High-performance Ta-doped Li₇La₃Zr₂O₁₂ garnet oxides with AlN additive

Garnet-type oxide is one of the most promising solid-state electrolytes (SSEs) for solid-state lithium-metal batteries (SSLMBs). However, the Li dendrite formation in garnet oxides obstructs the further development of the SSLMBs seriously. Here, we report a high-performance garnet oxide by using AlN as a sintering additive and Li as an anode interface layer. AlN with high thermal conductivity can promote the sintering activity of the garnet oxides, resulting in larger particle size and higher relative density. Moreover, Li₃N with high ionic conductivity formed at grain boundaries and interface can also improve Li-ion transport kinetics. As a result, the garnet oxide electrolytes with AlN show enhanced thermal conductivity, improved ionic conductivity, reduced electronic conductivity, and increased critical current density (CCD), compared with the counterpart using Al₂O₃ sintering aid. In addition, Li symmetric cells and Li|LiFePO₄ (Li|LFP) half cells using the garnet electrolyte with the AlN additive exhibit good electrochemical performances. This work provides a simple and effective strategy for high-performance SSEs.