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Preface vii

1. Renewable Energy and the Hydrogen Economy 1

Krishnan Rajeshwar, Robert McConnell, Kevin Harrison, and Stuart Licht

1 Renewable Energy and the Terawatt Challenge 1

2 Hydrogen as a Fuel of the Future 3

3 Solar Energy and the Hydrogen Economy 11

4 Water Splitting and Photosynthesis 12

5 Completing the Loop: Fuel Cells 14

6 Concluding Remarks 16

References 16

2. The Solar Resource 19

Daryl R. Myers

1 Introduction: Basic Properties of the Sun 19

2 The Spectral Distribution of the Sun as a Radiation Source 20

3 The Earth's Atmosphere as a Filter 22

4 Utilization of Solar Spectral Regions: Spectral Response of

Materials 25

5 Reference Spectral Distributions 32

6 Summary 38

References 38

3. Electrolysis of Water 41

Kevin Harrison and Johanna Ivy Levene

1 Introduction 41

2 Electrolysis of Water 43

2.1 Alkaline 44

2.2 Proton Exchange Membrane 45

3 Fundamentals of Water Electrolysis 50

3.1 First Principles 50

3.2 Overpotentials 52

4 Commercial Electrolyzer Technologies 54

5 Electrolysis System 55

5.1 Energy Efficiency 56

5.2 Electricity Costs 58

6 Opportunities for Renewable Energy 59

7 Conclusions 60

References 61

4. A Solar Concentrator Pathway to Low-Cost Electrolytic Hydrogen 65

Robert McConnell

1 Direct Conversion of Concentrated Sunlight to Electricity 65

2 The CPV Market 66

3 Higher and Higher Conversion Efficiencies 69

4 CPV Reliability 72

5 Following in Wind Energy's Footsteps 73

6 Low-Cost Hydrogen from Hybrid CPV Systems 75

7 Describing the Hybrid CPV System 76

8 Discussion 81

9 Hydrogen Vision Using Hybrid Solar Concentrators 82

10 Conclusions 83

Acknowledgements 84

References 84

5. Thermochemical and Thermal/Photo Hybrid Solar Water Splitting 87

Stuart Licht

1 Introduction to Solar Thermal Formation of Hydrogen 87

1.1 Comparison of Solar Electrochemical, Thermal & Hybrid

Water Splitting 87

2 Direct Solar Thermal Water Splitting to Generate Hydrogen Fuel 90

2.1 Development of Direct Solar Thermal Hydrogen 90

2.2 Theory of Direct Solar Thermal Hydrogen Generation 91

2.3 Direct Solar Thermal Hydrogen Processes 92

3 Indirect (Multi-step) Solar Thermal Water Splitting to Generate

Hydrogen Fuel 94

3. 1 Historical Development of Multi-Step Thermal Processes for Water Electrolysis 94

3.2 Comparison of Multi-step Indirect Solar Thermal

Hydrogen Processes 96

3.3 High-Temperature, Indirect-Solar Thermal Hydrogen

Processes 96

4 Hybrid Solar Thermal/Electrochemical/Photo (STEP) Water

Splitting 99

4.1 Historical Development of Hybrid Thermal Processes 99

4.2 Theory of Hybrid Solar Hydrogen Generation 99

4.3 Elevated Temperature Solar Hydrogen Processes and Components 111

5 Future Outlook and Concluding Remarks 116

References 116

6. Molecular Approaches to Photochemical Splitting of Water 123

Frederick M. MacDonnell

1 Scope 123

2 Fundamental Principles 124

3 Nature's Photosynthetic Machinery 125

4 Design of Artificial Photosystems 129

5 The Ideal Sensitizer: Does Rubpy Come Close? 133

5.1 Stability 133

5.2 Photophysics and Photochemistry 136

6 Supramolecular Assemblies: Dyads, Triads and Beyond 138

6.1 Energy Transfer Quenching: Antenna Complexes 138

6.2 Bichromophores: Increasing Excited-State Lifetimes 140

6.3 Reductive and Oxidative Quenching: Dyads and Triads with Donors and Acceptors 142

6.4 Single versus Multi-Electron Processes 145

7. OER and HER Co-Catalysts 150

7.1 Mimicking the Oxygen Evolving Center: Water Oxidation Catalysts 150

7.2 The Hydrogen Evolving Reaction (HER): Hydrogen

Evolution Catalysts 153

8. Future Outlook and Concluding Remarks 154

Acknowledgements 156

References 156

7. Hydrogen Generation from Irradiated Semiconductor-Liquid

Interfaces 167

Krishnan Rajeshwar

1 Introduction and Scope 167

2 Types of Approaches 170

3 More on Nomenclature and the Water Splitting Reaction Requirements 172

4 Efficiency of Photoelectrolysis 178

5 Theoretical Aspects 180

6 Oxide Semiconductors 183

6.1 Titanium Dioxide: Early Work 183

6.2 Studies on the Mechanistic Aspects of Processes at the TiÜ2-Solution Interface 186

6.3 Visible Light Sensitization of TiÜ2 186

6.4 Recent Work on TiÜ2 on Photosplitting of Water or on the Oxygen Evolution Reaction 187

6.5 Other Binary Oxides 190

6.6 Perovskite Titanates and Related Oxides 192

6.7 Tantalates and Niobates 197

6.8 Miscellaneous Multinary Oxides 198

7 Nitrides, Oxynitrides and Oxysulfides 200

8 Metal Chalcogenide Semiconductors 202

8.1 Cadmium Sulfide 202

8.2 Other Metal Chalcogenides 204

9 Group III-V Compound Semiconductors 205

10 Germanium and Silicon 206

11 Silver Halides 208

12 Semiconductor Alloys and Mixed Oxides 208

12.1 Semiconductor Composites 208

13 Photochemical Diodes and Twin-Photosystem Configurations for

Water Splitting 210

14 Other Miscellaneous Approaches and Hydrogen Generation from

Media Other than Water 211

15 Concluding Remarks 213

Acknowledgments 213

References 213

8. Photobiological Methods of Renewable Hydrogen Production 229

Maria L. Ghirardi, Pin Ching Maness, and Michael Seibert

1 Introduction 229

2 Green Algae 230

2.1 Mechanism of Hydrogen Production 230

2.2 Hydrogenase-Catalyzed H2 Production 233

2.3 [FeFe]-hydrogenases 234

3 Cyanobacteria 235

3.1 Mechanisms of Hydrogen Production 235

3.2 Hydrogenase-Catalyzed H2 Production 236

3.3 [NiFe] -Hydrogenases 238

3.4 Nitrogenase-Catalyzed H2 Production 240

3.5 Nitrogenases 241

4. Other Systems 242

4.1 Non-Oxygenic Purple, Non-Sulfur Photosynthetic Bacteria 242

4.2 Mixed Light/Dark Systems 243

4.3 Bio-Inspired Systems 244

5 Scientific and Technical Issues 245

5.1 General 245

5.2 Oxygen Sensitivity of [FeFe]-Hydrogenases 246

5.3 Oxygen Sensitivity of [NiFe]-Hydrogenases 248

5.4 Competition between Different Pathways for

Photosynthetic Reductants 249

5.5 Down-Regulation of Electron Transport Rates 250

5.6 Low-Light Saturation Properties of Photosynthetic

Organisms 251

5.7 Photobioreactor and System Costs 252

5.8 Genomics Approaches 254

6 Future Directions 254

Acknowledgments 255

References 255

9. Centralized Production of Hydrogen using a Coupled Water

Electrolyzer-Solar Photovoltaic System 273

James Mason and Ken Zweibel

1 Introduction 273

2 Description of a PV Electrolytic H2 Production and Distribution

System 274

3 Capital Investment and Levelized Price Estimates 281

4 Sensitivity Analysis: H2 Production and PV Electricity Prices 285

5 Economic Analysis of Second Generation (Year 31-Year 60) H2 Systems 289

6 Life Cycle Energy and GHG Emissions Analyses 294

6.1 Life Cycle Analysis Methods 294

6.2 Life Cycle Energy and GHG Emissions Analyses Results 296

7 System Energy Flow/Mass/Balance Analysis 296

8 Conclusions: Summary of Results and Suggestions for Future

Analysis 298

Appendices 305

1 Energy Units and CO2 Equivalent Emissions Estimates 305

2 Levelized Price Estimates Derived by Net Present Value

Cash Flow Analysis 305

3 Adiabatic Compression Formula 307

4 Deviations from DOE H2A Assumptions 308

5 Summary of Reviewer Comments with Responses 309

References 312

Index 315

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