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To address these challenges, a mesoporous PtPd\u2010HEO (HEO\u00a0=\u00a0high entropy oxide) heterostructure is assembled in situ from a metal\u2013organic framework (MOF)\u2010derived high entropy alloy (HEA) in this work. Mass activity exceeding that of commercial Pt\/C by more than an order of magnitude is demonstrated by this catalyst. A peak power density of 155\u00a0mW cm\n                    <jats:sup>\u22122<\/jats:sup>\n                    and long\u2010term operational stability are achieved in a DMFC assembled with mesoporous PtPd\u2010HEO, surpassing the performance of cells based on Pt\/C and PtPd\/C. In situ spectroscopic studies combined with density functional theory (DFT) simulations reveal that the valence electronic structure of the PtPd alloy is modulated by the HEO component, resulting in improved selectivity for non\u2010CO pathways and increased formation of reactive hydroxyl species. Superior MOR catalytic activity and durability for PtPd\u2010HEO are attributed to this synergistic electronic tuning and the porous structure. The development of HEO\u2010based mesoporous heterostructures is proposed as a promising strategy for the design of next\u2010generation catalysts in energy conversion and sustainable technologies.\n                  <\/jats:p>","DOI":"10.1002\/anie.202518458","type":"journal-article","created":{"date-parts":[[2025,9,25]],"date-time":"2025-09-25T09:53:37Z","timestamp":1758794017000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":30,"title":["Mesoporous PtPd Alloy \u2010 High Entropy Oxide Heterostructures for Efficient Electrocatalytic Methanol Oxidation Reaction"],"prefix":"10.1002","volume":"64","author":[{"given":"Jing","family":"Yang","sequence":"first","affiliation":[{"name":"Department of Applied Biology and Chemical Technology The Hong Kong Polytechnic University  Hung Hom Hong Kong SAR China"},{"name":"School of Energy and Power Engineering Jiangsu University  Zhenjiang 212013 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Di","family":"Si","sequence":"additional","affiliation":[{"name":"Department of Applied Biology and Chemical Technology The Hong Kong Polytechnic University  Hung Hom Hong Kong SAR China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"LinLin","family":"Yang","sequence":"additional","affiliation":[{"name":"Catalonia Institute for Energy Research\u2010IREC  Sant Adri\u00e0 de Bes\u00f2s Barcelona 08930 Spain"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Heng\u2010Quan","family":"Chen","sequence":"additional","affiliation":[{"name":"Key Laboratory of the Ministry of Education for Advanced Catalysis Materials Institute of Physical Chemistry Zhejiang Normal University  Jinhua 321004 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Ren","family":"He","sequence":"additional","affiliation":[{"name":"Catalonia Institute for Energy Research\u2010IREC  Sant Adri\u00e0 de Bes\u00f2s Barcelona 08930 Spain"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Congxu","family":"Wang","sequence":"additional","affiliation":[{"name":"Department of Applied Biology and Chemical Technology The Hong Kong Polytechnic University  Hung Hom Hong Kong SAR China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Wengang","family":"Huang","sequence":"additional","affiliation":[{"name":"School of Chemical Engineering University of Queensland  St. Lucia QLD 4072 Australia"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Fusong","family":"Kang","sequence":"additional","affiliation":[{"name":"Department of Applied Biology and Chemical Technology The Hong Kong Polytechnic University  Hung Hom Hong Kong SAR China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Zhipeng","family":"Liu","sequence":"additional","affiliation":[{"name":"Department of Applied Biology and Chemical Technology The Hong Kong Polytechnic University  Hung Hom Hong Kong SAR China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yi","family":"Xiao","sequence":"additional","affiliation":[{"name":"Key Laboratory of Power Station Energy Transfer Conversion and System Ministry of Education North China Electric Power University  Beijing 102206 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Tao","family":"Wang","sequence":"additional","affiliation":[{"name":"Key Laboratory of Power Station Energy Transfer Conversion and System Ministry of Education North China Electric Power University  Beijing 102206 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-0109-9367","authenticated-orcid":false,"given":"Zeyu","family":"Deng","sequence":"additional","affiliation":[{"name":"Department of Materials Science and Engineering National University of Singapore  9 Engineering Drive 1 Singapore 117575 Singapore"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-1075-9649","authenticated-orcid":false,"given":"Jingjie","family":"Ge","sequence":"additional","affiliation":[{"name":"Department of Applied Biology and Chemical Technology The Hong Kong Polytechnic University  Hung Hom Hong Kong SAR China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-1916-6484","authenticated-orcid":false,"given":"Zhigang","family":"Hu","sequence":"additional","affiliation":[{"name":"School of Materials Science and Engineering Shanghai Jiao Tong University  Shanghai 200240 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-7533-3251","authenticated-orcid":false,"given":"Andreu","family":"Cabot","sequence":"additional","affiliation":[{"name":"Catalonia Institute for Energy Research\u2010IREC  Sant Adri\u00e0 de Bes\u00f2s Barcelona 08930 Spain"},{"name":"ICREA Pg. 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