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      Splitting Water with Cobalt

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      Angewandte Chemie International Edition

      Wiley-Blackwell

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          Ru(II) polypyridine complexes: photophysics, photochemistry, eletrochemistry, and chemiluminescence

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

            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.
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              The Mechanism of Water Oxidation: From Electrolysis via Homogeneous to Biological Catalysis

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                Author and article information

                Journal
                Angewandte Chemie International Edition
                Angew. Chem. Int. Ed.
                Wiley-Blackwell
                14337851
                August 01 2011
                August 01 2011
                : 50
                : 32
                : 7238-7266
                Article
                10.1002/anie.201007987
                © 2011
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