中国物理B ›› 2024, Vol. 33 ›› Issue (8): 88203-088203.doi: 10.1088/1674-1056/ad41b9

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Defect chemistry engineering of Ga-doped garnet electrolyte with high stability for solid-state lithium metal batteries

Sihan Chen(陈思汗)1, Jun Li(黎俊)1, Keke Liu(刘可可)1, Xiaochen Sun(孙笑晨)1, Jingwei Wan(万京伟)1,2, Huiyu Zhai(翟慧宇)1,2, Xinfeng Tang(唐新峰)1,‡, and Gangjian Tan(谭刚健)1,†   

  1. 1 State Key Laboratory of Advanced Technology for Materials Synthesis and Processing, Wuhan University of Technology, Wuhan 430070, China;
    2 International School of Materials Science & Engineering, Wuhan University of Technology, Wuhan 430070, China
  • 收稿日期:2024-01-30 修回日期:2024-04-12 出版日期:2024-08-15 发布日期:2024-07-15
  • 通讯作者: Gangjian Tan, Xinfeng Tang E-mail:gtan@whut.edu.cn;tangxf@whut.edu.cn
  • 基金资助:
    This work was financially supported by the National Natural Science Foundation of China (Grant No. 52171221) and the National Key Research and Development Program of China (Grant No. 2019YFA0704900).

Defect chemistry engineering of Ga-doped garnet electrolyte with high stability for solid-state lithium metal batteries

Sihan Chen(陈思汗)1, Jun Li(黎俊)1, Keke Liu(刘可可)1, Xiaochen Sun(孙笑晨)1, Jingwei Wan(万京伟)1,2, Huiyu Zhai(翟慧宇)1,2, Xinfeng Tang(唐新峰)1,‡, and Gangjian Tan(谭刚健)1,†   

  1. 1 State Key Laboratory of Advanced Technology for Materials Synthesis and Processing, Wuhan University of Technology, Wuhan 430070, China;
    2 International School of Materials Science & Engineering, Wuhan University of Technology, Wuhan 430070, China
  • Received:2024-01-30 Revised:2024-04-12 Online:2024-08-15 Published:2024-07-15
  • Contact: Gangjian Tan, Xinfeng Tang E-mail:gtan@whut.edu.cn;tangxf@whut.edu.cn
  • Supported by:
    This work was financially supported by the National Natural Science Foundation of China (Grant No. 52171221) and the National Key Research and Development Program of China (Grant No. 2019YFA0704900).

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摘要： Ga-doped Li$_{7}$La$_{3}$Zr$_{2}$O$_{12}$ (Ga-LLZO) has long been considered as a promising garnet-type electrolyte candidate for all-solid-state lithium metal batteries (ASSLBs) due to its high room temperature ionic conductivity. However, the typical synthesis of Ga-LLZO is usually accompanied by the formation of undesired LiGaO$_{2}$ impurity phase that causes severe instability of the electrolyte in contact with molten Li metal during half/full cell assembly. In this study, we show that by simply engineering the defect chemistry of Ga-LLZO, namely, the lithium deficiency level, LiGaO$_{2}$ impurity phase is effectively inhibited in the final synthetic product. Consequently, defect chemistry engineered Ga-LLZO exhibits excellent electrochemical stability against lithium metal, while its high room temperature ionic conductivity ($\sim 1.9 \times 10^{-3}$ S$\cdot$cm$^{-1}$) is well reserved. The assembled Li/Ga-LLZO/Li symmetric cell has a superior critical current density of 0.9 mA$\cdot$cm$^{-2}$, and cycles stably for 500 hours at a current density of 0.3 mA$\cdot$cm$^{-2}$. This research facilitates the potential commercial applications of high performance Ga-LLZO solid electrolytes in ASSLBs.

关键词: Ga-doped Li$_{7}$La$_{3}$Zr$_{2}$O$_{12}$ (Ga-LLZO), defect chemistry engineering, high room temperature ionic conductivity, electrochemical stability

Abstract: Ga-doped Li$_{7}$La$_{3}$Zr$_{2}$O$_{12}$ (Ga-LLZO) has long been considered as a promising garnet-type electrolyte candidate for all-solid-state lithium metal batteries (ASSLBs) due to its high room temperature ionic conductivity. However, the typical synthesis of Ga-LLZO is usually accompanied by the formation of undesired LiGaO$_{2}$ impurity phase that causes severe instability of the electrolyte in contact with molten Li metal during half/full cell assembly. In this study, we show that by simply engineering the defect chemistry of Ga-LLZO, namely, the lithium deficiency level, LiGaO$_{2}$ impurity phase is effectively inhibited in the final synthetic product. Consequently, defect chemistry engineered Ga-LLZO exhibits excellent electrochemical stability against lithium metal, while its high room temperature ionic conductivity ($\sim 1.9 \times 10^{-3}$ S$\cdot$cm$^{-1}$) is well reserved. The assembled Li/Ga-LLZO/Li symmetric cell has a superior critical current density of 0.9 mA$\cdot$cm$^{-2}$, and cycles stably for 500 hours at a current density of 0.3 mA$\cdot$cm$^{-2}$. This research facilitates the potential commercial applications of high performance Ga-LLZO solid electrolytes in ASSLBs.

Key words: Ga-doped Li$_{7}$La$_{3}$Zr$_{2}$O$_{12}$ (Ga-LLZO), defect chemistry engineering, high room temperature ionic conductivity, electrochemical stability

中图分类号:  (Lithium-ion batteries)

  • 82.47.Aa
82.33.Pt (Solid state chemistry) 31.15.-p (Calculations and mathematical techniques in atomic and molecular physics) 82.45.Gj (Electrolytes)