Qu Yunpeng, Su Chang, Wang Lin, Li Borui, Jiang Wanyuan, Li Runyang, Pei Mengfan, Song Wenkai, Zhuo Shuo, Jin Xin, Liu Dongming, Jian Xigao, Hu Fangyuan
School of Materials Science and Engineering, State Key Laboratory of Fine Chemicals, Frontiers Science Center for Smart Materials Oriented Chemical Engineering, Technology Innovation Center of High Performance Resin Materials (Liaoning Province), Dalian University of Technology, Dalian, 116024, China.
State Key Laboratory of Fine Chemicals, Frontiers Science Center for Smart Materials Oriented Chemical Engineering, School of Chemical Engineering, Technology Innovation Center of High Performance Resin Materials (Liaoning Province), Dalian University of Technology, Dalian, 116024, China.
Angew Chem Int Ed Engl. 2025 Jul;64(27):e202506731. doi: 10.1002/anie.202506731. Epub 2025 May 30.
Achieving stable operation under a wide temperature range is the direction of development for the practical application of solid-state lithium batteries. However, the suboptimal ionic conductive properties exhibited by the electrolyte, the uncontrolled growth of lithium dendrites due to the deposition of inhomogeneous Li and the potential safety hazards caused by unstable interfaces have seriously affected the cycle life of the battery at extreme temperatures. Herein, a fluoropolymer-containing plastic-crystal-based electrolyte (FPCE) has been developed by means of a structural engineering process, with the objective of optimizing the solid electrolyte interface (SEI). The integration of solvent structure simulation and experimental results demonstrates that FPCE regulates Li transport, promotes the in-situ formation of the LiF-rich inorganic-organic hybrid SEI, and enhances the overall stability of the battery. Consequently, FPCE assists in preserving stable LFP|FPCE|Li cells cycling, with 5000 cycles at a high current density of 10 C and an average capacity decay rate of merely 0.00448% per cycle. Furthermore, the Ah-level pouch cells demonstrate the capacity to operate stably within the temperature range of -10 to 80 °C. This study provides a valuable strategy for the design of wide-temperature solid-state polymer electrolytes.
在宽温度范围内实现稳定运行是固态锂电池实际应用的发展方向。然而，电解质表现出的次优离子传导性能、由于锂不均匀沉积导致的锂枝晶不受控制的生长以及不稳定界面引起的潜在安全隐患，严重影响了电池在极端温度下的循环寿命。在此，通过结构工程工艺开发了一种含氟聚合物的塑性晶体基电解质（FPCE），目的是优化固体电解质界面（SEI）。溶剂结构模拟与实验结果的结合表明，FPCE调节锂传输，促进富含LiF的无机 - 有机混合SEI的原位形成，并增强电池的整体稳定性。因此，FPCE有助于保持稳定的LFP|FPCE|Li电池循环，在10 C的高电流密度下可循环5000次，平均每次循环的容量衰减率仅为0.00448%。此外，Ah级软包电池展示了在-10至80°C温度范围内稳定运行的能力。本研究为宽温度固态聚合物电解质的设计提供了有价值的策略。
