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All-solid-state lithium batteries (ASSLBs), which use solid electrolytes instead of liquid ones, have become a hot research topic due to their high energy and power density, ability to solve battery safety issues, and capabilities to fulfill the increasing demand for energy storage in electric vehicles and smart grid applications. Garnet-type solid electrolytes have attracted considerable interest as they meet all the properties of an ideal solid electrolyte for ASSLBs. The garnet-type Li7La3Zr2O12 (LLZO) has excellent environmental stability; experiments and computational analyses showed that this solid electrolyte has a high lithium (Li) ionic conductivity (10-4-10-3 S·cm-1), an electrochemical window as wide as 6 V, stability against Li metal anode, and compatibility with most of the cathode materials. In this review, we present the fundamentals of garnet-type solid electrolytes, preparation methods, air stability, some strategies for improving the conductivity based on experimental and computational results, interfacial issues, and finally applications and challenges for future developments of LLZO solid electrolytes for ASSLBs.


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Garnet-type solid electrolyte: Advances of ionic transport performance and its application in all-solid-state batteries

Show Author's information P. M. GONZALEZ PUENTEaShangbin SONGbShiyu CAObLeana Ziwen RANNALTERaZiwen PANbXing XIANGaQiang SHENaFei CHENa,b( )
State Key Lab of Advanced Technology for Materials Synthesis and Processing, Wuhan University of Technology, Wuhan 430070, China
International School of Materials Science and Engineering, Wuhan University of Technology, Wuhan 430070, China

Abstract

All-solid-state lithium batteries (ASSLBs), which use solid electrolytes instead of liquid ones, have become a hot research topic due to their high energy and power density, ability to solve battery safety issues, and capabilities to fulfill the increasing demand for energy storage in electric vehicles and smart grid applications. Garnet-type solid electrolytes have attracted considerable interest as they meet all the properties of an ideal solid electrolyte for ASSLBs. The garnet-type Li7La3Zr2O12 (LLZO) has excellent environmental stability; experiments and computational analyses showed that this solid electrolyte has a high lithium (Li) ionic conductivity (10-4-10-3 S·cm-1), an electrochemical window as wide as 6 V, stability against Li metal anode, and compatibility with most of the cathode materials. In this review, we present the fundamentals of garnet-type solid electrolytes, preparation methods, air stability, some strategies for improving the conductivity based on experimental and computational results, interfacial issues, and finally applications and challenges for future developments of LLZO solid electrolytes for ASSLBs.

Keywords:

Li7La3Zr2O12 (LLZO), solid electrolytes, lithium ionic conductivity, lithium concentration, mobility of lithium-ion, air stability, solid-state batteries
Received: 01 January 2021 Revised: 04 April 2021 Accepted: 27 April 2021 Published: 27 September 2021 Issue date: October 2021
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Publication history

Received: 01 January 2021
Revised: 04 April 2021
Accepted: 27 April 2021
Published: 27 September 2021
Issue date: October 2021

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© The Author(s) 2021

Acknowledgements

This work is supported by the National Key R&D Program of China (Nos. 2018YFB0905600 and 2017YFB0310400), the National Natural Science Foundation of China (No. 51972246), Fundamental Research Funds for the Central Universities in China, State Key Laboratory of Advanced Electromagnetic Engineering and Technology (Huazhong University of Science and Technology), the "111" project (No. B13035), and the Science and Technology Project of Global Energy Interconnection Research Institute Co., Ltd. (No. SGGR0000WLJS1801080). We would like to thank Asst. Prof. Teresita Padilla-Benavides (Wesleyan University, USA) for help with the language editing.

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