John Chételat

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 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.

Habitat-specific bioaccumulation of methylmercury in invertebrates of small mid-latitude lakes in North America

We examined habitat-specific bioaccumulation of methylmercury (MeHg) in aquatic food webs by comparing concentrations in pelagic zooplankton to those in littoral macroinvertebrates from 52 mid-latitude lakes in North America. Invertebrate MeHg concentrations were primarily correlated with water pH, and after controlling for this influence, pelagic zooplankton had significantly higher MeHg concentrations than littoral primary consumers but lower MeHg than littoral secondary consumers. Littoral primary consumers and pelagic zooplankton are two dominant prey for fish, and greater MeHg in zooplankton is likely sufficient to increase bioaccumulation in pelagic feeders. Intensive sampling of 8 lakes indicated that habitat-specific bioaccumulation in invertebrates (of similar trophic level) may result from spatial variation in aqueous MeHg concentration or from more efficient uptake of aqueous MeHg into the pelagic food web. Our findings demonstrate that littoral-pelagic differences in MeHg bioaccumulation are widespread in small mid-latitude lakes.

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.

Temporal variability of water chemistry in flowing waters of the northeastern United States: does river size matter?

The seasonal variability of discharge, water chemistry, suspended sediment, and suspended algal abundance was examined in temperate rivers of the northeastern United States to evaluate the accepted (but rarely tested) assumption that streams are more temporally variable than large rivers. Temporal variance of discharge and water-column characteristics was determined for 108 stations on 98 rivers with data measured between May to October of 1978 by the US National Stream Quality Accounting Network (NASQAN). Temporal variance of water-column characteristics increased in relation to the mean estimate of the variable (r2 = 0.69–0.93, p < 0.001) with the exception of pH (p > 0.05). River size, estimated by median discharge, had little effect (partial r2 = 0.01–0.02, p < 0.05) or no effect (p > 0.05) on the temporal variance of water-column characteristics after accounting for differences in the mean. In contrast, hydrological variability (measured by the coefficient of variation of daily discharge, flood frequency, number of months with floods) was negatively related with median discharge (r2 = 0.25–0.38, p < 0.001). When rivers were separated into regional drainage basins, hydrological variability was strongly related to median discharge in some regions (r2 = 0.45–0.76, p < 0.001) and not in others (p > 0.05). Temporal variance of water-column characteristics was not affected by river size within individual drainage basins. The intensity of upstream impoundment (measured by the number of impoundments and total impoundment storage volume) also negatively influenced the seasonal variability of discharge (r2 = 0.08–0.24, p < 0.01) but had little effect (partial r2 = 0.01–0.03, p < 0.05) or no effect (p > 0.05) on the temporal variance of water-column characteristics. Power functions are provided as guidelines for sampling design to estimate the number of samples required to obtain a mean with a given level of precision for each of the water-column characteristics. Nutrient status may be more important to consider than river size when determining sampling frequency for monitoring programs. On average, water chemistry is as variable in large rivers as in small ones.

Bioaccumulation and Trophic Transfer of Mercury and Selenium in African Sub-Tropical Fluvial Reservoirs Food Webs (Burkina Faso)

The bioaccumulation and biomagnification of mercury (Hg) and selenium (Se) were investigated in sub-tropical freshwater food webs from Burkina Faso, West Africa, a region where very few ecosystem studies on contaminants have been performed. During the 2010 rainy season, samples of water, sediment, fish, zooplankton, and mollusks were collected from three water reservoirs and analysed for total Hg (THg), methylmercury (MeHg), and total Se (TSe). Ratios of δ13C and δ15N were measured to determine food web structures and patterns of contaminant accumulation and transfer to fish. Food chain lengths (FCLs) were calculated using mean δ15N of all primary consumer taxa collected as the site-specific baseline. We report relatively low concentrations of THg and TSe in most fish. We also found in all studied reservoirs short food chain lengths, ranging from 3.3 to 3.7, with most fish relying on a mixture of pelagic and littoral sources for their diet. Mercury was biomagnified in fish food webs with an enrichment factor ranging from 2.9 to 6.5 for THg and from 2.9 to 6.6 for MeHg. However, there was no evidence of selenium biomagnification in these food webs. An inverse relationship was observed between adjusted δ15N and log-transformed Se:Hg ratios, indicating that Se has a lesser protective effect in top predators, which are also the most contaminated animals with respect to MeHg. Trophic position, carbon source, and fish total length were the factors best explaining Hg concentration in fish. In a broader comparison of our study sites with literature data for other African lakes, the THg biomagnification rate was positively correlated with FCL. We conclude that these reservoir systems from tropical Western Africa have low Hg biomagnification associated with short food chains. This finding may partly explain low concentrations of Hg commonly reported in fish from this area.

High Methylmercury in Arctic and Subarctic Ponds is Related to Nutrient Levels in the Warming Eastern Canadian Arctic.

Permafrost thaw ponds are ubiquitous in the eastern Canadian Arctic, yet little information exists on their potential as sources of methylmercury (MeHg) to freshwaters. They are microbially active and conducive to methylation of inorganic mercury, and are also affected by Arctic warming. This multiyear study investigated thaw ponds in a discontinuous permafrost region in the Subarctic taiga (Kuujjuarapik-Whapmagoostui, QC) and a continuous permafrost region in the Arctic tundra (Bylot Island, NU). MeHg concentrations in thaw ponds were well above levels measured in most freshwater ecosystems in the Canadian Arctic (>0.1 ng L(-1)). On Bylot, ice-wedge trough ponds showed significantly higher MeHg (0.3-2.2 ng L(-1)) than polygonal ponds (0.1-0.3 ng L(-1)) or lakes (<0.1 ng L(-1)). High MeHg was measured in the bottom waters of Subarctic thaw ponds near Kuujjuarapik (0.1-3.1 ng L(-1)). High water MeHg concentrations in thaw ponds were strongly correlated with variables associated with high inputs of organic matter (DOC, a320, Fe), nutrients (TP, TN), and microbial activity (dissolved CO2 and CH4). Thawing permafrost due to Arctic warming will continue to release nutrients and organic carbon into these systems and increase ponding in some regions, likely stimulating higher water concentrations of MeHg. Greater hydrological connectivity from permafrost thawing may potentially increase transport of MeHg from thaw ponds to neighboring aquatic ecosystems.

Mercury in the Canadian Arctic terrestrial environment : An Update

Contaminants in the Canadian Arctic have been studied over the last twenty years under the guidance of the Northern Contaminants Program. This paper provides the current state of knowledge on mercury (Hg) in the Canadian Arctic terrestrial environment. Snow, ice, and soils on land are key reservoirs for atmospheric deposition and can become sources of Hg through the melting of terrestrial ice and snow and via soil erosion. In the Canadian Arctic, new data have been collected for snow and ice that provide more information on the net accumulation and storage of Hg in the cryosphere. Concentrations of total Hg (THg) in terrestrial snow are highly variable but on average, relatively low (<5 ng L(-1)), and methylmercury (MeHg) levels in terrestrial snow are also generally low (<0.1 ng L(-1)). On average, THg concentrations in snow on Canadian Arctic glaciers are much lower than those reported on terrestrial lowlands or sea ice. Hg in snow may be affected by photochemical exchanges with the atmosphere mediated by marine aerosols and halogens, and by post-depositional redistribution within the snow pack. Regional accumulation rates of THg in Canadian Arctic glaciers varied little during the past century but show evidence of an increasing north-to-south gradient. Temporal trends of THg in glacier cores indicate an abrupt increase in the early 1990 s, possibly due to volcanic emissions, followed by more stable, but relatively elevated levels. Little information is available on Hg concentrations and processes in Arctic soils. Terrestrial Arctic wildlife typically have low levels of THg (<5 μg g(-1) dry weight) in their tissues, although caribou (Rangifer tarandus) can have higher Hg because they consume large amounts of lichen. THg concentrations in the Yukons Porcupine caribou herd vary among years but there has been no significant increase or decrease over the last two decades.

Temperature and the Sulfur Cycle Control Monomethylmercury Cycling in High Arctic Coastal Marine Sediments from Allen Bay, Nunavut, Canada

Monomethylmercury (MMHg) is a neurotoxin of concern in the Canadian Arctic due to its tendency to bioaccumulate and the importance of fish and wildlife in the Inuit diet. In lakes and wetlands, microbial sediment communities are integral to the cycling of MMHg; however, the role of Arctic marine sediments is poorly understood. With projected warming, the effect of temperature on the production and degradation of MMHg in Arctic environments also remains unclear. We examined MMHg dynamics across a temperature gradient (4, 12, 24 °C) in marine sediments collected in Allen Bay, Nunavut. Slurries were spiked with stable mercury isotopes and amended with specific microbial stimulants and inhibitors, and subsampled over 12 days. Maximal methylation and demethylation potentials were low, ranging from below detection to 1.13 pmol g(-1) h(-1) and 0.02 pmol g(-1) h(-1), respectively, suggesting that sediments are likely not an important source of MMHg to overlying water. Our results suggest that warming may result in an increase in Hg methylation - controlled by temperature-dependent sulfate reduction, without a compensatory increase in demethylation. This study highlights the need for further research into the role of high Arctic marine sediments and climate on the Arctic marine MMHg budget.

Carbon sources for lake food webs in the Canadian High Arctic and other regions of Arctic North America

We investigated the role of autochthonous and terrestrial carbon in supporting aquatic food webs in the Canadian High Arctic by determining the diet of the dominant primary consumer, aquatic chironomids. These organisms were studied in fresh waters on 3 islands of the Arctic Archipelago (~74–76°N) including barren polar desert watersheds and a polar oasis with lush meadows. Stomach content analysis of 578 larvae indicated that chironomids primarily ingested diatoms and sediment detritus with little variation among most genera. Carbon and nitrogen stable isotope mixing models applied to 2 lakes indicated that benthic algae contributed 68–95% to chironomid diet at a polar desert site and 70–78% at a polar oasis site. Detritus, originating from either phytoplankton or terrestrial sources, also contributed minor amounts to chironomid diet (0–32%). Radiocarbon measurements for the 2 lakes showed that old terrestrial carbon did not support chironomid production. Carbon stable isotope ratios of chironomids in other High Arctic lakes provided further dietary evidence that was consistent with mixing model results. These findings indicate that, in the Canadian High Arctic, chironomids (and fish that consume them) are supported primarily by benthic algae in both polar desert and oasis lakes. In contrast, our review of carbon flow studies for lakes in other Arctic regions of North America shows that terrestrial carbon and phytoplankton can be important energy sources for consumers. This study provides a baseline to detect future climate-related impacts on carbon pathways in High Arctic lakes.