Novel Visible Light-Driven Photocatalytic Chlorine Activation Process for Carbamazepine Degradation in Drinking Water

Photolysis of free chlorine (HOCl/ClO-) is an advanced oxidation process (AOP) to produce hydroxyl (HO center dot) and other radicals for refractory micropollutant degradation. However, HOCl/ClO- is only conducive to activation and production of radicals by ultraviolet (UV) light. For the first time, we show the use of visible light (>400 nm) to produce HO center dot and ClO center dot, through use of graphitic carbon nitride (g-C3N4) and photogenerated h(vb)(+), e(cb)(-), and O-2(center dot-) in the presence of HOCl/ClO-, which was termed visible light g-C3N4-enabled chlorine AOP (VgC-AOP). The VgC-AOP increased the pseudo first-order degradation rate constant of a model micropollutant, carbamazepine, by 16 and 7 times higher than that without g-C3N4 and HOCl/ClO-, respectively, and remained active over multiple use cycles. Effects of water quality [pH, alkalinity, Cu(II), and natural organic matter (NOM)] and the operational conditions (g-C3N4 and HOCl/ClO- concentrations, irradiation wavelength, and dose) were investigated. Of particular significance is its superior performance in the presence of NOM, which absorbs less light at visible light wavelengths and scavenges less surface-bonded reactive species, compared against UV/TiO2 or UV/chlorine AOPs. The VgC-AOP is practically relevant, feasible, and easily implementable and it expands the potential types of light sources (e.g., LEDs and solar light).