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High Temperature
Solid Oxide Fuel Cells
Fundamentals, Desig
and Apdirations
J;
2 '

cubhash r cinghal and Kevin Kendal

 h Temperature
Solid Oxide Fuel Cells:
Fundamentals, Design and Applications
 ~

High Temperature
Solid Oxide Fuel Cells:
Fundamentals, Design and Applications

Edited by:
Subhash C Singhal and Kevin Kendall

ELSEVIER
UK ElsevierLtd, The Boulevard, LangfordLane,Kidlington, Oxford OX5 IGB, UK
USA Elsevier Inc, 360 Park AvenueSouth, New York, NY 10010-1710,USA
JAPAN Elsevier Japan,Tsunashima Building Annex, 3-20-12 Yushima.
Bunlryo-ku,Tokyo 113, Japan

Copyright 02003 Elsevier Ltd.

All rights reserved. No part of this publication may be reproduced, stored in
a retrieval system or transmitted in any form or by anj7 means: electronic,
electrostatic, magnetic tape, mechanical, photocopying, recording or
otherwise, without prior permission in writing from the publishers.

British Library Cataloguing in Publication Data

High temperature solid oxide fuel cells: fundamentals,
design and applications
1.Solid oxide fuel cells
I. Singhal, Subhash C. 11. Kendall, Kevin, 1943-
62 1.3’12429
ISBN 1856173879

Library of Congress Cataloging-in-PublicationData

High temperature solid oxide fuel cells: fundamentals, design and
applications / edited by Subhash C. Singhal and Kevin Kendall.
p. cm.
Includes bibliographical references and index.
ISBN 1-85617-387-9 (hardcover)
1.Solidoxidefuelcells. I. Singhal, SubhashC. II.Kendal1,Kevin, 1943-
TIC2931 .H54 2002
62 1.31’2429-dc2 1 2002040761

No responsibility is assumed by the Publisher for any injury and/or damage

to persons or property as a matter of products liability, negligence or
otherwise, or from any use or operation of any methods, products,
instructions or ideas contained in the material herein.
Published by
Elsevier Advanced Technology, The Boulevard, Langford Lane, Kidlington
Oxford OX5 lGB, UK
Tel.: +44(0) 1865 843000
Fax: +44(0) 1865 843971
Typeset by Variorum Publishing Ltd, Lancaster and Rugby
Printed and bound in Great Britain by MPG Books Ltd, Bodmin, Cornwall
Contents

List of Contributors xi
Preface xv

Chapter 1 Introduction to SOFCs

1.1 Background 1
1.2 Historical Summary 2
1.3 Zirconia Sensors for Oxygen Measurement 4
1.4 Zirconia Availability and Production 5
1.5 High-Quality Electrolyte Fabrication Processes 7
1.6 Electrode Materials and Reactions 8
1.7 Interconnection for Electrically Connecting the Cells 11
1.8 Cell and Stack Designs 12
1.9 SOFC Power Generation Systems 14
1.10 Fuel Considerations 15
1.11 Competition and Combination with Heat Engines 17
1.12 Application Areas and Relation to Polymer Electrolyte
Fuel Cells 18
1.13 SOFC-Related Publications 19
References 19

Chapter 2 History
2.1 The Path to the First Solid Electrolyte Gas Cells 23
2.2 From Solid Electrolyte Gas Cells to Solid Oxide Fuel Cells 26
2.3 First Detailed Investigations of Solid Oxide Fuel Cells 29
2.4 Progressin the 1960s 32
2.5 On the Path to Practical Solid Oxide Fuel Cells 40
References 44

Chapter 3 Thermodynamics
3.1 Introduction 53
3.2 The Ideal Reversible SOFC 56
3.3. Voltage Losses by Ohmic Resistance and by Mixing
Effects by Fuel Utilisation 62
vi High Temperature Solid Oxide Fuel Cells: Fundamentals, Design and Applications

3.4 Thermodynamic Definition of a Fuel Cell Producing

Electricity and Heat 66
3.5 Thermodynamic Theory of SOFC Hybrid Systems 69
3.6 Design Principles of SOFC Hybrid Systems 77
3.7 Summary 80
References 81

Chapter 4 Electrolytes
4.1 Introduction 83
4.2 Fluorite-Structured Electrolytes 83
4.3 Zirconia-Based Oxide Ion Conductors 89
4.4 Ceria-Based Oxide Ion Conductors 92
4.5 Fabrication of ZrOz and Ce02-BasedElectrolyte Films 94
4.6 Perovskite-Structured Electrolytes 96
4.6.1 LaA103 97
4.6.2 LaGa03 Doped with Ca, Sr andMg 99
4.6.3 LaGaOs Doped with Transition Elements 104
4.7 Oxides with Other Structures 106
4.7.1 Brownmillerites (e.g. Ba2InzO6) 106
4.7.2 Non-cubic Oxides 108
4.8 Proton-Conducting Oxides 110
4.9 Summary 112
References 112

Chapter 5 Cathodes
5.1 Introduction 119
5.2 Physical and Physicochemical Properties of
Perovskite Cathode Materials 120
5.2.1 Lattice Structure, Oxygen Nonstoichiometry,
and Valence Stability 120
5.2.2 Electrical Conductivity 123
5.2.3 Thermal Expansion 125
5.2.4 Surface Reaction Rate and Oxide Ion
Conductivity 126
5.3 Reactivity of Perovskite Cathodes with Zr02 130
5.3.1 Thermodynamic Considerations 130
5.3.1.1 Reaction ofperovskites with the
Zirconia Component in YSZ 130
5.3.1.2 Reactionofperovskite with the
yttria (dopant) component in YSZ 130
5.3.1.3 Interdiffusion between Perovskite
and Fluorite Oxides 131
5.3.2 Experimental Efforts 132
5.3.3 Cathode/Electrolyte Reactions and Cell
Performance 134
5.3.4 Cathodes for Intermediate Temperature SOFCs 1 36
 Contents vii

5.4 Compatibility of Perovskite Cathodes with

Interconnects 138
5.4.1 Compatibilityof Cathodes with Oxide
Interconnects 138
5.4.2 Compatibilityof Cathodes with Metallic
Interconnects 139
5.5 Fabrication of Cathodes 142
5.6 Summary 143
References 143

Chapter 6 Anodes
6.1 Introduction 149
6.2 Requirements for an Anode 150
6.3 Choice of Cermet Anode Components 151
6.4 Cermet Fabrication 153
6.5 Anode Behaviour Under Steady-State Conditions 156
6.6 Anode Behaviour Under Transients Near Equilibrium 158
6.7 Behaviour of Anodes Under Current Loading 160
6.8 Operation of Anodes with Fuels other than Hydrogen 164
6.9 Anodes for Direct Oxidation of Hydrocarbons 165
6.10 Summary 168
References 169

Chapter 7 Interconnects
7.1 Introduction 173
7.2 Ceramic Interconnects (Lanthanum and
Yttrium Chromites) 174
7.2.1 Electrical Conductivity 174
7.2.2 Thermal Expansion 177
7.2.3 Thermal Conductivity 178
7.2.4 Mechanical Strength 178
7.2.5 Processing 179
7.3 Metallic Interconnects 181
7.3.1 Chromium-Based Alloys 181
7.3.2 Ferritic Steels 182
7.3.3 Other Metallic Materials 186
7.4 Protective Coatings and Contact Materials for
Metallic Interconnects 187
7.5 Summary 189
References 190

Chapter 8 Cell and Stack Designs

8.1 Introduction 197
8.2 Planar SOFC Design 197
8.2.1 Cell Fabrication 205
viii High Temperature Solid Oxide Fuel CeJIs: Fundamentals, Design and Applications

8.2.1.1 Cell Fabrication Based on

Particulate Approach 205
8.2.1.2 Cell Fabrication Based on
Deposition Approach 206
8.2.2 Cell and Stack Performance 208
8.3 Tubular SOFC Design 210
8.3.1 Cell Operation and Performance 213
8.3.2 Tubular Cell Stack 2 14
8.3.3 Alternative Tubular Cell Designs 216
8.4 Microtubular SOFC Design 219
8.4.1 Microtubular SOFC Stacks 222
8.5 Summary 224
References 22 5

Chapter 9. Electrode Polarisations

9.1 Introduction 230
9.2 Ohmic Polarisation 232
9.3 Concentration Polarisation 233
9.4 Activation Polarisation 237
9.4.1 Cathodic Activation Polarisation 243
9.4.2 Anodic Activation Polarisation 249
9.5 Measurement of Polarisation (By Electrochemical
Impedance Spectroscopy) 251
9.6 Summary 257
References 257

Chapter 10 Testing of Electrodes, Cells and Short Stacks

10.1 Introduction 261
10.2 Testing Electrodes 262
10.3 Testing Cells and 'Short' Stacks 267
10.4 Area-SpecificResistance (ASR) 2 72
10.5 Comparison of Test Results on Electrodes and
on Cells 277
10.5.1 Non-activated Contributions to the
Total Loss 280
10.5.2 Inaccurate Temperature Measurements 2 80
10.5.3 Cathode Performance 281
10.5.4 Impedance Analysis of Cells 282
10.6 The Problem of Gas Leakage in Cell Testing 283
1 0 . 6 , l Assessment of the Size of the Gas Leak 284
10.7 Summary 286
References 286

Chapter 11 Cell, Stack and System Modelling

11.1 Introduction 293
11.2 Flow and Thermal Models 294
 Contents ix

11.2.1 Mass Balance 295

11.2.2 Conservation ofMomentum 295
11.2.3 Energy Balance 296
11.3 Continuum-Level Electrochemistry Model 299
11.4 Chemical Reactions and Rate Equations 303
11.5 Cell- and Stack-LevelModelling 308
11.6 System-LevelModelling 314
11.7 Thermomechanical Model 315
11.8 Electrochemical Models at the Electrode Level 318
11.8.1 Fundamentals and Strategy of
Electrode-Level Models 319
11.8.2 ElectrodeModels Based on a Mass
Transfer Analysis 321
11.8.3 One-DimensionalPorous Electrode
Models Based on Complete
Concentration, Potential, and
Current Distributions 322
11.8.4 Monte Carlo or Stochastic Electrode
Structure Model 324
11.8.4.1 Electrode or Cell Models Applied to
Ohmic Resistance-Dominated Cells 324
1 1.8.4.2 Diagnostic Modelling of
Electrodes to Elucidate Reaction
Mechanisms 324
11.8.4.3 Models ofMixed Ionic and
Electronic Conducting (MIEC)
Electrodes 325
11.9 Molecular-Level Models 325
11.10 Summary 326
References 327

Chapter 12 Fuels and Fuel Processing

12.1 Introduction 333
12.2 RangeofFuels 335
12.3 Direct and Indirect Internal Reforming 338
12.3.1 Direct Internal Reforming 340
12.3.2 Indirect Internal Reforming 341
12.4 Reformation of Hydrocarbons by Steam,
COz and Partial Oxidation 342
12.5 Direct Electrocatalytic Oxidation of Hydrocarbons 346
12.6 CarbonDeposition 347
12.7 Sulphur Tolerance and Removal 351
12.8 Anode Materials in the Context of Fuel Processing 352
12.9 Using Renewable Fuels in SOFCs 3 54
12.10 Summary 355
References 356
x High Temperature SoIid Oxide Fuel Cells: Fundamentals, Design and Applications

Chapter 13 Systems and Applications

13.1 Introduction 3 63
13.2 Trends in the Energy Markets and SOFCApplicability 365
13.3 Competing Power Generation Systems and SOFC
Applications 367
13.4 SOFC System Designs and Performance 3 70
13.4.1 Atmospheric SOFC Systems for Distributed
Power Generation 3 70
13.4.2 Residential, Auxiliary Power and Other
Atmospheric SOFC Systems 3 73
13.4.3 Pressurised SOFC/TurbineHybrid Systems 3 74
13.4.4 System Control and Dynamics 3 76
13.4.5 SOFC System Costs 3 78
13.4.6 Example of a SpecificSOFC System
Application 3 79
13.5 SOFC System Demonstrations 380
13.5.1 Siemens Westinghouse Systems 3 80
13.5.1.1 100 kWAtmospheric
SOFC System 380
13.5.1.2 220 kWPressurised
SOFC/GT Hybrid System 383
13.5.1.3 Other Systems 384
13.5.2 Sulzer Hexis Systems 385
13.5.3 SOFC Systems ofother Companies 386
13.6 Summary 388
References 389

Index 393
List of Contributors

Harlan U Anderson
Electronic Materials Applied Research Center, 104 Straumanis Hall, University
ofMissouri-Rolla, Rolla, MO 65410-1240, USA
[email protected]

Rob J F van Gerwen,

KEMA Power Generation & Sustainables, KEMA Nederland BV, PB 9035, 6800
ET Arnhem, The Netherlands
[email protected]

Peter Vang Hendriksen

Materials Research Department, Risra National Laboratory, DK-4000 Roskilde,
Denmark
[email protected]
Teruhisa Horita
National Institute of Advanced Industrial Science and Technology, AIST
Tsukuba CentralNo. 5, Higashi 1-1-1,Tsukuba, Ibaraki 305-8565, Japan
[email protected]

Tatsumi Ishihara
Department of Applied Chemistry, Faculty of Engineering, Kyushu University,
Hakozaki 6-10-1, Higashi-ku, Fukuoka 812-8581, Japan
[email protected]
Ellen Ivers-Tiffee
Institut fur Werkstoffe der Elektrotechnik IWE, Universitat Karlsruhe (TH),
Adenauerring 20, 7613 1Karlsruhe, Germany
[email protected]
Kevin Kendall
School of Chemical Engineering, The University of Birmingham, Edgbaston,
Birmingham B15 2TT, UIC
[email protected]
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