Electrolyte design implications of ion-pairing in low-temperature Li metal batteries
Abstract
The reversibility of Li metal batteries suffers beneath 0 °C due to a heightened charge-transfer barrier. Herein, the introduction of ion-pairs within the electrolyte is shown to improve this behavior, enabling hundreds of cycles down to −40 °C.
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DME-based LHCE systems with bis(2,2,2-trifluoroethyl) ether as diluent allow modulation of the degree of ion-pairing while maintaining relatively low bulk viscosity.
“bis(2,2,2-trifluoroethyl) ether (BTFE) as the diluent, which allows for the modulation of the degree of ion-pairing while maintaining a relatively low bulk viscosity [58].”
From Review on Low-Temperature Electrolytes for Lithium-Ion and Lithium Metal Batteries (2023) · cites this paper as [58]
Both experimental and theoretical results demonstrated a distinct ion-pairing transition when the local concentration exceeds 4 M (3:1 BTFE/DME ratio), resulting in stable cycling of LMA and NMC811 cathodes even at low temperatures.
“Both experimental and theoretical results demonstrated that there is a distinct ion-pairing transition when the local concentration exceeds 4 M (3:1 BTFE/DME ratio), which resulted in stable cycling of LMA and NMC811 cathodes even at LTs.”
From Review on Low-Temperature Electrolytes for Lithium-Ion and Lithium Metal Batteries (2023) · cites this paper as [58]
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Co‐Solvation Tunes Ion Pairing and Interphases to Stabilize High‐Voltage Sodium Metal Batteries
Khan, M. S., Rahman, M. A., Shahali, H., Wang, G., Weston, J. S., Ramsurn, H., Asadi, A., Hussaini, S. R., & Amiri, A. (2026) · Advanced Functional Materials · doi:10.1002/adfm.77962 · Cited by 1
“Therefore, the mixed-solvent formulation provides a favorable trade-off by suppressing extreme aggregation while enabling controlled ion association, a balance that has been associated with improved low-temperature electrolyte performance [ 44 ].”
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“With the highest theoretical specific capacity (3860 mAh g − 1 ) and lowest redox potential ( − 3.04 V vs. the standard hydrogen electrode) [3], lithium (Li) metal has emerged as a promising anodic material by providing a potential pathway in elevating the energy density [4, 5].”
InfluentialZhao, D.-N., Luo, J., Su, Z.-X., Dou, H.-Z., He, J., Zhang, J.-W., Zhao, Y.-J., Xu, X.-F., Wang, P., Zhang, N.-S., et al. (2026) · Chemical Engineering Journal · doi:10.1016/j.cej.2026.179880 · Cited by 1
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“By reducing the binding energy between Li + and solvent molecules, this strategy promotes the entry of anions into the primary solvation sheath, thereby lowering the desolvation energy barrier and inducing the formation of an inorganic-rich SEI [34–36].”
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Self-citationA review of low-temperature lithium metal battery research
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“[8] Zou et al record that a novel electrolyte, which be easily removed from the solvent and is favorable for interfacial movie formation, has been designed for lithium metallic batteries at low temperatures.”
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Landscaping dual-ion batteries architected by MXene materials
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“As displayed in Figure 5b , the GPE-based Na|NVP cell maintained stable operation over 300 cycles at 1 C and − 20 ◦ C, which is highly competitive compared with previously reported GPE-based SMBs under similar conditions [ 13, 50, 51 ].”
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Self-citationAnode‐Free Alkali Metal Batteries Under Extreme Temperatures
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Carbon Anodes for Low‐Temperature Nonaqueous Alkali Metal‐Ion Batteries
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“For instance, designing the localized high-concentration electrolytes [11] is one of the most effective strategies.”
Strongly coordinating anions and cosolvent synergy enabled lithium metal batteries
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Rational Electrolyte Formulation for Sodium Metal Batteries Operating in Extremely Cold Environments
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- Authors
- Holoubek, J., Kim, K., Yin, Y., Wu, Z., Liu, H., Li, M., Chen, A., Gao, H., Cai, G., Pascal, T. A., Liu, P., & Chen, Z.
- Affiliations
- University of California San Diego (US)
- Corresponding author
- Pascal, Tod A.
- Liu, Ping
- Chen, Zheng
- ORCID
- Venue
- Energy & Environmental Science
- Publisher
- Royal Society of Chemistry (RSC)
- Published
- 2022
- Volume
- 15
- Issue
- 4
- Pages
- 1647-1658
- ISSN
- 1754-5692 (ISSN-L)
- 1754-5706
- OpenAlex
- W4225918206
- Cited by
- 241
- References
- 0
- Citations by year
- 2026: 32 · 2025: 69 · 2024: 64 · 2023: 51 · 2022: 25
- FWCI
- 14.31
- Type
- journal article
- Language
- en
- Open access
- closed
- Locations
- Energy & Environmental Science (publishedVersion)
- Funders
- National Science Foundation (DMR-2011924, ECCS-1542, ACI-1548562148)
- National Aeronautics and Space Administration (ECF 80NSSC18K1512, 80NSSC20K1174)
- 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 batteries, low-temperature batteries, ion pairing, electrolyte design, charge transfer barrier, cycling reversibility, lithium metal anode
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