High rate and stable cycling of lithium metal anode
Open accessAbstract
Lithium metal is an ideal battery anode. However, dendrite growth and limited Coulombic efficiency during cycling have prevented its practical application in rechargeable batteries. Herein, we report that the use of highly concentrated electrolytes composed of ether solvents and the lithium bis(fluorosulfonyl)imide salt enables the high-rate cycling of a lithium metal anode at high Coulombic efficiency (up to 99.1%) without dendrite growth. With 4 M lithium bis(fluorosulfonyl)imide in 1,2-dimethoxyethane as the electrolyte, a lithium|lithium cell can be cycled at 10 mA cm(-2) for more than 6,000 cycles, and a copper|lithium cell can be cycled at 4 mA cm(-2) for more than 1,000 cycles with an average Coulombic efficiency of 98.4%. These excellent performances can be attributed to the increased solvent coordination and increased availability of lithium ion concentration in the electrolyte. Further development of this electrolyte may enable practical applications for lithium metal anode in rechargeable batteries.
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When electrolytes containing high concentrations of LiTFSI or LiFSI are used in Li metal anode cells, they can form salt anion-derived SEI with a LiF-rich component that is beneficial for anode protection and electrochemical performance.
“When the electrolytes containing high concentration of these salts are used in Li metal anode cells, they can form salt anion-derived SEI with a LiF-rich component which is beneficial for anode protection and electrochemical performance [104].”
From Review on Low-Temperature Electrolytes for Lithium-Ion and Lithium Metal Batteries (2023) · cites this paper as [104]
The Results section (“Formation of a stable SEI layer”; page not available) reports that a protective SEI forms with 4 M LiFSI-DME and that increasing fluoride content during cycling may result from anion degradation. It does not identify the SEI as LiF-rich or establish the same SEI mechanism for highly concentrated LiTFSI in Li-metal cells; its discussion of concentrated LiTFSI concerns Li|graphite cells. (LLM, conf=0.87)
Experimental — accuracy not yet measuredLithium-metal batteries have a high Coulombic efficiency above 99.1%, withstand more than 6000 charging cycles, and after 1000 cycles maintain an average Coulombic efficiency of 98.4%.
“Lithium-metal batteries have a high Coulombic efficiency (above 99.1%), withstanding more than 6000 charging cycles, and, after 1000 cycles they maintain an average Coulombic efficiency of 98.4% [101].”
From A Review on Electric Vehicles: Technologies and Challenges (2021) · cites this paper as [101]
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Self-citation
- Authors
- Qian, J., Henderson, W. A., Xu, W., Bhattacharya, P., Engelhard, M., Borodin, O., & Zhang, J.-G.
- Affiliations
- Pacific Northwest National Laboratory (US)
- DEVCOM Army Research Laboratory (US)
- Corresponding author
- Zhang, Ji-Guang
- ORCID
- Venue
- Nature Communications
- Published
- 2015-02-20
- Volume
- 6
- Issue
- 1
- Pages
- 6362-6362
- ISSN
- 2041-1723 (ISSN-L)
- PMC
- PMC4346622
- OpenAlex
- W2047775546
- Cited by
- 2,561
- References
- 42
- Citations by year
- 2026: 172 · 2025: 204 · 2024: 240 · 2023: 255 · 2022: 257 · 2021: 287 · 2020: 290 · 2019: 287 · 2018: 257 · 2017: 174 · 2016: 102 · 2015: 35
- FWCI
- 91.30
- Type
- journal article
- Language
- en
- Open access
- gold
- doi.org
- Locations
- Nature Communications (publishedVersion, cc-by)
- Europe PMC (PubMed Central) (publishedVersion, cc-by)
- PubMed Central (publishedVersion, cc-by)
- PubMed (publishedVersion)
- OSTI OAI (U.S. Department of Energy Office of Scientific and Technical Information) (submittedVersion, cc-by)
- RePEc: Research Papers in Economics (submittedVersion)
- Funders
- U.S. Department of Energy (DE-AC05?, DE‐AC05‐76RLO1830)
- Battelle (DE-AC05, DE‐AC05‐76RLO 1830)
- Office of Science (DE-AC05-76RLO 1830)
- Basic Energy Sciences (DE-AC05-76RLO1830)
- Biological and Environmental Research (DE-AC05-76RLO-1830)
- Army Research Laboratory (DE-AC05-76RLO1830)
- Pacific Northwest National Laboratory (DE-AC05-76RLO 1830)
- 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 › Electrical and Electronic Engineering › Advanced battery technologies research
- Keywords
- lithium metal anode, dendrite suppression, high-rate cycling, Coulombic efficiency, concentrated electrolytes, LiFSI, 1,2-dimethoxyethane, ether solvents, solvent coordination, lithium ion concentration, rechargeable batteries
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