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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...

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Autores principales: Kapil, Nidhi, Weissenberger, Tobias, Cardinale, Fabio, Trogadas, Panagiotis, Nijhuis, T. Alexander, Nigra, Michael M., Coppens, Marc‐Olivier
Formato: Online Artículo Texto
Lenguaje:English
Publicado: John Wiley and Sons Inc. 2021
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.
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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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