Efficient degradation of tetracycline in wide pH range using MgNCN/MgO nanocomposites as novel H₂O₂ activator

Currently existing Fenton-like catalysts were limited in wastewater treatment owing to their potential transition-metal poisoning, narrow applicable pH range and high dependence on external energy excitation. In this work, the MgNCN/MgO nanocomposites were firstly synthesized by a facile one-pot calcination of melamine and basic magnesium carbonate, and used as novel H₂O₂ activator for antibiotic removal. It was found that the MgNCN/MgO composite calcined at 550°C with the mass ratio of melamine to basic magnesium carbonate at 2:1, exhibited an excellent catalytic ability to tetracycline (TC) degradation in a wide pH range of 4-10 without any external energy input. More than 90% of TC (100 mL, 50 mg/L) could be degraded within 30 min by 10 mg of the nanocomposite in the presence of 0.2 mL of 30 wt% H₂O₂. Based on the experimental results, it was concluded that the Mg-N coordination between MgNCN and MgO in MgNCN/MgO nanocomposites activated H₂O₂ to produce primary singlet oxygen (¹O₂) and minor hydroxyl radicals (·OH), responding for TC degradation. In addition, the degradation pathways of TC were deduced by determining the generated intermediates during the degradation process. This work provided a novel idea for designing transition-metal-free catalysts for nonradical activation of H₂O₂ in the absence of external energy excitation.