期刊
PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA
卷 105, 期 46, 页码 17632-17635出版社
NATL ACAD SCIENCES
DOI: 10.1073/pnas.0807153105
关键词
catalysis; redox mediator; electron transfer
资金
- The Chemical Sciences, Geosciences, and Biosciences Division of the Office of Basic Energy Sciences, US Department of Energy
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 (2H(2)O + 4 h nu -> O-2 + 2 H-2) or water reduction of CO2 to methanol (2 H2O + CO2 + 6 h nu -> CH3OH + 3/2 O-2), or hydrocarbons, which could provide clean, renewable energy. The blue ruthenium dimer, cis,cis-[(bpy)(2)(H2O)(RuORuIII)-O-III(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 approximate to 30 have been obtained, and preliminary electrochemical experiments have demonstrated that mediator-assisted electrocatalytic water oxidation is also attainable.
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