Li3BO3-Li3PO4 Composites for Efficient Buffer Layer of Sulphide-Based All-Solid-State Batteries

Abstract

All-solid-state batteries (ASSBs) based on sulphide electrolytes are promising next-generation energy storage systems because they are expected to have improved safety, increased volumetric energy density, and a wide operating temperature range. However, side reactions at the cathode/electrolyte interface deteriorate the electrochemical performance and limit the commercialization of ASSBs. Surface coating of the cathode is an efficient approach for overcoming this issue. In this study, new Li3BO3 (LBO)-Li3PO4 (LPO) composites were applied as coating materials for high-Ni cathodes (NCM). PO4-based materials (such as LPO) have been used as coating layers because of their good chemical stability in sulphide electrolytes. However, the ionic conductivity of LPO is slightly insufficient compared to those of generally used ternary oxides. The addition of LBO could compensate for the low ionic conductivity of LPO and may provide better protection against sulphide electrolytes owing to the effect of LBO, which has been used as a good coating material. As expected, the LBO-LPO composites (LBPO) NCM exhibited superior discharge capacity, rate capability, and cyclic performance compared to the pristine and LPO-coated NCMs. X-ray photoelectron spectroscopy (XPS) and energy-dispersive X-ray spectroscopy (EDS) analyses confirmed that the LBPO coating on the cathodes successfully suppressed the byproduct formation and an undesirable interfacial layer, which are attributed to interfacial side reactions. This result clearly shows the potential of the LBPO coating as an excellent buffer layer to stabilise the oxide cathode/sulphide electrolyte interface.