Transition metal electro-catalysts have previously been shown to convert carbon dioxide to carbon monoxide, which is promising for future energy schemes. Recent efforts have focused on (N^N)Mn(CO)3X complexes due to their performance and exclusion of expensive metals (X = anionic ligand, N^N = bidentate N-donor ligand). My presentation will focus on the characterization of proposed intermediates of (N^N)Mn(CO)3X (N^N = bpy). First, I will discuss the stability of the proposed (bpy)Mn(CO)4+ species, and how it may be pertinent to a catalytic cycle for CO2 reduction. Next, I will discuss how this complex can be used to prepare the (bpy)Mn(CO)3X (X = C(O)OH, C(O)OMe) species, and explore their electrochemical properties. Finally, I will compare the electrochemical behavior of two (bpy)Mn(CO)3X complexes (X= C(O)OH, OCHO) , to see at what potentials diverging reactivity, CO production versus formate production, occurs. Taken together, this work provides a better understanding of how to favor a protonation-first pathway for CO production, which occurs at lower overpotentials than the reduction-first mechanism. This will overall contribute more broadly to our understanding of electrocatalytic CO2 reduction.

Characterization of proposed intermediates in the electrocatalytic reduction of CO2 to CO at Mn complexes

ACS Spring 2022

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