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Gold catalysts containing interstitial carbon atoms boost hydrogenation activity

Supported gold nanoparticles are emerging catalysts for heterogeneous catalytic reactions, including selective hydrogenation. The traditionally used supports such as silica do not favor the heterolytic dissociation of hydrogen on the surface of gold, thus limiting its hydrogenation activity. Here we...

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Autores principales: Sun, Yafei, Cao, Yueqiang, Wang, Lili, Mu, Xiaotong, Zhao, Qingfei, Si, Rui, Zhu, Xiaojuan, Chen, Shangjun, Zhang, Bingsen, Chen, De, Wan, Ying
Formato: Online Artículo Texto
Lenguaje:English
Publicado: Nature Publishing Group UK 2020
Materias:
Acceso en línea:https://www.ncbi.nlm.nih.gov/pmc/articles/PMC7490344/
https://www.ncbi.nlm.nih.gov/pubmed/32929094
http://dx.doi.org/10.1038/s41467-020-18322-x
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author Sun, Yafei
Cao, Yueqiang
Wang, Lili
Mu, Xiaotong
Zhao, Qingfei
Si, Rui
Zhu, Xiaojuan
Chen, Shangjun
Zhang, Bingsen
Chen, De
Wan, Ying
author_facet Sun, Yafei
Cao, Yueqiang
Wang, Lili
Mu, Xiaotong
Zhao, Qingfei
Si, Rui
Zhu, Xiaojuan
Chen, Shangjun
Zhang, Bingsen
Chen, De
Wan, Ying
author_sort Sun, Yafei
collection PubMed
description Supported gold nanoparticles are emerging catalysts for heterogeneous catalytic reactions, including selective hydrogenation. The traditionally used supports such as silica do not favor the heterolytic dissociation of hydrogen on the surface of gold, thus limiting its hydrogenation activity. Here we use gold catalyst particles partially embedded in the pore walls of mesoporous carbon with carbon atoms occupying interstitial sites in the gold lattice. This catalyst allows improved electron transfer from carbon to gold and, when used for the chemoselective hydrogenation of 3-nitrostyrene, gives a three times higher turn-over frequency (TOF) than that for the well-established Au/TiO(2) system. The d electron gain of Au is linearly related to the activation entropy and TOF. The catalyst is stable, and can be recycled ten times with negligible loss of both reaction rate and overall conversion. This strategy paves the way for optimizing noble metal catalysts to give an enhanced hydrogenation catalytic performance.
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spelling pubmed-74903442020-09-25 Gold catalysts containing interstitial carbon atoms boost hydrogenation activity Sun, Yafei Cao, Yueqiang Wang, Lili Mu, Xiaotong Zhao, Qingfei Si, Rui Zhu, Xiaojuan Chen, Shangjun Zhang, Bingsen Chen, De Wan, Ying Nat Commun Article Supported gold nanoparticles are emerging catalysts for heterogeneous catalytic reactions, including selective hydrogenation. The traditionally used supports such as silica do not favor the heterolytic dissociation of hydrogen on the surface of gold, thus limiting its hydrogenation activity. Here we use gold catalyst particles partially embedded in the pore walls of mesoporous carbon with carbon atoms occupying interstitial sites in the gold lattice. This catalyst allows improved electron transfer from carbon to gold and, when used for the chemoselective hydrogenation of 3-nitrostyrene, gives a three times higher turn-over frequency (TOF) than that for the well-established Au/TiO(2) system. The d electron gain of Au is linearly related to the activation entropy and TOF. The catalyst is stable, and can be recycled ten times with negligible loss of both reaction rate and overall conversion. This strategy paves the way for optimizing noble metal catalysts to give an enhanced hydrogenation catalytic performance. Nature Publishing Group UK 2020-09-14 /pmc/articles/PMC7490344/ /pubmed/32929094 http://dx.doi.org/10.1038/s41467-020-18322-x Text en © The Author(s) 2020 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
Sun, Yafei
Cao, Yueqiang
Wang, Lili
Mu, Xiaotong
Zhao, Qingfei
Si, Rui
Zhu, Xiaojuan
Chen, Shangjun
Zhang, Bingsen
Chen, De
Wan, Ying
Gold catalysts containing interstitial carbon atoms boost hydrogenation activity
title Gold catalysts containing interstitial carbon atoms boost hydrogenation activity
title_full Gold catalysts containing interstitial carbon atoms boost hydrogenation activity
title_fullStr Gold catalysts containing interstitial carbon atoms boost hydrogenation activity
title_full_unstemmed Gold catalysts containing interstitial carbon atoms boost hydrogenation activity
title_short Gold catalysts containing interstitial carbon atoms boost hydrogenation activity
title_sort gold catalysts containing interstitial carbon atoms boost hydrogenation activity
topic Article
url https://www.ncbi.nlm.nih.gov/pmc/articles/PMC7490344/
https://www.ncbi.nlm.nih.gov/pubmed/32929094
http://dx.doi.org/10.1038/s41467-020-18322-x
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