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A gold catalyst stabilized in an open-porosity TS-1 zeolite for the direct epoxidation of propylene

Nature Synthesis (2026)Cite this article

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Abstract

Synthesis of hierarchical zeolites has been proven to be an effective strategy for improving reactant accessibility to active sites and extending catalyst lifetimes. Existing synthesis methods typically generate mesopores within zeolite crystallites instead of inside zeolites with an open-structure porosity. Here we have developed a general synthesis method by optimizing the crystallization conditions and molecular structures of the polymer template and linkage reagent, resulting in the formation of hierarchical MFI-, MEL-, BEA- and CHA-type zeolites with open porosity formed by highly interconnected microporous channels. Based on this method, we prepare a hierarchical TS-1 zeolite with open porosity as a support for a gold catalyst. The resultant Au/TS-1 catalyst exhibits high activity and stability for the direct epoxidation of propylene with H2 and O2, which is associated with the intimate contact between the gold and titanium sites and the zeolite’s unique pore structure.

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Fig. 1: Challenges in catalyst design for direct epoxidation of propylene with H2 and O2.
Fig. 2: Electron microscopy characterization of the TS-1 zeolite materials and Au/TS-1 catalysts.
Fig. 3: High-resolution electron microscopy characterizations of Au/TS samples with different morphologies.
Fig. 4: Three-dimensional structural characterization of Au/TS samples by electron tomography.
Fig. 5: Spectroscopy characterization of various Au/TS-1 materials.
Fig. 6: Formation mechanism of hierarchical zeolites with open porosity.
Fig. 7: Catalytic performance of Au/TS-1 catalysts for direct epoxidation of propylene.

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All data supporting this study are included within the article or its Supplementary Information. Source data are provided with this paper.

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Acknowledgements

L.L. and Q.-M.W. thank the National Key R&D Program of China for financial support (2022YFA1503901). L.L. thanks the National Natural Science Foundation of China for financial support (92477122, 22272087). M.L.-H. thanks PID2022-142312NB-I00 funding by MCIN/AEI/10.13039/50110001103 and by “ERDF A way of making Europe” for financial support. The in situ XANES experiments were performed at the NOTOS BL16 beamline at ALBA Synchrotron with the collaboration of ALBA staff. We thank Y. Li for preparing the cross-section slice of zeolite materials by ultramicrotomy.

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Authors and Affiliations

  1. Engineering Research Center of Advanced Rare-Earth Materials of Ministry of Education, Department of Chemistry, Tsinghua University, Beijing, China

    Feng He, Xiaomeng Dou, Quan-Ming Wang & Lichen Liu

  2. Departamento de Ciencia de los Materiales e Ingeniería Metalúrgica y Química Inorgánica, Facultad de Ciencias, Universidad de Cádiz, Puerto Real, Spain

    Miguel Lopez-Haro

  3. Department of Applied Biology and Chemical Technology and Research Institute for Smart Energy, The Hong Kong Polytechnic University, Hong Kong, China

    Tianxiang Chen

  4. ALBA Synchrotron Light Source, Barcelona, Spain

    Carlo Marini

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  1. Feng He
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Contributions

L.L. conceived the project. F.H. carried out the materials synthesis and the structural characterizations. M.L.-H. carried out the 3D structural analysis of the Au–zeolite samples. T.C. and C.M. conducted the in situ XAS measurements and analysed the data. X.D. contributed to the catalytic tests of the direct epoxidation reaction. Q.-M.W. contributed to the experiment design, data analysis and manuscript revision. L.L. wrote the manuscript with input from all the other authors.

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Correspondence to Quan-Ming Wang or Lichen Liu.

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Nature Synthesis thanks Changbum Jo, James W. Harris and Grandprix T. M. Kadja for their contribution to the peer review of this work. Primary Handling Editor: Alexandra Groves, in collaboration with the Nature Synthesis team

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Supplementary information

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Supplementary Methods, Figs. 1–141 and Tables 1–4.

Supplementary Video 1 (download MP4 )

Reconstructed 3D structure of Au/TS-GPI sample.

Supplementary Video 2 (download MP4 )

Reconstructed 3D structure of Au/TS-NaOH sample.

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Statistical source data.

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He, F., Lopez-Haro, M., Chen, T. et al. A gold catalyst stabilized in an open-porosity TS-1 zeolite for the direct epoxidation of propylene. Nat. Synth (2026). https://doi.org/10.1038/s44160-025-00988-0

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