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Published on: April 22, 2016
Highly Active Ruthenium CNC Pincer Photocatalysts for Visible-Light-Driven Carbon Dioxide Reduction
Sanjit Das1, Roberta R Rodrigues2, Robert W Lamb3
1Department of Chemistry and Biochemistry , University of Alabama , Shelby Hall , Tuscaloosa , Alabama 35487 , United States.
Abstract:
Five ruthenium catalysts described herein facilitate self-sensitized carbon dioxide reduction to form carbon monoxide with a ruthenium catalytic center. These catalysts include four new and one previously reported CNC pincer complexes featuring a pyridinol derived N-donor and N-heterocyclic carbene (NHC) C-donors derived from imidazole or benzimidazole. The complexes have been characterized fully by spectroscopic and analytic methods, including X-ray crystallography. Introduction of a 2,2'-bipyridine (bipy) coligand and phenyl groups on the NHC ligand was necessary for rapid catalysis. [(CNC)Ru(bipy)(CH3CN)](OTf)2 is among the most active and durable photocatalysts in the literature for CO2 reduction without an external photosensitizer. The role of the structure of this complex in catalysis is discussed, including the importance of the pincer's phenyl wingtips, the bipyridyl ligand, and a weakly coordinating monodentate ligand.
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