Citation: Hai Su, Haikuo Zhang, Zifeng Chen, Mengjie Li, Jiwei Zhao, Haiyan Xun, Jie Sun, Yunhua Xu. Electrolyte and interphase engineering through solvation structure regulation for stable lithium metal batteries[J]. Chinese Chemical Letters, ;2023, 34(12): 108640. doi: 10.1016/j.cclet.2023.108640 shu

Electrolyte and interphase engineering through solvation structure regulation for stable lithium metal batteries

Hai Su ^a ,
Haikuo Zhang ^b ,
Zifeng Chen ^a ,
Mengjie Li ^a ,
Jiwei Zhao ^a ,
Haiyan Xun ^a ,
Jie Sun ^c ,
Yunhua Xu ^{a, *,}

a.
School of Materials Science and Engineering, Key Laboratory of Advanced Ceramics and Machining Technology (Ministry of Education), and Tianjin Key Laboratory of Composite and Functional Materials, Tianjin University, Tianjin 300072, China
b.
State Key Laboratory of Silicon Materials, School of Materials Science and Engineering, Zhejiang University, Hangzhou 310027, China
c.
Key Laboratory for Green Chemical Technology of Ministry of Education, School of Chemical Engineering and Technology, Tianjin University, Tianjin 300072, China

yunhua.xu@tju.edu.cn

Received Date: 4 May 2023
Revised Date: 15 May 2023
Accepted Date: 31 May 2023
Available Online: 4 June 2023

Figures(6)

Lithium metal batteries (LMBs) are considered to be one of the most promising high-energy-density battery systems. However, their practical application in carbonate electrolytes is hampered by lithium dendrite growth, resulting in short cycle life. Herein, an electrolyte regulation strategy is developed to improve the cyclability of LMBs in carbonate electrolytes by introducing LiNO₃ using trimethyl phosphate with a slightly higher donor number compared to NO₃⁻ as a solubilizer. This not only allows the formaion of Li⁺-coordinated NO₃⁻ but also achieves the regulation of electrolyte solvation structures, leading to the formation of robust and ion-conductive solid-electrolyte interphase films with inorganic-rich inner and organic-rich outer layers on the Li metal anodes. As a result, high Coulombic efficiency of 99.1% and stable plating/stripping cycling of Li metal anode in Li||Cu cells were realized. Furthermore, excellent performance was also demonstrated in Li||LiNi_0.83Co_0.11Mn_0.06O₂ (NCM83) full cells and Cu||NCM83 anode-free cells using high mass-loading cathodes. This work provides a simple interphase engineering strategy through regulating the electrolyte solvation structures for high-energy-density LMBs.
- Lithium metal batteries,
- Lithium nitrate,
- Trimethyl phosphate,
- Solvation structures,
- Solid-electrolyte interphases
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