Radical-constructed intergrown titanosilicalite interfaces for efficient direct propene epoxidation with H 2 and O 2

Lin, Dong, Feng, Xiang, Xu, Yang, Lewis, Richard J., Chen, Xiao, Davies, Thomas E., Pattisson, Samuel, Douthwaite, Mark, Yin, Defu, He, Qiuming, Zheng, Xiuhui, Chen, De, Yang, Chaohe and Hutchings, Graham J. ORCID: https://orcid.org/0000-0001-8885-1560 2025. Radical-constructed intergrown titanosilicalite interfaces for efficient direct propene epoxidation with H 2 and O 2. Nature Communications 16 (1) , 5515. 10.1038/s41467-025-60637-0

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Abstract

The development of titianosilicates is considered a major milestone in oxidative catalysis due to the ability of framework Ti sites to co-ordinate hydrogen peroxide/peroxy species. Herein, we demonstrate that interfacial Ti sites can be constructed through the vertical intergrowth of two MFI-type zeolite surfaces along [100] and [010] projections, with the assistance of UV-induced hydroxyl radicals. The application of these intergrown titanosilicalites as supports for Au species are observed to simultaneously offer a 2.1-fold and 3.0-fold increase in propene oxide (PO) formation rate and Au efficiency, respectively, when compared to standard Au/TS-1 catalysts. Mechanistic studies reveal that the intergrown interface Ti sites allow for lower-energy epoxidation pathways with more efficient activation of key oxygen-transfer intermediates. These results provide insights into the development of zeolite intergrown interface sites (e.g., titanosilicalite/silicalite-1/ZSM-5) and may allow for further advancements in the epoxidation of a range of key feedstocks.

Item Type:	Article
Date Type:	Published Online
Status:	Published
Schools:	Schools > Chemistry Research Institutes & Centres > Cardiff Catalysis Institute (CCI)
Additional Information:	License information from Publisher: LICENSE 1: URL: http://creativecommons.org/licenses/by/4.0/, Type: open-access
Publisher:	Nature Research
ISSN:	2041-1723
Date of First Compliant Deposit:	7 July 2025
Date of Acceptance:	30 May 2025
Last Modified:	07 Jul 2025 13:15
URI:	https://orca.cardiff.ac.uk/id/eprint/179595

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