Mechanism of Water Oxidation by Single-Site Ruthenium Complex Catalysts

作者：Concepcion Javier J; Tsai Ming Kang; Muckerman James T; Meyer Thomas J^*

来源：Journal of the American Chemical Society, 2010, 132(5): 1545-1557.

DOI：10.1021/ja904906v

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.

• 出版日期2010-2-10