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标题：Mediator-assisted water oxidation by the ruthenium “blue dimer” cis,cis-[(bpy)2(H2O)RuORu(OH2)(bpy)2]4+
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作者：Javier J. Concepcion ; Jonah W. Jurss ; Joseph L. Templeton 等
期刊名称：Proceedings of the National Academy of Sciences
印刷版ISSN：0027-8424
电子版ISSN：1091-6490
出版年度：2008
卷号：105
期号：46
页码：17632-17635
DOI：10.1073/pnas.0807153105
语种：English
出版社：The National Academy of Sciences of the United States of America
摘要：Light-driven water oxidation occurs in oxygenic photosynthesis in photosystem II and provides redox equivalents directed to photosystem I, in which carbon dioxide is reduced. Water oxidation is also essential in artificial photosynthesis and solar fuel-forming reactions, such as water splitting into hydrogen and oxygen (2 H2O + 4 h{nu} [->] O2 + 2 H2) or water reduction of CO2 to methanol (2 H2O + CO2 + 6 h{nu} [->] CH3OH + 3/2 O2), or hydrocarbons, which could provide clean, renewable energy. The "blue ruthenium dimer," cis,cis-[(bpy)2(H2O)RuIIIORuIII(OH2)(bpy)2]4+, was the first well characterized molecule to catalyze water oxidation. On the basis of recent insight into the mechanism, we have devised a strategy for enhancing catalytic rates by using kinetically facile electron-transfer mediators. Rate enhancements by factors of up to {approx}30 have been obtained, and preliminary electrochemical experiments have demonstrated that mediator-assisted electrocatalytic water oxidation is also attainable.
关键词：catalysis ; redox mediator ; electron transfer