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Modern Aspects of Electrochemistry 41

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Volume 41 of the prominent series Modern Aspects of Electrochemistry covers a range of topics in Electrochemistry and Electrochemical Engineering. The topics include the second chapter on the survey of experimental techniques and devices of solid state electrochemistry begun by Professor Joachim Maier in Volume 39. Chapter two contains a review of synthesis and characterization of nanoporous carbons and their electrochemical applications. The next chapter reviews and discusses the use of graphs in the study of chemical reaction network. The book also reviews and discusses mathematical models of three dimensional electrode structures.

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Contents
Chapter 1 SOLID STATE ELECTROCHEMISTRY II: DEVICES AND TECHNIQUES Joachim Maier  I. Introduction ........................................................................... 1 II. Electrochemical Devices and Applications .......................... 6  1. Electrochemical (Composition) Sensors ........................ 7  (i10) Bulk Conductivity Sensor (Mode 1).......................  (ii) Surface Conductivity Sensors (Mode 2)................. 11  (iii14) Galvanic Sensors (Mode 3) ....................................  (iv) Extension 18to Acid–Base Active Gases ...................  2. Electrochemical (Composition) Actors .......................... 23  3. Electrochemical Energy Storage and Conversion Devices ................................................. 29  (i) Fuel Cells ................................................................ 30  (ii.................................................................. 58) Batteries  (iiiStorage Devices:) Other Supercapacitors and Photobatteries ........................ 68 III. Electrochemical Techniques ................................................. 74  1. Determination of Bulk Parameters ................................. 76  2. Determination of Boundary Parameters ......................... 77  3. Electrochemical Polarization—The Effect of Selectively Blocking Electrodes ................................ 81  (i) Heuristic Considerations......................................... 81  (iiSteady-State Response: The Evaluation) The  of Partial Conductivities ......................................... 88  (iiiInstationary Behavior: The Evaluation) The of the Chemical Diffusion Coefficient ................... 94  4. Chemically Imposed Gradients ...................................... 97  (iPolarization and Concentration) Chemical Cell Experiment ...................................................... 97  (ii) Oxygen Permeation................................................. 100  (iii) Zero-Driving 100Force Method ...................................  (iv) Chemical Relaxation............................................... 101
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 5. Coulometric Titration ..................................................... 104  6. Thermodynamic Data from Electrochemical Cells Involving Solid Electrolytes ........................................... 106  7. Modifications in the Evaluation of Electrochemical Measurements Due to Internal Defect Reactions ........... 109  8. Dynamic Interactions...................................................... 112  9. Transport in Inhomogeneous, Heterogeneous,  and Composite Systems ................................................. 114  10. Related Techniques......................................................... 120 IV. Conclusions........................................................................... 120  Acknowledgment .................................................................. 121  A Appendix 1—Terminal Potential Difference ................. 121  B Appendix 2—Electrochemical Polarization ................... 122  C Appendix 3—Chemical Polarization and Relaxation .... 124  D Appendix 4—Electrolytic Domain Boundaries ............. 125  E Appendix 5—Coulometric Titration .............................. 126  F Appendix 6—Point Electrode Resistance ...................... 127  Symbols ................................................................................ 127  References ............................................................................ 128
Chapter 2 SYNTHESIS AND CHARACTERIZATION OF NANOPOROUS CARBON AND ITS ELECTROCHEMICAL APPLICATION TO ELECTRODE MATERIAL FOR SUPERCAPACITORS Gyoung-Ja Lee and Su-Il Pyun  I. Introduction........................................................................... 139 II. Preparation of Porous Carbons ............................................. 141  1. Activation Method .......................................................... 141  2. Templating Method ........................................................ 143 III. Structural Characteristics of Porous Carbons ....................... 145  1. Types of Adsorption Isotherms and Hysteresis Loops...................................................... 145  2. Determinations of Surface Area and Pore Size Distribution .............................................. 150 IV. Fractal Characteristics of Porous Carbons............................ 154  1. Molecular Probe Method Using Gas Adsorption ........... 155  2. Image Analysis Method.................................................. 162
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V. Electrochemical Characteristics of Carbon-Based Porous Electrodes For Supercapacitor: The Uses of AC-Impedance Spectroscopy, Current Transient and Cyclic Voltammetry.............................................................. 166  1. General Theory of Electrochemical Behavior of Porous Electrodes ....................................................... 166  2. Effect of Geometric Heterogeneity on Ion Penetration into the Pores during Double-Layer Charging/Discharging..................................................... 169  3. Effect of Surface Inhomogeneity on Ion Penetration into the Pores during Double-Layer Charging/Discharging..................................................... 175 VI. Concluding Remark .............................................................. 183  Acknowledgements .............................................................. 185 Notation ................................................................................ 186  References ............................................................................ 190
Chapter 3 THE USE OF GRAPHS IN THE STUDY OF ELECTROCHEMICAL REACTION NETWORKS Joseph D. Fehribach  I. Introduction........................................................................... 197 II. Reaction Species Graphs ...................................................... 200  1. Kinetic Graphs ................................................................ 201  2. Bipartite Graphs.............................................................. 203 III. Reaction Mechanism Graphs ................................................ 205  1. MCFC Cathodic Reactions ............................................. 206  (i) Peroxide Mechanism .............................................. 206  (iiMechanism........................... 208) Superoxide-Peroxide  2. HER Reactions ............................................................... 209 IV. Reaction Route Graphs ......................................................... 211  1. MCFC Cathodic Reactions ............................................. 212  2. HER Reactions ............................................................... 213 V. Discussion: Other Reaction Graphs...................................... 217  Acknowledgments ................................................................ 218 218References ............................................................................
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Chapter 4 APPROXIMATE ANALYTICAL SOLUTIONS FOR MODELS OF THREE-DIMENSIONAL ELECTRODES BY ADOMIAN’S DECOMPOSITION METHOD Keith Scott and Yan-Ping Sun  I. Introduction........................................................................... 222 II. Adomian’s Decomposition Method (ADM)......................... 223 III. Example of Applications to Catalytic reactions ................... 226  1. Model Solution ............................................................... 229  (i) Catalyst 229Slab ...........................................................  (ii......................................... 232) Spherical Catalyst Pellet  2. Concentration Profiles and Effectiveness....................... 234  (i) Concentration Profiles ............................................ 234  (ii) Effectiveness........................................................... 235 IV. Application to the Influence of Mass Transport in Electrocatalysts .................................. 239  1. Internal Diffusion and Film Mass Transport .................. 244  2. Agglomerate Model of Electrocatalysis ......................... 248 V. Application to Models For Three-Dimensional Electrodes.............................................................................. 251  1. The General Form of Model of Three-Dimension Electrodes...................................... 251  2. Porous Electrode Reactor ............................................... 252  3. Packed-Bed Electrode Reactor ....................................... 260  4. Simplification of Packed-Bed Electrode with a Low Conversion........................................................... 271 VI. Examples of Packed-Bed Electrodes applications............... 275  1. Electrochemical Reduction of Nitrobenzene in a Packed-Bed Electrode Reactor ................................ 275  2. Direct Electrochemical Oxidation of Propylene in a Sparged Packed-Bed Electrode Reactor .................. 282  3. Two-Dimensional Model of Packed-Bed Electrodes ........................................................................ 287 VII. Conclusions ......................................................................... 292 293Acknowledgement ...............................................................  Symbols ............................................................................... 293  1. ADM’s Nomenclature ................................................. 293  2. Nomenclatures in this Paper ........................................... 293  Appendix: ADM Mathematica Codes ................................. 296  1. ADM to Solve One ODE................................................ 296 2. ADM to Solve the Coupled ODE’s ................................ 299  References ........................................................................... 303
Index ........................................................................................... 305
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