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

The LiNi0.8Co0.1Mn0.1O2 (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 (LiDFOB) 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 H2O/HF in the electrolyte to increase the electrolyte stability. Owing to the synergistic effect of LiDFOB and TMSP, the Li/ LiNi0.8Co0.1Mn0.1O2 half cells exhibit the capacity retention 76.3% after 500 cycles at a super high voltage of 4.7 V, the graphite/LiNi0.8Co0.1Mn0.1O2 full cells exhibit high capacity retention of 82.8% after 500 cycles at 4.5 V, and Li/LiNi0.8Co0.1Mn0.1O2 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. (c) 2022 Science China Press. Published by Elsevier B.V. and Science China Press. All rights reserved.

Automated summary

In this study, LiDFOB and TMSP were used as dual additives to optimize LiNi0.8Co0.1Mn0.1O2 cathode materials, reducing electrolyte decomposition and cathode interface reactions under high voltage, thereby improving the cycle life and capacity retention of the batteries.