The global distribution of linear and cyclic volatile methyl silxoanes (VMS) was investigated at 20 sites worldwide, including 5 locations in the Arctic, using sorbent-impregnated polyurethane foam (SIP) disk passive air samplers. Cyclic VMS are currently being considered for regulation because they are high production volume chemicals that are potentially persistent, bioaccumulative, and toxic. Linear and cyclic VMS (including L3, L4, L5, D3, D4, D5, and D6) were analyzed for in air at all urban, background, and Arctic sites. Concentrations of D3 and D4 are significantly correlated, as are D5 and D6, which suggests different sources for these two pairs of compounds. Elevated concentrations of D3 and D4 on the West coast of North America and at high elevation sites suggest these sites are influenced by trans-Pacific transport, while D5 and D6 have elevated concentrations in urban areas, which is most likely due to personal care product use. Measured concentrations of D5 were compared to modeled concentrations generated using both the Danish Eulerian Hemispheric Model (DEHM) and the Berkeley-Trent Global Contaminant Fate Model (BETR Global). The correlation coefficients (r) between the measured and modeled results were 0.73 and 0.58 for the DEHM and BETR models, respectively. Agreement between measurements and models indicate that the sources, transport pathways, and sinks of D5 in the global atmosphere are fairly well understood.
Decamethylcyclopentasiloxane (D(5)) is a volatile compound used in personal care products that is released to the atmosphere in large quantities. Although D(5) is currently under consideration for regulation, there have been no field investigations of its atmospheric fate. We employed a recently developed, quality assured method to measure D(5) concentration in ambient air at a rural site in Sweden. The samples were collected with daily resolution between January and June 2009. The D(5) concentration ranged from 0.3 to 9 ng m(-3), which is 1-3 orders of magnitude lower than previous reports. The measured data were compared with D(5) concentrations predicted using an atmospheric circulation model that included both OH radical and D(5) chemistry. The model was parametrized using emissions estimates and physical chemical properties determined in laboratory experiments. There was good agreement between the measured and modeled D(5) concentrations. The results show that D(5) is clearly subject to long-range atmospheric transport, but that it is also effectively removed from the atmosphere via phototransformation. Atmospheric deposition has little influence on the atmospheric fate. The good agreement between the model predictions and the field observations indicates that there is a good understanding of the major factors governing D(5) concentrations in the atmosphere.
River ecosystems are influenced by contaminants in the water column, in the pore water and adsorbed to sediment particles. When exchange across the sediment‐water interface (hyporheic exchange) is included in modeling, the mixing coefficient is often assumed to be constant with depth below the interface. Novel fiber‐optic fluorometers have been developed and combined with a modified EROSIMESS system to quantify the vertical variation in mixing coefficient with depth below the sediment‐water interface. The study considered a range of particle diameters and bed shear velocities, with the permeability Péclet number, PeK between 1000 and 77,000 and the shear Reynolds number, Re*, between 5 and 600. Different parameterization of both an interface exchange coefficient and a spatially variable in‐sediment mixing coefficient are explored. The variation of in‐sediment mixing is described by an exponential function applicable over the full range of parameter combinations tested. The empirical relationship enables estimates of the depth to which concentrations of pollutants will penetrate into the bed sediment, allowing the region where exchange will occur faster than molecular diffusion to be determined.
Cyclic volatile methylsiloxanes are being subjected to regulatory scrutiny as possible PBT chemicals. The investigation of bioaccumulation has yielded apparently contradictory results, with high laboratory fish bioconcentration factors on the one hand and low field trophic magnification factors on the other. In this study, octamethylcyclotetrasiloxane (D4), decamethylcyclopentasiloxane (D5), and dodecamethylcyclohexasiloxane (D6) were studied along with polychlorinated biphenyls (PCBs) in sediments, ragworm, and flounder from six sites in the Humber Estuary. Bioaccumulation was evaluated using multimedia bioaccumulation factors (mmBAFs) which quantified the fraction of the contaminant present in the aquatic environment that is transferred to the biota. PCB 180, a known strongly bioaccumulative chemical, was used as a benchmark. The mean mmBAF of D5 was about twice that of PCB 180 in both polycheates and flounder, while for D4 it was 6 and 14 times higher, respectively. The mmBAF of D6 was a factor 5-10 lower than that of PCB180. The comparatively strong multimedia bioaccumulation of D4 and D5, even in the absence of biomagnification, was explained by both compounds having a >100 times stronger tendency to partition into lipid rather than into organic carbon, while PCB 180 partitions to a similar extent into both matrices.
Triclosan (TCS) is a broad-spectrum antimicrobial used in consumer products including toothpaste and hand soap. After being used, TCS is washed or rinsed off and residuals that are not biodegraded or otherwise removed during wastewater treatment can enter the aquatic environment in wastewater effluents and sludges. The environmental exposure and toxicity of TCS has been the subject of various scientific and regulatory discussions in recent years. There have been a number of publications in the past 5 y reporting toxicity, fate and transport, and in-stream monitoring data as well as predictions from aquatic risk assessments. State-of-the-science probabilistic exposure models, including Geography-referenced Regional Exposure Assessment Tool for European Rivers (GREAT-ER) for European surface waters and Pharmaceutical Assessment and Transport Evalutation (PhATEe) for US surface waters, have been used to predict in-stream concentrations (PECs). These models take into account spatial and temporal variability in river flows and wastewater emissions based on empirically derived estimates of chemical removal in wastewater treatment and in receiving waters. These model simulations (based on realistic use levels of TCS) have been validated with river monitoring data in areas known to be receiving high wastewater loads. The results suggest that 90th percentile (low flow) TCS concentrations are less than 200 ng/L for the Aire-Calder catchment in the United Kingdom and between 250 ng/L (with in-stream removal) and 850 ng/L (without in-stream removal) for a range of US surface waters. To better identify the aquatic risk of TCS, a species sensitivity distribution (SSD) was constructed based on chronic toxicity values, either no observed effect concentrations (NOECs) or various percentile adverse effect concentrations (EC10-25 values) for 14 aquatic species including fish, invertebrates, macrophytes, and algae. The SSD approach is believed to represent a more realistic threshold of effect than a predicted no effect concentration (PNEC) based on the data from the single most sensitive species tested. The log-logistic SSD was used to estimate a PNEC, based on an HC5,50 (the concentration estimated to affect the survival, reproduction and/or growth of 5% of species with a 50% confidence interval). The PNEC for TCS was 1,550 ng/L. Comparing the SSD-based PNEC with the PECs derived from GREAT-ER and PhATE modeling to simulate in-river conditions in Europe and the United States, the PEC to PNEC ratios are less than unity suggesting risks to pelagic species are low even under the highest likely exposures which would occur immediately downstream of wastewater treatment plant (WWTP) discharge points. In-stream sorption, biodegradation, and photodegradation will further reduce pelagic exposures of TCS. Monitoring data in Europe and the United States corroborate the modeled PEC estimates and reductions in TCS concentrations with distance downstream of WWTP discharges. Environmental metabolites, bioaccumulation, biochemical responses includ...
Triclosan (TCS) is a broad-spectrum antimicrobial used in consumer products including toothpaste and hand soap. After being used, TCS is washed or rinsed off and residuals that are not biodegraded or otherwise removed during wastewater treatment can enter the aquatic environment in wastewater effluents and sludges. The environmental exposure and toxicity of TCS has been the subject of various scientific and regulatory discussions in recent years. There have been a number of publications in the past 5 y reporting toxicity, fate and transport, and in-stream monitoring data as well as predictions from aquatic risk assessments. State-of-the-science probabilistic exposure models, including Geography-referenced Regional Exposure Assessment Tool for European Rivers (GREAT-ER) for European surface waters and Pharmaceutical Assessment and Transport Evalutation (PhATE) for US surface waters, have been used to predict in-stream concentrations (PECs). These models take into account spatial and temporal variability in river flows and wastewater emissions based on empirically derived estimates of chemical removal in wastewater treatment and in receiving waters. These model simulations (based on realistic use levels of TCS) have been validated with river monitoring data in areas known to be receiving high wastewater loads. The results suggest that 90th percentile (low flow) TCS concentrations are less than 200 ng/L for the Aire-Calder catchment in the United Kingdom and between 250 ng/L (with in-stream removal) and 850 ng/L (without in-stream removal) for a range of US surface waters. To better identify the aquatic risk of TCS, a species sensitivity distribution (SSD) was constructed based on chronic toxicity values, either no observed effect concentrations (NOECs) or various percentile adverse effect concentrations (EC10-25 values) for 14 aquatic species including fish, invertebrates, macrophytes, and algae. The SSD approach is believed to represent a more realistic threshold of effect than a predicted no effect concentration (PNEC) based on the data from the single most sensitive species tested. The log-logistic SSD was used to estimate a PNEC, based on an HC5,50 (the concentration estimated to affect the survival, reproduction and/or growth of 5% of species with a 50% confidence interval). The PNEC for TCS was 1,550 ng/L. Comparing the SSD-based PNEC with the PECs derived from GREATER and PhATE modeling to simulate in-river conditions in Europe and the United States, the PEC to PNEC ratios are less than unity suggesting risks to pelagic species are low even under the highest likely exposures which would occur immediately downstream of wastewater treatment plant (WWTP) discharge points. In-stream sorption, biodegradation, and photodegradation will further reduce pelagic exposures of TCS. Monitoring data in Europe and the United States corroborate the modeled PEC estimates and reductions in TCS concentrations with distance downstream of WWTP discharges. Environmental metabolites, bioaccumulation, biochemical responses includin...
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