Localized High-Concentration Sulfone Electrolytes for High-Efficiency Lithium-Metal Batteries

Summary To enable next-generation high-energy-density lithium (Li)-metal batteries (LMBs), an electrolyte that has simultaneous high Li-metal Coulombic efficiency (CE) and high anodic stability on cathodes is of significant importance. Sulfones are known for strong resistance against oxidation, yet their application in LMBs is restricted because of their poor compatibility with Li-metal anodes, high viscosity, and poor wettability. Here, we demonstrate that a high Li CE over 98% can be achieved in concentrated sulfone-based electrolytes. Furthermore, the viscosity and wettability issues of sulfones are resolved by the addition of a fluorinated ether, 1,1,2,2-tetrafluoroethyl-2,2,3,3-tetrafluoropropyl ether, to form a localized high-concentration electrolyte (LHCE), which not only provides further improvement in Li CE (98.8%) but also remains anodically stable with high-voltage cathodes, suppresses Al corrosion, and enables LMBs to operate in a wide temperature range. As a result, significantly improved cycling performance of LMBs has been realized with sulfone-based LHCE.