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NHC‐Containing Manganese(I) Electrocatalysts for the Two‐Electron Reduction of CO2
Authors:Dr Jay Agarwal  Travis W Shaw  Charles J Stanton III  Prof?Dr George F Majetich  Prof?Dr Andrew B Bocarsly  Prof?Dr Henry F Schaefer III
Institution:1. Center for Computational Quantum Chemistry, University of Georgia (USA);2. Department of Chemistry, Princeton University (USA);3. Department of Chemistry, University of Georgia (USA)
Abstract:The synthesis and characterization of the first catalytic manganese N‐heterocyclic carbene complexes are reported: MnBr(N‐methyl‐N′‐2‐pyridylbenzimidazol‐2‐ylidine)(CO)3 and MnBr(N‐methyl‐N′‐2‐pyridylimidazol‐2‐ylidine)(CO)3. Both new species mediate the reduction of CO2 to CO following two‐electron reduction of the MnI center, as observed with preparative scale electrolysis and verified with 13CO2. The two‐electron reduction of these species occurs at a single potential, rather than in two sequential steps separated by hundreds of millivolts, as is the case for previously reported MnBr(2,2′‐bipyridine)(CO)3. Catalytic current enhancement is observed at voltages similar to MnBr(2,2′‐bipyridine)(CO)3.
Keywords:carbon dioxide  catalysis  electrochemistry  manganese  N‐heterocyclic carbenes
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