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Subnanometre PtSn alloyed clusters encapsulated in silicalite-1 sustain high productivity in propane dehydrogenation

Nature Catalysis (2026) Cite this article

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Abstract

Propane dehydrogenation (PDH) processes typically operate at low weight-hourly space velocities of about 10 h−1 to ensure catalyst stability, limiting propylene productivity to around 0.1 molC3H6 gcatalyst−1 h−1. Here we report that controlling the formation of subnanometre PtSn alloyed clusters encapsulated in silicalite-1 affords a catalyst that can sustain high propylene productivities. At 165 h−1, the catalyst achieved about 1 molC3H6 gcatalyst−1 h−1 for more than 300 hours, with >99% propylene selectivity. Furthermore, the spent catalyst can be effectively regenerated using simple air calcination. Detailed characterization and computational modelling attribute the high PDH performance to the distinctive electronic structures of the Pt sites within subnanometre alloyed clusters. The dynamic structures of these subnanometre alloyed clusters probably allow these Pt sites to access a broader range of electronic and structural configurations, expanding the reaction’s accessible energy landscape and effectively breaking the longstanding trade-off between productivity and stability that constrains conventional PDH catalysts.

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Fig. 1: Electron microscopy imaging and analysis of Pt1Sn1(II)@S-1.
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Fig. 2: XAFS spectroscopy characterization of the catalysts studied.
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Fig. 3: PDH performance of Pt1Sn1(II)@S-1 along with its counterparts.
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Fig. 4: Benchmarking Pt1Sn1(II)@S-1 against state-of-the-art PDH catalysts.
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Fig. 5: Modelling of the encapsulated 4Pt4Sn, MD snapshots and the corresponding projected density of states.
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Fig. 6: DFT-derived free-energy diagrams for the PDH process on different subnanometre clusters.
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Data availability

The data supporting the findings of this study are available via Figshare at https://doi.org/10.6084/m9.figshare.31743865 (ref. 69) or from the corresponding authors upon request.

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Acknowledgements

We thank S. Shi and J. Chen from National University of Singapore for help with preparation of XPS PtSn reference sample. We thank C. Wu from Sichuan University for help with EXAFS fitting analysis. We thank Y. Wang (Washington State University and Pacific Northwest National Laboratory, USA), F. Xiao (Zhejiang University, China), J. Li (Tsinghua University, China) and S. Furukawa (The University of Osaka, Japan) for helpful discussions and suggestions regarding this work. S.L. dedicates this work to the memory of one of his best friends, K. Chen. Funding: this work is supported by the Singapore National Research Foundation under grant award no. NRF-NRFF11-2019-0002 and the Singapore Low-Carbon Energy Research Funding Initiative hosted under A*STAR (grant award nos. U2102d2005, U2102d2006 and U2305d4003). Y.T. and G.L. were supported by the fund of Guangdong Provincial Key Laboratory of Computational Science and Material Design (grant no. 2019B030301001), high-level special funds of Southern University of Science and Technology (grant no. G03050K002) and the National Foundation of Natural Science, China (grant no. 52273226). All DFT calculations were carried out on the Taiyi cluster supported by the Center for Computational Science and Engineering of Southern University of Science and Technology. This research is supported by AISI-NUS Joint Research Initiative Fund (grant no. A-8003323-00-00). This research used 7-BM of the National Synchrotron Light Source II, a US Department of Energy (DOE) Office of Science User Facility operated for the DOE Office of Science by BNL under contract no. DE-SC0012704.

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  1. These authors contributed equally: Shangchen Lu, Yaxin Tang, Bingqing Yao.

Authors and Affiliations

  1. Department of Materials Science and Engineering, College of Design and Engineering, National University of Singapore, Singapore, Singapore

    Shangchen Lu, Yaxin Tang, Bingqing Yao, Chaokai Xu, Yankun Du, Shengdong Tan, Binbin Zhao, Wenhao Yuan & Qian He

  2. State Key Laboratory of Quantum Functional Materials, Department of Materials Science and Engineering, Southern University of Science and Technology, Shenzhen, Guangdong, China

    Yaxin Tang, Huanhuan Yang & Guangfu Luo

  3. Department of Chemistry, Faculty of Science, National University of Singapore, Singapore, Singapore

    Yishui Ding, Xingjie Fu, Jiong Lu & Wei Chen

  4. Institute of Sustainability for Chemicals, Energy and Environment (ISCE²), Agency for Science, Technology and Research in Singapore (A*STAR), Jurong Island, Singapore

    Shibo Xi

  5. Department of Chemical and Biomolecular Engineering, College of Design and Engineering, National University of Singapore, Singapore, Singapore

    Kang Hui Lim, Sibudjing Kawi & Ning Yan

  6. Thermo Fisher Scientific, Hillsboro, OR, USA

    C. Austin Wade

  7. National Synchrotron Light Source II (NSLS-II), Brookhaven National Laboratory, Upton, NY, USA

    Dali Yang & Lu Ma

  8. Key Laboratory for Advanced Materials and Joint International Research Laboratory of Precision Chemistry and Molecular Engineering, School of Chemistry and Molecular Engineering, East China University of Science and Technology, Shanghai, China

    Sheng Dai

  9. Centre for Hydrogen Innovations, National University of Singapore, Singapore, Singapore

    Ning Yan, Jiong Lu & Qian He

  10. Department of Physics, Faculty of Science, National University of Singapore, Singapore, Singapore

    Wei Chen

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Contributions

S.L. and Q.H. conceived of the project directions and designed the experiments. S.L. conducted the catalyst preparation, catalytic evaluation and sample characterizations. Y.T. conducted the theoretical simulations and drafted the simulation section of the paper under the supervision of G.L. H.Y. and G.L. carried out additional calculations during the review process. B.Y. performed STEM characterizations under the supervision of Q.H. and S.D., conducted the EDS study and drafted the electron microscopy section of the paper. Y.D. conducted the XPS characterization and analysed the data under the supervision of W.C. S.X. conducted the in situ X-ray absorption spectroscopy characterization in the SSLS and analysed the data. K.H.L. conducted the CO chemisorption experiments and data analysis under the supervision of S.K. C.X. and B.Z. constructed the PDH reactor and helped with data analysis. Y.D. helped CO-diffuse reflectance Fourier transform infrared spectroscopy and H2 TPR experiments under the supervision of N.Y. X.F. carried out the ICP-OES analysis of the catalysts under the supervision of J.L. S.T. performed EDS analysis. W.Y. performed HAADF image analysis. C.A.W. contributed to the EDS studies on the Thermo Fisher Spectra Ultra microscope at the Hillsboro NanoPort. L.M. and D.Y. carried out some preliminary in situ and ex situ X-ray absorption spectroscopy studies in the BNL. S.L., Y.T., B.Y., G.L. and Q.H. wrote the paper, which has been reviewed by all authors.

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Correspondence to Guangfu Luo or Qian He.

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Supplementary information

Supplementary Information (download PDF )

Supplementary Figs. 1–53, Notes 1–4 and Tables 1–8.

Supplementary Video 1 (download MOV )

MD simulation showing rapid structural reconstruction of 4Pt4Sn confined in silicalite-1 during PDH.

Supplementary Video 2 (download MP4 )

An animation of the MD simulation of C3H7 dissociating to C3H6 + H on 4Pt4Sn embedded in zeolite.

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Lu, S., Tang, Y., Yao, B. et al. Subnanometre PtSn alloyed clusters encapsulated in silicalite-1 sustain high productivity in propane dehydrogenation. Nat Catal (2026). https://doi.org/10.1038/s41929-026-01538-3

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