Improving Electrochemical Stability and Low‐Temperature Performance with Water/Acetonitrile Hybrid Electrolytes
Abstract
Although the “water‐in‐salt” electrolyte has significantly expanded the electrochemical stability window of aqueous electrolytes from 1.23 to 3 V, its inevitable hydrogen evolution under 1.9 V versus Li+/Li prevents the practical use of many energy‐dense anodes. Meanwhile, its liquidus temperature at 17 °C restricts its application below ambient temperatures. An advanced hybrid electrolyte is proposed in this work by introducing acetonitrile (AN) as co‐solvent, which minimizes the presence of interfacial water at the negatively charged electrode surface, and generates a thin and uniform interphase consisting of an organic outer layer based on nitrile (CN) and sulfamide (R‐S‐N‐S) species and an inner layer rich in LiF. Such an interphase significantly suppresses water reduction and expands the electrochemical stability window to an unprecedented width of 4.5 V. Thanks to the low freezing point (−48 °C) and low viscosity of AN, the hybrid electrolyte is highly conductive in a wide temperature range, and enables a LiMn 2 O 4/Li 4 Ti 5 O 12 full cell at both ambient and sub‐ambient temperatures with excellent cycling stability and rate capability. Meanwhile, such a hybrid electrolyte also inherits the nonflammable nature of aqueous electrolyte. The well‐balanced merits of the developed electrolyte make it suitable for high energy density aqueous batteries.
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Xu's group increased the salt concentration of LiTFSI to 15.3 M in AN-WiSE, minimizing interfacial water at the negatively charged electrode surface, resulting in a uniform and thin interphase with an organic outer layer and a LiF-rich inner layer.
“Xu's group [84] increased the salt concentration of LiTFSI to 15.3 M in AN-WiSE, where the presence of interfacial water at the negatively charged electrode surface has been minimized, resulting in uniform and thin interphase consisting of an organic outer layer based on nitrile and sulfamide species and an inner layer rich in LiF.”
From Review on Low-Temperature Electrolytes for Lithium-Ion and Lithium Metal Batteries (2023) · cites this paper as [84]
The stable electrochemical window was expanded to 4.5 V, enabling a LiMn2O4/Li4Ti5O12 full cell with excellent cycling stability and rate capability at both ambient and sub-ambient temperatures.
“More importantly, the stable electrochemical window has been expended to 4.5 V, enabling a LiMn 2 O 4 / Li 4 Ti 5 O 12 full cell with excellent cycling stability and rate capability at both ambient and sub-ambient temperatures.”
From Review on Low-Temperature Electrolytes for Lithium-Ion and Lithium Metal Batteries (2023) · cites this paper as [84]
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“31,32 When ACN is used in organic-aqueous hybrid electrolytes, it is often in highly concentrated or saturated electro-lytes 30,33,34 ; however, it has also been used in aqueous zinc-ion batteries at dilute salt concentrations.”
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- Authors
- Chen, J., Vatamanu, J., Xing, L., Borodin, O., Chen, H., Guan, X., Liu, X., Xu, K., & Li, W.
- Affiliations
- South China Normal University (CN)
- DEVCOM Army Research Laboratory (US)
- Corresponding author
- Xing, Lidan
- Xu, Kang
- Venue
- Advanced Energy Materials
- Publisher
- Wiley
- Published
- 2019-11-22
- Volume
- 10
- Issue
- 3
- ISSN
- 1614-6832 (ISSN-L)
- 1614-6840
- OpenAlex
- W2990932651
- Cited by
- 260
- References
- 0
- Citations by year
- 2026: 14 · 2025: 40 · 2024: 41 · 2023: 39 · 2022: 53 · 2021: 47 · 2020: 26
- FWCI
- 11.31
- Type
- journal article
- Language
- en
- Open access
- closed
- Locations
- Advanced Energy Materials (publishedVersion)
- Funders
- National Natural Science Foundation of China (21573080)
- Science and Technology Planning Project of Guangdong Province (2017B090901020)
- 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
- water-in-salt electrolytes, hybrid electrolytes, electrochemical stability window, hydrogen evolution suppression, lithium metal anode, low-temperature performance, solid electrolyte interphase, LiF, sulfamides, nitriles, freezing point, LiMn2O4 cathode, Li4Ti5O12 cathode, non-flammable electrolytes
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