Origin of dendrite-free lithium deposition in concentrated electrolytes

Yawei Chen, Menghao Li, Yue Liu, Yulin Jie, Wanxia Li, Fanyang Huang, Xinpeng Li, Zixu He, Xiaodi Ren, Yunhua Chen, Xianhui Meng, Tao Cheng (), Meng Gu (), Shuhong Jiao () and Ruiguo Cao ()
Additional contact information
Yawei Chen: University of Science and Technology of China
Menghao Li: Southern University of Science and Technology
Yue Liu: Soochow University
Yulin Jie: University of Science and Technology of China
Wanxia Li: University of Science and Technology of China
Fanyang Huang: University of Science and Technology of China
Xinpeng Li: University of Science and Technology of China
Zixu He: University of Science and Technology of China
Xiaodi Ren: University of Science and Technology of China
Yunhua Chen: NIO Incorporation
Xianhui Meng: NIO Incorporation
Tao Cheng: Soochow University
Meng Gu: Southern University of Science and Technology
Shuhong Jiao: University of Science and Technology of China
Ruiguo Cao: University of Science and Technology of China

Nature Communications, 2023, vol. 14, issue 1, 1-12

Abstract: Abstract The electrolyte solvation structure and the solid-electrolyte interphase (SEI) formation are critical to dictate the morphology of lithium deposition in organic electrolytes. However, the link between the electrolyte solvation structure and SEI composition and its implications on lithium morphology evolution are poorly understood. Herein, we use a single-salt and single-solvent model electrolyte system to systematically study the correlation between the electrolyte solvation structure, SEI formation process and lithium deposition morphology. The mechanism of lithium deposition is thoroughly investigated using cryo-electron microscopy characterizations and computational simulations. It is observed that, in the high concentration electrolytes, concentrated Li+ and anion-dominated solvation structure initiate the uniform Li nucleation kinetically and favor the decomposition of anions rather than solvents, resulting in inorganic-rich amorphous SEI with high interface energy, which thermodynamically facilitates the formation of granular Li. On the contrary, solvent-dominated solvation structure in the low concentration electrolytes tends to exacerbate the solvolysis process, forming organic-rich mosaic SEI with low interface energy, which leads to aggregated whisker-like nucleation and growth. These results are helpful to tackle the long-standing question on the origin of lithium dendrite formation and guide the rational design of high-performance electrolytes for advanced lithium metal batteries.

Date: 2023
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DOI: 10.1038/s41467-023-38387-8

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