Synthesis of Sb-doped Li10P3S12I solid electrolyte and their electrochemical performance in solid-state batteries

Abstract

The glass-ceramic Li10P3S12I solid electrolyte exhibited moderate ionic conductivity of ∼3 mS cm−1, but it shows low interface stability with lithium, poor moisture stability, and the electrochemical performance is not well established with respect to lithium. In this work, we enhance the ionic conductivity, interface stability, and air stability using Sb-substitution in Li10P3S12I glass-ceramic solid electrolyte using a high-energy ball milling process followed by a low heat treatment process. The ionic conductivity analysis reveals that the prepared Li10.1P2.95Sb0.05S12I glass ceramic composition shows a higher ionic conductivity of 5.9 mS cm−1 at 25 °C than Li10.1P2.95Sb0.05S12I (5.06 mS cm−1). The Li10.1P2.95Sb0.05S12I glass ceramic symmetric cell exhibits a better critical current density of 1 mA cm−2 than bare (0.7 mA cm−2). Also, it demonstrates better DC cyclability at 0.25 mA cm−2 without internal short circuits after 80 cycles. The Sb-substitution not only enhanced the ionic conductivity, also increased the moisture stability according to HSAB theory. The lithium solid-state battery is constructed using the Li10.1P2.95Sb0.05S12I electrolyte that demonstrates a high discharge capacity of 146 mAh g−1 at 0.1C rate than bare electrolyte (126 mAh g−1).