Carbon dioxide (CO2) emissions have been connected to climate change. Transforming atmospheric CO2 into value-added products offers an opportunity to capture these emissions and mitigate negative climate effects. CO2 is thermodynamically stable, so conversion efforts employ a variety of molecular catalysts to activate the CO2 molecule. Here we present several Ru complexes with redox active (non-innocent) ligands that are capable of metal-ligand cooperativity (MLC), and we describe their use as CO2 reduction catalysts. This approach offers tunability through both the metal center and ligand environment for catalysis coupled with redox-activity in the ligand which enables monitoring of binding through electrochemical behavior. Cyclic voltammetry analysis provides redox chemistry metrics and mechanistic information for these complexes in the presence and absence of CO2 and a proton source. Bulk electrolysis experiments with and without proton sources coupled with product analysis involving gas chromatography and nuclear magnetic resonance spectroscopy provide information on Faradaic efficiencies for generated products, turnover number, side reactions, and catalyst stability. Future directions will build on knowledge obtained from this study and previous work to incorporate new ligand structures to optimize CO2 reduction performance and electrocatalytic stability.

Electrocatalytic reduction of CO2 with coordination complexes capable of metal-ligand cooperativity and ligand-centered redox activity

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ACS Fall 2022

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