Y-Doped NASICON-type LiZr2(PO4)3 Solid Electrolytes for Lithium Metal Batteries

Low ionic conductivity limits the development of NASICON-type LiZr2(PO4)(3) (LZP) for solid-state batteries. Here, we present the possible factors that may affect the conductivity and further establish the relationships among conductivity, crystal structure, relative density, grain size, chemical composition, and elemental distribution. The conditions for the existence of the four phases of LZP (alpha, alpha', ss, and ss') and the phase transition processes among them are systematically clarified. With secondary ion mass spectrometry, the spatial distribution of elements within the grains and grain boundaries is clearly presented. On the basis of our results, proper elemental doping, high sintering temperature, and especially fast cool down rate are all indispensable to stabilize the high-conductivity (alpha) phase at room temperature. Finally, we demonstrate the feasibility of lithium-based batteries with this LZP solid electrolyte and commercial cathodes. This work provides insights for preparing LZP with high conductivity and paves the way for the development of solid-state batteries.