文献类型：期刊文献

英文题名：In Situ Dual Crosslinked Composite Quasi-Solid Electrolytes Enable Multiple Continuous Ion Transport Channels for Ultra-Long Cycle and High Load Lithium Metal Batteries

作者：Liu, Honghao[1];Li, Di[2];Yang, Yuzi[1];Lan, Yu[1];Zhao, Xianming[1];Zhong, Tianyu[1];Hu, Tao[1];Luo, Songteng[1];Guan, Mengjia[1];Li, Yongsheng[1]

机构：[1]East China Univ Sci & Technol, Sch Mat Sci & Engn, Shanghai Engn Res Ctr Hierarch Nanomat,Lab Low Dim, Frontier Sci Ctr Mat Biol & Dynam Chem,Minist Educ, Shanghai 200237, Peoples R China;[2]Nanjing Univ Sci & Technol, Sch Energy & Power Engn, Nanjing 210094, Peoples R China

年份：2025

卷号：15

期号：34

外文期刊名：ADVANCED ENERGY MATERIALS

收录：;EI(收录号：20252718711860);WOS:【SCI-EXPANDED(收录号:WOS:001519034300001)】；

基金：H.L. and D.L. contributed equally to this work. This work was funded by the Shanghai Pilot Program for Basic Research (22TQ1400100-13). The Leading Talents in Shanghai in 2018. The 111 project (B14018).

语种：英文

外文关键词：composite quasi-solid electrolyte; high-loading electrode; in situ polymerization; ultra-long cycle; zeolite

摘要：Composite quasi-solid electrolytes (CQSEs) have emerged as promising candidates for solid-state lithium metal batteries (SSLMBs) through synergistic integration of inorganic fillers and polymer matrices. However, intrinsic interfacial incompatibility between organic/inorganic phases impedes continuous Li+ migration pathways, leading to compromised ionic dynamics and cycling stability. In this work, surface-modifiable lithiated zeolite (LiZSM-5) is utilized for functional group grafting and designing a hemiacetal-amine polymer (Trimer) with fast ion conduction. A dual-crosslinked CQSE with multiple continuous Li+ transport channels through integrated zeolite frameworks and polymeric conduction networks has been obtained by in situ polymerization. Combined experimental and computational analyses reveal that the abundant copolymer chain segments synergistically interact with Lewis acid sites on LiZSM-5, optimizing Li+ transport pathways to achieve exceptional ionic conductivity (3.7 mS cm-1) and Li+ transference number (0.89). The optimized CQSE enables ultralong cycling stability exceeding 11 000 h in Li symmetric cells and sustains 800 cycles in LiNi0.8Co0.1Mn0.1O2|CQSE|Li full cells at 0.5 C with high active material loading. Remarkably, 1 Ah soft-pack battery displays excellent cycling stability alongside excellent safety characteristics under mechanical abuse tests. This interfacial engineering strategy provides fundamental insights into constructing continuous ion-transport networks through organic/inorganic phase coordination, suggesting promising avenues for a scalable high-energy-density battery.