Modern aspects of electrochemistry no 18 white

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LIST OF CONTRIBUTORS L I BOGUSLAVSKY A N Frumkin Institute of Electrochemistry Academy of Sciences of the USSR Moscow, USSR MARK E ORAZEM Department of Chemical Engineering University of Virginia Charlottesville, Virginia LAURENCE D BURKE Chemistry Department University College Cork Cork, Ireland PAUL J SIDES Department of Chemical Engineering Carnegie-Mellon University Pittsburgh, Pennsylvania F HINE Nagoya Institute of Technology Nagoya, Japan B V TILAK Occidental Chemical Corporation Research Center Grand Island, New York HIDEAKI KITA Department of Chemistry Faculty of Science Hokkaido University Sapporo, Japan MICHAEL E G LYONS Chemistry Department Trinity College Dublin, Ireland JOHN NEWMAN Materials and Molecular Research Division Lawrence Berkeley Laboratory and Department of Chemical Engineering University of California Berkeley, California KOHEI UOSAKI Department of Chemistry Faculty of Science Hokkaido University Sapporo, Japan K VISWANATHAN Occidental Chemical Corporation Research Center Grand Island, New York A Continuation Order Plan is available for this series A continuation order will bring delivery of each new volume immediately upon publication Volumes are billed only upon actual shipment For further information please contact the publisher MODERN ASPECTS OF ELECTROCHEMISTRY No 18 Edited by RALPH E WHITE Department of Chemical Engineering Texas A&M University College Station, Texas J O'M BOCKRIS Department of Chemistry Texas A&M University College Station, Texas and B E CONWAY Department of Chemistry University of Ottawa Ottawa, Ontario, Canada PLENUM PRESS • NEW YORK AND LONDON The Library of Congress cataloged the first volume of this title as follows: Modern aspects of electrochemistry, no [1] Washington, Butterworths, 1954v illus., 23 cm No 1-2 issued as Modern aspects series of chemistry Editors: no 1J Bockris (with B E Conway, No ) Imprint varies: no 1, New York, Academic P r e s s - N o 2, London, Butterworths Electrochemistry —Collected works I Bockris, John O'M ed II Conway, B E ed (Series: Modern aspects series of chemistry) QD552.M6 54-12732 rev ISBN 0-306-42312-X © 1986 Plenum Press, New York A Division of Plenum Publishing Corporation 233 Spring Street, New York, N.Y 10013 All rights reserved No part of this book may be reproduced, stored in a retrieval system, or transmitted in any form or by any means, electronic, mechanical, photocopying, microfilming, recording, or otherwise, without written permission from the Publisher Printed in the United States of America Preface This volume of Modem Aspects of Electrochemistry contains six chapters The first four chapters are about phenomena of interest at the microscopic level and the last two are on phenomena at the macroscopic level In the first chapter, Uosaki and Kita review various theoretical models that have been presented to describe the phenomena that occur at an electrolyte/semiconductor interface under illumination In the second chapter, Orazem and Newman discuss the same phenomena from a different point of view In Chapter 3, Boguslavsky presents state-of-the-art considerations of transmembrane potentials and other aspects of active transport in biological systems Next, Burke and Lyons present a survey of both the theoretical and the experimental work that has been done on hydrous oxide films on several metals The last two chapters cover the topics of the production of chlorine and caustic and the phenomena of electrolytic gas evolution In Chapter 5, Hine et al describe the engineering aspects of the three processes used in the chlor-alkali industry, and in Chapter 6, Sides reviews the macroscopic phenomena of nucleation, growth, and detachment of bubbles, and the effect of bubbles on the conductivity of and mass transfer in electrolytes Texas A&M University Texas A&M University University of Ottawa R E White J O'M Bockris B E Conway Contents Chapter THEORETICAL ASPECTS OF SEMICONDUCTOR ELECTROCHEMISTRY Kohei Uosaki and Hideaki Kita I Introduction II Electronic Energy Levels of Semiconductor and Electrolyte Junctions between Two Electronic Conductors Semiconductor/ Electrolyte Interface III Potential Distribution at Semiconductor/Electrolyte Interface Schottky Barrier Effect of the Redox Potential on the Potential Drop in the Semiconductor at the Semiconductor/Electrolyte Interfaces Distribution of Externally Applied Potential at the Semiconductor/Electrolyte Interfaces IV Distribution of Energy States for Ions of Redox System in Solution Importance of the Energy Levels of Redox Couples Gurney's Model Gerischer's Model Continuum Solvent Polarization Fluctuation Model Validity of the Models Vll 2 13 14 15 20 23 23 24 29 32 35 viii Contents V Rate Expressions for Electron Transfer at Illuminated Semiconductor/Electrolyte Interfaces Phenomenological Description The Model of Bockns and Uosaki Butler's Model—Semiconductor/Electrolyte Interface as a Schottky Barrier Competition between Surface Recombination and Charge Transfer Effects of Recombination in Space Charge Region Effects of Grain Boundary Recombination VI Concluding Remarks References 37 37 38 42 45 51 53 54 55 Chapter PHOTOELECTROCHEMICAL DEVICES FOR SOLAR ENERGY CONVERSION Mark E Orazem and John Newman I Semiconductor Electrodes Physical Description The Mechanism of Cell Operation II Mathematical Description Semiconductor Electrolyte Semiconductor-Electrolyte Interface Boundary Conditions Counterelectrode III Photoelectrochemical Cell Design Choice of Materials Solution of the Governing Equations The Influence of Cell Design IV Conclusions Notation References 62 63 66 69 70 76 78 82 83 84 85 87 91 98 99 101 Contents ix Chapter ELECTRON TRANSFER EFFECTS AND THE MECHANISM OF THE MEMBRANE POTENTIAL L I Boguslavsky I Introduction II Modeling Nonenzymatic Systems of Electron Transfer in the Initial Part of the Respiratory Chain of Mitochondria Respiratory Chain Potentials of the Respiratory Chain Elements Ubiquinones in the Respiratory Chain Participation of Membrane Lipids in the Functioning of the Respiratory Chain Transmembrane Potentials in the Chain NADHCoenzyme Q-O Participation of FMN in the Oxidation of Membrane Lipids Participation of FMN in the Transmembrane Transport of Protons Participation of FMN in the Transmembrane Transport of Electrons Interaction of FMN with Other Chain Components III Potential Generation on Bilayer Membranes Containing Chlorophyll Chlorophyll at the Membrane/Electrolyte Interface Redox Potentials of Chlorophyll Reactions of Chlorophyll Inserted in the Membrane with the Redox Components in an Aqueous Solution under Illumination Transmembrane Potentials in the Chain OX-CHLRED IV Possible Mechanisms of the Motion of Electrons and Protons in the Membrane Hypotheses on the Mechanism of Electron Motion in Biological Membranes 113 115 115 116 118 119 122 127 130 134 135 137 137 138 138 141 144 145 x Contents Ion Permeability of Bilayer Membranes in the Iodine/Iodide System Controlled by Redox Reactions at the Interface Electron and Proton Transport in Bilayers Containing Chlorophyll and Quinones under Illumination Possible Conductance Mechanisms in Bilayers Containing Ubiquinone Hypothesis on the Mechanism of Proton Transport in Biological Membranes Potentials of Coupling Membranes V Conclusions References 148 151 152 153 155 161 163 Chapter ELECTROCHEMISTRY OF HYDROUS OXIDE FILMS Laurence D Burke and Michael E G Lyons I II III IV V VI Introduction Formation of Hydrous Oxides Acid-Base Properties of Oxides Structural Aspects of Hydrous Oxides Transport Processes in Hydrous Oxide Films Theoretical Models of the Oxide-Solution Interphase Region Classical Models Nonclassical Models VII Platinum Monolayer Oxidation Hydrous Oxide Growth on Platinum VIII Palladium IX Gold Monolayer Behavior Hydrous Oxide Growth 169 171 173 179 182 188 189 189 191 191 198 205 208 208 210 Contents xi X Iridium Monolayer Growth Hydrous Oxide Films XI Rhodium Hydrous Oxide Growth Behavior of Rh/Pt Alloys XII Ruthenium XIII Some Nonnoble Metals Iron and Cobalt Nickel and Manganese Tungsten XIV Conclusion Addendum References 213 213 214 224 224 226 227 230 230 233 238 239 241 243 Chapter CHEMISTRY AND CHEMICAL ENGINEERING IN THE CHLOR-ALKALI INDUSTRY F Hine, B V Tilak, and K Viswanathan I Introduction II Chemical and Electrochemical Principles Involved in Chlor-Alkali Production III Manufacturing Processes Importance of Brine Purification Diaphragm Cell Process Membrane Cell Process Mercury Cell Process IV Electrode Materials and Electrode Processes Anodes Cathodes V Engineering Aspects in Chlor-Alkali Operations Chemical Engineering Aspects of Amalgam Decomposition Chemical Engineering Aspects of Porous Diaphragms 249 250 253 253 256 259 260 263 263 268 270 270 279 xii VI Ion-Exchange Membranes and Membrane Technology General Requirements of Membranes for ChlorAlkali Production Properties of Membranes and Their Performance Characteristics Engineering Design Aspects of Ion-Exchange Membrane Cell Technology Advantages Afforded by Membrane Technology State of the Art of Membrane Cell Technology Notation References Contents 287 287 288 292 295 296 297 298 Chapter PHENOMENA AND EFFECTS OF ELECTROLYTIC GAS EVOLUTION Paul J Sides I Introduction II Nucleation, Growth, and Detachment of Bubbles Nucleation Growth Detachment Effect of Additives and Operating Parameters III Electrical Effects of Gas Evolution Conductivity of Bulk Dispersions Electrical Effects of Bubbles on Electrodes IV Mass Transfer at Gas-Evolving Electrodes Penetration Theory The Hydrodynamic Model The Microconvection Model Microscopic Investigation V Summary Notation References 303 304 304 306 312 315 318 318 330 342 342 344 347 348 348 349 352 Index 355 .. .MODERN ASPECTS OF ELECTROCHEMISTRY No 18 Edited by RALPH E WHITE Department of Chemical Engineering Texas A&M University College Station, Texas J O'M BOCKRIS Department of Chemistry... Department of Chemistry University of Ottawa Ottawa, Ontario, Canada PLENUM PRESS • NEW YORK AND LONDON The Library of Congress cataloged the first volume of this title as follows: Modern aspects of electrochemistry, ... electrochemistry, no [1] Washington, Butterworths, 1954v illus., 23 cm No 1-2 issued as Modern aspects series of chemistry Editors: no 1J Bockris (with B E Conway, No ) Imprint varies: no 1, New York,
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Xem thêm: Modern aspects of electrochemistry no 18 white , Modern aspects of electrochemistry no 18 white , II. ELECTRONIC ENERGY LEVELS OF SEMICONDOCTOR AND ELECTROLYTE, III. POTENTIAL DISTRIBUTION AT SEMICONDUCTOR / ELECTROLYTE INTERFACE, IV. DISTRIBUTION OF ENERGY STATES FOR IONS OF REDOX SYSTEM IN SOLUTION, V. RATE EXPRESSIONS FOR ELECTRON TRANSFER AT ILLUMINATED INTERFACE, Ch 2. Photoelectrochemical Devices for Solar Energy Conversion, II. MODELING NONENZYMATIC SYSTEMS OF ELECTRON TRANSFER, III. POTENTIAL GENERATION ON BILAYER MEMBRANES CONTAINING CHLOROPHYLL, IV. POSSIBLE MECHANISMS OF THE MOTION OF ELECTRONS AND PROTONS IN THE MEMBRANE, III. ACID-BASE PROPERTIES OF OXIDES, IV. STRUCTURAL ASPECTS OF HYDROUS OXIDES, II. CHEMICAL AND ELECTROCHEMICAL PRINCIPLES, II. NUCLEATION, GROWTH, AND DETACHMENT OF BUBBLES, III. ELECTRICAL EFFECTS OF GAS EVOLUTION, IV. MASS TRANSFER AT GAS-EVOLVING ELECTRODES

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