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Title: Lithium metal penetration induced by electrodeposition through solid electrolytes: Example in single-crystal Li6La3ZrTaO12 garnet
Authors: Swamy, TusharPark, RichardSheldon, Brian W.Rettenwander, DanielPorz, LukasBerendts, StefanUecker, ReinhardCarter, W. CraigChiang, Yet-Ming
Publishers version: https://doi.org/10.1149/2.1391814jes
URI: https://oa.tib.eu/renate/handle/123456789/11680
http://dx.doi.org/10.34657/10713
Issue Date: 2018
Published in: Journal of The Electrochemical Society 165 (2018), Nr. 16
Journal: Journal of The Electrochemical Society
Volume: 165
Issue: 16
Page Start: A3648
Page End: A3655
Publisher: Pennington, NJ : Electrochemical Society
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.
Keywords: Coulombic efficiency; Electric field distributions; Electrochemomechanical; Electrodeposition current densities; Higher energy density; Initiation sites; Lithium metal anode; Vickers microindentation
Type: article; Text
Publishing status: publishedVersion
DDC: 540
620
660
License: CC BY 4.0 Unported
Link to license: https://creativecommons.org/licenses/by/4.0/
Appears in Collections:Chemie
Ingenieurwissenschaften

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Swamy, Tushar, Richard Park, Brian W. Sheldon, Daniel Rettenwander, Lukas Porz, Stefan Berendts, Reinhard Uecker, W. Craig Carter and Yet-Ming Chiang, 2018. Lithium metal penetration induced by electrodeposition through solid electrolytes: Example in single-crystal Li6La3ZrTaO12 garnet. 2018. Pennington, NJ : Electrochemical Society
Swamy, T., Park, R., Sheldon, B. W., Rettenwander, D., Porz, L., Berendts, S., Uecker, R., Carter, W. C. and Chiang, Y.-M. (2018) “Lithium metal penetration induced by electrodeposition through solid electrolytes: Example in single-crystal Li6La3ZrTaO12 garnet.” Pennington, NJ : Electrochemical Society. doi: https://doi.org/10.1149/2.1391814jes.
Swamy T, Park R, Sheldon B W, Rettenwander D, Porz L, Berendts S, Uecker R, Carter W C, Chiang Y-M. Lithium metal penetration induced by electrodeposition through solid electrolytes: Example in single-crystal Li6La3ZrTaO12 garnet. Vol. 165. Pennington, NJ : Electrochemical Society; 2018.
Swamy, T., Park, R., Sheldon, B. W., Rettenwander, D., Porz, L., Berendts, S., Uecker, R., Carter, W. C., & Chiang, Y.-M. (2018). Lithium metal penetration induced by electrodeposition through solid electrolytes: Example in single-crystal Li6La3ZrTaO12 garnet (Version publishedVersion, Vol. 165). Version publishedVersion, Vol. 165. Pennington, NJ : Electrochemical Society. https://doi.org/https://doi.org/10.1149/2.1391814jes
Swamy T, Park R, Sheldon B W, Rettenwander D, Porz L, Berendts S, Uecker R, Carter W C, Chiang Y-M. Lithium metal penetration induced by electrodeposition through solid electrolytes: Example in single-crystal Li6La3ZrTaO12 garnet. 2018;165(16). doi:https://doi.org/10.1149/2.1391814jes


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