Preparation of Amorphous Solid Electrolytes in The System Li2S-Al2S3-P2S5 by High-energy Ball-milling Methods

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Lithium-ion conducting solid electrolytes in the composition (100-x)Li3PS4·xLiAlS2 (mol %) were prepared by use of a high-energy ball-milling process at room temperature. Amorphous samples were obtained in the composition range of x = 0 to x = 13.1. In the samples with x ≥ 18.2, a crystalline Al2S3 phase was remained after the ball-milling for 35 h. The lithium ion conductivity at 298K of the obtained samples was increased with an increase in the compositional parameter x and attained the maximum (σ298K = 6.0 × 10-4Scm-1 at 298K) at x = 13.1. Measurement of DC polarization confirmed that the main carrier for the conduction of the samples was lithium ions. A laboratory-scale all-solid-state battery using the amorphous 86.9Li3PS4·13.1LiAlS2 (mol %) as solid electrolytes, Li4.4Si as anode, and TiS2 as cathode materials showed good discharge-charge cycle performance at room temperature.