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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Main Authors: Seo, Han Gil, Staerz, Anna, Kim, Dennis S, LeBeau, James M, Tuller, Harry L
Other Authors: Massachusetts Institute of Technology. Department of Materials Science and Engineering
Format: Article
Language:English
Published: Wiley 2023
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.
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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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