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Nano Research 2023, 16(7): 9344-9351 https://doi.org/10.1007/s12274-023-5559-4
Research Article | Issue | Published: 13 March 2023

Stable all-solid-state Li-Te battery with Li3TbBr6 superionic conductor

Show Author's Information Zhichao Zeng1,§,  Xiaomeng Shi1,§,  Mingzi Sun2,  Hongtu Zhang1,  Wei Luo3,  Yunhui Huang3,  Bolong Huang2( ),  Yaping Du1( ),  Chun-Hua Yan1,4,5
Tianjin Key Lab for Rare Earth Materials and Applications, Center for Rare Earth and Inorganic Functional Materials, Haihe Laboratory of Sustainable Chemical Transformations, Smart Sensing Interdisciplinary Science Center, School of Materials Science and Engineering, National Institute for Advanced Materials, Nankai University, Tianjin 300350, China
Department of Applied Biology and Chemical Technology, The Hong Kong Polytechnic University, Hung Hom, Kowloon, Hong Kong 999077, China
Institute of New Energy for Vehicles, School of Materials Science and Engineering, Tongji University, Shanghai 201804, China
Beijing National Laboratory for Molecular Sciences, State Key Laboratory of Rare Earth Materials, Chemistry and Applications, PKU-HKU Joint Laboratory in Rare Earth Materials and Bioinorganic Chemistry, College of Chemistry and Molecular Engineering, Peking University, Beijing 100871, China
College of Chemistry and Chemical Engineering, Lanzhou University, Lanzhou 730000, China

§ Zhichao Zeng and Xiaomeng Shi contributed equally to this work.

Keywords:
superionic conductor, solid electrolytes, all-solid-state lithium batteries, Li-Te solid battery, rare-earth halide
Topics:
Lithium batteries
Cite this article:
Zeng Z, Shi X, Sun M, et al. Stable all-solid-state Li-Te battery with Li3TbBr6 superionic conductor. Nano Research, 2023, 16(7): 9344-9351. https://doi.org/10.1007/s12274-023-5559-4
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Abstract Full text Electronic supplementary material About this article

Rare-earth (RE) halide solid electrolytes (HSEs) have been an emerging research area due to their good electrochemical and mechanical properties for all-solid-state lithium batteries (ASSBs). However, only very limited types of HSEs have been reported with high performance. In this work, tens of grams of RE-HSE Li3TbBr6 (LTbB) was synthesized by a vacuum evaporation-assisted method. The as-prepared LTbB displays a high ionic conductivity of 1.7 mS·cm−1, a wide electrochemical window, and good formability. Accordingly, the assembled solid lithium-tellurium (Li-Te) battery based on the LTbB HSE exhibits excellent cycling stability up to 600 cycles, which is superior to most previous reports. The processes and the chemicals during the discharge/charge of Li-Te batteries have been studied by various in situ and ex situ characterizations. Theoretical calculations have demonstrated the dominant conductivity contributions of the direct [octahedral]–[octahedral] ([Oct]–[Oct]) pathway for Li ion migrations in the electrolyte. The Tb sites guarantee efficient electron transfer while the Li 2s orbitals are not affected during migration, leading to a low activation barrier. Therefore, this successful fabrication and application of LTbB have offered a highly competitive solution for solid electrolytes in ASSBs, indicating the great potential of RE-based HSEs in energy devices.


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Abstract
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Electronic supplementary material
About this article

Stable all-solid-state Li-Te battery with Li3TbBr6 superionic conductor

Show Author's information Zhichao Zeng1,§, Xiaomeng Shi1,§, Mingzi Sun2, Hongtu Zhang1, Wei Luo3, Yunhui Huang3, Bolong Huang2( ), Yaping Du1( ), Chun-Hua Yan1,4,5
Tianjin Key Lab for Rare Earth Materials and Applications, Center for Rare Earth and Inorganic Functional Materials, Haihe Laboratory of Sustainable Chemical Transformations, Smart Sensing Interdisciplinary Science Center, School of Materials Science and Engineering, National Institute for Advanced Materials, Nankai University, Tianjin 300350, China
Department of Applied Biology and Chemical Technology, The Hong Kong Polytechnic University, Hung Hom, Kowloon, Hong Kong 999077, China
Institute of New Energy for Vehicles, School of Materials Science and Engineering, Tongji University, Shanghai 201804, China
Beijing National Laboratory for Molecular Sciences, State Key Laboratory of Rare Earth Materials, Chemistry and Applications, PKU-HKU Joint Laboratory in Rare Earth Materials and Bioinorganic Chemistry, College of Chemistry and Molecular Engineering, Peking University, Beijing 100871, China
College of Chemistry and Chemical Engineering, Lanzhou University, Lanzhou 730000, China

§ Zhichao Zeng and Xiaomeng Shi contributed equally to this work.

Abstract

Rare-earth (RE) halide solid electrolytes (HSEs) have been an emerging research area due to their good electrochemical and mechanical properties for all-solid-state lithium batteries (ASSBs). However, only very limited types of HSEs have been reported with high performance. In this work, tens of grams of RE-HSE Li3TbBr6 (LTbB) was synthesized by a vacuum evaporation-assisted method. The as-prepared LTbB displays a high ionic conductivity of 1.7 mS·cm−1, a wide electrochemical window, and good formability. Accordingly, the assembled solid lithium-tellurium (Li-Te) battery based on the LTbB HSE exhibits excellent cycling stability up to 600 cycles, which is superior to most previous reports. The processes and the chemicals during the discharge/charge of Li-Te batteries have been studied by various in situ and ex situ characterizations. Theoretical calculations have demonstrated the dominant conductivity contributions of the direct [octahedral]–[octahedral] ([Oct]–[Oct]) pathway for Li ion migrations in the electrolyte. The Tb sites guarantee efficient electron transfer while the Li 2s orbitals are not affected during migration, leading to a low activation barrier. Therefore, this successful fabrication and application of LTbB have offered a highly competitive solution for solid electrolytes in ASSBs, indicating the great potential of RE-based HSEs in energy devices.

Keywords: superionic conductor, solid electrolytes, all-solid-state lithium batteries, Li-Te solid battery, rare-earth halide

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Publication history
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Acknowledgements

Publication history

Received: 29 November 2022
Revised: 07 February 2023
Accepted: 09 February 2023
Published: 13 March 2023
Issue date: July 2023

Copyright

© Tsinghua University Press 2023

Acknowledgements

Acknowledgements

This work was supported by the National Key R&D Program of China (No. 2021YFA1501101), the Natural Science Foundation of China (No. 21971117), Functional Research Funds for the Central Universities, Nankai University (No. 63186005), Tianjin Key Lab for Rare Earth Materials and Applications (No. ZB19500202), the National Natural Science Foundation of China/Research Grant Council Joint Research Scheme (No. N_PolyU502/21), 111 Project (No. B18030) from China, Outstanding Youth Project of Tianjin Natural Science Foundation (No. 20JCJQJC00130), Key Project of Tianjin Natural Science Foundation (No. 20JCZDJC00650), the Projects of Strategic Importance of The Hong Kong Polytechnic University (No. 1-ZE2V), Shenzhen Fundamental Research Scheme-General Program (No. JCYJ20220531090807017), National Postdoctoral Program for Innovative Talents (No. BX20220157), Open Foundation of State Key Laboratory of Featured Metal Materials and Life-cycle Safety for Composite Structures (No. 2022GXYSOF07), and Haihe Laboratory of Sustainable Chemical Transformations. B. L. H. also thanks the support from Research Centre for Carbon-Strategic Catalysis (RCCSC), Research Institute for Smart Energy (RISE), and Research Institute for Intelligent Wearable Systems (RI-IWEAR) of the Hong Kong Polytechnic University.

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