# Modeling-Making-Modulating High-Entropy Alloy with Activated Water-Dissociation Centers for Superior Electrocatalysis https://mdr.nims.go.jp/datasets/40463459-52f5-4be1-bf40-8efbd5991377 ## File - [manuscript.pdf](https://mdr.nims.go.jp/filesets/329411ac-442f-4caa-839f-f3347d0324f3/download) ([Detail](https://mdr.nims.go.jp/filesets/329411ac-442f-4caa-839f-f3347d0324f3.md)) ## Id 40463459-52f5-4be1-bf40-8efbd5991377 ## Local identifier ## Visibility open_to_public ## State published ## Created at 2025-10-07T23:56:22.532642Z ## Updated at 2026-02-16T09:37:28.774993Z ## Published at 2026-09-02T23:27:23.609033Z ## Doi https://doi.org/10.48505/nims.5797 ## First published url https://doi.org/10.1021/jacs.5c08012 ## Date published 2025-09-17 ## Recorded date published 2025-9-17 ## Resource type journal_article ## Manuscript type accepted_manuscript ## Collection ## Title - title: Modeling-Making-Modulating High-Entropy Alloy with Activated Water-Dissociation Centers for Superior Electrocatalysis title_type: original lang: en ## Description - description: 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. description_type: abstract lang: und ## Creator - name: Ho Ngoc Nam role: author - name: Ravi Nandan role: author organization: National Institute for Materials Science - name: Lei Fu role: author - name: Yingji Zhao role: author - name: Yunqing Kang role: author - name: Tetsuya Fukushima role: author - name: Kazunori Sato role: author - name: Yusuke Asakura role: author - name: Ovidiu Cretu role: author orcid: https://orcid.org/0000-0002-1822-8172 organization: National Institute for Materials Science - name: Jun Kikkawa role: author orcid: https://orcid.org/0000-0003-0659-1844 organization: National Institute for Materials Science - name: Joel Henzie role: author orcid: https://orcid.org/0000-0002-9190-2645 organization: National Institute for Materials Science - name: Jonathan P. Hill role: author orcid: https://orcid.org/0000-0002-4229-5842 organization: National Institute for Materials Science - name: Takeshi Yanai role: author - name: Quan Manh Phung role: author - name: Yusuke Yamauchi role: author ## Contact agent ## Publisher organization: American Chemical Society (ACS) ## Managing organization ## Keyword - subject: High entropy alloys schema: not_defined - subject: Electrocatalysis schema: not_defined - subject: Materials Informatics schema: not_defined - subject: Mesoporous Metal schema: not_defined ## Rights - description: 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. identifier: http://rightsstatements.org/vocab/InC/1.0/ ## Other identifier(s) ## Data origin - data_origin_type: other ## Embargo start_date: 2025-09-03 end_date: 2026-09-03 ## Journal - title: Journal of the American Chemical Society issn: '00027863' volume: '147' issue: '37' start_page: 33545 end_page: 33558 ## Conference ## Related item ## Funding - identifier: JPMJER2003 funder_name: Exploratory Research for Advanced Technology - identifier: FL230100095 funder_name: Australian Research Council - identifier: 24H00449 funder_name: Japan Society for the Promotion of Science - identifier: 24K17694 funder_name: Japan Society for the Promotion of Science - identifier: FY2025 funder_name: Hibi Science and Technology Foundation - identifier: P220632 funder_name: Japan Society for the Promotion of Science ## Instrument ## Instrument operator ## Instrument managing organization ## Measurement method ## Specimen ## Chemical composition ## Structure for specimen ## Structural feature for specimen ## Specific property for specimen ## Process for specimen treatment ## Computational method ## Energy level/transition state ## Software ## Custom property ## Fileset - id: 329411ac-442f-4caa-839f-f3347d0324f3 filename: manuscript.pdf content_type: application/pdf size: 1991667 md5: 4b8669b334a65eeddea21f51e17f4edf ## Thumbnail fileset_id: 329411ac-442f-4caa-839f-f3347d0324f3 filename: manuscript.pdf