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Evaluating the fate and behaviour of cyclic volatile methyl siloxanes in two contrasting North American lakes using a multi-media model

Whelan, M.J.
Chemosphere 2013 v.91 pp. 1566-1576
emissions, half life, hydrolysis, lakes, models, partition coefficients, sediments, siloxanes, temperature, wastewater, wastewater treatment, watersheds, Lake Ontario, Minnesota, Mississippi River, Wisconsin
The behaviour of cyclic volatile methyl siloxanes (cVMS) in lakes was explored using a fugacity-based steady-state non-equilibrium multimedia fate and transport model (a modified version of QWASI). Three substances were investigated: Octamethylcyclotetrasiloxane (D4), Decamethylcyclopentasiloxane (D5) and Dodecamethylcyclohexasiloxane (D6) in two contrasting North American lakes: Lake Ontario and Lake Pepin (a natural shallow lake on the Mississippi river between Minnesota and Wisconsin). Values for the principal partition coefficients and the hydrolysis rate constant were adjusted for the mean annual temperatures of each lake. Hydrolysis rate constants were also adjusted for the fraction of chemical calculated to be in the freely dissolved phase. Half-lives in sediment were calculated from partitioning theory, assuming hydrolysis can occur only in the dissolved phase. Best estimates of substance-specific emissions were obtained by combining current per capita approximations of usage and fraction lost to domestic waste water, the population of the lake catchment and cVMS removal in waste water treatment. Concentrations were generally lower and chemical residence times longer in Lake Ontario than in Lake Pepin, owing to greater depth, a higher hydraulic retention time and a higher degree of dilution. Overall persistence in Lake Pepin is significantly influenced by the high rate of sediment burial assumed in the model, as well as by a relatively high rate of water discharge. Despite the many similarities of the compounds considered, the dominant loss mechanisms vary significantly and are not the same in each lake system. This highlights the pitfalls of subjective evaluation of chemical fate and illustrates the important role which models have to play in providing a quantitative framework for assessing chemical behaviour objectively under the influence of a complex and interacting set of factors.