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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...
Autores principales: | , , , , , , , , , , , , , |
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Formato: | Online Artículo Texto |
Lenguaje: | English |
Publicado: |
Nature Publishing Group UK
2019
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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. |
format | Online Article Text |
id | pubmed-6385229 |
institution | National Center for Biotechnology Information |
language | English |
publishDate | 2019 |
publisher | Nature Publishing Group UK |
record_format | MEDLINE/PubMed |
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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