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In conventional aqueous electrolytes, this percolated water network supports proton relay, hydrogen evolution reaction (HER), local alkalization, by\u2010product precipitation, and Zn\n                    <jats:sup>2+<\/jats:sup>\n                    flux distortion, thereby forming a self\u2010amplifying failure loop at the Zn\/electrolyte interface. Herein, we propose a molecular gating strategy to regulate this reactive water network using 4\u2010hydroxy\u20102\u2010butanone (HBN) as a dual\u2010site hydrogen\u2010bond modulator. The carbonyl and hydroxyl groups of HBN competitively interact with water, fragmenting the continuous H\n                    <jats:sub>2<\/jats:sub>\n                    O\u2013H\n                    <jats:sub>2<\/jats:sub>\n                    O hydrogen\u2010bond network into low\u2010cooperativity water domains and suppressing proton\u2010relay HER. Concurrently, HBN mildly reshapes the Zn\n                    <jats:sup>2+<\/jats:sup>\n                    solvation sheath environment toward a less water\u2010dominated configuration, moderating interfacial charge\u2011transfer while preserving essential Zn\n                    <jats:sup>2+<\/jats:sup>\n                    transport. This topology\u2010gated aqueous regime simultaneously suppresses water\u2010induced side reactions, prevents alkaline passivation\u2010driven Zn\n                    <jats:sup>2+<\/jats:sup>\n                    flux distortion, and enables compact Zn deposition. Consequently, the optimized electrolyte affords highly reversible Zn plating\/stripping with an average Coulombic efficiency of 99.12% over 800 cycles and supports a 1.0 Ah\u2010level NVO||Zn pouch cell for 70 cycles with negligible capacity decay.\n                  <\/jats:p>","DOI":"10.1002\/anie.7342949","type":"journal-article","created":{"date-parts":[[2026,10,2]],"date-time":"2026-10-02T07:40:50Z","timestamp":1790926850000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Molecular Gating of the Reactive Water Topological Network for Stable Aqueous Zn Batteries"],"prefix":"10.1002","author":[{"given":"Shaohua","family":"Han","sequence":"first","affiliation":[{"name":"School of Materials Science and Engineering Hunan Provincial Key Laboratory of Electronic Packaging and Advanced Functional Materials Central South University  Changsha Hunan P. R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0009-0001-3666-2394","authenticated-orcid":false,"given":"Weijie","family":"Fan","sequence":"additional","affiliation":[{"name":"School of Materials Science and Engineering Hunan Provincial Key Laboratory of Electronic Packaging and Advanced Functional Materials Central South University  Changsha Hunan P. R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Zekai","family":"Mei","sequence":"additional","affiliation":[{"name":"School of Instrument Science and Technology Xi'an Jiaotong University  Xi'an Shaanxi P. R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-2520-7406","authenticated-orcid":false,"given":"Shen","family":"Gong","sequence":"additional","affiliation":[{"name":"School of Materials Science and Engineering Hunan Provincial Key Laboratory of Electronic Packaging and Advanced Functional Materials Central South University  Changsha Hunan P. R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-4542-7409","authenticated-orcid":false,"given":"Yangyang","family":"Liu","sequence":"additional","affiliation":[{"name":"School of Instrument Science and Technology Xi'an Jiaotong University  Xi'an Shaanxi P. R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-0858-4533","authenticated-orcid":false,"given":"Jiang","family":"Zhou","sequence":"additional","affiliation":[{"name":"School of Materials Science and Engineering Hunan Provincial Key Laboratory of Electronic Packaging and Advanced Functional Materials Central South University  Changsha Hunan P. R. 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