Efficient photocatalytic destruction of recalcitrant micropollutants using graphitic carbon nitride under simulated sunlight irradiation

The ubiquity of micropollutants (MPs) in aquatic environments has attracted increasing concern for public health and ecological security. Compared to conventional biological treatment, photocatalytic processes show more efficiency in degrading MPs, but they require expensive materials and complicated synthesis processes. This study developed an economic photocatalytic process to degrade micropollutants. We synthesized urea-based graphitic carbon nitride (g-C3N4) by a facile one-step pyrolysis method and evaluated the photocatalytic efficiency of carbamazepine (CBZ). Under simulated solar irradiation, g-C3N4 could achieve 100% removal efficiency of 0.1 mg/L CBZ in spiked wastewater effluent within 15 min, and 86.5% removal efficiency in wastewater influent after 20 min of irradiation. The porous structure of g-C3N4 promoted effective charge separation and mass transport of CBZ near the catalyst surface, enabling a high kinetic rate (0.3662 min (-1)). Reactive oxygen species trapping experiments revealed that superoxide radicals (O-2(center dot-)) and holes (h(+)) were the major active radicals. Electron paramagnetic resonance (EPR) further confirmed the presence of O-2(center dot-), (OH)-O-center dot, O-1(2) and holes. The pH, light intensity and initial CBZ concentration were found to have significant impacts on the removal efficiency of CBZ. Possible reaction intermediates were identified and the degradation pathway was proposed. Multiple MPs were selected to further demonstrate photocatalytic efficiency of g-C3N4. The facile synthesis, superior efficiency, and versatility of g-C3N4 make it a promising catalyst for application in tertiary wastewater treatment processes. (C) 2021 The Authors. Published by Elsevier B.V. on behalf of Chinese Society for Environmental Sciences, Harbin Institute of Technology, Chinese Research Academy of Environmental Sciences.

Automated summary

This study developed an economic photocatalytic process to degrade micropollutants using a synthesized urea-based graphitic carbon nitride (g-C3N4). The g-C3N4 exhibited high efficiency in degrading carbamazepine (CBZ) under simulated solar irradiation, with significant impacts of pH, light intensity, and initial CBZ concentration on removal efficiency. The presence of superoxide radicals and holes as major active radicals was confirmed, suggesting g-C3N4's potential as a promising catalyst for tertiary wastewater treatment processes.