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1.
The spatial and temporal distribution of elemental Hg (Hg°) and reactive Hg (HgR) has been studied on Pallette Lake, Wisconsin during May – August, 1993 and May, 1994. In general, Hg° concentrations near the lake surface greatly exceeded saturation with respect to atmospheric Hg° indicating a flux out (?) of the lake. Evasional losses were estimated using a thin film model and averaged ?101 pmol m?2 d?1 during July and August, 1993. A large portion of atmospherically deposited Hg is re-emitted. Thus, in-lake Hg° production' and evasion to the atmosphere will significantly reduce the amount of Hg which is transported to the sediments, the principal site of methylation. Laboratory experiments were conducted to ascertain the rate of Hg° formation from Hg(II). Reduction was significantly lower in heat sterilized lakewater suggesting Hg° production was biologically mediated. The temporal distribution of epilimnetic Hg°, as measured at the lake center, was influenced by Hg° evasion, Hg° production and advective transport of water parcels of differing Hg content. Spatial gradients in Hg° and HgR were identified and a transport model was employed to estimate the advective flux of Hg°. The importance of atmospheric deposition and sediment-water interaction as sources of HgR to epilimnetic waters were examined. Porewater concentrations of Hg° and HgR were determined on several occasions. During May, 1994, the depletion of lakewater HgR following a input pulse due to rain was observed and the estimated removal rate (16–20% d?1) agrees well with reduction rates obtained in the laboratory (23% d?1).  相似文献   

2.
Biogeochemical cycling of mercury (Hg) in the ocean and air-sea exchange are integral parts of the global Hg cycle. Ionic Hg (i.e. reactive Hg-Hg°) is converted in ocean surface waters to elemental Hg (Hg°) with the subsequent loss, via gas evasion, of the Hg° to the atmosphere. During a recent cruise in the North Atlantic Ocean, Hg° in surface waters was a substantial fraction of the reactive Hg (85%, on average) and there was a relationship between photosynthetic pigment concentration and Hg°. In addition, there was evidence of Hg bound to “collodial” material (of greater than 1,000 molecular weight). Ionic Hg concentrations were around 0.15 pM, similar to the average colloidal Hg concentration of 0.2 pM. Methylated Hg compounds, both dimethylHg (DMHg) and monomethylHg (MMHg), were found in the deeper waters with DMHg being the predominant methylated species. This contrasts with freshwater lakes where MMHg is the principal species and no DMHg has been found. Preliminary modelling, using estimated rate constants for the formation and decomposition of DMHg and MMHg, predicts an enhanced stability of DMHg in ocean waters relative to fresh water. Deep ocean waters, formed by sinking of surface waters, can preserve DMHg that was produced in the more productive surface regime.  相似文献   

3.
Different species of mercury have different physical/chemical properties and thus behave quite differently in air pollution control equipment and in the atmosphere. In general, emissions of mercury from coal combustion sources are approximately 20–50% elemental mercury (Hg°) and 50–80% divalent mercury (Hg(II)), which may be predominantly HgCl2. Emissions of mercury from waste incinerators are approximately 10–20% Hg° and 75–85% Hg(II). The partitioning of mercury in flue gas between the elemental and divalent forms may be dependent on the concentration of particulate carbon, HCl and other pollutants in the stack emissions. The emission of mercury from combustion facilities depends on the species in the exhaust stream and the type of air pollution control equipment used at the source. Air pollution control equipment for mercury removal at combustion facilities includes activated carbon injection, sodium sulfide infection and wet lime/limestone flue gas desulfurization. While Hg(II) is water-soluble and may be removed from the atmosphere by wet and dry deposition close to combustion sources, the combination of a high vapor pressure and low water-solubility facilitate the long-range transport of Hg° in the atmosphere. Background mercury in the atmosphere is predominantly Hg°. Elemental mercury is eventually removed from the atmosphere by dry deposition onto surfaces and by wet deposition after oxidation to water-soluble, divalent mercury.  相似文献   

4.
As with many urban environments, a number of sources of airborne elemental mercury (Hg°) exist in New York City, yet little research has been conducted to examine the flux and sources of mercury in New York. In this study, we conducted ambient monitoring of Hg° at six locations in New York City. Airborne Hg° averaged 3.84±0.10 ng m-3 and 3.70±0.08 ng m-3 in the boroughs of Manhattan and Brooklyn respectively, yet only 2.69±0.03 ng m-3 in a more residential neighborhood in Queens. Both precipitation and ambient temperature were significantly correlated with ambient Hg° levels in New York City, suggesting that the surface emission of mercury from urban surfaces plays a role in urban Hg° concentrations. Local sources were also seen to contribute to urban Hg° levels by leading to `spikes' of Hg° in which elevated concentrations were recorded for short periods of time.  相似文献   

5.
Surface waters of the Scheldt Estuary were sampled on various occasions between 1991 and 1994. Longitudinal particulate Hg (PM) concentrations ranged from 0.4 – 1.7 μgHg/g and are essentially controlled by physical mixing of polluted fluvial particulates with relatively unpolluted marine particulates. Total dissolved mercury (TDM)concentrations ranged from 0.5 to 5.2 ng/L and are strongly influenced by removal and mobilization processes in the upper estuary, while in the lower estuary mixing processes cause a progressive decrease in TDM towards the mouth. Speciation studies showed that dissolved Hg is predominantly bound to strong complexing ligands (organic substances) in the upper estuary, but this fraction decreases with increasing salinity. In June 1993, however, the reactive mercury fraction was also high in the upper estuary. Model calculations showed that a conditional stability constant for Hg- humic acid interactions of 1019 was a good estimate for the Scheldt estuary. Dissolved methylmercury was analyzed on three occasions. Significant seasonal variations were observed with concentrations ranging from 11 to 120 pg/L in the winter and 80 to 400 pg/L in summer. Supersaturation of Hg° is observed throughout the whole estuary resulting in an estimated evasion flux of 140–1400 ng/m2 day.  相似文献   

6.
It has been shown that an untreated mercury-polluted floodplain soil (containing 10 μg/g per dry weight (d.w.) total Hg and 12 ng/g (d.w.) monomethylmercury compounds (MMM)) of the river Elbe in Northern Germany contains both dimethylmercury (DMM) and elemental mercury (Hg°). This is the first time ever that DMM has been detected in unmodified soils. A novel purge- and-trap-technique involving a sequential thermodesorption-separation of the two species after trapping on a carbon molecular sieve (CMS) has been developed that allows the determination of the two species DMM and Hg° from aqueous solutions or soil samples by GC-CVAFS. The compounds' identities as Hg-species were confirmed by GC-ICP/MS. A DMM-concentration of 740 pg/g (d.w.) was determined in the soil; the Hg°-concentration was found to be at least four times larger, but could not yet be quantified. Since no precautions against losses via evapoartion were taken during sampling and storage, the original concentrations were probably much higher. Both DMM and Hg° are easily purged with N2 from soils as well as from soil suspensions, indicating that the two species may readily evaporate from those soils under natural conditions. The amount of DMM determined in the soil suspension was significantly lower (80 pg/g (d.w.)) compared to that in the original soil sample, suggesting that DMM might not be stable under these conditions. Also, it was shown that in natural samples, MMM can be converted into DMM in the presence of sulfide, at S2?-levels as low as 100 μg/g.  相似文献   

7.
Atmospheric mobilization and exchange at the air-water interface are significant features of biogeochemical cycling of Hg at the Earth's surface. Our marine studies of Hg have been extended to terrestrial aquatic systems, where we are investigating the tropospheric cycling, deposition and air-water exchange of Hg in the mid-continental lacustrine environs of northcentral Wisconsin. This program is part of a multidisciplinary examination into the processes regulating the aquatic biogeochemistry of Hg in temperate regions. Trace-metal-free methodologies are employed to determine Hg and alkylated Hg species at the picomolar level in air, water and precipitation. We have found Hg concentrations and atmospheric fluxes in these fresh water systems to be similar to open ocean regions of the Northern Hemisphere. A well constrained mass balance for Hg has been developed for one of the lakes, Little Rock Lake, which is an extensively studied clear water seepage lake that has been divided with a sea curtain into two basins, one of which is untreated (reference pH: 6.1) while the other is being experimentally acidified (current pH: 4.7). This budget shows that the measured total atmospheric Hg deposition (ca. 10 μg m−2 yr−1) readily accounts for the total mass of Hg in fish, water and accumulating in the sediments of Little Rock Lake. This analysis demonstrates the importance of atmospheric Hg depositional fluxes to the geochemical cycling and bioaccumulation of Hg in temperate lakes. It further suggests that modest increases in atmospheric Hg loading could lead directly to enhanced levels of Hg in biota. Analogous modeling for monomethylmercury (MMHg) is as yet limited. Nevertheless, preliminary data for the atmospheric deposition of MMHg indicate that this flux is insufficient. to account for the amounts of MMHg observed in biota. An in-lake synthesis of MMHg is implicated. The importance of volatile Hg which is principally in the elemental form, and its evasion to the atmosphere is also illustrated. We suggest that the in-lake production of Hg° can reduce the Hg (II) substrate used in the in-lake microbiological synthesis of MMHg.  相似文献   

8.
Foliar exchange of mercury vapor: Evidence for a compensation point   总被引:1,自引:0,他引:1  
Historical studies for crop and weed species documented elemental Hg vapor (Hg°) deposition to foliage, but they used Hg° concentrations that were orders of magnitude higher than levels now known to occur under background conditions, possibly creating artificially high gradients between the atmosphere and landscape surfaces. Measurements of Hg° exchange with white oak (Quercus alba L.), red maple (Acer rubrum L.), Norway spruce (Picea abies L.), and yellow-poplar (Liriodendron tulipifera L.) foliage were conducted in an open gas exchange system that allows for simultaneous measurements of CO2, H2O and Hg° exchange under controlled environmental conditions. When Hg° concentrations were held at 0.5 to 1.5 ng m?3, red maple (Acer rubrum L.), Norway spruce (Picea abies L.), yellow-poplar (Liriodendron tulipifera L.), and white oak (Quercus alba L.) foliage exhibited mean Hg° emissions of 5.5, 1.7, 2.7, and 5.3 ng m?2 h?1, respectively. At Hg° concentrations between 9 and 20 ng m?3 little net exchange of Hg° was observed. However at concentrations between 50 and 70 ng m?3 the Hg° was deposited to foliage at rates between 22 and 38 ng m?2 h?1. These data suggest that dry foliar surfaces in terrestrial forest landscapes may be a dynamic exchange surface that can function as a source or sink dependent on the magnitude of current Hg° concentrations. These data provide evidence of species-specific compensation concentrations (or compensation points) for Hg° deposition to seedling foliage in the 10–25 ng m?3 range.  相似文献   

9.
The Tekran 2537A mercury vapour analyser, designed to measure Hg in air by cold vapour atomic fluorescence spectrometry, has been modified to determine Hg in solution. The new ‘front-end’, required to generate Hg° vapour from acidified waters or acid leachates, is described. Using 1% NaBH4 as reducing agent, a 12 mL water sample can be analysed, at a rate of 1 every 6 min, for Hg to a detection limit of 0.8 ppt (ng L-1). Instrumental precision is typically 1% relative standard deviation (RSD) at levels of Hg from 10 to 200 ppt. Results for 10 analyses of the international water standard, NIST 1642b, are 1530±20 ppt Hg, agreeing well with the certified value of 1480±130 ppt. Nineteen geological standard reference materials (soils, sediments and tills) were used to assess accuracy. Results for these samples, digested in aqua regia in triplicate, showed good agreement with recommended values for all but two, SO-3 and TILL-1. However, results by this method for these two standards were confirmed by an independent method, direct atomic absorption spectrometry. Average method precision was shown to be 5% RSD over the range 10 ng g- 1 to 35 μg g-1 Hg.  相似文献   

10.
Total Gaseous Mercury (TGM) data (n = 5125) measured from September 9 to November 30, 1994 in Southern Québec with an automatic TGM analyser (Tekran®) are used to study the behaviour of TGM with ozone and the water vapour mixing ratio. Results show, as a whole, no straight-forward correlation between TGM and ozone concentrations. A significant correlation between TGM and water vapour mixing ratio was measured. Some back reduction of Hg(II) to Hg° in the aqueous phase and subsequent evaporation of Hg° according to Henry‘s Law is expected. The latter correlation seems to be partly ozone dependent since under ’clean conditions‘ (ozone < 30 ppbv) the slope of TGM vs the water vapour mixing ratio is twice that during ‘polluted conditions’ (ozone ≥ 30 ppbv) which suggests some compensation effects under polluted conditions (counteracting the back-reduction of Hg(II) to Hg° in the aqueous phase). Oxidation of TGM by ozone during high moisture conditions (water vapour mixing ratio ~14g/kg) seems to appear at the threshold ozone concentration ≥ 30 ppbv.  相似文献   

11.
The release of mercury (Hg) from dental amalgam fillings has been verified by several authors. In this study, the emission rate of Hg°-vapor from the oral cavity (O-Hg) and the urinary Hg-excretion rate (U-Hg) have been studied with 34 healthy individuals. In ten cases, the urinary excretions of silver (U-Ag) and the fecal excretions of Hg and Ag (F-Hg, F-Ag) were also monitored. All variables, except U-Ag, were significantly related to the load of amalgam. According to this study, an individual with a moderate load of amalgam, i.e. 30 restored surfaces, is predicted to exhibit the following emission rates: O-Hg=22, U-Hg=3, F-Hg=60 and F-Ag=27 μg/d (d=24 hours), consistent with a gross mass balance for Hg of approximately 60 μg/d. The corresponding systemic uptake of Hg was estimated to 12 μg/d based on external data relating air Hg°-exposures to urinary Hg-excretions. The worst case individual showed a gross mass balance of 200 μg Hg/d connected to a systemic uptake of 70 μg Hg/d. These values were compared to the average intake of total-Hg by a Swedish diet (2 μg/d) and to the WHO's tolerable value for intake of total-Hg by food (45 μg/d). Upscaled to the entire Swedish population (8 mill.), the data suggests a fecal/urinary emission to the environment of 100 kg Hg yearly originating from a population load of amalgam fillings containing 90,000 kg of Hg.  相似文献   

12.
A simple, mechanistic model of mercury (Hg) dynamics in a lake has been developed, based on the fugacity/aquivalence approach of Mackay (1991) and Mackay and Diamond (1989) and its extension to treat several interconverting chemical species (Diamond et al., 1992). The model considers the distribution of inorganic (HgII), elemental (Hg°) and methyl (MeHg) mercury species between dissolved and particle-sorbed phases, and fate and transport in a system consisting of a well-mixed water column and an active sediment layer. Hg can enter the lake from watershed runoff and by atmospheric deposition directly to the lake surface. Once in the lake, Hg exchanges between water and air, and water and sediments, and exits by sediment burial, advective flow and volatilization. The model was applied to a hypothetical drainage lake on the Canadian Shield. Model estimates of water and sediment concentrations compare well with measured values. The results suggest that the three Hg species experience significantly different fates and persistence, with overall Hg dynamics dominated by the fate of HgII (the predominant species). A sensitivity analysis illustrates the importance of physical/chemical properties and lake characteristics on the total amount and behavior of Hg in the lake.  相似文献   

13.
Mercury fallout was measured 10 m from the selected emission site, the Sulfur Banks fumarole area, Hawaii Volcanoes National Park; at stations on Maui and Oahu, respectively 200 km and 380 km distant from the Sulfur Banks; and at the Hawaii Geothermal Project drill site, only 40 km from source. Sulfur Banks and Oahu measurements were carried out on six occasions between 1972 and 1976, each time within the same 24 h period. Gold foil was used for collection of elemental mercury (Hg°) and copper foil for both oxidized (Hgox) and elemental forms. The rate of deposition at the Sulfur Banks was high ? 800 μm m?2 day?1, or 300 kgkm?2 annually. The same figure applied to the relatively nearby geothermal project site. At both remote stations the fallout rate was approximately 10 fold lower. At four measurement times out of six the ratio HgO/Hgox ranged from 0.195 to 0.463 at the Sulfur Banks source and from 1.80 to 5.15 at the remote stations. On two occasions, heavy rains selectively reduced Hgox at the emission site. Model calculations compared Sulfur Banks fallout with rates of re-emission of Hg by vegetation, and the importance of the biotic factor in determination of mass balances and fluxes was emphasized. Aspects of the geochemistry and toxicology of Hg were considered briefly in relation to emission and deposition, and to the occurrence of Hg°.  相似文献   

14.
Mercury(II) toxicity experiments with green algae are complicated by the fast reduction and evaporation of Hg. A Hg buffer system is described, which considerably stabilizes the Hg(II) concentration in test solutions. The Hg buffer consists of mercury(II) chloride and N-methyliminodiacetic acid (MIDA). Dissociation of Hg-MIDA complex compensates for loss of Hg. With this system experiments were performed with Hg(II) concentrations between 0.02 and 2.0 mg I?1 at temperatures between 15° and 30°C. No effect of MIDA on the growth of the green alga Scenedesmus acutus was detected.  相似文献   

15.
Aqueous and atmospheric Hg° concentrations for remote marine areas such as the equatorial Pacific Ocean and for coastal seas such as the North Sea and the Scheldt Estuary are discussed. Biological processes seem to be at the origin of the supersaturated Hg° concentrations in the water. On the other hand, transfer velocities across the air-sea interface were calculated with a classical shear turbulence model and with a wave breaking model. With these data, Hg° fluxes from the sea to the atmosphere were calculated: in the Pacific Ocean they range from 0.43 to 6.5 μg g Hg.m?2. yr?1 at a wind speed of 2.8 m.s?1 and from 10.3 to 156 μg Hg.m?2 yr?1 at a wind speed of 54 m.s?1, but they are still higher when wave breaking is considered (from 11 to 168 μg Hg.m?2.yr?1). These transfer fluxes are an order of magnitude higher in the Scheldt Estuary.  相似文献   

16.
Increases in industrial mercury (Hg) emissions in recent years have led many researchers to believe that Hg from the atmosphere constitutes a main source of Hg to aquatic biota in the absence of point source discharges. Established background levels for fish (0.2–1.0 mg kg-1) now exceed the pre industrial level of 0.15 mg kg-1, suggesting an anthropogenic origin. This review of recent literature illustrates how levels of mercury (Hg) species in the atmosphere are effectively transported into the aquatic arena, where chemical parameters combine to determine bioaccumulation rates in fish. Limited studies on methyl mercury (MeHg) in precipitation shown that concentrations average from 5% of total-Hg (T-Hg), to 1% in industrial regions. Observations of increased Hg is snow and precipitation from the Arctic Circle, related to poleward atmospheric circulation patterns, also demonstrate a spring maximum accompanying ozone depletion. Increases in oxidants and soil derived Hg in the atmosphere during the summer best explain summer Hg maximums observed in precipitation, while increased temperatures raise fish metabolism increasing Hg uptake through respiration and ingestion rate. The major route of entry for MeHg to fish appears to be biomagnification, after input from precipitation, runoff and inlake methylation. Regions buffered against acid precipitation maintain low fish-Hg levels by reduced MeHg production and maintaining gill function. When considering the bioaccumulation of Hg in fish this study shows that there are many variables to consider, not all of which originate from inside the aquatic arena. Both catchment and atmospheric processes combine with aquatic variables to dictate the overall levels of MeHg observed in fish tissue. There now appears to be sufficient knowledge to develop an axiom for the identification of aquatic systems likely to be susceptible to bioaccumulation from atmospheric derived Hg.  相似文献   

17.
The speciation of mercury (Hg) in Minamata Bay (Japan) was studied over a 2-year period (2006?C2008). Concentrations of dissolved total Hg, dissolved methylmercury (MeHg), particulate total Hg, and suspended solids were 0.43?±?0.14 ng/l (mean?±?standard deviation), 0.10?±?0.06 ng/l, 3.04?±?2.96 ng/l, and 5.94?±?2.10 mg/l, respectively. Correlations between concentrations of particulate total Hg and suspended solids at four depths (surface: 0 m; mid-depth: ?6 m, ?10 m; and bottom +1 m layer) were only significant in the bottom +1 m layer. The mean dissolved MeHg concentration and the ratio of dissolved MeHg to dissolved total Hg were considerably higher in summer compared to other seasons. The data suggest that bottom sediment was not the sole source of MeHg, and that MeHg may be produced in the water column by the conversion of divalent Hg eluted from resuspended bottom sediment. The correlation between seawater characteristics such as salinity, temperature, dissolved oxygen (DO), and dissolved MeHg concentration indicates that Hg methylation could be influenced by the heterotrophic activity of microorganisms in the seawater. In particular, inverse correlations were observed between DO, salinity, and MeHg concentration. However, dissolved MeHg concentrations did not correlate with seawater characteristics such as pH or chlorophyll-a.  相似文献   

18.
This is a preliminary study of the reactions of mercury (Hg) in the human mouth with dental amalgams. It was conducted by analysing saliva samples from subjects with amalgam fillings and control subjects with no amalgams. Samples were collected both prior to and after cleaning the mouth. These samples were analyzed for elemental mercury (Hg0), inorganic mercury (Hg2+) and methylmercury (MeHg). We concluded that the concentrations after cleaning represented the systemic concentrations. Hg2+ and MeHg were found in all systemic samples from both subjects and controls, while Hg0 was found only in the samples from subjects with amalgams. In the control group, the concentrations found before and after cleaning the mouth were equivalent. In the amalgam group, concentrations of Hg2+ found before cleaning the mouth were 10 to 40 times higher than those found after cleaning, suggesting that the oxidation reaction of Hg° into Hg2+ takes place. For MeHg, a similar but less pronounced pattern as Hg2+ was found, supporting methylation in the mouth.  相似文献   

19.
Plants expressing a modified bacterial mercury reductase, merA, are highly resistant to Hg(II) toxicity as a result of the enzymatically catalyzed electrochemical reduction of Hg(II) to the much less toxic and volatile Hg(0). merA expression may allow plants to manifest a suite of responses to mercury exposure, making them more capable than wild-type plants of interacting with and removing mercury from contaminated soil or water. We have engineered merA-expressing Nicotiana tabacum (tobacco) as a model plant for examining these responses. Mercury resistance was demonstrated by germinating and growing merA tobacco seeds on semi-solid medium spiked with a HgCl2 concentration acutely toxic to wild-type plants. On similar growth medium, merA plant roots penetrated a highly concentrated, localized Hg(II) zone of HgS (cinnibar) more readily than wild-type roots. In hydroponic medium spiked with HgCl2, merA plants maintained higher evapotranspiration activity than wild-type plants. The ability of merA Hg(II)-reductive activity to counter typical plant-catalyzed Hg(0) oxidation to Hg(II) was demonstrated by a lower net foliar absorption of atmospheric Hg(0) than wild-type plants. Mercury translocation through merA plants was examined through reciprocally grafted merA and wild-type tobacco grown on HgCl2-spiked hydroponic medium. Elevated mercury concentrations in wild-type shoots grafted to merA roots suggest the vertical movement of mercury within merA tissues or plants may be facilitated by dynamic balance between native Hg(0) oxidation and MerA-catalyzed Hg(II) reduction. These experiments demonstrate that merA-engineered tobacco plants display an array of tissue-level and whole-plant attributes which should allow for more efficient mercury extraction and processing compared to the wild-type.  相似文献   

20.
Sampling is conducted during 2006 in Lahontan Reservoir, Nevada to investigate seasonal variation of total mercury (THg) and methylmercury (MeHg) partitioning in different phytoplankton size fractions as a function of point source (fluvial) mercury (Hg) loads, reservoir residence time, and algal growth. Carson River Hg inputs into the reservoir are extremely dynamic with spring loads two orders of magnitude larger than summer loads. Chlorophyll a measurements show two periods of algal growth. A small amount of algal growth occurs March to May. A second more substantial bloom occurs in the late summer, which is dominated by large, filamentous algae. THg concentrations (C b) and partitioning coefficients (K d) in total suspended particulate matter (SPM) are highest when fluvial inputs of Hg-contaminated sediment are large and are not necessarily associated with living biomass. However, MeHg K d in the small size fraction is indirectly related to fluvial loads and more strongly associated with living biomass in the later portion of the summer when algal growth occurs and reservoir residence times are longer. Data suggest size distinction is important to MeHg partitioning in the reservoir. Lumping all sizes into a single SPM sample will bias the analysis toward low MeHg C b and low MeHg K d in late summer when Aphanizomenon flos-aquae dominates the phytoplankton assemblage.  相似文献   

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