Kapil, N; Weissenberger, T; Cardinale, F; Trogadas, P; Nijhuis, TA; Nigra, MM; Coppens, M; (2021) Precisely Engineered Supported Gold Clusters as a Stable Catalyst for Propylene Epoxidation. Angewandte Chemie , 133 (33) pp. 18333-18341. 10.1002/ange.202104952.

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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, 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.

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