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Identification of LiH and nanocrystalline LiF in the solid–electrolyte interphase of lithium metal anodes
Abstract
A comprehensive understanding of the solid-electrolyte interphase (SEI) composition is crucial to developing high-energy batteries based on lithium metal anodes. A particularly contentious issue concerns the presence of LiH in the SEI. Here we report on the use of synchrotron-based X-ray diffraction and pair distribution function analysis to identify and differentiate two elusive components, LiH and LiF, in the SEI of lithium metal anodes. LiH is identified as a component of the SEI in high abundance, and the possibility of its misidentification as LiF in the literature is discussed. LiF in the SEI is found to have different structural features from LiF in the bulk phase, including a larger lattice parameter and a smaller grain size ( + transport and explain why an ionic insulator, like LiF, has been found to be a favoured component for the SEI. Finally, pair distribution function analysis reveals key amorphous components in the SEI.
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“The relative contents of LiH, LiF and dead Li 0 in SEI are quantified, showing higher (LiF) sei and lower dead Li 0 contents in SEIs recovered from the HCE compared with their LCE counterparts.”
From Review on Low-Temperature Electrolytes for Lithium-Ion and Lithium Metal Batteries (2023) · cites this paper as [163]
In the citing paper
“PDF technique differentiated key amorphous components originated from the decomposition of solvents (no good components) or anion (good components), mostly SEI LiF sei .”
From Review on Low-Temperature Electrolytes for Lithium-Ion and Lithium Metal Batteries (2023) · cites this paper as [163]
In the citing paper
“High abundance of LiH was confirmed by XRD.”
From Review on Low-Temperature Electrolytes for Lithium-Ion and Lithium Metal Batteries (2023) · cites this paper as [163]
In the citing paper
“Differing from conventional bulk LiF, they discovered a new type of LiF differing from bulk LiF, and named it as SEI (LiF) sei , which has unique structural features including larger lattice parameter and smaller grain size (< 3 nm), and is favored for Li + transport.”
From Review on Low-Temperature Electrolytes for Lithium-Ion and Lithium Metal Batteries (2023) · cites this paper as [163]
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“Due to the low surface diffusion resistance, LiF is conducive to guiding Li+ deposition rapidly and is an ideal component for the surface coating of lithium [30,31].”
BackgroundTowards interactional management for power batteries of electric vehicles
He, R., Xie, W., Wu, B., Brandon, N. P., Liu, X., Li, X., & Yang, S. (2023) · RSC Advances · doi:10.1039/d2ra06004c · Cited by 18
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Electrochemical Atomic Force Microscopy Study on the Dynamic Evolution of Lithium Deposition
Shi, X., Yang, J., Wang, W.-Y., Liu, Z.-P., & Shen, C. (2023) · Materials · doi:10.3390/ma16062278 · Cited by 8
“Many efforts have been made to investigate this mechanism [30,31], especially in solid electrolytes [32,33].”
BackgroundUnderstanding Solid Electrolyte Interphase Nucleation and Growth on Lithium Metal Surfaces
Angarita-Gomez, S., & Balbuena, P. (2021) · Batteries · doi:10.3390/batteries7040073 · Cited by 8
“Crystalline and amorphous SEI components [52] have been found in different electrolytes studied using pair distribution function (PDF) and X-ray diffraction (XRD) techniques [53] as well as cryoelectron microscopy (cryo-EM) [54] and cryogenic transmission electron microscopy (cryo-TEM) [50], emphasizing the importance…”
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Temperature-Regulated Prelithiated Graphite Anode for an Improved Lithium-Ion Capacitor
Lu, Y., Zheng, J.-S., Lv, X., Shao, J., Jin, L.-M., & Zhang, C.-M. (2024) · ACS Applied Energy Materials · doi:10.1021/acsaem.4c00778 · Cited by 7
Comonomer-Tuned Gel Electrolyte Enables Ultralong Cycle Life of Solid-State Lithium Metal Batteries.
Fu, Y.-L., Chen, Y.-F., & Zhou, L.-M. (2022) · ACS Applied Materials and Interfaces · doi:10.1021/acsami.2c09771 · Cited by 7
Surface coatings to mitigate phase separation in LiFePO4 during lithium-ion battery discharge
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Understanding Lithium Hydride in Lithium Metal Batteries: Advances, Controversies, and Perspectives
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Water as Additive Directing Lithium Electrodeposition
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Mai, Z., Ge, Y., Feng, Y., Luo, K., Zhang, H., Huang, M., Meng, J.-S., & Wang, X.-P. (2026) · Green Chemistry · doi:10.1039/d5gc05012j · Cited by 5
Self-citationWhat role does LiF play In anode-free lithium metal batteries?
Bao, H., Xu, G.-F., Ke, J.-M., Zhao, J., Wang, C.-W., & Liu, F.-R. (2026) · Journal of Materials Chemistry A · doi:10.1039/d5ta10160c · Cited by 5
Self-citationEngineering thin 3D Li-composite foil negative electrodes with high mechanical toughness
Wang, Y.-H., Tan, S., Zhang, C.-H., Guo, J.-C., Luo, X.-X., Jin, R.-X., Huang, L.-B., Su, X.-C., Li, C., Zhang, X.-S., et al. (2026) · Nature Communications · doi:10.1038/s41467-026-69155-z · Cited by 4
Geng, N.-N., Lu, C.-K., Li, W.-B., Liu, Q.-X., Zhou, Z.-X., Yang, T., Cui, Y., Zhang, G.-B., & Lin, X.-D. (2026) · ENERGY & ENVIRONMENTAL MATERIALS · doi:10.1002/eem2.70188 · Cited by 4
Dense Nano-Tips Homogenize Lithium Deposition
Chen, H.-Q., Li, X.-S., Ling, M., Gao, X.-H., Zhao, D., & Chen, Z. (2026) · Advanced Powder Materials · doi:10.1016/j.apmate.2026.100401 · Cited by 4
Metadata
- Authors
- Shadike, Z., Lee, H., Borodin, O., Cao, X., Fan, X., Wang, X., Lin, R., Bak, S.-M., Ghose, S., Xu, K., Wang, C., Liu, J., Xiao, J., Yang, X.-Q., & Hu, E.
- Affiliations
- Brookhaven National Laboratory (US)
- Pacific Northwest National Laboratory (US)
- DEVCOM Army Research Laboratory (US)
- University of Maryland, College Park (US)
- Corresponding author
- Xiao, Jie
- Yang, Xiao-Qing
- Hu, Enyuan
- ORCID
- Venue
- Nature Nanotechnology
- Published
- 2021-01-28
- Volume
- 16
- Issue
- 5
- Pages
- 549-554
- ISSN
- 1748-3387 (ISSN-L)
- 1748-3395
- OpenAlex
- W3124559210
- Cited by
- 320
- References
- 0
- Citations by year
- 2026: 42 · 2025: 54 · 2024: 66 · 2023: 77 · 2022: 55 · 2021: 26
- FWCI
- 16.47
- Type
- journal article
- Language
- en
- Open access
- closed
- Locations
- Nature Nanotechnology (publishedVersion)
- PubMed (publishedVersion)
- OSTI OAI (U.S. Department of Energy Office of Scientific and Technical Information) (submittedVersion)
- Funders
- DOE | Office of Energy Efficiency & Renewable Energy | Vehicle Technologies Office (DE-SC0012704, DE-AC02-05CH11231)
- 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 › Automotive Engineering › Battery Modeling and Management
- Keywords
- solid electrolyte interphase, lithium metal anode, lithium hydride, lithium fluoride, SEI composition, Li+ transport, lattice parameters, grain size, Rietveld refinement, pair distribution function analysis
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