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Title: Atomic Layer Deposition of the Solid Electrolyte Garnet Li 7 La 3 Zr 2 O 12

Abstract

Lithium solid electrolytes are a promising platform for achieving high energy density, long-lasting, and safe rechargeable batteries, which could have widespread societal impact. In particular, the ceramic oxide garnet Li7La3Zr2O12 (LLZO) has been shown to be a promising electrolyte due to its stability and high ionic conductivity. Two major challenges for commercialization are manufacturing of thin layers and creating stable, low-impedance, interfaces with both anode and cathode materials. Atomic Layer Deposition (ALD) has recently been shown as a potential method for depositing both solid electrolytes and interfacial layers to improve the stability and performance at electrode-electrolyte interfaces in battery systems. Herein we present the first reported ALD process for LLZO, demonstrating the ability to tune composition within the amorphous film and anneal to achieve the desired cubic garnet phase. Formation of the cubic phase was observed at temperatures as low as 555°C, significantly lower than is required for bulk processing. Additionally, challenges associated with achieving a dense garnet phase due to substrate reactivity, morphology changes and Li loss under the necessary high temperature annealing are quantified via in situ synchrotron diffraction.

Authors:
 [1];  [1];  [1];  [1]; ORCiD logo [1];  [1];  [1];  [2]; ORCiD logo [3];  [1]; ORCiD logo [1]
  1. Department of Mechanical Engineering, University of Michigan, Ann Arbor, Michigan 48109, United States
  2. Department of Mechanical Engineering and Materials Science, University of Pittsburgh, Pittsburgh, Pennsylvania 15261, United States
  3. Environmental Molecular Sciences Laboratory, Pacific Northwest National Laboratory, Richland, Washington 99354, United States
Publication Date:
Research Org.:
Pacific Northwest National Laboratory (PNNL), Richland, WA (US), Environmental Molecular Sciences Laboratory (EMSL)
Sponsoring Org.:
USDOE Advanced Research Projects Agency - Energy (ARPA-E)
OSTI Identifier:
1390428
Report Number(s):
PNNL-SA-124464
Journal ID: ISSN 0897-4756; 48885; KP1704020
DOE Contract Number:  
AC05-76RL01830
Resource Type:
Journal Article
Resource Relation:
Journal Name: Chemistry of Materials; Journal Volume: 29; Journal Issue: 8
Country of Publication:
United States
Language:
English
Subject:
solid electrolyte; Atomic layer deposition; LLZO; garnet; Environmental Molecular Sciences Laboratory

Citation Formats

Kazyak, Eric, Chen, Kuan-Hung, Wood, Kevin N., Davis, Andrew L., Thompson, Travis, Bielinski, Ashley R., Sanchez, Adrian J., Wang, Xiang, Wang, Chongmin, Sakamoto, Jeff, and Dasgupta, Neil P. Atomic Layer Deposition of the Solid Electrolyte Garnet Li 7 La 3 Zr 2 O 12. United States: N. p., 2017. Web. doi:10.1021/acs.chemmater.7b00944.
Kazyak, Eric, Chen, Kuan-Hung, Wood, Kevin N., Davis, Andrew L., Thompson, Travis, Bielinski, Ashley R., Sanchez, Adrian J., Wang, Xiang, Wang, Chongmin, Sakamoto, Jeff, & Dasgupta, Neil P. Atomic Layer Deposition of the Solid Electrolyte Garnet Li 7 La 3 Zr 2 O 12. United States. doi:10.1021/acs.chemmater.7b00944.
Kazyak, Eric, Chen, Kuan-Hung, Wood, Kevin N., Davis, Andrew L., Thompson, Travis, Bielinski, Ashley R., Sanchez, Adrian J., Wang, Xiang, Wang, Chongmin, Sakamoto, Jeff, and Dasgupta, Neil P. Thu . "Atomic Layer Deposition of the Solid Electrolyte Garnet Li 7 La 3 Zr 2 O 12". United States. doi:10.1021/acs.chemmater.7b00944.
@article{osti_1390428,
title = {Atomic Layer Deposition of the Solid Electrolyte Garnet Li 7 La 3 Zr 2 O 12},
author = {Kazyak, Eric and Chen, Kuan-Hung and Wood, Kevin N. and Davis, Andrew L. and Thompson, Travis and Bielinski, Ashley R. and Sanchez, Adrian J. and Wang, Xiang and Wang, Chongmin and Sakamoto, Jeff and Dasgupta, Neil P.},
abstractNote = {Lithium solid electrolytes are a promising platform for achieving high energy density, long-lasting, and safe rechargeable batteries, which could have widespread societal impact. In particular, the ceramic oxide garnet Li7La3Zr2O12 (LLZO) has been shown to be a promising electrolyte due to its stability and high ionic conductivity. Two major challenges for commercialization are manufacturing of thin layers and creating stable, low-impedance, interfaces with both anode and cathode materials. Atomic Layer Deposition (ALD) has recently been shown as a potential method for depositing both solid electrolytes and interfacial layers to improve the stability and performance at electrode-electrolyte interfaces in battery systems. Herein we present the first reported ALD process for LLZO, demonstrating the ability to tune composition within the amorphous film and anneal to achieve the desired cubic garnet phase. Formation of the cubic phase was observed at temperatures as low as 555°C, significantly lower than is required for bulk processing. Additionally, challenges associated with achieving a dense garnet phase due to substrate reactivity, morphology changes and Li loss under the necessary high temperature annealing are quantified via in situ synchrotron diffraction.},
doi = {10.1021/acs.chemmater.7b00944},
journal = {Chemistry of Materials},
number = 8,
volume = 29,
place = {United States},
year = {Thu Apr 13 00:00:00 EDT 2017},
month = {Thu Apr 13 00:00:00 EDT 2017}
}