Variations in thyroid hormone levels in endangered St. Lawrence Estuary belugas: Potential linkage with stress and organohalogen contaminant exposure.

The St. Lawrence Estuary (SLE) beluga (Delphinapterus leucas) population is highly exposed to an array of contaminants that were identified as one of the causes to the non-recovery of this endangered and declining population. In the last decade, an increasing number of parturition-associated complications and calf mortality has been reported in this population. It was suggested that elevated exposure to organohalogens (e.g., the halogenated flame retardants polybrominated diphenyl ethers [PBDEs]) and stress could play a role in this phenomenon by perturbing thyroid hormones. The objective of this study was to investigate the impact of concentrations of organohalogen contaminants and stress (cortisol levels) on thyroid hormone variations in adult male and female SLE belugas. Because plasma could not be collected in SLE belugas for ethical reasons, skin biopsy (n = 40) was used as a less-invasive alternative matrix to determine organohalogens (PBDEs and other halogenated flame retardants, polychlorinated biphenyls, and organochlorine pesticides), cortisol, and thyroid hormones (triiodothyronine [T3] and thyroxine [T4]), and their metabolites reverse T3 and 3,5-diiodothyronine [3,5-T2]). Cortisol and thyroid hormones were analyzed by ultra-performance liquid chromatography-multiple reactions monitoring mass spectrometry (UPLC-MRM/MS). This method was compared using skin and plasma samples obtained from Arctic belugas. Comparisons of linear models showed that cortisol was a weak predictor for T4, rT3 and 3,5-T2. Specifically, there was a weak significant negative association between T4 and cortisol levels. Moreover, in male SLE belugas, a weak significant positive association was found between T3 and Σ34PBDE concentrations in skin. Our findings suggest that stress (i.e., elevated skin cortisol levels) along with organohalogen exposure (mainly PBDEs) may be associated with thyroid hormone level perturbations in skin of cetaceans.

Do beluga whales truly migrate? Testing a key trait of the classical migration syndrome.

BACKGROUND: Migration enables organisms to access resources in separate regions that have predictable but asynchronous spatiotemporal variability in habitat quality. The classical migration syndrome is defined by key traits including directionally persistent long-distance movements during which maintenance activities are suppressed. But recently, seasonal round-trip movements have frequently been considered to constitute migration irrespective of the traits required to meet this movement type, conflating common outcomes with common traits required for a mechanistic understanding of long-distance movements. We aimed to test whether a cetacean ceases foraging during so-called migratory movements, conforming to a trait that defines classical migration. METHODS: We used location and dive data collected by satellite tags deployed on beluga whales (Delphinapterus leucas) from the Eastern Beaufort Sea population, which undertake long-distance directed movements between summer and winter areas. To identify phases of directionally persistent travel, behavioural states (area-restricted search, ARS; or Transit) were decoded using a hidden-Markov model, based on step length and turning angle. Established dive profiles were then used as a proxy for foraging, to test the hypothesis that belugas cease foraging during these long-distance transiting movements, i.e., they suppress maintenance activities. RESULTS: Belugas principally made directed horizontal movements when moving between summer and winter residency areas, remaining in a Transit state for an average of 75.4% (range = 58.5-87.2%) of the time. All individuals, however, exhibited persistent foraging during Transit movements (75.8% of hours decoded as the Transit state had ≥ 1 foraging dive). These data indicate that belugas actively search for and/or respond to resources during these long-distance movements that are typically called a migration. CONCLUSIONS: The long-distance movements of belugas do not conform to the traits defining the classical migration syndrome, but instead have characteristics of both migratory and nomadic behaviour, which may prove adaptive in the face of unpredictable environmental change. Such patterns are likely present in other cetaceans that have been labeled as migratory. Examination of not only horizontal movement state, but also the vertical behaviour of aquatic animals during directed movements is essential for identifying whether a species exhibits traits of the classical migration syndrome or another long-distance movement strategy, enabling improved ecological inference.

Contrasting intra-individual variation in size-based trophic and habitat shifts for two coastal Arctic fish species.

Within and among species variation in trophic and habitat shifts with body size can indicate the potential adaptive capacity of species to ecosystem change. In Arctic coastal ecosystems, which experience dramatic seasonal shifts and are undergoing rapid change, quantifying the trophic flexibility of coastal fishes with different migratory tactics has received limited attention. We examined the relationships among body length and condition (Fulton's K, phase angle from Bioelectrical Impedance Analysis) with trophic and habitat shifts (differences in δ15N and δ13C between blood tissues with different turnover rates) of two abundant and culturally important species, anadromous Arctic char (Salvelinus alpinus, n = 38) and sedentary Greenland cod (Gadus ogac, n = 65) during summer in coastal marine waters near Ulukhaktok, Northwest Territories, Canada. Habitat shifts (δ13C) increased with length (i.e., pelagic to benthic-littoral) and crossed-equilibrium (zero) at mid-sizes for both species. Seasonal trophic shifts (δ15N) were generally positive (i.e., increasing trophic level) for Arctic char and negative for Greenland cod. As hypothesised, intra-individual variation in size-based trophic shifts (δ15N-length residuals) increased with length for Arctic char. However, there were no trends with length in Greenland cod. Our findings highlight the importance of flexibility through ontogeny and mobility for Arctic char, whereas Greenland cod were generalist to localized prey and habitat across all sizes. The significant effect of body condition (phase angle) on size-based trophic shifts in Arctic char, and size-based habitat shifts in Greenland cod, highlight the potential trade-offs of contrasting life history strategies and capacity for ontogenetic niche plasticity.

Year-round utilization of sea ice-associated carbon in Arctic ecosystems.

Sea ice primary production is considered a valuable energy source for Arctic marine food webs, yet the extent remains unclear through existing methods. Here we quantify ice algal carbon signatures using unique lipid biomarkers in over 2300 samples from 155 species including invertebrates, fish, seabirds, and marine mammals collected across the Arctic shelves. Ice algal carbon signatures were present within 96% of the organisms investigated, collected year-round from January to December, suggesting continuous utilization of this resource despite its lower proportion to pelagic production. These results emphasize the importance of benthic retention of ice algal carbon that is available to consumers year-round. Finally, we suggest that shifts in the phenology, distribution and biomass of sea ice primary production anticipated with declining seasonal sea ice will disrupt sympagic-pelagic-benthic coupling and consequently the structure and the functioning of the food web which is critical for Indigenous Peoples, commercial fisheries, and global biodiversity.

A Multi-Matrix Metabolomic Approach in Ringed Seals and Beluga Whales to Evaluate Contaminant and Climate-Related Stressors.

As a high trophic-level species, ringed seals (Pusa hispida) and beluga whales (Delphinapterus leucas) are particularly vulnerable to elevated concentrations of biomagnifying contaminants, such as polychlorinated biphenyls (PCBs), polybrominated diphenyl ethers (PBDEs) and mercury (Hg). These species also face climate-change-related impacts which are leading to alterations in their diet and associated contaminant exposure. The metabolomic profile of marine mammal tissues and how it changes to environmental stressors is poorly understood. This study characterizes the profiles of 235 metabolites across plasma, liver, and inner and outer blubber in adult ringed seals and beluga whales and assesses how these profiles change as a consequence of contaminants and dietary changes. In both species, inner and outer blubber were characterized by a greater proportion of lipid classes, whereas the dominant metabolites in liver and plasma were amino acids, carbohydrates, biogenic amines and lysophosphatidylcholines. Several metabolite profiles in ringed seal plasma correlated with δ13C, while metabolite profiles in blubber were affected by hexabromobenzene in ringed seals and PBDEs and Hg in belugas. This study provides insight into inter-matrix similarities and differences across tissues and suggests that plasma and liver are more suitable for studying changes in diet, whereas liver and blubber are more suitable for studying the impacts of contaminants.

Evidence for three morphotypes among anadromous Arctic char (Salvelinus alpinus) sampled in the marine environment.

Variable resource use and responses to environmental conditions can lead to phenotypic diversity and distinct morphotypes within salmonids, including Arctic char (Salvelinus alpinus). Despite the cultural and economic importance of Arctic char in the Inuvialuit Settlement Region (ISR), limited data exist on the extent and presence of morphological diversity in this region. This is of concern for management given climate change impacts on regional fish populations. The authors investigated morphological diversity in anadromous Arctic char sampled during their summer marine migration-residency period when seasonal harvesting occurs in a coastal mixed-stock fishery. Geometric morphometric analysis was conducted using digital photographs of live Arctic char (n = 103) of which a sub-set was subsequently implanted with acoustic transmitters (n = 90) and released, and their overwintering lakes determined using active acoustic telemetry surveys. Twenty-three morphological landmarks were established and overlaid on digital images, and nine linear measurements of the body and head were recorded. Principle component analysis and K-means clustering based on linear measurements categorised fish into three morphotypes: slender body and slim head (n = 31), small and short head with a small mouth (n = 46) and elongated head shape with large mouth (n = 26). Tagged individuals of the three morphotypes occupied all lakes with no distinction observed. The three Arctic char morphotypes detected in this coastal mixed-stock fishery could represent adaptation to specific feeding-movement behaviours potentially tied to juvenile residency in freshwater systems, efficient exploitation of the marine prey pulse, or are relicts from ancestral types. To the authors' knowledge, this study is the first to identify distinct Arctic char morphotypes occurring in sympatry in the marine environment. Identifying phenotypic diversity will assist management to promote the sustainability of this regional fishery.

Investigating the dynamics of methylmercury bioaccumulation in the Beaufort Sea shelf food web: a modeling perspective.

High levels of methylmercury (MeHg) have been reported in Arctic marine biota, posing health risks to wildlife and human beings. Although MeHg concentrations of some Arctic species have been monitored for decades, the key environmental and ecological factors driving temporal trends of MeHg are largely unclear. We develop an ecosystem-based MeHg bioaccumulation model for the Beaufort Sea shelf (BSS) using the Ecotracer module of Ecopath with Ecosim, and apply the model to explore how MeHg toxicokinetics and food web trophodynamics affect bioaccumulation in the BSS food web. We show that a food web model with complex trophodynamics and relatively simple MeHg model parametrization can capture the observed biomagnification pattern of the BSS. While both benthic and pelagic production are important for transferring MeHg to fish and marine mammals, simulations suggest that benthic organisms are primarily responsible for driving the high trophic magnification factor in the BSS. We illustrate ways of combining empirical observations and modelling experiments to generate hypotheses about factors affecting food web bioaccumulation, including the MeHg elimination rate, trophodynamics, and species migration behavior. The results indicate that population dynamics rather than MeHg elimination may determine population-wide concentrations for fish and lower trophic level organisms, and cause large differences in concentrations between species at similar trophic levels. This research presents a new tool and lays the groundwork for future research to assess the pathways of global environmental changes in MeHg bioaccumulation in Arctic ecosystems in the past and the future.

Special issue on the AMAP 2021 assessment of mercury in the Arctic.

This Editorial presents an overview of the Special Issue on advances in Arctic mercury (Hg) science synthesized from the 2021 assessment of the Arctic Monitoring and Assessment Programme (AMAP). Mercury continues to travel to Arctic environments and threaten wildlife and human health in this circumpolar region. Over the last decade, progress has been achieved in addressing policy-relevant uncertainties in environmental Hg contamination. This includes temporal trends of Hg, its transport to and within the Arctic, methylmercury cycling, climate change influences, biological effects of Hg on fish and wildlife, human exposure to Hg, and forecasting of Arctic responses to different future scenarios of anthropogenic Hg emissions. In addition, important contributions of Indigenous Peoples to Arctic research and monitoring of Hg are highlighted, including through projects of knowledge co-production. Finally, policy-relevant recommendations are summarized for future study of Arctic mercury. This series of scientific articles presents comprehensive information relevant to supporting effectiveness evaluation of the United Nations Minamata Convention on Mercury.

Contributions and perspectives of Indigenous Peoples to the study of mercury in the Arctic.

Arctic Indigenous Peoples are among the most exposed humans when it comes to foodborne mercury (Hg). In response, Hg monitoring and research have been on-going in the circumpolar Arctic since about 1991; this work has been mainly possible through the involvement of Arctic Indigenous Peoples. The present overview was initially conducted in the context of a broader assessment of Hg research organized by the Arctic Monitoring and Assessment Programme. This article provides examples of Indigenous Peoples' contributions to Hg monitoring and research in the Arctic, and discusses approaches that could be used, and improved upon, when carrying out future activities. Over 40 mercury projects conducted with/by Indigenous Peoples are identified for different circumpolar regions including the U.S., Canada, Greenland, Sweden, Finland, and Russia as well as instances where Indigenous Knowledge contributed to the understanding of Hg contamination in the Arctic. Perspectives and visions of future Hg research as well as recommendations are presented. The establishment of collaborative processes and partnership/co-production approaches with scientists and Indigenous Peoples, using good communication practices and transparency in research activities, are key to the success of research and monitoring activities in the Arctic. Sustainable funding for community-driven monitoring and research programs in Arctic countries would be beneficial and assist in developing more research/monitoring capacity and would promote a more holistic approach to understanding Hg in the Arctic. These activities should be well connected to circumpolar/international initiatives to ensure broader availability of the information and uptake in policy development.

Temporal trends of mercury in Arctic biota: 10 more years of progress in Arctic monitoring.

Temporal trend analysis of (total) mercury (THg) concentrations in Arctic biota were assessed as part of the 2021 Arctic Monitoring and Assessment Programme (AMAP) Mercury Assessment. A mixed model including an evaluation of non-linear trends was applied to 110 time series of THg concentrations from Arctic and Subarctic biota. Temporal trends were calculated for full time series (6-46 years) and evaluated with a particular focus on recent trends over the last 20 years. Three policy-relevant questions were addressed: (1) What time series for THg concentrations in Arctic biota are currently available? (2) Are THg concentrations changing over time in biota from the Arctic? (3) Are there spatial patterns in THg trends in biota from the Arctic? Few geographical patterns of recent trends in THg concentrations were observed; however, those in marine mammals tended to be increasing at more easterly longitudes, and those of seabirds tended to be increasing in the Northeast Atlantic; these should be interpreted with caution as geographic coverage remains variable. Trends of THg in freshwater fish were equally increasing and decreasing or non-significant while those in marine fish and mussels were non-significant or increasing. The statistical power to detect trends was greatly improved compared to the 2011 AMAP Mercury Assessment; 70% of the time series could detect a 5% annual change at the 5% significance level with power ≥ 80%, while in 2011 only 19% met these criteria. Extending existing time series, and availability of new, powerful time series contributed to these improvements, highlighting the need for annual monitoring, particularly given the spatial and temporal information needed to support initiatives such as the Minamata Convention on Mercury. Collecting the same species/tissues across different locations is recommended. Extended time series from Alaska and new data from Russia are also needed to better establish circumarctic patterns of temporal trends.

A meta-collection of nitrogen stable isotope data measured in Arctic marine organisms from the Canadian Beaufort Sea, 1983-2013.

OBJECTIVES: Existing information on Arctic marine food web structure is fragmented. Integrating data across research programs is an important strategy for building a baseline understanding of food web structure and function in many Arctic regions. Naturally-occurring stable isotope ratios of nitrogen (δ15N) and carbon (δ13C) measured directly in the tissues of organisms are a commonly-employed method for estimating food web structure. The objective of the current dataset was to synthesize disparate δ15N, and secondarily δ13C, data in the Canadian Beaufort continental shelf region relevant to trophic and ecological studies at the local and pan-Arctic scales. DATA DESCRIPTION: The dataset presented here contains nitrogen and carbon stable isotope ratios (δ15N, δ13C) measured in marine organisms from the Canadian Beaufort continental shelf region between 1983 and 2013, gathered from 27 published and unpublished sources with associated sampling metadata. A total of 1077 entries were collected, summarizing 8859 individual organisms/samples representing 333 taxa across the Arctic food web, from top marine mammal predators to primary producers.

Body condition impacts blood and muscle oxygen storage capacity of free-living beluga whales (Delphinapterus leucas).

Arctic marine ecosystems are currently undergoing rapid environmental changes. Over the past 20 years, individual growth rates of beluga whales (Delphinapterus leucas) have declined, which may be a response to climate change; however, the scarcity of physiological data makes it difficult to gauge the adaptive capacity and resilience of the species. We explored relationships between body condition and physiological parameters pertaining to oxygen (O2) storage capacity in 77 beluga whales in the eastern Beaufort Sea. Muscle myoglobin concentrations averaged 77.9 mg g-1, one of the highest values reported among mammals. Importantly, blood haematocrit, haemoglobin and muscle myoglobin concentrations correlated positively to indices of body condition, including maximum half-girth to length ratios. Thus, a whale with the lowest body condition index would have ∼27% lower blood (26.0 versus 35.7 ml kg-1) and 12% lower muscle (15.6 versus 17.7 ml kg-1) O2 stores than a whale of equivalent mass with the highest body condition index; with the conservative assumption that underwater O2 consumption rates are unaffected by body condition, this equates to a >3 min difference in maximal aerobic dive time between the two extremes (14.3 versus 17.4 min). Consequently, environmental changes that negatively impact body condition may hinder the ability of whales to reach preferred prey sources, evade predators and escape ice entrapments. The relationship between body condition and O2 storage capacity may represent a vicious cycle, in which environmental changes resulting in decreased body condition impair foraging, leading to further reductions in condition through diminished prey acquisition and/or increased foraging efforts.

Intestinal polycyclic aromatic hydrocarbon-DNA adducts in a population of beluga whales with high levels of gastrointestinal cancers.

Carcinogenic polycyclic aromatic hydrocarbons (PAHs) were disposed directly into the Saguenay River of the St. Lawrence Estuary (SLE) by local aluminum smelters (Quebec, Canada) for 50 years (1926-1976). PAHs in the river sediments are likely etiologically related to gastrointestinal epithelial cancers observed in 7% of 156 mature (>19-year old) adult beluga found dead along the shorelines. Because DNA adduct formation provides a critical link between exposure and cancer induction, and because PAH-DNA adducts are chemically stable, we hypothesized that SLE beluga intestine would contain PAH-DNA adducts. Using an antiserum specific for DNA modified with several carcinogenic PAHs, we stained sections of paraffin-embedded intestine from 51 SLE beluga (0-63 years), 4 Cook Inlet (CI) Alaska beluga (0-26 years), and 20 beluga (0-46 years) living in Arctic areas (Eastern Beaufort Sea, Eastern Chukchi Sea, Point Lay Alaska) and aquaria, all with low PAH contamination. Stained sections showed nuclear light-to-dark pink color indicating the presence of PAH-DNA adducts concentrated in intestinal crypt epithelial lining cells. Scoring of whole tissue sections revealed higher values for the 51 SLE beluga, compared with the 20 Arctic and aquarium beluga (P = 0.003). The H-scoring system, applied to coded individual photomicrographs, confirmed that SLE beluga and CI beluga had levels of intestinal PAH-DNA adducts significantly higher than Arctic and aquarium beluga (P = 0.003 and 0.02, respectively). Furthermore, high levels of intestinal PAH-DNA adducts in four SLE beluga with gastrointestinal cancers, considered as a group, support a link of causality between PAH exposure and intestinal cancer in SLE beluga. Environ. Mol. Mutagen. 60:29-41, 2019. Published 2018. This article is a U.S. Government work and is in the public domain in the USA.

Effects of preparation on nutrient and environmental contaminant levels in Arctic beluga whale (Delphinapterus leucas) traditional foods.

For Canadian Arctic indigenous populations, marine mammal (MM) traditional foods (TFs) represent sources of both important nutrients and hazardous environmental contaminants. Food preparation is known to impact the nutrient and environmental contaminant content of processed items, yet the impacts of preparation on indigenous Arctic MM TFs remain poorly characterized. In order to determine how the various processes involved in preparing beluga blubber TFs affect their levels of nutrients and environmental contaminants, we collected blubber samples from 2 male beluga whales, aged 24 and 37 years, captured during the 2014 summer hunting season in Tuktoyaktuk, Northwest Territories, and processed them according to local TF preparation methods. We measured the levels of select nutrients [selenium (Se), polyunsaturated fatty acids (PUFAs)] and contaminants [organochlorine pesticides, perfluoroalkyl and polyfluoroalkyl substances (PFASs), polybrominated diphenyl ethers, polychlorinated biphenyls, polycyclic aromatic hydrocarbons (PAHs), mercury (Hg)] in raw and prepared (boiled, roasted, aged) beluga blubber TFs. The impacts of beluga blubber TF preparation methods on nutrient and environmental contaminant levels were inconsistent, as the majority of processes either did not appear to influence concentrations or affected the two belugas differently. However, roasting and ageing beluga blubber consistently impacted certain compounds: roasting blubber increased concentrations of hydrophilic substances (Se and certain PFASs) through solvent depletion and deposited PAHs from cookfire smoke. The solid-liquid phase separation involved in ageing blubber depleted hydrophilic elements (Se, Hg) and some ionogenic PFASs from the lipid-rich liquid oil phase, while PUFA levels appeared to increase, and hydrophobic persistent organic pollutants were retained. Ageing blubber adjacent to in-use smokehouses also resulted in considerable PAH deposition to processed samples. Our findings demonstrated that contaminant concentration differences were greater between the two sets of whale samples, based on age differences, than they were within each set of whale samples, due to variable preparation methods. When considering means to minimize human contaminant exposure while maximizing nutrient intake, consumption of aged liquid from younger male whales would be preferred, based on possible PUFA enhancement and selective depletion of hydrophilic environmental contaminants in this food item.

Latitudinal variation in ecological opportunity and intraspecific competition indicates differences in niche variability and diet specialization of Arctic marine predators.

Individual specialization (IS), where individuals within populations irrespective of age, sex, and body size are either specialized or generalized in terms of resource use, has implications on ecological niches and food web structure. Niche size and degree of IS of near-top trophic-level marine predators have been little studied in polar regions or with latitude. We quantified the large-scale latitudinal variation of population- and individual-level niche size and IS in ringed seals (Pusa hispida) and beluga whales (Delphinapterus leucas) using stable carbon and nitrogen isotope analysis on 379 paired ringed seal liver and muscle samples and 124 paired beluga skin and muscle samples from eight locations ranging from the low to high Arctic. We characterized both within- and between-individual variation in predator niche size at each location as well as accounting for spatial differences in the isotopic ranges of potential prey. Total isotopic niche width (TINW) for populations of ringed seals and beluga decreased with increasing latitude. Higher TINW values were associated with greater ecological opportunity (i.e., prey diversity) in the prey fish community which mainly consists of Capelin (Mallotus villosus) and Sand lance (Ammodytes sp.) at lower latitudes and Arctic cod (Boreogadus saida) at high latitudes. In beluga, their dietary consistency between tissues also known as the within-individual component (WIC) increased in a near 1:1 ratio with TINW (slope = 0.84), suggesting dietary generalization, whereas the slope (0.18) of WIC relative to TINW in ringed seals indicated a high degree of individual specialization in ringed seal populations with higher TINWs. Our findings highlight the differences in TINW and level of IS for ringed seals and beluga relative to latitude as a likely response to large-scale spatial variation in ecological opportunity, suggesting species-specific variation in dietary plasticity to spatial differences in prey resources and environmental conditions in a rapidly changing ecosystem.

Recent progress on our understanding of the biological effects of mercury in fish and wildlife in the Canadian Arctic.

This review summarizes our current state of knowledge regarding the potential biological effects of mercury (Hg) exposure on fish and wildlife in the Canadian Arctic. Although Hg in most freshwater fish from northern Canada was not sufficiently elevated to be of concern, a few lakes in the Northwest Territories and Nunavut contained fish of certain species (e.g. northern pike, Arctic char) whose muscle Hg concentrations exceeded an estimated threshold range (0.5-1.0 µg g(-1) wet weight) within which adverse biological effects begin to occur. Marine fish species generally had substantially lower Hg concentrations than freshwater fish; but the Greenland shark, a long-lived predatory species, had mean muscle Hg concentrations exceeding the threshold range for possible effects on health or reproduction. An examination of recent egg Hg concentrations for marine birds from the Canadian Arctic indicated that mean Hg concentration in ivory gulls from Seymour Island fell within the threshold range associated with adverse effects on reproduction in birds. Mercury concentrations in brain tissue of beluga whales and polar bears were generally lower than levels associated with neurotoxicity in mammals, but were sometimes high enough to cause subtle neurochemical changes that can precede overt neurotoxicity. Harbour seals from western Hudson Bay had elevated mean liver Hg concentrations along with comparatively high muscle Hg concentrations indicating potential health effects from methylmercury (MeHg) exposure on this subpopulation. Because current information is generally insufficient to determine with confidence whether Hg exposure is impacting the health of specific fish or wildlife populations in the Canadian Arctic, biological effects studies should comprise a major focus of future Hg research in the Canadian Arctic. Additionally, studies on cellular interactions between Hg and selenium (Se) are required to better account for potential protective effects of Se on Hg toxicity, especially in large predatory Arctic fish, birds, and mammals.

Mercury in the marine environment of the Canadian Arctic: review of recent findings.

This review summarizes data and information which have been generated on mercury (Hg) in the marine environment of the Canadian Arctic since the previous Canadian Arctic Contaminants Assessment Report (CACAR) was released in 2003. Much new information has been collected on Hg concentrations in marine water, snow and ice in the Canadian Arctic. The first measurements of methylation rates in Arctic seawater indicate that the water column is an important site for Hg methylation. Arctic marine waters were also found to be a substantial source of gaseous Hg to the atmosphere during the ice-free season. High Hg concentrations have been found in marine snow as a result of deposition following atmospheric mercury depletion events, although much of this Hg is photoreduced and re-emitted back to the atmosphere. The most extensive sampling of marine sediments in the Canadian Arctic was carried out in Hudson Bay where sediment total Hg (THg) concentrations were low compared with other marine regions in the circumpolar Arctic. Mass balance models have been developed to provide quantitative estimates of THg fluxes into and out of the Arctic Ocean and Hudson Bay. Several recent studies on Hg biomagnification have improved our understanding of trophic transfer of Hg through marine food webs. Over the past several decades, Hg concentrations have increased in some marine biota, while other populations showed no temporal change. Marine biota also exhibited considerable geographic variation in Hg concentrations with ringed seals, beluga and polar bears from the Beaufort Sea region having higher Hg concentrations compared with other parts of the Canadian Arctic. The drivers of these variable patterns of Hg bioaccumulation, both regionally and temporally, within the Canadian Arctic remain unclear. Further research is needed to identify the underlying processes including the interplay between biogeochemical and food web processes and climate change.

PCBs are associated with altered gene transcript profiles in arctic Beluga Whales (Delphinapterus leucas).

High trophic level arctic beluga whales (Delphinapterus leucas) are exposed to persistent organic pollutants (POP) originating primarily from southern latitudes. We collected samples from 43 male beluga harvested by Inuvialuit hunters (2008-2010) in the Beaufort Sea to evaluate the effects of POPs on the levels of 13 health-related gene transcripts using quantitative real-time polymerase chain reaction. Consistent with their role in detoxification, the aryl hydrocarbon receptor (Ahr) (r(2) = 0.18, p = 0.045 for 2008 and 2009) and cytochrome P450 1A1 (Cyp1a1) (r(2) = 0.20, p < 0.001 for 2008 and 2009; r(2) = 0.43, p = 0.049 for 2010) transcripts were positively correlated with polychlorinated biphenyls (PCBs), the dominant POP in beluga. Principal Components Analysis distinguished between these two toxicology genes and 11 other genes primarily involved in growth, metabolism, and development. Factor 1 explained 56% of gene profiles, with these latter 11 gene transcripts displaying greater abundance in years coinciding with periods of low sea ice extent (2008 and 2010). δ(13)C results suggested a shift in feeding ecology and/or change in condition of these ice edge-associated beluga whales during these two years. While this provides insight into the legacy of PCBs in a remote environment, the possible impacts of a changing ice climate on the health of beluga underscores the need for long-term studies.

Vitamin A and E profiles as biomarkers of PCB exposure in beluga whales (Delphinapterus leucas) from the western Canadian Arctic.

We evaluated the utility of vitamin A and E profiles as biomarkers of contaminant exposure in beluga whales (Delphinapterus leucas; n=66) harvested by the Inuvialuit in the Beaufort Sea. Blubber was an important repository for these vitamins, accounting for 76.8±2.6% of the total body store of vitamin A, and 98.5±0.4% of total vitamin E. While the free alcohol form of vitamin A (retinol) appeared highly regulated, the vitamin A esters were influenced by several biological factors including age, body condition and length. Vitamin E concentrations in liver and blubber were related to age, condition, length and feeding ecology, as described δ(15)N and δ(13)C. Despite the influence of these factors, collective results from univariate statistics, best fit multiple regressions, and principal component analysis (PCA) identified polychlorinated biphenyls (PCBs) as important determinants of vitamin concentrations and profiles in beluga tissues. Blubber PCB concentrations best explained variation of the first principal component in a PCA of hepatic vitamins (r(2)=0.13, p=0.014), and regression models found that vitamin A concentrations were negatively correlated with PCB levels in liver (esters: r(2)=0.19, p=0.001), but positively in plasma (retinol: r(2)=0.20, p=0.06) and blubber (retinol: r(2)=0.22, p=0.001, esters: r(2)=0.43, p<0.001). Our analyses provide a basis to propose an integrated toxicity reference value for disruption of vitamin A and E profiles in beluga of 1.6 mg/kg lw PCBs. This disruption of vitamin profiles by moderate levels of PCBs in an arctic cetacean highlights the global reach and impact of these legacy chemicals decades after their peak use.

Metabolic transformation shapes polychlorinated biphenyl and polybrominated diphenyl ether patterns in beluga whales (Delphinapterus leucas).

While the accumulation of persistent contaminants in marine mammals can be attributed directly to their prey, the role of metabolism in shaping patterns is often overlooked. In the present study, the authors investigated the role of metabolic transformation in influencing polychlorinated biphenyl (PCB) and polybrominated diphenyl ether (PBDE) patterns in offshore and nearshore groups of beluga whales (Delphinapterus leucas) and their prey. Congener profiles and principal components analysis (PCA) revealed similar PCB and PBDE patterns in beluga whales feeding either offshore or nearshore, despite divergent contaminant patterns in the putative prey of these two feeding groups. The clustering of PCBs into metabolically derived structure-activity groups (SAGs) and the separation of metabolizable and recalcitrant groups along principal component 1 of the PCA revealed the important role of metabolic transformation in shaping PCB patterns in beluga. Lack of metabolism for congeners with high ortho-chlorine content was revealed by metabolic slopes equal to or greater than 1.0. Metabolic slopes for all other SAGs were less than 1.0 (p<0.001), suggesting metabolism of congeners with ortho-meta and meta-para vicinal hydrogens via induction of cytochrome P450 enzymes (CYP1A/2B/3A). Metabolic indices less than 1.0 for PBDEs (p<0.001) suggested that beluga metabolized these poorly understood flame retardants. The strikingly similar PCB patterns in a captive beluga and free-ranging beluga from the Beaufort Sea provide additional evidence that metabolic transformation is a dominant driver of contaminant patterns in beluga.