Abstract
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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Extra data are available from the authors (lixiaoli@lzu.edu.cn) upon reasonable request.
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The authors gratefully acknowledge the financial support from the Natural Science Foundation of Gansu Province (No. 20JR10RA631) and the Open Project of Key Laboratory of Green Chemical Engineering Process of Ministry of Education (No. GCP20200207).
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Xiaoli Li proposed the project and provided the funds. Liyan He designed the experiments and synthesized the materials. Liyan He did the series of experiments and prepared the first draft of this manuscript. Hui Li, Jianzhi Wang, and Qifei Gao revised the manuscript. All co-authors contributed to this work.
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He, L., Li, H., Wang, J. et al. Peroxymonosulfate activation by Co-doped magnetic Mn3O4 for degradation of oxytetracycline in water. Environ Sci Pollut Res 29, 39249–39265 (2022). https://doi.org/10.1007/s11356-022-18929-1
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DOI: https://doi.org/10.1007/s11356-022-18929-1