Metal-free carbon nitride with boosting photo-redox ability realized by the controlled carbon dopants

Abstract

Metal-free carbon nitride with controlled carbon dopants (ACCN) was synthesized by one-step copolymerization of dicyandiamide (DCD) and ammonium citrate (AC). The obtained ACCN possesses narrower band gap compared to pure graphitic carbon nitride (CN), contributing to broader utilization region of visible light. It exhibits downshifted conduction band and valence band potential with the increased addition of AC. Carbon atoms replace the bridging nitrogen atoms in the framework of ACCN during calcination process, which greatly increase its electrical conductivity and charge separation efficiency. In addition, nitrogen defects and some carbon species linked to the introduced carbon atoms are detected in ACCN. They can also serve as electrons sink to promote the separation of electron-hole pairs. As a consequence, ACCN possesses improved redox ability in the degradation of sulfamethazine (SM2) under visible light. The removal ratio by optimal ACCN achieves 81% in 60 min and its reaction apparent rate constant (0.0277 min−1) is 6.6 times higher than that of CN (0.0042 min−1). Furtherly, the mechanism and reaction process during the photocatalytic degradation are studied specifically. This work provides a facile and green strategy to prepare nonmetal modified CN with boosting photo-redox ability for pollutants treatment.