Lisa L. Loseto

How does climate change influence arctic mercury

Recent studies have shown that climate change is already having significant impacts on many aspects of transport pathways, speciation and cycling of mercury within Arctic ecosystems. For example, the extensive loss of sea-ice in the Arctic Ocean and the concurrent shift from greater proportions of perennial to annual types have been shown to promote changes in primary productivity, shift foodweb structures, alter mercury methylation and demethylation rates, and influence mercury distribution and transport across the ocean-sea-ice-atmosphere interface (bottom-up processes). In addition, changes in animal social behavior associated with changing sea-ice regimes can affect dietary exposure to mercury (top-down processes). In this review, we address these and other possible ramifications of climate variability on mercury cycling, processes and exposure by applying recent literature to the following nine questions; 1) What impact has climate change had on Arctic physical characteristics and processes? 2) How do rising temperatures affect atmospheric mercury chemistry? 3) Will a decrease in sea-ice coverage have an impact on the amount of atmospheric mercury deposited to or emitted from the Arctic Ocean, and if so, how? 4) Does climate affect air-surface mercury flux, and riverine mercury fluxes, in Arctic freshwater and terrestrial systems, and if so, how? 5) How does climate change affect mercury methylation/demethylation in different compartments in the Arctic Ocean and freshwater systems? 6) How will climate change alter the structure and dynamics of freshwater food webs, and thereby affect the bioaccumulation of mercury? 7) How will climate change alter the structure and dynamics of marine food webs, and thereby affect the bioaccumulation of marine mercury? 8) What are the likely mercury emissions from melting glaciers and thawing permafrost under climate change scenarios? and 9) What can be learned from current mass balance inventories of mercury in the Arctic? The review finishes with several conclusions and recommendations.

Mercury in Arctic marine ecosystems: Sources, pathways and exposure

Mercury in the Arctic is an important environmental and human health issue. The reliance of Northern Peoples on traditional foods, such as marine mammals, for subsistence means that they are particularly at risk from mercury exposure. The cycling of mercury in Arctic marine systems is reviewed here, with emphasis placed on the key sources, pathways and processes which regulate mercury levels in marine food webs and ultimately the exposure of human populations to this contaminant. While many knowledge gaps exist limiting our ability to make strong conclusions, it appears that the long-range transport of mercury from Asian emissions is an important source of atmospheric Hg to the Arctic and that mercury methylation resulting in monomethylmercury production (an organic form of mercury which is both toxic and bioaccumulated) in Arctic marine waters is the principal source of mercury incorporated into food webs. Mercury concentrations in biological organisms have increased since the onset of the industrial age and are controlled by a combination of abiotic factors (e.g., monomethylmercury supply), food web dynamics and structure, and animal behavior (e.g., habitat selection and feeding behavior). Finally, although some Northern Peoples have high mercury concentrations of mercury in their blood and hair, harvesting and consuming traditional foods have many nutritional, social, cultural and physical health benefits which must be considered in risk management and communication.

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.

Transplacental transfer of polychlorinated biphenyls and polybrominated diphenyl ethers in arctic beluga whales (Delphinapterus leucas)

This study found that arctic beluga whales (Delphinapterus leucas) transferred, on average, 11.4% (7.5 mg) and 11.1% (0.1 mg) of their polychlorinated biphenyl (PCB) and polybrominated diphenyl ether (PBDE) blubber burden to their near-term fetuses. A single physicochemical parameter, log K(OW), largely explained this transplacental transfer for PCBs (r(2) =0.79, p < 0.00001) and PBDEs (r(2) = 0.37, p = 0.007), with congeners having a log K(OW) < 6.5 preferentially transferred to the fetus. Blubber concentrations of 257 ng/g lipid weight (lw) PCBs and 3.8 ng/g (lw) PBDEs in beluga fetuses highlights the exposure to endocrine-disrupting compounds during a critical developmental stage. The implications of detecting these levels of legacy PCBs and the flame retardant PBDEs in unborn arctic beluga are unclear.

Mercury toxicity in beluga whale lymphocytes: Limited effects of selenium protection

Increasing emissions of anthropogenic mercury represents a growing concern to the health of high trophic level marine mammals. In its organic form, this metal bioaccumulates, and can be toxic to several physiological endpoints, including the immune system. In this study, we (1) evaluated the effects of inorganic mercury (mercuric chloride, HgCl2) and organic mercury (methylmercuric chloride, MeHgCl) on the in vitro function of lymphocytes isolated from the peripheral blood of beluga whales (Delphinapterus leucas); (2) characterized the potential protective effects of sodium selenite (Na2SeO3) on cell proliferation of HgCl2 or MeHgCl-treated beluga whale lymphocytes; and (3) compared these dose-dependent effects to measurements of blood Hg in samples collected from traditionally harvested beluga whales in the western Canadian Arctic. Lymphocyte proliferative responses were reduced following exposure to 1 μM of HgCl2 and 0.33 μM of MeHgCl. Decreased intracellular thiol levels were observed at 10 μM of HgCl2 and 0.33 μM of MeHgCl. Metallothionein induction was noted at 0.33 μM of MeHgCl. Concurrent exposure of Se provided a degree of protection against the highest concentrations of inorganic Hg (3.33 and 10 μM) or organic Hg (10 μM) for T-lymphocytes. This in vitro protection of Se against Hg toxicity to lymphocytes may contribute to the in vivo protection in beluga whales exposed to high Hg concentrations. Current Hg levels in free-ranging beluga whales from the Arctic fall into the range of exposures which elicited effects on lymphocytes in our study, highlighting the potential for effects on host resistance to disease. The implications of a changing Arctic climate on Hg fate in beluga food webs and the consequences for the health of beluga whales remain pressing research needs.

Are Arctic Ocean ecosystems exceptionally vulnerable to global emissions of mercury? A call for emphasised research on methylation and the consequences of climate change.

Environmental context. Mercury is a global contaminant that has entered Arctic food webs in sufficient quantity to put at risk the health of top predators and humans that consume them. Recent research has discovered a photochemical process unique to the Arctic that leads to mercury deposition on frozen surfaces after polar sunrise, but the connection between mercury deposition and entry into food webs remains tenuous and poorly understood. We propose here that the Arctic Ocean’s sensitivity to the global mercury cycle depends far more on neglected post-deposition processes that lead to methylation within the ice–ocean system, and the vulnerability of these processes to changes occurring in the cryosphere. Abstract. Emissions, atmospheric transport and deposition have formed the emphasis of recent research to understand Hg trends in Arctic marine biota, with the expressed objective of predicting how biotic trends might respond to emission controls. To answer the question of whether the Arctic Ocean might be especially vulnerable to global mercury (Hg) contamination and how biota might respond to emission controls requires a distinction between the supply of Hg from source regions and the processes within the Arctic Ocean that sequester and convert mercury to monomethyl Hg (MeHg). Atmospheric Mercury Depletion Events (AMDEs) provide a unique Hg deposition process in the Arctic; however, AMDEs have yet to be linked quantitatively with Hg uptake in marine food webs. The difficulty in implicating AMDEs or emissions to biotic trends lie in the ocean where several poorly understood processes lead to MeHg production and biomagnification. We propose that sensitivity of the Arctic Ocean’s ecosystem to Hg lies not so much in the deposition process as in methylation processes within the ocean, Hg inputs from large drainage basins, and the vulnerability these to climate change. Future research needs to be better balanced across the entire Hg cycle.

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.

Importance of Eating Capelin: Unique Dietary Habits of Hudson Bay Beluga

Beluga whales (Delphinapterus leucas) fill an important ecological and economic role in Hudson Bay. However, little is known about their diet and a better understanding of beluga populations is required. Though Arctic cod (Boreogadus saida) are important forage fish species for many circumpolar marine predators, beluga are opportunistic feeders and may feed on a variety of prey items. Here, we compare the fatty acid profile of two key forage fish, Arctic cod and capelin (Mallotus villosus), to determine the relative importance of each species to the diets of beluga during the 1980s in three Canadian Eastern Arctic beluga populations: Western Hudson Bay, Cumberland Sound, and the High Arctic. First, we compared the two prey species using a Principle Component Analysis (PCA) to determine the fatty acids that best described each species. Five fatty acids dominated the Arctic cod profile (the 20 and 22 carbon length monounsaturates 20:1n7, 20:1n9, 22:1n9, 22:1n11, 22:1n7), and five fatty acids were representative of the capelin profile (18:2n6, 16, 22:6n3, 22:5n6, and 20:4n6). The levels of these ten fatty acids were significantly different between the two fish species. A discriminant function analysis followed by univariate tests, were performed on beluga fatty acid profiles to determine if populations could be differentiated. Results demonstrated significant differences among the three beluga populations. Finally, to examine the qualitative dietary importance of Arctic cod and capelin among the three beluga populations all fatty acid profiles were evaluated together with a PCA. We found the fatty acid profiles that segregated the Hudson Bay beluga population from others appeared to be associated with a capelin diet relative to the other beluga populations that appeared to feed more heavily on Arctic cod. The difference in fatty acid profiles and diet between the northern populations and the Hudson Bay population is discussed relative to possible environmental explanations.