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Common solvents are either only stable against lithium metal anode or only stable against LiNi<jats:sub><jats:italic>x<\/jats:italic><\/jats:sub>Mn<jats:sub><jats:italic>y<\/jats:italic><\/jats:sub>Co<jats:sub>1\u2010<jats:italic>x<\/jats:italic>\u2010<jats:italic>y<\/jats:italic><\/jats:sub>O<jats:sub>2<\/jats:sub> (NMC) cathode. There is significant effort trying to increase the cathode stability for ether electrolytes, which are in general stable against lithium metal anode. In comparison, there is much less effort trying to increase the anode stability of electrolytes that are stable against NMC cathode. One example is the sulfone\u2010based electrolyte. It has good cathode stability but is hindered from practical application because of (1) high viscosity and poor wetting capability and (2) poor anode stability. Here, we solve these issues by modifying the sulfone molecules using resonance and electron withdrawing effect. The viscosity is significantly reduced by delocalizing the electrons through introducing additional oxygen on the molecular backbone and applying appropriate fluorination. The resulting molecule 2,2,2\u2010trifluoroethyl mesylate (TFEM) has decreased Lewis basicity and less reactivity toward Li<jats:sup>+<\/jats:sup>. The electrolyte based on TFEM as single solvent enables cycling of LMB under harsh conditions of low N\/P ratio (21\u2005mg\/cm<jats:sup>2<\/jats:sup> NMC811 and 50\u2005\u03bcm Li) with 90\u2009% capacity retention after 160 cycles at C\/3 discharge rate.<\/jats:p>","DOI":"10.1002\/anie.202311051","type":"journal-article","created":{"date-parts":[[2023,9,13]],"date-time":"2023-09-13T11:38:41Z","timestamp":1694605121000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":32,"title":["Electron Delocalization Enables Sulfone\u2010based Single\u2010solvent Electrolyte for Lithium Metal Batteries"],"prefix":"10.1002","volume":"62","author":[{"given":"Muhammad","family":"Mominur Rahman","sequence":"first","affiliation":[{"name":"Chemistry Division Brookhaven National Laboratory  Upton NY 11973 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