Rapid degradation of tetracycline hydrochloride by heterogeneous photocatalysis coupling persulfate oxidation with MIL-53(Fe) under visible light irradiation

J Hazard Mater. 2020 Jun 15:392:122315. doi: 10.1016/j.jhazmat.2020.122315. Epub 2020 Feb 15.

Abstract

This work demonstrates a facile route to assemble MIL-53(Fe) by solvothermal method. Sulfate radical-based advanced oxidation processes (SR-AOPs) coupling with photocatalysis based on MIL-53(Fe) were investigated under visible light. The catalytic effect of MIL-53(Fe) for the degradation of tetracycline hydrochloride (TC-HCl) was systematically studied, as well as the reusability of the catalyst and the effect of operating parameters. The results indicated that 99.7 % of TC (300 mg/L) could be degraded within 80 min in the SR-AOPs coupling with photocatalysis processes, as compared to 71.4 % for the SR-AOPs and only 17.1 % for the photocatalysis. The trapping experiments and electron spin-resonance spectroscopy (ESR) showed the photogenerated electrons of MIL-53(Fe) under visible light irritation were trapped by persulfate to generated sulfate radicals which effectively suppressed the recombination of photogenerated carriers. And also, the SO4- could be formed by the conversion between Fe (Ⅲ) and Fe (Ⅱ) in MIL-53(Fe). Moreover, OH and O2- generated by the reaction increased significantly due to the increase of SO4- which generated more OH and reduced photogenerated carrier recombination respectively. Thus, the degradation efficiency of TC-HCl was improved. Furthermore, the degradation pathway for TC-HCl was proposed using the theoretical calculations and liquid chromatography coupled with mass spectrometry.

Keywords: Advanced oxidation processes; Degradation pathway; MIL-53(Fe); Photocatalyst; Sulfate radical.

Publication types

  • Research Support, Non-U.S. Gov't

MeSH terms

  • Anti-Bacterial Agents / chemistry*
  • Catalysis
  • Iron / chemistry
  • Iron / radiation effects*
  • Light*
  • Metal-Organic Frameworks / chemistry
  • Metal-Organic Frameworks / radiation effects*
  • Oxidation-Reduction
  • Photochemical Processes
  • Sodium Compounds / chemistry
  • Sodium Compounds / radiation effects*
  • Sulfates / chemistry
  • Sulfates / radiation effects*
  • Tetracycline / chemistry*
  • Water Pollutants, Chemical / chemistry*

Substances

  • Anti-Bacterial Agents
  • Metal-Organic Frameworks
  • Sodium Compounds
  • Sulfates
  • Water Pollutants, Chemical
  • sulfate radical
  • Iron
  • Tetracycline
  • sodium persulfate