Spatial distribution of U isotopes in sea-water sediments, Red Sea, Egypt

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.     

90Sr, 238U, 234U, 137Cs, 40K and 239/240Pu in Emmental type cheese produced in different regions of Western Europe

A method is presented for the determination of (90)Sr and uranium in Emmental type cheese collected in dairy plants from different European countries. Results display a significant correlation (r = 0.708 Student t-test = 6.02) between the (90)Sr content of the cheese and the altitude of grazing. The highest (90)Sr activity is 1.13 Bq kg(-1) of cheese and the lowest is 0.29 Bq kg(-1). Uranium activity is very low with a highest (238)U value of 27 mBq kg(-1). In addition, (234)U/(238)U ratio shows a large enrichment in (234)U for every location. Without any significant indication of the geographic origin of the cheese, this enrichment is believed to be due to the geological features of the pasture, soil and underground water. These results tend to prove that the contamination of milk by uranium originates principally from the water that the cows drink instead of the forage. This finding may have a great importance in models dealing with dairy food contamination by radionuclides following a nuclear accident. Also, the (90)Sr content and to a lesser extent the (234)U/(238)U ratio could be used to trace the authenticity of the origin of the cheese. (137)Cs activity is lower than the detection limit of 0.1 Bq kg(-1) in all the samples collected (n = 20). Based on natural (40)K activity in cheese (15-21 Bq kg(-1)), the decontamination factor for the alkaline cations from milk to cheese is about 20. Plutonium activity stays below the detection limit of 0.3 mBq kg(-1).     

Marked disequilibrium between 234Th and 230Th of the 238U natural radioactive decay chain in IAEA reference materials n. 312, 313 and 314

A new laboratory for the spectroscopy of natural radioactivity with a good energy resolution is presented. It consists of two distinct parts equipped, respectively, the first one with a HpGe γ-ray detector, whose setup has been already completed, and the second one with large area Silicon α-ray detectors and a radiochemical section for thin α-samples preparation, whose setup is yet in progress and will be the argument of a separate work.The γ-ray spectrometer was calibrated by means of IAEA Reference Materials n. 312, 313, 314 and 375. A large difference from the predictions of secular equilibrium emerged between the activities of ²³⁴Th and ²³⁰Th in Materials n. 312, 313 and 314.     

Distribution of long-lived radionuclides of the 238U series in the sediments of a small river in a uranium mineralized region of Spain

A study is presented on the distribution and mobilization of the natural U isotopes (238U and 234U), 230Th, and 226Ra in the sediments of a small river crossing an uranium mineralized zone where a disused uranium mine is located. Due to the preferential directions for surface run-off waters and to the mine's situation, one sampling point along the river bed was identified as a point of accumulation of radionuclides. The average values of the activity concentrations (Bq/kg) in this sediment sample were 5,025, 5,055, 5,915 and 1,694 for 238U, 234U, 230Th and 226Ra, respectively, while the respective average values of the activity concentrations (Bq/kg) for the sediment sample considered to give the background level were 125, 124, 131 and 370. Isotopic ratios between the descendants of 238U served to clarify some paths of distribution, involving the soils nearest to the sampling points and the location of these points with respect to the disused mine. The differences in behaviour found between the uranium, thorium and radium isotopes were associated to the mobility of these radionuclides in the fluvial system studied. Correlations between the radionuclide activity concentration ratios and stable element concentrations in the sediment samples were also investigated.     

(238)U, (234)U, (226)Ra, (210)Po concentrations of bottled mineral waters in Italy and their dose contribution

Due to the importance of bottled mineral water in human diet with special regard to children in lactation period, a monitoring of natural radioactivity in some bottled mineral waters produced in Italy was performed. Gross alpha and beta activities and (226)Ra, (238)U, (234)U, and (210)Po concentrations were measured. Gross alpha and beta activities were determined by standards ISO 9696 and ISO 9697; for (226)Ra determination liquid scintillation was used. The (238)U and (234)U concentrations were determined by alpha spectrometry after their separation from matrix by extraction chromatography and electroplating. (210)Po was measured by alpha spectrometry. The results revealed that the concentrations (mBqL(-1)) of (226)Ra, (238)U, (234)U, and (210)Po ranged from <10.00 to 52.50, from <0.17 to 89.00, from <0.17 to 79.00, and from <0.04 to 21.01, respectively. Uranium and radium concentrations do not reach the relevant recommended derived activity concentration (DWC). For polonium concentration, none of the samples reaches the relevant DWC in the case of adults and children, but one sample exceeds this value for infants. The dose contribution for different classes of age was calculated using the dose coefficient factors reported by EC Directive 96/29 EURATOM and certain annual intake. For children and adult age class, the calculated doses are quite similar and lower than 0.1mSvy(-1); for infants (<1y) in three cases the calculated dose ranges from 0.11 to 0.17mSvy(-1).     

238U series isotopes and 232Th in carbonates and black shales from the Lesser Himalaya: implications to dissolved uranium abundances in Ganga-Indus source waters

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.     

Radioactive and radiogenic isotopes in sediments from Cooper Creek, Western Arnhem Land

Protection of the environment post-mining is a key objective of rehabilitation, especially where runoff and erosion from rehabilitated mine sites could potentially lead to contamination of the surrounding land and watercourses. As part of an overall assessment of the success of rehabilitation at the former Nabarlek uranium (U) mine, an appraisal of stable lead (Pb) isotopes, radionuclides and trace metals within sediments and soils was conducted to determine the off site impacts from a spatial and temporal perspective. The study found localised areas on and adjacent to the site where soils had elevated levels of trace metals and radionuclides. Lead isotope ratios are highly radiogenic in some samples, indicating the presence of U-rich material. There is some indication that erosion products with more radiogenic Pb isotope ratios have deposited in sediments downstream of the former ore body. However, there is no indication that the radiogenic erosion products found on the mine site at present have significantly contaminated sediments further downstream of Cooper Creek.     

Heavy metals in water, sediments, plants and fish of Kali Nadi U.P. (India)

The distribution of heavy metals viz., Cd, Co, Cr, Cu, Fe, Mn, Ni, Pb and Zn in the water, sediments, plants and fish samples collected from the Kali Nadi (India) have been determined. The studies have shown that there was considerable variation in the concentration of heavy metals from one sampling station to the other which may be due to the variation in the quality of industrial and sewage wastes being added to the river at different places. The orders of the concentration of heavy metals in water, sediments, plants (Eicchornia crassipes) and fish (Heteropnuestes fossilis) were Fe > Zn > Cu > Mn > Cr > Ni > Pb > Co > Cd; Fe > Zn > Mn > Ni > Cr > Co > Cu > Pb > Cd; Fe > Mn > Zn > Cu > Ni > Co > Pb > Cr > Cd and Fe > Zn > Mn > Ni > Pb > Co > Cr > Cu > Cd, respectively.     

Spatiotemporal variation of dissolved (238)U in the Gironde fluvial-estuarine system (France)

Dissolved uranium ((238)U(D)) was measured within the Gironde fluvial-estuarine system (France), which is well known for its heavy metal pollution and its subsequent environmental effects. Dissolved (238)U activities exhibit the highest levels and variability in the small watersheds of the Isle and Riou-Mort rivers, ascribed to low discharges and the occurrence of peculiar features (local U ore deposits; Permian layers). The major tributaries of the Gironde Estuary: Garonne, Lot and Dordogne, show rather stable (238)U(D), higher than the global mean riverine uranium activity. In the Gironde Estuary (238)U(D) behaves conservatively along the river-estuary-ocean transect. Dissolved (238)U distribution in the Gironde fluvial-estuarine system can be explained by the characteristics of considered drainage basins. There is no evidence of anthropogenic pollution.     

234U and 230Th determination by FIA-ICP-MS and application to uranium-series disequilibrium in marine samples

A 234U and 230Th determination method based on an extraction chromatographic separation on a flow injection system coupled to a quadruple ICP-MS was developed. Two-milliliter UTEVA (Eichrom Co.) cartridges were applied as separation tool and 236U and 229Th as spikes. Loading and washing steps were carried out in 3 M HNO3 solution and 0.05 M ammonium oxalate applied to elute both uranium and thorium. The method was applied initially to the IAEA-327 soil reference sample and NIST SRM 4357 ocean sediment reference material, with the obtained 234U and 230Th concentrations in agreement with the reference levels. Samples from a deep-sea sediment core (2450 m water depth) were analyzed and based on 230Th/234U dating, a mean sedimentation rate of 3.3 cm ky(-1) was calculated. Samples from two sediment layers were also dated by 14C-AMS and the observed ages agree with the 230Th/234U results.     

Contamination of the southern Baltic Sea with 137Cs and 90Sr over the period 2000-2004

Changes of the (137)Cs activity concentrations in the southern Baltic Sea waters were investigated over the period 2000-2004 and distribution of the (90)Sr concentrations was determined in 2004. In the discriminated period further decrease of (137)Cs concentrations was observed. The average activity concentration of (137)Cs declined from 59.4Bq/m(3) in 2000 to 45.1Bq/m(3) in 2004. The greatest changes of (137)Cs activities occurred in 2003 as a consequence of the medium-size inflow of a saline waters from the North Sea. This inflow affected (137)Cs activities as well as its distribution in the Baltic Sea. Changes in (90)Sr activity concentrations proceeded at much slower rate. The average activity concentration of (90)Sr was equal to 8.7Bq/m(3) in 2004. The annual fluvial (137)Cs fluxes from the Vistula river were also estimated. In 2000, the (137)Cs load from Vistula was of an order of 0.15TBq/year, and in 2004 0.05TBq/year.     

The inflow of (238)Pu and (239+240)Pu from the Vistula River catchment area to the Baltic Sea

The aim of the work was to estimate plutonium inflow from the Vistula River’s catchments area to the Baltic Sea. There were differences in plutonium activities depending on season and sampling site. The highest activities of ²³⁸Pu and ^239+240Pu were transported from the Vistula River watershed to the Baltic Sea in spring and the lowest in summer. Annually, the southern Baltic Sea is enriched via the Vistula River with 10.3 MBq of ²³⁸Pu and 89.0 MBq of ^239+240Pu. The enhanced concentration of plutonium in water from the Vistula River is the result of its runoff from the Vistula drainage area, mostly from snowmelt, enhanced rainfalls and leached materials from river bed.     

Influence of soil texture on the distribution and availability of 238U, 230Th, and 226Ra in soils

The influence of soil texture on the distribution and availability of (238)U, (230)Th, and (226)Ra in soils was studied in soil samples collected at a rehabilitated uranium mine located in the Extremadura region in south-west Spain. The activity concentration (Bqkg(-1)) in the soils ranged from 60 to 750 for (238)U, from 60 to 260 for (230)Th, and from 70 to 330 for (226)Ra. The radionuclide distribution was determined in three soil fractions: coarse sand (0.5-2mm), medium-fine sand (0.067-0.5mm), and silt and clay (<0.067 mm). The relative mobility of the natural radionuclides in the different fractions was studied by comparison of the activity ratios between radionuclides belonging to the same radioactive series. The lability of these radionuclides in each fraction was also studied through selective extraction from the soils using a one-step sequential extraction scheme. Significant correlations were found for (238)U, (230)Th, and (226)Ra between the activity concentration per fraction and the total activity concentration in the bulk soil. Thus, from the determination of the activity concentration in the bulk soil, one could estimate the activity concentration in each fraction. Correlations were also found for (238)U and (226)Ra between the labile activity concentration in each fraction and the total activity concentration in bulk soil. Assuming that there is some particle-size fraction that predominates in the process of soil-to-plant transfer, the parameters obtained in this study should be used as correction factors for the transfer factors determined from the bulk soil in previous studies.     

226Ra/238U disequilibrium in an upland organic soil exhibiting elevated natural radioactivity

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.     

Plutonium concentrations in waters from the southern Baltic Sea and their distribution in cod (Gadus morhua) skin and gills

The concentrations of (238)Pu and (239+240)Pu in water samples and suspended particulate fractions, as well as in colloidal fraction from the southern Baltic Sea are presented. The (239+240)Pu concentration in surface seawater samples fall within range from 5.2 mBq.m(-3) for Gdańsk Bay to 150 mBq.m(-3) for Pomeranian Bay, most of which (from 52 to 96%) constituted filterable forms (相似文献   

Radiological impact from atmospheric releases of 238U and 226Ra from phosphate rock processing plants

Phosphate rocks are used extensively, mainly as a source of phosphorus for fertilizers and secondarily for phosphoric acid and other speciality chemicals. Phosphates are typically enriched in uranium and are thus one of the sources of technologically enhanced natural radiation (TENR) which increases exposure to man from natural radionuclides. Emissions from phosphate rock processing plants in gaseous and particulate form contain radionuclides, such as 238U and 226Ra, which are discharged into the environment causing radiation exposures to the population. About 10 MBq each of 238U and 226Ra are discharged into the environment each year from SICNG, a phosphate rock processing plant in Thessaloniki area, Northern Greece. The collective dose commitment to lung tissue resulting from atmospheric releases was estimated to be approximately 2 x 10(-9) person Gy t-1 for 238U and approximately 0.1 x 10(-9) person Gy t-1 for 226Ra, i.e. about 2 times higher than that estimated in the UNSCEAR reports issued in 1982, 1988, and 1993.     

On monitoring anthropogenic airborne uranium concentrations and (235)U/(238)U isotopic ratio by Lichen - bio-indicator technique

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.     

Origin and transport of U and Ra in riverine,estuarine and marine sediments of the Krka River,Croatia

Spatial distribution of ²³⁸U and ²²⁶Ra activities in sediment columns along the Krka River and estuary, were studied using gamma spectrometry. Markedly different ²³⁸U and ²²⁶Ra activities between riverine, estuarine and marine sediments were observed. Distribution of these radionuclides, as well as their anthropogenic and natural origin, was evaluated by activity measurements, taking into account sedimentation rates estimated by ¹³⁷Cs distribution in sediment columns.     

Scavenging of 234Th in the Eastern Irish Sea

Measurements of the disequilibria of ²³⁴Th/²³⁸U in seawater and in suspended particulate and seabed sediment in the eastern Irish Sea reveal that the residence time of dissolved ²³⁴Th (0·5–7·7 days) is controlled by the concentration of particles in suspension (0·4–6·9 mg litre⁻¹, which reflects the rate of sediment resuspension (0·5–5·9 kg m⁻²y⁻¹). The residence time of ²³⁴Th with respect to removal to the seabed is longer (7–50 d) and is less dependent on variations in the suspended load. Anthropogenic sources of ²³⁸U contribute up to 8–15% of the water column production of ²³⁴Th. Enhanced scavenging occurs near the coast and there appears to be a net horizontal flux of ²³⁴Th within this region.     

Distribution of uranium isotopes in surface water of the Llobregat river basin (Northeast Spain)

A study is presented on the distribution of ²³⁴U, ²³⁸U, ²³⁵U isotopes in surface water of the Llobregat river basin (Northeast Spain), from 2001 to 2006. Sixty-six superficial water samples were collected at 16 points distributed throughout the Llobregat river basin. Uranium isotopes were measured by alpha spectrometry (PIPS detectors). The test procedure was validated according to the quality requirements of the ISO17025 standard. The activity concentration for the total dissolved uranium ranges from 20 to 261 mBq L⁻¹. The highest concentrations of uranium were detected in an area with formations of sedimentary rock, limestone and lignite. A high degree of radioactive disequilibrium was noted among the uranium isotopes. The ²³⁴U/²³⁸U activity ratio varied between 1.1 and 1.9 and the waters with the lowest uranium activity registered the highest level of ²³⁴U/²³⁸U activity ratio. Correlations between uranium activity in the tested water and chemical and physical characteristics of the aquifer were found.