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Science. 2010 Apr 16;328(5976):342-5. doi: 10.1126/science.1185372. Epub 2010 Mar 11.

A fast soluble carbon-free molecular water oxidation catalyst based on abundant metals.

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1
Department of Chemistry, Emory University, Atlanta, GA 30322, USA.

Abstract

Traditional homogeneous water oxidation catalysts are plagued by instability under the reaction conditions. We report that the complex [Co4(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 O2 production > or = 5 s(-1) at pH = 8. The rate's pH sensitivity reflects the pH dependence of the four-electron O2-H2O couple. Extensive spectroscopic, electrochemical, and inhibition studies firmly indicate that [Co4(H2O)2(PW9O34)2]10- is stable under catalytic turnover conditions: Neither hydrated cobalt ions nor cobalt hydroxide/oxide particles form in situ.

PMID:
20223949
DOI:
10.1126/science.1185372
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