Study of the partitioning of uranium and thorium in Moroccan black shale

Moroccan black shale was analysed for uranium and thorium isotopes using alpha-spectrometry. A sequential leaching procedure was used to define the speciation of isotopes of the actinides in the material. As in most other organic rich rocks, uranium is highly enriched in the black shale. This actinide is associated predominantly with humic acids. Thorium (²³²Th) is a less mobile radionuclide in this environment as was expected from its chemical properties, and in agreement with the most widely adopted views in the published literature. It is partitioned between silicate minerals, pyrite and kerogen.     

Radioactivity in waters of Mt. Etna (Italy)

Radioactivity in underground waters from Mt. Etna was investigated on the basis of 13 samples. The samples were collected from springs, wells and galleries around the volcano. Water from nine out of thirteen intakes is used for consumption. Activity concentration of uranium isotopes ^234,238U, radium isotopes ^226,228Ra and radon ²²²Rn were determined with the use different nuclear spectrometry techniques. The measurements of radium and radon activity concentration were performed with the use of a liquid scintillation counter. The determination of uranium isotopes was carried out with the use of alpha spectrometry. All samples show uranium concentration above Minimum Detectable Activity (MDA), with the highest total uranium (²³⁴U + ²³⁸U) activity concentration equal to 130 mBq/l. For radium isotopes, all samples except one showed the activity concentration below MDA. Radon activity concentration was within the range from 1 to 13 Bq/l, hence these waters can be classified as low-radon waters.     

Nuclear pears: Recent developments and future prospects

We report studies of examples of reflection-asymmetric nuclei which are difficult to access using compound nucleus reactions. The octupole radium isotopes withN>132 and radon isotopes are not accessible by reactions employing stable targets and beams; we have shown that multinucleon transfer reactions can populate these nuclei with sufficient yield for their structure to be determined. We report high-spin studies in^{218, 220, 222}Rn and^{222, 224, 226, 228, 230}Ra: these show that the Ra isotopes withA<228 have the characteristics of octupole deformed nuclei whereas the Rn isotopes behave like octupole vibrators. Measurements of theB(E1)/B(E2) ratios indicate that the electric dipole moment in these nuclei is constant with spin. The most octupole deformed nuclei are predicted to be uranium isotopes withN≈132; measurements of the very fissile nucleus²²⁶U suggest that it is octupole deformed and has a large intrinsic electric dipole moment. Finally, we speculate that the best examples of pear shapes are the hyperdeformed minima predicted to lie low in uranium isotopes withN≈140; their signature of high-multiplicity low-energyE1 photon cascades should be detectable using present-day high-efficiency germanium arrays.     

Evolution of isotopic composition of reprocessed uranium during the multiple recycling in light water reactors with natural uranium feed

A complex approach based on the consistent modeling of neutron-physics processes and processes of cascade separation of isotopes is applied for analyzing physical problems of the multiple usage of reprocessed uranium in the fuel cycle of light water reactors. A number of scenarios of multiple recycling of reprocessed uranium in light water reactors are considered. In the process, an excess absorption of neutrons by the ²³⁶U isotope is compensated by re-enrichment in the ²³⁵U isotope. Specific consumptions of natural uranium for re-enrichment of the reprocessed uranium depending on the content of the ²³²U isotope are obtained.     

Production of Cs and Fr isotopes from a high-density UC targets with different grain dimensions

A UC target material of 11.3±0.5 g/cm^3 uranium density with the grain size of 20 and 5μm manufactured in a form of pills by the method of powder metallurgy has been tested on-line within the temperature range of 1800-2100 ^° C . The mass of uranium exposed to the beam was 4-7g. The yields and release rates of Cs and Fr isotopes produced by fission and spallation reactions of ²³⁸U by 1GeV protons have been measured. The yields of Cs and Fr isotopes obtained from the tested target materials have been compared, including yields of very short-lived Fr isotopes with half-lives down to 1ms. Temperature-resistant materials (porous graphite and tantalum foil) have been used for the internal-container construction, which holds the UC target pills inside a tungsten external container heated by the resistant heating. The fastest release and the highest efficiency for short-lived isotopes have been obtained for the targets with the internal container manufactured from the tantalum foil. Results of on-line tests of a big mass target (730g of 5μm grain UC target material) have been discussed.     

Fission decay properties of ultra neutron-rich uranium isotopes

The fission decay of highly neutron-rich uranium isotopes is investigated which shows interesting new features in the barrier properties and neutron emission characteristics in the fission process. ²³³U and ²³⁵U are the nuclei in the actinide region in the beta stability valley which are thermally fissile and have been mainly used in reactors for power generation. The possibility of occurrence of thermally fissile members in the chain of neutron-rich uranium isotopes is examined here. The neutron number N = 162 or 164 has been predicted to be magic in numerous theoretical studies carried out over the years. The series of uranium isotopes around it with N = 154–172 are identified to be thermally fissile on the basis of the fission barrier and neutron separation energy systematics; a manifestation of the close shell nature of N = 162 (or 164). We consider here the thermal neutron fission of a typical representative ²⁴⁹U nucleus in the highly neutron-rich region. Semiempirical study of fission barrier height and width shows that ²⁵⁰U nucleus is stable against spontaneous fission due to increase in barrier width arising out of excess neutrons. On the basis of the calculation of the probability of fragment mass yields and the microscopic study in relativistic mean field theory, this nucleus is shown to undergo exotic decay mode of thermal neutron fission (multi-fragmentation fission) whereby a number of prompt scission neutrons are expected to be simultaneously released along with the two heavy fission fragments. Such properties will have important implications in stellar evolution involving r-process nucleosynthesis.      

On-line production of Rb and Cs isotopes from uranium carbide targets

A series of on-line mass separation experiments have been performed at the IRIS facility to measure the yield and release of Rb and Cs neutron-rich isotopes produced by fission reaction of ²³⁸U. A 1 GeV proton beam was used to bombard uranium carbide targets with the densities of 11 g/cm³ and 1.5 g/cm³ held at temperatures in the range (2000-2230) ^°C. The release curves of Rb and Cs long-lived isotopes were measured from both kinds of targets. The overall production efficiency was determined making use of experimentally measured cross-sections of that isotope production. Comparison of the experimental yields of Rb and Cs isotopes with the calculated ones after corrections for losses due to finite release times suggests that the diffusion is the dominating process reducing the efficiency for short-lived isotopes. When normalized to the same thickness, an enhancement for the high-density rod target of the measured isotope yields is observed when going far from stability. This is possibly explained by the reactions induced by secondary neutrons. A significant odd-even effect with higher yields of Cs even neutron isotopes has been observed, confirming a similar effect obtained in earlier experiments.     

14C in uranium and thorium minerals: a signature of cluster radioactivity?

Various uranium and thorium minerals have been analysed with accelerator mass spectrometry to determine their ¹⁴C content. It is found that, whenever the contribution from secondary reactions such as the ¹¹B(α,p)¹⁴C is sufficiently low, the ¹⁴C concentration is consistent with that expected from ¹⁴C (spontaneous) cluster radioactivity from radium isotopes of the uranium and thorium natural series. Received: 15 February 1999     

Oscillatory extraction — New method of similar elements and isotopes separation

The new separation extraction method was created based on oscillatory extraction/stripping process in two extractors coupled by bulk liquid membrane (LM). The experimental setup to investigate the kinetics of non-stationary processes was built in Saint Petersburg State Institute of Technology in the Rare Earth Department. To induce the oscillatory extraction-stripping process the cyclic Belousov-Zhabotinsky (BZ) reaction or cyclic electrochemical oxidation-reduction was used. The possibility to use oscillatory extraction approach to separate similar elements by using the differences in their kinetic properties is demonstrated. The experimental evidences of uranium, cerium and neodymium isotopes separation were obtained. The separation of ¹⁴²Ce and ¹⁴⁰Ce isotopes between aqueous phases of two extractors coupled by bulk LM in the experiments with cyclic chemical oxidation/reduction with enrichment factor about 2.5% was observed. Under the same conditions the separation of the Nd isotopes (heavy isotopes of Nd — ¹⁴⁴Nd, ¹⁴⁵Nd, ¹⁴⁶Nd, ¹⁴⁸Nd, and ¹⁵⁰Nd from the light isotope — ¹⁴³Nd) in the same experiment with enrichment factor about 0.7–1.4% was observed.     

Target mass correction on the 3He polarized structure function

The diffusion-effusion model has been used to analyse the release and yields of Fr and Cs isotopes from uranium carbide targets of very different thicknesses (6.3 and 148 g/cm²) bombarded by a 1 GeV proton beam. Release curves of several isotopes of the same element and production efficiency versus decay half-life are well fitted with the same set of parameters. Comparison of efficiencies for neutron-rich and neutron-deficient Cs isotopes enables separation of the contributions from the primary (p + ²³⁸U) and secondary (n + ²³⁸U) reactions to the production of neutron-rich Cs isotopes. A rather simple calculation of the neutron contribution describes these data fairly well. The FLUKA code describes the primary and secondary-reaction contributions to the Cs isotopes production efficiencies for different targets quite well.     

Preliminary results of calculations for heavy-water nuclear-power-plant reactors employing <Superscript>235</Superscript>U, <Superscript>233</Superscript>U,and <Superscript>232</Superscript>Th as a fuel and meeting requirements of a nonproliferation of nuclear weapons

A physical design is developed for a gas-cooled heavy-water nuclear reactor intended for a project of a nuclear power plant. As a fuel, the reactor would employ thorium with a small admixture of enriched uranium that contains not more than 20% of ²³⁵U. It operates in the open-cycle mode involving ²³³U production from thorium and its subsequent burnup. The reactor meets the conditions of a nonproliferation of nuclear weapons: the content of fissionable isotopes in uranium at all stages of the process, including the final one, is below the threshold for constructing an atomic bomb, the amount of product plutonium being extremely small.     

Separation of Isotopes of Lithium and Uranium by Electromigration Using Cation-Exchange Membranes

Isotope separation by chromatographic electromigration has been studied for lithium (⁶Li and ⁷Li) and uranium (²³⁵U and ²³⁸U), using cation-exchange membranes as migration media. The membranes were pulled back against the direction of the movement of isotopic cations in a countercurrent manner. In both cases of the elements the lighter isotope, ⁶Li or ²³⁵U, was concentrated at the frontal part of a migration zone; at the extreme front the ⁶Li atom % increased to 16.8% from the original value of 7.5% after 386 cm migration, and the ²³⁵ U atom % rose to 0.743% from the original value of 0.723% after 200 cm migration. Isotope separation coefficients were experimentally determined: ε = (3.7 ± 0.4) μ 10^?3 for lithium isotopes, and two slightly different values ε = (4.9 ± 1.0) μ 10^?5 and (5.4 ± 1.1) μ 10^?5 for uranium isotopes. The steep isotope accumulation was observed in a narrow boundary region. A mathematical expression for the isotope accumulation curve was derived, and the slope of the curve was assessed for each experimental result.     

Neutron-rich isotope production using the uranium carbide multi-foil SPES target prototype

In the framework of the R&D program for the SPES (Selective Production of Exotic Species) project of the Istituto Nazionale di Fisica Nucleare (INFN), production yields of neutron-rich isotopes have been measured at the Holifield Radioactive Ion Beam Facility (HRIBF, Oak Ridge National Laboratory, USA). This experiment makes use of the multi-foil SPES target prototype composed of 7 uranium carbide discs, with excess of graphite (ratio C/U = 4 . 77 isotopes of medium mass (between 72 and 141amu), produced via proton-induced fission of uranium using a 40MeV proton beam, have been collected and analyzed for the target heated at 2000 ^° C target temperature.     

Hyperfine structure and isotope shift measurements on 235U and laser separation of uranium isotopes by two-step photoionization

Two-step photoionization of an atomic beam and quadrupole mass analysis have been used for the precise measurement of the isotope shift between uranium isotopes 235 and 238 and the hyperfine structure of ²³⁵U. For the 5915 Å ground-state transition 15 hfs components were found. The residual atomic beam was isotopically enriched by factors 2.5 and 10 for ²³⁵U and ²³⁸U, respectively.     

Accelerated alpha decay under laser exposure of metallic nanoparticles in aqueous solutions of uranium salt

The recent experimental results on the acceleration of alpha decay under laser exposure of metallic nanoparticles in aqueous solutions (D₂O or H₂O) of uranium salt UO₂Cl₂ are reviewed. It is demonstrated that the rate of the alpha decay of uranium branching depends on the laser wavelength and laser peak power both under exposure of the solution of uranium salt in colloidal solutions of metallic nanoparticles and under laser ablation of a bulk target in an aqueous solution. Tuning the laser wavelength to the plasmon resonance allows observation of large deviations of the contents of radio-nuclides of ²³⁸U branching from their equilibrium values. The effect of laser exposure is characterized by high isotopic selectivity towards the decay of different nuclides. Possible mechanisms of the laser-induced alpha decay of uranium isotopes and their potential applications are discussed.     

Evolution of vegetation and soil nutrients after uranium mining in Los Ratones mine (Cáceres,Spain)

The evolution of vegetation structure following mine rehabilitation is rather scarce in the literature. The concentration of long-lived radionuclides of the ²³⁸U series might have harmful effects on living organisms. We studied soil properties and the natural vegetation occurring along a gradient in Los Ratones, an area rehabilitated after uranium mining located in Cáceres, Spain. Soil and vegetation were sampled seasonally and physical and chemical properties of soil were analysed, including natural isotopes of ²³⁸U, ²³⁰Th, ²²⁶Ra and ²¹⁰Pb. Species richness, diversity, evenness and plant cover were estimated and correlated in relation to soil physical and chemical variables. The location of the sampling sites along a gradient had a strong explanatory effect on the herbaceous species, as well as the presence of shrubs and trees. Seasonal effects of the four natural isotopes were observed in species richness, species diversity and plant cover; these effects were directly related to the pH values in the soil, this being the soil property that most influences the plant distribution. Vegetation in the studied area resembles that of the surroundings, thus proving that the rehabilitation carried out in Los Ratones mine was successful in terms of understorey cover recovery.     

The origin of Cretaceous black shales: a change in the surface ocean ecosystem and its triggers

Black shale is dark-colored, organic-rich sediment, and there have been many episodes of black shale deposition over the history of the Earth. Black shales are source rocks for petroleum and natural gas, and thus are both geologically and economically important. Here, we review our recent progress in understanding of the surface ocean ecosystem during periods of carbonaceous sediment deposition, and the factors triggering black shale deposition. The stable nitrogen isotopic composition of geoporphyrins (geological derivatives of chlorophylls) strongly suggests that N₂-fixation was a major process for nourishing the photoautotrophs. A symbiotic association between diatoms and cyanobacteria may have been a major primary producer during episodes of black shale deposition. The timing of black shale formation in the Cretaceous is strongly correlated with the emplacement of large igneous provinces such as the Ontong Java Plateau, suggesting that black shale deposition was ultimately induced by massive volcanic events. However, the process that connects these events remains to be solved.     

Measurement of uranium and its isotopes at trace levels in environmental samples using mass spectrometry

Actinides have widely entered the environment as a result of nuclear accidents and atmospheric weapon testing. These radionuclides, especially uranium, are outstanding radioactive pollutants, due to their high radiotoxicity and long half-lives. In addition to this, since depleted uranium (DU) has been used in the Balkan conflict in 1999, there has been a concern about the possible consequences of its use for the people and environment. Therefore, accurate, precise and simple determination methods are necessary in order to evaluate the human dose and the concentration and effects of these nuclides in the environment. The principal isotopes of uranium e.g. ²³⁵U and ²³⁸U are of primordial origin and ²³⁴U present in radioactive equilibrium with ²³⁸U. ²³⁶U occurs in nature at ultra trace concentrations with a ²³⁶U: ²³⁸U atom ratio of 10⁻¹⁴. Concentrations of uranium in soil samples were determined using inductively coupled plasma mass spectrometry (ICP-MS) and isotope ratios of uranium were measured using a thermal ionisation mass spectrometer. Radioactive dis-equilibrium of ²³⁴/²³⁸U, depletion of ²³⁵/²³⁸U and significant evidence of ²³⁶U/²³⁸U were noticed in soil samples.      

Environmental Isotopes as a Useful Tool for Studies at Mixed Uranium Mill Tailings Sites

Abstract

Groundwaters in the area of a mixed landfill (domestic waste above uranium mill tailings) in Dresden (Saxony, Germany) were investigated for their isotope signatures to distinguish between different groundwater types. To determine between the two contamination sources (waste and uranium mill tailings) a multi parameter interpretation was done using both, the main hydrochemical parameters the radionuclides ²³⁴U, ²³⁸U, ²²⁶Ra and ²²²Rn as well as the environmental isotopes of the elements hydrogen, oxygen, sulphur and carbon.

The seepage water from the landfill shows higher δ³⁴S, δ¹⁸O and tritium values as the inflow. The tritium values give an idea about water movement in the dump and mean residence time of the groundwater. The water in the dump shows varying δ¹³C values which indicate different processes occurring in the dump.     

Natural radioactivity levels and associated health hazards from the terrestrial ecosystem in Rosetta branch of the River Nile,Egypt

Twenty soil and 25 sediment samples were collected from the banks and bottom of the River Nile in the surroundings of biggest cities located close to it. Natural radioactivity concentrations of ²²⁶Ra, ²³²Th and ⁴⁰K have been evaluated for all samples by means of γ spectrometric analysis. The radioactivity levels of soil and sediment samples fall within the internationally recommended values. Nevertheless, high natural background radiation zones are detected in the Kafr El-Zayat region due to the presence of a fertilizer factory, and in the Rosetta region due to the presence of black sand deposits. The absorbed dose rate, the γ index and excess life time cancer risk are calculated. High values for some of the radiation health parameters are detected in the Kafr El-Zayat and Rosetta regions representing a serious problem to public health because the soil and sediment are used as constructing material for buildings. Furthermore, the isotope analysis of uranium for representative collected sediment samples via α spectrometry showed average specific activities of 18.7?±?3.6, 0.087?±?0.0038 and 18.6?±?3.8 Bq kg^–1 for ²³⁴U, ²³⁵U and ²³⁸U, respectively. In general, these values confirm the balance in the isotopic abundance of U isotopes.