Abstract
Surface coating of cathodes is an essential process for all-solid-state batteries (ASSBs) based on sulfide electrolytes as it efficiently suppresses interfacial reactions between oxide cathodes and sulfide electrolytes. Based on computational calculations, Li3PO4 has been suggested as a promising coating material because of its higher stability with sulfides and its optimal ionic conductivity. However, it has hardly been applied to the coating of ASSBs due to the absence of a suitable coating process, including the selection of source material that is compatible with ASSBs. In this study, polyphosphoric acid (PPA) and (NH4)2HPO4 were used as source materials for preparing a Li3PO4 coating for ASSBs, and the properties of the coating layer and coated cathodes were compared. The Li3PO4 layer fabricated using the (NH4)2HPO4 source was rough and inhomogeneous, which is not suitable for the protection of the cathodes. Moreover, the water-based coating solution with the (NH4)2HPO4 source can deteriorate the electrochemical performance of high-Ni cathodes that are vulnerable to water. In contrast, when an alcohol-based solvent was used, the PPA source enabled the formation of a thin and homogeneous coating layer on the cathode surface. As a consequence, the ASSBs containing the Li3PO4-coated cathode prepared by the PPA source exhibited significantly enhanced discharge and rate capabilities compared to ASSBs containing a pristine cathode or Li3PO4-coated cathode prepared by the (NH4)2HPO4 source.
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