Lithium-compatible and air-stable vacancy-rich Li9N2Cl3 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; Shakouri, Mohsen; Feng, Renfei; Fu, Bolin; Abdolvand, Hamidreza; Fraser, Adam; Li, Ruying; Huang, Yining; Liu, Jue; Mo, Yifei; Sham, Tsun-Kong; Sun, Xueliang

doi:10.1126/sciadv.adh4626

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

Journal Article · Fri Oct 20 00:00:00 EDT 2023 · Science Advances

DOI:https://doi.org/10.1126/sciadv.adh4626· OSTI ID:2204560

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Western University, London, ON (Canada)
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)
University of Maryland, College Park, MD (United States)
Canadian Light Source, Saskatoon, SK (Canada)
Western University, London, ON (Canada); Eastern Institute for Advanced Study, Eastern Institute of Technology, Ningbo (China)

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 LiNi_0.83Co_0.11Mn_0.06O₂ 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.

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Research Organization:: Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities (SUF); National Science Foundation (NSF)

Grant/Contract Number:: AC05-00OR22725; 1940166

OSTI ID:: 2204560

Journal Information:: Science Advances, Vol. 9, Issue 42; ISSN 2375-2548

Publisher:: AAASCopyright Statement

Country of Publication:: United States

Language:: English

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