Characterization of solid-electrolyte/active-material composite particles with different surface morphologies for all-solid-state batteries

In all-solid-state lithium-ion batteries (ASS-LIBs), the electrode structure is an important factor that determines the battery performance; in particular, the formation of contact interface between the active material (AM) and solid electrolyte (SE) is an important issue associated with ASS-LIBs. Although we previously reported the formation of interfacial contacts between AM and SE by dry coating, the influence of the surface morphologies of composite particles on the performance of ASS-LIB was not revealed. In this study, we investigated the effects of the surface morphologies of composite particles on the performance of ASS-LIB. The surface morphologies of composite particles changed from "discrete" to "continuous" as the dry coating progressed. The cell prepared with composite particles showed higher ionic conductivity due to well-percolated ionic path than that prepared with simple mixture. Comparing the composite particles with different surface morphologies, the cell prepared with discrete-coating particles showed lower internal resistance due to higher ionic/electrical conductivity than that prepared with continuous-coating particles. Further, the cells prepared with discrete- and continuous-coating particles showed the highest charge and discharge capabilities, respectively. The results suggest that the contact areas of AM-SE and AM-AM were critical structural factors for the discharge and charge rate capability, respectively.