Stable Isotope analysis (SIA) is an ecological tool to help determine diet. The lipid content of ... more Stable Isotope analysis (SIA) is an ecological tool to help determine diet. The lipid content of animal tissues varies with time, individual and tissue. Lipids are depleted in 13C relative to carbohydrates and proteins. As a consequence, lipids are often removed from tissue samples before running SIA, to prevent introducing an ecological bias in the carbon stable isotope ratio. Chloroform/methanol is the most commonly used solvent due to its efficiency in removing lipids present in tissues. Non-lipid material (like membrane proteins bonded with lipids) extracted with the lipids by this solvent is poorly addressed in the literature. In addition, the effect of extracting non-lipid material on nitrogen stable isotope ratios is not clear but has the potential to be ecologically important. Other solvents are available to remove lipids from tissues, like petroleum ether or ethyl acetate. We quantified and qualified the effects of these different solvents on nitrogen and carbon stable isot...
Recent studies have shown that climate change is already having significant impacts on many aspec... more 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.
The Science of the total environment, Jan 14, 2014
This review summarizes our current state of knowledge regarding the potential biological effects ... more 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 (0.5-1.0μgg(-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 r...
Mercury is present at elevated levels in the top predators living in High Arctic ecosystems. Beca... more Mercury is present at elevated levels in the top predators living in High Arctic ecosystems. Because only methylmercury (MeHg) bioaccumulates in food chains, the sources need to be identified. In temperate environments, wetlands are considered to be the principal sources of MeHg, with sulfate-reducing bacteria (SRB) thought to be responsible. The present study investigated whether High Arctic wetlands produced MeHg and whether SRB were involved in MeHg formation. Frozen soil was collected from 18 High Arctic wetlands before ground thaw, and when analyzed for MeHg, values were low, averaging 0.065 ng/g. When soils were incubated for 30 and 60 d at typical summer Arctic soil temperatures (4 degrees C and 8 degrees C), MeHg increased up to 100-fold. These laboratory observations were consistent with field measurements of wetland surface water, where MeHg concentrations increased from near detection limits (0.02 ng/L) at the inflow to an average of 1.21 ng/L at the outflow. Both laboratory and field data showed MeHg production in High Arctic wetlands. The prevalence of SRB in soil was low, however, and DNA analysis of the dissimilatory sulfate-reductase gene specific to SRB was positive at only one site. The present study showed that wetlands in the High Arctic can produce MeHg but that SRB may not the dominant mercury methylators.
The production of dissolved gaseous mercury (DGM) in freshwater lakes is induced by solar radiati... more The production of dissolved gaseous mercury (DGM) in freshwater lakes is induced by solar radiation and is also thought to be linked to processes mediated by dissolved organic carbon (DOC). Studies investigating these processes using comparisons between lakes are often confounded by differences in DOC content and structure. In this study, we investigated the link between DOC concentrations and DGM production by using tangential ultrafiltration to manipulate DOC concentrations in water samples taken from a given lake. In this way, a range of samples with different DOC concentrations was produced without substantial changes to DOC structure or dissolved ions. This was repeated for four lakes in central Quebec: two with highly logged drainage basins and two with minimally logged drainage basins. On two separate days for each lake, water samples (filtered to remove >99% of microorganisms) with varying DOC concentrations were incubated in clear and dark Teflon bottles on the lake surface. DGM concentrations were measured at 3.5-h intervals over the course of 10.5 h. Levels of DGM concentrations increased with increasing cumulative irradiation for all lakes until approximately 4000 kJ m(-2) (400-750 nm, photosynthetically active radiation (PAR)), when DGM concentrations reached a plateau (between 20 and 200 pg L(-1)). When we assumed that DGM production was limited by the amount of photoreducible mercury, reversible first-order reaction kinetics fitted the observed data well (r2 ranging between 0.59 and 0.98, p < 0.05 with the exception of N70 100% DOC, 0% DOC, and K2 0% DOC with p = 0.06, 0.10, and 0.11, respectively). The DGM plateaus were independent of DOC concentrations but differed between lakes. In contrast, photoproduction efficiency (DGMprod) (i.e., the amount of DGM produced per unit radiation (fg L(-1) (kJ/m2)(-1)) below 4000 kJ m(-2) PAR) was linearly proportional to DOC concentration for both logged lakes (r2 = 0.97, p < 0.01) and nonlogged lakes (r2 = 0.52, p = 0.018) studied. Furthermore, logged lakes had a lower DGMprod per unit DOC (p < 0.01) than the nonlogged lakes. In these four lakes, the rate of DGM production per unit PAR was dependent on the concentration of DOC. The DGM plateau was independent of DOC concentration; however, there was a significant difference in DGM plateaus between lakes presumably due to different DOC structures and dissolved ions. This research demonstrates an important mechanism by which logging may exacerbate mercury levels in biota.
The trophodynamics of per- and polyfluorinated compounds and bromine-based flame retardants were ... more The trophodynamics of per- and polyfluorinated compounds and bromine-based flame retardants were examined in components of a marine food web from the western Canadian Arctic. The animals studied and their relative trophic status in the food web, established using stable isotopes of nitrogen (delta15N), were beluga (Delphinapterus leucas) > ringed seal (Phoca hispida) > Arctic cod (Boreogadus saida) > Pacific herring (Clupea pallasi) approximately equal to Arctic cisco (Coregonus autumnalis) > pelagic amphipod (Themisto libellula) > Arctic copepod (Calanus hyperboreus). For the brominated diphenyl ethers, the lipid adjusted concentrations of the seven congeners analyzed (Sigma7BDEs: -47, -85, -99, -100, -153, -154, and -209) ranged from 205.4 +/- 52.7 ng/g in Arctic cod to 2.6 +/- 0.4 ng/g in ringed seals. Mean Sigma7BDEs concentrations in Arctic copepods, 16.4 ng/g (n = 2, composite sample), were greater than those in the top trophic level (TL) marine mammals and suggests that (i) Arctic copepods are an important dietary component that delivers BDEs to the food web and (ii) because these compounds are bioaccumulative, metabolism and depletion of BDE congeners in top TL mammals is an important biological process. There were differences in the concentration profiles of the isomers of hexabromocyclododecane (HBCD) in the food web. The most notable difference was observed for beluga, where the alpha-isomer was enriched (accounting for approximately 90% of the SigmaHBCD body burden), relative to its primary prey species, Arctic cod, where the alpha-isomer accounted for only 20% of the SigmaHBCD body burden (beta: 4% and gamma: 78%). For the C8-C11 perfluorinated carboxylic acids, the trophic magnification factors (TMFs) were all greater than unity and increased with increasing carbon chain length. PFOS and its neutral precursor, PFOSA, also had TMF values greater than one. There were also pronounced differences in the PFOSA to PFOS ratio in ringed seal (0.04) and in beluga (1.4) and suggests that, in part, there are differences in the efficacy of biotransforming PFOSA by whale and seal top predators that both preferentially feed on Arctic cod.
Stable Isotope analysis (SIA) is an ecological tool to help determine diet. The lipid content of ... more Stable Isotope analysis (SIA) is an ecological tool to help determine diet. The lipid content of animal tissues varies with time, individual and tissue. Lipids are depleted in 13C relative to carbohydrates and proteins. As a consequence, lipids are often removed from tissue samples before running SIA, to prevent introducing an ecological bias in the carbon stable isotope ratio. Chloroform/methanol is the most commonly used solvent due to its efficiency in removing lipids present in tissues. Non-lipid material (like membrane proteins bonded with lipids) extracted with the lipids by this solvent is poorly addressed in the literature. In addition, the effect of extracting non-lipid material on nitrogen stable isotope ratios is not clear but has the potential to be ecologically important. Other solvents are available to remove lipids from tissues, like petroleum ether or ethyl acetate. We quantified and qualified the effects of these different solvents on nitrogen and carbon stable isot...
Recent studies have shown that climate change is already having significant impacts on many aspec... more 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.
The Science of the total environment, Jan 14, 2014
This review summarizes our current state of knowledge regarding the potential biological effects ... more 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 (0.5-1.0μgg(-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 r...
Mercury is present at elevated levels in the top predators living in High Arctic ecosystems. Beca... more Mercury is present at elevated levels in the top predators living in High Arctic ecosystems. Because only methylmercury (MeHg) bioaccumulates in food chains, the sources need to be identified. In temperate environments, wetlands are considered to be the principal sources of MeHg, with sulfate-reducing bacteria (SRB) thought to be responsible. The present study investigated whether High Arctic wetlands produced MeHg and whether SRB were involved in MeHg formation. Frozen soil was collected from 18 High Arctic wetlands before ground thaw, and when analyzed for MeHg, values were low, averaging 0.065 ng/g. When soils were incubated for 30 and 60 d at typical summer Arctic soil temperatures (4 degrees C and 8 degrees C), MeHg increased up to 100-fold. These laboratory observations were consistent with field measurements of wetland surface water, where MeHg concentrations increased from near detection limits (0.02 ng/L) at the inflow to an average of 1.21 ng/L at the outflow. Both laboratory and field data showed MeHg production in High Arctic wetlands. The prevalence of SRB in soil was low, however, and DNA analysis of the dissimilatory sulfate-reductase gene specific to SRB was positive at only one site. The present study showed that wetlands in the High Arctic can produce MeHg but that SRB may not the dominant mercury methylators.
The production of dissolved gaseous mercury (DGM) in freshwater lakes is induced by solar radiati... more The production of dissolved gaseous mercury (DGM) in freshwater lakes is induced by solar radiation and is also thought to be linked to processes mediated by dissolved organic carbon (DOC). Studies investigating these processes using comparisons between lakes are often confounded by differences in DOC content and structure. In this study, we investigated the link between DOC concentrations and DGM production by using tangential ultrafiltration to manipulate DOC concentrations in water samples taken from a given lake. In this way, a range of samples with different DOC concentrations was produced without substantial changes to DOC structure or dissolved ions. This was repeated for four lakes in central Quebec: two with highly logged drainage basins and two with minimally logged drainage basins. On two separate days for each lake, water samples (filtered to remove >99% of microorganisms) with varying DOC concentrations were incubated in clear and dark Teflon bottles on the lake surface. DGM concentrations were measured at 3.5-h intervals over the course of 10.5 h. Levels of DGM concentrations increased with increasing cumulative irradiation for all lakes until approximately 4000 kJ m(-2) (400-750 nm, photosynthetically active radiation (PAR)), when DGM concentrations reached a plateau (between 20 and 200 pg L(-1)). When we assumed that DGM production was limited by the amount of photoreducible mercury, reversible first-order reaction kinetics fitted the observed data well (r2 ranging between 0.59 and 0.98, p < 0.05 with the exception of N70 100% DOC, 0% DOC, and K2 0% DOC with p = 0.06, 0.10, and 0.11, respectively). The DGM plateaus were independent of DOC concentrations but differed between lakes. In contrast, photoproduction efficiency (DGMprod) (i.e., the amount of DGM produced per unit radiation (fg L(-1) (kJ/m2)(-1)) below 4000 kJ m(-2) PAR) was linearly proportional to DOC concentration for both logged lakes (r2 = 0.97, p < 0.01) and nonlogged lakes (r2 = 0.52, p = 0.018) studied. Furthermore, logged lakes had a lower DGMprod per unit DOC (p < 0.01) than the nonlogged lakes. In these four lakes, the rate of DGM production per unit PAR was dependent on the concentration of DOC. The DGM plateau was independent of DOC concentration; however, there was a significant difference in DGM plateaus between lakes presumably due to different DOC structures and dissolved ions. This research demonstrates an important mechanism by which logging may exacerbate mercury levels in biota.
The trophodynamics of per- and polyfluorinated compounds and bromine-based flame retardants were ... more The trophodynamics of per- and polyfluorinated compounds and bromine-based flame retardants were examined in components of a marine food web from the western Canadian Arctic. The animals studied and their relative trophic status in the food web, established using stable isotopes of nitrogen (delta15N), were beluga (Delphinapterus leucas) > ringed seal (Phoca hispida) > Arctic cod (Boreogadus saida) > Pacific herring (Clupea pallasi) approximately equal to Arctic cisco (Coregonus autumnalis) > pelagic amphipod (Themisto libellula) > Arctic copepod (Calanus hyperboreus). For the brominated diphenyl ethers, the lipid adjusted concentrations of the seven congeners analyzed (Sigma7BDEs: -47, -85, -99, -100, -153, -154, and -209) ranged from 205.4 +/- 52.7 ng/g in Arctic cod to 2.6 +/- 0.4 ng/g in ringed seals. Mean Sigma7BDEs concentrations in Arctic copepods, 16.4 ng/g (n = 2, composite sample), were greater than those in the top trophic level (TL) marine mammals and suggests that (i) Arctic copepods are an important dietary component that delivers BDEs to the food web and (ii) because these compounds are bioaccumulative, metabolism and depletion of BDE congeners in top TL mammals is an important biological process. There were differences in the concentration profiles of the isomers of hexabromocyclododecane (HBCD) in the food web. The most notable difference was observed for beluga, where the alpha-isomer was enriched (accounting for approximately 90% of the SigmaHBCD body burden), relative to its primary prey species, Arctic cod, where the alpha-isomer accounted for only 20% of the SigmaHBCD body burden (beta: 4% and gamma: 78%). For the C8-C11 perfluorinated carboxylic acids, the trophic magnification factors (TMFs) were all greater than unity and increased with increasing carbon chain length. PFOS and its neutral precursor, PFOSA, also had TMF values greater than one. There were also pronounced differences in the PFOSA to PFOS ratio in ringed seal (0.04) and in beluga (1.4) and suggests that, in part, there are differences in the efficacy of biotransforming PFOSA by whale and seal top predators that both preferentially feed on Arctic cod.
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