Search

In this study, we assembled a bulk-type all-solid-state battery comprised of a TiS2 positive electrode, LiBH4 electrolyte, and Li negative electrode. Our battery retained high capacity over 300 discharge–charge cycles when operated at 393 K and 0.2 C. The second discharge capacity was as high as 205 mAh g–1, corresponding to a TiS2 utilization ratio of 85%. The 300th discharge capacity remained as high as 180 mAh g–1 with nearly 100% Coulombic efficiency from the second cycle. Negligible impact of the exposure of LiBH4 to atmospheric-pressure oxygen on battery cycle life was also confirmed. To investigate the origin of the cycle durability for this bulk-type all-solid-state TiS2/Li battery, electrochemical measurements, thermogravimetry coupled with gas composition analysis, powder X-ray diffraction measurements, and first-principles molecular dynamics simulations were carried out. Chemical and/or electrochemical oxidation of LiBH4 occurred at the TiS2 surface at the battery operating temperature of 393 K...

Stable battery operation of a bulk-type all-solid-state lithium-sulfur battery was demonstrated by using a LiBH4 electrolyte. The electrochemical activity of insulating elemental sulfur as the positive electrode was enhanced by the mutual dispersion of elemental sulfur and carbon in the composite powders. Subsequently, a tight interface between the sulfur-carbon composite and the LiBH4 powders was manifested only by cold-pressing owing to the highly deformable nature of the LiBH4 electrolyte. The high reducing ability of LiBH4 allows using the use of a Li negative electrode that enhances the energy density. The results demonstrate the interface modification of insulating sulfur and the architecture of an all-solid-state Li-S battery configuration with high energy density.