffusion phenomena
may be predicted by means of a boundary layer model incorporating a mass transfer
coefficient for the peel. They also concluded that effective diffusion found during the
experiments is strongly dependent on time and cannot be considered as a constant.
Diffusion of sucrose in sugar beet root submerged in water was modeled by
means of the unstable diffusion equation, considering that all the sucrose can diffuse
freely in the material (Soddu and Gioia, 1979). In this work, the effect of cellular
structures on mass transfer was taken into account by the use of an apparent diffusion
coefficient. The authors found that in the fresh vegetable, a driving force smaller
than the one based on the total sucrose concentration regulates sucrose diffusion.
This means that not all the sucrose contained in the tissue takes an active role in
diffusion. Part of it is bound to cellular structures, and this amount strictly depends
on the configuration of such structures.
Conway et al. (1983) modeled water loss from 1 cm thick apple rings, considering
the slices as infinite homogeneous slabs. For this purpose, Fick’s unsteady state equa-
tion was used to predict water loss, assuming no surface resistance and no solids gain.
Beristain et al. (1990) used the same equation to model water loss during osmo-
dehydration of pineapple slices in sucrose solutions. The authors obtained diffusion
coefficients for water at different temperatures and concentrations by means of the
Park method (Crank, 1975). They concluded that for a high sucrose concentration
(70°Bx), the diffusion coefficient is not constant.
Hough et al. (1993) developed a model for osmotic dehydration of apple slices,
assuming unidirectional unsteady state pure diffusion. Mass balances for dehydration
and impregnation were applied separately. These authors took into account shrinkage,
and their model involves a numerical solution to the transport differential equations.
According to Yao and Le Maguer (1997), volumetric flow and changes in cellular
structure that take place during osmotic dehydration are the main factors that differentiate
mass transfer in osmodehydration from pure diffusion. Volume flow is strongly influ-
enced by changes in the cellular structure of the tissue. In pure diffusion, dimensionless
change of mass may be represented as a unique function of the Fourier number for mass
2
transfer (Fo = Dit/l ) (Crank, 1975), in which Di is the diffusion coefficient of specie i,
t is time of contact, and l is the half thickness of the slab. These criteria may be applied
to check for pure diffusion, considering variations in thickness of the slab.
Simpler models also exist based on mass balances, such as those reported by
Raoult-Wack et al. (1991) and Azuara et al. (1992). Parjoko et al. (1996) and
Mujaffar and Sankat (1998) successfully applied the Azuara et al. model to osmo-
dehydration of pineapple in palm tree sugar solutions and shark fillets in brine.
There have been studies involving complex microscopic models, which consider
nonreversible thermodynamic concepts in order to work out the contribution of each
component and a description of the role of the natural tissues in the process (Toupin
et al., 1989; Toupin and Le Maguer, 1989; Marcotte et al., 1991; Marcotte and Le
Maguer, 1992; Le Maguer and Yao, 1995; Yao and Le Maguer, 1996). In these models,
the cell is assumed to pass through three dehydration stages, which are a function of
the decrease in cellular volume (Toupin et al., 1989). Detailed microscopic models are
useful for explaining mass transfer at the cellular level. Water lost is related to osmotic

phenomena through natural membranes acting as semipermeable barriers (Le Maguer,
1988). However, studies carried out with agar gels by Raoult-Wack et al. (1991)
showed that it is possible to find the same dehydration effect without the existence of
selective membranes. Other works using normal and frozen (to eliminate the selec-
tiveness of membranes) apples confirmed that osmosis is not the main mechanism in
dehydration (Saurel et al., 1994). In frozen tissues, the dehydration mechanism was
diffusive and markedly related with a dense layer of solids on the surface of the product.
Analysis of these findings suggests that osmodehydration of homogeneous mate-
rials may be modeled as a diffusion process with a variable diffusion coefficient.

Golden Delicious apples were obtained from a local market. The fruits were cut into
disk-shaped pieces 46 mm in diameter and 4 mm thick and immediately immersed
into a 20 g/l solution of ascorbic acid for 5 min to control browning. In osmotic
dehydration, it is necessary to count with reliable kinetics the changes in mass that
are attributed to the process and not to variability of the product. To overcome this,
a continuous method of evaluation of the kinetics was used. With this method, it is
possible to obtain all the kinetics by measuring weight losses in the same sample
along the processing time (Azuara et al., 1998). The apple disks were dehydrated
by immersing into a 500 g/l sucrose solution set at 30, 40, or 50°C. A food:solution
ratio greater than 1:20 was maintained at all times. Samples were withdrawn peri-
odically up to a total drying time of 5 h. Immediately after sample withdrawal, the
disks were blotted with drying paper to remove excess solution. Each disk was
weighed and its thickness measured at at least three different points using a Mitutoyo
micrometer. After these measurements, the disks were returned to the osmotic solu-
tion to continue the process. At the end of the experiment, moisture content was
determined in each sample by placing it into vacuum oven for 24 h at 70°C (AOAC,
1984).
6.4 RESULTS
6.4.1 MATHEMATICAL MODELING
Work on concentration profiles along osmotic dehydration of apples carried out by
Salvatori et al. (1997) has shown the existence of a zone in the center of the samples
that keeps the initial conditions of the fresh fruit and that decreases in size with
time. This experimental evidence may suggest the possibility of developing a kinetic
equation based on the shrinking core model (Levenspiel, 1976).
Given that the thickness/diameter ratio of the apple disks was smaller than 0.1
(actual ratio = 0.086), the samples can be considered as semiinfinite plates, in which
fluxes of water and soluble solids are unidirectional (Vaccarezza et al., 1974).
According to the shrinking core theory, during the drying process the moist center
decreases and a crust is formed. The crust contains less moisture than the initial
water content between the surface and the moist core. At all times, core properties
are similar to those of the initial stages (Levenspiel, 1976). The shrinking core model

proposes that the total resistance to water transfer from the sample to the osmotic
solution can be explained by the existence of two resistances acting in series: an
internal one represented by an effective diffusion coefficient through the dried shell,
and an external one located in the film of fluid around the particle. The contribution
of each resistance towards the total one along OD is different, and the limiting one
will be that of higher value (Levenspiel, 1976).
Water loss (WFL) and solids gain (SG) during osmotic dehydration were cal-
culated using equations derived from mass balances (Azuara et al., 1992).
s1tWFL ∞
WFL = (6.1)
1 + s1t
s2 tSG ∞
SG = (6.2)
1 + s2 t
Apple samples had different initial moisture and solids content, causing the
scatter observed in WFL and SG values (Karathanos et al., 1995). To minimize the
variation, constants s1, s2, WFL∞, and SG∞ were calculated with equations developed
for a method for continuous evaluation of osmotic dehydration kinetics (Azuara
et al., 1998). The rate of water transfer per unit area from the moist core to the
surface and through the dehydrated crust is given by:
2  − dWFS  = Dw − dCw  (6.3)

πdo(do + 4 x)  dt   dx 
Azuara et al. (1992) proposed the following equation to calculate the effective
diffusion coefficient for foodstuffs having a flat slab geometry:
2
π tF 2  s110 
Dw = (6.4)
4  1 + s1t 
Figure 6.1 shows that a variable diffusion coefficient such as the one evaluated
with Equation (6.4) is a unique function of the Fourier number and thus can be
modeled as pure diffusion. The rate of water transfer per unit surface area of the
disk, from the food surface to the fluid, is given by:
2  − dWFS  = hw (C int sol − Cso) (6.5)

πdo(do + 4 lt )  dt 
By manipulating Equations (6.3), (6.4), and (6.5), it is possible to arrive at:
πd 0 (d 0 + 4 lt )(1 + s1t )2 (Cwi − Cwo)  d + 4 lt  8 lt + do   1

− = −(1 + α ) 0 ln   + (6.6)
2s1WFL ∞  4Dw  8 lc + do   hw

1
0.8
WFL/WFLα 0.6
0.4 thickness 2 mm
thickness 4 mm
thickness 6 mm
0.2
0
0 0.5 1 1.5 2
Fourier number
FIGURE 6.1 Dimensionless water loss vs. Fourier number for different thicknesses of apple
disks (T = 30°C).
Equation (6.6) shows that total resistance to mass transfer is the algebraic sum of
an internal diffusive resistance (shell resistance) plus a solids uptake resistance
through the film of solution surrounding the foodstuff. Therefore, the model can be
written in the following form:
Total resistance to = shell resistance + film resistance to

(6.7)
mass transfer to water flow waterflow
Equation (6.6) can be written in its dimensionless form:
π 2 d 0 F 2 l 0 2 (Cwi − Cwo)(1 + s1t )ML

−
 8l + d 0 
2 WFL ∞ ( WFL ∞ − SG ∞ ) ln  t 
 8l c + d 0 
4Dw(1 + s1t )ML
= − (1 + α ) (6.8)
 8l + d 0 
hws1t( WFL ∞ − SG ∞ )(d 0 + 4l t ) ln  t 
 8l c + d 0 
2
Ymod = (πs1lo /hw(WFL∞ – SG∞))Xmod. – (1 + α) (6.9)
The expression to estimate the half thickness of the moist core (lc) is:
lo
lc = (6.10)
1 + s1t

The half thickness of the apple disk at time t (lt) was adjusted with the following
equation:
2
l  l 
l t = l e + (l o − l e ) c  + cs1t  c  (6.11)
 t
l  lo 
Activation energy (Ea) can be estimated using an Arrhenius-type equation of the
following form:
Dw = Do e − Ea / RT (6.12)
Goodness of fit was estimated with the mean relative deviation modulus (P%)
between the experimental and predicted values:
m
| M i − M pi |
∑
100
P(%) = (6.13)
N i =1
Mi
6.5 DISCUSSION
Figure 6.2 shows the volume change of the apple disks (Vt/Vo) vs. moisture content
at 30°C. Three stages during the osmotic dehydration can be observed. The same
behavior was obtained when the drying process was carried out at 40 and 50°C.
These experimental results obtained using macroscopic measurements are in agreement
1
0
0.9 -0.2
Total resistance x 10-4 (min/cm)
0.8 -0.4
-0.6
Vt/Vo
Stage 3 Stage 2 Stage 1

0.7
-0.8
0.6
-1.0
0.5
-1.2
0.4 -1.4
0.5 0.6 0.7 0.8 0.9
Moisture (g water/g wet solid)
FIGURE 6.2 Changes in volume and total resistance during osmotic dehydration of apple disks.

TABLE 6.1
Parameters of the Model
Temperature Stage of hw (g water–m/g
−1
(ºC) WFL∞/Mo SG∞/Mo s1 min O.D. solids–s) (1 + α)
st −6
30 0.7156 0.1476 0.0317 1 1.244 × 10 1.5118
nd −7
2 2.900 × 10 2.4073
rd −8
3 2.200 × 10 7.8034
st −7
40 0.7505 0.1747 0.0531 1 3.543 × 10 1.9612
nd −8
2 3.013 × 10 5.8864
rd −9
3 4.472 × 10 14.5240
st −7
50 0.7602 0.2354 0.0903 1 3.221 × 10 2.5626
nd −8
2 5.047 × 10 7.5624
rd −9
3 3.922 × 10 21.6112
with the three stages theory proposed at the microscopic level by Toupin et al. (1989)
and Le Maguer and Yao (1995).
The mathematical model based on the shrinking core theory also predicted three
stages as a function of the total resistance to water flow (Figure 6.2). In the model,
α is a dimensionless parameter that is characteristic for each stage and that increases
with the amount of impregnated solids into the apple disk, which decreases as the
amount of washed solids by water flow increases. The parameters of each stage are
reported in Table 6.1. It can be observed that α increased as the osmotic dehydration
took place. A similar effect was observed when the temperature was increased. In
addition, the mass transfer coefficient for water (hw) had an opposite behavior as
compared with that of α. This may be due to the fact that impregnation on the
surface raised the film resistance to water flow.
In Figure 6.3 (dimensionless form of Equation (6.9)), the presence of the three
stages of osmodehydration at 40 and 50°C can be observed. At the end of each stage
and the beginning of the next one, an increment of (1 + α) and a decrease of hw
are observed. As seen in Figure 6.4, the diffusion coefficient of water (Dw) decreased
as the moisture content decreased. On the other hand, Dw increased with tempera-
ture. However, it should be noted that there is a zone of high moisture where Dw
increased as the moisture content decreased (Figure 6.4). In this zone, the osmotic
solution penetrates into the apple tissue to expel the trapped air from intercellular
spaces, facilitating the diffusion of water contained in the superficial cells. As a
consequence, the apple–solution interface increases and Dw also increases. At the
beginning of the second stage, an increase in the length of the water diffusion path
around the cells on the surface and the cells in the moist core occurs, which leads to
a decrease of Dw. The third stage is beyond collapse and Dw diminishes as moisture
content decreases.
Figure 6.5 depicts the variation of lt and lc with time. It can be seen that lt and
lc diminish faster along the first stage than in the second and third stages. Moreover,
in the third stage, the half thickness of the moist core (lc) is close to zero because
the equilibrium has almost been reached.

-1 0
-2 Stage 1 -2
-3 Stage 2 -4
Ymod (50°C)
Ymod (40°C)
-4
-6
-5
-8
-6
Stage 3
40°C -10
-7
50°C -12
-8
-9 -14
0 0.2 0.4 0.6 0.8 1 1.2 1.4 1.6
Xmod
FIGURE 6.3 Stages of osmotic dehydration (OD) obtained with Equation (6.9).
14
Stage 1
30°C
12
40°C
50°C
10
(m /s)
Stage 2
2
8
10
Stage 3
Dw × 10
0
0.3 0.4 0.5 0.6 0.7 0.8 0.9
Moisture (g water/g wet solid)
FIGURE 6.4 Variation in the diffusion coefficient during osmotic dehydration of apple disks.

0.2
0.15
lt or lc (cm)
lt 30°C
0.1 lt 40°C
lt 50°C
lc 30°C
0.05 lc 40°C
lc 50°C
0
0 50 100 150 200 250 300 350
Time (min)
FIGURE 6.5 Variation of lc and lt with time during osmotic dehydration of apple disks.
TABLE 6.2
Parameters for Equation (6.11)
Temperature (ºC) le (cm) c (cm) P (%)
30 0.14057 −0.04205 1.952

40 0.13079 −0.01848 1.755
50 0.13740 +0.02926 0.657
As shown in Table 6.2, lt can be calculated as a function of lc and the half-thickness

of the apple disk at equilibrium (le). A good fit was obtained with P values ≤1.952%.
Also, as the increment of temperature favors solids entrance and diminishes shrinkage,
correction factor c is less negative.
Activation energy (Ea) for water diffusion increased as the moisture content of the
apple disks decreased. For stage 1, the moisture content varied from 0.83 to 0.78 g
water/g wet solid, and Ea was in the range of 8.6 to 10.5 kcal/mol. For stage 2, the
moisture content varied from 0.78 to 0.56 g water/g wet solid, and Ea was in the range
of 10.5 to 13.0 kcal/mol. For stage 3, the moisture content varied from 0.56 to 0.50 g
water/g wet solid, and Ea was in the range of 13.0 to 17.7 kcal/mol.

6.6 CONCLUSIONS
To model osmotic dehydration as a pure diffusion process, it is necessary to account
for a nonconstant diffusion coefficient (Dw), which varies in such a way that the
dimensionless variation of mass can be represented as a unique function of the
Fourier number. It is possible to determine macroscopically the stages of the process
by measuring volume changes of a sample during the process. The shrinking core
model applied to this operation predicts the same stages as volume change measure-
ments do. This model takes into account water losses, solids entrance, weight losses,
and variation of sample thickness. The greater the impregnation, the lower the water
flux from the product to the solution. This may be due to the fact that impregnated
sugar molecules on the surface of the slices interact with water molecules, creating
an additional resistance to water flux from the sample to the medium. Shrinkage of
the discs decreases with impregnation and temperature. It was possible to predict
the change in sample thickness along the OD process, considering initial thickness
and size of the wet core.
NOMENCLATURE
c Constant for correction of thickness for solids gained and
temperature (cm)
3
Cintsol Interfacial solids concentration (g/cm )
3
Cso Volumetric concentration of sucrose in the solution (g/cm )
3
Cw Volumetric concentration of water in the apple (g/cm )
Cwi Volumetric concentration of water inside the apple disk at
3
time 0 (g/cm )
Cwo Volumetric concentration of water inside the osmotic solution
3
(g/cm )
do Initial diameter of the apple disk (cm)
2
Do Frequency factor (m /sec)
2
Dw Effective diffusion coefficient of water (m /sec)
Ea Activation energy (kcal/mol)
2
Fo = Dw t/lt Fourier number
mod exp
F = WFL∞ /WFL∞ Correction factor
hw Mass transfer coefficient of water based on the concentration
of osmotic solution (g of water–m/g of solids–sec)
lo Half-thickness of the apple disk at time 0 (cm)
lt Half-thickness of the apple disk at time t (cm)
lc Half-thickness of the moist core (cm)
le Half-thickness of the apple disk at equilibrium (cm)
Mi Experimental values
Mo Initial weight of the apple disk (g)
Mpi Predicted values
ML Weight lost by the food at time t (g)
N Number of experimental data

P Mean relative deviation modulus between the experimental
and predicted values (%)
R Universal gas constant (1.987 cal/mol K)
–1
s1 Constant related to water loss (min )
–1
s2 Constant related to solids gain (min )
SG Amount of solids gained by the apple disk at time t (g)
SG∞ Amount of solids gained by the apple disk at equilibrium (g)
t Time (min, sec)
3
Vo Volume of the apple disk at time 0 (cm )
3
Vt Volume of the apple disk at time t (cm )
WFL Amount of water lost by the apple disk at time t (g)
WFL∞ Amount of water lost by the apple disk at equilibrium (g)
mod
WFL∞ Value for WFL∞ obtained from Equation (1)
exp
WFL∞ Value for WFL∞ obtained experimentally
WFS Amount of water that remains in the apple disk at time t, but
that could leave the disk by diffusion (g)
x Position of a point in the circular plate in Cartesian
coordinates, measured in axial direction (cm)
α Unidimensional characteristic parameter for each stage
ACKNOWLEDGMENTS
To CYTED Project XI.13, IPN–México and Universidad Veracruzana–México for
support.
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Combined Effect of High
7 Hydrostatic Pressure
Pretreatment and
Osmotic Stress on Mass
Transfer during Osmotic
Dehydration
N.K. Rastogi, A. Angersbach, and D. Knorr
CONTENTS
7.1 Introduction
7.2.1 Raw Material Preparation
7.2.2 High Pressure Pretreatment
7.2.3 Osmotic Dehydration of Potato Slices
7.2.4 Determination of Water and Solute Diffusion Coefficients
during Osmotic Dehydration
7.2.5 Determination of Cell Disintegration Index (Zp)
7.4 Conclusion
Nomenclature
Acknowledgments
References
7.1 INTRODUCTION
Osmotic dehydration is a process of partial removal of water from plant tissues by
immersion in a concentrated solution of sugar or salt. Due to the difference in
osmotic pressure between the food and the solution, water is transported from the

material into the solution. The diffusion of water is accompanied by the simultaneous
counterdiffusion of solute from the osmotic solution into the tissue. Since the
membrane responsible for osmotic transport is not perfectly selective, other solutes
present in the cells can also be leached into the osmotic solution (Dixon and Jen,
1977; Lerici et al., 1985; Giangiacomo et al., 1987). The rate of diffusion of water
from any material made up of such tissues depends upon factors such as:
• The temperature and concentration of the osmotic solution

• The size and geometry of the material
• The solution to material mass ratio
• The level of agitation of the solution
A number of recent publications have described the influence of these variables on

mass transfer rates during osmotic dehydration (Roult-Wack et al., 1992; Torreggiani,
1993; Roult-Wack, 1994; Rastogi and Raghavarao, 1994, 1995, and 1997a and b;
Rastogi et al., 1997).
Given the low rate of mass transfer observed, a number of techniques have also
been tried to improve mass transfer rate. These techniques include the application of
a partial vacuum (Rastogi and Raghavarao, 1996; Fito, 1994) or ultrasound (Simal
et al., 1999) during treatment, and ultra high hydrostatic pressure (Rastogi and Niranjan,
1998) or high intensity electrical field pulses (Rastogi et al., 1999) to the material prior
to osmotic treatment.
Mass transfer during osmotic treatment occurs through semipermeable cell mem-
branes present in biological materials, which offer the dominant resistance to the
process. The state of the cell membrane can change from being partially to being
totally permeable, and this can lead to significant changes in tissue architecture.
During osmotic removal of water from foods, the osmotic dehydration front moves
from the surface of the food in contact with surrounding osmotic solution to the
center, which results in disintegration of cells due to osmotic stress. A mechanism
of osmotic water removal from biological materials has recently been proposed by
Rastogi et al. (2000a).
High hydrostatic pressure (HHP) pretreatment results in cell disintegration.
The cell disintegration index (Zp, as measured by an electrophysical measurement
based on electrical impedance analysis) after high pressure treatment increases
with time. It is well known that application of high pressures (100–800 MPa) causes
permeabilization of the cell structure (Farr, 1990; Dornenburg and Knorr, 1993;
Rastogi et al., 1994 and 2000b; Eshtiaghi et al., 1994). This phenomenon is
exploited here to enhance mass transfer rates during osmotic dehydration by pretreating
the samples at such high pressures. Osmotic dehydration of HHP-treated pineapple
has been reported to be faster than for untreated pineapple (Rastogi and Niranjan,
1998).
The aims of the present work are to investigate the combined effect of high
hydrostatic pressure and osmotic stress on the extent of membrane permeabilization
and to explain the mechanism of mass transfer during osmotic removal of water
from high pressure treated foods.

7.2.1 RAW MATERIAL PREPARATION
Fresh potatoes were purchased locally in large quantities and stored at low temper-
ature in order to have uniformity of the raw material. The potatoes were cut into
circular pieces of diameter 3.5 cm and thickness 1.0 cm. The average moisture
content of the potatoes was 86.5% on a wet basis.
7.2.2 HIGH PRESSURE PRETREATMENT

The potato slices were subjected to high hydrostatic pressures in an isostatic pressure
vessel (National Forge Europe, Belgium). The unit had a working volume of 700
ml, and its maximum recommended working pressure was 600 MPa. Maximum
pressure could be reached within 2 min, and the decompression time was about 10
sec. Potato samples were vacuum sealed in double polyethylene pouches and sub-
jected to pressures of 200, 300, and 400 MPa for 10 min at 25°C. The maximum
temperature experienced by the sample during pressurization was 35°C, and samples
were cooled to about 15°C during decompression. A mixture of distilled water and
press oil (97:3 v/v) was used as the medium for transmitting pressure.
7.2.3 OSMOTIC DEHYDRATION OF POTATO SLICES

High pressure treated and untreated potato slices were blotted with tissue to remove
external moisture and then subjected to osmotic dehydration. The samples were
weighed and suspended in the vessel containing the sugar solution (50°Brix) main-
tained at 25°C. The temperature was controlled using a constant temperature stirred
water bath. The ratio of the volume of the pieces to that of the medium was
maintained at 1:25 in order to ensure that the concentration of the osmotic solution
did not change significantly during the experiment. The samples were withdrawn at
regular intervals of 1 h, rinsed quickly, and blotted gently with tissue paper to remove
adhering water. The potato slices after osmotic treatment were cut longitudinally
into nine layers, ~1 mm length, and used to determine the moisture content and Zp
values with respect to the distance from the center of the sample. The samples were
then weighed and dried in a vacuum oven at 70°C for 18 h. The moisture and solid
content were expressed in terms of kg of water/kg of initial dry solids and kg of
solid/kg of initial dry solids, respectively. All the experiments were done in triplicate,
and average values have been reported. Relative moisture and solid content are
defined as follows:
Moisture content at any time (M)

Relative Moisture Content =
Initial moisture content (Mo )
Solid content at any time (S)

Relative Solid Content =
Initial solid content (So )

7.2.4 DETERMINATION OF WATER AND SOLUTE DIFFUSION
COEFFICIENTS DURING OSMOTIC DEHYDRATION
The solution of Fick’s second law for diffusion from an infinite slab (thickness 2l)
being dehydrated from both sides, with suitable assumptions and boundary condi-
tions, can be written for diffused moisture (Mr) and solid ratio (Sr) as (Crank, 1975):
∞
(m t − m ∞ )  2

∑ exp − n +  π 2 Fow 
8 1 1
Mr = = (7.1)
(m o − m ∞ ) π2 (2 n + 1) 2
  2  
n=0
∞
(st − s∞ )   1 2 
2
∑
8 1
Sr = = exp −
  n + π Fos  (7.2)
(so − s∞ ) π 2 n=0
(2 n + 1)2  2 
where Fow and Fos are the Fourier numbers for water and solute diffusion, respec-
tively, and are given by the following equations:
2
Fow = Dew t/l (7.3)
2
Fos = Des t/l (7.4)
where Dew and Des are the effective diffusion coefficients of water and solute, respec-
tively, and l is the half thickness of the infinite slab.
The values of Fow and Fos can be obtained using Equations (7.1) and (7.2) at different
moisture and solid ratios, and the values thus obtained are plotted against the corre-
sponding “t” values. The Dew and Des values are estimated from the slopes of these
plots (Rastogi and Raghavarao, 1997a and b).
7.2.5 DETERMINATION OF CELL DISINTEGRATION INDEX (ZP)

The conductivity–frequency spectra of high pressure treated and control samples of
potato were obtained (Angersbach et al., 1997, 1999; Knorr and Angersbach, 1998).
The cell disintegration index (Zp) was defined as:
Zp = 1 − b
(K′h − K′l ) ; 0 ≤ Zp ≤ 1 (7.5)
(K h − K l )
where b = Kh/K′h, Kl and K′l are the electrical conductivity of control and treated
samples measured in a low frequency field (1–5 kHz), and Kh and K′h are the electrical
conductivity of control and treated samples measured in a high frequency field (3–50
MHz). The cell disintegration index characterizes the proportion of cells with highly
permeable cell walls. Zp takes values between 0 and 1 corresponding to 100% intact
cells and total cell disintegration, respectively. It is an integral parameter that indicates
the relative reduction in the portion of intact cells in the cell system. A homogeneous
distribution of intact and permeabilized cells and noncellular compartments in the
measured system is a prerequisite for correct measurement. During osmotic treatment,
a reduction in cells can occur due to disintegration or shrinkage of cell membranes.

The conductivity of control and treated samples was determined with impedance
measurement equipment (Electronic Manufacture Company, Mahlsdorf, Germany)
between parallel disc electrodes (9.7 mm diameter) spaced 8 mm apart. The phase
voltages were of equal amplitude (between 1 and 5 V, peak to peak) and the frequency
changed between 3 and 50 MHz. A correction for the capacitance and inductance
(of about 1.2 µH) arising from the measuring cell was incorporated using Schwan’s
method (Schwan, 1963, 1968).
The cell disintegration index (Zp) values were measured immediately after the
high pressure treatment. The variation of Zp values with time was also measured for
the samples treated at 200, 300, and 400 MPa.

Typical plots of variation of moisture and solid content of control and high pressure
treated samples with immersion time during the course of osmotic dehydration are
shown in Figures 7.1a and 7.1b. The moisture and solid diffusion both increased due
to high pressure pretreatment. They also increased with an increase in pretreatment
pressure. In order to compare the mass transfer characteristics, the effective diffusion
coefficients of water diffusing out of the sample and solute infusing into the sample
were calculated. The rate of change of moisture as well as solid content was obtained
from Figures 7.1a and 7.1b for all the data and plotted against the average moisture
content and average solid content (Figures 7.2a and 7.2b), respectively, in order to
infer equilibrium moisture and solid content.
In order to calculate the Dew and Des values considering the unsteady state osmotic
dehydration, the typical values of Fow and Fos (at different moisture ratios correspond-
ing to t) obtained from Equations (7.1) and (7.2) are plotted against t (Figures 7.3a and
7.3b). The values of the effective diffusion coefficients are inferred from the slopes of
such plots. The relevant values are reported in Table 7.1. It is evident that the diffusion
coefficient for water increased due to high pressure pretreatment, giving shorter dehy-
dration times. There was also a simultaneous increase in solute diffusion coefficients.
This is attributed to the increase in cell permeability due to high pressure pretreatment.
In order to represent the exponential increase of water and solute diffusion
coefficients (Dew and Des) with the applied pressure, the values of –ln(Dew) and
–ln(Des) were plotted against 1/P (as shown in Figure 7.4), and correlations similar
TABLE 7.1
Effective Diffusion Coefficient for Water (Dew) and Solute
(Des) at Different Pressures
9 2 9 2
Treatment Pressure (MPa) Dew × 10 (m /sec) Des × 10 (m /sec)
Control 0.37 0.31

200 0.45 0.41
300 0.64 0.57
400 0.84 0.67

5.0
Control
200 MPa
Moisture Content (kg/kg)

4.5 300 MPa
400 MPa
4.0
3.5
3.0
0.0 1.0 2.0 3.0 4.0 5.0 6.0
Immersion Time (h)
(a)
2.4
Control
2.2 200 MPa
300 MPa
Solid Content (kg/kg)
2.0 400 MPa
1.8
1.6
1.4
1.2
1.0
0.0 1.0 2.0 3.0 4.0 5.0 6.0
Immersion Time (h)
(b)
FIGURE 7.1 Variation of (a) moisture and (b) solid content of control and high pressure
treated potato samples during the course of osmotic dehydration.
to the Arrhenius relation were obtained as:
  B 
Dew = A w exp − w  2
(R = 0.98) (7.6)
  P 
  B 
Des = As exp − s  2
(R = 0.99) (7.7)
  P 

0.4
Control
200 MPa
300 MPa
0.3
400 MPa
–dm/dt
0.2
0.1
0.0
3.0 3.2 3.4 3.6 3.8 4.0 4.2 4.4 4.6
Av. Moisture Content (kg/kg)

(a)
0.4
Control
200 MPa
0.3 300 MPa
400 MPa
ds/dt
0.2
0.1
0.0
1.0 1.5 2.0 2.5 3.0
Av. Solid Content (kg/kg)
(b)
FIGURE 7.2 Variation of (a) moisture removal (−dm/dt) and (b) solid uptake (−ds/dt) of
control and high pressure treated potato samples during the course of osmotic dehydration with
average moisture content and solid content, respectively.
–9 2 –9 2
The values of Aw, As, Bw, and Bs were 1.50 × 10 m /sec, 1.09 × 10 m /sec,
244.19 MPa, and 196.63 MPa, respectively.
The cell disintegration index (Zp) increases with an increase in high hydrostatic
pressure applied to the potato sample (Figure 7.5a). The Zp values were recorded
immediately after the high pressure treatment. The Zp values of the pressure-treated
potato increased with time at atmospheric pressure, and the equilibrium Zp values
also increased with pressure (Figure 7.5b). The Zp values of the center layer after

0.7
Control
0.6 200 MPa
0.5 300 MPa
400 MPa
0.4
Fow
0.3
0.2
0.1
0.0
0.0 1.0 2.0 3.0 4.0 5.0 6.0
Immersion Time (h)
(a)
0.7
Control
0.6 200 MPa
0.5 300 MPa
400 MPa
0.4
Fos
0.3
0.2
0.1
0.0
0.0 1.0 2.0 3.0 4.0 5.0 6.0
Immersion Time (h)
(b)
FIGURE 7.3 Variation of Fourier number of (a) water, Fow and (b) solute, Fos diffusion with time.
high pressure pretreatment were 0.039, 0.065, and 0.091 at 200, 300, and 400 MPa
and could reach 0.35, 0.45, and 0.53 within 6 h, respectively (Figure 7.6). The Zp
values of the center layer after 5 h in the case of samples treated at 400 MPa reached
up to 0.82, which is due to the combined effect of osmotic stress and high pressure
induced permeabilization (Figure 7.6c).
The increase in Zp values (or tissue softening or loss of texture) following high
pressure treatment was due to destruction of cell membranes and partial liberation
of cell substances. Upon high pressure treatment, polymethylesterase (PME)
enzyme, which is bound to the cell wall, is liberated and not completely inactivated
and brought in close contact with its substrate, the methylated pectin. This causes
deesterification not only during high pressure treatment, but also during the standing

21.9
Dew
Des
–ln(Dew) or –ln(Des)
21.6
21.3
21.0
20.7
0.002 0.003 0.004 0.005 0.006
1/P
FIGURE 7.4 Plot of −ln(De) with 1/P, representing the exponential increase of diffusion coeffi-
cients with pressure applied.
0.10
0.08
0.06
Zp
0.04
0.02
0.00
0 100 200 300 400
Pressure (MPa)
(a)
0.6
200 MPa
0.5 300 MPa
400 MPa
0.4
Zp
0.3
0.2
0.1
0.0
0.0 1.0 2.0 3.0 4.0 5.0 6.0
Time (h)
(b)
FIGURE 7.5 (a) Variation of cell disintegration index (Zp) with applied pressure. The Zp
values were measured immediately after high pressure treatment; (b) Variation of cell disin-
tegration index (Zp) with time at atmospheric pressure after high pressure treatment.

1.0
1h
2h
0.8 3h
4h
5h
0.6
Zp
0.4
0.2
0.0
0.0 0.1 0.2 0.3 0.4 0.5 0.6 0.7 0.8 0.9 1.0
Relative distance (l/lo)
(a)
1.0
1h
2h
3h
0.8 4h
5h
0.6
Zp
0.4
0.2
0.0
0.0 0.1 0.2 0.3 0.4 0.5 0.6 0.7 0.8 0.9 1.0
Relative Distance (l/lo)
(b)
FIGURE 7.6 Distribution of cell disintegration index with respect to distance from the center
of the potato samples (thickness 10 mm) during osmotic dehydration of control sample (a) and
samples pressure pretreated at 200 MPa (b) and 400 MPa (c) for 10 min. (Reprinted from
Rastogi, N.K., Angersbach, A., and Knorr, D., J. Food Eng., 45, 25–31, 2000 with permission
from Elsevier Science.)
time after the release of high pressure. The pressure treatment also causes partial
inactivation of PME. This reaction continues with time even after high pressure
treatment and results in time dependent softening of potato tissue. The alteration in
pectin results in loss of water and soluble solids (or extractable pectin) after high
pressure treatment (Stute et al., 1996). It has been reported in the literature that

1.0
0.8
0.6
Zp
0.4
1h
0.2 2h
3h
4h
5h
0.0
0.0 0.1 0.2 0.3 0.4 0.5 0.6 0.7 0.8 0.9 1.0
(c)
FIGURE 7.6 (Continued).
1.0
Relative Moisture Content (M/Mo)
0.9
0.8
1h
2h
0.7
3h
4h
5h
0.6
0.0 0.1 0.2 0.3 0.4 0.5 0.6 0.7 0.8 0.9 1.0
(a)
FIGURE 7.7 Distribution of relative moisture content with respect to distance from the center
following high pressure treatment, some fruits and vegetables soften over time at
atmospheric pressure (Basak and Ramaswamy, 1998; Rastogi et al., 2000b).
The profiles of the cell disintegration index (Zp) were different for samples treated
at 200, 300, and 400 MPa, due to differences in the degree of cell disintegration with

1.0

0.9
0.8
1h
0.7 2h
3h
4h
5h
0.6
0.0 0.1 0.2 0.3 0.4 0.5 0.6 0.7 0.8 0.9 1.0
Relative Distance (I/Io)
(b)
1.0
0.9
0.8
1h
0.7 2h
3h
4h
5h
0.6
0.0 0.1 0.2 0.3 0.4 0.5 0.6 0.7 0.8 0.9 1.0
(c)
the applied pressures (Figures 7.5a and 7.5b). The Zp values of the untreated sample
did not change with time and remained at zero. A typical variation in cell disinte-
gration index (Zp) of pressure-treated (200 and 400 MPa) and untreated potato
samples with distance from the center of the material for different dehydration times
is shown in Figure 7.6. It may be inferred from the figures that as the dehydration
front moved within the sample, it resulted in sudden increases in Zp values. The Zp
values of the center layer of potato after 5 h of osmotic dehydration for the control
and samples treated at 200, 300, and 400 MPa were 0.18, 0.28, and 0.82, respectively,
which showed that the variation in Zp values was due to the combined effect of osmotic
stress as the dehydration proceeded and high pressure induced permeabilization.

2.4
1h
2.2 2h
Relative Soild Content (S/So)

3h
4h
2.0 5h
1.8
1.6
1.4
1.2
1.0
0.0 0.1 0.2 0.3 0.4 0.5 0.6 0.7 0.8 0.9 1.0
(a)
2.4
1h
2.2 2h
3h
4h
2.0 5h
1.8
1.6
1.4
1.2
1.0
0.0 0.1 0.2 0.3 0.4 0.5 0.6 0.7 0.8 0.9 1.0
(b)
FIGURE 7.8 Distribution of relative solid content with respect to distance from the center
There was a progressive increase in Zp values as the osmotic dehydration proceeded.

The Zp values of all the layers, in the case of samples pressure treated at 400 MPa,
were higher than the control and the sample treated at 200 MPa at the corresponding
distances and immersion times (Figure 7.6).
The variations in relative moisture (M / Mo) and solid (S/So) content with
respect to the distance from the center of the material for the pressure-treated and
control potato samples for different treatment times are shown in Figures 7.7 and
7.8. It may be noted that the relative moisture was reduced and solid content

2.4
1h
2.2 2h

3h
4h
2.0 5h
1.8
1.6
1.4
1.2
1.0
0.0 0.1 0.2 0.3 0.4 0.5 0.6 0.7 0.8 0.9 1.0
(c)
increased in the case of samples treated at 200 and 400 MPa as compared to the
control.
7.4 CONCLUSION
High hydrostatic pressure pretreatment results in cell permeabilization. The cell per-
meabilization index after high pressure treatment increases with time. Osmotic dehy-
dration of high hydrostatic pressure treated foods is faster than that of untreated foods.
The state of the cell membrane during osmotic dehydration of high pressure pretreated
samples can change from being partially to totally permeable, which leads to significant
changes in the tissue architecture, resulting in increased mass transfer rates during
osmotic dehydration as compared to untreated samples, due to the combined effect of
cell permeabilization due to osmotic stress and high pressure induced permeabilization.
NOMENCLATURE
As, Bs Coefficients for solute diffusion in Equation (7.7)
Aw, Bw Coefficients for water diffusion in Equation (7.6)
2
Des Effective diffusion coefficient of solid (m /sec)
2
Dew Effective diffusion coefficient of water (m /sec)
Fos Fourier number of solid diffusion
Fow Fourier number of water diffusion
Kl, K′l Electrical conductivity of control and treated samples, respectively, measured
in a low frequency field (1–5 kHz) (mS/cm)
Kh, K′h Electrical conductivity of control and treated samples, respectively, measured
in a high frequency field (3–50 MHz) (mS/cm)

l Half thickness of infinite slab (m)
m Moisture content at t = t (kg/kg)
m∞ Moisture content at t = ∞ (kg/kg)
mo Initial moisture content at t = 0 (kg/kg)
P Pressure (MPa)
s Solid content at t = t (kg/kg)
s∞ Solid content at t = ∞ (kg/kg)
so Initial solid content at t = 0 (kg/kg)
t Immersion time (h)
Zp Cell disintegration index
ACKNOWLEDGMENTS
Author NKR gratefully acknowledges the support of the German Academic
Exchange Service (DAAD) for providing a research fellowship at Berlin University
of Technology to carry out this work. NKR is also grateful to Dr. V. Prakash, Director,
CFTRI and H. Krishna Murty, Head, Dept. of Food Engineering, for constant
encouragement.
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Hydrodynamic
8 Mechanisms in Plant
Tissues during Mass
Transport Operations
P. Fito, A. Chiralt, J. Martínez-Monzó, and J. Barat
CONTENTS
8.1 Introduction
8.2 HDM Promoted by External Pressure Changes
8.3 HDM Promoted by Cell Shrinkage in Osmotic Processes
8.4 HDM Promoted by Cell Matrix Relaxation in Long-Term
Osmotic Processes
8.5 Conclusions
Nomenclature
Acknowledgments
References
8.1 INTRODUCTION
In the processing of fruit and vegetables, solid–fluid systems (SFS) frequently occur
in different operations, such as osmotic dehydration, rehydration, candy processing,
boiling, and cooking, among others. The heat and mass transfer processes in such
systems have usually been modeled considering the food solid as a continuous phase.
Nevertheless, the cellular structure (intercellular spaces and cell compartmentation)
plays an important role in the definition of mechanisms involved in the process and
therefore in process kinetics. Recently, several studies have been carried out to
determine the influence of porosity on the response of fruit tissue to solid–liquid
operations (Fito, 1994; Fito and Pastor, 1994; Fito et al., 1996; Fito and Chiralt,
1997). In this way, a fast mass transfer mechanism (hydrodynamic mechanism,
HDM) has been described as occurring in process operations in which a porous solid
is immersed in a liquid phase; changes in temperature or pressure also take place.
The occluded gas inside the product pores is compressed or expanded according
to the pressure or temperature changes, while the external liquid is pumped into the

pores in line with the gas compression. An effective exchange of the product internal
gas with the external liquid is promoted in vacuum impregnation (VI) operations,
where a vacuum pressure (p1~50–100 mbar) is imposed on the system for a short
time (t1); afterwards, the atmospheric pressure (p2) is reestablished while the product
remains immersed in the liquid for a time t2 (Fito et al., 1996; Salvatori et al., 1998a).
The volume fraction of the initial sample (X) impregnated by the external liquid
when mechanical equilibrium is achieved in the sample has been modeled as a function
of the compression ratio r (given by Equation (8.1), where pc is capillary pressure),
sample effective porosity (εe), and sample volume deformations at the end of the
process (γ) and the vacuum step (γ1) (Equation (8.2)) (Fito et al., 1996). If γ = γ1 = 0,
Equation (8.1) gives the relationship for VI of stiff products.
p2 + pc
r= (8.1)
p1
ε e ( r − 1) = ( X − γ )r + γ 1 (8.2)
When there are no pressure changes (p1 = p2) in the system, capillary impreg-
nation will occur due to the capillary pressure; the lower the pressure in the system,
the greater the liquid penetration, according to Equations (8.1) and (8.2).
The possibility of introducing an external solution containing specific/selected
solutes inside the product pores has made VI a tool in fruit processing. The addition of
preservatives (antimicrobials, antibrowning agents, pH reducers, and others) or nutrients
(minerals, vitamins, etc.), fast water activity depression, and modifying physical prop-
erties, among others, may be some of the possible applications of VI (Chiralt et al., 1999).
Impregnation of the fruit pores due to hydrodynamic mechanisms has been seen
to occur without external pressure changes when the cellular tissue remains
immersed in a liquid phase for a long time (e.g., syrup canned and candied fruits).
This has been explained in terms of the capillary forces, pressure and temperature
fluctuations in the system, and relaxation phenomena of the shrunken cellular matrix
when hypertonic solutions are used in the treatments (Barat et al., 1998). Fito et al.
(2000) reported a contribution of HDM to the total mass transfer throughout the
osmotic process due to the pressure gradients in the tissue associated with internal
volume generation in line with cell water losses.
The aim of this work is to analyze the role of hydrodynamic mechanisms in
different kinds or times of processing in plant tissue–fluid systems and their impli-
cations in process kinetics, as well as the influence of the action of these mechanisms
on plant tissues in terms of product quality or process advantages.
8.2 HDM PROMOTED BY EXTERNAL PRESSURE CHANGES

The most effective action of HDM in the product pores is promoted by vacuum
impregnation operations. The compression ratio can reach very high values by using
common industrial pumps and, additionally, the product remains are impregnated at
the end of the process when normal pressure is recovered. Impregnation promoted by

applying high pressure in the system is not effective because the liquid introduced into
the pores in the compression step flows out when the system returns to atmospheric
conditions. For stiff matrices, the kinetics of impregnation are very fast, depending on
the pore size (length and diameter) and tortuosity and the liquid viscosity. Equation
(8.3) gives the relationship between the liquid penetration level and time, in terms of
the volume fraction of the pore impregnated (xv) at time t (t2) in a reduced way (xr)
(Equation (8.4)). The value of xve corresponds to the impregnated volume at mechanical
equilibrium, which can be obtained by Equation (8.2) when γ = γ1 = 0, since xv = X/εe.
Parameters B and k are described by Equations (8.5) and (8.6) (Chiralt et al., 1999).
t 1   1 − xr  
= − (x 2r − x 2r 0 ) − k ( x r − x r 0 ) + ln  (8.3)
B 2   1 − x r 0  
xv
xr = (8.4)
x ve
1
k = 1+ (8.5)
x ve
2
 eF  p2
B = 8µ t  (8.6)
 rp  ( p2 − p1 )
2
Figure 8.1 shows the predicted development of xr as a function of time (t2) after
the vacuum step for different values of the external liquid viscosity, and by consid-
ering a stiff matrix with pore size of 100 µm diameter, 1 cm length, and a tortuosity
factor Ft = 2. It can be observed that even for high viscosity liquids such as
hydrocolloids or concentrated sugars, the penetration times needed to reach the xve
are on the order of a few minutes (Figure 8.1a). This process length is near the time
required to achieve stationary pressure in the tank after the valve is opened to restore
the atmospheric pressure.
In real systems with a viscoelastic character, the kinetics of pore impregnation
are coupled with deformation–relaxation of the sample volume. A fast mechanical
pseudoequilibrium can be achieved in the first step, with a notable reduction of
product porosity coupled with partial liquid penetration. Afterwards, the true equi-
librium is reached through relaxation of the deformed porous matrix, which leads
to progressive liquid entry in line with sample volume recovery while the product
remains immersed. This two-step behavior will be especially promoted when long
penetration times, associated with high liquid viscosity or/and small pore diameter,
occur. For cylindrical (2 cm diameter and height) apple samples, Figure 8.1b shows
the sample volume fraction impregnated (X) and deformed (γ) after VI (10 min at
50 mbar) with a sugar isotonic solution and with 3% pectin sugar isotonic solution,
as a function of the length of the VI second step at atmospheric pressure. It can be
observed that at very short times, the sample volume reduces by about 5% and
slowly recovers in line with time increase. The impregnation levels increase more
quickly in the less viscous solution.

1
xr 0.8
33
(m /m )
0.6
0.4
0.01 Pa·s
0.2 0.1 Pa·s
1.0 Pa·s
0
0 20 40 60
t (s)
(a)
0.2
0.1
X /γ
-0.1
0 1000 2000 3000 4000
t(s)
(b)
FIGURE 8.1 (a) Impregnation kinetics of an ideal pore (100 µm diameter, 1 cm length, 2
tortuosity factor) for different viscosities (Pa s) of the external solution. (b) Development of
sample volume fraction impregnated (X, closed symbols) and deformed (γ, open symbols)
with time (t2), during VI of cylindrical apple (var. Granny Smith) samples with isotonic sugar
solution (squares) and 3% pectin isotonic sugar solution (circles).
It is remarkable that when solutions with high viscosity are used for VI, it is
advantageous to carry out the vacuum step with samples suspended above the
solution, rather than immersed in it. If not, difficulties of sample gas outflow cause
great sample deformation and very limited impregnation. Throughout the release of
the gas, it becomes entrapped in the external solution, thus forming stable foam
around the sample with much higher viscosity than the original fluid. During the
second VI step, part of the entrapped gas flows into the pores again, thus reducing
the impregnation effectiveness.
Table 8.1 shows the levels of deformation and impregnation of cylindrical apple
samples at the end of the vacuum step and of the process as a function of the

TABLE 8.1
Impregnation (X) and Deformation (γ) Levels of Apple (var. Granny
Smith) Cylindrical Samples (2 cm Diameter and Height) Reached in a
VI Operation (p1 = 50 mbar, t1 = 10 min, t2 = 15 min) with Isotonic
Sugar Solutions Containing Different Concentrations of Pectin
Pectin
concentration Viscosity
a a b b c
% µ (Pas) X1 γ1 X γ εe
0 0.0068 −0.035 0.013 0.14 −0.05 0.20

1 0.0202 −0.043 0.03 0.12 −0.02 0.15
2 0.0917 −0.011 0.10 0.07 −0.05 0.14
3 0.179 0.028 0.14 0.09 −0.06 0.13
d
3 0.179 −0.040 0.01 0,13 .0,05 0.19
a
At the end of the vacuum step.
b
At the end of the process.
c
Determined on the basis of theoretical model (Equation (8.2)) assuming mechanical equilibrium.
d
Samples were not immersed in the solution during the vacuum step.
impregnating solution viscosity. Effective sample porosity, calculated by Equation

(8.2), assuming mechanical equilibrium, also appears in Table 8.1. The decreasing
values of εe, in line with the solution viscosity increase, suggest that mechanical
equilibrium was not reached for t2 = 15 min. On the other hand, a greater effectiveness
of sample impregnation when the sample is not immersed in the viscous solution
during the vacuum step can be observed.
VI may promote fast compositional changes in fruit, which is useful in many cases
to ensure processed fruit stability (decrease of pH or water activity, introduction of
antibrowning agents or microbial preservatives) or quality (the improvement of the
sweet–sour taste relationship, fortification with specific nutrients). Prediction of com-
positional changes in short VI treatments can be easily obtained by applying Equations
(8.7) and (8.8), if the value of the impregnated volume fraction (X) and the density
0 IS
of the initial product (ρ ) and the impregnating solution (ρ ) are known (Chiralt et al.,
1999). From these equations, the required solution mass fraction (yi) of a determined
component (i.e., water, sugar, acid, additive, etc.) to achieve the desired level in the
VI
final product (mass fraction: xi ) can be calculated. Composition changes promoted
by concentration gradients between external solution and product were not taken into
account in Equation (8.7) due to the short length of VI processes. In Equation (8.7),
0
xi corresponds to the initial mass fraction of component i in the product.
x 0i + x HDM y i
x iVI = (8.7)
1 + x HDM
ρIS
x HDM = X (8.8)
ρ0

8.3 HDM PROMOTED BY CELL SHRINKAGE
IN OSMOTIC PROCESSES
Throughout osmotic processes in fruit and vegetables, a great cell volume reduction
occurs due to intracellular water loss. This implies the generation of internal voids
that provoke internal pressure depression, which promotes hydrodynamic flow of
the external solution from the sample interface to the internal voids. These pressure
gradients also contribute to the structural development pathway of cells, depending
on the kind of fluid (gas or liquid) in the tissue pores (Fito et al., 2000).
Figure 8.2 shows a scheme of how HDMs were promoted into the tissue, as well
as the sample cellular structure development. When the intercellular spaces are full of
liquid, osmosis promotes plasmolysis but no significant folding of the cell wall,
whereas the space between plasmalemma and cell wall is flooded by the extracellular
liquid (Martínez-Monzó et al., 1998a). In contrast, when intercellular spaces are occu-
pied by gas, osmosis provokes cell wall shrinkage without plasmalemma separations
(Salvatori et al., 1998b). This difference in behavior has been explained in terms of
the different pressure drop of gas or liquid phases during their flux towards the
intercellular space generated volumes (isgv in Figure 8.2). The balance of forces acting
on both sides of the plasmalemma–cell wall layer during cell water volume loss leads
to the separation of the double layer and to the flux of the external liquid through the
cell wall, or to cell wall deformation together with the plasmalemma (Fito et al., 2000).
In osmotic treatments of cellular tissues, HDM may act to a great extent at the
beginning of the process if a vacuum pulse is applied in the tank for a short period
(Pulsed Vacuum Osmotic Dehydration, PVOD), since the sample impregnation with
the osmotic solution is promoted. In treatments at atmospheric conditions (OD) or
at vacuum conditions (Vacuum Osmotic Dehydration, VOD) capillary pressure also
provokes HDM near the sample interface to a lesser extent. The different extent of
the external liquid flow into the tissue and the subsequent differences in the cellular
structure development will affect the tissue response to mass transport.
Figure 8.3 shows a comparison of the effective diffusivity values (De) in the fruit
liquid phase obtained in OD and PVOD treatments in apple slices (1 cm thick)
is containing gas phase

B
is isgv
A A
ic
JHDM is
B JW JHDM
M
Jw
is containing liquid phase
FIGURE 8.2 Scheme of cellular structure development during osmotic treatments depending
on the fluid present in the intercellular spaces (is) and water (Jw) and hydrodynamic (JHDM)
fluxes (isgv, intercellular space generated volume; ic, intracellular content; A and B, cell
bonding points).

12
De × 1010(m2/s) (PVOD)
10
25° Brix
8
35° Brix
6 45° Brix
4 55° Brix
2 65° Brix
0
0 2 4 6 8 10 12
De × 1010(m2/s)(OD)
2
FIGURE 8.3 Comparison of values of the effective diffusion coefficient (De, in m /sec) in
apple (Granny Smith) liquid phase (water plus solutes) obtained in OD and PVOD processes
carried out with different sucrose solutions (25 to 65°Brix) at 30, 40, and 50°C.
t (s)
0 4000 8000 12000
Ln Y 0
-0.1
-0.2
-0.3
-0.4
-0.5
-0.6
-0.7
-0.8
FIGURE 8.4 Kinetics of fruit liquid phase composition changes in cylindrical apple samples
(2 cm diameter and height) osmosed in 62°Brix rectified grape must, for nonimpregnated
♦), samples impregnated with an isotonic solution (••), and samples impregnated
samples (♦
with a 3% pectin isotonic solution ( ).
osmosed with different sucrose syrups (25–65°Brix) at 30, 40, and 50°C. Compo-
sitional change promoted by the vacuum pulse was corrected to make the De values
more comparable (Barat et al., 1997). Higher values of De in the PVOD process can
be observed; the higher the De value in OD, the greater the difference.
On the other hand, Figure 8.4 shows the influence of VI with isotonic solutions
of different viscosity on the kinetics of fruit liquid phase composition changes for
apple cylindrical samples. The reduced concentration of each component (Yi) was
defined in terms of the solute or water mass fractions (zi, i = water or solutes) in
the fruit liquid phase (water plus solutes) by Equation (8.9). The value of z at equi-
e
librium (zi ) was taken to be equal to that of the osmotic solution. The acceleration
of kinetics in line with the filling of the pores, without any changes in the initial
value of the process driving force, can be observed. Nevertheless, if the impregnating

solution viscosity is high, slower kinetics are observed. These results agree with a
great promotion of diffusion through the noncompartmented intercellular spaces
when filled with liquid phase, which is greatly affected by the liquid viscosity
(Martínez-Monzó et al., 1998b).
(z it − z ei )
Yi = (8.9)
(z 0i − z ie )
8.4 HDM PROMOTED BY CELL MATRIX RELAXATION

IN LONG-TERM OSMOTIC PROCESSES
In long-term osmotic processes such as those carried out in fruit candying, HDM
plays an important role in tissue development after compositional equilibrium
between the sample and the external solution has been reached. Sample mass and
volume decrease in line with osmotic dehydration until a minimum value is reached
at compositional equilibrium time tc. From this point, sample mass and volume begin
a slowly increasing pathway until almost all of the initial values are recovered. This
was observed initially in apple samples (Barat et al., 1998; Fito et al., 1998) and
was confirmed for other fruits (Barat, 1998).
Mass and sample volume recovery has been explained in terms of pressure
gradients generated in the shrunken cellular structure due to relaxation of cell walls,
where a great amount of free energy was stored during cell dehydration–shrinkage.
True equilibrium in the system implies free energy reduction by release of mechan-
ical stress. If the product remains immersed in the external solution, volume recovery
is coupled with liquid suction and therefore with mass gain. In this sense, the pressure
drop of liquid inflow will affect the sample volume relaxation rate, causing the
system (fruit plus external liquid) to behave as a viscoelastic solid. The overall
relaxation rate of the system will be greatly dependent on liquid viscosity and the
elastic character of the cellular matrix. The relative relaxation level will be deter-
mined by the total volume lost during osmotic treatment and the irreversible struc-
tural damage in the tissue. In this sense, cellular turgor will not be recovered, and
so the final sample volume will be reduced with respect to the initial value by the
intercellular volume associated with the turgid cell packaging.
HDM flow in this matrix relaxation process has been modeled on the basis of
a viscoelastic model (Equation (8.10)) (Peleg, 1980). In Equation (8.10), F0 and Ft are
respectively the initial force on the sample associated with a given deformation and
the force at a determined relaxation time. The constants A and B represent, respec-
tively, the total relative relaxation level and the relaxation rate. To fit Equation (8.10)
to the experimental mass recovery data, the following hypotheses are considered:
the mechanical stress on the matrix is released as flow pressure drops in the external
liquid; likewise, a laminar flow was assumed. From these hypotheses, force will be
given by Equation (8.11), thus obtaining Equation (8.12) to describe mass recovery.
0
The M values are the relative mass gain of the sample at each time. The function
0
(dM (t)/dt) was obtained by fitting a bi-exponential function to the experimental

0
curve (M vs. time) and calculating the derivative equation and its values at each
time.
F0 t 1 t
= + (8.10)
F0 − Ft AB A
8πµFt e  ∂M 0 (t ) 
F=   (8.11)
ρIS  ∂t 
(∂M 0 ( t ) / ∂t )0 t t 1 t
= = + (8.12)
(∂M 0 ( t ) / ∂t )0 − (∂M 0 ( t ) / ∂t )t YF AB A
Figure 8.5 shows a linear relationship between experimental points plotted as

defined by Equation (8.12) for OD and PVOD treatments of 1 cm thick apple slices,
with 55°Brix sucrose solution, at 30, 40, and 50°C. The scarce influence of temper-
ature and kind of treatment on the kinetics of HDM mass flow during sample stress
relaxation can be observed. Table 8.2 shows the mean values obtained for A and B
parameters for OD and PVOD treatments of apple slices in the 30–50°C range. The
values of A are near one in all cases, indicating that samples recover about 100%
of their initial mass throughout the examined time, with the relaxation rate being
affected by the syrup concentration. The relaxation is faster as the sucrose concen-
tration is lower (below 25°Brix), in agreement with the lower viscosity values of
the solutions.
4000
t/YF (h)
3000
55 OD 30°C
2000 55 OD 40°C
55 OD 50°C
55 PVOD 30°C
1000
55 PVOD 40°C
55 PVOD 50°C
0
0 1000 2000 3000 4000
t – tc (h)
FIGURE 8.5 Kinetics of HDM mass flow in long-term osmotic processes after compositional
equilibrium time (tc). Points correspond to osmosed apple slices (1 cm thick) in 55°Brix
sucrose solution for OD and PVOD treatments at different temperatures.

TABLE 8.2
A and B Parameters of Equation (10) for OD and PVOD
Treatments of Osmosed Apple Slices in Sucrose Syrups
(OS) of Different Concentrations
OD PVOD
°Brix (OS) A B A B
65 1.02 0.002 0.98 0.009

55 1.05 0.004 1.07 0.005
45 1.02 0.012 1.05 0.037
35 1.01 0.024 1.00 0.094
25 0.98 0.162 0.96 0.082
20 1.01 0.024 1.01 0.080
8.5 CONCLUSIONS
HDM plays an important role in solid–liquid operations with cellular products such
as fruit and vegetables. Through understanding and modeling the action of these
mechanisms, better process control will be possible. Promotion of these mechanisms
through the control of process variables may be a tool in designing new product
composition.
NOMENCLATURE
p Pressure (mbar), (subscript c: capillary; 1: at the vacuum step; 2: atmospheric)
µ Solution viscosity (Parsec)
3 3
xv Pore volume fraction impregnated by the solution (m /m )
xve Pore volume fraction impregnated by the solution at mechanical equilibrium
3 3
(m /m )
xr Reduced pore volume fraction impregnated by the solution (xv/xve)
εe Sample effective porosity
r Compression ratio
X1 Sample volume fraction impregnated by the solution at the end of the first
VI step
X Sample volume fraction impregnated by the solution at the end of the VI
process
1
γ Relative volume deformation of the sample due to pressure change at the
end of the first VI step
γ Relative volume deformation of the sample due to pressure change at the
end of the VI process
e Sample characteristic dimension (m)
rp Pore radius (m)
Ft Tortuosity factor of the sample pores

k Dimensionless parameter of the model of VI kinetics
B Time dimension parameter of the model of VI kinetics
0 3
ρ Density of the initial product (kg/m )
IS 3
ρ Density of the impregnating solution (kg/m )
xHDM Mass ratio of the impregnated solution in the initial product (kg/kg)
yiiv Mass fraction of the component i in the impregnating solution (kg/kg)
xi0 Mass fraction of component i in the impregnated product (kg/kg)
xi Mass fraction of component i in the initial product (kg/kg)
Yi Reduced driven force referred to component i
t
zi Mass fraction of component i in the food liquid phase at time t of the process
(kg/kg)
2
De Pseudodiffusion coefficient (m /sec)
0
M Mass relative change of the sample at each time (kg/kg)
t Process time (sec)
F Force (N)
ACKNOWLEDGMENTS
The authors thank the Comisión Interministerial de Ciencia y Tecnología (Spain),
CYTED program, and European Union (DGXII) for their financial support.
REFERENCES
Barat, J.M., Osmotic Dehydration Model Development as Unit Operation, Ph.D. Thesis,
Universidad Politécnica, Valencia, Spain, 1998.
Barat, J.M., Alvarruiz, A., Chiralt, A., and Fito, P., A mass transfer modelling in osmotic
dehydration, in Engineering and Food at ICEF 7, Jowitt, R., Ed., Sheffield Academic
Press, Sheffield, 1997, pp. G 81–84.
Barat, J.M., Chiralt, A., and Fito P., Equilibrium in cellular food osmotic solution systems as
related to structure, J. Food Sci., 63, 1–5, 1998.
Chiralt, A., Fito, P., Andrés, A., Barat, J.M., Martínez-Monzó, J., and Martínez-Navarrete, N.,
Vacuum impregnation: a tool in minimal processing of foods, in Processing of Foods:
Quality Optimization and Process Assessment, Oliveira, F.A.R. and Oliveira, J.C.,
Eds., CRC Press, Boca Raton, FL, 1999, pp. 341–356.
Fito, P., Andrés, A., Chiralt, A., and Pardo, P., Coupling of hydrodynamic mechanism and
deformation relaxation phenomena during vacuum treatments in solid porous food-
liquid systems, J. Food Eng., 27, 229–240, 1996.
Fito, P. and Chiralt, A., Osmotic dehydration: an approach to the modelling of solid food-
liquid operations, in Food Engineering 2000, Fito, P., Ortega-Rodríguez, E., and
Barbosa-Cánovas, G., Eds., Chapman and Hall, New York, 1997, pp. 231–252.
Fito, P., Chiralt, A., Barat, J.M., and Martínez-Monzó, J., Vacuum impregnation in fruit
processing, in Trends in Food Engineering, Lozano, J.E., Barbosa-Cánovas, G.,
Parada Arias, E., and Añón, M.C., Eds., Technomic, Lancaster, PA, 2000, pp. 149–164.
Fito, P., Chiralt, A., Barat, J., Salvatori, D., and Andrés, A., Some advances in osmotic
dehydration of fruits, Food Sci. Technol. Int., 4, 329–338, 1998.

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Akritidis, C.B., Marinos-Kouris, D., and Saravacos, G.D., Eds., Ziti Editions, Thessa-
loniki, 1998b, pp. 836–843.
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Salvatori, D., Andrés, A., Chiralt, A., and Fito, P., 1998a. The response of some properties
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profiles in osmotically dehydrated apple, J. Food Sci., 63, 606–610, 1998b.

Effect of Pretreatment on
9 the Drying Kinetics
of Cherry Tomato
(Lycopersicon esculentum
var. cerasiforme)
P.M. Azoubel and F.E.X. Murr
CONTENTS
9.1 Introduction
9.2 Basic Concepts
9.2.2 Sorption Isotherms
9.2.3 Drying
9.3 Mathematical Models
9.5.1 Cherry Tomato Characterization
9.5.3 Sorption Isotherms
9.5.4 Air Drying
9.6 Conclusions
Nomenclature
Acknowledgment
References
9.1 INTRODUCTION
The cherry tomato (L. esculentum var. cerasiforme) is considered the ancestral form
of tomato (Folquer, 1976). This tomato type is an excellent source of vitamins A
and C (Gould, 1974) and is used in salads and has been used as a supplement in
astronauts’ diet during long periods of residence in space, due to its fast in vitro
production (Kaur-Sawhney et al., 1996).

The tomato is a very perishable fruit, necessitating the removal of water for its
preservation. The drying of solids is a common form of preservation, allowing the
foodstuff to be kept for a longer period than would otherwise have been possible
(Hawlader et al., 1991). In addition, dried food can be stored and transported at a
relatively low cost. However, water removal leads to a serious decrease in food
nutritive and organoleptic values, such as lignified texture, slow or incomplete
rehydration, and loss of juiciness characteristics of fresh fruit and vegetables. More-
over, color and smell are affected in a negative way. It is generally known that dried
food of the best quality is obtained by means of freeze-drying, but this is one of the
most expensive methods. For these reasons, efforts are being made to perfect the
convection drying process. The preliminary treatment of the raw material is of crucial
importance. The utilization of an osmotic prestep can have important advantages in
terms of product quality and cost (Lenart, 1996).
The present study was carried out to determine the influence of osmotic pre-
treatment on the drying kinetics of cherry tomato, using a fixed bed dryer.
9.2 BASIC CONCEPTS

Osmotic dehydration of foods has recently gained attention as a processing method
to obtain better quality fruit products. It is based on the immersion of foods, whole
or in pieces, in hypertonic solution (sugars, sodium chloride, glycerol, sorbitol),
originating two simultaneous counter-current flows: an exit of water from the product
to the solution and a migration of solutes from the solution to the solid. A third flow
consists of the loss of some natural components, such as sugars, organic acids, and
mineral salts; although these may be quantitatively of no significant meaning in the
mass exchange, they can be important to the final nutritive value and organoleptic
properties of the food (Raoult-Wack et al., 1989).
The quantity and rate of water removal depend on several variables and pro-
cessing parameters. In general, the weight loss in osmosed fruit is increased by
increasing solute concentration of the osmotic solution, immersion time, temperature,
solution/ fruit ratio, and specific surface area of the food and by using a low pressure
system (Lerici et al., 1985).
Osmotic dehydration has generally been applied to fruit, vegetables, meat, and
fish (Raoult-Wack et al., 1994). This process will not yield a moisture low enough
to make the product shelf stable, but it is considered a prestep to air, freeze, and
vacuum drying (Lenart, 1996; Uddin et al., 1990).
Since the osmotic process generally results in some solute uptake, changes in
the composition of the food material that can influence the subsequent drying step
must be considered. One important property of a material relative to drying is its
water sorption isotherm, since this will determine the degree of drying required to
obtain a stable product (Islam and Flink, 1982).

9.2.2 SORPTION ISOTHERMS
Moisture sorption isotherms can be used to predict changes in food stability and to
select appropriate package materials and ingredients (Zhang et al., 1996).
The isotherm curve can be obtained in one of two directions. An adsorption
isotherm is made by placing a completely dry material into various atmospheres
of increasing relative humidity and measuring the weight gain due to water. The
desorption isotherm is found by placing the initially wet material under the same
relative humidities, but in this case measuring the loss in weight (Iglesias and
Chirife, 1982).
There are several experimental means to determine sorption isotherms (Gal,
1972). The principal methods are:
• Gravimetric—The sample weight change in equilibrium with different

water vapor pressures is determined.
• Manometric—The vapor pressure of water in equilibrium with a food at
a given moisture content is measured by a sensitive manometric device.
• Hygrometric—The equilibrium relative humidity of a small amount of
air in contact with a food at a given moisture content is measured by a
hygrometric device.
A number of mathematical models have been proposed for correlation, analysis,

and prediction of sorption data, including Guggenheim–Anderson–de Boer (GAB)
(van den Berg and Bruin, 1981), Brunauer–Emmett–Teller (BET) (Brunauer et al.,
1938), and the models of Halsey (1948) and Oswin (1946), as respectively described
in the following equations:
X m CGAB K GAB a w
X= (9.1)
[(1 − K GAB a w ) (1 − K GAB a w + CGAB K GAB a w )]
X m C BET a w
X= (9.2)
(1 − a w ) [1 − (C BET − 1) a w ]
−A
a w = exp  B  (9.3)
X 
B
 a 
X=A w  (9.4)
 1 − aw 
where X is the moisture content (kg/kg, dry basis); Xm is the monolayer moisture
content (kg/kg, dry basis); CGAB and KGAB are GAB constants; aw is the water activity;
CBET is BET constant; A and B are Halsey and Oswin constants.

9.2.3 DRYING
Dehydration or drying operations are important steps in the chemical and food
processing industries. The basic objective in drying food products is the removal of
water from the solids to a level at which microbial spoilage is minimized (Vagenas
et al., 1990).
Drying is a process of simultaneous heat and mass transfer. Heat transfer occurs
during evaporation of the moisture removed from the drying solid object, while mass
transfer takes place during the removal of moisture from the object’s surface by an
external drying fluid, which is usually air (Dincer and Dost, 1995).
The drying curve includes a constant drying rate region and a falling rate region.
The constant rate period indicates that a film of water is freely available at the drying
surface for evaporation into the drying medium, while the falling rate period indicates
an increased resistance to both heat and mass transfer and occurs when the surface
water no longer exists, and water to be evaporated comes from within the structure
and must be transported to the surface. However, for some material, only the falling
rate regions are observed (Hawlader et al., 1991).
A wide variety of dehydrated foods (snacks, dry mixes and soups, dried fruits,
etc.) are available today (Vagenas et al., 1990). In the tropics, fresh tomatoes are
available throughout the year, while in temperate regions tomatoes are a seasonal
crop, and hence, a surplus exists in one season and a shortage in another. Currently,
tomatoes are preserved in the forms of ketchup, paste, and juice (Hawlader et al.,
1991).
9.3 MATHEMATICAL MODELS

The prediction of the kinetics of osmotic dehydration of cherry tomato was based
on a two-parameter equation from mass balance, using data obtained during a
relatively short period of time, as developed by Azuara et al. (1992) and adapted to
spherical geometry:
2
π t  S1 r   WLmod 
Dt =   ⋅ ∞
exp  
(9.5)
36  1 + S1t   WL ∞  
2 mod exp
where Dt is the apparent diffusion coefficient (m /sec) at time t; WL ∞ and WL ∞
are the amounts of water (g water/100 g of sample) leaving the solid after infinite
time, predicted by the model and experimental data, respectively; r is the radius of
the sample; and S1 is a constant related to the water loss, calculated from the
following linear regression that associates the water lost (WL) with time (t) (Azuara
et al., 1992):
t 1 t
= + (9.6)
WL S1 ( WL ∞ ) WL ∞

The value at equilibrium, WL ∞, is fixed for the established conditions of temper-
exp
ature, time, and fruit to solution rate. When WL ∞ is unknown, by assuming that it
mod
equals WL ∞ , Equation (9.5) may be used to obtain a good estimation for Dt, as long
as the kinetics data are adequately fitted by Equation (9.6). The value of WL is a function
of the rate of water loss and time. WL increases as these variables increase, and can
be calculated as:
ww o − ( tw − ws)
WL = × 100 (9.7)
wso + ww o
where wwo and wso are the initial water and solid contents (g), respectively, and tw
is the total wet weight.
The average apparent diffusion coefficient is calculated by:
∑D t
Davg = 1
(9.8)
n
where n is the number of data points used.

For drying kinetics, considering the cherry tomato slice as a flat plate with
initially uniform moisture distribution, negligible external resistance to mass transfer,
and no shrinkage, the solution for Fick’s equation is (Crank, 1975):
∞
w − we
∑ (2i + 1) exp −(2i + 1)2 .π 2 .Deff. . 2 
8 1 t
= 2 (9.9)
wo − we π i=0
2
 L 
where w, we and w0 are the moisture content at t, the equilibrium, and the initial
moisture content, respectively (g water/g dry mass); t is drying time (sec); L is length
of plane thickness (m); and Deff is effective diffusion coefficient for moisture in
2
solids (m /sec). The equilibrium moisture content of a sample being dried depends
upon the moisture content of the air and the structure and type of material (Hawlader
et al., 1991) and was obtained from water sorption isotherms for cherry tomatoes
with and without the osmotic pretreatment.
For conditions where L is small and t is large, the terms in the summation in
Equation (9.9) corresponding to n > 1 are small, and the following approximation can
be made (Hawlader et al., 1991):
 w − we   8  π Deff t
2
ln   = ln 2  − (9.10)
 wo − we  π L2
where Deff can be measured from the slope of the plot of ln ww −−wwe against t or t/L .
2
o e

The mean relative deviation modulus (E, %) was used as a criterion to evaluate
the fit of the tested model, as applied to the experimental data. Values of E were
calculated using the following equation:
ν0 − ν p
∑
100
E= (9.11)
N ν0
where ν0 and νp are the observed and the predicted values, respectively. Values of
E less than or equal to 10% are considered to fit the experimental data satisfactorily.

Fresh cherry tomatoes harvested between the end of January and the middle of May
were purchased from a local market. The fruits were sorted visually for color
(completely red), size (approximately 2.8 cm diameter), and lack of physical damage,
and the physicochemical characteristics were determined according to Ranganna
(1977).
As the cherry tomato waxy skin presents a high resistance to mass transfer, the
fruits were washed and perforated with needles (1 mm diameter) (Shi et al., 1997)
2
to pin hole density of 16 holes/cm . The perforated cherry tomatoes were immersed in
NaCl and NaCl + sucrose (3:2) solutions of different concentrations (10 and 25% w/w)
at 25°C (room temperature) and agitation of 70 r/min, maintained in a temperature–
agitation controlled shaker (Tecnal, TE-421). In order to avoid any significant
dilution effect on the osmotic solution, a 1:10 fruit-to-solution ratio was used. At
different processing times, samples were withdrawn from the solution, rinsed with cold
water to remove adhering osmotic solution, and gently blotted to remove surface
moisture.
The water content of cherry tomato samples was determined gravimetrically by
vacuum oven drying at 70°C for 24 h. The salt content was determined by Mohr’s
titration method (Ranganna, 1977). Three replications were made.
Desorption isotherms of the samples were determined using the static gravimet-
ric method. Saturated salt solutions were prepared to give defined constant water
activity (Greenspan, 1977). Three replications of the same experiment were carried
out. After equilibrium was reached, the equilibrium moisture content was determined
(vacuum oven at 70°C for 24 h). The adequacy of the mathematical models of BET,
GAB, Halsey, and Oswin was verified.
For air drying experiments, a cabinet dryer was used, and the tests were con-
ducted at three different temperatures (50, 60, and 70°C) and two air velocities (0.75
and 2.60 m/sec). The tomatoes were cut into quarters along the longitudinal axis
and the seeds were removed. The samples (length of 1.8 mm) were spread uniformly
on a perforated stainless steel tray in a fixed bed dryer. The processing temperature
was controlled using precalibrated cooper-[constantan] thermocouples and the air
flow rate was monitored by an anemometer (TSI, 8330-M). The drying curves were
determined by periodic weighing of the tray on a semianalytical scale.

9.5.1 CHERRY TOMATO CHARACTERIZATION
The physicochemical characteristics of the cherry tomatoes used in the experiments
are shown in Table 9.1.
The total solids content, acidity, and soluble solids content were similar to the
values obtained by Gould (1974) for tomato, but the NaCl content was higher and
the reducing sugars content was lower. Sugars and organic acids were the majority
of the total dry matter content of the tomato fruit. Similar results for cherry tomato
were obtained by Picha (1987). The pH value was similar to the results of Petro-
Turza (1987) for tomato and the density to tomato pulp (Ranganna, 1977).

Characterizing the effect of osmotic dehydration on the air drying kinetics of cherry
tomatoes was the main objective of this study. The effect of the osmotic agent (NaCl
and the NaCl–sucrose mixture) and solution concentration (10 and 25% w/w), at room
temperature (25°C), was evaluated by determining moisture and salt contents, as shown
in Figure 9.1. The more concentrated the solution, the higher the percentages of water
loss and solid uptake, due to an increase in osmotic pressure gradient resulting in
increased mass transfer. This finding is in agreement with the results of Rastogi and
Raghavarao (1994) for the osmotic dehydration of carrots in sucrose solutions, and of
Vijayanand et al. (1995) for cauliflower in salt solutions. The rate of water loss was
faster in the first 2 h of the process, decreasing gradually while approaching the end
of the experiment, which was not sufficient in length for equilibrium to be reached,
except for the 10% solution.
Figure 9.1(b) shows the salt gain during the osmotic dehydration of cherry
tomato. It was observed that an increase in the concentration of the osmotic solution
gave higher salt gain within 6 h of processing. By fixing the concentration of the
TABLE 9.1
Physicochemical Characteristics
of Cherry Tomatoes
Analysis Mean Value
Moisture content (%) 94.39

Acidity (% citric acid) 0.64
NaCl (%) 0.65
Reducing sugars (%) 1.03
pH 4.04
Brix 5.53
Ascorbic acid (%) 31.39
Density (g/ml) 0.99

TABLE 9.2
Average Water Apparent Diffusion Coefficient (Davg)
Obtained from the Osmotic Dehydration Process
2 10 2
Sample S1(10 ) Davg (10 m /sec) E (%)
Sodium chloride (10%) 1.76 11.69 8.85

Sodium chloride (25%) 2.28 14.42 0.12
Sodium chloride + sucrose (10%) 0.40 2.17 3.68
Sodium chloride + sucrose (25%) 1.75 11.66 10.01
100 10
NaCl 10% NaCl 10%
NaCl 25% NaCl 25%
96 NaCl+sucrose 10% 8 NaCl+sucrose 10%
Water content (%)
NaCl+sucrose 25% NaCl+sucrose 25%
Salt gain (%)

6
92
4
88
2
84
0
0 60 120 180 240 300 360 0 60 120 180 240 300 360
Time (min) Time (min)
(a) (b)
FIGURE 9.1 Moisture (a) and salt gain (b) profiles of osmotically dehydrated cherry tomato.
solution, the effect of the osmotic agent can be evaluated. Our results showed that
the salt gain was lower when the mixed NaCl–sucrose solution was used.
The experimental water loss results were used to estimate the apparent water
diffusion coefficients. The time used for prediction by the proposed model was
180 min. Table 9.2 presents the obtained average water apparent diffusivities (Davg)
and S1 values. Increasing the osmotic solution concentration (10 to 25% w/w) caused
an increase in Davg. Changing the osmotic medium from salt to a mixed salt–sucrose
solution, at the same temperature, resulted in a decrease of the diffusion coefficient.
This is due to sodium chloride ionization in solution, and as the molecular weight
of sodium chloride is lower than that of sucrose, its rate of penetration into vegetable
tissues is higher. Higher values for S1 indicate a higher diffusion of water per unit
of time. The model was able to predict the entire osmotic dehydration process up
to equilibrium, using data obtained over a short period of time, with satisfactory
mean relative modulus.
Consumer demand for fresh, convenient, and safe vegetables has promoted
interest in processed products with fresh-like qualities (Shi et al., 1997). The osmotic
dehydration process was carried out within a short period of time in order to achieve

0.5
T= 50°C (fresh)
0.4
T= 70°C (fresh)
we (kg/kg)
0.3 T=50°C (NaCl 10%)
0.2
0.1
0.0
0.0 0.2 0.4 0.6 0.8 1.0
aw
FIGURE 9.2 Sorption isotherms for fresh and osmoticly dehydrated cherry tomato.
a high degree of dewatering with relatively small solids gain. Pretreatment with sodium
chloride, 10% w/w for 2 h, was chosen for the air drying experiments, and desorption
isotherms of these samples were determined.
9.5.3 SORPTION ISOTHERMS

The results of the experimental measurements of the equilibrium moisture content (we)
of cherry tomato with and without pretreatment, at relative humidity ranging from
10.75 to 81.20%, are shown in Figure 9.2. The pretreated sample obtained lower values
of water activity than the fresh fruit. Sloan and Labuza (1976) noted that components
such as glycerol or salt are particularly effective in reducing the water activity. No
temperature dependence of the experimental data of the fresh fruit can be seen. Similar
behavior was observed by Bolin (1980) for prunes. The results for 50°C were consid-
ered for all samples, and temperature independence was assumed for the osmotically
pretreated samples. It can be seen that the desorption isotherms do not intersect. For
products with high sugar content, the intersection of sorption isotherms can be observed
(Saravacos et al., 1986). For products with low sugar, high protein, or high starch,
there is no intersection point with increased temperature (Benado and Rizvi, 1985).
The results of direct nonlinear regression analysis of fitting the GAB, BET, Halsey,
and Oswin models to the experimental points (Tables 9.3, 9.4, and 9.5) showed that the
GAB equation was satisfactory in predicting the equilibrium moisture content of fresh
cherry tomato, and that the Halsey model presented the best fit for samples pretreated
in 10% NaCl osmotic solution for 2 h (Figure 9.3).
9.5.4 AIR DRYING

The effect of air temperature (50, 60, and 70°C) at air velocities of 0.75 and 2.60 m/sec
on the drying kinetics of cherry tomato is illustrated in Figure 9.4. Increasing the
temperature of the drying medium increased the drying potential and the moisture
removal rates. When the flow rate was increased at constant temperature, similar
behavior was observed. The effect of osmotic pretreatment was clearly verified at a
temperature of 50°C and air velocity of 2.60 m/sec. In this condition, the drying time
was reduced, with higher drying rates and effective diffusion coefficients (Table 9.6).
For the other conditions studied (60 and 70°C at both air velocities), the drying
time of pretreated samples with 10% NaCl solution was not faster when compared

TABLE 9.3
Estimated Parameters for Fresh Cherry Tomato
ο
at 50 C
Model Parameters R
2
E (%)
BET Xm C n
0.133 20.087 S 0.979 3.221
GAB Xm C K
0.138 95.615 0.781 0.990 2.278
Halsey A B
0.026 2.205 — 0.995 2.341
Oswin A B
0.227 0.335 — 0.990 2.171
TABLE 9.4
Estimated Parameters for Fresh Cherry Tomato
ο
at 70 C
Model Parameters R
2
E (%)
BET Xm C n
0.145 11.154 S 0.97 8.022
GAB Xm C K
0.135 51.868 0.822 0.99 3.747
Halsey A B
0.036 1.988 — 0.99 6.617
Oswin A B
0.231 0.370 — 0.99 3.353
TABLE 9.5
Estimated Parameters for Osmosed Cherry
ο
Tomato at 50 C
Model Parameters R
2
E (%)
BET Xm C n
0.575 0.11 S 0.98 6.060
GAB Xm C K
0.074 5.973 0.991 0.99 2.573
Halsey A B
0.069 1.099 — 0.99 2.211
Oswin A B
0.120 0.751 — 0.99 3.353

0.5
0.4
we (kg/kg)
fresh (GAB)
0.3
0.2
0.1 NaCl 10% (Halsey)
0.0
0.0 0.2 0.4 0.6 0.8 1.0
aw
FIGURE 9.3 Equilibrium moisture content at 50°C and the predictions of the GAB and
Halsey models for fresh and preteated cherry tomato, respectively.
1.0 fresh (T = 50°C)

(w – we)/(wo – we)
10% NaCl (T = 50°C)

0.8
fresh (T = 60°C)
0.6 10% NaCl (T = 60°C)
fresh (T = 70°C)
0.4 10% NaCl (T = 70°C)
0.2
0.0
0 20 40 60 80 100 120 140
Time (min)
(a)
1.0 fresh (T = 50°C)

(w – we)/(wo – we)
10% NaCl (T = 50°C)

0.8
fresh (T = 60°C)
10% NaCl (T = 60°C)
0.6
fresh (T = 70°C)
0.4 10% NaCl (T = 70°C)
0.2
0.0
0 20 40 60 80 100 120 140
Time (min)
(b)
FIGURE 9.4 Effect of temperature on water removal for fresh and osmotically dehydrated
cherry tomato at constant air velocities of 0.75 m/sec (a) and 2.60 m/sec (b).
to the untreated samples at the same air temperature and velocity, The effective
diffusion coefficients were lower, indicating a less favored diffusional process. The
differences in the effective diffusion coefficients can be attributed to the composi-
tional changes that occur following osmosis. The uptake of salt and the loss of water
that occur in osmosis give increased internal resistance to moisture movement.
However, the dried cherry tomato in 10% NaCl solution presented a flexible struc-
ture, smaller shrinkage, and a more natural coloration when compared with the dried

TABLE 9.6
Effective Diffusion Coefficients of
Air Dried Cherry Tomatoes
11 2
Deff (10 m /sec)
o
T ( C) v (m/sec) Fresh 10% NaCl
50 0.75 12.02 12.02

2.60 13.66 17.49
60 0.75 17.49 14.21
2.60 26.78 19.67
70 0.75 20.77 18.03
2.60 37.70 21.86
TABLE 9.7
Activation Energy for Diffusion in
Cherry Tomatoes
Sample v (m/sec) Ea (kJ/mol) R
Fresh 0.75 25.39 0.99

2.60 46.61 0.99
10% NaCl 0.75 18.31 0.99
2.60 10.56 0.99
fruit with no preliminary treatment. The same behavior was found by Lenart (1996)
for osmodehydrated dried apples.
Figure 9.5 shows the variation in the drying rate for all samples as a function
of moisture content with air velocity and temperature. For the given experimental
conditions, the samples did not show a constant rate of drying. Higher temperature,
higher air velocity and the pretreatment for the lower temperature increased the
potential for the transport of moisture, thus increasing the drying rate. For temper-
atures of 60 and 70°C, the untreated samples showed higher drying rates in the
beginning, due to a higher free water content.
The activation energy was estimated by an Arrhenius type equation, using the
value of effective diffusivity for each temperature from Table 9.6:
 − Ea 
Deff = A exp (9.12)
 RT 
where Ea is activation energy (kJ/mol), R is the universal gas constant (8.314 J/mol
K), A is the integration constant, and T is temperature (K).
The values of activation energy and the correlation coefficient are presented in
Table 9.7. The pretreated samples’ activation energy was much lower than that of
the fresh samples, indicating that temperature has less influence on drying rate for

0.05
–dw/dt (10 kg/kg sec)

fresh (T = 50°C)
0.04 10% NaCl (T = 50°C)
fresh (T = 60°C)
0.03 10% NaCl (T = 60°C)
2
fresh (T = 70°C)
0.02 10% NaCl (T = 70°C)
0.01
0.00
0.0 0.2 0.4 0.6 0.8 1.0
w (kg/kg)
(a)
0.08
–dw/dt (10 kg/kg sec)
fresh (T = 50°C)
10% NaCl (T = 50°C)
0.06 fresh (T = 60°C)
10% NaCl (T = 60°C)
0.04 fresh (T = 70°C)
2
10% NaCl (T = 70°C)
0.02
0.00
0.0 0.2 0.4 0.6 0.8 1.0
w (kg/kg)
(b)
FIGURE 9.5 Drying rate vs. moisture content at constant air velocities of 0.75 m/sec (a) and
2.60 m/sec (b).
salt osmosed fruits. These results are similar to those of Islam and Flink (1982) for
osmotically dehydrated potatoes in NaCl solution.
9.6 CONCLUSIONS
The rate of moisture removal and solids gain in the osmotic dehydration of cherry
tomato was directly related to the concentration of the solution, the osmotic agent
and the immersion time. In order to obtain a processed product with fresh-like
qualities, pretreatment with 10% NaCl solution for 2 h was the condition used prior
to drying.
The water apparent diffusivity for osmotic dehydration ranged from 2.17 ×
–10 –10 2
10 to 14.42 × 10 m /sec and the calculated effective diffusivity ranged from
–11 –11 2 –11
12.02 × 10 to 37.70 × 10 m /sec for fresh fruit and from 12.02 × 10 to 21.86 ×
–11 2
10 m /sec for cherry tomatoes pretreated in 10% NaCl solution for 2 h. For the
given experimental conditions, the samples did not show a constant rate of drying.
Osmotic dehydration of cherry tomato in 10% NaCl solution for 2 h before air
drying was efficient in increasing the water removal rate and the effective diffusion
o
coefficient, and in decreasing the drying time at 50 C with air velocity of 2.60 m/sec.

For all conditions studied, the osmodehydrated dried samples presented a flexible
structure, smaller shrinkage, and a more natural coloration when compared to dried
cherry tomato with no preliminary treatment.
The activation energy for effective diffusivity was lower for osmosed samples,
indicating less influence of temperature on drying rate.
NOMENCLATURE
2
Davg Moisture apparent diffusion coefficient, m /sec
2
Deff Moisture effective diffusion coefficient, m /sec
Ea Activation energy, kJ/mole
L Thickness, m
R Universal gas constant, J/mol K
R Radius, m
t Time, sec
w Moisture content, kg/kg
we Equilibrium moisture content, kg/kg
w0 Initial moisture content, kg/kg
WL Water loss, g water/100 g sample
WL∞ Amount of water leaving the solid at equilibrium, g water/100 g sample
T Temperature, K
ACKNOWLEDGMENT
The authors gratefully acknowledge the financial support of CAPES.
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Determination
10 of Concentration-
Dependent Effective
Moisture Diffusivity
of Plums Based on
Shrinkage Kinetics
A.L. Gabas, F.C. Menegalli, and J. Telis-Romero
CONTENTS
10.1 Introduction
10.2 Mathematical Model
10.3 Methodology
10.3.1 Material
10.3.2 Drying Apparatus and Conditions
10.3.3 Shrinkage Kinetics
10.4 Shrinkage and Effective Diffusivity
10.5 Conclusions
Nomenclature
Acknowledgment
References
10.1 INTRODUCTION
Air drying is one of the most used unit operations in food processing, and mathe-
matical modeling of the dehydration process is very useful in the design and opti-
mization of dryers (Madamba, 1997; Arrouz et al., 1998). Nevertheless, theoretical
simulations of drying processes require a substantial amount of computing time as
a consequence of the complexity of diffusion equations governing the process. A
drying process can be described completely using an appropriate drying model made

up of differential equations of heat and mass transfer in the interior of the product and
its interface with the drying agent (air). Knowledge of transport and material prop-
erties is necessary to apply any transport equation. Such properties as diffusivity
and mass and heat transfer coefficients, as well as thermal conductivity, must be
accurately estimated. Knowledge of additional properties such as equilibrium mois-
ture content, shrinkage, bulk density, specific volume, and porosity, is also required.
Many articles have recently been published concerning the estimation of the above-
mentioned properties (Zogzas et al., 1994; Madamba et al., 1994; Barbanti et al., 1994;
Newman et al., 1996; Sabarez et al., 1997; Karathanos, 1999; Telis et al., 2000).
Shrinkage is common during drying, and volume changes may affect the mois-
ture removal rate. Study of the shrinkage phenomenon is essential to better under-
stand drying kinetics and to improve the reliability of diffusivity based models
(Raghavan et al., 1995; Simal et al., 1996; Sanjuán et al., 1996).
Drying of plums (Prunus domestica) in drying tunnels produces prunes generally
at about 14–19% moisture content (wet basis), which have sufficiently low water
activity to avoid the problems of microbial spoilage, allowing long-term storage of
the fruit. These fruits are then rehydrated (35–40%) prior to packing and sale. Many
countries have a flourishing prune industry, including the U.S., France, Italy, Turkey,
Chile, Argentina, and Australia (Price et al., 1997). The drying kinetics of plums
have been investigated as a function of temperature in the range of 50 to 80°C using
a laboratory pilot plant. The volume change or shrinkage of grapes during thin layer
convective air drying has been described by a correlation with respect to water
content (Gabas et al., 1999). The method for evaluating effective diffusivity as a
function of moisture content and shrinkage during drying of plums is based on
numerical solution to Fick’s diffusion equation.
A number of studies have focused on modeling the drying process of fruits and
vegetables and solving the mass transfer equation analytically. Córdova-Quiroz et al.
(1996) obtained a simplification of boundary conditions of the mass transfer equation
in cylindrical slabs of carrots. They developed an alternative simplification for the
mathematical description of interfacial mass transfer, introducing a modified Biot
number. Hernández et al. (2000) proposed an analytical solution of a mass transfer
equation with concentration dependence of shrinkage and constant average water
diffusivity for mango slices and cassava parallelepipeds. Although the drying behav-
ior of a range of fruits and vegetables has been extensively studied, there is relatively
little work on the kinetics of drying of plums, especially simultaneously considering
shrinkage and diffusivity as a function of moisture content.
10.2 MATHEMATICAL MODEL

A mass balance for the drying process of plums can be applied by considering the fruit
as a sphere (Figure 10.1), according to the system of coordinates presented in Figure 10.2.
The partial differential equation resulting from the mass balance at a differential
2
volume element r (senφ)∆φ∆ψ∆r is shown as (Bird et al., 1960):
∂ ρA  → → → →
+ ∇⋅ ρA v  =  ∇⋅ D AB ∇ ρA  + q A (10.1)
∂t    

r(senφ)∆ψ
r ∆φ
∆r
flesh
stone
rs
rp
2
FIGURE 10.1 Differential volume element r (senφ)∆φ∆ψ∆r by considering the plum as a sphere.
∆r
r∆φ
∆φ r
r(sen φ)∆ψ
∆ψ
r senφ
2
FIGURE 10.2 System of spherical coordinates with the volume element r (senφ)∆φ∆ψ∆r for
the mass balance.
The following hypotheses are generally used to describe the mass transfer in
solid drying: unsteady state system, constant temperature and pressure, constant
mass density and diffusion coefficient, negligible convective mass transfer, and
absence of chemical reactions. Thus, assuming that internal resistance controls the
drying rate, the differential equation for spherical coordinates in terms of Fick’s

second law is (Bird et al., 1960):
∂ρA r
= D AB∇2ρA (10.2)
∂t
Most cereals (rice, corn, wheat, etc.) experience little change of volume during
the drying process. Therefore, the analytical solution of Equation (10.2) applies satis-
factorily to the study of these materials. On the other hand, for high moisture content
foods (potato, apple, persimmon, grape, plum, etc.) the volume variation is important,
and the analytical solution of Equation (10.2) obtained for diffusivity and volume
constant is not applicable, since the shrinkage and values of diffusivity as a function
of moisture content should be taken into account.
The drying process of plums can be studied by solving the second Fick’s law
by numerical methods, considering moving boundary conditions and diffusion coef-
ficient as a function of moisture content (Murray and Landis, 1959; Gabitto and
Aguerre, 1985; Sobral, 1987).
The plum is viewed as a composite spherical body comprised of two concentric
materials (stone and flesh). The flesh component of the spherical plum is divided
into N concentric spherical shells of equal thickness. The radial length of the fruit
decreases due to shrinkage; consequently, the thickness of each shell reduces as
drying progresses.
The following dimensionless groups are necessary in order to have Equation (10.2)
in a dimensionless form:
X − Xe
M= (10.3)
Xo − Xe
r
ξ= , in (r > rs) (10.4)
rpo
Deff t
Fo = (10.5)
r2
Substituting and rearranging the differential of Equations (10.3) and (10.4), and
using the definition of Fourier mass number (Equation (10.5)), the second Fick’s law
in spherical coordinates is developed and presented in the following form:
∂M 2 ∂M ∂2 M
= + 2 (10.6)
∂Fo ξ ∂ξ ∂ξ
with the initial and boundary conditions:
Fo = 0, M=1 (10.6a)
∂M
ξ = 1, = − Bi m Ms (10.6b)
∂ξ
rs ∂M
ξ= , =0 (10.6c)
rpo ∂ξ

Equation (10.6) cannot be integrated, since it does not represent a moving
boundary system, and shrinkage was not considered. In order to allow its integration,
the following substantial derivative is defined:
dM ∂M ∂M ∂ξ
= + (10.7)
dFo ∂Fo n ∂ξ ∂Fo n
as well as the expression that relates the position of an arbitrary nodal point with
the interface position:
n
ξ= ξ (10.8)
N p
Equation (10.8) can be derived to give:
∂ξ n ∂ξ p
= (10.9)
∂Fo N ∂Fo
Substituting equations (10.7), (10.8) and (10.9) in Equation (10.6), the repre-
sentative differential equation of the moving boundary system is:
dM  2 N n  ∂ξ p   ∂M ∂2 M
= + + 2 (10.10)
dFo  nξ p N  ∂Fo   ∂ξ ∂ξ
with the initial and boundary conditions:

Fo = 0, M=1 (10.10a)
∂M
ξ = ξp, = − Bi m Ms (10.10b)
∂ξ
rs ∂M
ξ= , =0 (10.10c)
rpo ∂ξ
Equation (10.10) represents the second Fick’s law expressing the drying process
considering shrinkage and diffusivity varying with average moisture content. Con-
sidering that this equation can be expressed in finite differences, it is solved using
Equations (10.11), (10.12), and (10.13):
dM M n ,i +1 − M n ,i
= (10.11)
dFo ∆Fo
∂M M n +1,i +1 − M n −1,i +1
= (10.12)
∂ξ 2 ∆ξ
∂2 M M n −1,i +1 − 2 M n ,i +1 + M n +1,i +1
= (10.13)
∂ξ 2 ∆ξ 2

Combination of equations (10.10), (10.11), (10.12) and (10.13) leads to:
M + M n −1,i +1 
M n ,i +1 − M n ,i = λ 2 k  n +1,i +1  + λ1 (M n −1,i +1 − 2 M n ,i +1 + M n +1,i +1 ) (10.14)
 2 
where:
∆Fo
λ1 = (10.14a)
∆ξ 2
∆Fo
λ2 = (10.14b)
∆ξ
2 N n  ∂ξ p 
k= + (10.14c)
nξ p N  ∂Fo 
i = temporary coordinate index;
n = space coordinate index;
with the following initial and boundary conditions:

Fo = 0, M=1 (10.14d)
(M N − M N −1 )
ξ = ξp, = − Bi m M N (10.14e)
∆ξ
rs
ξ= , M0 = M1 (10.14f)
rpo
A rearrangement of Equation (10.14) will result in:
 λ k  λ k
− λ1 + 2  M n −1,i +1 + (1 + 2λ1 )M n ,i +1 −  λ1 + 2  M n +1,i +1 = M n ,i (10.15)
 2   2 
In this way, the integration of Equation (10.2) consists of the solution of a system
constituted by the development of Equation (10.15) in a matrix form (n = 1 to n = N – 1).
For evaluation of Equation (10.14c), the particle radius and its derivation are
determined by applying the finite difference:
∂ξ p rpi − rpi −1
= (10.16)
∂Fo ∆Fo ⋅ rpo
The particle radius at a time ti and ti−1 is calculated from the relation between
volume and moisture content experimentally obtained for the total drying time. The
∆Fo term is evaluated as follows:
Deff ( x ) ∆t
∆Fo = 2
(10.17)
rpo
where ∆t is a time interval between the sample collection in the drying experi-
ments, and Deff ( x ) (effective moisture diffusivity) is calculated through an iterative

procedure aiming to adjust the experimental and calculated values of average residual
moisture.
The group of equations (10.14a, b, c) was completed considering ∆ξ equal to
1/N, since the nodal points number is constant.
In order to apply the boundary condition corresponding to Equation (10.14e), it
is necessary to evaluate the Biot mass number (Bim) by assuming a linear relationship
between the food material and the air moisture at equilibrium (Córdova-Quiroz et al.,
1996):
k c K eq rpo
Bi m = (10.18)
Deff
Y∗ = K eq X (10.18a)
The parameter Keq represents an average partition constant. It may be evaluated
with the equation suggested by Hernández et al. (2000):
Xe
K eq =
∫ Xo
(Y∗ / X)dX
(10.18b)
Xo − Xe
where
a w ( Pvap / P ) 18
Y∗ = (10.18c)
1 − a w ( Pvap / P ) 28
Data on water activity can be obtained from Gabas et al. (2000), showing the
desorption isotherms of plum pulp described by the Guggenheim–Anderson–de Boer
(GAB) model.
The mass transfer coefficient in Equation (10.18) can be calculated by an empirical
equation (Equation (10.19)) applied to mass transfer between spheres and air for
turbulent flow in fixed bed (Saravacos, 1986):
1 1
Sh = 2 + 0.6 Re p 2 Sc 3 (10.19)
The water vapor diffusivity in the air is evaluated by the Schmidt correlation
(Dãscãlescu, 1969):
(Ta + 273)1.81
D vap = 0.083 (10.20)
273
A computational program written in Fortran is applied to the numerical integra-
tion of Equation (10.2). Equation (10.15) is written in a matrix form and solved
using the Gauss-elimination procedure, obtaining the moisture profile. The space-
averaged moisture content in a plum material is given by:
rp
X =
∫ rs
X drp
(10.21)
rp − rs

and, in the dimensionless form:
ξp
M =
∫ ξs
M d ξp
(10.22)
ξ p − ξs
Equation (10.22) is integrated by using the composite Simpson’s rule to calculate

the average moisture content.
10.3 METHODOLOGY
10.3.1 MATERIAL
All the experimental measurements were made with plums of the Angeleno variety
acquired in a local market and kept at 7°C prior to use. The plums were pretreated
in a solution of 1.5% ethyloleate for 1 min at 50°C and then rinsed in a current of
water for 2 min.
10.3.2 DRYING APPARATUS AND CONDITIONS

The dryer used to conduct the experiments is a pilot-scale piece of equipment
consisting of three basic parts: an airflow rate control system, a drying air heating
section, and a drying chamber; it is equipped with a process control system based
on Fieldbus technology supplied by SMAR Industrial Equipment Ltd.
As indicated in Figure 10.3, a centrifugal fan (1) was used to force the air through
the drying chamber. The fan was driven by an electric motor with the airflow rate
being controlled by a frequency modulator (2) (Siemens, model MMV). An orifice
plate (3) connected to a pressure transmitter (SMAR, model LD302) (4) was installed
after the fan to measure the airflow during the process. Dry bulb (5) and wet bulb
(6) temperatures of the air stream were measured online using temperature trans-
mitters (SMAR, model TT302). The drying air was heated by passing through electric
resistances (7) controlled by a power converter (8) (Therma, model TH 6021A/80).
Before the drying chamber, a “beehive” (9) was installed for better distribution of
air in the product. The drying compartment (10) consisted of two square metal trays,
placed perpendicular to the airflow. These compartments were designed for experi-
ments of through drying. Thermocouples connected with temperature transmitters
(SMAR, model TT302) were placed before and after the trays (11,14), and at the
center (12) and surface (13) of the plums to analyze the evolution of temperature in
the product during the experiments. In order to integrate the instruments with the
Fieldbus system, a 4–20 mA current converter (SMAR, model IF302) (15) was used.
The equipment operation was monitored and controlled by means of a computer

(16) running the software AIMAX -WIN.
The drying experiments were carried out in air at temperatures in the range of
50 to 80°C and with an air velocity of approximately 1.5 m/sec.

14 16
10
13
12
11
9 15
6 5 4
2
7
8
3
1
FIGURE 10.3 Experimental drying apparatus: (1) centrifugal fan, (2) frequency modulator,
(3) orifice plate, (4) pressure transmitter, (5) dry bulb temperature, (6) wet bulb temperature,
(7) electric resistance heaters, (8) power converter, (9) beehive, (10) square metal trays,
(11) thermocouple before the trays, (12) thermocouple at the center of the plum, (13) thermo-
couple at the surface of the plum, (14) thermocouple after the trays, (15) current converter,
(16) computer.
10.3.3 SHRINKAGE KINETICS

The shrinkage kinetics of the particles was used to correlate instantaneous size
(spherical equivalent diameter) as a function of material moisture content. The
dimensional change of the plum was assumed to occur only in the flesh section
(rs < r < rp), and the volume of the stone component was considered constant
throughout the drying process. Samples were placed on the tray in a single layer.
The volume change was determined with about 48 plums, from which samples of
three were taken out periodically from the dryer, to measure the total volume by the
water displacement method. Moisture content of the samples was determined by
drying at 60°C under vacuum for 48 h (AOAC, 1990).
10.4 SHRINKAGE AND EFFECTIVE DIFFUSIVITY

The volume change or shrinkage during thin layer convective air drying of plums
is described as a linear function of moisture content by the following equation:
V/Vo = A + BX (10.23)
Table 10.1 shows the constants A and B at different temperatures and the coefficient
2
of determination (r ), which presented satisfactory values. This equation is used to
estimate the particle radius of the plum in the numerical solution described previously.

TABLE 10.1
Constants of Equation (23), Which
Describes the Volume Change during
Drying of Plums at Different Temperatures
o a a 2
T ( C) A B r
50 0.174 0.172 0.998

60 0.181 0.174 0.988
70 0.191 0.175 0.997
80 0.193 0.178 0.998
a
All fits had a significance level less than 5%.
1.0
0.8
0.6
V/Vo
0.4
T = 80°C
T = 70°C
T = 60°C
0.2
T = 50°C
0.0
0 1 2 3 4 5
Moisture content (dry basis)
FIGURE 10.4 Shrinkage during drying of plums.
Figure 10.4 shows the volume change of the plums at 50–80°C, where considerable
shrinkage is observed, although with little influence of temperature. This can be
attributed to the viscoelastic nature of the material, which suffers a structural collapse
during drying. Similar results were obtained for thin layer drying of Thompson seedless
grapes by Rhagavan et al. (1995), who found a linear relationship of volume change
as a function of the moisture content of the berries. Simal et al. (1996) employed a
diffusivity model with moving boundary conditions to simulate the drying kinetics of
seedless grapes of the Flame variety, with the volume change represented by plotting
V/V0 vs. X/X0 and by fitting a linear equation with similar constants.
The initial moisture content was similar for all samples of plums. The influence
of air drying temperature on the drying curves can be observed in Figure 10.5. As
expected, increases in the air temperature substantially shortened the drying time in
o
comparison with that observed at 50 C. The drying time required to evaporate 90%
o
of water was shorter by 39.8, 57.7, and 70.5% at 60, 70, and 80 C, respectively,
o
compared to that at 50 C. Therefore, it is evident that at the same water content, the

4.0
3.5

3.0
T = 80°C
2.5
T = 70°C
2.0 T = 60°C
T = 50°C
1.5
1.0
0.5
0.0
0 500 1000 1500 2000 2500
Drying time (min)
FIGURE 10.5 Drying curves of plums at different temperatures; symbols refer to experimental
data; (— —) analytical solution from Equation (10.2); ( ) numerical solution from
Equation (10.15).
drying rate is dependent on air temperature. Induction periods or constant drying

rate periods were not observed, and the drying was characterized only by the falling
rate period. Barbanti et al. (1994), writing about air drying kinetics of cultivar plums,
also observed that there was no constant drying rate period in this process. The
existence of only the falling rate period could be indicative of a diffusion-controlled
mechanism of drying.
It can be also seen in Figure 10.5 that the analytical model of Fick’s Law, consid-
ering radius and effective diffusivity constants, is not applicable to fit the experi-
mental data in the final drying period. However, during the drying period fitted by
this model, the plums had not reached the commercially desirable moisture content
(approximately 0.15 kg water/kg dry matter). In addition, according to Figure 10.4, the
radius of the plum is a function of moisture content, showing that shrinkage has to
be taken into account during the drying process. The apparent agreement between
the analytical solution of Equation (10.2) applied to plums and the experimental
data in a great part of the drying curves (Figure 10.5) could be explained by sup-
posing a simultaneous decrease in the effective diffusivity and in the radius, in such
a way that these effects compensated for each other. The numerical solution fitted
to the experimental data can be also seen in this figure. As expected, a good
adjustment was obtained for all drying curves, including for the final drying period.
From the numerical solution of Fick’s second law, the effective diffusivity as a
function of simultaneous shrinkage and moisture content can be calculated. Figure 10.6
presents the effective diffusivity behavior with decreasing moisture content of the
plums, and it can be observed that the effective diffusivity parameter is far from
being constant during the process. The effective diffusivity is more influenced by
o
moisture content at 80 C than at other temperatures. On the other hand, neglecting
o
the initial inductive period, the effective diffusivity at 60 and 50 C changes almost

1.00E-009
T = 80°C
Effective diffusivity (m2/s)

8.00E-010
T = 70°C
6.00E-010
T = 60°C
4.00E-010
T = 50°C
2.00E-010
0.0 0.5 1.0 1.5 2.0 2.5 3.0 3.5 4.0 4.5
FIGURE 10.6 Variation of effective diffusivity with moisture content of plums at different
temperatures.
90
T = 50°C
80
T = 60°C
T = 70°C
Temperature (°C)
70
T = 80°C
60
50
40
30
20
0 1 2 3 4
FIGURE 10.7 Evolution of temperature inside plums during drying.
linearly with decreasing moisture content. The increase of effective diffusivity in

this initial period could be attributed to the time necessary for the temperature of
the plum to increase until it reaches the drying process temperature. According to
Figure 10.7, in general, the temperature of the fruit begins to reach equilibrium with
the drying air at a moisture content of approximately 3.0 kg/kg dry mass. Sabarez
et al. (1997) reported that the resistance to moisture transfer through the skin layer
is important during drying of plums, particularly in the early stages of drying. These
authors concluded that the skin layer limits the maximum effective evaporation rate
from the plum surface and provides significant resistance to initial moisture loss.

39
38
Activation energy (kJ/mol)

37
36
35
34
33
32
0.0 0.5 1.0 1.5 2.0 2.5 3.0
FIGURE 10.8 Relationship between activation energy for water diffusion and moisture con-
tent in plums undergoing drying
Raghavan et al. (1995) obtained effective diffusivity values varying with moisture
content under convective and microwave drying of grapes, and these values were found
to decrease with decreasing water content. Effective diffusivity coefficients considering
shrinkage but not varying with moisture content were reported by Hawlader et al.
(1991) for tomatoes and by Simal et al. (1996), who obtained diffusivities of around
–10 –9 2 –1
4.7 × 10 to 1 × 10 m sec for grapes. Sabarez and Price (1999) studied the drying
of plums of the d’Agen variety and obtained Deff values in the range of 4.3 to 7.6 ×
–10 2 –1
10 m sec at 70, 75, and 80°C.
The temperature dependence of the diffusivity can be represented by an Arrhe-
nius type equation (Simal et al., 1996; Lewick et al., 1998; Simal et al., 2000). The
activation energy for diffusion is calculated by taking a log plot of effective diffu-
sivity at constant moisture content, against the reverse of the absolute air drying
temperature. The relationship between activation energy and moisture content is
presented in Figure 10.8. The tendency of increasing activation energy with decreas-
ing moisture content is expected, and the majority of researchers have recognized
this effect, especially for the low moisture content range. Satisfactory values of the
determination coefficient (0.99) were obtained during the fitting procedure.
10.5 CONCLUSIONS
The volumetric shrinkage of plums results in a linear correlation with respect to the
moisture content. The finite difference method can be used for more accurate pre-
dictions and simulation of the drying process, and effective diffusivity values can
be obtained as a function of moisture content, taking into account the shrinkage of
the material. In general, these values are found to decrease with decreasing moisture
content. The reported moisture diffusivity data at different temperatures falls between

–10 –10 2
1.2 × 10 and 8.9 × 10 m /sec. These results lead to the conclusion that shrinkage
and moisture content cannot be neglected in establishing reliable values of effective
diffusivity. The activation energy for diffusion is also dependent on the moisture
content. It increases with decreasing water content in plums undergoing drying.
NOMENCLATURE
A Constant in Equation (10.23)
aw Water activity
B Constant in Equation (10.23)
Bim Biot mass number ([kc ⋅Keq ⋅rpo]/Deff)
d Sphere diameter (m)
2
DAB Diffusion coefficient (m /sec)
2
Deff Effective diffusivity (m /sec)
2
Dvap Water vapor diffusivity in the air at a temperature Ta (m /h)
Ea Activation energy (kJ/mol)
2
Fo Fourier mass number ([Deff ⋅t]/[rpo] )
Keq Average partition constant
kc Mass transfer coefficient (m/sec)
m Mass (kg)
M Residual moisture content
Ms Dimensionless moisture content at the surface of the plums
N Number of nodal points
n Arbitrary nodal point
P Total pressure (atm)
Pvap Vapor pressure of water (atm)
qA Chemical reaction in Equation (10.1)
R Universal gas constant (8.314 J/mol K)
Rep Modified Reynolds number ([ρ⋅v⋅d]/µ)
rs Radius of the stone (kernel + shell) component (m)
rp Radius of the whole plum (m)
rpo Radius of the plum at t = 0 (m)
Sc Schmidt number (µ/ρ⋅Dvap)
Sh Sherwood number ([kc ⋅d]/Dvap)
Ta Air temperature (°C)
t Time (sec)
v elocity (m/sec)
3
V Volume (m )
3
Vo Initial volume (m )
X Moisture content dry basis (kg/kg dry matter)
Xo Initial moisture content (dry basis)
Xe Equilibrium moisture content (dry basis)
∗
Y Molar fraction at equilibrium

GREEK SYMBOLS
ξ Radial coordinate (m)
ξp Dimensionless particle radius (rp(t)/rpo)
3
ρ Density (kg/m )
µ Viscosity (kg/m sec)
ACKNOWLEDGMENT
The authors acknowledge financial support from São Paulo State Research Fund
Agency, FAPESP (Processes: 98/12283–5; 98/08738–7 and 98/05130–8).
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Modeling Dehydration
11 Kinetics and
Reconstitution
Properties of Dried
Jalapeño Pepper
R. Olivas-Vargas, F.J. Molina-Corral,
A. Pérez-Hernández, and E. Ortega-Rivas
CONTENTS
11.1 Introduction
11.4 Conclusions
Nomenclature
Acknowledgments
References
11.1 INTRODUCTION
Drying is a physical separation process that has the objective of removing a liquid
from a solid phase by means of thermal energy. The liquid is generally water and is
liberated by vaporization rather than by breaking chemical bonds between the liquid
and the solid; i.e., the liquid is not chemically bound to the solid. In most industrial
drying applications, it is neither necessary nor economically feasible to remove every
vestige of water from the solid; thus, commercially dry solids will usually contain a
certain amount of residual moisture, the amount of which is determined by a compro-
mise between product quality and economic factors. In food and biological materials,
low moisture levels are necessary to stop or slow the growth of spoilage microorgan-
isms, as well as the occurrence of undesirable biochemical and enzymatic reactions.
The fundamental principles underlying drying processes are, in general, those
typical of the science of heat and mass transfer. Drying, as a unit operation in food
and chemical engineering, is characterized by the separation, usually partial, of a

liquid contained within a solid by the process of vaporization of the liquid into a
gas phase. The mechanism of the drying process, as controlled by the principle of
heat and mass transfer, consists of the transport of mass from the interior of the
solid to the surface, the vaporization of the liquid at or near the surface, and the
transport of the vapor into the bulk gas phase. Simultaneously, heat is transferred
from the bulk gas phase to the solid phase, where all or a portion of it provides for
vaporization, and the remainder accumulates in the solid as a sensible heat. The
overall rate by which the above sequence of steps takes place defines the drying rate
and is inversely related to the drying time.
Regardless of how heat is provided, the drying cycle generally consists of three
steps:
1. Before any evaporation takes place, sensible heat must be added to the
drying mass until the boiling point of the liquid under the given operating
conditions is reached.
2. Once the boiling point is reached, evaporation takes place at a rate related
to the moisture level in the solid, and this rate is normally constant over
a certain moisture range.
3. At some condition, a critical moisture point is reached and the drying rate
begins to fall.
Constant rate drying is the first stage, in which drying occurs at or near the
boiling point of the liquid. There is no resistance to vaporization, since the moisture
appears on the surface of the solid, completely wetting the outer surface. The constant
drying rate is proportional to the difference between the vapor pressure of the liquid
covering the surface of the solid and that of the vapor surrounding the wetted solid.
It has been found that the vapor pressure of the wetting liquid is very close to that
of the pure liquid at the same temperature.
At the critical moisture content of the solid, the drying rate begins to fall because
there is not enough moisture to completely cover the solid surface. The reduced
amount of moisture being evaporated comes from the interstices of the solid through
the porous structure. Falling rate drying is controlled by the physical properties of
the liquid and solid. The rates of movement of the liquid and its vapor depend on
capillary size, glazing of the solid, pressure gradients between trapped liquid and
vapor, and the environs of the solid, as well as on cracking, checking, etc. At the
same time, the heat transfer rate to the interior of the solid is being slowed because
of the receding boundary of the liquid-wetted portion of the particle. This boundary
movement increases the resistance to heat flow because it reduces the thermal
conductivity within the solid. Cracking and checking disrupt the paths of heat
transfer, further reducing the rate.
Moisture migration during drying has been explained by different models. Four
mechanisms are recognized: capillarity, concentration gradient diffusion, vapor dif-
fusion by pressure difference, and layer diffusion across solid–fluid interfaces (Bren-
nan, 1994). Capillary forces are responsible for water retention in porous solids or
those of rigid construction, while osmotic pressure is responsible in aggregates of
fine powders and on the surface of the solid (Toei, 1983). It has been reported that

moisture migration by diffusion is the predominant mechanism in drying of many
food products, such as vegetables (Geankoplis, 1983).
Drying data are usually expressed as total weight of the material as a function
of time during the drying process. These data can also be expressed in terms of
drying rate by recalculation of some values. The moisture content is defined as the
ratio of the amount of water in the food to the amount of dry solids, i.e.,:
Wt − Fs
Xt = (11.1)
Fs
where Xt is the moisture expressed as weight of water/weight of dry solids, Wt is

the total weight of the material at time t, and Fs is the weight of the dry solids. An
additional important quantity used in designing drying processes is the free moisture
content X, which can be evaluated considering the equilibrium moisture content Xeq,
by the simple relation:
X = X t − X eq (11.2)
As previously mentioned, moisture contents can be recalculated to obtain drying

rates. The rate of drying R can be expressed proportional to the change in moisture
content as a function of time t, by the following relationship:
dX
R∝ (11.3)
dt
Individual values of dX/dt as a function of time t can be obtained from tangent

lines drawn to the curve of X vs. t. Replacing the proportionality condition in
Equation (11.3) by Fs /A, the drying rate can be represented by:
 Fs   dX 
R=− (11.4)
 A   dt 
where A is the drying surface area.

Drying of fruits and vegetables follows conventional dehydration theory, which
was adapted from drying of inorganic materials and other raw materials in the chemical
processing industry (Sarvacos and Charm, 1962). The advantages of reducing moisture
content below 5% in biological materials are well known: microbial and enzyme
activity are practically stopped, and transport costs are greatly reduced. However, fruits
and vegetables can also suffer undesired changes due to the drying process. Shrinkage,
case hardening, texture damage, and reconstitution difficulty can be caused by drying
(Brennan, 1994). Dehydrated vegetables, when reconstituted, cannot match the original
texture even if precautions are taken during the entire drying process.
The large scale of industrial drying makes the analysis of the process difficult.
Operators and process engineers often have only a few variables to use in formulating

any changes needed to control the operation. Typically, the feed rate is held constant
and the controlling variable is the drying medium temperature. The operator may
use exaggerated safety factors to prevent product build-up or over-drying. Mathe-
matical modeling may be considered an efficient tool to overcome inefficiencies of
drying plants such as damaged product, wasted energy, wear on the dryer, or
decreased throughput.
Models to describe dehydration of foods are necessary for process design,
improvement, and minimization of energy while keeping quality as unimpaired as
possible. Development of mathematical models to describe drying of porous solids
has been the topic of many research studies for many years. Heat and mass transfer
take place in a porous solid when it contains moisture and is subjected to any or all
of the gradients of concentration, partial vapor pressure, temperature, total pressure,
and external force fields. There has been no general agreement among researchers
on which driving forces predominate, considering different materials or media and
external drying conditions. More and more sophisticated drying models are becom-
ing available based on either a mechanistic classical approach or on nonequilibrium
thermodynamics. However, a major question that still remains is the determination
of the best driving forces and assumptions to be made for drying model formulation.
Another concern should be the determination of the coefficients and parameters used
in the model. The measurement or determination of the necessary coefficients should
be feasible and practical for general applicability of a drying model.
The research described here was directed towards developing a predictive math-
ematical model of jalapeño pepper drying and thermal damage, due to the economic
importance of this commodity, as well as its potential commercialization value as a
processed product.

Fresh green jalapeño peppers (Capsicum annuum L.) obtained from local markets
were used for the experiments. They were selected manually in order to obtain
peppers in good condition of uniform size (6–7 cm), and then sliced to an approx-
imate thickness of 5 mm using an electrical cutting machine (S.A. Bertuzzi; Brugh-
erio, Milano, Italy). The jalapeño slices were washed to remove seeds and allowed
to drain for 10 min. Samples of 180 g were placed over nine trays of a locally
manufactured dryer, diagrammatically illustrated in Figure 11.1. Air was heated by
a gas burner model HP225B LP (Adams Manufacturing Company; Cleveland, OH)
and directed in parallel direction towards the peppers at 5 m/sec and temperatures
of 60, 70, and 80°C. The drying time was 150 min. Dry bulb temperatures were
recorded using thermometers located at different positions, as shown in Figure 11.1.
Air velocity was measured using a Pitot tube (Dwyer Instruments, Inc.; Michigan
City, IN) connected to a differential inclined manometer according to ASTM (1995)
norm D3154. Moisture changes were determined by weight difference according to
AOAC (1990) method 6.004. To determine a rehydration ratio, samples of 5 g dried
slices were immersed in 400 ml water baths. The water baths were set at 75°C, and
the immersion time was 6 min.

198 cm
Trays
Thermometers
Exhaust
206 cm
Air
valve
Burner
64 cm 83.5 cm 49.5 cm
FIGURE 11.1 Schematic diagram of the tray dryer used for the experiments.
The results obtained were used to derive drying and rehydration kinetics pre-
dictive models by means of regression analysis, using the Statistica 5.5 software
(StatSoft, Inc., Tulsa, OK).

In fundamental drying research of food materials, ideally a model would contain a
minimum of restrictive assumptions, and all material property values needed for the
model would be obtained. The prediction of the drying characteristics based on
knowledge of composition and structure is complex due to the nature of solid
structures and the limited understanding of the moisture transport mechanism. An
alternative is the identification of the relevant driving forces and the use of
independent experimental tests that isolate the different driving forces to determine
the necessary model coefficients. The model should have the most possible theo-
retical meaning and require the minimum of experimental tests to determine the
coefficients.
The model developed in this work was derived according to the characteristics
described above. Drying kinetics were determined and the data were handled in a
mathematical way to evaluate the best fitting equations describing the drying curves.
To achieve this, drying conditions had to be controlled very carefully to ensure
constant velocity, constant moisture content, and constant temperature of the flowing
air. When these conditions were set, it was assumed that the drying rate represented
by Equation (11.4) could also be established entirely in terms of the moisture gradient

between the sample and the surrounding drying air, i.e.,
dX R
= K y (X R − Xe ) (11.5)
dt
where XR is the moisture content on a dry basis of the vegetable, Ky is a coefficient

governing the mass transfer, and Xe is the moisture content of the air.
To give the model a generalized characteristic, the moisture content was nor-
malized using the following dimensionless relation:
XR − Xe
Θ= (11.6)
X0 − Xe
where X0 is the moisture content of the material at the initial time, i.e., t = 0.
It can be demonstrated (Molina-Corral, 1988) that Equation (11.5) can be rear-
ranged by incorporating the normalized moisture content described by Equation (11.6),
to give the following relationship:
d  XR − Xe   X − Xe 
  = Ky  R  (11.7)
dt  X 0 − X e   X0 − Xe 
The normalized moisture content Θ can be made explicit and transposed to give:
dΘ
= K y dt (11.8)
Θ
Integrating Equation (11.8), the following relationship is therefore obtained:
ln Θ = K y t + C (11.9)
where C is the integration constant.

Taking natural logarithms on both sides of Equation (11.9) transforms it into
the following exponential expression:
K y +C
Θ=e (11.10)
Using logarithm’s laws it can be demonstrated (Molina-Corral, 1988) that Equation

(11.10) simply becomes the one presented below, which relates the variation of
moisture content of the material Θ as a function of time t and temperature T, i.e.,
Kyt
Θ=e (11.11)

TABLE 11.1
Regression Parameter Values for the
Dehydration and Rehydration Models
from Experimental Data
Parameter Dehydration Model Rehydration Model
−1 −2
β1 5.209 × 10 −7.3340 × 10
−2 −5
β2 3.730 × 10 1.6000 × 10
−2 −3
β3 1.550 × 10 2.5004 × 10
β4 0.0 0.0
−4 −5
β5 1.000 × 10 −2.4360 × 10
−4
β6 6.000 × 10 0.0
Equation (11.11) represents a one-exponential model known as the thin film

drying model. Such a model basically states that the drying constant, Ky in this case,
is a combination of the transport properties involved in drying and describes with
reasonable accuracy the drying kinetics of hygroscopic materials. When the previ-
ously mentioned constant conditions of velocity, moisture, and temperature of the
drying air are ensured, the transport properties most influential in drying of vegeta-
bles are time and temperature. The correlation exercises practiced in accordance
with the experimental data demonstrated that the best fitting model for the coefficient
governing the mass transfer Ky was a quadratic one expressed as:
K y = β1 + β2 t + β3T + β 4 t 2 + β5T 2 + β6 tT (11.12)
where the parameters β1, β2,…, β6 are those presented in Table 11.1.
The model for predicting moisture content as a function of time and temperature
was therefore given by:
2
+β5T 2 +β6 tT ) t
Θ = e(β1 +β2 t +β3T +β4t (11.13)
Figure 11.2 shows the experimental drying curves contrasted with the corre-
spondinc correspondent ones obtained using Equation (11.13) above at the three
temperatures tested. As can be seen, the mathematical model fit the experimental
2
data very well, judging by the high given values of the coefficient of determination R .
As stated earlier, moisture migration by diffusion is the predominant mass transfer
mechanism in drying of fruits and vegetables. It has also been reported (Toledo, 1991)
that diffusivity may be constant if cells do not collapse and pack together. This behavior
would be identified in firm solids such as grains, or in high moisture products such as
fruits and vegetables when physical changes such as water removal are minimal. As
shown in Figure 11.3, the presence of only a falling rate period for all the conditions
tested was confirmed. This trend was in agreement with the work reported by Turhan

1
0.8
0.6
S = 0.023
0.4
R2 = 0.99
0.2
0
0 30 60 90 120 150
(a)
0.8
Moisture content
0.6
S = 0.031
0.4
R2 = 0.99
0.2
0
0 30 60 90 120 150
(b)
0.8
0.6
0.4 S = 0.020
R2 = 0.99
0.2
0
0 30 60 90 120 150
(c)
Time (minutes)
FIGURE 11.2 Experimental (䉱) and calculated (—) drying curves for 60 (A), 70 (B), and
80°C (C) dehydration temperatures.

1.6
1.4
1.2
1
0.8
0.6
0.4
0.2
0
0 0.2 0.4 0.6 0.8 1
(a)
2
Drying rate (kg/h·m2)
1.5
0.5
0
0 0.2 0.4 0.6 0.8 1
(b)
2.4
1.6
1.2
0.8
0.4
0
0 0.2 0.4 0.6 0.8 1
(c)
Moisture content
FIGURE 11.3 Experimental drying rate curves for 60 (A), 70 (B), and 80°C (C) dehydration
temperatures.
and Turhan (1997), who found that peppers dehydrated without previous blanching
presented only a falling rate period in their drying kinetics.
The drying curves presented in Figure 11.2 also show the difference in drying
velocities according to the applied temperature. It can be observed that drying

kinetics were higher, with a similar trend, for the processes carried out at 70 and
80°C, but slower for the minimum temperature of 60°C. Thus, it can be argued that
drying kinetics were optimal at any of the higher temperatures, and that these levels
of heat were moderate enough to prevent undesirable phenomena such as case
hardening. It has been observed that in drying of some fruits, vegetables, meat, and
fish, as drying temperatures approach the water boiling range, a hard and imperme-
able film develops on the surface (Brennan et al., 1979). Case hardening can be more
severe during final stages of drying, where more than one falling rate period is
presented. Since there was only one falling rate period in this study, case hardening
was not a problem and drying kinetics developed quite well. However, as more
undesirable phenomena can be caused by high drying temperatures, it would be
advisable to use 70°C as the dehydration processing temperature in further applica-
tions, as drying behavior was similar at either 70 or 80°C.
In addition to case hardening, shrinkage and texture damage can be caused by
drying of vegetables, resulting in poor appearance and loss of some sensory
attributes. The amount of thermal damage in drying of vegetables is difficult to
evaluate, but it may be related in some way to structural alteration of the tissues due
to excessive heat. The degree to which a dehydrated sample will rehydrate is influ-
enced by such structural and chemical changes. Rehydration is maximized when
cellular and structural disruption is minimized. Several measures can be taken to
minimize structural alterations in order to improve the reconstitutability of dried
food products. The drying method and adjustment of drying conditions can result
in a product with good rehydration properties. For example, it has been reported
that freeze-drying causes fewer structural changes than any other method, with
minimal changes to the product’s hydrophilic properties (Heldman and Singh, 1981).
This procedure results in obtaining food pieces with an open pore structure that will
absorb water easily when reconstituted. However, freeze-drying is an expensive form
of dehydration for foods due to the slowness of the drying rate and the use of vacuum.
Since the vapor pressure of ice is very small, freeze-drying requires very low
pressures or very high vacuum.
For this reason, it is more feasible to try to obtain food products with good recon-
stitution properties by manipulating the operating variables of dryers. One possibility
is to partially dehydrate fruits by immersion in sugar solutions to promote water migra-
tion by osmotic pressure difference, then give them a gentle drying cycle in order to
obtain crisp products that rehydrate easily (Beltrán-Reyes et al., 1996). Also, the blanch-
ing method and drying temperatures can have an effect on reconstitution properties of
vegetables (Ortega-Rivas et al., 1997).
In this work, the amount of damage produced by the different drying conditions
was determined by estimating the rehydration ratio RR using the following relation:
w0
RR = (11.14)
wf
where w0 is the weight of the dry sample and wf is the weight of the rehydrated
sample.

1
0.9
60°C
Rehydration relation
0.8
0.7 70°C
0.6
0.5 80°C
0.4
0.3
0.2
0.1
0
0 20 40 60 80 100 120 140
Drying time (minutes)
FIGURE 11.4 Experimental rehydration curves.
Rehydration rates, estimated by Equation (11.14), are shown in Figure 11.4. The
best fitting model for the rehydration ratio, obtained using a procedure similar to
that in deriving Equation (11.13), was:
2
+β5T 2 +β6 tT ) t
RR = e(β1 +β2 t +β3T +β4t (11.15)
The parameters β1, β2,…, β6 are given in Table 11.1.

As can be observed in Figure 11.4, rehydration kinetics showed a trend opposite
to that of the drying process, i.e., the dried peppers rehydrated better at the lower
drying temperature and at the shorter treatment times. In general terms, the worst
rehydration characteristics were demonstrated by the peppers dried at 80°C. This
behavior could be due to the extent of tissue damage, which is expected to be more
severe at higher drying temperatures. It has been reported (Charm, 1971) that
excessive thermal damage, due to high drying temperatures, may be responsible for
poor appearance and loss of texture of dehydrated biological materials.
11.4 CONCLUSIONS
A mathematical model to describe dehydration of jalapeño pepper at normal oper-
ating conditions was developed. The model describes the drying process in terms
of the moisture migration as a function of time at different temperatures. The effect
of thermal damage as a function of rehydration capacity is also included. The
regression equations describing the model were highly correlated. The model can
be used to opt for the best compromise between drying capability and product quality.
Application of the model to a material similar to the one tested in the experiments
would indicate that the use of relatively high temperatures would make a product
practically bone dry, but with irreversible thermal damage, as its capacity to absorb
water in a reconstitution process would be impaired. A moderate drying temperature,
on the other hand, would result in a product with low moisture content and appropriate
rehydration properties. Since the model development was based on careful experimental

conditions and the use of fresh materials of random composition, it can be applied
with confidence to conditions different from those used at the University of Chihuahua.
The model is easy to adapt, and simple calculations could provide guidance in choosing
processing times and temperatures in advance as a function of the expected properties
of the product, avoiding waste of time, energy, and raw materials.
NOMENCLATURE
2
A Drying surface area, m
β Parameter of the regression model
C Integration constant
Fs Weight of dry solids, kg
Θ Normalized moisture content
2
Ky Coefficient governing the mass transfer, kg mol/sec m
2
R Rate of drying, kg water/h m
RR Rehydration relation
t Time, min
T Temperature, °C
w0 Weight of dry sample, g
wf Weight of rehydrated sample, g
Wt Total weight of wet material, kg
X Free moisture content, kg water/kg dry solid
Xe Moisture content of the air, kg water/kg dry air
Xeq Equilibrium moisture content, kg water/kg dry solid
XR Moisture content of vegetable, kg water/kg dry solid
Xt Total moisture content, kg water/kg dry solid
X0 Initial moisture content, kg water/kg dry solid
ACKNOWLEDGMENTS
The authors thank the National Council for Science and Technology (CONACyT)
as well as the Program for Academics Improvement (PROMEP), México, for pro-
viding funding to the project.
REFERENCES
ASTM, Standard test method for average velocity in a duct (Pitot tube method), Annual Book
of ASTM Standards, Vol 11.03, 1995, pp. 89–92.
Beltrán-Reyes, B., Ortega-Rivas, E., and Anzaldúa-Morales, A., Characterization of reconsti-
tuted apple paste in terms of rehydration and firmness, Food Sci. Technol. Int., 2,
307–313, 1996.
Brennan, J.G., Food Dehydration: A Dictionary and Guide, Butterworth-Heinemann, Stone-
ham, MA, 1994.

Brennan J.G., Butters, J.R., Cowell, N.D., and Lilly, A.E.V., Food Engineering Operations,
2nd ed., Applied Science, London, 1979.
Charm, S.E., The Fundamentals of Food Engineering, 2nd ed., AVI, Westport, CT, 1971.
Geankoplis, C.J., Transport Processes and Unit Operations, Allyn and Bacon, Boston, MA,
1983.
Heldman, D.R. and Singh, R.P., Food Process Engineering, Van Nostrand Reinhold, New
York, 1981.
Molina-Corral, F.J., Development of a Mathematical Model of Jalapeño Pepper Drying in a
Tray Dehydrator with Gas Heating Source, thesis, University of Chihuahua, México,
1988.
Ortega-Rivas, E., Moreno-Pérez, L.F., and Gasson-Lara, J.H., Effect of blanching and drying
temperatures on rehydration rate and texture of sweet potatoes, in Advances in Food
Engineering, Narsimhan, G., Okos, M.R., and Lombardo, S., Eds., Purdue Research
Foundation, West Lafayette, IN, 1997, pp. 81–85.
Sarvacos, G.D. and Charm, S.E., A study of the mechanism of fruits and vegetables dehy-
dration, Food Technol., 16, 78–81, 1962.
Toei, R., Drying mechanism of capillary porous bodies, in Advances in Drying, vol. 2,
Mujumdar, A.S., Ed., Hemisphere, New York, 1983.
Toledo, R.T., Fundamentals of Food Process Engineering, 2nd ed., Van Nostrand Reinhold,
New York, 1991.
Turhan, M. and Turhan, K.N., Drying kinetics of red pepper, J. Food Process. Preserv., 21,
209–223, 1997.

Application of an
12 Artificial Neural Network
for Moisture Transfer
Prediction Considering
Shrinkage during Drying
of Foodstuffs
J.A. Hernández-Pérez, M.A. Garcia-Alvarado,
G. Trystram, and B. Heyd
CONTENTS
12.1 Introduction
12.2.1 Neural Network Systems
12.2.2 Learning Algorithm
12.2.3 Database Preparation
12.3.1 Learning Bases of the Model
12.3.2 Validation of the Proposed Model
12.4 Conclusions
Nomenclature
References
12.1 INTRODUCTION
Air drying is an essential activity in food processing industries. On-line state esti-
mation and control of the air drying operation require the mathematical description
of food moisture evolution during the process.
The dynamics of the food drying process involve simultaneous heat and mass
transfer, where water is transferred by diffusion from the inside of food material
towards the air–food interface and from the interface to the air stream by convection;

heat is transferred by convection from the air to the air–food interface and by
conduction to the interior of the food (Balaban and Pigott, 1988; Karathanos et al.,
1990; Kiranoudis et al., 1993; Zogzas and Maroulis, 1996). This phenomenon has
been modeled with different levels of complexity; existing models do not permit
adequate control of the air drying process in industrial applications, mainly because
physical dynamic models (or detailed models), considering the complexity of the
process, usually result in coupled nonlinear differential equations with partial deriv-
atives, where numerical simulations require specialized software and are very time
consuming. It is important to mention that these detailed models are able to predict
within a wide range. The dynamic models can be simplified (Courtois et al., 1991;
Hernández et al., 2000), but these models cannot take into account the complexity
of the process, and some still contain ordinary nonlinear differential equations that
take too long to simulate for applications of control (Trelea et al., 1997b).
Empirical model representations approximate the drying kinetic by several line
segments (Daudin, 1982), high order polynomials (Techasena et al., 1992), neural
networks (Dornier et al., 1993), etc. These models have a narrower validity range
but require only a limited number of simple arithmetic operations for simulation
and can be easily incorporated in control software.
Shrinkage is an important factor in mathematical models of heat and mass transfer
for the prediction of food drying kinetics. Mulet (1994) tested models with different
levels of complexity, concluding that the main factor that must be considered in models
is product shrinkage. Models that take into account the shrinkage of the product are
models in which the volume is considered as a function of the content of moisture.
The shrinkage of biological products during drying is not perfectly homogeneous
(Ratti, 1994; Hernández, et al., 2000). It is interesting to mention that there is a
deviation of some predictions during food drying kinetics considering shrinkage at
lower moisture levels (Ψ < 0.05); this is due to the possible conclusion of the shrinkage
and the heterogeneous characteristics of the product that could be the product, and
this phenomenon’s behavior is typical for foodstuffs (Hernández et al., 2000).
The progress of neurobiology has allowed researchers to build mathematical
models of neurons to simulate neural behavior. Neural networks are recognized as
good tools for dynamic modeling and have been extensively studied since the
publication of the perceptron identification method (Rumelhart and Zipner, 1985).
The interest in such models lies in their modeling without any assumptions about
the nature of underlying mechanisms and in their ability to take into account non-
linearities and interactions between variables (Bishop, 1994). Recent results establish
that it is always possible to identify a neural model based on the perceptron structure,
with only one hidden layer, for either steady state or dynamic operations (with
recurrent models) (Hornik et al., 1989; Hornik, 1993). An outstanding feature of neural
networks is the ability to learn the solution of the problem from a set of examples
and to provide a smooth and reasonable interpolation for new data. Also, in the
field of food process engineering, neural networks are a good alternative to conven-
tional empirical modeling based on polynomial and linear regressions. For food
processes, the neural computing application keeps on growing (Linko and Zhu, 1992;
Huang and Mujamdar, 1993; Zhu et al., 1996; Linko et al., 1997; Trelea et al., 1997a;
Hernández-Pérez et al., 2000).

The aim of the present work was to test the ability of neural networks to model
and predict moisture transfer during air drying in foodstuffs. The model was validated
with experimental drying data of cassava parallelepipeds and mango slices.

12.2.1 NEURAL NETWORK SYSTEMS
Neural networks are composed of simple elements operating in parallel. As in nature,
the network function is determined largely by the connections between elements
(neurons); each connection between two neurons has a weight coefficient attached
to it. A neuron is grouped into distinct layers and interconnected according to a
given architecture. The standard network structure for function approximation is the
multiple layer perceptron (or feedforward network). The feedforward network often
has one or more hidden layers of sigmoid neurons followed by an output layer of
linear neurons. Multiple layers of neurons with nonlinear transfer functions allow
the network to learn nonlinear and linear relationships between input and output
vectors. The linear output layer lets the network produce values outside the range
–1 to +1 (Demuth and Beale, 1998; Limin, 1994). For multiple layer networks, we
use the number of layers to determine the superscript on the weight matrices. The
appropriate notation is used in two-layer networks. A simple view of network
structure and behavior is given in Figure 12.1. This network can be used as a general
function approximator. It can approximate any function with a finite number of
discontinuities, arbitrarily well, given sufficient neurons in the hidden layer.
The numbers of neurons in the input and output layers are given by the number
of input and output variables in the process under investigation. In this work, the
input layer consisted of five variables in the process (air temperature, air velocity,
IW1{1,1}
In1 Σ n1
LW2 {2,1}
In2 Σ n2
Σ Out
In k Σ ns
b1 b2
Input layer Hidden layer Output layer
FIGURE 12.1 The neural network computational model. k = number of inputs, In = inputs,
Out = output, thick lines = weights and biases.

shrinkage function of the moisture, time, and air humidity), one for each input. The
optimal number of neurons in the hidden layer(s) ns is difficult to specify and depends
on the type and complexity of the task; this is usually determined by trial and error.
Each neuron in the hidden layer has a bias b, which is added with the weighted
inputs to form the neuron input n. This sum, n, is the argument of the transfer
function f.
n = IW{1,1}In1 + IW{1,2}In2 + ··· + IW{1, k}Ink + b
The coefficients associated with the hidden layer are grouped into matrices IW1
(weights) and b1 (biases). The output layer contains one variable (moisture of the
product) for mango and cassava, respectively, which computes the weighted sum of
the signals provided by the hidden layer; the associated coefficients are grouped into
matrices LW2 and b2. Using the matrix notation, the network output can be given
by Equation (12.1).
2 1
Out = f (LW2f (IW1*In + b1) + b2) (12.1)
Hidden layer neurons may use any differentiable transfer function to generate their
1 2
output. In this work we used as f Tan-Sigmoid Function and for f Linear Transfer
Function. The number of network coefficients (weights and biases) is given by
Equation (12.2).
m = n(In + 1) + Out(n + 1) (12.2)
12.2.2 LEARNING ALGORITHM

A learning algorithm is defined as a procedure that adjusts the coefficients (weights
and biases) of a network in order to minimize an error function (usually a quadratic
one) between the network outputs for a given set of inputs and the correct outputs
already known (this procedure may also be referred to as a training algorithm). If
smooth nonlinearities are used, the gradient of the error function can be easily
computed by the classical backpropagation procedure (Rumelhart et al., 1986). Pre-
vious learning algorithms used this gradient directly in a steepest descent optimiza-
tion, but recent results have shown that second order methods are far more effective.
In this work, the Levenberg–Marquardt (trainlm), optimization procedure in the
Neural Network Toolbox of Matlab (Demuth and Beale, 1998) was used. The
algorithm of Levenberg is an approximation of Newton’s methods; this algorithm
was designed to approach second order training speed without having to compute
the Hessian matrix (Hagan and Menhaj, 1994). Despite the fact that computations
involved in each iteration are more complex than in the steepest descent case, the
convergence is faster, typically by a factor of 100. The root mean square error
(RMSE) between the experimental values and network predictions was used as a
criterion of model adequacy, as shown in Figure 12.2.

Xa
t
Lv
Process Ψ
Va
T°C
+
Optimization Method
RMSE (Levenberg-Marquardt)
Shrinkage +
-
Neural
Network
(weights and bias) Ψ̂
FIGURE 12.2 Recurrent network architecture for the drying kinetic considering the shrinkage
of the product and procedure used for learning of neural network.
12.2.3 DATABASE PREPARATION

Experimental data provided by Hernández et al. (2000), consisting of mass transfer
kinetics of mango slices, 4 × 4 cm with three slab thicknesses (0.50, 0.75, and 1.0
cm), and cassava parallelepipeds, 10 cm long with three thicknesses (1.0, 2.0, and
3.0 cm), were used. The experimental drying kinetics were carried out at three
different air temperatures and air velocities with a time of 10 h for each kinetic. The
arrangement was a 3*3*3 (slab thickness * air temperature * air velocity) complete
factorial design for mango and 3*3 (thickness * air temperature) complete factorial
design for cassava at constant air velocity, with two replicates. Tables 12.1 and 12.2
give the experimental conditions studied for each kinetic of mango and cassava.
Eperimental files were split into learning and test databases. The inputs of the
network were air temperature (T), air velocity (Va), shrinkage (Lv), time (t), and air
humidity (Xa); the output of the network was the food moisture content in dimen-
sionless form (Ψ̂) for mango. The same network was used for cassava but without
the input (Va). The food moisture evolution during drying was calculated by sample
weight loss of the product at times t = 0, 0.25, 0.50, 0.75, 1.0, 1.25, 1.50, 1.75, 2.0,
2.5, 3.0, 3.5, 4.0, 5.0, 6.0, 7.0, 8.0, 9.0, and 10.0 h. Wet and dry bulb temperatures
of the ambient air were measured with glass thermometers to estimate the air
moisture content (Xa).
Equation (12.3) was used to determine the variation of shrinkage during kinetic
drying of mango and cassava, as proposed by Hernández et al. (2000). This equation

TABLE 12.1
Experimental Conditions Studied for Mango
File Initial Thickness Air Temperature Air Velocity Time
Number Lo (cm) T (°C) Va (m/sec) t (h)
M1 0.5 50 0.5 0–10

M2 0.75 50 0.5 0–10
M3 1.0 50 0.5 0–10
M4 0.5 60 0.5 0–10
M5 0.75 60 0.5 0–10
M6 1.0 60 0.5 0–10
M7 0.5 70 0.5 0–10
M8 0.75 70 0.5 0–10
M9 1.0 70 0.5 0–10
M10 0.5 50 1.75 0–10
M11 0.75 50 1.75 0–10
M12 1.0 50 1.75 0–10
M13 0.5 60 1.75 0–10
M14 0.75 60 1.75 0–10
M15 1.0 60 1.75 0–10
M16 0.5 70 1.75 0–10
M17 0.75 70 1.75 0–10
M18 1.0 70 1.75 0–10
M19 0.5 50 3 0–10
M20 0.75 50 3 0–10
M21 1.0 50 3 0–10
M22 0.5 60 3 0–10
M23 0.75 60 3 0–10
M24 1.0 60 3 0–10
M25 0.5 70 3 0–10
M26 0.75 70 3 0–10
M27 1.0 70 3 0–10
is a function of moisture content of the product.
  X 
Lv = L 0 ∆L f + (1 − ∆L f )   (12.3)
  X 0  
where Lv represents the thickness (cm), L0 is the initial thickness (cm), ∆Lf repre-
sents the fraction of initial slab thickness at the end of drying (∆Lf = 0.55 for mango
and ∆Lf = 0.68 for cassava), and X and X0 are the moisture and initial moisture of
the product (g water/g dry matter). The selected experimental files were split into
learning and test databases to obtain a good representation of the situation diversity.
In each case:

TABLE 12.2
Experimental Conditions Studied for Cassava
File Initial Thickness Air Temperature Air Velocity Time
Number Lo (cm) T (°C) Va (m/sec) t (h)
C1 1 50 3 0–10
C2 1 60 3 0–10
C3 1 70 3 0–10
C4 2 50 3 0–10
C5 2 60 3 0–10
C6 2 70 3 0–10
C7 3 50 3 0–10
C8 3 60 3 0–10
C9 3 70 3 0–10
Mango
Eighteen experimental kinetics in learning database (M1, M3, M5, M6,
M7, M8, M10, M11, M14, M15, M16, M18, M20, M21, M22, M23,
M25, and M27)
Nine experimental kinetics in test database (M2, M4, M9, M12, M13,
M17, M19, M24, and M26)
Cassava
Six experimental kinetics in learning database (C1, C2, C4, C6, C8, and C9)
Three experimental kinetics in test database (C3, C5 and C7)
The learning database was obtained to optimize the neural network, and the test
database was reserved for the validation of the predictive capability of the model.

The proposed model for mango (Equation (12.4)) involved three neurons ns = 3 in
the hidden layer (18 weights and 4 bias) to determine the moisture transfer in a
dimensionless form. The same model, but without the input of air velocity (Va), was
used for cassava (15 weights and 4 bias). This model includes the effect of shrinkage
(Lv) as a function of the last moisture content. It is important to mention that the
mango slices were dried on one side, and cassava parallelepipeds were suspended
so drying took place on the four sides (two dimensions). The parallelepipeds were
of the same size and drying was homogeneous on the four sides, so we used as input
one only Lv for mango and cassava.
Ψ̂ represents the predicted moisture of the product in dimensionless form; Xe
is the moisture in equilibrium (g water/g dry matter). This moisture (Xe) was deter-
mined using the relationship of air moisture and the sorption isotherms that were exp-
erimentally obtained for mango and cassava in the laboratory (Equations (12.5) and
(12.6)). The moisture levels (X/X0) of Equation (12.3) were determined for the last output
network, which makes one closed boucle for (Lv), as represented in Equation (12.4).

X
Lv = L 0 ∆L f + (1 − ∆L f )
X0
T°
V
(12.4)
L (X − Xe )
Ψ̂ = (Xo − Xe )
t
X
bia
Mango: aw = 1 – exp[–exp(0.9154 + 0.5639lnX)] (12.5)
Cassava: aw = 1 – exp[–exp(–44.8 + 8.66lnT – 6.41lnX

−5 2
+ 0.049TlnX – 6.7 × 10 T lnX)] (12.6)
12.3.1 LEARNING BASES OF THE MODEL

Figure 12.3 gives the trial root mean square error (RSME) against the iteration
number in the case of mango and cassava, for one to six neurons in the hidden layer.
These results showed that the typical learning error decreased when the number of
neurons in the hidden layer increased, but for three or more neurons in the hidden
layer for mango, and two or more neurons for cassava, respectively, an additional
increase in structure complexity did not strongly decrease the RSME.
One problem that occurs during neural network training feedforward is called
over-fitting. The RSME on the training set is driven to a very small value, but when
new data are presented (e.g., test database) to the network, the RSME is large.
Therefore, the RSME on the test database is a good criterion to optimize the number
of iterations and avoid over-fitting. Figure 12.3 shows that for three (RMSE =
0.001408) or four (RMSE = 0.001323) neurons in the hidden layer, the error is
very small for mango, whereas for cassava the same error is obtained with two
(RMSE = 0.00149) or three (RMSE = 0.00148) neurons. In order to determine
the number of neurons in the hidden layer, we plotted the RMSE (learning and
test bases) against the number of neurons, as shown in Figure 12.4. This figure
presents over-fitting because the error on the test database can increase with the
number of neurons. The optimal number of neurons in the hidden layer is three for
both mango and cassava.
Figure 12.5 presents the simulated results against experimental data for test and
learning bases of mango and cassava; in all cases the prediction was correct, whatever
the level of moisture. However, at lower moisture contents an evident deviation
between experimental and simulated data was observed for mango. In order to
confirm these deviations, a plot of some drying experimental and predicted kinetics

1
10
- one neuron -- two neurons -. three neurons
0
10 .. four neurons - - five neurons -o- six neurons
Root-mean square error training

-1
10 MANGO
-2
10
-3
10
-4
10
0 20 40 60 80 100
Levenberg-Marquardt
1
10
- one neuron -- two neurons -. three neurons
0
Root-mean square error training
10 .. four neurons - - five neurons -o- six neurons
-1
10
CASSAVA
-2
10
-3
10
0 20 40 60 80 100
Levenberg-Marquardt
FIGURE 12.3 Test root mean square error (RMSE) vs. number of iterations and various
numbers of hidden neurons for mango and cassava.
(experimental M25, M27, C2, C8; see drying conditions in Tables 12.1 and 12.2) are
presented in semilog scale in Figure 12.6. This figure shows that at Ψ < 0.05 the
model cannot predict the drying curves. These deviations at lower moisture content
are also observed with detailed models (Hernández et al., 2000).

10-1
MANGO
-o- Learn
Root-mean square error

-2
10 - - Test
10-3
10-4
1 2 3 4 5 6
Number of neurons
10-1
CASSAVA
Root-mean square error
-o- Learn
- - Test
-2
10
10-3
1 2 3 4 5 6
Number of neurons
FIGURE 12.4 Comparison of RSME learn and test vs. the number of neurons in the two
cases (mango and cassava).
12.3.2 VALIDATION OF THE PROPOSED MODEL

Figure 12.7 depicts the ability of the models to predict drying kinetics at different
thicknesses, temperature, and air velocities in the experimental domain. This figure
shows some simulated results generated and experimental data obtained by the test
database (M4, M12, M26, C3, C5, and C7; see Tables 12.1 and 12.2). It is evident that

1
0.9 learn Mango
0.8 o test
0.7
0.6
Simulated
0.5
0.4
0.3
y = 0.0101 + 0.9838x
0.2 R=1
0.1
0
0 0.2 0.4 0.6 0.8 1
Experimental
0.9 learn
0.8 o test
0.7
0.6
Simulated
0.5 Cassava
0.4
y = 0.0144 + 0.9763x
0.3
0.2 R=1
0.1
0
0 0.2 0.4 0.6 0.8 1
Experimental
FIGURE 12.5 Simulated vs. experimental data for test and learning bases of mango and
cassava.
the model was successful in predicting the experimental drying kinetics, showing
the importance of the artificial neural network to simulate the drying curves of
foodstuffs. These models are not complex, and they can be used for on-line estima-
tion of air drying processes in industrial applications.
10 0
Mango
PSI = (X–Xe)/(Xo–Xe)
10 -1
T = 70°C
10 -2 o Lvo = 0.5 cm (M25)

* Lvo = 1 cm (M27)
- Predict
0 2 4 6 8 10
Time (hr)
0
10
-1 Cassava
10
T = 60°C
-2
10
o Lvo = 1.0 cm (C2)

* Lvo = 3.0 cm (C8)
-3 - Predict
10
0 2 4 6 8 10
Time (hr)
FIGURE 12.6 Experimental data and predicted results of the learning bases for mango and
cassava.
12.4 CONCLUSIONS
This study shows that neural network modeling can be used to obtain accurate sim-
ulation of the moisture transfer during food drying over a wide experimental range.
This neural network modeling was validated with experimental drying data. Tech-
nological interest in this kind of modeling must be related to the fact that it is
elaborated without any preliminary assumptions about the underlying mechanisms,
and also to its implementation facility and speed of simulation. The applications of

1
* Lvo = 0.5 cm T = 60°C Va = 0.5 m/sec
0.9 + Lvo = 1 cm T = 50°C Va = 1.75 m/sec
o Lvo = 0.75 cm T = 70°C Va = 3m/sec
0.8
- Prediction
0.7
0.6
0.5
0.4
0.3
0.2
Mango
0.1
0
0 2 4 6 8 10
Time (hr)
1 * Lvo = 1 cm T = 70°C Va = 3 m/s

0.9 + Lvo = 2 cm T = 60°C Va = 3 m/s
o Lvo = 3 cm T = 50°C Va = 3m/s
0.8 - Prediction
0.7
0.6
0.5
0.4
0.3
Cassava
0.2
0.1
0
0 2 4 6 8 10
Time (hr)
FIGURE 12.7 Experimental data and simulated curves generated with the proposed model
in the drying kinetics of mango and cassava. The symbols represent experimental moisture
evolution at different conditions.
artificial neural networks can be used for on-line state estimation and control of
drying processes.
NOMENCLATURE
k Number of input
In Input variables

Out Output variables
ns, n Neuron in the hidden layer
IW1, LW2 Matrix weight
b1, b2 Matrix bias
T Air temperature (°C)
Va Air velocity (m/sec)
Lv Thickness (cm)
L0 Initial thickness (cm)
t Time (h)
Xa Air moisture content (g water/g dry air)
X, X0 and Xe Food moisture content: in each time, initial, and in equilibrium,
respectively (g water/g dry matter)
aw Food water activity
GREEK SYMBOLS
Ψ, Ψ̂ Dimensionless variables (experimental and predicted moisture)
∆Lf Fraction of the initial characteristic length at the end of drying period (cm)
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Modeling of Prato
13 Cheese Salting: Fickian
and Neural Network
Approaches
A.F. Baroni, M.R. Menezes, E.A.A. Adell,
and E.P. Ribeiro
CONTENTS
13.1 Introduction
13.1.1 Mass Transfer Phenomena
13.1.2 Artificial Neural Networks
13.2.1 Cheese Processing
13.2.2 Cheese Sampling
13.2.3 Analytical Methods
13.3 Mathematical Modeling
13.3.1 Fickian Diffusion Model
13.3.2 Average Concentration
13.3.3 Neural Network Model
13.4.1 Cheese Composition
13.4.2 Salting Process
13.4.3 Performance of the Model Approaches
13.4.4 Statistical Analysis
13.4.5 Effective Diffusion Coefficients
13.5 Conclusions
Acknowledgments
References
13.1 INTRODUCTION
The production of cheese in Brazil is quite recent, having been consolidated from
an industrial standpoint in the beginning of the twentieth century, especially after
the arrival of Danish and Dutch immigrants in the state of Minas Gerais in 1920

(Furtado, 1991). Prato cheese holds a leading position in Brazilian production with
57,758 tons produced yearly. Within the universe of Brazilian cheese, Prato has the
highest technological standardization; it is the best characterized commercial cheese
(Oliveira, 1986; Ribeiro, 1996).
The expected average composition of ripened Prato cheese is 42 to 44% moisture,
26 to 29% fat, pH ranging from 5.2 to 5.4, and salt concentration 1.6 to 1.9%
(Furtado and Neto, 1994). Schiftan and Komatsu (1980) carried out experiments on
50 commercial Prato cheese samples and obtained average values of 40% moisture,
47.5% fat in the dry matter, 1.7% salt, and 3.5% ash. Furtado and Wolfschoon-
Pombo (1979) reported the average composition of Prato cheese as 53.0 to 59.2%
dry matter, 40.8 to 47.0% moisture, 25.3 to 30.5% fat and 47.7 to 51.5% fat in the
dry matter.
13.1.1 MASS TRANSFER PHENOMENA

Salting is one of the main steps of cheese production; thus, salt concentration
distribution is an important parameter affecting cheese quality and acceptability.
Salting plays a number of important roles in cheese, such as controlling the bio-
chemistry of cheese ripening and the water activity of young cheeses. Salting affects
the growth and survival of bacteria and the activity of cheese enzymes. Nowadays,
brine salting is the most widely used salting technique in the Brazilian cheese
industry. It is performed in an empirical way, and many times the distribution of the
salt in the final product is irregular. Salt is absorbed and penetrates into the cheese,
while an outer flux of water takes place. The amount of salt retained and water
removal by the cheese depend, mostly, on brine concentration and brining time
(Furtado and Neto, 1994).
Fick’s law of diffusion is usually used to represent mass changes during brine
salting of cheese. However, simplifications imposed on the model may affect its
accuracy. Geurts et al. (1974) modeled the brine salting of Gouda cheese applying
Fick’s law of diffusion. They obtained one-dimensional data on salt concentration
and moisture profiles in cheese pieces, measured as a function of time. The authors
noticed that the effective diffusion coefficient of salt within the cheese was consid-
erably lower than in free solution, due to factors such as tortuosity, viscosity, and
matrix restriction effects. However, Fick’s first law was not able to describe moisture
flux during the brining step. An empirical linear relationship between water content
and salt concentration was applied, resulting in a coefficient of proportionality of
the dewatering process. Guinee and Fox (1983, 1987) found similar results for water
and salt diffusion in Romano-type cheese. The same authors published a compre-
hensive review of salt and moisture diffusion of various cheeses in 1987. Luna and
Chavez (1992) and Turhan and Kaletunç (1992) also investigated water movement
during brine salting of cheese. Payne and Morison (1999) used a Maxwell–Stefan
multi-component approach to model salt and water diffusion in cheese based on
published data. This refined approach, taking into account diffusive interactions
among salt, water, and cheese matrix, still requires a large number of assumptions
during the modeling.

13.1.2 ARTIFICIAL NEURAL NETWORKS
Artificial neural networks (ANNs) have been of interest because they enable direct
modeling of nonlinear processes without requiring a prespecified detailed relation-
ship. ANNs have been increasingly used in food and chemical engineering for several
purposes. They have been applied recently in the prediction of quality attributes in
beef (Park et al., 1994), the snack frying process (Huang et al., 1998b), and cheddar
cheese (Muir et al., 1997); improvement of control loops in food processing (Huang
et al., 1998a; Benne et al., 2000); classification problems, such as classification of
beef (Park et al., 1994); and prediction of protein functionality (Arteaga and Nagai,
1993), moisture attained in a rehydration process of dried rice (Ramesh et al., 1996),
pressure drop of non-Newtonian fluids in tubes (Adhikari and Jindal, 2000), and
drying in a fluidized bed (Balasubramanian et al., 1996), among other applications.
Artificial neural networks consist of a large number of simple interconnected
nonlinear processing units (neurons) arranged in a layered structure, having adjust-
able connection weights. These weights are the internal parameters of the network.
The input neurons are connected to the output neurons through layers of hidden
nodes. Each neuron receives information in the form of inputs from other neurons
and processes it through some function, typically nonlinear, called the activation
function (Psichogios and Ungar, 1992). The general structure of a multilayered neural
network with one output is shown in Figure 13.1.
Due to the parallel structure and the ability to learn by adjusting the connection
weights, ANNs can handle nonlinear relationships where mathematical models are
not available without need of any previous knowledge on the relationships of the
process variables (Psichogios and Ungar, 1992; Balasubramanian et al., 1996; Park
et al., 1994; Adhikari and Jindal, 2000; Ramesh et al., 1996).
During the network learning procedure, weights are adjusted so that the intro-
duction of a set of inputs produces the desired set of outputs. The most widely used
neural network learning method is backpropagation. This method uses an iterative
gradient search technique to minimize a performance function, equal to the mean
Hidden 1
Input 1
.
.
.
Input n Output 1
.
1 .
.
Threshold Hidden n
value
Threshold 1
value
FIGURE 13.1 General structure of a multilayered neural network with one output.

difference between the desired and the actual network outputs (Psichogios and
Ungar, 1992). The neural network process model should have as few neurons in the
hidden layer as possible, respecting accuracy limitations (Huang et al., 1998b).
The aims of this work are to model mass transfer during brine salting of Prato
cheese by a traditional phenomenological model and an empirical approach and to
compare their results.

13.2.1 CHEESE PROCESSING
The cheese manufacturing trials were carried out in a dairy pilot plant of the
Chemistry and Food Engineering Department of the Mauá Institute of Technology.
In each experiment, 100 l of milk were used per cheese vat to produce twelve pieces
3
of cheese with a mean weight of 1.0 kg and dimensions of (11.5 × 5.5 × 5.5) cm each.
During the cheesemaking process, pasteurised, refrigerated whole milk was first
heated to 32°C in a cheese vat. It was then inoculated with 1% of Probat 8/12
WIESBY culture (composed of Lactococcus lactis subsp. lactis + L. lactis subsp.
cremoris + L. lactis subsp. lactis biovar. diacetilactis + Leuconostoc mesenteroides
subsp. cremoris), a calcium chloride solution (23 g/100 l of milk) was added, the
“urucum” coloring (10 ml/100 l of milk) was added, and calf rennet (WIESBY) was
added (2 g/100 l of milk). The curd was formed during approximately 35 min and
was cut to a size of ca. 0.8 to 1.0 cm. The temperature of the curd and whey mixture
was raised slowly and maintained at 40°C for 60 min. Whey was subsequently
drained, and the curd was placed in Prato hoops and held at room temperature (25°C)
throughout pressing (2 kg weights) for 4 h, during which the cheese pieces were
inverted five times, held (2 h), and then brined.
13.2.2 CHEESE SAMPLING

The cheese pieces were immersed in nonagitated brine solutions of 15, 20, and 25%
NaCl (w/w) at 10°C with a brine:cheese ratio of 2:1 (v/v). These are the usual
conditions for Brazilian Prato cheese manufacturing. At each sampling time (30, 60,
120, 240, 360, and 480 min), one sample was removed from the brine vessel. After
that, all samples and the control sample were divided into three regions: external,
intermediate, and internal, as shown in Figure 13.2. These samples, classified by
region, were weighed, ground, and kept at −10°C prior to chemical analysis.
Note that in Figure 13.2 only two cut directions are shown; the third is the same
as the vertical cut (B), once these two directions have the same dimensions (B = C =
5.5 cm).
13.2.3 ANALYTICAL METHODS

In the control cheese samples, acidity, fat content (Atherton and Newlander, 1981),
ash content, pH, total solids, and protein (AOAC, 1984) were analyzed. Salt content
and moisture of all ground samples were determined by the Volhard method (AOAC,
1984). Analytical assays were performed in triplicate.

External
Intermediate
Internal
B/6
B/6
B/3
y
B/6
z
B/6 C
A/6 A/6 A/3 A/6 A/6
x
FIGURE 13.2 Schematic representation of cheese cut.
13.3 MATHEMATICAL MODELING

13.3.1 FICKIAN DIFFUSION MODEL
Considering tridimensional unsteady state mass transfer, the phenomenon of Fickian
diffusion for rectangular geometry is described by the following equation:
∂C A  ∂2C A ∂2C A ∂2C A 

= Deff  + +  (13.1)
∂t  ∂x 2 ∂y 2 ∂z 2 
where CA is the salt concentration in cheese and Deff is the effective diffusivity.
It was assumed that the cheese was homogeneous, that brine concentration
remained constant during the experiments and was equal to the salt concentration
at cheese surfaces, and that no film resistance existed between the brine and cheese
faces. These assumptions correspond to an infinite Biot number and unity equilib-
rium distribution coefficient (K).
To solve Equation (13.1), it was necessary to apply the solution suggested by
Neumann (Crank, 1975), a product of the solutions of three plane sheets:
f (x, y, z, t) = Ψ (x,t)⋅ζ (y, t)⋅ϕ (z, t) (13.2)
The solution for a single plane sheet is given by:

∞
CA − C As  − Deff (2 n + 1)2 π 2 t 
∑ 8
= exp   (13.3)
C A0 − C As n=0
(2 n + 1)2 π 2  2a 2 
Initial condition:
t = 0, z > 0, CA = CA0
Boundary conditions:
t > 0, z = 0, CA = CAs
∂C A
t > 0, z = a, =0
∂z

where CA0 is the initial salt concentration in cheese, CAs is the salt concentration on
the cheese surface, n is the number of terms of the series, and 2a is the plane sheet
thickness size in directions x, y, and z.
Since all variables of Equation (13.3) are known except Deff, the effective diffu-

sivity (Deff) was obtained by a least squares estimation using Microsoft Excel (1997)
to fit experimental data, with 100 terms of the series considered.
13.3.2 AVERAGE CONCENTRATION

The proposed model predicted the average concentration of salt within cheese as a
function of time. It was calculated from experimental data measured at three regions
(internal, intermediate, and external) of the cheese piece; hence, one divided the
total experimental volume V in integrating volumes Vi representing each region of
cheese analyzed. The average concentration CA was calculated as follows:
∑C V i i
CA = i =1
(13.4)
V
13.3.3 NEURAL NETWORK MODEL

A neural network model was constructed using a multilayer perceptron architecture.
The network had two inputs, brining time and brine concentration, because these
variables have a greater effect than other process variables on salt diffusion, and one
output, average salt concentration in cheese.
The training algorithm used was the well-known backpropagation algorithm,
using the experimental data obtained, so as to minimize the differences between
desired and calculated values of average salt concentration in cheese.
Determination of the number of hidden neurons is commonly done empirically.
The procedure used to choose the structure of the artificial neural network was a
systematic trial and error procedure using two data sets (training and testing) in an
attempt to avoid overfitting and underfitting. A description of these phenomena can
be found elsewhere (Huang et al., 1998b; Arteaga and Nagai, 1993).
From the 21 vectors available, containing the two inputs and the output, 18 were
used to form the training set, while the remaining data formed the testing set. Data
were presented to training in a random manner in order to achieve a better training.
Error for comparison between structures was calculated by the sum of the squared
error between the value in the training or test set and the value calculated by the
ANNs.
The method for choosing the number of nodes in the hidden layer is presented
as follows (Zorzetto et al., 2000). Topology of the network was chosen initially to
have a large number of hidden nodes, i.e., 10 nodes. Training was carried out until
a minimum error for the test set was observed with this number of hidden nodes.
This step is shown in Figure 13.3.

5.0 0.25
training testing
4.0 0.2
Squared error - training
Squared error - testing

3.0 0.15
2.0 0.1
1.0 0.05
0.0 0
0 50 100 150 200 250
Number of iterations
FIGURE 13.3 Squared error for training and testing sets with 10 hidden nodes.
Brine time
Brine Average
concentration concentration
1
Threshold
value
Threshold 1
value
FIGURE 13.4 Neural network model for Prato cheese salting.
As can be observed from Figure 13.3, minimum squared error for the testing set
was reached with 100 iterations. Using the same number of iterations found in this
structure, i.e., 100 iterations, nodes in the hidden layer were gradually cut off, until
the smallest structure that could provide the same performance was reached.
Following this procedure, it was noticed that minimum error was reached using
10 nodes in the hidden layer. However, differences in the testing error among the
structures were not high. Thus, it was decided to use a smaller network with five
hidden nodes to accelerate the training procedure, while still having an admissible
error. From this analysis, the network topology used in this work is shown in
Figure 13.4.

13.4.1 CHEESE COMPOSITION
The average pH of Prato cheese before brine salting was 5.20 ± 0.01. Results of the
mean centesimal composition analysis are shown in Table 13.1.
13.4.2 SALTING PROCESS

It is important to evaluate the changes of salt concentration within the cheese during
the salting process to select the best operating conditions (especially salting time
and brine concentration). As presented in Figure 13.5, no influence of brine concen-
tration was observed in the internal portion of the cheese, but it is important to notice
that although the values of salt concentration increased with time, the amount of
salt permeated is almost null. However, at the intermediate position (Figure 13.6),
differences of about 75% can be observed after 240 min between 15 and 20–25%
NaCl. These variations become clear for the external region (Figure 13.7), where the
solution of 15% NaCl yielded a lower salt concentration for all time periods studied.
Nevertheless, no considerable differences between 20 and 25% NaCl were found
even in this position.
TABLE 13.1
Composition of Control Cheese Samples (%)
Average Standard Deviation
Moisture 48.3 0.4

Fat 27.2 0.2
Fat (dry matter) 52.6 0.4
Total protein 20.5 0.1
Ash 4.00 0.01
Internal
0.3
Salt Concentration (%)
15% NaCl
0.2
20% NaCl
25% NaCl
0.1
0
0 100 200 300 400 500 600
Time (min)
FIGURE 13.5 Salt concentration at the internal position.

Intermediate
0.3

0.2 15% NaCl
20% NaCl
0.1
25% NaCl
0.0
0 100 200 300 400 500 600
Time (min)
FIGURE 13.6 Salt concentration at the intermediate position.
External
4.0
3.0
15% NaCl
2.0 20% NaCl
25% NaCl
1.0
0.0
0 100 200 300 400 500 600
Time (min)
FIGURE 13.7 Salt concentration at the external position.
Since the initial moisture of cheese samples varied for each trial, normalized
values M /Mi (moisture wet basis/initial moisture) were plotted against time
(Figure 13.8). It is important to note the greater water loss of cheese treated with 25%
NaCl solution—more than 10% of the initial value—when compared to the other
solutions (maximum of 5% moisture loss).
It can be concluded that the concentration of 15% NaCl in the solution did not
provide a gradient of activity coefficient high enough to maintain a driving force
for efficient mass transfer between the sodium chloride in solution and the liquid
phase in cheese. Besides, Furtado (1991) reported that salt concentrations lower than
17% cause a smoothing of the Prato cheese skin, probably due to hydration of the
surface. As can be seen, the water loss of the cheese salted in 15% NaCl brine
solution was minimal, with a small moisture increase after 360 min.
However, as mentioned before, the increase of brine concentration from 20 to
25% NaCl did not raise the sodium chloride concentration within the cheese for all
studied conditions. This behavior can be explained by a greater outward water flux
of 25% NaCl solution when compared to 20% NaCl (Figure 13.8). This dewatering
could lead to the formation of a hard skin on the surface of the cheese, thus avoiding

1.00
0.98
0.95 15% NaCl
M / Mi
20% NaCl
0.93
25% NaCl
0.90
0.88
0 100 200 300 400 500 600
Time (min)
FIGURE 13.8 Normalized average moisture of cheese samples.
salt penetration. These assumptions agreed with the visual observation that the cheese
treated in 25% NaCl concentration showed small fissures on the cheese surface,
probably due to shrinkage leading to modifications of skin permeability.
13.4.3 PERFORMANCE OF THE MODEL APPROACHES

Figure 13.9 allows a general visualization of the performance of the models for
average salt concentration prediction at different brine salt concentrations. It can be
observed from these plots that the neural network model had a better adjustment to
the experimental data than Fick’s model did. Although experimental data did not
show the expected behavior from the theoretical analysis due to experimental errors
as shown in Figure 13.9(a), the neural network model had a good agreement with
these data. Hence, the neural model does not require information regarding the
understanding of the process, but on the other hand does not bring any additional
comprehension. Theoretical knowledge and analysis of data are of principal impor-
tance during the selection of training and testing data in order to avoid discrepancy
in the neural model.
Fick’s model did not present a good fit to the experimental data, probably due
to some model assumptions, especially concerning the unity equilibrium distribution
coefficient, since it used a nonagitated solution and a low solution:cheese ratio.
These factors could lead to a dilution of the solution with time and a varying
concentration at the cheese surface.
13.4.4 STATISTICAL ANALYSIS

One-way ANOVA (α = 0.01) tests were performed in order to detect significant
differences between experimental average salt concentrations and those predicted
2
by Fickian and neural models. The correlation index (R ) and the sum of squared
errors (SSE) between calculated and experimental data were also calculated.

3.0
1.2 2.5
Average Salt Concentration (%)

2.5
1.0
2
0.8 2.0
1.5
Exp 15%
0.6 Exp 20% 1.5
Neural 15% Exp 25%
1 Neural 20%
0.4 Neural 25%
Fick 15% Fick 20% 1.0
Fick 25%
0.2 0.5
0.5
0.0 0
0 100 200 300 400 500 600 0 100 200 300 400 500 600 0.0
0 100 200 300 400 500 600
Time (min)
Time Exp. Time Exp. Time Exp.

Fick SE F Neural SE N Fick SE F Neural SE N Fick SE F Neural SE N
(min) Data (min) Data (min) Data
0 0.000 0.090 0.0081 0.029 0.0009 0 0.000 0.120 0.0144 0.022 0.0005 0 0.000 0.150 0.0226 0.025 0.0006
30 0.306 0.301 0.0000 0.275 0.0009 30 0.373 0.558 0.0343 0.358 0.0002 30 0.433 0.588 0.0243 0.412 0.0004
60 0.344 0.368 0.0006 0.390 0.0020 60 0.656 0.785 0.0166 0.683 0.0007 60 0.704 0.827 0.0152 0.735 0.0010
120 0.470 0.518 0.0023 0.436 0.0012 120 1.129 1.105 0.0006 1.114 0.0002 120 1.205 1.165 0.0016 1.182 0.0005
240 0.670 0.729 0.0035 0.653 0.0003 240 1.728 1.551 0.0315 1.730 0.0000 240 1.829 1.637 0.0367 1.835 0.0000
360 0.876 0.890 0.0002 0.893 0.0003 360 2.211 1.888 0.1040 2.188 0.0005 360 2.256 1.995 0.0680 2.257 0.0000
480 1.086 1.025 0.0037 1.084 0.0000 480 2.349 2.170 0.0323 2.357 0.0001 480 2.565 2.294 0.0732 2.551 0.0002
SUM 0.0185 0.0056 SUM 0.2337 0.0022 SUM 0.2417 0.0028
(a) 15 % NaCl (b) 20 % NaCl (c) 25 % NaCl
SE F – Squared error Fick model
SE N – Squared error neural model
FIGURE 13.9 Model performances at brine salting in 15% (a), 20% (b), and 25% (c) NaCl solutions.
TABLE 13.2
Modeling Results
Fickian Neural
2 2
R FRatio P R FRatio P
15% NaCl 0.9893 1.792E–03 0.999 0.9933 8.387E–06 0.995

20% NaCl 0.9912 0.002 0.932 0.9996 3.600E–07 0.999
25% NaCl 0.9972 6.759E–07 0.999 0.9995 6.759E–07 0.999
Note: Fratio = Fcalculated/Ftable
TABLE 13.3
Effective Diffusion Coefficients
as a Function of the Salt
Concentration
7 2
Deff. 10 (cm /sec)
15% NaCl 1.64

20% NaCl 4.25
25% NaCl 3.00
The data analyzed by ANOVA (Table 13.2) showed no significant differences

(p ≥ 0.01) between the experimental data and Fickian models or between the
experimental data and ANN models.
It is known that for a reliable statistical investigation some statistical parameters
should be analyzed simultaneously, thus preventing a misinterpreted conclusion. One
can observe that the better fit to experimental data was obtained by the neural model,
2
which showed greater R value, lower SSE parameters, and smaller F ratios for all
brine concentrations tested.
The advantage of this procedure is that it is not necessary to have any previous
knowledge about the process to model it. On the other hand, from the neural network
it was not possible to understand the physical behavior of the process, once it was
modeled from a “black box” approach. Hence, this approach is suitable when it is not
necessary to have a detailed understanding of the process, or in process control strategies
such as Internal Model Control (IMC). Statistical analysis for the Fickian diffusion
model also showed good results, making it possible to calculate the effective diffusivity
coefficient, which is related to the mass transfer rate. However, some attention must be
paid to Fick’s model because of the previous discussions regarding Figure 13.9.
13.4.5 EFFECTIVE DIFFUSION COEFFICIENTS

Effective diffusion values were affected by brine concentration. The brine solution
of lowest concentration, 15% NaCl, presented the lowest Deff (Table 13.3). On the
other hand, the 20% NaCl solution showed the highest effective diffusion coefficient,

rather than 25% NaCl. Reduced effective diffusivity with increasing salt concentra-
tion has been previously reported (Turhan and Kalentuç, 1992) for Turkey white
cheese. The authors associated this occurrence with a lower outer water flux in
relation to inner salt penetration for the solutions of lower concentration. Regardless,
Deff values are similar to those presented by Zorrilla and Rubiolo (1996) for Fynbo
cheese and slightly slower than those reported by Turhan and Kalentuç (1992),
probably due to compositional differences.
13.5 CONCLUSIONS
Although statistical analysis demonstrated that neural network as well as Fickian
diffusion models can successfully model salt diffusion in Prato cheese, observations
on the experimental data plotted together with the applied models showed a notice-
ably better fit with the ANN approach, mainly because of the inadequacy of some
assumptions on the resolution of Fick’s law.
No considerable difference in salt concentration as a function of time was detected
between brine concentrations of 20 and 25%. However, cheese treated in 25% NaCl
solution had a larger moisture loss than that brined at 20% NaCl. For 15% NaCl
solution, the salt penetration and water removal were less intense. Marginal salt uptake
was found at the internal and intermediate regions even after 480 min of processing.
Effective diffusion coefficients were affected by brine concentration. A maximum value
was found at the 20% NaCl solution rather than 25% NaCl, due to greater dehydration
of the cheese samples treated with the latter solution.
ACKNOWLEDGMENTS
The authors gratefully acknowledge Prof. Walter Borzani and Prof. Marcello Nitz for
their helpful discussions and suggestions and students Graziela dos Santos Viola and
Rafaela R. C. Bandeira de Mello for their valuable assistance during the experiments.
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continuous snack food frying process, Trans. ASAE, 41, 1511–1517, 1998a.
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Influence of Vacuum
14 Pressure on Salt
Transport during Brining
of Pressed Curd
A. Chiralt, P. Fito, C. Gonzalez-Martínez,
and A. Andrés
CONTENTS
14.1 Introduction
14.2.1 Cheesemaking
14.2.2 Salting Treatments
14.2.3 Analysis of the Concentration Profiles
14.2.4 Analytical Controls
14.3.1 NaCl Concentration Profiles
14.3.2 Modeling Salt Transport through Profile Development
14.4 Conclusions
Nomenclature
Acknowledgments
References
14.1 INTRODUCTION
Salting of cheese is usually carried out by brine immersion (BI) for a lengthy period
of time (24–48 h, depending on the cheese size), and this causes technological and
quality problems in cheesemaking. The process implies the management of great
amounts of brine and the development of sharp salt concentration profiles in the
cheese pieces, which may provoke ripening problems in some cases (Guinee and
Fox, 1987). Recently, a new salting procedure has been described (vacuum impreg-
nation, VI), which makes the salting process shorter (thus reducing the involved
brine volumes) and the salt concentration profile in cheese flatter (Chiralt and Fito,
1997; Andrés et al., 1997). This new process is based on the action of hydrodynamic

mechanisms (HDM) associated with pressure changes. In the VI process, vacuum
pressure is applied in the salting tank at the beginning of the process for a time t1,
after which the atmospheric pressure is restored for a time t2. During the vacuum
period, the occluded gas in the pressed curd is expanded and flows out. When
atmospheric pressure is restored, the residual gas is compressed, leading to the entry
of the external brine into the curd pores. In this way, a greater salt uptake occurs in
the cheese pieces than when using the conventional immersion for the same salting
time, and a different salt profile is achieved (Andrés et al., 1997).
Salting of cheese by BI has been described as a diffusion process, but capillary
mechanisms may also play an important role in the salt uptake (Geurts et al., 1980).
The capillary input of the external brine in the curd pores can contribute to quite an
extent to the total salt gain when subatmospheric pressure is applied in the salting
tank. Capillary penetration in a pore occurs coupled with the compression of the
occluded internal gas. The volume fraction of the sample penetrated by the external
liquid (Xc) is a function of the capillary pressure (pc), the pressure in the system (p),
and the effective porosity of the product (ε) (Fito, 1994; Fito and Pastor, 1994).
According to Equation (1), the lower the pressure in the system (p), the greater the
capillary penetration.
Xc = ε [pc/(p + pc)] (14.1)
When atmospheric pressure (p2) is restored in the tank at vacuum pressure (p1),
the HDM react, leading to a great penetration of external liquid. The volume fraction
of the sample penetrated by the external liquid (XHDM) has been modeled by Equa-
tions (14.2) and (14.3) in stiff matrices (Fito, 1994). Nevertheless, pressure changes
in the system can also promote sample deformations when the solid matrix exhibits
a viscoelastic behavior (Fito et al., 1996). The restoring of atmospheric pressure
after a vacuum period can promote curd compression and partial collapse of its
pores, decreasing the effectiveness of capillary phenomena for salting.
XHDM = ε (1 – 1/r) (14.2)
r = (p2/p1) + (pc/p1) (14.3)
The aim of this work is to analyze the contribution of the different mass transfer
mechanisms in cheese salting in order to minimize the salting time by using subat-
mospheric pressures. Analysis of the concentration profiles in a product throughout
a mass transfer process is a good approach to clarify the mass transfer mechanisms
involved in the process. In this sense, NaCl and moisture concentration profiles have
been analyzed in cheeses at different times of salting by using:
• BI (brine immersion): salting process at atmospheric pressure

• VI (vacuum impregnation): salting process at vacuum pressure (p1)
• PVI (pulse vacuum impregnation): a two-step salting process; the former
(t1) at vacuum pressure (p1), and the latter (t2) at atmospheric pressure (p2).

14.2.1 CHEESEMAKING
Cheeses were processed at the food technology pilot plant of the Universitat
Autónoma of Barcelona. Ewe’s milk from Manchega sheep was supplied by the
university dairy farm. Cheeses were manufactured from pasteurized milk (15 sec at
72°C), in a 250 l vat, according to standard protocol. Milk (100 l in each batch) was
heated to 31°C, and 2% lactic starter (Lactococcus lactis ssp. lactis plus L. lactis
ssp. cremoris; AM Larbus S.A., Barcelona) was added. After 35 min, the milk
coagulum was cut into 8–10 mm cubes with a wire knife. The curds were heated at
a rate of 1°C per 5 min to reach 36°C and held at this temperature for 10 min prior
to wheying. The curd was molded into cylindrical pieces (10 cm high and 18 cm
diameter) of about 2.5 kg and pressed following two steps: first, for 1 h at 800 Pa;
second, cheeses were turned upside down and pressed again for 3 h at 1600 Pa.
14.2.2 SALTING TREATMENTS

Salting treatments were carried out with a 24% (w/w) brine in a stirred tank at 10°C.
A pressure of 50 mbar was applied during the vacuum periods.
Development of salt and moisture concentration profiles throughout the salting
process was analyzed in cylindrical samples of cheese (6 cm diameter, 10 cm high),
the lateral surface of which was covered with a film in order to avoid radial mass
transfer during salting. The experiments were carried out using two curd batches
and applying different salting times (Table 14.1): t1, time at p1 = 50 mbar and t2,
time at atmospheric pressure (p2).
14.2.3 ANALYSIS OF THE CONCENTRATION PROFILES

A sharp tubular cork borer (20 mm internal diameter) was used to take out cylindrical
samples from salted curd pieces in the axial direction at different times during salting.
Starting at the surface in direct contact with the brine, each sample cylinder was
TM
sliced into disks (1.5 mm thick) with a tissue slicer EMS (Fort, Washington)
model OTS-3000–04. The distance to the interface (d) of the disks of each cylinder
core was identified by the order of slicing. At each distance to the interface, moisture
and salt were analyzed in respective disks.
TABLE 14.1
Salting Treatments for the Analysis of the Salt
Concentration Profile Development
t1 (h) t2 (h)
Salting Treatment p1 = 50 mbar p2 = 1013 mbar Curd Batch
BI 0 0.5, 2, 8, 17 1
PVI 0.5 0; 1.5; 7.5; 16.5 2
VI 0.5; 2; 8; 17 0 1, 2

14.2.4 ANALYTICAL CONTROLS
For sodium chloride determination, samples were homogenized in distilled water at
9000 r/min in an ULTRATURRAX T25 for 5 min and centrifuged to remove any fine
debris present in the sample. An aliquot of exactly 500 µl of centrifuged sample was
taken and titrated in a chloride analyzer (Sherwood, Mod. 926). Moisture content was
determined by drying of the samples at 105°C until a constant weight was reached.

14.3.1 NACL CONCENTRATION PROFILES
Figure 14.1 shows the NaCl concentration profiles for each treatment at 8 and 17 h
salting times, in terms of the reduced salt concentration Y(t,d) (Equation (14.4)) in
the cheese liquid phase (water plus salt), as a function of the distance d to the
interface. In Equation (14.4), z is the salt mass fraction in the cheese liquid phase
at time t (zt), t = 0 (z0) and at equilibrium (ze). The equilibrium value has been taken
to be equal to the brine concentration, according to previous studies (González et al.,
1999). By comparison with the concentration profiles in curds from the same pro-
duction batch, at a determined time of salting, it can be observed that when vacuum
pressure was used, salt penetration was deeper than in the traditional BI method
because of the capillary mechanisms, especially in the lower part of the cheeses
where more pores exist. The effectiveness of the VI process is greater than that of PVI.
Y1 Y1
0.8 (a) 0.8 (b)
0.6 0.6
0.4 0.4
0.2 0.2
d(mm) d(mm)
0 0
0 10 20 30 40 50 0 10 20 30 40 50
Y1 Y1
(c) (d)
0.8 0.8
0.6 0.6
0.4 0.4
0.2 0.2
d(mm) d(mm)
0 0
0 10 20 30 40 50 0 10 20 30 40 50
FIGURE 14.1 Experimental concentration profiles in the upper (a and c) and lower (b and d)
part of the curd, at 8 h (a and b) and 17 h (c and d) of salting by the different procedures
(BI—batch1: ο, PVI—batch2: ◊, VI—batch1: 䊐, VI—batch2: ∆).

This suggests that the pore collapses to quite an extent when atmospheric pressure
is restored, inhibiting the HDM penetration. After 17 h of salting, the concentration
profile was not fully developed in cheeses salted by BI and PVI. However, 8 and
17 h were enough to reach a fully developed profile, in the lower and upper part
respectively, of curd pieces salted by VI. Differences in porosity of the lower and
upper part of the curd (in relation to the plug position during pressing) have been
explained in terms of the viscoelastic response during pressing (Chiralt and Fito, 1997).
This leads to heterogeneous salt transport in the piece, especially if hydrodynamic
mechanisms are promoted.
zt − ze
Y= (14.4)
z0 − ze
14.3.2 MODELING SALT TRANSPORT THROUGH PROFILE

DEVELOPMENT
A pseudodiffusional approach was used to model salt transport in the cheese liquid
phase. Equation (14.5) (Crank, 1975) was fitted to the experimental profiles at the
different salting times by using a nonlinear optimization method to obtain the
effective pseudo diffusion coefficient De for each treatment and curd zone. Equation
(14.5) has been applied considering a number of terms (value of n) great enough to
satisfy Equation (14.6). The obtained values of De for the different samples are
shown in Table 14.2. Despite the scarce physical meaning of De when there is a
notable action of hydrodynamic mechanisms, De values reflect the differences
observed in the profiles. Nevertheless, great deviations in the predicted profiles with
respect to the experimental points were observed.
∞
( − )n  − De t(2 n + 1)2 π 2  (2 n + 1)πl
∑ 2n1+ 1 exp
4
Y(l, t ) =  cos (14.5)
π n=0
4e 2  2e
Y (l, t ) − Yn −1 (l, t )
< 0.01 (14.6)
Yn (l, t )
TABLE 14.2
Values of the Pseudo Diffusion Coefficient (De ×
10 2
10 , m /sec) Obtained from the Modeling
of the Concentration Profile for Each Treatment
and Curd Zone (Lower and Upper Part)
Treatment Upper Part Lower Part
BI-1 4.4 5.2

PVI-2 6.1 8.4
VI-1 4.6 7.7
VI-2 9.5 12.3

Ypred
1.00
0.95
0.90
0.85
0.80
0.80 0.85 0.90 0.95 1.00
Yexp
(a)
Ypred
1.00
0.95
0.90 BI-1
VI-1
VI-2
0.85
PVI-2
0.80
0.80 0.85 0.90 0.95 1.00
Yexp
(b)
FIGURE 14.2 Comparison of experimental Y mean values with those predicted from the
models: (a) pseudodiffusional model (PDM) for the different salting treatments in the lower
(closed symbols) and upper (open symbols) part of the curd, (b) PDM (䊏) and advancing
disturbance front (ADF: ◊) models, for all treatments.
Mean values of Y were calculated for each case by integrating the concentration
profiles at a determined salting time, and their values were compared with those
obtained from the De values applying Equation (14.7) (Crank, 1975). Figure 14.2a
shows the comparison between predicted and experimental values, and a greater
deviation for treatments carried out under vacuum conditions can be observed.
0.5
 De t 
Y = 1− 2 (14.7)
 πl 2 
On the basis of these results, a model developed to predict concentration profiles

was applied (Fito et al., 1998; Salvatori et al., 1998; Salvatori et al., 1999). This model

TABLE 14.3
Location of the Advancing Disturbance Front (df; mm) in the
Upper (UP) and Lower (LP) Part of the Curd, as a Function
of Salting Treatment and Time
BI-1 PVI-1 VI-1 VI-2
Salting Time (h) UP LP UP LP UP LP UP LP
0.5 7.7 10.5 7.7 10.5 9.3 10.8 20.1 22.6

2 13.1 13.8 13.5 16.8 19.8 30.8 27.0 25.9
a a
8 24.4 26.7 21.1 26.4 33.9 37.7
a a a a
17 30.5 30.1 31.2 32.2
a
Fully developed profile.
TABLE 14.4
Parameters df0 and ν Describing the ADF Rate in the Upper
(UP) and Lower (LP) Part of the Curd Salted
by Different Treatments
BI-1 PVI-1 VI-1 VI-2
Parameter UP LP UP LP UP LP UP LP
df0 3.62 7.06 3.62 7.06 2.25 0 14.7 15.6

ν 6.66 6.13 6.66 6.13 11.4 20.5 8.19 8.5
is based on the definition of an advancing disturbance front (ADF) in the material

where mass transport occurs. ADF has been defined as a virtual plane that separates
the zone of the product near the interface where the original concentration status
has been disturbed by mass transport phenomena from the rest of the sample where
no changes in concentration or mass fluxes are evident. The location of the ADF in
the cheese samples has been estimated as the distance (df) to the plane sheet interface
where Y(t,d) = 0.99. Table 14.3 gives the values of df for the different treatments at
each time. The df vs. time relationships have been modeled by Equation (14.8), where
df0 and ν parameters reflect the particular influence of the properties of each curd
on salting rate (González, 1999). Table 14.4 gives the obtained values for each
treatment. The advanced rate of ADF in the cheese dropped as the salting process
progressed and was greatly affected by the curd porosity and water content in VI
treatments.
d f = d f 0 + ν ⋅ t 0.5 (14.8)
When the values of Y(t,d) were plotted as a function of a reduced distance to

the interface z (Equation (14.9)) according to the ADF model, two generalized

1
0.8
0.6
Y
0.4
0.2
0
0 0.2 0.4 0.6 0.8 1
z
(a)
1
0.8
0.6
Y
0.4
0.2
0
0 0.2 0.4 0.6 0.8 1
z
(b)
FIGURE 14.3 Generalized profiles in terms of the reduced distance to the interface (z) for
VI (a) and BI/PVI (b) treatments (VI-1: ο, VI-2: ∆, BI-1: ◊, PVI-2: +). Line: ADF fitted model.
profiles were obtained. One of these profiles corresponds to the vacuum treatments
(VI) and the other to the BI and PVI treatments (Figure 14.3). The ADF model,
shown in Equation (14.10), could be fitted to the points of these generalized profiles
by a nonlinear procedure for z < 1, thus obtaining the characteristic model parameters
(K and z0). In the ADF model, K is a facility coefficient to mass transport of the
system, whereas z0 is a reduced distance near the interface immediately equilibrated
with the external medium (Fito et al., 1998). The obtained values of z0 in all cases
were zero, and K values were 1.075 and 1.145, respectively, for VI and BI/PVI

treatments. The close fitting of this model to experimental points can be seen in
Figure 14.3 (lines). At z ≥ 1, Y = 1 for all treatments.
z = d / df (14.9)
K( z − z 0 )
Y= (14.10)
(z − z 0 ) + (1 − z 0 ) ⋅ (K − 1)
The ADF model also allows prediction of the mean values of Y(t) in the cases
where samples were not completely affected by disturbance (concentration profile not
fully developed) (Fito et al., 1998). Equation (14.11) gives the Y(t) mean values as a
m
function of K and the maximum z value (zt ) of each sample at each time (Salvatori
et al., 1999). Figure 14.3b shows the close agreement between experimental and pre-
dicted values.
  1   1 
Y( t ) = 1 − 1 − K 1 + (K − 1) ln1 −    m  (14.11)
   K    z t 
It can be observed in addition that the ADF model allows prediction of the mean
reduced concentrations better than the pseudodiffusional model (PDM), but only for
those situations when the concentration profile is not fully developed. Nevertheless,
in practical terms, this situation occurs in industrial salting of this kind of cheese for
the usual overall amounts of salt required. The common Y mean values range between
0.88 and 0.84, which correspond to salt levels of 1.5–2.0% in the cheese. These values
are lower than the mean value of Y in the sample disturbed zone (z < 1) for the BI
and PVI treatments and of the order of those reached in the VI treatments. Therefore,
at the end of the usual salting process, the cheese status corresponds to the non-fully
developed concentration profile, and the ADF model will be applicable with more
accurate predictions than those reached with the SDM.
14.4 CONCLUSIONS
Brining at vacuum pressure greatly enhances salting kinetics due to the promotion
of hydrodynamic transport coupled with diffusion in the cheese liquid phase. The
salt concentration profiles developed during VI salting can be better modeled by an
advancing disturbance front model than by diffusional equations. Curd porosity and
moisture greatly affect salt transport kinetics, especially when hydrodynamic mech-
anisms are promoted in the curd pores by vacuum pressure. The greater the curd
porosity and moisture, the faster the salting process. Therefore, special control of
these variables will be recommended during cheese production, ensuring a homo-
geneous salt uptake during the brining process.
NOMENCLATURE
d Distance in the sample to the interface (m)
df Distance of the advancing disturbance front (ADF) to the interface (m)
2
De Pseudodiffusional coefficient (m /sec)

e Sample half-thickness (m)
K ADF model parameter (dimensionless)
l Distance from any point in the sample to center (m)
p Pressure (mbar) (subscript c, capillary; 1, at the vacuum step; 2, atmospheric)
t Salting time (sec)
Y Reduced driven force
z Reduced distance to the sample interface (d/df)
zt Mass fraction of salt in the cheese liquid phase (water plus salt) at time t,
(subscript e, equilibrium; 0, initial value)
z0 ADF model parameter (dimensionless)
ACKNOWLEDGMENTS
The authors thank the Comisión Interministerial de Ciencia y Tecnología (Spain)
and CYTED program for their financial support.
REFERENCES
Andrés, A., Panizzolo, L., Camacho, M.M., Chiralt, A., and Fito, P., Distribution of salt in
Manchego type cheese after brining, in Engineering and Food at ICEF 7, Jowitt, R.,
Ed., Sheffield Academic Press, Sheffield, 1997, pp. 133–136.
Chiralt, A. and Fito, P., Salting of Manchego cheese by vacuum impregnation, in Food
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man and Hall, New York, 1997, pp. 215–230.
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deformation relaxation phenomena during vacuum treatments in solid porous food-
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Effects of Water
15 Concentration and Water
Vapor Pressure on the
Water Vapor Permeability
and Diffusion of
Chitosan Films
J.L. Wiles, P.J. Vergano, F.H. Barron, J.M. Bunn,
and R.F. Testin
CONTENTS
15.1 Introduction
15.2.1 Water Vapor Permeability Coefficients
15.2.2 Solubility Coefficients
15.2.3 Diffusion Coefficients
15.4 Conclusions
Nomenclature
References
15.1 INTRODUCTION
The mechanism for water vapor permeation through hydrophilic films is extremely
complex. The complexity is due to nonlinear water sorption isotherms and water
content dependent diffusivities (Schwartzberg, 1986). Hydrophilic films are usually
used in applications where water vapor migration is not detrimental or water solubility
is advantageous (Donhowe and Fennema, 1994). The water vapor transmission of
hydrophilic films varies nonlinearly with the water vapor partial pressure gradient.
Since chitosan films are cationic and strongly hydrophilic, water interacts with the
polymer matrix and increases permeation for water vapor (Pascat, 1986).

TABLE 15.1
Water Vapor Permeability from Prior Studies on Chitosan Films
Water Vapor
Permeability
(g/m/sec/mmHg) Reference Conditions Description of Film
−8
1.30 × 10 Muzzarelli et al., 1974 38.7°C & 90% RH Chitosan membranes
−9
4.79 × 10 Wong et al., 1992 Ambient Chitosan–lipid films
−9
3.35 × 10 Butler et al., 1996 25°C & 50% RH Chitosan–plasticizer
−8 −9
2.65 × 10 to 8.15 × 10 Caner, et al., 1998 25°C & 50% RH Chitosan–plasticizer
−9 −9
4.42 × 10 to 7.79 × 10 Park, 1998 25°C & 50% RH Chitosan–plasticizer
Most polymer plastic films demonstrate ideal or Fickian permeability behavior

because little or no interaction between the film and the permeant occurs. Thus, Fick’s
first and Henry’s laws apply. Films that are hydrophilic in nature or react to organic
vapors will demonstrate non-Fickian behavior because of the interaction between the
permeant and the polymer film. The film’s thickness, moisture content, temperature,
time, and pressure affect the water vapor permeation rate. For experimental purposes,
most of these variables can be controlled during testing. Other influences on the
permeation process include the nature of the polymer and the nature of the permeant
(Pascat, 1986). Diffusion coefficients (D) for hydrophilic films such as chitosan films
may tend to increase with increasing water vapor concentration. Diffusion measured
in steady state is a mean value over the range of concentration with flux still being
constant through the film. Since D is concentration dependent, the concentration gra-
dient is not linearly dependent on distance through the film (Crank, 1975).
Table 15.1 shows the water vapor permeability coefficients of chitosan films
from previous work with this biopolymer. The hygroscopicity of chitin and chitosan
is comparable to that of cellulose derivatives, but chitin’s surface is less active and
permeable to water (Muzzarelli, 1977). Due to chitin’s insolubility in water, it is
chemically treated to increase water solubility. As a result of this treatment, films
made with chitosan have significant uptake of water and water vapor. At the present,
no research has studied the permeability characteristics of chitosan films over a wide
range of relative humidity (RH) conditions. The water vapor permeability (WVP)
characteristic of chitosan film’s dependency on water concentration is important
because of the magnitude of its effects.
Hauser and McLaren (1948) developed a model to predict the WVP of hydro-
philic films under any RH gradient. Models are used to predict WVP over a large
range of relative humidity conditions. McHugh and Krochta (1994) used the Hauser
and McLaren method to predict WVPs of whey protein isolate and glycerin films. They
concluded that RH had an exponential effect on the WVP of whey protein films. They
recommended that all researchers who study edible films should consider this method.
The objective of this study was to determine the water vapor permeability,
solubility, and diffusion coefficients of chitosan films over a wide range of relative
humidity conditions at 25°C. Previously measured water vapor transmission rates

TABLE 15.2
Measured WVTR, Thickness, and Water Concentration at Various Relative
ο
Humidity Conditions at 25 C for Chitosan Films
LSMEANS
% Relative LSMEANS of LSMEANS of of concentration WVTR × Thickness
2 3
Humidity WVTR (g/m /day) thickness (m) (g/m ) (g/m/day)
−5 4 −4
11 6.65 3.98 × 10 4.64 × 10 2.64 × 10
−5 4 −4
23 14.2 3.93 × 10 6.36 × 10 5.58 × 10
−5 4 −3
33 36.5 3.98 × 10 8.36 × 10 1.45 × 10
−5 5 −3
43 126 3.92 × 10 1.09 × 10 4.95 × 10
−5 5 −2
53 278 3.98 × 10 1.38 × 10 1.11 × 10
−5 5 −2
69 504 4.42 × 10 1.99 × 10 2.23 × 10
−5 5 −2
75 719 4.85 × 10 2.28 × 10 3.48 × 10
−5 5 −2
84 1140 5.93 × 10 2.76 × 10 6.76 × 10
(WVTR) and thickness changes due to water vapor sorption, which are given in
Table 15.2, were used to determine the WVP of chitosan films (Wiles, 2000; Wiles
et al., 2000). Before determining the permeability characteristics of chitosan films,
changes in thickness due to swelling by water vapor sorption were measured (Wiles,
2000) and applied to this study.

Chitosan films of three levels of deacetylation (91.7%, 84.0%, 73.0%) were prepared
by casting a 2% chitosan solution onto a level glass plate. Water sorption isotherms
were determined using the method of discontinuous registration of weight changes
in a static system (Labuza, 1984). Two standard test methods were used to determine
WVTR of chitosan films (Wiles et al., 2000). All film samples were conditioned for
2 weeks at their specified relative humidity and 25°C. Chitosan films were tested
according to ASTM E96–80 (ASTM, 1980), the Desiccant Method, and ASTM F
1249–90 (ASTM, 1990) on the Permatran W600 (MOCON, Minneapolis, MN).
15.2.1 WATER VAPOR PERMEABILITY COEFFICIENTS

2
Equation (15.1) expresses water vapor permeability coefficients in units of g⋅m/m /
day/mmHg, achieved by measuring the WVTR, multiplying it by the thickness, and
dividing by the water vapor partial pressure difference. Thickness measurement takes
swelling into account. A mathematical model was used to describe swelling as a
function of ambient water vapor pressure (Wiles, 2000). The model was based on
data obtained by using the scanning electron microscopy (SEM) and optical micro-
scope to measure swelling. The thickness model was fitted with a polynomial curve
2
with a R of 1.00.
WVP = WVTR l/(p1 − p1) (15.1)

WVP is defined as the steady amount of water vapor flow in unit time through unit
area of a film of unit thickness driven by water vapor pressure difference across the
film’s parallel surfaces under specified temperature and RH conditions (ASTM, 1980).
15.2.2 SOLUBILITY COEFFICIENTS

Solubility coefficient (S) can be derived from the moisture sorption isotherm. From
the measurement for determining the moisture sorption isotherm, the amount of
water (grams) per unit of water vapor pressure (mmHg) is measured in a volume
3
(m ). The volume measurement takes swelling into account.
15.2.3 DIFFUSION COEFFICIENTS

Diffusion coefficients are calculated at each water vapor pressure by using the
measured value of WVP and dividing it by the measured value of S at the same
water vapor pressure.
WVP
D=
S
g
m 2 m ⋅ sec⋅ mmHg
= (15.2)
sec g
m ⋅ mmHg
3
If flux (WVTR) and concentrations are known, another method uses the equation:
D = F(l)/∆C (15.3)
F is WVTR, l is the film’s thickness, and ∆C is the change in water concentration

in the film across the gradient. In the calculation of D, some assumptions are made
about the permeation process in chitosan films. Diffusion and swelling are limited
to one dimension, i.e., perpendicular to the film’s surface, which is parallel to
thickness. It is assumed that the water vapor pressure gradient is linear across the
film in the range where a particular value of D is calculated.

The experimental design used was a randomized block design performed in three
replications with 290 permeation and 682 sorption data measurements. Least-squares
means (LSMEANS) were calculated for thickness, permeability, diffusion, and sol-
ubility coefficients using the General Linear Models (GLM) of SAS (SAS, 1996).
It was determined that no significant difference existed in water vapor permeability
characteristics among the types of chitosan films made using 91.7%, 84.0%, and
73.0% deacetylated chitosan. Therefore, the data points are all compiled together in
this study for further statistical analysis. LSMEANS of measured values were analyzed

and fitted with curves using a nonlinear (NLIN) procedure in SAS. The NLIN
procedure uses the Gauss–Newton iterative method to regress the residuals onto the
partial derivatives of the model until the parameter estimates converge. These models
were used to express the relationships of permeability and diffusion in chitosan films.

In all cases except for solubility of the chitosan films (Figure 15.1), the values increased
with an increase in water vapor pressure. Exponential curves were fitted to the
LSMEANS of the measured values and plotted using NLIN procedure in SAS.
Figures 15.2 and 15.3 show the exponential relationship of WVP and D with increases
in water vapor pressure. Water vapor permeability and diffusion coefficients are not
constant but vary with water vapor partial pressure and concentration (Figures 15.2
and 15.3).
Concentration of sorbed penetrant (water vapor) and temperature are the two
main factors affecting polymer chain segmental motion. Temperature was controlled
at 25°C for this study. The presence of water increases the free volume of the chitosan
film, therefore increasing permeability and diffusion (Rogers, 1985). Deviations from
8.00E-02
WVTR x thickness
7.00E-02
(g m /m /day)
6.00E-02
5.00E-02
2
4.00E-02
3.00E-02
2.00E-02
1.00E-02
0.00E+00
0.0E+00
5.0E+04
1.0E+05
1.5E+05
2.0E+05
2.5E+05
3.0E+05
3
Water Concentration (g/m )
FIGURE 15.1 A plot of WVTR × thickness vs. concentration can be used as an estimate of
the dependence of diffusion on concentration from the slope.
Exponential
LSMEANS
Water Vapor Permeability
5.00E-08
(g/m/sec/mmHg)
4.00E-08
3.00E-08
2.00E-08
1.00E-08
0.00E+00
0 5 10 15 20 25
Water Vapor Pressure (mmHg)
FIGURE 15.2 The relationship between water vapor permeability of chitosan films and water
vapor pressure at 25°C.

Exponential
LSMEANS
Water Vapor Diffusion

4.00E-12
3.00E-12
(m2/s)
2.00E-12
1.00E-12
0.00E+00
0 5 10 15 20 25
FIGURE 15.3 The relationship between water vapor diffusion of chitosan films and water
typical Fickian behavior are associated with the finite rates at which the polymer
structure may change in response to the sorption or desorption of penetrant molecules
(Crank, 1975). Chitosan films exhibit non-Fickian diffusion behavior. A plot of
WVTR times thickness vs. water concentration of the film quantifies and displays
this nonideal behavior (Figure 15.1). The initial dry thicknesses were adjusted accord-
ing to the change in thickness (swelling) due to water vapor sorption at the higher
water vapor pressures (Table 15.2). The average percentages of increase in thickness
were 11% from 16.3 (69% RH) to 17.8 (75% RH) mmHg of water vapor pressure
and 22% from 17.8 (75% RH) to 19.9 (84% RH) mmHg of water vapor pressure.
Frisch (1957) obtained an expression for the time lag in linear diffusion through
a membrane with a concentration dependent diffusion coefficient without solving
the diffusion equation. Frisch’s method determined the relationship between diffu-
βC
sion and concentration in the form of D = D0 e . Stern and Saxena (1980) also
assumed that the concentration dependent diffusion coefficient was an exponential
function of concentration. Zhou and Stern (1989) stated that this exponential expres-
sion for the dependency of concentration by diffusion describes the overall effect
of water concentration on the diffusivity in glassy polymer but cannot explain the
individual components of the sorption separately. Systems such as hydrophilic chi-
tosan films have strong interaction between water vapor and the film itself, which
deviates from ideal behavior by the swelling and plasticizing effects that vary with
water vapor partial pressure. Figure 15.3 agrees with Frisch and others, showing that
D is an exponential function of water concentration.
Water vapor solubility of chitosan films showed a slight decrease from the initial
solubility at intermediate water vapor pressures, with a gradual increase at higher
water vapor pressures. This gave a U-shaped curve (Figure 15.4).
Water concentration inside the film also increased substantially with an increase
in water vapor pressure (Table 15.2). Here again, the effect of water vapor pressure
on water concentration in chitosan films increased exponentially.
Permeability measurements were made at eight levels of water vapor partial
pressure. The concentration gradient was, in every case, 0 mmHg on one side of the
chitosan film, with the other having the prescribed test water vapor pressure. By using
the equation for determining the permeability constant of a multilayer film or
laminate (Equation (15.4)), the individual permeability in each range of water vapor

1.80E+04
Solubility (g/m /mmHg)

1.60E+04
1.40E+04
1.20E+04
3 1.00E+04
8.00E+03
6.00E+03
4.00E+03
2.00E+03
0.00E+00
0 5 10 15 20 25
FIGURE 15.4 The relationship between water vapor solubility in chitosan films and water
5.00E-08
4.00E-08
Permeability per 3.00E-08

Layer
(g/m/sec/mmHg) 2.00E-08
1.00E-08
0.00E+00
0.00–2.68
2.68–5.34
5.34–7.77
7.77–10.23
10.23–12.54
12.54–16.32
16.32–17.84
17.84–19.99
Water Vapor Pressure Range (mmHg)
FIGURE 15.5 The water vapor ranges represent the eight different layers of permeability in
the chitosan film.
pressure can be calculated (Figure 15.5) and the range of the possible thicknesses
of this layer can be determined. In this case, the multilayer film consists of eight
layers, which are the eight different water vapor pressure ranges shown in Figure 15.5.
This information, which is calculated and not measured, can be used to give some
insight into the concentration gradient inside the chitosan film at various levels of
water vapor pressure. It is important to keep the layers in order of low to high water
vapor pressures arranged in the direction of diffusion through the film. If layers are
rearranged, then the calculation of permeability per layer is not possible because of
the water vapor pressure dependence of diffusion.
Using the data in Figure 15.5, the calculated permeability of each layer can be
plotted over a possible range of layer thickness. The equation to calculate the
permeability of a laminate or multilayer film was used to determine the permeability

at each layer according to its water vapor partial pressure range. If the individual
thickness (xn) and permeability coefficient (Pn) are known for each layer, the per-
meability of the layered film (PT) can be calculated from the following equations if
individual P values are independent of pressure (Crank, 1975; Rogers et al., 1957).
xT
PT = (15.4)
x1 x 2 xn
+ + ⋅⋅⋅ +
P1 P 2 Pn
The thickness range limits are then used to plot the steady state water concen-
tration gradient in the chitosan films at various %RH. Figures 15.6–15.12 graphically
represent the steady state concentration gradients across chitosan films at various
water vapor partial pressures or %RH at 25°C.
From the concentration–distance curves, it can be determined that the pattern
of concentration inside the film has a consistent pattern with increasing relative
humidity. Water vapor diffusion occurs in the direction from high concentration to
low concentration of water vapor. These plots show graphically that when chitosan
films reach steady state diffusion, the majority of the concentration distance through
Water Concentration (g/m3)
7.00E+04
6.00E+04
5.00E+04
4.00E+04
3.00E+04
2.00E+04
1.00E+04
0.00E+00
0 0.2 0.4 0.6 0.8 1
Distance (Dimensionless)
FIGURE 15.6 The steady-state concentration distributions across the chitosan film when D =
0 β(c)
D e from 23 to 0% relative humidity at 25°C.
1.00E+05
8.00E+04
6.00E+04
4.00E+04
2.00E+04
0.00E+00
0 0.2 0.4 0.6 0.8 1
0 β(c)

1.20E+05
1.00E+05
8.00E+04
6.00E+04
4.00E+04
2.00E+04
0.00E+00
0 0.2 0.4 0.6 0.8 1
0 β(c)
1.60E+05
Water Concentration
1.40E+05
1.20E+05
1.00E+05
(g/m3)
8.00E+04
6.00E+04
4.00E+04
2.00E+04
0.00E+00
0 0.2 0.4 0.6 0.8 1
0 β(c)
3
2.50E+05
2.00E+05
1.50E+05
1.00E+05
5.00E+04
0.00E+00
0 0.2 0.4 0.6 0.8 1
0 β(c)
the film is at the higher concentration with a sharp decrease in concentration toward
the low concentration end of the curve. This is not typical of most polymer plastic
films, but it is the norm for hydrophilic chitosan films. This pattern may be found
in other types of hydrophilic films.

3
2.50E+05
2.00E+05
1.50E+05
1.00E+05
5.00E+04
0.00E+00
0 0.2 0.4 0.6 0.8 1
0 β(c)
3.00E+05
2.50E+05
2.00E+05
1.50E+05
1.00E+05
5.00E+04
0.00E+00
0 0.2 0.4 0.6 0.8 1
0 β(c)
15.4 CONCLUSIONS
Water vapor partial pressure and concentration have a positive effect on the WVP
and D of chitosan films. These dependencies are non-Fickian in behavior and can
be expressed exponentially except for S. Sorption and diffusion of water vapor are
dependent on the sorbed concentration of water. Water vapor swells and plasticizes
the chitosan film’s polymer structure to increase the mobilities of both the chitosan
polymer segments and water penetrant molecules. Deviations from Fickian behavior
are the results of increased penetrant–polymer and penetrant–penetrant interaction.
From the permeation models and results, there is an indication of two modes of diffusion
in the permeation process from 2.68 to 19.99 mmHg of water vapor partial pressure. The
first mode, from 2.68 to 7.77 mmHg of pressure, is linear in behavior. At water vapor
pressures above 7.77 mmHg pressure, the mode of diffusion is exponential in behavior.
This study has shown the importance of reporting the actual water vapor partial
pressure gradient parameters because of changes that occur in the chitosan film’s
polymer structure due to the plasticizing effect of water vapor. This concept also applies
to most biopolymer films. For example, stating a water vapor pressure gradient of 50%
instead of the water vapor partial pressure range is not adequate because of the
deviations from ideal sorption or diffusion behavior due to the dependency on the

water concentration in the film, which changes with water vapor pressure. The per-
meability measured from 0 to 50% RH is different from that measured from 50 to
100% RH due to microstructural changes in the film due to water at different water
concentrations, although the apparent pressure gradient is the same.
From the graphical representation of the steady state concentration–distance curves,
the concentration gradient through the chitosan film is not ideal through the film and
therefore does not obey Henry’s law. The concentration–diffusion curves of chitosan
films demonstrate the merit of using the saturation/differential method (Demorest and
Mayer, 1996) for measuring the steady state permeation of chitosan films. By condition-
ing films to equilibrium moisture content or water concentration, these films reach steady
state diffusion faster than if they were initially void of permeant. This occurs because of
the lesser change needed in the concentration gradient, as shown in the concentration–dis-
tance curves. Chitosan films that are fully conditioned have fewer stresses in them from
the relaxation and swelling of the polymer chains of the film as compared to a film that
is dry or void of water vapor. This occurs because the film has already been exposed to
water vapor in order to reach equilibrium. Chitosan films that are nearer equilibrium
moisture conditions before testing resulted in more precise WVP measurements.
NOMENCLATURE
WVP Water vapor permeability coefficient (g/m/sec/mmHg)
2
WVTR Water vapor transmission rate (g/m /d)
l Film’s thickness (m)
p1 Water vapor partial pressure at film’s surface outside the cup (mmHg)
p2 Water vapor partial pressure at the underside of the film towards the
desiccant (mmHg)
p1 − p2 Water vapor partial pressure difference (mmHg)
2
D Diffusion coefficient (m /sec)
2
S Solubility coefficient (g/m /mmHg)
2
F Flux (g/m /d)
3
∆C Change in water concentration across the film (g/m )
2
D0 Diffusion coefficient when concentration is zero (m /sec)
e The base of natural logarithms (2.71828)
β Constant characterizing the concentration dependency
3
c Concentration of water in film (g/m )
PT Permeability coefficient of a multilayer film (g/m/sec/mmHg)
xT Total thickness of multilayer film (m)
xn Layer thickness (m)
Pn Layer permeability coefficient (g/m/sec/mmHg)
REFERENCES
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Standards, E96–80, American Society for Testing and Materials, Philadelphia, 1980.
ASTM, Standard test method for water vapor transmission rate through plastic film and
sheeting using a modulated infrared sensor, in ASTM Book of Standards, F1249,
American Society for Testing and Materials, Philadelphia, 1990.

Butler, B.L., Vergano, P.J., Testin R.F., Bunn, J.M., and Wiles, J.L., Mechanical and barrier
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Water Vapor
16 Permeability, Water
Solubility, and
Microstructure
of Emulsified
Starch–Alginate–Fatty
Acid Composite Films
Y. Wu, C.L. Weller, F. Hamouz, S.L. Cuppett,
and M. Schnepf
CONTENTS
16.1 Introduction
16.2.1 Materials
16.2.2 Preparation of Films
16.2.3 Thickness
16.2.4 Conditioning
16.2.5 Water Vapor Permeability (WVP)
16.2.6 Water Solubility (WS)
16.2.7 Scanning Electron Microscopy (SEM)
16.3.1 Water Vapor Permeability
16.3.2 Water Solubility
16.3.3 Microstructure of Starch–Alginate–Fatty Acid Composite Films
16.4 Conclusions
Nomenclature
Acknowledgments
References

16.1 INTRODUCTION
In the formation of edible films, polysaccharides and proteins are generally used for
their ability to establish polymer interactions and create a continuous network respon-
sible for the mechanical properties of the films (Krochta, 1992; Callegarin et al., 1997).
Edible films produced from polysaccharides and proteins, however, are highly sensitive
to water and provide limited resistance to moisture transmission due to the substantial
inherent hydrophilicity of the film-forming substances and to the considerable amount
of hydrophilic plasticizers incorporated into the films (Guilbert, 1986; Krochta, 1992;
Gennadios et al., 1994b; Guilbert et al., 1996; Callegarin et al., 1997). In contrast, lipids,
such as neutral lipids of glycerides, long-chain fatty acids, waxes, resins, and oils,
provide their moisture transfer barrier property for the film because of their hydrophobic
nature (Hernandez, 1994; Callegarin et al., 1997), but films made from lipids alone are
usually too brittle (Kester and Fennema, 1986; Guilbert, 1986; Krochta, 1992). Com-
posite films of polysaccharide–lipid (Kamper and Fennema, 1984a, b, 1985; Kester
and Fennema, 1989; Greener and Fennema, 1989; Hagenmaier and Shaw, 1990;
Koelsch and Labuza, 1992; Wong et al., 1992; Debeaufort et al., 1993; Park et al.,
1994; Sapru and Labuza, 1994; Callegarin et al., 1997) or protein–lipid (Avena-
Bustillos and Krochta, 1993; Gennadios et al., 1993; McHugh and Krochta, 1994a, b;
Gontard et al., 1994, 1995; Saravia, 1995; Shellhammer and Krochta, 1997b; Rhim et al.,
1999), in laminated or emulsion forms, have been developed and have shown increased
moisture resistance and improved functionality for edible packaging application.
Starch–alginate coatings have been applied on precooked pork chops (Handley
et al., 1996; Hargens-Madsen et al., 1995) and ground beef patties (Ma-Edmonds
et al., 1995) to inhibit lipid oxidation and the formation of warmed-over flavor.
However, the poor moisture barrier property of starch–alginate films hinders them
from being used to control moisture loss in precooked meat products. When free-
standing starch–alginate films were applied on precooked meat products in a previous
study, moisture absorption and film swelling were observed on these films and the
packaged meat became dry over time (unpublished data). Mechanical properties and
other barrier properties can be lost upon the hydration of the swollen films. Incor-
poration of fatty acids into starch–alginate films, therefore, may provide hydropho-
bicity and increase film resistance to water transmission.
In this study, the effect of fatty acids (lauric, palmitic, and stearic acids) on the
moisture barrier property of starch–alginate films was evaluated in terms of water vapor
permeability and water solubility. Microstructure examination was performed to help
elucidate the structure–function relation of starch–alginate–fatty acid composite films.

16.2.1 MATERIALS
CstarEmCap 0637, a lipophilic modified starch, was obtained from Cerestar USA
Inc. (Hommond, IN). Sodium alginate was provided by Kelco Division of Merck
and Co. (Rahway, NJ). Glycerin was purchased from Mallinckrodt Baker Chemical
(Phillipsburg, NJ). Lauric acid (LA), palmitic acid (PA), and stearic acid (SA) were

purchased from Sigma Chemical Co. (St. Louis, MO). Lecithin (Lecigran 5750), an
emulsifier, was provided by Riceland Foods Inc. (Little Rock, AK). Ethyl alcohol
(USP dehydrated, absolute-200 proof) was purchased from McCormick Distilling
Co., Inc. (Weston, MO).
16.2.2 PREPARATION OF FILMS

A control (0% fatty acid) starch–alginate film solution was prepared by slowly
dissolving 5 g starch and 2 g alginate in a constantly stirred mixture of distilled
water (127.3 ml), ethanol (63.6 ml), and glycerin (2.1 g). Additionally, three other
starch–alginate–fatty acid film solutions were prepared using LA, PA, and SA. For
each starch–alginate–fatty acid film, four levels of each fatty acid (10, 20, 30, or
40% w/w of starch and alginate) were used. An emulsion with each fatty acid was
prepared by adding a portion of the fatty acid into the 200 ml starch–alginate film
solution with 30% (w/w of fatty acid) of lecithin. The solution was then heated to
o
boiling (78 C) with stirring to completely melt the fatty acid. All added fatty acids
had melting points lower than the boiling point of the film solution. Each boiled
solution was homogenized using an Ultra-Turrax T25 homogenizer (Janke & Kunkel
GMBH & Co. KG, Staufen, Germany) at 9500 r/min for 2 min, strained through
eight-layered cheesecloth (grade 40, Fisher Scientific), and poured onto a leveled
Teflon coated glass plate (21 cm × 35 cm). Film thickness was controlled by casting
volumes of solutions having the same amount of solids (8.82 g) onto each plate.
Films were allowed to dry at ambient conditions for about 24 h. Then they were
peeled from the plate, and samples for property testing were cut. Water vapor
permeability (WVP) and water solubility testing samples were squares of 7 × 7 and
2 × 2 cm, respectively.
16.2.3 THICKNESS
Film thickness was measured to the nearest 2.54 µm (0.1 mil) with a hand-held
micrometer (B.C. Ames Co., Waltham, MA). Five thickness measurements were
taken on each WVP sample, one at the center and four around the perimeter, and
the mean values were used in WVP calculations.
16.2.4 CONDITIONING
All film samples for WVP and WS were conditioned for 2 d in an environmental
chamber (Model RC-5492, PGC Parameter Generation & Control, Inc., Black Moun-
tain, NC) set at 50% RH and 25°C before testing (ASTM Standard Method D 618-61,
ASTM, 1995a).
16.2.5 WATER VAPOR PERMEABILITY (WVP)

. 2
WVP (g mm/m ⋅ h ⋅ KPa) was calculated as:
WVP = (WVTR ⋅ L)/ ∆p (16.1)

WVTR was determined gravimetrically using a modified ASTM Method E 96-95
(ASTM, 1995b). Film specimens were mounted on poly(methyl methacrylate) cups
filled with distilled water up to 1 cm from the film underside. The cups were placed
in an environmental chamber set at 25°C and 50% RH. A fan was operated within
the chamber, creating an air velocity of 198 m/min over the surface of the cups to
remove permeating water vapors. Weights of the cups were recorded every h for a
period of 8 h. Steady state was reached after about 1 h. Slopes of the steady state
(linear) portion of weight loss vs. time curves were determined by linear regression
2
to estimate WVTR. Coefficient of determination (R ) for all reported data was 0.99
or greater. In calculating WVP, the effect of resistance of the stagnant air layer
between the film undersides and the surface of water in cups was corrected for
(McHugh et al., 1993; Gennadios et al., 1994b). For each type of film, WVP
measurements were replicated three times.
16.2.6 WATER SOLUBILITY (WS)

WS was calculated as the percentage of soluble matter to initial dry matter in each
film sample using the method of Gontard et al. (1992), with some modifications.
Three randomly selected samples from each type of film were first dried at 105°C
for 24 h to determine initial dry matter. After drying, films were immersed in 30 ml
of distilled water in a 50 ml beaker. Beakers were covered with Parafilm “M” wrap
(American National Can, Greenwich, CT) and stored in an environmental chamber
at 25°C for 12 h with occasional gentle stirring. Since all film samples disintegrated
into small pieces after soaking in water, the sample solutions were set for another
10 min to allow the undissolved sample pieces to deposit on the bottom of the
beakers. The supernatant of the solution (water) was then discarded and the deposited
undissolved sample was poured into an aluminum drying dish with the water residue
and oven dried at 105°C for 24 h. The weight of solubilized matter was calculated
by subtracting the weight of undissolved dry matter from the weight of initial dry
matter and expressed as a percentage of the initial dry matter content. Film samples
were weighed to the nearest 0.0001 g before and after drying. WS was determined
in triplicate for each type of film.
16.2.7 SCANNING ELECTRON MICROSCOPY (SEM)

Microstructural characteristics of starch–alginate film samples were examined using
an AMRAY 1000A electronic microscope (AMRAY Inc., Bedford, MA), while those
of starch–alginate–fatty acid composite film samples were examined using a JSM-
6100 scanning microscope (JEOL, Tokyo, Japan). All film samples were prepared
using the same methods as for preparing films for WVP and WS testing, but without
adding glycerin. Samples were mounted on an aluminum stub with copper tape, first
coated with carbon by vacuum evaporation on a Denton DV-502 vacuum evaporator
(Denton Inc., Cherry Hill, NJ) and then sputter coated with gold–palladium alloy
with a EBTEC sputter coater (EBTEC Co., Agawam, MA). Samples were examined
using an accelerating voltage of 20 kV. Images were recorded on Polaroid film (Type
o
665) and photographed at a tilt angle of 60 to the electron beam for views in the
cross section.

Means and standard deviations on a completely randomized design with three rep-
lications were determined using the Genera Linear Models procedure in the SAS
program (SAS Institute Inc., 1990). Fisher’s protected least significant differences
(Fisher’s protected LSD) were calculated to indicate differences among mean values.
Significance was accepted at a level of P < 0.05.

16.3.1 WATER VAPOR PERMEABILITY
The WVP values, along with the thickness values and actual RH conditions at the
undersides of films during testing, of control starch–alginate film and emulsified
composite starch–alginate–fatty acid films are presented in Table 16.1. The WVP of
. 2
the control starch–alginate film was 5.14 g mm/m ⋅ h⋅KPa. This value was of the
2
same order of magnitude as mean WVP values of 2.20 g⋅ mm/m ⋅h ⋅ KPa and
. 2
2.99–8.78 g mm/m ⋅ h⋅ KPa previously reported for polysaccharide films made from
methyl cellulose (Gennadios et al., 1994a) and chitosan (Rhim et al., 1998), respectively,
which were tested with the same method and same conditions, i.e., 25°C and
100/50% RH gradient, as in the present study.
TABLE 16.1
Water Vapor Permeability (WVP) and Water Solubility (WS)
of Starch–Alginate Films with Lauric Acid (LA), Palmitic Acid (PA),
or Stearic Acid (SA)
a a a
Fatty Acid in Film Thickness RH Inside Cup WVP WS
2 ·
(% of Starch–Alginate) (µm) (%) (g·mm / m · h·KPa) (%)
g b b
Control 0 106 77.1 ± 1.06 5.14 ± 0.05 54.53 ± 2.62
f b bc
LA 10 148 84.4 ± 1.20 4.74 ± 1.11 52.78 ± 1.84
de cde bc
20 128 88.9 ± 1.16 2.52 ± 0.07 52.84 ± 0.93
cde cde d
30 127 89.9 ± 1.78 2.22 ± 0.47 47.60 ± 0.57
bcd efg de
40 126 90.5 ± 1.28 2.04 ± 0.31 46.29 ± 2.87
f c c
PA 10 101 85.2 ± 0.52 2.91 ± 0.19 51.40 ± 0.61
f cd d
20 96 84.8 ± 1.22 2.86 ± 0.24 47.89 ± 0.53
f c ef
30 103 85.5 ± 0.25 2.91 ± 0.18 44.74 ± 0.92
ef cde def
40 109 87.3 ± 3.80 2.60 ± 0.92 45.47 ± 1.11
f cde de
SA 10 90 85.0 ± 2.35 2.69 ± 0.58 47.26 ± 0.98
de def f
20 106 89.7 ± 2.44 2.07 ± 0.25 43.51 ± 2.52
b g g
30 116 93.3 ± 0.46 1.25 ± 0.10 38.09 ± 0.32
bc fg g
40 111 92.6 ± 1.08 1.30 ± 0.11 35.80 ± 1.70
a
Mean of three replicates ± standard deviation. Measured at 25°C and 100/50% RH gradient. RH at
film undersides inside cups and WVP were corrected to account for resistance of stagnant air layer
between film underside and water surface (Gennadios et al., 1994b).
b–g
Means within a column are significantly (P < 0.05) different.

With the exception of films with 10% LA, WVP of starch–alginate films was
2
significantly reduced by incorporation of LA, PA, or SA to as low as 1.25 g⋅ mm/m ⋅
h⋅ KPa for films with 30% SA. Decreases in WVP of starch–alginate films may be
attributed to the increased hydrophobicity and the structural complexity imparted
into starch–alginate films by the fatty acids, which is further discussed in the SEM
result section in this work. Fatty acids have been successfully used to reduce WVP
of emulsified cellulose ether films (Kamper and Fennema, 1984a,b; Hagenmaier and
Shaw, 1990; Koelsch and Labuza, 1992; Sapru and Labuza, 1994) and chitosan films
(Wong et al., 1992). The reduction of WVP has also been observed with addition
of fatty acids into wheat gluten films (Gontard et al., 1994; Derksen et al., 1995),
whey protein films (McHugh and Krochta, 1994b), and soy protein isolate films
(Rhim et al., 1999) using emulsion technique.
Generally, with increasing length of the lipid hydrocarbon chain, as well as
concentration of the lipid, resistance of a lipid film to water vapor transmission
increases (Fennema et al., 1993; Callegarin et al., 1997; Shellhammer and Krochta,
1997a). As shown in Table 16.1, the effect of chain length on WVP was mainly shown
by the significant differences in WVP values found between SA films and LA and
PA films in the present study. In general, incorporation of SA into starch–alginate
films resulted in the lowest WVP values at all levels when compared with the
incorporation of LA and PA. The WVP values of films with PA and LA were similar,
except at the level of 10%, where PA was more effective than LA in reducing WVP.
WVP decreased significantly as fatty acid concentration increased in films with LA
and SA. However, increasing PA concentration did not significantly reduce WVP. For
films with LA and PA, a fatty acid content of 40% resulted in the lowest WVP, while
the lowest WVP was obtained in films with 30% of SA. The overall WVP change
pattern in this study suggests that there is an optimum concentration of fatty acid
at which WVP can be lowered most effectively.
According to Kamper and Fennema (1984a), increasing the stearic acid concen-
tration in emulsified hydroxypropyl methylcellulose–fatty acid films decreased their
WVP until an optimum was reached. Hagenmaier and Shaw (1990) found that
hydroxypropyl methylcellulose–fatty acid emulsion films had decreased WVP as the
fatty acid concentration increased from 23 to 45%. However, an increase in perme-
ability occurred above a volume fraction of stearic acid of 46%. Similar results have
been reported by Sapru and Labuza (1994) in methyl cellulose–stearic acid com-
posite films, by Gontard et al. (1994) in wheat gluten–lipid composite films, and by
Rhim et al. (1999) in soy protein isolate films composed with LA and PA. Sapru
and Labuza (1994) found that when the stearic acid volume was above 22%, the
increase in WVP was attributed to inadequate filling of the void volume within the
stearic acid crystallites by the methyl cellulose–polyethylene glycol matrix.
16.3.2 WATER SOLUBILITY

Similar to WVP, WS is an indication of the hydrophilicity of a film. Moreover, WS
is affected by the chemical nature and the structural integrity of films. As shown in
Table 16.1, incorporation of fatty acids significantly reduced WS of starch–alginate
films by as much as 34% with 40% stearic acid. The overall WS decreased as the

chain length of fatty acid increased, as indicated by significant differences between
film types. WS reduction was more pronounced at increasing levels of fatty acid in
the films. It was also observed that films, with or without fatty acids, disintegrated
easily after 12 h of soaking. WS, apparently, is more affected by the hydrophilic
nature of films rather than by their structural integrity. WS (total soluble matter) of
soy protein–fatty acid films has been reported to be less than that of soy protein
films without fatty acids (Gennadios et al., 1997). Lai et al. (1997) determined water
absorption rate, another property related to hydrophilicity of zein–fatty acid sheets,
and reported that the amount of water absorbed deceased as fatty acid levels increased
in the sheets. However, a sharp increase in WS beyond a threshold lipid material
content has been observed in wheat gluten–lipid composite films (Gontard et al.,
1994) and soy protein–fatty acid composite films (Rhim et al., 1999). These dis-
crepancies may be attributed to the types of matrix materials used for film formation,
the types and amounts of emulsifiers added into the films, and the differences in
film homogeneity and structure.
16.3.3 MICROSTRUCTURE OF STARCH–ALGINATE–FATTY ACID

COMPOSITE FILMS
To better understand the structure–function relation existing in starch–fatty acid
composite films, scanning electron microscopic examination was performed on the
control starch–alginate film and films with 30% fatty acids. Variations in microstruc-
ture among these films were evident from a comparison of the SEM photomicro-
graphs, as shown in Figure 16.1.
The structure of starch–alginate film without the addition of fatty acid was
compact and dense, and the film surface had a smooth contour free from pores and
cracks (Figure 16.1A). One of the basic physical properties of carbohydrates is that
they attract water. Hydrophilicity is expected due to their numerous hydroxyl groups,
which form hydrogen bonds with water molecules (Whistler and Daniel, 1985). It
is also believed that water molecules can interact with the matrix and increase the
permeation rate when they penetrate hydrophilic materials (Pascat, 1986). The hydro-
philic nature of the starch–alginate film, therefore, accounts for the water perme-
ability value obtained in the present study (Table 16.1).
When fatty acids were incorporated into the starch–alginate film, the film micro-
structure was changed dramatically (Figure 16.1B, C, and D). This change in the film
structure may play a key role in the barrier properties of the composite films, as
evidenced by the reduction in WVP and WS of the films. For all fatty acid composite
films, there was no obvious migration of the fatty acid to the air–film surface, as noted
by other authors using methylcellulose derivatives as the base component (Greener
and Fennema, 1989; Vojdani and Torres, 1989, 1990). Microstructures in the cross
sections of these films showed some differences. A stratified flaky structure was
found in the starch–alginate–LA film (Figure 16.1B). This layer structure could
be easily observed visually. A similar, but more compact, stacking layer structure
has been noted in a chitosan–LA film (Wong et al., 1992). The arrangement of
flaky layers of starch–alginate films provided an extended network of channels
lined with hydrophobic molecules. The lower WVP of starch–alginate–LA films

(a) (b)
(c) (d)
FIGURE 16.1 Photomicrographs taken by scanning electron microscopy of starch–alginate–fatty acid composite films (fatty acid = 30% starch–alginate,
w/w). A: Pure starch–alginate film; B: Starch–alginate–lauric acid film; C: Starch–alginate–palmitic acid film; D: Starch–alginate– stearic acid film (bar =
20.8 µm).
(Table 16.1) suggests that this network hindered the penetration of water molecules
through the films.
The structure of starch–alginate–PA showed a nonhomogeneous or irregular
layered sponge-like structure (Figure 16.1C). Although the network of this structure
is more complicated than that of films with LA, which may have contributed to the
lower WS in films with PA, the nonhomogeneous distribution of PA may account
for a WVP that did not significantly differ from that of films with different contents
of PA and from that of LA films. PA has been incorporated into zein sheets by Lai
et al. (1997). They reported that layered structures were progressively formed, and
that the structures became more compact when the concentration of PA was increased
from 0 to 50% of corn zein protein in zein sheets. This change in structure was
shown to coincide with the decreased water absorption of the zein sheets.
In starch–alginate–SA films, the structure was somewhat similar to that shown
by PA films (Figure 16.1D). However, the layered sponge-like structure of SA films
was highly channeled, and SA was evenly distributed in the continuous starch–alginate
matrix, which may set up a more tortuous path or increased path length for diffusing
water molecules than those found in the other films. Consequently, films with SA
exhibited the lowest WVP and WS values among all composite films. It is believed
that a fine particle size and even distribution of lipids are important to the effective-
ness of an emulsion film (Wong et al., 1992; McHugh and Krochta, 1994a; Debeau-
fort and Voilley, 1995). The existence of stearic hindrance and tortuosity in the film
structure also influences the permeability of films (Holton et al., 1994). According
to Koelsch (1994), the high degree of inherent tortuosity that resulted from an even
interlocking network within methylcellulose–SA emulsified composite films was
responsible for the low WVP values of the films. In these films, the interlocking
network of SA chains within the support matrix reached a maximum (i.e., maximum
tortuosity) at about 30% SA, a concentration similar to our optimum SA level for
starch–alginate–fatty acid films.
Besides the dispersion of fatty acids in the base matrix, complex formation between
starch amylose/amylopectin fractions and fatty acids may also account for the changed
microstructures, and thus the lowered WVP and WS values for the fatty acid composite
films. Fatty acids can form inclusion complexes with helical amylose and possibly with
the longer outer chains of amylopectin. Such complexes resist entry of water (Whistler
and Daniel, 1985). Gray and Schoch (1962) demonstrated that the presence of fatty
acids decreased the swelling and solubilization of starch by forming a fatty acid–amy-
lopectin complex. Lagendijk and Pennings (1970) found that the amount of fatty acid
complexed with amylopectin increased linearly with increasing fatty acid chain length.
16.4 CONCLUSIONS
Moisture barrier properties of starch–alginate films can be improved substantially by
incorporation of LA, PA, and SA. The reduction in WVP and WS of starch–alginate
films was more pronounced as the fatty acid chain length increased and at increasing
levels of fatty acids in general. The tortuous network formed by the interaction of
fatty acids and the starch–alginate matrix may contribute improved barrier properties.

The more uniform the distribution of the fatty acid molecules, and the higher degree
of the tortuosity of the network formed by the fatty acids in the film’s microstructure,
the better the moisture barrier property of the film.
NOMENCLATURE
2
WVP Water vapor permeability (g⋅mm/m ⋅ h⋅ KPa)
2
WVPR Measured water vapor transmission rate through a film (g/m ⋅ h)
L Film thickness (m)
∆p Partial water vapor pressure difference across the two sides of a film (Pa)
ACKNOWLEDGMENTS
We express special appreciation to Tom Bargar in the Department of Veterinary and
Biomedical Sciences at the University of Nebraska–Lincoln for assistance in scan-
ning electron microscopy.
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Mass Transport
17 Phenomena during
the Recovery of Volatile
Compounds by
Pervaporation
T. Schäfer and J.G. Crespo
CONTENTS
17.1 Introduction
17.2 The Principles of Pervaporation
17.2.1 Nonideal Transport Phenomena at the Membrane
Surfaces: Concentration Polarization
17.2.2 Nonideal Transport Phenomena in the Membrane
Polymer: Swelling and Flux Coupling
17.3 Technical Aspects of Pervaporation
17.4 Advantages and Applications of Pervaporation in the Food Industry
17.4.1 Hydrophilic Pervaporation
17.4.2 Organophilic Pervaporation
17.5 Conclusions
References
17.1 INTRODUCTION
This chapter presents pervaporation as a membrane separation process for the selec-
tive removal and recovery of dilute compounds from a bulk liquid. First, the principle
of pervaporation will be described, followed by a discussion of its main transport
phenomena and a mathematical description of ideal conditions. Pervaporation is, at
first sight, not a complicated process. It is, however, rather versatile. This is on the
one hand an advantage, because pervaporation can be adapted and integrated in
process lines with considerable flexibility. On the other hand, this versatility has led
to an abundance of different individual applications that cannot readily be compared.
Recently, attempts have been made in the literature to search for empirical rules on

pervaporation in individual situations. It is, however, the authors’ opinion that instead
of empirical rules, a concise but comprehensive understanding of the scientific back-
ground of pervaporation fosters the creativity necessary for a flexible and appropriate
process design. The essentials of this background will be presented for ideal conditions
in the first section, “The Principles of Pervaporation,” in conjunction with a discussion
of the most relevant nonideal phenomena.
The second part of this chapter, “Technical Aspects of Pervaporation,” will dem-
onstrate how the theory is put into practice.
The final section will illustrate the theoretical information provided by selected
case studies with special regard to applications in the food industry. The potential,
as well as the limits, of pervaporation will be discussed in comparison with other
separation techniques, and it will be shown how careful process design allows the
application of pervaporation to diverse separation problems.
17.2 THE PRINCIPLES OF PERVAPORATION

Pervaporation is a membrane separation process that employs dense, nonporous mem-
branes for the selective separation of dilute solutes from a liquid bulk solvent (Néel,
1991). The separation concept of pervaporation is based on the molecular interaction
between the feed components and the dense membrane polymer. This differs from
pressure-driven membrane separation processes involving porous membranes, such as
microfiltration, where the general separation concept is primarily based on molecular
size exclusion. Pervaporation is a process very similar to vapor permeation, the only
difference being that in the latter the feed is not liquid, but a vapor. It should, however,
be clearly distinguished from membrane distillation (Luque de Castro and Gámiz-
García, 2000), in which a porous membrane is in contact with a liquid feed, and feed
components evaporate through the membrane pores. In this case, the membrane poly-
mer does not have any selective impact on the solute transport, but merely serves as
a mechanical barrier (Lawson and Lloyd, 1997).
The principle of pervaporation is illustrated in Figure 17.1. A nonporous membrane
separates a liquid feed, commonly close to atmospheric pressure, from a downstream
compartment in which a vacuum is applied. When the feed contacts the membrane,
the solutes (denoted i in Figure 17.1) sorb in the membrane surface due to solute–poly-
mer interactions (Figure 17.1, bottom, I). These solute–polymer interactions imply that
the solvating power of the polymer is higher with regard to some solutes than that of
the bulk solvent. Under ideal conditions, a thermodynamic equilibrium will be reached
when the chemical potential of the solute i is equal in the membrane surface and the
liquid phase adjacent to it. The sorption of these solutes at the membrane surface
creates a solute concentration gradient across the membrane, resulting in a diffusive
net flux of solute across the membrane polymer (Figure 17.1, bottom, II).
In pervaporation, any solute that has diffused toward the membrane downstream
surface is ideally instantaneously desorbed and subsequently removed by a vacuum
applied on the downstream side of the membrane (Figure 17.1, bottom, III). As a
consequence, the solute concentration on the membrane downstream surface remains
practically zero, and a maximum concentration gradient between the two membrane
surfaces is maintained. As a result, the diffusive net flux across the membrane is maximal.

liquid µi feed >> µi permeate vapor
phase phase
(ambient (vacuum)
pressure)
i
i i
pfeed i i pperm
i
selective, nonporous highly porous

membrane support
I II III
i i i
i i i i i
i i i i i i
i i i i
i i i ii i
i i i
i i i i i i i
i i i
i i vacuum
i i i
FIGURE 17.1 The principle of solute transport across the membrane in pervaporation.
If the vacuum is not sufficiently low to desorb all of the solutes reaching the membrane
downstream surface, the concentration of solute i at the membrane downstream surface
will not be equal to zero. As a consequence, the concentration gradient will decrease
and so will the diffusive net flux across the membrane. The driving force in pervapo-
ration is thus the gradient of the concentration, or more precisely of the chemical
potential, of a solute across the selective membrane.
It should be noted that the role of the vacuum in pervaporation is merely the
efficient desorption and removal of solutes from the membrane downstream surface,
hence maintaining the driving force of the process. The pressure difference between
the two sides of the membrane does not directly affect the transport of an individual
component i within the membrane polymer, as is the case in pressure-driven processes
involving porous membranes. Ideally, the molecular motion of a component i within
the membrane polymer is purely diffusive and thus independent of any operating
conditions beyond the membrane surfaces. Of course, these operating conditions con-
tribute to determining the concentration of component i on the membrane surfaces,
according to which, in turn, a certain diffusive net flux of this component across the
membrane results.
To ensure the maximal concentration gradient, the downstream pressure must
be low enough to remove any solute at the membrane downstream face. Because
the solute i leaves the membrane downstream surface due to the vacuum in the vapor

state, the downstream concentration of solute i is more conveniently expressed in
terms of its partial pressure, according to Dalton’s law:
p ip = y i ⋅ p p (17.1)
p
where pi is the partial pressure of i in the permeate, yi is the molar fraction of I,
p
and p is the total downstream pressure. The solute feed concentration can be expressed
in terms of its partial pressure in the feed by
p if = x i ⋅ γ i ⋅ p 0i (17.2)
f
Equation (17.2) is a modified Raoult’s law where pi is the partial pressure of a
compound i in the feed (Pa), xi is the molar fraction of I, and γi is the activity
coefficient of i in the feed. The saturated vapor pressure of i (Pa) at a given
0
temperature is denoted by pi . The activity coefficient γi accounts for nonideal behav-
ior of the solute in the feed solution as, for example, in the case of aqueous salt
solutions (increased activity coefficient of the solute due to the salting-out effect)
or aqueous ethanol solutions (decreased activity coefficient of the solute due to a
co-solvent effect of ethanol).
For the partial pressure gradient of solute i across the membrane, it hence
follows:
∆p i = p if − p ip = x i ⋅ γ i ⋅ p 0i − y i ⋅ p p (17.3)
Rearranging Equation (17.3) gives the minimum total downstream pressure

p f
necessary for ensuring flux of a defined solute i across the membrane, i.e., pi < pi:
x i ⋅ γ i ⋅ p 0i
pp < (17.4)
yi
As long as Equation (17.4) is fulfilled, any compound possessing at least some

volatility may be recovered from a liquid feed by pervaporation. Some aspects of
Equation (17.4) should be emphasized and will be referred to later:
0
1. A low volatile compound (low pi ) might still be very well recovered by
pervaporation if its activity coefficient γi in the feed solution is high.
2. The driving force can be high either by a low total downstream pressure
or by a high saturated vapor pressure of the solute, for example through
heating of the feed solution.
3. Increasing the total upstream pressure does not effectively increase fluxes
because the bulk feed is liquid and thus of low compressibility.
Assuming a constant solute feed concentration and instantaneous removal of

any solute on the membrane downstream face, the selective transport of the solute
i from the bulk feed to the downstream (vacuum) compartment can hence ideally
be described by successive steps as:

c mem,
i
f
µmem,
i
f
µ l, bulk
i
c l,i bulk c mem,

i
p
µmem,
i
p
p
µpi
c i
FIGURE 17.2 The ideal profile of the concentration and chemical potential of a solute i in
the membrane polymer according to the equations derived in the text.
1. An equilibrium partitioning (sorption) of the solute i between the liquid

bulk feed and the membrane upstream surface
2. A diffusion of solute i across the membrane polymer toward the membrane
downstream surface
3. An equilibrium partitioning (desorption) of the solute i between the mem-
brane downstream surface and the permeate vapor, as shown in Figure 17.2
For the equilibrium partitioning in steps 1 and 3, it follows that:
cimem, f c mem, p
l ,bulk
= Si = i p (17.5)
ci ci
mem,f, l,bulk mem,p p
where ci ci , ci , and ci are the concentration of i in the membrane at the
upstream interface, in the bulk liquid, in the membrane at the downstream interface,
and in the permeate, respectively, and Si is the sorption (partitioning) coefficient of
i in the homogenous membrane polymer. For the ideal diffusion of solute i across
the membrane polymer toward the membrane downstream surface, Fick’s First Law
applies:
dc mem c mem, f − cimem, p

J i = Dimem ⋅ = Dimem ⋅ i (17.6)
dz z
where Ji is the flux of solute i across the membrane, z is the selective membrane
mem
thickness, and Di is the diffusion coefficient of i in the selective membrane
polymer. Combining Equations (17.5) and (17.6) yields the transport model most
applied in pervaporation, the so-called solution–diffusion model (Lee, 1975). This
−2 −1
model gives the overall solute flux across the membrane Ji (kg·m ·sec ) as
∆ci (c l, bulk − cip )

J i = Si ⋅ Dimem ⋅ = Pi ⋅ i (17.7)
z z
2 −1
Pi (m ·sec ) is the so-called permeability of i in the membrane and a product
of the solubility and the diffusivity of the solute i in the membrane. Because the

solute concentration is related to the solute partial pressure, the driving force can
also be expressed as a partial pressure gradient of the solute i across the membrane
yielding
∆p i ( p f − p ip )
J i = Si ⋅ Dimem ⋅ = Pi′⋅ i (17.8)
z z
−1 −1 −1
with the permeability coefficient Pi′ in (kg·m ·sec ·Pa ).
It has been observed that the permeability Pi of solute i in a membrane can be
described by an Arrhenius-type equation.
Equation (17.4) can be rearranged to
γ i ⋅ p i0 y i
> = βimol (17.9)
pp xi
mol
where βi is defined as the molar enrichment factor of i. If an enrichment of
mol
compound i is desired in the permeate, βi has to be greater than unity, and hence
has the quotient yi/xi. An enrichment of compound i in the permeate is thus obtained
by a low downstream pressure, a high saturated vapor pressure of compound i, or
its high and positive activity coefficient in the feed solution. It is common to use
the enrichment factor βi as the ratio of the mass concentration of i in the permeate,
p −3 f −3
ci (kg·m ), to the mass concentration of i in the feed, ci (kg·m ), rather than the
mol
molar enrichment factor βi :
cip
= βi (17.10)
cif
The ratio of the enrichment factors of a compound i and a compound j indicates

the selectivity αij that a membrane has for compound i in comparison with compound j:
cip
βi cf
= p i = α ij (17.11)
βj cj
c fj
For a given separation problem of a solute i from a bulk solvent j, the partial
flux Ji, or more generally the permeability Pi, the enrichment βi, and the selectivity
αij, are the parameters that characterize the separation performance of a pervapora-
tion process.
When deriving the equations mentioned above, some assumptions were implic-
itly made with regard to the ideal transport of solute to, across, and away from the
membrane. In pervaporation, nonideal transport phenomena can occur in the feed
liquid phase adjacent to the membrane upstream surface, within the membrane
polymer, and in the vapor phase adjacent to the membrane downstream face. All of
these phenomena will be discussed in the following sections.

17.2.1 NONIDEAL TRANSPORT PHENOMENA AT THE MEMBRANE
SURFACES: CONCENTRATION POLARIZATION
In Equations (17.7) and (17.8), perfect mixing of the feed bulk liquid and instant
removal of solutes leaving the membrane downstream face were assumed. If these
assumptions are not valid, boundary layers will develop on both sides of the mem-
brane, affecting the solute transport to and away from the respective membrane
surface.
When feed components sorb in the membrane, a local concentration gradient
develops in the liquid phase adjacent to the membrane upstream face. Due to this
gradient, transport of components from the bulk liquid into the liquid–membrane
interface occurs, replenishing the components sorbed in the membrane. This trans-
port of components across the liquid phase adjacent to the membrane can be either
convective or diffusive, depending on the hydrodynamic conditions over the mem-
brane surface. If the flux of a solute i across the liquid phase toward the membrane
is lower than that across the membrane, solute i will be depleted in the liquid phase
over the membrane upstream surface, resulting in a liquid solute concentration lower
than that in the bulk feed (Figure 17.3A). Because the partitioning of the solute into
the membrane is determined by the solute concentration in the liquid at the membrane
upstream surface, the concentration of i in the membrane upstream surface, Equation
(17.5), will be lower than expected according to its bulk feed concentration, as will
the concentration gradient over the membrane and hence the trans-membrane flux.
This phenomenon is denoted concentration polarization and affects mainly the fluxes
of compounds of high sorption coefficient, even under turbulent hydrodynamic con-
ditions over the membrane, as will be shown.
Under poor hydrodynamic conditions, a stagnant boundary layer forms over the
membrane in which the solute transport is purely diffusive. Similar to the mass
transport equation developed above for the solute transport across the membrane,
c mem,f
i c mem,f
i
c mem,pbl
i
mem,bl
c i
c l,bulk
i
c mem,p
i c l,bulk
i
c mem,p
i
c ip c ip
c l,bl
i
concentration membrane membrane concentration

boundary layer thickness z thickness z boundary layer
thickness δf thickness δp
(a) (b)
FIGURE 17.3 The ideal concentration profile of a solute i in the concentration boundary
layer and in the membrane for the case of concentration polarization on (A) the membrane
upstream side and (B) the membrane downstream side. The dotted line indicates the ideal
concentration profile without any concentration polarization.

the diffusive solute flux across this boundary layer can be described as
dc bl c f − cil,bl
J i = Dif ⋅ = Dif ⋅ i (17.12)
dz δ
f l,bl
where ci is the bulk liquid feed concentration of solute i, ci is the concentration of
f
solute i in the liquid adjacent to the membrane surface, Di is the diffusion coefficient
of i in the liquid boundary layer, and δ is the concentration boundary layer thickness.
Equation (17.12) implies that no solute–solute interactions occur in the boundary
layer and is therefore only valid for dilute solutions.
A similar phenomenon as described above can be found on the membrane
downstream face. Because in pervaporation one aims at employing selective mem-
branes as thin as possible for obtaining high fluxes (see Equation 17.6), most mem-
branes are composites consisting of a thin selective membrane and a macroporous
support for mechanical stability and easier handling. The macroporous support faces
the downstream compartment (Figure 17.1) and ideally should not interact with the
solutes. During pervaporation, however, the narrow pores of the support constitute
a mass transport resistance to the vacuum. This resistance results in a hindered
transport of solutes away from the membrane downstream surface, causing an
accumulation of solute in the pores of the support and hence a local increase of the
solute concentration and thus downstream pressure. Assuming thermodynamic equi-
librium at the membrane downstream face, this will cause the solute concentration
to increase in the membrane downstream surface (see Equation 17.5), resulting in
a lower concentration gradient and hence a reduced flux across the membrane.
Especially if the solute possesses a low partial pressure, the pressure drop in the
macroporous support can cause the transmembrane flux to cease totally.
17.2.2 NONIDEAL TRANSPORT PHENOMENA IN THE MEMBRANE

POLYMER: SWELLING AND FLUX COUPLING
In Equation (17.5), a Henry-type sorption of the solute in the membrane polymer was
assumed, i.e., the sorption coefficient was assumed linearly dependent on the solute
concentration. When sorbing in the membrane polymer, the solutes cause a membrane
swelling, which is the more pronounced the higher the degree of solute–polymer
interaction or the higher the solute concentration in the feed. At high solute feed
concentrations, the membrane polymer can swell to such an extent that its intrinsic
properties are significantly altered and strong nonideal interactions occur. These
interactions and the swelling of the polymer can be described for complex mixtures
by the Flory–Huggins theory (Flory, 1953; Mulder, 1991) and for binary mixtures
by the solubility parameter theory if the feed components are hydrophobic (Hilde-
brand and Scott, 1949; Mulder, 1991).
Even if the swelling of the membrane is less pronounced, it can affect the
transport of solute across the membrane. Because a vacuum is applied for the removal
of the solutes on the membrane downstream face, this side of the membrane is
ideally “dry” in comparison to the more swollen and hence more flexible membrane

upstream face resulting from the solute uptake. This anisotropy of the membrane
results in a nonuniform diffusivity of solute within the membrane, or in other words,
mem
Di will be concentration dependent and not constant across the membrane. One
way to account for this phenomenon empirically is the relationship
π i ⋅φ
Dimem = Dimem,0 ⋅ e (17.13)
mem,0
where Di is the diffusion coefficient of i in the membrane at zero concentration
(under ideal conditions), πi is the so-called plasticizing constant, which is an
empirical parameter for the degree of swelling of the membrane polymer caused
by the solute, and φI is the volume fraction of solute in the membrane polymer.
Equation (17.13) is merely empirical. A more phenomenological approach that
considers the mobility of the permeating solute as a function of the free space
available within the membrane polymer network is the free volume theory (Fujita,
1961; Fels and Huang, 1971), which has been discussed elsewhere (Huang and
Rhim, 1991).
In Equations (17.5) through (17.8) and (17.12) it is assumed that only solute–
polymer and no solute–solute interactions occur. This excludes the possibility of
synergistic effects between membrane permeants, such as flux coupling. Flux cou-
pling takes place when a permeant of low diffusivity (“slower” permeant) is dragged
through the membrane polymer by a permeant of higher diffusivity (“faster” per-
meant), resulting in higher fluxes of the slower permeant than expected. The opposite
might also happen, i.e., the slowing down of the diffusion of the faster permeant by
the slower one. The Maxwell–Stefan approach is capable of describing such nonideal
phenomena (Wesselingh and Krishna, 1990). This theory assumes that the driving
force for a solute i within a multicomponent mixture equals the sum of frictional
resistances between solutes resulting from their relative motion while diffusing
through the membrane polymer, as expressed by:
1 dµ i
n
v j − vi
⋅
RT dz
= ∑x⋅
j=1
j
D0ji
(17.14)
where dµi/dz is the local chemical potential gradient of i; xj is the mole fraction of
solutes j = 1…n, vj is the local velocities of components j = 1…n, vi is the local
0 0
velocity of i, Dji is the Maxwell–Stefan interaction parameter, with 1/Dji indicating
a friction coefficient between components j and i, R is the universal gas constant, and
T is the absolute temperature. Equation (17.14) represents the general Maxwell–Stefan
equation. Applied to the special case of solute flux across a polymer, Equation (17.14)
needs to be adapted, which is accounted for in detail elsewhere (Heintz and Stephan,
1994). The Maxwell–Stefan approach is recommended for cases in which a strong
nonideal behavior is observed because it is mathematically far more demanding than
the equations presented above. It should be stressed, however, that for nonideal
systems the Maxwell–Stefan approach might be the most elegant and efficient way
to describe the transport phenomena.

The fundamentals of pervaporation were outlined above in the most simplified
way, based on the mass conservation principle and Fick’s first law, and discussed
with regard to nonideal phenomena that may arise. Nonideal phenomena in pervap-
oration can be very complex and may demand individual solutions, which explains
why until now no general mass transport model has been developed for pervapora-
tion. To describe the mass transport across the dense membrane in a given situation,
it might therefore be best to start with the simplest approach assuming Fickian
diffusion. If, under the operating conditions of interest, nonideal mass transport
phenomena are observed, a choice can still be made between an empirical adjustment
of the ideal model or the use of a more complex structured model such as the ones
mentioned above. In the latter case, one should be aware that most of the structured
models still employ one or more empirical parameters that must be adjusted to
experimental data. In addition, the experimental effort of determining all model
parameters usually exceeds that needed for empirical models. An empirical model,
on the other hand, will only be valid within the range of operating conditions studied
and does not allow any extrapolation of the data.
17.3 TECHNICAL ASPECTS OF PERVAPORATION

A typical pervaporation set-up is depicted in Figure 17.4. The liquid feed solution is
recirculated continuously between the feed reservoir (1) and the pervaporation mod-
ule (2). Pervaporation modules can be configured in a plate-and-frame, hollow fiber,
or spiral wound mode (Rautenbach et al., 1991; Mulder, 1997; Fleming and Slater,
1992). The solutes permeating through the membrane leave the membrane down-
stream face as a vapor due to the vacuum that is established initially by the vacuum
pump (4). The phase transition of the permeating solutes from the liquid to the vapor
state goes along with heat consumption. This heat is taken up from the environment,
retentate 5
F P T
2
feed
P
1
T T permeate
4 3
fraction 2 fraction 1
FIGURE 17.4 A schematic standard pervaporation set-up. 1: feed tank; 2: pervaporation module;
3: condensation unit; 4: vacuum pump; 5: heat exchanger; F: flow control; P: pressure indicator/
control; T: temperature control.

namely the bulk feed, which consequently cools. In modules with a large membrane
area, this causes a temperature drop between the feed and the retentate and must be
compensated for. On the industrial scale, heat exchangers (5) are therefore imple-
mented in the feed circuit. In laboratory units, this temperature drop may be neglected
because the membrane area is commonly small in comparison to the recirculation
rate of the feed, which is maintained at a controlled temperature. Instead of using
a vacuum for maintaining the driving force, an inert gas can be swept over the
membrane downstream surface for the removal of the permeate solutes (sweeping
gas pervaporation). However, this mode of operation is less efficient for maintaining
the driving force, and it renders the condensation of the permeate solutes from the
sweeping gas stream more difficult.
The permeate vapor is recovered in condensers at a temperature that allows a
quantitative condensation of the vapor. The condensation can optionally be carried out
in a series of condensation stages at different temperatures in order to achieve a
permeate fractionation and increased enrichment of target compounds (3). As will be
illustrated, a careful design of the condensation strategy is indispensable and most
important in pervaporation. Once the vacuum is established, the vacuum pump (4) is
shut off and ideally the condensation unit alone maintains the vacuum. Only if non-
condensable gases permeate the membrane and enter the downstream compartment is
continuous operation of the vacuum pump required for removal of these noncondens-
able gases, which otherwise would lead to an increased downstream pressure.
Theoretically, scaling up is straightforward in pervaporation, and the fluxes
obtained on a laboratory scale can serve as a basis for the plant design on the larger
scale. However, because it is common and easy to design laboratory-scale experi-
ments close to ideal conditions, which on the larger scale would be uneconomical,
care must be taken when up-scaling laboratory experiments with regard to the
hydrodynamic conditions, the vacuum pressure, and the condensation strategy.
Industrial size plate-and-frame modules, for example, consist of a stack of tightly
packed membranes over which the feed solution is recirculated (Mulder, 1997).
The membranes are separated by spacers and the permeate withdrawn optionally
by a central permeate pipe (Stürken, 1994). Pressure losses on both the feed and
the permeate sides of the packed membranes occur and need to be accounted for in
the module design. On the feed side, the hydrodynamic conditions over the mem-
brane will be less uniform than on the laboratory scale, resulting in more pronounced
concentration polarization. On the permeate side, the packed configuration of the
membranes may constitute a mass transport resistance to the vacuum, resulting in
a downstream pressure locally higher than that measured in the main vacuum duct.
Both aspects may cause solute fluxes lower than expected and a possible shift in
selectivities.
On the laboratory scale, the permeate vapor is commonly condensed at about
77°K using liquid nitrogen. For economic reasons, the condensation temperature on
the industrial scale should be considerably higher. Because condensation efficiency
is determined by both the condenser temperature and the residence time of the
permeate vapor in the condenser, careful design of the condensation unit becomes
crucial. It should be noted that a lower downstream pressure, desirable for high
solute fluxes, goes along with a higher permeate vapor velocity in the downstream

compartment, and hence a lower residence time in the condenser. As a consequence,
either the heat exchange area or the condenser temperature must be adjusted accord-
ingly. A fractionated condensation at different condensation temperatures can sig-
nificantly increase the process performance, if the permeate composition allows
(Brüschke et al., 1992; Baudot and Marin, 1997), as it enables further product
enrichment and a more flexible and defined condensation of the permeate vapor.
In the case of coupling a pervaporation unit to an active fermentation, special
attention must be paid to noncondensable fermentation off-gases, such as carbon
dioxide from a yeast fermentation, which can permeate through the membrane in
large quantities. Using liquid nitrogen on the laboratory scale, most of these gases
are condensed. On the industrial scale, however, these gases may pass the conden-
sation unit virtually unaffected, lowering both the partial pressure and residence time
of other permeants in the condenser. The consequence can be a strongly decreased
condenser efficiency resulting in considerable loss of the more volatile permeate
vapor compounds.
The technical aspects of pervaporation as outlined above illustrate that for
process optimization all process parameters must be considered, since they strongly
affect each other. It should also be pointed out that although pervaporation is in
principle a membrane separation process, its selectivity and effectiveness may be
significantly determined by mass and heat transport phenomena occurring beyond
the membrane surfaces.
17.4 ADVANTAGES AND APPLICATIONS OF

PERVAPORATION IN THE FOOD INDUSTRY
As can be seen from the brief description of the pervaporation separation principle,
in comparison to mere evaporative techniques the membrane constitutes an addi-
tional transport resistance; however, it allows a far more selective recovery of solutes
due to solute–polymer interactions. Membrane polymers can be widely tailor made
for individual applications. One membrane polymer is barely applicable to every
imaginable separation problem, as will be shown in the following section.
17.4.1 HYDROPHILIC PERVAPORATION

The most successful application of pervaporation on the industrial scale has been
the dehydration of ethanol. Distillations of ethanol/water mixtures reach an azeotropic
point at about 95.6 wt% of ethanol. The azeotrope can only be broken and the
remaining water removed by adding entrainers such as benzene to the ethanol/water
mixture. Entrainers constitute an environmental problem as well as requiring addi-
tional downstream processing for their subsequent removal from the final product.
Using hydrophilic polyvinylalcohol (PVA) membranes, pervaporation has been
successfully coupled to distillation for water removal, yielding a final purity of
ethanol of about 99.95 wt% without the need to employ entrainers. PVA is a
crystalline or so-called glassy polymer, with the polymer chains constituting a rigid
network of little flexibility (Mulder, 1997). Both ethanol and water sorb in PVA;
however, due to its larger molecular size, the diffusivity of ethanol through the rigid

PVA network is strongly hindered in comparison to water. Because the use of glassy
polymers has been restricted so far mainly because of the selective removal of water
from organic solvents, such as dichloroethylene, isopropylalcohol, and tetrahydro-
furan, this separation has been widely referred to as hydrophilic pervaporation.
17.4.2 ORGANOPHILIC PERVAPORATION

The removal of organic compounds from aqueous solutions, also called organophilic
pervaporation, requires the use of a more flexible polymer structure. Almost all organic
compounds are of a larger molecular size than water, and their diffusivity is hindered
in glassy structures. Membranes used for the separation of organic compounds from
water are therefore of a rubbery nature, with a more flexible polymeric network.
Evidently, an eased diffusivity for the organic compounds goes along with that of
water, resulting in a considerable loss of membrane selectivity. Therefore, special
attention is given to modification of rubbery polymers so that strong solute–polymer
interactions are promoted, greatly enhancing the sorption of the organic solute in the
membrane polymer in comparison with water. For example, using a silicon rubber
membrane, a toluene/water separation factor of about 970 has been reported (Baker
et al., 1997). Using an ethylene-propylene 1,4-hexadiene copolymer (EPDM) of sim-
ilar thickness, these researchers obtained a separation factor of 33,400. This illustrates
the importance of selecting or developing the appropriate membrane for the individual
separation task.
Glassy and rubbery membranes differ strongly with regard to the flexibility of
their polymeric structure. Within the more rigid polymeric network of a glassy mem-
brane, the diffusivity of components will be strongly related to their molecular volume,
whereas in the more flexible structure of a rubbery membrane, it is less the diffusivity
that differs strongly for different components, but far more the solute–polymer inter-
action. This is why the selectivity of glassy membranes is more diffusion controlled,
while the selectivity of rubbery membranes is more sorption controlled.
In food technology, the main interest in applying pervaporation is in separating
organic compounds from an aqueous solution, i.e., the recovery of aroma compounds
(so-called bioflavors) formed by microbial fermentations and biotransformations.
Bioflavors are preferable to chemically synthesized ones due to their better public
acceptance. In addition, bioflavors often exhibit a greater aromatic diversity than their
chemically synthesized counterparts, as is the case, for example, with vanillin (Berger,
1995). Aroma concentrates are widely used as food additives to enhance the overall
flavor of foods or to compensate for the loss of aromas during food processing. They
must hence represent the organoleptic characteristics of the aroma origin as well as be
free of any harmful chemical contamination resulting from the aroma recovery process.
Traditional aroma recovery processes such as distillation, adsorption, and solvent
extraction often are discouraged because they operate at an elevated temperature that
deteriorates the aroma quality, are not environmentally friendly due to high energy
consumption and the use of toxic solvents, or involve elaborate purification steps to
remove solvent residues from the final food product (Fleming, 1992; Schreiber et al.,
1997). As a consequence, in recent years separation processes operating at gentler
temperatures and avoiding harmful extraction aids have been investigated. These include

steam distillation, air stripping (Le Thanh et al., 1993), the spinning cone column
(Wright and Pyle, 1996), supercritical carbon dioxide extraction (Jolly, 1981), and
membrane separation processes (Baudot and Marin, 1997).
Bioflavors consist of aroma compounds of very differing physicochemical prop-
erties (Berger, 1995). Hence, the in situ recovery of these aromas from a microbial
fermentation broth requires a process capable of simultaneously extracting aroma
compounds of differing chemical nature. In addition, disturbing of or interfering
with the ongoing bioconversion process should also be avoided. Thus, the recovery
process should be efficient at the bioconversion temperature, usually close to ambi-
ent, as well as recover, for example, low and high volatile compounds equally well.
Pervaporation can be operated continuously at low temperature, does not require
any extraction aid, and does not exert high stress on the active biocatalyst (Schäfer
and Crespo, 2000). It is a membrane separation process that has been extensively
studied on the laboratory scale for the recovery of flavor compounds (Baudot and
Marin, 1997; Karlsson and Träghård, 1993). Membrane fouling is a minor problem
in pervaporation because the membranes used are nonporous.
Organophilic pervaporation linked to a bioconversion process has until now
solely been studied for the recovery of individual aroma compounds or inhibiting
metabolic products (Böddeker, 1994; Lamer et al., 1996; Rajagopalan et al., 1994).
Most research on aroma recovery by organophilic pervaporation has been conducted
using aqueous aroma model solutions (Börjesson et al., 1996; Baudot and Marin,
1997), with the emphasis on the engineering aspects of pervaporation. An evaluation
of the actual organoleptic value of an aroma concentrate obtained by pervaporation
has only been reported recently (Schäfer et al., 1999).
A few examples are presented to illustrate the separation principles outlined
above, as well as to demonstrate the potential of pervaporation to respond to very
diverse aroma separation problems under well-defined operating conditions.
Based on Equation (17.4), it was mentioned that low volatile compounds can still
be recovered by pervaporation, given that their activity coefficient in the feed solution
is sufficiently high. Two examples of such low volatile compounds are γ-decalactone
(boiling point 554°K) and vanillin (boiling point 515°K). Both compounds possess
a saturated vapor pressure below 1 Pa at ambient temperature but a high activity in
aqueous solution due to their hydrophobicity.
TM
Using a PDMS GFT 1060 membrane, a silicon membrane supported by a
macroporous support, γ-decalactone was successfully recovered by pervaporation from
−1
an aqueous feed solution with an initial concentration of 100 mg·kg (Baudot et al.,
1999). However, a strong dependence of the γ-decalactone flux on the total downstream
pressure was observed (Figure 17.5). While the water flux decreased linearly with
increasing downstream pressure, the γ-decalactone flux decreased exponentially. This
observation can be explained by the differing capacity of the vacuum to remove both
the water and γ-decalactone solutes that have diffused toward the membrane down-
0
stream surface. Because γ-decalactone is very slightly volatile (Pi of γ-decalactone at
303.15°K is 0.65 Pa while that of water is 4200 Pa), a slight increase of the total
downstream pressure can cause an accumulation of γ-decalactone solutes in the
macroporous support on the membrane downstream side, and concentration polariza-
tion occurs, resulting in a lower γ-decalactone flux. On the contrary, the decrease in

150 1.5
γ-decalactone flux [ g·m ·h ]

–1
]
–2
–1
water flux [ g·m ·h
–2
100 1.0
50 0.5
0 0.0
0 500 1000 1500 2000
total permeate pressure [ Pa ]
FIGURE 17.5 The flux of water (䊊) and γ-decalactone (䊉) as a function of the total down-
stream pressure (Data from Baudot et al., J. Membrane Sci., 158(1–2), 167, 1999).
water flux with increasing total downstream pressure is solely due to a decreased
driving force within the premeate pressure range depicted.
The recovery of vanillin (Böddeker et al., 1997) by a homogeneous polyether–
block–polyamide membrane is unique in that vanillin crystallizes at ambient tem-
perature in the downstream compartment due to its high melting point, without any
need for condensation. Any other more volatile solutes permeating the membrane
pass the crystallized vanillin and can either be subsequently condensed or discarded.
It should be noted that for such a demanding separation problem composite mem-
branes cannot be used, as the pressure loss within the macroporous support can be
sufficient to cause the condensation of vanillin at the membrane downstream face.
While most applications of pervaporation deal with the removal of single aroma
compounds, little has been reported on the recovery of a distinct aroma profile. An
example of such an aroma profile is that of a muscatel wine formed during the
vinification process. The aroma produced by yeast during wine must fermentation
comprises up to 800 aroma compounds (Rapp, 1990), which makes it a challenge to
recover aromas without altering their organoleptic quality. Using a polyoctylmethyl-
siloxane–polyetherimide (POMS–PEI) composite membrane, a muscatel wine must
aroma concentrate can be obtained that is faithful to its origin and of high organoleptic
value according to sensory panel evaluation (Schäfer et al., 1999).
With the aroma profile of muscatel wine must consisting of a subtle balance
among individual aroma compounds of varying physicochemical properties, it is not
obvious that their transport across the membrane polymer results in an aroma
concentrate organoleptically faithful to the aroma of the feed solution. In fact, it has
been observed that concentration polarization phenomena on the feed side strongly
affect the permeate composition (Figure 17.6). Based on the equations presented above,
the water-free mass fraction of four representative aroma compounds in the permeate,
ethyl acetate, ethyl butanoate, ethyl hexanoate and linalool, was simulated as a

permeate mass fraction [ % ]
60
40
20
0
0.01 0.1 1 10
ratio boundary layer/membrane thickness [ ]
FIGURE 17.6 The permeate mass fraction in wt% as a function of the ratio boundary layer/
membrane thickness. The permeate composition is calculated on a water-free basis for a dilute
aqueous feed solution of ethyl acetate (solid), ethyl butanoate (dotted), ethyl hexanoate (long
dash), and linalool (short dash).
function of the hydrodynamic boundary layer/membrane thickness on the basis of

their sorption coefficient Si, as well as their diffusion coefficients in water and the
membrane. Of the compounds investigated, ethyl hexanoate showed the highest
affinity for the membrane polymer and ethyl acetate the lowest. Diffusion coefficients
varied slightly among the compounds, however, to a much lesser extent than their
respective sorption coefficients. As can be seen in Figure 17.6, only below a boundary
layer/membrane thickness ratio of about 0.01 does the permeate mass fraction remain
constant. In other words, if a membrane of 20 µm thickness is used during pervapo-
ration, the hydrodynamic boundary layer thickness should be less than 0.20 µm in
order to avoid any shift in the permeate mass fraction due to concentration polarization.
Highly turbulent conditions are hence required over the membrane. Less turbulent
conditions will lead to a thicker hydrodynamic boundary layer, resulting in a shift in
the permeate mass fraction, as is indicated by the dotted vertical lines in Figure 17.6.
17.5 CONCLUSIONS
The principles of pervaporation and its advantages for the recovery of volatile
compounds from bioconversions in particular have been presented and discussed. It
has been shown that pervaporation is a versatile process that should be understood
as a whole, and the process components of which can be adapted to individual separation
problems. This versatility allows the invention of novel, tailor-made process strate-
gies differing from the standard process design as depicted in Figure 17.4. One
might, for example, think of alternative methods for capturing aroma compounds in
the vapor permeate. The vapor permeate does not necessarily have to be condensed
before the vacuum pump. Using liquid ring vacuum pumps, it may be condensed in
the pump itself. Using dry vacuum pumps, it may be captured after the pump under
a higher pressure than that of the vacuum. This opens the possibility of conceiving

various alternatives for capturing aromas, such as the recovery of the aromas in an
adsorptive matrix resulting immediately in a final product, as for example for appli-
cations of controlled release. Likewise, other steps during the pervaporation process
may be optimized and adapted for an individual separation problem.
REFERENCES
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concentration polarization on the separation of volatile organic compounds from water
by pervaporation, J. Membrane Sci., 137, 159–172, 1997.
Baudot, A. and Marin, M., Pervaporation of aroma compounds: comparison of membrane
performances with vapor–liquid equilibria and engineering aspects of process
improvement, Trans. IChemE., 75C, 117–142, 1997.
Baudot, A., Souchon, I., and Marin, M., Total permeate pressure influence on the selectivity
of the pervaporation of aroma compounds, J. Membrane Sci., 158, 167–185, 1999.
Berger, R.G., Aroma Biotechnology, Springer, Berlin, 1995.
Böddeker, K.W., Recovery of volatile bioproducts by pervaporation, in Membrane Processes
in Separation and Purification, Crespo, J.G. and Böddeker, K.W., Eds., Kluwer,
Dordrecht, The Netherlands, 1994, pp. 195–207.
Böddeker, K.W., Gatfield, I.L., Jähnig, J., and Schorm, C., Pervaporation at the vapor pressure
limit: vanillin, J. Membrane Sci., 137, 155–158, 1997.
Börjesson, J., Karlsson, H.O.E., and Trägårdh, G., Pervaporation of a model apple juice
solution: comparison of membrane performance, J. Membrane Sci., 119, 229–239,
1996.
Brüschke, H.E.A., Schneider, W., and Tusel, G.F., Patent DE 3804236C2, 1992.
Fels, M. and Huang, R.Y.M., Theoretical interpretation of the effect of mixture composition
on separation of liquids in polymers, in Permselective Membranes, Rogers, C.E., Ed.,
Dellke Inc., New York, 1971, pp. 89–97.
Fleming, H.L., Consider membrane pervaporation, Chem. Eng. Proc., 7, 46–52, 1992.
Fleming, H.L. and Slater, C.S., Pervaporation: design, in Membrane Handbook, Ho, W.S. and
Sirkar, K.K., Eds., Chapman and Hall, New York, 1992.
Flory, P.J., Principles of Polymer Chemistry, Cornell University Press, Ithaca, NY, 1953.
Fujita, H., Diffusion in polymer–diluent systems, Fortschr. Hochpolym. Forschung, 3, 1–47,
1961.
Heintz, A. and Stephan, W., A generalized solution–diffusion model of the pervaporation
process through composite membranes, Part II. Concentration polarization, coupled
diffusion and the influence of the porous support layer, J. Membrane Sci., 89,
153–169, 1994.
Hildebrand, J.H. and Scott, R.L., The Solubility of Non-Electrolytes, Plenum Press, New York,
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Huang, R.Y.M. and Rhim, J.W., Separation characteristics of pervaporation membrane sepa-
ration processes, in Pervaporation Membrane Separation Processes, Huang, R.Y.M,
Ed., Elsevier, Amsterdam, 1991, pp. 111–180.
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Aug/Sept 1981, pp. 36–40.
Karlsson, H.O.E., and Träghård, G., Pervaporation of dilute organic–water mixtures. a liter-
ature review on modelling studies and applications to aroma compound recovery,
J. Membrane Sci., 76, 121–146, 1993.

Lamer, T., Spinnler, H.E., Souchon, I., and Voilley, A., Extraction of benzaldehyde from
fermentation broth by pervaporation, Process Biochem., 31, 533–542, 1996.
Lawson, K.W. and Lloyd, D.R., Membrane distillation, J. Membrane Sci., 124, 1–25, 1997.
Le Thanh, M., Voilley, A., and Tanluu, R.P., The influence of the composition of model liquid
culture medium on vapor liquid partition coefficient of aroma substances, Sci. Ali-
ment., 13, 699, 1993.
Lee, C.H., Theory of reverse osmosis and some other membrane permeation operations,
J. Appl. Polym. Sci., 19, 83–95, 1975.
Luque de Castro, M.D. and Gámiz-García, L., Analytical pervaporation: an advantageous
alternative to headspace and purge-and-trap techniques, Chromatographia, 52,
265–272, 2000.
Mulder, M., Basic Principles of Membrane Technology, Kluwer, Dordrecht, 1997.
Mulder, M.H.V., Introduction to pervaporation, in Pervaporation Membrane Separation Pro-
cesses, Huang, R.Y.M., Ed., Elsevier, Amsterdam, 1991, pp. 1–86.
Néel, J., Thermodynamic principles of pervaporation, in Pervaporation Membrane Separation
Processes, Huang, R.Y.M., Ed., Elsevier, Amsterdam, 1991, pp. 225–251.
Rajagopalan, N., Cheryan, M., and Matsuura, T., Recovery of diacetyl by pervaporation,
Biotechnol. Tech., 8, 869–872, 1994.
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perception, Fresenius J. Anal. Chem., 337, 777–785, 1990.
Rautenbach, R., Herion, C., and Meyer-Blumenroth, U., Engineering aspects of pervaporation:
calculation of transport resistances, module optimization and plant design, in Per-
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dam, 1991, pp. 225–251.
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Biotechnol. Bioeng., 62, 412–421, 1999.
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Ultrasonic Mass Transfer
18 Enhancement in Food
Processing
A. Mulet, J. Cárcel, J. Benedito, C. Rosselló,
and S. Simal
CONTENTS
18.1 Introduction
18.2 Generation Methods of Power Ultrasound
18.3 Applications
18.3.1 Gas–Solid Mass Transfer Process
18.4 Liquid–Solid Mass Transfer Process
18.4.1 Influence of the Material Treated
18.4.2 Influence of Ultrasound Intensity
18.5 Conclusions
Nomenclature
References
18.1 INTRODUCTION
High intensity ultrasound produces a variety of effects, such as radiation pressure,
streaming, cavitation, and interface instabilities. These effects can influence mass
transfer processes by producing changes in concentration gradients, diffusion coef-
ficients, or boundary layer (Liang, 1993). Heating produced by absorption of ultra-
sonic energy (thermoacoustic effect) can also affect mass diffusion.
The transducers most commonly used to generate high intensity ultrasound are
piezoelectric (Mason, 1998). Based on this technique, ultrasonic cleaning baths are
the commercial systems where most experimental results have been obtained and
published in the literature. Ultrasonic probe systems with mechanical amplifiers are
also used when it is necessary to concentrate the generated acoustic energy. These
two methods used to produce ultrasound are suitable for treatments in a liquid
environment. Another arrangement of transducers is required for applications in
gaseous media, due to their low density, and is responsible for their low specific
acoustic impedance.

In order to control a process, it is necessary to measure the main parameters. In
ultrasonic applications, the amount and characteristics of the energy applied need
to be known. The measurement of power and frequency enables not only a correct
evaluation of the importance of these factors in the process, but also the appropriate
process control.
The use of high intensity ultrasound has been considered to enhance mass transfer
for different products and processes such as brining of meat (Sajas and Gorbatow,
1978) and cheese (Sánchez et al., 1999), drying of rice (Muralidhara et al., 1985) and
carrots (Gallego-Juárez et al., 1999), osmotic dehydration of apples (Floros and Liang,
1994; Simal et al., 1998), and extraction processes of several products such as pectin
from apples (Panchev et al., 1988), chymosin from the fourth stomach of milk-fed
calves to manufacture cheese (Kim and Zayas, 1991), bioactive principles from plant
materials (Vinaturo et al., 1997), and even extractions with supercritical fluids (Jun
et al., 1997).
The aim of this work is to examine the application of high intensity ultrasound
to mass transfer processes. Four cases are analyzed to show the influence of trans-
mission medium and the material considered. Three are applications in a liquid
medium and the fourth is in a gaseous medium. The cases in a liquid medium are:
a structured material, microscopically isotropic and with a large quantity of air-filled
pores (osmotic dehydration of apple); a low structured, macroscopically isotropic
material with a large quantity of liquid-filled pores (pressed cheese curd in brine,
an intermediate product in some cheese manufacturing processes); and a highly
structured, anisotropic material with low porosity (pork loin in brine). For the mass
transfer process in a gaseous medium, a structured vegetal, nonisotropic material
with partially air-filled pores will be considered (carrot dried with hot air).
18.2 GENERATION METHODS OF POWER

ULTRASOUND
Piezoelectric transducers convert a high frequency alternating current into mechan-
ical vibrations. The most common applications of power ultrasound in mass transfer
processes take place between a solid and a liquid medium. For these cases, ultrasonic
cleaning baths are the most commonly used commercial equipment. In ultrasonic
baths, the transducers are attached to the bottom of the bath. When they start to
oscillate, vibrations are transmitted into the liquid. Standing waves are created by
reflection of the emitted sound waves at the liquid/air interface. High and low
intensities are obtained at fixed levels (half wavelength) throughout the bath depth.
As a consequence, the ultrasonic field formed inside a bath is irregular and influenced
by liquid height and the introduced loading (Figure 18.1).
The technology of ultrasonic probe systems is also based on piezoelectric trans-
ducers. A “horn” is attached to a piezoelectric sandwich transducer in order to
amplify the generated acoustic energy. The length of the horn is generally a half
wavelength (or a multiple). The horn shape makes it possible to concentrate the
ultrasonic energy. The gain for a given form of the horn is defined by a specific
ratio of the diameter of the two faces of the horn. If D is the driven face and d is
the emitting face for an exponential horn, the ratio is D/d. This means that for a

2.8
Hydrophone Transducers
2.6
Acoustic pressure (bar) 2.4 Out
2.2
2.0
1.8
1.6
1.4
1.2 Water
surface
1.0
0 5 10 15 20
Distance from the bottom (cm)
FIGURE 18.1 Example of the acoustic pressure variation vs. the distance from the bottom
in an ultrasonic bath.
uniform cylinder there is no gain in wave amplitude, but rather the horn acts as an
extender for the transference of the acoustic energy. For a stepped horn, the gain
2
is (D/d) .
Horns are generally made of titanium due to the high resistance of this material
to fatigue and erosion. The erosion of the transmitter surface causes a fall in the
power. Variation in horn length can affect the frequency.
For applications of power ultrasound in gaseous media, the most important
problems are related to the efficient generation and transmission of ultrasonic energy.
It is necessary to achieve ultrasonic generators that meet the following requirements:
good impedance matching with the air, large amplitude of vibration, high directional
radiation, and high power capacity. In addition, for large-scale industrial applications,
extensive radiating area would be required in the transducers. Presently, no com-
mercial transducers meeting all the aforementioned conditions are available.
A new type of ultrasonic generator has recently been developed (Gallego-Juárez
et al., 1989). It is comprised of a transducer with a stepped-plate radiator and an
electronic unit for driving the transducer (Figure 18.2). The design of the stepped profile
of the radiating plate allows control of the vibration and radiation pattern, thus
permitting distribution of the vibration amplitude and, consequently, the acoustic
field, according to the needs of the specific application. The signal frequency can
slide during operation in association with changes in the mechanical load. Keeping
the voltage and current signals in the transducer in phase, a specifically designed
electronic circuit can automatically correct the frequency of the generated signal so
that the electronic system drives the transducer by producing a signal within the
very narrow band corresponding to the resonance frequency of the transducer.

Radiating
plate Piezoelectric
ceramics
Mechanical
Sandwich
amplifier
FIGURE 18.2 Structure of the stepped-plate transducer. (From Gallego-Juárez, J.A. et al.,
Drying Technol., 17, 597–608, 1999, courtesy of Marcel Dekker.)
One important point in the use of high intensity ultrasound is the power mea-
surement. Due to problems of sonic wave reflections and the wearing out of trans-
mitters, the power and frequency applied to samples may be modified. Hydrophones
can supply local information on the acoustic pressure and frequency (Pugin and
Turner, 1990). The signal created by a hydrophone may be captured and treated
through an oscilloscope. This allows characterization of the acoustic field and iden-
tification of standing waves, high and low intensity zones, etc.
A calorimetric method is another way to measure the input of the acoustic power
into a medium. The method consists of the measurement of the temperature rise
against the time in adiabatic conditions when ultrasound is applied (Margulis and
Maximenco, 1990). The average power absorbed is:
dT
P = mC p
dt
where m is the liquid mass treated, Cp is the heat capacity and dT/dt is the variation
of temperature T with time t that can be approximated by ∆T/∆t. As can be seen in
Figure 18.3, there is a linear temperature increase. These unpublished data corre-
spond to the results of experiments performed by the authors.
A good correlation between acoustic pressure measured by a hydrophone and
power estimated through the rate of the temperature increase was found
(Figure 18.4). The measurements were carried out in a 600 ml glass beaker with
400 ml saturated brine. The starting temperature was the same in all cases (3°C).
18.3 APPLICATIONS
18.3.1 GAS–SOLID MASS TRANSFER PROCESS
Drying carrots is an example of mass transfer from a solid medium to a gas medium.
Gallego-Juárez et al. (1989) carried out experiments drying carrots with and without
application of airborne ultrasound. A special generator unit and a stepped plate were

6
Temperature of the medium (°C)

5
3
Start of the ultrasound
application
2
0
0 50 100 150 200 250
Time (sec)
FIGURE 18.3 Temperature increase with application of ultrasound with a sound probe system.
20
Calorimetric measurement (W/cm2)
18
16
14
12
10
8
y = 33.922x – 18.22
6
R2 = 0.9958
4
2
0.5 0.7 0.9 1.1 1.3
Hydrophone pressure (bar)
FIGURE 18.4 Correlation between power ultrasound estimation by a calorimetric method

and measurement of the acoustic pressure with a hydrophone.
used (Gallego-Juárez, et al. 1989). The experimental tests mainly consisted of mea-
suring the water content of food samples after different times of application of high-
intensity ultrasonic fields in combination with forced air at various temperatures and
flow velocities. In all experiments, the frequency was kept constant at about 20 kHz
while different sound pressure levels were applied. The experimental set-up can be
seen in Figure 18.5.
Different drying temperatures, air velocities, and power ultrasound were used.
From data published by Gallego-Juárez et al. (1998), it is possible to calculate an

TABLE 18.1
Diffusivities Calculated for Dehydration with and
without Airborne Ultrasound
−6 2
Experiment Diffusivity × 10 (m /h)
T = 60°C; Without ultrasound 2.67

T = 60°C; With ultrasound 4.86
T = 90°C; Without ultrasound 6.22
T = 90°C; With ultrasound 7.74
T = 115°C; With and without ultrasound 11.35
Source: Data from Gallego-Juárez et al. (1998).

Air velocity (V) = 1.3 m/sec; carrot samples 14 mm × 2 mm
Transducer
Electronic
generator
Sample Vibrating
Hot air plate
generator
Support
plate
FIGURE 18.5 Experimental set-up for forced air drying assisted by airborne ultrasound.
(From Gallego-Juárez, J.A. et al., Drying Technol., 17, 597–608, 1999, courtesy of Marcel
Dekker.)
effective diffusivity of water. For that purpose, a diffusive model for carrots proposed
by Mulet (1994) was used. The less complex model was chosen for its simplicity.
It was assumed that the solid temperature was constant and equal to drying air
temperature and that the diffusivity was constant during drying experiments; the
shrinkage was not considered. The model is valid if external resistance to mass
transfer is negligible. Mulet et al. (1987) indicated that the air flow had no influence
2
on carrot drying rate when greater than 6000 kg/hm (≈1.29 m/sec). Mitchell and
2
Potts (1958) fixed this flux limit at 4200 kg/hm (≈0.9 m/sec). The analyzed exper-
iments were carried out at constant air velocity of 1.3 m/sec, hence the process was
controlled by internal resistance. The diffusivities were calculated from Gallego-
Juárez et al.’s results and are shown in Table 18.1. The values are similar to those
−6
found in the literature. Mulet (1994) reported an effective diffusivity of 6.3 × 10
2 2
m /h for carrot cubes using an air flow of 8000 kg/hm at 60°C through drying.
The obtained values showed that under similar conditions the carrot diffusivity
in experiments carried out with ultrasound was higher than in experiments without

Transducer
Electronic
generator
Hot air Samples Vibrating

generator plate
Suction
Support system
plate
Drain
channels
Static
pressure
FIGURE 18.6 Experimental set-up for dehydration by directly coupled ultrasonic vibration.
(From Gallego-Juárez, J.A. et al., Drying Technol., 17, 597–608, 1999, courtesy of Marcel
Dekker.)
ultrasound. When the drying air temperature increased, the relative influence of
ultrasound decreased. For an air temperature of 115°C, Gallego-Juárez (1998) did
not find differences between applying and not applying ultrasound. The ultrasound
pressure levels used by these authors were 155 and 163 dB. No important differences
in sample water content were found between samples dehydrated under these acous-
tic pressures. Significant differences were found only in the fast-drying zone (i.e.,
the first 10 min).
The main difficulty in dehydration by airborne ultrasonic radiation is the low
penetration of the acoustic energy into the food material due to the mismatch between
acoustic impedances. Acoustic impedance is defined as the product of density and
sound speed in the material. When ultrasonic waves arrive at the air–material interface,
a high percentage of their energy is reflected due to impedance differences between
gas and solid. In order to avoid this problem, Gallego-Juárez et al. (1999) carried out
another kind of experiment. A stepped-plate transducer was applied to the product
directly, and static pressure was simultaneously exerted on the samples (Figure 18.6).
To facilitate water removal, an air flow of 1 m/sec at 22°C was applied. Assuming again
that internal resistance controls the process, an effective diffusivity using the afore-
−6 2
mentioned model can be calculated. The result was 21.92 × 10 m /h. This diffusivity
was higher than that found in 115°C drying air temperature experiments. In fact, the
drying process is more powerful, since the final moisture of the samples could be less
than 1% (Gallego-Juárez et al., 1999). These results show that this procedure may be
useful for food products with components sensitive to high temperature.
The main mechanism involved may be the “sponge effect.” Ultrasound produces
contractions and expansions of the material, and water is forced to exit from the
vegetal matrix. Additionally, the acoustic stress may create microchannels that assist
the water evacuation.

18.4 LIQUID–SOLID MASS TRANSFER PROCESS
18.4.1 INFLUENCE OF THE MATERIAL TREATED
In ultrasound application in liquid media, an important parameter that should be
kept in mind is the viscosity of the liquid. If this is high, the ultrasonic energy may
be absorbed within a few centimeters from the emitters (Mason and Cordemans,
1996). The surface tension is another important factor, since it can prevent the
appearance of cavitation phenomena.
The solid material processed (in a liquid) is another factor to be considered when
examining the effects produced by ultrasound.
Simal et al. (1998) studied ultrasound influence (0.81 ± 0.17 bar; 40 kHz) in
osmotic dehydration of apples at different temperatures. Water loss and sucrose gain
were measured in apple cube samples at different times during the osmotic process.
The results showed an acceleration of water loss and sugar gain rate when ultrasound
was applied. In Figure 18.7, the differences between experiments with agitation of
osmotic solution and with ultrasound are shown.
The difference in water content after 3 h of treatment was approximately 25% lower
in the ultrasonic experiment. The increase of dry matter in ultrasonic treatment relative
to agitation experiments was about 40% at 50°C and 15% at 70°C after 3 h. Simal et al.
(1998) found that the solute gain was more important at 40°C with ultrasonic application
than at 70°C with agitation.
Sánchez et al. (1999) carried out experiments on pressed cheese curd brining,
an intermediate process in some types of cheese manufacture. Three kinds of brining
100
Difference (%) between ultrasonic and
80
60
agitation brining
40
20
-20
-40
0 2000 4000 6000 8000 10000 12000
Time (sec)
FIGURE 18.7 Difference (% d.m.) in water content and solute content between ultrasonic
and agitation experience for apple osmotic dehydration. 50°C, solute content; 70°C,
solute content; 50°C, water content; 70°C, water content. Difference = 100 × (content
with ultrasound − content with agitation)/content with ultrasound.

30
25
Difference (%) between ultrasonic and static

20
15
brining 10
-5
-10
-15
-20
0 2000 4000 6000 8000 10000 12000
Time (sec)
FIGURE 18.8 Difference (% d.m.) in water content and solute content between ultrasonic
and static brining of pressed cheese curd. 5°C, solute content; 10°C, solute content;
5°C, water content; 10°C, water content. Difference = 100 × (content with ultrasound–
content in static conditions)/content with ultrasound.
were tested: with brine agitation (dynamic conditions); without brine agitation (static
conditions); and with applications of ultrasound. An ultrasonic cleaning bath was
used as an ultrasonic generator (1.7 ± 0.22 bar; 30 kHz). The difference between
ultrasonic and static conditions in 5 and 10°C experiments are shown in Figure 18.8.
In this case, the decrease in water content was more important than the increase of
solute content.
Both processes (osmotic dehydration of apples and pressed cheese curd brining),
with and without ultrasonic applications, fitted well to a diffusional model (Simal
et al., 1998; Sánchez et al., 1999), thus an effective diffusivity can be calculated.
The Arrhenius equation was adequate to model temperature influence on diffusivity
in all cases except for solute gain in osmotic dehydration of apple. The fact that
apple cubes osmotically treated at different temperatures gained similar amounts of
sucrose during the drying process could indicate that the main mechanism involved
in sucrose transfer from the osmotic solution into the solid when sonication was
used was not of a diffusional nature. A different mechanism for solute gain should
be explored. As can be seen in Figures 18.7 and 18.8, the difference of solute and
water between ultrasonic and nonultrasonic experiments had distinct behavior.
Apple is a porous product with partially air-filled pores. Pressed curd is also a
porous product, but its pores are filled with liquid. In osmotic dehydration of apple,
the sponge effect, produced by ultrasound, forces the occluded air in the pores to
exit. Then the osmotic solution enters the pores. Ultrasound produces a pressure
assisted osmotic dehydration. Positive and negative pressures occur with the same
frequency as the ultrasound is applied. The entry of solution into the apple matrix

produces an important increase of sugar in ultrasonic assisted osmotic dehydration
according to a mechanism other than diffusion.
Similar results were obtained by Shi and Fito (1993). These authors found that
although an increase in the solution temperature had a favorable effect on the rate
of water diffusion, no significant influence of temperature on sugar gain could be
observed in apricot and pineapple samples treated through vacuum osmotic dehy-
dration. This could explain the lack of influence of temperature on the sugar gain
process.
The proportion of air in cheese pores is lower than that in apple pores. Thus, the
influence of ultrasonic compressions and expansions is less important. In the first
stages of brining, the pore air is “liberated” by ultrasound. Then the differences with
regard to static conditions of brining are important. When there is no air in the pores,
the effect of ultrasound decreases. Chiralt and Fito (1996) found in vacuum impreg-
nation of Manchego cheese that during vacuum treatment the outflow of gas involved
a residual whey release as well, because it was interchanged with brine during the
inflow of the external liquid step when atmospheric pressure was restored. This could
be the reason that the difference in salt content between ultrasonic and nonultrasonic
experiments remains after the first stage of brining in the time span considered.
Another factor that may explain the different behavior between apple and cheese
could be their different structure. The rigid structure of apples makes them a better
ultrasonic vibration conductor than cheese, which presents a “rubbery” structure where
the ultrasound waves are more easily absorbed.
In both cases, apple and cheese, the water content decreased in experiments with
ultrasound more quickly than in experiments without ultrasound. For the time spans
considered, the difference in water content between ultrasonic and nonultrasonic
experiments increased with the time of treatment. The ultrasonic waves could pro-
duce microcurrents in the solid–liquid interface that cause an increase of diffusion
coefficients and a decrease of the boundary layer of diffusion. Therefore, the water
loss process may be influenced by ultrasound waves due to their effect on external
resistance or/and internal resistance.
18.4.2 INFLUENCE OF ULTRASOUND INTENSITY

The effects produced by ultrasound in mass transfer processes are influenced by the
intensity applied. Several authors have described the existence of an intensity thresh-
old; for lower intensities no ultrasound effects were observed. Arkhangel’skii and
Statnikov (1973) found that this threshold in acoustic evaporation was about 140 dB.
The effect of acoustic streaming becomes greater than the influence of natural
convection. High intensity produces high acoustic vibration, more violent cavitation,
and greater microstreaming; thus the influence of ultrasound is intensified.
In order to show ultrasound intensity effects, Cárcel et al. (1999) carried out
several brining experiments using pork. Loin pork was brined in a NaCl-saturated
brine for 45 min. Experiments were performed with and without ultrasound appli-
cation. In the case of ultrasonic brining, nonexternal agitation was applied to the
brine. In nonultrasonic brining, the experiments were carried out with and without
brine agitation. For ultrasonic experiments, two types of generators were used: an

TABLE 18.2
Mean Values and Confidence Intervals (95%) for
Salt Gain in Pork Loin after 45 Minutes of Brining
Experiment g NaCl/g Initial Dry Matter
Nonultrasonic without agitation 0.16 ± 0.08

Nonultrasonic with agitation 0.18 ± 0.08
Ultrasonic bath 0.18 ± 0.06
Sound probe system 0.38 ± 0.08
ultrasonic cleaning bath and a probe system. The acoustic pressures applied with
the bath and with the probe system were 0.81 ± 0.05 bar (40 kHz) and 1.07 ± 0.20
bar (20 kHz), respectively. During brining, the temperature of the brine was main-
tained at a constant 2.0 ± 0.5°C. Final moisture and salt gain were measured. For
every type of salting, at least three replications were carried out. In experiments
with brine agitation, a strong stirring was used to create negligible external resistance
to mass transfer.
An ANOVA was performed on the final moisture and NaCl gain of samples in
the different experiments. Four groups of experiments were considered (nonultra-
sonic and nonagitation, nonultrasonic and agitation, using an ultrasonic bath, and
using a sonic probe system treatment).
For final moisture content, at a 95% level of confidence, no differences between
different brining groups were observed. However, the experiments carried out with
a probe system showed a higher final moisture, and at the 90% level of confidence,
this group was significantly different.
On the other hand, significant differences were found for salt gain between
groups (95%), as can be seen in Table 18.2. The samples treated with the sound probe
system gained more NaCl than the others. No differences were found between
agitation, nonagitation brine, and ultrasound applied by means of the ultrasonic bath.
Treatments in an ultrasonic bath consisted of the application of an ultrasonic
energy in a volume of liquid. The fact is that all carcasses vibrate to produce an
ultrasonic field more or less irregular in all quantities of liquid contained. The sound
probe system can generate a high intensity field in a small zone and then produce
an ultrasonic field when focused. Just below the probe tip, the maximum ultrasonic
power is generated. If a sample is placed at this point, it receives a large amount of
the acoustic pressure emitted.
Pork loin is not a porous material, so the effects of ultrasound are less important
than for other foods. According to the literature, when the intensity of ultrasound is
above the threshold, the salt gain should be increased with respect to the nonultrasonic
brining. In that case, the effects created by ultrasound become important when the
intensity is sufficient. Only then, microstreaming, contractions and expansions of mate-
rial, cavitation, etc., force the entry of salt into the meat matrix. However, this high
intensity seems to affect the exit of water from the pork loin, an effect different from
the one found in apple and cheese osmotic dehydration, where an increase in water loss
was observed.

18.5 CONCLUSIONS
High intensity ultrasound enhances the mass transfer process, affecting internal as well
as external resistance to mass transfer. The propagating medium, material treated, and
intensity applied can influence the effects produced by ultrasound. Different technol-
ogies are needed for applications in gas and liquid media. Stepped-plate transducers
generate the intensity to accelerate the drying of carrots with air. The decrease of the
boundary layer and successive contractions and expansions produced by ultrasound
aid water exit from carrot matrix. In liquid applications, mass transfer is also improved.
Water loss in osmotic dehydration of apple and cheese brining is increased by appli-
cations of ultrasound. The material structure also affects the influence of ultrasound.
The removal of air from apple pores is assisted by ultrasound, and the air is replaced
by osmotic solution. Thus, solute increase in a solid matrix is very important. Cheese
pores have less air occluded and, as a consequence, the influence of ultrasound on
solute gain is less important. Additionally, apple structure better transmits ultrasound
than does cheese. Pork loin has no large pores, and therefore mass transfer is difficult.
Nonsignificant differences appear between applications of ultrasound by means of a
commercial cleaning bath and agitation or nonagitation brine experiments. Higher
ultrasonic intensity generated by a probe system accelerated salt gain. This shows the
existence of a threshold where the influence of ultrasound appears. Commercial baths
do not usually reach this threshold for some products, and no differences appear, as
reported in the literature. High intensities applied to meat increase salt gain and make
water loss difficult. These effects could lead to an increase in the process efficiency.
NOMENCLATURE
D Diameter of driven face of a transductor; m
d Diameter of emitting face of a transductor; m
P Power; W
m Mass; kg
Cp Heat capacity; J/kg°C
T Temperature; °C
t Time; sec
REFERENCES
Arkhangel’skii, M.E. and Statnikov, Y.G., The action of ultrasonic vibrations on diffusion, in
Physical Principles of Ultrasonic Technology, Vol. 2, Rozenberg, L.D., Ed., Plenum
Press, New York, 1973.
Cárcel, J.A., Benedito, J., Llull, P., Clemente, G., and Mulet, A., Influence of Ultrasound in
Meat Brining, Proceedings of AICHE-CoFE 99, Dallas, November 2–5, 1999, pp.
163–170.
Chiralt, A. and Fito, P., Salting of Manchego-type cheese by vacuum impregnation, in Food
Engineering 2000, Chapman and Hall, New York, 1996, pp. 215–230.
Floros, J.D. and Liang, H., Acoustically assisted diffusion through membranes and bio-
materials, Food Technol., December 1994, pp. 79–84.

Gallego-Juárez, J.A., Some applications of air-borne power ultrasound to food processing, in
Ultrasound in Food Processing, Povey, M.J.W. and Mason, T.J., Eds., Blackie, Glas-
gow, 1998, pp. 127–143.
Gallego-Juárez, J.A., Rodriguez-Corral, G., Gálvez-Moraleda, J.C., and Yang, T.S., A new
high-intensity ultrasonic technology for food dehydration, Drying Technol., 17,
597–608, 1999.
Gallego-Juárez, J.A., Rodríguez-Corral, G., San Emetano, J.L., and Montoya-Vitini, F., Elec-
troacoustic unit for generating high sonic and ultrasonic intensities in gases and
interphases, Spanish patent 8903371, 1989; European patent No. EP 450.030.A1,
1991; U.S. patent No. 5,299,175, 1994.
Jun, C., Kedie, Y., Shulai, C., Adschiri, T., and Arai, K., Effects of Ultrasound on Mass
Transfer in Supercritical Extraction, The 4th International Symposium on Supercrit-
ical Fluids, Sendai, Japan, May 11–14, 1997, pp. 707–710.
Kim, S.M. and Zayas, J.K., Effects of ultrasound treatment on the properties of chymosin, J.
Food Sci., 56, 926–930, 1991.
Liang, H., Modelling of ultrasound assisted and osmotically induced diffusion in plant tissue,
thesis, Purdue University, Lafayette, IN, 1993.
Margulis, M.A. and Maximenco, N.A., Appendix: measurement of ultrasound-absorbed power
(calorimetric methods), in Advances in Sonochemistry, Vol. 2, Mason, T.J., Ed., JAI
Press, London, 1990, pp. 288–289.
Mason, T.J., Power ultrasound in food processing: the way forward, in Ultrasound in Food
Processing, Povey, M.J.W. and Mason, T.J., Eds., Blackie, Glasgow, 1998, pp. 105–
126.
Mason, T.J. and Cordemans, E.D., Ultrasonic intensification of chemical processing and
related operations: a review, Trans. IchemE., 74, 511–516, 1996.
Mitchell, T.J. and Potts, C.S., Through-circulation drying of vegetables. III. Carrots, J. Sci.
Food Agric., 9, 93–98, 1958.
Mulet, A., Drying modelling and water diffusivity in carrots and potatoes, J. Food Eng., 22,
329–348, 1994.
Mulet, A., Berna, A., Borrás, M., and Piñaga, F., Effect of air flow rate on carrot drying,
Drying Technol., 5, 245–258, 1987.
Muralidhara, H.S., Ensminger, D., and Putnam, A., Acoustic dewatering and drying (low and
high frequency): state of the art review, Drying Technol., 3, 529–566, 1985.
Panchev, I., Kirchev, N., and Kratchanov, C., Improving pectin technology. II. Extraction
using ultrasonic treatment, Int. J. Food Sci. Technol., 23, 337–341, 1988.
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Sonochemistry, Vol. 1, Mason, T.J., Ed., JAI Press, London, 1990, pp. 81–118.
Sajas, J.F. and Gorbatow, W.M., Use of ultrasound in meat technology, Fleischwirtschaft, 58,
1009–1021, 1978.
Sánchez, E.S., Simal, S., Femenia, A., Benedito, J., and Rosselló C., Influence of ultrasound
on mass transport during cheese brining, Eur. Food Res. Technol., 209, 215–219, 1999.
Shi, Q.S. and Fito, P. 1993. Vacuum osmotic dehydration of fruits, Drying Technol., 11,
1432–1442, 1993.
Simal, S., Benedito, J., Sánchez, E.S., and Rosselló, C., Use of ultrasound to increase mass
transport rates during osmotic dehydration, J. Food Eng., 36, 323–336, 1998.
Vinatoru, M., Toma, M., Radu, O., Filip, P.I., Lazurca, D., and Mason T.J., The use of
ultrasound for the extraction of bioactive principles from plant materials, Ultrason.
Sonochem., 4, 135–139, 1997.

Mass Transfer and
19 Residence Time Studies in
Spinning Cone Columns
M.E. Vargas-Ugalde, K. Niranjan, D.L. Pyle,
and G.F. Gutiérrez-López
CONTENTS
19.1 Introduction
19.2 Background
19.2.1 Flavor Recovery Technology
19.2.2 The Spinning Cone Column
19.2.3 Mass Transfer Coefficients
19.2.4 Mean Residence Time
19.3.1 Equipment
19.3.1.1 SCC 1000 Flavourtech
19.3.1.2 SCC Perspex Laboratory Model
19.3.2 Methods
19.3.2.1 Determination of Overall Volumetric Mass Transfer
Coefficients (KLa)
19.3.2.2 Evaluation of the Mean Residence Time
19.4.1 Mass Transfer
19.4.2 Mean Residence Time
19.5 Conclusions
Nomenclature
Acknowledgments
References
19.1 INTRODUCTION
The Spinning Cone Column (SCC) is a multistage liquid–gas contacting unit with
increasing applications in food processing. SCC is a type of distillation equipment
that operates under vacuum pressures. It presents many advantages because of its
mass transfer efficiency, the short processing times involved, and its ability to handle

highly viscous and non-Newtonian liquids under reduced pressure. An understanding
of some of the mechanisms of simultaneous transfer of momentum, heat, and mass
in this equipment is necessary to save energy and to improve not only the separation
efficiency, but also the basis for selection, design, and control of columns and processes
involved. Despite the extensive use of this technology, few studies have been conducted
concerning the performance and mathematical modeling of this equipment.
To study the mass transfer and the residence time distribution in this device, a
Perspex model geometrically similar to the pilot plant SCC 1000 Flavourtech Europe
LTD installed at the University of Reading, U.K., was employed. This model uses
air to simulate the steam current. For these experiments, two spinning and two
stationary cones were employed; residence time experiments were also performed
in the pilot equipment.
19.2 BACKGROUND
19.2.1 FLAVOR RECOVERY TECHNOLOGY
The main objective when processing foods is preservation; the processes used include
evaporation, pasteurization, high temperature–short time pasteurization, distillation,
drying, and other operations. By applying these processes, it is possible to extend the
shelf life of many food materials. However, in most heat treatment procedures, the
operating conditions may change the original properties of a product. The use of low
temperature and vacuum pressure is a popular way of maintaining flavor and aroma
characteristics.
In most cases, compounds responsible for flavor and aroma are present in
products in small amounts; they are highly volatile and extremely sensitive to heat
damage. To minimize losses of aroma and flavor when processing foods, flavor/
aroma recovery technology is widely used. Basically, this technology consists of
removing and collecting volatiles before the main process and reincorporating them
into the final product at the last stage of processing. In this way, the original sensory
characteristics are maintained (Schobinger, 1999).
Flavor recovery technique was initially applied to process juice fruits around
1940. There exist different kinds of equipment to perform the separation of volatiles;
the use of a particular one depends on the product characteristics, the process costs,
and the final quality to be obtained.
19.2.2 THE SPINNING CONE COLUMN

Among the uses of the SCC in the food industry are (Menzi and Emch, 1989;
Flavourtech, 1998):
• Aroma recovery from fruit and vegetable juices, botanicals, herbs and spices
• Dealcoholization of drinks
• Desulfiting of grape juice
• Removal of tannins
• Coffee, tea, and citrus byproduct processing
• Removal of off-odors from dairy products

In fruit juice processing, the SCC is employed just before the product enters the
concentrator. Through the use of SCC, a substantial aroma recovery can be achieved
with a low evaporation rate (from 0.5 to 2.0% depending on the fruit) (Craig, 1987;
Schobinger, 1999).
The SCC resembles a combination of centrifuge–distillation units, and it is clas-
sified in the same group of equipment as the packed, bubble-cap, and plate columns
(Menzi and Emch, 1989; Shah, 1995).
In this equipment, the inert stripping gas—nitrogen or steam at low temperatures —
removes a vapor stream of volatile compounds from liquids or slurries. Internally, the
column contains two series of inverted cones. A series of fixed cones is attached to
the inside wall of the column; another series of cones, parallel to those fixed, is
attached to a rotating shaft. The stationary and rotating cones alternate vertically.
The product comes in to the top of the column, flows down the upper surface of the
first fixed cone, and drops onto the first rotating cone due to gravity. Then, due to
centrifugal force, the liquid is spun into a turbulent thin film that is forced upward
to the top of the spinning cone, dropping onto the next stationary cone. The product
then goes from cone to cone to the bottom of the column, following a spiral trajectory.
The gas for stripping comes into the bottom of the column and flows upward, passing
across the surface of the thin film of liquid and collecting volatile compounds along
its path. On the underside of the rotating cones are baffles that create a high degree
of turbulence in the rising vapor stream. The vapor flows out of the top of the column
and passes through a condensing system, which captures the volatile compounds in a
concentrated liquid form. The remaining liquid or slurry is pumped out of the bottom
of the column (Flavourtech, 1991).
19.2.3 MASS TRANSFER COEFFICIENTS

In chemical and food engineering, empirical correlations are commonly used in
many situations because real systems exhibit a different behavior from ideal, and it
is not easy to determine the contribution of each of the variables involved in a
particular case. Although these correlations cannot be applied to general cases, they
are useful to predict the behavior of a given phenomenon within the range of
conditions studied.
The rates of mass transfer between gas and liquid phases are strongly affected
by the solubility of the gaseous components in the liquid. Oxygen is among the
sparingly soluble gases in aqueous solutions. The solubility of a gas in a liquid
depends on the temperature, the equilibrium partial pressure of the solute gas in the
gas phase, and the concentration of the solute gas in the liquid phase (Aiba et al.,
1973). The total pressure on the system also affects the solubility, but when the value
of this parameter is lower than 5 atm, the solubility of gases can be considered
independent of the total pressure.
In those cases where the concentration of dissolved gas is small and the tem-
perature and pressure are far from the critical temperature and pressure of the gas,
Henry’s law can express the solubility of a gas in a liquid:
p=Hx (19.1)

Henry’s constant (H) is affected by temperature, concentration of dissolved salts,
and pH.
For a sparingly soluble gas, such as oxygen, the overall gas transfer rate (R) is
given by the flux equation:
*
R = KLa (c − c) (19.2)
Volumetric R and a are evaluated considering the total liquid volume, since the
gas hold-up is considered negligible for calculation purposes.
Concentration patterns in the SCC are not those of a perfectly mixed tank, but
they resemble those of plug flow. Then, the log mean oxygen concentration applies,
and it is possible to calculate KLa from a mass balance, assuming the oxygen
concentration in the liquid phase is equal to zero:
(V KLa) ∆clm = L ∆c (19.3)
For cylinders and disks rotating in an infinite fluid, several equations have been
developed to predict mass transfer rates. In Sherwood et al. (1975) the following
relationship for cylinders is reported:
2/3 0.664
JD = St Sc = (kc/U) Sc (19.4)
The same authors reported the following equation for oxygen transport to a
5 6
rotating disk in salt water for values of Re between 6 × 10 and 2 × 10 and Sc
numbers between 120 and 1200.
k cd
= 5.6 Re1.1 Sc0.333 (19.5)
D
They reported a semitheoretical relationship for the turbulent region:
k cd
= α Re 0.4 Sc0.25 (19.6)
D
They also described electrochemical studies by Bagotskaya, who found values

of kc proportional to the first power of rotational speed in the case of turbulent flow
on a rotating disk.
Blanch and Clark (1996) have reported α and β values (see Equation 19.7) to
obtain kLa in bubble columns and airlift contactors as a function of the superficial
gas velocity and liquid properties for low liquid viscosities. In these systems, α
values from 0.4 to 1.09 and β values from 0.89 to 1.23 were reported.
β
kLa = α vs (19.7)
Blanch and Clark (1996) also reported on correlations for kLa in stirred tanks
for inviscid systems as follows:

For coalescing (clean) dispersions:
−2 0.4 0.5
kLa = 2.6 × 10 (Po/V) vs (19.8)
For noncoalescing (dirty) dispersions:
−3 0.7 0.2
kLa = 2.0 × 10 (Po/V) vs (19.9)
−3
These equations were obtained for power inputs from 500 to 10,000 watt m
and small vessels of up to several thousand liters (Blanch and Clark, 1996)
Zivdar (1997) reported results on mass transfer characteristics of structured
packed columns 0.1 m in diameter were evaluated for humidification of air and oxygen
desorption from water. Gas and liquid transfer mass coefficients were dependent on
the corresponding flow rates, and gas phase mass transfer was also influenced by
change of liquid hold-up due to gas flow.
19.2.4 MEAN RESIDENCE TIME

The measurement of residence time distributions (RTD) is useful to estimate the
performance of process equipment or to find how much it deviates from the ideal
behavior. Even when the overall flow rate may have no detectable variation, not all
particles passing through the system stay there for the same length of time. For a
single system, there is a spread of residence times, which can be caused by chan-
nelling, recycling, or creation of stagnant regions of fluid in the vessel.
The residence time distribution function, E(t), is defined considering that the
fraction of product in the outlet stream that has been in the system for a length of
time between t and t + dt is equal to Edt (Denbig and Turner, 1984), so that:
∞
∫ 0
E( t )dt = 1 (19.10)
The average time spent by a product flowing at flow rate v through a vessel
volume V is equal to V/v. If the density of the flowing stream does not change as
it passes through the system and for a no-back-mixing situation, the mean residence
time (MRT) is equal to V/v and:
∞
MRT =
∫ 0
tE( t )dt (19.11)

Two types of spinning cone columns were used in this work: a pilot plant SCC1000
model (Flavourtech LTD, Europe), and a Perspex laboratory model. To determine
the dissolved oxygen concentration in the laboratory column, a JENWAY 9071
dissolved oxygen meter was used. Compressed nitrogen was the degassing agent
used to eliminate oxygen from deionized water during the measurements.

An injection gun (APV Co. Ltd.) and a spectrophotometer (CECIL 1000 Series,
CE1021 model) were used for the residence time distribution (RTD) studies with
cochineal red A spec Pure 70 BAYER AG as a tracer. The carboxymethylcellulose
(CMC) working solutions were prepared with Blanose CMC 7HF Sodium Car-
boxymethylcellulose Aqualon, Hercules Inc.
19.3.1 EQUIPMENT
19.3.1.1 SCC 1000 Flavourtech
The SCC column 1000 is composed of a vertical stainless steel cylinder 2.0 m in
height and 0.33 m in diameter, with 40 cones and a capacity range of 100–1000
−1 −1
l h . The rotating speed varies from 26 to 160 sec ; nitrogen or low temperature
steam can be used as the stripping medium, and the column usually operates at
vacuum pressures (Flavourtech, 1991).
19.3.1.2 SCC Perspex Laboratory Model
To get information about the performance of the SCC, a Perspex model geometrically
similar to the pilot plant column was employed in this research. The model is 0.2
m in height and 0.37 m in diameter; it has three stationary and two spinning cones.
It works at atmospheric pressure, and air is used instead of steam or nitrogen for
hydrodynamic purposes. The model has a shaft 50 mm in radius, and the column
inner radius is 185 mm. Both the spinning and the stationary cones have inner and
outer radii of 50 and 145 mm, respectively. Four pressure taps are also available,
and it is possible to change shaft velocity, number of cones, and liquid and air flow
rates. A diagram of this column is presented in Figure 19.1.
air N2
Perspex Column cin
pt
Oxygen
cones probe
tank pt
solution
shaft motor
Recirculation or drain tube
cout
pump
water pool
pt = pressure tappings
FIGURE 19.1 Schematic diagram of the SCC laboratory Perspex model.

TABLE 19.1
Conditions for Mass Transfer Experiments
Water Flow Rate Nitrogen Flow Rate
3 −1 5 3 −1 4 −1
(m sec × 10 ) (m sec × 10 ) Cone Velocity (sec )
4.2, 5.8, 11.7 8, 1.2, 1.6, 2.0 26, 47, 79, 131
For the RTD determinations, several experiments were performed using the pilot
plant SCC.
19.3.2 METHODS
19.3.2.1 Determination of Overall Volumetric Mass Transfer
Coefficients (KLa)
KLa were calculated by measuring the dissolved oxygen concentration in deionized

water at the bottom of the column until the condition of equilibrium was reached,
employing a deoxygenating method using nitrogen as the displacing gas (Heineken,
1971; Atkinson and Mavituna, 1991), based on the factorial experimental design
presented in Table 19.1.
19.3.2.2 Evaluation of the Mean Residence Time
Water and carboxymethylcellulose (CMC) at 0.5 and 1% w/w were used, employing
different conditions in both the Perspex model and the pilot plant SCC, as presented
in Table 19.2.
Mean residence time (MRT) was measured by a pulse method (Levenspiel,
−3
1972) using cochineal red dye as a tracer (0.15 g cm for the laboratory model and
−3
0.3 g cm for the pilot column) and measuring the concentration as a function of
time by reading the absorbance of the samples at the exit of the equipment in a
spectrophotometer CECIL 1021 and by applying Equation (19.11).

19.4.1 MASS TRANSFER
KLa values for the conditions presented in Table 19.1 were calculated by applying
3
Equation (19.3) for a tank volume (V) of 0.0215 m . Oxygen concentration values at
−3
the inlet of the system (cin) fell within 0.007 to 0.008 kg m for most of the trials.
The equilibrium oxygen concentration (cout) was measured with an oxygen probe
immersed in the water pool formed at the bottom of the column. Equilibrium was
considered to have been reached when no change of this measured value was
registered by the probe (see Figure 19.1).
In Figure 19.2, calculated KLa values as a function of angular velocity of the
−4 3 −1
cones and gas flow rate for a liquid flow rate of 4.2 × 10 m sec are presented.
In Figure 19.3, calculated KLa values as a function of gas flow rate and liquid flow

TABLE 19.2
Conditions for Determination of Mean Residence Time Experiments
SCC Perspex Model

−1
Water Cone velocity (sec ) 26, 47, 79, 131
3 −1 5
Liquid flow rate (m sec ) × 10 3.3, 6.7
3 −1 4
Gas flow rate (m sec ) × 10 0, 18.33
CMC Concentration (%) 0.5 1.0
3 −1 5
Liquid flow rate (m sec ) × 10 1.6, 3.3 0.8
3 −1 4
Gas flow rate (m sec ) × 10 0 0
−1
Cone velocity (sec ) 79, 47, 131 79
SCC Pilot Plant

−1
Water Cone velocity (sec ) 26, 61
3 −1 5
3 −1
Gas flow rate (m sec ) 0
−1
CMC Cone velocity (sec ) 26, 61
0.5%
3 −1 5
3 −1
Gas flow rate (m sec ) 0
0.007
0.006
0.005
KLa sec-1
0.004
0.003 131
0.002 79
0.001 47
Angular velocity
0 sec-1
26
7.88 11.81 15.83 19.67
Gas flow rate
m3sec-1 × 10-4
−4 3 −1
FIGURE 19.2 KLa for oxygen in water. Liquid flow rate = 4.2 × 10 m sec .

0.009
0.008
0.007
0.006
-1
KLa sec
0.005
0.004 11.67
0.003
0.002 5.83
0.001
Liquid
flow rate
4.17 m sec × 10
3 -1 -5
0
7.88
11.81
15.83
Gas flow rate 19.67
m3 sec -1 × 10-4
−1
FIGURE 19.3 KLa for oxygen in water. Angular velocity = 47 sec .
−1
rate for an angular velocity of 47 sec are presented. From Figures 19.2 and 19.3, it is
possible to observe that KLa increases with gas and liquid flow rates and angular
velocity; this agrees with findings made by Zivdar (1997) for structured packed columns.
Empirical correlations reported in the literature for mass transfer descriptions
for rotating disks, cylinders (Sherwood et al., 1975), bubble columns, and stirred
tanks (Blanch and Clark, 1996) showed that the dimensionless mass transfer number
0.5
depends on the value of (Re) .
An empirical correlation (Equation 19.12) of KLa values and ω, L, and G was
obtained by means of the S.A.S. statistical program (S.A.S. Institute, 1989) using an
iterative nonlinear least squares methodology based on the Gauss–Newton method.
0.489
KLa = 2.254 (19.12)
It is possible to observe that KLa depends on the dynamic parameters with an
exponent close to 0.5. This may indicate that mass transfer in the SCC follows a
similar trend as in other situations reported in the literature (Sherwood et al., 1975;
Blanch and Clark, 1996; Zivdar, 1997).
19.4.2 MEAN RESIDENCE TIME

An example of the E curves obtained using the Perspex laboratory model is presented
in Figure 19.4. From Figure 19.4, a plug flow pattern can be observed. Similar
findings have been reported by other authors when working with a SCC (Shah, 1995;
Menzi and Emch, 1989).

0.09
0.08
0.07
0.06 Fluid: Water

Angular velocity = 79 sec-1
E value
0.05
Air flow rate = 6.7 x 10-5 m3sec-1
0.04 Liquid flow rate= 18.33 x 10-4 m3sec-1
0.03
0.02
0.01
0
0 100 200 300 400
time sec
FIGURE 19.4 Example of an E curve.
TABLE 19.3
Mean Residence Time (MRT) for Water in the SCC Perspex
Laboratory Model
Conditions
Liquid Flow Rate Air Flow Rate
−1 3 −1 5 3 −1
Cone Velocity (sec ) (m sec × 10 ) (m sec ) MRT (sec)
26 3.3 0 16
26 3.3 18.33 20
26 6.7 0 13
26 6.7 18.33 17
47 3.3 0 13
47 3.3 18.33 16
47 6.7 0 16
47 6.7 18.33 13
79 3.3 0 14
79 3.3 18.33 15
79 6.7 0 12
79 6.7 18.33 12
131 3.3 0 29
131 3.3 18.33 29
131 6.7 0 18
131 6.7 18.33 14
Mean residence times (MRT) for water and CMC were calculated from these E
curves (Figure 19.4).
Values of MRT for water and CMC are presented in Tables 19.3 and 19.4,
respectively. For the conditions studied in the Perspex laboratory model, residence

TABLE 19.4
Mean Residence Time (MRT) for CMC in the SCC Perspex
Laboratory Model
Conditions
Liquid Flow Air Flow Concentration
−1 3 –1 5 3 –1
Cone Velocity (sec ) (m sec × 10 ) (m sec ) (%) MRT (sec)
79 0.8 0 1.0 199

79 3.3 0 0.5 30
79 1.6 0 0.5 71
47 3.3 0 0.5 29
131 3.3 0 0.5 35
300
Mean Residence Time (MRT)
Code [ letter] / [value ] / [value] on x-axis

250 represents: [product (W = water, C = CMC0.5%)] /
[liquid flow rate m3sec-1 x 10-5] / [cone velocity sec-1]
200
150
100
50
0
26 61 26 /2
6 61 26 61
8/ 8/ 6/ 6/ 1/ 1/
2. 2. 5. 5.
6 5. 11
.
11
.
C C C W W W W
FIGURE 19.5 Mean residence time for water and CMC (0.5%) in the SCC pilot plant.
time for water was not influenced by air nor by liquid flow rate, nor even by cone
rotating velocity. The average MRT obtained for this equipment was about 17
seconds.
In the case of experiments using 1% CMC solution (apparent viscosity: 960 cP
−1
at 10 sec at T = 25°C), MRT was about 11.7 times greater than the average MRT
−1
for water. When using 0.5% CMC solution (apparent viscosity: 200 cP at 10 sec
ο
at T = 25 C), MRT was 1.8 to 4.2 times greater than values for water.
The influence of liquid flow rate on MRT was determined using 0.5% CMC solu-
−5 3 −1
tions. At 3.3 × 10 m sec , the MRT was 2.4 times lower than at a flow rate of 1.6 ×
−5 3 −1 −1
10 m sec . There was no influence of cone velocity on MRT for 79 and 47 sec . The
−1
time for 131 sec was longer; this can be explained by flooding conditions in the first
spinning cone (Shah, 1995).
Results for the experiments in the SCC pilot plant are presented in Figure 19.5. It
is possible to observe that MRT for water depends on flow rate as well as on cone
velocity, becoming shorter at higher values of both variables, as expected. The effect
of viscosity on MRT can be observed from the experiments with CMC 0.5% at the

same conditions. MRT for CMC is 1.62 times greater than MRT for water. In the
−5 3 −1
experiments with water at 5.6 × 10 m sec , MRT is 1.28 times greater for a cone
−1 −5 3 −1
speed of 26 than 61 sec . From experiments at a flow rate of 11.1 × 10 m sec
−1
and rotating velocity of 26 sec , MRT is 1.14 times greater than that obtained at a
−1
rotating speed of 61 sec .
In Figure 19.5, the effect of the liquid flow rate using water on MRT is shown,
−1
comparing results at a constant angular speed. At 26 sec , MRT is 1.67 times greater
−5 3 −1 −5 3 −1 −1
for a flow rate of 5.6 × 10 m sec than for 11.1 × 10 m sec . At 61 sec , MRT
−5 3 −1 −5 3
is 1.49 times greater for a flow rate of 5.6 × 10 m sec than for 11.1 × 10 m
−1
sec . The effect of liquid flow rate using CMC solution (0.5%) is shown comparing
−1 −5 3 −1
data for a constant speed. MRT at 26 sec and 2.8 × 10 m sec is 1.72 times
−5 3 −1
greater than MRT for 5.6 × 10 m sec . With a flow rate of CMC solution (0.5%)
−5 3 −1 −1
of 2.8 × 10 m sec , MRT obtained at an angular velocity of 26 sec is 1.05 times
−1
greater than MRT at 61 sec .
19.5 CONCLUSIONS
Mass transfer into the spinning cone column depends on angular cone velocity and
liquid and gas flow rate; it is higher at higher values for these variables; their influence
can be represented by a power equation.
Mean residence time is affected by liquid flow rate, cone speed, and viscosity of
the product; the influence of liquid flow rate is greater than the influence of cone speed.
The combined effect of high mass transfer rates and short mean residence times
for the product into the column brings an advantage for the recovery of aromas and
flavors in foods, since it diminishes the damage caused by heat and processing time
to these volatile compounds. However, the evidence of a long tail in the residence time
distribution must be considered, since this means that some of the volatiles are still
present after the mean process and may be affected by having longer processing times.
The information given in this work may be used for finding appropriate operating
conditions for a particular product, aiming to obtain as much mass transfer as
possible within the economic limits of power requirements for pumping the liquid
and for rotating the cones so as to obtain low MRT.
NOMENCLATURE
2 −3
a Bubble surface area per unit volume; (m m )
−3
c Dissolved oxygen concentration in the bulk liquid; (kg m )
−3
c* Solubility of oxygen in equilibrium with pG (c* = pG/H); (kg m )
∆c Concentration difference between the inlet and the outlet of the system;
(cin − cout)
∆clm Logarithmic mean of concentration difference between the inlet and the
 
 (c − c ) 
outlet of the system  inc out 
 ln cout 
in

2 −1
D Diffusivity coefficient; (cm sec )
d Disk diameter; (m)
E(t) Residence time distribution function
3 −1
G Gas flow rate; (m sec )
−1
H Henry’s law constant; (atm mole fraction )
JD Mass transfer dimensionless group
kc Individual mass transfer coefficient in Equations (19.4), (19.5) and
−1
(19.6); (cm sec )
−1
KLa Overall volumetric mass transfer coefficient based on the liquid phase; (sec )
−1
kLa Individual volumetric mass transfer coefficient based on the liquid phase; (s )
3 −1
L Liquid flow rate; (m sec )
l Characteristic length; (cm)
MRT Mean residence time; (sec)
p Partial pressure of the solute in the gas phase; (atm)
pG Gas pressure; (atm)
−3
Po/V Gassed power per volume; (watt m )
−3 −1
R Overall oxygen transfer rate; (kg m sec )
Re Reynolds number based on diameter and peripheral velocity of disk in
Equation (19.5); (d U ρ/µ)
RTD Residence time distribution
Sc Schmidt number; (µ/ρ D)
Sh Sherwood number; (kc l/D)
St Stanton number; (Sh/Re Sc)
t Time; (sec)
−1
U Peripheral velocity of cylinder in Equation (19.4); (m sec )
3
V Reactor volume; (m )
−1
v Material flow rate in a reactor; (m sec )
−1 −1
vs Superficial velocity; (cm sec in Equation (19.7); m sec in Equations (19.8)
and (19.9))
x Mole fraction of the solute in the liquid phase (molar concentration of the
dissolved gas for sparingly soluble gases)
α Coefficient in Equation (19.7)
β Exponent in Equation (19.7)
−1 −1
µ Viscosity; (g cm sec )
−3
ρ Density (g cm )
−1
ω Angular velocity of the cone; (sec )
ACKNOWLEDGMENTS
The authors thank the ALFA Network: Food Quality in Food Engineering, coordi-
nated by the University of Reading, U.K., EU Contract Number ALR/B 7–3011/
94.04–5.0130.9; Flavourtech Europe Ltd. for allowing the use of the Spinning Cone
Column model 1000; FES Cuautitlán-UNAM, ENCB-IPN, and CYTED project
Xl.13.

REFERENCES
Aiba, S., Humphrey, S., and Millis, F., Biochemical Engineering, 2nd ed., Academic Press,
New York, 1973, pp. 163–194.
Atkinson B. and Mavituna, F., Gas–liquid mass transfer and mixing, in Biochemical Engi-
neering and Biotechnology Handbook, Macmillan Pub. Ltd., U.K., 1991, pp. 703–731.
Blanch, H.W. and Clark, D.S., Biochemical Engineering, Marcel Dekker, New York, 1996,
pp. 388–392.
Craig, A.J.M., Flavor recovery by the Flavortech Recovery System, Food Technol. Aust., 39,
102–104, 1987.
Denbig, K.G. and Turner, J.C.R., Chemical Reactor Theory: An Introduction, 3rd ed., Cam-
bridge University Press, Cambridge, 1984.
Flavourtech, Ltd., SCC Treatment of UHT Milk, SCC Technical Bulletin TB, February 21,
1998.
Flavourtech Ltd., Finally: Processed and Packaged Foods and Beverages Can Taste as Good
as the Originals, Commercial Bulletin, 1991.
Heineken, F.G., Oxygen mass transfer and oxygen respiration rate measurements utilising
fast response oxygen electrodes, Biotech. Bioeng., 13, 599–618, 1971.
Levenspiel, O., Chemical Reaction Engineering, 2nd ed., John Wiley and Sons, New York,
1972, pp. 253–325.
Menzi, H. and Emch, F., The spinning cone column: An efficient separator of aroma volatiles
from a liquid, Lebensmit. Wiss. Technical., 22, 324–328, 1989.
S.A.S. Institute Inc., The S.A.S. System for Microsoft Windows, Release 6.10, Cary, N.C.,
1989.
Schobinger, U., Progress in fruit juice technology during the last 50 years — A survey, Fruit
Process., 7, 275–281, 1999.
Shah, N.A., Study of the Fluid Dynamics in the Spinning Cone Column, thesis, University
of Reading, 1995.
Sherwood, T.K., Pigford, R.I., and Wilke, C.H.R., Mass Transfer, McGraw-Hill, New York,
1975, pp. 236–241.
Zivdar, M., Distillation for Food Flavour Separations, seminar, July 4, 1997, Department of
Chemical Engineering, University of Sydney, Australia, http://www.chem.eng.usyd.
edu.au.

Part III
Heat Transfer

Transport Phenomena
20 during Double-Sided
Cooking of Meat Patties
S.E. Zorrilla, S. Wichchukit, and R.P. Singh
CONTENTS
20.1 Introduction
20.2 Mathematical Model
20.2.1 The Basic Equation
20.2.2 The Melting Moving Boundary
20.2.3 The Evaporating Moving Boundary
20.3 Thermal Properties
20.3.1 Contact Heat Transfer Coefficient
20.4 Simulation and Model Validation
20.5 Future Considerations
20.6 Conclusions
Nomenclature
References
20.1 INTRODUCTION
In 1998, 5.5 billion hamburgers or cheeseburgers were served in commercial res-
taurants in the United States (NCBA, 1998). Unfortunately, since 1982 several
outbreaks caused by Escherichia coli O157:H7 have been linked to the consumption
of beef patties (D’Sa et al., 2000). Consequently, the U.S. Department of Agriculture
(USDA) and U.S. Food and Drug Administration (FDA) have recommended cooking
ground beef products to 71°C for home preparation and 68°C for 15 sec for food service,
respectively (USDA, 1998; FDA, 1997). However, suitable procedures for measuring
internal temperature in beef patties are difficult, especially at food service establish-
ments. As a result, patties may be overcooked with undesirable textural and sensory
characteristics or undercooked and microbiologically unsafe. Therefore, a funda-
mental understanding of the heat transfer process is necessary to design equipment
and sensors that ensure the desired safety and quality goals during beef patty cooking.
One widely used beef patty cooking method in restaurants involves placing
frozen patties between two heated plates with the plate surface temperatures generally

greater than 160°C. As heat penetrates the patty, a thawing process begins. As heating
continues, higher temperatures cause protein denaturation and considerable lowering
in water holding capacity (Lawrie, 1991). Water and fat may be partially squeezed
out because of meat shrinkage and external pressure. Near the patty surface, brown-
ing reactions occur, and a combination of dehydration and high temperature lead to
the formation of a crust (Dagerskog and Bengtsson, 1974). In a simplified model,
as heat penetrates the frozen patty, two moving boundaries can be distinguished: the
thawing and the evaporation boundaries (Singh, 2000). Predictive mathematical
models based on classical transport phenomena equations can be a useful tool to
represent this process.
20.2 MATHEMATICAL MODEL

Different mathematical models for studying the contact cooking process in ham-
burger patties have been developed (Dagerskog, 1979a, b; Ikediala et al., 1996; Pan
et al., 2000; Zorrilla and Singh, 2000a, b). Dagerskog (1979a) proposed a model
of heat transfer based on the heat conduction equation. Internal mass transfer was
based on an empirical relation between water retaining capacity and temperature.
Dagerskog (1979b) modified this original model for use with the frozen state. In
both cases, the models were solved by finite difference methods. However, exper-
imental and theoretical values did not agree well.
Ikediala et al. (1996) modeled the heat transfer in unfrozen meat patties during
single-sided pan frying with and without turn-over. The main assumptions were that
heat was transferred inside the patty by conduction with no heat generation and
negligible meat patty shrinkage or swelling. These authors considered cylindrical
geometry and incorporated the heat removed due to moisture loss, which was
experimentally determined. The model was solved by a finite element method.
Pan et al. (2000) developed a model for cooking a frozen hamburger patty based
on the enthalpy formulation, considering the effect of mass transfer and variable heating
temperature and heat transfer coefficient. Water and fat losses were obtained experi-
mentally and were found to affect the thermal properties. The mathematical prediction
taking into account mass transfer did not significantly improve the prediction results.
Zorrilla and Singh (2000a) developed a simplified one-dimensional model to
predict temperature profiles in a frozen meat patty during double-sided cooking.
Conduction was considered the main mechanism for heat transfer, and enthalpy
formulation was used to avoid the discontinuity problem of the phase change during
melting. The mathematical formulation considered different top and bottom heating
temperatures and was validated by comparing predicted and experimental tempera-
ture profiles obtained at 163 and 204°C for the bottom plate and 177 and 221°C for
the top plate, respectively. Zorrilla and Singh (2000b) extended the model to a two-
dimensional cylindrical geometry. The results showed no significant difference when
a cylindrical geometry or radial shrinkage was considered to predict the temperature
at the geometric center of a patty under normal conditions of hamburger cooking.
However, the two-dimensional model provides a description of temperature in
regions close to the circumferential edge of the patty, which is not possible with the
one-dimensional model.

20.2.1 THE BASIC EQUATION
The heat conduction equation for a homogeneous, isotropic solid in a cylindrical
coordinate system is (Ozisik, 1993):
1 ∂  ∂T  1 ∂  ∂T  ∂  ∂T  ∂T
 kr  +  k  +  k  + g = ρC p (20.1)
r ∂r  ∂r  r 2 ∂φ  ∂φ  ∂z  ∂z  ∂t
where T is the temperature in the solid; t is the time; r, φ, and z are the cylindrical
coordinates; g is the heat generation term; k is the thermal conductivity; ρ is the
density; and Cp is the specific heat. When no heat is generated and temperature has
no φ dependence, Equation (20.1) becomes:
1 ∂  ∂T  ∂  ∂T  ∂T
 kr  +  k  = ρC p (20.2)
r ∂r  ∂r  ∂z  ∂z  ∂t
A meat patty is not a homogeneous solid. However, if the thermal properties

are considered as effective properties, and assuming local thermal equilibrium among
the different phases present such as ice, fat, and nonfat solids, Equation (20.2) is
still valid (Farkas et al., 1996).
During cooking of a frozen beef patty, ice melts and water partially evaporates,
while solid fat melts. Assuming that the energy involved in fat melting is negligible,
only two moving boundaries need to be considered.
20.2.2 THE MELTING MOVING BOUNDARY

In problems involving melting or solidification, the location of the moving solid–
liquid interface is not known a priori, and it has to be determined as part of the
solution (Ozisik, 1994). As a result, phase change boundary problems are nonlinear
and their analytical solution is difficult. The situation is more complex when the
material is nonhomogeneous. The actual phase change takes place over a wide range
of temperatures at which food properties change considerably. Mannapperuma and
Singh (1988) proposed a method using the approach of enthalpy formulation to solve
this heat conduction problem involving gradual phase change. Therefore, Equation
(20.2) can be written in terms of enthalpy (H) as:
1 ∂ ∂T(H)  ∂  ∂T(H)  ∂H
 rk(H)  +  k(H) = (20.3)
r ∂r  ∂r  ∂z  ∂z  ∂t
valid for the region where the thawing process takes place.
20.2.3 THE EVAPORATING MOVING BOUNDARY

The water boiling at an interface separates two regions of different thermal properties.
In immersion frying of potatoes, these regions are core and crust (Farkas et al., 1996).

In cooking of hamburger patties, these regions are better defined as core and sear
layer. There are different methods to consider this boundary. Farkas et al. (1996)
considered two regions and solved coupled heat and mass transfer equations for
each one. Because the crust thickness is thin compared with core dimensions for
the usual cooking times, a linear temperature change in the crust region can be
assumed (Vijayan and Singh, 1997).
Table 20.1 shows the boundary and initial conditions to complete the mathemat-
ical formulation.
TABLE 20.1
Summary of Boundary and Initial Conditions to Complete the Mathematical
Formulation during Double-Sided Cooking of Meat Patties
Heat Transfer in the Core
Boundary Conditions
T = Tb z = S1(r,t), S2(r,t); 0 < r < a(t); t > 0 (20.4)
∂T
=0 r = 0; S1(r,t) < z < S2(r,t); t > 0 (20.5)
∂r
∂T
−k = h c (T − Ta ) r = a(t); S1(r,t) < z < S2(r,t); t > 0 (20.6a)
∂r
T = Tb r = R(z,t); S1(r,t) < z < S2(r,t); t > 0 (20.6b)
Initial Condition
T = T0 t = 0; S1(r,t) < z < S2(r,t); 0 < r < a(t) (20.7)
Heat Balances at Interfaces between Core and Crust

∂T ∂T ∂S ( r, t )
− k crust +k = λ vρx w i z = Si(r,t); i = 1, 2; t > 0 (20.8)
∂z ∂z ∂t
∂T ∂T ∂R(z, t )
− k crust +k = λ vρx w r = R(z,t); t > 0 (20.9)
∂r ∂r ∂t
Heat Balances and Approximations at Surface

∂T
− k crust = h(Tp1 ( t ) − T) z = 0; t > 0 (20.10)
∂z
∂T Tb − T
= z = 0; t > 0 (20.11)
∂z S1 ( r, t )
∂T
− k crust = h(T − Tp 2 (t )) z = L; t > 0 (20.12)
∂z
∂T Tb − T
= z = L; t > 0 (20.13)
∂z L − S2 ( r, t )
∂T
− k crust = h c (T − Ta ) r = a(t); t > 0 (20.14)
∂r
∂T Tb − T
= r = a(t); t > 0 (20.15)
∂r a( t ) − R(z, t )

Equations (20.6b), (20.9), (20.14), and (20.15) are valid when the boiling tem-
perature is reached in the radial direction.
20.3 THERMAL PROPERTIES

Thermal properties are important to complete the mathematical description. How-
ever, while information about the thermal properties of frozen and unfrozen foods
at ambient temperature is widely available, data at higher temperatures are scarce.
Urbicain and Lozano (1997), Cleland and Valentas (1997), Rahman (1995), and
Sweat (1994) reported predictive equations, correlations, and experimental values
for thermal properties considering different composition and temperature ranges.
Their equations can be used to estimate the properties at lower and ambient tem-
peratures. In Table 20.2, experimental values and correlations for thermal properties
of ground beef products during cooking conditions are given.
20.3.1 CONTACT HEAT TRANSFER COEFFICIENT

The contact heat transfer coefficient appears between two solids that are not per-
fectly in contact. In this case, the contact depends on the grill and patty surface
characteristics and the characteristics of any other medium between them. Because
juice is released as the cooking process takes place, that medium is a thin layer of
fat/air/moisture. Generally, a constant value of this coefficient is assumed for
TABLE 20.2
Thermal Properties of Meat Patties during Cooking
Property Source
3
Density (kg/m )
a
ρ = 1300 − 300 x w − 400 x f − (0.4 x w + 0.7 x f )T
b
1.025 (30–75°C)
Apparent Specific Heat (J/kg°C)

C p = 1600 − 2600 x w + 15T x f a
Thermal Conductivity (W/m°C)

a
k = 0.5 − 0.92 x f + 0.0024T
c
k = 0.001(668.4 − 704 x f − 305 x w + 1.35T)
b
0.35 to 0.41 (5–70°C)
Note: xw = water content in decimal fraction; xf = fat content in decimal fraction;

T = temperature in °C.
a
Dagerskog, M., Lebensm.-Wiss. Technol., 12, 217–224, 1979.
b
Pan, Z., thesis, University of California, Davis, 1998.
c
Baghe-Khandan, M.S., Okos, M.R., and Sweat, V.E., Trans. ASAE, 25, 1118–1122, 1982.

calculations (Dagerskog, 1979a; Ikediala et al., 1996). Most research papers address
contact between metals under steady state conditions (Madhusudana, 1996), but little
information is available on contact heat transfer coefficient values for solid foods.
Houšová and Topinka (1985) have shown experimentally that the contact heat
transfer coefficient depends on product type, contact plate temperature, contact pressure,
and stage in the heat treatment. The heat transfer coefficients measured were in the
2
range of 200 to 1200 W/m °C. Dagerskog and Sörenfors (1978) found contact heat
transfer coefficient values for cooking of minced meat patty in the range of 260 ±
2 2
50 W/m °C during contact cooking and 90 ± 20 W/m °C during cooking in a
convection oven. Dagerskog (1979a) obtained contact heat transfer coefficient values
2
in the range of 425 ± 33 W/m °C during double-sided contact frying of meat patties.
Pan (1998) experimentally determined values of this coefficient by measuring the heat
flux involved and the temperatures of the heating surface and the patty surface. The
2
contact heat transfer coefficients obtained were in the range of 200 to 1200 W/m °C.
Wichchukit et al. (2000) obtained contact heat transfer coefficient values, h,
under various cooking conditions and determined the changes in heat transfer coef-
ficient during the cooking process and the influence of factors for each cooking
condition on heat transfer coefficient. Contact heat transfer coefficient values were
calculated using Newton’s law of cooling and measuring the heat flux transferring
from the grill plate to a hamburger patty, the grill plate temperature, and the patty
surface temperature. Different temperatures (177, 191, 204°C), different gap thick-
nesses between plates (10.0, 10.5, 11.0 mm) and top or bottom plate were considered
in a split–split plot design to study the influence of these operating variables.
Average h values for the conditions studied are shown in Figure 20.1. The h
2
values varied with cooking time and were in the range of 250 to 650 W/m °C. A
maximum value of h was observed in the beginning, and later it reached an asymp-
totic value. At the beginning of the cooking process, the solid frozen patty offers
more resistance to the deformation caused by compression from the top plate,
resulting in an increase of the contact area. The decrease in the heat transfer after
about 60 sec may be related to the fact that at this point the hamburger is almost
completely thawed. Therefore, the hamburger is easily compressed, and the interfa-
cial contact forces and contact area may decrease.
When the gap thickness between plates decreases, the patty is more compressed,
the contact area increases, and the heat transfer may increase. However, under com-
pression the fat and water discharge also increases, changing the composition of the
layer between the hamburger and the plate, thus affecting the heat transfer. A higher
peak of h was observed for a 10.5 mm gap thickness compared with the value for
a 11.0 mm gap thickness (P < 0.05). The maximum values for h involving the bottom
plate were higher than those involving the top plate (P < 0.05). The grill has top
heating plates covered with Teflon release sheets to prevent the material from sticking
to the plate. Some experiments were carried out placing the release sheet on the
bottom plate, and a similar trend as with the top plate was observed. Therefore, it
may be concluded that the release sheet offered resistance to heat transfer to the
hamburger patties during cooking.
The asymptotic values for h involving the bottom plate were also higher than
those involving the top plate (P < 0.05). When the plate temperature increased, the

Bottom plate Top plate
Gap thickness = 10.0 mm

800 800
600 600
h (W/m2°C)
h (W/m2°C)
400 400
200 200
0 0
0 20 40 60 80 100 120 0 20 40 60 80 100 120
Time (sec) Time (sec)

800 800
600 600
h (W/m °C)
h (W/m2°C)
2
400 400
200 200
0 0
0 20 40 60 80 100 120 0 20 40 60 80 100 120

800 800
600 600
h (W/m °C)
h (W/m °C)
2
400 400
200 200
0 0
0 20 40 60 80 100 120 0 20 40 60 80 100 120
FIGURE 20.1 Average contact heat transfer coefficients involving top and bottom plates for
different gap thicknesses and set grill temperatures: (—) 177°C, (—) 191°C, (- - -) 204°C.
asymptotic value of h decreased (P < 0.05). The asymptotic values for 177 and 191
2
or 204°C were 350 and 250 W/m °C, respectively. At high temperatures, more
dehydration near the patty surface occurs, increasing the cohesive forces of the
protein matrix. Therefore, adhesion to the grill surface may decrease, decreasing the
contact area and the contact heat transfer coefficient.

20.4 SIMULATION AND MODEL VALIDATION
The solution of the system comprised of Equations (20.3–20.15) was obtained
numerically using finite difference methods (Zorrilla and Singh, 2000a, b). A com-
puter program was written in Fortran (Digital Visual Fortran Version 5.0). The input
data included gap thickness between plates, radius of the patty, product composition,
unfreezable water content, initial freezing point, initial temperature of the product,
plate temperature history, surrounding air temperature, contact heat transfer coef-
ficient, combined radiation and convection heat transfer coefficient at the circum-
ferential surface, and total cooking time.
The gap thickness, radius of the patty, product composition, initial temperature
of product, plate temperature history, and total cooking time were measured during
the experiment. Thermal properties varying with temperature were calculated using
the procedure developed by Mannapperuma (1988) based on composition, thermal
properties for the unfrozen state, unfreezable water content, and initial freezing point.
Thermal properties for the unfrozen state were estimated using correlations based
on the composition (24% fat content, 60% w.b. moisture, 16% protein content), and
3
the following values were obtained: density, 1026.7 kg/m ; apparent specific heat,
3268 J/kg°C; thermal conductivity, 0.416 W/m°C; unfreezable water, 4%, and initial
freezing point, –1°C (Cleland and Valentas, 1997).
2
An average contact heat transfer coefficient of 900 W/m °C, a combined radiation
and convection heat transfer coefficient at the circumferential surface of the patty
2
of 60 W/m °C (Geankoplis, 1993), and the average value of the plate temperatures
as a surrounding air temperature were assumed. The last assumption was verified
experimentally. Typical simulated temperature distributions in two dimensions
(radial and axial) are plotted in Figures 20.2 and 20.3 for 50 and 124 sec of cooking
time. It is evident that temperature changes in the circumferential region of the patty
(region near r = a) are different from the changes in the central region (region near
r = 0). Preliminary results showed that this difference affects texture parameters. A
one-dimensional model would not be able to find such differences in temperature
profiles.
The experimental validation is not easy because of the difficulty of appropri-
ately placing the thermocouples. Although thermocouples are placed carefully at
the beginning, when the cooking starts, it is possible for them to change position
because of the softening of the material. Validation is generally carried out by
measuring the temperature at the geometric center of the patty. Typical experi-
mental and predicted temperatures at the patty center are shown in Figure 20.4
(Zorrilla and Singh, 2000a). The predicted values correspond to a simulation for
the one-dimensional model. However, Zorrilla and Singh (2000b) observed that
the two-dimensional model has no significant effect on the prediction of temperature
at the geometric center. For simulation, a constant contact heat transfer coefficient
was used. If the experimental h values were used, a lower center temperature
would have been predicted because the h values measured are in the range of
2
250–650 W/m °C and are lower than the value assumed for simulations (900
2
W/m °C). However, the calculations carried out with the experimental h values
will lead to safer cooking times.

220
180
Temperature (°C)
140
100
60
58.4
20
46.7
35.1
-20 23.4 Radial distance
from center, r, mm
0.0
11.7
1.1
2.2
3.3
4.4
5.5
6.6
0.0
7.7
8.8
9.9
11.0
Distance from top patty surface, z, mm
FIGURE 20.2 Temperature distribution in a hamburger patty at 50 sec of cooking time (L =

2 2
11 mm; a = 58 mm; Tp1 = 221°C; Tp2 = 204°C; h = 900 W/m °C; Ta = 212°C; hc = 60 W/m °C).
220
180
Temperature (°C)
140
100
60
58.4
20
46.7
35.1
-20 23.4 Radial distance
from center, r, mm
0.0
11.7
1.1
2.2
3.3
4.4
5.5
6.6
0.0
7.7
8.8
9.9
11.0
Distance from top patty surface, z, mm
FIGURE 20.3 Temperature distribution in a hamburger patty at 124 sec of cooking time (L =
2 2
11 mm; a = 58 mm; Tp1 = 221°C; Tp2 = 204°C; h = 900 W/m °C; Ta = 212°C; hc = 60 W/m °C).

250
Set top plate temperature = 221°C
200
Set bottom plate temperature = 204°C

Temperature (°C)
150
100
50
-50
0 25 50 75 100 125
Time (sec)
FIGURE 20.4 Experimental (ⵧ) and predicted (—) temperatures at patty center (L = 11 mm;
2
h = 900 W/m °C).
20.5 FUTURE CONSIDERATIONS

The mathematical model is the first step of an optimization process (Banga et al., 1991,
1997). The results of predictive heat transfer models help to address food safety issues
associated with the survival of pathogens. On the other hand, the optimization proce-
dure must take into account information related not only to microbial destruction, but
also to textural and sensory characteristics. In recent years, texture has become an
important attribute indicative of hamburger patty quality (Berry, 1994; Bigner-George
and Berry, 2000; Dreeling et al., 2000; Ju and Mittal, 1999, 2000). Moreover, instru-
mental methods for textural properties have been successfully correlated with sensory
data and are often more precise and reproducible (Beilken et al., 1991). Zorrilla et al.
(2000) related the textural and cooking parameters with the plate temperature and gap
thickness between plates during double-sided cooking of meat patties as an attempt
to relate physical results to any change in the heat transfer mechanism. For correlations,
the volume averaged temperature, T, was used:
∫∫∫ T(z, t) dV ∫
L
T(z, t ) dz
T= V
= 0
(20.16)
∫∫∫ dV
V
L
where T(z,t) is the temperature profile inside the patty for a one-dimensional model,
and L is the gap thickness between plates. An example of the regression surfaces
obtained is shown in Figure 20.5. In this case, cooking loss is one of the cooking
parameters studied.

38
Cooking loss (%)

38
34
Cooking loss (%)

34
30
30
26
26
22
)
90
e (°C
22 85 tur
80
p era
11 75 tem
Gap th 10.5 70 ge
d
icknes 10 65 era
s (mm) 9.5 e-av
lum
Vo
FIGURE 20.5 Cooking loss values correlated with volume averaged temperature and gap
thickness between plates.
The optimization problem can be formulated as follows: Find the heating policy
of a hamburger contact cooking process in order to obtain minimum cooking loss while
ensuring the mandatory level of microbiological destruction and final temperature at
the coldest point. At present, the optimization process is a subject of current study.
20.6 CONCLUSIONS
Mathematical models based on classical transport phenomena equations satisfacto-
rily predicted the temperature profiles inside hamburger patties during double-sided
contact cooking. A model considering a one-dimensional geometry appropriately
predicts temperature profiles at the geometric center, while a model for a two-
dimensional cylindrical geometry provides a temperature history at regions close to
the circumferential edge of the patty, which is not possible with a one-dimensional
model. The contact heat transfer coefficient is one of the parameters needed to
complete the mathematical formulation. Since little information is available on heat
transfer coefficient values for solid foods, a detailed discussion was included. The
contact heat transfer coefficient changes during the cooking process. The small gap
thickness enhances the contact between a patty and the grill surfaces. A Teflon release
sheet offers finite resistance to heat transfer to the hamburger patties during cooking.
Higher heat transfer coefficient values after reaching maximum value were found
with the low set grill temperature and may result from the adhesion phenomenon
occurring between the patty surface and the grill surfaces.
NOMENCLATURE
a Radius of the patty, m
Cp Apparent specific heat, J/kg°C

3
g Heat generation term, J/m sec
2
h Contact heat transfer coefficient, W/m °C
2
hc Combined radiation and convection heat transfer coefficient, W/m °C
3
H Enthalpy, J/m
k Thermal conductivity in the core, W/m°C
kcrust Crust thermal conductivity, W/m°C
L Gap thickness, m
r Cylindrical coordinate, m
R Position of moving boundary that separates the crust region from the core
region in the radial direction, m
S1, S2 Positions of moving boundary that separate the crust region from the core
region in the axial direction, m
t Time, sec
T Temperature, °C
T Volume averaged temperature, °C
Ta Surrounding air temperature, °C
Tb Boiling temperature, °C
Tp1, Tp2 Plate temperatures, °C
T0 Initial temperature, °C
xf Fat content, decimal fraction
xw Water content, decimal fraction
z Cylindrical coordinate, m
GREEK SYMBOLS
λv Latent heat of water vaporization, J/kg
3
ρ Hamburger density, kg/m
φ Cylindrical coordinate
REFERENCES
Baghe-Khandan, M.S., Okos, M.R., and Sweat, V.E., The thermal conductivity of beef as
affected by temperature and composition, Trans. ASAE, 25, 1118–1122, 1982.
Banga, J.R., Alonso, A.A., and Singh, R.P., Stochastic dynamic optimization of batch and
semi-continuous bioprocesses, Biotechnol. Prog., 13, 326–335, 1997.
Banga, J.R., Perez-Martin, R.I., Gallardo, J.M., and Casares, J.J., Optimization of the thermal
processing of conduction-heated canned foods: study of several objective functions,
J. Food Eng., 14, 25–51, 1991.
Beilken, S.L., Eadie, L.M., Griffiths, I., Jones, P.N., and Harris, P.V., Assessment of the textural
quality of meat patties: correlation of instrumental and sensory attributes, J. Food
Sci., 56, 1465–1469, 1991.
Berry, B.W., Fat level, high temperature cooking and degree of doneness affect sensory,
chemical and physical properties of beef patties, J. Food Sci., 59, 10–14, 1994.
Bigner-George, M.E. and Berry, B.W., Thawing prior to cooking affects sensory, shear force,
and cooking properties of beef patties, J. Food Sci., 65, 2–8, 2000.

Cleland, D.J. and Valentas, K.J., Prediction of freezing time and design of food freezers, in
Handbook of Food Engineering Practice, Valentas, K.J., Rotstein, E., and Singh, R.P.,
Eds., CRC Press LLC, Boca Raton, FL, 1997, pp. 71–123.
Dagerskog, M., Pan frying of meat patties I. A study of heat and mass transfer, Lebensm.-
Wiss. Technol., 12, 217–224, 1979a.
Dagerskog, M., Pan frying of meat patties II. Influence of processing conditions on heat
transfer, crust color formation, cooking losses and sensory quality, Lebensm.-Wiss.
Technol., 12, 225–230, 1979b.
Dagerskog, M. and Bengtsson, N.E., Pan frying of meat patties: relationship among crust
formation, yield, composition, and processing conditions, Lebensm.-Wiss. Technol.,
7, 202–207, 1974.
Dagerskog, M. and Sörenfors, P., A comparison between four different methods of frying
meat patties I. Heat transfer, yield and crust formation, Lebensm.-Wiss. Technol., 11,
306–311, 1978.
Dreeling, N., Allen, P., and Butler, F., Effect of cooking method on sensory and instrumental
texture attributes of low-fat beefburgers, Lebensm.-Wiss. Technol., 33, 234–238, 2000.
D’Sa, E.M., Harrrison, M.A., Williams, S.E., and Broccoli, M.H., Effectiveness of two
cooking systems in destroying Escherichia coli O157:H7 and Listeria monocytogenes
in ground beef patties, J. Food Protection, 63, 894–899, 2000.
Farkas, B.E., Singh, R.P., and Rumsey, T.R., Modeling heat and mass transfer in immersion
frying. I. Model development, J. Food Eng., 29, 211–226, 1996.
FDA, Food Code, chapter 3, 3–401.11. http://vm.cfsan.fda.gov/~dms/fc-3.html, 1997.
Geankoplis, C.J., Transport Processes and Unit Operation, 3rd ed., Prentice Hall, Englewood
Cliffs, NJ, 1993.
Houšová, J. and Topinka, P., Heat transfer during contact cooking of minced meat patties,
J. Food Eng., 4, 169–188, 1985.
Ikediala, J.N., Correia, L.R., Fenton, G.A., and Ben-Abdallah, N., Finite element modeling
of heat transfer in meat patties during single-sided pan-frying, J. Food Sci., 61, 796–802,
1996.
Ju, J. and Mittal, G.S., Effects of fat-substitutes, fat levels and cooking methods on the quality
of beef patties, J. Food Process. Preserv., 23, 87–107, 1999.
Ju, J. and Mittal, G.S., Relationships of physical properties of fat-substitutes, cooking methods
and fat levels with quality of ground beef patties, J. Food Process. Preserv., 24,
125–142, 2000.
Lawrie, R.A., Meat Science, 5th ed., Pergamon Press, Oxford, 1991.
Madhusudana, C.V., Thermal Contact Conductance, Springer-Verlag, New York, 1996.
Mannapperuma, J.D., Thawing of foods in humid air, dissertation, University of California,
Davis, 1988.
Mannapperuma, J.D. and Singh, R.P., Prediction of freezing and thawing times of foods using
a numerical method based on enthalpy formulation, J. Food Sci., 53, 626–630, 1988.
NCBA, (National Cattlemen’s Beef Association) on the Internet at: http://www.
beeffood service.com/working/fs.dll?beef, 1998.
Ozisik, M.N., Heat Conduction, John Wiley & Sons, New York, 1993.
Ozisik, M.N., Finite Difference Methods in Heat Transfer, CRC Press, Boca Raton, FL, 1994.
Pan, Z., Predictive modeling and optimization of hamburger patty contact-cooking process,
dissertation, University of California, Davis, 1998.
Pan, Z., Singh, R.P., and Rumsey, T.R., Predictive modeling of contact-heating process for
cooking a hamburger patty, J. Food Eng., 46, 9–19, 2000.
Rahman, S., Food Properties Handbook, CRC Press LLC, Boca Raton, FL, 1995.
Singh, R.P., Moving boundaries in food engineering, Food Technol., 54, 44–53, 2000.

Sweat, V.E., Thermal properties of foods, in Engineering Properties of Foods, Rao, M.A. and
Rizvi, S.S.H., Eds., Marcel Dekker, New York, 1994, pp. 99–138.
Urbicain, M.J. and Lozano, J.E., Thermal and rheological properties of foodstuffs, in Hand-
book of Food Engineering Practice, Valentas, K.J., Rotstein, E., and Singh, R.P., Eds.,
CRC Press LLC, Boca Raton, FL, 1997, pp. 425–486.
USDA, USDA urges consumers to use food thermometer when cooking ground beef patties,
Food Safety and Inspection Service, United States Department of Agriculture,
Washington, DC http://www.fsis.usda.gov/OA/news/colorpr.htm, 1998.
Vijayan, J. and Singh, R.P., Heat transfer during immersion frying of frozen foods, J. Food
Eng., 34, 293–314, 1997.
Wichchukit, S., Zorrilla, S.E., and Singh, R.P., Heat transfer coefficients in contact cooking
of meat patties as influenced by process conditions, presented at the Institute of Food
Technologists Annual Meeting, Dallas, 2000.
Zorrilla, S.E., Rovedo, C.O., and Singh, R.P., A new approach to correlate textural and cooking
parameters with operating conditions during double-sided cooking of meat patties,
J. Texture Stud., 31, 499–523, 2000.
Zorrilla, S.E. and Singh, R.P., Heat transfer in meat patties during double-sided cooking, Food
Sci. Technol. Res., 6, 130–135, 2000a.
Zorrilla, S.E. and Singh, R.P., Heat transfer in double-sided cooking of meat patties consid-
ering two-dimensional geometry and radial shrinkage, presented at the Institute of
Food Technologists Annual Meeting, Dallas, 2000b.

Thermal Processing
21 of Particulate Foods by
Steam Injection. Part 1.
Heating Rate Index
for Diced Vegetables
CONTENTS
21.1 Introduction
21.2 Theoretical Considerations
21.3.1 Equipment Design
21.3.2 Data Acquisition
21.3.3 Equipment Operation
21.3.4 Food Samples and Test Sensor Preparation
21.3.5 Data Analysis
21.4.1 Time–Temperature Data
21.4.1.1 Regression for fh and jh Values
21.4.1.2 Temperature at the Food Surface
21.4.2 Heating Rate Index (fh) and the Lag Factor (jh)
21.4.2.1 fhc Values
21.4.2.2 Lag Factor and j Values
21.4.2.3 Errors Associated with fh and jh Values
21.4.2.4 Particle-to-Particle Interaction
21.4.2.5 Steam Flow Direction
21.4.2.6 SMFR and Steam Temperature
21.4.3 Heat Transfer Coefficient (h) and the Biot Number (Bi)
21.4.4 Product Quality
21.4.5 Moisture Loss
21.4.6 Process Implications on Product Blanching/Sterilization

21.5 Conclusions
Nomenclature
References
21.1 INTRODUCTION
Although steam is commercially employed to sterilize and blanch food products,
there is a lack of readily available data that can be used with confidence to simulate
packed bed heating of diced vegetables by steam injection. Basic parameters and
properties required are the food product thermal diffusivity at temperatures over
100°C and the convective surface heat transfer coefficient (h value) for steam. Data
on h values for food processing applications range from 400 (Zhang and Cavalieri,
2 2
1991) to 12,000 W/m °C (Tung et al., 1990). An h value of about 5000 W/m °C is
commonly employed (Skjöldebrand and Ohlsson, 1993) for steam heating, but for
a 12-mm food cube this provides a Biot number (Bi) of about 50, indicating infinite
resistance to surface heat transfer. This may not be so in light of data presented by
Rumsey et al. (1980), Pannu et al. (1990) and Zhang and Cavalieri (1991), which
show that 0.1 ≤ Bi ≤ 40. Also, very little work has been documented in the area of
packed bed processing of moist food solids with steam.
Thus, the objectives of this study were to investigate the steam injection packed
bed heating of potato and carrot cubes/slices. Food center and surface temperatures
were measured under a variety of process conditions. The specific objective was to
assess the influence of steam temperature, flow rate, flow direction (upward and
downward), food particle size/shape, and particle-to-particle interaction on product
1
temperature and the food particle heating rate (fh) during packed bed heating.
21.2 THEORETICAL CONSIDERATIONS

The transient heat transfer equation for an object of simple shape, initially at a
uniform temperature Ti, exposed to a step-change immersion into a heating medium
at temperature Ts, can be expressed as follows (Luikov, 1968):
∞
Ts − T( x,t )
θ object =
Ts − Ti
= ∑A B e
n =1
n n
− β n2 Fo
(21.1)
Values for An, Bn, and βn are dependent on object shape (infinite slab, sphere,
or infinite cylinder), and T(x,t) (or T without a subscript) represents the time-dependent
temperature at a fixed location x within the solid. The Fourier number is defined as
2
Fo = αt/R , with α being the thermal diffusivity, t the time, and R the half thickness.
Furthermore, the infinite summation can be approximated by only the first term (n = 1),
provided Fo > 0.2 (Heisler, 1947; Singh, 1982). Using first term approximation and
by taking logarithms of both sides, Equation (21.1) simplifies to Equation (21.2).
1
The f and j values defined and used here are the true “lumped” form of the analytical transient heat
conduction equation, with f as the exponential component and j the first two terms (A and B) of Equation
(21.1). The f and j values are used for comparison of products and thermocouple location.

For infinite slabs and cubes, the time-temperature data can be analyzed by making
the appropriate substitutions from Equations (21.4) and (21.5), respectively, into
Equation (21.2).
 Τ − Τi 
t = fh ln jh s  (21.2)
 Τs − Τ 
2sin β1  β1 x 
A1 = ; B1 = cos  and β1tan β1 = Bi (21.3)
β1 + sin β1cos β1  R 
Infinite slab:
R2
fh = and jh = A1B1 (21.4)
(β1 )2 α
Cube:
R2
fh = and jh = (A1B1 )3 (21.5)
3(β1 )2 α
Equation (21.2) is extensively used for evaluating the straight line segment of
the heating curve, with fh and jh representing the negative inverse slope (heating rate
index) and the intercept, respectively, obtained from a semilogarithmic plot of the
2
temperature ratio at the center (θc) vs. time.
A second set of subscripts, c and s, representing the center or surface, respec-
tively, are added to fh and jh. Thus, fhc and fhs represent the f value at the center and
at the surface layer, respectively. Equations (21.4) and (21.5) show that f values are
position independent (fhc = fhs), but j values are not (jhc ≠ jhs) because B1 is location
dependent (Figure 21.1). Care has to be taken in computing the jhs value of a cube
because it is location sensitive. However, at the geometric center, jhc = A1, as B1 = 1
since x = 0.

21.3.1 EQUIPMENT DESIGN
Details of the test apparatus are presented in Figure 21.2. Steam enters from the
bottom into the annular jacket, which is equipped with a steam trap and an electric
heating coil. A three-way valve is used to direct good quality (dry) steam exiting
from the top of the annular jacket into the processing chamber for product treatment.
Two three-way valves are required (Figure 21.2, top) to ensure continuous steam
flow through the processing chamber or to redirect steam flow via the bypass line.
Steam exits as water after passing through a steam condensation unit. Flexible hoses
2
Note that a factor of 2.303 is used with the decimal logarithm scale (log 10). For the log 10 scale:
fh = 2.303⋅fh. The natural logarithm (ln) scale was used in this study.

Case 1
Center of X-Y plane Y
Surface of Z plane
-X Case 3
Surface of all 3 planes
X, Y and Z
Food
Cube
Case 4
Surface of Y plane
Off-center on X & Z planes
Case 2 -Z
Surface of Y & Z planes
Off-center on X plane
FIGURE 21.1 Location influence for estimating j values.
(hose-1 and hose-2) were used to redirect steam flow through the processing chamber
via the three-way valves. Thus, steam flow direction (upward or downward) into the
processing chamber can be changed by switching the flexible hoses at locations A-
A and B-B. Figure 21.2 depicts steam flowing in the upward direction. Each of the
four thermocouple locations, T1–T4, is equipped with two thermocouples and a
pressure gauge. One thermocouple from each of the four points was connected to
the data acquisition unit. The second thermocouple was connected to a digital display
unit for visual verification of pressure and temperature.
21.3.2 DATA ACQUISITION

®
The data acquisition system consisted of a Personal Computer (PC), MetraByte
® ®
hardware (MetraByte Corporation, Taunton, MA), the Lotus 1–2–3 spreadsheet
®
program (Lotus Development Corporation, Cambridge, MA) and Labtec Note-
®
book (Laboratory Technologies Corporation, Wilmington, MA) software packages.
®
The MetraByte hardware package included a DASH-8 eight-channel 12-bit high-
®
speed A/D converter and timer/counter board and an EXP-16 expansion board with
16 pairs of screw terminals for the attachment of thermocouple wires. The software
package provided real time graphic display of the heating process.
21.3.3 EQUIPMENT OPERATION

The pressure was regulated using a Taylor Lin-E-Aire valve (Taylor Instrument
Company, Broadview Heights, OH) and controlled pneumatically by an Electromax
digital process controller (Leeds and Northrup, North Wales, PA). For system start-
up, approximate system pressure and temperature were achieved in the bypass mode
with the digital process controller. Steam mass flow rate (SMFR) was determined by
collecting condensate discharge for 120 sec (Figure 21.2, top). Condensing steam to
water is the most reliable method for obtaining data on steam flow rate. Depending on

Personal
Hose-1
Computer Bypass Line
T-4
Food Container B-B T-2 3-Way Valve
Processing Chamber
Needle Valve
Annular Jacket
T-1
PRV: Pressure Cold Water
A-A
Regulating Valve
T-3 Hose-2
Steam Condensation
Steam for Mass Flow Rate
Supply Temp. Pressure Measurement
Measurement
Steam to Water
Steam Out
Cover Plate
Thermocouples
Rubber Seals Dimensions & Details

Process Simulator
Electric Heating Element Material: Aluminum
Height = 21 cm
6-Thermocouple Probe I D = 15.2 cm
Annular space = 2.5 cm
Food Container Condensation Unit
Material: Copper tubing
Annular Jacket
Tube Dia. = 1.9 cm
(Steam Heating)
Coil height = 40 cm
Coil dia. = 20 cm
Processing Chamber
# of turns = 12
A.C. Supply
Steam In Steam Supply
Pressure: 275 – 550 kPa
Steam Trap Quality: Unknown
Steam from Jacket Processing Chamber

to Processing Chamber Pressure Release Valve
FIGURE 21.2 Schematics of the laboratory apparatus for heating diced vegetables in steam.
the desired SMFR, flow conditions were established by manually adjusting the
needle valve (#SS-1RS8; Whitey Co., Highland Heights, OH) located prior to the
condensation unit (Figure 21.2), by restricting steam discharge.
The annular jacket performs four tasks:
1. It acts as a buffer tank.

2. It removes condensed water through the steam trap.

3. It acts as a thermal jacket for the processing chamber.
4. It performs steam superheating.
For all experiments, a few degrees of superheat (5–15°C) were provided.

Detailed information about the equipment and its operation has been presented
elsewhere (Pannu, 1992).
All test containers were flanged to facilitate their installation into the heating
chamber. The container flange fits into a recessed slot with thermocouple wires sand-
wiched between two silicone rubber rings. This ensures good sealing; no leakage of
steam was observed. For each test, the food batch was weighed and transferred to the
test container in layers to facilitate positioning of the test sensors and thermocouple
wires. Two screws were inserted from the bottom of the flange to attach the test
container with the two rubber rings and thermocouple wires to the cover plate. The
assembly was placed next to the simulator to facilitate the connection of thermocouple
wires to the data logger. Subsequently, the cover plate/food container assembly was
installed in place and tightly secured with four butterfly nuts. After commencing data
acquisition, steam was diverted to the processing chamber via the three-way valve.
The data acquisition system provided real time graphic display of the heating
process. Temperatures were recorded until the center temperature of food particles
reached that of the heating medium; the steam supply to the processing chamber was
then cut off. The product was cooled to 100°C by slow depressurization of the heating
chamber. Data acquisition was terminated when the product had cooled to 100°C. The
food container was then removed, product quality visually inspected, and thermocou-
ple location/placement verified. SMFR was measured before and during the test and
after termination of heating. Temperature data from the steam inlet/exit, preheating
chamber, heating chamber, food surface, and center and other locations were used to
evaluate the performance of the equipment under selected processing conditions.
Time-temperature data were recorded at 1 sec intervals with strategically located
fine wire (36-gauge) copper-constantan thermocouples. Special test sensors were
fabricated by positioning two thermocouples into the food pieces (Figure 21.3a).
These were embedded in the food material to register the temperature history of
36-gauge type-T 1/2 cube

thermocouple wire thickness
Food
Cube
Wooden toothpick
Fine cord
diameter = 1.2 mm
(a) (b)
FIGURE 21.3 (a) Placement of thermocouple probe in the food cube. (b) Details of the
thermocouple probe.

individual solids. Heating time of the food particulates was continually monitored
and manually controlled. Steam supply was shut off and redirected through the
bypass line when the food particle center temperature reached that of steam. The
steam flowing through the processor was condensed to liquid water for determining
the system steam mass flow rate (SMFR). Since process come-up time was very
short (~5 sec), stable processing conditions were achieved, and heat losses were
negligible with a steam jacket surrounding the food treatment chamber.
21.3.4 FOOD SAMPLES AND TEST SENSOR PREPARATION

Food cubes were prepared by cutting peeled potatoes and carrots into slices and then
passing the slices through a french fry cutter. The material was sorted, washed, surface
dried with paper towels, sealed in plastic containers, and set aside for 2 h to allow the
product to attain a uniform initial temperature (Ti). Temperatures at the center and the
surface layer of a food particle were measured by installing special thermocouple
probes into selected food pieces (Figure 21.3b). The probes were constructed with
thermocouple junctions positioned half the food piece thickness apart and were secured
on opposite sides (180° apart) of a wooden toothpick with a fine cotton thread.
A 1.2-mm hole was drilled into the test sample to facilitate the correct positioning
of the thermocouples and to prevent particle shape distortion (Figure 21.3a). The
wooden toothpick assembly was soaked in water for about 2 h prior to installation
into the test piece to avoid migration of water from food to wood and to minimize
the thermal insulation effects of wood. Only food cubes of uniform size (measured
with a digital caliper) and shape were selected for the construction of the test sensors.
Three food sensors were positioned at the top, bottom, and center of the food
bed. The top and bottom sensors were placed one food layer away from the top
layer and bottom layer of the food bed, respectively. Experiments were conducted
with approximately 180 g of food and in a container that resembled a 300 × 400 can
(Pannu, 1992). Potato and carrot pieces were processed in two shapes (cubes and
slices) and two sizes. Moisture content was determined by vacuum drying in a
laboratory oven at 70°C for 48 h. Quality and physical structure of the processed
food cubes were examined visually.
21.3.5 DATA ANALYSIS

Interactive Lotus 1-2-3 macro programs were developed (Pannu, 1992) to analyze
the data and obtain temperature–time graphs. The linear segment of the heating
curve was used to obtain an estimate of ƒh and the corresponding intercept jh.

21.4.1 TIME–TEMPERATURE DATA
Typical time–temperature data for steam flowing downward at a rate of 3.8 g/sec
through a bed of large (12 mm) potato cubes are shown in Table 21.1. Temperatures
of steam from the supply line to the processor are in column 2, and those of steam
exiting from the superheater (annular jacket) in column 3. Data for steam entering/exiting

TABLE 21.1
a
Typical Time–Temperature Data for Steam Flowing Downward at a
Rate of 3.8 g/sec through a Bed of Potato Cubes (12 mm)
Sensor Location in the Food Bed
1 2 3 4 5 6 7 8 9 10 11 12
Bottom Center Top
1
Time V sup V aj V top V bot Fc Fs Fc Fs Fc Fs V pc
(sec) (°C) (°C) (°C) (°C) (°C) (°C) (°C) (°C) (°C) (°C) (°C)
–4 124.2 132.7 28.3 32.4 20.0 17.2 18.2 18.2 20.0 28.9 63.0
–3 124.5 132.7 28.6 32.4 20.0 17.2 17.9 18.2 20.0 29.2 63.0
–2 124.5 132.7 28.6 32.4 20.0 17.6 17.9 18.2 20.0 29.2 63.0
–1 124.2 132.7 28.3 32.4 20.0 17.2 18.2 18.2 20.0 29.5 63.3
0 124.7 131.2 28.3 32.4 20.0 17.6 18.2 18.2 20.3 29.5 63.3
1 125.7 134.2 42.9 33.0 19.7 17.6 18.2 18.5 20.6 30.1 63.3
2 125.2 131.2 102.1 36.5 20.0 61.9 18.8 34.8 21.2 75.4 63.0
3 123.9 122.2 115.3 115.5 21.8 89.9 21.5 74.3 23.0 103.4 93.7
4 123.4 123.7 121.7 122.2 24.2 107.3 23.6 85.9 24.7 114.3 110.1
5 123.9 126.7 122.9 123.2 26.8 114.0 25.9 93.4 25.9 117.8 116.3
6 123.9 129.2 123.7 123.9 28.9 118.6 26.8 99.5 26.8 120.4 121.9
10 125.0 130.2 122.4 122.7 34.2 121.4 31.0 109.4 30.1 121.7 122.9
15 123.9 130.5 122.2 122.2 38.6 121.9 35.4 113.7 33.6 121.9 122.7
20 123.9 130.7 122.2 122.4 43.7 122.1 40.9 114.8 39.4 122.1 123.2
25 123.9 131.2 122.7 122.7 50.3 122.3 48.3 116.8 46.3 122.2 123.7
30 124.2 131.5 122.7 122.7 57.4 122.4 55.7 117.3 54.3 122.4 123.9
35 123.9 131.7 123.2 123.2 64.9 122.5 63.0 118.4 62.4 122.6 123.9
40 123.9 131.7 123.2 123.2 71.8 122.6 70.2 118.6 70.2 122.4 123.9
45 124.2 131.7 123.2 123.3 78.7 122.8 75.9 118.6 77.0 122.8 123.9
50 124.2 131.7 123.2 123.4 84.9 122.9 81.9 119.4 83.5 123.1 124.2
55 124.4 131.7 123.2 123.4 90.2 123.2 87.3 119.6 89.2 122.9 123.9
60 124.2 132.0 123.2 123.4 94.7 123.2 91.5 120.2 94.2 123.2 123.9
65 124.2 131.7 123.4 123.2 98.9 123.2 95.3 120.5 98.4 123.4 124.2
Cooling by Depressurization
133 124.2 132.5 122.4 122.7 120.1 123.2 118.6 122.2 120.1 122.4 123.9
134 124.5 132.5 121.9 122.2 120.4 122.9 118.9 122.2 120.1 122.2 123.4
135 124.2 132.5 121.9 121.4 120.1 122.4 119.1 122.2 120.4 121.9 122.9
136 124.5 132.5 121.7 120.6 120.4 121.9 119.1 121.9 120.4 121.7 122.4
138 124.5 132.7 118.9 119.4 120.1 119.9 119.1 120.6 120.1 120.1 120.6
140 124.5 132.2 116.8 117.6 119.1 118.1 119.1 118.6 119.1 118.6 118.4
155 124.2 132.2 103.2 100.7 101.5 100.5 101.8 101.0 101.8 101.3 101.3
160 124.2 132.2 102.9 100.5 100.5 99.5 100.2 99.5 100.5 100.0 100.0
Note: V: vapor; sup: steam supply; aj: exit at annular jacket; bot: bottom location; pc:
processing chamber; Fc: food center; Fs: food surface.
a
Time–temperature data recorded at 1 sec intervals have been abbreviated for presentation.

at the top and bottom of the processing chamber, respectively, are in columns 4 and 5.
Column 12 provides steam temperatures inside the chamber; the data in columns 6
through 11 are from food sensors. The time scale in column 1 was corrected to reflect
the true time zero; this was accomplished by comparing temperature data in columns
4 or 5. A sudden jump in temperature indicated the time when steam first entered the
processing chamber and was assigned the value of t = 1 sec.
21.4.1.1 Regression for fh and jh Values
Results for fh and jh can vary depending on the values of Ts and Ti and the range selected
for regression (Larkin, 1989). To overcome this problem and eliminate bias, Lotus
macros were used to carry out the regression analysis. Ts was computed as an average
of 93 temperature readings recorded in columns 4, 5, and 12 (Table 21.1). Ti for each
food sensor was computed as an average of the food center temperature between t =
–5 and 0 sec. The time period selected for the regression analysis was t = 50 to 100
sec for f and j values at the center of the large cube and from 15 to 35 sec for surface
temperature data. For the small cubes, the range selected was between 40 and 80 sec
for center temperature data and between 10 and 25 sec for surface temperature data.
−7
The regression range was selected by calculating te with αpotato = 1.6 × 10
2
m /sec (Kostaropoulos et al., 1975) for Fo = 0.2. An estimate for the isothermal
heating time (te), at which the curvilinear portion of a heating curve terminates, can
also be obtained with Equation (21.6) (Hayakawa, 1982). For a cube, jhc ≈ 2.0; by
assuming that fhc = 35 × 2.303 (log 10 scale), te ≈ 55 sec. A te value of 45 sec was
obtained by using Fo = 0.2. Thus, the time periods selected for regression were
justifiable. However, these methods cannot be applied for surface temperature data.
te = 0.7fh( jh – 1) (21.6)
Semilogarithmic plots obtained from temperatures registered at the food center

and surface layer are presented in Figure 21.4. A value for fhs is only possible
0.5
0
Temp. Ratio (Ta – T)(Ta – Ti)
Temperature Ratio (in-scale)
-0.5
-1
-1.5
-2
-2.5
-3
-3.5
Food center
-4 Food surface
-4.5
0 20 40 60 80 100 120
Heating Time (sec)
FIGURE 21.4 Semilogarithmic plots from packed bed heating of large (11.5-mm) carrot
cubes at 126°C with steam.

130 130
120 120
110 (A-1) 110 (B-1)
100 100
90 90
Temperature (C)
80 80
70 70
60 60
50 50
40 Steam 40 Steam
F-top F-top
30 F-cen 30 F-cen
F-bot 20 F-bot
20
10 10
-10 10 30 50 70 90 110 130 -10 10 30 50 70 90 110 130
Heating time (sec) Heating time (sec)
0.0 0.0
-0.2 -0.2
Temp Ratio = (Ta – T)/(Ta – Ti)
-0.4 Temp Ratio = (Ta – T)/(Ta – Ti) -0.4
-0.6 (A-2) -0.6 (B-2)

-0.8 -0.8
-1.0
-1.0
-1.2
-1.2
-1.4
-1.4
-1.6
-1.6
-1.8 Upward Flow Downward Flow
-2.0 -1.8
F-top F-top
-2.2 -2.0 F-cen
F-cen
-2.4 F-bot -2.2 F-bot
-2.6 -2.4
0 20 40 60 80 100 0 20 40 60 80 100
Heating time (sec) Heating time (sec)
FIGURE 21.5 Comparing temperature profiles for upward (A) and downward (B) flow steam
trough a bed of 11.7-mm potato cubes processed at 125°C with steam. Bottom plots (A-2
and B-2) compare f values at food bed top, center, and bottom locations.
provided the surface temperature is lower than that of the heating medium. Data
2
for regression analysis provided R values of 0.97 or better for fhc, as opposed to
0.92 or better for fhs.
Typical temperature data and the dimensionless temperature ratio results (ln
scale) obtained from food cubes placed at the top, center, and bottom locations
within the food bed are presented in Figure 21.5. The two cases presented here show
steam flow in the upward (A1) and downward (B1) directions through a bed of large
(11.7 mm length) potato cubes. Data in plots A2 and B2 were used to obtain the
heating rate index (slope: fh) and the intercept (jh). SMFR and steam temperatures
for these experiments were approximately 5 g/sec and 124°C, respectively.
Figure 21.5 and Tables 21.1 and 21.2 show that the food sensors registered nearly
the same initial temperature, but the temperatures changed rapidly as steam was
injected into the processing chamber, indicating that food was heated uniformly
throughout the bed since the transducers located at the top, center, and bottom
positions registered similar temperature increases.

21.4.1.2 Temperature at the Food Surface
Food surface temperatures (Figure 21.4) were obtained from a 12-mm carrot cube
located at the center of the food bed and processed at 126°C with steam flowing
upwards. Temperature recorded at the food surface is highlighted in Table 21.1. These
data show that food surface temperatures rose rapidly but took approximately 20–40
sec to reach steam temperature. The fact that temperatures measured at the food
surface were slightly lower than the temperature of the steam indicated that Bi was
less than 40, suggesting that high temperature short time (HTST) processing of diced
vegetables involves finite resistance to surface heat transfer. The h value data eval-
uated in this work also show that Bi was less than 40.
21.4.2 HEATING RATE INDEX (fh) AND THE LAG FACTOR (jh)
21.4.2.1 fhc Values
Tables 21.2 and 21.3 provide results for fhc at the top, center, and bottom locations
of the food bed and for fhs, jhc and jhs. Data for the latter three are lumped as an
average of the data obtained at the top, center, and bottom locations. Additional
experimental runs were carried out with the large potato cubes to study the influence
of SMFR and steam temperature on product heating. The initiation of the linear
heating segment after approximately 45 sec (center) and 10 sec (surface) showed
that the previously defined ranges for regression analysis are correct (Figure 21.4).
In general, the experimental values for fhc and fhs obtained from the heating of potato
cubes varied between 31 and 35 sec for the larger cubes and between 23 and 26 sec
for the smaller cubes. Carrot samples provided slightly lower f values, ranging
between 28 and 30 sec for the larger cubes and between 21 and 23 sec for the smaller
cubes. Carrot cubes heated faster because they have a higher thermal diffusivity.
The data also show that f values at the cube surface were similar to those at the
food cube center. However, in some instances, larger than general values (under-
scored) for fhc were obtained. This issue, together with j values, is discussed later.
Potatoes and carrots were also processed in the form of cylindrical slices/slabs.
The diameter to thickness ratio indicated in Tables 21.2 and 21.3 refers to the fact
that the thin slices were cylindrical. Results show that even for a cylinder thickness
to diameter ratio of 1:5, a criterion for an infinite slab was not satisfied, since fh slab <
3fh cube. For a ratio of 1:5, the lateral surface of the cylinder represents 30% of its
total surface area. Thus, f values for slabs should be less than three times those of
cubes of equivalent thickness. It is interesting to note that a 1:5 ratio provided an fh
value 2.3 times larger, whereas a 1:4 ratio provided an fh value twice as large as that
of a cube of the same thickness.
21.4.2.2 Lag Factor and j Values
The jhc values obtained for food cubes were lower than the theoretical value of 2.0.
Since j values are location sensitive, small directional errors at the center of food cubes
were probably amplified. Average jhc values of 1.69 and 1.63 were obtained for the

TABLE 21.2
fh and jh for Steam-Injection Heating of Diced Potato Samples in Packed Beds
f Value at Particle
a
Center Surface j Values at
Steam
Run Temp Flow SMFR Bottom Center Top Particle
No. °C Direction (g/sec) (sec) (sec) (sec) (sec) Center Surface
Large Cubes (Length = 11.7 mm)

1.1 126.5 Up 1.15 34.0 34.9 32.4 32.9 1.688 0.108
c c
1.2 124.2 Up 1.32 40.5 45.0 32.0 31.8 1.557 0.113
1.3 118.2 Up 1.97 31.5 32.1 31.6 33.2 1.747 0.117
1.4 123.3 Up 2.33 32.2 33.7 33.3 33.1 1.903 0.117
1.5 124.1 Up 2.53 34.3 34.9 33.6 31.3 1.726 0.121
1.6 123.9 Up 3.88 34.5 34.9 34.5 34.0 1.765 0.101
1.7 123.7 Up 5.25 33.5 33.8 32.7 32.2 1.663 0.103
1.8 131.6 Up 7.05 35.0 34.7 34.1 32.1 1.474 0.108
c
1.9 131.5 Up 7.27 33.3 49.5 31.5 34.0 1.845 0.103
1.10 124.4 Down 1.27 31.0 34.2 31.9 33.3 1.830 0.109
1.11 118.2 Down 1.95 31.8 32.3 30.7 32.3 1.645 0.108
1.12 119.0 Down 1.97 32.8 34.2 30.9 32.8 1.552 0.125
1.13 124.1 Down 2.55 33.8 38.0 32.4 31.6 1.663 0.106
1.14 123.8 Down 3.83 32.5 37.8 31.8 34.8 1.711 0.117
1.15 123.8 Down 5.28 34.8 37.0 34.5 31.7 1.651 0.119
1.16 130.5 Down 7.32 32.1 37.4 32.3 32.6 1.619 0.110
Small Cubes (Length = 9.9 mm)

2.1 125.6 Up 1.32 24.4 25.7 24.1 24.4 1.683 0.115
2.2 123.8 Up 2.50 24.5 25.9 23.8 24.2 1.693 0.118
2.3 124.1 Down 1.22 24.0 24.2 23.9 23.8 1.487 0.123
c
2.4 130.4 Down 2.58 22.7 33.9 23.9 22.8 1.639 0.124
b
Potato Slabs (Thickness = 9.9 mm)
3.2 124.9 Up 1.30 56.1 59.2 59.3 55.4 1.119 0.096
3.1 124.6 Up 2.40 55.8 57.6 52.6 53.2 1.158 0.051
3.4 125.2 Down 1.32 59.0 63.8 53.2 57.2 1.116 0.077
c
3.3 124.6 Down 2.53 58.3 101.2 56.7 58.1 1.131 0.081
Note: SMFR, steam mass flow rate.

a
f values at particle center are at bed locations: bottom, center, and top.
b
The length to thickness ratio of the slabs was greater than 5.
c
Data out of range.
large and small potato cubes and 1.90 and 1.58 for carrot cubes, respectively. The
experimental average jhs values for large/small potato and carrot cubes obtained from
the data (Tables 21.2 and 21.3) were 0.112, 0.12, 0.111 and 0.114, respectively, which
compare favorably with the theoretical value of 0.15 (1.26 * 1.26 * 0.095 = 0.15).

TABLE 21.3
fh and jh for Steam-Injection Heating of Diced Carrot Samples in Packed Beds
f Value at Particle
a
Center Surface j Values
Steam
Run Temp. Flow SMFR Bottom Center Top at Particle
No. °C Direction (g/sec) (sec) (sec) (sec) (sec) Center Surface
Large Carrot Cubes (Length = 11.5 mm)

1.1 126.1 Up 1.32 29.7 28.9 29.7 27.6 1.841 0.117
1.2 118.6 Up 1.85 28.5 29.6 28.8 28.3 2.058 0.108
1.3 126.7 Up 2.55 29.2 29.3 28.9 29.1 1.857 0.121
1.4 117.9 Down 1.92 29.1 32.7 28.6 28.7 1.908 0.111
1.5 125.9 Down 2.02 30.2 29.7 29.1 29.4 1.839 0.105
1.6 126.7 Down 2.58 29.6 30.2 29.4 28.6 1.783 0.103
Small Carrot Cubes (Length = 9.8 mm)

2.1 125.3 Up 1.32 20.3 21.8 21.4 20.9 1.823 0.121
2.2 125.2 Up 2.53 21.1 21.5 20.9 20.7 1.261 0.109
2.3 117.6 Down 1.87 21.8 22.5 20.5 22.2 1.794 0.111
2.4 124.0 Down 2.60 22.5 22.9 22.9 21.1 1.441 0.115
b
Large Cylindrical Carrot Slabs (Thickness = 11.5 mm)
d
3.1 126.0 Up 1.83 64.0 108.5 63.4 62.6 1.121 0.113
3.2 126.6 Up 2.40 60.2 71.2 74.3 68.9 1.163 0.112
3.3 124.2 Up 2.53 — 56.7 — 52.2 1.134 0.101
3.4 125.0 Up 2.55 68.7 74.3 56.7 70.9 1.212 0.104
3.5 125.4 Down 2.47 58.9 56.2 56.4 58.4 1.115 0.099
c
Cylindrical Potato Slabs (Thickness = 9.8 mm)
4.1 118.4 Up 1.83 43.6 50.9 40.9 43.1 1.218 0.097
4.2 125.5 Up 2.47 45.5 43.8 39.4 46.1 1.161 0.118
4.3 124.2 Up 2.53 — 42.9 — 43.8 1.118 0.114
4.4 125.7 Down 1.33 47.6 44.0 46.7 39.9 1.213 0.109
4.5 124.2 Down 2.50 43.1 43.9 41.1 43.5 1.141 0.102
Note: SMFR, steam mass flow rate.

a
f values at particle center are at bed locations: bottom, center, and top.
b
The diameter to thickness ratio of the cylindrical carrot slabs was between 3:1 and 3.5:1.
c
The diameter to thickness ratio of the cylindrical potato slabs was between 3.5:1 and 4:1.
d
Datum out of range.
21.4.2.3 Errors Associated with fh and jh Values
In analyzing the sources of error associated with f and j values, it was observed that
a ±1°C change in Ts (steam temperature) altered fhc by less than 5%. However, this
was not so for jhc, fhs, and jhs values. The influence of small changes in Ts on f and
j values is shown in Figure 21.6, using the surface temperature data with Ts − 1 defined
as error 1 and Ts + 1 as error 2. This was done because the temperature ratio (θs)

1
0
Food center

-1
-2
-3 ERROR 2
-4
CORRECTED
-5
Food surface
-6 ERROR 1
-7
0 20 40 60 80 100
Heating Time (sec)
FIGURE 21.6 Influence of error 1 (Ts – 1) and error 2 (Ts + 1) on the experimental fhs value.
at the surface layer is very sensitive to changes in Ts. Results show that fhs increased
with increases in Ts. Furthermore, the value of jhc could be related to that of fhc.
During the course of this study, a small increase in steam temperature over time was
observed (Figure 21.4). Thus, the use of a slightly lower Ts value would result in a
steeper slope. Although such a change had negligible influence on the fhc value, the
impact on j value was large since the data were plotted on a logarithmic scale. An
in-depth analysis of fhc variations due to factors such as environment and computation
procedure was not carried out.
21.4.2.4 Particle-to-Particle Interaction
Deviations from general fhc values, presented in Tables 21.2 and 21.3, are due to
particle-to-particle interaction. It was indicated earlier that some adhesion of potato
cubes was observed due to gelatinization of starch. Particle adhesion resulted in a
larger particle mass, and hence the f value increased. However, small variations in
the value of fh can be attributed to: (1) edge contacts and (2) experimental errors
associated with variability in particle size. Furthermore, a closer inspection of
Table 21.2 shows that slightly higher f values were obtained at the center of the food
bed. This effect was not as pronounced for carrot cubes (Table 21.3) as for potato
cubes. The slightly higher f value for potato cubes, at the center location of the bed,
is possibly a result of condensate build-up, which may have slightly depressed the
heating rate.
21.4.2.5 Steam Flow Direction
It is difficult to define which flow direction is superior from temperature and f value
data. However, data recorded on food bed heights showed that 180 g of large potato
cubes provided an average bed height of 73 mm before processing. This reduced to
64 and 68 mm after treatment due to bed settling, for downward and upward steam

flow, respectively. Since these data are specific to the simulator used in this study,
no general conclusions could be drawn.
21.4.2.6 SMFR and Steam Temperature
Steam velocity (SMFR) and processing temperature did not have any influence on
particle heating rate within the range tested. The data for large potato cubes show
that similar f values were obtained with steam processing temperatures of 118 and
131°C. An increase in temperature of 9°C (from 118 to 127°C) also produced
similar results for carrot cubes. Data also show that a sixfold increase in SMFR
did not influence the particle heating rate. It can thus be concluded that the steam
process temperature and SMFR have negligible influence on the product heating
rate.
21.4.3 HEAT TRANSFER COEFFICIENT (h) AND THE BIOT NUMBER (Bi)
It was indicated earlier that a finite surface resistance to heat transfer occurs during
packed bed HTST processing of diced vegetables in steam. In cases where 0.1 <
Bi < 100, the internal dissipation of heat, although slow, maintains its capacity to
keep the surface temperature lower than that of the heating medium, as observed.
The system h value and the Biot number can be estimated with Equations (21.3)
and (21.5), and by using thermal property data (thermal diffusivity, α, and thermal
conductivity, k). From results reported by Kostaropoulos et al. (1975) and Pannu
−7 2
et al. (1990), the following data are available: αpotato = 1.6 * 10 m /sec, kpotato =
−7 2
0.62 W/m°C, αcarrot = 1.7 * 10 m /sec and kcarrot = 0.66 W/m°C. From the data
presented in Tables 21.2 and 21.3, we obtain: fpotato = 33.1 sec, fcarrot = 29.3 sec,
Rpotato = 1.17/200 m and Rcarrot = 1.15/200 m. For large cubes, the following results
were obtained by using Equations (21.2) and (21.5): β1 potato = 1.47, Bipotato = 14.2,
2 2
hpotato = 1500 W/m °C, β1 carrot = 1.49, Bicarrot = 17.8 and hcarrot = 2000 W/m °C.
Similar h values were obtained by using f value data for the smaller (9.9 mm)
2
food cubes. These results are higher than the value of 1100 W/m °C reported by
2
Ling et al. (1974) but in the range of 1900–2500 W/m °C reported by Pannu et al.
(1990). The latter study was conducted using single particles. However, the above
results for the system heat transfer coefficients are lower than the minimum value
2
of 5000 W/m °C for condensing water vapor, as reported by Holman (1976), for
processing of food containers and pouches with steam. Thus, there is need for
additional work in this area.
21.4.4 PRODUCT QUALITY

Product handling and particle identity were observed by placing processed products
on a plate. Potato cubes processed at ≤125°C retained their shape and identity.
However, potato cubes processed at 130°C were fragile and overcooked, and there
was evidence of particle breakup. In a few instances, it was noticed that potato cubes
adhered to each other as well as to the processing container wall. On the other hand,
carrot cubes showed no clumping, and the particles maintained their shape and

TABLE 21.4
Moisture Content of Raw and Processed Food Particulates
and Visual Observations
Initial Final Moisture

Batch Mass Mass Content
No. Treatment (g) (g) (%) Visual Observation
Potato Cubes
1.1 Uncooked 8.28 1.65 80.07
1.2 Uncooked 8.54 1.71 79.98
1.3 Cooked 8.34 1.58 81.06 Good shape
1.4 Cooked 8.14 1.52 81.33 Good, some adhesion
1.5 Cooked 8.44 1.61 80.92 Some adhesion to the
container
1.6 Cooked 8.12 1.52 81.28 Good shape
Carrot Cubes
2.1 Uncooked 7.72 0.78 89.90
2.2 Uncooked 8.47 0.89 89.49
2.3 Cooked 7.25 0.91 87.45 Good, no adhesion
integrity. Processed carrots were more intense in color than the raw product and did
not adhere to the container wall.
21.4.5 MOISTURE LOSS

Table 21.4 shows that there was no significant gain or loss in food moisture content
during the processing of potato and carrot cubes in steam. The small increase in
moisture of processed potato samples is attributable to higher moisture retention of
gelatinized starch. On the other hand, moisture loss by processed carrots probably
takes place due to collapse of cellular structure.
21.4.6 PROCESS IMPLICATIONS ON PRODUCT BLANCHING/STERILIZATION

To achieve commercial sterility, it is necessary for the center of the food particle to
undergo heat treatment to achieve a lethality of 3 min or more (Heldman and Hartel,
1997). The thermal resistance kinetic parameters for Clostridium botulinum are D121
of 0.26 minutes and a z value of 10°C (Perkins et al., 1975). For a 12D process, the
particle needs to be held at 121°C for 3 min. Problems such as these need to be
resolved through a biological validation study. Furthermore, the definition of the
cold point “in the can” may also need to be redefined for packed bed processing.

In this work, it was shown that there was no cold spot in the food container
(processing “can”) after 5 to 10 sec of heating during steam injection heating of
diced particles. The cold spot effectively is the particle center point, dispersed
throughout the “can.”
It is generally recognized that HTST processing will provide a product of
superior quality in the case of blanching (Heldman and Hartel, 1997). Thus, the role
of steam injection heating in providing optimally processed vegetables for ready-
to-eat meal packages also needs to be evaluated. As blanching/pasteurization require-
ments are less severe, packed bed heating of particles in batches by steam injection
can provide adequate processing. Listeria monocytogenes, which has been of great
concern in recent times, has D70 = 0.14 to 0.27 min and a z value between 6 and 7.5°C
(Gaze et al., 1989). As other microorganisms of interest present similar trends, using
this microorganism as reference and the temperature data presented in Table 21.4,
it can be shown that pasteurization requirements for large potato cubes (11.7 mm)
are satisfied after approximately 80 sec of steam heating at 125°C. Thus, the data
presented in this study can be used to determine thermal process adequacy for various
microorganisms of interest.
21.5 CONCLUSIONS
The concept of processing food particles in preweighed lots seems promising, and
its potential in aseptic processing warrants further investigation. The results of this
study show that batch heating of carrot and potato cubes in packed beds with steam
provides a processed product that retains shape, identity, and color. Furthermore,
steam heating prevents physical losses due to leaching, and under proper conditions
the product heats uniformly with negligible gain or loss of moisture. Sensitivity of
the temperature data can be appreciated from the fact that carrot and potato cubes
produced noticeably different fh values, indicating different heating rates. SMFR
(velocity) and steam temperature have only minimal influence on product heating
rate. This study also confirms that finite resistance to surface heat transfer occurs
during packed bed heating of food particles by steam injection. By using literature
values for food thermal properties, the apparent surface heat transfer coefficient
2
value was found to range from 1500 to 2000 W/m °C with Bi on the order of 14–17
for 1.2-cm food cubes. There is need for additional work on h values associated
with steam processing, as well as a sensitivity analysis of the influence of process
temperature on fh. Process validation, product cook quality, process optimization,
and means to aseptically cool the product are areas that need further attention.
NOMENCLATURE
2 −1
α Thermal diffusivity (m sec )
β Characteristic root, Equation (21.1)
q Unaccomplished temperature ratio, Equation (21.1)
Bi Biot number (= hR/k)
2
Fo Fourier number (= αt/R )

fh Heating rate index; negative inverse slope in Equations (21.2), (21.4) and
(21.5) (sec)
2
H Convective heat transfer coefficient (W/m °C)
Jh Thermal lag factor/intercept, Equation (21.2)
K Thermal conductivity (W/m°C)
R Characteristic length (m); 1 2 thickness of cube or slice
T Time (sec)
Ts Steam temperature (°C)
Ti Initial (food) temperature (°C)
T(x,t) Variable internal (particulate) temperature (°C)
REFERENCES
Gaze, J.E., Brown, G.D., Gaskell, D.E., and Banks, J.G., Heat resistance of Listeria mono-
cytogenes in homogenates of chicken, beef steak, and carrot, Food Microbiol., 6, 251,
1989.
Hayakawa, K.I., Empirical formula for estimating nonlinear survivor curves of thermal vul-
nerable factors, Can. Inst. Food Sci. Technol., 32, 59, 1982.
Heisler, M.P., Temperature charts for induction and constant temperature heating, Trans.
ASME, 69, 227, 1947.
Heldman, D.R. and Hartel, R.W., Principles of Food Processing, Thomson Publishers, New
York, 1997.
Holman, J.P., Heat Transfer, 4th ed., McGraw-Hill, New York, 1976.
Kostaropoulous, A.E., Spiess, W.E.L., and Wolf, W., Reference values for thermal diffusivity
of foodstuffs, Lebensm.-Wiss. Technol., 8, 108, 1975.
Larkin, J.W., Use of modified Ball’s formula method to evaluate aseptic processing of foods
containing particulates, Food Technol., 43, 124, 1989.
Ling, C.C.A., Bomben, J.L., Farakas, D.F., and King, C.J., Heat transfer from condensing
steam to vegetable pieces, J. Food Sci., 39, 692, 1974.
Luikov, A.V., Analytical Heat Diffusion Theory, Academic Press, New York, 1968.
Pannu, K.S., High Temperature Transient Heating of Vegetables by Steam Injection, thesis,
Laval University, Ste-Foy, Quebec, 1992.
Pannu, K.S., Castaigne, F., Ramaswamy, H., Arul, J., Audet, P., and Desilets, D., Rapid
Sterilization of Particulate Food by Steam Injection: Evaluation of Thermal Parameters,
ASAE paper #90–6527, presented at the 1990 ASAE winter meeting, Chicago, 1990.
Perkins, W.E., Ashton, D.S., and Evancho, G.M., Influence of the z value of Clostridium
botulinum on the accuracy of process calculation, J. Food Sci., 40, 1189, 1975.
Rumsey, T., Farakas, D.F., and Hudson, J.S., Measuring steam heat transfer coefficient of
vegetables, Trans. ASAE, 24, 1048, 1980.
Singh, R.P., Thermal diffusivity in food processing, Food Technol., 36, 87, 1982.
Skjöldebrand, C. and Ohlsson, T., A computer simulation program for evaluation of the
continuous heat treatment of particulate food products. Part 2: Utilization, J. Food
Eng., 20, 167–181, 1993.
Tung, M.A., Britt, I.J., and Ramaswamy, H.S., Food sterilization in steam/air retorts, Food
Technol., 44, 105, 1990.
Zhang, Q. and Cavalieri, R.P., Thermal model for steam blanching of green beans and
determination of surface heat transfer coefficient, Trans. ASAE, 34, 182, 1991.

Thermal Processing
22 of Particulate Foods
by Steam Injection.
Part 2. Convective
Surface Heat Transfer
Coefficient for Steam
CONTENTS
22.1 Introduction
22.2.1 Computational
22.2.2 Equipment and Experimental
22.3.1 Temperature Profiles
22.3.2 Impact of Flow Direction
22.3.3 Transducer Location in the Food Bed
22.3.4 Influence of Steam Mass Flow Rate (SMFR)
22.3.5 Steam Temperature Effects
22.3.6 Influence of Particle Size
22.3.7 Inert Material vs. Food
22.3.8 h Values of Food vs. Metal
22.4 Conclusions
References
22.1 INTRODUCTION
Batch heating of solid foods by steam injection was investigated to determine
feasibility and process requirements. This method has potential for high temperature
short time (HTST) processing conditions, which are favorable for minimizing nutrient

loss and improving quality of the processed product. Furthermore, product steriliza-
tion by steam processing is desirable from the standpoint of minimization of effluent
(wastewater) discharge (Poulsen, 1986). The basic premise of this process is that a
preweighed quantity of food particulates would be held in specially designed con-
tainers and batch heated by flowing steam, which allows HTST processing, with the
product flowing continuously. Construction of a laboratory processor and determi-
nation of the heating rate of food particulates in a packed bed with steam are
described elsewhere (Pannu et al., Chap. 21, this volume). This chapter describes
the determination of the surface convective heat transfer coefficient (h value)
obtained during packed bed heating with steam.
Heat process development involves not only the determination of processing
conditions, but also the prediction of product heating time. Basic information require-
ments are thermal and physical property data for food, thermal property data for
steam, steam flow conditions, and the mode of heat transfer. Batch heating of diced
carrots and potato cubes showed that the resistance to heat transfer at the food surface
was not negligible and that the Biot number was less than 40 when food pieces were
heated with steam (Pannu et al., Chap. 21, this volume). These results are in agree-
ment with those reported by Rumsey et al. (1980) and Pannu et al. (1990). In addition,
2
surface heat transfer coefficient values of approximately 2000 W/m °C were obtained
with food cubes (Pannu et al., Chap. 21, this volume). These are inferior to the
2
minimum h value of 5000 W/m °C associated with condensing steam (Holman,
1976). This disparity of results requires explanation.
To obtain reliable estimates for product heating time, it is imperative to correctly
define h and the associated Biot (Bi) number. An assumption that Bi > 40 is valid for
the processing of metal cans and pouches in condensing steam because these objects
have a characteristically large size. However, heating time estimates of 113 and 103 sec
were obtained for steam processing of 12-mm potato and carrot cubes, respectively,
where steam temperature was 125°C and the product initial and final temperatures
were 25 and 121°C, respectively. Calculations used the first term approximation for
the transient heat conduction in the equation of Luikov (1968), assuming infinite Biot
−7
number (Bi > 40). The normally accepted thermal diffusivity values of 1.6 × 10 and
−7 2
1.7 × 10 m /sec (Kostaropoulos et al., 1975) were used for potato and carrot, respec-
tively. However, with Bi ≈ 15, the heating time increased to 130 and 115 sec for the
potato and carrot cubes, respectively. The latter values for product heating time are in
agreement with our experimental data (Pannu et al., Chap. 21, this volume) and provide
2
h value estimates for steam on the order of 1500 to 2000 W/m °C.
The most common explanation for decrease in h value is the presence of air in
the steam. Tung et al. (1990) reported that even a small amount of air present in
steam could dramatically decrease the h value. Othmer (1929) reported h values of
2
steam with an air content of 0, 1, and 2% to be 15,900, 7900 and 5200 W/m °C,
respectively. On the other hand, Pflug (1964) found that the h value decreased to
2 2
1300 W/m °C (from about 5000 W/m °C) with 10% air in the steam. Tung et al.
(1984) obtained h values higher than those of Pflug (1964), but their data support
the hypothesis that h values decrease with increasing air content. In addition, they
showed that h values were higher during downward steam flow but were not dependent
on steam temperature. These differences in results obtained by various researchers

can, at least in part, be attributed to the variations in “come-up time” and/or the
“flush time” in different retorts.
A second explanation for h value depression, specific to the food processing
situation, is the phenomenon described as “gassing out,” where gases present in fruit
and vegetable tissue are released during heating. Brown (1974), Ling et al. (1974),
and Zhang and Cavalieri (1991) reported that h values decreased to 400–1100
2
W/m °C during the processing of vegetables in condensing steam because of the
“gassing out” effect, leading to the formation of a layer of noncondensable gases at
the boundary layer of the food particle.
Despite its importance, the h value for steam relating to food processing has not
2
been specified by application but is generally said to range from 400 to 16,000 W/m °C
(Tung et al., 1984). Holman (1976) indicated that the h value for condensing steam
2 2
could range from 5000 to 100,000 W/m °C. The estimate of 5000 W/m °C reported by
Pflug (1964) has gained acceptance in the food industry and is also the value suggested
by Skjöldebrand and Ohlsson (1993) as the condensing steam to wall h value. This
2 2
value of 5000 W/m °C is superior to the values of 850 –1700 W/m °C reported by
2
Rumsey et al. (1980) and 1800 –2500 W/m °C reported by Pannu et al. (1990). Thus,
it is imperative to understand the factors contributing to the reduction in h value.
Packed bed heating with steam injection was investigated primarily to evaluate
the h value for steam under a variety of heating conditions and, secondly, to gain
an understanding of how steam flow and condensation effect could affect packed
bed heating. The convective surface heat transfer coefficient was determined with
temperature measurements obtained from metal cubes placed in the bed of food
pieces and inert material. The h values were reported for steam heating of packed
beds as affected by process variables such as steam flow direction, flow rate, and
temperature, as well as bed characteristics such as particle size and bed composition
(food vs. inert material).

22.2.1 COMPUTATIONAL
The internal resistance to heat transfer is small in metal cubes, and hence the lumped
heat capacity method is appropriate for estimation of h values, provided the Biot
number is small (Bi ≈ 0.1 or lower). Equation (22.1) was used to compute h values
from temperatures registered at the geometric center of metal cubes.
Ts − T( t ) −(hA/ρCpV)t
= θsolid = e (22.1)
Ts − Ti
The terms A, ρ, Cp, V, and L represent the solid surface area, density, specific
heat, volume, and characteristic length, respectively. Subscripts for temperature (T),
listed as s, i, and t, denote steam, initial (metal cube), and time t (metal cube),
respectively. The density and specific heat data are from Holman (1976). ρ and Cp
3 3
for steel are 7830 kg/m and 465 J/kg°C, and those for aluminum are 2707 kg/m and
896 J/kg°C, respectively.

22.2.2 EQUIPMENT AND EXPERIMENTAL
Details on apparatus construction and operation have been described elsewhere
(Pannu et al., Chap. 21, this volume). The test apparatus had steam superheating
capability to provide dry saturated steam to the central treatment chamber. Experi-
ments were conducted with good quality saturated steam, as the outer annular jacket
(steam superheater) was always maintained at a slightly higher temperature than the
interior treatment chamber, such that heat losses in the central treatment zone were
negligible (Pannu, 1992). Two three-way valves and flexible hoses were used for
the process setup and to control the steam flow direction through the particle bed.
The test apparatus also had provision for regulating the steam velocity through the
chamber. Steam was condensed to liquid water, and the condensate collected at
intervals was used to determine steam mass flow rate (SMFR).
A test container with a diameter of 7.5 cm and a height of 10.3 cm was filled
with glass beads of diameter 6 or 14 mm or with rehydrated chickpeas (diameter ≈
11 mm), to a bed height of 9 cm. For all experiments, three metal cubes (transducers)
were positioned in the particle bed at the top, center, and bottom locations to obtain
the desired time–temperature data. The top and bottom transducers were positioned
approximately 1 cm below and above the bed extremities, respectively. Thermocou-
ples and pressure gauges were also positioned at strategic locations to allow obser-
vation and control of steam pressure and the temperature of the process (Pannu et al.,
Chap. 21, this volume).
The metal transducers were fabricated by positioning a fine-wire copper con-
stantan (36 gauge, type-T) thermocouple at the geometric center of each metal cube.
To accomplish this task, a 0.7-mm hole was drilled into each metal cube at the
central axis up to a depth equivalent to half the cube dimension. An epoxy cement
with high heat resistance and high thermal conductivity was used to bond the
thermocouples in place (Omegabond 200, Omega Engineering Inc., Stamford, CT).
The cube-shaped metal (aluminum and steel) transducers were constructed in three
sizes (9.5, 11.1 and 12.7 mm). Most of the experiments were conducted using the
11.1-mm aluminum cubes. The metal transducers and other thermocouples recorded
temperatures at 1 reading/sec for 30 sec, followed by 5 readings/sec (fast test
cycle) for the next 60 sec. Thereafter, the data logger recorded the temperatures
at 1 reading/2 sec until shutdown. Steam was injected into the central processing
chamber once the data logger commenced recording data at the fast test cycle.

Abbreviated time–temperature data acquired for a typical run are given in Table 22.1.
This experiment was carried out with steam at a temperature of approximately 140°C
at a flow rate of 3.37 g/sec, flowing downwards through a bed of rehydrated chickpeas.
Steam temperatures were monitored at three locations (columns 4 to 6). The refer-
ence thermocouple (Ref, column 4) was located 2 cm below the test container and
measured the temperature of steam inside the processing chamber. Locations Top
(column 5) and Bottom (column 6) measured steam temperatures at the entry and
exit positions, respectively, of the apparatus. Temperature data from these three

TABLE 22.1
a
Abbreviated Time–Temperature Data for a Typical Run
1 2 3 4 5 6 7 8 9
Time (sec) Steam Temperature (°C) Transducer Temperature (°C)
Actual Corrected Ref Top Bot Bot Cen Top
1 0.0 –32.0 22.5 51.0 45.9 23.1 22.8 22.8

2 10.0 –22.0 22.7 50.7 45.9 23.4 23.1 22.8
3 20.0 –12.0 23.1 50.1 45.6 23.4 22.8 22.5
4 30.0 –2.0 23.1 50.1 45.6 23.6 23.1 23.1
5 31.0 –1.0 23.1 50.4 45.3 23.4 23.1 22.5
6 31.2 –0.8 23.4 49.9 45.3 23.4 22.8 22.5
7 31.4 –0.6 23.1 49.9 45.3 23.4 23.1 22.8
8 31.6 –0.4 23.4 100.6 45.9 23.6 23.4 23.4
9 31.8 –0.2 23.4 107.4 45.6 23.6 25.7 29.6
11 32.0 0.0 23.4 114.1 46.1 27.2 33.1 47.6
13 32.2 0.2 89.8 120.2 46.7 38.4 48.1 65.3
14 32.4 0.4 122.5 124.3 48.7 52.7 64.5 80.4
15 32.6 0.6 126.3 129.3 57.2 64.7 79.8 92.1
16 32.8 0.8 131.1 132.8 84.4 79.0 91.6 102.2
17 33.0 1.0 135.1 136.3 111.0 87.9 101.4 110.0
18 33.2 1.2 136.6 138.0 124.5 96.4 109.7 116.1
19 33.4 1.4 138.0 138.8 130.8 103.2 116.6 121.5
20 33.6 1.6 138.5 140.0 134.8 107.9 122.2 125.0
21 33.8 1.8 138.8 140.3 137.5 112.5 126.3 128.1
22 34.0 2.0 139.3 140.8 138.0 116.6 129.6 130.6
23 34.2 2.2 139.3 140.8 138.8 119.5 131.8 132.1
24 34.4 2.4 139.3 140.8 138.8 121.7 133.8 133.8
25 34.6 2.6 139.8 141.5 137.8 123.8 135.3 134.6
26 34.8 2.8 138.3 140.5 138.0 125.3 136.6 135.3
27 35.0 3.0 138.3 140.0 136.3 127.4 137.0 136.1
29 37.0 5.0 139.3 140.8 139.8 137.8 139.5 139.0
31 39.0 7.0 139.3 141.3 140.3 138.3 139.5 139.3
34 42.0 10.0 139.5 141.3 140.3 139.0 140.0 139.8
Note: Ref, Bot, Cen: Reference, Bottom, and Center, respectively.

a
Downward flow of steam (140°C), at the rate of 3.4 g/sec, through a bed of rehydrated chickpeas.
locations facilitated the adjustment of real time (column 3) and calculation of the
steam temperature (Ts). The dimensionless temperature ratios (θ) were calculated
for each of the metal transducers, and their natural logarithms [ln(θ)] were plotted
against heating time. The h value was computed for each metal cube by determining
the slope (X coefficient, Table 22.2) of the linear region of the semilogarithmic plot,
using standard regression analysis.

TABLE 22.2
Basic Information and Standard Regression Analysis to
Determine h Value
Material: Chickpeas
Mass: 240 g
Steam Mass Flow Rate: 3.37 g/m
Processing Temperature: 140.1°C
Transducer:
Location Bottom Center Top
Material: Steel Aluminum Aluminum
Size: 1 (cm) 1.111 1.111 1.270
3
Density: ρ (kg/m ) 7830 2707 2707
Specific heat: Cp (J/kg°C) 465 896 896
Regression Analysis:
Number of data points 21 21 21
Degrees of freedom 19 19 19
X coefficient –0.662 –1.214 –1.120
Standard error of coefficient 0.0066 0.0127 0.0070
2
R 99.9 99.8 99.9
2
Estimated h values (W/m °C) 4465 5455 5748
Estimated Biot Number (–) 0.459 0.148 0.176

22.3.1 TEMPERATURE PROFILES
Typical temperature profiles obtained from metal transducers under upward and
downward steam flow conditions are shown in Figures 22.1a and 22.1b. They indicate
that an instant rise in temperature was evident when steam was injected into the
processing chamber, and that all metal transducers had a uniform and constant initial
temperature just prior to heat treatment. Furthermore, the lower transducer was first
to register temperature rise when the flow of steam was upward, and the inverse was
true during downward flow. The semilogarithmic plots indicated that linearization
was possible after a very short lag period.
Biot number values of 0.459 and 0.15 for the 11-mm steel and aluminum test
transducers were obtained with the data presented in Table 22.2. The Biot criterion
(of Bi ≤ 0.1) was not satisfied by the steel transducer. For this reason, most of the
investigation was conducted with aluminum transducers.
22.3.2 IMPACT OF FLOW DIRECTION

The h values obtained with steam flowing through a bed of rehydrated chickpeas
are presented in Figures 22.2 to 22.4. Comparative data for food and glass beads
are presented in Figure 22.5. Figure 22.2 shows the transducer locations and h values

Small glass beads Large glass beads
120 130
110 120
100 110
Temperature (°C)
Temperature (°C)
90 100
80 90
70 Upward Flow 80 Downward Flow
60 SMFR = 5.5 g/s 70 SMFR = 2.1 g/s
50 Top 60 Top
40 Center 50 Center
Bottom Bottom
30 Steam 40 Steam
20 30
-1 0 1 2 3 4 5 6 7 -1 0 1 2 3 4 5
Heating Time (sec) Heating Time (sec)
(a) (b)
FIGURE 22.1 Temperatures registered by the metal cubes in beds of 6 mm (a) and 14 mm
(b) glass beads.
6000 DOWNWARD
SMFR
5.67 g/s 1.58 g/s 0 cm 9 cm
h-value (W/m2°C)
5500 DOWNWARD 7.67 g/s 1.50 g/s 1 cm 8 cm
5000
4.5 cm 4.5 cm
4500 UPWARD
8 cm 1 cm
9 cm 0 cm
4000
0 2 4 6 8 10
Distance (cm): Bed height = 9 cm UPWARD
FIGURE 22.2 The influence of steam flow rate (SMRF), flow direction, bed height, and
location on h values. Experiments were conducted at 120°C with rehydrated chickpeas.
obtained with steam temperatures of ≈120°C in a bed of rehydrated chickpeas under

different steam flow rates, with upward and downward flow of steam. In general,
all these plots show that h values were higher during downward flow of steam, and
the results are in agreement with the general trend reported by Tung et al. (1984).
However, the influence of flow direction vanished when live steam at 100°C
(atmospheric pressure) was injected (Figure 22.3), and h values were found to be
2
between 4300 and 4500 W/m °C. The h values remained nearly the same for down-
2
ward flow but decreased to about 4000 W/m °C for upward flow with pressurized
steam at 110°C. Although this may appear to be an anomaly, it can be understood
when the contribution of phase change or condensation of steam to heat transfer is
taken into consideration. With live steam, a quasi-total condensation is expected,
whereas it is partial with pressurized steam. At 100°C, the h value is not significantly
affected by steam flow direction, presumably because the level of condensation in
both directions is nearly the same. With an increase in steam temperature, the h value
increases but with a constant disparity between flow directions. This difference has

6000
5500 OPEN
HEATING DOWNWARD
h-value (W/m2°C) AT 100°C
5000
UPWARD
4500
4000
3500
3000
100 110 120 130 140 150
Temperature (°C)
FIGURE 22.3 The influence of steam flow direction and temperature on h values. Steam
flowed at a rate of ∼3.4 g/sec through a bed of rehydrated chickpeas.
6000
DOWNWARD Steam Flow Direction
Top UPWARD
5500 Center DOWNWARD
h-value (W/m2°C)
Bottom
5000
4500
4000
1 2 3 4 5 6
Steam Mass Flow Rate (g/sec)
FIGURE 22.4 The influence of steam flow rate, direction, and location on h at temperature
of ∼115°C in a bed of rehydrated chickpeas.
to do with the degree of condensation and/or thickness of the condensate film, which
can play a role in the resistance to heat transfer. The results indicate that with
downward flow, a higher level of condensation occurs and/or condensate is flushed
out more effectively.
The results also indicate that there is a lesser degree of condensation with pres-
surized steam compared with live steam, and that condensation behavior of pressur-
ized steam is affected by its flow direction. Condensation of steam occurs because
of temperature and pressure drops through the particulate bed. It is conceivable that

5500
Large glass beads
Chickpeas
Small glass beads
5000
h-value (W/m2°C)
4500
Steam Flow Direction

UPWARD
DOWNWARD
4000
0 2 4 6 8 10
Steam Mass Flow Rate (g/sec)
FIGURE 22.5 The influence of bed composition, particle size, steam flow rate, and flow
direction at a temperature of ∼120°C on h values in beds of 6 mm and 14 mm glass beads
and rehydrated chickpeas. The h values were pooled from all three locations.
the drop in steam temperature due to sensible heat exchange may not be significantly
different between the flow directions. But the drop in steam pressure can be different
because downward flow tends to compact the packed bed, while upward flow tends
to expand it. Consequently, higher pressure drop and reduced void bed volume would
take place during downward flow, while the reverse would be true for upward flow.
Reduced void space would facilitate retention of a smaller quantity of condensate.
Thus, enhanced condensation (latent heat transfer) and reduced condensate film (heat
transfer resistance) should lead to a higher h value during downward flow than
upward flow under similar heating conditions.
Because condensation plays a role, the boundary layer formed by the condensate
(liquid water) should be a consideration in heat transfer. Luikov (1968) showed that
h is related to the boundary layer thickness (δ) and k, the thermal conductivity of
the condensate layer, by equations (2a) and (2b):
(Ts − Tps )
h(Ts – Tps) = kf (22.2a)
δ
kf
or δ = (22.2b)
h
where Ts and Tps are the steam and particle surface temperatures, respectively. An
estimate of δ from Equation (22.2b) yields values of 0.3 mm for food materials and
0.12 mm for metal cubes. Larger boundary layer thicknesses increase the resistance
to heat transfer and reduce h value.

22.3.3 TRANSDUCER LOCATION IN THE FOOD BED
The h values were location sensitive, and more so with steam flowing downward
than upward (Figures 22.2 and 22.4). In downward flow, the h values at the uppermost
location were highest, and they decreased with bed height; i.e., h values were highest
at the point of steam entry into the bed and lowest at the exit end. This was also
evident in time–temperature plots for glass beads because the metal transducer at
the top location had a steeper slope. In upward steam flow, slightly higher h values
were obtained at the top location (Figure 22.2); this is contrary to downward flow,
as h values were higher at the exit. Overall, h values were more uniform in upward
flow but slightly lower at the bed center.
22.3.4 INFLUENCE OF STEAM MASS FLOW RATE (SMFR)

The effect of steam mass flow rate on the value of h is depicted in Figures 22.4 and
22.5. Figure 22.4 shows the changes in h value registered by metal cubes placed in
rehydrated chickpeas at steam temperature of 115°C for both flow directions. Figure 22.5
shows the changes in h value for glass beads of diameter 6 and 14 mm and rehydrated
chickpeas at 120°C, with steam flow in both upward and downward directions. In the
range of SMFR, 1.2 to 5.8 g/sec and Ts ≈ 115°C, (Figure 22.4), h values registered in
a bed of chickpeas showed small increases with increase in SMFR at all locations with
downward flow. The h values increased at the top, center, and bottom of the food bed
2 2
by about 8% (5000 to 5400 W/m °C), 5% (4650 to 4900 W/m °C), and 14% (4300 to
2
4900 W/m °C), respectively, during downward flow (Figure 22.4). However, the change
in h value was negligible when the direction of the steam flow was upward.
The pooled data (average for all three locations) presented in Figure 22.5 show
that at 120°C the metal transducers experienced small increases in h values, in beds
of large glass beads as well as for chickpeas, for both upward and downward flow
of steam. However, the increase in h value was negligible for small glass beads for
both directions of steam flow (Figure 22.6). Overall, the effect of SMFR on h value
was small; the flow direction of steam, as well as particle location, had stronger
influences. Nonetheless, the influence of SMFR was noticeable for packed beds with
larger void spaces, such as large glass beads or chickpeas. The effect waned when
the void volumes became small, as in the case of small glass beads.
22.3.5 STEAM TEMPERATURE EFFECTS

The effect of steam temperature on h values for rehydrated chickpeas at SMFR of
3.4 g/sec in both the upward and downward flow of steam is shown in Figure 22.3,
pooling data for the three locations. To compare the influence of temperature effects
(Figure 22.6) in the three different beds, glass beads of two different sizes and
chickpeas, h value data for similar temperatures but different SMFR were pooled
for both flow directions and location to provide average values. Whatever the direc-
tion or particle size of the bed, h increased with temperature at nearly the same rate.
A high h value recorded at 100°C can be attributed to a very high level of conden-
sation of live steam. As steam temperature or pressure was increased, h value remained
the same or decreased up to 110°C, depending on steam flow direction; above this

6000
5500
h-value (W/m2°C)
5000
4500
4000
Large glass beads (φ = 14 mm)
OPEN Chickpeas (φ = 11 mm)
3500
HEATING Small glass beads (φ = 6 mm)
AT 100°C
3000
100 110 120 130 140
Temperature (°C)
FIGURE 22.6 The influence of temperature on h in beds of 6 mm and 14 mm glass beads

and ∼11 mm rehydrated chickpeas. Data for similar temperatures but different flow rates were
pooled for both flow directions and location to obtain mean values.
temperature, h value increased steadily (Figure 22.3). This suggests that the condensa-
tion effect is reduced with pressurized steam. However, the temperature effect compen-
sates for the contribution of condensation to heat transfer and hence, the h value increases
above 110°C. In effect, quasi-total steam condensation is achieved with pressurized
steam at ~108°C in a downward flow and at ~125°C with upward flow (Figure 22.3).
The effects of steam flow direction, SMFR, and temperature on h value can also
be understood through the condensation effect. When dry steam first enters the
packed bed and makes contact with the cold particles, partial condensation occurs
and a film of water is deposited on the particle surface, and some of the free void
space is filled with the condensate. Since smaller size particles provide more resis-
tance to fluid flow and also have smaller open spaces, it is probable that slightly
more water is entrapped because of capillary edge effects, and this increases the
boundary layer and consequently reduces the h value. Because condensate is tightly
held between the small beads, SMFR and flow direction do not appear to influence
the h value (Figure 22.5). However, as particle diameter increases, void spaces are
larger, and as the bed opens up, resulting in better condensate flushing and fluid
flow, the effects of SMFR and flow direction come into play (Figures 22.4 and 22.5).
Furthermore, heat transfer involves not only sensible heat, but also latent heat
effects due to condensation. Hence, the differences in h value ultimately depend on
the degree of condensation, fluid flow through the bed, and locations depending on
the direction of steam flow. In addition, the dry steam provided for heating can, and
most likely does, exit as wet steam. The amount of free water that can be readily
carried away by the exiting wet steam is probably related to bed restrictions, SMFR,
and temperature. Thus, as temperature increases, effects related to the degree of
wetness of exiting steam become important, and the h value increases as the con-
densate boundary layer shrinks.

22.3.6 INFLUENCE OF PARTICLE SIZE
The influence of particle size on h value is shown in Figures 22.5 and 22.6. Figure 22.5
shows the effect of particle size on h value at various SMFR, while Figure 22.6
provides data on h values at various temperatures. It is clear from these data that h
values are dependent on the particle size of the bed. The value of h is higher in
packed beds of larger particle size, attributable to larger void spaces within the bed.
22.3.7 INERT MATERIAL VS. FOOD

Figure 22.6 indicates that glass beads (inert) and chickpeas display similar trends in the
profile of h value with temperature of steam. Large glass beads (diameter 14 mm) show
higher h values at all steam temperatures, and small glass beads (diameter 6 mm) show
lower values than chickpeas (~diameter 11 mm), which are intermediate in size. Fur-
thermore, assuming chickpeas to be spheres, and ignoring the end effects, the porosity
of all three beds is similar. Hence, differences in h value data are attributable to the
void spaces between particles rather than to their composition or to the gassing-out
effect, which is a possibility since rehydrated chickpeas contain air dissolved in the
rehydrated tissue.
22.3.8 h VALUES OF FOOD VS. METAL

Pannu et al. (Chap. 21, this volume) determined h values for steam processing of
12-mm potato and carrot cubes. Potato and carrot cubes produced h values of about
2
1500 and 2000 W/m °C, respectively; in comparison, similar size metal cubes
2
produced h values ranging between 4300 and 5500 W/m °C (Figures 22.2 to 22.6).
2
The value of about 5000 W/m °C is in agreement with h values for condensing
steam reported by Pflug (1964) and Skjöldebrand and Ohlsson (1993). The results
of this study and previous results (Pannu et al., 1990) show that food particles do
not produce h values similar to those obtained with metal transducers.
The h values obtained with food pieces were about 40% lower than those
obtained with metal cubes under similar process conditions. The obvious differences
between these two materials are thermal diffusivity and boundary layer thickness of
condensed water. The thermal diffusivity of metals is far higher than that of food
−5 2 −7 2
materials (~8.4 × 10 m /sec for aluminum vs. ~1.6 and 1.7 × 10 m /sec for potato
and carrot, respectively). Furthermore, the water film thickness on metals should be
lower because water does not adhere well to metal surfaces, whereas the hydration
layer around food facilitates the formation of a thicker boundary layer.
22.4 CONCLUSIONS
The h values provided by metal cubes embedded in particle beds heated with steam
2
were closer to the value of 5000 W/m °C of h reported by Pflug (1964). These h values
2
are significantly higher than the value of 2000 W/m °C obtained for food cubes
2
(Pannu et al., Chap. 21, this volume), but lower than the value of 12,000 W/m °C
reported by Tung et al. (1984). The h values were not appreciably affected by SMFR
over the range tested. Higher h values were obtained by downward steam flow and

higher steam temperature and in beds of larger size particles. It appears that the
gassing-out phenomenon is not involved in the reduction of h values, nor in altering
the heat transfer characteristics of steam.
Excessive condensation of the heating fluid in the particle bed increases the
boundary layer thickness and enhances the resistance to heat transfer. The h values
obtained from metal cubes during steam heating were about 2.5-fold higher than
those obtained from food of similar size and shape. These differences are attributable
to thermal diffusivity and the boundary layer thickness of the condensate. Thus,
good quality dry steam is necessary for efficient and uniform heating of food beds
to avoid build-up of condensate.
REFERENCES
Brown, G.E., Importance of surface heat transfer during steam heat and heat/hold processes,
J. Food Sci., 39, 1066, 1974.
Kostaropoulous, A.E., Spiess, W.E.L., and Wolf, W., Reference values for thermal diffusivity
of foodstuffs, Lebensm.-Wiss. Technol., 8, 108, 1975.
Ling, C.C.A., Bomben, J.L., Farakas, D.F., and King, C.J., Heat transfer from condensing
steam to vegetable pieces, J. Food Sci., 39, 692, 1974.
Luikov, A.V., Analytical Heat Diffusion Theory, Academic Press, New York, 1968.
Othmer, D.F., The condensation of steam, Ind. Eng. Chem., 21, 576, 1929.
Pannu, K.S., High Temperature Transient Heating of Vegetables by Steam Injection. Ph.D.
thesis, Laval University, Ste-Foy, Quebec, 1992.
Pannu, K.S., Castaigne, F., and Arul, J., Chap. 21, this volume.
Pannu, K.S., Castaigne, F., Ramaswamy, H., Arul, J., Audet, P., and Desilets, D., Rapid Steril-
ization of Particulate Food by Steam Injection: Evaluation of Thermal Parameters,
ASAE paper # 90–6527, Presented at the 1990 ASAE winter meeting, Chicago, 1990.
Pflug, I.J., Evaluation of heating media for processing food in flexible packages. Phase I.
Final report, contract DA19-AMC-145(N), U.S. Army Natick Laboratories, Natick,
MA, 1964.
Poulsen, K.P., Optimization of vegetable blanching, Food Technol., 40, 122–129, 1986.
Rumsey, T., Farakas, D.F., and Hudson, J.S., Measuring steam heat transfer coefficient to
vegetables, Trans. ASAE, 24, 1048, 1980.
Skjöldebrand, C. and Ohlsson, T., A computer simulation program for evaluation of the
continuous heat treatment of particulate food products. Part 2: Utilization, J. Food
Eng., 20, 167–181, 1993.
Tung, M.A., Britt, I.J., and Ramaswamy, H.S., Food sterilization in steam/air retorts, Food
Technol., 44, 105, 1990.
Tung, M.A., Ramaswamy, H.S., Smith, T., and Stark, R., Surface heat transfer coefficients
for steam/air mixtures in two pilot scale retorts, J. Food Sci., 49, 939, 1984.
Zhang, Q. and Cavalieri, R.P., Thermal model for steam blanching of green beans and
determination of surface heat transfer coefficient, Trans. ASAE, 34, 182, 1991.

Modeling of Heat
23 Conduction in
Elliptical Cross
Sections (Oval Shapes)
Using Numerical Finite
Difference Models
F. Erdoǧdu, M.O. Balaban, and K.V. Chau
CONTENTS
23.1 Introduction
23.2.1 Power Curves Method
23.2.2 An Alternate Flexible Method
23.4 Conclusions and Suggestions
Nomenclature
References
23.1 INTRODUCTION
Heat transfer is an important part of several unit operations in food processing. Foods
commonly have irregular shapes, and heat transfer analysis is usually avoided because
of the difficult mathematical treatment and numerical solutions (Erdoǧdu et al., 1998b).
There has been a wealth of studies, programs and accumulated knowledge of heat
transfer in circular cylinders. This is not the case for elliptical cross sections. There
have been several studies regarding heat transfer in elliptical cross sections (Erdoǧdu,
1996).
McLahlan (1945) was the first to publish analytical equations governing the heat
transfer in an infinite elliptical cylinder with a uniform initial temperature and subjected
to an infinite convective heat transfer coefficient. The numerical solution for

McLahlan’s equation was provided by Kirkpatrick and Stokey (1959) for ellipses
having eccentricities of 0.6, 0.7, 0.8, and 0.9 against Fourier numbers of 0.1, 0.2, 0.5,
and 1.0 at certain locations of the geometry. Manson et al. (1974) predicted the transient
temperatures in conduction heating of pear-shaped objects using a finite difference
model. Simpson et al. (1989) evaluated thermal processes of foods in oval-shaped
containers using a finite difference approximation of the differential equation for
transient heat conduction in three dimensions. Eshleman (1976), Califano and Zaritzky
(1993), Sheen et al. (1993), Akterian and Fikiin (1994), and Kim and Teixeira (1997)
developed finite difference methods for simulating heat conduction in irregularly
shaped foods. Erdoǧdu et al. (1998b) developed a volume element based approach on
finite difference models for heat transfer in elliptical cross sections by using power
curves. They also reported that the use of power curves, assuming heat transfer is
along the curve, can be considered a favored method for heat transfer problems in
elliptical cross sections since it reduces the three-dimensional problem into two
dimensions in finite cylinders and the two-dimensional problem into one dimension
in infinite cylinders. It was also possible to accurately predict the center temperatures
in conductively heated elliptical cylinders by substituting them with a right circular
cylinder with equal ratio of surface area to volume when the eccentricity of the ellipse
was lower than 0.9.
However, neither of these methods was flexible enough to accept different
boundary conditions at the surface or inside the surface (e.g., different convective
heat transfer coefficient and surface temperatures at the different parts of the surface
or nonhomogeneous thermophysical properties inside the geometry). Thus, the
development of a flexible alternate finite difference solution to heat transfer problems
in elliptical cross sections to eliminate the previous methods’ deficiencies would be
valuable. Therefore, the objectives of this study were to review the power curves
method, to develop an alternate flexible volume element based approach to accept
different boundary conditions at the surface and nonhomogeneous thermophysical
properties inside, and to compare these methods.

23.2.1 POWER CURVES METHOD
As explained by Erdoǧdu (1996) and Erdoǧdu et al. (1998b), the following procedure
was used to generate the numerical network by the power curves method.
The equations representing the power curves and an ellipse with half-major axis
“a” and half-minor axis “b” (and also elliptical isotherms) are shown in Equations
(23.1) and (23.2).
y = c ⋅ xn (23.1)
x2 y2
+ =1 (23.2)
a 2 b2

Since the power curves are orthogonal to the elliptic isotherms, the product of
the slope of the power curves and ellipses must be equal to –1 at their intersection.
Equidistant points (the number of power curves) on the perimeter of the ellipse with
known values of “a” and “b” were found. These points are at the intersections
between the ellipse and the power curves, and the arc length of an ellipse between
the horizontal axis and angle 2 was given by:
p = a⋅
∫0
1 − Sin 2 θ ⋅ dθ (23.3)
where e is the eccentricity (the measure of the roundness of ellipse) and is given by:
a 2 − b2
e= (23.4)
a
The arc length between two intersection points was: perimeter/(number of power
curves + 1). Equation (23.3) was used to determine the angle necessary for a given
arc length; a bisection method was applied to find the intersection point xint, yint. Then,
knowing the “a,” “b,” “xint,” and “yint” values, the coefficients of the power curves were
calculated using the orthogonality requirement between the ellipse and power curves:
y int
n= (23.5)
sp ⋅ x int
n −1
where sp ( = c ⋅ n ⋅ x int ) is the slope of the power curve at the intersection point. Then,
the concentric ellipses with major and minor axes decreasing at the same proportions
were drawn. The intersection points between the power curves and the concentric
ellipses were determined by solving Equation (23.6) using the Newton–Raphson
method (Erdoǧdu, 1996; Erdoǧdu et al., 1998b).
x 2int c2 ⋅ x 2intn
f= + −1 (23.6)
a2 b2
For an elliptical cross section of a given thickness, a volume element was defined
as the volume between two consecutive ellipses and power curves (Figure 23.1). The
area bounded by the minor axis and any heat flow line was given by Equation (23.7),
and the area of a given volume element was obtained by successive subtraction of areas
(Erdoǧdu, 1996; Erdoǧdu et al., 1998b). The volume of each element was calculated by
multiplying its area by its thickness approximating the curved surfaces by planar surfaces.
x2
b⋅ 1− 2
x int a
A=
∫ ∫
0 c⋅x n
dy ⋅ dx (23.7)

a
a
a
b
b
a
b
b b
b a
b
b b b
b
b a
b b b
b b
b b b
cc b a
c b b b b
c b b
FIGURE 23.1 Representation of volume element network in an elliptical cross section for the
power curves method. (Adapted from Erdoǧdu, F., Balaban, M.O., and Chau, K.V., J. Food
Eng., 38, 223–239, 1998.)
Then, the finite difference equations were generated by writing energy balance
equations for each volume element. The outer surface nodes were treated as nonca-
pacitance surface nodes (NCSN) (Chau and Gaffney, 1990; Welt et al., 1997;
Erdoǧdu, 1996; Erdoǧdu et al., 1998b). The equations generated for an infinite
elliptical cylinder (Figure 23.1) are given below for surface volume elements (a),
volume elements between surface and center along the heat flow lines (b), and center
volume elements (c), respectively.
Volume element type a:
 
k⋅A 
n +1 ∆t  i , j−1 n −1 1 n 
Ti, j = Ti, j +
n
⋅ ⋅ (Ti, j − Ti, j ) +
n
⋅ ( T∞ − Ti, j ) (23.8)
ρ ⋅ c p ⋅ Vi, j  ∆ri, j−1 1 ∆ri, j 
 + 
 h ⋅ A i, j k ⋅ A i, j 
Volume element type b:
∆t  k ⋅ A i, j−1 k ⋅ A i, j 
Tin, j+1 = Tin, j + ⋅ ⋅ (Tin, j−1 − Tin, j ) + ⋅ (Tin, j+1 − Tin, j ) (23.9)
ρ ⋅ c p ⋅ Vi, j  ∆ri, j−1 ∆ri, j 
Volume element type c:
∆t  k ⋅ A i, j−1 
Tin, j+1 = ⋅ ⋅ (Tin, j−1 − Tin, j ) (23.10)
ρ ⋅ c p ⋅ Vi, j  ∆ri, j−1 
In the case of finite elliptical cylinders, where heat flow is assumed to be in the
longitudinal direction and along the heat flow line, nine finite difference equations

were needed. A detailed description for the generation of these equations was given
by Erdoǧdu (1996) and Erdoǧdu et al. (1998b).
An explicit method was used to solve the finite difference equations. At the end
of each time step, there were slightly different temperatures for the center volume
elements. Therefore, the overall volume average temperature of the center elements
was calculated. For the next time step, the initial temperature of all the center volume
elements was taken as the average temperature. The computer program to solve
these equations was written in Visual Basic V. 6.0 (Microsoft, 1994). The details of
the program are given in Erdoǧdu (1996) and Erdoǧdu et al. (1998b).
23.2.2 AN ALTERNATE FLEXIBLE METHOD

The following procedure was used to generate the numerical network for the alternate
flexible method for the numerical evaluation of conduction heat transfer in elliptical
cylinders. By using Equations (23.1), (23.2), and (23.3), the equidistant points on the
perimeter of the ellipse with known values of “a,” “b,” and “P” were found, and the
θ angle values giving this equidistant arc length between the points (Equation (23.3))
were evaluated using a bisection method. The x and y values of the equidistant points
were determined using a bisection method with the known θ value. The boundaries
of the volume elements were formed by drawing lines parallel to the x and y axes
from the equidistant points. The points where the lines parallel to the x axis intersected
with the boundary were used as the starting point for the points parallel to the y axis,
and all these were applied to the other three quadrants in a cross section (Figure 23.2).
Type 5
d: Type 4 b
Quadrant 4 e b Quadrant 1
e c
b Type 3
e c c
e c c c b
Type 6
c c c c b: Type 2
e
Type 7
f g g g g g a: Type 1
Quadrant 3 Quadrant 2
FIGURE 23.2 Representation of volume element network in an elliptical cross section for
the alternate flexible approach.

Vn
yn – 1
yn
xn – 1 xn
FIGURE 23.3 Representation of volume of a surface element in the volume element network
for the alternate flexible approach.
Surface volume elements were treated as capacitance surface nodes (CSN) (Welt
et al., 1997). The volume and surface area of the volume elements were determined
by using those of a rectangle for the inside nodes, and by integration for the surface
nodes. The volume of a surface element for a known thickness (∆l) is given in
Equation (23.11) (Figure 23.3):
 xn 
∫
b
Vn =  ⋅ a 2 − x 2 ⋅ dx − [( x n − x n −1 ) ⋅ ( y n − y n −1 )] ⋅ ∆ l  (23.11)
 a 
x n −1 
The heat transfer area of the CSN was taken as the curve bordered by the
equidistant points. It was the product of arc length and the given thickness. The
finite difference equations were generated developing energy balance equations for
each volume element. The thermal and physical properties of each volume element
were independent of the others. Figure 23.4 shows the different types of volume
elements in quadrant 1 of an elliptical cross section. Equations (23.12) to (23.18)
are the generated finite difference equations for these volume elements.
Volume element type 1:
 1 k ⋅ YA q1,i, j+1 
1 − ∆t ⋅ ⋅  q1,i, j 
 (ρ ⋅ c p ⋅ V)q1,i, j  ∆x q1,i, j 
Tqn1+1 (i, j) = Tqn1 (i, j) ⋅  
  
+ k q 2,i, j ⋅ XA q1,i, j+1 + h 
 q1,i , j ⋅ YA q1,i , j  
∆y q1,i, j 
 
 k q1,i, j ⋅ YA q1,i, j+1 n k ⋅ XA q1,i, j+1 n 

 ⋅ Tq1 (i, j + 1) + q 2,i, j ⋅ Tq1 (i − 1, j + 1)
∆x q1,i, j ∆y q1,i, j
+ ∆t ⋅  
 
+ h q1,i, j ⋅ YA q1,i, j−1 ⋅ Tq∞1,n (i, j) 
(23.12)

Type 3
Volume element Type 1 Type 2 (i+1,j-1)q1
h convection
h convection
(i,j)=(1,2)
(i,j+1) q1 (i,j)q1 (i,j) q1
(i,j+1) q1 (i,j+1)q1 (i,j)q1 (i,j-1) q1
(i,j)q2 (i-1,j+1)q1
(i-1,j+1)q1
Type 5
Type 4 (i+1,j-1)q1
h convection
(i,j)q4 (i,j)q1
(i,j)q4 (i,j)q1 (i,j-1)q1
(i-1,j+1)q1
(i-1,j+1)q1
Type 6 Type 7
(i+1,j-1) q1 (i+1,j-1) q1
(i,j)q1 (i,j-1)q1 (i,j+1) q1 (i,j) q1 (i,j-1) q1

(i,j)q4
(i,j)q2 (i,j) q2
FIGURE 23.4 Representation of different volume elements in quadrant 1 for the alternate
flexible approach (see Figure 23.1).

 1  k q1, i, j + 1 ⋅ YA q1, i, j 
1 − ∆t ⋅ ⋅ 
 (ρ ⋅ c p ⋅ V) q1, i, j  ∆x q1, i, j 
Tqn1+ 1 (i, j) = Tqn1 (i, j) ⋅  
 
 k q1, i − 1, j + 1 ⋅ XA q1, i − 1, j + 1 
+ ∆y q1, i, j
+ h q1, i, j ⋅ YA q1, i, j − 1  
  
 k q1, i, j + 1 ⋅ YA q1, i, j n k q 2, i, j ⋅ XA q1, i − 1, j + 1 n 

 ⋅ Tq1 (i, j + 1) + ⋅ Tq1 (i − 1, j + 1)
+ ∆t ⋅  ∆ x q1, i , j ∆ y q1, i , j 
 
+ h q1, i, j ⋅ YA q1, i, j − 1 ⋅ Tq∞1, n (i, j) 
 
(23.13)
  k q1,i, j+1 ⋅ YA q1,i, j 

1 − ∆t ⋅ 1 
⋅
 (ρ ⋅ c p ⋅ V)q1,i, j  ∆x q1,i, j 
 
 k ⋅ XA k ⋅ XA 
Tqn1+1 (i, j) = Tqn1 (i, j) ⋅ + q1,i −1, j−1 q1,i , j−1
+ q1,i +1, j−1 q1,i +1, j−1 
 ∆y q1,i, j−1 ∆y q1,i +1, j−1 
 
 
 k q1,i −1, j+1 ⋅ XA q1,i, j  
 +  
 ∆ y q1,i , j  
 k q1,i, j+1 ⋅ YA q1,i, j n k ⋅ XA q1,i, j−1 n 

 ⋅ Tq1 (i, j + 1) + q1,i, j−1 ⋅ Tq1 (i, j − 1) 
∆x q1,i, j ∆y q1,i, j−1
 
+ ∆t ⋅  
 k q1,i +1, j−1 ⋅ XA q1,i +1, j−1 n k q1,i −1, j+1 ⋅ XA q1,i, j n 
+ ∆y q1,i +1, j−1
⋅ Tq1 (i + 1, j − 1) +
∆y q1,i, j
⋅ Tq1 (i − 1, j + 1)
 
(23.14)
 1  k q 4, i, j ⋅ YA q1, i, j 
1 − ∆t ⋅ ⋅ 
 (ρ ⋅ c p ⋅ V) q1, i, j  ∆x q1, i, j 
Tqn1+ 1 (i, j) = Tqn1 (i, j) ⋅  
 
 k q1, i − 1, j + 1 ⋅ XA q1, i, j 
+ ∆y q1, i, j
+ h q1, i, j ⋅ YA q1, i, j  
  
 k q 4, i, j ⋅ YA q1, i, j n k q1, i − 1, j + 1 ⋅ XA q1, i, j n 

 ⋅ Tq 4 (i, j) + ⋅ Tq1 (i − 1, j + 1)
+ ∆t ⋅  ∆ x q1, i , j ∆ y q1, i , j  (23.15)
 
+ h q1, i, j ⋅ YA q1, i, j ⋅ Tq∞1, n (i, j) 
 

 1  k q 4, i, j ⋅ YA q1, i, j 
1 − ∆t ⋅ ⋅ +
 (ρ ⋅ c p ⋅ V) q1, i, j  ∆x q1, i, j 
Tqn1+ 1 (i, j) = Tqn1 (i, j) ⋅  
 
 k q1, i, j − 1 ⋅ YA q1, i, j − 1 k q1, i − 1, j + 1 ⋅ XA q1, i, j  
 + 
∆x q1, i, j − 1 ∆y q1, i, j  

 k q 4, i, j ⋅ YA q1, i, j n k q1, i, j − 1 ⋅ YA q1, i, j − 1 n 

 ⋅ Tq 4 (i, j) + ⋅ Tq1 (i, j − 1) + 
 ∆ x q1, i , j ∆ x q1, i , j − 1  (23.16)
+ ∆t ⋅  
 k q1, i − 1, j + 1 ⋅ XA q1, i, j n 
 ⋅ Tq1 (i − 1, j + 1) 
 ∆ y q1, i , j 
 1 k ⋅ YA q1,i, j 
1 − ∆t ⋅ ⋅  q 4 ,i , j 
 (ρ ⋅ c p ⋅ V)q1,i, j  ∆x q1,i, j 
Tqn1+1 (i, j) = Tqn1 (i, j) ⋅  
  
+ k q 2,i, j ⋅ XA q1,i, j + k q1,i, j−1 ⋅ YA q1,i, j−1 + k q1,i +1, j−1 ⋅ XA q1,i +1, j−1 
 ∆y q1,i, j ∆x q1,i, j−1 ∆y q1,i +1, j−1 
 
 k q 4,i, j ⋅ YA q1,i, j n k ⋅ XA q1,i, j n 

 ⋅ Tq 4 (i, j) + q 2,i, j ⋅ Tq 2 (i, j) 
∆x q1,i, j ∆yy q1,i, j
 
+ ∆t ⋅  
 k q1,i, j−1 ⋅ YA q1,i, j−1 n k q1,i +1, j−1 ⋅ XA q1,i +1, j−1 n 
+ ∆ x
⋅ Tq1 (i, j − 1) +
∆ y
⋅ Tq1 (i + 1, j − 1)
 q1,i , j−1 q1,i +1, j−1 
(23.17)
 1  k q1, i, j + 1 ⋅ YA q1, i, j 
1 − ∆t ⋅ ⋅ 
 (ρ ⋅ c p ⋅ V) q1, i, j  ∆x q1, i, j 
Tqn1+ 1 (i, j) = Tqn1 (i, j) ⋅  
 
 q1, i, j − 1
k ⋅ YA q1, i , j − 1 k q1, i + 1, j − 1 ⋅ XA q1, i + 1, j − 1 k q 2, i , j ⋅ XA 
q1, i , j 
 + + + 
∆x q1, i, j − 1 ∆y q1, i + 1, j − 1 ∆y q1, i, j  

 k q1, i, j ⋅ YA q1, i, j n k q1, i, j − 1 ⋅ YA q1, i, j − 1 n 

 ⋅ Tq1 (i, j + 1) + ⋅ Tq1 (i, j − 1) 
 ∆ x q1, i , j ∆ x q1, i , j − 1 
+ ∆t ⋅  
 k q1, i + 1, j − 1 ⋅ XA q1, i + 1, j − 1 n k q 2, i, j ⋅ XA q1, i, j n 
+ ⋅ Tq1 (i + 1, j − 1) + ⋅ Tq 2 (i, j)
 ∆ y q1, i + 1, j − 1 ∆ y q1, i , j 
(23.18)

An explicit method was used to solve these finite difference equations. All
calculations were performed using a computer program written in Visual Basic V.
6.0 (Microsoft, 1994). The developed program calculated the temperature distribu-
tion in elliptical cross sections using the power curves method and alternate flexible
approach. The flow diagram for the developed program for both approaches is given
in Figure 23.5.
A. Volume element network generation

Data Input:
a: half-major, b: half-minor axis for elliptical cross-section for
volume element network generation and all thermophysical
properties
Calculation of:
eccentricity, perimeter, arc length between two intersection points
and the coordinates of the intersection points using Eqs. 3.4.1
to 3.4.6
B. Calculation of the physical properties of the volume elements and

generation of finite difference equations
Defining the volume elements for power curves method of the

alternate flexible approach
Calculation of the area and volume of each volume element using

Eqs. 3.4.7 to 3.4.11 and the distances between the volume
elements in each direction
C. Generation of finite difference equations and the solution using an

explicit procedure
Generation of finite difference equations (using Eqs. 3.4.8 to 3.4.10

for the power curves method and Eqs. 3.4.12 to 3.4.18 for power
curves method for the alternate flexible approach) by writing energy
balances for each volume element, and using an explicit procedure
to solve these equations knowing outside temperatures, product
properties, and heat transfer conditions on the surface
FIGURE 23.5 Flow diagram of the developed program for the power curves method and the
alternate flexible approach.

The NCSN and CSN volume element finite difference models developed for mod-
eling of heat conduction in elliptical cross sections were validated by experiments.
Long plexiglass elliptical cylinders with eccentricities of 0.63 (a = 2.2 cm, b = 1.7
cm, l = 15 cm) and 0.69 (a = 1.25 cm, b = 0.9 cm, l = 8 cm) were used for the
validation studies. The thermal conductivity, heat capacity, and density of these
3
cylinders were 0.1875 W/m-K, 1465.4 J/kg-K, and 1190 kg/m , respectively (Poly-
cast Technology, 1996).
Heating experiments were performed in a well-agitated water bath (infinite h),
2
and cooling was done in ice slush (h ≈200 W/m °K) (Erdoǧdu et al., 1998a).
Time–temperature data from the experiments were gathered using Type-T, 36 gauge
thermocouples (Ecklund, Fort Myers, FL), inserted and stabilized in the cylinders, and
a data acquisition system (DAS-TC, Kethley Metrabyte, Taunton, MA). The experi-
mental data were compared with the model results. Ten experiments were conducted
for the validation studies at temperatures of 75 and 85°C. Figures 23.6 and 23.7 show
the comparison of two of the experimental and predicted temperatures (at center and
off-center points) of “infinite” elliptical cylinders of eccentricity of 0.69 and 0.63 by
the alternate flexible approach and the power curves method. In both approaches, the
model predictions were close to the experimental results. Since a circular cross section
can be described as an elliptical cross section with equal “a” and “b” values, both
approaches can also be used for simulation studies in circular cylinders.
The advantage of the power curves method is that it reduces the heat transfer
problem from three- to two-dimensional in finite cylinders, and from two- to one-
dimensional in infinite cylinders. However, the advantage of the second approach
over the power curves method is that it allows simulations with different boundary
conditions in different directions and different volume elements, as seen in Figure 23.8.
100
80
Temperature (°C)
60
40
20
0
0 5 10 15 20 25 30 35
Time (min)
Model Center Exp. Center Model Off-center

Exp. Off-center Medium Temperature
FIGURE 23.6 Comparison of experimental and model center temperatures in a long elliptical
cylinder (a = 2.2 cm, b = 1.7 cm, l = 15 cm, e = 0.63; by alternate flexible approach).

100
Temperature (°C)
80
60
40
20
0
0 5 10 15 20
Time (min)
Model Center Exp. Center Model off-center

Exp. off-center Medium Temperature
FIGURE 23.7 Comparison of experimental and model center temperatures in a long elliptical
cylinder (a = 1.25 cm, b = 0.9 cm, l = 8 cm, e = 0.69; by power curves method).
Quadrant 4 Quadrant 1
T1, h1 T1, h1
Quadrant 2
T2, h2
Quadrant 3
T2, h2
* Shaded areas show the volume elements with different thermophysical properties.
FIGURE 23.8 Representation of using the alternate flexible approach for different boundary
conditions and volume element properties.

For example, the heat transfer problem for an elliptic–cylindrical shaped food with
each half having different boundary conditions, such as one half in sauce and the
other facing air, can be solved using the developed alternate flexible approach. Since
the power curves method assumes the heat transfer along the power curves, not
between them, it becomes impossible to use this method for this kind of problem.
Other examples showing the efficacy of the second method include the following:
Burfoot and James (1988) reported that the heat transfer coefficient is location
dependent for thawing and cooking of cylindrical shaped meats. Burfoot et al. (1990)
compared the heating and cooling times of meat joints. The developed alternate
flexible approach can be easily used for both problems, taking into account the
different thermophysical properties of meat joints and including the bones inside
the meats. The flexibility of the second method when applied to systems with
nonhomogeneous initial temperature distribution can be given as another example
of the efficacy of this method.
23.4 CONCLUSIONS AND SUGGESTIONS

Both power curves and the developed alternate flexible approach were successfully
applied to analyze the heat conduction in elliptical cross sections. Both of these
methods can also be used to predict the temperature distribution in response to
dynamic surface temperature history. The Windows-based software developed in this
study calculated the temperature distribution in infinite elliptical cylinders for both
approaches at any given time, knowing outside temperature (constant or variable),
product properties (homogeneous or heterogeneous), and heat transfer conditions at
the surface (constant throughout the surface or variable).
The validation of the second approach for different food systems and modifica-
tion to simulate the heat transfer in finite cylinders and finite slabs will result in a
powerful tool which can be used for the analysis of thermal processing in food
systems with nonhomogeneous thermal properties.
NOMENCLATURE
a Half-major axis for ellipse, m
2
Ai,j Surface area of the volume element i, j, m
b Half-minor axis for ellipse, m
c Constant
cp Heat capacity, J/kg-K
cp qm,i,j Heat capacity of volume element i, j in quadrant m, J/kg-K
∆r Distance between the volume elements along the heat flow line, m
∆t Time step used in explicit solution method, sec
∆l Thickness for a volume element
e Eccentricity of an ellipse
f Function for the intersection points of ellipses and power curves
2
h Convective heat transfer coefficient, W/m -K
k Thermal conductivity, W/m-K

kqm,i,j Thermal conductivity of volume element i, j in quadrant m, W/m-K
n Constant
p Perimeter of an ellipse, m
3
ρ Density, kg/m
3
ρqm,i,j Density of volume element i, j in quadrant m, kg/m
se Slope of a tangent line at any point on the ellipse
sp Slope of a tangent line at any point on the power curve
Tin,j Temperature of the volume element i, j at the time step n, °C
n +1
T i, j
Temperature of the volume element i, j at the next time step, °C
n
T (i, j)
qm
Temperature of the volume element i, j at the time step n for quadrant
m, °C
n+1
Tqm (i, j) Temperature of the volume element i, j at the next time step for quadrant
m, °C
∞,n
Tqm (i, j) Medium temperature of the volume element i, j at the next time step
for quadrant m, °C
θ The angle of the line connecting the center of an ellipse and a point
on the ellipse circumference, radian
3
Vi,j Volume of the volume element i, j, m
xint,yint Intersection points between a heat flow line and an ellipse
XAqm,i,j The surface area of the volume element i, j in quadrant m in y direction,
∫
m
∫
YAqm,i,j The surface area of the volume element i, j in quadrant m in x direction, m
REFERENCES
Akterian, S.G. and Fikiin, K.A., Numerical simulation of unsteady heat conduction in arbitrary
shaped canned foods during sterilization processes, J. Food Eng., 21, 343–354, 1994.
Burfoot, D. and James, S.J., The effects of spatial variations of heat transfer coefficient on
meat processing times, J. Food Eng., 7, 41–61, 1998.
Burfoot, D., Self, K.P., Hudson, W.R., Wilkins, T.J., and James, S.J., Effect of cooking and
cooling method on the processing times, mass losses and bacterial condition of large
meat joints, Int. J. Food Sci. Technol., 25, 657–667, 1990.
Califano, A.N. and Zaritzky, N.E., A numerical method for simulating heat transfer in heter-
ogeneous and irregularly shaped foodstuffs, J. Food Process Eng., 16, 159–171, 1993.
Chau, K.V. and Gaffney, J.J., A finite difference model for heat and mass transfer in products
with internal heat generation and transpiration, J. Food Sci., 55, 484–487, 1990.
Erdoǧdu, F., Modeling of temperature distribution in shrimp, and measurement of its effect
on texture, shrinkage and yield loss, thesis, University of Florida, Gainesville, 1996.
Erdoǧdu, F., Balaban, M.O., and Chau, K.V., Automation of heat transfer coefficient deter-
mination: development of a Windows-based software tool, Food Technol. Turkey, 10,
66–75, 1998a
Erdoǧdu, F., Balaban, M.O., and Chau, K.V., Modeling of heat conduction in elliptical
cross-section: I. Development and testing of the model, J. Food Eng., 38, 223–239,
1998b.
Eshleman, W.D., A numerical method for predicting heat transfer in axi-symmetrical shaped
solids, thesis, University of Florida, Gainesville, 1976.

Kim, K.H. and Teixeira, A.A., Predicting internal temperature response to conduction-heating
of odd-shaped solids, J. Food Process Eng., 20, 51–63, 1997.
Kirkpatrick, E.T. and Stokey, W.F., Transient heat conduction in elliptical plates and cylinders,
J. Heat Transfer, 80, 54–60, 1959.
Manson, J.E., Stumbo, C.R., and Zahradnik, J.W., Evaluation of thermal process for conduc-
tion heating foods in pear-shaped containers, J. Food Sci., 39, 276–281, 1974.
McLahlan, N.W., Heat conduction in elliptical cylinder and an analogous electromagnetic
problem, Philosophical Magazine, 36, 600–609, 1945.
Microsoft Corporation, Visual Basic Professional, Version 3.0, Microsoft, Redmond, WA,
1994.
Polycast Technology, Thermal Property Data for Acrylic Plexiglass, Polycast, Westport, CT, 1996.
Sheen, S., Tong, C.H., Fu, Y., and Lund, D.B., Lethality of thermal processes for food in
anomalous-shaped plastic containers, J. Food Eng., 20, 199–213, 1993.
Simpson, R., Aris, I., and Torres, J.A., Sterilization of conduction-heated foods in oval-shaped
containers, J. Food Sci., 54, 1327–1331, 1363, 1989.
Welt, B.A., Teixeira, A.A., Chau, K.V., Balaban, M.O., and Hintenlang, D.E., Explicit finite
difference methods for heat transfer simulation and thermal process design, J. Food
Sci., 62, 230–236, 1997.

Heat Transfer Coefficient
24 for Model Cookies in a
Turbulent Multiple Jet
Impingement System
N. Nitin and M.V. Karwe
CONTENTS
24.1 Introduction
24.1.1 Flow Field in a Submerged Turbulent Jet
24.1.1.1 Free Jet
24.1.1.2 Impinging Jet
24.1.1.3 Flow Field in Turbulent Multiple Submerged Jets
24.1.2 Heat Transfer Characteristics of a Single
Impinging Jet
24.1.3 Heat Transfer Characteristics for Multiple Jet Configurations
24.2.1 Experiments (Stationary Mode)
24.2.2 Experiments (Rotational Mode)
24.3.1 Maximum Jet Velocity
24.3.2 Heat Transfer Coefficient
24.4 Conclusions
Nomenclature
Acknowledgment
References
24.1 INTRODUCTION
Jet impingement technology is used in several industrial applications such as electronic
cooling, cooling of hot metal plates and gas turbine blades, high performance low weight
heat exchangers, and driers. In the food industry, jet impingement technology has been
used in baking and freezing operations for faster and better processing due to high heat
transfer rates with better quality retention. Jet impingement ovens are used to bake pizza

shells, crackers, and cookies and to toast ready-to-eat cereals. Prior studies (Walker and
Sparman, 1989) showed that jet impingement ovens could not only reduce the time of
processing by a factor of about two, but also produce good quality products in terms
of better moisture retention. However, little is known about the detailed transport
phenomena associated with multiple jet impingement oven systems.
Several researchers have experimentally investigated the heat transfer associated
with impinging jets. The major studies in this area have been carried out to under-
stand the fluid flow in a single and multiple jet system. A few studies have focused
on heat transfer characteristics. Most of the heat transfer studies apply only to a
narrow range of Reynolds numbers, with the major focus on cooling applications
over a flat surface.
Jets can be broadly classified as submerged or nonsubmerged. When the medium
of the jet is the same as the surrounding medium, it is classified as a submerged jet.
Submerged jets can be further divided into two categories, free jets and impinging
jets. The majority of industrial applications involve impinging jets. In impinging
jets, a jet of liquid or gas comes from a nozzle and impinges on a desired surface,
while in the case of free jets there is no target surface for impingement. Submerged
impinging jets can be further classified as laminar or turbulent jets. When the
Reynolds number based on the nozzle diameter of the jet exceeds 3000, it is generally
classified as a turbulent jet. In this chapter, we focus on turbulent submerged jets
because they are used in food processing operations. cvf(Van Dyke, 1982)
FIGURE 24.1 Laminar region near the nozzle in a turbulent free jet with Reynolds number
Re = 30,000. (From Van Dyke, M., An Album of Fluid Motion, The Parabolic Press, Stanford,
CA, 1982. With permission.)

shows a typical turbulent jet (Re = 30,000) coming out of a tube of diameter 6.35
mm. It shows a laminar region near the nozzle before the jet becomes turbulent.
Since the nature of the flow depends upon the axial downstream distance, the heat
transfer characteristic in jet impingement will depend upon the distance of the target
plate from the nozzle.
24.1.1 FLOW FIELD IN A SUBMERGED TURBULENT JET

24.1.1.1 Free Jet
Flow field studies (Gardon and Akfirat, 1965) for a submerged single turbulent free
jet have shown that as the jet comes out of a nozzle, there is a mixing of the jet air
with the surrounding air with an increase in the width of the mixing region. This is
shown schematically in Figure 24.2 (Gardon et al., 1965). In the initial region of
about 4–5 nozzle diameters, the mixing of the jet air with surrounding air takes
place only at jet boundaries. The mixing results in an exchange of momentum of
the jet at the jet boundaries with the surrounding medium. This exchange of momen-
tum decreases the jet velocity at the jet boundary, while the centerline velocity does
not change significantly over this initial region, characterized as a potential core
region. Beyond this potential core region, the centerline velocity decreases as more
and more of the surrounding fluid is entrained. This results in an increase in the
@ Z/D= 12
@ Z/D= 2 @ Z/D= 6
U/ UE
0 1
U/ UE
0 1
U/ UE
0 1 VELOCITY
VELOCITY
VELOCITY
TURBULENCE
TURBULENCE
MIXING TURBULENCE
REGION
0 0.2
U’/ UM 0 0.2
POTENTIAL CORE U’/ UM
0 0.2
’
U / UM
FIGURE 24.2 Schematic distribution of velocity and turbulence in an axis-symmetric jet.

U = jet velocity; UE = jet exit velocity; UM = r.m.s. value of fluctuating component of velocity;
U′ = centerline velocity of jet; Z/D = ratio of axial distance to nozzle diameter. (Adapted
from Gardon, R. and Akfirat, J.C., Int. J. Heat Mass Transfer, 8, 1261–1272, 1965.)

D
FREE JET
STAGNATION ZONE
LATERAL SPREAD
REGION
PLATE
FIGURE 24.3 Schematic diagram of three zones in a single impinging jet.
width of the mixing region. The mixing of the surrounding air with the jet air
generates turbulence in the free jet (Gardon and Akfirat, 1964; Gardon and Cobon-
pue, 1961). Figure 24.2 shows that the turbulence level increases with the increase
in jet length. The peak of the turbulence shifts from the outer region of the jet to
the center of the jet with downstream distance.
24.1.1.2 Impinging Jet
Flow studies (Gardon and Akfirat, 1964; Martin, 1977) have indicated that flow in
a turbulent single impinging jet can be divided into three regions: the free jet region,
the stagnation region, and the lateral spread region. Figure 24.3 shows these three
regions in a single impinging jet. In the free jet region, the flow behavior is the same
as discussed above for the free submerged turbulent jet. The impinging jet behaves as
free jet up to a distance of about 1–1.5 nozzle diameters from the impinging surface.
After this, deceleration of the impinging jet begins as the jet enters into the stagnation
region. In the stagnation region there is impingement and deflection of the jet. In
this region, the jet experiences a deceleration (Gardon and Akfirat, 1965). The axial
velocity decreases rapidly, and the static pressure rises. In the lateral spread region,
the negative pressure gradient causes a rapid increase in the radial velocity near the
deflection region, and it drops away to a region away from it. This drop in velocity
is due to wider area available for the same mass of material to flow and also due to
the viscous losses at the wall.
24.1.1.3 Flow Field in Turbulent Multiple Submerged Jets
The majority of studies in the flow field of multiple jets geometry for turbulent
regime (Re ~ 25,000) have been done using nonsubmerged water jets (Viskanta and
Huber, 1994b; Saripalli, 1983). Only a few studies on flow field have been reported
using a submerged air jet system. One of the major flow field studies (Marcoft,
1999) using a submerged air multiple jets configuration has been done using the
technique of LDA (Laser Doppler Anemometry). It was used to map the velocity
field for three- and four-jet configurations. The results showed that the axial velocity
contours for multiple submerged air jet configurations show similar trends in the

60
Uz (m/sec)
40
23.94
20.16
16.38
20 Jet #3 12.61
Y(mm)
8.83
Jet #2
5.05
0 1.28
-2.50
Jet #1 -6.27
-20 -10.05
-40
-80 -60 -40 -20 0 20
X(mm)
-X
+Z
10 mm
FIGURE 24.4 Contours of constant axial (uz) velocity for three jets impinging on a flat plate.
Measurements made in a plane 10 mm from the flat plate.
free mixing and stagnation region as discussed for single jet configuration. Figure 24.4
and Figure 24.5 show the details of velocity contours at a distance of 10 mm from
the impingement plate for three- and four-jet configurations, respectively. In addition
to the characteristics of the velocity field for a single jet, the measured velocity
profiles also showed negative velocity regions in the lateral flow regime. These
negative velocity regions result because of the interaction between the adjacent jets,
which causes flow reversal in the lateral flow regime of the multiple jets. This region
has been shown to be of great importance in describing the heat transfer character-
istics of multiple jets (Marcoft, 1999). For measurements made close to the flat plate,
the magnitude of maximum negative velocity in these regions was almost 50% of
the maximum jet velocity measured near the nozzle exit. The range of this negative
velocity depends on the nozzle-to-nozzle spacing, velocity of the jets, and nozzle-
to-plate spacing. Similar results of jet interaction resulting in reverse flow have been
shown (Viskanta and Huber, 1994b; Saripalli, 1981) using water jets. Both of these
studies have shown the formation of an interaction fountain, i.e., the reverse flow
in between the adjacent impinging jets. Figure 24.6 shows the details of the reverse
flow in the form of an interaction fountain between the adjacent jets for water jets.

Jet #3
40
20 Jet #4
Uz (m/sec)
21.49
18.18
0 14.87
11.56
8.25
-20 Jet #2 4.94
1.62
Y -1.69
(mm) Jet #1
-5.00
-40
-8.31
-60
-80
-100
-80 -60 -40 -20 0 20 40
X (mm)
-X
+Z
10 mm
FIGURE 24.5 Contours of constant axial (uz) velocity for four jets impinging on a flat plate.
Measurements made in a plane 10 mm from the flat plate.
INTERACTION
INTERACTION FOUNTAIN
FOUNTAIN
FIGURE 24.6 Schematic diagram of reverse flow (interaction fountain) in multiple jet con-
figurations.
24.1.2 HEAT TRANSFER CHARACTERISTICS OF A SINGLE IMPINGING JET

The heat transfer characteristics for a single jet impinging on a flat surface show
maxima in the magnitude of the heat transfer coefficient in the stagnation region of
the jet. The magnitude of these maxima is shown to be a function of the Reynolds
number and nozzle-to-plate separation (Gardon and Akfirat, 1964; Martin, 1977).
With an increase in Reynolds number and in nozzle-to-plate spacing up to 5–6 nozzle
diameters, the magnitude of the maxima in heat transfer coefficient increases (Gardon
and Akfirat, 1965). Figure 24.7 (Gardon and Akfirat, 1965) shows the variation of
heat transfer coefficient at different nozzle-to-plate spacings. The increase in heat
transfer coefficient with the increase in nozzle-to-plate spacing is due to the increase

LOCAL HEAT TRANSFER COEFFICIENT, h (Btu/h ft2 degF) 100
B = 1/8 in. B = 1/8 in. B = 1/8 in.
Ree = 11000 Ree = 11000 Ree = 11000
8 8
6
80
5
16
2
zn / B zn / B zn / B = 1/3
60
32
2
40 5 8
6 16
8 32
80
80
20
(a) 2 ≤ zn / B ≤ 8 (b) 8 ≤ zn / B ≤ 80 (c) zn / B = 1/3

0
-20 -10 0 10 20 -20 -10 0 10 20 -20 -10 0 10 20
DISTANCE FROM STAGNATION POINT, x/B
FIGURE 24.7 Lateral variation of local heat transfer coefficients between a plate and an
impinging two-dimensional air jet at different nozzle-to-plate distances. (From Gardon, R.
and Akfirat, J.C., Int. Heat Mass Transfer, 8, 1261–1272, 1965. With permission.)
in level of turbulence developed as a result of mixing of the surrounding air while

the centerline velocity is nearly constant (Gardon and Akfirat, 1965). For nozzle-to-
plate spacing greater than eight nozzle diameters, a decrease in the magnitude of
maxima for the heat transfer coefficient around the stagnation region is observed,
as shown in Figure 24.7. This has been explained by the decrease in the velocity of
the jet with no appreciable increase in the turbulence level with an increase in the
distance from the jet nozzle beyond seven nozzle diameters. This clearly shows that
the magnitude of the maxima in heat transfer coefficient in the stagnation region is
due to two parameters, turbulence and jet velocity.
The studies of small nozzle-to-plate spacing, i.e., between 0.25 and 1 nozzle
diameters, have shown great potential for cooling applications in the electronic
packaging industry (Viskanta and Huber, 1994a). This study showed that at a large
Reynolds number (Re ~ 15,000) and small nozzle-to-plate spacing (0.25–1 nozzle
diameters), the maximum in the heat transfer coefficient is observed not at the
stagnation point as for large nozzle-to-plate spacing (5–6 nozzle diameters), but at a
distance away from the center. Figure 24.8 (Viskanta et al., 1994a) shows the variation
of local heat transfer coefficient (represented in terms of the dimensionless heat
transfer number, Nusselt number (Nu)) for small nozzle-to-plate spacing.
Similar trends were also observed by others (Goldstein and Seol, 1991; Ichimiya
and Okuyama, 1980; Lytle and Webb, 1994; Saad et al., 1980). For nozzle-to-plate
spacing of less than one nozzle diameter, the local heat transfer coefficient in the
stagnation region increases as the distance between the plate and the nozzle
decreases. The existence of secondary maxima in the local heat transfer has also
been indicated for small nozzle-to-plate spacing, whereas there is a monotonous

(a)
120
100 0.25
Local Nusselt number NuD

1.0
80
60
40
H/D = 6.0
20
0
0 0.5 1 1.5 2 2.5 3
r/D
(b)
140
120 0.25
Local Nusselt number NuD
1.0
100
80
60 H/D = 6.0
40
20
0
0 0.5 1 1.5 2 2.5 3
r/D
FIGURE 24.8 Effect of separation distance (H/D) on local Nusselt number distributions for
Reynolds number (a) 10,300 and (b) 17,100. (From Huber, A.M. and Viskanta, R., ASME J.
Heat Transfer, 116, 573, 1994a. With permission.)
decrease in heat transfer coefficient in the lateral region for large nozzle-to-plate
spacing. This difference in the variation of heat transfer coefficient at very small
nozzle-to-plate spacing (less than one nozzle diameter) has been attributed to the
difference in the nature of the jet. For very small spacing the shear layer does not
develop, as the jet does not get a chance to mix with the surrounding air. The
existence of local maxima near the center of the jet has been attributed to the sudden
acceleration of the fluid after impinging on the plate (Viskanta and Huber, 1994a).
In the lateral spread region of a single jet, the heat transfer coefficient drops
monotonously with the radial distance for nozzle-to-plate spacing greater than five
nozzle diameters. For nozzle-to-plate spacing between two and five nozzle diameters,
the heat transfer does not drop monotonously, as in the earlier case. There are small

secondary maxima in the heat transfer coefficient around the stagnation point. This
point is illustrated in Figure 24.7. Beyond these small secondary maxima in the lateral
region for the case of nozzle-to-plate spacing of between two and five nozzle diameters,
the heat transfer coefficient drops monotonously in the lateral spread region of the jet.
The drop in the heat transfer coefficient is steeper in the case of smaller nozzle-to-
plate spacing (Gardon and Akfirat, 1965; Martin, 1977). Thus, the magnitude of the
heat transfer coefficient is more uniform over a wider area for higher nozzle-to-plate
spacing; however, the magnitude of the maxima at stagnation point decreases for large
nozzle-to-plate spacing (greater than eight nozzle diameters). For nozzle-to-plate spac-
ing of less than one nozzle diameter, there is a sharp increase in the magnitude of the
secondary heat transfer coefficient maxima in the lateral jet region (Figures 24.7 and
24.8). The location of these secondary maxima has been found to be a function of the
Reynolds number and plate-to-jet spacing. Studies (Martin, 1977; Viskanta and Huber,
1994a) have shown that for smaller nozzle-to-plate spacing, the average heat transfer
coefficient is higher due to existence of these secondary maxima.
24.1.3 HEAT TRANSFER CHARACTERISTICS FOR MULTIPLE

JET CONFIGURATIONS
Relatively few studies have been carried out to characterize heat transfer in multiple
jet configurations. The heat transfer characteristics for multiple jets in the stagnation
region are expected to be similar to those of a single jet. In the lateral spread region,
some difference in heat transfer characteristics is expected due to interaction of
adjacent jets. As described earlier, the fluid flow in the case of the multiple jet system
shows an interaction between adjacent jets depending upon the spacing of adjacent
jets. This interaction, which induces the reverse flow, has been shown to significantly
increase the heat transfer for multiple jet configurations (Lytle and Webb, 1994;
Viskanta and Huber, 1994b). The existence of secondary maxima in the lateral region
due to jet interaction has also been shown in the study by Viskanta and Huber
(1994b). The increase in the heat transfer coefficient has been attributed to increased
turbulence due to jet interaction.
The objective of our study reported in this chapter was to determine the corre-
lations for average surface heat transfer coefficient for a cookie-shaped object in a
pilot scale jet impingement oven. The variation of the heat transfer with position of
the model object in the oven, size of the model object, rotation of the oven plate,
air velocity, and air temperature was investigated.

During baking or cooking in a jet impingement oven, simultaneous heat and mass
transfer occurs. The resistance to heat transfer in an actual baking operation lies both
in the hot fluid and the food material. Since our goal was to determine only the surface
heat transfer characteristics, we chose a lumped mass approach. In this approach, the
resistance offered by the material to heat transfer was kept negligible, which happens
when the Biot number is less than 0.1. Aluminum disks were used as model cookies

in this study. Aluminum has a high thermal conductivity value (200 W/mK). Therefore,
the Biot number (=hH/ks) based on the thickness of the disk was expected to be much
less than 0.1, where h is the average surface heat transfer coefficient and it is supposed
2
<2000 W/m K, ks is the conductivity of the solid, and H is the thickness of the disk.
This requirement was later verified from the experimental results. In jet impingement,
forced convection heat transfer occurs, and in forced heat convection the h value
depends only on the shape of the object and not on the thermal properties of the object.
Selection of this approach also eliminates the mass transfer process in the system.
So, from the transient heat transfer response of the system to step change in ambient
temperature, h can be calculated from the response time τ of the system using
Equation (24.1).
For Bi < 0.1, the variation of temperature of the cookies with time is given by
−t/τ
(Tt − To)/(Ti − To) = e (24.1)
where Tt = temperature at the center of the cookie at any time t, Ti = initial temperature
of the cookie, To = temperature of the heating medium, t = time, and τ = time constant
of the cookie.
τ = mcp/h A (24.2)
where m = mass of the cookie, cp = heat capacity, h = average surface heat transfer
coefficient, and A = surface area of the cookie.
The slope of the plot of ln (Tt − To)/(Ti – To) vs. time (t) will be –1/τ, from
which h can be calculated.
The study was carried out using a pilot plant scale jet impingement oven (Jetzone,
Wolverine Corporation, Merrimac, MA). Figure 24.9 shows the schematic diagram
of the multiple jets and test chamber and the position of the jet tubes. The impingement
oven consisted of an air filter, three electric heaters, a blower, a plenum chamber,
an electric motor, a rotating turntable, an aluminum bowl, and an exhaust fan. During
processing, heated air was directed downward from the plenum chamber through
13 parallel jet tubes to impinge on a product in the bowl, which was placed on a
rotary (maximum of 60 r/min) turntable. During operation, the bowl was lifted until
it pressed against the glass canopy. A rubber bushing sealed the bowl with the glass
canopy. The maximum pressure in the plenum chamber that could be maintained
was 1200 Pa (five in water). Each jet tube was 420 mm long with an inner diameter
of 17.6 mm. The maximum velocity in each jet was 50 m/sec. The temperature of
the jets could be maintained between room temperature and 232°C. Aluminum disks
of different diameters were selected to study the effect of variation of size of the
model object on the heat transfer coefficient. The sizes of different model aluminum
cookies studied are listed in Table 24.1. The 50 and 35 mm cookies with thicknesses
of 10 and 15 mm, respectively, were selected so that the cookies would have the
same total surface area. The 8 mm diameter cookie with a thickness of 10 mm was
selected to study the effect of variation of the local average heat transfer for cookies
placed right under the jet, as the diameter of this cookie was smaller than the jet diameter.

TABLE 24.1
Description of Dimensions of Model Cookies
Diameter Thickness Area/Mass Ratio
2
Geometry (mm) (mm) (mm /kg)
Disk 50 10 6.58E-04
Disk 20 10 1.73E-03
Disk 8 10 2.15E-03
Disk 35 15 6.58E-04
Plenum Chamber
Glass
Canopy
Jet Tubes
(13)
Rubber
Bushing
Aluminum
Bowl
Turntable
(a)
2 6 10
1 3 7 11 13
53.4 mm
18.6
mm
4 8 12
53.2 mm
9 (b)
FIGURE 24.9 Schematic diagram of (a) the test chamber and (b) positions of the jet tubes.

During the experiment, the aluminum cookies were placed on a wooden plate so
that no heat transfer would take place from the bottom of the aluminum bowl due
to conduction.
To get the transient temperature response, a thermocouple was inserted at the
center of the cookie from the bottom. To measure the cookie center temperature (Tt)
and the jet air temperature (To), T-type thermocouples made using 30-gauge wires
were used. The response time for these thermocouples in this system was on the order
of 0.5 seconds. To measure the cookie center temperature, a hole was drilled up to
half the thickness of the cookie, and a thermocouple supported on metal tubing was
inserted. In order to ensure proper contact between the cookie and the thermocouple,
the hole was filled with high conductivity Omegatherm paste (Omega Engineering,
Inc., Stamford, CT). The variation of temperature with time in stationary mode of the
turntable was recorded using Keithley Metrabyte data acquisition hardware and
TestPoint software (Keithley Inc., Cleveland, OH). During the rotation mode of the
turntable, the ACR data acquisition system (Webco Controls Inc., Ambler, PA) was
used to record the temperature versus time. The ACR system consisted of a program-
mable data logger box, which could be attached to the rotating bowl.
To develop heat transfer coefficient correlations in terms of Reynolds number,
experiments were carried out at different values of jet velocity, which was varied
by varying the plenum pressure. The maximum jet velocity under each jet was
measured using a pitot tube (Airflow Technical Products, Netcong, NJ).
24.2.1 EXPERIMENTS (STATIONARY MODE)

Temperature measurement experiments were carried out without rotation of the
turntable. The metal cookie was placed inside the aluminum bowl at different
positions. The base of the metal bowl was insulated using a piece of wood of the
same diameter as the bowl in order to eliminate any conduction heat transfer to the
cookie from the base of the bowl. The experiments were carried out under jets #3,
#7, and #11 and midway between jet #3 and jet #7 (see Figure 24.9). The jet temper-
atures were varied at four levels (65, 94, 121, and 148°C). The air pressure in the
plenum chamber was varied at four levels (250, 500, 775, and 1050 Pa). Full factorial
design was implemented with three replications. The same experimental design was
carried out for all the different cookie sizes selected for the study.
24.2.2 EXPERIMENTS (ROTATIONAL MODE)

Under this set-up, the major objective was to study the effect of rotation on the heat
transfer coefficient as compared to the stationary mode. The cookie was placed under
the center of jet # 3, which was off-center with respect to the center of the bowl.
The jet temperature was maintained at 107°C and the pressure was varied at 250
and 1050 Pa. The speeds of rotation of the turntable were 12 and 60 r/min. The
experiments were designed to have all possible combinations of rotation speed and
pressures with three replications of each data set. The data were collected using the
ACR portable data logger. For analyzing the effect of rotation, the data were also
collected in stationary mode under same conditions of temperature and pressures

using the same data acquisition system. For the rotation mode, the experiments were
carried out for the 50 mm diameter disk with 10 mm thickness and 20 mm diameter
with 10 mm thickness.

24.3.1 MAXIMUM JET VELOCITY
Figure 24.10 shows variation of maximum jet velocity measured at 20 mm from the
tube ends as a function of pressure in the plenum chamber for the three different
jets under different conditions of temperature. The results showed an expected
nonlinear increase in velocity with an increase in the jet air pressure. The results
Jet #3 Jet #7
45 45
40 VELOCITY (m/sec) 40
VELOCITY (m/sec)
35 35
65¡C 65¡C
30 94¡C 30 94¡C
121¡C 121¡C
25 25
148¡C 148¡C
20 20
15 15
0 500 1000 1500 0 500 1000 1500
PRESSURE (Pa) PRESSURE (Pa)
(a) (b)
Jet #11
45
40
VELOCITY (m/sec)
35
65¡C
30
94¡C
25 121¡C
148¡C
20
15
0 500 1000 1500
PRESSURE (Pa)
(c)
FIGURE 24.10 Variation of maximum jet velocity with pressure in the plenum chamber:
(a) jet #3, (b) jet #7, (c) jet #11.

also indicated the increase in velocity with increase in temperature at a given
pressure. This was expected, as the density of the air decreases with increase in
temperature. The results of the velocity measurement experiments using the pitot
tube indicated a fair amount of uniformity in the maximum velocity under different
jets at same conditions of temperature and pressure. The velocity values ranged from
18 to 44 m/sec. The experimentally determined value of maximum velocity was
used to calculate the Reynolds number values.
24.3.2 HEAT TRANSFER COEFFICIENT

The results for the average heat transfer coefficient (h), obtained from Equation (24.2.),
are presented in terms of average Nusselt number (Nu), as a function of the Reynolds
number (Re) and Prandtl number (Pr), defined as follows:
Nud = hD/ka Re = ρVD/µ Pr = Cp µ/ka
where h is calculated using Equation (24.2), ka is the thermal conductivity of air, ρ

is the density of air, V is the maximum jet velocity, D is the jet tube inside diameter,
and µ is the viscosity of air. All properties for air were evaluated at corresponding
jet temperatures. Pr number was almost constant (0.65–0.70) over the entire range
of experimental conditions. Hence, it was taken as constant.
Figure 24.11 shows the variation of Nu with Re under different jets with the
bowl stationary. The Nu values varied from 60 to 120, which correspond to a range
2
of heat transfer coefficient (h) of 140–200 W/m K. The results indicate no significant
difference in the average heat transfer coefficient for a 50 mm cookie placed under
different jets. This indicates that the average value of the heat transfer coefficient
for a 50 mm diameter disk is uniform under different positions in the jet impingement
oven. Similar results were obtained for the 35 mm diameter model cookie with
15 mm thickness.
140
120
NUSSELT NUMBER (Nu)
100
80 Jet #7
Jet #3
60
Between Jet #3
40 and Jet #7
20
0
0 10000 20000 30000 40000
REYNOLDS NUMBER (Re)
FIGURE 24.11 Variation of average Nusselt number (Nu) with Reynolds number (Re) at
different positions in an oven for a 50 mm diameter cookie with 10 mm thickness.

140
120
NUSSELT NUMBER (Nu)
100
#7 (35 mm)
Between #3 and
80
#7 (35 mm)
#3 (35 mm)
60 #7 (50 mm)
#3 (50 mm)
40
Between #3 and
#7 (50 mm)
20
0
0 5000 10000 15000 20000 25000 30000 35000
REYNOLDS NUMBER (Re)
FIGURE 24.12 Variation of average Nusselt number (Nu) with Reynolds number (Re) for
50 mm and 35 mm diameter aluminum cookies with 10 mm and 15 mm thickness, respectively.
Figure 24.12 shows the comparison of the results for the 35 mm diameter cookie
with 15 mm thickness with that of the 50 mm cookie with 10 mm thickness. The
results showed no significant difference in the average heat transfer coefficient for
the two cookie-shaped disks with the same total surface area. The results for the
8 mm diameter cookie with 10 mm thickness showed a higher value of the heat
transfer coefficient. Earlier studies have shown that a local maximum exists in the
heat transfer coefficient right under the jet, i.e., in the stagnation region. Since this
8 mm cookie was just half the diameter of jet, it experienced a peak in local maxima
with the result that the average heat transfer coefficient over a small area showed a
higher value as compared to the other two cookie sizes.
To determine the importance of the operating parameters, jet air pressure and
temperature, on the h values an analysis of variance (ANOVA) for the two-factor
experiment was carried out. It showed that only pressure had a statistically significant
effect on the h value, while temperature did not have significant effect on the heat
transfer coefficient.
To determine the effect of bowl rotation, experiments were carried out with and
without rotation of the bowl under jet #3. Figure 24.13 (a) and (b) shows the variation
of h with bowl rotation at two different plenum pressures for two different sizes of
model cookies. Based on the estimated systematic error in the experimental set-up,
the error bars are drawn to compare the results of the heat transfer coefficient
experienced by a model cookie in a stationary mode with that of a cookie in a
rotational mode. In the case of the 50 mm diameter cookies no effect of rotation
was observed at both levels of rotation speed of the bowl and both levels of plenum
pressure. In the case of the 20 mm diameter cookie, the effect of rotation was

300
250
200 Plenum Pressure

= 250 Pa
h ( W/m2 K)
150
Plenum Pressure
= 1050 Pa
100
50 (a)
0
0 50 100
ROTATION SPEED (RPM)
250
200
Plenum Pressure
= 250 Pa
150
h (W/m2K)
Plenum Pressure
= 1050 Pa
100
50
(b)
0
0 50 100
ROTATION SPEED (RPM)
FIGURE 24.13 Effect of bowl rotation on average heat transfer coefficient for (a) a model
cookie with 20 mm diameter with 10 mm thickness; (b) a model cookie with 50 mm diameter
with 10 mm thickness. The bars indicate the range of error.

TABLE 24.2
Heat Transfer Correlations at Different Jet Positions for a 50 mm
Aluminum Cookie
2
Jet Number Heat Transfer Correlation R
0.595
3 Un = 0.227 Re 0.942
0.387
7 Un = 2.077 Re 0.906
0.609
Between 3 and 7 (off center) Un = 0.210 Re 0.938
0.414
11 Un = 1.68 Re 0.978
observed at low plenum pressure (250 Pa) and low level of rotation speed (12 r/min).
The value of the average heat transfer coefficient experienced by the model cookie
at low plenum pressure and low rotational speed was lower than the value observed
without rotation for the same conditions. This result can be explained on the basis
of the existence of local maxima right under the jet. As the larger diameter cookie
spends a longer time under the jet as compared to the smaller cookie, h is not affected
by rotation in the case of the larger diameter cookie. Another plausible explanation
for this can be based on the response time of the model cookie. The smaller diameter
cookie has a smaller response time to the changes in h as compared to the larger
diameter cookie. Thus, the effect of rotation is observed in the smaller diameter
cookie as compared to the larger diameter model cookie.
The correlations for Nu as a function of Re were generated using SAS (SAS,
Inc., Cary, NC). The correlations are shown in Table 24.2. The correlations show a
power law dependence of Nu on Re with the exponent varying between 0.4 and 0.6.
Similar correlations have been reported (Martin, 1977) for single and multiple jets
impinging on a flat surface for the Reynolds number in the range of 2,000 to 120,000.
These correlations have a similar power law relation, and the range of the exponent
of Reynolds number was between 0.55 and 0.7. Thus, the correlations developed
for the cookie-shaped objects in a jet impingement oven were similar to those
developed over a flat surface.
24.4 CONCLUSIONS
The measured values of the average heat transfer coefficient were within the range
of values reported in the literature. The results indicated that the variation of the
average heat transfer coefficient under and between different jets was small. How-
ever, a local maximum in heat transfer under each jet was observed. This indicates
that a part of the cookie right under the jet will experience higher heat transfer than
the rest of the cookie. So, for cookies placed on a moving belt in an industrial
application, smaller cookies will experience more fluctuation in the heat transfer
coefficient as compared to larger cookies, depending on the size of the nozzle and
the spacing between the nozzles. This was confirmed by the rotation experiment in
which the smaller diameter cookie showed measurable variation in the h value as
compared to the larger diameter cookie under the same set-up.

NOMENCLATURE
D Diameter of the nozzle (m)
Cp Specific heat (J/kg K)
H Distance between the nozzle and the target plate (m)
To Temperature of the heating medium (K)
Ti Initial temperature of the model cookie (K)
Tt Temperature at the center of the cookie at any time t (K)
V Maximum jet velocity (m/sec)
2
h Average heat transfer coefficient (W/m K)
ka Thermal conductivity of air (W/m K)
m Mass of the cookie (kg)
r Radial distance (m)
t Time (sec)
uz Axial velocity (m/sec)
z Distance between the nozzle and target plate (m)
Nu Nusselt number (h D/ka)
Pr Prandtl number (Cp µ/ka)
Re Reynolds number (DVρ/µ)
3
ρ Density (kg/m )
µ Viscosity (Pa sec)
ACKNOWLEDGMENT
This work was supported by a grant (#9801317) from the U.S. Department of
Agriculture, under the National Research Initiative Competitive Grants Program.
REFERENCES
Gardon, R. and Akfirat, J.C., Heat Transfer Characteristics of Impinging Two-dimensional
Air Jets, ASME-HT-20, 1964.
Gardon, R. and Akfirat, J.C., The role of turbulence in determining the heat transfer charac-
teristics of impinging jets, Int. J. Heat Mass Transfer, 8, 1261–1272, 1965.
Gardon, R. and Cobonpue, J., Heat Transfer Between a Flat Plate and Jets of Air Impinging
on It, International Heat Transfer Conference, Part II, 1961, pp. 454–460.
Goldstein, R.J. and Seol, W.S., Heat transfer to a row of impinging circular air jets including
the effect of entrainment, Int. J. Heat Mass Transfer, 34, 2133–2147, 1991.
Huber, A.M. and Viskanta, R., Convective heat transfer to a confined impinging array of air
jets with spent air exits, ASME J. Heat Transfer, 116, 573, 1994.
Ichimiya, K. and Okuyama, K., Characteristics of Impingement Heat Transfer Caused by
Circular Jets with Confined Walls, Proceedings of the Third International Heat Trans-
fer Conference, 1980, pp. 523–532.
Lytle, D. and Webb, B.W., Air jet impingement heat transfer at low nozzle-plate spacings,
Int. J. Heat Mass Transfer, 37, 1687–1697, 1994.
Marcoft, H., Measurement of Velocity Distribution in a Jet Impingement Oven Using Laser
Doppler Anemometry, thesis, Rutgers University, New Brunswick, NJ, 1999.

Martin, H., Heat and mass transfer between impinging gas jets and solid surfaces, Adv. Heat
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Saad, N.R., Mujumdar, A.S., and Douglas, W.J.M., Heat transfer under multiple turbulent slot
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Van Dyke, M., An Album of Fluid Motion, The Parabolic Press, Stanford, CA, 1982.
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Future, Technical Bulletin, American Institute of Baking, 11, 1, 1989.

Flow Dynamics and Heat
25 Transfer in Helical
Heat Exchangers
P. Coronel and K.P. Sandeep
CONTENTS
25.1 Introduction
25.1.1 Dean Effect, Factors Affecting It, and Means
of Inducing Secondary Flow
25.1.2 Friction Factor
25.1.3 Laminar and Turbulent Flow
25.1.4 Residence Time Distribution (RTD)
25.1.5 Heat Transfer Coefficients
25.2 Experiments
25.3 Concluding Remarks
Nomenclature
References
25.1 INTRODUCTION
In an attempt to improve the rate of heat transfer and the uniformity of heating,
many novel types of heat exchangers have been manufactured. One such category
is helical heat exchangers (Figure 25.1). A variety of helical heat exchangers are in
use in the food industry; however, the underlying principle and hence the design
criteria are not well understood. This has resulted in much use of trial and error in
ascertaining the appropriate combination of system and process parameters for the
design of a process.
Once we understand the principle of mixing occurring in a helical tube, we can
design helical heat exchangers and holding tubes in a much more efficient manner,
which in turn will result in a much more uniform process from both a fluid mechanics
and a heat transfer standpoint. However, flow in coiled tubes is much more compli-
cated than in straight tubes, and hence the design of helical heat exchangers that
operate at a high efficiency is not straightforward. Several basic theoretical, numer-
ical, and experimental studies have been conducted in this area, and a summary of
these studies is presented here.

Inner Coil Outlet Outer Coil Outlet
Hot Water Outlet

Hot Water Inlet
Outer Coil Inlet Inner Coil Inlet
FIGURE 25.1 Schematic drawing of a helical heat exchanger.
25.1.1 DEAN EFFECT, FACTORS AFFECTING IT, AND MEANS

OF INDUCING SECONDARY FLOW
Just as flow and heat transfer in straight tubes are dependent on the Reynolds number,
the Dean number ( N De = N Re r / R , where r is the radius of the tube and R is the
radius of the helical coil) governs the type of flow and rate of heat transfer in curved
tubes. The Dean number is the ratio of the square root of the product of inertial and
centrifugal forces to the viscous forces. Since secondary flow is induced by centrifugal
forces, the magnitude of the Dean number is a measure of the extent of secondary
flow. It is also important to note that no secondary flow will be induced for an
inviscid fluid.
The secondary flow pattern arises due to the centrifugally induced pressure
gradient (a small but finite pressure gradient is required to balance the centrifugal
force), which is approximately uniform across the cross section, driving the slower

moving fluid near the wall inward and the faster moving fluid at the core outward.
The vortices are almost symmetrical and the stagnation points (or centers) are located
less than halfway from the center to the periphery. The region of maximum velocity
moves outward depending on the value of the Dean number. Beyond a certain value
of the Dean number, the double helical streamlined flow changes to turbulent flow.
For flow in curved pipes, the pressure increases monotonically from the inner
convex wall to the outer concave wall across any cross section due to the centrifugal
forces existing because of the curvature in the tube. However, the centrifugal force
first increases and then decreases as we move from the inner to outer wall after
attaining a maximum value along a line parallel to the horizontal axis.
Figure 25.2a shows the ideal secondary flow conditions in a helical tube. The
secondary flow field consists of a relatively inviscid core and a viscous boundary layer.
Inside Outside
(a)
Inside Outside
(b)
FIGURE 25.2 Secondary flow profiles in a helical tube showing (a) ideal and (b) free
convection at a low Reynolds number.

Inside Outside
(a)
Inside Outside
(b)
FIGURE 25.3 Axial velocity contours in a helical tube: (a) low Dean numbers; (b) high
Dean numbers.
Figure 25.2b shows the secondary flow in a helical tube at low Reynolds numbers
where free convection is a dominant factor and gravity, aided by density difference,
causes flow in the vertical direction. Similarly, Figure 25.3a shows the axial velocity
contour at low Dean numbers (where the contours are almost symmetrical), while
Figure 25.3b shows the asymmetric axial velocity contours at high Dean numbers.
The main factor affecting the extent of mixing taking place in a helical system
is the ratio of tube diameter to coil diameter. Other effects include particle flow rate
and concentration. Several other techniques (and their benefits) used by various
manufacturers are also described, for example, corrugated tubes and use of baffles.

The secondary flow phenomenon in curved pipes has received great attention
after Dean’s (1927, 1928) analysis of the problem. Dean (1927, 1928) and Dean and
Hurst (1959) investigated the flow in helically coiled circular tubes and reported that
a pair of symmetric vortices formed on the cross sectional plane due to centrifugal
force. Dean also obtained, by solving the Navier–Stokes equations, the equations of
motion for incompressible laminar flow in the case of small curvature ratios.
Taylor and Yarrow (1929) found that secondary flow could stabilize laminar
flow, providing transition Reynolds numbers as high as 6000 to 8000 in a curved
tube, as compared to 2100 in a straight tube, even when the inlet flow was turbulent.
Koutsky and Adler (1964) pointed out that the pressure drop in a tube formed into
a helix can be up to four times as great as that in an identical straight tube. They
also found that stable laminar flow can be maintained in helices at Reynolds numbers
up to 8000. Both of these facts imply the existence of strong secondary flow in
helices. Studies by Mori and Nakayama (1965), Patankar (1974), Kao (1987), and
Futagami and Aoyama (1988) showed that the presence of secondary flow could
increase the rate of momentum and mass and heat transfer.
For flow in a helical tube of square cross section, the centrifugal force causes a
secondary flow with a pair of counter-rotating vortices. For values of the Dean
number above the critical value, the secondary flow pattern has an additional pair
of vortices near the central outer region; this phenomenon is referred to as Dean’s
instability, and is known to increase the friction factor. Studies by Bara et al. (1992),
Cheng et al. (1976), and Kumar et al. (1989) reveal this phenomenon. This phenom-
enon is not, however, observed when the cross section of the pipe is inclined (Duh
and Shih, 1989). The instability phenomenon was observed by Masliyah (1980) in
semicircular tubes and by Nandakumar and Masliyah (1982) and Dennis and Ng
(1982) in circular tubes. Studies by Choi et al. (1979) suggested that there could be
several pairs of vortices in the entry section of a curved tube.
It is known that for a given pressure gradient, the flow rate in a coiled tube is
lower than that in a straight tube. Berger et al. (1983) presented the following
correlation to determine the nondimensional volumetric flow rate in a curved pipe:
2 4
˙
V  N 2De   N 2De 
c
= 1 − 0. 0306   + 0 .012   (25.1)
π R2 u  288   288 
where u is the average velocity in a straight pipe of the same radius under the same
axial pressure gradient.
The beneficial effects of secondary flow were made use of by Carlson (1991)
to develop helical heat exchangers that resulted in uniform heating of viscous fluids
and foods containing particulates. In addition to making use of the secondary flow,
Carlson placed baffles outside the pipes to increase the heat transfer coefficient on
the heating medium side by inducing turbulence.
Muguercia et al. (1993) measured the primary and secondary flow velocities of
water in a curved pipe using the Laser Doppler Anemometry technique. Maximum
secondary velocity was found to increase linearly with axial velocity. These research-
ers reported that the secondary flow is created by the centrifugal force, forcing the

fluid to move toward the outer wall. The fluid, after reaching the outer wall edges,
turns to the top or the bottom of the tube, making its way to the inner wall through
the region near the pipe wall. Also reported was that the two secondary flow vortices
were asymmetric due to the torsion effect of the coiled pipe geometry. Increasing
the Reynolds number from 1000 to 2500 caused the maximum dimensionless axial
velocity (ratio of maximum to mean axial velocity) to increase from 1.70 to 1.80.
Fluid elements in the high axial velocity region appeared to be pushed toward the
outer wall by centrifugal force.
The effect of pitch on primary and secondary flow in fully developed turbulent
flow through helically coiled pipes was studied numerically by Yang and Ebadian
(1994, 1995). These researchers showed that the secondary flow distorted the axial
flow and pushed the high axial flow region toward the outer wall. For the same pitch
and curvature ratio, torsion effect (a rotational force due to finite pitch) is much
larger in laminar flow than in turbulent flow as a result of the dominating centrifugal
force effect, due to much higher axial velocities in turbulent flow. These authors
observed that the two vortices formed across the pipe cross section were symmetric
for zero pitch. However, for a finite pitch, the torsion effect resulted in the loss of
symmetry of the two secondary flow vortices.
Fiedler (1997) presented a brief description of the effect of two consecutive bends
oriented in different planes on inducing swirl in the fluid flow field. Thomson et al.
(1998) studied low Dean number convective heat transfer in helical ducts of rectangular
cross section and found that torsion, which is known to increase friction factor, caused
a decrease in the fully developed Nusselt number compared to that in a pure toroidal
flow Hence, they recommended that torsion be minimized to enhance heat transfer.
25.1.2 FRICTION FACTOR

As a fluid flows through a tube, losses in energy (Ef) and pressure (Pf) due to friction
occur, determined as follows:
∆ Pf u2 L
Ef = = 2f (25.2)
ρ d
In the above equation, f is the friction factor, which varies with the type of pipe,
flow conditions, and system geometry. The friction factor for laminar flow in a
straight pipe is given by fs = 16/NRe and for turbulent flow is usually determined
from the Moody (1944) diagram. An alternative way to determine the friction factor
is to use the following equation by Colebrook (1939) to perform an iterative analysis:
1  1 ε 1.255 
= − 4 ln  +  (25.3)
f  3.7 d N Re f 
These are standard methods for determining friction factors in straight pipes.
However, for curved pipes, many additional factors, such as coil diameter, pitch,
and Dean number, come into play, and hence no standard formula or procedure is
available. Manlapaz and Churchill (1980) published a list of studies conducted for

the determination of friction factors in curved pipes. In the following section, a list
of other correlations developed based on various studies in curved pipes is presented.
White (1929) developed the following correlation to determine the friction factor
under laminar flow conditions:
−1
 0.45 2.2 
fc    11.6   
= 1 − 1 −  for 11.6 < NDe < 2000 (25.4)
fs    N De   
   
White (1932) extended the laminar flow study and developed the following
correlation to determine the friction factor for the case of turbulent flow:
fc = 0.08 N −Re0.25 + 0.012( r / R )0.5 for 15,000 < NRe < 100,000 (25.5)
Several other correlations have been developed for different flow conditions and
different geometries of holding tubes. In correlations such as the one listed below
(Yang and Chang, 1994) other parameters have been factored into the correlation:
fc
= 0.689 N 0De.0817 N 0Pr.0081 N 0Ra.0068 δ 0.084 (25.6)
fs
where δ = r/R, for 10 < NDe < 25,000, 0.7 < NPr < 100, 0 < NRa < 320, and 0.01 <
δ < 0.8.
25.1.3 LAMINAR AND TURBULENT FLOW

The flow behavior and heat transfer of fluids and particulates in pipes depends largely
on whether the flow is laminar or turbulent. Turbulent flow is generally associated
with high heat transfer, but so is the presence of secondary flow under laminar flow
conditions. Thus, it is important to characterize the type of flow occurring in pipes
under various situations. For flow in a straight pipe, laminar conditions are said to
prevail if the Reynolds number is less than 2100 or 2300. For curved pipes, the
presence of secondary flow stabilizes the flow pattern, and turbulence is delayed.
The results of some studies conducted to determine the critical value of the Reynolds
number that separates laminar and turbulent flow are given below.
White (1929) conducted experiments with oil and water for different curvatures
of helical tubes. For NRe > 100 and d/D = 1/50, a curved pipe had greater resistance
than a straight pipe of the same diameter and length. The resistance to flow was 2.9
times that in a straight pipe at NRe = 6000 (~NRe when flow becomes turbulent).
When d/D = 1/15, turbulent flow was seen at NRe ~ 9000, and when d/D = 1/2050,
turbulence was seen at NRe ~ 2250 to 3200. Several correlations (for example,
Equation (7), developed by Kutateladze and Borishanskii (1966)) have been devel-
oped to determine the critical Reynolds number:
N Rec = 2300 + 12930 ( r / R )0.3 for 0.0417 < d/D < 0.166 (25.7)

25.1.4 RESIDENCE TIME DISTRIBUTION (RTD)
Uniformity of heating is important when considering flow in tubes in the chemical,
food, pharmaceutical, and various other industries, as it relates to product quality, cost
of production, and other factors. As a Newtonian fluid flows through a straight pipe
under laminar flow conditions, a parabolic velocity profile develops. Thus, different
fluid elements take different times to pass through the pipe, and the distribution in the
time spent by various fluid elements in the pipe is referred to as the Residence Time
Distribution (RTD). RTD becomes narrower or broader in a tube depending on the
type of flow and type of fluid. In order to achieve uniform heating, a narrow RTD is
desired. Some methods for narrowing RTD are to induce turbulence or to use helical
pipes. The effect of helical pipes in narrowing RTD is described below.
Taylor (1953) described the process by which axial dispersion of a solute in a
helical tube was reduced by radial diffusion, which is now usually referred to as
Taylor dispersion. Radial mixing due to molecular diffusion is complemented by
convective secondary motions in a helical tube. Koutsky and Adler (1964) showed
that axial dispersion could be greatly reduced as compared to a straight tube when
the tube was formed into a helix. They found that this effect was more pronounced
in the turbulent region. The study also indicated that in a laminar flow regime, the
fluid elements on the secondary flow streamlines of smaller perimeter moved down-
stream more rapidly than those on larger streamlines. More narrow and peaked tracer
distributions were observed as a result of reduced axial dispersion, especially at high
Reynolds numbers. These researchers reported that the transition to turbulent flow
(3000 < NRe < 7000) was more gradual and occurred at higher Reynolds numbers
in helical tubes when compared to straight tubes. The strength of secondary flow at
low curvatures was diminished by the onset of turbulent flow, whereas at high
curvatures secondary flow was shown to be still effective in reducing the axial
dispersion even at higher Reynolds numbers. They also observed that the axial
dispersion in helical tubes in the Reynolds number range of 7,000–40,000 was
considerably less than that in laminar flow.
Saxena and Nigam (1984) studied the flow inversion in helical coils and utilized
the centrifugal force concept to develop secondary flow in laminar flow systems. They
reported that a 90° bend located midway in the coiled tube was more effective when
compared to 30, 45, and 60° bends in inducing secondary flow, thus narrowing the
RTD. They also found that increasing the number of bends (more than three) signifi-
cantly decreased the RTD. The study revealed that up to a Dean number (NDe) of 1.5,
the secondary flow was responsible for narrowing the RTD, whereas above 1.5, the
change in the direction of centrifugal force caused RTD narrowing by mixing the fluid
elements.
Mathematical modeling by Liu and Zuritz (1995) and Sandeep et al. (1995)
indicated that RTD in helical tubes was always narrower than the RTD in straight
tubes of similar lengths and diameters. Parametric analyses were conducted to
ascertain the effects of various system and process parameters for the cases of single
and two-phase flows.
Sandeep et al. (1997) found that the two counter-rotating vortices that developed
in the radial direction in the case of helical flow are responsible for mixing the fluid

elements and reducing the velocity gradient across the tube, which in turn results in
a decrease in the RTD. Residence time distribution in a helically coiled tube and a
chaotic system, where the tube was formed into an array of bends with the plane of
curvature of each bend making a 90° angle with that of the adjacent one, was studied
by Castelain et al. (1997) within the Reynolds number range of 800–13,500. These
authors reported that for Reynolds numbers higher than 2500, a chaotic system was
20% more effective in minimizing the axial dispersion than a helically coiled tube
having the same number of bends. They attributed this further improvement to the
chaotic trajectories resulting from the change in the plane of Dean vortices due to the
bends of the chaotic system. The two configurations were reported to be comparable
in terms of their axial dispersion effect for Reynolds numbers less than 2500.
25.1.5 HEAT TRANSFER COEFFICIENTS

Heat transfer for laminar flow in a straight tube (heat exchanger or holding tube) is
usually low since very little mixing in the radial direction occurs. However, flow in
a coiled tube is fully three-dimensional, and the rate of heat transfer can be much
higher than that in a straight tube. This is due to the development of secondary flow
(in the directions normal to the main direction of flow) due to the pressure gradient
imposed as a result of the centrifugal forces present in the curved section. The
secondary flow serves as a means of redistributing fluid elements in the radial
direction, thereby transferring heat more efficiently between the bulk of the fluid
and the fluid elements near the tube wall. Various studies have been conducted in
helical tubes to determine Nusselt number correlations under different flow and
system conditions in helical tubes, and some of those correlations are shown below.
Seban and McLaughlin (1963) developed the following equations to predict the
heat transfer coefficient under laminar and turbulent flow conditions:
Laminar flow:
1/ 3
f 
N Nu = 0.13 N1Pr/3  c N 2Re 
 8 
with fc being determined from White’s (1929) correlation.

Turbulent flow:
fc
N Nu = N N 0.4 with fc = 0.023 N −Re0.15 ( r / R ) 0.01
8 Re Pr
2
for NRe (r/R) > 6
The first order approximation for determination of the Nusselt number for flow
in a coiled tube developed by Mori and Nakayama (1965) is as follows:
N Nuc 0.1979 0.5

= N De (25.8)
N Nus z

where z is the ratio of the thickness of the thermal and velocity boundary layer and
is given by:
2   
0.5
77 
z = 1 + 1 +   for NPr ≥ 1 and
11   4 N 2Pr 
 
(25.9)
1   10 
0.5

z= 2 +  2 − 1  for NPr ≤ 1
5   N Pr  

Ozisik and Topakoglu (1968) developed the following expression for Nusselt
number in a curved pipe:
−1
48  V˙ 2  C1 r 2 
N Nu = ˙  1 − R 2 
c
(25.10)
11  Vs
where
1  C2  C2  6.95513 N 2Pr   
C1 = −71.6 + 165.47 + 7 N Pr +  9.96576 +  
264  112  2.8  1.1   
2
C2 = NRe /36 and
˙
V r 2  1.541 C 22 
˙
c
= 1 − 2 
+ 1.1 C 2 − 1 (25.11)
Vs 48 R  67.2 
with V̇c and V̇s being the mass flow rates in the curved and straight tubes, respectively.
Dravid et al. (1971) conducted numerical studies for flow in a helical tube for
small aspect ratios and for the case where axial conduction is negligible in compar-
ison with axial convection (NPe > 20). They developed the following correlation for
heat transfer coefficient at distances close to the inlet of the tube:
N Nuc
= 0.447N1De/ 6 (25.12)
N Nus
At NDe = 125, the heat transfer coefficient in the helical tube is the same as that in
the straight tube. It should not, however, be inferred that for lower values of the Dean
number the heat transfer coefficient is higher in the straight tube, since at short distances
from the inlet the temperature field does not significantly penetrate the secondary flow
field. Based on their experimental study, Dravid et al. (1971) developed the following
correlation for the asymptotic Nusselt numbers applicable for 50 < NDe < 2000 and
5 < NPr < 175:
[
N Nu = 0.76 + 0.65 N De N 0Pr.175 ] (25.13)

The asymptotic Nusselt numbers for the straight tube case are 3.66 for the case
of constant wall temperature and 4.36 for the case of constant wall heat flux. These
values are significantly higher for the helical tube case.
Oliver and Asghar (1976) developed the following Nusselt number correlation
for flow in a helical coil:
0.14
µ 
N Nu  w 
 µb 
= 1.75 N Gz
0.13
(
1 + 0.36 N 0De.25 ) for 4 < NDe < 60 (25.14)
0.14
µ 
N Nu  w 
 µb 
= 1.75 N Gz
0.13
(
1 + 0.118 N 0De.5 ) for 60 < NDe < 2000 (25.15)
Janssen and Hoogendoorn (1978) developed the following Nusselt number cor-
relations for different ranges of Dean numbers:
( ) ( )
1/ 6
N Nu = 1.7 N 2De N Pr for NDe < 20 and N 2De N Pr 0.5 > 100 (25.16)
( )
1/ 6
N Nu = 0.9 N 2Re N Pr for 20 < NDe < 100 (25.17)
N Nu = 0.7 N 0Re.43 N1Pr/6 ( r / R ) 0.07 for 100 < NDe < 8300 (25.18)
These researchers concluded that the effect of d/D can be neglected for Dean
numbers less than 100 in the fully developed thermal region. They also found that for
( )
all cases with N 2De N Pr > 100, the Nusselt number in the fully developed thermal re-
gion was proportional to N1Pr/6 and that for the thermal entry region, the Nusselt number
was proportional to N1Pr/3 .
Abul-Hamayel and Bell (1979) conducted experimental studies of heating of
ethylene glycol, distilled water, and butyl alcohol in a helical coil with D/d = 20.2
and developed the following Nusselt number correlation:
  N Gr  
3.94
N Nu
  N Re  
[
= 4.36 + 2.84 2   1 + 0.0276 N 0De.75 N 0Pr.197 ]
(25.19)
2.78 −1.33 N Gr
  N Gr    µ  0.14
N 2De
× 1 + 0.9348 2  e  b 
  N De    µ b 
6
for 92 < NRe < 5500, 2.2 < NPr < 101, and 760 < NGr < 10 .

In the above equation, the quantities in the first, second, third, and fourth brackets
are the expressions for flow in a straight tube, secondary flow contribution, natural
convection contribution, and viscosity correction factor, respectively.
Yang and Chang (1994) developed the following Nusselt number correlation as
a function of Dean number, Prandtl number, Rayleigh number, and curvature:
N Nuc
= 0.42 N 0De.111 N 0Pr.21 N 0Ra.0513 δ − 0.0974 (25.20)
N Nus
where δ = r/R, for 10 < NDe < 25,000, 0.7 < NPr < 100, 0 < NRa < 320, and 0.01 < δ < 0.8.
Thus, it can be seen that different correlations have been developed for different
flow conditions and different tube geometries. It is thus important to look into the range
of applicability of various correlations before applying them to different situations.
25.2 EXPERIMENTS
In order to compare heat transfer coefficients in straight and helical heat exchangers,
we conducted studies using both configurations. The helical heat exchanger used was
a Multicoil heat exchanger (VRC Co., Inc., Cedar Rapids, IA). The Multicoil heat
exchanger (Figure 25.4) consists of a shell within which two coils of tubes (inner coil
and outer coil) are situated. The heating medium (pressurized water) flows in the shell
at a very high flow rate and recirculates through the system while the product flows
inside the coiled tube(s). Baffles present outside the coils increase the turbulence of
the heating medium and thus enhance the outside heat transfer coefficient. Either one
or both of the coils can be used, and they can be connected in a series or parallel
configuration. A shell and tube heat exchanger that utilizes steam and has an automatic
control system to maintain a desired temperature is used to provide the hot water to
heat the product. The temperature and pressure of both the product and heating medium
are monitored at various locations within the system. The outer shell of the Multicoil
heat exchanger is insulated to minimize heat loss to the surroundings.
City water was used as the test fluid, and the properties of water (thermal conduc-
tivity, density, and specific heat) were calculated using correlations (Popiel and Wojt-
kowiak, 1998). The first set of experiments involved pumping the product using a
piston pump (Model 629A, Marlen Research Corp., Overland Park, KS) through the
system (Multicoil heat exchanger, holding tube, and four tubular coolers) at different
flow rates (0.19–0.63 kg/sec) and at different set point temperatures (100–150°C). The
first two tubular cooling units utilized city water as the cooling medium, while the
third and fourth coolers utilized a 30% propylene glycol solution. Temperatures of the
product and heating medium were monitored at various locations within the system
using type-T thermocouples and recorded in a data acquisition system using the
software PC208W (Model CR10, Campbell Scientific, Inc., Logan, UT). The volu-
metric flow rate of the heating medium was measured using an external flowmeter
(Model 1010WP1, Controlotron, Inc, Hauppauge, NY), and the volumetric flow rate
of the product was determined by noting the time taken by the product to fill a

FIGURE 25.4 Schematic representation of the Multicoil heat exchanger.
container of known volume. The specifications of the experimental set-up are given
in Table 25.1. The holding tube and tubular cooling units did not have any insulation
on the outside.
The Multicoil heat exchanger is similar to a countercurrent heat exchanger and was
modeled as a countercurrent heat exchanger for calculation purposes. Based on the

TABLE 25.1
Specifications of the Experimental Set-Up
Multicoil Heat Exchanger

Total length of outer coil of Multicoil heat exchanger = 39.6 m
Diameter of outer coil of Multicoil heat exchanger = 0.3 m
a
I.D. of pipe of Multicoil heat exchanger = 0.01 m
b
O.D. of pipe of Multicoil heat exchanger = 0.013 m
Thermal conductivity of the material of the pipe = 16 W/m-K
Holding Tube
Length of holding tube = 48.8 m
a
I.D. of holding tube = 0.023
Tubular Coolers
Length of each of the four coolers = 6.1 m
a
I.D. of the inner pipe = 0.023 m
b
O.D. of the inner pipe = 0.025 m
a
I.D. of the outer pipe = 0.048 m
b
O.D. of the outer pipe = 0.05 m
Thermal conductivity of the material of the pipe = 16 W/m-K
a
I.D. = inside dimension.
b
O.D. = outside dimension.
recorded temperatures and flow rates, the overall heat transfer coefficient in the
Multicoil heat exchanger and the tubular coolers were determined using the following
equations:
˙ =m
Q ˙ c p ∆T
(25.21)
˙ = U A ∆T
Q lm lm
where Q̇ is the energy gained by the product.

The results of the calculations are summarized in Figure 25.5. It can be seen
from this figure that the overall heat transfer coefficient was always higher (more
than double) in the Multicoil heat exchanger than in the tubular coolers. Based on
the limited experimental runs, there does not seem to be any effect of set point
temperature on the overall heat transfer coefficient.
The next study was conducted with the objective of determining the effect of
the diameter of the helical coil on the overall heat transfer coefficient. In order to
determine this, we conducted experiments with water as the product and pumped it
through both the inner and outer coils separately, but at the same flow rate. A similar
analysis to the one performed above was carried out to determine the overall heat

10.0
9.0
8.0
7.0
U (W/m2-K)
6.0
5.0
4.0
3.0
2.0
1.0
3 4 5 6 7 8 9 10
Flow rate (gpm)
Outer, 93 °C Outer, 121 °C Outer, 149 °C Straight tube
FIGURE 25.5 Overall heat transfer coefficient in helical and straight heat exchangers.
11,000
10,000
9,000
8,000
U (W/m2-K)
7,000
6,000
5,000
4,000
3,000
2,000
1,000
2.5 3.5 4.5 5.5 6.5 7.5 8.5 9.5
Flow Rate (gpm)
Inner 93 Outer 93
FIGURE 25.6 Overall heat transfer coefficient in the inner and outer coils of the Multicoil
heat exchanger.
transfer coefficient. The results of the calculations are summarized in Figure 25.6.
It can be seen from this figure that the overall heat transfer coefficient was always
higher in the coil of smaller radius than in the coil of larger radius.
Another study was conducted to directly compare the amount of energy trans-
ferred in the Multicoil heat exchanger and in tubular coolers. In order to perform
this, the product (water) was pumped through the same system as described above
at a specific flow rate (0.26 kg/sec) and a specific set point temperature (121°C)
through one of the coils (outer coil), with hot water flowing through the system at
10.25 kg/sec. The mass flow rates of city water in the first and second coolers were

TABLE 25.2
Comparison of Tubular and Multicoil Heat Exchangers (at 0.26 kg/sec)

Energy gained by product = 118,244 W
2
Overall heat transfer coefficient = 3,889 W/m -K
Cooler #1
Energy lost by product = 66,989 W
2
Cooler #2
2
Cooler #3
2
Overall heat transfer coefficient = 901 W/m -K
Cooler #4
Energy lost by product = 7950 W
2
a
Net gain in energy based on the inlet and exit temperatures of the product = 6441 W
a
Net gain in energy based on energy gained in heater and energy lost in coolers = 7438 W
a
The difference in the above two values is due to experimental errors and the fact that we neglected
heat loss in the holding tube.
1.58 and 0.94 kg/sec, respectively, while the mass flow rates of glycol in the third
and fourth coolers were 0.74 and 0.47 kg/sec, respectively. The results of the
experiments are summarized in Table 25.2. A similar experiment was conducted
at a product flow rate of 8.16 g/min. The only other change in the experimental
conditions was that the mass flow rate of city water in the first cooler was 1.71 instead
of 1.58 kg/sec. The results of this experiment are summarized in Table 25.3.
From Tables 25.2 and 25.3 it can be seen that the energy transferred in the
Multicoil heat exchanger was much higher than that transferred in each of the coolers.
This is further seen from the fact that the overall heat transfer coefficient in the
Multicoil heat exchanger was much higher than that in any of the coolers. This is
due to two factors:
1. The outside heat transfer coefficient was much higher in the Multicoil
heat exchanger due to the high flow rate of the heating medium and the
presence of the baffles.
2. The high inside heat transfer coefficient in the Multicoil heat exchanger
was due to the development of secondary flow.

TABLE 25.3
Comparison of Tubular and Multicoil Heat Exchangers (at 0.52 kg/sec)

Energy gained by product = 235,857 W
2
Cooler #1
2
Cooler #2
2
Cooler #3
2
Cooler #4
2
a
Net gain in energy based on the inlet and exit temperatures of the product = 47,006 W
a
Net gain in energy based on energy gained in heater and energy lost in coolers = 45,098 W
a
The difference in the above two values is due to experimental errors and the fact that we neglected
heat loss in the holding tube.
25.3 CONCLUDING REMARKS

Numerous studies have been conducted on secondary flow in helical tubes in order to
either understand the fundamental principles of flow and heat transfer in coils or to
determine friction factors, pressure drops, extent of secondary flow, axial dispersion
coefficient, critical Reynolds number, or Nusselt number, and how various system
and process parameters affect them. However, there is no standard correlation or
law that can be applied to all scenarios of helical tube flow (unlike in straight tubes);
hence, readers are cautioned to carefully review the conditions under which the
equations are applicable.
Based on the experiments conducted in the Multicoil heat exchanger and tubular
cooling units, it can be seen that the overall heat transfer coefficient in the Multicoil
heat exchanger is much higher than that in the tubular coolers. It was also seen that
the smaller the radius of the coil of the heat exchanger, the higher the heat transfer
coefficient. However, it should be noted that the pressure drop in a coil of smaller
radius is higher than that in a coil of larger radius. In conclusion, it is noted that the
use of helical heat exchangers can result in rapid and relatively uniform processing
of a product, thereby resulting in a high quality product.

NOMENCLATURE
2
A Area, m
cp Specific heat, J/kg-K
C1, C2 Constants
d Diameter of tube, m
dp Particle diameter, m
D Coil diameter, m
Dvertical Vertical dimension, m
Ef Energy loss due to friction, J/kg
f Friction factor
2
g Acceleration due to gravity, m/sec
2
h Convective heat transfer coefficient, W/m -K
k Thermal conductivity, W/m-K
L Length of pipe, m
ṁ Mass flow rate, kg/sec
NDe Dean number N De = N Re r / R
βf g ρf (Tsurface − T∞ ) D3vertical
NGr Grashof number N Gr =
µ 2f
N Re N Pr
NGz Graetz number N Gz =
x/D
hD
NNu Nusselt number N Nu =
kf
NPe Peclet number NPe = (NRe)(NPr)
C Pf µ f
NPr Prandtl number N Pr =
kf
NRa Rayleigh number NRa = (NGr)(NPr)
ρf uD
NRe Reynolds number N Re =
µr
N Rec Critical Reynolds number
Q̇ Energy transferred per unit time, W

r Radius of tube, m
R Radius of helical coil, m
T Temperature, K
Tsurface Surface temperature, K
T∞ Bulk fluid temperature, K
u Average velocity, m/sec
2
U Overall heat transfer coefficient, W/m -K
3
V̇ Volumetric flow rate, m /sec
x Distance from entrance, m
z Ratio of thickness of thermal to velocity boundary layer

SUBSCRIPTS
b Bulk fluid temperature
c Coiled (or helical) tube
f Fluid
lm Logarithmic mean
p Particle
s Straight tube
w Wall temperature
GREEK SYMBOLS
−1
β Coefficient of volumetric thermal expansion, K
δ Dimensionless curvature
∆Pf Pressure loss due to friction, Pa
∆T Change in temperature, K
µ Viscosity, Pa-sec
3
ρ Density, kg/m
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Relating Food Frying to
26 Daily Oil Abuse. Part I.
Determination of Surface
Heat Transfer Coefficients
with Metal Balls
CONTENTS
26.1 Introduction
26.4 Conclusions
Nomenclature
Acknowledgments
References
26.1 INTRODUCTION
During immersion frying, convective heat transfer occurs at the food–oil interface
(Singh, 1995; Sahin et al., 1999; Costa et al., 1999). The mode of heat/mass transfer
in deep fat frying is rather complex because it is difficult to precisely define and/or
quantify the vigorous movement of water vapor bubbles escaping at the food surface.
An added complication is that the thermophysical properties of the food material
continually change due to moisture depletion and temperature change (Costa et al.,
1999; Hallstrom et al., 1988). Data on the convective surface heat transfer coefficients
(h values) obtained during food frying through the use of metal transducers, food, and
model foods have been reported in the literature (Sahin et al., 1999; Costa et al., 1999;
Pannu and Chinnan, 1999; Dincer, 1996; Miller et al., 1994). Selected results are
presented in Table 26.1 to show the large range that exists for these reported results.
For the development of predictive models, it is usually assumed that the h value
is constant during immersion frying. Comprehensive mathematical models were
developed by Farkas et al. (1996a, b) and Farid and Chen (1998) to quantify heat

TABLE 26.1
Some Reported h Value Data Obtained for Food Frying
2
h Value (W/m °C) Temp. (°°C) Material/Shape Source
~110 140–160 Potato/finite cylinder Pannu and Chinnan (1999)

90–200 150–190 Model food/finite slab Sahin et al. (1999)
250–300 170–190 Metal/sphere Miller et al. (1994)
250–600 140–180 Potato/French fry Costa et al. (1999)
300–650 140–180 Metal/French fry Costa et al. (1999)
a
~14 180 Potato/long cylinder Dincer (1996)
a
Heat and mass transfer have been decoupled; h-value is only for heating.
and mass transfer during food frying. Large variations in h value data obtained
during frying, with food vs. without food, have led researchers to use two h values
for the development of predictive models (Farkas, 1996a; Costa et al., 1999). One
h value is used in the absence of bubbling and another for the bubbling phase. It is
also assumed that a nonbubbling phase is followed by an enhanced bubbling phase,
and that at the end there is reduced bubbling as less moisture is evaporated. However,
this is not true when commercially prepared frozen foods are deep fried. Under such
conditions there is an instantaneous condition of high turbulence or, more specifi-
cally, forced convection conditions are created as the surface ice melts, producing
a vigorous bubbling action.
Costa et al. (1997) also reported that the bubbling action increases to a maximum
value prior to decreasing, and this can be related to the water loss rate. Thus, bubbling
may be expected to have an influence on h values. In the absence of bubbling, h
value data reported in the literature, and obtained through the use of metal trans-
2
ducers, range between 220 and 300 W/m °C (Miller, et al., 1994; Tseng et al., 1996;
Pannu and Chinnan, 1999). Fellows (1996) provided similar data for the nonbubbling
2
phase, along with h values of 800 to 1000 W/m °C for the surface boiling conditions.
Based on product surface temperatures, Hubart and Farkas (1998) predicted that for
2
frying at 180°C, the h value started at 300 W/m °C, increased to a maximum value
2 2
of 1100 W/m °C and then decreased to below 200 W/m °C after 900 sec of frying.
Pannu and Chinnan (1999) conducted a heat transfer study by heating finite potato
cylinders (with a diameter and length of 2.54 cm) in hot oil at 70 and 90°C (no
moisture loss) and compared these results with those obtained during frying at
160°C. Their results show that the heating rate index values obtained at the food
center and the mid-plane (between center and surface) were identical for the first
two cases. In addition, similar values were obtained under frying conditions for the
first 120 sec at the mid-plane and for 200 sec at the food center. Based on these and
additional data for moisture loss, the h value was computed to range between 100
2
and 130 W/m °C. These values are similar to those reported by Sahin et al. (1999),
2
but lower than the h value of about 250 W/m °C obtained with metal transducers.
Additional details on methods that can be employed to obtain a value for the overall

convective surface heat transfer coefficient (U) from moisture loss data are provided
in Part 2 of our study (Pannu and Chinnan, Chap. 27, this volume).
Sahin et al. (1999) used a model food made from aluminum wool and mashed
potatoes to conduct their study. Thin square slabs (0.3 × 5 × 5 cm) were vertically
suspended in hot oil to minimize the variability of h values on product geometry.
In essence, h values were determined by solving the conduction equation after
compiling a database on transducer moisture loss and product temperature as a
function of time, and by varying the thermal properties as a function of temperature
and moisture. The h values obtained by Sahin et al. (1999) show a stepwise increase
2
from 90 to 200 W/m °C as oil temperature increased from 150 to 190°C.
In comparison, Costa et al. (1999) reported that h values are time dependent.
Data with metal transducers show that h values peak 10 to 40 sec after frying begins
and thereafter start to decline. For potato crisps the peak occurs before that for
French fries, and the peak also occurs earlier as the frying oil temperature increases,
indicating that h values are tied to the moisture evaporation characteristics. Essen-
tially, the peak is related to the high moisture evaporation regions because higher
moisture loss rates induce more bubbling and provide higher h values. Thus, peak
h values occur shortly after immersion for the thin potato crisps. This suggests that
frozen foods should provide the highest h value immediately after they are immersed
into the hot oil. The experimental data of Costa et al. (1999) showed peak h values
2 2
of about 750 W/m °C (after 15 sec of frying) and 650 W/m °C (after 35 sec of
frying) for crisps and French fries, respectively, at a frying temperature of 180°C.
However, the peak h value measured directly from French fries at a processing
2
temperature of 140°C was about 600 W/m °C and higher than the value of 440
2
W/m °C obtained with the metal transducer.
Data in the literature suggest that the oil viscosity, heat capacity, and surface
tension are the primary physical properties that may influence the product heating
rate (Blumenthal, 1991; Miller et al., 1994). Blumenthal (1991) outlines the surfac-
tant theory and suggests that the heat transfer rate from oil to food can change as
the oil quality degrades through use. It is clearly stated that during food frying heat
is transferred from the nonaqueous medium (oil) into the mostly aqueous medium
(food). Thus, during food frying there is an oil–water interface that does not exist
when metal transducers are used to ascertain the h value. Therefore, metal transduc-
ers may not register changes in h values due to the buildup of surfactants. This is
supported by results presented by Tseng et al. (1996), who showed that the h value
is not affected until the oil discard point is reached. Surfactants should be regarded
as wetting agents that increase the contact time between oil and food (Blumenthal,
1991) through the oil–water interface. Therefore, excessive darkening and drying at
the food surface as a result of oil breakdown may be related to the above phenomenon
and not to h values obtained with metal transducers.
Parameters commonly used to define discard point are foaming due to buildup
of surfactants, oil color, smoke point, dielectric properties, free fatty acid (FFA)
levels, and total polar compounds. The first three are visual parameters and probably
the ones most commonly used. Miller et al. (1994) used h value data to study the
influence of temperature and oil type on oil use (abuse) and found that the major
effect was due to viscosity. However, the differences in h values were rather small.

Further, although the transient heating equations indicate that h values for heating
and cooling should be similar, no comparative data are available.
The objectives related to this part of our research were to estimate h values with
metal balls in a range of food frying conditions. Specific objectives were to: determine
h value without food; compare h value data for heating vs. cooling in the same
temperature range; determine h value during the frying of commercial grade frozen
French fries (par-fries) and breaded chicken fillets; observe the influence of loading
condition (less food vs. more food); and study the influence of oil abuse on h value data.

A schematic of the equipment and tools required to conduct this research is presented
in Figure 26.1. Although the picture shows one metal ball suspended in the pot fryer,
four metal balls were simultaneously immersed into the hot (or cold) oil to obtain
the time–temperature data. A fine wire (36 gauge, type K) thermocouple was posi-
tioned at the geometric center of each ball. To accomplish this task, a 0.8-mm hole
was drilled into each ball in the central axis up to a depth equivalent to half the ball
diameter. Omegabond 200 (Omega Engineering Inc., Stamford, CT), a high temper-
ature, high thermal conductivity epoxy cement, was used to bond the thermocouples
in place.
The diameter of the small aluminum and stainless steel balls used in this study
was 1.27 cm (0.5 inch), and the large balls had a diameter of 2.54 cm (1.0 inch).
The four balls were suspended on a frame to facilitate their simultaneous immersion
into the frying medium and were identified as Al- 1 2 , SS- 1 2 , Al-1 and SS-1
(Figure 26.2), with 1 2 and 1 indicating ball diameters of 1.27 cm and 2.54 cm,
respectively. The fifth thermocouple used to measure the oil temperature was also
attached to the frame and positioned at the same height as the balls. Kitchen pot
fryers (3.5 l capacity) were employed for this study, and commercial grade hydro-
genated soybean oil was used as the food frying medium.
Commercial grade, frozen (for the food service sector) breaded uncooked
chicken fillets (~85 g of breast meat) and par-fries (1-cm thick French fries) were
used. A 1:7.5 food-to-oil ratio was used, i.e., ~340 g of food were fried in 2.6 kg
Pot Fryer
Thermocouple wire:
Type K - 36 gauge
Metal ball
FIGURE 26.1 Schematic of “tools” used to conduct the frying study.

200 00 40 80 120
Oil
Al-1/2
150 Al-1 SS-1 -1
SS-1
SS-1/2
Temp. (C)
Ln (T. R.)
-2 Al-1
Abused Oil
50 FFA > 1.5 -3
SS-1/2
Al-1/2
0 -4
0 20 40 Time (sec) 80 100 120 Time (sec)
FIGURE 26.2 Typical temperature data registered by the metal balls during heating in oil at
190°C. Data in the right graph were used to obtain h value data. (Al and SS refer to aluminum
and stainless steel, respectively; suffix 1 2 or 1 refers to the metal ball diameter in inches.)
of oil. Food batches were fried every 20 min at a temperature of 180°C for 5 min
(cook cycle) followed by drain/cool for 5 min (Table 26.2). The 10 min gap between
batches provided time for preparation of the next batch and permitted the pot fryers
to return to the initial set temperature. Twenty food batches were fried daily over a
7.5 h period, and make-up oil was added after 10 batches had been fried. At the end
of each day, the frying oil was filtered to remove debris and charred materials, and
make-up oil was added to maintain the 2.6 kg level after a 50 ml oil sample was
removed for analysis (Table 26.2).
Days 1, 4, and 7 were chosen to conduct the variable food mass study using six
batches of French fries and 14 batches of chicken fillets. The frying protocol for the
variable food mass study is detailed in Part 2 (Pannu and Chinnan, Chap. 27, this
volume). On days 2, 3, 5, 6, and 8, two batches of French fries and 18 batches of
chicken fillets were fried, as shown in Table 26.2. The overall mass of food fried
each day was approximately 6.7 kg, with the normal loading condition defined as
340 g of French fries or four chicken fillets.
For a few experiments, chicken fillet and French fry pieces were instrumented to
obtain temperature profiles. Fine wire (36 gauge, type K) thermocouples were posi-
tioned at the geometric center of a 7-cm French fry and a chicken fillet. Thermocouples
were also inserted close to the food surface. Food surface for the chicken fillet repre-
sented the top part of the breading layer. The instrumented French fry was placed on
top of the four chicken fillet pieces and subsequently processed in 180°C oil.
Experiments with metal balls were conducted at varying intervals to cover the
8-day test period. Temperature data from the metal balls were recorded at 0.5 sec
intervals. The exterior food temperature data were recorded prior to the commence-
ment of food frying, i.e., in between batches. The experiments with food were
conducted by immersing the metal transducers 60 to 90 sec after commencement
of food frying. A time delay was employed for safety reasons because of enhanced
bubbling and oil splattering at the commencement of frying due to ice melt conditions.

TABLE 26.2
Example of Experimental Protocol Used in Frying Studies
File Name: ABC-2 Frying Cycle 2 of 8 days Date: April 30, 1999
Weight of Empty Fryer: 1.612 kg Weight of Oil: 2.615 kg
Batch # Time Food (g) Product Batch # Time Food (g) Product
1 9:00 325.6 CH-4 11 13:20 356.8 CH-4

2 9:20 332.8 CH-4 12 13:40 308.5 CH-4
3 9:40 348.3 CH-4 13 14:00 310.7 CH-4
4 10:00 340.7 CH-4 14 14:20 313.3 CH-4
5 10:20 310.2 CH-4 15 14:40 313.9 CH-4
6 10:40 319.9 CH-4 16 15:00 340.5 CH-4
7 11:00 313.2 CH-4 17 15:20 351.4 CH-4
8 11:20 350.4 CH-4 18 15:40 324.8 CH-4
9 11:40 350.6 FF 19 16:00 344.4 FF
10 12:00 346.5 CH-4 20 16:20 407.3 CH-4
TOTAL W1 = 3338.2 TOTAL W2 = 3371.6
Note: FF: French fries; CH, chicken.

1) Weight of fryer + oil + basket: 4440 g at start
2) Weight of fryer + oil + basket: 4412 g at noon
a) Oil loss = 1–2 28 g
3) Weight of fryer + oil + basket: 4440 g after oil addition
4) Weight of fryer + oil + basket: 4415 g at end
b) Oil loss = 1–2 25 g
c) Total oil loss = a + b 53 g
d) Total food fried = W1+W2 6710 g
Note: Frying basket weight = 4440 – (1612 + 2615) = 213 g
In addition, when 340 g of frozen food are rapidly immersed in hot oil, very unstable
processing conditions exist in the beginning, resulting in a rapid drop in oil temper-
ature. Such conditions make it difficult to obtain accurate time–temperature data
during the first 60 sec of frying.
Further, the metal balls were immersed in cold oil (room temperature) at all
times when not in use. This was done to ensure that the balls had a uniform initial
temperature. Thus, for the cooling experiments, the balls were returned to the cold
oil reservior (also 2.6 kg of oil) after the balls had attained steady temperature in
the heating cycle. Time–temperature data for this study were recorded using the HP-
34970 (Hewlett Packard, Palo Alto, CA) data acquisition unit. The natural logarithm
(ln) of the dimensionless temperature ratio was plotted against time to provide a
value for the inverse slope and used to determine h value by the lumped capacity
method. Equation (26.1) was used to compute h values from temperatures registered
at the geometric center of the metal balls. The terms A, ρ, Cp and V represent the
solid surface area, density, specific heat, and volume, respectively. Subscripts for

temperature (T) listed as a, i, and (t) denote ambient (oil), initial (metal ball), and
the variable time-dependent temperature (metal ball), respectively.
Ta − T( t ) −(hA/ρCpV)t
= T. R. = θBall = e (26.1)
Ta − Ti
Thermal property data for ρ and Cp used to estimate the h values were (Holman,
1976):
3
ρStainless steel = 7897 kg/m CpStainless steel = 452 J/kg°C
3
ρAluminum = 2707 kg/m Cp Aluminum = 896 J/kg°C

Typical time–temperature data obtained during the heating of metal balls in oil are
shown in Figure 26.2. The graph on the right shows that there were no lag factors,
and straight lines were obtained when the natural logarithm of the dimensionless
temperature ratio was plotted vs. time. The data presented also show that the smaller
metal balls heated faster and that aluminum balls registered accelerated heating in
comparison to stainless steel balls.
Table 26.3 summarizes the data for h values obtained under free convection heating
conditions. The results show that transducer material and ball diameter do not appear to
appreciably influence the h value data. However, if average values are considered, the
2
large and small balls provide mean h values of 230 and 250 W/m °C, respectively. These
results are similar to those reported by Miller et al. (1994). The low Biot numbers
(Bi = h R/k) of 0.015 and 0.06 obtained for the large aluminum and stainless steel balls,
with thermal conductivity, k, of 204 and 50 W/m°C, respectively, indicate minimal
internal resistance to heat transfer and justify the use of the lumped capacity approach.
Results presented in Table 26.3 also show that the h values are not influenced by oil abuse,
as FFA values increased from a low of 0.05 (fresh oil) to a high of 1.55 on day 8.
TABLE 26.3
Comparison of h Value Data for Fresh vs. Used Frying
Oil (Free Convection)
2
h Value (W/m °C)
Day FFA Temp. (°°C) Al- 1 2 SS- 1 2 Al-1 SS-1
1 <0.05 185 220 250 220 215

2 0.22 190 270 255 245 230
4 0.67 180 235 275 245 225
6 1.10 185 260 250 230 220
8 1.55 185 230 250 240 225
Note: FFA: Free fatty acids

The surfactant theory should not be questioned, since metal balls cannot be compared
to food pieces as they do not have an oil–water interface. Indeed, the surfactant theory
results correctly predicted food surface color darkening through increased oil use/abuse.
Heating/cooling characteristics similar to those outlined above are depicted in
Figure 26.3. However, a visual comparison of the log-normal temperature data shows
that h values during cooling were lower than for heating (steeper slopes), and this
is validated by results detailed in Table 26.4.
TABLE 26.4
Comparison of h Value Data for Heating
vs. Cooling (Free Convection)
2
h Value (W/m °C)
Temperature (°°C) Heating Cooling
Cold Heat Cool Al-1 SS-1 Al-1 SS-1
22 135 22 185 180 150 160

25 150 25 200 195 160 165
26 175 26 235 225 170 185
30 180 30 220 215 175 185
27 192 27 235 230 185 195
Heating Cooling
200
Temperature (C)
SS-1/2
150
Al-1/2 Al-1 Al-1
SS-1
100
SS-1
Fresh Oil Al-1/2
50 SS-1/2
FFA < 0.1
0
0 20 40 60 80 100 120 0 20 40 60 80 100
0
SS-1
SS-1 -1
Ln(T.R.)
Al-1/2 Al-1
SS-1/2
Al-1/2 Al-1 -2
SS-1/2
-3
-4
FIGURE 26.3 Temperature data comparing heating vs. cooling conditions. (Al and SS refer to
aluminum and stainless steel, respectively; suffix 1 2 or 1 refers to the metal ball diameter in
inches.)

TABLE 26.5
h Value Data without Food and during Frying with Food
2
h Value (W/m °C)
a
Condition Temp. (°°C) Time (sec) Al- 1 2 SS- 1 2 Al-1 SS-1
No food 185 — 220 250 220 215

CH, 4 pieces 185 90 400 345 340 405
CH, 4 pieces 185 60 550 510 480 440
FF, 340 g 185 60 1070 885 780 450
FF, 340 g 185 60 960 850 725 620
Note:CH: chicken fillet; FF: French fries.

a
Time after commencement of food frying.
HEATING
COOLING
FIGURE 26.4 A pictorial representation of the plume effect.
Figure 26.4 is a pictorial representation of what probably occurs during heating

and cooling. During heating, density differentials force the oil plume to move down-
wards, and there is a negligible impact on the heating rate, whereas during cooling
hot oil begins to move upward. As cooling occurs due to oil mixing, a shroud is created
around the hot ball, and the cooling rate is altered. It is important to understand that
we are addressing the issue of what occurs under free convection conditions.
In addition to the above, results presented in Table 26.4 also compare what occurs
as the temperature differential (δT) is increased. It can be observed that higher h values
were obtained as δT was increased. Although it should be possible to link this phe-
nomenon to the system dependent average oil viscosity value, this was not done.
Results for h values obtained under a variety of different food frying conditions
are presented in Tables 26.5 and 26.6. Table 26.5 compares the h value data for no
food with food frying conditions. Results show that the metal balls provided h values
about two- to fourfold higher than those obtained without food. Further, values
2
higher than 1000 W/m °C were obtained when metal balls were immersed along
with the frozen food. However, it was difficult to analyze such data because the oil
temperature in the pot fryer rapidly dropped by 15 to 20°C due to ice melt, providing
an unstable variable ambient temperature condition. In addition, because the metal

TABLE 26.6
Influence of Loading Condition on h Value for French Fries
2
Loading h Value (W/m °C)
a
Mass (g) % Temp. (°°C) Al- 1 2 SS- 1 2 Al-1 SS-1
FF: 220 70 180 1000 605 500 580

FF: 340 100 180 860 510 425 445
FF: 390 115 180 890 745 705 615
FF: 440 130 180 650 840 650 560
a
340 g was the standard mass and considered 100% for the comparison study
200
French Fries Chicken No food
340 g 4 pcs 340 g
SS-1/2
150 Al-1
Al-1/2 Al-1/2 Al-1 SS-1
SS-1/2
Al-1
SS-1/2
Al-1/2 SS-1
SS-1
50
0
0 20 40 60 0 20 40 60 80 0 20 40 60 80 100 120
Time (sec)
FIGURE 26.5 Temperature data comparing different food frying conditions. (Al and SS refer
to aluminum and stainless steel, respectively; suffix 1 2 or 1 refers to the metal ball diameter in
inches.)
balls were in contact with the food, there was a large variability in the h value data.
All told, the results clearly show that the h values dramatically increased due to
bubbling and forced convection conditions. The data presented in Figure 26.5 give
a visual perspective of what occurs. Information in this figure shows that metal balls
immersed in the fryer containing French fries (FF) registered the fastest rise in
temperature in comparison to chicken fillets (CH) and the no food frying conditions.
This occurred despite the facts that the metal balls were immersed approximately
60 sec after commencement of frying, and that oil temperature (Ta) dropped by more
than 30 and 10°C for FF and CH, respectively, primarily due to ice melt and water
evaporation.
Before looking at some interesting summarized results, it is pertinent to further
elaborate the ice melt phenomenon. Thermocouple locations in CH and FF were
described in an earlier section. However, additional observations about the thermo-
couple location were obtained by examining the initial temperatures registered and
are shown in Figure 26.6. Surface thermocouples showed initial temperatures slightly
in excess of 0°C (indicating food–air interface), and the thermocouples located at

0 100 200 300
190 0
Oil
CH-BL
140 -0.25
Temperature (C)
Ln (Temp Ratio)
FF-BL
French fry
90
Chicken French fry Chicken
40 -0.75
-10 -1.00
0 40 80 120 160 200 240 280 320 360 Time (sec)
Time (sec)
FIGURE 26.6 Temperature data comparing cooking characteristics of French fry to those of
chicken fillet. (CH, chicken fillet; FF, French fry; BL, boundary layer.)
the center indicated temperatures below zero. The data also showed that the French
fries thawed rapidly.
After commencement of frying, the FF were completely thawed after 10 sec,
whereas the CH piece took approximately 100 sec to register center temperatures
in excess of 0°C. A rapid increase in temperature at the surface (boundary layer:
BL) and temperatures in excess of 100°C suggest that these thermocouples were
protruding slightly outside the food surface. Overall, the time–temperature data
presented in Figure 26.6 provide clarification on why rapid and larger temperature
drops were registered during the processing of frozen FF. Similar, but smaller, tem-
perature drops occur in food service commercial fryers because these units employ
more powerful heating elements.
Returning to the data presented in Table 26.5, it can be observed that during the
frying of chicken fillets, lower h values were obtained at the 90 sec mark in com-
parison to 60 sec after the start of frying. This shows that as turbulence subsided
after the rapid melt of the surface ice layer, the h values were reduced. These results
are comparable to those provided by Costa et al. (1999) and Hubart and Farkas
(1998), in which it was shown that the variable h value is reduced as frying
progresses. Comparing data from chicken to that of French fries shows that higher
h values were obtained during the immersion of FF. Costa et al. (1999) compared
potato crisps with French fries and reported higher h values for the crisps. Thus,
higher evaporative rates provide more turbulent frying conditions and larger asso-
ciated h values.
Prior to discussing the somewhat contradictory results presented in Table 26.6,
it is pertinent to define the three major measurement and evaluation errors. It is
believed that the primary error related to h value determination during the cooking
of French fries was due to transducer (ball) contact with the food particulates. When
bubbling food particulates are in contact with or in close proximity to the transducer,
the heating boundary layer is continually altered. Because bubbles can adhere to
and/or burst on the ball surface, an error is incorporated into the temperatures
registered by the metal balls. Thus, there was a noticeable scatter in the h value data
obtained. The second error is due to the fact that the Biot criterion (Bi ≤ 0.1) is not

2
satisfied for stainless steel balls when h values increase beyond 400 and 800 W/m °C
for the large and small balls, respectively. Error 3 is unique and to the best of our
knowledge a subject that has not received much attention. This error can possibly
be explained on the basis of the theory of turbulence and forced convection. Bubbling
induces turbulent forced convection heating conditions, and as such the ball diameter
needs to be taken into account and tied to the dimensionless Nusselt number (Nu).
Thus, a question to be addressed in future studies is whether the lumped capacity
approach can be used to estimate h values under turbulent bubbling conditions.
Although the results obtained and presented here are exciting, a link between h
values and Nu was not established. However, in general terms it can be stated that
the lower h values provided by larger balls need to be associated with Nu. Thus,
information for the associated Reynolds number and the Prandtl number is
required, along with temperature-dependent data for the oil thermal conductivity
and viscosity.
The data presented in Table 26.6 show that due to errors associated with the
measurement of h values, we were unable to quantify the influence of more food
vs. less food. Fryer limitation was also a negative factor, because under high loading
conditions the large temperature drop suffered was followed by a long period of
slow recovery or, more specifically, almost no recovery (see Figure 26.5). However,
the scattered data indicate that metal transducers consistently registered higher h
values due to turbulent bubbling conditions. The highest h value obtained for the
least food (220 g) situation was due to turbulence and the fact that there was a
smaller temperature drop in the fryer because less food was fried. Our experience
with this part of the study showed that there is a need to cage (isolate) transducers
so that more consistent data can be obtained.
Not precluding the above, one final hypothesis also needs to be considered with
respect to loading conditions and different food materials. In very simple terms it
can be defined as the microclimate/environment that exists in the fryer when different
food products are fried. When the data for FF provided in Table 26.5 are combined
2
with the data in Table 26.6, average h values of 905, 740, 630, and 545 W/m °C are
obtained for Al- 1 2 , SS- 1 2 , Al-1, and SS-1, respectively, and these data appear to
be closely grouped together for each transducer. This shows that there is a need to
link Nu to fryer oil temperature, transducer size, and transducer material. For this
reason, h value data should be related to the product being fried. A case on micro-
climate is put forth because the data of Costa et al. (1999) showed that crisps and
French fries provided noticeably different peak h values. We believe that the results
presented and discussed in this chapter will help other researchers to further elaborate
the data on h values associated with deep fat frying.
26.4 CONCLUSIONS
The experimental data presented show that metal transducers provide relatively high
h values when food materials are being cooked in hot fryer oil, and this was
associated with the turbulent mixing regime. It is interesting to note that the degree
of oil abuse did not appear to influence the h value (Table 26.2). The comparison
of chicken fillet vs. French fries shows that larger pieces lose moisture at a slower

rate (due to larger mass to surface area ratios), and because bubbling was reduced,
the apparent h value was smaller (Table 26.5).
NOMENCLATURE
2
A Surface area (m )
Bi Biot number
Cp Specific heat (J/kg°C)
2
H Convective surface heat transfer coefficient (W/m °C)
K Thermal conductivity (W/m°C)
R Ball radius (m)
T Time (sec)
T Temperature (°C)
T.R. Temperature ratio
3
V Volume (m )
θ Temperature ratio
3
ρ density (kg/m )
ACKNOWLEDGMENTS
The authors thank Glenn D. Farrell (Research Coordinator I) and Vijaya Man-
tripragada (Lab Technician II) for their assistance. Author Pannu thanks the Biolog-
ical Systems Engineering Department of Washington State University and Dr.
Gustavo V. Barbosa-Cánovas for time and facilities provided for the preparation of
this manuscript.
REFERENCES
Blumenthal, M.M., A look at the chemistry and physics of deep-fat frying, Food Technol.,
45, 68–71, 1991.
Costa, R.M., Fernanda, A.R.O., Delaney, O., and Gekas, V., Analysis of the heat transfer
coefficient during potato frying, J. Food Eng., 39, 293–299, 1999.
Costa, R.M., Oliveira, F.A.R., and Gekas, V., Application of image analysis to the study of
water losses from potato slices during frying, in Engineering and Food at ICEF 7,
Part I, Jowitt, R., Ed., Sheffield Academic Press, Sheffield, 1997.
Dincer, I., Modelling for heat and mass transfer parameters in deep-frying of products, Heat
Mass Transfer, 32, 109–113, 1996.
Farid, M.M. and Chen, X.D., The analysis of heat mass transfer during frying of food using
a moving boundary solution procedure, Heat Mass Transfer, 34, 69–77, 1998.
frying. I. Model development, J. Food Eng., 29, 211–226, 1996a.
frying. II. Model solution and verification, J. Food Eng., 29, 227–248, 1996b.
Fellows, P.J., Food Processing Technology — Principles and Practice, Woodhead Publishing
Ltd., Cambridge, U.K., 1996.

Hallstrom, B., Skjoldebrand, C., and Tragardh, C., Heat Transfer and Food Products, Elsevier
Applied Science, New York, 1988.
Hubart, J.L. and Farkas, B.E., Determination of the convective heat transfer coefficient during
frying, in Drying ’98, Aktridis, C.B., Marinos-Kouris, D., and Saravakos, G.D., Eds.,
Ziti Editions, Thessaloniki, 1998.
Miller, K.S., Singh, R.P., and Farkas, B.E., Viscosity and heat transfer coefficient for canola,
corn, palm and soybean oil, J. Food Process. Preserv., 18, 461–472, 1994.
Pannu, K.S. and Chinnan, M.S., Heat Transfer Coeffecient Associated with Heating/Frying
of Food Pieces in Oil, abstract (#8–11), Annual Meeting of the Institute of Food
Technologists, Chicago, July 23–28, 1999.
Pannu, K.S. and Chinnan, M.S., chap. 4.1, this volume.
Sahin, S., Sastry, S.K., and Bayindirli, L., The determination of convective heat transfer
coefficient during frying, J. Food Eng., 39, 307–311, 1999.
Singh, R.P., Heat and mass transfer in foods during deep-fat frying, Food Technol., 49,
134–137, 1995.
Tseng, Y.C., Moreira, R., and Sun, X., Total frying-use time effects on soybean-oil deterio-
ration and on tortilla chip quality, Int. J. Food Sci. Technol., 31, 287–294, 1996.

Part IV
Combined Transfer Phenomena

Relating Food Frying to
27 Daily Oil Abuse. Part 2.
A Practical Approach
for Evaluating Product
Moisture Loss, Oil Uptake,
and Heat Transfer
CONTENTS
27.1 Introduction
27.3.1 Moisture Loss
27.3.2 Oil Uptake
27.3.3 Heat Transfer
27.4 Conclusion
Nomenclature
Acknowledgments
References
27.1 INTRODUCTION
During deep fat frying a series of complex physical and chemical changes com-
mences immediately after the immersion of high-moisture food products into hot
oil (Singh, 1995; Saguy and Pinthus, 1995; Saguy et al., 1998). The chemical
reactions alter the product characteristics as well as the quality of the cooking
medium, i.e., the frying oil. Essentially, frying is a heat–mass transfer operation
where the cooking oil/fat imparts several desirable quality attributes such as flavor,
texture, appearance, and mouthfeel to the food products. These desirable changes
imparted to the cooked food are a combined result of moisture loss, crust formation,
protein denaturation, starch gelatinization, oil/fat uptake, and numerous microstructural

changes within the food (Blumenthal, 1991; Saguy and Pinthus, 1995; Saguy et al.,
1998). However, undesirable changes are imparted to the cooking medium due to
oil–water interaction and oxidation, along with changes caused by heating, cooking,
the transfer of foreign materials from food to oil, and the accumulation of food
residues/debris (Blumenthal, 1991; Saguy et al., 1998).
Experimental data from studies that simulate and resemble normal cooking (food
processing) conditions are required for the development and validation of predictive
mathematical models. Food processing methods, including deep fat frying, utilize heat
for product cooking. Thus, a set of boundary conditions is defined and a value is assigned
for the convective heat transfer coefficient (h value) to facilitate the development of
models to predict the initial and subsequent transfer of heat from the medium to the
food solids (Singh, 1995; Farkas et al., 1996). Pannu and Chinnan (Chap. 26, this
volume) provided a brief overview of methods currently employed to obtain data for
this critical parameter, i.e., the h value. Through the presentation of literature data and
experimental results they showed that the large variability in h values obtained with
metal transducers was process related. Thus, a simple method was developed to obtain
data for the apparent and/or overall heat transfer coefficient directly from food pieces
by using the product moisture loss data (Pannu and Chinnan, 1999) and elaborated here.
In comparison to frying, the cooking of solids in steam, water, or sauce is a simple
operation because heat transfer predominates, and mass transfer effects are usually
ignored for mathematical model development. Such simplifying assumptions are not
valid for cooking by deep fat frying, as three (and often four) dominant energy-demand-
ing processes commence simultaneously after the food is immersed into hot oil. These
processes can be defined to represent heating, moisture loss, crust formation (Singh,
1995; Saguy et al., 1998), and the less recognized fourth process of thawing (ice to
water, as in the case of frying frozen food). Oil uptake need not be included in the
above category because it can be reasoned that this process is not energy demanding,
and its influence on thermal property data can be incorporated into the heat transfer
equations during process calculations. Thawing during frying of frozen products can
significantly affect the product temperature rise and in turn the cook value. Data pre-
sented by Pannu and Chinnan (Chap. 26, this volume) show that it takes approximately
100 sec for complete ice meltdown to occur at the center of a 340 g chicken fillet during
ο
frying at 160 C. Results provided by Rao and Delaney (1995) indicate that it takes 400
sec for the core temperature of a prebreaded frozen chicken thigh to reach the melting
ο
point (0 C). Thus, consideration should be given to this aspect of deep fat frying,
especially for the establishment of product cook values related to food safety issues.
In addition, instantaneous sputtering and bubbling occur as a result of ice melting
during frying of frozen products. This indicates that water evaporation starts immediately
after the frozen food is immersed into hot oil. Because of this, the moisture loss curves
obtained with frozen foods do not depict the customary lag characteristics found at the
beginning of a typical drying curve. Little or no information is available in the literature
on lag factors associated with moisture loss during the deep fat frying of food products.
Products that are not frozen and/or food materials with less surface moisture depict some
form of lag because there is a noticeably subdued time-delayed bubbling action.
The bubbling action, whether vigorous (turbulent) or subdued, is a result of mois-
ture flashing to steam and the vapor channeling its way through the oil. Thus, it can

be reasoned that higher bubbling rates indicate that the product is losing larger amounts
of moisture. Most of the research related to studying the moisture loss characteristics
of food during deep fat frying has been conducted by removing selected food pieces
at set intervals from the fryer during the cooking process and then assessing the amount
of moisture loss (Baumann and Escher, 1995; Ufheil and Escher, 1996). Such tests
are valuable because information is simultaneously obtained for moisture loss, crust
development, and oil migration/uptake. However, a major limitation of this method is
that the initial mass and the final mass of each individual food particle must be known,
and several precisely manufactured uniform food pieces of the same size and shape
must be available. Further, because the tests are conducted with few food pieces, it is
difficult to precisely quantify oil migration and moisture losses that occur during the
transfer process from the fryer to the weighing container (Ufheil and Escher, 1996).
Limitations related to sample preparation make it difficult to ascertain the mois-
ture loss characteristics of commercially prepared frozen foods during deep fat frying
by the above method. Pannu and Chinnan (1999) developed a simple technique
called active moisture loss measurement and obtained moisture loss data by placing
a pot fryer on a balance and by recording the fryer weight change at 20 sec intervals.
Through active moisture loss measurements, it was also possible to map the transition
phase that occurs when food materials become buoyant and move from the sink to
floating stage. Moisture loss characteristics change during floating because the oil
transfers less heat to the food. The active moisture loss method provides good bulk
data and a clearer picture of the food dehydration process during deep fat frying.
The process of quantifying oil/fat migration into food products is challenging. It
is difficult to precisely define the time period and amount of oil/fat absorbed by the
food due to the vacuum effect created by product cooling after the product is removed
from the hot oil (Ufheil and Escher, 1996; Saguy et al., 1998). Ufheil and Escher
(1996) stated that oil content analysis conducted on potato slices removed from hot
oil during frying does not provide conclusive evidence on when and how much oil is
transferred to the food. Thus, the authors conducted experiments with Sudan Red used
as a lipid staining dye to define the time period at which oil migration occurs during
the frying of potato slices. Their results indicate that majority of oil was absorbed by
the potato slices after removal from the frying medium. In addition, their experimental
results also indicate that oil uptake by potato slices manufactured from potato tubers
with higher density was lower than for slices from lower density potato tubers.
In general, it can be stated that oil uptake is a function of product type, initial
moisture content, product thickness, frying temperature, and frying time (Ufheil and
Escher, 1996; Saguy et al., 1998). It has been shown that oil uptake increases as the
product moisture content increases, thickness decreases, oil temperature decreases,
and frying time increases (Blumenthal, 1991; Ufheil and Escher, 1996; Saguy et al.,
1998). However, Saguy and Pinthus (1995) indicated that food additives affect oil
uptake and moisture loss characteristics, and this may be one reason why donuts
made from dough with higher initial moisture content absorb less oil. Thus, the use
of different formulations and food additives can alter the water retention capability
of food and in turn influence its oil uptake capacity (Saguy and Pinthus, 1995).
Product heating, dehydration, crust formation, the influence of surfactant buildup
due to oil reuse/abuse, and oil uptake are all tied together. The continuous outflow of

steam during the entire cooking period indicates that the pressure inside the food is
greater than that of the environment. This phenomenon limits the entry of oil through
the surface (crust) to within the food. Thus, oil uptake is localized to the crust region,
and the polymers present in the frying oil are mainly adsorbed on the outer layers of
the deep fat fried food (Blumenthal, 1991; Ufheil and Escher, 1996; Saguy et al.,
1998). As the fryer oil becomes contaminated through repeated use, the surface tension
of the oil at the oil–food interface is reduced because surface active agents are produced
by lipid oxidation (Blumenthal, 1991; Singh, 1995; Saguy et al., 1998). An increase
in the surfactant levels also induces increases in the food–oil contact time, heat trans-
mission to the food surface, and oil adsorption by the crust. Although excessive heat
is available at the food surface due to more oil–food contact, the amount of thermal
energy utilized and transmitted by conduction to the interior remains unaltered (is
constant). Therefore, foods cooked in used/abused oil depict excessive darkening and
drying at the food surface (Blumenthal, 1991). The results presented by Pannu and
Chinnan (Chap. 26, this volume) support the above-described phenomenon as the
convective heat transfer coefficients estimated with metal transducers did not change
through oil use (day 1 vs. day 8). Although the surface food color and off-flavor effects
are marginally acceptable at the 1.5% free fatty acids (FFA) level but are more
pronounced at the 3% FFA level (Jacobson, 1991), we did not attain the higher degree
of oil abuse in our eight-day study. Thus, it is probable that the moisture loss charac-
teristics of the food may not be affected at the 1.5% FFA level. Research on the
chemistry of oil breakdown and the role of surfactants in deep fat frying is well
documented (Perkins, 1967; Blumenthal, 1991; Pinthus and Saguy, 1994; Saguy and
Pinthus, 1995; Paul and Mittal, 1996; Saguy et al., 1998) and is not reviewed here.
The objectives of this research were divided into two parts. The first objective
was to estimate the moisture loss and oil uptake characteristics of commercially
prepared frozen par-fries and breaded chicken fillets. The active measurement pro-
cedure was employed to study the influence of (1) fryer loading condition (less food
vs. more food) and (2) oil abuse on moisture loss and oil uptake by food. The second
objective was to determine the overall convective heat transfer coefficient (U) by
using food moisture loss data. Moisture loss data from frozen French fries and
breaded chicken fillets were evaluated to determine whether comparable U values
were obtained for the food under different loading conditions.

A kitchen pot fryer (3.5 liter capacity) and commercial grade hydrogenated soybean
oil were used for the food frying study. Figure 27.1 is a schematic representation of the
method employed and the tools required. The fryer was placed on an Ohaus laboratory
balance (Model 120W, Florham, NJ), and a preweighed lot of food was then placed
into the fryer basket, as depicted in Figure 27.1 (center). Thereafter, the balance was
tared to zero and the food basket was immersed into the hot cooking oil. Weight changes
(negative numbers) due to moisture evaporation (Figure 27.1, left) were manually
ο
recorded on a data sheet at 20 sec intervals. Food frying was conducted at 180 C for
5 min. After completion of the cook cycle, the food basket was removed from the hot
oil and the product was allowed to drain/cool for an additional 5 min (similar to

Time(sec) Wt. (g)
----------------------------
0 0.0
20 5.0
40 8.5
60 12.0
BALANCE BALANCE 80 18.0
- 037 g 000 g
FIGURE 27.1 Pot-fryer with food fried on a balance for moisture loss determination. Study
compares fresh oil vs. abused oil (oil used for more than one day.
Figure 27.1, center). Product weight loss during this cooling/drain period was recorded
every 60 sec. Thereafter, the contents of the food basket were transferred to a container,
and the fried product weight was recorded. The final balance weight with the empty
basket was also recorded to determine the degree of oil loss by the fryer. Although such
losses were small, they provided a means for crosschecking the overall success of each
moisture loss experiment and validating the oil uptake data.
Oil uptake was calculated as total moisture loss less the product (food) weight
change. Total moisture loss was the final negative value provided by the tared (active)
balance. Product weight change was defined as the difference between the initial
product weight before frying and the weight of the fried product recovered from the
fryer basket. It should be noted that after oil is absorbed by the product, the value
for active moisture loss recorded during frying will be larger than the value obtained
for product weight change.
Details on methodology and protocol employed are detailed elsewhere (Pannu
and Chinnan, Chap. 26, this volume). For the variable food mass study (days 1, 4,
and 7), six batches of par-fries and 14 batches of chicken fillets were fried in the
order outlined in Table 27.1. Variable food mass for French fries was designated as
±15 and ±30% above or below the normal batch weight of 340 g and for chicken
as 3, 4, and 5 fillets. This was done to ensure that the same mass of food was fried
each day. The normal weight was defined as 340 g because the average weight of
a chicken fillet was approximately 85 g, and four chicken fillets were designated as
the standard loading condition.
Unfortunately, a transcribing error was made during the protocol preparation
and instead of 290 g (85% of normal loading) of French fries 220 g (65% of normal
loading) were processed under batch 5 (Table 27.1). Thus, no data are available for
the 85% loading level of French fries. In addition, we did not identify whether all the
breaded chicken came from the same lot. At the data analysis stage, it was realized
that the breaded chicken pieces were from two different lots. Breaded chicken fillets
cooked on most days had an average mass of 85 g, whereas those utilized on the
morning of day 7 weighed slightly more (95 g) and were most likely from a different

TABLE 27.1
Experimental Protocol for the Variable Food Mass Frying Study, Along with
Data Compiled for Product and Oil Usage
File Name: ABC-1; Frying Cycle 1 of 8 days; Date: April 29, 1999
Weight of Empty Fryer: 1.629 kg; Weight of Oil: 2.615 kg
Batch # Time Food (g) Product Batch # Time Food (g) Product
1 9:00 317.6 CH-4 11 13:20 306.4 CH-4

2 9:20 235.1 CH-3 12 13:40 240.9 FF (–30%)
3 9:40 385.4 CH-5 13 14:00 440.2 FF (+30%)
4 10:00 330.2 CH-4 14 14:20 325.0 CH-4
a
5 10:20 223.6 FF (−35%) 15 14:40 310.5 CH-4
a
6 10:40 393.3 FF 16 15:00 331.3 CH-4
7 11:00 328.7 CH-4 17 15:20 316.1 CH-4
8 11:20 340.2 FF (base-line) 18 15:40 341.7 FF (base-line)
9 11:40 347.0 CH-4 19 16:00 293.8 CH-4
10 12:00 345.3 CH-4 20 16:20 303.8 CH-4
TOTAL W1 = 3246.3 TOTAL W2 = 3199.8
Note: FF, French fries; CH, chicken.
1) Weight of fryer + oil + basket: 4443 g at start

2) Weight of fryer + oil + basket: 4379 g at noon
a) Oil loss = 1–2 54 g
3) Weight of fryer + oil + basket: 4431 g after oil addition
4) Weight of fryer + oil + basket: 4374 g at end
b) Oil loss = 3–4 57 g
c) Total oil loss = a + b 111 g
d) Total food fried = W1 + W2 6646 g
a
Due to a transcribing error, ~220 g of French-fries (–35%) were processed for batch 5 instead of the
required ~290 g (−15%). Thus, no data were obtained for the −15% level.
manufactured lot (later verified). Because the moisture loss and oil uptake data were
drastically affected, we suspect that the preparation method and breading were
different for the two lots. Fryer limitations also contributed to an error because it was
ο
not possible to precisely maintain the 180 C initial cooking temperature. Moisture loss
results for the extra studies (defined later) were analyzed to obtain data on the rate
of moisture loss for each of the three food frying conditions.
The following explains how moisture loss data can be used to obtain a value for the
overall convective surface heat transfer coefficient (U). The primary assumption required
ο
to obtain U is that after the food temperature has stabilized to 100 C, most of the thermal
energy (qHT) provided by the hot oil is utilized for moisture evaporation (qML). It should
be noted that due to constant moisture evaporation the food temperature remains steady
ο
at approximately 100 C for an extended period of time. Thus, it can be stated that:
qHT ≈ qML (27.1)
qHT = U A (∆T) ≈ qML = mλ (27.2)

2
with q as energy (W), U as the overall heat transfer coefficient (W/m °C), λ = 2257
J/g (latent heat for evaporation/g of water), m as the mass of water loss per unit time
and ∆T = TOil − 100. As an example, in Equation (2) the surface area (A) of an average
2
French fry (30.84 cm ) was obtained by weighing a batch, counting the number of fries,
and determining the weight per unit length and the average fry thickness. The term ∆T
is the fryer oil temperature less 100°C. qML is obtained by multiplying λ by the moisture
loss (ML in g/sec) data obtained during active frying for a fixed time period.

27.3.1 MOISTURE LOSS
The active moisture loss measurement method was simple, rapid and effective. The
method also helped provide a better understanding of the frying process because it
allowed differentiation between the sink and floating conditions that are a norm of the
deep fat frying process. Typical moisture loss curves obtained for this three-day
comparative study are presented in Figures 27.2 and 27.3. The data show that in
comparison to French fries (FF), chicken fillets (CH) lose less moisture; CH also lose
moisture at a uniform rate. The FF data for moisture loss appear to follow a curvilinear
mode. Thus, questions related to the constant rate drying characteristics of FF and CH
during deep fat frying need to be addressed. A careful inspection of the data for French
fries showed that the reduced moisture loss phase commenced after 200 sec of cooking.
It was observed that the point at which FF started to float was close to this time.
After flotation occurs, more than a quarter of the food surface is exposed to air.
Because heat transfer decreases, the rate of moisture loss also decreases. Thus,
moisture loss characteristics are altered at this point, and this is the reason for the
downward dip in the moisture curve. Further, flotation or buoyancy are related to
the product bulk density and provide visual verification of the fact that the cooked
15
Day 1-m Day 4-m Day 7-m
245 g (3 pcs) 260 g (3 pcs) 280 g (3 pcs)
325 g (4 pcs) 335 g (4 pcs) 385 g (4 pcs)
370 g (5 pcs) 410 g (5 pcs) 480 g (5 pcs)
% Moisture Loss
10
Product Change
0
0 100 200 300 0 100 200 300 0 100 200 300
Time (sec) Time (sec) Time (sec)
FIGURE 27.2 Moisture loss curves comparing the influence of oil use and loading conditions
for deep fat fried chicken fillets.

40 40
Day 1-m Day 4-m Day 7-m
30 30
% Moisture Loss
20 20
10 10
230 g 220 g 220 g
340 g 340 g 340 g
390 g 390 g 390 g
0 0
0 100 200 300 0 100 200 300 0 100 200 300
Time (sec) Time (sec) Time (sec)
for French fries deep fat fried in the morning.
50
FF: 240 g
FF: 340 g
FF: 440 g
40 CH: 270 g (3 pcs)
CH: 360 g (4 pcs)
CH: 455 g (5 pcs)
% Moisture Loss
30
French fries: float
20
Chicken: float
10
0
0 100 200 Time (sec) 400 500 600
for French fries and chicken fillets deep fat fried for 10 minutes.
product has attained a density equivalent to that of the hot oil. Since the density of
3
the hot cooking oil is about 800 kg/m at 160°C, this suggests that at the point of
flotation the high moisture frozen FF have lost about 20 to 25% of their initial mass
through water evaporation. The FF data support this phenomenon because the
moisture loss curves show that the point of inflection occurs after FF lose 20%
moisture. Additional tests with a longer cook period (10 min) were later conducted
to verify the constant rate dehydration phenomenon for the deep fat frying of frozen
products. These results are presented in Figure 27.4 and clearly show the two distinct
constant rate dehydration rates for FF. It is to be noted that a majority of the predictive
mathematical models developed do not take into account the influence of flotation.
Therefore, further research in this area is warranted.

At first glance, the data for moisture loss by the CH (Figure 27.2) do not provide
a clear picture of the process. Product change is probably the only valid explanation
for moisture loss (and oil uptake) differences recorded on day 7. A quick calculation
for product mass (with the data on product mass provided in Figure 27.2) showed that
the day 7 fillets weighed approximately 10% more than those used on the previous days.
Data for day 1 and 4 show that CH registered a moisture loss of approximately 11%
(w.b.). The small differences in moisture loss data are attributed to the variability in
oil temperature and the surface area effects. The kitchen fryer was limited in its ability
to maintain a constant temperature and rapidly regain the temperature losses suffered
due to food surface ice melt. Thus, the temperature lowering effect was less pro-
nounced when less food was cooked, and this produced a slightly higher moisture loss.
The CH moisture loss data (Figure 27.2) provide some interesting observations on
the lag phenomenon mentioned earlier. The day 4 and day 7 data elaborate this point,
as it can be clearly observed that more moisture was lost in the first 20 to 40 sec of
frying. The data show that the accelerated moisture loss phase is followed by a curvi-
linear lag phase and subsequently by constant rate dehydration. Results in Figure 27.4
also clearly define the three stages and show that the constant rate period for CH
commences after 140 sec of cooking. In comparison, FF data (Figure 27.3) show that
ice melt (thawing) and the lag phase occur simultaneously and terminate after 40 to 50
sec. Smaller and less defined lag phases are expected with smaller size food particles.
Comparative results show that after 300 sec of cooking, FF lose more moisture
than CH, 30 vs. 11%, respectively. The four major differences between the two products
are surface area, product thickness, food type/structure, and the initial moisture content
(69 and 59% for FF and CH, respectively). Besides product differences, a simple
calculation shows that mass to surface area ratios for FF and CH were approximately
2
0.21 and 0.48 g/cm , respectively. Thus, higher moisture losses by FF, a product with
a smaller mass–area ratio, are in agreement with theory (Saguy et al., 1998).
Reduced moisture loss due to temperature lowering effects (fryer limitation)
were also noted for FF. On the afternoon of day 7, the cooking of FF at locations
12 and 13 (Table 27.1) was switched, and more food was followed by less food. It
was observed that in comparison to other days, less moisture loss was recorded by
240 g of FF. Although loading conditions may influence the moisture loss rate during
frying, no conclusions could be drawn in this study because the processing temper-
atures were not constant. Further, the data presented in Figure 27.3 for the 340 g
tests show that an increase in FFA from 0.05% (day 1) to 1.3% (day 7) did not affect
the moisture loss characteristics of the frozen FF. Thus, it can be concluded that oil
abuse had negligible influence on product moisture loss.
Because surfactants promote enhanced oil–food contact, one would expect the
product heating rate to increase. However, this did not occur. The moisture loss
characteristics remained unaltered and did not increase as would be expected. This
suggests that the value of the apparent heat transfer coefficient was not affected, as
FFA values increased to the 1.55% test levels, and it is supportive of the h value
data reported in Pannu and Chinnan, Chap. 26, this volume. Thus the rate at which
thermal energy was absorbed and utilized for moisture loss by the FF remained
unaltered, and excess heat available due to enhanced oil–food contact induced
surface burning (charring) effects.

27.3.2 OIL UPTAKE
The consolidated data for oil uptake are presented in Table 27.2. To make a justifiable
comparison, it is pertinent to look at the data for case 2 (column 5) where 340 g of
product were cooked. The data for chicken show no oil uptake by this product.
However, because breading picks up oil/fat, the results indicate that some form of
oil/fat migration occurs from the chicken to the fryer oil. Overall, it can be stated
that the results for chicken tend to indicate that there is no or negligible change in
the fryer oil content. Data presented in the study by Pannu and Chinnan (Chap. 26,
this volume), where only two batches of FF were processed on day 2, show that
only 53 g of oil were lost after 6710 g of product was fried, and oil uptake was less
than 1% for the entire day. In this variable mass study, however, where six batches
of FF were fried (Table 27.1) 1.7% oil was lost or picked up by the food. Thus,
accounting for oil losses due to splattering and other experimental errors, it can be
stated that the global results match well with the active data.
The results for FF show that oil uptake at the 340 g level is consistent and
indicate that on average the product absorbed an additional 3.8% oil. The 3.8% oil
uptake was calculated on a wet basis and translates to 5.6% of the final product
weight, assuming 32% moisture loss (Figure 27.3). We use the word “additional” for
TABLE 27.2
Oil Uptake by Chicken Fillets (CH) and French Fries (FF)
c
% Oil Uptake
a b d
Day FFA Product Case 1 Case 2 Case 3 Average
1 <0.05 CH 0.6 (252–3) −0.1(323–4) −0.4(367–5) 0.0

4 0.67 CH 0.6 (273–3) −0.9(328–4) 0.5(413–5) 0.1
7 1.30 CH 2.8 (283–3) 2.8(386–4) 2.5(485–5) 2.7
1 <0.05 FF–m 5.9 (234) 4.1 (341) 4.9 (390) 5.0
1 0.10 FF–a 4.0 (246) 4.0 (343) 4.2 (445) 4.1
4 0.67 FF–m 7.9 (221) 3.4 (341) 5.5 (391) 5.6
4 0.77 FF–a 3.7 (240) 3.1 (341) 3.7 (439) 3.5
7 1.30 FF–m 4.2 (221) 4.0 (343) 6.0 (390) 4.7
7 1.40 FF–a 5.0 (241) 4.1 (343) 4.9 (441) 4.7
Avg. FF — FF 5.1 (230) 3.8 (342) 4.9 (415) 4.6
e
Extra 0.20 CH 1.6 (268–3) −0.7(361–4) −0.1(453–5) 0.2
Extra 0.20 FF 6.7 (243) 7.2 (341) 5.9 (442) 6.6
a
FFA: Free fatty acids.
b
CH: chicken fillet; FF–m: French fries–morning; FF–a: FF–afternoon. Also note that chicken
fillets received from supplier for day 7 were from a different batch.
c
Values in parentheses for FF refer to product mass in grams. For CH, they refer to chicken
fillets, mass and number of pieces.
d
Cases 1, 2, and 3 refer to variable mass of food fried (value in parentheses). Case 2 is the norm
(340 g or four pieces of chicken). Cases 1 and 3 are less and more than the norm, respectively.
e
Tests were conducted after the 8-day study, and product was cooked for 10 min (norm was
5 min).

FF because the par-fries already contained oil/fat from prior processing. Data pro-
vided by Saguy et al. (1998) indicate that cooked FF have an oil content between
7.6 and 14.8 g/100 g. The FF processed in this study fall within the above range
after an appropriate number is added to the 5.6% value. However, because oil uptake
levels remained constant, it can be stated that surfactant buildup (at the level tested)
does not appear to affect the oil uptake characteristics of the frozen FF.
Oil uptake data presented for cases 1, 2, and 3 (Table 27.2) refer to less food, daily
norm (340 g), and greater food loading conditions, respectively. The data on oil uptake
are in agreement with other data in the literature. By comparing the data for the 10-
min cooking period with the other results for FF (normally cooked for 5 min), it can
be observed that oil uptake increases as processing time is lengthened (Table 27.2).
Further, the cooking oil temperatures for cases 1 and 3 were higher and lower than
for case 2, respectively. This was because the fryer registered higher temperature drops
when more food was cooked. This influenced oil uptake; results show that on average
there was more oil uptake by FF for higher and lower cooking temperatures. Finally,
to validate our oil uptake data, a global calculation was made with data presented in
Table 27.1. The information presented shows that 1980 g of FF were cooked on day 1.
Using the overall oil uptake number of 4.6% (Table 27.2; average data for FF), 91 g
(1980 g × 0.046) of oil was absorbed by the FF. This number is slightly lower than
the tabulated value of 111 g (Table 27.1, item c: total oil loss), indicating that CH
pieces did not pick up oil, and suggesting that the loss of fat by the meat is balanced
by the oil uptake by the breading. The process of oil movement and/or exchange needs
to be studied. In addition, there is also a need to clarify why two similar breading
compositions provided such different oil uptake data for CH pieces.
27.3.3 HEAT TRANSFER

Figure 27.5 graphically depicts temperatures during the food frying process and
shows that the product internal temperature did not increase beyond 100°C during
the water evaporation stage. This also holds true for a point located just below the
food surface. In their study, Pannu and Chinnan (Chap. 26, this volume) reported
that the center temperature of the FF and CH reached 100°C after 70 and ~320 sec,
respectively. Since FF and CH begin to float after 200 and 440 sec (Figure 27.4),
200
160 Oil
Temperature (°C)
120
80
Surface
Center
40
0
Time (sec)
FIGURE 27.5 Temperature profiles normally obtained for deep fat frying.

TABLE 27.3
Data Obtained for the Overall Convective Heat Transfer
Coefficient (U)
a 2
Test Mass (g) Number of Pieces ML (g/sec) ∆T (°C) U (W/m °C)
FF-1 243 37 0.36 70 102

FF-2 341 52 0.46 67 96
FF-3 442 67 0.51 51 109
Average of above: 102.3
CH-1 268 3 0.13 65 80
CH-2 361 4 0.19 66 86
CH-3 456 5 0.22 59 87
Average of above: 84.3
Note: ML: moisture loss.

a
∆T as defined in Equation 27.2 (Frying oil temperature – 100°C).
respectively, the time period selected for moisture loss data used to calculate U was
defined as 80 to 180 sec for FF and 320 to 420 sec for CH.
2
Results tabulated in Table 27.3 indicate that U is approximately 102 W/m °C
2
for FF and 84 W/m °C for CH. For food frying, U and h should be the same because
of the assumption that food is homogenous and h is uniform under transient heating
conditions. A distinction is made here because of the controversy that surrounds the
means to correctly determine and/or define h. Further, an examination of the moisture
loss curves (Figures 27.2–4) shows that a distinct lag phase occurs prior to the
commencement of constant rate dehydration. During this lag period, part of the energy
is used for product heating and the other part for water evaporation at the food surface.
Since only a very small fraction of energy is required for product heating, an overall
2
h (U) or an apparent h value of 100 W/m °C should satisfy this requirement.
Data reported by Dincer (1996) define the decoupled h value component for
2
heating during food frying as 14 W/m °C. This implies that an overall h of 100
2
W/m °C will provide 14% of the energy (on a declining scale) for product heating
and the rest for dehydration and food structural changes. The U values obtained and
reported here are similar to the h value obtained by Pannu and Chinnan (1999) and
those reported by Sahin et al. (1999). Further, the heat transfer data show that loading
conditions did not alter the U value. This indicates that moisture loss rates are not
influenced by loading conditions but are related to the fryer oil temperature.
27.4 CONCLUSION
A simple method has been presented to study moisture loss and oil uptake and to
quantify the rate of heat transfer during deep fat frying. The results from our pot
fryer study show that moisture loss is product dependent and that the rate of
moisture loss increases at higher temperatures. Oil uptake is also product dependent.
Oil uptake by frozen French fries (par-fries) was approximately 4.6% (wet basis),

but chicken fillets did not appear to have any net oil uptake. Because breading
absorbs some frying oil, this suggests that the fillets released a small amount of
chicken fat. Our experimental data and procedure show that it is possible to obtain
an estimate for the overall heat transfer coefficient with the moisture loss data. U
2
was estimated as 84 and 102 W/m °C for chicken fillets and French fries, respec-
tively. However, moisture loss data show that this value decreases after the product
becomes buoyant.
NOMENCLATURE
2
A Surface area (m )
2
h Convective surface heat transfer coefficient (W/m °C)
m Mass (g)
q Energy (W)
2
U Overall surface heat transfer coefficient (W/m °C)
∆T Temperature differential (°C)
λ Latent heat for evaporation (J/g)
ACKNOWLEDGMENTS
The authors thank Glenn D. Farrell (Research Coordinator I) and Vijaya Mantripragada
(Lab Technician II) for their assistance. Author Pannu thanks the Biological Systems
Engineering Department of Washington State University and Dr. Gustavo V. Barbosa-
Cánovas for time and facilities provided for the preparation of this manuscript.
REFERENCES
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45(2), 68–71, 1991.
Dincer, I., Modelling for heat and mass transfer parameters in deep-frying of products, Heat
Mass Transfer, 32, 109–113, 1996.
Jacobson, G.A., Quality control in deep-fat frying operations, Food Technol., 45(2), 72–74,
1991.
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of Food Pieces in Oil, Abstr. (#8–11), Annual Meeting of the Institute of Food
Technologists, Chicago, July 23–28, 1999.
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properties, J. Food Process Eng., 19, 201–221, 1996.
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Technol., 21, 125, 1967.
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chicken pieces, Food Technol., 49(4), 138–141, 1995.
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Heat and Mass Transfer
28 during the Frying
Process of Donuts
J.F. Vélez-Ruiz and M.E. Sosa-Morales
CONTENTS
28.1 Introduction.
28.2 Heat and Mass Transfer Modeling
28.3.1 Donut Preparation
28.3.2 Frying Equipment
28.3.4 Frying Experiments
28.3.5 Determination of Moisture and Oil Contents
28.3.6 Evaluation of Transport and Physical Properties
28.3.7 Experimental Design and Data Analysis
28.4.1 Moisture and Oil Contents
28.4.2 Heat Transfer
28.4.4 Experimental Correlations
28.5 Conclusions
Nomenclature
References
28.1 INTRODUCTION
Frying is a traditional means of food preparation, and many fried food items have
physical and sensory attributes that consumers consider desirable. The frying process
produces physicochemical changes and presents engineering challenges due to the
applied high temperatures and combined heat and mass transfer mechanisms during
this type of cooking. In addition, flour transformation during cooking involves com-
plex phenomena, in which water as an essential ingredient has an important role,
since it determines the conformational state of proteins and carbohydrates, affects

the interactions between the formulation constituents, and contributes to dough struc-
turing (Maache-Rezzoug et al., 1998).
Some advances have been reached in relation to deep fat frying of foods, covering
different aspects such as chemical deterioration of frying oil, influence of physical
properties of vegetable oil on food products, effects of physical and chemical char-
acteristics of foodstuffs on the final product, mass and heat transfer during frying,
and mathematical modeling of transfer phenomena of foods with defined geometries
(Vélez and Xique, 1999). Although some studies on donuts have been reported, data
on physical changes and transport phenomena during frying of donuts are scarce.
Therefore, the objectives of this chapter are to introduce proposed analytical solu-
tions for heat and mass transfer phenomena and to analyze the effect of three oil
temperatures (180, 190, and 200°C) and different residence times on the physical
characteristics of donuts and oil through the frying process.
28.2 HEAT AND MASS TRANSFER MODELING

During frying, heat and mass transfer take place simultaneously. Heat is transferred
to the surface by convection and to the product inside by conduction. Even though
most frying processes are conducted at high oil temperatures (150–200ºC), the
temperature of the food product is only about 100ºC, at which water changes from
liquid to vapor. With the increase of product temperature, other biochemical trans-
formations occur, such as starch gelatinization and protein denaturation, among
others. At the same time, the mass transfer phenomenon has been focused on two
fluids—oil and water; water in a frying food migrates from the central portion to
the outside, replacing the evaporated mass, while fat is initially absorbed and later
desorbed (Ateba and Mittal, 1994).
Since the pioneering work of Rice and Gamble (1989) on the modeling of
moisture loss, several approaches have been proposed. Rice and Gamble (1989)
developed a mass transfer model for potato slices during frying, taking Newman’s
solution to the differential equation of mass transfer and considering the slice as an
infinite slab. They applied Equation (28.1) to calculate apparent diffusion coefficients
(Da) of potato slices during the frying process, where C1 was assumed as negligible,
and second and subsequent series terms become so small as to be negligible:
∞
w − c1   (2 n + 1) 2 π 2 D a t  
∑
8 1
= 2   exp −  (28.1)
c 0 − c1 π n=0  (2 n + 1)
2
 4 d 2  
Ateba and Mittal (1994) solved the heat and mass transfer equations for deep
fat frying of beef meatballs that were used to simulate the frying process. The fat
diffusivity, conductivity, and equilibrium fat content were determined from simula-
tion and compared with experimental data from the frying of this meat product.
Singh (1995) and Farkas et al. (1996) established four partial differential equa-
tions (Equations (28.2–5)) for heat and mass transfer phenomena of the core and
crust regions in an infinite slab, based on four distinct stages of the frying process:

1. Heat transfer in core region:
∂2 T ∂T ∂T
k II + NβxCpβ = (εβρβCpβ + ε σρσ Cpσ ) (28.2)
∂x 2
∂x ∂t
2. Mass transfer in core region:
∂Cβ ∂ 2 Cβ
= Dβα (28.3)
∂t ∂x 2
3. Heat transfer in crust region:
∂T ∂2 T ∂T
(ε γ ργ Cp γ + ε σρσ Cpσ ) = k I 2 + Nγ xCp γ (28.4)
∂t ∂x ∂x
4. Mass transfer in crust region:
∂  ∂Pγ 
ρ =0 (28.5)
∂x  γ ∂x 
To solve Equations (28.2–28.5) using three initial and eight boundary conditions,
an implicit finite difference method was used to convert those partial differential
equations into nonlinear algebraic ones. A mainframe computer using the
Gauss–Seidel iteration was used to solve the nonlinear equations; initial moisture
content, oil temperature, and physical properties were needed to run the simulation.
Both computed and measured results were obtained and compared, and very good
agreement was obtained.
Dincer and Yildiz (1996) utilized a model in which a new parameter (frying profile)
was defined by analogy to a cooling profile. They developed the analytical solution
for cylindrical shape and applied the solution to the frying process of sausages at
180ºC. The thermal and mass diffusivities for sausage samples were predicted; the
comparison between determined and experimental data showed high accuracy.
Most of the analytically developed models have practical limitations due to the
need for complex calculations; therefore, most of them have been completed with
numerical equations and solutions by applying the finite element method. Rao and
Delaney (1995) used a first-order approximation for time and a second-order approx-
imation for space derivatives, in which the finite difference method was conducted
using a Fortran program. Equation (28.6) became the computational model, which
evaluates the future value (n + 1) of the central node from the present values (n) in
all six surrounding nodes:
T (i, j, k, n + 1) = {1 − 2m (xd + yd + zd)} · T (i, j, k, n)

+ m · xd [T (i + 1, j, k, n) + T (i − 1, j, k, n)]
+ m · yd. [T (i, j + 1, k, n) + T (i, j − 1, k, n)]
+ m · zd. [T (i, j, k + 1, n) + T (i, j, k − 1, n)] (28.6)

Alternatively, empirical models, though lacking a theoretical basis, may provide
suitable and simpler relationships. For instance, Gamble et al. (1987), Costa and Oliveira
(1999), and Vélez-Ruiz et al. (2001) proposed empirical models for water loss and/or
oil uptake contents through the frying process of foods such as potato slices, potato
tubers, and chicken strips, respectively. The three approaches have advantages and
limitations, but they represent useful tools in the interpretation of the frying process. In
this work, the phenomena of heat and mass transfer during the frying of donuts was
studied.

28.3.1 DONUT PREPARATION
The dough was prepared using a laboratory mixing apparatus, Kitchen Aid KSM
90 model (St. Joseph, MI). To get the same characteristics in all batches, a precise
order for adding the ingredients (wheat flour, water, egg, butter, sugar, salt, and
others) was followed. Each batch required a mixing time of 12 to 18 min.
After mixing, the dough was removed and extended with a roller to reach a sheet
thickness of 1.5 to 2.0 cm with the help of an aluminum platform. The dough was
then cut, and donut specimens were formed with a special device. For fermented
dough, a rest time of 30 min was allowed at 35ºC. After that, the same methodology
for donut preparation was followed.
28.3.2 FRYING EQUIPMENT

Immersion frying was carried out on a batch operation basis. A commercial batch fryer
(F2 model, Mexican Taurus, Tlaxcala, México) with a stainless steel tank of 5 L
capacity was used, in which the oil was heated by electrical resistors at the bottom of
the tank.

A thin thermocouple was specifically inserted in the ring half of the donut samples,
ensuring the position by measurement of the sample dimensions. The temperatures
at the geometric center of the sample and bulk oil were measured by means of
thermocouples attached to a Digi-Sense data logger (Scanning Thermocouple Ther-
mometer, 92800–00 model, Cole–Parmer Instruments Co., Barrington, IL), with a
sampling frequency of 15 sec.
28.3.4 FRYING EXPERIMENTS

Sunflower oil was used as the cooking medium, utilizing the commercial fryer for
processing three to six samples, depending on the experimental conditions. The
experiment was initiated once the desired oil temperature was reached, and the oil
bath temperature was thermostatically controlled. Samples were taken by periodi-
cally removing a sample from the fryer and placing it on absorbent paper until it
reached room temperature. Then, the specific measurements were taken.

28.3.5 DETERMINATION OF MOISTURE AND OIL CONTENTS
Moisture content was determined following the official method 39.1.02 (AOAC,
1995) by drying in a hot-air oven (HDP 334 model, MAPSA, Monterrey, México);
at least four donut samples were used for moisture determination.
Oil content was determined (at least in duplicate) using the Goldfisch method
(3500100 model, Labconco, Co. Kansas City, MO), using 30–40 ml of petroleum
ether and an extraction time of six hours.
28.3.6 EVALUATION OF TRANSPORT AND PHYSICAL PROPERTIES

An overall heat transfer coefficient was obtained from the heat transfer gained by
the donut (Equation (28.7)) for some specific frying periods. The heat transfer was
evaluated as the net energy gained by the donut through heating, water heating, and
evaporation corresponding to the sensible (mDCpdT + mwCpdT) and latent heat
(mW λ), respectively. Therefore, by using a heat transfer surface of the immersed
donut, the heat transfer was computed with Equation (28.7):
Q = [mD(CpD dT/dt) + mW(CpwdT + λ)] = UAs∆T (28.7)
A convective heat transfer coefficient was evaluated from the donut temperature
profile through the frying process and oil heating by using Equation (28.8):
dT
Q = m O Cp O = hA s (Toil − Tdonut ) (28.8)
dt
This differential equation can be solved with initial condition T = T0 for t = 0, as:
 T − Toil  hA s
ln  = t (28.9)
 T0 − Toil  moCpo
Thus, according to Rahman (1995), the values of h may be calculated from the
slope of the line by plotting ln [(T − Toil)/(T0 − Toil)] vs. t.
Thermal conductivity, volumetric specific heat, and thermal diffusivity were
measured with a Thermolink instrument (Decagon Devices Inc., Pullman, WA) at
room temperature.
Mass transfer diffusivity was evaluated by solving proposed differential equa-
tions (Crank, 1975) for two geometries: a hollow cylinder and a twisted infinite
cylinder. The internal radius (a) and external radius (b) were measured for this
purpose with a Vernier scale (Mod. Scala, MetroMex, México).
28.3.7 EXPERIMENTAL DESIGN AND DATA ANALYSIS

A factorial design with three temperatures (180, 190, and 200ºC) and nine to 13
sampling times was employed. ANOVA was conducted using specialized software.
Fitting models were obtained from Microcal Origin 3.0, CA-Cricket Graph III 1.5.2
and/or JMP SAS 3.02 versions.

28.4.1 MOISTURE AND OIL CONTENTS
The values for average moisture content of the donuts and its standard deviation as a
function of time at each oil temperature are presented in Figure 28.1 (a = 180°C; b =
190°C; c = 200°C). The oil content of donuts, including total and gained oil, during
the frying process is shown in Figure 28.2. The oil content was expressed in two ways:
total oil and gained oil (Figure 28.2, above and below, respectively). The latter was
obtained as the difference between the total oil content and the dough oil content.
The evaporation rate was higher during the first 30 sec of frying, becoming fairly
constant as the process continued. Moisture transfer during the frying process
appears to be similar to a drying profile, with an initial rapid fall period followed
by a constant drying stage, with a shorter initial period at higher temperatures. This
double mass transfer rate has been commonly observed in deep fat frying products
such as potato slices (Gamble et al., 1987), tortilla chips (Moreira et al., 1995), and
tapioca chips (Vasanti et al., 1996), and also for bakery products such as biscuits
(Turhan and Ozilgen, 1991).
Similarly, the oil uptake increased with the frying time and in reverse order to
temperature (Figure 28.2, below), exhibiting a rapid increase during the first 30–45
sec, which can be attributed to replacement of the evaporated water. In the last part
of the curve at all three temperatures, an apparent oil desorption was observed. This
increasing trend of oil content and gained oil as a function of frying time agrees
with findings by other authors (Gamble et al., 1987; Ateba and Mittal, 1994; Moreira
et al., 1995), but disagrees with findings on temperature effect on snacks such as
amaranth, black gram, and green gram prepared from some cereals and legumes
(Annapure et al., 1998). In the final stages of the process an apparent desorption
was observed at the three studied temperatures; the structure of the food was
compacted and did not admit more fat sorption in the puffed space. This effect was
also observed by Balasubramanian et al. (1995) for chicken nuggets and by Ateba
and Mittal (1994), who reported that the oil desorption was due to capillarity action.
28.4.2 HEAT TRANSFER

The heat transfer phenomenon was driven by two physical aspects; the first was the
sensible energy required to heat the donut from an initial temperature to the boiling point;
the second thermal change was the energy needed to evaporate water at the boiling point.
The requirements of sensible heat decreased as the frying process developed,
and vaporization heat was dependent upon the amount of evaporated water. The
temperature history of the solid ring center of the donut and the frying oil are given
in Figure 28.3, at the three experimental temperatures (a = 180°C; b = 190°C; c =
200°C). The central ring temperature increased rapidly at the beginning and pla-
teaued at around 90–105°C from 60 to 180 sec, depending on the oil temperature.
This profile is basically due to unstable heating of the sample and the water evap-
oration phenomenon from the surface. Within the experimental conditions studied,
a difference between the asymptotic sample temperature and the oil temperature was
recorded, in which the central temperature of the samples never reached 93 for

38
36
Moisture content (%wb)

experimental average
34
@180°C
32
Fitting (log)
30
28
26
24
22
20
0 15 30 45 60 75 90 105 120 135 150 165 180
Frying time (sec)
(a)
38
36
experimental average
34 @190°C
32 Fitting (log)
30
28
26
24
22
20
0 15 30 45 60 75 90 105 120 135 150 165 180
Frying time (sec)
(b)
40
38 experimental
36 average @200°C
34 Fitting (log)
32
30
28
26
24
22
20
0 15 30 45 60 75 90 105 120 135 150 165 180
Frying time (sec)
(c)
FIGURE 28.1 Moisture transfer profiles of donuts during deep fat frying at three oil tem-
peratures: a) 180°C; b) 190°C; and c) 200°C.

18
16
Total content and gained oil (%)

14
180…C
12 190…C
200…C
180…C
10 190…C
200…C
8
0
0 20 40 60 80 100 120 140
Frying time (sec)
FIGURE 28.2 Oil content profile (total: above; gained: below) of deep fat fried donuts as
influenced by frying temperature and time.
180°C, 96 for 190°C, or 108 for 200°C, respectively. So, the observed asymptotic
sample temperature followed a trend with respect to the oil temperature, in contrast
to the temperature difference of 87, 94, and 92°C between sample and oil, respectively.
Thermal properties of donuts for each oil temperature, measured at different
frying times, are summarized in Table 28.1. Basically, the thermal conductivity was
constant for donuts (0.0968–0.0978 W/mºC), at the three temperatures and during
the entire frying process. The specific heat varied somewhat with oil temperature
and showed a small increase with process time. Thus, from the specific heat, tem-
perature difference, and evaporated water, the involved energy was evaluated, and
the overall heat transfer coefficient was computed (Equations (28.7) and (28.8)); the
obtained values are included in Table 28.1.
Even though the Biot number is large (>30), the lumped parameter approach
(Equation (28.9)) allows evaluation of the convective heat transfer coefficient. The
surface heat transfer coefficient changed for each experimental temperature (Table 28.1).
As expected, the heat transfer coefficient increased with oil temperature, in agree-
ment with Miller et al. (1994), who reported the corresponding coefficients for canola,
2
corn, palm, and soybean oils from 250 to 276 W/m °C, and with Vijayan and Singh
2
(1997), who employed surface heat transfer coefficients of 300 and 500 W/m °C for
simulation of the frying process for frozen foods.
Temperature predictions using Equations (28.7–28.9) exhibited error percentages
less than 12.5% for 180 and 200°C (Figure 28.3a and 28.3c). On the other hand, for
frying of donuts at 190°C, the error for temperature prediction was only 4.3%
(Figure 28.3b).

In order to determine the moisture diffusivities for water loss, the moisture content
profile was utilized, assuming a diffusional mechanism for mass transfer. Two
equations were obtained for diffusion in a cylinder; the corresponding differential

200
180
Donut temperature (°C)

160
140 average temperature
120 fitting
oil temperature
100
80
60
40
20
0
0 15 30 45 60 75 90 105 120
Frying time (sec)
(a)
200
180
160
average temperature
140 fitting
120 oil temperature
100
80
60
40
20
0
0 15 30 45 60 75 90 105 120
Frying time (sec)
(b)
220
200
180
160 average temperature
140 fitting
120 oil temperature
100
80
60
40
20
0
0 15 30 45 60 75 90 105 120
Frying time (sec)
(c)
FIGURE 28.3 Temperature profiles of donuts during deep fat frying at three oil temperatures:
a) 180°C; b) 190°C; and c) 200°C.

TABLE 28.1
a,b
Transport Properties and Computed Heat Transfer for Donuts during the Frying Process
Average Water Average
c 2 6 2
Time (sec) k (W/mºC) Cp (kJ/kgºC) Loss (kg) ∆T (ºC) Q (W) U (W/m ºC) D (× 10 m /sec)
d
180ºC h = 158.63
15–30 0.0978 (0.0005) 2.436 (0.011) 0.00121 151.08 255.89 216.31 1.361 (0.398)
45–75 0.0975 (0.0001) 2.714 (0.015) 0.00022 126.67 89.19 93.47 0.551 (0.121)
90–180 0.0974 (0.0001) 2.714 (0.015) 0.00030 96.83 50.61 75.63 0.295 (0.057)
d
190ºC h = 269.54
15–30 0.0972 (0.0002) 2.165 (0.005) 0.00135 146.08 310.14 253.62 1.434 (0.410)
45–75 0.0968 (0.0001) 2.539 (0.004) 0.00020 101.03 85.15 105.37 0.603 (0.135)
90–180 0.0972 (0.0001) 2.728 (0.006) 0.00023 88.95 25.16 35.54 0.326 (0.078)
d
200ºC h = 296.84
15–30 0.0974 (0.0001) 2.331 (0.003) 0.00135 169.64 293.20 222.76 1.060 (0.237)
45–75 0.0974 (0.0001) 2.647 (0.003) 0.00027 122.48 122.96 132.99 0.508 (0.106)
90–180 0.0970 (0.0001) 2.963 (0.003) 0.00027 95.60 28.46 37.15 0.282 (0.047)
a
Average of nine samples.
b
Values in parentheses are standard deviations.
c
Equation (28.7).
d
Equation (28.9).
equations (Equations (28.10) and (28.12)) proposed by Crank (1975) were solved for
the first series term, and solutions (Equations (28.11) and (28.13)) presented:
1. For a hollow cylinder (where r is a ring point [a ≤ r ≤ b]):
J 0 (aα n )U 0 ( rα n )
∞
C − C0
C1 − C0
= 1− π ∑ J
n =1 0
( n ) 0( n )
aα + J b α
(
exp − Dα 2n t ) (28.10)
with a = 0.0122 m, b = 0.0385 m, r = 0.02535 m, C0 = initial moisture con-

tent, and C1 = C2 = 0.
C = C0 (1.204314e −14205.8Dt ) (28.11)
2. For a twisted infinite cylinder:
∞
C − C1 exp( − Dα 2n t )J 0 ( rα n )
∑
2
= 1− (28.12)
C 0 − C1 a n =1
α n J1 (aα n )
with c = 0.0115 m, r = 0.00575 m, and C1 = 0.
C = C0 (1 − 1.07511e −42553.9 Dt ) (28.13)
Thus, the diffusion coefficients were evaluated for each sampling time, ranging
−7 −6 2
from 1.41 × 10 to 3.86 × 10 m /sec; the corresponding average mass diffusion
coefficients, obtained from the hollow cylinder solution, which had a better fit than
the twisted infinite cylinder, are included in Table 28.1. Mass diffusion coefficients
are not temperature dependent from the statistical viewpoint (α = 0.01); therefore,
−6
a D average of 1.285 × 10 was obtained, based on the first 30 sec of frying for
the three temperatures. D values were higher than those reported for other fried
products, such as potato (Rice and Gamble, 1989), tortilla chips (Moreira et al.,
1995), sausage (Dincer and Yildiz, 1996), and chicken strips (Vélez-Ruiz et al.,
2001), as a consequence of differences in moisture content, product porosity and
structure, and product shape, among other variables.
Mass diffusion coefficients exhibited a decreasing trend for the three periods at
each temperature. As expected, this decreasing trend as a function of frying time
indicates a moisture content less available for evaporation and a higher internal
resistance due to structural changes of the donut. Moisture content predictions using
the solution for the hollow cylinder are better than for the twisted infinite cylinder,
with errors less than 10.5% in comparison with the predicted values obtained for
the other geometry.

28.4.4 EXPERIMENTAL CORRELATIONS
Based on the central temperature, average moisture content, average gained oil, and
measured thermal properties of donuts, some empirical models were generated for
each frying temperature. Of the applied mathematical relationships, one fitted the
experimental data very well. The best fitted equations are included in Table 28.2,
corresponding to each frying temperature.
The aforementioned parameters were fitted by different mathematical relation-
ships. Central temperature was well fitted (r = 0.99) by a linear equation (Equations
(28.14–17)), though the frying time was only 120 sec; furthermore, the central
temperature profile was described by two linear trends for 190 and 200ºC. For the
whole frying process (180 sec), the moisture content was adequately fitted (r ≥
0.92) by logarithmic relationships (Equations (28.18–20)), whereas the gained oil
was fitted (r ≥ 0.92) by quadratic equations (Equations (28.21–23)) at the three
oil temperatures.
Additionally, the average moisture content and average oil content of donuts
(Table 28.2) were correlated to the square of the frying time as proposed by Gamble
et al. (1987); as expected, the fitting was better than the log model used. In com-
parison with the obtained logarithmic equations, for moisture content at 180 and
200ºC and for oil content, the regression values were very good, r = 0.93, 0.96, and
0.95 for 180, 190, and 200ºC, respectively. The relationship between moisture loss
and oil absorption of donut samples and the square root of frying time suggests a
convective mass transfer controlled exchange. In such an exchange the outer water is
rapidly lost, generating a stream of vapor bubbles and producing a dry surface. This
external dryness provides a diffusion gradient favoring the moisture transfer from
internal cells, and then oil may adhere to the donut and enter free spaces formed as
the water escapes.
Also, for practical purposes, both moisture and oil contents for donuts were
correlated and the corresponding equations are also included in Table 28.2 for each
frying temperature; thus, if the moisture content is measured, the oil content may
be quickly quantified by means of these generated equations (Equations (28.30–32)).
28.5 CONCLUSIONS
The process of immersion frying of donuts was studied experimentally at three oil
temperatures. After investigation of the effects of temperature, moisture, oil, and
transport properties, it was concluded that all parameters were influenced by two
variables: oil temperature and frying time.
The present study underlines the importance of the interactive effects of the two
frying variables on the heat and mass transfer phenomena and the physical properties
of donuts through the deep fat frying process. The analytical and empirical approaches
were satisfactorily employed to generate the corresponding mathematical relation-
ships of the donut parameters and properties given in this work.
Some of the presented data, such as thermal conductivity, diffusion coefficients,
and empirical correlations, can be employed in analogue food products in order to
predict or design deep fat frying processes and equipment.

TABLE 28.2
Empirical Relationships for Temperature, Moisture, and Gained Oil of Donuts during the Frying Process
Parameter Frying Temperature (°C) Best Equation r Time Range (sec) Equation
Central temperature 180 T = 22.72 + 0.505t 0.994 0–120 (28.14)

190 T = 17.77 + 1.035t 0.988 0–180 (28.15)
200 T = 21.69 + 1.415t 0.994 0–45 (28.16)
T = 80.67 + 0.155t 0.999 60–120 (28.17)
Moisture content 180 W = 36.99 – 5.57 log t 0.933 0–180 (28.18)
190 W = 37.03 – 5.95 log t 0.959 0–180 (28.19)
200 W = 39.61 – 7.48 log t 0.918 0–180 (28.20)
2
Gained oil 180 OG = 1.313 + 0.160t – 0.0010t 0.924 0–180 (28.21)
2
190 OG = 0.602 + 0.113t – 0.0005t 0.949 0–180 (28.22)
2
200 OG = 0.595 + 0.162t – 0.0012t 0.951 0–180 (28.23)
1/2 1/2
As a function of t 180 W = 34.09 – 0.790 t 0.960 0–180 (28.24)
1/2
190 W = 34.14 – 0.869 t 0.946 0–180 (28.25)
1/2
200 W = 33.27 – 0.833 t 0.962 0–180 (28.26)
1/2
180 O = 9.122 + 0.689 t 0.934 0–180 (28.27)
1/2
190 O = 7.519 + 0.650 t 0.958 0–180 (28.28)
1/2
200 O = 9.596 + 0.601 t 0.949 0–180 (28.29)
W/O relationship 180 O = 34.26 – 0.726 W 0.970 0–180 (28.30)
190 O = 28.50 – 0.593 W 0.955 0–180 (28.31)
200 O = 32.41 – 0.683 W 0.948 0–180 (28.32)
The obtained empirical models for donuts can be applied to make valid and
valuable predictions about central temperature, moisture, and oil contents, as well
as product dimensions in the different stages of deep fat frying. Good agreement
was observed between the proposed model and measured parameters at the three
experimental temperatures.
According to the results obtained in this investigation, donuts processed in our
laboratory could have been fried in 75–120 sec, in reverse relation to the oil tem-
perature. Therefore, we can conclude that it should be possible to produce fried food
products of any kind with desired quality attributes by using mainly controlled frying
process conditions. However, more research is needed to further elucidate the char-
acteristics of the heat transfer phenomena and the physical property changes incurred
during the frying process.
NOMENCLATURE
a Internal radius (m) (Equations (28.10) and (28.11), also in As)
2 2
As Heat transfer surface of the immersed donut, As = π(b – a ) +
(1/2)(2πeb + 2πea)
b External radius (m) (Equations (28.10) and (28.11), also in As)
c Infinite cylinder radius (Equation (28.13))
c0 Initial concentration (%),
c1 Surface concentration (%)
C Water content (kg of water/kg of sample) at any time t (Equations
(28.10–28.13))
C0 Initial moisture content (Equations (28.10) and (28.11))
C1 Moisture content at the internal part of the donut (kg of water/kg of
sample) (Equations (28.10) and (28.11))
C2 Moisture content at the external part of the donut (kg of water/kg of
sample)
Cp Specific heat (J/kgºC)
CpD Donut-specific heat (J/kgºC)
CpO Oil specific heat (J/kgºC)
CpW Specific heat of water (J/kgºC)
d Slice thickness (m) (Equation (28.1))
2
D Diffusivity or mass diffusion coefficient (m /sec) (Equation (28.1))
2
Da Apparent diffusion coefficient (m /sec)
dT/dt Profile temperature
e Donut thickness in As (m)
i, j, k Direction vectors in the x, y, and z direction, and n is the present time
(Equation (28.6))
I, II Crust region and core region (Equations (28.2–28.5))
2
h Convective heat transfer coefficient (W/(m °C))
J0 Bessel function of first kind of order zero
J1 Bessel function of the first kind of first order
k Effective thermal conductivity (W/mºC)

2/3
m Modulus proportional to δt/(δxδyδz) (Equation (28.6))
mD Mass of donut (kg)
mW Mass of evaporated water (kg)
mO Oil mass (kg)
n Number of series terms
2
N Flux of the liquid water (kg/m sec)
O Oil content (%)
OG Gained oil (%), OG = oil content of donut – initial oil of dough
P Pressure (Pa)
Q Energy gained by the donut (W)
r Point in the donut ring (a ≤ r ≤ b), (m)
t Time (sec), incremental time (Equation (28.6))
T Temperature (ºC)
T(i, j, k, n) Temperature at i, j, and k at time n (Equation (28.6))
∆T temperature difference, ∆T = Toil − Tdonut
2
U Overall heat transfer coefficient (W/m °C)
U0 (rαn) equal to J0(rαn) Y0(bαn) − J0(bαn) Y0(rαn), and αns are the positive
roots of U0(rαn) = 0, Y0 is the Bessel function of second kind of order zero
w Moisture content (% w.b.) (Equation (28.1))
x Transfer direction (m)
2 2/3
xd Equal to (δy × δz/δx )
2 2/3
yd Equal to (δx × δz/δy )
2 2/3
zd Equal to (δx × δy/δz )
σ Liquid water fraction
3 3
ε Volume fraction (m /m )
γ Water vapor fraction
φ Oil fraction
σ Solid fraction
3
ρ Density (kg/m )
λ Vaporization heat of water (2256 J/kg)
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Influence of Liquid
29 Water Transport on
during Deep-Fat Frying
O. Vitrac, A.-L. Raoult-Wack, and G. Trystram
CONTENTS
29.1 Introduction
29.2.1 Calcium Alginate Gels
29.2.2 Frying Equipment
29.2.3 Temperature Measurements inside the Frying Material
29.2.4 Geometry of the Frying Material
29.2.5 Kinetics of Water Losses
29.2.6 Procedure to Assess Water Losses in Liquid State
during Frying
29.3.1.1 Kinetic of Water Losses
29.3.1.2 Mass Flow Rate of Water at the Exchange Surface
29.3.2 Temperature Distribution
29.3.2.1 T∞ = 120°C
29.3.2.2 T∞ = 180°C
29.3.3 Assessment of Liquid Water Mobility in Gel Slices
29.4 Conclusion
Nomenclature
References
29.1 INTRODUCTION
Deep-fat frying is one of the most common unit operations used in the preparation
of cooked, dried, textured, and formulated foods such as fish, chicken, and vegeta-
bles, especially potatoes. This unit operation may be also used for unconventional
applications such as a texturization step for oily materials prior to oil extraction

(Hounhouigan et al., 1997), dehydration of fruits by vacuum frying (Aw et al., 1998),
and drying and formulation of wood (Vitrac et al., 1999).
This unit operation is carried out by immersing materials with a high water
content in hot oil, with the temperature generally ranging between 30 to 80°C above
the boiling point of water. As a result, both high temperature and high oil density
lead to a high heat transfer rate between the oil and the wet material. Furthermore,
steam bubbles escaping from the material surface are gassed, drastically improving
heat transfer (Farkas and Hubbard, 2000).
Materials subjected to severe surface temperature and heat fluxes undergo var-
ious physicochemical and biochemical changes related to internal vaporization of
water. Short frying times lead to final products with a dried crispy exterior, which
contrasts with a soft and rich crumb, such as French fries or doughnuts. Long frying
times lead to products made of a continuous dried crust, such as chips or crisps. In
both cases, the final structure, achieved by water removal, influences final texture
(Pinthus et al., 1995, 1998) and oil absorption during the cooling stage (Ufheil and
Escher, 1996; Saguy et al., 1997; Moreira et al., 1997).
However, the effect of such a structure on heat and mass transfer during frying
has not been assessed very much. Until now, it was assumed that the steam flowed
through the dried porous crust following a pressure gradient and that the liquid water
migrated in the saturated region according to a diffusional (Farkas et al., 1996) or
a capillary mechanism (Ni and Datta, 1999). The regions would have been separated
by a dehydration front moving toward the center of the material. Such a hypothesis
was attractive since it offered a simple distribution of vaporization location inside
the frying material and opened the way to a macroscopic modeling of heat and
mass transfer during frying (Mittelman et al., 1984). Recent results suggest that the
position of the theoretical moving vaporization front, such as in chip making, might
not be proportional to the vaporization rate, since no increase in the inner thermal
resistance, as well as no decrease in the convective heat flux, were observed in
cassava slices with thickness ranging between 1 and 2 mm (Vitrac, 2000; Vitrac
et al., 2001).
The objective of this work is to test an alternative assumption, according to
which liquid water may be transported inside the material (sometimes with high
relative velocity) during frying following total pressure and deformation gradients,
and not by a diffusion-like mechanism as previously described in the literature.
Indeed, during other operations of intense drying, this transport of water is known
to occur significantly in the following situations:
High permeability of the solid matrix to vapor and liquid water

High friction losses in the porous material leading to filtration of liquid water
towards the outer surface driven by the inner steam overpressure
Failures in the solid matrix
In order not to induce any pressure release by intrusive measurements, experi-

ments were carried out on formulated thermostable gels (calcium alginate gels)
enabling embedding instruments inside the material. Moreover, to widen the investigation
scope, two model gel materials with the availability of water for transport were tested.

29.2.1 CALCIUM ALGINATE GELS
Calcium alginate (type SG 300, SKW System, France) gels without starch, denoted
S0, or with potato native starch (23% wet basis), denoted S1, were made in the
presence of tetra-sodium-diphosphate as calcium chelatant. Their final water contents
were, respectively, 73 and 93% w/w (wet basis). Gels were prepared at 55°C, cast
in Teflon cylindrical molds (80 mm diameter × 5 mm long) including prepositioned
thermocouples. After gelification, the location of the sensors was observed through
gels under intense lighting. The gel cylinders were then secured together with their
Teflon mold to a rigid anchoring apparatus that was used to immerse and hold gels
vertically under the oil surface.
29.2.2 FRYING EQUIPMENT

A large household deep fat fryer, filled with 5 kg of palm oil, and supplied with a
1600 W submerged electrical resistance, was used in all tests. The frying temperature
was controlled by a numerical proportional-integrated-derived (PID) controller using
the average of five type T thermocouples located at different depths in the oil bath.
All the acquisitions (acquisition rate of 5 Hz) and controls were programmed on
LabView 5.0 (National Instruments, Austin, TX) and achieved respectively with a
high precision temperature data logger (model PC4350 for ISA bus, National Instru-
ments) and a multifunction analog I/O data acquisition card (model ATMIO16E for
ISA bus, National Instruments) connected to a thyristor power controller (model
TE10A, Eurotherm, France).
29.2.3 TEMPERATURE MEASUREMENTS INSIDE THE FRYING MATERIAL

An approximation of the temperature profile inside the frying material was obtained
by the temperatures of three K micro-thermocouples (∅ = 0.25 mm) located at
various depths in 5 mm gel slices.
29.2.4 GEOMETRY OF THE FRYING MATERIAL

An approximation of the geometry of the slice immediately after frying (2 to 4 sec)
was obtained by three-dimensional reconstruction (i.e., by creating a three-dimen-
sional photorealistic computer model of the real fried slice). Our technique combines
distance measurements and 16-bit digital pictures (resolution 640 × 480) carried out
with a 5 × 5 laser grid generator and a digital camera (model QuickCam Pro,
Logitech, Fremont, CA), as described in Figure 29.1.
The heights of the 25 vertices projected on each slice surface were measured
by triangulation according to Equation (29.1) and notations presented in Figure 29.1

FIGURE 29.1 Methodology for three-dimensional reconstruction of slices immediately after
frying: (a) experimental device: (b) principle of three-dimensional reconstruction with a
reference plane (step 1: reference image, step 2: slice image, step 3: three-dimensional
deformation of image 2); (c) orthogonal basis for triangulation; (d) principle of displacement
field analysis between two images (local and global).
by comparing pictures with and without samples.
 d(1115, ) tan(β + δ ) − tan δ

 β such as : =
2 δ
 d( 5,25) tan
 cos β 2

 α i = arcsin[cos(β + y i δ ) cos(x i δ)] (29.1)

 h i = tan(α i )d( Pi , Q i )( O,x,y )

where δ is the angle of the laser cone (here 9.6°) and d is the Euclidian distance
operator.

Calibration was carried out on rough and smooth samples with known geometries
with 0.1 mm accuracy. The three-dimensional computed models of the initial and
fried slice were used to assess the global shrinkage of the slice in volume and in
cross section. In particular, it was verified that additional shrinkage was not observed
during the few seconds required to remove the slice from oil and to position it under
the laser and camera device.
29.2.5 KINETICS OF WATER LOSSES

Water content of gels was obtained after frying and draining on paper towel by
drying a 5 g sample for 24 h at 103°C in an air oven. The water content of each
slice was expressed in kg of water per kg of nonfat dry solids, noted WS, according
to Equation (29.2).
W(t)
WS( t ) = η( t ) ⋅ (29.2)
1 − W0
(t) 0
where W and W are the water content on a wet basis, respectively, at time t and
(t)
t = 0 and η is the apparent frying yield (i.e., the ratio between final and initial slice
masses) at time t. Kinetics of water losses were smoothed using an infinite sum of
exponential decays as follows:
n t
−
WS( t ) ≈ WS∞ + ∑i =1
λi ⋅ e τi
(29.3)
where WS∞ = water content at thermal equilibrium with oil.

Nonlinear parameters (τi ) were adjusted by a direct research method (Nelder
and Mead’s simplex), whereas linear parameters (λi) were computed from a New-
ton least square method. The development order n was defined by the rank of the
covariance matrix computed after QR decomposition (generally order 2 or 3 was
required). Equation (29.3) was used to compute the flow rate of water at the
−2 −1
exchange surface in kg⋅m ⋅s (qm) in both liquid and steam states from Equation
(29.4).
dWS( t ) 1 dWS
(t)
q (mt) = ρS( t ) ⋅ E ( t ) ⋅ = ρS0 ⋅ E 0 ⋅ ( t ) ⋅ (29.4)
dt αΣ dt
−3 (t)
where ρS( t ) = apparent solid density (kg of nonfat solids ⋅m of slice), E = half
thickness of the slice, and α (Σt ) = cross-section shrinkage of the slice.
29.2.6 PROCEDURE TO ASSESS WATER LOSSES IN LIQUID STATE

DURING FRYING
Gel slice cylinders were deep fat fried in a 2 kg sedimentation flask filled with 1 kg
of palm oil previously heated to 180°C, as shown in Figure 29.2. The sample was
maintained immersed at the top of the flask while digital pictures (resolution 640 × 480)

FIGURE 29.2 Procedure to visualize liquid release from gel slices (a) during frying, (b) after
cooling. (c) Detail of liquid water volume recovered at the bottom of the flask.
of the flask bottom were recorded at 10 Hz using a digital camera (model QuickCam
Pro, Logitech, Fremont, CA) with contrasted lighting. After 60 sec of frying, 1 kg of
palm oil at room temperature (20°C) was added to reduce the oil temperature below
the boiling point. Then, the heavy liquid recovered from the bottom of the flask was
removed and centrifuged. The supernatant was eliminated with a pipette, and the
remaining volume of water was measured. It was also verified that liquid did not
come from possible steam condensation at the top of the flask.

29.3.1.1 Kinetic of Water Losses
Figure 29.3 presents the residual content of 5 mm thick cylinders vs. frying time at
120, 150, and 180°C for both formulations, S0 and S1. Each point was achieved from
mass balance over an individual slice of gel. As previously described by Baumann
and Escher (1995), immersion in hot oil led to an intense drying that was variable

FIGURE 29.3 Kinetics of water losses during deep-fat frying of 5 mm thick gel slices
formulated without (S0) and with (S1) starch.
between samples. Dispersion was higher when the water content decreased sharply;
this was interpreted as a high sensibility of transfers to initial frying conditions or
material behavior.
Respective to formulations S0 and S1, this initial high drying rate was followed
by shrinkage of about 30 and 20% in the radial direction and of about 25 and
10% in the transverse direction after the vaporization of 50% of initial water
content. Further drying did not induce significant additional shrinkage regardless
of the frying temperature. Hence, the porous solid structure was not apparently
deformable.
The assessed drying kinetics confirmed trends that have been previously
observed on real materials of similar geometry, in particular exponential decay of
water content and higher drying rates when the oil temperature is higher. Thus, half
of the initial water content was removed during the first 3 min of frying at 120°C
(oil temperature 20°C above the boiling point of water) for both S0 and S1 gels. For
the S1 gel, this time duration was divided by two and three when the difference of
temperature between the oil and the boiling point of water increased respectively
up to 2.5 (at 150°C) and 4 times (at 180°C).

FIGURE 29.4 Flow rate of water (liquid and steam) at the exchange surface vs. residual
water content during frying of 5-mm thick gel slices formulated without (S0) and with (S1)
starch.
For the S0 gel, this typical time duration at 120°C was drastically reduced by 6
down to 30 sec for temperatures greater than or equal to 150°C. However, the kinetics
of the S0 gel presented other unusual features, such as:
1. Higher drying rates for S0 gel than for S1, whereas the initial water content
in S0 gel was 24% higher (m/m wet basis) than in S1 gel
2. Similar drying kinetics of S0 gel when the residual water was above 40%
of the initial water content and oil temperature ranged between 150 and
180°C
These results suggest that the mechanisms of heat and mass transport responsible
for gel dehydration might be different at temperatures above 150°C than at 120°C.
Moreover, the intensity of mass transfer would be much higher for the S0 gel than
for the S1 gel since the drying time of the S0 gel was shorter, and the initial amount
of water reported to solid mass was four times higher.
29.3.1.2 Mass Flow Rate of Water at the Exchange Surface
Figure 29.3 shows the mass flow rate of water per unit of area (qm) vs. residual water
content computed from discrete water losses (see Figure 29.3) and by taking into
account the modification of surface exchange area due to the slice shrinkage. The
curves confirmed that at the initial state of frying a significant amount of water was

vaporized at an almost constant rate for both formulations. However, for similar
external conditions and surface area, qm values were more than twice as high for
the S0 gel than for the S1 one.
For the S1 gel and different external conditions, maximum values were almost
in the expected proportion of temperature difference between oil and saturation (T∞ −
Tsat). In the S0 gel, the effect of external conditions was less significant when the
oil temperature was higher.
The low curvature of qm vs. WS implies that transfers were controlled by a
combination of internal and external conditions and not only by the thickening of
the dried region (Derdour et al., 2000). If we assume that only the external conditions
prevail when a constant rate is achieved with a surface temperature of about Tsat,
the convective heat transfer coefficient is given by:
q max
h max = ∆H v m
(29.5)
T∞ − Tsat
6 −1
where ∆Hv = latent heat of water vaporization (2.44⋅10 J⋅kg ).
Equation (29.5) implies that water losses can be achieved only by internal or
3 −2 −1
superficial vaporization. This has led to maximum values of h over 8.5⋅10 W⋅m ⋅K ,
3 −2 −1
increasing with T∞ up to 2.5⋅10 W⋅m ⋅K . For both formulations, such results were
quite unexpected, since:
• The magnitudes were twice to ten times higher than those generally cited
in the literature, with maximum values between 0.4 and 0.8 (Costa et al.,
3 −2 −1
1999) and 1.1⋅10 W⋅m ⋅K (Farkas and Hubbard, 2000; Hubbard and
Farkas, 1999) when the vaporization rate is maximum.
• Both external and internal resistances were significantly lower at higher
temperature.
Thus, the drying behavior of the material during frying might depend not only
on external conditions (heat flux, temperature) and the amount of residual water, but
also on the ability of liquid water to migrate towards the exchange surface. In particular,
it was demonstrated that, in the case of materials with high initial water content,
migration of liquid water according a total pressure gradient could be significant
(Vitrac et al., 2000; Vitrac, 2000; Ni and Datta, 1999). Microscopic observations
also showed that the difference in frying material behavior according to oil temper-
ature could also be related to different physicochemical modifications of the
exchange surface, such as transition from rubbery to glassy state resulting from a
competition between heating and intense drying.
29.3.2 TEMPERATURE DISTRIBUTION

In order to assess heat transfer within slices, the temperature distribution at three
different vertical positions was measured during frying for both compositions and
for two extreme frying temperatures, 120 and 180°C. The results are given in
Figure 29.5 for an initial slice temperature of 25°C.

FIGURE 29.5 Temperature distribution in 5-mm thick gel in function of gel formulation and
frying temperature: (a) S0 gel, 120°C; (b) S1 gel, 120°C; (c) S0 gel, 180°C; (d) S1 gel, 180°C.

29.3.2.1 T∞ = 120°C
At low temperature (120°C), similar distributions were measured for both compo-
sitions. After a rapid increase above the boiling point, the temperature remained
approximately constant somewhat above 100°C. The duration of the temperature
plateau was longer when the thermocouple probe was deeper in the material. It was
assumed to correspond to a temperature of a gel core (or crumb) filled with free
water, the volume of which was decreasing progressively as the vaporization front
moved deeper inside the material. When the thermocouple was located behind the
drying front, its temperature increased rapidly up to the oil temperature.
Note that after the surface temperature reached the boiling point of water at
atmospheric pressure inside the material, it increased and seemed to remain between
110 and 115°C for a short time before returning more or less rapidly to the boiling
point of water at atmospheric pressure. Such a situation was observed in all condi-
tions and was sometimes followed by an inflexion in temperature profile character-
ized by the center temperature overtaking the intermediate temperature
(Figure 29.5a). This outstanding but significant phenomenon should be interpreted
as reflecting transient shifts in liquid–vapor water equilibrium induced by a local
increase in total pressure inside the material leading to radial heterogeneity in
longitudinal temperature profile. In fact, an overpressure front would start close to
the surface and move with the vaporization front towards the center of the material
(Perré et al., 1993; Vitrac et al., 2000).
The overpressure value would be strongly dependent on values of steam perme-
ability in the crust, the drying rate, and the distance between the evaporation location
and the surface. At the beginning of frying, it would not exceed 70 or 80 kPa
(corresponding to an increase in boiling temperature of about 15–20°C) and would
be maximal at the center of the slices during the rest of frying, with values between
30 and 40 kPa (corresponding to an increase in boiling temperature of about 5–10°C).
Inflexion in temperature profile or disruptions in variation of temperature with time
would be the result of a pressure release caused by the opening of cracks (experi-
mentally observed after frying) at the material surface.
Such a mechanism would dramatically affect the spatial distribution of vapor-
ization locations by enhancing moisture migration on the way to the outer surface,
in particular close to the cracks. Thus, this transport would prevent the outer surface
from a temperature increase (i.e., a significant overheating above the boiling point)
and induce an apparent cooling effect.
29.3.2.2 T∞ = 180°C
At higher temperature (180°C), similar phenomena were reproduced with similar

overpressure effects. However, different temperature profiles were significantly
obtained for both formulations.
The temperature gradient in S1 gel slices did not exceed 20°C on half thickness
(2.5 mm), while it was three times higher in S0 gel slices. Thus, strong differences in
S0 gel matrix structure and water content were observed between the outer surface and
the center. Two minutes after frying, the outer surface was dry and highly porous,

whereas the crumb was apparently not very different from the initial gel. Such high
differences between the temperature profiles in S0 and S1 gel slices were unexpected,
since the drying rate value at the “almost constant drying rate period” was at least
twice as high as in S0 gel than in S1 (Figures 29.3 and 29.4). Indeed, in S1 gel the
temperature difference between the outer surface and oil, to which the overall heat
transfer rate was proportional, was about 60–70°C, while it was only about 20–25°C
in S0 gel slices.
Many hypotheses could be put forward:
1. Higher convective heat transfer coefficient in gel with higher water content
caused by higher bubbling intensity
2. Steam film (of low thermal conductivity) surrounding gel slices that would
reduce heat transfer in S1 gel slices and prevent them from superficial
overheating
3. A penetration front of oil into the material during frying
4. A strong mechanism of liquid water transport toward/up to the outer
surface occurring during frying that would partially uncouple heat and
mass transfer
The first hypothesis assumes that only external heat transfer would control the
drying rate and that the inner thermal resistance would be nonsignificant, and that was
not compatible with a high temperature gradient within slices. The second hypothesis
does not agree with the experiment, since no slug or film steam flow was observed
during frying of S1 gel slices; moreover, such flows would be more probable at very
high drying rates, such as those determined during frying of S0 gel slices. In the same
manner, oil migration into a wet material vs. steam flow and a total pressure gradient
was not realistic during frying and in contradiction with the literature. Thus, the last
hypothesis was retained by default. However, it brought forth two questions:
1. Why were more noisy data obtained for the outer temperature surface of
S0 gel slices (whatever the replication)?
2. Why were possible water losses in the liquid state not followed by tem-
peratures around the boiling point (maximal theoretical temperature of
the liquid phase)?
29.3.3 ASSESSMENT OF LIQUID WATER MOBILITY IN GEL SLICES

Finally, so as to determine if the previously assessed transport of a significant amount
of liquid water decreased drastically close to the outer surface or was able to cross
the porous dried crust, the amount of liquid water ejected directly in hot oil was
appraised with a modified frying device previously described. Figure 29.6 shows the
phenomenon observed at the bottom of the flask, twenty-five centimeters below the
location where the S0 gel slice was fried.
During the first 30 seconds, vapor bubbles ejecting from the gel slice were
observed at the top of the flask without noticeable changes at the bottom. At around
30 seconds after immersion in hot oil, falling droplets were observed, initially with
large diameter around 2–3 mm but quickly becoming smaller in size and higher in

FIGURE 29.6 Visualization of liquid water ejection during frying at 180°C of a 5-mm thick
gel slice formulated without starch (S0).
concentration. No further vaporization of the liquid recovering at the bottom of the

flask and denser than oil was noticed (no bubbles were seen rising at the bottom of
the flask). After the oil cooled below the boiling point, it was verified that the liquid
was water. After 1 minute of frying, 25 to 30% of the initial water of the slice was
recovered at the bottom of the flask. This experiment showed that at least 25% of
initial water was removed from the slice without vaporization and energy consump-
tion. Similar phenomena were observed in S1 gel, but during the same time period
the mass of liquid ejected without vaporization did not exceed 3 to 8% of the initial
mass of water at 180°C.
These results showed clearly that liquid water could be transported inside
frying material from the core on the way to the outer surface. Such a mechanism
enhanced heat and mass transfer during frying (1) by improving the convective
heat flux by protecting the temperature at the surface from heating significantly
over the boiling point, and (2) by allowing dehydration without requiring heat
consumption. Two conditions might influence this transport and therefore the
behavior of the frying material:
1. Materials with high permeability to steam (large pores, low tortuosity)

would also have a high permeability to liquid water (as S0 gel did) and
would then allow high liquid velocity flow within the dried zone
2. Materials that present, during frying, a well-defined and thick porous crust
(as the S1 gel did) would develop high-pressure gradients. They would
induce a gradual filtration of liquid water in the crust, the porosity and
the steam permeability of which would be reduced sharply by normal
stresses in the direction of water flow and by the presence of liquid water.
respectively.
In the first case described, the high velocity of liquid water flow relative to the
solid matrix would lead to unexpected phenomena such as nonthermal equilibrium
among all phases (solid, steam, liquid water) close to the outer surface. Thus, this
interpretation would explain why noisy surface temperatures significantly above the
boiling point were measured at the surface of S0 gel slices fried at 180°C, despite
the fact that a large amount of liquid water flowed through the surface. This phe-
nomenon, which was observed during frying of fruits (e.g., apple), as well as water

losses in the liquid state, would be responsible for a rapid heating and darkening of
the material surface. Starchy materials such as potato, cassava, or plantain (with
chip or French fry geometry) would belong to the second category (i.e., as S1 gels)
according to their behavior during frying.
According to these results, the limit condition of heat transfer at the exchange
surface in the form of Equation (29.5) should be modified in order to take into
account (1) high mass transfer rate at the exchange surface in both vapor and liquid
states and (2) possible partial uncoupling between heat and mass transfer at material
scale. The general limit condition could be written for equal temperatures among all
phases (condition of local thermal equilibrium) and a shrinking material as follows.
r r r r
[( k eff ∇T) + Γ( q m ) ⋅ ∆H v ⋅ ρl (v l − v S )] ⋅ n = h ( q m ) ⋅ (TΣ − T∞ ) (29.6)
where keff = effective thermal conductivity of the exchange surface, ρ1 = intrinsic

r r
density of water, v l and v S = averaged velocity of liquid water and solid matrix,
r
n = normal vector to the exchange surface, and TΣ = averaged surface temperature.
In Equation (29.6), Γ( q m ) is a phenomenological adimensioned coefficient that
takes a value between 0 and 1 depending on vaporization rate and the structure of
the frying material. For dense materials such as starchy products or wood (nonfood
application), Γ( q m ) would be close to 1. It would be lower than 1 for water-rich
materials such as fruits, vegetables, gels, and sludges (nonfood application). Meat
products could be intermediate.
29.4 CONCLUSION
Model gels formulated with (S1) and without (S0) starch were used to assess the
transport of liquid water within the material during deep fat frying. This transport,
not previously described in the literature, was proposed as a possible explanation of
some unexpected results concerning the overall drying kinetics or temperature of
the studied materials, such as apparent uncoupling between drying rate and heat
transfer rate. The mechanism of liquid water transport appeared in zones where
water was highly available (i.e., free water saturated zones) and was the consequence
of a total pressure gradient created by friction losses in steam flow escaping from
the frying material.
Thus, the large unsaturated volumes created in alginate gels made possible a
migration of liquid water in the crumb and towards the dried crust. In S1 gel slices,
this transport led at high temperature to a cooling effect of the outer surface,
improving convective heat transfer and minimizing the thermal gradient inside
the material. In materials with high porous crust and high liquid water mobility in
the crumb, such as S0 gel slices, a significant amount of liquid water appears to be
pushed outside the material without vaporization. In this last case, no cooling effect
was observed, and surface temperature remained at a temperature significantly higher
than the boiling point. These outstanding phenomena of nonthermal equilibrium
would be promoted by intense shrinkage (i.e., strong deformation gradient) and
ruptures in crust solid matrix, and underlined the complexity of the physics of frying.

According to these results, previous predictive models of frying unit operation
must be modified in order to be generalized to new materials (e.g., fruits, vegetables,
and gels) or new applications (e.g., frying of wood or sludge). A minimal modifi-
cation is proposed by introducing a new and more general heat transfer limit con-
dition for deep frying.
From the technological point of view, the results of partial uncoupling between
heat and mass transfer require complementary studies in order to:
1. Classify frying behaviors (i.e., levels of uncoupling between materials

with different composition and structure)
2. Assess the implication of such uncoupling on frying functionalities (i.e.,
drying, cooking, creation of structure/texture, formulation, microbial inac-
tivation) for food and nonfood materials and on the final product quality
(texture, coloration, aroma and vitamin losses, oil uptake, etc.)
3. Possibly improve such a mechanism of uncoupling and thus reduce heat
consumption for water removal during frying
NOMENCLATURE
E Half thickness [m]
O Origin
P Laser grid vertex on reference plane (Oxy)
Q Laser grid vertex at slice surface
T Temperature [°C]
−1
W Water content [kg⋅kg ]
d Euclidian distance operator
−2 −1
h Height relative to (Oxy) or convective heat transfer coefficient [Wm ·K ]
−1 −1
k Heat conductivity [Wm ⋅K ]
n Normal vector
−2 −1
q Mass flow rate per unit of area [kg⋅m ⋅sec ]
t Time (sec)
x Coordinate along (Ox)
y Coordinate along (Oy)
z Coordinate along (Oz)
GREEK SYMBOLS
−1
∆Hv Latent heat of vaporization of water [J⋅kg ]
2 −2
α OPS or OQS angle [rad] or cross-section shrinkage [m ⋅m ]
β Laser angle with (Oz) [rad]
δ Angle of laser cone [rad]
−1
η Frying yield [kg⋅kg ]
λ Amplitude coefficient of continuous in time water content approximation
−1
[kg⋅kg ]
−3 −3
ρ, ρ Intrinsic density [kg⋅m ], apparent density [kg⋅m ]
−1
τ Time constant of continuous in time water content approximation [sec ]

SUBSCRIPTS
eff Effective
i Index of vertices [1–25] or of coefficient
l Relative to mass flow of liquid water
m Relative to mass flow of water (liquid and vapor)
v Relative to mass flow of steam
s Relative to solid matrix
Σ Relative to slice cross-section
∞ Relative to oil (far from the slice)
EXPONENTS
0 Initial
∞ Infinite in time
REFERENCES
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Costa, R.M., Oliveira, F.A.R., Delaney, O., and Gekas, V., Analysis of the heat transfer
coefficient during potato frying, J. Food Eng., 39, 293–299, 1999.
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Numerical Simulation
30 of Transient
Two-Dimensional
Profiles of Temperature,
Concentration, and Flow
of Liquid Food in a Can
during Sterilization
A.G. Abdul-Ghani, M.M. Farid, and X.D. Chen
CONTENTS
30.1 Introduction
30.2 Computational Fluid Dynamics (CFD) and the Food Industry
30.3 Basic Model Equations and Solution Procedure
30.3.1 Computational Grid
30.3.2 Convection and Temporal Discretization
30.3.3 Computational Model and Governing Equations
30.3.3.1 Energy Balance
30.3.3.2 Momentum Balance in the z Direction
30.3.3.3 Momentum Balance in the r Direction
30.3.3.4 Continuity Equation
30.3.3.5 Mass Balance for Bacteria
30.3.3.6 Mass Balance for Vitamins
30.3.4 Kinetics of Deactivation of Bacteria and Destruction of Vitamin C
30.3.5 Assumptions Made in the Current Numerical Simulation
30.4 Temperature Measurements in the Can during Sterilization
30.5.1 Flow Pattern
30.5.2 Slowest Heating Zone (SHZ) and Temperature Profile
30.5.3 Concentration Profiles of Bacteria and Vitamins
30.6 Conclusions

Nomenclature
Acknowledgments
References
30.1 INTRODUCTION
Canning is one of the most effective means of food preservation, and it is used to
preserve a large part of our food supply. Despite significant advances in food
processing operations involving the use of thermal energy, conventional thermal
sterilization is still common. Thermal sterilization is the process of heating at a
specified temperature/time to eliminate pathogenic spores from the food product.
In the canning industry, this process usually involves the application of steam to
heat the food in the can to a given temperature; the can is then held at that
temperature for a period sufficient to kill the microorganisms. The sterilization
process not only extends the shelf life of the food, but also affects its nutritional
and sensory quality. One of the challenges to the food canning industry is to
minimize these quality losses, meanwhile providing an adequate process to achieve
the desired degree of sterility. The optimization of such a process is possible
because of the strong temperature dependence of bacterial spore inactivation as
compared to the rate of quality destruction, sensory as well as nutritional (Lund,
1977). For this reason, an estimate of the heat transfer rate is required in order to
obtain optimum processing conditions and to improve product quality. Also, a
better understanding of the mechanism of the heating process will lead to improved
performance in the process, and perhaps to energy savings. Basic principles for
determining the performance of different but related processes have been presented
by May (1997) and Wilbur (1996).
Foods such as canned tuna, thick syrups, purees, and concentrates are usually
assumed to be heated by pure conduction. For these foods, the required processing
time is generally determined by analytical or numerical solution to the heat conduc-
tion equation (Datta et al., 1986). For example, Dincer et al. (1993) studied transient
heat transfer during sterilization of canned foods using a conduction equation with
constant wall temperature as a boundary condition. Lanoiselle et al. (1986) devel-
oped a linear recursive model to represent the heat transfer inside a can during
sterilization in a retort and predicted the internal temperature distribution in canned
foods during thermal processing. Akterian (1994) developed a numerical model for
the determination of the unsteady state temperature field in conduction heated canned
foods of various shapes and boundary conditions.
A number of numerical heat transfer studies have been conducted to model
sterilization, taking into account the effect of natural convection. Datta and Teixeira
(1987, 1988) predicted transient temperature and velocity profiles during natural
convection heating of canned liquid foods. They also predicted distinct internal
circulation at the bottom of the can and showed that the slowest heating zone is
a doughnut-shaped region located near the bottom of the can at about one tenth
of the can height. Kumar and Bhattacharya (1991) carried out a simulation of the
sterilization of viscous liquid food in a metal can in an upright position and heated

from the side wall (T = 121°C) in a still retort. They also presented a simulation
of the same can when its bottom and top surfaces were insulated (Kumar et al.,
1990). The results indicated that natural convection tends to push the slowest
heating region to the bottom of the can. The simulation of Ghani et al. (1998)
showed that the presence of an air gap at the top of a can filled with a viscous
liquid carboxymethyl cellulose (CMC) had no significant effect on the rate of
heating. This was due to the strong effect of the natural convection current, even
though the liquid was highly viscous. Ghani et al. (1998) also studied the effect
of the convective boundary caused by steam heating. The results were similar to
the constant wall temperature case, due to the high value of the heat transfer
coefficient of the condensing steam. This suggests that the assumption of constant
wall temperature is appropriate for any general-purpose simulation.
In the above simulations the temperature distribution at the end of the heating
process in the can was assumed to be an important measure of sterility of food
products. However, it is necessary to keep the food under that condition for a
specified period of time to ensure an efficient kill of microorganisms. In reality, the
death of microorganisms is expected to begin at an early stage of heating, especially
at locations near the wall, where the temperature approaches 121°C very quickly.
Hence, it is necessary to solve the partial differential equation governing bacterial
concentration, coupled with the equations of continuity, momentum, and energy.
Datta (1991) followed this approach to study sterilization of liquid food in a nonagi-
tated cylindrical enclosure heated from all sides and described the computational
procedure for obtaining the full range of biochemical changes during processing
without explicitly following the liquid elements. This author showed that the lowest
sterilization achieved by any portion of the fluid in the system was considerably
more than the sterilization level normally calculated by using the temperature of the
slowest heating zone (SHZ). In the analysis presented by Datta (1991), the bacteria
were assumed to undergo convective motion only (i.e., diffusion was neglected).
Ghani et al. (1999b) developed a computational procedure for describing the
changes in concentrations of live bacteria and their transient spatial distributions
during the sterilization process. In addition to convective transfer, the effect of
diffusion of bacteria in liquid food was also studied, and the bacteria were assumed
to diffuse in the liquid food following the modified Brownian diffusion equation.
It was found that the motion of bacteria was controlled by convective motion, and
that the diffusion effect was negligible. In this work, liquid food was tagged and
followed, which is computationally difficult for most flow situations of interest
(Datta, 1991).
Chemical and biochemical reactions in liquid food during heating are tempera-
ture dependent. Such reactions not only destroy microorganisms, but also some
valuable nutrients. Because such destruction processes are temperature dependent,
the distribution of temperature results in unavoidable spatial distributions of the
reaction products. These distributions can be easily quantified in the case of con-
ductive heating of solid materials. However, the situation becomes complex when
the fluid is in motion. In this case, temperature and concentration profiles are
influenced strongly by the natural convection in the liquid food (Ghani et al., 1999b).
The destruction of vitamins follows a first order reaction similar to microbial destruction.

In general, the value of the decimal reduction time (D), the time needed to destroy
90% of the microorganisms or a particle or food component is higher for vitamins
than for microorganisms and enzymes. As a result, nutritional proprieties may be
better retained by the use of higher temperatures and shorter times during heat
processing(Fellows, 1996). This was studied by Ghani et al. (1999c, 2000), in studies
in which more detailed mechanisms of heating in fluid motion were considered, and
the effects of increasing sterilization temperature on deactivation of bacteria and
vitamin C destruction were analyzed.
30.2 COMPUTATIONAL FLUID DYNAMICS (CFD)

AND THE FOOD INDUSTRY
CFD offers a powerful design and investigative tool to process engineers. Its appli-
cation would assist in a better understanding of the complex physical mechanisms
that govern the thermal, physical, and rheological properties of food materials. CFD
has only recently been applied to food processing applications. CFD has seen
applications in many different processing industries, including airflow in clean rooms,
ovens, and chillers; flow of foods in continuous-flow systems; and convection patterns
during thermal processing (Scott and Richardson, 1997).
The observation of the slowest heating zone is a difficult task and requires
knowledge of detailed transient flow patterns and temperature profiles, due to the
complex nature of heat transfer in natural convection heating. The partial differential
equations governing such a system need to be solved in their entirety using numerical
techniques. In this work, sterilization of canned liquid food (carrot–orange soup) in
a still retort was studied and analyzed using CFD. The results were presented in the
form of transient temperature, concentration, and velocity profiles. The PHOENICS
code used in this work is based on the finite volume method, as developed by
Patankar and Spalding (1972). The key characteristic of this method is the immediate
discretization of the integral equation of flow into the physical three-dimensional
space, i.e., the computational domain covers the entire can, which is divided into a
number of divisions in the three dimensions. The details of this code can be found
in the PHOENICS manuals, especially the PHOENICS Input Language (PIL) manual.
30.3 BASIC MODEL EQUATIONS AND SOLUTION

PROCEDURE
30.3.1 COMPUTATIONAL GRID
The boundary layer at the heated walls and its thickness are important parameters
of the numerical convergence of the solution. Temperature and velocities have their
largest variations in this region. To adequately resolve this boundary layer flow, i.e.,
to keep discretization error small, the mesh should be optimized, and a large con-
centration of grid points is needed in this region. If the boundary layer is not resolved
adequately, the underlying physics of the flow will be lost, and the simulation will

be erroneous. On the other hand, in the rest of the domain, where the variations in
temperature and velocity are small, the use of a fine mesh will lead to increases in
computation time without any significant increase in accuracy. Thus, a nonuniform
grid system is needed to resolve the physics of the flow properly (Ghani et al., 2000).
A nonuniform grid system was used in the simulation with 3500 nodal points:
70 in the axial direction and 50 in the radial direction, graded in both directions
with a finer grid near the wall. The computations were performed for a can with a
radius of 0.037 m and height of 0.11 m. The can’s outer surface (top, bottom, and
side) was heated at a constant temperature (121°C) throughout the heating period.
The natural convection heating of carrot–orange soup was simulated for 3000 sec.
Ten steps were taken to achieve the first 200 sec of heating, another 10 steps to
reach 1000 sec, and 30 steps for the total of 3000 sec of heating. This required 4 h
of CPU time on the UNIX IBM RS6000 workstations at the University of Auckland.
Solutions were obtained using a variety of grid sizes and time steps, and the results
show that the solutions are time-step independent and weakly dependent on grid
variation.
30.3.2 CONVECTION AND TEMPORAL DISCRETIZATION

An important consideration in CFD is the discretization of the convection terms in
the finite volume equations. The accuracy, numerical stability, and boundedness of
the solution depend on the numerical scheme used for these terms. The central issue
is the specification of an appropriate relationship between the convected variables
stored at the cell center, and its value at each of the cell faces (Malin and Waterson,
1999). The convection discretization scheme used for all variables in our simulations
was the hybrid-differencing scheme (HDS). The HDS of Spalding (1972), used in
PHOENICS, switches the discretization of the convective terms between central
differencing scheme (CDS) and upwind differencing scheme (UDS), according to
the local cell Peclet number.
The cell Peclet number Pe (ratio of mass convection to diffusion) for both
bacteria and vitamin C within the flow domain in the z direction is:
u∆z
Pe = (30.1)
α
where u and ∆z are the typical velocity and cell depth in the z direction. The mass
diffusivity α of the bacteria and the vitamins in the fluid is given by the Stockes–
Einstein equation:
KT
α= (30.2)
6 πµa
where K is the Boltzman constant, T is the temperature, µ is the apparent viscosity

and a is the radius of the particle. The calculated cell Peclet numbers within the
3 4
flow domain in this study were of the order of 10 –10 ; hence the diffusion of bacteria
and vitamin C was ignored.

30.3.3 COMPUTATIONAL MODEL AND GOVERNING EQUATIONS
Because of the axisymmetry of the cylindrical can used in our simulation, heat
transfer was simplified into a two-dimensional problem. The partial differential
equations governing natural convection of the fluid being heated are given below:
30.3.3.1 Energy Balance
∂T ∂T ∂T k  1 ∂  ∂T  ∂2 T 
+v +u = r  + (30.3)
∂t ∂r ∂z ρC p  r ∂r  ∂r  ∂z 2 
In order to simplify the analysis, the buoyancy force caused by density variation
with temperature is defined by the Boussinesq approximation shown in Equation (30.4):
ρ = ρref [1 − β(T − Tref )] (30.4)
which is used in the body force term of the momentum equation in the vertical
direction:
30.3.3.2 Momentum Balance in the z Direction
 ∂u ∂u ∂u  ∂p  1 ∂  ∂u  ∂2 u 
ρ + v +u  =− + µ  r  + 2  + ρref g[1 − β(T − Tref )] (30.5)
 ∂t ∂r ∂z  ∂z  r ∂r  ∂r  ∂z 
where β is the thermal expansion coefficient of the liquid and Tref and ρref are the
reference temperature and density respectively. The momentum equation in the radial
direction is:
30.3.3.3 Momentum Balance in the r Direction
 ∂v ∂v ∂v  ∂p  ∂ 1 ∂  ∂ v
2
ρ +v +u  =− + µ  ( rv) + 2  (30.6)
 ∂t ∂r ∂z  ∂r  ∂r  r ∂r  ∂z 
The above equations were coupled with the equation of continuity:
30.3.3.4 Continuity Equation
1 ∂ ∂
( rρv) + (ρu) = 0 (30.7)
r ∂r ∂z
In addition to these equations, the following equations for concentrations of
bacteria and vitamins are introduced:
30.3.3.5 Mass Balance for Bacteria
∂C r b ∂C r b ∂C r b
+v +u = −k bC r b (30.8)
∂t ∂r ∂z

30.3.3.6 Mass Balance for Vitamins
∂C r v ∂C r v ∂C r v
+v +u = −k vC r v (30.9)
∂t ∂r ∂z
The relative concentrations of bacteria and vitamin (Crb and Crv) in Equations
(30.8) and (30.9) were taken as dimensionless species concentrations, defined as the
ratio of real time concentrations (Cb and Cv) to the initial concentrations (Cbo and
Cvo) multiplied by 100.
The boundary conditions used were:
1. At wall r = R, 0 ≤ z ≤ H, T = Tw , u = 0, and v = 0
2. At top surface z = H, 0 ≤ r ≤ R, T = Tw , u = 0, and v = 0
3. At bottom surface z = 0, 0 ≤ r ≤ R, T = Tw , u = 0, and v = 0
4. At center line r = 0, 0 ≤ z ≤ H, ∂T/∂r = 0, ∂u/∂r = 0, and v = 0.
The initial conditions used were: T = Tref = 121°C, Crb = 100, Crv = 100, u = 0,
and v = 0. The properties of carrot–orange soup used in the simulation were: ρ =
−3 −1 −1 −1 −1 −1
1026 kg m , CP = 3880 Jkg K , k = 0.596 Wm K and β = 0.0002 K , as
reported by Rahman (1995) and Hayes (1987). The properties were calculated from
the values reported for all food materials used in the soup, using their mass fractions.
Most previous numerical studies have been applied to Newtonian foods; in reality,
foods are generally non-Newtonian. Due to the extremely high viscosity of the liquid
food used in our simulation, the shear rate would be small. Hence, viscosity can be
assumed independent of shear rate, and the fluid will behave as a Newtonian fluid.
This Newtonian approximation is valid for most liquid food materials such as tomato
puree, carrot puree, green bean puree, apple sauce, apricot puree, and banana puree,
which are regularly canned and usually preserved by heating (Steffe et al., 1986). In
the simulation presented in this study, the viscosity was assumed to be a function of
temperature, following a second order polynomial. Nonlinear curve fitting was used
to the available measurements to obtain the constants of the polynomial.
The magnitude of the Grashof number for the viscous liquid used in our simu-
−2
lation was in the range of 10 (using maximum temperature difference and maximum
viscosity), giving a good indication that natural convection flow is laminar. In our
previous publications (Ghani et al., 1999a, 2000), the retort temperature was assumed
to rise to 121°C instantly. However, in this work the rise in the retort temperature
was measured and used in the simulations.
30.3.4 KINETICS OF DEACTIVATION OF BACTERIA

AND DESTRUCTION OF VITAMIN C
The rates of deactivation of bacteria and destruction of vitamin C are usually assumed
to follow first order kinetics (Rueter, 1993). It is known that the reaction rate
constants are functions of temperature and are usually described by the Arrhenius
equation:

For bacteria:
 −E b 
k b = A b exp  (30.10)
 RT 
For vitamins:
 −E v 
k v = A v exp  (30.11)
 RT 
In food process engineering, decimal reduction time (D) is commonly used to

define the reaction rates of quality changes. The relationship between the reaction
rate constant and the decimal reduction time is (Heldman and Hartel, 1997):
2.303
kT = (30.12)
D
The decimal reduction time and activation energy of the deactivation of bacteria
(Clostridium botulinum in this study) and the destruction of vitamin C (ascorbic
−1 −1
acid) are 0.2 min, 245 min, 300 kJ· (kg mol) , and 100 kJ· (kg mol) , respectively
(Fryer et al., 1997). The reaction rate constants kb and kv for bacteria and vitamin C
were calculated using Equation (30.12) with the reported values of decimal reduction
times. Equations (30.10) and (30.11) were used to calculate the frequency factors
11 −1
of the Arrhenius equation, Ab and Av, giving values of 2.5 × 10 sec for bacteria
9 −1
and 2.85 × 10 sec for vitamin C (ascorbic acid in this study). The Arrhenius
equation, used to describe the kinetics of the biochemical changes, is introduced to
the existing software package PHOENICS.
30.3.5 ASSUMPTIONS MADE IN THE CURRENT NUMERICAL SIMULATION

To simplify the problem, the following assumptions were made:
1. Heat generation due to viscous dissipation is negligible, due to the use of

highly viscous liquid with very low velocities (Mills, 1995).
2. Specific heat (Cp), thermal conductivity (k), and volume expansion coef-
ficient (β) are constants.
3. The assumption of no-slip condition at the inside wall of the can is valid.
4. The thermal boundary conditions were applied to liquid boundaries rather
than the outer boundaries of the can, which is reasonable due to the high
thermal conductivity of the metal can.
5. The effects of molecular diffusion of bacteria and vitamin C were neglected
due to the strong influence of the convection current. This last assumption
has been verified in our previous publication (Ghani et al., 1999b).

30.4 TEMPERATURE MEASUREMENTS IN THE CAN
DURING STERILIZATION
The temperature at the geometric center of a can heated in a retort by condensing
steam was measured. A single can filled with carrot–orange soup was placed in an
Easteel Pilot Plant Retort, which operates using steam at 121°C. The measurements
were performed for a single can having a radius and height of 0.036 m and 0.106 m,
respectively. The can was placed in an upright position and heated for 50 min
for complete sterilization. The equipment used for these measurements is as
follows:
1. TSC9601 track sense temperature probe

2. Track sense interface station and RS cable
3. Track sense wireless data logging system by ELLAB
4. E-Val software kit, run on a silicon 486 PC
5. Easteel pilot plant retort
A thermocouple probe with the specifications mentioned above was placed at

the bottom of the can, such that the tip of the thermocouple measured the temperature
at the geometric center of the can.

30.5.1 FLOW PATTERN
Figure 30.1 shows the velocity and the flow profiles of the carrot–orange soup in a
can heated by steam condensing along its outside surface. Both profiles show that the
liquid adjacent to the wall or the top or bottom surfaces will receive heat from the
condensing steam, causing it to expand and thus get lighter. The liquid away from
the sidewall stays at a much lower temperature. The buoyancy force created by the
change in liquid density due to temperature variation (from the wall to the core)
produces an upward flow near the sidewall. The hot liquid rising is deflected by the top
wall and then travels radially towards the core. Being heavier, the liquid in the core
moves downward and then towards the wall. Thus, a recirculating flow is created.
Figure 30.1 also shows that the liquid adjacent to the wall is at rest because of
the no-slip boundary conditions. The magnitude of the maximum axial velocity at
–1
the mid-height near the wall is 0.35 mm sec at t = 20 min. These results are in
reasonable agreement with the results of Kumar and Bhattacharya (1991), who used
high viscosity liquid and the same heating conditions. The magnitude of the velocity
vectors obtained can be explained in terms of the Grashof number, which represents
the ratio of the buoyancy force to viscous force. As heating progresses, a more
uniform temperature is obtained, reducing the buoyancy force in the liquid and
leading to significant reduction in the velocity.
Hiddink (1975) reported that for viscous fluids the thickness of the ascending
liquid region near the wall was greater than that of water, which can be attributed

m/sec
Stagnant zones
FIGURE 30.1 Theoretical predictions of streamline and velocity vector profiles of carrot–
orange soup in a can heated by condensing steam after 20 min. The right-hand side of each
figure is the center line.
to the large difference in the values of viscosity of the two fluids. The reported
thickness is about 12–14 mm for the viscous liquid, as compared to 6–7 mm for
water. Kumar and Bhattacharya (1991) illustrated that the thickness of ascending
liquid for a more viscous liquid is in the range of 15–16 mm. Figure 30.1 shows
that the thickness of ascending viscous liquid (carrot–orange soup) was about 18
mm, the distance between the location of the stagnant region and the wall (measured
based upon the actual can dimension). Datta and Teixeira (1987) reported the for-
mation of secondary flow (or eddies formation) at the bottom of the can near the
centerline. However, a simulation conducted by Kumar and Bhattacharya (1991) for
highly viscous liquid (CMC) did not show any formation of secondary flow or eddies.
In our simulation, the secondary flow is evident in all the cases studied, which is
expected whenever there is heating from the bottom (see Figure 30.1).

30.5.2 SLOWEST HEATING ZONE (SHZ) AND TEMPERATURE PROFILE
The temperature profiles for different periods of heating are presented in the form
of isotherms in Figure 30.2. The isotherms at t = 1 min are almost identical to those
that would be produced by pure conduction heating, but over time the isotherms are
seen to be strongly influenced by convection. Within a short period of heating, the
fluid near the bottom is still heated by conduction. However, instability results from
the large difference in the temperature between the heated bottom surface and the
colder liquid coming in contact with it. This instability in the bottom layer gives
rise to bursts of convective cells (i.e., the Benard convection cells). For a light viscous
liquid food, such as milk, orange juice, or water, the irregular shape of the isotherms
appears at the early stage of heating near the bottom. This is caused by the random
nature of Benard convective cell formation (Ghani et al., 1999a).
The SHZ in the can (i.e., the location of the lowest temperature at a given time)
is not a stationary region in the liquid undergoing convection heating. Its location
is not at the geometric center of the can, as it is in the case of conduction heating.
Initially, the contents of the can are at uniform temperature. As heating progresses,
the mode of heat transfer changes from conduction to convection, and the SHZ
moves from the geometric center to the heel of the can as shown in Figure 30.2.
The SHZ is pushed toward the bottom of the can, and it appears that the SHZ keeps
moving during heating and eventually stays in a region at about 10–15% of the can
height from the bottom. Traditionally, the movement of the coldest point has been
considered a critical parameter in identifying the SHZ for food products in thermal
(a) (b) (c)
FIGURE 30.2 Theoretical predictions of temperature profiles (°C) in a can filled with carrot–
orange soup and heated by condensing steam after periods of (a) 1 min; (b) 3 min; (c) 50 min.
The right-hand side of each figure is the center line. Convection is the dominating mechanism
of heat transfer inside the can.

process designs. Zechman and Pflug (1989) reported a location of the SHZ at about
10% height from the bottom, whereas Datta and Teixeira (1987) found that it
migrated to slightly higher locations (15% from the bottom). These observations
are in agreement with those found in this work and also with those reported by
Kumar and Bhattacharya (1991). Figure 30.2 shows that the SHZ develops a
peculiar shape after a short period of heating and does not cover the entire bottom
section of the can.
The simulation also shows that the secondary flow tends to push the SHZ
towards the wall, as may be clearly seen in Figure 30.2. According to this finding,
careful consideration must be made in representing the coldest point by the measured
temperature at the axis of the can, particularly at extreme locations close to the top
and bottom, as may be seen in Figure 30.2. The temperature of the SHZ in the
carrot–orange soup reached about 100°C in 33 min, in comparison to 2–3 min for
water, which was predicted in our previous simulation (Ghani et al., 1999a). In that
simulation, the change of the temperature of the SHZ with heating time based on
constant viscosity (measured at the film temperature) and the viscosity as function
of temperature were presented. When the viscosity is assumed as a function of
temperature, a much faster heating rate is observed. This shows the importance
of taking into account the variation of viscosity with temperature, which has not
been considered in the simulation of water as a liquid food in most previous
research.
Figure 30.3 shows the result of the simulation for the same can described earlier
but based on pure conduction heating. Here it can be seen that the slowest heating
zone stays at the geometric center of the can during the entire heating period.
FIGURE 30.3 Theoretical analysis of temperature profiles (°C) in a can filled with carrot–
orange soup and heated by conduction only after periods of (a) 1 min; (b) 3 min; (c) 50 min.
The right-hand side of each figure is the center line. Conduction is the only mechanism of
heat transfer within the can.

30.5.3 CONCENTRATION PROFILES OF BACTERIA AND VITAMINS
Figure 30.4 shows the calculated relative bacterial concentration profiles in a metal
can filled with carrot–orange soup, heated by steam from all sides, after different
periods of heating in a still retort. A higher rate of bacterial deactivation occurs at
FIGURE 30.4 Theoretical predictions of relative bacterial concentration (dimensionless) pro-

files in a can filled with carrot–orange soup and heated by condensing steam after periods
of (a) 3 min; (b) 20 min; (c) 40 min; (d) 50 min. The right-hand side of each figure is the
center line.

the top of the can, where the temperature is higher. However, the bulk of the can
remains little affected in regard to bacterial death. It can also be seen that during
the early stage of heating, the bacteria are killed only at locations close to the wall
of the can, and this is not influenced by the flow pattern shown in Figure 30.1. After
3 min of heating, the bacterial concentration profile shown in Figure 30.4a seems
to be influenced mainly by the temperature profile (Figure 30.2b). However, the bulk
of the can remains little affected with regard to bacterial death.
As the heating progressed, the concentration of bacteria dropped to the low
practical level, which illustrates what is likely to occur in practice. Figures 30.4b,
30.4c, and 30.4d show the results of the simulation after much longer time periods
of 20, 40, and 50 min, respectively. The bacterial concentration profiles are very
different from those observed at the beginning of heating. Figures 30.4b, 30.4c, and
30.4d show clearly that deactivation of bacteria is influenced significantly by both
temperature and flow pattern, unlike that observed in Figure 30.4a. Figure 30.4 also
shows that the SHZ and highest bacteria zone (HBZ), which is the location of the
highest concentration of bacteria, occur at almost the same region in the can. The
position of the HBZ is clearly influenced by the flow pattern, showing the existence
of two stagnant regions. Only after 50 min of heating are most of the bacteria
deactivated. It should be noted that this is only true for the highly viscous liquid
used in the simulation; a much shorter time would be required for sterilization of
liquids of low viscosity such as milk, light orange juice, etc.
Figure 30.5 shows the influence of thermal sterilization on vitamin C in the same
can filled with carrot–orange soup. This figure concludes the results of the simulation
at different heating periods and for a retort temperature of 121°C, showing clearly
the effect of flow pattern (Figure 30.1) on vitamin C destruction. The figure also
shows that maximum vitamin C destruction occurs at locations near the wall and
especially at the top of the can, which are the locations of highest temperatures.
Figures 30.4 and 30.5 show that the concentrations of both bacteria and vitamin C
depend not only on the temperature, but also on the flow pattern.
These locations of minimum destruction belong to minimum liquid velocity
(stagnant zones shown in Figure 30.1) and low temperature zones. The influence of
flow pattern on vitamin C concentrations is even stronger as the location of the high
vitamin concentration occurs almost within the stagnant zone.
The theoretical predictions of relative bacterial concentrations at the HBZ are
shown in Figure 30.6. At the early stage of heating, the HBZ remains at the same
initial temperature; hence, Figure 30.6 shows no significant reduction in bacteria
count. As the heating progresses, the effect of temperature becomes very strong due
to its exponential effect on the rate of bacterial deactivation. A minimum process
has been established to ensure that the probability of pathogen survival in a food is
negligible; this is the 12-D process for low-acid canned foods, which is based on
the regulation for low-acid canned food (LACF) established by the Food and Drug
Administration in the United States, typical examples of product safety. In this
process, the D value for the most thermal resistant pathogenic spores in the product,
such as those used in our simulation (Clostridium botulinum), is utilized. The 12-D
process suggests that the microbial population will be reduced from some initial
population by 12 log cycles, even if the initial population was as high as 1000 spores

FIGURE 30.5 Theoretical predictions of relative concentration profiles (dimensionless) of
residual vitamin C in a can filled with carrot–orange soup and heated by condensing steam
after periods of: (a) 3 min; (b) 20 min; (c) 40 min; (d) 50 min. The right-hand side of each
figure is the center line.
per unit mass product (Heldman and Hartel, 1997). Figure 30.6 shows that the
–10
relative concentration of bacteria dropped from 100% to 1 × 10 % at the HBZ in
50 min, which represents the time required for complete sterilization at 121°C. This
12
means that there is a probability of 1 to 10 of live bacteria remaining, acceptable
in the regulation of LACF.

Percentage of bacteria count
100
1
0.01
0.0001
1E-06
1E-08
1E-10
0 10 20 30 40 50
Time (min)
FIGURE 30.6 Theoretical predictions of relative bacterial concentration at the HBZ vs. time
of sterilization.
Average relative vitamin C
100
concentration
80
60
0 10 20 30 40 50
Time (min)
FIGURE 30.7 Theoretical predictions of average relative concentration of vitamin C vs. time
of sterilization.
The relative concentration of bacteria in the SHZ, as shown in Figure 30.4, is a good
measure of food sterility. However, in the case of vitamin destruction, it is necessary
to calculate the average of relative vitamin concentration in the whole can, which is
calculated as the weighted average of the local concentrations as follows:
L R
∑ ∑ rC∆zr
2
Cave =
R2L z=0 r =0
The average percentage destruction of the relative concentration of vitamin C

was found to be about 25% at the end of heating period. The influence of sterilization
on the destruction of vitamins B1 (thiamin) and B2 (riboflavin) has been well studied
by Ghani et al. (1999d). The results showed the strong influence of sterilization on
vitamin B1, which is in good agreement with findings reported by Fellows (1996)
for percentage loss of vitamins in canned and bottled foods. The calculated average
vitamin C concentrations are plotted in Figure 30.7.
Figures 30.6 and 30.7 show that the rate of deactivation of bacteria is higher
than the rate of destruction of vitamin C for the same time of heating, due to the
higher decimal reduction times (D) of vitamins than those of microorganisms. This
suggests that applying higher sterilization temperatures will reduce sterilization time.
However, the use of higher temperatures will also cause more destruction of vitamins.
Hence, it is likely that the best sterilization temperature may not always be 121°C,
depending on the types of food to be sterilized.

120
100
Temperature (°C)
80
60
40
Experimental
20 Theoretical-Convection
Theoretical-Conduction
0
0 10 20 30 40 50
Time (min)
FIGURE 30.8 Experimental measurements and theoretical predictions of temperature at the

geometric center of a can heated in a retort by condensing steam.
Figure 30.8 shows a comparison between the measured temperature at the geo-
metric center of the can and that obtained from computer simulations. Here, it can
be seen that the calculated center temperature of the can is higher than that measured
experimentally. This is to be expected due to the strong effect of the temperature
probe, which tends to reduce the convection current in the can because of its significant
size. However, Figure 30.6 shows that the measured temperature lies between the
predicted temperatures based on convection and conduction, suggesting that the
presence of the thermocouple probe reduced the convection in the can. Based on
this finding, we believe that measurements usually carried out in industry with such
a probe lead to longer sterilization time than necessary.
30.6 CONCLUSIONS
Transient temperature, velocity distribution, bacterial deactivation, and vitamin C
destruction evolving during natural convection heating of a viscous liquid (carrot–
orange soup) in a cylindrical metal can have been theoretically simulated. A com-
putational fluid dynamics software package (PHOENICS) was used for this purpose.
The governing equations for continuity, momentum, and energy conservation were
solved, together with those for bacteria and vitamin C concentrations. The Arrhenius
equation was used to describe the temperature dependency of the rates of deactivation
of bacteria and destruction of vitamin C.
The results of the simulation show a recirculating flow inside the can con-
sisting of liquid rising near the wall, radial flow, and uniform core flow down-
wards near the axis. The liquid inside the container showed an increase in
temperature towards the top. The SHZ (i.e., the location of the slowest heating zone)
covered the cross sectional area of the can at the early stages of heating while
it migrated towards the bottom of the can. The secondary flow at the bottom of
the can pushed the SHZ closer to the wall. The slowest heating zone developed
a peculiar shape after a short period of heating. Also, the SHZ kept moving
during heating and eventually stayed in a region of about 10–15% of the can
height from the bottom.

The simulations illustrate the effect of heating on deactivation of bacteria and
vitamin C destruction during thermal sterilization. Live bacteria and residual vitamin
C concentrations were found to depend on both temperature and flow pattern. It was
also found that the time needed for complete sterilization at 121°C for the car-
rot–orange soup used in the simulation was about 50 min.
NOMENCLATURE
−1
Ab Reaction frequency factor of bacteria, sec
−1
Av Reaction frequency factor of vitamin, sec
a Radius of the particle, m
−3
Cb Concentration of bacteria in food liquid, number of bacteria, m
−3
Cv Concentration of the vitamins in food liquid, kg m
−3
Cbo Initial concentration of bacteria, number of bacteria m
−3
Cvo Initial concentration of vitamins, kg m
Crb Relative bacteria concentration (Cb/Cbo)
Crv Relative vitamin concentration (Cv/Cvo)
−1 −1
CP Specific heat of liquid food, J kg K
D Decimal reduction time, min
2 −1
Db Diffusion coefficient of bacteria, m sec
2 −1
Dv Diffusion coefficient of vitamins, m sec
−1
Eb Activation energy of bacteria deactivation, kJ (kg mol)
−1
Ev Activation energy of vitamins destruction, kJ (kg mol)
gβ∆TL3ρ2
Gr Grashof number, G r =
µ2 −2
g Acceleration due to gravity, m sec
K Boltzman constant
−1 −1
k Thermal conductivity, W m K
−1
kb Reaction rate constant of bacterial deactivation, sec
−1
kv Reaction rate constant of vitamin destruction, sec
L Height of the can, m
u∆z
Pe Peclet number, Pe = α
p Pressure, Pa
r Radial position from center line, m
ro Radius of the can, m
−1 −1
R Gas constant, kJ (kg mol) K
t Heating time, sec
T Temperature, °C
Tw Wall temperature, °C
Tref Reference temperature, °C
−1
u Velocity in vertical direction, m sec
−1
v Velocity in radial direction, m sec
z Distance in vertical direction from the bottom, m
2 −1
α Mass diffusivity of bacteria or vitamin C, m sec
−1
β Thermal expansion coefficient, K
µ Apparent viscosity, Pa.sec

−3
ρ Density, kg m
−3
ρref Reference density, kg m
ACKNOWLEDGMENTS
The authors thank Collin Watson, process and development manager at Heinz Watties
Australasia, for allowing the experimental work to be done at the company site located
in Hastings, New Zealand. The authors also acknowledge Associate Professor Peter
J. Richards of the mechanical engineering department for his valuable discussions.
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Heating Behavior of
31 Canned Liquid/Particle
Mixtures during
End-over-End Agitation
Processing
S.S. Sablani, H.S. Ramaswamy,
and H. Krishnamurthy
CONTENTS
31.1 Introduction
31.2 Theoretical Development
31.2.1 Transient Conduction Heat Transfer
31.2.2 Transient Convection Heat Transfer
31.2.3 Convective Heat Transfer Coefficients
31.4 Data Analysis
31.5.2 Heating Behavior of Newtonian Liquid/Particle Mixtures
31.5.3 Heating Behavior of Non-Newtonian Liquid/Particle Mixtures
31.6 Conclusions
Nomenclature
References
31.1 INTRODUCTION
Mechanical agitation of cans in rotary retorts enhances heat transfer rates to liquid
particle mixtures that might otherwise heat at much slower rates (conduction to mild
convection). Agitation processing not only has the potential to improve quality
retention, but also to reduce energy consumption during processing. Semisolid and
viscous foods such as sauces and soups containing meat or vegetables are mostly

processed in rotational retorts. Thermal sterilization of such products requires that
the center of the target particle receive a predetermined minimum heat process.
Heat transfer in such systems has been analyzed using heat penetration parameters
(heating rate index, fh, and heating lag factor, jch) and convective heat transfer
coefficients (overall heat transfer coefficient, U, and fluid-to-particle heat transfer
coefficient, hfp).
Early studies focused only on convective heat transfer rates to canned liquids
(Berry et al., 1979; Berry and Bradshaw, 1980, 1982; Berry and Dickerson, 1981).
These were product-specific studies on the influence of agitation on heat transfer rates.
Some later studies evaluated heat transfer coefficients for liquid–particle mix-
tures in cans subjected to axial and end-over-end agitation (Lenz and Lund, 1978;
Anantheswaran and Rao, 1985; Deniston et al., 1987; Fernandez et al., 1988; Rao
and Anantheswaran, 1988; Stoforos and Merson, 1991, 1992). These studies mostly
used a rigid thermocouple to measure the liquid and particle temperatures, and the
motion of test particles was restricted. Naveh and Kopelman (1980) studied the effect
of orientation of agitation on the overall heat transfer coefficient and found that U
was improved by a factor of two to three in end-over-end rotation compared with
an axial mode of rotation. Parchomchuk (1977) proposed a new method of circular
oscillation for agitation processing of canned food and reported that the agitating
forces produced were similar to those caused by end-over-end rotation. The heat
transfer rates to canned liquids when using a smaller radius of rotation during circular
oscillation were reported to be comparable to those obtained during end-over-end
agitation.
More recently, several studies were conducted on heat transfer to liquid–particle
mixtures in cans undergoing end-over-end processing at the McGill University
(Sablani and Ramaswamy, 1995, 1996, 1997, 1998, 1999; Ramaswamy and Sablani,
1997a, b; Pandey et al., 1997; Krishnamurthy et al., 2000) using Newtonian as well
as non-Newtonian liquids. In these studies, a technique was developed using a fine
flexible thermocouple to measure the convective heat transfer coefficients associated
with end-over-end rotational processing of canned particulate liquids. The technique
allowed sufficient particle motion during processing and provided more realistic
transient temperatures for estimation of heat transfer rates. The flexible thermocouple
approach was used to quantify the influence of various system- and product-related
parameters on convective heat transfer coefficients and heat penetration parameters.
For designing a sterilization process, heat penetration parameters such as heating
rate index, fh, and the lag factors, jch and jcc, are frequently used. Few studies have
been carried out on the effect of system and product parameters on the heat transfer
rates to liquid–particle mixtures in cans. Several factors influence the heat penetration
rate into the food particles in a container during rotational sterilization. The most
relevant factors include retort temperature, rotational speed, mode of rotation, radius
of rotation, can head space, and product viscosity, as well as the Newtonian/non-
Newtonian nature, liquid to particle ratio, particle size, particle shape, etc. (Sablani,
1996).
The objective of this chapter is to provide an overview of the influence of system-
and product-related parameters on the heating behavior of canned particulate New-
tonian/non-Newtonian liquids during end-over-end agitation rotation processing.

31.2 THEORETICAL DEVELOPMENT
In thermal processing of a canned particulate food system, heat is first transferred
from the heating medium in the retort to liquid inside the can (involving an overall
heat transfer coefficient, U) and then from the can liquid to the particles (involving
the fluid-to-particle heat transfer coefficient, hfp). Hence, the particle center is the
slowest heating/cooling point in the system. In order to establish thermal process
schedules for canned liquid/particle mixtures, information on the temperature history
at the particle center is needed, in addition to thermal resistance characteristics of
the test microorganisms (z and Fo).
31.2.1 TRANSIENT CONDUCTION HEAT TRANSFER

The transient heat flow in a spherical particle immersed in fluid of constant temper-
ature can be described by the following partial differential equations:
∂ 2 T 2 ∂T 1 ∂T
+ = (31.1)
∂r 2 r ∂r α ∂t
where r represents the radius of the sphere. The solution for the spacial temperature
in the form of an infinite summation series is given by:
∞
T − Tr (δ 2n + (Bi − 1) 2 sin(δ n )
∑
2 Bi
U= = sin(δ n r / a ). exp( −δ 2n Fo) (31.2)
Ti − Tr r / a n =1
δ 2n (δ 2n + Bi(Bi − 1))
where δn is the nth positive root of
δ cot δ = 1 − Bi (31.3)
For sufficiently long heating time (Fo > 0.2), the terms in the infinite summation
series in Equation (31.2) converge rapidly, and in most cases may be accurately
approximated by the first term of the series. Furthermore, at the center of a sphere,
r = 0, imposing these conditions, Equation (31.2) can be simplified for center
temperatures in a sphere as:
U o = R exp( −SFo) (31.4)
where R and S are the characteristic functions of the Biot number, as given below:
2 Bi[δ12 + (Bi − 1) 2 ]sin δ1

R= (31.5)
[δ12 + Bi(Bi − 1)]δ1
S = δ12 (31.6)

The concept of heating/cooling rate index (fh/fc) and lag factor (jch/jcc) parameters
to characterize the temperature history in a food has been well recognized. The heat
penetration parameters are obtained from a plot of the logarithm of the temperature
difference between the retort (Tr) and the product (T) [i.e., log (Tr − T)] vs. heating
time (on linear abscissa)]. The heating rate index, fh, is obtained as the time taken
for the straight-line portion of the curve to pass through one log cycle, and jch is
obtained as the ratio of (Tr − Tpih) and (Tr − Ti). The experimental time–temperature
data obtained at the particle center can be used to make process calculation using
the General and Improved General methods. On the other hand, formula methods
such as the Ball and Stumbo methods make use of heat penetration data (fh, jch, jcc)
in order to establish process calculation. The dimensionless center temperature can
be correlated with heat penetration parameters as:
T − Tr
= j 10 − t / fh (31.7)
Ti − Tr
For a spherical food particle being heated by a medium under conditions of

finite surface and internal resistance, the following can be obtained from Equations
(31.3–31.7):
2.303
fh = (31.8)
Sα
jch = R (31.9)
For a given surface heat transfer coefficient/Biot number, the δ can be obtained
from Equation (31.3). The constants R and S can be calculated from Equations (31.5)
and (31.6). Once R and S are known, the heat penetration parameters can be
estimated through Equations (31.8) and (31.9). Details of the equations related to
the other geometries can be found in Ball and Olson (1957) and Ramaswamy et al.
(1982).
31.2.2 TRANSIENT CONVECTION HEAT TRANSFER

In transient convection heat transfer in canned fluid, the temperature at all locations
changes with time. The rate of heat transfer from the heating medium to the can
fluid will depend on the thickness of the boundary layer between the can fluid and
the wall. This heat transfer rate is quantified in terms of overall heat transfer
coefficient. The equation that describes the rate of heat flow from heating medium
to the can fluid is:
dQ
= UA(Tl − T) (31.10)
dt

where U is the overall heat transfer coefficient. In the heating of fluid in the can,
the change in the quantity of heat in the fluid per unit of time is a function of the
mass of the fluid, m, and the specific heat, Cpf, and mean temperature:
dQ dT
= mC pf (31.11)
dt dt
By solving Equations (31.10) and (31.11), and separating the variable and
integrating over temperature and time, the Equation (31.12) is obtained:
T − Tr
= exp( − UAt / 2.303mC pf ) (31.12)
Ti − Tr
By comparing Equation (31.12) with Equation (31.7), the following can be

obtained:
2.303mC pf
fh = (31.13)
UA
jch = 1.0 (31.14)
The particle center temperature can also be obtained by knowing the overall
convective heat transfer coefficients. In the case of fluid particle mixtures in the can,
the heat transfer can be analyzed by the overall heat transfer coefficient, U, and the
fluid-to-particle heat transfer coefficient, hfp.
31.2.3 CONVECTIVE HEAT TRANSFER COEFFICIENTS

In this approach, the overall energy balance on the canned liquid/particle system
can be used:
dTl d < Tp >

UA c (Tr − Tl ) = m l C pl + m p C pp (31.15)
dt dt
The following are assumed for deriving Equation (31.15): uniform initial and
transient temperatures for liquid, constant heat transfer coefficient, constant thermal
and physical properties for both liquid and particles, and no energy accumulation
in the can wall. The second term on the right side of Equation (31.15) can be described
as the heat transferred to particles from the liquid through the particle surface, and
Equation (31.15) can be rewritten as:
dTl
UA c (Tr − Tl ) = m l C pl + h fp A p ( Tl − Tps ) (31.16)
dt
It is also assumed that the particle receives heat only from the liquid and not
from the can wall when it impacts, i.e., heat is transferred first from the can wall to
the liquid and then to the particles. The transient heat flow in a particle immersed

in fluid can be described by the following partial differential equations (Jaluria and
Torrance, 1996):
∂T
∇.k∇T = ρC p (31.17)
∂t
The initial and boundary conditions are:
T = Ti t=0 (31.18)
∂T
−k = h fp (T − Tl ) t > 0 at the surface (31.19)
∂n
where n is the normal at the surface taken positive outward.

Using the finite difference method, the fluid-to-particle heat transfer coefficient,
hfp, can be estimated by solving the governing partial differential equations (Equa-
tions (31.17–19)) of conduction heat transfer. The inverse heat transfer approach,
where surface heat flux is estimated using one or more measured temperature
histories inside a heat-conducting body, is used to estimate hfp values. The overall
heat transfer coefficient, U, can be determined by integrating Equation (31.16) over
the set process time (Ramaswamy and Sablani, 1997a,b). In order to calulate U, it
is necessary to have the transient temperatures of the liquid and particle surface. In
Equation (31.16), the experimentally measured value of the liquid is used, and the
transient temperature of the particle surface is computed from Equations (31.17–19).
Once the convective heat transfer coefficients (U and hfp) are known for a range
of processing conditions, the equations mentioned above (31.15–31.19) can be used
to predict the liquid and particle center temperatures. The predicted time–temperature
data can then be used to establish the thermal process schedule.
In situations where the associated viscosities of the liquid are high (as in the
case of highly viscous Newtonian or non-Newtonian carrier fluids), the liquid portion
tends to have only limited convection except at high rotation speeds. The system
then moves predominantly towards conduction heating behavior, with characteristi-
cally nonuniform temperature distribution throughout the container. Under such a
scenario, the concept of U and hfp is difficult to recognize; however, the concept of
fh and jch would still be valuable for comparative purposes and for the purpose of
establishing thermal processing schedules. Hence, in this chapter, we have compared
all conditions of rotational processing involving both Newtonian and non-Newtonian
liquids using the fh and jch concept.

Water and high temperature bath oil (model 100 CST at 38°C, Fisher Scientific Ltd.,
Montreal), giving different viscosity levels, were used as Newtonian model liquids.
Guar gum, a cross-linked waxy starch with commercial applications in several food
preparations (soups, gravies, and pudding) was used to prepare non-Newtonian

test samples containing 0–1% (w/v) gum. The gum solutions were made 12 h before
the experiment to allow the gum to hydrolyze. The rheological properties of the
prepared solutions were determined with a Haake RV2 concentric cylinder rotation
viscometer.
3
Nylon spheres (density = 1128 kg/m , heat capacity = 2073 J/kgK, thermal
conductivity = 0.369 W/mK) of different diameters (0.01905, 0.02225, and 0.025 m)
were used as particles. Can liquid temperature was measured at the geometric center
of the cans using CNS needle type thermocouples. For the purpose of measuring
particle transient temperatures, a fine hole was drilled to the center of the spherical
particle, which was filled with a 1:1 mixture of epoxy resin and hardener. A fine wire
(0.0762 mm diameter) copper-constantan thermocouple was inserted into the center.
The thermocouple-equipped particle was mounted inside the can using brass con-
nectors (stuffing box for plastic pouches C-5.2, Ecklund Harrison Technologies, Inc.,
Cape Coral, FL) at half the height of the can. The thermocouple wire attached to
the particle was long enough (half the can height) to allow particle movement inside
the can, and short enough to avoid entangling with the needle-type thermocouple
used for measuring the liquid temperature. In this type of arrangement, the particle
was fairly free to move during processing. The thermocouple-equipped particle was
positioned near the geometric center of the can. The other ends of both thermocouples
were connected to a 32-circuit slip ring assembly through 24 AWG copper-constan-
tan thermocouple wire (Omega Engineering Corp., Stamford, CT). The thermocou-
ple inputs were recorded at 15-sec time intervals using a data acquisition system
and LABTECH NOTEBOOK (Laboratory Technologies Corporation, Wilmington,
MA) software or an HP datalogger (HP3497/HP34901, Hewlett Packard, Loveland,
CO).
Cans of size 307 × 409 (0.0873 m diameter × 0.116 m height) containing the
test liquid and multiple particles were subjected to end-over-end rotational process-
ing in a pilot scale rotary, single cage, full water immersion retort (Stock Rotomat-
PR900; Hermann Stock Maschinenfabrick, Germany). A common air over pressure
of 70 kPa was used for all test runs with the Rotomat. The cans were arranged in
vertical orientation (can axis perpendicular to axis of rotation) to give end-over-end
rotation to the cans. In some test runs, as opposed to the end-over-end rotation in a
continuous fashion, the cage was rotated for a few rounds in one direction, stopped
and rotated in the opposite direction giving an oscillatory mode of operation for the
end-over-end agitation.
With Newtonian liquids (Sablani, 1996), three experimental designs were
selected to study the influence of different system and product parameters. The
experimental variables used were: three particle concentrations (20, 30, and 40%
v/v); three rotational speeds (10, 15, and 20 r/min); and two kinematic viscosities
−6 −4 2
(1.0 × 10 and 1.0 × 10 m /sec). Three rotational speeds (10, 15, and 20 r/min),
−6 −4 2
two kinematic viscosities (1.0 × 10 and 1.0 × 10 m /sec), and three particle
diameters (0.01905, 0.02225, 0.025 m) were selected to study the influence of
particle size. A can head space of 0.01 m, a radius of rotation of 0.19 m, and a retort
temperature of 120°C were used as fixed parameters. In order to study the influence
of mode of end-over-end agitation, the experimental variables were: three radii of
rotation (0, 0.13, and 0.26 m); three speeds of rotation (8, 16, and 24 r/min); and

two modes of rotation (continuous and oscillatory). In this case, the particle diameter
of 0.025 m, a high temperature bath oil, a can head space of 0.01 m, and a retort
temperature of 120°C were used as fixed parameters. A full factorial experimental
design was employed in each of the three studies. Four replicate cans were kept at
a given radius of rotation, and each processing condition was repeated twice.
With non-Newtonian liquids (Krishnamurthy et al., 2000), nine cans at three
radii of rotation (0, 0.1, and 0.19 m, three replicates) were loaded into the cage, and
the rest of the space was filled with dummy cans containing water. Five retort
temperatures (110, 115, 120, 125, and 130°C), five rotational speeds (0, 5, 10, 15,
and 20 r/min), five particle concentrations (10, 15, 20, 25, and 30% v/v), and five
guar gum concentrations (0.00, 0.25, 0.50, 0.75, and 1.00% w/v guar gum) were
employed as system (operating) variables. A central composite rotatable design
(CCRD) was used for the experiments.
31.4 DATA ANALYSIS

Since small variations in initial temperature and heating medium temperature were
unavoidable, liquid and particle transient temperatures were normalized to an initial
temperature of 20°C and the respective retort temperature (110, 115, 120, 125, or
130°C). Heat penetration parameters (fh and jch) were evaluated from the plots of
logarithms of differences in the retort temperature and the temperature of liquid/
particle vs. time. The heating rate index and heating lag parameters for liquid and
particle were analyzed using statistical analysis software available on the McGill
University (Montreal) computer network. An analysis of variance (ANOVA) proce-
dure was used to evaluate the level of significance of system and product parameters
and their interactions. Process lethality (Fo) and cook value (Co) were calculated for
each processing condition by numerical integration of time–temperature data (z =
10°C and reference temperature 121.1°C for Fo, and z = 33°C and reference tem-
perature 100°C for Co):
∫
Fo = 10 ( T −121.1)/ z dt
∫
C o = 10 ( T −100 )/ 33 dt (31.20)
When the process lethalities of test runs are not constant, as in the present study,
the ratio Co/Fo gives a relative parameter for comparing the degree of cooking at
various retort temperatures, with higher ratios indicating more severe cooking con-
ditions (Ramaswamy et al., 1993).

Typical linear and semilogarithmic time–temperature profiles of the can liquid and
particle center are shown in Figure 31.1. The retort come-up times varied from 2 to
4 min and showed logarithmic come-up profiles. Initially, heat is transferred from
the heating medium to the can liquid through the can wall and then to the particle.

140 2.5
Log (Tr – Tpih)
120 2.0 Log (Tr – Tih)
Liquid
100 1.5 Particle center

Temperature (°C)
jch = (Tr – Tpih)/(Tr – Tih)
Log(Tr – T)
80 1.0
fh
60 0.5
40 Retort 0.0
0 5 10 15
Liquid
20 -0.5
Particle center
0 -1.0
0 5 10 15 20
FIGURE 31.1 Typical time temperature profiles of liquid and particle.
In the early part of heating, particle center temperature was lower than the liquid
temperature; this is due to convective heat transfer resistance at the particle surface
and conductive resistance inside the particle. The liquid temperature was lower than
the retort heating medium temperature due to conductive resistance of the can wall
and to external and internal convective resistance at the can wall surface. In the latter
part of heating, the difference between liquid and particle temperatures generally
decreased as these temperatures approached the heating medium temperature.
31.5.2 HEATING BEHAVIOR OF NEWTONIAN

LIQUID/PARTICLE MIXTURES
Analysis of variance of results with Newtonian liquids showed that all factors under
study affected fh for both liquid and particle, except the rotation effect on particle
fh (Table 31.1). All factors were found to influence (p < 0.05) liquid and particle jch
except the effects of radius of rotation and mode of rotation on particle j and radius
of rotation effect on liquid jch. Of the six factors considered, only viscosity influenced
the liquid Co/Fo (p < 0.005). All factors influenced particle Co/Fo (p < 0.05), except
radius of rotation. Although two-way interaction effects were significant in some
instances, their overall contribution to the main effects was very small.
The effects of different factors considered on the heating rate index of the particle
and liquid are shown in Figure 31.2.
The fh value of liquid decreases with an increasing rotational speed (17% decrease
between 10 and 20 r/min), presumably due to the enhanced mixing resulting in faster
heat transfer rates. Increasing rotational speed from 10 to 20 r/min decreased the particle
f value by 11%.
Moving cans away from the center of the cage to 0.13 or 0.26 m radius of
rotation did not influence (p > 0.05) either liquid or particle fh. From a thermal

TABLE 31.1
Analysis of Variance Results (% Sum of Squares and Significance Level)
Showing the Influence of System and Product Parameters on Three Variables
Considered (fh, jch, and Co/Fo) while Employing Newtonian Liquids
Effect of RS, V, PC Effect of RS, V, PS Effect of RS, MR, RR
A: Parameters for
Liquid Portion fh jch Co/Fo fh jch Co/Fo fh jch Co/Fo
a a a a a
Rotational speed (RS) 2.5 11.0 1.7 3.2 1.7 1.0 71.9 13.9 2.4
a a
Mode of rotation (MR) — — — — — — 13.8 37 0
a
Radius of rotation — — — — — — 2.0 2.0 2.6
(RR)
a a a a a a
Viscosity (V) 87.0 5.3 8.7 87.9 17 13.1 — — —
a a
Particle concentration 2.1 29.4 1.9 — — — — — —
(PC)
a a
Particle size (PS) — — — 4.8 9.4 3.9 — — —
B: Parameters For
Particles
a a a b a a a a
Rotational speed (RS) 1.7 1.31 2.9 3.6 2.7 5.5 68.4 30.0 66.0
a a
Mode of rotation (MR) — — — — — — 19.0 2.0 21.0
Radius of rotation (RR) — — — — — — 0.6 2.8 0.5
a a a a a a
Viscosity (V) 78.6 4.7 74.0 8.0 18.7 73.4 — — —
a a b
Particle concentration 11.7 39.4 12.4 — — — — — —
(PC)
a a a
Particle size (PS) — — — 9.1 13.7 9.5 — — —
Note: RS, rotational speed; MR, mode of rotation; RR, radius of rotation; V, viscosity of fluid; PC, particle
concentration; PS, particle size.
a
p < 0.005.
b
p < 0.05.
processing design point of view, this is a desirable situation. The smaller the influence
of radius of rotation, the higher the uniformity in terms of lethality achieved in cans
placed at different locations in the retort for processing.
Shifting from the continuous mode of end-over-end rotation to the oscillatory
mode increased both liquid and particle fh values by 10%.
The fh values of liquid and particle were higher at all the processing conditions
when high viscosity fluid oil was used; this could be due to the thicker boundary
layer (Sablani and Ramaswamy, 1997a). The temperature of the water reached the
heating medium temperature more rapidly, indicating a faster rate of heat transfer.
Increasing the level of particle concentration from 20 to 40% increased the
average fh value of the particle by 28%, but increased that of the liquid only by 5%.
Increasing particle concentration resulted in a packed bed situation, reducing the
free movement of particles, thus increasing the fh value for the particle. Particle
motion and mixing have an important effect on the associated heat transfer rates

min min
14 Rotation Speed 14 Mode of Rotation
12 12
10 10 rpm Continuous
10
8 15 rpm Oscillatory
8
6 20 rpm
6
4 4
2 2
0 0
Liquid Particle Liquid Particle
min min
14 Radius of Rotation 14 Viscosity
12 12
0.0 m Water
10 10
0.13 m Oil
8 8
0.26 m
6 6
4 4
2 2
0 0
min min Particle Size

14 14
Particle Concentration
12 12 0.0190 m
20% 10
10 0.0225 m
30% 8
8 0.0250 m
40%
6 6
4 4
2 2
0 0
FIGURE 31.2 Effect of processing conditions on heating rate index (fh, min) with Newtonian
liquid and particle mixture in cans.
(Ramaswamy and Sablani, 1997a). The presence of multiple particles is expected

to cause secondary agitation, which will influence the mixing of materials in the
cans (Sablani and Ramaswamy, 1998). The small increase in liquid fh indicated that
increased particle concentration increased the drag forces exerted by the particle on
the liquid.

The fh values of liquid increased by 24% when the particle diameter was
increased from 0.01905 to 0.025 m. On the other hand, the particle fh increased 27%
as particle size increased from 0.01905 to 0.02225 m, while a further increase in
diameter up to 0.025 m decreased the fh by 8%. Lenz and Lund (1978) also observed
a decrease in heat transfer rates to liquid and particles (U and hfp) as particle diameter
increased from 0.021 to 0.03 m in a 60% aqueous sucrose solution. Deniston et al.
(1987), however, did not find a straightforward relationship for heat transfer rates
(U) associated with canned liquids.
In general, factors affecting fh also affected the jch values, except that the mode
of rotation did not influence the particle jch, and neither mode of rotation nor speed
of rotation influenced the particle jch. Particle concentration had the greatest influence
on the liquid and particle jch (Figure 31.3). Increasing particle concentration reduced
the free movement and liquid/particle mixing, which delayed the constant heating
rate of the product.
The Fo value (process lethality) of a process indicates process severity with
respect to microbial destruction and is the key in process time establishments. Co
(cook value), on the other hand, indicates the cumulative equivalent of cooking
minutes at 100°C. The ratio Co/Fo gives a relative measure of the degree of cooking
and could be a suitable multiplier in cases where process time is not constant
(Ramaswamy et al., 1993).
Liquid viscosity had the greatest influence on liquid Co/Fo (p < 0.005). The liquid
ratio Co/Fo was 10% higher for oil than for water. Rotational speed and liquid viscosity
effects were more pronounced on particle Co/Fo ratio (Figure 31.4). At any condition,
the particle Co/Fo was always higher than the ratio Co/Fo of liquid. This is because in
the sterilization of canned liquid–particle mixtures, heat is first transferred from the
heating medium to the canned liquid through the wall, then to the particles. In such
a situation, some overprocessing of the liquid portion is normal. Any attempt to
minimize the overprocessing of the canned liquid portion will be desirable.
Temperature is supposed to be the most influential factor on Co/Fo (as will be
demonstrated with the non-Newtonian fluids), which is part of the reason for the
well-accepted phenomenon that high temperature short time (HTST) techniques
provide a quality advantage. The bulk of the above studies, however, were carried
out at a constant temperature (120°C), and hence the temperature effect is not
illustrated.
31.5.3 HEATING BEHAVIOR OF NON-NEWTONIAN

LIQUID/PARTICLE MIXTURES
Statistical analysis of results with non-Newtonian liquids (Krishnamurthy et al.,
2000) on fh, jch, and Co/Fo during the thermal process are presented in Table 31.2.
The results revealed that both guar gum concentration and rotational speed influenced
fh significantly (p < 0.05). Further, both gum and particle concentrations influenced
the jch (p < 0.05) of liquid, but only particle concentration was important with respect
to particle jch. Of the four factors considered, only retort temperature influenced
Co/Fo (p < 0.005). An interaction between the factors retort temperature and gum

min min
2 2
Rotation Speed Mode of Rotation
1.5 10 rpm 1.5 Continuous
15 rpm
1 20 rpm 1 Oscillatory
0.5 0.5
0 0
min min
2 2
Radius of Rotation Viscosity
1.5 0.0 m 1.5
Water
0.13 m
Oil
1 0.26 m 1
0.5 0.5
0 0
min min
2 Particle Concentration 2
Particle Size
20%
1.5 1.5 0.0190 m
30%
0.0225 m
1 40%
1 0.0250 m
0.5 0.5
0 0
FIGURE 31.3 Effect of processing conditions on heating lag factor with Newtonian liquid
and particle mixture in cans.
concentration in their effect on Co/Fo was also observed (0.005 < p < 0.05), but was
of less significance compared to the main effects. Radius of rotation did not have
any significant effect on any of the heat transfer parameters considered.
All factors that influenced the heat penetration parameters (fh and jch) with
Newtonian liquids also influenced liquid and particle fh and jch with different magnitudes.

min min
10 10
Rotation Speed Mode of Rotation
8 8
10 rpm Continuous
6 15 rpm 6
Oscillatory
4 20 rpm 4
2 2
0 0
min min
10 10
Radius of Rotation Viscosity
8 0.0 m 8 Water
6 0.13 m 6 Oil
0.26 m
4 4
2 2
0 0
min min
10 Particle Concentration 10 Particle Size
8 20% 8 0.0190 m
30% 0.0225 m
6 6
40% 0.0250 m
4 4
2 2
0 0
FIGURE 31.4 Effect of processing conditions on Co /Fo with Newtonian liquid and particle
mixture in cans.
In general, fh and jch values with non-Newtonian liquids were higher than those
obtained with Newtonian liquids, indicating that rate of heat transfer to both liquid
and particles was slower in the former case. This can be attributed to poor mixing
of non-Newtonian liquid and particles. Guar gum concentration was the major factor

TABLE 31.2
Analysis of Variance Results (% Sum of Squares and Significance Level) Showing the Influence of Operating
Variables on the Three Variables Considered (fh, jch, and Co /Fo) at Three Radii of Rotation (center, 100, and
190 mm) with Non-Newtonian Liquids
fh jch Co/Fo
Center 100 mm 190 mm Center 100 mm 190 mm Center 100 mm 190 mm
A: Parameters for Liquid Portion
a a a a a a
Solution concentration 46.0 51.14 42.24 85.50 74.00 71.38 0.58 3.00 1.32
b b b
Particle concentration 9.00 14.20 18.52 7.64 15.55 14.81 7.60 5.90 7.00
a a a
Retort temperature 8.00 10.71 9.96 1.00 3.00 3.03 70.16 83.96 84.41
b b b
Rotational speed 12.10 20.12 23.08 1.00 4.75 4.71 6.40 1.44 4.90
B: Parameters for Particles

a a a b
Gum concentration 58.38 51.38 51.38 11.19 23.87 10.27 2.34 2.08 1.00
b b b
Particle concentration 5.86 7.89 7.89 38.19 38.75 25.61 1.40 1.23 1.4
a a a
Retort temperature 9.57 7.32 7.32 4.95 6.4 4.95 86.03 87.08 85.12
b b b
Rotational speed 24.46 31.19 20.87 10.27 9.51 10.27 1.36 1.21 0.00
a
p < 0.005.
b
p < 0.05.
min min
12 Rotation Speed 12 Retort Temperature
10 20 rpm 10 130°C
8 15 rpm 8 125°C
10 rpm 120°C
6 6
5 rpm 115°C
4 4
0 rpm 110°C
2 2
0 0
min min
12 12
Gum Concentration Particle Concentration
10 1.0% 10 0.3%
8 0.75% 8 0.25%
6 0.5% 0.2%
6
0.25% 0.15%
4 4
0.0% 0.1%
2 2
0 0
FIGURE 31.5 Effect of processing conditions on heating rate index (fh, min) with non-
Newtonian liquid/particle mixture in cans. (From Krishnamurthy, H., Sanchez, G., Ramaswamy,
H.S., Sablani, S.S., and Pandey, P.K., poster presentation at ICEF8, Puebla, Mexico, April 10–13,
2000. With permission.)
accounting for nearly 40 to 50% of the total variation in heating rate index, followed
by rotational speed accounting for 12 to 24%.
Figure 31.5 demonstrates typical variations in fh under different conditions. In
general, fh was found to increase with increasing gum concentration and decreasing
rotational speed. This was expected and can be explained based on apparent viscosity,
which is highest for 1% guar gum and lowest for water. The decreasing effect of
rotational speed on fh results from the forced mixing of can contents due to relative
motion (turbulence) of liquid and particles in the can.
Guar gum concentration was again the major factor accounting for 74% of the
total variation in heating lag (jch) of the liquid (Figure 31.6). Particle concentration
came next with 15%. The samples with the highest solution and particle concentrations

min min
3.5 3.5
Rotation Speed
3 3 Retort Temperature
20 rpm
130°C
2.5 15 rpm 2.5
125°C
2 10 rpm 2
120°C
1.5 5 rpm 1.5
115°C
1 0 rpm 1
110°C
0.5 0.5
0 0
min min
3.5 3.5 Particle Concentration
Gum Concentration
3 3
1.0%
2.5 0.3%
0.75% 2.5
2 0.25%
0.5% 2
0.2%
1.5 0.25% 1.5
0.15%
1 0.0% 1
0.1%
0.5 0.5
0 0
FIGURE 31.6 Effect of processing conditions on heating lag factor with non-Newtonian
liquid/particle mixture in cans. (From Krishnamurthy, H., Sanchez, G., Ramaswamy, H.S.,
Sablani, S.S., and Pandey, P.K., poster presentation at ICEF8, Puebla, Mexico, April 10–13, 2000.
With permission.)
exhibited a greater lag factor compared to the other four levels, possibly due to the
high initial viscosity (strongly non-Newtonian). Contrary to expectation, retort tem-
perature and rotational speed did not significantly affect lag factor. Particle concen-
tration was the only major factor, accounting for 38% of the total variation in particle
heating lag.
As shown in Figure 31.7, the ratio Co/Fo for non-Newtonian liquids dramatically
decreased from about 40 to 1.5 as temperature increased from 110 to 130°C. Overall,
the magnitude of Co/Fo for liquid and particle was larger than that observed with
Newtonian liquids, suggesting slower heat transfer rates with non-Newtonian solu-
tions. The effect of gum concentration on this ratio was small, but the increasing
trend was clear. The cook quality of the product could thus be improved by high
temperature short time processing.

Surface Response Graph
for Co/Fo (Liquids)
40
35
30
25
Co/Fo
20
15
10
5
110
0 115
120 (C)
0.25 0.50 0.75 1.00 130125 perat
ure
Gum Concentratio
n (%w/v) Tem
ort
Ret
Surface Response Graph

for Co/Fo (Particle)
40
35
30
25
Co/Fo
20
15
10
5
0 110
Gum 0.3 0.5 115
Con 120
cen 0.8
trat 1.00 130 125 )
ion ure (C
(%w Te m perat
/v) Retort
FIGURE 31.7 Response surface plots of Co /Fo as a function of retort temperature and guar
gum concentration. (From Krishnamurthy, H., Sanchez, G., Ramaswamy, H.S., Sablani, S.S.,
and Pandey, P.K., poster presentation at ICEF8, Puebla, Mexico, April 10–13, 2000. With
permission.)
31.6 CONCLUSIONS
With Newtonian liquids, liquid viscosity and rotational speed had major effects on
fh and Co/Fo, while the effects of particle concentration and rotational speed were
more pronounced with jch. The influence of mode of rotation and particle size on the
different thermal process parameters was minimal. The effect of radius of rotation
was not significant. With non-Newtonian liquids, the gum concentration and rotational
speeds had a major effect on the heating rate index (fh) for both liquid and particles,
and the effect of particle concentration was especially noticed on lag factor (jch) for

both liquid and particles. Co/Fo was highly influenced by the retort temperature, and
a trend was observed when it came to the effect of gum concentration. Both heating
rate index and heating lag factor values were higher with non-Newtonian liquid/par-
ticle mixtures than those observed with Newtonian liquid/particle mixtures.
NOMENCLATURE
a Radius of sphere, m
2
A Total external surface area, m
Bi Biot number = hfp a/k
Co Cook value, min
Cp Heat capacity, J/kgK
2
Fo Fourier number = αt/a
Fo Process lethality, min
fh Heating rate index, sec
2
hfp Fluid-to-particle heat transfer coefficient, W/m K
jch Heating lag factor
k Thermal conductivity, W/mK
m Mass, kg
R A function of Biot number
S A function of Biot number
T Temperature, °C
t Time, sec
2
U Overall heat transfer coefficient, W/m K
U (T – Tr)/(Ti − Tr)
<> Volumetric average
SUBSCRIPTS
c Can
i Initial condition
l Liquid
p Particle
r Retort
s Surface
GREEK SYMBOLS
2
α Thermal diffusivity, m /sec
δ Characteristic root (Equation (31.3))
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Res., 32, 39–84, 1988.
Sablani, S.S., Heat Transfer Studies of Liquid Particle Mixtures in Cans Subjected to End-
Over-End Processing, Ph.D. thesis, McGill University, Montreal, 1996.

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Dimensionless
32 Correlations for Forced
Convection Heat Transfer
to Spherical Particles
under Tube-Flow
Heating Conditions
H.S. Ramaswamy and M.R. Zareifard
CONTENTS
32.1 Introduction
32.2 Theoretical Background
32.3.1 Calorimetric Method
32.3.2 Particle Oscillatory Motion Method
32.5 Conclusions
Nomenclature
References
32.1 INTRODUCTION
One of the potential advantages of aseptic processing of particulate foods is the
minimum loss of nutrients and overall quality improvement due to the use of a high
temperature, short time processing technique. To design a process that ensures the
commercial sterility of processed foods, thermal process calculations require accu-
rate time–temperature data. Due to difficulties in measuring the temperature of a
particle as it moves through the heat exchanger and holding tube sections of an
aseptic processing system, the particle center temperatures are usually predicted by
mathematical modeling. Data on residence time distribution (RTD) and associated

fluid-to-particle heat transfer coefficient (hfp) in a continuous flow system are nec-
essary in such models (Dignan et al., 1989). Numerous studies have been carried
out to evaluate hfp under a wide range of experimental conditions simulating some
aspects of aseptic processing. Several of these studies have made use of particles
fixed in a tube for gathering time–temperature data, while others have used novel
approaches to monitor transient temperatures of moving particles.
Dimensional analysis is a useful technique for generalization of data, as it
reduces the number of variables that must be studied and permits the grouping of
physical variables that affect the process of heat transfer. In the dimensional analysis
of convection heat transfer, the Nusselt number (Nu), a dimensionless measure of
convective heat transfer coefficient, is correlated with other dimensionless numbers
such as the Reynolds (Re), Prandtl (Pr), and Grashof (Gr) numbers. Kramers (1946),
Ranz and Marshal (1952), and Whitaker (1972) were early researchers who presented
empirical equations for heat transfer correlations. During the last decade, several
researchers have developed different forms of correlations to predict fluid-to-particle
heat transfer coefficients for processing of particulate food under a range of tube-
flow conditions (Sastry and Zuritz, 1987; Chandarana et al., 1988, 1990; Zuritz et al.,
1990; Mwangi et al., 1992; Balasubramaniam, 1993; Zitoun and Sastry, 1994a,b;
Astrom and Bark, 1994; Bhamidipati and Singh, 1995; Awuah and Ramaswamy,
1996; Chakrabandhu and Singh, 1998).
The objectives of this study were to develop dimensionless correlations for
experimental data obtained from two techniques allowing particle motion during the
heating process: a calorimetric method in which the particle was free to move and
rotate along the length of holding tube (Ramaswamy and Zareifard, 2000), and a
particle oscillatory motion method in which the particle was allowed controlled
movement in an oscillatory fashion (Zareifard and Ramaswamy, 2001).
32.2 THEORETICAL BACKGROUND

Heat transfer from liquid to particles in continuous processing of multi-phase sys-
tems is affected by both liquid and particle thermophysical properties as well as
system parameters. In the dimensional analysis of forced convection heat transfer,
the fluid-to-particle heat transfer coefficient (hfp) is expressed in terms of the Nusselt
number (Nu), which is generally described as a function of other dimensionless
numbers [Nu = f (Re, Pr, Gr)]. Different forms of dimensionless correlations have
been published concerning the flow field and heat transfer to particles in tube-flow
conditions. Kramers (1946), Ranz and Marshal (1952), and Whitaker (1972) pre-
sented the following equations for forced convection conditions, respectively:
0.15 0.31 0.5

Kramers (1946): Nu = 2 + 1.3 Pr + 0.66 Pr Re (32.1)
0.5 0.33
Ranz and Marshal (1952): Nu = 2 + 0.6 Re + Pr (32.2)
0.5 0.66 0.4 0.25

Whitaker (1972): Nu = 2 + (0.4 Re + 0.06 Re ) Pr (µ∞/µs) (32.3)

These correlations involve the Reynolds number as a dominant factor influencing
hfp. However, some researchers have defined the Reynolds number based on either
fluid or particle velocity, while others have used the relative velocity between particle
and fluid, also called slip velocity, which is the difference between fluid and particle
velocities. The slip velocity appears to be more suitable under the conditions of this
study. The Whitaker (1972) model suggests that fluid velocity far removed from the
particle should be used to calculate Re number. The particle velocity is easy to
measure. However, the fluid velocity in tube-flow conditions of a two-phase system
is a source of differences among the researchers. In the case of tube-flow conditions
with moving particles, several additional factors can influence particle motion and
thus the fluid-to-particle heat transfer coefficient. Particle shape and size, thermo-
physical properties of both particle and carrier fluid, and system parameters such as
tube diameter and fluid flow rate are some influencing factors. These parameters can
be grouped into dimensionless forms and included in the correlations. Further, to
improve the prediction of the developed model, other groups of dimensionless
numbers, such as the Peclet, Froude, and Rayleigh numbers, or dimensionless ratios
2
such as Gr/Re , d/D, αf/αp, and µ∞/µs have also been included in the empirical
equations. Some published empirical equations are presented in Table 32.1.
In the present study, the Nusselt number and generalized forms of the Reynolds,
Prandtl, and Grashof numbers were used and calculated as follows:
Nu = hfp dp/kf (32.4)
GRe = ρ Vs dp/µ (32.5)
GPr = Cp µ/kf (32.6)
2 3
GGr = g β ρ ∆T dp /µ (32.7)
where:
Vs = Vf − Vp (32.8)
∆T = (Tf − Tip)/2 (32.9)
2 2
Vf = Q/π (Rt − Rp ) (32.10)
Cp = 1.675 + 0.025 (%W) (32.11)
n−3 n 1−n
µ=2 m (3n + 1/n) (dp/Vs) (32.12)
2
kf = [326.575 + 1.0412 T − 0.000337 T ] [(0.796 + 0.009346 (%W)] (32.13)

TABLE 32.1
Some Published Dimensionless Correlations for Estimating Nusselt Number under Forced Convection Heat Transfer Conditions
Equation [Nu = f (Re, Pr…..)]
2
Reference Fluid Particle R
0.15 0.5 0.31
Kramers (1946) Air, oil, water Sphere (steel) 2 + 1.3Pr + 0.66Re Pr —
0.5 0.33
Ranz and Marshal (1952) Air Sphere 2 + 0.6Re Pr —
0.5 0.66 0.4 0.25
Whitaker (1972) Air, oil, water Sphere 2 + (0.4Re + 0.06Re ) Pr (µs/µ∞) —
a 0.21 0.14
Zuritz and Sastry (1987) CMC Mushroom (aluminum) 2 + 2.95Re Pr 0.99
0.44 0.35
Chandarana et al. (1988) Starch Cubes (silicone) 0.55Re Pr 0.92
0.43
Chandarana et al. (1988) Water Cubes (silicone) 0.85Re 0.95
1.6 0.89
Chandarana et al. (1990) Starch Cubes (silicone) 2 + 0.028Re Pr 0.79
1.08
Chandarana et al. (1990) Water Cubes (silicone) 2 + 0.0333Re 0.89
b 0.00455
Sastry et al. (1990) Water Sphere (hollow al ) moving therm. 6.46E–26[Re (d/D)] 0.82
b 0.0125 85.67 –342.5
Sastry et al. (1990) Water Sphere (hollow al ) moving therm. 2.7E–27Re (d/D) Pr 0.92
b 0.23 0.14 1.79
Zuritz et al. (1990) CMC Mushroom (al ) 2 + 28.37Re Pr (d/D) 0.96
0.108
Awuah et al. (1993) CMC Cylinders (carrot) 2.45(Pr Gr) 0.80
0.113
Awuah et al. (1993) CMC Cylinders (potato) 2.02(Pr Gr) 0.88
0.54
Astrom and Bark (1994) Silicon oil Spheres (lead) 8 + 2.53Re —
0.61
Astrom and Bark (1994) Silicon oil Cubes (lead) 8 + 2.25Re —
0.2 0.33
Bhamidipati and Singh (1995) CMC Cylinder (temp. sensor) 0.27Re Pr 0.85
0.132 –0.08
Kelly et al. (1995) CMC Sphere, cube, cylinder (aluminum) 2 + 19.36Re Pr 0.83
0.59 0.28
Baptista et al. (1997a) CMC Sphere (hollow aluminum) stationary Nus + 0.64Re Pr —
0.71 0.42 0.28
Baptista et al. (1997a) CMC Sphere (hollow aluminum) rotating Nus + 0.17Re Pr (rp/Rt) —
0.33 0.5
Nus = 2 + 0.025 Pr Gr
0.29 1.52 4.35
Chakrabandhu and Singh (1998) CMC Cubes (sodium alginate) stationary 18197Re Pr (d/D) 0.91
0.86 0.22 1.67
Chakrabandhu and Singh (1998) CMC Cubes (sodium alginate) rotating 338Re Pr (d/D) 0.89
a
CMC = carboxymethyl cellulose.
b
al = aluminum.
Data from two previous reports (Ramaswamy and Zareifard, 2000; Zareifard and
Ramaswamy, 2001) were used for developing correlations under tube-flow condi-
tions. The techniques for evaluating hfp have been detailed by Zareifard and
Ramaswamy (1997, 1999). A brief description of the two methods is given below
for reference:
32.3.1 CALORIMETRIC METHOD

The calorimetric method (Zareifard and Ramaswamy, 1999) involves an indirect
measurement of particle temperature. Instead of recording the particle center point
temperature, the mass average (bulk) temperature of a freely moving particle, which
is not attached to any thermocouple, is estimated using a calorimeter. Therefore, the
particle is allowed to flow with the carrier fluid along the tube without any restriction.
The technique consists of introducing a particle at an upstream location into a holding
tube, in which a carrier fluid under prestabilized temperature and flow conditions is
circulated, and retrieving it from a downstream location after a known time interval.
The particle is transferred immediately into a specially constructed calorimeter, and
its bulk temperature is determined upon equilibration. Knowing the medium tem-
perature, particle initial temperature, exposure time (residence time), and thermo-
physical properties, the associated hfp is computed from the evaluated bulk temper-
ature of the particle using an iterative numerical technique. The procedure involves
numerical computation, by trial and error, of bulk temperature (also known as mass
average temperature) for a given heating time (residence time), using the available
property data and an assumed hfp value, and comparing it with the experimental value.
Aluminium spherical particles of three sizes (19.05, 22.22, and 25.4 mm in diameter)
were used as test particles in a Pyrex glass holding tube (45 mm inside diameter).
32.3.2 PARTICLE OSCILLATORY MOTION METHOD

The particle oscillatory motion method (Zareifard and Ramaswamy, 1997) involves
direct measurement of center point temperature of thermocouple-equipped parti-
cles fixed at the center of a set of circular holding tubes of different radii cut out
in quarter lengths. An assembly of four such tubes is supported by an aluminum
shaft and connected to a programmable servo motor equipped with an electronic
board for imparting preset oscillatory motions.
Spherical nylon particles of three different sizes (12.7, 16, and 17.5 mm in
diameter) as well as spherical particles (17.5 mm in diameter) made of aluminum
epoxy (Soudotec Inc., Lachine, Quebec) were used as the test particles. The aluminum
epoxy particle was formed by mixing aluminum powder and epoxy resin in a soft
form. All test particles were drilled to insert thermocouples to their geometric centers.
The assembly of holding tubes containing the particles was kept in a cooling tank
at 5°C for equilibration of the temperature in test particles, and an appropriate
oscillatory motion was programmed to result in particle linear velocity in the range
0.06 to 0.21 m/sec. The assembly was then transferred to the test tank containing
a heating medium at a preset temperature. Time–temperature data were gathered at

3-sec time intervals using a data logger connected to a personal computer. Water as
well as two concentrations (0.5 and 1% w/w) of commercial carboxymethyl cellulose,
CMC (Sigma, St. Louis, MO) were used as the heating media.
Thermophysical properties of the different test particles such as density (ρ),
thermal diffusivity (α) and heat capacity (Cp) were experimentally evaluated using
procedures described elsewhere (Sablani and Ramaswamy, 1996). The thermal con-
ductivity (k) was calculated as k = ρCpα. Rheological data for test fluids at different
concentration and temperature were obtained in the form of power law model
parameters [consistency coefficient (m) and flow behavior index (n)] using a rota-
tional viscometer Model RV20 (Haake Mess-Technik, Karlsruhe, Germany) as
described by Abdelrahim and Ramaswamy (1995). These data are summarized in
Tables 32.2 and 32.3. Data obtained on hfp from the two techniques are given in Tables
32.4 and 32.5 and were used for developing the dimensionless correlations.
TABLE 32.2
Thermophysical Properties of Spherical Test Particles
a b b
Material Aluminum Aluminum Epoxy Nylon
3
Density (kg/m ) 2707 1750 1128
Heat capacity (J/kg K) 896 1370 2073
Thermal conductivity (W/m K) 204 1.13 0.37
2
Thermal diffusivity (m /sec) 8.42E–5 4.7E–7 1.58E–7
a
From Holman, G.P., Heat Transfer, McGraw-Hill, New York, 1990.
b
Measured experimentally.
TABLE 32.3
The Power Law Model Parameters of CMC Solutions
for Different Concentrations and Temperatures
Determined Using a Rotational Viscometer
CMC Temp. M
% °C Pa.sec
n
n
0.25 50 0.150 ± 0.031 0.785 ± 0.030

0.25 60 0.052 ± 0.018 0.821 ± 0.015
0.25 70 0.011 ± 0.028 0.976 ± 0.021
0.50 50 0.510 ± 0.020 0.590 ± 0.011
0.50 60 0.252 ± 0.033 0.681 ± 0.026
0.50 70 0.115 ± 0.045 0.754 ± 0.017
1 50 1.715 ± 0.151 0.560 ± 0.019
1 60 1.191 ± 0.101 0.510 ± 0.029
1 70 0.778 ± 0.082 0.583 ± 0.031
Note: Results are means ± standard deviations of three replicates (m:

consistency coefficient; n: flow behavior index).

TABLE 32.4
2
Values of hfp (W/m ·K) Associated with Aluminum Spherical Particles
of Different Sizes and Fluid Flow Rates with Various Fluid
Concentrations and Temperatures Using the Calorimetric Approach
% CMC Concentration
F (l/min) P T (°C) 0.0 0.25 0.5 1
s 740 (2.7)
m 50 800 (2.5)
l 870 (2.3)
s 680 (1.5)
9 m 60 730 (1.4)
l 800 (1.2)
s 650 (1.5)
m 70 700 (1.4)
l 750 (1.3)
s 920 (2.2) 790 (2.5) 750 (4.0)
m 50 690 (0.1) 880 (1.1) 860 (1.2)
l 980 (0.1) 950 (1.0) 900 (1.1)
s 890 (2.2) 770 (1.3) 710 (1.4)
11 m 60 990 (0.2) 830 (1.2) 780 (1.3)
l 1020 (1.0) 930 (1.1) 870 (1.1)
s 880 (2.3) 750 (1.3) 680 (1.5)
m 70 930 (2.1) 810 (2.5) 720 (1.4)
l 980 (0.1) 900 (1.1) 840 (1.2)
s 1090 (1.8) 890 (2.2)
m 50 1100 (1.8) 910 (2.2)
l 1190 (1.8) 1020 (2.9)
s 1070 (0.9) 820 (1.2)
13 m 60 1120 (3.6) 870 (1.1)
l 1180 (2.5) 970 (1.0)
s 1430 (3.5) 1000 (1.0) 740 (2.7)
m 70 1730 (3.5) 1070 (3.7) 810 (1.2)
l 2200 (2.7) 1140 (3.5) 890 (2.2)
s 1310 (1.5)
m 50 1420 (3.5)
l 1490 (4.0)
s 1260 (1.6)
16 m 60 1310 (1.5)
l 1390 (2.2)
s 1730 (5.2) 1240 (3.2)
m 70 2150 (3.7) 1320 (1.5)
l 2550 (2.3) 1350 (2.2)
s 2030 (3.4)
19 m 70 2300 (2.6)
l 2660 (3.4)
Note: Values of hfp are the means of four replicates, and the coefficient of variation is given in
parentheses. F: fluid flow rate; T: fluid temperature; P: particle size: s, small; m, medium; l, large.

TABLE 32.5
2
Values of hfp (W/m ·K) Associated with Different Fluid Concentrations and
Temperatures for Spherical Particles of Different Sizes and Materials at Vari-
ous Particle Velocities Using the Particle Oscillatory Motion Technique
2 2
Vp hfp (W/m ·K) Vp hfp (W/m ·K)
C (% CMC) T (°C) (m/sec) AL NL (m/sec) NS NM
0.10 1460 (11) 1120 (7) 0.06 1100 (11) 1070 (11)
0 60 0.16 1830 (11) 1310 (6) 0.09 1250 (12) 1120 (10)
0.21 2020 (9) 1410 (6) 0.12 1410 (8) 1320 (8)
0.10 590 (15) 460 (15) 0.06 520 (15) 430 (10)
60 0.16 950 (6) 620 (7) 0.09 720 (15) 580 (9)
0.21 1220 (9) 690 (9) 0.12 750 (18) 610 (12)
0.10 750 (5) 500 (18) 0.06 530 (3) 460(9)
0.5 70 0.16 — — 0.09 — —
0.21 1360 (9) 730 (7) 0.12 790 (12) 640 (15)
0.10 1140 (6) 640 (16) 0.06 600 (18) 520 (11)
80 0.16 1290 (3) 740 (14) 0.09 790 (9) 680 (13)
0.21 1380 (12) 800 (4) 0.12 840 (8) 730 (9)
0.10 530 (10) 430 (17) 0.06 360 (16) 350 (14)
60 0.16 570 (10) 520 (12) 0.09 420 (11) 440 (9)
0.21 630 (11) 620 (19) 0.12 570 (4) 530 (16)
0.10 650 (7) 490 (8) 0.06 490 (13) 430 (13)
1.0 70 0.16 730 (10) 530 (18) 0.09 530 (17) 510 (4)
0.21 880 (7) 660 (10) 0.12 610 (12) 580 (9)
0.10 720 (10) 500 (18) 0.06 520 (7) 470 (12)
80 0.16 1010 (8) 560 (17) 0.09 520 (10) 500 (4)
0.21 1110 (4) 740 (8) 0.12 660 (5) 640 (10)
Note: Values of hfp are the means of four replicates, and the coefficient of variation is given in parentheses.
Vp: particle velocity; T: medium temperature; C: medium concentration; AL; aluminum epoxy; NL: nylon
large; NS: nylon small; NM: nylon medium.

In the literature, the heat transfer coefficients associated with pure forced convection
with unbounded flow are generally modeled in dimensionless forms, as shown in
Equation (32.14).
c d
Nu = A + B Re Pr (32.14)
For tube-flow conditions involving biphasic systems, other dimensionless terms
are added to make the correlations better explain the experimental variability. In the
present study, regression analyses were performed starting with the simplest form
of correlation: Nu = f (GRe). This was progressively expanded to include other
dimensionless numbers such as GPr and GGr as well as other dimensionless groups:
2
αf/αp, GGr/GRe , d/D, Vp/Vf, and Vp/Vs. After successful improvement of the model

prediction by including other variables was observed, a multiple regression technique
with a backward elimination procedure using the SAS statistical package (SAS
Institute, 1994) to obtain the best model was adopted. The models were individually
developed with data from the calorimetric method and particle oscillatory motion
method and subsequently with the pooled data (600+ experimental values).

Regression analysis between the Nusselt number and other dimensionless groups
2
resulted in a number of correlations with different coefficients of determination (R )
and coefficients of variation (CV). Overall, these coefficients varied over the fol-
2
lowing ranges: 0.4 < R < 0.99; 1 < CV < 15%. As more dimensionless groups were
2
added to the correlation, the associated R and CV values demonstrated a progressive
improvement of the model. The following is the sequence of the regression analysis
with data obtained from the calorimetric method:
0.147 2
Nu = 2 + 1.84 E–1 GRe (R = 0.60; CV = 7.1) (32.15)
0.601 0.448 2
Nu = 2 + 2.49 E–1 GRe GPr (R = 0.71; CV = 6.1) (32.16)
0.440 0.681 0.191 2
Nu = 2 + 3.51 E–2 GRe GPr GGr (R = 0.73; CV = 5.8) (32.17)
0.25 –2.18
Nu = 2 + 1.15 E11 GRe GPr
−1.125 4.508 2
× GGr (d/D) (R = 0.91; CV = 3.2) (32.18)
0.479 −0.655 −0.526
Nu = 2 + 3.80 E4 GRe GPr GGr
2.293 0.514 2
× (d/D) (Vp/Vs) (R = 0.97; CV = 1.8) (32.19)
The simplistic form of the correlation relating Nu to just GRe (Equation (32.15))
yielded a fairly poor fit and largely scattered data points (not shown). This was
expected because GRe alone cannot be expected to explain all the variability asso-
ciated with Nu. The second correlation in the form of Nu as a function of Re and
Pr (Equation (32.16)) is commonly employed in many published reports including
the well known Ranz and Marshal correlation. Logarithmic plots of experimental
vs. predicted Nu based on Equations (32.16–19) are presented in Figure 32.1. The
2
R improved somewhat (from 0.6 to 0.7) with the inclusion of Pr in the model
(Equation (32.16), Figure 32.1a). Adding Gr to the model (Equation (32.17),
2 2
Figure 32.1b) did not improve R much since the range of Gr/Re employed was
less than 1.0, indicating that experimental conditions involved forced convection
rather than natural convection. Adding the ratio of particle-to-tube diameter d/D
(Equation (32.18), Figure 32.1c) resulted in a good improvement of the model, and
2
R increased from 0.7 to 0.9. Including the ratio of particle-to-slip velocity, Vp/Vs
(Equation (32.19), Figure 32.1d), also contributed to improving model prediction.
2
This combination model had an R greater than 0.97.
Because additional different forms of dimensionless numbers could have the
potential to improve the model performance, a multiple regression technique with
backward elimination of statistically insignificant (p > 0.05) terms was employed
to achieve the optimal model configuration. The regression analysis with the back-
ward elimination procedure resulted in the following model equation with the best

2 2
Predicted Log Nu R2 = 0.71 R2 = 0.73
Predicted Log Nu
1.8 1.8
1.6 1.6
1.4 1.4
1.2 1.2
1 1
1 1.2 1.4 1.6 1.8 2 2.2 1 1.2 1.4 1.6 1.8 2 2.2
Experimental Log Nu Experimental Log Nu
(a) (b)
2.2
2 2
R2 = 0.91 R2 = 0.97
Predicted Log Nu
Predicted Log Nu
1.8 1.8
1.6 1.6
1.4 1.4
1.2 1.2
1 1
1 1.2 1.4 1.6 1.8 2 2.2 1 1.2 1.4 1.6 1.8 2 2.2
Experimental Log Nu Experimental Log Nu
(c) (d)
FIGURE 32.1 Logarithmic plot of experimental vs. predicted Nusselt numbers using different
models: (a) Equation (32.16); (b) Equation (32.17); (c) Equation (32.18); (d) Equation (32.19).
2
fit (R = 0.98), employing about 300 experimental data points obtained from the
calorimetric method under different conditions:
0.589 0.977 0.231 −0.607 0.731 −8.402

Nu = 2 + 5.89 E24 GRe GPr GGr (Vp/Vf) (Vp/Vs) (αf/αp)
(32.20)
Figure 32.2 shows the plot of Nusselt numbers calculated from Equation (32.20)
vs. experimental values of Nusselt numbers obtained with the calorimetric method.
The same procedure, backward elimination, was also used for data obtained
2
from the particle oscillatory motion method, and the best model (R = 0.88) was
found to be:
2.032 1.120 −1.843 2 −0.316 0.305
Nu = 2 + 2.27 E–8 GPr GGr (d/D) (GGr/GRe ) (αf/αp) (32.21)

2.2
2
R2 = 0.98
1.8
Predicted Log Nu
1.6
1.4
1.2
1
1 1.2 1.4 1.6 1.8 2 2.2
Experimental Log Nu
FIGURE 32.2 Logarithmic plot of experimental vs. predicted Nusselt number for the best
model for data from the calorimetric method (Equation (32.20)).
Contributions from natural convection were accounted for by introducing both

2 2
GGr and the GGr/GRe ratio in Equation (32.21). The magnitude of Gr/Re describes
the ratio of buoyant to inertia forces indicating free, forced, and mixed convection
regimes (Chapman, 1989). Yuge (1960) indicated that forced convection dominates
2
for flow over a sphere when condition Gr/Re < 0.01 is satisfied. According to
Johnson et al. (1988), mixed convection occurs when the ratio falls between 0.08
and 5.1. Figure 32.3 shows the logarithmic plot of Nusselt numbers calculated from
Equation (32.21) vs. experimental values of Nusselt numbers obtained from the
particle oscillatory motion method. Model prediction of Nu using Equation (32.20)
2
(developed from the calorimetric approach) resulted in a better fit with an R of 0.98
than model Equation (32.21) (developed from oscillatory motion technique) with an
2 2 2
R of 0.88. The model R represents a combination of partial R associated with
individual parameters included in the model. Obviously, it is important to include
meaningful dimensionless numbers in the model. In this regard, the variables in
Equation (32.20) appear to do a better job (with calorimetric approach data). The
same variables did not give similar results with the data obtained from the oscillatory
technique. The lack of rotational motion of the particles (because of the attachment
of the thermocouple to the particle) could be a reason for the discrepancy. The overall
2
lower R associated with Equation (32.21) also indicates that perhaps some additional
parameters may be necessary to describe the rather unusual oscillatory motion for
the particles.

2
R2 = 0.88
1.5
Predicted Log Nu
0.5
0.5 1 1.5 2
Experimental Log Nu
FIGURE 32.3 Logarithmic plot of experimental vs. predicted Nusselt number for the best
model for data from the oscillatory motion technique (Equation (32.21)).
Multiple regression and backward elimination for all of the 600 experimental
2
data values obtained from both methods resulted in the following model (R = 0.91)
after including all the possible influencing factors associated with hfp:
0.555 −0.294 −0.352 1.628 1.748 −0.533
Nu = 2 + 4.45 E2 GRe GPr GGr (d/D) (Vp/Vf) (Vp/Vs)
0.227
× (αf/αp) (32.22)
The validity of the above equation is limited to the following ranges of the
dimensionless group numbers: 2.9 < GRe < 7660; 2.5 < GPr < 3077; 4.15 < GGr
< 1.5 E7; 0.2 < d/D < 0.6; 0.30 < Vp/Vf < 1; 0.43 < Vp/Vs < 3.37; and 0.33 < αf/αp
< 1892. Figure 32.4 shows the logarithmic plot of the Nusselt number calculated
from Equation (32.22) vs. experimental values of Nusselt numbers obtained from
the pooled data including both calorimetric and particle oscillatory motion methods.
It is worth mentioning that in the heat transfer literature the convective heat
transfer coefficient in the form of the Nusselt number is correlated to the Reynolds
and Prandtl numbers due to the influence of properties associated with the carrier
fluid, which can affect the boundary conditions. The constant value of two has been
reported in the developed correlations to be considered as a limiting Nusselt number
value for the steady state heat conduction between fluid and sphere. This number
may vary for different particle geometry (Whitaker, 1976). In the present study,
particle-to-tube diameter ratio (d/D) and thermal diffusivity ratio (αf/αp), as well as
velocity ratios (Vp/Vf or Vp/Vs) were found to be appropriate for hfp correlations
under tube-flow situations investigated.

2.2
2 R2 = 0.91
1.8
Predicted Log Nu
1.6
1.4
1.2
0.8
0.6
0.6 0.8 1 1.2 1.4 1.6 1.8 2 2.2
Experimental Log Nu
FIGURE 32.4 Logarithmic plot of experimental vs. predicted Nusselt number for the overall
model from the combined data (Equation (32.22)).
Dimensionless numbers as well as the associated coefficients in the above models

are different from those reported in the literature. Attempts to compare the above
model with others in the literature resulted in either overestimation or underestima-
tion of the Nusselt number. Comparison with well-known correlations such as those
of Ranz and Marshal (1952) or Whitaker (1972) is not possible because these
equations were derived for an unbounded flow situation. In general, it is difficult to
compare the empirical equations in the literature because of differences in experi-
mental procedures, and most importantly, differences in the range of Re number and
other dimensionless numbers which might differ from the experimental condition
for the present study.
32.5 CONCLUSIONS
Dimensionless correlations between Nusselt number and other dimensionless num-
bers were developed for data obtained from a particle oscillatory motion method
and a calorimetric approach separately as well as for the combination of data from
both. A multiple regression analysis with backward elimination procedure was used
to obtain the best model with statistically significant parameters associated with hfp.
Heat transfer to the particle from the carrier medium was modelled using Reynolds,
Prandtl, and Grashof numbers. Their relationships were attributed to the carrier fluid
and various parameters affecting the boundary condition. In addition, particle-to-
tube diameter ratio (d/D) and thermal diffusivity ratio (αf/αp) as well as velocity
ratio (Vp/Vf) were found to be appropriate for hfp correlations under tube-flow and

force convection situations investigated in the present study. Nusselt numbers esti-
mated from the developed models showed good agreement with experimental data
2
(R = 0.88–0.98).
NOMENCLATURE
a Radius of sphere (m)
Cp Heat capacity (J/Kg °C)
d Particle diameter (m)
D Inside tube diameter (m)
2
g Local acceleration due to gravity (m/sec )
2
hfp Fluid-to-particle heat transfer coefficient (W/m K)
k Thermal conductivity (W/m K)
n
m Consistency coefficient (Pa.sec )
n Flow behavior index
Rt Radius of the tube
Rp Radius of the particle
Tf Fluid or medium temperature
Ti Initial temperature
Tp Particle temperature
Vf Fluid velocity (m/sec)
Vp Particle velocity (m/sec)
Vs Slip velocity (m/sec)
W Moisture content (%)
GREEK LETTERS
2
α Thermal diffusivity (m /sec)
β Root of characteristic equation or thermal expansion coefficient (1/K)
3
ρ Density (kg/m )
2
µ Dynamic or apparent viscosity (µ = ρυ) (N.sec/m )
2
µ∞ Fluid apparent viscosity at bulk fluid temperature (N.sec/m )
DIMENSIONLESS NUMBERS
Bi Biot number (hfp a/kp)
2 3 2
Gr Grashof number (g β ρ ∆T d /µ )
Pr Prandtl number (µ Cp/kf or υ/α)
Re Reynolds number (ρ V d/µ)
Nu Nusselt number (hfp a/kf)
SUBSCRIPTS
f Fluid
fp Fluid-to-particle
i Initial

p Particle
s Surface or slip
∞ Ambient
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33 Modeling in Microwave
and Spouted Bed
Combined Drying
of Particulate Food
Products
H. Feng and J. Tang
CONTENTS
33.1 Introduction
33.2 Model Development
33.2.1 Transport Relations
33.2.2 Mass Balance
33.2.3 Energy Balance
33.2.4 Governing Equations
33.2.5 Initial and Boundary Conditions
33.3 Model Reduction
33.4 Effective Moisture Diffusivity
33.5 Permeability of Apple Tissues
33.6 Dielectric Properties and Microwave Power Absorption
33.7 Numerical Analysis
33.8 Experimental
33.9 Model Validation
33.10 Conclusions
Nomenclature
Acknowledgments
References
Appendix

33.1 INTRODUCTION
Microwave drying involves simultaneous heat, mass, and momentum transfer, as
well as volumetric heat generation. The internal heat generation results in the devel-
opment of a gas/vapor pressure gradient from interior to product surface that dis-
tinguishes microwave drying from other drying methods (Turner and Jolly, 1991).
Internal heat generation also produces a positive temperature gradient (from the interior
to the surface), in contrast to the negative temperature gradient produced during drying
by conventional hot air heating. A comprehensive heat and mass transfer analysis that
takes into account the contribution of the pressure gradient to moisture migration is
desirable in order to understand the underlying physics involved in microwave drying
and to predict temperature and moisture changes during drying.
Moisture exists in porous food material in the forms of free water, bound water,
and vapor. The migration of moisture through the food can be caused by the indi-
vidual or combined contributions of moisture, temperature, and pressure gradients.
In microwave drying, free water transport has been attributed to diffusion (Torringa
et al., 1996; Adu and Otten, 1996) or capillary flow (Wei et al., 1985; Constant et al.,
1996; Lian et al., 1997; Turner et al., 1998; Ni et al., 1999). For vapor migration,
diffusion (Lian et al., 1997), capillary flow (Turner et al., 1998; Ni et al., 1999) and
a combination of capillary flow and diffusion (Chen and Schmidt, 1990; Constant
et al., 1996) have been considered as transport mechanisms. Few studies have con-
sidered the migration of bound water. In studies regarding the mechanism of bound
water transfer, Turner et al. (1998) assumed that bound water transfer was caused
by diffusion, while Chen and Pei (1989) employed a capillary mechanism to char-
acterize bound water flow.
Knowledge of thermophysical and dielectric properties is essential to a heat and
mass transfer analysis in microwave drying. There is a lack of understanding of the
thermophysical and dielectric properties needed in such an analysis, especially for
food materials. Moisture diffusivity, permeability, and dielectric properties were used
in this study to account for moisture gradient driven flow, pressure gradient driven
flow, and microwave heat generation. It is important to understand the effect of
moisture content and product temperature on these properties.
In order to understand more about microwaves and their application to drying,
it is necessary to develop a comprehensive heat and mass transfer model for micro-
wave and spouted bed combined drying of hygroscopic porous food products; to
determine moisture diffusivity, permeability, and dielectric properties for a model
food, apple tissue; and to experimentally validate the model developed in this study.
33.2 MODEL DEVELOPMENT

In this study, drying of a particulate product was conducted in a spouted bed placed
in a microwave cavity. Microwave energy was applied to the cavity at a constant and
adjustable rate. The hot air velocity was set such that the aerodynamic conditions
needed to sustain stable fluidization in the spouted bed could be realized. The pneu-
matic agitation in the spouted bed helped to improve the heating uniformity among
particles during microwave drying. The hot air flow was at constant temperature.

The following assumptions were used in model development: the material is
homogeneous and isotropic on the macro scale; transport of free water is governed by
the generalized Darcy’s law; bound water transport is driven by chemical potential
difference (Stanish et al., 1986; Gong, 1992); and transport in the gas phase is deter-
mined by the contribution of convection and diffusion. Other assumptions included:
1. Local thermodynamic equilibrium exists, that is, the solid, liquid, and gas
phases are at the same average temperature at any moment in a control
volume.
2. Solid, liquid, and gas phases are continuous.
3. The binary gas mixture of air and vapor obeys the ideal gas law.
4. Vapor pressure as a function of moisture content and temperature can be
estimated using sorption isotherms.
5. The model material used in this study, diced apples, can be treated as
equivalent spheres.
6. The diced apples are exposed to a uniform microwave field.
7. Electromagnetic field intensity is uniform throughout diced apples.
The governing equations for microwave drying were derived at a macroscopic

level. Variables examined in this study are averaged values over a control volume.
This approach was first proposed by Whitaker (1977) and has been widely used in
multiphase heat and mass transfer studies related to drying of porous materials
(Bories, 1991).
33.2.1 TRANSPORT RELATIONS

Fluid velocities in a multiphase porous food system are given by the generalized
Darcy’s law:
r Kk rf r
uf = − (∇Pg − ∇Pc − ρf g) (33.1)
µf
r Kk rg r
ug = − (∇Pg − ρg g) (33.2)
µg
where the capillary pressure Pc = Pg – Pf. Diffusion of vapor and air is governed by
Fick’s law:
r r ρ 
jv = − ja = − ρg D av ∇ v  (33.3)
 ρg 
In many food materials, bound water migration is important. It has been found
that migration of the bound water cannot be simply treated as a diffusion process
(Chen and Pei, 1989). In the present study, a universal driving force, the chemical

potential gradient, was employed as the driving force for the bound water flow
(Gong, 1992). The bound water flux is then given by:
∂ µb
n b = D b (1 − ε ′) (33.4)
∂z
From the local thermodynamic equilibrium assumption, the chemical potential

of bound water, µ′b, equals the chemical potential of vapor, µ′v. Hence thermody-
namic relations for vapor can be used to express the bound water flux. A detailed
derivation can be found elsewhere (Stanish et al., 1986), and the resulting equation
is given in Equation (33.7).
Thermal diffusion through a food material is controlled by Fourier’s law:
r
q = − λ eff ∇T (33.5)
33.2.2 MASS BALANCE

The mass balance equations for free water, bound water, vapor, and air can be written
as:
∂Xf r
Free water: (1 − ε )ρs + ∇ ⋅n f = − m
˙ (33.6)
∂t
∂X b r
Bound water: (1 − ε )ρs + ∇⋅ n b = − m
˙b (33.7)
∂t
∂X v r
Vapor: (1 − ε )ρs + ∇⋅ n v = m
˙ +m
˙b (33.8)
∂t
∂Xa r
Air: (1 − ε )ρs + ∇⋅ n a = 0 (33.9)
∂t
In Equations (33.6–9), the mass fluxes are specified by:
r r Kk rf Kk rf
Free water: n f = ρf u f = − ρf ∇Pl = − ρf ∇( Pg − Pc ) (33.10)
µf µf
r r  ε ∇Pv Sv 
Bound water: n b = ρb u b = −ρb D b (1 − ε ′) − ∇T (33.11)
 ρv Mv 
r r r Kk rg ρ 
Vapor: n v = ρv u v + jv = − ρv ∇Pg − ρg Dav ∇ v  (33.12)
µg  ρg 

r r r Kk rg ρ 
Air: n a = ρa u a + ja = −ρa ∇Pg + ρg Dav ∇ v  (33.13)
µg  ρg 
v r r Kk rg
Gas: n g = n a + n v = − ρg ∇Pg (33.14)
µg
In Equation (33.10), the free water transfer caused by gravity is ignored, and in
Equation (33.14), ρg = ρa + ρv.
33.2.3 ENERGY BALANCE

The total energy balance for a representative elementary volume is written as (Bird
et al., 1960):
∂ r r DP
(ρ h ) + ∇ ⋅(ρ uh ) = − (∇ q ) − ( τ: ∇ u) + +Φ (33.15)
∂t Dt
r
The viscous dissipation term ( τ:∇µ ) and pressure work term (DP/Dt) are usually
negligible. Hence, Equation (33.15) reduces to an enthalpy balance equation:
∂ r
(ρ h ) + ∇ ⋅(ρ uh ) = − (∇ q ) + Φ (33.16)
∂t
where
ρ h = ρs h s + ρv h v + ρa h a + (ρf + ρb ) h l (33.17)
r r r r r
ρ uh = ρv u v h v + ρa u a h a + (ρf u f + ρb u b ) h l (33.18)
33.2.4 GOVERNING EQUATIONS

Due to the geometric symmetry, moisture transfer was assumed to take place only
in the radial direction. Hence, a one-dimensional heat and mass transfer problem in
spherical coordinates was considered. The total moisture transport equation can be
obtained by adding Equations (33.6) to (33.8); the temperature equation was obtained
by substituting Equations (33.5), (33.17), and (33.18) into the enthalpy balance
equation (Equation (33.16)), and the total pressure equation was obtained from the
air balance equation (Equation (33.9)). The resulting drying equations are as follows:
∂Xl 1 ∂  2 ∂Xl ∂T ∂ Pg 
= 2 D X r + DT r 2 + DP r 2  (33.19)
∂t r ∂r  ∂r ∂r ∂r 

∂Xl ∂T 1 ∂  2 ∂Xl ∂T ∂ Pg 
C TX + C TT = 2 D r + D TT r 2 + D TP r 2 +Φ (33.20)
∂t ∂t r ∂ r  TX ∂r ∂r ∂r 
∂Xl ∂T ∂ Pg 1 ∂  a 2 ∂Xl ∂T ∂ Pg 
C PX + C PT + C PP = 2 D X r + D aT r 2 + D aP r 2 
∂t ∂t ∂t r ∂r  ∂r ∂r ∂r 
(33.21)
k
In Equations (33.19) to (33.21), Dij and Cij are kinetic and capacity coefficients,
respectively. The subscripts i and j can be temperature, moisture, or pressure, while
the superscript k denotes air, free water, bound water, or vapor. The expressions for
these coefficients are detailed in this chapter’s Appendix
33.2.5 INITIAL AND BOUNDARY CONDITIONS

Initial conditions can be written as:
Xl t =0 = X0 T t =0 = T0 Pg t =0 = Patm (33.22)
Because of the pneumatic agitation in a spouted bed, it is reasonable to assume

that moisture arriving at a sample surface from the interior evaporates immediately
and is carried away by the hot air stream. The moisture transfer boundary condition
in spherical coordinates is then given by:
 ∂Xl ∂T ∂ Pg 
−(1 − ε )ρs  D X + DT + DP = ε h m (ρ vs − ρ v∞ ) (33.23)
 ∂r ∂r ∂ r 
r =R0
An energy balance over the interface can be set up to obtain the temperature
boundary condition:
∂T  ∂Xl ∂T ∂ Pg 
− λ eff
∂r
(
= h ( T∞ − Ts ) − ∆h v (1 − ε )ρs  D fX + D Xb
∂r
)
+ D fT + D Tb(∂r
+ D fP )∂r 

r =R0 
(33.24)
Pressure at the surface of a spherical particle can be written as:
P r =R0 = Patm (33.25)
The symmetry condition at the center of the sphere must be satisfied:
∂ Xl ∂T ∂ Pg
= = =0 (33.26)
∂r r=0
∂r r=0
∂r r=0

33.3 MODEL REDUCTION
To simplify the microwave drying equations given in Equations (33.19–33.21) and
(33.22–33.26) for numerical analysis and further elucidation of the mechanisms, a
scaling method was used to analyze the magnitude of each term in the equations.
The following scaling groups were used (Plumb et al., 1986):
r t T − T0 Pg − Patm
r∗ = ; t∗ = ; T∗ = ; Pg∗ =
R0 tc Tmax − T0 Pmax − Patm
Xl Xb − Xe ρvs P T
X∗l = ; X∗b = ; ρ∗vs = = vs ∞ ; (33.27)
X0 X0 − Xe ρ v∞ Pv∞ Ts
R0 µ a∞ R 20 K 0 Pmax − Patm Φ
tc = = ; uc = ; Φ∗ =
u c K 0 ( Pmax − Patm ) µ a∞ R0 Φ0
In the scaling analysis, a comparison of the magnitude of each dimensionless

group helped to determine which terms were insignificant and hence negligible. In
the analysis, a term with a coefficient at least one magnitude smaller than the other
terms was considered negligible and was eliminated from the drying equations. The
magnitude for each term was assessed by using literature values of the physical,
thermal, and transport parameters in the capacity and kinetic coefficients. For moisture-
dependent parameters, two extreme moistures, X0 = 7.0 (db) and Xl = 0.1 (db), were
used to estimate the range of the coefficients. For temperature-dependent parameters,
an average drying temperature of 343°K was used. Detailed analyses can be found
elsewhere (Feng, 2000). Simplified drying equations can be written as:
∂  ∗2  ∂ X∗l ( Pmax − Patm ) ρf Kk rf ∂ Pg  

∗
∂ X1∗ Tc
=  r D X +  (33.28)
∂ t∗ R 20 X 0 r ∗2 ∂ r ∗   eff 0 ∂ r ∗ 1− ε ρs µ f ∂ r ∗  
Tmax − T0 ∂ T∗ Tmax − T0 ∂  ∗
∗2 ∂ T  ˙ + Φ Φ∗
(ρC p )eff =  λ r  + ∆h v M (33.29)
tc ∂ t∗ R 20 r ∗2 ∂ r ∗  eff ∂ r∗  0
ρaρs X 0 ∂ X∗l  1 − ε ρs  ε M a Pmax − Patm ∂ Pg∗

(1 − ε ) ∗
+ 1 − Xl 
ρf t c ∂ t  ε ρf + ρ b  R ′ T tc ∂ t∗
1 ∂  ∗2 Kk rg ∂ Pg∗ 
= 2 ∗2 r ( Pmax − Patm )ρa  (33.30)
R r
0 ∂ r∗  µ g ∂ r ∗ 
The simplified boundary conditions are given by:
∗
1  ∂ X∗ P − Patm ρf Kk rf ∂ Pg  ερv∞ h m ∗
 Deff X 0 ∗l + max ∗ 
=− (ρ − 1) (33.31)
R0  ∂r 1 − ε ρs µ f ∂ r  (1 − ε )ρs vs
r ∗ =1

λ eff (Tmax − T0 ) ∂ T∗
− = h (T∞ − T0 ) − hTs∗ (Tmax − T0 )
R0 ∂ r∗ ∗
r =1
∗
∆h v (1 − ε )ρs  ∂ X∗ ( P − P ) ρ Kk rf ∂ Pg 
− Deff X 0 ∗l + max atm f  (33.32)
R0  ∂r 1− ε ρs µ f ∂ r ∗ 
P*| r*=1 =0 (33.33)
∂ X ∗l ∂T∗ ∂ Pg∗
= = =0 (33.34)
∂r∗ r∗ = 0
∂r∗ ∗
∂r∗ ∗
r =0 r =0
It can be seen from Equations (33.28–33.34) that terms with capillary pressure
were eliminated through the scaling analysis. The remaining unknown parameters in
Equations (33.28–33.34) include effective moisture diffusivity, intrinsic and relative
permeabilities, and dielectric properties. Experiments were designed and conducted
in this study to measure these properties as function of moisture and temperature.
All other thermal and transport relations for apples are from the literature and are
listed in Table 33.1.
TABLE 33.1
Correlations for Physical, Thermal, Thermodynamic, Dielectric, and Mass
Transfer Parameters
Parameter Correlation Reference
1.282 + 1.65(1.899 + X l )X l
Porosity, ε' ε′ = Feng, 2000
(1 + 1.65X l )(1.899 + X l )
Viscosity of free water, µf µ f (T) = µ f 0 exp(a − bT + cT 2 + dT 3 − eT 4 ) Turner, 1991
−4
µf0 = 1 × 10 ; a = 29.619;
−4
b = 0.152; c = 0.648 × 10 ;
−6 −8
d = 0.815 × 10 ; e = 0.120 × 10
Viscosity of gas, µg µ g (T) = µ g 0 {T 1/ 2 / (a + b / T − c / T 2 + d / T 3 )} Turner, 1991
a = 0.672; b = 85.229; c = 2111.475;
−6
d = 106417.0; µg0 = 1 × 10
Latent heat of water, ∆hv
6 2
∆hv = 2.792 × 10 − 160 T − 3.43 T Stanish et al., 1986
Effective thermal conductivity λeff = 0.12631 + 0.0595 Xl Donsì et al., 1996
of apple, λeff
Thermal conductivity λ a = 0.0035 + 7.67 × 10 −5 ∗ T Turner, 1991
of air, λa
Effective specific heat 27.21 X l Niesterus, 1996
of apple, Cpeff C peff = 1415 +
1 + Xl
Air–vapor binary diffusivity, 1.75 Stanish et al., 1986
101325  T 
Dav D av = 2.20 × 10 −5
Pg  273.15 

33.4 EFFECTIVE MOISTURE DIFFUSIVITY
The effective moisture diffusivity Deff combines the contributions of both bound
water and free water. From Equation (33.28), it can be seen that Deff can be deter-
mined with a hot air–only drying test at moderate temperatures, in which the internal
vapor generation is negligible. Drying tests with apple tissues were conducted, and
Deff was obtained using the slope method (Feng et al., 2000a). Deff as function of
moisture content and temperature is given in the following equation:
 a + a2 ∗ Xl 
D eff = a 0 ∗ exp − 1  (33.35)
 T 
−4 3 2
where a0 = 6.273 × 10 ; a1 = 5.843 × 10 ; and a2 = –2.038 × 10 .
33.5 PERMEABILITY OF APPLE TISSUES

Intrinsic and relative permeabilities of apple tissues were measured with a set-up
designed based on the following relation:
K (ε ) k rg ∆Pg
Q g = ug A = − A (33.36)
µg H
From Equation (33.36), when the gas phase flow rate Qg and pressure drop over
a specimen ∆Pg are determined, the product of intrinsic permeability K and gas
relative permeability krg can be obtained. The separation of K with krg was achieved
by conducting a dry sample test in which krg = 1 and thus K as function of porosity
could be attained. Details of the set-up and experimental procedures can be found
in Feng et al. (2002b).
The intrinsic permeability K(ε) of apple tissue as a function of porosity was
determined by the above method and can be fitted to a Kozeny–Carman equation:
ε3
K(ε ) = 5.578 × 10 −12 (33.37)
(1 − ε ) 2
The gas and liquid relative permeabilities for apple tissue were also determined
(Feng et al., 2002b) and can be correlated to saturation level S using the following
empirical equations:
k rg = 1.01 e −10.86 S (33.38)
k rl = S3 (33.39)

33.6 DIELECTRIC PROPERTIES AND MICROWAVE
POWER ABSORPTION
Dielectric constant ε* and loss factor ε″ are important parameters in the determina-
tion of microwave penetration depth and volumetric heat generation. The open-ended
coaxial probe technique was used to measure ε* and ε″ for apple tissues over a
moisture content range of 4 to 87.5% (wb) and at 22 and 60°C. From measured
results with apple tissues, a correlation of loss factor ε″ with moisture and temper-
ature changes was obtained (Feng et al., 2000):
ε ′′ = a 1 + a 2 T + a 3 T 2 + a 4 X + a 5 X T + a 6 X T 2 + a 7 X 2 + a 8 X 2 T + a 9 X 3 (33.40)
where a1 = −23.5999; a2 = 0.158233; a3 = −0.000256978; a4 = −1.87998; a5 =

−6 −5
0.00768435; a6 = −5.6363 × 10 ; a7 = 0.0289568; a8 = −7.66337 × 10 ; a9 =
−5
−4.09947 × 10 .
Microwave power absorption by the sample during drying can be obtained using:
ε ′′
Φ = Φ0 (33.41)
ε ′′0
where Φ0 is the absorbed microwave power at the beginning of a microwave and

spouted bed drying (MWSB) drying test. It is given by Φ0 = Φinput − Φreflect, the
difference between measured input and reflected power. ε ′′0 is the loss factor corre-
sponding to the value at the beginning of a drying test.
33.7 NUMERICAL ANALYSIS

The simplified drying equations (Equations (33.28) to (33.34)) are coupled and
highly nonlinear. The finite difference method was used to find numerical solutions.
The analytical domain was a sphere with a diameter of 5 mm divided into 15 layers,
each with a thickness δ = 1/3 mm. A time step of 1 sec was selected in the simulation.
The Crank–Nicolson scheme was used to discretize the partial differential equations
for the internal nodes. The boundary conditions at nodes 0 and 16 were discretized
with a three-point formula to obtain the same accuracy as with internal nodes. The
moisture, temperature, and gas pressure equations were solved simultaneously. A
program was written using Matlab to implement the simulation. Details of the finite
difference formulation can be found elsewhere (Feng, 2000).
33.8 EXPERIMENTAL
A microwave and spouted bed combined drying system was developed to conduct
drying tests to validate the model simulation. This system consisted of a 2.45 GHz
microwave supply system and a hot air system (Figure 33.1). In the microwave
supply system, a magnetron generated the microwaves, a wave guide transmitted

1 2
3
10 5
11 6
12 7
Air
8
9
FIGURE 33.1 Schematic of 2.45 GHz microwave and spouted bed drying system. 1. Direc-
tion coupler; 2. circulator; 3. magnetron; 4. power controller; 5. power meter; 6. temperature
controller; 7. HP network analyzer; 8. air pump; 9. heater; 10. three-stub tuner; 11. microwave
cavity; 12. spouted bed.
the waves to the cavity, and a directional coupler with power meters measured power
components. In the system, a circulator with a water load was installed to absorb
the reflected power and a three-stub tuner was used to adjust the matching impedance
of the drying cavity. The power generated from the magnetron could be continuously
adjusted using the power controller. Both the incident and the reflected power were
measured using HP power meters so that the power absorbed by the drying sample
could be accurately determined.
Diced Red Delicious apples (Malus domestica Borkh) with average initial mois-
ture content of 20.2% (wb) were used as the model food in the validation. The
spouted bed superficial air velocity was 2.1 m/sec in all experiments, the velocity
at which a stable particle circulation can be achieved during drying to ensure uniform
heating. Forty grams of diced apples were used in each drying test. Moisture loss
was monitored by periodically weighing the sample on an electric balance. The
average moisture content of samples was determined using the vacuum oven method
(AOAC, 1990). The drying temperature of the dice was measured at the core of ten
randomly chosen apple pieces with a type T thermocouple (response time 0.8 sec) at
predesignated time intervals. The pressure increase during microwave heating was
measured using fresh apples with a fiber optical pressure probe, which has a reso-
lution of 1 kPa. The pressure probe was led through a hole opened on the wall of
the spouted bed and inserted into the center of a fresh-cut apple sample sealed with

vacuum grease to prevent vapor leakage. A data acquisition system was used to
record the pressure data.
33.9 MODEL VALIDATION

Figure 33.2 compares the predicted and experimentally determined moisture con-
tents for MWSB and spouted bed (SB) drying. In MWSB drying, the data reported
were the averages of four replicates, and drying tests were conducted at microwave
power density of 4 W/g (wb) and hot air temperature of 70°C. For SB alone drying,
the same air conditions as for MWSB drying were used, and experiments were
performed in triplicate. Relatively small error bars in Figure 33.2 indicate good
repeatability in drying tests.
The simulated moisture content followed an exponential decay curve that char-
acterizes drying in the falling rate period for hygroscopic materials. At the beginning
of drying, the simulation slightly underestimated moisture loss. The assumption of
spherical geometry for apple dice might be a major reason for this discrepancy due
to an underestimation of the surface-to-volume ratio. Generally, model predictions
were in good agreement with experiments for both drying methods.
The temperatures measured from diced apples and predicted with the model are
compared in Figure 33.3 for MWSB (MW power 4 W/g and air temperature 70°C)
and SB (air temperature 70°C) drying. Temperature prediction in MWSB drying
agreed well with the measured values. At the beginning of drying, the hot air heated
the apple dice from outside, and the microwaves heated volumetrically. This led to
a rapid increase in product temperature. When the apple dice surface temperature
surpassed the air temperature, the air started to cool the apple dice. The center
temperature, however, continued to increase as a result of microwave heating until it
reached about 83°C, when a balance between the energy supplied by microwaves
and the heat losses due to surface convective cooling and evaporation was established.
25
Model prediction
Moisture Content (wb), %
20 SB drying test
MWSB drying test
15
10
0
0 10 20 30 40 50 60 70 80 90
Drying Time, min
FIGURE 33.2 Moisture content comparison between model predictions and experimental
results for microwave and spouted bed (MWSB) drying and spouted bed (SB) drying. (From
Feng, H. et al., AICHE J., 47(7), 1499–1509, 2001. With permission.)

90
80
Bed temperature
70
Temperature, °C
60
50
40
30
Model prediction
20 SB drying test
10 MWSB drying test
0
0 10 20 30 40 50 60 70 80 90
Drying Time, min
FIGURE 33.3 Temperature comparison between model predictions and experimental results
for MWSB and SB drying. (From Feng, H. et al., AICHE J., 47(7), 1499–1509, 2001. With
permission.)
10
8
Over-pressure, kPa
Experiment #1
2 Experiment #2
Experiment #3
0 Model
0 1 2 3 4 5
Drying Time, min
FIGURE 33.4 Comparison of predicted and measured pressures for MWSB drying with
microwave power 10 W/g, hot-air temperature 70°C and initial moisture content 84% (wb).
(From Feng, H. et al., AICHE J., 47(7), 1499–1509, 2001. With permission.)
The product temperature remained nearly constant throughout the rest of drying.
This is a unique feature associated with MWSB drying. The high surface heat transfer
in the spouted bed helped to maintain a nearly constant drying temperature. This
temperature leveling effect prevents the product from overheating and charring.
Therefore, MWSB drying has potential application in drying of heat-sensitive food
products. In SB drying, the sample temperature approached air temperature at a
slightly lower rate compared to that of MWSB drying, and the predicted temperature
agreed well with the bed temperature.
The over-pressure readings measured with the fiber optical probe are compared
to model prediction in Figure 33.4. Experiments to validate model prediction of
pressure were conducted at conditions different from those for moisture and

temperature verification. This is because at the moisture content of commercial
evaporated diced apple (20.2%), and the power level used in moisture and temper-
ature validation tests, the over-pressure generated is lower than the threshold of the
pressure probe (1 kPa). To generate a vapor pressure above the threshold of the
pressure probe (1 kPa), fresh apple samples in a cylindrical shape (8 mm in diameter
and 15 mm in length), and microwave power of 10 W/g and sample moisture of
84% (wb) were used in the tests. The measured pressure increased during the first
two minutes of drying to reach a peak and started to decrease thereafter. At this
stage, the moisture content of the sample remained high, and hence volumetric
heating was still intensive enough to maintain the pressure. Therefore, the measured
pressure decrease might have been caused by a gradual failure of the seal to the
pressure probe.
33.10 CONCLUSIONS
The comprehensive heat and mass transfer drying model developed in this study was
demonstrated to be an effective tool to predict moisture, temperature, and pressure
history and distribution for MWSB of particulate foods. The model prediction of
moisture, temperature, and pressure agreed with experimental results. A temperature
leveling effect was predicted and in agreement with experiment results. This unique
temperature leveling effect in MWSB drying makes it possible to use this method
for drying heat-sensitive food products.
NOMENCLATURE
C Capacity coefficient
−1 −1
Cp Specific heat, J·kg K
D Kinetic coefficient; material derivative
2 −1
Dav Binary air–vapor diffusivity, m ·sec
2 −1
Db Bound water diffusivity, m ·sec
−2
g Gravitational acceleration, m·sec
−1 −2 −1
h Enthalpy, J·kg ; surface heat transfer coefficient, W·m K
−1
∆hv Latent heat of free water, J·kg
−2 −1
j Diffusive mass flux, kg·m ·sec
kr Relative permeability
2
K Intrinsic permeability, m
−3 −1
ṁ Moisture evaporation rate, kg·m ·sec
−1
M Molar mass, kg·mol
−2 −1
n Mass flux, kg·m sec
P Pressure, Pa
Pc Capillary pressure, Pa
−2 −1
q Heat flux, J·m ·sec
−1
R Sample radius, m
−1 −1
R′ Universal gas constant, J·mol K
S Saturation
t Time, sec

T Average absolute temperature, K
−1
u Spouted bed air superficial velocity, m·sec
−1
X Moisture content (dry basis), kg H2O·(kg solid)
GREEK SYMBOLS
ε Porosity [(gas + liquid)/total volume], tolerance limit on iteration scheme
ε′ Porosity defined in Table I (gas volume/total volume); dielectric constant
ε* Dielectric constant
ε″ Dielectric loss factor
−3
Φ Heat source, W·m
−1 −1
λ Thermal conductivity, W·m ·K ; wave length, m
−1 −1
µ Dynamic viscosity, kg·m ·sec
µ′ Chemical potential
−3
ρ Density, kg·m
−3
ρs Solid density (solid mass/solid volume), kg·m
−2
τ Shear stress tensor, kg·m
SUBSCRIPTS AND SUPERSCRIPTS

0 At saturated condition or free space; initial condition (refers to fresh sample)
a Air
atm Atmospheric pressure
b Bound water, bulk density
eff Effective
f Free water
g Gas = air + vapor
l Liquid = free water + bound water
max Maximum values
P Pressure
s Solid, or relating to surface
T Temperature
v Vapor
w Total moisture = free water + bound water + vapor
X Moisture
∞ Surrounding
ACKNOWLEDGMENTS
Support for this research has been provided by Washington State University IMPACT
Center and the Northwest Center for Small Fruits Research. Special thanks go to
Dr. Ovid Plumb and Dr. Ralph Cavalieri for their valuable input to this work. The
authors would like to thank Timothy Wig and Wayne DeWitt for assistance in
developing the 2.45 GHz MWSB drying system, and TreeTop, Inc., Selah, WA, for
donating evaporated apples.

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APPENDIX
1 ρf Kk rf  ∂ Pc  1 ρf Kk rf  ∂ Pc 
D fX = − ; D fT = −  
1 − ε ρs µ f  ∂ X w  T 1 − ε ρs µ f  ∂ T  X
w
1 ρf Kk rf
D fP =
1 − ε ρs µ f
1 − ε ′ D b ε R ′ T  ∂ Pv 
D Xb =
1 − ε ρs Pv M v  ∂ X w  T
1 − ε ′ D b  Sv ε R ′ T  ∂ Pv  
D Tb = −  −   ; D P = 0
b
1 − ε ρs  M v Pv M v  ∂ T  X 
 w
Dav Pg Ma M v  ∂ Pv 
D Xv =
(1 − ε )ρs R ′ T( Pg M a + (M v − M a )Pv )  ∂ X w  T
Dav Pg Ma M v  ∂ Pv 
D Tv =  
(1 − ε )ρs R ′ T( Pg M a + (M v − M a )Pv )  ∂ T  X
w
1  P M Kk rg D av M a M v Pv 
D Pv =  v v − 
(1 − ε )ρs  R ′ T µ g R ′ T( Pg M a + (M v − M a )Pv ) 
Mv  (1 − ε )ρs Pv  (1 − ε )ρs  1 ∂Pv 

C TX = ∆h v − + ε − X 
R′  ρf + ρ b T  ρf + ρ b l  T ∂ X l 
Mv  (1 − ε )ρs  ∂( Pv / T)
C TT = (ρC p ) eff + ∆h v ε − X
R′  ρf + ρb l  ∂ T

D TX = ∆h v (1 − ε )ρsD Xv ; D TT = λ eff + ∆h v (1 − ε )ρsD Tv
D TP = ∆h v (1 − ε )ρsD Pv
ε M a  Pg − Pv  1 − ε ρs   1 − ε ρs  1 ∂Pv 
C PX = −   − 1 − Xl  
R ′  T  ε ρf + ρb   ε ρf + ρ b  T ∂ X l 
εMa  1 − ε ρs   Pg ∂( Pv / T) 
C PT = 1 − ε ρ + ρ X l   T 2 − ∂ T 
R′  f b 
εMa  1 − ε ρs  1
C PP = 1 − ε ρ + ρ X l  T
R′  f b 
Mv Pg M a  ∂ Pv 
D aX = − (1 − ε )ρs D Xv = − D av  ∂X 
R ′ T Pg M a + (M v − M a )Pv  wT
Mv Pg M a  ∂ Pv 
D aT = − (1 − ε )ρs D Tv = − D av  
R ′ T Pg M a + (M v − M a )Pv  ∂ T  X
w
( Pg − Pv )M a Kk rg Mv Pv M a
D aP = + D av
R′T µg R ′ T Pg M a + (M v − M a )Pv

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Transport Phenomena

© 2003 by CRC Press LLC

Transport phenomena in food processing / edited by Jorge Welti-Chanes, Jorge F. Vélez-Ruiz,

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No claim to original U.S. Government works

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A. Angersbach A.F. Baroni

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M.A. Castro S.L. Cuppett

X.D. Chen M.M. Farid

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F.C. Menegalli N. Nitin

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C.L. Weller S.E. Zorrilla

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Part II Mass Transfer

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Part III Heat Transfer

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1.2 MASS TRANSFER VARIABLES

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FIGURE 1.1 Scheme of individual and bulk velocities of a binary mixture.

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where vi is the velocity of component i with respect to stationary coordinates.

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1.2.4 FLUX RELATIONS FOR BINARY SYSTEMS

Substituting V from Equation (1.12) into Equation (1.22),

Since N A = C A V A and N B = C B V B , for component A, Equation (1.23) becomes:

A similar mathematical derivation gives for component B:

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1. Diffusion of A through stagnant B, NB = 0

1.3 MASS TRANSFER BY DIFFUSION

1.3.1 STEADY STATE DIFFUSION

1.3.2 MOLECULAR DIFFUSION IN GASES, LIQUIDS, AND SOLIDS

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The diffusion coefﬁcient of component A through B (DAB) may be estimated for

1.3.2.2 Molecular Diffusion in Liquids

The diffusivity of a solute A in a dilute solution B (DAB) can be predicted by the

1.3.2.3 Molecular Diffusion in Solids

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which applies for equimolar counter-diffusion.

1.3.3 UNSTEADY STATE DIFFUSION

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Solutions to unsteady state diffusion equations can be obtained by analytical, numer-

where Co and C are the molar concentration at time t = 0 and t = ∞, respectively.

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Y, Unaccomplished change T1 − T c1 − c (c1 / K ) − c

Note: T0 and c0 = temperature and concentration at time t = 0, respectively; T1 and c1 = temperature

1.4 MASS TRANSFER BY CONVECTION

1.4.1 FILM THEORY AND MASS TRANSFER COEFFICIENT

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Similarly, the corresponding expression for mass ﬂux is:

1.4.2 TWO-FILM THEORY AND MASS TRANSFER COEFFICIENT