Finely tailoring the local ensembles in heterostructured high entropy alloy catalysts through pulsed annealing
Open accessAbstract
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. Local structure control is challenging in high entropy alloy (HEA) catalysts. Here, the authors report finely tailoring the local clustering in HEA catalysts through rational composition design and sequential pulse annealing, achieving enhanced activity and stability for ethanol electrooxidation.
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Although HEAs provide diverse surface atomic configurations that can in principle enhance catalytic performance, their intrinsic heterogeneity also introduces limitations.
“Although HEAs provide diverse surface atomic config- urations that can in principle enhance catalytic performance, their intrinsic heterogeneity also introduces limitations.30,60”
From High-Entropy Alloy Aerogels with High-Density Solid–Solid Heterointerfaces for Alkaline Hydrogen Evolution (2026) · cites this paper as [60]
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- Authors
- Zeng, K., Hu, R., Zhang, J., Li, X., Xu, Y., Mu, X., Wu, H., Liu, S., Liu, H., Chen, J., Wang, Z., Zhou, J., Liang, Z., Gao, W., Wu, D., & Yao, Y.
- Affiliations
- State Key Laboratory of Materials Processing and Die & Mould Technology (CN)
- Soochow University (CN)
- Jilin University (CN)
- Nanyang Technological University (SG)
- Peking University (CN)
- Huazhong University of Science and Technology (CN)
- Corresponding author
- Wang, Zhiqiang
- Liang, Zhiqiang
- Gao, Wang
- Wu, Dongshuang
- Yao, Yonggang
- ORCID
- Venue
- Nature Communications
- Published
- 2025-04-10
- Volume
- 16
- Issue
- 1
- Pages
- 3403-3403
- ISSN
- 2041-1723 (ISSN-L)
- PMC
- PMC11985931
- OpenAlex
- W4409318139
- Cited by
- 58
- References
- 60
- Citations by year
- 2026: 38 · 2025: 20
- FWCI
- 8.01
- Type
- journal article
- Language
- en
- Open access
- gold
- doi.org
- Licence
- Locations
- Nature Communications (publishedVersion, cc-by-nc-nd)
- PubMed Central (publishedVersion, cc-by-nc-nd)
- PubMed (publishedVersion)
- DR-NTU (Nanyang Technological University) (publishedVersion, cc-by-nc-nd)
- RePEc: Research Papers in Economics (submittedVersion)
- DOAJ (DOAJ: Directory of Open Access Journals) (submittedVersion, cc-by-sa)
- Funders
- Australian Cancer Research Foundation
- National Research Foundation Singapore (AS232/XAS/20067)
- Ministry of Education - Singapore (Tier 1, AcRF-Tier 1, AcRF‐Tier2, RG81/22, MOE-T2EP10123-0003, Tier 2)
- National Natural Science Foundation of China (22173034, 52101255, 52371223)
- Ministry of Education, India
- Collaborative Innovation Center of Suzhou Nano Science and Technology
- Beijing National Laboratory for Molecular Sciences (BNLMS202405)
- Topics
- Physical Sciences › Energy › Renewable Energy, Sustainability and the Environment › Electrocatalysts for Energy Conversion
- Physical Sciences › Engineering › Mechanical Engineering › High Entropy Alloys Studies
- Physical Sciences › Materials Science › Materials Chemistry › Catalytic Processes in Materials Science
- Keywords
- high-entropy alloys, heterostructured catalysts, ethanol electrooxidation, compositional design, phase separation, catalyst stability, electrocatalysis
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