DOE OSTI · 3374306
Reactive CO 2 capture via controlled amine speciation in non-aqueous electrolytes
Abstract
Current efforts to integrate CO 2 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 CO 2 streams. Here, in this study, we explore reactive capture in aprotic media. By shifting the amine–CO 2 adduct speciation to carbamic acid (instead of carbamate) in dimethyl sulfoxide, we increased CO 2 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% CO 2 , 17% O 2 , 66% N 2 ), 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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Gomes, Reginaldo J. [Univ. of Chicago, IL (United States)] (ORCID:000000019613545X), Li, Jianping [Argonne National Laboratory (ANL), Argonne, IL (United States)], Xu, Jiayi [Argonne National Laboratory (ANL), Argonne, IL (United States); Univ. of Chicago, IL (United States)] (ORCID:0000000317636251), Sarkar, Bidushi [Univ. of Chicago, IL (United States)] (ORCID:0000000347833870), Mohebi, Matin [Univ. of Chicago, IL (United States)] (ORCID:0009000447516853), Gabriel, Joshua [Argonne National Laboratory (ANL), Argonne, IL (United States)], Mathew, Tony Joseph [Argonne National Laboratory (ANL), Argonne, IL (United States)] (ORCID:0000000348722670), Roy, Ishaan [Univ. of Chicago, IL (United States)], Paulson, Noah [Argonne National Laboratory (ANL), Argonne, IL (United States)] (ORCID:0000000235489120), Liu, Cong [Argonne National Laboratory (ANL), Argonne, IL (United States); Univ. of Chicago, IL (United States)] (ORCID:0000000221455034), Iloeje, Chukwunwike O. [Argonne National Laboratory (ANL), Argonne, IL (United States); Univ. of Chicago, IL (United States)] (ORCID:0000000234269425), Amanchukwu, Chibueze V. [Univ. of Chicago, IL (United States); Argonne National Laboratory (ANL), Argonne, IL (United States)] (ORCID:0000000265731213). 2026-04-17. Reactive CO 2 capture via controlled amine speciation in non-aqueous electrolytes. https://doi.org/10.1038/s41560-026-02035-4
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