Natural and synthetic estrogens in wastewater treatment plant effluent and the coastal ocean
Citable URI
https://hdl.handle.net/1912/6285Location
Massachusetts BayDOI
10.1575/1912/6285Keyword
Water reuse; Chemical oceanography; Oceanus (Ship : 1975-) Cruise OC437; Louis S. St. Laurent (Ship) CruiseAbstract
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.
Description
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
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Suggested Citation
Thesis: 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/1912/6285Related items
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