Synthesizing an inorganic-rich solid electrolyte interphase by tailoring solvent chemistry in carbonate electrolyte for enabling high-voltage lithium metal batteries  

作　　者：Qiwen Ran Hongyuan Zhao Jintao Liu Lei Li Qiang Hu Fuquan Nie Xingquan Liu Sridhar Kormarneni 

机构地区：[1]School of Materials and Energy,University of Electronic Science and Technology of China,Chengdu 610054,Sichuan,China [2]Department of Ecosystem Science and Management and Materials Research Institute,204 Energy and the Environment Laboratory,The Pennsylvania State University,University Park,PA 16802,USA [3]Research Center for Electrochemistry and Energy Engineering,Henan Institute of Science and Technology,Xinxiang 453003,Henan,China

出　　处：《Journal of Energy Chemistry》2023年第7期475-483,I0010,共10页能源化学（英文版）

基　　金：supported by the Natural Science Foundation of Henan Province(No.202300410163);the Innovative Research Team(in Science and Technology)in University of Henan Province(No.20IRTSTHN016);the Outstanding Talent Introduction Project of University of Electronic Science and Technology of China(No.08JC00303);the Innovative Research Team of Sichuan Fuhua New Energy High-Tech Co.,Ltd.(No.621006)。

摘　　要：High-voltage(>4.0 V)lithium metal battery(LBM)is considered to be one of the most promising candidates for next-generation high-energy batteries.However,the commercial carbonate electrolyte delivers a poor compatibility with Li metal anode,and its organic dominated solid electrolyte interphase(SEI)shows a low interfacial energy and a slow Li^(+)diffusion ability.In this work,an inorganic LiF-Li_(3)N rich SEI is designed to enable high-voltage LBM by introducing nano-cubic LiF and LiNO_(3)into1 M LiPF_(6)ethylene carbonate(EC)/dimethyl carbonate(DMC)(v:v=1:1)electrolyte.Specifically,the unique nano-cubic structure of as-synthetized LiF particles achieves its high concentration dissolution in carbonate electrolyte to enhance the interfacial energy of SEI.In addition,tetramethylene sulfolane(TMS)is used as a carrier solvent to dissolve LiNO_(3)in the carbonate electrolyte,thereby deriving a Li_(3)N-rich SEI.As a result,the as-designed electrolyte shows a high average Li plating/striping CE of 98.3%after 100 cycles at 0.5 m A cm^(-2)/0.5 mA h cm^(-2).Furthermore,it also enables the ultrathin Li(~50μm)‖LiNi_(0.8)Co_(0.1)Mn_(0.1)O_(2)(NCM,4.4 mA h cm^(-2))full cell to deliver a high-capacity retention of 80.4%after 100 cycles with an outstanding average CE of 99.7%.Notably,the practical application prospect of the modified electrolyte is also estimated in LiNi_(0.8)Co_(0.1)Mn_(0.1)O_(2)‖Li pouch cell with an energy density of 261.2 W h kg^(-1).This work sheds light on the internal mechanism of Li^(+)transport within the inorganic dominated SEI and provides a simple approach to stabilize the high-voltage LMBs.

关 键 词：Li metal battery Carbonate electrolyte Nano-cubic LiF LiNO_(3) Tetramethylene sulfolane 

分 类 号：TM912[电气工程—电力电子与电力传动] O646.1[理学—物理化学]