Microstructural Evolution and Enhanced Macroscopic Properties of La-Doped TiO₂-SiO₂ Composite Films Under Gradient Annealing

In this study, La-doped TiO₂-SiO₂ composite films were deposited on glass substrates by radio-frequency magnetron sputtering. The evolution of microstructure and macroscopic properties was systematically investigated across an annealing temperature range of 350–650 °C. The results show that the La-doped TiO₂-SiO₂ composite structure effectively suppresses abnormal grain growth and delays the anatase-to-rutile phase transition, thereby improving the films’ high-temperature structural stability. Notably, the composite film annealed at 550 °C (LS-550) exhibits the highest anatase crystallinity and forms a dense, smooth (RMS = 1.37 nm), crack-free nanocrystalline network. In terms of wettability, the improved hydrophilicity is attributed to the combined effects of La incorporation and hydrophilic silanol (Si-OH) groups in the amorphous SiO₂ phase. As a result, the water contact angle of the LS-550 film decreases dramatically to 28.0°, indicating excellent hydrophilicity. Moreover, the LS-550 film demonstrates an optimal photocatalytic degradation efficiency of approximately 76% for methylene blue, significantly outperforming the pure TiO₂ film. Furthermore, the enhanced mechanical performance is associated with the combined effects of the SiO₂-containing amorphous phase and the finer microstructure induced by La incorporation. Consequently, the critical load (Lc) of the LS-550 film reaches 75.64 mN, significantly exceeding that of the pure TiO₂ film annealed at the same temperature (61.25 mN). In summary, the composite film annealed at 550 °C concurrently achieves high crystallographic thermal stability, robust interfacial mechanical durability, excellent surface hydrophilicity, and enhanced photocatalytic activity, thereby offering practical guidance for developing TiO₂-based coatings with self-cleaning potential for high-rise building curtain walls.