Molecular Dynamics Studies on the Lithium Ion Conduction Behaviors Depending on Tilted Grain Boundaries with Various Symmetries in Garnet-Type Li7La3Zr2O12

Grain boundary (GB) structure is a critical parameter that significantly affects the macroscopic properties of materials; however, the evaluation of GB characteristics by modern analytical methods remains an extremely challenging task. In this work, Li+ conductivity degradation at the GBs of cubic Li7La3Zr2O12 (LLZO) with a garnet framework (which represents the most promising candidate material for solid electrolytes utilized in all-solid-state batteries) has been investigated by various molecular dynamics approaches combined with newly developed analytical techniques. It was found that the transboundary diffusion of Li ions was generally slower than their diffusion in the bulk regardless of the GB symmetry; however, this effect strongly depended on the concentration of Li-deficient sites (trapping Li vacancies) in the GB layer. Furthermore, the compactness and density of the combined GB regions represent the key parameters affecting the overall Li+ conductivity of polycrystalline LLZO films.