This work is focused on the photocatalytic activities of undoped ZnO, Co (1%) doped ZnO (CZO) and In (1%) doped ZnO (IZO) thin films grown on flexible PEI (Polyetherimide) substrate by spray pyrolysis. The photodegradation of crystal violet dye was investigated under UV and sunlight irradiations. Doping and excitation energy effects on photocatalytic efficiencies are discussed. All ZnO thin films show high photocatalytic efficiency up to 80% under either UV or sunlight irradiations for 210 min. However, CZO has the higher photocatalytic performance under UV irradiation. While, the photodegradation efficiency of IZO was enhanced under sunlight irradiation due to the narrowing of its optical gap. These results are discussed based on structural, morphological and optical investigations. The photocatalytic stability of ZnO films was studied as well. So, after three photocatalysis cycles, all ZnO thin films still effective. The obtained results are promising for the use of doped ZnO/PEI as talented photocatalysts for applications in large surfaces with various geometries for photodegradation of hazardous pollutants.

The development of photoactive systems to solve serious environmental problems is a key objective of researchers and remains a real challenge. Herein, n–p heterojunction ZnO-based composites were developed to achieve better photocatalytic performance in methylene blue (MB) degradation under natural solar irradiation. The hydrothermal technique was used to synthesize zinc oxide (ZnO)/metal oxide (MO) composites, with a molar ratio of 1 : 1 (MO = Mn₃O₄; Fe₃O₄; CuO; NiO). Various characterization techniques were used for the analysis of the structural, morphological and optical properties. X-ray diffraction (XRD), Scanning Electron Microscopy (SEM), Energy Dispersive X-ray Spectroscopy (EDX) Diffuse Reflectance Spectroscopy analysis (DRS), and Diffuse Reflectance Spectroscopy analysis (DRS) validated the presence of two phases for each sample, excluding any impurities. Indeed, the ZnO structure was not affected by the coupling with MO, confirming that MO was well dispersed on the surface of the ZnO crystalline lattice for each composite. Eventually, the photocatalytic performance evaluation test of the synthesized photocatalysts was carried out on aqueous MB solution. According to the results, the ZnO/Fe₃O₄ nano-catalyst showed the best photodegradation efficiency. This result suggests that the formation of Fe₃O₄/ZnO as a p/n heterojunction reduces the recombination of photo-generated electron/hole pairs and broadens the solar spectral response range, resulting in significant photocatalytic efficiency. Meanwhile, the possible mechanism for degradation of the MB was discussed.