Skip to main content
Log in

Elimination of Selected Emerging Contaminants by the Combination of Membrane Filtration and Chemical Oxidation Processes

  • Published:
Water, Air, & Soil Pollution Aims and scope Submit manuscript

Abstract

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.

This is a preview of subscription content, log in via an institution to check access.

Access this article

Price excludes VAT (USA)
Tax calculation will be finalised during checkout.

Instant access to the full article PDF.

Fig. 1
Fig. 2
Fig. 3
Fig. 4
Fig. 5

Similar content being viewed by others

References

  • 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.

    Article  CAS  Google Scholar 

  • 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.

    Article  Google Scholar 

  • 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.

    Article  Google Scholar 

  • 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.

    Article  CAS  Google Scholar 

  • 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.

    Article  CAS  Google Scholar 

  • 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.

    Article  CAS  Google Scholar 

  • 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.

    Article  CAS  Google Scholar 

  • 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.

    Article  CAS  Google Scholar 

  • 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.

    Article  CAS  Google Scholar 

  • Canonica, S., Meunier, L., & von Gunten, U. (2008). Phototransformation of selected pharmaceuticals during UV treatment of drinking water. Water Research, 42, 121–128.

    Article  CAS  Google Scholar 

  • 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.

    Article  CAS  Google Scholar 

  • 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.

    Article  CAS  Google Scholar 

  • 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.

    Article  CAS  Google Scholar 

  • Elovitz, M. S., & von Gunten, U. (1999). Hydroxyl radical/ozone ratios during ozonation processes. I. The RCT concept. Ozone Science & Engineering, 21, 239–260.

    Article  CAS  Google Scholar 

  • 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.

    Article  CAS  Google Scholar 

  • 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.

    Article  Google Scholar 

  • 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.

    Article  CAS  Google Scholar 

  • 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.

    Article  CAS  Google Scholar 

  • 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.

    Article  CAS  Google Scholar 

  • 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.

    Article  CAS  Google Scholar 

  • 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.

    Article  CAS  Google Scholar 

  • 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.

    Article  Google Scholar 

  • 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.

    Article  CAS  Google Scholar 

  • 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.

    Article  CAS  Google Scholar 

  • 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.

    Article  CAS  Google Scholar 

  • 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.

    Article  CAS  Google Scholar 

  • 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.

    Article  CAS  Google Scholar 

  • Sharma, V. K. (2008). Oxidative transformation of environmental pharmaceuticals by Cl2, ClO2, O3, and Fe (VI): kinetics assessment. Chemosphere, 73, 1379–1386.

    Article  CAS  Google Scholar 

  • 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.

    Article  CAS  Google Scholar 

  • 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.

    Article  CAS  Google Scholar 

  • 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.

    Article  Google Scholar 

  • 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.

    Article  Google Scholar 

  • 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.

    Article  Google Scholar 

  • 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.

    Google Scholar 

  • von Gunten, U. (2003). Ozonation of drinking water. Part I. Oxidation kinetics and product formation. Water Research, 37, 1443–1467.

    Article  Google Scholar 

  • 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.

    Article  CAS  Google Scholar 

Download references

Acknowledgments

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.

Author information

Authors and Affiliations

Authors

Corresponding author

Correspondence to Juan L. Acero.

Rights and permissions

Reprints and permissions

About this article

Check for updates. Verify currency and authenticity via CrossMark

Cite this article

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

Download citation

  • Received:

  • Accepted:

  • Published:

  • DOI: https://doi.org/10.1007/s11270-015-2404-8

Keywords

Navigation