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. 2019 May 28;9(29):16496-16508.
doi: 10.1039/c9ra02757b. eCollection 2019 May 24.

Catalytic degradation of diclofenac from aqueous solutions using peroxymonosulfate activated by magnetic MWCNTs-CoFe3O4 nanoparticles

Yousef Dadban Shahamat  1 , Mohammad Ali Zazouli  2 , Mohammad Reza Zare  3 , Nezamaddin Mengelizadeh  4
Affiliations

Catalytic degradation of diclofenac from aqueous solutions using peroxymonosulfate activated by magnetic MWCNTs-CoFe3O4 nanoparticles

Yousef Dadban Shahamat et al. RSC Adv. .

Abstract

CoFe3O4 nanoparticles supported on multi-walled carbon nanotubes (MWCNTs-CoFe3O4) were synthesized by the co-precipitation method as a novel catalyst for degradation of diclofenac (DCF). The comparative experiments indicated that MWCNTs-CoFe3O4 has a better catalytic activity in degradation of DCF and activation of peroxymonosulfate (PMS) compared to other catalytic systems. This can be attributed to the interaction of MWCNTs with CoFe3O4 in accelerating the absorption process and activating the PMS (E a = 22.93 kJ mol-1). The removal efficiencies of DCF and total organic carbon (TOC) were 99.04% and 50.11%, under optimum conditions, e.g., pH of 7, PMS dosage of 4 mM, DCF concentration of 30 mg L-1, catalyst dosage of 500 mg L-1, and reaction time of 120 min. The oxidation of DCF was fitted by the pseudo-first-order kinetic model and the constant rate was increased by increasing the pH, temperature, dosage of PMS and catalyst. The production of reactive species was studied using scavengers such as TBA and ethanol and the results showed that sulfate radical is the reactive species responsible for the degradation of DCF. The MWCNTs-CoFe3O4 catalyst showed high stability and reusability based on five successful repeated reactions, X-ray diffraction and energy dispersive X-ray spectroscopy analysis. Based on the intermediates detected by gas chromatography-mass spectrometry (GC-MS), the possible pathways for DCF catalytic oxidation were proposed. The results explained that the PMS/MWCNTs-CoFe3O4 system is a promising method for treating DCF solution due to high efficiency, good reusability of catalyst and greater PMS activation.

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Conflict of interest statement

There are no conflicts to declare.

Figures

Fig. 1
Fig. 1. SEM images of MWCNTs (a), MWCNTs-Fe3O4 (b) and MWCNTs-CoFe3O4 (c).
Fig. 2
Fig. 2. TEM images of MWCNTs-Fe3O4 (a) and MWCNTs-CoFe3O4 (b); EDX spectra of MWCNTs-CoFe3O4 (c); magnetic properties of MWCNTs-CoFe3O4 (d).
Fig. 3
Fig. 3. XRD patterns of MWCNTs, Fe3O4, MWCNTs-Fe3O4 and MWCNTs-CoFe3O4.
Fig. 4
Fig. 4. FTIR spectrum of MWCNTs, Fe3O4, MWCNTs-Fe3O4 and MWCNTs-CoFe3O4.
Fig. 5
Fig. 5. The removal efficiency of DCF (a), COD and TOC (b) under different conditions (reaction conditions: pH = 7, MWCNTs-CoFe3O4 = 200 mg L−1, Co2+ = 16.5 mg L−1, PMS = 2 mM, DCF = 30 mg L−1).
Fig. 6
Fig. 6. Effect of solution pH on the removal efficiency of DCF.
Fig. 7
Fig. 7. Effect of MWCNTs-CoFe3O4 dosage on the removal efficiency of DCF.
Fig. 8
Fig. 8. Effect of PMS dosage on the removal efficiency of DCF.
Fig. 9
Fig. 9. Effect of initial DCF concentration on the removal efficiency of DCF.
Fig. 10
Fig. 10. Effect of temperature at presence (a) and without presence of catalyst (b) on the removal efficiency of DCF.
Fig. 11
Fig. 11. Effect of various anions on the removal efficiency of DCF (a) and kinetic constant rate (b).
Fig. 12
Fig. 12. Influence of TBA and ethanol on the removal efficiency of DCF (a) and kinetic constant rate (b).
Fig. 13
Fig. 13. (a) Catalytic performance of recycled MWCNTs-CoFe3O4 for DCF removal, (b) COD and TOC removal; (c) EDS analysis and (d) XRD pattern of MWCNTs-CoFe3O4 after the 4th cycle of DCF removal.
Fig. 14
Fig. 14. The degradation pathways of DCF in MWCNTs-CoFe3O4/PMS process.
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