Observation of Order and Disorder in Solid-Electrolyte Interphases of Lithium-Metal Anodes

Fuente: arXiv
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Autori principali: Koh, Hyeongjun, Detsi, Eric, Stach, Eric A.
Natura: Preprint
Pubblicazione: 2025
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author Koh, Hyeongjun
Detsi, Eric
Stach, Eric A.
author_facet Koh, Hyeongjun
Detsi, Eric
Stach, Eric A.
contents Battery interfaces critically influence lithium-metal battery performance through their role in ion diffusion and dendrite formation. However, structural characterization of these interfaces has remained challenging due to limitations in high-resolution methods and artifacts from electron irradiation. Using cryogenic conditions for both specimen preparation and scanning electron nanobeam diffraction, we can determine the structural organization at the interface between the vitrified electrolyte and adjacent layers. We identified two distinct interface types: one showing short-range order adjacent to lithium metal, and another displaying a mixed structure of short-range ordering and defective lithium fluoride nanoscale crystallites at a copper collector. Notably, short-range order appeared exclusively in electrolytes demonstrating high reversibility. Our results establish that solid-electrolyte-interphase structure directly influences lithium deposition morphology and battery performance. This methodology opens new possibilities for high-resolution characterization of interfaces in energy storage materials, advancing our understanding of their critical structural properties.
format Preprint
id arxiv_https___arxiv_org_abs_2505_03956
institution arXiv
publishDate 2025
record_format arxiv
spellingShingle Observation of Order and Disorder in Solid-Electrolyte Interphases of Lithium-Metal Anodes
Koh, Hyeongjun
Detsi, Eric
Stach, Eric A.
Materials Science
Atomic Physics
Battery interfaces critically influence lithium-metal battery performance through their role in ion diffusion and dendrite formation. However, structural characterization of these interfaces has remained challenging due to limitations in high-resolution methods and artifacts from electron irradiation. Using cryogenic conditions for both specimen preparation and scanning electron nanobeam diffraction, we can determine the structural organization at the interface between the vitrified electrolyte and adjacent layers. We identified two distinct interface types: one showing short-range order adjacent to lithium metal, and another displaying a mixed structure of short-range ordering and defective lithium fluoride nanoscale crystallites at a copper collector. Notably, short-range order appeared exclusively in electrolytes demonstrating high reversibility. Our results establish that solid-electrolyte-interphase structure directly influences lithium deposition morphology and battery performance. This methodology opens new possibilities for high-resolution characterization of interfaces in energy storage materials, advancing our understanding of their critical structural properties.
title Observation of Order and Disorder in Solid-Electrolyte Interphases of Lithium-Metal Anodes
topic Materials Science
Atomic Physics
url https://arxiv.org/abs/2505.03956