Nanoconfined Polymerization Facilitates Efficient Li <sup>+</sup> Transportation in Quasi‐Solid Electrolytes
Tuoya Naren, Qianfeng Gu, Ruheng Jiang, Yanwei Zhao, Lei Zhang, Antai Zhu, Xiang Wang, Jinghang Wu, Zongmin Zheng, Chun‐Sing Lee, Gui‐Chao Kuang, Libao Chen, Fu‐Rong Chen, Qichun Zhang
Abstract
Abstract Conventional gel polymer electrolytes (GPEs) struggle with lithium dendrite growth and long‐term cycling stability due to low ionic conductivity. A nanoconfined polymerization (NCP) strategy was employed to develop a composite GPE (PDA@CityU‐43) comprising porous COF and linear polymers. The crosslinked polymer chains are confined within the nanopores of CityU‐43 along c ‐direction, improving polymer distribution and filler‐polymer compatibility. The PDA@CityU‐43 achieves a high ionic conductivity (6.02 × 10 −3 S cm −1 at 25 °C) and a high Li + transference number (0.82), which is favorable to enhance Li + transport dynamics and induce uniform Li + deposition. Thus, the Li||Li cell can stably operate over 6000 h at 0.1 mA cm −2 and 0.1 mAh cm −2 . The Li||PDA@CityU‐43||LFP demonstrates significantly improved cycling stability at 5C, a reversible capacity of 108 mAh/g after 300 cycles. The Li||PDA@CityU‐43||NCM 811 cells with high mass loading (∼5.8 mg cm −2 ) exhibits 72.5% capacity retention after 100 cycles. This NCP strategy offers a new approach to designing advanced GPEs for Li metal batteries.