ELECTROCHEMICAL SYSTEMS
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1 ELECTROCHEMICAL SYSTEMS Third Edition JOHN NEWMAN and KAREN E. THOMAS-ALYEA University of California, Berkeley ELECTROCHEMICAL SOCIETY SERIES WILEY- INTERSCIENCE A JOHN WILEY & SONS, INC PUBLICATION
2 PREFACE TO THE THIRD EDITION xv PREFACE TO THE SECOND EDITION xvii PREFACE TO THE FIRST EDITION xix 1 INTRODUCTION Definitions / Thermodynamics and Potential / Kinetics and Rates of Reaction / Transport / Concentration Oveipotential and the Diffusion Potential / Overall Cell Potential / 21 Problems / 25 Notation / 25 v
3 Vi CONTENTS PART A THERMODYNAMICS OF ELECTROCHEMICAL CELLS 27 2 THERMODYNAMICS IN TERMS OF ELECTROCHEMICAL POTENTIALS Phase Equilibrium / Chemical Potential and Electrochemical Potential / Definition of Some Thermodynamic Functions / Cell with Solution of Uniform Concentration / Transport Processes in Junction Regions / Cell with a Single Electrolyte of Varying Concentration / Cell with Two Electrolytes, One of Nearly Uniform Concentration / Cell with Two Electrolytes, Both of Varying Concentration / Standard Cell Potential and Activity Coefficients / Pressure Dependence of Activity Coefficients / Temperature Dependence of Cell Potentials / 70 Problems / 72 Notation / 82 References / 83 3 THE ELECTRIC POTENTIAL The Electrostatic Potential / Intermolecular Forces / Outer and Inner Potentials / Potentials of Reference Electrodes / The Electric Potential in Thermodynamics / 94 Notation / 96 References / 97 4 ACTIVITY COEFFICIENTS Ionic Distributions in Dilute Solutions / Electrical Contribution to the Free Energy / Shortcomings of the Debye-ffiickel Model / Binary Solutions / Multicomponent Solutions / Measurement of Activity Coefficients / 116
4 VII 4.7 Weak Electrolytes /119 Problems / 122 Notation / 127 References / REFERENCE ELECTRODES Criteria for Reference Electrodes / Experimental Factors Affecting The Selection of Reference Electrodes / The Hydrogen Electrode / The Calomel Electrode and Other Mercury-Mercurous Salt Electrodes / The Mercury-Mercuric Oxide Electrode / Silver-Silver Halide Electrodes / Potentials Relative to a Given Reference Electrode / 142 Notation / 147 References / POTENTIALS OF CELLS WITH JUNCTIONS Nernst Equation / Types of Liquid Junctions / Formulas for Liquid-Junction Potentials / Determination of Concentration Profiles / Numerical Results / Cells with Liquid Junction / Error in the Nernst Equation / Potentials Across Membranes / 162 Problems / 163 Notation / 167 References / 167 PART В ELECTRODE KINETICS AND OTHER INTERFACIAL PHENOMENA STRUCTURE OF THE ELECTRIC DOUBLE LAYER Qualitative Description of Double Layers / Gibbs Adsorption Isotherm / 177
5 7.3 The Lippmann Equation / The Diffuse Part of the Double Layer / Capacity of the Double Layer in the Absence of Specific Adsorption / Specific Adsorption at an Electrode-Solution Interface / 195 Problems / 195 Notation / 199 References / 200 ELECTRODE KINETICS Heterogeneous Electrode Reactions / Dependence of Current Density on Surface Overpotential / Models for Electrode Kinetics / Effect of Double-Layer Structure / The Oxygen Electrode / Methods of Measurement / Simultaneous Reactions / 230 Problems / 233 Notation / 236 References / 237 ELECTROKINETIC PHENOMENA Discontinuous Velocity at an Interface / Electro-Osmosis and the Streaming Potential / Electrophoresis / Sedimentation Potential / 256 Problems / 257 Notation / 260 References / 261 ELECTROCAPILLARY PHENOMENA Dynamics of Interfaces / Electrocapillary Motion of Mercury Drops / Sedimentation Potentials for Falling Mercury Drops / 266 Notation / 267 References / 268
6 ix PART С TRANSPORT PROCESSES IN ELECTROLYTIC SOLUTIONS INFINITELY DILUTE SOLUTIONS Transport Laws / Conductivity, Diffusion Potentials, and Transference Numbers / Conservation of Charge / The Binary Electrolyte / Supporting Electrolyte / Multicomponent Diffusion by Elimination of the Electric Field / Mobilities and Diffusion Coefficients / Electroneutrality and Laplace's Equation / Moderately Dilute Solutions / 289 Problems / 291 Notation / 294 References / CONCENTRATED SOLUTIONS Transport Laws / The Binary Electrolyte / Reference Velocities / The Potential / Connection with Dilute-Solution Theory / Multicomponent Transport / Liquid-Junction Potentials /310 Problems /311 Notation /313 References / THERMAL EFFECTS Thermal Diffusion / Heat Generation, Conservation, and Transfer / Heat Generation at an Interface / Thermogalvanic Cells / 326 Problems / 330
7 X CONTENTS Notation / 332 References / TRANSPORT PROPERTIES Infinitely Dilute Solutions / Solutions of a Single Salt / Multicomponent Solutions / Integral Diffusion Coefficients for Mass Transfer / 340 Problem / 343 Notation / 343 References / FLUID MECHANICS Mass and Momentum Balances / Stress in a Newtonian Fluid / Boundary Conditions / Fluid Flow to a Rotating Disk / Magnitude of Electrical Forces / Turbulent Flow / Mass Transfer in Turbulent Flow / 363 Problem / 366 Notation / 366 References / 368 PART D CURRENT DISTRIBUTION AND MASS TRANSFER IN ELECTROCHEMICAL SYSTEMS FUNDAMENTAL EQUATIONS Transport in Dilute Solutions / Electrode Kinetics / 374 Notation / CONVECTIVE-TRANSPORT PROBLEMS Simplifications for Convective Transport / The Rotating Disk / The Graetz Problem / 382
8 Xi 17.4 The Annulus / Two-Dimensional Diffusion Layers in Laminar Forced Convection / Axisymmetric Diffusion Layers in Laminar Forced Convection / A Flat Plate in a Free Stream / Rotating Cylinders / Growing Mercury Drops / Free Convection / Combined Free and Forced Convection / Limitations of Surface Reactions / Binary and Concentrated Solutions / 404 Problems / 406 Notation /413 References / APPLICATIONS OF POTENTIAL THEORY Simplifications for Potential-Theory Problems / Primary Current Distribution / Secondary Current Distribution / Numerical Solution by Finite Differences / Principles of Cathodic Protection / 430 Problems / 449 Notation / 456 References / EFFECT OF MIGRATION ON LIMITING CURRENTS Analysis / Correction Factor for Limiting Currents / Concentration Variation of Supporting Electrolyte / Role of Bisulfate Ions / Paradoxes with Supporting Electrolyte / Limiting Currents for Free Convection / 480 Problems / 486 Notation / 488 References / 489
9 XII CONTENTS 20 CONCENTRATION OVERPOTENTIAL Definition / Binary Electrolyte / Supporting Electrolyte / Calculated Values / 495 Problems / 496 Notation / 497 References / CURRENTS BELOW THE LIMITING CURRENT The Bulk Medium / The Diffusion Layers / Boundary Conditions and Method of Solution / Results for the Rotating Disk / 506 Problems /510 Notation /512 References / POROUS ELECTRODES Macroscopic Description of Porous Electrodes / Nonuniform Reaction Rates / Mass Transfer / Battery Simulation / Double-Layer Charging and Adsorption / Flow-Through Electrochemical Reactors / 553 Problems 558 Notation 561 References SEMICONDUCTOR ELECTRODES Nature of Semiconductors / Electric Capacitance at the Semiconductor-Solution Interface / Liquid-Junction Solar Cell / Generalized Interfacial Kinetics / Additional Aspects / 592
10 XÜi Problems / 596 Notation / 599 References / 600 APPENDIX A PARTIAL MOLAR VOLUMES 603 APPENDIX В VECTORS AND TENSORS 605 APPENDIX С NUMERICAL SOLUTION OF COUPLED, ORDINARY DIFFERENTIAL EQUATIONS 611 INDEX 635
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