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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Vydané v:	ChemSusChem Ročník 13; číslo 2; s. 400 - 411
Hlavní autori:	Leonard, McLain E., Clarke, Lauren E., Forner‐Cuenca, Antoni, Brown, Steven M., Brushett, Fikile R.
Médium:	Journal Article
Jazyk:	English
Vydavateľské údaje:	Germany Wiley Subscription Services, Inc 19.01.2020
Predmet:	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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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. 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.
AbstractList	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.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. 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. 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.
Author	Forner‐Cuenca, Antoni Leonard, McLain E. Clarke, Lauren E. Brown, Steven M. Brushett, Fikile R.
Author_xml	– sequence: 1 givenname: McLain E. orcidid: 0000-0003-4572-5251 surname: Leonard fullname: Leonard, McLain E. organization: Massachusetts Institute of Technology – sequence: 2 givenname: Lauren E. orcidid: 0000-0003-4780-2791 surname: Clarke fullname: Clarke, Lauren E. organization: Massachusetts Institute of Technology – sequence: 3 givenname: Antoni orcidid: 0000-0002-7681-0435 surname: Forner‐Cuenca fullname: Forner‐Cuenca, Antoni organization: Eindhoven University of Technology – sequence: 4 givenname: Steven M. orcidid: 0000-0002-4360-6286 surname: Brown fullname: Brown, Steven M. organization: Massachusetts Institute of Technology – sequence: 5 givenname: Fikile R. orcidid: 0000-0002-7361-6637 surname: Brushett fullname: Brushett, Fikile R. email: brushett@mit.edu organization: Massachusetts Institute of Technology
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Keywords	gas diffusion electrodes wetting energy conversion electrochemistry carbon dioxide reduction
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Snippet	Managing the gas–liquid interface within gas‐diffusion electrodes (GDEs) is key to maintaining high product selectivities in carbon dioxide electroreduction.... Managing the gas-liquid interface within gas-diffusion electrodes (GDEs) is key to maintaining high product selectivities in carbon dioxide electroreduction....
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SubjectTerms	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
Title	Investigating Electrode Flooding in a Flowing Electrolyte, Gas‐Fed Carbon Dioxide Electrolyzer
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