Water/Sulfolane Hybrid Electrolyte Achieves Ultralow‐Temperature Operation for High‐Voltage Aqueous Lithium‐Ion Batteries
Abstract
Aqueous batteries are promising candidates for large‐scale energy storage due to their high safety and low cost. However, the narrow electrochemical stability window (ESW, 1.23 V) and high melting point (0 °C) of water limit the energy density and low‐temperature operation of aqueous batteries. In this work, sulfolane is introduced as a co‐solvent to obtain a water/sulfolane hybrid electrolyte, which participates in the solvated sheath of lithium ions, strengthens the OH bond of water, and disrupts the large‐scale hydrogen bond network. Such an elaborate strategy not only expands the ESW of the hybrid electrolyte to 3.8 V, but also lowers the glass‐transition temperature to −110 °C. As proof of concept, the LiMn 2 O 4/Li 4 Ti 5 O 12 full batteries assembled by the hybrid electrolyte display high voltage (2.7 V) and excellent low‐temperature performance of 98% capacity retention from 0 to −20 °C, which can even discharge normally and illume an LED light (rated power of 0.02 W, excitation voltage of 1.8 V) at −65 °C.
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An expanded electrochemical stability window of 3.8 V was achieved due to the formation of a sulfolane-containing solvation sheath and strengthened O-H bond of water, inhibiting water decomposition.
“An expanded electrochemical stability window of 3.8 V has been achieved due to the formation of SL contained solvation sheath and strengthen O-H bond of water, inhibiting the decomposition of water.”
From Review on Low-Temperature Electrolytes for Lithium-Ion and Lithium Metal Batteries (2023) · cites this paper as [86]
The LMO/LTO full cell demonstrated a high operating voltage of 2.7 V and an ultrahigh specific capacity retention ratio up to 98% from 0 to -20 °C.
“As a result, the LMO/LTO full cell demonstrated a high operating voltage of 2.7 V and excellent electrochemical performance with an ultrahigh specific capacity retention ratio up to 98% from 0 to -20 °C.”
From Review on Low-Temperature Electrolytes for Lithium-Ion and Lithium Metal Batteries (2023) · cites this paper as [86]
Liu's group selected sulfolane as cosolvent of antifreeze and water activity inhibitor because of its low toxicity, high miscibility with water, high oxidation stability, and strong interaction with water molecules.
“In another work reported by Liu's group [86], sulfolane (SL) was selected as the cosolvent of antifreeze and the activity inhibitor of water, because of its low toxicity, high miscibility with water, high oxidation stability and strong interaction with water molecules.”
From Review on Low-Temperature Electrolytes for Lithium-Ion and Lithium Metal Batteries (2023) · cites this paper as [86]
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“S1 ), which is consistent with the general expectations for dilute electrolytes [ 23 ].”
- Authors
- Liu, J., Yang, C., Chi, X., Wen, B., Wang, W., & Liu, Y.
- Affiliations
- Chinese Academy of Sciences (CN)
- Corresponding author
- Yang, Cheng
- Liu, Yu
- Venue
- Advanced Functional Materials
- Publisher
- Wiley
- Published
- 2021-10
- Volume
- 32
- Issue
- 1
- ISSN
- 1616-301X (ISSN-L)
- 1616-3028
- OpenAlex
- W3203728506
- Cited by
- 89
- References
- 0
- Citations by year
- 2026: 4 · 2025: 22 · 2024: 26 · 2023: 24 · 2022: 13
- FWCI
- 4.63
- Type
- journal article
- Language
- en
- Open access
- closed
- Locations
- Advanced Functional Materials (publishedVersion)
- Funders
- National Natural Science Foundation of China (51901240)
- Topics
- Physical Sciences › Engineering › Electrical and Electronic Engineering › Advanced battery technologies research
- Physical Sciences › Engineering › Electrical and Electronic Engineering › Advanced Battery Materials and Technologies
- Physical Sciences › Engineering › Electrical and Electronic Engineering › Advancements in Battery Materials
- Keywords
- aqueous lithium-ion batteries, hybrid electrolytes, low-temperature operation, electrochemical stability window, glass transition temperature, hydrogen bond network, LiMn2O4 cathode, Li4Ti5O12 anode, high-voltage batteries
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