4.7 Article

Rapid catalytic water oxidation by a single site, Ru carbene catalyst

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DALTON TRANSACTIONS
卷 40, 期 15, 页码 3789-3792

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ROYAL SOC CHEMISTRY
DOI: 10.1039/c0dt01178a

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  1. Army Research Office [W911NF-09-1-0426]
  2. U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences [DE-SC0001011]

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Compared to earlier single site catalysts, greatly enhanced rates of electrocatalytic water oxidation by the Ru carbene catalyst [Ru(tpy)(Mebim-py)(OH2)](2+) (tpy = 2,2': 6',2 ''-terpyridine; Mebim-py = 3-methyl-1-pyridylbenzimidazol-2-ylidene) have been observed. The mechanism appears to be the same with proton coupled electron transfer (PCET) activation toRu(V)=O3+ followed by O-O coupling and further oxidation. An important factor in the enhanced reactivity of the carbene complex may come from increased driving force for the O-O bond forming step.

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