期刊
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
卷 15, 期 24, 页码 9503-9507出版社
ROYAL SOC CHEMISTRY
DOI: 10.1039/c3cp51946e
关键词
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资金
- UNC Energy Frontier Research Center (EFRC) for Solar Fuels, an EFRC
- U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences [DE-SC0001011]
- Army Research Office [W911NF-09-1-0426]
- Office of Basic Energy Sciences, U.S. Department of Energy [DE-FG02-09ER16121]
The complex [Ru(tpy)(bpy)(S)](2+) (tpy = 2,2':6',2 ''-terpyridine, bpy = 2,2'-bipyridine, S = solvent) is an electrocatalyst for water or proton reduction to hydrogen and for reduction of acetone to iso-propanol in CH3CN. Electrocatalysis is initiated by sequential 1e(-) reductions at the tpy and bpy ligands followed by addition of water to give a ruthenium hydride intermediate. Significant rate enhancements for hydrogen evolution are observed with added weak acids, such as H2PO4-, for the latter, with a rate enhancement of 10(4) compared to water. The reactivity of the in situ electrogenerated hydride toward hydride transfer is promoted by ligand reduction.
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