Tailoring the grain boundary structure and chemistry of the dendrite-free garnet solid electrolyte Li6.1Ga0.3La3Zr2O12

Abstract Garnet-type Li6.1Ga0.3La3Zr2O12 (LGLZO) exhibits high ionic conductivity and extremely low electronic conductivity. The electrochemical properties strongly depend on the characteristics of the grain boundaries and pores in the oxide–ceramic electrolyte. Currently, the main issue of LGLZO is...

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Main Authors: Rae-Hyun Lee, Chea-Yun Kang, Jong-Kyu Lee, Bong-Soo Jin, Kyong-Nam Kim, Hyun-Soo Kim, Jung-Rag Yoon, Seung-Hwan Lee
Format: Article
Language:English
Published: Nature Portfolio 2024-08-01
Series:NPG Asia Materials
Online Access:https://doi.org/10.1038/s41427-024-00563-7
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author Rae-Hyun Lee
Chea-Yun Kang
Jong-Kyu Lee
Bong-Soo Jin
Kyong-Nam Kim
Hyun-Soo Kim
Jung-Rag Yoon
Seung-Hwan Lee
author_facet Rae-Hyun Lee
Chea-Yun Kang
Jong-Kyu Lee
Bong-Soo Jin
Kyong-Nam Kim
Hyun-Soo Kim
Jung-Rag Yoon
Seung-Hwan Lee
author_sort Rae-Hyun Lee
collection DOAJ
description Abstract Garnet-type Li6.1Ga0.3La3Zr2O12 (LGLZO) exhibits high ionic conductivity and extremely low electronic conductivity. The electrochemical properties strongly depend on the characteristics of the grain boundaries and pores in the oxide–ceramic electrolyte. Currently, the main issue of LGLZO is its large grain boundary resistance due to high-temperature sintering. Herein, we propose an effective method for reinforcing the chemical and structural characteristics of the grain boundaries using a Li2O-B2O3-Al2O3 (LBA) sintering aid. In this study, the LBA sintering aid is critical because it fills grain boundaries and void spaces. As a result, LGLZO solid-state electrolytes with sintering aids significantly enhance the ionic conductivity and reduce the activation energy, especially in the grain boundary region. Another crucial issue is the formation of Li dendrites in LGLZO. Since dendritic Li propagates along the grain boundaries, the optimized LGLZO solid-state electrolyte demonstrates excellent stability against Li metals. Overall, the LGLZO electrolyte with the LBA sintering aid exhibits stable long-term cycling performance due to the well-designed grain boundaries.
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institution Kabale University
issn 1884-4057
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publishDate 2024-08-01
publisher Nature Portfolio
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spelling doaj-art-7b83b85721d34e9382f9777665657a432025-01-19T12:28:53ZengNature PortfolioNPG Asia Materials1884-40572024-08-0116111210.1038/s41427-024-00563-7Tailoring the grain boundary structure and chemistry of the dendrite-free garnet solid electrolyte Li6.1Ga0.3La3Zr2O12Rae-Hyun Lee0Chea-Yun Kang1Jong-Kyu Lee2Bong-Soo Jin3Kyong-Nam Kim4Hyun-Soo Kim5Jung-Rag Yoon6Seung-Hwan Lee7Department of Battery Convergence Engineering, Kangwon National UniversityDepartment of Battery Convergence Engineering, Kangwon National UniversityDepartment of Battery Convergence Engineering, Kangwon National UniversityDepartment of Materials Science and Engineering, Korea Electrotechnology Research Institute (KERI)Department of Semiconductor Engineering, Daejeon UniversityDepartment of Materials Science and Engineering, Korea Electrotechnology Research Institute (KERI)R&D Center, Samwha CapacitorDepartment of Battery Convergence Engineering, Kangwon National UniversityAbstract Garnet-type Li6.1Ga0.3La3Zr2O12 (LGLZO) exhibits high ionic conductivity and extremely low electronic conductivity. The electrochemical properties strongly depend on the characteristics of the grain boundaries and pores in the oxide–ceramic electrolyte. Currently, the main issue of LGLZO is its large grain boundary resistance due to high-temperature sintering. Herein, we propose an effective method for reinforcing the chemical and structural characteristics of the grain boundaries using a Li2O-B2O3-Al2O3 (LBA) sintering aid. In this study, the LBA sintering aid is critical because it fills grain boundaries and void spaces. As a result, LGLZO solid-state electrolytes with sintering aids significantly enhance the ionic conductivity and reduce the activation energy, especially in the grain boundary region. Another crucial issue is the formation of Li dendrites in LGLZO. Since dendritic Li propagates along the grain boundaries, the optimized LGLZO solid-state electrolyte demonstrates excellent stability against Li metals. Overall, the LGLZO electrolyte with the LBA sintering aid exhibits stable long-term cycling performance due to the well-designed grain boundaries.https://doi.org/10.1038/s41427-024-00563-7
spellingShingle Rae-Hyun Lee
Chea-Yun Kang
Jong-Kyu Lee
Bong-Soo Jin
Kyong-Nam Kim
Hyun-Soo Kim
Jung-Rag Yoon
Seung-Hwan Lee
Tailoring the grain boundary structure and chemistry of the dendrite-free garnet solid electrolyte Li6.1Ga0.3La3Zr2O12
NPG Asia Materials
title Tailoring the grain boundary structure and chemistry of the dendrite-free garnet solid electrolyte Li6.1Ga0.3La3Zr2O12
title_full Tailoring the grain boundary structure and chemistry of the dendrite-free garnet solid electrolyte Li6.1Ga0.3La3Zr2O12
title_fullStr Tailoring the grain boundary structure and chemistry of the dendrite-free garnet solid electrolyte Li6.1Ga0.3La3Zr2O12
title_full_unstemmed Tailoring the grain boundary structure and chemistry of the dendrite-free garnet solid electrolyte Li6.1Ga0.3La3Zr2O12
title_short Tailoring the grain boundary structure and chemistry of the dendrite-free garnet solid electrolyte Li6.1Ga0.3La3Zr2O12
title_sort tailoring the grain boundary structure and chemistry of the dendrite free garnet solid electrolyte li6 1ga0 3la3zr2o12
url https://doi.org/10.1038/s41427-024-00563-7
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