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Research Article | Open Access

Co-doping strategy enhanced the ionic conductivity and excellent lithium stability of garnet-type Li7La3Zr2O12 electrolyte in all solid-state lithium batteries

Ziqiang Xua,b, Xin Hua, Bowen Fua, Kashif Khana, Jintian Wua,c, Teng Lia, Haiping Zhoua, Zixuan Fanga(), Mengqiang Wua,b()
School of Materials and Energy, University of Electronic Science and Technology of China, Chengdu, 611731, Sichuan, China
Yangtze Delta Region Institute (HuZhou), University of Electronic Science and Technology of China, Huzhou, 313001, Zhejiang, China
School of Chemical Engineering, Sichuan University of Science & Engineering, Zigong, 643000, China

Peer review under responsibility of The Chinese Ceramic Society.

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Abstract

Garnet-type Li7La3Zr2O12 (LLZO) is one of the most promising solid-state electrolytes (SSEs). However, the application of LLZO is limited by structural instability, low ionic conductivity, and poor lithium stability. To obtain a garnet-type solid electrolyte with a stable structure and high ionic conductivity, a series of TaCe co-doping cubic Li6·4La3ZrTa0.6CeO12 (LLZTCO, x = 0, 0.02, 0.04, 0.06, 0.08, 0.10, 0.20, 0.30) electrolytes were successfully synthesized through conventional solid-phase method. The Ta5+ doping can introduce more lithium vacancies and effectively maintain the stability of the cubic phase. The Ce4+ with a larger ionic radius is introduced into the lattice to widen the Li+ migration bottleneck size, which significantly increased the ionic conductivity to 1.05 × 10−3 S/cm. It also shows excellent stability to lithium metal by the optimization of Li+ transport channel. Li||LLZTCO||Li symmetric cells can cycle stably for more than 6 000 h at a current density of 0.1 mA/cm2 without any surface modifications. The commercialization potential of LLZTCO samples in all solid-state lithium batteries (ASSLBs) is confirmed by the prepared LiFePO4||LLZTCO||Li cells with a capacity retention rate of 98% after 100 cycles at 0.5C. This new co-doping method presents a practical solution for the realization of high-performance ASSLBs.

Keywords

Solid-state electrolytesGarnet-typeCo-dopingBottleneck sizeIonic conductivityLithium stability

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Journal of Materiomics
Volume 9 Issue 4,
July 2023
Pages 651-660
DOI: 10.1016/j.jmat.2023.01.007
Cite this article:
Xu Z, Hu X, Fu B, et al. Co-doping strategy enhanced the ionic conductivity and excellent lithium stability of garnet-type Li7La3Zr2O12 electrolyte in all solid-state lithium batteries. Journal of Materiomics, 2023, 9(4): 651-660. https://doi.org/10.1016/j.jmat.2023.01.007
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