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Highly stable preferential carbon monoxide oxidation by dinuclear heterogeneous catalysts

Atomically dispersed catalysts have been shown highly active for preferential oxidation of carbon monoxide in the presence of excess hydrogen (PROX). However, their stability has been less than ideal. We show here that the introduction of a structural component to minimize diffusion of the active me...

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Autores principales: Zhao, Yanyan, Dai, Sheng, Yang, Ke R., Cao, Sufeng, Materna, Kelly L., Lant, Hannah M. C., Kao, Li Cheng, Feng, Xuefei, Guo, Jinghua, Brudvig, Gary W., Flytzani-Stephanopoulos, Maria, Batista, Victor S., Pan, Xiaoqing, Wang, Dunwei
Formato: Online Artículo Texto
Lenguaje:English
Publicado: National Academy of Sciences 2022
Materias:
Acceso en línea:https://www.ncbi.nlm.nih.gov/pmc/articles/PMC9910598/
https://www.ncbi.nlm.nih.gov/pubmed/36577066
http://dx.doi.org/10.1073/pnas.2206850120
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author Zhao, Yanyan
Dai, Sheng
Yang, Ke R.
Cao, Sufeng
Materna, Kelly L.
Lant, Hannah M. C.
Kao, Li Cheng
Feng, Xuefei
Guo, Jinghua
Brudvig, Gary W.
Flytzani-Stephanopoulos, Maria
Batista, Victor S.
Pan, Xiaoqing
Wang, Dunwei
author_facet Zhao, Yanyan
Dai, Sheng
Yang, Ke R.
Cao, Sufeng
Materna, Kelly L.
Lant, Hannah M. C.
Kao, Li Cheng
Feng, Xuefei
Guo, Jinghua
Brudvig, Gary W.
Flytzani-Stephanopoulos, Maria
Batista, Victor S.
Pan, Xiaoqing
Wang, Dunwei
author_sort Zhao, Yanyan
collection PubMed
description Atomically dispersed catalysts have been shown highly active for preferential oxidation of carbon monoxide in the presence of excess hydrogen (PROX). However, their stability has been less than ideal. We show here that the introduction of a structural component to minimize diffusion of the active metal center can greatly improve the stability without compromising the activity. Using an Ir dinuclear heterogeneous catalyst (DHC) as a study platform, we identify two types of oxygen species, interfacial and bridge, that work in concert to enable both activity and stability. The work sheds important light on the synergistic effect between the active metal center and the supporting substrate and may find broad applications for the use of atomically dispersed catalysts.
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spelling pubmed-99105982023-06-28 Highly stable preferential carbon monoxide oxidation by dinuclear heterogeneous catalysts Zhao, Yanyan Dai, Sheng Yang, Ke R. Cao, Sufeng Materna, Kelly L. Lant, Hannah M. C. Kao, Li Cheng Feng, Xuefei Guo, Jinghua Brudvig, Gary W. Flytzani-Stephanopoulos, Maria Batista, Victor S. Pan, Xiaoqing Wang, Dunwei Proc Natl Acad Sci U S A Physical Sciences Atomically dispersed catalysts have been shown highly active for preferential oxidation of carbon monoxide in the presence of excess hydrogen (PROX). However, their stability has been less than ideal. We show here that the introduction of a structural component to minimize diffusion of the active metal center can greatly improve the stability without compromising the activity. Using an Ir dinuclear heterogeneous catalyst (DHC) as a study platform, we identify two types of oxygen species, interfacial and bridge, that work in concert to enable both activity and stability. The work sheds important light on the synergistic effect between the active metal center and the supporting substrate and may find broad applications for the use of atomically dispersed catalysts. National Academy of Sciences 2022-12-28 2023-01-03 /pmc/articles/PMC9910598/ /pubmed/36577066 http://dx.doi.org/10.1073/pnas.2206850120 Text en Copyright © 2022 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
Zhao, Yanyan
Dai, Sheng
Yang, Ke R.
Cao, Sufeng
Materna, Kelly L.
Lant, Hannah M. C.
Kao, Li Cheng
Feng, Xuefei
Guo, Jinghua
Brudvig, Gary W.
Flytzani-Stephanopoulos, Maria
Batista, Victor S.
Pan, Xiaoqing
Wang, Dunwei
Highly stable preferential carbon monoxide oxidation by dinuclear heterogeneous catalysts
title Highly stable preferential carbon monoxide oxidation by dinuclear heterogeneous catalysts
title_full Highly stable preferential carbon monoxide oxidation by dinuclear heterogeneous catalysts
title_fullStr Highly stable preferential carbon monoxide oxidation by dinuclear heterogeneous catalysts
title_full_unstemmed Highly stable preferential carbon monoxide oxidation by dinuclear heterogeneous catalysts
title_short Highly stable preferential carbon monoxide oxidation by dinuclear heterogeneous catalysts
title_sort highly stable preferential carbon monoxide oxidation by dinuclear heterogeneous catalysts
topic Physical Sciences
url https://www.ncbi.nlm.nih.gov/pmc/articles/PMC9910598/
https://www.ncbi.nlm.nih.gov/pubmed/36577066
http://dx.doi.org/10.1073/pnas.2206850120
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