文献类型：期刊文献

英文题名：Ion-Sieving Calixarene Fillers Boost Li plus Transport in Quasi-Solid Electrolytes for High-Loading Lithium Metal Batteries

作者：Liu, Honghao[1];Li, Di[2];Lan, Yu[1];Hu, Tao[1];Yang, Yuzi[1];Zhong, Tianyu[1];Zhou, Miaomiao[3];Guan, Mengjia[1];Li, Yongsheng[1]

机构：[1]East China Univ Sci & Technol, Frontier Sci Ctr Mat Biol & Dynam Chem, Sch Mat Sci & Engn, Key Lab Ultrafine Mat,Minist Educ,Lab Low Dimens M, Shanghai, Peoples R China;[2]Nanjing Univ Sci & Technol, Sch Energy & Power Engn, Nanjing, Peoples R China;[3]Univ Chinese Acad Sci, Hangzhou Inst Adv Study, Sch Chem & Mat Sci, Hangzhou, Peoples R China

年份：2026

外文期刊名：ANGEWANDTE CHEMIE-INTERNATIONAL EDITION

收录：;WOS:【SCI-EXPANDED(收录号:WOS:001776404900001)】；

基金：This work was financially supported by the Shanghai Pilot Program for Basic Research (22TQ1400100-13), and the Leading Talents in Shanghai in 2018.

语种：英文

外文关键词：calixarene; composite quasi-solid electrolyte; high-load electrodes; in situ polymerization; size-selection mechanism

摘要：Calixarenes (CAs), featuring unique cavity architectures and exceptional host-guest capabilities, provide an attractive molecular platform for tailoring ion coordination and transport behaviors in solid-state electrolytes (SSEs). Despite these structural advantages, their potential in SSEs has been rarely explored. Herein, we design a calix[6]arene-functionalized (C6A) polymer quasi-solid electrolyte (PECQSE) via in situ polymerization, in which a cross-linked matrix is formed between urethane-functionalized poly(ethylene oxide) (PEG-IEM) and ethoxylated trimethylolpropane triacrylate (ETPTA). The incorporation of C6A establishes a size-selective, interaction-dominated ion-regulation framework, in which bulky TFSI- exhibit restricted mobility, while Li+ transport is facilitated along conduction pathways, resulting in Li+ transference number of 0.76. Meanwhile, hydrogen-bonding interactions between C6A phenolic hydroxyl groups and urethane segments suppress PEG crystallinity and promote LiTFSI dissociation. These interactions facilitate interfacial LiTFSI reduction and support the formation of a LiF/Li2O-rich SEI, which guides uniform lithium deposition and suppresses dendrite growth. Consequently, Li|Li symmetric cells exhibit ultralong cycling stability exceeding 7000 h with low polarization and high-loading LiFePO4|Li full cells retain 80.6% capacity after 700 cycles at 2 C. The assembled 1 Ah pouch cell delivers excellent safety and durability with 91.8% retention after 240 cycles, demonstrating an effective interfacial engineering strategy for next-generation lithium metal batteries.