Precisely Engineered Supported Gold Clusters as a Stable Catalyst for Propylene Epoxidation
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 en...
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Veröffentlicht in: | Angewandte Chemie International Edition 2021-08, Vol.60 (33), p.18185-18193 |
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Format: | Artikel |
Sprache: | eng |
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Zusammenfassung: | 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, 31P 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.
A stable and selective Au/TS‐1 catalyst is synthesised for direct gas phase epoxidation of propylene to propylene oxide, a key commodity chemical. The synthesis methodology is highly versatile for obtaining a stable, supported gold catalyst. The stabilising ligands play an important role in providing enhanced stability to the Au nanoparticles. |
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ISSN: | 1433-7851 1521-3773 |
DOI: | 10.1002/anie.202104952 |