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Title: Elastic Properties of the Solid Electrolyte Li7La3Zr2O12 (LLZO)

Abstract

The oxide known as LLZO, with nominal composition Li7La3Zr2O12, is a promising solid electrolyte for Li-based batteries due to its high Li-ion conductivity and chemical stability with respect to lithium. Solid electrolytes may also enable the use of metallic Li anodes by serving as a physical barrier that suppresses dendrite initiation and propagation during cycling. Prior linear elasticity models of the Li electrode/solid electrolyte interface suggest that the stability of this interface is highly dependent on the elastic properties of the solid separator. For example, dendritic suppression is predicted to be enhanced as the electrolyte s shear modulus increases. In the present study a combination of first-principles calculations, acoustic impulse excitation measurements, and nanoindentation experiments are used to determine the elastic constants and moduli for highconductivity LLZO compositions based on Al and Ta doping. The calculated and measured isotropic shear moduli are in good agreement and fall within the range of 56-61 GPa. These values are an order of magnitude larger than that for Li metal and far exceed the minimum value ( 8.5 GPa) believed to be necessary to suppress dendrite initiation. These data suggest that LLZO exhibits sufficient stiffness to warrant additional development as a solid electrolyte formore » Li batteries.« less

Authors:
 [1];  [2];  [1];  [3];  [2];  [4];  [1];  [1]
  1. Univ. of Michigan, Ann Arbor, MI (United States)
  2. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
  3. Michigan Technological Univ., Houghton, MI (United States)
  4. Army Research Lab., Adelphi, MD (United States)
Publication Date:
Research Org.:
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Sponsoring Org.:
USDOE Office of Energy Efficiency and Renewable Energy (EERE)
OSTI Identifier:
1261353
Grant/Contract Number:  
AC05-00OR22725
Resource Type:
Accepted Manuscript
Journal Name:
Chemistry of Materials
Additional Journal Information:
Journal Volume: 28; Journal Issue: 1; Journal ID: ISSN 0897-4756
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats

Yu, Seungho, Schmidt, Robert D., Garcia-mendez, Regina, Herbert, Erik G., Dudney, Nancy J., Wolfenstine, Jeff, Sakamoto, Jeff, and Seigel, Donald. Elastic Properties of the Solid Electrolyte Li7La3Zr2O12 (LLZO). United States: N. p., 2015. Web. doi:10.1021/acs.chemmater.5b03854.
Yu, Seungho, Schmidt, Robert D., Garcia-mendez, Regina, Herbert, Erik G., Dudney, Nancy J., Wolfenstine, Jeff, Sakamoto, Jeff, & Seigel, Donald. Elastic Properties of the Solid Electrolyte Li7La3Zr2O12 (LLZO). United States. doi:10.1021/acs.chemmater.5b03854.
Yu, Seungho, Schmidt, Robert D., Garcia-mendez, Regina, Herbert, Erik G., Dudney, Nancy J., Wolfenstine, Jeff, Sakamoto, Jeff, and Seigel, Donald. Wed . "Elastic Properties of the Solid Electrolyte Li7La3Zr2O12 (LLZO)". United States. doi:10.1021/acs.chemmater.5b03854. https://www.osti.gov/servlets/purl/1261353.
@article{osti_1261353,
title = {Elastic Properties of the Solid Electrolyte Li7La3Zr2O12 (LLZO)},
author = {Yu, Seungho and Schmidt, Robert D. and Garcia-mendez, Regina and Herbert, Erik G. and Dudney, Nancy J. and Wolfenstine, Jeff and Sakamoto, Jeff and Seigel, Donald},
abstractNote = {The oxide known as LLZO, with nominal composition Li7La3Zr2O12, is a promising solid electrolyte for Li-based batteries due to its high Li-ion conductivity and chemical stability with respect to lithium. Solid electrolytes may also enable the use of metallic Li anodes by serving as a physical barrier that suppresses dendrite initiation and propagation during cycling. Prior linear elasticity models of the Li electrode/solid electrolyte interface suggest that the stability of this interface is highly dependent on the elastic properties of the solid separator. For example, dendritic suppression is predicted to be enhanced as the electrolyte s shear modulus increases. In the present study a combination of first-principles calculations, acoustic impulse excitation measurements, and nanoindentation experiments are used to determine the elastic constants and moduli for highconductivity LLZO compositions based on Al and Ta doping. The calculated and measured isotropic shear moduli are in good agreement and fall within the range of 56-61 GPa. These values are an order of magnitude larger than that for Li metal and far exceed the minimum value ( 8.5 GPa) believed to be necessary to suppress dendrite initiation. These data suggest that LLZO exhibits sufficient stiffness to warrant additional development as a solid electrolyte for Li batteries.},
doi = {10.1021/acs.chemmater.5b03854},
journal = {Chemistry of Materials},
number = 1,
volume = 28,
place = {United States},
year = {2015},
month = {12}
}

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Works referencing / citing this record:

Free-standing transition metal oxide electrode architectures for electrochemical energy storage
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Free-standing transition metal oxide electrode architectures for electrochemical energy storage
journal, July 2019