Electrolyte Engineering for 5 V Lithium Metal Batteries
Abstract
ABSTRACT Lithium‐metal batteries employing lithium‐rich manganese‐based oxide (LRMO) cathodes offer great potential for achieving gravimetric energy densities exceeding 750 Wh kg −1 . However, their practical deployment is hindered by severe electrolyte decomposition and rapid capacity fade, particularly under high‐voltage conditions. Herein, N ‐methyltrifluoroacetamide (NMTFA) as a novel electrolyte additive is introduced, in combination with lithium difluoro(oxalato)borate (LiDFOB), to modulate the electrolyte solvation structure and enhance interfacial stability. Endowed with lone pair electrons and an N‐H bond, NMTFA acts as an electron donor capable of scavenging oxygen radicals released from the LRMO cathode, thereby mitigating electrolyte degradation and suppressing gas evolution. Additionally, hydrogen‐bonding interactions between NMTFA and the primary solvent, along with the incorporation of DFOB − anions into the primary solvation sheath, weaken Li + ‐solvent interactions, promoting the formation of a nitrogen‐/boron‐rich interphase that facilitates faster Li + desolvation and improves electrode stability. As a result, the Li||LRMO full cell delivers exceptional cycling stability, retaining over 70% of its initial capacity after 800 cycles at a cut‐off voltage of 4.8 V and over 80% retention after 300 cycles at 5.0 V. This study provides critical insights into the rational design of advanced electrolytes for high‐voltage lithium‐metal batteries.
Article Details
Authors (14)
Mengmin Jia
Collaborative Innovation Center of Henan Province For Green Manufacturing of Fine Chemicals, Key Laboratory of Green Chemical Media and Reactions, Ministry of Education, Henan Province Engineering Research Center of Special Electrolytes for Secondary Batteries in Low‐Altitude Aircraft,School of Chemistry and Chemical Engineering Henan Normal University Xinxiang P. R. China
Canhui Wu
Collaborative Innovation Center of Henan Province For Green Manufacturing of Fine Chemicals, Key Laboratory of Green Chemical Media and Reactions, Ministry of Education, Henan Province Engineering Research Center of Special Electrolytes for Secondary Batteries in Low‐Altitude Aircraft,School of Chemistry and Chemical Engineering Henan Normal University Xinxiang P. R. China
Mengjia Hu
Third Military Medical University, Chongqing, China
Lin Wang
Zhuangzhuang Zhang
Nana Shen
Collaborative Innovation Center of Henan Province For Green Manufacturing of Fine Chemicals, Key Laboratory of Green Chemical Media and Reactions, Ministry of Education, Henan Province Engineering Research Center of Special Electrolytes for Secondary Batteries in Low‐Altitude Aircraft,School of Chemistry and Chemical Engineering Henan Normal University Xinxiang P. R. China
Liang Wang
Dai‐Huo Liu
School of Chemistry and Chemical Engineering Henan Normal University Xinxiang 453007 P.R. China
Bao Wang
Pushpendra Kumar
Qian Li
Bao Li
College of Materials Science and Engineering
Dongmei Dai
Collaborative Innovation Center of Henan Province For Green Manufacturing of Fine Chemicals, Key Laboratory of Green Chemical Media and Reactions, Ministry of Education, Henan Province Engineering Research Center of Special Electrolytes for Secondary Batteries in Low‐Altitude Aircraft,School of Chemistry and Chemical Engineering Henan Normal University Xinxiang P. R. China
Jun Ming
State Key Laboratory of Rare Earth Resource Utilization Changchun Institute of Applied Chemistry Chinese Academy of Sciences Changchun China