Mechanism of Water Oxidation by Single-Site Ruthenium Complex Catalysts

被引：416
|
作者：
Concepcion, Javier J. [1 ]
Tsai, Ming-Kang [2 ]
Muckerman, James T. [2 ]
Meyer, Thomas J. [1 ]
机构：
[1] Univ N Carolina, Dept Chem, Chapel Hill, NC 27599 USA
[2] Brookhaven Natl Lab, Dept Chem, Upton, NY 11973 USA
来源：
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY | 2010年 / 132卷 / 05期
关键词：
MOLECULAR-OXYGEN; IONIC-SOLUTIONS; PHOTOSYSTEM-II; DIOXYGEN; REACTIVITY; HYDROPEROXO; INSERTION; FAMILY; OSMIUM; REDOX;
D O I：
10.1021/ja904906v
中图分类号：
O6 [化学];
学科分类号：
0703 ;
摘要：
The mechanism of Ce(IV) water oxidation catalyzed by [Ru(tpy)(bpm)(OH2)](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=O3+ and three peroxidic intermediates that have been characterized by a combination of spectroscopy and DFT calculations.
引用
收藏
页码：1545 / 1557
页数：13
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