Mercury speciation in pilot whale from Faroe Islands, 1977-2015.

Mercury (Hg) is a naturally occurring heavy metal, but human activities and natural processes have led to increased pollution with Hg in the environment. Organic mercury, such as methyl mercury (MeHg), is considered more toxic than most inorganic mercury compounds. MeHg is rapidly taken up by aquatic organisms and bioaccumulates through the aquatic food web. The bioaccumulation causes high levels of MeHg in apex predators, such as pilot whales. Pilot whale meat is a traditional food source on the Faroe Islands; thus the consumption of pilot whale meat can lead to high Hg exposures in humans. The majority of the total Hg in pilot whale and fish is generally assumed to be MeHg. However, the relative amount of MeHg to total Hg can be highly variable. For risk assessment, it is relevant to know both the MeHg and the total Hg content. This study summarizes the knowledge of muscle MeHg concentrations relative to total Hg concentrations in pilot whales in the Faroe Islands. The pilot whale tissue was sampled during 1977-78, 1986-87, 2009-2010, and 2015. The 2015 samples included two pairs of fetuses/mothers. The results showed that the 1977-78 pilot whale muscle samples had lower relative concentrations of MeHg to total Hg compared to samples from the subsequent years. This discrepancy between early and later years could not solely be explained by increased demethylation related to concentration differences. Instead, the difference is more likely explained by variations in relative amounts of MeHg in prey of the pilot whales. In the fetuses the total Hg concentration was 20% of the Hg concentration in the mother. The relative MeHg concentrations in the fetuses were also lower (∼20%-30%) than in the mother. However, the MeHg to total Hg fraction in the fetus was similar or higher than in the mother.

Temporal trends of persistent organic pollutants in Arctic marine and freshwater biota.

More than 1000 time-series of persistent organic pollutants (POPs) in Arctic biota from marine and freshwater ecosystems some extending back to the beginning of 1980s were analyzed using a robust statistical method. The Arctic area encompassed extended from Alaska, USA in the west to northern Scandinavian in the east, with data gaps for Arctic Russia and Arctic Finland. The aim was to investigate whether temporal trends for different animal groups and matrices were consistent across a larger geographical area. In general, legacy POPs showed decreasing concentrations over the last two to three decades, which were most pronounced for α-HCH and least pronounced for HCB and ß-HCH. Few time-series of legacy POPs showed increasing trends and only at sites suspected to be influenced by local source. The brominated flame retardant congener BDE-47 showed a typical trend of increasing concentration up to approximately the mid-2000s followed by a decreasing concentration. A similar trend was found for perfluorooctane sulfonic acid (PFOS). These trends are likely related to the relatively recent introduction of national and international controls of hexa- and hepta-BDE congeners and the voluntary phase-out of PFOS production in the USA in 2000. Hexabromocyclododecane (HBCDD) was the only compound in this study showing a consistent increasing trend. Only 12% of the long-term time-series were able to detect a 5% annual change with a statistical power of 80% at α < 0.05. The remaining 88% of time-series need additional years of data collection before fulfilling these statistical requirements. In the case of the organochlorine long-term time-series, 45% of these would require >20 years monitoring before this requirement would be fulfilled.

Hepatic phase I and II biotransformation responses and contaminant exposure in long-finned pilot whales from the Northeastern Atlantic.

Faroe Island pilot whales have been documented to have high body burdens of organohalogen contaminants (OHCs), including polychlorinated biphenyls (PCBs) and polybrominated diphenyl ethers (PBDEs), but low burdens of their respective hydroxylated metabolites (OH-PCBs and OH-PBDEs). The present study investigated the hepatic expression and/or catalytic activities of phase I and II biotransformation enzymes in relation to hepatic concentrations of target OHCs, including OH-PCBs and OH-PBDEs, in long-finned pilot whales (Globicephala melas) from the Northeastern Atlantic. CYP1A, 2B, 2E and 3A protein expressions were identified in juveniles and adult males, but not in adult females. Ethoxyresorufin-O-deethylase (EROD) activity was significantly lower in adult females than in juveniles and adult males. Using multivariate analyses to investigate relationships between biological responses and OHC concentrations, a positive relationship was identified between EROD and OHCs. The activity levels of phase II conjugating enzymes (uridine 5'-diphospho-glucuronosyltransferase [UDPGT], and glutathione S-transferase [GST]) were low. The analyses of mRNA expression did not show correlative relationships with OHC concentrations, but cyp1a and ahr transcripts were positively correlated with EROD activity. We suggest that the low concentrations of OH-PCBs and OH-PBDEs reported in pilot whales is probably due to the identified low phase I biotransformation activities in the species.

Steroid hormones and persistent organic pollutants in plasma from North-eastern Atlantic pilot whales.

Persistent organic pollutants (POPs) are known to have endocrine disruptive effects, interfering with endogenous steroid hormones. The present study examined nine steroid hormones and their relationships with the concentrations of selected POPs in pilot whales (Globicephala melas) from the Faroe Islands, NE Atlantic. The different steroids were detected in 15 to all of the 26 individuals. High concentrations of progesterone (83.3-211.7pmol/g) and pregnenolone (PRE; 4.68-5.69pmol/g) were found in three adult females indicating that they were pregnant or ovulating. High androgen concentrations in two of the males reflected that one was adult and that one (possibly) had reached puberty. In males a significant positive and strong correlation between body length and testosterone (TS) levels was identified. Furthermore, positive and significant correlations were found between 4-OH-CB107/4'-OH-CB108 and 17ß-estradiol in males. In adult females significant positive correlations were identified between PRE and CB149 and t-nonachlor, between estrone and CB138, -149, -187 and p,p'-DDE, between androstenedione and CB187, and between TS and CB-99 and -153. Although relationships between the POPs and the steroid hormones reported herein are not evidence of cause-effect relationships, the positive correlations between steroids and POPs, particularly in females, suggest that POPs may have some endocrine disrupting effects on the steroid homeostasis in this species.

Relationships between concentrations of selected organohalogen contaminants and thyroid hormones and vitamins A, E and D in Faroese pilot whales.

Pilot whales (Globicephala melas) from the Faroe Islands, North-East Atlantic, have high body concentrations of organohalogenated compounds (OHCs), such as polychlorinated biphenyls (PCBs), organochlorinated pesticides (OCPs) and brominated flame retardants (BFRs). The aim of the present study was to examine if and to what extent blood plasma and liver concentrations of several groups of these OHCs are related to concentrations of relevant nutritional and hormonal biomarkers in pilot whales. Thyroid hormones (THs: total and free thyroxine and total and free triiodothyronine) and vitamin A (retinol), D (25-hydroxyvitamin D3) and E (α-tocopherol) were analysed in plasma (n=27) and vitamin A (total vitamin A, retinol and retinyl palmitate) and E (α- and γ-tocopherol) were analysed in liver (n=37) of Faroe Island pilot whales. Correlative relationships between the biomarkers and OHC concentrations previously analysed in the same tissues in these individuals were studied. The TH concentrations in plasma were significantly higher in juveniles than in adults. Vitamin D concentrations in plasma and α- and γ-tocopherol in liver were higher in adults than in juveniles. Multivariate statistical modelling showed that the age and sex influenced the relationship between biomarkers and OHCs. Some significant positive relationships were found between OHCs and thyroid hormone concentrations in the youngest juveniles (p<0.05). In plasma of juvenile whales α-tocopherol was also positively correlated with all the OHCs (p<0.05). Only few significant correlations were found between single OHCs and retinol and vitamin D in plasma within the age groups. There were significant negative relationships between hepatic PBDE concentrations and retinol (BDE-47) and γ-tocopherol (BDE-49, -47, -100, -99, -153) in liver. The relationships between OHCs and THs or vitamins suggest that in pilot whales OHCs seem to have minor effects on TH and vitamin concentrations.

Legacy and emerging organic pollutants in liver and plasma of long-finned pilot whales (Globicephala melas) from waters surrounding the Faroe Islands.

Concentrations of PCBs, organochlorine pesticides (OCPs), brominated flame retardants and a suite of relevant metabolites of these POPs, in all 175 different compounds, were determined in liver and plasma of traditionally hunted pilot whales (n=14 males and n=13 females of different age groups) from the Faroe Islands. The main objectives of this study were to determine differences in the presence and concentrations of the compounds in the liver and plasma, how they depend on developmental stage (calves, sub adults, and adult females), and to assess maternal transfer of the compounds to suckling calves. Generally, the lipid weight (lw) concentrations of quantified POPs in the liver and plasma of pilot whales were positively correlated, and lw concentrations of most POPs did not differ between these matrices. However, concentrations of some individual POPs differed significantly (p<0.05) between plasma and liver; CB-153 (p=0.044), CB-174 (p=0.027) and BDE-47 (p=0.017) were higher in plasma than in liver, whereas p,p'-DDE (p=0.004) and HCB (p<0.001) were higher in liver than in plasma. POP concentrations differed between age/gender groups with lower levels in adult females than in juveniles. The relative distribution of compounds also differed between the age groups, due to the influence of the maternal transfer of the compounds. The results indicated that larger, more hydrophobic POPs were transferred to the offspring less efficiently than smaller or less lipid soluble compounds. Very low levels of both OH- and/or MeSO2-PCB and PBDE metabolites were found in all age groups, with no significant (p>0.05) differences between the groups, strongly suggesting a very low metabolic capacity for their formation in pilot whales. The lack of difference in the metabolite concentrations between the age groups also indicates less maternal transfer of these contaminant groups compared to the precursor compounds.

Pristine Arctic: background mapping of PAHs, PAH metabolites and inorganic trace elements in the North-Atlantic Arctic and sub-Arctic coastal environment.

As the ice cap of the Arctic diminishes due to global warming, the polar sailing route will be open larger parts of the year. These changes are likely to increase the pollution load on the pristine Arctic due to large vessel traffic from specific contaminant groups, such as polycyclic aromatic hydrocarbons (PAHs). A well-documented baseline for PAH concentrations in the biota in the remote regions of the Nordic Seas and the sub-Arctic is currently limited, but will be vital in order to assess future changes in PAH contamination in the region. Blue mussels (Mytilus edulis) were collected from remote sites in Greenland, Iceland, the Faroe Islands, Norway and Sweden as well as from urban sites in the same countries for comparison. Cod (Gadus morhua) was caught north of Iceland and along the Norwegian coast. Sixteen priority PAH congeners and the inorganic trace elements arsenic, cadmium, mercury and lead were analysed in the blue mussel samples as well as PAH metabolites in cod bile. Σ16PAHs ranged from 28 ng/g dry weight (d.w.) (Álftafjörður, NW Iceland) to 480 ng/g d.w. (Ísafjörður, NW Iceland). Mussel samples from Mjóifjörður, East Iceland and Maarmorilik, West Greenland, contained elevated levels of Σ16PAHs, 370 and 280 ng/g d.w., respectively. Levels of inorganic trace elements varied with highest levels of arsenic in mussels from Ísafjörður, Iceland (79 ng/g d.w.), cadmium in mussels from Mjóifjörður, Iceland (4.3 ng/g d.w.), mercury in mussels from Sørenfjorden, Norway (0.23 ng/g d.w.) and lead in mussels from Maarmorilik, Greenland (21 ng/g d.w.). 1-OH-pyrene was only found above limits of quantification (0.5 ng/mL) in samples from the Norwegian coast, ranging between 44 and 140 ng/ml bile. Generally, PAH levels were low in mussels from the remote sites investigated in the study, which indicates limited current effect on the environment.