Synthesis and Electrochemical Performance of Spheroid LiNi1/3Co1/3Mn1/3O2 in the Electrolyte Modified by Ethylene Sulfate and Methylene Methanedisulfonate

Abstract

In this study, spheroid LiNi1/3Co1/3Mn1/3O2 (NCM111) cathode material were synthesized using LiOH with Ni0.5Co0.2Mn0.3(OH)2 precursor by a simple solid-state reaction, and characterized by X-ray diffraction and scanning electron microscopy. Electrochemical behavior of NCM111 was investigated by electrochemical impedance spectroscopy (EIS) combining with cyclic voltammogram (CV) and charge/discharge test in the 1 M LiPF6-EC:EMC electrolyte with ethylene sulfate (DTD) and methylene methanedisulfonate (MMDS) additives either singly or in combination with high cutoff voltage of 3.0–4.5 V at room temperature of 25 °C or elevated temperature of 55 °C. It was found that DTD additive can increase the initial coulombic efficiency of NCM111, and the spheroid NCM111 can obtain the maximum initial discharge capacity of 177.81 mAh/g with the 2 wt% DTD, and keep 92.29% capacity retention after 80 cycles. The MMDS additives would decrease the initial discharge capacity of the NCM111, and enhance significantly long cycle life of the NCM111 with the capacity retention of 99.23% over 80 cycles at high voltage of 4.5 V. The additive combination 2 wt% DTD + 1 wt% MMDS was an optimal additive combination, demonstrating the 102.2% capacity retention over 80 cycles at room temperature and the 94.2% capacity retention over 70 cycles at elevated temperature of 55 °C. EIS results revealed that the additive blend of 2 wt% DTD + 1 wt% MMDS can drastically lower the kinetics impedance and suppress the growth rate of R ct for the NCM111 electrode.