Natural and synthetic estrogens in wastewater treatment plant effluent and the coastal ocean
Griffith, David R.
MetadataShow full item record
KeywordWater reuse; Chemical oceanography; Oceanus (Ship : 1975-) Cruise OC437; Louis S. St. Laurent (Ship) Cruise
Steroidal estrogens are potent endocrine disrupting chemicals that are naturally excreted by vertebrates (e.g., humans and fish) and can enter natural waters through the discharge of treated and raw sewage. Because estrogens are detrimental to aquatic organisms at picomolar concentrations, many studies have measured so-called “free” estrogen concentrations in wastewater effluents, rivers, and lakes. Yet, to our knowledge, no studies have characterized the broader range of estrogens that includes free, conjugated, and halogenated forms. Conjugated estrogens are important because they can be easily converted to potent free forms by bacteria in wastewater treatment plants and receiving waters. And halogenated estrogens, produced during wastewater disinfection, are only slightly less potent than free estrogens but much more likely to bioaccumulate. We have developed a tandem mass spectrometry method that is capable of simultaneously quantifying free, conjugated, and halogenated estrogens at picomolar levels in wastewater effluent and coastal seawater. The method was validated using treated effluent from the greater Boston metropolitan area, where we found that halogenated estrogens represented over 50% of the total estrogen discharge flux. A kinetic model of estrogen halogenation was used to predict the distribution of free and halogenated forms in wastewater effluent and suggested that chlorinated estrogens may be formed en route to the wastewater treatment plant. In the receiving waters of Massachusetts Bay, we detected a range of conjugated, free, and halogenated forms at concentrations that were well-predicted by dilution near the sewage outfall. Farther downstream, we found significantly higher estrone concentrations which points to large inputs of estrogens from sources other than sewage. Finally, we have used compound-specific measurements of 13C and 14C in commercial and pharmaceutical estrogen preparations to evaluate the potential for using carbon isotopes to distinguish between synthetic and endogenous steroids in wastewater and other environmental matrices. Our results show that synthetic estrogens and progestogens exhibit significantly depleted δ13C values (~ -30‰) compared to endogenous steroids (-16‰ to -26‰). This isotopic difference should make it possible to apportion synthetic and endogenous hormone sources in complex environments.
Submitted in partial fulfillment of the requirements for the degree of Doctor of Philosophy at the Massachusetts Institute of Technology and the Woods Hole Oceanographic Institution September 2013
Suggested CitationThesis: Griffith, David R., "Natural and synthetic estrogens in wastewater treatment plant effluent and the coastal ocean", 2013-09, DOI:10.1575/1912/6285, https://hdl.handle.net/1912/6285
Showing items related by title, author, creator and subject.
The Subduction experiment : cruise report R/V Oceanus : cruise number 240 leg 3 : subduction 1 mooring deployment cruise, 17 June-5 July 1991 Trask, Richard P.; Brink, Nancy J. (Woods Hole Oceanographic Institution, 1993-03)Subduction is the mechanism by which water masses formed in the mixed layer and near the surface of the ocean find their way into the upper thermocline. The subduction process and its underlying mechanisms were studied ...
Spatial variability of bottom turbulence over a linear sand ridge mooring deployment and AUTOSUB AUV survey cruise report R/V RRS Challenger, cruise number 146 Broken Bank, North Sea, U.K., 17 – 28 August 1999 cruise report Voulgaris, George; Trowbridge, John H.; Terray, Eugene A. (Woods Hole Oceanographic Institution, 2001-08)Two successful AUTOSUB deployments were carried out during August 1999 as part of the AUTOSUB Thematic Program project titled “Spatial Variability of Bottom Turbulence over a Linear Sand Ridge,” funded by the Natural ...
The Subduction experiment : cruise report RRS Charles Darwin cruise number 73 subduction 3 mooring deployment and recovery cruise, 30 September-26 October 1992 Trask, Richard P.; Jenkins, William J.; Sherman, Jeffrey; McPhee, Neil M.; Ostrom, William M.; Payne, Richard E. (Woods Hole Oceanographic Institution, 1993-03)Subduction is the mechanism by which water masses formed in the mixed layer and near the surface of the ocean find their way into the upper thermocline. The subduction process and its underlying mechanisms were studied ...