by Reginaldo J. Gomes, Jianping Li, Jiayi Xu, Bidushi Sarkar, Matin Mohebi, Joshua Gabriel, Tony Joseph Mathew, Ishaan Roy, Noah Paulson, Cong Liu, Chukwunwike O. Iloeje & Chibueze V. Amanchukwu

Current efforts to integrate CO2 capture and electrochemical conversion (reactive capture) are often performed under aqueous conditions, resulting in undesired hydrogen evolution and reliance on precious metal catalysts and pure CO2 streams. Here we explore reactive capture in aprotic media. By shifting the amine–CO2 adduct speciation to carbamic acid (instead of carbamate) in dimethyl sulfoxide, we increased CO2 uptake threefold compared with an aqueous medium, suppressing hydrogen evolution and supporting a 78% Faradaic efficiency towards CO over an earth-abundant zinc catalyst. Under simulated high-oxygen-content flue gas (17% CO2, 17% O2, 66% N2), we also obtained up to 43% CO Faradaic efficiency over multiple capture–conversion cycles. Our findings showcase the confluence of reactant speciation, electrolyte composition and electrocatalyst design in enabling selective and active electrochemical transformations.

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