An understanding of solute-solute interactions is essential for aquatic systems as this can affect the fate and behaviour of micropollutants in the environment and engineered systems. Despite the importance of solute-solute interactions there is a general lack of understanding which may be attributed to the fact that many engineering models overlook solute-solute interactions and that the quantification of such interactions is inherently difficult. When solute-solute interactions are considered, they are often studied at unrepresentative concentrations and do not consider the influence of organic matter type or solution chemistry. Steroidal hormones, such as estradiol and estrone, were selected as model micropollutants as they are ubiquitous in the aquatic environment due to constant introduction of wastewater effluent, and can have implications for growth and development of organisms including impaired fertility and behavioural abnormalities. The purpose of this study was to develop a methodology to quantify solute-solute interactions at environmental concentrations, and to determine the implications of such interactions in membrane filtration. A solid-phase microextraction (SPME) technique was developed to quantify solutesolute interactions at environmental (low) concentrations. Using SPME, organic matter-water partition coefficients (log KOM) were measured for a range of steroidal hormones including estradiol, estrone, progesterone and testosterone with different organic matter types such as humic acid. The dominant mechanism of hormoneorganic matter interactions was identified as hydrogen bonding. In the case of estrone and progesterone the log KOM values were significantly influenced by organic matter type and concentration, as well as solution chemistry. No difference was observed for estradiol and testosterone due to generally weaker sorption to organic matter. Previous studies have indicated that the presence of organic matter can alter micropollutant retention in membrane filtration. Much of the current literature focuses on solute-membrane interactions, as the influence of solute-solute interactions are typically difficult to determine in membrane filtration. Therefore, hormone-organic matter interactions were studied to determine if this interaction had an influence on hormone removal by ultrafiltration (UF) using a range of molecular weight cut-off (MWCO) membranes. The results indicated increased retention of estrone in the presence of humic acid, while organic matter concentration and solution chemistry influenced retention by affecting solute-solute interactions. The findings of this study indicate the importance of solute-solute interactions in membrane filtration and experimental log KOM results were used to quantify the findings and elucidate the influences of 1) membrane sorption, 2) solute-solute interactions and 3) solute-foulant interactions. Further, the removal of steroidal hormones using a magnetic ion exchange (MIEX®) resin with a range of MWCO UF membranes was studied as such sorbents can be used to improve micropollutant removal in wastewater treatment. Greater removal with IX-UF was observed compared to UF alone and the main hormone removal mechanisms were sorption to MIEX® and solute-fouling interactions. The findings of this study indicate that it is indeed possible to quantify solute-solute interactions at environmental concentrations using SPME, with hydrogen bonding being the main mechanism of interaction for steroidal hormones and organic matter. Further, micropollutant retention by membrane filtration can be influenced by solutesolute interactions.
| Identifer | oai:union.ndltd.org:bl.uk/oai:ethos.bl.uk:562594 |
| Date | January 2009 |
| Creators | Neale, Peta Anne |
| Contributors | Schäfer, Andrea. : Glass, Donald |
| Publisher | University of Edinburgh |
| Source Sets | Ethos UK |
| Detected Language | English |
| Type | Electronic Thesis or Dissertation |
| Source | http://hdl.handle.net/1842/4106 |
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