Degradation of Metronidazole Antibiotic Using a Novel Synthesized Magnetic Nanocomposite in Heterogeneous Fenton-like Catalytic Process

Document Type : Research Paper


1 Assist. Prof., Social Determinants of Health Research Center, Dept. of Environmental Health Engineering, School of Health, Birjand University of Medical Sciences, Birjand, Iran

2 Assoc. Prof., Social Determinants of Health Research Center, Dept. of Environmental Health Engineering, School of Health, Birjand University of Medical Sciences, Birjand, Iran

3 Assoc. Prof., Dept. of Science and Environemntal Engineering, Faculty of Natural Resources and Environment, Science and Research Branch, Islamic, Azad University, Tehran, Iran

4 Prof., Dept. of Chemistry, Faculty of Science, University of Birjand, Iran


Antibiotics are organic pollutants that are introduced into surface water and underground water sources due to urban and industrial effluents. Due to their high stability, they do not only disrupt the common processes of sewage treatment, but also have toxic effects on humans and other living organisms, and their removal have therefore been considered. This is an experimental study in a laboratory scale with the aim of evaluating the efficiency of the new FeNi3/SiO2/CuS magnetic nanocomposite for the decomposition of metronidazole in the presence of H2O2 as a heterogeneous Fenton- like catalytic process in aqueous solutions. In present study, firstly, this nanocomposite was synthesized and characterized by FESEM, TEM, FTIR, XRD and VSM. This study, which was performed on synthetic sewage in batch system, parameters such as pH (3, 5, 7, 9 and 11), nanocomposite dose (0.005- 0.1 g/L), metronidazole concentration (10-30 mg/L) and the concentration of hydrogen peroxide (50-200 mg/L) at ambient temperature was investigated. The obtained results showed that the highest percentage of removal of metronidazole in pH =7, nanocomposite dose (0.1 g/L), hydrogen peroxide concentration of 150 mg/L for 20 mg/L contaminant concentration at time of 180 minutes, 77.92%. Also, the kinetic rate of degradation flowed pseudo-first-order equation (R2=0.95) and the degradation constant rate of this reaction is 0/0038 (1/min). Based on the results obtained from this study, it can be concluded that Hentrogenase Fenton like catalytic process has a very good effect in removing metronidazole antibiotic contamination from aqueous solutions.


Main Subjects

Ali, A. A., Abdelrahim, M. E., Elmoslamy, N. A., Said, A. S. & Meabed, M. H. 2014. Comparison between nitazoxanide and metronidazole in the treatment of protozoal diarrhea in Children. Medicine Science, 3, 1162-1173.
Ayoub, K., Nélieu, S., Van Hullebusch, E. D., Labanowski, J., Schmitz-Afonso, I., Bermond, A., et al. 2011. Electro-Fenton removal of TNT: evidences of the electro-chemical reduction contribution. Applied Catalysis B: Environmental, 104, 169-176.
Bendesky, A., Menéndez, D. & Ostrosky-Wegman, P. 2002. Is metronidazole carcinogenic? Mutation Research/Reviews in Mutation Research, 511, 133-144.
Beyki, M. H., Shirkhodaie, M. & Shemirani, F. 2016. Polyol route synthesis of a Fe3O4@ CuS nanohybrid for fast preconcentration of gold ions. Analytical Methods, 8, 1351-1358.
Carrales-Alvarado, D., Ocampo-Pérez, R., Leyva-Ramos, R. & Rivera-Utrilla, J. 2014. Removal of the antibiotic metronidazole by adsorption on various carbon materials from aqueous phase. Journal of Colloid and Interface Science, 436, 276-285.
Catrinescu, C., Teodosiu, C., Macoveanu, M., Miehe-Brendlé, J. & Le Dred, R. 2003. Catalytic wet peroxide oxidation of phenol over Fe-exchanged pillared beidellite. Water Research, 37, 1154-1160.
Çelik, A. & Aras Ateş, N. 2006. The frequency of sister chromatid exchanges in cultured human peripheral blood lymphocyte treated with metronidazole in vitro. Drug and Chemical Toxicology, 29, 85-94.
Chen, J. & Zhu, L. 2007. UV-Fenton discolouration and mineralization of Orange II over hydroxyl-Fe-pillared bentonite. Journal of Photochemistry and Photobiology A: Chemistry, 188, 56-64.
Daud, N. & Hameed, B. 2010. Decolorization of Acid Red 1 by Fenton-like process using rice husk ash-based catalyst. Journal of Hazardous Materials, 176, 938-944.
Djeffal, L., Abderrahmane, S., Benzina, M., Fourmentin, M., Siffert, S. & Fourmentin, S. 2014. Efficient degradation of phenol using natural clay as heterogeneous Fenton-like catalyst. Environmental Science and Pollution Research, 21, 3331-3338.
Eslami, A., Amini, M. M., Yazdanbakhsh, A. R., Mohseni‐Bandpei, A., Safari, A. A. & Asadi, A. 2016. N, S co‐doped TiO2 nanoparticles and nanosheets in simulated solar light for photocatalytic degradation of non‐steroidal anti‐inflammatory drugs in water: a comparative study. Journal of Chemical Technology & Biotechnology, 91, 2693-2704.
Farzadkia, M., Esrafili, A., Baghapour, M. A., Shahamat, Y. D. & Okhovat, N. 2014. Degradation of metronidazole in aqueous solution by nano-ZnO/UV photocatalytic process. Desalination and Water Treatment, 52, 4947-4952.
Galván-Tejada, N., Bernès, S., Castillo-Blum, S. E., Nöth, H., Vicente, R. & Barba-Behrens, N. 2002. Supramolecular structures of metronidazole and its copper (II), cobalt (II) and zinc (II) coordination compounds. Journal of Inorganic Biochemistry, 91, 339-348.
Herculano, R. D., Guimarães, S. A. C., Belmonte, G. C., Duarte, M. a. H., Oliveira Júnior, O. N. D., Kinoshita, A., et al. 2010. Metronidazole release using natural rubber latex as matrix. Materials Research, 13, 57-61.
Huang, R., Fang, Z., Yan, X. & Cheng, W. 2012. Heterogeneous sono-fenton catalytic degradation of bisphenol A by Fe3O4 magnetic nanoparticles under neutral condition. Chemical Engineering Journal, 197, 242-249.
Kasim, N. A., Whitehouse, M., Ramachandran, C., Bermejo, M., Lennernäs, H., Hussain, A. S., et al. 2004. Molecular properties of WHO essential drugs and provisional biopharmaceutical classification. Molecular Pharmaceutics, 1, 85-96.
Kudo, T., Endo, Y., Taguchi, R., Yatsu, M. & Ito, K. 2015. Metronidazole reduces the expression of cytochrome P450 enzymes in HepaRG cells and cryopreserved human hepatocytes. Xenobiotica, 45, 413-419.
Lau, A. H., Lam, N. P., Piscitelli, S. C., Wilkes, L. & Danziger, L. H. 1992. Clinical pharmacokinetics of metronidazole and other nitroimidazole anti-infectives. Clinical Pharmacokinetics, 23, 328-364.
Lindberg, R., Jarnheimer, P.-Å., Olsen, B., Johansson, M. & Tysklind, M. 2004. Determination of antibiotic substances in hospital sewage water using solid phase extraction and liquid chromatography/mass spectrometry and group analogue internal standards. Chemosphere, 57, 1479-1488.
Liu, R., Chiu, H., Shiau, C.-S., Yeh, R. Y.-L. & Hung, Y.-T. 2007. Degradation and sludge production of textile dyes by Fenton and photo-Fenton processes. Dyes and Pigments, 73, 1-6.
Liu, X., Wang, F., Chen, Z., Megharaj, M. & Naidu, R. 2014. Heterogeneous fenton oxidation of Direct Black G in dye effluent using functional kaolin-supported nanoscale zero iron. Environmental Science and Pollution Research, 21, 1936-1943.
Liu, X., Zhang, Q., Yu, B., Wu, R., Mai, J., Wang, R., et al. 2016. Preparation of Fe3O4/TiO2/C nanocomposites and their application in Fenton-like catalysis for dye decoloration. Catalysts, 6 (9), Article No. 146.
Luo, W., Zhu, L., Wang, N., Tang, H., Cao, M. & She, Y. 2010. Efficient removal of organic pollutants with magnetic nanoscaled BiFeO3 as a reusable heterogeneous fenton-like catalyst. Environmental Science and Technology, 44, 1786-1791.
Nasseri, M. A. & Sadeghzadeh, S. M. 2013. A highly active FeNi3–SiO2 magnetic nanoparticles catalyst for the preparation of 4H-benzo [b] pyrans and Spirooxindoles under mild conditions. Journal of the Iranian Chemical Society, 10, 1047-1056.
Nidheesh, P. 2015. Heterogeneous fenton catalysts for the abatement of organic pollutants from aqueous solution: a review. RSC Advances, 5, 40552-40577.
Pradhan, A. C., Nanda, B., Parida, K. & Das, M. 2013. Quick photo-fenton degradation of phenolic compounds by Cu/Al2O3–MCM-41 under visible light irradiation: small particle size, stabilization of copper, easy reducibility of Cu and visible light active material. Dalton Transactions, 42, 558-566.
Safari, G., Hoseini, M., Kamali, H., Moradirad, R. & Mahvi, A. 2014. Photocatalytic degradation of tetracycline antibiotic from aqueous solutions using UV/TiO2 and UV/H2O2/TiO2. Journal of Health,5(3), 203-213. (In Persian)
Sánchez‐Polo, M., Rivera‐Utrilla, J., Prados‐Joya, G. & Ocampo‐Pérez, R. 2012. Metronidazole photodegradation in aqueous solution by using photosensitizers and hydrogen peroxide. Journal of Chemical Technology and Biotechnology, 87, 1202-1208.
Shen, J., Zhu, J., Kong, Y., Li, T. & Chen, Z. 2013. Synthesized heterogeneous Fenton-like goethite (FeOOH) catalyst for degradation of p-chloronitrobenzene. Water Science and Technology, 68, Article No. 1614.
Tian, S., Zhang, J., Chen, J., Kong, L., Lu, J., Ding, F., et al. 2013. Fe2 (MoO4)3 as an effective photo-fenton-like catalyst for the degradation of anionic and cationic dyes in a wide pH range. Industrial and Engineering Chemistry Research, 52, 13333-13341.
Wang, R., Liu, X., Wu, R., Yu, B., Li, H., Zhang, X., et al. 2016. Fe3O4/SiO2/C nanocomposite as a high-performance fenton-like catalyst in a neutral environment. RSC Advances, 6, 8594-8600.
Yang, S.-T., Zhang, W., Xie, J., Liao, R., Zhang, X., Yu, B., et al. 2015. Fe3O4@ SiO2 nanoparticles as a high-performance Fenton-like catalyst in a neutral environment. RSCAdvances, 5, 5458-5463.
Zhou, S., Shao, Y., Gao, N., Zhu, S., Ma, Y. & Deng, J. 2014. Chlorination and chloramination of tetracycline antibiotics: disinfection by-products formation and influential factors. Ecotoxicology and Environmental Safety, 107, 30-35.