Hg Pools Research Articles

Mercury isotope signatures of digests and sequential extracts from industrially contaminated soils and sediments

Environmental mercury (Hg) pollution is a matter of global concern. Mercury speciation controls its environmental behaviour, and stable isotope ratios can potentially trace Hg movement through environmental compartments. Here we investigated Hg in industrially contaminated soils and sediments (Visp, Valais, Switzerland) using concentration and stable isotope analysis (CV-MC-ICP-MS) of total digests, and a four-step sequential extraction procedure. The sequential extraction employed (1) water (labile Hg species), (2) NaOH or Na4P2O7 (organically-bound Hg), (3) hydroxylamine-HCl (Hg bound to Mn and Fe (oxyhydr)oxides), and (4) aqua regia (residual Hg pools). The majority of Hg was extracted in step 4 and up to 36% in step 2. Mercury bound to organic matter was the dominant source of Hg in water, NaOH and Na4P2O7 extracts. Sulfides and colloidal oxide minerals were possible additional sources of Hg in some samples. The inconsistent comparative performance of NaOH and Na4P2O7 extractions showed that these classical extractants may not extract Hg exclusively from the organically-bound pool. Samples taken at the industrial facility displayed the greatest isotopic variation (δ202Hg: −0.80‰ ± 0.14‰ to 0.25‰ ± 0.13‰, Δ199Hg: −0.10‰ ± 0.03‰ to 0.02‰ ± 0.03‰; all 2SD) whereas downstream of the facility there was much less variation around average values of δ202Hg = −0.47‰ ± 0.11‰ and Δ199Hg = −0.05‰ ± 0.03‰ (1SD, n = 19). We interpret the difference as the result of homogenisation by mixing of canal sediments containing Hg from the various sources at the industrial facility with preservation of the mixed industrial Hg signature downstream. In contrast to previous findings, Hg isotopes in the sequential extracts were largely similar to one another (2SD < 0.14‰), likely demonstrating that the Hg speciation was similar among the extracts. Our results reveal that Hg resides in relatively stable soil pools which record an averaged isotope signature of the industrial sources, potentially facilitating source tracing studies with Hg isotope signatures at larger spatial scales further downstream.

Organic horizon and mineral soil mercury along three clear-cut forest chronosequences across the northeastern USA.

Mercury (Hg) is a globally distributed pollutant trace metal that has been increasing in terrestrial environments due to rising anthropogenic emissions. Vegetation plays an important role in Hg sequestration in forested environments, but increasing tree removal for biofuels and wood products may affect this process. The long-term effect of clear-cutting on forest soil Hg remains uncertain, since most studies are limited to measuring changes for <10years following a single harvest event. The chronosequence approach, which substitutes space for time using forest stands of different ages since clear-cutting, allows for investigation of processes occurring over decades to centuries. Here, we utilized three clear-cut forest soil chronosequences across the northeastern USA to understand Hg accumulation and retention over several decades. Total Hg concentrations and pools were quantified for five soil depth increments along three chronosequences. Our results showed Hg concentrations and pools decreased in the initial 20years following clear-cutting. Mineral soil Hg pools decreased 21-53% (7-14mgm-2) between 1-5-year-old stands and 15-25-year-old stands but mineral soil Hg pools recovered in 55-140-year-old stands to similar values as measured in 1-5-year-old stands. Our study is one of the first to demonstrate a decrease and recovery in Hg pool size. These changes in Hg did not correspond with changes in bulk density, soil C, or pH. We utilized a simple two-box model to determine how different Hg fluxes affected organic and mineral soil horizon Hg pools. Our simple model suggests that changes in litterfall and volatilization rates could have caused the observed changes in organic horizon Hg pools. However, only increases in leaching could reproduce observed decreases to mineral soil Hg pools. Further studies are needed to determine the mechanism of Hg loss from forest soils following clear-cutting.

Exotic Earthworms Decrease Cd, Hg, and Pb Pools in Upland Forest Soils of Vermont and New Hampshire USA.

Exotic earthworms are present in the forests of northeastern USA, yet few studies have documented their effects on pollutant metals in soil. The objective of this study was to identify if Cd, Hg, and Pb strong-acid extractable concentrations and pools (bulk inventories) in forest soils decreased with the presence of exotic earthworms. We compared 'Low Earthworm Abundance' (LEA) sites (≤10g m-2 earthworms, n = 13) and 'High Earthworm Abundance' (HEA) (>10g m-2 earthworms, n = 17) sites at five watersheds across Vermont and New Hampshire. Organic horizon Cd, Hg, and Pb concentrations were lower at HEA than LEA sites. Organic horizon and total soil pools of Cd and Hg were negatively correlated with earthworm biomass. Soil profile Cd and Hg concentrations were lower at HEA than LEA sites. Our results suggest earthworms are decreasing accumulation of Cd, Hg, and Pb in forest soils, potentially via greater mobilization through organic matter disruption or bioaccumulation.

Long-term trends of surface-water mercury and methylmercury concentrations downstream of historic mining within the Carson River watershed

The Carson River is a vital water resource for local municipalities and migratory birds travelling the Pacific Flyway. Historic mining practices that used mercury (Hg) to extract gold from Comstock Lode ore has left much of the river system heavily contaminated with Hg, a practice that continues in many parts of the world today. Between 1998 and 2013, the United States Geological Survey (USGS) collected and analyzed Carson River water for Hg and methylmercury (MeHg) concentrations resulting in a sixteen year record of unfiltered total mercury (uf.THg), filtered (dissolved) Hg (f.THg), total methylmercury (uf.MeHg), filtered MeHg (f.MeHg), and particulate-bound THg (p.THg) and MeHg (p.MeHg) concentrations. This represents one of the longest continuous records of Hg speciation data for any riverine system, thereby providing a unique opportunity to evaluate long-term trends in concentrations and annual loads. During the period of analysis, uf.THg concentration and load trended downward at rates of −0.85% and −1.8% per year, respectively. Conversely, the f.THg concentration increased at a rate of 1.7% per year between 1998 and 2005, and 4.9% per year between 2005 and 2013. Trends in flow-normalized partition coefficients for both Hg and MeHg suggest a statistically significant shift from the particulate to the filtered phase. The upwardly accelerating f.THg concentration and observed shift from the solid phase to the aqueous phase among the pools of Hg and MeHg within the river water column signals an increased risk of deteriorating ecological conditions in the lower basin with respect to Hg contamination. More broadly, the 16-year trend analysis, completed 140 years after the commencement of major Hg releases to the Carson River, provides a poignant example of the ongoing legacy left behind by gold and silver mining techniques that relied on Hg amalgamation, and a cautionary tale for regions still pursuing the practice in other countries.

Soil hydrology, physical and chemical properties and the distribution of carbon and mercury in a postglacial lake-plain wetland

Northern wetland soils hold globally significant carbon (C) and mercury (Hg) stocks whose cycling feeds back to atmospheric pollution, climate change, and the trophic dynamics of adjacent aquatic ecosystems. At a more local level, patterns of variation in the hydrologic, physical and chemical properties of wetland soils inform the appreciation of these ecosystems in their own right; describing patterns of variation, their potential drivers and consequences is a key step towards placing wetland soils in the context of broader landscape-level processes, such as C and Hg export to aquatic ecosystems. In this case study, we investigated a 10ha, 3000year old lake-plain wetland in the Great Lakes region (U.S.A.), located at the interface between a 120ha, first-order watershed and a 6700ha inland lake. We monitored water tables, measured soil morphology and physical characteristics, applied interpolation and mapping to model hydrologic flowpaths and spatial variation in soil depth, morphology, total C and Hg stocks, and used chemical analyses (elemental concentrations and isotope signatures, UV–Vis and FTIR spectroscopy) to quantify relationships between soil C and Hg pools, organic matter composition, and C cycling rates. Key findings from this site include: 1) whole-profile soil C and Hg stocks are readily predicted from soil depth; 2) soil saturation is semipermanent but spatially and temporally variable; 3) accumulated organic soil materials are dominated by aromatic moieties, but possess considerable amounts of labile polysaccharides; 4) subtle, topography- mediated hydrologic flowpaths create profiles of interbedded organic and mucky sand horizons with sharp discontinuities in their C and Hg concentrations. Compared to peatlands across the region and North America, soil depths and C stocks are rather low, averaging 84cm and 394Mgha−1, respectively. On the contrary, total Hg concentrations of organic soil materials (137 and 191ngg−1 for fibric vs. sapric, respectively) are at the high end for wetlands of the Great Lakes region, and more representative of those observed in areas of the eastern U.S. with historically elevated atmospheric deposition. Given past and potentially increased future variation in hydrologic regimes due to climate change, the presence of banded (sandy) profiles that may act as preferential flowpaths, and the large quantities of Hg and labile C held in these soils, they may act as significant sources of C and Hg to the atmosphere or adjacent aquatic ecosystems.

Mercury concentrations and pools in four adjacent coniferous and deciduous upland forests in Beijing, China

AbstractUnderstanding of forest mercury (Hg) pools is important for quantifying the global atmospheric Hg removal. We studied gaseous elemental Hg (GEM) concentrations, litterfall Hg depositions, and pool sizes in four adjacent stands at Mount Dongling to assess Hg dynamics in the forested catchment and the potential of Hg release during wildfires. The average GEM concentration was 2.5 ± 0.5 ng m−3, about 1.5 times of the background levels in the Northern Hemisphere. In all four stands, Hg concentrations increase in the following order: bole wood &lt; branch/twig &lt; bark &lt; mineral soil &lt; needles/leaves &lt; litterfall &lt; Oi litter &lt; Oe soil &lt; Oa organic soil. The Hg pools of aboveground biomass were comparable in the forests of larch, oak, and Chinese pine, which were much greater than that of mixed broadleaf stands due to lower biomass. The total Hg pools in ecosystems were similar in the four stands, because of the comparable Hg pool in the soil horizons (0–40 cm), which accounted for over 97% of the total ecosystem Hg storage in the four stands. Although Hg pools of the forest ecosystem in north China were comparable to North America and North Europe, Hg storage in forests constituted a high threat for large Hg emission pulses to the atmosphere by wildfires. The potential Hg emissions from the combustion at the four stands were ranged from 0.675 to 1.696 mg m−2.

Stable isotope composition of mercury forms in flue gases from a typical coal-fired power plant, Inner Mongolia, northern China

Mercury forms emitted from coal combustion via air pollution control devices are speculated to carry different Hg isotope signatures. Yet, their Hg isotope composition is still not reported. Here, we present the first onsite Hg isotope data for gaseous elemental Hg (GEM) and gaseous oxidized Hg (GOM) of flue gases from a typical lignite-fired power plant (CFPP). Significant mass dependent fractionation (MDF) and insignificant mass independent fractionation (MIF) are observed between feed coal and coal combustion products. As compared to feed coal (δ202Hg=−2.04±0.25‰), bottom ash, GEM and GOM in flue gases before and after wet flue gas desulfurization system significantly enrich heavy Hg isotopes by 0.7–2.6‰ in δ202Hg, while fly ash, desulfurization gypsum and waste water show slight but insignificant enrichment of light Hg isotopes. GEM is significantly enriched heavy Hg isotopes compared to GOM and Hg in fly ash. Our observations verify the previous speculation on Hg isotope fractionation mechanism in CFPPs, and suggest a kinetically-controlled mass dependent Hg isotope fractionation during transformation of Hg forms in flue gases. Finally, our data are compared to Hg isotope compositions of atmospheric Hg pools, suggesting that coal combustion Hg emission is likely an important atmospheric Hg contributor.

Emissions of forest floor and mineral soil carbon, nitrogen and mercury pools and relationships with fire severity for the Pagami Creek Fire in the Boreal Forest of northern Minnesota

Forest fires cause large emissions of C (carbon), N (nitrogen) and Hg (mercury) to the atmosphere and thus have important implications for global warming (e.g. via CO2 and N2O emissions), anthropogenic fertilisation of natural ecosystems (e.g. via N deposition), and bioaccumulation of harmful metals in aquatic and terrestrial systems (e.g. via Hg deposition). Research indicates that fires are becoming more severe over much of North America, thus increasing element emissions during fire. However, there has been little research relating forest floor and mineral soil losses of C, N and Hg to on-the-ground indices of fire severity that enable scaling up those losses for larger-scale accounting of fire-level emissions. We investigated the relationships between forest floor and mineral soil elemental pools across a range of soil-level fire severities following the 2011 Pagami Creek wildfire in northern Minnesota, USA. We were able to statistically differentiate losses of forest floor C, N and Hg among a five-class soil-level fire severity classification system. Regression relationships using soil fire severity class were able to predict remaining forest floor C, N and Hg pools with 82–96% confidence. We correlated National Aeronautics and Space Administration Airborne Visible and Infrared Imaging Spectrometer-Classic imagery to ground-based plot-scale estimates of soil fire severity to upscale emissions of C, N and Hg to the fire level. We estimate that 468 000 Mg C, 11 000 Mg of N and over 122 g of Hg were emitted from the forest floor during the burning of the 28 310 ha upland area of the Pagami Creek fire.

Soil mercury distribution in adjacent coniferous and deciduous stands highly impacted by acid rain in the Ore Mountains, Czech Republic

Forests play a primary role in the cycling and storage of mercury (Hg) in terrestrial ecosystems. This study aimed to assess differences in Hg cycling and storage resulting from different vegetation at two adjacent forest stands - beech and spruce. The study site Načetín in the Czech Republic's Black Triangle received high atmospheric loadings of Hg from coal combustion in the second half of the 20th century as documented by peat accumulation rates reaching 100 μg m−2 y−1. In 2004, the annual litterfall Hg flux was 22.5 μg m−2 y−1 in the beech stand and 14.5 μg m−2 y−1 in the spruce stand. Soil concentrations and pools of Hg had a strong positive relation to soil organic matter and concentrations of soil sulfur (S) and nitrogen (N). O-horizon Hg concentrations ranged from 245 to 495 μg kg−1 and were greater in the spruce stand soil, probably as a result of greater dry Hg deposition. Mineral soil Hg concentrations ranged from 51 to 163 μg kg−1 and were greater in the beech stand soil due to its greater capacity to store organic carbon (C). The Hg/C ratio increased with depth from 0.3 in the O-horizon to 3.8 μg g−1 in the C horizon of spruce soil and from 0.7 to 2.7 μg g−1 in beech soil. The Hg/C ratio was greater at all mineral soil depths in the spruce stand. The organic soil Hg pools in beech and spruce stands (6.4 and 5.7 mg m−2, respectively) were considerably lower than corresponding mineral soil Hg pools (39.1 and 25.8 mg m−2). Despite the important role of S in Hg cycling, differences in soil Hg distribution at both stands could not be attributed to differences in soil sulfur speciation.

Effects of Nutrient Loading and Mercury Chemical Speciation on the Formation and Degradation of Methylmercury in Estuarine Sediment.

Net formation of methylmercury (MeHg) in sediments is known to be affected by the availability of inorganic divalent mercury (Hg(II)) and by the activities of Hg(II) methylating and MeHg demethylating bacteria. Enhanced autochthonous organic matter deposition to the benthic zone, following increased loading of nutrients to the pelagic zone, has been suggested to increase the activity of Hg(II) methylating bacteria and thus the rate of net methylation. However, the impact of increased nutrient loading on the biogeochemistry of mercury (Hg) is challenging to predict as different geochemical pools of Hg may respond differently to enhanced bacterial activities. Here, we investigate the combined effects of nutrient (N and P) supply to the pelagic zone and the chemical speciation of Hg(II) and of MeHg on MeHg formation and degradation in a brackish sediment-water mesocosm model ecosystem. By use of Hg isotope tracers added in situ to the mesocosms or ex situ in incubation experiments, we show that the MeHg formation rate increased with nutrient loading only for Hg(II) tracers with a high availability for methylation. Tracers with low availability did not respond significantly to nutrient loading. Thus, both microbial activity (stimulated indirectly through plankton biomass production by nutrient loading) and Hg(II) chemical speciation were found to control the MeHg formation rate in marine sediments.

Mercury dynamics and mass balance in a subtropical forest, southwestern China

Abstract. The mid-subtropical forest area in southwest China was affected by anthropogenic mercury (Hg) emissions over the past 3 decades. We quantified mercury dynamics on the forest field and measured fluxes and pools of Hg in litterfall, throughfall, stream water and forest soil in an evergreen broadleaved forest field in southwestern China. Total Hg (THg) input by the throughfall and litterfall was assessed at 32.2 and 42.9 µg m−2 yr−1, respectively, which was remarkably higher than those observed from other forest fields in the background of North America and Europe. Hg fluxes across the soil–air interface (18.6 mg m−2 yr−1) and runoff and/or stream flow (7.2 µg m−2 yr−1) were regarded as the dominant ways for THg export from the forest field. The forest field hosts an enormous amount of atmospheric Hg, and its reserves is estimated to be 25 341 µg m2. The ratio of output to input Hg fluxes (0.34) is higher compared with other study sites. The higher output / input ratio may represent an important ecological risk for the downstream aquatic ecosystems, even if the forest field could be an effective sink of Hg.

A synthesis of terrestrial mercury in the western United States: Spatial distribution defined by land cover and plant productivity

A synthesis of published vegetation mercury (Hg) data across 11 contiguous states in the western United States showed that aboveground biomass concentrations followed the order: leaves (26μgkg−1)~branches (26μgkg−1)>bark (16μgkg−1)>bole wood (1μgkg−1). No spatial trends of Hg in aboveground biomass distribution were detected, which likely is due to very sparse data coverage and different sampling protocols. Vegetation data are largely lacking for important functional vegetation types such as shrubs, herbaceous species, and grasses.Soil concentrations collected from the published literature were high in the western United States, with 12% of observations exceeding 100μgkg−1, reflecting a bias toward investigations in Hg-enriched sites. In contrast, soil Hg concentrations from a randomly distributed data set (1911 sampling points; Smith et al., 2013a) averaged 24μgkg−1 (A-horizon) and 22μgkg−1 (C-horizon), and only 2.6% of data exceeded 100μgkg−1. Soil Hg concentrations significantly differed among land covers, following the order: forested upland>planted/cultivated>herbaceous upland/shrubland>barren soils. Concentrations in forests were on average 2.5 times higher than in barren locations. Principal component analyses showed that soil Hg concentrations were not or weakly related to modeled dry and wet Hg deposition and proximity to mining, geothermal areas, and coal-fired power plants. Soil Hg distribution also was not closely related to other trace metals, but strongly associated with organic carbon, precipitation, canopy greenness, and foliar Hg pools of overlying vegetation. These patterns indicate that soil Hg concentrations are related to atmospheric deposition and reflect an overwhelming influence of plant productivity — driven by water availability — with productive landscapes showing high soil Hg accumulation and unproductive barren soils and shrublands showing low soil Hg values. Large expanses of low-productivity, arid ecosystems across the western U.S. result in some of the lowest soil Hg concentrations observed worldwide.

Mercury in coniferous and deciduous upland forests in northern New England, USA: implications of climate change

Abstract. Climatic changes in the northeastern US are expected to cause coniferous stands to transition to deciduous stands over the next hundred years. Mercury (Hg) sequestration in forest soils may change as a result. In order to understand potential effects of such a transition, we studied aboveground vegetation and soils at paired coniferous and deciduous stands on eight mountains in Vermont and New Hampshire, USA. Organic horizons at coniferous stands accumulated more total Hg (THg; 42 ± 6 g ha−1) than deciduous stands (30 ± 4 g ha−1). Total Hg pools in the mineral horizons were similar for coniferous (46 ± 8 g ha−1) and deciduous stands (45 ± 7 g ha−1). Soil properties (C, % clay, and pH) explained 56 % of the variation in mineral soil Hg concentration when multiply regressed. Foliar and bole wood Hg concentrations were generally greater for coniferous species than deciduous species. Using allometric equations, we estimated that aboveground accumulation of Hg in foliage and woody biomass was similar between vegetation types but that coniferous stands have significantly smaller annual litterfall fluxes (0.03 g ha−1 yr−1) than deciduous stands (0.24 g ha−1 yr−1). We conclude that organic horizon Hg accumulation is influenced by vegetation type but mineral horizon Hg accumulation is primarily controlled by soil properties. Further investigations into the effect of vegetation type on volatilization, atmospheric deposition, and leaching rates are needed to constrain regional Hg cycling rates.

Anthropogenic mercury sequestration in different soil types on the southeast coast of China

Soil is a major pool of anthropogenically emitted mercury (Hg) and will in turn be a source of atmospheric Hg contamination. It was hypothesized that accumulation of anthropogenic Hg in the soil at a regional scale is associated with the amount of Hg emitted to the atmosphere and soil type. A total of 448 horizon samples were collected from the typical soil types of the Yangtze River Delta and Pearl River Delta. Titanium (Ti) was selected as a reference element to discriminate anthropogenic Hg from the Hg associated with pedogenic processes. Soil pools of anthropogenic Hg were quantified to show the difference in Hg sequestration among soil types and regions. Soil pools of anthropogenic Hg ranged from 0.70 to 6971 g/ha in the Yangtze River Delta (YRD) and from 35.81 to 13098.71 g/ha in the Pearl River Delta (PRD). The estimated soil Hg pools were well correlated with the amounts of Hg emitted in these two regions. Soil properties, namely organic matter content, amorphous iron oxides, and cation exchange capacity, were significantly (p < 0.01) and positively correlated with soil Hg accumulation. Meanwhile, soil organic matter was the most important factor to determine the depth distribution of Hg in soil profile of the majority of soils. Perudic Cambisols and Stagnic Anthrosols which contained higher content of amorphous iron oxides had the highest soil Hg pools, indicating the importance of amorphous iron oxides other than organic matter to the Hg retention in soil. Soil and soil horizons with low pH and high salinity did show a low accumulation of Hg probably due to the remobilization of Hg under such conditions. In addition to the amount of Hg emitted, soil types may be a major factor in controlling the sequestration of anthropogenic Hg in both regions. Stagnic Anthrosols are an important pool for retention of anthropogenic Hg.

Mercury isotope signatures in contaminated sediments as a tracer for local industrial pollution sources.

Mass-dependent fractionation (MDF) and mass-independent fractionation (MIF) may cause characteristic isotope signatures of different mercury (Hg) sources and help understand transformation processes at contaminated sites. Here, we present Hg isotope data of sediments collected near industrial pollution sources in Sweden contaminated with elemental liquid Hg (mainly chlor-alkali industry) or phenyl-Hg (paper industry). The sediments exhibited a wide range of total Hg concentrations from 0.86 to 99 μg g(-1), consisting dominantly of organically-bound Hg and smaller amounts of sulfide-bound Hg. The three phenyl-Hg sites showed very similar Hg isotope signatures (MDF δ(202)Hg: -0.2‰ to -0.5‰; MIF Δ(199)Hg: -0.05‰ to -0.10‰). In contrast, the four sites contaminated with elemental Hg displayed much greater variations (δ(202)Hg: -2.1‰ to 0.6‰; Δ(199)Hg: -0.19‰ to 0.03‰) but with distinct ranges for the different sites. Sequential extractions revealed that sulfide-bound Hg was in some samples up to 1‰ heavier in δ(202)Hg than organically-bound Hg. The selectivity of the sequential extraction was tested on standard materials prepared with enriched Hg isotopes, which also allowed assessing isotope exchange between different Hg pools. Our results demonstrate that different industrial pollution sources can be distinguished on the basis of Hg isotope signatures, which may additionally record fractionation processes between different Hg pools in the sediments.

Differentiated availability of geochemical mercury pools controls methylmercury levels in estuarine sediment and biota.

Neurotoxic methylmercury (MeHg) formed from inorganic divalent mercury (Hg(II)) accumulates in aquatic biota and remains at high levels worldwide. It is poorly understood to what extent different geochemical Hg pools contribute to these levels. Here we report quantitative data on MeHg formation and bioaccumulation, in mesocosm water-sediment model ecosystems, using five Hg(II) and MeHg isotope tracers simulating recent Hg inputs to the water phase and Hg stored in sediment as bound to natural organic matter or as metacinnabar. Calculations for an estuarine ecosystem suggest that the chemical speciation of Hg(II) solid/adsorbed phases control the sediment Hg pool's contribution to MeHg, but that input of MeHg from terrestrial and atmospheric sources bioaccumulates to a substantially greater extent than MeHg formed in situ in sediment. Our findings emphasize the importance of MeHg loadings from catchment runoff to MeHg content in estuarine biota and we suggest that this contribution has been underestimated.

Changing climate alters inputs and pathways of mercury deposition to forested ecosystems

Although land cover and meteorological conditions are known to impact mercury (Hg) deposition processes, few studies have addressed how changes in forest cover and shifting climatic conditions will impact the Hg cycle. The purpose of this study was to examine the effects of forest type (hardwood vs. conifer) and meteorological variation on atmospheric Hg deposition in two forest stands in Huntington Wildlife Forest in upstate New York, USA. Mercury deposition associated with litterfall was similar between the hardwood and conifer stands, but total Hg deposition was greater in the coniferous stand due to larger throughfall Hg. Soil evasion losses of Hg were significantly higher in the hardwood plot. Although Hg deposition was greater and evasion losses were lower in the conifer plot, soil Hg pools were smaller than in the hardwood plot. Annual variability in meteorological conditions was substantial between 2009 and 2010, and changes in Hg deposition over this period appear to be related to variation in temperature and precipitation quantity. The results from this study suggest that projected increases in temperature and precipitation in the northeastern United States could alter Hg deposition and availability by decreasing litterfall Hg inputs and increasing throughfall Hg inputs.

Distribution and Pools of Mercury in Czech Forest Soils

Parts of the Czech Republic received extreme loading of acid deposition from coal combustion in the second half of the twentieth century. Although associated Hg deposition was not directly measured, Hg deposition rates calculated from peat cores approach 100 μg m−2 year−1. We quantified the soil concentrations and pools of Hg with carbon (C), sulfur (S), and nitrogen (N)—elements closely associated with soil organic matter at five sites across the Czech Republic—four sites known for extreme deposition levels of S and N compounds in the twentieth century, and one site relatively less impacted. The site-specific means of O-horizon Hg concentrations ranged from 277 to 393 μg kg−1, while means of Hg concentrations in mineral soil ranged from 22 to 95 μg kg−1. The mean Hg/C ratio across sites increased from ∼0.5 μg Hg g−1 C in the Oi-horizon to ∼5 μg Hg g−1 C in the C-horizon due to the progressive mineralization of soil organic matter. The soil Hg/C increase was accompanied by a soil C/N decrease, another indicator of soil organic matter mineralization. Soil Hg/C also increased as soil C/S decreased, suggesting that Hg was stabilized by S functional groups within the soil organic matter. Mineral soil Hg pools (8.9–130.0 mg m−2) dominated over organic soil Hg pools (5.3–10.1 mg m−2) at all sites. Mineral soil Hg pools correlated more strongly with total soil S and oxalate-extractable Fe than with total soil C. Total soil Hg pools could be accounted for by a time period of atmospheric inputs that was short relative to the age of the soils. The cross site variability of Hg soil pools was not sensitive to the local Hg deposition history but rather related to the capacity of soil to store and stabilize organic matter.

Post‐Fire Comparisons of Forest Floor and Soil Carbon, Nitrogen, and Mercury Pools with Fire Severity Indices

Forest fires are important contributors of C, N, and Hg to the atmosphere. In the fall of 2011, a large wildfire occurred in northern Minnesota and we were able to quickly access the area to sample the forest floor and mineral soil for C, N, and Hg pools. When compared with unburned reference soils, the mean loss of C resulting from fire in the forest floor and the upper 20 cm of mineral soil was 19.3 Mg ha−1, for N the mean loss was 0.17 Mg ha−1, and for Hg the mean loss was 9.3 g ha−1. To assess the influence of fire severity on the forest floor and mineral soils, we used an established method that included a soil burn severity index and a tree burn severity index with a gradient of severity classes. It was apparent that the unburned reference class had greater forest floor C, N, and Hg pools and higher C/N ratios than the burned classes. The C/N ratios of the 0‐ to 10‐ and 10‐ to 20‐cm mineral soils in the unburned reference class were also greater than in the burned classes, indicating that a small amount of C was lost and/or N was gained, potentially through leaching unburned forest floor material. However, with a couple of exceptions, the severity classes were unable to differentiate the forest floor and mineral soil impacts among soil burn and tree burn severity indices. Developing burn severity indices that are reflective of soil elemental impacts is an important first step in scaling ecosystem impacts both within and across fire events.

Spatial and vertical distribution of mercury in upland forest soils across the northeastern United States

Assessing current Hg pools in forest soils of the northeastern U.S. is important for monitoring changes in Hg cycling. The forest floor, upper and lower mineral horizons were sampled at 17 long-term upland forest sites across the northeastern U.S. in 2011. Forest floor Hg concentration was similar across the study region (274 ± 13 μg kg−1) while Hg amount at northern sites (39 ± 6 g ha−1) was significantly greater than at western sites (11 ± 4 g ha−1). Forest floor Hg was correlated with soil organic matter, soil pH, latitude and mean annual precipitation and these variables explained approximately 70% of the variability when multiple regressed. Mercury concentration and amount in the lower mineral soil was correlated with Fe, soil organic matter and latitude, corresponding with Bs horizons of Spodosols (Podzols). Our analysis shows the importance of regional and soil properties on Hg accumulation in forest soils.