Experimental Measurement of Overpotential Sources during Anodic Gas Evolution in Aqueous and Molten Salt Systems

Current interrupt and galvanostatic EIS techniques were utilized in a complementary fashion to characterize the different sources of overpotential during anodic gas evolution. Room temperature anodic evolution of oxygen at a nickel working electrode in aqueous potassium hydroxide and the high temper...

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Main Authors: Chmielowiec, Brian John, Fujimura, Tatsuki, Otani, Tomohiro, Aoyama, Kiego, Nohira, Toshiyuki, Homma, Takayuki, Fukunaka, Yasuhiro, Allanore, Antoine
Other Authors: Massachusetts Institute of Technology. Department of Materials Science and Engineering
Format: Article
Language:English
Published: The Electrochemical Society 2021
Online Access:https://hdl.handle.net/1721.1/131147
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author Chmielowiec, Brian John
Fujimura, Tatsuki
Otani, Tomohiro
Aoyama, Kiego
Nohira, Toshiyuki
Homma, Takayuki
Fukunaka, Yasuhiro
Allanore, Antoine
author2 Massachusetts Institute of Technology. Department of Materials Science and Engineering
author_facet Massachusetts Institute of Technology. Department of Materials Science and Engineering
Chmielowiec, Brian John
Fujimura, Tatsuki
Otani, Tomohiro
Aoyama, Kiego
Nohira, Toshiyuki
Homma, Takayuki
Fukunaka, Yasuhiro
Allanore, Antoine
author_sort Chmielowiec, Brian John
collection MIT
description Current interrupt and galvanostatic EIS techniques were utilized in a complementary fashion to characterize the different sources of overpotential during anodic gas evolution. Room temperature anodic evolution of oxygen at a nickel working electrode in aqueous potassium hydroxide and the high temperature (348°C) anodic evolution of chlorine at a glassy carbon working electrode in molten (LiCl)[subscript 57.5-](KCl)[subscript 13.3-](CsCl)[subscript 29.2 ] where investigatd. Combining of the two techniques enables to separate the total measured overpotential into its ohmic, charge transfer, and mass transfer components. Potential decay curves indicated that natural convection (due to both bubble evolution and density driven flow) was a major driving force in reestablishing equilibrium conditions at the working electrode surface. During oxygen evolution, charge transfer resistance dominated the total overpotential at low current densities, but as the current density approached ~100mA/cm[superscript 2], mass transfer overpotentials and ohmic overpotential became non-negligible. The mass transfer overpotential during chlorine evolution was found to be half that found during oxygen evolution.
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spelling mit-1721.1/1311472022-10-02T06:00:49Z Experimental Measurement of Overpotential Sources during Anodic Gas Evolution in Aqueous and Molten Salt Systems Chmielowiec, Brian John Fujimura, Tatsuki Otani, Tomohiro Aoyama, Kiego Nohira, Toshiyuki Homma, Takayuki Fukunaka, Yasuhiro Allanore, Antoine Massachusetts Institute of Technology. Department of Materials Science and Engineering MIT Materials Research Laboratory Current interrupt and galvanostatic EIS techniques were utilized in a complementary fashion to characterize the different sources of overpotential during anodic gas evolution. Room temperature anodic evolution of oxygen at a nickel working electrode in aqueous potassium hydroxide and the high temperature (348°C) anodic evolution of chlorine at a glassy carbon working electrode in molten (LiCl)[subscript 57.5-](KCl)[subscript 13.3-](CsCl)[subscript 29.2 ] where investigatd. Combining of the two techniques enables to separate the total measured overpotential into its ohmic, charge transfer, and mass transfer components. Potential decay curves indicated that natural convection (due to both bubble evolution and density driven flow) was a major driving force in reestablishing equilibrium conditions at the working electrode surface. During oxygen evolution, charge transfer resistance dominated the total overpotential at low current densities, but as the current density approached ~100mA/cm[superscript 2], mass transfer overpotentials and ohmic overpotential became non-negligible. The mass transfer overpotential during chlorine evolution was found to be half that found during oxygen evolution. Naval Research (Contract N00014-12-1-0521) 2021-08-09T17:30:07Z 2021-08-09T17:30:07Z 2019-06 2019-04 2019-09-05T13:04:31Z Article http://purl.org/eprint/type/JournalArticle 0013-4651 1945-7111 https://hdl.handle.net/1721.1/131147 Chmielowiec, Brian John et al. "Experimental Measurement of Overpotential Sources during Anodic Gas Evolution in Aqueous and Molten Salt Systems." Journal of The Electrochemical Society 166, 10 (June 2019): E323. © 2019 The Author(s) en http://dx.doi.org/10.1149/2.1001910jes Journal of The Electrochemical Society Creative Commons Attribution-NonCommercial-NoDerivs License http://creativecommons.org/licenses/by-nc-nd/4.0/ application/pdf application/pdf The Electrochemical Society Prof. Allanore
spellingShingle Chmielowiec, Brian John
Fujimura, Tatsuki
Otani, Tomohiro
Aoyama, Kiego
Nohira, Toshiyuki
Homma, Takayuki
Fukunaka, Yasuhiro
Allanore, Antoine
Experimental Measurement of Overpotential Sources during Anodic Gas Evolution in Aqueous and Molten Salt Systems
title Experimental Measurement of Overpotential Sources during Anodic Gas Evolution in Aqueous and Molten Salt Systems
title_full Experimental Measurement of Overpotential Sources during Anodic Gas Evolution in Aqueous and Molten Salt Systems
title_fullStr Experimental Measurement of Overpotential Sources during Anodic Gas Evolution in Aqueous and Molten Salt Systems
title_full_unstemmed Experimental Measurement of Overpotential Sources during Anodic Gas Evolution in Aqueous and Molten Salt Systems
title_short Experimental Measurement of Overpotential Sources during Anodic Gas Evolution in Aqueous and Molten Salt Systems
title_sort experimental measurement of overpotential sources during anodic gas evolution in aqueous and molten salt systems
url https://hdl.handle.net/1721.1/131147
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