Lithium Metal Penetration Induced by Electrodeposition through Solid Electrolytes: Example in Single-Crystal Li 6 La 3 ZrTaO 12 Garnet
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.
- Publication Date:
- Research Org.:
- Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States); Brown Univ., Providence, RI (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC)
- OSTI Identifier:
- 1483923
- Alternate Identifier(s):
- OSTI ID: 1610726
- Grant/Contract Number:
- SC0002633; SC0018113
- Resource Type:
- Published Article
- Journal Name:
- Journal of the Electrochemical Society
- Additional Journal Information:
- Journal Name: Journal of the Electrochemical Society Journal Volume: 165 Journal Issue: 16; Journal ID: ISSN 0013-4651
- Publisher:
- IOP Publishing - The Electrochemical Society
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 36 MATERIALS SCIENCE; Electrochemistry; Materials Science
Citation Formats
Swamy, Tushar, Park, Richard, Sheldon, Brian W., Rettenwander, Daniel, Porz, Lukas, Berendts, Stefan, Uecker, Reinhard, Carter, W. Craig, and Chiang, Yet-Ming. Lithium Metal Penetration Induced by Electrodeposition through Solid Electrolytes: Example in Single-Crystal Li 6 La 3 ZrTaO 12 Garnet. United States: N. p., 2018.
Web. doi:10.1149/2.1391814jes.
Swamy, Tushar, Park, Richard, Sheldon, Brian W., Rettenwander, Daniel, Porz, Lukas, Berendts, Stefan, Uecker, Reinhard, Carter, W. Craig, & Chiang, Yet-Ming. Lithium Metal Penetration Induced by Electrodeposition through Solid Electrolytes: Example in Single-Crystal Li 6 La 3 ZrTaO 12 Garnet. United States. https://doi.org/10.1149/2.1391814jes
Swamy, Tushar, Park, Richard, Sheldon, Brian W., Rettenwander, Daniel, Porz, Lukas, Berendts, Stefan, Uecker, Reinhard, Carter, W. Craig, and Chiang, Yet-Ming. Thu .
"Lithium Metal Penetration Induced by Electrodeposition through Solid Electrolytes: Example in Single-Crystal Li 6 La 3 ZrTaO 12 Garnet". United States. https://doi.org/10.1149/2.1391814jes.
@article{osti_1483923,
title = {Lithium Metal Penetration Induced by Electrodeposition through Solid Electrolytes: Example in Single-Crystal Li 6 La 3 ZrTaO 12 Garnet},
author = {Swamy, Tushar and Park, Richard and Sheldon, Brian W. and Rettenwander, Daniel and Porz, Lukas and Berendts, Stefan and Uecker, Reinhard and Carter, W. Craig and Chiang, Yet-Ming},
abstractNote = {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.},
doi = {10.1149/2.1391814jes},
journal = {Journal of the Electrochemical Society},
number = 16,
volume = 165,
place = {United States},
year = {Thu Nov 29 00:00:00 EST 2018},
month = {Thu Nov 29 00:00:00 EST 2018}
}
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