The rapid growth of the textile industry has led to the increasing generation of wastewater containing synthetic dyes such as methylene blue (MB), which are toxic, persistent, and resistant to natural degradation. In this study, TiO₂–layered double hydroxide (TiO₂–LDH) photocatalysts were synthesized using the coprecipitation method with an M²⁺/M³⁺ molar ratio of 3, followed by calcination at 300 °C. X-ray diffraction (XRD) analysis confirmed the presence of the anatase TiO₂ phase and characteristic LDH diffraction peaks, indicating the successful formation of the TiO₂–LDH composite. Brunauer–Emmett–Teller (BET) analysis revealed a specific surface area of 15.027 m² g⁻¹ with a hierarchical mesoporous–macroporous structure. The photocatalytic degradation performance was evaluated by varying the MB concentration (10 and 20 ppm), catalyst dosage (0.025, 0.05, and 0.10 g), solution pH (4, 7, and 10), reaction time (60, 90, and 120 min), and UV irradiation. The optimum degradation conditions were achieved at an MB concentration of 10 ppm, catalyst dosage of 0.10 g, pH 10, and a reaction time of 120 min under UV irradiation. Under these conditions, the TiO₂/MgAl photocatalyst exhibited the highest degradation efficiency of 95%, followed by TiO₂/MgZnAl (90%) and TiO₂/ZnAl (86%). The enhanced photocatalytic activity under alkaline conditions was attributed to the increased generation of highly reactive hydroxyl radicals (•OH), which accelerated the degradation of MB molecules. Based on the characterization results and photocatalytic performance, the TiO₂–LDH composites demonstrated excellent potential for the removal of methylene blue from aqueous solutions and represent a promising alternative photocatalytic material for wastewater treatment applications.
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