Peroxymonosulfate activation by Co-doped magnetic Mn3O4 for degradation of oxytetracycline in water
2022
He, Liyan | Li, Hui | Wang, Jianzhi | Gao, Qifei | Li, Xiaoli
Co-doped magnetic Mn₃O₄ was synthesized by the solvothermal method and adopted as an effective catalyst for the degradation of oxytetracycline (OTC) in water. Synergistic interactions between Co-Mn₃O₄ and Fe₃O₄ not only resulted in the enhanced catalytic activity through the activation of peroxymonosulfate (PMS) to degrade OTC but also made Fe₃O₄/Co-Mn₃O₄ easy to be separated and recovered from aqueous solution. 94.2% of OTC could be degraded within 60 min at an initial OTC concentration of 10 mg L⁻¹, catalyst dosage of 0.2 g L⁻¹, and PMS concentration of 10 mM. The high efficiency of OTC removal was achieved in a wider pH range of 3.0–10.0. Co (II), Co (III), Fe (II), Fe (III), Mn (II), Mn (III), and Mn (IV) on Fe₃O₄/Co-Mn₃O₄ were identified as catalytic sites based on XPS analysis. The free radical quenching experiments showed that O₂•⁻ radicals and ¹O₂ played the main role in the degradation process and the catalytic degradation of OTC involved both free radical and non-free radical reactions. Eventually, the intermediates of OTC degradation were examined, and the possible decomposition pathways were proposed. The excellent catalytic performances of Fe₃O₄/Co-Mn₃O₄ came from the fact that the large specific surface area could provide abundant active sites for the activation of PMS and the redistribution of inter-atomic charges accelerated the redox reactions of metal ions. The high degradation efficiency and rate constant of OTC in actual water samples indicated that Fe₃O₄/Co-Mn₃O₄ had a good practical application potential.
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