Solvated Structure of Hybrid Tetraglyme‐Aqueous Electrolyte Dissolving High‐Concentration LiTFSI‐LiFSI for Dual‐Ion Battery

The solvated structure of a highly concentrated hybrid tetraglyme (G4)-water electrolyte was studied for an increasing cycle stability and performance of a KS6 used dual-ion battery. Hybrid solvent of G4 and water with a weight ratio of 2 to 8 was able to dissolve 9LiFSI-1LiTFSI supporting salts up to 37 mol kg-1 (37 mol kg-1 G2W8). In spite of such high concentration of supporting salts, reasonable charge and discharge performance of dual-ion battery (discharge capacity of ≈40 mAh g-1 and coulombic efficiency of 90 %) were exhibited over 300 cycles. This was attributed to the decreased hydrogen evolution reaction (HER) potential to -1.05 V vs. Ag/AgCl by addition of G4. From Fourier-transform infrared, nuclear magnetic resonance, and Raman spectroscopies, G4 molecules were more strongly coordinated to Li+ to form ion pairs of [Li(G4)x (H2 O)y ]+ complex in hybrid G4-water electrolyte. Co-intercalation of bis(trifluoromethanesulfonyl)imide (TFSI- ) and bis(fluorosulfonyl)imide (FSI- ) into graphitic carbon KS6 cathode was confirmed in hybrid aqueous electrolyte.