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Dynamic structure of active sites in ceria-supported Pt catalysts for the water gas shift reaction

Oxide-supported noble metal catalysts have been extensively studied for decades for the water gas shift (WGS) reaction, a catalytic transformation central to a host of large volume processes that variously utilize or produce hydrogen. There remains considerable uncertainty as to how the specific fea...

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Autores principales: Li, Yuanyuan, Kottwitz, Matthew, Vincent, Joshua L., Enright, Michael J., Liu, Zongyuan, Zhang, Lihua, Huang, Jiahao, Senanayake, Sanjaya D., Yang, Wei-Chang D., Crozier, Peter A., Nuzzo, Ralph G., Frenkel, Anatoly I.
Formato: Online Artículo Texto
Lenguaje:English
Publicado: Nature Publishing Group UK 2021
Materias:
Acceso en línea:https://www.ncbi.nlm.nih.gov/pmc/articles/PMC7876036/
https://www.ncbi.nlm.nih.gov/pubmed/33568629
http://dx.doi.org/10.1038/s41467-021-21132-4
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author Li, Yuanyuan
Kottwitz, Matthew
Vincent, Joshua L.
Enright, Michael J.
Liu, Zongyuan
Zhang, Lihua
Huang, Jiahao
Senanayake, Sanjaya D.
Yang, Wei-Chang D.
Crozier, Peter A.
Nuzzo, Ralph G.
Frenkel, Anatoly I.
author_facet Li, Yuanyuan
Kottwitz, Matthew
Vincent, Joshua L.
Enright, Michael J.
Liu, Zongyuan
Zhang, Lihua
Huang, Jiahao
Senanayake, Sanjaya D.
Yang, Wei-Chang D.
Crozier, Peter A.
Nuzzo, Ralph G.
Frenkel, Anatoly I.
author_sort Li, Yuanyuan
collection PubMed
description Oxide-supported noble metal catalysts have been extensively studied for decades for the water gas shift (WGS) reaction, a catalytic transformation central to a host of large volume processes that variously utilize or produce hydrogen. There remains considerable uncertainty as to how the specific features of the active metal-support interfacial bonding—perhaps most importantly the temporal dynamic changes occurring therein—serve to enable high activity and selectivity. Here we report the dynamic characteristics of a Pt/CeO(2) system at the atomic level for the WGS reaction and specifically reveal the synergistic effects of metal-support bonding at the perimeter region. We find that the perimeter Pt(0) − O vacancy−Ce(3+) sites are formed in the active structure, transformed at working temperatures and their appearance regulates the adsorbate behaviors. We find that the dynamic nature of this site is a key mechanistic step for the WGS reaction.
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spelling pubmed-78760362021-02-24 Dynamic structure of active sites in ceria-supported Pt catalysts for the water gas shift reaction Li, Yuanyuan Kottwitz, Matthew Vincent, Joshua L. Enright, Michael J. Liu, Zongyuan Zhang, Lihua Huang, Jiahao Senanayake, Sanjaya D. Yang, Wei-Chang D. Crozier, Peter A. Nuzzo, Ralph G. Frenkel, Anatoly I. Nat Commun Article Oxide-supported noble metal catalysts have been extensively studied for decades for the water gas shift (WGS) reaction, a catalytic transformation central to a host of large volume processes that variously utilize or produce hydrogen. There remains considerable uncertainty as to how the specific features of the active metal-support interfacial bonding—perhaps most importantly the temporal dynamic changes occurring therein—serve to enable high activity and selectivity. Here we report the dynamic characteristics of a Pt/CeO(2) system at the atomic level for the WGS reaction and specifically reveal the synergistic effects of metal-support bonding at the perimeter region. We find that the perimeter Pt(0) − O vacancy−Ce(3+) sites are formed in the active structure, transformed at working temperatures and their appearance regulates the adsorbate behaviors. We find that the dynamic nature of this site is a key mechanistic step for the WGS reaction. Nature Publishing Group UK 2021-02-10 /pmc/articles/PMC7876036/ /pubmed/33568629 http://dx.doi.org/10.1038/s41467-021-21132-4 Text en © The Author(s) 2021 Open Access This article is licensed under a Creative Commons Attribution 4.0 International License, which permits use, sharing, adaptation, distribution and reproduction in any medium or format, as long as you give appropriate credit to the original author(s) and the source, provide a link to the Creative Commons license, and indicate if changes were made. The images or other third party material in this article are included in the article’s Creative Commons license, unless indicated otherwise in a credit line to the material. If material is not included in the article’s Creative Commons license and your intended use is not permitted by statutory regulation or exceeds the permitted use, you will need to obtain permission directly from the copyright holder. To view a copy of this license, visit http://creativecommons.org/licenses/by/4.0/.
spellingShingle Article
Li, Yuanyuan
Kottwitz, Matthew
Vincent, Joshua L.
Enright, Michael J.
Liu, Zongyuan
Zhang, Lihua
Huang, Jiahao
Senanayake, Sanjaya D.
Yang, Wei-Chang D.
Crozier, Peter A.
Nuzzo, Ralph G.
Frenkel, Anatoly I.
Dynamic structure of active sites in ceria-supported Pt catalysts for the water gas shift reaction
title Dynamic structure of active sites in ceria-supported Pt catalysts for the water gas shift reaction
title_full Dynamic structure of active sites in ceria-supported Pt catalysts for the water gas shift reaction
title_fullStr Dynamic structure of active sites in ceria-supported Pt catalysts for the water gas shift reaction
title_full_unstemmed Dynamic structure of active sites in ceria-supported Pt catalysts for the water gas shift reaction
title_short Dynamic structure of active sites in ceria-supported Pt catalysts for the water gas shift reaction
title_sort dynamic structure of active sites in ceria-supported pt catalysts for the water gas shift reaction
topic Article
url https://www.ncbi.nlm.nih.gov/pmc/articles/PMC7876036/
https://www.ncbi.nlm.nih.gov/pubmed/33568629
http://dx.doi.org/10.1038/s41467-021-21132-4
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