Lithium Metal Penetration Induced by Electrodeposition through Solid Electrolytes: Example in Single-Crystal Li 6 La 3 ZrTaO 12 Garnet

Swamy, Tushar; Park, Richard; Sheldon, Brian W.; Rettenwander, Daniel; Porz, Lukas; Berendts, Stefan; Uecker, Reinhard; Carter, W. Craig; Chiang, Yet-Ming

doi:10.1149/2.1391814jes

Title: Lithium Metal Penetration Induced by Electrodeposition through Solid Electrolytes: Example in Single-Crystal Li ₆ La ₃ ZrTaO ₁₂ Garnet

Journal Article · Thu Nov 29 00:00:00 EST 2018 · Journal of the Electrochemical Society

DOI:https://doi.org/10.1149/2.1391814jes· OSTI ID:1483923

Swamy, Tushar; Park, Richard;

;

; Porz, Lukas; Berendts, Stefan; Uecker, Reinhard; Carter, W. Craig;

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.

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Research Organization:: Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States); Brown Univ., Providence, RI (United States)

Sponsoring Organization:: USDOE Office of Science (SC)

Grant/Contract Number:: SC0002633; SC0018113

OSTI ID:: 1483923

Alternate ID(s):: OSTI ID: 1610726

Journal Information:: Journal of the Electrochemical Society, Journal Name: Journal of the Electrochemical Society Vol. 165 Journal Issue: 16; ISSN 0013-4651

Publisher:: IOP Publishing - The Electrochemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 150 works

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Title: Lithium Metal Penetration Induced by Electrodeposition through Solid Electrolytes: Example in Single-Crystal Li 6 La 3 ZrTaO 12 Garnet

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Title: Lithium Metal Penetration Induced by Electrodeposition through Solid Electrolytes: Example in Single-Crystal Li ₆ La ₃ ZrTaO ₁₂ Garnet