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Existing strategies predominantly rely on static confinement or adsorption, which cannot adapt to evolving iodine speciation during charge\u2013discharge, causing a trade\u2010off between shuttle suppression and redox kinetics. In this study, we report a proton\u2010switching strategy that regulates interfacial iodine chemistry via electrochemically driven protonation\u2013deprotonation within an imine\u2010linked two\u2010dimensional polymer framework, thereby dynamically rewiring interfacial electrostatics during cycling. During discharge, protonation of imine generates positively polarized C\u2550NH\n                    <jats:sup>+<\/jats:sup>\n                    sites that stabilize I\n                    <jats:sup>\u2212<\/jats:sup>\n                    through electrostatic interactions, enabling controlled reduction of polyiodides without accumulation. Upon charging, deprotonation restores the neutral framework, favoring polyiodide stabilization and efficient iodine oxidation. As a result, the constructed Zn\u2013I\n                    <jats:sub>2<\/jats:sub>\n                    battery delivers 51\u00a0000 cycles at 20 A g\n                    <jats:sup>\u22121<\/jats:sup>\n                    at 25\u00b0C and sustains over 70\u00a0000 cycles at \u221220\u00b0C. This durability is retained at a high iodine loading of 35.7\u00a0mg cm\n                    <jats:sup>\u22122<\/jats:sup>\n                    , delivering an areal capacity of 5 mAh cm\n                    <jats:sup>\u22122<\/jats:sup>\n                    over 2000 cycles with negligible decay, placing this system among the most durable Zn\u2013I\n                    <jats:sub>2<\/jats:sub>\n                    batteries.\n                  <\/jats:p>","DOI":"10.1002\/anie.4465475","type":"journal-article","created":{"date-parts":[[2026,8,5]],"date-time":"2026-08-05T12:20:56Z","timestamp":1785932456000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Proton\u2010Switching Regulates Interfacial Iodine Chemistry for Long\u2010Life Zinc\u2013Iodine Batteries"],"prefix":"10.1002","volume":"65","author":[{"ORCID":"https:\/\/orcid.org\/0000-0002-2547-4072","authenticated-orcid":false,"given":"Feifei","family":"Wang","sequence":"first","affiliation":[{"name":"Max Planck Institute For Microstructure Physics  Halle (Saale) Germany"},{"name":"Center for Advancing Electronics Dresden (cfaed) and Faculty of Chemistry and Food Chemistry Technische Universit\u00e4t Dresden  Dresden Germany"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Guoqin","family":"Liu","sequence":"additional","affiliation":[{"name":"Max Planck Institute For Microstructure Physics  Halle (Saale) Germany"},{"name":"Center for Advancing Electronics Dresden (cfaed) and Faculty of Chemistry and Food Chemistry Technische Universit\u00e4t Dresden  Dresden Germany"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yuhang","family":"Zhuang","sequence":"additional","affiliation":[{"name":"Center for Advancing Electronics Dresden (cfaed) and Faculty of Chemistry and Food Chemistry Technische Universit\u00e4t Dresden  Dresden Germany"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Peng","family":"Zhang","sequence":"additional","affiliation":[{"name":"Max Planck Institute For Microstructure Physics  Halle (Saale) Germany"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0009-0001-8109-2706","authenticated-orcid":false,"given":"Zhengwei","family":"Li","sequence":"additional","affiliation":[{"name":"Chair of Organic Chemistry I Faculty of Chemistry and Food Chemistry Technische Universit\u00e4t Dresden  Dresden Germany"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Songshan","family":"Bi","sequence":"additional","affiliation":[{"name":"Center for Advancing Electronics Dresden (cfaed) and Faculty of Chemistry and Food Chemistry Technische Universit\u00e4t Dresden  Dresden 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