Abstract
This study presents the main results about the removal of the antibiotic cefotaxime (CTX) under simulated sunlight radiation using heterogeneous photocatalysis with titanium dioxide (TiO2) and zinc oxide (ZnO) in aqueous solutions. The effects of pH and catalyst initial load on pollutant removal were assessed considering the response surface methodology and a central composite circumscribed experimental design, which allowed to determine the optimized conditions that lead to a higher substrate elimination. Experimental results indicated that evaluated parameters have a significant effect on antibiotic removal in both TiO2 and ZnO suspensions. In addition, the role of photogenerated holes, hydroxyl, and superoxide anion radicals on CTX degradation was evaluated to clarify the reaction mechanism. Finally, analysis of the dissolved organic carbon content in solutions and the antibacterial activity of treated samples showed that photocatalytic treatments were able to reduce a considerable portion of the organic matter present in the systems and its antimicrobial activity.
This is a preview of subscription content, log in via an institution to check access.
Similar content being viewed by others
References
Affam, A. C., & Chaudhuri, M. (2013). Degradation of pesticides chlorpyrifos, cypermethrin and chlorothalonil in aqueous solution by TiO2 photocatalysis. Journal of Environmental Management, 130, 160–165. https://doi.org/10.1016/j.jenvman.2013.08.058.
Borges, M. E., Sierra, M., Cuevas, E., García, R. D., & Esparza, P. (2016). Photocatalysis with solar energy: sunlight-responsive photocatalyst based on TiO2 loaded on a natural material for wastewater treatment. Solar Energy, 135, 527–535. https://doi.org/10.1016/j.solener.2016.06.022.
Chen, Y., Yang, S., Wang, K., & Lou, L. (2005). Role of primary active species and TiO2 surface characteristic in UV-illuminated photodegradation of Acid Orange 7. Journal of Photochemistry and Photobiology A: Chemistry, 172(1), 47–54. https://doi.org/10.1016/j.jphotochem.2004.11.006.
Cheng, M., Zeng, G., Huang, D., Lai, C., Xu, P., Zhang, C., & Liu, Y. (2015). Hydroxyl radicals based advanced oxidation processes (AOPs) for remediation of soils contaminated with organic compounds: a review. Chemical Engineering Journal, 284, 582–598. https://doi.org/10.1016/j.cej.2015.09.001.
Daneshvar, N., Salari, D., & Khataee, A. (2004). Photocatalytic degradation of azo dye acid red 14 in water on ZnO as an alternative catalyst to TiO2. Journal of Photochemistry and Photobiology A: Chemistry, 162(2), 317–322. https://doi.org/10.1016/S1010-6030(03)00378-2.
Dhatshanamurthi, P., Shanthi, M., & Swaminathan, M. (2017). An efficient pilot scale solar treatment method for dye industry effluent using nano-ZnO. Journal of Water Process Engineering, 16, 28–34. https://doi.org/10.1016/j.jwpe.2016.12.002.
Dimitrakopoulou, D., Rethemiotaki, I., Frontistis, Z., Xekoukoulotakis, N. P., Venieri, D., & Mantzavinos, D. (2012). Degradation, mineralization and antibiotic inactivation of amoxicillin by UV-A/TiO2 photocatalysis. Journal of Environmental Management, 98, 168–174. https://doi.org/10.1016/j.jenvman.2012.01.010.
Giraldo, A. L., Peñuela, G. A., Torres-Palma, R. A., Pino, N. J., Palominos, R. A., & Mansilla, H. D. (2010). Degradation of the antibiotic oxolinic acid by photocatalysis with TiO2 in suspension. Water Research, 44(18), 5158–5167. https://doi.org/10.1016/j.watres.2010.05.011.
Ji, G., Zhang, B., & Wu, Y. (2012). Combined ultrasound/ozone degradation of carbazole in APG1214 surfactant solution. Journal of Hazardous Materials, 225–226, 1–7. https://doi.org/10.1016/j.jhazmat.2012.02.044.
Leal, J. F., Henriques, I. S., Correia, A., Santos, E. B. H., & Esteves, V. I. (2017). Antibacterial activity of oxytetracycline photoproducts in marine aquaculture’s water. Environmental Pollution, 220, 644–649. https://doi.org/10.1016/j.envpol.2016.10.021.
Li, B., & Zhang, T. (2013). Different removal behaviours of multiple trace antibiotics in municipal wastewater chlorination. Water Research, 47(9), 2970–2982. https://doi.org/10.1016/j.watres.2013.03.001.
Li, D., Zhu, Q., Han, C., Yang, Y., Jiang, W., & Zhang, Z. (2015). Photocatalytic degradation of recalcitrant organic pollutants in water using a novel cylindrical multi-column photoreactor packed with TiO2-coated silica gel beads. Journal of Hazardous Materials, 285, 398–408. https://doi.org/10.1016/j.jhazmat.2014.12.024.
Lima, M. J., Silva, C. G., Silva, A. M. T., Lopes, J. C. B., Dias, M. M., & Faria, J. L. (2017). Homogeneous and heterogeneous photo-Fenton degradation of antibiotics using an innovative static mixer photoreactor. Chemical Engineering Journal, 310, 342–351. https://doi.org/10.1016/j.cej.2016.04.032.
Lin, Y., Ferronato, C., Deng, N., Wu, F., & Chovelon, J.-M. (2009). Photocatalytic degradation of methylparaben by TiO2: Multivariable experimental design and mechanism. Applied Catalysis B: Environmental, 88(1–2), 32–41. https://doi.org/10.1016/j.apcatb.2008.09.026.
Lin, Y., Ferronato, C., Deng, N., & Chovelon, J.-M. (2011). Study of benzylparaben photocatalytic degradation by TiO2. Applied Catalysis B: Environmental, 104(3–4), 353–360. https://doi.org/10.1016/j.apcatb.2011.03.006.
Lopez-Alvarez, B., Torres-Palma, R. A., & Peñuela, G. (2011). Solar photocatalitycal treatment of carbofuran at lab and pilot scale: effect of classical parameters, evaluation of the toxicity and analysis of organic by-products. Journal of Hazardous Materials, 191(1–3), 196–203. https://doi.org/10.1016/j.jhazmat.2011.04.060.
Michael, I., Rizzo, L., McArdell, C. S., Manaia, C. M., Merlin, C., Schwartz, T., et al. (2013). Urban wastewater treatment plants as hotspots for the release of antibiotics in the environment: A review. Water Research, 47(3), 957–995. https://doi.org/10.1016/j.watres.2012.11.027.
Miranda-García, N., Suárez, S., Sánchez, B., Coronado, J. M., Malato, S., & Maldonado, M. I. (2011). Photocatalytic degradation of emerging contaminants in municipal wastewater treatment plant effluents using immobilized TiO2 in a solar pilot plant. Applied Catalysis B: Environmental, 103(3–4), 294–301. https://doi.org/10.1016/j.apcatb.2011.01.030.
Moctezuma, E., Leyva, E., Aguilar, C. A., Luna, R. A., & Montalvo, C. (2012). Photocatalytic degradation of paracetamol: intermediates and total reaction mechanism. Journal of Hazardous Materials, 243, 130–138. https://doi.org/10.1016/j.jhazmat.2012.10.010.
Palominos, R. A., Mondaca, M. A., Giraldo, A., Peñuela, G., Pérez-Moya, M., & Mansilla, H. D. (2009). Photocatalytic oxidation of the antibiotic tetracycline on TiO2 and ZnO suspensions. Catalysis Today, 144(1), 100–105. https://doi.org/10.1016/j.cattod.2008.12.031.
Rahul, Jyoti, S., Naz, F., & Siddique, Y. H. (2015). Evaluation of the toxic potential of cefotaxime in the third instar larvae of transgenic Drosophila melanogaster. Chemico-Biological Interactions, 233, 71–80. https://doi.org/10.1016/j.cbi.2015.03.004.
Raja, P., Bozzi, A., Mansilla, H., & Kiwi, J. (2005). Evidence for superoxide-radical anion, singlet oxygen and OH-radical intervention during the degradation of the lignin model compound (3-methoxy-4-hydroxyphenylmethylcarbinol). Journal of Photochemistry and Photobiology A: Chemistry, 169(3), 271–278. https://doi.org/10.1016/j.jphotochem.2004.07.009.
Ribeiro, A. R., & Schmidt, T. C. (2017). Determination of acid dissociation constants (pKa) of cephalosporin antibiotics: computational and experimental approaches. Chemosphere, 169, 524–533. https://doi.org/10.1016/j.chemosphere.2016.11.097.
Rodriguez-Mozaz, S., Chamorro, S., Marti, E., Huerta, B., Gros, M., Sànchez-Melsió, A., et al. (2015). Occurrence of antibiotics and antibiotic resistance genes in hospital and urban wastewaters and their impact on the receiving river. Water Research, 69, 234–242. https://doi.org/10.1016/j.watres.2014.11.021.
Rossmann, J., Schubert, S., Gurke, R., Oertel, R., & Kirch, W. (2014). Simultaneous determination of most prescribed antibiotics in multiple urban wastewater by SPE-LC–MS/MS. Journal of Chromatography B, 969, 162–170. https://doi.org/10.1016/j.jchromb.2014.08.008.
Saitoh, T., & Shibayama, T. (2016). Removal and degradation of β-lactam antibiotics in water using didodecyldimethylammonium bromide-modified montmorillonite organoclay. Journal of Hazardous Materials, 317, 677–685. https://doi.org/10.1016/j.jhazmat.2016.06.003.
Sojic, D. V., Anderluh, V. B., Orcic, D. Z., & Abramovic, B. F. (2009). Photodegradation of clopyralid in TiO2 suspensions: identification of intermediates and reaction pathways, 168, 94–101. doi:https://doi.org/10.1016/j.jhazmat.2009.01.134.
Tai, C., Peng, J.-F., Liu, J.-F., Jiang, G.-B., & Zou, H. (2004). Determination of hydroxyl radicals in advanced oxidation processes with dimethyl sulfoxide trapping and liquid chromatography. Analytica Chimica Acta, 527(1), 73–80. https://doi.org/10.1016/j.aca.2004.08.019.
Yu, X., Tang, X., Zuo, J., Zhang, M., Chen, L., & Li, Z. (2016). Distribution and persistence of cephalosporins in cephalosporin producing wastewater using SPE and UPLC-MS/MS method. Science of the Total Environment, 569, 23–30. https://doi.org/10.1016/j.scitotenv.2016.06.113.
Zhu, L., Santiago-Schübel, B., Xiao, H., Hollert, H., & Kueppers, S. (2016). Electrochemical oxidation of fluoroquinolone antibiotics: mechanism, residual antibacterial activity and toxicity change. Water Research, 102, 52–62. https://doi.org/10.1016/j.watres.2016.06.005.
Zúñiga-Benítez, H., & Peñuela, G. A. (2016). Methylparaben removal using heterogeneous photocatalysis: effect of operational parameters and mineralization/biodegradability studies. Environmental Science and Pollution Research. 1–9. doi:https://doi.org/10.1007/s11356-016-6468-9.
Zúñiga-Benítez, H., Soltan, J., & Peñuela, G. A. (2016). Application of ultrasound for degradation of benzophenone-3 in aqueous solutions. International journal of Environmental Science and Technology, 13(1), 77–86. https://doi.org/10.1007/s13762-015-0842-x.
Acknowledgements
Authors want to thank FONDECYT (Chile, Grant 1080230), “Fondo de Sostenibilidad 2016-2017” Vicerrectoría de Investigación Universidad de Antioquia and the Alpha Network on Sustainable Technologies for Drinking and Wastewater Treatment (TECSPAR) for support this work. Dr. Zúñiga-Benítez thanks COLCIENCIAS (Colombia) for support his doctoral studies.
Author information
Authors and Affiliations
Corresponding author
Rights and permissions
About this article
Cite this article
León, D.E., Zúñiga-Benítez, H., Peñuela, G.A. et al. Photocatalytic Removal of the Antibiotic Cefotaxime on TiO2 and ZnO Suspensions Under Simulated Sunlight Radiation. Water Air Soil Pollut 228, 361 (2017). https://doi.org/10.1007/s11270-017-3557-4
Received:
Accepted:
Published:
DOI: https://doi.org/10.1007/s11270-017-3557-4