Evaluating the Effect of Electrolyte Additive Functionalities on NMC622/Si Cell Performance

Unstable electrode/electrolyte interface is the major cause of degradation for silicon (Si)-based anodes for lithium (Li)-ion batteries. Development of functional electrolyte additives can provide a viable path toward stabilizing the dynamic Si/electrolyte interface, which will benefit the development of high energy density Li-ion batteries. Here, we evaluate polymerizable electrolyte additives with varying functional groups (fluorocarbon, thiophosphate, and fluorophosphazene). The additives are examined using LiNi0.6Mn0.2Co0.2O2/Si full cells where the cycle performance and impedance are measured. Electrochemical tests show that the fluorine-containing additives provide better passivation at the Si electrode, leading to enhanced full cell performance. Among the three additives examined, best electrochemical performance is observed from the fluorocarbon-containing compound, followed by fluorophosphazene- and thiophosphate-containing compounds. Characterization of the solid electrolyte interphase (SEI) on cycled electrodes using Auger electron spectroscopy (AES), X-ray photoelectron spectroscopy (XPS), and attenuated total reflectance Fourier transform infrared spectroscopy (ATR-FTIR) reveal that higher concentration of fluorine and lithium oxide, and lower concentration of carbonate and organic species correlate with enhanced electrochemical performance.

Automated summary

The unstable electrode/electrolyte interface is the main cause of degradation in silicon-based anodes for lithium-ion batteries. Developing functional electrolyte additives can stabilize the dynamic Si/electrolyte interface and benefit the development of high-energy-density Li-ion batteries. Among the evaluated polymerizable electrolyte additives with different functional groups, the fluorine-containing additives show the best passivation effect on the Si electrode and enhance the performance of the full cell.