Visible light-driven NH2Cl activation by g-C3N4 photocatalysis producing reactive nitrogen species to degrade bisphenol A

Abstract

The photolysis of monochloramine (NH₂Cl), a widely used disinfectant, under UVC irradiation produces different radicals for the micropollutant degradation. For the first time, this study demonstrates the degradation of bisphenol A (BPA) via the NH₂Cl activation by graphitic carbon nitride (g-C₃N₄) photocatalysis using visible light-LEDs at 420 nm, termed as the Vis₄₂₀/g-C₃N₄/NH₂Cl process. The process produces •NH₂, •NH₂OO, •NO and •NO₂ via the e_CB^-- and O₂^•--induced activation pathways and •NHCl and NHClOO• via the h_VB⁺-induced activation pathway. The produced reactive nitrogen species (RNS) enhanced 100% of the BPA degradation compared with the Vis₄₂₀/g-C₃N₄. Density functional theory calculations confirmed the proposed NH₂Cl activation pathways and further demonstrated that e_CB^-/O₂^•- and h_VB⁺ induced the cleavage of N-Cl and N-H bonds in NH₂Cl, respectively. The process converted 73.5% of the decomposed NH₂Cl to nitrogen-containing gas, compared with that of approximately 20% in the UVC/NH₂Cl process, leaving much less ammonia, nitrite and nitrate in water. Among different operating conditions and water matrices tested, of particular significance is natural organic matter of 5 mgDOC/L only reduced 13.1% of the BPA degradation compared against that of at least 46% reduction in the UVC/NH₂Cl process. Only 0.017-0.161 µg/L of disinfection byproducts were produced, two orders of magnitudes lower than that in the UVC/chlorine and UVC/NH₂Cl processes. The combined use of visible light-LEDs, g-C₃N₄ and NH₂Cl significantly improves the micropollutant degradation and reduces the energy consumption and byproduct formation of the NH₂Cl-based AOP.

Keywords: Emerging environmental risk; NH(2)Cl activation; Photocatalysis; Reactive nitrogen species; g-C(3)N(4).