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A solvation\u2010equilibrium\u2010locked electrolyte (SELE) is reported by combining dimethyl sulfite (DMS), a low\u2010freezing weakly solvating solvent, with Pyr\n                    <jats:sub>13<\/jats:sub>\n                    DFOB (1\u2010methyl\u20101\u2010propylpyrrolidinium difluoro(oxalato)borate) as an ionic\u2010liquid co\u2010solvent. Cooperative ion\u2013dipole and weak C\u2013H\u22efO interactions between DMS and Pyr\n                    <jats:sub>13<\/jats:sub>\n                    <jats:sup>+<\/jats:sup>\n                    regulate the free\u2010solvent reservoir, while TFSI\n                    <jats:sup>\u2212<\/jats:sup>\n                    (bis(trifluoromethanesulfonyl)imide) and DFOB\n                    <jats:sup>\u2212<\/jats:sup>\n                    enrich the primary Li\n                    <jats:sup>+<\/jats:sup>\n                    coordination shell. Variable\u2010temperature\n                    <jats:sup>7<\/jats:sup>\n                    Li NMR, Raman, and molecular dynamics simulations show that solvent\u2010separated ion pairs, contact ion pairs, and aggregates remain nearly invariant from \u221260\u00b0C to 60\u00b0C, unlike the strongly temperature\u2010responsive Pyr\n                    <jats:sub>13<\/jats:sub>\n                    DFOB\u2010free electrolyte. This locked anion\u2010rich solvation structure reduces solvent coordination around Li\n                    <jats:sup>+<\/jats:sup>\n                    , mitigates solvent\u2010derived interfacial decomposition and gas evolution, and promotes LiF\u2010 and borate\u2010rich interphases on Li metal and NMC811. Consequently, Li||NMC811 cells deliver discharge capacity at \u221285\u00b0C and operate up to 120\u00b0C, while pouch cells remain functional after cooling to \u2212122.9\u00b0C. A 6.6 Ah Li||Ni90 pouch cell further achieves 565\u00a0Wh kg\n                    <jats:sup>\u22121<\/jats:sup>\n                    under lean\u2010electrolyte conditions, establishing solvation\u2010equilibrium locking as a molecular design principle for lithium metal batteries operating over a broad temperature range.\n                  <\/jats:p>","DOI":"10.1002\/adma.75409","type":"journal-article","created":{"date-parts":[[2026,10,15]],"date-time":"2026-10-15T06:47:47Z","timestamp":1792046867000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Solvation\u2010Equilibrium Locking Enables Ultrawide\u2010Temperature Operation of High\u2010Voltage Lithium\u2010Metal Batteries"],"prefix":"10.1002","author":[{"given":"Qingyu","family":"Dong","sequence":"first","affiliation":[{"name":"Beijing Key Laboratory of Environmental Science and Engineering School of Materials Science and Engineering Beijing Institute of 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 Beijing China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yang","family":"Li","sequence":"additional","affiliation":[{"name":"National Key Laboratory of Chemical and Physical Power Sources Tianjin Institute of Power Sources  Tianjin China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Li","family":"Li","sequence":"additional","affiliation":[{"name":"Beijing Key Laboratory of Environmental Science and Engineering School of Materials Science and Engineering Beijing Institute of Technology  Beijing China"},{"name":"Shandong Key Laboratory of Advanced Chemical Energy Storage and Intelligent Safety Advanced Technology Research Institute Beijing Institute of Technology  Jinan China"},{"name":"Innovative Research Team in High\u2010Safety Energy Storage System and Smart Microgrids of Guangdong Province Beijing Institute of Technology (Zhuhai)  Zhuhai China"},{"name":"Collaborative Innovation Center of Electric Vehicles in Beijing  Beijing 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