Observing the structural diversity of electrochemically deposited lithium metal in three dimensions

Li，Xiangyan1; Han，Bing1; Zou，Yucheng1; Ke，Ruohong1; Deng，Yonghong1; Wu，Sudong2,3,4; Zhao，Yusheng6; Shao，Huaiyu5; Guo，Junpo5; Gu，Meng1

2023-05-30

10.1016/j.jpowsour.2023.232948

JOURNAL OF POWER SOURCES   Impact Factor & Quartile

0378-7753

1873-2755

Lithium metal batteries (LMBs) are considered to be next-generation high-energy-density storage devices because of the ultrahigh theoretical specific capacity and low reduction potential of the Li metal anode. The electroplating/stripping behavior of Li metal and the properties of the solid-electrolyte interphase (SEI) are key issues that must be well understood. Traditional structural investigations using electron microscopy can facilitate this understanding, but they lack three-dimensional information. Herein, the burgeoning technique, cryogenic electron tomography, is used in the study of LMBs to visualize the morphology of electrochemically deposited Li metal and the SEI in various electrolytes. High-aspect-ratio dendrites are formed in ethylene carbonate-diethyl carbonate (EC-DEC) and EC-DEC/vinylene carbonate electrolytes, whereas irregularly shaped Li metal is formed in an EC-DEC-fluoroethylene carbonate electrolyte. In contrast, the use of a 1,3-dioxolane-1,2-dimethoxyethane-LiNO electrolyte produces spherical Li metal. Three-dimensional reconstructions of the Li dendrites formed after half-charging revealed polyhedral-shaped “dead Li” tightly wrapped by a folded SEI layer, indicating the mechanism of “dead Li” formation. The non-uniform stripping rate of Li and the elimination of electron conduction paths by the surrounding SEI husks lead to the formation of such “dead Li.”

Cryogenic electron tomography Dead Li Deposited metallic Li Li metal battery Solid-electrolyte interphase

SCI

English

First ; Corresponding

National Natural Science Foundation of China[52273225] ; Shenzhen Fundamental Research Funding[JCYJ20210324115809026] ; Shenzhen Natural Science Fund[20200925154115001] ; Shenzhen Science and Technology Program[KQTD20190929173815000] ; Guangdong Innovative and Entrepreneurial Research Team Program[2019ZT08C044] ; China Postdoctoral Science Foundation[2022M711467]

Chemistry ; Electrochemistry ; Energy & Fuels ; Materials Science

Chemistry, Physical ; Electrochemistry ; Energy & Fuels ; Materials Science, Multidisciplinary

WOS:000960456200001

ELSEVIER

MATERIALS SCIENCE

2-s2.0-85150423215

Scopus

1.Department of Materials Science and Engineering,Southern University of Science and Technology,Shenzhen,518055,China
2.Academy for Advanced Interdisciplinary Studies,Southern University of Science and Technology,Shenzhen,518055,China
3.Guangdong-Hong Kong-Macao Joint Laboratory for Photonic-Thermal-Electrical Energy Materials and Devices,Southern University of Science and Technology,Shenzhen,518055,China
4.Key Laboratory of Energy Conversion and Storage Technologies,Southern University of Science and Technology,Shenzhen,518055,China
5.Joint Key Laboratory of the Ministry of Education,Institute of Applied Physics and Materials Engineering (IAPME),University of Macau,Macau SAR,China
6.Eastern Institute for Advanced Study,Zhejiang,315200,China

Li，Xiangyan,Han，Bing,Zou，Yucheng,et al. Observing the structural diversity of electrochemically deposited lithium metal in three dimensions[J]. JOURNAL OF POWER SOURCES,2023,567.

Li，Xiangyan.,Han，Bing.,Zou，Yucheng.,Ke，Ruohong.,Deng，Yonghong.,...&Gu，Meng.(2023).Observing the structural diversity of electrochemically deposited lithium metal in three dimensions.JOURNAL OF POWER SOURCES,567.

Li，Xiangyan,et al."Observing the structural diversity of electrochemically deposited lithium metal in three dimensions".JOURNAL OF POWER SOURCES 567(2023).