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Title: New Insights on the Structure of Electrochemically Deposited Lithium Metal and Its Solid Electrolyte Interphases via Cryogenic TEM

Abstract

Lithium metal has been considered as the “holy grail” anode material for rechargeable batteries though the dendritic growth and low Coulombic efficiency (CE) have crippled its practical use for decades. Its high chemical reactivity and low stability make it difficult to explore the intrinsic chemical and physical properties of the electrochemically deposited lithium (EDLi) and its accompanied solid electrolyte interphase (SEI). To prevent the dendritic growth and enhance the electrochemical reversibility, it is crucial to understand the nano- and meso- structures of EDLi. However, Li metal is very sensitive to beam damage and has low contrast for commonly used characterization techniques such as electron microscopy. Inspired by biological imaging techniques, this work demonstrates the power of cryogenic (cryo)- electron microscopy to reveal the detailed structure of EDLi and the SEI composition at the nano scale while minimizing beam damage during imaging. Surprisingly, the results show that the nucleation dominated EDLi (five minutes at 0.5 mA cm-2) is amorphous while there is some crystalline LiF present in the SEI. The EDLi grown from various electrolytes with different additives exhibits distinctive surface properties. Consequently, these results highlight the importance of the SEI and its relationship with the CE. Our findings not onlymore » illustrate the capabilities of cryogenic microscopy for beam (thermal)-sensitive materials, but it yields crucial structural information of the EDLi evolution with and without electrolyte additives.« less

Authors:
ORCiD logo; ; ; ; ; ; ; ORCiD logo [1];  [1]; ORCiD logo [1]; ORCiD logo [1]; ORCiD logo
  1. Energy and Environmental Directorate, Pacific Northwest National Laboratory, 902 Battelle Boulevard, Richland, Washington 99354, United States
Publication Date:
Research Org.:
Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
Sponsoring Org.:
USDOE Office of Energy Efficiency and Renewable Energy (EERE), Vehicle Technologies Office (EE-3V)
OSTI Identifier:
1414546
Report Number(s):
PNNL-SA-128910
Journal ID: ISSN 1530-6984; VT1201000
DOE Contract Number:
AC05-76RL01830
Resource Type:
Journal Article
Resource Relation:
Journal Name: Nano Letters; Journal Volume: 17; Journal Issue: 12
Country of Publication:
United States
Language:
English
Subject:
Li metal; electrochemical deposition; SEI

Citation Formats

Wang, Xuefeng, Zhang, Minghao, Alvarado, Judith, Wang, Shen, Sina, Mahsa, Lu, Bingyu, Bouwer, James, Xu, Wu, Xiao, Jie, Zhang, Ji-Guang, Liu, Jun, and Meng, Ying Shirley. New Insights on the Structure of Electrochemically Deposited Lithium Metal and Its Solid Electrolyte Interphases via Cryogenic TEM. United States: N. p., 2017. Web. doi:10.1021/acs.nanolett.7b03606.
Wang, Xuefeng, Zhang, Minghao, Alvarado, Judith, Wang, Shen, Sina, Mahsa, Lu, Bingyu, Bouwer, James, Xu, Wu, Xiao, Jie, Zhang, Ji-Guang, Liu, Jun, & Meng, Ying Shirley. New Insights on the Structure of Electrochemically Deposited Lithium Metal and Its Solid Electrolyte Interphases via Cryogenic TEM. United States. doi:10.1021/acs.nanolett.7b03606.
Wang, Xuefeng, Zhang, Minghao, Alvarado, Judith, Wang, Shen, Sina, Mahsa, Lu, Bingyu, Bouwer, James, Xu, Wu, Xiao, Jie, Zhang, Ji-Guang, Liu, Jun, and Meng, Ying Shirley. Thu . "New Insights on the Structure of Electrochemically Deposited Lithium Metal and Its Solid Electrolyte Interphases via Cryogenic TEM". United States. doi:10.1021/acs.nanolett.7b03606.
@article{osti_1414546,
title = {New Insights on the Structure of Electrochemically Deposited Lithium Metal and Its Solid Electrolyte Interphases via Cryogenic TEM},
author = {Wang, Xuefeng and Zhang, Minghao and Alvarado, Judith and Wang, Shen and Sina, Mahsa and Lu, Bingyu and Bouwer, James and Xu, Wu and Xiao, Jie and Zhang, Ji-Guang and Liu, Jun and Meng, Ying Shirley},
abstractNote = {Lithium metal has been considered as the “holy grail” anode material for rechargeable batteries though the dendritic growth and low Coulombic efficiency (CE) have crippled its practical use for decades. Its high chemical reactivity and low stability make it difficult to explore the intrinsic chemical and physical properties of the electrochemically deposited lithium (EDLi) and its accompanied solid electrolyte interphase (SEI). To prevent the dendritic growth and enhance the electrochemical reversibility, it is crucial to understand the nano- and meso- structures of EDLi. However, Li metal is very sensitive to beam damage and has low contrast for commonly used characterization techniques such as electron microscopy. Inspired by biological imaging techniques, this work demonstrates the power of cryogenic (cryo)- electron microscopy to reveal the detailed structure of EDLi and the SEI composition at the nano scale while minimizing beam damage during imaging. Surprisingly, the results show that the nucleation dominated EDLi (five minutes at 0.5 mA cm-2) is amorphous while there is some crystalline LiF present in the SEI. The EDLi grown from various electrolytes with different additives exhibits distinctive surface properties. Consequently, these results highlight the importance of the SEI and its relationship with the CE. Our findings not only illustrate the capabilities of cryogenic microscopy for beam (thermal)-sensitive materials, but it yields crucial structural information of the EDLi evolution with and without electrolyte additives.},
doi = {10.1021/acs.nanolett.7b03606},
journal = {Nano Letters},
number = 12,
volume = 17,
place = {United States},
year = {Thu Nov 02 00:00:00 EDT 2017},
month = {Thu Nov 02 00:00:00 EDT 2017}
}