Initiation of dendritic failure of LLZTO via sub-surface lithium deposition

The occurrence of lithium deposition in occluded spaces within ceramic electrolytes due to electronic leakage currents can jeopardise the commercialization of power-dense solid-state batteries. Here, we utilize plasma-FIB serial sectioning to visualize the surface and sub-surface of a garnet solid e...

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Main Authors: Siniscalchi, M, Shi, Y, Li, G, Gibson, JS, Weatherup, RS, Bonilla, RS, Speller, SC, Grovenor, CRM
Format: Journal article
Language:English
Published: Royal Society of Chemistry 2024
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author Siniscalchi, M
Shi, Y
Li, G
Gibson, JS
Weatherup, RS
Bonilla, RS
Speller, SC
Grovenor, CRM
author_facet Siniscalchi, M
Shi, Y
Li, G
Gibson, JS
Weatherup, RS
Bonilla, RS
Speller, SC
Grovenor, CRM
author_sort Siniscalchi, M
collection OXFORD
description The occurrence of lithium deposition in occluded spaces within ceramic electrolytes due to electronic leakage currents can jeopardise the commercialization of power-dense solid-state batteries. Here, we utilize plasma-FIB serial sectioning to visualize the surface and sub-surface of a garnet solid electrolyte (LLZTO) after lithium plating. We study the morphology of surface spallation cracks, which represent the initial stage of dendrite formation. Employing a LiMg anode, we track the magnesium diffusion around these surface cracks with EDS. The absence of magnesium in early-stage cracks suggests they form due to the pressure build-up from the deposition of pure lithium in occluded pores near the electrolyte surface. These spallation cracks act as current focusing and stress concentration hot spots. Electron beam induced current imaging demonstrates that short-circuiting lithium dendrites grow from the spallations during plating. Thus, the sub-surface deposition of lithium is a possible explanation for the initiation of lithium dendrites in LLZTO.
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spelling oxford-uuid:34ba62d7-80a3-4848-a639-7f970f849eec2024-04-15T16:32:59ZInitiation of dendritic failure of LLZTO via sub-surface lithium depositionJournal articlehttp://purl.org/coar/resource_type/c_dcae04bcuuid:34ba62d7-80a3-4848-a639-7f970f849eecEnglishSymplectic ElementsRoyal Society of Chemistry2024Siniscalchi, MShi, YLi, GGibson, JSWeatherup, RSBonilla, RSSpeller, SCGrovenor, CRMThe occurrence of lithium deposition in occluded spaces within ceramic electrolytes due to electronic leakage currents can jeopardise the commercialization of power-dense solid-state batteries. Here, we utilize plasma-FIB serial sectioning to visualize the surface and sub-surface of a garnet solid electrolyte (LLZTO) after lithium plating. We study the morphology of surface spallation cracks, which represent the initial stage of dendrite formation. Employing a LiMg anode, we track the magnesium diffusion around these surface cracks with EDS. The absence of magnesium in early-stage cracks suggests they form due to the pressure build-up from the deposition of pure lithium in occluded pores near the electrolyte surface. These spallation cracks act as current focusing and stress concentration hot spots. Electron beam induced current imaging demonstrates that short-circuiting lithium dendrites grow from the spallations during plating. Thus, the sub-surface deposition of lithium is a possible explanation for the initiation of lithium dendrites in LLZTO.
spellingShingle Siniscalchi, M
Shi, Y
Li, G
Gibson, JS
Weatherup, RS
Bonilla, RS
Speller, SC
Grovenor, CRM
Initiation of dendritic failure of LLZTO via sub-surface lithium deposition
title Initiation of dendritic failure of LLZTO via sub-surface lithium deposition
title_full Initiation of dendritic failure of LLZTO via sub-surface lithium deposition
title_fullStr Initiation of dendritic failure of LLZTO via sub-surface lithium deposition
title_full_unstemmed Initiation of dendritic failure of LLZTO via sub-surface lithium deposition
title_short Initiation of dendritic failure of LLZTO via sub-surface lithium deposition
title_sort initiation of dendritic failure of llzto via sub surface lithium deposition
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