Xiong Bing-Qing, Zhang Jianwei, Nian Qingshun, Liu Xiaoye, Jiang Jinyu, Wang Zihong, Yang Zhenzhong, Ren Xiaodi
Hefei National Research Center for Physical Science at the Microscale, CAS Key Laboratory of Materials for Energy Conversion, Department of Materials Science and Engineering, University of Science and Technology of China, Anhui, 230026, China.
Key Laboratory of Polar Materials and Devices (MOE), Department of Electronics, East China Normal University, Shanghai, 200241, China.
Angew Chem Int Ed Engl. 2025 Jan 2;64(1):e202413502. doi: 10.1002/anie.202413502. Epub 2024 Oct 29.
Garnet LiLaZrO (LLZO)-based solid-state electrolytes (SSEs) hold promise for realizing next-generation lithium metal batteries with high energy density. However, the high stiffness of high-temperature sintered LLZO makes it brittle and susceptible to strain during the fabrication of solid-state batteries. Cold-pressed LLZO exhibits improved ductility but suffers from insufficient Li conductivity. Here, we report cold-pressed Ta-doped LLZO (Ta-LZ) particles integrated with ductile LiPSCl (LPSC) via a Li conductive Li-containing Ta-Cl structure. This configuration creates a continuous Li conduction network by enhancing the Li exchange at the Ta-LZ/LPSC interface. The resulting Ta-LZ/LPSC SSE exhibits Li conductivity of 4.42×10 S cm and a low activation energy of 0.31 eV. Li symmetric cells with Ta-LZ/LPSC SSE demonstrate excellent Li dendrite suppression ability, with an improved critical current density of 5.0 mA cm and a prolonged cycle life exceeding 600 h at 1 mA cm. Our finding provides valuable insights into developing cold-pressed ceramic powder electrolytes for high-performance all-solid-state batteries.
基于石榴石型LiLaZrO（LLZO）的固态电解质（SSE）有望实现具有高能量密度的下一代锂金属电池。然而，高温烧结的LLZO的高硬度使其变脆，并且在固态电池制造过程中易受应变影响。冷压LLZO的延展性有所改善，但锂电导率不足。在此，我们报道了通过含锂的Ta-Cl结构将冷压的掺Ta的LLZO（Ta-LZ）颗粒与韧性的LiPSCl（LPSC）集成在一起。这种结构通过增强Ta-LZ/LPSC界面处的锂交换来创建连续的锂传导网络。所得的Ta-LZ/LPSC固态电解质的锂电导率为4.42×10 S cm，活化能低至0.31 eV。具有Ta-LZ/LPSC固态电解质的锂对称电池表现出出色的抑制锂枝晶的能力，临界电流密度提高到5.0 mA cm，在1 mA cm下循环寿命延长超过600 h。我们的发现为开发用于高性能全固态电池的冷压陶瓷粉末电解质提供了有价值的见解。
