Lithium-compatible and air-stable vacancy-rich Li 9 N 2 Cl 3 for high–areal capacity, long-cycling all–solid-state lithium metal batteries

Author:

Li Weihan12ORCID,Li Minsi12ORCID,Chien Po-Hsiu3ORCID,Wang Shuo4ORCID,Yu Chuang1,King Graham5ORCID,Hu Yongfeng5ORCID,Xiao Qunfeng5,Shakouri Mohsen5ORCID,Feng Renfei5ORCID,Fu Bolin1ORCID,Abdolvand Hamidreza1ORCID,Fraser Adam1,Li Ruying1ORCID,Huang Yining3ORCID,Liu Jue3ORCID,Mo Yifei46ORCID,Sham Tsun-Kong2ORCID,Sun Xueliang17ORCID

Affiliation:

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/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.

Publisher

American Association for the Advancement of Science (AAAS)

Subject

Multidisciplinary

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