title: Oxygen-driven transition from two-dimensional to three-dimensional transport behaviour in β-Li3PS4 electrolyte.
abstract: Solid state electrolytes with high Li ion conduction are vital to the development of all-solid-state lithium batteries. Lithium thiophosphate Li3PS4 is the parent material of a series of Li superionic conductors Li10MX2S12 (M = Ge, Sn,…; X = P, Si,…), and β-Li3PS4 shows relatively high ionic conductivity itself, though it is not room-temperature stable. The positive effects of introducing O dopants into β-Li3PS4 to stabilize the crystal phase and improve the ionic conducting behaviour are revealed in this study. With the aid of first-principles density functional theory (DFT) computations and quasi-empirical bond-valence calculations, the effects of O doping at different concentrations on the properties of β-Li3PS4 is thoroughly investigated from the aspects of lattice structures, electronic structures, ionic transport properties, the interface stability against Li and the thermodynamic stability. An oxygen-driven transition from two-dimensional to three-dimensional transport behaviour is found and the oxygen dopants play the role as a connector of 2D paths. Based on all these simulation results, hopefully our research can provide a new strategy for the modification of lithium thiophosphate solid electrolytes.
authors.affiliation: Beijing National Laboratory for Condensed Matter Physics, Institute of Physics, Chinese Academy of Sciences, Beijing 100190, China. rjxiao@iphy.ac.cn.
authors.forename: Xuelong
authors.initials: X
authors.lastname: Wang
authors.affiliation: Beijing National Laboratory for Condensed Matter Physics, Institute of Physics, Chinese Academy of Sciences, Beijing 100190, China. rjxiao@iphy.ac.cn.
authors.forename: Ruijuan
authors.initials: R
authors.lastname: Xiao
authors.affiliation: Beijing National Laboratory for Condensed Matter Physics, Institute of Physics, Chinese Academy of Sciences, Beijing 100190, China. rjxiao@iphy.ac.cn.
authors.forename: Hong
authors.initials: H
authors.lastname: Li
authors.affiliation: Beijing National Laboratory for Condensed Matter Physics, Institute of Physics, Chinese Academy of Sciences, Beijing 100190, China. rjxiao@iphy.ac.cn.
authors.forename: Liquan
authors.initials: L
authors.lastname: Chen