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Whereas commercial separators in alkaline batteries, without ion regulation capability, fail to suppress severe dendrite and passivation of anionic [Zn(OH)\n 4<\/jats:sub>\n ]\n 2\u2012<\/jats:sup>\n and accelerate ion transport of anionic OH\n \u2012<\/jats:sup>\n . Herein, we tailor the coordination structures of alkali\u2010stable cationic complexes in polymer separators (CCPS) to construct anionic OH\n \u2012<\/jats:sup>\n selective transfer channels. Synchrotron spectroscopic characterizations and theoretical calculations reveal that the low\u2010coordination cationic complexes expose more positive charge density, electrostatically attracting more negative charge from [Zn(OH)\n 4<\/jats:sub>\n ]\n 2\u2012<\/jats:sup>\n . In situ electrochemical digital holography technology and time\u2010of\u2010flight secondary ion mass spectrometry analyses further confirm the homogeneous [Zn(OH)\n 4<\/jats:sub>\n ]\n 2\u2012<\/jats:sup>\n distribution at the CCPS\u2010electrode interface, oriented Zn deposition, and impeded passivation. As a result, CCPS enables alkaline Zn||Cu cells to operate over 5500 cycles at 1\u00a0mA cm\n \u20122<\/jats:sup>\n with a high coulombic efficiency of 99.99%. Alkaline Ni\u2013Zn batteries exhibit ultrastable cycling over 1000 cycles at 6 C and maintain 86.17% of their maximum capacity at 10 C. Our work may provide practical and effective separator strategies to accelerate the commercialization of alkaline batteries.\n <\/jats:p>","DOI":"10.1002\/adma.74613","type":"journal-article","created":{"date-parts":[[2026,8,14]],"date-time":"2026-08-14T10:38:30Z","timestamp":1786703910000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":1,"title":["Cationic Complex Polymer Separator Confined Anionic [Zn(OH)\n 4<\/sub>\n ]\n 2\u2012<\/sup>\n Reduction for Stable Alkaline Batteries"],"prefix":"10.1002","volume":"38","author":[{"given":"Zhihao","family":"Sun","sequence":"first","affiliation":[{"name":"Laboratory of Advanced Materials Aqueous Battery Center Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials Shanghai Wusong Laboratory of Materials Science Collaborative Innovation Center of Chemistry for Energy Materials State Key Laboratory of Porous Materials for Separation and Conversion College of Smart 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