The Effect of Some Nitriles as Electrolyte Additives in Li-Ion Batteries

Abstract

The effect of the nitrile electrolyte additives, succinonitrile (SN), adiponitrile (AN) and pimelonitrile (PN) was studied using High Precision Charger at Dalhousie University, automated cell storage and AC impedance. Li[Ni1/3Mn1/3Co1/3]O2/graphite (NMC111/graphite) cells containing the nitrile electrolyte additives showed no significant effect on the cycling between 2.8 V and 4.2 V and storage at 4.2 V at 60. ± 0.1°C. However, when the high cutoff voltage increased to 4.5 V in Li[Ni0.4Mn0.4Co0.2]O2/graphite (NMC442/graphite) cells, the addition of 2 wt% SN and 2 wt% vinylene carbonate (VC) reduced the reversible capacity loss and gas generation during storage experiments at 60. ± 0.1°C compared to 2 wt% VC alone. The addition of 2 wt% SN also caused a large impedance growth during the 4.5 V storage period, but that could be suppressed by the addition of 1 wt% ethylene sulfite (ES) + 1 wt% tris(trimethlysilyl) phosphite (TTSPi) or 2 wt% trimethylene sulfate (TMS) + 2 wt% TTSPi. This work shows that SN leads to meaningful improvements in storage properties at voltages higher than 4.4 V. This also suggests that SN can enhance the long-term cycle life of the high voltage NMC/graphite cells by suppressing electrolyte oxidation at the positive electrode.