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

Authors
  • Chen, Zuofeng
  • Glasson, Christopher R K
  • Holland, Patrick L
  • Meyer, Thomas J
Type
Published Article
Journal
Physical Chemistry Chemical Physics
Publisher
The Royal Society of Chemistry
Publication Date
Jun 28, 2013
Volume
15
Issue
24
Pages
9503–9507
Identifiers
DOI: 10.1039/c3cp51946e
PMID: 23681418
Source
Medline
License
Unknown

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 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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