Investigation of dissolved uranium content in the watershed of Seine River (France)

A systematic survey of dissolved uranium activity was carried out in the Seine and the Marne over one year. A small watershed, the Grand Morin, included in the Seine one, was also investigated from stream to medium-sized rivers. The Melarchez stream exhibits low but variable dissolved 238U levels (3.3 +/- 2.0 mBq l(-1)). Thereafter, uranium activities show a rapid increase to reach, from the Grand Morin River, a rather constant range (8-11 mBq l(-1)). On the Marne before the confluence with the Seine, dissolved 238U is nearly invariable (9.1 +/- 0.8 mBq l(-1)), for flow rates comprised between 60 and 423 m3 s(-1). Dissolved 238U in the Seine corresponds to almost triple the global mean riverine uranium concentration. In the estuary of the Seine, uranium shows a gradual increase, resulting from conservative mixing of river with sea waters.     

Determination of extremely low (236)U/(238)U isotope ratios in environmental samples by sector-field inductively coupled plasma mass spectrometry using high-efficiency sample introduction

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.     

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.     

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.     

Use of HPGe gamma-ray spectrometry to assess the isotopic compositiion of uranium in soils

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.     

Distribution of naturally occurring radionuclides (U, Th) in Timahdit black shale (Morocco)

Attention has been focused recently on the use of Moroccan black oil shale as the raw material for production of a new type of adsorbent and its application to U and Th removal from contaminated wastewaters. The purpose of the present work is to provide a better understanding of the composition and structure of this shale and to determine its natural content in uranium and thorium. A black shale collected from Timahdit (Morocco) was analyzed by powder X-ray diffraction and SEM techniques. It was found that calcite, dolomite, quartz and clays constitute the main composition of the inorganic matrix. Pyrite crystals are also present. A selective leaching procedure, followed by radiochemical purification and alpha-counting, was performed to assess the distribution of naturally occurring radionuclides. Leaching results indicate that 238U, 235U, 234U, 232Th, 230Th and 228Th have multiple modes of occurrence in the shale. U is interpreted to have been concentrated under anaerobic conditions. An integrated isotopic approach showed the preferential mobilization of uranium carried by humic acids to carbonate and apatite phases. Th is partitioned between silicate minerals and pyrite.     

Disequilibrium between uranium and its progeny in the Lake Issyk-Kul system (Kyrgyzstan) under a combined effect of natural and manmade processes

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.     

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.     

Isotopic composition and origin of uranium and plutonium in selected soil samples collected in Kosovo

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).     

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.     

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.     

234U and 238U isotopes in water and sediments of the southern Baltic

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.     

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.     

Distribution of uranium and radium isotopes in an aquifer of a semi-arid region (Manouba-Essijoumi, Northern Tunisia)

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.     

Uranium in sediments, mussels (Mytilus sp.) and seawater of the Krka river estuary

The response of an aquatic environment to the decrease of phosphate discharges from a technologically improved transhipment terminal, situated at the Croatian Adriatic coast in the port of Sibenik, has been assessed based on uranium activity and concentration in sediment, seawater and mussels Mytilus sp. The highest 238U activities (485+/-16Bqkg(-1) dry weight) were found in the sediment sample collected from the sampling site closest to the terminal. The maximum concentrations in the sediment samples are above the natural ranges and clearly indicate the harbour activities' influence. The 238U/226Ra activity ratios in sediment samples demonstrate the decreasing trend of phosphate ore input. Mussel samples showed levels of 238U activities in the range from 12.1+/-2.9 to 19.4+/-7.2 Bqkg(-1) dry weight, thus being slightly higher than in normally consumed mussels. Only the seawater, taken just above the bottom sediment at the sampling site closest to the terminal, shows a slightly higher uranium concentration (3.1+/-0.2 microgL(-1)) when compared to the samples taken in upper seawater layers (2.1+/-0.2 microgL(-1)) but is in the range of the concentration level of uranium in natural seawater. Since the transhipment terminal in the port of Sibenik was modernised in 1988, discharge of phosphate ore into the seawater was drastically reduced and, consequently, uranium concentration levels in seawater have decreased. However, enhanced uranium activity levels are still found in deeper sediment layer samples and in mussel.     

Uranium series isotopes in the Avon Valley, Nova Scotia

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.     

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.     

Concentration and characteristics of depleted uranium in biological and water samples collected in Bosnia and Herzegovina

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.     

Specific activity and hazards of granite samples collected from the Eastern Desert of Egypt

Fifty granitic rock samples were collected from different plutons in the central part of the Eastern Desert of Egypt and were analyzed for specific concentrations of (238)U, (232)Th and (40)K radionuclei. The measurements were carried out using a high performance and stability Nomad Plus spectroscopy system attached to a 1.7 keV (FWHM) HPGe detector. The spectra were analyzed using the direct gamma counting comparison method as well as the traditional absolute efficiency curve method. The highest average value of (238)U concentration (1184 Bq kg(-1)) was observed at EI Misikat region whereas the highest average values of (40)K and (232)Th concentration (2301.8 and 162.5 Bq kg(-1) respectively), were detected at Gabal Homret Waggat area. The radium equivalent activity (Ra(eq)), the absorbed dose rate (D), the external hazard index (H(ex)) and the annual gonadal dose equivalent were also calculated and compared to the international recommended values. Radon exhalation rate from the rock samples were measured using the activated charcoal canister method. The average value of radon exhalation varies from 0.052 to 0.69 Bq m(-2) h(-1) and depends on the specific concentration of uranium.     

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.