Solid-state batteries
with desirable advantages, including high-energy
density, wide temperature tolerance, and fewer safety-concerns, have
been considered as a promising energy storage technology to replace
organic liquid electrolyte-dominated Li-ion batteries. Solid-state
electrolytes (SSEs) as the most critical component in solid-state
batteries largely lead the future battery development. Among different
types of solid-state electrolytes, garnet-type Li7La3Zr2O12 (LLZO) solid-state electrolytes
have particularly high ionic conductivity (10–3 to
10–4 S/cm) and good chemical stability against Li
metal, offering a great opportunity for solid-state Li-metal batteries.
Since the discovery of garnet-type LLZO in 2007, there has been an
increasing interest in the development of garnet-type solid-state
electrolytes and all solid-state batteries. Garnet-type electrolyte
has been considered one of the most promising and important solid-state
electrolytes for batteries with potential benefits in energy density,
electrochemical stability, high temperature stability, and safety.
In this Review, we will survey recent development of garnet-type LLZO
electrolytes with discussions of experimental studies and theoretical
results in parallel, LLZO electrolyte synthesis strategies and modifications,
stability of garnet solid electrolytes/electrodes, emerging nanostructure
designs, degradation mechanisms and mitigations, and battery architectures
and integrations. We will also provide a target-oriented research
overview of garnet-type LLZO electrolyte and its application in various
types of solid-state battery concepts (e.g., Li-ion, Li–S,
and Li–air), and we will show opportunities and perspectives
as guides for future development of solid electrolytes and solid-state
batteries.
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