Polymerized-ionic-liquid-based solid polymer electrolyte for ultra-stable lithium metal batteries enabled by structural design of monomer and crosslinked 3D network  

作　　者：Lingwang Liu Jiangyan Xue Yiwen Gao Shiqi Zhang Haiyang Zhang Keyang Peng Xin Zhang Suwan Lu Shixiao Weng Haifeng Tu Yang Liu Zhicheng Wang Fengrui Zhang Daosong Fu Jingjing Xu Qun Luo Xiaodong Wu 

机构地区：[1]School of Nano-Tech and Nano-Bionics,University of Science and Technology of China,Hefei,230026,China [2]i-Lab,Suzhou Institute of Nano-Tech and Nano-Bionics(SINANO),Chinese Academy of Sciences,Suzhou,215123,China [3]School of Materials Science and Engineering,Shanghai University,Shanghai,200444,China [4]Tianmu Lake Institute of Advanced Energy Storage Technologies,Liyang,213300,China [5]Institute of Physics Chinese Academy of Sciences,Beijing,100190,China [6]College of Material Science and Engineering,Hohai University,Changzhou,213022,China

出　　处：《Materials Reports(Energy)》2025年第1期61-69,共9页材料导报(能源)(英文)

基　　金：financially supported by the National Key R&D Program of China(Grant No.2022YFE0207300);National Natural Science Foundation of China(Grant Nos.22179142 and 22075314);Jiangsu Funding Program for Excellent Postdoctoral Talent(Grant No.2024ZB051 and 2023ZB836);the technical support for Nano-X from Suzhou Institute of Nano-Tech and Nano-Bionics,Chinese Academy of Sciences(SINANO).

摘　　要：Solid polymer electrolytes(SPEs)have attracted much attention for their safety,ease of packaging,costeffectiveness,excellent flexibility and stability.Poly-dioxolane(PDOL)is one of the most promising matrix materials of SPEs due to its remarkable compatibility with lithium metal anodes(LMAs)and suitability for in-situ polymerization.However,poor thermal stability,insufficient ionic conductivity and narrow electrochemical stability window(ESW)hinder its further application in lithium metal batteries(LMBs).To ameliorate these problems,we have successfully synthesized a polymerized-ionic-liquid(PIL)monomer named DIMTFSI by modifying DOL with imidazolium cation coupled with TFSI^(-)anion,which simultaneously inherits the lipophilicity of DOL,high ionic conductivity of imidazole,and excellent stability of PILs.Then the tridentate crosslinker trimethylolpropane tris[3-(2-methyl-1-aziridine)propionate](TTMAP)was introduced to regulate the excessive Li^(+)-O coordination and prepare a flame-retardant SPE(DT-SPE)with prominent thermal stability,wide ESW,high ionic conductivity and abundant Lit transference numbers(t_(Li+)).As a result,the LiFePO_(4)|DT-SPE|Li cell exhibits a high initial discharge specific capacity of 149.60 mAh g^(-1)at 0.2C and 30℃with a capacity retention rate of 98.68%after 500 cycles.This work provides new insights into the structural design of PIL-based electrolytes for long-cycling LMBs with high safety and stability.

关 键 词：Polymerized ionic liquid Solid polymer electrolyte Structural design Crosslinked 3D network Lithium metal battery 

分 类 号：TM912[电气工程—电力电子与电力传动]