Bioaccumulation of 17α-Ethinylestradiol in Fish

The active synthetic constituent of oral contraceptives 17α- ethinylestradiol (EE2) and its natural steroidal estrogen analogues are being released into the aquatic environment mainly via wastewater treatment plants (WWTPs). Although steroidal estrogens have been frequently reported in very low concentrations in the environment, they have been placed at the top of the list of endocrine disrupting chemicals (EDCs) for their high estrogenic activity in non-target aquatic species like fish and frogs. Almost 30 years worth of intensive research has moved the problem of endocrine disruption in the aquatic environment from being a hypothesis to a well-known cause-and-effect story. However, the fate and effects of many pharmaceuticals, including EE2, remain poorly understood. Thus, the main objective of this thesis was to investigate EE2 bioaccumulation in fish by field and laboratory studies. An optimized sample preparation and analytical method protocol was achieved to detect EE2 in its biologically active form in whole fish tissue at trace levels (ng/g). Shorthead redhorse suckers (ShRHS) (Moxostoma macrolepidotum) collected in proximity to a WWTP in the St. Clair River have significantly accumulated EE2 with an average of 1.5 ng/g. EE2 bioaccumulation was limited to fish exhibiting intersex and with induced vitellogenin (VTG). EE2 was absent in fish from a reference site. Positive correlations between EE2 and lipid content as well as "15N supported the hypothesis of EE2 bioaccumulation in wild ShRHSs. A wider survey was carried out to explore patterns of EE2 bioaccumulation in the pelagic and benthic food-wed of the St. Clair IV River, Ontario. In the WWTP effluents and nearby surface waters, EE2 levels were extremely low and below our method detection limits. All of the seven sampled species from different trophic levels and the sediment samples collected from the impacted sites and the reference sites did not have any measurable EE2 concentrations. A laboratory controlled study where male goldfish (Carassius auratus) were exposed to EE2 via water versus food demonstrated that fish can rapidly accumulate EE2 by both routes of exposure. The uptake constant for water was 45 h-1 and the bioconcentration factor for EE2 in fish was 377. The fast uptake rate of EE2 via water coincided with a much slower elimination rate constant of 0.0786 h-1. The assimilation efficiency of 0.106 for EE2 by goldfish was determined by EE2 dietary exposure, which was used to predict EE2 accumulation under different exposure scenarios. The work presented here was the first demonstration of EE2 bioaccumulation in wild fish and the first to model EE2 bioaccumulation from water and dietary exposure in laboratory-exposed fish