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

Weihan 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

doi:10.1126/sciadv.adh4626

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

Sci Adv. 2023 Oct 20;9(42):eadh4626. doi: 10.1126/sciadv.adh4626. Epub 2023 Oct 20.

Authors

Weihan Li^{1

2}, Minsi Li^{1

2}, Po-Hsiu Chien³, Shuo Wang⁴, Chuang Yu¹, Graham King⁵, Yongfeng Hu⁵, Qunfeng Xiao⁵, Mohsen Shakouri⁵, Renfei Feng⁵, Bolin Fu¹, Hamidreza Abdolvand¹, Adam Fraser¹, Ruying Li¹, Yining Huang³, Jue Liu³, Yifei Mo^{4

6}, Tsun-Kong Sham², Xueliang Sun^{1

7}

Affiliations

¹ Department of Mechanical and Materials Engineering, Western University, London, ON N6A 5B9, Canada.
² Department of Chemistry and Soochow-Western Centre for Synchrotron Radiation Research, Western University, London, ON N6A 5B7, Canada.
³ Neutron Scattering Division, Oak Ridge National Laboratory, Oak Ridge, TN 37831, USA.
⁴ Department of Materials Science and Engineering, University of Maryland, College Park, MD 20742, USA.
⁵ Canadian Light Source, 44 Innovation Boulevard, Saskatoon, SK S7N 2V3, Canada.
⁶ Maryland Energy Innovation, University of Maryland, College Park, MD 20742, USA.
⁷ Eastern Institute for Advanced Study, Eastern Institute of Technology, Ningbo, Zhejiang 315200, P.R. China.

Abstract

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.