Realizing the synergistic effect of electronic modulation over graphitic carbon nitride for highly efficient photodegradation of bisphenol A and 2-mercaptobenzothiazole: Mechanism, degradation pathway and density functional theory calculation

Abstract

Here, we successfully synthesized a brown carbon nitride (CY-C₃N₄) co-modified with oxygen bridge and porous defects via a universal acylation method. Excitingly, density functional theory (DFT) calculation shows that the introduction of oxygen bridges in the calcination polymerization process can adjust the electronic structure and energy band position of the new material. Further, the results of elemental analysis and X-ray photoemission spectroscopy test indicate that the oxygen bridge structure was successfully introduced into the skeleton of carbon nitride. The results show that 0.1CY-C₃N₄ can remove bisphenol A (BPA) and 2-mercaptobenzothiazole (MBT) with a removal rate of approximately 99% in 90 min and 20 min, respectively. Its degradation rate is 17.94 times and 3.85 times faster than that the original carbon nitride, respectively. Further, through HPLC-MS analysis, the intermediate products of the reaction process were analyzed in depth to propose a possible photocatalytic degradation route. Free radical capturing test and ESR spectroscopy indicate that the formative hydroxyl radical (OH), superoxide radical (O₂^-), singlet oxygen (¹O₂) and hole (h⁺) all play a key role in the photodegradation. This study provides a new way to synthesize brown carbon nitrides with oxygen bridges and porous defects for environmental applications.

Keywords: 2-mercaptobenzothiazole; Bisphenol A; Brown carbon nitride; Degradation; Photocatalysis.