文献类型：期刊文献

英文题名：Ion-Sieving Calixarene Fillers Boost Li+ 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] Lab of Low-Dimensional Materials Chemistry, Key Laboratory for Ultrafine Materials of Ministry of Education, Frontier Science Center of the Materials Biology and Dynamic Chemistry, School of Materials Science and Engineering, East China University of Science and Technology, Shanghai, China; [2] School of Energy and Power Engineering, Nanjing University of Science and Technology, Nanjing, China; [3] School of Chemistry and Materials Science, Hangzhou Institute for Advanced Study, University of Chinese Academy of Sciences, Hangzhou, China

年份：2026

外文期刊名：Angewandte Chemie - International Edition

收录：EI(收录号：20262220812665)

语种：英文

外文关键词：Crosslinking - Ethylene - Fillers - Ions - Lithium - Lithium compounds - Lithium deposits - Lithium-ion batteries - Phosphorus compounds - Polymerization - Seebeck effect - Solid electrolytes - Solid-State Batteries

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 insitu 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 7000h 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. ? 2026 Wiley-VCH GmbH.