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説明:

High-entropy alloys (HEAs) have recently emerged as promising electrocatalysts for complex reactions owing to their tunable electronic structures and diverse, unique binding sites. However, their vast compositional space, in terms of both elemental variety and atomic ratios, presents a major challenge to the rational design of high-performance catalysts, as experimental efforts are often hindered by ambiguous element selection and inefficient trial-and-error methods. In this work, a bottom-up research strategy using machine learning-assisted first-principles calculations was applied to accelerate the design of quinary HEAs toward efficient multielectron transfer reactions. Here, we report the design of PtPdRhRuMo, which exhibits key physicochemical properties favoring the methanol oxidation reaction. Notably, the incorporation of Mo as the fifth element significantly activates specific binding sites on HEA surfaces, enhancing methanol adsorption and, in particular, the water dissociation ability. This facilitates hydroxyl species formation, which effectively mitigates CO intermediate adherence while promoting the complete oxidation of CH3OH to CO2 via alternative reaction pathways. Guided by theoretical predictions, experimental samples with different morphologies of mesoporous PtPdRhRuMo catalyst (m-HEANP(Mo) nanoparticles and m-HEAF(Mo) thin film) were then synthesized, demonstrating superior electrocatalysis with a large current density of up to 18.20 mA cm^–2 and a mass activity of 9.89 A mgPt^–1, alongside the long-term durability for efficient methanol electrooxidation applications.

権利情報:

• In Copyright
  

  This document is the Accepted Manuscript version of a Published Work that appeared in final form in Journal of the American Chemical Society, copyright © 2025 American Chemical Society after peer review and technical editing by the publisher. To access the final edited and published work see https://doi.org/10.1021/jacs.5c08012.

キーワード: High entropy alloys, Electrocatalysis, Materials Informatics, Mesoporous Metal

刊行年月日: 2025-09-17

出版者: American Chemical Society (ACS)

掲載誌:

• Journal of the American Chemical Society (ISSN: 00027863) vol. 147 issue. 37 p. 33545-33558

研究助成金:

• Exploratory Research for Advanced Technology JPMJER2003
• Australian Research Council FL230100095
• Japan Society for the Promotion of Science 24H00449
• Japan Society for the Promotion of Science 24K17694
• Hibi Science and Technology Foundation FY2025
• Japan Society for the Promotion of Science P220632

原稿種別: 著者最終稿 (Accepted manuscript)

MDR DOI: https://doi.org/10.48505/nims.5797

公開URL: https://doi.org/10.1021/jacs.5c08012

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更新時刻: 2026-02-16 18:37:28 +0900

MDRでの公開時刻: 2026-09-03 08:27:23 +0900