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Title: Optimization of Lithium Content and Sintering Additives in Tape Cast Lithium Garnet Electrolyte Sheets

Abstract

The lithium garnet (LLZO) remains one of the most promising electrolyte materials for producing solid state batteries. Tape casting is one method for producing the thin ceramic electrolyte layer required for a high-performance solid state battery. Processing of LLZO is complicated by several factors including lithium volatilization, abnormal grain growth and phase instability. Many of these issues are exacerbated in tape cast sheets by the sheets' higher surface area to volume ratio, when compared to pellet processing methods. Here, we report on an environmentally friendly aqueous tape casting process for LLZO using methylcellulose as a binder and compare final sheet properties to other, solvent-based, options. Solids loading, binder content, dispersant composition, and wetting agent type are varied to improve ease of casting and enhance properties of the as-cast tape. Lithium content in sintered LLZO sheets is controlled by the inclusion of excess Li2CO3 as lithium source in the ceramic tape itself and by a novel method of producing a lithium-saturated furnace atmosphere. Sintering time and temperature are optimized, and rapid thermal processing is investigated as a method of reducing lithium loss. Al2O3 and MgO are examined for use as sintering additives. Characterization of LLZO sheets is performed with XRD, EISmore » and SEM. Li2CO3 and sintering additive levels are optimized for ionic conductivity and density. The optimization effort improved the conductivity and density of 100µm thick sintered sheets to greater than 3x10-4 S/cm conductivity and 90% density.« less

Authors:
ORCiD logo [1];  [1];  [1]
  1. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Publication Date:
Research Org.:
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Sponsoring Org.:
USDOE Office of Energy Efficiency and Renewable Energy (EERE), Transportation Office. Vehicle Technologies Office
OSTI Identifier:
1798742
Grant/Contract Number:  
AC02-05CH11231
Resource Type:
Accepted Manuscript
Journal Name:
Meeting abstracts (Electrochemical Society. Online)
Additional Journal Information:
Journal Name: Meeting abstracts (Electrochemical Society. Online); Journal Volume: MA2020-02; Journal Issue: 5; Journal ID: ISSN 2151-2043
Publisher:
Electrochemical Society
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE

Citation Formats

Jonson, Robert, Shen, Fengyu, and Tucker, Mike. Optimization of Lithium Content and Sintering Additives in Tape Cast Lithium Garnet Electrolyte Sheets. United States: N. p., 2020. Web. https://doi.org/10.1149/ma2020-025931mtgabs.
Jonson, Robert, Shen, Fengyu, & Tucker, Mike. Optimization of Lithium Content and Sintering Additives in Tape Cast Lithium Garnet Electrolyte Sheets. United States. https://doi.org/10.1149/ma2020-025931mtgabs
Jonson, Robert, Shen, Fengyu, and Tucker, Mike. Mon . "Optimization of Lithium Content and Sintering Additives in Tape Cast Lithium Garnet Electrolyte Sheets". United States. https://doi.org/10.1149/ma2020-025931mtgabs.
@article{osti_1798742,
title = {Optimization of Lithium Content and Sintering Additives in Tape Cast Lithium Garnet Electrolyte Sheets},
author = {Jonson, Robert and Shen, Fengyu and Tucker, Mike},
abstractNote = {The lithium garnet (LLZO) remains one of the most promising electrolyte materials for producing solid state batteries. Tape casting is one method for producing the thin ceramic electrolyte layer required for a high-performance solid state battery. Processing of LLZO is complicated by several factors including lithium volatilization, abnormal grain growth and phase instability. Many of these issues are exacerbated in tape cast sheets by the sheets' higher surface area to volume ratio, when compared to pellet processing methods. Here, we report on an environmentally friendly aqueous tape casting process for LLZO using methylcellulose as a binder and compare final sheet properties to other, solvent-based, options. Solids loading, binder content, dispersant composition, and wetting agent type are varied to improve ease of casting and enhance properties of the as-cast tape. Lithium content in sintered LLZO sheets is controlled by the inclusion of excess Li2CO3 as lithium source in the ceramic tape itself and by a novel method of producing a lithium-saturated furnace atmosphere. Sintering time and temperature are optimized, and rapid thermal processing is investigated as a method of reducing lithium loss. Al2O3 and MgO are examined for use as sintering additives. Characterization of LLZO sheets is performed with XRD, EIS and SEM. Li2CO3 and sintering additive levels are optimized for ionic conductivity and density. The optimization effort improved the conductivity and density of 100µm thick sintered sheets to greater than 3x10-4 S/cm conductivity and 90% density.},
doi = {10.1149/ma2020-025931mtgabs},
journal = {Meeting abstracts (Electrochemical Society. Online)},
number = 5,
volume = MA2020-02,
place = {United States},
year = {2020},
month = {11}
}

Journal Article:
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This content will become publicly available on November 23, 2021
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