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This study proposes an innovative strategy to replace OER with the thermodynamically favorable methanol oxidation reaction (MOR) while producing high\u2010value formic acid. The study develops a novel series of metallic ammonium phosphate electrocatalysts (NPOs\u00b7nH\n                    <jats:sub>2<\/jats:sub>\n                    O) through a facile chemical precipitation method, including the high\u2010entropy FeCoNiCuMn\u2010NPO\u00b7nH\n                    <jats:sub>2<\/jats:sub>\n                    O. The unique superstructure coupled with multi\u2010element synergy enables abundant active site exposure, optimized electronic configuration, and enhanced charge transfer capability. Remarkably, the high\u2010entropy catalyst demonstrates exceptional bi\u2010functional performance: achieving ultralow overpotentials of 204\/289\u00a0mV at 10\/100\u00a0mA cm\n                    <jats:sup>\u22122<\/jats:sup>\n                    for OER, and requiring only 1.3\u00a0V versus RHE to deliver 10\u00a0mA cm\n                    <jats:sup>\u22122<\/jats:sup>\n                    in MOR\u2010assisted electrolysis. Particularly, it exhibits high normalized activity (electrochemically active surface area activity: 16.6\u00a0mA cm\n                    <jats:sup>\u22122<\/jats:sup>\n                    , mass activity: 980\u00a0mA mg\n                    <jats:sup>\u22121<\/jats:sup>\n                    ) with 94% Faradaic efficiency for formic acid production. The catalyst maintains &gt;120\u00a0h stability at industrial\u2010level current density (100\u00a0mA cm\n                    <jats:sup>\u22122<\/jats:sup>\n                    ), outperforming most reported transition metal\u2010based electrocatalysts. This work establishes a new paradigm for designing high\u2010entropy electrocatalysts through structural engineering and composition optimization, providing crucial insights for sustainable energy conversion and biomass valorization.\n                  <\/jats:p>","DOI":"10.1002\/smtd.202500502","type":"journal-article","created":{"date-parts":[[2025,4,8]],"date-time":"2025-04-08T07:26:46Z","timestamp":1744097206000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":6,"title":["High\u2010Entropy Metal Ammonium Phosphate Superstructure Nanocatalysts for Highly Efficient Water Oxidation and Methanol Oxidation"],"prefix":"10.1002","volume":"9","author":[{"given":"Yu","family":"Pang","sequence":"first","affiliation":[{"name":"Key Laboratory of Eco\u2010chemical Engineering, International Science and Technology Cooperation Base of Eco\u2010chemical Engineering and Green Manufacturing Qingdao University of Science and Technology  Qingdao 266042 P. 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