Visible-light-driven photocatalytic removal of antibiotics by newly designed C3N4@MnFe2O4-graphene nanocomposites

J Hazard Mater. 2017 Aug 15:336:81-92. doi: 10.1016/j.jhazmat.2017.04.012. Epub 2017 Apr 6.

Abstract

Newly designed magnetic g-C3N4/MnFe2O4/graphene (C3N4@MnFe2O4-G) composites with enhanced photocatalytic activity were successfully synthesized. The photocatalytic behavior of C3N4@MnFe2O4-G was assessed in photo Fenton-like degradation of antibiotic pollutants, including metronidazole, amoxicillin, tetracycline and ciprofloxacin, using persulfate (S2O82-) as an oxidant under visible light illumination. The C3N4@MnFe2O4-G composites show a superior catalytic activity with 94.5% removal of metronidazole that was almost 3.5 times as high as that of the pure g-C3N4, which could be attributed to the synergistic promoting effect of the favorable adsorptivity, enhanced light absorption intensity, high migration efficiency of charge carriers and longer lifetime of separated electron-hole pairs derived from the formation of the heterojunction between the g-C3N4 and MnFe2O4. Moreover, the self-redox properties of iron and manganese atoms in MnFe2O4 induced by S2O82- were particularly beneficial for the generation of SO4-. The quenching tests and electron spin resonance (ESR) display that h+, O2-, SO4- and OH are responsible for the antibiotics decomposition. The heterogeneous photocatalyst could be easily recovered by an extra magnetic field and reused several times without any obvious deterioration in catalytic activity. According to the investigation of active species and identified intermediates, the possible photocatalytic mechanism and reaction pathways have been proposed.

Keywords: Antibiotic pollutants; MnFe(2)O(4); Persulfate; Synergistic promoting effect; g-C(3)N(4).

MeSH terms

  • Adsorption
  • Anti-Bacterial Agents / isolation & purification*
  • Catalysis
  • Electron Spin Resonance Spectroscopy
  • Ferric Compounds / chemistry*
  • Light
  • Manganese Compounds / chemistry*
  • Microscopy, Electron, Scanning
  • Microscopy, Electron, Transmission
  • Nanocomposites / chemistry*
  • Nitriles / chemistry*
  • Oxidation-Reduction
  • Photolysis*
  • Spectrophotometry, Ultraviolet
  • Spectroscopy, Fourier Transform Infrared
  • Water Pollutants, Chemical / isolation & purification*
  • Water Purification / methods*
  • X-Ray Diffraction

Substances

  • Anti-Bacterial Agents
  • Ferric Compounds
  • Manganese Compounds
  • Nitriles
  • Water Pollutants, Chemical
  • manganese ferrite
  • cyanogen