Radical-constructed intergrown titanosilicalite interfaces for efficient direct propene epoxidation with H2 and O2

Dong Lin, Xiang Feng (), Yang Xu, Richard J. Lewis (), Xiao Chen, Thomas E. Davies, Samuel Pattisson, Mark Douthwaite, Defu Yin, Qiuming He, Xiuhui Zheng, Chen De, Chaohe Yang and Graham J. Hutchings ()
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Dong Lin: China University of Petroleum
Xiang Feng: China University of Petroleum
Yang Xu: China University of Petroleum
Richard J. Lewis: Cardiff University
Xiao Chen: Tsinghua University
Thomas E. Davies: Cardiff University
Samuel Pattisson: Cardiff University
Mark Douthwaite: Cardiff University
Defu Yin: China University of Petroleum
Qiuming He: China University of Petroleum
Xiuhui Zheng: China University of Petroleum
Chen De: Norwegian University of Science and Technology
Chaohe Yang: China University of Petroleum
Graham J. Hutchings: Cardiff University

Nature Communications, 2025, vol. 16, issue 1, 1-12

Abstract: 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.

Date: 2025
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DOI: 10.1038/s41467-025-60637-0

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