期刊
SCIENCE
卷 328, 期 5976, 页码 342-345出版社
AMER ASSOC ADVANCEMENT SCIENCE
DOI: 10.1126/science.1185372
关键词
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资金
- U.S. Department of Energy [DE-FG02-03ER-15461]
- French Ministere de l'Education Nationale, de la Recherche, et de la Technologie
Traditional homogeneous water oxidation catalysts are plagued by instability under the reaction conditions. We report that the complex [Co-4(H2O)(2)(PW9O34)(2)](10-), comprising a Co4O4 core stabilized by oxidatively resistant polytungstate ligands, is a hydrolytically and oxidatively stable homogeneous water oxidation catalyst that self-assembles in water from salts of earth-abundant elements (Co, W, and P). With [Ru(bpy)(3)](3+) (bpy is 2,2'-bipyridine) as the oxidant, we observe catalytic turnover frequencies for O-2 production >= 5 s(-1) at pH = 8. The rate's pH sensitivity reflects the pH dependence of the four-electron O-2-H2O couple. Extensive spectroscopic, electrochemical, and inhibition studies firmly indicate that [Co-4(H2O)(2)(PW9O34)(2)](10-) is stable under catalytic turnover conditions: Neither hydrated cobalt ions nor cobalt hydroxide/oxide particles form in situ.
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