Efficient evolution of reactive oxygen species over the coordinated π-delocalization g-C3N4 with favorable charge transfer for sustainable pollutant elimination

Abstract

Reactive oxygen species (ROS) as efficient and green oxidants can be generated through various catalytic methods, which is important for environmental chemistry and chemical engineering. Here we construct an efficient photocatalytic system to evolve ROS for environmental purification. In the work, the coordinated g-C3N4 photocatalysts (Cu/C3N4) are designed by interacting N 2p lone electrons at vacancy site of tri-s-triazine polymer with 3d orbits of Cu2+, resulting in the extended π-delocalization structure of g-C3N4. Experimental and theoretical calculations confirm that the extended π-delocalization structure of Cu/C3N4 strengthens the light capturing capability from ultraviolet to near infrared light, favors the charge transfer from N 2p of C3-N to the linked C, and Cu atoms. As a result, the efficient evolution of ROS including O2− (13 μmol L−1 h−1), and H2O2 (550 μmol L−1 h−1) can be completed over Cu/C3N4 photocatalysts. Cu/C3N4 photocatalysts results in a highly efficient generation of ROS and also exhibited a sustainable removal efficiency for NO, and HCHO, which demonstrates a promising application in the field of environmental purification.