Electrogenerated polypyridyl ruthenium hydride and ligand activation for water reduction to hydrogen and acetone to iso-propanol

Chen, Zuofeng, Glasson, Christopher R.K., Holland, Patrick L., and Meyer, Thomas J. (2013) Electrogenerated polypyridyl ruthenium hydride and ligand activation for water reduction to hydrogen and acetone to iso-propanol. Physical Chemistry Chemical Physics, 15. pp. 9503-9507.

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Abstract

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 104 compared to water. The reactivity of the in situ electrogenerated hydride toward hydride transfer is promoted by ligand reduction.

Item ID: 33465
Item Type: Article (Research - C1)
ISSN: 1463-9084
Funders: US Department of Energy (DOE), Army Research Office (ARO)
Projects and Grants: DOE Award DE-SC0001011, ARO Grant W911NF-09-1- 0426, DOE DE-FG02-09ER161
Date Deposited: 29 May 2014 01:29
FoR Codes: 03 CHEMICAL SCIENCES > 0302 Inorganic Chemistry > 030207 Transition Metal Chemistry @ 50%
03 CHEMICAL SCIENCES > 0305 Organic Chemistry > 030503 Organic Chemical Synthesis @ 50%
SEO Codes: 85 ENERGY > 8505 Renewable Energy > 850504 Solar-Photovoltaic Energy @ 50%
97 EXPANDING KNOWLEDGE > 970103 Expanding Knowledge in the Chemical Sciences @ 50%
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