Cation Crossover Limits Accessible Current Densities for Zero-Gap Alkaline CO2 Reduction to Ethylene

Simonson, Hunter; Henckel, Danielle; Klein, W. Ellis; Neyerlin, K.C.; Smith, Wilson A.

doi:10.1021/acssuschemeng.4c06744

Cation Crossover Limits Accessible Current Densities for Zero-Gap Alkaline CO2 Reduction to Ethylene

Journal Article · Wed Jan 08 04:00:00 EST 2025 · ACS Sustainable Chemistry & Engineering

DOI:https://doi.org/10.1021/acssuschemeng.4c06744· OSTI ID:2522822

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Traditional CO2 reduction systems often fail in an alkaline environment due to the interaction of CO2 with a high-pH electrolyte, where carbonate and bicarbonate ion formation results in potassium-containing salt precipitation. The presence of the salt crystals causes a reduction in the selectivity of the electrolyzer toward CO2 conversion. Here, the critical operational variables, which elicit the salting out process, are investigated (i.e., ion transport). When the electrolyzer exceeds a critical current density, H2 evolution dominates CO2 reduction due to salt formation, which is confirmed by postmortem cross-sectional SEM-EDS of the electrode. The critical current density decreases with an increasing membrane thickness or anolyte ionic strength. Cathode salt formation is mediated by the unmitigated crossover of cations from the anolyte to the cathode across an anion exchange membrane, through which cations are imperfectly excluded. It is likely that electric field-driven migration promotes an increase in concentration of potassium across the membrane, until, at the critical current density for that electrolyzer arrangement, the concentration of potassium and bicarbonate ions exceeds the solubility limit of KHCO3, leading to salt precipitation.

Research Organization:: National Renewable Energy Laboratory (NREL), Golden, CO (United States)

Sponsoring Organization:: Shell

DOE Contract Number:: AC36-08GO28308

OSTI ID:: 2522822

Report Number(s):: NREL/JA-5900-90340; MainId:92118; UUID:580f0c00-7fc6-4a56-a37c-e0562a0f0def; MainAdminId:76160

Journal Information:: ACS Sustainable Chemistry & Engineering, Journal Name: ACS Sustainable Chemistry & Engineering Journal Issue: 2 Vol. 13

Country of Publication:: United States

Language:: English

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