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 e...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-C_(3)N_(4))by a facile one-step pyrolysis method and evaluated the photocatalytic efficiency of carbamazepine(CBZ).Under simulated solar irradiation,g-C_(3)N_(4) 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-C_(3)N_(4) 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)^(·-))and holes(h^(+))were the major active radicals.Electron paramagnetic resonance(EPR)further confirmed the presence of O_(2)^(·-),·OH,^(1)O_(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-C_(3)N_(4).The facile synthesis,superior efficiency,and versatility of g-C_(3)N_(4) make it a promising catalyst for application in tertiary wastewater treatment processes.展开更多
基金funding support through the project DP 170104330the support by Australian Research Council Future Fellowship(FT170100196).
文摘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-C_(3)N_(4))by a facile one-step pyrolysis method and evaluated the photocatalytic efficiency of carbamazepine(CBZ).Under simulated solar irradiation,g-C_(3)N_(4) 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-C_(3)N_(4) 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)^(·-))and holes(h^(+))were the major active radicals.Electron paramagnetic resonance(EPR)further confirmed the presence of O_(2)^(·-),·OH,^(1)O_(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-C_(3)N_(4).The facile synthesis,superior efficiency,and versatility of g-C_(3)N_(4) make it a promising catalyst for application in tertiary wastewater treatment processes.