Interfacial architecture for extra Li+ storage in all-solid-state lithium batteries

Abstract

The performance of nanocomposite electrodes prepared by controlled ball-milling of TiS2 and a Li2S-P2S5 solid electrolyte (SE) for all-solid-state lithium batteries is investigated, focusing on the evolution of the microstructure. Compared to the manually mixed electrodes, the ball-milled electrodes exhibit abnormally increased first-charge capacities of 416 mA h g-1and 837 mA h g-1 in the voltage ranges 1.5-3.0 V and 1.0-3.0 V, respectively, at 50 mA g-1 and 30°C. The ball-milled electrodes also show excellent capacity retention of 95% in the 1.5-3.0 V range after 60 cycles as compared to the manually mixed electrodes. More importantly, a variety of characterization techniques show that the origin of the extra Li+ storage is associated with an amorphous Li-Ti-P-S phase formed during the controlled ball-milling process.