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Precisely Engineered Supported Gold Clusters as a Stable Catalyst for Propylene Epoxidation

Kapil, N; Weissenberger, T; Cardinale, F; Trogadas, P; Nijhuis, TA; Nigra, MM; Coppens, M-O; (2021) Precisely Engineered Supported Gold Clusters as a Stable Catalyst for Propylene Epoxidation. Angewandte Chemie International Edition 10.1002/anie.202104952. (In press). Green open access

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Abstract

Designing a stable and selective catalyst with high H2 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 O2 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.

Type: Article
Title: Precisely Engineered Supported Gold Clusters as a Stable Catalyst for Propylene Epoxidation
Location: Germany
Open access status: An open access version is available from UCL Discovery
DOI: 10.1002/anie.202104952
Publisher version: https://doi.org/10.1002/anie.202104952
Language: English
Additional information: © 2021 The Authors. Angewandte Chemie International Edition published by Wiley-VCH GmbH This is an open access article under the terms of the Creative Commons Attribution License, which permits use, distribution and reproduction in any medium, provided the original work is properly cited.
Keywords: catalyst stability, epoxidation, gold, heterogeneous catalysis, propylene
UCL classification: UCL
UCL > Provost and Vice Provost Offices > UCL BEAMS
UCL > Provost and Vice Provost Offices > UCL BEAMS > Faculty of Engineering Science
UCL > Provost and Vice Provost Offices > UCL BEAMS > Faculty of Engineering Science > Dept of Chemical Engineering
URI: https://discovery.ucl.ac.uk/id/eprint/10131299
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