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...
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| Format: | Article |
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Frontiers Media S.A.
2022-06-01
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| Series: | Frontiers in Chemistry |
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| Online Access: | https://www.frontiersin.org/articles/10.3389/fchem.2022.913419/full |
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| author | Marcus Wohlgemuth Moritz L. Weber Lisa Heymann Christoph Baeumer Christoph Baeumer Felix Gunkel |
| author_facet | Marcus Wohlgemuth Moritz L. Weber Lisa Heymann Christoph Baeumer Christoph Baeumer Felix Gunkel |
| author_sort | Marcus Wohlgemuth |
| collection | DOAJ |
| 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 La0.6Sr0.4CoO3-δ catalysts follow the inverse relationship, while for LaNiO3-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. |
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| institution | Directory Open Access Journal |
| issn | 2296-2646 |
| language | English |
| last_indexed | 2024-12-12T16:16:22Z |
| publishDate | 2022-06-01 |
| publisher | Frontiers Media S.A. |
| record_format | Article |
| series | Frontiers in Chemistry |
| spelling | doaj.art-ae32dea5bb4b4bb9a5735f02309356a72022-12-22T00:19:06ZengFrontiers Media S.A.Frontiers in Chemistry2296-26462022-06-011010.3389/fchem.2022.913419913419Activity-Stability Relationships in Oxide Electrocatalysts for Water ElectrolysisMarcus Wohlgemuth0Moritz L. Weber1Lisa Heymann2Christoph Baeumer3Christoph Baeumer4Felix Gunkel5Peter Gruenberg Institute and JARA-FIT, Forschungszentrum Juelich GmbH, Jülich, GermanyPeter Gruenberg Institute and JARA-FIT, Forschungszentrum Juelich GmbH, Jülich, GermanyPeter Gruenberg Institute and JARA-FIT, Forschungszentrum Juelich GmbH, Jülich, GermanyPeter Gruenberg Institute and JARA-FIT, Forschungszentrum Juelich GmbH, Jülich, GermanyMESA+ Institute for Nanotechnology, Faculty of Science and Technology, University of Twente, Enschede, NetherlandsPeter Gruenberg Institute and JARA-FIT, Forschungszentrum Juelich GmbH, Jülich, GermanyThe 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 La0.6Sr0.4CoO3-δ catalysts follow the inverse relationship, while for LaNiO3-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.https://www.frontiersin.org/articles/10.3389/fchem.2022.913419/fullwater electrolysisoxide electrocatalysisactivity-stability relationsperovskite—type oxidegreen hydrogenoxygen evolution reaction |
| spellingShingle | Marcus Wohlgemuth Moritz L. Weber Lisa Heymann Christoph Baeumer Christoph Baeumer Felix Gunkel Activity-Stability Relationships in Oxide Electrocatalysts for Water Electrolysis Frontiers in Chemistry water electrolysis oxide electrocatalysis activity-stability relations perovskite—type oxide green hydrogen oxygen evolution reaction |
| 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 | water electrolysis oxide electrocatalysis activity-stability relations perovskite—type oxide green hydrogen oxygen evolution reaction |
| url | https://www.frontiersin.org/articles/10.3389/fchem.2022.913419/full |
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