Lithium Metal Penetration Induced by Electrodeposition through Solid Electrolytes: Example in Single-Crystal Li[subscript 6]La[subscript 3]ZrTaO[subscript 12] Garnet
Name
J. Electrochem. Soc.-2018-Swamy-A3648-55.pdf
Description
Published version
Size
1022.85 KB
Format
Adobe PDF
Checksum (MD5)
a7ef7d93f5f0d3cdd52a479a3b99faf0
Author(s)
Swamy, Tushar
Park, Richard J.-Y.
Sheldon, Brian W.
Rettenwander, Daniel
Porz, Lukas
Berendts, Stefan
Uecker, Reinhard
Carter, W Craig
Chiang, Yet-Ming
Date Issued
November 2018
Journal
Journal of The Electrochemical Society
Publisher
The Electrochemical Society
Citation
Swamy, Tushar et al., "Lithium Metal Penetration Induced by Electrodeposition through Solid Electrolytes: Example in Single-Crystal Li[subscript 6]La[subscript 3]ZrTaO[subscript 12] Garnet." Journal of The Electrochemical Society 165, 16 (November 2018): A3648-A3655 ©2018 Authors
Version
Final published version
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 Li[subscript 6]La[subscript 3]ZrTaO[subscript 12] 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.
MIT Department
Massachusetts Institute of Technology. Department of Mechanical Engineering
Massachusetts Institute of Technology. Department of Materials Science and Engineering
Terms of Use
Creative Commons Attribution 4.0 International license
Persistent DSpace Link
DOI of Published Version
https://doi.org/10.1149/2.1391814JES
