Skip to main content
SpringerLink
Log in

Occurrence and fate of steroid estrogens in the largest wastewater treatment plant in Beijing, China

  • Published:
Environmental Monitoring and Assessment Aims and scope Submit manuscript

Abstract

Concern over steroid estrogens has increased rapidly in recent years due to their adverse health effects. Effluent discharge from wastewater treatment plants (WWTPs) is the main pollutant source for environmental water. To understand the pollutant level and fate of steroid estrogens in WWTPs, the occurrence of estrone (E1), 17-β-estradiol (E2), estriol (E3), and 17-β-ethinylestradiol (EE2) was investigated in the Gaobeidian WWTP in Beijing, China. Water samples from influent as well as effluent from second sedimentation tanks and advanced treatment processes were taken monthly during 2006 to 2007. In influent, steroid estrogen concentrations varied from 11.6 to 1.1 × 102 ng/l, 3.7 to 1.4 × 102 ng/l, no detection (nd) to 7.6×102 ng/l and nd to 3.3 × 102 ng/l for E1, E2, E3, and EE2, respectively. Compared with documented values, the higher steroid estrogen concentrations in the WWTP influent may be due to higher population density, higher birthrate, less dilution, and different sampling time. Results revealed that a municipal WWTP with an activated sludge system incorporating anaerobic, anoxic, and aerobic processes could eliminate natural and synthetic estrogens effectively. The mean elimination efficiencies were 83.2%, 96.4%, 98.8%, and 93.0% for E1, E2, E3, and EE2, respectively. The major removal mechanism for natural estrogens and synthetic estrogen EE2 were biodegradation and sorption on the basis of mass balance in water, suspension particles, and sludge. In the WWTP effluent, however, the highest concentrations of E1, E2, E3, and EE2 attained were 74.2, 3.9, 5.1, and 4.6 ng/l, respectively. This is concerning as residual steroid estrogens in WWTP effluent could lead to pollution of the receiving water. Advanced flocculation treatment was applied in the WWTP and transformed the residual estrogen conjugates to free species, which were reduced further by filtration with removal shifting from 32% to 57% for natural estrogen, although no EE2 was removed.

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

Access this article

Log in via an institution

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

Instant access to the full article PDF.

Institutional subscriptions

Fig. 1
Fig. 2
Fig. 3
Fig. 4
Fig. 5
Fig. 6

Similar content being viewed by others

References

  • Andersen, H., Siegrist, H., Halling, S. B., & Ternes, T. A. (2003). Fate of estrogens in a municipal sewage treatment plant. Environmental Sciences and Technology, 37, 4021–4026.

    Article  CAS  Google Scholar 

  • Atalay, E., Karaali, K., Akar, M., Ari, E. S., Simsek, M., Atalay, S., & Zorlu, G. (2005). Early impact of hormone replacement therapy on vascular hemodynamics detected via ocular colour. Doppler analysis Maturitas, 50, 282–288.

    CAS  Google Scholar 

  • Baronti, C., Curini, R., D’Ascenzo, G., Di Corcia, A., Gentili, A., & Samperi, R. (2000). Monitoring natural and synthetic estrogens at activated sludge sewage treatment plants and in a receiving river water. Environmental Sciences and Technology, 34, 5059–5066.

    Article  CAS  Google Scholar 

  • Beijing Statistical Yearbook (2006), Beijing Municipal Bureau of Statistics, www.bjstats.gov.cn/tjnj/2006-tjnj/content/mV98_08-10.htm.

  • Belfroid, A. C., Van der Horst, A., Vethaak, A. D., Schäfer, A. J., Rijs, G. B. J., Wegener, J., & Cofino, W. P. (1999). Analysis and occurrence of estrogenic hormones and their glucuronides in surface water and waste water in The Netherlands. The Science of the Total Environment, 225, 101–108.

    Article  CAS  Google Scholar 

  • Birkett, J. W., & Lester, J. N. (2003). Endocrine Disrupters in Wastewater and Sludge Treatment Processes. Boca Raton London New York Washington, D.C: ACRC Press Company.

    Google Scholar 

  • Blok, J., Wösten, M. A. D. (2000). Origin and fate of natural estrogens in the environment (in Dutch) RIWA. Amsterdam, Haskoning.

  • Braga, O., Smythe, G., Schafer, A. I., & Feitz, R. J. (2005). Fate of steroid estrogens in Australian inland and coastal wastewater treatment plants. Environmental Sciences and Technology, 39, 3351–3358.

    Article  CAS  Google Scholar 

  • Carballa, M., Fink, G., Omi, l. F., Lema, J. M., & Ternes, T. (2008). Determination of the solid–water distribution coefficient (Kd) for pharmaceuticals, estrogens and musk fragrances in digested sludge. Water Research, 42, 287–295.

    Article  CAS  Google Scholar 

  • Cargouët, M., Perdiz, D., Mouatassim, S. A., Tamisier, K. S., & Levi, Y. (2004). Assessment of river contamination by estrogenic compounds in Paris area (France). The Science of the Total Environment, 324, 55–66.

    Article  Google Scholar 

  • Chang, H., Wan, Y., Wu, S., Fan, Z., & Hu, J. (2011). Occurrence of androgens and progestogens in wastewater treatment plants and receriving river waters: Comparison to estrogens. Water Research, 45, 732–740.

    Article  CAS  Google Scholar 

  • Chen, C., Wen, T., Wang, G., Cheng, H., Lin, Y., & Lien, G. W. (2007). Determining estrogenic steroids in Taipei waters and removal in drinking water treatment using high-flow solid-phase extraction and liquid chromatography/tandem mass spectrometry. The Science of the Total Environment, 378, 352–365.

    Article  CAS  Google Scholar 

  • Christensen, F. M. (1998). Pharmaceuticals in the environment; a human risk? Regulatory Toxicology Pharmmacology, 28(3), 212–221.

    Article  CAS  Google Scholar 

  • Clara, M., Strenn, B., Saracevic, E., & Kreuzinger, N. (2004). Adsorption of bisphenol-A, 17β-estradiole and 17α-ethinylestradiole to sewage sludge. Chemosphere, 56, 843–851.

    Article  CAS  Google Scholar 

  • Cui, C., Ji, S., & Ren, H. (2006). Determination of steroid estrogens in wastewater treatment plant of a controceptives producing factory. Environmental Monitoring and Assessment, 121, 409–419.

    Article  CAS  Google Scholar 

  • D’Ascenzo, G., Di Corcia, A., Gentili, A., Mancini, R., Mastropasqua, R., Nazzari, M., & Samperi, R. (2003). Fate of natural estrogen conjugates in municipal sewage transport and treatment facilities. The Science of the Total Environment, 302, 199–209.

    Article  Google Scholar 

  • David, R. H., John, T. N., Thomas, J. G., & Nancy, G. L. (2002). Estrogen receptor agonist fate during wastewater and biosolids treatment processes: A mass balance analysis. Environmental Sciences and Technology, 36, 4533–4539.

    Article  Google Scholar 

  • Desbrow, C., Routledge, E. J., Brighty, G. C., Sumpter, J. P., & Waldock, M. (1998). Identification of estrogenic chemicals in STW effluent. 1. Chemical fractionation and in vitro biological screening. Environmental Sciences and Technology, 32, 1549–1558.

    Article  CAS  Google Scholar 

  • Fan, Z., Wu, S., Chang, H., & Hu, J. (2011). Behavior of glucocorticoids, androgens and progestogens in a municipal sewage treatment plant: Comparison to estrogens. Environmental Sciences and Technology, 45, 2725–2733.

    Article  CAS  Google Scholar 

  • Fawell, J. K., Sheahan, D., James, H. A., Hurst, M., & Scott, S. (2001). Oestrogens and oestrogenic activity in raw and treated water in Seven Trent Water. Water Research, 35(5), 1240–1244.

    Article  CAS  Google Scholar 

  • Jin, S., Yang, F., Liao, T., Hui, Y., & Xu, Y. (2008). Seasonal variation of estrogenic compounds and their estrogenicities in influent and effluent from a municipal sewage treatment plant in China. Environmental Toxicology and Chemistry, 27(1), 146–153.

    Article  CAS  Google Scholar 

  • Jobling, S., Nolan, M., Tyler, C. R., Brighty, G., & Sumpter, J. P. (1998). Widespread sexual disruption in wild fish. Environmental Sciences and Technology, 32, 2498–2506.

    Article  CAS  Google Scholar 

  • Johnson, A. C., & Sumpter, J. P. (2001). Removal of endocrine disrupting chemicals in activated sludge treatment works. Environmental Sciences and Technology, 35(24), 4697–4703.

    Article  CAS  Google Scholar 

  • Johnson, A. C., & Williams, R. J. (2004). A model to estimate influent and effluent concentrations of estradiol, estrone, and ethinylestradiol at sewage treatment works. Environmental Sciences and Technology, 38(13), 3649–3658.

    Article  CAS  Google Scholar 

  • Johnson, A. C., Belfroid, A., & Di Corcia, A. (2000). Estimating steroid oestrogen inputs into activated sludge treatment works and observations on their removal from the effluent. The Science of the Total Environment, 256(2–3), 163–173.

    Article  CAS  Google Scholar 

  • Katzung, B. G. (1995). Basic & clinical pharmacology. Norwalk, Connecticut: Appleton & Lange.

    Google Scholar 

  • Kirk, L. A., Tyler, C. R., Lye, C. M., & Sumpter, J. P. (2002). Changes in estrogenic and androgenic activities at different stages of treatment in wastewater treatment works. Environmental Toxicology and Chemistry, 21(5), 972–979.

    Article  CAS  Google Scholar 

  • Kolpin, D. W., Furlong, E. T., Meyer, M. T., Thurman, E. M., Zaugg, S. D., Barber, L. B., & Buxton, H. T. (2002). Pharmaceuticals, hormones, and other organic wastewater contaminants in U.S. streams, 1999–2000: A national reconnaissance. Environmental Sciences and Technology, 36, 1202–1211.

    Article  CAS  Google Scholar 

  • Körner, W., Bolz, U., Sussmuth, W., Hiller, G., Schuller, W., Hanf, V., & Hagenmaier, H. (2000). Input/output balance of estrogenic active compounds in a major municipal sewage plant in Germany. Chemosphere, 40, 1131–1142.

    Article  Google Scholar 

  • Kuster, M., Maria, J. L. A., & Barcelo, D. (2004). Analysis and distribution of estrogens and progestogens in sewage sludge, soils and sediments. TrAC Trends in Analytical Chemistry, 23(10–11), 790–798.

    Article  CAS  Google Scholar 

  • Kuster, M., Alda, M. J. L., & Barceló, D. (2005). Estrogens and progestogens in wastewater, sludge, sediments, and soil (pp. 1–24). Verlag Berlin Heidelberg: Springer.

    Google Scholar 

  • Lai, K. M., Johnson, K. L., Scrimshaw, M. D., & Lester, J. N. (2000). Binding of water borne steroid estrogens to solid phases in river and estuarine systems. Environmental Sciences and Technology, 34, 3890–3894.

    Article  CAS  Google Scholar 

  • Larsson, D. G. J., Adolfsson-Erici, M., Parkkonen, J., Pettersson, M., Berg, A. H., Olsson, P. E., & Forlin, L. (1999). Ethinyloestradiol—An undesired fish contraceptive? Aquatic Toxicology, 45, 91–97.

    Article  CAS  Google Scholar 

  • Layton, A. C., Gregory, B. W., Seward, J. R., Schultz, T. W., & Sayler, G. S. (2000). Mineralization of steroidal hormones by biosolids in wastewater treatment systems in Tennessee U.S.A. Environmental Sciences and Technology, 34(18), 3925–3931.

    Article  CAS  Google Scholar 

  • Lee, H. B., & Liu, D. (2002). Degradation of 17β-eatradiol and its metabolites by sewage bacteria. Water, Air, & Soil Pollution, 134, 353–368.

    Article  CAS  Google Scholar 

  • Lei, B., Huang, S., Zhou, Y., Wang, D., & Wang, Z. (2009). Levels of six estrogens in water and sediment from three rivers in Tianjin area, China. Chemosphere, 76, 36–42.

    Article  CAS  Google Scholar 

  • Ma, T., Wan, X., Huang, Q., Wang, Z., & Liu, J. (2005). Biomarker responses and reproductive toxicity of the effluent from a Chinese large sewage treatment plant in Japanese medaka (Oryzias latipes). Chemosphere, 59, 281–288.

    Article  CAS  Google Scholar 

  • Ma, M., Rao, K., & Wang, Z. (2007). Occurrence of estrogenic effects in sewage and industrial wastewaters in Beijing, China. Environmental Pollution, 147, 331–336.

    Article  CAS  Google Scholar 

  • Maggs, J. L., Grimmer, S. F. M., L’e-Orme, M., Breckenridge, A. M., Park, B. K., & Gilmore, I. T. (1983). The biliary and urinary metabolites of [3H] 17α-ethynylestradiol in women. Xenobiotica, 13(7), 421–431.

    Article  CAS  Google Scholar 

  • Martinović, D., Denny, J. S., Schmieder, P. K., Ankley, G. T., & Sorensen, P. W. (2008). Temporal variation inthe estrogenicity of a sewage treatment plant effluent and its biological significance. Environmental Sciences and Technology, 42, 3421–3427.

    Article  Google Scholar 

  • Mastrup, M., Jensen, R. L., Schfäer, A. I., & Khan, S. (2001). Fate modeling—An important tool for water recycling. In A. I. Schfäer, P. Sherman, & T. D. Waite (Eds.), Recent advances in water recycling technologies (pp. 103–112). Brisbane: Australia.

    Google Scholar 

  • Matsui, S., Takigami, H., Matsuda, T., Taniguchi, N., Adachi, J., Kawami, H., & Shimizu, Y. (2000). Estrogen and estrogen mimics contamination in water and the role of sewage treatment. Water Science and Technology, 42, 173–179.

    CAS  Google Scholar 

  • Means, J. C., Wood, S. G., Hasset, J. J., & Banwart, W. L. (1982). Sorption of amino- and carboxy-substituted polynuclear aromatic hydrocarbons by sediments and soils. Environmental Sciences and Technology, 16(2), 93–98.

    Article  CAS  Google Scholar 

  • Muriel, A., Youssef, F. M., Rajeshwar, D. T., Craig, D. A., & Rao, Y. S. (2006). Endocrine disrupting compounds removal from wastewater, a new challenge. Process Biochemistry, 41, 525–539.

    Article  Google Scholar 

  • Nakada, N., Shinohara, H., Murata, A., Kiri, K., Managaki, S., Sato, N., & Takada, H. (2007). Removal of selected pharmaceuticals and personal care products (PPCPs) and endocrine-disrupting chemicals (EDCs) during sand filtration and ozonation at a municipal sewage treatment plant. Water Research, 41, 4373–4382.

    Article  CAS  Google Scholar 

  • Ong, P. E. A., Chang, S., Waite, T. D., Schäfer, A. I. Fane AG. Removal of trace contamination using coagulation, PAC and microfiltration hybrid processes. In: Recent advances in water recycling technologies. 26 November 2001 Workshop, Brisbane.

  • Peter, G. F. (1990). Metabolism of 17 [alpha]-ethynylestradiol in humans. Life Sciences, 47, 1981–1988.

    Article  Google Scholar 

  • Ranney, R. E. (1977). Comparative metabolism of 17α-ethynyl steroid used in oral contraceptive. Journal of Toxicology and Environmental Health, 3, 139–166.

    Article  CAS  Google Scholar 

  • Rodgers-Gray, T. P., Jobling, S., Morris, S., Kelly, C., Kirby, S., Janbakhsh, A., Harries, J. E., Waldock, M. J., Sumpter, J. P., & Tyler, C. R. (2000). Long-term temporal changes in the estrogenic composition of treated sewage effluent and its biological effects on fish. Environmental Sciences and Technology, 34, 1521–1528.

    Article  CAS  Google Scholar 

  • Rogers, H. R. (1996). Sources, behaviour and fate of organic contaminants during sewage treatment and sewage sludges. The Science of the Total Environment, 185, 3–26.

    Article  CAS  Google Scholar 

  • Routledge, E. J., Sheahan, D., Desbrow, C., Brighty, G. C., Waldock, M., & Sumpter, J. P. (1998). Identification of estrogenic chemicals in STW effluent. 2. In vivo responses in trout and roach. Environmental Sciences and Technology, 32, 1559–1565.

    Article  CAS  Google Scholar 

  • Servos, M. R., Bennie, D. T., Burnison, B. K., Jurkovic, A., McInnis, R., Neheli, T., Schnell, A., Seto, P., Smyth, S. A., & Ternes, T. A. (2005). Distribution of estrogens, 17[beta]-estradiol and estrone, in Canadian municipal wastewater treatment plants. The Science of the Total Environment, 336, 155–170.

    Article  CAS  Google Scholar 

  • Shore, L. S., Gurevitz, M., & Shemesh, M. (1993). Estrogen as an environmental pollutant. Bulletin of Environmental Contamination and Toxicology, 51, 361–366.

    Article  CAS  Google Scholar 

  • Sun, Q., Deng, S., Huang, J., Shen, G., & Yu, G. (2007). Contributors to estrogenic activity in wastewater from a large wastewater treatment plant in Beijing, China. Environmental Toxicology and Pharmacology, 25, 20–26.

    Article  Google Scholar 

  • Svenson, A., Allard, A., & Ek, M. (2003). Removal of estrogenicity in Swedish municipal sewage treatment plants. Water Research, 37(18), 4433–4443.

    Article  CAS  Google Scholar 

  • Tabak, H. H., Boomhuff, R. N., & Bunch, R. L. (1981). Steroid hormones as water pollutants II. Studies on the persistence and stability of natural urinary and synthetic ovulation-inhibiting hormones in untreated and treated wastewaters. Dev. Ind. Microbiol., 22, 497–519.

    CAS  Google Scholar 

  • Ternes, T. A. (1998). Occurrence of drugs in German sewage treatment plants and rivers. Water Research, 32(11), 3245–3260.

    Article  CAS  Google Scholar 

  • Ternes, T. A., Kreckel, P., & Mueller, J. (1999). Behavious and occurrence of estrogens in municipal sewage treatment plants—II. Aerobic batch experiments with activated sludge. The Science of the Total Environment, 225, 91–99.

    Article  CAS  Google Scholar 

  • Ternes, T. A., Stumpf, M., Mueller, J., Haberer, K., Wilken, R. D., & Servos, M. (1999). Behavious and occurrence of estrogens in municipal sewage treatment plants—I. Investigation in Germany, Canada and Brazil. The Science of the Total Environment, 225, 81–90.

    Article  CAS  Google Scholar 

  • Ternes, T. A., Andersen, H., Gilberg, D., & Bonerz, M. (2002). Determination of estrogens in sludge and sediments by liquid extraction and GC/MS/MS. Analytical Chemistry, 74, 3498–3504.

    Article  CAS  Google Scholar 

  • Tyler, C. R., Jobling, S. R., & Sumpter, J. P. (1998). Endocrine disruption in wildlife: a critical review of the evidence. Critical Reviews in Toxicology, 28, 319–361.

    Article  CAS  Google Scholar 

  • US Environmental Protection Agency. (1997). Special report on environmental endocrine disruption: An effects assessment and analysis, Washington, DC, USA, 111 p.

  • Vethaak, A. D., Lahr, J., Schrap, S. M., Belfroid, A. C., Rijs, G. B. J., Gerritsen, A., de Boer, J., Bulder, A. S., Grinwis, G. C. M., Kuiper, R. V., Legler, J., Murk, T. A. J., Peijnenburg, W., Verhaar, H. J. M., & de Voogt, P. (2005). An integrated assessment of estrogenic contamination and biological effects in the aquatic environment of The Netherlands. Chemosphere, 59, 511–524.

    Article  CAS  Google Scholar 

  • Zha, J., Sun, L., Zhou, Y., Ma, M., & Wang, Z. (2008). Assessment of 17a-ethinylestradiol effects and underlying mechanisms in a continuous, multigeneration exposure of the Chinese rare minnow (Gobiocypris, rarus). Toxicology and Applied Pharmacology, 226, 298–308.

    Article  CAS  Google Scholar 

  • Zhou, Y., Zhou, J., Xu, Y., Zha, J., Ma, M., & Wang, Z. (2009). An alternative method for the determination of estrogens in surface water and wastewater treatment plant effluent using pre-column trimethylsilyl derivatization and gas chromatography/mass spectrometry. Environmental Monitoring and Assessment, 158, 35–49.

    Article  CAS  Google Scholar 

  • Zhou, Y., Zha, J., Xu, Y., Lei B., Wang Z. (2011). Occurrences of six steroid estrogens from different effluents in Beijing, China. Environmental Monitoring and Assessment, in press.

Download references

Acknowledgements

We thank Dr. Jun Zhou for providing us with the WWTP information and Dr. Xiaoqing He for providing us with help during the sampling period. This work was supported by the Chinese Academy of Sciences (KZCX1-YW-06) and the National Basic Research Program of China (2007CB407301).

Author information

Authors and Affiliations

  1. State Key Laboratory of Environmental Aquatic Chemistry, Research Center for Eco-Environmental Sciences, Chinese Academy of Sciences, PO Box 2871, Beijing, 100085, People’s Republic China

    Yiqi Zhou, Jinmiao Zha & Zijian Wang

Authors
  1. Yiqi Zhou
    View author publications

    You can also search for this author in PubMed Google Scholar

  2. Jinmiao Zha
    View author publications

    You can also search for this author in PubMed Google Scholar

  3. Zijian Wang
    View author publications

    You can also search for this author in PubMed Google Scholar

Corresponding author

Correspondence to Zijian Wang.

Rights and permissions

Reprints and permissions

About this article

Cite this article

Zhou, Y., Zha, J. & Wang, Z. Occurrence and fate of steroid estrogens in the largest wastewater treatment plant in Beijing, China. Environ Monit Assess 184, 6799–6813 (2012). https://doi.org/10.1007/s10661-011-2459-y

Download citation

  • Received:

  • Accepted:

  • Published:

  • Issue Date:

  • DOI: https://doi.org/10.1007/s10661-011-2459-y

Keywords

Search

Navigation