Molecule‑Level Multiscale Design of Nonflammable Gel Polymer Electrolyte to Build Stable SEI/CEI for Lithium Metal Battery  

作　　者：Qiqi Sun Zelong Gong Tao Zhang Jiafeng Li Xianli Zhu Ruixiao Zhu Lingxu Wang Leyuan Ma Xuehui Li Miaofa Yuan Zhiwei Zhang Luyuan Zhang Zhao Qian Longwei Yin Rajeev Ahuja Chengxiang Wang 

机构地区：[1]Key Laboratory for Liquid‑Solid Structural Evolution and Processing of Materials(Ministry of Education),School of Materials Science and Engineering,Shandong University,Jinan 250061,People’s Republic of China [2]Condensed Matter Theory,Department of Physics and Astronomy,Uppsala University,Uppsala 75120,Sweden

出　　处：《Nano-Micro Letters》2025年第1期404-423,共20页纳微快报（英文版）

基　　金：supported by the National Natural Science Foundation of China(Nos.52172214,52272221,52171182);the Postdoctoral Innovation Project of Shandong Province(No.202102003);The Key Research and Development Program of Shandong Province(2021ZLGX01);the Qilu Young Scholar Program;HPC Cloud Platform of Shandong University are also thanked.

摘　　要：The risk of flammability is an unavoidable issue for gel polymer electrolytes(GPEs).Usually,flameretardant solvents are necessary to be used,but most of them would react with anode/cathode easily and cause serious interfacial instability,which is a big challenge for design and application of nonflammable GPEs.Here,a nonflammable GPE(SGPE)is developed by in situ polymerizing trifluoroethyl methacrylate(TFMA)monomers with flame-retardant triethyl phosphate(TEP)solvents and LiTFSI–LiDFOB dual lithium salts.TEP is strongly anchored to PTFMA matrix via polarity interaction between-P=O and-CH_(2)CF_(3).It reduces free TEP molecules,which obviously mitigates interfacial reactions,and enhances flame-retardant performance of TEP surprisingly.Anchored TEP molecules are also inhibited in solvation of Li^(+),leading to anion-dominated solvation sheath,which creates inorganic-rich solid electrolyte interface/cathode electrolyte interface layers.Such coordination structure changes Li^(+)transport from sluggish vehicular to fast structural transport,raising ionic conductivity to 1.03 mS cm^(-1) and transfer number to 0.41 at 30℃.The Li|SGPE|Li cell presents highly reversible Li stripping/plating performance for over 1000 h at 0.1 mA cm^(−2),and 4.2 V LiCoO_(2)|SGPE|Li battery delivers high average specific capacity>120 mAh g^(−1) over 200 cycles.This study paves a new way to make nonflammable GPE that is compatible with Li metal anode.

关 键 词：Anchoring effect Nonflammable gel electrolyte In situ cross-linked Electrode-electrolyte interface Li metal battery 

分 类 号：TQ317[化学工程—高聚物工业] TM912[电气工程—电力电子与电力传动]