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Self- regeneration of Au/CeO(2) based catalysts with enhanced activity and ultra-stability for acetylene hydrochlorination

Replacement of Hg with non-toxic Au based catalysts for industrial hydrochlorination of acetylene to vinyl chloride is urgently required. However Au catalysts suffer from progressive deactivation caused by auto-reduction of Au(I) and Au(III) active sites and irreversible aggregation of Au(0) inactiv...

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Autores principales: Ye, Lin, Duan, Xinping, Wu, Simson, Wu, Tai-Sing, Zhao, Yuxin, Robertson, Alex W., Chou, Hung-Lung, Zheng, Jianwei, Ayvalı, Tuğçe, Day, Sarah, Tang, Chiu, Soo, Yun-Liang, Yuan, Youzhu, Tsang, Shik Chi Edman
Formato: Online Artículo Texto
Lenguaje:English
Publicado: Nature Publishing Group UK 2019
Materias:
Acceso en línea:https://www.ncbi.nlm.nih.gov/pmc/articles/PMC6385229/
https://www.ncbi.nlm.nih.gov/pubmed/30796236
http://dx.doi.org/10.1038/s41467-019-08827-5
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author Ye, Lin
Duan, Xinping
Wu, Simson
Wu, Tai-Sing
Zhao, Yuxin
Robertson, Alex W.
Chou, Hung-Lung
Zheng, Jianwei
Ayvalı, Tuğçe
Day, Sarah
Tang, Chiu
Soo, Yun-Liang
Yuan, Youzhu
Tsang, Shik Chi Edman
author_facet Ye, Lin
Duan, Xinping
Wu, Simson
Wu, Tai-Sing
Zhao, Yuxin
Robertson, Alex W.
Chou, Hung-Lung
Zheng, Jianwei
Ayvalı, Tuğçe
Day, Sarah
Tang, Chiu
Soo, Yun-Liang
Yuan, Youzhu
Tsang, Shik Chi Edman
author_sort Ye, Lin
collection PubMed
description Replacement of Hg with non-toxic Au based catalysts for industrial hydrochlorination of acetylene to vinyl chloride is urgently required. However Au catalysts suffer from progressive deactivation caused by auto-reduction of Au(I) and Au(III) active sites and irreversible aggregation of Au(0) inactive sites. Here we show from synchrotron X-ray absorption, STEM imaging and DFT modelling that the availability of ceria(110) surface renders Au(0)/Au(I) as active pairs. Thus, Au(0) is directly involved in the catalysis. Owing to the strong mediating properties of Ce(IV)/Ce(III) with one electron complementary redox coupling reactions, the ceria promotion to Au catalysts gives enhanced activity and stability. Total pre-reduction of Au species to inactive Au nanoparticles of Au/CeO(2)&AC when placed in a C(2)H(2)/HCl stream can also rapidly rejuvenate. This is dramatically achieved by re-dispersing the Au particles to Au(0) atoms and oxidising to Au(I) entities, whereas Au/AC does not recover from the deactivation.
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spelling pubmed-63852292019-02-25 Self- regeneration of Au/CeO(2) based catalysts with enhanced activity and ultra-stability for acetylene hydrochlorination Ye, Lin Duan, Xinping Wu, Simson Wu, Tai-Sing Zhao, Yuxin Robertson, Alex W. Chou, Hung-Lung Zheng, Jianwei Ayvalı, Tuğçe Day, Sarah Tang, Chiu Soo, Yun-Liang Yuan, Youzhu Tsang, Shik Chi Edman Nat Commun Article Replacement of Hg with non-toxic Au based catalysts for industrial hydrochlorination of acetylene to vinyl chloride is urgently required. However Au catalysts suffer from progressive deactivation caused by auto-reduction of Au(I) and Au(III) active sites and irreversible aggregation of Au(0) inactive sites. Here we show from synchrotron X-ray absorption, STEM imaging and DFT modelling that the availability of ceria(110) surface renders Au(0)/Au(I) as active pairs. Thus, Au(0) is directly involved in the catalysis. Owing to the strong mediating properties of Ce(IV)/Ce(III) with one electron complementary redox coupling reactions, the ceria promotion to Au catalysts gives enhanced activity and stability. Total pre-reduction of Au species to inactive Au nanoparticles of Au/CeO(2)&AC when placed in a C(2)H(2)/HCl stream can also rapidly rejuvenate. This is dramatically achieved by re-dispersing the Au particles to Au(0) atoms and oxidising to Au(I) entities, whereas Au/AC does not recover from the deactivation. Nature Publishing Group UK 2019-02-22 /pmc/articles/PMC6385229/ /pubmed/30796236 http://dx.doi.org/10.1038/s41467-019-08827-5 Text en © The Author(s) 2019 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
Ye, Lin
Duan, Xinping
Wu, Simson
Wu, Tai-Sing
Zhao, Yuxin
Robertson, Alex W.
Chou, Hung-Lung
Zheng, Jianwei
Ayvalı, Tuğçe
Day, Sarah
Tang, Chiu
Soo, Yun-Liang
Yuan, Youzhu
Tsang, Shik Chi Edman
Self- regeneration of Au/CeO(2) based catalysts with enhanced activity and ultra-stability for acetylene hydrochlorination
title Self- regeneration of Au/CeO(2) based catalysts with enhanced activity and ultra-stability for acetylene hydrochlorination
title_full Self- regeneration of Au/CeO(2) based catalysts with enhanced activity and ultra-stability for acetylene hydrochlorination
title_fullStr Self- regeneration of Au/CeO(2) based catalysts with enhanced activity and ultra-stability for acetylene hydrochlorination
title_full_unstemmed Self- regeneration of Au/CeO(2) based catalysts with enhanced activity and ultra-stability for acetylene hydrochlorination
title_short Self- regeneration of Au/CeO(2) based catalysts with enhanced activity and ultra-stability for acetylene hydrochlorination
title_sort self- regeneration of au/ceo(2) based catalysts with enhanced activity and ultra-stability for acetylene hydrochlorination
topic Article
url https://www.ncbi.nlm.nih.gov/pmc/articles/PMC6385229/
https://www.ncbi.nlm.nih.gov/pubmed/30796236
http://dx.doi.org/10.1038/s41467-019-08827-5
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