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Cited by 409Advanced Battery Materials and TechnologiesAdvancements in Battery MaterialsAdvanced Battery Technologies Research

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

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Wang, Xuefeng, Zhang, Minghao, Alvarado, Judith, Wang, Shen, Sina, Mahsa, Lu, Bingyu, Bouwer, James, Xu, Wu +4 more·2017·Nano Letters
DOI 10.1021/acs.nanolett.7b03606
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Abstract

Lithium metal has been considered the “holy grail” anode material for rechargeable batteries despite the fact that its 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 accompanying solid electrolyte interphase (SEI). To prevent the dendritic growth and enhance the electrochemical reversibility, it is crucial to understand the nano- and mesostructures 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 nanoscale while minimizing beam damage during imaging. Surprisingly, the results show that the nucleation-dominated EDLi (5 min 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 also yield crucial structural information on the EDLi evolution with and without electrolyte additives.

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  • Cryo-TEM for the first time elucidated the nanostructure of electrochemically deposited Li (EDLi) and its surface SEI film.

    “For the first time, cryo-TEM elucidates the nanostructure of the electrochemically deposited Li (EDLi) and its surface SEI film.”

    From Review on Low-Temperature Electrolytes for Lithium-Ion and Lithium Metal Batteries (2023) · cites this paper as [164]

  • Cryo-EM outperforms other techniques for characterizing the sensitive chemical composition, spatial distribution, and nanoscale morphology of the SEI.

    “In the former [164], cryo-EM was reported to outperform other techniques used for characterizing the sensitive chemical composition and spatial distribution of the SEI, as well as the morphology at nanoscale.”

    From Review on Low-Temperature Electrolytes for Lithium-Ion and Lithium Metal Batteries (2023) · cites this paper as [164]

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Cited by

Sorted by citations

Authors
Wang, X., Zhang, M., Alvarado, J., Wang, S., Sina, M., Lu, B., Bouwer, J., Xu, W., Xiao, J., Zhang, J.-G., Liu, J., & Meng, Y. S.
Affiliations
Pacific Northwest National Laboratory (US)
Corresponding author
Meng, Ying Shirley
ORCID
Venue
Nano Letters
Publisher
American Chemical Society (ACS)
Published
2017-11-02
Volume
17
Issue
12
Pages
7606-7612
ISSN
  • 1530-6984 (ISSN-L)
  • 1530-6992
DOI
10.1021/acs.nanolett.7b03606
OpenAlex
W2767187748
Cited by
409
References
2
Citations by year
2026: 23 · 2025: 32 · 2024: 49 · 2023: 45 · 2022: 44 · 2021: 65 · 2020: 61 · 2019: 59 · 2018: 30 · 2017: 1
FWCI
17.17
Type
journal article
Language
en
Open access
Locations
  • Nano Letters (publishedVersion)
  • PubMed (publishedVersion)
  • OSTI OAI (U.S. Department of Energy Office of Scientific and Technical Information) (submittedVersion)
  • eScholarship (California Digital Library) (submittedVersion)
Funders
Vehicle Technologies Program
Topics
  • Physical Sciences › Engineering › Electrical and Electronic Engineering › Advanced Battery Materials and Technologies
  • Physical Sciences › Engineering › Electrical and Electronic Engineering › Advancements in Battery Materials
  • Physical Sciences › Engineering › Automotive Engineering › Advanced Battery Technologies Research
Keywords
lithium metal anode, solid electrolyte interphase, lithium dendrite growth, Coulombic efficiency, cryo-electron microscopy, beam damage, lithium fluoride, electrolyte additives, lithium nucleation
MeSH terms
Electric Conductivity, Electrolytes, Fluorides, Lithium, Membranes, Artificial, Lithium Compounds, Microscopy, Electron, Transmission, Electrochemical Techniques

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