Regulation Mechanism of Aluminum Concentration on the Structure, Morphology, and Hydrogen Barrier Performance of ZrO₂/Al₂O₃-CeO₂ Composite Coatings

To address the inherent drawbacks of micro-arc oxidation (MAO), this study employed MAO combined with sol–gel processing to fabricate ZrO₂/Al₂O₃-CeO₂ composite coatings on ZrH_1.8 surfaces, aiming to solve the hydrogen evolution problem of zirconium hydride (ZrH_1.8) materials in high-temperature environments. By adjusting the aluminum concentration in the sol (0.1~0.5 mol/L), a series of composite thin films were prepared on the ZrH_1.8 surface using MAO combined with dip-coating, and their surface morphology and phase composition were characterized. The microstructure, morphology, and hydrogen barrier performance of the thin films were systematically analyzed using scanning electron microscopy (SEM), XRD, laser confocal microscopy, and quadrupole mass spectrometry. The results showed that the composite coating had a low surface porosity, with a maximum hydrogen permeation reduction factor (PRF) of 18.1. When the aluminum concentration was 0.4 mol/L, the relative content of tetragonal ZrO₂ (T-ZrO₂) reached 13.88%, the surface porosity was as low as 4.87%, and the initial temperature of hydrogen loss was increased to 730 °C. Mechanism analysis indicated that CeO₂ may stabilize the tetragonal phase (T-ZrO₂) of ZrO₂ through solid solution effects and inhibit the phase transformation to monoclinic phase (M-ZrO₂), thereby reducing cracks caused by volume expansion. Meanwhile, the synergistic effect of the MAO densified layer and the sol–gel sealed porous layer significantly reduced the coating porosity and blocked hydrogen diffusion paths, thus achieving excellent hydrogen barrier performance under high-temperature conditions.