An All-Fluorinated Ester Electrolyte for Stable High-Voltage Li Metal Batteries Capable of Ultra-Low-Temperature Operation
Abstract
Improving the energy output of batteries at sub-zero temperatures is crucial to the long-term application of advanced electronics in extreme environments. This can generally be accomplished by employing high-voltage cathodes, applying Li metal anodes, and improving the electrolyte chemistry to provide facile kinetics at ultralow temperature. However, systems capable of all three of these have seldom been studied. Herein, we demonstrate the design of such a system through solvent fluorination, applying a 1 M LiPF 6 in a methyl 3,3,3-trifluoropionate (MTFP)/fluoroethylene carbonate (FEC) (9:1) electrolyte that simultaneously provided high-voltage cathode and Li metal anode reversibility at room temperature. This performance was attributed to the production of fluorine-rich interphases formed in the MTFP-based system, which was investigated by X-ray photoelectron spectroscopy (XPS). Furthermore, the all-fluorinated electrolyte provided 161, 149, and 133 mAh g –1 when discharged at −40, −50, and −60 °C, respectively, far exceeding the performance of the commercial electrolyte. This work provides new design principles for high-voltage batteries capable of ultra-low-temperature operation.
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Chen et al. used a fluorinated carboxylic ester as cosolvent for a low-temperature electrolyte and obtained both low viscosity and high oxidation stability.
“Chen et al. [68] used a fluorinated carboxylic ester as cosolvent for an LT electrolyte and obtained both low viscosity and high oxidation stability.”
From Review on Low-Temperature Electrolytes for Lithium-Ion and Lithium Metal Batteries (2023) · cites this paper as [68]
Cycling Li||NMC811 between 2.0 and 4.5 V, the electrolyte using MTFP/FEC as solvent retained 150 mAh g-1 after over 250 cycles at room temperature, while the non-fluorinated counterpart retained 110 mAh g-1.
“Cycling Li||NMC811 cell between 2.0 and 4.5 V, the electrolyte using methyl 3,3,3-trifluoropropionate (MTFP)/FEC as the solvent retained 150 mAh g -1 capacity after cycling at RT for over 250 cycles, while the cell using non-fluorinated counterpart only retained 110 mAh g -1 , as shown in Fig. 9c.”
From Review on Low-Temperature Electrolytes for Lithium-Ion and Lithium Metal Batteries (2023) · cites this paper as [68]
Although MTFP slightly increased viscosity, after room-temperature charging, the Li||NMC811 cell using MTFP electrolytes delivered comparable capacity retention (~80%) as MP electrolytes at -40 °C, much higher than that using EC-DEC as solvent (~10%).
“Furthermore, although MTFP slightly increased the viscosity, after RT charging, the Li||NMC811 cell using MTFP electrolytes delivered comparable capacity retention (~ 80%) as MP electrolytes did at -40 °C, which is much higher than that using EC-DEC as solvent (~10 %) (Fig. 9d).”
From Review on Low-Temperature Electrolytes for Lithium-Ion and Lithium Metal Batteries (2023) · cites this paper as [68]
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Tailoring electrolyte solvation for Li metal batteries cycled at ultra-low temperature
Holoubek, J., Liu, H., Wu, Z., Yin, Y., Xing, X., Cai, G., Yu, S., Zhou, H., Pascal, T. A., Chen, Z., et al. (2021) · Nature Energy · doi:10.1038/s41560-021-00783-z · Cited by 851 · see citing works
Self-citationReview on Low-Temperature Electrolytes for Lithium-Ion and Lithium Metal Batteries
Tan, S., Shadike, Z., Cai, X., Lin, R., Kludze, A., Borodin, O., Lucht, B. L., Wang, C., Hu, E., Xu, K., et al. (2023) · Electrochemical Energy Reviews · doi:10.1007/s41918-023-00199-1 · Cited by 118 · see citing works
- Authors
- Holoubek, J., Yu, M., Yu, S., Li, M., Wu, Z., Xia, D., Bhaladhare, P., Gonzalez, M. S., Pascal, T. A., Liu, P., & Chen, Z.
- Affiliations
- University of California San Diego (US)
- Corresponding author
- Chen, Zheng
- ORCID
- Venue
- ACS Energy Letters
- Publisher
- American Chemical Society (ACS)
- Published
- 2020-04-09
- Volume
- 5
- Issue
- 5
- Pages
- 1438-1447
- ISSN
- 2380-8195 (ISSN-L)
- OpenAlex
- W3015446784
- Cited by
- 351
- References
- 5
- Citations by year
- 2026: 35 · 2025: 53 · 2024: 58 · 2023: 76 · 2022: 66 · 2021: 45 · 2020: 18
- FWCI
- 17.59
- Type
- journal article
- Language
- en
- Open access
- closed
- Licence
- Locations
- ACS Energy Letters (publishedVersion)
- Funders
- Jacobs School of Engineering, University of California, San Diego
- National Aeronautics and Space Administration (ECF 80NSSC18K1512)
- National Science Foundation (ECCS-1542148)
- 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
- fluorinated electrolytes, lithium metal batteries, high-voltage cathodes, fluoroethylene carbonate, LiPF6, lithium metal anode, high-voltage lithium-ion batteries
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