Fluid Solid Reaction Engineering Preface xi Nomenclature xii Chapter 1 The Basics of Reaction Kinetics for Chemical Reaction Engineering 1 1.1 The Scope of Chemical Reaction Engineering I 1.2 The Extent of Reaction 8 1.3 The Rate of Reaction 16 1.4 General Properties of the Rate Function for a Single Reaction 19 1.5 Examples of Reaction Rates 24 Chapter 2 Rate Constants of Elementary Reactions 53 2.1 Elementary Reactions 53 2.2 Arrhenius Temperature Dependence of the Rate Constant 54 2.3 Transition-State Theory 56 Chapter 3 Reactors for Measuring Reaction Rates 64 3.1 Ideal Reactors 64 3.2 Batch and Semibatch Reactors 65 3.3 Stirred-Flow Reactors 70 3.4 Ideal Tubular Reactors 76 3.5 Measurement of Reaction Rates 82 3.5.1 Batch Reactors 84 3.5.2 Flow Reactors 87 Chapter 4 The Steady-State Approximation: Catalysis 100 4.1 Single Reactions 100 4.2 The Steady-State Approximation 105 4.3 Relaxation Methods 124 Chapter 5 Heterogeneous Catalysis 133 5.1 Introduction 133 5.2 Kinetics of Elementary Steps: Adsorption, Desorption, and Surface Reaction 140 5.3 Kinetics of Overall Reactions 157 5.4 Evaluation of Kinetic Parameters 171 Chapter 6 Effects of Transport Limitations on Rates of Solid-Catalyzed Reactions 184 6.1 Introduction 184 6.2 External Transport Effects 185 6.3 Internal Transport Effects 190 6.4 Combined Internal and External Transport Effects 218 6.5 Analysis of Rate Data 228 Chapter 7 Microkinetic Analysis of Catalytic Reactions 240 7.1 Introduction 240 7.2 Asymmetric Hydrogenation of Prochiral Olefins 240 ix x Contents 7.3 Ammonia Synthesis on Transition Metal Catalysts 246 7.4 Ethylene Hydrogenation on Transition Metals 252 7.5 Concluding Remarks 257 Chapter 8 Nonideal Flow in Reactors 260 8.1 Introduction 260 8.2 Residence Time Distribution (RTD) 262 8.3 Application of RTD Functions to the Prediction of Reactor Conversion 269 804 Dispersion Models for Nonideal Reactors 272 8.5 Prediction of Conversion with an AxiallyDispersed PFR 277 8.6 Radial Dispersion 282 8.7 Dispersion Models for Nonideal Flow in Reactors 282 Chapter 9 Nonisothermal Reactors 286 9.1 The Nature of the Problem 286 9.2 Energy Balances 286 9.3 Nonisothermal Batch Reactor 288 9.4 Nonisothermal Plug Flow Reactor 297 9.5 Temperature Effects in a CSTR 303 9.6 Stability and Sensitivity of Reactors Accomplishing Exothermic Reactions 305 Chapter 10 Reactors Accomplishing Heterogeneous Reactions 315 10.1 Homogeneous Versus Heterogeneous Reactions in Tubular Reactors 315 10.2 One-Dimensional Models for Fixed-Bed Reactors 317 10.3 Two-Dimensional Models for Fixed-Bed Reactors 325 lOA Reactor Configurations 328 10.5 Fluidized Beds with Recirculating Solids 331 Appendix A Review of Chemical Equilibria 339 A.1 Basic Criteria for Chemical Equilibrium of Reacting Systems 339 A.2 Determination of Equilibrium Compositions 341 Appendix B Regression Analysis 343 B.1 Method of Least Squares 343 B.2 Linear Correlation Coefficient 344 B.3 Correlation Probability with a Zero Y-Intercept 345 BA Nonlinear Regression 347 Appendix C Transport in Porous Media 349 C.1 Derivation of Flux Relationships in One-Dimension 349 C.2 Flux Relationships in Porous Media 351 Index 355
Preface xi
Nomenclature xii
Chapter 1
The Basics of Reaction Kinetics
for Chemical Reaction
Engineering 1
1.1 The Scope of Chemical Reaction
Engineering I
1.2 The Extent of Reaction 8
1.3 The Rate of Reaction 16
1.4 General Properties of the Rate Function for a
Single Reaction 19
1.5 Examples of Reaction Rates 24
Chapter 2
Rate Constants of Elementary
Reactions 53
2.1 Elementary Reactions 53
2.2 Arrhenius Temperature Dependence of the
Rate Constant 54
2.3 Transition-State Theory 56
Chapter 3
Reactors for Measuring Reaction
Rates 64
3.1 Ideal Reactors 64
3.2 Batch and Semibatch Reactors 65
3.3 Stirred-Flow Reactors 70
3.4 Ideal Tubular Reactors 76
3.5 Measurement of Reaction Rates 82
3.5.1 Batch Reactors 84
3.5.2 Flow Reactors 87
Chapter 4
The Steady-State Approximation:
Catalysis 100
4.1 Single Reactions 100
4.2 The Steady-State Approximation 105
4.3 Relaxation Methods 124
Chapter 5
Heterogeneous Catalysis 133
5.1 Introduction 133
5.2 Kinetics of Elementary Steps: Adsorption,
Desorption, and Surface Reaction 140
5.3 Kinetics of Overall Reactions 157
5.4 Evaluation of Kinetic Parameters 171
Chapter 6
Effects of Transport Limitations
on Rates of Solid-Catalyzed
Reactions 184
6.1 Introduction 184
6.2 External Transport Effects 185
6.3 Internal Transport Effects 190
6.4 Combined Internal and External Transport
Effects 218
6.5 Analysis of Rate Data 228
Chapter 7
Microkinetic Analysis of Catalytic
Reactions 240
7.1 Introduction 240
7.2 Asymmetric Hydrogenation of Prochiral
Olefins 240
ix
x Contents
7.3 Ammonia Synthesis on Transition Metal
Catalysts 246
7.4 Ethylene Hydrogenation on Transition
Metals 252
7.5 Concluding Remarks 257
Chapter 8
Nonideal Flow in Reactors 260
8.1 Introduction 260
8.2 Residence Time Distribution (RTD) 262
8.3 Application of RTD Functions to the
Prediction of Reactor Conversion 269
804 Dispersion Models for Nonideal
Reactors 272
8.5 Prediction of Conversion with an AxiallyDispersed
PFR 277
8.6 Radial Dispersion 282
8.7 Dispersion Models for Nonideal Flow
in Reactors 282
Chapter 9
Nonisothermal Reactors 286
9.1 The Nature of the Problem 286
9.2 Energy Balances 286
9.3 Nonisothermal Batch Reactor 288
9.4 Nonisothermal Plug Flow Reactor 297
9.5 Temperature Effects in a CSTR 303
9.6 Stability and Sensitivity of Reactors
Accomplishing Exothermic Reactions 305
Chapter 10
Reactors Accomplishing
Heterogeneous Reactions 315
10.1 Homogeneous Versus Heterogeneous
Reactions in Tubular Reactors 315
10.2 One-Dimensional Models for Fixed-Bed
Reactors 317
10.3 Two-Dimensional Models for Fixed-Bed
Reactors 325
lOA Reactor Configurations 328
10.5 Fluidized Beds with Recirculating Solids 331
Appendix A
Review of Chemical Equilibria 339
A.1 Basic Criteria for Chemical Equilibrium of
Reacting Systems 339
A.2 Determination of Equilibrium
Compositions 341
Appendix B
Regression Analysis 343
B.1 Method of Least Squares 343
B.2 Linear Correlation Coefficient 344
B.3 Correlation Probability with a Zero
Y-Intercept 345
BA Nonlinear Regression 347
Appendix C
Transport in Porous Media 349
C.1 Derivation of Flux Relationships in
One-Dimension 349
C.2 Flux Relationships in Porous Media 351
Index 355
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