Abstrakt

In this study, a novel TiO2/Ti3C2/MnFe2O4 magnetic photocatalyst with dual properties, enabling (i) improved photocatalytic degradation with PMS activation under simulated solar light and (ii) magnetic separation after the degradation process in an external magnetic field was developed and applied for the efficient photodegradation pharmaceutically active compounds (PhACs) frequently present in wastewater and surface waters worldwide. MXene was used as a Ti precursor for anatase/rutile synthesis and as a co-catalyst in the photodegradation process. Manganese ferrite with ferrimagnetic properties was coupled with the TiO2/Ti3C2 composite to facilitate the magnetic separation after the purification process in an external magnetic field. Moreover, MnFe2O4 was used for PMS activation, producing •SO4- radicals with a strong oxidation ability and higher redox potential of 2.5–3.1 V (vs. NHE) than •OH radicals with a standard oxidation–reduction potential of 2.8 V. The effect of the manganese ferrite content in the composite structure (5 wt% and 20 wt%) on the physicochemical properties and photocatalytic activity of the magnetic photocatalyst was investigated. Furthermore, the most photocatalytic active composite of TiO2/MXene/5%MnFe2O4 was used for peroxymonosulphate-assisted photocatalytic degradation of ibuprofen and carbamazepine. The effect of peroxymonosulphate concentration (0.0625 mM, 0.125 mM, and 0.25 mM) and the synergistic effect of PMS activation on photocatalytic degradation was studied. Based on the obtained results, it was found that TiO2/MXene/5%MnFe2O4/PMS process is an efficient advanced treatment technology for the oxidation of emerging contaminants that are not susceptible to biodegradation. Carbamazepine and ibuprofen were completely degraded within 20 min and 10 min of the PMS-assisted photodegradation process under simulated solar light. The trapping experiments confirmed that •SO4- and •O2- are the main oxidising species involved in the CBZ degradation, while •SO4- and h+ in the IBP degradation. Furthermore, introducing interfering ions of Na+, Ca2+, Mg2+, Cl-, and SO42– in the model seawater did not affect the removal efficiency of both pharmaceuticals. In terms of reusability, the performance of the TiO2/MXene/5% MnFe2O4/PMS photocatalyst was stable after four subsequent cycles of carbamazepine and ibuprofen degradation.

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