Abstract
Rational carbonate electrolyte chemistry is critical for the development of high-voltage lithium metal batteries(LMBs).However,the implementation of traditional carbonate electrolyte is greatly hindered by the generation of an unstable electrode interphase and corrosive by-product(HF).Herein,we propose a triple-function eutectic solvent additive of N-methylacetamide(NmAc)with LiNO3 to enhance the sta-bility and compatibility of carbonate electrolyte.Firstly,the addition of NmAc significantly improves the solubility of LiNO3 in carbonate electrolyte by forming an eutectic pair,which regulates the Li+solvation structure and leads to dense and homogenous Li plating.Secondly,the hydrolysis of acidic PF5 is effec-tively alleviated due to the strong complexation of NmAc with PF5,thus reducing the generation of cor-rosive HF.In addition,the optimized cathode electrolyte interphase layer decreases the structural degradation and transition metal dissolution.Consequently,Li‖LiNi0.6Co0.2Mn0.2O2(NCM622)cells with the designed electrolyte deliver superior long-term cycle reversibility and excellent rate capability.This study unveils the rationale for incorporating eutectic solvent additives within carbonate electrolytes,which significantly contribute to the advancement of their practical application for high-voltage LMBs.
基金项目
National Natural Science Foundation of China(22379166)
Natural Science Foundation for Distinguished Young Scholars of Hunan Province(2022JJ10089)
Central South University Innovation-Driven Research Program(2023CXQD034)
High-Performance Computing Center of Central South University()