The concept of the use of recycled uranium for increasing the degree of security of export deliveries of fuel for light-water reactors

The present paper deals with investigation of the possibilities for reducing the risk of proliferation of fissionable materials by means of increasing the degree of protection of fresh fuel intended for light-water reactors against unsanctioned use in the case of withdrawal of a recipient country of deliveries from IAEA safeguards. It is shown that the use of recycled uranium for manufacturing export nuclear fuel makes transfer of nuclear material removed from the fuel assemblies for weapons purposes difficult because of the presence of isotope ²³²U, whose content increases when one attempts to enrich uranium extracted from fresh fuel. In combination with restricted access to technologies for isotope separation by means of establishing international centers for uranium enrichment, this technical measure can significantly reduce the risk of proliferation associated with export deliveries of fuel made of low-enriched uranium. The assessment of a maximum level of contamination of nuclear material being transferred by isotope ²³²U for the given isotope composition of the initial fuel is obtained. The concept of further investigations of the degree of security of export deliveries of fuel assemblies with recycled uranium intended for light-water reactors is suggested.     

Analysis of the Effect of Restrictions on Isotopes 232,234,236U in Marketable LEU on the Choice of Methods for Enriching Reprocessed Uranium in Cascades of Centrifuges

Physics of Atomic Nuclei - The study addresses the problems of reprocessed uranium re-enrichment. It is shown that, in the most general formulation, the problem of reprocessed uranium re-enrichment...     

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.      

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.      

Physical Aspects of the Waste of Re-Enrichment Utilization for Recycled Uranium from VVER-1000/1200 Spent Fuel Reprocessing in Molten Salt Reactors

Physics of Atomic Nuclei - The problems of utilization of waste from re-enrichment of regenerated uranium from 232U isotope in a reactor with circulating liquid fuel based on melts of metal...     

Isotope shift and hyperfine structure of the highly excited atomic uranium

The laser induced fluorescence method using atomic beam combined with Doppler-free two-photon absorption technique was applied for the measurement of isotope shifts and hyperfine structures of atomic uranium including ²³⁴U, ²³⁵U, ²³⁶U and ²³⁸U isotopes. The isotope shifts between ²³⁸U-²³⁴U, ²³⁸U-²³⁵U, ²³⁸U-²³⁶U, and the hyperfine structure of ²³⁵U were obtained in the high lying odd levels around 4 eV. Received 3 December 2001 / Received in final form 4 July 2002 Published online 29 October 2002 RID="a" ID="a"e-mail: oba@analchem.tokai.jaeri.go.jp     

Experimental study of uranium isotope fractionation of rock material from two aquifers

This paper presents results of a study carried out in order to estimate the uranium isotope fractionation ²³⁴U/²³⁸U in groundwater from laboratory experiments. Matrix rock from borcholes in a Triassic sandstone aquifer and a Pleistocene sand aquifer was leached with 1 N HCl, 0.1 N HCl and deionized water.

Additionally, the uranium isotope composition of the bulk rock (index “R”) and several groundwater samples of corresponding horizons were analysed. The results indicate the relation between the portion of leached uranium (index “L”) and the observed activity ratio ²³⁴U/²³⁸U (AU)

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If this relation can be confirmed by further investigations new possibilities of using uranium isotopes in hydrogeology would be made available

Die Arbeit stellt Ergebnisse einer Studie vor, die zur Abschützung der Uranium-Isotopenfraktionierung ²³⁴U/²³⁸U im Grundwasser aus Laborexperimenten durchgeführt wurde. Matrixgestein von Bohrlöchern in einem Triassischen Sandstein-Grundwasserleiter und einem aus pleislozänen Sanden bestehenden Grundwasserleiter wurde mit 1 N HCl, 0,1 HCl und entionisiertem Wasser gelaugt. Auβerdem wurden die Uranium-Isotopenzusammensetzung des Gesteins (Index “R”) und einige Grundwasserproben zugehöriger Horizonte analysiert. Die Ergebnisse zeigen cine Beziehung zwischen dem Anteil des gelaugten Uraniums (Index “L”) und dem Aktivitätsverhältnis ²³⁴U/²³⁸U (AU)

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Wenn diese Relation durch weitere Untersuchungen bestäligt werden kann, eröffnen sich neue Möglichtkeiten für die Nutzung der Uraniumisotope in der Hydrogeologie.     

Fast determination of uranium and radium in waters of variable composition

The effects of uranium and its progeny radium are known to be harmful and their measurements in drinking water are necessary for careful monitoring. Fast and accurate methods for determination of uranium and radium in water samples with various salinity and activities concentrations have been developed. High Resolution Inductively Coupled Plasma Mass Spectrometry is used for direct measurement of uranium. Calibration is performed with ²³⁸U standards and ²⁰⁹Bi is used as internal standard to correct the matrix effects and plasma instability. The radium is determined by photon electron rejected alpha liquid spectrometry after a chemical separation procedure that includes co-precipitation of radium with barium sulphate, transformation of the sulphate to carbonate and extraction of radium in the scintillation cocktail. The minimal detectable activities of 3.5×10⁻⁸ Bq kg⁻¹ for uranium and 2.3×10⁻⁴ Bq kg⁻¹ for radium are obtained.     

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.     

On the role of fusion neutron source with thorium blanket in forming the nuclide composition of the nuclear fuel cycle of the Russian Federation

The possible role of available thorium resources of the Russian Federation in utilization of thorium in the closed (U–Pu)-fuel cycle of nuclear power is considered. The efficiency of application of fusion neutron sources with thorium blanket for economical use of available thorium resources is demonstrated. The objective of this study is the search for a solution of such major tasks of nuclear power as reduction of the amount of front-end operations in the nuclear fuel cycle and enhancement of its protection against uncontrolled proliferation of fissile materials with the smallest possible alterations in the fuel cycle. The earlier results are analyzed, new information on the amount of thorium resources of the Russian Federation is used, and additional estimates are made. The following basic results obtained on the basis of the assumption of involving fusion reactors with Th-blanket in future nuclear power for generation of the light uranium fraction ^232+233+234U and ²³¹Pa are formulated. (1) The fuel cycle would shift from fissile ²³⁵U to ²³³U, which is more attractive for thermal power reactors. (2) The light uranium fraction is the most “protected” in the uranium fuel component, and being mixed with regenerated uranium, it would become reduced-enrichment uranium fuel, which would relieve the problem of nonproliferation of the fissile material. (3) The addition of ²³¹Pa into the fuel would stabilize its neutron-multiplying properties, thus making it possible to implement a long fuel residence time and, as a consequence, increase the export potential of the whole nuclear power technology. (4) The available thorium resource in the vicinity of Krasnoufimsk is sufficient for operation of the large-scale nuclear power industry of the Russian Federation with an electric power of 70 GW for more than one quarter of a century. The general conclusion is that involvement of a small number of fusion reactors with Th-blanket in the future nuclear power industry of the Russian Federation would to a large extent solve its problems and increase its export potential.     

贫铀球壳中D-T中子诱发的铀反应率的测量与分析

为校验次临界能源堆的概念设计,在R19.4/30.0 cm的贫铀球壳装置上采用活化法开展14 MeV中子学积分实验.布放6片贫铀活化片于球壳中与入射D离子束90°方向上的不同位置处活化,用HPGe探测器测量238U(n,γ)反应、238U(n,f)及235U(n,f)反应和238U(n,2n)各反应产物发射的特征γ射线,得到了相应的反应率.238U(n,γ)反应率的不确定度为3.6％-3.7％,238U(n,D和235U(n,f)反应率的不确定度为5.1％-5.9％,238U(n,2n)反应率的不确定为4.3％-4.7％.用MCNP5程序在ENDF66c数据库下进行模拟计算,238U(n,γ)反应率的计算值/实验值(C/E)为0.972-1.034,238U(n,f)和235U(n,f)反应率的C/E为0.983-1.058,238U(n,2n)反应率的C/E为0.979-1.019.     

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.     

Breeding of 233U in the thorium–uranium fuel cycle in VVER reactors using heavy water

A method is proposed for achieving optimal neutron kinetics and efficient isotope transmutation in the ²³³U–²³²Th oxide fuel of water-moderated reactors with variable water composition (D₂O, H₂O) that ensures breeding of the ²³³U and ²³⁵U isotopes. The method is comparatively simple to implement.     

Production of nuclear polarization of unstable nuclei via polarization transfer reactions

To determine experimental conditions suitable for isotope analysis, we studied the plume dynamics of uranium. A uranium oxide sample was ablated by 2nd harmonic radiation from a Nd:YAG laser at a fluence of 0.5 J/cm². The temporal evolution of the ablation plume was investigated in 800 Pa helium environment. It was found that the observation at 3–5 μs after the ablation at the height of about 2.5 mm are most suited for obtaining higher sensitivity. Using the established conditions, we obtained the limit of detection of the isotope ratio (²³⁵U/²³⁸U) to be 0.01 %. In addition, the limit of detection of elemental abundance of uranium in uranium glass was also evaluated.     

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.     

Accelerated alpha-decay of uranium isotopes induced by exposure of aqueous solution of uranium salt with gold nanoparticles to laser radiation

Laser-induced accelerated alpha-decay of ²³²U nuclei under laser exposure of Au nanoparticles in aqueous solutions of uranium salt has been experimentally studied. It is demonstrated that the decrease in the alpha-activity depends strongly on the peak intensity of laser radiation in the liquid and reaches a maximum at 10¹²–10¹³Wcm^?2. The decrease in the alpha-activity of the exposed solutions is accompanied by deviation of gamma-activities of daughter nuclides of ²³²U from their equilibrium values. Experimental data on the accelerated alpha-decay of ²³⁸U under similar experimental conditions are also presented. Possible mechanisms of laser effect on the alpha-activity are discussed in terms of the amplification of the electric field of laser wave on metallic nanoparticles.     

Trace determination of uranium preconcentrated using graphene oxide by total reflection X-ray fluorescence spectrometry

A new method based on dispersive microsolid phase extraction using graphene oxide (GO) as a solid adsorbent and total reflection X-ray fluorescence (TXRF) spectrometry is proposed for trace determination of uranium. In the developed methodology, a suspension of GO was injected into uranium-spiked multielement solutions including rubidium; after filtration, the membrane filter with collected GO was placed in a small volume of internal standard acid solution and the eluent containing uranium was deposited onto a fluorine resin-coated slide glass, which is a disposable sample stage. Using GO was effective for removal of rubidium from the measurement solution to avoid interference between Rb Kα peak and U Lα peak. The high enrichment factor of 150 enables obtaining uranium detection limits of 0.042, 0.087, and 0.12 μg L⁻¹ for ionic strength of 0.01, 0.1, and 1 mol L⁻¹, respectively. Such low detection limits were obtained by using a benchtop TXRF spectrometer with 5-min measurement. The proposed method is suitable for trace uranium determination in water, including high salinity samples.     

On the equilibrium isotopic composition of the thorium–uranium–plutonium fuel cycle

The equilibrium isotopic compositions and the times to equilibrium in the process of thorium–uranium–plutonium oxide fuel recycling in VVER-type reactors using heavy water mixed with light water are estimated. It is demonstrated thEhfat such reactors have a capacity to operate with self-reproduction of active isotopes in the equilibrium mode.     

Radiation dose-dependent risk on individuals due to ingestion of uranium and radon concentration in drinking water samples of four districts of Haryana,India

Uranium gets into drinking water when the minerals containing uranium are dissolved in groundwater. Uranium and radon concentrations have been measured in drinking water samples from different water sources such as hand pumps, tube wells and bore wells at different depths from various locations of four districts (Jind, Rohtak, Panipat and Sonipat) of Haryana, India, using the LED flourimetry technique and RAD7, electronic silicon solid state detector. The uranium (²³⁸U) and radon (²²²Rn) concentrations in water samples have been found to vary from 1.07 to 40.25?µg?L^?1 with an average of 17.91?µg?L^?1 and 16.06?±?0.97 to 57.35?±?1.28?Bq?L^?1 with an average of 32.98?±?2.45?Bq?L^?1, respectively. The observed value of radon concentration in 43 samples exceeded the recommended limits of 11?Bq?L^?1 (USEPA) and all the values are within the European Commission recommended limit of 100?Bq?L^?1. The average value of uranium concentration is observed to be within the safe limit recommended by World Health Organization (WHO) and Atomic Energy Regulatory Board. The annual effective dose has also been measured in all the water samples and is found to be below the prescribed dose limit of 100?µSv?y^?1 recommended by WHO. Risk assessment of uranium in water is also calculated using life time cancer risk, life time average daily dose and hazard quotient. The high uranium concentration observed in certain areas is due to interaction of ground water with the soil formation of this region and the local subsurface geology of the region.     

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.