The Optimal Amount of Lithium Difluorophosphate as an Additive for Si‐Dominant Anodes in an Application‐Oriented Setup

Fluoroethylene carbonate (FEC) and vinylene carbonate (VC) are considered the most effective electrolyte additives for improving the solid electrolyte interphase (SEI) of Si-containing anodes while lithium difluorophosphate (LiDFP) is known to improve the interphases of cathode materials and graphite. Here, we combine VC, FEC, and different amounts of LiDFP in a highly-concentrated electrolyte to investigate the effect on Si-dominant anodes in detail. Cycle life tests, electrochemical impedance spectroscopy and rate tests with anode potential monitoring were conducted in Si/NCM pouch cells. The results reveal that adding LiDFP to the electrolyte improves all performance criteria of the full cells, with a concentration of 1 wt% being the optimal value for most cases. Post-mortem analyses using scanning electron microscopy and x-ray photoelectron spectroscopy showed that a more beneficial SEI film was formed for higher LiDFP concentrations, which led to less decomposition of electrolyte components and a better-maintained anode microstructure.