Britt D. Hall

Food as the Dominant Pathway of Methylmercury Uptake by Fish

A field experiment was conducted to determine the degree to which fish accumulated methylmercury (MeHg) via their food or via passive uptake from water through the gills. Finescale dace (Phoxinus neogaeus) were held in 2000 L enclosed pens floating in an undisturbed, oligotrophic lake in northwestern Ontario. Fish were exposed to water containing either low (0.10–0.40 ng L-1), intermediate (0.45–1.30 ng L-1), or high (0.80–2.1 ng L-1) concentrations of MeHg. Zooplankton with either low (0.16–0.18 µg g-1 d.w.) or high (0.28–0.76 µg g-1 d.w.) concentrations of MeHg were added daily to each pen. Fish fed zooplankton with high concentrations of MeHg had significantly higher concentrations of mercury in muscle after 32 days than fish fed zooplankton with low concentrations of MeHg (ANCOVA, P<0.0001). Fish feeding on zooplankton with low concentrations of MeHg had the same amount of Hg in their tissues as fish at the start of the experiment. Uptake from water was at most 15%. This is the first experiment to confirm that food is the dominant pathway of MeHg bioaccumulation in fish at natural levels of MeHg.

Wetlands as principal zones of methylmercury production in southern Louisiana and the Gulf of Mexico region

It is widely recognized that wetlands, especially those rich in organic matter and receiving appreciable atmospheric mercury (Hg) inputs, are important sites of methylmercury (MeHg) production. Extensive wetlands in the southeastern United States have many ecosystem attributes ideal for promoting high MeHg production rates; however, relatively few mercury cycling studies have been conducted in these environments. We conducted a landscape scale study examining Hg cycling in coastal Louisiana (USA) including four field trips conducted between August 2003 and May 2005. Sites were chosen to represent different ecosystem types, including: a large shallow eutrophic estuarine lake (Lake Pontchartrain), three rivers draining into the lake, a cypress-tupelo dominated freshwater swamp, and six emergent marshes ranging from a freshwater marsh dominated by Panicum hemitomon to a Spartina alterniflora dominated salt marsh close to the Gulf of Mexico. We measured MeHg and total Hg (THg) concentrations, and ancillary chemical characteristics, in whole and filtered surface water, and filtered porewater. Overall, MeHg concentrations were greatest in surface water of freshwater wetlands and lowest in the profundal (non-vegetated) regions of the lake and river mainstems. Concentrations of THg and MeHg in filtered surface water were positively correlated with the highly reactive, aromatic (hydrophobic organic acid) fraction of dissolved organic carbon (DOC). These results suggest that DOC plays an important role in promoting the mobility, transport and bioavailability of inorganic Hg in these environments. Further, elevated porewater concentrations in marine and brackish wetlands suggest coastal wetlands along the Gulf Coast are key sites for MeHg production and may be a principal source of MeHg to foodwebs in the Gulf of Mexico. Examining the relationships among MeHg, THg, and DOC across these multiple landscape types is a first step in evaluating possible links between key zones for Hg(II)-methylation and the bioaccumulation of mercury in the biota inhabiting the Gulf of Mexico region.

Impacts of Reservoir Creation on the Biogeochemical Cycling of Methyl Mercury and Total Mercury in Boreal Upland Forests

The FLooded Upland Dynamics Experiment (FLUDEX) at the Experimental Lakes Area (ELA) in northwest Ontario was designed to test the hypothesis that methylmercury (MeHg) production in reservoirs is related to the amount, and subsequent decomposition, of flooded organic matter. Three upland forest sites that varied in the amounts of organic carbon stored in vegetation and soils (Low C, 30,870 kg C ha−1; Medium C, 34,930 kg C ha−1; and High C, 45,860 kg C ha−1) were flooded annually from May to September with low-organic carbon, low-MeHg water pumped from a nearby lake. Within five weeks of flooding, MeHg concentrations in the reservoir outflows exceeded those in reservoir inflows and remained elevated for the duration of the experiment, peaking at 1.60 ng L−1 in the Medium C reservoir. We estimated the net production of MeHg in each reservoir by calculating annual changes in pools of MeHg stored in flooded soils, periphyton, zooplankton, and fish. Overall, there was an initial pulse of MeHg production (range = 120–1590 ng m−2 day−1) in all FLUDEX reservoirs that lasted for 2 years, after which time net demethylation (range = 360–1230 ng MeHg degraded m−2 day−1) began to reduce the pools of MeHg in the reservoirs, but not back to levels found prior to flooding. Rates of MeHg production were generally related to the total amount of organic carbon flooded to create the reservoirs. Large increases in MeHg stores in soils compared to those in water and biota indicate that flooded soils were the main sites of MeHg production. This study should assist hydroelectric utilities and government agencies in making informed decisions about selecting sites for future reservoir development to reduce MeHg contamination of the reservoir fisheries.

Assessment of mercury bioaccumulation within the pelagic food web of lakes in the western Great Lakes region

While mercury is a health hazard to humans and wildlife, the biogeochemical processes responsible for its bioaccumulation in pelagic food webs are still being examined. Previous studies have indicated both “bottom-up” control of piscivorous fish Hg content through methylmercury.(MeHg) supply, as well as site-specific trophic factors. We evaluated ten studies from the western Great Lakes region to examine the similarity of MeHg trophic transfer efficiency within the pelagic food web, and assessed regional-scale spatial variability. Analyses of bioaccumulation and biomagnification factors between water, seston, zooplankton, and preyfish indicated that the largest increases in MeHg occurred at the base of the food web, and that the relative extent of trophic transfer was similar between sites. Positive correlations were observed between aqueous unfiltered MeHg, total Hg, and dissolved organic carbon, and measures of the efficiency of MeHg trophic transfer were consistent across widely disparate systems (both natural and experimentally manipulated) throughout North America. Such similarity suggests that the aqueous supply of MeHg is largely controlling bioaccumulation in pelagic food webs, while local, lake-specific variability can result from an array of trophic (biological) factors.

Carbon Dioxide and Methane Production in Small Reservoirs Flooding Upland Boreal Forest

The FLooded Uplands Dynamics EXperiment (FLUDEX) was designed to assess the impact of reservoir creation on carbon cycling in boreal forests by (a) determining whether production of the greenhouse gases (GHG) carbon dioxide (CO2) and methane (CH4) in reservoirs is related to the amount of organic carbon (OC) stored in the flooded landscape, (b) examining temporal trends in GHG production during initial stages of flooding, and (c) considering the net difference between GHG fluxes before and after flooding to estimate the true effect of reservoir creation on atmospheric GHG levels. Three forested sites that varied in the amount of OC stored in soils and vegetation (30,870–45,860 kg C ha–1) were experimentally flooded from June to September in 1999–2001. Throughout the study, net CO2 and CH4 production in all three reservoirs was not related to overall site OC storage. During the 1st flooding season, net CO2 production in the three reservoirs was 703–797 kg C ha–1, but it decreased during the 2nd and 3rd flooding seasons to between 408 and 479 kg C ha–1. However, CH4 production increased in all reservoirs with each flooding season, from about 3.2–4.6 kg C ha–1 in 1999 to 12.8–24.9 kg C ha–1 in 2000 and 29.7–35.2 kg C ha–1 in 2001. Over the long term, effects of boreal reservoir creation on atmospheric GHG levels may be largely due to net changes in CH4 cycling between the undisturbed and flooded ecosystems.

Mercury concentrations in surface water and harvested waterfowl from the prairie pothole region of Saskatchewan.

Mercury cycling in prairie ecosystems is poorly understood. We examined methylmercury (MeHg) concentrations in whole water from 49 diverse prairie wetlands and lakes in Saskatchewan. We also determined total Hg (THg) concentrations in waterfowl harvested by hunters for consumption. Average whole water MeHg concentrations ranged from 0.02 to over 4 ng L(-1) and were higher in water from wetland ponds compared to those in lakes. High MeHg concentrations in prairie wetlands present the possibility of increased Hg concentrations in biota inhabiting these and other similar systems. We therefore measured THg in 72 birds representing 13 species of waterfowl that commonly use prairie aquatic habitats. A large range in THg concentrations was observed among individual birds, with values ranging from below the detection limit to over 435 ng g(-1). When waterfowl were classified according to diet, we observed clear evidence of THg biomagnification with increasing proportion of animal prey consumed. THg concentrations in waterfowl collected by hunters did not exceed consumption guidelines of 0.5 mg kg(-1) developed for fish. This is the first study that has reported MeHg concentrations in water from the prairie pothole region of southern Saskatchewan.

Concentrations of methylmercury in invertebrates from wetlands of the Prairie Pothole Region of North America

Prairie wetlands may be important sites of mercury (Hg) methylation resulting in elevated methylmercury (MeHg) concentrations in water, sediments and biota. Invertebrates are an important food resource and may act as an indicator of MeHg exposure to higher organisms. In 2007-2008, invertebrates were collected from wetland ponds in central Saskatchewan, categorized into functional feeding groups (FFGs) and analyzed for total Hg (THg) and MeHg. Methylmercury and THg concentrations in four FFGs ranged from 0.2-393.5 ng · g(-1) and 9.7-507.1 ng · g(-1), respectively. Methylmercury concentrations generally increased from gastropods with significantly lower average MeHg concentrations compared to other invertebrate taxa. Surrounding land use (agricultural, grassland and organic agricultural) may influence MeHg concentrations in invertebrates, with invertebrate MeHg concentrations being higher from organic ponds (457.5 ± 156.7 ng · g(-1)) compared to those from grassland ponds (74.8 ± 14.6 ng · g(-1)) and ponds on agricultural lands (32.8 ± 6.2 ng · g(-1)).

Mercury methylation in high and low-sulphate impacted wetland ponds within the prairie pothole region of North America

Using enriched stable (201)Hg injections into intact sediment cores, we provide the first reported Hg methylation potential rate constants (km) in prairie wetland ponds (0.016-0.17 d(-1)). Our km values were similar to other freshwater wetlands and did not differ in ponds categorized with high compared to low surface water concentrations of sulphate. Sites with high sulphate had higher proportions of methylmercury (MeHg) in sediment (2.9 ± 1.6% vs. 1.0 ± 0.3%) and higher surface water MeHg concentrations (1.96 ± 1.90 ng L(-1)vs. 0.56 ± 0.55 ng L(-1)). Sediment-porewater partitioning coefficients were small, and likely due to high ionic activity. Our work suggests while km measurements are useful for understanding mercury cycling processes, they are less important than surface water MeHg concentrations for assessing MeHg risks to biota. Significant differences in MeHg concentrations between sites with high and low sulphate concentrations may also inform management decisions concerning wetland remediation and creation.

Mercury and methylmercury in aquatic sediment across western North America.

Large-scale assessments are valuable in identifying primary factors controlling total mercury (THg) and monomethyl mercury (MeHg) concentrations, and distribution in aquatic ecosystems. Bed sediment THg and MeHg concentrations were compiled for >16,000 samples collected from aquatic habitats throughout the West between 1965 and 2013. The influence of aquatic feature type (canals, estuaries, lakes, and streams), and environmental setting (agriculture, forest, open-water, range, wetland, and urban) on THg and MeHg concentrations was examined. THg concentrations were highest in lake (29.3±6.5μgkg(-1)) and canal (28.6±6.9μgkg(-1)) sites, and lowest in stream (20.7±4.6μgkg(-1)) and estuarine (23.6±5.6μgkg(-1)) sites, which was partially a result of differences in grain size related to hydrologic gradients. By environmental setting, open-water (36.8±2.2μgkg(-1)) and forested (32.0±2.7μgkg(-1)) sites generally had the highest THg concentrations, followed by wetland sites (28.9±1.7μgkg(-1)), rangeland (25.5±1.5μgkg(-1)), agriculture (23.4±2.0μgkg(-1)), and urban (22.7±2.1μgkg(-1)) sites. MeHg concentrations also were highest in lakes (0.55±0.05μgkg(-1)) and canals (0.54±0.11μgkg(-1)), but, in contrast to THg, MeHg concentrations were lowest in open-water sites (0.22±0.03μgkg(-1)). The median percent MeHg (relative to THg) for the western region was 0.7%, indicating an overall low methylation efficiency; however, a significant subset of data (n>100) had percentages that represent elevated methylation efficiency (>6%). MeHg concentrations were weakly correlated with THg (r(2)=0.25) across western North America. Overall, these results highlight the large spatial variability in sediment THg and MeHg concentrations throughout western North America and underscore the important roles that landscape and land-use characteristics have on the MeHg cycle.

Effects of in‐channel beaver impoundments on mercury bioaccumulation in Rocky Mountain stream food webs

Beavers (Castor spp.) are ecosystem engineers and important modifiers of freshwater ecosystems. They create impoundments that flood the surrounding landscape and modify the flow of materials through streams, thus potentially increasing nutrients, productivity and the availability of toxic methyl mercury (MeHg) to downstream food webs. Here we quantify food web-available MeHg in water, periphyton, and invertebrates collected from 15 streams up- and down-stream from beaver impoundments in the Rocky Mountain foothills of Western Canada. While nutrients, algal biomass, and total invertebrate standing stock were not significantly elevated below ponds, MeHg concentrations (average increase of 1.7×) and percent of total Hg that was MeHg (average increase of 1.3×) showed a trend of higher values in all compartments downstream and the difference was significant in predatory invertebrates. This suggests that beaver impoundments can increase the availability and subsequent uptake of MeHg by basal food web organisms even if their immediate influence on nutrients and resources is limited. As beaver populations continue to rebound, more research is needed to fully characterise the effects of beavers on nutrient and contaminant cycling under different biogeochemical conditions.