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Application of the Marcus Cross Relation to Hydrogen Atom Transfer/Proton-Coupled Electron Transfer Reactions | p. 1 |
Introduction | p. 1 |
An Introduction to Marcus Theory | p. 2 |
Predicting Organic Hydrogen Atom Transfer Rate Constants | p. 5 |
Obtaining Self-Exchange Rate Constants and Equilibrium Constants | p. 6 |
Tests of the Cross Relation for Organic HAT Reactions | p. 7 |
Solvent Effects on HAT Rate and Equilibrium Constants | p. 11 |
A Test Case: Reactions of Bulky Phenoxyl Radicals with TEMPOH | p. 12 |
Tests of the Cross Relation using KSE-Corrected Self-Exchange Rate Constants | p. 13 |
Predicting HAT Rate Constants for Transition Metal Complexes | p. 14 |
Applying the Cross Relation as a Function of Temperature; the Importance of Using Free Energies | p. 16 |
Applying the Cross Relation to Oxidations by [RuIV(O)(bpy)2(py)]2+ | p. 17 |
Precursor and Successor Complexes for HAT | p. 18 |
Applying the Cross Relation for Transition Metal HAT | p. 20 |
Transition Metal Systems that Deviate from the Cross Relation | p. 21 |
Conclusions: Implications and Limitations of the Cross Relation for Hydrogen Atom Transfer Reactions | p. 23 |
References | p. 27 |
A Transition-State Perspective of Proton-Coupled Electron Transfers | p. 32 |
Introduction | p. 32 |
Theory | p. 34 |
Hydrogen Atom Transfers | p. 34 |
Proton Transfers in Hydrogen-Bonded Systems | p. 37 |
Electron Transfers | p. 40 |
Concerted Proton-Electron Transfers | p. 47 |
Applications | p. 48 |
HAT in the Benzyl/Toluene Self-Exchange | p. 48 |
PCET in the Phenoxyl/Phenol Self-Exchange | p. 50 |
CPET in Soybean Lipoxygenase-1 | p. 52 |
Conclusions | p. 53 |
References | p. 54 |
Experimental Approaches Towards Proton-Coupled Electron Transfer Reactions in Biological Redox Systems | p. 57 |
Introduction | p. 57 |
Definitions | p. 57 |
Thermodynamics of PCET Reactions | p. 61 |
Kinetics of PCET Reactions | p. 64 |
Experimental Kinetic Approaches to Analyse PCET Reactions | p. 69 |
Case Studies | p. 73 |
PCET in Nitrite Reductase | p. 73 |
Hydride Transfer Reactions in Old Yellow Enzymes | p. 76 |
Concluding Remarks | p. 79 |
References | p. 79 |
Metal Ion-Coupled and Proton-Coupled Electron Transfer in Catalytic Reduction of Dioxygen | p. 89 |
Introduction | p. 89 |
PCET from Electron Donors to O2 | p. 91 |
MCET from Electron Donors to O2 | p. 97 |
MCET from O2•-Mn+ to p-Benzoquinones | p. 99 |
Catalytic Two-Electron Reduction of O2 via MCET and PCET | p. 103 |
Catalytic Four-Electron Reduction of O2 | p. 109 |
Cofacial Dicobalt Porphyrin and Porphyrin-Corrole Dyads | p. 109 |
Mononuclear Cu Complexes | p. 115 |
A Heterodinuclear Indium-Ruthenium Complex | p. 118 |
Mononuclear Mn Complexes | p. 119 |
Summary and Conclusions | p. 121 |
Acknowledgements | p. 121 |
References | p. 121 |
Proton-Coupled Electron Transfer in Natural and Artificial Photosynthesis | p. 126 |
Introduction | p. 126 |
Proton-Coupled Electron Transfer Reactions | p. 128 |
Interfacial PCET | p. 129 |
Thermodynamics of Water Splitting and CO2 Reduction | p. 130 |
Natural Photosynthesis | p. 132 |
Structure and Mechanism of Photosystem II | p. 133 |
PCET in Photosystem II | p. 136 |
Artificial Photosynthesis | p. 137 |
Model Systems for Photosystem II | p. 138 |
Water Oxidation Catalysts | p. 139 |
Proton and CO2 Reduction | p. 144 |
Concluding Remarks | p. 145 |
References | p. 145 |
Subject Index | p. 152 |
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