Fabrication of a Perylene Tetracarboxylic Diimide–Graphitic Carbon Nitride Heterojunction Photocatalyst for Efficient Degradation of Aqueous Organic Pollutants

Abstract

Metal-free g-C₃N₄ is a promising candidate for the next-generation visible light-responsive photocatalyst; however, high recombination probability of the photogenerated charge carriers on g-C₃N₄ limits its photocatalytic activity. To further increase the intrinsic photocatalytic activity of g-C₃N₄, here, perylene tetracarboxylic diimide-g-C₃N₄ (PDI/GCN) heterojunctions are prepared by one-step imidization reaction between perylene tetracarboxylic dianhydride (PTCDA) and g-C₃N₄ in aqueous solution. By the combination of various testing results, it is confirmed that the surface hybridization of PTCDA and g-C₃N₄ in the PDI/GCN heterojunctions via O═C-N-C═O covalent bonds occurs at lower PTCDA-to-g-C₃N₄ weight percentage. By selecting p-nitrophenol (PNP) and levofloxacin (LEV) as the target organic pollutants, the visible-light photocatalytic performance of the PDI/GCN heterojunctions is studied. It shows that the PDI/GCN heterojunction prepared at a PTCDA-to-g-C₃N₄ weight percentage of 1% exhibits remarkably higher visible-light photocatalytic degradation and mineralization ability toward aqueous target pollutants as compared with g-C₃N₄ and Degussa P25 TiO₂. On the basis of the experimental results including photoelectrochemistry, indirect chemical probe, and electron spin resonance spectroscopy, it is verified that the surface hybridization in the heterojunctions is responsible for this enhanced photocatalytic activity via accelerating the migration and separation of the photogenerated charge carriers, causing to produce more active species like ^•O₂^-, h_VB⁺, and ^•OH for deep oxidation of PNP or LEV to CO₂ and inorganic anions.