Uranium isotopes in groundwater from the continental intercalaire aquifer in Algerian Tunisian Sahara (Northern Africa)

The disequilibrium between ²³⁴U and ²³⁸U is commonly used as a tracer of groundwater flow. This paper aims to identify uranium contents and uranium isotopic disequilibria variation in groundwater sampled from deep Continental Intercalaire aquifer (southern Algeria and Tunisia). Large variations in both U contents (0.006–3.39 ppb) and ²³⁴U/²³⁸U activity ratios (0.4–15.38) are observed. We conduct a first assessment in order to verify whether the results of our investigation support and complete previous hydrogeological and isotopic studies. The dissolved U content and ²³⁴U/²³⁸U activity ratio data were plotted on a two-dimensional diagram that was successfully utilized on sharing the CI aquifer into different compartments submitted to different oxidising/reducing conditions and leads also to distinguished two preferential flow paths in the Nefzaoua/Chott Fejej discharge area. Uranium isotopes disequilibrium indicate that ranium chemistry is mainly controlled by water–rock interaction enhanced by long residence time recognised for this aquifer.     

Direct comparison of 210Po, 234Th and POC particle-size distributions and export fluxes at the Bermuda Atlantic Time-series Study (BATS) site

Particle-reactive, naturally occurring radionuclides are useful tracers of the sinking flux of organic matter from the surface to the deep ocean. Since the Joint Global Ocean Flux Study (JGOFS) began in 1987, the disequilibrium between ²³⁴Th and its parent ²³⁸U has become widely used as a technique to measure particle export fluxes from surface ocean waters. Another radionuclide pair, ²¹⁰Po and ²¹⁰Pb, can be used for the same purpose but has not been as widely adopted due to difficulty with accurately constraining the ²¹⁰Po/²¹⁰Pb radiochemical balance in the ocean and because of the more time-consuming radiochemical procedures. Direct comparison of particle flux estimated in different ocean regions using these short-lived radionuclides is important in evaluating their utility and accuracy as tracers of particle flux. In this paper, we present paired ²³⁴Th/²³⁸U and ²¹⁰Po/²¹⁰Pb data from oligotrophic surface waters of the subtropical Northwest Atlantic and discuss their advantages and limitations. Vertical profiles of total and particle size-fractionated ²¹⁰Po and ²³⁴Th activities, together with particulate organic carbon (POC) concentrations, were measured during three seasons at the Bermuda Atlantic Time-series Study (BATS) site. Both ²¹⁰Po and ²³⁴Th reasonably predict sinking POC flux caught in sediment traps, and each tracer provides unique information about the magnitude and efficiency of the ocean's biological pump.     

Uranium-thorium disequilibrium in north-east Atlantic waters

In this paper we report and compare the concentrations of 234Th and 238U measured in surface and subsurface waters collected in the course of a sampling campaign in the north east Atlantic in June-July 1998. Dissolved 234Th concentrations in surface waters ranged from 5 to 20 Bq m(-3), showing a large deficiency relative to 238U concentrations (typically 42 Bq m-3). This disequilibrium is indicative of active 234Th scavenging from surface waters. Observed 234Th/238U activity ratios, together with corresponding 234Th particulate concentrations, were used to calculate mean residence times for 234Th with respect to scavenging onto particles (tau(diss)) and subsequent removal from surface waters (tau(part)). Residence times in the range 5-30 days were determined for tau(diss) and 4-18 days for tau(part) (n=14). In addition, ultrafiltration experiments at six stations in the course of the same expedition revealed that in north-east Atlantic surface waters a significant fraction (46+/-17%; n=6) of the thorium in the (operationally-defined) dissolved phase (<0.45 microm) is in colloidal form. These observations are consistent with the 'colloidal pumping' model in which it is assumed that 234Th is rapidly absorbed by colloidal particles, which then aggregate, albeit at a slower rate, into larger filterable particles. In essence, colloids act as intermediaries in the transition from the fully dissolved to the filter-retained (>0.45 microm) phase. Thus, the time (tau(c)) for fully dissolved 234Th to appear in the filter-retained fraction is dependent on the rate of colloidal aggregation. Here, we determined tau(c) values in the range 3-17 days.     

Uranium isotopes in Tunisian bottled mineral waters

²³⁴U and ²³⁸U activity concentrations and their relative effective doses have been determined in 10 bottled mineral waters in Tunisia. Alpha spectrometry was used as technique to measure uranium isotopes. The obtained isotopic ratio ²³⁴U/²³⁸U varies between 1.1 and 3 which means that the two isotopes are not in radioactive equilibrium. Measured activity concentration varies between 3.2 and 40 mBq/l for ²³⁴U and between 1.5 and 26.3 mBq/l for ²³⁸U. Effective doses (assuming 2 litres per day of water consumption) coming from this two isotopes are found to vary between 0.16 and 2.02 μSv/a which is lower than the maximum recommended dose level by the WHO.     

Anthropogenic radionuclides in sediment in the Japan Sea: distribution and transport processes of particulate radionuclides

Distributions of anthropogenic radionuclides (⁹⁰Sr, ¹³⁷Cs and ^239+240Pu) in seabed sediment in the Japan Sea were collected during the period 1998–2002. Concentration of ⁹⁰Sr, ¹³⁷Cs and ^239+240Pu in seabed sediment was 0.07–1.6 Bq kg⁻¹, 0.4–9.1 Bq kg⁻¹ and 0.002–1.9 Bq kg⁻¹, respectively. In the northern basin of the sea (Japan Basin), ^239+240Pu/¹³⁷Cs ratios in seabed sediment were higher and their variation was smaller compared to that in the southeastern regions of the sea. The higher ^239+240Pu/¹³⁷Cs ratios throughout the Japan Basin were considered to reflect production of Pu-enriched particles in the surface layer and substantial sinking of particulate materials in this region. In the southern regions of the Japan Sea (<38°N), both inventories and ^239+240Pu/¹³⁷Cs ratios in sediment were larger than those in the other regions. In the southern Japan Sea, observations suggested that supply of particulate radionuclides by the Tsushima Warm Current mainly enhanced accumulation of the radionuclides in this region.     

Radionuclide content of building materials and associated gamma dose rates in Egyptian dwellings

Studies have been carried out to determine the natural radioactivity in some building materials (bricks, tiles, marble and ceramics) and their associated radiation hazard. The radioactivity concentrations of ²²⁶Ra ²³²Th and ⁴⁰K were measured using a gamma spectrometer with a Hp–Ge detector. The activities of ²³⁸U and ²³⁴U were measured using an alpha-spectrometer with a surface barrier detector after applying a radiochemical procedure. The ²³⁴U/²³⁸U isotopic ratios were calculated. The radium equivalent activities and the radiation hazard index associated with the natural radionuclides were calculated. A computer program was developed and applied to calculate the dose rate a person will receive from the walls of a room constructed from the studied building materials.     

Determination of total content and isotopic compositions of plutonium and uranium in environmental samples for safeguards purposes by ICP-QMS

The aim of this work was to determine the concentrations and isotopic compositions of plutonium and uranium in environmental samples for safeguards purposes. An analytical method was developed with a plutonium and uranium separation procedure based on extraction chromatography (using 2 mL TEVA and UTEVA columns) and detection with a quadrupole ICP-MS applying an ultra-sonic nebulizer coupled with a membrane desolvation system. Starting from blank swipes, the background equivalent concentration (BEC) was 8 fg for ²³⁹Pu and 1 ng ²³⁸U. The method was successfully applied to certified reference materials as well as to round robin samples obtained in the framework of the inter-laboratory exercise program, promoted by the Brazilian–Argentine Agency for Accounting and Control of Nuclear Materials (ABACC), together with the US Department of Energy (USDOE). After the introduction of an additional ion-exchange separation step, the methodology was applied to the IAEA-384 sediment reference sample with precise and accurate total plutonium and uranium, ²⁴⁰Pu/²³⁹Pu, ²⁴¹Pu/²³⁹Pu, ²³⁴U/²³⁸U and ²³⁵U/²³⁸U atomic ratio results.     

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.     

Fractionation of natural radionuclides in soils from the vicinity of a former uranium mine ?irovski vrh, Slovenia

As a result of former uranium mining and milling activities at ?irovski vrh, Slovenia, 0.6 million tons of uranium mill tailings (UMT) were deposited onto a nearby waste pile Boršt. Resulting enhanced levels of natural radionuclides in UMT could pose threat for the surrounding environment. Therefore, sequential extraction protocol was performed to assess mobility and bioavailability of ²³⁸U, ²³⁴U, ²³⁰Th and ²²⁶Ra in soils from the waste pile and its surrounding. The radionuclides associated with exchangeable, organic, carbonate, Fe/Mn oxides and residual fraction, respectively, were determined. Results showed that the highest activity concentrations for the studied radionuclides were on the bottom of the waste pile. In non-contaminated locations, about 80% of all radionuclides were in the residual fraction. Considering activity concentrations in the UMT, ²³⁸U and ²³⁴U are the most mobile. Mobility of ²²⁶Ra is suppressed by high sulphate concentrations and is similar to mobility of ²³⁰Th.     

Suitable gamma energy for gamma-spectrometric determination of U in surface soil samples of a high rainfall area in India

The paper presents a systematic study on suitability of various gamma lines for monitoring of ²³⁸U activity in soil samples around a uranium mineralized zone of Kylleng Pyndengsohiong Mawthabah (Domiasiat), Meghalaya in India. The area lies in a plateau region which recieves the highest average annual rainfall (12,000 mm) in the world. The geochemical behaviour of the uranium and its daughter products at such wet climatic conditions imposes restrictions to assess ²³⁸U through gamma lines of radon decay products. Soil samples were collected from nine locations around the uranium mineralization zone for analysis. The ratio of the concentration of uranium obtained from gamma energies of radium daughter products to the 63.29 keV of ²³⁴Th was found to vary from 1.01 to 2.07, which indicates a pronounced disequilibrium between uranium and radium daughters. The results obtained from various gamma energies were validated from the data generated by Instrumental Neutron Activation Analysis (INAA) technique. The ²³⁸U activities from the two analytical methods show a well fitted regression line with correlation coefficient 0.99 which validates the reliability of 63.29 keV energy for estimation of uranium in such conditions.     

The transfer of 60Co from feed into vitamin B12 in cow liver,milk and beef

The transfer of the radionuclide ⁶⁰Co from feed to milk, meat and the organs of a cow and its incorporation into vitamin B12 were studied in order to determine the transfer coefficient of ⁶⁰Co into vitamin B12 in cattle. Upper limits of transfer coefficients for ⁶⁰Co organically complexed into vitamin B12 were determined to be 6·0 × 10⁻⁵ days/litre in milk and 3·9 × 10⁻⁵ days/kg in meat, based on values measured after 140 days in bovine liver.     

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.     

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.     

Biomagnification of 7Be, 234Th, and 228Ra in marine organisms near the northern Pacific coast of Japan

Enrichment of natural radionuclides of thorium, radium and beryllium in several kinds of marine organisms was investigated near the Pacific coast of Miyagi Pref., Japan. The radioactivity of 7Be, 210Pb, 234Th, 238U, 228Ra and 137Cs was measured using gamma spectrometry. High concentrations of 234Th were observed in ascidian livers (50-400 Bq/kg dry) and excrement (2000-2900 Bq/kg dry), although the parent 238U concentrations were less than 3 Bq/kg dry. Such extreme disequilibrium between 238U and 234Th activity was observed in other organisms (barnacles, mussels and brown algae). Relatively high concentrations of 228Ra were detected in ascidian livers and were observed to decrease according to its half-life (5.75 year), suggesting disequilibrium with its parent 232Th. High concentrations (about 1900-5000 Bq/kg dry) of 7Be were detected in ascidian liver. Possible mechanisms for the observed biomagnification and bioaccumulation of these radionuclides in the organisms analyzed were proposed.     

Environmental characterization and radio-ecological impacts of non-nuclear industries on the Red Sea coast

The Red Sea is a deep semi-enclosed and narrow basin connected to the Indian Ocean by a narrow sill in the south and to the Suez Canal in the north. Oil industries in the Gulf of Suez, phosphate ore mining activities in Safaga-Quseir region and intensified navigation activities are non-nuclear pollution sources that could have serious radiological impacts on the marine environment and the coastal ecosystems of the Red Sea. It is essential to establish the radiological base-line data, which does not exist yet, and to investigate the present radio-ecological impact of the non-nuclear industries to preserve and protect the coastal environment of the Red Sea. Some natural and man-made radionuclides have been measured in shore sediment samples collected from the Egyptian coast of the Red Sea. The specific activities of 226Ra and 210Pb (238U) series, 232Th series, 40K and 137Cs (Bq/kg dry weight) were measured using gamma ray spectrometers based on hyper-pure germanium detectors. The specific activities of 210Po (210Pb) and uranium isotopes (238U, 235U and 234U) (Bq/kg dry weight) were measured using alpha spectrometers based on surface barrier (PIPS) detectors after radiochemical separation. The absorbed radiation dose rates in air (nGy/h) due to natural radionuclides in shore sediment and radium equivalent activity index (Bq/kg) were calculated. The specific activity ratios of 228Ra/226Ra, 210Pb/226Ra, 226Ra/238U and 234U/238U were calculated for evaluation of the geo-chemical behaviour of these radionuclides. The average specific activity of 226Ra (238U) series, 232Th series, 40K and 210Pb were 24.7, 31.4, 427.5 and 25.6 Bq/kg, respectively. The concentration of 137Cs in the sediment samples was less than the lower limit of detection. The Red Sea coast is an arid region with very low rainfall and the sediment is mainly composed of sand. The specific activity of 238U, 235U and 234U were 25.3, 2.9 and 25.0 Bq/kg. The average specific activity ratios of 226Ra/228Ra, 210Pb/226Ra and 234U/238U were 1.67, 1.22 and 1.0, respectively. The relationship between 226Ra/228Ra activity ratio and sample locations along the coastal shoreline indicates the increase of this ratio in the direction of the Shuqeir in the north and Safaga in the south where the oil exploration and phosphate mining activities are located. These activities may contribute a high flux of 226Ra. The concentration and distribution pattern of 226Ra in sediment can be used to trace the radiological impact of the non-nuclear industries on the Red Sea coast.     

Inverse dependency of particle residence times in ponds to the concentration of phosphate, the limiting nutrient

234Th, a commonly used short-lived particle-reactive tracer in marine systems, was measured in three different holding pond series at the Rocky Flats Environmental Technology Site (RFETS), Colorado, along with its parent nuclide 238U, to determine steady-state residence times of particle-reactive actinides such as Pu, and of particles. Series B ponds, which received industrial effluent that includes ortho-phosphate (PO4) and actinides, differed from series A and C ponds, which did not. This difference was also evident in the calculated particle residence times, which were <1 day for the ponds B4 and B5, where PO4 concentrations were higher (1.4 and 1.8 mg/l), and 3 and 3.4 days for ponds A3 and C2, respectively, where ortho-phosphate concentrations were lower (<0.1 mg/l). Particle residence times thus showed an inverse relationship with the concentration of ortho-phosphate, the limiting nutrient in fresh water systems. The same relationship to the concentration of ortho-phosphate or any of the other nutrient elements was not evident for the residence times of dissolved 234Th, which ranged between 0.1 and 2 days. This can be attributed to higher concentrations of dissolved and particulate ligands with greater binding potential for actinides such as four-valent Th and Pu in ponds with higher ortho-phosphate concentrations. Regardless of actual ortho-phosphate concentration, however, at water residence (holding) times of 1 month in these ponds, particles and associated actinides would be expected to be completely removed from the pond water to sediments.     

Uranium isotopes in groundwater from the “Jeffara coastal aquifer” (southeastern Tunisia)

The distributions of ²³⁸U and ²³⁴U in groundwater from the “Jeffara aquifer” were studied by using alpha spectrometric methods. The concentration ranges of ²³⁸U and ²³⁴U/²³⁸U activity ratios were 1.34 ± 0.17 to 3.43 ± 0.38 ppb, and 1.43 ± 0.23 to 1.82 ± 0.27 respectively. Variations in concentrations can be related not only to lithostratigraphic formations but also to different origins of groundwater. U content of Jeffara are found very similar to those of Continental Intercalaire aquifer in both El Hamma and Chenchou regions, indicating that the Continental Intercalaire is the dominant source of the groundwater.     

Fallout distribution in Padua and Northeast Italy after the chernobyl nuclear reactor accident

The radioactive cloud from the Chernobyl nuclear reactor accident arrived in northeast Italy on 30 April 1986. Ground-level air activities detected in Padua reached maximum values of 28·6, 19·2, 3·3, 1·7 and 7·5 Bq m⁻³ for ¹³¹I, ¹³²Te(¹³²I), ¹³⁷Cs and ¹⁰³Ru, respectively, on 1 May; about 10 days later, the activities had fallen to less than 1% of peak values. Considerations of cloud homogeneity are reported.The distribution of fallout radionuclides in Padua was evaluated on the basis of radioactivity detected on natural surfaces. The average committed dose equivalent to the thyroid for adult people in Padua through ¹³¹I inhalation was estimated at 0·37 mSv. Soil activity was monitored daily in samples collected in Padua during the first weeks of May 1986. Fallout deposition over northeast Italy was measured on 75 surface soil samples collected during June 1986 and long-lived radionuclide distribution maps were derived.     

The distribution and inventory of fallout plutonium in sediments of the Ligurian Sea near La Spezia,Italy

Pu concentrations in surface sediments of the Ligurian Sea are about ten times higher than in adjacent river sediments and are highly correlated with sediment porosities. The integrated inventory of ^239,240Pu in a sediment core is calculated to be 3·5 mCi km^?2, nearly twice the average input from fallout at these latitudes, apparently because Pu is removed from seawater by particle scavenging.The sedimentation rate is calculated from the depth of the ^239,240Pu maximum to be 0·52 ± 0·06 cmy^?1.     

Size distributions and growth of natural and chernobylderived submicron aerosols in Tennessee

The median aerodynamic diameters of aerosol-associated SO₄²⁻, ²¹⁰Pb, ⁷Be, and Chernobyl-derived fission products in Tennessee were examined using high-volume cascade impactors. Regardless of season, the ‘steady-state’ size distributions of SO₄²⁻ shifted to larger sizes than found for either ²¹⁰Pb or ⁷Be, and for ⁷Be sizes showed a weaker seasonal dependency than for either SO₄²⁻ or ²¹⁰Pb. It is suggested that the size differences are the result of the different spatial distributions of these species in the atmosphere during aerosol formation and growth. The mean growth rate of aerosols between ≈0·2 μm and ≈0·4 μm was estimated to be ≈0·03 μm d⁻¹ from a comparison of the median diameter of ²¹⁰Pb when it is first produced from ²¹⁴Po decay with the median diameter after a mean atmospheric residence time of 7 d.Measurements of the size distributions of radioactive aerosols released during the nuclear reactor accident at Chernobyl were made in May and June 1986, and provided rare information on growth rates of aerosols released to the atmosphere over a short time period. A linear growth rate of ≈0·013 μm d⁻¹ was observed in the lower troposphere after the median diameter had reached ≈0·4 μm. Chernobyl-derived ^134,137Cs was less soluble than ⁷Be, suggesting the presence of an aerosol core derived from reactor constituents. An analysis of time intervals and trends in both concentrations and isotopic ratios, when compared to Soviet data on the time course of radioactive releases from the damaged reactor, suggested that the large releases which occurred in early May were an important component of the globally transported ¹³⁷Cs.