Microwave Synthesis of Visible-Light-Activated g-C₃N₄/TiO₂ Photocatalysts

The preparation of visible-light-driven photocatalysts has become highly appealing for environmental remediation through simple, fast and green chemical methods. The current study reports the synthesis and characterization of graphitic carbon nitride/titanium dioxide (g-C₃N₄/TiO₂) heterostructures through a fast (1 h) and simple microwave-assisted approach. Different g-C₃N₄ amounts mixed with TiO₂ (15, 30 and 45 wt. %) were investigated for the photocatalytic degradation of a recalcitrant azo dye (methyl orange (MO)) under solar simulating light. X-ray diffraction (XRD) revealed the anatase TiO₂ phase for the pure material and all heterostructures produced. Scanning electron microscopy (SEM) showed that by increasing the amount of g-C₃N₄ in the synthesis, large TiO₂ aggregates composed of irregularly shaped particles were disintegrated and resulted in smaller ones, composing a film that covered the g-C₃N₄ nanosheets. Scanning transmission electron microscopy (STEM) analyses confirmed the existence of an effective interface between a g-C₃N₄ nanosheet and a TiO₂ nanocrystal. X-ray photoelectron spectroscopy (XPS) evidenced no chemical alterations to both g-C₃N₄ and TiO₂ at the heterostructure. The visible-light absorption shift was indicated by the red shift in the absorption onset through the ultraviolet-visible (UV-VIS) absorption spectra. The 30 wt. % of g-C₃N₄/TiO₂ heterostructure showed the best photocatalytic performance, with a MO dye degradation of 85% in 4 h, corresponding to an enhanced efficiency of almost 2 and 10 times greater than that of pure TiO₂ and g-C₃N₄ nanosheets, respectively. Superoxide radical species were found to be the most active radical species in the MO photodegradation process. The creation of a type-II heterostructure is highly suggested due to the negligible participation of hydroxyl radical species in the photodegradation process. The superior photocatalytic activity was attributed to the synergy of g-C₃N₄ and TiO₂ materials.