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Designing electrolytes and interphases for high-energy lithium batteries

Nature Reviews Chemistry volume 8, pages 30–44 (2024)Cite this article

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Abstract

High-energy and stable lithium-ion batteries are desired for next-generation electric devices and vehicles. To achieve their development, the formation of stable interfaces on high-capacity anodes and high-voltage cathodes is crucial. However, such interphases in certain commercialized Li-ion batteries are not stable. Due to internal stresses during operation, cracks are formed in the interphase and electrodes; the presence of such cracks allows for the formation of Li dendrites and new interphases, resulting in a decay of the energy capacity. In this Review, we highlight electrolyte design strategies to form LiF-rich interphases in different battery systems. In aqueous electrolytes, the hydrophobic LiF can extend the electrochemical stability window of aqueous electrolytes. In organic liquid electrolytes, the highly lithiophobic LiF can suppress Li dendrite formation and growth. Electrolyte design aimed at forming LiF-rich interphases has substantially advanced high-energy aqueous and non-aqueous Li-ion batteries. The electrolyte and interphase design principles discussed here are also applicable to solid-state batteries, as a strategy to achieve long cycle life under low stack pressure, as well as to construct other metal batteries.

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Fig. 1: Key scientific challenges when designing electrolytes.
Fig. 2: Illustration of the universal electrolyte design principles.
Fig. 3: Design strategies for the LiF-rich solid electrolyte interphase (SEI).
Fig. 4: Li dendrite growth in an all-solid-state battery.
Fig. 5: Cell failure (lithium dendrite growth and/or crack formation) mechanism and strategies to prevent dendrite growth and crack formation.
Fig. 6: Interface design for lithium dendrite suppression.

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Acknowledgements

The authors acknowledge funding from the US Department of Energy (DOE) under Award number DEEE0008856, ARPA-E under Award of DE-AR0000781, Advanced Battery Materials Research (BMR) Program (Battery500 Consortium Phase 2) under DOE contract no. DE-AC05-76RL01830 from the Pacific Northwest National Laboratory (PNNL) and the US Department of Energy (DOE) through ARPA-E grant DEAR0000389.

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  1. Department of Chemical and Biomolecular Engineering, University of Maryland, College Park, MD, USA

    Hongli Wan, Jijian Xu & Chunsheng Wang

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H. W., J. X. and C. W. conceived the idea and wrote the draft. All the authors edited and revised the manuscript.

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Wan, H., Xu, J. & Wang, C. Designing electrolytes and interphases for high-energy lithium batteries. Nat Rev Chem 8, 30–44 (2024). https://doi.org/10.1038/s41570-023-00557-z

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