Efficient Visible Light Driven Degradation of Antibiotic Pollutants by Oxygen-Doped Porous Graphitic Carbon Nitride Nanosheets Via the Homogeneous Supramolecular Assembly of Urea

Abstract

The porous oxygen-doped CN nanosheets (CNO) were synthesized by an ecofriendly and efficient self-assembled approach using a sole urea as the precursor. The CNO photocatalysts were derived from the hydrogen-bonded cyanuric acid-urea supramolecular complex, which were obtained by pretreatment of urea at high temperature and pressure. The formation process of the supramolecular intermediate and the CNO nanosheets were investigated. Moreover, doping amount of O in CNO could be controlled by the time of the high-pressure thermal polymerization of urea. The characterization results shown that the O atoms were successfully doped into the framework of CN by substitution the N atoms to form the C-O structures. The obtained CNO photocatalysts demonstrated the excellent visible-light photocatalytic performances for sulfamerazine (SMR) degradation, which was ascribed to synergistic interaction of porous structure and O doping. The degradation intermediates of SMR were identified and the degradation pathway were also proposed. Furthermore, density function theory (DFT) calculations proved that O doping changed the electronic structure of CN, resulting in more easier to activate O₂. This work provides a novel perceptive for the development of high-performance nonmetal photocatalysts by using the homogeneous supramolecular assembly, which exhibits great potential in the environmental treatment.

Keywords: oxygen-doped, porous nanosheets, supramolecular complex, visible light photocatalysis, sulfamerazine, density functional theory