Polychlorinated alkanes (PCAs), otherwise known as chlorinated paraffins, are contaminants of emerging Arctic concern where our understanding of their occurrence and trophic transfer in Arctic food webs remains limited. To investigate biomagnification potential of PCAs, we analyzed short-chain PCAs: C10-C13 and medium-chain PCAs-C14-17 in three Arctic species: polar cod (Boreogadus saida), ringed seal (Pusa hispida), and polar bear (Ursus maritimus) and Subarctic capelin (Mallotus villosus) samples collected from the northern Barents Sea in 2017 and 2021. PCAs-C10-13 concentrations were low, but detectable in all species, while PCAs-C14-17 concentrations were mainly below detection limits in the mammals. PCAs did not biomagnify, as the lowest concentrations were found in polar bear (0.7 ng g-1 lw) and the highest in capelin (56.9 ng g-1 lw). The PCA homologue profiles were similar among Arctic species, with PCAs-C10-13 dominating in polar cod and marine mammals, which may suggest a contribution from long-range atmospheric transport.In contrast, PCAs-C14-17 were most abundant in the Subarctic capelin, likely reflecting a different exposure. Despite differing PCAs-C14-17 concentrations among the two fish species, their PCAs-C14-17 homologue profile was similar, indicating uniform global production trends. Subarctic capelin is increasingly being preyed upon by Arctic predators and may facilitate the biological transport of PCAs-C14-17 into Arctic ecosystems.These findings suggest that climate-driven shifts in species distribution may have the potential to alter contaminant exposure pathways in Arctic marine food webs.
Our understanding of the environmental behavior, bioaccumulation and concentrations of chlorinated paraffins (CPs) and Dechloranes (Dec) in the Arctic environment is still limited, particularly in freshwater ecosystems. In this descriptive study, short chain (SCCPs) and medium chain (MCCPs) CPs, Dechlorane Plus (DP) and analogues, and polychlorinated biphenyls (PCBs) were measured in sediments, benthic organisms, three-spined stickleback (Gasterosteus aculeatus), Arctic char (Salvelinus alpinus) and brown trout (Salmo trutta) in two Sub-Arctic lakes in Northern Norway. Takvannet (TA) is a remote lake, with no known local sources for organic contaminants, while Storvannet (ST) is situated in a populated area. SCCPs and MCCPs were detected in all sediment samples from ST with concentration of 42.26–115.29 ng/g dw and 66.18–136.69 ng/g dw for SCCPs and MCCPs, respectively. Only SCCPs were detected in TA sediments (0.4–5.28 ng/g dw). In biota samples, sticklebacks and benthic organisms showed the highest concentrations of CPs, while concentrations were low or below detection limits in both char and trout. The congener group patterns observed in both lakes showed SCCP profiles dominated by higher chlorinated congener groups while the MCCPs showed consistency in their profiles, with C14 being the most prevalent carbon chain length. Anti- and syn-DP isomers were detected in all sediment, benthic and stickleback samples with higher concentrations in ST than in TA. However, they were only present in a few char and trout samples from ST. Dec 601 and 604 were below detection limits in all samples in both lakes. Dec 603 was detected only in ST sediments, sticklebacks and 2 trout samples, while Dec 602 was the only DP analogue found in all samples from both lakes. While there were clear differences in sediment concentrations of DP and Dec 602 between ST and TA, differences between lakes decreased with increasing δ15N. This pattern was similar to the PCB behavior, suggesting the lake characteristics in ST are playing an important role in the lack of biomagnification of pollutants in this lake. Our results suggest that ST receives pollutants from local sources in addition to atmospheric transport.
Cyclic volatile methylsiloxanes (cVMS) and short-chain chlorinated paraffins (SCCPs) use has been restricted in recent years due to environmental health concerns. Both of these classes of emerging contaminants possess long range transport potential (LRTP), highlighting the need for continuous monitoring to assess effectiveness of implemented regulations. However, emission source elucidation and understanding processes affecting atmospheric transport remain challenging. Atmospheric levels of cVMSs and SCCPs were simultaneously monitored at a background monitoring site in Norway from January–July 2020. Concentrations obtained from active air samplers ranged from 49.9 to 845 (mean: 208) pg/m3 for ƩSCCPs and from 0.4 to 3.5 (mean: 1.5), 1.1–15 (mean: 5.6) and 0.1–0.9 (mean: 0.4) ng/m3 for octamethylcyclotetrasiloxane (D4), decamethylcyclopentasiloxane (D5) and dodecamethylcyclohexasiloxane (D6), respectively. As SCCPs pose several challenges to analysts, different quantification methodologies and blank handling procedures were investigated to ensure reliable environmental measurements. Simulations using a Lagrangian atmospheric transport model (FLEXPART) revealed air masses impacting sampling measurements were of Oceanic origin, but periodic emission events from Europe and Russia were also observed. Seasonal pattern in cVMS concentrations was mainly driven by atmospheric degradation via hydroxyl radical reaction, whereas SCCP concentrations were more influenced by periodic anthropogenic inputs from local and continental Europe. No clear correlation could be observed with SCCP atmospheric concentrations and temperature over the entire sampling campaign. However, increased volatilization at elevated temperatures may be important with emissions originating from local sources. Higher chlorinated homologue groups dominated during the winter season and declined towards spring and summer, whereas reverse was found for the lower and more volatile chlorinated homologue groups.
Field data from two latitudinal transects in Europe and Canada were gathered to better characterize the atmospheric fate of three cyclic methylsiloxanes (cVMSs), i.e., octamethyl-cyclotetrasiloxane (D4), decamethylcyclopentasiloxane (D5) and dodecamethylcyclohexasiloxane (D6). During a year-long, seasonally resolved outdoor air sampling campaign, passive samplers with an ultra-clean sorbent were deployed at 15 sampling sites covering latitudes ranging from the source regions (43.7-50.7 °N) to the Arctic (79-82.5 °N). For each site, one of two passive samplers and one of two field blanks were separately extracted and analyzed for the cVMSs at two different laboratories using gas-chromatography-mass spectrometry. Whereas the use of a particular batch of sorbent and the applied cleaning procedure to a large extent controlled the levels of cVMS in field blanks, and therefore also the method detection and quantification limits, minor site-specific differences in field blank contamination were apparent. Excellent agreement between duplicates was obtained, with 95% of the concentrations reported by the two laboratories falling within a factor of 1.6 of each other. Nearly all data show a monotonic relationship between the concentration and distance from the major source regions. Concentrations in source regions were comparatively constant throughout the year, while the concentration gradient towards remote regions became steeper during summer when removal via OH radicals is at its maximum. Concentrations of the different cVMS oligomers were highly correlated within a given transect. Changes in relative abundance of cVMS oligomers along the transect were in agreement with relative atmospheric degradation rates via OH radicals.
Herring gulls (Larus argentatus) are opportunistic feeders, resulting in contaminant exposure depending on area and habitat. We compared contaminant concentrations and dietary markers between two herring gull breeding colonies with different distances to extensive human activity and presumed contaminant exposure from the local marine diet. Furthermore, we investigated the integrity of DNA in white blood cells and sensitivity to oxidative stress. We analyzed blood from 15 herring gulls from each colony—the urban Oslofjord near the Norwegian capital Oslo in the temperate region and the remote Hornøya island in northern Norway, on the Barents Sea coast. Based on d13C and d34S, the dietary sources of urban gulls differed, with some individuals having a marine and others a more terrestrial dietary signal. All remote gulls had a marine dietary signal and higher relative trophic level than the urban marine feeding gulls. Concentrations (mean ± standard deviation [SD]) of most persistent organic pollutants, such as polychlorinated biphenyl ethers (PCBs) and perfluorooctane sulfonic acid (PFOS), were higher in urban marine (PCB153 17 ± 17 ng/g wet weight, PFOS 25 ± 21 ng/g wet wt) than urban terrestrial feeders (PCB153 3.7 ± 2.4 ng/g wet wt, PFOS 6.7 ± 10 ng/g wet wt). Despite feeding at a higher trophic level (d15N), the remote gulls (PCB153 17 ± 1221 ng/g wet wt, PFOS 19 ± 1421 ng/g wet wt) were similar to the urban marine feeders. Cyclic volatile methyl siloxanes were detected in only a few gulls, except for decamethylcyclopentasiloxane in the urban colony, which was found in 12 of 13 gulls. Only hexachlorobenzene was present in higher concentrations in the remote (2.6 ± 0.42 ng/g wet wt) compared with the urban colony (0.34 ± 0.33 ng/g wet wt). Baseline and induced DNA damage (doublestreak breaks) was higher in urban than in remote gulls for both terrestrial and marine feeders. Environ Toxicol Chem 2022;41:2466–2478. © 2022 The Authors. Environmental Toxicology and Chemistry published by Wiley Periodicals LLC on behalf of SETAC.
Climate change-driven increases in air and sea temperatures are rapidly thawing the Arctic cryosphere with potential for remobilization and accumulation of legacy persistent organic pollutants (POPs) in adjacent coastal food webs. Here, we present concentrations of selected POPs in zooplankton (spatially and seasonally), as well as zoobenthos and sculpin (spatially) from Isfjorden, Svalbard. Herbivorous zooplankton contaminant concentrations were highest in May [e.g., ∑polychlorinated biphenyls (8PCB); 4.43, 95% CI: 2.72–6.3 ng/g lipid weight], coinciding with the final stages of the spring phytoplankton bloom, and lowest in August (∑8PCB; 1.6, 95% CI: 1.29–1.92 ng/g lipid weight) when zooplankton lipid content was highest, and the fjord was heavily impacted by sediment-laden terrestrial inputs. Slightly increasing concentrations of α-hexachlorocyclohexane (α-HCH) in zooplankton from June (1.18, 95% CI: 1.06–1.29 ng/g lipid weight) to August (1.57, 95% CI: 1.44–1.71 ng/g lipid weight), alongside a higher percentage of α-HCH enantiomeric fractions closer to racemic ranges, indicate that glacial meltwater is a secondary source of α-HCH to fjord zooplankton in late summer. Except for α-HCH, terrestrial inputs were generally associated with reduced POP concentrations in zooplankton, suggesting that increased glacial melt is not likely to significantly increase exposure of legacy POPs in coastal fauna.
An optimized low volume sampler was developed to determine both gas- and particle bound concentrations of short and medium-chain chlorinated paraffins (S/MCCPs). Background contamination was limited by the sampler design, providing method quantification limits (MQLs) at least two orders of magnitude lower than other studies within the gas (MQL: 500 pg (ΣSCCPs), 1.86 ng (ΣMCCPs)) and particle (MQL: 500 pg (ΣSCCPs), 1.72 ng (ΣMCCPs) phases. Good repeatability was observed between parallel indoor measurements (RSD ≤ 9.3% (gas), RSD ≤ 14% (particle)) with no breakthrough/saturation observed after a week of continuous sampling. For indoor air sampling, SCCPs were dominant within the gas phase (17 ± 4.9 ng/m3) compared to MCCPs (2.7 ± 0.8 ng/m3) while the opposite was observed in the particle bound fraction (0.28 ± 0.11 ng/m3 (ΣSCCPs) vs. 2.7 ± 1.0 ng/m3 (ΣMCCPs)). Only SCCPs in the gas phase could be detected reliably during outdoor sampling and were considerably lower compared to indoor concentrations (0.27 ± 0.10 ng/m3). Separation of the gas and particle bound phase was found to be crucial in applying the appropriate response factors for quantification based on the deconvoluted S/MCCP sample profile, thus avoiding over- (gas phase) or underestimation (particle phase) of reported concentrations. Very short chain chlorinated paraffins (vSCCPs, C5-C9) were also detected at equal or higher abundance compared to SCCP congener groups (C10-C13) congener groups, indicating an additional human indoor inhalation risk.
Understanding the drivers and effects of exposure to contaminants such as mercury (Hg) and organochlorine compounds (OCs) in Antarctic wildlife is still limited. Yet, Hg and OCs have known physiological and fitness effects in animals, with consequences on their populations. Here we measured total Hg (a proxy of methyl-Hg) in blood cells and feathers, and 12 OCs (seven polychlorinated biphenyls, PCBs, and five organochlorine pesticides, OCPs) in plasma of 30 breeding female Antarctic petrels Thalassoica antarctica from one of the largest colonies in Antarctica (Svarthamaren, Dronning Maud Land). This colony is declining and there is poor documentation on the potential role played by contaminants on individual physiology and fitness. Carbon (delta C-13) and nitrogen (delta N-15) stable isotope values measured in the females' blood cells and feathers served as proxies of their feeding ecology during the pre-laying (austral spring) and moulting (winter) periods, respectively. We document feather Hg concentrations (mean +/- SD, 2.41 +/- 0.83 mu g g(-1) dry weight, dw) for the first time in this species. Blood cell Hg concentrations (1.38 +/- 0.43 mu g g(-1) dw) were almost twice as high as those reported in a recent study, and increased with pre-laying trophic position (blood cell delta N-15). Moulting trophic ecology did not predict blood Hg concentrations. PCB concentrations were very low (Sigma(7)PCBs, 0.35 +/- 0.31 ng g(-1) wet weight, ww). Among OCPs, HCB (1.02 +/- 0.36 ng g(-1) ww) and p, p'-DDE (1.02 +/- 1.49 ng g(-1) ww) residues were comparable to those of ecologically-similar polar seabirds, while Mirex residues (0.72 +/- 0.35 ng g(-1) ww) were higher. PCB and OCP concentrations showed no clear relationship with pre-laying or moulting feeding ecology, indicating that other factors overcome dietary drivers. OC residues were inversely related to body condition, suggesting stronger release of OCs into the circulation of egg-laying females upon depletion of their lipid reserves. Egg volume, hatching success, chick body condition and survival were not related to maternal Hg or OC concentrations. Legacy contaminant exposure does not seem to represent a threat for the breeding fraction of this population over the short term. Yet, exposure to contaminants, especially Mirex, and other concurring environmental stressors should be monitored over the long-term in this declining population.
Active sampling methodology for atmospheric monitoring of cyclic volatile methylsiloxanes (cVMS) was improved to reduce sampling artifacts. A new sorbent, ABN Express (ABN), was evaluated for storage stability and measurement accuracy. Storage stability of cVMS on ABN showed less than 1% degradation of the individual C-13-labelled octamethylcyclotetrasiloxane (C-13(4)-D4), decamethylcyclopentasiloxane (C-13(5)-D5) and dodecamethylcyclohexasiloxane (C-13(6)-D6) after 14 days storage at room temperature and at -20 degrees C whereas significant degradation was observed on ENV+ sorbent at room temperature (37-62 %) and -20 degrees C (9-16 %). C-13(4)-D4 formed on ENV+ spiked with C-13(5)-D5, and both C-13(4)-D4 and C-13(5)-D5 formed on ENV+ spiked with C-13(6)-D6. However, this was not observed on the ABN sorbent. Performance of ABN was compared to ENV+ through an 8-month Arctic sampling campaign at the Zeppelin Observatory (Ny Alesund, Svalbard). Good agreement between ABN and ENV+ was observed for D4 in the spring/summer months. However, D5 and D6 was found to be consistently higher on the ABN sorbent during this time period with D6 showing the greatest deviation. During the winter months, larger deviations were observed between ABN and ENV+ sorbents with a factor of 4 times higher atmospheric concentrations of both D5 and D6 found on ABN; indicating sorbent related degradation on ENV+. Our findings show that the ABN sorbent provides greater stability and accuracy for atmospheric monitoring of cVMS. Implications of these improvements towards atmospheric fate processes will be discussed. (C) 2020 The Authors. Published by Elsevier Ltd.
Volatile methylsiloxanes (VMS) have been identified as contaminants of emerging concern in aquatic systems. Here, we report on the presence of VMS in sediment and wastewater from Arctic regions in 2014 to 2016 and model their persistence in Adventfjorden in Longyearbyen, Svalbard. Total concentrations of VMS in sediment were dominated by D4 and D5 and ranged from 0.0024 to 1.7 ng g-1 at Svalbard (Longyearbyen), from 4.0 to 43 ng g-1 in Greenland (Nuuk) and from 0.19 to 21 ng g-1 in the Canadian Archipelago. Concentrations in wastewater samples from Svalbard ranged from 12 to 156 ng L-1. Large variability in reported values of the partition ratio between organic carbon and water (KOC) and enthalpy of sorption (ΔHOC; often estimated from enthalpy of phase change between octanol and water, ΔHOW) of VMS has resulted in high uncertainty in evaluating persistence in aquatic systems. We evaluated previously reported KOC and ΔHOC values from the literature in predicting measured VMS concentrations in sediment and wastewater in scenarios using a fugacity-based multimedia model for VMS concentrations in Svalbard. We tested two different model scenarios: (1) KOC and ΔHOW measurements for three cyclic VMS previously reported by Kozerski et al. (Environ. Toxicol. Chem., 2014, 33, 1937-1945) and Xu and Kropscott (Environ. Chem., 2014, 33, 2702-2710) and (2) the KOC and ΔHOC measurements from Panagopoulos et al. (Environ. Sci. Technol., 2015, 49, 12161-12168 and Environ. Sci. Technol. Lett., 2017, 4(6), 240-245). Concentrations of VMS in sediment predicted from concentrations in wastewater in scenario 2 were in good agreement with measured concentrations, whereas in scenario 1, predicted concentrations were 2 to 4 orders of magnitude lower. Such large discrepancies indicate that the differences in the predicted concentrations are more likely to be attributed to KOC and ΔHOC than to uncertainty in environmental parameters or emission rates.
While migratory seabirds dominate ecotoxicological studies within the Arctic, there is limited knowledge about exposure and potential effects from circulating legacy and emerging contaminants in species who reside in the high-Arctic all year round. Here, we focus on the case of the Mandt's Black guillemot (Cepphus grylle mandtii) breeding at Kongsfjorden, Svalbard (79.00°N, 11.66°E) and investigate exposure to legacy and emerging contaminants in relation to individual physiological status, i.e. body condition, oxidative stress and relative telomere length. Despite its benthic-inshore foraging strategy, the Black guillemot displayed overall similar contaminant concentrations in blood during incubation (∑PCB11 (15.7 ng/g w.w.) > ∑PFAS5 (9.9 ng/g w.w.) > ∑Pesticides9 (6.7 ng/g w.w.) > ∑PBDE4 (2.7 ng/g w.w.), and Hg (0.3 μg/g d.w.) compared to an Arctic migratory seabird in which several contaminant-related stress responses have been observed. Black guillemots in poorer condition tended to display higher levels of contaminants, higher levels of reactive oxygen metabolites, lower plasmatic antioxidant capacity, and shorter telomere lengths; however the low sample size restrict any strong conclusions. Nevertheless, our data suggests that nonlinear relationships with a threshold may exist between accumulated contaminant concentrations and physiological status of the birds. These findings were used to build a hypothesis to be applied in future modelling for describing how chronic exposure to contaminants may be linked to telomere dynamics.
Eggs of snow buntings (Plectrophenax nivealis) were applied as a bio-indicator to examine differences in exposure to legacy persistent organic pollutants (POPs) and perflouroalkyl subtances (PFAS) from the terrestrial environment surrounding the settlements of Longyearbyen, Barentsburg and Pyramiden on Svalbard, Norway. Significantly higher concentrations of summed polychlorinated biphenyls (sumPCB7) in eggs collected from Barentsburg (2980 ng/g lipid weight (1w)) and Pyramiden (3860 ng/g lw) compared to Longyearbyen (96 ng/g 1w) are attributed to local sources of PCBs within these settlements. Similar findings were observed for p,p'-didilorodiphenyldichloroethylene (p,p'-DDE) where higher median concentrations observed in Pyramiden (173 ng/g lw) and Barentsburg (75 ng/g lw) compared to Longyearbyen (48 ng/g 1w) may be influenced by guano inputs from breeding seabird populations. although other point sources cannot be ruled out Concentrations of perfluorooctane sulphonate (PROS) and several perfluorinated carboxylic acids (PFCAs) in snow bunting eggs were found to be statistically higher in the populated settlements of Longyearbyen and Barentsburg compared to the abandoned Pyramiden. Narrow foraging ranges of snow buntings during breeding season was useful in assessing point sources of exposure for PCBs and PFAS at particular sites with extreme differences observed between nest locations. SumPCB7 concentrations ranged fMrn 2 mu g/g ww to below detection limits between nest sites located less than a kilometer from each other in Pyramiden. Similar findings were observed in Longyearbyen, where several PFCAs ranged from 2 to 55 times higher between nest sites with similar spatial distances. These findings indicate that snow buntings can be a useful bio-indicator offering high spatial resolution for contaminant source apportionment in terrestrial environments on Svalbard. (C) 2019 Elsevier B.V. All rights reserved.
This chapter reviews volatile methyl siloxanes (VMS) in polar regions (i.e., at latitudes above the polar circles), including their sources, measured concentrations, and the effect of polar environmental conditions on behavior of VMS. Knowledge about VMS in polar regions has been centered on cyclic VMS (cVMS) due to their widespread use and presence in the environment. Due to their high volatility, cVMS are mainly emitted to and remain in the atmosphere, where they eventually degrade. cVMS are present in Arctic air due to both long-range atmospheric transport and local sources within the Arctic. There is no evidence that cVMS deposit to surface media to a significant extent, not even under polar environmental conditions. However, cVMS are emitted via wastewater, and many Arctic communities have limited wastewater treatment where low removal efficiency of cVMS from wastewater can result in high emissions. cVMS concentrations in sediments and aquatic biota close to wastewater outlets in the Norwegian Arctic are comparable to those at temperate latitudes. Sporadic detections of cVMS in biota and surface media in remote Arctic and Antarctic regions need further investigation to be confirmed. Very few measurements are reported for linear VMS (lVMS) in polar regions, with a majority of studies reporting findings below detection limits. The understanding of how Arctic conditions, including low temperatures and strong seasonality, affect the environmental behavior and bioaccumulation of VMS has been expanded through modelling studies. However, important knowledge gaps remain regarding temperature dependence of partitioning behavior in aquatic environments, biotransformation rates in polar biota, and the influence of physiological and behavioral adaptations of polar biota on bioaccumulation of VMS.
Arctic-breeding geese acquire resources for egg production from overwintering grounds, spring stopover sites and breeding grounds, where pollutant exposure may differ. We investigated the effect of migration strategy on pollutant occurrence of lipophilic polychlorinated biphenyls (PCBs) and protein-associated poly- and perfluoroalkyl substances (PFASs) and mercury (Hg) in eggs of herbivorous barnacle geese ( Branta leucopsis) from an island colony on Svalbard. Stable isotopes (δ13C and δ15N) in eggs and vegetation collected along the migration route were similar. Pollutant concentrations in eggs were low, reflecting their terrestrial diet (∑PCB = 1.23 ± 0.80 ng/g ww; ∑PFAS = 1.21 ± 2.97 ng/g ww; Hg = 20.17 ± 7.52 ng/g dw). PCB concentrations in eggs increased with later hatch date, independent of lipid content which also increased over time. Some females may remobilize and transfer more PCBs to their eggs, by delaying migration several weeks, relying on more polluted and stored resources, or being in poor body condition when arriving at the breeding grounds. PFAS and Hg occurrence in eggs did not change throughout the breeding season, suggesting migration has a greater effect on lipophilic pollutants. Pollutant exposure during offspring production in arctic-breeding migrants may result in different profiles, with effects becoming more apparent with increasing trophic levels.
This study investigates persistence (P) and long-range transport potential (LRTP) of cyclic volatile methylsiloxanes (cVMS) based on the field measurements in the Northern Hemisphere. The field data consisted of published outdoor air concentrations of octamethylcyclotetrasiloxane (D4), decamethylcyclopentasiloxane (D5) and dodecamethylcyclohexasiloxane (D6) at urban, suburban, rural and remote locations excluding the point sources. Three major trends were observed. First, D4 and D6 concentrations were correlated with measured concentrations for D5 at the same times and locations in the majority of the datasets, reflecting the common sources and similar removal mechanism(s) for these compounds. Second, as the sampling sites changed from the source to remote locations along a south-to-north transect, average cVMS concentrations in air decreased in an exponential manner. The empirical characteristic travel distances (eCTD) extracted from these spatial patterns were smaller than model estimated values and differed in order among individual compounds (D4 ∼ D5 < D6). Finally, D5/D6 concentration ratios were also found to decrease exponentially along the same spatial gradient, contrary to model predictions of an increase based on current knowledge of mechanisms controlling atmospheric cVMS degradation. These findings suggest that there may be additional removal process(es) for airborne cVMS, currently not accounted for, that requires further elucidation.
Cyclic volatile methylsiloxanes (cVMS) are used in personal care products and emitted to aquatic environments through wastewater effluents, and their bioaccumulation potential is debated. Here, a new bentho-pelagic version of the ACC-HUMAN model was evaluated for polychlorinated biphenyls (PCBs) and applied to cVMS in combination with measurements to explore their bioaccumulation behavior in a subarctic lake. Predictions agreed better with measured PCB concentrations in Arctic char (Salvelinus alpinus) and brown trout (Salmo trutta) when the benthic link was included than in the pelagic-only model. Measured concentrations of decamethylcyclopentasiloxane (D5) were 60 ± 1.2 (Chironomidae larvae), 107 ± 4.5 (pea clams Pisidium sp.), 131 ± 105 (three-spined sticklebacks: Gasterosteus aculeatus), 41 ± 38 (char), and 9.9 ± 5.9 (trout) ng g-1 wet weight. Concentrations were lower for octamethylcyclotetrasiloxane (D4) and dodecamethylcyclohexasiloxane (D6), and none of the cVMS displayed trophic magnification. Predicted cVMS concentrations were lower than measured in benthos, but agreed well with measurements in fish. cVMS removal through ventilation was an important predicted loss mechanism for the benthic-feeding fish. Predictions were highly sensitive to the partition coefficient between organic carbon and water (KOC) and its temperature dependence, as this controlled bioavailability for benthos (the main source of cVMS for fish).