Development of Pyridine-Boron Trifluoride Electrolyte Additives for Lithium-Ion Batteries

Abstract

A series of novel electrolyte additives based on Lewis acid/base adducts has been designed and successfully synthesized. The synthesis is very simple: a pyridine derivative is mixed with boron trifluoride dissolved in diethyl ether to yield a solid crystalline product. The effect of Pyridine-Boron Trifluoride (PBF) and its derivatives have been thoroughly evaluated in Li[Ni1/3Mn1/3Co1/3]O2/graphite and Li[Ni0.42Mn0.42Co0.16]O2/graphite pouch cells. Evaluation experiments, including high voltage storage, gas production, electrochemical impedance spectroscopy measurements, ultra high precision cycling and long-term cycling were carried out on cells containing the novel additives. The results were compared to baseline experiments on cells with well-known additives such as vinylene carbonate (VC), prop-1-ene sultone (PES), methylene methane disulfonate (MMDS), tris(-trimethyl-silyl)-phosphite (TTSPi) and triallyl phosphate (TAP). The PBF additives are competitive with all known additives in NMC/graphite cells, which, combined with their low cost and facile synthesis, suggest this series of novel additives will be useful in high-voltage/high-temperature lithium ion battery applications. The PBF additives yield cells which show excellent capacity retention and maintain low impedance during high voltage cycling, in contrast to cells containing VC.