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Review Issue
Challenge and Solution of Garnet Oxide Solid Electrolyte for All-Solid-State Lithium Battery
Journal of the Chinese Ceramic Society 2025, 53(6): 1672-1684
Published: 19 May 2025
Abstract PDF (21.3 MB) Collect
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Garnet-type solid electrolytes are the most promising materials available, which attract much attention, due to their high ionic conductivity, wide electrochemical window, and stability with lithium. However, some challenges such as surface stability, lithium dendrite penetration, and cost remain critical for its industrialization. This review focuses on the crystal structure and ion conduction mechanisms of garnet-type oxide solid electrolyte (Li7La3Zr2O12, LLZO) to investigate the formation mechanisms and removal strategies for surface passivation layers, including lithium carbonate and lithium hydroxide. For the lithium dendrite penetration of LLZO, potential solutions are explored in view of the black and surface properties electrolyte. For the industrialization, this review analyzes the cost optimization strategies for garnet-type solid electrolytes, aiming to provide valuable insights for industrial advancement.

Summary and prospects

Garnet-type oxide solid electrolytes hold a significant promise for solid-state batteries due to their high ionic conductivity and wide electrochemical window. However, large-scale production faces several challenges, i.e., 1) poor stability against air leading to the formation of lithium carbonate, 2) preventing the growth of lithium dendrites at the anode interface, and 3) high costs. These issues hinder the application of garnet-type all-solid-state batteries. Future development in garnet oxide solid electrolyte should focus on the following aspects. First, the surface alkalinity and the mechanism of lithium carbonate formation should be characterized accurately. It is crucial to contrude the excessive addition of lithium raw materials. While excess lithium can compensate for lithium losses during the heating and lead to lithium accumulation on the surface. Thus, a dynamic equilibrium must be established between the lithium supplement during sintering and the residual lithium on the surface. Furthermore, the formation of lithium carbonate is a dynamic process. Removing lithium carbonate is thus insufficient. Instead, it is indicated to convert lithium carbonate into a protective barrier that is both conductive to lithium ions and stable in air. Second, previous work proposed to mitigate the growth of lithium dendrites at LLZO/Li interface via incorporating the artificial solid electrolyte interphases (SEI) or buffer layers, which could facilitate a uniform electric field distribution and promote even lithium deposition at the interface. Moreover, the fabrication of highly densified LLZO represents an idea approach to alleviate the lithium dendrite growth. Third, , rare-earth elements are widely used for doping to improve the ionic conductivity, which increases the cost of raw materials. The existing low-cost element doping, such as Si, Fe, Ca and W, are developed. In addition, developing a low-carbon sintering method is also an important way to reduce the cost. All-solid-state lithium batteries show a great potential with the continuous research efforts.

Open Access Review Issue
Design of Solid Electrolytes with Fast Ion Transport: Computation-Driven and Practical Approaches
Energy Material Advances 2023, 4: 0015
Published: 28 February 2023
Abstract PDF (29.4 MB) Collect
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For next-generation all-solid-state metal batteries, the computation can lead to the discovery of new solid electrolytes with increased ionic conductivity and excellent safety. Based on computational predictions, a new proposed solid electrolyte with a flat energy landscape and fast ion migration is synthesized using traditional synthesis methods. Despite the promise of the predicted solid electrolyte candidates, conventional synthetic methods are frequently hampered by extensive optimization procedures and overpriced raw materials. It is impossible to rationally develop novel superionic conductors without a comprehensive understanding of ion migration mechanisms. In this review, we cover ion migration mechanisms and all emerging computational approaches that can be applied to explore ion conduction in inorganic materials. The general illustrations of sulfide and oxide electrolyte structures as well as their fundamental features, including ion migration paths, dimensionalities, defects, and ion occupancies, are systematically discussed. The major challenges to designing the solid electrolyte and their solving strategies are highlighted, such as lattice softness, polarizability, and structural disorder. In addition to an overview of recent findings, we propose a computational and experimental approach for designing high-performance solid electrolytes. This review article will contribute to a practical understanding of ion conduction, designing, rapid optimization, and screening of advanced solid electrolytes in order to eliminate liquid electrolytes.

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