Mercury in freshwater ecosystems of the Canadian Arctic: recent advances on its cycling and fate.

The Canadian Arctic has vast freshwater resources, and fish are important in the diet of many Northerners. Mercury is a contaminant of concern because of its potential toxicity and elevated bioaccumulation in some fish populations. Over the last decade, significant advances have been made in characterizing the cycling and fate of mercury in these freshwater environments. Large amounts of new data on concentrations, speciation and fluxes of Hg are provided and summarized for water and sediment, which were virtually absent for the Canadian Arctic a decade ago. The biogeochemical processes that control the speciation of mercury remain poorly resolved, including the sites and controls of methylmercury production. Food web studies have examined the roles of Hg uptake, trophic transfer, and diet for Hg bioaccumulation in fish, and, in particular, advances have been made in identifying determinants of mercury levels in lake-dwelling and sea-run forms of Arctic char. In a comparison of common freshwater fish species that were sampled across the Canadian Arctic between 2002 and 2009, no geographic patterns or regional hotspots were evident. Over the last two to four decades, Hg concentrations have increased in some monitored populations of fish in the Mackenzie River Basin while other populations from the Yukon and Nunavut showed no change or a slight decline. The different Hg trends indicate that the drivers of temporal change may be regional or habitat-specific. The Canadian Arctic is undergoing profound environmental change, and preliminary evidence suggests that it may be impacting the cycling and bioaccumulation of mercury. Further research is needed to investigate climate change impacts on the Hg cycle as well as biogeochemical controls of methylmercury production and the processes leading to increasing Hg levels in some fish populations in the Canadian Arctic.

Quantifying Hg within ectomycorrhizal fruiting bodies, from emergence to senescence.

Ectomycorrhizal fruiting bodies (basidiomata) collected from forested areas in southwestern New Brunswick were analyzed for total mercury, sulphur, nitrogen, and carbon concentrations (THg, TS, TN, and TC, respectively). This analysis was done for caps and stalks and by development stage (emergent, mature, senescent) across 27 species associated with five classes, eight families, and 13 genera. Across the species, THg correlated positively with TN and TS, thereby implying N as well as S mitigated transfer of Hg from the mycelia into the basidiomata, with THg ranging from 3 to 10 457 ppb. TS, TN, and TC varied from 0.07 to 1, 1 to 11, and 43 to 53 %, respectively. Cap and stalk THg, TS, TN, and TC were also correlated to one another, with mean stalk/cap ratios of 0.59, 0.76, 0.71, and 0.98, respectively. Soil availability indexed by THg, TS, TN, and TC within the forest floor contributed to basidiomatal THg as well. THg, THg/TS, and THg/N varied strongly by species. These variations involved: (i) no growth dilution and no volatilization (Group I), (ii) growth dilution only (Group II), (iii) growth dilution followed by loss during senescence (Group III), and (iv) growth dilution combined with loss from emergence onward (Group IV). Depending on species, TN and TS remained the same or declined from 100 % at emergence to about 80 and 70 % at senescence. Lack of THg decline for the Group I species would be due to HgS encapsulation. Reanalyzing the freeze-dried samples revealed that THg continued to drop during the first year of air-dry storage for the Group II, II, and IV species, but TS, TN, and TC remained stable. The results were quantified by way of best-fitted regression models.

Factors affecting water strider (Hemiptera: Gerridae) mercury concentrations in lotic systems.

Water striders (Hemiptera: Gerridae) have been considered as a potential sentinel for mercury (Hg) contamination of freshwater ecosystems, yet little is known about factors that control Hg concentrations in this invertebrate. Striders were collected from 80 streams and rivers in New Brunswick, Canada, in August and September of 2004 through 2007 to assess the influence of factors such as diet, water chemistry, and proximity to point sources on Hg concentrations in this organism. Higher than average Hg concentrations were observed in the southwest and Grand Lake regions of the province, the latter being the location of a coal-fired power plant that is a source of Hg (approximately 100 kg annually), with elevated Hg concentrations in the lichen Old Man's Beard (Usnea spp.) in its immediate vicinity. Across all streams, pH and total organic carbon of water were relatively weak predictors of strider Hg concentrations. Female striders that were larger in body size than males had significantly lower Hg concentrations within sites, suggestive of growth dilution. There was no relationship between percent aquatic carbon in the diet and Hg concentrations in striders. For those striders feeding solely on terrestrial carbon, Hg concentrations were higher in animals occupying a higher trophic level. Mercury concentrations were highly variable in striders collected monthly over two growing seasons, suggesting short-term changes in Hg availability. These measurements highlight the importance of considering both deposition and postdepositional processes in assessing Hg bioaccumulation in this species. They also suggest that striders may be more appropriate as a terrestrial rather than an aquatic Hg sentinel, underscoring the importance of understanding the origin of food for organisms used in contaminant studies.

New evidence on variations of human body burden of methylmercury from fish consumption.

Epidemiologic studies commonly use mercury (Hg) level in hair as a valid proxy to estimate human exposure to methylmercury (MeHg) through fish consumption. This study presents the results yielded by a complete data set on fish consumption habits, Hg levels in edible fish resources, and corresponding Hg accumulation in hair, gathered in three distinct communities of eastern Canada. For one of these communities, the average hair Hg concentration was 14 times less than the expected value based on calculated daily oral exposure and current knowledge of MeHg metabolism. This finding could be explained by differences in specific genetic characteristics and/or interactive effects of other dietary components.

Sulphate, nitrogen and base cation budgets at 21 forested catchments in Canada, the United States and Europe.

To assess the concern over declining base cation levels in forest soils caused by acid deposition, input-output budgets (1990s average) for sulphate (SO(4)), inorganic nitrogen (NO(3)-N; NH(4)-N), calcium (Ca), magnesium (Mg) and potassium (K) were synthesised for 21 forested catchments from 17 regions in Canada, the United States and Europe. Trend analysis was conducted on monthly ion concentrations in deposition and runoff when more than 9 years of data were available (14 regions, 17 sites). Annual average SO(4) deposition during the 1990s ranged between 7.3 and 28.4 kg ha(-1) per year, and inorganic nitrogen (N) deposition was between 2.8 and 13.8 kg ha(-1) per year, of which 41-67% was nitrate (NO(3)-N). Over the period of record, SO(4) concentration in deposition decreased in 13/14 (13 out of 14 total) regions and SO(4) in runoff decreased at 14/17 catchments. In contrast, NO(3)-N concentrations in deposition decreased in only 1/14 regions, while NH(4)-N concentration patterns varied; increasing at 3/14 regions and decreasing at 2/14 regions. Nitrate concentrations in runoff decreased at 4/17 catchments and increased at only 1 site, whereas runoff levels of NH(4)-N increased at 5/17 catchments. Decreasing trends in deposition were also recorded for Ca, Mg, and K at many of the catchments and on an equivalent basis, accounted for up to 131% (median 22%) of the decrease in acid anion deposition. Base cation concentrations in streams generally declined over time, with significant decreases in Ca, Mg and K occurring at 8, 9 and 7 of 17 sites respectively, which accounted for up to 133% (median 48%) of the decrease in acid anion concentration. Sulphate export exceeded input at 18/21 catchments, likely due to dry deposition and/or internal sources. The majority of N in deposition (31-100%; median 94%) was retained in the catchments, although there was a tendency for greater NO(3)-N leaching at sites receiving higher (<7 kg ha(-1) per year) bulk inorganic N deposition. Mass balance calculations show that export of Ca and Mg in runoff exceeds input at all 21 catchments, but K export only exceeds input at 16/21 sites. Estimates of base cation weathering were available for 18 sites. When included in the mass balance calculation, Ca, Mg and K exports exceeded inputs at 14, 10 and 2 sites respectively. Annual Ca and Mg losses represent appreciable proportions of the current exchangeable soil Ca and Mg pools, although losses at some of the sites likely occur from weathering reactions beneath the rooting zone and there is considerable uncertainty associated with mineral weathering estimates. Critical loads for sulphur (S) and N, using a critical base cation to aluminium ratio of 10 in soil solution, are currently exceeded at 7 of the 18 sites with base cation weathering estimates. Despite reductions in SO(4) and H(+) deposition, mass balance estimates indicate that acid deposition continues to acidify soils in many regions with losses of Ca and Mg of primary concern.

Mercury exposure in two coastal communities of the Bay of Fundy, Canada.

There is a rising global concern with regard to mercury (Hg) exposure among coastal populations. Two communities on the Bay of Fundy (New Brunswick, Canada) were assessed by hair monitoring and dietary methods. Average concentration of total Hg in hair was 0.70+/-0.55 mg/kg (N=91) at Grand Manan and 0.42+/-0.15 mg/kg (N=52) at St. Andrews/St. Stephen. Average daily consumption of fresh fish and shellfish was 50+/-40 g/day for Grand Manan and 19+/-19 g/day for St. Andrews/St. Stephen. Average daily total Hg intake estimated from the food frequency and 24-h recall questionnaires was 0.05+/-0.04 microg Hg/kg bw/day at Grand Manan and 0.03+/-0.04 microg Hg/kg bw/day at St. Andrews/St. Stephen. A significant correlation (r=0.47, P=0.002) between Hg intake and hair was observed for Grand Manan. Low Hg intakes and body burden can be attributed to the low Hg levels found in the species commonly consumed: haddock, canned tuna, lobster, and pollock (all below 0.2 microg/g wet weight). The results showed that Hg exposure in these Canadian coastal communities is low; fish with higher levels of Hg (shark, tuna, swordfish, pickerel, and bass) are not consumed locally.

Water striders (family Gerridae): mercury sentinels in small freshwater ecosystems.

To circumvent some of the previous limitations associated with contaminant-monitoring programs, we tested the suitability of the water strider (Hemiptera: Gerridae) as a mercury sentinel by comparing total mercury concentrations in water striders and brook trout (Salvelinus fontinalis) from a variety of stream sites in New Brunswick, Canada. There was a strong association between the two variables across sites (r(2)=0.81, P<0.001) in systems where both atmospheric deposition and a point source (an abandoned gold mine) were likely contributing to ambient mercury levels. In a small stream draining the gold mine tailings pile, water striders had mercury concentrations an order of magnitude higher than those from reference locations. Temporal variation at three southern New Brunswick stream sites was non-significant. These results suggest that water strider mercury levels accurately quantify food chain entry of the element. The use of sentinel species holds great potential for expanding contaminant-monitoring programs.