Mechanism of water oxidation by single-site ruthenium complex catalysts

Javier J. Concepcion; Ming Kang Tsai; James T. Muckerman; Thomas J. Meyer

doi:10.1021/ja904906v

Mechanism of water oxidation by single-site ruthenium complex catalysts

Javier J. Concepcion, Ming Kang Tsai, James T. Muckerman, Thomas J. Meyer

Research output: Contribution to journal › Article › peer-review

432 Citations (Scopus)

Abstract

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^VdO³⁺ and three peroxidic intermediates that have been characterized by a combination of spectroscopy and DFT calculations.

Original language	English
Pages (from-to)	1545-1557
Number of pages	13
Journal	Journal of the American Chemical Society
Volume	132
Issue number	5
DOIs	https://doi.org/10.1021/ja904906v
Publication status	Published - 2010 Feb 10
Externally published	Yes

ASJC Scopus subject areas

Catalysis
General Chemistry
Biochemistry
Colloid and Surface Chemistry

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10.1021/ja904906v

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abstract = "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 RuVdO3+ and three peroxidic intermediates that have been characterized by a combination of spectroscopy and DFT calculations.",

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AU - Tsai, Ming Kang

AU - Muckerman, James T.

AU - Meyer, Thomas J.

PY - 2010/2/10

Y1 - 2010/2/10

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AB - 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 RuVdO3+ and three peroxidic intermediates that have been characterized by a combination of spectroscopy and DFT calculations.

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Mechanism of water oxidation by single-site ruthenium complex catalysts

Abstract

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