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Electrochemical Systems

eBook - The ECS Series of Texts and Monographs

Erschienen am 11.02.2021, Auflage: 4/2021
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Bibliografische Daten
ISBN/EAN: 9781119514626
Sprache: Englisch
Umfang: 608 S., 20.07 MB
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Format: PDF
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Beschreibung

Provides a comprehensive understanding of a wide range of systems and topics in electrochemistry

This book offers complete coverage of electrochemical theories as they pertain to the understanding of electrochemical systems. It describes the foundations of thermodynamics, chemical kinetics, and transport phenomenaincluding the electrical potential and charged species. It also shows how to apply electrochemical principles to systems analysis and mathematical modeling. Using these tools, the reader will be able to model mathematically any system of interest and realize quantitative descriptions of the processes involved.

This brand new edition ofElectrochemical Systemsupdates all chapters while adding content on lithium battery electrolyte characterization and polymer electrolytes. It also includes a new chapter on impedance spectroscopy. Presented in 4 sections, the book covers: Thermodynamics of Electrochemical Cells, Electrode Kinetics and Other Interfacial Phenomena, Transport Processes in Electrolytic Solutions, and Current Distribution and Mass Transfer in Electrochemical Systems. It also features three appendixes containing information on: Partial Molar Volumes, Vectors and Tensors, and Numerical Solution of Coupled, Ordinary Differential Equations.

Details fundamental knowledge with a thorough methodologyThoroughly updated throughout with new material on topics including lithium battery electrolyte characterization, impedance analysis, and polymer electrolytesIncludes a discussion of equilibration of a charged polymer material and an electrolytic solution (the Donnan equilibrium)A peerless classic on electrochemical engineering

Electrochemical Systems, Fourth Edition is an excellent resource for students, scientists, and researchers involved in electrochemical engineering.

Autorenportrait

John Newman, PhD, has been a Professor of Chemical Engineering at the University of California, Berkeley, since 1963, is a member of the National Academy of Engineering, and the recipient of several awards from The Electrochemical Society.

Nitash P. Balsara, PhD, holds the Charles W. Tobias Chair in Electrochemistry at the Department of Chemical and Biomolecular Engineering, University of California, Berkeley, where he has been a professor since 2000.

Inhalt

Preface To The Fourth Edition xv

Preface To The Third Edition xvii

Preface To The Second Edition xix

Preface To The First Edition xxi

1 Introduction 1

1.1 Definitions 2

1.2 Thermodynamics and Potential 3

1.3 Kinetics and Rates of Reaction 6

1.4 Transport 8

1.5 Concentration Overpotential and the Diffusion Potential 15

1.6 Overall Cell Potential 18

Problems 20

Notation 21

Part A Thermodynamics of Electrochemical Cells 23

2 Thermodynamics In Terms of Electrochemical Potentials 25

2.1 Phase Equilibrium 25

2.2 Chemical Potential and Electrochemical Potential 27

2.3 Definition of Some Thermodynamic Functions 30

2.4 Cell with Solution of Uniform Concentration 36

2.5 Transport Processes in Junction Regions 39

2.6 Cell with a Single Electrolyte of Varying Concentration 40

2.7 Cell with Two Electrolytes, One of Nearly Uniform Concentration 44

2.8 Cell with Two Electrolytes, Both of Varying Concentration 47

2.9 LithiumLithium Cell With Two Polymer Electrolytes 49

2.10 Standard Cell Potential and Activity Coefficients 50

2.11 Pressure Dependence of Activity Coefficients 58

2.12 Temperature Dependence of Cell Potentials 59

Problems 61

Notation 68

References 70

3 The Electric Potential 71

3.1 The Electrostatic Potential 71

3.2 Intermolecular Forces 74

3.3 Outer and Inner Potentials 76

3.4 Potentials of Reference Electrodes 77

3.5 The Electric Potential in Thermodynamics 78

Notation 79

References 80

4 Activity Coefficients 81

4.1 Ionic Distributions in Dilute Solutions 81

4.2 Electrical Contribution to the Free Energy 84

4.3 Shortcomings of the DebyeHückel Model 87

4.4 Binary Solutions 89

4.5 Multicomponent Solutions 92

4.6 Measurement of Activity Coefficients 94

4.7 Weak Electrolytes 96

Problems 99

Notation 103

References 104

5 Reference Electrodes 107

5.1 Criteria for Reference Electrodes 107

5.2 Experimental Factors Affecting Selection of Reference Electrodes 109

5.3 The Hydrogen Electrode 110

5.4 The Calomel Electrode and Other MercuryMercurous Salt Electrodes 112

5.5 The MercuryMercuric Oxide Electrode 114

5.6 SilverSilver Halide Electrodes 114

5.7 Potentials Relative to a Given Reference Electrode 116

Notation 119

References 120

6 Potentials of Cells With Junctions 121

6.1 Nernst Equation 121

6.2 Types of Liquid Junctions 122

6.3 Formulas for Liquid-Junction Potentials 123

6.4 Determination of Concentration Profiles 124

6.5 Numerical Results 124

6.6 Cells with Liquid Junction 128

6.7 Error in the Nernst Equation 129

6.8 Potentials Across Membranes 131

6.9 Charged Membranes Immersed in an Electrolytic Solution 131

Problems 135

Notation 138

References 138

Part B Electrode Kinetics and Other Interfacial Phenomena 141

7 Structure of The Electric Double Layer 143

7.1 Qualitative Description of Double Layers 143

7.2 Gibbs Adsorption Isotherm 148

7.3 The Lippmann Equation 151

7.4 The Diffuse Part of the Double Layer 155

7.5 Capacity of the Double Layer in the Absence of Specific Adsorption 160

7.6 Specific Adsorption at an ElectrodeSolution Interface 161

Problems 161

Notation 164

References 165

8 Electrode Kinetics 167

8.1 Heterogeneous Electrode Reactions 167

8.2 Dependence of Current Density on Surface Overpotential 169

8.3 Models for Electrode Kinetics 170

8.4 Effect of Double-Layer Structure 185

8.5 The Oxygen Electrode 187

8.6 Methods of Measurement 192

8.7 Simultaneous Reactions 193

Problems 195

Notation 199

References 200

9 Electrokinetic Phenomena 203

9.1 Discontinuous Velocity at an Interface 203

9.2 Electro-Osmosis and the Streaming Potential 205

9.3 Electrophoresis 213

9.4 Sedimentation Potential 215

Problems 216

Notation 218

References 219

10 Electrocapillary Phenomena 221

10.1 Dynamics of Interfaces 221

10.2 Electrocapillary Motion of Mercury Drops 222

10.3 Sedimentation Potentials for Falling Mercury Drops 224

Notation 224

References 225

Part C Transport Processes In Electrolytic Solutions 227

11 Infinitely Dilute Solutions 229

11.1 Transport Laws 229

11.2 Conductivity, Diffusion Potentials, and Transference Numbers 232

11.3 Conservation of Charge 233

11.4 The Binary Electrolyte 233

11.5 Supporting Electrolyte 236

11.6 Multicomponent Diffusion by Elimination of the Electric Field 237

11.7 Mobilities and Diffusion Coefficients 238

11.8 Electroneutrality and LaplaceS Equation 240

11.9 Moderately Dilute Solutions 242

Problems 244

Notation 247

References 247

12 Concentrated Solutions 249

12.1 Transport Laws 249

12.2 The Binary Electrolyte 251

12.3 Reference Velocities 252

12.4 The Potential 253

12.5 Connection with Dilute-Solution Theory 256

12.6 Example Calculation Using Concentrated Solution Theory 257

12.7 Multicomponent Transport 259

12.8 Liquid-Junction Potentials 262

Problems 263

Notation 264

References 266

13 Thermal Effects 267

13.1 Thermal Diffusion 268

13.2 Heat Generation, Conservation, and Transfer 270

13.3 Heat Generation at an Interface 272

13.4 Thermogalvanic Cells 274

13.5 Concluding Statements 276

Problems 277

Notation 279

References 280

14 Transport Properties 283

14.1 Infinitely Dilute Solutions 283

14.2 Solutions of a Single Salt 283

14.3 Mixtures of Polymers and Salts 286

14.4 Types of Transport Properties and Their Number 295

14.5 Integral Diffusion Coefficients for Mass Transfer 296

Problem 298

Notation 298

References 299

15 Fluid Mechanics 301

15.1 Mass and Momentum Balances 301

15.2 Stress in a Newtonian Fluid 302

15.3 Boundary Conditions 303

15.4 Fluid Flow to a Rotating Disk 304

15.5 Magnitude of Electrical Forces 307

15.6 Turbulent Flow 310

15.7 Mass Transfer in Turbulent Flow 314

15.8 Dissipation Theorem for Turbulent Pipe Flow 316

Problem 318

Notation 319

References 321

Part D Current Distribution and Mass Transfer In Electrochemical Systems 323

16 Fundamental Equations 327

16.1 Transport in Dilute Solutions 327

16.2 Electrode Kinetics 328

Notation 329

17 Convective-Transport Problems 331

17.1 Simplifications for Convective Transport 331

17.2 The Rotating Disk 332

17.3 The Graetz Problem 335

17.4 The Annulus 340

17.5 Two-Dimensional Diffusion Layers in Laminar Forced Convection 344

17.6 Axisymmetric Diffusion Layers in Laminar Forced Convection 345

17.7 A Flat Plate in a Free Stream 346

17.8 Rotating Cylinders 347

17.9 Growing Mercury Drops 349

17.10 Free Convection 349

17.11 Combined Free and Forced Convection 351

17.12 Limitations of Surface Reactions 352

17.13 Binary and Concentrated Solutions 353

Problems 354

Notation 359

References 360

18 Applications of Potential Theory 365

18.1 Simplifications For Potential-Theory Problems 366

18.2 Primary Current Distribution 367

18.3 Secondary Current Distribution 370

18.4 Numerical Solution by Finite Differences 374

18.5 Principles of Cathodic Protection 375

Problems 389

Notation 396

References 397

19 Effect of Migration On Limiting Currents 399

19.1 Analysis 400

19.2 Correction Factor for Limiting Currents 402

19.3 Concentration Variation of Supporting Electrolyte 404

19.4 Role of Bisulfate Ions 409

19.5 Paradoxes with Supporting Electrolyte 413

19.6 Limiting Currents for Free Convection 417

Problems 423

Notation 424

References 426

20 Concentration Overpotential 427

20.1 Definition 427

20.2 Binary Electrolyte 429

20.3 Supporting Electrolyte 430

20.4 Calculated Values 430

Problems 431

Notation 432

References 433

21 Currents Below The Limiting Current 435

21.1 The Bulk Medium 436

21.2 The Diffusion Layers 437

21.3 Boundary Conditions and Method of Solution 438

21.4 Results for the Rotating Disk 440

Problems 444

Notation 446

References 447

22 Porous Electrodes 449

22.1 Macroscopic Description of Porous Electrodes 450

22.2 Nonuniform Reaction Rates 457

22.3 Mass Transfer 462

22.4 Battery Simulation 463

22.5 Double-Layer Charging and Adsorption 477

22.6 Flow-Through Electrochemical Reactors 478

Problems 482

Notation 484

References 486

23 Semiconductor Electrodes 489

23.1 Nature of Semiconductors 490

23.2 Electric Capacitance at the SemiconductorSolution Interface 499

23.3 Liquid-Junction Solar Cell 502

23.4 Generalized Interfacial Kinetics 506

23.5 Additional Aspects 509

Problems 513

Notation 514

References 516

24 Impedance 517

24.1 Frequency Dispersion at a Disk Electrode 519

24.2 Modulated Flow With a Disk Electrode 522

24.3 Porous Electrodes for Batteries 526

24.4 KramersKronig Relation 528

Problems 530

Notation 531

References 532

Appendix A Partial Molar Volumes 535

Appendix B Vectors and Tensors 537

Appendix C Numerical Solution of Coupled, Ordinary Differential Equations 543

Index 567

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