Synthesis of glass-ceramic Li2S-P2S5-based electrolyte for solid-state batteries

Abstract: In this project, solid sulphur based Li3PS4 electrolytes doped with Li4SiO4 were synthesised using two methods. In method A, a bought β-Li3PS4 electrolyte from Nei Corp was doped with 5 mole per cent Li4SiO4, resulting in a glass-ceramic electrolyte. In method B, the electrolyte was synthesised using 5Li4SiO4-95(75Li2S-25P2S5), resulting in a glassy material. In addition, a reference was synthesised using 75Li2S-25P2S5. Ball milling was the method of choice to dope the glass ceramic electrolyte and synthesise the glassy electrolyte. The dopant Li4SiO4 was synthesised using the chemicals SiO2 and Li2CO3. All samples were analysed using Raman, XPS, XRD, and EIS. In the end, it was found that doping the bought β-Li3PS4electrolyte with Li4SiO4 increased the ionic conductivity. While introducing Li4SiO4 to the glassy electrolyte lowered the ionic conductivity. The increase in ionic conductivity in the glass ceramic electrolyte was partly attributed to the increase in amorphous content, which happened when it was ball-milled and suppressed P-S-P bonds. The decrease in ionic conductivity that happened when doping the glassy material, is most likely caused by residual Li2S that seems unable to react due to the dopant.