Technical Papers
Mar 1, 2012

Fate of Endocrine-Disrupting and Pharmaceutically Active Substances in Sand Columns Fed with Secondary Effluent

Publication: Journal of Environmental Engineering
Volume 138, Issue 10

Abstract

Sorption and biotransformation of six endocrine disrupting compounds (EDCs) [estrone (E1), 17β-estradiol (E2), estriol (E3), 17α-ethynylestradiol (EE2), 4-tert-octylphenol (4-t-OP), and bisphenol A (BPA)] and two pharmaceutically active compounds (PhACs) [ibuprofen (IBU) and naproxen (NAP)] were studied in microcosms and columns under conditions that simulate the percolation of effluent through sandy soil on reclaimed land in Singapore. Sorption isotherms followed a linear model, except for IBU and BPA, for which a Freundlich model was used, and for NAP, which sorbed too little to be measurable. Degradation experiment results showed that aerobic conditions were more favorable for the degradation of EDCs than anaerobic or anoxic conditions. E3 and 4-t-OP were totally removed within 40 days, whereas EE2, BPA, IBU, and NAP were persistent. However, under anaerobic conditions, E1 was formed from E2 and vice versa, reaching steady-state conditions after approximately 15 days. To simulate the groundwater (GW) recharge condition, eight laboratory-scale soil aquifer treatment (SAT)–saturated sand columns (each with a length of 1.0 m) were operated in series. Secondary effluent (SE) and ultrafiltered effluent augmented with the target compounds was applied to two identical sets of eight columns, respectively. With secondary effluent and ultrafiltered SE as the feed, the target compounds were completely removed after 8 m of infiltration, with the exception of NAP, which persisted at 1μg/L in the effluent of recharged columns after an operating time of 3 pore volumes (PV). The higher removal rate in SE recharged columns is attributed to the higher nutrient content, microbial populations, and a longer period of acclimatization. Small-scale batch studies showed that E2, EE2, IBU, and NAP removal was primarily a result of biological transformation that was faster under aerobic than anaerobic conditions.

Get full access to this article

View all available purchase options and get full access to this article.

Acknowledgments

The authors thank San San Chow, Chenqi Hu, and Yue-hua Chen for their assistance in the chemical measurements. Funding support from the Agency for Science and Technology (ASTAR), Singapore, and Nanyang Technological University (NTU) are acknowledged.

References

Bledzka, D., Gryglik, D., and Miller, J. (2009). “Photolytic degradation of 4-tert-octylhenol in aqueous solution.” Environ. Prot. Eng., 35, 235–247.
Bursch, W. et al. (2004). “Endocrine disrupters in the aquatic environment: The Australian approach—ARCEM.” Water Sci. Technol., 50, 293–300.
Carballa, M. et al. (2004). “Behavior of pharmaceuticals, cosmetics and hormones in a sewage treatment plant.” Water Res., 38(12), 2918–2926.
Carballa, M., Omil, F., and Lema, J. M. (2005). “Removal of cosmetic ingredients and pharmaceuticals in sewage primary treatment.” Water Res., 39(19), 4790–4796.
Casey, F. M., Larsen, G. L., Hakk, H., and Simunek, J. (2003). “Fate and transport of 17β-estradiol in soil-water systems.” Environ. Sci. Technol., 37(11), 2400–2409.
Chua, L. H. C. et al. (2007). “Hydrostratigraphy and geochemistry at a coastal sandfill.” Hydrogeol. J., 15(8), 1591–1604.
Colucci, M. S., and Topp, E. (2001). “Persistence of estrogenic hormones in agricultural soil: II. 17{alpha}-ethynylestradiol.” J. Environ. Qual., 30(6), 2077–2080.
Czajka, C. P., and Londry, K. L. (2006). “Anaerobic biotransformation of estrogens.” Sci. Total Environ., 367(2–3), 932–941.
Daughton, C. G., and Ternes, T. A. (1999). “Pharmaceuticals and personal care products in the environment: Agents of subtle change?” Environ. Health Perspect., 107, 907–938.
Drewes, J. E., Reinhard, M., and Fox, P. (2003). “Comparing microfiltration-reverse osmosis and soil-aquifer treatment for indirect potable reuse of water.” Water Res., 37(15), 3612–3621.
Hanselman, T. A., Graetz, D. A, and Wilkie, A. C. (2003). “Manure-borne estrogens as potential environmental contaminants: A review.” Environ. Sci. Technol., 37(24), 5471–5478.
Johnson, A. C., and Sumpter, J. P. (2001). “Removal of endocrine-disrupting chemicals in activated sludge treatment works.” Environ. Sci. Technol., 35(24), 4697–4703.
Jurgens, M. D., Holthaus, K. I. E., Johnson, A. C., Smith, J. J. L., Hetheridge, M., and Williams, R. J. (2002). “The potential for estradiol and ethinylestradiol degradation in English rivers.” Environ. Toxicol. Chem., 21(3), 480–488.
Kavlock, R. J. (1999). “Overview of endocrine disruptor research activity in the United States.” Chemosphere, 39(8), 1227–1236.
Lai, K. M., Johnson, K. L., Scrimshaw, M. D., and Lester, J. N. (2000). “Binding of waterborne steroid estrogens to solid phases in river and estuarine systems.” Environ. Sci. Technol., 34(18), 3890–3894.
Lai, K. M., Scrimshaw, M. D., and Lester, J. N. (2002). “Biotransformation and bioconcentration of steroid estrogens by Chlorella vulgaris.” Appl. Environ. Microbiol., 68(2), 859–864.
Lee, H. B., and Liu, D. (2002). “Degradation of 17β-Estradiol and its metabolites by sewage bacteria.” Water Air Soil Pollut., 134(1/4), 351–366.
Lee, L. S., Strock, T. J., Sarmah, A. K., and Rao, P. S. C. (2003). “Sorption and dissipation of testosterone, estrogens, and their primary transformation products in soils and sediment.” Environ. Sci. Technol., 37(18), 4098–4105.
Lucas, S. D., and Jones, D. L. (2006). “Biodegradation of estrone and 17β-estradiol in grassland soils amended with animal wastes soil.” Soil Biol. Biochem., 38(9), 2803–2815.
McLachlan, J. A. (2001). “Environmental signaling: What embryos and evolution teach us about endocrine disrupting chemicals.” Endocr. Rev., 22(3), 319–341.
Montgomery-Brown, J., Drewes, J. E., Fox, P., and Reinhard, M. (2003). “Behavior of alkylphenol polyethoxylate metabolites during soil aquifer treatment.” Water Res., 37(15), 3672–3681.
Pal, A., Gin, K. Y. H., Lin, A. Y. C., and Reinhard, M. (2010). “Impacts of emerging organic contaminantson freshwater resources: review of recent occurrences, sources, fate, and effects.” Sci. Total Environ., 408(24), 6062–6069.
Schäfer, A. I., Nghiem, L. D., and Waite, T. D. (2003). “Removal of the natural hormone estrone from aqueous solutions using nanofiltration and reverse osmosis.” Environ. Sci. Technol., 37(1), 182–188.
Scheytt, T., Mersmann, P., Lindstädt, R., and Heberer, T. (2005). “Determination of sorption coefficients of pharmaceutically active substances carbamezepine, diclofenac, and ibuprofen, in sandy sediments.” Chemosphere, 60(2), 245–253.
Schwarzenbach, R. P., Gschwend, P. M., and Imboden, D. M. (1993). Environmental organic chemistry, Schwarzenbach, R. P.ed., Wiley, New York, 116–122.
Sedlak, D. L., Gray, J. L., and Pinkston, K. E. (2000). “Understanding microcontaminants in recycled water.” Environ. Sci. Technol., 34(23), 508A–515A.
Shareef, A., Angove, M. J., and Wells, J. D. (2006). “Optimization of silylation using N-methyl-N-(trimethylsilyl)-trifluoroacetamide,N,O-bis-(trimethyl.silyl)-trifluoroacetamide and N-(tert-butyldimethylsilyl)-N-methyltrifluoroacetamide for the determination of the estrogens estrone and 17 alphaethinylestradiol by gas chromatography–mass spectrometry.” J. Chromatogr. A, 1108, 121–128.
Shi, J., Fujisawa, S., Nakai, S., and Hosomi, M. (2004a). “Biodegradation of natural and synthetic estrogens by nitrifying activated sludge and ammonia-oxidizing bacterium Nitrosomonas europaea.” Water Res., 38(9), 2323–2330.
Shi, J. H., Suzuki, Y., Nakai, S., and Hosomi, M. (2004b). “Microbial degradation of estrogens using activated sludge and night soil-composting microorganisms.” Water Sci. Technol., 50, 153–159.
Ternes, T. A., Kreckel, P., and Mueller, J. (1999). “Behaviour and occurrence of estrogens in municipal sewage treatment plants—II. Aerobic batch experiments with activated sludge.” Sci. Total Environ., 225(1–2), 91–99.
Vader, J. S. et al. (2000). “Degradation of ethinyl estradiol by nitrifying activated sludge.” Chemosphere, 41(8), 1239–1243.
Ying, G.-G., and Kookana, R. S. (2003). “Degradation of five selected endocrine-disrupting chemicals in seawater and marine sediment.” Environ. Sci. Technol., 37(7), 1256–1260.
Ying, G.-G., and Kookana, R. S. (2005). “Sorption and degradation of estrogen-like-endocrine disrupting chemicals in soil.” Environ. Toxicol. Chem., 24(10), 2640–2645.
Ying, G.-G., Kookana, R. S., and Dillon, P. (2003). “Sorption and degradation of selected five endocrine disrupting chemicals in aquifer material.” Water Res., 37(15), 3785–3791.
Ying, G.-G., Kookana, R. S., and Dillon, P. (2004). “Attenuation of two estrogen compounds in aquifer materials supplemented with sewage effluent.” Ground Water Monit. Rem., 24, 102–107.
Yu, Z. Q., Xiao, B. H., Huang, W. L., and Peng, P. (2004). “Sorption of steroid estrogens to soils and sediments.” Environ. Toxicol. Chem., 23(3), 531–539.

Information & Authors

Information

Published In

Go to Journal of Environmental Engineering
Journal of Environmental Engineering
Volume 138Issue 10October 2012
Pages: 1067 - 1076

History

Received: Apr 27, 2011
Accepted: Feb 27, 2012
Published online: Mar 1, 2012
Published in print: Oct 1, 2012

Permissions

Request permissions for this article.

Authors

Affiliations

Jinxia Ke
Academic staff, School of Applied Science, Republic Polytechnic, 9 Woodland Ave. 9, Singapore 738964.
Karina Yew Hoong Gin [email protected]
Associate Professor, Dept. of Civil and Environmental Engineering, National Univ. of Singapore, Blk E1A-07-03, 1 Engineering Dr. 2, Singapore 119756 (corresponding author). E-mail: [email protected]
Lai Heng Tan
Environmental Engineer, DHI Water & Environment (S) Pte Ltd, 200 Pandan Loop, #08-03 Pantech 21, Singapore 128388.
Martin Reinhard
Professor (Research), Dept. of Civil and Environmental Engineering, Y2E2 Building, 473 Via Ortega, Stanford Univ., Stanford, CA 94305-4020.

Metrics & Citations

Metrics

Citations

Download citation

If you have the appropriate software installed, you can download article citation data to the citation manager of your choice. Simply select your manager software from the list below and click Download.

Cited by

View Options

Get Access

Access content

Please select your options to get access

Log in/Register Log in via your institution (Shibboleth)
ASCE Members: Please log in to see member pricing

Purchase

Save for later Information on ASCE Library Cards
ASCE Library Cards let you download journal articles, proceedings papers, and available book chapters across the entire ASCE Library platform. ASCE Library Cards remain active for 24 months or until all downloads are used. Note: This content will be debited as one download at time of checkout.

Terms of Use: ASCE Library Cards are for individual, personal use only. Reselling, republishing, or forwarding the materials to libraries or reading rooms is prohibited.
ASCE Library Card (5 downloads)
$105.00
Add to cart
ASCE Library Card (20 downloads)
$280.00
Add to cart
Buy Single Article
$35.00
Add to cart

Get Access

Access content

Please select your options to get access

Log in/Register Log in via your institution (Shibboleth)
ASCE Members: Please log in to see member pricing

Purchase

Save for later Information on ASCE Library Cards
ASCE Library Cards let you download journal articles, proceedings papers, and available book chapters across the entire ASCE Library platform. ASCE Library Cards remain active for 24 months or until all downloads are used. Note: This content will be debited as one download at time of checkout.

Terms of Use: ASCE Library Cards are for individual, personal use only. Reselling, republishing, or forwarding the materials to libraries or reading rooms is prohibited.
ASCE Library Card (5 downloads)
$105.00
Add to cart
ASCE Library Card (20 downloads)
$280.00
Add to cart
Buy Single Article
$35.00
Add to cart

Media

Figures

Other

Tables

Share

Share

Copy the content Link

Share with email

Email a colleague

Share