CO2 Reduction with High Bulk Turnover Numbers at Small Overpotentials by a fac-Mn(bpy)(CO)3L Complex with a Redox-Active, Electron Reservoir Ligand
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The electrocatalytic CO 2 reduction reaction (CRR) is required to convert CO 2 into useful commodity chemicals with renewable energy thereby reducing global greenhouse gas emissions. We report significantly enhanced CRR activity by incorporating the s-donating, e - reservoir ligand Imdye (1-imidazole-2,4,6-tri(carbazol-9-yl)-3,5-dicyanobenzene) within the complex fac -[Mn I (bpy)(CO) 3 (Imdye)] + (bpy = 2,2'-bipyridine). The reduction potentials of Imdye, Mn I/0 , and CO 2 to CO are close, allowing the active catalyst [Mn 0 (bpy)(CO) 2 (Imdye - )] - to provide 2e - to CO 2 at small overpotentials. This system reduces CO 2 to CO with bulk turnover numbers up to 830 very near the CRR reduction potential. This CRR activity arose from Imdye promoting the CRR at small overpotentials, and from utilizing the electrooxidation of CH 3 OH/H 2 O to CO 2 , 6H + and 6e - at the Pt counter electrode, neutralizing pH changes from the CRR. These strategies will apply to most CRR electrocatalytic systems.
