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
Showing items related by title, author, creator and subject.
The ecology of colonial radiolarians : their colony morphology, trophic interactions and associations, behavior, distribution, and the photosynthesis of their symbionts Swanberg, Neil Ralph (Massachusetts Institute of Technology and Woods Hole Oceanographic Institution, 1979-08)Colonial radiolarians (Spumellaria) are among the most common and abundant large zooplankton, but they have been little studied by modern biologists. Colonies were found on 98% of epipelagic diving stations in the period ...
A determination of air-sea gas exchange and upper ocean biological production from five noble gases and tritiugenic helium-3 Stanley, Rachel H. R. (Massachusetts Institute of Technology and Woods Hole Oceanographic Institution, 2007-09)The five noble gases (helium, neon, argon, krypton, and xenon) are biologically and chemically inert, making them ideal oceanographic tracers. Additionally, the noble gases have a wide range of solubilities and molecular ...
Elkins, Lynne J. (Massachusetts Institute of Technology and Woods Hole Oceanographic Institution, 2009-02)To explore the ability of melting mafic lithologies to produce alkaline ocean-island basalts (OIB), an experimental study was carried out measuring clinopyroxene (Cpx)- melt and garnet (Gt)-melt partition coefficients ...