Journal of Water and Wastewater; Ab va Fazilab (in persian)

Journal of Water and Wastewater; Ab va Fazilab (in persian)

Removal of Tetracycline from Aqueous Environments Using CTF-P Photocatalyst with Organic-Covalent Structure under Visible Light

Document Type : Research Paper

Authors
1 PhD. Candidate, Dept. of the Environmental Engineering, College of Engineering, Hamedan Branch, Islamic Azad University, Hamedan, Iran
2 Prof., Dept. of the Environment, College of Basic Sciences, Hamedan Branch, Islamic Azad University, Hamedan, Iran
3 Prof., Dept. of Environmental Health Engineering, Faculty of Health, Kurdistan University of Medical Sciences, Sanandaj, Iran
Abstract
Tetracycline is a common commercial antibiotic that is used in large quantities against bacteria and a wide range of microorganisms. The presence of TC in pharmaceutical industries and hospital wastewater can cause an unpleasant odor, skin disorders, and microbial resistance in pathogenic agents, and can lead to the death of effective microorganisms responsible for purifying wastewater. Therefore, its removal before entering into the environment is of great importance. Given the importance of the issue, this study evaluates the efficiency of TC removal from aqueous environments using a photocatalyst with an organic-covalent structure under visible light. In this study, a photocatalyst with an organic-covalent structure (CTF-P) was synthesized by reflux method and its efficiency was investigated. To identify the synthetic photocatalyst characterization, transmission electron microscopy, scanning electron microscopy, X-ray diffraction, elemental mapping analysis (EDX-Mapping), Fourier transform infrared spectroscopy, nitrogen adsorption-desorption analysis (BET) and diffuse reflectance spectroscopy were employed. Moreover, the effects of pH variables (4-9), photocatalyst concentration (10-40 mg) and contact time ((-30)-180 min) on the removal process were evaluated. Based on the results obtained, maximum removal efficiency was achieved at a 90 min contact time, 30 mg of photocatalyst content, and pH=7. The study of scavengers showed that the oxidants (i.e. , e- and ) play an important role in the degradation process of TC from wastewater. As shown, CTF-P photocatalyst with organic-covalent structure could be used as an effective material for the removal of TC from industrial wastewater under visible light.
Keywords

Asgari, G., Alahabadi, A., Shomoossi, N., Yazdani-Aval, M., Shabanloo, A., Darvishmotevalli, M. et al., 2024. Mineralization and biodegradability improvement of textile wastewater using persulfate/dithionite process. Biomass Conversion and Biorefinery, 14, 21363-21373. https://doi.org/10.1007/s13399-023-04128-6.
Carino, I. S., Pasqua, L., Testa, F., Aiello, R., Puoci, F., Iemma, F. and Picci, N., 2007. Silica-based mesoporous materials as drug delivery system for methotrexate release. Drug Delivery, 14, 491-495. https://doi.org/10.1080/10717540701606244.
Camara, A. G., Sousa, R. P., Costa, M. J. S., Dantas, E. J. M., Frety, R., Luz, G. E. et al., 2025. Heterostructured g-C3N4-TiO2 nanocomposites applied to p-toluic acid degradation under solar light-induced photocatalytic process. Journal of Photochemistry and Photobiology A: Chemistry, 459, 116021. https://doi.org/10.1016/j.jphotochem.2024.116021.
Chen, R., Zhang, H., Dong, Y. and Shi, H., 2024. Dual metal ions/BNQDs boost PMS activation over copper tungstate photocatalyst for antibiotic removal: intermediate, toxicity assessment and mechanism. Journal of Materials Science and Technology, 170, 11-24. https://doi.org/10.1016/j.jmst.2023.07.005.
Gao, H., Angadi, J., Wang, S., Zhou, X., Yang, H., Al-Enizi, A. M. et al., 2024. Designing of Z-scheme MgFe2O4/Fe2O3 coupled CoCr2O4 heterojunction with high photocatalytic activity for the removal of tetracycline hydrochloride in wastewater. Advanced Sustainable Systems, 8, 2300533. https://doi.org/10.1002/adsu.202300533.
Hu, X., Long, Y., Fan, M., Yuan, M., Zhao, H., Ma, J. et al., 2019. Two-dimensional covalent organic frameworks as self-template derived nitrogen-doped carbon nanosheets for eco-friendly metal-free catalysis. Applied Catalysis B: Environmental, 244, 25-35. https://doi.org/10.1016/j.apcatb.2018.11.028.
Jin, J., Xu, M., Dong, F., Hu, H., Yang, Y., Jin, W. et al., 2024. Synthesis of novel Cu2WS4/Bi2WO6 heterojunctions and evaluation of their photocatalytic activity for removal of tetracycline under visible light irradiation. Optical Materials, 147, 114700. https://doi.org/10.1016/j.optmat.2023.114700.
Koundle, P., Nirmalkar, N. and Boczkaj, G., 2025. High performance ozone nanobubbles based advanced oxidation processes (AOPs) for degradation of organic pollutants under high pollutant loading. Journal of Environmental Management, 374, 124107. https://doi.org/10.1016/j.jenvman.2025.124107.
Li, Y., Wang, H., Liu, J., Liu, X., Guan, J., Fu, J. et al., 2024. Synthesis of a novel Bi19Cl3S27/Bi2MoO6 Z-type heterojunction for efficient photocatalytic removal of tetracycline antibiotic and Cr (VI): intermediate toxicity and mechanism insight. Environmental Research, 263, 120212. https://doi.org/10.1016/j.envres.2024.120212.
Liu, B., Li, Y., Wu, Y. and Xing, S., 2021. Enhanced degradation of ofloxacin by persulfate activation with Mn doped CuO: synergetic effect between adsorption and non-radical activation. Chemical Engineering Journal, 417, 127972. https://doi.org/10.1016/j.cej.2020.127972.
Liu, J., Li, Y., Liu, X., Fu, J., Li, J., Liu, Y. et al., 2024. Synthesis of a novel flower-like Bi4Ti3O12/AgI Z-type heterojunction for efficient photocatalytic removal of tetracycline antibiotic and RhB. Journal of Water Process Engineering, 67, 106262. https://doi.org/10.1016/j.jwpe.2024.106262.
Mahdavi, R. and Ashraf Talesh, S. S., 2021. Enhanced selective photocatalytic and sonocatalytic degradation in mixed dye aqueous solution by ZnO/GO nanocomposites: response surface methodology. Materials Chemistry and Physics, 267, 124581. https://doi.org/10.1016/j.matchemphys.2021.124581.
Pan, Y., Lin, B., Li, X., Li, X., Hu, C., Chen, Z. et al., 2025. Porous hierarchical sphere g-C3N4 with coordinated Co-ions as an efficient and stable self-fenton photocatalyst for the removal of antibiotic. Separation and Purification Technology, 354, 129456. https://doi.org/10.1016/j.seppur.2024.129456.
Ravi, R. and Golder, A. K., 2025. Photocatalytic and biological degradation processes to mineralize pharmaceutically active compounds and catalyst recovery: a review. Coordination Chemistry Reviews, 523, 216267. https://doi.org/10.1016/j.ccr.2024.216267.
Siddiq, H. A., Alhifthi, A., Ghubayra, R. and Madkour, M., 2025. Layered bismuthene forming the interfacial pathway for rapid charge transfer in CuNb13O33/g-C3N5 photocatalyst for enhancing ciprofloxacin degradation. Journal of Photochemistry and Photobiology A: Chemistry, 459, 116073. https://doi.org/10.1016/j.jphotochem.2024.116073.
Sohrabi, N., Mohammadi, R., Ghassemzadeh, H. R. and Heris, S. S. S., 2021. Equilibrium, kinetic and thermodynamic study of diazinon adsorption from water by clay/GO/Fe3O4: modeling and optimization based on response surface methodology and artificial neural network. Journal of Molecular Liquids, 328, 115384. https://doi.org/10.1016/j.molliq.2021.115384.
Xiang, X., Zhang, M., Huang, Q., Mao, Y., Jia, J., Zeng, X. et al., 2024. Construction of S-scheme CuInS2/ZnIn2S4 heterostructures for enhanced photocatalytic activity towards Cr(VI) removal and antibiotics degradation. Chemosphere, 352, 141351. https://doi.org/10.1016/j.chemosphere.2024.141351.
Yu, G., Sun, Q., Yang, Y., Chen, S., Long, Y., Li, Y. et al., 2024. BiOCl-based composites for photocatalytic degradation of antibiotics: a review of synthesis method, modification, factors affecting photodegradation and toxicity assessment. Journal of Alloys and Compounds, 981, 173733. https://doi.org/10.1016/j.jallcom.2024.173733.
Zandipak, R., Bahramifar, N., Torabi, M., Calero, M., Muñoz-Batista, M. J. and Solís, R. R., 2024a. Synergistic effect of graphitic-like carbon nitride and sulfur-based thiazole-linked organic polymer heterostructures for boosting the photocatalytic degradation of pharmaceuticals in water. Chemical Engineering Journal, 494, 152843. https://doi.org/10.1016/j.cej.2024.152843.
Zandipak, R., Bahramifar, N., Younesi, H. and Zolfigol, M. A., 2024b. Electro-photocatalyst effect of N-S-doped carbon dots and covalent organic triazine framework heterostructures for boosting photocatalytic degradation of phenanthrene in water. Chemosphere, 364, 142980. https://doi.org/10.1016/j.chemosphere.2024.142980.
Zandipak, R., Bahramifar, N., Younesi, H. and Zolfigol, M. A., 2025a. Decoration of carbon nanodots on conjugated triazine framework nanosheets as Z-scheme heterojunction for boosting opto-electro photocatalytic degradation of organic hydrocarbons from petrochemical wastewater. Journal of Environmental Chemical Engineering, 13, 115380. https://doi.org/10.1016/j.jece.2025.115380.
Zandipak, R., Bahramifar, N., Younesi, H. and Zolfigol, M. A., 2025b. Photocatalytic degradation of rhodamine B dye from aqueous media using imide conjugated polymer photocatalyst under visible light. Iranian Journal of Health and Environment, 17, 741-756. (In Persian) [Link]
Zandipak, R. and Sobhanardakani, S., 2018. Novel mesoporous Fe3O4/SiO2/CTAB–SiO2 as an effective adsorbent for the removal of amoxicillin and tetracycline from water. Clean Technologies and Environmental Policy, 20, 871-885. https://doi.org/10.1007/s10098-018-1507-5.