Probing the heterogeneous nature of LiF in solid–electrolyte interphases

Xiangsi Liu, Shuyang Li, Chen Yuan, Bizhu Zheng, Gangya Cheng, Yufan Chen, Xingyu Lu, Danyu Gu, Baijiang Lv, Hao Li, Zihan Yan, Hui Qian, Yizhou Zhu (), Dalin Sun, Yun Song () and Yuxuan Xiang ()
Additional contact information
Xiangsi Liu: Westlake University
Shuyang Li: Fudan University
Chen Yuan: Westlake University
Bizhu Zheng: Westlake University
Gangya Cheng: Westlake University
Yufan Chen: Fudan University
Xingyu Lu: Westlake University
Danyu Gu: Westlake University
Baijiang Lv: China Academy of Engineering Physics
Hao Li: China Academy of Engineering Physics
Zihan Yan: Westlake University
Hui Qian: Westlake University
Yizhou Zhu: Westlake University
Dalin Sun: Fudan University
Yun Song: Fudan University
Yuxuan Xiang: Westlake University

Nature, 2025, vol. 646, issue 8083, 102-107

Abstract: Abstract The electrolyte–electrode interface serves as the foundation for a myriad of chemical and physical processes. In battery chemistry, the formation of a well-known solid–electrolyte interphase (SEI) plays a pivotal role in ensuring the reversible operations of rechargeable lithium-ion batteries (LIBs)1,2. However, characterizing the precise chemical composition of the low crystallinity and highly sensitive SEI presents a formidable challenge3. Here, taking lithium fluoride (LiF)—a widely studied and considered crucial SEI component4–7—as an example, we use 19F solid-state nuclear magnetic resonance (NMR) and identify that LiF formed in SEI (LiFSEI) has fruitful spectroscopy features that originated from the formation of limited LiF–LiH solid solutions: H-rich phase (LiH1−yFy) and F-rich phase (LiF1−xHx), which is further validated by 6Li isotope NMR, synchrotron X-ray diffraction and cryo-electron microscopy (cryo-EM). By characterizing SEI formed in various electrolytes, we confirm the dominance of LiH1−yFy in high-coulombic-efficiency electrolyte, which can be rationalized by the fact that LiF–LiH solid solution shows improved ionic conductivity over LiF. As a proof of concept, we demonstrate that LiH1−yFy-rich coating layer presents obvious advantages compared with LiF-rich coating layer in lithium-metal batteries. This revised understanding of the heterogeneous nature of SEI components would provide new insights for electrode–electrolyte interface design.

Date: 2025
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DOI: 10.1038/s41586-025-09498-7

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