Wen Kaihua, Guan Shundong, Liu Sijie, Yuan Haocheng, Liang Ying, Yu Dengfeng, Zhang Zheng, Li Liangliang, Nan Ce-Wen
State Key Laboratory of New Ceramics and Fine Processing, School of Materials Science and Engineering, Tsinghua University, Beijing, 100084, China.
Small. 2024 Feb;20(6):e2304164. doi: 10.1002/smll.202304164. Epub 2023 Sep 29.
Flexible composite polymer electrolytes (CPEs) with inorganic electrolyte fillers dispersed in polymer electrolytes integrate the merits of the polymer and inorganic electrolytes and have attracted much attention in recent years. In order to increase the electrochemical performance, especially the low lithium (Li)-ion transference number in traditional dual-ion Li salt-containing CPEs, single-ion conductive CPEs are synthesized with a single-ion polymer conductor (SIPC) as the matrix and Li La Zr Ta O (LLZTO) particles as the active fillers. The single-ion conductive CPEs show a high Li-ion transference number (up to 0.96), high room-temperature (RT) ionic conductivity (>1.0 × 10 S cm ), wide electrochemical stability window (>5.0 V, vs Li/Li ), and excellent long-term cycling stability with Li metal at RT (3200 h). Based on the SIPC-LLZTO CPE, the solid-state lithium metal batteries with LiFePO - and LiCoO -based cathodes deliver average discharge capacities of 159 mAh g for 600 cycles and 119 mAh g for 200 cycles at RT, respectively. This study sheds light on the design of high-performance CPEs for next-generation solid-state lithium metal batteries.
无机电解质填料分散在聚合物电解质中的柔性复合聚合物电解质（CPEs）兼具聚合物电解质和无机电解质的优点，近年来备受关注。为了提高电化学性能，特别是传统含双离子锂盐的CPEs中较低的锂离子迁移数，以单离子聚合物导体（SIPC）为基体、LiLaZrTaO（LLZTO）颗粒为活性填料合成了单离子导电CPEs。单离子导电CPEs表现出高锂离子迁移数（高达0.96）、高室温（RT）离子电导率（>1.0×10 S cm）、宽电化学稳定窗口（>5.0 V，相对于Li/Li）以及在室温下与锂金属的优异长期循环稳定性（3200 h）。基于SIPC-LLZTO CPE，具有LiFePO-和LiCoO-基阴极的固态锂金属电池在室温下分别在600次循环和200次循环中提供平均放电容量为159 mAh g和119 mAh g。这项研究为下一代固态锂金属电池高性能CPEs的设计提供了思路。
