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Time series of contaminants in the Arctic are an important instrument to detect emerging issues and to monitor the effectiveness of chemicals regulation, based on the assumption of a direct reflection of changes in primary emissions. Climate change has the potential to influence these time trends, through direct physical and chemical processes and/or changes in ecosystems. This study was part of an assessment of the Arctic Monitoring and Assessment Programme (AMAP), analysing potential links between changes in climate-related physical and biological variables and time trends of persistent organic pollutants (POPs) in Arctic biota, with some additional information from the Antarctic. Several correlative relationships were identified between POP temporal trends in freshwater and marine biota and physical climate parameters such as oscillation indices, sea-ice coverage, temperature and precipitation, although the mechanisms behind these observations remain poorly understood. Biological data indicate changes in the diet and trophic level of some species, especially seabirds and polar bears, with consequences for their POP exposure. Studies from the Antarctic highlight increased POP availability after iceberg calving. Including physical and/or biological parameters in the POP time trend analysis has led to small deviations in some declining trends, but did generally not change the overall direction of the trend. In addition, regional and temporary perturbations occurred. Effects on POP time trends appear to have been more pronounced in recent years and to show time lags, suggesting that climate-related effects on the long time series might be gaining importance.

Climate change may affect temporal trends of persistent organic pollutants (POPs) in Arctic wildlife. We studied how biological and climate variables influence temporal trends of selected POP groups in landlocked Arctic char muscle and in ringed seal blubber from West and East Greenland. The variables included fish length or animal age, sex, a stable nitrogen isotope, sea ice extent, air or seawater temperature, salinity and the Arctic Oscillation Index (AOI). Model selection for multiple regression showed that the most important predictors varied among POP groups, species and region. Decreasing time trends were found for all POP groups with the exception of hexachlorobenzene (HCB) concentration which remained stable in Arctic char and ringed seals from West Greenland. When retained in the most parsimonious model, the AOI was positively associated with POP concentrations for East Greenland seals, but negatively for West Greenland seals. Seawater temperature and sea ice extent were positively associated with POP concentrations. The effects of explanatory variables on the annual rates of change in POP concentrations were relatively minor relative to the decline caused by reduction in POP emissions following national and international regulations introduced since the 1970s.

The polar bear (Ursus maritimus) is among the Arctic species exposed to the highest concentrations of long-range transported bioaccumulative contaminants, such as halogenated organic compounds and mercury. Contaminant exposure is considered to be one of the largest threats to polar bears after the loss of their Arctic sea ice habitat due to climate change. The aim of this review is to provide a comprehensive summary of current exposure, fate, and potential health effects of contaminants in polar bears from the circumpolar Arctic required by the Circumpolar Action Plan for polar bear conservation. Overall results suggest that legacy persistent organic pollutants (POPs) including polychlorinated biphenyls, chlordanes and perfluorooctane sulfonic acid (PFOS), followed by other perfluoroalkyl compounds (e.g. carboxylic acids, PFCAs) and brominated flame retardants, are still the main compounds in polar bears. Concentrations of several legacy POPs that have been banned for decades in most parts of the world have generally declined in polar bears. Current spatial trends of contaminants vary widely between compounds and recent studies suggest increased concentrations of both POPs and PFCAs in certain subpopulations. Correlative field studies, supported by in vitro studies, suggest that contaminant exposure disrupts circulating levels of thyroid hormones and lipid metabolism, and alters neurochemistry in polar bears. Additionally, field and in vitro studies and risk assessments indicate the potential for adverse impacts to polar bear immune functions from exposure to certain contaminants., (Copyright © 2019 Elsevier B.V. All rights reserved.)

A suite of perfluoroalkyl substances (PFASs) and polychlorinated naphthalenes (PCNs) were determined in 41 peregrine falcon eggs collected in South Greenland between 1986 and 2014. Median concentrations of perfluorinated sulfonic acids (ΣPFSA) and perfluorinated carboxylic acids (ΣPFCA) were 303 ng/g dry weight (dw) (58 ng/g wet weight, ww) and 100 ng/g dw (19 ng/g ww), respectively, which was comparable to other studies. Perfluorooctane sulfonate (PFOS) accounted for 94% on average of all PFSAs, but did not show a significant time trend. Perfluorohexane sulfonate (PFHxS), perfluoroheptane sulfonate (PFHpS) and perfluorodecane sulfonate (PFDS) showed non-linear decreases over the study period, while some long-chain PFCAs increased significantly. The PCN profile was dominated by the penta-, hexa- and tetrachlorinated congeners CN-52/60, CN-66/67 and CN-42. CN-54, an indicator of combustion, accounted for 2.4% of ΣPCN on average. All PCN congeners showed a decreasing tendency, which was significant for lipid-normalized concentrations of CN-53, CN-54 and CN-63. The ΣPCN median concentration was 21 ng/g lipid weight, which is in the high end of concentrations reported for bird eggs. The PCN and PFAS concentrations add to an already high contaminant burden and a complex chemical cocktail in the peregrine falcon population in Greenland, mainly reflecting contaminant exposure during migration and winter stays in Central and South America., (Copyright © 2018 Elsevier B.V. All rights reserved.)

Polar bears (Ursus maritimus) are among the world's highest trophic level marine predators and as such have some of the highest tissue concentrations of organohalogen contaminants (OHCs) among Arctic biota. In this paper we present the results of a three decade (1983-2013) risk assessment of OHC exposure and effects on reproduction, immunity, and cancer (genotoxicity) in polar bears from Central East Greenland. Risk of adverse effects are evaluated using a risk quotient (RQ) approach with derivation from measured OHC concentrations in polar bear tissue and critical body residues (CBR) extrapolated for polar bears using physiologically-based pharmacokinetic modelling (PBPK). The additive RQs for all OHCs in polar bears were above the threshold for all effect categories (RQ > 1) in every year, suggesting this population has been at significant and continuous risk of contaminant-mediated effects for over three decades. RQs peaked in 1983 (RQ > 58) and again in 2013 (RQ > 50) after a period of decline. These trends follow ΣPCB levels during that time, and contributed almost all of the risk to immune, reproductive, and carcinogenic effects (71-99% of total RQ). The recent spike in RQs suggests a major shift in polar bear contaminant exposure from climate related changes in food composition and hereby the increased risk of adverse health effects. In the context of lifetime exposure ΣPCB and PFOS levels showed the interactive importance of year of birth, age, and emission history. In conclusion, the results indicate that East Greenland polar bears have been exposed to OHC levels over the period of 1983-2013 that potentially and continuously affected individual and theoretically also population health, with a peaking risk in the more recent years., (Copyright © 2018 Elsevier Ltd. All rights reserved.)

Persistent organic pollutants (POPs) are long-range transported to the Arctic via atmospheric and oceanic currents, where they biomagnify to high concentrations in the tissues of apex predators such as polar bears (Ursus maritimus). A major concern of POP exposure is their physiological effects on vital organ-tissues posing a threat to the health and survival of polar bears. Here we examined the relationship between selected POPs and baculum bone mineral density (BMD) in the East Greenland and seven Canadian subpopulations of polar bears. BMD was examined in 471 bacula collected between years 1996-2015 while POP concentrations in adipose tissue were determined in 67-192 of these individuals collected from 1999 to -2015. A geographical comparison showed that baculum BMD was significantly lowest in polar bears from East Greenland (EG) when compared to Gulf of Boothia (GB), Southern Hudson (SH) and Western Hudson (WH) Bay subpopulations (all p < 0.05). The calculation of a T-score osteoporosis index for the EG subpopulation using WH bears as a reference group gave a T-score of -1.44 which indicate risk of osteopenia. Concentrations of ΣPCB 74 (polychlorinated biphenyls), ΣDDT 3 (dichlorodiphenyltrichloroethanes), p,p'-DDE (dichlorodiphenyldichloroethylene), ΣHCH 3 (hexachlorohexane) and α-HCH was significantly highest in EG bears while ΣPBDE (polybrominated diphenyl ethers), BDE-47 and BDE-153 was significantly highest in SH bears (all p < 0.04). Statistical analyses of individual baculum BMD vs. POP concentrations showed that BMD was positively correlated with ΣPCB 74 , CB-153, HCB (hexachlorobenzene), ΣHCH, β-HCH, ClBz (chlorobenzene), ΣPBDE and BDE-153 (all p < 0.03). In conclusion, baculum density was significantly lowest in East Greenland polar bears despite the positive statistical correlations of BMD vs. POPs. Other important factors such as nutritional status, body mass and body condition was not available for the statistical modelling. Since on-going environmental changes are known to affect these, future studies need to incorporate nutritional, endocrine and genetic parameters to further understand how POP exposure may disrupt bone homeostasis and affect baculum BMD across polar bear subpopulations., (Copyright © 2018 Elsevier Ltd. All rights reserved.)

We investigated skull size (condylobasal length; CBL) and bone mineral density (BMD) in polar bears (Ursus maritimus) from East Greenland (n = 307) and Svalbard (n = 173) sampled during the period 1892-2015 in East Greenland and 1964-2004 at Svalbard. Adult males from East Greenland showed a continuous decrease in BMD from 1892 to 2015 (linear regression: p < 0.01) indicating that adult male skulls collected in the early pre-pollution period had the highest BMD. A similar decrease in BMD over time was not found for the East Greenland adult females. However, there was a non-significant trend that the skull size of adult East Greenland females was negatively correlated with collection year 1892-2015 (linear regression: p = 0.06). No temporal change was found for BMD or skull size in Svalbard polar bears (ANOVA: all p > 0.05) nor was there any significant difference in BMD between Svalbard and East Greenland subpopulations. Skull size was larger in polar bears from Svalbard than from East Greenland (two-way ANOVA: p = 0.003). T-scores reflecting risk of osteoporosis showed that adult males from both East Greenland and Svalbard are at risk of developing osteopenia. Finally, when correcting for age and sex, BMD in East Greenland polar bears increased with increasing concentrations of persistent organic pollutants (POPs) i.e. ΣPCB (polychlorinated biphenyls), ΣHCH (hexachlorohexane), HCB (hexachlorobenzene) and ΣPBDE (polybrominated diphenyl ethers) while skull size increased with ΣHCH concentrations all in the period 1999-2014 (multiple linear regression: all p < 0.05, n = 175). The results suggest that environmental changes over time, including exposure to POPs, may affect bone density and size of polar bears., (Copyright © 2017 Elsevier Inc. All rights reserved.)

Median levels of regulated flame retardants, i.e., polybrominated diphenyl ethers (PBDEs), brominated biphenyl (BB)-153, and hexabromocyclododecane (HBCD), in 33-48 eggs of peregrine falcons (Falco peregrinus) from Greenland were 1909, 359, and 5.98 ng/g lipid weight (lw), respectively, and generally intermediate to levels in North America and Europe. Unregulated flame retardants had lower median concentrations of 1.06 (2-ethylhexyl-2,3,4,5-tetrabromobenzoate, EH-TBB), 2.42 (1,2-bis(2,4,6-tribromophenoxy)-ethane, BTBPE), 0.52 (2,4,6-tribromophenyl 2,3-dibromopropyl ether, DPTE), and 4.78 (dechlorane plus) ng/g lw. Although these compounds are often described as recent replacements for PBDEs, they were also present in eggs from the 1980s. BDE-209 was the only compound with a significant increase (+7.2% annual change) between 1986 and 2014, while BB-153 and DPTE decreased significantly (-8.0% and -2.8% annual change, respectively). Dechlorane plus showed a nonsignificant increase. Individual birds, equipped with light-logging geolocators, confirmed the contaminant exposure over a large geographical area as the birds spent nearly equal time periods in their breeding and wintering grounds in Greenland and Central/South America, respectively, interrupted by 5-6 weeks of migration through North America.

Besides globally banned "legacy" persistent organic pollutants, other compounds might be present in Arctic wildlife, for which regulation was introduced recently (the insecticide endosulfan), is considered (short-chain chlorinated paraffins, SCCPs) or does not exist (octachlorostyrene, OCS, a byproduct of manufacturing and combustion processes involving chlorine). The purpose of this study was to analyze the time trend of endosulfan (1986-2012) in ringed seals and to address the levels of SCCPs and OCS in wildlife species from Greenland (black guillemot, glaucous gull, ringed seal, polar bear), while taking a critical standpoint to analytical methods typically applied. The metabolite endosulfan sulfate was the only endosulfan compound consistently above detection limits, with a median concentration of 0.23 ng/g lipid weight (lw) and a significant annual decrease of -5.6%. The low-resolution mass spectrometry (LRMS) method appeared accurate and sufficiently precise; however, the gel permeation chromatography had to balance lipid removal and analyte loss. SCCPs and OCS were present in all samples. OCS median concentrations were between 2.8 (ringed seal blubber) and 29 (glaucous gull liver) ng/g lw, determined by a straightforward dual column electron capture detection method. SCCPs were analyzed by LRMS, following removal of potential interferences, and had median concentrations of several 100 ng/g wet weight. While the method showed good precision and recovery rates as well as acceptable accuracy in control samples, the Greenland samples had high concentrations in an Arctic context, possibly indicating limited selectivity of the LRMS method.

The risk from POP (persistent organic pollutant) exposure and subsequent reproductive, immunotoxic and liver histopathological effects was evaluated in a classical parallel trial on Greenland sledge dogs (Canis familiaris) fed contaminated minke whale (Balaenoptera acutorostrata) blubber. First the critical body residues (CBRs) were estimated using the physiologically-based pharmacokinetic (PBPK) model for seven POP compounds based on rat critical daily doses (CDDs). These were then compared with the actual daily oral POP doses (DD) and body residues (BR) in the sledge dogs by calculating risk quotients (RQDD: DD/CDD; RQBR: BR/CBR; ≥1 indicates risk). The results showed that risk quotients for reproductive, immunotoxic and liver histopathological effects were significantly lowest in the control group (p<0.01) while risk quotients based on daily doses (RQDD) were significantly lower than RQs based on body residues (RQBR) (all p<0.01). RQBR in the exposed group ranged from 1.0-12 for reproductive and immunotoxic effects while those for liver histopathological effects ranged from 0.7-3.0. PCBs (polychlorinated biphenyls) and chlordanes were the dominant driver behind high immune and reproductive RQs while dieldrin was the most important factor behind RQs for liver histopathology. Principal component analyses and Spearman rank correlation analyses showed that complement and cellular immune parameters were significantly negative correlated with RQBR (all p<0.05) while logistic regression showed that RQDD had a significant effect on the number of born cups (p=0.03). No significantly relations were found between RQs and hormone concentrations, number of gestations, antibody titres or liver histopathology. These results confirm previous studies showing that POP exposure negatively impacts steroid hormones, various immune parameters, as well as liver histopathology in sledge dogs. It is also clear that RQBR is the best reflector of health effects from POP exposure and that it is especially accurate in predicting immune and reproductive effects. We recommend that PBPK modelled (CBR) and RQBR should be used in the assessment of POP exposure and health effects in Arctic top predators., (Copyright © 2015 Elsevier Ltd. All rights reserved.)

Industrially produced chemicals have been a major environmental concern across our entire Globe since the onset of rapid industrial development around the early 1900. Many of the substances being used are known to be endocrine disrupting chemicals (EDCs) and are also known to be long-range dispersed and to biomagnify to very high concentrations in the tissues of Arctic apex predators such as polar bears (Ursus maritimus). A major concern relating to EDCs is their effects on vital organ-tissues such as bone and it is possible that EDCs represent a more serious challenge to the species' survival than the more conventionally proposed prey reductions linked to climate change. We therefore analyzed penile bone mineral density (BMD) as a key phenotype for reproductive success in 279 polar bear samples born 1990-2000 representing eight polar bear subpopulations. Since EDC concentrations were not available from the same specimens, we compared BMD with published literature information on EDC concentrations. Latitudinal and longitudinal BMD and EDC gradients were clearly observed, with Western Hudson bears having the highest BMD and lowest EDCs, and North East Greenland polar bears carrying the lowest BMD and highest EDCs. A BMD vs. polychlorinated biphenyls (PCB) regression analysis showed that BMD decreased as a function of the eight subpopulations' PCB concentrations and this relationship was close to being significant (p=0.10, R(2)=0.39). Risk quotient (RQ) estimation demonstrated that PCBs could be in a range that may lead to disruption of normal reproduction and development. It is therefore likely that EDCs directly affect development and bone density in polar bears. Canadian bears had in general the best health and the North East Greenland subpopulation being at the highest risk of having negative health effects. While reductions in BMD is in general unhealthy, reductions in penile BMD could lead to increased risk of species extinction because of mating and subsequent fertilization failure as a result of weak penile bones and risk of fractures. Based on this, future studies should assess how polar bear subpopulations respond upon EDC exposure since information and understanding about their circumpolar reproductive health is vital for future conservation., (Copyright © 2014 Elsevier Inc. All rights reserved.)

Systematic monitoring of persistent organic pollutants (POPs) in the Arctic has been conducted for several years, in combination with assessments of POP levels in the Arctic, POP exposure and biological effects. Meanwhile, environmental research continues to detect new contaminants some of which could be potential new Arctic pollutants. This study summarizes the empirical evidence that is currently available of those compounds in the Arctic that are not commonly included in chemical monitoring programmes. The study has focused on novel flame retardants, e.g. alternatives to the banned polybrominated diphenyl ethers (PBDEs), current-use pesticides and various other compounds, i.e. synthetic musk compounds, siloxanes, phthalic acid esters and halogenated compounds like hexachlorobutadiene, octachlorostyrene, pentachlorobenzene and polychlorinated naphthalenes. For a number of novel brominated flame retardants, e.g. 2,3-bibromopropyl-2,4,6-tribromophenyl ether (DPTE), bis(2-ethylhexyl)tetrabromophthalate (TBPH), 2-ethylhexyl-2,3,4,5-tetrabromobenzoate (TBB), 1,2-bis(2,4,6-tribromophenoxy)-ethane (BTBPE), decabromodiphenyl ethane (DBDPE), pentabromoethylbenzene (PBEB) and hexabromobenzene (HBBz), transport to the Arctic has been documented, but evidence of bioaccumulation is sparse and ambiguous. For short-chain chlorinated paraffins and dechlorane plus, however, increasing evidence shows both long-range transport and bioaccumulation. Ice cores have documented increasing concentrations of some current-use pesticides, e.g. chlorpyrifos, endosulfan and trifluralin, and bioaccumulation has been observed for pentachloroanisole, chorpyrifos, endosulfan and metoxychlor, however, the question of biomagnification remains unanswered., (Copyright © 2014 Elsevier Ltd. All rights reserved.)

This paper studied the levels and organ distribution of the toxic heavy metal cadmium in scallops from unpolluted Greenlandic waters. The scallops had an average cadmium concentration of 2.93 ± 0.94 μg/g wet weight in the total soft tissues and no concentration dependent effect was found for gender or size (both p>0.05). The kidney was the primary organ for cadmium accumulation with a mean of 226.2 ± 111.7 μg/g wet weight, and despite the small weight of the kidney, it appeared as the principal contributor of cadmium with 92% of the total cadmium body burden. The cadmium concentrations in the total soft tissues far exceeded the EU-limit of 1 μg/g wet weight for cadmium in bivalves. Based on this, selective evisceration of the cadmium-rich kidney and digestive gland during processing can be regarded as a reliable measure to be taken in order to reduce the cadmium content of scallops used for human consumption., (Copyright © 2014 Elsevier Ltd. All rights reserved.)

The former Black Angel lead-zinc mine in Maarmorilik, West Greenland, is a historic example of how mining activity may result in a significant impact on the surrounding fjord system in terms of elevated concentrations of especially lead (Pb) and zinc (Zn) in seawater, sediments and surrounding biota. In order to shed light on the present contamination and possible effects in the fjord we initiated a range of studies including a pilot study on gill and liver morphology of common sculpins (Myoxocephalus scorpius) around Maarmorilik. Sculpins were caught and sampled at five different stations known to represent a gradient of Pb concentrations. Fish livers from all specimens were analyzed for relevant elements in the area: Fe, Zn, As, Cu, Se, Cd, Pb, Ag, Hg, Co and Ni. Lead, As and Hg showed significant differences among the five stations. For 20% of the sculpins, Hg concentrations were in the range of lowest observed effect dose (LOED) of 0.1-0.5 μg/g ww for toxic threshold on reproduction and subclinical endpoints. Likewise LOEDs for tissue lesions, LOEDs for biochemistry, growth, survival and reproduction were exceeded for Cd (0.42-1.8 μg/g ww) and for As (11.6 μg/g ww) in 28% and 85% of the sculpins, respectively. Similar to this, the no observed effect dose (NOED) for biochemistry was exceeded for Pb (0.32 μg/g ww) and for growth, mortality and reproduction for Zn (60-68 μg/g ww) in 33% and 24% of the sculpins, respectively. For all sculpins, females were significantly larger than males and for five of the elements (Fe, Co, Ni, Cu, Se) females had higher concentrations. The chronic lesions observed in liver (mononuclear cell infiltrates, necrosis, vacuolar hepatocytes, portal fibrosis, bile duct hyperplasia, active melanomacrophage centers) and gills (fusion and edema of secondary lamellae, laminar telangiectasis, mononuclear cell infiltrates, blebs) were similar to those in the literature studies for both wild and laboratory exposed sculpins and other fish species carrying similar or higher Hg concentrations. Ignoring sex and size, specimens with hepatic cell infiltrates had the highest concentrations of most elements, a relation that was also found for gill telangiectasis and Hg (all p < 0.05). When controlling for sex and size, the prevalence of vacuolar hepatocytes and endoparasites was significantly highest at the three most contaminated stations and similar differences were found for liver necrosis. We suggest that beside exposure to mining-related elements, other environmental factors, such as parasites, might be co-factors in the development of the observed liver and gill lesions. Therefore, sculpin liver and gill pathology are likely to be suitable health indicators when biomonitoring gradients of mining and other element related activity effects; while a larger study is required to fully evaluate the relationships., (Copyright © 2014 Elsevier Inc. All rights reserved.)

Human exposure to persistent organic pollutants (POPs) and the potential health impact in the Arctic far from the emission sources have been highlighted in numerous studies. As a supplement to human POP biomonitoring studies, a physiologically based pharmacokinetic (PBPK) model was set up to estimate the fate of POPs in Greenlandic Inuit's liver, blood, muscle and adipose tissue following long-term exposure to traditional Greenlandic diet. The PBPK model described metabolism, excretion and POP accumulation on the basis of their physicochemical properties and metabolic rates in the organisms. Basic correlations between chemically analyzed blood POP concentrations and calculated daily POP intake from food questionnaire of 118 middle age (18-35years) Greenlandic Inuits from four cities in West Greenland (Qaanaaq: n=40; Qeqertarsuaq: n=36; Nuuk: n=20; Narsaq: n=22) taken during 2003 to 2006 were analyzed. The dietary items included were polar bear, caribou, musk oxen, several marine species such as whales, seals, bird and fish as well as imported food. The contaminant concentrations of the dietary items as well as their chemical properties, uptake, biotransformation and excretion allowed us to estimate the POP concentration in liver, blood, muscle and adipose tissue following long-term exposure to the traditional Greenlandic diet using the PBPK model. Significant correlations were found between chemically analyzed POP blood concentrations and calculated daily intake of POPs for Qeqertarsuaq, Nuuk and Narsaq Inuit but not for the northernmost settlement Qaanaaq, probably because the highest blood POP level was found in this district which might mask the interview-based POP calculations. Despite the large variation in circulating blood POP concentrations, the PBPK model predicted blood concentrations of a factor 2-3 within the actual measured values. Moreover, the PBPK model showed that estimated blood POP concentration increased significantly after consumption of meals. For individuals who had a high internal burden of POPs accumulated over years, the estimated blood levels were less influenced by recent meal intake. The model results also indicated that of the POPs accumulated in the body the concentrations were highest for CB-153 (oxychlordane: 0.6%; DDE and CB-99: 2.9%; HCB: 4.4%; CB-153: 34.5%). Furthermore, the model also estimated a significant internal body POP burden even several years after the mentioned dietetic shift and that contaminant accumulation was 2-6 folds faster than the decay after a shift to a diet low in contaminants. Using the PBPK model approach, we seek to improve the knowledge on contaminant body burden in humans of the Arctic. However, it should be noted that calculations of daily POP intake may be subject to considerable uncertainty due to imprecise information from the dietary interview. Based on these results we suggest that PBPK modeling is implemented as a tool in future human health exposure and effect assessments in Greenland., (Copyright © 2013 Elsevier Ltd. All rights reserved.)

Time-series of perfluorinated alkylated substances (PFASs) in East Greenland polar bears and East and West Greenland ringed seals were updated in order to deduce whether a response to the major reduction in perfluoroalkyl production in the early 2000s had occurred. Previous studies had documented an exponential increase of perfluorooctane sulphonate (PFOS) in liver tissue from both species. In the present study, PFOS was still the far most dominant compound constituting 92% (West Greenland ringed seals), 88% (East Greenland ringed seals) and 85% (East Greenland polar bears). The PFOS concentrations increased up to 2006 with doubling times of approximately 6 years for the ringed seal populations and 14 years in case of polar bears. Since then a rapid decrease has occurred with clearing half-lives of approximately 1, 2 and 4 years, respectively. In polar bears perfluorohexane sulphonate (PFHxS) and perfluorooctane sulphonamide (PFOSA) also showed decreasing trends in recent years as do perfluorodecanoic acid (PFDA) and perfluoroundecanoic acid (PFUnA). For the West Greenland ringed seal population perfluorooctanoic acid (PFOA), perfluorononanoic acid (PFNA), PFDA and PFUnA peaked in the mid 2000s, whereas PFNA, PFDA and PFUnA in the East Greenland population have been stable or increasing in recent years. The peak of PFASs in Greenland ringed seals and polar bears occurred at a later time than in Canadian seals and polar bears and considerably later than observed in seal species from more southern latitudes. We suggest that this could be explained by the distance to emission hot-spots and differences in long-range transport to the Arctic., (Copyright © 2013 Elsevier Ltd. All rights reserved.)

Legacy organochlorine contaminants were determined in adipose tissues from 294 polar bears (Ursus maritimus) sampled in East Greenland in 23 of the 28years between 1983 and 2010. Of 19 major legacy contaminants and congeners (ΣPCB, 4 PCB congeners (CB153, 180, 170/190), ΣDDT, p,p'-DDE, p,p' -DDD and p,p'-DDT, α- and β-hexachlorocyclohexane (HCH), HCB, octachlorostyrene, dieldrin, oxychlordane, cis- and trans-chlordane, cis- and trans-nonachlor, heptachlor epoxide and BB-153), 18 showed statistically significant average yearly declines of -4.4% (range: -2.0 to -10.8%/year) among subadult polar bears (i.e. females<5years, males<6years). For example, the ∑PCB concentrations declined 2.7 fold from 22730ng/g lw (95% C.I.: 12470-32990ng/g lw) in 1983-1986 to 8473ng/g lw (95% C.I.: 6369-9776ng/g lw) in 2006-2010. Similar but fewer statistically significant trends were found for adult females and adult males likely due to smaller sample size and years. Despite declines as a result of international regulations, relatively high levels of these historic pollutants persist in East Greenland polar bear tissues., (Copyright © 2012 Elsevier Ltd. All rights reserved.)

Brominated flame retardants were determined in adipose tissues from 294 polar bears (Ursus maritimus) sampled in East Greenland in 23 of the 28years between 1983 and 2010. Significant linear increases were found for sum polybrominated diphenyl ether (ΣPBDE), BDE100, BDE153, and hexabromocyclododecane (HBCD). Average increases of 5.0% per year (range: 2.9-7.6%/year) were found for the subadult polar bears. BDE47 and BDE99 concentrations did not show a significant linear trend over time, but rather a significant non-linear trend peaking between 2000 and 2004. The average ΣPBDE concentrations increased 2.3 fold from 25.0ng/g lw (95% C.I.: 15.3-34.7ng/g lw) in 1983-1986 to 58.5ng/g lw (95% C.I.: 43.6-73.4ng/g lw) in 2006-2010. Similar but fewer statistically significant trends were found for adult females and adult males likely due to smaller sample size and years. Analyses of δ(15)N and δ(13)C stable isotopes in hair revealed no clear linear temporal trends in trophic level or carbon source, respectively, and non-linear trends differed among sex and age groups. These increasing concentrations of organobromine contaminants contribute to complex organohalogen mixture, already causing health effects to the East Greenland polar bears., (Copyright © 2012 Elsevier Ltd. All rights reserved.)

Rapid climate changes are occurring in the Arctic, with substantial repercussions for arctic ecosystems. It is challenging to assess ecosystem changes in remote polar environments, but one successful approach has entailed monitoring the diets of upper trophic level consumers. Quantitative fatty acid signature analysis (QFASA) and fatty acid carbon isotope (δ(13) C-FA) patterns were used to assess diets of East Greenland (EG) polar bears (Ursus maritimus) (n = 310) over the past three decades. QFASA-generated diet estimates indicated that, on average, EG bears mainly consumed arctic ringed seals (47.5 ± 2.1%), migratory subarctic harp (30.6 ± 1.5%) and hooded (16.7 ± 1.3%) seals and rarely, if ever, consumed bearded seals, narwhals or walruses. Ringed seal consumption declined by 14%/decade over 28 years (90.1 ± 2.5% in 1984 to 33.9 ± 11.1% in 2011). Hooded seal consumption increased by 9.5%/decade (0.0 ± 0.0% in 1984 to 25.9 ± 9.1% in 2011). This increase may include harp seal, since hooded and harp seal FA signatures were not as well differentiated relative to other prey species. Declining δ(13) C-FA ratios supported shifts from more nearshore/benthic/ice-associated prey to more offshore/pelagic/open-water-associated prey, consistent with diet estimates. Increased hooded seal and decreased ringed seal consumption occurred during years when the North Atlantic Oscillation (NAO) was lower. Thus, periods with warmer temperatures and less sea ice were associated with more subarctic and less arctic seal species consumption. These changes in the relative abundance, accessibility, or distribution of arctic and subarctic marine mammals may have health consequences for EG polar bears. For example, the diet change resulted in consistently slower temporal declines in adipose levels of legacy persistent organic pollutants, as the subarctic seals have higher contaminant burdens than arctic seals. Overall, considerable changes are occurring in the EG marine ecosystem, with consequences for contaminant dynamics., (© 2013 John Wiley & Sons Ltd.)

The present study compares blood plasma clinical-chemical parameters (BCCPs) in birds from three geographically distinct North Atlantic Great skua (Stercorarius skua) colonies. Birds from these sites bioaccumulate different POP (persistent organic pollutant) concentrations and that enabled us to compare Great skua BCCPs in different exposure scenarios. Persistent organic pollutants (organochlorines: PCB, DDT, chlordanes, HCB, HCH, mirex and brominated flame retardants: PBDEs) and nineteen BCCPs were analysed in 114 adult Great skuas sampled during summer 2009 in North Atlantic colonies at Bjørnøya (n=42), Iceland (n=57) and Shetland (n=15). Specimens from Bjørnøya had the highest blood plasma concentrations of all contaminant groups followed by Iceland and Shetland birds, respectively (ANOVA: p<0.05). Most of the 19 BCCP parameters followed the pattern of colony differences found for contaminants, with Bjørnøya having the highest concentrations. However seven BCCPs, the three liver enzymes ALKP, ALAT and GGT as well as bile acids, cholesterol, sodium and potassium, did not differ between colonies (ANOVA: p>0.05). Therefore correlation analyses of these seven BCCPs vs. POPs were done on the combined colony data while the analyses of the remaining 12 BCCPs were carried out for each colony separately. The analyses of combined colony data showed that the blood plasma concentration of liver enzymes ALAT and GGT increased with increasing concentrations of ΣPBDE and ΣHCH, HCB and ΣCHL, respectively (all Pearson's p<0.05). In Great skuas from Shetland, the important osmotic transport protein albumin increased with increasing concentrations of ΣPCB and ΣDDT, while total blood plasma protein increased with ΣPCB, ΣDDT, ΣHCH and HCB concentrations (all Pearson's p<0.05). In both Bjørnøya and Iceland skuas, blood plasma pancreatic enzyme amylase decreased with increasing ΣHCH concentrations while the erythrocyte waste product total bilirubin in blood plasma increased with increasing ΣHCH and ΣPBDE concentrations in Iceland Great skuas (all Pearson's p<0.05). In Bjørnøya birds, blood plasma urea from protein metabolism (reflects kidney function) increased with increasing ΣPBDE concentrations (Pearson's p<0.05). Furthermore, a redundancy analysis showed that 10.6% of the variations in BCCPs could be explained by the variations in POP concentrations. Based on these results we suggest that liver and renal functions could be negatively affected by different POP compounds. It is, however, uncertain if the colony BCCP differences and their relationship to POP concentrations reflect health effects that could have an overall impact on the populations via reduced survival and reproduction parameters., (Copyright © 2013 Elsevier Inc. All rights reserved.)

Organohalogen contaminants bioaccumulate to high concentrations in tissues of polar bears (Ursus maritimus). The exposure levels are in the order to be toxic to inner organs like liver and kidney. We therefore investigated the temporal development of lesions in liver (n=115) and kidney (n=122) samples from East Greenland polar bears taken over the 12 year period from 1999 to 2010. Seven liver and seven kidney lesions were observed of which six were age-related. Controlling for this, the analyses showed that hepatic steatosis and renal cell infiltrations, glomerular sclerosis and tubular hyperplasia decreased over the investigated time period (all p<0.05). Similarly, hypertrophy of hepatic Ito cells, renal glomerular capillary wall thickening and interstitial fibrosis increased over the study period (all p<0.05). Regarding contaminant, concentrations of polybrominated diphenyl ethers in adipose tissue were negatively associated with hepatic mononuclear cell infiltrations (p=0.05) and a similar trend was found for Hg (p=0.09). Hexachlorobenzene was positively associated with portal cell infiltrations and hepatic lipid granulomas, while polychlorinated biphenyls were negatively associated with the prevalence of steatosis (both p<0.05) and a similar trend was found for hexachlorocyclohexanes (p=0.08). Mercury was positively correlated with the frequencies of hypertrophic Ito cells (p=0.002) and a similar trend was found for perfluorooctanesulfonic acid (p=0.07). In renal tissue, hexachlorocyclohexanes were positively associated with medullar hyaline casts (p=0.03) and a similar trend was found for cell infiltrations (p=0.08). There was a trend of trans-nonachlor being positively associated with glomerular sclerosis (p=0.06) while dichlorodiphenyltrichloroethanes were negatively associated with tubular hyperplasia (p=0.02). These results suggest that specific liver and renal lesions have decreased or increased over time and that long-range transported organohalogen contaminants and mercury may be among the co-factors responsible for these observations. These relationships are important to take into account when biomonitoring health and pollution in wildlife species such as polar bears., (Copyright © 2012 Elsevier Ltd. All rights reserved.)

Raptors are exposed to biomagnifying and toxic organohalogenated compounds (OHCs) such as organochlorines, brominated flame retardants and perfluorinated compounds. To investigate how OHC exposure may affect biochemical pathways we collected blood plasma from Norwegian northern goshawk (n=56), golden eagle (n=12) and white-tailed eagle (n=36) nestlings during three consecutive breeding seasons. We found that blood plasma concentrations of calcium, sodium, creatinine, cholesterol, albumin, total protein, urea, inorganic phosphate, protein:creatinine, urea:creatinine and uric acid:creatinine ratios and liver enzymes ALKP and ALAT were positively correlated to PCBs, chlordanes, p,p'-DDE, HCB, PFCs and/or PBDEs. Total bilirubin and glucose were negatively correlated to PCBs while magnesium and potassium were negatively correlated to HCB and p,p'-DDE. In addition, protein:creatinine and ALAT were also negatively correlated to PCBs and PFCs, respectively. The most significant relationships were found for the highly contaminated northern goshawks and white-tailed eagles. The statistical relationships between OHCs and BCCPs indicate that biochemical pathways could be influenced while it is uncertain if such changes have any health effects. The OHC concentrations were below concentrations causing reproductive toxicity in adults of other raptor species but similar to those of concern for endocrine disruption of thyroid hormones in e.g., bald eagles., (Copyright © 2012 Elsevier Inc. All rights reserved.)

We examined the use of mercury (Hg) and nitrogen and carbon stable isotopes in teeth of polar bear (Ursus maritimus) from Svalbard as biotracers of temporal changes in Hg pollution exposure between 1964 and 2003. Teeth were regarded as a good matrix of the Hg exposure, and in total 87 teeth of polar bears were analysed. Dental Hg levels ranged from 0.6 to 72.3 ng g(-1) dry weight and increased with age during the first 10 years of life. A decreasing time trend in Hg concentrations was observed over the recent four decades while no temporal changes were found in the stable isotope ratios of nitrogen (δ(15)N) and carbon (δ(13)C). This suggests that the decrease of Hg concentrations over time was more likely due to a lower environmental Hg exposure in this region rather than a shift in the feeding habits of Svalbard polar bears.

This study investigated spatial and temporal trends of lead (Pb) and zinc (Zn) in resident and transplanted Flavocetraria nivalis lichens near the former Black Angel Mine in Maarmorilik, West Greenland. The objectives of the study were to evaluate resident and transplanted lichens for monitoring dust contamination and investigate trends in mine-related dust contamination near the mine. The mine operated between 1973 and 1990 and lichens were regularly sampled between 1986 and 2009. When the mine operated, elevated concentrations of Pb, Zn and other elements were observed in resident lichens up to 35 km from Maarmorilik. In the period after mine closure, Pb and Zn concentrations in resident lichens decreased with 1-11% and 0-6% per year, respectively. From 1996 to 2009, lichens were transplanted into the study area from an uncontaminated site and collected the following year. After 1 year, transplanted lichens showed elevated concentrations of Pb and Zn but contained consistently less Pb and Zn compared to resident lichens (24±23% and 63±37%, respectively). During the most recent sampling in 2009, transplanted lichens still showed significantly elevated Pb concentrations (up to a factor 270) within a distance of 20 km from Maarmorilik. Zinc concentrations were only significantly elevated at sites within 5 km from the mine. Time-series regression analyses showed no significant decreases in Pb and Zn in transplanted lichens at any of the sites during the period 1996-2009. In conclusion, our study showed that resident F. nivalis lichens could not be used to evaluate the recent annual dust contamination in Maarmorilik. Lichen transplants, however, were considered adequate for assessing spatial and temporal trends in Pb and Zn contamination from recently deposited dust. The continuous dispersal of contaminated dust in Maarmorilik almost 20 years after mine closure reveals a slow recovery from mining contamination in this arctic area., (Copyright © 2011 Elsevier B.V. All rights reserved.)

A statistically robust method was applied to 83 time-series of mercury in Arctic biota from marine, freshwater and terrestrial ecosystems with the purpose of generating a 'meta-analysis' of temporal trend data collected over the past two to three decades, mostly under the auspices of the Arctic Monitoring and Assessment Program (AMAP). Sampling locations ranged from Alaska in the west to northern Scandinavia in the east. Information from recently published temporal trend studies was tabulated to supplement the results of the statistical analyses. No generally consistent trend was evident across tissues and species from the circumpolar Arctic during the last 30years or so. However, there was a clear west-to-east gradient in the occurrence of recent increasing Hg trends, with larger numbers and a higher proportion of biotic datasets in the Canadian and Greenland region of the Arctic showing significant increases than in the North Atlantic Arctic. Most of the increasing datasets were for marine species, especially marine mammals. A total of 16 (19%) out of the 83 time-series could be classified as "adequate", where adequate is defined as the number of actual monitoring years in a time-series being equal to or greater than the number of years of sampling required to detect a 5% annual change in Hg concentrations, with a significance level of P<0.05 and 80% statistical power. At the time of the previous AMAP Assessment, only 10% of the Hg time-series were deemed adequate. If an additional 5years of data were to be added to the current set of time-series, it is predicted that 53% of time-series would become adequate., (Copyright © 2011 Elsevier B.V. All rights reserved.)

A statistically robust method was applied to 316 time-series of 'legacy' persistent organic pollutants (POPs) in Arctic biota from marine, freshwater and terrestrial ecosystems with the purpose of generating a 'meta-analysis' of temporal trend data collected over the past two to three decades for locations from Alaska in the west to northern Scandinavian in the east. Information from recently published temporal trend studies was tabulated and comparisons were also drawn with trends in arctic air. Most of the analysed time-series of legacy POP compounds showed decreasing trends, with only a few time-series showing significantly increasing trends. Compounds such as alpha-HCH, gamma-HCH and SigmaDDT had a relatively high proportion of time-series showing significantly decreasing trends; SigmaCHL had the lowest proportion. beta-HCH was an exception, where long-range transport through the ocean, and not the atmosphere, may explain several increasing trends that were detected in the Canadian Arctic. Moving east from the Canadian Arctic there was a trend towards a greater proportion of significantly decreasing trends. Several time-series for DDE and SigmaDDT showed significantly non-exponential trends, most often with a period of relative stability followed by a decrease. The median 'minimum detectable annual change within a 10-year period' for all of the time-series considered was 12% which did not meet the desirable level of statistical power capable of detecting a 5% annual change with a significance level of 5% within a 10-year period. The trends observed in the biota were consistent with decreasing trends of legacy POPs reported for Arctic air which appear to follow historic decreases in emissions. However, recent decreases in air are also starting to show signs of levelling off which may be an indication that atmospheric concentrations and, consequently those in the biota, are being less driven by primary sources and more by environmental processes and degradation., (Copyright 2009 Elsevier B.V. All rights reserved.)

The aim of this study is to elucidate if DDE (dichlorodiphenyldichloroethylene) or PCB (polybrominated diphenyls), are responsible for the pathological alterations observed in Swedish otter bone tissues. Femurs from 86 male otters collected between 1832 and 2004 were measured using peripheral quantitative computed tomography (pQCT). Some otters had very high and others fairly low concentrations of OCs (ranging between 1.4-970 mg SigmaPCB/kg l.w. and 0.0-24 mg DDE/kg l.w. in muscle tissue). Positive relationships were found between three of the four cortical bone variables analysed (area, content and thickness) and SigmaPCB concentration, while no significant relationships with DDE concentration were found. None of the trabecular variables were significantly related to PCB or DDE concentration. Three of the four trabecular bone variables showed decreasing values in the beginning and increasing values at the end of period 1974-2004. No temporal trends were found for cortical bone variables. OC concentrations decreased between 1974 and 2004., (Copyright (c) 2010 Elsevier Inc. All rights reserved.)

Organohalogen contaminants (OHCs) may affect various physiological parameters in birds including blood chemistry. We therefore examined blood plasma clinical-chemical parameters and OHCs in golden eagle, white-tailed eagle and goshawk chicks from Northern Norway. Correlation analyses on pooled data showed that alkaline phosphatase (ALKP), glucose and creatinine were significantly negatively correlated to various OHCs (all: p<0.05; r: -0.43 to -0.55; n=23), while alanine aminotransferase (ALAT), total protein, cholesterol, uric acid, total bilirubin, ratios protein:creatinine and uric acid:creatinine were significantly positively correlated to various OHCs (all: p<0.05; r: 0.43-0.96). Based on these relationships, we suggest that the OHC concentrations found in certain raptor chicks of Northern Scandinavia may impact blood plasma biochemistry in a way that indicates impacts on liver, kidney, bone, endocrinology and metabolism. In order to elaborate further on these relationships and mechanisms, we recommend that a larger study should take place in the near future.

Polar bears (Ursus maritimus) feed mainly on ringed seal (Phoca hispida) and consume large quantities of blubber and consequently have one of the highest tissue concentrations of organohalogen contaminants (OHCs) worldwide. In East Greenland, studies of OHC time trends and organ system health effects, including reproductive, were conducted during 1990-2006. However, it has been difficult to determine the nature of the effects induced by OHC exposures on wild caught polar bears using body burden data and associated changes in reproductive organs and systems. We therefore conducted a risk quotient (RQ) evaluation to more quantitatively evaluate the effect risk on reproduction (embryotoxicity and teratogenicity) based on the critical body residue (CBR) concept and using a physiologically-based pharmacokinetic (PBPK) model. We applied modelling approaches to PCBs, p,p'-DDE, dieldrin, oxychlordane, HCHs, HCB, PBDEs and PFOS in East Greenland polar bears based on known OHC pharmacokinetics and dynamics in laboratory rats (Rattus rattus). The results showed that subcutaneous adipose tissue concentrations of dieldrin (range: 79-1271 ng g(-1) lw) and PCBs (range: 4128-53,923 ng g(-1) lw) reported in bears in the year 1990 were in the range to elicit possible adverse health effects on reproduction in polar bears in East Greenland (all RQs > or = 1). Similar results were found for PCBs (range: 1928-17,376 ng g(-1) lw) and PFOS (range: 104-2840 ng g(-1) ww) in the year 2000 and for dieldrin (range: 43-640 ng g(-1) lw), PCBs (range: 3491-13,243 ng g(-1) lw) and PFOS (range: 1332-6160 ng g(-1) ww) in the year 2006. The concentrations of oxychlordane, DDTs, HCB and HCHs in polar bears resulted in RQs<1 and thus appear less likely to be linked to reproductive effects. Furthermore, sumRQs above 1 suggested risk for OHC additive effects. Thus, previous suggestions of possible adverse health effects in polar bears correlated to OHC exposure are supported by the present study. This study also indicates that PBPK models may be a supportive tool in the evaluation of possible OHC-mediated health effects for Arctic wildlife.

We investigated the impact from dietary OC (organochlorine) exposure and restricted feeding (emaciation) on bone mineral density (BMD; g hydroxy-apatite cm(-2)) in femoral, vertebrate, skull and baculum osteoid tissue from farmed Arctic blue foxes (Vulpes lagopus). For femur, also biomechanical properties during bending (displacement [mm], load [N], energy absorption [J] and stiffness [N/mm]) were measured. Sixteen foxes (EXP) were fed a wet food containing 7.7% OC-polluted minke whale (Balaenoptera acutorostrata) blubber in two periods of body fat deposition (Aug-Dec) and two periods of body fat mobilisation (Jan-July) in which the food contained less energy and only 2% blubber. SigmaOC food concentration in the food containing 7.7% whale blubber was 309 ng/g wet mass. This corresponded to a SigmaOC exposure of ca. 17 microg/kg body mass/d and a responding SigmaOC residue in subcutaneous adipose tissue of ca. 1700 ng/g live mass in the 8 EXP fat foxes euthanized after 16 months. A control group (CON) composed of 15 foxes were fed equal daily caloric amounts of clean pork (Sus scrofa) fat. After 16 months, 8 EXP and 7 CON foxes were euthanized (mean body mass=9.25 kg) while the remaining 8 EXP and 8 CON foxes were given restricted food rations for 6 months resulting in a body weight reduction (mean body mass=5.46 kg). The results showed that only BMD(skull) vs. BMD(vertebrae) were significantly correlated (R=0.68; p=0.03; n=10) probably due to a similar composition of trabecular and cortical osteoid tissue. No difference in any of the BMD measurements or femoral biomechanical properties was found between EXP and CON foxes although BMD baculum was 1.6-folds lower in the EXP group. However, lean summer foxes had significantly lower femoral biomechanical properties measured as displacement (mm), energy absorption (J) and time (s) biomechanical properties than fat winter foxes (all p<0.004). This indicates lower stiffness and softer bones from fasting which is in agreement with previous studies. Further, it should be kept in mind when studying bone tissues in Arctic mammals also in order to avoid confounding effects from body condition.

Polybrominated diphenyl ethers (PBDEs) were analysed in adipose tissue from 92 East Greenland polar bears (Ursus maritimus) sampled during 1999-2001. Mean SigmaPBDE concentrations were 70 ng/g lipid weight (lw) (range: 22-192 ng/g lw) and showed no relationship with age or sex. Of the 32 analysed PBDE congeners; BDE47, BDE153, BDE99 and BDE100 dominated, and comprised 99.6% of the SigmaPBDE concentration. The SigmaPBDE concentration had a highly significant correlation with SigmaPCB, SigmaCHL, dieldrin, HCB and SigmaHCH concentrations. We found a seasonal pattern of median SigmaPBDE concentration with 1.2 to 1.8 times higher concentrations in March to July than the rest of the year. The seasonal variation also provides a clue to the seasonal exposure, bio-availability, toxic exposure and degradation. We suggest that future geographical PBDE data comparisons may not need corrections for sex or age, but such data sets should be corrected for seasonal variability, using the presented correctional trigonometric regression.