The efficient degradation of high concentration phenol by Nitrogen-doped perovskite La2CuO4 via catalytic wet air oxidation: Experimental study and DFT calculation

Herein, N-doped perovskite La2CuO4 (LCO) (N-LCO(M)) was fabricated by sol–gel rapid calcination method using melamine (M) as N source/ligand, and applied for the catalytic wet air oxidation (CWAO) to degrade high-concentration phenol-containing simulated wastewater. The experimental results exhibited that N-LCO(M) illustrated enhanced phenol degradation efficiency. Thereinto, 87.9% COD degradation efficiency was achieved in simulated wastewater containing 8000 mg/L phenol, while for undoped LCO prepared with citric acid (CA) as ligand (LCO(CA)) was only 43.8%. The systematic characterizations and density functional theory (DFT) calculations were utilized to verify the above results. The results revealed that N doping favored the formation of more oxygen vacancies (*) and facilitated the charge transfer between Cu and O. More oxygen vacancies (*) reinforced the ability of N-LCO(M) to adsorb O2 to form reactive oxygen species (O*), and meanwhile, the charge transfer between Cu and O was manifested as the redox cycle of the catalytic active metal Cu2+/Cu1+. The redox cycle also promoted the formation of O2− and HO, making the more exhaustive degradation of phenol. This successfully proved that N doping was core to improving the activity and stability of N-LCO(M). Moreover, a possible mechanism of phenol degradation was proposed based on the experimental results and DFT calculations. Eventually, the toxicity of the intermediate products was further evaluated by quantitative structure–activity relationship (QSAR) analysis, showing the significantly reduced toxicity of the intermediate products. Overall, the proposed CWAO technique is a green and promising wastewater treatment method.