《Electrochemical Impedance Spectroscopy in PEM Fuel Cells：Fundamentals an...
《Electrochemical Impedance Spectroscopy in PEM Fuel Cells：Fundamentals and Applications》质子交换膜燃料电池的电化学阻抗谱：原理与应用
作者：
Xiao-Zi Yuan
Chaojie Song
Haijiang Wang
Jiujun Zhang
National Research Council of Canada
Institute for Fuel Cell Innovation
出版社：Springer
出版时间：2010年
目录
Acronyms and Abbreviations...............................................................................xi
1 PEM Fuel Cells and their Related Electrochemical Fundamentals ............. 1
1.1 Fuel Cell Description.................................................................................. 1
1.2 Fuel Cell Types.......................................................................................... 4
1.2.1 H2/Air Fuel Cells ............................................................................ 5
1.2.2 Direct Liquid Fuel Cells ................................................................. 8
1.2.3 Alkaline Fuel Cells ....................................................................... 10
1.2.4 Phosphoric Acid Fuel Cells .......................................................... 11
1.3 Fuel Cell Challenges................................................................................ 12
1.4 PEM Fuel Cell Electrochemistry ............................................................. 13
1.4.1 Electrochemistry Fundamentals.................................................... 13
1.4.2 Polarization Curves ...................................................................... 20
1.4.3 Current Interruption......................................................................20
1.4.4 Chronoamperometry.....................................................................21
1.4.5 Cyclic Voltammetry ..................................................................... 22
1.4.6 Electrochemical Impedance Spectroscopy ...................................26
1.5 Fuel Cell Analysis.................................................................................... 28
1.5.1 Open Circuit Voltage....................................................................29
1.5.2 Cell Voltage Under Load.............................................................. 31
1.5.3 Ohmic Drop..................................................................................34
1.5.4 Mass Transfer Drop......................................................................34
1.5.5 Fuel Cell Efficiencies ................................................................... 35
1.6 Chapter Summary ....................................................................................36
References................................................................................................36
2 Electrical Fundamentals................................................................................. 39
2.1 Introduction..............................................................................................39
2.2 Direct Current Circuits............................................................................. 40
2.2.1 Ohm’s Law...................................................................................40
2.2.2 Series and Parallel Circuits........................................................... 41
2.2.3 Kirchhoff’s Laws..........................................................................42
2.2.4 Resistors in DC Circuits ............................................................... 43
2.2.5 Capacitors in DC Circuits............................................................. 45
2.2.6 Inductors in DC Circuits............................................................... 49
2.3 Alternating Current Circuits .................................................................... 50
2.3.1 Sinusoidal Systems.......................................................................50
2.3.2 Resistors in AC Circuits ............................................................... 52
viii Contents
2.3.3 Capacitors in AC Circuits............................................................. 53
2.3.4 Inductors in AC Circuits............................................................... 53
2.4 Complex Algebra and Impedance............................................................ 54
2.4.1 AC Impedance of a Resistor–Capacitor Circuit............................ 56
2.4.2 AC Impedance of a Resistor–Inductor Circuit ............................. 59
2.4.3 AC Impedance of a Capacitor–Inductor Circuit ........................... 61
2.4.4 AC Impedance of a Resistor–Capacitor–Inductor Circuit ............ 63
2.5 Network Circuit Analysis ........................................................................ 72
2.5.1 Topological Features of a Network .............................................. 72
2.5.2 Network Theorems .......................................................................73
2.5.3 Transient Network Analysis ......................................................... 78
2.6 Basic Knowledge for Understanding EIS ................................................ 81
2.6.1 Introduction ..................................................................................81
2.6.2 Nyquist and Bode Plots ................................................................ 82
2.6.3 Equivalent Circuit Models............................................................ 84
2.6.4 Data Fitting of EIS........................................................................ 89
2.6.5 Applications..................................................................................92
2.7 Chapter Summary... .................................................................................93
References................................................................................................93
3 Impedance and its Corresponding Electrochemical Processes ................... 95
3.1 Electrode/Electrolyte Interfaces................................................................95
3.1.1 Introduction ..................................................................................95
3.1.2 Equivalent Circuit of an Electrode/Electrolyte Interface.............. 96
3.1.3 Differences Between Solid State and Aqueous Electrochemistry 97
3.2 Faradaic Impedance .................................................................................98
3.2.1 Calculation of the Faradaic Impedance at the Equilibrium
Electrode Potential.. ..................................................................... 98
3.2.2 Kinetic Parameters from Zf ......................................................... 104
3.2.3 Vectorgraphs of Faradaic Impedance....................... ............ ......108
3.3 Total Impedance of an Electrochemical System.................................... 109
3.3.1 Calculated Zf Based on Experimental Measurements................. 109
3.3.2 Graphic Presentations of the Total Impedance ........................... 112
3.3.3 Impedance Plots of Real Electrochemical Systems Using the
Complex Plane ........................................................................... 116
3.3.4 Semicircle Rotation of the Impedance........................................ 118
3.4 Correlation of EIS with Other Electrochemical Techniques.................. 123
3.4.1 EIS and the Polarization Curve................................................... 123
3.4.2 EIS and Current Interruption ...................................................... 128
3.5 EIS Measurements ................................................................................. 129
3.6 Advantages and Limitations of EIS ....................................................... 133
3.6.1 EIS Advantages ..........................................................................133
3.6.2 EIS Limitations........................................................................... 134
3.7 Chapter Summary ..................................................................................135
References..............................................................................................136
Contents ix
4 EIS Equivalent Circuits................................................................................ 139
4.1 Electrochemical Elements......................................................................... 139
4.1.1 Lumped Elements.......................................................................139
4.1.2 Frequency-Dependent Elements.................................................140
4.1.3 Bounded Frequency-Dependent Elements.................................. 142
4.2 Basic Equivalent Circuits....................................................................... 143
4.2.1 Simple Combinations of Electrical Elements........ ..................... 143
4.2.2 Randles Cell................................................................................ 154
4.2.3 Structural Circuits....................................................................... 168
4.2.4 Other Circuits .............................................................................177
4.3 Brief Discussion of Equivalent Circuits in PEM Fuel Cells .................. 180
4.3.1 Gas Diffusion Layers.................................................................. 180
4.3.2 Catalyst Layers ........................................................................... 180
4.3.3 Proton Exchange Membranes..................................................... 184
4.3.4 Conductive Polymers..................................................................184
4.3.5 Membrane Electrode Assemblies ............................................... 191
4.4 Chapter Summary ..................................................................................191
References..............................................................................................191
5 EIS Diagnosis for PEM Fuel Cell Performance ......................................... 193
5.1 Ex Situ Diagnosis................................................................................... 193
5.1.1 Electrode Characterization ......................................................... 193
5.1.2 Membrane Characterization ....................................................... 202
5.1.3 Comparison of Ex Situ and In Situ EIS Methods ....................... 212
5.2 In Situ Diagnosis.................................................................................... 213
5.2.1 Different Gas Feeding Modes..................................................... 214
5.2.2 Measurement Modes ..................................................................237
5.2.3 Operating Conditions..................................................................239
5.2.4 Reference Electrodes .................................................................. 243
5.3 EIS Under Heavy Duty .......................................................................... 250
5.3.1 Introduction ................................................................................250
5.3.2 Grounded Mode.......................................................................... 251
5.3.3 Floating Mode ............................................................................ 254
5.4 Fast EIS..................................................................................................255
5.4.1 Principles and Measurements ..................................................... 255
5.4.2 Differences Between Frequency Domain and Time Domain ..... 256
5.5 Chapter Summary ..................................................................................257
References..............................................................................................258
6 EIS Applications ........................................................................................... 263
6.1 EIS Applications in PEMFCs ................................................................ 263
6.1.1 Optimization of MEA Structure ................................................. 264
6.1.2 Ionic Conductivity ...................................................................... 288
6.1.3 Contamination ............................................................................295
6.1.4 Stack and Individual Cell Impedance ......................................... 298
6.1.5 Localized EIS .............................................................................307
6.1.6 EIS at High Temperatures .......................................................... 313
x Contents
6.2 EIS Applications in DMFCs .................................................................. 323
6.2.1 Ex Situ Methanol Oxidation ....................................................... 323
6.2.2 In Situ Anode Reaction .............................................................. 335
6.2.3 Determination of the Ionic Resistance........................................ 338
6.2.4 In Situ Cathode Reaction............................................................ 339
6.3 Chapter Summary ..................................................................................342
References..............................................................................................342
Appendix A: Fourier Transform....................................................................... 347
Appendix B: Laplace Transform...................................................................... 353
Appendix C: Kramers–Kronig Transform...................................................... 363
Appendix D: Effects of Equivalent Circuit Parameters on Nyquist Plots ..... 371
Contributor Biographies.................................................................................... 411
Index .................................................................................................................... 413
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