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Such limitations can be effectively mitigated by employing biphasic electrolytes featuring a liquid\u2010liquid interface, which enables efficient immobilization of the dissolved reaction intermediates. However, such systems frequently employ toxic organic solvents, which not only pose flammability risks but also struggle to adapt to extreme temperature conditions. Herein, we design a novel self\u2010stratified biphasic electrolyte via liquid\u2010liquid phase separation of choline chloride (ChCl)\u2010trifluoroacetamide (TFA) deep eutectic solvent (DES) and ZnSO\n                    <jats:sub>4<\/jats:sub>\n                    \/H\n                    <jats:sub>2<\/jats:sub>\n                    O\/ ethylene glycol solution. The upper DES phase effectively confines polyiodide anions, suppresses shuttle effect and stabilizes I\n                    <jats:sup>+<\/jats:sup>\n                    species, while the bottom aqueous phase regulates Zn\n                    <jats:sup>2+<\/jats:sup>\n                    solvation structure and inhibits dendrite formation and side reactions. Benefiting from the synergistic functional separation, the Zn\u2010I\n                    <jats:sub>2<\/jats:sub>\n                    battery realizes highly reversible four\u2010electron conversion, effectively suppresses battery self\u2010discharge, and delivers superior cycling stability over 21000 cycles as well as wide temperature tolerance ranging from \u221230\u00b0C to 50\u00b0C. This work offers novel insights into the design of safe and eco\u2010friendly biphasic electrolytes and provides an effective strategy for the construction of high\u2010performance 4eZIBs.\n                  <\/jats:p>","DOI":"10.1002\/adma.74606","type":"journal-article","created":{"date-parts":[[2026,8,12]],"date-time":"2026-08-12T08:33:40Z","timestamp":1786523620000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":1,"title":["A Self\u2010Phase\u2010Separated Deep Eutectic Solvent\u2010Based Biphasic Electrolyte for Durable Four\u2010Electron Zn\u2010I\n                    <sub>2<\/sub>\n                    Batteries Across Wide\u2010Temperature Range"],"prefix":"10.1002","volume":"38","author":[{"given":"Wenhui","family":"Wang","sequence":"first","affiliation":[{"name":"Institutes of Physical Science and Information Technology School of Materials Science and Engineering Key Laboratory of Environment\u2010Friendly Polymeric Materials of Anhui Province Anhui University  Hefei P. R. China"},{"name":"Anhui Provincial Key Laboratory of Green Carbon Chemistry Fuyang Normal University  Fuyang Anhui P. R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0009-0002-8287-6067","authenticated-orcid":false,"given":"Yangyang","family":"Liu","sequence":"additional","affiliation":[{"name":"Institutes of Physical Science and Information Technology School of Materials Science and Engineering Key Laboratory of Environment\u2010Friendly Polymeric Materials of Anhui Province Anhui University  Hefei P. R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Shilong","family":"Li","sequence":"additional","affiliation":[{"name":"Institutes of Physical Science and Information Technology School of Materials Science and Engineering Key Laboratory of Environment\u2010Friendly Polymeric Materials of Anhui Province Anhui University  Hefei P. R. 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China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0009-0001-5954-2221","authenticated-orcid":false,"given":"Longhai","family":"Zhang","sequence":"additional","affiliation":[{"name":"Institutes of Physical Science and Information Technology School of Materials Science and Engineering Key Laboratory of Environment\u2010Friendly Polymeric Materials of Anhui Province Anhui University  Hefei P. R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-6570-2781","authenticated-orcid":false,"given":"Yun","family":"Gao","sequence":"additional","affiliation":[{"name":"Institutes of Physical Science and Information Technology School of Materials Science and Engineering Key Laboratory of Environment\u2010Friendly Polymeric Materials of Anhui Province Anhui University  Hefei P. R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-3268-5708","authenticated-orcid":false,"given":"Shilin","family":"Zhang","sequence":"additional","affiliation":[{"name":"School of Chemical Engineering The University of Adelaide  Adelaide Australia"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-6188-6886","authenticated-orcid":false,"given":"Chaofeng","family":"Zhang","sequence":"additional","affiliation":[{"name":"Institutes of Physical Science and Information Technology School of Materials Science and Engineering Key Laboratory of Environment\u2010Friendly Polymeric Materials of Anhui Province Anhui University  Hefei P. R. China"},{"name":"Anhui Provincial Key Laboratory of Green Carbon Chemistry Fuyang Normal University  Fuyang Anhui P. R. 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