Rechargeable Li/LiFePO 4 cells using N-methyl- N-butyl pyrrolidinium bis(trifluoromethane sulfonyl)imide–LiTFSI electrolyte incorporating polymer additives

Abstract

We have incorporated polymer additives such as poly(ethylene glycol) dimethyl ether (PEGDME) and tetra(ethylene glycol) dimethyl ether (TEGDME) into N-methyl- N-butylpyrrolidinium bis(trifluoromethane sulfonyl)imide (PYR 14TFSI)–LiTFSI mixtures. The resulting PYR 14TFSI + LiTFSI + polymer additive ternary electrolyte exhibited relatively high ionic conductivity as well as remarkably low viscosity over a wide temperature range compared to the PYR 14TFSI + LiTFSI binary electrolytes. The charge/discharge cyclability of Li/LiFePO 4 cells containing the ternary electrolytes was investigated. We found that Li/PYR 14TFSI + LiTFSI + PEGDME (or TEGDME)/LiFePO 4 cells containing the two different polymer additives showed very similar discharge capacity behavior, with very stable cyclability at room temperature (RT). Li/PYR 14TFSI + LiTFSI + TEGDME/LiFePO 4 cells can deliver about 127 mAh/g of LiFePO 4 (74.7% of theoretical capacity) at 0.054 mA/cm 2 (0.2C rate) at RT and about 108 mAh/g of LiFePO 4 (63.4% of theoretical capacity) at 0.023 mA/cm 2 (0.1C rate) at −1 °C for the first discharge. The cell exhibited a capacity fading rate of approximately 0.09–0.15% per cycle over 50 cycles at RT. Consequently, the PYR 14TFSI + LiTFSI + polymer additive ternary mixture is a promising electrolyte for cells using lithium metal electrodes such as the Li/LiFePO 4 cell reported here. These cells showed the capability of operating over a significant temperature range (∼0–∼30 °C).