Lithium-ion diffusion in the grain boundary of polycrystalline solid electrolyte Li_6.75La₃Zr_1.5Ta_0.5O₁₂ (LLZTO): a computer simulation and theoretical study

Abstract

Lithium-ion diffusion ability in solid electrolytes is crucial for the performance and safety of lithium-ion batteries. However, the lithium-ion diffusion coefficient of Li6.75La3Zr1.5Ta0.5O12 (LLZTO) measured experimentally is much lower than...

Going against the Grain: Atomistic Modeling of Grain Boundaries in Solid Electrolytes for Solid-State Batteries

“…Alternatively, the doping of Al at LLZO GBs was found to have a minimal impact on the Li-ion conductivity as a result of the immobile Al ions blocking nearby Li-ion hopping. DFT and AIMD simulations were also conducted for Ta-doped LLZO and it was again found that the GBs in this material result in significant interfacial resistance, possibly due to the formation of secondary phases with high Li-ion migration barriers …”

“…DFT and AIMD simulations were also conducted for Ta-doped LLZO and it was again found that the GBs in this material result in significant interfacial resistance, possibly due to the formation of secondary phases with high Li-ion migration barriers. 74 Perovskite oxide solid electrolytes have also received attention due to their GB properties. We carried out an atomistic modeling study of GBs in Li 3x La (2/3)−x TiO 3 (0 < x < 0.16, LLTO) using classical MD simulations.…”