Lithium-compatible and air-stable vacancy-rich Li9N2Cl3 for high–areal capacity, long-cycling all–solid-state lithium metal batteries

W. Li; M. Li; P.-H. Chien; S. Wang; C. Yu; G. King; Y. Hu; Q. Xiao; M. Shakouri; R. Feng; B. Fu; H. Abdolvand; A. Fraser; R. Li; Y. Huang; J. Liu; Y. Mo; T.-K. Sham; X. Sun

Science Advances 9 (2023) eadh4626-eadh4626

Attaining substantial areal capacity (>3 mAh/cm2) and extended cycle longevity in all?solid-state lithium metal batteries necessitates the implementation of solid-state electrolytes (SSEs) capable of withstanding elevated critical current densities and capacities. In this study, we report a high-performing vacancy-rich Li9N2Cl3 SSE demonstrating excellent lithium compatibility and atmospheric stability and enabling high?areal capacity, long-lasting all?solid-state lithium metal batteries. The Li9N2Cl3 facilitates efficient lithium-ion transport due to its disordered lattice structure and presence of vacancies. Notably, it resists dendrite formation at 10 mA/cm2 and 10 mAh/cm2 due to its intrinsic lithium metal stability. Furthermore, it exhibits robust dry-air stability. Incorporating this SSE in Ni-rich LiNi0.83Co0.11Mn0.06O2 cathode-based all?solid-state batteries, we achieve substantial cycling stability (90.35% capacity retention over 1500 cycles at 0.5 C) and high areal capacity (4.8 mAh/cm2 in pouch cells). These findings pave the way for lithium metal batteries to meet electric vehicle performance demands. A vacancy-rich Li9N2Cl3 solid-state electrolyte enables high performing all-solid-state lithium metal batteries.