Investigating Electrode Flooding in a Flowing Electrolyte, Gas‐Fed Carbon Dioxide Electrolyzer

Leonard, McLain E.; Clarke, Lauren E.; Forner‐Cuenca, Antoni; Brown, Steven M.; Brushett, Fikile R.

doi:10.1002/cssc.201902547

Title: Investigating Electrode Flooding in a Flowing Electrolyte, Gas‐Fed Carbon Dioxide Electrolyzer

Journal Article · 17 December 2019 · ChemSusChem

DOI: https://doi.org/10.1002/cssc.201902547 · OSTI ID:1579595

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Department of Chemical Engineering Massachusetts Institute of Technology Cambridge MA 02139 USA
Department of Chemical Engineering Massachusetts Institute of Technology Cambridge MA 02139 USA, Membrane Materials and Processes Department of Chemical Engineering and Chemistry Eindhoven University of Technology Het Kranenveld 14, P.O. Box 513, 5600 MB Eindhoven The Netherlands

Abstract Managing the gas–liquid interface within gas‐diffusion electrodes (GDEs) is key to maintaining high product selectivities in carbon dioxide electroreduction. By screening silver‐catalyzed GDEs over a range of applied current densities, an inverse correlation was observed between carbon monoxide selectivity and the electrochemical double‐layer capacitance, a proxy for wetted electrode area. Plotting current‐dependent performance as a function of cumulative charge led to data collapse onto a single sigmoidal curve indicating that the passage of faradaic current accelerates flooding. It was hypothesized that high cathode alkalinity, driven by both initial electrolyte conditions and cathode half‐reactions, promotes carbonate formation and precipitation which, in turn, facilitates electrolyte permeation. This mechanism was reinforced by the observations that post‐test GDEs retain less hydrophobicity than pristine materials and that water‐rinsing and drying electrodes temporarily recovers peak selectivity. This knowledge offers an opportunity to design electrodes with greater carbonation tolerance to improve device longevity.

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Sponsoring Organization:: USDOE

OSTI ID:: 1579595

Journal Information:: ChemSusChem, Journal Name: ChemSusChem Vol. 13 Journal Issue: 2; ISSN 1864-5631

Publisher:: Wiley Blackwell (John Wiley & Sons)Copyright Statement

Country of Publication:: Germany

Language:: English

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