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1.
A method by inductively coupled plasma mass spectrometry (ICP-MS) was developed which allows the measurement of (236)U at concentration ranges down to 3 x 10(-14)g g(-1) and extremely low (236)U/(238)U isotope ratios in soil samples of 10(-7). By using the high-efficiency solution introduction system APEX in connection with a sector-field ICP-MS a sensitivity of more than 5,000 counts fg(-1) uranium was achieved. The use of an aerosol desolvating unit reduced the formation rate of uranium hydride ions UH(+)/U(+) down to a level of 10(-6). An abundance sensitivity of 3 x 10(-7) was observed for (236)U/(238)U isotope ratio measurements at mass resolution 4000. The detection limit for (236)U and the lowest detectable (236)U/(238)U isotope ratio were improved by more than two orders of magnitude compared with corresponding values by alpha spectrometry. Determination of uranium in soil samples collected in the vicinity of Chernobyl nuclear power plant (NPP) resulted in that the (236)U/(238)U isotope ratio is a much more sensitive and accurate marker for environmental contamination by spent uranium in comparison to the (235)U/(238)U isotope ratio. The ICP-MS technique allowed for the first time detection of irradiated uranium in soil samples even at distances more than 200 km to the north of Chernobyl NPP (Mogilev region). The concentration of (236)U in the upper 0-10 cm soil layers varied from 2 x 10(-9)g g(-1) within radioactive spots close to the Chernobyl NPP to 3 x 10(-13)g g(-1) on a sampling site located by >200 km from Chernobyl.  相似文献   

2.
Soil samples collected from locations in Kosovo where depleted uranium (DU) ammunition was expended during the 1999 Balkan conflict were analysed for uranium and plutonium isotopes content (234U, 235U, 236U, 238U, 238Pu, (239 + 240)Pu). The analyses were conducted using gamma spectrometry (235U, 238U), alpha spectrometry (238Pu, (239 + 240)Pu), inductively coupled plasma-mass spectrometry (ICP-MS) (234U, 235U, 236U, 238U) and accelerator mass spectrometry (AMS) (236U)). The results indicated that whenever the U concentration exceeded the normal environmental values (approximately 2 to 3 mg/kg) the increase was due to DU contamination. 236U was also present in the released DU at a constant ratio of 236U (mg/kg)/238U (mg/kg) = 2.6 x 10(-5), indicating that the DU used in the ammunition was from a batch that had been irradiated and then reprocessed. The plutonium concentration in the soil (undisturbed) was about 1 Bq/kg and, on the basis of the measured 238Pu/(239 + 240)Pu, could be entirely attributed to the fallout of the nuclear weapon tests of the 1960s (no appreciable contribution from DU).  相似文献   

3.
The Kadji-Sai abandoned field of U-bearing brown coal on the southern coast of Lake Issyk-Kul (Kyrgyzstan) poses a threat of radioactive pollution to the world's fifth deepest and second largest pristine highland lake. The valleys of ephemeral streams in the lake catchment are filled with coarse-grained sand and clay, with a background U--Ra activity of 35--55 Bqkg(-1). High activity areas vs. this background come from three sources: (1) scarce outcrops of uraniferous brown coal and mining wastes containing fragments of this coal with (238)U/(226)Ra ratios of 0.8 due to uranium losses through weathering; (2) manmade anomalies caused by a radioactive waste dump, where U was extracted from the ash of coal burnt at a coal-fired power plant. As a result, the (238)U/(226)Ra ratios become 0.15--0.25; (3) six catch pools terraced below the mine, where U activity decreases downslope, and (238)U/(226)Ra ratios reach 150--200. Uranium lost in the extraction process may have been retained on the terraces. The distribution pattern of radionuclides in the bottom sediments of the lake is controlled by water depth and offshore distance. The upper section of homogeneous limy--argillic deposits in the lake center remains undisturbed by currents, as indicated by regular sub-exponential distribution of atmospheric (137)Cs and (210)Pb(atm). Sedimentation rate in the lake center for the past century, found from (210)Pb, was 0.32 mmyr(-1). (238)U/(226)Ra in deep-water sediments was about 3. The activity of uranium adsorbed by sediments from the lake water was estimated by subtraction of the Ra-equilibrium component from the total U activity. Thus, the flux of dissolved U to the bottom sediments was as 2.07 x 10(-7)gcm(-2)yr(-1). The upper section of near-shore deposits was disturbed by currents, with (137)Cs and (210)Pb(atm) more or less uniformly distributed in this layer. Peaks of (226)Ra and (210)Pb occur at different depths from 5 to 20 cm below the sediment surface, with (238)U/(226)Ra ratios 0.28--0.44. The presence of mullite in these sediments indicated that radioactive ash penetrated into the lake in the past. At present, (226)Ra in the ash is buried under a non-radioactive cap.  相似文献   

4.
A January 1966 accident dispersed Pu and other nuclear bomb materials in the vicinity of Palomares, a village in southeastern Spain. Radioactive particles were identified in a soil sample collected in 1998 and analytical results obtained from one of the isolated particles are presented here. Isolation of the particle was performed using gamma-ray spectrometry and imaging plates. Scanning electron microscopy with X-ray microanalysis revealed the presence of U and Pu as well as Pb and Fe in the particle of approximately 10microm diameter. Radioisotopes of U, Pu, and Am were quantified using radiometric methods, inductively coupled plasma mass spectrometry and secondary ion mass spectrometry. The elevated (235)U/(238)U atom ratio indicates enriched U, and the Pu atom ratios are consistent with weapons-grade material. This work demonstrates that the analysis of individual particles provides information not available through bulk sample analysis.  相似文献   

5.
During Balkan conflicts in 1994-1995, depleted uranium (DU) ordnance was employed and was left in the battlefield. Health concern is related to the risk arising from contamination of the environment with DU penetrators and dust. In order to evaluate the impact of DU on the environment and population in Bosnia and Herzegovina, radiological survey of DU in biological and water samples were carried out over the period 12-24 October 2002. The uranium isotopic concentrations in biological samples collected in Bosnia and Herzegovina, mainly lichens, mosses and barks, were found to be in the range of 0.27-35.7 Bq kg(-1) for (238)U, 0.24-16.8 Bq kg(-1) for (234)U, and 0.02-1.11 Bq kg(-1) for (235)U, showing uranium levels to be higher than in the samples collected at the control site. Moreover, the (236)U in some of the samples was detectable. The isotopic ratios of (234)U/(238)U showed DU to be detectable in many biological samples at most sites examined, but in very low levels. The presence of DU in the biological samples was as a result of DU contamination in air. The uranium concentrations in water samples collected in Bosnia and Herzegovina were found to be in the range of 0.27-16.2 m Bq l(-1) for (238)U, 0.41-15.6 m Bq l(-1) for (234)U and 0.012-0.695 m Bq l(-1) for (235)U, and two water samples were observed to be DU positive; these values are much lower than those in mineral water found in central Italy and below the WHO guideline for public drinking water. From radiotoxicological point of view, at this moment there is no significant radiological risk related to these investigated sites in terms of possible DU contamination of water and/or plants.  相似文献   

6.
Isotopes of uranium in the sea-water sediments collected from two different areas (El Hamraween harbour and Ras El Behar) on the Egyptian coast of the red sea have been studied using radiochemical separation procedures and alpha-particle spectrometry. Activity concentrations of 238U, 235U, 234U were calculated. The activities observed indicated enhanced radioactivity levels in sea-water sediments of El Hamraween harbour area due to the activities of phosphate shipment operation. Secular equilibrium between 234U and 238U was found in the analyzed samples. The average activity ratio of 235U/238U was close to the value 0.046 for uranium in nature.  相似文献   

7.
Groundwaters from the Sebkhet Essijoumi drainage basin, situated in northern Tunisia, West of the city of Tunis, were sampled and analyzed for uranium and radium isotopes. Low (234)U/(238)U activity ratios coupled with relatively high (228)Ra and (238)U concentrations were found in the Manouba plain phreatic aquifer, at the northern part of the basin, where remote sensing has indicated that this plain corresponds to the main humid zone of the area. Low (234)U/(238)U ratios probably reflected short residence time for waters in the Manouba plain, and high ratios longer residence time in the south, where water reaching the phreatic aquifer seems to have previously circulated in rocks constituting the southern hills. Assuming that, in the Manouba plain aquifer, the groundwater flows downstream from the Oued Lill pass area to the South-West of the Sebkha, the difference in the (228)Ra/(226)Ra activity ratio suggests that the residence time of water has been 2.8 years longer near the Sebkha than upstream.  相似文献   

8.
Uranium series isotopes in the Avon Valley, Nova Scotia   总被引:1,自引:0,他引:1  
An U-series isotopic study was carried out in the waters of the Avon Valley, Nova Scotia. The fresh and acidic recharge waters flow rapidly through the watershed composed of a granitic highland and a sedimentary, largely carbonate, lowland plain, before draining to the sea. There is no significant anthropogenic pollution; but, naturally elevated U levels can be encountered within the bedrock. Nonetheless, the U concentrations of the surface and groundwater are low (generally within the range of several hundredths to several tenths of a microg l(-1)), except in the proximity to weathering of U mineralization. The dissolved U in the surface waters appears to be stabilized by organic rather than inorganic complexes. Both the groundwaters and surface waters have similar (234)U/(238)U activity ratios that rarely deviate from secular equilibrium by more than 20% throughout the watershed. The magnitude of the (234)U/(238)U activity ratio is not determined by lithology but rather by the weathering mechanism, the high rate of flushing, and the leaching of local U mineralization. Dissolved Ra is consistently absent. The dissolved Rn concentrations, though variable, are measurable even in surface waters. This may be due to a continual degassing from the U-enriched bedrock or release from local sites of U mineralization underlying the surface water sources.  相似文献   

9.
This paper presents the results of a study into the anomalous 226Ra/238U disequilibrium (226Ra/238U of 0.5-9) exhibited by an upland organic soil in Co. Donegal, Ireland. Radiochemical speciation of 226Ra, 238U and 225Ra indicates that in this organic soil the high 226Ra/238U ratio is due to loss of 235U relative to 226Ra via oxidation and mobilisation of 238U in the upper layers of the soil and subsequent loss in solution. At the lower, more reducing depths of the soil profile, 238U and 226Ra are essentially in equilibrium. Loss of 238U appears to occur primarily from the easily oxidised organic and iron oxide fractions of the soil, samples exhibiting high 226Ra/238U ratios displaying significantly lower 238U levels in these fractions than samples whose ratio is below the average value for the soil of the valley. Selective enrichment of 226Ra by plants or preferential leaching of 226Ra from the underlying rock is not supported by the results of this study.  相似文献   

10.
The aim of this work was to determine the concentration of 234U and 238U and calculate the values of the 234U/238U activity ratio in waters and sediments from the various regions of the southern Baltic Sea: Gdańsk Deep, S?upsk Narrow and Bornholm Deep. The concentration of uranium in analysed sediments from southern Baltic increase with core depth to what probably is connected with diffusion from sediments to water through interstitial water, where uranium concentration is much higher than in bottom water. The highest concentrations of uranium were observed in sediments of S?upsk Narrow (0.66-7.11 mg kg(-1) d.w.) and S?upsk Bank (0.61-6.93 mg kg(-1) d.w.), the lowest in sediments from Bornholm Deep (0.54-3.77 mg kg(-1) d.w.). The 234U/238U activity ratio results indicated that the sedimentation of terrigenic material and Vistula River transport are the general sources of uranium in the southern Baltic sediments. The value of 234U/238U activity ratio in sediments from reduction areas from southern Baltic (Gdańsk Deep and Bornholm Deep) indicated that reduction process of U(VI) to U(IV) and removing of anthropogenic uranium from seawater to sediments constitutes a small part only in Gdańsk Deep.  相似文献   

11.
Phosphate and environmental samples were collected from Abu Tartor phosphate mine and the surrounding region. The activity concentration of 226Ra (238U) series, 232Th series and 40K were measured using a gamma-ray spectrometer. The activities of uranium isotopes (238U, 235U and 234U) and 210Pb were measured using an alpha spectrometer and a low-background proportional gas counting system, respectively, after radiochemical separation. The results are discussed and compared with the levels in phosphate rocks from different countries. It seems that the Abu Tartor phosphate deposit has the lowest radioactivity level of exploited phosphate of sedimentary origin. 226Ra/238U, 210Pb/226Ra, 234U/238U and 226Ra/228Ra activity ratios were calculated and are discussed. The radioactivity levels in the surrounding region and the calculated exposure dose (nGy/h) will be considered as a pre-operational baseline to estimate the possible radiological impacts due to mining, processing and future phosphate industrial activities. To minimize these impacts, the processing wastes should be recycled to the greatest possible extent.  相似文献   

12.
Gamma-ray spectrometry was used to determine uranium activity and investigate the presence of depleted uranium in soil samples collected from camping sites of the Greek expeditionary force in Kosovo. Assessment of 238U concentrations was based on measurements of the 63.3 keV and 92.38 keV emissions of its first daughter nuclide, 234Th. To determine the isotopic ratio of 238U/235U, secular equilibrium along the two radioactive series was first ensured and thereby the contribution of 235U under the 186 keV peak was deduced. The uranium activity in the samples varied from 48 to 112 Bq kg(-1), whereas the activity ratio of 238U/235U averaged 23.1+/-4.3.  相似文献   

13.
A reconnaissance study has been made on the distribution of 238U, 234U, 232Th and 230Th in soils, water, suspended particulate matter (SPM) and bottom sediments in the Kali river basin around Kaiga, its estuarine region and the adjacent Arabian Sea to obtain the baseline data of U-Th series nuclides in view of the commissioning of nuclear power reactors at Kaiga, near Karwar, on the southwest coast of India. Drainage basin soils developed over greywackes (the dominant litho-unit upstream) are lower in 238U/Al and 232Th/Al ratios by factors of 3-5 in comparison with those developed over tonalitic gneisses (the dominant litho-unit downstream). The dominance of the former type of soils is reflected in the composition of river-bottom sediments derived from the upstream drainage basin during the monsoon. The 232Th in bottom sediments tends to increase towards the estuarine and coastal areas, presumably due to deposition of heavy minerals and onshore transport of coastal sediments into the estuary. The dissolved U in the Kali river is low (0.001-0.02 microg/l) when compared to the major Indian rivers as the Kali river flows through U-poor greywackes. Thus, the input of dissolved U to the Kali estuary is dominated by sea water. Although there is some evidence for the removal of dissolved U at low salinity during estuarine mixing, its behaviour is conservative in the lower estuary (at higher salinities). The removal rate of dissolved U from the Kali river basin is similar to that reported from other tropical river basins. The U flux from all the west-flowing rivers of Peninsular India is estimated at 26.3 x 10(6) g/yr to the Arabian Sea which is about 2% of the flux from the Himalayan rivers to the Bay of Bengal.  相似文献   

14.
The oxidation states of uranium in depleted uranium (DU) particles were determined by synchrotron radiation based mu-XANES, applied to individual particles isolated from selected samples collected at different sites in Kuwait. Based on scanning electron microscopy with X-ray microanalysis prior to mu-XANES, DU particles ranging from submicrons to several hundred micrometers were observed. The median particle size depended on sources and sampling sites; small-sized particles (median 13 microm) were identified in swipes taken from the inside of DU penetrators holes in tanks and in sandy soil collected below DU penetrators, while larger particles (median 44 microm) were associated with fire in a DU ammunition storage facility. Furthermore, the (236)U/(235)U ratios obtained from accelerator mass spectrometry demonstrated that uranium in the DU particles originated from reprocessed fuel (about 10(-2) in DU from the ammunition facility, about 10(-3) for DU in swipes). Compared to well-defined standards, all investigated DU particles were oxidized. Uranium particles collected from swipes were characterized as UO(2), U(3)O(8) or a mixture of these oxidized forms, similar to that observed in DU affected areas in Kosovo. Uranium particles formed during fire in the DU ammunition facility were, however, present as oxidation state +5 and +6, with XANES spectra similar to solid uranyl standards. Environmental or health impact assessments for areas affected by DU munitions should therefore take into account the presence of respiratory UO(2), U(3)O(8) and even UO(3) particles, their corresponding weathering rates and the subsequent mobilisation of U from oxidized DU particles.  相似文献   

15.
Both soil and plant samples of nine different plant species grown in soils from southeastern China contaminated with uranium mine tailings were analyzed for the plant uptake and translocation of 238U, 226Ra and 232Th. Substantial differences were observed in the soil-plant transfer factor (TF) among these radionuclides and plant species. Lupine (Lupinus albus) exhibited the highest uptake of 238U (TF value of 3.7x10(-2)), while Chinese mustard (Brassica chinensis) had the least (0.5x10(-2)). However, in the case of 226Ra and 232Th, the highest TFs were observed for white clover (Trifolium pratense) (3.4x10(-2)) and ryegrass (Lolium perenne) (2.1x10(-3)), respectively. 232Th in the tailings/soil mixture was less available for plant uptake than 226Ra or 238U, and this was especially evident for Chinese mustard and corn (Zea mays). The root/shoot (R/S) ratios obtained for different plants and radionuclides shown that Indian mustard had the smallest R/S ratios for both 226Ra (5.3+/-1.2) and 232Th (5.3+/-1.7), while the smallest R/S ratio for 238U was observed in clover (2.8+/-0.9).  相似文献   

16.
Lichens are widely used to assess the atmospheric pollution by heavy metals and radionuclides. However, few studies are available in publications on using lichens to qualitatively assess the atmospheric pollution levels. The paper presents research results applying epiphytic lichens as bio-monitors of quantitative atmospheric contamination with uranium. The observations were conducted during 2.5 years in the natural environment. Two experimental sites were used: one in the vicinity of a uranium contamination source, the other one - at a sufficient distance away to represent the background conditions. Air and lichens were sampled at both sites monthly. Epiphytic lichens Hypogimnia physodes were used as bio-indicators. Lichen samples were taken from various trees at about 1.5m from the ground. Air was sampled with filters at sampling stations. The uranium content in lichen and air samples as well as isotopic mass ratios (235)U/(238)U were measured by mass-spectrometer technique after uranium pre-extraction. Measured content of uranium were 1.45 mgkg(-1) in lichen at 2.09 E-04 microgm(-3) in air and 0.106 mgkg(-1) in lichen at 1.13 E-05 microgm(-3) in air. The relationship of the uranium content in atmosphere and that in lichens was determined, C(AIR)=exp(1.1 x C(LICHEN)-12). The possibility of separate identification of natural and man-made uranium in lichens was demonstrated in principle.  相似文献   

17.
238U and (232)Th concentrations and the extent of (238)U-(234)U-(230)Th radioactive equilibrium have been measured in a suite of Precambrian carbonates and black shales from the Lesser Himalaya. These measurements were made to determine their abundances in these deposits, their contributions to dissolved uranium budget of the headwaters of the Ganga and the Indus in the Himalaya and to assess the impact of weathering on (238)U-(234)U-(230)Th radioactive equilibrium in them. (238)U concentrations in Precambrian carbonates range from 0.06 to 2.07 microg g(-1). The 'mean' U/Ca in these carbonates is 2.9 ng U mg(-1) Ca. This ratio, coupled with the assumption that all Ca in the Ganga-Indus headwaters is of carbonate origin and that U and Ca behave conservatively in rivers after their release from carbonates, provides an upper limit on the U contribution from these carbonates, to be a few percent of dissolved uranium in rivers. There are, however, a few streams with low uranium concentrations, for which the carbonate contribution could be much higher. These results suggest that Precambrian carbonates make only minor contributions to the uranium budget of the Ganga-Indus headwaters in the Himalaya on a basin wide scale, however, they could be important for particular streams. Similar estimates of silicate contribution to uranium budget of these rivers using U/Na in silicates and Na* (Na corrected for cyclic and halite contributions) in river waters show that silicates can contribute significantly (approximately 40% on average) to their U balance. If, however, much of the uranium in these silicates is associated with weathering resistant minerals, then the estimated silicate uranium component would be upper limits.Uranium concentration in black shales averages about 37 microg g(-1). Based on this concentration, supply of U from at least approximately 50 mg of black shales per liter of river water is needed to balance the average river water U concentration, 1.7 microg L(-1) in the Ganga-Indus headwaters. Data on the abundance and distribution of black shales in their drainage basin are needed to test if this requirement can be met. (234)U/(238)U activity ratios in both carbonates and black shales are at or near equilibrium, thus preferential mobilization of (234)U from these deposits, if any, is within analytical uncertainties. (230)Th is equivalent to or in excess of (238)U in most of the carbonates. (230)Th/(238)U>1 indicates that during weathering, uranium is lost preferentially over Th. (232)Th concentrations in carbonates are generally quite low, <0.5 microg g(-1), though with a wide range, 0.01-4.8 microg g(-1). The variation in its concentrations seem to be regulated by aluminosilicate content of the carbonates as evident from the strong positive correlation between (232)Th and Al.  相似文献   

18.
Radiochemical results (238U, 226Ra and 228Ra activities; 234U/238U, 228Ra/226Ra and 226Ra/238U activity ratios) are reported for 42 natural water samples collected from wells, hot mineral springs, rivers, tap water, lakes and irrigation water in 15 Moroccan locations. Results show that 238U activity varies between 4.5 and about 309 mBq l(-1) in wells, 0.6 and 8.5 mBq l(-1) in hot springs, 9.7 and 28 mBq l(-1) in rivers, 2.5 and 16 mBq l(-1) in tap waters and between 6 and 24 mBq l(-1) in lakes. The 234U/238U activity ratio varies in the range 0.87-3.35 in all analyzed water samples except for hot springs where it reaches values higher than 7. Unlike well water, mineral water samples present low 238U activities and high 234U/238U activity ratios and 226Ra activities. The highest activity of radium in mineral water is 150 times higher than the highest activity of 226 Ra found in well water. 226Ra/238U activity ratios are in the ranges 0.07-1.14 in wells, 0.04-0.38 in rivers, 0.04-2.48 in lakes, and 1.79-2115 in springs. The calculated equivalent doses to all the measured activities are inferior to the maximum contaminant levels recommended by the International Commission of Radioprotection and they do not present any risk for public health in Morocco.  相似文献   

19.
In order to determine whether or not uranium depleted in 235U and derived from the British Nuclear Fuels Ltd (BNFL) nuclear fuel reprocessingg plant at Sellafield, Cumbria, UK can be detected in environmental samples, we have investigated the isotopic composition of uranium in ammonium carbonate leachates from marine and terrestial samples from near Sellafield. Some show a depletion in 235U and the presence of 236U which unequivocally identifies the presence of uranium derived from BNFL. The 234U/238U activity ratio and total uranium content of samples are not significantly different from those of natural uranium abundances. The highest concentrations of uranium are found in anaerobic organic-rich silts and the lowest in sandy silts and coarse-grained sands.  相似文献   

20.
Radionuclides from past uranium mining in rivers of Portugal   总被引:2,自引:0,他引:2  
During several decades and until a few years ago, uranium mines were exploited in the Centre of Portugal and wastewaters from uranium ore milling facilities were discharged into river basins. To investigate enhancement of radioactivity in freshwater ecosystems, radionuclides of uranium and thorium series were measured in water, sediments, suspended matter, and fish samples from the rivers Vouga, D?o, Távora and Mondego. The results show that these rivers carry sediments with relatively high naturally occurring radioactivity, and display relatively high concentrations of radon dissolved in water, which is typical of a uranium rich region. Riverbed sediments show enhanced concentrations of radionuclides in the mid-section of the Mondego River, a sign of past wastewater discharges from mining and milling works at Urgeiri?a confirmed by the enhanced values of (238)U/(232)Th radionuclide ratios in sediments. Radionuclide concentrations in water, suspended matter and freshwater fish from that section of Mondego are also enhanced in comparison with concentrations measured in other rivers. Based on current radionuclide concentrations in fish, regular consumption of freshwater species by local populations would add 0.032 mSv a(-1) of dose equivalent (1%) to the average background radiation dose. Therefore, it is concluded that current levels of enhanced radioactivity do not pose a significant radiological risk either to aquatic fauna or to freshwater fish consumers.  相似文献   

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