SCI和EI收录∣中国化工学会会刊

中国化学工程学报 ›› 2022, Vol. 44 ›› Issue (4): 140-147.DOI: 10.1016/j.cjche.2021.03.030

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Enhanced electrochemical performance of garnet-based solid-state lithium metal battery with modified anodic and cathodic interfaces

Deen Yan1, Huangwang Mai2, Wen Chen1, Wei Yang1, Hanbo Zou1, Shengzhou Chen1   

  1. 1 School of Chemistry and Chemical Engineering, Guangzhou University, Guangzhou 510006, China;
    2 Guangzhou Tinci Materials Technology Co., Ltd., Guangzhou 510760, China
  • 收稿日期:2020-11-14 修回日期:2021-02-25 出版日期:2022-04-28 发布日期:2022-06-18
  • 通讯作者: Hanbo Zou,E-mail:zouhb@gzhu.edu.cn;Shengzhou Chen,E-mail:szchen@gzhu.edu.cn
  • 基金资助:
    This work was subsidized by the National Natural Science Foundation of China (21776051), the Nation Science Foundation of Guangdong (2018A030313423), and the College Students' Innovation and Entrepreneurship Training Program (S201911078039).

Enhanced electrochemical performance of garnet-based solid-state lithium metal battery with modified anodic and cathodic interfaces

Deen Yan1, Huangwang Mai2, Wen Chen1, Wei Yang1, Hanbo Zou1, Shengzhou Chen1   

  1. 1 School of Chemistry and Chemical Engineering, Guangzhou University, Guangzhou 510006, China;
    2 Guangzhou Tinci Materials Technology Co., Ltd., Guangzhou 510760, China
  • Received:2020-11-14 Revised:2021-02-25 Online:2022-04-28 Published:2022-06-18
  • Contact: Hanbo Zou,E-mail:zouhb@gzhu.edu.cn;Shengzhou Chen,E-mail:szchen@gzhu.edu.cn
  • Supported by:
    This work was subsidized by the National Natural Science Foundation of China (21776051), the Nation Science Foundation of Guangdong (2018A030313423), and the College Students' Innovation and Entrepreneurship Training Program (S201911078039).

摘要: Due to high ionic conductivity and wide electrochemical window, the garnet solid electrolyte is considered as the most promising candidate electrolyte for solid-state lithium metal batteries. However, the high contact impedance between metallic lithium and the garnet solid electrolyte surface seriously hampers its further application. In this work, a Li-(ZnO)x anode is prepared by the reaction of zinc oxide with metallic lithium and in situ coated on the surface of Li6.8La3Zr1.8Ta0.2O12(LLZTO). The anode can be perfectly bound to the surface of LLZTO solid electrolyte, and the anode/electrolyte interfacial resistance was reduced from 2319 to 33.75 Ω·cm2. The Li-(ZnO)0.15|LLZTO|Li-(ZnO)0.15 symmetric battery exhibits a stable Li striping/plating process during charge-discharging at a constant current density of 0.1 mA·cm-2 for 100 h at room temperature. Moreover, a Li-(ZnO)0.15|LLZTO-SPE|LFP full battery, comprised of a polyethylene oxide-based solid polymer electrolyte (SPE) film as an interlayer between LiFePO4 (LFP) cathode and LLZTO solid electrolyte, presents an excellent performance at 60 ℃. The discharge capacity of the full battery reaches 140 mA·h·g-1 at 0.1 C and the capacity attenuation is less than 3% after 50 cycles.

关键词: Lithium metal battery, Solid-state electrolyte, Li-ZnO anode

Abstract: Due to high ionic conductivity and wide electrochemical window, the garnet solid electrolyte is considered as the most promising candidate electrolyte for solid-state lithium metal batteries. However, the high contact impedance between metallic lithium and the garnet solid electrolyte surface seriously hampers its further application. In this work, a Li-(ZnO)x anode is prepared by the reaction of zinc oxide with metallic lithium and in situ coated on the surface of Li6.8La3Zr1.8Ta0.2O12(LLZTO). The anode can be perfectly bound to the surface of LLZTO solid electrolyte, and the anode/electrolyte interfacial resistance was reduced from 2319 to 33.75 Ω·cm2. The Li-(ZnO)0.15|LLZTO|Li-(ZnO)0.15 symmetric battery exhibits a stable Li striping/plating process during charge-discharging at a constant current density of 0.1 mA·cm-2 for 100 h at room temperature. Moreover, a Li-(ZnO)0.15|LLZTO-SPE|LFP full battery, comprised of a polyethylene oxide-based solid polymer electrolyte (SPE) film as an interlayer between LiFePO4 (LFP) cathode and LLZTO solid electrolyte, presents an excellent performance at 60 ℃. The discharge capacity of the full battery reaches 140 mA·h·g-1 at 0.1 C and the capacity attenuation is less than 3% after 50 cycles.

Key words: Lithium metal battery, Solid-state electrolyte, Li-ZnO anode