Abstract
LiNi0.8Co0.1Mn0.1O2 (NCM811) is one of the most promising cathode materials in high-energy-density Li-ion batteries (LIBs) because of its high capacity and low cost. However, it still suffers from irreversible capacity fading at high cut-off voltages. This is mainly because high voltage accelerates the hydrolysis reaction of lithium hexafluorophosphate with trace water to generate byproducts such as highly corrosive hydrogen fluoride (HF) resulting in an unstable cathode–electrolyte interface and continuous irreversible phase transitions. Here, we modify a conventional electrolyte by adding the dual additives of tetrabutyl titanate (TBT) and lithium difluoroxalate borate (LiDFOB) to form a stable Ti-, B-, and F-rich interfacial layer to eliminate the unfavorable cathode-electrolyte side reactions and suppress deleterious phase transitions. Additionally, TBT can stabilize the electrolyte by removing H2O/HF. With the synergistic effect of the dual additives, the cycling stability of NCM811 at high voltages is enhanced considerably. The Li∣NCM811 cell with dual additives exhibits a high capacity retention rate of 86% after 200 cycles at 1 C and a high cut-off voltage of 4.5 V. This strategy provides a reference for designing high-voltage electrolytes for LIBs.
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