Molecular Catalysts for Energy Conversion

By: Tatsuhiro Okada (Editor), Masao Kaneko (Editor)

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Hardcover | 7 May 2012

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Over the past decade the topic of energy and environment has been ackno- edged among many people as a critical issue to be solved in 21st century since the Kyoto Protocol came into e?ect in 1997. Its political recognition was put forward especially at Heiligendamm in 2007, when the e?ect of carbon dioxide emission and its hazard in global climate were discussed and shared univ- sallyascommonknowledge.Controllingtheglobalwarmingintheeconomical framework of massive development worldwide through this new century is a very challenging problem not only among political, economical, or social c- cles but also among technological or scienti?c communities. As long as the humans depend on the combustion of fossil for energy resources, the waste heat exhaustion and CO emission are inevitable. 2 In order to establish a new era of energy saving and environment benign society, which is supported by technologies and with social consensus, it is important to seek for a framework where new clean energy system is inc- porated as infrastructure for industry and human activities. Such a society strongly needs innovative technologies of least CO emission and e?cient en- 2 ergy conversion and utilization from remaining fossil energies on the Earth. Energy recycling system utilizing natural renewable energies and their c- version to hydrogen may be the most desirable option of future clean energy society. Thus the society should strive to change its energy basis, from foss- consuming energy to clean and recycling energy.

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Non-Fiction Engineering & Technology Mechanical Engineering & Materials Materials Science Science Physics Nuclear Physics Energy Technology & Engineering Electrical Engineering Energy Conversion & Storage Chemistry Physical Chemistry

Catalysis Optical Physics Industrial Chemistry & Manufacturing Technologies Industrial Chemistry Atomic & Molecular Physics

Preface	p. V
List of Contributors	p. XVII
List of Abbreviations	p. XXI
Historical Overview and Fundamental Aspects of Molecular Catalysts for Energy Conversion	p. 1
Introduction: Why Molecular Catalysts? A New Era of Biomimetic Approach Toward Efficient Energy Conversion Systems	p. 1
Molecular Catalysts for Fuel Cell Reactions	p. 2
Oxygen Reduction Catalysts	p. 3
Fuel Oxidation Catalysts	p. 13
Molecular Catalysts for Artificial Photosynthetic Reaction	p. 17
Water Oxidation Catalyst	p. 18
Reduction Catalyst	p. 18
Photodevices for Photoinduced Chemical Reaction in the Water Phase	p. 25
Summary	p. 29
References	p. 30
Charge Transport in Molecular Catalysis in a Heterogeneous Phase	p. 37
Introduction	p. 37
Charge Transport (CT) by Molecules in a Heterogeneous Phase	p. 38
General Overview	p. 38
Mechanism of Charge Transport	p. 39
Charge Transfer by Molecules Under Photoexcited State in a Heterogeneous Phase	p. 46
Overview	p. 46
Mechanism of Charge Transfer at Photoexcited State in a Heterogeneous Phase	p. 47
Charge Transfer and Electrochemical Reactions in Metal Complexes	p. 50
Charge Transfer in Metal Complexes	p. 50
Charge Transfer at Electrode Surfaces	p. 53
Oxygen Reduction Reaction at Metal Macrocycles	p. 55
Proton Transport in Polymer Electrolytes	p. 59
Proton Transfer Reactions	p. 59
Proton Transport in Polymer Electrolytes	p. 60
Summary	p. 62
References	p. 63
Electrochemical Methods for Catalyst Evaluation in Fuel Cells and Solar Cells	p. 67
Introduction	p. 67
Electrochemical Measuring System for Catalyst Research in Fuel Cells	p. 68
Reference Electrode	p. 68
Rotating Ring-Disk Electrode	p. 69
Gas Electrodes of Half-Cell Configuration	p. 74
Fuel Cell Test Station	p. 76
Electrochemical Methods for Electrocatalysts	p. 79
Electrochemical Measuring System for Heterogeneous Charge Transport and Solar Cells	p. 86
Testing Method of Charge Transport in Heterogeneous Systems	p. 86
Evaluation of Charge Transport by Redox Molecules Incorporated in a Heterogeneous Phase	p. 88
AC Impedance Spectroscopy to Evaluate Charge Transport, Conductivity, Double-Layer Capacitance, and Electrode Reaction	p. 89
I-V Characteristics of Solar Cells	p. 93
Impedance Spectroscopy to Evaluate Multistep Charge Transport of a Dye-Sensitized Solar Cell	p. 94
Summary	p. 97
References	p. 101
Molecular Catalysts for Fuel Cell Anodes	p. 103
Introduction	p. 103
Concept of Composite Electrocatalysts in Fuel Cells	p. 105
Methanol Oxidation Reaction	p. 107
Mechanism of Methanol Oxidation Reaction	p. 107
New Electrocatalysts for Methanol Oxidation Reaction	p. 108
Structure of Composite Catalysts	p. 112
Formic Acid Oxidation Reaction	p. 118
Mechanism of Formic Acid Oxidation	p. 118
Formic Acid Oxidation on Composite Catalysts	p. 119
CO-Tolerant Electrocatalysts for Hydrogen Oxidation Reaction	p. 123
Electrochemical and Fuel Cell Testing	p. 123
Durability Testing	p. 127
Structural Characterization	p. 127
Summary	p. 134
References	p. 134
Macrocycles for Fuel Cell Cathodes	p. 139
Introduction	p. 139
Molecular Design of Macrocycles for Fuel Cell Cathodes	p. 141
Diporphyrin Cobalt Complexes and Related Catalysts	p. 142
Diporphyrin Cobalt Complexes	p. 142
Polypyrrole Cobalt Complexes	p. 144
Cobalt Thienylporphyrins	p. 149
Porphyrin Assemblies Based on Intermolecular Interaction	p. 153
Multinuclear Complexes as Electron Reservoirs	p. 158
Summary	p. 159
References	p. 160
Platinum-Free Catalysts for Fuel Cell Cathode	p. 163
Introduction	p. 163
Drawbacks of Using Pt as Catalysts in PEFC	p. 164
Mechanistic Aspects of Oxygen Reduction by Cathode Catalyst	p. 165
Platinum-Free Catalysts for Fuel Cell Cathode	p. 166
Metal Particles	p. 167
Metal Oxides, Carbides, Nitrides, and Chalcogenides	p. 168
Carbon Materials	p. 171
Metal Complex-Based Catalysts	p. 172
Catalysts Designed from Dinuclear Metal Complexes	p. 177
Summary	p. 180
References	p. 181
Novel Support Materials for Fuel Cell Catalysts	p. 185
Introduction	p. 185
Performance of Electrocatalysts Using Carbon Nanotubes	p. 187
<$>H_2 -O_2<$> Fuel Cell	p. 187
DMFC	p. 191
Why Is Carbon Nanotube So Effective as Support Material?	p. 194
References	p. 197
Molecular Catalysts for Electrochemical Solar Cells and Artificial Photosynthesis	p. 199
Introduction	p. 199
Overview on Principles of Molecule-Based Solar Cells	p. 200
Photon Absorption	p. 201
Suppression of Charge Recombination to Achieve Effective Charge Separation	p. 201
Diffusion of Separated Charges	p. 202
Electrode Reaction	p. 202
Dye-Sensitized Solar Cell (DSSC)	p. 202
Artificial Photosynthesis	p. 208
Dark Catalysis for Artificial Photosynthesis	p. 211
Dark Catalysis for Water Oxidation	p. 212
Dark Catalysis for Proton Reduction	p. 213
Conclusion and Future Scopes	p. 213
References	p. 214
Molecular Design of Sensitizers for Dye-Sensitized Solar Cells	p. 217
Introduction	p. 217
Metal-Complex Sensitizers	p. 219
Molecular Structures of Ru-Complex Sensitizers	p. 219
Electron-Transfer Processes	p. 224
Performance of DSSCs Based on Ru Complexes	p. 226
Other Metal-Complex Sensitizers for DSSCs	p. 229
Porphyrins and Phthalocyanines	p. 230
Organic Dyes	p. 231
Molecular Structures of Organic-Dye Sensitizers for DSSCs	p. 231
Performance of DSSCs Based on Organic Dyes	p. 236
Electron Transfer from Organic Dyes to TiO₂	p. 237
Electron Diffusion Length	p. 240
Stability	p. 242
Photochemical and Thermal Stability of Sensitizers	p. 242
Long-Term Stability of Solar-Cell Performance	p. 243
Summary and Perspectives	p. 244
References	p. 245
Fabrication of Charge Carrier Paths for High Efficiency Cells	p. 251
Introduction	p. 251
Fabrication of Electron-Paths	p. 252
Suppression of Black-Dye Aggregation in a Pressurized CO₂ Atmosphere	p. 255
Two-Layer TiO₂ Structure for Efficient Light Harvesting	p. 256
TCO-Less All-Metal Electrode-Type DSC	p. 257
Ion-Path in Quasi-Solid Medium	p. 257
Summary	p. 260
References	p. 260
Environmental Cleaning by Molecular Photocatalysts	p. 263
Introduction	p. 263
Oxidative Methods for the Photodegradation of Pollutants in Wastewater	p. 264
Comparison of Different Methods of UV Processes for Water Cleaning	p. 264
Photodegradation of Pollutants with Oxygen in the Visible Region of Light	p. 268
Visible Light Decomposition of Ammonia to Nitrogen with Ru(bpy)₃²⁺ as Sensitizer	p. 287
Nitrogen Pollutants and Their Photodecomposition	p. 287
Photochemical Electron Relay with Ammonia	p. 287
Photochemical Decomposition of Ammonia to Dinitrogen by a Photosensitized Electron Relay	p. 290
Visible Light Responsive Organic Semiconductors as Photocatalysts	p. 291
Photoelectrochemical Character of Organic Semiconductors in Water Phase	p. 291
Photoelectrochemical Oxidations by Irradiation with Visible Light	p. 292
Photochemical Decomposition of Amines Using Visible Light and Organic Semiconductors	p. 293
References	p. 294
Optical Oxygen Sensor	p. 299
Introduction	p. 300
Theoretical Aspect of Optical Oxygen Sensor of Porphyrins	p. 300
Advantage of Optical Oxygen Sensing	p. 300
Principle of Optical Oxygen Sensor	p. 301
Brief History of Optical Oxygen Sensors	p. 303
Optical Oxygen Sensor by Phosphorescence Intensity	p. 304
Phosphorescent Compounds	p. 304
Immobilization of Phosphorescent Molecules for Optical Oxygen Sensor and Measurement System	p. 304
Optical Oxygen Sensor with Platinum Octaethylporphyrin Polystyrene Film (PtOEP-PS Film)	p. 307
Optical Oxygen Sensor with PtOEP and Supports	p. 309
Application of Optical Oxygen Sensor for Air Pressure Measurements	p. 311
Optical Oxygen Sensor by Phosphorescence Lifetime Measurements	p. 313
Advantages of Phosphorescence Lifetime Measurement	p. 313
Phosphorescence Lifetime Measurement	p. 314
Distribution of Oxygen Concentration Inside Single Living Cell by Phosphorescence Lifetime Measurement	p. 315
Optical Oxygen Sensor T-T Absorption	p. 318
Advantage of Optical Oxygen Sensor Based on T-T Absorption	p. 320
Optical Oxygen Sensor Based on the Photoexcited Triplet Lifetime Measurement	p. 320
Optical Oxygen Sensor Based on Stationary T-T Absorption (Stationary Quenching)	p. 325
Summary	p. 327
References	p. 327
Adsorption and Electrode Processes	p. 329
Introduction	p. 329
Adsorption Isotherms and Kinetics	p. 330
Langmuir Isotherms	p. 330
Freundlich Isotherm	p. 332
Temkin Isotherm	p. 332
Application for Selective Reaction on Metal Surface by Adsorbate	p. 334
Slab Optical Waveguide Spectroscopy	p. 339
Principle	p. 340
Application of Slab Optical Waveguide Spectroscopy	p. 342
Methods of Digital Simulation for Electrochemical Measurements	p. 344
Formulation of Electrochemical System	p. 344
Finite Differential Methods	p. 351
Digital Simulation for Polymer-Coated Electrodes	p. 354
Hydrostatic Condition	p. 355
Hydrodynamic Condition	p. 357
Classical Monte Carlo Simulation for Charge Propagation in Redox Polymer	p. 358
Visualization of Charge Propagation	p. 359
Determination of a Charge Hopping Distance	p. 361
References	p. 363
Spectroscopic Studies of Molecular Processeson Electrocatalysts	p. 367
Introduction	p. 367
The Preparation and Spectroscopic Characterization of Fuel Cell Catalysts	p. 369
Catalyst Preparation by Electroless Plating and Direct Hydrogen Reduction Methods: Practical Application for High Performance PEFC	p. 369
In Situ IRAS Studies of Methanol Oxidation on Fuel Cell Catalysts	p. 377
Spectroscopic Studies of Methanol Oxidation on Pt Surfaces	p. 382
Electrooxidation of Methanol on Pt(111) in Acid Solutions: Effects of Electrolyte Anions during Electrocatalytic Reactions	p. 382
Methanol Oxidation Mechanisms on Pt(111) Surfaces	p. 388
Conclusions	p. 392
References	p. 393
Strategies for Structural and Energy Calculation of Molecular Catalysts	p. 395
Introduction	p. 395
Computational Methods	p. 396
Basis Set and Electron Correlation Effects on Geometry and Conformational Energy	p. 397
Intermolecular Forces	p. 397
Basis and Electron Correlation Effects on Intermolecular Interactions	p. 398
Calculations of Transition Metal Complexes	p. 402
Examples of the Ab Initio Calculation for Molecular Catalysts	p. 402
Summary	p. 409
References	p. 409
Future Technologies on Molecular Catalysts	p. 411
Introduction	p. 411
Road Map for Clean Energy Society	p. 412
Hydrogen Production	p. 415
Natural Gas	p. 415
Renewable Energy Source	p. 415
Biomass	p. 417
Hydrogen Utilization	p. 418
Hydrogen Storage	p. 419
Energy Conversion	p. 419
Biomimetic Approach and Role of Molecular Catalysts for Energy-Efficient Utilization	p. 420
Summary	p. 421
References	p. 422
Index	p. 423
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Molecular Catalysts for Energy Conversion

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