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Artificially steering electrocatalytic oxygen evolution reaction mechanism by regulating oxygen defect contents in perovskites

The regulation of mechanism on the electrocatalysis process with multiple reaction pathways is more efficient and essential than conventional material engineering for the enhancement of catalyst performance. Here, by using oxygen evolution reaction (OER) as a model, which has an adsorbate evolution...

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Autores principales: Lu, Min, Zheng, Yao, Hu, Yang, Huang, Bolong, Ji, Deguang, Sun, Mingzi, Li, Jianyi, Peng, Yong, Si, Rui, Xi, Pinxian, Yan, Chun-Hua
Formato: Online Artículo Texto
Lenguaje:English
Publicado: American Association for the Advancement of Science 2022
Materias:
Acceso en línea:https://www.ncbi.nlm.nih.gov/pmc/articles/PMC9337758/
https://www.ncbi.nlm.nih.gov/pubmed/35905191
http://dx.doi.org/10.1126/sciadv.abq3563
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author Lu, Min
Zheng, Yao
Hu, Yang
Huang, Bolong
Ji, Deguang
Sun, Mingzi
Li, Jianyi
Peng, Yong
Si, Rui
Xi, Pinxian
Yan, Chun-Hua
author_facet Lu, Min
Zheng, Yao
Hu, Yang
Huang, Bolong
Ji, Deguang
Sun, Mingzi
Li, Jianyi
Peng, Yong
Si, Rui
Xi, Pinxian
Yan, Chun-Hua
author_sort Lu, Min
collection PubMed
description The regulation of mechanism on the electrocatalysis process with multiple reaction pathways is more efficient and essential than conventional material engineering for the enhancement of catalyst performance. Here, by using oxygen evolution reaction (OER) as a model, which has an adsorbate evolution mechanism (AEM) and a lattice oxygen oxidation mechanism (LOM), we demonstrate a general strategy for steering the two mechanisms on various La(x)Sr(1−x)CoO(3−δ). By delicately controlling the oxygen defect contents, the dominant OER mechanism on La(x)Sr(1−x)CoO(3−δ) can be arbitrarily transformed between AEM-LOM-AEM accompanied by a volcano-type activity variation trend. Experimental and computational evidence explicitly reveal that the phenomenon is due to the fact that the increased oxygen defects alter the lattice oxygen activity with a volcano-type trend and preserve the Co(0) state for preferably OER. Therefore, we achieve the co-optimization between the activity and stability of catalysts by altering the mechanism rather than a specific design of catalysts.
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spelling pubmed-93377582022-08-09 Artificially steering electrocatalytic oxygen evolution reaction mechanism by regulating oxygen defect contents in perovskites Lu, Min Zheng, Yao Hu, Yang Huang, Bolong Ji, Deguang Sun, Mingzi Li, Jianyi Peng, Yong Si, Rui Xi, Pinxian Yan, Chun-Hua Sci Adv Physical and Materials Sciences The regulation of mechanism on the electrocatalysis process with multiple reaction pathways is more efficient and essential than conventional material engineering for the enhancement of catalyst performance. Here, by using oxygen evolution reaction (OER) as a model, which has an adsorbate evolution mechanism (AEM) and a lattice oxygen oxidation mechanism (LOM), we demonstrate a general strategy for steering the two mechanisms on various La(x)Sr(1−x)CoO(3−δ). By delicately controlling the oxygen defect contents, the dominant OER mechanism on La(x)Sr(1−x)CoO(3−δ) can be arbitrarily transformed between AEM-LOM-AEM accompanied by a volcano-type activity variation trend. Experimental and computational evidence explicitly reveal that the phenomenon is due to the fact that the increased oxygen defects alter the lattice oxygen activity with a volcano-type trend and preserve the Co(0) state for preferably OER. Therefore, we achieve the co-optimization between the activity and stability of catalysts by altering the mechanism rather than a specific design of catalysts. American Association for the Advancement of Science 2022-07-29 /pmc/articles/PMC9337758/ /pubmed/35905191 http://dx.doi.org/10.1126/sciadv.abq3563 Text en Copyright © 2022 The Authors, some rights reserved; exclusive licensee American Association for the Advancement of Science. No claim to original U.S. Government Works. Distributed under a Creative Commons Attribution NonCommercial License 4.0 (CC BY-NC). https://creativecommons.org/licenses/by-nc/4.0/This is an open-access article distributed under the terms of the Creative Commons Attribution-NonCommercial license (https://creativecommons.org/licenses/by-nc/4.0/) , which permits use, distribution, and reproduction in any medium, so long as the resultant use is not for commercial advantage and provided the original work is properly cited.
spellingShingle Physical and Materials Sciences
Lu, Min
Zheng, Yao
Hu, Yang
Huang, Bolong
Ji, Deguang
Sun, Mingzi
Li, Jianyi
Peng, Yong
Si, Rui
Xi, Pinxian
Yan, Chun-Hua
Artificially steering electrocatalytic oxygen evolution reaction mechanism by regulating oxygen defect contents in perovskites
title Artificially steering electrocatalytic oxygen evolution reaction mechanism by regulating oxygen defect contents in perovskites
title_full Artificially steering electrocatalytic oxygen evolution reaction mechanism by regulating oxygen defect contents in perovskites
title_fullStr Artificially steering electrocatalytic oxygen evolution reaction mechanism by regulating oxygen defect contents in perovskites
title_full_unstemmed Artificially steering electrocatalytic oxygen evolution reaction mechanism by regulating oxygen defect contents in perovskites
title_short Artificially steering electrocatalytic oxygen evolution reaction mechanism by regulating oxygen defect contents in perovskites
title_sort artificially steering electrocatalytic oxygen evolution reaction mechanism by regulating oxygen defect contents in perovskites
topic Physical and Materials Sciences
url https://www.ncbi.nlm.nih.gov/pmc/articles/PMC9337758/
https://www.ncbi.nlm.nih.gov/pubmed/35905191
http://dx.doi.org/10.1126/sciadv.abq3563
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