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Herein, we demonstrate that the strong electronic metal\u2013support interactions (EMSIs) established between FeOCl and a composite carbon (GC) support could steer the 2e\n                    <jats:sup>\u2212<\/jats:sup>\n                    ORR toward a direct 3e\n                    <jats:sup>\u2212<\/jats:sup>\n                    ORR pathway, boosting the yield of \u00b7OH. Combined characterizations and DFT calculations revealed that the average net charge on Fe atoms was increased owing to charge redistribution within the FeOCl driven by the strong EMSIs, enabling the optimized adsorption of O\n                    <jats:sub>2<\/jats:sub>\n                    and key intermediates (*OOH and *HOOH), thus facilitating the efficient \u00b7OH generation. The resulting FeOCl\/GC 3e\n                    <jats:sup>\u2212<\/jats:sup>\n                    ORR system achieved a \u00b7OH yield of 128.8 \u00b5mol g\n                    <jats:sub>cat<\/jats:sub>\n                    <jats:sup>\u22121<\/jats:sup>\n                    min\n                    <jats:sup>\u22121<\/jats:sup>\n                    , which was seven times that of the conventional Fe\n                    <jats:sub>2<\/jats:sub>\n                    O\n                    <jats:sub>3<\/jats:sub>\n                    \/GC electro\u2010Fenton system, allowing rapid water decontamination with an apparent rate constant of 1.15 min\n                    <jats:sup>\u22121<\/jats:sup>\n                    . Moreover, the sufficient \u00b7OH production realized over 90% decontamination efficiency retained after 25 cycles, highlighting its potential for practical application. This work establishes strong EMSIs as a powerful strategy for regulating ORR pathways to enhance \u00b7OH generation in the electro\u2010Fenton system.\n                  <\/jats:p>","DOI":"10.1002\/anie.8484914","type":"journal-article","created":{"date-parts":[[2026,9,27]],"date-time":"2026-09-27T16:45:59Z","timestamp":1790527559000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["The Strong Electronic Metal\u2013Support Interactions Mediated Direct Three\u2010Electron Oxygen Reduction for Enhanced Hydroxyl Radical Generation"],"prefix":"10.1002","author":[{"ORCID":"https:\/\/orcid.org\/0009-0006-1225-8158","authenticated-orcid":false,"given":"Shuxun","family":"Chen","sequence":"first","affiliation":[{"name":"State Key Laboratory of Green Papermaking and Resource Recycling, Shanghai Engineering Research Center of Solid Waste Treatment and Resource Recovery, School of Environmental Science and Engineering Shanghai Jiao Tong University  Shanghai P. 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