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1.
The concentrations of total mercury and methylmercury in sediments were determined at the dam of the Wujiangdu Reservoir in different seasons. Total mercury (HgT) levels in the whole sediment profile were 254.2±47.0 ng/g in winter, 254.2±31.6 ng/g in spring, and 256.7±60.8 ng/g in summer, without significant variations in different seasons or at different depths. In contrast, the methylmercury (MeHg) compounds were most abundant at the sediment-water interface and decreased progressively with depth. MeHg contents of the sediments during different seasons are highly dependent on microbial activity, and seem to be higher when Hg (II)-methylating microorganisms are active. Thus, MeHg levels tend to rise in the loci where nutrient supplies and biological productivity are favorable. The percentage of HgT that is present as MeHg in the sediments increased gradually from December 2003 to April 2004 and to July 2004.  相似文献   

2.
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   

3.
Microbial mercury (Hg) methylation and methylmercury (MeHg) degradation processes were examined using radiolabled model Hg compounds in San Francisco Bay-Delta surface sediments during three seasonal periods: late winter, spring, and fall. Strong seasonal and spatial differences were evident for both processes. MeHg production rates were positively correlated with microbial sulfate reduction rates during late winter only. MeHg production potential was also greatest during this period and decreased during spring and fall. This temporal trend was related both to an increase in gross MeHg degradation, driven by increasing temperature, and to a build-up in pore water sulfide and solid phase reduced sulfur driven by increased sulfate reduction during the warmer seasons. MeHg production decreased sharply with depth at two of three sites, both of which exhibited a corresponding increase in reduced sulfur compounds with depth. One site that was comparatively oxidized and alkaline exhibited little propensity for net MeHg production. These results support the hypothesis that net MeHg production is greatest when and where gross MeHg degradation rates are low and dissolved and solid phase reduced sulfur concentrations are low.  相似文献   

4.
《Applied Geochemistry》2006,21(11):1924-1939
The Idrija Mine, the second largest Hg mine in the world, ceased operation in 1995, but still delivers large quantities of Hg downstream including into the northern Adriatic Sea, 100 km away. Transformation of Hg species in sediment in sites over 60 km from the mine, including marine sites in the Adriatic Sea, was measured to determine the ability of the system to transform and mobilize Hg and to produce methylmercury (MeHg). Cores from a freshwater impoundment, a brackish estuarine site, and three marine sites in the Gulf of Trieste were sectioned anaerobically, and Hg methylation and MeHg demethylation activities determined using radio-techniques (203Hg for methylation and 14C-MeHg for demethylation). Total and dissolved Hg and MeHg were determined as were other geochemical parameters. In addition, rates of SO4 reduction were determined in marine sediment using a 35S technique. Mercury was readily methylated and demethylated at all sites. Marine sediment was investigated in winter and summer with rates of Hg transformation and SO4 reduction corresponding only in winter. Methylation of Hg in summer displayed subsurface peaks that may have been influenced by bioturbation. Total Hg and MeHg were most abundant in the freshwater, estuarine, and near-shore marine sites, but dissolved pore water Hg and MeHg were highest in the estuarine region where S cycling appeared ideal for the mobilization of Hg. The impoundment sediment also seemed to be a ‘hotspot’ of Hg transformations. MeHg demethylation occurred via the oxidative demethylation pathway (CO2 produced from MeHg), except in surficial sediment offshore in the Gulf during winter, where sediment was more oxidizing and significant amounts of CH4 were liberated during MeHg degradation via reductive demethylation. The CH4 formation was likely due to an increased influence from the expression of MeHg degradative enzymes encoded by the mer detoxification bacterial genetic system. The freshwater site also liberated CH4 from MeHg, but it appeared to be due to oxidative demethylation by methanogenic bacteria.  相似文献   

5.
In this paper, the relationship between sulfate reduction potential and mercury methylation potential was studied in the Aha, Baihua and Hongfeng reservoirs from Guiyang City. The methylmercury (MeHg) concentrations of lake water in the Aha Reservoir were greatly elevated as compared to those of the Hongfeng and Baihua reservoirs, which was correlated with its distinctly high SRB abundance, SO42-, and S2- concentrations. Among the three reservoirs, however, the highest MeHg was observed in in the top several centimenters of pore water profile in the Hongfeng Reservoir where the lowest S2- in pore water occurred. The distributions of MeHg in lake water and pore water showed the highest methylation potential occurred at water-sediment surface for the Aha Reservoir and the in the top several centimenters of sediments for the Hongfeng Reservoir. It is guessed that the highest mercury methylation only occurs at the sites with certain sulfide concentrations.  相似文献   

6.
Karen A. Merritt  Aria Amirbahman   《Earth》2009,96(1-2):54-66
Considerable recent research has focused on methylmercury (MeHg) cycling within estuarine and coastal marine environments. Because MeHg represents a potent neurotoxin that may magnify in marine foodwebs, it is important to understand the mechanisms and environmental variables that drive or constrain methylation dynamics in these environments. This critical review article explores the mechanisms hypothesized to influence aqueous phase and sediment solid phase MeHg concentrations and depth-specific inorganic Hg (II) (Hgi) methylation rates (MMR) within estuarine and coastal marine environments, and discusses issues of terminology or methodology that complicate mechanism-oriented interpretation of field and laboratory data. Mechanisms discussed in this review article include: 1) the metabolic activity of sulfate reducing bacteria (SRB), the microbial group thought to dominate mercury methylation in these environments; 2) the role that Hgi concentration and/or speciation play in defining depth-specific Hgi methylation rates; and 3) the depth-dependent balance between MeHg production and consumption within the sedimentary environment. As discussed in this critical review article, the hypothesis of SRB community control on the Hgi methylation rate in estuarine and coastal marine environments is broadly supported by the literature. Although Hgi speciation, as a function of porewater inorganic sulfide and/or dissolved organic matter concentration and/or pH, may also play a role in observed variations in MMR, the nature and function of the controlling ligand(s) has not yet been adequately defined. Furthermore, although it is generally recognized that the processes responsible for MeHg production and consumption overlap spatially and/or kinetically in the sedimentary environment, and likely dictate the extent to which MeHg accumulates in the aqueous and/or sediment solid phase, this conceptual interpretation requires refinement, and would benefit greatly from the application of kinetic modeling.  相似文献   

7.
The Delaware River Estuary (DRE) is a cornerstone of industrialization, shipping, and urban usage, and has a long history of human impact on pollution and recovery. Mercury (Hg) is a contaminant of concern in the DRE based upon concentrations in some fish samples that were found to exceed State and Federal fish tissue criteria. Methylation of Hg often follows a seasonal pattern as its production is biologically mediated. Surveys were conducted in November 2011, April 2012, and July 2012 to assess this effect. We sampled surface and bottom water at six sites spanning the estuarine turbidity maximum (ETM) in the main channel of the river, plus three sediment sites at shallow, subtidal locations. Our results indicate there is a clear seasonal increase in both water column and sediment methylmercury (MeHg) and %MeHg concentrations in the ETM during July. Water-column-filtered total mercury (HgT), suspended particle HgT, and MeHg concentrations were found to fluctuate little with location or season in the ETM. In contrast, sediment MeHg, water-column-filtered MeHg, and pore water HgT varied seasonally. Furthermore, pore water MeHg levels were elevated in concert with increased k meth rates in July. Estimated river input and sediment and atmospheric depositional MeHg flux were compared seasonally. River flux was more than an order of magnitude higher than sediment flux in April, coinciding with higher fluvial transport. However, during July, river flux decreases and sediment flux becomes a larger relative source. This trend has potential implications for fish and other biota residing in the DRE during summer.  相似文献   

8.
In order to find out whether Aha Lake was polluted by the acid mining waste water or not, the concentration and distribution of different mercuryspecies in the water columns and sediment profile collected from Aha Lake were investigated. It was found that discernible seasonal variation of different mercury species in water body were obtained in the Aha Reservoir. With regards to the whole sampling periods, the concentrations of HgP in the Aha Reservoir water body were evidently correlated to the concentrations of total mercury, showing that total mercury was mostly associated with particle mercury. The concentrations of methylmercury in water body were also evidently correlated to the concentrations of dissolved mercury. The dissolved mercury evidently affects the distribution and transportation of methylmercury. However, there is no correlation between methylmercury and total mercury. The dissolved mercury, reactive mercury, dissolved methylmercury levels in the water body of high flow period were much higher than those in low flow period. The distribution, speciation and levels of mercury within the Aha Reservoir water body were governed by several factors, such as the output of river, the release of sediment . Discernible seasonal variation of total mercury and methylmercury in porewater was described during the sampling periods, with the concentrations in high flow period generally higher than those in low flow period. The methylmercury in pore water column was evidently correlated to that of the sediment. The results indicated that highly elevated MeHgD concentrations in the porewater were produced at the depths from 2 to 5 cm in the sediment profile, and decreased sharply with depth. A positive correlation has been found between MeHgD formation and sulfate reducing bacterial activity. These highly elevated concentrations of MeHgD at the intersurface between waters and sediments suggest a favorable methylation condition. Moreover,  相似文献   

9.
San Pablo Bay is an estuary, within northern San Francisco Bay, containing elevated sediment mercury (Hg) levels because of historic loading of hydraulic mining debris during the California gold-rush of the late 1800s. A preliminary investigation of benthic microbial Hg cycling was conducted in surface sediment (0-4 cm) collected from one salt-marsh and three open-water sites. A deeper profile (0-26 cm) was evaluated at one of the open-water locations. Radiolabeled model Hg-compounds were used to measure rates of both methylmercury (MeHg) production and degradation by bacteria. While all sites and depths had similar total-Hg concentrations (0.3-0.6 ppm), and geochemical signatures of mining debris (as )Nd, range: -3.08 to -4.37), in-situ MeHg was highest in the marsh (5.4Dž.5 ppb) and А.7 ppb in all open-water sites. Microbial MeHg production (potential rate) in 0-4 surface sediments was also highest in the marsh (3.1 ng g-1 wet sediment day-1) and below detection (<0.06 ng g-1 wet sediment day-1) in open-water locations. The marsh exhibited a methylation/demethylation (M/D) ratio more than 252 that of all open-water locations. Only below the surface 0-4-cm horizon was significant MeHg production potential evident in the open-water sediment profile (0.2-1.1 ng g-1 wet sediment day-1). In-situ Hg methylation rates, calculated from radiotracer rate constants, and in-situ inorganic Hg(II) concentrations compared well with potential rates. However, similarly calculated in-situ rates of MeHg degradation were much lower than potential rates. These preliminary data indicate that wetlands surrounding San Pablo Bay represent important zones of MeHg production, more so than similarly Hg-contaminated adjacent open-water areas. This has significant implications for this and other Hg-impacted systems, where wetland expansion is currently planned.  相似文献   

10.
The first advisory to limit consumption of Florida Bay fish due to mercury was issued in 1995. Studies done by others in the late 1990s found elevated water column concentrations of both total Hg (THg) and methylmercury (MeHg) in creeks discharging from the Everglades, which had its own recognized mercury problem. To investigate the significance of allochthonous MeHg discharging from the upstream freshwater Everglades, we collected surface water and sediment along two transects from 2000 to 2002. Concentrations of THg and MeHg, ranging from 0.36 ng THg/L to 5.98 ng THg/L and from <0.02 ng MeHg/L to 1.79 ng MeHg/L, were elevated in the mangrove transition zone when compared both to upstream canals and the open waters of Florida Bay. Sediment concentrations ranged from 5.8 ng THg/g to 145.6 ng THg/g and from 0.05 ng MeHg/g to 5.4 ng MeHg/g, with MeHg as a percentage of THg occasionally elevated in the open bay. Methylation assays indicated that sediments from Florida Bay have the potential to methylate Hg. Assessment of mass loading suggests that canals delivering stormwater from the northern Everglades are not as large a source as direct atmospheric deposition and in situ methylation, especially within the mangrove transition zone.  相似文献   

11.
We present here the first mercury speciation study in the water column of the Southern Ocean, using a high-resolution south-to-north section (27 stations from 65.50°S to 44.00°S) with up to 15 depths (0-4440 m) between Antarctica and Tasmania (Australia) along the 140°E meridian. In addition, in order to explore the role of sea ice in Hg cycling, a study of mercury speciation in the “snow-sea ice-seawater” continuum was conducted at a coastal site, near the Australian Casey station (66.40°S; 101.14°E). In the open ocean waters, total Hg (HgT) concentrations varied from 0.63 to 2.76 pmol L−1 with “transient-type” vertical profiles and a latitudinal distribution suggesting an atmospheric mercury source south of the Southern Polar Front (SPF) and a surface removal north of the Subantartic Front (SAF). Slightly higher mean HgT concentrations (1.35 ± 0.39 pmol L−1) were measured in Antarctic Bottom Water (AABW) compared to Antarctic Intermediate water (AAIW) (1.15 ± 0.22 pmol L−1). Labile Hg (HgR) concentrations varied from 0.01 to 2.28 pmol L−1, with a distribution showing that the HgT enrichment south of the SPF consisted mainly of HgR (67 ± 23%), whereas, in contrast, the percentage was half that in surface waters north of PFZ (33 ± 23%). Methylated mercury species (MeHgT) concentrations ranged from 0.02 to 0.86 pmol L−1. All vertical MeHgT profiles exhibited roughly the same pattern, with low concentrations observed in the surface layer and increasing concentrations with depth up to an intermediate depth maximum. As for HgT, low mean MeHgT concentrations were associated with AAIW, and higher ones with AABW. The maximum of MeHgT concentration at each station was systematically observed within the oxygen minimum zone, with a statistically significant MeHgTvs Apparent Oxygen Utilization (AOU) relationship (p < 0.001). The proportion of HgT as methylated species was lower than 5% in the surface waters, around 50% in deep waters below 1000 m, reaching a maximum of 78% south of the SPF. At Casey coastal station HgT and HgR concentrations found in the “snow-sea ice-seawater” continuum were one order of magnitude higher than those measured in open ocean waters. The distribution of HgT there suggests an atmospheric Hg deposition with snow and a fractionation process during sea ice formation, which excludes Hg from the ice with a parallel Hg enrichment of brine, probably concurring with the Hg enrichment of AABW observed in the open ocean waters. Contrastingly, MeHgT concentrations in the sea ice environment were in the same range as in the open ocean waters, remaining below 0.45 pmol L−1. The MeHgT vertical profile through the continuum suggests different sources, including atmosphere, seawater and methylation in basal ice. Whereas HgT concentrations in the water samples collected between the Antarctic continent and Tasmania are comparable to recent measurements made in the other parts of the World Ocean (e.g., Soerensen et al., 2010), the Hg species distribution suggests distinct features in the Southern Ocean Hg cycle: (i) a net atmospheric Hg deposition on surface water near the ice edge, (ii) the Hg enrichment in brine during sea ice formation, and (iii) a net methylation of Hg south of the SPF.  相似文献   

12.
Concentrations of total Hg in sediments near six drilling sites in the Gulf of Mexico were elevated well above average background values of 40–80 ng/g. The excess Hg was associated with barite from discharged drilling mud. In contrast with total Hg, concentrations of methylmercury (MeHg) in these sediments did not vary significantly at nearfield (<100 m) versus farfield (>3 km) distances from the drilling sites. Observed variability in concentrations of MeHg were related to local differences in redox state in the top 10 cm of sediment. Low to non-detectable concentrations of MeHg were found in nearfield sediments that were anoxic, highly reducing and contained abundant H2S. At most drilling sites, nearfield samples with high concentrations of total Hg (>200 ng/g) had similar or lower amounts of MeHg than found at background (farfield) stations. Higher values of MeHg were found in a few nearfield sediments at one site where concentrations of TOC were higher and where sediments were anoxic and moderately reducing. Overall, results from this study support the conclusion that elevated concentrations of MeHg in sediments around drilling sites are not a common phenomenon in the Gulf of Mexico.  相似文献   

13.
为了弄清楚普定水库汞的地球化学循环特征,用金汞齐-冷原子荧光光谱法(CVAFS)和气相色谱技术(GC), 研究了乌江流域上游普定水库水体剖面和沉积物间隙水剖面汞的赋存形态(总汞 THg)、溶解态汞(DHg)、活性汞(RHg)、颗粒态汞(PHg)、总甲基汞(TMeHg)、溶解态甲基汞(DMeHg)和颗粒态甲基汞(PMeHg)的分布特征.结果显示,普定水库水体总汞浓度为1.29～3.18 ng/L, 活性汞浓度为0.09～0.43 ng/L, 总甲基汞浓度为0.06～0.18 ng/L.沉积物间隙水中溶解态汞浓度为2.65 ～11.47 ng/L, 溶解态甲基汞浓度为0.06 ～1.16 ng/L.实验数据表明,普定水库水体中溶解态汞和颗粒态含量相当,其中颗粒态汞占总汞的比例为46%,并与总汞存在极显著相关性(R=0.929,n=20,P＜0.01),溶解态汞与总汞相关性不明显(R=-0.067,n=20);冬季普定水库甲基汞以溶解态甲基汞为主,溶解态甲基汞占总甲基汞的比例为63%,溶解态甲基汞与总甲基汞无明显相关关系(R=0.292,n=20),颗粒态甲基汞与总甲基汞存在极显著的相关性(R=0.815,n=20,P＜0.01).试验数据表明沉积物孔隙水溶解态汞与溶解态甲基汞浓度明显高于上覆水体, 是普定水库水体中汞的一个重要来源.  相似文献   

14.
Samples of authigenic material, sediment overlying water and oxic surface sediment (0–0.5-cm depth) from a perennially oxygenated lacustrine basin were analysed to investigate which solid phases are important for binding a suite of trace elements (Ag, As, Ca, Cd, Cu, Hg, In, methylmercury (MeHg), Mg, Mo, Pb, Sb and Zn). The authigenic material, which was collected with inert Teflon sheets deployed for several years across the sediment–water interface, contained mainly poorly crystallized Fe oxyhydroxides and natural organic matter, presumably humic substances derived from the watershed. Manganese oxyhydroxides were not present in the collected authigenic material due to the slightly acidic condition (pH = 5.6) of the lake that prevents the formation and recycling of these compounds. Conditional equilibrium constants for the adsorption of cationic (KFe–M) and anionic (KFe–A) trace elements onto the authigenic Fe oxyhydroxides were estimated from their concentrations in the authigenic material and in bottom water samples. These field-derived values of KFe–M and KFe–A were compared with those predicted by the surface complexation model, using laboratory-derived intrinsic adsorption constants and the water composition at the study site. Equilibrium constants (KPOM–M) were also calculated for the adsorption of the cationic trace elements onto the humic substances contained in the diagenetic material. The field-derived values of KPOM–M were compared to those predicted by the speciation code WHAM 6 for the complexation of the trace elements by dissolved humic substances in the lake. Combining the results of the present study with those on the distributions of trace elements in the porewater and solid-phase sediments reported in previous studies at the same site, it was determined whether the trace elements bind preferentially to Fe oxyhydroxides or natural organic matter in oxic sediments. The main inferences are that the anionic trace elements As, Mo and Sb, as well as the cationic metal Pb are preferentially bound to the authigenic Fe oxyhydroxides whereas the other trace elements, and especially Hg and MeHg, are preferentially bound to the humic substances.  相似文献   

15.
A mass-flow event triggered by the 1996 flood in the Saguenay region buried the mercury-contaminated indigenous sediments at the head of the Saguenay Fjord under up to 50 cm of postglacial deltaic sediments. The vertical distributions of total mercury and methyl-mercury in the sediments and pore waters were measured in box cores recovered from the Saguenay Fjord within and outside the affected area prior to and on six consecutive years after the flood. The total solid mercury (THgs) profiles show that remobilization was limited and most of the mercury remobilized from the contaminated, indigenous sediments was trapped below or slightly above the former sediment–water interface by authigenic acid-volatile sulfides (AVS). Nonetheless, a small fraction of the remobilized mercury diffused into the flood layer, some of it was methylated and/or scavenged by organic matter and AVS. Elevated solid-phase methyl-mercury concentrations, [MeHgs], at depth in the sediment are correlated to peak AVS and THgs but, in the absence of elevated dissolved methyl-mercury concentrations, [MeHgd], the higher [MeHgs] may reflect an earlier episode of Hg methylation, the product of which was scavenged by the AVS and buried. Throughout the sediment cores, sediment–water partitioning of MeHg and Hg(II) appears to be controlled in great part by the AVS and residual organic matter content of the sediment.  相似文献   

16.
Uranium geochemistry has been investigated in three acid lakes located on the Canadian Shield and one circumneutral lake in the Appalachian Region of Eastern Canada. In all Shield lakes, dissolved U concentrations were higher in the porewater than in the overlying water. In one of them, whose hypolimnion is perennially oxic, U released to porewater at depths of Fe remobilization was removed from the porewater at depths of Fe oxyhydroxides precipitation; these similarities in the U and Fe profiles indicate that part of the U becomes associated to Fe oxyhydroxides. The dissolved U and Fe profiles in the other two Shield lakes, whose hypolimnions were anoxic when sampled, did not show any significant recycling of these elements in the vicinity of the sediment-water interface and both elements diffused from the sediment to the overlying water. In contrast, in the Appalachian Lake, dissolved U concentrations were higher in the overlying water than in porewater, strongly decreased at the vicinity of the sediment-water interface and then remained relatively constant with sediment depth. Diagenetic modeling of the porewater U profiles, assuming steady-state, reveals that authigenic U always represented ?3% of the total U concentration in the sediments of all lakes. This observation indicates that diagenetic reactions involving U are not quantitatively important and that most of the U was delivered to the sediments at our study sites as particulate U and not through diffusion across the sediment-water interface, as is seen in continental margin sediments. Comparison of the U:Corg and U:Fe molar ratios in diagenetic material collected across the sediment-water interface with Teflon sheets and in surface sediments (0-0.5 cm) of the lake having a perennially oxic hypolimnion suggest that solid phase U was mainly bound to organic matter originating from the watershed; a strong statistical correlation between sediment non-lithogenic U and Corg in the Appalachian Lake supports this contention. Thermodynamic calculations of saturation states suggest that dissolved U was not removed from porewater through precipitation of UO2(s), U3O7(s) and U3O8(s) as previously proposed in the literature.  相似文献   

17.
The Wabigoon River (Ontario, Canada) was affected by dams starting in 1898 and was polluted with pulp and paper mill wastes starting in 1913 and mercury from a chlor-alkali plant from 1962 to 1975. A dated sediment core from a riverine lake was analysed to investigate resultant changes in the biogeochemistry of mercury as revealed by variations in mercury isotope ratios and sediment chemistry. A total mercury maximum formed by the mercury pollution coincided with minimums in the δ-values of the 198Hg/202Hg, 199Hg/202Hg, 200Hg/202Hg, and 201Hg/202Hg ratios, and the δ-values decreased in the order δ201Hg > δ200Hg > δ199Hg > δ198Hg. Thus, mass-dependent fractionation caused depletion in lighter isotopes, implying evaporation of Hg(0) and pollution of the atmosphere as well as the river-lake system. Concurrently, mass-independent fractionation caused 199Hg enrichment, possibly reflecting an independently documented upsurge in methylmercury production, and 201Hg depletion, suggesting removal of methylmercury with anomalously high 201Hg/199Hg ratios by aquatic organisms and accumulation of 201Hg-depleted inorganic Hg(II) in sediments. The δ201Hg/δ199Hg ratio rose abruptly when mercury pollution began, reflecting the resultant increase in methylmercury production, and remained high but gradually declined as the pollution abated, paralleling trends shown by methylmercury in aquatic organisms. The δ201Hg/δ199Hg ratio of pre-1962 background mercury increased ca. 1898 and ca. 1913–1929, suggesting accelerated methylmercury production due to stimulation of microbial activities by the damming of the river and the input of pulp and paper mill wastes, respectively. Other variations were linked to economic and technological factors that affected pulp and paper manufacture.  相似文献   

18.
Two sampling campaigns were carried out in March and August 2005 representing dry and wet seasons, respectively, to investigate the distribution patterns of Hg species in the water column and sediment profiles at two sampling stations in Aha Reservoir located in Guiyang, Southwestern China. Aha Reservoir has been contaminated by Hg due to small scale coal mining activities. Mercury concentrations in both water and sediment were elevated. A clearly seasonal variation of dissolved Hg (DHg), particulate Hg (PHg) and total Hg (THg) concentrations in the water column was observed. The concentrations of these Hg species in the wet season were significantly higher than in the dry season. Runoff input and diffusion of Hg from sediments could be the reasons for elevated concentrations of these Hg species in the wet season. The contaminated sediment is acting as a secondary contamination source for both inorganic Hg (IHg) and methylmercury (MeHg) to the overlying water. The cycling of Mn in the sediment governs the diffusion process of IHg to the water column. In the dry season (winter and spring), Mn occurs as MnO2 because the uppermost part of sediment is in an oxic condition and Hg ions are absorbed by MnO2. In the wet season (summer and fall), the uppermost part of the sediment profile is in a reduced condition because of stratification of the water column and MnO2 is reduced to Mn2+, which results in transformation of Hg2+ into porewater as Mn2+ became soluble. This causes a higher diffusive flux of IHg from sediment to overlying water in the wet season. Both sampling stations showed a consistent trend that THg concentrations decreased in the uppermost part of sediment cores. This demonstrated that the measures taken to reduce ADM contamination to Aha Reservoir also reduced Hg input to the reservoir. Methyl Hg diffusive fluxes from sediment to overlying water were higher in the wet season than the dry season demonstrating that high temperatures favor Hg methylation processes in sediment.  相似文献   

19.
《Applied Geochemistry》2006,21(11):2010-2022
This work focuses on two possible sources of Hg in tropical soils, (i) lithogenic Hg from in situ weathering of soil parental material, and (ii) exogenic Hg from natural long-term atmospheric inputs and anthropogenic input from past and present industrial activities. The concentration of lithogenic Hg [Hg]lithogenic was based on comparison of measured Hg concentration with those of elements resistant to weathering such as Nb, U, Zn, Fe. Exogenic Hg was quantified by subtracting [Hg]lithogenic from total Hg concentrations. This calculation was applied to 4 French Guiana soil profiles, 3 profiles on the same toposequence (ferralsol, acrisol, hydromorphic soil) and one acrisol close to a Au mine, where elemental Hg is used. In all profiles, [Hg]lithogenic varied slightly and was always below 40 μg kg−1, whereas [Hg]exogenic varied considerably and reached 500 μg kg−1. The highest [Hg]exogenic was calculated for the upper horizon of the acrisol close to Au mining activity, but also in the ferralsol. Concentrations of Hg were insignificant in the compact alterite in acrisols. It was concluded that pedogenesis processes that affect the natural Hg supply, combined with anthropogenic sources, explain the Hg concentrations in these tropical soils.  相似文献   

20.
Spatial variation in mercury (Hg) and methylmercury (MeHg) bioaccumulation in urban coastal watersheds reflects complex interactions between Hg sources, land use, and environmental gradients. We examined MeHg concentrations in fauna from the Delaware River estuary, and related these measurements to environmental parameters and human impacts on the waterway. The sampling sites followed a north to south gradient of increasing salinity, decreasing urban influence, and increasing marsh cover. Although mean total Hg in surface sediments (top 4 cm) peaked in the urban estuarine turbidity maximum and generally decreased downstream, surface sediment MeHg concentrations showed no spatial patterns consistent with the examined environmental gradients, indicating urban influence on Hg loading to the sediment but not subsequent methylation. Surface water particulate MeHg concentration showed a positive correlation with marsh cover whereas dissolved MeHg concentrations were slightly elevated in the estuarine turbidity maximum region. Spatial patterns of MeHg bioaccumulation in resident fauna varied across taxa. Small fish showed increased MeHg concentrations in the more urban/industrial sites upstream, with concentrations generally decreasing farther downstream. Invertebrates either showed no clear spatial patterns in MeHg concentrations (blue crabs, fiddler crabs) or increasing concentrations further downstream (grass shrimp). Best-supported linear mixed models relating tissue concentration to environmental variables reflected these complex patterns, with species specific model results dominated by random site effects with a combination of particulate MeHg and landscape variables influencing bioaccumulation in some species. The data strengthen accumulating evidence that bioaccumulation in estuaries can be decoupled from sediment MeHg concentration, and that drivers of MeHg production and fate may vary within a small region.  相似文献   

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