Enhanced photocatalytic degradation of organic contaminants over CaFe2O4 under visible LED light irradiation mediated by peroxymonosulfate

doi:10.1016/j.jmst.2020.05.057

Abstract

Abstract:

A simple sol-gel approach is proposed herein to fabricate CaFe₂O₄ for the degradation of various organic pollutants (rhodamine B (RhB), tetracycline hydrochloride, humic acid, and methylene orange) under LED light irradiation mediated by peroxymonosulfate (PMS). The results indicate that the calcination temperature can significantly influence the performance of CaFe₂O₄ for PMS activation, and the CaFe₂O₄ sample obtained at 800 °C (CaFe₂O₄-800) exhibits the best efficiency in degrading RhB, which is much higher than that of Fe₂O₃-800. This can be attributed to the efficient separation of photogenerated electrons (e^-) and holes (h⁺) by PMS, which is validated by transient photocurrent response and photoluminescence measurements. Results from density functional theory calculations indicate that the valence band of CaFe₂O₄-800 exhibits a high concentration of carriers and weak localization of electrons, which are favorable for PMS activation. Radical scavenging results confirm that h⁺ and O₂?^- are the dominant reactive species. Moreover, CaFe₂O₄-800 not only demonstrated a stable performance during eight cycling runs with negligible iron leaching but also exhibited excellent degradation efficiency under natural water and sunlight. Finally, the mechanism and pathway of RhB degradation by the CaFe₂O₄-800/PMS/LED system are also proposed. This work presents the enormous prospect of CaFe₂O₄ as an environmentally benign photocatalyst for PMS activation.

Key words: CaFe₂O₄, Peroxymonosulfate, LED light, Degradation, DFT calculations

Sheng Guo, Zhixiong Yang, Huali Zhang, Wei Yang, Jun Li, Kun Zhou. Enhanced photocatalytic degradation of organic contaminants over CaFe₂O₄ under visible LED light irradiation mediated by peroxymonosulfate[J]. J. Mater. Sci. Technol., 2021, 62: 34-43.

Figures/Tables 13

Fig. 1. Schematic illustration of the formation procedure of CaFe2O4.

Fig. 2. XRD patterns of CaFe2O4-700, CaFe2O4-800, CaFe2O4-900, and CaFe2O4-800C.

Fig. 3. SEM images of (a) CaFe2O4-700, (b) CaFe2O4-800, and (c) CaFe2O4-900 and (d-f) TEM images of CaFe2O4-800.

Fig. 4. XPS spectra of CaFe2O4-800: (a) survey; (b) Ca 2p; (c) Fe 2p; (d) O 1s.

Fig. 5. (a) UV-vis DRS of CaFe2O4-700, CaFe2O4-800, CaFe2O4-900, and Fe2O3-800 and (b) plots of the (αhv)2 versus photo energy (hv) of CaFe2O4-700, CaFe2O4-800, and CaFe2O4-900.

Fig. 6. (a) Effect of calcination temperature on RhB degradation by the CaFe2O4-800/PMS/LED system, (b) RhB degradation under different reaction conditions, (c) reaction rate of RhB degradation under different reaction conditions, effects of (d) catalyst dosage, (e) PMS concentration, and (f) solution pH on RhB degradation by the CaFe2O4-800/PMS/LED system.

Fig. 7. (a) Effect of anion ions (10 mM) on RhB degradation by the CaFe2O4-800/PMS/LED system, (b) degradation of different pollutants by the CaFe2O4-800/PMS/LED system, (c) degradation of RhB in natural water samples by the CaFe2O4-800/PMS/LED system, and (d) degradation of RhB under different light conditions.

Fig. 8. (a) Cyclic experiments for the CaFe2O4-800/PMS/LED system and (b) XRD patterns of the fresh and used CaFe2O4-800.

Fig. 9. (a) Degradation of RhB by the Fe3+/PMS/LED and CaFe2O4-800/PMS/LED systems and (b) effect of scavengers on RhB degradation by the CaFe2O4-800/PMS/LED system.

Fig. 10. Mechanism illustration of RhB degradation by the CaFe2O4-800/PMS/LED system.

Fig. 11. (a) Photocurrent responses of CaFe2O4 with and without PMS under LED light irradiation and (b) PL spectra of CaFe2O4 suspension with and without PMS.

Fig. 12. Charge densities of VBM in CaFe2O4. The charge accumulation is presented in blue and depletion in yellow.

Fig. 13. Proposed pathway for RhB degradation by the CaFe2O4-800/PMS/LED system.

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Enhanced photocatalytic degradation of organic contaminants over CaFe₂O₄ under visible LED light irradiation mediated by peroxymonosulfate

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