4.7 Article

Highly efficient and stable FeIIFeIII LDH carbon felt cathode for removal of pharmaceutical ofloxacin at neutral pH

Journal

JOURNAL OF HAZARDOUS MATERIALS
Volume 393, Issue -, Pages -

Publisher

ELSEVIER
DOI: 10.1016/j.jhazmat.2020.122513

Keywords

Surface catalysis; Heterogeneous electro-Fenton; (FeFeIII)-Fe-II LDH-CF; Ofloxacin; Reusability

Funding

  1. National Natural Science Foundation of China [21773129, 21811530274, 21976096, 21273120]
  2. National Key Research and Development Program of China [2016YFC0400706]
  3. Tianjin Science and Technology Program [19PTZWHZ00050]
  4. Tianjin Development Program for Innovation and Entrepreneurship, National High-level Foreign Experts Project [G20190002011]
  5. 111 program, Ministry of Education of the People's Republic of China [T2017002]
  6. Fundamental Research Funds for the Central Universities, Nankai University

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The traditional electro-Fenton (EF) has been facing major challenges including narrow suitable range of pH and non-reusability of catalyst. To overcome these drawbacks we synthesized (FeFeIII)-Fe-II-layered double hydroxide modified carbon felt ((FeFeIII)-Fe-II LDH-CF) cathode via in situ solvo-thermal process. Chemical composition and electrochemical characterization of (FeFeIII)-Fe-II LDH-CF were tested and analyzed. The apparent rate constant of decay kinetics of ofloxacin (OFC) with (FeFeIII)-Fe-II LDH-CF (0.18 min(-1)) at pH 7 was more than 3 times higher than that of homogeneous EF (0.05 min(-1)) at pH 3 with 0.1 mM Fe2+ under same current density (9.37 mA cm(-2)). Also, a series of experiments including evolution of solution pH, iron leaching, OFC removal with trapping agent and quantitative detection of hydroxyl radicals ((OH)-O-center dot) were conducted, demonstrating the dominant role of (OH)-O-center dot generated by surface catalyst via Fe-II/Fe-III on LDH cathode for degradation of organics as well contributing to high efficiency and good stability at neutral pH. Besides, formation and evolution of aromatic intermediates, carboxylic acids and inorganic ions (F-, NH4+ and NO3-) were identified by High-Performance Liquid chromatography, Gas Chromatography-Mass Spectrometry and ionic chromatography analyses. These findings allowed proposing a plausible degradation pathway of OFC by (OH)-O-center dot generated in the heterogeneous EF process.

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