Research progress on key interfacial issues in lithium lanthanum zirconium oxide-based solid-state

doi:10.19799/j.cnki.2095-4239.2022.0097

Abstract

Abstract:

Compared with the current commercial lithium-ion batteries based on organic liquid electrolytes, solid-state lithium (Li) batteries using solid-state electrolytes hold great potential in improving safety and energy density, making them one of the important development directions for next-generation Li batteries. Among many solid-state electrolyte materials, Li₇La₃Zr₂O₁₂ (LLZO), a typical garnet-type solid electrolyte, has attracted extensive attention due to its high Li-ion conductivity and excellent chemical stability against lithium and wide electrochemical windows.However, the introduction of solid lithium lanthanum zirconium oxide (LLZO) causes many interfacial problems, such as noncontinuous physical contact, stress-strain, charge redistribution, and electrochemical instability. These problems affect the electrochemical performance of batteries and induce many new physical and chemical phenomena that require extensive exploration. In this review, from two perspectives of the external interface between the LLZO-based solid electrolyte and the electrode and the intrinsic interface inside the solid electrolyte and the composite electrode, the following topics are extensively discussed based on the research progress in our group and the frontier theoretical viewpoints in this field: First, the formation mechanism of lithium carbonate (Li₂CO₃) on the LLZO powder surface, its influence on electrochemical properties and the strategies to overcome this problem. Second, the effects of the internal interface regulation of LLZO-based electrolyte layers on the Li-ion conductivity and the electrochemical performance of the battery. Third, the characteristics of the LLZO/Li interface and the penetration growth of Li metal in LLZO-based ceramic electrolytes. The mechanism of Li infiltration and dendritic growth induced by the electric field, charge transfer, and stress-strain is also explicitly discussed. Fourth, existing problems of intrinsic interface inside the composite cathode and its integrated construction with the external interface against the solid electrolyte layer. By analyzing and summarizing the key science and technology of LLZO interfacial problems, this review inspires new insights into solving the critical problems of the garnet-type solid electrolyte/electrode interface and promoting the development of high-performance solid-state lithium batteries.

Key words: garnet electrolytes, solid-solid interface, charge transfer, interface manipulation, solid-state lithium batteries

CLC Number:

TM 911

Pengbo ZHAI, Dongmei CHANG, Zhijie BI, Ning ZHAO, Xiangxin GUO. Research progress on key interfacial issues in lithium lanthanum zirconium oxide-based solid-state[J]. Energy Storage Science and Technology, 2022, 11(9): 2847-2865.

Figures/Tables 11

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