Origin of dendrite-free lithium deposition in concentrated electrolytes

Chen，Yawei1; Li，Menghao2,3; Liu，Yue4; Jie，Yulin1; Li，Wanxia1; Huang，Fanyang1; Li，Xinpeng1; He，Zixu1; Ren，Xiaodi1; Chen，Yunhua5; Meng，Xianhui5; Cheng，Tao4; Gu，Meng2; Jiao，Shuhong1; Cao，Ruiguo1

2023-12-01

10.1038/s41467-023-38387-8

Nature Communications   影响因子和分区

2041-1723

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.

SCI

英语

NI论文

通讯

Guangdong Innovative and Entrepreneurial Research Team Program[2019ZT08C044];National Natural Science Foundation of China-Yunnan Joint Fund[22279127];National Natural Science Foundation of China-Yunnan Joint Fund[52072358];Science, Technology and Innovation Commission of Shenzhen Municipality[KQTD20190929173815000];National Natural Science Foundation of China-Yunnan Joint Fund[U21A2082];

Science & Technology - Other Topics

Multidisciplinary Sciences

WOS:001053796300022

NATURE PORTFOLIO

2-s2.0-85158949337

Scopus

1.Hefei National Laboratory for Physical Science at Microscale,CAS Key Laboratory of Materials for Energy Conversion,Department of Materials Science and Engineering,University of Science and Technology of China,Hefei,230026,China
2.Department of Materials Science and Engineering,Southern University of Science and Technology,Shenzhen,518055,China
3.School of Materials Science and Engineering,Harbin Institute of Technology,Harbin,150001,China
4.Institute of Functional Nano and Soft Materials (FUNSOM),Soochow University,Suzhou,215123,China
5.NIO Incorporation,Shanghai,201800,China

Chen，Yawei,Li，Menghao,Liu，Yue,et al. Origin of dendrite-free lithium deposition in concentrated electrolytes[J]. Nature Communications,2023,14(1).

Chen，Yawei.,Li，Menghao.,Liu，Yue.,Jie，Yulin.,Li，Wanxia.,...&Cao，Ruiguo.(2023).Origin of dendrite-free lithium deposition in concentrated electrolytes.Nature Communications,14(1).

Chen，Yawei,et al."Origin of dendrite-free lithium deposition in concentrated electrolytes".Nature Communications 14.1(2023).