Aprotic Electrolytes Beyond Organic Carbonates: Transport Properties of LiTFSI Solutions in S‐Based Solvents

This work illustrates a physico-chemical study of the structural, dynamic, and transport properties of electrolytes made of LiTFSI solutions in sulphoxide and sulphone solvent mixtures. Experimental measurements, by Raman and NMR spectroscopies, as well as electrochemical impedance spectroscopy, reveal the formation of a variety of ionic aggregates depending on the solvent composition that significantly affect the ion mobility and conductivity of the electrolyte. Mixtures containing tetrahydrothiophene-1-oxide exhibit a larger ion mobility due to a rapid exchange mechanism between solvent molecules, whereas the use of tetramethylene sulphone favors the formation of ionic aggregates due to the strong dipolar interactions between solvent molecules.