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1.
Controlling bioaccumulation of toxic monomethylmercury (MMHg) in aquatic food chains requires differentiation between biotic and abiotic pathways that lead to its production and degradation. Recent mercury (Hg) stable isotope measurements of natural samples suggest that Hg isotope ratios can be a powerful proxy for tracing dominant Hg transforming pathways in aquatic ecosystems. Specifically, it has been shown that photo-degradation of MMHg causes both mass dependent (MDF) and mass independent fractionation (MIF) of Hg isotopes. Because the extent of MDF and MIF observed in natural samples (e.g., fish, soil and sediments) can potentially be used to determine the relative importance of pathways leading to MMHg accumulation, it is important to determine the potential role of microbial pathways in contributing to the fractionation, especially MIF, observed in these samples. This study reports the extent of fractionation of Hg stable isotopes during degradation of MMHg to volatile elemental Hg and methane via the microbial Hg resistance (mer) pathway in Escherichia coli carrying a mercury resistance (mer) genetic system on a multi-copy plasmid. During experimental microbial degradation of MMHg, MMHg remaining in reactors became progressively heavier (increasing δ202Hg) with time and underwent mass dependent Rayleigh fractionation with a fractionation factor α202/198 = 1.0004 ± 0.0002 (2SD). However, MIF was not observed in any of the microbial MMHg degradation experiments indicating that the isotopic signature left by mer mediated MMHg degradation is significantly different from fractionation observed during DOC mediated photo-degradation of MMHg. Additionally, a clear suppression of Hg isotope fractionation, both during reduction of Hg(II) and degradation of MMHg, was observed when the cell densities increased, possibly due to a reduction in substrate bioavailability. We propose a multi-step framework for understanding the extent of fractionation seen in our MMHg degradation experiments and, based on estimates of the rates of the various steps involved in this mer mediated pathway, suggest which steps in the process could contribute towards the observed extent of fractionation. This framework suggests that at lower cell densities catalysis by MerB was the rate limiting step while at higher cell densities transport into the cell, which does not cause fractionation, became the rate limiting step. In addition to presenting evidence for absence of MIF during mer mediated Hg transformations, based on the nature of Hg compounds and microbe-Hg interactions, we suggest that the nuclear spin dependent MIF (i.e., the magnetic isotope effect) is also unlikely to occur during other non mer mediated ‘dark’ microbial Hg transformations (e.g., formation of MMHg and oxidative degradation of MMHg). Because of the important implications of the absence of MIF during biological processes on Hg isotope systematics, we discuss theoretical considerations and experimental strategies that could be used to confirm this suggestion.  相似文献   

2.
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   

3.
We examined the hydroclimatic signal in a record of annual lamina (varve) thickness from High Arctic Lake A, Ellesmere Island (83°00.00′N, 75°30.00′W). In this unglacierized catchment, nival melt is the dominant source for meltwater and transport of sediment to the lake, and autumn snowfall is highly influential on varve thickness through the amount of snow available for melt in the following year. For the period during which climatic data are available, varve thickness in Lake A was significantly correlated (r = 0.50, p < 0.01) with the cumulative snowfall from August to October (ASO) during the previous year and, to a lesser extent, ASO mean daily temperature (r = 0.39, p < 0.01) at Alert, Nunavut (175 km east). The varve thickness record, interpreted as a proxy record of ASO snowfall and, by extension, ASO temperature, indicated above-mean conditions during five periods of the past millennium, including most of the 20th century. These results corresponded well to other available high-resolution proxy climate records from the region, with some discrepancies prior to AD 1500 and during the period AD 1700-1900.  相似文献   

4.
基于2012年消融期6~9月在祁连山老虎沟12号冰川采集冰川融水径流样品,分析探讨冰川融水中粉尘颗粒物对融水理化性质的影响。结果表明,粉尘特征在消融期的变化很好地反映了冰川消融过程,融水中粉尘浓度和粒径众数在冰川强烈消融期的7月份表现为最高。粉尘体积粒径分布主要包括大气气溶胶超细颗粒（0~3.0 μm,主要为PM 2.5）,大气粉尘颗粒（3.0~20 μm）,以及局地源的粗颗粒（20~100 μm）;对雪冰消融释放的粉尘部分（3.0~20 μm）粒径分布正态拟合结果说明,融水中粉尘颗粒物有很大部分来源于积雪中的粉尘运移所致。同时,融水中化学离子相对组成及其浓度消融期变化都与粉尘有较好的一致性,意味着粉尘对融水化学要素有重要影响。此外,pH值和电导率（EC）消融期的变化也反映了粉尘对融水物理指标的影响。在粉尘浓度较高时,融水pH值和电导率也表现出高值;融水径流中的悬移质颗粒物（SPM）浓度和溶解质固体（TDS）浓度具有较为一致的变化过程,反映了粉尘对于融水中溶解质含量也有较大影响。  相似文献   

5.
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   

6.
Globally, the ongoing retreat of mountain glaciers will ultimately diminish fresh water supplies. This has already begun in watersheds with greatly reduced glacial coverage. Still unknown are the affects of glacial retreat on downstream water quality, including the threats to human and ecosystem health. In the Cordillera Blanca, retreating glaciers have exposed sulfide-rich rock outcrops, negatively affecting the quality of the glacial meltwater. This study has evaluated glacial melt stream hydrogeochemistry in the sulfide-bearing Rio Quilcay watershed (∼9°27′S, ∼77°22′W) during the 2008 dry season. Surface water samples were collected from the upper 12 km of the watershed during the 2008 dry season. Dissolved (0.4 μm) and unfiltered acidified (pH < 2) Al, Co, Cu, Fe, Ni, Mn, Pb, Zn and dissolved major ions and organic C (DOC) concentrations were quantified and pH and temperature were measured in the field. Twenty of 22 stream samples had pH values below 4, generating significantly (p < 0.01, α = 0.05) greater cation denudation normalized to discharge than other worldwide glacier-fed streams. Additionally, dissolved trace and minor element concentrations were comparable to acid mine drainage. Non-conservative dissolved element behaviors resulted from adsorption/desorption reactions in tributary mixing zones. At low pH values, hydrous Fe oxides acted as the dominant sorption surfaces. The poor water quality observed in Cordillera Blanca headwaters coupled with the likely exposure of additional sulfide-rich outcrops from ongoing glacial retreat may pose water quality challenges.  相似文献   

7.
Spatial variations of δD and δ18O among seven tributaries and their water sources were investigated in the Heishui Valley of the Yangtze River, China during the dry-season in 2004. A one-way ANOVA (analysis of variation) test showed that both δD (p?18O (p?=?0.045) spatially varied among the seven tributaries. The plot of δ18O versus δD for the river water collected at different locations showed that isotopic fractionation occurred during the snow and glacial melting process. The depleted δ18O and δD in the tributary waters distributed above the local meteoric water line (LMWL) suggested that the glacial and early snowpack meltwater largely recharged these streams during the early spring. The meltwater was isotopically distinguishable from the precipitation and river water, which had been evaporated during warmer and drier times. If glaciers and snow accumulation diminish with future climate warming, the recharge of these tributaries’ baseflow will decline and the security of the water resource in this watershed will be threatened.  相似文献   

8.
Atmospheric mercury (Hg) is delivered to ecosystems via rain, snow, cloud/fog, and dry deposition. The importance of snow, especially snow that has passed through the forest canopy (throughfall), in delivering Hg to terrestrial ecosystems has received little attention in the literature. The snowpack is a dynamic system that links atmospheric deposition and ecosystem cycling through deposition and emission of deposited Hg. To examine the magnitude of Hg delivery via snowfall, and to illuminate processes affecting Hg flux to catchments during winter (cold season), Hg in snow in no-canopy areas and under forest canopies measured with four collection methods were compared: (1) Hg in wet precipitation as measured by the Mercury Deposition Network (MDN) for the site in Acadia National Park, Maine, USA, (2) event throughfall (collected after snowfall cessation for accumulations of >8 cm), (3) season-long throughfall collected using the same apparatus for event sampling but deployed for the entire cold season, and (4) snowpack sampling. Estimates (mean ± SE) of Hg deposition using these methods during the 91-day cold season in 2004–2005 at conifer sites showed that season-long throughfall Hg flux (1.80 μg/m2) < snowpack Hg (2.38 ± 0.68 μg/m2) < event throughfall flux (5.63 ± 0.38 μg/m2). Mercury deposition at the MDN site (0.91 μg/m2) was similar to that measured at other no-canopy sites in the area using the other methods, but was 3.4 times less than was measured under conifer canopies using the event sampling regime. This indicates that snow accumulated under the forest canopy received Hg from the overstory or exhibited less re-emission of Hg deposited in snow relative to open areas. The soil surface of field-scale plots were sprayed with a natural rain water sample that contained an Hg tracer (202Hg) just prior to the first snowfall to explore whether some snowpack Hg might be explained from soil emissions. The appearance of the 202Hg tracer in the snowpack (0–64% of the total Hg mass in the snowpack) suggests that movement of Hg from the soil into the snowpack is possible. However, as with any tracer study the 202Hg tracer may not precisely represent the reactivity and mobility of natural Hg in soils.  相似文献   

9.
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   

10.
This study describes time series analysis of snow-melt, radiation data and energy balance for a seasonal snow cover at Dhundi field station of SASE, which lies in Pir Panjal range of the N-W Himalaya, for a winter season from 13 January to 12 April 2005. The analysis shows that mean snow surface temperature remains very close to the melting temperature of snow. It was found close to −1°C for the complete observational period which makes the snow pack at Dhundi moist from its beginning. The average air temperature over this period was found to be 3.5°C with hourly average variation from −5.5°C to 13°C. The snow surface at this station received a mean short wave radiation of 430W m−2, out of which 298W m−2 was reflected back by the snow surface with mean albedo value of 0.70. The high average temperature and more absorption of solar radiation resulted in higher thermal state of the snowpack which was further responsible for faster and higher densification of the snowpack. Net radiation energy was the major component of surface energy budget with a mean value of 83W m−2. Bulk transfer model was used to calculate turbulent fluxes. The net energy was utilized for satisfying cold content and snow-melt by using measured snow surface temperature and density of snow pack. The mean square error between calculated and measured daily snow-melt was found to be approximately 6.6mm of water equivalent.  相似文献   

11.
乌鲁木齐河流域季节积雪的基本特征   总被引：5，自引：0，他引：5  
张志忠  杨大庆 《冰川冻土》1992,14(2):129-133
  相似文献   

12.
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   

13.
The fate of the Rare Earth Elements (REE) were investigated in different types of archives of atmospheric deposition in the Black Forest, Southern Germany: (1) a 70 cm snow pack collected on the domed part of a raised bog and representing 2 months of snow accumulation, (2) a snow sample collected close to the road about 500 m from the peat bog, (3) two species of lichens and (4) a peat profile representing 400 years of peat accumulation as well as a “preanthropogenic” sample and the living moss layer from the top of the core. REE concentrations in peat are significantly correlated to Ti which is a lithogenic conservative element suggesting that REE are immobile in peat bog environments. Snow, lichens and peat samples show similar PAAS (Post Archean Australian Shale) normalized REE distributions suggesting that the complete atmospheric REE signal is preserved in the peat profile. However, the annual flux of REE accumulated by the peat is ca. 10 times greater than that of the bulk winter flux of REE. This difference probably indicates that the REE concentrations in the snowpack are not representative of the average REE flux over the whole year. Despite the pronounced geological differences between this site (granite host-rock) and a previously studied peat bog in Switzerland (limestone host-rock) similar REE distribution patterns and accumulation rates were found at both sites. Given that both sites confirm an Upper Continental Crust signature, the data suggests both sites are influenced by regional and not local, soil-derived lithogenic aerosols.  相似文献   

14.
Snow was sampled and analyzed for total mercury (THg) on the Idaho National Engineering and Environmental Laboratory (INEEL) and surrounding region prior to the start-up of a large (9-11 g/h) gaseous mercury emission source. The objective was to determine the effects of the source on local and regional atmospheric deposition of mercury. Snow samples collected from 48 points on a polar grid near the source had THg concentrations that ranged from 4.71 to 27.26 ng/L; snow collected from regional background sites had THg concentrations that ranged from 0.89 to 16.61 ng/L. Grid samples had higher concentrations than the regional background sites, which was unexpected because the source was not operating yet. Emission of Hg from soils is a possible source of Hg in snow on the INEEL. Evidence from Hg profiles in snow and from unfiltered/filtered split samples supports this hypothesis. Ongoing work on the INEEL is investigating Hg fluxes from soils and snow.  相似文献   

15.
The occurrence of wet-snow avalanches is, in general, poorly understood. For 20 years (winters of 1975–1976 to 1994–1995), the avalanche activity has been observed in the Dischma valley near Davos (Eastern Swiss Alps). The study area comprises a large starting zone of north-easterly aspect (2,300 m a.s.l.) with several avalanche paths. We have analyzed the occurrence data in combination with meteorological and snowpack data collected at an elevation of 2,090 m a.s.l. During the 20-year observation period, almost 800 wet-snow avalanches were observed, about 4.5 times more loose snow avalanches than slab avalanches. Considering both types of avalanches jointly, snow depth, precipitation and air temperature showed the highest correlation with avalanche activity. Most loose snow avalanches occurred when air temperature was high and/or after a precipitation period. Slab avalanches occurrence was primarily related to warm air temperatures and snowpack properties such as the isothermal state and the existence of capillary barriers. Radiation did not show up as a significant variable. The results suggest that in a transitional snow climate wet-snow avalanches are, as dry snow avalanches, often related to precipitation events, and that wet slab instability strongly depends on snowpack properties in relation to warming of the snowpack and melt water production.  相似文献   

16.
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   

17.
雪冰中汞的研究进展   总被引：1，自引：0，他引：1  
汞是具有特殊物理化学性质的重金属元素,其较强的挥发性使之能够参与全球尺度传输,汞的高毒性又能对人类和高等生物体产生极大危害,因而汞是一种全球性污染物,在近几十年来备受科学界的关注.汞的全球生物地球化学循环演化规律是目前环境科学领域的研究热点.冰冻圈是地球系统的关键组成部分之一,是各圈层相互作用的重要环节;而雪冰是冰冻圈的主体,是环境和气候记录的良好载体之一.对南极、北极和中低纬高海拔冰川现代雪冰和冰芯中汞的季节变化、空间差异以及历史变化的研究成果进行了综述,总结了北极和亚北极地区汞的雪/气界面过程研究,归纳了汞的实验室检测手段和方法.针对该领域目前研究上的空白和热点,分别对利用冰芯高分辨率和长时间序列记录重建工业革命以来汞的变化历史(特别在青藏高原)、中低纬冰川区汞的雪/气界面过程、雪冰中汞的同位素分析等进行了展望.  相似文献   

18.
Sites of monomethylmercury (MMHg) production in Amazonian regions have been identified in hydraulic reservoirs, lake sediments and wetlands, but tailings ponds have not yet received sufficient attention for this purpose. This work evidenced high MMHg production within the water column and the interstitial water of two tailings ponds of French Guiana Au mines located; (i) in a small scale exploitation (Combat) where Hg was used for Au amalgamation, and (ii) in an industrial on-going Au mine (Yaoni) processing without Hg. The (MMHg)D maximum (2.5 ng L−1) occurred in the oxic water column above the sediment-water interface (SWI) of the most recent tailings pond (Combat), where the substrate was fresh, the redox transition was sharp and the pool of total Hg was large. In the Yaoni pond, the (MMHg)D maximum concentration (1.4 ng L−1) was located at the SWI where suboxic conditions prevailed. Using the (MMHg)D concentration as a proxy for Hg methylation rates, the present results show that Hg methylation may occur in various redox conditions in tailings ponds, and are favored in areas where the organic matter regeneration is more active.A 3-month long laboratory experiment was performed in oxic and anoxic boxes filled with high turbidity waters from the Combat Au mine to simulate tailings ponds. Slaked lime was added in an experimental set (2 mg L−1) and appeared to be very efficient for the reduction of suspended particulate matter (SPM) to environmentally acceptable concentrations. However, at the end of the experiment, large (MMHg)D concentrations were monitored under treated anoxic conditions with the (MMHg)D maximum located at the SWI above the Fe-reducing zones. No (MMHg)D was detected in oxic experiments. The use of slaked lime for SPM decantation appears to be an efficient and non-onerous process for Au miners to avoid Hg methylation in tailings ponds when it is combined with rapid drainage of the mine waters. A subsequent human intervention is however necessary for the recovery of soil structure through the cover of dried ponds with organic rich materials and reforestation to avoid the stagnation of rain waters and the occurrence of anoxia.  相似文献   

19.
《Applied Geochemistry》2005,20(3):627-638
Concentrations of total Hg and methylmercury (MMHg) in riparian soil, mine-waste calcine, sediment, and moss samples collected from abandoned Hg mines in Wanshan district, Guizhou province, China, were measured to show regional dispersion of Hg-contamination. High total Hg and MMHg concentrations obtained in riparian soils from mined areas, ranged from 5.1 to 790 mg kg−1 and 0.13 to 15 ng g−1, respectively. However, total Hg and MMHg concentrations in the soils collected from control sites were significantly lower varying from 0.1 to 1.2 mg kg−1 and 0.10 to 1.6 ng g−1, respectively. Total Hg and MMHg concentrations in sediments varied from 90 to 930 mg kg−1 and 3.0 to 20 ng g−1, respectively. Total Hg concentrations in mine-waste calcines were highly elevated ranging from 5.7 to 4400 mg kg−1, but MMHg concentrations were generally low ranging from 0.17 to 1.1 ng g−1. Similar to the high Hg concentrations in soil and sediments, moss samples collected from rocks ranged from 1.0 to 95 mg kg−1 in total Hg and from 0.21 to 20 ng g−1 in MMHg. Elevated Hg concentrations in mosses suggest that atmospheric deposition might be an important pathway of Hg to the local terrestrial system. Moreover, the spatial distribution patterns of Hg contamination in the local environment suggest derivation from historic Hg mining sites in the Wanshan area.  相似文献   

20.
Mercury isotope fractionation during liquid-vapor evaporation experiments   总被引：2，自引：0，他引：2  
Liquid-vapor mercury isotope fractionation was investigated under equilibrium and dynamic conditions. Equilibrium evaporation experiments were performed in a closed glass system under atmospheric pressure between 0 and 22 °C, where vapor above the liquid was sampled at chemical equilibrium. Dynamic evaporation experiments were conducted in a closed glass system under 10−5 bar vacuum conditions varying (1) the fraction of liquid Hg evaporated at 22 °C and (2) the temperature of evaporation (22-100 °C). Both, residual liquid and condensed vapor fractions were analyzed using stannous chloride CV-MC-ICP-MS.Equilibrium evaporation showed a constant liquid-vapor fractionation factor (α202/198) of 1.00086 ± 0.00022 (2SD, n = 6) within the 0-22 °C range. The 22 °C dynamic evaporations experiments displayed Rayleigh distillation fractionation behavior with liquid-vapor α202/198 = 1.0067 ± 0.0011 (2SD), calculated from both residual and condensed vapor fractions. Our results confirm historical data (1920s) from Brönsted, Mulliken and coworkers on mercury isotopes separation using evaporation experiments, for which recalculated δ202Hg′ showed a liquid-vapor α202/198 of 1.0076 ± 0.0017 (2SD). This liquid-vapor α202/198 is significantly different from the expected kinetic α202/198 value ((202/198)0.5 = 1.0101). A conceptual evaporation model of back condensation fluxes within a thin layer at the liquid-vapor interface was used to explain this discrepancy. The δ202Hg′ of condensed vapor fractions in the 22-100 °C temperature range experiments showed a negative linear relationship with 106/T2, explained by increasing rates of exchange within the layer with the increase in temperature.Evaporation experiments also resulted in non-mass-dependent fractionation (NMF) of odd 199Hg and 201Hg isotopes, expressed as Δ199Hg′ and Δ201Hg′, the deviation in ‰ from the mass fractionation relationship with even isotopes. Liquid-vapor equilibrium yielded Δ199Hg′/Δ201Hg′ relationship of 2.0 ± 0.6 (2SE), which is statistically not different from the one predicted for the nuclear field shift effect (Δ199Hg/Δ201Hg ≈ 2.47). On the other hand, evaporation under dynamic conditions at 22 °C led to negative anomalies in the residual liquid fractions that are balanced by positive anomalies in condensed vapors with lower Δ199Hg′/Δ201Hg′ ratios of 1.2 ± 0.4 (2SD). This suggests that either magnetic isotope effects may have occurred without radical chemistry or an unknown NMF process on odd isotopes operated during liquid mercury evaporation.  相似文献   

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