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However, existing strategies mainly rely on solvent engineering, whereas lithium salt design remains underexplored. Herein, we design an asymmetric lithium salt, lithium (N, N\u2010dimethylsulfamoyl) (trifluoromethanesulfonyl)imide (LiDMTFSI), featuring an electron\u2010donating dimethylamino group that enhances the anion's nucleophilicity and Lewis basicity. By introducing a push\u2010pull effect on the anionic charge, LiDMTFSI shifts the solvation structure from solvent\u2010rich to anion\u2010rich, thereby facilitating the co\u2010dissolution of beneficial lithium salt. The resulting solvent\u2010deficient solvation sheath governs the interphasial chemistry to favor the formation of a compact inorganic\u2010rich SEI (e.g., LiF, Li\n                    <jats:sub>2<\/jats:sub>\n                    O, Li\n                    <jats:sub>3<\/jats:sub>\n                    N, Li\n                    <jats:sub>2<\/jats:sub>\n                    S, and other beneficial components) with excellent mechanical integrity and interfacial ion transport, enabling uniform Li deposition and mitigating parasitic side\u2010reactions. A high Li plating\/stripping Coulombic efficiency of 99.1% was achieved in dilute carbonate\u2010based electrolytes, and full cells with ultrathin Li anodes and high\u2010loading NMC811 cathodes demonstrated consistent operation for over 120 cycles with 83% capacity retention at a high voltage of 4.3\u00a0V. These findings underscore the potential of anion molecular design as a powerful strategy for interphasial engineering in high\u2010energy LMBs.\n                  <\/jats:p>","DOI":"10.1002\/anie.202523528","type":"journal-article","created":{"date-parts":[[2025,12,31]],"date-time":"2025-12-31T07:12:22Z","timestamp":1767165142000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":5,"title":["Rational Design of Asymmetric Lithium Salts with Multi\u2010Functional Capabilities for Stable Lithium Metal Batteries"],"prefix":"10.1002","volume":"65","author":[{"ORCID":"https:\/\/orcid.org\/0000-0002-0215-4690","authenticated-orcid":false,"given":"Yuhao","family":"Wu","sequence":"first","affiliation":[{"name":"Department of Chemical Engineering Tsinghua University  Beijing 100084 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Hai","family":"Wang","sequence":"additional","affiliation":[{"name":"School of 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