Effect of FSI Based Ionic Liquid on High Voltage Li-Ion Batteries

Abstract

In this manuscript, a functionalized ionic liquid 1-cyanoethyl-2-methyl-3-allylimidazolium bis (trifluoromethanesulfonimide) salt (CEMAImTFSI) was synthesized and explored as an electrolyte component to improve the oxidation resistance of the electrolyte in high-voltage lithium-ion batteries. Based on the calculation by Gaussian 09, CEMAImTFSI has a higher highest occupied molecular orbital (HOMO) value than the organic solvents ethylene carbonate (EC) and dimethyl carbonate (DMC), suggesting that CEMAImTFSI is more susceptible to oxidation than EC and DMC. Moreover, a low Li+ binding energy value of –3.71 eV and the lower lowest unoccupied molecular orbital (LUMO) enable CEMAImTFSI to migrate easily to the surface of the LiNi0.5Mn1.5O4 cathode and participate in the formation of the SEI (solid electrolyte interphase) film, protecting the electrode materials. Electrochemical studies showed that the LiNi0.5Mn1.5O4/Li cell with 1.0 mol/L LiPF6-EC/DMC/10 vol% has the best cycling stability in the voltage range of 3–5 V. The initial discharge specific capacity of the cells was 131.03 mAh·g−1 at 0.2 C, and even after 50 cycles the discharge specific capacity value of 126.06 mAhg−1 was observed, with the cell showing a capacity retention as high as 96.2%. Even at the rate of 5 C, the average discharge specific capacity of the cell was still 109.30 mAh·g−1, which was 1.95 times higher than the cell without the CEMAImTFSI addition. The ionic liquid molecules adsorption on the cell electrode surface was confirmed by X-ray photoelectron spectroscopic (XPS) analysis after charge–discharge measurements.