Ultralow Young's Modulus Phosphosulfate Solid Electrolytes for High-Voltage All-Solid-State Batteries.

作者：Jia-Cong Li, Yu-Ge Cao, Pushun Lu, Wu-Jie Dong, Zhongxing Xu, Yan Liu, Ying-Jie Wan, Hui Bi, Fu-Qiang Huang · 发表于：Small · 年份：2026 · DOI：10.1002/smll.74986 · 研究领域：Medicine

Intimate solid-solid interfacial contact is critical for high-performance all-solid-state lithium batteries (ASSLBs), which require solid-state electrolytes (SSEs) with exceptional mechanical softness to eliminate grain boundaries. Oxide, sulfide, and halide solid electrolytes all fail to balance Young's modulus, ionic conductivity, and high-voltage oxidation stability, with each having a respective drawback in one of the three properties. Herein, we develop nanocrystalline/amorphous composite oxyanion-halide SSEs through dual-anion engineering by incorporating SO4 2- or PO4 3- into a zirconium chloride matrix. The optimized sulfate-based and phosphate-based electrolytes exhibit local Young's modulus of ∼0.4 and ∼0.9 GPa, with room-temperature ionic conductivities of 2.1 and 2.2 mS cm- 1, respectively. These SSEs also show high oxidative stability and cost-effectiveness ($79.7 US kg-1). When paired with 4.6 V high-voltage cathodes (LiCoO2, NCM88), ASSLBs deliver remarkable cycling performance: >90% capacity retention after 1000 cycles and >70% after 1800 cycles at 1 C. This design resolves the core interfacial challenge for ASSLBs, offering a practical, low-cost electrolyte solution for next-generation high-energy-density batteries.