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Fundamental Mass Transfer Concepts in Engineering Applications

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Fundamental Mass Transfer Concepts in Engineering
Applications
Fundamental Mass Transfer Concepts in Engineering
Applications

Authored by İsmail Tosun

CRC Press
Taylor & Francis Group
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 Dedication

To Nurten and Derviş Şamlı

Contents

Preface.............................................................................................................................................. xv

Authors...........................................................................................................................................xvii

Chapter 1 Introduction ............................................................................................................. 1

1.1 Basic Concepts................................................................................................ 1
1.2 Definitions....................................................................................................... 2
1.2.1 Steady-State ....................................................................................... 2
1.2.2 Uniform.............................................................................................. 2
1.2.3 Equilibrium ........................................................................................ 2
1.2.4 Flux .................................................................................................... 3
1.3 Molecular Flux................................................................................................ 3
1.3.1 Newton’s Law of Viscosity ................................................................3
1.3.2 Fourier’s Law of Heat Conduction.....................................................4
1.3.3 Fick’s First Law of Diffusion.............................................................5
1.3.4 Dimensionless Numbers .................................................................... 5
1.4 Convective Flux ..............................................................................................6
1.5 Total Flux........................................................................................................7
1.6 Transfer Coefficients.......................................................................................7
1.6.1 Dimensionless Numbers .................................................................... 8
Reference ................................................................................................................. 8

Chapter 2 Conservation of Chemical Species ..........................................................................9

2.1 Definitions....................................................................................................... 9
2.1.1 Concentrations ................................................................................... 9
2.1.2 Velocities..........................................................................................11
2.1.3 Mass and Molar Fluxes....................................................................13
2.1.4 Diffusive Mass/Molar Fluxes in Different Reference
Velocity Frames ...............................................................................18
2.1.5 Diffusive Flux Transformations .......................................................22
2.1.5.1 Transformation of J∗ to J ............................................... 26
2.2 The Species Continuity Equation ................................................................. 27
2.2.1 Homogeneous Reaction Rate Expression ........................................ 29
2.2.2 Heterogeneous Reaction Rate Expression ....................................... 31
2.3 The Species Continuity Equation in Terms of Fluxes ..................................31
2.3.1 Mass Basis ....................................................................................... 31
2.3.2 Molar Basis ...................................................................................... 32
2.4 Governing Equations for a Binary System ...................................................34
2.4.1 Fick’s First Law of Diffusion...........................................................35
2.4.2 Total Mass/Molar Flux Expressions ................................................37
2.4.3 Various Forms of the Species Continuity Equation .........................37
2.4.4 Fick’s Second Law of Diffusion ......................................................40
2.5 Driving Forces for Diffusion ........................................................................40
2.5.1 Thermodynamics Preliminaries ....................................................... 41

vii
viii Contents

2.5.2 Two-Bulb Diffusion Experiment......................................................42

2.5.3 Other Driving Forces of Mass Transfer ........................................... 44
2.6 Estimation of Diffusion Coefficients ............................................................ 45
2.6.1 Diffusion Coefficients for Gases...................................................... 45
2.6.1.1 Chapman–Enskog theory................................................. 46
2.6.1.2 Fuller–Schettler–Giddings correlation ............................49
2.6.2 Diffusion Coefficients for Liquids ................................................... 50
2.7 Boundary Conditions at Phase Interfaces ..................................................... 54
2.7.1 Vapor–Liquid Interface .................................................................... 54
2.7.2 Solid–Fluid Interface ....................................................................... 57
2.7.3 Liquid–Liquid Interface ................................................................... 59
2.7.4 Other Boundary Conditions ............................................................. 59
2.7.5 Jump Boundary Condition ............................................................... 60
Reference ...............................................................................................................65

Chapter 3 Foundations of Diffusion in Multicomponent Mixtures........................................ 67

3.1 Generalized Fick’s Law ................................................................................ 67
3.1.1 Diffusive Flux Expressions .............................................................. 67
3.1.2 Transformation of Fick Diffusion Coefficients................................ 72
3.1.3 Properties of Fick Diffusion Coefficient Matrices ........................... 73
3.2 MS Equations................................................................................................ 75
3.2.1 Isothermal Diffusion in the Absence of External Body Forces ....... 76
3.3 Calculation of the Thermodynamic Factor ................................................... 78
3.3.1 Thermodynamic Factor Based on the Activity Coefficient.............. 78
3.3.2 Thermodynamic Factor Based on the Fugacity Coefficient.............84
3.4 MS Equations in the form of Generalized Fick Equations ........................... 86
3.4.1 Binary Mixture................................................................................. 87
3.4.2 Ternary Mixture ............................................................................... 89
3.4.3 Quaternary Mixture..........................................................................93
3.5 Prediction of Diffusion Coefficients ............................................................. 94
3.5.1 Vignes Equation ............................................................................... 94
3.5.2 Darken Equation .............................................................................. 97
3.6 Governing Equations for Dilute Gas Mixtures ............................................. 99
3.6.1 Special Case for Nk = 0 (i  k)........................................................99
Reference .............................................................................................................107

Chapter 4 Mass Transfer in Binary Systems without Bulk Flow:

Steady-State Examples ........................................................................................ 109
4.1 Diffusion of Fluids Through Solids and/or Membraness ........................... 109
4.1.1 Diffusion in Cartesian Coordinates................................................ 109
4.1.2 Diffusion in Cylindrical Coordinates............................................. 115
4.1.3 Diffusion in Spherical Coordinates................................................ 118
4.2 Equimolar Counterdiffusion ....................................................................... 121
4.2.1 Equimolar Counterdiffusion in a Tapered Conical Duct ............... 122
4.3 Evaporation of a Liquid in a Capillary Tube .............................................. 124
4.3.1 Limiting Case for Small Values of yAo ........................................... 126
4.3.2 Velocities........................................................................................ 126
4.3.3 Total Molar Flux of Species B ....................................................... 127
4.4 Diffusion Through a Stagnant Liquid......................................................... 127
4.4.1 Analysis Based on the Molar-Average Velocity ............................ 127
Contents ix

4.4.2 Analysis Based on the Volume-Average Velocity.......................... 128

4.4.3 Velocities........................................................................................ 129
4.5 Diffusion with a Heterogeneous Reaction .................................................. 131
4.5.1 Velocities........................................................................................ 133
4.6 Diffusion and Reaction in a Cylindrical Catalyst Pore............................... 134
4.6.1 Effectiveness Factor .......................................................................138
4.7 Diffusion and Reaction In a Spherical Catalyst.......................................... 139
4.7.1 Effectiveness Factor .......................................................................140
4.8 Diffusion in a Liquid with a Homogeneous Reaction ................................ 142
4.9 Diffusion with Heterogeneous and Homogeneous Reactions .................... 150
Reference .............................................................................................................159

Chapter 5 Mass Transfer in Binary Systems without Bulk Flow:

Pseudosteady-State Examples .............................................................................161
5.1 Pseudosteady-State Approximation............................................................ 161
5.2 Mass Transfer Coefficient........................................................................... 162
5.2.1 Physical Interpretation of the Mass Transfer Coefficient ..............163
5.2.2 Other Definitions of Mass Transfer Coefficients ........................... 164
5.2.3 Two-Film Theory ...........................................................................165
5.3 Mass Transfer Correlations......................................................................... 166
5.3.1 Flow over a Flat Plate ....................................................................167
5.3.2 Flow over a Single Sphere .............................................................167
5.3.3 Flow over a Single Cylinder ..........................................................169
5.3.4 Flow in Circular Pipes ...................................................................169
5.3.5 Flow in Packed Beds...................................................................... 170
5.3.6 Solid–Liquid Suspensions in Agitated Tanks ................................ 171
5.3.7 Hollow Fiber Geometries............................................................... 172
5.4 Diaphragm Cell........................................................................................... 173
5.4.1 Validity of the Pseudosteady-State Approximation .......................174
5.5 Stefan Diffusion Problem ........................................................................... 174
5.5.1 Simplification for Small Values of yAo ........................................... 176
5.5.2 Validity of the Pseudosteady-State Approximation .......................176
5.5.3 Application of the Jump Species Continuity Equation .................. 176
5.6 Evaporation of a Liquid Droplet................................................................. 177
5.6.1 Simplification for Small Values of yeq A ........................................... 178
5.6.2 Validity of the Pseudosteady-State Approximation .......................178
5.7 Sublimation of a Naphthalene Sphere ........................................................179
5.7.1 Stagnant Air ...................................................................................179
5.7.2 Air Moves at a Certain Velocity..................................................... 179
5.8 Shrinking Particle Model ............................................................................180
5.9 Shrinking Core Model ................................................................................ 182
5.9.1 Rectangular Geometry ...................................................................182
5.9.2 Spherical Geometry ....................................................................... 184
Reference .............................................................................................................191

Chapter 6 Mass Transfer in Binary Systems without Bulk Flow:

Unsteady-State Examples.................................................................................... 193
6.1 Governing Equations .................................................................................. 193
6.2 Diffusion into a Rectangular Slab............................................................... 194
x Contents

6.2.1 Calculation of the Molar Flux – An Alternative Approach ........... 196

6.2.2 Solution for Short Times................................................................ 198
6.2.3 Diffusion into a Semi-Infinite Domain .......................................... 200
6.2.4 Solution for Long Times ................................................................ 202
6.3 Drug Release from a Spherical Matrix ....................................................... 202
6.3.1 Investigation of the Limiting Cases ...............................................205
6.4 Diffusion and Reaction in a Polymer Microsphere .................................... 206
6.5 Drug Release from a Cylindrical Matrix .................................................... 210
6.6 Diffusion into a Slab from a Limited Volume of Solution ......................... 213
6.7 Loschmidt Diffusion Cell ...........................................................................216
6.8 Diffusion from Instantaneous Sources........................................................ 219
6.8.1 Diffusion from a Plane Source....................................................... 219
6.8.2 Diffusion from a Line Source ........................................................ 222
6.8.3 Diffusion from a Point Source ....................................................... 223
Reference .............................................................................................................239

Chapter 7 Mass Transfer in Binary Systems with Bulk Flow.............................................. 241

7.1 Governing Equations .................................................................................. 241
7.2 Forced Convection Mass Transfer in a Pipe ............................................... 242
7.2.1 Asymptotic Solution for Large Values of z.................................... 246
7.2.2 Asymptotic Solution for Small Values of z.................................... 247
7.3 More on the Forced Convection Mass Transfer in a Pipe........................... 249
7.3.1 Sherwood Number for Constant Wall Concentration .................... 250
7.3.2 Sherwood Number for Constant Wall Mass Flux .......................... 252
7.4 Convective Mass Transport with a Wall Reaction in a Pipe ....................... 254
7.5 Diffusion into a Falling Liquid Film........................................................... 257
7.5.1 Expression for the Sherwood Number........................................... 258
7.5.2 Long Contact Times....................................................................... 259
7.5.3 Short Contact Times....................................................................... 260
7.6 Stefan Diffusion Problem Revisited: Unsteady-State Case ........................ 262
7.7 Stefan Tube at Supercritical Conditions ..................................................... 266
7.7.1 Limiting Case When Ω = 0 ........................................................... 270
7.8 Diffusion from Instantaneous Sources........................................................ 271
7.8.1 Diffusion from a Plane Source....................................................... 271
7.8.2 Diffusion from a Line Source ........................................................ 272
7.8.3 Diffusion from a Point Source ....................................................... 273
7.9 Convection and Diffusion in a Semi-Infinite Medium................................ 273
7.10 Development of Taylor–Aris Theory.......................................................... 275
Reference .............................................................................................................286

Chapter 8 Mass Transfer in Multicomponent Mixtures ....................................................... 289

8.1 Two-Bulb Diffusion Experiment by Duncan and Toor............................... 289
8.2 MS Equations.............................................................................................. 293
8.2.1 Steady-State Mass Transfer in Ternary Gas Mixtures ................... 294
8.2.2 Two-Bulb Diffusion Experiment Revisited:
Unsteady-State Case ...................................................................... 311
8.3 MS Equations for Coupled Driving Forces ................................................ 313
8.3.1 Diffusion Induced by a Temperature Gradient (Thermal
Diffusion) ....................................................................................... 316
8.3.2 Diffusion Induced by a Pressure Gradient (Pressure Diffusion).... 317
Contents xi

8.3.3 Diffusion Induced by an Electrostatic Potential Gradient ............. 318

Reference .............................................................................................................326

Chapter 9 Approximate Solution of the Species Continuity Equation ................................ 329

9.1 Two-Point Hermite Expansion.................................................................... 329
9.2 Drug Release from a Slab ...........................................................................330
9.2.1 Analytical Solution ........................................................................ 333
9.2.2 Approximate Solution by Area Averaging.....................................334
9.2.3 Comparison of Results................................................................... 335
9.2.4 Limiting Case for Equal Bulk Concentrations............................... 336
9.3 Diffusion into a Slab from a Limited Volume of Solution ......................... 336
9.3.1 Analytical Solution ........................................................................ 336
9.3.2 Approximate Solution by Area Averaging.....................................337
9.3.3 Comparison of Results................................................................... 339
9.4 Convective Mass Transport between two Parallel Plates with a
Wall Reaction.............................................................................................. 339
9.4.1 Analytical Solution ........................................................................ 341
9.4.2 Approximate Solution by Area Averaging.....................................343
9.4.3 Comparison of Results................................................................... 345
Reference .............................................................................................................345

Appendix A Vector and Tensor Algebra .................................................................................. 347

A.1 The Operations on Vectors..........................................................................347
A.1.1 Addition ......................................................................................... 347
A.1.2 Scalar Multiplication...................................................................... 348
A.1.3 Scalar (or Dot) Product .................................................................. 348
A.1.4 Vector (or Cross) Product...............................................................349
A.2 Basis and Basis Vectors .............................................................................. 349
A.3 Summation Convention .............................................................................. 350
A.4 Second-Order Tensors ................................................................................ 351
A.4.1 Trace of a Tensor............................................................................352
A.4.2 Invariants of a Tensor.....................................................................353
A.5 Vector and Tensor Differential Operations ................................................. 353
A.5.1 Gradient of a Scalar Field .............................................................. 353
A.5.2 Divergence of a Vector Field..........................................................353
A.5.3 Curl of a Vector Field..................................................................... 354
A.5.4 Gradient of a Vector Field.............................................................. 354
A.5.5 Laplacian of a Scalar Field ............................................................ 354
A.5.6 Some Useful Identities................................................................... 355
A.6 Vector and Tensor Algebra in Curvilinear Coordinates.............................. 355
A.6.1 Dot and Cross Product Operations................................................. 357
A.6.2 Differential Operations .................................................................. 357
A.7 Vector and Tensor Integral Theorems......................................................... 358
A.7.1 Green’s Transformation ................................................................. 358
A.7.2 The Leibniz Formula...................................................................... 358

Appendix B Order of Magnitude (Scale) Analysis.................................................................. 359

Reference .............................................................................................................361
xii Contents

Appendix C Matrices ............................................................................................................... 363

C.1 Basic Matrix Operations .............................................................................363
C.2 Determinants............................................................................................... 364
C.2.1 Some Properties of Determinants .................................................. 365
C.3 Types of Matrices........................................................................................ 365
C.3.1 Transpose of a Matrix .................................................................... 365
C.3.2 Unit Matrix..................................................................................... 366
C.3.3 Symmetric and Skew-Symmetric Matrices.................................... 366
C.3.4 Singular Matrix .............................................................................. 366
C.3.5 Trace of a Matrix............................................................................ 366
C.3.6 Inverse of a Matrix ......................................................................... 366
C.4 Eigenvalues and Eigenvectors of a Matrix.................................................. 367
C.4.1 Some Properties of Eigenvalues and Eigenvectors ........................ 368
C.5 Solution of Algebraic Equations – Cramer’s Rule ..................................... 368
C.6 Matrix Operations Using Mathcad .............................................................369
Reference .............................................................................................................370

Appendix D Ordinary Differential Equations ..........................................................................371

D.1 First-Order ODEs........................................................................................ 371
D.1.1 Separable Equation ........................................................................ 371
D.1.2 Exact Equation ............................................................................... 371
D.1.3 Homogeneous Equation ................................................................. 372
D.1.4 Bernoulli Equation .........................................................................372
D.2 Second-Order ODEs ................................................................................... 373
D.2.1 Solution of a Homogeneous Equation ........................................... 373
D.2.2 Solution of a Nonhomogenous Equation ....................................... 373
D.2.3 Bessel’s Equation ........................................................................... 374
D.3 Special Cases of Second-Order Differential Equations.............................. 375
D.3.1 Cartesian Coordinate System.........................................................375
D.3.2 Cylindrical Coordinate System ...................................................... 376
D.3.3 Spherical Coordinate System.........................................................377
Reference .............................................................................................................378

Appendix E Partial Differential Equations .............................................................................. 379

E.1 Preliminaries ............................................................................................... 379
E.1.1 Classification of Partial Differential Equations ............................. 379
E.1.2 Orthogonal Functions..................................................................... 379
E.1.3 Second-Order Self-Adjoint Differential Equations........................380
E.1.4 Sturm–Liouville Problem .............................................................. 381
E.1.5 Fourier Series ................................................................................. 382
E.2 Analytical Solution of PDEs....................................................................... 384
E.2.1 Separation of Variables .................................................................. 385
E.2.2 Similarity Solution ......................................................................... 395
E.2.3 The Laplace Transform Technique ................................................397
E.2.4 The Fourier Transform Technique .................................................407
E.3 Duhamel’s Theorem.................................................................................... 409
E.4 Solution of PDEs by Mathcad .................................................................... 410
E.4.1 Determination of Eigenvalues........................................................ 410
E.4.2 Numerical Solution of Parabolic PDEs.......................................... 411
Reference .............................................................................................................416
Contents xiii

Appendix F Critical Constants and Acentric Factors .............................................................. 417

Appendix G Physical Properties of Water................................................................................ 421

Appendix H Mathcad Subroutines ...........................................................................................423

H.1 Multicomponent – Wilson .......................................................................... 423
H.2 Multicomponent – NRTL ........................................................................... 423
H.3 Root............................................................................................................. 423
H.4 Mixture ....................................................................................................... 423

Appendix I Suggested Books for Further Reading................................................................. 427

Appendix J Constants and Conversion Factors....................................................................... 429

J.1 Physical Constants ...................................................................................... 429
J.2 Conversion Factors ..................................................................................... 429

Index .............................................................................................................................................. 431

Preface
This book is intended as a text for upper undergraduate and graduate courses on mass transfer. The
focus is to teach the foundations of mass transfer and to equip students with sufficient mathemat-
ical skills to tackle problems with confidence. An overview of the book is shown schematically
in Figure P.1. The presented material is for a one-semester course, and it provides sufficient back-
ground for students interested in pursuing further research on the topics not covered in this book.
Since mathematics is an integral part of mass transfer, readers should go over Appendices A, C,
D, and E before they start reading Chapter 1. Students usually struggle with the elimination of terms
in the governing equations because they do not know the order of magnitude values or the physical
significance of these terms. The purpose of Appendix B is to introduce the order of magnitude
(or scale) analysis to students in order to enable them to make reasonable estimations.
Chapter 1 covers the basic concepts and their characteristics. The terms appearing in the conser-
vation equations for mass, momentum, and energy are discussed qualitatively, and the similarities
between mass, momentum, and energy transport are pointed out. Chapter 2 provides the foundations
for the formulation of mass transfer problems. Those who do not want to cover multicomponent
mass transfer may skip Chapter 3. Mass transfer in binary systems without bulk flow is covered in
Chapters 4–6. Steady-state, pseudosteady-state, and unsteady-state examples are given in Chapters
4, 5, and 6, respectively. Chapter 7 deals with the mass transfer in binary systems in the case of
bulk flow. Chapter 9 is optional; it shows how the area averaging technique together with two-point
Hermite expansion is used to obtain an approximate solution.

Chapter 1
Introduction

Chapter 2
Conservation of Chemical Species

Binary Systems Multicomponent Systems

Without Bulk Flow With Bulk Flow

Chapter 4 Chapter 3
Steady-State Examples Foundations of Diffusion in
Multicomponent Mixtures
Chapter 7
Chapter 5 Convective Mass
Pseudosteady-State Examples Transfer
Chapter 8
Chapter 6 Mass Transfer in
Unsteady-State Examples Multicomponent Mixtures

Chapter 9
Approximate Solution of the
Species Continuity Equation

Figure P.1 Arrangement of the chapters.

xv
xvi Preface

Nowadays engineering calculations are carried out by mathematical software packages, such as
Mathcad, Matlab, and Polymath. It is extremely important for engineering students to learn and
practice the use of these modern computational tools. Mathcad worksheets provided in the book
show the steps to be followed in the calculations.
Chapters 3 and 8 talk about mass transfer in multicomponent mixtures. Maxwell–Stefan mul-
ticomponent mass transfer calculations are lengthy and time-consuming. Students usually become
bogged down in the details of the calculations and lose the big picture. The Mathcad subroutine
given in Chapter 8 for the “shooting method” carries out the complex calculations in a straightfor-
ward manner and enables students to conduct a parametric study.
Not only are answers to all the problems in the book provided, but also step-by-step solution
procedures are given in most problem statements, facilitating its use as a self-study reference book.
My colleagues Harun Koku, Canan Özgen, Turgut Tokdemir, and Hayrettin Yücel made many
helpful suggestions during the preparation of the book. Their efforts are greatly appreciated. Above
all, I am grateful to my wife, Ayşe, for her unwavering support and understanding ever since we got
married.
Suggestions and criticisms from instructors and students using this book would be appreciated.

İsmail Tosun
(itosun@metu.edu.tr)
Ankara, Turkey
January 2019
 Author
Professor İsmail Tosun received his BS and MS degrees from the Middle East Technical University
(METU) in 1972 and 1974, respectively, and a PhD degree from the University of Akron, Ohio in
1977, all in Chemical Engineering.
After spending a year as a post-doctoral fellow at the University of Akron and completing his
military service in Ankara, he started his academic career as an assistant professor at the METU
Chemical Engineering Department in 1981. He was promoted to Associate Professorship in 1984
and to full Professorship in 1989. As a Fulbright Scholar and a Visiting Professor, Prof. Tosun was
in the United States from 1987 to 1989.
From 1990 to 1993, Prof. Tosun was the Assistant-Dean of the Graduate School at METU. Then
he acted as the Dean of Graduate School until 1997. In January of 1997, Prof. Tosun was appointed
to the Council of Higher Education (YOK), which, in a way, acts as the National Board of Trustees.
After completing his term of 4 years as the Vice-President, he returned to his academic career at
METU in January of 2001.
His research and teaching interests are mathematical modeling, solid–liquid separation processes,
transport phenomena, and thermodynamics. He is the author or co-author of over 60 publications.
Prof. Tosun is also the author of the following books:

1. Modeling in Transport Phenomena – A Conceptual Approach, 2nd Ed., Elsevier, 2007.

2. The Thermodynamics of Phase and Reaction Equilibria, Elsevier, 2012.
3. Thermodynamics – Principles and Applications, World Scientific, 2015.

xvii

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