Wilkinson, John L. (2017) Occurrence, bioaccumulation, fate and transport of pharmaceuticals, plasticisers, illicit drugs and perfluorinated compounds in the aquatic environment. (PhD thesis), Kingston University, .

Abstract

Mass produced chemicals have revolutionised the way in which humans live and has led to both a significant increase in quality of life and a concomitant change in the way we pollute our habitats. Such chemicals include pharmaceuticals, plasticisers, perfluorinated compounds and metabolites which enter rivers via sources such as sewage treatment works (STW) effluent outfalls. The presence and distribution of these contaminants is of concern due to their increasing use and ability of some to biologically affect non-target aquatic organisms at trace (ng/L) levels. This work investigated the fate and distribution of selected pharmaceuticals, plasticisers, illict drugs, perfluorinated compunds (PFCs) and metabolites are investigated in three rivers of southern England. Specific objectives included establishing spatial distribution patterns of selected contaminants along the entire course of rivers receiving inputs from multiple STWs, their partition between bound (to suspended particulate material) and dissolved phases of river water, accumulation in sediment, bioaccumulation in primary producers including plants and biofilm/ periphyton, bioaccumulation in benthic aquatic organisms, adsorption of studied contaminants to polyethlene microparticles (similar to those used in cosmetic products) both in the lab and in rivers, and adsorption to 'natural' replacements for polyethylene microparticles (MPs). Spatial distribution analysis showed that selected contaminants are ubiquitous in the studied rivers with trace levels of plasticisers and perfluorinated compounds identified in river headwaters and beyond. Within the rivers studied in this work, pharmaceuticals were shown to be exclusively introduced by STW effluent and persisted exclusively in the dissolved phase of river water through the studies areas. Plasticisers and PFCs however were additionally introduced via runoff from streets, at times at higher concentrations than in SFWs effluent outfall and bound to suspended particulate material. Only PFCs and plasticisers were found to be bioaccumulative or very bioaccumulative in aquatic plants, biofilm. periphton and benthic organisms, and accumulated in sediment. Illicit drugs were only found in STW effluent and downstream river flow, almost exclusively in the dissolved phase of collected water. Laboratory assessment of adsorption to polyethylene MPs showed adsorption largely occurred via a linear isotherm and only for PFCs. However, trace levels of pharmaceuticals and an illicit drug urinary metabolite were extracted from polyethylene MPs deployed downstream from STW effluent outfalls in three rivers. Investigation of a 'natural' alternative to polyethyle MPs (walnut husk Mps) showed adsorption to these replacement particles occurred to a greater amount with more of the studied contaminants than to polyethylene MPs. This work significantly contributes to the knowledge of organis contaminant occurrence, bioaccumulation, fate and distribution in the aquatic environment. Future research should focus on elucidating the fate and distribution of conugated pharmaceuticals and metabolites in the aquatic environment, establishing organism-specific contaminant bioaccumulation guideline, the effect of microparticle fragmentation on contaminant adsorption, identification of adsorption-free MPs for use in cosmetic products and developing study designs to incorporate environmental epigenetics with toxicology and chemistry in the aquatic environment.

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