Fluorinated Ether Based Electrolyte for High-Energy Lithium–Sulfur Batteries: Li+ Solvation Role Behind Reduced Polysulfide Solubility

By employing new electrolytes, the polysulfide shuttle phenomenon, one of the main problems of lithium–sulfur (Li–S) batteries, can be significantly reduced. Here we present excellent coulombic efficiencies as well as adequate performance of high-energy Li–S cells by the use of a fluorinated ether (TFEE) based electrolyte at low electrolyte loading. The observed altered discharge profile was investigated both by electrochemical experiments and an especially tailored COSMO-RS computational approach, while the details of the discharge mechanism were elucidated by two operando techniques: XANES and UV/Vis spectroscopy. A significant decrease of polysulfide solubility compared to tetraglyme is due to different Li+ solvation mode.

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