Efficient visible light driven degradation of antibiotic pollutants by oxygen-doped graphitic carbon nitride via the homogeneous supramolecular assembly of urea

Abstract

Graphitic carbon nitride (CN), as a non-metal material, has emerged as a promising photocatalyst to address environmental issues with the favorable band gap and chemical stability. 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 homogeneous supramolecular assembly was advantageous to the formation of uniform porous and oxygen-doped CN nanosheets. 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 functional 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.