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1.
The sites at Bangombé and Okélobondo (Oklo) in Gabon provide a unique opportunity to study the behaviour of products from natural nuclear reactions in the vicinity of reactor zones which were active around two billion years ago. The Commission of the European Communities initiated the Oklo Natural Analogue Programme. One of the principal aims was to study indications of present time migration of elements from the reactor zones under ambient conditions. The hydrogeological and hydrochemical data from the Oklo sites were modelled in order to better understand the geochemical behaviour of radionuclides in the natural system, by using independent models and by comparing the modelling outcome. Two modelling approaches were used: M3 code (hydrochemical mixing and mass balance model), developed by the Swedish Nuclear Fuel and Waste Management Company (SKB) and HYTEC (reactive transport model) developed by Ecole des Mines de Paris.Two different reactor zones were studied: Bangombé, a shallow site, the reactor being at 11 m depth, and OK84 at Okélobondo, situated at about 450 m depth, more comparable with a real repository location. This allowed the validation of modelling tools in two different sedimentary environments: one shallow, with a more homogeneous layering situated in an area of meteoric alteration, and the other offering the opportunity to study radionuclide migration from the reaction zone over a distance of 450 m through very heterogeneous sedimentary layers.The modeling results indicate that the chemical reactions retarding radionuclide transport are very different at the two sites. At Bangombé, the decomposition of organic material consumes oxygen and at Okélobondo the oxygen is consumed by inorganic reactions resulting, in both cases, in uranium retardation. Both modelling approaches (statistic with M3 code and deterministic with HYTEC code) could describe this situation.The goal of this exercise is to test codes which can help to describe and understand the processes taking place at the sites, validate the models with in situ data, and thus build confidence in the tools used for future site characterization. Ultimately, this allows identifying and selecting processes and parameters that can be used as input into repository performance assessment calculations and modelling exercises.  相似文献   

2.
The sites at Bangombé and Okélobondo (Oklo) in Gabon provide a unique opportunity to study the behaviour of products from natural nuclear reactions in the vicinity of reactor zones which were active around two billion years ago. The Commission of the European Communities initiated the Oklo Natural Analogue Programme. One of the principal aims was to study indications of present time migration of elements from the reactor zones under ambient conditions. The hydrogeological and hydrochemical data from the Oklo sites were modelled in order to better understand the geochemical behaviour of radionuclides in the natural system, by using independent models and by comparing the modelling outcome. Two modelling approaches were used: M3 code (hydrochemical mixing and mass balance model), developed by the Swedish Nuclear Fuel and Waste Management Company (SKB) and HYTEC (reactive transport model) developed by Ecole des Mines de Paris. Two different reactor zones were studied: Bangombé, a shallow site, the reactor being at 11 m depth, and OK84 at Okélobondo, situated at about 450 m depth, more comparable with a real repository location. This allowed the validation of modelling tools in two different sedimentary environments: one shallow, with a more homogeneous layering situated in an area of meteoric alteration, and the other offering the opportunity to study radionuclide migration from the reaction zone over a distance of 450 m through very heterogeneous sedimentary layers. The modeling results indicate that the chemical reactions retarding radionuclide transport are very different at the two sites. At Bangombé, the decomposition of organic material consumes oxygen and at Okélobondo the oxygen is consumed by inorganic reactions resulting, in both cases, in uranium retardation. Both modelling approaches (statistic with M3 code and deterministic with HYTEC code) could describe this situation. The goal of this exercise is to test codes which can help to describe and understand the processes taking place at the sites, validate the models with in situ data, and thus build confidence in the tools used for future site characterization. Ultimately, this allows identifying and selecting processes and parameters that can be used as input into repository performance assessment calculations and modelling exercises.  相似文献   

3.
A new strategy for characterisation of airborne uranium contamination based on ICP mass spectrometric analysis of tree bark is described. The uranium content of tree barks (50 samples) obtained from diverse locations (remote, rural, industrial) varied over almost four orders of magnitude (0.001-8.3 micrograms/g U) with maximum concentrations recorded in the vicinity of a nuclear fuel fabrication plant (0.70-8.3 micrograms/g U). Elevated concentrations were also observed near a coal-fired power station (0.25-0.38 microgram/g U). Isotopic analysis revealed significant deviation from the natural uranium isotope ratio (235U/238U, 0.00725) at four nuclear installations (235U/238U, 0.0055-0.0097). These findings indicate that tree bark serves as an effective biomonitor for uranium and, with isotopic analysis, discrimination between nuclear and non-nuclear emissions is realised.  相似文献   

4.
This paper presents the results of a detailed field investigation that was performed for studying groundwater recharge processes and solute downward migration mechanisms prevailing in the unsaturated zone overlying a chalk aquifer in Belgium. Various laboratory measurements were performed on core samples collected during the drilling of boreholes in the experimental site. In the field, experiments consisted of well logging, infiltration tests in the unsaturated zone, pumping tests in the saturated zone and tracer tests in both the saturated and unsaturated zones. Results show that gravitational flows govern groundwater recharge and solute migration mechanisms in the unsaturated zone. In the variably saturated chalk, the migration and retardation of solutes is strongly influenced by recharge conditions. Under intense injection conditions, solutes migrate at high speed along the partially saturated fissures, downward to the saturated zone. At the same time, they are temporarily retarded in the almost immobile water located in the chalk matrix. Under normal recharge conditions, fissures are inactive and solutes migrate slowly through the chalk matrix. Results also show that concentration dynamics in the saturated zone are related to fluctuations of groundwater levels in the aquifer. A conceptual model is proposed to explain the hydrodispersive behaviour of the variably saturated chalk. Finally, the vulnerability of the chalk to contamination issues occurring at the land surface is discussed.  相似文献   

5.
Oxidation of pyrite at the Nopal I uranium deposit, Peña Blanca district, Chihuahua, Mexico has resulted in the formation of Fe-oxides/hydroxides. Anomalous U concentrations (i.e. several hundred to several thousand ppm) measured in goethite, hematite, and amorphous Fe-oxyhydroxides in a major fracture that crosscuts the deposit and the absence of U minerals in the fracture suggest that U was retained during secondary mineral growth or sorbed on mineral surfaces. Mobilization and transport of U away from the deposit is suggested by decreasing U concentrations in fracture-infilling materials and in goethite and hematite with distance from the deposit. Greater than unity 234U/238U activity ratios measured in fracture-infilling materials indicate relatively recent ( < 1 Ma) U uptake from fluids that carried excess 234U. Systematic decreases in 234U/238U activity ratios of fracture materials with distance from the deposit suggest a multistage mobilization process, such as remobilization of U from 234U-enriched infill minerals or differential or diminished transport of U-bearing solutions containing excess 234U.  相似文献   

6.
The contribution of the conflict of 1999 to the environmental levels of uranium in the Balkan area was evaluated by means of lichens used as biomonitors. The average U concentration found in lichens in the present study was in line with the values reported for lichens from other countries and well below the levels found in lichens collected in areas with natural or anthropogenic sources of U. Measurement of isotopic ratios 235U/238U allowed to exclude the presence of depleted uranium. According to these results, we could not detect widespread environmental contamination by depleted uranium in the Balkan area.  相似文献   

7.
Uranium is being actively transported from uraniferous sedimentary rocks into a peat bog at the Broubster natural analogue site in Caithness, Scotland. Massive calcareous sandstone within the Caithness Flags sequence is the main source of uranium which resides primarily within diagenetic apatite and dispersed U---Si---Ti phases. Supergene weathering processes have decalcified the sandstone and are effective in mobilising uranium by groundwater leaching, primarily along a fault zone. Uranium transport in solution by means of groundwater and surface flows is effectively terminated by retardation within 4-kyr-old peat deposits laid down on boulder clay. This process of secondary fixation has resulted in a young uranium anomaly in the peat which comprises in excess of 0.1 wt% U. The site has been investigated comprehensively to define the geometry of the anomaly together with the hydrogeology, hydrochemistry, petrology, mineralogy and the nature of the peat sink-term. The main physical and geochemical properties of the system, including the uranium decay series radionuclide distributions in water and solid samples, are documented in this paper. From these data, the processes governing the distribution of uranium have been quantified using a three-dimensional groundwater flow package and an equilibrium speciation model incorporating a recently developed electrostatic surface complexation model to account for cation-organic interactions. The results described form part of a coordinated project on natural radionuclide migration undertaken to improve confidence in predictive methods used for radiological assessment.  相似文献   

8.
The long-term mobility of actinides in groundwaters is important for siting nuclear waste facilities and managing waste-rock piles at uranium mines. Dissolved organic carbon (DOC) may influence the mobility of uranium, but few field-based studies have been undertaken to examine this in typical groundwaters. In addition, few techniques are available to isolate DOC and directly quantify the metals complexed to it. Determination of U-organic matter association constants from analysis of field-collected samples compliments laboratory measurements, and these constants are needed for accurate transport calculations. The partitioning of U to DOC in a clay-rich aquitard was investigated in 10 groundwater samples collected between 2 and 30 m depths at one test site. A positive correlation was observed between the DOC (4-132 mg/L) and U concentrations (20-603 microg/L). The association of U and DOC was examined directly using on-line coupling of Asymmetrical Flow Field-Flow Fractionation (AsFlFFF) with UV absorbance (UVA) and inductively coupled plasma-mass spectrometer (ICP-MS) detectors. This method has the advantages of utilizing very small sample volumes (20-50 microL) as well as giving molecular weight information on U-organic matter complexes. AsFlFFF-UVA results showed that 47-98% of the DOC (4-136 mg C/L) was recovered in the AsFlFFF analysis, of which 25-64% occurred in the resolvable peak. This peak corresponded to a weight-average molecular weight of about 900-1400 Daltons (Da). In all cases, AsFlFFF-ICP-MS suggested that相似文献   

9.
Abstract

Uranium mining and ore processing are known to be harmful to the environment and human health if the waste generated is not managed properly. The aim of the present study is to determine the radiological indices in the mill tailings and review the possible attempts to utilize and minimize its hazardous effect. The activity concentrations of natural radionuclides, 238U, 232Th, 226Ra, and 40K have been measured by gamma spectrometry using HP-Ge detector. The average activity concentrations of 238U, 232Th, 226Ra, and 40K in the tailings wastes were 2071.8, 59.92, 6921.262, and 445. 57?Bq/kg respectively which are higher than the international average limit. The ranges of hazard indices such as Radium equivalent activity (Raeq), external hazard index (Hex), internal hazard index (Hin), γ-radiation hazard index Iγ, Dose rate (nGy/h) and annual effective dose equivalent (AED), were estimated. Uraniumm isotopic ratios in the ore –material and mill tailing samples indicate migration out of radionuclides to the surrounding environment causing contamination and many dangerous diseases. Fairly, all investigated tailing waste samples do not satisfy the universal standards, the studied wastes relatively still have high uranium contents and need reprocessing.  相似文献   

10.
This paper reports the results of a study using lichens as biomonitors to investigate the environmental distribution of uranium and other trace elements at selected Kosovo sites. The results suggested that the use of depleted uranium (DU) ammunitions in Kosovo did not cause a diffuse environmental contamination in such a way to have caused a detectable U enrichment in lichens. Also isotopic (235)U/(238)U measurements did not indicate the presence of DU particles in lichens. The present results also provided no indication of intense environmental contamination by the other trace elements analyzed, with the exception of Kosovska Mitrovica, where a diffuse environmental contamination by several heavy elements such as Pb, Zn, As and Cd was found.  相似文献   

11.
Humic colloid-borne migration of uranium in sand columns   总被引:3,自引:0,他引:3  
Column experiments were carried out to investigate the influence of humic colloids on subsurface uranium migration. The columns were packed with well-characterized aeolian quartz sand and equilibrated with groundwater rich in humic colloids (dissolved organic carbon (DOC): 30 mg dm(-3)). U migration was studied under an Ar/1% CO2 gas atmosphere as a function of the migration time, which was controlled by the flow velocity or the column length. In addition, the contact time of U with groundwater prior to introduction into a column was varied. U(VI) was found to be the dominant oxidation state in the spiked groundwater. The breakthrough curves indicate that U was transported as a humic colloid-borne species with a velocity up to 5% faster than the mean groundwater flow. The fraction of humic colloid-borne species increases with increasing prior contact time and also with decreasing migration time. The migration behavior was attributed to a kinetically controlled association/dissociation of U onto and from humic colloids and also a subsequent sorption of U onto the sediment surface. The column experiments provide an insight into humic colloid-mediated U migration in subsurface aquifers.  相似文献   

12.
Activity concentrations, inventories and activity ratios of 137Cs, 238Pu, 239?+?240Pu and 241Am in soil profiles were surveyed in the dry tundra and the adjoining proglacial zones of glaciers at a High Arctic site on Svalbard. Vertical profiles of radionuclide activities were determined in up to 14-cm-thick soil sequences. Additionally, soil properties (pH, organic matter, texture, mineral composition and sorption capacity) were analyzed. Results obtained in this study revealed a large range of activity concentrations and inventories of the fallout radionuclides from the undetectable to the uncommonly high levels (inventories of 30,900?±?940, 47?±?6, 886?±?80 and 296?±?19 Bq/m2 for 137Cs, 238Pu, 239?+?240Pu and 241Am, respectively) found in two profiles from the proglacial zone. Concentration of these initially airborne radionuclides in the proglacial zone soils is related to their accumulation in cryoconites that have a large ability to concentrate trace metals. The cryoconites develop on the surface of glaciers, and the material they accumulate is deposited on land surface after the glaciers retreat. The radionuclide inventories in the tundra soils, which effectively retain radionuclides due to high organic matter contents, were comparable to the global fallout deposition for this region of the world. The 238Pu/239?+?240Pu activity ratios for tundra soils suggested global fallout as the dominant source of Pu. The 238Pu/239?+?240Pu and 239?+?240Pu/137Cs activity ratios in the proglacial soils pointed to possible contributions of these radionuclides from other, unidentified sources.  相似文献   

13.
Seedlings of Helianthus annuus L. (HA) and Brassica juncea (BJ) were used to test the effect of the pH, the presence of phosphates, and the addition of ethylene-diamine-tetraacetic acid (EDTA) or citrate on the uptake and the translocation of uranium isotopes ((238)U, (235)U, and (234)U) and (226)Ra. The results indicated that the presence of phosphates generally reduces the uptake and transfer of uranium from the roots to the shoots of HA. In the case of BJ, while phosphate enhanced the retention of uranium by roots, the translocation was poorer. Likewise, for (226)Ra, the best translocation was in the absence of phosphates for both species. The addition of citrate increased the translocation of uranium for both species, but had no clear effect on the transfer of (226)Ra. The effect of EDTA was much more moderate both for uranium and for (226)Ra, and for both plant species. Only noticeable was a slightly better uptake of (226)Ra by BJ at neutral pH, although the translocation was lower.  相似文献   

14.
Natural analogues allow scientists to investigate biogeochemical processes relevant to radioactive waste disposal that occur on time scales longer than those that may be studied by time-limited laboratory experiments. The Palmottu U-Th deposit in Finland and the Bangombé natural nuclear reactor in Gabon involve the study of natural uranium, and are both considered natural analogues for subsurface radioactive waste disposal. The microbial population naturally present in groundwater may affect the redox conditions, and hence, the radionuclide solubility and migration. Therefore, groundwater samples from the two sites were investigated for microbial populations. The total numbers of cells ranged from 10(4) to 10(6) cells ml(-1). Iron-reducing bacteria (IRB) were the largest culturable microbial population in the Palmottu groundwater and were present at up to 1.3 x 10(5) cells ml(-1). Sulfate-reducing bacteria (SRB) and acetogens could also be cultured from the Palmottu groundwater. The numbers of IRB and SRB were largest in groundwater with the lowest uranium concentrations. Removal of dissolved U(VI) from solution was concomitant with the growth of IRB enrichment cultures and the reduction of iron. The redox buffer in the Palmottu groundwater consists of iron and uranium species, both of which are affected by IRB. IRB and aerobic heterotrophs were cultured from the Bangombé groundwater, where redox potentials are buffered by iron and organic carbon species. Microbial populations similar to those found at Palmottu and Bangombé are found throughout the Fennoscandian Shield, a potential host rock for subsurface radioactive waste disposal. These results confirm that microorganisms can be expected to play a role in stabilizing radioactive waste disposed of in the subsurface by lowering redox potential and immobilizing radionuclides.  相似文献   

15.
Commercially known Ahmer oxide paints are prepared from raw material mainly composed of red iron oxides (hematite) and iron oxyhydroxides. The raw material used in manufacturing of Ahmer oxide comes from some localities in southwest Sinai such as Abu Thor, Allouga, and El lehian. The adsorption of uranium and other radioelements on iron oxides could make the raw material (red iron oxides) and their products environmentally hazardous. The studied samples were subjected to radiometric analysis using NaI (Tl) gamma-ray spectrometer. The average activity concentration of U, Th, Ra, and K are 108.7, 458.8, 88.8, and 627.5?Bq?kg?1, respectively in raw material and 136.4, 14.6, 58.3, and 95.9?Bq?kg?1 in Ahmer oxide. High values of activity concentrations of 238U, 226Ra, and 40K were recorded in Allouga and El lehian raw material. High radioactivities of Allouga and El lehian raw material are mainly attributed to the presence of torbernite, zircon, and monazite, in addition to adsorbed elemental uranium in Ahmer oxide. absorbed dose rate (D), annual effective dose equivalent, radium equivalent activity (Raeq), external hazard index (Hex), and internal hazard index (Hin), as well as representative gamma index (Iγ) were determined from the activity concentrations of 226Ra, 232Th, and 40K. Some of the studied samples do not satisfy the universal standards.  相似文献   

16.
GOAL, SCOPE AND BACKGROUND: During the Balkan conflict in 1999, soil in contaminated areas was enriched in depleted uranium (DU) isotopic signature, relative to the in-situ natural uranium present. After the military activities, most of kinetic DU penetrators or their fragments remained buried in the ground in certain geomorphological and geochemical environments exposed to local weathering conditions. The contamination distribution, mobility and/or fixation of DU in the contaminated soil profile at one hot spot were the subject of our study. The results should disclose what happened with released DU corrosion products in three years elapsed, given the scope of their geochemical fractionation, and mark out the most probable host substrates in investigated soil type. METHODS: Gamma-spectrometric analysis of soil samples taken in the DU penetrator impact-zone was done to obtain present contamination levels. Set of samples is subjected to five-step and three-step sequential extraction procedures, specifically selective to different physical/chemical associations in soil. The stable elements are determined in extracts by the atomic absorption spectroscopy. After the ion-exchange based uranium separation procedure, alpha-spectrometric analysis of obtained fractions was done and DU distribution in five extraction phases found from 235U/238U and 234U/238U isotopic ratios. RESULTS: Depleted uranium concentration falls down to the 1% of the initial value, at approximately 150 mm distance to the source. Carbonates and iron/manganese hydrous oxides are indicated as the most probable substrates for depleted uranium in the characterized soil type. Therefore, in the highly contaminated soil samples, depleted uranium is still weakly bonded and easy exchangeable. The significant levels of organic-bonded depleted uranium are found in surface soil only. DISCUSSION: Dependence of the fractionation on the contamination levels is evident. Samples with higher DU contents have shown a longer maintenance in the exchangeable phases, probably because adsorption/desorption mass transfer through the medium was not very fast. Organic-bonded, depleted uranium is present in surface soil samples due to its higher humus content. Considering geochemical composition of investigated soil, the indicating chemical associations as substrates are in agreement with some considerations based on the results for low-level waste unsaturated zones. CONCLUSIONS: The soil contamination with depleted uranium in investigated area is still 'spot' type and not widespread. Dependence of the fractionation on the contamination levels and presence of weakly bonded, depleted uranium in the hot spots areas is evident. RECOMMENDATIONS AND PERSPECTIVES: A detailed study may be undertaken with suitable extractive reagents to define a bio-available fraction of depleted uranium in soil. The comparison of results for different soil types investigated by the same methodology may be useful. An applied combination of physical/chemical procedures and analysis may help in the decision making on the remediation strategy for sites contaminated with depleted uranium used in military operations.  相似文献   

17.

Groundwater pollution of the watershed is mainly influenced by the multifaceted interactions of natural and anthropogenic processes. In this study, classic chemical and multivariate statistical methods were utilized to assess the groundwater quality and ascertain the potential contamination sources affecting the groundwater quality of Galma sub-watershed in a tropical savanna. For this purpose, the data set of 18 groundwater quality variables covering 57 different sampling boreholes (BH) was used. The groundwater samples essentially contained the cations in the following order of dominance: Ca2+ ?>?Na+ ?>?Mg2+ ?>?K+. However, the anions had HCO3?>?Cl?>?SO4–2?>?NO3 respectively. The hydrochemical facies classified the groundwater types of the sub-watershed into mixed Ca–Mg–Cl type of water, which means no cations and anions exceeds 50%. The second dominant water type was Ca–Cl. The Mg–HCO3 water type was found in BH 9, and Na–Cl water type in BH 29 of the studied area. The weathering of the basement rocks was responsible for the concentrations of these ions in the groundwater chemistry of the sub-watershed. Hierarchical cluster analysis (HCA) grouped the groundwater samples (boreholes) into five clusters that are statistically significant regarding the similarities of groundwater quality characteristics. The principal component analysis (PCA) extracted two major principal components explained around 65% of the variance and suggested the natural and anthropogenic processes especially the agricultural pollutants including synthetic fertilizers, and leaching of agricultural waste as the main factors affecting the groundwater quality. The integrated method proved to be efficient and robust for groundwater quality evaluation, as it guaranteed the precise assessment of groundwater chemistry in the sub-watershed of the tropical savanna. The findings of this investigation could be useful to the policy makers for developing effective groundwater management plans for the groundwater resources and protection of the sub-watershed.

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18.
Aquifer sediments collected via split-spoon sampling in two new groundwater wells in the 200-UP-1 operable unit at the Hanford Site were characterized and showed typical Ringold Unit E Formation properties dominated by gravel and sand. High iron-oxide content in Fe oxide/clay coatings caused the highest U(VI) adsorption as quantified by batch K(d) values, indicating iron oxides are the key solid adsorbent in the 200-UP-1 sediments that affect U(VI) fate and mobility. Even though U(VI) adsorption on the gravel-sized fraction of the sediments is considered to be negligible, careful characterization should be conducted to determine U(VI) adsorption on gravel, because of presence of Fe oxides coatings and diffusion-controlled adsorption into the gravel particles' interior surfaces. A linear adsorption isotherm was observed up to 10(-6) M (238 microg/L) of total U(VI) concentration in batch U(VI) adsorption tests with varying total U(VI) concentrations in spiked groundwater. U(VI) adsorption decreased with increasing concentrations of dissolved carbonate, because strong anionic aqueous uranium-carbonate complexes formed at high pH and high alkalinity conditions. Noticeable uranium desorption hysteresis was observed in a flow-through column experiment, suggesting that desorption K(d) values for aged uranium-contaminated sediments at the Hanford Site can be larger than adsorption K(d) values determined in short-term laboratory experiments and slow uranium release from contaminated sediments into the groundwater is expected.  相似文献   

19.
Little is known about the importance of drainage/irrigation channels and biogeochemical processes in arsenic distribution of shallow groundwaters from the Hetao basin. This investigation shows that although As concentrations are primarily dependent on reducing conditions, evaporation increases As concentration in the centre of palaeo-lake sedimentation. Near drainage channels, groundwater As concentrations are the lowest in suboxic-weakly reducing conditions. Results demonstrate that both drainage and irrigation channels produce oxygen-rich water that recharges shallow groundwaters and therefore immobilize As. Groundwater As concentration increases with a progressive decrease in redox potential along the flow path in an alluvial fan. A negative correlation between SO42− concentrations and δ34S values indicates that bacterial reduction of SO42− occurs in reducing aquifers. Due to high concentrations of Fe (>0.5 mg L−1), reductive dissolution of Fe oxides is believed to cause As release from aquifer sediments. Target aquifers for safe drinking water resources are available in alluvial fans and near irrigation channels.  相似文献   

20.
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