MgO-supported CuO with encapsulated structure for enhanced peroxymonosulfate activation to remove thiamphenicol

Abstract

Copper-base catalysts with high load content of CuO were commonly utilized to activate peroxymonosulfate (PMS) for removal of contaminants but limited catalytic efficiency and increased risk of copper ion leaching restricted their use. In this paper, Cu-Mg mixed metal oxides with highly dispersed minute quantities of CuO were successfully prepared by one-pot synthesis for efficiently activating PMS to remove thiamphenicol (TAP), which was economical and environmentally friendly. The catalytic activities of catalysts with different molar ratios of Cu and Mg for PMS and their characteristics were evaluated, illustrating the optimal molar ratio of Cu and Mg (1:15, named CuMg-MMO) in the catalyst. For the CuMg-MMO catalyst, MgO widely dispersed and wrapped CuO nanoparticles, minimized the copper ion leaching and promoted the generation of Cu-OH complex and non-radical species. In the CuMg-MMO/PMS system, the influence factors for TAP degradation were analyzed, including different systems, catalyst dosages, PMS concentrations, temperatures, initial pH values, TAP concentrations, anions (NO3-, HCO3-, Cl-, HPO42- and H2PO4-) and natural organic matter (NOM) concentrations. Under the optimal conditions (i.e., [catalyst]: 75 mg/L, [PMS]: 0.3 mM, temperature: 30 °C and initial pH: 6.5), TAP removal efficiency obtained by this system was 99.9%. SO4·-, ·O2- and 1O2 played more important roles than HO· in TAP degradation. Four successive repeated experiments indicated that CuMg-MMO possessed good reusability and stability. PMS decomposition, mineralization of TAP, the activation mechanism of PMS and possible degradation pathways of TAP were analyzed.