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1.
Uranium mining in southeastern Germany resulted in significant environmental risks. Closure of the mines and subsequent rises of water levels may result in heavy-metal and radionuclide-bearing mine waters penetrating aquifers that are used for water supply. While there are certain (geo-)technical constraints on the schedule with which flooding of the mines can proceed, this process must not result in aggravating the problem of metal release. Evaluation of the likely 'natural' geochemical situation of Königstein mine after mining has ceased, and different scenarios for the release of metals indicates that rapid flooding, albeit avoiding unnecessary aeration of the waters, is likely to result in reducing conditions and consequently low U-solubilities.  相似文献   

2.
The late-Hercynian granites of Königshain underwent multistage hydrothermal processes. Extensive high-temperature late-magmatic alteration is, for example, indicated by low Zr/Hf and an REE pattern displaying the tetrad effect. Intensive post-magmatic alteration of the granite occurred along brittle structures. At least two main stages of post-magmatic hydrothermal alteration are involved. The first high-temperature stage, which is characterized by albitization and/or quartz leaching (episyenitization), resulted from fluid–rock interaction with late-magmatic fluids that very probably mixed with external low-salinity fluids. Quartz dissolution was triggered by vapour condensation and/or the cooling of these fluids (below 450??°C) along brittle structures. The high porosity resulting from quartz leaching during stage 1 assisted subsequent circulation of low-temperature fluids at stage 2; the latter is characterized by the chloritization and illitization of episyenites. Almost all major and trace elements were enriched or depleted during one of the main alteration stages. However, Zr, Hf, Th, and Ti were immobile during post-magmatic alteration. The significant depletion of LREE and the enrichment of HREE in albitized samples is controlled by the dissolution of monazite and the new formation of HREE-rich polycrase-(Y) or aeschynite-(Y) during post-magmatic stage 1. Negative Ce anomalies of episyenites are associated with illitization and suggest oxidizing conditions during stage 2.  相似文献   

3.
4.
An overview is presented of a 4-year study by the Äspö Task Force on Modelling of Groundwater Flow and Transport of Solutes, whose primary aim was to build a bridge between the approaches used for site characterisation (SC) and performance assessment (PA) associated with nuclear waste repositories. Eleven modelling teams representing six national radioactive waste organisations participated in eight modelling exercises whose objectives were: to assess simplifications used in PA models; to determine how, and to what extent, experimental tracer and flow experiments can constrain the range of parameters used in PA models; to support the design of SC programmes to assure that the results have optimal value for PA calculations; and to improve the understanding of site-specific flow and transport behaviour at different scales using SC models. The modelling tasks were concerned with flow and transport through single and multiple near-planar features on SC and PA timescales, including the diffusion of solutes into multiple immobile zones adjacent to fracture surfaces. In general, tracer tests provide only limited quantitative constraints on retention parameter values relevant to PA but nevertheless provide insight about the flow and transport processes, which is a key element of the bridge between SC and PA.  相似文献   

5.
《Applied Geochemistry》1999,14(7):917-925
The origin of salinity within the Äspö groundwater system is investigated by combining interpretations of conservative dissolved ions and of stable isotope ratios in water. The interpretation concludes that the groundwater salinity results from a mixing between Baltic Sea water intrusion and a deep seated saline groundwater of marine origin. This conclusion supports the geochemical model developed for the Äspö site. The residence time of the deep salinity is assessed by comparing the 36Cl content of dissolved salt at different depths and the secular equilibrium value of the host rock. The 36Cl of deepest levels corresponding to the highest salinity, is in equilibrium with rock, suggesting a penetration of the deep salinity into the host rock more than 1.5 Ma ago.  相似文献   

6.
《Applied Geochemistry》2000,15(1):35-49
A comparative assessment of two reactive-transport models, PHREEQC and HYDROGEOCHEM (HGC), was done to determine the suitability of each for simulating the movement of acidic contamination in alluvium. For simulations that accounted for aqueous complexation, precipitation and dissolution, the breakthrough and rinseout curves generated by each model were similar. The differences in simulated equilibrium concentrations between models were minor and were related to (1) different units in model output, (2) different activity coefficients, and (3) ionic-strength calculations. When adsorption processes were added to the models, the rinseout pH simulated by PHREEQC using the diffuse double-layer adsorption model rose to a pH of 6 after pore volume 15, about 1 pore volume later than the pH simulated by HGC using the constant-capacitance model.In PHREEQC simulation of a laboratory column experiment, the inability of the model to match measured outflow concentrations of selected constituents was related to the evident lack of local geochemical equilibrium in the column. The difference in timing and size of measured and simulated breakthrough of selected constituents indicated that the redox and adsorption reactions in the column occurred slowly when compared with the modeled reactions. MINTEQA2 and PHREEQC simulations of the column experiment indicated that the number of surface sites that took part in adsorption reactions was less than that estimated from the measured concentration of Fe hydroxide in the alluvium.  相似文献   

7.
The aim of this research was to predict groundwater levels in the Neishaboor plain, Iran, using a ??panel-data?? model. Panel-data analysis endows regression analysis with both spatial and temporal dimensions. The spatial dimension pertains to a set of cross-sectional units of observation. The temporal dimension pertains to periodic observations of a set of variables characterizing these cross-sectional units over a particular time span. Firstly, the available observation wells in the Neishaboor plain were clustered according to their fluctuation behavior using the ??Ward?? method, which resulted in six areal zones. Then, for each cluster, an observation well was selected as its representative, and for each zone, values of monthly precipitation and temperature, as independent variables, were estimated by the inverse-distance method. Finally, the performance of different panel-data regression models such as fixed-effects and random-effects models were investigated. The results showed that the two-way fixed-effects model was superior. The performance indicators for this model (R 2?=?0.97, RMSE?=?0.05?m and ME?=?0.81?m) reveal the effectiveness of the method. In addition, the results were compared with the results of an artificial-neural-network (ANN) model, which demonstrated the superiority of the panel-data model over the ANN model.  相似文献   

8.
Markus Egli 《GeoJournal》1998,44(1):73-89
Data on element fluxes (Ca, K, N) are presented which were obtained in the course of an extended project on element-cycling in a forested ecosystem near Möhlin, northwestern Switzerland. Current fluxes of Ca, K, and N could be compared with historical fluxes (1969–1993) with the help of soil chemistry inventories since 1969, data on the forest management, and atmospheric deposition. Since 1969, soil chemistry has significantly changed due to a distinct disintegration of humus. The decomposition of organic matter influenced strongly the element cycling. Due to this mineralization high amounts of N were released. It is, however, not fully clear in which chemical form N has been transferred out of the system. Two possible hypotheses on the N losses are defined. According to the calculated proton budget and measured element changes in the soil, it is hypothized that a large part of the mineralized organic N presumably was transformed into N2 or more likely into N2O. A complete nitrification of organically bound N to NO3 is also discussed but is, however, considered as less probable. In contrast to K, Ca proved to be a very sensitive element: the exchangeable Ca stock has been decreased sharply. The analysis of the current fluxes of Ca, K, and N reveals that nitrogen is abundantly present in the forest system with the consequence that the ecological balance is shifted in favour of N. Accordingly, the supply of base cations is rather scarce for the plants. Furthermore, the influence of forest management on element fluxes seems to be substantial, especially on the fluxes of base cations, but can be reduced with simple measures (e.g. removal of the bark of coniferous trees).  相似文献   

9.
Uranium and Th are important radioactive elements. Most studies were focused on their environmental impact from uranium deposits and mining sites. But other sorts of mines such as rare metals mines are associated highly with uranium and thorium, too. In China, the Irtysh River is the only river that runs into the Arctic Ocean. The famous Koktokay rare metal pegmatite deposit is located in the headwater region of this river and has been exploited for several decades. The waste ore piled along the riverside as long as several kilometers. The wastewater flom the concentrating plant is discharged into the river directly. In addition, uranium and thorium can be leached from the waste ore into the river in the weathering process. So it is necessary to study the uranium and thorium distribution in the branch and trunk streams of the Irtysh River and the wastewater from the mining site impact on it. In this study, the contents of uranium and thorium in water samples from the Irtysh River and rare metal mine wastewater have been detected directly with ICP-MS. Uranium and thorium distribution and geochemical behaviors in the Irtysh River basin have been studied. The environmental uranium and thorium pollution status in the Irtysh River and wastewater from a rare metal mine impact on it have also been evaluated. The study shows that uranium and thorium contents in wastewater from a rare metal mine are as high as 78.311 μg/L and 0.627 μg/L, respectively, so we should also pay attention to the radioactive pollution from the rare metal mine. The average contents of U and Th in the branch streams of the Irtysh River are 0.572 μg/L and 0.015 μg/L, respectively. At the mean time, in the trunk of the Irtysh River, average thorium content is 0.019 μg/L while U is up to 2.234 μg/L, much higher than the average content (0.0309 μg/L) of the world rivers. From upstream to downstream in the trunk of the Irtysh River, thorium content declines gradually due to dilution by other branches and deposition itself.  相似文献   

10.
《Applied Geochemistry》2000,15(9):1383-1397
Water pollution arising from base metal sulphide mines is problematic in many countries, yet the hydrogeology of the subsurface contaminant sources is rarely well-characterized. Drainage water pumped from an active F–Pb mine in northern England has unusual chemistry (alkaline with up to 40 mg.l−1 Zn) which profoundly impacts the ecology of the receiving watercourse. Detailed in-mine surveys of the quantity and quality of all ground water inflows to the mine were made. These revealed major, temporally persistent heterogeneities in ground water quality, with three broad types of water identified as being associated with distinct hydrostratigraphic units. Type I waters (associated with the Firestone Sill aquifer) are cool (<10°C), Ca–HCO3–SO4 waters, moderately mineralized (specific electrical conductance (SEC)≤410 μS.cm−1) with <4 mg.l−1 Zn. Type II waters (associated with the Great Limestone aquifer) are warmer (≈15°C), of Ca–SO4 facies, highly mineralized (SEC≤1500 μS.cm−1) with ≤40 mg.l−1 Zn. Type III waters (in the deepest workings) are tepid (>18°C), of Ca–HCO3–SO4 facies, intermediately mineralized (SEC≤900 μS.cm−1) with ≤13 mg.l−1 Zn, and with significant Fe (≤12 mg.l−1) and Pb (≤8 mg/l). Monotonic increases in temperature and Cl concentration with depth contrast with peaks in total mineralization, SO4 and Zn at medium depth (in Type II waters). Sulphate, Pb and Zn are apparently sourced via oxidation of galena and sphalerite, which would release each metal in stoichiometric equality with SO4. However, molal SO4 concentrations typically exceed those of Pb and Zn by 2–3 orders of magnitude, which mineral equilibria suggest is due to precipitation of carbonate “sinks” for these metals. Contaminant loading budgets demonstrate that, although Type II waters amount to only 25% of the total ground water inflow to the mine, they account for almost 60% of the total Zn loading. This observation has important management implications for both the operational and post-abandonment phases of the mine life cycle.  相似文献   

11.
An isotopic geochronological study of dispersed uranium mineralization was performed in the granitic rocks of the Urtui pluton in the framework of the Strel’tsovka uranium ore field and in the Yamsky site of the Urov-Uryumkan granite-gneiss arch. Two stages of such mineralization—783 ± 26 Ma in the Urtui granitic pluton and 138.6 ± 2.3 Ma in the Yamsky site—have been established. The emplacement of granite pertaining to the Unda Complex disturbed the U-Pb isotopic system in uraninite from the Urtui granitic pluton and resulted in redeposition of uranium phase dated at 262 ± 34 Ma. The young, probably, recent process gave rise to the redistribution of radiogenic lead in the U-bearing phases developing after uraninite.  相似文献   

12.
Uranium processing and mining activities that generate many contaminants, such as high concentrations of U (VI), sulfate and heavy metals (Zn, Cu, Ni, etc), may pose a serious threat to the groundwater resources. In recent years, considerable research has been conducted respectively on two kinds of permeable reactive barriers (PRB), including zerovalent iron (ZVI) and sulfate reducing bacteria (SRB), for in-situ removal of these pollutants from groundwater. However, little investigation has been carried out on the potential benefits of bioaugmenting ZVI barriers to enhance the elimination of the pollutants by combining ZVI with SRB systems. The main goal of this study was to conduct batch and column experiments to determine whether the combination of SRB and ZVI can function synergistically and accelerate the rate of pollutant removal. The results of anaerobic batch experiments demonstrated that although the integrated ZVI/PRB system itself has no ability to reduce and remove sulfate directly, SRB can utilize hydrogen gas produced during the slow process of ZVI corrosion as an electron donor to raise biomass yields significantly and accelerate reductive sulfate removal. In particular, ferrous cations produced as the byproduct of ZVI corrosion process reacted with hydrogen sulfide from sulfate reduction and formed iron-bearing sulfide precipitates, which can stimulate the growth of SRB and promote sulfate removal activity by eliminating the biotoxicity of hydrogen sulfide. It was also shown that secondary mineral products (pyrite/ferrous sulfide) formed as a consequence of microbial sulfate reduction and ZVI corrosion process can enhance the microbial precipitation of soluble U (VI) as insoluble uraninite(uranium dioxide).  相似文献   

13.
The ores of the Yata gold mine in China are rich in arsenic and antimony, so the exploitation of this mine may also lead to the release of As and Sb to adjacent environments, such as stream water, stream sediment, soil, plants, and crops. To understand the environmental impact of mine tailings, samples of water, sediment, soil, plant and crop were collected and analyzed. In summer of 2005, the tailings dump was seriously flushed by a heavy flood, and the mine waste was transported far away. Samples were collected in December of 2004 and January of 2006, respectively, and the impact of the flood on the release of toxic elements was evaluated. The result shows that the Yata creek, which drains the mining area, was severely contaminated by As and Sb. The dissolved As and Sb in water are 86-1140 μg/L and 65-370 μg/L, the particulate As and Sb are 38-2100 μg/L and 25-420 μg/L, whereas As and Sb in the sediment are 190-760 μg/g and 69-210 μg/g, respectively. In water environment, As and Sb show a similar feature to SO4^2- since As and Sb exist dominantly as anions--H2AsO4^-, HAsO4^2- and SbO3^-. In contrast to Fe, Cu, Pb, Zn, which migrate mostly in particulate form, As and Sb tend to transport in dissolved form.  相似文献   

14.
Investigations were undertaken in the riparian zone near Shangba village, an AMD area, in southern China to determine the effects that river–groundwater interactions and groundwater residence time have had on environmental quality and geochemical evolution of groundwater. Based on the Darcy’s law and ionic mass balances as well as the method of isotopic tracer, the results showed that there were active interactions between AMD-contaminated river water and groundwater in the riparian zone in the study area. River water was found to be the main source of groundwater recharge in the northwestern part of the study area, whereas groundwater was found to be discharging into the river in the southeastern part of the study area throughout the year. End-member mixing analysis quantified that the contributions of river water to groundwater decreased gradually from 35.9% to negligible levels along the flow path. The calculated mixing concentrations of major ions indicated that water–rock reactions were the most important influence on groundwater quality. The wide range of Ca2+?+?Mg2+ and HCO3? ratios and the change of groundwater type from Ca2+–SO42? type to a chemical composition dominated by Ca2+–HCO3? type indicated a change of the major water–rock reaction process from the influence of H2SO4 (AMD) to that of CO2 (soil respiration) along a groundwater flow path. Furthermore, the kinetics interpretation of SO42? and HCO3? concentrations suggested that the overlapping time of their kinetics triggered the hydrochemical evolution and the change of major weathering agent. This process might take approximately 8 years and this kinetic time will be continued when a steady source of contamination enter the aquifer.  相似文献   

15.
Acid mine drainage (AMD) has been recognized as a major environmental pollution problem over past decades. This pollutant effluent is complex and is characterized by elevated concentrations of iron and sulfate, low pH, and high concentrations of a wide variety of metals depending on the host rock geology. Massive inadvertent discharges from acid mines have given rise to dramatic cases of ecological damage. These events indicate an improved understanding of the mechanism controlling metal transport to the river is important, since the aquatic ecology will be affected, to some degree, dependent on the phase (dissolved or particulate) in which the metal is transported. In this study, polluted water samples were collected along the Hengshi River near the Dabaoshan mine, Guangdong, China, in April 2005. The concentrations of dissolved Cu, Zn, Cd and Pb have been determined using ICP-MS and the chemical speciation of those metals in suspended particles was examined using BCR methods and SEM/EDX mineralogical analysis. Combining these two sets of data, the intention was to develop geochemical concepts, which explain the behavior of Cu, Zn, Cd and Pb in particle-water interactions of heavy metals in AMD. The results show that the dissolved heavy metals exhibited non-conservative behavior in the Hengshi River. The dissolved and particulate Cu, Zn, Cd and Pb have the similar spatial distribution, which decreased gradually along the river except in the lower reaches because of the absorption-desorption between dissolved and particulate phases. Although the metal concentrations in both phases were elevated, dissolved metals were dominant and had the maximum concentrations in the low pH region.  相似文献   

16.
Half a millennium mercury production at Idrija is reflected in increased mercury contents in all environmental segments. The bulk of roasting residues from the middle of the 19th century to 1977 was discharged directly into the Idrijca River, and the material was carried at high waters to the Soca River and farther into the Adriatic Sea. It has been estimated that 45500 tons of mercury were emitted into the environment during the operating period of the mine, which ceased production in 1994. In the lower reaches of the Idrijca the riverine deposits with high mercury contents have been, and will be in the future a source of mercury polluted sediment. Stream sediments were monitored at the same locations along the Idrijca and Soca rivers (70 kin) every 5 years since 1991 (1991-2005). Grain size distribution was determined by dry sieving and fractions for geochemical analysis were prepared (〈0.04 and 〈0.125 mm). Soils on river terraces were sampled at 5 localities in the lower course of Idrijca. At two locations of the terrace profiles the samples of averaged meadow forage and plantain (Plantago lanceolata) were collected within a 50-meters radius. We found that there was no decrease in mercury concentration in active river sediments during the last 20 years. Upstream from the Idrija Town the mercury concentrations in active river sediments vary from 1 to 10 mg/kg (average 3.3 mg/kg). From Idrija to Spodnja Idrija the mercury concentrations increase extremely and vary greatly (32-4,121 mg/kg, the average is 734 mg/kg). From Spodnja ldrija to the Idrijca-Soca confluence is the average 218 mg/kg, and 57 mg/kg downstream in the Soca River sediments.  相似文献   

17.
The concentrations of uranium, iron and the major constituents were determined in groundwater samples from aquifer containing uranyl phosphate minerals (meta-autunite, meta-torbernite and torbernite) in the Köprüba?? area. Groundwater samples from wells located at shallow depths (0.5–6 m) show usually near neutral pH values (6.2–7.1) and oxidizing conditions (Eh = 119–275 mV). Electrical conductivity (EC) values of samples are between 87 and 329 μS/cm?1. They are mostly characterized by mixed cationic Ca dominating bicarbonate types. The main hydrogeochemical process is weathering of the silicates in the shallow groundwater system. All groundwater in the study area are considered undersaturated with respect to torbernite and autunite. PHREEQC predicted UO2(HPO4) 2 2? as the unique species. The excellent positive correlation coefficient (r = 0.99) between U and PO4 indicates the dissolved uranium in groundwater would be associated with the dissolution of uranyl phosphate minerals. The groundwater show U content in the range 1.71–70.45 μg/l but they are mostly lower than US EPA (2003) maximum contaminant level of 30 μg/l. This low U concentrations in oxic groundwater samples is attributed to the low solubility of U(VI) phosphate minerals under near neutral pH and low bicarbonate conditions. Iron closely associated with studied sediments, were also detected in groundwater. The maximum concentration of Fe in groundwater samples was 2837 μg/l, while the drinking water guidelines of Turkish (TSE 1997) and US EPA (2003) were suggested 200 and 300 μg/l, respectively. Furthermore, iron and uranium showed a significant correlation to each other with a correlation coefficient (r) of 0.94. This high correlation is probably related to the iron-rich sediments which contain also significant amounts of uranium mineralization. In addition to pH and bicarbonate controlling dissolution of uranyl phosphates, association of uranyl phosphates with iron (hydr) oxides seems to play important role in the amount of dissolved U in shallow groundwater.  相似文献   

18.
The Singhbhum Shear Zone in eastern India is one of the largest repositories of uranium and copper in India. Besides uranium and copper, apatite-magnetite mineralization is widespread in this shear zone. This study aims at deciphering the physico-chemical evolution of magnetite mineralization in relation to progressive shearing integrating field relations, micro-textures, structures and compositions of magnetite in the Banduhurang uranium mine. Apatite-magnetite ores occur as discrete patches, tongues, and veins in the strongly deformed, fine grained quartzchlorite schist. Textures and microstructures of magnetite indicate at least three stages of magnetite formation. Coarsegrained magnetite (magnetite-1) with long, rotational, and complex strain fringes, defined by fibrous and elongate quartz, is assigned to a stage of pre-/early-shearing magnetite formation. Medium grained magnetite (magnetite-2), characterized by single non-rotational strain fringe equivalent to the youngest fringe of magnetite-1, grew likely at the mid-/late-stage of shearing. Fine grained magnetite (magnetite-3) is generally devoid of any pressure shadow. This indicates even a much later stage of formation of this magnetite, presumably towards the closing stage of shearing. Some of the magnetite-1 grains are optically heterogeneous with a dark, pitted Cr-Ti-bearing core overgrown by lighter, fresh rim locally containing pyrite, chalcopyrite, and chlorite inclusions. The cores are also locally characterized by high Al and Si content. Homogeneous magnetite-1 is optically and compositionally similar to the overgrowth of heterogeneous magnetite-1. This homogeneous magnetite-1 that grew as separate phase is contemporaneous with the overgrowth on pitted core of heterogeneous magnetite-1. Magnetite-2 is compositionally very similar to homogeneous magnetite-1, but is devoid of sulfide inclusion. Magnetite-3 is generally devoid of any silicate or sulfide inclusion and is most pure with least concentrations of trace/minor elements. The high Al and Si content in some magnetite can be explained by coupled substitution that involves substitution of Si4+ for Fe3+ in the tetrahedral sites and Fe2+ for Fe3+ in the octahedral sites, with a simple substitution of Al3+ for Fe3+ in the octahedral sites. The mode of occurrences of apatite-magnetite ores indicates a predominantly hydrothermal origin of most magnetite. However, the Cr-Ti-bearing magnetite-1 cores and inferred mafic nature of the original protolith indicates that some magnetite was inherited from the original igneous rock. We propose that the pre-/early-shearing hydrothermal event of magnetite formation was associated with sulfide mineralization and alteration of existing magmatic magnetite. The second stage of magnetite formation at the mid-/late-stage of shearing was not associated with sulfide formation. Finally, fine-grained compositionally pure magnetite formed at the closing stage of shearing likely due to metamorphism of Fe-rich protolith.  相似文献   

19.
20.
The Podljubelj mercury mine lies in the NW part of Slovenia. The ore is of hydrothermal-vein type. The ore deposit was exploited between the years 1557 and 1902. Total production of the mine was 110000 tons of ore (360 tons of Hg). A smelter located close to the mine had been in operation since 1855. The waste material from the mine and the smelter was dumped in close vicinity of the mine. Total quantity of the waste has been estimated at 170000 tons. In order to establish environmental impacts, soil and stream sediment samples were investigated. Soil samples were collected at two different depths (horizons A and B) in a 100 m grid within an 88 ha area. In the vast area also 11 samples of stream sediments were considered. Heavy metals were determined by means of cold vapor atomic absorption spectrometry CV-AAS after aqua regia digestion. Based on the chemical analyses of samples, the estimated mercury mean for soils is 3.67 mg/kg (0.35-244 mg/kg) for horizon A and 1.39 mg/kg (0.17-71.7 mg/kg) for horizon B. The estimated mercury mean for stream sediments is 0.64 mg/kg (0.065-1.36 mg/kg). The concentrations of mercury in soils generally decrease with depth and distance from the mine. The highest content of Hg was determined in a sample taken in the immediate vicinity of the smelter (719 mg/kg). The results have shown that on the 9 ha of the study area, the contents of Hg in soils exceeded the officially set limit value for soils (10 mg/kg). High contents of Hg in soil around the abandoned smelter are a consequence of former atmospheric emissions and technological losses. High contents of Hg were also found in the mine and smelter waste dump. At the edges of the study area and in the samples of stream sediments, Hg concentrations are low.  相似文献   

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