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.

Garnet-Type Solid-State Electrolytes: Materials, Interfaces, and Batteries.

This review article deals with the ionic conductivity of solid‐state electrolytes for lithium batteries. It has discussed the mechanisms of ion conduction in ceramics, polymers, and ceramic‐polymer composite electrolytes. In ceramic electrolytes, ion transport is accomplished with mobile point defects in a crystal. Li+ ions migrate mainly via the vacancy mechanism, interstitial mechanism, or interstitial‐substitutional exchange mechanism. In solid polymer electrolytes, Li+ ions are transported mainly via the segment motion, ion hopping (Grotthuss mechanism), or vehicle mechanism (mass diffusion). This study has also introduced various electrolyte materials including perovskite oxides, garnet oxides, sodium superionic conductors, phosphates, sulfides, halides, cross‐linked polymers, block‐copolymers, metal‐organic frameworks, covalent organic frameworks, as well as ceramic‐polymer composites. In addition, it has highlighted some strategies to improve the ionic conductivity of solid‐state electrolytes, such as doping, defect engineering, microstructure tuning, and interface modification.

https://onlinelibrary.wiley.com/doi/pdfdirect/10.1002/ese3.1163

Ionic conductivity and ion transport mechanisms of solid‐state lithium‐ion battery electrolytes: A review

Organic batteries for a greener rechargeable world

The Role of Interlayer Chemistry in Li‐Metal Growth through a Garnet‐Type Solid Electrolyte

To satisfy the ever-increasing demand for higher energy density, solid-state batteries (SSBs) have received significant attention due to their potential in providing energy densities greater than 400 Wh kg−1. And as a key material in SSBs, the garnet-type Li7La3Zr2O12 (LLZO) electrolyte is particularly promising because of its high ionic conductivity at room temperature and excellent chemical stability against Li metal. And although great progress has been achieved for garnet electrolytes, many critical issues remain in terms of the practical application of garnet-based SSBs with truly high energy densities. Based on this, this review will provide an overview of the current progress in solid garnet batteries in terms of electrolyte fabrication and interfacial engineering in prototype cells. In addition, various strategies used to meet application requirements are comprehensively reviewed, including not only strategies to enhance energy density, but also methods to enhance rate capability, extend cycle life, decrease cost and reduce thermal runaways. Furthermore, crucial challenges are presented and future research directions are proposed in the development of high-performance solid lithium batteries.

Comprehensive Investigation into Garnet Electrolytes Toward Application-Oriented Solid Lithium Batteries

Recently, all-solid-state batteries (ASSBs) have attracted increasing interest owing to their higher energy density and safety. As the core material of ASSBs, the characteristics of the solid electrolyte largely determine the performance of the battery. Thus far, a variety of inorganic solid electrolytes have been studied, including the NASICON-type, LISICON-type, perovskite-type, garnet-type, glassy solid electrolyte, and so on. The garnet Li7La3Zr2O12 (LLZO) solid electrolyte is one of the most promising candidates because of its excellent comprehensively electrochemical performance. Both, experiments and theoretical calculations, show that cubic LLZO has high room-temperature ionic conductivity and good chemical stability while contacting with the lithium anode and most of the cathode materials. In this paper, the crystal structure, Li-ion transport mechanism, preparation method, and element doping of LLZO are introduced in detail based on the research progress in recent years. Then, the development prospects and challenges of LLZO as applied to ASSBs are discussed.

/pdf/modeling-preparation-and-elemental-doping-of-li7la3zr2o12-9y902y488r.pdf

Modeling, Preparation, and Elemental Doping of Li7La3Zr2O12 Garnet-Type Solid Electrolytes: A Review

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Modeling, Preparation, and Elemental Doping of Li7La3Zr2O12 Garnet-Type Solid Electrolytes: A Review