Tuning Surface Acidity of Mixed Conducting Electrodes: Recovery of Si‐Induced Degradation of Oxygen Exchange Rate and Area Specific Resistance
Metal oxides are an important class of functional materials, and for many applications, ranging from solid oxide fuel/electrolysis cells, oxygen permeation membranes, and oxygen storage materials to gas sensors (semiconducting and electrolytic) and catalysts, the interaction between the surface and...
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Format: | Article |
Language: | English |
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Wiley
2023
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Online Access: | https://hdl.handle.net/1721.1/148048 |
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author | Seo, Han Gil Staerz, Anna Kim, Dennis S LeBeau, James M Tuller, Harry L |
author2 | Massachusetts Institute of Technology. Department of Materials Science and Engineering |
author_facet | Massachusetts Institute of Technology. Department of Materials Science and Engineering Seo, Han Gil Staerz, Anna Kim, Dennis S LeBeau, James M Tuller, Harry L |
author_sort | Seo, Han Gil |
collection | MIT |
description | Metal oxides are an important class of functional materials, and for many applications, ranging from solid oxide fuel/electrolysis cells, oxygen permeation membranes, and oxygen storage materials to gas sensors (semiconducting and electrolytic) and catalysts, the interaction between the surface and oxygen in the gas phase is central. Ubiquitous Si-impurities are known to impede this interaction, commonly attributed to the formation of glassy blocking layers on the surface. Here, the surface oxygen exchange coefficient (kchem ) is examined for Pr0.1 Ce0.9 O2-δ (PCO), a model mixed ionic electronic conductor, via electrical conductivity relaxation measurements, and the area-specific resistance (ASR) by electrochemical impedance spectroscopy. It is demonstrated that even low silica levels, introduced by infiltration, depress kchem by a factor 4000, while the ASR increases 40-fold and we attribute this to its acidity relative to that of PCO. The ability to fully regenerate the poisoned surface by the subsequent addition of basic Ca- or Li-species is further shown. This ability to not only recover Si-poisoned surfaces by tuning the relative surface acidity of an oxide surface, but subsequently outperform the pre-poisoned response, promises to extend the operating life of materials and devices for which the catalytic oxygen/solid interface reaction is central. |
first_indexed | 2024-09-23T11:44:42Z |
format | Article |
id | mit-1721.1/148048 |
institution | Massachusetts Institute of Technology |
language | English |
last_indexed | 2024-09-23T11:44:42Z |
publishDate | 2023 |
publisher | Wiley |
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spelling | mit-1721.1/1480482023-02-15T03:29:18Z Tuning Surface Acidity of Mixed Conducting Electrodes: Recovery of Si‐Induced Degradation of Oxygen Exchange Rate and Area Specific Resistance Seo, Han Gil Staerz, Anna Kim, Dennis S LeBeau, James M Tuller, Harry L Massachusetts Institute of Technology. Department of Materials Science and Engineering Metal oxides are an important class of functional materials, and for many applications, ranging from solid oxide fuel/electrolysis cells, oxygen permeation membranes, and oxygen storage materials to gas sensors (semiconducting and electrolytic) and catalysts, the interaction between the surface and oxygen in the gas phase is central. Ubiquitous Si-impurities are known to impede this interaction, commonly attributed to the formation of glassy blocking layers on the surface. Here, the surface oxygen exchange coefficient (kchem ) is examined for Pr0.1 Ce0.9 O2-δ (PCO), a model mixed ionic electronic conductor, via electrical conductivity relaxation measurements, and the area-specific resistance (ASR) by electrochemical impedance spectroscopy. It is demonstrated that even low silica levels, introduced by infiltration, depress kchem by a factor 4000, while the ASR increases 40-fold and we attribute this to its acidity relative to that of PCO. The ability to fully regenerate the poisoned surface by the subsequent addition of basic Ca- or Li-species is further shown. This ability to not only recover Si-poisoned surfaces by tuning the relative surface acidity of an oxide surface, but subsequently outperform the pre-poisoned response, promises to extend the operating life of materials and devices for which the catalytic oxygen/solid interface reaction is central. 2023-02-14T17:12:42Z 2023-02-14T17:12:42Z 2022-12-03 2023-02-14T16:54:43Z Article http://purl.org/eprint/type/JournalArticle https://hdl.handle.net/1721.1/148048 Seo, Han Gil, Staerz, Anna, Kim, Dennis S, LeBeau, James M and Tuller, Harry L. 2022. "Tuning Surface Acidity of Mixed Conducting Electrodes: Recovery of Si‐Induced Degradation of Oxygen Exchange Rate and Area Specific Resistance." Advanced Materials. en 10.1002/adma.202208182 Advanced Materials Creative Commons Attribution-NonCommercial-NoDerivs License http://creativecommons.org/licenses/by-nc-nd/4.0/ application/pdf Wiley Wiley |
spellingShingle | Seo, Han Gil Staerz, Anna Kim, Dennis S LeBeau, James M Tuller, Harry L Tuning Surface Acidity of Mixed Conducting Electrodes: Recovery of Si‐Induced Degradation of Oxygen Exchange Rate and Area Specific Resistance |
title | Tuning Surface Acidity of Mixed Conducting Electrodes: Recovery of Si‐Induced Degradation of Oxygen Exchange Rate and Area Specific Resistance |
title_full | Tuning Surface Acidity of Mixed Conducting Electrodes: Recovery of Si‐Induced Degradation of Oxygen Exchange Rate and Area Specific Resistance |
title_fullStr | Tuning Surface Acidity of Mixed Conducting Electrodes: Recovery of Si‐Induced Degradation of Oxygen Exchange Rate and Area Specific Resistance |
title_full_unstemmed | Tuning Surface Acidity of Mixed Conducting Electrodes: Recovery of Si‐Induced Degradation of Oxygen Exchange Rate and Area Specific Resistance |
title_short | Tuning Surface Acidity of Mixed Conducting Electrodes: Recovery of Si‐Induced Degradation of Oxygen Exchange Rate and Area Specific Resistance |
title_sort | tuning surface acidity of mixed conducting electrodes recovery of si induced degradation of oxygen exchange rate and area specific resistance |
url | https://hdl.handle.net/1721.1/148048 |
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