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High-loading single Pt atom sites [Pt-O(OH)(x)] catalyze the CO PROX reaction with high activity and selectivity at mild conditions

The preferential oxidation of CO (PROX) in hydrogen-rich fuel gas streams is an attractive option to remove CO while effectively conserving energy and H(2). However, high CO conversion with concomitant high selectivity to CO(2) but not H(2)O is challenging. Here, we report the synthesis of high-load...

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Autores principales: Cao, Sufeng, Zhao, Yanyan, Lee, Sungsik, Yang, Shize, Liu, Jilei, Giannakakis, Georgios, Li, Mengwei, Ouyang, Mengyao, Wang, Dunwei, Sykes, E. Charles H., Flytzani-Stephanopoulos, Maria
Formato: Online Artículo Texto
Lenguaje:English
Publicado: American Association for the Advancement of Science 2020
Materias:
Acceso en línea:https://www.ncbi.nlm.nih.gov/pmc/articles/PMC7299615/
https://www.ncbi.nlm.nih.gov/pubmed/32596455
http://dx.doi.org/10.1126/sciadv.aba3809
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author Cao, Sufeng
Zhao, Yanyan
Lee, Sungsik
Yang, Shize
Liu, Jilei
Giannakakis, Georgios
Li, Mengwei
Ouyang, Mengyao
Wang, Dunwei
Sykes, E. Charles H.
Flytzani-Stephanopoulos, Maria
author_facet Cao, Sufeng
Zhao, Yanyan
Lee, Sungsik
Yang, Shize
Liu, Jilei
Giannakakis, Georgios
Li, Mengwei
Ouyang, Mengyao
Wang, Dunwei
Sykes, E. Charles H.
Flytzani-Stephanopoulos, Maria
author_sort Cao, Sufeng
collection PubMed
description The preferential oxidation of CO (PROX) in hydrogen-rich fuel gas streams is an attractive option to remove CO while effectively conserving energy and H(2). However, high CO conversion with concomitant high selectivity to CO(2) but not H(2)O is challenging. Here, we report the synthesis of high-loading single Pt atom (2.0 weight %) catalysts with oxygen-bonded alkaline ions that stabilize the cationic Pt. The synthesis is performed in aqueous solution and achieves high Pt atom loadings in a single-step incipient wetness impregnation of alumina or silica. Promisingly, these catalysts have high CO PROX selectivity even at high CO conversion (~99.8% conversion, 70% selectivity at 110°C) and good stability under reaction conditions. These findings pave the way for the design of highly efficient single-atom catalysts, elucidate the role of ─OH species in CO oxidation, and confirm the absence of a support effect for our case.
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spelling pubmed-72996152020-06-25 High-loading single Pt atom sites [Pt-O(OH)(x)] catalyze the CO PROX reaction with high activity and selectivity at mild conditions Cao, Sufeng Zhao, Yanyan Lee, Sungsik Yang, Shize Liu, Jilei Giannakakis, Georgios Li, Mengwei Ouyang, Mengyao Wang, Dunwei Sykes, E. Charles H. Flytzani-Stephanopoulos, Maria Sci Adv Research Articles The preferential oxidation of CO (PROX) in hydrogen-rich fuel gas streams is an attractive option to remove CO while effectively conserving energy and H(2). However, high CO conversion with concomitant high selectivity to CO(2) but not H(2)O is challenging. Here, we report the synthesis of high-loading single Pt atom (2.0 weight %) catalysts with oxygen-bonded alkaline ions that stabilize the cationic Pt. The synthesis is performed in aqueous solution and achieves high Pt atom loadings in a single-step incipient wetness impregnation of alumina or silica. Promisingly, these catalysts have high CO PROX selectivity even at high CO conversion (~99.8% conversion, 70% selectivity at 110°C) and good stability under reaction conditions. These findings pave the way for the design of highly efficient single-atom catalysts, elucidate the role of ─OH species in CO oxidation, and confirm the absence of a support effect for our case. American Association for the Advancement of Science 2020-06-17 /pmc/articles/PMC7299615/ /pubmed/32596455 http://dx.doi.org/10.1126/sciadv.aba3809 Text en Copyright © 2020 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). http://creativecommons.org/licenses/by-nc/4.0/ This is an open-access article distributed under the terms of the Creative Commons Attribution-NonCommercial license (http://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 Research Articles
Cao, Sufeng
Zhao, Yanyan
Lee, Sungsik
Yang, Shize
Liu, Jilei
Giannakakis, Georgios
Li, Mengwei
Ouyang, Mengyao
Wang, Dunwei
Sykes, E. Charles H.
Flytzani-Stephanopoulos, Maria
High-loading single Pt atom sites [Pt-O(OH)(x)] catalyze the CO PROX reaction with high activity and selectivity at mild conditions
title High-loading single Pt atom sites [Pt-O(OH)(x)] catalyze the CO PROX reaction with high activity and selectivity at mild conditions
title_full High-loading single Pt atom sites [Pt-O(OH)(x)] catalyze the CO PROX reaction with high activity and selectivity at mild conditions
title_fullStr High-loading single Pt atom sites [Pt-O(OH)(x)] catalyze the CO PROX reaction with high activity and selectivity at mild conditions
title_full_unstemmed High-loading single Pt atom sites [Pt-O(OH)(x)] catalyze the CO PROX reaction with high activity and selectivity at mild conditions
title_short High-loading single Pt atom sites [Pt-O(OH)(x)] catalyze the CO PROX reaction with high activity and selectivity at mild conditions
title_sort high-loading single pt atom sites [pt-o(oh)(x)] catalyze the co prox reaction with high activity and selectivity at mild conditions
topic Research Articles
url https://www.ncbi.nlm.nih.gov/pmc/articles/PMC7299615/
https://www.ncbi.nlm.nih.gov/pubmed/32596455
http://dx.doi.org/10.1126/sciadv.aba3809
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