Total Hg Fluxes Research Articles

Needle age and precipitation as drivers of Hg accumulation and deposition in coniferous forests from a southwestern European Atlantic region

Vegetation and climate are critical in the biogeochemical cycle of Hg in forest ecosystems. The study assesses the influence of needle age and precipitation on the accumulation of Hg in needle biomass and its deposition by litterfall in thirty-one pine plantations spread throughout two biogeographical regions in SW Europe. Well-developed branches of Pinus pinaster were sampled and pine needles were classified according to 4 age classes (y0, y1, y2, y3). The concentration of total Hg (THg) was analyzed in the samples and Hg content in needle biomass and its deposition by litterfall were estimated. The concentration of total Hg (THg) increased with needle age ranging from 9.1 to 32.7 μg Hg kg−1 in the youngest and oldest needles, respectively. The rate of Hg uptake (HgR) three years after needle sprouting was 10.2 ± 2.3 μg Hg kg−1 yr−1, but it decreased with needle age probably due to a diminution in photosynthetic activity as needles get older. The average total Hg stored in needle biomass (HgWt) ranged from 5.6 to 87.8 mg Hg ha−1, with intermediate needle age classes (y1 and y2) accounting for 70% of the total Hg stored in the whole needle biomass. The average deposition flux of Hg through needle litterfall (HgLt) was 1.5 μg Hg m−2 yr−1, with the y2 and y3 needles contributing most to the total Hg flux. The spatial variation of THg, HgWt and HgLt decreased from coastal pine stands, characterized by an oceanic climate, to inland pine stands, a feature closely related to the dominant precipitation regime in the study area. Climatic conditions and needle age are the main factors affecting Hg accumulation in tree foliage, and should be considered for an accurate assessment of forest Hg pools at a regional scale and their potential consequences in the functioning of terrestrial ecosystems.

Melting Himalayas and mercury export: Results of continuous observations from the Rongbuk Glacier on Mt. Everest and future insights

Glaciers in the Himalayan region have been receding rapidly in recent decades, drawing increasing concerns about the release of legacy pollutants (e.g., mercury (Hg)). To investigate the distribution, transport and controlling factors of Hg in glacier-fed runoff, from June 2019 to July 2020, a continuous monitoring and an intensive sampling campaign were conducted in the Rongbuk Glacier-fed basin (RGB) on the north slope of Mt. Everest in the middle Himalayas. The total Hg (THg) and methyl Hg (MeHg) concentrations were 1.56 ± 0.85 and 0.057 ± 0.025 ng/L, respectively, which were comparable to the global background levels and were mainly affected by the total suspended particulate matter (TSP). In addition, THg and MeHg showed significant diurnal variations, with peak values appearing at approximately 17:00 (upstream) and 19:00 (downstream). Based on the annual runoff and average Hg concentration, the annual export fluxes of THg and MeHg were estimated to be 441 g and 16 g, respectively. The yields of THg and MeHg in the RGB were 1.6 and 0.06 μg/m2/year, respectively. Currently, the annual Hg export of meltwater runoff in the Himalayan region is approximately 337 kg/year. When flowing through the proglacial lake, the THg concentrations decreased by 32% and 15% in the proglacial lake water and in the outlet, respectively, indicating that proglacial lakes had a sedimentation effect on the Hg transport. The Hg export from meltwater runoff in the Himalayas will likely increase considering the meltwater runoff has been projected to increase in the future. Nonetheless, emerging proglacial lakes may exert ambiguous effects on the glacier exported Hg under changing climate. Proglacial lakes could lower the levels and amounts of Hg in the glacier runoff, whereas the outburst of proglacial lakes could lead to an instantaneous release of Hg stored in lake waters and sediments. Our analysis shed light on the environmental impact of glacier retreat in the Himalayas and highlighted the need for integrated monitoring and study of Hg in glacier runoff and glacial lakes.

250-year records of mercury and trace element deposition in two lakes from Cajas National Park, SW Ecuadorian Andes

Historical records of trace elements in lake sediments provide source-to-sink information about potentially toxic pollutants across space and time. We investigated two lakes located at different elevations in the Ecuadorian Andes to understand how trace element fluxes are related to (i) geology, (ii) erosion in the watersheds, and (iii) local point sources and atmospheric loads. In remote Lake Fondococha (4150 m a.s.l.), total Hg fluxes stay constant between ca. 1760 and 1950 and show an approximately 4.4-fold increase between pre-1950 and post-1950 values. The post-1950 increase in fluxes of other trace elements (V, Cr, Co, Ni, Cu, Zn, As, Cd, and Pb) is lower (2.1–3.0-fold) than for Hg. Mostly lithogenic sources and enhanced soil erosion contribute to their post-1950 increase (lithogenic contribution: > 85%, Hg: ~ 58%). Average post-1950 Hg fluxes are approximately 4.3 times higher in peri-urban Lake Llaviucu (3150 m a.s.l.) than in the remote Lake Fondococha. Post-1950 fluxes of the other trace elements showed larger differences between Lakes Fondococha and Llaviucu (5.2 < 25–29.5-fold increase; Ni < Pb–Cd). The comparison of the post-1950 average trace element fluxes that are derived from point and airborne sources revealed 5–687 (Hg–Pb) times higher values in Lake Llaviucu than in Lake Fondococha suggesting that Lake Llaviucu’s proximity to the city of Cuenca strongly influences its deposition record (industrial emissions, traffic, caged fishery). Both lakes responded with temporary drops in trace element accumulations to park regulations in the 1970s and 1990s, but show again increasing trends in recent times, most likely caused by increase in vehicular traffic and openings of copper and gold mines around Cajas National Park.

Decreasing litterfall mercury deposition in central European coniferous forests and effects of bark beetle infestation

We evaluated a 14-year trend (2003–2017) in mercury (Hg) concentrations and fluxes in six litterfall categories (needles, bark, twigs, cones, lichen, and a mixture of unidentified fragments) at six research plots situated in two central European unmanaged mountain forest stands, dominated by mature Norway spruce. One of the stands (catchment of Plešné Lake, PL) was infested by bark beetle and all mature spruces died at three of four research plots during the study. One PL plot and two plots in the second stand (catchment of Čertovo Lake, CT) were intact and used as a control. At the intact plots, the litterfall Hg deposition averaged 45 and 32 μg/m2/year in the PL and CT catchments, respectively, while bulk precipitation Hg deposition was an order of magnitude lower (2.6 μg/m2/year). In the individual litter categories, Hg concentrations averaged 223, 195, 126, 81, 79 and 30 μg/kg in lichen, unidentified fragments, bark, twigs, needles and cones, respectively. As a result of decreasing European Hg emissions, Hg concentrations in most litter categories decreased from 2003 to 2017. Consequently, the litter-associated Hg flux to the forest floor decreased from 66 to 23 μg/m2/year during 2003–2017. The litterfall mass fluxes exhibited no trends at the intact plots. In contrast, the litter-associated Hg flux increased 5-fold after tree dieback due to elevated litterfall, averaging 218 μg/m2/year Hg at the PL infested plots during 2004–2009. The relative contribution of individual litter categories to the total Hg flux shifted from needle to bark and twig dominance. Starting in 2010, Hg flux decreased to pre-disturbance levels for the following decade. The tree mortality in the PL catchment provided a unique opportunity to evaluate changes in litter-associated Hg fluxes to the forest floor during and after natural tree dieback.

Methyl and Total Mercury in Different Media and Associated Fluxes in a Watershed Forest, Southwest China.

Mercury (Hg) deposition in the forest ecosystem is a significant source of input for methyl Hg (MeHg) and total Hg (THg) to the subtropical forest field and downstream aquatic systems. Wet deposition, litterfall, runoff, and fluxes with forest soil percolate of MeHg and THg were sampled for two years in a watershed forest of southwest China. Results showed that the depositions of THg and MeHg through litterfall and throughfall were 86 µg m−2 yr−1 and 0.8 µg m−2 yr−1 respectively, with litterfall acting as a predominant route for the input of both THg and MeHg. The estimated fluxes of THg and MeHg in the throughfall and litterfall were 3 and 4 times greater than those in the precipitation. Methylmercury in the decomposed litter migrates during its erosion by surface runoff and the concentrations of MeHg were quite consistent with that in the surface runoff. Methylmercury mainly accumulated in the lower layer of the litter and upper layer of the soil (Oi), and its transfer through the soil cross-section was delayed. THg retention was not consistent with MeHg, probably with lower soil layers (Oe and Oa) storing and enriching THg in the forest ecosystem. The forest floor of the lower soil is an effective sink for THg but not for MeHg. Methylmercury accumulated in decomposing litter and upper soil layer might transfer with soil percolate, possessing potential ecological risks for residents living around the downstream aquatic systems.

Flux model to estimate the transport of mercury species in a contaminated lagoon (Ria de Aveiro, Portugal).

The concentrations of dissolved and particulate inorganic mercury (IHg(II)) and methylmercury (MeHg) from the contaminated Laranjo Bay (main freshwater discharge from the Antuã River) were measured by species-specific isotope dilution during six sampling campaigns at high and at low tide. Different effective riverine concentrations were calculated, based on salinity profiles, for specific hydrological conditions. The export fluxes of total Hg and MeHg (324 and 1.24molyear-1, respectively) from the bay to the rest of the Aveiro Lagoon are much higher than the input fluxes from the Hg source (3.9 and 0.05molyear-1) and from the Antuã River (10.4 and 0.10molyear-1). Resuspension of contaminated sediments from Laranjo Bay is crucial for the transport of both IHg(II) and MeHg. Methylation and/or selective enrichment into biogenic particles is responsible for the mobilization of MeHg. Sorption of dissolved IHg(II) onto suspended particles limits its export flux. This is one of the rarest examples where both speciation fluxes and partitioning of mercury are studied in a contaminated coastal environment. Despite the lower fraction of total MeHg (relative to total Hg), the contaminated lagoon may have an impact on coastal areas, particularly if change in the lagoon geometry occurs, due to sea level rise.

Emerging investigator series: the effect of wildfire on streamwater mercury and organic carbon in a forested watershed in the southeastern United States.

Wildfires alter forested ecosystems, which include large stores of mercury (Hg) and organic carbon, two compounds that are closely linked in vegetation, soils, and streamwater. Studies have shown that wildfires release elevated levels of mercury to the atmosphere which can be locally redeposited and leave charred organic material (vegetation and litter) on the soil surface. Both can contribute to the elevated mobilization of Hg into lakes and streams. However, no studies have conducted a detailed examination of hydrological transport of Hg following a wildfire. This study investigates the coupled transport of mercury and carbon at Twomile Run, a headwater stream located in the forested mountains of Shenandoah National Park, in the year following a low-severity wildfire. Weekly baseflow samples and bi-hourly high-flow storm samples were analyzed for dissolved and particulate mercury (HgD and HgP, respectively), dissolved organic carbon (DOC), UV absorbance at 254 nm (UV254, surrogate for DOC quantity and character), and total suspended solids (TSS), and were compared with identical measurements taken from a nearby unburned watershed. For all flow conditions sampled at the burned site (which did not include the 2 months following the fire), streamwater HgD and DOC concentrations, and corresponding UV254, were similar to the unburned system. TSS concentrations varied between sites but overall differences were relatively small in magnitude and likely attributable to site differences rather than fire effects. Notably, the HgP per unit of TSS at the burned site was an order of magnitude higher than the unburned site (2.66 and 0.13 ng HgP per mg TSS, respectively) for 8 months following the fire, resulting in elevated HgP concentrations for the range of flow conditions, after which there was a rapid return to non-disturbed conditions. Streamwater total Hg fluxes roughly doubled (0.55 to 1.04 μg m-2 yr-1) as a consequence of the fire, indicating that in addition to changing atmospheric and terrestrial Hg cycling, fires can rapidly and significantly alter the streamwater Hg which has implication for downstream ecosystems. These findings are particularly relevant as the occurrence and severity of wildfires are expected to increase in the mid-latitudes in response to climate change.

Flux of Total Mercury and Methylmercury to the Northern Gulf of Mexico from U.S. Estuaries

To better understand the source of elevated methylmercury (MeHg) concentrations in Gulf of Mexico (GOM) fish, we quantified fluxes of total Hg and MeHg from 11 rivers in the southeastern United States, including the 10 largest rivers discharging to the GOM. Filtered water and suspended particles were collected across estuarine salinity gradients in Spring and Fall 2012 to estimate fluxes from rivers to estuaries and from estuaries to coastal waters. Fluxes of total Hg and MeHg from rivers to estuaries varied as much as 100-fold among rivers. The Mississippi River accounted for 59% of the total Hg flux and 49% of the fluvial MeHg flux into GOM estuaries. While some estuaries were sources of Hg, the combined estimated fluxes of total Hg (~5200 mol y(-1)) and MeHg (~120 mol y(-1)) from the estuaries to the GOM were less than those from rivers to estuaries, suggesting an overall estuarine sink. Fluxes of total Hg from the estuaries to coastal waters of the northern GOM are approximately an order of magnitude less than from atmospheric deposition. However, fluxes from rivers are significant sources of MeHg to estuaries and coastal regions of the northern GOM.

Wet deposition fluxes of total mercury and methylmercury in core urban areas, Chongqing, China

Wet deposition fluxes of mercury (Hg) species were estimated during the period from June 2010 to July 2011 at 3 sites in core urban areas in Chongqing, China. Rain water was collected by automatic deposition sampler for total Hg (THg) and methylmercury (MeHg) analyses. Our results showed that annual wet deposition fluxes of THg and MeHg were 28.7 ± 5.1 and 0.28 ± 0.09 μg m−2 yr−1, respectively. We estimate that MeHg wet deposition contributes 9.2–19.6% of the total MeHg flux to a local reservoir. Cumulative THg fluxes collected from nine principal rainfall events (>1.5 μg m−2 yr−1) at three sampling sites accounted for 20% of annual overall THg wet deposition. Statistical analyses yielded significant relationship between rainfall amounts and Hg wet deposition fluxes (r2 = 0.76, p < 0.01 for THg; r2 = 0.65, p < 0.01 for MeHg), suggesting that rainfall is one of the most important factors controlling the Hg fluxes. Obvious seasonal variations of THg fluxes were observed, with the maximum value occurring in summer (accounting for 40% of total annual THg deposition) while minimum values occurred in winter in all the three sampling sites. 72-h backward trajectory analysis on nine large deposition events at the three sites, using HYSPLIT model indicated that most of air masses which contain a relatively high precipitation amount and pass through major Hg sources would have an elevated Hg load.

Mercury speciation in wet deposition samples collected from a coastal area of Minamata Bay

To better understand the methylation and demethylation of mercury (Hg) in the atmosphere, monomethyl mercury (MMHg) concentrations in wet deposition samples collected in the Minamata Bay area from September, 2009 to August, 2010 were determined. The concentrations of total Hg (dissolved Hg + particulate Hg) and dissolved reactive Hg were also measured. The volume-weighted mean concentrations of dissolved MMHg and total Hg were 0.061 and 5.9 ng L−1, respectively. Almost 90% of total Hg was in the dissolved phase and dissolved reactive Hg was the dominant Hg species in the wet deposition. The wet deposition fluxes of total Hg and reactive Hg increased in the rainy season (summer and fall), while the concentrations and wet deposition fluxes of MMHg were higher in winter and spring than in summer. Factors affecting this seasonal variation of MMHg were also considered. The MMHg in wet depositions may be decomposed by the increased levels of UV radiation in summer months, although MMHg can also be emitted from anthropogenic and biogenic sources and/or produced by photochemical reactions. Long-range transport from the Asian continent may also contribute to the seasonal variation of the wet MMHg deposition flux.

Climate change and watershed mercury export: a multiple projection and model analysis

Future shifts in climatic conditions may impact watershed mercury (Hg) dynamics and transport. An ensemble of watershed models was applied in the present study to simulate and evaluate the responses of hydrological and total Hg (THg) fluxes from the landscape to the watershed outlet and in-stream THg concentrations to contrasting climate change projections for a watershed in the southeastern coastal plain of the United States. Simulations were conducted under stationary atmospheric deposition and land cover conditions to explicitly evaluate the effect of projected precipitation and temperature on watershed Hg export (i.e., the flux of Hg at the watershed outlet). Based on downscaled inputs from 2 global circulation models that capture extremes of projected wet (Community Climate System Model, Ver 3 [CCSM3]) and dry (ECHAM4/HOPE-G [ECHO]) conditions for this region, watershed model simulation results suggest a decrease of approximately 19% in ensemble-averaged mean annual watershed THg fluxes using the ECHO climate-change model and an increase of approximately 5% in THg fluxes with the CCSM3 model. Ensemble-averaged mean annual ECHO in-stream THg concentrations increased 20%, while those of CCSM3 decreased by 9% between the baseline and projected simulation periods. Watershed model simulation results using both climate change models suggest that monthly watershed THg fluxes increase during the summer, when projected flow is higher than baseline conditions. The present study's multiple watershed model approach underscores the uncertainty associated with climate change response projections and their use in climate change management decisions. Thus, single-model predictions can be misleading, particularly in developmental stages of watershed Hg modeling.

Mercury in the Gulf of Mexico: Sources to receptors

Gulf of Mexico (Gulf) fisheries account for 41% of the U.S. marine recreational fish catch and 16% of the nation's marine commercial fish landings. Mercury (Hg) concentrations are elevated in some fish species in the Gulf, including king mackerel, sharks, and tilefish. All five Gulf states have fish consumption advisories based on Hg. Per-capita fish consumption in the Gulf region is elevated compared to the U.S. national average, and recreational fishers in the region have a potential for greater MeHg exposure due to higher levels of fish consumption. Atmospheric wet Hg deposition is estimated to be higher in the Gulf region compared to most other areas in the U.S., but the largest source of Hg to the Gulf as a whole is the Atlantic Ocean (>90%) via large flows associated with the Loop Current. Redistribution of atmospheric, Atlantic and terrestrial Hg inputs to the Gulf occurs via large scale water circulation patterns, and further work is needed to refine estimates of the relative importance of these Hg sources in terms of contributing to fish Hg levels in different regions of the Gulf. Measurements are needed to better quantify external loads, in-situ concentrations, and fluxes of total Hg and methylmercury in the water column, sediments, and food web.

Benthic transfer and speciation of mercury in wetland sediments downstream from a sewage outfall

In order to evaluate the role of hypoxic conditions of overlying water in the benthic flux and speciation of Hg, we analyzed sediment cores from hypoxic or oxic sites downstream from a sewage outfall in the Damyang Riverine Wetland, Korea. Each core was analyzed for total Hg (THg), monomethylmercury (MMHg), and elemental Hg (Hg 0) from sediment, and for THg and MMHg from pore water. Hypoxic conditions of the overlying water near the sewage outfall were associated with a peak production of Hg 0, but the lowest production of MMHg, in the upper 2 cm sediments. The benthic fluxes of THg and MMHg were estimated at 130–2109 ng m −2 day −1 and −12 to 260 ng m −2 day −1, respectively. The order of MMHg flux from sediment to overlying water at each site did not follow the order of MMHg concentration in sediment, but was highest in hypoxic water conditions. The results suggest that maintaining oxic conditions in wetland water is important for decreasing the transfer of MMHg from sediment into overlying water.

Legacy and Fate of Mercury and Methylmercury in the Florida Everglades

Mass inventories of total Hg (THg) and methylmercury (MeHg) and mass budgets of Hg newly deposited during the 2005 dry and wet seasons were constructed for the Everglades. As a sink for Hg, the Everglades has accumulated 914, 1138, 4931, and 7602 kg of legacy THg in its 4 management units, namely Water Conservation Area (WCA) 1, 2, 3, and the Everglades National Park (ENP), respectively, with most Hg being stored in soil. The current annual Hg inputs account only for 1-2% of the legacy Hg. Mercury transport across management units during a season amounts to 1% or less of Hg storage, except for WCA 2 where inflow inputs can contribute 4% of total MeHg storage. Mass budget suggests distinct spatiality for cycling of seasonally deposited Hg, with significantly lower THg fluxes entering water and floc in ENP than in the WCAs. Floc in WCAs can retain a considerable fraction (around 16%) of MeHg produced from the newly deposited Hg during the wet season. This work is important for evaluating the magnitude of legacy Hg contamination and for predicting the fate of new Hg in the Everglades, and provides a methodological example for large-scale studies on Hg cycling in wetlands.

New clues on the contribution of Earth’s volcanism to the global mercury cycle

Active volcanoes are thought to be important contributors to the atmospheric mercury (Hg) budget, and this chemical element is one of the most harmful atmospheric pollutants, owing to its high toxicity and long residence time in ecosystems. There is, however, considerable uncertainty over the magnitude of the global volcanic Hg flux, since the existing data on volcanogenic Hg emissions are sparse and often ambiguous. In an attempt to extend the currently limited dataset on volcanogenic Hg emissions, we summarize the results of Hg flux measurements at seven active open-conduit volcanoes; Stromboli, Asama, Miyakejima, Montserrat, Ambrym, Yasur, and Nyiragongo.. Data from the dome-building Soufriere Hills volcano are also reported. Using our determined mercury to SO2 mass ratios in tandem with the simultaneously-determined SO2 emission rates, we estimate that the 7 volcanoes have Hg emission rates ranging from 0.2 to 18 t yr-1 (corresponding to a total Hg flux of ~41 t·yr-1). Based on our dataset and previous work, we propose that a Hg/SO2 plume ratio ~10-5 is best-representative of gas emissions from quiescent degassing volcanoes. Using this ratio, we infer a global volcanic Hg flux from persistent degassing of ~95 t·yr-1 .

Mercury dynamics in relation to dissolved organic carbon concentration and quality during high flow events in three northeastern U.S. streams

Mercury (Hg) contamination is widespread in remote areas of the northeastern United States. Forested uplands have accumulated a large reservoir of Hg in soil from decades of elevated anthropogenic deposition that can be released episodically to stream water during high flows. The objective of this study was to evaluate spatial and temporal variations in stream water Hg species and organic matter fractions over a range of hydrologic conditions in three forested upland watersheds (United States). Mercury and organic matter concentrations increased with discharge at all three sites; however, the partitioning of Hg fractions (dissolved versus particulate) differed among sites and seasons. Associated with increased discharge, flow paths shifted from mineral soil under base flow to upper soil horizons. As flow paths shifted, greater concentrations of dissolved organic carbon (DOC) richer in aromatic substances were flushed from upper soil horizons to stream water. The hydrophobic organic matter associated with humic material from upper soils appears to have had a greater capacity to bind Hg. Because of the strong correlation between Hg and DOC, we hypothesize that there was a concurrent shift in the source of Hg with DOC from lower mineral soil to upper soil horizons. Our study suggests that stream discharge is an effective predictor of dissolved total Hg flux.

Spatial distribution of mercury and other trace elements in recent lake sediments from central Alberta, Canada: An assessment of the regional impact of coal-fired power plants

These have been growing concerns over the environmental impacts of the coal-fired power plants in the western Canadian province of Alberta, which collectively comprise one of the largest point sources of Hg and other trace elements nationally. The overall cumulative impact of the power plants since the beginning of their activities several decades ago has been a critical question for industry, government agencies, and the research community. This paper aims to delineate the cumulative geographic extent of impact by investigating the spatial distribution of mercury and other trace elements of environmental concern in nine freshwater lakes, which cover the large area surrounding the coal-fired power plants in central Alberta, Canada. 210-Lead dating was used in conjunction with physical evidence of deposited fly ash to determine the sediments' age and hence the depths corresponding to the onset of coal-fired power generation in 1956. Total mean concentrations and fluxes of elements of environmental concern with integrated values since 1956 were then determined. The concentration values do not reflect the catastrophic oil spill at Lake Wabamun in 2005. The post-1956 flux rates of As, Cd, Co, Cr, Cu, Hg, Mo, Ni, Pb, Sb, V, W, and Zn were generally highest in sediment cores obtained from two lakes adjacent to power plants. However, the variable prevailing wind directions played an important role in determining the aerial distribution of Hg and other trace elements to the southeast and to the west of the power plants. Post-1956 fluxes of most elements declined downwind (westward), consistent with strong easterly winds transporting metal pollution further to the west of the power plants. However, spatial interpolation of the data suggested a major southern extension to the area of maximum metal deposition, which has not been sampled by this or previous studies in the region. An atmospheric model estimate of total Hg flux in 2007 near the Genesee power plant was substantially lower than indicated by the most impacted lake sediments, which have integrated Hg fluxes since 1956. The most likely explanations for the model-sediment difference are either that a sharp spatial gradient of deposition exists in the region, and/or recent technology improvements by the power plants have substantially reduced Hg emissions.

Mercury transport in response to storm events from a northern forest landscape

AbstractConcentrations and fluxes of mercury (Hg) species in surface waters of forested watersheds are affected by hydrological events. The mechanisms of Hg transport during these events are poorly understood and yet may influence Hg bioavailability and exposure to aquatic biota. Three storm events with varying magnitude and intensity were investigated (June, September and November 2005) at a forested watershed in the Adirondack region of New York State, USA. Concentrations of Hg species increased during these events, both above and downstream of wetlands in the watershed. While Hg flux was higher from wetland drainage, the Hg flux from the upland site exhibited a greater relative increase to elevated runoff. Hg flux was controlled by discharge; however, Hg species concentrations were not well correlated with discharge, dissolved organic carbon (DOC), or total suspended solids (TSS) through the duration of events. A counter‐clockwise hysteresis response of DOC with increasing runoff contrasted with the clockwise response for total Hg, suggesting different contributions from source areas for these solutes. Correspondence with elevated total K and NO3− (α &lt; 0·05) during the rising limb of the hydrograph suggests rapid delivery of throughfall Hg, potentially enhanced by hillslope hollows, to the stream channel. As the watershed saturated, stream Hg appears to be derived from the soil Hg pool. Results suggest that particulate Hg did not contribute substantially to total Hg flux during events (&lt;25%). These results emphasize the role of watershed attributes and storm characteristics in Hg transport and bioavailability. Copyright © 2008 John Wiley &amp; Sons, Ltd.

The development and application of a mass balance model for mercury (total, elemental and methyl) using data from a remote lake (Big Dam West, Nova Scotia, Canada) and the multi-species multiplier method

Abstract Big Dam West, located in Kejimkujik Park, Nova Scotia, Canada, is a remote lake with elevated Hg concentrations in fish due in part to low pH and high dissolved organic carbon (DOC) concentrations. These features reflect the poor buffering capacity of peat lands in the flat drainage basin. To address the multiple species of Hg, a model was developed by coupling the “multiplier method” for multi-species chemicals with average concentration ratios to the Quantitative Water Air Sediment Interaction (QWASI) model. Elemental Hg was the “key species” modeled. Total Hg fluxes and concentrations were computed using concentration ratios. Many of the concentrations and Hg flux processes within the Big Dam West catchment had been previously measured with concentration ratios that were either computed or taken from the literature when measured data were not available. Measured values for total Hg concentration in each compartment (air, water, sediment) and Hg fluxes (e.g., precipitation, sediment deposition) enable verification of model concentration and flux estimates for total Hg in each environmental compartment. The model was also run with and without the inclusion of upward Hg fluxes from the underlying sediment to determine the significance of this controversial flux. The Hg QWASI model presented in this paper could be a valuable screening tool, especially for remote lakes, due to its ability to provide reasonable Hg estimates with a limited amount of data (water inflow rate, suspended particulate matter, sediment deposition velocity, and concentration of Hg in atmosphere and inflow water).

Evidence for Control of Mercury Accumulation Rates in Canadian High Arctic Lake Sediments by Variations of Aquatic Primary Productivity

Climate warming in the 20th Century has had profound effects on the limnology of High Arctic lakes, including substantial increases in autochthonous primary productivity (APP). Here, we report organic carbon and Hg core profiles from two lakes which support the hypothesis that 20th Century increases in sedimentary Hg at these latitudes were largely driven by APP increases, via Hg scavenging by algae and/or suspended detrital algal matter. Hydrocarbons quantitatively released by thermal cracking of algal-derived organic matter ("S2" carbon) were used to reconstruct past APP. Variation of S2 flux accounted for 87-91% of the variance in total Hg flux in the study lakes since 1854. Mercury and S2 carbon were also associated during the pre-Industrial Period, co-varying by as much as 30% during past warm/cool periods. As a test of the hypothesis, predicted values for 20th Century [Hg] were derived from pre-1900 Hg-S2 relationships. Measured 20th Century [Hg] was on average only 6-11% higher than that predicted in one lake, and 33% higher in the other. S2-normalization of [Hg] in the latter lake suggested that 78% of the average increase in 20th Century [Hg] could be explained by scavenging. These findings suggest that the atmospheric contribution of long-range anthropogenic Hg to High Arctic lakes may have been overestimated by several-fold because of this climate-driven process, and was responsible for no more than 22% of the 20th Century [Hg] increase in the study lakes.