Tailoring electrolyte enables high-voltage Ni-rich NCM cathode against aggressive cathode chemistries for Li-ion batteries

The LiNi_(0.8)Co_(0.1)Mn_(0.1)O_(2)(Ni-rich NCM)cathode materials suffer from electrochemical performance degradation upon cycling due to detrimental cathode interface reactions and irreversible surface phase transition when operating at a high voltage(≥4.5 V).Herein,a traditional carbonate electrolyte with lithium difluoro(oxalato)borate(Li DFOB)and tris(trimethylsilyl)phosphate(TMSP)as dual additives that can preferentially oxidize and decompose to form a stable F,B and Si-rich cathode-electrolyte interphase(CEI)that effectively inhibits continual electrolyte decomposition,transition metal dissolves,surface phase transition and gas generation.In addition,TMSP also removes trace H_(2)O/HF in the electrolyte to increase the electrolyte stability.Owing to the synergistic effect of Li DFOB and TMSP,the Li/LiNi_(0.8)Co_(0.1)Mn_(0.1)O_(2) half cells exhibit the capacity retention 76.3%after 500 cycles at a super high voltage of 4.7 V,the graphite/LiNi_(0.8)Co_(0.1)Mn_(0.1)O_(2)full cells exhibit high capacity retention of 82.8%after 500 cycles at 4.5 V,and Li/LiNi_(0.8)Co_(0.1)Mn_(0.1)O_(2)pouch cells exhibit high capacity retention 94%after 200 cycles at 4.5 V.This work is expected to provide an effective electrolyte optimizing strategy compatible with high energy density lithium-ion battery manufacturing systems.