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Roll-to-roll synthesis of multielement heterostructured catalysts

Abstract

Heterostructured catalysts are essential for energy conversion and storage. However, scaling up their synthesis while maintaining precise control over diverse components is challenging. Here we introduce the difference in oxidation potential between metals and carbon as a thermodynamic factor for designing multielement heterostructures. A roll-to-roll carbothermal shock technology was developed to achieve one-step synthesis and continuous manufacturing of multielement heterostructured catalysts. A variety of heterostructured catalysts, from single elements to high-entropy alloys, oxides and their combinations, could be synthesized using this method. In addition, kinetic tunability enables precise control over elemental distributions and helps to identify distinct elemental regions to guide the fine-tailoring of heterostructured catalysts. As a proof of concept, we demonstrated rapid screening of PtCo@La–TiO2 for alkaline hydrogen evolution. Our work proposes an advanced technology for rapid synthesis, screening and continuous production of multielement heterostructured catalysts.

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Fig. 1: Roll-to-roll synthesis of heterostructured catalysts.
Fig. 2: Rapid screening and structure characterization of multielement heterostructures.
Fig. 3: HER performance of PtCo@La–TiO2 catalyst.
Fig. 4: Thermodynamic guideline and general synthesis of multielement heterostructures.
Fig. 5: Dynamic tunability and element guideline map of multielement heterostructures.

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Data availability

All the data supporting the conclusions of this study are available within the Article and its Supplementary Information. Source data are provided with this paper.

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Acknowledgements

This work is supported by the National Key R&D Program of China (grant no. 2021YFA1202300), the National Natural Science Foundation of China (grant nos. 22325901, 52371223, 52401280, 52101255 and 52272046), the Beijing National Laboratory for Molecular Sciences (BNLMS202405) and the Fundamental Research Funds for the Central Universities of HUST (grant nos. 2023JCYJ004 and YCJJ20242227). Y.S. acknowledges the ‘Young Talent Support Plan’ of Xi’an Jiaotong University. Supercomputing facilities were provided by Hefei Advanced Computing Center. We thank the test support from the Analytical and Testing Center of Huazhong University of Science and Technology, the State Key Laboratory of Materials Processing, and Die and Mould Technology.

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Authors and Affiliations

Authors

Contributions

Y.Y. and B.Y.X. conceived and designed the project. W.S. synthesized the materials. W.S., H.L., H.Z., L.Z. and K.Y. carried out the electrochemical testing. W.S., Zihui Liang, J.Z., B.Y.X. and Y.Y. contributed to the characterization and related discussion. W.S., F.T., Y.L. and Zihui Liang performed the contact angle measurements. Y.S. and S.S. contributed to the theoretical calculations. J.Z., Y.W, Y.G., D.S. and Zhiqiang Liang. contributed to the STEM measurements. Y.L. designed the roll-to-roll equipment. W.S., H.L., Y.H., B.Y.X. and Y.Y. cowrote and revised the paper. All the authors discussed the results.

Corresponding authors

Correspondence to Bao Yu Xia or Yonggang Yao.

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Nature Synthesis thanks the anonymous reviewers 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

Supplementary Information

Supplementary Figs. 1–59 and Tables 1–7, and references.

Supplementary Movie 1

The roll-to-roll CTS process.

Supplementary Movie 2

The contact angle test of Pt/C electrode under-electrolyte.

Supplementary Movie 3

The contact angle test of Pt electrode under-electrolyte.

Supplementary Movie 4

The contact angle test of PtCo@TiO2 electrode under-electrolyte.

Supplementary Movie 5

The contact angle test of PtCo@La–TiO2 electrode under-electrolyte.

Source data

Source Data Fig. 1

Statistical source data.

Source Data Fig. 2

Statistical source data.

Source Data Fig. 3

Statistical source data.

Source Data Fig. 5

Statistical source data.

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Shi, W., Liu, H., Zhang, J. et al. Roll-to-roll synthesis of multielement heterostructured catalysts. Nat. Synth 4, 836–847 (2025). https://doi.org/10.1038/s44160-025-00758-y

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