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    Natural and synthetic estrogens in wastewater treatment plant effluent and the coastal ocean

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    Griffith_thesis.pdf (12.53Mb)
    Date
    2013-09
    Author
    Griffith, David R.  Concept link
    Metadata
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    Citable URI
    https://hdl.handle.net/1912/6285
    Location
    Massachusetts Bay
    DOI
    10.1575/1912/6285
    Keyword
     Water reuse; Chemical oceanography; Oceanus (Ship : 1975-) Cruise OC437; Louis S. St. Laurent (Ship) Cruise 
    Abstract
    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
    Collections
    • WHOI Theses
    • Marine Chemistry and Geochemistry (MC&G)
    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/1912/6285
     

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