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Finely tailoring the local ensembles in heterostructured high entropy alloy catalysts through pulsed annealing

Author

Listed:
  • Kaizhu Zeng

    (Huazhong University of Science and Technology)

  • Rong Hu

    (Huazhong University of Science and Technology)

  • Jianwei Zhang

    (Soochow University)

  • Xin Li

    (Jilin University)

  • Yifan Xu

    (Nanyang Technological University)

  • Xilong Mu

    (Peking University)

  • Hao Wu

    (Jilin University)

  • Shijing Liu

    (Huazhong University of Science and Technology)

  • Hanwen Liu

    (Huazhong University of Science and Technology)

  • Jinli Chen

    (Huazhong University of Science and Technology)

  • Zhiqiang Wang

    (Huazhong University of Science and Technology)

  • Jihan Zhou

    (Peking University)

  • Zhiqiang Liang

    (Soochow University)

  • Wang Gao

    (Jilin University)

  • Dongshuang Wu

    (Nanyang Technological University)

  • Yonggang Yao

    (Huazhong University of Science and Technology)

Abstract

High-entropy alloys (HEAs) are promising catalysts particularly adept for reactions involving multiple intermediates and requiring multifunctional active sites. However, conventional syntheses often result in either (kinetically) random-mixing HEA or (thermodynamically) phase-separated composites-both fail to fine-tune local structures and further optimizing their performances. Here we present finely tailoring the local ensembles in HEA catalysts through rational composition design and sequential pulsed annealing. Employing PdSnFeCoNi HEA as a model, pulsed annealing (e.g., 0.5 s heating at 1300 K for 30 cycles) leverages differences in enthalpic interactions and surface energies to control the formation of ultrafine PdSn clusters within the HEA matrix, yielding the heterostructured HEA/c-PdSn. Compared with random HEAs and commercial Pd/C, HEA/c-PdSn exhibits >5 − 10-fold higher mass activity and good stability (>90.6% retention after 2000 cycles) for ethanol oxidation. This enhancement arises from the synergy between active local ensembles and the multifunctional HEA matrix, which reduces overall limiting potential, mitigates sluggish C-C/C-H breaking, and enhances structural stabilization. Our findings provide a strategy for engineering heterostructured HEAs for broad catalytic applications.

Suggested Citation

  • Kaizhu Zeng & Rong Hu & Jianwei Zhang & Xin Li & Yifan Xu & Xilong Mu & Hao Wu & Shijing Liu & Hanwen Liu & Jinli Chen & Zhiqiang Wang & Jihan Zhou & Zhiqiang Liang & Wang Gao & Dongshuang Wu & Yongga, 2025. "Finely tailoring the local ensembles in heterostructured high entropy alloy catalysts through pulsed annealing," Nature Communications, Nature, vol. 16(1), pages 1-11, December.
  • Handle: RePEc:nat:natcom:v:16:y:2025:i:1:d:10.1038_s41467-025-58495-x
    DOI: 10.1038/s41467-025-58495-x
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    References listed on IDEAS

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