Activating a Low Overpotential CO2 Reduction Mechanism by a Strategic Ligand Modification on a Ruthenium Polypyridyl Catalyst |
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Authors: | Ben A. Johnson Dr. Somnath Maji Dr. Hemlata Agarwala Dr. Travis A. White Dr. Edgar Mijangos Prof. Dr. Sascha Ott |
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Affiliation: | Department of Chemistry, ?ngstr?m Laboratory, Uppsala University, Uppsala, Sweden |
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Abstract: | The introduction of a simple methyl substituent on the bipyridine ligand of [Ru(tBu3tpy)(bpy)(NCCH3)]2+ (tBu3tpy=4,4′,4′′‐tri‐tert‐butyl‐2,2′:6′,2′′‐terpyridine; bpy=2,2′‐bipyridine) gives rise to a highly active electrocatalyst for the reduction of CO2 to CO. The methyl group enables CO2 binding already at the one‐electron reduced state of the complex to enter a previously not accessible catalytic cycle that operates at the potential of the first reduction. The complex turns over with a Faradaic efficiency close to unity and at an overpotential that is amongst the lowest ever reported for homogenous CO2 reduction catalysts. |
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Keywords: | carbon dioxide reduction electrocatalysis overpotential reaction mechanisms ruthenium |
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