Lithium-compatible and air-stable vacancy-rich Li <sub>9</sub> N <sub>2</sub> Cl <sub>3</sub> for high–areal capacity, long-cycling all–solid-state lithium metal batteries
W.S. Li, Minsi Li, Po‐Hsiu Chien, Shuo Wang, Chuang Yu, Graham King, Yongfeng Hu, Qunfeng Xiao, Mohsen Shakouri, Renfei Feng, Bolin Fu, Hamidreza Abdolvand, Adam Fraser, Ruying Li, Yining Huang, Jue Liu, Yifei Mo, Tsun‐Kong Sham, Xueliang Sun
Abstract
Attaining substantial areal capacity (>3 mAh/cm 2 ) 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 Li 9 N 2 Cl 3 SSE demonstrating excellent lithium compatibility and atmospheric stability and enabling high–areal capacity, long-lasting all–solid-state lithium metal batteries. The Li 9 N 2 Cl 3 facilitates efficient lithium-ion transport due to its disordered lattice structure and presence of vacancies. Notably, it resists dendrite formation at 10 mA/cm 2 and 10 mAh/cm 2 due to its intrinsic lithium metal stability. Furthermore, it exhibits robust dry-air stability. Incorporating this SSE in Ni-rich LiNi 0.83 Co 0.11 Mn 0.06 O 2 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/cm 2 in pouch cells). These findings pave the way for lithium metal batteries to meet electric vehicle performance demands.