Preparation and Properties of Ta, Ba Co-Doped Garnet-Type Li7La3Zr2O12 Electrolyte

Abstract

Abstract: Conventional lithium-ion batteries using organic liquid electrolytes suffer from limited energy density and safety risks. To improve energy density and safety, all-solid-state lithium battery are developed using solid electrolytes. Among various inorganic solid-state electrolytes, the garnet-type Li₇La₃Zr₂O₁₂ electrolytes have attracted a great deal of attention, owing to high ionic conductivity and the excellent stability against Li metal. In order to further improve the conductivity, the garnet-type electrolytes Ta and Ba co-doped Li₇La₃Zr₂O₁₂ (Li_7-x+yLa_3-yBa_yZr_2-xTa_xO₁₂) were prepared using solid-state synthesis method. The crystal structure, morphology and ionic conductivity of Li_7-x+yLa_3-yBa_yZr_2-xTa_xO₁₂ (0.4≤x≤0.6, 0≤y≤0.05) electrolytes were systematically investigated by X-ray diffraction (XRD), scanning electron microscope (SEM) and electrochemical impedance spectroscopy (EIS), respectively. The results show that Ta⁵⁺ doping stabilizes the cubic phase. Meanwhile, Ba²⁺ as dopand and sintering agent can decrease the total resistance by promoting the growth of grains and ceramic densification. Notably, the Li_6.45La_2.95Ba_0.05Zr_1.4Ta_0.6O₁₂ sample presents a total conductivity of 1.07×10^-3 S·cm^-1 at room temperature and an activation energy of 0.378 eV. Ta⁵⁺/Ba²⁺ co-doping strategy is conducive to the preparation of garnet-type electrolyte materials with high density and high conductivity.

Key words: solid-state electrolyte, garnet, Li₇La₃Zr₂O₁₂, doping, density, conductivity

CLC Number:

TM911.3

SHEN Ao, ZHOU Jiacheng, XIE Dianchen, JIANG Xue, MA Shucheng, LUO Yali. Preparation and Properties of Ta, Ba Co-Doped Garnet-Type Li₇La₃Zr₂O₁₂ Electrolyte[J]. BULLETIN OF THE CHINESE CERAMIC SOCIETY, 2022, 41(9): 3279-3287.

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Preparation and Properties of Ta, Ba Co-Doped Garnet-Type Li₇La₃Zr₂O₁₂ Electrolyte

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