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Activity-Stability Relationships in Oxide Electrocatalysts for Water Electrolysis
The oxygen evolution reaction (OER) is one of the key kinetically limiting half reactions in electrochemical energy conversion. Model epitaxial catalysts have emerged as a platform to identify structure-function-relationships at the atomic level, a prerequisite to establish advanced catalyst design...
Autores principales: | , , , , |
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Formato: | Online Artículo Texto |
Lenguaje: | English |
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Frontiers Media S.A.
2022
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Materias: | |
Acceso en línea: | https://www.ncbi.nlm.nih.gov/pmc/articles/PMC9259975/ https://www.ncbi.nlm.nih.gov/pubmed/35815219 http://dx.doi.org/10.3389/fchem.2022.913419 |
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author | Wohlgemuth, Marcus Weber, Moritz L. Heymann, Lisa Baeumer, Christoph Gunkel, Felix |
author_facet | Wohlgemuth, Marcus Weber, Moritz L. Heymann, Lisa Baeumer, Christoph Gunkel, Felix |
author_sort | Wohlgemuth, Marcus |
collection | PubMed |
description | The oxygen evolution reaction (OER) is one of the key kinetically limiting half reactions in electrochemical energy conversion. Model epitaxial catalysts have emerged as a platform to identify structure-function-relationships at the atomic level, a prerequisite to establish advanced catalyst design rules. Previous work identified an inverse relationship between activity and the stability of noble metal and oxide OER catalysts in both acidic and alkaline environments: The most active catalysts for the anodic OER are chemically unstable under reaction conditions leading to fast catalyst dissolution or amorphization, while the most stable catalysts lack sufficient activity. In this perspective, we discuss the role that epitaxial catalysts play in identifying this activity-stability-dilemma and introduce examples of how they can help overcome it. After a brief review of previously observed activity-stability-relationships, we will investigate the dependence of both activity and stability as a function of crystal facet. Our experiments reveal that the inverse relationship is not universal and does not hold for all perovskite oxides in the same manner. In fact, we find that facet-controlled epitaxial La(0.6)Sr(0.4)CoO(3-δ) catalysts follow the inverse relationship, while for LaNiO(3-δ), the (111) facet is both the most active and the most stable. In addition, we show that both activity and stability can be enhanced simultaneously by moving from La-rich to Ni-rich termination layers. These examples show that the previously observed inverse activity-stability-relationship can be overcome for select materials and through careful control of the atomic arrangement at the solid-liquid interface. This realization re-opens the search for active and stable catalysts for water electrolysis that are made from earth-abundant elements. At the same time, these results showcase that additional stabilization via material design strategies will be required to induce a general departure from inverse stability-activity relationships among the transition metal oxide catalysts to ultimately grant access to the full range of available oxides for OER catalysis. |
format | Online Article Text |
id | pubmed-9259975 |
institution | National Center for Biotechnology Information |
language | English |
publishDate | 2022 |
publisher | Frontiers Media S.A. |
record_format | MEDLINE/PubMed |
spelling | pubmed-92599752022-07-08 Activity-Stability Relationships in Oxide Electrocatalysts for Water Electrolysis Wohlgemuth, Marcus Weber, Moritz L. Heymann, Lisa Baeumer, Christoph Gunkel, Felix Front Chem Chemistry The oxygen evolution reaction (OER) is one of the key kinetically limiting half reactions in electrochemical energy conversion. Model epitaxial catalysts have emerged as a platform to identify structure-function-relationships at the atomic level, a prerequisite to establish advanced catalyst design rules. Previous work identified an inverse relationship between activity and the stability of noble metal and oxide OER catalysts in both acidic and alkaline environments: The most active catalysts for the anodic OER are chemically unstable under reaction conditions leading to fast catalyst dissolution or amorphization, while the most stable catalysts lack sufficient activity. In this perspective, we discuss the role that epitaxial catalysts play in identifying this activity-stability-dilemma and introduce examples of how they can help overcome it. After a brief review of previously observed activity-stability-relationships, we will investigate the dependence of both activity and stability as a function of crystal facet. Our experiments reveal that the inverse relationship is not universal and does not hold for all perovskite oxides in the same manner. In fact, we find that facet-controlled epitaxial La(0.6)Sr(0.4)CoO(3-δ) catalysts follow the inverse relationship, while for LaNiO(3-δ), the (111) facet is both the most active and the most stable. In addition, we show that both activity and stability can be enhanced simultaneously by moving from La-rich to Ni-rich termination layers. These examples show that the previously observed inverse activity-stability-relationship can be overcome for select materials and through careful control of the atomic arrangement at the solid-liquid interface. This realization re-opens the search for active and stable catalysts for water electrolysis that are made from earth-abundant elements. At the same time, these results showcase that additional stabilization via material design strategies will be required to induce a general departure from inverse stability-activity relationships among the transition metal oxide catalysts to ultimately grant access to the full range of available oxides for OER catalysis. Frontiers Media S.A. 2022-06-23 /pmc/articles/PMC9259975/ /pubmed/35815219 http://dx.doi.org/10.3389/fchem.2022.913419 Text en Copyright © 2022 Wohlgemuth, Weber, Heymann, Baeumer and Gunkel. https://creativecommons.org/licenses/by/4.0/This is an open-access article distributed under the terms of the Creative Commons Attribution License (CC BY). The use, distribution or reproduction in other forums is permitted, provided the original author(s) and the copyright owner(s) are credited and that the original publication in this journal is cited, in accordance with accepted academic practice. No use, distribution or reproduction is permitted which does not comply with these terms. |
spellingShingle | Chemistry Wohlgemuth, Marcus Weber, Moritz L. Heymann, Lisa Baeumer, Christoph Gunkel, Felix Activity-Stability Relationships in Oxide Electrocatalysts for Water Electrolysis |
title | Activity-Stability Relationships in Oxide Electrocatalysts for Water Electrolysis |
title_full | Activity-Stability Relationships in Oxide Electrocatalysts for Water Electrolysis |
title_fullStr | Activity-Stability Relationships in Oxide Electrocatalysts for Water Electrolysis |
title_full_unstemmed | Activity-Stability Relationships in Oxide Electrocatalysts for Water Electrolysis |
title_short | Activity-Stability Relationships in Oxide Electrocatalysts for Water Electrolysis |
title_sort | activity-stability relationships in oxide electrocatalysts for water electrolysis |
topic | Chemistry |
url | https://www.ncbi.nlm.nih.gov/pmc/articles/PMC9259975/ https://www.ncbi.nlm.nih.gov/pubmed/35815219 http://dx.doi.org/10.3389/fchem.2022.913419 |
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