Mathematical Model-Assisted Ultrasonic Spray Coating for Scalable Production of Large-Sized Solid Oxide...

Thin solid oxide films are crucial for developing high-performance solid oxide-based electrochemical devices aimed at decarbonizing the global energy system. Among various methods, ultrasonic spray coating (USC) can provide the throughput, scalability, quality consistency, roll-to-roll compatibility, and low material waste necessary for scalable production of large-sized solid oxide electrochemical cells. However, due to the large number of USC parameters, systematic parameter optimization is required to ensure optimal settings. However, the optimizations in previous literature are either not discussed or not systematic, facile, and practical for scalable production of thin oxide films. In this regard, we propose an USC optimization process assisted with mathematical models. Using this method, we obtained optimal settings for producing high-quality, uniform 4 × 4 cm² oxygen electrode films with a consistent thickness of ∼27 μm in 1 min in a facile and systematic way. The quality of the films is evaluated at both micrometer and centimeter scales and meets desirable thickness and uniformity criteria. To validate the performance of USC-fabricated electrolytes and oxygen electrodes, we employ protonic ceramic electrochemical cells, which achieve a peak power density of 0.88 W cm^-2 in the fuel cell mode and a current density of 1.36 A cm^-2 at 1.3 V in the electrolysis mode, with minimal degradation over a period of 200 h. These results demonstrate the potential of USC as a promising technology for scalable production of large-sized solid oxide electrochemical cells.