Solid-state nuclear magnetic resonance for garnet-type based solid lithium electrolytes

Abstract

Solid-state batteries show high safety and theoretical energy density, receiving rapidly growing attention in both academic investigations and industrial applications. The garnet-type-based solid electrolytes (Garnet-SEs) play a vital role due to their high Li⁺ conductivity and electrochemical stability. The atomic structure at local environments, such as the Li⁺ coordination and site of doped ions, will have an important impact on the ability of transport and migration pathways that determine ion conductivity and electrochemical performances. In addition to the average structure from long-range perspective, the understanding at atomic level will be crucial for developing strategies to enhance ionic conductivity in Garnet-SEs. Solid-state NMR is a powerful tool that can probe the local atomic environments and dynamics on a molecular level. NMR is proven as a suitable technique for characterizing the light weight and small radius of Li elements, which is challenging for some conventional methods. In this review, atomic structure, ion pathways, and dynamic and microstructure formation of Garnet-SEs from the NMR view were discussed. These insights obtained from various NMR techniques will provide essential information for informing the control development and optimization of Garnet-SEs, contributing to the advancement of high-performance, safe, and reliable solid-state batteries.

Keywords

Solid electrolyte / nuclear magnetic resonance / local structure / lithium dynamic / migration pathway

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