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J Am Chem Soc. 2010 Feb 10;132(5):1545-57. doi: 10.1021/ja904906v.

Mechanism of water oxidation by single-site ruthenium complex catalysts.

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  • 1Department of Chemistry, University of North Carolina at Chapel Hill, Chapel Hill, North Carolina 27599, USA.


The mechanism of Ce(IV) water oxidation catalyzed by [Ru(tpy)(bpm)(OH(2))](2+) (tpy = 2,2':6',2''-terpyridine; bpm = 2,2'-bipyrimidine) and related single-site catalysts has been determined by a combination of mixing and stopped-flow experiments with spectrophotometric monitoring. The mechanism features O---O coupling by water attack on Ru(V)=O(3+) and three peroxidic intermediates that have been characterized by a combination of spectroscopy and DFT calculations.

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