In the realm of lithium superionic conductors,pursuing higher ionic conductivity is imperative,with the variance in lithium-ion concentration playing a determining role.Due to the permanent and temporary site-blocking...In the realm of lithium superionic conductors,pursuing higher ionic conductivity is imperative,with the variance in lithium-ion concentration playing a determining role.Due to the permanent and temporary site-blocking effects,especially at non-dilute concentrations,not all Li-ions contribute to ionic conductivity.Here,we propose a strategy to directly calculate effective mobile ion concentration in which multiple-ion correlated migration is considered in the percolation analysis with the input of Li-ion distributions and hopping behavior based on kinetic Monte Carlo simulation,termed P-KMC.We provide examples of two representative lithium superionic conductors,cubic garnet-type LixA3B2O12(0≤x≤9;A and B represent different cations)and perovskite-type LixLa2/3−x/3TiO3(0≤x≤0.5),to demonstrate the direct dependence of the ionic conductivity on the effective mobile ion concentration.This methodology provides a robust tool to identify the optimal compositions for the highest ionic conductivity in superionic conductors.展开更多
基金supported by the National Natural Science Foundation of China(Nos.92270124,52102313,92472207)the Hunan Provincial Natural Science Foundation of China(No.2023JJ40635)+1 种基金Shandong Province Natural Science Foundation(No.ZR2022ZD11)the High-Performance Computing Center of Shanghai University and Shanghai Engineering Research Center of Intelligent Computing Systems for providing computing resources and technical support.
文摘In the realm of lithium superionic conductors,pursuing higher ionic conductivity is imperative,with the variance in lithium-ion concentration playing a determining role.Due to the permanent and temporary site-blocking effects,especially at non-dilute concentrations,not all Li-ions contribute to ionic conductivity.Here,we propose a strategy to directly calculate effective mobile ion concentration in which multiple-ion correlated migration is considered in the percolation analysis with the input of Li-ion distributions and hopping behavior based on kinetic Monte Carlo simulation,termed P-KMC.We provide examples of two representative lithium superionic conductors,cubic garnet-type LixA3B2O12(0≤x≤9;A and B represent different cations)and perovskite-type LixLa2/3−x/3TiO3(0≤x≤0.5),to demonstrate the direct dependence of the ionic conductivity on the effective mobile ion concentration.This methodology provides a robust tool to identify the optimal compositions for the highest ionic conductivity in superionic conductors.
