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Journal of Advanced Ceramics 2024, 13(2): 166-175 https://doi.org/10.26599/JAC.2024.9220829
Research Article | Open Access | Issue | Published: 08 March 2024

Constructing electron-blocking grain boundaries in garnet to suppress lithium dendrite growth

Show Author's Information Xing Xiang1,2,3,4,  Zecheng Fang1,  Congkun Du1,  Zhenzhen Zhao1,  Jiajia Chen1,  Yanhua Zhang1,  Huihu Wang1,  Chenhuinan Wei1,  Fei Chen2,5( ),  Qiang Shen2,5
Hubei Provincial Key Laboratory of Green Materials for Light Industry, Hubei University of Technology, Wuhan 430068, China
Hubei Longzhong Laboratory, Wuhan University of Technology Xiangyang Demonstration Zone, Xiangyang 441000, China
Collaborative Innovation Center of Green Light-weight Materials and Processing, Hubei University of Technology, Wuhan 430068, China
New Materials and Green Manufacturing Talent Introduction and Innovation Demonstration Base, Hubei University of Technology, Wuhan 430068, China
State Key Lab of Advanced Technology for Materials Synthesis and Processing, Wuhan University of Technology, Wuhan 430070, China
Keywords:
microstructure, lithium dendrite, solid-state batteries, solid electrolyte, garnet
Cite this article:
Xiang X, Fang Z, Du C, et al. Constructing electron-blocking grain boundaries in garnet to suppress lithium dendrite growth. Journal of Advanced Ceramics, 2024, 13(2): 166-175. https://doi.org/10.26599/JAC.2024.9220829
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Abstract Full text About this article

Li7La3Zr2O12 (LLZO) is considered as a promising solid-state electrolyte due to its high ionic conductivity, wide electrochemical window, and excellent electrochemical stability. However, its application in solid-state lithium metal batteries (SSLMBs) is impeded by the growth of lithium dendrites in LLZO due to some reasons such as its high electronic conductivity. In this study, lithium fluoride (LiF) was introduced into Ta-doped LLZO (LLZTO) to modify its grain boundaries to enhance the performance of SSLMBs. A nanoscale LiF layer was uniformly coated on the LLZTO grains, creating a three-dimensional continuous electron-blocking network at the grain boundaries. Benefiting from the electronic insulator LiF and the special structure of the modified LLZTO, the symmetric cells based on LLZO achieved a high critical current density (CCD) of 1.1 mA·cm−2 (in capacity-constant mode) and maintained stability over 2000 h at 0.3 mA·cm−2. Moreover, the full cells combined with a LiFePO4 (LFP) cathode, demonstrated excellent cycling performance, retaining 97.1% of capacity retention after 500 cycles at 0.5 C. Therefore, this work provides a facile and effective approach for preparing a modified electrolyte suitable for high-performance SSLMBs.


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About this article

Constructing electron-blocking grain boundaries in garnet to suppress lithium dendrite growth

Show Author's information Xing Xiang1,2,3,4, Zecheng Fang1, Congkun Du1, Zhenzhen Zhao1, Jiajia Chen1, Yanhua Zhang1, Huihu Wang1, Chenhuinan Wei1, Fei Chen2,5( ), Qiang Shen2,5
Hubei Provincial Key Laboratory of Green Materials for Light Industry, Hubei University of Technology, Wuhan 430068, China
Hubei Longzhong Laboratory, Wuhan University of Technology Xiangyang Demonstration Zone, Xiangyang 441000, China
Collaborative Innovation Center of Green Light-weight Materials and Processing, Hubei University of Technology, Wuhan 430068, China
New Materials and Green Manufacturing Talent Introduction and Innovation Demonstration Base, Hubei University of Technology, Wuhan 430068, China
State Key Lab of Advanced Technology for Materials Synthesis and Processing, Wuhan University of Technology, Wuhan 430070, China

Abstract

Li7La3Zr2O12 (LLZO) is considered as a promising solid-state electrolyte due to its high ionic conductivity, wide electrochemical window, and excellent electrochemical stability. However, its application in solid-state lithium metal batteries (SSLMBs) is impeded by the growth of lithium dendrites in LLZO due to some reasons such as its high electronic conductivity. In this study, lithium fluoride (LiF) was introduced into Ta-doped LLZO (LLZTO) to modify its grain boundaries to enhance the performance of SSLMBs. A nanoscale LiF layer was uniformly coated on the LLZTO grains, creating a three-dimensional continuous electron-blocking network at the grain boundaries. Benefiting from the electronic insulator LiF and the special structure of the modified LLZTO, the symmetric cells based on LLZO achieved a high critical current density (CCD) of 1.1 mA·cm−2 (in capacity-constant mode) and maintained stability over 2000 h at 0.3 mA·cm−2. Moreover, the full cells combined with a LiFePO4 (LFP) cathode, demonstrated excellent cycling performance, retaining 97.1% of capacity retention after 500 cycles at 0.5 C. Therefore, this work provides a facile and effective approach for preparing a modified electrolyte suitable for high-performance SSLMBs.

Keywords: microstructure, lithium dendrite, solid-state batteries, solid electrolyte, garnet

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Publication history
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Publication history

Received: 04 September 2023
Revised: 23 October 2023
Accepted: 17 November 2023
Published: 08 March 2024
Issue date: February 2024

Copyright

© The Author(s) 2024.

Acknowledgements

Acknowledgements

This work is supported by the National Natural Science Foundation of China (No. 52202231), the Natural Science Foundation of Hubei Province (No. 2023AFB316), the Independent Innovation Projects of the Hubei Longzhong Laboratory (No. 2022ZZ-16), and the State Key Laboratory of Advanced Technology for Materials Synthesis and Processing (Wuhan University of Technology) (No. 2022-KF-23).

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This is an open access article under the terms of the Creative Commons Attribution 4.0 International License (CC BY 4.0, http://creativecommons.org/licenses/by/4.0/).

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