Enhanced Fenton-like degradation of sulfadiazine by single atom iron materials fixed on nitrogen-doped porous carbon.

ABSTRACT

The use of single-atom iron catalysts in heterogeneous Fenton-like reactions has demonstrated tremendous potential for antibiotic wastewater treatment. In this study, single-atom iron fixed on nitrogen-doped porous carbon materials (Fe-ISAs@CN) was synthesised using a metal organic framework (MOF) as a precursor. Fe-ISAs@CN was applied as a heterogeneous Fenton catalyst to activate H2O2 for the degradation of sulfadiazine (SDZ) in an aqueous solution. The physical and chemical properties of Fe-ISAs@CN were characterised by scanning electron microscopy (SEM), transmission electron microscope (TEM), high-angle annular dark-field scanning transmission electron microscopy (HAADF-STEM), X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), and rotating disk electrode (RDE) measurements. The results of our degradation experiments indicated that Fe-ISAs@CN exhibited remarkable activity and stability for the degradation of SDZ over a wide pH range; even after five cycles, Fe-ISAs@CN retained a high catalytic efficiency (>80%). The 5,5-dimethyl-1-oxaporphyrin-n-oxide (DMPO)-X signal captured by electron paramagnetic resonance (EPR) spectroscopy indicated that a large amount of hydroxyl radicals (OH) was produced in the reaction system. Quench tests indicated that the OH was the main active substance in the degradation of SDZ. The degradation products of the reaction were analysed by High Performance Liquid Chromatography-Mass Spectrometry (HPLC-MS), and possible degradation pathways for the SDZ degradation were proposed.