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1.
The role of the major biogeochemical processes in Hg cycling at the sediment–water interface was investigated in the Grado Lagoon (Northern Adriatic Sea). This wetland system has been extensively contaminated from the Idrija Hg Mine (Slovenia) through the Isonzo River suspended load carried by tidal fluxes. Three approaches were used to study the sediment–water exchange of total Hg (THg), methylmercury (MeHg), reactive Hg (RHg) and dissolved gaseous Hg (DGHg): (1) estimation of diffusive fluxes from porewater and overlying water concentrations, (2) measurements of benthic fluxes using a deployed light benthic chamber in situ and (3) measurements of benthic fluxes during oxic–anoxic transition with a laboratory incubation experiment. The THg solid phase, ranging between 9.5 and 14.4 μg g−1, showed slight variability with depth and time. Conversely, MeHg contents were highest (up to 21.9 ng g−1) at the surface; they tended to decrease to nearly zero concentration with depth, thus suggesting that MeHg production and accumulation occur predominantly just below the sediment–water interface. Porewater MeHg concentrations (0.9–7.9 ng L−1, 0.15–15% of THg) varied seasonally; higher contents were observed in the warmer period. The MeHg diffusive fluxes (up to 17 ng m−2 day−1) were similar to those in the nearby Gulf of Trieste [Covelli, S., Horvat, M., Faganeli, J., Brambati, A., 1999. Porewater distribution and benthic flux of mercury and methylmercury in the Gulf of Trieste (Northern Adriatic Sea). Estuar. Coast. Shelf Sci. 48, 415–428], although the lagoon sediments contained four-fold higher THg concentrations. Conversely, the THg diffusive fluxes in the lagoon (up to 110 ng m−2 day−1) were one- to two-fold higher than those previously estimated for the Gulf of Trieste. The diurnal MeHg benthic fluxes were highest in summer at both sites (41,000 and 33,000 ng m−2 day−1 at the fishfarm and in the open lagoon, respectively), thus indicating the influence of temperature on microbial processes. The diurnal variations of dissolved THg and especially MeHg were positively correlated with O2 and inversely with DIC, suggesting an important influence of benthic photosynthetic activities on lagoon benthic Hg cycling, possibly through the production of organic matter promptly available for methylation. The results from the dark chamber incubated in the laboratory showed that the regeneration of dissolved THg was slightly affected by the oxic–anoxic transition. Conversely, the benthic flux of MeHg was up to 15-fold higher in sediments overlain by O2 depleted waters. In the anoxic phase, the MeHg fluxes proceeded in parallel with Fe fluxes and the methylated form reached approximately 100% of dissolved THg. The MeHg is mostly released into overlying water (mean recycling efficiency of 89%) until the occurrence of sulphide inhibition, due to scavenging of the available Hg substrate for methylation. The results suggest that sediments in the Grado Lagoon, especially during anoxic events, should be considered as a primary source of MeHg for the water column.  相似文献   

2.
The Xunyang Hg mine (XMM) situated in Shaanxi Province is an active Hg mine in China. Gaseous elemental Hg (GEM) concentrations in ambient air were determined to evaluate its distribution pattern as a consequence of the active mining and retorting in the region. Total Hg (HgT) and methylmercury (MeHg) concentrations in riparian soil, sediment and rice grain samples (polished) as well as Hg speciation in surface water samples were measured to show local dispersion of Hg contamination. As expected, elevated concentrations of GEM were found, ranging from 7.4 to 410 ng m−3. High concentrations of HgT and MeHg were also obtained in riparian soils, ranged from 5.4 to 120 mg kg−1 and 1.2 to 11 μg kg−1, respectively. Concentrations of HgT and MeHg in sediment samples varied widely from 0.048 to 1600 mg kg−1 and 1.0 to 39 μg kg−1, respectively. Surface water samples showed elevated HgT concentrations, ranging from 6.2 to 23,500 ng L−1, but low MeHg concentrations, ranging from 0.022 to 3.7 ng L−1. Rice samples exhibited high concentrations of 50–200 μg kg−1 in HgT and of 8.2–80 μg kg−1 in MeHg. The spatial distribution patterns of Hg speciation in the local environmental compartments suggest that the XMM is the source of Hg contaminations in the study area.  相似文献   

3.
The Wanshan Hg mining area in Guizhou, China, was one of the world’s largest Hg producing regions. Numerous mine-waste and calcines still remain, leaching Hg to local rivers and streams and potentially impacting the local population. Several studies have been published on local environmental impacts of these mining and retorting residues, but a comprehensive, regional survey on the distribution of Hg in the rivers in the region, as presented in this paper, has not previously been conducted. This study focuses on the regional distribution and temporal variation of aqueous Hg fractions in the five main watercourses draining the Wanshan Hg mining and retorting area, covering more than 700 km2. Three sampling campaigns were carried out in 2007 and 2008, covering high flow, normal flow and low flow periods. Total (THg), particulate (PHg), dissolved (DHg) and reactive (RHg) Hg fractions were determined. All rivers had the highest Hg concentrations at sample sites about 100–500 m downstream of the mine wastes. Total Hg concentrations ranged from extremely high (up to 12,000 ng L−1) at the sample site just 100 m below mine wastes, to quite low in tributary streams (1.9 ng L−1, about 14 km downstream of the mine wastes). Total Hg and PHg concentrations were usually highest during high flow periods in the Hg-contaminated areas (i.e. THg ? 50 ng L−1), while in the less-impacted downstream areas (with THg < 50 ng L−1) the Hg concentrations were usually lowest during high flow periods. Although highly elevated concentrations of Hg in water samples were found just downstream of the mine wastes, the concentrations decreased sharply to well below 50 ng L−1 (US EPA Hg concentration standard for protection of fresh water), within only 6–8 km downstream. Concentrations of THg were highly dominated by and correlated with PHg (R2 = 0.996–0.999, P < 0.001); PHg constituted more than 80% of THg in Hg-contaminated areas, and could account for 99.6% of the THg close to the mine wastes.  相似文献   

4.
Water samples were collected during normal flow (2007) and during a drought period (2008) from five rivers and tributaries draining the Wanshan Hg mining district, Guizhou, China. Unfiltered methylmercury (MeHg) as well as particulate and dissolved fractions of MeHg (P-MeHg, D-MeHg) were measured to assess the spatial and temporal variation of MeHg contamination in the local river system. Most locations (about 80%) displayed higher MeHg concentrations during drought period than during normal discharge conditions. Concentrations of MeHg during the drought period ranged from <0.035 to 11 ng L−1 (geometric mean: 0.43), while during normal flow the concentrations ranged from <0.035 to only 3.4 ng L−1 (geometric mean: 0.21). Concentrations of MeHg were positively correlated with total Hg (THg) concentrations (R2 = 0.20–0.58, P < 0.001) and inversely related to distance from the calcines, during both sampling periods (R2 = 0.34 and 0.23, P < 0.001, for low and normal flow, respectively) indicating that calcines may be important sources of MeHg to the downstream environment. Approximately 39% of MeHg was bound to particulates and the rest was transported in the dissolved phase along stretches of the entire river, which was different from THg, as this was mainly transported bound to particulates (commonly more than 80%).  相似文献   

5.
The River Nura in Central Kazakhstan has been heavily polluted by Hg originating from an acetaldehyde plant. A number of studies were undertaken to investigate the transport, fate and bioavailability of Hg in this river system. The sediments within a 20 km section of the river downstream of the effluent outfall canal are highly polluted and are acting as a strong source of surface water contamination. Mercury transport in the river is dominated by the remobilization of contaminated bed sediments and river bank erosion during the annual spring flood. Peak Hg concentrations in unfiltered surface water samples during a larger than usual flood event in 2004 were in the order of 1600–4300 ng L−1. The majority of the particulate-bound Hg appears to be sedimented in the shallow Intumak reservoir 75 km downstream of the source of the pollution, leading to a drop in aqueous Hg concentrations by an order of magnitude. Nevertheless, background concentrations of Hg in surface water are not reached until at least 200 km downstream, and during the flood period Hg is also detected in the terminal wetlands of the river.Mercury concentrations in sediment cores taken from the river bed in the most contaminated section of the Nura ranged from 9.95 to 306 mg kg−1. Methylmercury (MeHg) levels in shallow sediment cores were highest in surface sediments and ranged between 4.9 and 39 μg kg−1, but were generally less than 0.1% of total Hg (THg). A significant inverse relationship was found between THg concentrations and the percentage of MeHg formed in the sediments, irrespective of the sampling depth. The observed relationship was confirmed by comparison with results from a different river system, indicating that it may be true also for other highly contaminated aquatic systems. It is hypothesized that at high THg levels in severely contaminated sediments, the accumulation of MeHg may be limited by increasingly efficient demethylation processes, and that this underlying trend in sediments is the reason why MeHg levels in surface water are often found to be higher at less contaminated sites compared to upstream sites.Mercury concentrations in biota in the most contaminated section of the river were 15–20 times higher than background levels. Fish were found to be impacted for more than 125 km downstream from the source, indicating significant transport of dissolved MeHg to downstream areas and/or in-situ MeHg production in less contaminated downstream reaches. There were also indications that impoundments may increase the bioavailability of Hg.  相似文献   

6.
Mercury contamination in aquatic environments is of worldwide concern because of its high biomagnification factor in food chains and long-range transport. The rivers, estuary and the bay along the northwestern Bohai Sea coast, northeastern China have been heavily contaminated by Hg due to long-term Zn smelting and chlor-alkali production. This work investigated the distributions of total Hg (THg) and monomethylmercury (MMHg) in the water, sediment and hydrophytes from this area. Concentrations of THg in sediment (0.5–64 mg kg−1) and water (39–2700 ng L−1) were elevated by 1–3 orders of magnitude compared to background concentrations, which induced high concentrations of MMHg in these media. The highest concentration of MMHg in sediment reached 35 μg kg−1, which was comparable to that in the Hg mining area, Wanshan, China, and the highest MMHg concentration of 3.0 ng L−1 in the water sample exceeded the MMHg Chinese drinking water guideline of 1.0 ng L−1. Concentrations of THg in a sediment profile from Jinzhou Bay were found to be consistent with annual Hg emission flux from a local Zn smelter (r = 0.74, p < 0.01), indicating that Hg contamination was mainly caused by Zn smelting locally. For some freshwater hydrophytes, concentrations of THg and MMHg ranged from 5.2 to 100 μg kg−1 and 0.15 to 12 μg kg−1, respectively. Compared to sediment, concentrations of THg in hydrophytes were 2–3 orders of magnitude lower but MMHg was comparable or higher, indicating that the bioaccumulation in plants was distinct for the two Hg species studied. The data suggest that a significant load of Hg has been released into the northwestern coastal region of the Bohai Sea.  相似文献   

7.
Atmospheric mercury deposition on snow at springtime has been reported in polar regions, potentially posing a threat to coastal and inland ecosystems receiving meltwaters. However, the post-depositional fate of Hg in snow is not well known, and no data are available on Hg partitioning in polar snow. During snowmelt, we conducted a survey of Hg concentrations, partitioning and speciation in surface snow and at depth, over sea ice and over land along a 100 km transect across Cornwallis Island, NU, Canada. Total Hg concentrations [THg] in surface snow were low (less than 20 pmol L−1) and were significantly higher in marine vs. inland environments. Particulate Hg in surface snow represented up to 90% of total Hg over sea ice and up to 59% over land. At depth, [THg] at the snow/sea ice interface (up to 300 pmol L−1) were two orders of magnitude higher than at the snow/lake ice interface (ca. 2.5 pmol L−1). Integrated snow columns, sampled over sea-ice and over land, showed that particulate Hg was mostly bound to particles ranging from 0.45 to 2.7 μm. Moreover, melting snowpacks over sea ice and over lake ice contribute to increase [THg] at the water/ice interfaces. This study indicates that, at the onset of snowmelt, most of the Hg in snow is in particulate form, particularly over sea ice. Low Hg levels in surface snow suggest that Hg deposited through early spring deposition events is partly lost to the atmosphere from the snowpack before snowmelt. The sea ice/snow interface may constitute a site for Hg accumulation, however. Further understanding of the cycling of mercury at the sea ice/snow and sea ice/seawater interfaces is thus warranted to fully understand how mercury enters the arctic food webs.  相似文献   

8.
Lake Iso Valkjärvi (southern Finland, Europe) was divided in two with a plastic curtain in 1991. One half was neutralized with CaCO3, and the other acted as a control. Mercury concentrations of perch (Perca fluviatilis) and northern pike (Esox lucius) in the limed and control side of the lake were studied both before and after the treatment. Average Hg concentrations of perch and pike were 0.40 and 1.2 μg g−1 (ww) in the early 1980s and 0.25 and 0.72 μg g−1 (ww) a decade later at the time of liming. Ten years after the liming the Hg concentrations of perch in the limed and control sides of the lake were 0.21 and 0.28 μg g−1 (ww) and those of pike were 0.69 and 0.43 μg g−1 (ww), respectively. Nitrogen isotope ratios (δ15N) for perch in the sampling period 2002–2004 showed wide variation suggesting variable trophic positions for individual fish. Pike formed two groups according to their δ15N-values, suggesting that zoobenthos dominated the diet of pike around 20 cm in length and fish that of the larger pikes. Because the δ15N-values of fish were at similar levels in the limed and control sides of L. Iso Valkjärvi, differences in food web structure cannot account for the different fish Hg concentrations. A more likely explanation is water quality induced differences in the dynamics and bioavailability of Hg, leading to decreased formation of methyl Hg.  相似文献   

9.
Mercury air/surface exchange was measured over litter-covered soils with low Hg concentrations within various types of forests along the eastern seaboard of the USA. The fieldwork was conducted at six forested sites in state parks in South Carolina, North Carolina, New Jersey, Pennsylvania, New York and Maine from mid-May to early June 2005. The study showed that the Hg air/surface exchange was consistently very low and similar (overall daytime mean flux = 0.2 ± 0.9 ng m−2 h−1, n = 310, for all six sites monitored) with the various forest types. These flux values are comparable with those found in a year-long study in Tennessee (yearly daytime mean = 0.4 ± 0.5 ng m−2 h−1), but lower than many previous flux results reported for background soils. The Hg fluxes at all sites oscillated around zero, with many episodes of deposition (negative fluxes) occurring in both daytime and nighttime. While there were particular days showing significant correlations among the Hg air/surface exchange and certain environmental parameters, perhaps because of the low fluxes encountered, few significant correlations were found for any particular day of sampling between the Hg flux and environmental parameters such as solar radiation, soil temperature, air temperature (little variability seen), relative humidity, and ambient air Hg concentrations. Factors driving the Hg exchange as previously found for enriched soils may not hold for these background litter-covered forest soils. The results suggest that spatial variations of the Hg air/surface exchange were small among these different forest types for this particular time of year.  相似文献   

10.
Recent Lake Tanganyika Hg deposition records were derived using 14C and excess 210Pb geochronometers in sediment cores collected from two contrasting depositional environments: the Kalya Platform, located mid-lake and more removed from watershed impacts, and the Nyasanga/Kahama River delta region, located close to the lake’s shoreline north of Kigoma. At the Kalya Platform area, pre-industrial Hg concentrations are 23 ± 0.2 ng/g, increasing to 74 ng/g in modern surface sediment, and the Hg accumulation rate has increased from 1.0 to 7.2 μg/m2/a from pre-industrial to present, which overall represents a 6-fold increase in Hg concentration and accumulation. At the Nyasanga/Kahama delta region, pre-industrial Hg concentrations are 20 ± 3 ng/g, increasing to 46 ng/g in surface sediment. Mercury accumulation rate has increased from 30 to 70 μg/m2/a at this site, representing a 2–3-fold increase in Hg concentration and accumulation. There is a lack of correlation between charcoal abundance and Hg accumulation rate in the sediment cores, demonstrating that local biomass burning has little relationship with the observed Hg concentration or Hg accumulation rates. Examined using a sediment focusing-corrected mass accumulation rate approach, the cores have similar anthropogenic atmospheric Hg deposition profiles, suggesting that after accounting for background sediment concentrations the source of accumulating Hg is predominantly atmospheric in origin. In summary, the data document an increase of Hg flux to the Lake Tanganyika ecosystem that is consistent with increasing watershed sediment delivery with background-level Hg contamination, and regional as well as global increases in atmospheric Hg deposition.  相似文献   

11.
Gaseous elemental mercury (GEM) and reactive gaseous mercury (RGM) were measured over 2-week seasonal field campaigns near Salmon Falls Creek Reservoir in south-central Idaho from the summer of 2005 through the fall of 2006 and over the entire summer of 2006 using automated Tekran Hg analyzers. GEM, RGM, and particulate Hg (HgP) were also measured at a secondary site 90 km to the west in southwestern Idaho during the summer of 2006. The study was performed to characterize Hg air concentrations in the southern Idaho area for the first time, estimate Hg dry deposition rates, and investigate the source of observed elevated concentrations. High seasonal variability was observed with the highest GEM (1.91 ± 0.9 ng m−3) and RGM (8.1 ± 5.6 pg m−3) concentrations occurring in the summer and lower values in the winter (1.32 ± 0.3 ng m−3, 3.2 ± 2.9 pg m−3 for GEM, RGM, respectively). The summer-average HgP concentrations were generally below detection limit (0.6 ± 1 pg m−3). Seasonally averaged deposition velocities calculated using a resistance model were 0.034 ± 0.032, 0.043 ± 0.040, 0.00084 ± 0.0017 and 0.00036 ± 0.0011 cm s−1 for GEM (spring, summer, fall and winter, respectively) and 0.50 ± 0.39, 0.40 ± 0.31, 0.51 ± 0.43 and 0.76 ± 0.57 cm s−1 for RGM. The total annual RGM + GEM dry deposition estimate was calculated to be 11.9 ± 3.3 μg m−2, or about 2/3 of the total (wet + dry) deposition estimate for the area. Periodic elevated short-term GEM (2.2–12 ng m−3) and RGM (50–150 pg m−3) events were observed primarily during the warm seasons. Back-trajectory modeling and PSCF analysis indicate predominant source directions to the SE (western Utah, northeastern Nevada) and SW (north-central Nevada) with fewer inputs from the NW (southeastern Oregon and southwestern Idaho).  相似文献   

12.
The distribution and speciation of mercury (Hg) in the water column, the inputs (wet deposition and tributaries) and the outputs (atmospheric evasion and outlet) of an artificial partially anoxic tropical lake (Petit-Saut reservoir, French Guiana) were investigated on a seasonal basis in order to appraise the cycling and transformations of this metal. The total mercury (HgT) concentrations in the oxygenated epilimnetic waters averaged 5 ± 3 pmol L−1 in the unfiltered samples (HgTUNF) and 4 ± 2 pmol L−1 in the dissolved (HgTD) phase (<0.45 μm). On average, the monomethylmercury (MMHg) constituted 8%, 40% and 18% of the HgT in the dissolved phase, the particulate suspended matter and in the unfiltered samples, respectively. Covariant elevated concentrations of particulate MMHg and chlorophyll a in the epilimnion suggest that phytoplankton is an active component for the MMHg transfer in the lake. In the anoxic hypolimnion the HgTUNF averages 13 ± 6 pmol L−1 and the HgTD 8 ± 4 pmol L−1. The averages of MMHgP and MMHgD in hypolimnetic waters were two and three times the corresponding values of the epilimnion, 170 ± 90 pmol g−1 and 0.9 ± 0.5 pmol L−1, respectively. In the long dry and wet seasons, at the flooded forest and upstream dam sampling stations, the vertical profiles of MMHgD concentrations accounted for two distinct maxima: one just below the oxycline and the other near the benthic interface. Direct wet atmospheric deposition accounted for 14 moles yr−1 HgTUNF, with 0.7 moles yr−1 as MMHgUNF, while circa 76 moles yr−1 of HgTUNF, with 4.7 moles yr−1 as MMHgUNF, coming from tributaries. Circa 78 moles (∼17% as MMHg) are annually exported through the dam, while 23 moles yr−1 of Hg0 evolve in the atmosphere. A mass balance calculation suggests that the endogenic production of MMHgUNF attained 8.1 moles yr−1, corresponding to a methylation rate of 0.06% d−1. As a result, the Petit-Saut reservoir is a large man-made reactor that has extensively altered mercury speciation in favor of methylated species.  相似文献   

13.
《Applied Geochemistry》2006,21(11):1855-1867
Methylmercury (MeHg) and total Hg (THg) concentrations in soil profiles were monitored in the Thur River basin (Alsace, France), where a chlor-alkali plant has been located in the city of Vieux-Thann since the 1930s. Three soil types were studied according to their characteristics and location in the catchment: industrial soil, grassland soil and alluvial soil. Contamination of MeHg and THg in soil was important in the vicinity of the plant, especially in industrial and alluvial soil. Concentrations of MeHg reached 27 ng g−1 and 29,000 ng g−1 for THg, exceeding the predictable no effect concentration. Significant ecotoxicological risk exists in this area and remedial actions on several soil types are suggested. In each type of soil, MeHg concentrations were highest in topsoil, which decreased with depth. Concentrations of MeHg were negatively correlated with soil organic matter and total S, particularly when MeHg concentrations exceeded 8 ng g−1. Under these conditions, MeHg concentrations in soil seemed to be influenced by THg, soil organic matter and total S concentrations. It was found that high MeHg/THg ratios (near 2%) in soil were mainly related to the combined soil environmental conditions such as low THg concentrations, low organic C/N ratios (<11) and relatively low pH (5–5.5). Nevertheless, even when the MeHg/THg ratio was low (∼0.04%), MeHg and THg concentrations were elevated, up to 13 ng g−1 and to 29,000 ng g−1, respectively. Thus, both THg and MeHg concentrations should be taken into account to assess potential environmental risks of Hg.  相似文献   

14.
Mercury (Hg) concentrations and isotopic compositions were examined in shallow-water surface sediment (0-2 cm) from San Francisco (SF) Bay to determine the extent to which historic Hg mining contributes to current Hg contamination in SF Bay, and to assess the use of Hg isotopes to trace sources of contamination in estuaries. Inter-tidal and wetland sediment had total Hg (HgT) concentrations ranging from 161 to 1529 ng/g with no simple gradients of spatial variation. In contrast, inter-tidal and wetland sediment displayed a geographic gradient of δ202Hg values, ranging from −0.30‰ in the southern-most part of SF Bay (draining the New Almaden Hg District) to −0.99‰ in the northern-most part of SF Bay near the Sacramento-San Joaquin River Delta. Similar to SF Bay inter-tidal sediment, surface sediment from the Alviso Slough channel draining into South SF Bay had a δ202Hg value of −0.29‰, while surface sediment from the Cosumnes River and Sacramento-San Joaquin River Delta draining into north SF Bay had lower average δ202Hg values of −0.90‰ and −0.75‰, respectively. This isotopic trend suggests that Hg-contaminated sediment from the New Almaden Hg District mixes with Hg-contaminated sediment from a low δ202Hg source north of SF Bay. Tailings and thermally decomposed ore (calcine) from the New Idria Hg mine in the California Coast Range had average δ202Hg values of −0.37 and +0.03‰, respectively, showing that Hg calcination fractionates Hg isotopes resulting in Hg contamination from Hg(II) mine waste products with higher δ202Hg values than metallic Hg(0) produced from Hg mines. Thus, there is evidence for at least two distinct isotopic signals for Hg contamination in SF Bay: Hg associated with calcine waste materials at Hg mines in the Coast Range, such as New Almaden and New Idria; and Hg(0) produced from these mines and used in placer gold mines and/or in other industrial processes in the Sierra Nevada region and SF Bay area.  相似文献   

15.
Mercury fluxes from air/surface interfaces in paddy field and dry land   总被引：3，自引：0，他引：3  
In order to provide insight into the characteristics of Hg exchange in soil/water-air surface from cropland (including paddy field and dry land), Hg fluxes were measured in Chengjiang. Mercury fluxes were measured using the dynamic flux chamber method, coupled with a Lumex® multifunctional Hg analyzer RA-915+ (Lumex Ltd., Russia). The Hg fluxes from paddy field and dry land were alternatively measured every 30 min. Data were collected for 24-48 h once per month for 5 months. Mercury fluxes in both fields were synchronously measured under the same conditions to compare Hg emissions between paddy field and dry land over diurnal and seasonal periods and find out what factors affect Hg emission on each surface. These results indicated that air Hg concentrations at the monitoring site was double the value observed at the global background sites in Europe and North America. The Hg release fluxes were 46.5 ± 22.8 ng m−2 h−1 in the warm season, 15.5 ± 18.8 ng m−2 h−1 in the cold season for dry land, and 23.8 ± 15.6 ng m−2 h−1 in the warm season, 6.3 ± 11.9 ng m−2 h−1 in the cold season for paddy field. Solar radiation is important in the emission of Hg over both sites. Hg exchange at the soil/air and water/air interfaces showed temporal variations. The amount of Hg emission from dry land was higher than that from the paddy field, and the emission in daytime was higher than that at night. Moreover, Hg emissions from land covered by crops, was lower than that for bare land.  相似文献   

16.
Contaminated fluvial sediments represent both temporary sinks for river-borne pollutants and potential sources in case of natural and/or anthropogenic resuspension. Reservoir lakes play a very important role in sediment dynamics of watersheds and may offer great opportunities to study historical records of river-borne particles and associated elements transported in the past. The fate and potential environmental impact of Hg depends on its abundance, its carrier phases and its chemical speciation. Historical Hg records and solid state Hg speciation were compared in sediments from two contrasting reservoirs of the Lot River (France) upstream and downstream from a major polymetallic pollution (e.g. Cd, Zn) source. Natural (geochemical background) and anthropogenic Hg concentrations and their relationships with predominant carrier phases were determined. The results reveal important historical Hg contamination (up to 35 mg kg−1) of the downstream sediment, reflecting the historical evolution of industrial activity at the point source, i.e. former coal mining, Zn ore treatment and post-industrial remediation work. Single chemical extractions (ascorbate, H2O2, KOH) suggest that at both sites most (∼75%) of the Hg is bound to organic and/or reactive sulphide phases. Organo-chelated (KOH-extracted) Hg, representing an important fraction in the uncontaminated sediment, shows similar concentrations (∼0.02 mg kg−1) at both sites and may be mainly attributed to natural inputs and/or processes. Although, total Hg concentrations in recent surface sediments at both sites are still very different, similar mono-methylmercury concentrations (up to 4 μg kg−1) and vertical distributions were observed, suggesting comparable methylation-demethylation processes. High mono-methylmercury concentrations (4–15 μg kg−1) in 10–40 a-old, sulphide-rich, contaminated sediment suggest long-term persistence of mono-methylmercury. Beyond historical records of total concentrations, the studied reservoir sediments provided new insights in solid state speciation and carrier phases of natural and anthropogenic Hg. In case of sediment resuspension, the major part of the Hg historically stored in the Lot River sediments will be accessible to biogeochemical recycling in the downstream fluvial-estuarine environment.  相似文献   

17.
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18.
《Applied Geochemistry》2006,21(11):1868-1879
Ultra-clean sampling methods and approaches typically used in pristine environments were applied to quantify concentrations of Hg species in water and microbial biomass from hot springs of Yellowstone National Park, features that are geologically enriched with Hg. Microbial populations of chemically-diverse hot springs were also characterized using modern methods in molecular biology as the initial step toward ongoing work linking Hg speciation with microbial processes. Molecular methods (amplification of environmental DNA using 16S rDNA primers, cloning, denatured gradient gel electrophoresis (DGGE) screening of clone libraries, and sequencing of representative clones) were used to examine the dominant members of microbial communities in hot springs. Total Hg (THg), monomethylated Hg (MeHg), pH, temperature, and other parameters influential to Hg speciation and microbial ecology are reported for hot springs water and associated microbial mats.Several hot springs indicate the presence of MeHg in microbial mats with concentrations ranging from 1 to 10 ng g−1 (dry weight). Concentrations of THg in mats ranged from 4.9 to 120,000 ng g−1 (dry weight). Combined data from surveys of geothermal water, lakes, and streams show that aqueous THg concentrations range from l to 600 ng L−1. Species and concentrations of THg in mats and water vary significantly between hot springs, as do the microorganisms found at each site.  相似文献   

19.
Lake Constance is one of Europe’s largest oligotrophic lakes and provides a water source for more than 4.5 million people in Germany and Switzerland. We present here a 12 month study on iodine concentrations, speciation and fluxes to and from the lake to gain a quantitative understanding of the limnic iodine cycle. Monthly water samples were obtained from all major tributaries (14) and the outflow to construct a mass-balance model. Sediment traps were also deployed in the lake for two years at two different stations. Total soluble iodine (TSI) in aqueous samples were analysed by ICP-MS and speciation (iodide, iodate and soluble organically bound iodine, SOI) by ion chromatography-ICP-MS. Iodine concentrations in the Alpine tributaries (1-2 μg l−1) decreased over the summer months due to increasing proportions of snow and glacial melt water from the Alps, while iodine levels in the lowland rivers (∼2-10 μg l−1) increased over the summer. Deposition of TSI to the catchment (16,340 kg I yr−1) was similar to the TSI out-flux by rivers (16,000 kg I yr−1). By also including the particulate riverine iodine flux out of the catchment (∼12,350 kg I yr−1) it is shown that the catchment is a net source of iodine, with the highest particulate fluxes coming from the Alpine rivers. The total TSI flux to the lake was 16,770 kg I yr−1, the largest proportion coming from the Alpenrhein (43%), followed by the Schussen (8%) and Bregenzer Ach (7.7%). Overall the mass-balance for TSI in the lake was negative, with more iodine flowing out of the lake than in (−2050 kg I yr−1; 12% of TSI in-flux). To maintain mass-balance, 8.8 μg I m−2 d−1 from the Obersee and 23 μg I m−2 d−1 from the Untersee must be released from the sediments into the water column. Thus, in comparison with the total iodine flux to the sediments measured by the sediment traps (4762-8075 kg I yr−1), up to 39% of the deposited iodine may be mobilised back into the lake. SOI was the dominant iodine fraction entering the lake, with a total flux of 10,290 kg I yr−1 (64% of TSI input), followed by iodate (3120 kg I yr−1) and iodide (2760 kg I yr−1). Net formation of SOI from iodide and iodate was also noted within the lake, with an estimated production of 6560 kg I yr−1, suggesting a strong role for biology in iodine cycling. In conclusion, organically bound iodine was the dominant iodine species in aqueous and solid phases in Lake Constance, despite low DOC concentrations (<2 mg l−1), and thus is expected to play an important role in iodine cycling in most freshwater environments.  相似文献   

20.
This article presents an analysis of Geological Survey of Canada (GSC) open-file data for total Hg concentrations (THg) in stream and lake sediments at 142,028 sampling locations. This analysis was done for select survey zones across Canada, with emphasis on discerning THg-relevant geographic, geological, atmospheric and topographic controls. THg was generally highest in areas affected by mining and smelting, followed by areas with high metallogenic source locations. Background levels for THg were elevated in the more populated areas along the south, but dropped toward the remote and coldest locations in the east, north and west. This trend was correlated (R2 = 0.74; P < 0.0001) with the 2005 GRAHM projections (Global/Regional Atmospheric Heavy Metals Model) for atmospheric Hg deposition (zones and locations with major geogenic sources and mining activities removed). Mean THg was higher for upland lakes (100.9 ± 0.5 SE, ppb) and streams (71.7 ± 0.6 SE, ppb) than for lowland lakes (94.4 ± 0.86 SE, ppb) and streams (64.2 ± 1.26 SE, ppb). The east-central portion of the Yukon Territory (Selwyn Basin) was analyzed in further detail. Here, THg within the sediments increased with increasing loss-on-ignition and increasing trace-element concentrations, and decreased with an increasing wet-area component per catchment above the sediment sampling locations. The characterization and quantification of these Hg trends is important for modeling and mapping health risks to ecosystems and communities across Canada and elsewhere.  相似文献   

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