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

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 sele...

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Vydáno v:ChemSusChem Ročník 13; číslo 2; s. 400 - 411
Hlavní autoři: Leonard, McLain E., Clarke, Lauren E., Forner‐Cuenca, Antoni, Brown, Steven M., Brushett, Fikile R.
Médium: Journal Article
Jazyk:angličtina
Vydáno: Germany Wiley Subscription Services, Inc 19.01.2020
Témata:
Alkalinity
Carbon
Carbon dioxide
carbon dioxide reduction
Carbon monoxide
Carbonation
Cathodes
Collapse
Diffusion electrodes
electrochemistry
Electrodes
Electrolytes
Energy conversion
Flooding
gas diffusion electrodes
Hydrophobicity
Selectivity
Wetted electrodes
wetting
gas diffusion electrodes
wetting
energy conversion
electrochemistry
carbon dioxide reduction
ISSN:1864-5631, 1864-564X, 1864-564X
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Shrnutí: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. A matter of time: Gas‐diffusion electrodes (GDEs) for carbon dioxide electroreduction are screened over a range of applied current densities, and an inverse correlation is observed between carbon monoxide selectivity and the electrochemical double‐layer capacitance, a proxy for wetted electrode area. This knowledge offers an opportunity to design electrodes with greater carbonation tolerance to improve device longevity.
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ISSN:1864-5631
1864-564X
1864-564X
DOI:10.1002/cssc.201902547