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Lithium Metal Penetration Induced by Electrodeposition through Solid Electrolytes: Example in Single-Crystal Li₆La₃ZrTaO₁₂ Garnet

Swamy, Tushar ; Park, Richard ; Sheldon, Brian W. ; Rettenwander, Daniel ; Porz, Lukas ; Berendts, Stefan ; Uecker, Reinhard ; Carter, W. Craig ; Chiang, Yet-Ming (2023):
Lithium Metal Penetration Induced by Electrodeposition through Solid Electrolytes: Example in Single-Crystal Li₆La₃ZrTaO₁₂ Garnet. (Publisher's Version)
In: Journal of The Electrochemical Society, 165 (16), pp. A3648-A3655. IOP Publishing, ISSN 0013-4651, e-ISSN 1945-7111,
DOI: 10.26083/tuprints-00023229,
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Item Type: Article
Origin: Secondary publication service
Status: Publisher's Version
Title: Lithium Metal Penetration Induced by Electrodeposition through Solid Electrolytes: Example in Single-Crystal Li₆La₃ZrTaO₁₂ Garnet
Language: English
Abstract:

Solid electrolytes potentially enable rechargeable batteries with lithium metal anodes possessing higher energy densities than today's lithium ion batteries. To do so the solid electrolyte must suppress instabilities that lead to poor coulombic efficiency and short circuits. In this work, lithium electrodeposition was performed on single-crystal Li₆La₃ZrTaO₁₂ garnets to investigate factors governing lithium penetration through brittle electrolytes. In single crystals, grain boundaries are excluded as paths for lithium metal propagation. Vickers microindentation was used to introduce surface flaws of known size. However, operando optical microscopy revealed that lithium metal penetration propagates preferentially from a different, second class of flaws. At the perimeter of surface current collectors smaller in size than the lithium source electrode, an enhanced electrodeposition current density causes lithium filled cracks to initiate and grow to penetration, even when large Vickers defects are in proximity. Modeling the electric field distribution in the experimental cell revealed that a 5-fold enhancement in field occurs within 10 micrometers of the electrode edge and generates high local electrochemomechanical stress. This may determine the initiation sites for lithium propagation, overriding the presence of larger defects elsewhere.

Journal or Publication Title: Journal of The Electrochemical Society
Volume of the journal: 165
Issue Number: 16
Place of Publication: Darmstadt
Publisher: IOP Publishing
Classification DDC: 500 Naturwissenschaften und Mathematik > 530 Physik
500 Naturwissenschaften und Mathematik > 540 Chemie
Divisions: 11 Department of Materials and Earth Sciences > Material Science > Nonmetallic-Inorganic Materials
Date Deposited: 21 Feb 2023 10:43
Last Modified: 25 May 2023 06:17
DOI: 10.26083/tuprints-00023229
Corresponding Links:
URN: urn:nbn:de:tuda-tuprints-232297
URI: https://tuprints.ulb.tu-darmstadt.de/id/eprint/23229
PPN: 507934032
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