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Nature Communications, volume 14, issue 1, publication number 2655

Origin of dendrite-free lithium deposition in concentrated electrolytes

Yawei Chen 1
Menghao Li 2, 3
Yue Liu 4
Yulin Jie 1
Wanxia Li 1
Fanyang Huang 1
Xinpeng Li 1
Zixu He 1
Xiaodi Ren 1
Yunhua Chen 5
Xianhui Meng 5
Tao Cheng 4
Meng Gu 2
Shuhong Jiao 1
Ruiguo Cao 1
Publication typeJournal Article
Publication date2023-05-09
Quartile SCImago
Q1
Quartile WOS
Q1
Impact factor16.6
ISSN20411723, 20411723
General Chemistry
General Biochemistry, Genetics and Molecular Biology
Multidisciplinary
General Physics and Astronomy
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.

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GOST Copy
Chen Y. et al. Origin of dendrite-free lithium deposition in concentrated electrolytes // Nature Communications. 2023. Vol. 14. No. 1. 2655
GOST all authors (up to 50) Copy
Chen Y., Li M., Liu Y., Jie Y., Li W., Huang F., Li X., He Z., Ren X., Chen Y., Meng X., Cheng T., Gu M., Jiao S., Cao R. Origin of dendrite-free lithium deposition in concentrated electrolytes // Nature Communications. 2023. Vol. 14. No. 1. 2655
RIS |
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RIS Copy
TY - JOUR
DO - 10.1038/s41467-023-38387-8
UR - https://doi.org/10.1038/s41467-023-38387-8
TI - Origin of dendrite-free lithium deposition in concentrated electrolytes
T2 - Nature Communications
AU - Chen, Yawei
AU - Li, Menghao
AU - Liu, Yue
AU - Jie, Yulin
AU - Li, Wanxia
AU - Huang, Fanyang
AU - Li, Xinpeng
AU - He, Zixu
AU - Ren, Xiaodi
AU - Chen, Yunhua
AU - Meng, Xianhui
AU - Cheng, Tao
AU - Gu, Meng
AU - Jiao, Shuhong
AU - Cao, Ruiguo
PY - 2023
DA - 2023/05/09 00:00:00
PB - Springer Nature
IS - 1
VL - 14
SN - 2041-1723
SN - 2041-1723
ER -
BibTex
Cite this
BibTex Copy
@article{2023_Chen,
author = {Yawei Chen and Menghao Li and Yue Liu and Yulin Jie and Wanxia Li and Fanyang Huang and Xinpeng Li and Zixu He and Xiaodi Ren and Yunhua Chen and Xianhui Meng and Tao Cheng and Meng Gu and Shuhong Jiao and Ruiguo Cao},
title = {Origin of dendrite-free lithium deposition in concentrated electrolytes},
journal = {Nature Communications},
year = {2023},
volume = {14},
publisher = {Springer Nature},
month = {may},
url = {https://doi.org/10.1038/s41467-023-38387-8},
number = {1},
doi = {10.1038/s41467-023-38387-8}
}
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