Abstract Scope |
Ceramic-based solid-state electrolytes in solid-state batteries for energy storage have attracted much attention. High-entropy ceramics show promising properties in various fields. Here, we design and fabricate a series of Li-garnet (Li7La3Zr2O12, LLZO) based high-entropy electrolytes for improved ionic conductivity. We include multiple factors such as defect energy, valence, and atomic radius to design the chemical formulas. We start with materials with equimolar ratio substituting elements on the Zr site to validate the design factors and the results are in good agreement with our hypothesis. Among these materials, Li7La3Zr0.5Nb0.5Ta0.5Hf0.5O12 shows promising thermal stability, sinterability, and ionic conductivity. We also apply the compositionally complex concept to improve the ionic conductivity further. Detailed crystal structure analysis based on X-ray and neutron diffractions reveals the Li-ion conducting mechanisms. Application and manufacturing case studies of such materials will also be presented. |