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

Wu Yang; Peidong Hong; Dandan Yang; Ya Yang; Zijian Wu; Chao Xie; Junyong He; Kaisheng Zhang; Lingtao Kong; Jinhuai Liu

doi:10.1016/j.jcis.2021.03.168

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

J Colloid Interface Sci. 2021 Sep:597:56-65. doi: 10.1016/j.jcis.2021.03.168. Epub 2021 Apr 1.

Authors

Wu Yang¹, Peidong Hong², Dandan Yang², Ya Yang², Zijian Wu³, Chao Xie³, Junyong He³, Kaisheng Zhang⁴, Lingtao Kong⁵, Jinhuai Liu⁶

Affiliations

¹ Institutes of Physical Science and Information Technology, Anhui University, Hefei 230601, PR China; Environmental Materials and Pollution Control Laboratory, Institute of Solid State Physics, HFIPS, Chinese Academy of Sciences, Hefei 230031, PR China.
² Environmental Materials and Pollution Control Laboratory, Institute of Solid State Physics, HFIPS, Chinese Academy of Sciences, Hefei 230031, PR China; Department of Chemistry, University of Science and Technology of China, Hefei, Anhui 230026, PR China.
³ Environmental Materials and Pollution Control Laboratory, Institute of Solid State Physics, HFIPS, Chinese Academy of Sciences, Hefei 230031, PR China.
⁴ Environmental Materials and Pollution Control Laboratory, Institute of Solid State Physics, HFIPS, Chinese Academy of Sciences, Hefei 230031, PR China. Electronic address: kszhang@iim.ac.cn.
⁵ Environmental Materials and Pollution Control Laboratory, Institute of Solid State Physics, HFIPS, Chinese Academy of Sciences, Hefei 230031, PR China. Electronic address: ltkong@iim.ac.cn.
⁶ Institutes of Physical Science and Information Technology, Anhui University, Hefei 230601, PR China; Environmental Materials and Pollution Control Laboratory, Institute of Solid State Physics, HFIPS, Chinese Academy of Sciences, Hefei 230031, PR China. Electronic address: jhliu@iim.ac.cn.

PMID: 33862447
DOI: 10.1016/j.jcis.2021.03.168

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.

Keywords: Catalysis mechanism; Fenton-like reaction; Highly efficient catalyst; Single-atom iron; Sulfadiazine.