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Current research predominantly focuses on zinc ions, while the critical role of anions in mediating these degradation pathways has been largely overlooked. Herein, we present a \u201ccation group\u2010driven dual\u2010track regulation\u201d strategy by engineering a cationic hydrogel electrolyte composed of poly(acryloyloxyethyl trimethyl ammonium chloride) (PDAC) and ZnCl\n                    <jats:sub>2<\/jats:sub>\n                    . The immobilized quaternary ammonium groups (\u2500N\n                    <jats:sup>+<\/jats:sup>\n                    (CH\n                    <jats:sub>3<\/jats:sub>\n                    )\n                    <jats:sub>3<\/jats:sub>\n                    ) electrostatically confine Cl\n                    <jats:sup>\u2012<\/jats:sup>\n                    anions, thereby creating highly efficient Zn\n                    <jats:sup>2+<\/jats:sup>\n                    \u2010selective migration channels and suppressing competing side reactions. Simultaneously, these cationic groups adsorb onto high\u2010energy zinc crystal facets, guiding (002)\u2010oriented Zn deposition and effectively inhibiting dendrite growth. The optimized PDAC\u2010based electrolyte delivers a high ionic conductivity of 5.3\u00a0mS\u00a0cm\n                    <jats:sup>\u22121<\/jats:sup>\n                    at \u221250\u00b0C, a Zn\n                    <jats:sup>2+<\/jats:sup>\n                    transference number of 0.87, and exceptional average reversibility of Zn plating\/stripping (98%) in Zn||Cu cells down to \u221240\u00b0C. Moreover, PDAC\u2010optimized ZHSCs demonstrate outstanding cyclability over 20\u00a0000 at \u221240\u00b0C (95.2% capacity retention). This work establishes a generalizable electrolyte design paradigm that concurrently addresses kinetic and interfacial limitations, paving the way for dendrite\u2010free, high\u2010performance Zn\u2010based energy storage systems operable under low\u2010temperature conditions.\n                  <\/jats:p>","DOI":"10.1002\/smll.202514685","type":"journal-article","created":{"date-parts":[[2026,3,9]],"date-time":"2026-03-09T10:30:27Z","timestamp":1773052227000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":2,"title":["Cation Group\u2010Driven Dual\u2010Track Regulation Enables Dendrite\u2010Free and Low\u2010Temperature Zn\u2010Ion Hybrid Supercapacitors"],"prefix":"10.1002","volume":"22","author":[{"given":"Kun","family":"Zhang","sequence":"first","affiliation":[{"name":"Institute of Energy Innovation College of Materials Science and Engineering &amp; College of Mining Engineering Taiyuan University of Technology  Taiyuan China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Ranfeng","family":"Wang","sequence":"additional","affiliation":[{"name":"Institute of Energy Innovation College of Materials Science and Engineering &amp; College of Mining Engineering Taiyuan University of Technology  Taiyuan China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Tao","family":"Feng","sequence":"additional","affiliation":[{"name":"Institute of Energy Innovation College of Materials Science and Engineering &amp; College of Mining Engineering Taiyuan University of Technology  Taiyuan China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yuede","family":"Pan","sequence":"additional","affiliation":[{"name":"Institute of Energy Innovation College of Materials Science and Engineering &amp; College of Mining Engineering Taiyuan University of Technology  Taiyuan 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