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Nonetheless, there is a relative dearth of attention regarding the structural evolution of HEAs under electrochemical conditions. We herein used platinum\u2010group HEA nanocubes, initially enclosed by well\u2010defined {100} facets, as electrocatalysts for the multistep ethanol oxidation reaction (EOR). Notably, the prepared catalysts demonstrate an 8.3\u2010fold enhancement in specific activity during electrochemical cycling, driven by the structural evolution of catalyst facets. This transformation leads to a severely beveled cubic morphology characterized by an approximately equal distribution of {100}, {110}, and {111} facets, while preserving the compositional homogeneity and high\u2010entropy nature, as confirmed by high\u2010resolution transmission electron microscopy and synchrotron\u2010based x\u2010ray absorption spectroscopy. In situ surface\u2010enhanced infrared absorption spectroscopy, electrochemical stripping experiments, and computational calculations reveal that the enhanced performance originates from improved C\u2500C bond cleavage and superior resistance to poisoning by formate intermediates (HCOO\n                    <jats:sub>ad<\/jats:sub>\n                    ). These features promote complete oxidation of ethanol to CO\n                    <jats:sub>2<\/jats:sub>\n                    , a critical step for maximizing efficiency in direct alcohol fuel cells for renewable energy applications.\n                  <\/jats:p>","DOI":"10.1002\/anie.8871821","type":"journal-article","created":{"date-parts":[[2026,7,11]],"date-time":"2026-07-11T17:21:08Z","timestamp":1783790468000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":1,"title":["Electrochemically Induced Structural Evolution to Generate Optimized High\u2010Entropy\u2010Alloy Electrocatalysts for Ethanol Oxidation"],"prefix":"10.1002","volume":"65","author":[{"ORCID":"https:\/\/orcid.org\/0009-0004-6044-5076","authenticated-orcid":false,"given":"Yueh\u2010Chun","family":"Hsiao","sequence":"first","affiliation":[{"name":"Stephenson Institute for Renewable Energy and Department of Chemistry University of Liverpool  Liverpool 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