Journal
CHEMSUSCHEM
Volume 13, Issue 2, Pages 400-411Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/cssc.201902547
Keywords
carbon dioxide reduction; electrochemistry; energy conversion; gas diffusion electrodes; wetting
Funding
- National Science Foundation [DMR-1419807]
- Center for Nanoscale Systems at Harvard University
- DOE SBIR [DE-SC0015173]
- SNSF [PZEZP2_172183]
- U.S. Department of Energy (DOE) [DE-SC0015173] Funding Source: U.S. Department of Energy (DOE)
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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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