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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...

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Autores principales: 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
Formato: Online Artículo Texto
Lenguaje:English
Publicado: American Association for the Advancement of Science 2023
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.
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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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