The elimination of five selected emerging contaminants (1-H-benzotriazole, N,N-diethyl-m-toluamide (DEET), chlorophene, 3-methylindole, and nortriptyline HCl) dissolved in different water matrices (surface water and secondary effluents) was carried out by sequential membrane filtration and chemical oxidation processes. First, a membrane filtration (ultrafiltration (UF) or nanofiltration(NF)) pre-treatment was conducted, and both permeate and retentate were afterwards treated by chemical oxidation, using ozone or chlorine. The application of UF and especially of NF provided a large volume of permeate, whose quality can be improved by a chemical treatment to completely remove residual contaminants except 1-H-benzotriazole. Chlorination and especially ozonation have demonstrated to be effective for the reduction of emerging contaminants in the concentrated stream, thus generating an effluent that might be recycled to the activated sludge treatment in the wastewater treatment plants (WWTP). In a second group of experiments, a chemical oxidation pre-treatment (by using ozone, chlorine, O3/H2O2, ultraviolet (UV) radiation, or UV/H2O2) was applied followed by a nanofiltration process. Results of removals and rejection coefficients for the emerging contaminants showed that the chemical pre-treatment exerted a positive influence on the subsequent NF process, not only in terms of ECs removal but also of dissolved organic carbon content (DOC) reduction. While global removals higher than 97 % were reached for DEET, chlorophene, 3-methylindole, and nortriptyline HCl, lower values were obtained for 1-H-benzotriazole, especially for chlorine pre-treatment and in those water matrices with high content of natural organic matter. Therefore, both sequential treatments are promising to remove the selected micropollutants while reducing the chlorine doses needed to achieve final water disinfection.
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Acero, J. L., Benitez, F. J., Real, F. J., Roldán, G., & Rodriguez, E. (2013). Chlorination and bromination kinetics of emerging contaminants in aqueous systems. Chemical Engineering Journal, 219, 43–50.
Anwar Sadmani, A. H. M., Andrews, R. C., & Bagley, D. M. (2014). Nanofiltration of pharmaceutically active compounds as a function of compound interactions with DOM fractions and cations in natural water. Separation and Purification Technology, 122, 462–471.
Benitez, F. J., Acero, J. L., Real, F. J., & Garcia, C. (2009). Combination of chemical oxidation-membrane filtration processes for the elimination of phenyl-ureas in water matrices. Journal of Chemical Technology & Biotechnology, 84, 1883–1893.
Benitez, F. J., Acero, J. L., Garcia-Reyes, F. J., Real, F. J., Roldán, G., Rodriguez, E., & Molina-Diaz, A. (2013a). Oxidation of chlorophene by ozonation: kinetics, identification of by-products and reaction pathways. Chemical Engineering Journal, 230, 447–455.
Benitez, F. J., Acero, J. L., Garcia-Reyes, F. J., Real, F. J., Roldán, G., Rodriguez, E., & Molina-Diaz, A. (2013b). Determination of the reaction rate constants and decomposition mechanisms of ozone with two model emerging contaminants: DEET and nortriptyline. Industrial & Engineering Chemistry Research, 52, 17064–17073.
Benitez, F. J., Acero, J. L., Real, F. J., Roldán, G., & Rodriguez, E. (2013c). Modeling the photodegradation of emerging contaminants in waters by UV radiation and UV/H2O2 system. Journal of Environmental Science and Health, Part A: Toxic/Hazardous Substances and Environmental Engineering, 48, 120–128.
Benitez, F. J., Acero, J. L., Real, F. J., Roldán, G., & Rodriguez, E. (2015). Ozonation of benzotriazole and methylindole: kinetic modeling, identification of intermediates and reaction mechanisms. Journal of Hazardous Materials, 282, 224–232.
Bichsel, Y., & von Gunten, U. (1999). Determination of iodine and iodate by ion chromatography with postcolumn reaction and UV/visible detection. Analytical Chemistry, 71, 34–38.
Buxton, G. V., Greenstock, C. L., Helman, W. P., & Ross, A. B. (1988). Critical review of rate constants for oxidation of hydrated electrons, hydrogen atoms and hydroxyl radicals (AOH/AO−) in aqueous solutions. Journal of Physical and Chemical Reference Data, 17, 513–886.
Canonica, S., Meunier, L., & von Gunten, U. (2008). Phototransformation of selected pharmaceuticals during UV treatment of drinking water. Water Research, 42, 121–128.
Comerton, A. M., Andrews, R. C., Bagley, D. M., & Hao, C. (2008). The rejection of endocrine disrupting and pharmaceutically active compounds by NF and RO membranes as a function of compound and water matrix properties. Journal of Membrane Science, 313, 323–335.
Costanzo, S. D., Watkinson, A. J., Murby, E. J., Kolpin, D. W., & Sandstrom, M. W. (2007). Is there a risk associated with the insect repellent DEET (N,N-diethyl-m-toluamide) commonly found in aquatic environments? Science of the Total Environment, 384, 214–220.
Dolar, D., Kosutic, K., Perisa, M., & Babic, S. (2013). Photolysis of enrofloxacin and removal of its photodegradation products from water by reverse osmosis and nanofiltration membranes. Separation and Purification Technology, 115, 1–8.
Elovitz, M. S., & von Gunten, U. (1999). Hydroxyl radical/ozone ratios during ozonation processes. I. The RCT concept. Ozone Science & Engineering, 21, 239–260.
Heberer, T. (2002). Occurrence, fate and removal of pharmaceutical residues in the aquatic environment: a review of recent research data. Toxicology Letters, 131, 5–17.
Illueca-Muñoz, J., Mendoza-Roca, J. A., Iborra-Clar, A., Bes-Pia, A., Fajardo-Montañana, V., Martinez-Francisco, F. J., & Bernacer-Bonora, I. (2008). Study of different alternatives of tertiary treatments for wastewater reclamation to optimize the water quality for irrigation reuse. Desalination, 222, 222–229.
James, C. P., Germain, E., & Judd, S. (2014). Micropollutant removal by advanced oxidation of microfiltered secondary effluent for water reuse. Separation and Purification Technology, 127, 77–83.
Jansen, R. H. S., Zwijnenburg, A., van der Meer, W. G. J., & Wessling, M. (2006). Outside-in trimming of humic substances during ozonation in a membrane contactor. Environmental Science & Technology, 40, 6460–6465.
Jelic, A., Gros, M., Ginebreda, A., Cespedes-Sanchez, R., Ventura, F., Petrovic, M., & Barcelo, D. (2011). Occurrence, partition and removal of pharmaceuticals in sewage water and sludge during wastewater treatment. Water Research, 45, 1165–1176.
Kim, H.-A., Choi, J.-H., & Takizawa, S. (2007). Comparison of initial filtration resistance by pretreatment processes in the nanofiltration for drinking water treatment. Separation and Purification Technology, 56, 354–362.
Langford, K. H., & Thomas, K. V. (2009). Determination of pharmaceutical compounds in hospital effluents and their contribution to wastewater treatment works. Environment International, 35, 766–770.
Linlin, W., Xuan, Z., & Meng, Z. (2011). Removal of organic matter in municipal effluent with ozonation, slow sand filtration and nanofiltration as high quality pre-treatment option for artificial groundwater recharge. Chemosphere, 83, 693–699.
Loos, R., Gawlik, B. M., Locoro, G., Rimaviciute, E., Contini, S., & Bidoglio, G. (2009). EU wide survey of polar organic persistent pollutants in European river waters. Environmental Pollution, 157, 561–568.
Perez-Gonzalez, A., Urtiaga, A. M., Ibañez, R., & Ortiz, I. (2012). State of the art and review on the treatment technologies of water reverse osmosis concentrates. Water Research, 46, 267–283.
Rivera-Utrilla, J., Sánchez-Polo, M., Ferro-García, M. A., Prados-Joya, G., & Ocampo-Pérez, R. (2013). Pharmaceuticals as emerging contaminants and their removal from water. A review. Chemosphere, 93, 1268–1287.
Sanches, S., Penetra, A., Rodrigues, A., Cardoso, V. V., Ferreira, E., Benoliel, M. J., Barreto Crespo, M. T., Crespo, J. G., & Pereira, V. J. (2013). Removal of pesticides from water combining low pressure UV photolysis with nanofiltration. Separation and Purification Technology, 115, 73–82.
Saquib, M., Vinckier, C., & Van der Bruggen, B. (2010). The effect of UF on the efficiency of O3/H2O2 for the removal of organics from surface water. Desalination, 260, 39–42.
Sharma, V. K. (2008). Oxidative transformation of environmental pharmaceuticals by Cl2, ClO2, O3, and Fe (VI): kinetics assessment. Chemosphere, 73, 1379–1386.
Sim, W.-J., Lee, J.-W., Lee, E.-S., Shin, S.-K., Hwang, S.-R., & Oh, J.-E. (2011). Occurrence and distribution of pharmaceuticals in wastewater from households, livestock farms, hospitals and pharmaceutical manufactures. Chemosphere, 82, 179–186.
Staehelin, J., & Hoigne, J. (1985). Decomposition of ozone in water in the presence of organic solutes acting as promoters and inhibitors of radical chain reactions. Environmental Science & Technology, 19, 1206–1213.
Tijani, O. J., Fatoba, O. O., & Petrik, L. F. (2013). A review of pharmaceuticals and endocrine-disrupting compounds: sources, effects, removal and detections. Water, Air, & Soil Pollution, 224, 1770–1809.
Tijani, O. J., Fatoba, O. O., Madzivire, G., & Petrik, L. F. (2014). A review of combined advanced oxidation technologies for the removal of organic pollutants from water. Water, Air, & Soil Pollution, 225, 2102–2132.
Van der Bruggen, B., Manttari, M., & Nystrom, M. (2008). Drawbacks of applying nanofiltration and how to avoid them: a review. Separation and Purification Technology, 63, 251–263.
Van Geluwe, S., Vinckier, C., Bobu, E., Trandafir, C., Vanelslander, J., Braeken, L., & Van der Bruggen, B. (2010). Eightfold increased membrane flux of NF 270 by O3 oxidation of natural humic acids without deteriorated permeate quality. Journal of Chemical Technology & Biotechnology, 85, 1480–1488.
von Gunten, U. (2003). Ozonation of drinking water. Part I. Oxidation kinetics and product formation. Water Research, 37, 1443–1467.
Wray, H. E., Andrews, R. C., & Bérubé, P. R. (2014). Surface shear stress and retention of emerging contaminants during ultrafiltration for drinking water treatment. Separation and Purification Technology, 122, 183–191.
Authors gratefully acknowledge financial support from the MINECO of Spain and FEDER Funds through Project CTQ2013-41354-R and from Gobierno de Extremadura and FSE Funds through Project RNM021. E. Rodriguez thanks to the Gobierno de Extremadura and FSE Funds for her FPI Ph.D. Grant.
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Acero, J.L., Benitez, F.J., Real, F.J. et al. Elimination of Selected Emerging Contaminants by the Combination of Membrane Filtration and Chemical Oxidation Processes. Water Air Soil Pollut 226, 139 (2015). https://doi.org/10.1007/s11270-015-2404-8
- Emerging contaminants
- Chemical oxidation
- Membrane filtration
- Sequential treatments
- Global removals
- Rejection coefficients