Investigating Electrode Flooding in a Flowing Electrolyte, Gas‐Fed Carbon Dioxide Electrolyzer
© 2019 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim 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 inver...
| Main Authors: | , , , , |
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| Other Authors: | |
| Format: | Article |
| Language: | English |
| Published: |
Wiley
2021
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| Online Access: | https://hdl.handle.net/1721.1/134642 |
| _version_ | 1811083600005693440 |
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| author | Leonard, McLain E Clarke, Lauren E Forner‐Cuenca, Antoni Brown, Steven M Brushett, Fikile R |
| author2 | Massachusetts Institute of Technology. Department of Chemical Engineering |
| author_facet | Massachusetts Institute of Technology. Department of Chemical Engineering Leonard, McLain E Clarke, Lauren E Forner‐Cuenca, Antoni Brown, Steven M Brushett, Fikile R |
| author_sort | Leonard, McLain E |
| collection | MIT |
| description | © 2019 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim 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. |
| first_indexed | 2024-09-23T12:35:38Z |
| format | Article |
| id | mit-1721.1/134642 |
| institution | Massachusetts Institute of Technology |
| language | English |
| last_indexed | 2024-09-23T12:35:38Z |
| publishDate | 2021 |
| publisher | Wiley |
| record_format | dspace |
| spelling | mit-1721.1/1346422023-11-14T19:40:43Z 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 Massachusetts Institute of Technology. Department of Chemical Engineering © 2019 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim 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. 2021-10-27T20:05:56Z 2021-10-27T20:05:56Z 2020 2021-06-09T15:06:39Z Article http://purl.org/eprint/type/JournalArticle https://hdl.handle.net/1721.1/134642 en 10.1002/CSSC.201902547 ChemSusChem Creative Commons Attribution-Noncommercial-Share Alike http://creativecommons.org/licenses/by-nc-sa/4.0/ application/pdf Wiley Other repository |
| spellingShingle | Leonard, McLain E Clarke, Lauren E Forner‐Cuenca, Antoni Brown, Steven M Brushett, Fikile R Investigating Electrode Flooding in a Flowing Electrolyte, Gas‐Fed Carbon Dioxide Electrolyzer |
| title | Investigating Electrode Flooding in a Flowing Electrolyte, Gas‐Fed Carbon Dioxide Electrolyzer |
| title_full | Investigating Electrode Flooding in a Flowing Electrolyte, Gas‐Fed Carbon Dioxide Electrolyzer |
| title_fullStr | Investigating Electrode Flooding in a Flowing Electrolyte, Gas‐Fed Carbon Dioxide Electrolyzer |
| title_full_unstemmed | Investigating Electrode Flooding in a Flowing Electrolyte, Gas‐Fed Carbon Dioxide Electrolyzer |
| title_short | Investigating Electrode Flooding in a Flowing Electrolyte, Gas‐Fed Carbon Dioxide Electrolyzer |
| title_sort | investigating electrode flooding in a flowing electrolyte gas fed carbon dioxide electrolyzer |
| url | https://hdl.handle.net/1721.1/134642 |
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