Use of Organic Esters as Cosolvents in Electrolytes for Lithium-Ion Batteries with Improved Low Temperature Performance
Open accessAbstract
The electrolyte composition plays a strong role in determining the low temperature performance of lithium-ion cells, both in terms of ionic mobility in the electrolyte solution, as well as forming suitable surface films on the electrode surfaces. A series of ester solvents was chosen for incorporation into multicomponent electrolyte formulations due to their favorable physiochemical properties ( i.e. , low viscosity, low melting point, and high permittivity), as well as good compatibility with carbonaceous anodes and mixed metal cathodes ( i.e. , and In addition to determining the relative facility of lithium intercalation and deintercalation in Li-carbon cells as a function of temperature, a number of conventional electrochemical methods were employed to further enhance the understanding of the nature of the electrode surface films in these ester-based electrolytes, including dc polarization and ac impedance measurements. A distinct trend was observed with respect to the stability of the surface films formed. In solutions containing low molecular weight cosolvents ( i.e. , methyl acetate and ethyl acetate) the surface films appear resistive and inadequately protective, whereas electrolytes containing higher molecular weight esters resulted in surface films with more desirable attributes. Promising electrolyte formulations were further evaluated in prototype lithium-ion cells (AA-size) and fully characterized in terms of their low temperature discharge performance. © 2002 The Electrochemical Society. All rights reserved.
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A methyl propionate-based electrolyte showed the best performance and delivered the highest capacity at -40 °C.
“As shown in Fig. 5a, the MP-based electrolyte showed the best performance and delivered the highest capacity at LT (-40 °C).”
From Review on Low-Temperature Electrolytes for Lithium-Ion and Lithium Metal Batteries (2023) · cites this paper as [40]
The Prototype Cell Performance section reports that ester-containing electrolytes outperformed an all-carbonate electrolyte at −40 °C. But the paper’s studied esters are methyl acetate, ethyl acetate, ethyl propionate, and ethyl butyrate—not methyl propionate—and it does not establish that a methyl propionate electrolyte delivered the highest capacity. Page numbers are unavailable in our copy. (LLM, conf=0.88)
Experimental — accuracy not yet measuredEsters with shorter alkyl chains have the advantage of better ionic conductivity for the bulk electrolyte but the disadvantage of forming more resistive and less protective solid electrolyte interphases compared with longer-chain counterparts.
“It was concluded that esters with shorter alkyl chains have the advantage in getting better ionic conductivity for the bulk electrolyte, but the disadvantage in forming more resistive and less protective SEIs as compared to longer chain counterparts.”
From Review on Low-Temperature Electrolytes for Lithium-Ion and Lithium Metal Batteries (2023) · cites this paper as [40]
Rapid capacity decay at -20 °C occurred when using electrolytes with methyl acetate and ethyl acetate esters, although higher initial capacity was delivered.
“Figure 5b shows the rapid capacity decay at -20 °C when using electrolytes with MA and EA esters (2 and 3), although higher initial capacity was delivered.”
From Review on Low-Temperature Electrolytes for Lithium-Ion and Lithium Metal Batteries (2023) · cites this paper as [40]
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Logan, E., Hebecker, H., Eldesoky, A., Luscombe, A., Johnson, M. B., & Dahn, J. (2020) · Journal of The Electrochemical Society · doi:10.1149/1945-7111/abbbbe · Cited by 53 · see citing works
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Thermal Characteristics and Safety Aspects of Lithium-Ion Batteries: An In-Depth Review
Madani, S., Ziebert, C., & Marzband, M. (2023) · Symmetry · doi:10.3390/sym15101925 · Cited by 50 · see citing works
“…characterization [41] Lithium-ion batteries Sony (US18650) cell Analysis of electrochemical and thermal Behavior [42] Lithium/polymer-electrolyte Heat transfer phenomena [43] Lithium-ion batteries Thermal modeling and design considerations [44] Lithium polymer lithium/polymer-electrolyte batteries”
BackgroundCarbon-nanofiber composite electrodes for thin and flexible lithium-ion batteries
Wu, M.-S., Lee, J.-T., Chiang, P.-C. J., & Lin, J.-C. (2007) · doi:10.1007/s10853-006-1062-z · Cited by 49
Methyl Acetate as a Co-Solvent in NMC532/Graphite Cells
Li, J., Li, H., Ma, X.-W., Stone, W., Glazier, S. L., Logan, E., Tonita, E., Gering, K., & Dahn, J. (2018) · doi:10.1149/2.0861805jes · Cited by 49
A Study of Three Ester Co-Solvents in Lithium-Ion Cells
Ma, X.-W., Arumugam, R., Ma, L., Logan, E., Tonita, E., Xia, J., Petibon, R., Kohn, S., & Dahn, J. (2017) · doi:10.1149/2.0411714jes · Cited by 48
Novel Low-Temperature Electrolyte Using Isoxazole as the Main Solvent for Lithium-Ion Batteries.
Tan, S., Rodrigo, U. N., Shadike, Z., Lucht, B., Xu, K., Wang, C.-S., Yang, X.-Q., & Hu, E. (2021) · ACS Applied Materials and Interfaces · doi:10.1021/acsami.1c05894 · Cited by 47 · see citing works
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Jurng, S., Park, S., Yoon, T., Kim, H.-S., Jeong, H., Ryu, J. H., Kim, J. J., & Oh, S. M. (2016) · Journal of The Electrochemical Society · doi:10.1149/2.0051609jes · Cited by 44 · see citing works
A Critical Evaluation of the Advanced Electrolyte Model
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Effect of anode binders on low-temperature performance of automotive lithium-ion batteries
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Yin, Y., & Dong, X.-L. (2023) · Interdisciplinary Materials · doi:10.1002/idm2.12105 · Cited by 39 · see citing works
“Smart et al.([50]) have investigated the effects of various linear carboxylate esters and compared the electrochemical performance of graphite‐based LIBs at low temperature, which shows that electrolyte modification with appropriate carboxylate solvents would be viable to improve the ionic conductivity at low temperat…”
BackgroundLow temperature electrochemical performance of β-LixV2O5 cathode for lithium-ion batteries
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Electrolyte Development for Enhancing Sub‐Zero Temperature Performance of Secondary Batteries
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Structural Interactions within Lithium Salt Solvates: Cyclic Carbonates and Esters
Seo, D. M., Afroz, T., Allen, J. L., Boyle, P., Trulove, P., Long, H. C. D., & Henderson, W. (2014) · doi:10.1021/jp5079168 · Cited by 35
Behavior of Li-Ion Cells in High-Intensity Radiation Environments
Ratnakumar, B., Smart, M., Whitcanack, L., Davies, E., Chin, K., Deligiannis, F., & Surampudi, S. (2004) · Journal of The Electrochemical Society · doi:10.1149/1.1666128 · Cited by 35 · see citing works
Self-citation
- Authors
- Smart, M. C., Ratnakumar, B. V., & Surampudi, S.
- Affiliations
- California Institute of Technology (US)
- ORCID
- Smart, M. C.
- Venue
- Journal of The Electrochemical Society
- Publisher
- The Electrochemical Society
- Published
- 2002
- Volume
- 149
- Issue
- 4
- Pages
- A361
- ISSN
- 0013-4651 (ISSN-L)
- OpenAlex
- W2028749795
- Cited by
- 234
- References
- 18
- Citations by year
- 2026: 5 · 2025: 18 · 2024: 23 · 2023: 24 · 2022: 24 · 2021: 17 · 2020: 14 · 2019: 8 · 2018: 11 · 2017: 7 · 2016: 5 · 2015: 9 · 2014: 5 · 2013: 7 · 2012: 5
- FWCI
- 8.05
- Type
- journal article
- Language
- en
- Open access
- bronze
- doi.org
- Locations
- Journal of The Electrochemical Society (publishedVersion)
- Funders
- National Aeronautics and Space Administration
- California Institute of Technology
- Defense Advanced Research Projects Agency
- Jet Propulsion Laboratory
- Topics
- Physical Sciences › Engineering › Electrical and Electronic Engineering › Advancements in Battery Materials
- Physical Sciences › Engineering › Automotive Engineering › Advanced Battery Technologies Research
- Physical Sciences › Engineering › Electrical and Electronic Engineering › Advanced Battery Materials and Technologies
- Keywords
- lithium-ion batteries, low-temperature performance, electrolyte formulation, surface films, lithium intercalation, methyl acetate, ethyl acetate, ionic conductivity, electrode-electrolyte interface, low-temperature discharge
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