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Precisely Engineered Supported Gold Clusters as a Stable Catalyst for Propylene Epoxidation
Designing a stable and selective catalyst with high H(2) utilisation is of pivotal importance for the direct gas‐phase epoxidation of propylene. This work describes a facile one‐pot methodology to synthesise ligand‐stabilised sub‐nanometre gold clusters immobilised onto a zeolitic support (TS‐1) to...
Autores principales: | , , , , , , |
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Formato: | Online Artículo Texto |
Lenguaje: | English |
Publicado: |
John Wiley and Sons Inc.
2021
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Materias: | |
Acceso en línea: | https://www.ncbi.nlm.nih.gov/pmc/articles/PMC8456944/ https://www.ncbi.nlm.nih.gov/pubmed/34085370 http://dx.doi.org/10.1002/anie.202104952 |
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author | Kapil, Nidhi Weissenberger, Tobias Cardinale, Fabio Trogadas, Panagiotis Nijhuis, T. Alexander Nigra, Michael M. Coppens, Marc‐Olivier |
author_facet | Kapil, Nidhi Weissenberger, Tobias Cardinale, Fabio Trogadas, Panagiotis Nijhuis, T. Alexander Nigra, Michael M. Coppens, Marc‐Olivier |
author_sort | Kapil, Nidhi |
collection | PubMed |
description | Designing a stable and selective catalyst with high H(2) utilisation is of pivotal importance for the direct gas‐phase epoxidation of propylene. This work describes a facile one‐pot methodology to synthesise ligand‐stabilised sub‐nanometre gold clusters immobilised onto a zeolitic support (TS‐1) to engineer a stable Au/TS‐1 catalyst. A non‐thermal O(2) plasma technique is used for the quick removal of ligands with limited increase in particle size. Compared to untreated Au/TS‐1 catalysts prepared using the deposition precipitation method, the synthesised catalyst exhibits improved catalytic performance, including 10 times longer lifetime (>20 days), increased PO selectivity and hydrogen efficiency in direct gas phase epoxidation. The structure‐stability relationship of the catalyst is illustrated using multiple characterisation techniques, such as XPS, (31)P MAS NMR, DR‐UV/VIS, HRTEM and TGA. It is hypothesised that the ligands play a guardian role in stabilising the Au particle size, which is vital in this reaction. This strategy is a promising approach towards designing a more stable heterogeneous catalyst. |
format | Online Article Text |
id | pubmed-8456944 |
institution | National Center for Biotechnology Information |
language | English |
publishDate | 2021 |
publisher | John Wiley and Sons Inc. |
record_format | MEDLINE/PubMed |
spelling | pubmed-84569442021-09-27 Precisely Engineered Supported Gold Clusters as a Stable Catalyst for Propylene Epoxidation Kapil, Nidhi Weissenberger, Tobias Cardinale, Fabio Trogadas, Panagiotis Nijhuis, T. Alexander Nigra, Michael M. Coppens, Marc‐Olivier Angew Chem Int Ed Engl Research Articles Designing a stable and selective catalyst with high H(2) utilisation is of pivotal importance for the direct gas‐phase epoxidation of propylene. This work describes a facile one‐pot methodology to synthesise ligand‐stabilised sub‐nanometre gold clusters immobilised onto a zeolitic support (TS‐1) to engineer a stable Au/TS‐1 catalyst. A non‐thermal O(2) plasma technique is used for the quick removal of ligands with limited increase in particle size. Compared to untreated Au/TS‐1 catalysts prepared using the deposition precipitation method, the synthesised catalyst exhibits improved catalytic performance, including 10 times longer lifetime (>20 days), increased PO selectivity and hydrogen efficiency in direct gas phase epoxidation. The structure‐stability relationship of the catalyst is illustrated using multiple characterisation techniques, such as XPS, (31)P MAS NMR, DR‐UV/VIS, HRTEM and TGA. It is hypothesised that the ligands play a guardian role in stabilising the Au particle size, which is vital in this reaction. This strategy is a promising approach towards designing a more stable heterogeneous catalyst. John Wiley and Sons Inc. 2021-07-09 2021-08-09 /pmc/articles/PMC8456944/ /pubmed/34085370 http://dx.doi.org/10.1002/anie.202104952 Text en © 2021 The Authors. Angewandte Chemie International Edition published by Wiley-VCH GmbH https://creativecommons.org/licenses/by/4.0/This is an open access article under the terms of the http://creativecommons.org/licenses/by/4.0/ (https://creativecommons.org/licenses/by/4.0/) License, which permits use, distribution and reproduction in any medium, provided the original work is properly cited. |
spellingShingle | Research Articles Kapil, Nidhi Weissenberger, Tobias Cardinale, Fabio Trogadas, Panagiotis Nijhuis, T. Alexander Nigra, Michael M. Coppens, Marc‐Olivier Precisely Engineered Supported Gold Clusters as a Stable Catalyst for Propylene Epoxidation |
title | Precisely Engineered Supported Gold Clusters as a Stable Catalyst for Propylene Epoxidation |
title_full | Precisely Engineered Supported Gold Clusters as a Stable Catalyst for Propylene Epoxidation |
title_fullStr | Precisely Engineered Supported Gold Clusters as a Stable Catalyst for Propylene Epoxidation |
title_full_unstemmed | Precisely Engineered Supported Gold Clusters as a Stable Catalyst for Propylene Epoxidation |
title_short | Precisely Engineered Supported Gold Clusters as a Stable Catalyst for Propylene Epoxidation |
title_sort | precisely engineered supported gold clusters as a stable catalyst for propylene epoxidation |
topic | Research Articles |
url | https://www.ncbi.nlm.nih.gov/pmc/articles/PMC8456944/ https://www.ncbi.nlm.nih.gov/pubmed/34085370 http://dx.doi.org/10.1002/anie.202104952 |
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