Removal of steroid hormones and personal care products in wastewater by chemical precipitation
DOI:
https://doi.org/10.15626/Eco-Tech.2007.085Keywords:
Coagulation; Estrogens; Flocculation ; Oestrogens; Parabens; Powdered activated carbon; Sorption, Xenobiotic organic compounds; YES assay.Abstract
The presence of steroid hormones and endocrine disrupting compounds (EDC) in the
environment has been connected with the drop in semen quality in men and the number of
hem1aphrodite fish observed downstream wastewater treatment plants. EDC originating from
down-the-drain chemicals can be reduced by mitigation options but the naturally occurring
hormones must be removed though end-of-pipe treatment. In this study, coagulation and
flocculation as well as these two techniques combined with sorption were applied to remove
estrone, I 7P-estradiol and the synthetic hormone I7a-ethynylestradiol as well as the
preservatives methyl paraben, ethyl paraben, propyl paraben, butyl paraben and isobutyl
paraben from primary and secondary treated municipal wastewater. It was found that
coagulation with both iron and aluminium together with an anionic flocculant successfully
removed organic matter and dissolved phosphorous but not the hormones and only up to 30%
of the parabens. This was seen both in the chemical analyses of the individual substances and
well as in an assay of the oestrogenic effects. Applications of powdered activated carbon preand post the chemical coagulation-flocculation significantly increased the oestrogen removal,
which is consistent with existing literature. The treatment processes in the studied wastewater
treatment plant removed both the oestrogens and the parabens to below the limit of detection ,
though a detectable but small oestrogenicity in the effluent cannot be disregarded.
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References
Sharpe, R., Skakkeba:k, N., 1993. Are Oestrogens Involved in Falling Sperm Counts and Disorders of the Male Reproductive Tract'.1 The Lancet 341, 1392- 1395. https://doi.org/10.1016/0140-6736(93)90953-E
Purdom, CE., Hardiman, PA., Bye, VJ. , Eno, NC, Tyler, C , Sumpter, J ., 1994. Oestrogenic effects of effluents from sewage treatment works. Chem Ecol. 8, 275-85. https://doi.org/10.1080/02757549408038554
Larsson, D.GJ., Adolfsson-Erici, M. , Parkkonen, J. , Pettersson, M. , Berg, A.H., Olsson, P.E., Forlin, L , 1999. Ethinyloestradiol - an undesired fish contraceptive'.I, Aquatic Toxicology, 45, 91-97. https://doi.org/10.1016/S0166-445X(98)00112-X
Desbrow, C , Routledge, EJ., Brightly, G.C, Sumpter, J.P. , Waldock, M., 1998. Identification of Oestrogenic Chemicals in STW Effluent I. Chemical Fractionation and in Vitro Biological Screening, Env. Sci.& Tech. , 32 (11), 1549-1557. https://doi.org/10.1021/es9707973
Bjerregaard, P. , Andersen , D.N., Pedersen, K.L, Pedersen, S.N., Korsgaard, 8. , 2003. Oestrogenic effect of propylparaben (propyl hydroxy benzoate) in rainbow trout Oncorhynchus mykiss after exposure via food and water. Comput. Biochem. Physiol. 136C, 309- 317. https://doi.org/10.1016/j.cca.2003.10.004
Routledge, EJ., Sheahan, D., Desbrow, C, Brightly, G.C, Waldock, M. , Sumpter, J.P., 1998. Identification of Estrogenic Chemicals in STW Effluent 2. In Vivo Responses in Trout and Roach, Env. Sci.& Tech , 32 ( 11 ), 1559-1565. https://doi.org/10.1021/es970796a
Adler, P. , Steger-Hartmann, T Kalbfus, W ., 200 L Vorkommen natiirlicher und synthetischer 6strogener Steroide in Wiissen des sud- und mitteldeutschen Raumes, Acta Hydrochimica et Hydrobiologica, 29 (4), 227-24 L (in German).
Belfroid, A.C, Van der Horst, A. , Vethaak, A.D. , Schafer, AJ., Rijs, G.BJ. , Wegener, J., Cofino, W.P., 1999. Analysis and occurence of estrogenic hormones and their glucuronides in surface water and waste water in The Netherlands, Sci. Tot. Env., 225 , 101-108. https://doi.org/10.1016/S0048-9697(98)00336-2
Benijts, T, Lambert, W., De Leenheer, A., 2004. Analysis of multiple endocrine disrupters in environmental waters via wide-spectrum solid-phase extraction and dualpolarity ionization LC-ion trap-MS/MS, Analytical Chemistry, 76 (3), 704- 711. https://doi.org/10.1021/ac035062x
Ternes, TA., Stumpf, M. , Mueller, J. , Harberer, K. , Wilken , R.D. , Servos, M., 1999. Behavior and occurence of estrogens in municipal sewage treatment plants - L Investigations in Germany, Canada and Brazil, Sci. Tot. Env., I (225), 81-90. https://doi.org/10.1016/S0048-9697(98)00334-9
Andersen , H. , Siegrist, H. , Halling-Sorensen, 8., Ternes, T.A. , 2003. Fate of Estrogens in a Municipal Sewage Treatment Plant, Env. Sci. & Tech, 3 7 ( 18), 4021-4026. https://doi.org/10.1021/es026192a
Joss, A., Andersen , H., Ternes, T., Riehle, P. , Siegrist, H. , 2004. Removal of estrogens in municipal wastewater treatment under aerobic and anaerobic conditions: consequences for plant optimization, Env. Sci.& Tech, 38, 3047-3055. https://doi.org/10.1021/es0351488
Kjolholt, J. , Nielsen , P. and Stuer-Lauridsen, F., 2003. Hormonforstyrrende stoffer og la:gemidler i spildevand. Environmental Project no. 799. Danish EPA. (in Danish)
Lee, H-8., Peart, T.E., Svoboda, M.L, 2005 . Detennination of endocrine-disruptingphenols, acidic pharmaceuticals and personal-care products in sewage by solid-phase extraction and gas chromatography-mass spectrometry, J Chrom. A., 1094, 122-129. https://doi.org/10.1016/j.chroma.2005.07.070
Svenson, A. , Allard, AS., Ek, M. , 2003. Removal of oestrogenicity in Swedish municipal sewage treatment plants. Wat. Res., 37, 4433-4443. https://doi.org/10.1016/S0043-1354(03)00395-6
Remberger, M. , Woldegiorgis, A. , Kaj, L , Andersson, J. , Cousins, A.P. , Dusan, 8., Ekheden, Y. , Brorstrom-Lunden, E., 2006. Results from the Swedish Screening 2005, Subreport 2. Biocides, report BI 700, IVL, Swedish Environmental Research Institute, November 2006.
Eriksson, E., Auffarth , K., Eilersen, A-M., Henze, M. , Ledin, A., 2003. Household chemicals and personal care products as sources for xenobiotic organic compounds in grey wastewater, Water SA , 29 (2), 135-146. https://doi.org/10.4314/wsa.v29i2.4848
Alslev, B., Korsgaard, B., Bjerregaard, P., 2005. Estrogenicity of butylparaben in rainbow trout Oncorhynchus mykiss exposed via food and water, Aquatic toxicity, 72, 295-304. https://doi.org/10.1016/j.aquatox.2005.01.005
Eriksson, E. , Andersen, H.R., Ledin, A. , 2007. Source identification and substance flow analysis of parabens in Denmark. Manuscript submitted for publication. https://doi.org/10.1016/j.jhazmat.2007.12.022
Yeoman, S., Stephenson, T., Lester, JN ., Perry, R. , 1988. The removal of phosphorus during wastewater treatment: a review. Environ Polh1t. 49 (3), 183-233.
D' Ascenzo, G., Di Carcia, A., Gentili, A., Mancini , R. , Mastropasqua, R. , Nazzari, M., Samperi, R. , 2003. Fate of natural oestrogen conjugates in municipal sewage transport and treatment facilities, Sci. Tot. Env., 302, 199-209. https://doi.org/10.1016/S0048-9697(02)00342-X
Soni, M.G. , Carabin, LG., Burdock, G.A. , 2005. Safety assessment of esters of phydroxybenzoic acid (parabens), Food and Chemical Toxicology, 43, 985-1015. https://doi.org/10.1016/j.fct.2005.01.020
Hazardous Substances Data Bank (HSDB®), 2006. Online database. Accessible via http://tox netnIm.nih.gov/cgi-bin/s i s/htmlgen?HS DB
SPARC on-line calculator, 2006. Accessible via http://ibmlc2.chem.uga.edu/sparc/index.cfm?CF!D=234649&CFTOKEN=24906756
US. EPA, 2006. Estimation Program Interface (EPI) Suite v3.12, inherent data from PhysProp. Retrieved from http://www.epa.gov/opptintr/exposure/pubs/episuite.htm
Syracuse Research Corporation, 2006. KowWin Interactive LogKow (KowWin) Demo. Accessible via http://www.syrres.com/esc/est_kowdemo.htm
US. EPA, 2006. Estimation Program Interface (EPI) Suite v3. I 2, estimated data. Retrieved from http://www.epa.gov/opptintr/exposure/pubs/episuite.htm
Lewis, KM. , Archer, RD., 1979. pKa values of estrone, 17 beta-estradiol and 2- methoxyestrone. Steroids , 34(5), 485-99. https://doi.org/10.1016/S0039-128X(79)80011-2
Li, G. , Gregory, J., 1991 Flocculation and sedimentation of high-turbidity waters. Wat. Res., 25 (9), 1137-1143. https://doi.org/10.1016/0043-1354(91)90207-7
Nark is, N., Yusim , S., 2004. Advanced treatment of effluents by simultaneous powdered activated carbon adsorption and flocculation. Journal of Dispersion Science and Technology, 25 (5), 695- 702. https://doi.org/10.1081/DIS-200027330
Routledge, E.J. , Sumpter, J.P. , 1996. Estrogenic activity of surfactants and some of their degradation products assessed using a recombinant yeast screen. Environ. Toxicol. Chem. 15, 241 - 248. https://doi.org/10.1002/etc.5620150303
Montgomery, D.C, 2005 . Design and analysis of experiments, 6th ed., John Wiley & Sons, USA, ISBN 0-4 71-48735-X.
Matsui , S., Takigami, H. , Matsunda, T., Taniguchi , N., Adachi, J. , Kawami , H., Shimizu, Y. , 2000. Estrogen and estrogen mimics contamination in water and the role of sewage treatment, Wat. Sci. & Tech. , 42 ( 12), 173-179. https://doi.org/10.2166/wst.2000.0265
Bodzek, M. , Dudziak, M. , 2006. Elimination of steroidal sex hormones by conventional water treatment and membrane processes, Desalination , 198, 24-32. https://doi.org/10.1016/j.desal.2006.09.005
Westerhoff, P. , Yoon, Y., Snyder, S., Wert, E., 2005. Fate of Endocrine-Disruptor, Pham1aceutical, and Personal Care Product Chemicals during Simulated Drinking Water Treatment Processes, Env. Sci.& Tech, 39 ( 17), 6649-6663. https://doi.org/10.1021/es0484799
Ballard, BO., MacKay, A., 2005. Estimating the removal of anthropogenic organic chemicals from raw drinking water by coagulation flocculation. J Env. Eng. , 131 (I), 108-118. https://doi.org/10.1061/(ASCE)0733-9372(2005)131:1(108)
Chang, S. , Waite, TD. Ong, PEA., Schafer, AL, Fane, AG., 2004. Assessment of Trace Oestrogenic Contaminants Removal by Coagulant Addition, Powdered Activated Carbon Adsorption and Powdered Activated Carbon/Microfiltration Processes. J Env. Eng., 130 (7), 736- 742. https://doi.org/10.1061/(ASCE)0733-9372(2004)130:7(736)
Yoon, Y. , Westerhoff, P. , Snyder, SA., Esparza, M., 2003. HPLC-fluorescence detection and adsorption of bisphenol A, I 7beta-estradiol, and I 7alpha-ethynyl estradiol on powdered activated carbon. Wat. Res. , 37 (4), 3530-3537. https://doi.org/10.1016/S0043-1354(03)00239-2
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Copyright (c) 2007 Eva Eriksson , Heidi Birch, Henrik R. Andersen , Mogens Henze
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