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High\u2010entropy alloys (HEAs), despite their promise for catalysis, remain unexplored in acidic CO\n                    <jats:sub>2<\/jats:sub>\n                    electrolysis plagued by difficult control over reaction pathways on multi\u2010metal sites and severe metal dissolution in acidic and reductive environments. Here, we unlock the first demonstration of acidic CO\n                    <jats:sub>2<\/jats:sub>\n                    electrolysis over a mildly synthesized nano\u2010coral HEA catalyst via rationally directed electron reordering. The tailored electron pairing effect engenders a distinctive Cu\u2010O\u2013C\u2013Ag heteronuclear bidentate coupling configuration of oxygenated intermediates, which facilitates the C\u2500O bond elongation and cleavage, substantially lowering energy barrier of the rate\u2010determining *COOH\u2010to\u2010*CO conversion. Concurrently, the orchestrated charge redistribution among synergistic metal atoms strengthens intermetallic bonding, elevating the dissolution energy of constituent metals and conferring robust corrosion resistance in acidic electrolyte. The designed senary HEA catalyst delivers, for the first time, efficient acidic CO\n                    <jats:sub>2<\/jats:sub>\n                    electroreduction, achieving near\u2010unity CO Faradaic efficiency (FE) of 99% and sustained operation with FE exceeding 90% for over 180\u00a0h. Such catalyst also exhibits remarkable performance across pH\u2010universal electrolytes, enabling generally applicable CO\n                    <jats:sub>2<\/jats:sub>\n                    electrolysis. This work establishes a new paradigm for regulating intermediates adsorption on HEA structure, opening up a pathway for HEA catalysts toward acidic CO\n                    <jats:sub>2<\/jats:sub>\n                    electrolysis.\n                  <\/jats:p>","DOI":"10.1002\/adma.75161","type":"journal-article","created":{"date-parts":[[2026,9,28]],"date-time":"2026-09-28T07:35:14Z","timestamp":1790580914000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Heteronuclear Bidentate Coupling of Oxygenated Intermediates Unlocking Selective and Long\u2010Lasting Acidic CO\n                    <sub>2<\/sub>\n                    Electrolysis on High\u2010Entropy Alloys"],"prefix":"10.1002","author":[{"given":"Xiaoyong","family":"Ma","sequence":"first","affiliation":[{"name":"State Key Laboratory of Solidification Processing Center for Nano Energy Materials School of Materials Science and Engineering Northwestern 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Engineering Northwestern Polytechnical University  Xi'an China"},{"name":"Advanced Power Research Institute of Northwestern Polytechnical University in Sichuan Tianfu New Area  Chengdu China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Haoze","family":"Zhang","sequence":"additional","affiliation":[{"name":"State Key Laboratory of Solidification Processing Center for Nano Energy Materials School of Materials Science and Engineering Northwestern Polytechnical University  Xi'an China"},{"name":"Advanced Power Research Institute of Northwestern Polytechnical University in Sichuan Tianfu New Area  Chengdu China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Qing","family":"Zhang","sequence":"additional","affiliation":[{"name":"Vacuum Interconnected Nanotech Workstation Suzhou Institute of Nano\u2010Tech and Nano\u2010Bionics Chinese Academy of Sciences  Suzhou Jiangsu 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