Corresponding Author

Jian-Feng Li(li@xmu.edu.cn)


The purpose of this study is to optimize the electrochemical degradation of oxytetracycline (OTC) in water using a low cost and simple preparation method. In this paper, the Fe3O4 magnetic nanoparticles were used as catalysts to activate the electrochemical oxidation system of peroxydisulfates (PDS) which acted as electrolytes to provide active free radicals in order to improve the degradation of OTC under the condition of applying current. As one of the tetracycline antibiotics (TCs), OTC is one of the most used antibiotics in the world, therefore, it is necessary to study the effective degradation of OTC. By means of field emission scanning electron microscopy (FESEM), X-ray diffraction (XRD) and other characterization methods, it was proved that the Fe3O4 magnetic nanoparticles at about 150 nm were successfully prepared by a simple hydrothermal method. Firstly, it is suggested that the application of electric current and the presence of Fe3O4 magnetic nanoparticles are necessary for the effective degradation of OTC. Secondly, the optimal reaction experiment confirmed an excellent OTC degradation ability by combination of Fe3O4 magnetic nanoparticles and current. The optimal reaction conditions were as follows: the concentration of PDS was 4.0 mmol·L-1, the initial pH value of the solution was 7, and the current density j was 30 mA·cm-2. When the dosage of Fe3O4 magnetic nanoparticles was 0.1 g·L-1 and the initial OTC concentration was 70 mg·L-1, the degradation rate of OTC could reach 88.75% within 60 min and the rate constant of the first-order kinetics simulation curve could reach 0.06069. In addition, the variation of UV-vis characteristic peak of OTC during the degradation process revealed that the change of OTC concentration was not due to simple physical adsorption, but through the complete degradation of active free radicals. In addition, after the continuous circulation of Fe3O4 magnetic nanoparticles for 5 times, the degradation rate of OTC could still reach more than 68%, proving that Fe3O4 magnetic nanoparticles have good catalytic stability. The presence of Fe3O4 magnetic nanoparticles and the application of electric current could promote the formations of SO4·- and ·OH, respectively. The radical quenching experiments showed that both SO4 ·- and ·OH were active free radicals degraded by antibiotics. This work uses a low-cost catalyst to enhance an electrochemical degradation of OTC. The experimental operation is simple, the degradation rate is fast, and the energy consumption is low. It is promising to practical applications.

Graphical Abstract


electrochemical oxidation, oxytetracycline degradation, Fe3O4 magnetic nanoparticles, stability

Publication Date


Online Available Date


Revised Date


Received Date



[1] Xu S S, Lü Y P, Zhang Y. 3D hydrangea-like Mn3O4@(PSS/PDDA/Pt)n with ultrafine Pt nanoparticles modified anode for electrochemical oxidation of tetracycline[J]. J. Taiwan Inst. Chem. E., 2020, 112: 240-250.
doi: 10.1016/j.jtice.2020.06.009 URL

[2] Tang S F, Zhao M Z, Yuan D L, Li X, Wang Z T, Zhang X Y, Jiao T F, Ke J. Fe3O4 nanoparticles three-dimensional electro-peroxydisulfate for improving tetracycline degradation[J]. Chemosphere, 2021, 268: 129315.
doi: 10.1016/j.chemosphere.2020.129315 URL

[3] Ren F J, Wang T, Liu H T, Liu D S, Zhong R, You C Y, Zhang W J, Lv S Y, Liu S S, Zhu H, Chang L, Wang B. CoMn2O4 nanoparticles embed in graphene oxide aerogel with three-dimensional network for practical application prospects of oxytetracycline degradation[J]. Sep. Purif. Te-chnol., 2021, 259: 118179.

[4] Halling-Sorensen B, Sengelov G, Tjornelund J. Toxicity of tetracyclines and tetracycline degradation products to environmentally relevant bacteria, including selected tetracycline-resistant bacteria[J]. Arch. Environ. Contam. Toxicol., 2002, 42(3): 263-271.
doi: 10.1007/s00244-001-0017-2 URL

[5] Daghrir R, Drogui P. Tetracycline antibiotics in the environment: a review[J]. Environ Chem Lett., 2013, 11(3): 209-227.
doi: 10.1007/s10311-013-0404-8 URL

[6] Gao Y, Li Y, Zhang L, Huang H, Hu J J, Shah S M, Su X G. Adsorption and removal of tetracycline antibiotics from aqueous solution by graphene oxide[J]. J. Colloid Interface Sci., 2012, 368: 540-546.
doi: 10.1016/j.jcis.2011.11.015 URL

[7] Khan M H, Bae H, Jung J Y. Tetracycline degradation by ozonation in the aqueous phase: proposed degradation intermediates and pathway[J]. J. Hazard. Mater., 2010, 181(1-3): 659-665.
doi: 10.1016/j.jhazmat.2010.05.063 URL

[8] Yang Q X, Yang X F, Yan Y, Sun C, Wu H J, He J, Wang D S. Heterogeneous activation of peroxymonosulfate by different ferromanganese oxides for tetracycline degradation: Structure dependence and catalytic mechanism[J]. Chem. Eng. J., 2018, 348: 263-270.
doi: 10.1016/j.cej.2018.04.206 URL

[9] Wang J B, Zhi D, Zhou H, He X W, Zhang D Y. Evaluating tetracycline degradation pathway and intermediate toxicity during the electrochemical oxidation over a Ti/Ti4O7 anode[J]. Water Res., 2018, 137: 324-334.
doi: 10.1016/j.watres.2018.03.030 URL

[10] Zhang Y Q, Zuo S J, Zhang Y, Ren G B, Pan Y W, Zhang Q Z, Zhou M H. Simultaneous removal of tetracycline and disinfection by a flow-through electro-peroxone process for reclamation from municipal secondary effluent[J]. J. Hazard. Mater., 2019, 368: 771-777.
doi: 10.1016/j.jhazmat.2019.02.005 URL

[11] Xie L B, Mi X Y, Liu Y G, Li Y, Sun Y, Zhan S H, Hu W P. Highly efficient degradation of polyacrylamide by an Fe-doped Ce0.75Zr0.25O2 solid solution/CF composite cathode in a heterogeneous electro-fenton process[J]. ACS Appl. Mater. Interfaces., 2019, 11(34): 30703-30712.
doi: 10.1021/acsami.9b06396 URL

[12] Guo P C, Qiu H B, Yang C W, Zhang X, Shao X Y, Lai Y L, Sheng G P. Highly efficient removal and detoxification of phenolic compounds using persulfate activated by MnOx@OMC: Synergistic mechanism and kinetic analysis[J]. J. Hazard. Mater., 2021, 402(15): 123846-123855.
doi: 10.1016/j.jhazmat.2020.123846 URL

[13] Guo H, Su S, Liu Y, Ren X H, Guo W L. Enhanced catalytic activity of MIL-101(Fe) with coordinatively unsaturated sites for activating persulfate to degrade organic pollutants[J]. Environ. Sci. Pollut. Res., 2020, 27: 17194-17204.
doi: 10.1007/s11356-020-08316-z URL

[14] Gao Y, Wang Q, Ji G Z, Li A M. Degradation of antibiotic pollutants by persulfate activated with various carbon materials[J]. Chem. Eng. J., 2022, 429: 132387-132400.
doi: 10.1016/j.cej.2021.132387 URL

[15] Song H R, Yan L X, Jiang J, Ma J, Pang S Y, Zhai X D, Zhang W, Li D. Enhanced degradation of antibiotic sulfamethoxazole by electrochemical activation of PDS using carbon anodes[J]. Chem. Eng. J., 2018, 344: 12-20.
doi: 10.1016/j.cej.2018.03.050 URL

[16] Cao M H, Hou Y Z, Zhang E, Tu S X, Xiong S L. Ascorbic acid induced activation of persulfate for pentachloro-phenol degradation[J]. Chemosphere, 2019, 229: 200-205.
doi: 10.1016/j.chemosphere.2019.04.135 URL

[17] Matzek L W, Carter K E. Activated persulfate for organic chemical degradation: A review[J]. Chemosphere, 2016, 151: 178-188.
doi: 10.1016/j.chemosphere.2016.02.055 pmid: 26938680

[18] Keyikoglu R, Karatas O, Khataee A, Kobya M, Can O T, Soltani R D C, Isleyen M. Peroxydisulfate activation by in-situ synthesized Fe3O4 nanoparticles for degradation of atrazine: Performance and mechanism[J]. Sep. Purif. Te-chnol., 2020, 247: 116925.

[19] Ganiyu S O, Zhou M H, Martínez-Huitle C A. Heterogeneous electro-Fenton and photoelectro-Fenton processes: A critical review of fundamental principles and application for water/wastewater treatment[J]. Appl. Catal. B., 2018, 235: 103-129.
doi: 10.1016/j.apcatb.2018.04.044 URL

[20] Bagheri S, TermehYousefi A, Do T O. Photocatalytic pathway toward degradation of environmental pharmaceutical pollutants: structure, kinetics and mechanism approach[J]. Catal. Sci. Technol., 2017, 7: 4548-4569.
doi: 10.1039/C7CY00468K URL

[21] Ike I A, Linden K G, Orbell J D, Duke M. Critical review of the science and sustainability of persulphate advanced oxidation processes[J]. Chem. Eng. J., 2018, 338: 651-669.
doi: 10.1016/j.cej.2018.01.034 URL

[22] Zhang C, Li F, Wen R B, Zhang H K, Elumalai P, Zheng Q, Chen H Y, Yang Y J, Huang M Z, Ying G. G. Heterogeneous electro-Fenton using three-dimension NZVI-BC electrodes for degradation of neonicotinoid wastewater[J]. Water Res., 2020, 182: 115975.
doi: 10.1016/j.watres.2020.115975 URL

[23] Poblete R, Oller I, Maldonado M I, Cortes E. Improved landfill leachate quality using ozone, UV solar radiation, hydrogen peroxide, persulfate and adsorption processes[J]. J. Environ. Manage., 2019, 232: 45-51.
doi: 10.1016/j.jenvman.2018.11.030 URL

[24] Dong Z Y, Zhang Q, Chen B Y, Hong J M. Oxidation of bisphenol A by persulfate via Fe3O4-α-MnO2 nanoflower-like catalyst: Mechanism and efficiency[J]. Chem. Eng. J., 2019, 357: 337-347.
doi: 10.1016/j.cej.2018.09.179 URL



To view the content in your browser, please download Adobe Reader or, alternately,
you may Download the file to your hard drive.

NOTE: The latest versions of Adobe Reader do not support viewing PDF files within Firefox on Mac OS and if you are using a modern (Intel) Mac, there is no official plugin for viewing PDF files within the browser window.