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Hydrogen spillover assisted by oxygenate molecules over nonreducible oxides

Spontaneous migration of atomic hydrogen species from metal particles to the surface of their support, known as hydrogen spillover, has been claimed to play a major role in catalytic processes involving hydrogen. While this phenomenon is well established on reducible oxide supports, its realization...

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Autores principales: Tan, Mingwu, Yang, Yanling, Yang, Ying, Chen, Jiali, Zhang, Zhaoxia, Fu, Gang, Lin, Jingdong, Wan, Shaolong, Wang, Shuai, Wang, Yong
Formato: Online Artículo Texto
Lenguaje:English
Publicado: Nature Publishing Group UK 2022
Materias:
Acceso en línea:https://www.ncbi.nlm.nih.gov/pmc/articles/PMC8933562/
https://www.ncbi.nlm.nih.gov/pubmed/35304451
http://dx.doi.org/10.1038/s41467-022-29045-6
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author Tan, Mingwu
Yang, Yanling
Yang, Ying
Chen, Jiali
Zhang, Zhaoxia
Fu, Gang
Lin, Jingdong
Wan, Shaolong
Wang, Shuai
Wang, Yong
author_facet Tan, Mingwu
Yang, Yanling
Yang, Ying
Chen, Jiali
Zhang, Zhaoxia
Fu, Gang
Lin, Jingdong
Wan, Shaolong
Wang, Shuai
Wang, Yong
author_sort Tan, Mingwu
collection PubMed
description Spontaneous migration of atomic hydrogen species from metal particles to the surface of their support, known as hydrogen spillover, has been claimed to play a major role in catalytic processes involving hydrogen. While this phenomenon is well established on reducible oxide supports, its realization on much more commonly used non-reducible oxides is still challenged. Here we present a general strategy to enable effective hydrogen spillover over non-reducible SiO(2) with aid of gaseous organic molecules containing a carbonyl group. By using hierarchically-porous-SiO(2)-supported bimetallic Pt-Fe catalysts with Pt nanoparticles exclusively deposited into the micropores, we demonstrate that activated hydrogen species generated on the Pt sites within the micropores can be readily transported by these oxygenate molecules to Fe sites located in macropores, leading to significantly accelerated hydrodeoxygenation rates on the latter sites. This finding provides a molecule-assisted approach to the rational design and optimization of multifunctional heterogeneous catalysts, reminiscent of the role of molecular coenzymes in bio-catalysis.
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spelling pubmed-89335622022-04-01 Hydrogen spillover assisted by oxygenate molecules over nonreducible oxides Tan, Mingwu Yang, Yanling Yang, Ying Chen, Jiali Zhang, Zhaoxia Fu, Gang Lin, Jingdong Wan, Shaolong Wang, Shuai Wang, Yong Nat Commun Article Spontaneous migration of atomic hydrogen species from metal particles to the surface of their support, known as hydrogen spillover, has been claimed to play a major role in catalytic processes involving hydrogen. While this phenomenon is well established on reducible oxide supports, its realization on much more commonly used non-reducible oxides is still challenged. Here we present a general strategy to enable effective hydrogen spillover over non-reducible SiO(2) with aid of gaseous organic molecules containing a carbonyl group. By using hierarchically-porous-SiO(2)-supported bimetallic Pt-Fe catalysts with Pt nanoparticles exclusively deposited into the micropores, we demonstrate that activated hydrogen species generated on the Pt sites within the micropores can be readily transported by these oxygenate molecules to Fe sites located in macropores, leading to significantly accelerated hydrodeoxygenation rates on the latter sites. This finding provides a molecule-assisted approach to the rational design and optimization of multifunctional heterogeneous catalysts, reminiscent of the role of molecular coenzymes in bio-catalysis. Nature Publishing Group UK 2022-03-18 /pmc/articles/PMC8933562/ /pubmed/35304451 http://dx.doi.org/10.1038/s41467-022-29045-6 Text en © This is a U.S. Government work and not under copyright protection in the US; foreign copyright protection may apply 2022 https://creativecommons.org/licenses/by/4.0/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/ (https://creativecommons.org/licenses/by/4.0/) .
spellingShingle Article
Tan, Mingwu
Yang, Yanling
Yang, Ying
Chen, Jiali
Zhang, Zhaoxia
Fu, Gang
Lin, Jingdong
Wan, Shaolong
Wang, Shuai
Wang, Yong
Hydrogen spillover assisted by oxygenate molecules over nonreducible oxides
title Hydrogen spillover assisted by oxygenate molecules over nonreducible oxides
title_full Hydrogen spillover assisted by oxygenate molecules over nonreducible oxides
title_fullStr Hydrogen spillover assisted by oxygenate molecules over nonreducible oxides
title_full_unstemmed Hydrogen spillover assisted by oxygenate molecules over nonreducible oxides
title_short Hydrogen spillover assisted by oxygenate molecules over nonreducible oxides
title_sort hydrogen spillover assisted by oxygenate molecules over nonreducible oxides
topic Article
url https://www.ncbi.nlm.nih.gov/pmc/articles/PMC8933562/
https://www.ncbi.nlm.nih.gov/pubmed/35304451
http://dx.doi.org/10.1038/s41467-022-29045-6
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