Manufacturing Process Optimization of Oxide-Based Multilayer Ceramic Batteries Using Multilayer Ceramic Processing Technologies

Multilayer ceramic batteries (MLCBs) have attracted increasing attention as compact all-solid-state energy-storage devices that can be manufactured using multilayer ceramic processing technologies. In this study, an MLCC-compatible fabrication process for oxide-based MLCBs was developed using Li₁₊ₓAlₓTi₂₋ₓ(PO₄)₃ (LATP) solid electrolytes, Li₃V₂(PO₄)₃ (LVP) cathodes, and Cu current collectors. Commercial LATP powders were evaluated in terms of particle-size distribution, phase purity, thermal stability, and ionic conductivity. The selected LATP powder was subsequently employed for tape-cast green-sheet fabrication, and the effects of polyvinyl butyral (PVB) binder content on slurry rheology and sheet microstructure were investigated. An optimized binder composition containing 11 wt% PVB (BM-2/BH-3 = 3:7) provided improved processability and microstructural uniformity. Drying conditions during sequential electrode printing were also optimized to suppress sheet warpage and improve multilayer registration. Thermogravimetric and differential thermal analyses (TG–DTA) were used to establish an optimized two-step debinding and co-firing process under a controlled reducing atmosphere. The resulting multilayer structures exhibited uniform densification without significant blistering, delamination, or interfacial defects. Charge–discharge measurements confirmed that electrochemical functionality was retained after the complete manufacturing process, yielding a discharge capacity of approximately 2.5–2.7 μAh.