Electrochemical Process Engineering. A Guide to the Design of Electrolytic Plant
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1 Electrochemical Process Engineering A Guide to the Design of Electrolytic Plant
2 Electrochemical Process Engineering A Guide to the Design of Electrolytic Plant F. Goodridge and K. Scott University of Newcastle upon Tyne Newcastle upon Tyne, England Springer Science+ Business Media, LLC
3 Library of Congress Cataloging-In-Publication Data GoodrIdge. F., Electrochemlcal process engineering : a guide to the design of electrolytic plant I F. Goodridge and K. Scott. p. c. Includes bibliographical references and Index. ISBN ISBN (ebook) DOI / ElectrocheMistry, Industrial. I. Scott, K. 1Kennethl, II. Title. TP255.G ' dc CIP ISBN Springer Science+ Business Media New York Originally published by Plenum Press, New York in 1995 Softcover reprint of the hardcover 1st edition 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
4 Our sincere thanks are due to our colleague Dr. R. E. Plimley for his considerable help during the preparation of this book.
5 Preface As the subtitle indicates, the overriding intention of the authors has been to provide a practical guide to the design of electrolytic plant. We wanted to show that the procedures for the design and optimization of such a plant are essentially simple and can be performed by readers comparatively new to the electrochemical field. It was important to realize that electrochemical engineering should not be confused with applied electrochemistry but had to be based on the principles of chemical engineering. For this reason, reference is often made to standard chemical engineering texts. Since this is a practical guide rather than a textbook, we have included a large number of worked examples on the principle that a good worked example is worth many paragraphs of text. In some examples we have quoted costs, e.g., of chemicals, plant or services. These costs are merely illustrative; current values will have to be obtained from manufacturers or journals. If this is not possible, approximate methods are available for updating costs to present-day values (see Refs. 1 and 3, Chapter 6). At the end of the book you will realize that there has been no recommendation or discussion of particular software packages for costing or design. There are two reasons for this omission. First, we wanted to emphasize the basic principles of design so that readers would be in a position to question in an informed way the basic assumptions of any design package. Second, changes and updates in design software are so frequent that any recommendations would soon be out of date. Although design software packages including electrochemical stages are still not numerous, any final design today will be computer-based. This has been no handicap vii
6 viii Preface to the present book, which is concerned mainly with preliminary cost estimation and design. We have emphasized the use of reaction, reactor, and process models. We have tried to show-and this is a message close to our hearts-that even simple models can lead to significant savings. For example, minimizing pilot plant experimentation can reduce development cost considerably. A reaction model can tell the development scientist or engineer which parameters under investigation are particularly important, in this way shortening experimentation time. One might ask, "If design methods are based on chemical engineering, is it worthwhile to present a text specializing in electrochemical plant?" The answer is that, in our experience of running short courses in electrochemical engineering, scientists and engineers have found it useful to be presented with detailed examples of the application of chemical engineering principles to an electrochemical situation. The reason can be found in university training, where electrochemistry is still the Cinderella of reaction techniques, particularly in chemical engineering courses. The treatment to be found below is loosely based on the short courses we have been running for many years in the Department of Chemical and Process Engineering at the University of Newcastle upon Tyne, England. Enthusiastic response from participants all over the world has led us to hope that this book will be considered as useful as, apparently, the courses have been. The book has been written for undergraduate and graduate students of science and engineering, as well as for the practicing chemist and chemical engineer who have had little previous experience of designing and scaling up electrochemical processes. Our sincere thanks are due to our colleague Dr. R. E. Plimley for his considerable help during the preparation of this book. University of Newcastle upon Tyne F. Goodridge K. Scott
7 Contents Chapter 1 Introduction to Electrochemical Engineering 1.1. What is Electrochemical Engineering? Aims and Intentions of this Book The Industrial Importance of Electrolytic Processes Some Basic Concepts and Definitions Electrolytic Cells and Faraday's Law Basic Terminology Faraday's Law Current Density, Electrode Potential, and Current Efficiency Exchange Current Density The Double Layer Cell Voltage Criteria for Reactor Performance Electrochemical and Catalytic Reactions, and Reactors References Chapter 2 Aspects of Mass and Heat Transfer and the Energetics of Electrolytic Cell Systems 2.1. Introduction Some Basic Aspects of Fluid Dynamics Mass Transfer Mass Flux in a Fully Developed Turbulent Regime ix
8 X Contents Entrance and Exit Effects Obtaining Numerical Values of kl by Calculation Rectangular Flow Channels The Annulus Rotating Cylinder Electrodes Rotating Disk Electrodes Obtaining Numerical Values of kl by Experiment The Chemical System The Experimental Arrangement Turbulent Flow Promoters Inert Promoters Electroactive Promoters Mass Transfer in Two-Phase Flow Energetics Voltage Requirements Open-Circuit Voltage The Effect of Temperature on Open-Circuit Voltage The Effect of Activity or Concentration on Open-Circuit Voltage Parallel Reactions Ohmic Voltage Losses Electrolyte Resistance Gas Evolution Diaphragm Resistance Resistance of Solid Conductors Total Cell Voltage Energy Balances Thermodynamic Relationships Reactor Energy Balances o2ol. Continuous Operation Batch Operation Energy Balance for Aluminum Production Concluding Remarks References Chapter 3 Rate Processes and Reaction Models 301. Rate Processes Elementary and Overall Reactions
9 Contents xl Chapter Kinetics of Elementary Reactions Velocity Constant Reversibility and Irreversibility The Effect of Temperature on Reaction Rate Reaction Mechanisms and Rate Laws Steady State Approximation and the Development of Rate Laws The Rate-Determining Step Transition State Theory Derivation of Some Kinetic Relationships Steps in an Electrode Process Charge Transfer, Activation, or Kinetic Control Diffusion or Mass Transport Control Charge Transfer and Diffusion Control Combined Charge Transfer with Adsorption on the Electrode Electrocatalysis Reaction Models General Considerations Experimental Methods of Obtaining Model Constants Methodology Experimental Equipment Ohmic Correction to the Electrode Potential Methods of Determining the Ohmic Correction Examples of Reaction Models The Reduction of U(VI) to U(IV) The Production of p-anisidine Concluding Remarks References Reactor Models 4.1. General Considerations The Batch Reactor Batch Reactors without Electrolyte Recycle Batch Reactors with Electrolyte Recycle
10 xli Contents Recirculation through a Plug-Flow Batch Reactor Recirculation through a Stirred-Tank Reactor Modeling Batch Reactors The Continuous Reactor Concluding Remarks References Chapter 5 Electrolytic Reactor Design, Selection, and Scale-up 5.1. Electrolytic Reactor Designs Classifications of Reactors Scheme Based on Reactor Engineering Principles Scheme Based on Electrochemical Modes of Operation Electrical Connections to Cells Hydraulic Connections General Purpose Flow Electrolyzers Other Cell Designs Electrolytic Reactor Selection Scale-up of Electrolytic Reactors General View of Scale-up Procedures Design Scheme for the Scale-up of Electrochemical Reactors Effect of Scale-up on Reactor Performance Scale-up Methods and Similarity Reactor Size and Geometric Similarity Fluid Mechanics and Kinematic Similarity Concentration Distribution and Chemical Similarity Current Distribution and Electrical Similarity Heat Transfer and Thermal Similarity The Effect of Scale-up on Mass Transfer The Effect of Scale-up on Current Distribution Primary Current Distribution Secondary Current Distribution Tertiary Current Distribution The Effect of Gas Evolution on Current Distribution
11 Contents xiii The Effect of Finite Electrode Conductivity on Current Distribution Current Distribution in Three-Dimensional Electrodes Concluding Remarks Multiple Electrode Modules Time Factors References Chapter 6 Cost Estimation, Profit Appraisal, Process Modeling, and Optimization 6.10 Cost Estimation and Profit Appraisal ol.l. Costing Procedures Capital and Capital-Related Costs Production and Production-Related Costs Example of a Predesign Cost Estimate for Producing Glyoxylic Acid by the Electrolytic Reduction of Oxalic Acid ol.2ol. Basis for Cost Estimation Process Conditions Capital Costs Production Costs Capital Depreciation ol.2o6o Added Value per kg of Glyoxylic Acid Costing Figures for a Product Throughput of 1000 kg/annum Maximum Amount of Glyoxylic Acid that Can Be Produced per Annum with the Two-Module Cell ol.2o9o Costing Figures for a Product Throughput of 4000 kg/ Annum Comments on the Above Cost Calculations Profitability Criteria for Optimization Process Modeling and Optimization Example of the Optimization of Current Density in a Batch Reactor Interactions Between an Electrochemical Reactor and Associated Unit Processes Example of a Process Model to Demonstrate Interaction The Electrochemical Reactions
12 xlv Contents Mass Balance The Reactor The Distillation Column Interactive Behavior Example of Optimization and a Choice between Alternatives Concluding Remarks Afterword Costs Specific to Electrolytic Processes Duty of Heat Exchangers Continuous Operation Batch Operation References Appendix: Notation of Variables Index
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