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1.
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   

2.
Zinc smelting and chlor-alkali production are major sources of Hg contamination to the environment, potentially leading to serious impacts on the health of the local population. Huludao, NE China has been heavily contaminated by Hg due to long-term Zn smelting and chlor-alkali production. The aim of this work was to determine Hg accumulation in the aquatic and terrestrial environment, as well as in the human population of Huludao. The investigation included: (a) Hg accumulation in sediments, Spirogyra algae, crucian carp and shrimp, (b) Hg distribution in soil, vegetables and corn, and (c) assessment of potential health effects of Hg exposure associated with total Hg (T-Hg) concentrations in human hair. Measured T-Hg concentrations in sediments of Wuli River ranged from 0.15 to 15.4 mg kg−1, with the maximum Hg concentration in sediment exceeding the background levels in Liaoning Province by 438 times. The maximum T-Hg levels in Spirogyra, crucian carp and shrimp were 13.6, 0.36, and 0.44 mg kg−1, respectively. Total-Hg concentrations in hair of the human population varied from 0.05 to 3.25 mg kg−1 (average 0.43 mg kg−1). However, the frequency of paraesthesia to most inhabitants in Huludao was estimated to be lower than 5%, with only one person rated at 50%. The results indicated minimal adverse health effects of Hg exposure to the inhabitants of Huludao, despite the serious Hg contamination of the environment.  相似文献   

3.
Mining/smelting wastes and reservoir sediment cores from the Lot River watershed were studied using mineralogical (XRD, SEM–EDS, EMPA) and geochemical (redox dynamics, selective extractions) approaches to characterize the main carrier phases of trace metals. These two approaches permitted determining the role of post-depositional redistribution processes in sediments and their effects on the fate and mobility of trace metals. The mining/smelting wastes showed heterogeneous mineral compositions with highly variable contents of trace metals. The main trace metal-bearing phases include spinels affected by secondary processes, silicates and sulfates. The results indicate a clear change in the chemical partitioning of trace metals between the reservoir sediments upstream and downstream of the mining/smelting activities, with the downstream sediments showing a 2-fold to 5-fold greater contribution of the oxidizable fraction. This increase was ascribed to stronger post-depositional redistribution of trace metals related to intense early diagenetic processes, including dissolution of trace metal-bearing phases and precipitation of authigenic sulfide phases through organic matter (OM) mineralization. This redistribution is due to high inputs (derived from mining/smelting waste weathering) at the water–sediment interface of (i) dissolved SO4 promoting more efficient OM mineralization, and (ii) highly reactive trace metal-bearing particles. As a result, the main trace metal-bearing phases in the downstream sediments are represented by Zn- and Fe-sulfides, with minor occurrence of detrital zincian spinels, sulfates and Fe-oxyhydroxides. Sequestration of trace metals in sulfides at depth in reservoir sediments does not represent long term sequestration owing to possible resuspension of anoxic sediments by natural (floods) and/or anthropogenic (dredging, dam flush) events that might promote trace metal mobilization through sulfide oxidation. It is estimated that, during a major flood event, about 870 t of Zn, 18 t of Cd, 25 t of Pb and 17 t of Cu could be mobilized from the downstream reservoir sediments along the Lot River by resuspension-induced oxidation of sulfide phases. These amounts are equivalent to 13-fold (Cd), ∼6-fold (Zn), 4-fold (Pb) the mean annual inputs of the respective dissolved trace metals into the Gironde estuary.  相似文献   

4.
《Applied Geochemistry》2006,21(3):515-527
Dissolved and particulate Hg fluxes in the Lot–Garonne–Gironde fluvial-estuarine system were obtained from observation of daily discharge and suspended particulate matter (SPM) concentrations. In addition to the measurements of the total dissolved (<0.45 μm) and particulate Hg (>0.45 μm), called HgTD and HgTP respectively, the dissolved inorganic Hg species (HgRD) were determined monthly. Geochemical background values for HgTP in sediments and SPM were similar to crustal values and to typical concentrations in SPM of non-contaminated river systems, respectively. The Riou Mort watershed already known as the origin of important historical polymetallic (e.g., Cd, Zn) pollution was identified as an important Hg point source. In the downstream Lot River, Hg concentrations were clearly higher than those in other moderately contaminated systems. The mean relative contribution of HgRD to HgTD in the Lot River and in the Garonne River was close to 25% and 50%, respectively, and showed no correlation with water discharge or SPM concentration. Depending on the origin and nature of SPM, HgTP concentrations were correlated or not with particulate organic C (POC). Maximum HgTP concentrations were measured in samples containing low POC concentrations and were attributed to sediment resuspension. In contrast, high POC concentrations (6–17%) during algal blooms were associated with low/moderate HgTP concentrations (<0.5 mg kg−1) at different sites, suggesting that Hg concentrations in fluvial phytoplankton may be limited by bioavailability of dissolved Hg and/or physiologically controlled Hg accumulation. Mercury was mostly (up to 98%) transported in the particulate phase with estimated annual Hg fluxes at the outlet of the Lot River system ranging from 35 to 530 kg a−1 for the past decade. The minimum anthropogenic component (58–84% of total Hg fluxes) could not be explained by present Riou Mort point source contributions, suggesting important Hg release from contaminated sediment as a major source and from downstream point sources (e.g., coal-fired power plants and/or metal processing industries). HgTP concentrations and fluxes were strongly related to hydrologic variations and were clearly increased by riverbed dredging during lock construction. Therefore, the estimated Hg stocks in the Lot River sediment (5–13 tons) represent an important potential Hg source for the downstream fluvial-estuarine system.  相似文献   

5.
Groundwater and sediment samples (∼ 1 m depth) at sites representative of different groundwater pathways were collected to determine the aqueous speciation of sulfur and the fractionation of sulfur isotopes in aqueous and solid phases. In addition, selected sediment samples at 5 depths (from oxic to anoxic layers) were collected to investigate the processes controlling sulfur biogeochemistry in sedimentary layers. Pyrite was the dominant sulfur-bearing phase in the capillary fringe and groundwater zones where anoxic conditions are found. Low concentrations of pyrite (< 5.9 g kg− 1) coupled with high concentrations of dissolved sulfide (4.81 to 134.7 mg L− 1) and low concentrations of dissolved Fe (generally < 1 mg L− 1) and reducible solid-phase Fe indicate that availability of reactive Fe limits pyrite formation. The relative uniformity of down-core isotopic trends for sulfur-bearing mineral phases in the sedimentary layers suggests that sulfate reduction does not result in significant sulfate depletion in the sediment. Sulfate availability in the deeper sediments may be enhanced by convective vertical mixing between upper and lower sedimentary layers due to evaporative concentration. The large isotope fractionation between dissolved sulfate and sedimentary sulfides at Owens Lake provides evidence for initial fractionation from bacterial sulfate reduction and additional fractionation generated by sulfide oxidation followed by disproportionation of intermediate oxidation state sulfur compounds. The high salinity in the Owens Lake brines may be a factor controlling sulfate reduction and disproportionation in hypersaline conditions and results in relatively constant values for isotope fractionation between dissolved sulfate and total reduced sulfur.  相似文献   

6.
Sediments from the Aquia aquifer in coastal Maryland were collected as part of a larger study of As in the Aquia groundwater flow system where As concentration are reported to reach levels as high as 1072 nmol kg−1, (i.e., ∼80 μg/L). To test whether As release is microbially mediated by reductive dissolution of Fe(III) oxides/oxyhydroxides within the aquifer sediments, the Aquia aquifer sediment samples were employed in a series of microcosm experiments. The microcosm experiments consisted of sterilized serum bottles prepared with aquifer sediments and sterilized (i.e., autoclaved), artificial groundwater using four experimental conditions and one control condition. The four experimental conditions included the following scenarios: (1) aerobic; (2) anaerobic; (3) anaerobic + acetate; and (4) anaerobic + acetate + AQDS (anthraquinone-2,6-disulfonic acid). AQDS acts as an electron shuttle. The control condition contained sterilized aquifer sediments kept under anaerobic conditions with an addition of AQDS. Over the course of the 27 day microcosm experiments, dissolved As in the unamended (aerobic and anaerobic) microcosms remained constant at around ∼28 nmol kg−1 (2 μg/L). With the addition of acetate, the amount of As released to the solution approximately doubled reaching ∼51 nmol kg−1 (3.8 μg/L). For microcosm experiments amended with acetate and AQDS, the dissolved As concentrations exceeded 75 nmol kg−1 (5.6 μg/L). The As concentrations in the acetate and acetate + AQDS amended microcosms are of similar orders of magnitude to As concentrations in groundwaters from the aquifer sediment sampling site (127-170 nmol kg−1). Arsenic concentrations in the sterilized control experiments were generally less than 15 nmol kg−1 (1.1 μg/L), which is interpreted to be the amount of As released from Aquia aquifer sediments owing to abiotic, surface exchange processes. Iron concentrations released to solution in each of the microcosm experiments were higher and more variable than the As concentrations, but generally exhibited similar trends to the As concentrations. Specifically, the acetate and acetate + AQDS amended microcosm typically exhibited the highest Fe concentrations (up to 1725 and 6566 nmol kg−1, respectively). The increase in both As and Fe in the artificial groundwater solutions in these amended microcosm experiments strongly suggests that microbes within the Aquia aquifer sediments mobilize As from the sediment substrate to the groundwaters via Fe(III) reduction.  相似文献   

7.
The concentrations of Re, as well as those of several other geochemical variables, were measured in dated sediment cores and in porewater samples from four lacustrine basins in Eastern Canada: one, perennially oxic, located 40 km from Québec City and three, seasonally anoxic, located within 25 km of non-ferrous metal smelters. The drainage basins of these lakes are uninhabited and have not been affected by human activity or wildfires. All of the depth profiles of dissolved Re indicate: higher Re concentrations in the water overlying the sediment than in the porewater; diffusion of Re across the sediment-water interface; a progressive decrease in porewater Re concentrations to reach minimum values of ∼0.5 pM within a 10-cm sediment depth interval. Modeling of these Re porewater profiles with a one-dimensional transport-reaction equation indicates that Re is removed from porewater within this depth interval. Based on thermodynamic predictions of Re speciation and of saturation states and on comparison of these predictions with sulfide porewater profiles, we infer that Re is removed from porewater by precipitation of rheniite (ReS2(s)). The rate constant for the formation of ReS2(s) in sediments is estimated from the modeling exercise to be 0.51 ± 0.64 × 10−21 mol cm−3 s−1. Accumulation of sedimentary Re shows a strong authigenic component, as in anoxic marine sediments. Sharp increases in solid-phase Re during the last century are attributed to atmospheric deposition of anthropogenic Re deriving from coal burning and nearby smelter emissions.  相似文献   

8.
Waters from abandoned Sb-Au mining areas have higher Sb (up to 2138 μg L−1), As (up to 1252 μg L−1) and lower Al, Zn, Li, Ni and Co concentrations than those of waters from the As-Au mining area of Banjas, which only contain up to 64 μg L−1 As. In general, Sb occurs mainly as SbO3− and As H2AsO4−. In general, waters from old Sb-Au mining areas are contaminated in Sb, As, Al, Fe, Cd, Mn, Ni and NO2−, whereas those from the abandoned As-Au mining area are contaminated in Al, Fe, Mn, Ni, Cd and rarely in NO2−. Waters from the latter area, immediately downstream of mine dumps are also contaminated in As. In stream sediments from Sb-Au and As-Au mining areas, Sb (up to 5488 mg kg−1) and As (up to 235 mg kg−1) show a similar behaviour and are mainly associated with the residual fraction. In most stream sediments, the As and Sb are not associated with the oxidizable fraction, while Fe is associated with organic matter, indicating that sulphides (mainly arsenopyrite and pyrite) and sulphosalts containing those metalloids and metal are weathered. Arsenic and Sb are mainly associated with clay minerals (chlorite and mica; vermiculite in stream sediments from old Sb-Au mining areas) and probably also with insoluble Sb phases of stream sediments. In the most contaminated stream sediments, metalloids are also associated with Fe phases (hematite and goethite, and also lepidocrocite in stream sediments from Banjas). Moreover, the most contaminated stream sediments correspond to the most contaminated waters, reflecting the limited capacity of stream sediments to retain metals and metalloids.  相似文献   

9.
We measured the vertical distributions of Mo, Fe, Mn, sulfide, sulfate, organic carbon, major ions, and pH in sediment porewater from one perennially oxic and three seasonally anoxic lacustrine basins in Eastern Canada, as well as those of Mo, acid volatile sulfide, Fe, Mn, Al, organic C, 210Pb and 137Cs in sediment cores from the same sites. The only input of anthropogenic Mo to these lakes comes from atmospheric deposition.The relatively monotonous distribution of Mo in the porewater of three seasonally anoxic basins suggests that Mo is not redistributed in the sedimentary column during periods of anoxia. In contrast, porewater Mo profiles obtained at three sampling dates in a perennially oxic basin display sharp Mo peaks below the sediment-water interface, indicating redistribution subsequent to deposition. Modeling of these latter porewater Mo profiles with a diagenetic reaction-transport equation coupled to comparisons among the various porewater and solid phase profiles reveal that Mo is released at 1-2 cm depth as a consequence of the reductive dissolution of Fe oxyhydroxides and scavenged both at the vicinity of the sediment-water interface, by re-adsorption onto authigenic Fe oxyhydroxides, and deeper in the sediments where dissolved sulfide concentrations are higher. The estimated rate constant for the adsorption of Mo onto Fe oxyhydroxides is 36 ± 45 cm3 mol−1 s−1.Diagenetic modeling indicates that authigenic Mo in sediments of the perennially oxic basin represents about one-third of the total solid phase Mo in the first cm below the sediment-water interface and only one tenth below this horizon. If we assume that no authigenic Mo is accumulated in the seasonally anoxic lake sediments we conclude that the sediment Mo concentrations, which are up to 3-16 times higher than the average lithogenic composition, depending on the lake, are mainly due to atmospheric deposition of anthropogenic Mo and not to the formation of authigenic Mo phases. Reconstructed historical records of the atmospheric Mo deposition indicate maximum values in the 1970s and 1980s and significant decreases since then. Emissions to the atmosphere associated with the smelting of non-ferrous ores and coal combustion appear to be the most important sources of anthropogenic Mo.  相似文献   

10.
We re-evaluate the cycling of molybdenum (Mo) and rhenium (Re) in the near-surface environment. World river average Mo and Re concentrations, initially based on a handful of rivers, are calculated using 38 rivers representing five continents, and 11 of 19 large-scale drainage regions. Our new river concentration estimates are 8.0 nmol kg−1 (Mo), and 16.5 pmol kg−1 (Re, natural + anthropogenic). The linear relationship of dissolved Re and in global rivers (R2 = 0.76) indicates labile continental Re is predominantly hosted within sulfide minerals and reduced sediments; it also provides a means of correcting for the anthropogenic contribution of Re to world rivers using independent estimates of anthropogenic sulfate. Approximately 30% of Re in global rivers is anthropogenic, yielding a pre-anthropogenic world river average of 11.2 pmol Re kg−1. The potential for anthropogenic contribution is also seen in the non-negligible Re concentrations in precipitation (0.03-5.9 pmol kg−1), and the nmol kg−1 level Re concentrations of mine waters. The linear Mo- relationship (R2 = 0.69) indicates that the predominant source of Mo to rivers is the weathering of pyrite. An anthropogenic Mo correction was not done as anthropogenically-influenced samples do not display the unambiguous metal enrichment observed for Re. Metal concentrations in high temperature hydrothermal fluids from the Manus Basin indicate that calculated end-member fluids (i.e. Mg-free) yield negative Mo and Re concentrations, showing that Mo and Re can be removed more quickly than Mg during recharge. High temperature hydrothermal fluids are unimportant sinks relative to their river sources 0.4% (Mo), and 0.1% (pre-anthropogenic Re). We calculate new seawater response times of 4.4 × 105 yr (τMo) and 1.3 × 105 yr (τRe, pre-anthropogenic).  相似文献   

11.
To understand the geochemical cycle of Hg in hypereutrophic freshwater lake, two sampling campaigns were conducted in Lake Taihu in China during May and September of 2009. The concentrations of unfiltered total Hg (unfTHg) were in the range of 6.8–83 ng L−1 (28 ± 18 ng L−1) in the lake water and total Hg in the sediment was 12–470 ng g−1, both of which are higher than in other background lakes. The concentration of unfTHg in ∼11% of the lake water samples exceeded the second class of the Chinese environmental standards for surface water of 50 ng L−1 (GB 3838-2002), indicating that a high ecological risk is posed by the Hg in Lake Taihu. However, the concentrations of unfiltered total MeHg (unfMeHg) were relatively low in the lake water (0.14 ± 0.05 ng L−1, excluding two samples with 0.81 and 1.0 ng L−1). Lake sediment MeHg varied from 0.2–0.96 ng g−1, with generally low ratios of MeHg/THg of <1%. The low concentrations of TMeHg in the lake water may have resulted from a strong uptake by the high primary productivity and the demethylation of MeHg in oxic conditions. In addition, contrary to the results of previous research conducted in deep-water lakes and reservoirs, the low concentrations of MeHg and low ratio of MeHg/THg in the lake sediment indicates that the net methylation of Hg was not accelerated by the elevated organic matter load created by the eutrophication of Lake Taihu. The results also showed that sediments were a source of THg and MeHg in the water. Higher diffusion fluxes of THg and MeHg may be partly responsible for the higher concentrations of THg in the lake water in May, 2009.  相似文献   

12.
Exposure of humans to monomethylmercury (MMHg) occurs primarily through consumption of marine fish, yet there is limited understanding concerning the bioaccumulation and biogeochemistry of MMHg in the biologically productive coastal ocean. We examined the cycling of MMHg in sediments at three locations on the continental shelf of southern New England in September 2003. MMHg in surface sediments is related positively to inorganic Hg (Hg(II) = total Hg − MMHg), the geographical distribution of which is influenced by organic material. Organic matter also largely controls the sediment-water partitioning of Hg species and governs the availability of dissolved Hg(II) for methylation. Potential gross rates of MMHg production, assayed by experimental addition of 200Hg to intact sediment cores, are correlated inversely with the distribution coefficient (KD) of Hg(II) and positively with the concentration of Hg(II), most probably as HgS0, in 0.2-μm filtered pore water of these low-sulfide deposits. Moreover, the efflux of dissolved MMHg to overlying water (i.e., net production at steady state) is correlated with the gross potential rate of MMHg production in surface sediments. These results suggest that the production and efflux of MMHg from coastal marine sediments is limited by Hg(II), loadings of which presumably are principally from atmospheric deposition to this region of the continental shelf. The estimated diffusive flux of MMHg from the shelf sediments averages 9 pmol m−2 d−1. This flux is comparable to that required to sustain the current rate of MMHg accumulation by marine fish, and may be enhanced by the efflux of MMHg from near-shore deposits contaminated more substantially with anthropogenic Hg. Hence, production and subsequent mobilization of MMHg from sediments in the coastal zone may be a major source of MMHg to the ocean and marine biota, including fishes consumed by humans.  相似文献   

13.
Two sediment cores retrieved at the northern slope of Sakhalin Island, Sea of Okhotsk, were analyzed for biogenic opal, organic carbon, carbonate, sulfur, major element concentrations, mineral contents, and dissolved substances including nutrients, sulfate, methane, major cations, humic substances, and total alkalinity. Down-core trends in mineral abundance suggest that plagioclase feldspars and other reactive silicate phases (olivine, pyroxene, volcanic ash) are transformed into smectite in the methanogenic sediment sections. The element ratios Na/Al, Mg/Al, and Ca/Al in the solid phase decrease with sediment depth indicating a loss of mobile cations with depth and producing a significant down-core increase in the chemical index of alteration. Pore waters separated from the sediment cores are highly enriched in dissolved magnesium, total alkalinity, humic substances, and boron. The high contents of dissolved organic carbon in the deeper methanogenic sediment sections (50-150 mg dm−3) may promote the dissolution of silicate phases through complexation of Al3+ and other structure-building cations. A non-steady state transport-reaction model was developed and applied to evaluate the down-core trends observed in the solid and dissolved phases. Dissolved Mg and total alkalinity were used to track the in-situ rates of marine silicate weathering since thermodynamic equilibrium calculations showed that these tracers are not affected by ion exchange processes with sediment surfaces. The modeling showed that silicate weathering is limited to the deeper methanogenic sediment section whereas reverse weathering was the dominant process in the overlying surface sediments. Depth-integrated rates of marine silicate weathering in methanogenic sediments derived from the model (81.4-99.2 mmol CO2 m−2 year−1) are lower than the marine weathering rates calculated from the solid phase data (198-245 mmol CO2 m−2 year−1) suggesting a decrease in marine weathering over time. The production of CO2 through reverse weathering in surface sediments (4.22-15.0 mmol CO2 m−2 year−1) is about one order of magnitude smaller than the weathering-induced CO2 consumption in the underlying sediments. The evaluation of pore water data from other continental margin sites shows that silicate weathering is a common process in methanogenic sediments. The global rate of CO2 consumption through marine silicate weathering estimated here as 5-20 Tmol CO2 year−1 is as high as the global rate of continental silicate weathering.  相似文献   

14.
Lead concentrations and isotopic composition of sediment samples collected from three sites within the Lebanese coastal zones were measured: at Akkar, Dora and Selaata. Akkar is located far from any direct source of contamination, while Dora and Selaata receive urban and industrial wastes, respectively. Low Pb concentrations (6–16 μg g−1) were detected in the Akkar sediments, and high concentrations of Pb (70–101 μg g−1) were detected in the Dora sediments. Measuring stable isotope ratios of Pb makes it possible to identify the principal sources of Pb in the Akkar sediments as Pb emitted from gasoline combustion and Pb originating from natural sources. On the other hand, Pb stable isotopic ratios in Dora sediments indicate that they are more highly influenced by anthropogenic sources. Isotopic Pb ratios in the Selaata deposits, where Pb concentrations range between 5 and 35 μg g−1, have an exceptional radiogenic signature for marine sediments 1.25 < 206Pb/207Pb < 1.6 and 0.5 < 206Pb/208Pb < 0.67, which shows the impact of the phosphogypsum discharged by Selaata’s chemical plant. Isotopic Pb analysis applied to EDTA extracts, to test the mobility of Pb, shows that that this mobility is high (>60%) after 24 h of extraction, and that the extracted Pb is less radiogenic than the residual Pb.  相似文献   

15.
Sixty five urban road dust samples were collected from different land use areas of ∼240 km2 in Xi’an, China. The concentrations of Ag, As, Cr, Cu, Hg, Pb, Sb and Zn were determined to investigate potentially harmful element (PHE) contamination, distribution and possible sources. In addition, the concentrations in different size fractions were measured to assess their potential impact on human health. The highest concentrations were found in the fraction with particle diameters between 80 μm and 101 μm, the finest particles (<63 μm) were not the most important carriers for Ag, As, Cd, Cr, Cu, Hg, Pb and Zn. The percentages of these elements in particles with diameters less than 63 μm (PM63) and less than 101 μm (PM101) were in the range of 7–15%, and 30–55%, respectively. Three main factors influencing element distributions have been identified: (a) industrial activities; (b) prior agricultural land use; and (c) other activities commonly found in urban areas, such as traffic, coal combustion, waste dumping, and building construction/renovation. The highest concentrations were found in industrial areas for As (20 mg kg−1), Cr (853 mg kg−1), Cu (1071 mg kg−1), Pb (3060 mg kg−1) and Zn (2112 mg kg−1), and in previous agricultural areas for Ag and Hg, indicating significant contributions from industrial activities and prior agricultural activities.  相似文献   

16.
At a watershed scale, sediments and soil weathering exerts a control on solid and dissolved transport of trace elements in surface waters and it can be considered as a source of pollution. The studied subwatershed (1.5 km2) was located on an As-geochemical anomaly. The studied soil profile showed a significant decrease of As content from 1500 mg kg−1 in the 135–165 cm deepest soil layer to 385 mg kg−1 in the upper 0–5 cm soil layer. Directly in the stream, suspended matter and the <63 μm fraction of bed sediments had As concentrations greater than 400 mg kg−1. In all these solid fractions, the main representative As-bearing phases were determined at two different observation scales: bulk analyses using X-ray absorption structure spectroscopy (XAS) and microanalyses using scanning electron microscope (SEM) and associated electron probe microanalyses (EPMA), as well as micro-Raman spectroscopy and synchrotron-based micro-scanning X-ray diffraction (μSXRD) characterization. Three main As-bearing phases were identified: (i) arsenates (mostly pharmacosiderite), the most concentrated phases As in both the coherent weathered bedrock and the 135–165 cm soil layer but not observed in the river solid fraction, (ii) Fe-oxyhydroxides with in situ As content up to 15.4 wt.% in the deepest soil layer, and (iii) aluminosilicates, the least concentrated As carriers. The mineralogical evolution of As-bearing phases in the soil profile, coupled with the decrease of bulk As content, may be related to pedogenesis processes, suggesting an evolution of arsenates into As-rich Fe-oxyhydroxides. Therefore, weathering and mineralogical evolution of these As-rich phases may release As to surface waters.  相似文献   

17.
The shallow aquifer beneath the Western Snake River Plain (Idaho, USA) exhibits widespread elevated arsenic concentrations (up to 120 μg L−1). While semi-arid, crop irrigation has increased annual recharge to the aquifer from approximately 1 cm prior to a current rate of >50 cm year−1. The highest aqueous arsenic concentrations are found in proximity to the water table (all values >50 μg L−1 within 50 m) and concentrations decline with depth. Despite strong vertical redox stratification within the aquifer, spatial distribution of aqueous species indicates that redox processes are not primary drivers of arsenic mobilization. Arsenic release and transport occur under oxidizing conditions; groundwater wells containing dissolved arsenic at >50 μg L−1 exhibit elevated concentrations of O2 (average 4 mg L−1) and NO3 (average 8 mg L−1) and low concentrations of dissolved Fe (<20 μg L−1). Sequential extractions and spectroscopic analysis of surficial soils and sediments indicate solid phase arsenic is primarily arsenate and is present at elevated concentrations (4–45 mg kg−1, average: 17 mg kg−1) relative to global sedimentary abundances. The highest concentrations of easily mobilized arsenic (up to 7 mg kg−1) are associated with surficial soils and sediments visibly stained with iron oxides. Batch leaching experiments on these materials using irrigation waters produce pore water arsenic concentrations approximating those observed in the shallow aquifer (up to 152 μg L−1). While As:Cl aqueous phase relationships suggest minor evaporative enrichment, this appears to be a relic of the pre-irrigation environment. Collectively, these data indicate that infiltrating irrigation waters leach arsenic from surficial sediments to the underlying aquifer.  相似文献   

18.
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   

19.
To establish a natural background and its temporal and spatial variability for the area around Casey Station in the Windmill Islands, East Antarctica, the authors studied major and trace element concentrations and the distribution of organic matter in marine and lacustrine sediments. A wide range of natural variability in trace metal concentrations was identified between sites and within a time scale of 9 ka (e.g., Ni 5–37 mg kg−1, Cu 20–190 mg kg−1, Zn 50–300 mg kg−1, Pb 4.5–34 mg kg−1). TOC concentrations are as high as 3 wt.% at the marine sites and 20 wt.% at the lacustrine sites, and indicate highly productive ecosystems. These data provide a background upon which the extent of human impact can be established, and existing data indicate negligible levels of disturbance. Geochemical and lithological data for a lacustrine sediment core from Beall Lake confirm earlier interpretation of recent climatic changes based on diatom distribution, and the onset of deglaciation in the northern part of the Windmill Islands between 8.6 and 8.0 ka BP. The results demonstrate that geochemical and lithological data can not only be used to define natural background values, but also to assess long-term climatic changes of a specific environment. Other sites, however, preserve a completely different sedimentary record. Therefore, inferred climatic record, and differences between sites, can be ascribed to differences in elevation, distance from the shore, water depth, and local catchment features. The extreme level of spatial variability seems to be a feature of Antarctic coastal areas, and demonstrates that results obtained from a specific site cannot be easily generalized to a larger area.  相似文献   

20.
The distribution, partition and speciation of mercury (Hg) were studied along the redox gradient of an anthropogenically perturbed tropical estuary, the Sinnamary Estuary in French Guiana. This system is a partially mixed estuary characterized by an anoxic freshwater end-member, while the marine end-member consists of the Amazon Plume.The set up of an artificial oxygenation system in the anoxic freshwater end-member generates sharp gradients of major chemical species (iron, sulfides, etc.) coupled with intense organic matter (OM) turnover. The coexistence of oxygenated waters and dissolved sulfides in an organic rich environment depicts the Upper Sinnamary Estuary (USE: part of Sinnamary Estuary under the tidal influence but upstream of the salt intrusion) as a potential site for Hg methylation. The concentrations of all mercury compounds (HgT) in the unfiltered samples (HgTUNF), in the dissolved (HgTD) and particulate (HgTP) phases of the USE average 11 ± 3, 6 ± 2 and 5 ± 3 (i.e. 600 ± 200 pmol g−1) pmol L−1, respectively. Average concentrations of monomethylmercury (MMHg) in the unfiltered (MMHgUNF), dissolved (MMHgD) and particulate (MMHgP) phases were 3.7 ± 1.0, 2.0 ± 0.9 and 1.8 ± 1.2 (i.e. 220 ± 130 pmol g−1) pmol L−1, respectively. Water oxygenation and sulfides concentrations emerged to play a critical role in controlling MMHg levels. Additionally, iron cycling, acid-base mechanisms, and redox-dependent processes were involved in the MMHg partitioning between phases.Overall, the USE constitutes a biogeochemical reactor that gathers partitioning and methylation processes. The permanent MMHg inputs from the anoxic freshwater end-member combined with the intense endogenous Hg methylation ensures high-MMHg levels in both dissolved and particulate phases. To illustrate, the USE exports 60 ± 20% more MMHgUNF than it imports: 5.5 ± 0.7 vs. 3.5 ± 1.2 kg year−1.  相似文献   

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