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Ir-Sn pair-site triggers key oxygen radical intermediate for efficient acidic water oxidation
The anode corrosion induced by the harsh acidic and oxidative environment greatly restricts the lifespan of catalysts. Here, we propose an antioxidation strategy to mitigate Ir dissolution by triggering strong electronic interaction via elaborately constructing a heterostructured Ir-Sn pair-site cat...
Autores principales: | , , , , , , , , , , , , |
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Formato: | Online Artículo Texto |
Lenguaje: | English |
Publicado: |
American Association for the Advancement of Science
2023
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Materias: | |
Acceso en línea: | https://www.ncbi.nlm.nih.gov/pmc/articles/PMC10584348/ https://www.ncbi.nlm.nih.gov/pubmed/37851800 http://dx.doi.org/10.1126/sciadv.adi8025 |
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author | Zheng, Xiaobo Yang, Jiarui Li, Peng Wang, Qishun Wu, Jiabin Zhang, Erhuan Chen, Shenghua Zhuang, Zechao Lai, Weihong Dou, Shixue Sun, Wenping Wang, Dingsheng Li, Yadong |
author_facet | Zheng, Xiaobo Yang, Jiarui Li, Peng Wang, Qishun Wu, Jiabin Zhang, Erhuan Chen, Shenghua Zhuang, Zechao Lai, Weihong Dou, Shixue Sun, Wenping Wang, Dingsheng Li, Yadong |
author_sort | Zheng, Xiaobo |
collection | PubMed |
description | The anode corrosion induced by the harsh acidic and oxidative environment greatly restricts the lifespan of catalysts. Here, we propose an antioxidation strategy to mitigate Ir dissolution by triggering strong electronic interaction via elaborately constructing a heterostructured Ir-Sn pair-site catalyst. The formation of Ir-Sn dual-site at the heterointerface and the resulting strong electronic interactions considerably reduce d-band holes of Ir species during both the synthesis and the oxygen evolution reaction processes and suppress their overoxidation, enabling the catalyst with substantially boosted corrosion resistance. Consequently, the optimized catalyst exhibits a high mass activity of 4.4 A mg(Ir)(−1) at an overpotential of 320 mV and outstanding long-term stability. A proton-exchange-membrane water electrolyzer using this catalyst delivers a current density of 2 A cm(−2) at 1.711 V and low degradation in an accelerated aging test. Theoretical calculations unravel that the oxygen radicals induced by the π* interaction between Ir 5d-O 2p might be responsible for the boosted activity and durability. |
format | Online Article Text |
id | pubmed-10584348 |
institution | National Center for Biotechnology Information |
language | English |
publishDate | 2023 |
publisher | American Association for the Advancement of Science |
record_format | MEDLINE/PubMed |
spelling | pubmed-105843482023-10-19 Ir-Sn pair-site triggers key oxygen radical intermediate for efficient acidic water oxidation Zheng, Xiaobo Yang, Jiarui Li, Peng Wang, Qishun Wu, Jiabin Zhang, Erhuan Chen, Shenghua Zhuang, Zechao Lai, Weihong Dou, Shixue Sun, Wenping Wang, Dingsheng Li, Yadong Sci Adv Physical and Materials Sciences The anode corrosion induced by the harsh acidic and oxidative environment greatly restricts the lifespan of catalysts. Here, we propose an antioxidation strategy to mitigate Ir dissolution by triggering strong electronic interaction via elaborately constructing a heterostructured Ir-Sn pair-site catalyst. The formation of Ir-Sn dual-site at the heterointerface and the resulting strong electronic interactions considerably reduce d-band holes of Ir species during both the synthesis and the oxygen evolution reaction processes and suppress their overoxidation, enabling the catalyst with substantially boosted corrosion resistance. Consequently, the optimized catalyst exhibits a high mass activity of 4.4 A mg(Ir)(−1) at an overpotential of 320 mV and outstanding long-term stability. A proton-exchange-membrane water electrolyzer using this catalyst delivers a current density of 2 A cm(−2) at 1.711 V and low degradation in an accelerated aging test. Theoretical calculations unravel that the oxygen radicals induced by the π* interaction between Ir 5d-O 2p might be responsible for the boosted activity and durability. American Association for the Advancement of Science 2023-10-18 /pmc/articles/PMC10584348/ /pubmed/37851800 http://dx.doi.org/10.1126/sciadv.adi8025 Text en Copyright © 2023 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 Zheng, Xiaobo Yang, Jiarui Li, Peng Wang, Qishun Wu, Jiabin Zhang, Erhuan Chen, Shenghua Zhuang, Zechao Lai, Weihong Dou, Shixue Sun, Wenping Wang, Dingsheng Li, Yadong Ir-Sn pair-site triggers key oxygen radical intermediate for efficient acidic water oxidation |
title | Ir-Sn pair-site triggers key oxygen radical intermediate for efficient acidic water oxidation |
title_full | Ir-Sn pair-site triggers key oxygen radical intermediate for efficient acidic water oxidation |
title_fullStr | Ir-Sn pair-site triggers key oxygen radical intermediate for efficient acidic water oxidation |
title_full_unstemmed | Ir-Sn pair-site triggers key oxygen radical intermediate for efficient acidic water oxidation |
title_short | Ir-Sn pair-site triggers key oxygen radical intermediate for efficient acidic water oxidation |
title_sort | ir-sn pair-site triggers key oxygen radical intermediate for efficient acidic water oxidation |
topic | Physical and Materials Sciences |
url | https://www.ncbi.nlm.nih.gov/pmc/articles/PMC10584348/ https://www.ncbi.nlm.nih.gov/pubmed/37851800 http://dx.doi.org/10.1126/sciadv.adi8025 |
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