Exploring interfacial stability for Zr-doped sulfide solid electrolyte with first-principle calculation

First-principles calculations are employed to investigate the interfacial properties on the Zr-doped sulfide solid electrolytes. Theoretical calculation results show that the PS₄ tetrahedral structure near the Li/Li₃PS₄ interface is severely damaged, whereas the Zr-doped sulfide solid electrolyte interface structure has a slight deformation. The Li ions migration energy barrier on the Zr-doped sulfide solid electrolyte interface is relatively lower than that on the Li/Li₃PS₄. Moreover, the stress-strain analysis indicates that the Li/Li₃PS₄ interface structure experiences a maximum strain of only 6 %, while the Zr-doped sulfide solid electrolyte interface structure experiences a maximum strain of 10 %. This may be attributed to the ability of Zr doping to prevent S²⁻ diffusion into the lithium metal anode and stabilize the Li ion transport skeleton. Therefore, Zr doping can improve the interface structure stability. This study will provide a useful perspective for designing high performance of solid electrolytes for the application of all-solid-state batteries.