The conversion of carbon dioxide (CO2) to chemicals and fuels is vital because it simultaneously valorizes CO2 and incentivizes CO2 capture. Electrocatalytic CO2 conversion is of great interest because it is scalable and can be done at ambient temperature and pressure. However, these reactions are typically performed in water. Aqueous CO2 conversion is plagued by undesired hydrogen evolution from water breakdown that contributes to poor product selectivity, faradaic efficiency, and energy efficiency. Fortunately, aprotic organic solvents are not susceptible to hydrogen evolution and are typically used industrially to strip gas streams of CO2. However, when electrocatalytic CO2 conversion is performed in aprotic organic media, the product distribution is severely limited. Here, we study the influence of solvation in controlling electrocatalytic CO2 conversion. We modulate solvation behavior in aprotic solvents by controlling cation-anion-solvent interactions, and correlate bulk solvation phenomena to the reactions occurring at the catalyst-electrolyte interface. Our work provides insights highlighting the importance of reaction microenvironment in tuning overall electrocatalytic behavior, and enabling efficient and selective electrochemical transformations.

Solvation-enabled electrocatalytic conversion of carbon dioxide to desired products

ACS Spring 2022

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