NONE 20260505080618295 wseas/wseas content-registration-form+ja@crossref.org content-registration-form WSEAS TRANSACTIONS ON ENVIRONMENT AND DEVELOPMENT 1790-5079 2224-3496 Yousra Aissaoui Useful Materials Laboratory (LMU), National Institute for Physical and Chemical Research and Analysis (INRAP), BiotechPole Ariana 2020, TUNISIA Malika Trabelsi-Ayadi Laboratory of Application Chemistry to the Resources and Natural Substances and the Environment (LACReSNE), Faculty of Science of Bizerte, University of Carthage, Zarzouna, Bizerte 7021, TUNISIA Ibtissem Ghorbel-Abid Useful Materials Laboratory (LMU), National Institute for Physical and Chemical Research and Analysis (INRAP), BiotechPole Ariana 2020, TUNISIA Conventional water treatment plants are often not equipped to effectively eliminate micropollutants such as antibiotics. Sulfamethoxazole (SMX) and trimethoprim (TMP) are widely used in human and veterinary treatment. This study aims to remove these two antibiotics from aqueous solution using natural clay as an adsorbent. A Box-Behnken matrix was used to model and optimize the process. the textural, structural, and morphological properties of raw and purified natural clay were studied. Four independent variables were selected: the initial concentration, pH, contact time, and temperature. Under the experimental conditions, the system reached equilibrium in 80 min. The maximum adsorption of SMX and TMP was approximately 98%. The maximum adsorption capacity was estimated to be 250 mg.g-1 and 190 mg.g-1 at pH 6. According to the Box-Behnken model, high correlation coefficient values and p values greater than 0.05 corresponded to a good fit to the optimal combination of process parameters. 05 05 2026 05 05 2026 429 35 https://creativecommons.org/licenses/by/4.0/deed.en_US 10.37394/232015.2026.22.35 https://wseas.com/journals/ead/2026/a705115-013(2026).pdf A. Pal, K. Y.-H. Gin, A. Y.-C. Lin, M. Reinhard, Impacts of emerging organic contaminants on freshwater resources: Review of recent occurrences, sources, fate and effects, Science of the Total Environment, Vol. 408, No. 24, 2010, pp. 6062–6069. https://doi.org/10.1016/j.scitotenv.2010.09.026 T. Cherian, C. Ragavendran, S. Vijayan, S. Kurien, W. J. G. M. Peijnenburg, A review on the fate, human health and environmental impacts, as well as regulation of antibiotics used in aquaculture, Environmental Advances, Vol. 13, 2023, pp. 100411. https://doi.org/10.1016/j.envadv.2023.100411 Seafood Watch, Understanding the use and impact of antibiotics in aquaculture, Monterey Bay Aquarium, Seafood Sustainability Series, Vol. 1, 2023. https://www.seafoodwatch.org/ [Access Date: 01/01/2026] A. El Badawy, D. Hamza, Z. Ahmed, M. A. Sabry, Seasonal and environmental drivers of antibiotic resistance and virulence in Escherichia coli from aquaculture and their public health implications, Scientific Reports, Vol. 15, 2025, pp. 16100. https://doi.org/10.1038/s41598-025-98498-8 T.-Y. Wang, M. Cheng, X. Wang, H.-R. Zhu, A. Huang, N. Zhang, X.-D. Hao, L.-T. Hao, C. Shi, Characteristics, impacts and high-efficiency treatment technologies for antibiotic residues in aquaculture wastewater: A review, SSRN Electronic Journal, 2024. https://doi.org/10.2139/ssrn.5046669 Y. Aissaoui, G. Jiménez-Skrzypek, J. GonzálezSálamo, M. Trabelsi-Ayadi, I. Ghorbel-Abid, J. Hernández-Borges, Determination of Multiclass Antibiotics in Fish Muscle Using a QuEChERSUHPLC-MS/MS Method, Foods, Vol. 13, No. 7, 2024, p. 1081. https://doi.org/10.3390/foods13071081 U. Salma, A. Hossain, M. Shafiujjaman, Y. Nishimura, M. Tokomura, R. Tanoue, T. Kunisue, K. Watanabe, M. Raknuzzaman, T. Amagai, M. Makino, Occurrence, risks, and mitigation of antibiotic pollution in Bangladeshi aquaculture systems, Environmental Chemistry & Ecotoxicology, Vol. 7, 2025, pp. 351-363. https://doi.org/10.1016/j.enceco.2025.01.007 D. Schar, E. Y. Klein, R. Laxminarayan, M. Gilbert, T. P. Van Boeckel, Global trends in antimicrobial use in aquaculture, Scientific Reports, Vol. 10, 2020, pp. 21878. https://doi.org/10.1038/s41598-020-78849-3 M. Pepi, S. Focardi, Antibiotic-resistant bacteria in aquaculture and climate change: A challenge for health in the Mediterranean area, International Journal of Environmental Research and Public Health, Vol. 18, No. 11, 2021, pp. 5723. https://doi.org/10.3390/ijerph18115723 B. Habibi, I. Ghorbel-Abid, R. Lahsini, D. Chehimi Ben Hassen, M. Trabelsi-Ayadi, Development and validation of a rapid HPLC method for multiresidue determination of erythromycin, clarithromycin, and azithromycin in aquaculture fish muscles, Acta Chromatographica, Vol. 31, No. 2, 2019, pp. 109–112. https://doi.org/10.1556/1326.2017.00376 F. Fenni, A. Sunyer-Caldú, H. Ben Mansour, M. S. Diaz-Cruz, Occurrence and risks of pharmaceuticals in Mahdia’s coastline (Tunisia): Distribution, antibiotic resistance, and ecotoxicological impact, Environmental Science and Pollution Research, Vol. 32, 2025, pp. 18419–18433. https://doi.org/10.1007/s11356- 025-36743-3 F. C. Cabello, H. P. Godfrey, A. H. Buschmann, H. J. Dölz, Aquaculture as yet another environmental gateway to the development and globalisation of antimicrobial resistance, The Lancet Infectious Diseases, Vol. 16, No. 7, 2016, pp. 127–133. https://doi.org/10.1016/S1473-3099(16)00100- 6 D. Coêlho de Sá Júnior, R. B. Vieira, G. U. de Souza Cruz, G. de A. L. F. Furtado, B. P. Oliveira, F. M. D. Bastos, I. F. Batista, V. C. O. Silva, C. A. de O. A. Neto, I. G. Santos, L. M. L. S. L. Costa, A. L. de P. M. Zanina, K. N. Marinho, L. G. Pereira, L. T. Tavares, M. E. S. Albuquerque, S. L. G. P. Cardoso, The impact of climate change on infectious diseases and antibiotic resistance, International Journal of Advanced Engineering Research and Science, Vol. 11, No. 2, 2024, pp. 14–18. https://doi.org/10.22161/ijaers.112.3 E. S. Okeke, K. I. Chukwudozie, R. Nyaruaba, R. E. Ita, A. Oladipo, O. Ejeromedoghene, E. O. Atakpa, C. V. Agu, C. O. Okoye, Antibiotic resistance in aquaculture and aquatic organisms: A review of current nanotechnology applications for sustainable management, Environmental Science and Pollution Research, Vol. 29, 2022, pp. 69241–69274. https://doi.org/10.1007/s11356-022-22319-y M. von Ahnen, K. Tang, I. van de Ven, A. C. Hambly, H. R. Andersen, N. Lorenzen, P. B. Pedersen, Removal of residual antibiotics from aquaculture effluents by denitrifying woodchip bioreactors, Aquaculture, Vol. 608, 2025, pp. 742761. https://doi.org/10.1016/j.aquaculture.2025.7427 61 Y. L. Shang, M. Huang, L. Zhao, P. He, Y. Liu, H. Pan, S. Cao, X. Liu, Adsorption performance and mechanisms of tetracycline on montmorillonite, ACS Omega, Vol. 9, No. 1, 2024, pp. 692–699. https://doi.org/10.1021/acsomega.3c06478 L. Mahouachi, T. Rastogi, W. Palm, I. GhorbelAbid, D. Chehimi Ben Hassen, K. Kümmerer, Natural clay as a sorbent to remove pharmaceutical micropollutants from wastewater, Chemosphere, Vol. 258, 2020, pp. 127213. https://doi.org/10.1016/j.chemosphere.2020.12 7213 H. Abd-ElFattah, R. Kamel, A. Maged, S. Kharbish, Harnessing clays and clay composites for efficient removal of pharmaceutical contaminants from water: A review, Frontiers in Scientific Research and Technology, Vol. 10, No. 1, 2025, pp. 85–100. https://doi.org/10.21608/fsrt.2025.344419.1143 G. G. Hacıosmanoğlu, C. Mejías, J. Martín, J. L. Santos, I. Aparicio, E. Alonso, Antibiotic adsorption by natural and modified clay minerals as designer adsorbents for wastewater treatment: A comprehensive review, Journal of Environmental Management, Vol. 317, 2022, pp. 115397. https://doi.org/10.1016/j.jenvman.2022.115397 G. E. P. Box, D. W. Behnken, Some new threelevel designs for the study of quantitative variables, Technometrics, Vol. 2, 1960, pp. 455– 475. https://doi.org/10.1080/00401706.1960.104899 12 I. Maldonado, A. P. Vega Quispe, M. Gutiérrez, Optimization of the elimination of antibiotics by Lemna gibba and Azolla filiculoides using response surface methodology, Frontiers in Environmental Science, Vol. 10, 2022, pp. 940971. https://doi.org/10.3389/fenvs.2022.940971 A. Kazemi, E. Ebrahimpour, M. Esmaeilbeigi, F. Gheitasi, F. Einollahipeer, M. Mohammadrezai, Optimizing oxytetracycline removal from aqueous solutions using activated carbon from barley lignocellulosic wastes: Isotherms and thermodynamic studies, Scientific Reports, Vol. 14, 2024, No. 21629. https://doi.org/10.1038/s41598-024-73142-z M. A. Zamiri, J. Wang, C. H. Niu, Competitive adsorption and molecular interaction study of sulfamethoxazole and trimethoprim on biomassbased activated carbon, Chemosphere, Vol. 385, 2025, No. 144591. https://doi.org/10.1016/j.chemosphere.2025.14 4591 S. Barakan, V. Aghazadeh, A. Samiee Beyragh, S. Mohammadi, Thermodynamic, kinetic and equilibrium isotherm studies of As(V) adsorption by Fe(III)-impregnated bentonite, Environment, Development and Sustainability, Vol. 22, 2020, pp. 5273–5295. https://doi.org/10.1007/s10668-019-00424-2 Ahmad Khan, Mohammad Saleem Akhtar, Saba Akbar, Khalid Saifullah Khan, Mazhar Iqbal, Ana Barrientos‑Velazquez, Youjun Deng, Effects of metal-polycation pillaring and exchangeable cations on aflatoxin adsorption by smectite, Clays and Clay Minerals, Vol. 70, No. 2, 2022, pp. 155–164. https://doi.org/10.1007/s42860-021-00159-0 C. J. Wang, Z. Li, W. T. Jiang, J. S. Jean, C. C. Liu, Cation exchange interaction between antibiotic ciprofloxacin and montmorillonite, Journal of Hazardous Materials, Vol. 183, 2010, pp. 309–314. https://doi.org/10.1016/j.jhazmat.2010.07.025 J. D. Russell, A. R. Fraser, Spectroscopic and chemical determinative methods, in Clay Mineralogy, Springer, 1994, pp. 11–67. https://doi.org/10.1007/978-94-011-0727-3_2 (text in Chinese) Y. J. Zhang, W. Y. Dong, H. Wang, G. K. Yan, Y. Chang, H. Wang, Y. Ling, Adsorption effect and mechanism of sulfamethoxazole and trimethoprim on corncob, Journal of Environmental Engineering Technology, Vol. 13, No. 3, 2023, pp. 1108– 1117. https://doi.org/10.12153/j.issn.1674- 991X.20220375 C. Mejías, J. L. Santos, J. Martín, I. Aparicio, E. Alonso, Thermodynamic and kinetic investigation of the adsorption and desorption of trimethoprim and its main metabolites in Mediterranean crop soils, Molecules, Vol. 28, No. 1, 2023, Article No. 437. https://doi.org/10.3390/molecules28010437 S. Jodeh, A. Jaber, G. Hanbali, Y. Massad, Z. S. Safi, S. Radi, V. Mehmeti, A. Berisha, S. Tighadouini, O. Dagdag, Experimental and theoretical study for removal of trimethoprim from wastewater using organically modified silica with pyrazole-3-carbaldehyde bridged to copper ions, BMC Chemistry, Vol. 16, 2022, p. 17. https://doi.org/10.1186/s13065-022-00814- 0 T. De Oliveira, E. Fernandez, L. Fougère, E. Destandau, M. Boussafir, M. Sohmiya, Y. Sugahara, R. Guégan, Competitive association of antibiotics with a clay mineral and organoclay derivatives as a control of their lifetimes in the environment, ACS Omega, Vol. 3, No. 11, 2018, pp. 15332–15342. https://doi.org/10.1021/acsomega.8b02049 S. Chianese, A. Fenti, J. Blotevogel, D. Musmarra, P. Iovino, Trimethoprim removal from wastewater: Adsorption and electrooxidation comparative case study, Case Studies in Chemical and Environmental Engineering, Vol. 8, 2023, p. 100433. https://doi.org/10.1016/j.cscee.2023.100433 R. Li, W. Sun, L. Xia, Z. U., X. Sun, Z. Wang, Y. Wang, X. Deng, Adsorption of Toxic Tetracycline, Thiamphenicol and Sulfamethoxazole by a Granular Activated Carbon (GAC) under Different Conditions, Molecules, Vol. 27, No. 22, 2022, p. 7980. https://doi.org/10.3390/molecules27227980 R. Lavecchia, A. Zuorro, O. Baaloudj, M. Brienza, Trimethoprim removal from aqueous solutions via volcanic ash-soil adsorption: process modeling and optimization, Water, Vol. 16, No. 15, 2024, p. 2209. https://doi.org/10.3390/w16152209 J. Berges, S. Moles, M. P. Ormad, R. Mosteo, J. Gómez, Antibiotics removal from aquatic environments: Adsorption of enrofloxacin, trimethoprim, sulfadiazine, and amoxicillin on vegetal powdered activated carbon, Environmental Science and Pollution Research, Vol. 28, 2021, pp. 8442–8452. https://doi.org/10.1007/s11356-020-10972-0 A. Mirzaei, L. Yerushalmi, Z. Chen, F. Haghighat, Photocatalytic degradation of sulfamethoxazole by hierarchical magnetic ZnO@g-C₃N₄: RSM optimization, kinetic study, reaction pathway and toxicity evaluation, Journal of Hazardous Materials, Vol. 359, 2018, pp. 516–526. https://doi.org/10.1016/j.jhazmat.2018.07.077 Y. Ou, X. Zhang, H. Li, L. Wang, Magnetically separable Fe-MIL-88B_NH₂ carbonaceous nanocomposites for efficient removal of sulfamethoxazole from aqueous solutions, Journal of Colloid and Interface Science, Vol. 570, 2020, pp. 163–172. https://doi.org/10.1016/j.jcis.2020.02.116 Y. He, C. Liu, X-Yu. Tang, Q-S. Xian, J-Q. Zhang, Z. Guan, Biochar impacts on sorptiondesorption of oxytetracycline and florfenicol in an alkaline farmland soil as affected by field ageing, Science of The Total Environment, Vol. 671, 2019, pp. 928-936. https://doi.org/10.1016/j.scitotenv.2019.03.414