Iron Oxide Nanoparticles Supported on Mesoporous MCM-41 for Efficient Adsorption of Hazardous β-Lactamic Antibiotics
- 205 Downloads
In this work, the effect of crystallite size, defects, and surface area of iron oxyhydroxide particles supported on mesoporous MCM-41 on the adsorption of hazardous β-lactamic antibiotics was investigated. Different adsorbents were prepared by impregnation of 5, 10, 20, and 50 wt% of Fe followed by treatment at 150–400 °C. Mössbauer, XRD, BET, TG, FTIR, and Raman analyses suggested that treatment at 150 °C produced a mixture of α-Fe2O3, FeOOH, and highly dispersed Fe3+ species. At higher temperatures, different phases were gradually converted to hematite with crystallite sizes varying from 1 to 5 nm. Both, Fe content and temperature, strongly affected the amoxicillin, cephalexin, and ceftriaxone adsorption at pH 5, 7, and 9, with the best results obtained for the sample 20Fe150 (20% Fe treated at 150 °C), ca. 25 mgAMX g−1 which decreased to 17, 6, and 4 mgAMX g−1 (AMX = amoxicillin) upon treatment at higher temperatures. These results combined with competitive adsorption using AMX/phosphate and H2O2 decomposition experiments suggested that the antibiotic molecules are likely adsorbing by complexation on Fe3+ surface species of poorly crystallized small particles of Fe oxyhydroxide phases. It was observed that below a critical crystallite size of 3 nm, the AMX adsorption was very sensitive and strongly increased.
KeywordsIron oxide MCM-41 Amoxicillin Adsorption
We thank the Center of Microscopy at the Universidade Federal de Minas Gerais (http://www.microscopia.ufmg.br) for providing the equipment and technical support for experiments involving electron microscopy. This research used resources of the Brazilian Synchrotron Light Laboratory (LNLS), an open national facility operated by the Brazilian Centre for Research in Energy and Materials (CNPEM) for the MCTIC (Proposal 20160824). The assistance of Alexandre Carvalho, beamline staff is especially acknowledged.
The authors gratefully acknowledge the financial support of CNPq, INCT-MIDAS, CAPES, and FAPEMIG.
- Abouaitah, K.E.A., Farghali, A.F. , Swiderska-Sroda, A., Lojkowsi, W., Razin, A.M., & Khedr, M.H. (2016). Mesoporous silica materials in drug delivery system: pH/glutathione-responsive release of poorly water-soluble pro-drug quercetin from two and three-dimensional pore-structure nanoparticles. Journal of Nanomedicine Nanotechnology, 7. https://doi.org/10.4172/2157-7439.1000360.
- Barrera, D., Villarroel-Rocha, J., Tara, J. C., Basaldella, E. I., & Sapag, K. (2014). Synthesis and textural characterization of a templated nanoporous carbon from MCM-22 zeolite and its use as adsorbent of amoxicillin and ethinylestradiol. Adsorption, 20, 967–976. https://doi.org/10.1007/s10450-014-9640-x.CrossRefGoogle Scholar
- Becker, D., Della Giustina, S. V., Rodriguez-Mozaz, S., Schoevaart, R., Barcelo, D., de Cazes, M., Belleville, M. P., Sanchez-Marcano, J., de Gunzburg, J., Couillerot, O., Völker, J., Oehlmann, J., & Wagner, M. (2016). Removal of antibiotics in wastewater by enzymatic treatment with fungal laccase—degradation of compounds does not always eliminate toxicity. Bioresource Technology, 219, 500–509. https://doi.org/10.1016/j.biortech.2016.08.004.CrossRefGoogle Scholar
- Colomban, P. (2011). Potential and drawbacks of Raman (micro)spectrometry for the understanding of iron and steel corrosion. New Trends Dev. Automot. Syst. Eng., 567–584. https://doi.org/10.5772/13436.
- Costa, R. C. C., Moura, F. C. C., Oliveira, P. E. F., Magalhaes, F., Ardisson, J. D., & Lago, R. M. (2010). Controlled reduction of red mud waste to produce active systems for environmental applications: heterogeneous Fenton reaction and reduction of Cr(VI). Chemosphere, 78, 1116–1120. https://doi.org/10.1016/j.chemosphere.2009.12.032.CrossRefGoogle Scholar
- Johnson, A. C., Keller, V., Dumont, E., & Sumpter, J. P. (2015). Assessing the concentrations and risks of toxicity from the antibiotics ciprofloxacin, sulfamethoxazole, trimethoprim and erythromycin in European rivers. Sci. Total Environ., 511, 747–755. https://doi.org/10.1016/j.scitotenv.2014.12.055.CrossRefGoogle Scholar
- Kanakaraju, D., Kockler, J., Motti, C. A., Glass, B. D., & Oelgemöller, M. (2015). Titanium dioxide/zeolite integrated photocatalytic adsorbents for the degradation of amoxicillin. Applied Catalysis B: Environmental, 166-167, 45–55. https://doi.org/10.1016/j.apcatb.2014.11.001.CrossRefGoogle Scholar
- Liang, Z. J., Zhaob, Z. W., Sun, T. Y., Shi, W. X., & Cui, F. Y. (2016). Adsorption of quinolone antibiotics in spherical mesoporous silica: effects of the retained template and its alkyl chain length. Journal of Hazardous Materials, 305, 8–14. https://doi.org/10.1016/j.jhazmat.2015.11.033.CrossRefGoogle Scholar
- Liu, M. M., Hou, L. A., Yu, S. L., Xi, B. D., Zhao, Y., & Xia, X. F. (2013). MCM-41 impregnated with a zeolite precursor: synthesis, characterization and tetracycline antibiotics removal from aqueous solution. Chemical Engineering Journal, 223, 678–687. https://doi.org/10.1016/j.cej.2013.02.088.CrossRefGoogle Scholar
- Liu, J. C., Lu, G. H., Xie, Z. X., Zhang, Z. H., Li, S., & Yan, Z. H. (2015). Occurrence, bioaccumulation and risk assessment of lipophilic pharmaceutically active compounds in the downstream rivers of sewage treatment plants. Sci. Total Environ., 511, 54–62. https://doi.org/10.1016/j.scitotenv.2014.12.033.CrossRefGoogle Scholar
- Moura, F.C.C., Ardisson, J.D., Macedo, W.A.A., Albuquerque, A.S. & Lago, R.M.(2007). Investigation of the solid state reaction of LaMnO3 with Fe0 and its effect on the catalytic reactions with H2O2. 18, 322–329. https://doi.org/10.1016/j.apcatb.2014.04.010.
- Moura, F. C. C., Tristão, J. C., Pereira, M. C., Lago, R. M., & Fabris, J. D. (2008). Controlled reduction of LaFex Mny Moz O3/Al2O3 composites to produce highly dispersed and stable Fe0 catalysts: a Mössbauer investigation. Int. J. Appl. or Innov. Eng. Manag., 11, 233–238. https://doi.org/10.1021/ie970870y.Google Scholar
- Pereira, M. C., Tavares, C. M., Fabris, J. D., Lago, R. M., Murad, E., & Criscuolo, P. S. (2007). Characterization of a tropical soil and a waste from kaolin mining and their suitability as heterogeneous catalysts for Fenton and Fenton-like reactions. Clay Minerals, 42, 299–306. https://doi.org/10.1180/claymin.2007.042.3.03.CrossRefGoogle Scholar
- Pereira, J. H. O. S., Reis, A. C., Homem, V., Silva, J. A., Alves, A., Borges, M. T., Boaventura, R. A. R., Vilar, V. J. P., & Nunes, O. C. (2014). Solar photocatalytic oxidation of recalcitrant natural metabolic by-products of amoxicillin biodegradation. Water Research, 65, 307–320. https://doi.org/10.1016/j.watres.2014.07.037.CrossRefGoogle Scholar
- Purceno, A. D., Teixeira, A. P. C., de Souza, N. J., Fernandez-Outon, L. E., Ardisson, J. D., & Lago, R. M. (2012). Hybrid magnetic amphiphilic composites based on carbon nanotube/nanofibers and layered silicates fragments as efficient adsorbent for ethynilestradiol. Journal of Colloid and Interface Science, 379, 84–88. https://doi.org/10.1016/j.jcis.2012.04.018.CrossRefGoogle Scholar
- Raziye Ferdowsi, S.M.K. & Layali, I. (2015). Treatment of antibiotics from wastewater by adsorption onto low adsorbent. International Journal of Analysis on Pharmaceutical Biomedical Science. 44–50.Google Scholar
- Ribeiro-Santos, T. A., Henriques, F. F., Villarroel-Rocha, J., de Castro, M. C. M., Magalhaes, W. F., Windmuller, D., Sapag, K., Lago, R. M., & Araujo, M. H. (2016). Hydrophobic channels produced by micelle-structured CTAB inside MCM-41 mesopores: a unique trap for the hazardous hormone ethinyl estradiol. Chemical Engineering Journal, 283, 1203–1209. https://doi.org/10.1016/j.cej.2015.08.029.CrossRefGoogle Scholar
- Schwanke, A. J., & Pergher, S. B. (2012). Peneiras moleculares mesoporosas MCM-41: uma perspectiva histórica, o papel de cada reagente na síntese e sua caracterização básica. Perspectivas, 36, 113–125.Google Scholar
- Teixeira, A. P. C., Purceno, A. D., de Paula, C. C. A., da Silva, J. C. C., Ardisson, J. D., & Lago, R. M. (2013). Efficient and versatile fibrous adsorbent based on magnetic amphiphilic composites of chrysotile/carbon nanostructures for the removal of ethynilestradiol. Journal of Hazardous Materials, 248-249, 295–302. https://doi.org/10.1016/j.jhazmat.2013.01.014.CrossRefGoogle Scholar
- Widyasari-Mehta, A., Hartung, S., & Kreuzig, R. (2016). From the application of antibiotics to antibiotic residues in liquid manures and digestates: A screening study in one European center of conventional pig husbandry. Journal of Environmental Management, 177, 129–137. https://doi.org/10.1016/j.jenvman.2016.04.012.CrossRefGoogle Scholar
- Xu, W. H., Zhang, G., Zou, S. C., Li, X. D., & Liu, Y. C. (2007). Determination of selected antibiotics in the Victoria Harbour and the Pearl River, South China using high-performance liquid chromatography-electrospray ionization tandem mass spectrometry. Environmental Pollution, 145, 672–679. https://doi.org/10.1016/j.envpol.2006.05.038.CrossRefGoogle Scholar