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Sample records for 239pu actinides combined

  1. Effects of combined exposure of rats to 239PuO2 and whole-body X irradiation. II

    Using F344/N rats, we are studying the biological effects of inhalation exposure to 239PuO2 aerosols combined with whole-body exposure to X rays. Data from this study will provide an improved estimate of the cancer risk from combined exposures in people. A total of 2136 (66%) of the 3232 rats to be entered into this study have been exposed. We have achieved lung burdens of 239Pu and X-ray exposures within the ranges desired. Life shortening has occurred among rats receiving whole-body exposure to X rays, but not among those exposed only to 239PuO2. (author)

  2. Consistent Data Assimilation of Actinide Isotopes: 235U and 239Pu

    In this annual report we illustrate the methodology of the consistent data assimilation that allows to use the information coming from integral experiments for improving the basic nuclear parameters used in cross section evaluation. A series of integral experiments were analyzed using the EMPIRE evaluated files for 235U, 238U, and 239Pu. Inmost cases the results have shown quite large worse results with respect to the corresponding existing evaluations available for ENDF/B-VII. The observed discrepancies between calculated and experimental results were used in conjunction with the computed sensitivity coefficients and covariance matrix for nuclear parameters in a consistent data assimilation. Only the GODIVA and JEZEBEL experimental results were used, in order to exploit information relative to the isotope of interest that are, in this particular case: 235U and 239Pu. The results obtained by the consistent data assimilation indicate that with reasonable modifications (mostly within the initial standard deviation) it is possible to eliminate the original large discrepancies on the Keff of the two critical configurations. However, some residual discrepancy remains for a few fission spectral indices that are, most likely, to be attributed to the detector cross sections.

  3. Effects of combined inhalation exposure of rats to 239PuO2 and beryllium metal

    We exposed rats acutely to achieve one of two initial lung burdens (ILBs) of 239PuO2 alone or in combination with one of three ILBs of beryllium metal. Additional control groups of rats were sham exposed to air. Currently, approximately 58% of all rats planned for inclusion have been exposed. This report describes procedures used for the exposure, maintenance, and evaluation of rats in this study. Most of the animals are to be held for their life span in order to quantitate cancer incidence, with other animals assigned to serial sacrifice groups for quantitation of Pu and Be retention and determination of translocation patterns. Exposure to beryllium at any of the three doses tested retarded clearance of plutonium from the lung by a factor of approximately six. Acute inflammatory responses were studied in a separate group of rats exposed to Be. Except for rats receiving the highest ILB of beryllium metal, no differences between exposed and sham-exposed control groups have yet been noted in terms of mortality, weight changes, and clinical signs. (author)

  4. Effects of combined exposure of F344 rats to inhaled 239PuO2 and a chemical carcinogen (NNK)

    Workers in nuclear weapons facilitates have a significant potential for exposure to chemical carcinogens and to radiation from external sources or from internally deposited radionuclides such as 239Pu. Although the carcinogenic effects of inhaled 239Pu and many chemicals have been studied individually, very little information is available on their combined effects. One chemical carcinogen that workers could be exposed to, via tobacco smoke, is the tobacco-specific nitrosamine 4-(N-Methyl-N-nitrosamino)-1-(3-pyridyl)-1-butanone (NNK), a product of the curing of tobacco and pyrolysis of nicotine in tobacco. NNK causes lung tumors in rats, regardless of the route of administration and to a lesser extent tumors in the liver, nasal passages, and pancreas. The purpose of this study is to characterize the effects of combined exposure of rats to NNK and internally deposited plutonium, as well as to these agents alone

  5. Status of 239Pu evaluations

    This paper summarises the current status of nuclear data evaluations for n+239Pu. The nuclear data we address include fission, capture, scattering cross-sections, as well as the prompt fission neutron energy spectrum, which has large sensitivities to the criticality benchmark testing. The evaluated nuclear data files currently available for 239Pu are compared, and the source of differences in the cross-sections are discussed. Some open questions on the statistical model calculations for deformed systems are also given. (authors)

  6. Quantitative estimation of the combined effect of external γ-radiation and incorporated α-radiation (239Pu) by the biochemical indices of rat immune system

    The combined effect of external γ-radiation (137Cs, 103-26 mC/kg) and incorporated α-radiation (239Pu nitrate, 93-9.3 kBq/kg body mass) was estimated by changes in the nucleic acid metabolism and the number of cells in rat thymus, spleen and bone marrow. The data obtained were processed using a model of multiplicate action of the factors which is equivalent, in the case of low effects, to a traditional model of additive effects. The results of the combined action of the two factors may be estimated by the coefficient of the interaction and the coefficient of the enhancement of the effects

  7. Determination of plutonium isotopes (238Pu, 239Pu, 240Pu, 241Pu) in environmental samples using radiochemical separation combined with radiometric and mass spectrometric measurements

    Xu, Yihong; Qiao, Jixin; Hou, Xiaolin;

    2014-01-01

    This paper reports an analytical method for the determination of plutonium isotopes (238Pu, 239Pu, 240Pu, 241Pu) in environmental samples using anion exchange chromatography in combination with extraction chromatography for chemical separation of Pu. Both radiometric methods (liquid scintillation...... counting and alpha spectrometry) and inductively coupled plasma mass spectrometry (ICP-MS) were applied for the measurement of plutonium isotopes. The decontamination factors for uranium were significantly improved up to 7.5×105 for 20 g soil compared to the level reported in the literature......, this is critical for the measurement of plutonium isotopes using mass spectrometric technique. Although the chemical yield of Pu in the entire procedure is about 55%, the analytical results of IAEA soil 6 and IAEA-367 in this work are in a good agreement with the values reported in the literature or reference...

  8. Transmutation of 239Pu with spallation neutrons

    Incineration studies of plutonium were carried out at the Synchrophasotron of the Joint Institute for Nuclear Research (JINR), Dubna, using proton beams with energies of 0.53 GeV and 1.0 GeV. Solid lead targets (8 cm in diameter and 20 cm long) were surrounded with 6 cm thick paraffin as neutron moderator and then irradiated. The transmutation of 239Pu and the associated production of fission products 91Sr, 92Sr, 97Zr, 99Mo, 103Ru, 105Ru, 129Sb, 132Te, 133I, 135I and 143Ce were studied in the present work. The plutonium samples (each 449 mg) were placed on the outer surface of moderator. For 1.0 GeV proton beam, the fission rate of 239Pu is 0.0032 atoms per proton in one gram plutonium samples, for 0.53 GeV proton this value is 0.0022. The experimental uncertainty is about 15%. The experiments are compared to two theoretical model calculations with moderate success, using the Dubna Cascade Model (CEM) and the LAHET code. The practical incineration rate of 239Pu is very high. For example: if one uses 10 mA, 1 GeV proton beams under the same (fictive) experimental conditions, the incineration rate of 239Pu via fission is 3 mg out of the 449 mg sample per day. For 0.53 GeV protons the corresponding rate is 2 mg per day. (author)

  9. Gamma-ray intensities of 239Pu

    Relative intensities of 239Pu γ-rays were precisely measured with a Ge(Li) detector which was accurately calibrated and corrections were made for self-absorption of γ-rays. Accuracies of 1-2% were obtained for strong γrays. Detector efficiences were calibrated with a standard source of 133Ba and γ-ray sources of 152Eu, 154Eu and 182Ta. Intensities per decay were determined by the measured γ-ray intensities, weight and isotopic abundance of plutonium in the source. (author)

  10. Adsorption behavior of 239Pu by Gaomiaozi bentonite

    Adsorption behavior of 239Pu by Gaomiaozi bentonite as a function of the factors of aqueous phase pH value, 239Pu initial concentration and ionic species is studied by static adsorption experiments in this paper. The following results are obtained. Adsorption equilibrium time of 239Pu by Gaomiaozi bentonite samples is about 24 h, and the adsorption distribution ratio Kd value of 239Pu increases with the pH value, but decreases with increasing initial concentration of 239Pu. And adsorption of 239Pu by bentonite samples with different ionic species show that anions affect the most on adsorption of bentonite is CO32-, followed by HCO3- and SO42-, whereas Cl- and NO3- hardly have any influence on the adsorption of bentonite. (authors)

  11. In vitro dose-response of macrophages to 239PuO2 and 241AmO2

    As part of a study designed to examine various means of solubilizing actinide particles within macrophages, we have measured the in vitro effects of 241AmO2 and 239PuO2 on these cells. Dose distribution within the cell population was estimated by autoradiography and compared to cell detachment as a function of time. The 241AmO2 and 239PuO2 were toxic in proportion to their radioactivity rather than their mass. Approximately 385 intracellular disintegrations are required from either radionuclide to cause cells to detach from the flask surface

  12. Fission of 239Pu with resonance neutrons

    A measurement of fission fragment energy and mass distributions in the 239Pu(n,f) resolved resonance region has been performed applying the twin Frisch-gridded ionization chamber technique. An improved pile-up rejection system has been developed to cope with the strong α background. The results for the mass and mean total kinetic energy (TKE-bar) distributions for resolved resonances do not show any strong 'pattern' of fluctuations, unlike it was the case for 235U(n,f) in the same neutron energy region. This can be explained in the frame of existing theoretical models, according to which the only possible low-energy spin states available (Jπ=0+, 1+) belong to two well separated (∼1.25 MeV) transition state bands with given fission fragment properties. An anti-correlation between TKE-bar and ν-barp was found to be not significant. The obtained small spin dependence of TKE-bar of about 70 keV is in agreement with literature values. A slight correlation was found between TKE-bar versus 1/Γf. But also this was considered not to be significant. (author)

  13. Prompt Fission Neutron Emission in Resonance Fission of 239Pu

    Hambsch, Franz-Josef; Varapai, Natallia; Zeinalov, Shakir; Oberstedt, Stephan; Serot, Olivier

    2005-05-01

    The prompt neutron emission probability from neutron-induced fission in the resonance region is being investigated at the time-of-flight facility GELINA of the IRMM. A double Frisch-gridded ionization chamber is used as a fission-fragment detector. For the data acquisition of both the fission-fragment signals as well as the neutron detector signals the fast digitization technique has been applied. For the neutron detection, large-volume liquid scintillation detectors from the DEMON collaboration are used. A specialized data analysis program taking advantage of the digital filtering technique has been developed to treat the acquired data. Neutron multiplicity investigations for actinides, especially in resonance neutron-induced fission, are rather scarce. They are, however, important for reactor control and safety issues as well as for understanding the basic physics of the fission process. Fission yield measurements on both 235U and 239Pu without prompt neutron emission coincidence have shown that fluctuation of the fission-fragment mass distribution exists from resonance to resonance, larger in the case of 235U. To possibly explain these observations, the question now is whether the prompt neutron multiplicity shows similar fluctuations with resonance energy.

  14. Biosorption of 239Pu by immobilized sargassum fusiforme

    Sargassum fusiforme was immobilized with calcium alginates and its biosorption property to 239Pu was studied by batch and column methods. Biosorption equilibrium time of immobilized Sargassum fusiforme biosorbent to 239Pu is 120 min and biosorption efficiency is over 99.2% when the initial concentration of 239Pu is 21.5 kBq/L and pH is 2.5-5.0. After five times repetition biosorption-desorption cycles biosorption efficiency is still over 98.0% when the velocity of flow is 2 ml/min in column experiment. Immobilized Sargassum fusiforme biosorbent is better to 239Pu due to its better chemical stability, mechanical strength, lower cost, high biosorption efficiency and repeated biosorption-desorption cycles. (authors)

  15. Effects of monomeric 239Pu on the pregnant rabbit

    The effects of 239Pu treatment (0, 10 or 40 μCi/kg) on hematological measurements in pregnant rabbits were studied at 29 days of gestation. Mean clotting times were significantly increased in all plutonium-treated rabbits. There was also a significant increase in clotting time with increasing time between plutonium dosing and sample collection in rabbits injected with 10 μCi/kg. Platelet counts were significantly decreased in all rabbits exposed to 239Pu for 14 days or greater. Hematocrits were significantly depressed in rabbits exposed to 239Pu for 20 days. It is speculated that monomeric 239Pu accumulates at a hematopoietic site close to that affected in X-irradiated animals. (U.K.)

  16. Decreased pulmonary clearance of 239PuO2 and lung toxicity induced by inhaled beryllium metal in rats

    Workers in nuclear industries may be accidentally exposed to both beryllium and plutonium. To characterized the effects of combined exposures to these agents on their pulmonary clearance, groups of F344/N rats inhaled aerosols of beryllium metal and 239PuO2 to result in initial lung burdens for beryllium metal of 0, 50, 150, and 450 μg, and for 239PuO2 of 0, 56, and 170 Bq. Rats were exposed to each possible beryllium/plutonium combination. The whole-body clearance half time of 239Pu in the absence of beryllium metal was approximately 50 days. For rats exposed to both materials, however, 239Pu clearance half-times ranged from 280 to 410 days, with no apparent dose-dependent effect of beryllium metal. Analysis of the lungs for both agents confirmed this pattern of retention. The lungs of beryllium metal-exposed rats displayed a hemorrhagic, exudative pneumonitis, with an influx of neutrophils, and later, progressive fibrosis accompanied by macrophage and epithelial cell hyperplasia. Enhanced 239PuO2 retention will increase the radiation dose to the lung and may result in an eventual synergistic neoplastic response in rats exposed to the two agents

  17. Calculation of 239Pu neutron inelastic cross sections

    We have calculated cross sections for neutron-induced reactions on 239Pu between 0.001 and 5 MeV, with particular emphasis on inelastic scattering. Coupled-channel and Hauser-Feshbach statistical models were used. Within the coupled-channel calculations we employed neutron optical parameters derived from simultaneous fits to total, elastic, inelastic, and resonance data. The resulting transmission coefficients were used in Hauser-Feshbach statistical calculations having a fission channel based on a double-humped barrier representation. Barrier parameters and transition state enhancements needed to reproduce well the (n,f) cross sections between 0.001 and 5 MeV were in general agreement with those from other published analyses. Calculated compound-nucleus and direct-reaction components for inelastic scattering were combined incoherently, and the resultant cross sections agreed well with the Bruyeres-le-Chatel measurements for scattering from levels occupying the ground state rotational band. Our results are in substantial disagreement with ENDF/B-V values for these levels. We are presently performing DWBA calculations to determine direct-reaction components for states occupying higher-lying vibrational bands

  18. Biological effects in intramuscular 239Pu administration during chelatotherapy

    Durable (up to 64 days) application of complexones (Ca and Zn DTPA) in the case of intramuscular administration of 239Pu large amounts in rats is studied. The results of studying the biological effect proving considerable decrease of the average lifespan of rats are given

  19. Strain differences in the embryotoxicity of 239Pu

    Comparison of the embryolethality of monomeric 239Pu injected at 9 days of gestation demonstrated that the sensitivity of Charles River CD strain was greater than that of Hilltop Wistar rats. Subsequent comparisons showed that rats derived from the Hilltop Fischer strain were more sensitive than the Wistar and, although not directly compared, more sensitive than the CD

  20. Preliminary Study on the Determination of ~(235)U and ~(239)Pu Using Delayed Neutron Counting Method

    2011-01-01

    The preliminary study on the fast measurements of 235U and 239Pu in samples containing 235U, 239Pu and 235U-239Pu mixture using delayed neutron counting method is introduced. All samples were irradiated for 30 s using the 30 kW Miniature Neutron

  1. Subcellular binding of 239Pu in the liver of selected species of rodents

    The subcellular distribution of 239Pu in the liver of selected rodent species was investigated as well as the relation between 239Pu and the iron metabolism. The goal of the investigation was to find out why the liver discharge of 239Pu from the liver varies so much between species. (orig.)

  2. Role of protracted exposure on the toxicology of inhaled 239PuO2

    Studies were initiated to examine in rats the effects of a protracted exposure to inhaled 239PuO2. Graphs are presented to show effect of multiple exposures to 239PuO2 on the deposition and clearance of 239Pu in the alveoli

  3. Evaluation of covariances for resolved resonance parameters of 235U, 238U, and 239Pu in JENDL-3.2

    Evaluation of covariances for resolved resonance parameters of 235U, 238U, and 239Pu was carried out. Although a large number of resolved resonances are observed for major actinides, uncertainties in averaged cross sections are more important than those in resonance parameters in reactor calculations. We developed a simple method which derives a covariance matrix for the resolved resonance parameters from uncertainties in the averaged cross sections. The method was adopted to evaluate the covariance data for some important actinides, and the results were compiled in the JENDL-3.2 covariance file. (author)

  4. Surrogate Reaction Measurement of Angular Dependent 239Pu (n , f) Probabilities

    Koglin, Johnathon; Burke, Jason; Casperson, Robert; Jovanovic, Igor

    2015-10-01

    The surrogate method has previously been used to measure (n , f) cross sections of difficult to produce actinide isotopes. These measurements have inaccuracies at excitation energies below 1.5 MeV where the distribution of angular momentum states populated in the compound nucleus created by neutron absorption significantly differs from that arising from direct reactions. A method to measure the fission probability of individual angular momentum states arising from 239Pu (d , pf) and 239Pu (α ,α' f) reactions has been developed. This experimental apparatus consists of charged particle detectors with 40 keV FWHM resolution at 13 angles up and downstream of the particle beam. A segmented array of photovoltaic (solar) cells is used to measure the angular distribution of fission fragments. This distribution uniquely identifies the populated angular momentum states. These are fit to expected distributions to determine the contribution of each state. The charged particle and fission rates matrix obtained from this analysis determines fission probabilities of specific angular momentum states in the transition nucleus. Development of this scheme and first results will be discussed.

  5. Inhaled 239PuO2 in rats with pulmonary emphysema

    The modifying effects of a pre-existing lung disease (emphysema) on the deposition, distribution, retention, and effects of inhaled 239PuO2 in the rat are being investigated. Preliminary observations indicated that the deposition and retention patterns for 239Pu particles inhaled by rats with emphysema and control rats were similar, but the distribution of inhaled 239Pu immediately after exposure was different. Respiratory function measured through one year after exposure to 239Pu was consistent with emphysema and was not altered by the 239Pu lung burden. Long-term observations are continuing. 4 references, 2 tables

  6. Metabolic pathways of 239Pu immediately after administration

    239Pu chloride was given to male rats intravenously or by the oral route. The early stages of the Pu metabolism are characterized by a fast distribution in liver and skeleton and a high concentration in the intestine and the muscle tissue. The rate of elimination from the liver and muscles was the same for both types of application. With injection into different parts of the vascular system, the binding to protein and other tissue components was identical. 239Pu is practically not absorbed from the gastrointestinal tract if given perorally. The absorbed fraction had an osteotropic character, i.e. the plutonium was bound to the organic as well as to the mineral fraction. When Pu chloride is injected intravenously, there is a slow redistribution from the characteristic hepatotropic to the osteotropic type. The function of the liver as a barrier against the plutonium is not very prominent and seems to depend on the type of compound given. (MG/AK)

  7. Neutron Resonance Parameters and Covariance Matrix of 239Pu

    Derrien, Herve [ORNL; Leal, Luiz C [ORNL; Larson, Nancy M [ORNL

    2008-08-01

    In order to obtain the resonance parameters in a single energy range and the corresponding covariance matrix, a reevaluation of 239Pu was performed with the code SAMMY. The most recent experimental data were analyzed or reanalyzed in the energy range thermal to 2.5 keV. The normalization of the fission cross section data was reconsidered by taking into account the most recent measurements of Weston et al. and Wagemans et al. A full resonance parameter covariance matrix was generated. The method used to obtain realistic uncertainties on the average cross section calculated by SAMMY or other processing codes was examined.

  8. Low level 239PuO2 life-span studies

    The purpose of this projet is to determine the dose-response curve for lung-tumor incidence in rats following inhalation of 239PuO2 at levels producing a lifespan radiation dose of 2 to 100 rad. In preliminary studies, rats were intratracheally instilled with, or inhaled 169Yb-239PuO2 or 169Yb-Yb2O3 particles. Whole-body, excreta and tissue levels of 169Yb were determined by external gamma counting; 239Pu levels were determined radiochemically by scintillation counting. It was found that 169Yb dissociated from 239PuO2 and was cleared more rapidly from the lung and the whole body. Despite this fact, however, whole-body counts performed at 7 days after exposure to 169Yb-239PuO2 gave a reproducible measure of the 239Pu lung burden

  9. Characterization of a neutron source of 239PuBe

    The spectrum equivalent dose and environmental equivalent dose f a 239PuBe source have been determined. The appropriate handling of a neutron source depends on the knowledge of its characteristics, such as its energy distribution, total rate of flowing and dosimetric magnitudes. In many facilities have not spectrometer that allows to determine the spectrum and then area monitors are used that give a dosimetric magnitude starting from measuring the flowing rate and the use of conversion factors, however this procedure has many limitations and it is preferable to measure the spectra and starting from this information the interest dosimetric magnitudes are calculated. In this work a Bonner sphere spectrometer has been used with a 6LiI(Eu) scintillator obtaining the count rates that produce, to a distance of 100 cm, a 239PuBe source of 1.85E(11) Bq. The spectrum was reconstructed starting from the count rates using BUNKIUT code and response matrix UTA4. With the spectrum information was calculated the source intensity, total flow, energy average, equivalent dose rate, environmental equivalent dose rate, equivalent dose coefficient and environmental equivalent dose coefficient. By means of two area monitors for neutrons, Eberline ASP-1 and LB 6411 of Berthold the equivalent dose and environmental equivalent dose were measured. The determinate values were compared with those reported in literature and it found that are coincident inside 17%. (Author)

  10. Decommissioning of a 239Pu contaminated incinerator facility

    In early 1978, a plutonium contaminated incinerator facility at the Los Alamos Scientific Laboratory (LASL), Los Alamos, New Mexico, was decommissioned. The project involved dismantling the facility and disposal by burial or by retrievable storage of the debri at an on-site waste disposal area. Contaminated soil from the 0.5 hectare area was buried. The facility was constructed in 1951 to incinerate plutonium contaminated wastes. It was later used as a decontamination facility. The major features included a 185 m2 control building, incinerator, cyclone dust collector, spray cooler, venturi scrubber, air filter bank, ash separator, and two 140,000 litres ash storage tanks. Preliminary soil contamination surveys were performed by a LASL developed portable phoswich detector system. Final soil contamination levels were measured with a zinc sulphide gross alpha scintillation system. Six hundred cubic metres of debris and 1200 m3 of soil contaminated with less than 10 nCi 239 Pu/g were buried at the LASL disposal area. Five cubic metres of 239 Pu contaminated ash residues were packed and stored to meet the Department of Energy's 20 year retrievable storage criteria. (author)

  11. Multilevel analysis of the low energy 239Pu cross sections

    It is well known that the ENDF/B-V representation of the 239Pu resonance region is not satisfactory: below 1 eV the cross sections are given by smooth files (file 3) rather than by resonance parameters. Above 1 eV the single-level formalism used in ENDF/B-V necessitates a structured file 3 contribution. The present paper presents the results of an R-matrix multilevel analysis of several recent data sets as well as of the older data. The analysis is concerned with the region up to 30 eV, an energy region that is important for thermal reactors and for which no recent multilevel analyses had previously been available

  12. R-matrix analyses of the 235U and 239Pu neutron cross sections

    The resonance parameter analysis code SAMMY was used to perform consistent resonance analyses of several 235U and 239Pu fission and capture cross section and transmission measurements up to 110 eV for 235U and up to 1 keV for 239Pu. The method of analysis, the measurement selection and the results are briefly outlined in this paper

  13. Random Probability Analysis of 48Ca +239Pu Experimental Data

    Strauss, S. Y.; Henderson, R. A.; Stoyer, M. A.; Abdullin, A. F. Sh.; Brewer, N. T.; Dmitriev, S. N.; Grzywacz, R. K.; Hamilton, J. H.; Itkis, M. G.; Miernik, K.; Oganessian, Yu. Ts.; Polyakov, A. N.; Roberto, J. B.; Rykaczewski, K. P.; Sabelnikov, A. V.; Sagaidak, R. N.; Shirokovsky, I. V.; Shumeyko, M. V.; Subbotin, V. G.; Sukhov, A. M.; Tsyganov, Yu. S.; Utyonkov, V. K.; Voinov, A. A.; Vostokin, G. K.

    2014-09-01

    Element 114 (Fl), was discovered at the Flerov Laboratory of Nuclear Reactions (FLNR) using the 48Ca +244Pu reaction and the Dubna Gas-Filled Recoil Separator (DGFRS). The structural properties of the super heavy elements are still largely unknown. The extent of the region of enhanced stability near Z = 114 and N = 184 is not completely known. To examine these properties, a new experimental data set has been taken using the 48Ca +239Pu reaction at the DGFRS, in an effort to look for lighter isotopes of Fl. Progress on the production of lighter isotopes of Fl, cross-section measurements, and any nuclear decay properties will be discussed. Comparisons with reactions using heavier 242,244Pu targets and Monte Carlo random probability analysis will be highlighted. Element 114 (Fl), was discovered at the Flerov Laboratory of Nuclear Reactions (FLNR) using the 48Ca +244Pu reaction and the Dubna Gas-Filled Recoil Separator (DGFRS). The structural properties of the super heavy elements are still largely unknown. The extent of the region of enhanced stability near Z = 114 and N = 184 is not completely known. To examine these properties, a new experimental data set has been taken using the 48Ca +239Pu reaction at the DGFRS, in an effort to look for lighter isotopes of Fl. Progress on the production of lighter isotopes of Fl, cross-section measurements, and any nuclear decay properties will be discussed. Comparisons with reactions using heavier 242,244Pu targets and Monte Carlo random probability analysis will be highlighted. This work was performed under Contract DE-AC52-07NA27344 and Grant DE-NA0002135.

  14. Inhaled 239PuO2 in rats with pulmonary emphysema. II

    The modifying effects of pre-existing pulmonary emphysema on deposition, distribution, retention, and effects of inhaled 239PuO2 in the rat were investigated. The presence of emphysema in the rats tested was indicated by respiratory function measurements and confirmed microscopically. Initial lung burdens of 239Pu per kg body weight were less in rats with emphysema than in control rats; however, the retention of 239Pu was similar in emphysematous and control rats. Survival and lung tumor occurrence were similar in emphysematous and control rats exposed to 239PuO2. We concluded that rats with pre-existing pulmonary emphysema were not more sensitive to the effects of inhaled 239PuO2 than control rats. (author)

  15. The removal of inhaled 239Pu from beagle dogs by bronchopulmonary lavage and chelation therapy

    The efficacy of bronchopulmonary lavage and chelatan therapy for removing 239Pu from beagle dogs after inhalation of 239Pu aerosols having different solubilities has been investigated. The four aerosols used were nebulized from a solution of 239PuCl4 and heat treated at temperatures of 325, 600, 900 and 11500C. Groups of six beagle dogs were exposed to each of the aerosols. Subsequently, three dogs in each group were treated by lavage and intravenous injections of DTPA. The remaining three dogs in each group served as untreated controls. It was found that bronchopulmonary lavage treatment was effective in removing nearly half of the 239Pu activity from the lung regardless of the aerosol production temperature. This early removal of 239Pu activity resulted in a significant reduction in daily dose rate and therefore cumulative α dose to lung. The effectiveness of DTPA treatment depended on aerosol production temperature, and was effective in reducing accumulation of 239Pu in liver and skeleton of the dogs that inhaled aerosols produced at 3250 and 6000C by enhancing urinary excretion of 239Pu. (U.K.)

  16. Numerical prediction of 239Pu migration in unsaturated porous media under infiltration scenario

    In terms of the study on site selection of a radioactive waste disposal repository in northwest China, a numerical prediction of 239Pu migration for potential groundwater pollution in the unsaturated zone was conducted with the HYDRUS-1D model. The results showed that the groundwater will not be contaminated by the migration of soluble 239Pu. And there is little possibility that 239Pu migration through groundwater path might have an unacceptable impact on exosphere. Measurements of the distribution coefficient, Kd, are critical in the determination of sorption-induced retardation of radionuclide transport. (authors)

  17. Distribution of 239Pu and 241Am in the human skeleton

    The 241Am and 239Pu distribution in the skeletons of two former nuclear workers has been measured. The skeletons of both individuals appear to be within normal limits for Caucasian men about 50 y old. Both had lower limb bones that were heavier than the age controls and Case I had upper-body bones that were lighter than the age control group. The distribution of americium in the skeleton of Case I, 25 years post exposure, indicated that a more rapid turnover of initially deposited americium on the bone surfaces of cancellous bone, as compared to that deposited on the bone surfaces of compact bone, had occurred. This resulted in a larger proportion of americium located in the compact bone of the extremities and a lesser quantity in the more cancellous bones of the vertebral column, pelvis and rib cage. A similar shift in the distribution of plutonium occurred in Case II in the 35 y since initial deposition, but at a slower rate than that for americium. The ratio of each actinide in the liver to that in the systemic system (liver content/systemic system content) was 0.065 and 0.436, for americium and plutonium, respectively, suggesting that a much more rapid turnover of americium in the liver, compared to plutonium, provided a much larger fraction of that nuclide for circulatory feedback to the remodeling skeletal system. 8 references, 3 tables

  18. Toxicity of 239PuO2 inhaled by aged Beagle dogs. X

    The influence of age at exposure on the metabolism, dosimetry, and biological effects of inhaled 239PuO2 particles is being studied in aged Beagle dogs (8.0-10.5 yr of age at exposure). Forty-eight dogs inhaled 239PuO2 particles with an activity median aerodynamic diameter of 1.5 mm to achieve graded levels of initial pulmonary burdens (IPB) ranging from 0.02-0.66 μCi 239Pu/kg body weight (0.75-24 kBq/kg). Twelve other dogs were exposed to the aerosol diluent only. All forty-eight exposed dogs have died, including two in the past year. The twelve control dogs have also died, including one in the past year. Radiation pneumonitis and pulmonary fibrosis have been the primary causes of death in these aged dogs exposed to 239PuO2. (author)

  19. Malignancy of transplanted hamster lung lesions induced by inhaled 239PuO2

    Selected sites from the lungs of hamsters that had inhaled 239PuO2 aerosol were serially transplanted into the cheek pouches of recipient hamsters. Up to 13 mo postexposure, no evidence of malignancy has appeared

  20. Low-level inhaled-239PuO2 life-span studies in rats

    This study determined the dose-response curve for lung tumor incidence in rats after inhalation of high-fired 239PuO2, which gave radiation doses to the lung of from ∼5 to >1000 rads. Exposed rats were given a single, nose-only, inhalation exposure to 169Yb-239PuO2 aerosol (AMAD, 1.6 +- 0.11 μm). The effective half-time for 169Yb in the lung was 14 days, whereas ∼76% of 239Pu was cleared with a half-time of 20 days and 24%, with a half-time of 180 days. Whole-body counting for 169Yb at 14 days after exposure was an accurate method for determining 239Pu IAD in individual rats, even at IAD's as low as 0.60 nCi of 239Pu. The 239Pu lung-clearance curve and an equation describing changes in lung weight with body weight and age were used to determine lung radiation doses. The IAD's of exposure groups were 0.60 +- 0.15 nCi of 239Pu (1000 rats), 0.98 +- 0.25 (531 rats), 2.4 +- 0.69 (209 rats), 5.7 +- 1.2 (98 rats), and 7.5 +- 2.0 to 150 +- 37 nCi (300 rats); corresponding radiation doses to the lung estimated at 3 years after exposure were 8.3, 14, 33, 79, and 100 to 2100 rads, respectively. 71 refs., 5 figs., 4 tabs

  1. Repeated inhalation exposure of rats to aerosols of 239PuO2. V

    The biological responses following protracted alpha irradiation of rat lungs are being studied. Groups of rats have been exposed once, or repeatedly, to aerosols of 239PuO2 to achieve, or to re-establish, lung burdens of 239Pu that will result in projected lifetime alpha-radiation doses to the lungs of 20, 60, 200, or 600 rad. There were dose related increases in the incidence of primary lung tumors In the rats exposed once or repeatedly to 239PuO2. Repeated inhalation exposure of rats to 239PuO2 did not increase the incidence of lung tumors, their time of occurrence nor the risk of death with a lung tumor per unit of absorbed alpha dose to the lung compared to doses received following single exposures. These findings are consistent with those in Beagle dogs repeatedly exposed to 239PuO2 in other studies, but are not consistent with previous observations In mice. The findings in mice indicated protraction of the alpha dose to the lung by repeated inhalation exposure was more carcinogenic than similar doses after a single inhalation exposure. (author)

  2. Migration of 239Pu in soluble and insoluble forms in soil

    A field experiment study was performed at the rural site of South-East Lithuania. The main tasks of the study included an evaluation of the peculiarities of partition of 239Pu in soluble (239Pu(NO3)4, 239PuCl3) and insoluble (239PuO2) forms in soddy and forest soil horizons. The results of durable experiments (418 and 326 days) have shown that from 44.1% to 92.2% of 239Pu of investigated chemical forms were accumulated in the top (0-5 cm) soil layer. Some share (5.7-39.2%) of plutonium from studied chemical forms was found in the 5-20 cm layers of studied soil samples (columns). Obtained distribution of plutonium in soil layers may be attributed to the consideration that the migration rate to the soil depth for plutonium is 0.1-1.0 cm x y-1 but for some part of plutonium 10 times higher migration rate is characteristic as well. Plutonium transfer factor (TF) to the grassland plants was calculated, the values ranged from 10-2 to 10-1. (author)

  3. Sensitivities of five alpha continuous air monitors for detection of airborne {sup 239}Pu

    McIsaac, C.V.; Amaro, C.R.

    1992-07-01

    Results of measurements of the sensitivities of five alpha continuous air monitors (CAMs) for detection of airborne {sup 239}Pu are presented. Four commercially available alpha CAMs (Kurz model 8311, Merlin Gerin Edgar, RADeCO model 452, and Victoreen model 758) and a prototype alpha CAM currently in use at Argonne National Laboratory- West (ANL-W) were tested sampling natural ambient air and laboratory-generated atmospheres laden with either blank dust or dust containing nCi/g concentrations of {sup 239}Pu. Cumulative alpha spectra were stored at 30 or 60 minute intervals during each sampling and were subsequently analyzed using three different commonly used alpha spectrum analysis algorithms. The effect of airborne dust concentration and sample filter porosity on detector resolution and sensitivity for airborne {sup 239}Pu are described.

  4. Sensitivities of five alpha continuous air monitors for detection of airborne sup 239 Pu

    McIsaac, C.V.; Amaro, C.R.

    1992-07-01

    Results of measurements of the sensitivities of five alpha continuous air monitors (CAMs) for detection of airborne {sup 239}Pu are presented. Four commercially available alpha CAMs (Kurz model 8311, Merlin Gerin Edgar, RADeCO model 452, and Victoreen model 758) and a prototype alpha CAM currently in use at Argonne National Laboratory- West (ANL-W) were tested sampling natural ambient air and laboratory-generated atmospheres laden with either blank dust or dust containing nCi/g concentrations of {sup 239}Pu. Cumulative alpha spectra were stored at 30 or 60 minute intervals during each sampling and were subsequently analyzed using three different commonly used alpha spectrum analysis algorithms. The effect of airborne dust concentration and sample filter porosity on detector resolution and sensitivity for airborne {sup 239}Pu are described.

  5. Sensitivities of five alpha continuous air monitors for detection of airborne 239Pu

    Results of measurements of the sensitivities of five alpha continuous air monitors (CAMs) for detection of airborne 239Pu are presented. Four commercially available alpha CAMs (Kurz model 8311, Merlin Gerin Edgar, RADeCO model 452, and Victoreen model 758) and a prototype alpha CAM currently in use at Argonne National Laboratory- West (ANL-W) were tested sampling natural ambient air and laboratory-generated atmospheres laden with either blank dust or dust containing nCi/g concentrations of 239Pu. Cumulative alpha spectra were stored at 30 or 60 minute intervals during each sampling and were subsequently analyzed using three different commonly used alpha spectrum analysis algorithms. The effect of airborne dust concentration and sample filter porosity on detector resolution and sensitivity for airborne 239Pu are described

  6. Biochemical effects of inhaled 239PuO2 on lung lipids

    Results of experiments carried out to assess the effect of 239Pu α irradiation on lung lipid biosynthesis and to determine the lungs ability to incorporate palmitate into lavage lecithin and its turnover are reported. The experiments were carried out on rats which had inhaled 239PuO2 particles. The study of palmitate incorporation into lipids shows conclusively that for medium (23 to 42 nCi) or high (more than 100 nCi) lung depositions the incorporation by isolated mitochondria is significantly (P 239PuO2 were positive, with respect to controls in 8 of 10 instances, when measured following the label of palmitate in lung lavage lecithin. The interpretation of the significant result (P < 0.05) is that: (1) initial and/or final lecithin pool sizes were different, (2) transfer rates were affected between blood and lung, or (3) rates of degradation of lung lavage lecithin were affected. (U.K.)

  7. Covariances for 239Pu induced cross section in the resonance range using the CONRAD code

    This paper will present the evaluation of neutron induced cross sections covariances for the 239Pu in the resonance range. The methodology used is based on marginalization and retroactive technique to allow the treatment of experimental systematic uncertainties such as normalization. In addition, as sensitivity studies performed on iso-thermal temperature moderator analysis have demonstrated the need for improving the description of the 239Pu neutron cross sections in the sub-thermal energy range and knowing the poor accuracy of the EXFOR data below the thermal energy range, integral trends have to be taken into account in this evaluation work. The focus of the presentation is to show results obtained on the 239Pu capture and fission neutron cross sections in the resonance range with an exhaustive integral validation. (authors)

  8. Medical Care for Accidental Deposition of Plutonium (239Pu) Within the Body

    With expanding uses of plutonium chances for accidental deposition within the body are increasing. Metabolism of plutonium within the body is variable, depending on chemical composition, particle size and shape, monomeric or polymeric physical state, route of entry (inhalation,or through wounds) and many other factors. A notable exception is the negligible absorption from the gastrointestinal tract. It is difficult to determine lung deposition of poorly soluble plutonium by either bioassay or in vivo counting. The intravenous administration of the chelating agent tri-sodium calcium salt of diethylenetriamine- pentaacetic acid (DTPA), soon after an accident, is quite effective in removing soluble plutonium which has been inhaled or deposited in wounds. Conditions requiring prolonged therapy are described. Effectiveness of treatment of 239Pu body depositions is greatly influenced by the solubility of the plutonium at the site of deposition. Size, frequency and duration of dose of DTPA is recommended. Mice developed fibrosarcomas following subcutaneous injections of 0.064 μCi of 239Pu, while an employee apparently developed a pre-cancerous condition after subcutaneous deposition of only 0.005 μCi. It is our policy to recommend excision of any measurable quantity of 239Pu in a superficial wound when this may be accomplished with little hazard. The maximum permissible deposition in skin or subcutaneous tissue may be much lower than that for depositions in bone liver, lung or tracheo-bronchial lymph nodes. No limiting value has been set for depositions in wounds by any official body; The surgeon must balance the benefits to be secured against the risk of the operation. A wound bearing 239Pu should be immediately washed with DTPA, normal saline, or water, in that order of preference. Methods of removal of 239Pu from the intact skin are briefly discussed. A U.S. Plutonium Registry will assist in evaluating depositions of 239Pu and effectiveness of therapy by reconciling

  9. Exploratory study of fission product yields of neutron-induced fission of 235U , 238U , and 239Pu at 8.9 MeV

    Bhatia, C.; Fallin, B. F.; Gooden, M. E.; Howell, C. R.; Kelley, J. H.; Tornow, W.; Arnold, C. W.; Bond, E.; Bredeweg, T. A.; Fowler, M. M.; Moody, W.; Rundberg, R. S.; Rusev, G. Y.; Vieira, D. J.; Wilhelmy, J. B.; Becker, J. A.; Macri, R.; Ryan, C.; Sheets, S. A.; Stoyer, M. A.; Tonchev, A. P.

    2015-06-01

    Using dual-fission chambers each loaded with a thick (200 -400 -mg /c m2) actinide target of 235 ,238U or 239Pu and two thin (˜10 -100 -μ g /c m2) reference foils of the same actinide, the cumulative yields of fission products ranging from 92Sr to 147Nd have been measured at En= 8.9 MeV . The 2H(d ,n ) 3He reaction provided the quasimonoenergetic neutron beam. The experimental setup and methods used to determine the fission product yield (FPY) are described, and results for typically eight high-yield fission products are presented. Our FPYs for 235U(n ,f ) , 238U(n ,f ) , and 239Pu(n ,f ) at 8.9 MeV are compared with the existing data below 8 MeV from Glendenin et al. [Phys. Rev. C 24, 2600 (1981), 10.1103/PhysRevC.24.2600], Nagy et al. [Phys. Rev. C 17, 163 (1978), 10.1103/PhysRevC.17.163], Gindler et al. [Phys. Rev. C 27, 2058 (1983), 10.1103/PhysRevC.27.2058], and those of Mac Innes et al. [Nucl. Data Sheets 112, 3135 (2011), 10.1016/j.nds.2011.11.009] and Laurec et al. [Nucl. Data Sheets 111, 2965 (2010), 10.1016/j.nds.2010.11.004] at 14.5 and 14.7 MeV, respectively. This comparison indicates a negative slope for the energy dependence of most fission product yields obtained from 235U and 239Pu , whereas for 238U the slope issue remains unsettled.

  10. Pulmonary immune response of dogs after exposure to 239PuO2

    This study evaluated the cell-mediated (CMI) and humoral immune responses in four Beagle dogs five to six years after single inhalation exposures to different monodisperse 239PuO2 aerosols (0.72-1.4μm activity median aerodynamic diameter). These exposures resulted in initial lung burdens ranging from 19 to 35kBq. The immune responses induced by lung immunization of dogs that had inhaled 239PuO2 were not suppressed by large doses of chronic alpha irradiation of the lungs and tracheobronchial lymph nodes, indicating that local pulmonary immune responses are preserved despite severe radiation-induced alteration of these tissues. (author)

  11. Effects of inhalation of 239PuO2 on immune responses following lung immunization

    Results of this study indicated that the number of antibody-forming cells in lung-associated lymph nodes after intratracheal immunization was significantly lower in animals exposed to 239PuO2. Only a few antibody-forming cells were found in spleen and cervical lymph nodes. Thus, 239PuO2 exposure suppressed immune responses in lung-associated lymph nodes, although their filtering capacity was unaffected and antigen did not translocate to the spleen. Changes in immunologic responses were observed as the animals aged and the number of antibody-forming cells gradually decreased in the lung-associated lymph nodes and increased in the spleen

  12. Effects of 239Pu administered at 9 days of gestation on hematologic development of the rat

    Injection of pregnant rats with monomeric 239Pu after 9 days of gestation decreased their leukocyte and reticulocyte counts at 5 and 10 days postexposure. Most of the fetal hematologic enumerative values were unaffected by injection of monomeric 239Pu. There was, however, a major change in the maturation of the cells of the erythroid series, as indicated by a difference in the distribution between cell types. The weight of the yolk sac and fetal liver, and the cellularity of the fetal spleen were decreased

  13. Effect of inhaled 239PuO2 on alveolar Type II cells

    Morphological changes of rat alveolar type II (AT-II) cells were studied at 8 and 10 months following inhalation of 239PuO2 to elucidate the biological role of AT-II cells in the induction of lung tumours. TEM micrographs of random sections of lung were analysed qualitatively and quantitatively using an automatic image analyser. Eighteen morphometric parameters were obtained according to stereological principles. The results showed that, following the inhalation of 239PuO2, AT-II cells became less differentiated and the metabolism of the pulmonary surfactant in AT-II cells was disturbed. (author)

  14. Effect of inhaled 239PuO2 on alveolar type II cells

    Morphological changes of rat alveolar type II (AT-II) cells were studied at 8 and 10 months following inhalation of 239PuO2 to elucidate the biological role of At-II cells in the induction of lung tumours. TEM micrographs of random sections of lung were analysed qualitatively and quantitatively using an automatic image analyser. Eighteen morphometric parameters were obtained according to stereo logical principles. The results showed that, following the inhalation of 239PuO2, AT-II cells became less differentiated and the metabolism of the pulmonary surfactant in AT-II cells was disturbed

  15. Response of CR-39 plastic track detector to 239Pu and 252Cf sources

    CR-39 plastic track detectors have been irradiated with 239Pu and 252Cf sources separately at nuclear physics laboratory B.H.U., Varanasi to investigate track recording properties of detector material. All detectors etched in 6.25N NaOH solution at different temperatures for different hours. The bulk and track etch rates are calculated for both detectors (irradiated by 239Pu and 252Cf sources separately). The diameter and sensitivity along the trajectory of the track have been determined at different temperatures. (author)

  16. Effects of pregnancy and lactation on the toxicity of 239Pu

    Nulliparous, pregnant, or lactating Wistar rats were injected intravenously with 0, 0.5 or 2.0 μCi of 239Pu per kilogram of body weight. Half of each group were repeatedly bred while the others were held for observation without further treatment. Treatment with either dose of 239Pu decreased the median time to appearance of mammary tumors. Repeated breeding tended to increase the mean time to appearance. Longevity was decreased in a dose-related fashion by Pu administration. Repeated breeding did not influence survival in a major way

  17. Potential of Vetiveria zizanoides L. Nash for phytoremediation of plutonium ((239)Pu): Chelate assisted uptake and translocation.

    Singh, Shraddha; Fulzele, D P; Kaushik, C P

    2016-10-01

    Plants have demonstrated a great potential to remove toxic elements from soils and solutions and been successfully used for phytoremediation of important radionuclides. Uptake potential of vetiver plants (V. zizanoides) for the remediation of (239)Pu in hydroponic and soil conditions was studied in the present work. High efficiency of V. zizanoides for the removal of (239)Pu was recorded with 66.2% being removed from the hydroponic solution after 30 days. However, remediation of (239)Pu from soil was limited. Remediation of (239)Pu from soil was increased with the addition of chelating agents citric acid (CA) and diethylenetriaminepentaacetic acid (DTPA). Accumulation of (239)Pu was recorded higher in roots than shoots, however its translocation from roots to shoots increased in the presence of chelators in hydroponic as well as soil conditions. DTPA was found more effective than CA showing higher translocation index (TI). Increase in TI was observed 8 and 6 times in the solution and soil respectively when plants were exposed to (239)Pu-DTPA in comparison to only (239)Pu. The present study demonstrates that V. zizanoides plant is a potential plant for phytoremediation of (239)Pu. PMID:27318195

  18. Modifying effects of pre-existing fibrosis in rats exposed to aerosols of 239PuO2. II

    We have initiated a study using rats to determine the modifying effects of pre-existing pulmonary fibrosis on the retention and biological effects of inhaled 239PuO2. Pulmonary fibrosis was induced by intratracheal instillation of 8.5 IU/kg body weight of bleomycin at 45 to 49 days before inhalation exposure to an aerosol of 239PuO2. The clearance of 239Pu from the lungs of rats was decreased significantly (p 239Pu, apparently by entrapping the particles in fibrotic areas of the lung. The life span of the rats with pulmonary fibrosis was decreased by up to 25% compared with control rats having similar initial lung burdens of 239Pu. (author)

  19. Biological effects of 239PuO2 inhalation in the Rhesus monkey

    Rhesus monkeys were exposed to polydisperse, high-fired 239PuO2 aerosols and have been studied for 3 yr to determine the biological effects associated with this inhalation exposure. Initial lung burdens in 16 monkeys exposed to aerosols of 239PuO2 ranged from 7 to 1800 nCi. Two monkeys are serving as controls. The inhaled 239 PuO2 was retained with a long effective half-life in the lung with some translocation from the lung to the pulmonary lymph nodes. In animals exposed to high levels of 239PuO2, there was a depression in the number of lymphocytes in the peripheral blood. However, blood lymphocytes cultured at time periods up to 30 mo after inhalation showed no increase in chromosome aberration frequency. An animal with an estimated initial lung burden of 1000 nCi showed marked alterations in respiratory function. Only slight respiratory changes were detected in the other animals evaluated. To date, three monkeys have died, two of radiation pneumonitis and the third of gastric torsion. Comparing these data from Rhesus monkeys with those obtained from baboons and Beagle dogs indicate that Rhesus monkeys are similar to dogs in their early radiation response

  20. Pulmonary distribution of inhaled 239PuO2 in dogs

    Dogs exposed to 239PuO2 by inhalation were killed from 1 to 69 mo postexposure. The distribution of plutonium in the lungs, which was studied by analyzing autoradiographs, changed relative to time postexposure. This study investigates methods of measuring these changes

  1. Isotope ratios of 240Pu/239Pu in soil samples from different areas

    Plutonium concentrations and 240Pu/239Pu atom ratios in soil samples from Japan and other areas in the world (including IAEA standard reference materials) were determined by ICP-MS. The range of 240Pu/239Pu atom ratios observed in 21 Japanese soil samples was 0.155 - 0.194 and the average was 0.180 ± 0.011, which is comparable to the global fallout value. A low ratio of about 0.05, which is derived from Pu-bomb, was found in samples from Nishiyama (Nagasaki) and Mururoa Atoll (IAEA-368), while a high ratio of about 0.31 was found in a sample from Bikini Atoll (Marshall Islands). The ratio for Irish Sea sediment (IAEA-135) was 0.21, which was higher than the global fallout value, suggesting the influence by the contamination from the Sellafield facility. The 240Pu/239Pu atom ratios in soils from the Chernobyl area were determined, and the ratio was found to be very high (about 0.4), indicating the high burn-up grade of the reactor fuel. These results show that the 240Pu/239Pu ratio can be used as a finger print to identify the source of the contamination. (author)

  2. Yield-Energy Evaluation of 85Kr of 239Pu+n Fission

    2008-01-01

    <正>The yields of 85Kr, the important production of the 239Pu fission, were re-evaluated over the incident neutron energy 1-15 MeV, based upon all the experimental data. The yields as function of energ

  3. Effects of inhaled 239PuO2 on the primary immune response of beagle dogs

    Effects of inhaled 239PuO2 on the humoral component of the immune system were measured by intravenous immunizations of beagle dogs with keyhole limpet hemocyanin (KLH). With this T-cell-dependent antigen, a significant decrease in primary antibody response was observed in exposed versus unexposed dogs

  4. R-matrix analysis of the 239Pu cross sections up to 1 keV

    The results are reported of an R-matrix resonance analysis of the 239Pu neutron cross sections up to 1 keV. After a description of the method of analysis the nearly 1600 resonance parameters obtained are listed and extensive graphical and numerical comparisons between calculated and measured cross-section and transmission date are presented. 47 refs., 47 figs., 8 tabs

  5. Chromosome aberration frequency in blood lymphocytes of animals with 239Pu lung burdens

    Other investigators have suggested a causal relationship between accidental 239Pu exposures in man and the presence of chromosome aberrations in blood lymphocytes. To assess this relationship experimimentally, 16 Rhesus monkeys and 171 Chinese hamsters were exposed by inhalation to 239PuO2 aerosols and an additional five hamsters were injected with 239Pu citrate and the frequency of aberrations in blood lymphocytes determined. After an initial rapid clearance phase, the 239Pu was retained in the monkey lung with a long effective half-life (greater than 500 days). At 30 days after inhalation, 99 percent of the sacrifice body burden was in the lungs of both species. The ranges of cumulative radiation dose to the hamster lungs 30 days after inhalation were calculated to be 80 to 170, 220 to 540, and 830 to 2120 rads for initial lung burden levels of 10 to 30, 30 to 70, and 180 to 260 nCi/g, respectively. By 120 days, these doses were calculated to be 40 to 350, 500 to 710, and 1440 to 2170 rads. Hamsters with the highest lung burdens had a median survival time of about 80 days. No deaths occurred in any of the other treated hamsters or monkeys by 250 days after 239Pu inhalation. Hamsters sacrificed at 30 days showed an increase in chromosome aberration frequency with increasing dose to lung. By 120 days after inhalation, the aberration frequency in the controls was 0.012. The frequency in animals with doses that produced significant life shortening (1440 to 2170 rads) had decreased to 0.018 and to 0.032 aberrations/cell in animals with lung doses of 500 to 710 rads. At 380 days after injection of 60 nCi 239Pu citrate/gm, hamster lymphocytes had an aberration frequency of 0.048 aberrations/cell. The level of chromosome damage in the 239PuO2 exposed monkeys at 30 and 90 days after inhalation was not different than observed in controls. (U.S.)

  6. Radiation effect of 239PuO2 on human cells in vitro

    In this paper, the in vitro short and long term effects of 239PuO2 on human embryo lung fibroblast are reported. The short term effect observed is the changes in proliferation and survival of the cell line which were exposed to 239PuO2 with concentration of 0.0006 μCi/mL for a week. On 7th day, the proliferation was only 4.88 PDN (population doubling number), while the control was 10.5 PDN. On the 6th day the surviving fraction of the treated cells was 56.3% and that of the control was 96%. For the long term effect studies, the follow-up observation for 12 groups of cell culture exposed to 239PuO2 of 0.0015 and 0.003 μCi/mL was made. In the cultures exposed to 239PuO2 of 0.003 μCi/mL, the shape of the cells became shorter and their life-span shortened with a higher mortality and death appears early. In 7 cultures exposed to 239PuO2 of 0.0015 μCi/mL, the change in cell morphology was the same as above and their life span was shortened by 58.7% averagely in comparison with control. On other two cultures of them not only was no life-span shortening found, but it was longer than that in the control and their inherent characteristics of regionol arrangment disappeared. At last epithelium-like shape of transformed cells were appeared. In the electron microscope siking of the nuclear membranes into nucleus and hypertrophy of the nucleolus with netted structure can be observed. The nuclear volume increased largely and the ratio between nucleus and cytoplasm increased

  7. Applicability of {sup 239}Pu as a tracer for soil erosion in the wet-dry tropics of northern Australia

    Lal, R., E-mail: rajeev.lal@anu.edu.au [Department of Nuclear Physics, Research School of Physics and Engineering, Australian National University, Canberra, ACT 0200 (Australia); Tims, S.G.; Fifield, L.K. [Department of Nuclear Physics, Research School of Physics and Engineering, Australian National University, Canberra, ACT 0200 (Australia); Wasson, R.J.; Howe, D. [Charles Darwin University, Darwin, NT 0810 (Australia)

    2013-01-15

    The technique of accelerator mass spectroscopy (AMS) has been employed to determine modern soil loss rates through the analysis of {sup 239}Pu profiles in soil cores from the Daly basin in Northern Territory, Australia. In areas in which soil conservation banks were not present or were only added recently (<25a) and which had a history of grazing and cultivation the measured soil loss rates over the past {approx}50 years were 7.5-19.5 t ha{sup -1} a{sup -1}. The measured rates are up to 5 times higher compared to agricultural and uncultivated areas within soil conservation banks in other parts of the catchment. High intensity seasonal rainfall combined with reduction in land cover due to grazing and episodic bush fires are primary factors influencing erosion although other impacts on the landscape such as tillage generated runoff and land clearing seem to be responsible for accelerated sediment production.

  8. Evaluating and adjusting 239Pu, 56Fe, 28Si and 95Mo nuclear data with a Monte Carlo technique

    In this paper, Monte Carlo optimization and nuclear data evaluation are combined to produce optimal adjusted nuclear data files. The methodology is based on the so-called 'Total Monte Carlo' and the TALYS system. Not only a single nuclear data file is produced for a given isotope, but virtually an infinite number, defining probability distributions for each nuclear quantity. Then each of these random nuclear data libraries is used in a series of benchmark calculations. With a goodness-of-fit estimator, best 239Pu, 56Fe, 28Si and 95Mo evaluations for that benchmark set can be selected. A few thousands of random files are used and each of them is tested with a large number of fast, thermal and intermediate energy criticality benchmarks. From this, the best performing random file is chosen and proposed as the optimum choice among the studied random set. (authors)

  9. Applicability of 239Pu as a tracer for soil erosion in the wet-dry tropics of northern Australia

    The technique of accelerator mass spectroscopy (AMS) has been employed to determine modern soil loss rates through the analysis of 239Pu profiles in soil cores from the Daly basin in Northern Territory, Australia. In areas in which soil conservation banks were not present or were only added recently (−1 a−1. The measured rates are up to 5 times higher compared to agricultural and uncultivated areas within soil conservation banks in other parts of the catchment. High intensity seasonal rainfall combined with reduction in land cover due to grazing and episodic bush fires are primary factors influencing erosion although other impacts on the landscape such as tillage generated runoff and land clearing seem to be responsible for accelerated sediment production.

  10. 240Pu/239Pu atom ratios in seawater from the western North Pacific and its marginal sea

    Full text: The atom ratio of 240Pu/239Pu is known to be a useful tracer to identify the sources of plutonium in the ocean. The objectives of this study are to measure the 239+240Pu activities and 240Pu/239Pu atom ratios in seawater from the western North Pacific and its marginal sea and to discuss the transport processes of plutonium. The 240Pu/239Pu atom ratios were measured with sector-field ICPMS. The atom ratios were significantly higher than the mean global fallout ratio. These high atom ratios proved the existence of close-in fallout plutonium originating from the Pacific proving grounds. (author)

  11. Characterization of a neutron source of {sup 239}PuBe; Caracterizacion de una fuente de neutrones de {sup 239}PuBe

    Hernandez V, R.; Chacon R, A.; Hernandez D, V. M.; Mercado, G. A.; Vega C, H. R. [Universidad Autonoma de Zacatecas, Unidad Academica de Estudios Nucleares, Calle Cipres No. 10, Fracc. La Penuela, 98068 Zacatecas (Mexico); Ramirez G, J. [Instituto Nacional de Estadistica Geografia e Informatica, Direccion General de Innovacion y Tecnologia de Informacion, Av. Heroes de Nacozari Sur 2301, Fracc. Jardines del Parque, 20276 Aguascalientes (Mexico)], e-mail: ruben_zac@yahoo.com

    2009-10-15

    The spectrum equivalent dose and environmental equivalent dose f a {sup 239}PuBe source have been determined. The appropriate handling of a neutron source depends on the knowledge of its characteristics, such as its energy distribution, total rate of flowing and dosimetric magnitudes. In many facilities have not spectrometer that allows to determine the spectrum and then area monitors are used that give a dosimetric magnitude starting from measuring the flowing rate and the use of conversion factors, however this procedure has many limitations and it is preferable to measure the spectra and starting from this information the interest dosimetric magnitudes are calculated. In this work a Bonner sphere spectrometer has been used with a {sup 6}LiI(Eu) scintillator obtaining the count rates that produce, to a distance of 100 cm, a {sup 239}PuBe source of 1.85E(11) Bq. The spectrum was reconstructed starting from the count rates using BUNKIUT code and response matrix UTA4. With the spectrum information was calculated the source intensity, total flow, energy average, equivalent dose rate, environmental equivalent dose rate, equivalent dose coefficient and environmental equivalent dose coefficient. By means of two area monitors for neutrons, Eberline ASP-1 and LB 6411 of Berthold the equivalent dose and environmental equivalent dose were measured. The determinate values were compared with those reported in literature and it found that are coincident inside 17%. (Author)

  12. Studies of Neutron-Induced Fission of 235U, 238U, and 239Pu

    Duke, Dana; TKE Team

    2014-09-01

    A Frisch-gridded ionization chamber and the double energy (2E) analysis method were used to study mass yield distributions and average total kinetic energy (TKE) release from neutron-induced fission of 235U, 238U, and 239Pu. Despite decades of fission research, little or no TKE data exist for high incident neutron energies. Additional average TKE information at incident neutron energies relevant to defense- and energy-related applications will provide a valuable observable for benchmarking simulations. The data can also be used as inputs in theoretical fission models. The Los Alamos Neutron Science Center-Weapons Neutron Research (LANSCE - WNR) provides a neutron beam from thermal to hundreds of MeV, well-suited for filling in the gaps in existing data and exploring fission behavior in the fast neutron region. The results of the studies on 238U, 235U, and 239Pu will be presented. LA-UR-14-24921.

  13. Investigation of the resonance self-shielding effect in the α-value of 239Pu

    Gamma-spectra from 1 to 15 multiplicities were measured on 122 m flight path of the IBR-30 pulsed neutron booster using a 16-section liquid scintillation detector of a total volume of 80 l for two thin metallic radiator-samples of 239Pu in the presence of a filter-samples with four thickness: 0.3, 0.5, 1 and 2.3 mm in the neutron beam and without them. The multiplicity distribution spectra, the average multiplicities and the alpha value α = σγ/σf for 27 resonances in the energy region 7-170 eV and for the energy group in the region 4.65-2150 eV with and without filter-samples of 239Pu in the beam were obtained. The self-shielding effect in the alpha value and the average multiplicity in limits 5-40% of experimental value is observed

  14. Toxicity of 239PuO2 in immature Beagle dogs. X

    Immature beagles have been exposed by inhalation to a monodisperse aerosol of 239PuO2 (1.5 μm AMAD) to compare the biological effects with those being observed in dogs exposed to a similar aerosol when they were young or aged adults. The study includes 96 dogs exposed to 239PuO2 and 12 controls. A total of 66 experimental and 11 control dogs are still alive. Six dogs died during the past year, all of radiation-related causes. Five dogs died from lung carcinomas and the sixth dog died of pneumonia/fibrosis, but with a lung tumor. With the large number of dogs still alive in this study, it is still premature to compare the cancer dose-response relationships for the immature and adult dogs. (author)

  15. R matrix analysis of the 239Pu cross sections up to 600 eV

    The ENDF/B-V representation of the 239Pu neutron cross sections in the resonance region is unsatisfactory: the single-level formalism is used, necessitating a structured file 3 contribution. Furthermore, Salvatores et al. have stressed the need to extend the resolved resonance region above the present ENDF/B limit of 300 eV for the calculation of Doppler effect and self-shielded group cross sections. The purpose of our work is to improve the representation of the 239Pu cross sections by using a multilevel formalism (which avoids the need for the file 3 contributions) and by extending the resolved resonance range from 300 up to 600 eV. The present resonance analysis is based on the Reich-Moore multilevel formalism and was performed with the Bayesian code SAMMY. The resonance parameters published in 1974 by Derrien were used as prior information. More than 200 levels and 1000 resonance parameters are included in the analysis

  16. Alpha and conversion electron spectroscopy of 238,239Pu and 241Am and alpha-conversion electron coincidence measurements

    Dion, Michael P.; Miller, Brian W.; Warren, Glen A.

    2016-09-01

    A technique to determine the isotopic constituents of a mixed actinide sample has been proposed by a coincident alpha-conversion electron measurement. This presents a unique signature to allow the unfolding of isotopes that possess overlapping alpha particle energy and reduce backgrounds of an unseparated sample. The work presented here are results of conversion electron spectroscopy of 241Am, 238Pu and 239Pu using a dual-stage peltier-cooled 25 mm2 silicon drift detector and alpha spectroscopy with a passivated ion implanted planar silicon detector. The conversion electron spectra were evaluated from 20-55 keV based on fits to the dominant conversion electron emissions, which allowed the relative conversion electron emission intensities to be determined. These measurements provide crucial singles spectral information and calibration to aid in the coincident measurement approach. Furthermore, an alpha-conversion electron spectrometer was assembled using the silicon based detectors described and results of a coincident spectrum analysis is reported for 241Am.

  17. Fission Mode Influence on Prompt Neutrons and γ-rays Emitted in the Reaction 239Pu(nth,f)

    Serot, O.; Litaize, O.; Regnier, D.

    Recently, a Monte-Carlo code, which simulates the fission fragment de-excitation process, has been developed at CEA- Cadarache. Our aim is to get a tool capable to predict spectra and multiplicities of prompt particles (neutron and gamma) and to investigate possible correlations between fission observables. One of the main challenges is to define properly the share of the available excitation energy at scission between the two nascent fission fragments. Initially, after the full acceleration of the fission fragments, these excitation energies were treated within a Fermi-gas approximation in aT2 (where a and T stand for the level density parameter and the nuclear temperature) and a mass dependent law of the temperature ratio (RT=TL/TH, with TL and TH the temperature of the light and heavy fragment) has been proposed. With this RT-law, the main fission observables of the 252Cf(sf) could be reproduced. Here, in order to take into account the fission modes by which the fissioning nucleus undergoes to fission, we have adopted a specific RT-law for each fission mode. For actinides, the main fission modes are called Standard I, Standard II and Super Long (following Brosa's terminology). This new procedure has been applied in the case of the thermal neutron induced fission of 239Pu, reaction for which fission modes are rather well known.

  18. Neutron-induced transmutation reactions in 237Np, 238Pu, and 239Pu at the massive natural uranium spallation target

    Transmutation reactions in the 237Np, 238Pu, and 239Pu samples were investigated in the neutron field generated inside a massive (m = 512 kg) natural uranium spallation target. The uranium target assembly QUINTA was irradiated with the deuteron beams of kinetic energy 2, 4, and 8 GeV provided by the Nuclotron accelerator at the Joint Institute for Nuclear Research (JINR) in Dubna. The neutron-induced transmutation of the actinide samples was measured off-line by implementing methods of gamma-ray spectrometry with HPGe detectors. Results of measurement are expressed in the form of both the individual reaction rates and average fission transmutation rates. For the purpose of validation of radiation transport programs, the experimental results were compared with simulations of neutron production and distribution performed by the MCNPX 2.7 and MARS15 codes employing the INCL4-ABLA physics models and LAQGSM event generator, respectively. In general, a good agreement between the experimental and calculated reaction rates was found in the whole interval of provided beam energies

  19. Early effects of inhaled 239Pu(NO3)4 aerosols in beagle dogs

    Beagle dogs given a single inhalation exposure to 239Pu(NO3)4, and observed for life-span dose-effect relationship, died from radiation pneumonitis (4 of 5) at the highest dosage level, 14 to 25 mo postexposure. There were also indications in these dogs of radiation osteosis, characterized by peritrabecular fibrosis. Leukopenia, lymphopenia, neutropenia and decreased numbers of circulating monocytes and eosinophils occurred at the two highest dosage levels, as previously reported

  20. Analysis of the 239Pu neutron cross sections from 300 to 2000 eV

    A recent high-resolution measurement of the neutron fission cross section of 239Pu has allowed the extension from 1 to 2 keV of a previously reported resonance analysis of the neutron cross sections, and an improvement of the previous analysis in the range 0.3 to 1 keV. This report analyzes this region. 8 refs., 1 fig., 2 tabs

  1. Presence of plutonium isotopes, {sup 239}Pu and {sup 240}Pu, in soils from Chile

    Chamizo, E., E-mail: echamizo@us.es [Centro Nacional de Aceleradores, Avda. Thomas Alba Edison, 7, 41092 Sevilla (Spain); Garcia-Leon, M., E-mail: manugar@us.es [Departamento de Fisica Atomica, Molecular y Nuclear, Universidad de Sevilla, Avda. Reina Mercedes sn, 41012 Seville (Spain); Peruchena, J.I., E-mail: jiperuchena@gmail.com [Centro Nacional de Aceleradores, Avda. Thomas Alba Edison, 7, 41092 Sevilla (Spain); Cereceda, F., E-mail: francisco.cereceda@usm.cl [Laboratorio de Quimica Ambiental, Centro de Tecnologias Ambientales (CETAM), Universidad Tecnica Federico Santa Maria, Casilla 110-V, Valparaiso (Chile); Vidal, V., E-mail: victor.vidal@usm.cl [Laboratorio de Quimica Ambiental, Centro de Tecnologias Ambientales (CETAM), Universidad Tecnica Federico Santa Maria, Casilla 110-V, Valparaiso (Chile); Pinilla, E., E-mail: epinilla@unex.es [Departamento de Quimica Analitica, Facultad de Ciencias, Universidad de Extremadura, Avda. de Elvas sn, 06071 Badajoz (Spain); Miro, C., E-mail: cmiro@unex.es [Departamento de Fisica Aplicada, Universidad de Extremadura, Avda. de la Universidad sn, 10071 Caceres (Spain)

    2011-12-15

    Plutonium is present in every environmental compartment, due to a variety of nuclear activities. The Southern Hemisphere has received about 20% of the global {sup 239}Pu and {sup 240}Pu environmental inventory, with an important contribution of the so-called tropospheric fallout from both the atmospheric nuclear tests performed in the French Polynesia and in Australia by France and United Kingdom, respectively. In this work we provide new data on the impact of these tests to South America through the study of {sup 239}Pu and {sup 240}Pu in soils from different areas of Northern, Central and Southern Chile. The obtained results point out to the presence of debris from the French tests in the 20-40 Degree-Sign Southern latitude range, with {sup 240}Pu/{sup 239}Pu atomic ratios quite heterogeneous and ranging from 0.02 to 0.23. They are significantly different from the expected one for the global fallout in the Southern Hemisphere for the 30-53 Degree-Sign S latitude range (0.185 {+-} 0.047), but they follow the same trend as the reported values by the Department of Energy of United States for other points with similar latitudes. The {sup 239+240}Pu activity inventories show as well a wider variability range in that latitude range, in agreement with the expected heterogeneity of the contamination.

  2. 235 U consumption and 239 Pu formation on IPR-R1 reactor

    On the present world conjuncture it is necessary a rigorous storage and utilization control of nuclear materials under safeguard, specially those considered as strategic and those that could be used on the nuclear armaments fabrications as 235U and 239Pu. Brazil have signed and ratified many international pacts related to the peaceful utilization of the nuclear materials, making the compromise to attend nuclear safeguard procedures accorded with international regulatory organizations. The main goal of this work is the development of a simplified method for the estimation of the 239Pu productivity during the operation of the IPR-R1, TRIGA Mark-1 type, nuclear research reactor, that can achieve the maximum power of 100 KWt. A computational algorithm have been made to calculate the consumption of 235U on the fuel elements used on the reactor and the subsequent 239Pu formation (by the neutronic capture process), using the power generated by the reactor since the first criticality. The particular geometry of this kind of reactor allowed the calculation of the burn factors of the fuel elements discriminated by nuclear concentric rings, based on the thermal neutrons field distribution observed on experiments accomplished during a time period in similar reactors and on the IPR-R1. The simplified block diagram of the process, based on the calculation described above, is presented

  3. Presence of plutonium isotopes, 239Pu and 240Pu, in soils from Chile

    Plutonium is present in every environmental compartment, due to a variety of nuclear activities. The Southern Hemisphere has received about 20% of the global 239Pu and 240Pu environmental inventory, with an important contribution of the so-called tropospheric fallout from both the atmospheric nuclear tests performed in the French Polynesia and in Australia by France and United Kingdom, respectively. In this work we provide new data on the impact of these tests to South America through the study of 239Pu and 240Pu in soils from different areas of Northern, Central and Southern Chile. The obtained results point out to the presence of debris from the French tests in the 20–40° Southern latitude range, with 240Pu/239Pu atomic ratios quite heterogeneous and ranging from 0.02 to 0.23. They are significantly different from the expected one for the global fallout in the Southern Hemisphere for the 30–53°S latitude range (0.185 ± 0.047), but they follow the same trend as the reported values by the Department of Energy of United States for other points with similar latitudes. The 239+240Pu activity inventories show as well a wider variability range in that latitude range, in agreement with the expected heterogeneity of the contamination.

  4. Investigations of the chemical forms of 239Pu and 241Am in estuarine sediments and a salt marsh soil

    Estuarine sediments and a salt marsh soil have been fractionated by non-destructive procedures. The distribution of 239Pu and 241Am in these fractions has been determined by gel permeation chromatography and extraction with complexing agents. (author)

  5. Neutron inelastic-scattering cross sections of 232Th, 233U, 235U, 238U, 239Pu and 240Pu

    Differential-neutron-emission cross sections of 232Th, 233U, 235U, 238U, 239Pu and 240Pu are measured between approx. = 1.0 and 3.5 MeV with the angle and magnitude detail needed to provide angle-integrated emission cross sections to approx. 232Th, 233U, 235U and 238U inelastic-scattering values, poor agreement is observed for 240Pu, and a serious discrepancy exists in the case of 239Pu

  6. Modification of 239Pu metabolism in the blood in various modes of iron preparation administration in the body

    A study was made of the intravenous, intraperitoneal and oral routes of iron administration. It was shown that the oral route of the entry of appropriate amounts of iron in the body made it possible to saturate the transferrin spare capacity and hence to influence 239Pu metabolism in the blood. The results obtained can be employed for improving sensitivity of indirect dosimetry methods of 239Pu in the body using chelates

  7. Group cross-sections and resonance self-shielding factors for 239Pu in the unresolved resonance region

    The authors analyse experimental data on the transmission and fission self-indication functions for 239Pu in the unresolved resonance region. Use is made of the method of generating a cross-section structure based on the multi-level R-matrix formalism (stochastic K-matrix method). Evaluations of the average resonance parameters and group constants for 239Pu are made. (author)

  8. Cytogenetic and other biological effects of 239PuO2 inhaled by the rhesus monkey

    Sixteen immature rhesus monkeys were exposed via inhalation to an insoluble, polydisperse 239PuO2 aerosol labeled with 169Yb which had an activity median aerodynamic diameter of 1.6 μm and a sigma/sub g/ of 1.6. Four groups with three monkeys per group were exposed to achieve initial 239Pu lung burdens of 1000 to 2000, 200 to 300, 20 to 65, and 2 to 10 nCi, respectively. To determine early retention and distribution of the aerosol, four additional monkeys were exposed with initial lung burdens of 200 to 600 nCi and were sacrificed 4 hr and 30 days after inhalation exposure. Two monkeys were sham exposed and served as controls. Using data derived from external whole-body counting of the 169Yb label, it was estimated that the inhaled 239PuO2 was retained in the body with an average effective half-life of 1000 days with some translocation from the lung to the pulmonary lymph nodes. Chromosome aberrations were scored in blood lymphocytes cultured 1, 3, 7, 19, 31, and 43 months after inhalation. Only in animals with cumulative lung doses greater than 1000 rad was there a significant increase in the frequency of rings and dicentrics when compared to the controls. An animal with an estimated initial lung burden of 1000 nCi showed marked alterations in respiratory function 30 days prior to his death from pulmonary fibrosis 990 days after inhalation exposure. Only slight respiratory changes were detected in the other animals evaluated. To date, three monkeys have died, two with initial lung burdens of 1800 and 1000 nCi 239Pu which died from radiation pneumonitis and the third with an initial lung burden of 20 nCi which died of gastric torsion presumably not related to Pu exposure. Comparison of survival data from rhesus monkeys with those obtained from baboons and beagles indicates that rhesus monkeys, baboons, and dogs are similar in their early response to inhaled 239PuO2

  9. 239PU(N, f) at Resonance Energies and its Multi-Modal Interpretation

    Hambsch, F.-J.; Bax, H.; Ruskov, I.; Demattè, L.

    2003-10-01

    A measurement of fission fragment total kinetic energy (TKE) and mass yield distributions Y (A,TKE) in the 239Pu(n,f) resolved resonance region has been performed applying the twin Frisch gridded ionization chamber technique. Special emphasis was devoted to cope with the strong α-activity of this isotope by an improved pile-up rejection system. Up to about 200 eV all fission resonances could be resolved and their two-dimensional mass yield and TKE distribution, Y(A,TKE), measured. Compared to the results on 235U(n,f), much smaller fluctuations of the fission fragment mass and TKE have been observed in the case of 239Pu. From a physical point of view such fluctuations have been expected for the fission fragment properties, because the only possible lowenergy spin states (Jπ=0+,1+) belong to well separated (about 1.25 MeV) transition state bands. Hence, it was expected to observe differences in the fission fragment mass and TKE distributions between spin 0+ and 1+ resonances. However, no spin dependence and only a slight anti-correlation of the TKE with the prompt neutron multiplicity, νp. has been found in the resolved resonance energy region above 1 eV. Within the multi-modal random neck-rupture (MM-RNR) model the Y(A,TKE) distributions have been fitted assuming three fission modes, two asymmetric and one symmetric one. The branching ratio of the two asymmetric modes shows similar fluctuations as the experimental TKE. Recently, a new theoretical approach has given a solution to the absence of pronounced fluctuations of the fission properties in the case of 239Pu. Since only one transition state is involved in the fission of 0+ and 1+ resonances with a given fission fragment distribution, no fluctuations are expected.

  10. In vitro studies of actinides and alveolar macrophages

    The toxicity of 239PuO2, 239Pu(NO3)4, and 241AmO2 to rabbit alveolar macrophages in culture was assessed. Comparison of toxicity of 239Pu(NO3)4 and 241AmO2 at the same radiation dose level indicates toxicity is due to radiation and not the chemical form of the actinide. Investigations were begun to determine the effect of serum macrophages and DTPA on 241AmO2 solubility

  11. Direct reduction of 238PuO2 and 239PuO2 to metal

    The process for reducing 700 g 239PuO2 to metal is a standard procedure at Los Alamos National Laboratory. This process is based on research for reducing 200 g 238PuO2 to metal. This report describes in detail the experiments and development of the 200-g process. The procedure uses calcium metal as the reducing agent in a molten CaCl2 solvent system. The process to convert impure plutonia to high-purity metal by oxide reduction followed by electrorefining is also described

  12. Distribution and retention of 239Pu in the tree shrew (Tupaia belangeri) following intramuscular injection

    The retention of intramuscularly injected monomeric 239Pu has been studied in the tree shrew (Tupaia belangeri), a primitive prosimian species. Resorption from the injection site is rapid, and the main depository organs are skeleton and liver with approximately 50 and 20% of the absorbed dose, respectively. The half life of retention in skeleton is approximately 500-600 days and in liver approximately 150 days, these half lives are compared to data for the retention of transuranium elements in other animal species. Indications of liver lesions were found in 5 animals and 1 animal died at day 790 with an osteosarcoma. (author)

  13. The evaluation of the mass distribution data for 238U, 239Pu and 242Pu fission

    The mass distribution data for 238U at En=1.5, 5.5, 8.3, 11.3, 14.9, 22.0, 27.5, 50.0, 99.5, 160.0 MeV, Ep=20.0, 60.0 MeV 239Pu at En=0.17, 7.9, 14.5 MeV and 242Pu at En=15.1 MeV were evaluated and recommended based on the main available experimental data up to now. The experimental data were make necessary corrections and their errors were also made necessary adjustments. The problems concerned were discussed

  14. Status of 239Pu cross-section evaluation in the resonance region at Cadarache

    Some aspects of the evaluations of 239 Pu cross-sections in the resonance region have been presented in this report. A set of resonance parameters assembling the results of a multilevel analysis in the energy range thermal to 200 eV and the result of a single analysis in the energy range 200 eV - 660eV is proposed for the calculation of the cross-sections in the energy range thermal-600eV. These parameters provide a quite good representation of the most recent measured fission cross-sections

  15. Repeated inhalation exposure of Beagle dogs to aerosols of 239PuO2. XII

    Beagle dogs were exposed once or semi-annually for 10 yr by inhalation to aerosols of 239PuO2 to study the relative doses and effects of these two types of exposures. All exposures have been completed. Dogs exposed at high levels died predominantly of radiation pneumonitis and pulmonary fibrosis. Dogs exposed at lower levels, either once or repeatedly, are dying of a variety of causes including lung cancer. Dogs have survived up to 11 yr after their first exposure. Preliminary results suggest that single and repeated exposures cause similar health effects for equal accumulated radiation doses. (author)

  16. Dominant lethal tests of male mice given 239Pu salt injections

    To study the possible genetic effects of 239Pu manifesting in dominant lethals, five test series (E1-E5) were performed. Males from an inbred CBA strain were given 239Pu salt injections intravenously and mated weekly to 3 CBA females each for 12 to 24 weeks. Some interruptions in the mating scheme were made. For the first two test series (E1, E2) 239Pu nitrate solution and 239Pu citrate, used in E3-E5, were prepared. The solution was millipore filtered just prior to injection. Among a total of 10255 implants sired by males given Pu-nitrate in E1 and E2 no significant excess of intra-uterine death relative to 7216 control implants occurred. Test series E3-E5 with 60 males each, used three groups of 20, with one control group. In E3, 0.5 μCi and 0.1 μCi were given per male/group, respectively; in E4 and E5, 0.25 μCi and 0.05 μCi, respectively. The males given 0.5 μCi in E3 became successively sterile from the 7th week. The results in E3-E5 point in the same direction with significant excess of intra-uterine death in E3 and E5. In E4 the females from matings from the 9th, 14th and 16th week, and in E5 females from the 9th week, were allowed to litter to give F1 offspring. Dominant lethal tests of F1 males gave concordant results in all four samples, showing significantly excessive death in offspring to F1 males whose fathers had received Pu. The excessive death was evenly distributed and did not indicate the presence of semisterile F1 males. In tests of Pu-injected males and of F1 males a remarkable excess of death in late stages of foetal development was observed. Such effects had never before been observed in this CBA strain in tests of extrinsic and intrinsic exposure to ionizing irradiation

  17. Determination of isobar composition and yields of 239Pu fission-products by thermal neutrons

    On the research nuclear reactor WWR-SM of INP Uz AS by means of mass-spectrometer the heavy fission-products of 239Pu nuclei induced by thermal neutrons are measured in ranges of mass Ai = 125 -157, kinetic energies Ek = 45 - 87 MeV and effective ionic charges z* = 18 - 30. 102 isobar nuclei in composition of the measured fission-products, also the partial yields of the each element giving the contribution to formation of a total yield of heavy fission-product with mass Ai are defined. (authors)

  18. On the ENDF/B unresolved resonance region formalism representation for 239Pu

    The purpose of this work is to compare the performance of several cross-section evaluation files for the calculation of average cross sections in the unresolved resonance region and to test the validity of the ENDF/B methodology for the calculation of self-shielding factors in this region. The 239Pu neutron cross sections were used for this comparison since a multilevel R-matrix analysis was available, which extended the resolved resonance region from its present ENDF/B limit of 300 eV up to 1 keV. 12 refs., 2 tabs

  19. R-matrix analysis of the 239Pu neutron cross sections

    239Pu neutron cross-section data in the resolved resonance region were analyzed with the R-Matrix Bayesian Program SAMMY. Below 30 eV the cross sections computed with the multilevel parameters are consistent with recent fission and transmission measurements as well as with older capture and alpha measurements. Above 30 eV no suitable transmission data were available and only fission cross-section measurements were analyzed. However, since the analysis conserves the complete covariance matrix, the analysis can be updated by the Bayes method as transmission measurements become available. To date, the analysis of the fission measurements has been completed up to 300 eV. (author)

  20. Effects of cigarette smoke exposure on pulmonary clearance of 239PuO2 in rats

    Groups of rats were exposed or sham exposed to cigarette smoke for 7 mo, at which time they were exposed to an aerosol of 239PuO2. Rats were then subjected to whole-body counting (17-keV X-rays) periodically, beginning at day 4 after plutonium exposure, and smoke exposures or sham exposures were resumed on day 7. Clearance of plutonium from the lungs of cigarette-smoke-exposed rats was significantly slower than that from the sham-exposed rats' lungs. The difference between the two groups became significant 7 days after the resumption of cigarette-smoke exposures

  1. Radiosensitivity of vertebral bone marrow CFU-S surviving in mice internally contaminated with 239Pu or 241Am

    The radiosensitivity of pluripotent hemopoietic stem cells was studied in ICR ''Swiss'' mice (28 g/mouse) given i.v. 198.6 kBq 239Pu/kg as citrate complex or 208.6 kBq 241Am/kg as nitrate at the age of 10 weeks. The bone marrow cells were examined at the early and late phases of radionuclide contamination. To obtain data for survival curves and D0 of stem cells the CFU-S assay was used and the donor vertebral marrow cells were exposed to the complementary X-irradiation either early after injection to the heavily irradiated recipients or to the ''in vitro'' irradiation given before the transplantation. To determine the iron uptake in splenic erythroid progeny the recipients given marrow cells unexposed to the X-rays received 37 kBq 59Fe 6 h before they were killed and the relative activity per colony was calculated. The radiation effect of the used actinides on the bone marrow cells resulted in decreased cellularity and seriously altered both relative and absolute CFU-S numbers. The radiosensitivity of CFU-S increased in all intervals examined (D0 from 0.60 to 0.86 Gy, in controls 0.97 to 1.06 Gy) and was more expressed when the CFU-S were exposed to the X-rays immediately after the bone marrow cell transplantation to the heavily irradiated hosts. The stem cell pool appeared, especially at older age, to be affected also in its ability to produce erythrocytic progeny. (orig.)

  2. Effect of physical exercise on the state of the heart and central hemodynamics in dogs exposed to external (60Co) and internal (239PuO2) irradiation

    Experiments were conducted on mongrel dogs aged 2 to 4 with the body mass of 15.1 ± 0.9 kg. The animals were exposed to combined and isolated γ-irradiation at a dose of 51.6 mC/kg and submicron 239PuO2 in the amount not less than 7 kBq/kg. Single circular irradiation was provided from 60Co γ-sources at a dose rate of 1.03-1.3 mA/kg. 239PuO2 was inhaled 6 days after irradiation. 20 min. running on a tredbahn with the speed of 4.7 km/h served as a physical exercise model. The dogs were examined 0.5, 1, 1.5 and 4 yrs. after the initiation of the experiment at rest and within 1 h after physical exercise. Methods of tetrapolar chest rheography and electrocardiography were employed. It was shown that in the combined effect of two radiation factors the rates of increase in the cardiac index were inhibited at the expense of physical exercise influence as compared to those in the isolated radionuclide effect and resulted from less ''economical'' heart action

  3. Comparison of early mortality in baboons and dogs after inhalation of 239PuO2

    Results from experiments with baboons were compared with those from experiments with dogs to determine the relative sensitivity of the two species to early mortality from inhaled 239PuO2. To ensure a valid comparison of data developed at two laboratories, methodology differences were minimized by establishing a common pool of raw data, using the same computer programs to analyze the data, and standardizing assumptions regarding the calculation of plutonium concentration in lungs. Several comparison methods were used involving variations in estimating different parameters used in these calculations. Although nearly all comparisons suggested baboons were slightly more sensitive, none of the methods for comparing the relationship between dose and survival time showed consistently significant differences between baboons and dogs. Although the baboons were physiologically and morphologically immature when exposed to plutonium, whereas the dogs were mature, we concluded that adult baboons and dogs are similarly sensitive to the early effects of inhaled 239PuO2. Since only early mortality was considered in this comparison, the results do not apply to possible late effects caused by much lower levels of plutonium than were used in these experiments

  4. Preliminary evaluation of lung doses for dogs exposed to 239PuO2

    A group of beagle dogs exposed to inhaled 239PuO2 is being followed for life-span effects. This paper reports preliminary lung dose estimates and dose-response relationships for incidence of lung tumors and radiation pneumonitis which have been observed to date. Doses were estimated by using both conventional dose-averaging and microdosimetric techniques. Cascade impactor sampling data were used to reconstruct the original plutonium aerosol size distributions unique to each of about 120 individual dogs exposed to 239PuO2. Data providing the initial plutonium lung burden and lifetime lung retention-clearance functions of plutonium for each dog were used for calculating average dose rates, cumulative absorbed doses, and specific energy distributions. A linear dose-response relationship for lung tumor induction was estimated on the basis of cumulative lung dose. Average time to death was estimated as a function of average dose rate. Conclusions regarding the potential value of microdosimetry in the interpretation of such dose-response relationships are discussed. 8 refs., 5 figs., 1 tab

  5. Lymphocytopenia induced in beagle dogs by inhalation of 239PuO2

    To determine the life-span dose-effect relationships of inhaled plutonium, we gave 124 beagle dogs a single exposure of 239PuO2 2 to 3 years ago at six different levels, i.e., 4, 20, 80, 300, 1100, or 5800 nCi mean initial alveolar depositions. Another group (20 dogs) served as controls. All dogs were about 18 months old. At the four highest exposure levels, a chronic lymphocytopenia developed which correlated with the initial alveolar plutonium burden in regard to magnitude of depression and time of development after exposure. The nadir occurred near 10 months after exposure in dogs receiving 5800, 1100, and 300 nCi, with corresponding lymphocyte levels 40, 55, and 75 percent, respectively, of those observed in control dogs. In the 80-nCi level the nadir occurred about 2 years after exposure at approximately 80 percent of control values. At the two lowest doses, i.e., 4 and 20 nCi, no effect on lymphocyte concentrations was noted 3 years after exposure. The persistent lymphocytopenia related to plutonium inhalation may be of significance in the subsequent development of pulmonary neoplasms previously observed in beagles at this laboratory 8 to 11 years after initial lung depositions of 200 to 1000 nCi of 239Pu

  6. Artificial neural networks applied in the spectrometry of a 239Pu-Be source

    To explore the potential use of a neutron source and to define the procedure to handle it under safety conditions, features like neutron spectrum and the ambient dose equivalent of the source must be known. The aim of this work was to determine the spectrum, the total fluence rate and the ambient dose equivalent of a 185 GBq 239Pu-Be neutron source. Using Monte Carlo methods the spectrum, the total fluence rate, and the ambient dose equivalent of a 239Pu-Be were calculated. The spectrum was calculated at 50, 100, 200 and 300 cm from the source in air using MCNP X and MCNP 4C codes. The neutron spectrum was also obtained, at 100 cm, using a Bonner sphere spectrometer whose count rates were used to unfold the neutron spectrum, the unfolding was carried out using an Artificial Neural Network for neutron spectrometry. With the spectrum, the total neutron fluence and the ambient dose equivalent were determined. Calculated results were compared with measured values where Monte Carlo results were smaller than those measured. These differences were attributed to the presence of 241Pu during the source manufacturing. In order to match calculated and measured quantities a 0.102 w/o of 241Pu was estimated. After corrections the differences between calculated and experimental results were 1%. This result shows the advantages of using Artificial Neural Networks technology in the unfolding of neutron spectrum using as a single piece of information the count rates of a Bonner sphere spectrometer. (author)

  7. Alligator Rivers Analogue project. Geochemistry of 239Pu, 129I, 99Tc and 36Cl

    One objective of this research programme has been to evaluate the applicability of uranium orebodies as natural analogues for testing radionuclide release-rate models used in performance assessment activities. The investigated nuclides included three of the most persistent radioactive constituents of high-level wastes from nuclear fission power reactors: plutonium-239, iodine-129, and technetium-99. The feasibility of uranium minerals as analogues for the behavior of these nuclear reaction products (NRP) in spent fuel relies upon a capability to characterise NRP concentrations in the source minerals. Measured abundances of natural 239Pu, 99Tc and 129I in uranium ores are compared to calculated abundances in order to evaluate the degree to retention of these radionuclides by the ore. This modelling study also shows the extent to which various NRP are correlated, such that one provides a constraint on the production rates of others. Under most conditions, 36Cl, another long-lived neutron-capture product found in uranium ores, is shown to be an ideal in-situ monitor of the 235U fission rate, which is the dominant source term for 129I and possibly a significant one for 99Tc. Similarly, 239Pu/U ratios can be used to establish limits on the 238U neutron-induced fission rate; the ratios measured in this study suggest that 238U induced fission comprises 129I and 99Tc. 79 refs., 21 tabs., 18 figs

  8. New data on the toxicity and translocation of inhaled 239PuO2 in baboons

    In 1973-1974, baboons were exposed to a polydispersed aerosol of 239PuO2, prepared at 10000C, at the Commissariat a l'Energie Atomique in France. The data published in 1978 for these baboons were used by Bair et al (1980), for comparison with those obtained in beagles exposed to 239PuO2 at the Pacific Northwest Laboratory, USA. Since our 1978 publication, 8 baboons have died or were killed by euthanasia when moribund, and 11 were still alive when the present report was drafted. Two of the eight baboons died of lung squamous cell carcinoma at 2171 and 2528 days respectively. The remaining 6 died of fibrosis, interstitial pneumonia or diseases unrelated to Pu toxicity. The relationship observed in the eight baboons between initial lung burden and survival time shows that their lifespan was longer than expected from the data curve based on the findings for the first 1000 days. However, this increased survival time was not observed if the lifespan was expressed as a function of the average lung burden. (author)

  9. Comparison of acute mortality in baboons and dogs after inhalation of 239PuO2

    Results from experiments with baboons were compared with those from experiments with dogs to determine the relative sensitivity of the two species to acute mortality from inhaled 239PuO2. To assure a valid comparison of data developed at two laboratories, methodology differences were minimized by establishing a common pool of raw data, using the same computer programs to analyze the data, and standardizing assumptions regarding the calculation of radiation doses to lungs. Several comparison methods were used involving variations in estimating different parameters such as the concentration of plutonium in the lungs. Although nearly all comparisons suggested baboons were slightly more sensitive, none of the methods for comparing the relationship between dose and survival time showed consistently significant differences between baboons and dogs. Although the baboons were physiologically and morphologically immature when exposed to plutonium, whereas the dogs were mature, it was concluded that adult baboons and dogs are similarly sensitive to the acute effects of inhaled 239PuO2. Since only acute mortality was considered in this comparison, the results do not apply to possible late effects caused by much lower levels of plutonium than were used in these experiments

  10. Occurrence of bone cancer among young adult Beagles given 239Pu

    Two hundred thirty-five young adult Beagles of both sexes were each given a single intravenous injection of 239Pu-citrate at graded dose-levels averaging about 0.026 to 106 kBq/kg when they were about 1 1/2 years of age and were maintained for lifespan observation. An additional 133 young adult Beagles of both sexes were entered into the experiment as control animals. All of these animals have now died or have been removed from the colony, and the occurrence of skeletal malignancies has been determined from histological examination. There were a total of 85 radiographically apparent malignant bone tumors in 77 dogs given 239Pu, and there was one control animal that developed a skeletal malignancy. Most of these were osteosarcomas, but there were seven chondrosarcomas of bone, one liposarcoma of bone, and in addition, there was one plasma cell myeloma and one ameloblastoma (admantinoma). Only those dogs that survived to at least the minimum latent period for death with radiation-induced bone sarcoma are included in the tabulation. There appeared to be a linear relationship between the percent of dogs with bone tumor and the average skeletal dose up to a dose of about 1 Gy. All dose-levels with skeletal doses of about 2 Gy and greater exhibited close to 100% occurrence

  11. Role of 239Pu-induced chromosome alterations and mutated Ki-v-ras oncogene during liver-cancer induction in Chinese hamsters and mice

    Chromosome aberrations and mutated oncogenes can cause important changes during carcinogenesis. Model systems are being studied in which defined cellular and molecular changes can be quantitated and altered, and tumor frequency, type, and time of appearance can be evaluated. Dose-response relationships for Pu Citrate-induced chromosome aberrations and liver cancer were measured in Chinese hamsters. Chromosome aberrations increased linearly according to dose, with a slope of 4.8 x 10-1 aberrations/cell/Gy; liver-tumor incidence was 1.1 x 10-1 tumors/animal/Gy. The dose was calculated at the 50% survival time. The interaction between Pu and Ki-v-ras, an altered, dominant-acting oncogene, on the induction of liver cancer was measured in B6C3F1 mice. The neo oncogene was used as a negative control in these studies. The Ki-v-ras oncogene was inserted into a viral vector and incorporated into the livers of mice either 30 days before or after the incorporation of 239Pu. Compared with both the controls and the mice injected with a single insult, mortality increased in groups of animals that received combined exposure to oncogenes, CCl4, and 239Pu. The relationships between molecular and cellular damage and the induction of cancer is being defined in both mice and Chinese hamsters

  12. Microlocalization of 239Pu in structural elements of the interalveolar septa after inhalation of its various compounds and pentacin

    A quantitative and qualitative evaluation of 239 Pu mictodistribution in the structural elements of the interalveolar septa after inhalation of three plutonium compounds different in solubility is made. Thirty minutes after the inhalation 55.3-85.3% of plutonium (dioxide>nitrate>=citrate) was revealed in rhe cells, predominantly in the microphages. More than half of the isotope found in the noncellular elements, lies in the surface layer of the alveoli and the intercellular matter. First 239Pu is seen as ''stars'' of tracks (dioxide), mainly (nitrate) or exclusively (citrate) as individual tracks. The different extent of plutonium elimination from the interalveolar septa (dioxide239Pu from the cells is mainly determined by its escape from the macrophages (dioxide) or from all cellular elements (nitrate, citrate). Pentacin accelates elimination of plutonium from the most of the structural elements of the interalveolar septa (citrate>nitrate)

  13. 239Pu(n,2n) 238Pu cross section inferred from IDA calculations and GEANIE measurements

    Chen, H; Ormand, W E; Dietrich, F S

    2000-09-01

    This report presents the latest {sup 239}Pu(n,2n){sup 238}Pu cross sections inferred from calculations performed with the nuclear reaction-modeling code system, IDA, coupled with experimental measurements of partial {gamma}-ray cross sections for incident neutron energies ranging from 5.68 to 17.18 MeV. It is found that the inferred {sup 239}Pu(n,2n){sup 238}Pu cross section peaks at E{sub inc} {approx} 11.4 MeV with a peak value of approximately 326 mb. At E{sub inc} {approx} 14 MeV, the inferred {sup 239}Pu(n,2n){sup 238}Pu cross section is found to be in good agreement with previous radio-chemical measurements by Lockheed. However, the shape of the inferred {sup 239}Pu(n,2n){sup 238}Pu cross section differs significantly from previous evaluations of ENDL, ENDF/B-V and ENDF/B-VI. In our calculations, direct, preequilibrium, and compound reactions are included. Also considered in the modeling are fission and {gamma}-cascade processes in addition to particle emission. The main components of physics adopted and the parameters used in our calculations are discussed. Good agreement of the inferred {sup 239}Pu(n,2n){sup 238}Pu cross sections derived separately from IDA and GNASH calculations is shown. The two inferences provide an estimate of variations in the deduced {sup 239}Pu(n,2n){sup 238}Pu cross section originating from modeling.

  14. Investigation of forming mechanism of instantaneous neutron spectrum of 235U, 239Pu, 252Cf nuclei fission

    Formation mechanism of prompt neutrons spectrum during the fission of the 235U, 239Pu nuclei by thermal and fast neutrons and spontaneous fission of 252Cf is investigated. The formation procedure for prompt neutrons spectrum during the fission of nuclei as superposition of three partial evaporation Weisskopf spectra with the mean energy of neutrons 0.4, 2.06 and 2.8 MeV is proposed. Formation mechanism of the spectrum just as during the fission of the 235U, 239Pu nuclei by thermal and fast neutrons, so spontaneous fission of the 252Cf nuclei is identical

  15. Calculation of 239Pu fission observables in an event-by-event simulation

    Vogt, R; Randrup, J; Pruet, J; Younes, W

    2010-03-31

    The increased interest in more exclusive fission observables has demanded more detailed models. We describe a new computational model, FREYA, that aims to meet this need by producing large samples of complete fission events from which any observable of interest can then be extracted consistently, including any interesting correlations. The various model assumptions are described and the potential utility of the model is illustrated. As a concrete example, we use formal statistical methods, experimental data on neutron production in neutron-induced fission of {sup 239}Pu, along with FREYA, to develop quantitative insights into the relation between reaction observables and detailed microscopic aspects of fission. Current measurements of the mean number of prompt neutrons emitted in fission taken together with less accurate current measurements for the prompt post-fission neutron energy spectrum, up to the threshold for multi-chance fission, place remarkably fine constraints on microscopic theories.

  16. Pulmonary distribution of inhaled 239PuO2 in dogs

    The distribution of plutonium in the lungs was studied by analyzing autoradiographs from dogs killed up to 69 months after single, nose-only exposures to 239PuO2 aerosols. Within 5 months of exposure, the pattern of alpha-star distribution was relatively dispersed and uniform throughout the lung section, changing by 12 months to a less uniform distribution that exhibited focal concentration, subpleural concentration, and alpha-star aggregation. Increased subpleural concentrations were demonstrated infve of six dogs killed 12 or more months after exposure. The percentage of alpha stars found in localized regions of relatively high concentration and the portion found in aggregation (define here as two or more alpha stars with overlapping tracks) increased with tie postexposure. The data demonstrate that an initial relatively uniform dispersion of plutonium particles changed with time to a focally concentrated distribution with relatively small tissue volume containing most of the pulmonary plutonium burden

  17. The self-absorption effect of gamma rays in 239Pu

    Nuclear materials assay with gamma-ray spectrum measurement is a well-established method for safeguards. However, for a thick source, the self-absorption of characteristic low-energy gamma rays has been a handicap to accurate assay. The author has carried out Monte Carlo simulations to study this effect using the 239Pu α-decay gamma-ray spectrum as an example. The thickness of a plutonium metal source can be considered a function of gamma-ray intensity ratios. In a practical application, gamma-ray intensity ratios can be obtained from a measured spectrum. With the help of calculated curves, scientists can find the source thickness and make corrections to gamma-ray intensities, which then lead to an accurate quantitative determination of radioactive isotopes in the material

  18. Quantitative scanning electron microscopic autoradiography of inhaled 239PuO2

    We have applied the scanning electron microscope (SEM) to obtain autoradiographs of particles of 239PuO2 deposited in rat lung. The technique was used to obtain quantitative information on the clearance rates of particles from the alveoli, bronchioles and trachea up to 240 d after exposure. At all times, the concentration of particles on the surface of the bronchioles was an order of magnitude greater than on the tracheal surface. The clearance of Pu from both regions followed a biphasic pattern, similar to that obtained by radiometric analysis of the whole lung. Most of the radiation dose to the bronchiolar epithelium originated from Pu particles in peribronchiolar alveoli in which they were preferentially retained, compared to other alveolar regions. The prolonged retention of particles in the peribronchiolar alveoli may be a significant factor in the induction of lung carcinomas

  19. Aerosols generated by 239PU and 233U droplets burning in air

    The inhalation hazards of radioactive aerosols produced by the explosive disruption and subsequent combustion of metallic plutonium in air are not adequately understood. Results of a study to determine whether uranium can be substituted for plutonium in such a situation in which experiments were performed under identical conditions with laser-ignited, single, freely falling droplets of 239Pu and 233U are reported. The total amounts of aerosol produced were studied quantitatively as a function of time during the combustion. Also, particle size distributions of selected aerosols were studied with aerodynamic particle separation techniques. Results showed that the ultimate quantity of aerosols, their final particle size distributions, and depositions as a function of time are not identical mainly because of the different vapor pressures of the metals, and the unlike degrees of violence of the explosions of the droplets

  20. The simultaneous determination of 235U and 239Pu using delayed neutron activation analysis

    Delayed neutron activation analysis (DNAA) remains one of the most sensitive methods of nondestructively determining fissile materials in a variety of sample matrices, provided that the samples contain only a single fissile component. This has historically been the limiting factor in many applications of DNAA, and often chemically destructive methods of analysis have needed to be utilized for many real-world samples. This work seeks to develop a method that will allow for DNAA to be utilized on samples containing multiple fissile components. Initial efforts, presented here, show that using a multivariate linear regression model to describe the delayed neutron emission profile of an irradiated sample allows for the concurrent determination of fissile nuclides in samples containing both 235U and 239Pu, without chemical separations and using only a single counting step. (author)

  1. Comparison of rats and dogs exposed to 239PuO2

    Rats and dogs inhaled aerosols of 239PuO2 at comparable ages relative to their lifespan. Both received a single exposure. The estimated lung doses at death in dogs were between 1100 and 11,000 rad. From two inhalation experiments, rats receiving doses in this range were chosen from the high-level exposed animals for comparison. Based on this data base, several comparisons were investigated. Metabolism of the material was compared for all animals and for animals which developed lung tumors. The differences in histopathology and tumor incidence in the lung were also reviewed. Although there were several differences between species, there were also many similarities. On-going research in dogs should produce data which will allow clarification of these relationships

  2. Toxicity of inhaled 239PuO2 in immature beagle dogs

    Immature beagle dogs have been exposed by inhalation to a 1.5 μm aerodynamic diameter monodisperse aerosol of 239PuO2 to compare the biological effects with those seen in young adult and aged dogs exposed to a similar aerosol. To date, 18 dogs have been exposed to the aerosol, resulting in graded initial lung burdens ranging from 0.003 to 0.38 μCi/kg body weight. Two dogs have been exposed to the aerosol diluent and serve as controls. Two of the 18 exposed animals were sacrificed 8 days after exposure to provide information on initial deposition and distribution. All other exposed animals are alive 400 days after exposure. No dogs were exposed during the past year because of an outbreak of canine parvovirus enteritis which caused death in 8 to 10 week-old dogs

  3. A comparative study of the carcinogenetic effects of 241Am, 239Pu and 237Np

    In this experiment, 420 wistar rats were used to study the comparative carcinogenetic effects of 241Am, 239Pu and 237Np. These nuclides were injected to animals intravenously, subcutaneously or directly into the lung (Stansen's lung puncture method) in doses of 1.0, 5.0 and 8.5 μCi/kg, respectively. As soluble nitrate, the nuclides were rapidly transfered from the site of injection into the bone and the liver. Osteosarcomas were found in some animals 8 months to one year after intoxication. Diagnosis of osteosarcoma is based on the histopatological examination and X-ray photography. In the Am-poisoned rats the incidence of osteosarcoma is about 31-74%, varied with different doses and different routes of intoxication; in Pu-poisoned rats, the incidence of osteosarcoma is about 55-66%. while in Np-poisoned rats, it is about 36-53%. Primary lung cancers were also found in those animals poisoned by means of Stansen's lung puncture method with the above three nuclides. The incidence of primary lung cancers is about 6% in Am-and Pu-poisoned rats and 13% in Np-poisoned rats. The incidence of metastasis of osteosarcoma in lung is about 25-65% for Am-poisoned rats, 45-55% for Pu-poisoned rats and 41-80% for Np-poisoned rats. The life-span of above poisoned rats was significantly shorter than that of the normal control animals. The chemical weight for 241Am, 239Pu and 237Np in same unit of radioactivity (1.0 μCi) equals to 0.308 μg, 15.9 μg and 1418.7 μg, respectively. For this reason, we have to pay more attention to the chemical mass effect in carcinogenesis of the above three nuclides

  4. Dosimetry and response in rat pulmonary epithelium following inhalation of 239PuO2

    The distribution of inhaled 239PuO2 and pathologic changes have been studied in the lung of rats. The clearance of inhaled 237239PuO2 from the lung is a function of the amount of deposited Pu with a decrease in early alveolar clearance with increasing lung burden. With increasing time post-exposure there is a greater concentration of PuO2 and an increased aggregation of PuO2 particles in subpleural regions of the lung. Fibrotic and metaplastic lesions in the lung were usually focal, being found in subpleural regions associated with aggregates of PuO2. An average of 12 +- 6 percent of the lung volume was fibrotic at 530 days after an initial alveolar deposition of 180 nCi 239Pu. Lung tumors occupied 4 +- 6 percent and epithelial metaplasias less than 1 percent of the lung volume at this time. Cell proliferation as assayed by tritiated thymidine autoradiography was greater in fibrotic, metaplastic and neoplastic regions than in areas of normal alveolar-bronchiolar epithelium. Turnover times ranged from about 6 days for fibrotic lesions to 1 to 3 days for metaplastic and neoplastic lesions. The lung tumor doubling times were 57 to 116 days due to tumor cell necrosis and other factors that limit tumor cell survival. Cell proliferation rates for adenomatous metaplasia were similar to those for adenocarcinoma while those for squamous cell metaplasia were similar to those for squamous cell carcinoma. Squamous lesions exhibited a more rapid growth than did adenomatous lesions

  5. Initial deposition and early clearance of inhaled 239Pu(NO3)4 aerosols in beagle dogs

    Data from exposures of 113 beagle dogs to 239Pu(NO3)4 aerosols were analyzed for effects of aerosol properties on deposition and early clearance. The percent of inhaled aerosols deposited was not significantly dependent on particle size or aerosol concentration. The early clearance rate was significantly slower at the highest exposure levels than at medium and low levels

  6. Comparison of metabolism and late effects in dogs and rats exposed to 239PuO2

    Lung tumors were observed proportionally earlier in relation to expected life span in dogs than in rats after inhalation of 239PuO2. Dogs appear to translocate a higher percentage of initial lung burden to liver, skeleton and thoracic lymph nodes than rats

  7. Experimental determination of residual nuclei formation cross sections in 660 MeV proton reactions with 239Pu and natU

    Experimental cross sections for proton induced reactions of an energy of 660 MeV with various fission products, minor actinides, and 'major' actinides (plutonium, uranium, thorium) are studied. The paper describes 239Pu and natural U experiments; other experiments have already been published or are planned. Cross section determination consist of three parts: experiment, data processing, and mathematical codes simulation of the problem. This paper deals only with experiment description and data processing methodology. 4 irradiation experiments have been performed: 2 with natural uranium targets and 2 with plutonium targets. Each two experiments were identical, differences were only in irradiation time (and of course another sample was used). Uranium samples were in the thin foil form while plutonium was in dioxide form in a duralumin container. Shorter irradiation time experiments were used to observe isotopes with half-lives in the range of minutes and hours while the longer ones were used to observe long-lived isotopes. The irradiated samples were submitted to γ spectroscopy about 5 minutes after the end of irradiation. A total number of 105 uranium spectra and 156 plutonium spectra were acquired. Measured data were processed using standard γ spectrometry methods and standard software packages as well as home-made programs were used to determine cross-sections. Neither final results of processing, nor simulation of plutonium experiment are paper-ready at the moment. Uranium data have partially already been presented, final complete results are planned to be published with plutonium results together in reviewed journal

  8. Effect of alpha irradiation of the lungs from inhaled 239PuO2 on the immunity of mice to Listeria monocytogenes

    The pulmonary clearance of inhaled Listeria monocytogenes from the lungs of nonimmunized and immunized mice was observed 3 to 4 or 26 wks after prior exposure to 239PuO2 to achieve initial lung burdens of 2.6, 5.0 and 11.9 nanocuries (nCi). Mice from 239PuO2 and sham-exposed groups were immunized against L. monocytogenes and 1 wk later challenged via the respiratory route. Pulmonary clearance was suppressed in mice with an 11.9 nCi initial lung burden of 239Pu 26 wk after 239PuO2 inhalation but not in the mice with initial lung burdens of 2.6 and 5.0 nCi at 4 to 5 or 27 wk after 239PuO2 exposure. Mice with a mean initial lung burden of 11.9 nCi of 239Pu, which were immunized against L. monocytogenes 26 wk after 239PuO2 inhalation, had a decreased survival after respiratory challenge with L. monocytogenes when compared to immunized control animals. Body weight gain and hematological differences did not correlate with suppressed pulmonary clearance or decreased survival. Pulmonary lavage studies indicated that fewer alveolar macrophages were recoverable from mice with a mean initial lung burden of 11.9 nCi of 239Pu 26 wk after 239PuO2 inhalation. It was concluded that an initial lung burden of 11.9 nCi of 239Pu which delivered approximately 700 rads of alpha radiation to the lungs of mice resulted in decreased pulmonary clearance and decreased survival of mice which had been immunized against L. monocytogenes

  9. 239Pu Prompt Fission Neutron Spectra Impact on a Set of Criticality and Experimental Reactor Benchmarks

    Peneliau, Y.; Litaize, O.; Archier, P.; De Saint Jean, C.

    2014-04-01

    A large set of nuclear data are investigated to improve the calculation predictions of the new neutron transport simulation codes. With the next generation of nuclear power plants (GEN IV projects), one expects to reduce the calculated uncertainties which are mainly coming from nuclear data and are still very important, before taking into account integral information in the adjustment process. In France, future nuclear power plant concepts will probably use MOX fuel, either in Sodium Fast Reactors or in Gas Cooled Fast Reactors. Consequently, the knowledge of 239Pu cross sections and other nuclear data is crucial issue in order to reduce these sources of uncertainty. The Prompt Fission Neutron Spectra (PFNS) for 239Pu are part of these relevant data (an IAEA working group is even dedicated to PFNS) and the work presented here deals with this particular topic. The main international data files (i.e. JEFF-3.1.1, ENDF/B-VII.0, JENDL-4.0, BRC-2009) have been considered and compared with two different spectra, coming from the works of Maslov and Kornilov respectively. The spectra are first compared by calculating their mathematical moments in order to characterize them. Then, a reference calculation using the whole JEFF-3.1.1 evaluation file is performed and compared with another calculation performed with a new evaluation file, in which the data block containing the fission spectra (MF=5, MT=18) is replaced by the investigated spectra (one for each evaluation). A set of benchmarks is used to analyze the effects of PFNS, covering criticality cases and mock-up cases in various neutron flux spectra (thermal, intermediate, and fast flux spectra). Data coming from many ICSBEP experiments are used (PU-SOL-THERM, PU-MET-FAST, PU-MET-INTER and PU-MET-MIXED) and French mock-up experiments are also investigated (EOLE for thermal neutron flux spectrum and MASURCA for fast neutron flux spectrum). This study shows that many experiments and neutron parameters are very sensitive to

  10. Evaluation of chelation concentration and cation separation of actinides at ultra-trace levels in urine matrix

    The feasibility of measuring picogram levels of actinides in a urine matrix using ion chromatography coupled on-line to an inductively coupled plasma quadrupole mass spectrometer (IC-Q-ICPMS) was investigated. A chelation column for separation of matrix ions and preconcentration of the actinides was combined with a cation-exchange column for separation of the actinides. Sample preparation required simple addition of ammonium acetate to adjust the pH of the urine matrix. Spike solutions containing 232Th, 237Np, 238U, 239Pu, and 241Am were added to undiluted urine, diluted urine (1 : 9) and water. This approach enhanced the signal sensitivities of all the tested actinides over two orders of magnitude in the water matrix, while certain elements (especially Am) can still be effectively concentrated in undiluted urine. (author)

  11. Incidence of liver tumors in beagles with body burdens of 239Pu or 241Am

    Tetravalent 239Pu or trivalent 241Am in a citrate buffer, given via a single intravenous injection to beagles, induced very pronounced liver changes, usually at relatively long postinjection times. The lesions consisted of cell injury or cell necrosis which was followed by nodular hyperplasia and a significant incidence of primary liver tumors. The most frequent neoplasm was the bile duct adenoma, followed by the bile duct carcinoma. A lesser number of sarcomas were also induced, especially fibrosarcomas. The number of hepatic cell tumors was low. An abnormally high incidence of both hyperplastic nodules and primary liver tumors occurred at long postinjection times and at average doses extending down to ∼10 rads. The various nodular lesions and liver tumors frequently occurred as incidental findings in dogs dying from other causes, especially bone cancer. In comparison to bone neoplasia, the liver was a much less important target organ in the high-dose level groups, but in some of the low-dose groups, especially in the 241Am groups, the risk of radiation-induced liver cancer was approximately equal to or exceeded the risk of skeletal tumors. However, in any projection of the risks observed in this animal model to man, one should be mindful that the beagle skeleton is approximately 25 times more sensitive to radiation-induced bone neoplasia than is the human skeleton (Mays et al., 1976) and that the radiosensitivity difference for the beagle and human liver is unknown. 41 refs., 8 figs., 5 tabs

  12. Evaluation of the thermal cross sections of 239Pu and 241Pu

    The thermal neutron cross sections of the isotopes 239Pu and 241Pu have been evaluated in the thermal neutron energy region below 1.0 eV. The method of evaluation fitted energy-dependent data constrained by a modified Adler-Adler multilevel resonance fission and capture formalism and multilevel Breit-Wigner scattering theory. The energy dependence of the number of neutrons per fission was prescribed in the theory by introducing nu as fitted resonance spin-dependent values. The data were fitted in a resonance parameter fitting code, RPFC, using the method of maximum likelihood. The code fits simultaneously the total and partial energy-dependent cross section data to the theory. The types of data explicitly fitted are total, fission, capture, total scattering, coherent scattering, and absorption cross sections plus the quantities alpha, total nu and eta. Relative energy-dependent data with precision errors are fitted along with absolute values and errors at chosen energies. RPFC also allows energy-scale adjustment and Doppler broadening of selected data sets, and fits correlated data of two isotopes simultaneously. Reference experimental data bases of original data plus condensed and modified data were assembled for the evaluation for each isotope. 19 figures, 9 tables

  13. Effects of the herbicide glyphosate on the uptake of 239Pu and 241Am to vegetation

    Glyphosate (n-phosphonomethyl glycine) is a broad spectrum herbicide widely used in lowland agriculture, forestry and improved upland pastures. Although its metal chelating properties are well established, its interaction with radionuclides remains unknown. A pot experiment was conducted to determine the effect of soil applications of glyphosate on the uptake of 239Pu and 241Am to peas and carrots grown in loam, peat and sand soils. Soil-to-plant transfer factors were calculated for treated and untreated soils at harvest. The most marked effect was an increase in 241Am uptake to crops grown in loam soil. Supplementary laboratory batch experiments were conducted by shaking radiolabelled soil and its associated soil solution with glyphosate. The activity concentration of 241Am increased ten fold in the liquid phase of loam soils treated with glyphosate. It is postulated that this 241Am desorption could have been mediated by the formation of a stable Am-glyphosate complex which was subsequently more available for crop uptake than Am alone. (author)

  14. Photofission product yields of 238U and 239Pu with 22-MeV bremsstrahlung

    Wen, Xianfei; Yang, Haori

    2016-06-01

    In homeland security and nuclear safeguards applications, non-destructive techniques to identify and quantify special nuclear materials are in great demand. Although nuclear materials naturally emit characteristic radiation (e.g. neutrons, γ-rays), their intensity and energy are normally low. Furthermore, such radiation could be intentionally shielded with ease or buried in high-level background. Active interrogation techniques based on photofission have been identified as effective assay approaches to address this issue. In designing such assay systems, nuclear data, like photofission product yields, plays a crucial role. Although fission yields for neutron-induced reactions have been well studied and readily available in various nuclear databases, data on photofission product yields is rather scarce. This poses a great challenge to the application of photofission techniques. In this work, short-lived high-energy delayed γ-rays from photofission of 238U were measured in between linac pulses. In addition, a list-mode system was developed to measure relatively long-lived delayed γ-rays from photofission of 238U and 239Pu after the irradiation. Time and energy information of each γ-ray event were simultaneously recorded by this system. Cumulative photofission product yields were then determined using the measured delayed γ-ray spectra.

  15. Pulmonary retention and tissue distribution of 239Pu nitrate in F344 rats and syrian hamsters inhaling carbon tetrachloride

    Carbon tetrachloride (CCl4) has been used extensively in the nuclear weapons industry, so it is possible that nuclear plant workers have been exposed to CCl4 and plutonium compounds. Potential for future exposure exists during open-quotes cleanupclose quotes operations at weapon production sites such as the Hanford, Washington, and Rocky Flats, Colorado, facilities. The current Threshold Limit Value for CCl4 is 5 ppm; however, concentrations of CCl4 occurring in the nuclear weapons facilities over the past 40-50 y are unknown and may have exceeded this value. The pilot study described in this report is designed to determine whether subchronic inhalation of CCl4 by CDFregister(F-344)/CrlBR rats and Syrian golden hamsters, at concentrations expected to produce some histologic changes in liver, alters the hepatic retention and toxic effects of inhaled 239Pu nitrate 239Pu(NO3)4

  16. Study of neutron-deficient isotopes of Fl in the 239Pu, 240Pu + 48Ca reactions

    Voinov, A. A.; Utyonkov, V. K.; Brewer, N. T.; Oganessian, Yu Ts; Rykaczewski, K. P.; Abdullin, F. Sh; Dmitriev, S. N.; Grzywacz, R. K.; Itkis, M. G.; Miernik, K.; Polyakov, A. N.; Roberto, J. B.; Sagaidak, R. N.; Shirokovsky, I. V.; Shumeiko, M. V.; Tsyganov, Yu S.; Subbotin, V. G.; Sukhov, A. M.; Sabelnikov, A. V.; Vostokin, G. K.; Hamilton, J. H.; Stoyer, M. A.; Strauss, S. Y.

    2016-07-01

    The results of the experiments aimed at the synthesis of Fl isotopes in the 239Pu + 48Ca and 240Pu + 48Ca reactions are presented. The experiment was performed using the Dubna gas-filled recoil separator at the U400 cyclotron. In the 239Pu+48Ca experiment one decay of spontaneously fissioning 284Fl was detected at 245-MeV beam energy. In the 240Pu+48Ca experiment three decay chains of 285Fl were detected at 245 MeV and four decays were assigned to 284Fl at the higher 48Ca beam energy of 250 MeV. The α-decay energy of 285Fl was measured for the first time and decay properties of its descendants 281Cn, 277Ds, 273Hs, 269Sg, and 265Rf were determined more precisely. The cross section of the 239Pu(48Ca,3n)284Fl reaction was observed to be about 20 times lower than those predicted by theoretical models and 50 times less than the value measured in the 244Pu+48Ca reaction. The cross sections of the 240Pu(48Ca,4-3n)284,285Fl at both 48Ca energies are similar and exceed that observed in the reaction with lighter isotope 239Pu by a factor of 10. The decay properties of the synthesized nuclei and their production cross sections indicate rapid decrease of stability of superheavy nuclei with departing from the neutron number N=184 predicted to be the next magic number.

  17. Probing energy dissipation, γ-ray and neutron multiplicity in the thermal neutron-induced fission of 239Pu

    Pahlavani, M. R.; Mirfathi, S. M.

    2016-04-01

    The incorporation of the four-dimensional Langevin equations led to an integrative description of fission cross-section, fragment mass distribution and the multiplicity and energy distribution of prompt neutrons and γ-rays in the thermal neutron-induced fission of 239Pu. The dynamical approach presented in this paper thoroughly reproduces several experimental observables of the fission process at low excitation energy.

  18. Extrapolation to man of the relation between activity and damage to organism of laboratory animals internally contaminated with 239Pu

    The relations were analyzed between the initial amount of the radionuclide deposited and mortality. The mortality curves were analyzed using the Gompaertz relation and the exponential relation was found between the rate of the mortality changes and 239Pu activity. Using comparative analysis the results of the model were approximated to man and compared with data published in the literature on human contamination. The comparison did not exclude the validity of the applied model. (author)

  19. Estimation of uncertainties in resonance parameters of {sup 56}Fe, {sup 239}Pu, {sup 240}Pu and {sup 238}U

    Nakagawa, Tsuneo; Shibata, Keiichi [Japan Atomic Energy Research Inst., Tokai, Ibaraki (Japan). Tokai Research Establishment

    1997-05-01

    Uncertainties have been estimated for the resonance parameters of {sup 56}Fe, {sup 239}Pu, {sup 240}Pu and {sup 238}U contained in JENDL-3.2. Errors of the parameters were determined from the measurements which the evaluation was based on. The estimated errors have been compiled in the MF32 of the ENDF format. The numerical results are given in tables. (author)

  20. Comparison of evaluations for 235U, 239Pu, 240Pu, 241Pu and 242Pu with integral measurements

    The evaluations for 235U, 239Pu, 240Pu, 241Pu and 242Pu are considered. Intercomparison is made of the neutron cross section data from INDL/A, ENDL-84, ENDF/B-5 and ENDF/B-6 (where applicable). Integral measurements of the spectrum averaged cross sections are compared to the values derived from evaluated data libraries. (author). 40 refs, 49 figs, 11 tabs

  1. Determination of 240Pu/239Pu isotope ratios in Kara Sea and Novaya Zemlya sediments using accelerator mass spectrometry

    Accelerator mass spectrometry (AMS) has been used to determine Pu activity concentrations and 240Pu/239Pu isotope ratios in sediments from the Kara Sea and radioactive waste dumping sites at Novaya Zemlya. Measured 239,240Pu activities ranged from 0.06 - 9.8 Bq/kg dry weight, 240Pu/239Pu atom ratios ranged from 0.13 to 0.28, and 238Pu/239,240Pu activity ratios from 0.02 to 0.6. Perturbations from global fallout isotope ratios were evident at three sites: the Yenisey Estuary and Abrosimov Fjords where 240Pu/239Pu ratios were lower (0.13-0.14); and Stepovogo Fjord sediments where ratios were higher (up to 0.28) than fallout ratios. Based on procedural blanks, detection limits for AMS were below 1 fg Pu and the method showed good precision for isotope ratio measurements, minimal matrix, interference and memory effects. For high level samples, comparison between alpha spectrometry and AMS gave good agreement for measurement of 239,240Pu activity concentrations. (author)

  2. Fission Product Yields for 14 MeV Neutrons on 235U, 238U and 239Pu

    Mac Innes, M.; Chadwick, M. B.; Kawano, T.

    2011-12-01

    We report cumulative fission product yields (FPY) measured at Los Alamos for 14 MeV neutrons on 235U, 238U and 239Pu. The results are from historical measurements made in the 1950s-1970s, not previously available in the peer reviewed literature, although an early version of the data was reported in the Ford and Norris review. The results are compared with other measurements and with the ENDF/B-VI England and Rider evaluation. Compared to the Laurec (CEA) data and to ENDF/B-VI evaluation, good agreement is seen for 235U and 238U, but our FPYs are generally higher for 239Pu. The reason for the higher plutonium FPYs compared to earlier Los Alamos assessments reported by Ford and Norris is that we update the measured values to use modern nuclear data, and in particular the 14 MeV 239Pu fission cross section is now known to be 15-20% lower than the value assumed in the 1950s, and therefore our assessed number of fissions in the plutonium sample is correspondingly lower. Our results are in excellent agreement with absolute FPY measurements by Nethaway (1971), although Nethaway later renormalized his data down by 9% having hypothesized that he had a normalization error. The new ENDF/B-VII.1 14 MeV FPY evaluation is in good agreement with our data.

  3. Fission Product Yields for 14 MeV Neutrons on 235U, 238U and 239Pu

    We report cumulative fission product yields (FPY) measured at Los Alamos for 14 MeV neutrons on 235U, 238U and 239Pu. The results are from historical measurements made in the 1950s–1970s, not previously available in the peer reviewed literature, although an early version of the data was reported in the Ford and Norris review. The results are compared with other measurements and with the ENDF/B-VI England and Rider evaluation. Compared to the Laurec (CEA) data and to ENDF/B-VI evaluation, good agreement is seen for 235U and 238U, but our FPYs are generally higher for 239Pu. The reason for the higher plutonium FPYs compared to earlier Los Alamos assessments reported by Ford and Norris is that we update the measured values to use modern nuclear data, and in particular the 14 MeV 239Pu fission cross section is now known to be 15–20% lower than the value assumed in the 1950s, and therefore our assessed number of fissions in the plutonium sample is correspondingly lower. Our results are in excellent agreement with absolute FPY measurements by Nethaway (1971), although Nethaway later renormalized his data down by 9% having hypothesized that he had a normalization error. The new ENDF/B-VII.1 14 MeV FPY evaluation is in good agreement with our data.

  4. First measurements of 236U concentrations and 236U/239Pu isotopic ratios in a Southern Hemisphere soil far from nuclear test or reactor sites

    The variation of the 236U and 239Pu concentrations as a function of depth has been studied in a soil profile at a site in the Southern Hemisphere well removed from nuclear weapon test sites. Total inventories of 236U and 239Pu as well as the 236U/239Pu isotopic ratio were derived. For this investigation a soil core from an undisturbed forest area in the Herbert River catchment (17°30′ – 19°S) which is located in north-eastern Queensland (Australia) was chosen. The chemical separation of U and Pu was carried out with a double column which has the advantage of the extraction of both elements from a relatively large soil sample (∼20 g) within a day. The samples were measured by Accelerator Mass Spectrometry using the 14UD pelletron accelerator at the Australian National University. The highest atom concentrations of both 236U and 239Pu were found at a depth of 2–3 cm. The 236U/239Pu isotopic ratio in fallout at this site, as deduced from the ratio of the 236U and 239Pu inventories, is 0.085 ± 0.003 which is clearly lower than the Northern Hemisphere value of ∼0.2. The 236U inventory of (8.4 ± 0.3) × 1011 at/m2 was more than an order of magnitude lower than values reported for the Northern Hemisphere. The 239Pu activity concentrations are in excellent agreement with a previous study and the 239+240Pu inventory was (13.85 ± 0.29) Bq/m2. The weighted mean 240Pu/239Pu isotopic ratio of 0.142 ± 0.005 is slightly lower than the value for global fallout, but our results are consistent with the average ratio of 0.173 ± 0.027 for the southern equatorial region (0–30°S). - Highlights: • Exploration of uranium-236 (236U) and plutonium-239 (239Pu) in the Southern Hemisphere by accelerator mass spectrometry. • We report the depth profile for both isotopes from a forest site well removed from nuclear test or reactor sites. • 236U and 239Pu were deposited at the same time due to nuclear weapons tests but show a slightly different depth dependence. • The

  5. Simultaneous evaluation for (n,f) cross section of 235U, 239Pu, 238U and (n,γ) cross sections of 238U

    The fission cross sections for 235U, 238U, 239Pu, the capture cross sections for 238U and the ratios for 239Pu(n,f)/235U(n,f), 238U(m,f)/235U(n,f), 238U(n,γ)/235U(n,f) were firstly evaluated respectively. The experimental data were collected, analysed, selected and corrected. The data were fitted with spline fit program

  6. The absolute total delayed neutron yields, relative abundances and half-lives of delayed neutron groups in 6- and 8-group model format from neutron induced fission of 232Th, 233U, 236U, 239Pu, and 241Am in the energy range from 0.35 MeV (or threshold energy) to 5 MeV

    The latest evaluation of delayed neutron constants was made for main fuel nuclides (235U, 238U, 239Pu) within an working group under the auspices of the Nuclear Energy Agency’s (NEA) Working Party on International Evaluation Cooperation (WPEC), Subgroup 6 (SG6) in 1999 [1]. As a result of this work the total delayed yields for the above nuclides were essentially corrected as compared with Tuttle’s recommended data set [2]. For the total delayed yields from 238U correction is +5.6%, for thermal induced fission of 239Pu - +3.4% and for fast neutron induced fission of 239Pu - +3.2%. This is a direct indication that there is a need for a continuing effort on delayed neutron data improving. From now, this will be mainly directed at satisfying new requirements emerging from the current trends in reactor technology, such as: the use of high burn-up fuel, the burning of plutonium stocks, the general growing interest in fuel recycling strategies, and new concept of actinide burners

  7. Study of delayed neutron decay curves from thermal neutron induced fission of 235U and 239Pu

    The results of measurements of decay curves for delayed neutrons, obtained in the thermal neutron induced fission of 235U and 239Pu, are presented. The data were obtained by the periodical irradiation method on the IBR-2 pulsed reactor in the time interval from 5 to 730 msec after the end of irradiation. The comparison of the measured curves with the curves calculated with using several known from literature parameter sets (relative weights and half-lives of 6 or 8 exponents) was carried out. The new 7-group parameter set, which describes experimental data better, is proposed. (author)

  8. Reactor Decay Heat in 239Pu: Solving the γ Discrepancy in the 4-3000-s Cooling Period

    The β feeding probability of 102,104,105,106,107Tc, 105Mo, and 101Nb nuclei, which are important contributors to the decay heat in nuclear reactors, has been measured using the total absorption technique. We have coupled for the first time a total absorption spectrometer to a Penning trap in order to obtain sources of very high isobaric purity. Our results solve a significant part of a long-standing discrepancy in the γ component of the decay heat for 239Pu in the 4-3000 s range.

  9. Reactor decay heat in 239Pu: solving the γ discrepancy in the 4-3000-s cooling period.

    Algora, A; Jordan, D; Taín, J L; Rubio, B; Agramunt, J; Perez-Cerdan, A B; Molina, F; Caballero, L; Nácher, E; Krasznahorkay, A; Hunyadi, M D; Gulyás, J; Vitéz, A; Csatlós, M; Csige, L; Aysto, J; Penttilä, H; Moore, I D; Eronen, T; Jokinen, A; Nieminen, A; Hakala, J; Karvonen, P; Kankainen, A; Saastamoinen, A; Rissanen, J; Kessler, T; Weber, C; Ronkainen, J; Rahaman, S; Elomaa, V; Rinta-Antila, S; Hager, U; Sonoda, T; Burkard, K; Hüller, W; Batist, L; Gelletly, W; Nichols, A L; Yoshida, T; Sonzogni, A A; Peräjärvi, K

    2010-11-12

    The β feeding probability of (102,104,105,106,107)Tc, 105Mo, and 101Nb nuclei, which are important contributors to the decay heat in nuclear reactors, has been measured using the total absorption technique. We have coupled for the first time a total absorption spectrometer to a Penning trap in order to obtain sources of very high isobaric purity. Our results solve a significant part of a long-standing discrepancy in the γ component of the decay heat for 239Pu in the 4-3000 s range. PMID:21231223

  10. Energy dependence of mass, charge, isotopic, and energy distributions in neutron-induced fission of 235U and 239Pu

    Pasca, H.; Andreev, A. V.; Adamian, G. G.; Antonenko, N. V.; Kim, Y.

    2016-05-01

    The mass, charge, isotopic, and kinetic-energy distributions of fission fragments are studied within an improved scission-point statistical model in the reactions 235U+n and 239Pu+n at different energies of the incident neutron. The charge and mass distributions of the electromagnetic- and neutron-induced fission of 214,218Ra, 230,232,238U are also shown. The available experimental data are well reproduced and the energy-dependencies of the observable characteristics of fission are predicted for future experiments.

  11. Retention, distribution, and excretion of 239PuO2 particles labeled with 169Yb in the Rhesus monkey after a single acute inhalation exposure

    Sixteen Rhesus monkeys were exposed to a high fired 239PuO2 aerosol labeled with 169Yb, and retention, distribution, and excretion patterns were determined. After an early rapid clearance phase, which had a half-life of less than one day, the remaining plutonium was retained in the lungs with a half-life that appeared to be greater than 500 days. By 30 days after exposure, 99 percent of the 239Pu in the body was in the lungs. At this time, 6 to 10 percent of the 169Yb burden was in the carcass and skeleton suggesting that there was dissociation of some 169Yb from the particles. The remaining 169Yb activity was in the lungs. There was little 239Pu in the liver, bone, or lymph nodes. The particulate material was cleared rapidly from the gastrointestinal and upper respiratory tracts and appeared in feces over the first four days. The level of 239Pu in feces returned to background by six days. Urinary excretion of 239Pu reached a peak by 8 to 10 days and then remained at a constant rate throughout the remainder of the experiment. These data are useful in calculating radiation dose to a variety of organs and relating this dose to the appearance of late effects from inhaled alpha-emitting particles. (U.S.)

  12. Synthesis and study of 239Pu-doped ceramics based on zircon, (Zr,Pu)Sio4, and hafnon, (Hf,Pu)SiO4

    Zircon, ZrSiO4, as well as its Hf-analogue hafnon, HfSiO4, have been proposed for use as durable Pu host phases for the immobilization of weapons grade Pu and other actinides. Four samples of Pu-doped ceramics based on the zircon and hafnon structures were synthesized through sintering in air using precursors containing 5-6 and 10 wt% 239Pu. Synthesized ceramic samples were studied by X-ray powder diffraction (XRD), scanning electron microscopy (SEM), microprobe method, MCC-1 leach test at 25 and 90 deg C. Inclusions of separated a PuO2 phase in the matrix of zircon-based ceramic and presumably, (Pu,Hf)O2 phase in the hafnon-based ceramic were observed for samples obtained from precursors doped with 10 wt% Pu. No separated Pu-phases in significant amounts were identified in the matrices of both ceramics obtained from the precursors doped with 5-6 wt% Pu. It was found that normalized Pu mass losses (without correction on ceramic porosity) for samples doped with 10 wt% Pu which contain separated inclusions of PuO2 or (Pu1Hf)O2 after 14/28 days were approximately (in g/m2) - for zircon: 0.2/0.2 - at 90 deg C and 0.03/0.04 - at 25 deg C and for hafnon: 0.02/0.04 - at 90 deg C and 0.01/0.01 - at 25 deg C. The losses of Pu from samples doped with 5-6 wt% are 1-2 order of magnitude less. It was suggested that optimal amount of Pu which could be incorporated by zircon and hafnon lattices does not exceed 7 wt%. An important additional conclusion is that Pu-doped ceramic based on zircon or hafnon can be successfully fabricated excluding hot pressing method. Copyright (2001) Material Research Society

  13. Determination of long-lived actinides in soil leachates by inductively coupled plasma: Mass spectrometry

    Inductively coupled plasma -- mass spectrometry (ICP-MS) was used to concurrently determine multiple long-lived (t1/2 > 104 y) actinide isotopes in soil samples. Ultrasonic nebulization was found to maximize instrument sensitivity. Instrument detection limits for actinides in solution ranged from 50 mBq L-1 (239Pu) to 2 μBq L-1 (235U) Hydride adducts of 232Th and 238U interfered with the determinations of 233U and 239 Pu; thus, extraction chromatography was, used to eliminate the sample matrix, concentrate the analytes, and separate uranium from the other actinides. Alpha spectrometric determinations of 230Th, 239Pu, and the 234U/238U activity ratio in soil leachates compared well with ICP-MS determinations; however, there were some small systematic differences (ca. 10%) between ICP-MS and a-spectrometric determinations of 234U and 238U activities

  14. Toxicity of inhaled 239PuO2 in immature, young adult and aged Syrian hamsters. V

    Human populations that might be exposed in the event of a catastrophic nuclear accident would include individuals with widely differing ages. To obtain better information on the possible effects of age on observed dose-response relationships for inhaled 239PuO2, groups of Syrian hamsters were exposed via inhalation at either 28 (immature), 84 (young adults) or 340 (aged) days of age to polydisperse aerosols of 239PuO2. The projected graded levels of initial lung burden were 240, 60, 15, 3.8, 0.95, 0.25 and 0.029 nCi for the immature and young adult animals and 240, 60, 15 and 3.8 nCi for the aged animals. Additional animals were included in the 60 nCi initial lung burden level for serial sacrifice to determine the radiation dose pattern. All other animals were maintained for life span observation. For all age groups, less than 1% of the sacrifice body burden was found in all tissues other than lung. Mortality data analysis indicated significant life shortening only in animals that received the highest level inital lung burden. These early deaths were related to radiation pneumonitis and pulmonary fibrosis. No pulmonary neoplasms were observed

  15. The induction of nuclear abnormalities in the alveolar macrophages of mouse lung after inhalation of 239PuO2

    Effects of inhaled 239PuO2 on the free-cell population of the lungs of CBA/H mice have been studied using broncho-alveolar lavage following initial alveolar depositions (IADs) of 209 to 2800 Bq. The numbers of pulmonary alveolar macrophages (PAM) were quantified using a radioactive tracer technique. The number of PAM declined soon after exposure; the extent of the depression and the time taken to reach the nadir were both dose-dependent. Numbers eventually returned to normal but, with high IADs, only after 3 months. The number of binucleate PAM and those with micronuclei increased following relatively low IADs in a dose-dependent manner. Micronucleate PAM were the most sensitive indicator of cellular damage as a result of 239PuO2 inhalation, providing a short-term assessment of radiation damage to lung cells at doses known to produce lung tumors. The results also provide further evidence that mitosis in PAM, or in their precursor cells, does occur within the lung. (author)

  16. Mass Yields and Average Total Kinetic Energy Release in Fission for 235U, 238U, and 239Pu

    Duke, Dana

    2015-10-01

    Mass yield distributions and average total kinetic energy (TKE) in neutron induced fission of 235U, 238U, and 239Pu targets were measured with a gridded ionization chamber. Despite decades of fission research, our understanding of how fragment mass yields and TKE depend on incident neutron energy is limited, especially at higher energies (above 5-10 MeV). Improved accuracy in these quantities is important for nuclear technology as it enhances our simulation capabilities and increases the confidence in diagnostic tools. The data can also guide and validate theoretical fission models where the correlation between the fragment mass and TKE is of particular value for constraining models. The Los Alamos Neutron Science Center - Weapons Neutron Research (LANSCE - WNR) provides a neutron beam with energies from thermal to hundreds of MeV, well-suited for filling in the gaps in existing data and exploring fission behavior in the fast neutron region. The results of the studies on target nuclei 235U, 238U, and 239Pu will be presented with a focus on exploring data trends as a function of neutron energy from thermal through 30 MeV. Results indicate clear evidence of structure due to multi-chance fission in the TKE . LA-UR-15-24761.

  17. Investigation of resonance structure and Doppler-effect of cross sections for 232 Th, 235 U and 239 Pu

    The results of measuring the neutron transmissions for 232 Th, 235 U and 239 Pu metal samples carried out at the 60 m, 123 m and 1006 m flight paths of the Dubna IBR-30 booster in the neutron energy range of 2 eV - 200 keV are given and discussed. The measurements were made at the room and liquid nitrogen temperatures. The batteries of 3 boron and 26 helium counters were used as detectors. The results of the calculations of analogous transmissions realized on the base of the evaluated data libraries BROND-2, ENDF/B-6 and JENDL-3 by means of the GRUCON computer program package are also given. It is concluded that the 235 U Doppler coefficients and effective total cross sections taken from measured transmissions are in a good agreement with calculation results based on the ENDF/B-6 library at energies of 2.15 eV - 200 keV. The BROND-2 and JENDL-3 parameters give the Doppler coefficients and effective cross sections which are 10-30% higher than the experimental and ENDF/B-6 ones at the resonance energies of 46.5 - 465 eV. For 239 Pu there is agreement of the experimental and calculational results within the experimental error limits. For 232 Th experimental values for the Doppler coefficients and effective cross sections are 10-15% higher than the calculated ones with all libraries in resonance energy region. 9 refs., 2 tabs., 1 fig

  18. Measurement of 239Pu in urine samples at ultra-trace levels using a 1 MV compact AMS system

    Routine bioassay monitoring of Pu intake in exposed workers of research and nuclear industry is usually performed by alpha spectrometry. This technique involves large sample volumes of urine and time-consuming preparative and counting protocols. Compact accelerator mass spectrometry (AMS) facilities make feasible the determination of ultra low-level Pu activity concentrations and Pu isotopic ratios in biological samples (blood, urine and feces), being a rapid and cost-effective measurement technique. The plutonium results in urine samples presented here have been obtained on the 1 MV compact AMS system sited at the Centro Nacional de Aceleradores (CNA), in Seville, Spain. In this work, a different methodological approach has been developed alternative to the 'classical' preparation of urine samples for alpha spectrometry. The procedure avoids the Pu precipitation step, and involves acid sample evaporation and acid digestion in a microwave oven. Finally, purification of plutonium was achieved by using chromatography columns filled up with BioRad AG1X2 anion exchange resin (Bio-Rad Laboratories Inc.). The total time needed for analysis is about 10 h, unlike the 'classical' methods based on alpha spectrometry which need about 1 week. At present, it has been demonstrated that this method allows quantifying 239Pu activity concentrations in urine of, at least, 30 μBq (13 fg 239Pu). We can conclude that the procedure would be suitable to perform in vitro routine bioassay measurements. Moreover, the innovative application of AMS opens new and interesting analytical alternatives in this field.

  19. Nuclear data evaluation for 239Pu in the energy region 100 075. ev - 15 MeV

    The present work incorporates the results of the new nuclear data evaluation for 239Pu. The complete file compiled by the authors in 1974 was practically completely re-examined. The most substantial changes were made above 0.5 keV. In the region of unresolved resonances (0.3-100 keV), the channel contribution to the process widths for a given state and some other aspects were taken into account. The fission cross section and the α-value were evaluated with regard for the correlation of experimental errors. The non-spherical potential with optimized parameters was used to make calculations by the optical and statistical models. The contribution of pre-equilibrium emission was taken into account in calculations of secondary neutron spectra. The new standard anti nusub(sp)(252Csub(f)) was used to calculate anti nusub(p). The 26-group constants and g-Westcott factors were obtained from the evaluated data. The complete file of the evaluated data for 239Pu is presented in the ENDF/B format and conveyed to the Nuclear Data Section of the IAEA. (author)

  20. Inhaled 239PuO2 and/or total-body gamma radiation: Early mortality and morbidity in rats and dogs

    Rats and beagle dogs were given doses of 60Co gamma radiation and/or body burdens of 239PuO2 within lethal ranges in an experiment to determine and compare morbidity and mortality responses of both species within 1 year after exposure. Radiation-induced morbidity was assessed by measuring changes in body weights, hematologic parameters, and pulmonary-function parameters. Gamma radiation caused transient morbidity, reflected by immediately depressed blood cell concentrations and by long-term loss of body weight and diminished pulmonary function in animals of both species that survived the acute gamma radiation syndrome. Inhaled plutonium caused a loss of body weight and diminished pulmonary function in both species, but its only effect on blood cell concentrations was lymphocytopenia in dogs. Combined gamma irradiation and plutonium lung burdens were synergistic, in that animals receiving both radiation insults had higher morbidity and mortality rates than would be predicted based on the effect of either kind of radiation alone. Plutonium lung burdens enhanced the effect of gamma radiation in rats within the first 30 days of exposure, and gamma radiation enhanced the long-term effect of plutonium lung burdens in both species. Rats were less sensitive to both kinds of radiation, whether administered alone or in combination. 71 refs., 105 figs., 48 tabs

  1. Inhaled /sup 239/PuO/sub 2/ and/or total-body gamma radiation: Early mortality and morbidity in rats and dogs

    Filipy, R.E.; Decker, J.R.; Lai, Y.L.; Lauhala, K.E.; Buschbom, R.L.; Hiastala, M.P.; McGee, D.R.; Park, J.F.; Kuffel, E.G.; Ragan, H.A.; Cannon, W.C.; Yaniv, S.S.; Scott, B.R.

    1988-08-01

    Rats and beagle dogs were given doses of /sup 60/Co gamma radiation and/or body burdens of /sup 239/PuO/sub 2/ within lethal ranges in an experiment to determine and compare morbidity and mortality responses of both species within 1 year after exposure. Radiation-induced morbidity was assessed by measuring changes in body weights, hematologic parameters, and pulmonary-function parameters. Gamma radiation caused transient morbidity, reflected by immediately depressed blood cell concentrations and by long-term loss of body weight and diminished pulmonary function in animals of both species that survived the acute gamma radiation syndrome. Inhaled plutonium caused a loss of body weight and diminished pulmonary function in both species, but its only effect on blood cell concentrations was lymphocytopenia in dogs. Combined gamma irradiation and plutonium lung burdens were synergistic, in that animals receiving both radiation insults had higher morbidity and mortality rates than would be predicted based on the effect of either kind of radiation alone. Plutonium lung burdens enhanced the effect of gamma radiation in rats within the first 30 days of exposure, and gamma radiation enhanced the long-term effect of plutonium lung burdens in both species. Rats were less sensitive to both kinds of radiation, whether administered alone or in combination. 71 refs., 105 figs., 48 tabs.

  2. Plutonium concentration and 240Pu/239Pu atom ratio in biota collected from Amchitka Island, Alaska: recent measurements using ICP-SFMS

    Three underground nuclear tests, including the Unites States' largest, were conducted on Amchitka Island, Alaska. Monitoring of the radiological environment around the island is challenging because of its remote location. In 2008, the Department of Energy (DOE) Office of Legacy Management (LM) became responsible for the long term maintenance and surveillance of the Amchitka site. The first DOE LM environmental survey occurred in 2011 and is part of a cycle of activities that will occur every 5 years. The University of Alaska Fairbanks, a participant in the 2011 study, provided the lichen (Cladonia spp.), freshwater moss (Fontinalis neomexicanus), kelp (Eualaria fistulosa) and horse mussel (Modiolus modiolus) samples from Amchitka Island and Adak Island (a control site). These samples were analyzed for 239Pu and 240Pu concentration and 240Pu/239Pu atom ratio using inductively coupled plasma sector field mass spectrometry (ICP-SFMS). Plutonium concentrations and 240Pu/239Pu atom ratios were generally consistent with previous terrestrial and marine studies in the region. The 239+240Pu levels (mBq kg−1, dry weight) ranged from 3.79 to 57.1 for lichen, 167–700 for kelp, 27.9–148 for horse mussel, and 560–573 for moss. Lichen from Adak Island had higher Pu concentrations than Amchitka Island, the difference was likely the result of the higher precipitation at Adak compared to Amchitka. The 240Pu/239Pu atom ratios were significantly higher in marine samples compared to terrestrial and freshwater samples (t-test, p 240Pu/239Pu ratios in terrestrial samples are within the range of global fallout. • Elevated 240Pu/239Pu in marine samples was characteristic of North Pacific Ocean. • Potential sources of enriched Pu to the marine environment regionally are suggested. • Pu ratios cannot by themselves explain the enriched Pu in seawater around Amchitka

  3. Statistical Tests for the Detection of Intermediate Structures in the Fission Cross-Sections of 235U and 239Pu

    The existence of intermediate structures in the neutron-induced fission cross sections of 235U and 239Pu was pointed out in 1957 by Egelstaff. An interpretation, recently proposed by Cao et al. and Blons et al., was based on the Strutinsky calculations of the deformation energies of the compound nucleus when shell effects are included in the liquid-drop model. The theoretical interpretation in terms of current reaction theories has been given by Weigmann and Lynn. The purpose of this paper is to develop and evaluate various statistical tests intended for the detection and interpretation of these narrow intermediate fission structures. A fission cross-section was computed in the interval 0-5 keV using randomly generated parameters with distributions chosen to mock up the 235U nucleus. The Jπ = 4- state fission width was ''modulated'' in the manner suggested by Weigmann's work. Auto-correlation and cumulative average tests were done on these mock-up cross-sections to determine if the correct average spacing of the shape isomer levels could be obtained by such tests. It is shown that the usual correlation tests tend to overestimate the spacing between structures. A proposed technique is based on the direct analysis of the averaged cross-section which affords a method of correcting for peaks of the intermediate structure below the detectability limit of the usual statistical tests. The techniques developed on the basis of the mock-up cross-sections were used to analyse the fission cross-sections of 235U and 239Pu. Average spacings of 227 and 312 eV were found for those two nuclei, respectively. These values are somewhat lower than the ones reported by Cao and Blons, which were based only on the auto-correlation analysis. The energy of the second minimum in the fission barrier was found to be 3.1 MeV for 235U and 2.9 for 239Pu. Both values are in close agreement with the values of 3 MeV predicted by Strutinsky. (author)

  4. Transfer and translocation of {sup 241}Am, {sup 239}Pu, {sup 137}Cs and {sup 85}Sr after partial foliar contamination of bean plants

    Henner, P.; Colle, C.; Morello, M. [CEA Cadarache (DEI/SECRE/LRE), Laboratory of Radioecology and Ecotoxicology, Institute for Radioprotection and Nuclear Safety, 13 - Saint-Paul-lez-Durance (France)

    2004-07-01

    Bean plants at the flowering development stage were contaminated by soaking their two first leaves for 3 hours in a solution containing one of the actinides {sup 241}Am or {sup 239}Pu, or both {sup 137}Cs and {sup 85}Sr. The aim of the study was to assess the adequacy of using the values of Cs/Sr for the foliar transfer parameters of transuranic actinides, as used for example in the ASTRAL code to calculate the contamination of agricultural products after a nuclear accident. Secondly, these experiments were launched to tentatively determine specific values for the foliar transfer parameters for Am and Pu, despite technical limitations due to high radiotoxicity of these isotopes which prevented the contamination of the whole foliage of bean plants. Cs and Sr were used to compare the results with those obtained with other modes of contamination, by dry deposition of aerosols for example. Results showed that the soaking protocol was adequate to compare the foliar transfer of various radionuclides, although it should be difficult to provide specific values because of partial contamination of the foliage. Foliar transfer factors, expressed as Bq.kg{sup -1}{sub dw} {sub pods}/Bq.L{sup -1}{sub solution} (2.5x10{sup -2}) and translocation factors, dimensionless, (2.3x10{sup -3}) for Am and for Pu (1.5x10{sup -3} and 7.5x10{sup -5} respectively), compared to those for Sr (respectively 3.6x10{sup -3} and 5.9x10{sup -4}) and for Cs (respectively 2.9x10{sup -1} and 1.3x10{sup -1}), were studied using this procedure. Transfer and translocation factors for Am were significantly higher than those for Sr, but were smaller than those for Cs. Therefore, Am can be classified as a medium mobile radionuclide in plant. Transfer and translocation of Pu were significantly lower than these for Sr and for Am. Besides, the transfer and translocation factors of Am and Pu only differed from one order of magnitude or less from the one of Sr, which could be in the usual range of variation

  5. Role of self-irradiation defects on the ageing of 239PuCoGa5

    Low-temperature accumulation and annealing experiments, in conjunction with electrical resistivity and critical current density measurements, were used to study the ageing of the actinide superconductor PuCoGa5. These measurements reveal that 2-nm-sized non-superconducting point-like regions are the main damages formed during room temperature ageing; smaller point-like defects are irrelevant to transport properties. Defect sizes and densities deduced from experiment agree with Transmission Electron Microscopy observations. (authors)

  6. Uncertainty Budget and Efficiency Analysis for the 239Pu (n,2ny) Partial Reaction Cross-Section Measurements

    The 239Pu(n,2nγ)238Pu partial reaction cross-section, σ(n,2nγ), has been measured as a function of neutron energy for several transitions in 238Pu. Partial γ-ray cross sections for yrast, ''collector'' transitions, can provide especially valuable constraints on the magnitude and shape of the total (n,2n) reaction cross-section. In essence, nuclear reaction models will be used to infer the shape and magnitude of the total (n,2n) reaction cross-section from the measured partial γ-ray cross-sections. The reason for undertaking this somewhat indirect approach is that previous measurements of the 239Pu(n,2nγ) have been hampered by a variety of constraints. Activation measurements have several hurdles: (1) intense flux and long counting times are required to overcome the relatively long half-life of 238Pu (87 years) and (2) isotopically pure samples of 239Pu in an environment free of 238Pu contamination are difficult to come by. Neutron counting experiments are subject to significant uncertainties because (1) large background statistics from fission neutrons and (2) the experimental fission neutron multiplicity spectrum is subject to systematic errors because the flux of low-energy neutrons which induce fissions in thermally-fissile 239Pu is very difficult to characterize. In this measurement, spallation neutrons are provided by the LANSCE/WNR facility, and reaction neutron energies are determined via time-of-flight. Neutron flux is monitored in-beam with one 235U fission chamber and one 238U fission chamber. The 238U is not sensitive to background from low-energy neutrons, whereas the 235U fission chamber has better statistics. Hence, in essence the partial γ-ray cross sections are normalized to the evaluated fission cross sections of 235U and 238U. As a check of our normalization to provide additional constraints to the nuclear reaction modeling, benchmark measurements of natFe(n, n(prime)γ) and 235U(n,2nγ) have also been undertaken. The secondary γ-rays are

  7. Evaluating the 239Pu Prompt Fission Neutron Spectrum Induced by Thermal to 30 MeV Neutrons

    Neudecker D.

    2016-01-01

    Full Text Available We present a new evaluation of the 239Pu prompt fission neutron spectrum (PFNS induced by thermal to 30 MeV neutrons. Compared to the ENDF/B-VII.1 evaluation, this one includes recently published experimental data as well as an improved and extended model description to predict PFNS. For instance, the pre-equilibrium neutron emission component to the PFNS is considered and the incident energy dependence of model parameters is parametrized more realistically. Experimental and model parameter uncertainties and covariances are estimated in detail. Also, evaluated covariances are provided between all PFNS at different incident neutron energies. Selected evaluation results and first benchmark calculations using this evaluation are briefly discussed.

  8. Fission fragment charge and mass distributions in 239Pu(n,f) in the adiabatic nuclear energy density functional theory

    Regnier, D; Schunck, N; Verriere, M

    2016-01-01

    Accurate knowledge of fission fragment yields is an essential ingredient of numerous applications ranging from the formation of elements in the r-process to fuel cycle optimization for nuclear energy. The need for a predictive theory applicable where no data is available is an incentive to develop a fully microscopic approach to fission dynamics. In this work, we calculate the pre-neutron emission charge and mass distributions of the fission fragments formed in the neutron-induced fission of 239Pu using a microscopic method based on nuclear energy density functional (EDF) method, where large amplitude collective motion is treated adiabatically using the time dependent generator coordinate method (TDGCM) under the Gaussian overlap approximation (GOA). Fission fragment distributions are extracted from the flux of the collective wave packet through the scission line. We find that the main characteristics of the fission charge and mass distributions can be well reproduced by existing energy functionals even in tw...

  9. The deposition, distribution and retention of inhaled 239PuO2 in the lungs of rats with pulmonary emphysema

    Individuals with chronic obstructive lung disease, such as emphysema, may be more susceptible to injury from other inhaled pollutants. However, dose-response studies of inhaled radionuclides conducted to aid in estimating the biological effects of inhaled radionuclides in man have typically used healthy laboratory animals. Changes in radionuclide deposition, distribution and retention in the lungs as the result of pre-existing lung diseases could alter the radiation dose or the resulting biological effects. An experimental animal model for human emphysema, in which emphysema is induced by the intratracheal instillation of either elastase or papain, has been reviewed. This model was used to study the effects of pulmonary emphysema on the deposition, distribution and retention of inhaled 239PuO2 in rats. (author)

  10. Development of a rapid radiochemical procedure for the separation of /sup 235m/U from 239Pu

    We have developed a rapid radiochemical procedure for the isolation and purification of /sup 235m/U (t/sub 1/2/ = 26 minutes) from 239Pu samples up to 250 mg. Purpose of developing the procedure was to measure the thermal neutron fission cross section of the isomeric meta state of 235U. We used rapid small-scale anion exchange columns that absorbed uranium in concentrated HBr but did not absorb plutonium. Uranium was easily eluted with very dilute HF. The separation time required 25 to 35 minutes. We were able to attain a separation factor of uranium from plutonium of approximately 1 x 1010 with samples ranging from 1 x 1010 to 3 x 1011. The ratio of the fission cross sections for the meta to ground state was measured to be 1.42. 4 figs., 1 tab

  11. Estimation of 239Pu independent and cumulative fission product yields from the chain yield data using a Bayesian technique

    The independent and cumulative fission product yields (FPYs) are obtained by using the Bayesian technique based on the evaluated mass chain yield, where required constraints such as the normalization can be straightforwardly included. We apply this technique to the 239Pu FPY data at neutron incident energies of 0.5, 2.0, and 14 MeV, where the most updated mass chain yield ENDF/B-VII.1 data are available. The obtained yield data are compared with the evaluated values by England and Rider in ENDF/B-VI, and differences from their values are investigated. We show that the modern decay data used, such as branching ratios to ground and metastable states, cause differences in the evaluated individual and cumulative fission yields. (author)

  12. Determination of the 240Pu/239Pu atom ratio in low activity environmental samples by alpha spectrometry and spectral deconvolution

    In this paper, a simple technique, based on commercially-available software developed for gamma spectra analysis (MicroSAMPO trademark), is described by which this complex multiplet can be resolved at the much lower activities typical of many environmental samples. In our approach, it is not necessary to make any alterations to the normal alpha spectrometric set-up (including energy dispersion), other than to improve collimation. The instrumental function is defined for each spectrum by fitting a modified gaussian with exponential tails to the comparatively well-resolved 242Pu ''doublet'' (used as tracer) and, if present, the 238Pu ''doublet''. The fitted peaks are used to create an energy calibration file with which, using published energy data, the positions (in channels) of the component peaks of the multiplet are predicted. These positions are not altered subsequently when MicroSAMPO's interactive multiplet analysis facility is used to quantify the relative spectral intensities of the components. Before calculating the 240Pu/239Pu ratio, it is advisable to correct for coincidence summing of alpha particles and conversion electrons. The technique has been applied to the determination of the 240Pu/239Pu ratio in a set of environmental samples, most of which were supplied by IAEA-MEL under their laboratory intercomparison programme. Subsequently, replicate samples were analysed independently using thermal ionisation mass spectrometry. The agreement between the two sets of data was most satisfactory. Further validation of this deconvolution technique was provided by the good agreement between the measured alpha-emission probabilities for the component peaks in the 239,240Pu multiplet and published values. (orig.)

  13. Intercomparison study of inductively coupled plasma mass spectrometry, thermal ionization mass spectrometry and fission track analysis of μBq quantities of 239Pu in synthetic urine

    Even today, some Marshall Islanders are looking forward to permanently resettling their islands after five decades. The U.S. Department of Energy and the resettled residents require reasonable but cost-prudent assurance that the doses to resident from residual 239Pu will not exceed recognized international standards or recommendations, as estimated from the excretion of 239Pu in urine. The goal of this study was to evaluate the bias, uncertainty and sensitivity of analytical techniques that measure 3-56 μBq 239Pu in synthetic urine. The analytical techniques studied in this work included inductively coupled plasma mass spectrometry, thermal ionization mass spectrometry and fission track analysis. The results of the intercomparison demonstrated that all three techniques were capable of marking the measurements, although not with equal degree of bias and uncertainty. The estimated minimum detectable activity was 1 μBq of 239Pu per synthetic urine sample. This exercise is also the first effort to certify test materials of plutonium in the nBqxg-1 range. (author)

  14. Perturbation in the 240Pu/239Pu global fallout ratio in local sediment following the nuclear accidents at Thule (Greenland) and Palomares (Spain)

    It is well established that the main source of the plutonium found in marine sediments throughout the Northern Hemisphere is global stratospheric fallout, characterized by a typical 240Pu/239Pu atom ratio of ∼0.18. Measurements of perturbations in this ratio at various sites which had been subjected to close-in fallout, mainly from surface-based testing, has confirmed the feasibility of using this ratio to distinguish plutonium from different fallout sources. In the present study, the 240Pu/239Pu ratio has been examined in samples of sediment collected at Thule (Greenland) and Palomares (Spain), where accidents involving the release and dispersion of plutonium from fractured nuclear weapons occurred in 1968 and 1966, respectively. The 240Pu/239Pu ratio was measured by high-resolution alpha spectrometry and spectral deconvolution. The analytical results showed that at Thule the mean 240Pu/239Pu atom ratio was 0.033±0.004, while at Palomares the equivalent ratio appeared to be significantly higher at 0.056±0.003. Both ratios are consistent with those reported for soils samples at the Nevada site and Nagasaki, and are clearly indicative of weapons-grade plutonium. 27 refs., 1 fig., 2 tabs

  15. The biokinetics of four 239Pu/241Am dioxide bearing dusts in the rat after inhalation: the implications for occupational exposure

    The aims of the work described here were to provide an experimental basis for evaluating the committed effective dose equivalent per unit intake together with the ALI for four industrial oxide bearing dusts, and to assess the extent to which 241Am could be used for estimating the 239Pu content of the lung after an accidental intake of these materials. (author)

  16. Analytical Method for Pu-239, Pu-240, Np-237 and Tc-99 using Inductively Coupled Plasma Mass Spectrometry

    An efficient analytical method for Pu isotopes (Pu-239 and Pu-240), Np-237 and Tc-99 in environmental samples has been developed using sector field inductively coupled plasma mass spectrometry (SF-ICPMS) detection. The chemical separation of Pu in terrestrial samples, soil, and sediment was carried out on two extraction resins, Sr-Spec and TEVA, which were sequentially combined in PrepLab, an integrated liquid handing device. By reducing the final eluent volume to 2.4 mL, directly injecting it to SF-ICPMS, and employing MCN-6000, a membrane desolvating sample introduction system, the analysis of Pu isotopes was found to be feasible in 1 g of soil. The detection limits of Pu-239, Pu-240, and Pu-242 were approximately 4 fg mL-1 (9.2 Bq mL-1), 3 fg mL-1 (25 Bq mL-1), and 6 fg mL-1 (0.87 Bq mL-1), which represent total amounts of 9.6, 7.2, and 14 fg, respectively, in the final eluent. Chemical separation and measurement were fully automated by a sequential injection (SI) program in an on-line system, and the analysis could thereby be completed within roughly 5 hours. The reliability of this method was confirmed by a validity test with several certified standard reference materials (NIST-4350b, IAEA-6, IAEA-300, IAEA-367, IAEA-368, IAEA-375). The analytical method for Pu in environmental seawater is different from that of terrestrial samples owing to the strong interference effect of U as well as ultra-low level Pu. Although the principle of chemical separation is nearly the same as in soil, seawater was co-precipitated with Fe(OH)2 in the pre-treatment step and a micro TEVA column (50 L) was used in the on-line system to improve precision and the lower detection limit. With this method, it was possible to analyze ultra-trace level Pu isotopes in only 5 L of surface seawater within 1 day, and the precision for Pu-239 and Pu-240 was less than 3.4% (n=7) and 5% (n=7), respectively. The accuracy of this method was verified by analysis of reference seawater (IAEA-381) as

  17. Analytical Method for Pu-239, Pu-240, Np-237 and Tc-99 using Inductively Coupled Plasma Mass Spectrometry

    Kim, Cheol Su

    2007-02-15

    An efficient analytical method for Pu isotopes (Pu-239 and Pu-240), Np-237 and Tc-99 in environmental samples has been developed using sector field inductively coupled plasma mass spectrometry (SF-ICPMS) detection. The chemical separation of Pu in terrestrial samples, soil, and sediment was carried out on two extraction resins, Sr-Spec and TEVA, which were sequentially combined in PrepLab, an integrated liquid handing device. By reducing the final eluent volume to 2.4 mL, directly injecting it to SF-ICPMS, and employing MCN-6000, a membrane desolvating sample introduction system, the analysis of Pu isotopes was found to be feasible in 1 g of soil. The detection limits of Pu-239, Pu-240, and Pu-242 were approximately 4 fg mL-1 (9.2 Bq mL-1), 3 fg mL-1 (25 Bq mL-1), and 6 fg mL-1 (0.87 Bq mL-1), which represent total amounts of 9.6, 7.2, and 14 fg, respectively, in the final eluent. Chemical separation and measurement were fully automated by a sequential injection (SI) program in an on-line system, and the analysis could thereby be completed within roughly 5 hours. The reliability of this method was confirmed by a validity test with several certified standard reference materials (NIST-4350b, IAEA-6, IAEA-300, IAEA-367, IAEA-368, IAEA-375). The analytical method for Pu in environmental seawater is different from that of terrestrial samples owing to the strong interference effect of U as well as ultra-low level Pu. Although the principle of chemical separation is nearly the same as in soil, seawater was co-precipitated with Fe(OH)2 in the pre-treatment step and a micro TEVA column (50 L) was used in the on-line system to improve precision and the lower detection limit. With this method, it was possible to analyze ultra-trace level Pu isotopes in only 5 L of surface seawater within 1 day, and the precision for Pu-239 and Pu-240 was less than 3.4% (n=7) and 5% (n=7), respectively. The accuracy of this method was verified by analysis of reference seawater (IAEA-381) as

  18. Perturbation in the 240Pu/239Pu global fallout ratio in local sediments following the nuclear accidents at Thule (Greenland) and Palomares (Spain).

    Mitchell, P I; León Vintró, L; Dahlgaard, H; Gascó, C; Sánchez-Cabeza, J A

    1997-08-25

    It is well established that the main source of the plutonium found in marine sediments throughout the Northern Hemisphere is global stratospheric fallout, characterized by a typical 240Pu/239Pu atom ratio of approximately 0.18. Measurement of perturbations in this ratio at various sites which had been subjected to close-in fallout, mainly from surface-based testing (e.g. Bikini Atoll, Nevada test site, Mururoa Atoll), has confirmed the feasibility of using this ratio to distinguish plutonium from different fallout sources. In the present study, the 240Pu/239Pu ratio has been examined in samples of sediment (and soil) collected at Thule (Greenland) and Palomares (Spain), where accidents involving the release and dispersion of plutonium from fractured nuclear weapons occurred in 1968 and 1966, respectively. The 240Pu/239Pu ratio was measured by high-resolution alpha spectrometry and spectral deconvolution, and confirmed in the case of the most active samples by high-resolution X-ray spectrometry. Only samples which displayed plutonium heterogeneities, i.e. hot particles or concentrations well in excess (at least two orders of magnitude) of those expected from global fallout, were selected for analysis. The analytical results showed that at Thule the mean 240Pu/239Pu atom ratio was 0.033 +/- 0.004 (n = 4), while at Palomares the equivalent ratio appeared to be significantly higher at 0.056 +/- 0.003 (n = 4). Both ratios are indicative of low burn-up plutonium and are consistent with those reported for weapons-grade plutonium. It is noteworthy that the mean 238Pu/239Pu activity ratio in the Thule samples, at 0.0150 +/- 0.0017 (n = 4), was also lower than that measured in the Palomares samples, namely, 0.0275 +/- 0.0012 (n = 4). The 241Pu/239Pu ratios were similarly different. Finally, the data show, in contrast to Palomares, that not all of the samples from the Thule accident site were contaminated with plutonium of identical isotopic composition. PMID:9241884

  19. Phenyl trifluoromethyl sulfone as diluent in a grouped actinide extraction process. Extraction properties of the solvent components TBP and CyMe4-BTBP

    The grouped actinide extraction (GANEX) process combines two extractants CyMe4-BTBP and TBP in a diluent, in this study phenyl trifluoromethyl sulfone (FS-13). The extraction of U-235, Np-239, Pu-238, Am-241, Cm-244 and Eu-152 has been investigated in four different systems. System 1: 70 %vol FS-13, 30 %vol TBP and 10 mM CyMe4-BTBP, system 2: 70 %vol FS-13 and 30 %vol TBP, system 3: 100 %vol FS-13 and 10 mM CyMe4-BTBP and system 4: pure FS-13. In all cases 4 M HNO3 was used as aqueous phase. In system 1 all actinides were extracted and separated from the lanthanides. In both system 2 and 3 mainly U and Pu were extracted. In system 4 none of the metals were extracted. (author)

  20. Neutron emission effects on fragment mass and kinetic energy distribution from fission of 239Pu induced by thermal neutrons

    The average of fragment kinetic energy () and the multiplicity of prompt neutrons (ν(bar sign)) as a function of fragment mass (m*), as well as the fragment mass yield (Y (m*)) from thermal neutron induced fission of 239Pu, have been measured by Tsuchiya et al.. In that work the mass and kinetic energy are calculated from the measured kinetic energy of one fragment and the difference of time of flight of the two complementary fragments. However they do not present their results about the standard deviation σE*(m*). In this work we have made a numerical simulation of that experiment, assuming an initial distribution of the primary fragment kinetic energy (E(A)) with a constant value of the standard deviation as function of fragment mass σE(A)). As a result of that simulation we obtain the dependence σE*(m*) which presents an enhancement between m* = 92 and m* 110, and a peak at m* = 121. (orig.)

  1. Neutron emission effects on fragment mass and kinetic energy distribution from fission of 239Pu induced by thermal neutrons

    The average of fragment kinetic energy (E-bar sign*) and the multiplicity of prompt neutrons (ν(bar sign)) as a function of fragment mass (m*), as well as the fragment mass yield (Y(m*)) from thermal neutron-induced fission of 239Pu have been measured by Tsuchiya et al.. In that work the mass and kinetic energy are calculated from the measured kinetic energy of one fragment and the difference of time of flight of the two complementary fragments. However they do not present their results about the standard deviation σE*(m*). In this work we have made a numerical simulation of that experiment which reproduces its results, assuming an initial distribution of the primary fragment kinetic energy (E(A)) with a constant value of the standard deviation as function of fragment mass (σE(A)). As a result of the simulation we obtain the dependence σE*(m*) which presents an enhancement between m* = 92 and m* = 110, and a peak at m* = 121.

  2. A Study of the Resonance Interaction Effect between 238U and 239Pu in Lower Energy Region

    An investigation has been made of the statistical frequency function for the distances between the 238U and the 239Pu resonances in the region 4-244 eV. It is concluded that the frequency function is probably constant but that the distances diverge appreciably from a constant function in the actual case, and that the divergence is such that the interaction effect on the resonance integral is smaller than would be expected from statistical considerations. This is also confirmed by calculations on the interaction effect. These have been performed using three different methods, namely: a) considering the actual positions and widths of the resonances, b) assuming a constant frequency function for the resonance. spacing and applying a theory developed by Rowlands and E A Fischer. c) applying a simplified, approximate method for calculations based on the statistical theory. The calculations are made for two temperatures and two values of the plutonium enrichment. It is shown that the average cross sections are considerably larger than the statistical calculations indicate

  3. Radionuclide distribution dynamics in skeletons of beagles fed 90Sr: Correlation with injected 226Ra and 239Pu

    Data for the bone-by-bone redistribution of 90Sr in the beagle skeleton are reported for a period of 4000 d following a midgestation-to-540-d-exposure by ingestion. The partitioned clearance model (PCM) that was originally developed to describe bone-by-bone radionuclide redistribution of 226Ra after eight semimonthly injections at ages 435-535 d has been fitted to the 90Sr data. The parameter estimates for the PCM that describe the distribution and clearance of 226Ra after deposition on surfaces following injection and analogous parameter estimates for 90Sr after uniform deposition in the skeleton as a function of Ca mass are given. Fractional compact bone masses per bone group (mi,COM) are also predicted by the model and compared to measured values; a high degree of correlation (r = 0.84) is found. Bone groups for which the agreement between the model and experimental values of mi,COM was poor had tissue-to-calcium weight ratios about 1.5 times those for bones that agreed well. Metabolically defined surface in PCM is initial activity fraction per Ca fraction in a given skeletal component for intravenously injected alkaline earth (Sae) radionuclides; comparisons are made to similarly defined surface (Sact) values from 239Pu injection studies. The patterns of Sae and Sact distribution throughout the skeleton are similar

  4. Reciprocal translocations in ageing mice and mice with long-term low-level 239Pu contamination

    Single intravenous injections of 185 Bq monomeric 239Pu were given to male mice, and the frequency of primary spermatocytes with reciprocal translocations, determined 724 days after treatment, was not significantly different from that of age-matched untreated controls. These old animals showed significantly higher aberration frequencies than young adults. The data therefore show that for low initial activity and very long retention time the possible cytogenetic effects of incorporated nuclide does not change the age-related pattern of increase of spontaneous chromosome aberrations. Considerations of the main variables involved in the induction of cytogenetic effects of incorporated plutonium, based on literature data, indicate that the initial injected activity, the estimated total accumulated average organ dose, and the retention time interact in a complex way; as far as can be seen at present, the effects seem to be dependent mainly on the initial activity at short times after contamination, while the retention time appears to be predominant in the case of long-term observations. (author)

  5. Evaluation of the thermal-neutron constants for 233U, 235U, 239Pu and 241Pu

    A consistent set of best values of the 2200 meter/second neutron cross sections, Westcott g-factors, and fission neutron yields for 233U, 235U, 239Pu and 241Pu are presented. A least squares fitting program, LSF, is used to obtain the best fit and to estimate the sensitivity of these fissile parameters to the quoted uncertainties in experimental data. The half-lives of the uranium and plutonium nuclides have been evaluated and these have been used to reassess the significant experimental data. The latest revision of the spontaneous fission neutron yield anti nu, of 252Cf and the foil thickness corrections to the fission neutron yield ratios of fissile nuclei to 252Cf are included. These lead to greater consistency in the data used for anti nu (252Cf). Similarly, the 234U half-life as revised leads to improved consistency in the 235U fission cross section. Comparison is made with the values from ENDF/B-V and other evaluations

  6. Re-entrainment of {sup 239}PuO{sub 2} Particles Captured on HEPA Filter Fibres

    Yamada, Y.; Koizumi, A.; Miyamoto, K

    1999-07-01

    Filter performance is very important not only before use but also in use. In addition to particle collection, particle retention or dispersion rate should be evaluated. Re-entrainment of {sup 239}PuO{sub 2} particles collected on HEPA filter fibres was investigated under various conditions of air flow direction, air flow rate, air flow pattern and dust loading. Plutonium aerosols with an activity median aerodynamic diameter of 0.45 {mu}m and a geometric standard deviation of 2.0 were used. Dispersion rate per hour, which is defined as activity ratio on the sampling filter downstream to that on the source filter, under forward flow, was measured as less than 2.3 x 10{sup -7} h{sup -1}. Under reverse flow, higher dispersion rates were observed, but the dispersion decreased with repeated sample runs. A high air flow rate increased the dispersion rate. There was no significant differences among air flow patterns. Dispersion rate depended strongly on the dust loading level. For example, at 2.9 times the loading of atmospheric aerosols compared with the initial pressure drop the dispersion rate was increased by approximately 100 times to 10{sup -2} h{sup -1}. (author)

  7. Coulomb effects in isobaric cold fission from reactions 233U(nth,f), 235U(nth,f), 239Pu(nth,f) and 252Cf(sf)

    Montoya, Modesto

    2014-01-01

    The Coulomb effect hypothesis, formerly used to interpret fluctuations in the curve of maximal total kinetic energy as a function of light fragment mass in reactions 233U(nth,f), 235U(nth,f) and 239Pu(nth,f), is confirmed in high kinetic energy as well as in low excitation energy windows, respectively. Data from reactions 233U(nth,f), 235U(nth,f), 239Pu(nth,f) and 252Cf(sf) show that, between two isobaric fragmentations with similar Q-values, the more asymmetric charge split reaches the higher value of total kinetic energy. Moreover, in isobaric charge splits with different Q-values, similar preference for asymmetrical fragmentations is observed in low excitation energy windows.

  8. Evaluation of quantitative factors of 90Sr, 137Cs, 239Pu, 241Am transfer from contaminated soil with gastric and intestine juices of cows

    The biological availability and parameters of transuranium elements metabolism in an organism of cows pasturing in the Chernobyl NPP alienation zone are evaluated. The values of the radioactivity of 90Sr, 137Cs, 239Pu and 241Am are presented in samples of gastric and intestine juices of cows as well as in simulative solutions after soil processing by them. Quantitative parameters of 90Sr, 137Cs, 239Pu and 241Am transfer from solid phase of soil to gastric, intestine juice of cows as well as to simulative solutions have been estimated on the basis of results of laboratory incubation experiments. A prevailing role of enzyme complex and microflora of gastrointestinal tract in radionuclides transfer from solid phase of soil to solution has been shown

  9. Assinatura da deposição atmosférica de testes nucleares em sedimentos da costa brasileira (240+239Pu e 137Cs

    Christian J. Sanders

    2012-01-01

    Full Text Available The aim of this review is to take a look at Cold War era nuclear tests signatures found in Brazilian coastal sediments. Both137Cs and 240+239Pu signatures have been documented in mangrove, coastal mudflats and continental shelf sediments, associated with above ground nuclear tests beginning in the 1950's. The dates associated to the anthropogenic radionuclide signatures 137Cs and 240+239Pu along sediment columns are confirmed by 210Pb geochronology in many of the studies highlighted in this review. The results outlined in this review characterize the extent to which nuclear fallout products reach the Brazilian coast in quantities sufficient for detection, allowing the use of these radioisotopes as geochronometers.

  10. Comparison of the ENDF/B-V and SOKRATOR evaluations of 235U, 239Pu, 240Pu and 241Pu at low neutron energies

    The US and USSR's most recent evaluationsof 235U, 239Pu, 240Pu and 241Pu are compared over the thermal region and over the first few resonances. The two evaluations rest on essentially the same experimental data base and the differences reflect different approaches to the representation of the cross sections or different weightings of the experimental results. It is found that over the thermal and resolved ranges the two evaluations are very similar. Some differences in approaches are briefly discussed

  11. Long-term effects of inhaled Ca-DTPA in rats previously exposed to 239Pu(NO3)4 aerosols

    Inhaled Ca-DTPA given 20 days after 239Pu(NO3)4 inhalation was marginally effective (p = 0.10) in reducing the amount of Pu in rat lung. This reduction in Pu lung burden did not, however, affect the later induction of lung tumors. An increased osteosarcoma incidence was noted in control rats exposed only to nitric acid aerosols. Complete tumor incidence data are not yet available. (U.S.)

  12. The subcellular distribution of 239Pu, 241Am and 59Fe in the liver of rat and Chinese hamster as dependent on time

    The subcellular distribution of monomeric 239Pu, 241Am and iron in rat and Chinese hamster liver has been investigated by sucrose-, metrizamide- and Percoll-density gradients. In rat liver, the transuranium elements become and remain bound to typical lysosomes primary storage organelle in Chinese hamster liver. However, their apparent density in sucrose decreases with time, which possible indicates transition into telolysomes. The transuranium nuclides show a subcellular distribution which is quite different from that of iron. (orig.)

  13. Some pathophysiological and biochemical changes in dogs with different forms of lesions induced by inhalation of /sup 239/Pu and /sup 241/Am nitrates

    Kalmykova, Z.I.; Tokarskaya, Z.B.; Buldakov, L.A.; Nifatov, A.P.; Vedeneev, V.S.

    Dogs were acutely, subacutely and chronically inhaled with polymeric /sup 239/Pu and monomeric /sup 241/Am nitrates. Distinctly directed changes were observed in the protein fraction and glycoproteins, as well as in transaminases and sorbitoldehydrogenase of the blood serum, which were attributed to unequal radiation loads to the lungs and the organs of the secondary deposition of nuclides, and also to different degree of the respiratory distress.

  14. XAS and XRD study of annealed 238Pu- and 239Pu-substituted zircons (Zr0.92Pu0.08SiO4)

    An annealing study has been completed on two compositionally identical Pu-substituted zircons (Zr0.92Pu0.08SiO4) prepared 18 yr ago with different 238Pu/239Pu isotopic ratios. The activity and accumulated dose for each material varies greatly due to the very different half-lives of 238Pu (87.7 yr) and 239Pu (24 100 yr). The predominantly 238Pu-substituted zircon is in a highly amorphous state after accumulating a dose of 2.8x1019 α-decays/g, which is a factor of two higher than the dose previously determined necessary to amorphize this material. The 239Pu-substituted zircon has remained highly crystalline after an accumulated dose of 1.2x1017 α-decays/g. The Pu in both samples is trivalent due to sintering under reducing conditions. The short-range and long-range structures of each sample have been characterized by detailed X-ray absorption spectroscopy and X-ray diffraction (XRD) methods. The oxidation of Pu3+ to Pu4+ in the crystalline 239Pu-substituted zircon during annealing in air resulted in a decrease in lattice distortion due to the decrease in ionic radius of Pu3+ to Pu4+ on the Zr4+ site. A significant amount of PuO2 exsolved from the zircon structure after annealing at 1200 deg. C in air. Detailed characterization of the amorphous 238Pu-substituted zircon demonstrated that while devoid of long-range order it still retained a distorted zircon structure and composition over a length scale of 0.5 nm. The recrystallization of the amorphous 238Pu-substituted zircon could be achieved directly at temperatures as low as 1200 deg. C when annealed for 12 h in air; however, annealing at 1000 deg. C resulted in decomposition into constituent oxides

  15. Suppression of the pulmonary clearance of Staphylococcus aureus in mice that had inhaled either 144CeO2 or 239PuO2

    The rate of pulmonary clearance of inhaled Staphylococcus aureus in mice was determined at intervals after inhalation exposure to either 144CeO2 or 239PuO2. In mice with mean initial lung burdens between 0.6 and 4.7 μCi 144Ce the pulmonary clearance of S. aureus was suppressed up to 12 weeks after inhalation of 144CeO2. In mice with mean initial lung burdens between 1.3 and 29.0 μCi 239Pu the pulmonary clearance of S. aureus was suppressed up to 26 weeks after inhalation of 239PuO2. The suppressed pulmonary clearance of S. aureus appeared to correlate with the radiation dose rate to the lungs at the time of exposure to bacteria but not with the cumulative radiation dose to the lungs. The changes in bacterial clearance did not appear to be correlated with changes in body weight, hematological parameters, or radiation-induced histopathological changes. Altered bacterial clearance may be related to radiation damage to pulmonary macrophages. It was concluded that irradiation of the lung from radionuclides inhaled in relatively insoluble forms may result in increased bacterial invasion of the lungs

  16. Radiosensitivity and proliferative activity of vertebral CFU-s surviving in mice injected with oncogenic activities of 239Pu or 241Am

    Survival, radiosensitivity and capability to produce differentiated progeny were studied in CFU-S from lumbar vertebrae of mice injected with 198.6 kBq 239Pu/kg or 208.6 kBq 241Am/kg. The CFU-S assay and 59Fe uptake by spleen colonies were used. The number of CFU-S from treated mice was significantly lower than in the controls. Higher radiosensitivity of CFU-S from 239Pu- or 241Am-treated mice was demonstrated using additional exposure to 0.5 Gy X-rays 1, 24, 48, 72 hrs after cell transplant and expressed more accurately by survival curves obtained 1 hr after the marrow cell injection. The effect of 239Pu on CFU-S was characterized by D0 0.58 Gy (n=0.91) and that of 241Am by D0 0.64 Gy (n=0.91); corresponding control values were D0 0.89 Gy, n=1.11. Lower iron utilization due not only to the decreased CFU-S numbers, but also to the defective production of erythrocytes per one CFU-S was found. The complexity of radiation effect on hematopoietic stem cells was demonstrated by the present study. (author)

  17. Calculation of prompt fission product average cross sections for neutron-induced fission of 235U and 239Pu

    Yield-weighted average cross sections of neutron radiative capture, (n,2n), and (n,3n) reactions over prompt fission products (FPs) from 235U and 239Pu are calculated. The prompt fission production yields are taken from the ENDF/B-VII.0 library. The FPs for each fissile material exist over a range of approximately 1000 neutron-rich nuclides. Several nuclear reaction codes are utilized for calculating the cross sections on each individual fission product - EMPIRE-2.19, TALYS-1.0, GNASH, and CoH. The influence of the FP isomers on the average cross sections is examined with TALYS. We investigate the dependence of the average cross sections on the number of FPs taken for averaging. It is shown that the average capture cross section is much more sensitive to the number of FPs included, compared with the (n,2n) and (n,3n) reactions. An intercomparison of the calculated cross sections with the different reaction codes is carried out. In the capture reaction, EMPIRE predicted lower cross section than TALYS and CoH owing to different default assumptions used in the γ-ray strength function modeling. Moreover, the pre-equilibrium models implemented in each code give different predictions for the neutron-emission reactions, although the differences are relatively small. We also discuss a difference between the macroscopic and microscopic calculation options in TALYS for the pre-equilibrium model, optical potential model, and γ-ray strength function. The predictive capability of the reaction codes for the capture reaction is examined by comparing their calculations with the ENDF data, which are based on measurements. Compared with the historic Foster and Arthur's evaluation, our new (n,2n) predictions are similar, although our capture predictions are almost an order of magnitude higher. Recommended cross sections for use in applications have been tabulated in ENDF-formatted files. (author)

  18. Feedback on 239Pu and 240Pu nuclear data and associated covariances through the CERES integral experiments

    Benchmark measurements of irradiated and un-irradiated fuel samples were performed in the framework of the CERES collaborative program between AEA (UK Atomic Energy Agency) and CEA (French Atomic Energy Commission). These experiments provide relevant data for the validation of fuel burn-up and criticality-safety calculations for the whole fuel cycle. As part of this program, pile-oscillation measurements were carried out on a range of mixed-oxide samples with plutonium of various mass and isotopic contents, both in the MINERVE and DIMPLE reactors. Four core configurations, two over-thermalized situations and two pressurized water reactor (PWR)-type situations, were constituted with different forward and adjoint flux spectra, emphasizing fission and/or capture contributions. The experiments were analyzed using reference TRIPOLI4 calculations with the JEFF-3.1.1 library, using exact three-dimensional models of the core configurations. In a first step, calculations of each DIMPLE configuration were performed and compared with the experiment, showing very good agreements with a maximum C-E of -230 pcm. In the second step, reactivity worth experiments were analyzed, using recently developed exact-perturbation capabilities in TRIPOLI4. A consistent assimilation of calculation over experiment discrepancies was performed with the CONRAD code, using the integral data assimilation method. Covariance matrix on multigroup neutron cross sections and multiplicities were generated and significant trends were identified, especially on the 239Pu and 240Pu capture cross sections in the thermal energy range (E < 0.1 eV). Further investigations should be required to confirm these conclusions, due to the strong dependence of these trends and of posterior covariances to prior covariances. (author)

  19. Event-by-event study of prompt neutrons from 239Pu(n,f)

    Vogt, R; Randrup, J; Pruet, J; Younes, W

    2009-07-23

    Employing a recently developed Monte-Carlo model, we study the fission of {sup 240}Pu induced by neutrons with energies from thermal to just below the threshold for second chance fission. Current measurements of the mean number of prompt neutrons emitted in fission, together with less accurate measurements of the neutron energy spectra, place remarkably fine constraints on predictions of microscopic calculations. In particular, the total excitation energy of the nascent fragments must be specified to within 1MeV to avoid disagreement with measurements of the mean neutron multiplicity. The combination of the Monte-Carlo fission model with a statistical likelihood analysis also presents a powerful tool for the evaluation of fission neutron data. Of particular importance is the fission spectrum, which plays a key role in determining reactor criticality. We show that our approach can be used to develop an estimate of the fission spectrum with uncertainties several times smaller than current experimental uncertainties for outgoing neutron energies of less than 2 MeV.

  20. Event-by-Event Study of Prompt Neutrons from 239Pu

    Vogt, R; Randrup, J; Pruet, J; Younes, W

    2010-01-15

    Employing a recently developed Monte Carlo model, we study the fission of {sup 240}Pu induced by neutrons with energies from thermal to just below the threshold for second chance fission. Current measurements of the mean number of prompt neutrons emitted in fission, together with less accurate measurements of the neutron energy spectra, place remarkably fine constraints on predictions of microscopic calculations. In particular, the total excitation energy of the nascent fragments must be specified to within 1 MeV to avoid disagreement with measurements of the mean neutron multiplicity. The combination of the Monte Carlo fission model with a statistical likelihood analysis also presents a powerful tool for the evaluation of fission neutron data. Of particular importance is the fission spectrum, which plays a key role in determining reactor criticality. We show that our approach can be used to develop an estimate of the fission spectrum with uncertainties several times smaller than current experimental uncertainties for outgoing neutron energies of less than 2 MeV.

  1. Matrix effects corrections in DDT assay of {sup 239}Pu with the CTEN instrument

    Hollas, C.L.; Arnone, G.; Brunson, G.; Coop, K. [Los Alamos National Lab., NM (United States)

    1997-11-01

    The accuracy of transuranic (TRU) waste assay using the differential die-away technique depends upon significant corrections to compensate for the effects of the matrix material in which the TRU waste is located. We have used a new instrument, the combined thermal/epithermal neutron (CTEN) instrument for the assay of TRU waste, to develop methods to improve the accuracy of these corrections. Neutrons from a pulsed 14-MeV neutron generator are moderated in the walls of the CTEN cavity and induce fission in the TRU material. The prompt neutrons from these fission events are detected in cadmium-wrapped {sup 3}He neutron detectors. We have developed methods of data acquisition and analysis to extract correlation in the neutron signals resulting from fission during active interrogation. This correlation information, in conjunction with the total number of neutrons detected, is used to determine the fraction of fission neutrons transmitted through the matrix material into the {sup 3}He detectors. This determination allows us to cleanly separate the matrix effects into two processes: matrix modification upon the neutron interrogating flux and matrix modification upon the fraction of fission neutrons transmitted to the neutron detectors. Recent results indicate that for some matrix systems, corrections for position dependent effects within the matrix are possible. 7 refs., 7 figs., 1 tab.

  2. Fission fragment charge and mass distributions in 239Pu(n ,f ) in the adiabatic nuclear energy density functional theory

    Regnier, D.; Dubray, N.; Schunck, N.; Verrière, M.

    2016-05-01

    Background: Accurate knowledge of fission fragment yields is an essential ingredient of numerous applications ranging from the formation of elements in the r process to fuel cycle optimization for nuclear energy. The need for a predictive theory applicable where no data are available, together with the variety of potential applications, is an incentive to develop a fully microscopic approach to fission dynamics. Purpose: In this work, we calculate the pre-neutron emission charge and mass distributions of the fission fragments formed in the neutron-induced fission of 239Pu using a microscopic method based on nuclear density functional theory (DFT). Methods: Our theoretical framework is the nuclear energy density functional (EDF) method, where large-amplitude collective motion is treated adiabatically by using the time-dependent generator coordinate method (TDGCM) under the Gaussian overlap approximation (GOA). In practice, the TDGCM is implemented in two steps. First, a series of constrained EDF calculations map the configuration and potential-energy landscape of the fissioning system for a small set of collective variables (in this work, the axial quadrupole and octupole moments of the nucleus). Then, nuclear dynamics is modeled by propagating a collective wave packet on the potential-energy surface. Fission fragment distributions are extracted from the flux of the collective wave packet through the scission line. Results: We find that the main characteristics of the fission charge and mass distributions can be well reproduced by existing energy functionals even in two-dimensional collective spaces. Theory and experiment agree typically within two mass units for the position of the asymmetric peak. As expected, calculations are sensitive to the structure of the initial state and the prescription for the collective inertia. We emphasize that results are also sensitive to the continuity of the collective landscape near scission. Conclusions: Our analysis confirms

  3. The subcellular distribution of 239Pu, 241Am and 59Fe in the liver of rat and Chinese hamster as dependent on time

    The subcellular distribution of monomeric 239Pu, 241Am and iron in rat and Chinese hamster liver has been investigated by sucrose-, metrizamide- and Percoll-density gradients. In rat liver, the transuranium elements become and remain bound to typical lysosomes up to several months after incorporation. Lysosomes are also the primary storage organelle in Chinese hamster liver. However, their apparent density in sucrose decreases with time, which possibly indicates transition into telolysomes. The transuranium nuclides show a subcellular distribution which is quite different from that of iron. (orig.)

  4. Evaluation of fission cross sections and covariances for {sup 233}U, {sup 235}U, {sup 238}U, {sup 239}Pu, {sup 240}Pu, and {sup 241}Pu

    Kawano, Toshihiko [Kyushu Univ., Fukuoka (Japan); Matsunobu, Hiroyuki [Data Engineering, Inc. (Japan); Murata, Toru [AITEL Corporation, Tokyo (JP)] [and others

    2000-02-01

    A simultaneous evaluation code SOK (Simultaneous evaluation on KALMAN) has been developed, which is a least-squares fitting program to absolute and relative measurements. The SOK code was employed to evaluate the fission cross sections of {sup 233}U, {sup 235}U, {sup 238}U, {sup 239}Pu, {sup 240}Pu, and {sup 241}Pu for the evaluated nuclear data library JENDL-3.3. Procedures of the simultaneous evaluation and the experimental database of the fission cross sections are described. The fission cross sections obtained were compared with evaluated values given in JENDL-3.2 and ENDF/B-VI. (author)

  5. Beta-decay half-lives of neutron rich Cu and Ni isotopes produced by thermal fission of 235U and 239Pu

    The half-lives of very neutron rich isotopes of Ni and Cu have been measured. The isotopes are produced in very asymmetric thermal fission of 235U and 239Pu at the I.L.L. high flux reactor. They are separated by means of the Lohengrin spectrometer. They are identified with a ΔE-E ionization chamber and implanted in one of the 8 Si planar detectors where the β- particles are also detected. The time correlations between the implantation and the detection of β- particles provide the half-life. The values obtained are compared to current theoretical predictions

  6. Simultaneous multi-level analysis of the total and fission cross-sections of 239Pu up to 160 eV

    In order to describe cross-sections a multi-level scheme based on S-matrix theory was used taking the Doppler effect and the resolution into account. A multi-level analysis of the total cross-section and fission cross-section of 239Pu was made by the least-squares method in the energy region up to 160 eV. The experimental cross-section data used have a good resolution. The multi-level parameters can be used to represent all the features of the detailed energy structure of experimental cross-sections where the regions of interference minima are of the greatest interest. (author)

  7. Measurement/Evaluation Techniques and Nuclear Data Associated with Fission of 239Pu by Fission Spectrum Neutrons

    Baisden, P; Bauge, E; Ferguson, J; Gilliam, D; Granier, T; Jeanloz, R; McMillan, C; Robertson, D; Thompson, P; Verdon, C; Wilkerson, C; Young, P

    2010-03-16

    This Panel was chartered to review and assess new evaluations of work on fission product data, as well as the evaluation process used by the two U.S. nuclear weapons physics laboratories. The work focuses on fission product yields resulting from fission spectrum neutrons incident on plutonium, and includes data from measurements that had not been previously published as well as new or revised fission product cumulative yield data, and related quantities such as Q values and R values. This report documents the Panel's assessment of the work presented by Los Alamos National Laboratory (LANL) and Lawrence Livermore National Laboratory (LLNL). Based on the work presented we have seven key observations: (1) Experiments conducted in the 1970s at LANL, some of which were performed in association with a larger, NIST-led, program, have recently been documented. A preliminary assessment of this work, which will be referred to in this document as ILRR-LANL, shows it to be technically sound. (2) LLNL has done a thorough, unbiased review and evaluation of the available literature and is in the process of incorporating the previously unavailable LANL data into its evaluation of key fission product yields. The results of the LLNL effort, which includes a preliminary evaluation of the ILRR-LANL data, have been documented. (3) LANL has also conducted an evaluation of fission product yields for fission spectrum neutrons on plutonium including a meta-analysis of benchmark data as part of a planned upgrade to the ENDF/B compilation. We found that the approach of using meta-analysis provides valuable additional insight for evaluating the sparse data sets involved in this assessment. (4) Both laboratories have provided convincing evidence for energy dependence in the fission product yield of {sup 147}Nd produced from the bombardment of {sup 239}Pu with fission spectrum neutrons over an incident neutron energy range of 0.2 to 1.9 MeV. (5) Consistent, complete, and explicit treatment

  8. Plutonium isotopes 238Pu, 239+240Pu, 241Pu and 240Pu/239Pu atomic ratios in the southern Baltic Sea ecosystem

    Dagmara I. Strumińska-Parulska

    2010-09-01

    Full Text Available The paper summarizes the results of plutonium findings in atmospheric fallout samples and marine samples from the southern Baltic Sea during our research in 1986-2007. The activities of 238Pu and 239+240Pu isotopes were measured with an alpha spectrometer. The activities of 241Pu were calculated indirectly by 241Am activity measurements 16-18 years after the Chernobyl accident. The 240Pu/239Pu atomic ratios were measured using accelerator mass spectrometry (AMS. The 241Pu activities indicate that the main impact of the Chernobyl accident was on the plutonium concentration in the components of the Baltic Sea ecosystem examined in this work. The highest 241Pu/239+240Pu activity ratio was found in sea water (140 ± 33. The AMS measurements of atmospheric fallout samples collected during 1986 showed a significant increase in the 240Pu/239Pu atomic ratio from 0.29 ± 0.04 in March 1986 to 0.47 ± 0.02 in April 1986.

  9. Long-term effects of low-level 239Pu contamination on murine bone-marrow stem cells and their progeny

    The effects of long-term internal contamination with 13.3 kBq kg-1239Pu injected intravenously were studied in 10-week-old ICR (SPF) female mice. Radiosensitivity of spleen colony-forming units (CFU-S) and 125IUdR incorporation into proliferating cells of vertebral bone marrow and spleens were determined in plutonium-treated and control animals one year after nuclide injection. The CFU-S in 239Pu-treated mice were more sensitive to X-rays (D0 = 0.52 +- 0.01 Gy) than in controls (D0 = 0.84 +- 0.02 Gy). 125IUdR incorporation into bone marrow and spleen cells was reduced after plutonium contamination. At one year following plutonium injection, the occurrence of chromosome aberrations was evaluated in metaphase figures of femoral bone marrow cells. The frequency of aberrations increased early after plutonium treatment, at later intervals it tended to decrease but not below the control level. While the relative numbers of vertebral marrow CFU-S decreased significantly, but only to 86% of normal, cellularity of vertebral bone marrow, peripheral blood counts and survival of 239Pu-treated mice did not differ from the control data. (author)

  10. Measurement of the 240Pu/239Pu mass ratio using a transition-edge-sensor microcalorimeter for total decay energy spectroscopy.

    Hoover, Andrew S; Bond, Evelyn M; Croce, Mark P; Holesinger, Terry G; Kunde, Gerd J; Rabin, Michael W; Wolfsberg, Laura E; Bennett, Douglas A; Hays-Wehle, James P; Schmidt, Dan R; Swetz, Daniel; Ullom, Joel N

    2015-04-01

    We have developed a new category of sensor for measurement of the (240)Pu/(239)Pu mass ratio from aqueous solution samples with advantages over existing methods. Aqueous solution plutonium samples were evaporated and encapsulated inside of a gold foil absorber, and a superconducting transition-edge-sensor microcalorimeter detector was used to measure the total reaction energy (Q-value) of nuclear decays via heat generated when the energy is thermalized. Since all of the decay energy is contained in the absorber, we measure a single spectral peak for each isotope, resulting in a simple spectral analysis problem with minimal peak overlap. We found that mechanical kneading of the absorber dramatically improves spectral quality by reducing the size of radioactive inclusions within the absorber to scales below 50 nm such that decay products primarily interact with atoms of the host material. Due to the low noise performance of the microcalorimeter detector, energy resolution values of 1 keV fwhm (full width at half-maximum) at 5.5 MeV have been achieved, an order of magnitude improvement over α-spectroscopy with conventional silicon detectors. We measured the (240)Pu/(239)Pu mass ratio of two samples and confirmed the results by comparison to mass spectrometry values. These results have implications for future measurements of trace samples of nuclear material. PMID:25723106

  11. Precision and accuracy in the determination of sup(238)Pu/(sup(239)Pu + sup(240)Pu) alpha activity ratio by alpha spectrometry

    Investigations were carried out for the evaluation of precision and accuracy in determining sup(238)Pu/(sup(239)Pu + sup(240)Pu) activity ratio by α spectrometry from the point of view of determining sup(238)Pu accurately in plutonium samples and in exploiting Isotope Dilution Alpha Spectrometry (IDAS) for determining the concentration of plutonium in the irradiated fuel dissolver solutions. Synthetic mixtures with α activity ratios ranging from 0.01 to 10 were prepared using sup(238)Pu and sup(239)Pu isotopes. Different methods which can be routinely used were tried to calculate the α activity ratio from the α spectrum taken on electrodeposited sources prepared from these mixtures. An accuracy of better than 0.5% and a precision of +- 0.2% (1 sigma) is demonstrated in the determination of α activity ratios ranging from 0.01 to 10 using electrodeposited sources and the evaluation method based on the geometric progression decrease (G.P.) for the far tail of the spectrum. (auth.)

  12. Measurements of the ratio fo 239Pu and 235U fission cross sections in the 0.024-7.4 MeV neutron energy range

    Aimed at improving the accuracy of available nuclear data 239Pu-to-235U fission cross section ratios were measured in a broad range of neutron energies. The measurements were taken in electrostatic accelerators with the Li(p,n)-,T(p,n)- and D(d,n) reactions used as neutron sources. The fission fragments were registered by a twin ionization chamber. The measured energy dependence curve of the fission cross section ratios was calibrated by means of an auxiliary technique employing glass detectors. The quantity ratio of the fissioning nuclei in 239Pu- and 235U layers was determined by two independent methods: from the alpha-activity in the layers and by taking measurements in the reactor thermal column. The total errors in the measured results makes up 1.4 to 1.5% for the most portion of the investigated neutron energy range, while rowing up to 1.7 to 2% in the range below 100 keV

  13. Early retention and distribution of monomeric 237Pu(IV) and 239Pu(IV) in C57BL/Do mice

    The early metabolism of monomeric Pu may depend upon its in vivo concentration, since in higher concentrations it may polymerize forming radiocolloids and be subject to phagocytosis. In this study the early biological behavior of 237Pu(IV) and 239Pu(IV), administered by intraperitoneal injection in citrate solution into C57BL/Do mice, is compared with the in vivo concentrations of these two nuclides differing by a factor of 105. 237Pu is also used as a γ-ray tracer of the α-emitting 239Pu in order to determine the latter's biological retention and tissue distribution. The results show no significant difference in the metabolism of the two nuclides throughout a 91 day serial sacrifice schedule. However, there is a significant sex dependence in the total body retention of Pu primarily due to a factor of 2.7 greater quantity of Pu excreted by the female during the first 24 hours post-injection. Furthermore, the half-time for removal of Pu from the livers of males is 42.7 +- 5.5 days and from livers of females 29.0 +- 2.7 days

  14. A study of 239Pu production rate in a water cooled natural uranium blanket mock-up of a fusion-fission hybrid reactor

    Feng, Song; Liu, Rong; Lu, Xinxin; Yang, Yiwei; Xu, Kun; Wang, Mei; Zhu, Tonghua; Jiang, Li; Qin, Jianguo; Jiang, Jieqiong; Han, Zijie; Lai, Caifeng; Wen, Zhongwei

    2016-03-01

    The 239Pu production rate is important data in neutronics design for a natural uranium blanket of a fusion-fission hybrid reactor, and the accuracy and reliability should be validated by integral experiments. The distribution of 239Pu production rates in a subcritical natural uranium blanket mock-up was obtained for the first time with a D-T neutron generator by using an activation technique. Natural uranium foils were placed in different spatial locations of the mock-up, the counts of 277.6 keV γ-rays emitted from 239Np generated by 238U capture reaction were measured by an HPGe γ spectrometer, and the self-absorption of natural uranium foils was corrected. The experiment was analyzed using the Super Monte Carlo neutron transport code SuperMC2.0 with recent nuclear data of 238U from the ENDF/B-VII.0, ENDF/B-VII.1, JENDL-4.0u2, JEFF-3.2 and CENDL-3.1 libraries. Calculation results with the JEFF-3.2 library agree with the experimental ones best, and they agree within the experimental uncertainty in general with the average ratios of calculation results to experimental results (C/E) in the range of 0.93 to 1.01.

  15. Alveolar macrophage kinetics after inhalation of 239PuO2 by CBA/Ca mice: Changes in synthesis of DNA

    For workers in the nuclear industry, the primary route for the entry of radioactive materials into the body is by inhalation, and the rate of clearance of particles from the pulmonary region of the lung is an important factor in determining radiation dose. It is the function of alveolar macrophages (AM) to maintain the sterility of the lung and to remove insoluble particles from the respiratory surfaces and airways. The AM population is not static, and under normal conditions the loss of macrophages from the alvoli via the conducting airways is balanced by renewal. In this investigation the effects of inhaled 239PuO2 (plutonium dioxide) particles on the synthesis of DNA by AM were studied at times up to 77 days after exposure. We also measured the number of cells recovered by bronchoalveolar lavage and the incidence of AM with nuclear aberrations. The latter provides a sensitive indicator of the effects of radiation. One of the earliest effects observed after exposure to 239PuO2 is a reduction in the number of AM recovered by lavage. This reduction is associated with a 3-fold reduction in the proportion of AM undergoing DNA synthesis at early times after exposure. The overall mean pulse labeling index of AM recovered from sham-exposed mice is 1.68%, and no trends is observed with time. At later times after exposure there is a concurrent increase both in the number of AM recovered by lavage and the proportion of AM in the S-phase of the cell cycle. This repopulation of the AM pool is associated with an increase in the incidence of AM with nuclear aberrations. The results of this study are consistent with the theory of an intrapulmonary pool of proliferating macrophages. The depletion of the AM pool and the latency in the induction of nuclear aberrations after exposure to 239PuO2 can be attributed to a radiation-induced inhibition of cell division in addition to interphase death of AM. 57 refs., 4 figs

  16. Migration Simulation of 239 Pu in Groundwater From Melt Glass%熔岩玻璃体239Pu在地下水中的迁移模拟研究

    包敏; 王群书

    2014-01-01

    针对内华达核试验场CHESHIRE地下核试验状况和近场水文地质参数,建立了熔岩玻璃体239 Pu的溶解释放和迁移模型。估算了熔岩玻璃体释放产生239 Pu的速率,将释放出的239 Pu分为溶解态和胶体态,以软件FEFLOW作为建模工具,数值模拟了10万年内溶解态239 Pu和胶体态239 Pu在地下水中的污染羽分布。模拟结果表明,溶解态239 Pu不能发生远距离迁移,影响迁移的关键参数是分配系数,当分配系数大于10 mL/g后,可忽略溶解态239 Pu的远距离迁移;胶体态239 Pu在爆心下游形成较固定的污染晕,距爆心1.3 km处的胶体态239 Pu的模拟活度浓度长期处于10-2 Bq/L ;影响胶体态239 Pu迁移的主要因素包括熔岩玻璃体的溶解速度、熔岩玻璃体释放239 Pu形成胶体态239 Pu的比例、岩层渗透系数。由模拟结果可见,只有当239 Pu形成胶体粒子后才可能发生远距离迁移。%According to the circumstances of an underground nuclear test CHESHIRE at the Nevada Test Site ,a model was developed to simulate the dissolution and migration of 239 Pu from melt glass in groundwater .The release rate of 239 Pu was calculated and the released 239 Pu was divided into dissolved fraction and colloid fraction . The pollution plumes for dissolved 239 Pu and colloid 239 Pu were simulated in 100 000 years by software FEFLOW .The results show that the dissolved 239 Pu can’t migration far away from the melt glass and sorption coefficient is the key parameter .If sorption coefficient is more than 10 mL/g ,the long distance migration of dissolved 239 Pu can be ignored .The colloid 239 Pu plume will be long-standing in the downstream of the melt glass .The 239 Pu con-centration at 1.3 km away from the melt glass would be 10-2 Bq/L for a long time .The parameters effecting colloid 239 Pu migration are the melt glass release rate ,the colloid fraction ratio and aquifer conductivity .It can be concluded

  17. Role of self-irradiation defects on the ageing of {sup 239}PuCoGa{sub 5}

    Jutier, F.; Griveau, J.C.; Colineau, E.; Wastin, F.; Rebizant, J.; Boulet, P.; Wiss, T.; Thiele, H. [European Commiss, Joint Res Ctr, Inst Transuranium Elements, D-76125 Karlsruhe, (Germany); Van der Beek, C.J. [CEA Saclay, DSM/DRECAM/LSI, CEA-CNRS-Ecole Polytechnique, UMR 7642, Lab Solides Irradies, F-91191 Gif-sur-Yvette, (France); Simoni, E. [Institut de Physique Nucleaire, F-91406 Orsay Cedex, (France)

    2007-06-15

    Low-temperature accumulation and annealing experiments, in conjunction with electrical resistivity and critical current density measurements, were used to study the ageing of the actinide superconductor PuCoGa{sub 5}. These measurements reveal that 2-nm-sized non-superconducting point-like regions are the main damages formed during room temperature ageing; smaller point-like defects are irrelevant to transport properties. Defect sizes and densities deduced from experiment agree with Transmission Electron Microscopy observations. (authors)

  18. Simultaneous measurement of 239Pu, 240Pu, 241Pu, and 242Pu by high resolution inductively coupled plasma mass spectrometer (HR ICP-MS) in marine sediments

    Transuranics elements are of particular interest in radioecological studies because of their radiotoxicity and their potential use to decipher source fingerprints and transport processes. The simultaneous measurement of 239Pu, 240Pu, 241Pu, and 242Pu in environmental samples requires a specific chemical procedure. This work deals with an analytical procedure which yields a very high grade of purification of Pu suitable for ultra low level detection by HR ICP-MS, from marine sediments. After the elimination of major elements (Fe, Al, Mg...) by a first chromatographic separation, a new device of purification by solvent extraction and concentration by a second chromatographic separation is used to obtain a concentrated and high purified solution of plutonium. The chemical procedure have been validated on IAEA certified sediment samples and on sediment samples collected in the roads of Cherbourg which had been previously analysed by other techniques (a spectrometry and thermo-ionisation mass spectrometer). (author)

  19. Estimating Reaction Cross Sections from Measured (Gamma)-Ray Yields: The 238U(n,2n) and 239Pu(n,2n) Cross Sections

    Younes, W

    2002-11-18

    A procedure is presented to deduce the reaction-channel cross section from measured partial {gamma}-ray cross sections. In its simplest form, the procedure consists in adding complementary measured and calculated contributions to produce the channel cross section. A matrix formalism is introduced to provide a rigorous framework for this approach. The formalism is illustrated using a fictitious product nucleus with a simple level scheme, and a general algorithm is presented to process any level scheme. In order to circumvent the cumbersome algebra that can arise in the matrix formalism, a more intuitive graphical procedure is introduced to obtain the same reaction cross-section estimate. The features and limitations of the method are discussed, and the technique is applied to extract the {sup 235}U (n,2n) and {sup 239}Pu(n,2n) cross sections from experimental partial {gamma}-ray cross sections, coupled with (enhanced) Hauser-Feshbach calculations.

  20. Neutron induced fission cross section ratios for 232Th, /sup 235,238/U, 237Np, and 239Pu from 1 to 400 MeV

    Time-of-flight measurements of neutron induced fission cross section ratios for 232Th, /sup 235,238/U, 237Np, and 239Pu, were performed using the WNR high intensity spallation neutron source located at Los Alamos National Laboratory. A multiple-plate gas ionization chamber located at a 20-m flight path was used to simultaneously measure the fission rate for all samples over the energy range from 1 to 400 MeV. Because the measurements were made with nearly identical neutron fluxes, we were able to cancel many systematic uncertainties present in previous measurements. This allows us to resolve discrepancies among different data sets. In addition, these are the first neutron-induced fission cross section values for most of the nuclei at energies above 30 MeV. 8 refs., 3 figs

  1. Aerosol sampling and characterization for hazard evaluation. Progress report, October 1, 1977-September 30, 1978. [/sup 239/Pu aerosol monitor performance in work area

    Scripsick, R.C.; Tillery, M.I.; Stafford, R.G.; Romero, P.O.

    1979-11-01

    Measurements of the dilution of air contaminants between worker breathing zone and area air samplers were made by releasing a test fluorescent aerosol in workrooms equipped with aerosol surveillance systems. These data were used to evaluate performance and suggest improvements in design of alarming air monitor systems. In one workroom studied, average half-hour breathing zone air concentration needed to trigger alarm was found to be 960 times the maximum permissible air concentration for occupational exposure to soluble /sup 239/Pu (MPC/sub a/). It was shown that alternative monitor placement in this room could result in decreasing average triggering concentration to 354 times the MPC/sub a/. Analysis of data from impaction-autoradiographic sizing comparison studies showed average disintegration to track ratio called track efficiency factor, to be 2.7 +- 0.4.

  2. Transmutation of 129I, 237Np, 238Pu, 239Pu, and 241Am using neutrons produced in target-blanket system `Energy plus Transmutation' by relativistic protons

    J Adam; K Katovsky; A Balabekyan; V G Kalinnikov; M I Krivopustov; H Kumawat; A A Solnyshkin; V I Stegailov; S G Stetsenko; V M Tsoupko-Sitnikov; W Westmeier

    2007-02-01

    Target-blanket facility `Energy + Transmutation' was irradiated by proton beam extracted from the Nuclotron Accelerator in Laboratory of High Energies of Joint Institute for Nuclear Research in Dubna, Russia. Neutrons generated by the spallation reactions of 0.7, 1.0, 1.5 and 2 GeV protons and lead target interact with subcritical uranium blanket. In the neutron field outside the blanket, radioactive iodine, neptunium, plutonium and americium samples were irradiated and transmutation reaction yields (residual nuclei production yields) have been determined using -spectroscopy. Neutron field's energy distribution has also been studied using a set of threshold detectors. Results of transmutation studies of 129I, 237Np, 238Pu, 239Pu and 241Am are presented.

  3. 133Ba as a gamma-ray surrogate source for 1kg HEU and 10g 239Pu and 252Cf as a Neutron Surrogate for Pu

    Monte Carlo was performed for the purpose of relating gamma-ray signal strength from 1kg of HEU and 10g of 239Pu (as described in the ASTM standards) to the radiation emitted from an amount of 133Ba. A determination was made on the amount of 133Ba that could act as a surrogate for the specified amounts of HEU and Pu. 133Ba is not the ideal source to use as a surrogate for HEU because of its higher energies. 133Ba was chosen as the surrogate since it has a half-life of 10.54 years, rather then the more ideal surrogate of 57Co which has a half-life of 271 days. A similar Monte Carlo was performed for the purpose of relating neutron signal strength from 200g of Pu (as described in the ASTM standards) to the radiation emitted from an amount of shielded 252Cf. A determination was made on the amount of 252Cf necessary to act as a surrogate for the 200g of Pu. An ASTM standard source is a metallic sphere, cube, or right cylinder of SNM having maximum self-attenuation of its emitted radiation. For plutonium, the source should be at least 93% 239Pu, less than 6.5% 240Pu, and less than 0.5% impurities. A cadmium filter of at least 0.08cm thick should be used to reduce the impact of 241Am. For uranium, the source should contain at least 95% 235U and less than 0.25% impurities. For neutron detector testing, the neutron source shall be placed in a lead shielding container that reduces the gamma radiation from the source to 1% of its unshielded value

  4. In vivo measurement of actinides in the human lung

    The problems associated with the in vivo detection and measurement of actinides in the human lung are discussed together with various measurement systems currently in use. In particular, the methods and calibration procedures employed at the Lawrence Livermore Laboratory, namely, the use of twin Phoswich detectors and a new, more realistic, tissue-equivalent phantom, are described. Methods for the measurement of chest-wall thickness, fat content, and normal human background counts are also discussed. Detection-efficiency values and minimum detectable activity estimates are given for three common actinides, 238Pu, 239Pu, and 241Am

  5. Radionuclide concentrations in soils and vegetation at Low-Level Radioactive Waste Disposal Area G during the 1998 growing season (with a cumulative summary of 3H and 239Pu over time)

    Soils and unwashed overstory and understory vegetation were collected at eight locations within and around Area G, a disposal facility for low-level, radioactive solid waste at Los Alamos National Laboratory. The samples were analyzed for 3H, 238Pu, 239Pu, 90Sr, 241Am, 137Cs, totU. Most of the radionuclide concentrations in soils and vegetation were within the upper 95% level of background concentrations except for 3H and 239Pu. Tritium concentrations in vegetation from most sites were greater than background concentrations of about 2 pCi mL-1. The concentrations of 239Pu in soils and understory vegetation were largest in samples collected several meters north of the transuranic waste pad area and were consistent with previous results. Based on 3H and 239Pu data through 1998, it was shown that concentrations were (1) significantly greater than background concentrations (p < 0.05) in soils and vegetation collected from most locations at Area G, and (2) there was no systematic increase or decrease in concentrations with time apparent in the data

  6. Radionuclide concentrations in soils and vegetation at Low-Level Radioactive Waste Disposal Area G during the 1998 growing season (with a cumulative summary of {sup 3}H and {sup 239}Pu over time)

    P. R. Fresquez; M. H. Ebinger; R. J. Wechsler; L. Naranjo, Jr.

    1999-11-01

    Soils and unwashed overstory and understory vegetation were collected at eight locations within and around Area G, a disposal facility for low-level, radioactive solid waste at Los Alamos National Laboratory. The samples were analyzed for {sup 3}H, {sup 238}Pu, {sup 239}Pu, {sup 90}Sr, {sup 241}Am, {sup 137}Cs, {sup tot}U. Most of the radionuclide concentrations in soils and vegetation were within the upper 95% level of background concentrations except for {sup 3}H and {sup 239}Pu. Tritium concentrations in vegetation from most sites were greater than background concentrations of about 2 pCi mL{sup {minus}1}. The concentrations of {sup 239}Pu in soils and understory vegetation were largest in samples collected several meters north of the transuranic waste pad area and were consistent with previous results. Based on {sup 3}H and {sup 239}Pu data through 1998, it was shown that concentrations were (1) significantly greater than background concentrations (p < 0.05) in soils and vegetation collected from most locations at Area G, and (2) there was no systematic increase or decrease in concentrations with time apparent in the data.

  7. Minior Actinide Doppler Coefficient Measurement Assessment

    Nolan E. Hertel; Dwayne Blaylock

    2008-04-10

    The "Minor Actinide Doppler Coefficient Measurement Assessment" was a Department of Energy (DOE) U-NERI funded project intended to assess the viability of using either the FLATTOP or the COMET critical assembly to measure high temperature Doppler coefficients. The goal of the project was to calculate using the MCNP5 code the gram amounts of Np-237, Pu-238, Pu-239, Pu-241, AM-241, AM-242m, Am-243, and CM-244 needed to produce a 1E-5 in reactivity for a change in operating temperature 800C to 1000C. After determining the viability of using the assemblies and calculating the amounts of each actinide an experiment will be designed to verify the calculated results. The calculations and any doncuted experiments are designed to support the Advanced Fuel Cycle Initiative in conducting safety analysis of advanced fast reactor or acceoerator-driven transmutation systems with fuel containing high minor actinide content.

  8. Actinides AMS at CIRCE and 236U and Pu measurements of structural and environmental samples from in and around a mothballed nuclear power plant

    De Cesare, M.; Fifield, L. K.; Sabbarese, C.; Tims, S. G.; De Cesare, N.; D'Onofrio, A.; D'Arco, A.; Esposito, A. M.; Petraglia, A.; Roca, V.; Terrasi, F.

    2013-01-01

    Accelerator mass spectrometry (AMS) is presently the most sensitive technique for the measurement of long-lived actinides, e.g. 236U and 239Pu. A new actinide line is in operation at the Center for Isotopic Research on Cultural and Environmental heritage (CIRCE) in Caserta, Italy. Using the actinide line a uranium mass sensitivity of around 4 μg has been reached measuring with a 16-strip silicon detector, and a 239Pu background level of below 0.1 fg has been obtained. In this work we also discuss preliminary results for environmental and structural samples from in and around the Garigliano nuclear power plant (GNPP), presently in the decommissioning phase. Measurements on environmental samples from the vicinity of the plant allow the assessment of contamination, if any, over the years. Measurements of structural samples from the plant are relevant to the optimization of the decommissioning program for the GNPP.

  9. Actinides AMS at CIRCE and 236U and Pu measurements of structural and environmental samples from in and around a mothballed nuclear power plant

    Accelerator mass spectrometry (AMS) is presently the most sensitive technique for the measurement of long-lived actinides, e.g. 236U and 239Pu. A new actinide line is in operation at the Center for Isotopic Research on Cultural and Environmental heritage (CIRCE) in Caserta, Italy. Using the actinide line a uranium mass sensitivity of around 4 μg has been reached measuring with a 16-strip silicon detector, and a 239Pu background level of below 0.1 fg has been obtained. In this work we also discuss preliminary results for environmental and structural samples from in and around the Garigliano nuclear power plant (GNPP), presently in the decommissioning phase. Measurements on environmental samples from the vicinity of the plant allow the assessment of contamination, if any, over the years. Measurements of structural samples from the plant are relevant to the optimization of the decommissioning program for the GNPP.

  10. Decay Heat Analyses after Thermal-Neutron Fission of 235U and 239Pu by SCALE-6.1.3 with Recently Available Fission Product Yield Data

    The heat reaches about 1.5% after one hour and falls to 0.4% after a day. After a week it will be about 0.2%. The reactor, however, still requires further cooling for several years to keep the fuel rods safe. In general, the decay heat in the reactors can be calculated using a summation calculation method, which is simply the sum of the activities of the fission products produced during the fission process and after the reactor shutdown weighted by the mean decay energies. Consequently, the method is strongly dependent on the available nuclear structure data. Nowadays, the method has been implemented in various burnup and depletion programs such as ORIGEN and CINDER. In this study, the decay heat measurements after thermal-neutron fission of 235U and 239Pu have been evaluated by the ORIGEN-S with the decay data and fission product yield libraries included in the SCALE-6.1.3 software package. The new libraries were applied to the decay heat calculations, and the results were compared with those by the ORIGEN reference calculation. The decay heat measurements for very short cooling times after thermal-neutron fission of 235U and 239Pu have been evaluated by the ORIGEN-S summation calculation. The reference calculation results by the latest ORIGEN data libraries of the SCALE-6.1.3 have been validated with the measurements by ORNL and Studsvik. In addition, the generation of the new ORIGEN yield libraries has been completed based on the ENDF/B-VII.1, JEFF-3.1.1, JENDL/FPY-2011, and JENDL-4.0. The new libraries have been successfully applied to the decay heat calculations and comparative analyses have been devoted to verifying the importance of the fission product yield data when estimating the decay heat values for each isotope in a very short time. The decay data library occupies an important position in the ORIGEN summation calculation along with the fission product yield library

  11. A comparison of the natural survival of beagle dogs injected intravenously with low levels of 239Pu, 226Ra, 228Ra, 228Th, or 90Sr

    The natural survival, relative to properly chosen controls, of 26 beagle dogs injected once intravenously with an average of 0.58 +/- 0.04 kBq 239Pu/kg, 23 dogs injected with 2.31 +/- 0.43 kBq 226Ra/kg, 13 dogs injected with 1.84 +/- 0.26 kBq 228Ra/kg, 12 dogs injected with 0.56 +/- 0.030 kBq 228Th/kg, and 12 dogs injected with 21.13 +/- 1.74 kBq 90Sr/kg was evaluated statistically. The amounts of these radionuclides are related directly to the estimated maximum permissible body burdens for humans suggested in ICRP II (1959). They constitute a level of exposure that initially was assumed to cause no deleterious effects in dogs. This study had two objectives: (1) identification of homogeneous control groups against which to evaluate the survival of the irradiated groups and (2) comparison of the survival characteristics and estimation of mortality or hazard rate ratios for control dogs vs dogs injected with the baseline dosages given above. It was shown, by goodness-of-fit plots, that the Cox proportional hazards model was an appropriate method of analysis. Therefore, covariates that possibly could influence survival were tested for significance. Only the effects of grand mal seizure, which is caused in epileptic dogs by an external stimulus and can be fatal if untreated, were significant (P less than 0.0001). Consequently, in the final model, death from grand mal seizure was considered as accidental. After censoring the dogs dying from grand mal seizure, it was established that the data for the control groups from previous and contemporary experiments could be pooled. The change in hazard rates relative to controls resulting from exposure to the baseline radionuclide level was modest, 1.6 times for 239Pu (P = 0.033), 1.0(4) for 226Ra (P = 0.86), 1.9 for 228Ra (P = 0.035), 2.5 for 228Th (P less than 0.001), and 0.52 for 90Sr (P = 0.041)

  12. Comparative effects of protracted exposures to 60Co γ-radiation and 239Pu α-radiation on breeding performance in female mice

    Breeding performances are compared of hybrid female mice given 239Pu(5 or 10μCikg-1 body mass in 1 per cent trisodium citrate via the tail-vein), or kept in a 10rad/day or 20rad/day 60Co γ-irradiation field (but mated in the control area), or unirradiated. Ovarian dose-rates from the injected plutonium were initially 0.8 and 1.7 rad/day, changing little thereafter; actual γ-ray dose-rates to breeding females averaged around 8 and 16 rad/day respectively. Both γ-ray treatments affected reproductive performance more than the plutonium injections, with respect to duration of fertility and to offspring per litter in successive 4-weekly periods, though overall mean litter-sizes were not significantly less than controls. The r.b.e. for these effects on reproduction, attributed to germ-cell killing, is about 2.5 for the α particles vs. γ-rays, lower than for testis mass reduction in males. This low r.b.e. may be connected with inhomogeneity of α-particle dose within the ovary, but it is known that fission neutron versus gamma r.b.e.'s for impairment of female fertility are also lower than those for impairment of male fertility. (Author)

  13. Study of High-Resolution Spectroscopy of Plutonium. Part I. Contribution to the Classification of the Arc Spectrum. Part II. Determination of the Magnetic Moment of 239Pu

    The study of the hyperfine structure and isotope shift enabled the positions of the first five levels of the multiplet 7F0-6 belonging to the fundamental configuration 5f67s2 to be determined. The classification of the arc spectrum begun in this way led to 25 odd levels, the number of classified lines (70) representing about 30 p. 100 of the light emitted by this hollow cathode in the visible. In addition, the isotope shifts of many lines and the data given by the King furnace show that the first levels of the configuration 5f56d7s2 are also low less than 8000 cm-1 above the fundamental level 7F0. The proximity of the configuration f6s2 and f5ds2 shows that the bonding energies of the 5f and 6d electrons are of the same order of magnitude and this fact must be responsible for the multiple valences belonging to plutonium. From the hyperfine structure of spark lines (Pu II) the interval factor a7 for the electron was deduced giving for the calculated nuclear moment of 239Pu a value of +0.21 ±0.06 μN. The position of the hyperfine components show that the nuclear moment is positive, although the theoretical value given by B. R. Mottelson and S. Nillson is negative and equal to -0.1 μN. (author)

  14. Use of faecal excretion function for quick estimation of initial and existing lung burden for occupational exposure control due to 239Pu for S-class of intake

    Two functions namely initial lung deposition and lung retention per unit faecal excretion rate are constructed primarily based on the excretion pattern of four subjects exposed to 239Pu. In the absence of initial clear knowledge about the class of compound inhaled, faecal to urine excretion ratio was used to infer the type of inhaled class. Trends in the urine and faecal data had suggested that the intake was due to mixed class of plutonium compound for each case. With the assumption of 1:1 mixture of plutonium M and S class inhaled compound, faecal excretion rates for only S-class intake were worked out. Uptake inferred based on their urinary data had suggested it to be of similar level within 40% of uncertainty for 5 μm particle size distribution. Data, all the four cases, were pooled for analysis citing the similar level of intake, particle size distribution, nature and pattern of work. The function obtained was tested for S-class lung retention and faecal excretion rate value. These functions are handy tool for estimating initial lung burden and lung retention value for low level of S-class plutonium intake based on subject faecal analysis data. (authors)

  15. Estimation of multi-group cross section covariances for 235,238U, 239Pu, 241Am, 56Fe, 23Na and 27Al

    This paper presents the methodology used to estimate multi-group covariances for some major isotopes used in reactor physics. The starting point of this evaluation is the modelling of the neutron induced reactions based on nuclear reaction models with parameters. These latest are the vectors of uncertainties as they are absorbing uncertainties and correlation arising from the confrontation of nuclear reaction model to microscopic experiment. These uncertainties are then propagated towards multi-group cross sections. As major breakthroughs were then asked by nuclear reactor physicists to assess proper uncertainties to be used in applications, a solution is proposed by the use of integral experiment information at two different stages in the covariance estimation. In this paper, we will explain briefly the treatment of all type of uncertainties, including experimental ones (statistical and systematic) as well as those coming from validation of nuclear data on dedicated integral experiment (nuclear data oriented). We will illustrate the use of this methodology with various isotopes such as 235,238U, 239Pu, 241Am, 56Fe, 23Na and 27Al. (authors)

  16. The Association of Inbreeding With Lung Fibrosis Incidence in Beagle Dogs That Inhaled 238PuO2 or 239PuO2.

    Wilson, Dulaney A.; Brigantic, Andrea M.; Morgan, William F.

    2011-09-12

    Studies of health effects in animals after exposure to internally deposited radionuclides were intended to supplement observational studies in humans. Both nuclear workers and Beagle dogs have exhibited plutonium associated lung fibrosis; however, the dogs smaller gene pool may limit the applicability of findings to humans. Data on Beagles that inhaled either plutonium-238 dioxide (238PuO2) or plutonium-239 dioxide (239PuO2) were analyzed. Wright's Coefficient of Inbreeding was used to measure genetic or familial susceptibility and was assessed as an explanatory variable when modeling the association between lung fibrosis incidence and plutonium exposure. Lung fibrosis was diagnosed in approximately 80% of the exposed dogs compared with 23.7% of the control dogs. The maximum degree of inbreeding was 9.4%. Regardless of isotope, the addition of inbreeding significantly improved the model in female dogs but not in males. In female dogs an increased inbreeding coefficient predicted decreased hazard of a lung fibrosis diagnosis. Lung fibrosis was common in these dogs with inbreeding affecting models of lung fibrosis incidence in females but not in males. The apparent protective effect in females predicted by these models of lung fibrosis incidence is likely to be minimal given the small degree of inbreeding in these groups.

  17. Speciation analysis of 129I, 137Cs, 232Th, 238U, 239Pu and 240Pu in environmental soil and sediment

    The environmental mobility and bioavailability of radionuclides are related to their physicochemical forms, namely species. We here present a speciation analysis of important radionuclides including 129I (also 127I), 137Cs, 232Th, 238U and plutonium isotopes (239Pu and 240Pu) in soil (IAEA-375) and sediment (NIST-4354) standard reference materials and two fresh sediment samples from Øvre Heimdalsvatnet Lake, Norway. A modified sequential extraction protocol was used for the speciation analysis of these samples to obtain fractionation information of target radionuclides. Analytical results reveal that the partitioning behaviour, and thus the potential mobility and bioavailability, are exclusively featured for the individual radionuclide. Iodine is relatively mobile and readily binds to organic matter, while plutonium is mainly bound to both organic matter and nitric acid leachable fractions. Thorium is predominated in nitric acid leachable fraction and caesium is primarily observed in nitric acid and aqua regia leachable fractions and residue. Our analytical results reveal that around 50% of uranium might still remain in the residue which could not be extracted with aggressive acid, namely, aqua regia.

  18. Microdistribution and Long-Term Retention of 239Pu (NO3)4 in the Respiratory Tracts of an Acutely Exposed Plutonium Worker and Experimental Beagle Dogs

    Nielsen, Christopher E.; Wilson, Dulaney A.; Brooks, Antone L.; McCord, Stacey; Dagle, Gerald E.; James, Anthony C.; Tolmachev, Sergei Y.; Thrall, Brian D.; Morgan, William F.

    2012-11-01

    The long-term retention of inhaled soluble forms of plutonium raises concerns as to the potential health effects in persons working in nuclear energy or the nuclear weapons program. The distributions of long-term retained inhaled plutonium-nitrate [239Pu (NO3)4] deposited in the lungs of an accidentally exposed nuclear worker (Human Case 0269) and in the lungs of experimentally exposed beagle dogs with varying initial lung depositions were determined via autoradiographs of selected histological lung, lymph node, trachea, and nasal turbinate tissue sections. These studies showed that both the human and dogs had a non-uniform distribution of plutonium throughout the lung tissue. Fibrotic scar tissue effectively encapsulated a portion of the plutonium and prevented its clearance from the body or translocation to other tissues and diminished dose to organ parenchyma. Alpha radiation activity from deposited plutonium in Human Case 0269 was observed primarily along the sub-pleural regions while no alpha activity was seen in the tracheobronchial lymph nodes of this individual. However, relatively high activity levels in the tracheobronchial lymph nodes of the beagles indicated the lymphatic system was effective in clearing deposited plutonium from the lung tissues. In both the human case and beagle dogs, the appearance of retained plutonium within the respiratory tract was inconsistent with current biokinetic models of clearance for soluble forms of plutonium. Bound plutonium can have a marked effect on the dose to the lungs and subsequent radiation exposure has the potential increase in cancer risk.

  19. Capture and Fission rate of 232-Th, 238-U, 237-Np and 239-Pu from spallation neutrons in a huge block of lead.

    Vlachoudis, Vasilis

    2000-01-01

    The study is centered on the research of the incineration possibility of nuclear waste, by the association of a particle accelerator with a multiplying medium of neutrons, in the project "Energy Amplifier" of C. Rubbia. It consists of the experimental determination of the rates of capture and fission of certain elements (232-Th, 238-U, 237-Np and 239-Pu) subjected to a fluence of fast spallation neutrons. These neutrons are produced by the interaction of high kinetic energy protons (several GeV) provided by the CERN-PS accelerator, on a large lead solid volume. The measurement techniques used in this work, are based on the activation of elements in the lead volume and the subsequent gamma spectroscopy of the activated elements, and also by the detection of fission fragment traces. The development, of a Monte Carlo code makes it possible, on one hand, to better understand the relevant processes, and on the other hand, to validate the code, by comparison with measurements, for the design and the construction of...

  20. Ultra-sensitive Mass Spectrometric and Other Advanced Methods Applied to Biological Samples. Second interlaboratory comparison study for the analysis of 239Pu in synthetic urine at the μBq (∼100 aCi) level by mass spectrometry

    As a follow up to the initial 1998 intercomparison study, a second study was initiated in 2001 as part of the ongoing evaluation of the capabilities of various ultra-sensitive methods to analyze 239Pu in urine samples. The initial study was sponsored by the Department of Energy, Office of International Health Programs to evaluate and validate new technologies that may supersede the existing fission tract analysis (FTA) method for the analysis of 239Pu in urine at the μBq/l level. The ultra-sensitive techniques evaluated in the second study included accelerator mass spectrometry (AMS) by LLNL, thermal ionization mass spectrometry (TIMS) by LANL and FTA by the University of Utah. Only the results for the mass spectrometric methods will be presented. For the second study, the testing levels were approximately 4, 9, 29 and 56 μBq of 239Pu per liter of synthetic urine. Each test sample also contained 240Pu at a 240Pu/239Pu atom ratio of ∼0.15 and natural uranium at a concentration of 50 μBq/ml. From the results of the two studies, it can be inferred that the best performance at the μBq level is more laboratory specific than method specific. The second study demonstrated that LANL-TIMS and LLNL-AMS had essentially the same quantification level for both isotopes. Study results for bias and precision and acceptable performance compared to ANSI N13.30 and ANSI N42.22 have been compiled. (author)

  1. Statistical evaluation of lung, bone, and liver tumors in rats exposed to aerosols of 238PuO2, 239PuO2, and 244CmO2

    The Mantel--Haenszel procedure was applied to the evaluation of tumor data from exposures to aerosols of 238PuO2, 239PuO2, and 244CmO2. Significance was evident for lung tumors for all three transuranics, for osteosarcomas in animals exposed to 244CmO2, and was suggested for liver tumors in animals exposed to 244CmO2

  2. Procedures for the use of Lexan and Makrofol SSNTDs in the detection of environmental concentrations of 235U and 239Pu

    Solid State Nuclear Track Detectors are used to study a variety of atomic particles. Polycarbonate SSNTD is used to study environmental concentrations of 235U and 239Pu in human urine and feces through fission track analysis. The samples of interest are deposited upon a Lexan slide, covered with a piece of Makrofol and exposed to a neutron fluence of 1.1 X 1017. The fissile isotopes in the sample fission and the resulting fission fragments pass through either the surface of the Lexan or the surface of the Makrofol. The positive Coulombic attraction of the ionized fission fragments causes the electrons of the polycarbonate lattice to move towards the path of these particles, resulting in the breakage of chemical bonds in the lattice. The detector is then chemically etched in 6.5 N KOH that preferentially dissolves the damaged polycarbonate left in the path of the fission fragment. The chemically etched fission tracks are permanent records of the path of the fission fragment. The etched fission tracks in Lexan are optically counted using a microscope and the fission tracks in Makrofol are counted using a Spark Chamber. The amount of fissile material in the original sample can be calculated from the number of fission tracks. This paper presents further details of procedures for etching fission tracks in Lexan and Makrofol and for operating a Spark Chamber to count etched fission tracks in Makrofol. The physics of fission track formation in dielectric detectors is also discussed, as well as the physics of the Spark Chamber

  3. Evaluation of the {sup 239}Pu prompt fission neutron spectrum induced by neutrons of 500 keV and associated covariances

    Neudecker, D., E-mail: dneudecker@lanl.gov [Theoretical Division, Los Alamos National Laboratory, P.O. Box 1663, MS-B283, NM 87545 (United States); Talou, P., E-mail: talou@lanl.gov [Theoretical Division, Los Alamos National Laboratory, P.O. Box 1663, MS-B283, NM 87545 (United States); Kawano, T., E-mail: kawano@lanl.gov [Theoretical Division, Los Alamos National Laboratory, P.O. Box 1663, MS-B283, NM 87545 (United States); Smith, D.L., E-mail: donaldlarnedsmith@gmail.com [Nuclear Engineering Division, Argonne National Laboratory, 1710 Avenida del Mundo #1506, Coronado, CA 92118 (United States); Capote, R., E-mail: r.capotenoy@iaea.org [Nuclear Data Section, International Atomic Energy Agency Vienna, Vienna International Centre, P.O. Box 100, A-1400 Vienna (Austria); Rising, M.E., E-mail: mrising@lanl.gov [X-Division, Los Alamos National Laboratory, P.O. Box 1663, MS-F663, NM 87545 (United States); Kahler, A.C., E-mail: akahler@lanl.gov [Theoretical Division, Los Alamos National Laboratory, P.O. Box 1663, MS-B283, NM 87545 (United States)

    2015-08-11

    We present evaluations of the prompt fission neutron spectrum (PFNS) of {sup 239}Pu induced by 500 keV neutrons, and associated covariances. In a previous evaluation by Talou et al. (2010), surprisingly low evaluated uncertainties were obtained, partly due to simplifying assumptions in the quantification of uncertainties from experiment and model. Therefore, special emphasis is placed here on a thorough uncertainty quantification of experimental data and of the Los Alamos model predicted values entering the evaluation. In addition, the Los Alamos model was extended and an evaluation technique was employed that takes into account the qualitative differences between normalized model predicted values and experimental shape data. These improvements lead to changes in the evaluated PFNS and overall larger evaluated uncertainties than in the previous work. However, these evaluated uncertainties are still smaller than those obtained in a statistical analysis using experimental information only, due to strong model correlations. Hence, suggestions to estimate model defect uncertainties are presented, which lead to more reasonable evaluated uncertainties. The calculated k{sub eff} of selected criticality benchmarks obtained with these new evaluations agree with each other within their uncertainties despite the different approaches to estimate model defect uncertainties. The k{sub eff} one standard deviations overlap with some of those obtained using ENDF/B-VII.1, albeit their mean values are further away from unity. Spectral indexes for the Jezebel critical assembly calculated with the newly evaluated PFNS agree with the experimental data for selected (n,γ) and (n,f) reactions, and show improvements for high-energy threshold (n,2n) reactions compared to ENDF/B-VII.1.

  4. Sensitivity of ICP-MS, PERALS and alpha spectrometry for the determination of actinides

    The purpose of this study was to compare the sensitivity of the three most popular techniques for the determination of minor actinides at environmental levels: ICP-MS, PERALS and solid state alpha spectrometry. For each method the limit of detection and the resolution were estimated in order to study the content and isotopic composition of the actinides. The sensitivities of the three determination techniques were compared. Two international reference materials, IAEA-135 (Irish Sea sediment) and IAEA-300 (Baltic Sea sediment) were analyzed for activity concentrations of 238Pu, 239Pu, 240Pu, 241Pu and 241Am. (authors)

  5. Study on Prompt Fission Neutron Spectra and Associated Covariances for 235U(nth,f) and 239Pu(nth,f)

    Berge, L.; Litaize, O.; Serot, O.; Jean, C. De Saint; Archier, P.; Peneliau, Y.

    normalization of experimental spectra, and the uncertainty on the energy-dependent neutron detection efficiency. We show the resulting PFNS and associated covariance matrix in the case of thermal neutron-induced fission of 235U and 239Pu.

  6. Anthropogenic Actinides in the Environment

    The use of nuclear energy and the testing of nuclear weapons have led to significant releases of anthropogenic isotopes, in particular a number of actinide isotopes generally not abundant in nature. Most prominent amongst these are 239Pu, 240Pu, and 236U. The study of these actinides in nature has been an active field of study ever since. Measurements of actinides are applied to nuclear safeguards, investigating the sources of contamination, and as a tracer for a number of erosion and hydrology studies. Accelerator Mass Spectrometry (AMS) is ideally suited for these studies and generally offers higher sensitivities than competing techniques, like ICP-MS or decay counting. Recent advances in AMS allow the study of “minor” plutonium isotopes (241Pu, 242Pu, and 244Pu). Furthermore, 236U can now be measured at the levels expected from the global stratospheric fall-out of the atmospheric nuclear weapon tests in the 1950s and 1960s. Even the pre-anthropogenic isotope ratios could be within reach. However, the distribution and abundance levels of these isotopes are not well known yet. I will present an overview of the field, and in detail two recent studies on minor plutonium isotopes and 236U, respectively.(author)

  7. ANSI/ANS-8.15-1981(R87): Nuclear criticality control of special actinide elements

    The American National Standard, open-quotes Nuclear Criticality Safety in Operations with Fissionable Materials Outside Reactotorsclose quotes American National Standards Institute/American Nuclear Society (ANSI/ANS)-8.1-1983(R88) provides guidance for the nuclides 233U, 235U, and 239Pu. These three nuclides are of primary interest in out-of-reactor criticality safety since they are the most commonly encountered in the vast majority of operations. However, some operations can involve nuclides other than 233U, 235U, and 239Pu in sufficient quantities that their effect on criticality safety could be of concern. ANSI/ANS-8.15-1981(R87) open-quotes Nuclear Criticality Control of Special Actinide Elements,close quotes provides guidance for 15 such nuclides. The standard was approved for use on November 9, 1981. When it received its first 5-yr review, no changes were made, and it was reaffirmed effective October 30, 1987. The standard was again reviewed and reaffirmed without changes in December 1995. The next 5-yr review of the standard is due in December 2000. The affected nuclides are 237Np, 238Pu, 240Pu, 242Pu, 241Am, 243Am, 244Cm, 239Pu, 241Pu, 242mAm, 243Cm, 245Cm, 247Cm, 249Cf, and 251Cf

  8. Detection of internally deposited actinides. Part II. Statistical techniques and risk analysis

    Since a considerable number of workers at Oak Ridge National Laboratory work with compounds of the transuranic elements, computer techniques have been developed to evaluate phoswich spectra in order to determine lung burdens following accidental inhalation of 239Pu, 241Am, 244Cm or other isotopes. Two unfolding methods which have been found useful in the analysis of such cases are presented and discussed. These techniques have been used successfully to detect low levels of 239Pu, 241Am, 244Cm, 233U, 90Sr, and 153Gd in contaminated workers; but because of the current importance of 239Pu, emphasis is placed on detection of that isotope in the presence of 241Am and natural human background. In the health physics tradition of emphasizing benefit vs. risk, we also analyze uncertainties inherent in external counting of the actinides from the viewpoint of statistical risk analysis and derive decision criteria which are useful in determining whether various radioactive species have, in fact, been detected. These criteria are somewhat different from those encountered using traditional counting statistics and derive from the realization that some errors will always be made in scanning large numbers of radiation workers. The optimum decision strategy for the determination of lung burden is, therefore, one which minimizes the long-term risk of error. The usefulness of this approach to whole body counting will be discussed and analyzed

  9. Simultaneous determination of radiocesium ((135)Cs, (137)Cs) and plutonium ((239)Pu, (240)Pu) isotopes in river suspended particles by ICP-MS/MS and SF-ICP-MS.

    Cao, Liguo; Zheng, Jian; Tsukada, Hirofumi; Pan, Shaoming; Wang, Zhongtang; Tagami, Keiko; Uchida, Shigeo

    2016-10-01

    Due to radioisotope releases in the Fukushima Dai-ichi Nuclear Power Plant (FDNPP) accident, long-term monitoring of radiocesium ((135)Cs and (137)Cs) and Pu isotopes ((239)Pu and (240)Pu) in river suspended particles is necessary to study the transport and fate of these long-lived radioisotopes in the land-ocean system. However, it is expensive and technically difficult to collect samples of suspended particles from river and ocean. Thus, simultaneous determination of multi-radionuclides remains as a challenging topic. In this study, for the first time, we report an analytical method for simultaneous determination of radiocesium and Pu isotopes in suspended particles with small sample size (1-2g). Radiocesium and Pu were sequentially pre-concentrated using ammonium molybdophosphate and ferric hydroxide co-precipitation, respectively. After the two-stage ion-exchange chromatography separation from the matrix elements, radiocesium and Pu isotopes were finally determined by ICP-MS/MS and SF-ICP-MS, respectively. The interfering elements of U ((238)U(1)H(+) and (238)U(2)H(+) for (239)Pu and (240)Pu, respectively) and Ba ((135)Ba(+) and (137)Ba(+) for (135)Cs and (137)Cs, respectively) were sufficiently removed with the decontamination factors of 1-8×10(6) and 1×10(4), respectively, with the developed method. Soil reference materials were utilized for method validation, and the obtained (135)Cs/(137)Cs and (240)Pu/(239)Pu atom ratios, and (239+240)Pu activities showed a good agreement with the certified/information values. In addition, the developed method was applied to analyze radiocesium and Pu in the suspended particles of land water samples collected from Fukushima Prefecture after the FDNPP accident. The (135)Cs/(137)Cs atom ratios (0.329-0.391) and (137)Cs activities (23.4-152Bq/g) suggested radiocesium contamination of the suspended particles mainly originated from the accident-released radioactive contaminates, while similar Pu contamination of suspended

  10. Field studies on the terrestrial behavior of actinide elements in East Tennessee

    Field studies on the comparative uptake of various actinide elements (232Th, 233U, 238U, 239Pu, 241Am, and 244Cm) by plants and animals inhabiting historically contaminated environments on the Oak Ridge National Laboratory (ORNL) reservation in East Tennessee are summarized. The present-day pattern of actinide element bioaccumulation from a flood plain site contaminated with Pu in 1944 is U > Th approx. Pu. Thus the environmentally dispersed 239Pu exhibits a transfer from floodplain soil to biota comparable to that of indigenous 232Th and less than that of the indigenous 238U. This ranking agrees with the chemical extractability of U, Th, and Pu from soil, using either weak acids or strongly basic reagents. The pattern of actinide element uptake from the shoreline of a historically contaminated pond is Pu 238U = 233U. This ranking also agrees with the chemical extractability of Pu, Am, Cm, and U from shoreline sediment, using weak acids. Results from field studies at ORNL agree with what has been generally inferred about the relative food chain transfer of the actinides, based on laboratory studies and field studies at other sites in the United States. Because they share the same valence state, there are apparent strong similarities in soil sorption, plant uptake, and animal uptake between trivalent Am and Cm and between tetravalent Pu and Th. Available evidence suggests that knowledge of the behavior of naturally occurring 232Th in the terrestrial food chain can be useful for predicting the long-term fate of environmentally dispersed 239Pu, while data on 238U might be used to place an upper limit on the expected long-term food chain transfer of all transuranic elements except Np. 33 references, 5 figures, 1 table

  11. Intensified proliferative activity of the CFU-S in vertebral bone marrow of 239Pu-treated mice as one of the factors involved in the induction of granulocytic leukemia

    Using the exocolonizing test, 59Fe utilization technique and classical cytology, 210 days after i.v. injection of 166.7 kBq of 239Pu/kg in about 30% of contaminated mice a proliferative activity was observed in vertebral bone marrow, characterized by high relative numbers of pluripotent hemopoietic stem cells, significantly higher than in the seriously damaged vertebral bone marrow of other 239Pu-treated mice and even higher than in untreated controls. Also the amount of cells in the granulocytic series increased. After transplantation to the heavily irradiated syngeneic hosts the stem cells differentiated into splenic colonies with higher iron utilization than in corresponding controls. Higher numbers of mature granulocytes were also found in the peripheral blood and the spleen. It is assumed that this activity was an inadequate reparative response of the hemopoietic stem cell compartment to the damaging effect and it is considered to be the critical phase which not only preceded the induction of granulocytic leukemia but also created conditions favorable for leukemic transformation of the hemopoietic stem cells. (author)

  12. Containment of actinides in zirconolite CaZrTi2O7 and alpha irradiation resistance

    Zirconolite is a potential inorganic matrix witch is currently investigated in order to provide durable containment of the trivalent and tetravalent minor actinides like neptunium, curium, americium and small quantities of un-recyclable plutonium separated from others nuclear wastes. To confirm the actinide loading capacity of the zirconolite structure and to study the physical and chemical stability of this type of crystalline structure when subjected to alpha self-irradiation, zirconolite ceramic pellets were fabricated with 10 wt% plutonium oxide. An initial pellet batch was fabricated in a glove box with 239PuO2 (half-life 24 000 years) in April 2002 (75.06 at% 239Pu, 0.18 at% 238Pu, 20.96 at% 240Pu, 3.12 at% 241Pu, 0.68 at% 242Pu). Another batch was fabricated in a hot cell with 238PuO2 (half-life 87 years) in July 2002 (83.56 at% 238Pu, 14.34 at% 239Pu, 1.83 at% 240Pu, 0.111 at% 241Pu, 0.152 at% 242Pu). The prepared pellets are dense (> 93.3% of the theoretical density on average) and free of cracks. They are characterized by a grain size of between 10 and 20 micrometers. X-ray diffraction analyses confirmed the presence of the zirconolite 2M crystalline structure. Actinides create irradiation damages (amorphization, He accumulation, etc.) in the zirconolite crystalline structure, as a result of alpha decays. The physical properties of 238Pu-zirconolite ceramics were characterized up to about 2 x 1018 αdecay/g. (authors)

  13. Rapid methods for determination of small amount of actinides in waste waters

    A rapid method of plutonium and actinide sum (Ac) (except uranium) determination in waste waters has been developed. For rapid isolation of 239Pu and Ac sum a method of extraction to iron hydroxide myomphate (IHM), consisting in Ac deposition on iron hydroxide, solvent extraction by monoisooctylmethylphosphinic acid and flotation of the disperse phase into solid extract of IHM, has been applied. The method permits to concentrate plutonium quantitatively from solutions in all of its forms, including colloid ones. For analysis of solid extracts α-spectroimetric instrumentation is used. The analysis sensitivity is 1 Bg/l, relative standard deviation - 0.3. 10 refs.; 1 fig.; 2 tabs

  14. Comparative food-chain behavior and distribution of actinide elements in and around a contaminated fresh-water pond

    The bioaccumulation of 233234U, 238U, 238Pu, 239240Pu, 241Am, and 244Cm in both native and introduced biota was studied at Pond 3513, a former low-level radioactive waste settling basin at Oak Ridge National Laboratory. This system, which was decommissioned in 1976 after more than 30 years use, contains approximately 5 Ci of 239240Pu; inventories of other actinide isotopes are considerably less. Significantly higher concentrations of actinides in fish that were allowed access to sediments indicated that sedimentary particulates may be the primary source of transuranics to biota in shallow fresh-water ecosystems. Our study determined habitat, in particular the degree of association of an organism with the sediment-water interface, to be the primary factor in controlling transuranic concentrations in aquatic biota. In most of the biological samples analyzed, excluding samples suspected of being contaminated by sediment, 241Am/239Pu, 244Cm/239Pu, and 238U/239Pu ratios were greater than the respective ratio in sediment while 233234U/238U, and 239240Pu/238Pu ratios were not different from the respective ratios in sediment. The relative uptake of actinides from contaminated sediment by aquatic and terrestrial biota at this site was U > Cm greater than or equal to Am > Pu. The relative extractability of actinides from shoreline sediment was U > Cm approx. = Am > Pu; we also observed the same relative ranking for sediment-water exchange in situ. Concentrations of transuranics in water, terrestrial vegetation, and vertebrate carcasses were less than 10% of the recommended public exposure maximum permissible concentration (MPC) of the ICRP

  15. Actinide inventory in Herndon’s georeactor operating throughout geologic time

    Highlights: • Actinide inventory of Herndon’s georeactor was analyzed by using a modified TRITON sequence in SCALE6. • The georeactor can function as a converter reactor, with a conversion efficiency of approximately 0.9 over billions of years. • Dominant mechanisms that dictate the variations of nuclide concentrations over geologic time were identified. - Abstract: Herndon proposed a nuclear fission reactor at the center of the Earth to explain changes in the geomagnetic field and the 3He/4He ratios observed from deep mantle sources. This study investigated the neutronic properties of the planetary-scale reactor by performing rigorous depletion simulations over geologic time by using a modified TRITON sequence in SCALE6. We also conducted analytical calculations of the rates of change of various actinides in the reactor core to identify the primary mechanisms involved in the nuclear system as a function of the operating time. The sound agreement between analytical and TRITON calculations on the predicted variations of the amounts of important actinides revealed that (1) the hypothetical nuclear georeactor is a fast-spectrum converter reactor burning only 235U; (2) the efficiency of fuel conversion approaches 0.9, and can be sustained for billions of years based on the cycle of 238U/239Pu/235U, rather than of 238U/239Pu or 232Th/233U; and (3) under appropriate conditions, the georeactor can operate at a constant power of 3 TW for up to 6.5 billion years

  16. The fission cross sections of 230Th, 232Th, 233U, 234U, 236U, 238U, 237Np, 239Pu and 242Pu relative 235U at 14.74 MeV neutron energy

    The measurement of the fission cross section ratios of nine isotopes relative to 235U at an average neutron energy of 14.74 MeV is described with particular attention to the determination of corrections and to sources of error. The results are compared to ENDF/B-V and to other measurements of the past decade. The ratio of the neutron induced fission cross section for these isotopes to the fission cross section for 235U are: 230Th - 0.290 +- 1.9%; 232Th - 0.191 +- 1.9%; 233U - 1.132 +- 0.7%; 234U - 0.998 +- 1.0%; 236U - 0.791 +- 1.1%; 238U - 0.587 +- 1.1%; 237Np - 1.060 +- 1.4%; 239Pu - 1.152 +- 1.1%; 242Pu - 0.967 +- 1.0%. 40 refs., 11 tabs., 9 figs

  17. Synchronous Changes of the Shape of Histograms Constructed from the Results of Measurements of 90-Sr Beta-Decay and 239-Pu Alpha-Decay Observed in More than 3000 km Distant Laboratories

    Filin E. Y.

    2015-07-01

    Full Text Available It was discovered many years ago that histograms constructed from the results of mea- surements of various natural processes are not random. The histogram shape was demonstrated to be determined by the diurnal rotation and circumsolar movement of the Earth and to be independent of the nature of the process considered [1-17]. The results of those works change our basic views about stochasticity of natural processes. When the time series of physical measurements, which are traditionally considered stochastic, are transformed into the series of histograms constructed for an optimally small num- ber of the results (i.e., optimally short segment of the time series, one can see regular changes in the histogram shape. The paper illustrates the main manifestations of this phenomenon by comparing the results of 90 Sr -radioactivity and 239 Pu -decay mea- surements, with the distance between the laboratories in which the data were collected being about 3000 km.

  18. Beta and gamma decay heat measurements between 0.1s--50,000s for neutron fission of 235U, 238U and 239Pu. Final report, June 1, 1992--December 31, 1996

    This is a final reporting on the composition of separate beta and gamma decay heat measurements following neutron fission of 235U and 238U and 239Pu and on cumulative and independent yield measurements of fission products of 235U and 238U. What made these studies unique was the very short time of 0.1 s after fission that could be achieved by incorporating the helium jet and tape transport system as the technique for transporting fission fragments from the neutron environment of the fission chamber to the low-background environment of the counting area. This capability allowed for the first time decay heat measurements to extend nearly two decades lower on the logarithmic delay time scale, a region where no comprehensive aggregate decay heat measurements had extended to. This short delay time capability also allowed the measurement of individual fission products with half lives as short as 0.2s. The purpose of such studies was to provide tests both at the aggregate level and at the individual nuclide level of the nation's evaluated nuclear data file associated with fission, ENDF/B-VI. The results of these tests are in general quite encouraging indicating this data base generally predicts correctly the aggregate beta and aggregate gamma decay heat as a function of delay time for 235U, 238U and 239Pu. Agreement with the measured individual nuclide cumulative and independent yields for fission products of 235U and 238U was also quite good although the present measurements suggest needed improvements in several individual cases

  19. Effects of combined exposure of F344 rats to radiation and chronically inhaled cigarette smoke

    Nuclear workers may be exposed to radiation in various forms, such as low-LET γ-irradiation or α-irradiation from inhaled 239PuO2 particles. These workers may then have increased risk for lung cancer compared to the general population. Of additional concern is the possibility that interactions between radiation and other carcinogens may increase the risk of cancer induction, compared to the risks from either type of agent alone. An important and common lung carcinogen is cigarette smoke. The purpose of this project is to better determine the combined effects of chronically inhaled cigarette smoke and either inhaled 239PuO2 or external, thoracic X-irradiation on the induction of lung cancer in rats. Histologic and dosimetric evaluations of rats in the CS + 239PuO2 study continue, and the study of CS + X rays is beginning

  20. Effects of combined exposure of F344 rats to radiation and chronically inhaled cigarette smoke

    Finch, G.L.; Nikula, K.J.; Barr, E.B. [and others

    1995-12-01

    Nuclear workers may be exposed to radiation in various forms, such as low-LET {gamma}-irradiation or {alpha}-irradiation from inhaled {sup 239}PuO{sub 2} particles. These workers may then have increased risk for lung cancer compared to the general population. Of additional concern is the possibility that interactions between radiation and other carcinogens may increase the risk of cancer induction, compared to the risks from either type of agent alone. An important and common lung carcinogen is cigarette smoke. The purpose of this project is to better determine the combined effects of chronically inhaled cigarette smoke and either inhaled {sup 239}PuO{sub 2} or external, thoracic X-irradiation on the induction of lung cancer in rats. Histologic and dosimetric evaluations of rats in the CS + {sup 239}PuO{sub 2} study continue, and the study of CS + X rays is beginning.

  1. Actinide chemistry using singlet-paired coupled cluster and its combinations with density functionals

    Garza, Alejandro J; Scuseria, Gustavo E

    2015-01-01

    Singlet-paired coupled cluster doubles (CCD0) is a simplification of CCD that relinquishes a fraction of dynamic correlation in order to be able to describe static correlation. Combinations of CCD0 with density functionals that recover specifically the dynamic correlation missing in the former have also been developed recently. Here, we assess the accuracy of CCD0 and CCD0+DFT (and variants of these using Brueckner orbitals) as compared to well-established quantum chemical methods for describing ground-state properties of singlet actinide molecules. The $f^0$ actinyl series (UO$_2^{2+}$, NpO$_2^{2+}$, PuO$_2^{2+}$), the isoelectronic NUN, and Thorium (ThO, ThO$^{2+}$) and Nobelium (NoO, NoO$_2$) oxides are studied.

  2. Evaluation study on silica/polymer-based CA-BTP adsorbent for the separation of minor actinides from simulated high-level liquid wastes

    A silica/polymer-based CA-BTP/SiO2-P adsorbent was prepared to separate minor actinides and some key radionuclides from HLLW. The adsorption properties of CA-BTP/SiO2-P toward 238U(VI), 239Pu(IV), 241Am(III), 99Tc(VII), 152Eu(III), and some typical fission products were studied. CA-BTP/SiO2-P stability against c-radiation was also evaluated. It found CA-BTP/SiO2-P showed very poor adsorption abilities toward U(VI) and most experimental FPs, while CA-BTP/SiO2-P exhibited higher adsorption abilities toward 241Am(III), 239Pu(IV), and 99Tc(VII) in 0.5-1 M HNO3 solution. Moreover, dry CA-BTP/SiO2-P demonstrated no instability when the radiation dose was up to 161 kGy. CA-BTP/SiO2-P adsorbent is a potential candidate for separating 241Am(III), 239Pu(IV), and 99Tc(VII) from HLLW. (author)

  3. Rapid determination of alpha emitters using Actinide resin.

    Navarro, N; Rodriguez, L; Alvarez, A; Sancho, C

    2004-01-01

    The European Commission has recently published the recommended radiological protection criteria for the clearance of building and building rubble from the dismantling of nuclear installations. Radionuclide specific clearance levels for actinides are very low (between 0.1 and 1 Bq g(-1)). The prevalence of natural radionuclides in rubble materials makes the verification of these levels by direct alpha counting impossible. The capability of Actinide resin (Eichrom Industries, Inc.) for extracting plutonium and americium from rubble samples has been tested in this work. Besides a strong affinity for actinides in the tri, tetra and hexavalent oxidation states, this extraction chromatographic resin presents an easy recovery of absorbed radionuclides. The retention capability was evaluated on rubble samples spiked with certified radionuclide standards (239Pu and 241Am). Samples were leached with nitric acid, passed through a chromatographic column containing the resin and the elution fraction was measured by LSC. Actinide retention varies from 60% to 80%. Based on these results, a rapid method for the verification of clearance levels for actinides in rubble samples is proposed. PMID:15177360

  4. Determination of actinides by alpha spectrometric methods

    The submitted thesis in its first part concern with content determination of plutonium, americium, uranium, thorium radionuclides, like the most significant representatives of actinides in environmental patterns, where by the primary consideration is a focusing on content of these actinides in samples of superior mycotic organisms - mushrooms. Following the published studies the mushrooms were monitored as organisms that could verify most of attributes putted on bioindicators in term of observation of substantial radionuclides in living environment. There were analyzed two groups of samples that came from two chosen locations, one of them is situated in Eastern Slovakia and the second one in West Slovakia. Except for mushrooms samples the examined radionuclides volumes were determined even in specimens of soil sub-base and some plants from chosen localities. The liquid - liquid extraction methods were used for determination of mass activities of actinides in samples for radiochemical separation of monitored radionuclides. The obtained results of plutonium and americium mass activities determination's lead us to carry out experiments that proved abilities of superior mycotic organisms to absorb and accumulate alpha radionuclides in their textures. We choose the oyster mushroom (Pleurotus ostreatus) species as an experimental object. Sporocarps of this mushroom were cultivated on substratum which is commercially exploited to cultivate it whereby this substratum was purposely contaminated by known activities of 239Pu and 241Am. We prepared five autonomous samples together. The values of mass activities of 239Pu and 241Am obtained by following analysis of prepared samples showed the ability of mushrooms to absorb observed actinides in their texture structures. On the basis of obtained mass activities it was possible to evaluate and numerically determine a transmitting factor's attributes of monitored radionuclides in sporocarps and in sub-base. Accordingly we defined

  5. Actinide-only burnup credit for spent fuel transport

    A conservative methodology is described that would allow taking credit for burn up in the criticality safety analysis of spent nuclear fuel packages. Requirements for its implementation include isotopic and criticality validation, generation of package loading criteria using limiting parameters, and assembly burn up verification by measurement. The method allows credit for the changes in the 234U, 235U, 236U, 238U, 238Pu, 239Pu, 240Pu, 241Pu, 242Pu, and 241Am concentrations with burnup. No credit for fission product neutron absorbers is taken. Analyses are included regarding the methodology's financial benefits and conservative margin. It is estimated that the proposed actinide-only burnup credit methodology would save 20% of the transport costs. Nevertheless, the methodology includes a substantial margin. Conservatism due to the isotopic correction factors, limiting modelling parameters, limiting axial profiles and exclusion of the fission products ranges from 10 to 25% k. (author)

  6. Neutron scattering studies in the actinide region

    This report discusses the following topics: Prompt fission neutron energy spectra for 235U and 239Pu; Two-parameter measurement of nuclear lifetimes; ''Black'' neutron detector; Data reduction techniques for neutron scattering experiments; Inelastic neutron scattering studies in 197Au; Elastic and inelastic scattering studies in 239Pu; and neutron induced defects in silicon dioxide MOS structures

  7. Comparative analysis between measured and calculated concentrations of major actinides using destructive assay data from Ohi-2 PWR

    Oettingen Mikołaj

    2015-09-01

    Full Text Available In the paper, we assess the accuracy of the Monte Carlo continuous energy burnup code (MCB in predicting final concentrations of major actinides in the spent nuclear fuel from commercial PWR. The Ohi-2 PWR irradiation experiment was chosen for the numerical reconstruction due to the availability of the final concentrations for eleven major actinides including five uranium isotopes (U-232, U-234, U-235, U-236, U-238 and six plutonium isotopes (Pu-236, Pu-238, Pu-239, Pu-240, Pu-241, Pu-242. The main results were presented as a calculated-to-experimental ratio (C/E for measured and calculated final actinide concentrations. The good agreement in the range of ±5% was obtained for 78% C/E factors (43 out of 55. The MCB modeling shows significant improvement compared with the results of previous studies conducted on the Ohi-2 experiment, which proves the reliability and accuracy of the developed methodology.

  8. About the first experiment on investigation of 129I, 237Np, 238Pu and 239Pu transmutation at the nuclotron 2.52 GeV deuteron beam in neutron field generated in U/Pb-assembly 'Energy plus transmutation'

    Preliminary results of the first experiment with energy 2.52 GeV at the electronuclear setup which consists of Pb-target (diameter 8.4 cm, length 45.6 cm) and natU-blanket (206.4 kg), transmutation samples of 129I, 237Np, 238Pu and 239Pu (radioecological aspect) are described. Hermetically sealed samples in notable amounts are gathered in atomic reactors and setups of industries which use nuclear materials and nuclear technologies were irradiated in the field of neutrons produced in the Pb-target and propagated in the natU-blanket. Estimates of transmutations were obtained as a result of measurements of gamma activities of the samples. The information about the space and energy distribution of neutrons in the volume of the lead target and the uranium blanket was obtained with the help of sets of activation threshold detectors (Al, Co, Y, I, Au, Bi and others), solid-state nuclear track detectors, 3He neutron detectors and nuclear emulsion. Comparison of the experimental data with the results of simulation with the MCNPX program was performed

  9. Energy dependence of relative abundances and periods of separate groups of delayed neutrons at neutron induced fission of 239Pu in a range of neutrons energies 0.37 - 5 MeV

    The fundamental role of delayed neutrons in behavior, control and safety of reactors is well known today. Delayed neutron data are of great interest not only for reactor physics but also for nuclear fission physics and astrophysics. The purpose of the present work was the measurement of energy dependence of delayed neutrons (DN) group parameters at fission of nuclei 239Pu in a range of energies of primary neutrons from 0.37 up to 5 MeV. The measurements were executed on installation designed on the basis of the electrostatic accelerator of KG - 2.5 SSC RF IPPE. The data are obtained in 6-group representation. It is shown, that there is a significant energy dependence of DN group parameters in a range of primary neutrons energies from thermal meanings up to 5 MeV, which is expressed in reduction of the average half-life of nuclei of the DN precursors on 10 %. The data, received in the present work, can be used at creation of a set of group constants for reactors with an intermediate spectrum of neutrons. (authors)

  10. Combining theoretical chemistry and Xanes multi-edge experiments to probe actinide valence states

    Both structural and electronic properties of the actinide cations are of fundamental interest in order to describe the intramolecular interactions. The 5f and 6d orbitals are the first partially or totally vacant states of these elements and their properties reflect the nature of the actinide-ligand bond. Because of its chemical and orbital selectivities, XANES spectroscopy is useful to probe the actinides' frontier orbitals and then understand the cation reactivity toward chelating ligands. The actinide L3 edge contains structural information on the coordination polyhedron because of important scattering features. But very little electronic information can be extracted, due to the short core-hole lifetime, broadening the edge signal. On the other hand, the actinide M4,5 edges provide a better resolution and allow one to achieve electronic and structural information. Furthermore, coupling simulations of the experimental spectra and quantum chemical calculations lead to quantitative information such as the determination of the actinide coordination sphere and its effective charge. (authors)

  11. Combining theoretical chemistry and Xanes multi-edge experiments to probe actinide valence states

    Fillaux, C.; Guilbaud, Ph.; Guillaumont, D.; Moisy, Ph.; Den Auwer, Ch. [CEA Valrho, Dir. de l' Energie Nucleaire (DEN/DRCP/SCPS), 30 - Marcoule (France); Berthet, J.C. [CEA Saclay, Dept. de Recherche sur l' Etat Condense, les Atomes et les Molecules (DSM/DRECAM/SCM), 91 - Gif sur Yvette (France); Conradsonc, St.D. [Los Alamos National Laboratory, Los Alamos, NM (United States); Hennig, C. [Forschungszentrum Rossendorf, ROBL at ESRF, 38 - Grenoble (France); Roques, J.; Simoni, E. [Institut de Physique Nucleaire, 91 - Orsay (France); Shuh, D.K.; Tyliszczak, T.; Castro-Rodriguez, I. [Lawrence Berkeley National Laboratory, Berkeley, CA (United States)

    2007-10-15

    Both structural and electronic properties of the actinide cations are of fundamental interest in order to describe the intramolecular interactions. The 5f and 6d orbitals are the first partially or totally vacant states of these elements and their properties reflect the nature of the actinide-ligand bond. Because of its chemical and orbital selectivities, XANES spectroscopy is useful to probe the actinides' frontier orbitals and then understand the cation reactivity toward chelating ligands. The actinide L3 edge contains structural information on the coordination polyhedron because of important scattering features. But very little electronic information can be extracted, due to the short core-hole lifetime, broadening the edge signal. On the other hand, the actinide M4,5 edges provide a better resolution and allow one to achieve electronic and structural information. Furthermore, coupling simulations of the experimental spectra and quantum chemical calculations lead to quantitative information such as the determination of the actinide coordination sphere and its effective charge. (authors)

  12. STRONTIUM AND ACTINIDE SEPARATIONS FROM HIGH LEVEL NUCLEAR WASTE SOLUTIONS USING MONOSODIUM TITANATE 1. SIMULANT TESTING

    HOBBS, D. T.; BARNES, M. J.; PULMANO, R. L.; MARSHALL, K. M.; EDWARDS, T. B.; BRONIKOWSKI, M. G.; FINK, S. D.

    2005-04-14

    High-level nuclear waste produced from fuel reprocessing operations at the Savannah River Site (SRS) requires pretreatment to remove {sup 137}Cs, {sup 90}Sr and alpha-emitting radionuclides (i.e., actinides) prior to disposal. Separation processes planned at SRS include caustic side solvent extraction, for {sup 137}Cs removal, and ion exchange/sorption of {sup 90}Sr and alpha-emitting radionuclides with an inorganic material, monosodium titanate (MST). The predominant alpha-emitting radionuclides in the highly alkaline waste solutions include plutonium isotopes {sup 238}Pu, {sup 239}Pu and {sup 240}Pu. This paper provides a summary of data acquired to measure the performance of MST to remove strontium and actinides from simulated waste solutions. These tests evaluated the influence of ionic strength, temperature, solution composition and the oxidation state of plutonium.

  13. A Lane consistent optical model potential for nucleon scattering on actinide nuclei with extended coupling

    Quesada, José Manuel; Capote, Roberto; Soukhovitski, Efrem S.; Chiba, Satoshi

    2016-03-01

    An extension for odd-A actinides of a previously derived dispersive coupledchannel optical model potential (OMP) for 238U and 232Th nuclei is presented. It is used to fit simultaneously all the available experimental databases including neutron strength functions for nucleon scattering on 232Th, 233,235,238U and 239Pu nuclei. Quasi-elastic (p,n) scattering data on 232Th and 238U to the isobaric analogue states of the target nucleus are also used to constrain the isovector part of the optical potential. For even-even (odd) actinides almost all low-lying collective levels below 1 MeV (0.5 MeV) of excitation energy are coupled. OMP parameters show a smooth energy dependence and energy independent geometry.

  14. A Lane consistent optical model potential for nucleon scattering on actinide nuclei with extended coupling

    Quesada José Manuel

    2016-01-01

    Full Text Available An extension for odd-A actinides of a previously derived dispersive coupledchannel optical model potential (OMP for 238U and 232Th nuclei is presented. It is used to fit simultaneously all the available experimental databases including neutron strength functions for nucleon scattering on 232Th, 233,235,238U and 239Pu nuclei. Quasi-elastic (p,n scattering data on 232Th and 238U to the isobaric analogue states of the target nucleus are also used to constrain the isovector part of the optical potential. For even-even (odd actinides almost all low-lying collective levels below 1 MeV (0.5 MeV of excitation energy are coupled. OMP parameters show a smooth energy dependence and energy independent geometry.

  15. Toxicity of inhaled 239PuO2 in Beagle dogs: A. Monodisperse 0.75-μm AMAD particles. B. Monodisperse 1.5-μm AMAD particles. C. Monodisperse 3.0--μm AMAD particles. XI

    Beagle dogs were exposed to monodisperse aerosols of 239PuO2 of 0.75, 1.5, or 30 μm activity median aerodynamic diameter (AMAD) to obtain information on the relative importance of homogeneity of alpha irradiation doses to the lung in producing biological effects. The dogs' initial pulmonary burdens (IPB) ranged from 0.0002-2.0 μCi (0.0074 to 74 kBq) 239Pu/kg of body mass. Thirty-six dogs were exposed to the aerosol diluent as controls. Forty-two of 48 dogs exposed to 0.75 μm AMAD particles have died; 67 of 96 have died in the study involving 1.5 μm AMAD particles; and 62 of 72 have died in the study involving the 3.0 μm AMAD particles. Seven of 36 control dogs have died. Most dogs exposed to 239Pu that have failed to survive have died with radiation pneumonitis and fibrosis and/or lung cancer. Surviving dogs have lived up to 4300 days after exposure. The data obtained to date indicate that the degree of uniformity of dose to the lung does not significantly modify the risk of lung cancer. (author)

  16. Actinide recycle

    A multitude of studies and assessments of actinide partitioning and transmutation were carried out in the late 1970s and early 1980s. Probably the most comprehensive of these was a study coordinated by Oak Ridge National Laboratory. The conclusions of this study were that only rather weak economic and safety incentives existed for partitioning and transmuting the actinides for waste management purposes, due to the facts that (1) partitioning processes were complicated and expensive, and (2) the geologic repository was assumed to contain actinides for hundreds of thousands of years. Much has changed in the few years since then. A variety of developments now combine to warrant a renewed assessment of the actinide recycle. First of all, it has become increasingly difficult to provide to all parties the necessary assurance that the repository will contain essentially all radioactive materials until they have decayed. Assurance can almost certainly be provided to regulatory agencies by sound technical arguments, but it is difficult to convince the general public that the behavior of wastes stored in the ground can be modeled and predicted for even a few thousand years. From this point of view alone there would seem to be a clear benefit in reducing the long-term toxicity of the high-level wastes placed in the repository

  17. Prompt Fission Neutron Spectra of Actinides

    Capote, R; Chen, Y J; Hambsch, F J; Kornilov, N V; Lestone, J P; Litaize, O; Morillon, B; Neudecker, D; Oberstedt, S; Ohsawa, T; Smith, D. L.

    2016-01-01

    The energy spectrum of prompt neutrons emitted in fission (PFNS) plays a very important role in nuclear science and technology. A Coordinated Research Project (CRP) “Evaluation of Prompt Fission Neutron Spectra of Actinides”was established by the IAEA Nuclear Data Section in 2009, with the major goal to produce new PFNS evaluations with uncertainties for actinide nuclei. The following technical areas were addressed: (i) experiments and uncertainty quantification (UQ): New data for neutron-induced fission of 233U, 235U, 238U, and 239Pu have been measured, and older data have been compiled and reassessed. There is evidence from the experimental work of this CRP that a very small percentage of neutrons emitted in fission are actually scission neutrons; (ii) modeling: The Los Alamos model (LAM) continues to be the workhorse for PFNS evaluations. Monte Carlo models have been developed that describe the fission phenomena microscopically, but further development is needed to produce PFNS evaluations meeting the uncertainty targets; (iii) evaluation methodologies: PFNS evaluations rely on the use of the least-squares techniques for merging experimental and model data. Considerable insight was achieved on how to deal with the problem of too small uncertainties in PFNS evaluations. The importance of considering that all experimental PFNS data are “shape” data was stressed; (iv) PFNS evaluations: New evaluations, including covariance data, were generated for major actinides including 1) non-model GMA evaluations of the 235U(nth,f), 239Pu(nth,f), and 233U(nth,f) PFNS based exclusively on experimental data (0.02 ≤ E ≤ 10 MeV), which resulted in PFNS average energies E of 2.00±0.01, 2.073±0.010, and 2.030±0.013 MeV, respectively; 2) LAM evaluations of neutron-induced fission spectra on uranium and plutonium targets with improved UQ for incident energies from thermal up to 30 MeV; and 3) Point-by-Point calculations for 232Th, 234U and 237Np targets; and (v) data

  18. Quantification of actinide alpha-radiation damage in minerals and ceramics.

    Farnan, Ian; Cho, Herman; Weber, William J

    2007-01-11

    There are large amounts of heavy alpha-emitters in nuclear waste and nuclear materials inventories stored in various sites around the world. These include plutonium and minor actinides such as americium and curium. In preparation for geological disposal there is consensus that actinides that have been separated from spent nuclear fuel should be immobilized within mineral-based ceramics rather than glass because of their superior aqueous durability and lower risk of accidental criticality. However, in the long term, the alpha-decay taking place in these ceramics will severely disrupt their crystalline structure and reduce their durability. A fundamental property in predicting cumulative radiation damage is the number of atoms permanently displaced per alpha-decay. At present, this number is estimated to be 1,000-2,000 atoms/alpha in zircon. Here we report nuclear magnetic resonance, spin-counting experiments that measure close to 5,000 atoms/alpha in radiation-damaged natural zircons. New radiological nuclear magnetic resonance measurements on highly radioactive, 239Pu zircon show damage similar to that caused by 238U and 232Th in mineral zircons at the same dose, indicating no significant effect of half-life or loading levels (dose rate). On the basis of these measurements, the initially crystalline structure of a 10 weight per cent 239Pu zircon would be amorphous after only 1,400 years in a geological repository (desired immobilization timescales are of the order of 250,000 years). These measurements establish a basis for assessing the long-term structural durability of actinide-containing ceramics in terms of an atomistic understanding of the fundamental damage event. PMID:17215840

  19. Fast Burner Reactor Devoted to Minor Actinide Incineration

    This study proposes a new fast reactor core concept dedicated to plutonium and minor actinide burning by transmutation. This core has a large power level of ∼1500 MW(electric) favoring the economic aspect. To promote plutonium and minor actinide burning as much as possible, total suppression of 238U, which produces 239Pu by conversion, and large quantities of minor actinides in the core are desirable. Therefore, the 238U-free fuel is homogeneously mixed with a considerable quantity of minor actinides.From the safety point of view, both the Doppler effect and the coolant (sodium) void reactivity become less favorable in a 238U-free core. To preserve these two important safety parameters on an acceptable level, a hydrogenated moderator separated from the fuel and nuclides, such as W or 99Tc, is added to the core in the place of 238U. Tungsten and 99Tc have strong capture resonances at appropriate energies, and 99Tc itself is a long-lived fission product to be transmuted with profit.This core allows the achievement of a consumption rate of ∼100 kg/TW(electric).h of transuranic elements, ∼70 kg/TW(electric).h for plutonium (due to 238U suppression), and 30 to 35 kg/TW(electric).h for minor actinides. In addition, ∼14 kg/TW(electric).h of 99Tc is destroyed when this element is present in the core (the initial loading of 99Tc is >4000 kg in the core).The activity of newly designed subassemblies has also been investigated in comparison to standard fast reactor subassemblies (neutron sources, decay heat, and gamma dose rate). Finally, a transmutation scenario involving pressurized water reactors and minor actinide-burning fast reactors has been studied to estimate the necessary proportion of burner reactors and the achievable radiotoxicity reduction with respect to a reference open cycle

  20. Energy Dependence of Fission Product Yields from 235U, 238U and 239Pu for Incident Neutron Energies Between 0.5 and 14.8 MeV

    Gooden, M. E.; Arnold, C. W.; Becker, J. A.; Bhatia, C.; Bhike, M.; Bond, E. M.; Bredeweg, T. A.; Fallin, B.; Fowler, M. M.; Howell, C. R.; Kelley, J. H.; Krishichayan; Macri, R.; Rusev, G.; Ryan, C.; Sheets, S. A.; Stoyer, M. A.; Tonchev, A. P.; Tornow, W.; Vieira, D. J.; Wilhelmy, J. B.

    2016-01-01

    Fission Product Yields (FPY) have historically been one of the most observable features of the fission process. They are known to have strong variations that are dependent on the fissioning species, the excitation energy, and the angular momentum of the compound system. However, consistent and systematic studies of the variation of these FPY with energy have proved challenging. This is caused primarily by the nature of the experiments that have traditionally relied on radiochemical procedures to isolate specific fission products. Although radiochemical procedures exist that can isolate all products, each element presents specific challenges and introduces varying degrees of systematic errors that can make inter-comparison of FPY uncertain. Although of high importance in fields such as nuclear forensics and Stockpile Stewardship, accurate information about the energy dependence of neutron induced FPY are sparse, due primarily to the lack of suitable monoenergetic neutron sources. There is a clear need for improved data, and to address this issue, a collaboration was formed between Los Alamos National Laboratory (LANL), Lawrence Livermore National Laboratory (LLNL) and the Triangle Universities Nuclear Laboratory (TUNL) to measure the energy dependence of FPY for 235U, 238U and 239Pu. The measurements have been performed at TUNL, using a 10 MV Tandem Van de Graaff accelerator to produce monoenergetic neutrons at energies between 0.6 MeV to 14.8 MeV through a variety of reactions. The measurements have utilized a dual-fission chamber, with thin (10-100 μg/cm2) reference foils of similar material to a thick (100-400 mg) activation target held in the center between the chambers. This method allows for the accurate determination of the number of fissions that occurred in the thick target without requiring knowledge of the fission cross section or neutron fluence on target. Following activation, the thick target was removed from the dual-fission chamber and gamma

  1. Study and development of a method allowing the identification of actinides inside nuclear waste packages, by active neutron or photon interrogation and delayed gamma-ray spectrometry

    An accurate estimation of the alpha-activity of a nuclear waste package is necessary to select the best mode of storage. The main purpose of this work is to develop a non-destructive active method, based on the fission process and allowing the identification of actinides (235U, 238U, 239Pu). These three elements are the main alpha emitters contained inside a package. Our technique is based on the detection of delayed gammas emitted by fission products. These latter are created by irradiation with the help of a neutron or photon beam. Performances of this method have been investigated after an Active Photon or Neutron Interrogation (INA or IPA). Three main objectives were fixed in the framework of this thesis. First, we measured many yields of photofission products to compensate the lack of data in the literature. Then, we studied experimental performances of this method to identify a given actinide (239Pu in fission, 235U in photofission) present in an irradiated mixture. Finally, we assessed the application of this technique on different mock-up packages for both types of interrogation (118 l mock-up package containing EVA in fission, 220 l mock-up package with a wall of concrete in photofission). (author)

  2. Determination of actinides in environmental and biological samples using high-performance chelation ion chromatography coupled to sector-field inductively coupled plasma mass spectrometry.

    Truscott, J B; Jones, P; Fairman, B E; Evans, E H

    2001-08-31

    High-performance chelation ion chromatography, using a neutral polystyrene substrate dynamically loaded with 0.1 mM dipicolinic acid, coupled with sector-field inductively coupled plasma mass spectrometry has been successfully used for the separation of the actinides thorium, uranium, americium, neptunium and plutonium. Using this column it was possible to separate the various actinides from each other and from a complex sample matrix. In particular, it was possible to separate plutonium and uranium to facilitate the detection of the former free of spectral interference. The column also exhibited some selectivity for different oxidation states of Np, Pu and U. Two oxidation states each for plutonium and neptunium were found, tentatively identified as Np(V) and Pu(III) eluting at the solvent front, and Np(IV) and Pu(IV) eluting much later. Detection limits were 12, 8, and 4 fg for 237Np, 239Pu, and 241Am, respectively, for a 0.5 ml injection. The system was successfully used for the determination of 239Pu in NIST 4251 Human Lung and 4353 Rocky Flats Soil, with results of 570+/-29 and 2939+/-226 fg g(-1), respectively, compared with a certified range of 227-951 fg g(-1) for the former and a value of 3307+/-248 fg g(-1) for the latter. PMID:11589474

  3. Neutron scattering studies in the actinide region

    During the report period we have investigated the following areas: Neutron elastic and inelastic scattering measurements on 14N, 181Ta, 232Th, 238U and 239Pu; Prompt fission spectra for 232Th, 235U, 238U and 239Pu; Theoretical studies of neutron scattering; Neutron filters; New detector systems; and Upgrading of neutron target assembly, data acquisition system, and accelerator/beam-line apparatus

  4. A high repetition rate solid state laser system for resonance ionization mass spectrometry of actinides

    A new, high repetition rate solid state laser system consisting of three Titanium-Sapphire (Ti:Sa) lasers pumped by one Nd:YAG laser has been set up for resonance ionization mass spectrometry for routine trace analysis of actinides. Each Ti:Sa laser produces up to 4 W of laser light with a bandwidth of 2-6 GHz continuously tuneable in a range from 725 to 900 nm. Using a three step ionization scheme with λ1=420.76 nm, λ2=847.28 nm and λ3239Pu, the overall detection efficiency of the setup has been measured to be ε=8.0x10-6. Thus a detection limit of 1x107 atoms of 239Pu is derived and opens up the way to use a reliable and easy to handle laser system for routine applications of RIMS

  5. Electrodeposition of actinide traces from aqueous alkaline solutions and tributyl phosphate

    The electrodeposition of uranium and trace quantities of 239Pu, 234Th, 144Ce on a stainless steel disk was investigated from 0.5-2.0M NaOH and the two-phase system, extract of actinides in TBP-aqueous solution of NaOH. The electrodeposition yield of the above elements reaches 98-100% in 40 min of electrolysis with current density 0.4-0.5 A/cm2. The presence of 0.5M Na2CO3, 2.0M NaNO3, 2.0M NaNO2, 0.2M NaF in alkaline solutions does not decrease the electrodeposition yield. The electrodeposited films meet all the requirements of α-spectrometry. The uranium oxidation states (V) and (IV) were determined in the electrodeposited films. (author) 9 refs.; 3 figs.; 1 tab

  6. Determination of actinide elements in environmental samples by ICP-MS

    Methods for the determination of the actinide elements in water, biological, soil and sediment samples have been developed using on-line solid phase extraction and high performance liquid chromatography (HPLC) coupled with inductively coupled plasma mass spectrometry (ICP-MS). Initial applications utilised a commercially available resin, namely TRU-Spec resin, for efficient removal of the matrix prior to elution of uranium and thorium analytes. Comparative analyses of reference materials and natural water samples from Plymouth and Dartmoor demonstrated significant improvement in precision and speed of analysis by using TRU-Spec coupled to ICP-MS compared with alpha spectrometry. Further applications of the TRU-Spec resin for the determination of the transuranic actinide elements neptunium, plutonium and americium, resulted in the successful determination of 239Pu and 217Np in biological reference materials. Detection limits were 700, 850, and 600 attograms (ag) for 237Np, 233Pu, and 241Am, respectively, for a 0.5 mI sample injection, and better than 200 ag g-1 with 50 ml pre-concentration when sector field (SF) ICP-MS was used. A method for the selective sequential elution of uranium and plutonium was also developed to facilitate the determination of 239Pu without interference due to the 238U1H+ polyatomic ion, caused by high concentrations of 238U in sediment samples. Investigations were performed into the use of a polymeric substrate, which was dynamically coated with chelating dyes such as xylenol orange and 4-(2-pyridylazo) resorcinol, and a silica substrate coated with permanently bonded iminodiacetic acid. The latter was used for the successful determination of uranium and thorium in certified reference material waters. However, the column was found to have a high affinity for iron, making it unsuitable for the determination of the actinides in soil and sediment samples. Subsequently, a polystyrene substrate which was dynamically coated with dipicolinic acid

  7. Limits of DPUI application associated with the number of particles within actinide aerosols

    Dose per unit intake (DPUI) of radionuclides is obtained using International Commission on Radiological Protection (ICRP) models. After inhalation exposure, the first model calculates the fraction of activity deposited within the different regions of the respiratory tract, assuming that the aerosol contains an infinite number of particles. Using default parameters for workers, an exposure to one annual limit of intake (ALI) corresponds to an aerosol of 239PuO2 containing ∼1 x 106 particles. To reach such an exposure, very low particle number might be involved especially for compounds having a high specific activity. This study provides examples of exposures to actinide aerosols for which the number of particles is too low for a standard application of the ICRP model. These examples, which involve physical studies of aerosols collected at the workplace and interpretation of bioassay data, show that the number of particles of the aerosol can be the main limit for the application of DPUI after inhalation exposure. (authors)

  8. Study and development of a method allowing the identification of actinides inside nuclear waste packages, by active neutron or photon interrogation and delayed gamma-ray spectrometry; Etude et developpement d'une technique de dosage des actinides dans les colis de dechets radioactifs par interrogation photonique ou neutronique active et spectrometrie des gamma retardes

    Carrel, F

    2007-10-15

    An accurate estimation of the alpha-activity of a nuclear waste package is necessary to select the best mode of storage. The main purpose of this work is to develop a non-destructive active method, based on the fission process and allowing the identification of actinides ({sup 235}U, {sup 238}U, {sup 239}Pu). These three elements are the main alpha emitters contained inside a package. Our technique is based on the detection of delayed gammas emitted by fission products. These latter are created by irradiation with the help of a neutron or photon beam. Performances of this method have been investigated after an Active Photon or Neutron Interrogation (INA or IPA). Three main objectives were fixed in the framework of this thesis. First, we measured many yields of photofission products to compensate the lack of data in the literature. Then, we studied experimental performances of this method to identify a given actinide ({sup 239}Pu in fission, {sup 235}U in photofission) present in an irradiated mixture. Finally, we assessed the application of this technique on different mock-up packages for both types of interrogation (118 l mock-up package containing EVA in fission, 220 l mock-up package with a wall of concrete in photofission). (author)

  9. Characterization of actinide physics specimens for the US/UK joint experiment in the Dounreay Prototype Fast Reactor

    The United States and the United Kingdom are engaged in a joint research program in which samples of the higher actinides are irradiated in the Dounreay Prototype Fast Reactor in Scotland. The purpose of the porogram is (1) to study the materials behavior of selected higher actinide fuels and (2) to determine the integral cross sections of a wide variety of the higher actinide isotopes. Samples of the actinides are incorporated in fuel pins inserted in the core. For the fuel study, the actinides selected are 241Am and 244Cm in the form of Am2O3, Cm2O3, and Am6Cm(RE)7O21, where (RE) represents a mixture of lanthanides. For the cross-section determinations, the samples are milligram quantities of actinide oxides of 248Cm, 246Cm, 244Cm, 243Cm, 243Am, 241Am, 244Pu, 242Pu, 241Pu, 240Pu, 239Pu, 238Pu, 237Np, 238U, 236U, 235U, 234U, 233U, 232Th, 230Th, and 231Pa encapsulated in vanadium. Coincident with the irradiations, neutron flux and energy spectral measurements are made with vanadium-encapsulated dosimeter materials located within the same fuel pins

  10. Feasibility of actinide separation from UREX-like raffinates using a combination of sulfur- and oxygen-donor extractants

    A synergistic combination of bis(o-trifluoromethylphenyl)dithios-phosphinic acid and trioctylphosphine oxide has been recently shown to selectively remove uranium, neptunium, plutonium and americium from aqueous environment containing up to 0.5 M nitric acid and 5.5 g/l fission products. Here the feasibility of performing this complete actinide recovery from aqueous mixtures is forecasted for a new organic formulation containing sulfur donor extractant of modified structure based on Am(III) and Eu(III) extraction data. A mixture of bis(bis-m,m-trifluoromethyl)phenyl)-dithios-phosphinic acid and TOPO in toluene enhances the extraction performance, accomplishing Am/Eu differentiation in aqueous mixtures up to 1 M nitric acid. The new organic recipe is also less susceptible to oxidative damage resulting from radiolysis. (authors)

  11. Generation of an actinide isotopes cross section set for fast reactor calculations using data from ENDL and ENDF/B-IV

    A Bondarenko format 25-group cross section set of actinide isotopes was generated for the fuel cycle evaluation and the incineration study in fast reactor systems. Evaluated Nuclear Data Library of Lawrence Livermore Laboratory (U.S.) was used as the source data. The actinide isotopes treated are the following 28: Th-232, U-233, U-234, U-235, U-236, U-237, Pu-238, Pu-239, Pu-240, Pu-241, Pu-242, Pu-243, Am-241, Am-242, Am-243, Cm-242, Cm-243, Cm-245, Cm-246, Cm-247, Cm-248, Bk-249, Cf-249, Cf-250, Cf-251, Cf-252 and a pseudo-fission product. ENDF/B-IV was used for U-238. The set was then collapsed to one energy group using a large LMFBR core spectrum for the comparison with other one-group sets. (author)

  12. Implications of postmortem human tissue analysis on biokinetic models for actinides

    Changes and refinements to original biokinetic models, based on postmortem radiochemical measurements of the concentration and distribution of actinides in tissues obtained from volunteer donors with known occupational experience with actinides, are discussed with emphasis on applications to operational health physics. Analysis of five whole body donations to the United States Transuranium Registry indicates that the 239Pu model put forth in ICRP Publication 30 is generally applicable, although there is a significant fraction missing from the model that is retained in the muscle. For 241Am, the more recent model put forth in ICRP Publication 48 fits the autopsy data better than the model in Publication 30, although the observed retention half-time in the liver is on the order of two to three years rather than 20 years proposed by the model. An estimated 20% of the initial systemic deposition for 241Am goes to the muscle, where it has a residence half-time estimated at ten years. For both Pu and Am, less than 5% of the skeletal actinide in the skeleton is found in the marrow. The highest concentrations appear to be associated with the periosteum and endosteum. A significantly greater fraction of inhaled Pu and Am is retained in the lungs than is predicted by current models. Differences in the actinide distribution between lung and the associated lymph nodes are observed in smokers as compared with non-smokers. (author) 30 refs.; 1 tab

  13. RAPID DETERMINATION OF ACTINIDES IN URINE BY INDUCTIVELY-COUPLED PLASMA MASS SPECTROMETRY AND ALPHA SPECTROMETRY: A HYBRID APPROACH

    Maxwell, S.; Jones, V.

    2009-05-27

    A new rapid separation method that allows separation and preconcentration of actinides in urine samples was developed for the measurement of longer lived actinides by inductively coupled plasma mass spectrometry (ICP-MS) and short-lived actinides by alpha spectrometry; a hybrid approach. This method uses stacked extraction chromatography cartridges and vacuum box technology to facilitate rapid separations. Preconcentration, if required, is performed using a streamlined calcium phosphate precipitation. Similar technology has been applied to separate actinides prior to measurement by alpha spectrometry, but this new method has been developed with elution reagents now compatible with ICP-MS as well. Purified solutions are split between ICP-MS and alpha spectrometry so that long- and short-lived actinide isotopes can be measured successfully. The method allows for simultaneous extraction of 24 samples (including QC samples) in less than 3 h. Simultaneous sample preparation can offer significant time savings over sequential sample preparation. For example, sequential sample preparation of 24 samples taking just 15 min each requires 6 h to complete. The simplicity and speed of this new method makes it attractive for radiological emergency response. If preconcentration is applied, the method is applicable to larger sample aliquots for occupational exposures as well. The chemical recoveries are typically greater than 90%, in contrast to other reported methods using flow injection separation techniques for urine samples where plutonium yields were 70-80%. This method allows measurement of both long-lived and short-lived actinide isotopes. 239Pu, 242Pu, 237Np, 243Am, 234U, 235U and 238U were measured by ICP-MS, while 236Pu, 238Pu, 239Pu, 241Am, 243Am and 244Cm were measured by alpha spectrometry. The method can also be adapted so that the separation of uranium isotopes for assay is not required, if uranium assay by direct dilution of the urine sample is preferred instead

  14. Actinides detection in the Pacific Coast of Mexico

    In this work is evaluated the activity of the alpha emitters, uranium and plutonium, in sand samples and seawater coming from diverse points of the Mexican Pacific Coast (Baja California, Jalisco, Colima and Guerrero). The used techniques were: radiochemistry separation and alpha spectrometry, with these techniques could be observed that the sand contains natural uranium and trace quantities of 239Pu and 240Pu combinations. The biggest activity in Pu was found in Finisterra, Baja California Sur (0.13 Bq/kg) and the minor (0 Bq/kg) in Miramar, Colima. The relationship between the geographical localization and the Pu activity suggests that while there is more interaction of the site with the oceanic currents, more is the content of Pu in the sands of the coast. (Author)

  15. AN INTEGRAL REACTOR PHYSICS EXPERIMENT TO INFER ACTINIDE CAPTURE CROSS-SECTIONS FROM THORIUM TO CALIFORNIUM WITH ACCELERATOR MASS SPECTROMETRY

    The principle of the proposed experiment is to irradiate very pure actinide samples in the Advanced Test Reactor (ATR) at INL and, after a given time, determine the amount of the different transmutation products. The determination of the nuclide densities before and after neutron irradiation will allow inference of effective neutron capture cross-sections. This approach has been used in the past and the novelty of this experiment is that the atom densities of the different transmutation products will be determined using the Accelerator Mass Spectroscopy (AMS) technique at the ATLAS facility located at ANL. It is currently planned to irradiate the following isotopes: 232Th, 235U, 236U, 238U, 237Np, 238Pu, 239Pu, 240Pu, 241Pu, 242Pu, 241Am, 243Am and 248Cm.

  16. Los Alamos National Laboratory thermal ionization mass spectrometry results from intercomparison study of inductively coupled plasma mass spectrometry, thermal ionization mass spectrometry, and fission track analysis of μBq quantities of 239Pu in synthetic urine (LA-UR-001698)

    In 1997, the Department of Energy, Office of International Health Programs (EH-63) contracted the National Institute of Standards and Technology (NIST) to perform an intercomparison to evaluate state-of-the-art analysis techniques for 239Pu in synthetic urine in μBq quantities. Sample preparation was performed by Yankee Atomic Environmental Laboratory. Five replicate samples at spike amounts of 3.7, 9.26, 29.6, and 55.6 μBq and a black amount were distributed to the participating laboratories in 200 g synthetic urine. Los Alamos National Laboratory (LANL) participated in the intercomparison using thermal ionization mass spectrometry (TIMS). LANL results, system improvements, and future intercomparisons are discussed. (author)

  17. Simultaneous measurement of {sup 239}Pu, {sup 240}Pu, {sup 241}Pu, and {sup 242}Pu by high resolution inductively coupled plasma mass spectrometer (HR ICP-MS) in marine sediments; Mesure des isotopes du plutonium des sediments marins par spectrometrie de masse a plasma couple inductivement haute resolution (HR ICP-MS)

    Bruneau, F

    1999-07-01

    Transuranics elements are of particular interest in radioecological studies because of their radiotoxicity and their potential use to decipher source fingerprints and transport processes. The simultaneous measurement of {sup 239}Pu, {sup 240}Pu, {sup 241}Pu, and {sup 242}Pu in environmental samples requires a specific chemical procedure. This work deals with an analytical procedure which yields a very high grade of purification of Pu suitable for ultra low level detection by HR ICP-MS, from marine sediments. After the elimination of major elements (Fe, Al, Mg...) by a first chromatographic separation, a new device of purification by solvent extraction and concentration by a second chromatographic separation is used to obtain a concentrated and high purified solution of plutonium. The chemical procedure have been validated on IAEA certified sediment samples and on sediment samples collected in the roads of Cherbourg which had been previously analysed by other techniques (a spectrometry and thermo-ionisation mass spectrometer). (author)

  18. Actinides-1981

    1981-09-01

    Abstracts of 134 papers which were presented at the Actinides-1981 conference are presented. Approximately half of these papers deal with electronic structure of the actinides. Others deal with solid state chemistry, nuclear physic, thermodynamic properties, solution chemistry, and applied chemistry.

  19. Actinides-1981

    Abstracts of 134 papers which were presented at the Actinides-1981 conference are presented. Approximately half of these papers deal with electronic structure of the actinides. Others deal with solid state chemistry, nuclear physic, thermodynamic properties, solution chemistry, and applied chemistry

  20. Subsurface Biogeochemistry of Actinides

    Kersting, Annie B. [Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States). Univ. Relations and Science Education; Zavarin, Mavrik [Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States). Glenn T. Seaborg Inst.

    2016-06-29

    A major scientific challenge in environmental sciences is to identify the dominant processes controlling actinide transport in the environment. It is estimated that currently, over 2200 metric tons of plutonium (Pu) have been deposited in the subsurface worldwide, a number that increases yearly with additional spent nuclear fuel (Ewing et al., 2010). Plutonium has been shown to migrate on the scale of kilometers, giving way to a critical concern that the fundamental biogeochemical processes that control its behavior in the subsurface are not well understood (Kersting et al., 1999; Novikov et al., 2006; Santschi et al., 2002). Neptunium (Np) is less prevalent in the environment; however, it is predicted to be a significant long-term dose contributor in high-level nuclear waste. Our focus on Np chemistry in this Science Plan is intended to help formulate a better understanding of Pu redox transformations in the environment and clarify the differences between the two long-lived actinides. The research approach of our Science Plan combines (1) Fundamental Mechanistic Studies that identify and quantify biogeochemical processes that control actinide behavior in solution and on solids, (2) Field Integration Studies that investigate the transport characteristics of Pu and test our conceptual understanding of actinide transport, and (3) Actinide Research Capabilities that allow us to achieve the objectives of this Scientific Focus Area (SFA and provide new opportunities for advancing actinide environmental chemistry. These three Research Thrusts form the basis of our SFA Science Program (Figure 1).

  1. Evaluation of possible physical-chemical processes that might lead to separations of actinides in ORNL waste tanks

    Del Cul, G.D.; Toth, L.M.; Bond, W.D.; Dai, S.

    1997-09-01

    The concern that there might be some physical-chemical process which would lead to a separation of the poisoning actinides ({sup 232}Th, {sup 238}U) from the fissionable ones ({sup 239}Pu, {sup 235}U) in waste storage tanks at Oak Ridge National Laboratory has led to a paper study of potential separations processes involving these elements. At the relatively high pH values (>8), the actinides are normally present as precipitated hydroxides. Mechanisms that might then selectively dissolve and reprecipitate the actinides through thermal processes or additions of reagents were addressed. Although redox reactions, pH changes, and complexation reactions were all considered, only the last type was regarded as having any significant probability. Furthermore, only carbonate accumulation, through continual unmonitored air sparging of the tank contents, could credibly account for gross transport and separation of the actinide components. From the large amount of equilibrium data in the literature, concentration differences in Th, U, and Pu due to carbonate complexation as a function of pH have been presented to demonstrate this phenomenon. While the carbonate effect does represent a potential separations process, control of long-term air sparging and solution pH, accompanied by routine determinations of soluble carbonate concentration, should ensure that this separations process does not occur.

  2. Evaluation of possible physical-chemical processes that might lead to separations of actinides in ORNL waste tanks

    The concern that there might be some physical-chemical process which would lead to a separation of the poisoning actinides (232Th, 238U) from the fissionable ones (239Pu, 235U) in waste storage tanks at Oak Ridge National Laboratory has led to a paper study of potential separations processes involving these elements. At the relatively high pH values (>8), the actinides are normally present as precipitated hydroxides. Mechanisms that might then selectively dissolve and reprecipitate the actinides through thermal processes or additions of reagents were addressed. Although redox reactions, pH changes, and complexation reactions were all considered, only the last type was regarded as having any significant probability. Furthermore, only carbonate accumulation, through continual unmonitored air sparging of the tank contents, could credibly account for gross transport and separation of the actinide components. From the large amount of equilibrium data in the literature, concentration differences in Th, U, and Pu due to carbonate complexation as a function of pH have been presented to demonstrate this phenomenon. While the carbonate effect does represent a potential separations process, control of long-term air sparging and solution pH, accompanied by routine determinations of soluble carbonate concentration, should ensure that this separations process does not occur

  3. Preparation of actinide specimens for the US/UK joint experiment in the Dounreay Prototype Fast Reactor

    A joint research program involving the United States and the United Kingdom was initiated about four years ago for the purpose of studying the fuel behavior of higher actinides using in-core irradiation in the fast reactor at Dounreay, Scotland. Simultaneously, determination of integral cross sections of a wide variety of higher actinide isotopes (physics specimens) was proposed. Coincidental neutron flux and energy spectral measurements were to be made using vanadium encapsulated dosimetry materials in the immediate region of the fuel pellets and physics samples. The higher actinide samples chosen for the fuel study were 241Am and 244Cm in the forms of Am2O3, Cm2O3, and Am6Cm(RE)7O21, where (RE) represents a mixture of lanthanides. Milligram quantities of actinide oxides of 248Cm, 246Cm, 244Cm, 243Cm, 243Am, 241Am, 244Pu, 242Pu, 241Pu, 240Pu, 239Pu, 238Pu, 237Np, 238U, 236U, 235U, 234U, 233U, 232Th, 230Th, and 231Pa were encapsulated to obtain nuclear cross section and reaction rate data for these materials

  4. MANTRA: An Integral Reactor Physics Experiment to Infer Actinide Capture Cross-sections from Thorium to Californium with Accelerator Mass Spectrometry

    G. Youinou; C. McGrath; G. Imel; M. Paul; R. Pardo; F. Kondev; M. Salvatores; G. Palmiotti

    2011-08-01

    The principle of the proposed experiment is to irradiate very pure actinide samples in the Advanced Test Reactor at INL and, after a given time, determine the amount of the different transmutation products. The determination of the nuclide densities before and after neutron irradiation will allow inference of effective neutron capture cross-sections. This approach has been used in the past and the novelty of this experiment is that the atom densities of the different transmutation products will be determined using the Accelerator Mass Spectrometry technique at the ATLAS facility located at ANL. It is currently planned to irradiate the following isotopes: 232Th, 235U, 236U, 238U, 237Np, 238Pu, 239Pu, 240Pu, 241Pu, 242Pu, 241Am, 243Am, 244Cm and 248Cm.

  5. MANTRA: An Integral Reactor Physics Experiment to Infer Actinide Capture Cross-sections from Thorium to Californium with Accelerator Mass Spectrometry

    The principle of the proposed experiment is to irradiate very pure actinide samples in the Advanced Test Reactor at INL and, after a given time, determine the amount of the different transmutation products. The determination of the nuclide densities before and after neutron irradiation will allow inference of effective neutron capture cross-sections. This approach has been used in the past and the novelty of this experiment is that the atom densities of the different transmutation products will be determined using the Accelerator Mass Spectrometry technique at the ATLAS facility located at ANL. It is currently planned to irradiate the following isotopes: 232Th, 235U, 236U, 238U, 237Np, 238Pu, 239Pu, 240Pu, 241Pu, 242Pu, 241Am, 243Am, 244Cm and 248Cm.

  6. Effects of combined exposure of F344 rats to inhaled Plutonium-239 dioxide and a chemical carcinogen (NNK)

    Lundgren, D.L.; Carlton, W.W. [Purdue Univ., Lafayette, IN (United States); Griffith, W.C. [and others

    1995-12-01

    Workers in nuclear weapons facilities have a significant potential for exposure to chemical carcinogens and to radiation from external sources or from internally deposited radionuclides such as {sup 239}Pu. Although the carcinogenic effects of inhaled {sup 239}Pu and many chemicals have been studied individually, very little information is available on their combined effects. One chemical carcinogen that workers could be exposed to via tobacco smoke is the tobacco-specific nitrosamine 4-(N-methyl-n-nitrosamino)-1-(3-pyridyl)-1(3-pyridyl)-1-butanone (NNK), a product of tobacco curing and the pyrolysis of nicotine in tobacco. NNK causes lung tumors in rats, regardless of the route of administration and to a lesser extent liver, nasal, and pancreatic tumors. From the results presented, it can be concluded that exposure to a chemical carcinogen (NNK) in combination with {alpha}-particle radiation from inhaled {sup 239}PuO{sub 2} acts in, at best, an additive manner in inducing lung cancer in rats.

  7. Alkaline phosphatase and transaminase activity in rat liver and blood serum at delayed periods following external γ-irradiation combined with internal exposure to plutonium 239

    A study was made of activity of alkaline phosphatase and alanine- and aspartate aminotransferase in rat liver and blood serum at remote times after external γ-irradiation combined with internal exposure to 239Pu nitrate delivered in two chronically effective doses. The radionuclide was shown to be mainly responsible for the changes observed in activity of the enzymes under study. The degree to which the changes were manifest depended upon dose of plutonium administered

  8. Mechanical environmental transport of actinides and ¹³⁷Cs from an arid radioactive waste disposal site.

    Snow, Mathew S; Clark, Sue B; Morrison, Samuel S; Watrous, Matthew G; Olson, John E; Snyder, Darin C

    2015-10-01

    Aeolian and pluvial processes represent important mechanisms for the movement of actinides and fission products at the Earth's surface. Soil samples taken in the early 1970's near a Department of Energy radioactive waste disposal site (the Subsurface Disposal Area, SDA, located in southeastern Idaho) provide a case study for studying the mechanisms and characteristics of environmental actinide and (137)Cs transport in an arid environment. Multi-component mixing models suggest actinide contamination within 2.5 km of the SDA can be described by mixing between 2 distinct SDA end members and regional nuclear weapons fallout. The absence of chemical fractionation between (241)Am and (239+240)Pu with depth for samples beyond the northeastern corner and lack of (241)Am in-growth over time (due to (241)Pu decay) suggest mechanical transport and mixing of discrete contaminated particles under arid conditions. Occasional samples northeast of the SDA (the direction of the prevailing winds) contain anomalously high concentrations of Pu with (240)Pu/(239)Pu isotopic ratios statistically identical to those in the northeastern corner. Taken together, these data suggest flooding resulted in mechanical transport of contaminated particles into the area between the SDA and a flood containment dike in the northeastern corner, following which subsequent contamination spreading in the northeastern direction resulted from wind transport of discrete particles. PMID:26107287

  9. Combined effects of radiation and other agents on the stomach cancer incidence among Mayak Atomic Plant workers

    The gravity of a problem of the combined action of radiation and other factors again was confirmed sessions UNSCEAR in May, 1998. It especially is important at study of cancer diseases in connection with the polyetiology and multistage of them development. The estimation of radiation, medico-biological factors and condition of life in occurrence of a stomach cancer among Mayak personnel was specified by case-cohort research. For a quota 503 men (157 cases of a stomach cancer, 346 men of the healthy personnel) attributive risk of the radiation factors was 8.8%, medico-biological - 57,2% (from them by greatest was influence chronic gastritis with secreting insufficiency - 35.4%), tobacco consumption - 31,6%. At an estimation of risk of a stomach cancer depending on external γ-irradiation best fitting was received at use of square-law model. The excess relative risk was 0,27 Gr-2 (F=44,5; P=0,007). For 239Pu incorporation was not revealed of distinct connection with stomach cancer incidences. Interaction of the radiation and non-radiation factors also was appreciated. The interaction of gastritis with external γ-irradiation or 239Pu was multiplicate. The interaction of smoking with γ-irradiation or 239Pu incorporation was multiplicate also. The distribution histological types of a stomach cancer among the workers of Mayak plant differed in comparison with not working. Among the workers the increase poorly differentiated adenocarcinoma was observed. (author)

  10. Combined effects of radiation and other agents on the stomach cancer incidence among Mayak Atomic Plant workers

    Zhuntova, G.V.; Tokarskaya, Z.B.; Belyaeva, Z.D. [Branch No 1 of State Research Center of Public Health Ministry of the Russian Federation, Ozyorsk (Russian Federation). Biophysics Inst.; Rovny, S.I.; Sirchikov, V.A.

    2000-05-01

    The gravity of a problem of the combined action of radiation and other factors again was confirmed sessions UNSCEAR in May, 1998. It especially is important at study of cancer diseases in connection with the polyetiology and multistage of them development. The estimation of radiation, medico-biological factors and condition of life in occurrence of a stomach cancer among Mayak personnel was specified by case-cohort research. For a quota 503 men (157 cases of a stomach cancer, 346 men of the healthy personnel) attributive risk of the radiation factors was 8.8%, medico-biological - 57,2% (from them by greatest was influence chronic gastritis with secreting insufficiency - 35.4%), tobacco consumption - 31,6%. At an estimation of risk of a stomach cancer depending on external {gamma}-irradiation best fitting was received at use of square-law model. The excess relative risk was 0,27 Gr{sup -2} (F=44,5; P=0,007). For {sup 239}Pu incorporation was not revealed of distinct connection with stomach cancer incidences. Interaction of the radiation and non-radiation factors also was appreciated. The interaction of gastritis with external {gamma}-irradiation or {sup 239}Pu was multiplicate. The interaction of smoking with {gamma}-irradiation or {sup 239}Pu incorporation was multiplicate also. The distribution histological types of a stomach cancer among the workers of Mayak plant differed in comparison with not working. Among the workers the increase poorly differentiated adenocarcinoma was observed. (author)

  11. Calorimetric assay of minor actinides

    Rudy, C.; Bracken, D.; Cremers, T.; Foster, L.A.; Ensslin, N.

    1996-12-31

    This paper reviews the principles of calorimetric assay and evaluates its potential application to the minor actinides (U-232-4, Am-241, Am- 243, Cm-245, Np-237). We conclude that calorimetry and high- resolution gamma-ray isotopic analysis can be used for the assay of minor actinides by adapting existing methodologies for Pu/Am-241 mixtures. In some cases, mixtures of special nuclear materials and minor actinides may require the development of new methodologies that involve a combination of destructive and nondestructive assay techniques.

  12. Calorimetric assay of minor actinides

    This paper reviews the principles of calorimetric assay and evaluates its potential application to the minor actinides (U-232-4, Am-241, Am- 243, Cm-245, Np-237). We conclude that calorimetry and high- resolution gamma-ray isotopic analysis can be used for the assay of minor actinides by adapting existing methodologies for Pu/Am-241 mixtures. In some cases, mixtures of special nuclear materials and minor actinides may require the development of new methodologies that involve a combination of destructive and nondestructive assay techniques

  13. Multi-podant diglycolamides and room temperature ionic liquid impregnated resins: An excellent combination for extraction chromatography of actinides.

    Gujar, R B; Ansari, S A; Verboom, W; Mohapatra, P K

    2016-05-27

    Extraction chromatography resins, prepared by impregnating two multi-podant diglycolamide ligands, viz. diglycolamide-functionalized calix[4]arene (C4DGA) and tripodal diglycolamide (T-DGA) dissolved in the room temperature ionic liquid 1-butyl-3-methylimidazolium bis(trifluoromethanesulfonyl)amide (RTIL: C4mimTf2N) on Chromosorb-W (an inert solid support), gave excellent results for the removal of trivalent actinides from acidic waste solutions. Distribution coefficient measurements on several metal ions showed selective sorption of Am(III) over hexavalent uranyl ions and other fission product elements such as strontium and cesium. The sorbed metal ions could be efficiently desorbed with a complexing solution containing guanidine carbonate and EDTA buffer. The sorption of Am(III) on both resins followed pseudo-second order rate kinetics with rate constants of 1.37×10(-6) and 6.88×10(-7)g/cpmmin for T-DGA and C4DGA resins, respectively. The metal sorption on both resins indicated the Langmuir monolayer chemisorption phenomenon with Eu(III) sorption capacities of 4.83±0.21 and 0.52±0.05mg per g of T-DGA and C4DGA resins, respectively. The results of column studies show that these resins are of interest for a possible application for the recovery of hazardous trivalent actinides from dilute aqueous solutions. PMID:27130582

  14. In-beam studies of high-spin states of actinide nuclei

    High-spin states in the actinides have been studied using Coulomb- excitation, inelastic excitation reactions, and one-neutron transfer reactions. Experimental data are presented for states in 232U, 233U, 234U, 235U, 238Pu and 239Pu from a variety of reactions. Energy levels, moments-of-inertia, aligned angular momentum, Routhians, gamma-ray intensities, and cross-sections are presented for most cases. Additional spectroscopic information (magnetic moments, M1/E2 mixing ratios, and g-factors) is presented for 233U. One- and two-neutron transfer reaction mechanisms and the possibility of band crossings (backbending) are discussed. A discussion of odd-A band fitting and Cranking calculations is presented to aid in the interpretation of rotational energy levels and alignment. In addition, several theoretical calculations of rotational populations for inelastic excitation and neutron transfer are compared to the data. Intratheory comparisons between the Sudden Approximation, Semi-Classical, and Alder-Winther-DeBoer methods are made. In connection with the theory development, the possible signature for the nuclear SQUID effect is discussed. 98 refs., 61 figs., 21 tabs

  15. Hydride interference on the determination of minor actinide isotopes by inductively coupled plasma mass spectrometry

    Hydrogen adducts of the major naturally occurring actinide isotopes 232Th and 238U were studied using an inductively coupled plasma mass spectrometer. The hydride:atomic ion ratios for both elements varied as a function of the parameters that were studied, i.e., nebulizer flow rate, solution uptake rate and desolvation conditions. When the instrument sensitivity for U and Th was optimized, 232ThH+:232Th+ was found to be (3.9±0.2) x 10-5 with pneumatic nebulization and (2.10±0.07) x 10-5 with ultrasonic nebulization. Under the same conditions, 238UH+:238U+ was found to be (3.2±0.2) x 10-5 and (1.8±0.1) x 10-5 using pneumatic and ultrasonic nebulization, respectively. Conditions that reduced hydrogen number density and/or increased plasma temperature decreased the hydride:atomic ion ratio. Such conditions are best if 233U and 239Pu are to be determined in the presence of 232Th and 238U. (Author)

  16. Recent actinide nuclear data efforts with the DANCE 4π BaF2 array

    Much of the recent work in the DANCE collaboration has focused on nuclides of interest to stockpile stewardship, attribution science and the advanced fuel cycle initiative. As an example, we have recently begun a program to produce high precision measurements of the key production and destruction reactions of important nuclear fuel elements and radiochemical diagnostic isotopes. The neutron capture targets that have been fielded under this program include several isotopes of uranium, plutonium and americium. However, neutron capture measurements on many of the actinides are complicated by the presence of γ-rays arising from low energy neutron-induced fission. To overcome this difficulty we have designed and implemented a dual parallel-plate avalanche counter fission-tagging detector. This design provides a high efficiency for detecting fission fragments and is self-contained to allow loading of pre-assembled target/detector assemblies into the neutron beam line at DANCE. Neutron capture measurements have been performed on 234,235,236U. The results for 236U are consistent with the Endf/B-6 evaluation while the results for 234U are as much as 20% lower than the Endf/B-6 evaluation in the keV region. The DANCE results for 234U(n,γ) have been incorporated into the Endf/B-7 evaluation. Planned measurements on 238,239Pu are also discussed

  17. In-beam studies of high-spin states of actinide nuclei

    Stoyer, M.A. (Lawrence Berkeley Lab., CA (USA). Nuclear Science Div. California Univ., Berkeley, CA (USA). Dept. of Chemistry)

    1990-11-15

    High-spin states in the actinides have been studied using Coulomb- excitation, inelastic excitation reactions, and one-neutron transfer reactions. Experimental data are presented for states in {sup 232}U, {sup 233}U, {sup 234}U, {sup 235}U, {sup 238}Pu and {sup 239}Pu from a variety of reactions. Energy levels, moments-of-inertia, aligned angular momentum, Routhians, gamma-ray intensities, and cross-sections are presented for most cases. Additional spectroscopic information (magnetic moments, M{sub 1}/E{sub 2} mixing ratios, and g-factors) is presented for {sup 233}U. One- and two-neutron transfer reaction mechanisms and the possibility of band crossings (backbending) are discussed. A discussion of odd-A band fitting and Cranking calculations is presented to aid in the interpretation of rotational energy levels and alignment. In addition, several theoretical calculations of rotational populations for inelastic excitation and neutron transfer are compared to the data. Intratheory comparisons between the Sudden Approximation, Semi-Classical, and Alder-Winther-DeBoer methods are made. In connection with the theory development, the possible signature for the nuclear SQUID effect is discussed. 98 refs., 61 figs., 21 tabs.

  18. Recent actinide nuclear data efforts with the DANCE 4{pi} BaF{sub 2} array

    Bredeweg, T.A.; Bond, E.M.; Couture, A.J.; Fitzpatrick, J.R.; Haight, R.C.; Hill, T.S.; Jandel, M.; O' Donnell, J.M.; Reifarth, R.; Rundberg, R.S.; Slemmons, A.K.; Tovesson, F.K.; Ullmann, J.L.; Vieira, D.J.; Wilhelmy, J.B.; Fowler, M.M.; Wouters, J.M. [Los Alamos National Laboratory, Los Alamos, NM (United States); Agvaanluvsan, U.; Becker, J.A.; Macri, R.A.; Parker, W.E.; Wilk, P.A.; Wu, C.Y. [Lawrence Livermore National Laboratory, Livermore, CA (United States); Ethvignot, T.; Granier, T. [CEA Bruyeres-le-Chatel, 91 (France)

    2008-07-01

    Much of the recent work in the DANCE collaboration has focused on nuclides of interest to stockpile stewardship, attribution science and the advanced fuel cycle initiative. As an example, we have recently begun a program to produce high precision measurements of the key production and destruction reactions of important nuclear fuel elements and radiochemical diagnostic isotopes. The neutron capture targets that have been fielded under this program include several isotopes of uranium, plutonium and americium. However, neutron capture measurements on many of the actinides are complicated by the presence of {gamma}-rays arising from low energy neutron-induced fission. To overcome this difficulty we have designed and implemented a dual parallel-plate avalanche counter fission-tagging detector. This design provides a high efficiency for detecting fission fragments and is self-contained to allow loading of pre-assembled target/detector assemblies into the neutron beam line at DANCE. Neutron capture measurements have been performed on {sup 234,235,236}U. The results for {sup 236}U are consistent with the Endf/B-6 evaluation while the results for {sup 234}U are as much as 20% lower than the Endf/B-6 evaluation in the keV region. The DANCE results for {sup 234}U(n,{gamma}) have been incorporated into the Endf/B-7 evaluation. Planned measurements on {sup 238,239}Pu are also discussed.

  19. Prompt fission neutron emission in resonance fission of 239Pu

    The prompt fission neutron emission probability was investigated at the time-of-flight facility GELINA at the IRMM. A double Frisch-gridded ionization chamber was used as a fission fragment detector. For the data acquisition of both fission fragment signals as well as the neutron detector signals the fast digitization technique has been applied. For the neutron detection large volume liquid scintillation detectors from the DEMON collaboration were used. A specialized data analysis program taking advantage of the digital filtering technique has been developed to treat the acquired data

  20. 239Pu metabolism in the blood after its intratracheal administration

    The kinetics of the resorbed from the lungs plutonium metabolism and the forms of its presence in the blood as well as the dynamics of its deposit in the organs of secondary deposition (liver, skeleton) were studied in experiment with female rats. It was shown (gel-filtration method) that plutonium is present in blood serum in various physico-chemical forms: bound with macroglobulin, γ-globulin and albumin-transferrin fractions of proteins and not bound with proteins; this or that form of plutonium may dominate in time (4 min-64 days)

  1. Some comments on the toxicity of 239Pu

    There is no simple method of expressing a concept such as toxicity. The toxicity of a material depends upon its form (solid, liquid, or gas), the method of entry into the body (ingestion, inhalation, or abrasion), and the individual it enters (young, old, sick, well, heavy cigarette smoker, or consumer of alcohol). Thus, statements such as ''plutonium is the most toxic material known to man'' are not only incorrect; they are meaningless. By taking the one aspect of plutonium which can be quantitated in a meaningful manner, the induction of malignant bone sarcomas in humans, the incremental risk presented to those who have been exposed to this radioelement has been shown to be quite small. By means of a hypothetical exposure of radium dial workers to plutonium instead of radium, an industry-wide exposure to plutonium would have been less harmful than the actual exposure to radium, in spite of the fact that plutonium appears to be far more toxic than radium. Further, the observation that, after radium was recognized as a toxic material, it no longer was a hazard in the dial industry, clearly demonstrates that hazardous radioactive materials can be handled safely. This has been demonstrated again with plutonium, for even though much larger quantities have been handled by many more individuals, there are no demonstrable cases of malignancies induced by this hazardous material. The absence of clearly demonstrable excesses of lung cancer in the large group of long-term thorium workers is reassuring, for it may imply that low doses to the lung have a very low probability of inducing lung cancers. It is concluded that plutonium, a highly toxic material, can be handled safely, as are many other hazardous materials that play important roles in our daily lives

  2. Actinides detection in the Pacific Coast of Mexico; Deteccion de actinidos en el Litoral Pacifico de Mexico

    Ordonez R, E.; Almazan T, M. G.; Cruz C, G. J.; Ramirez S, R., E-mail: eduardo.ordonez@inin.gob.mx [ININ, Carretera Mexico-Toluca s/n, 52750 Ocoyoacac, Estado de Mexico (Mexico)

    2013-10-15

    In this work is evaluated the activity of the alpha emitters, uranium and plutonium, in sand samples and seawater coming from diverse points of the Mexican Pacific Coast (Baja California, Jalisco, Colima and Guerrero). The used techniques were: radiochemistry separation and alpha spectrometry, with these techniques could be observed that the sand contains natural uranium and trace quantities of {sup 239}Pu and {sup 240}Pu combinations. The biggest activity in Pu was found in Finisterra, Baja California Sur (0.13 Bq/kg) and the minor (0 Bq/kg) in Miramar, Colima. The relationship between the geographical localization and the Pu activity suggests that while there is more interaction of the site with the oceanic currents, more is the content of Pu in the sands of the coast. (Author)

  3. ALMR potential for actinide consumption

    The Advanced Liquid Metal Reactor (ALMR) is a US Department of Energy (DOE) sponsored fast reactor design based on the Power Reactor, Innovative Small Module (PRISM) concept originated by General Electric. This reactor combines a high degree of passive safety characteristics with a high level of modularity and factory fabrication to achieve attractive economics. The current reference design is a 471 MWt modular reactor fueled with ternary metal fuel. This paper discusses actinide transmutation core designs that fit the design envelope of the ALMR and utilize spent LWR fuel as startup material and for makeup. Actinide transmutation may be accomplished in the ALMR core by using either a breeding or burning configuration. Lifetime actinide mass consumption is calculated as well as changes in consumption behavior throughout the lifetime of the reactor. Impacts on system operational and safety performance are evaluated in a preliminary fashion. Waste disposal impacts are discussed. (author)

  4. Comparison of actinide production in traveling wave and pressurized water reactors

    The geopolitical problems associated with civilian nuclear energy production arise in part from the accumulation of transuranics in spent nuclear fuel. A traveling wave reactor is a type of breed-burn reactor that could, if feasible, reduce the overall production of transuranics. In one possible configuration, a cylinder of natural or depleted uranium would be subjected to a fast neutron flux at one end. The neutrons would transmute the uranium, producing plutonium and higher actinides. Under the right conditions, the reactor could become critical, at which point a self-stabilizing fission wave would form and propagate down the length of the reactor cylinder. The neutrons from the fission wave would burn the fissile nuclides and transmute uranium ahead of the wave to produce additional fuel. Fission waves in uranium are driven largely by the production and fission of 239Pu. Simulations have shown that the fuel burnup can reach values greater than 400 MWd/kgIHM, before fission products poison the reaction. In this work we compare the production of plutonium and minor actinides produced in a fission wave to that of a UOX fueled light water reactor, both on an energy normalized basis. The nuclide concentrations in the spent traveling wave reactor fuel are computed using a one-group diffusion model and are verified using Monte Carlo simulations. In the case of the pressurized water reactor, a multi-group collision probability model is used to generate the nuclide quantities. We find that the traveling wave reactor produces about 0.187 g/MWd/kgIHM of transuranics compared to 0.413 g/MWd/kgIHM for a pressurized water reactor running fuel enriched to 4.95 % and burned to 50 MWd/kgIHM. (authors)

  5. Comparison of actinide production in traveling wave and pressurized water reactors

    Osborne, A.G.; Smith, T.A.; Deinert, M.R. [Department of Mechanical Engineering, University of Texas at Austin, Austin, TX (United States)

    2013-07-01

    The geopolitical problems associated with civilian nuclear energy production arise in part from the accumulation of transuranics in spent nuclear fuel. A traveling wave reactor is a type of breed-burn reactor that could, if feasible, reduce the overall production of transuranics. In one possible configuration, a cylinder of natural or depleted uranium would be subjected to a fast neutron flux at one end. The neutrons would transmute the uranium, producing plutonium and higher actinides. Under the right conditions, the reactor could become critical, at which point a self-stabilizing fission wave would form and propagate down the length of the reactor cylinder. The neutrons from the fission wave would burn the fissile nuclides and transmute uranium ahead of the wave to produce additional fuel. Fission waves in uranium are driven largely by the production and fission of {sup 239}Pu. Simulations have shown that the fuel burnup can reach values greater than 400 MWd/kgIHM, before fission products poison the reaction. In this work we compare the production of plutonium and minor actinides produced in a fission wave to that of a UOX fueled light water reactor, both on an energy normalized basis. The nuclide concentrations in the spent traveling wave reactor fuel are computed using a one-group diffusion model and are verified using Monte Carlo simulations. In the case of the pressurized water reactor, a multi-group collision probability model is used to generate the nuclide quantities. We find that the traveling wave reactor produces about 0.187 g/MWd/kgIHM of transuranics compared to 0.413 g/MWd/kgIHM for a pressurized water reactor running fuel enriched to 4.95 % and burned to 50 MWd/kgIHM. (authors)

  6. Leaching of actinide-doped nuclear waste glass in a tuff-dominated system

    A laboratory leaching test has been performed as part of a project to evaluate the suitability of tuff rocks at Yucca Mountain, Nevada, as a site for a high-level nuclear waste repository. Glass samples were placed in water inside tuff vessels, and then the tuff vessels were placed in water inside Teflon containers. Glass-component leach rates and migration through the tuff were measured for samples of the ATM-8 actinide glass, which is a PNL 76-68 based glass doped with low levels of 99Tc, 237Np, 238U, and 239Pu to simulate wastes. Disc samples of this glass were leached at 900C for 30, 90, and 183 days inside tuff vessels using a natural groundwater (J-13 well-water) as the leachant. At the end of each leaching interval, the J-13 water present inside and outside the rock vessel was analyzed for glass components in solutions. Boron, molybdenum, and technetium appear to migrate through the rock at rates that depend on the porosity of each vessel and the time. The actinide elements were found only in the inner leachate. Normalized elemental mass loss values for boron, molybdenum, and technetium were calculated using concentrations of the inner and outer leachates and assuming a negligible retention on the rock. The maximum normalized release was 2.3 g/m2 for technetium. Boron, molybdenum, technetium, and neptunium were released linearly with respect to each other, with boron and molybdenum released at about 85% of the technetium rate, and neptunium at 5 to 10% of the technetium rate. Plutonium was found at low levels in the inner leachate but was strongly sorbed on the steel and Teflon supports. Neptunium was sorbed to a lesser extent. 8 refs., 6 figs., 6 tabs

  7. Chemical compatibility of HLW borosilicate glasses with actinides

    During liquid storage of HLLW the formation of actinide enriched sludges is being expected. Also during melting of HLW glasses an increase of top-to-bottom actinide concentrations can take place. Both effects have been studied. Besides, the vitrification of plutonium enriched wastes from Pu fuel element fabrication plants has been investigated with respect to an isolated vitrification process or a combined one with the HLLW. It is shown that the solidification of actinides from HLLW and actinide waste concentrates will set no principal problems. The leaching of actinides has been measured in salt brine at 230C and 1150C. (orig.)

  8. The lanthanides and actinides

    This paper relates the chemical properties of the actinides to their position in the Mendeleev periodic system. The changes in the oxidation states of the actinides with increasing atomic number are similar to those of the 3d elements. Monovalent and divalent actinides are very similar to alkaline and alkaline earth elements; in the 3+ and 4+ oxidation states they resemble d elements in the respective oxidation states. However, in their highest oxidation states the actinides display their individual properties with only a slight resemblance to d elements. Finally, there is a profound similarity between the second half of the actinides and the first half of the lanthanides

  9. Determination of long-lived fission products and actinides in Savannah River Site HLW sludge and glass for waste acceptance

    Savannah River Site (SRS) is immobilizing the radioactive, high-level waste sludge in Tank 51 into a borosilicate glass for disposal in a geologic repository. A requirement for repository acceptance is that SRS report the concentrations of certain fission product and actinide radionuclides in the glass. This paper presents measurements of many of these concentrations in both Tank 51 sludge and the final glass. The radionuclides were measured by inductively coupled plasma mass spectrometry and α, β, and γ counting methods. Examples of the radionuclides are 90Sr, 137Cs, 238U and , 239Pu. Concentrations in the glass are 3.1 times lower due to dilution of the sludge with a nonradioactive glass forming frit in the vitrification process. Results also indicated that in both the sludge and glass the relative concentrations of the long lived fission products insoluble in caustic are in proportion to their yields from the fission of 235U waste in the SRS reactors. This allowed the calculation of a fission yield scaling factor. This factor in addition to the sludge dilution factor can be used to estimate concentrations of waste acceptance radionuclides that cannot be measured in the glass. Examples of these radionuclides are 79Se, 93Zr, and 107Pd. (author)

  10. DEVELOPMENT OF AN IMPROVED TITANATE-BASED SORBENT FOR STRONTIUM AND ACTINIDE SEPARATIONS UNDER STRONGLY ALKALINE CONDITIONS

    Hobbs, D.; Peters, T.; Taylor-Pashow, K.; Fink, S.

    2010-02-18

    High-level nuclear waste produced from fuel reprocessing operations at the Savannah River Site (SRS) requires pretreatment to remove {sup 134,137}Cs, {sup 90}Sr, and alpha-emitting radionuclides (i.e., actinides) prior to disposal onsite as low level waste. Separation processes at SRS include the sorption of {sup 90}Sr and alpha-emitting radionuclides onto monosodium titanate (MST) and caustic side solvent extraction of {sup 137}Cs. The MST and separated {sup 137}Cs is encapsulated along with the sludge fraction of high-level waste (HLW) into a borosilicate glass waste form for eventual entombment at a federal repository. The predominant alpha-emitting radionuclides in the highly alkaline waste solutions include plutonium isotopes {sup 238}Pu, {sup 239}Pu, and {sup 240}Pu; {sup 237}Np; and uranium isotopes, {sup 235}U and {sup 238}U. This paper describes recent results evaluating the performance of an improved sodium titanate material that exhibits increased removal kinetics and capacity for {sup 90}Sr and alpha-emitting radionuclides compared to the current baseline material, MST.

  11. The OSMOSE program for the qualification of integral cross sections of actinides: Preliminary results in a PWR-UOx spectrum

    The need for improved nuclear data for minor actinides has been stressed by various organizations throughout the world - especially for studies relating to plutonium management, waste incineration, transmutation of waste, and Pu burning in future nuclear concepts. Several international programs have indicated a strong desire to obtain accurate integral reaction rate data for improving the major and minor actinides cross sections. Data on major actinides (i.e. 235U, 236U, 238U, 239Pu, 240Pu, 241Pu, 242Pu and 241Am) are reasonably well-known and available in the Evaluated Nuclear Data Files (JEFF, JENDL, ENDF-BX However information on the minor actinides (i.e. 232Th, 233U, 237Np, 238Pu, 242Am, 243Am, 243Cm, 235Cm, 244Cm, 245Cm, 246Cm and 247Cm) is less well-known and considered to be relatively poor in some cases, having to rely on model and extrapolation of few data points. In this framework, the ambitious OSMOSE program between the Commissariat a l'Energie Atomique (CEA), Electricite de France (EDF) and the U.S. Dept. of Energy (DOE) has been undertaken with the aim of measuring the integral absorption rate parameters of actinides in the MINERVE experimental facility located at the CEA Cadarache Research Center. The OSMOSE Program (Oscillation in Minerve of isotopes in 'Eupraxic' Spectra) includes a complete analytical program associated with the experimental measurement program and aims at understanding and resolving potential discrepancies between calculated and measured values. In the OSMOSE program, the reactivity worth of samples containing separated actinides are measured in different neutron spectra using an oscillation technique with an overall expected accuracy better than 3%. Reactivity effects of less than 10 pcm (0.0001 or approximately 1.5 cents) are measured and compared with calibrations to determine the differential reactivity-worth of the individual samples. The first experimental results were obtained with a very good reproducibility in 2005 and

  12. Lanthanides and actinides in ionic liquids

    Binnemans, Koen

    2007-01-01

    This lecture gives an overview of the research possibilities offered by combining f-elements (lanthanides and actinides) with ionic liquids [1] Many ionic liquids are solvents with weakly coordinating anions. Solvation of lanthanide and actinide ions in these solvents is different from what is observed in conventional organic solvents and water. The poorly solvating behavior can also lead to the formation of coordination compounds with low coordination numbers. The solvation of f-elements can...

  13. Actinides and the environment

    The book combines in one volume the opinions of experts regarding the interaction of radionuclides with the environment and possible ways to immobilize and dispose of nuclear waste. The relevant areas span the spectrum from pure science, such as the fundamental physics and chemistry of the actinides, geology, environmental transport mechanisms, to engineering issues such as reactor operation and the design of nuclear waste repositories. The cross-fertilization between these various areas means that the material in the book will be accessible to seasoned scientists who may wish to obtain an overview of the current state of the art in the field of environmental remediation of radionuclides, as well as to beginning scientists embarking on a career in this field. refs

  14. Actinide environmental chemistry

    In order to predict release and transport rates, as well as design cleanup and containment methods, it is essential to understand the chemical reactions and forms of the actinides under aqueous environmental conditions. Four important processes that can occur with the actinide cations are: precipitation, complexation, sorption and colloid formation. Precipitation of a solid phase will limit the amount of actinide in solution near the solid phase and have a retarding effect on release and transport rates. Complexation increases the amount of actinide in solution and tends to increase release and migration rates. Actinides can sorb on to mineral or rock surfaces which tends to retard migration. Actinide ions can form or become associated with colloidal sized particles which can, depending on the nature of the colloid and the solution conditions, enhance or retard migration of the actinide. The degree to which these four processes progress is strongly dependent on the oxidation state of the actinide and tends to be similar for actinides in the same oxidation state. In order to obtain information on the speciation of actinides in solution, i.e., oxidation state, complexation form, dissolved or colloidal forms, the use of absorption spectroscopy has become a method of choice. The advent of the ultrasensitive, laser induced photothermal and fluorescence spectroscopies has made possible the detection and study of actinide ions at the parts per billion level. With the availability of third generation synchrotrons and the development of new fluorescence detectors, X-ray absorption spectroscopy (XAS) is becoming a powerful technique to study the speciation of actinides in the environment, particularly for reactions at the solid/solution interfaces. (orig.)

  15. New developments and methodology for actinide measurements at ultra trace levels

    Full text: The methodology developed in our laboratory is based on the combination of radiochemistry conducted in the cleanest laboratories, prior to measurements using mass spectrometers with detection limits in the sub femtogram range. The work describes first the different radiochemical procedures that are needed to completely purify a sample. When femtogram levels of 239Pu or 240Pu have to be measured, the matrix and uranium have to be completely removed. First to avoid the interferences generated on 239Pu by uranium hydrides i.e. 238UH and secondly to avoid the interferences of polyatomics generated by lead, bismuth, mercury...The contribution of 199Hg40Ar, 204Hg35Cl or 202Hg37Cl on 239Pu have been quantified and it is close to 10-6. Consequently, the radiochemistry, mainly based on anionic chromatography performed using ultra-pure reagents at crucial steps is detailed, leading to blanks with no more than ppt levels of 238U, lead, bismuth and mercury. Then, the way to improve the performance of mass spectrometers, ICP-MS and TIMS is described. Very low ICP-MS detection limits are a combination of very high sensitivity, low backgrounds and very low sample consumption. Low consumption is achieved by using micro nebulisers with a flow rate which doesn't exceed 50μl.min-1 without decreasing sensitivity. Enhancement of sensitivity with micro nebulisers is then possible by using desolvating systems that completely remove water from the sample, resulting in an increase in sensitivity by a factor of ten. Better performance of ICP-MS is also achievable when a collision cell is added, in order to decrease uranium hydrides and other polyatomics. Concerning TIMS, which generally suffers from a lack in sensitivity, total consumption of sample was studied in order to get better detection limits with respect to uranium isotopes and specifically 236U. The performance of TIMS and ICP-MS in terms of detection limits, precision, reliability, mass bias and isotopic fractionation

  16. The OSMOSE Experimental Program for the qualification of integral cross sections of actinides

    The need of better nuclear data on minor actinides has been stressed by various organizations throughout the world. It especially deals with the studies on plutonium management and waste incineration in existing systems and transmutation of waste or Pu burning in future nuclear concepts. To address this issue, a Working Party of the OECD has been concerned with identifying these needs and has produced a detailed High Priority Request List for Nuclear Data. The first step in obtaining better nuclear data consists in measuring accurate integral data and comparing them to integrated energy dependent data: this comparison provides a direct assessment of the effect of deficiencies in the differential data. Several international programs have indicated a strong desire to obtain accurate integral reaction rate data for improving the major and minor actinides cross sections. Data on major actinides (i.e. 235U, 236U, 238U, 239Pu, 240Pu, 241Pu, 242Pu and 241Am) are reasonably well-known and available in the Evaluated Nuclear Data Files (JEFF, JENDL, ENDF-B). However information on the minor actinides (i.e. 232Th, 233U, 237Np, 238Pu, 242Am, 243Am, 242Cm, 243Cm, 244Cm, 245Cm, 246Cm and 247Cm) is less well-known and considered to be relatively poor in some cases, having to rely on model and extrapolation of few data points. In this framework, the ambitious OSMOSE program between the Commissariat a l'Energie Atomique (CEA), Electricite de France (EDF) and the U.S. Department of Energy (DOE) has been undertaken with the aim of measuring the integral absorption rate parameters of actinides in the MINERVE experimental facility located at the CEA Cadarache Research Center. The OSMOSE Program (Oscillation in Minerve of isOtopes in 'Eupraxic' Spectra) includes a complete analytical program associated with the experimental measurement program and aims at understanding and resolving potential discrepancies between calculated and measured values. The OSMOSE program began in 2005 and will

  17. Immobilization of tetravalent actinides in three phosphate based ceramics: britholites, TPD and monazites/brabantites

    Three phosphate based ceramics were studied for the immobilization of tri- and tetravalent actinides: britholites Ca9Nd1-xAnxIV(PO4)5-x(SiO4)1+xF2, monazites/brabantites Ln1-2xIIICaxAnxIVPO4 and Thorium Phosphate Diphosphate (TPD) Th4-xAnxIV(PO4)4P2O7. For each material, the incorporation of Th, U(IV), or Ce(IV) in the structure was examined. This work was the early beginning of the incorporation of 239Pu and/or 238Pu in order to evaluate the effects of α -decay on these three crystallographic structures. The syntheses were carried out using dry chemistry methods, involving mechanical grinding then heating treatment (1100 deg C ≤ θ ≤ 1400 deg C). For britholites, we showed that the incorporation of thorium was complete for weight loading lower than 20 wt.% through the (Nd3+, PO43-) ↔ (Th4+, SiO44-) coupled substitution, leading to the preparation of solid solutions. Due to redox problems, the incorporation of uranium was limited to 5 to 8 wt.% and always led to a two-phase mixture of U-britholite and CaU2O5+y. For solid solutions based on TPD and for brabantites, the syntheses dealing with the incorporation of Th and/or U(IV) were improved by dry chemistry method using three mechanical grinding-calcination cycles. For both solids, homogeneous and single phase samples of the corresponding solid solutions were obtained. Finally, dense pellets of britholites, monazites/brabantites and TAnIVPD solid solutions were prepared in order to study their chemical durability during leaching tests. (authors)

  18. Research in actinide chemistry

    This research studies the behavior of the actinide elements in aqueous solution. The high radioactivity of the transuranium actinides limits the concentrations which can be studied and, consequently, limits the experimental techniques. However, oxidation state analogs (trivalent lanthanides, tetravalent thorium, and hexavalent uranium) do not suffer from these limitations. Behavior of actinides in the environment are a major USDOE concern, whether in connection with long-term releases from a repository, releases from stored defense wastes or accidental releases in reprocessing, etc. Principal goal of our research was expand the thermodynamic data base on complexation of actinides by natural ligands (e.g., OH-, CO32-, PO43-, humates). The research undertakes fundamental studies of actinide complexes which can increase understanding of the environmental behavior of these elements

  19. On the combination of delayed neutron and delayed gamma techniques for fission rate measurement in nuclear fuel

    Novel techniques to measure newly induced fissions in spent fuel after re-irradiation at low power have been developed and tested at the Proteus zero-power research reactor. The two techniques are based on the detection of high energy gamma-rays emitted by short-lived fission products and delayed neutrons. The two techniques relate the measured signals to the total fission rate, the isotopic composition of the fuel, and nuclear data. They can be combined to derive better estimates on each of these parameters. This has potential for improvement in many areas. Spent fuel characterisation and safeguard applications can benefit from these techniques for non-destructive assay of plutonium content. Another application of choice is the reduction of uncertainties on nuclear data. As a first application of the combination of the delayed neutron and gamma measurement techniques, this paper shows how to reduce the uncertainties on the relative abundances of the longest delayed neutron group for thermal fissions in 235U, 239Pu and fast fissions in 238U. The proposed experiments are easily achievable in zero-power research reactors using fresh UO2 and MOX fuel and do not require fast extraction systems. The relative uncertainties (1σ) on the relative abundances are expected to be reduced from 13% to 4%, 16% to 5%, and 38% to 12% for 235U, 238U and 239Pu, respectively. (authors)

  20. TUCS/phosphate mineralization of actinides

    Nash, K.L. [Argonne National Lab., IL (United States)

    1997-10-01

    This program has as its objective the development of a new technology that combines cation exchange and mineralization to reduce the concentration of heavy metals (in particular actinides) in groundwaters. The treatment regimen must be compatible with the groundwater and soil, potentially using groundwater/soil components to aid in the immobilization process. The delivery system (probably a water-soluble chelating agent) should first concentrate the radionuclides then release the precipitating anion, which forms thermodynamically stable mineral phases, either with the target metal ions alone or in combination with matrix cations. This approach should generate thermodynamically stable mineral phases resistant to weathering. The chelating agent should decompose spontaneously with time, release the mineralizing agent, and leave a residue that does not interfere with mineral formation. For the actinides, the ideal compound probably will release phosphate, as actinide phosphate mineral phases are among the least soluble species for these metals. The most promising means of delivering the precipitant would be to use a water-soluble, hydrolytically unstable complexant that functions in the initial stages as a cation exchanger to concentrate the metal ions. As it decomposes, the chelating agent releases phosphate to foster formation of crystalline mineral phases. Because it involves only the application of inexpensive reagents, the method of phosphate mineralization promises to be an economical alternative for in situ immobilization of radionuclides (actinides in particular). The method relies on the inherent (thermodynamic) stability of actinide mineral phases.

  1. Research in actinide chemistry

    1991-01-01

    This report contains research results on studies of inorganic and organic complexes of actinide and lanthanide elements. Special attention is given to complexes of humic acids and to spectroscopic studies.

  2. Production and investigation of thin films of metal actinides (Pu, Am, Cm, Bk, Cf)

    Radchenko, V. M.; Ryabinin, M. A.; Stupin, V. A.

    2010-03-01

    Under limited availability of transplutonium metals some special techniques and methods of their production have been developed that combine the process of metal reduction from a chemical compound and preparation of a sample for examination. In this situation the evaporation and condensation of metal onto a substrate becomes the only possible technology. Thin film samples of metallic 244Cm, 248Cm and 249Bk were produced by thermal reduction of oxides with thorium followed by deposition of the metals in the form of thin layers on tantalum substrates. For the production of 249Cf metal in the form of a thin layer the method of thermal reduction of oxide with lanthanum was used. 238Pu and 239Pu samples in the form of films were prepared by direct high temperature evaporation and condensation of the metal onto a substrate. For the production of 241Am films a gram sample of plutonium-241 metal was used containing about 18 % of americium at the time of production. Thermal decomposition of Pt5Am intermetallics in vacuum was used to produce americium metal with about 80% yield. Resistivity of the metallic 249Cf film samples was found to decrease exponentially with increasing temperature. The 249Cf metal demonstrated a tendency to form preferably a DHCP structure with the sample mass increasing. An effect of high specific activity on the crystal structure of 238Pu nuclide thin layers was studied either.

  3. Production and investigation of thin films of metal actinides (Pu, Am, Cm, Bk, Cf)

    Under limited availability of transplutonium metals some special techniques and methods of their production have been developed that combine the process of metal reduction from a chemical compound and preparation of a sample for examination. In this situation the evaporation and condensation of metal onto a substrate becomes the only possible technology. Thin film samples of metallic 244Cm, 248Cm and 249Bk were produced by thermal reduction of oxides with thorium followed by deposition of the metals in the form of thin layers on tantalum substrates. For the production of 249Cf metal in the form of a thin layer the method of thermal reduction of oxide with lanthanum was used. 238Pu and 239Pu samples in the form of films were prepared by direct high temperature evaporation and condensation of the metal onto a substrate. For the production of 241Am films a gram sample of plutonium-241 metal was used containing about 18 % of americium at the time of production. Thermal decomposition of Pt5Am intermetallics in vacuum was used to produce americium metal with about 80% yield. Resistivity of the metallic 249Cf film samples was found to decrease exponentially with increasing temperature. The 249Cf metal demonstrated a tendency to form preferably a DHCP structure with the sample mass increasing. An effect of high specific activity on the crystal structure of 238Pu nuclide thin layers was studied either.

  4. The clearance of Pu and Am from the respiratory system of rodents after the inhalation of oxide aerosols of these actinides either alone or in combination with other metals

    In this series of studies in rodents the lung clearance and tissue distribution of both plutonium and americium have been measured following their inhalation as mixed actinide oxides either alone or in combination with other metals. The aerosols used were materials to which workers in the nuclear industry may be occupationally exposed or which could be generated in the event of an accident in a reactor core or fuel fabrication plant. The studies showed that, at least for some PuO2 aerosols, the lung model currently being used by ICRP for estimating tissue doses from inhaled actinides may overestimate, by about a factor of ten, the amount of plutonium translocated to the blood. The presence of oxides of other metals can, however, appreciably influence the clearance of plutonium from the lung. While in some mixtures plutonium dioxide behaves as an insoluble (Class Y) compound and in others as a soluble (Class W) compound, it may also have transportability characteristics between these two extremes. Americium-241 behaves as a soluble (Class W) compound when inhaled as the oxide. However, if it is present in trace quantities in mixed-oxide aerosols its behaviour depends upon that of the materials present in greatest mass. (author)

  5. Actinide isotopic analysis systems

    This manual provides instructions and procedures for using the Lawrence Livermore National Laboratory's two-detector actinide isotope analysis system to measure plutonium samples with other possible actinides (including uranium, americium, and neptunium) by gamma-ray spectrometry. The computer program that controls the system and analyzes the gamma-ray spectral data is driven by a menu of one-, two-, or three-letter options chosen by the operator. Provided in this manual are descriptions of these options and their functions, plus detailed instructions (operator dialog) for choosing among the options. Also provided are general instructions for calibrating the actinide isotropic analysis system and for monitoring its performance. The inventory measurement of a sample's total plutonium and other actinides content is determined by two nondestructive measurements. One is a calorimetry measurement of the sample's heat or power output, and the other is a gamma-ray spectrometry measurement of its relative isotopic abundances. The isotopic measurements needed to interpret the observed calorimetric power measurement are the relative abundances of various plutonium and uranium isotopes and americium-241. The actinide analysis system carries out these measurements. 8 figs

  6. Incorporation of tetravalent actinides in three phosphated matrices: britholite, monazite/brabandite and thorium phosphate diphosphate (β-TPD)

    Three phosphate based ceramics were studied for the immobilization of tri- and tetravalent actinides: britholite Ca9Nd1-xAnxIV(PO4)5-x(SiO4)1+xF2, monazite/brabantite solid solutions Ln1-2xIII CaxAnxIPO4 and Thorium Phosphate Diphosphate (β-TPD) Th4-xAnxIV(PO4)4P2O7. For each material, the incorporation of thorium and uranium (IV) was studied as a surrogate of plutonium. This work was the early beginning of the incorporation of 239Pu and/or 238Pu in order to evaluate the effects of α-decay on the three crystallographic structures. The incorporation of tetravalent cations was carried out by dry chemistry methods, using mechanical grinding to improve the reactivity of the initial mixture then the homogeneity of final solid prepared after calcination at high temperature (1200-1400 deg C). For britholites, the thorium incorporation was complete for weight loading up to 20 wt.%, leading to the preparation of homogeneous and single phase solid solutions when using the coupled substitution (Nd3+, PO43-) ↔ (Th4+, SiO44-). Due to redox problems, the incorporation of uranium was limited to 5 to 8 wt.% and always led to a two-phase mixture of U-britholite and CaU2O5+y. The preparation of homogeneous solid solutions of β-TUPD and of brabantites containing thorium and uranium samples was successfully obtained using three steps of mechanical grinding/calcination. For each matrix, dense pellets were prepared prior to the study of their chemical behaviour during leaching tests. The chemical durability of brabantites and β-TUPD were found to be close to that reported in literature. The formation of neo-formed phases was also evidenced onto the surface of Th-britholite samples. (author)

  7. Radiochemistry and actinide chemistry

    The analysis of trace amounts of actinide elements by means of radiochemistry, is discussed. The similarities between radiochemistry and actinide chemistry, in the case of species amount by cubic cm below 1012, are explained. The parameters which allow to define what are the observable chemical reactions, are given. The classification of radionuclides in micro or macrocomponents is considered. The validity of the mass action law and the partition function in the definition of the average number of species for trace amounts, is investigated. Examples illustrating the results are given

  8. Actinide separative chemistry

    Actinide separative chemistry has focused very heavy work during the last decades. The main was nuclear spent fuel reprocessing: solvent extraction processes appeared quickly a suitable, an efficient way to recover major actinides (uranium and plutonium), and an extensive research, concerning both process chemistry and chemical engineering technologies, allowed the industrial development in this field. We can observe for about half a century a succession of Purex plants which, if based on the same initial discovery (i.e. the outstanding properties of a molecule, the famous TBP), present huge improvements at each step, for a large part due to an increased mastery of the mechanisms involved. And actinide separation should still focus R and D in the near future: there is a real, an important need for this, even if reprocessing may appear as a mature industry. We can present three main reasons for this. First, actinide recycling appear as a key-issue for future nuclear fuel cycles, both for waste management optimization and for conservation of natural resource; and the need concerns not only major actinide but also so-called minor ones, thus enlarging the scope of the investigation. Second, extraction processes are not well mastered at microscopic scale: there is a real, great lack in fundamental knowledge, useful or even necessary for process optimization (for instance, how to design the best extracting molecule, taken into account the several notifications and constraints, from selectivity to radiolytic resistivity?); and such a need for a real optimization is to be more accurate with the search of always cheaper, cleaner processes. And then, there is room too for exploratory research, on new concepts-perhaps for processing quite new fuels- which could appear attractive and justify further developments to be properly assessed: pyro-processes first, but also others, like chemistry in 'extreme' or 'unusual' conditions (supercritical solvents, sono-chemistry, could be

  9. Neutrons scattering studies in the actinide region

    During the report period were investigated the following areas: prompt fission neutron energy spectra measurements; neutron elastic and inelastic scattering from 239Pu; neutron scattering in 181Ta and 197Au; response of a 235U fission chamber near reaction thresholds; two-parameter data acquisition system; ''black'' neutron detector; investigation of neutron-induced defects in silicon dioxide; and multiple scattering corrections. Four Ph.D. dissertations and one M.S. thesis were completed during the report period. Publications consisted of three journal articles, four conference papers in proceedings, and eleven abstracts of presentations at scientific meetings. There are currently four Ph.D. and one M.S. candidates working on dissertations directly associated with the project. In addition, three other Ph.D. candidates are working on dissertations involving other aspects of neutron physics in this laboratory

  10. Synergistic extraction of actinides : Part I. Hexa-and pentavalent actinides

    A detailed discussion on the reported literature on the synergistic extraction of hexa- and pentavalent actinide ions, by different combinations of extractants and from different aqueous media, is presented. Structural aspects of the various complexes involved in synergism also are reviewed. A short account of the applications based on synergistic extraction is also given. (author)

  11. Photochemistry of the actinides

    It has been found that all three major actinides have a useful variety of photochemical reactions which could be used to achieve a separations process that requires fewer reagents. Several features merit enumerating: (1) Laser photochemistry is not now as uniquely important in fuel reprocessing as it is in isotopic enrichment. The photochemistry can be successfully accomplished with conventional light sources. (2) The easiest place to apply photo-reprocessing is on the three actinides U, Pu, and Np. The solutions are potentially cleaner and more amenable to photoreactions. (3) Organic-phase photoreactions are probably not worth much attention because of the troublesome solvent redox chemistry associated with the photochemical reaction. (4) Upstream process treatment on the raffinate (dissolver solution) may never be too attractive since the radiation intensity precludes the usage of many optical materials and the nature of the solution is such that light transmission into it might be totally impossible

  12. Recovering actinide values

    Actinide values are recovered from sodium carbonate scrub waste solutions containing these and other values along with organic compounds resulting from the radiolytic and hydrolytic degradation of neutral organophosphorus extractants such as tri-n butyl phosphate (TBP) and dihexyl-N, N-diethyl carbamylmethylene phosphonate (DHDECMP) which have been used in the reprocessing of irradiated nuclear reactor fuels. The scrub waste solution is made acidic with mineral acid, to form a feed solution which is then contacted with a water-immiscible, highly polar organic extractant which selectively extracts the degradation products from the feed solution. The feed solution can then be processed to recover the actinides for storage or recycled back into the high-level waste process stream. The extractant can be recycled after stripping the degradation products with a neutral sodium carbonate solution. (author)

  13. Actinides: why are they important biologically

    The following topics are discussed: actinide elements in energy systems; biological hazards of the actinides; radiation protection standards; and purposes of actinide biological research with regard to toxicity, metabolism, and therapeutic regimens

  14. Photoelectron spectra of actinide compounds

    A brief overview of the application of photoelectron spectroscopy is presented for the study of actinide materials. Phenomenology as well as specific materials are discussed with illustrative examples

  15. TOPICAL REPORT ON ACTINIDE-ONLY BURNUP CREDIT FOR PWR SPENT NUCLEAR FUEL PACKAGES

    A methodology for performing and applying nuclear criticality safety calculations, for PWR spent nuclear fuel (SNF) packages with actinide-only burnup credit, is described. The changes in the U-234, U-235, U-236, U-238, Pu-238, Pu-239, Pu-240, Pu-241, Pu-242, and Am-241 concentration with burnup are used in burnup credit criticality analyses. No credit for fission product neutron absorbers is taken. The methodology consists of five major steps. (1) Validate a computer code system to calculate isotopic concentrations of SNF created during burnup in the reactor core and subsequent decay. A set of chemical assay benchmarks is presented for this purpose as well as a method for assessing the calculational bias and uncertainty, and conservative correction factors for each isotope. (2) Validate a computer code system to predict the subcritical multiplication factor, keff, of a spent nuclear fuel package. Fifty-seven UO2, UO2/Gd2O3, and UO2/PuO2 critical experiments have been selected to cover anticipated conditions of SNF. The method uses an upper safety limit on keff (which can be a function of the trending parameters) such that the biased keff, when increased for the uncertainty is less than 0.95. (3) Establish bounding conditions for the isotopic concentration and criticality calculations. Three bounding axial profiles have been established to assure the ''end effect'' is accounted for conservatively. (4) Use the validated codes and bounding conditions to generate package loading criteria (burnup credit loading curves). Burnup credit loading curves show the minimum burnup required for a given initial enrichment. The utility burnup record is compared to this requirement after the utility accounts for the uncertainty in its record. Separate curves may be generated for each assembly design, various minimum cooling times and burnable absorber histories. (5) Verify that SNF assemblies meet the package loading criteria and confirm proper assembly selection prior to loading

  16. Combined exposure of F344 rats to beryllium metal and plutonium-239 dioxide

    Finch, G.L.; Carlton, W.W.; Rebar, A.H. [Purdue Univ., Lafayette, IN (United States)] [and others

    1995-12-01

    Nuclear weapons industry workers have the potential for inhalation exposures to plutonium (Pu) and other agents, such as beryllium (Be) metal. The purpose of this ongoing study is to investigate potential interactions between Pu and Be in the production of lung tumors in rats exposed by inhalation to particles of {sup 239}PuO{sub 2}, Be metal, or these agents in combination. Inhaled Pu deposited in the lung delivers high-linear-energy transfer, alpha-particle radiation and is known to induce pulmonary cancer in laboratory animals. Although the epidemiological evidence implicating Be in the induction of human lung cancer is weak and controversial, various studies in laboratory animals have demonstrated the pulmonary carcinogenicity of Be. As a result, Be is classified as a suspect human carcinogen in the United STates and as a demonstrated human carcinogen by the International Agency for Research on Cancer. This study is in progress.

  17. Neutron interrogation of actinides with a 17 MeV electron accelerator and first results from photon and neutron interrogation non-simultaneous measurements combination

    Sari, A., E-mail: adrien.sari@cea.fr [CEA, LIST, Laboratoire Capteurs et Architectures Electroniques, 91191 Gif-sur-Yvette Cedex (France); Carrel, F.; Lainé, F. [CEA, LIST, Laboratoire Capteurs et Architectures Electroniques, 91191 Gif-sur-Yvette Cedex (France); Lyoussi, A. [CEA, DEN, 13108 Saint-Paul-Lez-Durance Cedex (France)

    2013-10-01

    In this article, we demonstrate the feasibility of neutron interrogation using the conversion target of a 17 MeV linear electron accelerator as a neutron generator. Signals from prompt neutrons, delayed neutrons, and delayed gamma-rays, emitted by both uranium and plutonium samples were analyzed. First results from photon and neutron interrogation non-simultaneous measurements combination are also reported in this paper. Feasibility of this technique is shown in the frame of the measurement of uranium enrichment. The latter was carried out by combining detection of prompt neutrons from thermal fission and delayed neutrons from photofission, and by combining delayed gamma-rays from thermal fission and delayed gamma-rays from photofission.

  18. Effectiveness of mixed ligand chelation for the removal of plutonium and americium in the hamster

    DTPA and the combination of DTPA plus salicylic acid or other benzene derivatives which are ortho-di-substituted with functional groups containing one or more oxygen and/or nitrogen atoms as electron donors, were tested for their ability to remove 239Pu and/or 241Am from hamsters. Mixed ligand chelation of these actinides by combination of DTPA and any one of these compounds did not result in an increased efficacy for the removal of actinides, as has been reported elsewhere

  19. Partitioning of the rare earths and actinides between R7T7 nuclear glass alteration products and solution according to disposal conditions

    The alteration of nuclear glass by water is liable to release radionuclides into the environment. Determining the release kinetics of these elements and their aqueous chemical forms are therefore essential steps in establishing the safety of a geological repository site. Leach tests were conducted with a nonradioactive specimen of the French ''R7T7'' light water containment glass spiked with U and Th, and with two R7T7 specimens spiked with 237Np and 239Pu, respectively. The alteration solution compositions were representative of deep groundwater and contained carbonate, sulfate, phosphate, fluorine and chlorine ions. The release of U, Th, Np and Pu, as well as of the rare earths La, Ce and Nd were monitored by ICP mass spectrometry and by α spectrometry. Scanning and transmission electron microscopic examination of the nonradioactive altered glass surfaces was also performed to assess the partitioning balance for the rare earths, U and Th between the glass alteration products and solution. The mobility of these elements depends on two competing mechanisms. The rare earths and thorium are incorporated in the alteration products (gel); the retention process is assumed to involve chemisorption or coprecipitation, enhanced in the gel layer by the presence of phosphate ions in particular. Conversely, the aqueous species in the alteration solutions (mainly anions) form complexes with the actinides and rare earths; this phenomenon is particularly evident with U and Np. The presence of carbonate ions favors this mobility. Plutonium differs from U and Np in that it is adsorbed mainly on colloids formed by glass dissolution, the principal factors governing its chemical evolution in solution. (author). refs., 122 figs., 185 tabs

  20. Optical techniques for actinide research

    In recent years, substantial gains have been made in the development of spectroscopic techniques for electronic properties studies. These techniques have seen relatively small, but growing, application in the field of actinide research. Photoemission spectroscopies, reflectivity and absorption studies, and x-ray techniques will be discussed and illustrative examples of studies on actinide materials will be presented

  1. Sector field inductively coupled plasma mass spectrometry in the elemental and isotopic analysis of lanthanides and actinides

    Plutonium is one element which is indispensable in identifying the source and for estimating the hazardous effects of rad. The isotopic ratios of plutonium (240Pu/239Pu) and its total concentration in environmental samples were also precisely estimated by high resolution inductively coupled plasma mass spectrometry

  2. Managing Inventories of Heavy Actinides

    The Department of Energy (DOE) has stored a limited inventory of heavy actinides contained in irradiated targets, some partially processed, at the Savannah River Site (SRS) and Oak Ridge National Laboratory (ORNL). The 'heavy actinides' of interest include plutonium, americium, and curium isotopes; specifically 242Pu and 244Pu, 243Am, and 244/246/248Cm. No alternate supplies of these heavy actinides and no other capabilities for producing them are currently available. Some of these heavy actinide materials are important for use as feedstock for producing heavy isotopes and elements needed for research and commercial application. The rare isotope 244Pu is valuable for research, environmental safeguards, and nuclear forensics. Because the production of these heavy actinides was made possible only by the enormous investment of time and money associated with defense production efforts, the remaining inventories of these rare nuclear materials are an important part of the legacy of the Nuclear Weapons Program. Significant unique heavy actinide inventories reside in irradiated Mark-18A and Mark-42 targets at SRS and ORNL, with no plans to separate and store the isotopes for future use. Although the costs of preserving these heavy actinide materials would be considerable, for all practical purposes they are irreplaceable. The effort required to reproduce these heavy actinides today would likely cost billions of dollars and encompass a series of irradiation and chemical separation cycles for at least 50 years; thus, reproduction is virtually impossible. DOE has a limited window of opportunity to recover and preserve these heavy actinides before they are disposed of as waste. A path forward is presented to recover and manage these irreplaceable National Asset materials for future use in research, nuclear forensics, and other potential applications.

  3. Analysis of optical properties of actinide dioxides

    Ionic calculations, symmetry considerations, and detailed analysis of reflectivity experiments have been used to identify general features of the band structure of actinide dioxides with a fluorite lattice. The ionic calculations adjust atomic energy levels by the electrostatic energies arising from long range electric fields of the ionic lattice; the labelling of high lying energy bands is determined by symmetry; experimental analysis includes the use of appropriate sum rules. A combination of these considerations enable a tentative band scheme to be constructed. It is suggested that there are filled valence bands (GAMMA15,GAMMA'25) originating in oxygen 2p-states and empty conduction bands (GAMMA1,GAMMA12,GAMMA'25) originating in actinide 7s and 6d states. The mean band gap (Penn gap) is of the order of 14 eV. The actinide f-electron states, which lie approximately 5 eV below the conduction bands, are taken to be localized - at least in UO2. (author)

  4. Partitioning of the rare earths and actinides between R7T7 nuclear glass alteration products and solution according to disposal conditions; Partage des terres rares et des actinides entre solution et produits d`alteration du verre nucleaire type R7T7 en fonction des conditions de stockage

    Menard, O.

    1995-10-25

    The alteration of nuclear glass by water is liable to release radionuclides into the environment. Determining the release kinetics of these elements and their aqueous chemical forms are therefore essential steps in establishing the safety of a geological repository site. Leach tests were conducted with a nonradioactive specimen of the French ``R7T7`` light water containment glass spiked with U and Th, and with two R7T7 specimens spiked with {sup 237}Np and {sup 239}Pu, respectively. The alteration solution compositions were representative of deep groundwater and contained carbonate, sulfate, phosphate, fluorine and chlorine ions. The release of U, Th, Np and Pu, as well as of the rare earths La, Ce and Nd were monitored by ICP mass spectrometry and by {alpha} spectrometry. Scanning and transmission electron microscopic examination of the nonradioactive altered glass surfaces was also performed to assess the partitioning balance for the rare earths, U and Th between the glass alteration products and solution. The mobility of these elements depends on two competing mechanisms. The rare earths and thorium are incorporated in the alteration products (gel); the retention process is assumed to involve chemisorption or coprecipitation, enhanced in the gel layer by the presence of phosphate ions in particular. Conversely, the aqueous species in the alteration solutions (mainly anions) form complexes with the actinides and rare earths; this phenomenon is particularly evident with U and Np. The presence of carbonate ions favors this mobility. Plutonium differs from U and Np in that it is adsorbed mainly on colloids formed by glass dissolution, the principal factors governing its chemical evolution in solution. (author). refs., 122 figs., 185 tabs.

  5. Concentration of actinides in the food chain

    Considerable concern is now being expressed over the discharge of actinides into the environment. This report presents a brief review of the chemistry of the actinides and examines the evidence for interaction of the actinides with some naturally-occurring chelating agents and other factors which might stimulate actinide concentration in the food chain of man. This report also reviews the evidence for concentration of actinides in plants and for uptake through the gastrointestinal tract. (author)

  6. Environmental research on actinide elements

    The papers synthesize the results of research sponsored by DOE's Office of Health and Environmental Research on the behavior of transuranic and actinide elements in the environment. Separate abstracts have been prepared for the 21 individual papers

  7. Selective extraction of trivalent actinides from lanthanides with dithiophosphinic acids and tributylphosphate

    A variety of chemical systems have been developed to separate trivalent actinides from lanthanides based on the slightly stronger complexation of the trivalent actinides with ligands that contain soft donor atoms. The greater stability of the actinide complexes in these systems has often been attributed to a slightly greater covalent bonding component for the actinide ions relative to the lanthanide ions. The authors have investigated several synergistic extraction systems that use ligands with a combination of oxygen and sulfur donor atoms that achieve a good group separation of the trivalent actinides and lanthanides. For example, the combination of dicyclohexyldithiophosphinic acid and tributylphosphate has shown separation factors of up to 800 for americium over europium in a single extraction stage. Such systems could find application in advanced partitioning schemes for nuclear waste

  8. Properties of minor actinide nitrides

    The present status of the research on properties of minor actinide nitrides for the development of an advanced nuclear fuel cycle based on nitride fuel and pyrochemical reprocessing is described. Some thermal stabilities of Am-based nitrides such as AmN and (Am, Zr)N were mainly investigated. Stabilization effect of ZrN was cleary confirmed for the vaporization and hydrolytic behaviors. New experimental equipments for measuring thermal properties of minor actinide nitrides were also introduced. (author)

  9. THERMODYNAMICS OF THE ACTINIDES

    Cunningham, Burris B.

    1962-04-01

    Recent work on the thermodynamic properties of the transplutonium elements is presented and discussed in relation to trends in thermodynamic properties of the actinide series. Accurate values are given for room temperature lattice parameters of two crystallographic forms, (facecentred cubic) fcc and dhcp (double-hexagonal closepacked), of americium metal and for the coefficients of thermal expansion between 157 and 878 deg K (dhcp) and 295 to 633 deg K (fcc). The meiting point of the metal, and its magnetic susceptibility between 77 and 823 deg K are reported and the latter compared with theoretical values for the tripositive ion calculated from spectroscopic data. Similar data (crystallography, meiting point and magnetic susceptibility) are given for metallic curium. A value for the heat of formation of americium monoxide is reported in conjunction with crystallographic data on the monoxide and mononitride. A revision is made in the current value for the heat of formation of Am/O/sub 2/ and for the potential of the Am(III)-Am(IV) couple. The crystal structures and lattice parameters are reported for the trichloride, oxychloride and oxides of californium. (auth)

  10. Advanced Aqueous Separation Systems for Actinide Partitioning

    Nash, Ken [Washington State Univ., Pullman, WA (United States); Martin, Leigh [Idaho National Lab. (INL), Idaho Falls, ID (United States); Lumetta, Gregg [Pacific Northwest National Lab. (PNNL), Richland, WA (United States)

    2015-04-02

    necessary for commercial fuel processing supporting transmutation of transplutonium elements. This research project continued basic themes investigated by this research group during the past decade. In the Fuel Cycle Research and Development program at DOE, the current favorite process for accomplishing the separation of trivalent actinides from fission product lanthanides is the TALSPEAK process. TALSPEAK is a solvent extraction method (developed at Oak Ridge National Lab in the 1960s) based on the combination of a cation exchanging extractant (e.g., HDEHP), an actinide-selective aminopolycarboxylate complexing agent (e.g., DTPA), and a carboxylic acid buffer to control pH in the range of 3-4. Considerable effort has been expended in this research group during the past 8 years to elaborate the details of TALSPEAK in the interest of developing improved approaches to the operation of TALSPEAK-like systems. In this project we focused on defining aggregation phenomena in conventional TALSPEAK separations, on supporting the development of Advanced TALSPEAK processes, on profiling the aqueous complexation kinetics of lanthanides in TALSPEAK relevant aqueous media, on the design of new diglycolamide and N-donor extractants, and on characterizing cation-cation complexes of pentavalent actinides.

  11. Late effects of 239Pu injection in adult, weanling, newborn, and fetal rats

    Exposure to Pu decreased the latency of mammary tumor induction in all age groups; incidence varied with the age at injection, and with the dose. There were age-related differences in the effect of plutonium exposure on pituitary tumor incidence, as well as an association between the presence of both mammary and pituitary tumors. Prenatal exposure also increased the incidence of adrenal and pancreatic neoplasms in males

  12. Measurement and analysis of anti ν energy dependence for 233U, 238U, 239Pu

    The energy dependence of the average yield of prompt neutrons per fission (anti ν) for U233, U238 and Pu239 in the incident neutron energy range (Esub(n)) up to 5 MeV has been studied using an electrostatic accelerator. The recommended curves for anti ν (Esub(n)) has been obtained with the help of the polynomial least square method fitting. The resons of deviations from the linear dependence have been analysed

  13. Critical dimensions of systems containing 235U, 239Pu, and 233U: 1986 Revision

    This report is primarily a compilation of critical data obtained from experiments performed in a number of laboratories during the period of 1945 through 1985. It supplements the Nuclear Safety Guide [Report TID-7016 (Rev. 2)] in presenting critical data on which recommendations of the Guide are based. It must be emphasized that this report gives critical data without safety factors, so it is no substitute for the Guide or for the related document, The American National Standard for Nuclear Criticality Safety in Operations with Fissionable Materials Outside Reactors. Critical measurements with materials of interest in desired configurations yield information of greatest usefulness and accuracy. Where it is not feasible to obtain the desired critical data, for example, as a result of safety restrictions, subcritical data may be directly applicable, and in some cases may be extrapolated to approximate critical conditions. Critical conditions also may be approximated from the distribution of neutrons introduced into a subcritical assembly. These ''exponential experiments'' may be the only alternative where the quantity of material required is too great for a critical experiment. Calculated extensions of experimental data are included to show the nature of trends, not to substitute for results of experiments. They should be used with caution. A fundamental aim of this document is to illustrate relationships among critical data. The compilation and correlation of data for this purpose, from many measurements in a number of laboratories, require a certain amount of normalization or reduction to common terms. Frequently, for example, the effects of variations in geometry or density must be removed to show trends in data. The manner in which these alterations may be made is discussed in the early section Relations for Conversion to Standard Conditions. 195 refs

  14. Evaluation of Cross-Sections Uncertainties using Physical Constraints 238U, 239Pu and others..

    This presentation reports on nuclear data activities at CEA Cadarache, e.g. marginalization techniques to account for systematic uncertainties, use of Lagrange multipliers to impose simultaneous consistency constraints on several models, assimilation of integral data during the evaluation process, adjustment of nuclear reaction model parameters, evaluation of covariance matrices, etc. The CEA activities cover both differential and integral data and the possible synergies between SG39 and SG40-CIELO are highlighted. These two new subgroups have the potential to link evaluation and integral experiments beyond the traditional validation issues

  15. Characterization of peripheral-blood lymphocytes in lymphocytopenic dogs exposed to 239PuO2

    Mitogen stimulation assays of canine peripheral-blood lymphocytes in whole-blood and density-gradient-isolated lymphocyte cultures showed that a functional decrease had occurred in these lymphocyte populations from plutonium-exposed dogs, suggesting an alteration in immunocompetence

  16. Quantative autoradiography of inhaled 239PuO2 in the lung

    PuO2 particles behaved similarly in the lungs of rat and hamster. The relative concentrations of PuO2 up to 1-yr postexposure were 1.0 for lung parenchyma, 1.3 for subpleural areas, 0.5 for peribronchiolar regions and 0.2 for perivascular regions in the lungs

  17. Subcellular distribution of 239Pu in the liver of rat, mouse, Syrian and Chinese hamster

    An attempt was made to elucidate the biochemical mechanisms responsible for the species differences in the biological half life of plutonium-239 in the liver of rats, mice, Syrian hamsters and Chinese hamsters. Six days after intravenously administered Pu-239, the animals were given Triton i.p. which causes a shift of the density of the lysosomes and thus any lysosomally-associated material can be recognised by a parallel shift. On the tenth day, an MLP fraction was obtained by differential centrifugation of the liver homogenates; the distribution of radioactivity and marker enzymes was then examined after centrifugation of the MLP fraction in a sucrose density gradient. If the parallelism between the shift of Pu-239 and acid phosphatase is taken as a measure for the extent of lysosomal binding, there is clear evidence for association with these organelles for rats and mice, the species with rapid Pu elimination; however these organelles appear to become less important in the species with longer Pu retention, Syrian and especially Chinese hamster. (U.K.)

  18. Oncogene expression in primary lung tumors in dogs that inhaled 239PuO2

    Ten radiation-induced and three spontaneous lung tumors were analyzed for aberrant expression of known oncogenes. In 12 of 13 tumors tested, sequences hybridizing to the c-myc oncogene were expressed at levels 1.5 times higher than sequences hybridizing to β-actin. This level of oncogene expression was also observed in 9 of 13 tumors for 1 or more members of the ras family of oncogenes. Seven of thirteen tumors examined express sequences that hybridize with clones of v-ros or c-met. The ros and met clones both code for oncogenes whose normal homologues are transmembrane proteins related to the insulin receptor. (author)

  19. Fission Product Yields from Fission Spectrum n+ 239Pu for ENDF/B-VII.1

    Chadwick, M. B.; Kawano, T.; Barr, D. W.; Mac Innes, M. R.; Kahler, A. C.; Graves, T.; Selby, H.; Burns, C. J.; Inkret, W. C.; Keksis, A. L.; Lestone, J. P.; Sierk, A. J.; Talou, P.

    2010-12-01

    We describe a new cumulated fission product yield (FPY) evaluation for fission spectrum neutrons on plutonium that updates the ENDF/B-VI evaluation by England and Rider, for the forthcoming ENDF/B-VII.1 database release. We focus on FPs that are needed for high accuracy burnup assessments; that is, for inferring the number of fissions in a neutron environment. Los Alamos conducted an experiment in the 1970s in the Bigten fast critical assembly to determine fission product yields as part of the Interlaboratory Reaction Rate (ILRR) collaboration, and this has defined the Laboratory's fission standard to this day. Our evaluation includes use of the LANL-ILRR measurements (not previously available to evaluators) as well as other Laboratory FPY measurements published in the literature, especially the high-accuracy mass spectrometry data from Maeck and others. Because the measurement database for some of the FPs is small — especially for 99Mo — we use a meta-analysis that incorporates insights from other accurately-measured benchmark FP data, using R-value ratio measurements. The meta-analysis supports the FP measurements from the LANL-ILRR experiment. Differences between our new evaluations and ENDF/B-VI are small for some FPs (less than 1-2%-relative for 95Zr, 140Ba, 144Ce), but are larger for 99Mo (4%-relative) and 147Nd (5%-relative, at 1.5 MeV) respectively. We present evidence for an incident neutron energy dependence to the 147Nd fission product yield that accounts for observed differences in the FPY at a few-hundred keV average energy in fast reactors versus measurements made at higher average neutron energies in Los Alamos' fast critical assemblies. Accounting for such FPY neutron energy dependencies is important if one wants to reach a goal of determining the number of fissions to accuracies of 1-2%. An evaluation of the energy-dependence of fission product yields is given for all A values based on systematical trends in the measured data, with a focus on the energy dependence over the fast neutron energy range from 0.2-2 MeV. Based on these trends, we present an evaluation of the FPY data at 0.5 and 2.0 MeV average incident neutron energies. This new set of ENDF/B-VII data will enable users to linearly interpolate between the pooled FPY data at ˜0.5 MeV and our new data at 2 MeV to obtain FPYs at other energies. We intend to release the ENDF/B-VII.1 database in December 2011, and all released data are subject to CSEWG approval. It is possible that the released evaluated data will differ from those presented in this paper; the evaluated date presented here can be referred to as ENDF/B-VII.1 beta 0.

  20. Fission Product Yields from Fission Spectrum n+239Pu for ENDF/B-VII.1

    We describe a new cumulated fission product yield (FPY) evaluation for fission spectrum neutrons on plutonium that updates the ENDF/B-VI evaluation by England and Rider, for the forthcoming ENDF/B-VII.1 database release. We focus on FPs that are needed for high accuracy burnup assessments; that is, for inferring the number of fissions in a neutron environment. Los Alamos conducted an experiment in the 1970s in the Bigten fast critical assembly to determine fission product yields as part of the Interlaboratory Reaction Rate (ILRR) collaboration, and this has defined the Laboratory's fission standard to this day. Our evaluation includes use of the LANL-ILRR measurements (not previously available to evaluators) as well as other Laboratory FPY measurements published in the literature, especially the high-accuracy mass spectrometry data from Maeck and others. Because the measurement database for some of the FPs is small - especially for 99Mo - we use a meta-analysis that incorporates insights from other accurately-measured benchmark FP data, using R-value ratio measurements. The meta-analysis supports the FP measurements from the LANL-ILRR experiment. Differences between our new evaluations and ENDF/B-VI are small for some FPs (less than 1-2%-relative for 95Zr, 140Ba, 144Ce), but are larger for 99Mo (4%-relative) and 147Nd (5%-relative, at 1.5 MeV) respectively. We present evidence for an incident neutron energy dependence to the 147Nd fission product yield that accounts for observed differences in the FPY at a few-hundred keV average energy in fast reactors versus measurements made at higher average neutron energies in Los Alamos' fast critical assemblies. Accounting for such FPY neutron energy dependencies is important if one wants to reach a goal of determining the number of fissions to accuracies of 1-2%. An evaluation of the energy-dependence of fission product yields is given for all A values based on systematical trends in the measured data, with a focus on the energy dependence over the fast neutron energy range from 0.2-2 MeV. Based on these trends, we present an evaluation of the FPY data at 0.5 and 2.0 MeV average incident neutron energies. This new set of ENDF/B-VII data will enable users to linearly interpolate between the pooled FPY data at ∼0.5 MeV and our new data at 2 MeV to obtain FPYs at other energies.

  1. Actinide burning and waste disposal

    Here we review technical and economic features of a new proposal for a synergistic waste-management system involving reprocessing the spent fuel otherwise destined for a U.S. high-level waste repository and transmuting the recovered actinides in a fast reactor. The proposal would require a U.S. fuel reprocessing plant, capable of recovering and recycling all actinides, including neptunium americium, and curium, from LWR spent fuel, at recoveries of 99.9% to 99.999%. The recovered transuranics would fuel the annual introduction of 14 GWe of actinide-burning liquid-metal fast reactors (ALMRs), beginning in the period 2005 to 2012. The new ALMRs would be accompanied by pyrochemical reprocessing facilities to recover and recycle all actinides from discharged ALMR fuel. By the year 2045 all of the LWR spent fuel now destined f a geologic repository would be reprocessed. Costs of constructing and operating these new reprocessing and reactor facilities would be borne by U.S. industry, from the sale of electrical energy produced. The ALMR program expects that ALMRs that burn actinides from LWR spent fuel will be more economical power producers than LWRs as early as 2005 to 2012, so that they can be prudently selected by electric utility companies for new construction of nuclear power plants in that era. Some leaders of DOE and its contractors argue that recovering actinides from spent fuel waste and burning them in fast reactors would reduce the life of the remaining waste to about 200-300 years, instead of 00,000 years. The waste could then be stored above ground until it dies out. Some argue that no geologic repositories would be needed. The current view expressed within the ALMR program is that actinide recycle technology would not replace the need for a geologic repository, but that removing actinides from the waste for even the first repository would simplify design and licensing of that repository. A second geologic repository would not be needed. Waste now planned

  2. Kinetics of actinide complexation reactions

    Though the literature records extensive compilations of the thermodynamics of actinide complexation reactions, the kinetics of complex formation and dissociation reactions of actinide ions in aqueous solutions have not been extensively investigated. In light of the central role played by such reactions in actinide process and environmental chemistry, this situation is somewhat surprising. The authors report herein a summary of what is known about actinide complexation kinetics. The systems include actinide ions in the four principal oxidation states (III, IV, V, and VI) and complex formation and dissociation rates with both simple and complex ligands. Most of the work reported was conducted in acidic media, but a few address reactions in neutral and alkaline solutions. Complex formation reactions tend in general to be rapid, accessible only to rapid-scan and equilibrium perturbation techniques. Complex dissociation reactions exhibit a wider range of rates and are generally more accessible using standard analytical methods. Literature results are described and correlated with the known properties of the individual ions

  3. 33rd Actinide Separations Conference

    McDonald, L M; Wilk, P A

    2009-05-04

    Welcome to the 33rd Actinide Separations Conference hosted this year by the Lawrence Livermore National Laboratory. This annual conference is centered on the idea of networking and communication with scientists from throughout the United States, Britain, France and Japan who have expertise in nuclear material processing. This conference forum provides an excellent opportunity for bringing together experts in the fields of chemistry, nuclear and chemical engineering, and actinide processing to present and discuss experiences, research results, testing and application of actinide separation processes. The exchange of information that will take place between you, and other subject matter experts from around the nation and across the international boundaries, is a critical tool to assist in solving both national and international problems associated with the processing of nuclear materials used for both defense and energy purposes, as well as for the safe disposition of excess nuclear material. Granlibakken is a dedicated conference facility and training campus that is set up to provide the venue that supports communication between scientists and engineers attending the 33rd Actinide Separations Conference. We believe that you will find that Granlibakken and the Lake Tahoe views provide an atmosphere that is stimulating for fruitful discussions between participants from both government and private industry. We thank the Lawrence Livermore National Laboratory and the United States Department of Energy for their support of this conference. We especially thank you, the participants and subject matter experts, for your involvement in the 33rd Actinide Separations Conference.

  4. Thermal-hydraulics of actinide burner reactors

    As a part of conceptual study of actinide burner reactors, core thermal-hydraulic analyses were conducted for two types of reactor concepts, namely (1) sodium-cooled actinide alloy fuel reactor, and (2) helium-cooled particle-bed reactor, to examine the feasibility of high power-density cores for efficient transmutation of actinides within the maximum allowable temperature limits of fuel and cladding. In addition, calculations were made on cooling of actinide fuel assembly. (author)

  5. Mathematical modeling of the effects of aerobic and anaerobic chelate biodegradation on actinide speciation

    Biodegradation of natural and anthropogenic chelating agents directly and indirectly affects the speciation, and, hence, the mobility of actinides in subsurface environments. We combined mathematical modeling with laboratory experimentation to investigate the effects of aerobic and anaerobic chelate biodegradation on actinide [Np(IV/V), Pu(IV)] speciation. Under aerobic conditions, nitrilotriacetic acid (NTA) biodegradation rates were strongly influenced by the actinide concentration. Actinide-chelate complexation reduced the relative abundance of available growth substrate in solution and actinide species present or released during chelate degradation were toxic to the organisms. Aerobic bio-utilization of the chelates as electron-donor substrates directly affected actinide speciation by releasing the radionuclides from complexed form into solution, where their fate was controlled by inorganic ligands in the system. Actinide speciation was also indirectly affected by pH changes caused by organic biodegradation. The two concurrent processes of organic biodegradation and actinide aqueous chemistry were accurately linked and described using CCBATCH, a computer model developed at Northwestern University to investigate the dynamics of coupled biological and chemical reactions in mixed waste subsurface environments. CCBATCH was then used to simulate the fate of Np during anaerobic citrate biodegradation. The modeling studies suggested that, under some conditions, chelate degradation can increase Np(IV) solubility due to carbonate complexation in closed aqueous systems

  6. Mathematical modelling of the effects of aerobic and anaerobic chelate biodegradation on actinide speciation

    Biodegradation of natural and anthropogenic chelating agents directly and indirectly affects the speciation, and hence, the mobility of actinides in subsurface environments. We combined mathematical modelling with laboratory experimentation to investigate the effects of aerobic and anaerobic chelate biodegradation on actinide [Np(IV/V), Pu(IV)] speciation. Under aerobic conditions, nitrilotriacetic acid (NTA) biodegradation rates were strongly influenced by the actinide concentration. Actinide-chelate complexation reduced the relative abundance of available growth substrate in solution and actinide species present or released during chelate degradation were toxic to the organisms. Aerobic bioutilization of the chelates as electron-donor substrates directly affected actinide speciation by releasing the radionuclides from complexed form into solution, where their fate was controlled by inorganic ligands in the system. Actinide speciation was also indirectly affected by pH changes caused by organic biodegradation. The two concurrent processes of organic biodegradation and actinide aqueous chemistry were accurately linked and described using CCBATCH, a computer model developed at Northwestern University to investigate the dynamics of coupled biological and chemical reactions in mixed waste subsurface environments. CCBATCH was then used to simulate the fate of Np during anaerobic citrate biodegradation. The modelling studies suggested that, under some conditions, chelate degradation can increase Np(IV) solubility due to carbonate complexation in closed aqueous systems. (orig.)

  7. Actinides and Life's Origins.

    Adam, Zachary

    2007-12-01

    There are growing indications that life began in a radioactive beach environment. A geologic framework for the origin or support of life in a Hadean heavy mineral placer beach has been developed, based on the unique chemical properties of the lower-electronic actinides, which act as nuclear fissile and fertile fuels, radiolytic energy sources, oligomer catalysts, and coordinating ions (along with mineralogically associated lanthanides) for prototypical prebiotic homonuclear and dinuclear metalloenzymes. A four-factor nuclear reactor model was constructed to estimate how much uranium would have been required to initiate a sustainable fission reaction within a placer beach sand 4.3 billion years ago. It was calculated that about 1-8 weight percent of the sand would have to have been uraninite, depending on the weight percent, uranium enrichment, and quantity of neutron poisons present within the remaining placer minerals. Radiolysis experiments were conducted with various solvents with the use of uraniumand thorium-rich minerals (metatorbernite and monazite, respectively) as proxies for radioactive beach sand in contact with different carbon, hydrogen, oxygen, and nitrogen reactants. Radiation bombardment ranged in duration of exposure from 3 weeks to 6 months. Low levels of acetonitrile (estimated to be on the order of parts per billion in concentration) were conclusively identified in 2 setups and tentatively indicated in a 3(rd) by gas chromatography/mass spectrometry. These low levels have been interpreted within the context of a Hadean placer beach prebiotic framework to demonstrate the promise of investigating natural nuclear reactors as power production sites that might have assisted the origins of life on young rocky planets with a sufficiently differentiated crust/mantle structure. Future investigations are recommended to better quantify the complex relationships between energy release, radioactive grain size, fissionability, reactant phase, phosphorus

  8. Simultaneous photon and neutron interrogation using an electron accelerator in order to quantify actinides in encapsulated radioactive wastes

    Measuring out alpha emitters, such as (234,235,236,238U 238,239,240,242,244Pu, 237Np 241,243Am...), in solid radioactive waste, allows us to quantify the alpha activity in a drum and then to classify it. The SIMPHONIE (SIMultaneous PHOton and Neutron Interrogation Experiment) method, developed in this Ph.D. work, combines both the Active Neutron Interrogation and the Induced Photofission Interrogation techniques simultaneously. Its purpose is to quantify in only one measurement, fissile (235U, 239,241Pu...) and fertile (236,238U, 238,240Pu...) elements separately. In the first chapter of this Ph.D. report, we present the principle of the Radioactive Waste Management in France. The second chapter deals with the physical properties of neutron fission and of photofission. These two nuclear reactions are the basis of the SIMPHONIE method. Moreover, one of our purposes was to develop the ELEPHANT (ELEctron PHoton And Neutron Transport) code in view to simulate the electron, photon and neutron transport, including the (γ, n), (γ, 2n) and (γ, f) photonuclear reactions that are not taken into account in the MCNP4 (Monte Carlo N-Particle) code. The simulation codes developed and used in this work are detailed in the third chapter. Finally, the fourth chapter gives the experimental results of SIMPHONIE obtained by using the DGA/ETCA electron linear accelerators located at Arcueil, France. Fissile (235U, 239Pu) and fertile (238U) samples were studied. Furthermore, comparisons between experimental results and calculated data of photoneutron production in tungsten, copper, praseodymium and beryllium by using an electron LINear Accelerator (LINAC) are given. This allows us to evaluate the validity degree of the ELEPHANT code, and finally the feasibility of the SIMPHONIE method. (author)

  9. Actinide cation-cation complexes

    The +5 oxidation state of U, Np, Pu, and Am is a linear dioxo cation (AnO2+) with a formal charge of +1. These cations form complexes with a variety of other cations, including actinide cations. Other oxidation states of actinides do not form these cation-cation complexes with any cation other than AnO2+; therefore, cation-cation complexes indicate something unique about AnO2+ cations compared to actinide cations in general. The first cation-cation complex, NpO2+·UO22+, was reported by Sullivan, Hindman, and Zielen in 1961. Of the four actinides that form AnO2+ species, the cation-cation complexes of NpO2+ have been studied most extensively while the other actinides have not. The only PuO2+ cation-cation complexes that have been studied are with Fe3+ and Cr3+ and neither one has had its equilibrium constant measured. Actinides have small molar absorptivities and cation-cation complexes have small equilibrium constants; therefore, to overcome these obstacles a sensitive technique is required. Spectroscopic techniques are used most often to study cation-cation complexes. Laser-Induced Photacoustic Spectroscopy equilibrium constants for the complexes NpO2+·UO22+, NpO2+·Th4+, PuO2+·UO22+, and PuO2+·Th4+ at an ionic strength of 6 M using LIPAS are 2.4 ± 0.2, 1.8 ± 0.9, 2.2 ± 1.5, and ∼0.8 M-1

  10. Orbital effects in actinide systems

    Actinide magnetism presents a number of important challenges; in particular, the proximity of 5f band to the Fermi energy gives rise to strong interaction with both d and s like conduction electrons, and the extended nature of the 5f electrons means that they can interact with electron orbitals from neighboring atoms. Theory has recently addressed these problems. Often neglected, however, is the overwhelming evidence for large orbital contributions to the magnetic properties of actinides. Some experimental evidence for these effects are presented briefly in this paper. They point, clearly incorrectly, to a very localized picture for the 5f electrons. This dichotomy only enhances the nature of the challenge

  11. Fabrication of actinide mononitride fuel

    Fabrication of actinide mononitride fuel in JAERI is summarized. Actinide mononitride and their solid solutions were fabricated by carbothermic reduction of the oxides in N2 or N2-H2 mixed gas stream. Sintering study was also performed for the preparation of pellets for the property measurements and irradiation tests. The products were characterized to be high-purity mononitride with a single phase of NaCl-type structure. Moreover, fuel pins containing uranium-plutonium mixed nitride pellets were fabricated for the irradiation tests in JMTR and JOYO. (author)

  12. Research on the chemical speciation of actinides

    A demand for the safe and effective management of spent nuclear fuel and radioactive waste generated from nuclear power plant draws increasing attention with the growth of nuclear power industry. The objective of this project is to establish the basis of research on the actinide chemistry by using advanced laser-based highly sensitive spectroscopic systems. Researches on the chemical speciation of actinides are prerequisite for the development of technologies related to nuclear fuel cycles, especially, such as the safe management of high level radioactive wastes and the chemical examination of irradiated nuclear fuels. For supporting these technologies, laser-based spectroscopies have been performed for the chemical speciation of actinide in an aqueous solutions and the quantitative analysis of actinide isotopes in spent nuclear fuels. In this report, results on the following subjects have been summarized. (1) Development of TRLFS technology for chemical speciation of actinides, (2) Development of LIBD technology for measuring solubility of actinides, (3) Chemical speciation of plutonium complexes by using a LWCC system, (4) Development of LIBS technology for the quantitative analysis of actinides, (5) Development of technology for the chemical speciation of actinides by CE, (6) Evaluation on the chemical reactions between actinides and humic substances, (7) Chemical speciation of actinides adsorbed on metal oxides surfaces, (8) Determination of actinide source terms of spent nuclear fuel

  13. Environmental research on actinide elements

    Pinder, J.E. III; Alberts, J.J.; McLeod, K.W.; Schreckhise, R.G. (eds.)

    1987-08-01

    The papers synthesize the results of research sponsored by DOE's Office of Health and Environmental Research on the behavior of transuranic and actinide elements in the environment. Separate abstracts have been prepared for the 21 individual papers. (ACR)

  14. ENDF/B-V actinides

    This document summarizes the contents of the actinides part of the ENDF/B-V nuclear data library released by the US National Nuclear Data Center. This library or selective retrievals of it, are available from the IAEA Nuclear Data Section. (author)

  15. Decorporation of inhaled actinides by chelation therapy

    This article describes recent work in NRPB laboratories that has identified some of the factors influencing the behaviour of plutonium, americium and curium compounds in the body after inhalation, together with a number of experimental approaches that are being developed to optimise their treatment with DTPA. It is concluded that the most effective treatment has yet to be developed, but progress must depend on a better understanding of the factors governing the transport of actinides in the body. It cannot be assumed that because the inhaled material is readily translocated to blood, that treatment regimens with Ca-DTPA based solely on previous understanding of the metabolic fate of soluble actinide complexes will be successful. In fact, depending on the nature of the material involved in the accident, inhalation alone or combined with prolonged infusion of DTPA may be more effective than the periodic intravenous injections of the chelating agent alone. For poorly transportable materials such as insoluble plutonium-239 dioxide, chelation treatment remains essentially ineffective. (U.K.)

  16. Characterization studies of actinide contamination on Johnston Atoll

    This paper presents results that indicates that plutonium and americium contamination of Johnson Atoll soil and sludge from the cleanup plant settling pond is dispersed. The 241Am/239Pu ratio was essentially identical for all analyzed material. Except for one ''hot particle,'' no discrete Pu particles were located in untreated coral soil by SEM even though our sample contained both 241Am and 239Pu activity measurable by gammaray spectrometry. Alpha particle spectrometry analysis of sequentially filtered sludge showed small that activity is associated with particles as 0.4 μm in diameter. Thin section analysis revealed that the ''hot particle'' was a fragment of stainless steel with a layer of oxidized Pu, U, and other metals deposited on the outside. This Pu-containing layer was covered with a layer of coral soil that formed on the oxidized Pu/U phase during the process of weathering on JA. Analyses of all samples except the ''hot particle'' with SEM or TEM coupled with EDS did not reveal the presence of any distinct Pu phases, despite measurable activity in these samples. Together, these findings are consistent with the Pu and Am being highly dispersed throughout the contaminated soil and sludge. Direct evidence for association of Pu with coral was observed in the thin section of the ''hot particle.'' A possible mechanism for the dispersal of contamination is that weathering of fragments from the aborted missile leads to complexation of Pu with calcium carbonate followed by adsorption onto the coral soil surface. This process has not led to measurable fractionation of Am from its Pu parent

  17. Actinides recycling assessment in a thermal reactor

    Highlights: • Actinides recycling is assessed using BWR fuel assemblies. • Four fuel rods are substituted by minor actinides rods in a UO2 and in a MOX fuel assembly. • Performance of standard fuel assemblies and the ones with the substitution is compared. • Reduction of actinides is measured for the fuel assemblies containing minor actinides rods. • Thermal reactors can be used for actinides recycling. - Abstract: Actinides recycling have the potential to reduce the geological repository burden of the high-level radioactive waste that is produced in a nuclear power reactor. The core of a standard light water reactor is composed only by fuel assemblies and there are no specific positions to allocate any actinides blanket, in this assessment it is proposed to replace several fuel rods by actinides blankets inside some of the reactor core fuel assemblies. In the first part of this study, a single uranium standard fuel assembly is modeled and the amount of actinides generated during irradiation is quantified for use it as reference. Later, in the same fuel assembly four rods containing 6 w/o of minor actinides and using depleted uranium as matrix were replaced and depletion was simulated to obtain the net reduction of minor actinides. Other calculations were performed using MOX fuel lattices instead of uranium standard fuel to find out how much reduction is possible to obtain. Results show that a reduction of minor actinides is possible using thermal reactors and a higher reduction is obtained when the minor actinides are embedded in uranium fuel assemblies instead of MOX fuel assemblies

  18. Molecular solids of actinide hexacyanoferrate: Structure and bonding

    The hexacyanometallate family is well known in transition metal chemistry because the remarkable electronic delocalization along the metal-cyano-metal bond can be tuned in order to design systems that undergo a reversible and controlled change of their physical properties. We have been working for few years on the description of the molecular and electronic structure of materials formed with [Fe(CN)6]n- building blocks and actinide ions (An = Th, U, Np, Pu, Am) and have compared these new materials to those obtained with lanthanide cations at oxidation state +III. In order to evaluate the influence of the actinide coordination polyhedron on the three-dimensional molecular structure, both atomic number and formal oxidation state have been varied : oxidation states +III, +IV. EXAFS at both iron K edge and actinide LIII edge is the dedicated structural probe to obtain structural information on these systems. Data at both edges have been combined to obtain a three-dimensional model. In addition, qualitative electronic information has been gathered with two spectroscopic tools : UV-Near IR spectrophotometry and low energy XANES data that can probe each atom of the structural unit : Fe, C, N and An. Coupling these spectroscopic tools to theoretical calculations will lead in the future to a better description of bonding in these molecular solids. Of primary interest is the actinide cation ability to form ionic - covalent bonding as 5f orbitals are being filled by modification of oxidation state and/or atomic number.

  19. Synergistic extraction of actinides : Part II. Tetra-and trivalent actinides

    A detailed discussion on the synergistic solvent extraction behaviour of tetra- and trivalent actinide ions is presented. Structural aspects of the natural donor adducts of the tetravalent actinide ion chelates involved in synergism are also discussed. (author)

  20. Spin Hamiltonians for actinide ions

    The breakdown of Russel Saunders coupling for correlated f-levels of actinide ions is due to both spin orbit coupling and the crystalline electric field (CEF). Experiments on curium, an S-state ion in the metal for which the CEF is weak indicate a g-factor close to the Russel-Saunders value. Spin-orbit coupling is therefore too weak to produce jj coupling. This suggests a model for magnetic actinide ions in which the CEF ground multiplet is well separated from higher levels, completely determining thermodynamic magnetic properties. On this basis simplified spin Hamiltonians are derived for GAMMA1-GAMMA5 ground states in order to interpret thermodynamic measurements and ordering phenomena. (author)

  1. Actinide chemistry in ionic liquids.

    Takao, Koichiro; Bell, Thomas James; Ikeda, Yasuhisa

    2013-04-01

    This Forum Article provides an overview of the reported studies on the actinide chemistry in ionic liquids (ILs) with a particular focus on several fundamental chemical aspects: (i) complex formation, (ii) electrochemistry, and (iii) extraction behavior. The majority of investigations have been dedicated to uranium, especially for the 6+ oxidation state (UO2(2+)), because the chemistry of uranium in ordinary solvents has been well investigated and uranium is the most abundant element in the actual nuclear fuel cycles. Other actinides such as thorium, neptunium, plutonium, americium, and curiumm, although less studied, are also of importance in fully understanding the nuclear fuel engineering process and the safe geological disposal of radioactive wastes. PMID:22873132

  2. Actinide recovery techniques utilizing electromechanical processes

    Under certain conditions, the separation of actinides using electromechanical techniques may be an effective means of residue processing. The separation of granular mixtures of actinides and other materials discussed in this report is based on appreciable differences in the magnetic and electrical properties of the actinide elements. In addition, the high density of actinides, particularly uranium and plutonium, may render a simultaneous separation based on mutually complementary parameters. Both high intensity magnetic separation and electrostatic separation have been investigated for the concentration of an actinide waste stream. Waste stream constituents include an actinide metal alloy and broken quartz shards. The investigation of these techniques is in support of the Integral Fast Reactor (IFR) concept currently being developed at Argonne National Laboratory under the auspices of the Department of Energy

  3. Actinide Waste Forms and Radiation Effects

    Ewing, R. C.; Weber, W. J.

    Over the past few decades, many studies of actinides in glasses and ceramics have been conducted that have contributed substantially to the increased understanding of actinide incorporation in solids and radiation effects due to actinide decay. These studies have included fundamental research on actinides in solids and applied research and development related to the immobilization of the high level wastes (HLW) from commercial nuclear power plants and processing of nuclear weapons materials, environmental restoration in the nuclear weapons complex, and the immobilization of weapons-grade plutonium as a result of disarmament activities. Thus, the immobilization of actinides has become a pressing issue for the twenty-first century (Ewing, 1999), and plutonium immobilization, in particular, has received considerable attention in the USA (Muller et al., 2002; Muller and Weber, 2001). The investigation of actinides and

  4. Measurement of standard potentials of actinides (U,Np,Pu,Am) in LiCl-KCl eutectic salt and separation of actinides from rare earths by electrorefining

    Pyrochemical separation of actinides from rare earths in LiCl-KCl eutectic-liquid metal systems has been studied. The electromotive forces of galvanic cells of the form, Ag vertical stroke Ag(I), LiCl-KCl parallel actinide(III), LiCl-KCl vertical stroke actinide, were measured and standard potentials were determined for uranium, neptunium and plutonium to be -1.283 V, -1.484 V and -1.593 V (at 450 C vs. Ag/AgCl (1wt%-AgCl)), respectively. A typical cyclic voltammogram of americium chloride has two cathodic peaks, which suggests reduction Am(III)→Am(II) occurs followed by reduction of Am(II) to americium metal. Standard potential of Am(II)/Am(0) was estimated to be -1.642 V. Electrorefining experiments to separate actinides (U, Np, Pu and Am) from rare earths (Y, La, Ce, Nd and Gd) in LiCl-KCl eutectic salt were carried out. It was shown that the actinide metals were recovered on the cathodes and that americium was the most difficult to separate from rare earths. The actinide separation will be achieved by means of the combination of electrorefining with multistage extraction. (orig.)

  5. Distribution of neptunium and plutonium in New Mexico lichen samples (Usnea arizonica) contaminated by atmospheric fallout

    The concentrations of 237Np, 239Pu and 240Pu were determined in lichen samples (Usnea arizonica) that were collected from ten locations in New Mexico between 2011 and 2013 using isotope dilution inductively-coupled plasma mass spectrometry (ID-ICP-MS). The observed isotopic ratios for 237Np/239Pu and 240Pu/239Pu indicate trace contamination from global and regional fallout (e.g. Trinity test and atmospheric testing at the Nevada Test Site). The fact that actinide contamination is detected in recent lichen collections suggests continuous re-suspension of fallout radionuclides even 50 years after ratification of the Limited Test Ban Treaty. (author)

  6. XAFS study on electronic structure analysis of actinide complexes

    Structures and electronic states of actinide complexes in solution were reviewed in relation to chemical separation required from nuclear fuel processing and nuclear waste disposal. Actinide complexes formed from organic compounds were studied in respect of solvent extraction in a wet method for nuclear fuel reprocessing. Particular attention was paid to the experiments by XAFS using synchrotron radiation. A Fourier transformation form of EXAFS oscillation was shown for a U(VI)-amide complex in dodecane solution. The structure radial function of Uranium-DH2EHA (N, N-dihyxyl-2-ethylhexanamice) in solution was determined by EXAFS, and the contributions of two oxygens in an axial direction and of ligand atoms coordinated in an equatorial plane, which combined with a central uranium ion, were indicated in the structure radial function. Structure parameters for U-, Np- and Pu-TBP(Tributyl phosphate) complexes, and for U-amide complexes were listed in Table. A theory predicted a systematic increase of covalency for complexes formed from UO22+∼PO22+ and TEP with an increase of atomic number of actinides, but for U-amide and U∼Pu-TBP complexes the effect of covalency was not reflected in interatomic distances. Some correlations between distribution ratios and different substituents were found in the interatomic distances between uranium and ligand atoms-Distribution ratios of U(VI) depended on interatomic distances between actinide atoms and oxygen ions in carbonyl and in nitric acid. Similarity of chemical bonds in all U-amide complexes except DH2EHA was indicated from XANES spectra of U LIII absorption edge. Three structures for Np(V)-carbon complexes were shown in a ball-and-stick model, and the structure parameters determined by EXAFS were also summarized in Table. Separation of trivalent actinide from the same valent lanthanide was described in connection with soft donors, which have donors such as sulfur and nitrogen atoms. (Kazumata, Y.)

  7. PWRs potentialities for minor actinides burning

    In the frame of the SPIN program at CEA, the impacts of the minor actinides (MA) incineration in PWRs are analysed. The aim is to reduce the mass, the potential radiotoxicity level. The recycling of all actinide elements is evaluated in a PWR nuclear yard. A sensitivity study is done to evaluate the incineration for each minor actinide element. This gives the most efficient way of incineration for each MA elements in a PWR and helps to design a PWR burner. This burner is disposed in a PWR nuclear system in which the actinides are recycled until equilibrium. (author)

  8. Research on the chemical speciation of actinides

    A demand for the safe and effective management of spent nuclear fuel and radioactive waste generated from nuclear power plant draws increasing attention with the growth of nuclear power industry. The objective of this project is to establish the basis of research on the actinide chemistry by using highly sensitive and advanced laser-based spectroscopic systems. Researches on the chemical speciation of actinides are prerequisite for the development of technologies related to nuclear fuel cycles, especially, such as the safe management of high level radioactive wastes and the chemical examination of irradiated nuclear fuels. For supporting these technologies, laser-based spectroscopies have been applied for the chemical speciation of actinide in aqueous solutions and the quantitative analysis of actinide isotopes in spent nuclear fuels. In this report, results on the following subjects have been summarized. Development of TRLFS technology for the chemical speciation of actinides, Development of laser-induced photo-acoustic spectroscopy (LPAS) system, Application of LIBD technology to investigate dynamic behaviors of actinides dissolution reactions, Development of nanoparticle analysis technology in groundwater using LIBD, Chemical speciation of plutonium complexes by using a LWCC system, Development of LIBS technology for the quantitative analysis of actinides, Evaluation on the chemical reactions between actinides and humic substances, Spectroscopic speciation of uranium-ligand complexes in aqueous solution, Chemical speciation of actinides adsorbed on metal oxides surfaces

  9. Chemistry of actinides and fission products

    This task is concerned primarily with the fundamental chemistry of the actinide and fission product elements. Special efforts are made to develop research programs in collaboration with researchers at universities and in industry who have need of national laboratory facilities. Specific areas currently under investigation include: (1) spectroscopy and photochemistry of actinides in low-temperature matrices; (2) small-angle scattering studies of hydrous actinide and fission product polymers in aqueous and nonaqueous solvents; (3) kinetic and thermodynamic studies of complexation reactions in aqueous and nonaqueous solutions; and (4) the development of inorganic ion exchange materials for actinide and lanthanide separations. Recent results from work in these areas are summarized here

  10. Long-term plant availability of actinides

    Environmental releases of actinide elements raise issues about which data are very limited. Quantitative information is required to assess the long-term behavior of actinides and their potential hazards resulting from the transport through food chains leading to man. Of special interest is the effect of time on the changes in the availability of actinide elements for uptake by plants from soil. This study provides valuable information on the effects of weathering and aging on the uptake of actinides from soil by range and crop plants grown under realistic field conditions

  11. Chemical and Ceramic Methods Toward Safe Storage of Actinides

    A very important, extremely-long-term, use for monazite as a radwaste encapsulant has been proposed. The use of ceramic La-monazite for sequestering actinides (isolating them from the environment), especially plutonium and some other radioactive elements (e.g., fission-product rare earths), had been especially championed by Lynn Boatner of ORNL. Monazite may be used alone or, copying its compatibility with many other minerals in nature, may be used in diverse composite combinations

  12. Chemical and Ceramic Methods Toward Safe Storage of Actinides

    P.E.D. Morgan; R.M. Housley; J.B. Davis; M.L. DeHaan

    2005-08-19

    A very import, extremely-long-term, use for monazite as a radwaste encapsulant has been proposed. THe use of ceramic La-monazite for sequestering actinides (isolating them from the environment), especially plutonium and some other radioactive elements )e.g., fission-product rare earths), had been especially championed by Lynn Boatner of ORNL. Monazite may be used alone or, copying its compatibility with many other minerals in nature, may be used in diverse composite combinations.

  13. Calculated Atomic Volumes of the Actinide Metals

    Skriver, H.; Andersen, O. K.; Johansson, B.

    1979-01-01

    The equilibrium atomic volume is calculated for the actinide metals. It is possible to account for the localization of the 5f electrons taking place in americium.......The equilibrium atomic volume is calculated for the actinide metals. It is possible to account for the localization of the 5f electrons taking place in americium....

  14. Environmental chemistry of the actinide elements

    The environmental chemistry of the actinide elements is a new branch of science developing with the application of nuclear energy on a larger and larger scale. Various aspects of the environmental chemistry of the actinide elements are briefly reviewed in this paper, such as its significance in the nuclear waste disposal, its coverage of research fields and possible directions for future study

  15. PIE analysis for minor actinide

    Minor actinide (MA) is generated in nuclear fuel during the operation of power reactor. For fuel design, reactivity decrease due to it should be considered. Out of reactors, MA plays key role to define the property of spent fuel (SF) such as α-radioactivity, neutron emission rate, and criticality of SF. In order to evaluate the calculation codes and libraries for predicting the amount of MA, comparison between calculation results and experimentally obtained data has been conducted. In this report, we will present the status of PIE data of MA taken by post irradiation examinations (PIE) and several calculation results. (author)

  16. Superabsorbing gel for actinide, lanthanide, and fission product decontamination

    Kaminski, Michael D.; Mertz, Carol J.

    2016-06-07

    The present invention provides an aqueous gel composition for removing actinide ions, lanthanide ions, fission product ions, or a combination thereof from a porous surface contaminated therewith. The composition comprises a polymer mixture comprising a gel forming cross-linked polymer and a linear polymer. The linear polymer is present at a concentration that is less than the concentration of the cross-linked polymer. The polymer mixture is at least about 95% hydrated with an aqueous solution comprising about 0.1 to about 3 percent by weight (wt %) of a multi-dentate organic acid chelating agent, and about 0.02 to about 0.6 molar (M) carbonate salt, to form a gel. When applied to a porous surface contaminated with actinide ions, lanthanide ions, and/or other fission product ions, the aqueous gel absorbs contaminating ions from the surface.

  17. Study of lanthanum orthophosphates polymorphism, in view of actinide conditioning

    In order to perform researches on the substitution lanthanide-actinide in a view of actinide conditioning, a preliminary study of the polymorphism of lanthanum orthophosphates has been carried out by different techniques. LaPO4 formed by reaction of lanthanum nitrate with phosphoric acid contains 0.5 mol of water in open channel of the hexagonal structure (rhabdophane-type). The combination of thermogravimetric analysis, differential scanning calorimetry, X-ray diffraction and 31P solid-state nuclear magnetic resonance clearly shows the different steps of the thermal treatment. The zeolitic water evaporates between 180 and 280 deg. C. After heating up to 700 deg. C, a monoclinic structure (monazite-type) is formed by compacting the chains of PO4 tetrahedron alternating with LaO9 polyhedron

  18. Actinides analysis by accelerator mass spectrometry

    At the ANTARES accelerator at ANSTO a new beamline has been commissioned, incorporating new magnetic and electrostatic analysers, to optimise the efficiency for Actinides detection by Accelerator Mass Spectrometry (AMS). The detection of Actinides, particularly the isotopic ratios of uranium and plutonium, provide unique signatures for nuclear safeguards purposes. We are currently engaged in a project to evaluate the application of AMS to the measurement of Actinides in environmental samples for nuclear safeguards. Levels of certain fission products, Actinides and other radioactive species can be used as indicators of undeclared nuclear facilities or activities, either on-going or in the past Other applications of ultra-sensitive detection of Actinides are also under consideration. neutron-attenuation images of a porous reservoir rock

  19. Actinide co-conversion by internal gelation

    Suitable microstructures and homogenous microspheres of actinide compounds are of interest for future nuclear fuel or transmutation target concepts to prevent the generation and dispersal of actinide powder. Sol-gel routes are being investigated as one of the possible solutions for producing these compounds. Preliminary work is described involving internal gelation to synthesize mixed compounds including minor actinides, particularly mixed actinide or mixed actinide-inert element compounds. A parameter study is discussed to highlight the importance of the initial broth composition for obtaining gel microspheres without major defects (cracks, craters, etc.). In particular, conditions are defined to produce gel beads from Zr(IV)/Y(III)/Ce(III) or Zr(IV)/An(III) systems. After gelation, the heat treatment of these microspheres is described for the purpose of better understanding the formation of cracks after calcination and verifying the effective synthesis of an oxide solid-solution. (authors)

  20. Actinide ion sensor for pyroprocess monitoring

    Jue, Jan-fong; Li, Shelly X.

    2014-06-03

    An apparatus for real-time, in-situ monitoring of actinide ion concentrations which comprises a working electrode, a reference electrode, a container, a working electrolyte, a separator, a reference electrolyte, and a voltmeter. The container holds the working electrolyte. The voltmeter is electrically connected to the working electrode and the reference electrode and measures the voltage between those electrodes. The working electrode contacts the working electrolyte. The working electrolyte comprises an actinide ion of interest. The reference electrode contacts the reference electrolyte. The reference electrolyte is separated from the working electrolyte by the separator. The separator contacts both the working electrolyte and the reference electrolyte. The separator is ionically conductive to the actinide ion of interest. The reference electrolyte comprises a known concentration of the actinide ion of interest. The separator comprises a beta double prime alumina exchanged with the actinide ion of interest.

  1. Enhancing the actinide sciences in Europe through hot laboratories networking and pooling: from ACTINET to TALISMAN

    Since 2004, Europe supports the strengthening of the European actinides sciences scientific community through the funding of dedicated networks: (i) from 2004 to 2008, the ACTINET6 network of excellence (6. Framework Programme) gathered major laboratories involved in nuclear research and a wide range of academic research organisations and universities with the specific aims of funding and implementing joint research projects to be performed within the network of pooled facilities; (ii) from 2009 to 2013, the ACTINET-I3 integrated infrastructure initiative (I3) supports the cost of access of any academics in the pooled EU hot laboratories. In this continuation, TALISMAN (Trans-national Access to Large Infrastructures for a Safe Management of Actinides) gathers now the main European hot laboratories in actinides sciences in order to promote their opening to academics and universities and strengthen the EU-skills in actinides sciences. Furthermore, a specific focus is set on the development of advanced cutting-edge experimental and spectroscopic capabilities, the combination of state-of-the art experimental with theoretical first-principle methods on a quantum mechanical level and to benefit from the synergy between the different scientific and technical communities. ACTINET-I3 and TALISMAN attach a great importance and promote the Education and Training of the young generation of actinides scientists in the Trans-national access but also by organizing Schools (general Summer Schools or Theoretical User Lab Schools) or by granting students to attend International Conference on actinide sciences. (authors)

  2. The ALMR actinide burning system

    The advanced liquid-metal reactor (ALMR) actinide burning system is being developed under the sponsorship of the US Department of Energy to bring its unique capabilities to fruition for deployment in the early 21st century. The system consists of four major parts: the reactor plant, the metal fuel and its recycle, the processing of light water reactor (LWR) spent fuel to extract the actinides, and the development of a residual waste package. This paper addresses the status and outlook for each of these four major elements. The ALMR is being developed by an industrial group under the leadership of General Electric (GE) in a cost-sharing arrangement with the US Department of Energy. This effort is nearing completion of the advanced conceptual design phase and will enter the preliminary design phase in 1994. The innovative modular reactor design stresses simplicity, economics, reliability, and availability. The design has evolved from GE's PRISM design initiative and has progressed to the final stages of a prelicensing review by the US Nuclear Regulatory Commission (NRC); a safety evaluation report is expected by the end of 1993. All the major issues identified during this review process have been technically resolved. The next design phases will focus on implementation of the basic safety philosophy of passive shutdown to a safe, stable condition, even without scram, and passive decay heat removal. Economic projections to date show that it will be competitive with non- nuclear and advanced LWR nuclear alternatives

  3. Sensitivity analysis for actinide production and depletion in fast reactors

    In sensitivity analysis of the actinide production and depletion in fast reactors, a mathematical method of calculating sensitivity coefficients is improved and simplified by combining the time-dependent generalized perturbation technique with the eigenvalue method. Numerical calculations show that the eigenvalue method is well applicable in solving the nuclide chain equation and its adjoint equation and the cylic chains in the decay scheme of the actinides can be interpreted by means of complex eigenvalues. The sensitivity coefficients of actinide production and depletion in a 1000 MWe fast reactor are strongly dependent on the type of Pu fuel used, i.e. Pu fuel from BWR or Pu fuel from the blanket of FBR. The sensitivity coefficients due to variations of capture cross sections, σsub(n,2n) of 238U, lambda sub(β) of 241Pu and lambda sub(α) of 242Cm are especially large. Sensitivity analyses for the 1000 MWe fast reactors show that higher priorily should be given to decay constants of 241Pu and 242Cm, capture cross sections of 237Np, 241Am, 243Am and 242Pu, and fission cross sections of 237Np, 242Pu, 241Am and sup(242m)Am. (author)

  4. Molecular cluster theory of chemical bonding in actinide oxide

    The electronic structure of actinide monoxides AcO and dioxides AcO2, where Ac = Th, U, Np, Pu, Am, Cm and Bk has been studied by molecular cluster methods based on the first-principles one-electron local density theory. Molecular orbitals for nearest neighbor clusters AcO10-6 and AcO12-8 representative of monoxide and dioxide lattices were obtained using non-relativistic spin-restricted and spin-polarized Hartree-Fock-Slater models for the entire series. Fully relativistic Dirac-Slater calculations were performed for ThO, UO and NpO in order to explore magnitude of spin-orbit splittings and level shifts in valence structure. Self-consistent iterations were carried out for NpO, in which the NpO6 cluster was embedded in the molecular field of the solid. Finally, a ''moment polarized'' model which combines both spin-polarization and relativistic effects in a consistent fashion was applied to the NpO system. Covalent mixing of oxygen 2p and Ac 5f orbitals was found to increase rapidly across the actinide series; metal s,p,d covalency was found to be nearly constant. Mulliken atomic population analysis of cluster eigenvectors shows that free-ion crystal field models are unreliable, except for the light actinides. X-ray photoelectron line shapes have been calculated and are found to compare rather well with experimental data on the dioxides

  5. Experimental studies of actinides in molten salts

    Reavis, J.G.

    1985-06-01

    This review stresses techniques used in studies of molten salts containing multigram amounts of actinides exhibiting intense alpha activity but little or no penetrating gamma radiation. The preponderance of studies have used halides because oxygen-containing actinide compounds (other than oxides) are generally unstable at high temperatures. Topics discussed here include special enclosures, materials problems, preparation and purification of actinide elements and compounds, and measurements of various properties of the molten volts. Property measurements discussed are phase relationships, vapor pressure, density, viscosity, absorption spectra, electromotive force, and conductance. 188 refs., 17 figs., 6 tabs.

  6. Electronic structure and magnetic properties of actinides

    The study of the actinide series shows the change between transition metal behavior and lanthanide behavior, between constant weak paramagnetism for thorium and strong Curie-Weiss paramagnetism for curium. Curium is shown to be the first metal of the actinide series to be magnetically ordered, its Neel temperature being 52K. The magnetic properties of the actinides depending on all the peripheral electrons, their electronic structure was studied and an attempt was made to determine it by means of a phenomenological model. Attempts were also made to interrelate the different physical properties which depend on the outer electronic structure

  7. Actinide chemistry in the far field

    The environmental chemistry of the actinides is complicated due both to the extensive redox and coordination chemistry of the elements and also to the complexity of the reactive phases encountered in natural environments. In the far field, interactions with reactive surfaces, coatings and colloidal particles will play a crucial role in controlling actinide mobility. By virtue of both their abundance and reactivity; clays and other layer aluminosilicate minerals, hydrous oxides and organic matter (humic substances) are all identified as having the potential to react with actinide ions and some possible modes of interaction are described, together with experimental evidence for their occurrence. (author)

  8. Experimental studies of actinides in molten salts

    This review stresses techniques used in studies of molten salts containing multigram amounts of actinides exhibiting intense alpha activity but little or no penetrating gamma radiation. The preponderance of studies have used halides because oxygen-containing actinide compounds (other than oxides) are generally unstable at high temperatures. Topics discussed here include special enclosures, materials problems, preparation and purification of actinide elements and compounds, and measurements of various properties of the molten volts. Property measurements discussed are phase relationships, vapor pressure, density, viscosity, absorption spectra, electromotive force, and conductance. 188 refs., 17 figs., 6 tabs

  9. Spin and orbital moments in actinide compounds

    Lebech, B.; Wulff, M.; Lander, G.H.

    1991-01-01

    -electron band-structure calculations, is that the orbital moments of the actinide 5f electrons are considerably reduced from the values anticipated by a simple application of Hund's rules. To test these ideas, and thus to obtain a measure of the hybridization, we have performed a series of neutron scattering...... experiments designed to determine the magnetic moments at the actinide and transition-metal sublattice sites in compounds such as UFe2, NpCo2, and PuFe2 and to separate the spin and orbital components at the actinide sites. The results show, indeed, that the ratio of the orbital to spin moment is reduced as...

  10. Endohedral Fullerenes with Actinide-Actinide Bonds: Unwilling Bonding in U2@C80

    Foroutan-Nejad, C.; Patzschke, M.; Straka, Michal

    Opole: -, 2014. [MMNB 2014. Polish-Taiwanese Conference. From Molecular Modeling to Nano- and Biotechnology . 04.09.2014-06.09.2014, Opole] R&D Projects: GA ČR(CZ) GA14-03564S Grant ostatní: European Social Fund(XE) CZ.1.07/2.3.00/30.009 Institutional support: RVO:61388963 Keywords : endohedral actinide fullerene * U-U bonding * actinide-actinide bonding Subject RIV: CF - Physical ; Theoretical Chemistry

  11. Simultaneous photon and neutron interrogation using an electron accelerator in order to quantify actinides in encapsulated radioactive wastes; Double interrogation simultanee neutrons et photons utilisant un accelerateur d'electrons pour la caracterisation separee des actinides dans les dechets radioactifs enrobes

    Jallu, F

    1999-09-24

    Measuring out alpha emitters, such as ({sup 234,235,236,238}U {sup 238,239,240,242,}2{sup 44P}u, {sup 237}Np {sup 241,243}Am...), in solid radioactive waste, allows us to quantify the alpha activity in a drum and then to classify it. The SIMPHONIE (SIMultaneous PHOton and Neutron Interrogation Experiment) method, developed in this Ph.D. work, combines both the Active Neutron Interrogation and the Induced Photofission Interrogation techniques simultaneously. Its purpose is to quantify in only one measurement, fissile ({sup 235}U, {sup 239,241}Pu...) and fertile ({sup 236,238}U, {sup 238,240}Pu...) elements separately. In the first chapter of this Ph.D. report, we present the principle of the Radioactive Waste Management in France. The second chapter deals with the physical properties of neutron fission and of photofission. These two nuclear reactions are the basis of the SIMPHONIE method. Moreover, one of our purposes was to develop the ELEPHANT (ELEctron PHoton And Neutron Transport) code in view to simulate the electron, photon and neutron transport, including the ({gamma}, n), ({gamma}, 2n) and ({gamma}, f) photonuclear reactions that are not taken into account in the MCNP4 (Monte Carlo N-Particle) code. The simulation codes developed and used in this work are detailed in the third chapter. Finally, the fourth chapter gives the experimental results of SIMPHONIE obtained by using the DGA/ETCA electron linear accelerators located at Arcueil, France. Fissile ({sup 235}U, {sup 239}Pu) and fertile ({sup 238}U) samples were studied. Furthermore, comparisons between experimental results and calculated data of photoneutron production in tungsten, copper, praseodymium and beryllium by using an electron LINear Accelerator (LINAC) are given. This allows us to evaluate the validity degree of the ELEPHANT code, and finally the feasibility of the SIMPHONIE method. (author)

  12. PF-4 actinide disposition strategy

    The dwindling amount of Security Category I processing and storage space across the DOE Complex has driven the need for more effective storage of nuclear materials at LANL's Plutonium Facility's (PF-4's) vault. An effort was begun in 2009 to create a strategy, a roadmap, to identify all accountable nuclear material and determine their disposition paths, the PF-4 Actinide Disposition Strategy (PADS). Approximately seventy bins of nuclear materials with similar characteristics - in terms of isotope, chemical form, impurities, disposition location, etc. - were established in a database. The ultimate disposition paths include the material to remain at LANL, disposition to other DOE sites, and disposition to waste. If all the actions described in the document were taken, over half of the containers currently in the PF-4 vault would been eliminated. The actual amount of projected vault space will depend on budget and competing mission requirements, however, clearly a significant portion of the current LANL inventory can be either dispositioned or consolidated.

  13. Actinide recovery from pyrochemical residues

    We demonstrated a new process for recovering plutonium and americium from pyrochemical waste. The method is based on chloride solution anion exchange at low acidity, or acidity that eliminates corrosive HCl fumes. Developmental experiments of the process flow chart concentrated on molten salt extraction (MSE) residues and gave >95% plutonium and >90% americium recovery. The recovered plutonium contained 62- from high-chloride low-acid solution. Americium and other metals are washed from the ion exchange column with lN HNO3-4.8M NaCl. After elution, plutonium is recovered by hydroxide precipitation, and americium is recovered by NaHCO3 precipitation. All filtrates from the process can be discardable as low-level contaminated waste. Production-scale experiments are in progress for MSE residues. Flow charts for actinide recovery from electro-refining and direct oxide reduction residues are presented and discussed

  14. Subsurface interactions of actinide species and microorganisms. Implications for the bioremediation of actinide-organic mixtures

    By reviewing how microorganisms interact with actinides in subsurface environments, the way how bioremediation controls the fate of actinides is assessed. Actinides often are co-contaminants with strong organic chelators, chlorinated solvents, and fuel hydrocarbons. Bioremediation can immobilize the actinides, biodegrade the co-contaminants, or both. Actinides at the IV oxidation state are the least soluble, and microorganisms accelerate precipitation by altering the actinide's oxidation state or its speciation. The way how microorganisms directly oxidize or reduce actinides and how microbiological reactions that biodegrade strong organic chelators, alter the pH, and consume or produce precipitating anions strongly affect actinide speciation and, therefore, mobility is described. Why inhibition caused by chemical or radiolytic toxicities uniquely affects microbial reactions is explained. Due to the complex interactions of the microbiological and chemical phenomena, mathematical modeling is an essential tool for research on and application of bioremediation involving co-contamination with actinides. Development of mathematical models that link microbiological and geochemical reactions is described. Throughout, the key research needs are identified. (author)

  15. Subsurface interactions of actinide species and microorganisms : implications for the bioremediation of actinide-organic mixtures.

    Banaszak, J.E.; Reed, D.T.; Rittmann, B.E.

    1999-02-12

    By reviewing how microorganisms interact with actinides in subsurface environments, we assess how bioremediation controls the fate of actinides. Actinides often are co-contaminants with strong organic chelators, chlorinated solvents, and fuel hydrocarbons. Bioremediation can immobilize the actinides, biodegrade the co-contaminants, or both. Actinides at the IV oxidation state are the least soluble, and microorganisms accelerate precipitation by altering the actinide's oxidation state or its speciation. We describe how microorganisms directly oxidize or reduce actinides and how microbiological reactions that biodegrade strong organic chelators, alter the pH, and consume or produce precipitating anions strongly affect actinide speciation and, therefore, mobility. We explain why inhibition caused by chemical or radiolytic toxicities uniquely affects microbial reactions. Due to the complex interactions of the microbiological and chemical phenomena, mathematical modeling is an essential tool for research on and application of bioremediation involving co-contamination with actinides. We describe the development of mathematical models that link microbiological and geochemical reactions. Throughout, we identify the key research needs.

  16. Subsurface interactions of actinide species and microorganisms : implications for the bioremediation of actinide-organic mixtures

    By reviewing how microorganisms interact with actinides in subsurface environments, we assess how bioremediation controls the fate of actinides. Actinides often are co-contaminants with strong organic chelators, chlorinated solvents, and fuel hydrocarbons. Bioremediation can immobilize the actinides, biodegrade the co-contaminants, or both. Actinides at the IV oxidation state are the least soluble, and microorganisms accelerate precipitation by altering the actinide's oxidation state or its speciation. We describe how microorganisms directly oxidize or reduce actinides and how microbiological reactions that biodegrade strong organic chelators, alter the pH, and consume or produce precipitating anions strongly affect actinide speciation and, therefore, mobility. We explain why inhibition caused by chemical or radiolytic toxicities uniquely affects microbial reactions. Due to the complex interactions of the microbiological and chemical phenomena, mathematical modeling is an essential tool for research on and application of bioremediation involving co-contamination with actinides. We describe the development of mathematical models that link microbiological and geochemical reactions. Throughout, we identify the key research needs

  17. Preparation of actinide targets by electrodeposition

    Trautmann, N.; Folger, H.

    1989-10-01

    Actinide targets with varying thicknesses on different substrates have been prepared by electrodeposition either from aqueous solutions or from solutions of their nitrates in isopropyl alcohol. With these techniques the actinides can be deposited almost quantitatively on various backing materials within 15 to 30 min. Targets of thorium, uranium, neptunium, plutonium, americium, curium and californium with areal densities from almost carrier-free up to 1.4 mg/cm 2 on thin beryllium, carbon, titanium, tantalum and platinum foils have been prepared. In most cases, prior to the deposition, the actinides had to be purified chemically and for some of them, due to the limited amount of material available, recycling procedures were required. Applications of actinide targets in heavy-ion reactions are briefly discussed.

  18. Actinide research to solve some practical problems

    The following topics are discussed: generation of plutonium inventories by nuclear power plants; resettlement of the Marshallese Islanders into an actinide contaminated environment; high radiation background areas of the world; and radiation hazards to uranium miners

  19. Overview of actinide chemistry in the WIPP

    Borkowski, Marian [Los Alamos National Laboratory; Lucchini, Jean - Francois [Los Alamos National Laboratory; Richmann, Michael K [Los Alamos National Laboratory; Reed, Donald T [Los Alamos National Laboratory; Khaing, Hnin [Los Alamos National Laboratory; Swanson, Juliet [Los Alamos National Laboratory

    2009-01-01

    The year 2009 celebrates 10 years of safe operations at the Waste Isolation Pilot Plant (WIPP), the only nuclear waste repository designated to dispose defense-related transuranic (TRU) waste in the United States. Many elements contributed to the success of this one-of-the-kind facility. One of the most important of these is the chemistry of the actinides under WIPP repository conditions. A reliable understanding of the potential release of actinides from the site to the accessible environment is important to the WIPP performance assessment (PA). The environmental chemistry of the major actinides disposed at the WIPP continues to be investigated as part of the ongoing recertification efforts of the WIPP project. This presentation provides an overview of the actinide chemistry for the WIPP repository conditions. The WIPP is a salt-based repository; therefore, the inflow of brine into the repository is minimized, due to the natural tendency of excavated salt to re-seal. Reducing anoxic conditions are expected in WIPP because of microbial activity and metal corrosion processes that consume the oxygen initially present. Should brine be introduced through an intrusion scenario, these same processes will re-establish reducing conditions. In the case of an intrusion scenario involving brine, the solubilization of actinides in brine is considered as a potential source of release to the accessible environment. The following key factors establish the concentrations of dissolved actinides under subsurface conditions: (1) Redox chemistry - The solubility of reduced actinides (III and IV oxidation states) is known to be significantly lower than the oxidized forms (V and/or VI oxidation states). In this context, the reducing conditions in the WIPP and the strong coupling of the chemistry for reduced metals and microbiological processes with actinides are important. (2) Complexation - For the anoxic, reducing and mildly basic brine systems in the WIPP, the most important

  20. PWRs potentialities for minor actinides burning

    In the frame of the SPIN program at CEA, the impacts of the Minor Actinides (MA) incineration in PWRs are analysed. The aim is to reduce the mass and the potential radiotoxicity level. This study is done separately one on the Plutonium recycling. But the plutonium is essential. Thus, the recycling of all Actinide elements is evaluated in a PWR nuclear yard. A sensitivity study is done to evaluate the incineration for each Minor Actinide element. This gives us the most efficient way of incineration for each MA element in a PWR and help us to design a PWR burner. This burner is disposed in a PWR nuclear system in which the Actinides are recycled until equilibrium. (authors). 2 refs

  1. Electronic structure and correlation effects in actinides

    Albers, R.C.

    1998-12-01

    This report consists of the vugraphs given at a conference on electronic structure. Topics discussed are electronic structure, f-bonding, crystal structure, and crystal structure stability of the actinides and how they are inter-related.

  2. Advanced Aqueous Separation Systems for Actinide Partitioning

    Nash, Kenneth L.; Clark, Sue; Meier, G Patrick; Alexandratos, Spiro; Paine, Robert; Hancock, Robert; Ensor, Dale

    2012-03-21

    One of the most challenging aspects of advanced processing of spent nuclear fuel is the need to isolate transuranium elements from fission product lanthanides. This project expanded the scope of earlier investigations of americium (Am) partitioning from the lanthanides with the synthesis of new separations materials and a centralized focus on radiochemical characterization of the separation systems that could be developed based on these new materials. The primary objective of this program was to explore alternative materials for actinide separations and to link the design of new reagents for actinide separations to characterizations based on actinide chemistry. In the predominant trivalent oxidation state, the chemistry of lanthanides overlaps substantially with that of the trivalent actinides and their mutual separation is quite challenging.

  3. BWR Assembly Optimization for Minor Actinide Recycling

    G. Ivan Maldonado; John M. Christenson; J.P. Renier; T.F. Marcille; J. Casal

    2010-03-22

    The Primary objective of the proposed project is to apply and extend the latest advancements in LWR fuel management optimization to the design of advanced boiling water reactor (BWR) fuel assemblies specifically for the recycling of minor actinides (MAs).

  4. Neutron scattering studies in the actinide region. Progress report, August 1, 1991--July 31, 1994

    During the period August 1, 1991 to July 31, 1994 the authors report progress on the following: (a) prompt fission neutron energy spectra for 235U and 239Pu; (b) two-parameter measurement of nuclear lifetimes; (c) 'black' neutron detector; (d) data reduction techniques for neutron scattering experiments; (e) elastic and inelastic neutron scattering studies in 197Au; (f) elastic and inelastic neutron scattering studies in 239Pu; (g) neutron induced defects in silicon dioxide MOS structures; (h) response of a 235U fission chamber near reaction thresholds; (i) efficiency calibration of a liquid scintillation detector using the WNR facility at LAMPF; (j) prompt fission neutron energy spectrum measurements below the incident neutron energy; (k) multi-parameter data acquisition system; (l) accelerator improvements; (m) non-DOE supported research. Eight Ph.D. dissertations and two M.S. theses were completed during the report period. Publications consisted of 6 journal articles, 10 conference proceedings, and 19 abstracts of presentations at scientific meetings. One invited talk was given

  5. New molecules to separate actinides: the picolinamides

    The reprocessing of spent fuel is made with the Purex process, funded on liquid-liquid extraction of uranium nitrates(VI) and plutonium nitrates(IV) by the BTP (tributyl phosphate). To improve this proceeding, we look for extractants which allow, beyond U and Pu extractions, these of actinides (II) and allow separation of the whole actinides from the fission products, which have an important fraction of lanthanides. A new family seems to give good results: the picolinamides

  6. Superconductivity in rare earth and actinide compounds

    Rare earth and actinide compounds and the extraordinary superconducting and magnetic phenomena they exhibit are surveyed. The rare earth and actinide compounds described belong to three classes of novel superconducting materials: high temperature, high field superconductors (intermetallics and layered cuprates); superconductors containing localized magnetic moments; heavy fermion superconductors. Recent experiments on the resistive upper critical field of high Tc cuprate superconductors and the peak effect in the critical current density of the f-electron superconductor CeRu2 are discussed. (orig.)

  7. Lattice effects in the light actinides

    The light actinides show a variety of lattice effects that do not normally appear in other regions of the periodic table. The article will cover the crystal structures of the light actinides, their atomic volumes, their thermal expansion behavior, and their elastic behavior as reflected in recent thermal vibration measurements made by neutron diffraction. A discussion of the melting points will be given in terms of the thermal vibration measurements. Pressure effects will be only briefly indicated

  8. Molecular structure of actinides in biochemistry

    In case of internal contamination, drugs used for decorporation are scarce and do not act very specifically. For instance the sole de-corporating drug recommended for plutonium decontamination is a water-soluble ligand named DTPA (Diethylene-Triamino-Pentaacetate). The transport of DTPA to its organ-target and its bio-availability on the spot are not satisfactorily understood. The conventional method to develop new ligands is based on molecular approaches but it is not sufficient. A new method that combines methods from structural biochemistry with methods of bio-inorganic chemistry and with methods from physico-chemistry (particularly X-ray absorption spectroscopy) is so far the best way to understand molecular speciation and to detail the local arrangement of atoms around a cation for instance, which are valuable information to understand the behaviour of a ligand. EXAFS (Extended X-ray Absorption Fine structure Spectroscopy) measurements suggest that during the formation of a complex involving an actinide (An) and a ligand, the inter-atomic distance An-O decreases when the atomic number of the cation increases while it is the reverse in the case of An-N

  9. Evaluation of actinide partitioning and transmutation

    After a few centuries of radioactive decay the long-lived actinides, the elements of atomic numbers 89-103, may constitute the main potential radiological health hazard in nuclear wastes. This is because all but a very few fission products (principally technetium-99 and iodine-129) have by then undergone radioactive decay to insignificant levels, leaving the actinides as the principal radionuclides remaining. It was therefore at first sight an attractive concept to recycle the actinides to nuclear reactors, so as to eliminate them by nuclear fission. Thus, investigations of the feasibility and potential benefits and hazards of the concept of 'actinide partitioning and transmutation' were started in numerous countries in the mid-1970s. This final report summarizes the results and conclusions of technical studies performed in connection with a four-year IAEA Co-ordinated Research Programme, started in 1976, on the ''Environmental Evaluation and Hazard Assessment of the Separation of Actinides from Nuclear Wastes followed by either Transmutation or Separate Disposal''. Although many related studies are still continuing, e.g. on waste disposal, long-term safety assessments, and waste actinide management (particularly for low and intermediate-level wastes), some firm conclusions on the overall concept were drawn by the programme participants, which are reflected in this report

  10. Recent progress in actinide borate chemistry.

    Wang, Shuao; Alekseev, Evgeny V; Depmeier, Wulf; Albrecht-Schmitt, Thomas E

    2011-10-21

    The use of molten boric acid as a reactive flux for synthesizing actinide borates has been developed in the past two years providing access to a remarkable array of exotic materials with both unusual structures and unprecedented properties. [ThB(5)O(6)(OH)(6)][BO(OH)(2)]·2.5H(2)O possesses a cationic supertetrahedral structure and displays remarkable anion exchange properties with high selectivity for TcO(4)(-). Uranyl borates form noncentrosymmetric structures with extraordinarily rich topological relationships. Neptunium borates are often mixed-valent and yield rare examples of compounds with one metal in three different oxidation states. Plutonium borates display new coordination chemistry for trivalent actinides. Finally, americium borates show a dramatic departure from plutonium borates, and there are scant examples of families of actinides compounds that extend past plutonium to examine the bonding of later actinides. There are several grand challenges that this work addresses. The foremost of these challenges is the development of structure-property relationships in transuranium materials. A deep understanding of the materials chemistry of actinides will likely lead to the development of advanced waste forms for radionuclides present in nuclear waste that prevent their transport in the environment. This work may have also uncovered the solubility-limiting phases of actinides in some repositories, and allows for measurements on the stability of these materials. PMID:21915396

  11. Calibration of a large hyperpure germanium array for in-vivo detection of the actinides with a tissue-equivalent torso phantom

    For calibration of the array for internally deposited 238Pu, 239Pu, and 241Am, a tissue-equivalent anthropomorphic phantom, was used for efficiency determinations at the ORNL facility. This phantom consists of a tissue-equivalent torso into which is imbedded an adult male skeleton, interchangeable organs containing a homogeneous distribution of various radionuclides, and two sets of chest overlay plates for simulation of progressively thicker tissue over the chest, as well as differing thoracic fat contents

  12. Surface energy and work function of the light actinides

    Kollár, J.; Vitos, Levente; Skriver, Hans Lomholt

    1994-01-01

    We have calculated the surface energy and work function of the light actinides Fr, Ra, Ac, Th, Pa, U, Np, and Pu by means of a Green's-function technique based on the linear-muffin-tin-orbitals method within the tight-binding representation. In these calculations we apply an energy functional which...... combines the kinetic energy calculated within the atomic-sphere approximation with Coulomb- and exchange-correlation-energy terms calculated by means of the complete nonspherically symmetric charge density derived from the atomic-sphere potential within nonoverlapping and space-filling cells. The...... calculated surface energies and work functions are in good agreement with the limited experimental data....

  13. Physical mechanism analysis of burnup actinide composition in light water reactor MOX fuel and its application to uncertainty evaluation

    Highlights: • We discuss physical mechanisms for burnup actinide compositions in LWR’s MOX fuel. • Mechanisms of 244Cm and 238Pu productions are analyzed in detail with sensitivity. • We can evaluate the indirect effect on actinide productions by nuclear reactions. • Burnup sensitivity is applied to uncertainty evaluation of nuclide production. • Actinides can be categorized into patterns according to a burnup sensitivity trend. - Abstract: In designing radioactive waste management and decommissioning facilities, understanding the physical mechanisms for burnup actinide composition is indispensable to satisfy requirements for its validity and reliability. Therefore, the uncertainty associated with physical quantities, such as nuclear data, needs to be quantitatively analyzed. The present paper illustrates an analysis methodology to investigate the physical mechanisms of burnup actinide composition with nuclear-data sensitivity based on the generalized depletion perturbation theory. The target in this paper is the MOX fuel of the light water reactor. We start with the discussion of the basic physical mechanisms for burnup actinide compositions using the reaction-rate flow chart on the burnup chain. After that, the physical mechanisms of the productions of Cm-244 and Pu-238 are analyzed in detail with burnup sensitivity calculation. Conclusively, we can identify the source of actinide productions and evaluate the indirect influence of the nuclear reactions if the physical mechanisms of burnup actinide composition are analyzed using the reaction-rate flow chart on the burnup chain and burnup sensitivity calculation. Finally, we demonstrate the usefulness of the burnup sensitivity coefficients in an application to determine the priority of accuracy improvement in nuclear data in combination with the covariance of the nuclear data. In addition, the target actinides and reactions are categorized into patterns according to a sensitivity trend

  14. Hydration properties and ionic radii of actinide(III) ions in aqueous solution

    Ionic radii of actinide(III) cations (from U(III) to Cf(III)) in aqueous solution have been derived for the first time starting from accurate experimental determination of the ion-water distances obtained by combining extended X-ray absorption fine structure (EXAFS) results and molecular dynamics (MD) structural data. A strong analogy has been found between the lanthanide and actinide series concerning hydration properties. The existence of a contraction of the An-O distance along the series has been highlighted, while no decrease of the hydration number is evident up to Cf(III). (authors)

  15. Radioecology of the actinide elements

    Research progress is reported in sections entitled: scope of studies supported by the Department of Energy; oxidation state diagrams are a potential tool for studying the redox chemistry of Pu in natural waters; studies are initiated to investigate the effect of pH and organic matter on the distribution coefficients of Cm with natural sediments; the relative distributions of resuspended and direct deposited Pu in a corn canopy are quantified; the retention of Pu surface contamination by corn plants is being studied; Pu concentrations in tobacco are being determined; concentrations of Pu per unit mass and per unit surface area are compared for subterranean crops; models of Pu behavior in agricultural crops are being validated; distribution of aerially released Pu in loblolly pine plantations is independent of deposition rate; investigation of the effects of chelate and redox potential of the uptake of Pu and Cm by rice is underway; studies of Cm cycling in a floodplain forest have been initiated; the effects of unusually large Pu deposition onto a wheat ecosystem are being studied using computer simulations; long-term kinetic models of Pu behavior in plant-soil systems are being developed; scope of studies supported by the Nuclear Regulatory Commission; growth form of broadleaf crop may affect Pu contents; root uptake of Pu and Cm measured for rice root uptake of Pu and Cm measured for rice; long-term actinide uptake study is continuing at SREL; and uranium cycling in major southeastern agricultural crops being studied

  16. Actinide transmutation in nuclear reactors

    An optimization method is developed to maximize the burning capability of the ALMR while complying with all constraints imposed on the design for reliability and safety. This method leads to a maximal transuranics enrichment, which is being limited by constraints on reactivity. The enrichment can be raised by using the neutrons less efficiently by increasing leakage from the fuel. With the developed optimization method, a metallic and an oxide fueled ALMR were optimized. Both reactors perform equally well considering the burning of transuranics. However, metallic fuel has a much higher heat conductivity coefficient, which in general leads to better safety characteristics. In search of a more effective waste transmuter, a modified Molten Salt Reactor was designed. A MSR operates on a liquid fuel salt which makes continuous refueling possible, eliminating the issue of the burnup reactivity loss. Also, a prompt negative reactivity feedback is possible for an overmoderated reactor design, even when the Doppler coefficient is positive, due to the fuel expansion with fuel temperature increase. Furthermore, the molten salt fuel can be reprocessed based on a reduction process which is not sensitive to the short-lived spontaneously fissioning actinides. (orig./HP)

  17. An introduction to the Advanced Testing Line for Actinide Separations (ATLAS)

    Pope, N.G.; Yarbro, S.L.; Schreiber, S.B.; Day, R.S.

    1992-03-01

    The Advanced Testing Line for Actinide Separations (ATLAS) will evaluate promising plutonium recovery process modifications and new technologies. It combines advances in process chemistry, process control, process analytical chemistry, and process engineering. ATLAS has a processing capability equal to other recovery systems but without the pressure to achieve predetermined recovery quotas.

  18. An introduction to the Advanced Testing Line for Actinide Separations (ATLAS)

    The Advanced Testing Line for Actinide Separations (ATLAS) will evaluate promising plutonium recovery process modifications and new technologies. It combines advances in process chemistry, process control, process analytical chemistry, and process engineering. ATLAS has a processing capability equal to other recovery systems but without the pressure to achieve predetermined recovery quotas

  19. Solubility of actinide surrogates in nuclear glasses

    This paper discusses the results of a study of actinide surrogates in a nuclear borosilicate glass to understand the effect of processing conditions (temperature and oxidizing versus reducing conditions) on the solubility limits of these elements. The incorporation of cerium oxide, hafnium oxide, and neodymium oxide in this borosilicate glass was investigated. Cerium is a possible surrogate for tetravalent and trivalent actinides, hafnium for tetravalent actinides, and neodymium for trivalent actinides. The material homogeneity was studied by optical, scanning electron microscopy. Cerium LIII XANES spectroscopy showed that the Ce3+/Cetotal ratio increased from about 0.5 to 0.9 as the processing temperature increased from 1100 to 1400 deg. C. Cerium LIII XANES spectroscopy also confirmed that the increased Ce solubility in glasses melted under reducing conditions was due to complete reduction of all the cerium in the glass. The most significant results pointed out in the current study are that the solubility limits of the actinide surrogates increases with the processing temperature and that Ce3+ is shown to be more soluble than Ce4+ in this borosilicate glass

  20. Waste disposal aspects of actinide separation

    Two recent NRPB reports are summarized (Camplin, W.C., Grimwood, P.D. and White, I.F., The effects of actinide separation on the radiological consequences of disposal of high-level radioactive waste on the ocean bed, Harwell, National Radiological Protection Board, NRPB-R94 (1980), London, HMSO; Hill, M.D., White, I.F. and Fleishman, A.B., The effects of actinide separation on the radiological consequences of geologic disposal of high-level waste. Harwell, National Radiological Protection Board, NRPB-R95 (1980), London, HMSO). They describe preliminary environmental assessments relevant to waste arising from the reprocessing of PWR fuel. Details are given of the modelling of transport of radionuclides to man, and of the methodology for calculating effective dose equivalents in man. Emphasis has been placed on the interaction between actinide separation and the disposal options rather than comparison of disposal options. The reports show that the effects of actinide separation do depend on the disposal method. Conditions are outlined where the required substantial further research and development work on actinide separation and recycle would be justified. Toxicity indices or 'toxic potentials' can be misleading and should not be used to guide research and development. (U.K.)

  1. Use of fast reactors for actinide transmutation

    The management of radioactive waste is one of the key issues in today's discussions on nuclear energy, especially the long term disposal of high level radioactive wastes. The recycling of plutonium in liquid metal fast breeder reactors (LMFBRs) would allow 'burning' of the associated extremely long life transuranic waste, particularly actinides, thus reducing the required isolation time for high level waste from tens of thousands of years to hundreds of years for fission products only. The International Working Group on Fast Reactors (IWGFR) decided to include the topic of actinide transmutation in liquid metal fast breeder reactors in its programme. The IAEA organized the Specialists Meeting on Use of Fast Breeder Reactors for Actinide Transmutation in Obninsk, Russian Federation, from 22 to 24 September 1992. The specialists agree that future progress in solving transmutation problems could be achieved by improvements in: Radiochemical partitioning and extraction of the actinides from the spent fuel (at least 98% for Np and Cm and 99.9% for Pu and Am isotopes); technological research and development on the design, fabrication and irradiation of the minor actinides (MAs) containing fuels; nuclear constants measurement and evaluation (selective cross-sections, fission fragments yields, delayed neutron parameters) especially for MA burners; demonstration of the feasibility of the safe and economic MA burner cores; knowledge of the impact of maximum tolerable amount of rare earths in americium containing fuels. Refs, figs and tabs

  2. New reagents for actinide-lanthanide group separations

    Organic extractants which possess nitrogen or sulfur donor atoms preferentially complex the trivalent actinide. They are potential reagents for actinide lanthanide group separations, which can be performed at low pH without the addition of inorganic salts

  3. Separation of actinides with alkylpyridinium salts

    Various f-elements are separated as anionic complexes from both acidic and alkaline solutions by precipitation with alkylpyridinium salts. The precipitates are also cationic surfactants where the simple counter-ion (e.g. nitrate or chloride) is replaced by the negatively charged complex anion of an actinide or lanthanide. The low solubility of these precipitates is explained by a strong affinity of divalent complex counter-ions of f-elements to the quaternary nitrogen. Precipitations in solutions of nitric acid allow to separate tetravalent f-elements from other metals, in alkaline carbonate solutions tetravalent and hexavalent actinides are precipitated simultaneously. The last procedure yields precipitates, which are very intimate mixtures of hexavalent and tetravalent actinides. This allows to prepare mixed oxides in a simple way. (author) 6 refs.; 3 figs.; 3 tabs

  4. Neutron scattering studies of the actinides

    The electronic structure of actinide materials presents a unique example of the interplay between localized and band electrons. Together with a variety of other techniques, especially magnetization and the Mossbauer effect, neutron studies have helped us to understand the systematics of many actinide compounds that order magnetically. A direct consequence of the localization of 5f electrons is the spin-orbit coupling and subsequent spin-lattice interaction that often leads to strongly anisotropic behavior. The unusual phase transition in UO2, for example, arises from interactions between quadrupole moments. On the other hand, in the monopnictides and monochalcogenides, the anisotropy is more difficult to understand, but probably involves an interaction between actinide and anion wave functions. A variety of neutron experiments, including form-factor studies, critical scattering and measurements of the elementary excitations have now been performed, and the conceptual picture emerging from these studies will be discussed

  5. Coordination chemistry for new actinide separation processes

    The amount of wastes and the number of chemical steps can be decreased by replacing the PUREX process extractant (TBP) by, N.N- dialkylamides (RCONR'2). Large amounts of deep underground storable wastes can be stored into sub-surface disposals if the long lived actinide isotopes are removed. Spent nuclear fuels reprocessing including the partitioning of the minor actinides Np, Am, Cm and their transmutation into short half lives fission products is appealing to the public who is not favorable to the deep underground storage of large amounts of long half lived actinide isotopes. In this paper coordination chemistry problems related to improved chemical separations by solvent extraction are presented. 2 tabs.; 4 refs

  6. Research on Actinides in Nuclear Fuel Cycles

    The electrochemical/spectroscopic integrated measurement system was designed and set up for spectro-electrochemical measurements of lanthanide and actinide ions in high temperature molten salt media. A compact electrochemical cell and electrode system was also developed for the minimization of reactants, and consequently minimization of radioactive waste generation. By applying these equipment, oxidation and reduction behavior of lanthanide and actinide ions in molten salt media have been made. Also, thermodynamic parameter values are determined by interpreting the results obtained from electrochemical measurements. Several lanthanide ions exhibited fluorescence properties in molten salt. Also, UV-VIS measurement provided the detailed information regarding the oxidation states of lanthanide and actinide ions in high temperature molten salt media

  7. Radiolytic oxidation of UO{sub 2} pellets doped with alpha-emitters ({sup 238/239}Pu)

    Muzeau, B. [Commissariat a l' Energie Atomique, Rhone Valley Research Center DTCD/SECM/LMPA, BP 17 171, 30207 Bagnols-sur-Ceze Cedex (France); Jegou, C. [Commissariat a l' Energie Atomique, Rhone Valley Research Center DTCD/SECM/LMPA, BP 17 171, 30207 Bagnols-sur-Ceze Cedex (France)], E-mail: christophe.jegou@cea.fr; Delaunay, F. [Commissariat a l' Energie Atomique, Valduc Research Center, 21120 Is-sur-Tille (France); Broudic, V. [Commissariat a l' Energie Atomique, Rhone Valley Research Center DTCD/SECM/LMPA, BP 17 171, 30207 Bagnols-sur-Ceze Cedex (France); Brevet, A. [Commissariat a l' Energie Atomique, Valduc Research Center, 21120 Is-sur-Tille (France); Catalette, H. [Electricite de France, Les Renardieres Research Center, Route de Sens Ecuelles, 77250 Moret-sur-Loing (France); Simoni, E. [Institut de Physique Nucleaire, Bat. 100, 91406 Orsay Cedex (France); Corbel, C. [Laboratoire des Solides Irradies, UMR 7642-CNRS-CEA-Ecole Polytechnique, Ecole Polytechnique, 91128 Palaiseau Cedex (France)

    2009-01-07

    To assess the impact of alpha radiolysis of water on the oxidative dissolution of UO{sub 2} under anoxic conditions, two series of plutonium-doped samples (specific alpha activity 385 and 18 MBqg{sub UO{sub 2}}{sup -1}) were fabricated, characterized and leached in water of varying complexity (pure water, carbonated water, dissolved hydrogen). Given the very high reactivity of these samples in the presence of air and in order to minimize any prior surface oxidation, a strict experimental protocol was developed based on high-temperature annealing in Ar + 4% H{sub 2} with preleaching cycles. Failure to follow this protocol prevents absolute quantification of oxidation of the UO{sub 2} surface by water radiolysis in solutions. Preoxidation of the pellet surface can lead to uranium release in solution that is dependent on the alpha particle flux, revealing initial oxidation by radiolysis in air including potential traces of water. This makes difficult the accurate quantification of the radiolytic oxidation in water solutions. Controlling the initial surface condition of the samples finally allowed us to demonstrate that radiolytic oxidation in water-saturated media is governed by several threshold effects for which the main parameters are the sample alpha activity and the hydrogen concentration.

  8. Comparison and development of new extraction procedures for 239Pu, Ca, Fe and Cu organic complexes in soil

    Two new extraction methods - the silylation of the organic constituents of soil with trimethylchlorosilane (TMCS) and triethylchlorosilane (TECS) in the presence of dimethylformamide (DMF) -have been developed for mobilization of the organic complexes of Ca, Fe, Cu and Pu which might exist in some soils. By silylation of the carboxylic, phenolic, alcoholic and perhaps the amino moieties of humic and fulvic acids (the principal organic constituents of soils) the authors have modified the solubility of the humic substances with perhaps a minimum perturbation of the humate-metal ion complexes. These new extraction procedures, which used a non-aqueous solvent, have been compared with a variety of aqueous extraction procedures (sodium hydroxide, 1 M potassium chloride and diethylene triaminepentaacetic acid solution) and found to be superior in the release of the elements from soils. (author)

  9. Fission fragment charge and mass distributions in 239Pu(n,f) in the adiabatic nuclear energy density functional theory

    Regnier, D.; Dubray, N.; Schunck, N.; Verriere, M.

    2016-01-01

    Accurate knowledge of fission fragment yields is an essential ingredient of numerous applications ranging from the formation of elements in the r-process to fuel cycle optimization for nuclear energy. The need for a predictive theory applicable where no data is available is an incentive to develop a fully microscopic approach to fission dynamics. In this work, we calculate the pre-neutron emission charge and mass distributions of the fission fragments formed in the neutron-induced fission of ...

  10. Toxicity of inhaled 239PuO2 in immature, young adult and aged Syrian hamsters. IV

    Human populations that might be exposed in the event of a catastrophic nuclear accident would include individuals with widely differing ages. To obtain better information in the possible effects of age on observed dose-response relationships for inhaled 238PuO2, groups of Syrian hamsters were exposed via inhalation at either 28 (immature), 84 (young adults) or 340 (aged) days of age to polydisperse aerosols of 238PuO2. The graded levels of initial lung burden were 240, 60, 15, 3.8, 0.95, 0.25 and 0.029 nCi for the immature and young adult animals and 240, 60, and 3.8 nCi for the aged animals. Additional animals were included in the 60 nCi initial lung burden level for serial sacrifice to determine the radiation dose pattern. All other animals were maintained for life span observation. Lung retention determined for each age group varied in the fraction of the initial burden undergoing rapid initial clearance; 63% cleared with a half-time of 1.2 days for the immature group and 22% cleared with a half-time of 2 days for the young adult group. No separate initial phase of clearance was evident for the aged animals. For all age groups, less than 1% of the sacrifice body burden was found in all tissues other than lung. Mortality data analysis indicated significant life shortening only in animals which received the highest level initial lung burden. These early deaths were related to radiation pneumonitis and pulmonary fibrosis. No pulmonary neoplasms have been observed to date

  11. Transuranic concentrations in reef and pelagic fish from the Marshall Islands. [/sup 239/Pu, /sup 240/Pu

    Noshkin, V.E.; Eagle, R.J.; Wong, K.M.; Jokela, T.A.

    1980-09-01

    Concentrations of /sup 239 + 240/Pu are reported in tissues of several species of reef and pelagic fish caught at 14 different atolls in the northern Marshall Islands. Several regularities that are species dependent are evident in the distribution of /sup 239 + 240/Pu among different body tissues. Concentrations in liver always exceeded those in bone and concentrations were lowest in the muscle of all fish analyzed. A progressive discrimination against /sup 239 + 240/Pu was observed at successive trophic levels at all atolls except Bikini and Enewetak, where it was difficult to conclude if any real difference exists between the average concentration factor for /sup 239 + 240/Pu among all fish, which include bottom feeding and grazing herbivores, bottom feeding carnivores, and pelagic carnivores from different atoll locations. The average concentration of /sup 239 + 240/Pu in the muscle of surgeonfish from Bikini and Enewetak was not significantly different from the average concentrations determined in these fish at the other, lesser contaminated atolls. Concentrations among all 3rd, 4th, and 5th trophic level species are highest at Bikini where higher environmental concentrations are found. The reasons for the anomalously low concentrations in herbivores from Bikini and Enewetak are not known.

  12. Final Report for Nuclear Resonance Fluorescence Measurements of 239Pu above 2.5 MeV

    Johnson, M S; McNabb, D P

    2009-01-07

    Nuclear Resonance Fluorescence measurements were performed at the free electron laser facility at UC Santa Barbara using a bremsstrahlung beam. Three endpoint energies were chosen for the bremsstrahlung to cover as much area above 2.5 MeV as possible. We were able to set an upper limit of NRF state strengths between 2.5 and 3.8 MeV at roughly 38(5) eV barns at the 4-sigma level and 9(2) eV barns at the 1-sigma level. Published results on states near 2.4 MeV indicate strengths about 10(2) eV barns. Details of the results are presented in this report.

  13. Spatial statistical analysis of contamination level of 241Am and 239Pu, Thule, North-West Greenland

    Strodl Andersen, J. (JSA EnviroStat (Denmark))

    2011-10-15

    A spatial analysis of data on radioactive pollution on land at Thule, North-West Greenland is presented. The data comprises levels of 241Am and 239,240Pu on land. Maximum observed level of 241Am is 2.8x105 Bq m-2. Highest levels were observed near Narsaarsuk. This area was also sampled most intensively. In Groennedal the maximum observed level of 241Am is 1.9-104 Bq m-2. Prediction of the overall amount of 241Am and 239,240Pu is based on grid points within the range from the nearest measurement location. The overall amount is therefore highly dependent on the model. Under the optimal spatial model for Narsaarsuk, within the area of prediction, the predicted total amount of 241Am is 45 GBq and the predicted total amount of 239,240Pu is 270 GBq. (Author)

  14. Evaluation of fission product yields from fission spectrum n+239Pu using a meta analysis of benchmark data

    Chadwick, Mark B.

    2009-10-01

    Los Alamos conducted a dual fission-chamber experiment in the 1970s in the Bigten critical assembly to determine fission product data in a fast (fission neutron spectrum) environment, and this defined the Laboratory's fission basis today. We describe how the data from this experiment are consistent with other benchmark fission product yield measurements for 95,97Zr, 140Ba, 143,144Ce, 137Cs from the NIST-led ILRR fission chamber experiments, and from Maeck's mass-spectrometry data. We perform a new evaluation of the fission product yields that is planned for ENDF/B-VII.1. Because the measurement database for some of the FPs is small—especially for 147Nd and 99Mo—we use a meta-analysis that incorporates insights from other accurately-measured benchmark FP data. The %-relative changes compared to ENDF/B-VI are small for some FPs (less than 1% for 95Zr, 140Ba, 144Ce), but are larger for 99Mo (3%) and 147Nd (5%). We suggest an incident neutron energy dependence to the 147Nd fission product yield that accounts for observed differences in the FPY at a few-hundred keV average energy in fast reactors versus measurements made at higher average energies.

  15. Neutron multiplicity for neutron induced fission of 235U, 238U, and 239Pu as a function of neutron energy

    Recent development in the theory and practice of neutron correlation (''coincidence'') counting require knowledge of the higher factorial moments of the P/sub ν/ distribution (the probability that (ν) neutrons are emitted in a fission) for the case where the fission is induced by bombarding neutrons of more than thermal energies. In contrast to the situation with spontaneous and thermal neutron induced fission, where with a few exceptions the P/sub ν/ is reasonably well known, in the fast neutron energy region, almost no information is available concerning the multiplicity beyond the average value, [ν], even for the most important nuclides. The reason for this is the difficulty of such experiments, with consequent statistically poor and physically inconsistent results

  16. Successful DTPA therapy in the case of 239Pu penetration via injured skin exposed to nitric acid

    This paper presents results of the radiological study and DTPA therapy for a worker exposed to a plutonium nitrate solution. Plutonium levels were measured in excreta, blood, plasma and wound for several weeks. Plutonium renal clearance ranged from 110-190 ml min-1 to 3-4 ml min-1 at different stages of chelation therapy. Plutonium absorption into blood from the injured skin amounted to 4.3%. As a result of intensive therapy, 96% of absorbed plutonium was successfully excreted. (author)

  17. A comparison of the distribution of 239-Pu and calcein in the ilium of the female CBA mouse

    It is well recognised that plutonium 239 and certain vital stains such as calcein behave similarly when injected i.v. into experimental animals. Both are rapidly cleared from blood, and concentrate on bone surfaces. Certain differences of behaviour are also known, such as the competitive concentration of plutonium in liver and other soft tissues; and differences in the distribution of site of location of the substances on bone surface. Plutonium tends to concentrate evenly on all bone surfaces in proportion to the blood supply to that region, leading to higher concentrations on endosteal than periosteal surfaces. Calcein deposits at sites of mineralisation, which occur on both endosteum and periosteum in response to the demands of growth and remodelling. Subsequent behaviour of both substances would appear to depend entirely on the growth and remodelling activities of the bone, the deposits remaining fixed in position until the containing bone is resorbed or buried by freshly formed bone. Many studies of the distribution and dosimetry of plutonium in experimental animals, mainly dogs, and mice have been recorded. There is however, a lack of information concerning the behaviour of the radionuclide in man. More information is available on the behaviour in man and experimental animals of the vital stains, some of which are well known anti-biotics. Consequently, there is much to be gained if a knowledge of the behaviour of vital stains such as calcein can be used to predict the distribution of plutonium in the human skeleton. (orig.)

  18. Assessing the role of the (n, γ f) process in the low-energy fission of actinides

    Talou, Patrick; Lynn, J. E.; Kawano, T.; Mosby, S.; Couture, A.; Bouland, O.

    2016-06-01

    We review the role of the (n, γ f) process in the low-energy neutron-induced fission reaction of 239Pu. Recent measurements of the average total γ-ray energy released in this reaction were performed with the Detector for Advanced Neutron Capture Experiments (DANCE) at Los Alamos. Significant fluctuations of this quantity in the resonance region below 100 eV can be interpreted by invoking the presence of the indirect (n, γ f) process. Modern calculations of the probability for such an event to occur are presented.

  19. Actinide elements in aquatic and terrestrial environments

    Progress is reported on the following research projects: water-sediment interactions of U, Pu, Am, and Cm; relative availability of actinide elements from abiotic to aquatic biota; comparative uptake of transuranic elements by biota bordering Pond 3513; metabolic reduction of 239Np from Np(V) to Np(IV) in cotton rats; evaluation of hazards associated with transuranium releases to the biosphere; predicting Pu in bone; adsorption--solubility--complexation phenomena in actinide partitioning between sorbents and solution; comparative soil extraction data; and comparative plant uptake data

  20. Sequential analysis of selected actinides in urine

    The monitoring of personnel by urinalysis for suspected contamination by actinides necessitated the development and implementation of an analytical scheme that will separate and identify alpha emitting radionuclides of these elements. The present work deals with Pu, Am, and Th. These elements are separated from an ashed urine sample by means of coprecipitation and ion exchange techniques. The final analysis is carried out by electroplating the actinides and counting in a α-spectrometer. Mean recoveries of these elements from urine are: Pu 64%, Am 74% and Th 69%. (auth)

  1. Spin-Orbit Coupling in Actinide Cations

    Bagus, Paul S.; Ilton, Eugene S.; Martin, Richard L.; Jensen, Hans Jorgen A.; Knecht, Stefan

    2012-09-01

    The limiting case of Russell-Saunders coupling, which leads to a maximum spin alignment for the open shell electrons, usually explains the properties of high spin ionic crystals with transition metals. For actinide compounds, the spin-orbit splitting is large enough to cause a significantly reduced spin alignment. Novel concepts are used to explain the dependence of the spin alignment on the 5f shell occupation. We present evidence that the XPS of ionic actinide materials may provide direct information about the angular momentum coupling within the 5f shell.

  2. Spin-orbit coupling in actinide cations

    Bagus, Paul S.; Ilton, Eugene S.; Martin, Richard L.; Jensen, Hans Jørgen Aa.; Knecht, Stefan

    2012-09-01

    The limiting case of Russell-Saunders coupling, which leads to a maximum spin alignment for the open shell electrons, usually explains the properties of high spin ionic crystals with transition metals. For actinide compounds, the spin-orbit splitting is large enough to cause a significantly reduced spin alignment. Novel concepts are used to explain the dependence of the spin alignment on the 5f shell occupation. We present evidence that the XPS of ionic actinide materials may provide direct information about the angular momentum coupling within the 5f shell.

  3. Actinide and fission product separation and transmutation

    NONE

    1993-07-01

    The second international information exchange meeting on actinide and fission product separation and transmutation, took place in Argonne National Laboratory in Illinois United States, on 11-13 November 1992. The proceedings are presented in four sessions: Current strategic system of actinide and fission product separation and transmutation, progress in R and D on partitioning processes wet and dry, progress in R and D on transmutation and refinements of neutronic and other data, development of the fuel cycle processes fuel types and targets. (A.L.B.)

  4. Actinide phosphonate complexes in aqueous solutions

    Complexes formed by actinides with carboxylic acids, polycarboxylic acids, and aminopolycarboxylic acids play a central role in both the basic and process chemistry of the actinides. Recent studies of f-element complexes with phosphonic acid ligands indicate that new ligands incorporating doubly ionizable phosphonate groups (-PO3H2) have many properties which are unique chemically, and promise more efficient separation processes for waste cleanup and environmental restoration. Simple diphosphonate ligands form much stronger complexes than isostructural carboxylates, often exhibiting higher solubility as well. In this manuscript recent studies of the thermodynamics and kinetics of f-element complexation by 1,1 and 1,2 diphosphonic acid ligands are described

  5. Actinide and fission product separation and transmutation

    The second international information exchange meeting on actinide and fission product separation and transmutation, took place in Argonne National Laboratory in Illinois United States, on 11-13 November 1992. The proceedings are presented in four sessions: Current strategic system of actinide and fission product separation and transmutation, progress in R and D on partitioning processes wet and dry, progress in R and D on transmutation and refinements of neutronic and other data, development of the fuel cycle processes fuel types and targets. (A.L.B.)

  6. Actinide recycle in LMFBRs as a waste management alternative

    Beaman, S.L.

    1979-08-21

    A strategy of actinide burnup in fast reactor systems has been investigated as an approach for reducing the long term hazards and storage requirements of the actinide waste elements and their decay daughters. The actinide recycle studies also included plutonium burnup studies in the event that plutonium is no longer required as a fuel. Particular emphasis was placed upon the timing of the recycle program, the requirements for separability of the waste materials, and the impact of the actinides on the reactor operations and performance. It is concluded that actinide recycle and plutonium burnout are attractive alternative waste management concepts. 25 refs., 14 figs., 34 tabs.

  7. Actinide recycle in LMFBRs as a waste management alternative

    A strategy of actinide burnup in fast reactor systems has been investigated as an approach for reducing the long term hazards and storage requirements of the actinide waste elements and their decay daughters. The actinide recycle studies also included plutonium burnup studies in the event that plutonium is no longer required as a fuel. Particular emphasis was placed upon the timing of the recycle program, the requirements for separability of the waste materials, and the impact of the actinides on the reactor operations and performance. It is concluded that actinide recycle and plutonium burnout are attractive alternative waste management concepts. 25 refs., 14 figs., 34 tabs

  8. Multiconfigurational quantum chemistry for actinide containing systems: from isolated molecules to condensed phase

    Complete text of publication follows: Ab initio quantum chemistry is a mature science that allows the study of molecular species containing any of the atoms in the periodic system. In this lecture I will describe our latest achievements in the prediction of novel chemical bonds and chemical species, including the multiple bond in the early-di-actinide series [1] and some novel inorganic compounds containing the di-uranium moiety [2]. In nature most of actinide chemistry occurs in solution. We try to combine ab initio quantum chemistry with classical molecular dynamics simulations in order to understand the behavior of highly charged ions in solution. Our recent studies of uranyl [3] and Cm(III) [4] in water will be presented. References: [1] B. O. Roos, P.-A. Malmqvist and L. Gagliardi, Exploring the actinide-actinide bond: Theoretical studies of the chemical bond in Ac2, Th2, Pa2, and U2 J. Am. Chem. Soc. 128, 17000-17006 (2006) [2] G. La Macchia, M. Brynda, and L. Gagliardi, Quantum chemical calculations predict the diphenyl di-uranium compound, PhUUPh, to have a stable 1Ag ground state Angew. Chem. Int. Ed. 45, 6210-6213 (2006); [3] D. Hagberg, G. Karlstrom, B .O. Roos and L. Gagliardi, The coordination of uranyl in water: a combined quantum chemical and molecular simulation study J. Am. Chem. Soc. 127, 14250-14256 (2005); [4] E. Bednarz, D. Hagberg, L. Gagliardi in preparation

  9. Treatment of actinide-containing organic waste

    A method has been developed for reducing the volume of organic wastes and recovering the actinide elements. The waste, together with gaseous oxygen (air) is introduced into a molten salt, preferably an alkali metal carbonate such as sodium carbonate. The bath is kept at 7500 - 10000C and 0.5 - 10 atm to thermally decompose and partially oxidize the waste, while substantially reducing its volume. The gaseous effluent, mainly carbon dioxide and water vapour, is vented to the atmosphere through a series of filters to remove trace amounts of actinide elements or particulate alkali metal salts. The remaining combustion products are entrained in the molten salt. Part of the molten salt-combustion product mixture is withdrawn and mixed with an aqueous medium. Insoluble combustion products are then removed from the aqueous medium and are leached with a mixture of hydrofluoric and nitric acids to solubilize the actinide elements. The actinide elements are easily recovered from the acid solution using conventional techniques. (DN)

  10. Actinide measurements by AMS using fluoride matrices

    Cornett, R. J.; Kazi, Z. H.; Zhao, X.-L.; Chartrand, M. G.; Charles, R. J.; Kieser, W. E.

    2015-10-01

    Actinides can be measured by alpha spectroscopy (AS), mass spectroscopy or accelerator mass spectrometry (AMS). We tested a simple method to separate Pu and Am isotopes from the sample matrix using a single extraction chromatography column. The actinides in the column eluent were then measured by AS or AMS using a fluoride target matrix. Pu and Am were coprecipitated with NdF3. The strongest AMS beams of Pu and Am were produced when there was a large excess of fluoride donor atoms in the target and the NdF3 precipitates were diluted about 6-8 fold with PbF2. The measured concentrations of 239,240Pu and 241Am agreed with the concentrations in standards of known activity and with two IAEA certified reference materials. Measurements of 239,240Pu and 241Am made at A.E. Lalonde AMS Laboratory agree, within their statistical uncertainty, with independent measurements made using the IsoTrace AMS system. This work demonstrated that fluoride targets can produce reliable beams of actinide anions and that the measurement of actinides using fluorides agree with published values in certified reference materials.

  11. Trends in actinide processing at Hanford

    In 1989, the mission at the Hanford Site began a dramatic and sometimes painful transition. The days of production--as we used to know it--are over. Our mission officially has become waste management and environmental cleanup. This mission change didn't eliminate many jobs--in fact, budgets have grown dramatically to support the new mission. Most all of the same skilled crafts, engineers, and scientists are still required for the new mission. This change has not eliminated the need for actinide processing, but it has certainly changed the focus that our actinide chemists and process engineers have. The focus used to be on such things as increasing capacity, improving separations efficiency, and product purity. Minimizing waste had become a more important theme in recent years and it is still a very important concept in the waste management and environmental cleanup arena. However, at Hanford, a new set of words dominates the actinide process scene as we work to deal with actinides that still reside in a variety of forms at the Hanford Site. These words are repackage, stabilize, remove, store and dispose. Some key activities in each of these areas are described in this report

  12. Report of the panel on inhaled actinides

    Some topics discussed are as follows: assessment of risks to man of inhaling actinides; use of estimates for developing protection standards; epidemiology of lung cancer in exposed human populations; development of respiratory tract models; and effects in animals: dose- and effect-modifying factors

  13. Electronic Structure of the Actinide Metals

    Johansson, B.; Skriver, Hans Lomholt

    1982-01-01

    itinerant to localized 5f electron behaviour calculated to take place between plutonium and americium. From experimental data it is shown that the screening of deep core-holes is due to 5f electrons for the lighter actinide elements and 6d electrons for the heavier elements. A simplified model for the full...

  14. Actinide and fission product partitioning and transmutation

    The third international information exchange meeting on actinide and fission product partitioning and transmutation, took place in Cadarache France, on 12-14 December 1994. The proceedings are presented in six sessions : an introduction session, the major programmes and international cooperation, the systems studies, the reactors fuels and targets, the chemistry and a last discussions session. (A.L.B.)

  15. Actinide and fission product partitioning and transmutation

    NONE

    1995-07-01

    The third international information exchange meeting on actinide and fission product partitioning and transmutation, took place in Cadarache France, on 12-14 December 1994. The proceedings are presented in six sessions : an introduction session, the major programmes and international cooperation, the systems studies, the reactors fuels and targets, the chemistry and a last discussions session. (A.L.B.)

  16. Rapid determination of actinides in asphalt samples

    A new rapid method for the determination of actinides in asphalt samples has been developed that can be used in emergency response situations or for routine analysis. If a radiological dispersive device, improvised nuclear device or a nuclear accident such as the accident at the Fukushima Nuclear Power Plant in March, 2011 occurs, there will be an urgent need for rapid analyses of many different environmental matrices, including asphalt materials, to support dose mitigation and environmental clean-up. The new method for the determination of actinides in asphalt utilizes a rapid furnace step to destroy bitumen and organics present in the asphalt and sodium hydroxide fusion to digest the remaining sample. Sample preconcentration steps are used to collect the actinides and a new stacked TRU Resin + DGA Resin column method is employed to separate the actinide isotopes in the asphalt samples. The TRU Resin plus DGA Resin separation approach, which allows sequential separation of plutonium, uranium, americium and curium isotopes in asphalt samples, can be applied to soil samples as well. (author)

  17. Placental transfer of plutonium and other actinides

    The report is based on an extensive literature search. All data available from studies on placental transfer of plutonium and other actinides in man and animals have been collected and analysed, and the report presents the significant results as well as unresolved questions and knowledge gaps which may serve as a waypost to future research work. (orig./MG)

  18. ENDF/B-5 Actinides (Rev. 86)

    This document summarizes the contents of the Actinides part of the ENDF/B-5 nuclear data library released by the US National Nuclear Data Center. This library or selective retrievals of it, are available costfree from the IAEA Nuclear Data Section upon request. The present version of the library is the Revision of 1986. (author). Refs, figs and tabs

  19. Spin–orbit coupling in actinide cations

    Bagus, Paul S.; Ilton, Eugene S.; Martin, Richard L.;

    2012-01-01

    The limiting case of Russell–Saunders coupling, which leads to a maximum spin alignment for the open shell electrons, usually explains the properties of high spin ionic crystals with transition metals. For actinide compounds, the spin–orbit splitting is large enough to cause a significantly reduced...

  20. Toxicity ratios: Their use and abuse in predicting the risk from induced cancer

    The toxicity ratio concept assumes the validity of certain relationships. In some examples for bone sarcoma induction, the approximate toxicity of 239Pu in man can be calculated algebraically from the observed toxicity in the radium-dial painters and the ratio of 239Pu/226Ra toxicities in suitable laboratory mammals. In a species highly susceptible to bone sarcoma induction, the risk coefficients for both 239Pu and 226Ra are elevated, but the toxicity ratio of 239Pu to 226Ra tends to be similar to the ratio in resistant species. Among the tested species the toxicity ratio of 239Pu to 226Ra ranged from 6 to 22 (a fourfold range), whereas their relative sensitivities to 239Pu varied by a factor of 150. The toxicity ratio approach can also be used to estimate the actinide risk to man from liver cancer, by comparing to the Thorotrast patients; from lung cancer, by comparing to the uranium miners and the atomic-bomb survivors; and from neutron-induced cancers, by comparing to cancers induced by gamma rays. The toxicity ratio can be used to predict the risk to man from a specific type of cancer that has been reliably induced by a reference radiation in humans and that can be induced by both the reference and the investigated radiation in suitable laboratory animals. 26 refs., 3 figs., 1 tab