Molecular water oxidation catalysis: a key topic for new sustainable energy conversion schemes (Chichester, 2014). - ОГЛАВЛЕНИЕ / CONTENTS

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ОбложкаMolecular water oxidation catalysis: a key topic for new sustainable energy conversion schemes / ed. A.Llobet. - Chichester: Wiley, 2014. - xiii, 265 p.: ill. - Bibliogr. at the end of the chapters. - Ind.: p.257-265. - ISBN 978-1-118-41337-1
 

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Оглавление / Contents
 
List of Contributors ........................................... xi
Preface ........................................................ xv

1  Structural Studies of Oxomanganese Complexes for
   Water Oxidation Catalysis .................................... 1
   Ivan Rivaita, Gary W. Brudvig, and Victor S. Batista
   1.1  Introduction ............................................ 1
   1.2  Structural Studies of the OEC ........................... 2
   1.3  The Dark-Stable State of the OEC ........................ 4
   1.4  Biomimetic Oxomanganese Complexes ....................... 6
   1.5  Base-Assisted O-O Bond Formation ........................ 7
   1.6  Biomimetic Mn Catalysts for Artificial Photosynthesis ... 8
   1.7  Conclusion ............................................. 11
   Acknowledgments ............................................. 12
   References .................................................. 12
2  O-O Bond Formation by a Heme Protein: The Unexpected
   Efficiency of Chlorite Dismutase ............................ 15
   Jennifer L. DuBois
   2.1  Introduction ........................................... 15
   2.2  Origins of O2-Evolving Chlorite Dismutases (Clds) ...... 15
   2.3  Major Structural Features of the Proteins and their 
        Active Sites ........................................... 16
   2.4  Efficiency, Specificity, and Stability ................. 20
   2.5  Mechanistic Insights from Surrogate Reactions with 
        Peracids and Peroxide .................................. 22
   2.6  Possible Mechanisms .................................... 23
   2.7  Conclusion ............................................. 25
   Acknowledgements ............................................ 25
   References .................................................. 25
3  Ru-Based Water Oxidation Catalysts .......................... 29
   Laia Francàs, Roger Bofill, Jordi García-Antón, Lluis 
   Escriche, Xavier Sala and Antoni Llobet
   3.1  Introduction ........................................... 29
   3.2  Proton-Coupled Electron Transfer (PCET) and Water 
        Oxidation Thermodynamics ............................... 31
   3.3  O-O Bond Formation Mechanisms .......................... 33
   3.4  Polynuclear Ru Water Oxidation Catalysts ............... 34
   3.5  Mononuclear Ru WOCs .................................... 40
   3.6  Anchored Molecular Ru WOCs ............................. 42
   3.7  Light-Induced Ru WOCs .................................. 43
   3.8  Conclusion ............................................. 45
   Acknowledgments ............................................. 46
   References .................................................. 46
4  Towards the Visible Light-Driven Water Splitting Device:
   Ruthenium Water Oxidation Catalysts with Carboxylate-
   Containing Ligands .......................................... 51
   Lele Duan, Lianpeng Tong, and Licheng Sun
   4.1  Introduction ........................................... 51
   4.2  Binuclear Ru Complexes ................................. 52
   4.3  Mononuclear Ru Complexes ............................... 54
        4.3.1  Ru-O2N-N3 Analogs ............................... 55
        4.3.2  Ru-O2N2-N2 Analogs .............................. 57
   4.4  Homogeneous Light-Driven Water Oxidation ............... 68
        4.4.1  The Three-Component System ...................... 68
        4.4.2  The Supramolecular Assembly Approach ............ 69
   4.5  Water Oxidation Device ................................. 72
        4.5.1  Electrochemical Water Oxidation Anode ........... 72
        4.5.2  Photo-Anode for Water Oxidation ................. 74
   4.6  Conclusion ............................................. 75
   References .................................................. 75
   
5  Water Oxidation by Ruthenium Catalysts with Non-Innocent
   Ligands ..................................................... 77
   Tohru Wada, Koji Tanaka, James T. Muckerman, and Etsuko
   Fujita
   5.1  Introduction ........................................... 77
   5.2  Water Oxidation Catalyzed by Dinuclear Ruthenium 
        Complexes with NILs .................................... 81
   5.3  Water Oxidation by Intramolecular O-O Coupling with
        [Ru2II(μ-Cl)(bpy)2(btpyan)]3+ .......................... 85
   5.4  Mononuclear Ru-Aqua Complexes with a Dioxolene Ligand .. 91
        5.4.1  Structural Characterization ..................... 91
        5.4.2  Theoretical and Electrochemical
               Characterization ................................ 96
   5.5  Mechanistic Investigation of Water Oxidation by
        Dinuclear Ru Complexes with NILs: Characterization
        of Key Intermediates .................................. 101
   References ................................................. 107

6  Recent Advances in the Field of Iridium-Catalyzed 
   Molecular Water Oxidation .................................. 113
   James A. Woods, Stefan Bernhard, and Martin Albrecht
   6.1  Introduction .......................................... 113
   6.2  Bernhard 2008 [11] .................................... 114
   6.3  Crabtree 2009 ......................................... 115
   6.4  Crabtree 2010 ......................................... 116
   6.5  Macchioni 2010 ........................................ 117
   6.6  Albrecht/Bernhard 2010 ................................ 117
   6.7  Hetterscheid/Reek 2011 ................................ 118
   6.8  Crabtree2011 .......................................... 119
   6.9  Crabtree2011 .......................................... 120
   6.10 Lin 2011 .............................................. 120
   6.11 Macchioni 2011 ........................................ 122
   6.12 Grotjahn2011 .......................................... 123
   6.13 Fukuzumi2011 .......................................... 123
   6.14 Lin 2012 .............................................. 124
   6.15 Crabtree 2012 ......................................... 125
   6.16 Albrecht/Bernhard 2012 ................................ 125
   6.17 Crabtree 2012 ......................................... 126
   6.18 Beller 2012 ........................................... 127
   6.19 Lin 2012 .............................................. 128
   6.20 Lloblet and Macchioni 2012 ............................ 129
   6.21 Analysis .............................................. 130
   References ................................................. 131
   
7  Complexes of First Row d-Block Metals: Manganese ........... 135
   Philipp Kurz
   7.1  Background ............................................ 135
   7.2  Oxidation States of Manganese in an Aqueous 
        Environment ........................................... 137
   7.3  Dinuclear Manganese Complexes: Syntheses and
        Structures ............................................ 138
   7.4  Redox and Acid-Base Chemistry of Mn2-μ-WDL Systems .... 139
   7.5  Mn2 Systems: Oxygen Evolution (but not Water 
        Oxidation) Catalysis .................................. 142
   7.6  Mn2 Complexes/the OEC/Ru2 Catalysts: A Comparison ..... 144
   7.7  Heterogeneous Water Oxidation Catalysis by Mn>2
        Systems ............................................... 146
   7.8  Conclusion ............................................ 148
   Acknowledgements ........................................... 148
   References ................................................. 149
   
8  Molecular Water Oxidation Catalysts from Iron .............. 153
   W. Chadwick Ellis, Neal D. McDaniel, and Stefan Bernhard
   8.1  Introduction .......................................... 153
   8.2  Fe-Tetrasulfophthalocyanine ........................... 154
   8.3  Fe-TAML ............................................... 155
   8.4  Fe-mcp ................................................ 157
   8.5  Fe2O3 as a Microheterogeneous Catalyst ................ 158
   8.6  Conclusion ............................................ 160
   References ................................................. 161

9  Water Oxidation by Co-Based Oxides with Molecular
   Properties ................................................. 163
   Marcel Risch, Katharina Klingan, Ivelina Zaharieva, and
   Holger Dau
   9.1  Introduction .......................................... 163
   9.2  CoCat Formation ....................................... 164
   9.3  Structure and Structure-Function Relations ............ 166
   9.4  Functional Characterization ........................... 173
   9.5  Directly Light-Driven Water Oxidation ................. 175
   References ................................................. 180

10 Developing Molecular Copper Complexes for Water 
   Oxidation .................................................. 187
   Shoshanna M. Barnett, Christopher R. Waidmann, 
   Margaret L. Scheuermann, Jared C. Nesvet, Karen 
   Goldberg and James M. Mayer
   10.1 Introduction .......................................... 187
   10.2 A Biomimetic Approach ................................. 188
        10.2.1 Thermochemistry: Developing Oxidant/Base 
               Combinations as PCET Reagents .................. 189
        10.2.2 Copper Complexes with Alkylamine Ligands ....... 190
        10.2.3 Copper Complexes with Anionic Ligands .......... 195
        10.2.4 Lessons Learned: Thermochemical Insights 
               and Oxidant/Base Compatibility ................. 198
   10.3 An Aqueous System: Electrocatalysis with
        (bpy)Cu(II) Complexes ................................. 198
        10.3.1 System Selection: bpy + Cu ..................... 199
        10.3.2 Observing Electrocatalysis ..................... 199
        10.3.3 Catalyst Turnover Number and Turnover
               Frequency ...................................... 201
        10.3.4 Catalyst Speciation: Monomer, Dimer, or
               Nanoparticles? ................................. 203
   10.4 Conclusion ............................................ 206
   Acknowledgement ............................................ 206
   References ................................................. 207
11 Polyoxometalate Water Oxidation Catalytic Systems .......... 211
   Jordan M. Sumliner, James W. Wickers, Hongjin Lv, 
   Yurii V. Geletii, and Craig L. Hill
   11.1 Introduction .......................................... 211
   11.2 Recent POM WOCs ....................................... 214
   11.3 Assessing POM WOC Reactivity .......................... 220
   11.4 The Ru(bpy)32+/S2O82- System .......................... 221
   11.5 Ru(bpy)33+ as an Oxidant for POM WOCs ................. 222
   11.6 Additional Aspects of WOC System Stability ............ 224
   11.7 Techniques for Assessing POM WOC Stability ............ 224
   11.8 Conclusion ............................................ 227
   Acknowledgments ............................................ 228
   References ................................................. 228
12 Quantum Chemical Characterization of Water Oxidation 
   Catalysts .................................................. 233
   Pere Miró, Mehmed Z. Ertem, Laura Gagliardi, and
   Christopher J. Cramer
   12.1 Introduction .......................................... 233
   12.2 Computational Details ................................. 235
        12.2.1 Density Functional Theory Calculations ......... 235
        12.2.2 Multiconfigurational Calculations .............. 236
   12.3 Methodology ........................................... 237
        12.3.1 Solvation and Standard Reduction Potentials .... 237
        12.3.2 Multideterminantal State Energies .............. 238
   12.4 Water Oxidation Catalysts ............................. 238
        12.4.1 Ruthenium-Based Catalysts ...................... 238
        12.4.2 Cobalt-Based Catalysts ......................... 245
        12.4.3 Iron-Based Catalysts ........................... 248
   12.5 Conclusion ............................................ 251
   References ................................................. 252
   
Index ......................................................... 257


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