Abstract
Oxytetracycline (OTC) is listed as an emerging contaminant due to the adverse effects that it has on human health and the environment. Being a broad spectrum antibiotic, OTC is widely used and is found in large concentrations in wastewater. Advanced wastewater treatment is an effective method for the removal of this pollutant; however, these tertiary treatments are expensive and generally not applied in nondeveloped countries. In this work, the removal of OTC by adsorption using sustainable materials synthesized from hydroxyapatite (HA) and aluminosilicates by chemical precipitation method was performed. Four different adsorbent materials were obtained: mixing hydroxyapatite and kaolin (HA-K), hydroxyapatite with natural clay (HA-NC), hydroxyapatite with synthetic zeolite (HA-SZ), and hydroxyapatite with natural aluminosilicates (HA-NA). The adsorbent materials were characterized by FT-IR, pHpzc, cation exchange capacity (CEC), SEM/EDX, TEM (particle size), and XRD. Kinetic tests and adsorption isotherms of OTC were carried out by varying conditions of the aqueous media as pH value, temperature, and the presence of ionic strength. Different kinetic and isothermal models were applied to the obtained data. All the synthesized materials showed an acceptable sorption capacity for OTC removal. The elimination of this antibiotic was greater than 50% in the four synthesized materials. Experimental data showed a better fit to the Elovich kinetic model, indicative of a heterogeneous chemical sorption process. Kinetic and thermodynamic parameters showed that the synthetized materials from HA and aluminosilicates are potential and alternative adsorbent materials for OTC removal from water.
This is a preview of subscription content, log in via an institution to check access.
Similar content being viewed by others
References
Ahmaruzzaman, M. (2008). Adsorption of phenolic compounds on low-cost adsorbents: a review. Advances in Colloid and Interface Science, 143(1–2), 48–67. https://doi.org/10.1016/j.cis.2008.07.002.
Annamalai, J., & Namasivayam, V. (2015). Endocrine disrupting chemicals in the atmosphere: their effects on humans and wildlife. Environment International, 76, 78–97. https://doi.org/10.1016/j.envint.2014.12.006.
Appel, C., Ma, L. Q., Rhue, R. D., & Kennelley, E. (2003). Point of zero charge determination in soils and minerals via traditional methods and detection of electroacoustic mobility. Geoderma, 113(1–2), 77–93. https://doi.org/10.1016/S0016-7061(02)00316-6.
Atta, A. Y., Jibril, B. Y., Aderemi, B. O., & Adefila, S. S. (2012). Preparation of analcime from local kaolin and rice husk ash. Applied Clay Science, 61, 8–13. https://doi.org/10.1016/j.clay.2012.02.018.
Barrer, R. M., Papadopoulos, R., & Rees, L. V. C. (1967). Exchange of sodium in clinoptilolite by organic cations. Journal of Inorganic and Nuclear Chemistry, 29(8), 2047–2063. https://doi.org/10.1016/0022-1902(67)80466-4.
Carvajal Taborda, E. E., Días Forero, J. H., & Espitia Rico, M. (2013). Simulación Del Espectro Epr Del Radical Co2. Redes de Ingeniería, 4, 31. https://doi.org/10.14483/2248762x.6365.
Chang, P. H., Jean, J. S., Jiang, W. T., & Li, Z. (2009). Mechanism of tetracycline sorption on rectorite. Colloids and Surfaces A: Physicochemical and Engineering Aspects, 339(1–3), 94–99. https://doi.org/10.1016/j.colsurfa.2009.02.002.
Christelle, B. (2005). Contribution À L’Étude De L’Activation Thermique Du Kaolin : Évolution De La Structure Cristallographique Et Activité Pouzzolanique, 96–98 pp.
Cortés-Martinez, R., Martínez-Miranda, V., Solache-Ríos, M., & García-Sosa, I. (2004). Evaluation of natural and surfactant - modified zeolites in the removal of cadmium from aqueous solutions. Separation Science and Technology, 39(11), 2711–2730. https://doi.org/10.1081/SS-200026766.
Crespo-Alonso, M., Nurchi, V. M., Biesuz, R., Alberti, G., Spano, N., Pilo, M. I., & Sanna, G. (2013). Biomass against emerging pollution in wastewater: ability of cork for the removal of ofloxacin from aqueous solutions at different pH. Journal of Environmental Chemical Engineering, 1(4), 1199–1204. https://doi.org/10.1016/j.jece.2013.09.010.
Demirci, S., Ustaoǧlu, Z., Yilmazer, G. A., Sahin, F., & Baç, N. (2014). Antimicrobial properties of zeolite-X and zeolite-A ion-exchanged with silver, copper, and zinc against a broad range of microorganisms. Applied Biochemistry and Biotechnology, 172(3), 1652–1662. https://doi.org/10.1007/s12010-013-0647-7.
Earl, J. S., Wood, D. J., & Milne, S. J. (2006). Hydrothermal synthesis of hydroxyapatite. Journal of Physics: Conference Series, 26(1), 268–271. https://doi.org/10.1088/1742-6596/26/1/064.
Ersan, M., Guler, U. A., Acikel, U., & Sarioglu, M. (2015). Synthesis of hydroxyapatite/clay and hydroxyapatite/pumice composites for tetracycline removal from aqueous solutions. Process Safety and Environmental Protection, 96, 22–32. https://doi.org/10.1016/j.psep.2015.04.001.
Faria, P., Orfao, J., & Pereira, M. (2004). Adsorption of anionic and cationic dyes on activated carbons with different surface chemistries. Water Research, 38(8), 2043–2052. https://doi.org/10.1016/j.watres.2004.01.034.
Figueroa, R. A., Leonard, A., & Mackay, A. A. (2004). Modeling tetracycline antibiotic sorption to clays. Environmental Science and Technology, 38(2), 476–483. https://doi.org/10.1021/es0342087.
Foo, K. Y., & Hameed, B. H. (2010). Insights into the modeling of adsorption isotherm systems. Chemical Engineering Journal, 156(1), 2–10. https://doi.org/10.1016/j.cej.2009.09.013.
Garibay-Alvarado, J. A., Espinosa-Cristóbal, F., & Reyes-López, S. Y. (2017). Fibrous silica-hydroxyapatite composite by electrospinning. International Journal of Research-Granthaalayah, 5, 39–47. https://doi.org/10.5281/zenodo.345439.
Gillman, G. P., & Sumpter, E. A. (1986). Modification to the compulsive exchange method for measuring exchange characteristics of soils. Australian Journal of Soil Research, 24(1), 61–66. https://doi.org/10.1071/SR9860061.
Gu, C., & Karthikeyan, K. G. (2008). Sorption of the antibiotic tetracycline to humic-mineral complexes. Journal of Environmental Quality, 37(2), 704–711. https://doi.org/10.2134/jeq2007.0030.
Gu, C., Karthikeyan, K. G., Sibley, S. D., & Pedersen, J. A. (2007). Complexation of the antibiotic tetracycline with humic acid. Chemosphere, 66(8), 1494–1501. https://doi.org/10.1016/j.chemosphere.2006.08.028.
Harja, M., & Ciobanu, G. (2018). Studies on adsorption of oxytetracycline from aqueous solutions onto hydroxyapatite. Science of the Total Environment, 628–629, 36–43. https://doi.org/10.1016/j.scitotenv.2018.02.027.
Hejazifar, M., & Azizian, S. (2012). Adsorption of cationic and anionic dyes onto the activated carbon prepared from grapevine rhytidome. Journal of Dispersion Science and Technology, 33(6), 846–853. https://doi.org/10.1080/01932691.2011.579861.
Ho, Y. S., & McKay, G. (2000). The kinetics of sorption of divalent metal ions onto sphagnum moss peat. Water Research, 34(3), 735–742. https://doi.org/10.1016/S0043-1354(99)00232-8.
Huang, W., Peng, P., Yu, Z., & Fu, J. (2003). Effects of organic matter heterogeneity on sorption and desorption of organic contaminants by soils and sediments. Applied Geochemistry, 18(7), 955–972. https://doi.org/10.1016/S0883-2927(02)00205-6.
Huerta, B., Jakimska, A., Llorca, M., Ruhí, A., Margoutidis, G., Acuña, V., et al. (2015). Development of an extraction and purification method for the determination of multi-class pharmaceuticals and endocrine disruptors in freshwater invertebrates. Talanta, 132, 373–381. https://doi.org/10.1016/j.talanta.2014.09.017.
Islam, M., & Patel, R. K. (2007). Evaluation of removal efficiency of fluoride from aqueous solution using quick lime. Journal of Hazardous Materials, 143(1–2), 303–310. https://doi.org/10.1016/j.jhazmat.2006.09.030.
Jia, M., Wang, F., Bian, Y., Jin, X., Song, Y., Kengara, F. O., et al. (2013). Effects of pH and metal ions on oxytetracycline sorption to maize-straw-derived biochar. Bioresource Technology, 136, 87–93. https://doi.org/10.1016/j.biortech.2013.02.098.
Juan, R., Hernández, S., Andrés, J. M., & Ruiz, C. (2007). Synthesis of granular zeolitic materials with high cation exchange capacity from agglomerated coal fly ash. Fuel, 86(12–13), 1811–1821. https://doi.org/10.1016/j.fuel.2007.01.011.
Khan, A. A., & Singh, R. P. (1987). Adsorption thermodynamics of carbofuran on Sn (IV) arsenosilicate in H+, Na+ and Ca2+ forms. Colloids and Surfaces, 24(1), 33–42. https://doi.org/10.1016/0166-6622(87)80259-7.
Kithome, M., Paul, J. W., Lavkulich, L. M., & Bomke, A. A. (1998). Kinetics of ammonium adsorption and desorption by the natural zeolite clinoptilolite. Soil Science Society of America Journal, 62(3), 622–629. https://doi.org/10.2136/sssaj1998.03615995006200030011x.
Kuśnieruk, S., Wojnarowicz, J., Chodara, A., Chudoba, T., Gierlotka, S., & Lojkowski, W. (2016). Influence of hydrothermal synthesis parameters on the properties of hydroxyapatite nanoparticles. Beilstein Journal of Nanotechnology, 7(1), 1586–1601. https://doi.org/10.3762/bjnano.7.153.
Li, Z., Chang, P. H., Jean, J. S., Jiang, W. T., & Wang, C. J. (2010). Interaction between tetracycline and smectite in aqueous solution. Journal of Colloid and Interface Science, 341(2), 311–319. https://doi.org/10.1016/j.jcis.2009.09.054.
Li, G., Zhang, D., Wang, M., Huang, J., & Huang, L. (2013). Preparation of activated carbons from Iris tectorum employing ferric nitrate as dopant for removal of tetracycline from aqueous solutions. Ecotoxicology and Environmental Safety, 98, 273–282. https://doi.org/10.1016/j.ecoenv.2013.08.015.
Li, Y., Wang, S., Zhang, Y., Han, R., & Wei, W. (2017). Enhanced tetracycline adsorption onto hydroxyapatite by Fe(III) incorporation. Journal of Molecular Liquids, 247, 171–181. https://doi.org/10.1016/j.molliq.2017.09.110.
Li, Z. J., Qi, W. N., Feng, Y., Liu, Y. W., Ebrahim, S., & Long, J. (2019). Degradation mechanisms of oxytetracycline in the environment. Journal of Integrative Agriculture, 18(9), 1953–1960. https://doi.org/10.1016/S2095-3119(18)62121-5.
Liu, X., Zhang, H., Luo, Y., Zhu, R., Wang, H., & Huang, B. (2020). Sorption of oxytetracycline in particulate organic matter in soils and sediments: roles of pH, ionic strength and temperature. Science of the Total Environment, 714, 136628. https://doi.org/10.1016/j.scitotenv.2020.136628.
Luan, Z., & Fournier, J. A. (2005). In situ FTIR spectroscopic investigation of active sites and adsorbate interactions in mesoporous aluminosilicate SBA-15 molecular sieves. Microporous and Mesoporous Materials, 79(1–3), 235–240. https://doi.org/10.1016/j.micromeso.2004.11.012.
Luo, P., & Nieh, T. G. (1996). Preparing hydroxyapatite powders with controlled morphology. Biomaterials, 17(20), 1959–1964. https://doi.org/10.1016/0142-9612(96)00019-1.
Lyal’ko, I. S., Kaplichnyi, V. N., Shulyak, E. A., Gurin, V. S., Shapovalov, E. A., Savukov, V. T., & Stoyanov, P. A. (1981). Em-125 transmission electron microscope. Bulletin of the Academy of Sciences of the U.S.S.R. Physical Series, 47(6), 13–15.
Madejová, J. (2003). FTIR techniques in clay mineral studies. Vibrational Spectroscopy, 31(1), 1–10. https://doi.org/10.1016/S0924-2031(02)00065-6.
Miraboutalebi, S. M., Nikouzad, S. K., Peydayesh, M., Allahgholi, N., Vafajoo, L., & McKay, G. (2017). Methylene blue adsorption via maize silk powder: kinetic, equilibrium, thermodynamic studies and residual error analysis. Process Safety and Environmental Protection, 106, 191–202. https://doi.org/10.1016/j.psep.2017.01.010.
Mondale, K. D., Carland, R. M., & Aplan, F. F. (1995). The comparative ion exchange capacities of natural sedimentary and synthetic zeolites. Minerals Engineering, 8(4–5), 535–548. https://doi.org/10.1016/0892-6875(95)00015-I.
Mourabet, M., El Rhilassi, A., El Boujaady, H., Bennani-Ziatni, M., El Hamri, R., & Taitai, A. (2015). Removal of fluoride from aqueous solution by adsorption on hydroxyapatite (HAp) using response surface methodology. Journal of Saudi Chemical Society, 19(6), 603–615. https://doi.org/10.1016/j.jscs.2012.03.003.
Pan, X. D., Wu, P. G., Jiang, W., & Ma, B. J. (2015). Determination of chloramphenicol, thiamphenicol, and florfenicol in fish muscle by matrix solid-phase dispersion extraction (MSPD) and ultra-high pressure liquid chromatography tandem mass spectrometry. Food Control, 52, 34–38. https://doi.org/10.1016/j.foodcont.2014.12.019.
Panda, R. N., Hsieh, M. F., Chung, R. J., & Chin, T. S. (2003). FTIR, XRD, SEM and solid state NMR investigations of carbonate-containing hydroxyapatite nano-particles synthesized by hydroxide-gel technique. Journal of Physics and Chemistry of Solids, 64(2), 193–199. https://doi.org/10.1016/S0022-3697(02)00257-3.
Pyrz, W. D., & Buttrey, D. J. (2008). Particle size determination using TEM: a discussion of image acquisition and analysis for the novice microscopist. Langmuir, 24(20), 11350–11360. https://doi.org/10.1021/la801367j.
Qiu, H., Lv, L., Pan, B. C., Zhang, Q. J., Zhang, W. M., & Zhang, Q. X. (2009). Critical review in adsorption kinetic models. Journal of Zhejiang University: Science A, 10(5), 716–724. https://doi.org/10.1631/jzus.A0820524.
Reyes López, S. Y., Rodríguez, J. S., & Sueyoshi, S. S. (2013). Microstructural characterization of sanitaryware, the relationship spinel and mullite. Journal of Ceramic Processing Research, 14(4), 492–497.
Richardson, S. D., & Ternes, T. A. (2014). Water analysis: emerging contaminants and current issues. Analytical Chemistry, 86(6), 2813–2848. https://doi.org/10.1021/ac500508t.
Roque-Ruiz, J. H., Cabrera-Ontiveros, E. A., González-García, G., & Reyes-López, S. Y. (2016). Thermal degradation of aluminum formate sol-gel; synthesis of α-alumina and characterization by 1H, 13C and 27Al MAS NMR and XRD spectroscopy. Results in Physics, 6, 1096–1102. https://doi.org/10.1016/j.rinp.2016.11.052.
Ruhí, A., Acuña, V., Barceló, D., Huerta, B., Mor, J. R., Rodríguez-Mozaz, S., & Sabater, S. (2016). Bioaccumulation and trophic magnification of pharmaceuticals and endocrine disruptors in a Mediterranean river food web. Science of the Total Environment, 540, 250–259. https://doi.org/10.1016/j.scitotenv.2015.06.009.
Ruíz-Baltazar, Á. D. J., Reyes-López, S. Y., Silva-Holguin, P. N., Larrañaga, D., Estévez, M., & Pérez, R. (2018). Novel biosynthesis of Ag-hydroxyapatite: structural and spectroscopic characterization. Results in Physics, 9, 593–597. https://doi.org/10.1016/j.rinp.2018.03.016.
Sassman, S. A., & Lee, L. S. (2005). Sorption of three tetracyclines by several soils: assessing the role of pH and cation exchange. Environmental Science and Technology, 39(19), 7452–7459. https://doi.org/10.1021/es0480217.
Sharma, V. K., Johnson, N., Cizmas, L., McDonald, T. J., & Kim, H. (2016). A review of the influence of treatment strategies on antibiotic resistant bacteria and antibiotic resistance genes. Chemosphere, 150, 702–714. https://doi.org/10.1016/j.chemosphere.2015.12.084.
Shi, Z., Huang, X., Cai, Y., Tang, R., & Yang, D. (2009). Size effect of hydroxyapatite nanoparticles on proliferation and apoptosis of osteoblast-like cells. Acta Biomaterialia, 5(1), 338–345. https://doi.org/10.1016/j.actbio.2008.07.023.
Smoleń, D., Chudoba, T., Gierlotka, S., Kedzierska, A., Łojkowski, W., Sobczak, K., et al. (2012). Hydroxyapatite nanopowder synthesis with a programmed resorption rate. Journal of Nanomaterials, 2012. https://doi.org/10.1155/2012/841971.
Soria-Serna, L. A., Torres-Pérez, J., & Reyes-López, S. Y. (2018). Tetracycline adsorption on steam alternative activated carbon: kinetic and thermodynamic parameters. Desalination and Water Treatment, 114, 307–312. https://doi.org/10.5004/dwt.2018.22313.
Tan, I. A. W., Ahmad, A. L., & Hameed, B. H. (2008). Adsorption of basic dye on high-surface-area activated carbon prepared from coconut husk: equilibrium, kinetic and thermodynamic studies. Journal of Hazardous Materials, 154(1–3), 337–346. https://doi.org/10.1016/j.jhazmat.2007.10.031.
Tironi, A., Trezza, M. A., Irassar, E. F., & Scian, A. N. (2012). Thermal treatment of kaolin: effect on the pozzolanic activity. Procedia Materials Science, 1, 343–350. https://doi.org/10.1016/j.mspro.2012.06.046.
Torres-Perez, J., Gerente, C., & Andres, Y. (2012). Conversion of agricultural residues into activated carbons for water purification: application to arsenate removal. Journal of Environmental Science and Health - Part A Toxic/Hazardous Substances and Environmental Engineering, 47(8). https://doi.org/10.1080/10934529.2012.668390.
Torres-Pérez, J., Gérente, C., & Andrès, Y. (2012). Sustainable activated carbons from agricultural residues dedicated to antibiotic removal by adsorption. Chinese Journal of Chemical Engineering, 20(3). https://doi.org/10.1016/S1004-9541(11)60214-0.
Vadivelan, V., & Vasanth Kumar, K. (2005). Equilibrium, kinetics, mechanism, and process design for the sorption of methylene blue onto rice husk. Journal of Colloid and Interface Science, 286(1), 90–100. https://doi.org/10.1016/j.jcis.2005.01.007.
Wang, K., & Xing, B. (2005). Structural and sorption characteristics of adsorbed humic acid on clay minerals. Journal of Environmental Quality, 34(1), 342–349. https://doi.org/10.2134/jeq2005.0342.
Wang, Y., Chen, N., Wei, W., Cui, J., & Wei, Z. (2011). Enhanced adsorption of fluoride from aqueous solution onto nanosized hydroxyapatite by low-molecular-weight organic acids. Desalination, 276(1–3), 161–168. https://doi.org/10.1016/j.desal.2011.03.033.
Wei, W., Yang, L., Zhong, W., Cui, J., & Wei, Z. (2015). Mechanism of enhanced humic acid removal from aqueous solution using poorly crystalline hydroxyapatite nanoparticles. Digest Journal of Nanomaterials and Biostructures, 10(2), 663–680.
Yu, B., Bai, Y., Ming, Z., Yang, H., Chen, L., Hu, X., et al. (2017). Adsorption behaviors of tetracycline on magnetic graphene oxide sponge. Materials Chemistry and Physics, 198, 283–290. https://doi.org/10.1016/j.matchemphys.2017.05.042.
Zhao, Y., Geng, J., Wang, X., Gu, X., & Gao, S. (2011). Adsorption of tetracycline onto goethite in the presence of metal cations and humic substances. Journal of Colloid and Interface Science, 361(1), 247–251. https://doi.org/10.1016/j.jcis.2011.05.051.
Zhao, Y., Gu, X., Gao, S., Geng, J., & Wang, X. (2012). Adsorption of tetracycline (TC) onto montmorillonite: cations and humic acid effects. Geoderma, 183–184, 12–18. https://doi.org/10.1016/j.geoderma.2012.03.004.
Zhu, X., Liu, Y., Qian, F., Zhou, C., Zhang, S., & Chen, J. (2014). Preparation of magnetic porous carbon from waste hydrochar by simultaneous activation and magnetization for tetracycline removal. Bioresource Technology, 154, 209–214. https://doi.org/10.1016/j.biortech.2013.12.019.
Funding
This work was supported by the FOMIX-CONACYT (Mexico), under grant number CHIH-2012-C03-194671; PROMEP-SEP (Mexico) under grant number 103.5/12/3457; and CONACYT-Mexico for the scholarship for Alicia Martínez-Olivas.
Author information
Authors and Affiliations
Contributions
Alicia Martínez-Olivas: methodology, investigation, and writing—original draft. Jonatan Torres-Pérez: conceptualization, resources, writing—original draft, and funding acquisition. Patricia Balderas-Hernández: writing—review and editing. Simón Yobanny Reyes-López: writing—review and editing.
Corresponding author
Ethics declarations
Conflict of Interest
The authors declare that they have no conflicts of interest.
Additional information
Publisher’s Note
Springer Nature remains neutral with regard to jurisdictional claims in published maps and institutional affiliations.
Rights and permissions
About this article
Cite this article
Martínez-Olivas, A., Torres-Pérez, J., Balderas-Hernández, P. et al. Oxytetracycline Sorption onto Synthetized Materials from Hydroxyapatite and Aluminosilicates. Water Air Soil Pollut 231, 264 (2020). https://doi.org/10.1007/s11270-020-04638-3
Received:
Accepted:
Published:
DOI: https://doi.org/10.1007/s11270-020-04638-3