Journal
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
Volume 136, Issue 41, Pages 14598-14607Publisher
AMER CHEMICAL SOC
DOI: 10.1021/ja5085282
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- AFOSR through a Basic Research Initiative (BRI) grant [FA9550-12-1-0414]
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The addition of methyl acetamidomethyl groups at the 4,4'-positions of a 2,2'-bipyridyl ligand is found to enhance the rate of a bimolecular reduction mechanism of CO2 by Re(II)fac-tricarbonyl chloride complexes. Electrochemical studies, spectroelectrochemical measurements, and molecular dynamics simulations indicate that these methyl acetamidomethyl groups promote the formation of a hydrogen-bonded dimer. This supramolecular complex catalyzes the reductive disproportionation of CO2 to CO and CO32- at a lower overpotential (ca. 250 mV) than the corresponding single-site 2 e- reduction of CO2 to CO and H2O catalyzed by the corresponding model complex with a 4,4'-dimethyl-2,2'-bipyridyl ligand. These findings demonstrate that noncovalent self-assembly can modulate the catalytic properties of metal complexes by favoring alternate catalytic pathways.
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