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.

Li, Weihan; Li, Minsi; Chien, Po-Hsiu; Wang, Shuo; Yu, Chuang; King, Graham; Hu, Yongfeng; Xiao, Qunfeng et al. · Sci Adv · 2023

basic_science · Level V

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Abstract

Attaining substantial areal capacity (>3 mAh/cm<sup>2</sup>) 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<sub>9</sub>N<sub>2</sub>Cl<sub>3</sub> SSE demonstrating excellent lithium compatibility and atmospheric stability and enabling high-areal capacity, long-lasting all-solid-state lithium metal batteries. The Li<sub>9</sub>N<sub>2</sub>Cl<sub>3</sub> facilitates efficient lithium-ion transport due to its disordered lattice structure and presence of vacancies. Notably, it resists dendrite formation at 10 mA/cm<sup>2</sup> and 10 mAh/cm<sup>2</sup> due to its intrinsic lithium metal stability. Furthermore, it exhibits robust dry-air stability. Incorporating this SSE in Ni-rich LiNi<sub>0.83</sub>Co<sub>0.11</sub>Mn<sub>0.06</sub>O<sub>2</sub> 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<sup>2</sup> in pouch cells). These findings pave the way for lithium metal batteries to meet electric vehicle performance demands.