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In situ formation of cocatalytic sites boosts single-atom catalysts for nitrogen oxide reduction

Nitrogen oxide (NO(x)) pollution presents a severe threat to the environment and human health. Catalytic reduction of NO(x) with H(2) using single-atom catalysts poses considerable potential in the remediation of air pollution; however, the unfavorable process of H(2) dissociation limits its practic...

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Autores principales: Wang, Pengfei, Liu, Guoquan, Hao, Zhifei, Zhang, He, Li, Yi, Sun, Wenming, Zheng, Lirong, Zhan, Sihui
Formato: Online Artículo Texto
Lenguaje:English
Publicado: National Academy of Sciences 2023
Materias:
Acceso en línea:https://www.ncbi.nlm.nih.gov/pmc/articles/PMC9974487/
https://www.ncbi.nlm.nih.gov/pubmed/36787366
http://dx.doi.org/10.1073/pnas.2216584120
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author Wang, Pengfei
Liu, Guoquan
Hao, Zhifei
Zhang, He
Li, Yi
Sun, Wenming
Zheng, Lirong
Zhan, Sihui
author_facet Wang, Pengfei
Liu, Guoquan
Hao, Zhifei
Zhang, He
Li, Yi
Sun, Wenming
Zheng, Lirong
Zhan, Sihui
author_sort Wang, Pengfei
collection PubMed
description Nitrogen oxide (NO(x)) pollution presents a severe threat to the environment and human health. Catalytic reduction of NO(x) with H(2) using single-atom catalysts poses considerable potential in the remediation of air pollution; however, the unfavorable process of H(2) dissociation limits its practical application. Herein, we report that the in situ formation of Pt(Ti) cocatalytic sites (which are stabilized by Pt–Ti bonds) over Pt(1)/TiO(2) significantly increases NO(x) conversion by reducing the energy barrier of H(2) activation. We demonstrate that two H atoms of H(2) molecule are absorbed by adjacent Pt atoms in Pt–O and Pt–Ti, respectively, which can promote the cleave of H–H bonds. Besides, Pt(Ti) sites facilitate the adsorption of NO molecules and further lower the activation barrier of the whole de-NO(x) reaction. Extending the concept to Pt(1)/Nb(2)O(5) and Pd(1)/TiO(2) systems also sees enhanced catalytic activities, demonstrating that engineering the cocatalytic sites can be a general strategy for the design of high-efficiency catalysts that can benefit environmental sustainability.
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spelling pubmed-99744872023-08-14 In situ formation of cocatalytic sites boosts single-atom catalysts for nitrogen oxide reduction Wang, Pengfei Liu, Guoquan Hao, Zhifei Zhang, He Li, Yi Sun, Wenming Zheng, Lirong Zhan, Sihui Proc Natl Acad Sci U S A Physical Sciences Nitrogen oxide (NO(x)) pollution presents a severe threat to the environment and human health. Catalytic reduction of NO(x) with H(2) using single-atom catalysts poses considerable potential in the remediation of air pollution; however, the unfavorable process of H(2) dissociation limits its practical application. Herein, we report that the in situ formation of Pt(Ti) cocatalytic sites (which are stabilized by Pt–Ti bonds) over Pt(1)/TiO(2) significantly increases NO(x) conversion by reducing the energy barrier of H(2) activation. We demonstrate that two H atoms of H(2) molecule are absorbed by adjacent Pt atoms in Pt–O and Pt–Ti, respectively, which can promote the cleave of H–H bonds. Besides, Pt(Ti) sites facilitate the adsorption of NO molecules and further lower the activation barrier of the whole de-NO(x) reaction. Extending the concept to Pt(1)/Nb(2)O(5) and Pd(1)/TiO(2) systems also sees enhanced catalytic activities, demonstrating that engineering the cocatalytic sites can be a general strategy for the design of high-efficiency catalysts that can benefit environmental sustainability. National Academy of Sciences 2023-02-14 2023-02-21 /pmc/articles/PMC9974487/ /pubmed/36787366 http://dx.doi.org/10.1073/pnas.2216584120 Text en Copyright © 2023 the Author(s). Published by PNAS. https://creativecommons.org/licenses/by-nc-nd/4.0/This article is distributed under Creative Commons Attribution-NonCommercial-NoDerivatives License 4.0 (CC BY-NC-ND) (https://creativecommons.org/licenses/by-nc-nd/4.0/) .
spellingShingle Physical Sciences
Wang, Pengfei
Liu, Guoquan
Hao, Zhifei
Zhang, He
Li, Yi
Sun, Wenming
Zheng, Lirong
Zhan, Sihui
In situ formation of cocatalytic sites boosts single-atom catalysts for nitrogen oxide reduction
title In situ formation of cocatalytic sites boosts single-atom catalysts for nitrogen oxide reduction
title_full In situ formation of cocatalytic sites boosts single-atom catalysts for nitrogen oxide reduction
title_fullStr In situ formation of cocatalytic sites boosts single-atom catalysts for nitrogen oxide reduction
title_full_unstemmed In situ formation of cocatalytic sites boosts single-atom catalysts for nitrogen oxide reduction
title_short In situ formation of cocatalytic sites boosts single-atom catalysts for nitrogen oxide reduction
title_sort in situ formation of cocatalytic sites boosts single-atom catalysts for nitrogen oxide reduction
topic Physical Sciences
url https://www.ncbi.nlm.nih.gov/pmc/articles/PMC9974487/
https://www.ncbi.nlm.nih.gov/pubmed/36787366
http://dx.doi.org/10.1073/pnas.2216584120
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