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Tailoring electrolyte solvation for Li metal batteries cycled at ultra-low temperature
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Lithium metal batteries (LMBs) hold the promise to pushing cell level energy densities beyond 300 Wh kg-1 while operating at ultra-low temperatures (< -30°C). Batteries capable of both charging and discharging at these temperature extremes are highly desirable due to their inherent reduction of external warming requirements. Here we demonstrate that the local solvation structure of the electrolyte defines the charge-transfer behavior at ultra-low temperature, which is crucial for achieving high Li metal coulombic efficiency (CE) and avoiding dendritic growth. These insights were applied to Li metal full cells, where a high-loading 3.5 mAh cm-2 sulfurized polyacrylonitrile (SPAN) cathode was paired with a one-fold excess Li metal anode. The cell retained 84 % and 76 % of its room temperature capacity when cycled at -40 and -60 °C, respectively, which presented stable performance over 50 cycles. This work provides design criteria for ultra-low temperature LMB electrolytes, and represents a defining step for the performance of low-temperature batteries.
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“In contrast, the Li/SPAN cell using 1 M LiFSI in DOL/DME failed immediately at -60 °C.”
From Review on Low-Temperature Electrolytes for Lithium-Ion and Lithium Metal Batteries (2023) · cites this paper as [57]
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“The low binding energy of Li + (DEE) 1.8 provided a much favorable desolvation energy barrier to be overcome and resulted in excellent CE (98.4%) of Li/Cu cells at ultra-LTs (-60 °C), as shown in Fig. 8b.”
From Review on Low-Temperature Electrolytes for Lithium-Ion and Lithium Metal Batteries (2023) · cites this paper as [57]
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“Different from typical solvent-separated ion pair (SSIP) solvation structure, DEE electrolytes presented characteristic CIPs with 1.8 DEE oxygens and 2.0 FSI -oxygens per Li + .”
From Review on Low-Temperature Electrolytes for Lithium-Ion and Lithium Metal Batteries (2023) · cites this paper as [57]
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“Meanwhile, the Li + (DEE) 1.8 complexes possessed a much lower binding energy of -280 kJ mol -1 than that of Li + (DME) 2.3 (-414 kJ mol -1 ) formed in 1 M LiFSI in DOL-DME electrolytes shown in Fig. 8a.”
From Review on Low-Temperature Electrolytes for Lithium-Ion and Lithium Metal Batteries (2023) · cites this paper as [57]
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Self-citation
Metadata
- Authors
- Holoubek, J., Liu, H., Wu, Z., Yin, Y., Xing, X., Cai, G., Yu, S., Zhou, H., Pascal, T. A., Chen, Z., & Liu, P.
- Affiliations
- University of California San Diego (US)
- Corresponding author
- Pascal, Tod A.
- Chen, Zheng
- Liu, Ping
- ORCID
- Venue
- Nature Energy
- Published
- 2021-02-25
- Volume
- 6
- Issue
- 3
- Pages
- 303-313
- ISSN
- 2058-7546 (ISSN-L)
- PMC
- PMC7954221
- OpenAlex
- W3134786422
- Cited by
- 851
- References
- 53
- Citations by year
- 2026: 98 · 2025: 210 · 2024: 184 · 2023: 176 · 2022: 140 · 2021: 43
- FWCI
- 39.93
- Type
- journal article
- Language
- en
- Open access
- green
- www.ncbi.nlm.nih.gov
- Licence
- Locations
- Nature Energy (publishedVersion)
- PubMed (publishedVersion)
- PubMed Central (acceptedVersion)
- eScholarship (California Digital Library) (submittedVersion)
- RePEc: Research Papers in Economics (submittedVersion)
- Funders
- National Aeronautics and Space Administration (ECF 80NSSC18K1512)
- U.S. Department of Energy (DE-EE0007764)
- 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 › Aqueous and Flow Batteries
- Keywords
- lithium metal batteries, electrolyte solvation structure, Coulombic efficiency, lithium dendrite suppression, lithium metal anode, low-temperature battery performance
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