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Sample records for 239pu sovmestnaya otsenka

  1. Neutron Capture Cross Section of 239Pu

    Science.gov (United States)

    Mosby, S.; Arnold, C.; Bredeweg, T. A.; Couture, A.; Jandel, M.; O'Donnell, J. M.; Rusev, G.; Ullmann, J. L.; Chyzh, A.; Henderson, R.; Kwan, E.; Wu, C. Y.

    2014-09-01

    The 239Pu(n,γ) cross section has been measured over the energy range 10 eV - 10 keV using the Detector for Advanced Neutron Capture Experiments (DANCE) as part of a campaign to produce precision (n,γ) measurements on 239Pu in the keV region. Fission coincidences were measured with a PPAC and used to characterize the prompt fission γ-ray spectrum in this region. The resulting spectra will be used to better characterize the fission component of another experiment with a thicker target to extend the (n,γ) cross section measurement well into the keV region.

  2. (239)Pu fallout across continental Australia: Implications on (239)Pu use as a soil tracer.

    Science.gov (United States)

    Lal, R; Fifield, L K; Tims, S G; Wasson, R J

    2017-09-19

    At present there is a need for the development of new radioisotopes for soil erosion and sediment tracing especially as fallout (137)Cs levels become depleted. Recent studies have shown that (239)Pu can be a useful new soil erosion and sediment radioisotope tracer. (239)Pu was released in the major atmospheric nuclear weapons tests of 1950's and 1960's. However (239)Pu has a half-life of 24110 years and more than 99% of this isotope is still present in the environment today. In contrast (137)Cs with a half-life of 30.07 year has decayed to atom ratios range from 0.045 to 0.197, with averages of 0.139(0.017), 0.111(0.052) and 0.160(0.027) in the 10-20°S, 20-30°S and 30-40°S latitude bands respectively. The (240)Pu/(239)Pu atom ratios in Central Australia (0.069) likely represent fallout from the Australian tests which also have low (240)Pu/(239)Pu atom ratios i.e., Maralinga (0.113) and Montebello (0.045). The average ratios in the 20-30°S and 30-40° bands are closer to the global average (0.139 and 0.177 respectively when not including the close-in fallout data from the nuclear test sites) if the Australian test sites and Central Australian sites are neglected as they clearly represent the effects of close in fallout. Copyright © 2017 Elsevier Ltd. All rights reserved.

  3. [ECG indices in dogs after inhalation of 239Pu].

    Science.gov (United States)

    Karpova, V N

    1985-11-01

    Dogs of both sexes aged 2 to 4 were subjected to inhalation inoculation with polymer 239Pu or submicron 239PuO2 aerosols in amounts close to acute, subacute and chronically effective ones. ECG was recorded in standard, amplified and single leads (V3). All calculations were done by lead II. Signs of the right heart overburdening were noted in the presence of the P-pulmonale complex, deep S1 wave or cardiac electrical axis of SI-SII-SIII type. Signs of the right heart overburdening were revealed after inhalation of polimer 239Pu (70%). The absence of similar changes in damage caused by 239Pu could be attributed to its fast resorption from the lungs resulting in more moderate lesion of the respiratory organs.

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

    Institute of Scientific and Technical Information of China (English)

    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

  5. Neutron Resonance Parameters and Covariance Matrix of 239Pu

    Energy Technology Data Exchange (ETDEWEB)

    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.

  6. AMS of natural 236U and 239Pu produced in uranium ores

    Science.gov (United States)

    Wilcken, K. M.; Barrows, T. T.; Fifield, L. K.; Tims, S. G.; Steier, P.

    2007-06-01

    The rare isotopes 236U and 239Pu are produced naturally by neutron capture in uranium ores. Here we measure 236U and 239Pu by accelerator mass spectrometry (AMS) in the same ore samples for the first time. To ensure efficient extraction of both elements and isotopic equilibrium between the 239Pu in the ore and a 242Pu spike, we developed a new sample preparation protocol. AMS has clear advantages over previous methods because it achieves better discrimination against molecular interferences with higher sensitivity and shorter counting times. Measurements of 236U and 239Pu hold considerable promise as proxy indicators of neutron flux and uranium concentration.

  7. Gamma-ray Output Spectra from 239Pu Fission

    Directory of Open Access Journals (Sweden)

    Ullmann John

    2015-01-01

    Full Text Available Gamma-ray multiplicities, individual gamma-ray energy spectra, and total gamma energy spectra following neutron-induced fission of 239Pu were measured using the DANCE detector at Los Alamos. Corrections for detector response were made using a forward-modeling technique based on propagating sets of gamma rays generated from a paramaterized model through a GEANT model of the DANCE array and adjusting the parameters for best fit to the measured spectra. The results for the gamma-ray spectrum and multiplicity are in general agreement with previous results, but the measured total gamma-ray energy is about 10% higher. A dependence of the gamma-ray spectrum on the gamma-ray multplicity was also observed. Global model calculations of the multiplicity and gamma energy distributions are in good agreement with the data, but predict a slightly softer total-energy distribution.

  8. A Method for Continuous (239)Pu Determinations in Arctic and Antarctic Ice Cores.

    Science.gov (United States)

    Arienzo, M M; McConnell, J R; Chellman, N; Criscitiello, A S; Curran, M; Fritzsche, D; Kipfstuhl, S; Mulvaney, R; Nolan, M; Opel, T; Sigl, M; Steffensen, J P

    2016-07-05

    Atmospheric nuclear weapons testing (NWT) resulted in the injection of plutonium (Pu) into the atmosphere and subsequent global deposition. We present a new method for continuous semiquantitative measurement of (239)Pu in ice cores, which was used to develop annual records of fallout from NWT in ten ice cores from Greenland and Antarctica. The (239)Pu was measured directly using an inductively coupled plasma-sector field mass spectrometer, thereby reducing analysis time and increasing depth-resolution with respect to previous methods. To validate this method, we compared our one year averaged results to published (239)Pu records and other records of NWT. The (239)Pu profiles from the Arctic ice cores reflected global trends in NWT and were in agreement with discrete Pu profiles from lower latitude ice cores. The (239)Pu measurements in the Antarctic ice cores tracked low latitude NWT, consistent with previously published discrete records from Antarctica. Advantages of the continuous (239)Pu measurement method are (1) reduced sample preparation and analysis time; (2) no requirement for additional ice samples for NWT fallout determinations; (3) measurements are exactly coregistered with all other chemical, elemental, isotopic, and gas measurements from the continuous analytical system; and (4) the long half-life means the (239)Pu record is stable through time.

  9. AMS of natural {sup 236}U and {sup 239}Pu produced in uranium ores

    Energy Technology Data Exchange (ETDEWEB)

    Wilcken, K.M. [Department of Nuclear Physics, RSPhysSE, Australian National University, Canberra, ACT 0200 (Australia)]. E-mail: k.wilcken@suerc.gla.ac.uk; Barrows, T.T. [Department of Nuclear Physics, RSPhysSE, Australian National University, Canberra, ACT 0200 (Australia); Fifield, L.K. [Department of Nuclear Physics, RSPhysSE, Australian National University, Canberra, ACT 0200 (Australia); Tims, S.G. [Department of Nuclear Physics, RSPhysSE, Australian National University, Canberra, ACT 0200 (Australia); Steier, P. [VERA Laboratory, Institute for Isotopic Research and Nuclear Physics, University of Vienna, Waehringer Strasse 17, A-1090 Vienna (Austria)

    2007-06-15

    The rare isotopes {sup 236}U and {sup 239}Pu are produced naturally by neutron capture in uranium ores. Here we measure {sup 236}U and {sup 239}Pu by accelerator mass spectrometry (AMS) in the same ore samples for the first time. To ensure efficient extraction of both elements and isotopic equilibrium between the {sup 239}Pu in the ore and a {sup 242}Pu spike, we developed a new sample preparation protocol. AMS has clear advantages over previous methods because it achieves better discrimination against molecular interferences with higher sensitivity and shorter counting times. Measurements of {sup 236}U and {sup 239}Pu hold considerable promise as proxy indicators of neutron flux and uranium concentration.

  10. Hemodynamics and the parameters of the heart mass in the dog after inhalation of submicron /sup 239/Pu dioxide

    Energy Technology Data Exchange (ETDEWEB)

    Kalmykova, Z.I.; Buldakov, Z.I.; Kharunzhin, V.V.

    The growth of the right heart mass was mainly registered in dogs after inhalation of different quantities of /sup 239/Pu submicron dioxide. This was correlated with the value of /sup 239/Pu deposited in the lungs and associated with the systemic hemodynamic disorders.

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

    Science.gov (United States)

    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. Copyright © 2016 Elsevier Inc. All rights reserved.

  12. Solid Phase Extraction Disk Procedure to Determine 239Pu in Soils

    Directory of Open Access Journals (Sweden)

    ZHANG Ji-qiao;ZHAO Ya-ping;DING You-qian;ZHANG Sheng-dong;YANG Jin-ling

    2016-11-01

    Full Text Available 239Pu in many soil samples should be analyzed to survey radioactive pollution level in nuclear facilities and its affinity environment efficiently. In order to input the opt conditions for column experiment, the experiments of the static adsorption coefficient of 239Pu to solid phase extraction disk with different contact time, concentration of HNO3 and different temperature were carried out. The chemical procedure for the rapid separation and determination of 239Pu in soils had been formulated, which using solid phase extraction disk (EmporeTM Anion Exchange-SR as extraction material and liquid scintillation spectrometry counting as measurement. In the procedure, soil sample usage was 10 g, and were leached by 8 mol/L HNO3, the chemical recovery of the procedure was about 78.9%, and the minimum detectable concentration was 3.7 Bq/kg. It took less than 3 hours once and the presence of 137Cs, 90Sr-90Y and natural uranium, 241Am, 99Tc did not interfere with the procedure, owning high DF of them. The procedure can be used extensively in determination of 239Pu in soils.

  13. Rapid Separation of 239Pu and 241Am in Environment Soil Samples

    Institute of Scientific and Technical Information of China (English)

    YANG; Jin-ling; ZHANG; Ji-qiao; HUANG; Kun; DING; You-qian; ZHAO; Ya-ping

    2015-01-01

    In the nuclear sites and the surroundings which are the main environmental monitored area,the allowances of 239Pu and 241 Am are less than0.1Bq/g as the extremely toxic species.So it is very important and practical to establish rapid and convenient analysis methods for them.With

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

    Institute of Scientific and Technical Information of China (English)

    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

  15. Nucleogenic {sup 36}Cl, {sup 236}U and {sup 239}Pu in uranium ores

    Energy Technology Data Exchange (ETDEWEB)

    Wilcken, K.M. [Department of Nuclear Physics, RSPhysSE, Australian National University, Canberra, ACT 0200 (Australia); Scottish Universities Environmental Research Centre, Scottish Enterprise Technology Park, Rankine Avenue, East Kilbride G75 0QF (United Kingdom)], E-mail: K.Wilcken@suerc.gla.ac.uk; Fifield, L.K.; Barrows, T.T.; Tims, S.G.; Gladkis, L.G. [Department of Nuclear Physics, RSPhysSE, Australian National University, Canberra, ACT 0200 (Australia)

    2008-08-15

    The nucleogenic isotopes {sup 36}Cl, {sup 236}U and {sup 239}Pu are produced naturally in subsurface environments via neutron capture of thermal and epithermal neutrons. Concentrations are, however, very low and accelerator mass spectrometry (AMS) is required for quantitative measurements. A particular challenge is presented by the measurement of {sup 236}U/{sup 238}U ratios down to the level of 10{sup -13} that is expected from rocks with low uranium concentration. Here, we present the AMS methodology that has been developed at the ANU for measuring {sup 236}U/{sup 238}U ratios at this level. The more established methodologies for {sup 36}Cl and {sup 239}Pu measurements are also summarised. These capabilities are then used to characterize the {sup 36}Cl, {sup 236}U and {sup 239}Pu concentrations in a range of uranium ores. A simple model of the neutron production and capture processes in subsurface environments has been developed and is presented. It is shown that nucleogenic {sup 36}Cl, {sup 236}U and {sup 239}Pu can be used to determine both thermal and epithermal neutron fluxes in subsurface environments. Potential applications include uranium exploration and monitoring of the environmental impact of uranium mining.

  16. Nucleogenic 36Cl, 236U and 239Pu in uranium ores

    Science.gov (United States)

    Wilcken, K. M.; Fifield, L. K.; Barrows, T. T.; Tims, S. G.; Gladkis, L. G.

    2008-08-01

    The nucleogenic isotopes 36Cl, 236U and 239Pu are produced naturally in subsurface environments via neutron capture of thermal and epithermal neutrons. Concentrations are, however, very low and accelerator mass spectrometry (AMS) is required for quantitative measurements. A particular challenge is presented by the measurement of 236U/ 238U ratios down to the level of 10 -13 that is expected from rocks with low uranium concentration. Here, we present the AMS methodology that has been developed at the ANU for measuring 236U/ 238U ratios at this level. The more established methodologies for 36Cl and 239Pu measurements are also summarised. These capabilities are then used to characterize the 36Cl, 236U and 239Pu concentrations in a range of uranium ores. A simple model of the neutron production and capture processes in subsurface environments has been developed and is presented. It is shown that nucleogenic 36Cl, 236U and 239Pu can be used to determine both thermal and epithermal neutron fluxes in subsurface environments. Potential applications include uranium exploration and monitoring of the environmental impact of uranium mining.

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

    Energy Technology Data Exchange (ETDEWEB)

    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)

  18. Dependence of dose coefficients for inhaled 239Pu on absorption parameters.

    Science.gov (United States)

    Suzuki, K; Sekimoto, H; Ishigure, N

    2001-01-01

    With regard to dissolution of particles in the respiratory tract after inhalation, the International Commission on Radiological Protection (ICRP) has classified all radionuclides into only three types according to the chemical form of compounds, and default values of absorption parameters are proposed for each type. However, it is just a simplification to estimate doses for practical use, and there is a possibility of unfitness in such an assortment. A code has been developed to reproduce the ICRP's dose coefficients for 239Pu, which is one of the most important elements for occupational exposure. By using this code, the respective absorption parameters were modified, and the effect owing to these changes evaluated. It was shown consequently that changes of absorption parameters do not greatly influence the effective doses of 239Pu for workers.

  19. Prompt γ-ray production in neutron-induced fission of 239Pu

    Science.gov (United States)

    Ullmann, J. L.; Bond, E. M.; Bredeweg, T. A.; Couture, A.; Haight, R. C.; Jandel, M.; Kawano, T.; Lee, H. Y.; O'Donnell, J. M.; Hayes, A. C.; Stetcu, I.; Taddeucci, T. N.; Talou, P.; Vieira, D. J.; Wilhelmy, J. B.; Becker, J. A.; Chyzh, A.; Gostic, J.; Henderson, R.; Kwan, E.; Wu, C. Y.

    2013-04-01

    Background: The prompt gamma-ray spectrum from fission is important for understanding the physics of nuclear fission, and also in applications involving fission. Relatively few measurements of the prompt gamma spectrum from 239Pu(n,f) have been published.Purpose: This experiment measured the multiplicity, individual gamma energy spectrum, and total gamma energy spectrum of prompt fission gamma rays from 239Pu(n,f) in the neutron energy range from thermal to 30 keV, to test models of fission and to provide information for applications.Method: Gamma rays from neutron-induced fission of 239Pu were measured using the DANCE gamma-ray calorimeter. Fission events were tagged by detecting fission products in a parallel-plate avalanche counter in the center of DANCE. The measurements were corrected for detector response using a geant4 model of DANCE. A detailed analysis for the gamma rays from the 1+ resonance complex at 10.93 eV is presented.Results: A six-parameter analytical parametrization of the fission gamma-ray spectrum was obtained. A Monte Carlo Hauser-Feshbach calculation provided good general agreement with the data, but some differences remain to be resolved.Conclusions: An analytic parametrization can be made of the gamma-ray multiplicity, energy distribution, and total-energy distribution for the prompt gamma rays following neutron-induced fission of 239Pu. This parametrization may be useful for applications. Modern Monte Carlo Hauser-Feshbach calculations can do a good job of calculating the fission gamma-ray emission spectrum, although some details remain to be understood.

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

    Energy Technology Data Exchange (ETDEWEB)

    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.

  1. Transuranic advanced disposal systems: preliminary /sup 239/Pu waste-disposal criteria for Hanford

    Energy Technology Data Exchange (ETDEWEB)

    Kennedy, W.E. Jr.; Aaberg, R.L.; Napier, B.A.; Soldat, J.K.

    1982-09-01

    This report contains the draft results of a study sponsored by the US Department of Energy (DOE) to determine preliminary /sup 239/Pu waste disposal criteria for the Hanford Site. The purpose of this study is to provide a preliminary evaluation of the feasibility of various defense TRU advanced disposal options at the Hanford Site. Advanced waste disposal options include those developed to provide greater confinement than provided by shallow-land burial. They will be used to complement the waste geologic disposal in achieving permanent disposal of selected TRU wastes. An example systems analysis is discussed with assumed performance objectives and Hanford-specific disposal conditions, waste forms, site characteristics, and engineered barriers. Preliminary waste disposal criteria for /sup 239/Pu are determined by applying the Allowable Residual Contamination Level (ARCL) method. This method is based on compliance with a radiation dose rate limit through a site-specific analysis of the potential for radiation exposure to individuals. A 10,000-year environmental performance period is assumed, and the dose rate limit for human intrusion is assumed to be 500 mrem/yr to any exposed individual. Preliminary waste disposal criteria derived by this method for /sup 239/Pu in soils at the Hanford Site are: 0.5 nCi/g in soils between the surface and a depth of 1 m, 2200 nCi/g of soil at a depth of 5 m, and 10,000 nCi/g of soil at depths 10 m and below. These waste disposal criteria are based on exposure scenarios that reflect the dependence of exposure versus burial depth. 5 figures, 7 tables.

  2. European roe deer antlers as an environmental archive for fallout (236)U and (239)Pu.

    Science.gov (United States)

    Froehlich, M B; Steier, P; Wallner, G; Fifield, L K

    2016-01-01

    Anthropogenic (236)U and (239)Pu were measured in European roe deer antlers hunted between 1955 and 1977 which covers and extends beyond the period of intensive nuclear weapons testing (1954-1962). The antlers were hunting trophies, and hence the hunting area, the year of shooting and the approximate age of each animal is given. Uranium and plutonium are known to deposit in skeletal tissue. Since antler histology is similar to bone, both elements were expected in antlers. Furthermore, roe deer shed their antlers annually, and hence antlers may provide a time-resolved environmental archive for fallout radionuclides. The radiochemical procedure is based on a Pu separation step by anion exchange (Dowex 1 × 8) and a subsequent U purification by extraction chromatography using UTEVA(®). The samples were measured by Accelerator Mass Spectrometry at the VERA facility (University of Vienna). In addition to the (236)U and (239)Pu concentrations, the (240)Pu/(239)Pu isotopic ratios were determined with a mean value of 0.172 ± 0.023 which is in agreement with the ratio of global fallout (∼0.18). Rather high (236)U/(238)U ratios of the order of 10(-6) were observed. These measured ratios, where the (236)U arises only from global fallout, have implications for the use of the (236)U/(238)U ratio as a fingerprint for nuclear accidents or releases from nuclear facilities. Our investigations have shown the potential to use antlers as a temporally resolved archive for the uptake of actinides from the environment.

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

    Energy Technology Data Exchange (ETDEWEB)

    G. Palmiottti; H. Hiruta; M. Salvatores

    2011-09-01

    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 {sup 235}U, {sup 238}U, and {sup 239}Pu. 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: {sup 235}U and {sup 239}Pu. 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 K{sub eff} 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.

  4. Transuranic advanced disposal systems: preliminary /sup 239/Pu waste-disposal criteria for Hanford

    Energy Technology Data Exchange (ETDEWEB)

    Kennedy, W.E. Jr.; Napier, B.A.; Soldat, J.K.

    1982-08-01

    An evaluation of the feasibility and potential application of advanced disposal systems is being conducted for defense transuranic (TRU) wastes at the Hanford Site. The advanced waste disposal options include those developed to provide greater confinement than provided by shallow-land burial. An example systems analysis is discussed with assumed performance objectives and various Hanford-specific disposal conditions, waste forms, site characteristics, and engineered barriers. Preliminary waste disposal criteria for /sup 239/Pu are determined by applying the Allowable Residual Contamination Level (ARCL) method. This method is based on compliance with a radiation dose rate limit through a site-specific analysis of the potential for radiation exposure to individuals. A 10,000 year environmental performance period is assumed, and the dose rate limit for human intrusion is assumed to be 500 mrem/y to any exposed individual. Preliminary waste disposal criteria derived by this method for /sup 239/Pu in soils at the Hanford Site are: 0.5 nCi/g in soils between the surface and a depth of 1 m, 2200 nCi/g of soil at a depth of 5 m, and 10,000 nCi/g of soil at depths 10 m and below. These waste disposal criteria are based on exposure scenarios that reflect the dependence of exposure versus burial depth. 2 figures, 5 tables.

  5. 239Pu(n,2n) 238Pu cross section inferred from IDA calculations and GEANIE measurements

    Energy Technology Data Exchange (ETDEWEB)

    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.

  6. Investigation of zircon/zirconia ceramics doped with {sup 239}Pu and {sup 238}Pu

    Energy Technology Data Exchange (ETDEWEB)

    Burakov, B.E.; Anderson, E.B.; Zamoryanskaya, M.V.; Nikolaeva, E.V.; Strykanova, E.E.; Yagovkina, M.A. [V.G. Khlopin Radium Institute, Saint Petersburg (Russian Federation)

    2001-07-01

    Several samples of crystalline double-phase ceramics based on zircon, (Zr,Pu)SiO{sub 4} and zirconia, (Zr,Pu)O{sub 2}, were synthesized by sintering in air, precursors containing approximately 5-6 and 10 wt% {sup 239}Pu, respectively. One sample doped with 5-6 wt% {sup 238-39-40}Pu was also obtained under the same conditions. All ceramic samples were studied by X-ray powder diffraction (XRD), scanning electron microscopy (SEM), electron probe microanalysis (EPMA) and MCC-1 leach test in deionized water at 90 C. Results indicate that even radiation damaged zircon/zirconia ceramics retain high chemical resistance and mechanical durability. (author)

  7. Characterization of a {sup 239}PuBe isotopic neutron source

    Energy Technology Data Exchange (ETDEWEB)

    Vega C, H. R.; Hernandez D, V. M. [Universidad Autonoma de Zacatecas, Unidad Academica de Estudios Nucleares, Cipres No. 10, Fracc. La Penuela, 98068 Zacatecas (Mexico); Rivera M, T. [IPN, Centro de Investigacion en Ciencia Aplicada y Tecnologia Avanzada, Calz. Legaria No. 694, Col. Irrigacion, 11500 Mexico D. F. (Mexico); Sanchez, A., E-mail: fermineutron@yahoo.com [IPN, Escuela Superior de Fisica y Matematicas, 07738 Mexico D. F. (Mexico)

    2012-10-15

    A Bonner sphere spectrometer was used to determine the features of a {sup 239}PuBe neutron source used to operate the ESFM-Ipn Subcritical Reactor. The spectrometer is a {sup 6}Lil(Eu) scintillator and 2, 3, 5, 8, 10 and 12 inches-diameter polyethylene spheres, that was located 100 cm from the neutron source. The count rates obtained with the spectrometer were unfolded using the NSDUAZ code and neutron spectrum, total fluence, and ambient dose equivalent were determined. A Monte Carlo calculation, using the MCNP5 code, was carried out to estimate the spectrum and integral features being less that values obtained experimentally due to the presence of {sup 241}Pu in the Pu used to fabricate the source. Using the experimental information the actual neutron yield and the mass fraction of {sup 241}Pu was estimated. (Author)

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

    Energy Technology Data Exchange (ETDEWEB)

    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.

  9. Dependence of dose coefficients for {sup 239}Pu on transfer rates and absorption parameters

    Energy Technology Data Exchange (ETDEWEB)

    Suzuki, K.; Sekimoto, H. [Research Laboratory for Nuclear Reactors, Tokyo Institute of Technology, Tokyo (Japan); Ishigure, N. [Division of Radiotoxicology and Protection, National Institute of Radiological Sciences, Chiba (Japan)

    2000-05-01

    As it is reported of the biokinetic models and parameter values of the International Commission on Radiological Protection (ICRP) for dose estimation have uncertainties owing to insufficiency of human data. For most radionuclides, the data underlying such models and parameters of ICRP usually depend on animal experiments. Moreover, these values or model parameter are also greatly different between mammalian species. Recently, various radiation protection organizations are considering the biokinetic uncertainties from standpoints of data's sources, quality and completeness. In practice, a sensitivity analysis of doses to parameters is significant for the purpose of risk assessment. In general, movement or material in the body is depicted as a system of first-order processes, and parameter values are expressed as transfer rates between compartments. In this study, we made a code to reproduce the ICRP's dose coefficients for {sup 239}Pu, which is one of the most important elements for occupational exposure and its effective dose is much concerned with its own distribution in the body for dominance of alpha-decay. By using this code, we modified each transfer rate in a factor of 2, 3 and 4 in order to evaluate the effects, and calculated the sensitivities of effective doses due to these changes. Additionally, we examined the effects of modification of absorption parameters f{sub r}, S{sub r} and S{sub s}, which represent the absorption of particles from respiratory tract into blood. Consequently, the transfer rates that give a large sensitivity were specified, and it was shown that changes of transfer rates and absorption parameters are not so influential on effective doses for {sup 239}Pu in many cases. (author)

  10. 239Pu Prompt Fission Neutron Spectra Impact on a Set of Criticality and Experimental Reactor Benchmarks

    Science.gov (United States)

    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

  11. Using 239Pu as a tracer for fine sediment sources in the Daly River, Northern Australia

    Science.gov (United States)

    Lal, R.; Fifield, L. K.; Tims, S. G.; Wasson, R. J.; Howe, D.

    2015-04-01

    The Daly River drains a large (52500 km2) and mainly undisturbed catchment in the Australian wet-dry tropics. Clearing and cropping since 2002 have raised concerns about possible increased sediment input into the river and motivated this study of its fine sediment sources. Using 239Pu as a tracer it is shown that the fine sediments originate mainly from erosion by gullying and channel change. Although the results also indicate that the surface soil contribution to the river channel sediments from sheet erosion has increased to 5-22% for the Daly River and 7-28% for the Douglas River (a tributary of the Daly River) in 2009 vs. 3-6% for the Daly River and 4-9% for the Douglas River in 2005. This excess top soil likely originates from thecleared land adjacent to the Daly River since 2005. However, channel widening largely as a result of hydrologic change is still the dominant sediment source in this catchment.

  12. Using 239Pu as a tracer for fine sediment sources in the Daly River, Northern Australia

    Directory of Open Access Journals (Sweden)

    Lal R.

    2015-01-01

    Full Text Available The Daly River drains a large (52500 km2 and mainly undisturbed catchment in the Australian wet–dry tropics. Clearing and cropping since 2002 have raised concerns about possible increased sediment input into the river and motivated this study of its fine sediment sources. Using 239Pu as a tracer it is shown that the fine sediments originate mainly from erosion by gullying and channel change. Although the results also indicate that the surface soil contribution to the river channel sediments from sheet erosion has increased to 5-22% for the Daly River and 7-28% for the Douglas River (a tributary of the Daly River in 2009 vs. 3-6% for the Daly River and 4-9% for the Douglas River in 2005. This excess top soil likely originates from thecleared land adjacent to the Daly River since 2005. However, channel widening largely as a result of hydrologic change is still the dominant sediment source in this catchment.

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

    Science.gov (United States)

    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.

  14. An examination of the potential fission-bomb weaponizability of nuclides other than 235U and 239Pu

    Science.gov (United States)

    Reed, B. Cameron

    2017-01-01

    Long-lived fissionable isotopes other than uranium-235 and plutonium-239 are examined for possible use in fission weapons. A few other isotopes are potentially weaponizable and in some cases have been tried or their criticality experimentally demonstrated. In most cases, however, promising isotopes are either extremely rare, difficult to produce in quantity, or hazardous to handle. Some isotopes can serve to boost the yield of fission weapons, but 235U and 239Pu are likely to remain the only practical primary fuels for nuclear weapons. In view of this, and the fact that this analysis gives no engineering details on the design of nuclear weapons, this paper will be of no assistance to putative bomb-makers; rather, my purpose is to clarify the physics similarities between 235U and 239Pu that make them suitable candidates for fission weapons.

  15. Probing energy dissipation, γ-ray and neutron multiplicity in the thermal neutron-induced fission of {sup 239}Pu

    Energy Technology Data Exchange (ETDEWEB)

    Pahlavani, M.R.; Mirfathi, S.M. [University of Mazandaran, Department of Nuclear Physics, Faculty of Basic Science, Babolsar (Iran, Islamic Republic of)

    2016-04-15

    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 {sup 239}Pu. The dynamical approach presented in this paper thoroughly reproduces several experimental observables of the fission process at low excitation energy. (orig.)

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

    Energy Technology Data Exchange (ETDEWEB)

    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)

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

    Science.gov (United States)

    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.

  18. Analysis of plutonium isotope ratios including (238)Pu/(239)Pu in individual U-Pu mixed oxide particles by means of a combination of alpha spectrometry and ICP-MS.

    Science.gov (United States)

    Esaka, Fumitaka; Yasuda, Kenichiro; Suzuki, Daisuke; Miyamoto, Yutaka; Magara, Masaaki

    2017-04-01

    Isotope ratio analysis of individual uranium-plutonium (U-Pu) mixed oxide particles contained within environmental samples taken from nuclear facilities is proving to be increasingly important in the field of nuclear safeguards. However, isobaric interferences, such as (238)U with (238)Pu and (241)Am with (241)Pu, make it difficult to determine plutonium isotope ratios in mass spectrometric measurements. In the present study, the isotope ratios of (238)Pu/(239)Pu, (240)Pu/(239)Pu, (241)Pu/(239)Pu, and (242)Pu/(239)Pu were measured for individual Pu and U-Pu mixed oxide particles by a combination of alpha spectrometry and inductively coupled plasma mass spectrometry (ICP-MS). As a consequence, we were able to determine the (240)Pu/(239)Pu, (241)Pu/(239)Pu, and (242)Pu/(239)Pu isotope ratios with ICP-MS after particle dissolution and chemical separation of plutonium with UTEVA resins. Furthermore, (238)Pu/(239)Pu isotope ratios were able to be calculated by using both the (238)Pu/((239)Pu+(240)Pu) activity ratios that had been measured through alpha spectrometry and the (240)Pu/(239)Pu isotope ratios determined through ICP-MS. Therefore, the combined use of alpha spectrometry and ICP-MS is useful in determining plutonium isotope ratios, including (238)Pu/(239)Pu, in individual U-Pu mixed oxide particles. Copyright © 2016 Elsevier B.V. All rights reserved.

  19. Use of fission track analysis technique for the determination of MicroBequerel level of 239Pu in urine samples from radiation workers handling MOX fuel.

    Science.gov (United States)

    Yadav, J R; Rao, D D; Kumar, Ranjeet; Aggarwal, S K

    2011-07-01

    Fission track analysis (FTA) technique for the determination of (239)Pu excreted through urine has been standardized using blank samples, tracer and (239)Pu spikes. Double stage anion exchange separation protocol has been applied and an average radiochemical recovery of (239)Pu of 18% was obtained. An average track registration efficiency of 11 tracks per μBq of (239)Pu, irradiated to 0.35×10(17) neutron fluence was established. Reagent blank urine samples from 11 controlled subjects were analyzed by FTA and an average of 149±14 tracks was obtained. Minimum detectable activity of 34μBqL(-1) of urine sample was obtained and will be useful for monitoring chronic exposure cases handling MOX fuel.

  20. Commentary on inhaled {sup 239}PuO{sub 2} in dogs - a prophylaxis against lung cancer?

    Energy Technology Data Exchange (ETDEWEB)

    Cuttler, J.M. [Cuttler and Assoc., Vaughan, Ontario (Canada); Feinendegen, L. [Brookhaven National Laboratories, Upton, New York (United States)

    2015-06-15

    Several studies on the effect of inhaled plutonium-dioxide particulates and the incidence of lung tumors in dogs reveal beneficial effects when the cumulative alpha-radiation dose is low. There is a threshold at an exposure level of about 100 cGy for excess tumor incidence and reduced lifespan. The observations conform to the expectations of the radiation hormesis dose-response model and contradict the predictions of the Linear No-Threshold (LNT) hypothesis. These studies suggest investigating the possibility of employing low-dose alpha-radiation, such as from {sup 239}PuO {sub 2} inhalation, as a prophylaxis against lung cancer. (author)

  1. Reactor Decay Heat in 239Pu: Solving the Gamma Discrepancy in the 4–3000-s Cooling Period

    Energy Technology Data Exchange (ETDEWEB)

    Algora, A.; Sonzogni, A.; Algora,A.; Jordan,D.; Tain,J.L.; Rubio,B.; Agramunt,J.; Perez-Cerdan,A.B.; Molina,F; Caballero,L.; Nacher,E.; Krasznahorkay,A.; Hunyadi,M.D.; Gulyas,J; Vitez,A.; Csatlos,M.; Csige,L.; Aysto,J.; Penttila,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.; Huller,W.; Batist,L.; Gelletly,W.; Nichols,A.L.; Yoshida,T.; Sonzogni,A.A.; Perajarvi,K.

    2010-11-08

    The {beta} feeding probability of {sup 102,104,105,106,107}Tc, {sup 105}Mo, and {sup 101}Nb 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 {gamma} component of the decay heat for {sup 239}Pu in the 4-3000 s range.

  2. A generalized method for characterization of 235U and 239Pu content using short-lived fission product gamma spectroscopy

    Science.gov (United States)

    Knowles, Justin; Skutnik, Steven; Glasgow, David; Kapsimalis, Roger

    2016-10-01

    Rapid nondestructive assay methods for trace fissile material analysis are needed in both nuclear forensics and safeguards communities. To address these needs, research at the Oak Ridge National Laboratory High Flux Isotope Reactor Neutron Activation Analysis facility has developed a generalized nondestructive assay method to characterize materials containing fissile isotopes. This method relies on gamma-ray emissions from short-lived fission products and makes use of differences in fission product yields to identify fissile compositions of trace material samples. Although prior work has explored the use of short-lived fission product gamma-ray measurements, the proposed method is the first to provide a complete characterization of isotopic identification, mass ratios, and absolute mass determination. Successful single fissile isotope mass recoveries of less than 6% recovery bias have been conducted on standards of 235U and 239Pu as low as 12 ng in less than 10 minutes. Additionally, mixtures of fissile isotope standards containing 235U and 239Pu have been characterized as low as 198 ng of fissile mass with less than 7% recovery bias. The generalizability of this method is illustrated by evaluating different fissile isotopes, mixtures of fissile isotopes, and two different irradiation positions in the reactor. It is anticipated that this method will be expanded to characterize additional fissile nuclides, utilize various irradiation facilities, and account for increasingly complex sample matrices.

  3. Fission Product Yields of 233U, 235U, 238U and 239Pu in Fields of Thermal Neutrons, Fission Neutrons and 14.7-MeV Neutrons

    Science.gov (United States)

    Laurec, J.; Adam, A.; de Bruyne, T.; Bauge, E.; Granier, T.; Aupiais, J.; Bersillon, O.; Le Petit, G.; Authier, N.; Casoli, P.

    2010-12-01

    The yields of more than fifteen fission products have been carefully measured using radiochemical techniques, for 235U(n,f), 239Pu(n,f) in a thermal spectrum, for 233U(n,f), 235U(n,f), and 239Pu(n,f) reactions in a fission neutron spectrum, and for 233U(n,f), 235U(n,f), 238U(n,f), and 239Pu(n,f) for 14.7 MeV monoenergetic neutrons. Irradiations were performed at the EL3 reactor, at the Caliban and Prospero critical assemblies, and at the Lancelot electrostatic accelerator in CEA-Valduc. Fissions were counted in thin deposits using fission ionization chambers. The number of fission products of each species were measured by gamma spectrometry of co-located thick deposits.

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

    Science.gov (United States)

    Srncik, M; Tims, S G; De Cesare, M; Fifield, L K

    2014-06-01

    The variation of the (236)U and (239)Pu 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 (236)U and (239)Pu as well as the (236)U/(239)Pu 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 (236)U and (239)Pu were found at a depth of 2-3 cm. The (236)U/(239)Pu isotopic ratio in fallout at this site, as deduced from the ratio of the (236)U and (239)Pu inventories, is 0.085 ± 0.003 which is clearly lower than the Northern Hemisphere value of ∼0.2. The (236)U inventory of (8.4 ± 0.3) × 10(11) at/m(2) was more than an order of magnitude lower than values reported for the Northern Hemisphere. The (239)Pu activity concentrations are in excellent agreement with a previous study and the (239+240)Pu inventory was (13.85 ± 0.29) Bq/m(2). The weighted mean (240)Pu/(239)Pu 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).

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

    Energy Technology Data Exchange (ETDEWEB)

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

    2016-09-01

    A technique to determine the isotopics of a mixed actinide sample has been proposed by measuring the coincidence of the alpha particle during radioactive decay with the conversion electron (or Auger) emitted during the relaxation of the daughter isotope. This presents a unique signature to allow the deconvolution of isotopes that possess overlapping alpha particle energy. 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. A passivated ion implanted planar silicon detector provided measurements of alpha spectroscopy. 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 to aid in the coincident measurement approach.

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

    Directory of Open Access Journals (Sweden)

    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.

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

    CERN Document Server

    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...

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

    Science.gov (United States)

    Neudecker, D.; Talou, P.; Kawano, T.; Kahler, A. C.; Rising, M. E.; White, M. C.

    2016-03-01

    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.

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

    Science.gov (United States)

    Lal, R.; Tims, S. G.; Fifield, L. K.; Wasson, R. J.; Howe, D.

    2013-01-01

    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 (soil loss rates over the past ∼50 years were 7.5-19.5 t ha-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. Applicability of {sup 239}Pu as a tracer for soil erosion in the wet-dry tropics of northern Australia

    Energy Technology Data Exchange (ETDEWEB)

    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.

  11. Fission Product Yield Study of 235U, 238U and 239Pu Using Dual-Fission Ionization Chambers

    Science.gov (United States)

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

    2014-05-01

    To resolve long-standing differences between LANL and LLNL regarding the correct fission basis for analysis of nuclear test data [M.B. Chadwick et al., Nucl. Data Sheets 111, 2891 (2010); H. Selby et al., Nucl. Data Sheets 111, 2891 (2010)], a collaboration between TUNL/LANL/LLNL has been established to perform high-precision measurements of neutron induced fission product yields. The main goal is to make a definitive statement about the energy dependence of the fission yields to an accuracy better than 2-3% between 1 and 15 MeV, where experimental data are very scarce. At TUNL, we have completed the design, fabrication and testing of three dual-fission chambers dedicated to 235U, 238U, and 239Pu. The dual-fission chambers were used to make measurements of the fission product activity relative to the total fission rate, as well as for high-precision absolute fission yield measurements. The activation method was employed, utilizing the mono-energetic neutron beams available at TUNL. Neutrons of 4.6, 9.0, and 14.5 MeV were produced via the 2H(d,n)3He reaction, and for neutrons at 14.8 MeV, the 3H(d,n)4He reaction was used. After activation, the induced γ-ray activity of the fission products was measured for two months using high-resolution HPGe detectors in a low-background environment. Results for the yield of seven fission fragments of 235U, 238U, and 239Pu and a comparison to available data at other energies are reported. For the first time results are available for neutron energies between 2 and 14 MeV.

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

    Energy Technology Data Exchange (ETDEWEB)

    Mitchell, P.I.; Vintro, L.L. [University Coll., Dublin (Ireland). Dept. of Physics; Dahlgaard, H. [Risoe National Lab., Roskilde (Denmark); Gasco, C.; Sanchez-Cabeza, J.A. [Barcelona Univ. (Spain). Dept. de Fisica Teorica

    1995-12-31

    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 {sup 240}Pu/{sup 239}Pu atom ratio of {approx}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 {sup 240}Pu/{sup 239}Pu 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 {sup 240}Pu/{sup 239}Pu ratio was measured by high-resolution alpha spectrometry and spectral deconvolution. The analytical results showed that at Thule the mean {sup 240}Pu/{sup 239}Pu 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.

  13. Short-Lived Fission Products Yield Measurement for 239pu(nth ,f)%239Pu(nth,f)短寿命裂变产物产额测量

    Institute of Scientific and Technical Information of China (English)

    刘世龙; 杨毅; 冯晶

    2012-01-01

    采用γ能谱相对测量方法,以97Zr为内标参考核素,完成了239Pu( nth,f)短寿命裂变产物88Rb、95Y、101Mo、101Tc、…Csg、142 La等核素的累积产额测量.实验测得88Rb、”Y、101Mo、101Tc、38Csg、142La的累积产额数据分别为(1.32±0.05)%、(4.69±0.22)%、(6.13±0.32)%、(6.10土0.22)%、(6.24±0.24)%、(4.74±o.17)%.对高纯锗探测器中高能端效率刻度、样品封装与辐照、γ谱测量几何条件设计、γ谱测量与数据分析进行了研究.实验测量裂变产物核素分别位于非对称裂变质量分布双驼峰曲线轻峰的左侧、中部和右侧,重峰的中部与右侧.%The cumulative fission yields of short-lived nuclides 88Rb, 95Y, 101Mo, 101Tc, 119 Cs81 and 14!La in thermal neutron induced fission of 230Pu have been determined by gamma-ray spectrometry relative method. "Zr is selected as the reference nuclide. The determined cumulative fission yields are given as following: the Y(88Rb) = (1. 32 + 0. 05) %, Y(95Y) = (4.69 + 0.22)%, Y(101Mo) = (6. 13 + 0. 32 )%, Y(10'Tc)= (6.10 + 0.22)%, Y(I38Cse) = (6. 24 + 0. 24)%, Y(14ELa) = (4. 74 + 0. 17)%. The major work include HPGe detector efficiency calibration, sample sealing and irradiation, gamma-ray measurement and data analysis. The determined nuclides are located in left, middle, right of light group, and in middle, right of heavy group for asymmetric fission model. The accurate yields data supply a gap for domestic nuclear database, and reflect the fission products mass distribution character in thermal neutron induced fission of 239Pu.

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

    Science.gov (United States)

    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.

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

    Science.gov (United States)

    Montoya, M.; Rojas, J.; Lobato, I.

    2010-08-01

    The average of fragment kinetic energy (E*) and the multiplicity of prompt neutrons (ν) 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.

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

    Science.gov (United States)

    Zavorka, L.; Adam, J.; Baldin, A. A.; Caloun, P.; Chilap, V. V.; Furman, W. I.; Kadykov, M. G.; Khushvaktov, J.; Pronskikh, V. S.; Solnyshkin, A. A.; Sotnikov, V.; Stegailov, V. I.; Suchopar, M.; Tsoupko-Sitnikov, V. M.; Tyutyunnikov, S. I.; Voronko, V.; Vrzalova, J.

    2015-04-01

    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.

  17. Photofission product yields of {sup 238}U and {sup 239}Pu with 22-MeV bremsstrahlung

    Energy Technology Data Exchange (ETDEWEB)

    Wen, Xianfei; Yang, Haori, E-mail: haori.yang@oregonstate.edu

    2016-06-11

    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 {sup 238}U 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 {sup 238}U and {sup 239}Pu 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.

  18. Photo-fission Product Yield Measurements at Eγ=13 MeV on 235U, 238U, and 239Pu

    Science.gov (United States)

    Tornow, W.; Bhike, M.; Finch, S. W.; Krishichayan, Fnu; Tonchev, A. P.

    2016-09-01

    We have measured Fission Product Yields (FPYs) in photo-fission of 235U, 238U, and 239Pu at TUNL's High-Intensity Gamma-ray Source (HI γS) using mono-energetic photons of Eγ = 13 MeV. Details of the experimental setup and analysis procedures will be discussed. Yields for approximately 20 fission products were determined. They are compared to neutron-induced FPYs of the same actinides at the equivalent excitation energies of the compound nuclear systems. In the future photo-fission data will be taken at Eγ = 8 . 0 and 10.5 MeV to find out whether photo-fission exhibits the same so far unexplained dependence of certain FPYs on the energy of the incident probe, as recently observed in neutron-induced fission, for example, for the important fission product 147Nd. Work supported by the U. S. Dept. of Energy, under Grant No. DE-FG02-97ER41033, and by the NNSA, Stewardship Science Academic Alliances Program, Grant No. DE-NA0001838 and the Lawrence Livermore, National Security, LLC under Contract No. DE-AC52-07NA27344.

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

    Directory of Open Access Journals (Sweden)

    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.

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

    Science.gov (United States)

    Bu, Kaixuan; Cizdziel, James V; Dasher, Douglas

    2013-10-01

    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 (239)Pu and (240)Pu concentration and (240)Pu/(239)Pu atom ratio using inductively coupled plasma sector field mass spectrometry (ICP-SFMS). Plutonium concentrations and (240)Pu/(239)Pu atom ratios were generally consistent with previous terrestrial and marine studies in the region. The ((239)+)(240)Pu 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 (240)Pu/(239)Pu atom ratios were significantly higher in marine samples compared to terrestrial and freshwater samples (t-test, p Pu occurred into the North Pacific Ocean, likely from the Marshall Island high yield nuclear tests, but other potential sources, such as the Kamchatka Peninsula Rybachiy Naval Base and Amchitka Island underground nuclear test site cannot be ruled out.

  1. Reassessment of 239Pu on planchets from human urine samples at ultra-trace levels using Aridus-ICPSFMS and AMS.

    Science.gov (United States)

    Hernández-Mendoza, Héctor; Chamizo, Elena; Delgado, Antonio; García-León, Manuel; Yllera, Abel

    2012-12-01

    New analytical methods developed at the facilities here, based on two ultra-sensitive mass spectrometry (MS) techniques, inductively coupled plasma sector field mass spectrometer with a desolvator system (Aridus-ICP-SFMS) and accelerator MS (AMS), have been applied in this work for the reassessment of (239)Pu in alpha spectrometry (AS) planchets corresponding to spiked human urine samples. The obtained (239)Pu minimum detectable activities (MDAs) values by Aridus-ICP-SFMS and AMS were 3 fg (∼6.92 µBq) and 0.4 fg (∼0.92 µBq), respectively, per sample, which are much better than those attainable by AS [50 fg (∼115.3 µBq) of (239)Pu per sample, approximately]. Therefore, it is demonstrated that the MS techniques employed in this work are very powerful tools for internal dosimetry studies in human urine samples, giving excellent results when the reassessment of AS planchets is needed (samples with a Pu concentration below or at the MDA levels measurable by AS). This work is the continuation of an article published in J. Anal. At. Spectrom. 25 (1410-1415) 2010.

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

    Science.gov (United States)

    Xu, Yihong; Qiao, Jixin; Hou, Xiaolin; Pan, Shaoming; Roos, Per

    2014-02-01

    This paper reports an analytical method for the determination of plutonium isotopes ((238)Pu, (239)Pu, (240)Pu, (241)Pu) 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 × 10(5) 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 values, revealing that the developed method for plutonium determination in environmental samples is reliable. The measurement results of (239+240)Pu by alpha spectrometry agreed very well with the sum of (239)Pu and (240)Pu measured by ICP-MS. ICP-MS can not only measure (239)Pu and (240)Pu separately but also (241)Pu. However, it is impossible to measure (238)Pu using ICP-MS in environmental samples even a decontamination factor as high as 10(6) for uranium was obtained by chemical separation.

  3. Feasibility study of 235U and 239Pu characterization in radioactive waste drums using neutron-induced fission delayed gamma rays

    Science.gov (United States)

    Nicol, T.; Pérot, B.; Carasco, C.; Brackx, E.; Mariani, A.; Passard, C.; Mauerhofer, E.; Collot, J.

    2016-10-01

    This paper reports a feasibility study of 235U and 239Pu characterization in 225 L bituminized waste drums or 200 L concrete waste drums, by detecting delayed fission gamma rays between the pulses of a deuterium-tritium neutron generator. The delayed gamma yields were first measured with bare samples of 235U and 239Pu in REGAIN, a facility dedicated to the assay of 118 L waste drums by Prompt Gamma Neutron Activation Analysis (PGNAA) at CEA Cadarache, France. Detectability in the waste drums is then assessed using the MCNPX model of MEDINA (Multi Element Detection based on Instrumental Neutron Activation), another PGNAA cell dedicated to 200 L drums at FZJ, Germany. For the bituminized waste drum, performances are severely hampered by the high gamma background due to 137Cs, which requires the use of collimator and shield to avoid electronics saturation, these elements being very penalizing for the detection of the weak delayed gamma signal. However, for lower activity concrete drums, detection limits range from 10 to 290 g of 235U or 239Pu, depending on the delayed gamma rays of interest. These detection limits have been determined by using MCNPX to calculate the delayed gamma useful signal, and by measuring the experimental gamma background in MEDINA with a 200 L concrete drum mock-up. The performances could be significantly improved by using a higher interrogating neutron emission and an optimized experimental setup, which would allow characterizing nuclear materials in a wide range of low and medium activity waste packages.

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

    Science.gov (United States)

    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

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

    Science.gov (United States)

    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.

  6. Vertical distributions of radionuclides ((239+240)Pu, (240)Pu/(239)Pu, and (137)Cs) in sediment cores of Lake Bosten in Northwestern China.

    Science.gov (United States)

    Liao, Haiqing; Bu, Wenting; Zheng, Jian; Wu, Fengchang; Yamada, Masatoshi

    2014-04-01

    Artificial radionuclides ((137)Cs, (239+240)Pu, (241)Pu, (241)Am) deposited in lacustrine sediments have been used for dating as well as radionuclide source identification. In the present work, we investigated the vertical distributions of (239+240)Pu and (137)Cs activities, (240)Pu/(239)Pu atom ratios, and (239+240)Pu/(137)Cs activity ratios in sediment cores collected from Lake Bosten, which is the lake closest to the Lop Nor Chinese Nuclear Weapon Test site in northwestern China. Uniformly high concentrations of (239+240)Pu and (137)Cs were found in the upper layers deposited since 1964 in the sediment cores, and these were controlled by the resuspension of soil containing radionuclides from the nearby land surface. As the Chinese nuclear tests varied remarkably in yield, the mixing of the tropospheric deposition from these tests and the stratospheric deposition of global fallout has led to a (240)Pu/(239)Pu atom ratio that is similar to that of global fallout and to a (239+240)Pu/(137)Cs activity ratio that is slightly higher than that of global fallout. However, a low (240)Pu/(239)Pu atom ratio of 0.080 and high (239+240)Pu/(137)Cs activity ratio of 0.087, significantly different from the global fallout values, were observed in one sediment core (07BS10-2), indicating the inhomogenous tropospheric deposition from the Chinese nuclear tests in Lake Bosten during 1967-1973. These results are important to understand the influence of the CNTs on the radionuclide contamination in Lake Bosten.

  7. Feasibility study of {sup 235}U and {sup 239}Pu characterization in radioactive waste drums using neutron-induced fission delayed gamma rays

    Energy Technology Data Exchange (ETDEWEB)

    Nicol, T. [CEA, DEN, Cadarache, Nuclear Measurement Laboratory, F-13108 Saint-Paul-lez-Durance (France); FZJ, Institute of Energy and Climate Research – Nuclear Waste Management and Reactor Safety, Wilhelm-Johnen-Straße, d-52425 Jülich (Germany); Pérot, B., E-mail: bertrand.perot@cea.fr [CEA, DEN, Cadarache, Nuclear Measurement Laboratory, F-13108 Saint-Paul-lez-Durance (France); Carasco, C. [CEA, DEN, Cadarache, Nuclear Measurement Laboratory, F-13108 Saint-Paul-lez-Durance (France); Brackx, E. [CEA, DEN, Marcoule, Metallography and Chemical Analysis Laboratory, F-30207 Bagnols-sur-Cèze (France); Mariani, A.; Passard, C. [CEA, DEN, Cadarache, Nuclear Measurement Laboratory, F-13108 Saint-Paul-lez-Durance (France); Mauerhofer, E. [FZJ, Institute of Energy and Climate Research – Nuclear Waste Management and Reactor Safety, Wilhelm-Johnen-Straße, d-52425 Jülich (Germany); Collot, J. [Laboratoire de Physique Subatomique et de Cosmologie, Université Grenoble Alpes, CNRS/IN2P3 Grenoble (France)

    2016-10-01

    This paper reports a feasibility study of {sup 235}U and {sup 239}Pu characterization in 225 L bituminized waste drums or 200 L concrete waste drums, by detecting delayed fission gamma rays between the pulses of a deuterium-tritium neutron generator. The delayed gamma yields were first measured with bare samples of {sup 235}U and {sup 239}Pu in REGAIN, a facility dedicated to the assay of 118 L waste drums by Prompt Gamma Neutron Activation Analysis (PGNAA) at CEA Cadarache, France. Detectability in the waste drums is then assessed using the MCNPX model of MEDINA (Multi Element Detection based on Instrumental Neutron Activation), another PGNAA cell dedicated to 200 L drums at FZJ, Germany. For the bituminized waste drum, performances are severely hampered by the high gamma background due to {sup 137}Cs, which requires the use of collimator and shield to avoid electronics saturation, these elements being very penalizing for the detection of the weak delayed gamma signal. However, for lower activity concrete drums, detection limits range from 10 to 290 g of {sup 235}U or {sup 239}Pu, depending on the delayed gamma rays of interest. These detection limits have been determined by using MCNPX to calculate the delayed gamma useful signal, and by measuring the experimental gamma background in MEDINA with a 200 L concrete drum mock-up. The performances could be significantly improved by using a higher interrogating neutron emission and an optimized experimental setup, which would allow characterizing nuclear materials in a wide range of low and medium activity waste packages.

  8. 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

    Energy Technology Data Exchange (ETDEWEB)

    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)

  9. Cross-section measurements for {sup 239}Pu(n,f) and {sup 6}Li(n,{alpha}) with a lead slowing-down spectrometer

    Energy Technology Data Exchange (ETDEWEB)

    Rochman, D. [National Nuclear Data Center, Brookhaven National Laboratory, Upton, NY 11973-5000 (United States)]. E-mail: drochman@bnl.gov; Haight, R.C. [Los Alamos National Laboratory, Los Alamos, NM 87545 (United States)]. E-mail: haight@lanl.gov; O' Donnell, J.M. [Los Alamos National Laboratory, Los Alamos, NM 87545 (United States)]. E-mail: odonnell@lanl.gov; Wender, S.A. [Los Alamos National Laboratory, Los Alamos, NM 87545 (United States)]. E-mail: wender@lanl.gov; Vieira, D.J. [Los Alamos National Laboratory, Los Alamos, NM 87545 (United States)]. E-mail: vieira@lanl.gov; Bond, E.M. [Los Alamos National Laboratory, Los Alamos, NM 87545 (United States)]. E-mail: bond@lanl.gov; Bredeweg, T.A. [Los Alamos National Laboratory, Los Alamos, NM 87545 (United States)]. E-mail: toddb@lanl.gov; Wilhelmy, J.B. [Los Alamos National Laboratory, Los Alamos, NM 87545 (United States)]. E-mail: j_wilhelmy@lanl.gov; Granier, T. [Commissariat a l' Energie Atomique, 91680 Bruyeres-le-Chatel (France)]. E-mail: granier@cea.fr; Ethvignot, T. [Commissariat a l' Energie Atomique, 91680 Bruyeres-le-Chatel (France)]. E-mail: ethvignot@cea.fr; Petit, M. [Commissariat a l' Energie Atomique, 91680 Bruyeres-le-Chatel (France)]. E-mail: petit@cea.fr; Danon, Y. [Rensselaer Polytechnic Institute, Troy, NY 12180 (United States)]. E-mail: danony@rpi.edu; Romano, C. [Rensselaer Polytechnic Institute, Troy, NY 12180 (United States)]. E-mail: romanc2@rpi.edu

    2006-08-01

    We present fission cross-section measurements with {approx}10ng of {sup 239}Pu performed using the LANSCE Lead Slowing-Down Spectrometer. Results of Li6(n,{alpha}) measurements with a sample size of 760ng of {sup 6}Li are also reported. This technical achievement demonstrates the feasibility of measuring neutron-induced fission cross-section on samples with 10ng of fissile actinides that are available on ultra-small quantities. Furthermore, results on neutron-induced alpha emission show that measurements for astrophysics purposes are feasible with the LSDS.

  10. Cross-section measurements for 239Pu(n,f) and 6Li(n, α) with a lead slowing-down spectrometer

    Science.gov (United States)

    Rochman, D.; Haight, R. C.; O'Donnell, J. M.; Wender, S. A.; Vieira, D. J.; Bond, E. M.; Bredeweg, T. A.; Wilhelmy, J. B.; Granier, T.; Ethvignot, T.; Petit, M.; Danon, Y.; Romano, C.

    2006-08-01

    We present fission cross-section measurements with ˜10 ng of 239Pu performed using the LANSCE Lead Slowing-Down Spectrometer. Results of Li6(n,α) measurements with a sample size of 760 ng of 6Li are also reported. This technical achievement demonstrates the feasibility of measuring neutron-induced fission cross-section on samples with 10 ng of fissile actinides that are available on ultra-small quantities. Furthermore, results on neutron-induced alpha emission show that measurements for astrophysics purposes are feasible with the LSDS.

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

    Directory of Open Access Journals (Sweden)

    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.

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

    Science.gov (United States)

    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

    2015-04-07

    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.

  13. The gender-specific chest wall thickness prediction equations for routine measurements of {sup 239}Pu and {sup 241}Am within the lungs using HPGE detectors

    Energy Technology Data Exchange (ETDEWEB)

    Vickers, L.R. [Pantex Plant, Amarillo, TX (United States)

    1996-03-01

    The current chest wall thickness prediction equation is not applicable to use in routine lung counting measurements for detection of low energy photons (17-60 keV) within the lungs of male and female subjects. The current chest wall thickness prediction equation was derived for the NaI-CsI {open_quotes}phoswich{close_quotes} detection system, which is not the routine detection system in use; the subject position was supine, which is not the routine position; the equation did not account for the intercostal tissue thicknesses of muscle and adipose which significantly attenuate low energy photons (17-60 keV); it was derived from male subjects only and is used to predict the chest wall thickness of female subjects for whom it is not applicable. The current chest wall thickness prediction equation yields unacceptable percent errors in the HPGe detection efficiency calibration for {sup 239}Pu and {sup 241}Am (17- and 59.5-keV photons, respectively) relative to the gender-specific HPGe chest wall thickness prediction equations of this paper (+284% to -73% for {sup 239}Pu; +42% to -39% for {sup 241}Am). As a result, use of the current chest wall thickness prediction equation yields unacceptable percent errors (proportional in magnitude to the percent errors in the detection efficiency calibration) in the calculation of the minimum detectable activity (Bq) or in an initial assessment of a radioactive contamination exposure detected by a routine lung count measurement. 17 refs., 6 figs., 12 tabs.

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

    Institute of Scientific and Technical Information of China (English)

    包敏; 王群书

    2014-01-01

    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 that only colloid 239 Pu can migrate far away from the melt glass .%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

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

    Indian Academy of Sciences (India)

    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.

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

    Energy Technology Data Exchange (ETDEWEB)

    Leon Vintro, L. [University Coll., Dublin (Ireland). Dept. of Experimental Phys.; Mitchell, P.I. [University Coll., Dublin (Ireland). Dept. of Experimental Phys.; Condren, O.M. [University Coll., Dublin (Ireland). Dept. of Experimental Phys.; Moran, M. [Lawrence Livermore National Lab., Livermore, CA (United States); Vives i Batlle, J. [University Coll., Dublin (Ireland). Dept. of Experimental Phys.; Sanchez-Cabeza, J.A. [Dept. de Fisica, Universidad Autonoma de Barcelona, Bellaterra (Spain)

    1996-02-01

    In this paper, a simple technique, based on commercially-available software developed for gamma spectra analysis (MicroSAMPO {sup 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 {sup 242}Pu ``doublet`` (used as tracer) and, if present, the {sup 238}Pu ``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 {sup 240}Pu/{sup 239}Pu 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 {sup 240}Pu/{sup 239}Pu 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 {sup 239,240}Pu multiplet and published values. (orig.).

  17. Integration of measurements with atmospheric dispersion models: Source term estimation for dispersal of (239)Pu due to non-nuclear detonation of high explosive

    Science.gov (United States)

    Edwards, L. L.; Harvey, T. F.; Freis, R. P.; Pitovranov, S. E.; Chernokozhin, E. V.

    1992-10-01

    The accuracy associated with assessing the environmental consequences of an accidental release of radioactivity is highly dependent on our knowledge of the source term characteristics and, in the case when the radioactivity is condensed on particles, the particle size distribution, all of which are generally poorly known. This paper reports on the development of a numerical technique that integrates the radiological measurements with atmospheric dispersion modeling. This results in a more accurate particle-size distribution and particle injection height estimation when compared with measurements of high explosive dispersal of (239)Pu. The estimation model is based on a non-linear least squares regression scheme coupled with the ARAC three-dimensional atmospheric dispersion models. The viability of the approach is evaluated by estimation of ADPIC model input parameters such as the ADPIC particle size mean aerodynamic diameter, the geometric standard deviation, and largest size. Additionally we estimate an optimal 'coupling coefficient' between the particles and an explosive cloud rise model. The experimental data are taken from the Clean Slate 1 field experiment conducted during 1963 at the Tonopah Test Range in Nevada. The regression technique optimizes the agreement between the measured and model predicted concentrations of (239)Pu by varying the model input parameters within their respective ranges of uncertainties. The technique generally estimated the measured concentrations within a factor of 1.5, with the worst estimate being within a factor of 5, very good in view of the complexity of the concentration measurements, the uncertainties associated with the meteorological data, and the limitations of the models. The best fit also suggest a smaller mean diameter and a smaller geometric standard deviation on the particle size as well as a slightly weaker particle to cloud coupling than previously reported.

  18. Alpha and conversion electron spectroscopy of {sup 238,239}Pu and {sup 241}Am and alpha-conversion electron coincidence measurements

    Energy Technology Data Exchange (ETDEWEB)

    Dion, Michael P., E-mail: michael.dion@pnnl.gov; Miller, Brian W.; Warren, Glen A.

    2016-09-11

    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 {sup 241}Am, {sup 238}Pu and {sup 239}Pu using a dual-stage peltier-cooled 25 mm{sup 2} 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 {sup 241}Am.

  19. Transmutation of $^{239}$Pu and Other Nuclides Using Spallation Neutrons Produced by Relativistic Protons Reacting with Massive U- and Pb-Targets

    CERN Document Server

    Adam, J; Bamblevski, V P; Barabanov, M Yu; Bradnova, V; Chaloun, P; Hella, K M; Kalinnikov, V G; Krivopustov, M I; Kulakov, B A; Perelygin, V P; Pronskikh, V S; Pavliouk, A V; Solnyshkin, A A; Sosnin, A N; Stegailov, V I; Tsoupko-Sitnikov, V M; Zaverioukha, O S; Adloff, J C; Debeauvais, M; Brandt, R; Langrock, E J; Vater, P; Van, J S; Westmeier, W; Dwivedi, K K; Guo Shi Lun; Li Li Qiang; Hashemi-Nezhad, S R; Kievets, M K; Lomonosova, E M; Zhuk, I V; Modolo, G; Odoj, R; Zamani-Valassiadou, M

    2001-01-01

    Experimental studies on the transmutation of some long-lived radioactive waste nuclei, such as ^{129}I, ^{237}Np, and ^{239}Pu, as well as on natural uranium and lanthanum (all of them used as sensors) were carried out at the Synchrophasotron of the Laboratory for High Energies (JINR, Dubna). Spallation neutrons were produced by relativistic protons with energies in the range of 0.5 GeV\\le E(p)\\le 1.5 GeV interacting with 20 cm long uranium or lead target stacks. The targets were surrounded by 6 cm paraffin moderators. The radioactive sensors mentioned above were positioned on the outside surface of the moderator and contained typically approximately 0.5 up to 1 gram of long-lived isotopes. The highly radioactive targets were produced perfectly well-sealed in aluminum containers by the Institute of Physics and Power Engineering, Obninsk, Russia. From the experimentally observed transmutation rates one can easily extrapolate, that in a subcritical nuclear power assembly (or "energy amplifier") using a 10 mA pr...

  20. A high-resolution multi-parametric study of sup 239 Pu(n sub th , f) with the Cosi-Fan-Tutte spectrometer

    Energy Technology Data Exchange (ETDEWEB)

    Boucheneb, N. (Inst. de Physique, USTHB, Algiers (Algeria) Centre d' Etudes Nucleaires, 33 - Bordeaux-Gradignan (France)); Asghar, M. (Inst. de Physique, USTHB, Algiers (Algeria)); Barreau, G.; Doan, T.P.; Leroux, B.; Sicre, A. (Centre d' Etudes Nucleaires, 33 - Bordeaux-Gradignan (France)); Geltenbrot, P.; Oed, A. (Inst. Laue-Langevin, 38 - Grenoble (France))

    1991-12-09

    The Cosi-Fan-Tutte spectrometer has been used to measure for the first time in one go the mass-nuclear charge-energy correlations of well-resolved light group masses for {sup 239}Pu(n{sub th}, f). About 2x10{sup 6} events were collected and analysed. The global mass distribution is consistent with the Lohengrin data. The mean proton odd-even effects in yields and energy are {delta}{sub p}=(11.8{+-}0.3)% and {delta}E{sub K}{sup o-e}=0.49{+-}0.15 MeV respectively. The {delta}{sub p}(E{sub L}) varies from {approx equal}7% to {approx equal}25% for E{sub L}=90 to 116 MeV. The present analysis consists of 21 values of E{sub L} compared to only 5 values for Lohengrin. The apparent mean neutron odd-even effect {delta}{sub n}=(3.5{+-}0.1)% is much lower than the {delta}{sub n}=(6.5{+-}0.7)% for Lohengrin. The mean value of conditional variance <{sigma}{sub Z}{sup 2}(Zvertical strokeA)>=(0.42{+-}0.02); the <{sigma}{sub Z}{sup 2}(Zvertical strokeA)> increases from {sup 230}Th to {sup 250}Cf and this behaviour turns out to be important for understanding the dynamics of the fission process. (orig.).

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

    CERN Document Server

    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...

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

    Energy Technology Data Exchange (ETDEWEB)

    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.

  3. Determination of Fission Product Yields of 235U, 238U and 239Pu for Neutron Energies from 0.5 to 14.8 MeV

    Science.gov (United States)

    Gooden, Matthew; Arnold, Charles; Becker, John; Bhatia, Chitra; Bhike, Megha; Fowler, Malcolm; Howell, Calvin; Kelley, John; Stoyer, Mark; Tonchev, Anton; Tornow, Werner; Vieira, Dave; Wilhelmy, Jerry

    2014-03-01

    A joint TUNL-LANL-LLNL collaboration has been formed to study the issue of possible energy dependences for certain fission product isotopes. Work has been carried out at the TUNL 10 MV Tandem accelerator which produces nearly mono-energetic neutrons via either 2H(d,n)3He,3H(d,n)4He,or3H(p,n)3He reactions. Three dual fission ionization chambers dedicated to 235U, 238U and 239Pu thick target foils and thin monitor foils respectively, were exposed to the neutron beams. After irradiation, thick target foils were gamma counted over a period of 1-2 months and characteristic gamma rays from fission products were recorded using HPGe detectors at TUNL's low background counting area. Using the dual fission chambers, relative fission product yield were determined at a high precision of 2-3 % as well as absolute fission product yields at a lower precision of 5-6 %. Preliminary results will be presented for a number of fission product isotopes over the incident neutron energy range of 0.5 to 14.8 MeV.

  4. Energy Dependence of Neutron-Induced Fission Product Yields of 235U, 238U and 239Pu Between 0.5 and 14.8 MeV

    Science.gov (United States)

    Gooden, Matthew; Tornow, Werner; Tonchev, Anton; Vieira, Dave; Wilhelmy, Jerry; Arnold, Charles; Fowler, Malcolm; Stoyer, Mark

    2014-09-01

    Under a joint collaboration between TUNL-LANL-LLNL, a set of absolute fission product yield measurements have been performed. The energy dependence of a number of cumulative fission products between 0.5 and 14.8 MeV have been measured using quasi-monoenergetic neutron beams for three actinide targets, 235U, 238U and 239Pu, between 0.5 and 14.8 MeV. The FPYs were measured by a combination of activation utilizing specially designed dual-fission chambers and γ-ray counting. The dual-fission chambers are back-to-back ionization chambers encasing a target with thin deposits of the same target isotope in each chamber. This method allows for the direct measurement of the fission rate in the activation target with no reference to the fission cross-section, reducing uncertainties. γ-ray counting was performed on well-shield HPGe detectors over a period of 2 months per activation to properly identify fission products. Reported are absolute cumulative fission product yields for incident neutron energies of 0.5, 1.37, 2.4, 4.6 and 14.8 MeV.

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

    Energy Technology Data Exchange (ETDEWEB)

    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.

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

    Energy Technology Data Exchange (ETDEWEB)

    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.

  7. Microdistribution and long-term retention of 239Pu (NO3)4 in the respiratory tracts of an acutely exposed plutonium worker and experimental beagle dogs.

    Science.gov (United States)

    Nielsen, Christopher E; Wilson, Dulaney A; Brooks, Antone L; McCord, Stacey L; 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 [(239)Pu (NO(3))(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 histologic lung, lymph node, trachea, and nasal turbinate tissue sections. These studies showed that both the human and dogs had a nonuniform 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 subpleural 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 to increase cancer risk.

  8. Ultra-trace determination of (90)Sr, (137)Cs, (238)Pu, (239)Pu, and (240)Pu by triple quadruple collision/reaction cell-ICP-MS/MS: Establishing a baseline for global fallout in Qatar soil and sediments.

    Science.gov (United States)

    Amr, Mohamed A; Helal, Abdul-Fattah I; Al-Kinani, Athab T; Balakrishnan, Perumal

    2016-03-01

    The development of practical, fast, and reliable methods for the ultra-trace determination of anthropogenic radionuclides (90)Sr, (137)Cs, (238)Pu, (239)Pu, and (240)Pu by triple quadruple collision/reaction cell inductively coupled plasma mass spectrometry (CRC-ICP-MS/MS) were investigated in term of its accuracy and precision for producing reliable results. The radionuclides were extracted from 1 kg of the environmental soil samples by concentrated nitric and hydrochloric acids. The leachate solutions were measured directly by triple quadrupole CRC-ICP-MS/MS. For quality assurance, a chemical separation of the concerned radionuclides was conducted and then measured by single quadrupole-ICP-MS. The developed methods were next applied to measure the anthropogenic radionuclides (90)Sr, (137)Cs, (238)Pu, (239)Pu, and (240)Pu in soil samples collected throughout the State of Qatar. The average concentrations of (90)Sr, (137)Cs, (238)Pu, (239)Pu, and (240)Pu were 0.606 fg/g (3.364 Bq/kg), 0.619 fg/g (2.038 Bq/kg), 0.034 fg/g (0.0195 Bq/kg), 65.59 fg/g (0.150 Bq/kg), and 12.06 fg/g (0.103 Bq/kg), respectively.

  9. Energy dependence of fission product yields from 235U, 238U, and 239Pu with monoenergetic neutrons between thermal and 14.8 MeV

    Science.gov (United States)

    Gooden, Matthew; Arnold, Charles; Bhike, Megha; Bredeweg, Todd; Fowler, Malcolm; Krishichayan; Tonchev, Anton; Tornow, Werner; Stoyer, Mark; Vieira, David; Wilhelmy, Jerry

    2017-09-01

    Under a joint collaboration between TUNL-LANL-LLNL, a set of absolute fission product yield measurements has been performed. The energy dependence of a number of cumulative fission product yields (FPY) have been measured using quasi-monoenergetic neutron beams for three actinide targets, 235U, 238U and 239Pu, between 0.5 and 14.8 MeV. The FPYs were measured by a combination of fission counting using specially designed dual-fission chambers and γ-ray counting. Each dual-fission chamber is a back-to-back ionization chamber encasing an activation target in the center with thin deposits of the same target isotope in each chamber. This method allows for the direct measurement of the total number of fissions in the activation target with no reference to the fission cross-section, thus reducing uncertainties. γ-ray counting of the activation target was performed on well-shielded HPGe detectors over a period of two months post irradiation to properly identify fission products. Reported are absolute cumulative fission product yields for incident neutron energies of 0.5, 1.37, 2.4, 3.6, 4.6, 5.5, 7.5, 8.9 and 14.8 MeV. Preliminary results from thermal irradiations at the MIT research reactor will also be presented and compared to present data and evaluations. This work was performed under the auspices of the U.S. Department of Energy by Los Alamos National Security, LLC under contract DE-AC52-06NA25396, Lawrence Livermore National Laboratory under contract DE-AC52-07NA27344 and by Duke University and Triangle Universities Nuclear Laboratory through NNSA Stewardship Science Academic Alliance grant No. DE-FG52-09NA29465, DE-FG52-09NA29448 and Office of Nuclear Physics Grant No. DE-FG02-97ER41033.

  10. Uncertainty analyses in the resolved resonance region of {sup 235}U, {sup 238}U, and {sup 239}Pu with the Reich-Moore R-matrix theory for JENDL-3.2

    Energy Technology Data Exchange (ETDEWEB)

    Kawano, Toshihiko [Kyushu University, Interdisciplinary Graduate School of Engineering Sciences, Kasuga, Fukuoka (Japan); Shibata, Keiichi [Japan Atomic Energy Research Inst., Tokai, Ibaraki (Japan). Tokai Research Establishment

    2002-08-01

    A simple method to estimate covariances for resolved resonance parameters was developed. 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. The method developed here derives a covariance matrix for the resolved resonance parameters which gives an appropriate uncertainty of the averaged cross sections. The method was adopted to evaluate the covariance data for {sup 235}U, {sup 238}U, and {sup 239}Pu resonance parameters in JENDL-3.2, with the Reich-Moore R-matrix formula. (author)

  11. 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.

    Science.gov (United States)

    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

  12. {sup 137}Cs, {sup 239+240}Pu and {sup 240}Pu/{sup 239}Pu atom ratios in the surface waters of the western North Pacific Ocean, eastern Indian Ocean and their adjacent seas

    Energy Technology Data Exchange (ETDEWEB)

    Yamada, Masatoshi; Zheng, Jian; Wang, Zhong-Liang [Nakaminato Laboratory for Marine Radioecology, National Institute of Radiological Sciences, Isozaki 3609, Hitachinaka, Ibaraki 311-1202 (Japan)

    2006-07-31

    Surface seawater samples were collected along the track of the R/V Hakuho-Maru cruise (KH-96-5) from Tokyo to the Southern Ocean. The {sup 137}Cs activities were determined for the surface waters in the western North Pacific Ocean, the Sulu and Indonesian Seas, the eastern Indian Ocean, the Bay of Bengal, the Andaman Sea, and the South China Sea. The {sup 137}Cs activities showed a wide variation with values ranging from 1.1 Bq m{sup -3} in the Antarctic Circumpolar Region of the Southern Ocean to 3 Bq m{sup -3} in the western North Pacific Ocean and the South China Sea. The latitudinal distributions of {sup 137}Cs activity were not reflective of that of the integrated deposition density of atmospheric global fallout. The removal rates of {sup 137}Cs from the surface waters were roughly estimated from the two data sets of Miyake et al. [Miyake Y, Saruhashi K, Sugimura Y, Kanazawa T, Hirose K. Contents of {sup 137}Cs, plutonium and americium isotopes in the Southern Ocean waters. Pap Meteorol Geophys 1988;39:95-113] and this study to be 0.016 yr{sup -1} in the Sulu and Indonesian Seas, 0.033 yr{sup -1} in the Bay of Bengal and Andaman Sea, and 0.029 yr{sup -1} in the South China Sea. These values were much lower than that in the coastal surface water of the western Northwest Pacific Ocean. This was likely due to less horizontal and vertical mixing of water masses and less scavenging. {sup 239+240}Pu activities and {sup 240}Pu/{sup 239}Pu atom ratios were also determined for the surface waters in the western North Pacific Ocean, the Sulu and Indonesian Seas and the South China Sea. The {sup 240}Pu/{sup 239}Pu atom ratios ranged from 0.199+/-0.026 to 0.248+/-0.027 on average, and were significantly higher than the global stratospheric fallout ratio of 0.18. The contributions of the North Pacific Proving Grounds close-in fallout Pu were estimated to be 20% for the western North Pacific Ocean, 39% for the Sulu and Indonesian Seas and 42% for the South China Sea by using

  13. {sup 137}Cs, {sup 239+24}Pu and {sup 24}Pu/{sup 239}Pu atom ratios in the surface waters of the western North Pacific Ocean, eastern Indian Ocean and their adjacent seas

    Energy Technology Data Exchange (ETDEWEB)

    Yamada, Masatoshi [Nakaminato Laboratory for Marine Radioecology, National Institute of Radiological Sciences, Isozaki 3609, Hitachinaka, Ibaraki 311-1202 (Japan)]. E-mail: m_yamada@nirs.go.jp; Zheng Jian [Nakaminato Laboratory for Marine Radioecology, National Institute of Radiological Sciences, Isozaki 3609, Hitachinaka, Ibaraki 311-1202 (Japan); Wang Zhongliang [Nakaminato Laboratory for Marine Radioecology, National Institute of Radiological Sciences, Isozaki 3609, Hitachinaka, Ibaraki 311-1202 (Japan); State Key Laboratory of Environmental Geochemistry, Institute of Geochemistry, Chinese Academy of Sciences, Guanshui Road 46, Guiyang 550002 (China)

    2006-07-31

    Surface seawater samples were collected along the track of the R/V Hakuho-Maru cruise (KH-96-5) from Tokyo to the Southern Ocean. The {sup 137}Cs activities were determined for the surface waters in the western North Pacific Ocean, the Sulu and Indonesian Seas, the eastern Indian Ocean, the Bay of Bengal, the Andaman Sea, and the South China Sea. The {sup 137}Cs activities showed a wide variation with values ranging from 1.1 Bq m{sup -3} in the Antarctic Circumpolar Region of the Southern Ocean to 3 Bq m{sup -3} in the western North Pacific Ocean and the South China Sea. The latitudinal distributions of {sup 137}Cs activity were not reflective of that of the integrated deposition density of atmospheric global fallout. The removal rates of {sup 137}Cs from the surface waters were roughly estimated from the two data sets of Miyake et al. [Miyake Y, Saruhashi K, Sugimura Y, Kanazawa T, Hirose K. Contents of {sup 137}Cs, plutonium and americium isotopes in the Southern Ocean waters. Pap Meteorol Geophys 1988;39:95-113] and this study to be 0.016 yr{sup -1} in the Sulu and Indonesian Seas, 0.033 yr{sup -1} in the Bay of Bengal and Andaman Sea, and 0.029 yr{sup -1} in the South China Sea. These values were much lower than that in the coastal surface water of the western Northwest Pacific Ocean. This was likely due to less horizontal and vertical mixing of water masses and less scavenging. {sup 239+24}Pu activities and {sup 24}Pu/{sup 239}Pu atom ratios were also determined for the surface waters in the western North Pacific Ocean, the Sulu and Indonesian Seas and the South China Sea. The {sup 24}Pu / {sup 239}Pu atom ratios ranged from 0.199 {+-} 0.026 to 0.248 {+-} 0.027 on average, and were significantly higher than the global stratospheric fallout ratio of 0.18. The contributions of the North Pacific Proving Grounds close-in fallout Pu were estimated to be 20% for the western North Pacific Ocean, 39% for the Sulu and Indonesian Seas and 42% for the South China Sea by

  14. (137)Cs, (239+240)Pu concentrations and the (240)Pu/(239)Pu atom ratio in a sediment core from the sub-aqueous delta of Yangtze River estuary.

    Science.gov (United States)

    Pan, S M; Tims, S G; Liu, X Y; Fifield, L K

    2011-10-01

    A sediment core collected from the sub-aqueous delta of the Yangtze River estuary was subjected to analyses of (137)Cs and plutonium (Pu) isotopes. The (137)Cs was measured using γ-spectrometry at the laboratories at the Nanjing University and Pu isotopes were determined with Accelerator Mass Spectrometry (AMS), measurements made at the Australian National University. The results show considerable structure in the depth concentration profiles of the (137)Cs and (239+240)Pu. The shape of the vertical (137)Cs distribution in the sediment core was similar to that of the Pu. The maximum (137)Cs and (239+240)Pu concentrations were 16.21 ± 0.95 mBq/g and 0.716 ± 0.030 mBq/g, respectively, and appear at same depth. The average (240)Pu/(239)Pu atom ratio was 0.238 ± 0.007 in the sediment core, slightly higher than the average global fallout value. The changes in the (240)Pu/(239)Pu atom ratios in the sediment core indicate the presence of at least two different Pu sources, i.e., global fallout and another source, most likely close-in fallout from the Pacific Proving Grounds (PPG) in the Marshall Islands, and suggest the possibility that Pu isotopes are useful as a geochronological tool for coastal sediment studies. The (137)Cs and (239+240)Pu inventories were estimated to be 7100 ± 1200 Bq/m(2) and 407 ± 27 Bq/m(2), respectively. Approximately 40% of the (239+240)Pu inventory originated from the PPG close-in fallout and about 50% has derived from land-origin global fallout transported to the estuary by the river. This study confirms that AMS is a useful tool to measure (240)Pu/(239)Pu atom ratio and can provide valuable information on sedimentary processes in the coastal environment.

  15. Influences of parameter uncertainties within the ICRP-66 respiratory tract model: regional tissue doses for 239PuO2 and 238UO2/238U3O8.

    Science.gov (United States)

    Farfán, Eduardo B; Huston, Thomas E; Bolch, W Emmett; Vernetson, William G; Bolch, Wesley E

    2003-04-01

    This paper extends an examination of the influence of parameter uncertainties on regional doses to respiratory tract tissues for short-ranged alpha particles using the ICRP-66 respiratory tract model. Previous papers examined uncertainties in the deposition and clearance aspects of the model. The critical parameters examined in this study included target tissue depths, thicknesses, and masses, particularly within the thoracic or lung regions of the respiratory tract. Probability density functions were assigned for the parameters based on published data. The probabilistic computer code LUDUC (Lung Dose Uncertainty Code) was used to assess regional and total lung doses from inhaled aerosols of 239PuO2 and 238UO2/238U3O8. Dose uncertainty was noted to depend on the particle aerodynamic diameter. Additionally, dose distributions were found to follow a lognormal distribution pattern. For 239PuO2 and 238UO2/238U3O8, this study showed that the uncertainty in lung dose increases by factors of approximately 50 and approximately 70 for plutonium and uranium oxides, respectively, over the particle size range from 0.1 to 20 microm. For typical exposure scenarios involving both radionuclides, the ratio of the 95% dose fractile to the 5% dose fractile ranged from approximately 8-10 (corresponding to a geometric standard deviation, or GSD, of about 1.7-2) for particle diameters of 0.1 to 1 microm. This ratio increased to about 370 for plutonium oxide (GSD approximately 4.5) and to about 600 for uranium oxide (GSD approximately 5) as the particle diameter approached 20 microm. However, thoracic tissue doses were quite low at larger particle sizes because most of the deposition occurred in the extrathoracic airways. For 239PuO2, median doses from LUDUC were found be in general agreement with those for Reference Man (via deterministic LUDEP 2.0 calculations) in the particle range of 0.1 to 5 microm. However, median doses to the basal cell nuclei of the bronchial airways (BB

  16. New measurements of (n,γ) and (n,fission) cross sections and capture-to-fission ratios for ^233,235U and ^239Pu using the DANCE 4π BaF2 array

    Science.gov (United States)

    Bredeweg, T. A.; Jandel, M.; Fowler, M. M.; Bond, E. M.; Haight, R. C.; Keksis, A. L.; O'Donnell, J. M.; Reifarth, R.; Rundberg, R. S.; Ullmann, J. L.; Vieira, D. J.; Wilhelmy, J. B.; Wouters, J. M.; Becker, J. A.; Parker, W. E.; Wu, C. Y.; Baker, J. D.; McGrath, C. A.

    2009-10-01

    Accurate neutron nuclear data are important to many issues in stockpile stewardship, nuclear reactor design and re-certification, nuclear non-proliferation and nuclear forensics. Of particular interest are the production and destruction reactions for all of the major and most of the minor actinides. The competition between capture and fission in many of the actinides presents both an obstacle and an opportunity for large γ detector arrays such as DANCE. Additional instrumentation is required to deconvolve the two contributions to the total observed γ-ray spectrum. However, conducting a simultaneous measurement can simplify background treatment and other sources of systematic uncertainty. An outline of the current experimental program will be presented along with results from neutron capture measurements on ^233,235U and ^239Pu.

  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

    Directory of Open Access Journals (Sweden)

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

    Energy Technology Data Exchange (ETDEWEB)

    Kim, Do Heon; Gil, Choong-Sup; Lee, Young-Ouk [Korea Atomic Energy Research Institute, Daejeon (Korea, Republic of)

    2014-10-15

    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 {sup 235}U and {sup 239}Pu 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 {sup 235}U and {sup 239}Pu 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.

  19. Estimation of covariances of {sup 16}O, {sup 23}Na, Fe, {sup 235}U, {sup 238}U and {sup 239}Pu neutron nuclear data in JENDL-3.2

    Energy Technology Data Exchange (ETDEWEB)

    Shibata, Keiichi [Japan Atomic Energy Research Inst., Tokai, Ibaraki (Japan). Tokai Research Establishment; Nakajima, Yutaka; Kawano, Toshihiko; Oh, Soo-Youl; Matsunobu, Hiroyuki; Murata, Toru

    1997-10-01

    Covariances of nuclear data have been estimated for 6 nuclides contained in JENDL-3.2. The nuclides considered are {sup 16}O, {sup 23}Na, Fe, {sup 235}U, {sup 238}U, and {sup 239}Pu, which are regarded as important for the nuclear design study of fast reactors. The physical quantities for which covariances are deduced are cross sections, resolved and unresolved resonance parameters, and the first order Legendre-polynomial coefficient for the angular distribution of elastically scattered neutrons. As for {sup 235}U, covariances were obtained also for the average number of neutrons emitted in fission. The covariances were estimated by using the same methodology that had been used in the JENDL-3.2 evaluation in order to keep a consistency between mean values and their covariances. The least-squares fitting code GMA was used in estimating covariances for reactions of which JENDL-3.2 cross sections had been evaluated by taking account of measurements. In nuclear model calculations, the covariances were calculated by the KALMAN system. The covariance data obtained were compiled in the ENDF-6 format, and will be put into the JENDL-3.2 Covariance File which is one of JENDL special purpose files. (author). 193 refs.

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

    Energy Technology Data Exchange (ETDEWEB)

    De Saint Jean, C.; Archier, P.; Noguere, G.; Litaize, O.; Vaglio-Gaudard, C.; Bernard, D.; Leray, O. [CEA, DEN, DER, Cadarache, F-13108 Saint-Paul-lez-Durance (France)

    2012-07-01

    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 {sup 235,238}U, {sup 239}Pu, {sup 241}Am, {sup 56}Fe, {sup 23}Na and {sup 27}Al. (authors)

  1. A method of measurement of (239)Pu, (240)Pu, (241)Pu in high U content marine sediments by sector field ICP-MS and its application to Fukushima sediment samples.

    Science.gov (United States)

    Bu, Wenting; Zheng, Jian; Guo, Qiuju; Aono, Tatsuo; Tazoe, Hirofumi; Tagami, Keiko; Uchida, Shigeo; Yamada, Masatoshi

    2014-01-01

    An accurate and precise analytical method is highly needed for the determination of Pu isotopes in marine sediments for the long-term marine environment monitoring that is being done since the Fukushima Dai-ichi Nuclear Power Plant accident. The elimination of uranium from the sediment samples needs to be carefully checked. We established an analytical method based on anion-exchange chromatography and SF-ICP-MS in this work. A uranium decontamination factor of 2 × 10(6) was achieved, and the U concentrations in the final sample solutions were typically below 4 pg mL(-1), thus no extra correction of (238)U interferences from the Pu spectra was needed. The method was suitable for the analysis of (241)Pu in marine sediments using large sample amounts (>10 g). We validated the method by measuring marine sediment reference materials and our results agreed well with the certified and the literature values. Surface sediments and one sediment core sample collected after the nuclear accident were analyzed. The characterization of (241)Pu/(239)Pu atom ratios in the surface sediments and the vertical distribution of Pu isotopes showed that there was no detectable Pu contamination from the nuclear accident in the marine sediments collected 30 km off the plant site.

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

    Science.gov (United States)

    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

  3. 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)

    Energy Technology Data Exchange (ETDEWEB)

    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)

  4. Neutron powder diffraction study of 239PuD x

    Science.gov (United States)

    Bartscher, W.; Boeuf, A.; Caciuffo, R.; Fournier, J. M.; Haschke, J. M.; Manes, L.; Rebizant, J.; Rustichelli, F.; Ward, J. W.

    1985-05-01

    A neutron powder diffraction study has been carried out on several deuterids of Plutonium (PuD 2.25,PuD 2.33, PuD 2.65) to determine the positions of deuterium atoms in the host metal f.c.c. lattice. It has been found that vacancies occur in the tetrahedral sites. Moreover, with increasing deuterium concentration, octahedral interstitial deuterium atoms are displaced from their ideal positions. These results can be explained by the formation of clusters. Finally, at low temperature, these compounds become ferromagnetically ordered. An ordered magnetic moment μ 0≈0.8 μ B has been measured on all compounds.

  5. [239Pu and chromosomal aberrations in human peripheral blood lymphocytes].

    Science.gov (United States)

    Okladnikova, N D; Osovets, S V; Kudriavtseva, T I

    2009-01-01

    The genome status in somatic cells was assessed using the chromosomal aberration (CA) test in peripheral blood lymphocytes from 194 plutonium workers exposed to occupational radiation mainly from low-transportable compounds of airborne 230Pu. Pu body burden at the time of cytogenetic study varied from values close to the method sensitivity to values multiply exceeding the permissible level. Standard (routine) methods of peripheral blood lymphocytes cultivation were applied. Chromatid- and chromosomal-type structural changes were estimated. Aberrations were estimated per 100 examined metaphase cells. The quantitative relationship between the CA frequency and Pu body burden and the absorbed dose to the lung was found. Mathematical processing of results was carried out based on the phenomenological model. The results were shown as theoretical and experimental curves. The threshold of the CA yield was 0.43 +/- 0.03 kBq (Pu body burden) and 6.12 +/- 1.20 cGy (absorbed dose to the lung).

  6. Toxicological versus Radiological Hazards of {sup 239}Pu

    Energy Technology Data Exchange (ETDEWEB)

    Tansky, R.R.

    2001-07-26

    Plutonium is frequently referred to as ''the most toxic substance known to man''. While there are other chemicals that cause more immediately serious health consequences, plutonium does have the lowest permissible levels for any of the radioactive elements. Concentration limits for plutonium and its compounds are based on its radiotoxicity, specifically carcinogenicity, not on its chemical toxicity.

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

    Science.gov (United States)

    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.

  8. The 239 Pu(n,2n)238Pu cross section: preliminary calculations

    Energy Technology Data Exchange (ETDEWEB)

    Chen, H; Reffo, G; Ross, M A; White, R M

    1999-03-12

    The primary motivation for the present work is to provide theoretical values for the ratio of the partial 239Pu(n,2nx{gamma})238Pu to total 239 Pu(n,2n)238Pu cross section for several discrete gamma transitions. Results and conclusions of preliminary calculations from threshold to 20 MeV are presented. Calculations are based on theoretical models with parameters obtained from the literature or from our ad hoc systematics. Optical model cross sections and transmission coefficients were determined using the coupled-channels method. The calculations included a preequilibrium component followed by multiple particle and gamma-ray emissions. Fission competition was included at all stages of de-excitation. Suggestions for further verifications and possible improvements are provided.

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

    Energy Technology Data Exchange (ETDEWEB)

    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.

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

    Energy Technology Data Exchange (ETDEWEB)

    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.

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

    Energy Technology Data Exchange (ETDEWEB)

    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.

  12. Spatial statistical analysis of contamination level of 241Am and 239Pu, Thule, North-West Greenland

    DEFF Research Database (Denmark)

    Strodl Andersen, Jens

    intensively. In Grønnedal 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......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 2.8×105 Bq m-2. Highest levels were observed near Narsaarsuk. This area was also sampled most...

  13. Evaluation of fission product yields from fission spectrum n+239Pu using a meta analysis of benchmark data

    Science.gov (United States)

    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.

  14. Migration of plutonium from freshwater ecosystem at Hanford. [/sup 238/Pu, /sup 239/Pu, /sup 240/Pu

    Energy Technology Data Exchange (ETDEWEB)

    Emery, R. M.; Klopfer, D. C.; McShane, M. C.

    1977-09-01

    A reprocessing waste pond at Hanford has been inventoried to determine quantities of plutonium (Pu) that have been accumulated since its formation in 1944. Expressions of export were developed from these inventory data and from informed assumptions about the vectors which act to mobilize material containing Pu. This 14-acre pond provides a realistic illustration of the mobility of Pu in a lentic ecosystem. The ecological behavior of Pu in this pond is similar to that in other contaminated aquatic systems having widely differing limnological characteristics. Since its creation, this pond has received about one Ci of /sup 239/,/sup 240/Pu and /sup 238/Pu, most of which has been retained by its sediments. Submerged plants, mainly diatoms and Potamogeton, accumulate >95% of the Pu contained in biota. Emergent insects are the only direct biological route of export, mobilizing about 5 x 10/sup 3/ nCi of Pu annually, which is also the estimated maximum quantity of the Pu exported by waterfowl, birds and mammals collectively. There is no apparent significant export by wind, and it is not likely that Pu has migrated to the ground water below U-Pond via percolation. Although this pond has a rapid flushing rate, a eutrophic nutrient supply with a diverse biotic profile, and interacts with an active terrestrial environment, it appears to effectively bind Pu and prevent it from entering pathways to man and other life.

  15. Heterogeneous reduction of {sup 239}PuO{sub 2} by aqueous Fe(II) in the presence of hematite

    Energy Technology Data Exchange (ETDEWEB)

    Felmy, A.R.; Moore, D.A.; Qafoku, O.; Buck, E.; Ilton, E.S. [Pacific Northwest National Laboratory, Richland, WA (United States); Conradson, S.D. [Los Alamos National Laboratory, NM (United States)

    2013-07-01

    The reduction of PuO{sub 2}(am) by Fe(II) in the presence and absence of hematite was studied over a range of pH values and oxidation/reduction potentials. In contrast to thermodynamic predictions, the presence of hematite did not have a major effect on the overall reduction of PuO{sub 2}(am) to aqueous Pu(III). Instead the aqueous Pu(III) concentrations at longer time frames were accurately predicted using the measured Fe(II) concentration and existing thermodynamic data for the reaction: H{sub 2}O + H{sup +} + Fe{sup 2+} + PuO{sub 2}(am) {r_reversible} Pu{sup 3+} + Fe(OH){sub 3}(am) with log K = -0.6. The accuracy of this approach in all solutions containing aqueous Fe(II), coupled with the apparent lack of oxidation of Fe(II) by O{sub 2}(g), suggests that the Fe(OH){sub 3}(am) is formed by the oxidation of Fe(II) to Fe(III) by radiolysis. The continued generation of reactive amorphous iron hydroxide by radiolysis prevents thermodynamic equilibrium from being reached with more stable ferric oxide compounds, except possibly under acidic conditions where amorphous ferric hydroxide is soluble. The use of measured pe values, instead of aqueous Fe(II) measurements, also yields reasonable predictions of the final Pu(III) concentrations although the predictions are more uncertain. (orig.)

  16. Transuranic concentrations in reef and pelagic fish from the Marshall Islands. [/sup 239/Pu, /sup 240/Pu

    Energy Technology Data Exchange (ETDEWEB)

    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.

  17. Spatial statistical analysis of contamination level of 241Am and 239Pu, Thule, North-West Greenland

    Energy Technology Data Exchange (ETDEWEB)

    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)

  18. Leaching of UO2 pellets doped with alpha-emitters (238/239Pu) in synthetic deep Callovian-Oxfordian groundwater

    Science.gov (United States)

    Tribet, M.; Jégou, C.; Broudic, V.; Marques, C.; Rigaux, P.; Gavazzi, A.

    2010-03-01

    The reactivity of a polycrystalline UO2 surface under alpha irradiation in contact with groundwater is investigated, in the hypothesis of direct disposal of spent fuel in a deep geological repository. Two series of plutonium-doped UO2 samples (specific alpha activity of 18 and 385 MBq·g-1UO2) were leached in a synthetic Callovian-Oxfordian deep groundwater under anoxic conditions (Ar/CO2 3000 ppm, 3.5 bar relative pressure) to assess both the impact of alpha radiolysis of water and the complexing capacity of the groundwater ions on the dissolution of UO2. This study follows a prior one performed in pure and carbonated waters. Firstly, technical developments were necessary for the analyses in the groundwater solution because of its high salt concentrations: quantification limits were determined for the measurement of uranium and radiolytic H2O2 traces in this medium. Secondly, 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 followed, based on high-temperature annealing in Ar + 4% H2 with preleaching cycles. Each type of UO2 pellet was then leached under static conditions for 30 days (anoxic conditions, deep groundwater solutions). Results on the evolution of uranium releases are presented. For the lowest alpha activity (18 MBq·g-1UO2), uranium releases in groundwater were below the quantification limit of 2 × 10-8 mol·L-1 with a kinetic phosphorescence analyzer, even after 30 days. However, for higher alpha activity (385 MBq·g-1UO2) the uranium releases begin to exceed the quantification limit after 14 days of leaching and then increase exponentially. This increase is comparable to results previously obtained in carbonated solutions.

  19. Changes in the Shape of Histograms Constructed from the Results of 239-Pu Alpha-Activity Measurements Correlate with the Deviations of the Moon from the Keplerian Orbit

    Directory of Open Access Journals (Sweden)

    Shapovalov S. N.

    2009-10-01

    Full Text Available We have found that the shape of the histograms, constructed on the basis of the results of radioactivity measurements, changes in correlation with the distortions of the lunar Keplerian orbit (due to the gravitational influence of the Sun. Taking into account that the phenomenon of "macroscopic fluctuations" (regular changes in the fine structure of histograms constructed from the results of measurements of natural processes does not depend on the nature of the process under study, one can consider the correlation of the histogram shape with the Moon's deviations from the Keplerian orbit to be independent from the nature of the process the histograms were obtained on.

  20. Changes in the Shape of Histograms Constructed from the Results of 239-Pu Alpha-Activity Measurements Correlate with the Deviations of the Moon from the Keplerian Orbit

    Directory of Open Access Journals (Sweden)

    Shapovalov S. N.

    2009-10-01

    Full Text Available We have found that the shape of the histograms, constructed on the basis of the results of radioactivity measurements, changes in correlation with the distortions of the lunar Keplerian orbit (due to the gravitational influence of the Sun. Taking into account that the phenomenon of “macroscopic fluctuations” (regular changes in the fine structure of histograms constructed from the results of measurements of natural processes does not depend on the nature of the process under study, one can consider the correlation of the histogram shape with the Moon’s deviations from the Keplerian orbit to be independent from the nature of the process the histograms were obtained on.

  1. Medida de isótopos de Plutonio, 239Pu y 240Pu, mediante espectrometría de masas con aceleradores de baja energía

    OpenAIRE

    Chamizo Calvo, Elena

    2009-01-01

    El primer bloque, sobre la descripción de la técnica y de los dos sistemas empleados, comprende los Capítulos 2, 3 y 4. En el Capítulo 2 presentaremos los fundamento s del AMS de baja energía y las características de diseño de sus instalaciones. De esta forma, veremos que un sistema compacto de AMS no es simplemente una versión a escala de uno convencional, y justificaremos las razones por las que la comunidad científica se ha visto obligada durante 20 años a usar grandes aceleradores. En el ...

  2. Distribution of sup 137 Cs, sup 90 Sr, sup 238 Pu, sup 239 Pu, sup 241 Am and sup 244 Cm in Pond B, Savannah River Site

    Energy Technology Data Exchange (ETDEWEB)

    Whicker, F.W. (Colorado State Univ., Fort Collins, CO (USA)); Pinder, J.E. III; Bowling, J.W. (Savannah River Ecology Lab., Aiken, SC (USA)); Alberts, J.J. (Georgia Univ., Sapelo Island, GA (USA). Marine Inst.); Brisbin, I.L. Jr. (Savannah River Ecology Lab., Aiken, SC (USA))

    1989-05-01

    The gradual senescence of present-day operating nuclear facilities, and resultant contamination of aquatic and terrestrial ecosystems, emphasize the importance of understanding the behavior of radionuclides in the environment. Observations and deductions concerning mechanisms of radionuclide transport can contribute significantly to knowledge of fundamental ecological processes. This study emphasized the ecosystem-level distribution of several long-lived radionuclides in an abandoned reactor cooling impoundment after a twenty year period of chemical and biological equilibration. 90 refs., 14 figs., 5 tabs.

  3. OTSENKA OF STABILITY OF DIGITAL SYSTEM OF REGULATION BY MULTICOHERENT OBJECT

    Directory of Open Access Journals (Sweden)

    V. S. Kudryashov

    2012-01-01

    Full Text Available The algorithm for assessing the sustainability of digital object control system as an example of a multiply column for ammonia synthesis. The solution is performed using a discrete description of the regulatory system. Description of the system represented in the transfer functions of input-output. These results extend to a class of multiply connected unsymmetrical control objects.

  4. Economic evaluation of the technological development of coal extraction. Ekonomicheskaya otsenka tekhnologicheskogo razvitiya ugledobychu

    Energy Technology Data Exchange (ETDEWEB)

    Golland, E.B.; Rybakova, T.A.

    1985-01-01

    The monograph investigates the trends and prospects in the development of major technological directions in coal extraction. The characteristics of the development of the coal industry at the modern stage are analyzed and the basic trends of technical progress in coal extraction are characterized. Attention is devoted to the problems of evaluating the effectiveness and of determining the rational scales for using different technologies for coal extraction in the long range using economic and mathematical modeling. A model for optimizing the technological development of a coal basin is proposed. The results of calculation variants in terms of a model for the Kuzbass are presented.

  5. Beta and gamma decay heat measurements between 0.1s-50,000s for neutron fission of {sup 235}U, {sup 238}U and {sup 239}Pu. Progress report, March 1, 1993--January 31, 1994

    Energy Technology Data Exchange (ETDEWEB)

    Schier, W.A.; Couchell, G.P.

    1994-06-01

    Decay heat measurements following the fast fission of {sup 238}U are well underway. The He-jet system and spectrometers were moved to the 1 MW research reactor to gain sufficient fast neutron flux for these measurements. On the Van de Graaff accelerator, the He-jet capillary has been shortened so that beta and gamma measurements following the thermal neutron fission of {sup 235}U could be made down to delay times near 0.1 s. Gamma-ray response functions are now well characterized for gamma energies up to 1.5 MeV for our large Nal spectrometer. Such response functions out to high energies are needed to extract energy distributions of our measured gamma spectra. The response function unfolding program, FERD-PC, has been operated successfully with trial spectra. Comparisons of individual fission products for {sup 235}U(n{sub th}f) with ENDF/B-VI at short delay times suggest several improvements to the data base particularly in production probabilities. The new data acquisition and data analysis systems have arrived and will soon be brought on line extending considerably the capabilities of our research group.

  6. Pacific Northwest Laboratory annual report for 1976 to the ERDA Assistant Administrator for Environment and Safety. Part 1. Biomedical Sciences

    Energy Technology Data Exchange (ETDEWEB)

    Thompson, R.C.

    1977-05-01

    Separate abstracts were prepared for individual sections of this publication. In addition to research reports the publication also contains organization charts, author index, and appendixes showing data on selected parameters relative to life-span dose-effect studies with inhaled /sup 239/PuO/sub 2/, /sup 238/PuO/sub 2/, and /sup 239/Pu in beagles. (HLW)

  7. Neutron scattering studies in the actinide region. Progress report, August 1, 1992--July 31, 1993

    Energy Technology Data Exchange (ETDEWEB)

    Kegel, G.H.R.; Egan, J.J.

    1993-09-01

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

  8. Design and Simulation of High Radioactivity Fission Ionization Chamber

    Institute of Scientific and Technical Information of China (English)

    WANG; Qi

    2012-01-01

    <正>It is great effect that the fission neutron release in 239Pu(n, 2n) cross section measurement by using multi-unit gadolinium loaded liquid scintillation detector system, for the 239Pu fission cross section is larger than (n, 2n) cross section one order of magnitude. In order to deduct the effect of fission neutrons,

  9. Determining Pu-239 content by resonance transmission analysis using a filtered reactor beam.

    Energy Technology Data Exchange (ETDEWEB)

    Klann, R. T.

    1998-11-25

    A novel technique has been developed at Argonne National Laboratory to determine the {sup 239}Pu content in EBR-II blanket elements using resonance transmission analysis (RTA) with a filtered reactor beam. The technique uses cadmium and gadolinium filters along with a {sup 239}Pu fission chamber to isolate the 0.3 eV resonance in {sup 239}Pu. In the energy range from 0.1 to 0.5 eV, the total microscopic cross-section of {sup 239}Pu is significantly larger than the cross-sections of {sup 238}U and {sup 235}U. This large difference in cross-section allows small amounts of {sup 239}Pu to be detected in uranium samples. Tests using a direct beam from a 250 kW TRIGA reactor have been performed with stacks of depleted uranium and {sup 239}Pu foils. Preliminary measurement results are in good agreement with the predicted results up to about two weight percent of {sup 239}Pu in the sample. In addition, measured {sup 239}Pu masses were in agreement with actual sample masses with uncertainties less than 3.8 percent.

  10. Accelerator mass spectrometry (AMS) in plutonium analysis.

    Science.gov (United States)

    Strumińska-Parulska, Dagmara I

    The paper summarizes the results of the (240)Pu/(239)Pu atomic ratio studies in atmospheric fallout samples collected in 1986 over Gdynia (Poland) as well as three Baltic fish species collected in 1997 using the accelerator mass spectrometry. A new generation of AMS has been developed during last years and this method is an efficient and good technique to measure long-lived radioisotopes in the environment and provides the most accurate determination of the atomic ratios between (240)Pu and (239)Pu. The nuclide compositions of plutonium in filter samples correspond to their means of production. AMS measurements of atmospheric fallout collected in April showed sufficient increase of the (240)Pu/(239)Pu atomic ratio from 0.28 from March to 0.47. Also such high increase of (240)Pu/(239)Pu atomic ratio, close to reactor core (240)Pu/(239)Pu atomic ratio, was observed in September and equaled 0.47.

  11. Experiments at the GELINA facility for the validation of the self-indication neutron resonance densitometry technique

    Directory of Open Access Journals (Sweden)

    Rossa Riccardo

    2017-01-01

    Full Text Available Self-Indication Neutron Resonance Densitometry (SINRD is a passive non-destructive method that is being investigated to quantify the 239Pu content in a spent fuel assembly. The technique relies on the energy dependence of total cross sections for neutron induced reaction. The cross sections show resonance structures that can be used to quantify the presence of materials in objects, e.g. the total cross-section of 239Pu shows a strong resonance close to 0.3 eV. This resonance will cause a reduction of the number of neutrons emitted from spent fuel when 239Pu is present. Hence such a reduction can be used to quantify the amount of 239Pu present in the fuel. A neutron detector with a high sensitivity to neutrons in this energy region is used to enhance the sensitivity to 239Pu. This principle is similar to self-indication cross section measurements. An appropriate detector can be realized by surrounding a 239Pu-loaded fission chamber with appropriate neutron absorbing material. In this contribution experiments performed at the GELINA time-of-flight facility of the JRC at Geel (Belgium to validate the simulations are discussed. The results confirm that the strongest sensitivity to the target material was achieved with the self-indication technique, highlighting the importance of using a 239Pu fission chamber for the SINRD measurements.

  12. SINRD validation experiments at the Time-of-Flight facility GELINA

    OpenAIRE

    ROSSA R.; ALAERTS Gery; Borella, A.; HEYSE JAN; KOPECKY Stefan; Labeau, P. E.; PARADELA DOBARRO CARLOS; Pauly, N; Schillebeeckx, Peter; van der Meer, Klaas; WYNANTS Ruud

    2016-01-01

    Self-interrogation neutron resonance densitometry (SINRD) is a non-destructive analysis technique that can be used to quantify the amount of 239Pu in spent nuclear fuel. It is a passive method that relies on the detection of neutrons, which are emitted by the fuel. The amount of 239Pu is estimated from the ratio of the neutron intensity in the fast energy region and in a region close to the 0.296 eV resonance of 239Pu. The neutron intensity in the resonance region is obtained from a detection...

  13. Influence of radiation and non-radiation factors on pancreatic cancer incidence among Mayak PA workers

    Energy Technology Data Exchange (ETDEWEB)

    Zhuntova, G.V.; Tokarskaya, Z.B.; Belyaeva, Z.D. [Southern Ural Biophysics Institute (SUBI), Ozyorsk (Russian Federation); Syrchikov, V.A.; Grigoryeva, E.S. [Mayak Production Association (Mayak PA), Ozyorsk (Russian Federation)

    2006-07-01

    The finding of this nested case-control study suggests that high levels of 239 Pu incorporation (239 Pu body burden > 3.7), alcohol abuse and smoking were associated with increasing the risk of pancreatic cancer among Mayak PA workers chronically exposed to ionizing radiation. The contribution of non radiation factors (alcohol abuse and smoking) to pancreatic tumor incidence is greater (AR=51%) than 239 Pu incorporation kBq; AR = 7%). No significant effect of external gamma rays ({<=} 6.8 Gy), prior exposure to chemical agents, or chronic digestive diseases was found on the incidence of pancreatic tumor. Evaluation of the absorbed alpha-radiation pancreatic dose will permit to make more exact the 239 Pu risk estimation in the further extended study.

  14. Plutonium in Southern Hemisphere ocean Waters

    DEFF Research Database (Denmark)

    Hirose, K.; Aoyama, M.; Gastaud, J.

    2013-01-01

    Plutonium in seawater collected by the BEAGLE2003 cruise was determined using ICP- SF-MS and alpha spectrometry after Fe co-precipitation and radiochemical purification. Levels and distributions of dissolved plutonium activity concentrations in Southern Hemisphere ocean waters are summarized here......, including historical data. Pu-239 concentrations in surface water----of the central South Pacific (32.5 °S) in 2003 were around 1 mBq/m3. The 239Pu concentrations in the Indian Ocean surface waters (20°S) were similar to that in the South Pacific, whereas the 239Pu concentrations in the South Atlantic...... surface waters (30°S) were markedly lower than those in the South Pacific and Indian Oceans. The 239Pu vertical profile pattern was similar to that in the North Pacific subtropical gyre, although 239Pu concentrations in the deep South Pacific were significantly lower than those in the North Pacific. One...

  15. Seaborg's Plutonium? A Case Study in Nuclear Forensics

    Science.gov (United States)

    Norman, Eric B.; Thomas, Keenan J.; Telhami, Kristina E.

    2015-10-01

    Passive X-ray and gamma-ray analysis was performed on UC Berkeley's EH&S Sample S338. The object was found to contain 239Pu. No other radioactive isotopes were observed. The mass of 239Pu contained in this object was determined to be 2.0 +- 0.3 μg. These observations are consistent with the identification of this object as containing the 2.77- μg PuO2 (2.44 μg 239Pu) sample produced in 1942 and described by Glenn Seaborg and his collaborators as the first sample of 239Pu that was large enough to be weighed. This work was supported in part by the U.S. Dept. of Energy National Nuclear Security Administration under Award No. DE-NA0000979.

  16. Plutonium Isotopes ((239-241)Pu) Dissolved in Pacific Ocean Waters Detected by Accelerator Mass Spectrometry: No Effects of the Fukushima Accident Observed.

    Science.gov (United States)

    Hain, Karin; Faestermann, Thomas; Fimiani, Leticia; Golser, Robin; Gómez-Guzmán, José Manuel; Korschinek, Gunther; Kortmann, Florian; Lierse von Gostomski, Christoph; Ludwig, Peter; Steier, Peter; Tazoe, Hirofumi; Yamada, Masatoshi

    2017-02-21

    The concentration of plutonium (Pu) and the isotopic ratios of (240)Pu to (239)Pu and (241)Pu to (239)Pu were determined by accelerator mass spectrometry (AMS) in Pacific Ocean water samples (20 L each) collected in late 2012. The isotopic Pu ratios are important indicators of different contamination sources and were used to identify a possible release of Pu into the ocean by the Fukushima Daiichi Nuclear Power Plant (FDNPP) accident. In particular, (241)Pu is a well-suited indicator for a recent entry of Pu because (241)Pu from fallout of nuclear weapon testings has already significantly decayed. A total of 10 ocean water samples were prepared at the Radiochemie München of the TUM and analyzed at the Vienna Environmental Research Laboratory (VERA). Several samples showed a slightly elevated (240)Pu/(239)Pu ratio of up to 0.22 ± 0.02 compared to global fallout ((240)Pu/(239)Pu = 0.180 ± 0.007), whereas all measured (241)Pu-to-(239)Pu ratios were consistent with nuclear weapon fallout ((241)Pu/(239)Pu < 2.4 × 10(-3)), which means that no impact from the Fukushima accident was detected. From the average (241)Pu-to-(239)Pu ratio of 8-2(+3) ×10(-4) at a sampling station located at a distance of 39.6 km to FDNPP, the 1-σ upper limit for the FDNPP contribution to the (239)Pu inventory in the water column was estimated to be 0.2%. Pu, with the signature of weapon-grade Pu was found in a single sample collected around 770 km off the west coast of the United States.

  17. Methodological Study on AMS Measurement of Ultra-trace Pu Isotope Ratios at CIAE

    Institute of Scientific and Technical Information of China (English)

    DONG; Ke-jun; ZHAO; Qing-zhang; WANG; Chen; HE; Ming; JIANG; Shan; ZHANG; Hui; PANG; Yi-jun; SHEN; Hong-tao; WANG; Xiao-ming; XU; Yong-ning; WU; Shao-yong; YANG; Xu-ran; WANG; Xiang-gao

    2015-01-01

    The determination of ultra-trace plutonium is very important in different fields.A new measurement method of plutonium isotopic ratios with accelerator mass spectrometry(AMS)was developed at China Institute of Atomic Energy(CIAE).Two laboratory reference standards of 239Pu/240 Pu(ST1)and 239Pu/242 Pu(ST2)are17.241and 10.059,a flow blank,a commercial blank and three real samples were respectively

  18. Neutron scattering studies in the actinide region

    Energy Technology Data Exchange (ETDEWEB)

    Beghian, L.E.; Kegel, G.H.R.

    1991-08-01

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

  19. Neutron scattering studies in the actinide region. Progress report, August 1, 1988--July 31, 1991

    Energy Technology Data Exchange (ETDEWEB)

    Beghian, L.E.; Kegel, G.H.R.

    1991-08-01

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

  20. Isotope dilution gamma spectrometry for Pu using low energy photons

    Energy Technology Data Exchange (ETDEWEB)

    Paul, S.; Sarkar, A.; Alamelu, D.; Shah, R.V.; Aggarwal, S.K. [Bhabha Atomic Reseach Centre, Mumbai (India). Fuel Chemistry Div.

    2012-07-01

    Isotope dilution gamma spectrometry (IDGS) for determination of the Pu concentration, using high resolution gamma-ray spectrometry (HRGS) in the 40-150 keV energy range, is developed and described. The methodology involves purification of Pu by an anion exchange procedure, followed by the determination of Pu isotopic composition using HRGS. For isotope dilution, a pre-calibrated power reactor grade Pu ({proportional_to} 70 at. % {sup 239}Pu) solution from an Indian PHWR was used as a spike for research reactor grade Pu ({proportional_to} 95 at. % {sup 239}Pu) samples and vice versa. Changes in {sup 240}Pu/{sup 239}Pu (45.24 keV/51.62 keV) and {sup 241}Pu/{sup 239}Pu (148.57 keV/129.29 keV) activity ratios in the spiked samples were determined by gamma spectrometry. Using the atom ratios calculated from the measured activity ratios, the concentration of Pu in the sample was calculated using two different efficiency calibration methods. The isotopic composition and concentration of Pu samples both from power reactor and research reactor grade agreed well with the values obtained by isotope dilution-thermal ionization mass spectrometry. The present method also shows the superiority of using the {sup 240}Pu/{sup 239}Pu atom ratio against the {sup 241}Pu/{sup 239}Pu atom ratio in IDGS with respect to the accuracy and precision. (orig.)

  1. Plutonium isotope ratio variations in North America

    Energy Technology Data Exchange (ETDEWEB)

    Steiner, Robert E [Los Alamos National Laboratory; La Mont, Stephen P [Los Alamos National Laboratory; Eisele, William F [Los Alamos National Laboratory; Fresquez, Philip R [Los Alamos National Laboratory; Mc Naughton, Michael [Los Alamos National Laboratory; Whicker, Jeffrey J [Los Alamos National Laboratory

    2010-12-14

    Historically, approximately 12,000 TBq of plutonium was distributed throughout the global biosphere by thermo nuclear weapons testing. The resultant global plutonium fallout is a complex mixture whose {sup 240}Pu/{sup 239}Pu atom ratio is a function of the design and yield of the devices tested. The average {sup 240}Pu/{sup 239}Pu atom ratio in global fallout is 0.176 + 014. However, the {sup 240}Pu/{sup 239}Pu atom ratio at any location may differ significantly from 0.176. Plutonium has also been released by discharges and accidents associated with the commercial and weapons related nuclear industries. At many locations contributions from this plutonium significantly alters the {sup 240}Pu/{sup 239}Pu atom ratios from those observed in global fallout. We have measured the {sup 240}Pu/{sup 239}Pu atom ratios in environmental samples collected from many locations in North America. This presentation will summarize the analytical results from these measurements. Special emphasis will be placed on interpretation of the significance of the {sup 240}Pu/{sup 239}Pu atom ratios measured in environmental samples collected in the Arctic and in the western portions of the United States.

  2. Transfer of plutonium to rat embryos in vivo and in vitro

    Energy Technology Data Exchange (ETDEWEB)

    Takahashi, Sentaro; Sato, Hiroshi; Kubota, Yoshihisa; Inaba, Jiro (National Inst. of Radiological Sciences, Chiba (Japan))

    1992-12-01

    The [sup 239]Pu distribution in the 12.5-day-old rat conceptus was compared between in vivo and in vitro experimental systems to establish a possible mechanism of cross-palcental transfer of this radionuclide. In the in vivo study, plutonium citrate solution was injected intravenously to pregnant Wistar rats. In the in vitro study, either plutonium citrate or plutonium hydroxide colloid was administered, as a solution of Eagle MEM and FCS containing [sup 239]Pu at the concentration used in the maternal serum in the in vivo experiments, to rat conceptuses maintained by the whole-embryo culture method. The concentration of [sup 239]Pu in the yolk sac ([sup 239]Pu activity per gram wet weight) were much higher than in the embryo in both the in vivo and in vitro experiments, suggesting that the yolk sac may be an effective barrier against the transfer of plutonium to the embryos. The ratios of the [sup 239]Pu concentration in the yolk sac to that in the embryo were relatively constant with time after administration in the in vitro system; 18-27 for plutonium citrate and 67-84 for plutonium hydroxide. In the in vivo experiment, these ratios changed with time after injection; 15 at 5 min and 62 and 60 min after injection. This suggests that in the in vivo system, the chemical form of [sup 239]Pu changed with time after injection, probably to a macromolecular form such as the hydroxide colloid or plutonium-protein complex although [sup 239]Pu was injected to the maternal blood as citrate. (author).

  3. Multimedia contaminant environmental exposure assessment methodology as applied to Los Alamos, New Mexico

    Energy Technology Data Exchange (ETDEWEB)

    Whelan, G.; Thompson, F.L.; Yabusaki, S.B.

    1983-02-01

    The MCEA (Multimedia Contaminant Environmental Exposure Assessment) methodology assesses exposures to air, water, soil, and plants from contaminants released into the environment by simulating dominant mechanisms of contaminant migration and fate. The methodology encompasses five different pathways (i.e., atmospheric, terrestrial, overland, subsurface, and surface water) and combines them into a highly flexible tool. The flexibility of the MCEA methodology is demonstrated by encompassing two of the pathways (i.e., overland and surface water) into an effective tool for simulating the migration and fate of radionuclides released into the Los Alamos, New Mexico region. The study revealed that: (a) the /sup 239/Pu inventory in lower Los Alamos Canyon increased by approximately 1.1 times for the 50-y flood event; (b) the average contaminant /sup 239/Pu concentrations (i.e., weighted according to the depth of the respective bed layer) in lower Los Alamos Canyon for the 50-y flood event decreased by 5.4%; (c) approx. 27% of the total /sup 239/Pu contamination resuspended from the entire bed (based on the assumed cross sections) for the 50-y flood event originated from lower Pueblo Canyon; (d) an increase in the /sup 239/Pu contamination of the bed followed the general deposition patterns experienced by the sediment in Pueblo-lower Los Alamos Canyon; likewise, a decrease in the /sup 239/Pu contamination of the bed followed general sediment resuspension patterns in the canyon; (e) 55% of the /sup 239/Pu reaching the San Ildefonso Pueblo in lower Los Alamos Canyon originated from lower Los Alamos Canyon; and (f) 56% of the /sup 239/Pu contamination reaching the San Ildefonso Pueblo in lower Los Alamos Canyon was carried through towards the Rio Grande. 47 references, 41 figures, 29 tables.

  4. Possible differences in biological availability of isotopes of plutonium: Report of a workshop

    Energy Technology Data Exchange (ETDEWEB)

    Kercher, J.R.; Gallegos, G.M. [eds.

    1993-09-01

    This paper presents the results of a workshop conducted on the apparent different bioavailability of isotopes {sup 238}Pu and {sup 239}Pu. There is a substantial body of evidence that {sup 238}Pu as commonly found in the environment is more biologically available than {sup 239}Pu. Studies of the Trinity Site, Nevada Test Site from nonnuclear and nuclear events, Rocky Flats, Enewetak and Bikini, and the arctic tundra support this conclusion and indicate that the bioavailability of {sup 238}Pu is more than an order of magnitude greater than that of {sup 239}Pu. Plant and soil studies from controlled environments and from Savannah River indicate no isotopic difference in availability of Pu to plants; whereas studies at the Trinity Site do suggest a difference. While it is possible that these observations can be explained by problems in the experimental procedure and analytical techniques, this possibility is remote given the ubiquitous nature of the observations. Studies of solubility of Pu in the stomach contents of cattle grazing at the Nevada Test Site and from fish from Bikini Atoll both found that {sup 238}Pu was more soluble than {sup 239}Pu. Studies of the Los Alamos effluent stream indicate that as particle size decreases, the content of {sup 238}Pu relative to {sup 239}Pu increases.

  5. Performance characteristics of a Bioassay method for plutonium using thermal ionisation mass spectrometry (TIMS)

    Energy Technology Data Exchange (ETDEWEB)

    Linauskas, S.H.; Elliot, N.L.; Paterson, L.M.; Totland, M.M

    2003-01-01

    Plutonium-in-urine analysis by radiochemical isolation of Pu followed by thermal ionisation mass spectrometry (TIMS) is capable of high sensitivity and precision measurements {sup 239}Pu and {sup 240}Pu. Bias and precision estimates for the TIMS bioassay program at Chalk River Laboratories easily met the ANSI N13.30 performance criteria standards with {sup 239}Pu results of 1.5% and 3.0%, respectively. Analytical blanks derived from water, artificial urine and true urine samples did not produce any statistically different results. During a four-year period of development and implementation of {sup 239}Pu measurements by TIMS, average sample blank values were reduced from 3.9 fg (9.0 {mu}Bq) to 0.57 fg (1.3 {mu}Bq). This reduction was achieved through rigorous application of clean-room handling techniques throughout sample processing. Blank data were found to follow a Iognormal distribution, and current detection limit parameters for L{sub c} and L{sub d} at the 95% significance levels are 0.85 fg {sup 239}Pu (2.0 {mu}Bq) and 1.3 fg {sup 239}Pu (3.0 {mu}Bq), respectively. Detection limits in this range are expected to be sufficient to identify intakes of Pu/Am mixtures at levels that are around one-twentieth of an ALl or better under routine monitoring situations for ICRP Type S and Type M inhalation solubility classes. (author)

  6. Transport and scavenging of Pu in surface waters of the Southern Hemisphere Oceans

    DEFF Research Database (Denmark)

    Gastaud, J.; Povinec, P.P.; Aoyama, M.

    2011-01-01

    The distribution of 239Pu in Atlantic and Indian Ocean waters about four decades after their main injection from atmospheric nuclear weapons tests is discussed. Recent data obtained in the framework of the SHOTS (Southern Hemisphere Ocean Tracer Studies) projects are evaluated and compared...... with previous investigations. Seawater samples were collected during the round the globe BEAGLE2003 (Blue Ocean Global Expedition) along the 30°S transect in the Atlantic and the 20°S transect in the Indian Ocean. The results indicate transport of surface waters labelled with 239Pu from the western North...... Pacific via the Indonesian Seas to the South Indian Ocean and then to the South Atlantic Ocean. Along the whole BEAGLE2003 sampling route, the Atlantic Ocean has the lowest 239Pu content due to its particle scavenging on the long way from the western North Pacific. On the other hand, concentrations...

  7. Assessment of Degree of Applicability of Benchmarks for Gadolinium Using KENO V.a and the 238-Group SCALE Cross-Section Library

    Energy Technology Data Exchange (ETDEWEB)

    Goluoglu, S.

    2003-12-01

    A review of the degree of applicability of benchmarks containing gadolinium using the computer code KENO V.a and the gadolinium cross sections from the 238-group SCALE cross-section library has been performed for a system that contains {sup 239}Pu, H{sub 2}O, and Gd{sub 2}O{sub 3}. The system (practical problem) is a water-reflected spherical mixture that represents a dry-out condition on the bottom of a sludge receipt and adjustment tank around steam coils. Due to variability of the mixture volume and the H/{sup 239}Pu ratio, approximations to the practical problem, referred to as applications, have been made to envelop possible ranges of mixture volumes and H/{sup 239}Pu ratios. A newly developed methodology has been applied to determine the degree of applicability of benchmarks as well as the penalty that should be added to the safety margin due to insufficient benchmarks.

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

    Energy Technology Data Exchange (ETDEWEB)

    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.

  9. Compilation of multigroup cross-section covariance matrices for several important reactor materials

    Energy Technology Data Exchange (ETDEWEB)

    Drischler, J.D.; Weisbin, C.R.

    1977-10-01

    Multigroup cross-section covariance matrices are presented for fission in /sup 235/U, /sup 238/U, /sup 239/Pu, and /sup 241/Pu; capture in /sup 235/U, /sup 238/U, /sup 239/Pu, /sup 240/Pu, and /sup 241/Pu; fission neutron yield (anti nu) for /sup 235/U, /sup 238/U, /sup 239/Pu, and /sup 240/Pu; elastic scattering for Na and Fe; non-elastic reactions for Na and Fe; first-level inelastic scattering for /sup 238/U; and all reactions provided in the ENDF/B-IV covariance description of N, O, and C. Other data files generated are included for reference but have not yet been tested. The report presents the nultigroup data in six, ten, and fifteen energy group forms corresponding to weighting of the covariance data with fission (GODIVA), LMFBR (ZPR-6/7) and 1/E spectra, respectively.

  10. Subchronic inhalation of carbon tetrachloride alters the tissue retention of acutely inhaled plutonium-239 nitrate in F344 rats and syrian golden hamsters

    Energy Technology Data Exchange (ETDEWEB)

    Benson, J.M.; Barr, E.B.; Lundgren, D.L. [and others

    1995-12-01

    Carbon tetrachloride (CCl{sub 4}) has been used extensively in the nuclear weapons industry, so it is likely that nuclear plant workers have been exposed to both CCl{sub 4} and plutonium compounds. Future exposures may occur during {open_quotes}cleanup{close_quotes} operations at weapons productions sites such as the Hanford, Washington, and Rocky Flats, Colorado, facilities. Inhalation of 20 and 100 ppm CCl{sub 4} by hamsters reduces uptake of {sup 239}Pu solubilized from lung, shunting the {sup 239}Pu to the skeleton.

  11. Plutonium uptake by the green alga Scenedesmus obliquus (Turp) Kutz, as a function of isotope and oxidation state

    Energy Technology Data Exchange (ETDEWEB)

    Tkacik, M.F.

    1977-01-01

    This study was designed to determine the effect of plutonium chemical valence state on the availability of small concentrations of /sup 238/Pu and /sup 239/Pu to algae. The uptake experiments involved the green alga Scenedesmus obliquus, grown in batch cultures. Plutonium concentrations accumulated by this alga were linearly related to plutonium concentrations. There was no significant difference (rho = 0.05) in algal plutonium accumulations, on a mass basis, of either /sup 238/Pu or /sup 239/Pu in either Pu/sup +4/ or Pu/sup +6/ oxidation state at the concentrations studied.

  12. Active and passive CT for waste assay using LaBr3(Ce) detector

    Science.gov (United States)

    Roy, Tushar; More, M. R.; Ratheesh, Jilju; Sinha, Amar

    2017-01-01

    An active and passive computed tomography system has been developed that localizes and quantifies 239Pu in a waste drum. The active (transmission) measurement uses an external gamma source and LaBr3(Ce) detector to determine the attenuation map of waste drum contents at different selected energies. The passive (emission) measurement uses multiple LaBr3(Ce) detectors to record the spectra of gamma-rays emitted from within the drum. The active and passive data sets are then coupled to quantitatively assay drum contents for 239Pu.

  13. Proceedings of the Task 4 Waste Isolation Safety Assessment Program second contractor information meeting

    Energy Technology Data Exchange (ETDEWEB)

    None

    1978-01-01

    Volume 1 contains the following papers: Solution Species of {sup 239}Pu in Oxidizing Environments; Solution Species of {sup 239}Pu in the Environment; Theoretical and Experimental Evaluation of Waste Transport in Selected Rocks; Studies of Radionuclide Availability and Migration at the Nevada Test Site Relevant to Radioactive Waste Disposal; Systematic Study of Metal Ion Sorption on Selected Geologic Media; Chromatographic K/sub d/ values of Radionuclides; Effects of Redox Potentials on Sorption of Radionuclides by Geologic Media; and Transport Properties of Nuclear Waste in Geologic Media. Individual papers were processed.

  14. STEW: A Nonlinear Data Modeling Computer Program

    Energy Technology Data Exchange (ETDEWEB)

    Chen, H.

    2000-03-04

    A nonlinear data modeling computer program, STEW, employing the Levenberg-Marquardt algorithm, has been developed to model the experimental {sup 239}Pu(n,f) and {sup 235}U(n,f) cross sections. This report presents results of the modeling of the {sup 239}Pu(n,f) and {sup 235}U(n,f) cross-section data. The calculation of the fission transmission coefficient is based on the double-humped-fission-barrier model of Bjornholm and Lynn. Incident neutron energies of up to 5 MeV are considered.

  15. Intercalibration of selected anthropogenic radionuclides for the GEOTRACES Program

    DEFF Research Database (Denmark)

    Kenna, Timothy C.; Masqué, Pere; Mas, Jose Luis

    2012-01-01

    As part of the GEOTRACES Program, six laboratories participated in an intercalibration exercise on several anthropogenic radionuclides of interest. The effort was successful for 239,240Pu activity, 240Pu/239Pu isotope ratio, and 137Cs activity measured in filtered seawater samples from the Bermud...

  16. Variations in Pu isotopic composition in soils from the Spitsbergen (Norway): Three potential pollution sources of the Arctic region.

    Science.gov (United States)

    Łokas, E; Anczkiewicz, R; Kierepko, R; Mietelski, J W

    2017-07-01

    Although the polar regions have not been industrialised, numerous contaminants originating from human activity are detectable in the Arctic environment. This study reports evidence of (240)Pu/(239)Pu atomic ratios in the tundra and initial soils from different parts of west and central Spitsbergen and recognizes possible environmental inputs of non-global fallout Pu. The average atomic ratio of (240)Pu/(239)Pu equal to 0.179 (ranging between 0.129 and 0.201) in tundra soils are comparable to the characteristic ratio for global fallout (0.180). However, the (240)Pu/(239)Pu atomic ratios in the initial soils from proglacial zone of glaciers change within wide range between 0.1281 and 0.234 with the mean value of 0.169. By combining alpha and mass spectrometry, the three-sources model was used to identify the Pu sources in initial soils. Our study indicated that the main source of Pu is nuclear tests and that a second source with lower Pu ratio may come from weapons grade Pu (unexploded weapons grade Pu ie. material from bomb which didn't undergo nuclear explosions for example for security tests). Additionally, we found samples with high (238)Pu/(239+240)Pu activity ratios and with typical global fallout (240)Pu/(239)Pu atomic ratios, which are associated with separate sources of pure (238)Pu from the SNAP-9A satellite burn up in the atmosphere. Copyright © 2017 Elsevier Ltd. All rights reserved.

  17. Studies of Np and Pu in the marine environment of Swedish-Danish waters and the North Atlantic Ocean.

    Science.gov (United States)

    Lindahl, Patric; Roos, Per; Holm, Elis; Dahlgaard, Henning

    2005-01-01

    The long-lived anthropogenic radionuclides (237)Np, (239)Pu and (240)Pu were determined in marine environmental samples (seaweed and seawater) collected from Swedish-Danish waters and the North Atlantic Ocean at various locations on different occasions during the period 1991-2001. The measurements were performed with sector field Inductively Coupled Plasma Mass Spectrometry (ICP-MS) and conventional alpha spectrometry. The (237)Np activity concentrations in Fucus vesiculosus and surface seawater from the Swedish west coast and Danish waters ranged from 0.16+/-0.02 to 1.02+/-0.09 mBq kg(-1) (dry weight) and 0.65+/-0.02 to 1.69+/-0.02 mBq m(-3), respectively, depending on the location and sampling year. Most of the (237)Np in these waters is believed to originate from the Sellafield nuclear reprocessing plant, with some contribution from global fallout. The (240)Pu/(239)Pu atomic ratios in F. vesiculosus samples are reported in this study with an overall average of 0.17+/-0.03. The (237)Np and (239)Pu activity concentrations observed in surface seawater collected in North Atlantic waters ranged from 0.16+/-0.01 to 0.62+/-0.08 mBq m(-3) and from 0.64+/-0.05 to 4.27+/-0.08 mBq m(-3), respectively, and the (237)Np/(239)Pu atomic ratios were a good indicator of conservative behaviour of Np in marine waters.

  18. Progress of China Experimental Fast Reactor in 2011

    Institute of Scientific and Technical Information of China (English)

    2011-01-01

    1 Background Fast reactor is the reactor which realized the chain fission with fast neutron.As an optional type of generation Ⅳ reactor,fast reactor has three characters:1) It can change 238U to 239Pu and raise the uranium resource utilization

  19. Plutonium in Soils from Northeast China and Its Potential Application for Evaluation of Soil Erosion

    DEFF Research Database (Denmark)

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

    2013-01-01

    Surface and soil core samples from northeast China were analyzed for Pu isotopes. The measured 240Pu/239Pu atomic ratios and 239 1 240Pu/137Cs activity ratios revealed that the global fallout is the dominant source of Pu and 137Cs at these sites. Migration behavior of Pu varying with land type an...

  20. National Low-Level Waste Management Program Radionuclide Report Series, Volume 17: Plutonium-239

    Energy Technology Data Exchange (ETDEWEB)

    J. P. Adams; M. L. Carboneau

    1999-03-01

    This report, Volume 17 of the National Low-Level Waste Management Program Radionuclide Report Series, discusses the radiological and chemical characteristics of plutonium-239 (Pu-239). This report also discusses waste types and forms in which Pu-239 can be found, waste and disposal information on Pu-239, and Pu-239 behavior in the environment and in the human body.

  1. A multiple sampling ionization chamber for the External Target Facility

    Science.gov (United States)

    Zhang, X. H.; Tang, S. W.; Ma, P.; Lu, C. G.; Yang, H. R.; Wang, S. T.; Yu, Y. H.; Yue, K.; Fang, F.; Yan, D.; Zhou, Y.; Wang, Z. M.; Sun, Y.; Sun, Z. Y.; Duan, L. M.; Sun, B. H.

    2015-09-01

    A multiple sampling ionization chamber used as a particle identification device for high energy heavy ions has been developed for the External Target Facility. The performance of this detector was tested with a 239Pu α source and RI beams. A Z resolution (FWHM) of 0.4-0.6 was achieved for nuclear fragments of 18O at 400 AMeV.

  2. Analysis Method of 241Pu Radioactivity by Isotope Dilution-Extraction Liquid Scintillation Spectrometer

    Institute of Scientific and Technical Information of China (English)

    2008-01-01

    <正>241Pu is the only pure β emitter with the maximum energy of 20.81 keV in plutonium isotopes of 238Pu, 239Pu, 240Pu and 242Pu, in which 241Pu is mostly specific radioactivity because its half-life is 14.29 a.

  3. Neutrinos and Non-proliferation in Europe

    CERN Document Server

    Cribier, Michel

    2006-01-01

    Triggered by the demand of the IAEA, neutrino physicists in Europe involved with the Double Chooz experiment are studying the potential of neutrino detection to monitor nuclear reactors. In particular a new set of experiments at the ILL is planned to improve the knowledge of the neutrino spectrum emitted in the fission of 235U and 239Pu.

  4. Historical changes in 239Pu and 240Pu sources in sedimentary records in the East China Sea: Implications for provenance and transportation

    DEFF Research Database (Denmark)

    Wang, Jinlong; Baskaran, Mark; Hou, Xiaolin

    2017-01-01

    Concentrations and isotopic compositions of plutonium (Pu) are widely used for its source identification and to determine transport processes of Pu-associated particulate matter and water. We investigated the concentrations of 239Pu and 240Pu and their ratios in a number of sediment samples from...

  5. Time-resolved record of (236)U and (239,240)Pu isotopes from a coral growing during the nuclear testing program at Enewetak Atoll (Marshall Islands).

    Science.gov (United States)

    Froehlich, M B; Chan, W Y; Tims, S G; Fallon, S J; Fifield, L K

    2016-12-01

    A comprehensive series of nuclear tests were carried out by the United States at Enewetak Atoll in the Marshall Islands, especially between 1952 and 1958. A Porites Lutea coral that was growing in the Enewetak lagoon within a few km of all of the high-yield tests contains a continuous record of isotopes, which are of interest (e.g. (14)C, (236)U, (239,240)Pu) through the testing period. Prior to the present work, (14)C measurements at ∼2-month resolution had shown pronounced peaks in the Δ(14)C data that coincided with the times at which tests were conducted. Here we report measurements of (236)U and (239,240)Pu on the same coral using accelerator mass spectrometry, and again find prominent peaks in the concentrations of these isotopes that closely follow those in (14)C. Consistent with the (14)C data, the magnitudes of these peaks do not, however, correlate well with the explosive yields of the corresponding tests, indicating that smaller tests probably contributed disproportionately to the debris that fell in the lagoon. Additional information about the different tests can also be obtained from the (236)U/(239)Pu and (240)Pu/(239)Pu ratios, which are found to vary dramatically over the testing period. In particular, the first thermonuclear test, Ivy-Mike, has characteristic (236)U/(239)Pu and (240)Pu/(239)Pu signatures which are diagnostic of the first arrival of nuclear test material in various archives.

  6. Rapid and simultaneous determination of neptunium and plutonium isotopes in environmental samples by extraction chromatography using sequential injection analysis and ICP-MS

    DEFF Research Database (Denmark)

    Qiao, Jixin; Hou, Xiaolin; Roos, Per

    2010-01-01

    This paper reports an automated analytical method for rapid and simultaneous determination of plutonium isotopes (239Pu and 240Pu) and neptunium (237Np) in environmental samples. An extraction chromatographic column packed with TrisKem TEVA® resin was incorporated in a sequential injection (SI...

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

    DEFF Research Database (Denmark)

    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...

  8. Determination of plutonium isotopes in seawater reference materials using isotope-dilution ICP-MS.

    Science.gov (United States)

    Zheng, Jian; Yamada, Masatoshi

    2012-09-01

    We analyzed the activities of (239)Pu, (240)Pu, (239+240)Pu, (241)Pu, the ratio of number of atoms (atom ratio) for (240)Pu/(239)Pu, and the activity ratio of (241)Pu/(239+240)Pu in seawater reference materials, IAEA-443 and IAEA-381, using a highly sensitive isotope dilution sector field inductively coupled plasma mass spectrometry method. With a mean chemical yield of 65% determined with (242)Pu as a tracer, we found that the experimentally established values in IAEA-443 for (239)Pu, (240)Pu, (241)Pu and (239+240)Pu activities are almost the same as those in IAEA-381. Regarding the (239+240)Pu activity, we provided the most precise and accurate result among the twelve laboratories, which participated in the interlaboratory comparison. In addition, for the (240)Pu/(239)Pu atom ratio, our results for IAEA-381 (0.2315±0.0008) and IAEA-443 (0.2325±0.0008) are in good agreement with the IAEA information value (0.229±0.006), but have much smaller uncertainty. Since the new seawater reference material, IAEA-443, is commercially available, it can be used not only for method validation for seawater plutonium isotope ratio and activity analysis, but also for more general use as a plutonium isotope standard for mass discrimination correction for other environmental samples.

  9. Analysis of Sub-picogram Plutonium by Isotope Mass Spectrometry%亚皮克量级钚的质谱分析技术

    Institute of Scientific and Technical Information of China (English)

    龙开明; 汤磊; 贾宝亭; 刘雪梅; 杨天丽; 刘钊

    2005-01-01

    By using active carbon powder as ionization enhance matter, the detect sensitivity of 239Pu ,which was 0.5 pg (1±0.15, 95% confidence level), was about 20 times that of the tradition method. The sub-picogram plutonium sample was determined quantitatively by isotope dilution mass spectrometry (IDMS).

  10. Some considerations for comparing risk of radiation and chemicals

    Energy Technology Data Exchange (ETDEWEB)

    Yang Huating [China Institute for Radiation Protection, Taiyuan, Shanxi (China)

    2000-05-01

    Some basic concepts, used in radiation protection, are tried to be applied to the assessment of risks of environmental chemicals with the necessary variations. Dioxins may serve as an intermedium for the comparison of radiation and other chemicals. The death risk of dioxin induced cancers in life is 4.7x10{sup -4}, based on the intake of 1 pg/kg/day by using additive model and extrapolating linearly the results of the epidemiological study. And the risk is 2.6x10{sup -4} in life by multiplicative model. The death risk of radiation induced cancer is 4x10{sup -5}/a to the effective dose of 1 mSv/a for adult. Ingestion of 1 Bq of {sup 239}Pu will give rise to a committed effective dose of 2.5x10{sup -7} Sv, therefore, yearly ingestion of 1.47x10{sup -6} g of {sup 239}Pu is corresponding to 1 mSv/a. A definition of risk per year over mass ingested per year (1/{mu}g) may be suitable for the comparison of yearly risk of yearly-ingested masses of dioxins and {sup 239}Pu. The life expectancy and a reference body weight (averaged weights of man and woman adults) are chosen as 70 years and 64 kg respectively. The risks caused by ingestion of unit mass dioxin and {sup 239}Pu are given as follows: 2.87x10{sup -4}/{mu}g (2,3,7,8-TCDD, additive model), 1.69x10{sup -4}/{mu}g (2,3,7,8-TCDD, multiplicative model) and 2.3x10{sup -5}/{mu}g ({sup 239}Pu). These results show that dioxins are even riskier. The comparison among dioxins and other chemicals may be relatively easier. (author)

  11. Ultra-trace plutonium determination in small volume seawater by sector field inductively coupled plasma mass spectrometry with application to Fukushima seawater samples.

    Science.gov (United States)

    Bu, Wenting; Zheng, Jian; Guo, Qiuju; Aono, Tatsuo; Tagami, Keiko; Uchida, Shigeo; Tazoe, Hirofumi; Yamada, Masatoshi

    2014-04-11

    Long-term monitoring of Pu isotopes in seawater is required for assessing Pu contamination in the marine environment from the Fukushima Dai-ichi Nuclear Power Plant accident. In this study, we established an accurate and precise analytical method based on anion-exchange chromatography and SF-ICP-MS. This method was able to determine Pu isotopes in seawater samples with small volumes (20-60L). The U decontamination factor was 3×10(7)-1×10(8), which provided sufficient removal of interfering U from the seawater samples. The estimated limits of detection for (239)Pu and (240)Pu were 0.11fgmL(-1) and 0.08fgmL(-1), respectively, which corresponded to 0.01mBqm(-3) for (239)Pu and 0.03mBqm(-3) for (240)Pu when a 20L volume of seawater was measured. We achieved good precision (2.9%) and accuracy (0.8%) for measurement of the (240)Pu/(239)Pu atom ratio in the standard Pu solution with a (239)Pu concentration of 11fgmL(-1) and (240)Pu concentration of 2.7fgmL(-1). Seawater reference materials were used for the method validation and both the (239+240)Pu activities and (240)Pu/(239)Pu atom ratios agreed well with the expected values. Surface and bottom seawater samples collected off Fukushima in the western North Pacific since March 2011 were analyzed. Our results suggested that there was no significant variation of the Pu distribution in seawater in the investigated areas compared to the distribution before the accident.

  12. Neutron absorbers and detector types for spent fuel verification using the self-interrogation neutron resonance densitometry

    Energy Technology Data Exchange (ETDEWEB)

    Rossa, Riccardo, E-mail: rrossa@sckcen.be [SCK-CEN, Belgian Nuclear Research Centre, Boeretang, 200, B2400 Mol (Belgium); Université libre de Bruxelles, Ecole polytechnique de Bruxelles, Service de Métrologie Nucléaire (CP 165/84), Avenue F.D. Roosevelt, 50, B1050 Brussels (Belgium); Borella, Alessandro, E-mail: aborella@sckcen.be [SCK-CEN, Belgian Nuclear Research Centre, Boeretang, 200, B2400 Mol (Belgium); Labeau, Pierre-Etienne, E-mail: pelabeau@ulb.ac.be [Université libre de Bruxelles, Ecole polytechnique de Bruxelles, Service de Métrologie Nucléaire (CP 165/84), Avenue F.D. Roosevelt, 50, B1050 Brussels (Belgium); Pauly, Nicolas, E-mail: nipauly@ulb.ac.be [Université libre de Bruxelles, Ecole polytechnique de Bruxelles, Service de Métrologie Nucléaire (CP 165/84), Avenue F.D. Roosevelt, 50, B1050 Brussels (Belgium); Meer, Klaas van der, E-mail: kvdmeer@sckcen.be [SCK-CEN, Belgian Nuclear Research Centre, Boeretang, 200, B2400 Mol (Belgium)

    2015-08-11

    The Self-Interrogation Neutron Resonance Densitometry (SINRD) is a passive non-destructive assay (NDA) technique that is proposed for the direct measurement of {sup 239}Pu in a spent fuel assembly. The insertion of neutron detectors wrapped with different neutron absorbing materials, or neutron filters, in the central guide tube of a PWR fuel assembly is envisaged to measure the neutron flux in the energy region close to the 0.3 eV resonance of {sup 239}Pu. In addition, the measurement of the fast neutron flux is foreseen. This paper is focused on the determination of the Gd and Cd neutron filters thickness to maximize the detection of neutrons within the resonance region. Moreover, several detector types are compared to identify the optimal condition and to assess the expected total neutron counts that can be obtained with the SINRD measurements. Results from Monte Carlo simulations showed that ranges between 0.1–0.3 mm and 0.5–1.0 mm ensure the optimal conditions for the Gd and Cd filters, respectively. Moreover, a {sup 239}Pu fission chamber is better suited to measure neutrons close to the 0.3 eV resonance and it has the highest sensitivity to {sup 239}Pu, in comparison with a {sup 235}U fission chamber, with a {sup 3}He proportional counter, and with a {sup 10}B proportional counter. The use of a thin Gd filter and a thick Cd filter is suggested for the {sup 239}Pu and {sup 235}U fission chambers to increase the total counts achieved in a measurement, while a thick Gd filter and a thin Cd filter are envisaged for the {sup 3}He and {sup 10}B proportional counters to increase the sensitivity to {sup 239}Pu. We concluded that an optimization process that takes into account measurement time, filters thickness, and detector size is needed to develop a SINRD detector that can meet the requirement for an efficient verification of spent fuel assemblies.

  13. Temporal record of Pu isotopes in inter-tidal sediments from the northeastern Irish Sea

    Energy Technology Data Exchange (ETDEWEB)

    Lindahl, Patric, E-mail: patriclindahl@yahoo.com [School of Geography, Earth and Environmental Sciences, University of Plymouth, Drake Circus, Plymouth PL4 8AA (United Kingdom); Worsfold, Paul; Keith-Roach, Miranda [School of Geography, Earth and Environmental Sciences, University of Plymouth, Drake Circus, Plymouth PL4 8AA (United Kingdom); Andersen, Morten B. [Bristol Isotope Group, School of Earth Sciences, University of Bristol, Wills Memorial Building, Bristol BS8 1RJ (United Kingdom); Kershaw, Peter; Leonard, Kins [The Centre for Environment, Fisheries and Aquaculture Science, Lowestoft Laboratory, Pakefield Road, Suffolk NR33 0HT (United Kingdom); Choi, Min-Seok [Division of Earth and Environmental Science, Korea Basic Science Institute, 113 Gwahangno, Yusung-gu, Daejon 305-333 (Korea, Republic of); Boust, Dominique [Laboratoire de Radioecologie, Institut de Radioprotection et de Surete Nucleaire, BP 10, 50130 Cherbourg-Octeville (France); Lesueur, Patrick [University of Caen Basse Normandie, M2C UMR CNRS 6143, 14000 Caen (France)

    2011-11-01

    A depth profile of {sup 239}Pu and {sup 240}Pu specific activities and isotope ratios was determined in an inter-tidal sediment core from the Esk Estuary in the northeastern Irish Sea. The study site has been impacted with plutonium through routine radionuclide discharges from the Sellafield nuclear reprocessing plant in Cumbria, NW England. A pronounced sub-surface maximum of {approx} 10 kBq kg{sup -1} was observed for {sup 239+240}Pu, corresponding to the peak in Pu discharge from Sellafield in 1973, with a decreasing trend with depth down to {approx} 0.04 kBq kg{sup -1} in the deeper layers. The depth profile of {sup 239+240}Pu specific activities together with results from gamma-ray spectrometry for {sup 137}Cs and {sup 241}Am was compared with reported releases from the Sellafield plant in order to estimate a reliable sediment chronology. The upper layers (1992 onwards) showed higher {sup 239+240}Pu specific activities than would be expected from the direct input of annual Sellafield discharges, indicating that the main input of Pu is from the time-integrated contaminated mud patch of the northeastern Irish Sea. The {sup 240}Pu/{sup 239}Pu atom ratios ranged from {approx} 0.03 in the deepest layers to > 0.20 in the sub-surface layers with an activity-weighted average of 0.181. The decreasing {sup 240}Pu/{sup 239}Pu atom ratio with depth reflects the changing nature of operations at the Sellafield plant from weapons-grade Pu production to reprocessing spent nuclear fuel with higher burn-up times in the late 1950s. In addition, recent annual {sup 240}Pu/{sup 239}Pu atom ratios in winkles collected during 2003-2008 from three stations along the Cumbrian coastline showed no significant spatial or temporal differences with an overall average of 0.204, which supports the hypothesis of diluted Pu input from the contaminated mud patch. - Highlights: {yields} Depth profiles of {sup 239}Pu and {sup 240}Pu determined in a northeastern Irish Sea sediment. {yields

  14. Verification of plutonium content in spent fuel assemblies using neutron self-interrogation

    Energy Technology Data Exchange (ETDEWEB)

    Menlove, Howard O [Los Alamos National Laboratory; Menlove, Apencer H [Los Alamos National Laboratory; Tobin, Stephen J [Los Alamos National Laboratory

    2009-01-01

    The large amounts of plutonium in reactor spent fuel assemblies has led to increased research directed toward the measurement of the plutonium for safeguards verification. The high levels of fission product gamma-ray activity and curium neutron backgrounds have made the plutonium measurement difficult. We have developed a new technique that can directly measure both the {sup 235}U concentration and the plutonium fissile concentration using the intrinsic neutron emission fronl the curium in the fuel assembly. The passive neutron albedo reactivity (PNAR) method has been described previously where the curium neutrons are moderated in the surrounding water and reflect back into the fuel assembly to induce fissions in the fissile material in the assembly. The cadmium (Cd) ratio is used to separate the spontaneous fission source neutrons from the reflected thermal neutron fission reactions. This method can measure the sum of the {sup 235}U and the plutonium fissile mass, but not the separate components. Our new differential die-away self-interrogation method (DDSI) can be used to separate the {sup 235}U from the {sup 239}Pu. The method has been applied to both fuel rods and full assemblies. For fuel rods the epi-thermal neutron reflection method filters the reflected neutrons through thin Cd filters so that the reflected neutrons are from the epi-cadmium energy region. The neutron fission energy response in the epi-cadmium region is distinctly different for {sup 235}U and {sup 239}Pu. We are able to measure the difference between {sup 235}U and {sup 239}Pu by sampling the neutron induced fission rate as a function of time and multiplicity after the initial fission neutron is detected. We measure the neutron fission rate using list-mode data collection that stores the time correlations between all of the counts. The computer software can select from the data base the time correlations that include singles, doubles, and triples. The die-away time for the doubles

  15. Parity violation in ternary fission

    Science.gov (United States)

    Gönnenwein, F.; Belozerov, A. V.; Beda, A. G.; Burov, S. I.; Danilyan, G. V.; Martem'yanov, A. N.; Pavlov, V. S.; Shchenev, V. A.; Bondarenko, L. N.; Mostovoĭ, Yu. A.; Geltenbort, P.; Last, J.; Schreckenbach, K.

    1994-01-01

    The parity-violating correlation between incoming neutron spin and fragment momentum has been measured simultaneously for binary and ternary fission of 233U(n, f) and 239Pu(n, f). The experiment has been performed with a polarized cold neutron beam of the Institut Laue-Langevin in Grenoble/France. The ratios of the parity-violating asymmetry coefficients, α ternf and α binnf, for ternary and binary fission, respectively, are found to be {α ternf}/{α binnf = 1.05 ± 0.10 } and 1.12 ± 0.08 for the 233U and 239Pu target nucleus, respectively. Both experiments are compatible with {α ternf}/{α binnf = 1 }. The implications of this result for models of ternary fission are discussed. The conclusion drawn is that ternary particles are emitted at the very last stage of fission.

  16. The Geochemical Behaviour of Tc, Np, and Pu in Spent Nuclear Fuel in an Oxidizing Environment

    Energy Technology Data Exchange (ETDEWEB)

    Buck, Edgar C.; Hanson, Brady D.; McNamara, Bruce K.; R. Giere and P. Stille

    2004-10-01

    Studies at the Nopal and Shinkolowbwe uranium deposits show that the primary uraninite (UO2) altered to a suite of secondary uranyl minerals similar to those observed in corrosion tests with uranium oxide . Although the Nopal I deposit tells us something about the possible fate of uranium, it tells us little about the likely fate of the important long-lived radionuclides; iodine (129I), cesium (135Cs), technetium (99Tc), neptunium (237Np), and plutonium (239Pu). Most performance assessment (PA) models, assume conservatively, that as the UO2 matrix corrodes, the key radionuclides (129I, 99Tc, 237Np, and 239Pu) will be released congruently. In so doing, these PA models force increased reliance on human engineered barriers.

  17. Transport process of Pu isotope in marginal seas of the western North Pacific Ocean

    Energy Technology Data Exchange (ETDEWEB)

    Yamada, Masatoshi [Department of Radiation Chemistry, Institute of Radiation Emergency Medicine, Hirosaki University, Hirosaki, 036-8564, Aomori (Japan); Zheng, Jian [Research Center for Radiation Protection, National Institute of Radiological Sciences, 4-9-1 Anagawa, Inage, 263-8555, Chiba (Japan)

    2014-07-01

    Significant quantities of Pu isotopes have been released into the marine environment as the result of atmospheric nuclear weapons testing. Most radionuclides globally dispersed in atmospheric nuclear weapons testing were released into the environment during the 1950's and 1960's. In the western North Pacific Ocean, the principal source can be further distinguished as two distinct sources of Pu: close-in tropospheric fallout from nuclear weapons testing at the Pacific Proving Grounds (PPG) in the Marshall Islands and global stratospheric fallout. Since the {sup 240}Pu/{sup 239}Pu atom ratio is characteristic for the Pu emission source, information on Pu isotopic signature is very useful to better understand the transport process in the oceans and to identify the sources of Pu. The mean atom ratio of {sup 240}Pu/{sup 239}Pu from the global stratospheric fallout is 0.180 ±0.014 based on soil sample data, whereas that from close-in tropospheric fallout from the PPG is 0.33 - 0.36. The {sup 240}Pu/{sup 239}Pu atom ratios in seawater samples collected in marginal seas of the western North Pacific Ocean will provide important and useful data for understanding the process controlling Pu transport and for distinguishing future Pu sources. The objectives of this study were to measure the {sup 239+240}Pu concentrations and {sup 240}Pu/{sup 239}Pu atom ratios in seawater from the Sea of Okhotsk, Japan Sea, South China Sea and Sulu Sea and to discuss the transport process of Pu. Large-volume seawater samples (250 L each) were collected from the surface to the bottom in marginal seas of the western North Pacific Ocean with acoustically triggered quadruple PVC sampling bottles during the R/V Hakuho-Maru cruise. The {sup 239}Pu and {sup 240}Pu concentrations and {sup 240}Pu/{sup 239}Pu atom ratios were measured with a double-focusing SF-ICP-MS, which was equipped with a guard electrode to eliminate secondary discharge in the plasma and to enhance overall sensitivity. In

  18. Advanced modeling of prompt fission neutrons

    Energy Technology Data Exchange (ETDEWEB)

    Talou, Patrick [Los Alamos National Laboratory

    2009-01-01

    Theoretical and numerical studies of prompt fission neutrons are presented. The main results of the Los Alamos model often used in nuclear data evaluation work are reviewed briefly, and a preliminary assessment of uncertainties associated with the evaluated prompt fission neutron spectrum for n (0.5 MeV)+{sup 239}Pu is discussed. Advanced modeling of prompt fission neutrons is done by Monte Carlo simulations of the evaporation process of the excited primary fission fragments. The successive emissions of neutrons are followed in the statistical formalism framework, and detailed information, beyond average quantities, can be inferred. This approach is applied to the following reactions: {sup 252}Cf (sf), n{sub th} + {sup 239}Pu, n (0.5 MeV)+{sup 235}U, and {sup 236}Pu (sf). A discussion on the merits and present limitations of this approach concludes this presentation.

  19. Certified reference materials for radionuclides in Bikini Atoll sediment (IAEA-410) and Pacific Ocean sediment (IAEA-412).

    Science.gov (United States)

    Pham, M K; van Beek, P; Carvalho, F P; Chamizo, E; Degering, D; Engeler, C; Gascó, C; Gurriaran, R; Hanley, O; Harms, A V; Herrmann, J; Hult, M; Ikeuchi, Y; Ilchmann, C; Kanisch, G; Kis-Benedek, G; Kloster, M; Laubenstein, M; Llaurado, M; Mas, J L; Nakano, M; Nielsen, S P; Osvath, I; Povinec, P P; Rieth, U; Schikowski, J; Smedley, P A; Suplinska, M; Sýkora, I; Tarjan, S; Varga, B; Vasileva, E; Zalewska, T; Zhou, W

    2016-03-01

    The preparation and characterization of certified reference materials (CRMs) for radionuclide content in sediments collected offshore of Bikini Atoll (IAEA-410) and in the open northwest Pacific Ocean (IAEA-412) are described and the results of the certification process are presented. The certified radionuclides include: (40)K, (210)Pb ((210)Po), (226)Ra, (228)Ra, (228)Th, (232)Th, (234)U, (238)U, (239)Pu, (239+240)Pu and (241)Am for IAEA-410 and (40)K, (137)Cs, (210)Pb ((210)Po), (226)Ra, (228)Ra, (228)Th, (232)Th, (235)U, (238)U, (239)Pu, (240)Pu and (239+240)Pu for IAEA-412. The CRMs can be used for quality assurance and quality control purposes in the analysis of radionuclides in sediments, for development and validation of analytical methods and for staff training. Copyright © 2015 Elsevier Ltd. All rights reserved.

  20. Application of FORSS sensitivity and uncertainty methodology to fast reactor benchmark analysis

    Energy Technology Data Exchange (ETDEWEB)

    Weisbin, C.R.; Marable, J.H.; Lucius, J.L.; Oblow, E.M.; Mynatt, F.R.; Peelle, R.W.; Perey, F.G.

    1976-12-01

    FORSS is a code system used to study relationships between nuclear reaction cross sections, integral experiments, reactor performance parameter predictions, and associated uncertainties. This paper presents the theory and code description as well as the first results of applying FORSS to fast reactor benchmarks. Specifically, for various assemblies and reactor performance parameters, the nuclear data sensitivities were computed by nuclide, reaction type, and energy. Comprehensive libraries of energy-dependent coefficients have been developed in a computer retrievable format and released for distribution by RSIC and NNCSC. Uncertainties induced by nuclear data were quantified using preliminary, energy-dependent relative covariance matrices evaluated with ENDF/B-IV expectation values and processed for /sup 238/U(n,f), /sup 238/U(n,..gamma..), /sup 239/Pu(n,f), and /sup 239/Pu(..nu..). Nuclear data accuracy requirements to meet specified performance criteria at minimum experimental cost were determined.

  1. Plutonium determination in urine by techniques of mass spectrometry; Determinacion de plutonio en orina por tecnicas de espectrometria de masas

    Energy Technology Data Exchange (ETDEWEB)

    Hernandez M, H. [ININ, Departamento de Quimica, Carretera Mexico-Toluca s/n, 52750 Ocoyoacac, Estado de Mexico (Mexico); Yllera de Ll, A., E-mail: hector.hernandez520@gmail.com [Centro de Investigaciones Energeticas, Medioambientales y Tecnologicas, Departamento de Medio Ambiente, Av. Complutense 22, 28040 Madrid (Spain)

    2013-10-15

    The objective of this study was to develop an analytic method for quantification and plutonium reappraisal in plane tables of alpha spectrometry be means of the mass spectrometry technique of high resolution with plasma source inductively coupled and desolvator Aridus (Aridus-Hr-Icp-Ms) and mass spectrometry with accelerator (AMS). The obtained results were, the recovery percentage of Pu in the plane table was of ∼ 90% and activity minimum detectable obtained with Aridus-Hr-Icp-Ms and AMS was of ∼ 3 and ∼ 0.4 f g of {sup 239}Pu, respectively. Conclusion, the results demonstrate the aptitude of the Aridus-Hr-Icp-Ms and AMS techniques in the Pu reappraisal in plane tables with bigger speed and precision, improving the values notably of the activity minimum detectable that can be obtained with the alpha spectrometry (∼ 50 f g of {sup 239}Pu). (author)

  2. Plutonium interaction with a bacterial strain isolated from the waste isolation pilot plant (WIPP) environment

    Energy Technology Data Exchange (ETDEWEB)

    Strietelmeier, B.A.; Kraus, S.M.; Leonard, P.A.; Triay, I.R. [Los Alamos National Lab., NM (United States)] [and others

    1996-12-31

    This work was conducted as part of a series of experiments to determine the association and interaction of various actinides with bacteria isolated from the WIPP site. The majority of bacteria that exist at the site are expected to be halophiles, or extreme halophiles, due to the high concentration of salt minerals at the location. Experiments were conducted to determine the toxicity of plutonium-n-239, neptunium-237 and americium-243 to several species of these halophiles and the results were reported elsewhere. As an extension of these experiments, we report an investigation of the type of association that occurs between {sup 239}Pu and the isolate WIPP-1A, isolated by staff at Brookhaven National Laboratory, when grown in a high-salt, defined medium. Using scanning electron microscopy (SEM) techniques, we demonstrate a surface association of the {sup 239}Pu with the bacterial cells.

  3. Los Alamos National Laboratory Fission Basis

    Energy Technology Data Exchange (ETDEWEB)

    Keksis, A.L.; Chadwick, M.B.; Selby, H.D.; Mac Innes, M.R.; Barr, D.W.; Meade, R.A.; Burns, C.J.; Wallstrom, T.C. [Los Alamos National Laboratory, NM 87545 (United States)

    2011-07-01

    This report is an overview of two main publications that provide a comprehensive review of the Los Alamos National Laboratory (LANL) Fission Basis. The first is the experimental paper, {sup F}ission Product Data Measured at Los Alamos for Fission Spectrum and Thermal Neutrons on {sup 239}Pu, {sup 235}U, {sup 238}U, [Selby, H. D., et al., Nucl. Data Sheets, Vol. 111 2010, pp. 2891-2922] and the second is the theoretical paper, Fission Product Yields from Fission Spectrum n+ {sup 239}Pu for ENDF/B-VII.1, [Chadwick, M. B., et al., Nucl. Data Sheets, Vol. 111, 2010, pp. 2923-2964]. One important note is that none of this work would have been possible without the great documentation of the experimental details and results by G.W. Knobeloch, G. Butler, C.I. Browne, B. Erdal, B. Bayhurst, R. Prestwood, V. Armijo, J. Hasty and many others. (authors)

  4. Off-Site Radiation Exposure Review Project: Phase 2 soils program

    Energy Technology Data Exchange (ETDEWEB)

    McArthur, R.D.; Miller, F.L. Jr.

    1989-12-01

    To help estimate population doses of radiation from fallout originating at the Nevada Test Site, soil samples were collected throughout the western United States. Each sample was prepared by drying and ball-milling, then analyzed by gamma-spectrometry to determine the amount of {sup 137}Cs it contained. Most samples were also analyzed by chemical separation and alpha-spectrometry to determine {sup 239 + 240}Pu and by isotope mass spectroscopy to determine the ratios of {sup 240}Pu to {sup 239}Pu and {sup 241}Pu to {sup 239}Pu. The total inventories of cesium and plutonium at 171 sites were computed from the results. This report describes the sample collection, processing, and analysis, presents the analytical results, and assesses the quality of the data. 10 refs., 9 figs., 12 tabs.

  5. Development of an ultra-sensitive detection method for transuranium elements with respect to ocean water samples from Fukushima

    Energy Technology Data Exchange (ETDEWEB)

    Hain, Karin Margarete

    2016-03-30

    The development of a detection method for the identification of a possible emission of actinides into the Pacific Ocean by the Fukushima Daiichi Nuclear Power Plant (FDNPP) accident, was the major aim of this PhD thesis. It is shown in this work that in addition to the isotopic plutonium ratio {sup 240}Pu/{sup 239}Pu, which is an important signature for different contamination sources, the {sup 241}Pu/{sup 239}Pu ratio has to be determined, to distinguish between a Fukushima entry of actinides and nuclear weapon fallout in the Pacific Ocean. Furthermore, this study was aiming for the improvement of the data on the neptunium ({sup 237}Np) distribution in the ocean. For the detection of the trace concentrations of actinides in the order of mBq/m{sup 3} in a small sample volume of 20 L ocean water, the ultra-sensitive method accelerator mass spectrometry (AMS) was chosen. A chemical separation procedure for Pu and Np based on extraction chromatography was developed using mass spectrometry and radiometric analysis to determine the chemical recovery. {sup 241}Am, which causes isobaric background to {sup 241}Pu in mass spectrometric measurements, was separated with a suppression of at least 10{sup -4} from Pu by this method. The detection method adjusted to Pu and Np was successfully verified by analyzing the concentration of Pu in certified reference material with AMS at the Maier-Leibnitz-Laboratory (MLL) in Munich. Due to a temporary closure of the MLL, 12 sea water samples, collected in autumn 2012, were prepared at the Radiochemie Muenchen and measured at the Vienna Environmental Research Laboratory (VERA). The sampling station closest to the FDNPP was located at a distance of 39.6 km. Three of the samples showed a slightly elevated {sup 240}Pu/{sup 239}Pu ratio of up to 0.23{sup +0.04}{sub -0.03} compared to global fallout ({sup 240}Pu/{sup 239}Pu = 0.180±0.007), whereas all measured {sup 241}Pu/{sup 239}Pu ratios were clearly consistent with nuclear weapon

  6. Ultratrace and isotope ratios analyses of some radionuclides by ICP-MS

    Energy Technology Data Exchange (ETDEWEB)

    Helal, A.I.; Zahran, N.F.; Abd El-Lateef, A.M.; Mohsen, H.T. [Central Lab. for Elemental and Isotopic Analysis, N.R.C. Atomic Energy Authority, Cairo (Egypt); Amr, M.A. [Central Lab. for Elemental and Isotopic Analysis, N.R.C. Atomic Energy Authority, Cairo (Egypt); Nuclear Physics Dept., N.R.C., Atomic Energy Authority, Cairo (Egypt); Bashter, I.I. [Physics Dept., Faculty of Science, Zagazig Univ. (Egypt); Abbas, Y. [Physics Dept., Faculty of Science, Suez Canal Univ., Ismailia (Egypt)

    2004-07-01

    Extensive work is under way using high resolution-ICP-MS for {sup 90}Sr, {sup 234}U, {sup 235}U, {sup 238}U, {sup 239}Pu, {sup 240}Pu, and {sup 241}Am detection. Sample preparation procedures based on liquid-liquid extraction and ion exchange chromatography were developed. Sr, U, Pu, and Am were separated from their matrix and concentrated to improve the power of detection in the mass spectrometer. A microconcentric nebulizer with a desolvation introduction system (Ardius) is used. Instrumental limits of detection using Sr and U standard solutions are 0.01 ppt and 0.006 ppt for Sr and U, respectively. A study is presented on the mass interferences for the specified radionuclides. In the environmental samples investigated the {sup 90}Sr/{sup 86}Sr isotope ratio is 6.02 x 10{sup -9} and for {sup 240}Pu/{sup 239}Pu the isotope ratio is 0.17. (orig.)

  7. Improving neutronics simulations and uncertainties via a selection of nuclear data

    Energy Technology Data Exchange (ETDEWEB)

    Rochman, D. [Paul Scherrer Institut, Laboratory for Reactor Physics Systems Behaviour, Villigen (Switzerland); Koning, A.J.; Marck, S.C. van der [Nuclear Research and Consultancy Group NRG, Petten (Netherlands)

    2015-12-15

    This work presents a novel approach to improve neutronics simulations, as in the case of criticality calculations, by simply combining the results of a limited set of random evaluations. Another outcome of this work is to lower uncertainties due to nuclear data by integrating the information from criticality benchmarks into the neutronics simulations scheme. Examples are presented for the {sup 239}Pu nuclear data and calculations of criticality benchmarks and a MOX fuel pincell. (orig.)

  8. Reassessment of plutonium by alpha spectrometry planchets Aridus-DF-ICP-MS and 1 MV compact AMS; Reevaluacion de plutonio en planchetas de espectrometria alfa mediante ARIDUS-DF-ICP-MS y AMS compacto de 1 MV

    Energy Technology Data Exchange (ETDEWEB)

    Hernandez Mendoza, H.; Chamizo Calvo, E.; Yllera de Llano, A.

    2011-07-01

    The aim of this study was to develop and validate, for the first time in Spain, an analytical method for the reevaluation of planchets containing small amounts of 239Pu (between 8 and 40 fg) using two mass spectrometric techniques: mass spectrometry dual approach with inductively coupled plasma source and de solvated Aridus (Aridus-DF-ICP-MS) and accelerator mass spectrometry compact 1 MV (AMS).

  9. Investigation of plutonium concentration and distribution in burrowing crayfish from the White Oak Creek floodplain

    Energy Technology Data Exchange (ETDEWEB)

    Delaney, M.S.; Dahlman, R.C.; Craig, R.B.

    1979-01-01

    The White Oak floodplain was contaminated with several radionuclides, including /sup 239/Pu, during the Manhattan Project in 1944. Plutonium distribution in the soil is nonhomogeneous. An investigation was conducted to deterine Pu accumulation in a resident animal population. Crayfish were chosen because they complete their life-cycle within the contaminated environment, they directly contact contaminated muds, and they function in a food chain of significance to man. Two major conclusions of the research were that Pu concentrations in contaminated crayfish typically exceed those of control crayfish by two orders of magnitude and that if an incident were to occur in which a standard man ingested the soft tissues of ten crayfish from the floodplain, an insignificant whole body dose would accrue over the subsequent 50 years of life. The digestive tract of contaminated crayfish contained 21 to 33% of the Pu body burden, soft tissues contained 11 to 31% of the Pu body burden, and 48 to 62% of the Pu body burden of contaminated crayfish was associated with the carapace. Therefore, at a molt a large proportion of its accumulated Pu is deposited in the environment. A supplementary laboratory investigation using /sup 237/Pu included a chronic Pu uptake study by uncontaminated crayfish. In these crayfish, from 64 to 82% of the /sup 237/Pu was associated with the body tissues. Complementary data for /sup 237/Pu associated with the carapace ranged from 18 to 37% of the distribution. An inventory of /sup 239/Pu in crayfish at two sites on the floodplain was calculated by multiplying the estimated biomass of the crayfish by their average /sup 239/Pu concentration. This evaluation of Pu associated with the crayfish population was compared to an inventory of /sup 239/Pu in the soil in which they burrow and was found to be eight orders of magnitude less.

  10. Development of a multimedia radionuclide exposure model for low-level waste management

    Energy Technology Data Exchange (ETDEWEB)

    Onishi, Y.; Whelan, G.; Skaggs, R.L.

    1982-03-01

    A method is being developed for assessing exposures of the air, water, and plants to low-level waste (LLW) as a part of an overall development effort of a LLW site evaluation methodology. The assessment methodology will predict LLW exposure levels in the environment by simulating dominant mechanisms of LLW migration and fate. The methodology consists of a series of physics-based models with proven histories of success; the models interact with each other to simulate LLW transport in the ecosystem. A scaled-down version of the methodology was developed first by combining the terrestrial ecological model, BIOTRAN; the overland transport model, ARM; the instream hydrodynamic model, DKWAV; and the instream sediment-contaminant transport model, TODAM (a one-dimensional version of SERATRA). The methodology was used to simulate the migration of /sup 239/Pu from a shallow-land disposal site (known as Area C) located near the head of South Mortandad Canyon on the LANL site in New Mexico. The scenario assumed that /sup 239/Pu would be deposited on the land surface through the natural processes of plant growth, LLW uptake, dryfall, and litter decomposition. Runoff events would then transport /sup 239/Pu to and in the canyon. The model provided sets of simulated LLW levels in soil, water and terrestrial plants in the region surrounding the site under a specified land-use and a waste management option. Over a 100-yr simulation period, only an extremely small quantity (6 x 10/sup -9/ times the original concentration) of buried /sup 239/Pu was taken up by plants and deposited on the land surface. Only a small fraction (approximately 1%) of that contamination was further removed by soil erosion from the site and carried to the canyon, where it remained. Hence, the study reveals that the environment around Area C has integrity high enough to curtail LLW migration under recreational land use.

  11. Studies of Np and Pu in the marine environment of Swedish-Danish waters and the North Atlantic Ocean

    Energy Technology Data Exchange (ETDEWEB)

    Lindahl, Patric [Department of Radiation Physics, Lund University Hospital, SE-221 85 Lund (Sweden) and Korea Ocean Research and Development Institute, Ansan P.O. Box 29, Seoul 425-600 (Korea, Republic of)]. E-mail: patriclindahl@yahoo.com; Roos, Per [Risoe National Laboratory, P.O. Box 49, DK-4000 Roskilde (Denmark); Holm, Elis [Department of Radiation Physics, Lund University Hospital, SE-221 85 Lund (Sweden); Risoe National Laboratory, P.O. Box 49, DK-4000 Roskilde (Denmark); Dahlgaard, Henning [Risoe National Laboratory, P.O. Box 49, DK-4000 Roskilde (Denmark)

    2005-07-01

    The long-lived anthropogenic radionuclides {sup 237}Np, {sup 239}Pu and {sup 240}Pu were determined in marine environmental samples (seaweed and seawater) collected from Swedish-Danish waters and the North Atlantic Ocean at various locations on different occasions during the period 1991-2001. The measurements were performed with sector field Inductively Coupled Plasma Mass Spectrometry (ICP-MS) and conventional alpha spectrometry. The {sup 237}Np activity concentrations in Fucus vesiculosus and surface seawater from the Swedish west coast and Danish waters ranged from 0.16 {+-} 0.02 to 1.02 {+-} 0.09 mBq kg{sup -1} (dry weight) and 0.65 {+-} 0.02 to 1.69 {+-} 0.02 mBq m{sup -3}, respectively, depending on the location and sampling year. Most of the {sup 237}Np in these waters is believed to originate from the Sellafield nuclear reprocessing plant, with some contribution from global fallout. The {sup 240}Pu/{sup 239}Pu atomic ratios in F. vesiculosus samples are reported in this study with an overall average of 0.17 {+-} 0.03. The {sup 237}Np and {sup 239}Pu activity concentrations observed in surface seawater collected in North Atlantic waters ranged from 0.16 {+-} 0.01 to 0.62 {+-} 0.08 mBq m{sup -3} and from 0.64 {+-} 0.05 to 4.27 {+-} 0.08 mBq m{sup -3}, respectively, and the {sup 237}Np/{sup 239}Pu atomic ratios were a good indicator of conservative behaviour of Np in marine waters.

  12. Fukushima plutonium effect and blow-up regimes in neutron-multiplying media

    CERN Document Server

    Rusov, V D; Vaschenko, V M; Linnik, E P; Zelentsova, T N; Beglaryan, M E; Chernegenko, S A; Kosenko, S I; Molchinikolov, P A; Smolyar, V P; Grechan, E V

    2012-01-01

    It is shown that the capture and fission cross-sections of 238U and 239Pu increase with temperature within 1000-3000K range, in contrast to those of 235U, that under certain conditions may lead to the so-called blow-up modes, stimulating the anomalous neutron flux and nuclear fuel temperature growth. Some features of the blow-up regimes in neutron-multiplying media are discussed.

  13. Chronology of Pu isotopes and 236U in an Arctic ice core.

    Science.gov (United States)

    Wendel, C C; Oughton, D H; Lind, O C; Skipperud, L; Fifield, L K; Isaksson, E; Tims, S G; Salbu, B

    2013-09-01

    In the present work, state of the art isotopic fingerprinting techniques are applied to an Arctic ice core in order to quantify deposition of U and Pu, and to identify possible tropospheric transport of debris from former Soviet Union test sites Semipalatinsk (Central Asia) and Novaya Zemlya (Arctic Ocean). An ice core chronology of (236)U, (239)Pu, and (240)Pu concentrations, and atom ratios, measured by accelerator mass spectrometry in a 28.6m deep ice core from the Austfonna glacier at Nordaustlandet, Svalbard is presented. The ice core chronology corresponds to the period 1949 to 1999. The main sources of Pu and (236)U contamination in the Arctic were the atmospheric nuclear detonations in the period 1945 to 1980, as global fallout, and tropospheric fallout from the former Soviet Union test sites Novaya Zemlya and Semipalatinsk. Activity concentrations of (239+240)Pu ranged from 0.008 to 0.254 mBq cm(-2) and (236)U from 0.0039 to 0.053 μBq cm(-2). Concentrations varied in concordance with (137)Cs concentrations in the same ice core. In contrast to previous published results, the concentrations of Pu and (236)U were found to be higher at depths corresponding to the pre-moratorium period (1949 to 1959) than to the post-moratorium period (1961 and 1962). The (240)Pu/(239)Pu ratio ranged from 0.15 to 0.19, and (236)U/(239)Pu ranged from 0.18 to 1.4. The Pu atom ratios ranged within the limits of global fallout in the most intensive period of nuclear atmospheric testing (1952 to 1962). To the best knowledge of the authors the present work is the first publication on biogeochemical cycles with respect to (236)U concentrations and (236)U/(239)Pu atom ratios in the Arctic and in ice cores. Copyright © 2013 Elsevier B.V. All rights reserved.

  14. A multiple sampling ionization chamber for the External Target Facility

    Energy Technology Data Exchange (ETDEWEB)

    Zhang, X.H., E-mail: zhxh@impcas.ac.cn [Institute of Modern Physics, Chinese Academy of Sciences, Lanzhou 730000 (China); Tang, S.W.; Ma, P.; Lu, C.G.; Yang, H.R.; Wang, S.T.; Yu, Y.H.; Yue, K.; Fang, F. [Institute of Modern Physics, Chinese Academy of Sciences, Lanzhou 730000 (China); Yan, D.; Zhou, Y.; Wang, Z.M.; Sun, Y. [Institute of Modern Physics, Chinese Academy of Sciences, Lanzhou 730000 (China); University of Chinese Academy of Sciences, Beijing 100049 (China); Sun, Z.Y.; Duan, L.M. [Institute of Modern Physics, Chinese Academy of Sciences, Lanzhou 730000 (China); Sun, B.H. [School of Physics and Nuclear Energy Engineering, Beihang University, Beijing 100191 (China)

    2015-09-21

    A multiple sampling ionization chamber used as a particle identification device for high energy heavy ions has been developed for the External Target Facility. The performance of this detector was tested with a {sup 239}Pu α source and RI beams. A Z resolution (FWHM) of 0.4–0.6 was achieved for nuclear fragments of {sup 18}O at 400 AMeV.

  15. A breed and burn reshuffling scheme for an Astrid-like reactor concept design

    Energy Technology Data Exchange (ETDEWEB)

    Garcia C, E. Y.; Francois L, J. L., E-mail: eliasgarcerv@hotmail.com [UNAM, Facultad de Ingenieria, Departamento de Sistemas Energeticos, Paseo Cuauhnahuac 8532, 62550 Jiutepec, Morelos (Mexico)

    2016-09-15

    The greenhouse emissions has a serious impact on environmental terms, reason why energy supply needs to be provided by low carbon emission technologies. Nuclear power is and environmentally friendly energy with future concepts and designs that ensure safety, and in this paper is taken as a solution to be considered in the energy supply mix. This study presents an extension on the operation of the Advanced Sodium Technological Reactor for Industrial demonstration (Astrid) nuclear reactor through a breed and burn operation to extend the operation of the reactor. The Astrid nuclear reactor is a fourth generation sodium-cooled fast reactor of 1500 MWt h, and it considers an innovative design: the low void effect core (Cfv: Coeur a Faible effet de Vidange sodium) due to the reactor configuration and the radial and axial position of the fuel subassemblies. Previous research in the Astrid-like cores aimed the model validation of a conventional oxide-fueled core and its comparison with a proposed metallic-fueled core. Taking into account the amount of fissile material (mainly 239-Pu) after the first cycle, a reshuffling scheme was suggested, which consists in changing strategically the position of the nuclear fuel assemblies when the reactivity drops near to the critical state of the reactor. Two different reshuffling schemes were simulated in every developed model, having operation extensions of 805 days and 1775 days for the oxide and metallic designs respectively. The implementation of the reshuffling schemes in the developed models enhanced the fuel utilization and could save up to 2.20 and 5.96 tons of plutonium for oxide and metallic designs respectively, which has an economic impact. The breeding of 239-Pu achieved in the fertile zone of the metallic design reached half of the initial concentration of the 239-Pu in the fissile zone and for the oxide design, the breeding reached one third of the initial concentration of the 239-Pu in the fissile zone. (Author)

  16. Plutonium Bioassay Testing of U.S. Atmospheric Nuclear Test Participants and U.S. Occupation Forces of Hiroshima and Nagasaki, Japan

    Science.gov (United States)

    2015-10-30

    C H N IC A L R EP O R T This page intentionally left blank. STANDARD FORM 298 (Rev. 8/98) REPORT DOCUMENTATION PAGE Form Approved OMB No...release: distribution is unlimited. 13. SUPPLEMENTARY NOTES 14. ABSTRACT This report documents DTRA’s study conducted from 1994 to 2004 to...of 239Pu measurements by LANL and BNL .................................................... 12 Table 2. Locations and numbers of subjects contributing

  17. Calibration of 242 Pu Tracer by Mass Spectrometry%质谱法标定242 Pu指示剂

    Institute of Scientific and Technical Information of China (English)

    李冬梅; 徐江; 杜丽丽

    2014-01-01

    将高纯242 Pu浓度标准溶液与239 Pu混合,质谱法测量R239/242(A)先标定四水硫酸钚中239 Pu的浓度;再将四水硫酸钚与待标定的242 Pu指示剂混合,测量R239/242(A),标定242 Pu 指示剂的浓度。质谱测量还可标定得到242 Pu指示剂中的钚同位素丰度。采用两次同位素稀释质谱法标定242 Pu 指示剂快捷简便,可在2日内完成。测量精度高,242 Pu浓度的相对合成标准不确定度为0.75%,该指示剂可满足高精度分析工作的需求。%242 Pu is commonly employed as tracer for determination of 239 Pu in environmental samples.The 239 Pu concentration in Pu(SO4 )2 ·4H2 O solution was determined by isotope dilution-mass spectrometry (ID-MS)using a high pure 242 Pu spike.Then the 242 Pu tracer in our laboratary was calibrated by ID-MS using the calibrated 239 Pu solution as spike.By meas-uring the atom ratio of 239 Pu to 242 Pu twice by ID-MS,the concentration and abundance of the 242 Pu tracer in laboratary were finally calibrated.This method was proved to be efficient with high precision.The process could be finished within two days with an uncertainty of 0.75%. The calibrated 242 Pu tracer in laboratory could meet the demand of high-precision analysis.

  18. LA-ICP-MS for Pu source identification at Mayak PA, the Urals, Russia.

    Science.gov (United States)

    Cagno, S; Hellemans, K; Lind, O C; Skipperud, L; Janssens, K; Salbu, B

    2014-02-01

    Information on Pu in environmental samples is traditionally based on the determination of the (240+239)Pu activity via Alpha Spectrometry (AS). A large number of alpha spectrometry sources (planchettes) containing radiochemically separated Pu are therefore stored worldwide and are available for further analyses. These archive samples represent a resource from which valuable information on isotopic composition of alpha emitters including Pu can be obtained. The relative abundances of Pu isotopes can be used to trace specific Pu sources and characterize the relative contributions of different Pu sources in a sample. Thus, in addition to the total (239+240)Pu activity, determination of the (240)Pu/(239)Pu ratio can provide valuable information on the nature of the Pu emitting sources. The Pu isotopic ratios can be determined by mass spectrometry techniques such as Sector Field Inductively Coupled Plasma Mass Spectrometry (SF-ICPMS) or Accelerator Mass Spectrometry (AMS) that require dissolution and complete destruction of the material deposited on the planchettes. In this study Laser Ablation (LA)-quadrupole-ICP-MS has been employed for the analysis of (239)Pu/(240)Pu ratios from alpha-planchettes prepared from samples originating from the Mayak PA nuclear facility, Russia. The results are compared with data from AMS and show that the (240)Pu/(239)Pu ratios obtained by LA-ICP-MS can be utilized to distinguish weapons-grade Pu from civil reprocessing sources. Moreover, isotope ratio mapping can also be performed across the planchettes, allowing e.g. the visualization of possible inhomogeneities in the Pu-isotope distribution on their surface. Thus, this solid sample technique can be applied to extract additional information from existing archives of samples.

  19. Uncertainty analysis of doses from ingestion of plutonium and americium.

    Science.gov (United States)

    Puncher, M; Harrison, J D

    2012-02-01

    Uncertainty analyses have been performed on the biokinetic model for americium currently used by the International Commission on Radiological Protection (ICRP), and the model for plutonium recently derived by Leggett, considering acute intakes by ingestion by adult members of the public. The analyses calculated distributions of doses per unit intake. Those parameters having the greatest impact on prospective doses were identified by sensitivity analysis; the most important were the fraction absorbed from the alimentary tract, f(1), and rates of uptake from blood to bone surfaces. Probability distributions were selected based on the observed distribution of plutonium and americium in human subjects where possible; the distributions for f(1) reflected uncertainty on the average value of this parameter for non-specified plutonium and americium compounds ingested by adult members of the public. The calculated distributions of effective doses for ingested (239)Pu and (241)Am were well described by log-normal distributions, with doses varying by around a factor of 3 above and below the central values; the distributions contain the current ICRP Publication 67 dose coefficients for ingestion of (239)Pu and (241)Am by adult members of the public. Uncertainty on f(1) values had the greatest impact on doses, particularly effective dose. It is concluded that: (1) more precise data on f(1) values would have a greater effect in reducing uncertainties on doses from ingested (239)Pu and (241)Am, than reducing uncertainty on other model parameter values and (2) the results support the dose coefficients (Sv Bq(-1) intake) derived by ICRP for ingestion of (239)Pu and (241)Am by adult members of the public.

  20. Neutron sources and its dosimetric characteristics; Fuentes de neutrones y sus caracteristicas dosimetricas

    Energy Technology Data Exchange (ETDEWEB)

    Vega C, H.R.; Manzanares A, E.; Hernandez D, V.M.; Mercado S, G.A. [Universidad Autonoma de Zacatecas, A.P. 336, 98000 Zacatecas (Mexico); Gallego D, E.; Lorente F, A. [Universidad Politecnica de Madrid, C/Jose Gutierrez Abascal 2, E-28006 Madrid (Spain)

    2005-07-01

    By means of Monte Carlo methods the spectra of the produced neutrons {sup 252} Cf, {sup 252} Cf/D{sub 2}O, {sup 241} Am Be, {sup 239} Pu Be, {sup 140} La Be, {sup 239} Pu{sup 18}O{sub 2} and {sup 226} Ra Be have been calculated. With the information of the spectrum it was calculated the average energy of the neutrons of each source. By means of the fluence coefficients to dose it was determined, for each one of the studied sources, the fluence factors to dose. The calculated doses were H, H{sup *}(10), H{sub p,sIab} (10, 0{sup 0}), E{sub AP} and E{sub ISO}. During the phase of the calculations the sources were modeled as punctual and their characteristics were determined to 100 cm in the hole. Also, for the case of the sources of {sup 239} Pu Be and {sup 241} Am Be, were carried out calculations modeling the sources with their respective characteristics and the dosimetric properties were determined in a space full with air. The results of this last phase of the calculations were compared with the experimental results obtained for both sources. (Author)

  1. AMS of the Minor Plutonium Isotopes.

    Science.gov (United States)

    Steier, P; Hrnecek, E; Priller, A; Quinto, F; Srncik, M; Wallner, A; Wallner, G; Winkler, S

    2013-01-01

    VERA, the Vienna Environmental Research Accelerator, is especially equipped for the measurement of actinides, and performs a growing number of measurements on environmental samples. While AMS is not the optimum method for each particular plutonium isotope, the possibility to measure (239)Pu, (240)Pu, (241)Pu, (242)Pu and (244)Pu on the same AMS sputter target is a great simplification. We have obtained a first result on the global fallout value of (244)Pu/(239)Pu = (5.7 ± 1.0) × 10(-5) based on soil samples from Salzburg prefecture, Austria. Furthermore, we suggest using the (242)Pu/(240)Pu ratio as an estimate of the initial (241)Pu/(239)Pu ratio, which allows dating of the time of irradiation based solely on Pu isotopes. We have checked the validity of this estimate using literature data, simulations, and environmental samples from soil from the Salzburg prefecture (Austria), from the shut down Garigliano Nuclear Power Plant (Sessa Aurunca, Italy) and from the Irish Sea near the Sellafield nuclear facility. The maximum deviation of the estimated dates from the expected ages is 6 years, while relative dating of material from the same source seems to be possible with a precision of less than 2 years. Additional information carried by the minor plutonium isotopes may allow further improvements of the precision of the method.

  2. RAPID DETERMINATION OF 237 NP AND PU ISOTOPES IN WATER BY INDUCTIVELY COUPLED PLASMA MASS SPECTROMETRY AND ALPHA SPECTROMETRY

    Energy Technology Data Exchange (ETDEWEB)

    Maxwell, S.; Jones, V.; Culligan, B.; Nichols, S.; Noyes, G.

    2010-06-23

    A new method that allows rapid preconcentration and separation of plutonium and neptunium in water samples was developed for the measurement of {sup 237}Np and Pu isotopes by inductively-coupled plasma mass spectrometry (ICP-MS) and alpha spectrometry; a hybrid approach. {sup 238}U can interfere with {sup 239}Pu measurement by ICP-MS as {sup 238}UH{sup +} mass overlap and {sup 237}Np via peak tailing. The method provide enhanced removal of uranium by separating Pu and Np initially on TEVA Resin, then moving Pu to DGA resin for additional removal of uranium. The decontamination factor for uranium from Pu is almost 100,000 and the decontamination factor for U from Np is greater than 10,000. This method uses stacked extraction chromatography cartridges and vacuum box technology to facilitate rapid separations. Preconcentration is performed using a streamlined calcium phosphate precipitation method. Purified solutions are split between ICP-MS and alpha spectrometry so that long and short-lived Pu isotopes can be measured successfully. The method allows for simultaneous extraction of 20 samples (including QC samples) in 4 to 6 hours, and can also be used for emergency response. {sup 239}Pu, {sup 242}Pu and {sup 237}Np were measured by ICP-MS, while {sup 236}Pu, {sup 238}Pu, and {sup 239}Pu were measured by alpha spectrometry.

  3. Characterisation of the plutonium isotopic composition of a sediment core from Palomares, Spain, by low-energy AMS and alpha-spectrometry

    Energy Technology Data Exchange (ETDEWEB)

    Chamizo, E., E-mail: elechacal@alum.us.e [Centro Nacional de Aceleradores (CNA), Isla de la Cartuja, 41092 Seville (Spain); Jimenez-Ramos, M.C.; Enamorado, S.M. [Centro Nacional de Aceleradores (CNA), Isla de la Cartuja, 41092 Seville (Spain); Garcia-Leon, M. [Departamento de Fisica Atomica, Molecular y Nuclear, Universidad de Sevilla, 41012 Sevilla (Spain); Garcia-Tenorio, R. [Departamento de Fisica Aplicada II, E.T.S.A, Universidad de Sevilla, 41012 Sevilla (Spain); Mas, J.L. [Departamento de Fisica Aplicada I, Universidad de Sevilla, 41012 Sevilla (Spain); Masque, P. [Institut de Ciencia i Tecnologia Ambientals, Department de Fisica, Universitat Autonoma de Barcelona, 08193 Bellaterra (Spain); Merino, J. [Amphos 21, Pg. de Rubi 29-31, E-08197 Valldoreix (Spain); Sanchez-Cabeza, J.A. [Institut de Ciencia i Tecnologia Ambientals, Department de Fisica, Universitat Autonoma de Barcelona, 08193 Bellaterra (Spain); International Atomic Energy Agency, Marine Environment Laboratories, MC-98000 (Monaco)

    2010-04-15

    The measurement of plutonium isotopes, {sup 239}Pu and {sup 240}Pu, at 670 kV on the compact accelerator mass spectrometry (AMS) system at the Centro Nacional de Aceleradores (CNA) in Seville, Spain, is now a reality. In this work, we present first Pu AMS results for environmental samples: a sediment core collected in a submarine canyon in the Mediterranean coast of the Spanish region of Palomares, affected by a nuclear accident in 1966. From the study of the {sup 240}Pu/{sup 239}Pu atomic ratio profile, showing on average levels lower than 11%, we confirm that the weapon-grade plutonium released on land during the accident, with a characteristic {sup 240}Pu/{sup 239}Pu atomic ratio of 5.8%, has found its way into the marine environment. A two-plutonium sources mixture model (Palomares and fallout) is used to elucidate the percentage of the plutonium coming from the accident. As a validation exercise of the Pu AMS measuring technique and in order to obtain the {sup 238}Pu/{sup (239+240)}Pu activity ratios, samples were also studied by alpha-spectrometry (AS). The obtained AS {sup 239+240}Pu activity concentration results fit in with the AMS ones in a wide dynamic range, thus validating the AMS technique.

  4. Safe management of actinides in the nuclear fuel cycle: Role of mineralogy

    Science.gov (United States)

    Ewing, Rodney C.

    2011-02-01

    During the past 60 years, more than 1800 metric tonnes of Pu, and substantial quantities of the "minor" actinides, such as Np, Am and Cm, have been generated in nuclear reactors. Some of these transuranium elements can be a source of energy in fission reactions (e.g., 239Pu), a source of fissile material for nuclear weapons (e.g., 239Pu and 237Np), and of environmental concern because of their long-half lives and radiotoxicity (e.g., 239Pu and 237Np). There are two basic strategies for the disposition of these heavy elements: (1) to "burn" or transmute the actinides using nuclear reactors or accelerators; (2) to "sequester" the actinides in chemically durable, radiation-resistant materials that are suitable for geologic disposal. There has been substantial interest in the use of actinide-bearing minerals, especially isometric pyrochlore, A 2B 2O 7 (A = rare earths; B = Ti, Zr, Sn, Hf), for the immobilization of actinides, particularly plutonium, both as inert matrix fuels and nuclear waste forms. Systematic studies of rare-earth pyrochlores have led to the discovery that certain compositions (B = Zr, Hf) are stable to very high doses of alpha-decay event damage. Recent developments in our understanding of the properties of heavy element solids have opened up new possibilities for the design of advanced nuclear fuels and waste forms.

  5. Quantitative Analysis of Plutonium Content in Particles Collected from a Certified Reference Material by Total Nuclear Reaction Energy (Q Value) Spectroscopy

    Science.gov (United States)

    Croce, M. P.; Hoover, A. S.; Rabin, M. W.; Bond, E. M.; Wolfsberg, L. E.; Schmidt, D. R.; Ullom, J. N.

    2016-08-01

    Microcalorimeters with embedded radioisotopes are an emerging category of sensor with advantages over existing methods for isotopic analysis of trace-level nuclear materials. For each nuclear decay, the energy of all decay products captured by the absorber (alpha particles, gamma rays, X-rays, electrons, daughter nuclei, etc.) is measured in one pulse. For alpha-decaying isotopes, this gives a measurement of the total nuclear reaction energy (Q value) and the spectra consist of well-separated, narrow peaks. We have demonstrated a simple mechanical alloying process to create an absorber structure consisting of a gold matrix with small inclusions of a radioactive sample. This absorber structure provides an optimized energy thermalization environment, resulting in high-resolution spectra with minimal tailing. We have applied this process to the analysis of particles collected from the surface of a plutonium metal certified reference material (CRM-126A from New Brunswick Laboratory) and demonstrated isotopic analysis by microcalorimeter Q value spectroscopy. Energy resolution from the Gaussian component of a Bortels function fit was 1.3 keV FWHM at 5244 keV. The collected particles were integrated directly into the detector absorber without any chemical processing. The ^{238}Pu/^{239}Pu and ^{240}Pu/^{239}Pu mass ratios were measured and the results confirmed against the certificate of analysis for the reference material. We also demonstrated inter-element analysis capability by measuring the ^{241}Am/^{239}Pu mass ratio.

  6. Improvements in lung lavage to increase its effectiveness in removing inhaled radionuclides

    Energy Technology Data Exchange (ETDEWEB)

    Muggenburg, B.A.; Guilmette, R.A.; Romero, L.M.; Mewhinney, J.A.

    1991-12-31

    Lung lavage has been shown to be an effective method to remove insoluble radionuclides deposited and retained in the lung, but the treatment has been limited to the effective removal of only about 50% of the retained material. Reported here is change in lavage technique that slightly increases the effectiveness and the addition of high-frequency chest wall oscillation. The latter increased the effectiveness of the lavage procedure but also caused significant physiological complications. These studies were conducted in adult male and female beagles. The aerosol in the first study was {sup 239}PuO{sub 2} heat-treated at 850{degrees}C, obtained as powder from a commercial V-blending process. The dogs briefly inhaled the aerosol per nasi. The tissue content at death and the amount of {sup 239}Pu excreted and in the recovered lung lavage fluid was determined by radiochemical methods{sup 5}. These values were used to reconstruct the initial pulmonary burden of {sup 239} and the amount of {sup 239}Pu removed by lavage. In the second study, with the HFCWO, the aerosol was {sup 85}Sr fused in aluminosilicate particles. The IPB of {sup 85}Sr was determined by whole-body counting. The excreta and recovered lung lavage fluids were also assayed for {sup 85}Sr activity.

  7. Improvements in lung lavage to increase its effectiveness in removing inhaled radionuclides

    Energy Technology Data Exchange (ETDEWEB)

    Muggenburg, B.A.; Guilmette, R.A.; Romero, L.M.; Mewhinney, J.A.

    1991-01-01

    Lung lavage has been shown to be an effective method to remove insoluble radionuclides deposited and retained in the lung, but the treatment has been limited to the effective removal of only about 50% of the retained material. Reported here is change in lavage technique that slightly increases the effectiveness and the addition of high-frequency chest wall oscillation. The latter increased the effectiveness of the lavage procedure but also caused significant physiological complications. These studies were conducted in adult male and female beagles. The aerosol in the first study was {sup 239}PuO{sub 2} heat-treated at 850{degrees}C, obtained as powder from a commercial V-blending process. The dogs briefly inhaled the aerosol per nasi. The tissue content at death and the amount of {sup 239}Pu excreted and in the recovered lung lavage fluid was determined by radiochemical methods{sup 5}. These values were used to reconstruct the initial pulmonary burden of {sup 239} and the amount of {sup 239}Pu removed by lavage. In the second study, with the HFCWO, the aerosol was {sup 85}Sr fused in aluminosilicate particles. The IPB of {sup 85}Sr was determined by whole-body counting. The excreta and recovered lung lavage fluids were also assayed for {sup 85}Sr activity.

  8. Results of the Excreta Bioassay Quality Control Program for April 1, 2009 through March 31, 2010

    Energy Technology Data Exchange (ETDEWEB)

    Antonio, Cheryl L.

    2012-07-19

    A total of 58 urine samples and 10 fecal samples were submitted during the report period (April 1, 2009 through March 31, 2010) to General Engineering Laboratories, South Carolina by the Hanford Internal Dosimetry Program (IDP) to check the accuracy, precision, and detection levels of their analyses. Urine analyses for Sr, 238Pu, 239Pu, 241Am, 243Am 235U, 238U, elemental uranium and fecal analyses for 241Am, 238Pu and 239Pu were tested this year as well as four tissue samples for 238Pu, 239Pu, 241Am and 241Pu. The number of QC urine samples submitted during the report period represented 1.3% of the total samples submitted. In addition to the samples provided by IDP, GEL was also required to conduct their own QC program, and submit the results of analyses to IDP. About 33% of the analyses processed by GEL during the third year of this contract were quality control samples. GEL tested the performance of 21 radioisotopes, all of which met or exceeded the specifications in the Statement of Work within statistical uncertainty (Table 4).

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

    Energy Technology Data Exchange (ETDEWEB)

    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)

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

    Energy Technology Data Exchange (ETDEWEB)

    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.

  11. Fission waves can oscillate

    CERN Document Server

    Osborne, Andrew G

    2016-01-01

    Under the right conditions, self sustaining fission waves can form in fertile nuclear materials. These waves result from the transport and absorption of neutrons and the resulting production of fissile isotopes. When these fission, additional neutrons are produced and the chain reaction propagates until it is poisoned by the buildup of fission products. It is typically assumed that fission waves are soliton-like and self stabilizing. However, we show that in uranium, coupling of the neutron field to the 239U->239Np->239Pu decay chain can lead to a Hopf bifurcation. The fission reaction then ramps up and down, along with the wave velocity. The critical driver for the instability is a delay, caused by the half-life of 239U, between the time evolution of the neutron field and the production of 239Pu. This allows the 239Pu to accumulate and burn out in a self limiting oscillation that is characteristic of a Hopf bifurcation. Time dependent results are obtained using a numerical implementation of a reduced order r...

  12. A sensitivity study on neutronic properties of DUPIC fuel

    Energy Technology Data Exchange (ETDEWEB)

    Choi, Hang Bok; Roh, Gyu Hong [Korea Atomic Energy Research Institute, Taejon (Korea, Republic of)

    1998-12-31

    A sensitivity study has been done to determine the composition of DUPIC fuel from the viewpoint of neutronics fuel design. The spent PWR fuel compositions were generated and fissile contents adjusted by blending fresh uranium after mixing two spent PWR fuel assemblies. The {sup 239}Pu and {sup 235}U enrichments of DUPIC fuel were adjusted by controlling the amount of fresh uranium feed and the ratio of slightly enriched and depleted uranium in the feed uranium. Based on the material balance calculation, it is recommended that DUPIC fuel composition be such that spent PWR fuel utilization is more than 90%. A sensitivity study on the temperature reactivity coefficient of DUPIC fuel and shown that it is desirable to increase the {sup 239}Pu and {sup 235}U contents to reduce both the fuel and coolant temperature coefficients. On the other hand, refueling simulations of the DUPIC core have shown that the channel power peaking factor, which is a measure of the reactor trip margin, increases with the total fissile content. Considering these neutronic characteristics of the DUPIC fuel, it is recommended to have enrichments of 0.45 and 1.00 wt% for {sup 239}Pu and {sup 235}U, respectively. 3 refs., 2 tabs. (Author)

  13. Technical Basis Document: A Statistical Basis for Interpreting Urinary Excretion of Plutonium Based on Accelerator Mass Spectrometry (AMS) for Selected Atoll Populations in the Marshall Islands

    Energy Technology Data Exchange (ETDEWEB)

    Bogen, K; Hamilton, T F; Brown, T A; Martinelli, R E; Marchetti, A A; Kehl, S R; Langston, R G

    2007-05-01

    We have developed refined statistical and modeling techniques to assess low-level uptake and urinary excretion of plutonium from different population group in the northern Marshall Islands. Urinary excretion rates of plutonium from the resident population on Enewetak Atoll and from resettlement workers living on Rongelap Atoll range from <1 to 8 {micro}Bq per day and are well below action levels established under the latest Department regulation 10 CFR 835 in the United States for in vitro bioassay monitoring of {sup 239}Pu. However, our statistical analyses show that urinary excretion of plutonium-239 ({sup 239}Pu) from both cohort groups is significantly positively associated with volunteer age, especially for the resident population living on Enewetak Atoll. Urinary excretion of {sup 239}Pu from the Enewetak cohort was also found to be positively associated with estimates of cumulative exposure to worldwide fallout. Consequently, the age-related trends in urinary excretion of plutonium from Marshallese populations can be described by either a long-term component from residual systemic burdens acquired from previous exposures to worldwide fallout or a prompt (and eventual long-term) component acquired from low-level systemic intakes of plutonium associated with resettlement of the northern Marshall Islands, or some combination of both.

  14. Radionuclide concentrations in soils and vegetation at radioactive-waste disposal Area G during the 1996 growing season. Progress report

    Energy Technology Data Exchange (ETDEWEB)

    Fresquez, P.R.; Vold, E.L.; Naranjo, L. Jr.

    1997-07-01

    Soil and overstory and understory vegetation (washed and unwashed) collected at eight locations within and around Area G--a low-level radioactive solid-waste disposal facility at Los Alamos National laboratory--were analyzed for {sup 3}H, {sup 90}Sr, {sup 238}Pu, {sup 239}Pu, {sup 137}Cs, {sup 234}U, {sup 235}U, {sup 238}U, {sup tot}U, {sup 228}Ac, {sup 214}Bi, {sup 60}Co, {sup 40}K, {sup 54}Mn, {sup 22}Na, {sup 214}Pb, and {sup 208}Tl. Also, heavy metals (Ag, As, Ba, Be, Cd, Cr, Hg, Ni, Pb, Sb, Se, and Tl) in soil and vegetation were determined. In general, most radionuclide concentrations, with the exception of {sup 3}H and {sup 239}Pu, in soils and washed and unwashed overstory and understory vegetation collected from within and around Area G were within upper limit background concentrations. Tritium was detected as high as 14,744 pCi mL{sup {minus}1} in understory vegetation collected from transuranic (TRU) waste pad {number_sign}4, and the TRU waste pad area contained the highest levels of {sup 239}Pu in soils and in understory vegetation as compared to other areas at Area G.

  15. Safe management of actinides in the nuclear fuel cycle: Role of mineralogy; La gestion des actinides dans le cycle du combustible nucleaire: le role de la mineralogie

    Energy Technology Data Exchange (ETDEWEB)

    Ewing, R.C. [Department of Nuclear Engineering and Radiological Sciences, Department of Geological Sciences, Department of Materials Science and Engineering, University of Michigan, Ann Arbor, Michigan 48109-1005 (United States)

    2011-02-15

    During the past 60 years, more than 1800 metric tonnes of Pu, and substantial quantities of the 'minor' actinides, such as Np, Am and Cm, have been generated in nuclear reactors. Some of these transuranium elements can be a source of energy in fission reactions (e.g., {sup 239}Pu), a source of fissile material for nuclear weapons (e.g., {sup 239}Pu and {sup 237}Np), and of environmental concern because of their long-half lives and radiotoxicity (e.g., {sup 239}Pu and {sup 237}Np). There are two basic strategies for the disposition of these heavy elements: (1) to 'burn' or transmute the actinides using nuclear reactors or accelerators; (2) to 'sequester' the actinides in chemically durable, radiation-resistant materials that are suitable for geologic disposal. There has been substantial interest in the use of actinide-bearing minerals, especially isometric pyrochlore, A{sub 2}B{sub 2}O{sub 7} (A rare earths; B = Ti, Zr, Sn, Hf), for the immobilization of actinides, particularly plutonium, both as inert matrix fuels and nuclear waste forms. Systematic studies of rare-earth pyrochlores have led to the discovery that certain compositions (B = Zr, Hf) are stable to very high doses of alpha-decay event damage. Recent developments in our understanding of the properties of heavy element solids have opened up new possibilities for the design of advanced nuclear fuels and waste forms. (author)

  16. The features of neutronic calculations for fast reactors with hybrid cores on the basis of BFS-62-3A critical assembly experiments

    Energy Technology Data Exchange (ETDEWEB)

    Mitenkova, E. F.; Novikov, N. V. [Nuclear Safety Inst. of Russian Academy of Sciences, B. Tulskaya 52, Moscow, 115119 (Russian Federation); Blokhin, A. I. [State Scientific Center of Russian Federation, Inst. of Physics and Power Engineering Named after A.I. Leypunsky, Bondarenko Square 1, Obninsk, Kaluga Region, 249030 (Russian Federation)

    2012-07-01

    The different (U-Pu) fuel compositions are considered for next generation of sodium fast breeder reactors. The considerable discrepancies in axial and radial neutron spectra for hybrid reactor systems compared to the cores with UO{sub 2} fuel cause increasing uncertainty of generating the group nuclear constants in those reactor systems. The calculation results of BFS-62-3A critical assembly which is considered as full-scale model of BN-600 hybrid core with steel reflector specify quite different spectra in local areas. For those systems the MCNP 5 calculations demonstrate significant sensitivity of effective multiplication factor K{sub eff} and spectral indices to nuclear data libraries. For {sup 235}U, {sup 238}U, {sup 239}Pu the results of calculated radial fission rate distributions against the reconstructed ones are analyzed. Comparative analysis of spectral indices, neutron spectra and radial fission rate distributions are performed using the different versions of ENDF/B, JENDL-3.3, JENDL-4, JEFF-3.1.1 libraries and BROND-3 for Fe, Cr isotopes. For analyzing the fission rate sensitivity to the plutonium presence in the fuel {sup 239}Pu is substituted for {sup 235}U (enrichment 90%) in the FA areas containing the plutonium. For {sup 235}U, {sup 238}U, {sup 239}Pu radial fission rate distributions the explanation of pick values discrepancies is based on the group fission constants analyses and possible underestimation of some features at the experimental data recovery method (Westcott factors, temperature dependence). (authors)

  17. Deducing the 236Pu(n,f) and 237Pu(n,f) cross sections via the surrogate ratio method

    Science.gov (United States)

    Hughes, R. O.; Beausang, C. W.; Ross, T. J.; Burke, J. T.; Casperson, R. J.; McCleskey, M.; Cooper, N.; Escher, J. E.; Gell, K. B.; Good, E.; Humby, P.; Saastimoinen, A.; Tarlow, T. D.

    2013-10-01

    The short half-lives associated with certain minor actinide nuclei that are relevant to stockpile stewardship pursuits and the development of next-generation nuclear reactors make direct neutron measurements very challenging. In certain cases, a stable beam and target ``surrogate reaction'' can be used in lieu of the neutron-induced reaction, and the (n,f) cross section can then be deduced indirectly. Agreement between surrogate and direct measurements for (n,f) cross sections in actinide nuclei is usually within 10%. The present work reports on the measurement of the 236Pu(n,f) and 237Pu(n,f) cross sections via 239Pu(p,tf) and 239Pu(p,df) surrogate reactions, respectively. The experiment was performed at the Texas A&M University Cyclotron Facility using a 28.5 MeV proton beam to bombard 239Pu and 235U targets. Outgoing light ions were detected in coincidence with fission fragments using the STAR-LiTe detector array. Results of the analysis will be presented. This work was supported by DoE Grant Numbers: DE-FG52-09NA29454 and DE-FG02-05ER41379 (Richmond), DE-AC52-07NA27344 (LLNL) and DE-FG52-09NA29467 (TAMU).

  18. A sensitivity study on DUPIC fuel composition

    Energy Technology Data Exchange (ETDEWEB)

    Choi, Hang Bok; Roh, Gyu Hong

    1997-01-01

    In DUPIC fuel cycle, the spent pressurized water reactor (PWR) fuel is refabricated as a DUPIC fuel by a dry process. Because the spent PWR fuel composition depends on the initial enrichment and burnup condition of PWR fuel, the composition of a DUPIC fuel is not uniquely defined. Therefore, for the purpose of reducing the effects of such a composition heterogeneity on core performance, a composition adjustment of DUPIC fuel was studies. The composition adjustment was made in two steps: mixing two spent PWR fuel assemblies of higher and lower {sup 239}Pu contents and blending in fresh uranium with the mixed spent PWR fuels. Because the fuel and core performances depend on both the absolute amount of fissile isotopes and the ratio of major fissile isotope contents, a parametric study was performed to determine the reference compositions of {sup 235}U and {sup 239}Pu. The reference enrichments of {sup 235}U and {sup 239}Pu were determined such that the DUPIC core performance is comparable to that of a natural uranium core with high spent PWR fuel utilization and low fuel cycle cost. Under this condition, it is possible to utilize 90% of spent PWR fuels as the DUPIC fuel formula. On average, the amounts of slightly enriched and depleted uranium used for blending correspond to 8.6% and 10.6%, respectively, of the mass of candidate spent PWR fuels. (author). 16 refs., 30 tabs., 9 figs.

  19. Dosimetry of inhaled plutonium-239 dioxide in rodent lung: a morphometric study

    Energy Technology Data Exchange (ETDEWEB)

    Rhoads, K.

    1979-06-01

    Morphometric analysis of rat and hamster lung did not demonstrate any extensive changes in lung composition or structure following inhalation exposure to /sup 239/Pu0/sub 2/ at levels near that for maximum tumor yield in rats. The problem of dosimetry for this compound thus appears to be relatively uncomplicated by any major radiation-induced pathological alterations in the lung. Rat and hamster lung were found to be similar in structure and composition, with few significant differences which could be directly related to the different tumor responses. The distribution of /sup 239/Pu0/sub 2/ particles was not uniform in all regions of the lung; thus estimation of the dose to specific tissues or regions within the lung requires a correction for this effect. Species differences were found for particle distribution in the subpleural region and major airways, and in the spatial association of particles, both of which may affect the tumor development process. These regions contain the principal target cells for tumor production and serve as foci for the origin of tumors. Different dose distributions within these regions may therefore explain, at least in part, the difference in tumor response to inhaled /sup 239/Pu0/sub 2/ for rats and hamsters.

  20. Release of Pu isotopes from the Fukushima Daiichi Nuclear Power Plant accident to the marine environment was negligible.

    Science.gov (United States)

    Bu, Wenting; Fukuda, Miho; Zheng, Jian; Aono, Tatsuo; Ishimaru, Takashi; Kanda, Jota; Yang, Guosheng; Tagami, Keiko; Uchida, Shigeo; Guo, Qiuju; Yamada, Masatoshi

    2014-08-19

    Atmospheric deposition of Pu isotopes from the Fukushima Daiichi Nuclear Power Plant (FDNPP) accident has been observed in the terrestrial environment around the FDNPP site; however, their deposition in the marine environment has not been studied. The possible contamination of Pu in the marine environment has attracted great scientific and public concern. To fully understand this possible contamination of Pu isotopes from the FDNPP accident to the marine environment, we collected marine sediment core samples within the 30 km zone around the FDNPP site in the western North Pacific about two years after the accident. Pu isotopes ((239)Pu, (240)Pu, and (241)Pu) and radiocesium isotopes ((134)Cs and (137)Cs) in the samples were determined. The high activities of radiocesium and the (134)Cs/(137)Cs activity ratios with values around 1 (decay corrected to 15 March 2011) suggested that these samples were contaminated by the FDNPP accident-released radionuclides. However, the activities of (239+240)Pu and (241)Pu were low compared with the background level before the FDNPP accident. The Pu atom ratios ((240)Pu/(239)Pu and (241)Pu/(239)Pu) suggested that global fallout and the pacific proving ground (PPG) close-in fallout are the main sources for Pu contamination in the marine sediments. As Pu isotopes are particle-reactive and they can be easily incorporated with the marine sediments, we concluded that the release of Pu isotopes from the FDNPP accident to the marine environment was negligible.

  1. 238Pu: accumulation, tissue distribution, and excretion in Mayak workers after exposure to plutonium aerosols.

    Science.gov (United States)

    Suslova, Klara G; Sokolova, Alexandra B; Khokhryakov, Viktor V; Miller, Scott C

    2012-03-01

    The alpha spectrometry measurements of specific activity of 238Pu and 239Pu in urine from bioassay examinations of 1,013 workers employed at the radiochemical and plutonium production facilities of the Mayak Production Association and in autopsy specimens of lung, liver, and skeleton from 85 former nuclear workers who died between 1974-2009, are summarized.The accumulation fraction of 238Pu in the body and excreta has not changed with time in workers involved in production of weapons-grade plutonium production (e.g., the plutonium production facility and the former radiochemical facility). The accumulation fraction of 238Pu in individuals exposed to plutonium isotopes at the newer Spent Nuclear Fuel Reprocessing Plant ranged from 0.13% up to 27.5% based on the autopsy data. No statistically significant differences between 238Pu and 239Pu in distribution by the main organs of plutonium deposition were found in the Mayak workers. Based on the bioassay data,the fraction of 238Pu activity in urine is on average 38-69% of the total activity of 238Pu and 239Pu, which correlates with the isotopic composition in workplace air sampled at the Spent Nuclear Fuel Reprocessing Plant. In view of the higher specific activity of 238Pu, the contribution of 238Pu to the total internal dose, particularly in the skeleton and liver, might be expected to continue to increase, and continued surveillance is recommended.

  2. Plutonium concentration and isotopic ratio in soil samples from central-eastern Japan collected around the 1970s

    Science.gov (United States)

    Yang, Guosheng; Zheng, Jian; Tagami, Keiko; Uchida, Shigeo

    2015-04-01

    Obtaining Pu background data in the environment is essential for contamination source identification and assessment of environmental impact of Pu released from the Fukushima Daiichi nuclear power plant (FDNPP) accident. However, no baseline information on Pu isotopes in Fukushima Prefecture has been reported. Here we analyzed 80 surface soil samples collected from the central-eastern Japan during 1969-1977 for 239+240Pu activity concentration and 240Pu/239Pu atom ratio to establish the baseline before the FDNPP accident. We found that 239+240Pu activity concentrations ranged from 0.004 -1.46 mBq g-1, and 240Pu/239Pu atom ratios varied narrowly from 0.148 to 0.229 with a mean of 0.186 +/- 0.015. We also reconstructed the surface deposition density of 241Pu using the 241Pu/239Pu atom ratio in the Japanese fallout reference material. The obtained results indicated that, for the FDNPP-accident released 241Pu, a similar radiation impact can be estimated as was seen for the global fallout deposited 241Pu in the last decades.

  3. Determination of {sup 236}U and transuranium elements in depleted uranium ammunition by {alpha}-spectrometry and ICP-MS

    Energy Technology Data Exchange (ETDEWEB)

    Desideri, D.; Meli, M.A.; Roselli, C.; Testa, C. [General Chemistry Institute, Urbino University, Urbino (Italy); Boulyga, S.F.; Becker, J.S. [Central Department of Analytical Chemistry, Research Centre Juelich, Juelich (Germany)

    2002-11-01

    It is well known that ammunition containing depleted uranium (DU) was used by NATO during the Balkan conflict. To evaluate the origin of DU (the enrichment of natural uranium or the reprocessing of spent nuclear fuel) it is necessary to directly detect the presence of activation products ({sup 236}U, {sup 239}Pu, {sup 240}Pu, {sup 241}Am, and {sup 237}Np) in the ammunition. In this work the analysis of actinides by {alpha}-spectrometry was compared with that by inductively coupled plasma mass spectrometry (ICP-MS) after selective separation of ultratraces of transuranium elements from the uranium matrix. {sup 242}Pu and {sup 243}Am were added to calculate the chemical yield. Plutonium was separated from uranium by extraction chromatography, using tri-n-octylamine (TNOA), with a decontamination factor higher than 10{sup 6}; after elution plutonium was determined by ICP-MS ({sup 239}Pu and {sup 240}Pu) and {alpha}-spectrometry ({sup 239+240}Pu) after electroplating. The concentration of Pu in two DU penetrator samples was 7 x 10{sup -12} g g{sup -1} and 2 x 10{sup -11} g g{sup -1}. The {sup 240}Pu/{sup 239}Pu isotope ratio in one penetrator sample (0.12{+-}0.04) was significantly lower than the {sup 240}Pu/{sup 239}Pu ratios found in two soil samples from Kosovo (0.35{+-}0.10 and 0.27{+-}0.07). {sup 241}Am was separated by extraction chromatography, using di(2-ethylhexyl)phosphoric acid (HDEHP), with a decontamination factor as high as 10{sup 7}. The concentration of {sup 241}Am in the penetrator samples was 2.7 x 10{sup -14} g g{sup -1} and <9.4 x 10{sup -15} g g{sup -1}. In addition {sup 237}Np was detected at ultratrace levels. In general, ICP-MS and {alpha}-spectrometry results were in good agreement.The presence of anthropogenic radionuclides ({sup 236}U, {sup 239}Pu,{sup 240}Pu, {sup 241}Am, and {sup 237}Np) in the penetrators indicates that at least part of the uranium originated from the reprocessing of nuclear fuel. Because the concentrations of

  4. Determination of (236)U and transuranium elements in depleted uranium ammunition by alpha-spectrometry and ICP-MS.

    Science.gov (United States)

    Desideri, D; Meli, M A; Roselli, C; Testa, C; Boulyga, S F; Becker, J S

    2002-11-01

    It is well known that ammunition containing depleted uranium (DU) was used by NATO during the Balkan conflict. To evaluate the origin of DU (the enrichment of natural uranium or the reprocessing of spent nuclear fuel) it is necessary to directly detect the presence of activation products ((236)U, (239)Pu, (240)Pu, (241)Am, and (237)Np) in the ammunition. In this work the analysis of actinides by alpha-spectrometry was compared with that by inductively coupled plasma mass spectrometry (ICP-MS) after selective separation of ultratraces of transuranium elements from the uranium matrix. (242)Pu and (243)Am were added to calculate the chemical yield. Plutonium was separated from uranium by extraction chromatography, using tri- n-octylamine (TNOA), with a decontamination factor higher than 10(6); after elution plutonium was determined by ICP-MS ((239)Pu and (240)Pu) and alpha-spectrometry ((239+240)Pu) after electroplating. The concentration of Pu in two DU penetrator samples was 7 x 10(-12) g g(-1) and 2 x 10(-11) g g(-1). The (240)Pu/(239)Pu isotope ratio in one penetrator sample (0.12+/-0.04) was significantly lower than the (240)Pu/(239)Pu ratios found in two soil samples from Kosovo (0.35+/-0.10 and 0.27+/-0.07). (241)Am was separated by extraction chromatography, using di(2-ethylhexyl)phosphoric acid (HDEHP), with a decontamination factor as high as 10(7). The concentration of (241)Am in the penetrator samples was 2.7 x 10(-14) g g(-1) and <9.4 x 10(-15) g g(-1). In addition (237)Np was detected at ultratrace levels. In general, ICP-MS and alpha-spectrometry results were in good agreement. The presence of anthropogenic radionuclides ((236)U, (239)Pu,(240)Pu, (241)Am, and (237)Np) in the penetrators indicates that at least part of the uranium originated from the reprocessing of nuclear fuel. Because the concentrations of radionuclides are very low, their radiotoxicological effect is negligible.

  5. Long-range tropospheric transport of uranium and plutonium weapons fallout from Semipalatinsk nuclear test site to Norway.

    Science.gov (United States)

    Wendel, Cato Christian; Fifield, L Keith; Oughton, Deborah H; Lind, Ole Christian; Skipperud, Lindis; Bartnicki, Jerzy; Tims, Stephen G; Høibråten, Steinar; Salbu, Brit

    2013-09-01

    A combination of state-of-the-art isotopic fingerprinting techniques and atmospheric transport modelling using real-time historical meteorological data has been used to demonstrate direct tropospheric transport of radioactive debris from specific nuclear detonations at the Semipalatinsk test site in Kazakhstan to Norway via large areas of Europe. A selection of archived air filters collected at ground level at 9 stations in Norway during the most intensive atmospheric nuclear weapon testing periods (1957-1958 and 1961-1962) has been screened for radioactive particles and analysed with respect to the concentrations and atom ratios of plutonium (Pu) and uranium (U) using accelerator mass spectrometry (AMS). Digital autoradiography screening demonstrated the presence of radioactive particles in the filters. Concentrations of (236)U (0.17-23nBqm(-3)) and (239+240)Pu (1.3-782μBqm(-3)) as well as the atom ratios (240)Pu/(239)Pu (0.0517-0.237) and (236)U/(239)Pu (0.0188-0.7) varied widely indicating several different sources. Filter samples from autumn and winter tended to have lower atom ratios than those sampled in spring and summer, and this likely reflects a tropospheric influence in months with little stratospheric fallout. Very high (236)U, (239+240)Pu and gross beta activity concentrations as well as low (240)Pu/(239)Pu (0.0517-0.077), (241)Pu/(239)Pu (0.00025-0.00062) and (236)U/(239)Pu (0.0188-0.046) atom ratios, characteristic of close-in and tropospheric fallout, were observed in filters collected at all stations in Nov 1962, 7-12days after three low-yield detonations at Semipalatinsk (Kazakhstan). Atmospheric transport modelling (NOAA HYSPLIT_4) using real-time meteorological data confirmed that long range transport of radionuclides, and possibly radioactive particles, from Semipalatinsk to Norway during this period was plausible. The present work shows that direct tropospheric transport of fallout from atmospheric nuclear detonations periodically may have

  6. Carcinogenesis From Inhaled (PuO2)-Pu-239 in Beagles: Evidence for Radiation Homeostasis at Low Doses?

    Energy Technology Data Exchange (ETDEWEB)

    Fisher, Darrell R.; Weller, Richard E.

    2010-09-01

    From the early 1970s to the late 1980s, Pacific Northwest National Laboratory conducted life-span studies in beagle dogs on the biological effects of inhaled plutonium (239PuO2, 238PuO2, and 239Pu[NO3]4) to help predict risks associated with accidental intakes in workers. Years later, the purpose of the present follow-up study is to reassess the dose-response relationship for lung cancer induction in the 239PuO2 dogs compared to controls, with particular focus on the dose-response at low lung doses. A 239PuO2 aerosol (2.3 μm AMAD, 1.9 μm GSD) was administered to six groups of 20 young (18-month old) beagle dogs (10 males and 10 females) by inhalation at six different activity levels, as previously described in Laboratory reports. Control dogs were sham-exposed. In dose level 1, initial pulmonary lung depositions were 130 ± 48 Bq (3.5 ± 1.3 nCi), corresponding to 1 Bq g-1 lung tissue (0.029 ± 0.001 nCi g-1. Groups 2 through 6 received initial lung depositions (mean values) of 760, 2724, 10345, 37900, and 200000 Bq (22, 79, 300, 1100, and 5800 nCi) 239PuO2, respectively. For each dog, the absorbed dose to lungs was calculated from the initial lung burden and the final lung burden at time of death and lung mass, assuming a single, long-term retention function. Insoluble plutonium oxide exhibited long retention times in the lungs. Increased dose-dependent mortality due to lung cancer (bronchiolar-alveolar carcinoma, adenocarcinoma, epidermoid carcinoma) and radiation pneumonitis (highest exposures group) was observed in dogs exposed to 239PuO2. Calculated lung doses ranged from a few cGy in early-sacrificed dogs to 7764 cGy in dogs that experienced early deaths from radiation pneumonitis. Data were regrouped by lifetime lung dose and plotted as a function of lung tumor incidence. Lung tumor incidence in controls and zero-dose exposed dogs was 18% (5/28). However, no lung tumors were observed in 16 dogs with the lowest lung doses (8 to 22 cGy, mean 14.4 ± 7.6 c

  7. An assessment of the reported leakage of anthropogenic radionuclides from the underground nuclear test sites at Amchitka Island, Alaska, USA to the surface environment

    Energy Technology Data Exchange (ETDEWEB)

    Dasher, Douglas E-mail: ddasher@envircon.state.ak.us; Hanson, Wayne; Read, Stan; Faller, Scott; Farmer, Dennis; Efurd, Wes; Kelley, John; Patrick, Robert

    2002-07-01

    Three underground nuclear tests representing approximately 15-16% of the total effective energy released during the United States underground nuclear testing program from 1951 to 1992 were conducted at Amchitka Island, Alaska. In 1996, Greenpeace reported that leakage of radionuclides, {sup 241}Am and {sup 239+240}Pu, from these underground tests to the terrestrial and freshwater environments had been detected. In response to this report, a federal, state, tribal and non-governmental team conducted a terrestrial and freshwater radiological sampling program in 1997. Additional radiological sampling was conducted in 1998. An assessment of the reported leakage to the freshwater environment was evaluated by assessing {sup 3} H values in surface waters and {sup 240}Pu/{sup 239}Pu ratios in various sample media. Tritium values ranged from 0.41 Bq/l{+-}0.11 two sigma to 0.74 Bq/l{+-}0.126 two sigma at the surface water sites sampled, including the reported leakage sites. Only at the Long Shot test site, where leakage of radioactive gases to the near-surface occurred in 1965, were higher {sup 3}H levels of 5.8 Bq/l{+-}0.19 two sigma still observed in 1997, in mud pit no. 3. The mean {sup 240}Pu/{sup 239}Pu for all of the Amchitka samples was 0.1991{+-}0.0149 one standard deviation, with values ranging from 0.1824{+-}1.43% one sigma to 0.2431{+-}6.56% one sigma. The measured {sup 3}H levels and {sup 240}Pu/{sup 239}Pu ratios in freshwater moss and sediments at Amchitka provide no evidence of leakage occurring at the sites reported by Buske and Miller (1998 Nuclear-Weapons-Free America and Alaska Community Action on Toxics, Anchorage, Ak, p. 38) and Miller and Buske (1996 Nuclear Flashback: The Return to Anchitka, p. 35). It was noted that the marine sample; {sup 240}Pu/{sup 239}Pu ratios are statistically different than the global fallout ratios presented by Krey et al. (1976) and Kelley, Bond, and Beasley (1999). The additional non-fallout component {sup 240}Pu/{sup 239}Pu

  8. Application of a canine {sup 238}Pu dosimetry model to human bioassay data

    Energy Technology Data Exchange (ETDEWEB)

    Hickman, A.W. Jr. [Florida Univ., Gainesville, FL (United States)

    1991-08-01

    Associated with the use of 2{sup 238}Pu in thermoelectric power sources for space probes and power supplies for cardiac devices is the potential for human exposure to {sup 238}Pu, primarily by inhalation. In the event of human internal exposure, a means is needed for assessing the level of intake and calculating radiation doses. Several bioassay/dosimetry models have been developed for {sup 239}Pu. However, results from studies with laboratory animals have indicated that the biokinetics, and therefore the descriptive models, of {sup 238}Pu are significantly different from those for {sup 239}Pu. A canine model accounting for these differences has been applied in this work to urinary excretion data from seven humans occupationally exposed to low levels of an insoluble {sup 238}Pu compound. The modified model provides a good description of the urinary excretion kinetics observed in the exposed humans. The modified model was also used to provide estimates of the initial intakes of {sup 238}Pu for the seven individuals; these estimates ranged from 4.5 nCi (170 Bq) to 87 nCi (3200 Bq). Autopsy data on the amount and distribution of {sup 238}Pu retained in the organs may be used in the future to validate or refute both these estimates and the assumptions used to formulate the human model. Modification of the human model to simulate an injection exposure to {sup 239}Pu gave patterns of retention in the organs and urinary excretion comparable to those seen previously in humans; further modification of the model using fecal data (unavailable for the subjects of this study) is indicated.

  9. Historical reconstruction of Plutonium contamination in the Swiss-Italian Alps

    Directory of Open Access Journals (Sweden)

    Gabrieli J.

    2013-04-01

    Full Text Available Plutonium is present in the environment as a consequence of atmospheric nuclear tests carried out in the 1960s, nuclear weapons production and releases by the nuclear industry over the past 50 years. Approximately 6 tons of 239Pu have been released into the environment as a result of 541 atmospheric weapon tests Nuclear Pu fallout has been studied in various environmental archives, such as sediments, soil and herbarium grass. Mid-latitude ice cores have been studied as well, on Mont Blanc, the Western Alps and on Belukha Glacier, Siberian Altai. We present a Pu record obtained by analyzing 52 discrete samples of an alpine firn/ice core from Colle Gnifetti (M. Rosa, 4450 m a.s.l., dating from 1945 to 1991. The 239Pu signal was recorded directly, without preliminary cleaning or preconcentration steps, using an high resolution inductively plasma mass spectrometer equipped with a desolvation system. The 239Pu profile reflects the three main periods of atmospheric nuclear weapons testing: the earliest peak lasted from 1954/55 to 1958 and was caused by the first testing period reaching a maximum in 1958. Despite a temporary halt of testing in 1959/60, the Pu concentration decreased only by half with respect to the 1958 peak due to long atmospheric residence times. In 1961/62 Pu concentrations rapidly increased reaching a maximum in 1963. After the signing of the “Limited Test Ban Treaty” between USA and USSR in 1964, Pu deposition decreased very sharply reaching a minimum in 1967. The third period (1967-1975 is characterized by irregular Pu concentrations with smaller peaks which might be related to the deposition of Saharan dust contaminated by the French nuclear tests of the 1960s.

  10. Sequential injection approach for simultaneous determination of ultratrace plutonium and neptunium in urine with accelerator mass spectrometry.

    Science.gov (United States)

    Qiao, Jixin; Hou, Xiaolin; Roos, Per; Lachner, Johannes; Christl, Marcus; Xu, Yihong

    2013-09-17

    An analytical method was developed for simultaneous determination of ultratrace level plutonium (Pu) and neptunium (Np) using iron hydroxide coprecipitation in combination with automated sequential injection extraction chromatography separation and accelerator mass spectrometry (AMS) measurement. Several experimental parameters affecting the analytical performance were investigated and compared including sample preboiling operation, aging time, amount of coprecipitating reagent, reagent for pH adjustment, sedimentation time, and organic matter decomposition approach. The overall analytical results show that preboiling and aging are important for obtaining high chemical yields for both Pu and Np, which is possibly related to the aggregation and adsorption behavior of organic substances contained in urine. Although the optimal condition for Np and Pu simultaneous determination requires 5-day aging time, an immediate coprecipitation without preboiling and aging could also provide fairly satisfactory chemical yields for both Np and Pu (50-60%) with high sample throughput (4 h/sample). Within the developed method, (242)Pu was exploited as chemical yield tracer for both Pu and Np isotopes. (242)Pu was also used as a spike in the AMS measurement for quantification of (239)Pu and (237)Np concentrations. The results show that, under the optimal experimental condition, the chemical yields of (237)Np and (242)Pu are nearly identical, indicating the high feasibility of (242)Pu as a nonisotopic tracer for (237)Np determination in real urine samples. The analytical method was validated by analysis of a number of urine samples spiked with different levels of (237)Np and (239)Pu. The measured values of (237)Np and (239)Pu by AMS exhibit good agreement (R(2) ≥ 0.955) with the spiked ones confirming the reliability of the proposed method.

  11. Distribution of Np and Pu in Swedish lichen samples (Cladonia stellaris) contaminated by atmospheric fallout

    Energy Technology Data Exchange (ETDEWEB)

    Lindahl, Patric E-mail: patric.lindahl@radfys.lu.se; Roos, Per; Eriksson, Mats; Holm, Elis

    2004-07-01

    The activity concentrations of {sup 237}Np and the two Pu isotopes, {sup 239}Pu and {sup 240}Pu, were determined in lichen samples (Cladonia stellaris) contaminated by fallout from atmospheric nuclear test explosions and the Chernobyl accident. The samples were collected at 18 locations in Sweden, from north to south, between 1986 and 1988 and analysed with high-resolution inductively coupled plasma mass spectrometry (HR-ICP-MS) and alpha spectrometry. Data on the activity ratios {sup 238}Pu/{sup 239+240}Pu and {sup 134}Cs/{sup 137}Cs measured previously were also included in this study for comparison. The {sup 237}Np activity concentration ranged from 0.08{+-}0.01 to 2.08{+-}0.17 mBq kg{sup -1}, depending on the location of the sampling site and time of collection. The {sup 239+240}Pu activity concentration ranged from 0.09{+-}0.01 to 4.09{+-}0.15 Bq kg{sup -1}, with the {sup 240}Pu/{sup 239}Pu atomic ratio ranging between 0.16{+-}0.01 and 0.44{+-}0.03, the higher ratios indicating a combination of weapons test fallout and Chernobyl fallout. The {sup 237}Np/{sup 239}Pu atomic ratios ranged between 0.06{+-}0.01 and 0.42{+-}0.04, the lower ratios indicating combination of weapons test fallout and Chernobyl fallout. At a well-defined sampling site at Lake Rogen (62.32 deg. N, 12.38 deg. E), additional lichen samples were collected between 1987 and 1998 to study the distribution of Np and Pu in different layers. The concentrations of the two elements follow each other quite well in the profile.

  12. Ultra-trace determination of plutonium in marine samples using multi-collector inductively coupled plasma mass spectrometry

    Energy Technology Data Exchange (ETDEWEB)

    Lindahl, Patric, E-mail: patriclindahl@yahoo.com [Marine Environment Research Department, Korea Ocean Research and Development Institute, 1270 Sadong, Ansan 426-744 (Korea, Republic of); School of Geography, Earth and Environmental Sciences, University of Plymouth, Drake Circus, Plymouth PL48AA (United Kingdom); Keith-Roach, Miranda; Worsfold, Paul [School of Geography, Earth and Environmental Sciences, University of Plymouth, Drake Circus, Plymouth PL48AA (United Kingdom); Choi, Min-Seok; Shin, Hyung-Seon [Division of Earth and Environmental Science, Korea Basic Science Institute, 113 Gwahangno, Yusung-gu, Daejon 305-333 (Korea, Republic of); Lee, Sang-Hoon [Marine Geology and Geophysics Laboratory, Korea Ocean Research and Development Institute, 1270 Sadong, Ansan 426-744 (Korea, Republic of)

    2010-06-25

    Sources of plutonium isotopes to the marine environment are well defined, both spatially and temporally, which makes Pu a potential tracer for oceanic processes. This paper presents the selection, optimisation and validation of a sample preparation method for the ultra-trace determination of Pu isotopes ({sup 240}Pu and {sup 239}Pu) in marine samples by multi-collector (MC) ICP-MS. The method was optimised for the removal of the interference from {sup 238}U and the chemical recovery of Pu. Comparison of various separation strategies using AG1-X8, TEVA, TRU, and UTEVA resins to determine Pu in marine calcium carbonate samples is reported. A combination of anion-exchange (AG1-X8) and extraction chromatography (UTEVA/TRU) was the most suitable, with a radiochemical Pu yield of 87 {+-} 5% and a U decontamination factor of 1.2 x 10{sup 4}. Validation of the method was accomplished by determining Pu in various IAEA certified marine reference materials. The estimated MC-ICP-MS instrumental limit of detection for {sup 239}Pu and {sup 240}Pu was 0.02 fg mL{sup -1}, with an absolute limit of quantification of 0.11 fg. The proposed method allows the determination of ultra-trace Pu, at femtogram levels, in small size marine samples (e.g., 0.6-2.0 g coral or 15-20 L seawater). Finally, the analytical method was applied to determining historical records of the Pu signature in coral samples from the tropical Northwest Pacific and {sup 239+240}Pu concentrations and {sup 240}Pu/{sup 239}Pu atom ratios in seawater samples as part of the 2008 GEOTRACES intercalibration exercise.

  13. Arctic Ocean sea ice drift origin derived from artificial radionuclides.

    Science.gov (United States)

    Cámara-Mor, P; Masqué, P; Garcia-Orellana, J; Cochran, J K; Mas, J L; Chamizo, E; Hanfland, C

    2010-07-15

    Since the 1950s, nuclear weapon testing and releases from the nuclear industry have introduced anthropogenic radionuclides into the sea, and in many instances their ultimate fate are the bottom sediments. The Arctic Ocean is one of the most polluted in this respect, because, in addition to global fallout, it is impacted by regional fallout from nuclear weapon testing, and indirectly by releases from nuclear reprocessing facilities and nuclear accidents. Sea-ice formed in the shallow continental shelves incorporate sediments with variable concentrations of anthropogenic radionuclides that are transported through the Arctic Ocean and are finally released in the melting areas. In this work, we present the results of anthropogenic radionuclide analyses of sea-ice sediments (SIS) collected on five cruises from different Arctic regions and combine them with a database including prior measurements of these radionuclides in SIS. The distribution of (137)Cs and (239,240)Pu activities and the (240)Pu/(239)Pu atom ratio in SIS showed geographical differences, in agreement with the two main sea ice drift patterns derived from the mean field of sea-ice motion, the Transpolar Drift and Beaufort Gyre, with the Fram Strait as the main ablation area. A direct comparison of data measured in SIS samples against those reported for the potential source regions permits identification of the regions from which sea ice incorporates sediments. The (240)Pu/(239)Pu atom ratio in SIS may be used to discern the origin of sea ice from the Kara-Laptev Sea and the Alaskan shelf. However, if the (240)Pu/(239)Pu atom ratio is similar to global fallout, it does not provide a unique diagnostic indicator of the source area, and in such cases, the source of SIS can be constrained with a combination of the (137)Cs and (239,240)Pu activities. Therefore, these anthropogenic radionuclides can be used in many instances to determine the geographical source area of sea-ice.

  14. Pu-doped zirconolite for minor actinide containment

    Energy Technology Data Exchange (ETDEWEB)

    Deschanels, X.; Broudic, V.; Jegou, C.; Peuget, S.; Roudil, D.; Jorion, F.; Advocat, T

    2004-07-01

    Zirconolite is a potential matrix for the immobilization of the minor actinides stream produced by the reprocessing of the spent fuel. In order to check the incorporation of actinide into the structure, zirconolite ceramic pellets doped with 10 wt% in {sup 239}PuO{sub 2} were sintered. Characterization by SEM, XRD and XANES spectroscopy have been done on this material. The microstructural homogeneity of the pellets is good, and their relative density is higher than 90% of the theoretical density. XANES spectroscopy shows that Pu is at the oxidation state IV in this material. To investigate the effects of radiation damage on zirconolite structure, pellets doped with 10 wt% of {sup 238}PuO{sub 2} were fabricated. The {sup 238}Pu accelerates the radiation damage relative to the {sup 239}Pu because of its much higher specific activity (63.2 x 10{sup 10} Bq/g for {sup 238}Pu vs. 2.2 x 10{sup 9} Bq/g for {sup 238}Pu). Some pellets are storing at ambient, 250 deg. C and 500 deg C. Up 10{sup 19} {alpha}/cm{sup 3}, the macroscopic swelling of the samples stored at ambient is about 0.5% by 10{sup 18} {alpha}/cm{sup 3}, and the microscopic one near 0.35% by 10{sup 18} {alpha}/cm{sup 3}. Some microcracks are observed on these pellets. The samples started to become amorphous at 10{sup 19} {alpha}/cm{sup 3}. The swelling strongly decreases with the storage temperature of the samples. The leaching rate of {sup 239}Pu doped ceramics measured by Soxhlet tests at 100 deg. C in deionized water appears to be the same as inactive material. (authors)

  15. Activation of Alveolar Macrophages after Plutonium Oxide Inhalation in Rats: Involvement in the Early Inflammatory Response

    Energy Technology Data Exchange (ETDEWEB)

    Van der Meeren, A.; Tourdes, F.; Gremy, O.; Grillon, G.; Abram, M.C.; Poncy, J.L.; Griffiths, N. [CEA, DSV, DRR, SRCA, Centre DAM Ile de France, F-91297 Bruyeres Le Chatel, Arpajon (France)

    2008-07-01

    Alveolar macrophages play an important role in the distribution, clearance and inflammatory reactions after particle inhalation, which may influence long-term events such as fibrosis and tumorigenesis. The objectives of the present study were to investigate the early inflammatory events after plutonium oxide inhalation in rats and involvement of alveolar macrophages. Lung changes were studied from 3 days to 3 months after inhalation of PuO{sub 2} or different isotopic compositions (70% or 97% {sup 239}Pu) and initial lung deposits (range 2.1 to 43.4 kBq/rat). Analyses of bronchoalveolar lavages showed early increases in the numbers of granulocytes, lymphocytes and multi-nucleated macrophages. The activation of macrophages was evaluated ex vivo by measurement of inflammatory mediator levels in culture supernatants. TNF-alpha and chemokine MCP-1, MIP-2 and CINC-1 production was elevated from 7 days after inhalation and remained so up to 3 months. In contrast, IL-1 beta, IL-6 and IL-10 production was unchanged. At 6 weeks, pulmonary macrophage numbers and activation state were increased as observed from an immunohistochemistry study of lung sections with anti-ED1. Similarly, histological analyses of lung sections also showed evidence of inflammatory responses. In conclusion, our results indicate early inflammatory changes in the lungs of PuO{sub 2}-contaminated animals and the involvement of macrophages in this process. A dose-effect relationship was observed between the amount of radionuclide inhaled or retained at the time of analysis and inflammatory mediator production by alveolar macrophages 14 days after exposure. For similar initial lung deposits, the inflammatory manifestation appears higher for 97% {sup 239}Pu than for 70% {sup 239}Pu. (authors)

  16. Distributions of Pu isotopes in seawater and bottom sediments in the coast of the Japanese archipelago before and soon after the Fukushima Dai-ichi Nuclear Power Station accident.

    Science.gov (United States)

    Oikawa, Shinji; Watabe, Teruhisa; Takata, Hyoe

    2015-04-01

    A radioactivity measurement survey was carried out from 24 April 2008 to 3 June 2011 to determine the levels of plutonium isotopes and (240)Pu/(239)Pu atom ratios in the marine environments off the sites of commercial nuclear power stations around the Japanese islands; the sampling period extended to two months after the Fukushima Dai-ichi Nuclear Power Station accident. In our previous study (Oikawa et al., 2015), data on Pu isotopes and (241)Am in sediments have already been reported. In this study, we report those on Pu isotopes in seawater as well as sediments, and the characteristics of sediments in addition (e.g., ignition loss and biogenic opals). Concentrations of (239+240)Pu in seawater and bottom sediments remained nearly constant at all sampling locations during the survey period. In addition, no regional differences were observed in the (239+240)Pu concentrations in surface waters. Higher (239+240)Pu concentrations were found in bottom waters at deeper sampling locations, but the (240)Pu/(239)Pu atom ratios were nearly constant regardless of the water depth. Higher (239+240)Pu concentrations were also found in bottom sediments at deeper sampling locations, but vice versa for (240)Pu/(239)Pu atom ratios as reported in the previous report. The sediments samples from deeper locations showed the higher percentage of ignition loss as well as the higher content of biogenic opal. There was likely to be some driving force participating in the transfer of Pu isotopes associated with biogenic substances to the deeper seabed. The present survey showed that the accident at the Fukushima Dai-ichi Nuclear Power Station did not contribute much to the inventory of Pu isotopes in the adjacent sea area.

  17. Lung, liver and bone cancer mortality after plutonium exposure in beagle dogs and nuclear workers.

    Science.gov (United States)

    Wilson, Dulaney A; Mohr, Lawrence C; Frey, G Donald; Lackland, Daniel; Hoel, David G

    2010-01-01

    The Mayak Production Association (MPA) worker registry has shown evidence of plutonium-induced health effects. Workers were potentially exposed to plutonium nitrate [(239)Pu(NO(3))(4)] and plutonium dioxide ((239)PuO(2)). Studies of plutonium-induced health effects in animal models can complement human studies by providing more specific data than is possible in human observational studies. Lung, liver, and bone cancer mortality rate ratios in the MPA worker cohort were compared to those seen in beagle dogs, and models of the excess relative risk of lung, liver, and bone cancer mortality from the MPA worker cohort were applied to data from life-span studies of beagle dogs. The lung cancer mortality rate ratios in beagle dogs are similar to those seen in the MPA worker cohort. At cumulative doses less than 3 Gy, the liver cancer mortality rate ratios in the MPA worker cohort are statistically similar to those in beagle dogs. Bone cancer mortality only occurred in MPA workers with doses over 10 Gy. In dogs given (239)Pu, the adjusted excess relative risk of lung cancer mortality per Gy was 1.32 (95% CI 0.56-3.22). The liver cancer mortality adjusted excess relative risk per Gy was 55.3 (95% CI 23.0-133.1). The adjusted excess relative risk of bone cancer mortality per Gy(2) was 1,482 (95% CI 566.0-5686). Models of lung cancer mortality based on MPA worker data with additional covariates adequately described the beagle dog data, while the liver and bone cancer models were less successful.

  18. Novel insights into Fukushima nuclear accident from isotopic evidence of plutonium spread along coastal rivers.

    Science.gov (United States)

    Evrard, Olivier; Pointurier, Fabien; Onda, Yuichi; Chartin, Caroline; Hubert, Amélie; Lepage, Hugo; Pottin, Anne-Claire; Lefèvre, Irène; Bonté, Philippe; Laceby, J Patrick; Ayrault, Sophie

    2014-08-19

    The Fukushima Dai-ichi Nuclear Power Plant (FDNPP) accident led to important releases of radionuclides into the environment, and trace levels of plutonium (Pu) were detected in northeastern Japan. However, measurements of Pu isotopic atom and activity ratios are required to differentiate between the contributions of global nuclear test fallout and FDNPP emissions. In this study, we used a double-focusing sector field ICP-MS to measure Pu atom and activity ratios in recently deposited sediment along rivers draining the most contaminated part of the inland radioactive plume. Results showed that plutonium isotopes (i.e., (239)Pu, (240)Pu, (241)Pu, and (242)Pu) were detected in all samples, although in extremely low concentrations. The (241)Pu/(239)Pu atom ratios measured in sediment deposits (0.0017-0.0884) were significantly higher than the corresponding values attributed to the global fallout (0.00113 ± 0.00008 on average for the Northern Hemisphere between 31°-71° N: Kelley, J. M.; Bond, L. A.; Beasley, T. M. Global distribution of Pu isotopes and (237)Np. Sci. Total. Env. 1999, 237/238, 483-500). The results indicated the presence of Pu from FDNPP, in slight excess compared to the Pu background from global fallout that represented up to ca. 60% of Pu in the analyzed samples. These results demonstrate that this radionuclide has been transported relatively long distances (∼45 km) from FDNPP and been deposited in rivers representing a potential source of Pu to the ocean. In future, the high (241)Pu/(239)Pu atom ratio of the Fukushima accident sourced-Pu should be measured to quantify the supply of continental-originating material from Fukushima Prefecture to the Pacific Ocean.

  19. Analysis of {sup 236}U and plutonium isotopes, {sup 239,240}Pu, on the 1 MV AMS system at the Centro Nacional de Aceleradores, as a potential tool in oceanography

    Energy Technology Data Exchange (ETDEWEB)

    Chamizo, Elena; López-Lora, Mercedes [Centro Nacional de Aceleradores (Universidad de Sevilla, Consejo Superior de Investigaciones Científicas, Junta de Andalucía), Thomas Alva Edison 7, 41092 Seville (Spain); Villa, María [Departamento de Física Aplicada II, Universidad de Sevilla, Av. Reina Mercedes 4A, 41012 Seville (Spain); Servicio de Radioisótopos, Centro de Investigación, Tecnología e Innovación, Universidad de Sevilla, Av. Reina Mercedes 4B, 41012 Seville (Spain); Casacuberta, Núria [Laboratory of Ion Beam Physics, ETH Zürich, Otto-Stern-Weg 5, CH-8093 Zürich (Switzerland); López-Gutiérrez, José María [Centro Nacional de Aceleradores (Universidad de Sevilla, Consejo Superior de Investigaciones Científicas, Junta de Andalucía), Thomas Alva Edison 7, 41092 Seville (Spain); Departamento de Física Aplicada I, Escuela Universitaria Politécnica, Universidad de Sevilla, Virgen de África 7, 41011 Seville (Spain); Pham, Mai Khanh [IAEA-Environment Laboratories, Monte Carlo 98000 (Monaco)

    2015-10-15

    The performance of the 1 MV AMS system at the CNA (Centro Nacional de Aceleradores, Seville, Spain) for {sup 236}U and {sup 239,240}Pu measurements has been extensively investigated. A very promising {sup 236}U/{sup 238}U abundance sensitivity of about 3 × 10{sup −11} has been recently achieved, and background figures for {sup 239}Pu of about 10{sup 6} atoms were reported in the past. These promising results lead to the use of conventional low energy AMS systems for the analysis of {sup 236}U and {sup 239}Pu and its further application in environmental studies. First {sup 236}U results obtained on our AMS system for marine samples (sediments and water) are presented here. Results of two new IAEA reference materials (IAEA-410 and IAEA-412, marine sediments from Pacific Ocean) are reported. The obtained {sup 236}U/{sup 239}Pu atom ratios, of 0.12 and 0.022, respectively, show a dependency with the contamination source (i.e. local fallout from the US tests performed at the Bikini Atoll and general fallout). The results obtained for a third IAEA reference material (IAEA-381, seawater from the Irish Sea), are also presented. In the following, the uranium and plutonium isotopic compositions obtained on a set of 5 intercomparison seawater samples from the Arctic Ocean provided by the ETH Zürich are discussed. By comparing them with the obtained results on the 600 kV AMS facility Tandy at the ETH Zürich, we demonstrate the solidity of the CNA technique for {sup 236}U/{sup 238}U determinations at, at least, 7 × 10{sup −10} level. Finally, these results are discussed in their environmental context.

  20. Managing the Nuclear Fuel Cycle: Policy Implications of Expanding Global Access to Nuclear Power

    Science.gov (United States)

    2010-03-05

    with uranium to make mixed-oxide ( MOX ) fuel, in which the 239Pu largely substitutes for 235U. Two French reprocessing plants at La Hague can each...and France also have older plants to reprocess gas-cooled reactor fuel, and India has a 275-ton plant.53 About 200 metric tons of MOX fuel is used...to make MOX fuel for today’s nuclear power plants are modest. Existing commercial light water reactors use ordinary water to slow down, or “moderate

  1. Polycrystalline gamma plutonium's elastic moduli versus temperature

    Energy Technology Data Exchange (ETDEWEB)

    Migliori, Albert [Los Alamos National Laboratory; Betts, J [Los Alamos National Laboratory; Trugman, A [Los Alamos National Laboratory; Mielke, C H [Los Alamos National Laboratory; Mitchell, J N [Los Alamos National Laboratory; Ramos, M [Los Alamos National Laboratory; Stroe, I [WORCESTER POLYTECHNIC INSTITUTE

    2009-01-01

    Resonant ultrasound spectroscopy was used to measure the elastic properties of pure polycrystalline {sup 239}Pu in the {gamma} phase. Shear and longitudinal elastic moduli were measured simultaneously and the bulk modulus was computed from them. A smooth, linear, and large decrease of all elastic moduli with increasing temperature was observed. They calculated the Poisson ratio and found that it increases from 0.242 at 519 K to 0.252 at 571 K. These measurements on extremely well characterized pure Pu are in agreement with other reported results where overlap occurs.

  2. Assessment and reduction of proliferation risk of reactor-gradeplutonium regarding construction of ‘fizzle bombs’ by terrorists

    OpenAIRE

    Serfontein, Dawid E.; Mulder, Eben J.; Reitsma, Frederik

    2014-01-01

    The approximately 23.7 wt% 240Pu in reactor-grade plutonium denatures the 239Pu to the extent that it cannot fuel high yield nuclear weapons. 240Pu has a high spontaneous fission rate, which increases the spontaneous neutron flux within the fuel. When such a nuclear weapon is triggered, these neutrons cause the nuclear fission chain reaction to pre-detonate which blows the imploding fuel shell apart before the designed level of compression and reactivity could be attained, thereby greatly red...

  3. Consistency among integral measurements of aggregate decay heat power

    Energy Technology Data Exchange (ETDEWEB)

    Takeuchi, H.; Sagisaka, M.; Oyamatsu, K.; Kukita, Y. [Nagoya Univ. (Japan)

    1998-03-01

    Persisting discrepancies between summation calculations and integral measurements force us to assume large uncertainties in the recommended decay heat power. In this paper, we develop a hybrid method to calculate the decay heat power of a fissioning system from those of different fissioning systems. Then, this method is applied to examine consistency among measured decay heat powers of {sup 232}Th, {sup 233}U, {sup 235}U, {sup 238}U and {sup 239}Pu at YAYOI. The consistency among the measured values are found to be satisfied for the {beta} component and fairly well for the {gamma} component, except for cooling times longer than 4000 s. (author)

  4. Fine structure of histograms of alpha-activity measurements depends on direction of alpha particles flow and the Earth rotation: experiments with collimators

    CERN Document Server

    Shnoll, S E; Berulis, I I; Udaltsova, N V; Rubinstein, I A; Shnoll, Simon E.; Zenchenko, Konstantin I.; Berulis, Iosas I.; Udaltsova, Natalia V.; Rubinstein, Ilia A.

    2004-01-01

    The fine structure of histograms of measurements of 239Pu alpha-activity varies periodically, and the period of these variations is equal to sidereal day (1436 minutes). The periodicity is not observed in the experiments with collimator that restricts the alpha particles flow to be oriented to the Polar Star. Based on this study and other independent data, such as measurements conducted by the Arctic expedition, and similarity of the histograms in processes observed at different locations at the same local time, the conclusion was made, that the fine structure of statistical distributions of the observed processes depends on the celestial sphere.

  5. Tank 241-S-304, Grab samples, 304S-98-1, 304S-98-2 and 304S-98-3 analytical results for the final report

    Energy Technology Data Exchange (ETDEWEB)

    STEEN, F.H.

    1999-02-23

    This document is the final report for tank 241-S-304 grab samples. Four grab samples were collected from riser 4 on July 30, 1998. Analyses were performed in accordance with the Compatibility Grab Sampling and Analysis Plan (TSAP) (Sasaki, 1998) and the Data Quality Objectives for Tank Farms Waste Compatibility Program (DQO). The analytical results are presented in the data summary report (Table 1). None of the subsamples submitted for differential scanning calorimetry (DSC), total organic carbon (TOC) and plutonium 239 (Pu239) analyses exceeded the notification limits as stated in TSAP (Saaaki, 1998).

  6. Analysis on the Isotopic Ratio of Picogram Pu by TIMS%皮克量级钚同位素丰度比的TIMS分析

    Institute of Scientific and Technical Information of China (English)

    杨天丽; 龙开明; 刘雪梅; 刘钊; 汤磊

    2005-01-01

    The isotopic abundance ratios for Pu at 6.7 pg level were measured by thermal surface ionization mass spectrometry (TIMS). During the preparation of Pu samples carbon power was used as an emitting and stabilizing reagent, which increase the collection efficiency, the ion current intense and the ion emission stability for Pu. The measurment results indicate that the relative standard deviation of 2.7% for the isotopic abundance ratios of 240Pu to 239Pu is achieved when the 240Pu ion current is 8-20 cps.

  7. TANGRA-Setup for the Investigation of Nuclear Fission induced by 14.1 MeV neutrons

    OpenAIRE

    RUSKOV I.; Kopatch, Y; BYSTRITSKY V.; Skoy, V.; SHVETSOV V.; Hambsch, Franz-Josef; Oberstedt, Stephan; CAPOTE NOY R.; Sedyshev, P.; GROZDANOV D.; IVANOV I. Zh.; ALEKSAKHIN V. Yu.; BOGOLUBOV E. P.; BARMAKOV Y.; Khabarov, S. V.

    2015-01-01

    The new experimental setup TANGRA (Tagged Neutrons & Gamma Rays), for the investigation of neutron induced nuclear reactions, e.g. (n,xn’), (n,xn’γ), (n,γ), (n,f), on a number of important isotopes for nuclear science and engineering (235,238U, 237Np, 239Pu, 244,245,248Cm) is under construction and being tested at the Frank Laboratory of Neutron Physics (FLNP) of the Joint Institute for Nuclear Research (JINR) in Dubna. The TANGRA setup consists of: a portable neutron generator ING-27, wit...

  8. Design optimization of radiation shielding structure for lead slowing-down spectrometer system

    OpenAIRE

    Jeong Dong Kim; Sangjoon Ahn; Yong Deok Lee; Chang Je Park

    2015-01-01

    A lead slowing-down spectrometer (LSDS) system is a promising nondestructive assay technique that enables a quantitative measurement of the isotopic contents of major fissile isotopes in spent nuclear fuel and its pyroprocessing counterparts, such as 235U, 239Pu, 241Pu, and, potentially, minor actinides. The LSDS system currently under development at the Korea Atomic Energy Research Institute (Daejeon, Korea) is planned to utilize a high-flux (>1012 n/cm2·s) neutron source comprised of a high...

  9. U, Pu, and Am nuclear signatures of the Thule hydrogen bomb debris.

    Science.gov (United States)

    Eriksson, Mats; Lindahl, Patric; Roos, Per; Dahlgaard, Henning; Holm, Elis

    2008-07-01

    This study concerns an arctic marine environment that was contaminated by actinide elements after a nuclear accident in 1968, the so-called Thule accident In this study we have analyzed five isolated hot particles as well as sediment samples containing particles from the weapon material for the determination of the nuclear fingerprint of the accident. We report that the fissile material in the hydrogen weapons involved in the Thule accident was a mixture of highly enriched uranium and weapon-grade plutonium and that the main fissile material was 235U (about 4 times more than the mass of 239Pu). In the five hot particles examined, the measured uranium atomic ratio was 235U/238U = 1.02 +/- 0.16 and the Pu-isotopic ratios were as follows: 24Pu/239Pu = 0.0551 +/- 0.0008 (atom ratio), 238Pu/239+240Pu = 0.0161 +/- 0.0005 (activity ratio), 241Pu/239+240Pu = 0.87 +/- 0.12 (activity ratio), and 241Am/ 239+240Pu = 0.169 +/- 0.005 (activity ratio) (reference date 2001-10-01). From the activity ratios of 241Pu/241Am, we estimated the time of production of this weapon material to be from the late 1950s to the early 1960s. The results from reanalyzed bulk sediment samples showed the presence of more than one Pu source involved in the accident, confirming earlier studies. The 238Pu/239+240PU activity ratio and the 240Pu/ 239Pu atomic ratio were divided into at least two Pu-isotopic ratio groups. For both Pu-isotopic ratios, one ratio group had identical ratios as the five hot particles described above and for the other groups the Pu isotopic ratios were lower (238Pu/ 239+240PU activity ratio approximately 0.01 and the 240Pu/P239Pu atomic ratio 0.03). On the studied particles we observed that the U/Pu ratio decreased as a function of the time these particles were present in the sediment. We hypothesis that the decrease in the ratio is due to a preferential leaching of U relative to Pu from the particle matrix.

  10. Analysis of nuclear materials by energy dispersive x-ray fluorescence and spectral effects of alpha decay

    Energy Technology Data Exchange (ETDEWEB)

    Worley, Christopher G [Los Alamos National Laboratory

    2009-01-01

    Energy dispersive X-ray fluorescence (EDXRF) spectra collected from alpha emitters are complicated by artifacts inherent to the alpha decay process, particularly when using portable instruments. For example, {sup 239}Pu EDXRF spectra exhibit a prominent uranium L X-ray emission peak series due to sample alpha decay rather than source-induced X-ray fluorescence. A portable EDXRF instrument was used to collect spectra from plutonium, americium, and a Pu-contaminated steel sample. The plutonium sample was also analyzed by wavelength dispersive XRF to demonstrate spectral differences observed when using these very different instruments.

  11. An application of the RFQ Linac: Nuclear waste assay characterization

    Science.gov (United States)

    Lamkin, K.; Schultz, F.; Womble, P.; Humphrey, D.; Vourvopoulos, G.

    1997-02-01

    A collaboration between Oak Ridge National Laboratory and Western Kentucky University examines the problem of characterization and assay of nuclear waste with high intrinsic neutron and gamma-ray fields. This waste is defined as Remote Handled-Transuranic waste (RH-TRU). A Radiofrequency Quadrupole Linac is used to produce pulses of neutrons, which impinge on the drum that contains the nuclear waste. The neutrons, after being thermalized in the matrix of the drum, are captured by the fissile material (239Pu or 235U), which releases fast neutrons upon fission. Experimental results will be presented to show the versatility of employing the RFQ with the Differential Die-away Technique.

  12. In vivo measurement of actinides in the human lung. [Calibration and comparison of Phoswich, large-area proportional counter, and intrinsic germanium planar array detector systems

    Energy Technology Data Exchange (ETDEWEB)

    Anderson, A.L.; Campbell, G.W.; Griffith, R.V.

    1979-11-06

    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, /sup 238/Pu, /sup 239/Pu, and /sup 241/Am.

  13. Detection of {alpha} particles using semiconductors. Application to the control of plutonium extraction; Detection des particules {alpha} par semiconducteurs application au controle de l'extraction du plutonium

    Energy Technology Data Exchange (ETDEWEB)

    Tanguy, J. [Commissariat a l' Energie Atomique, Saclay (France). Centre d' Etudes Nucleaires

    1968-03-01

    A study is made of a particles produced by thick sources, using either diffused junction or surface barrier semiconductor detectors for controlling continuously the plutonium extraction process. For this, a presenting apparatus is described in which the solutions to be analyzed flow in contact with the detector protected by a thin mica membrane. A method is described which gives a precise recording of the spectra and which thus allows the separation of two or more {alpha} emitters present in the same solution. This method has been applied to the measurement of {sup 239}Pu in the the presence of {sup 241}Am with an accuracy of {+-}5 per cent. In the second part of the report is considered the detection of plutonium in solutions of {beta} - {gamma} emitting fission products. Pile-up is reduced by using a fast amplification chain associated to totally depleted thin detectors. Under these conditions a few mg of {sup 239}Pu can be detected in solutions of fission products having an activity of 100 curies/liter. A method is given for discriminating {alpha} and {beta} particles, it is based on the difference in the collection times for the charges liberated by these particles in the detector. (author) [French] On etudie la detection de particules {alpha} issues de sources epaisses par detecteurs semiconducteurs a jonction diffusee ou a barriere de surface pour le controle continu du procede d'extraction du plutonium. A cet effet on decrit un appareil presentateur dans lequel les solutions a analyser circulent au contact du detecteur protege par une membrane mince de mica. On decrit une methode qui permet par le trace precis des spectres de separer deux ou plusieurs emetteurs {alpha} presents dans une meme solution. Cette methode a ete appliquee a la mesure du {sup 239}Pu en presence de {sup 241}Am avec une precision de {+-} 5 pour cent. Dans la deuxieme partie on traite de la detection du plutonium dans des solutions de produits de fission emetteurs {beta} and {gamma

  14. Determination of the counting efficiency of phoswich detectors for the assessment of internal contamination in lungs and lymph nodes by using a mathematical model

    Science.gov (United States)

    Righetti, M. A.; Hernandez, D.; Spano, F.

    1989-08-01

    This article presents the comparison between the results obtained by applying a mathematical and a physical model to the determination of the calibration factors for the direct measurements of the 239Pu and 241Am burden in lungs and lymph nodes. The mathematical model simulates the photon transport through a modified MIRD-V male phantom using the Monte Carlo technique. The physical model is a Livermore phantom supplied by the IAEA under the frame of the contract no. 3698/RI/CF. The results obtained show a good agreement between both models, since the differences are smaller than 13%.

  15. Calculation Analysis of San Onofre Depletion MOX Fuel Experiment

    Energy Technology Data Exchange (ETDEWEB)

    Pavlovichev, AM

    2001-08-31

    The report provides calculation results of isotopic composition of spent MOX fuel irradiated in Sun Onofre PWR reactor. The calculation was performed by means of the MCU/BURNUP Monte Carlo code. The code is developed in Kurchatov Institute, Russia. The predicted isotope contents are compared with the measured ones. A purpose of this work is a verification both the code and the model of experiment description. Predicted plutonium content exceeds the measured one approximately by 3%. It is arise mainly from error of {sup 239}Pu isotope. Isotopic contents of the main plutonium and uranium isotopes are predicted with satisfactory precision.

  16. Leaching characteristics of actinides from simulated reactor waste glass

    Energy Technology Data Exchange (ETDEWEB)

    Weed, H.C.; Coles, D.G.; Bradley, D.J.; Mensing, R.W.; Schweiger, J.S.; Rego, J.H.

    1979-08-01

    Even without statistical analysis, some general trends can be seen in the results: leach rate increases with flow rate at high temperature, but is approximately independent of it at room temperature; agreement between the results from the one-pass method and those from the IAEA method are fair in the case of WIPP brine solution, and good in the case of the others; and the /sup 237/Np leach rate increases with temperature, but the /sup 239/Pu leach rate either decreases with temperature or does not change.

  17. Angular Anisotropy of the Fission Fragments in the Dinuclear System Mo del

    Institute of Scientific and Technical Information of China (English)

    T. M. Shneidman; A. V. Andreev; C. Massimi; M. T. Pigni; G. Vannini; A. Ventura; S. G. Zhou

    2015-01-01

    A theoretical evaluation of the collective excitation spectra of nucleus at large deformations is possible within the framework of the dinuclear system (DNS) model, which treats the wave function of the fissioning nucleus as a superposition of a mononucleus configuration and two-cluster configurations in a dynamical way, permitting exchange of nucleons between clusters. In this work the method of calculation of the potential energy and the collective spectrum of fissioning nucleus at scission point is presented. Combining the DNS model calculations and the statistical model of fission we calculate the angular distribution of fission fragments for the neutron–induced fission of 239Pu.

  18. Application of the dinuclear system model to fission process

    Directory of Open Access Journals (Sweden)

    Andreev A. V.

    2016-01-01

    Full Text Available A theoretical evaluation of the collective excitation spectra of nucleus at large deformations is possible within the framework of the dinuclear system model, which treats the wave function of the fissioning nucleus as a superposition of a mononucleus configuration and two-cluster configurations in a dynamical way, permitting exchange of nucleons between clusters. In this work the method of calculation of the potential energy and the collective spectrum of fissioning nucleus at scission point is presented. Combining the DNS model calculations and the statistical model of fission we calculate the mass, total kinetic energy, and angular distribution of fission fragments for the neutron–induced fission of 239Pu.

  19. Uptake and translocation of plutonium in two plant species using hydroponics.

    Science.gov (United States)

    Lee, J H; Hossner, L R; Attrep, M; Kung, K S

    2002-01-01

    This study presents determinations of the uptake and translocation of Pu in Indian mustard (Brassica juncea) and sunflower (Helianthus annuus) from Pu contaminated solution media. The initial activity levels of Pu were 18.50 and 37.00 Bq ml(-1), for Pu-nitrate [239Pu(NO3)4] and for Pu-citrate [239Pu(C6H5O7)+] in nutrient solution. Plutonium-diethylenetriaminepentaacetic acid (DTPA: [239Pu-C14H23O10N3] solution was prepared by adding 0, 5, 10, and 50 microg of DTPA ml(-1) with 239Pu(NO3)4 in nutrient solution. Concentration ratios (CR, Pu concentration in dry plant material/Pu concentration in nutrient solution) and transport indices (Tl, Pu content in the shoot/Pu content in the whole plant) were calculated to evaluate Pu uptake and translocation. All experiments were conducted in hydroponic solution in an environmental growth chamber. Plutonium concentration in the plant tissue was increased with increased Pu contamination. Plant tissue Pu concentration for Pu-nitrate and Pu-citrate application was not correlated and may be dependent on plant species. For plants receiving Pu-DTPA, the Pu concentration was increased in the shoots but decreased in the roots resulting in a negative correlation between the Pu concentrations in the plant shoots and roots. The Pu concentration in shoots of Indian mustard was increased for application rates up to 10 microg DTPA ml(-1) and up to 5 microg DTPA ml(-1) for sunflower. Similar trends were observed for the CR of plants compared to the Pu concentration in the shoots and roots, whereas the Tl was increased with increasing DTPA concentration. Plutonium in shoots of Indian mustard was up to 10 times higher than that in shoots of sunflower. The Pu concentration in the apparent free space (AFS) of plant root tissue of sunflower was more affected by concentration of DTPA than that of Indian mustard.

  20. Appendix to Health and Safety Laboratory environmental quarterly report. [Fallout radionuclides deposited and in surface air at various world sites; /sup 137/Cs and /sup 90/Sr in milk and drinking water in New York City; and stable Pb in surface air

    Energy Technology Data Exchange (ETDEWEB)

    Hardy, E.P. Jr.

    1977-07-01

    Tabulated data are presented on the deposition of fallout /sup 89/Sr and /sup 90/Sr at various world land sites through 1976; the ..gamma.. spectra and content of /sup 7/Be, /sup 95/Zr, /sup 137/Cs, /sup 144/Ce, /sup 90/Sr, /sup 210/Pb, /sup 238/Pu, /sup 239/Pu, and stable Pb in samples of surface air collected during 1966 at various world sites; and the content of fallout /sup 137/Cs and /sup 90/Sr in samples of drinking water and milk collected in New York City through 1976. (CH)

  1. Radioelement studies in the oceans. Progress report, January 1, 1977--December 31, 1977. [Transport of fallout radionuclides in Atlantic and Pacific Oceans and Mediterranean Sea during 1977

    Energy Technology Data Exchange (ETDEWEB)

    Bowen, V.T.

    1978-04-01

    Data are reported on the content of various fallout radionuclides in samples of seawater and sediments collected during 1977 in the Atlantic Ocean, Mediterranean Sea, and Pacific Ocean. Methods used for the preparation of samples for radiometric analysis are described briefly. Radionuclides found included /sup 137/Cs, /sup 134/Cs, /sup 242/Cm, /sup 244/Cm, /sup 90/Sr, /sup 238/Pu, /sup 239/Pu, /sup 240/Pu, and /sup 241/Am. A list is included of publications during the time period covered by this report.

  2. Systematics of fission cross sections at the intermediate energy region

    Energy Technology Data Exchange (ETDEWEB)

    Fukahori, Tokio; Chiba, Satoshi [Japan Atomic Energy Research Inst., Tokai, Ibaraki (Japan). Tokai Research Establishment

    1997-03-01

    The systematics was obtained with fitting experimental data for proton induced fission cross sections of Ag, {sup 181}Ta, {sup 197}Au, {sup 206,207,208}Pb, {sup 209}Bi, {sup 232}Th, {sup 233,235,238}U, {sup 237}Np and {sup 239}Pu above 20 MeV. The low energy cross section of actinoid nuclei is omitted from systematics study, since the cross section has a complicated shape and strongly depends on characteristic of nucleus. The fission cross sections calculated by the systematics are in good agreement with experimental data. (author)

  3. Chronology of Pu isotopes and {sup 236}U in an Arctic ice core

    Energy Technology Data Exchange (ETDEWEB)

    Wendel, C.C., E-mail: cato.wendel@umb.no [Isotope Laboratory, Department of Plant and Environmental Sciences, Agricultural University of Norway, P.O. Box 5003, N-1432 Aas (Norway); Oughton, D.H., E-mail: deborah.oughton@umb.no [Isotope Laboratory, Department of Plant and Environmental Sciences, Agricultural University of Norway, P.O. Box 5003, N-1432 Aas (Norway); Lind, O.C., E-mail: ole-christian.lind@umb.no [Isotope Laboratory, Department of Plant and Environmental Sciences, Agricultural University of Norway, P.O. Box 5003, N-1432 Aas (Norway); Skipperud, L., E-mail: lindis.skipperud@umb.no [Isotope Laboratory, Department of Plant and Environmental Sciences, Agricultural University of Norway, P.O. Box 5003, N-1432 Aas (Norway); Fifield, L.K., E-mail: keith.fifield@anu.edu.au [Department of Nuclear Physics, Australian National University, Canberra ACT 0200 (Australia); Isaksson, E., E-mail: elisabeth.isaksson@npolar.no [Norwegian Polar Institute, Fram Centre, Hjalmar Johansens Gate 14, N9296 Tromsø (Norway); Tims, S.G., E-mail: steve.tims@anu.edu.au [Department of Nuclear Physics, Australian National University, Canberra ACT 0200 (Australia); Salbu, B., E-mail: brit.salbu@umb.no [Isotope Laboratory, Department of Plant and Environmental Sciences, Agricultural University of Norway, P.O. Box 5003, N-1432 Aas (Norway)

    2013-09-01

    In the present work, state of the art isotopic fingerprinting techniques are applied to an Arctic ice core in order to quantify deposition of U and Pu, and to identify possible tropospheric transport of debris from former Soviet Union test sites Semipalatinsk (Central Asia) and Novaya Zemlya (Arctic Ocean). An ice core chronology of {sup 236}U, {sup 239}Pu, and {sup 240}Pu concentrations, and atom ratios, measured by accelerator mass spectrometry in a 28.6 m deep ice core from the Austfonna glacier at Nordaustlandet, Svalbard is presented. The ice core chronology corresponds to the period 1949 to 1999. The main sources of Pu and {sup 236}U contamination in the Arctic were the atmospheric nuclear detonations in the period 1945 to 1980, as global fallout, and tropospheric fallout from the former Soviet Union test sites Novaya Zemlya and Semipalatinsk. Activity concentrations of {sup 239+240}Pu ranged from 0.008 to 0.254 mBq cm{sup −2} and {sup 236}U from 0.0039 to 0.053 μBq cm{sup −2}. Concentrations varied in concordance with {sup 137}Cs concentrations in the same ice core. In contrast to previous published results, the concentrations of Pu and {sup 236}U were found to be higher at depths corresponding to the pre-moratorium period (1949 to 1959) than to the post-moratorium period (1961 and 1962). The {sup 240}Pu/{sup 239}Pu ratio ranged from 0.15 to 0.19, and {sup 236}U/{sup 239}Pu ranged from 0.18 to 1.4. The Pu atom ratios ranged within the limits of global fallout in the most intensive period of nuclear atmospheric testing (1952 to 1962). To the best knowledge of the authors the present work is the first publication on biogeochemical cycles with respect to {sup 236}U concentrations and {sup 236}U/{sup 239}Pu atom ratios in the Arctic and in ice cores. - Highlights: • Concentrations and atom ratios of Pu and {sup 236}U determined in an Arctic ice core. • Concentrations of U and Pu found to be higher pre- than post-moratorium. • U and Pu concentrations

  4. Assessing the role of the (n, γ f process in the low-energy fission of actinides

    Directory of Open Access Journals (Sweden)

    Talou Patrick

    2016-01-01

    Full Text Available 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.

  5. The CIELO Collaboration: Progress in International Evaluations of Neutron Reactions on Oxygen, Iron, Uranium and Plutonium

    Energy Technology Data Exchange (ETDEWEB)

    Chadwick, M. B.; Capote, R.; Trkov, A.; Kahler, A. C.; Herman, M. W.; Brown, D. A.; Hale, G. M.; Pigni, M.; Dunn, M.; Leal, L.; Plompen, A.; Schillebeecks, P.; Hambsch, F. -J.; Kawano, T.; Talou, P.; Jandel, M.; Mosby, S.; Lestone, J.; Neudecker, D.; Rising, M.; Paris, M.; Nobre, G. P. A.; Arcilla, R.; Kopecky, S.; Giorginis, G.; Cabellos, O.; Hill, I.; Dupont, E.; Danon, Y.; Jing, Q.; Zhigang, G.; Tingjin, L.; Hanlin, L.; Xichao, R.; Haicheng, W.; Sin, M.; Bauge, E.; Romain, P.; Morillon, B.; Salvatores, M.; Jacqmin, R.; Bouland, O.; De Saint Jean, C.; Pronyaev, V. G.; Ignatyuk, A.; Yokoyama, K.; Ishikawa, M.; Fukahori, T.; Iwamoto, N.; Iwamoto, O.; Kuneada, S.; Lubitz, C. R.; Palmiotti, G.; Kodeli, I.; Kiedrowski, B.; Roubtsov, D.; Thompson, I.; Quaglioni, S.; Kim, H. I.; KLee, Y. O.; Koning, A. J.; Carlson, A.; Fischer, U.

    2016-11-01

    The CIELO collaboration has studied neutron cross sections on nuclides that significantly impact criticality in nuclear technologies - 16O, 56Fe, 235,8U and 239Pu - with the aim of reducing uncertainties and resolving previous discrepancies in our understanding. This multi-laboratory pilot project, coordinated via the OECD/NEA Working Party on Evaluation Cooperation (WPEC) Subgroup 40 with support also from the IAEA, has motivated experimental and theoretical work and led to suites of new evaluated libraries that accurately reflect measured data and also perform well in integral simulations of criticality.

  6. Evolution of the Reactor Antineutrino Flux and Spectrum at Daya Bay.

    Science.gov (United States)

    An, F P; Balantekin, A B; Band, H R; Bishai, M; Blyth, S; Cao, D; Cao, G F; Cao, J; Chan, Y L; Chang, J F; Chang, Y; Chen, H S; Chen, Q Y; Chen, S M; Chen, Y X; Chen, Y; Cheng, J; Cheng, Z K; Cherwinka, J J; Chu, M C; Chukanov, A; Cummings, J P; Ding, Y Y; Diwan, M V; Dolgareva, M; Dove, J; Dwyer, D A; Edwards, W R; Gill, R; Gonchar, M; Gong, G H; Gong, H; Grassi, M; Gu, W Q; Guo, L; Guo, X H; Guo, Y H; Guo, Z; Hackenburg, R W; Hans, S; He, M; Heeger, K M; Heng, Y K; Higuera, A; Hsiung, Y B; Hu, B Z; Hu, T; Huang, E C; Huang, H X; Huang, X T; Huang, Y B; Huber, P; Huo, W; Hussain, G; Jaffe, D E; Jen, K L; Ji, X P; Ji, X L; Jiao, J B; Johnson, R A; Jones, D; Kang, L; Kettell, S H; Khan, A; Kohn, S; Kramer, M; Kwan, K K; Kwok, M W; Langford, T J; Lau, K; Lebanowski, L; Lee, J; Lee, J H C; Lei, R T; Leitner, R; Leung, J K C; Li, C; Li, D J; Li, F; Li, G S; Li, Q J; Li, S; Li, S C; Li, W D; Li, X N; Li, X Q; Li, Y F; Li, Z B; Liang, H; Lin, C J; Lin, G L; Lin, S; Lin, S K; Lin, Y-C; Ling, J J; Link, J M; Littenberg, L; Littlejohn, B R; Liu, J L; Liu, J C; Loh, C W; Lu, C; Lu, H Q; Lu, J S; Luk, K B; Ma, X Y; Ma, X B; Ma, Y Q; Malyshkin, Y; Martinez Caicedo, D A; McDonald, K T; McKeown, R D; Mitchell, I; Nakajima, Y; Napolitano, J; Naumov, D; Naumova, E; Ngai, H Y; Ochoa-Ricoux, J P; Olshevskiy, A; Pan, H-R; Park, J; Patton, S; Pec, V; Peng, J C; Pinsky, L; Pun, C S J; Qi, F Z; Qi, M; Qian, X; Qiu, R M; Raper, N; Ren, J; Rosero, R; Roskovec, B; Ruan, X C; Steiner, H; Stoler, P; Sun, J L; Tang, W; Taychenachev, D; Treskov, K; Tsang, K V; Tull, C E; Viaux, N; Viren, B; Vorobel, V; Wang, C H; Wang, M; Wang, N Y; Wang, R G; Wang, W; Wang, X; Wang, Y F; Wang, Z; Wang, Z; Wang, Z M; Wei, H Y; Wen, L J; Whisnant, K; White, C G; Whitehead, L; Wise, T; Wong, H L H; Wong, S C F; Worcester, E; Wu, C-H; Wu, Q; Wu, W J; Xia, D M; Xia, J K; Xing, Z Z; Xu, J L; Xu, Y; Xue, T; Yang, C G; Yang, H; Yang, L; Yang, M S; Yang, M T; Yang, Y Z; Ye, M; Ye, Z; Yeh, M; Young, B L; Yu, Z Y; Zeng, S; Zhan, L; Zhang, C; Zhang, C C; Zhang, H H; Zhang, J W; Zhang, Q M; Zhang, R; Zhang, X T; Zhang, Y M; Zhang, Y X; Zhang, Y M; Zhang, Z J; Zhang, Z Y; Zhang, Z P; Zhao, J; Zhou, L; Zhuang, H L; Zou, J H

    2017-06-23

    The Daya Bay experiment has observed correlations between reactor core fuel evolution and changes in the reactor antineutrino flux and energy spectrum. Four antineutrino detectors in two experimental halls were used to identify 2.2 million inverse beta decays (IBDs) over 1230 days spanning multiple fuel cycles for each of six 2.9 GW_{th} reactor cores at the Daya Bay and Ling Ao nuclear power plants. Using detector data spanning effective ^{239}Pu fission fractions F_{239} from 0.25 to 0.35, Daya Bay measures an average IBD yield σ[over ¯]_{f} of (5.90±0.13)×10^{-43}  cm^{2}/fission and a fuel-dependent variation in the IBD yield, dσ_{f}/dF_{239}, of (-1.86±0.18)×10^{-43}  cm^{2}/fission. This observation rejects the hypothesis of a constant antineutrino flux as a function of the ^{239}Pu fission fraction at 10 standard deviations. The variation in IBD yield is found to be energy dependent, rejecting the hypothesis of a constant antineutrino energy spectrum at 5.1 standard deviations. While measurements of the evolution in the IBD spectrum show general agreement with predictions from recent reactor models, the measured evolution in total IBD yield disagrees with recent predictions at 3.1σ. This discrepancy indicates that an overall deficit in the measured flux with respect to predictions does not result from equal fractional deficits from the primary fission isotopes ^{235}U, ^{239}Pu, ^{238}U, and ^{241}Pu. Based on measured IBD yield variations, yields of (6.17±0.17) and (4.27±0.26)×10^{-43}  cm^{2}/fission have been determined for the two dominant fission parent isotopes ^{235}U and ^{239}Pu. A 7.8% discrepancy between the observed and predicted ^{235}U yields suggests that this isotope may be the primary contributor to the reactor antineutrino anomaly.

  7. Determination of Pu content in a Spent Fuel Assembly by Measuring Passive Total Neutron count rate and Multiplication with the Differential Die-Away Instrument

    Energy Technology Data Exchange (ETDEWEB)

    Henzl, Vladimir [Los Alamos National Laboratory; Croft, Stephen [Los Alamos National Laboratory; Swinhoe, Martyn T. [Los Alamos National Laboratory; Tobin, Stephen J. [Los Alamos National Laboratory

    2012-07-13

    Inspired by approach of Bignan and Martin-Didier (ESARDA 1991) we introduce novel (instrument independent) approach based on multiplication and passive neutron. Based on simulations of SFL-1 the accuracy of determination of {sup tot}Pu content with new approach is {approx}1.3-1.5%. Method applicable for DDA instrument, since it can measure both multiplication and passive neutron count rate. Comparison of pro's & con's of measuring/determining of {sup 239}Pu{sub eff} and {sup tot}Pu suggests a potential for enhanced diversion detection sensitivity.

  8. Introducing Nuclear Data Evaluations of Prompt Fission Neutron Spectra

    Energy Technology Data Exchange (ETDEWEB)

    Neudecker, Denise [Los Alamos National Lab. (LANL), Los Alamos, NM (United States)

    2015-06-17

    Nuclear data evaluations provide recommended data sets for nuclear data applications such as reactor physics, stockpile stewardship or nuclear medicine. The evaluated data are often based on information from multiple experimental data sets and nuclear theory using statistical methods. Therefore, they are collaborative efforts of evaluators, theoreticians, experimentalists, benchmark experts, statisticians and application area scientists. In this talk, an introductions is given to the field of nuclear data evaluation at the specific example of a recent evaluation of the outgoing neutron energy spectrum emitted promptly after fission from 239Pu and induced by neutrons from thermal to 30 MeV.

  9. Innovative Fission Measurements with a Time Projection Chamber

    Energy Technology Data Exchange (ETDEWEB)

    Heffner, M D; Barnes, P D; Klay, J L

    2005-11-16

    This study explores a pioneering idea to utilize a Time Projection Chamber (TPC) to measure fission cross sections and other fission quantities. The TPC is inherently capable of measuring fragments from fission events, decay alphas, and beam-material scatters. This document explores whether the TPC can improve the precision of the {sup 239}Pu(n,f) cross section and measure other new and significant fission quantities simultaneously. This work shows that the TPC can in fact deliver sub-1% cross section measurements and should provide breakthroughs in both the quality and quantity of information available from neutron-induced fission experiments.

  10. γ-ray self-absorption of cylindrical fissile material

    Institute of Scientific and Technical Information of China (English)

    HUANG Yong-Yi; CHENG Yi-Ying; TIAN Dong-Feng; LU Fu-Quan; YANG Fu-Jia

    2005-01-01

    The self-absorption of γ-ray emitted from cylindrical fissile materials, such as 235U and 239Pu, does not possess spherical symmetry. The analytical formulae of self-absorption for γ-ray throughout the cylinder have been obtained. The intensity of γ-ray is a function of γ-ray outgoing directions and cylindrical configurations, accordingly one can acquire the information about geometrical configuration of cylindrical fissile materials through multi-location measurements. Further more, the method is given in this article. The result can be applied to the fissile material safeguard, such as nuclear monitoring and verifying.

  11. Prompt neutron fission spectrum mean energies for the fissile nuclides and /sup 252/Cf

    Energy Technology Data Exchange (ETDEWEB)

    Holden, N.E.

    1985-01-01

    The international standard for a neutron spectrum is that produced from the spontaneous fission of /sup 252/Cf, while the thermal neutron induced fission neutron spectra for the four fissile nuclides, /sup 233/U, /sup 235/U, /sup 239/Pu, and /sup 241/Pu are of interest from the standpoint of nuclear reactors. The average neutron energies of these spectra are tabulated. The individual measurements are recorded with the neutron energy range measured, the method of detection as well as the average neutron energy for each author. Also tabulated are the measurements of the ratio of mean energies for pairs of fission neutron spectra. 75 refs., 9 tabs. (LEW)

  12. Radioactive inventories from the Kyshtym and Karachay accidents: estimates based on soil samples collected in the South Urals (1990-1995)

    DEFF Research Database (Denmark)

    Aarkrog, A.; Dahlgaard, H.; Nielsen, S.P.;

    1997-01-01

    and Western radioecologists. The present study is a joint Russian-Ukrainian-Danish effort to make an independent estimate of the inventories of Sr-90, Cs-137 and Pu-239,Pu-240 from two major contamination events in the South Urals, namely, the Kyshtym accident in 1957 and the Karachay wind dispersion in 1967....... The calculations are based upon deposition measurements of the radionuclides carried out on soil samples assuming that the depositions decreased exponentially with distance from the two sources. The inventory estimates are compared with the available Russian information on the two accidents. (C) 1997 Elsevier...

  13. Development of a Grid Ionization Chamber for a Dram of α Ray

    Directory of Open Access Journals (Sweden)

    YANG Lu;WANG Qiang;ZHENG Yu-lai;WANG Guo-bao

    2016-11-01

    Full Text Available This article introduced the parallel grid ionization chamber that used to measure the α radioactivity, which had a independent vacuum system. The system was composed of main body of the chamber, gas-filled and electronics system. Energy resolution was 26 keV for 239Pu, background was 10 counts for one hour from 4 MeV to 6 MeV energy range, the stability of 24 hours was less than 0.5% . The chamber can measure the energy of nuclide and analyze the energy spectrum structure to identify nuclear.

  14. Radionuclides and heavy metals in rainbow trout from Tsichomo, Nana Ka, Wen Povi, and Pin De Lakes in Santa Clara Canyon

    Energy Technology Data Exchange (ETDEWEB)

    Fresquez, P.R.; Armstrong, D.R.; Naranjo, L. Jr.

    1998-04-01

    Radionuclide ({sup 3}H, {sup 90}Sr, {sup 137}Cs, {sup 238}Pu, {sup 239}Pu, and total uranium) and heavy metal (Ag, As, Ba, Be, Cd, Cr, Hg, Ni, Pb, Sb, Se, and TI) concentrations were determined in rainbow trout collected from Tsichomo, Nana Ka, Wen Povi, and Pin De lakes in Santa Clara Canyon in 1997. Most radionuclide and heavy metal concentrations in fish collected from these four lakes were within or just above upper limit background concentrations (Abiquiu reservoir), and as a group were statistically (p < 0.05) similar in most parameters to background.

  15. Evolution of the Reactor Antineutrino Flux and Spectrum at Daya Bay

    Science.gov (United States)

    An, F. P.; Balantekin, A. B.; Band, H. R.; Bishai, M.; Blyth, S.; Cao, D.; Cao, G. F.; Cao, J.; Chan, Y. L.; Chang, J. F.; Chang, Y.; Chen, H. S.; Chen, Q. Y.; Chen, S. M.; Chen, Y. X.; Chen, Y.; Cheng, J.; Cheng, Z. K.; Cherwinka, J. J.; Chu, M. C.; Chukanov, A.; Cummings, J. P.; Ding, Y. Y.; Diwan, M. V.; Dolgareva, M.; Dove, J.; Dwyer, D. A.; Edwards, W. R.; Gill, R.; Gonchar, M.; Gong, G. H.; Gong, H.; Grassi, M.; Gu, W. Q.; Guo, L.; Guo, X. H.; Guo, Y. H.; Guo, Z.; Hackenburg, R. W.; Hans, S.; He, M.; Heeger, K. M.; Heng, Y. K.; Higuera, A.; Hsiung, Y. B.; Hu, B. Z.; Hu, T.; Huang, E. C.; Huang, H. X.; Huang, X. T.; Huang, Y. B.; Huber, P.; Huo, W.; Hussain, G.; Jaffe, D. E.; Jen, K. L.; Ji, X. P.; Ji, X. L.; Jiao, J. B.; Johnson, R. A.; Jones, D.; Kang, L.; Kettell, S. H.; Khan, A.; Kohn, S.; Kramer, M.; Kwan, K. K.; Kwok, M. W.; Langford, T. J.; Lau, K.; Lebanowski, L.; Lee, J.; Lee, J. H. C.; Lei, R. T.; Leitner, R.; Leung, J. K. C.; Li, C.; Li, D. J.; Li, F.; Li, G. S.; Li, Q. J.; Li, S.; Li, S. C.; Li, W. D.; Li, X. N.; Li, X. Q.; Li, Y. F.; Li, Z. B.; Liang, H.; Lin, C. J.; Lin, G. L.; Lin, S.; Lin, S. K.; Lin, Y.-C.; Ling, J. J.; Link, J. M.; Littenberg, L.; Littlejohn, B. R.; Liu, J. L.; Liu, J. C.; Loh, C. W.; Lu, C.; Lu, H. Q.; Lu, J. S.; Luk, K. B.; Ma, X. Y.; Ma, X. B.; Ma, Y. Q.; Malyshkin, Y.; Martinez Caicedo, D. A.; McDonald, K. T.; McKeown, R. D.; Mitchell, I.; Nakajima, Y.; Napolitano, J.; Naumov, D.; Naumova, E.; Ngai, H. Y.; Ochoa-Ricoux, J. P.; Olshevskiy, A.; Pan, H.-R.; Park, J.; Patton, S.; Pec, V.; Peng, J. C.; Pinsky, L.; Pun, C. S. J.; Qi, F. Z.; Qi, M.; Qian, X.; Qiu, R. M.; Raper, N.; Ren, J.; Rosero, R.; Roskovec, B.; Ruan, X. C.; Steiner, H.; Stoler, P.; Sun, J. L.; Tang, W.; Taychenachev, D.; Treskov, K.; Tsang, K. V.; Tull, C. E.; Viaux, N.; Viren, B.; Vorobel, V.; Wang, C. H.; Wang, M.; Wang, N. Y.; Wang, R. G.; Wang, W.; Wang, X.; Wang, Y. F.; Wang, Z.; Wang, Z.; Wang, Z. M.; Wei, H. Y.; Wen, L. J.; Whisnant, K.; White, C. G.; Whitehead, L.; Wise, T.; Wong, H. L. H.; Wong, S. C. F.; Worcester, E.; Wu, C.-H.; Wu, Q.; Wu, W. J.; Xia, D. M.; Xia, J. K.; Xing, Z. Z.; Xu, J. L.; Xu, Y.; Xue, T.; Yang, C. G.; Yang, H.; Yang, L.; Yang, M. S.; Yang, M. T.; Yang, Y. Z.; Ye, M.; Ye, Z.; Yeh, M.; Young, B. L.; Yu, Z. Y.; Zeng, S.; Zhan, L.; Zhang, C.; Zhang, C. C.; Zhang, H. H.; Zhang, J. W.; Zhang, Q. M.; Zhang, R.; Zhang, X. T.; Zhang, Y. M.; Zhang, Y. X.; Zhang, Y. M.; Zhang, Z. J.; Zhang, Z. Y.; Zhang, Z. P.; Zhao, J.; Zhou, L.; Zhuang, H. L.; Zou, J. H.; Daya Bay Collaboration

    2017-06-01

    The Daya Bay experiment has observed correlations between reactor core fuel evolution and changes in the reactor antineutrino flux and energy spectrum. Four antineutrino detectors in two experimental halls were used to identify 2.2 million inverse beta decays (IBDs) over 1230 days spanning multiple fuel cycles for each of six 2.9 G Wth reactor cores at the Daya Bay and Ling Ao nuclear power plants. Using detector data spanning effective 239Pu fission fractions F239 from 0.25 to 0.35, Daya Bay measures an average IBD yield σ¯f of (5.90 ±0.13 )×10-43 cm2/fission and a fuel-dependent variation in the IBD yield, d σf/d F239, of (-1.86 ±0.18 )×10-43 cm2/fission . This observation rejects the hypothesis of a constant antineutrino flux as a function of the 239Pu fission fraction at 10 standard deviations. The variation in IBD yield is found to be energy dependent, rejecting the hypothesis of a constant antineutrino energy spectrum at 5.1 standard deviations. While measurements of the evolution in the IBD spectrum show general agreement with predictions from recent reactor models, the measured evolution in total IBD yield disagrees with recent predictions at 3.1 σ . This discrepancy indicates that an overall deficit in the measured flux with respect to predictions does not result from equal fractional deficits from the primary fission isotopes 235U, 239Pu, 238U, and 241Pu. Based on measured IBD yield variations, yields of (6.17 ±0.17 ) and (4.27 ±0.26 )×10-43 cm2 /fission have been determined for the two dominant fission parent isotopes 235U and 239Pu. A 7.8% discrepancy between the observed and predicted 235U yields suggests that this isotope may be the primary contributor to the reactor antineutrino anomaly.

  16. IN-SITU ASSAY OF TRANSURANIC RADIONUCLIDES IN THE VADOSE ZONE USING HIGH-RESOLUTION SPECTRAL GAMMA LOGGING - A HANFORD CASE STUDY

    Energy Technology Data Exchange (ETDEWEB)

    ROHAY VJ; HENWOOD P; MCCAIN R

    2009-11-30

    High-resolution spectral gamma logging in steel-cased boreholes is used to detect and quantify transuranic radionuclides in the subsurface. Pu-239, Pu-241, Am-241, and Np-237 are identified based on characteristic decay gammas. Typical minimum detectable levels are on the order of 20 to 40 nCi/g. In intervals of high transuranic concentrations, gamma rays from other sources may complicate analysis and interpretation. Gamma rays detected in the borehole may originate from three sources: decay of the parent transuranic radionuclide or a daughter; alpha interactions; and interactions with neutrons resulting from either spontaneous fission or alpha particle interactions.

  17. Interlaboratory reaction rate program. 12th progress report, November 1976-October 1979

    Energy Technology Data Exchange (ETDEWEB)

    Lippincott, E.P.; McElroy, W.N.; Preston, C.C. (comps.)

    1980-09-01

    The Interlaboratory Reaction Rate UILRR) program is establishing the capability to accurately measure neutron-induced reactions and reaction rates for reactor fuels and materials development programs. The goal for the principal fission reactions, /sup 235/U, /sup 238/U and /sup 239/Pu, is an accuracy to within +- 5% at the 95% confidence level. Accurate measurement of other fission and nonfission reactions is also required, but to a lesser accuracy, between +- 5% and 10% at the 95% confidence level. A secondary program objective is improvement in knowledge of the nuclear parameters involved in the standarization of fuels and materials dosimetry measurements of neutron flux, spectra, fluence and burnup.

  18. Verification measurements of the IRMM-1027 and the IAEA large-sized dried (LSD) spikes.

    Science.gov (United States)

    Jakopič, R; Aregbe, Y; Richter, S; Zuleger, E; Mialle, S; Balsley, S D; Repinc, U; Hiess, J

    2017-01-01

    In the frame of the accountancy measurements of the fissile materials, reliable determinations of the plutonium and uranium content in spent nuclear fuel are required to comply with international safeguards agreements. Large-sized dried (LSD) spikes of enriched (235)U and (239)Pu for isotope dilution mass spectrometry (IDMS) analysis are routinely applied in reprocessing plants for this purpose. A correct characterisation of these elements is a pre-requirement for achieving high accuracy in IDMS analyses. This paper will present the results of external verification measurements of such LSD spikes performed by the European Commission and the International Atomic Energy Agency.

  19. DETERMINATION OF 237NP AND PU ISOTOPES IN LARGE SOIL SAMPLES BY INDUCTIVELY COUPLED PLASMA MASS SPECTROMETRY

    Energy Technology Data Exchange (ETDEWEB)

    Maxwell, S.

    2010-07-26

    A new method for the determination of {sup 237}Np and Pu isotopes in large soil samples has been developed that provides enhanced uranium removal to facilitate assay by inductively coupled plasma mass spectrometry (ICP-MS). This method allows rapid preconcentration and separation of plutonium and neptunium in large soil samples for the measurement of {sup 237}Np and Pu isotopes by ICP-MS. {sup 238}U can interfere with {sup 239}Pu measurement by ICP-MS as {sup 238}UH{sup +} mass overlap and {sup 237}Np via {sup 238}U peak tailing. The method provides enhanced removal of uranium by separating Pu and Np initially on TEVA Resin, then transferring Pu to DGA resin for additional purification. The decontamination factor for removal of uranium from plutonium for this method is greater than 1 x 10{sup 6}. Alpha spectrometry can also be applied so that the shorter-lived {sup 238}Pu isotope can be measured successfully. {sup 239}Pu, {sup 242}Pu and {sup 237}Np were measured by ICP-MS, while {sup 236}Pu and {sup 238}Pu were measured by alpha spectrometry.

  20. Analytical method for the determination of Np and Pu in sea water by AMS with respect to the Fukushima accident

    Energy Technology Data Exchange (ETDEWEB)

    Hain, K., E-mail: karin.hain@mytum.de [Physics Department, Technische Universität München, James-Franck-Str.1, 85748 Garching (Germany); Faestermann, T.; Famulok, N.; Fimiani, L.; Gómez-Guzmán, J.M.; Korschinek, G. [Physics Department, Technische Universität München, James-Franck-Str.1, 85748 Garching (Germany); Kortmann, F.; Lierse von Gostomski, Ch. [Radiochemie München, Technische Universität München, Walther-Meißner-Str.3, 85748 Garching (Germany); Ludwig, P. [Physics Department, Technische Universität München, James-Franck-Str.1, 85748 Garching (Germany); Shinonaga, T. [Helmholtz Zentrum München, German Research Center for Environmental Health, Institute of Radiation Protection, Ingolstädter Landstrasse 1, 855764 Neuherberg (Germany)

    2015-10-15

    A chemical separation procedure for plutonium (Pu) and neptunium (Np) was developed using extraction chromatography, mass spectrometry and radiometric analysis to determine their concentrations and isotopic ratios in sea water. {sup 241}Am, which causes isobaric background to {sup 241}Pu in mass spectrometric measurements, was successfully separated from the Pu fraction by this method. Water samples which were spiked with {sup 242}Pu and {sup 237}Np or {sup 239}Np, respectively, were used for chemical yield determination. The chemical yields of Pu and Np, which were determined by alpha and gamma spectrometry at the Radiochemie München (RCM), of more than 85% were obtained. The developed method was applied to analyze the concentration of Pu and Np in the certified reference material, IAEA-443, by Accelerator Mass Spectrometry (AMS) at the Maier–Leibnitz-Laboratory (MLL) to check the applicability of the method to sea water samples. The concentrations of {sup 240}Pu, {sup 241}Pu and {sup 237}Np obtained in this study are in agreement with the certified and literature values within the uncertainties. Due to strong isotopic interference of {sup 239}Pu with {sup 238}U, it was not possible to analyze the concentration of {sup 239}Pu. Some modifications of the chemical separation method to suppress the uranium (U) fraction are under consideration. This method can be used for the analysis of Pu and Np in Pacific Ocean water samples collected after the Fukushima accident.

  1. Classification of hot particles from the Chernobyl accident and nuclear weapons detonations by non-destructive methods.

    Science.gov (United States)

    Zheltonozhsky, V; Mück, K; Bondarkov, M

    2001-01-01

    Both after the Chernobyl accident and nuclear weapon detonations, agglomerates of radioactive material, so-called hot particles, were released or formed which show a behaviour in the environment quite different from the activity released in gaseous or aerosol form. The differences in their characteristic properties, in the radionuclide composition and the uranium and actinide contents are described in detail for these particles. While nuclear bomb hot particles (both from fission and fusion bombs) incorporate well detectable trace amounts of 60Co and 152Eu, these radionuclides are absent in Chernobyl hot particles. In contrast, Chernobyl hot particles contain 125Sb and 144Ce which are absent in atomic bomb HPs. Obvious differences are also observable between fusion and fission bombs' hot particles (significant differences in 152Eu/l55Eu, 154Eu/155Eu and 238Pu/239Pu ratios) which facilitate the identification of HPs of unknown provensence. The ratio of 239Pu/240Pu in Chernobyl hot particles could be determined by a non-destructive method at 1:1.5. A non-destructive method to determine the content of non-radioactive elements by Kalpha-emission measurements was developed by which inactive Zr, Nb, Fe and Ni could be verified in the particles.

  2. Advanced disposal systems for transuranic waste: Preliminary disposal criteria for Plutonium-239 at Hanford

    Energy Technology Data Exchange (ETDEWEB)

    Kennedy, W.E.; Napier, B.A.; Soldat, J.K.

    1983-01-01

    An evaluation of the feasibility and potential application of advanced disposal systems is being conducted for defense transuranic (TRU) wastes at the Hanford site. The advanced waste disposal options include those developed to provide ''greater confinement'' than provided by shallow-land burial. An example systems analysis is discussed with assumed performance objectives and various Hanford-specific disposal conditions, waste forms, site characteristics, and engineered barriers. Preliminary waste disposal criteria for /sup 239/Pu are determined by applying the allowable residual contamination level (ARCL) method. This method is based on compliance with a radiation dose rate limit through a site specific analysis of the potential for radiation exposure to individuals. A 10,000-year environmental performance period is assumed, and the dose rate limit for human intrusion is assumed to be 500 mrem/yr to any exposed individual. Preliminary waste disposal criteria derived by this method for /sup 239/Pu in soils at the Hanford Site are 0.5 nCi/g in soils between the surface and a depth of 1 m, 2200 nCi/g of soil at a depth of 5 m, and 10,000 nCi/g of soil at depths 10 m and below. These waste disposal criteria are based on exposure scenarios that reflect the dependence of exposure versus burial depth.

  3. CMR Shuffler System: Passive Mode Calibration and Certification Report

    Energy Technology Data Exchange (ETDEWEB)

    Frame, Katherine C. [Los Alamos National Laboratory; Gomez, Cipriano D. [Retired CMR-OPS: OPERATIONS; Salazar, William R. [Los Alamos National Laboratory; Mayo, Douglas R. [Los Alamos National Laboratory; Vigil, Georgiana M. [Los Alamos National Laboratory; Crooks, William J. [Los Alamos National Laboratory; Stange, Sy [Los Alamos National Laboratory

    2012-07-20

    Los Alamos National Laboratory has a number of spherical confinement vessels (CVs) remaining from tests involving nuclear materials. These vessels have an inner diameter of 6 feet with 1 to 2 inch thick steel walls. The goal of the Confinement Vessel Disposition (CVD) project is to remove debris and reduce contamination inside the vessels. As debris is removed from the vessels, material will be placed in waste drums. Far-field gamma ray assay will be used to determine when a drum is nearing a {sup 239}Pu equivalent mass of less than 200 g. The drum will then be assayed using a waste drum shuffler operated in passive mode using a neutron coincidence counting method for accountability. This report focuses on the testing and calibration of the CMR waste drum shuffler in passive mode operation. Initial testing was performed to confirm previously accepted measurement parameters. The system was then calibrated using a set of weapons grade Pu (WGPu, {sup 239}Pu > 93%) oxide standards placed inside a 55 gallon drum. The calibration data ranges from Pu mass of 0.5 g to 188.9 g. The CMR waste drum shuffler has been tested and calibrated in passive mode in preparation for safeguards accountability measurements of waste drums containing material removed from CVs for the CVD project.

  4. Uranium-series constraints on radionuclide transport and groundwater flow at the Nopal I uranium deposit, Sierra Pena Blanca, Mexico.

    Science.gov (United States)

    Goldstein, Steven J; Abdel-Fattah, Amr I; Murrell, Michael T; Dobson, Patrick F; Norman, Deborah E; Amato, Ronald S; Nunn, Andrew J

    2010-03-01

    Uranium-series data for groundwater samples from the Nopal I uranium ore deposit were obtained to place constraints on radionuclide transport and hydrologic processes for a nuclear waste repository located in fractured, unsaturated volcanic tuff. Decreasing uranium concentrations for wells drilled in 2003 are consistent with a simple physical mixing model that indicates that groundwater velocities are low ( approximately 10 m/y). Uranium isotopic constraints, well productivities, and radon systematics also suggest limited groundwater mixing and slow flow in the saturated zone. Uranium isotopic systematics for seepage water collected in the mine adit show a spatial dependence which is consistent with longer water-rock interaction times and higher uranium dissolution inputs at the front adit where the deposit is located. Uranium-series disequilibria measurements for mostly unsaturated zone samples indicate that (230)Th/(238)U activity ratios range from 0.005 to 0.48 and (226)Ra/(238)U activity ratios range from 0.006 to 113. (239)Pu/(238)U mass ratios for the saturated zone are 1000 times lower than the U mobility. Saturated zone mobility decreases in the order (238)U approximately (226)Ra > (230)Th approximately (239)Pu. Radium and thorium appear to have higher mobility in the unsaturated zone based on U-series data from fractures and seepage water near the deposit.

  5. Uranium-series constraints on radionuclide transport and groundwater flow at the Nopal I uranium deposit, Sierra Pena Blanca, Mexico

    Energy Technology Data Exchange (ETDEWEB)

    Goldstein, S.J.; Abdel-Fattah, A.I.; Murrell, M.T.; Dobson, P.F.; Norman, D.E.; Amato, R.S.; Nunn, A. J.

    2009-10-01

    Uranium-series data for groundwater samples from the Nopal I uranium ore deposit were obtained to place constraints on radionuclide transport and hydrologic processes for a nuclear waste repository located in fractured, unsaturated volcanic tuff. Decreasing uranium concentrations for wells drilled in 2003 are consistent with a simple physical mixing model that indicates that groundwater velocities are low ({approx}10 m/y). Uranium isotopic constraints, well productivities, and radon systematics also suggest limited groundwater mixing and slow flow in the saturated zone. Uranium isotopic systematics for seepage water collected in the mine adit show a spatial dependence which is consistent with longer water-rock interaction times and higher uranium dissolution inputs at the front adit where the deposit is located. Uranium-series disequilibria measurements for mostly unsaturated zone samples indicate that {sup 230}Th/{sup 238}U activity ratios range from 0.005-0.48 and {sup 226}Ra/{sup 238}U activity ratios range from 0.006-113. {sup 239}Pu/{sup 238}U mass ratios for the saturated zone are <2 x 10{sup -14}, and Pu mobility in the saturated zone is >1000 times lower than the U mobility. Saturated zone mobility decreases in the order {sup 238}U{approx}{sup 226}Ra > {sup 230}Th{approx}{sup 239}Pu. Radium and thorium appear to have higher mobility in the unsaturated zone based on U-series data from fractures and seepage water near the deposit.

  6. Radioecological studies at the National Center of Accelerators based on the use of the accelerator mass spectrometry; Estudios radioecologicos en el Centro Nacional de Aceleradores basados en el uso de la Espectrometria de Masas con Acelerador (AMS)

    Energy Technology Data Exchange (ETDEWEB)

    Chamizo, E.; Lopez-Gutierrez, J. M.; Gomez-Guzman, J. M.; Santos, F. J.; Garcia-Leon, M.; Garcia-Tenorio, R.

    2013-03-01

    Since mid-2006 a compact Accelerator Mass Spectrometry (AMS) of 1 MV, Tandetron type, named SARA (Spanish Accelerator for Radionuclide Analysis) is installed at the National Accelerator Centre in Seville. After an initial period, to set-up the equipment and to study its capability to detect the long-lived radionuclides {sup 1}4C, {sup 1}0B, {sup 2}6Al, {sup 1}29I and plutonium isotopes ({sup 2}39Pu and {sup 2}40Pu) compared to other techniques of mass spectrometry (MS), numerous research lines in fields as diverse as archaeology, geology, palaeontology, oceanography, internal dosimetry, astrophysics and characterization of radioactive waste, among others, have been opened. In particular, since 2008 numerous contributions in the field of Radioecology have been done, based in the measurements of {sup 1}29I and Pu isotopes ({sup 2}39Pu and {sup 2}40Pu). In this article, some of these radioecological researches are summarized and presented, with special emphasis on showing that its accomplishment requires the application of the AMS technique, to be able to achieve sensitivities and detection limits which are impossible to reach when radiometric and mass spectrometry conventional techniques are applied. (Author) 13 refs.

  7. Neutron scattering studies in the actinide region. Progress report, August 1, 1991--July 31, 1994

    Energy Technology Data Exchange (ETDEWEB)

    Kegel, G.H.R.; Egan, J.J.

    1994-09-01

    During the period August 1, 1991 to July 31, 1994 the authors report progress on the following: (a) prompt fission neutron energy spectra for {sup 235}U and {sup 239}Pu; (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 {sup 197}Au; (f) elastic and inelastic neutron scattering studies in {sup 239}Pu; (g) neutron induced defects in silicon dioxide MOS structures; (h) response of a {sup 235}U 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.

  8. ORNL Resolved Resonance Covariance Generation for ENDF/B-VII.1

    Science.gov (United States)

    Leal, L.; Guber, K.; Wiarda, D.; Arbanas, G.; Derrien, H.; Sayer, R.; Larson, N.; Dunn, M.

    2012-12-01

    Resonance-parameter covariance matrix (RPCM) evaluations in the resolved resonance regionwere done at the Oak Ridge National Laboratory (ORNL) for the chromium isotopes, titanium isotopes, 19F, 58Ni, 60Ni, 35Cl, 37Cl, 39K, 41K, 55Mn, 233U, 235U, 238U, and 239Pu using the computer code SAMMY. The retroactive approach of the code SAMMY was used to generate the RPCMs for 233U. For 235U, the approach used for covariance generation was similar to the retroactive approach with the distinction that real experimental data were used as opposed to data generated from the resonance parameters. RPCMs for 238U and 239Pu were generated together with the resonance parameter evaluations. The RPCMs were then converted in the ENDF format using the FILE32 representation. Alternatively, for computer storage reasons, the FILE32 was converted in the FILE33 cross section covariance matrix (CSCM). Both representations were processed using the computer code PUFF-IV. This paper describes the procedures used to generate the RPCM and CSCM in the resonance region for ENDF/B-VII.1. The impact of data uncertainty in nuclear reactor benchmark calculations is also presented.

  9. A new code for modelling the near field diffusion releases from the final disposal of nuclear waste

    Science.gov (United States)

    Vopálka, D.; Vokál, A.

    2003-01-01

    The canisters with spent nuclear fuel produced during the operation of WWER reactors at the Czech power plants are planned, like in other countries, to be disposed of in an underground repository. Canisters will be surrounded by compacted bentonite that will retard the migration of safety-relevant radionuclides into the host rock. A new code that enables the modelling of the critical radionuclides transport from the canister through the bentonite layer in the cylindrical geometry was developed. The code enables to solve the diffusion equation for various types of initial and boundary conditions by means of the finite difference method and to take into account the non-linear shape of the sorption isotherm. A comparison of the code reported here with code PAGODA, which is based on analytical solution of the transport equation, was made for the actinide chain 4N+3 that includes 239Pu. A simple parametric study of the releases of 239Pu, 129I, and 14C into geosphere is discussed.

  10. Isotopic evidence for trapped fissiogenic REE and nucleogenic Pu in apatite and Pb evolution at the Oklo natural reactor

    Science.gov (United States)

    Horie, Kenji; Hidaka, Hiroshi; Gauthier-Lafaye, François

    2004-01-01

    A part of the boundary layer of reactor zone 10 at the Oklo natural reactor shows a unique petrologic texture, which contains high-grade uraninite and massive apatite concretions. In order to study distribution behavior of fission products around the boundary between the reactor zone and the wall rock and to clarify the relation of migration mechanisms of fission products with geochemical factors, in-situ isotopic analyses of Nd, Sm, Gd, Pb and U in uraninite and apatite from the sample were performed by Sensitive High Resolution Ion Microprobe (SHRIMP). Sm and Gd isotopic ratios of uraninite and apatite show evidence of neutron irradiation with fluence between 4.4-6.8×10 19 n/cm 2. Judging from the isotopic anomalies of Nd and U, the apatite coexisting with the uraninite plays an important role in trapping fissiogenic LREE and nucleogenic 239Pu into the structure. Systematic Pb isotopic data from apatite, uraninite, galena and minium suggest the following chronological interpretations. The apatite formed 1.92±0.01 Ga ago and trapped fissiogenic light REE and nucleogenic 239Pu that migrated from the reactor during the criticality. The uraninite around the boundary between reactor and sandstone dissolved once 1.1˜1.2 Ga ago. Galena grains were formed by U-Pb mobilization in association with the intrusion of dolerite dyke 0.45˜0.83 Ga ago. Minium was derived from recent dissolution of galena under locally oxidizing conditions.

  11. Results of The Excreta Bioassay Quality Control Program For April 1, 2010 Through March 31, 2011

    Energy Technology Data Exchange (ETDEWEB)

    Antonio, Cheryl L.

    2012-07-19

    A total of 76 urine samples and 10 spiked fecal samples were submitted during the report period (April 1, 2010 through March 31, 2011) to GEL Laboratories, LLC in South Carolina by the Hanford Internal Dosimetry Program (IDP) to check the accuracy, precision, and detection levels of their analyses. Urine analyses for 14C, Sr, for 238Pu, 239Pu, 241Am, 243Am, 235U, 238U, 238U-mass and fecal analyses for 241Am, 238Pu and 239Pu were tested this year. The number of QC urine samples submitted during the report period represented 1.1% of the total samples submitted. In addition to the samples provided by IDP, GEL was also required to conduct their own QC program, and submit the results of analyses to IDP. About 31% of the analyses processed by GEL during the first year of contract 112512 were quality control samples. GEL tested the performance of 23 radioisotopes, all of which met or exceeded the specifications in the Statement of Work within statistical uncertainty except the slightly elevated relative bias for 243,244Cm (Table 4).

  12. Vertical distributions of plutonium isotopes in marine sediment cores off the Fukushima coast after the Fukushima Dai-ichi Nuclear Power Plant accident

    Directory of Open Access Journals (Sweden)

    W. T. Bu

    2013-04-01

    Full Text Available The Fukushima Dai-ichi Nuclear Power Plant (FDNPP accident led to the release of large amounts of radionuclides into the atmosphere as well as direct discharges into the sea. In contrast to the intensive studies on the distribution of the released high volatility fission products, such as 131I, 134Cs and 137Cs, similar studies of the actinides, especially the Pu isotopes, are limited. To obtain the vertical distribution of Pu isotopes in marine sediments and to better assess the possible contamination of Pu from the FDNPP accident in the marine environment, we determined the activities of 239+240Pu and 241Pu as well as the atom ratios of 240Pu/239Pu and 241Pu/239Pu in sediment core samples collected in the western North Pacific off Fukushima from July 2011 to July 2012. We also measured surface sediment samples collected from seven Japanese estuaries before the FNDPP accident to establish the comprehensive background baseline data. The observed results of both the Pu activities and the Pu atom ratios for the sediments in the western North Pacific were comparable to the baseline data, suggesting that the FDNPP accident did not cause detectable Pu contamination to the studied regions prior to the sampling time. The Pu isotopes in the western North Pacific 30 km off the Fukushima coast originated from global fallout and Pacific Proving Ground close-in fallout.

  13. Development of self-interrogation neutron resonance densitometry (SINRD) to measure U-235 and Pu-239 content in a PWR spent fuel assembly

    Energy Technology Data Exchange (ETDEWEB)

    Lafleur, Adrienne M [Los Alamos National Laboratory; Charlton, William S [Los Alamos National Laboratory; Menlove, Howard O [Los Alamos National Laboratory; Swinhoe, Martyn T [Los Alamos National Laboratory

    2009-01-01

    The use of Self-Interrogation Neutron Resonance Densitometry (SINRD) to measure the {sup 235}U and {sup 239}Pu content in a PWR spent fuel assembly was investigated via Monte Carlo N-Particle eXtended transport code (MCNPX) simulations. The sensitivity of SINRD is based on using the same fissile materials in the fission chambers as are present in the fuel because the effect of resonance absorption lines in the transmitted flux is amplified by the corresponding (n, f) reaction peaks in fission chamber. These simulations utilize the {sup 244}Cm spontaneous fission neutrons to self-interrogate the fuel pins. The amount of resonance absorption of these neutrons in the fuel can be measured using {sup 235}U and {sup 239}Pu fission chambers placed adjacent to the assembly. We used ratios of different fission chambers to reduce the sensitivity of the measurements to extraneous material present in fuel. The development of SINRD to measure the fissile content in spent fuel is of great importance to the improvement of nuclear safeguards and material accountability. Future work includes the use of this technique to measure the fissile content in FBR spent fuel and heavy metal product from reprocessing methods.

  14. Propagation of Nuclear Data Uncertainties for ELECTRA Burn-up Calculations

    Science.gov (United States)

    Sjöstrand, H.; Alhassan, E.; Duan, J.; Gustavsson, C.; Koning, A. J.; Pomp, S.; Rochman, D.; Österlund, M.

    2014-04-01

    The European Lead-Cooled Training Reactor (ELECTRA) has been proposed as a training reactor for fast systems within the Swedish nuclear program. It is a low-power fast reactor cooled by pure liquid lead. In this work, we propagate the uncertainties in 239Pu transport data to uncertainties in the fuel inventory of ELECTRA during the reactor lifetime using the Total Monte Carlo approach (TMC). Within the TENDL project, nuclear models input parameters were randomized within their uncertainties and 740 239Pu nuclear data libraries were generated. These libraries are used as inputs to reactor codes, in our case SERPENT, to perform uncertainty analysis of nuclear reactor inventory during burn-up. The uncertainty in the inventory determines uncertainties in: the long-term radio-toxicity, the decay heat, the evolution of reactivity parameters, gas pressure and volatile fission product content. In this work, a methodology called fast TMC is utilized, which reduces the overall calculation time. The uncertainty of some minor actinides were observed to be rather large and therefore their impact on multiple recycling should be investigated further. It was also found that, criticality benchmarks can be used to reduce inventory uncertainties due to nuclear data. Further studies are needed to include fission yield uncertainties, more isotopes, and a larger set of benchmarks.

  15. Combining Total Monte Carlo and Benchmarks for Nuclear Data Uncertainty Propagation on a Lead Fast Reactor's Safety Parameters

    Science.gov (United States)

    Alhassan, E.; Sjöstrand, H.; Duan, J.; Gustavsson, C.; Koning, A. J.; Pomp, S.; Rochman, D.; Österlund, M.

    2014-04-01

    Analyses are carried out to assess the impact of nuclear data uncertainties on keff for the European Lead Cooled Training Reactor (ELECTRA) using the Total Monte Carlo method. A large number of 239Pu random ENDF-formatted libraries generated using the TALYS based system were processed into ACE format with NJOY-99.336 code and used as input into the Serpent Monte Carlo neutron transport code to obtain distribution in keff. The mean of the keff distribution obtained was compared with the major nuclear data libraries, JEFF-3.1.1, ENDF/B-VII.1 and JENDL-4.0. A method is proposed for the selection of benchmarks for specific applications using the Total Monte Carlo approach. Finally, an accept/reject criterion was investigated based on χ2 values obtained using the 239Pu Jezebel criticality benchmark. It was observed that nuclear data uncertainties in keff were reduced considerably from 748 to 443 pcm by applying a more rigid acceptance criteria for accepting random files.

  16. Uncertainties in fission-product decay-heat calculations

    Energy Technology Data Exchange (ETDEWEB)

    Oyamatsu, K.; Ohta, H.; Miyazono, T.; Tasaka, K. [Nagoya Univ. (Japan)

    1997-03-01

    The present precision of the aggregate decay heat calculations is studied quantitatively for 50 fissioning systems. In this evaluation, nuclear data and their uncertainty data are taken from ENDF/B-VI nuclear data library and those which are not available in this library are supplemented by a theoretical consideration. An approximate method is proposed to simplify the evaluation of the uncertainties in the aggregate decay heat calculations so that we can point out easily nuclei which cause large uncertainties in the calculated decay heat values. In this paper, we attempt to clarify the justification of the approximation which was not very clear at the early stage of the study. We find that the aggregate decay heat uncertainties for minor actinides such as Am and Cm isotopes are 3-5 times as large as those for {sup 235}U and {sup 239}Pu. The recommended values by Atomic Energy Society of Japan (AESJ) were given for 3 major fissioning systems, {sup 235}U(t), {sup 239}Pu(t) and {sup 238}U(f). The present results are consistent with the AESJ values for these systems although the two evaluations used different nuclear data libraries and approximations. Therefore, the present results can also be considered to supplement the uncertainty values for the remaining 17 fissioning systems in JNDC2, which were not treated in the AESJ evaluation. Furthermore, we attempt to list nuclear data which cause large uncertainties in decay heat calculations for the future revision of decay and yield data libraries. (author)

  17. The LANL/LLNL Prompt Fission Neutron Spectrum Program at LANSCE and Approach to Uncertainties

    Energy Technology Data Exchange (ETDEWEB)

    Haight, R.C., E-mail: haight@lanl.gov [Los Alamos National Laboratory, Los Alamos, NM 87545,USA (United States); Wu, C.Y. [Lawrence Livermore National Laboratory, Livermore, CA 94551 (United States); Lee, H.Y.; Taddeucci, T.N.; Perdue, B.A.; O' Donnell, J.M.; Fotiades, N.; Devlin, M.; Ullmann, J.L.; Bredeweg, T.A.; Jandel, M.; Nelson, R.O.; Wender, S.A.; Neudecker, D.; Rising, M.E.; Mosby, S.; Sjue, S.; White, M.C. [Los Alamos National Laboratory, Los Alamos, NM 87545,USA (United States); Bucher, B.; Henderson, R. [Lawrence Livermore National Laboratory, Livermore, CA 94551 (United States)

    2015-01-15

    New data on the prompt fission neutron spectra (PFNS) from neutron-induced fission with higher accuracies are needed to resolve discrepancies in the literature and to address gaps in the experimental data. The Chi-Nu project, conducted jointly by LANL and LLNL, aims to measure the shape of the PFNS for fission of {sup 239}Pu induced by neutrons from 0.5 to 20 MeV with accuracies of 3–5% in the outgoing energy from 0.1 to 9 MeV and 15% from 9 to 12 MeV and to provide detailed experimental uncertainties. Neutrons from the WNR/LANSCE neutron source are being used to induce fission in a Parallel-Plate Avalanche Counter (PPAC). Two arrays of neutron detectors are used to cover the energy range of neutrons emitted promptly in the fission process. Challenges for the present experiment include background reduction, use of {sup 239}Pu in a PPAC, and understanding neutron detector response. Achieving the target accuracies requires the understanding of many systematic uncertainties. The status and plans for the future will be presented.

  18. UPWARD MOVEMENT OF PLUTONIUM TO SURFACE SEDIMENTS DURING AN 11-YEAR FIELD STUDY

    Energy Technology Data Exchange (ETDEWEB)

    Kaplan, D.; Beals, D.; Cadieux, J.; Halverson, J.

    2010-01-25

    An 11-y lysimeter study was established to monitor the movement of Pu through vadose zone sediments. Sediment Pu concentrations as a function of depth indicated that some Pu moved upward from the buried source material. Subsequent numerical modeling suggested that the upward movement was largely the result of invading grasses taking up the Pu and translocating it upward. The objective of this study was to determine if the Pu of surface sediments originated from atmosphere fallout or from the buried lysimeter source material (weapons-grade Pu), providing additional evidence that plants were involved in the upward migration of Pu. The {sup 240}Pu/{sup 239}Pu and {sup 242}Pu/{sup 239}Pu atomic fraction ratios of the lysimeter surface sediments, as determined by Thermal Ionization Mass Spectroscopy (TIMS), were 0.063 and 0.00045, respectively; consistent with the signatures of the weapons-grade Pu. Our numerical simulations indicate that because plants create a large water flux, small concentrations over multiple years may result in a measurable accumulation of Pu on the ground surface. These results may have implications on the conceptual model for calculating risk associated with long-term stewardship and monitored natural attenuation management of Pu contaminated subsurface and surface sediments.

  19. Resolving Nevada Test Site and global fallout plutonium in attic dust and soils using [sup 137]Cs/[sup 239+240]Pu activity ratios

    Energy Technology Data Exchange (ETDEWEB)

    Cizdziel, J. (Univ. of Nevada, Reno, NV (United States)); Hodge, V. (Univ. of Nevada, Las Vegas, NV (United States). Dept. of Chemistry); Faller, S. (Environmental Protection Agency, Las Vegas, NV (United States). Radiation and Indoor Environments National Lab.)

    1999-07-01

    A simple equation using only [sup 137]Cs/[sup 239+240]Pu activity ratios was developed and evaluated as a means of resolving the plutonium in attic dust and soil from Nevada and Utah that came from Nevada Test Site fallout from that which came from global fallout. Applied to a historical data set of [sup 137]Cs and [sup 239+240]Pu activity concentrations in soils from Nevada and Utah, the activity ratio method gives results similar to the traditional [sup 240]Pu/[sup 239]Pu isotope mass ratio method. Considering the difficulty and expense of determining the [sup 240]Pu/[sup 239]Pu atom ratios, this activity ratio method is simpler, faster, and less costly, and may be useful for detecting and/or monitoring plutonium contamination in soils. Applied to samples of attic dust and soil collected from throughout southern Nevada and Utah during 1996 and 1997, it was found that all sites surveyed showed the presence of Nevada Test Site plutonium. Over 90% of the plutonium found in the samples from Beatty, Tonopah, and Queen City Summit, Nevada can be attributed to the Nevada Test Site.

  20. Korea-NEA Research Project for the Construction of Worldwide Reactor Physics Experiments Database and the Foundation of Sustainable Collaboration Environment

    Energy Technology Data Exchange (ETDEWEB)

    Kim, Sang Ji; Jang, Jin Wook

    2004-07-15

    740 documents on PWR, LMR and VHTR related critical experiments are procured by participating in the IRPhE Project under the auspices of the OECD/NEA Data Bank. These documents were reviewed in detail for classification, measurement technique study. Among the database, the SNEAK-7 critical benchmarks were selected for further analysis by modern analysis tool, which requires minimum amount of correction for the raw calculated value. The SNEAK-7A and 7B were selected due to their spectrum similarity with KALIMER-600. Core eigenvalue, spectral indices, central material worths were evaluated and compared with the measurement. JEF-2.2 predict core eigenvalues pretty well, while the conversion ratio was underestimated by about 3%. ENDF/B-VI overestimates core eigenvalue by about 500 pcm while the conversion ratio was underestimated by about 4%. Through the sensitivity analysis of core eigenvalue to the partial cross section, a problem in {sup 238}U capture cross section was identified and a necessity arose to reduce the measurement uncertainty of {sup 239}Pu due to the high high sensitivity of core eigenvalue to {sup 239}Pu fission cross section.

  1. Radiation-induced decomposition of U(VI) phases to nanocrystals of UO"2 [rapid communication

    Science.gov (United States)

    Utsunomiya, Satoshi; Ewing, Rodney C.; Wang, Lu-Min

    2005-12-01

    U 6+-phases are common alteration products, under oxidizing conditions, of uraninite and the UO 2 in spent nuclear fuel. These U 6+-phases are subjected to a radiation field caused by the α-decay of U, or in the case of spent nuclear fuel, incorporated actinides, such as 239Pu and 237Np. In order to evaluate the effects of α-decay events on the stability of the U 6+-phases, we report, for the first time, the results of ion beam irradiations (1.0 MeV Kr 2+) of U 6+-phases. The heavy-particle irradiations are used to simulate the ballistic interactions of the recoil-nucleus of an α-decay event with the surrounding structure. The Kr 2+-irradiation decomposed the U 6+-phases to UO 2 nanocrystals at doses as low as 0.006 displacements per atom (dpa). U 6+-phases accumulate substantial radiation doses (˜1.0 displacement per atom) within 100,000 yr if the concentration of incorporated 239Pu is as high as 1 wt.%. Similar nanocrystals of UO 2 were observed in samples from the natural fission reactors at Oklo, Gabon. Multiple cycles of radiation-induced decomposition to UO 2 followed by alteration to U 6+-phases provide a mechanism for the remobilization of incorporated radionuclides.

  2. Semianalytical Solutions of Radioactive or Reactive Tracer Transport in Layered Fractured Media

    Energy Technology Data Exchange (ETDEWEB)

    G.J. Moridis; G. S. Bodvarsson

    2001-10-01

    In this paper, semianalytical solutions are developed for the problem of transport of radioactive or reactive tracers (solutes or colloids) through a layered system of heterogeneous fractured media with misaligned fractures. The tracer transport equations in the matrix account for (a) diffusion, (b) surface diffusion (for solutes only), (c) mass transfer between the mobile and immobile water fractions, (d) linear kinetic or equilibrium physical, chemical, or combined solute sorption or colloid filtration, and (e) radioactive decay or first order chemical reactions. Any number of radioactive decay daughter products (or products of a linear, first-order reaction chain) can be tracked. The tracer-transport equations in the fractures account for the same processes, in addition to advection and hydrodynamic dispersion. Additionally, the colloid transport equations account for straining and velocity adjustments related to the colloidal size. The solutions, which are analytical in the Laplace space, are numerically inverted to provide the solution in time and can accommodate any number of fractured and/or porous layers. The solutions are verified using analytical solutions for limiting cases of solute and colloid transport through fractured and porous media. The effect of important parameters on the transport of {sup 3}H, {sup 237}Np and {sup 239}Pu (and its daughters) is investigated in several test problems involving layered geological systems of varying complexity. {sup 239}Pu colloid transport problems in multilayered systems indicate significant colloid accumulations at straining interfaces but much faster transport of the colloid than the corresponding strongly sorbing solute species.

  3. UPWARD MOVEMENT OF PLUTONIUM TO SURFACE SEDIMENTS DURING AN 11-YEAR FIELD STUDY

    Energy Technology Data Exchange (ETDEWEB)

    Kaplan, D.; Beals, D.; Cadieux, J.; Halverson, J.

    2010-01-25

    An 11-y lysimeter study was established to monitor the movement of Pu through vadose zone sediments. Sediment Pu concentrations as a function of depth indicated that some Pu moved upward from the buried source material. Subsequent numerical modeling suggested that the upward movement was largely the result of invading grasses taking up the Pu and translocating it upward. The objective of this study was to determine if the Pu of surface sediments originated from atmosphere fallout or from the buried lysimeter source material (weapons-grade Pu), providing additional evidence that plants were involved in the upward migration of Pu. The {sup 240}Pu/{sup 239}Pu and {sup 242}Pu/{sup 239}Pu atomic fraction ratios of the lysimeter surface sediments, as determined by Thermal Ionization Mass Spectroscopy (TIMS), were 0.063 and 0.00045, respectively; consistent with the signatures of the weapons-grade Pu. Our numerical simulations indicate that because plants create a large water flux, small concentrations over multiple years may result in a measurable accumulation of Pu on the ground surface. These results may have implications on the conceptual model for calculating risk associated with long-term stewardship and monitored natural attenuation management of Pu contaminated subsurface and surface sediments.

  4. Contribution to the chromatography of atmospheric gases (1963); Contribution a la chromatographie des gaz de l'air (1963)

    Energy Technology Data Exchange (ETDEWEB)

    Ghalamsiah, A. [Commissariat a l' Energie Atomique, Saclay (France). Centre d' Etudes Nucleaires

    1963-06-15

    In the first part, the author studies the gas-phase chromatographic separation of the atmospheric rare gases, of hydrogen, and of some gaseous compounds of carbon (CO, CO{sub 2}, CH{sub 4}) using inactive gases to obtain the most favourable operational conditions far this separation. In the second part, the optimum conditions for detecting non-active gases using an ionisation chamber and a {sup 239}Pu radioactive source emitting 5.15 MeV {alpha} particles are determined. (author) [French] Dans une premiere partie, l'auteur etudie la separation par chromatographie en phase gazeuse des gaz rares de l'air, de l'hydrogene, et de quelques composes gazeux du carbone (CO, CO{sub 2}, CH{sub 4}) en utilisant des gaz inactifs an vue d'obtenir les conditions experimenales les plus favorables en vue de cette separation. Dans une deuxieme partie, les conditions optimales de detection de gaz non actifs a l'aide d'une chambre d'ionisation, en utilisant comme source radioactive du {sup 239}Pu qui emet des particules {alpha} de 5,15 MeV, sont determinees. (auteur)

  5. Comparison of Two Approaches for Nuclear Data Uncertainty Propagation in MCNPX for Selected Fast Spectrum Critical Benchmarks

    Science.gov (United States)

    Zhu, T.; Rochman, D.; Vasiliev, A.; Ferroukhi, H.; Wieselquist, W.; Pautz, A.

    2014-04-01

    Nuclear data uncertainty propagation based on stochastic sampling (SS) is becoming more attractive while leveraging modern computer power. Two variants of the SS approach are compared in this paper. The Total Monte Carlo (TMC) method by the Nuclear Research and Consultancy Group (NRG) generates perturbed ENDF-6-formatted nuclear data by varying nuclear reaction model parameters. At Paul Scherrer Institute (PSI) the Nuclear data Uncertainty Stochastic Sampling (NUSS) system generates perturbed ACE-formatted nuclear data files by applying multigroup nuclear data covariances onto pointwise ACE-formatted nuclear data. Uncertainties of 239Pu and 235U from ENDF/B-VII.1, ZZ-SCALE6/COVA-44G and TENDL covariance libraries are considered in NUSS and propagated in MCNPX calculations for well-studied Jezebel and Godiva fast spectrum critical benchmarks. The corresponding uncertainty results obtained by TMC are compared with NUSS results and the deterministic Sensitivity/Uncertainty method of TSUNAMI-3D from SCALE6 package is also applied to serve as a separate verification. The discrepancies in the propagated 239Pu and 235U uncertainties due to method and covariance differences are discussed.

  6. Results of The Excreta Bioassay Quality Control Program For April 1, 2008 through March 31, 2009

    Energy Technology Data Exchange (ETDEWEB)

    Antonio, Cheryl L.

    2010-06-01

    A total of 62 urine samples and 6 spiked fecal samples were submitted during the report period (April 1, 2008 through March 31, 2009) to General Engineering Laboratories, South Carolina by the Hanford Internal Dosimetry Program (IDP) to check the accuracy, precision, and detection levels of their analyses. Urine analyses for Sr, 238Pu, 239Pu, 241Am, 243Am 235U, 238U, elemental uranium and fecal analyses for 241Am, 238Pu and 239Pu were tested this year. The number of QC urine samples submitted during the report period represented 1.3% of the total samples submitted. In addition to the samples provided by IDP, GEL was also required to conduct their own QC program, and submit the results of analyses to IDP. About 34% of the analyses processed by GEL during the third year of this contract were quality control samples. GEL tested the performance of 21 radioisotopes, all of which met or exceeded the specifications in the Statement of Work within statistical uncertainty. IDP concluded that GEL was performing well for all analyses tested, and concerns identified earlier were satisfactorily resolved (see section on Follow-up on Concerns During the Fourth Contract Year).

  7. Preparation of a multi-isotope plutonium AMS standard and preliminary results of a first inter-lab comparison

    Science.gov (United States)

    Dittmann, B.-A.; Dunai, T. J.; Dewald, A.; Heinze, S.; Feuerstein, C.; Strub, E.; Fifield, L. K.; Froehlich, M. B.; Tims, S. G.; Wallner, A.; Christl, M.

    2015-10-01

    The motivation of this work is to establish a new multi-isotope plutonium standard for isotopic ratio measurements with accelerator mass spectrometry (AMS), since stocks of existing solutions are declining. To this end, certified reference materials (CRMs) of each of the individual isotopes 239Pu, 240Pu, 242Pu and 244Pu were obtained from JRC IRMM (Joint Research Center Institute for Reference Materials and Measurements). These certified reference materials (IRMM-081a, IRMM-083, IRMM-043 and IRMM-042a) were diluted with nitric acid and mixed to obtain a stock standard solution with an isotopic ratio of approximately 1.0:1.0:1.0:0.1 (239Pu:240Pu:242Pu:244Pu). From this stock solution, samples were prepared for measurement of the plutonium isotopic composition by AMS. These samples have been measured in a round-robin exercise between the AMS facilities at CologneAMS, at the ANU Canberra and ETH Zurich to verify the isotopic ratio and to demonstrate the reproducibility of the measurements. The results show good agreement both between the different AMS measurements and with the gravimetrically determined nominal ratios.

  8. Status of the compact 1 MV AMS facility at the Centro Nacional de Aceleradores (Spain)

    Energy Technology Data Exchange (ETDEWEB)

    Chamizo, E. [Centro Nacional de Aceleradores (CNA), Avda. Thomas Alva Edison 7, Isla de la Cartuja, 41092 Seville (Spain); Lopez-Gutierrez, J.M. [Centro Nacional de Aceleradores (CNA), Avda. Thomas Alva Edison 7, Isla de la Cartuja, 41092 Seville (Spain); Dpto. de Fisica Aplicada I, Escuela Universitaria Politecnica, c/. Virgen de Africa 7, 41011 Seville (Spain)], E-mail: lguti@us.es; Ruiz-Gomez, A.; Santos, F.J. [Centro Nacional de Aceleradores (CNA), Avda. Thomas Alva Edison 7, Isla de la Cartuja, 41092 Seville (Spain); Garcia-Leon, M. [Centro Nacional de Aceleradores (CNA), Avda. Thomas Alva Edison 7, Isla de la Cartuja, 41092 Seville (Spain); Dpto. Fisica Atomica, Molecular y Nuclear, Avda. Reina Mercedes, s/n, 41012 Seville (Spain); Maden, C. [Centro Nacional de Aceleradores (CNA), Avda. Thomas Alva Edison 7, Isla de la Cartuja, 41092 Seville (Spain); Alfimov, V. [Institute of Particle Physics, HPK, ETH Hoenggerberg, CH-8093 Zurich (Switzerland)

    2008-05-15

    Since February 2006, the new 1 MV multielement compact AMS facility SARA (Spanish Accelerator for Radionuclides Analyses) at the Centro Nacional de Aceleradores (CNA) in Sevilla (Spain) is fully operative. During the first one and a half year of operation, the viability of the system for the measurement of {sup 10}Be, {sup 14}C, {sup 129}I and plutonium isotopes, {sup 239}Pu and {sup 240}Pu, has been evaluated. First results have demonstrated that, in terms of precision and detection limits, the performance of the device compares to other compact AMS facilities, although some progress can still be done in order to optimize its capacities. At this moment, background levels are in the order of 10{sup -14} for {sup 10}Be/{sup 9}Be, 10{sup -13} for {sup 129}I/{sup 127}I, 10{sup -15} for {sup 14}C/{sup 12}C (processed and unprocessed blank) and about 10{sup 6} atoms for plutonium isotopes: {sup 239}Pu, {sup 240}Pu and {sup 242}Pu. In this work, the current status of the AMS measurements at CNA for the above mentioned radionuclides is described.

  9. Measurements of low-level anthropogenic radionuclides from soils around Maralinga

    Science.gov (United States)

    Tims, Stephen G.; Tsifakis, Dimitrios; Srncik, Michaela; Fifield, L. Keith; Hancock, Gary J.; De Cesare, Mario

    2013-12-01

    The isotopes 239Pu and 240Pu are present in surface soils as a result of global fallout from nuclear weapons tests carried out in the 1950's and 1960's. These isotopes constitute artificial tracers of recent soil erosion and sediment movement. In practice the high throughput capabilities and high sensitivity of the AMS technique makes the study of Australia's geographically large areas viable using Pu isotopes. As part of its weapons development program the United Kingdom carried out a series of atmospheric and surface nuclear weapons tests at Maralinga, South Australia in 1956 and 1957. The contribution from the Maralinga tests to the Pu isotopic abundances present in the region around Maralinga is largely unknown. In global fallout, for example, the 240Pu/239Pu ratio is typically in the range 0.17 - 0.19, but the influence of the regional tests could lead to values outside this range. This would impact on the assessment techniques used in the soil and sediment tracer studies. We report recent measurements on soil samples collected from across the Maralinga Test site.

  10. Measurements of low-level anthropogenic radionuclides from soils around Maralinga

    Directory of Open Access Journals (Sweden)

    Tims Stephen G.

    2013-12-01

    Full Text Available The isotopes 239Pu and 240Pu are present in surface soils as a result of global fallout from nuclear weapons tests carried out in the 1950’s and 1960’s. These isotopes constitute artificial tracers of recent soil erosion and sediment movement. In practice the high throughput capabilities and high sensitivity of the AMS technique makes the study of Australia’s geographically large areas viable using Pu isotopes. As part of its weapons development program the United Kingdom carried out a series of atmospheric and surface nuclear weapons tests at Maralinga, South Australia in 1956 and 1957. The contribution from the Maralinga tests to the Pu isotopic abundances present in the region around Maralinga is largely unknown. In global fallout, for example, the 240Pu/239Pu ratio is typically in the range 0.17 - 0.19, but the influence of the regional tests could lead to values outside this range. This would impact on the assessment techniques used in the soil and sediment tracer studies. We report recent measurements on soil samples collected from across the Maralinga Test site.

  11. Isotopic composition and distribution of plutonium in northern South China Sea sediments revealed continuous release and transport of Pu from the Marshall Islands.

    Science.gov (United States)

    Wu, Junwen; Zheng, Jian; Dai, Minhan; Huh, Chih-An; Chen, Weifang; Tagami, Keiko; Uchida, Shigeo

    2014-03-18

    The (239+240)Pu activities and (240)Pu/(239)Pu atom ratios in sediments of the northern South China Sea and its adjacent Pearl River Estuary were determined to examine the spatial and temporal variations of Pu inputs. We clarified that Pu in the study area is sourced from a combination of global fallout and close-in fallout from the Pacific Proving Grounds in the Marshall Islands where above-ground nuclear weapons testing was carried out during the period of 1952-1958. The latter source dominated the Pu input in the 1950s, as evidenced by elevated (240)Pu/(239)Pu atom ratios (>0.30) in a dated sediment core. Even after the 1950s, the Pacific Proving Grounds was still a dominant Pu source due to continuous transport of remobilized Pu from the Marshall Islands, about 4500 km away, along the North Equatorial Current followed by the transport of the Kuroshio current and its extension into the South China Sea through the Luzon Strait. Using a simple two end-member mixing model, we have quantified the contributions of Pu from the Pacific Proving Grounds to the northern South China Sea shelf and the Pearl River Estuary are 68% ± 1% and 30% ± 5%, respectively. This study also confirmed that there were no clear signals of Pu from the Fukushima Daiichi Nuclear Power Plant accident impacting the South China Sea.

  12. Transport of (137)Cs, (241)Am and Pu isotopes in the Curonian Lagoon and the Baltic Sea.

    Science.gov (United States)

    Lujanienė, G; Remeikaitė-Nikienė, N; Garnaga, G; Jokšas, K; Šilobritienė, B; Stankevičius, A; Šemčuk, S; Kulakauskaitė, I

    2014-01-01

    Activities of (137)Cs, (241)Am and (239,240)Pu were analyzed with special emphasis on better understanding of radionuclide transport from land via the Neman River estuaries to the Baltic Sea and behavior in the marine environment. Although activity concentrations of (137)Cs in water samples collected the Baltic Sea were almost 100 times higher as compared to the Curonian Lagoon, its activities in the bottom sediments were found to be comparable. Activity (238)Pu/(239,240)Pu and atom (240)Pu/(239)Pu ratios indicated a different contribution of the Chernobyl-originated Pu to the suspended particulate matter (SPM) and bottom sediments. The largest amount of the Chernobyl-derived Pu was found in the smallest suspended matter particles of 0.2-1 μm in size collected in the Klaipeda Strait in 2011-2012. The decrease of characteristic activity (238)Pu/(239,240)Pu and atom (240)Pu/(239)Pu ratios towards the global fallout ones in surface soil and the corresponding increase of plutonium (Pu) ratios in the suspended particulate matter and bottom sediments have indicated that the Chernobyl-derived Pu, primarily deposited on the soil surface, was washed out and transported to the Baltic Sea. Behavior of (241)Am was found to be similar to that of Pu isotopes.

  13. Conversion electron spectrometry of Pu isotopes with a silicon drift detector.

    Science.gov (United States)

    Pommé, S; Paepen, J; Peräjärvi, K; Turunen, J; Pöllänen, R

    2016-03-01

    An electron spectrometry set-up was built at IRMM consisting of a vacuum chamber with a moveable source holder and windowless Peltier-cooled silicon drift detector (SDD). The SDD is well suited for measuring low-energy x rays and electrons emitted from thin radioactive sources with low self-absorption. The attainable energy resolution is better than 0.5keV for electrons of 30keV. It has been used to measure the conversion electron spectra of three plutonium isotopes, i.e. (238)Pu, (239)Pu, (240)Pu, as well as (241)Am (being a decay product of (241)Pu). The obtained mixed x-ray and electron spectra are compared with spectra obtained with a close-geometry set-up using another SDD in STUK and spectra measured with a Si(Li) detector at IRMM. The potential of conversion electron spectrometry for isotopic analysis of mixed plutonium samples is investigated. With respect to the (240)Pu/(239)Pu isotopic ratio, the conversion electron peaks of both isotopes are more clearly separated than their largely overlapping peaks in alpha spectra.

  14. Late Time Emission of Prompt Fission Gamma Rays

    CERN Document Server

    Talou, P; Stetcu, I; Lestone, J P; McKigney, E; Chadwick, M B

    2016-01-01

    The emission of prompt fission $\\gamma$ rays within a few nanoseconds to a few microseconds following the scission point is studied in the Hauser-Feshbach formalism applied to the deexcitation of primary excited fission fragments. Neutron and $\\gamma$-ray evaporations from fully accelerated fission fragments are calculated in competition at each stage of the decay, and the role of isomers in the fission products, before $\\beta$-decay, is analyzed. The time evolution of the average total $\\gamma$-ray energy, average total $\\gamma$-ray multiplicity, and fragment-specific $\\gamma$-ray spectra, is presented in the case of neutron-induced fission reactions of $^{235}$U and $^{239}$Pu, as well as spontaneous fission of $^{252}$Cf. The production of specific isomeric states is calculated and compared to available experimental data. About 7% of all prompt fission $\\gamma$ rays are predicted to be emitted between 10 nsec and 5 $\\mu$sec following fission, in the case of $^{235}$U and $^{239}$Pu $(n_{\\rm th},f)$ reactio...

  15. Plutonium isotopes in the terrestrial environment at the Savannah River Site, USA: a long-term study.

    Science.gov (United States)

    Armstrong, Christopher R; Nuessle, Patterson R; Brant, Heather A; Hall, Gregory; Halverson, Justin E; Cadieux, James R

    2015-02-01

    This work presents the findings of a long-term plutonium (Pu) study at Savannah River Site (SRS) conducted between 2003 and 2013. Terrestrial environmental samples were obtained at the Savannah River National Laboratory (SRNL) in the A-Area. Plutonium content and isotopic abundances were measured over this time period by α particle and thermal ionization mass spectrometry (3STIMS). We detail the complete process of the sample collection, radiochemical separation, and measurement procedure specifically targeted to trace plutonium in bulk environmental samples. Total plutonium activities were determined to be not significantly above atmospheric global fallout. However, the (238)Pu/(239+240)Pu activity ratios attributed to SRS are substantially different than fallout due to past (238)Pu production on the site. The (240)Pu/(239)Pu atom ratios are reasonably consistent from year to year and are lower than fallout indicating an admixture of weapons-grade material, while the (242)Pu/(239)Pu atom ratios are higher than fallout values, again due to actinide production activities. Overall, the plutonium signatures obtained in this study reflect a distinctive mixture of weapons-grade, heat source, and higher burn-up plutonium with fallout material. This study provides a unique opportunity for developing and demonstrating a blue print for long-term low-level monitoring of trace plutonium in the environment.

  16. Determination of plutonium content in high burnup pressurized water reactor fuel samples and its use for isotope correlations for isotopic composition of plutonium.

    Science.gov (United States)

    Joe, Kihsoo; Jeon, Young-Shin; Han, Sun-Ho; Lee, Chang-Heon; Ha, Yeong-Keong; Song, Kyuseok

    2012-06-01

    The content of plutonium isotopes in high burnup pressurized water reactor fuel samples was examined using both alpha spectrometry and mass spectrometry after anion exchange separation. The measured values were compared with results calculated by the ORIGEN-2 code. On average, the ratios (m/c) of the measured values (m) over the calculated values (c) were 1.22±0.16 for (238)Pu, 1.02±0.14 for (239)Pu, 1.08±0.06 for (240)Pu, 1.06±0.16 for (241)Pu, and 1.13±0.08 for (242)Pu. Using the Pu data obtained in this work, correlations were derived between the alpha activity ratios of (238)Pu/((239)Pu+(240)Pu), the alpha specific activities of Pu, and the atom % abundances of the Pu isotopes. Using these correlations, the atom % abundances of the plutonium isotopes in the target samples were calculated. These calculated results agreed within a range from 2 to 8% of the experimentally derived values according to the isotopes of plutonium.

  17. 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

    Energy Technology Data Exchange (ETDEWEB)

    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)

  18. Semianalytical solutions of radioactive or reactive tracer transport in layered fractured media

    Energy Technology Data Exchange (ETDEWEB)

    Moridis, G.J.; Bodvarsson, G.S.

    2001-10-10

    In this paper, semianalytical solutions are developed for the problem of transport of radioactive or reactive tracers (solutes or colloids) through a layered system of heterogeneous fractured media with misaligned fractures. The tracer transport equations in the matrix account for (a) diffusion, (b) surface diffusion (for solutes only), (c) mass transfer between the mobile and immobile water fractions, (d) linear kinetic or equilibrium physical, chemical, or combined solute sorption or colloid filtration, and (e) radioactive decay or first order chemical reactions. Any number of radioactive decay daughter products (or products of a linear, first-order reaction chain) can be tracked. The tracer-transport equations in the fractures account for the same processes, in addition to advection and hydrodynamic dispersion. Additionally, the colloid transport equations account for straining and velocity adjustments related to the colloidal size. The solutions, which are analytical in the Laplace space, are numerically inverted to provide the solution in time and can accommodate any number of fractured and/or porous layers. The solutions are verified using analytical solutions for limiting cases of solute and colloid transport through fractured and porous media. The effect of important parameters on the transport of {sup 3}H, {sup 237}Np and {sup 239}Pu (and its daughters) is investigated in several test problems involving layered geological systems of varying complexity. {sup 239}Pu colloid transport problems in multilayered systems indicate significant colloid accumulations at straining interfaces but much faster transport of the colloid than the corresponding strongly sorbing solute species.

  19. A fast semi-quantitative method for Plutonium determination in an alpine firn/ice core

    Science.gov (United States)

    Gabrieli, J.; Cozzi, G.; Vallelonga, P.; Schwikowski, M.; Sigl, M.; Boutron, C.; Barbante, C.

    2009-04-01

    Plutonium is present in the environment as a consequence of atmospheric nuclear tests carried out in the 1960s, nuclear weapons production and releases by the nuclear industry over the past 50 years. Plutonium, unlike uranium, is essentially anthropogenic and it was first produced and isolated in 1940 by deuteron bombardment of uranium in the cyclotron of Berkeley University. It exists in five main isotopes, 238Pu, 239Pu, 240Pu, 241Pu, 242Pu, derived from civilian and military sources (weapons production and detonation, nuclear reactors, nuclear accidents). In the environment, 239Pu is the most abundant isotope. Approximately 6 tons of 239Pu have been released into the environment as a result of 541 atmospheric weapon tests Nuclear Pu fallout has been studied in various environmental archives, such as sediments, soil and herbarium grass. Mid-latitude ice cores have been studied as well, on Mont Blanc, the Western Alps and on Belukha Glacier, Siberian Altai. We present a Pu record obtained by analyzing 52 discrete samples of an alpine firn/ice core from Colle Gnifetti (M. Rosa, 4450 m a.s.l.), dating from 1945 to 1991. The239Pu signal was recorded directly, without preliminary cleaning or preconcentration steps, using an ICP-SFMS (Thermo Element2) equipped with a desolvation system (APEX). 238UH+ interferences were negligible for U concentrations lower than 50 ppt as verified both in spiked fresh snow and pre-1940 ice samples. The shape of 239Pu profile reflects the three main periods of atmospheric nuclear weapons testing: the earliest peak starts in 1954/55 to 1958 and includes the first testing period which reached a maximum in 1958. Despite a temporary halt in testing in 1959/60, the Pu concentration decreased only by half with respect to the 1958 peak. In 1961/62 Pu concentrations rapidly increased reaching a maximum in 1963, which was about 40% more intense than the 1958 peak. After the sign of the "Limited Test Ban Treaty" between USA and URSS in 1964, Pu

  20. Signatures of special nuclear material: High-energy gamma rays following fission

    Energy Technology Data Exchange (ETDEWEB)

    Norman, Eric B.; Prussin, Stanley G.; Larimer, Ruth-Mary; Shugart, Howard; Browne, Edgardo; Smith, Alan R.; McDonald, Rchard J.; Nitsche, Heino; Gupta, Puja; Frank, Michael I.; Gosnell, Thomas B.

    2003-05-29

    Since September 11, 2001, much effort has been devoted to the development of new and improved means for the detection and prevention of the clandestine transport of special nuclear material (SNM, i.e. {sup 235}U or {sup 239}Pu) and other materials for producing weapons of mass destruction. In a recent Brief Communication, Borozdin et al. showed that cosmic-ray muons could be used to image dense objects inside containers. Here we describe a method for unequivocally identifying SNM in large seagoing containers. Our method is based on the fact that neutron-induced fission of {sup 235}U or {sup 239}Pu is followed by {beta} decays of short-lived fission fragments during which large numbers of high-energy {gamma} rays (above 3000 keV) are emitted. These {gamma} rays have energies above those of natural {gamma} background, are emitted with significantly greater intensity per fission than {beta}-delayed neutrons, have much higher probabilities of escaping hydrogenous cargo loadings than neutrons, and their energy spectra and time dependencies provide a unique signature of SNM. To demonstrate the main properties of high-energy delayed {gamma} rays, we produced neutrons by bombarding a 1-inch thick water-cooled Be target with 16-MeV deuterons from Lawrence Berkeley National Laboratory's 88-Inch Cyclotron. Neutrons were moderated using steel and polyethylene. We employed a pneumatic transfer system to shuttle targets from the irradiation location inside the polyethylene moderator to a remote shielded counting station. We irradiated {sup 235}U (93% isotopic content), {sup 239}Pu (95% isotopic content), wood, polyethylene, aluminum, sandstone, and steel targets for 30 seconds (in a thermal-neutron flux of 1.5 x 10{sup 6}/cm{sup 2}-sec) and acquired 10 sequential {gamma}-ray spectra, each of 3 sec. duration starting 3 sec. after the end of bombardment. We used an 80% relative efficiency coaxial germanium detector and a 30-cm x 30-cm x 10-cm plastic scintillator to detect

  1. Studies of Long-lived Radionuclides in the Environment - with Emphasis on {sup 99}Tc, {sup 237}Np and Pu Isotopes

    Energy Technology Data Exchange (ETDEWEB)

    Lindahl, Patric

    2003-03-01

    Studies of the long-lived anthropogenic radionuclides 99Tc, 237Np, 239Pu and 240Pu were performed in marine and terrestrial areas contaminated by different accidental and controlled releases of radioactive materials. The three main sources discussed in this thesis are nuclear weapons tests, nuclear reprocessing plants and the Chernobyl accident. Results are mainly based on measurements of environmental samples collected in different parts of Sweden. An analytical method for trace analysis of plutonium and neptunium in environmental samples using ICP-MS (Inductively Coupled Plasma Mass Spectrometry) is described, and the results compared with those from conventional alpha spectrometry. The use of activated carbon filters for the separation of 99Tc from marine waters, with an adsorption efficiency in the range of 70%, is described. During 1991, 1995 and 2001 brown seaweed samples were collected at several stations along the Swedish west coast. In addition to these locations, a well-defined site (Saerdal; 56.76 deg N, 12.63 deg E) was included from which 99Tc data were collected from 1967 to 2000. The effect of discharges from the Sellafield EARP (Enhanced Actinide Removal Plant) from 1995-1996 was observed in brown seaweed from the Swedish west coast 4-5 years later, with a ten-fold increase in 99Tc activity concentration. An inverse correlation between 99Tc and 137Cs concentrations in seaweed was observed due to continuous mixing of high-Tc-low-Cs (Atlantic Sea) and low-Tc-high-Cs (Baltic Sea) waters. Radioactive materials from the Chernobyl accident contaminated various part of Sweden and by analysing lichen samples from different areas an estimate of the deposited 237Np density could be made. Through the determination of 240Pu/239Pu and 237Np/239Pu atomic ratios, source identification could be made in Swedish lichen samples. In the areas most contaminated by the Chernobyl accident in Sweden, the Chernobyl-derived 237Np contribution was up to 30% of the total

  2. Criticality Evaluation of Plutonium-239 Moderated by High-Density Polyethylene in Stainless Steel and Aluminum Containers Suitable for Non-Exclusive Use Transport

    Energy Technology Data Exchange (ETDEWEB)

    Watson, T T

    2007-08-10

    Research is conducted at the Joint Actinide Shock Physics Experimental Facility (JASPER) on the effects of high pressure and temperature environments on plutonium-239, in support of the stockpile stewardship program. Once an experiment has been completed, it is necessary to transport the end products for interim storage or final disposition. Federal shipping regulations for nonexclusive use transportation require that no more than 180 grams of fissile material are present in at least 360 kilograms of contiguous non-fissile material. To evaluate the conservatism of these regulatory requirements, a worst-case scenario of 180g {sup 239}Pu and a more realistic scenario of 100g {sup 239}Pu were modeled using one of Lawrence Livermore National Laboratory's Monte Carlo transport codes known as COG 10. The geometry consisted of {sup 239}Pu spheres homogeneously mixed with high-density polyethylene surrounded by a cube of either stainless steel 304 or aluminum. An optimized geometry for both cube materials and hydrogen-to-fissile isotope (H/X) ratio were determined for a single unit. Infinite and finite 3D arrays of these optimized units were then simulated to determine if the systems would exceed criticality. Completion of these simulations showed that the optimal H/X ratio for the most reactive units ranged from 800 to 1600. A single unit of either cube type for either scenario would not reach criticality. An infinite array was determined to reach criticality only for the 180g case. The offsetting of spheres in their respective cubes was also considered and showed a considerable decrease in the number of close-packed units needed to reach criticality. These results call into question the current regulations for fissile material transport, which under certain circumstances may not be sufficient in preventing the development of a critical system. However, a conservative, theoretical approach was taken in all assumptions and such idealized configurations may not be

  3. Plutonium isotopes in the ocean off Japan after Fukushima

    Energy Technology Data Exchange (ETDEWEB)

    Buesseler, K.; Black, E.; Pike, S. [Woods Hole Oceanographic Institution (United States); Kenna, T. [Lamont-Doherty Earth Observatory (United States); Masque, P. [Universitat Autonoma de Barcelona (Spain)

    2014-07-01

    The Fukushima Dai-ichi nuclear power plants (NPPs) are known to be an unprecedented accidental source of {sup 137}Cs, {sup 134}Cs and other volatile radionuclides to the ocean. Much less is known however about the extent of input of refractory radionuclides such as plutonium to the environment. Limited available data from land soils and vegetation, suggest at least some atmospheric delivery of particulate Pu but at very low levels relative to pre-existing fallout sources. To resolve Fukushima derived Pu from weapons testing derived Pu, information regarding the Pu isotopic composition is needed. The {sup 240}Pu/{sup 239}Pu atom ratio determined by mass spectrometric techniques, and the {sup 238}Pu/{sup 239,240}Pu activity ratio as measured by alpha counting are diagnostic with respect to Pu source. We review and present new data on the Pu isotopic ratios and concentrations in the oceans, combining several data sets on dissolved (from bottle sampling), suspended particulates (from filtration), sinking particles (from sediment traps) and seafloor sediments (from cores) to look for the Fukushima Pu signal. In most samples, the {sup 240}Pu/{sup 239}Pu ratios are in the range of 0.20-0.23, characteristic of Pu ocean signal which is a combination of global fallout with a characteristic ratio of 0.18 and local fallout from the Pacific Proving Grounds with ratios higher than 0.24, and known from prior studies to influence the ocean off Japan. In 2011, in surface ocean waters, we found ratios {sup 240}Pu/{sup 239}Pu >0.3, which implies a component of Fukushima Pu had been delivered to the ocean, given NPP derived end-member ratios of 0.35-0.45. Fukushima derived Pu was not found deeper in the water column or even at all stations, consistent with its rapid removal from the ocean and the high background of pre-existing Pu in the waters and sediments, masking the new Fukushima sources. With this data a mass balance will be made between Pu from global fallout, local fallout and

  4. Uranium in the Nuclear Fuel Cycle: Creation of Plutonium (Invited)

    Science.gov (United States)

    Ewing, R. C.

    2009-12-01

    One of the important properties of uranium is that it can be used to “breed” higher actinides, particularly plutonium. During the past sixty years, more than 1,800 metric tonnes of Pu, and substantial quantities of the “minor” actinides, such as Np, Am and Cm, have been generated in nuclear reactors - a permanent record of nuclear power. Some of these transuranium elements can be a source of energy in fission reactions (e.g., 239Pu), a source of fissile material for nuclear weapons (e.g., 239Pu and 237Np), and of environmental concern because of their long-half lives and radiotoxicity (e.g., 239Pu and 237Np). In fact, the new strategies of the Advance Fuel Cycle Initiative (AFCI) are, in part, motivated by an effort to mitigate some of the challenges of the disposal of these long-lived actinides. There are two basic strategies for the disposition of these heavy elements: 1.) to “burn” or transmute the actinides using nuclear reactors or accelerators; 2.) to “sequester” the actinides in chemically durable, radiation-resistant materials that are suitable for geologic disposal. There has been substantial interest in the use of actinide-bearing minerals, such as zircon or isometric pyrochlore, A2B2O7 (A= rare earths; B = Ti, Zr, Sn, Hf), for the immobilization of actinides, particularly plutonium, both as inert matrix fuels and nuclear waste forms. Systematic studies of rare-earth pyrochlores have led to the discovery that certain compositions (B = Zr, Hf) are stable to very high doses of alpha-decay event damage1. The radiation stability of these compositions is closely related to the structural distortions that can be accommodated for specific pyrochlore compositions and the electronic structure of the B-site cation. Recent developments in the understanding of the properties of heavy element solids have opened up new possibilities for the design of advanced nuclear fuels and waste forms.

  5. Designing a mini subcritical nuclear reactor; Diseno de un mini reactor nuclear subcritico

    Energy Technology Data Exchange (ETDEWEB)

    Escobedo G, C. R.; Vega C, H. R.; Davila H, V. M., E-mail: rafelaescobedo@hotmail.com [Universidad Autonoma de Zacatecas, Unidad Academica de Estudios Nucleares, Jardin Juarez 147, Col. Centro, 98000 Zacatecas, Zac. (Mexico)

    2015-10-15

    In this work the design of a mini subcritical nuclear reactor formed by means of light water moderator, uranium as fuel, and isotopic neutron source of {sup 239}PuBe was carried out. The design was done by Monte Carlo methods with the code MCNP5 in which uranium was modeled in an array of concentric holes cylinders of 8.5, 14.5, 20.5, 26.5, 32.5 cm of internal radius and 3 cm of thickness, 36 cm of height. Different models were made from a single fuel cylinder (natural uranium) to five. The neutron source of {sup 239}PuBe was situated in the center of the mini reactor; in each arrangement was used water as moderator. Cross sections libraries Endf/Vi were used and the number of stories was large enough to ensure less uncertainty than 3%. For each case the effective multiplication factor k{sub e}-f{sub f}, the amplification factor and the power was calculated. Outside the mini reactor the ambient dose equivalent H (10) was calculated for different cases. The value of k{sub eff}, the amplification factor and power are directly related to the number of cylinders of uranium as fuel. Although the average energy of the neutrons {sup 239}PuBe is between 4.5 and 5 MeV in the case of the mini reactor for a cylinder, in the neutron spectrum the presence of thermal neutrons does not exist, so that produced fissions are generated with fast neutrons, and in designs of two and three rings the neutron spectra shows the presence of thermal neutrons, however the fissions are being generated with fast neutrons. Finally in the four and five cases the amount of moderator is enough to thermalized the neutrons and thereby produce the fission. The maximum value for k{sub eff} was 0.82; this value is very close to the assembly of Universidad Autonoma de Zacatecas generating a k{sub eff} of 0.86. According to the safety and radiation protection standards for the design of mini reactor of one, two and three cylinders they comply with the established safety, while designs of four and five

  6. Performance assessment of self-interrogation neutron resonance densitometry for spent nuclear fuel assay

    Energy Technology Data Exchange (ETDEWEB)

    Hu, Jianwei, E-mail: huj1@ornl.gov [Reactor and Nuclear Systems Division, Oak Ridge National Laboratory, 1 Bethel Valley Road, PO Box 2008, MS-6172, Oak Ridge, TN 37831-6172 (United States); Tobin, Stephen J.; LaFleur, Adrienne M.; Menlove, Howard O.; Swinhoe, Martyn T. [Nuclear Engineering and Nonproliferation Division, Los Alamos National Laboratory (United States)

    2013-11-21

    Self-Interrogation Neutron Resonance Densitometry (SINRD) is one of several nondestructive assay (NDA) techniques being integrated into systems to measure spent fuel as part of the Next Generation Safeguards Initiative (NGSI) Spent Fuel Project. The NGSI Spent Fuel Project is sponsored by the US Department of Energy's National Nuclear Security Administration to measure plutonium in, and detect diversion of fuel pins from, spent nuclear fuel assemblies. SINRD shows promising capability in determining the {sup 239}Pu and {sup 235}U content in spent fuel. SINRD is a relatively low-cost and lightweight instrument, and it is easy to implement in the field. The technique makes use of the passive neutron source existing in a spent fuel assembly, and it uses ratios between the count rates collected in fission chambers that are covered with different absorbing materials. These ratios are correlated to key attributes of the spent fuel assembly, such as the total mass of {sup 239}Pu and {sup 235}U. Using count rate ratios instead of absolute count rates makes SINRD less vulnerable to systematic uncertainties. Building upon the previous research, this work focuses on the underlying physics of the SINRD technique: quantifying the individual impacts on the count rate ratios of a few important nuclides using the perturbation method; examining new correlations between count rate ratio and mass quantities based on the results of the perturbation study; quantifying the impacts on the energy windows of the filtering materials that cover the fission chambers by tallying the neutron spectra before and after the neutrons go through the filters; and identifying the most important nuclides that cause cooling-time variations in the count rate ratios. The results of these studies show that {sup 235}U content has a major impact on the SINRD signal in addition to the {sup 239}Pu content. Plutonium-241 and {sup 241}Am are the two main nuclides responsible for the variation in the count

  7. Concordant plutonium-241-americium-241 dating of environmental samples: results from forest fire ash

    Energy Technology Data Exchange (ETDEWEB)

    Goldstein, Steven J [Los Alamos National Laboratory; Oldham, Warren J [Los Alamos National Laboratory; Murrell, Michael T [Los Alamos National Laboratory; Katzman, Danny [Los Alamos National Laboratory

    2010-12-07

    We have measured the Pu, {sup 237}Np, {sup 241}Am, and {sup 151}Sm isotopic systematics for a set of forest fire ash samples from various locations in the western U.S. including Montana, Wyoming, Idaho, and New Mexico. The goal of this study is to develop a concordant {sup 241}Pu (t{sub 1/2} = 14.4 y)-{sup 241}Am dating method for environmental collections. Environmental samples often contain mixtures of components including global fallout. There are a number of approaches for subtracting the global fallout component for such samples. One approach is to use {sup 242}/{sup 239}Pu as a normalizing isotope ratio in a three-isotope plot, where this ratio for the nonglobal fallout component can be estimated or assumed to be small. This study investigates a new, complementary method of normalization using the long-lived fission product, {sup 151}Sm (t{sub 1/2} = 90 y). We find that forest fire ash concentrates actinides and fission products with {approx}1E10 atoms {sup 239}Pu/g and {approx}1E8 atoms {sup 151}Sm/g, allowing us to measure these nuclides by mass spectrometric (MIC-TIMS) and radiometric (liquid scintillation counting) methods. The forest fire ash samples are characterized by a western U.S. regional isotopic signature representing varying mixtures of global fallout with a local component from atmospheric testing of nuclear weapons at the Nevada Test Site (NTS). Our results also show that {sup 151}Sm is well correlated with the Pu nuclides in the forest fire ash, suggesting that these nuclides have similar geochemical behavior in the environment. Results of this correlation indicate that the {sup 151}Sm/{sup 239}Pu atom ratio for global fallout is {approx}0.164, in agreement with an independent estimate of 0.165 based on {sup 137}Cs fission yields for atmospheric weapons tests at the NTS. {sup 241}Pu-{sup 241}Am dating of the non-global fallout component in the forest fire ash samples yield ages in the late 1950's-early 1960's, consistent with a peak

  8. Concordant 241Pu-241Am Dating of Environmental Samples: Results from Forest Fire Ash

    Science.gov (United States)

    Goldstein, S. J.; Oldham, W. J.; Murrell, M. T.; Katzman, D.

    2010-12-01

    We have measured the Pu, 237Np, 241Am, and 151Sm isotopic systematics for a set of forest fire ash samples from various locations in the western U.S. including Montana, Wyoming, Idaho, and New Mexico. The goal of this study is to develop a concordant 241Pu (t1/2 = 14.4 y)-241Am dating method for environmental collections. Environmental samples often contain mixtures of components including global fallout. There are a number of approaches for subtracting the global fallout component for such samples. One approach is to use 242Pu/239Pu as a normalizing isotope ratio in a three-isotope plot, where this ratio for the non-global fallout component can be estimated or assumed to be small. This study investigates a new, complementary method of normalization using the long-lived fission product, 151Sm (t1/2 = 90 y). We find that forest fire ash concentrates actinides and fission products with ~1E10 atoms 239Pu/g and ~1E8 atoms 151Sm/g, allowing us to measure these nuclides by mass spectrometric (MIC-TIMS) and radiometric (liquid scintillation counting) methods. The forest fire ash samples are characterized by a western U.S. regional isotopic signature representing varying mixtures of global fallout with a local component from atmospheric testing of nuclear weapons at the Nevada Test Site (NTS). Our results also show that 151Sm is well correlated with the Pu nuclides in the forest fire ash, suggesting that these nuclides have similar geochemical behavior in the environment. Results of this correlation indicate that the 151Sm/239Pu atom ratio for global fallout is ~0.164, in agreement with an independent estimate of 0.165 based on 137Cs fission yields for atmospheric weapons tests at the NTS. 241Pu-241Am dating of the non-global fallout component in the forest fire ash samples yield ages in the late 1950’s-early 1960’s, consistent with a peak in NTS weapons testing at that time. The age results for this component are in agreement using both 242Pu and 151Sm normalizations

  9. The solubility of {sup 242}PuO{sub 2} in the presence of aqueous Fe(II). The impact of precipitate preparation

    Energy Technology Data Exchange (ETDEWEB)

    Felmy, Andrew R.; Moore, Dean A.; Buck, Edgar; Kukkadapu, Ravi; Sweet, Lucas; Abrecht, David; Ilton, Eugene S. [Pacific Northwest National Laboratory, Richland, WA (United States); Conrados, Steven D. [Los Alamos National Laboratory, Los Alamos, NM (United States)

    2014-07-01

    The solubility of different forms of precipitated {sup 242}PuO{sub 2}(am) were examined in solutions containing aqueous Fe(II) over a range of pH values. The first series of {sup 242}PuO{sub 2}(am) suspensions were prepared from a {sup 242}Pu(IV) stock that had been treated with thenoyltrifluoroacetone (TTA) to remove the {sup 241}Am originating from the decay of {sup 241}Pu. These {sup 242}PuO{sub 2}(am) suspensions showed much higher solubilities at the same pH value and Fe(II) concentration than previous studies using {sup 239}PuO{sub 2}(am). X-ray absorption fine structure (XAFS) spectroscopy of the precipitates showed a substantially reduced Pu-Pu backscatter over that previously observed in {sup 239}PuO{sub 2}(am) precipitates, indicating that the {sup 242}PuO{sub 2}(am) precipitates purified using TTA lacked the long range order previously found in{sup 239}PuO{sub 2}(am) precipitates. The Pu(IV) stock solution was subsequently re-purified using an ion exchange resin and an additional series of {sup 242}PuO{sub 2}(am) precipitates prepared. These suspensions showed higher redox potentials and total aqueous Pu concentrations than the TTA purified stock solution. The higher redox potential and aqueous Pu concentrations were in general agreement with previous studies on {sup 242}PuO{sub 2}(am) precipitates, presumably due to the removal of possible organic compounds originally present in the TTA purified stock. {sup 242}PuO{sub 2}(am) suspensions prepared with both stock solutions showed almost identical solubilities in Fe(II) containing solutions even though the initial aqueous Pu concentrations before the addition of Fe(II) were orders of magnitude different. By examining the solubility of {sup 242}PuO{sub 2}(am) prepared from both stocks in this way we have essentially approached equilibrium from both the undersaturated and oversaturated conditions. The final aqueous Pu concentrations are predictable using a chemical equilibrium model which includes the

  10. Arctic Ocean sea ice drift origin derived from artificial radionuclides

    Energy Technology Data Exchange (ETDEWEB)

    Camara-Mor, P., E-mail: patricia.camara@uab.es [Institut de Ciencia i Tecnologia Ambientals, Universitat Autonoma de Barcelona, E-08193. Bellaterra (Spain); Masque, P. [Institut de Ciencia i Tecnologia Ambientals, Universitat Autonoma de Barcelona, E-08193. Bellaterra (Spain); Dpt. de Fisica, Universitat Autonoma de Barcelona, E-08193. Bellaterra (Spain); Garcia-Orellana, J. [Institut de Ciencia i Tecnologia Ambientals, Universitat Autonoma de Barcelona, E-08193. Bellaterra (Spain); Dpt. de Fisica, Universitat Autonoma de Barcelona, E-08193. Bellaterra (Spain); School of Marine and Atmospheric Sciences, Stony Brook University, Stony Brook, NY 11794-5000 (United States); Cochran, J.K. [School of Marine and Atmospheric Sciences, Stony Brook University, Stony Brook, NY 11794-5000 (United States); Mas, J.L. [Dpto. de Fisica Aplicada, Universidad de Sevilla, 41012, Seville. Spain (Spain); Chamizo, E. [Centro Nacional de Aceleradores (CNA), Avd. Thomas Alva Edison 7, Isla de la Cartuja, E-41092, Seville (Spain); Hanfland, C. [Alfred Wegener Institute for Polar and Marine Research, Am Handelshafen 12, D-27570 Bremerhaven (Germany)

    2010-07-15

    Since the 1950s, nuclear weapon testing and releases from the nuclear industry have introduced anthropogenic radionuclides into the sea, and in many instances their ultimate fate are the bottom sediments. The Arctic Ocean is one of the most polluted in this respect, because, in addition to global fallout, it is impacted by regional fallout from nuclear weapon testing, and indirectly by releases from nuclear reprocessing facilities and nuclear accidents. Sea-ice formed in the shallow continental shelves incorporate sediments with variable concentrations of anthropogenic radionuclides that are transported through the Arctic Ocean and are finally released in the melting areas. In this work, we present the results of anthropogenic radionuclide analyses of sea-ice sediments (SIS) collected on five cruises from different Arctic regions and combine them with a database including prior measurements of these radionuclides in SIS. The distribution of {sup 137}Cs and {sup 239,240}Pu activities and the {sup 240}Pu/{sup 239}Pu atom ratio in SIS showed geographical differences, in agreement with the two main sea ice drift patterns derived from the mean field of sea-ice motion, the Transpolar Drift and Beaufort Gyre, with the Fram Strait as the main ablation area. A direct comparison of data measured in SIS samples against those reported for the potential source regions permits identification of the regions from which sea ice incorporates sediments. The {sup 240}Pu/{sup 239}Pu atom ratio in SIS may be used to discern the origin of sea ice from the Kara-Laptev Sea and the Alaskan shelf. However, if the {sup 240}Pu/{sup 239}Pu atom ratio is similar to global fallout, it does not provide a unique diagnostic indicator of the source area, and in such cases, the source of SIS can be constrained with a combination of the {sup 137}Cs and {sup 239,240}Pu activities. Therefore, these anthropogenic radionuclides can be used in many instances to determine the geographical source area of sea-ice.

  11. Calculation of Pseudo Fission-product Data for Fast Reactor%快堆伪裂变产物数据的计算

    Institute of Scientific and Technical Information of China (English)

    刘廷进; 刘萍

    2002-01-01

    从微观评价核数据库出发,计算给出了快堆谱的伪裂变产物数据,包括一群的截面数据和多群的全套中子数据,裂变核有235U和239Pu.截面数据有全截面、弹性散射、非弹散射、(n,γ)、(n,2n)截面,多群全套中子数据还包括次级中子角分布和能谱.数据以ENDF/B-6格式给出,同时还分析讨论了数据误差和可靠性,数据可用于实际的快堆计算.

  12. Atmospheric transport of radionuclides emitted due to wildfires near the Chernobyl Nuclear Power Plant in 2015

    Science.gov (United States)

    Evangeliou, Nikolaos; Zibtsev, Sergey; Myroniuk, Viktor; Zhurba, Marina; Hamburger, Thomas; Stohl, Andreas; Balkanski, Yves; Paugam, Ronan; Mousseau, Timothy A.; Møller, Anders P.; Kireev, Sergey I.

    2016-04-01

    In 2015, two major fires in the Chernobyl Exclusion Zone (CEZ) have caused concerns about the secondary radioactive contamination that might have spread over Europe. The total active burned area was estimated to be about 15,000 hectares, of which 9000 hectares burned in April and 6000 hectares in August. The present paper aims to assess, for the first time, the transport and impact of these fires over Europe. For this reason, direct observations of the prevailing deposition levels of 137Cs and 90Sr, 238Pu, 239Pu, 240Pu and 241Am in the CEZ were processed together with burned area estimates. Based on literature reports, we made the conservative assumption that 20% of the deposited labile radionuclides 137Cs and 90Sr, and 10% of the more refractory 238Pu, 239Pu, 240Pu and 241Am, were resuspended by the fires. We estimate that about 10.9 TBq of 137Cs, 1.5 TBq of 90Sr, 7.8 GBq of 238Pu, 6.3 GBq of 239Pu, 9.4 GBq of 240Pu and 29.7 GBq of 241Am were released from both fire events. These releases could be classified as of "Level 3" on the relative INES (International Nuclear Events Scale) scale, which corresponds to a serious incident, in which non-lethal deterministic effects are expected from radiation. To simulate the dispersion of the resuspended radionuclides in the atmosphere and their deposition onto the terrestrial environment, we used a Lagrangian dispersion model. Spring fires redistributed radionuclides over the northern and eastern parts of Europe, while the summer fires also affected Central and Southern Europe. The more labile elements escaped more easily from the CEZ and then reached and deposited in areas far from the source, whereas the larger refractory particles were removed more efficiently from the atmosphere and thus did mainly affect the CEZ and its vicinity. For the spring 2015 fires, we estimate that about 80% of 137Cs and 90Sr and about 69% of 238Pu, 239Pu, 240Pu and 241Am were deposited over areas outside the CEZ. 93% of the labile and 97% of

  13. Even–odd effects in prompt emission of spontaneously fissioning even–even Pu isotopes

    Energy Technology Data Exchange (ETDEWEB)

    Tudora, A., E-mail: anabellatudora@hotmail.com [University of Bucharest, Faculty of Physics, Bucharest Magurele, POB MG-11, R-76900 (Romania); Hambsch, F.-J. [EC-JRC Institute for Reference Materials and Measurements (IRMM), Retieseweg 111, B-2440, Geel (Belgium); Giubega, G.; Visan, I. [University of Bucharest, Faculty of Physics, Bucharest Magurele, POB MG-11, R-76900 (Romania)

    2015-01-15

    The available experimental Y(A,TKE) data for {sup 236,238,240,242,244}Pu(SF) together with the Zp model prescription with appropriate parameters allows the investigation of even–odd effects in fragment distributions. The size of the global even–odd effect in Y(Z) is decreasing from {sup 244}Pu(SF) to {sup 236}Pu(SF) confirming the general observation of a decrease of the even–odd effect with the fissility parameter. Charge polarizations (ΔZ) and root-mean squares (rms) as a function of A of {sup 236–244}Pu(SF) were obtained for the first time. In the asymmetric fission region both ΔZ(A) and rms(A) exhibit oscillations with a periodicity of about 5 mass units due to the even–odd effects. The total average charge deviations 〈ΔZ〉 (obtained by averaging ΔZ(A) over the experimental Y(A) distribution) are of about |0.5| for all studied Pu(SF) systems. The comparison of the calculated ΔZ(A) and rms(A) of {sup 240}Pu(SF) with those of {sup 239}Pu(n{sub th},f) reported by Wahl shows an in-phase oscillation with a higher amplitude in the case of {sup 240}Pu(SF), confirming the higher even–odd effect in the case of SF. As in the previously studied cases ({sup 233,235}U(n{sub th},f), {sup 239}Pu(n{sub th},f), {sup 252}Cf(SF)) the even–odd effects in the prompt emission of {sup 236–244}Pu(SF) are mainly due to the Z even–odd effects in fragment distributions and charge polarizations and the N even–odd effects in the average neutron separation energies from fragments 〈Sn〉. The size of the global N even–odd effect in 〈Sn〉 is decreasing with the fissility parameter, being higher for the Pu(SF) systems compared to the previously studied systems. The prompt neutron multiplicities as a function of Z, ν(Z), exhibit sawtooth shapes with a visible staggering for asymmetric fragmentations. The size of the global Z even–odd effect in ν(Z) exhibits a decreasing trend with increasing fissility. The average prompt neutron multiplicities as a

  14. Manmade radionuclide vector in Austrian soil and vegetation near Temelin nuclear power plant

    Energy Technology Data Exchange (ETDEWEB)

    Sinojmeri, M.; Ringer, V. [Oesterreichische Agentur fuer Gesundheit und Ernaehrungssicherheit - AGES (Austria)

    2014-07-01

    Since Chernobyl NPP accident an environmental monitoring program concerning the Upper Austrian region near Czech Republic Nuclear Power Plant, NPP Temelin, is in progress between AGES and BMLFUV, the Austrian Federal Ministry of Agriculture, Forestry, Environment, Water and Food, in Austria. This paper presents the results obtained during the sampling campaign over biennial period of 2010-2011. Soil samples, grass and different cereal species were collected. Beside Cs-134, Cs-137 and Sr-89, Sr-90 isotopes, at this phase the number of isotopes determined was extended with plutonium isotopes Pu-238, Pu-239, Pu-240, Pu-241 and Am-241. A comparison of these results with the existing data so far is presented. New knowledge was obtained related the bio-kinetic parameters of these elements in the environment. Document available in abstract form only. (authors)

  15. Multigroup covariance matrices for fast-reactor studies

    Energy Technology Data Exchange (ETDEWEB)

    Smith, J.D. III; Broadhead, B.L.

    1981-04-01

    This report presents the multigroup covariance matrices based on the ENDF/B-V nuclear data evaluations. The materials and reactions have been chosen according to the specifications of ORNL-5517. Several cross section covariances, other than those specified by that report, are included due to the derived nature of the uncertainty files in ENDF/B-V. The materials represented are Ni, Cr, /sup 16/O, /sup 12/C, Fe, Na, /sup 235/U, /sup 238/U, /sup 239/Pu, /sup 240/Pu, /sup 241/Pu, and /sup 10/B (present due to its correlation to /sup 238/U). The data have been originally processed into a 52-group energy structure by PUFF-II and subsequently collapsed to smaller subgroup strutures. The results are illustrated in 52-group correlation matrix plots and tabulated into thirteen groups for convenience.

  16. Transport of radionuclides from the Mururoa and Fangataufa atolls through the marine environment

    Energy Technology Data Exchange (ETDEWEB)

    Mittelstaedt, E. [Bundesamt fuer Seeschiffahrt und Hydrographie, P.B. 301220, D-20305 Hamburg (Germany); Osvath, I.; Povinec, P.P.; Togawa, O. [International Atomic Energy Agency/Marine Environment Laboratory, 4 Quai Antoine 1er, B.P. 800, Monte Carlo (Monaco); Scott, E.M. [Department of Statistics, University of Glasgow, Glasgow (United Kingdom)

    1999-09-30

    The dispersion of radionuclides (3H, 90Sr, 137Cs, 239Pu) potentially released from the Mururoa and Fangataufa atolls through the South Pacific Ocean has been studied by means of computer models. The models used consisted of three differently structured compartmental models for the regional field and a hydrodynamic world ocean model for the far-field simulations. The outcome of regional modelling is predicted activity concentrations with time in different regions of French Polynesia (over up to 10000 years for plutonium). The far-field model simulates large-scale dispersion in the South Pacific Ocean over periods of up to 50 years. The overall result suggests that there will not be radioactive contamination of any radiological interest at inhabited sites in French Polynesia or anywhere else in the ocean at present or in the future.

  17. Pu and Am determination in the environment—method development

    Science.gov (United States)

    Afonin, M.; Simonoff, M.; Donard, O.; Michel, H.; Ardisson, G.

    2003-01-01

    A high resolution inductively coupled plasma mass spectrometric (HR-ICP-MS) method for the determination of plutonium isotopes, Am and the 240Pu/239Pu isotope ratio utilising modification of Pu-02-RC Plutonium in Soil Samples, Pu-03-RC Plutonium in Soil Residue—Total Dissolution Method, Pu-11-RC Plutonium Purification—Ion Exchange Technique, Pu-12-RC Plutonium and/or Americium in Soil or Sediments, HASL-300 was developed. Total plutonium concentrations (239+240Pu) measured in environmental samples by this HR-ICP-MS method were in good agreement with recommended data obtained from a-spectrometry. It was achieved the decreasing of the time to analyze the samples over than 33%.

  18. Novel Scintillation Detectors for Prompt Fission γ-Ray Measurements

    Science.gov (United States)

    Billnert, R.; Andreotti, E.; Hambsch, F.-J.; Hult, M.; Karlsson, J.; Marissens, G.; Oberstedt, A.; Oberstedt, S.

    In this work we present first results from measurements of prompt fission γ-rays from the spontaneous fission in 252Cf. New and accurate data on corresponding γ-rays from the reactions 235U(nth,f) and 239Pu(nth,f) are highly demanded for the modeling of new Generation-IV nuclear reactor systems. For these experiments we employed scintillation detectors made out of new materials (LaBr3, LaCl3 and CeBr3), whose properties were necessary to know in order to obtain reliable results. Hence, we have characterized these detectors. In all the important properties these detectors outshine sodium-iodine detectors that where used in the 1970s, when the existing data had been acquired. Our finding is that the new generation of scintillation detectors is indeed promising, as far as an improved precision of the demanded data is concerned.

  19. Precise determination of the 235U reactor antineutrino cross section per fission

    Science.gov (United States)

    Giunti, C.

    2017-01-01

    We investigate which among the reactor antineutrino fluxes from the decays of the fission products of 235U, 238U, 239Pu, and 241Pu may be responsible for the reactor antineutrino anomaly if the anomaly is due to a miscalculation of the antineutrino fluxes. We find that it is very likely that at least the calculation of the 235U flux must be revised. From the fit of the data we obtain the precise determination σ235 = (6.33 ± 0.08) ×10-43cm2 /fission of the 235U cross section per fission, which is more precise than the calculated value and differs from it by 2.2σ. The cross sections per fission of the other fluxes have large uncertainties and in practice their values are undetermined by the fit.

  20. A new MC-based method to evaluate the fission fraction uncertainty at reactor neutrino experiment

    CERN Document Server

    Ma, X B; Chen, Y X

    2016-01-01

    Uncertainties of fission fraction is an important uncertainty source for the antineutrino flux prediction in a reactor antineutrino experiment. A new MC-based method of evaluating the covariance coefficients between isotopes was proposed. It was found that the covariance coefficients will varying with reactor burnup and which may change from positive to negative because of fissioning balance effect, for example, the covariance coefficient between $^{235}$U and $^{239}$Pu changes from 0.15 to -0.13. Using the equation between fission fraction and atomic density, the consistent of uncertainty of fission fraction and the covariance matrix were obtained. The antineutrino flux uncertainty is 0.55\\% which does not vary with reactor burnup, and the new value is about 8.3\\% smaller.

  1. Active detection of shielded SNM with 60-keV neutrons

    Energy Technology Data Exchange (ETDEWEB)

    Hagmann, C; Dietrich, D; Hall, J; Kerr, P; Nakae, L; Newby, R; Rowland, M; Snyderman, N; Stoeffl, W

    2008-07-08

    Fissile materials, e.g. {sup 235}U and {sup 239}Pu, can be detected non-invasively by active neutron interrogation. A unique characteristic of fissile material exposed to neutrons is the prompt emission of high-energy (fast) fission neutrons. One promising mode of operation subjects the object to a beam of medium-energy (epithermal) neutrons, generated by a proton beam impinging on a Li target. The emergence of fast secondary neutrons then clearly indicates the presence of fissile material. Our interrogation system comprises a low-dose 60-keV neutron generator (5 x 10{sup 6}/s), and a 1 m{sup 2} array of scintillators for fast neutron detection. Preliminary experimental results demonstrate the detectability of small quantities (370 g) of HEU shielded by steel (200 g/cm{sup 2}) or plywood (30 g/cm{sup 2}), with a typical measurement time of 1 min.

  2. CRITICALITY CURVES FOR PLUTONIUM HYDRAULIC FLUID MIXTURES

    Energy Technology Data Exchange (ETDEWEB)

    WITTEKIND WD

    2007-10-03

    This Calculation Note performs and documents MCNP criticality calculations for plutonium (100% {sup 239}Pu) hydraulic fluid mixtures. Spherical geometry was used for these generalized criticality safety calculations and three geometries of neutron reflection are: {sm_bullet}bare, {sm_bullet}1 inch of hydraulic fluid, or {sm_bullet}12 inches of hydraulic fluid. This document shows the critical volume and critical mass for various concentrations of plutonium in hydraulic fluid. Between 1 and 2 gallons of hydraulic fluid were discovered in the bottom of HA-23S. This HA-23S hydraulic fluid was reported by engineering to be Fyrquel 220. The hydraulic fluid in GLovebox HA-23S is Fyrquel 220 which contains phosphorus. Critical spherical geometry in air is calculated with 0 in., 1 in., or 12 inches hydraulic fluid reflection.

  3. Characteristics of the magnetic analysis system for a compact MPR-type spectrometer

    Institute of Scientific and Technical Information of China (English)

    QI Jian-Min; ZHOU Lin; JIANG Shi-Lun; PENG Tai-Ping

    2010-01-01

    The magnetic proton recoil(MPR)spectrometer is a novel diagnostic instrument with high perfor-mance for measurements of neutron spectra in inertial confinement fusion(ICF)experiments and high power fusion devices.A compact MPR-type spectrometer dedicated to the research of pulsed deuterium-tritium(DT)neutron spectroscopy of special experimental conditions is currently under design.Analyses of the main parameters and performance of the magnetic analysis system through 3-D particle transport calculations and MonteCarlo simulations and calibration of the system performance as a test using CR-39 solid track detector and α particle from 239pu and 226Ra radioactive sources are presented in this paper.The results indicate that the magnetic analysis system will achieve a detection efficiency level of 10-5-10-4 at an energy resolution of 1.5%-2.1%,and fulfills the design goals of the spectrometer.

  4. Rapid Determination of Plutonium Isotopes in Environmental Samples Using Sequential Injection Extraction Chromatography and Detection by Inductively Coupled Plasma Mass Spectrometry

    DEFF Research Database (Denmark)

    Qiao, Jixin; Hou, Xiaolin; Roos, Per

    2009-01-01

    by detection of isolated analytes with inductively coupled plasma mass spectrometry (ICP-MS). The method has been devised for the determination of Pu isotopes at environmentally relevant concentrations, whereby it has been successfully applied to the analyses of large volumes/amounts of samples, for example......This article presents an automated method for the rapid determination of 239Pu and 240Pu in various environmental samples. The analytical method involves the in-line separation of Pu isotopes using extraction chromatography (TEVA) implemented in a sequential injection (SI) network followed....... The analytical results of Pu isotopes in the reference materials showed good agreement with the certified or reference values at the 0.05 significance level. Chemical yields of Pu ranged from 80 to 105%, and the decontamination factors for uranium, thorium, mercury and lead were all above 104. The duration...

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

    Energy Technology Data Exchange (ETDEWEB)

    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.

  6. Benchmark experiment for physics parameters of metallic-fueled LMFBR at FCA

    Energy Technology Data Exchange (ETDEWEB)

    Iijima, S.; Oigawa, H.; Sakurai, T.; Nemoto, T.; Okajima, S. [Japan Atomic Energy Research Inst., Tokai, Ibaraki (Japan). Tokai Research Establishment

    1996-09-01

    The calculated prediction for reactor physics parameters in a metallic-fueled LMFBR was tested using the benchmark experiments performed at FCA. The reactivity feedback parameters such as sodium void worth, Doppler reactivity worth and {sup 238}U-capture-to-{sup 239}Pu -fission ratio have been measured. The fuel expansion reactivity has also measured. Direct comparison with the results from similar oxide fuel assembly was made. Analysis was done with the JENDL-2 cross section library and JENDL-3.2. Prediction of reactor physics parameters with JENDL-3.2 in the metallic-fueled core agreed reasonably well with the measured values and showed similar trend to the results in the oxide fuel core. (author)

  7. Spectrometry and dosimetry of a neutron source

    Energy Technology Data Exchange (ETDEWEB)

    Vega C, H.R.; Manzanares A, E.; Hernandez D, V.M.; Ramirez G, J.; Hernandez V, R.; Chacon R, A. [Universidad Autonoma de Zacatecas, 98068 Zacatecas (Mexico)]. e-mail: fermineutron@yahoo.com

    2007-07-01

    Using Monte Carlo methods the spectrum, dose equivalent and ambient dose equivalent of a {sup 239}PuBe at several distances has been determined. Spectrum and both doses, at 100 cm, were determined-experimentally using a Bonner sphere spectrometer. These quantities were obtained by unfolding the spectrometer count rates using artificial neural networks. The dose equivalent, based in the ICRP 21 criteria, was measured with the area neutron dosemeter Eberline model NRI), at 100, 200 and 300 cm. All measurements were carried out in an open space to avoid the room return. With these results it was found that this source has a yield of 8.41E(6) n/s. (Author)

  8. A large area position-sensitive ionization chamber for heavy-ion-induced reaction studies

    Energy Technology Data Exchange (ETDEWEB)

    Pant, L.M. E-mail: lalit.pant@exp2.physik.uni-giessen.de; Biswas, D.C.; Dinesh, B.V.; Thomas, R.G.; Saxena, A.; Sawant, Y.S.; Choudhury, R.K

    2002-12-11

    A large area position-sensitive ionization chamber with a wide dynamic range has been developed to measure the mass, charge and energy of the heavy ions and the fission fragments produced in heavy-ion-induced reactions. The split anode geometry of the detector makes it suitable for both particle identification and energy measurements for heavy ions and fission fragments. The detector has been tested with {alpha} particles from {sup 241}Am-{sup 239}Pu source, fission fragments from {sup 252}Cf and the heavy-ion beams from the 14UD Mumbai Pelletron accelerator facility. Using this detector, measurements on mass and total kinetic energy distributions in heavy-ion-induced fusion-fission reactions have been carried out for a wide range of excitation energies. Results on deep inelastic collisions and mass-energy correlations on different systems using this detector setup are discussed.

  9. Sequential Injection Method for Rapid and Simultaneous Determination of 236U, 237Np, and Pu Isotopes in Seawater

    DEFF Research Database (Denmark)

    Qiao, Jixin; Hou, Xiaolin; Steier, Peter;

    2013-01-01

    An automated analytical method implemented in a novel dual-column tandem sequential injection (SI) system was developed for simultaneous determination of 236U, 237Np, 239Pu, and 240Pu in seawater samples. A combination of TEVA and UTEVA extraction chromatography was exploited to separate and purify...... target analytes, whereupon plutonium and neptunium were simultaneously isolated and purified on TEVA, while uranium was collected on UTEVA. The separation behavior of U, Np, and Pu on TEVA–UTEVA columns was investigated in detail in order to achieve high chemical yields and complete purification...... for the radionuclides of interest. 242Pu was used as a chemical yield tracer for both plutonium and neptunium. 238U was quantified in the sample before the separation for deducing the 236U concentration from the measured 236U/238U atomic ratio in the separated uranium target using accelerator mass spectrometry...

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

    Energy Technology Data Exchange (ETDEWEB)

    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.

  11. Cyclin D expression in plutonium-induced lung tumors in F344 rats

    Energy Technology Data Exchange (ETDEWEB)

    Hahn, F.F.; Kelly, G. [SouthWest Scientific Resources, Inc., Albuquerque, NM (United States)

    1995-12-01

    The genetic mechanisms responsible for {alpha}-radiation-induced lung cancer in rats following inhalation of {sup 239}Pu is an ongoing area of research in our laboratory. Previous studies have examined the status of the p53 gene by immunohistochemistry. Only two tumors (2/26 squamous cell carcinomas) exhibited detectable levels of p53 products. Both were the result of mutations in codons 280 and 283. More recent studies of X-ray-induced lung tumors in rats showed a similar lack of involvement of p53. In conclusion, we found that {alpha}-radiation-induced rat lung tumors have a high incidence (31 of 39) of cyclin D{sub 1} overexpression.

  12. Applications of Event-by-Event Fission Modeling with FREYA

    Directory of Open Access Journals (Sweden)

    Vogt R.

    2012-02-01

    Full Text Available The recently developed code FREYA (Fission Reaction Event Yield Algorithm generates large samples of complete fission events, consisting of two receding product nuclei as well as a number of neutrons and photons, all with complete kinematic information. Thus it is possible to calculate arbitrary correlation observables whose behavior may provide unique insight into the fission process. We first discuss the present status of FREYA, which has now been extended to include spontaneous fission. Concentrating on 239Pu(nth,f, 240Pu(sf and 252Cf(sf, we discuss the neutron multiplicity correlations, the dependence of the neutron energy spectrum on the neutron multiplicity, and the relationship between the fragment kinetic energy and the number of neutrons and their energies. We also suggest novel fission observables that could be measured with modern detectors.

  13. National Low-Level Waste Management Program Radionuclide Report Series

    Energy Technology Data Exchange (ETDEWEB)

    J.P. Adams; M.L. Carboneau; W.E. Allred

    1999-02-01

    The National Low Level Waste Management Program at the Idaho National Engineering and Environmental Laboratory has published a report containing key information about selected radionuclides that are most likely to contribute significantly to the radiation exposures estimated from a performance assessment of a low-level radioactive waste (LLW) disposal facility. The information includes physical and chemical characteristics, production means, waste forms, behavior of the radionuclide in soils, plants, groundwater, and air, and biological effects in animals and humans. The radionuclides included in this study comprise all of the nuclides specifically listed in 10CFR61.55, Tables 1 and 2, 3 H, 14 C, 59 Ni, 60 Co, 63 Ni, 90 Sr, 94 Nb, 99 Tc, 129 I, 137 Cs, 241 Pu, and 242 Cm. Other key radionuclides addressed in the report include 237 Np, 238 U, 239 Pu, and 241 Am. This paper summarizes key information contained within this report.

  14. National Low-Level Waste Management Program Radionuclide Report Series

    Energy Technology Data Exchange (ETDEWEB)

    Adams, James Paul; Carboneau, Michael Leonard; Allred, William Edgar

    1999-03-01

    The National Low Level Waste Management Program at the Idaho National Engineering and Environmental Laboratory has published a report containing key information about selected radionuclides that are most likely to contribute significantly to the radiation exposures estimated from a performance assessment of a low-level radioactive waste (LLW) disposal facility. The information includes physical and chemical characteristics, production means, waste forms, behavior of the radionuclide in soils, plants, groundwater, and air, and biological effects in animals and humans. The radionuclides included in this study comprise all of the nuclides specifically listed in 10CFR61.55, Tables 1 and 2, 3 H, 14 C, 59 Ni, 60 Co, 63 Ni, 90 Sr, 94 Nb, 99 Tc, 129 I, 137 Cs, 241 Pu, and 242 Cm. Other key radionuclides addressed in the report include 237 Np, 238 U, 239 Pu, and 241 Am. This paper summarizes key information contained within this report.

  15. Standard test method for nondestructive assay of special nuclear material holdup using Gamma-Ray spectroscopic methods

    CERN Document Server

    American Society for Testing and Materials. Philadelphia

    2007-01-01

    1.1 This test method describes gamma-ray methods used to nondestructively measure the quantity of 235U, or 239Pu remaining as holdup in nuclear facilities. Holdup occurs in all facilities where nuclear material is processed, in process equipment, in exhaust ventilation systems and in building walls and floors. 1.2 This test method includes information useful for management, planning, selection of equipment, consideration of interferences, measurement program definition, and the utilization of resources (1, 2, 3, 4). 1.3 The measurement of nuclear material hold up in process equipment requires a scientific knowledge of radiation sources and detectors, transmission of radiation, calibration, facility operations and error analysis. It is subject to the constraints of the facility, management, budget, and schedule; plus health and safety requirements; as well as the laws of physics. The measurement process includes defining measurement uncertainties and is sensitive to the form and distribution of the material...

  16. Special nuclear material detection with a mobile multi-detector system

    Energy Technology Data Exchange (ETDEWEB)

    Cester, D. [Dipartimento di Fisica, Universita di Padova, Via Marzolo 8, I-35131 Padova (Italy); Nebbia, G. [INFN Sezione di Padova, Via Marzolo 8, I-35131 Padova (Italy); Stevanato, L. [Dipartimento di Fisica, Universita di Padova, Via Marzolo 8, I-35131 Padova (Italy); INFN Sezione di Padova, Via Marzolo 8, I-35131 Padova (Italy); Viesti, G, E-mail: viesti@pd.infn.it [Dipartimento di Fisica, Universita di Padova, Via Marzolo 8, I-35131 Padova (Italy); INFN Sezione di Padova, Via Marzolo 8, I-35131 Padova (Italy); Neri, F.; Petrucci, S.; Selmi, S.; Tintori, C. [CAEN S.p.A., Via Vetraia 11, I-55049 Viareggio (Italy); Peerani, P.; Tomanin, A. [European Commission EC-JRC-ITU, I-21027 Ispra (Italy)

    2012-01-21

    The detection of special nuclear material has been studied with a mobile inspection system used both as a high sensitivity passive neutron/gamma spectroscopic tool and as an active inspection device using tagged neutrons. The detection of plutonium samples seems to be possible with passive interrogation, even for small samples, thanks to the yield of gamma ray and neutrons. Moreover the gamma ray spectrum shows clear signatures related to {sup 239}Pu. The passive detection of uranium is much more difficult because of the low neutron yield and of the easiness of shielding the gamma ray yield of highly enriched U samples. However, we show that active interrogation with tagged neutrons is able to provide signatures for the discrimination of uranium against other heavy metals.

  17. Special nuclear material detection with a mobile multi-detector system

    Science.gov (United States)

    Cester, D.; Nebbia, G.; Stevanato, L.; Viesti, G.; Neri, F.; Petrucci, S.; Selmi, S.; Tintori, C.; Peerani, P.; Tomanin, A.

    2012-01-01

    The detection of special nuclear material has been studied with a mobile inspection system used both as a high sensitivity passive neutron/gamma spectroscopic tool and as an active inspection device using tagged neutrons. The detection of plutonium samples seems to be possible with passive interrogation, even for small samples, thanks to the yield of gamma ray and neutrons. Moreover the gamma ray spectrum shows clear signatures related to 239Pu. The passive detection of uranium is much more difficult because of the low neutron yield and of the easiness of shielding the gamma ray yield of highly enriched U samples. However, we show that active interrogation with tagged neutrons is able to provide signatures for the discrimination of uranium against other heavy metals.

  18. The design and implementation of the AVNG measurement system

    Energy Technology Data Exchange (ETDEWEB)

    Macarthur, Duncan W [Los Alamos National Laboratory; Thron, Jonathan [Los Alamos National Laboratory; Razinkov, Sergey [RFNC-VNIIEF; Livke, Alexander [RFNC-VNIIEF; Kondratov, Sergey [RFNC-VNIIEF

    2010-01-01

    An attribute measurement system (AMS) measures a number of unclassified attributes of potentially classified material. By displaying these unclassified results only as red or green lights, the AMS protects potentially classified information while still generating confidence in the measurement result. The AVNG that we describe is an AMS built by RFNC-VNIIEF in Sarov, Russia. The AVNG detects neutron and gamma radiation signatures and displays the three unclassified attributes of 'plutonium presence,' 'plutonium mass >2 kg,' and 'plutonium isotopic ratio ({sup 240}Pu to {sup 239}Pu) < 0.1.' In this presentation, we will describe the design of the AVNG neutron and gamma detector subsystems, as well as the design of the entire AMS incorporating these detectors. We will also describe the construction of the AVNG and the final design that was demonstrated in June 2009.

  19. Effect of microorganisms on the plutonium oxidation states

    Energy Technology Data Exchange (ETDEWEB)

    Luksiene, Benedikta, E-mail: bena@ar.fi.lt [Center for Physical Sciences and Technology, Savanoriu ave 231, LT-02300 Vilnius (Lithuania); Druteikiene, Ruta [Center for Physical Sciences and Technology, Savanoriu ave 231, LT-02300 Vilnius (Lithuania); Peciulyte, Dalia [Nature Research Centre, Akademijos street 2, LT-08412 Vilnius (Lithuania); Baltrunas, Dalis; Remeikis, Vidmantas [Center for Physical Sciences and Technology, Savanoriu ave 231, LT-02300 Vilnius (Lithuania); Paskevicius, Algimantas [Nature Research Centre, Akademijos street 2, LT-08412 Vilnius (Lithuania)

    2012-03-15

    Particular microbes from substrates at the low-level radioactive waste repository in the Ignalina NPP territory were exposed to {sup 239}Pu (IV) at low pH under aerobic conditions. Pu(III) and Pu(IV) were separated and quantitatively evaluated using the modified anion exchange method and alpha spectrometry. Tested bacteria Bacillus mycoides and Serratia marcescens were more effective in Pu reduction than Rhodococcus fascians. Fungi Paecillomyces lilacinus and Absidia spinosa var. spinosa as well as bacterium Rhodococcus fascians did not alter the plutonium oxidation state. - Highlights: Black-Right-Pointing-Pointer Particular microbes from low-level radioactive waste repository were exposed to Pu (IV). Black-Right-Pointing-Pointer Some tested bacteria induced slight Pu (IV) reduction at low pH under aerobic conditions. Black-Right-Pointing-Pointer Tested fungi did not show peculiarities to alter Pu oxidation state. Black-Right-Pointing-Pointer The modified radiochemical method was applied to differentiate Pu oxidation states.

  20. Sequestration of radioactive iodine in silver-palladium phases in commercial spent nuclear fuel

    Energy Technology Data Exchange (ETDEWEB)

    Buck, Edgar C.; Mausolf, Edward J.; McNamara, Bruce K.; Soderquist, Chuck Z.; Schwantes, Jon M.

    2016-12-01

    Radioactive iodine is the Achilles’ heel in the design for the safe geological disposal of spent UO2 nuclear fuel. Iodine’s high solubility and anticipated instant release during waste package compromise jeopardize performance assessment calculations. However, dissolution studies have indicated that the instant release fraction (IRF) of radioiodine (I) does not correlate with increasing fuel burn-up. In fact, there is a peak in the release iodine at around 50-60 Mwd/kgU and with increasing burn-up the instant release of iodine decreases. Detailed electron microscopy analysis of high burn-up fuel (~80 MWd/kgU) has revealed the presence of (Pd,Ag)(I,Br) nano-particles. As UO2 fuels are irradiated, the Ag and Pd content increases, from 239Pu fission, enabling radioiodine to be retained. The occurrence of these phases in nuclear fuels may have significant implications for the long-term behavior of iodine.

  1. Evolving Density and Static Mechanical Properties in Plutonium from Self-Irradiation

    Energy Technology Data Exchange (ETDEWEB)

    Chung, B W; Thompson, S R; Lema, K E; Hiromoto, D S; Ebbinghaus, B B

    2008-07-31

    Plutonium, because of its self-irradiation by alpha decay, ages by means of lattice damage and helium in-growth. These integrated aging effects result in microstructural and physical property changes. Because these effects would normally require decades to measure, studies are underway to assess the effects of extended aging on the physical properties of plutonium alloys by incorporating roughly 7.5 weight % of highly specific activity isotope {sup 238}Pu into the {sup 239}Pu metal to accelerate the aging process. This paper presents updated results of self-irradiation effects on {sup 238}Pu-enriched alloys measured by immersion density, dilatometry, and tensile tests. After nearly 90 equivalent years of aging, both the immersion density and dilatometry show that the enriched alloys continue to decreased in density by {approx}0.002% per year, without void swelling. Quasi-static tensile measurements show that the aging process increases the strength of plutonium alloys.

  2. Average Neutron Total Cross Sections in the Unresolved Energy Range From ORELA High Resolutio Transmission Measurements

    Energy Technology Data Exchange (ETDEWEB)

    Derrien, H

    2004-05-27

    Average values of the neutron total cross sections of {sup 233}U, {sup 235}U, {sup 238}U, and {sup 239}Pu have been obtained in the unresolved resonance energy range from high-resolution transmission measurements performed at ORELA in the past two decades. The cross sections were generated by correcting the effective total cross sections for the self-shielding effects due to the resonance structure of the data. The self-shielding factors were found by calculating the effective and true cross sections with the computer code SAMMY for the same Doppler and resolution conditions as for the transmission measurements, using an appropriate set of resonance parameters. Our results are compared to results of previous measurements and to the current ENDF/B-VI data.

  3. World must build two atomic reactors each day the next hundred years. [Summary of and commentary on book, 'Mankind at the Turning Point'

    Energy Technology Data Exchange (ETDEWEB)

    1974-07-24

    In summarizing and commenting on the ideas presented in Mesarovic and Pestel's book ''Mankind at the Turning Point'' it is pointed out that the global energy crisis makes comprehensive long-term planning a necessity. Assuming, optimistically, that nuclear power alone is able to supply the total projected energy demand in 100 years, it is stated that this will require 3000 nuclear power stations, each with 8 fast breeder reactors, totally 100 GW(t). This means a net rate of construction of four reactors per week, which again means allowing for a 30-year life, two reactors per day, every day, for the next hundred years. Fueling of these reactors will require the production and transport of 15 x 10/sup 6/ kg of /sup 239/Pu per year. It is therefore obvious that the energy crisis is not only a technological, but also a political, social, and even psychological problem.

  4. Feasibility of Burning Civilian Grade Pu in the Modular HTR with Th Fuel Cycle

    Institute of Scientific and Technical Information of China (English)

    许云林; 经荥清

    2001-01-01

    The Modular High Temperature Gas-Cooled Reactor (HTR) can be usedto burn plutonium fuel to reduce Pu stockpiles because of its inherent safety characteristics and ability to burn a variety of fuel mixtures. The equilibrium core is calculated and analyzed for Pu enriched fuel. Fuel spheres with 7 g heavy metal including the civilian grade Pu and thorium are loaded into the reactor. An enrichment of 11% is chosen to provide the desired equilibrium core reactivity. The fuel and moderator temperature coefficients are both negative. The maximum fuel element temperature during normal operation and during a loss of coolant accident is less than 1500 ℃. 92% of 239Pu will be burnt during nomal operation. Therefore, a thorium fuel cycle in the modular HTR is an effective method for burning civilian grade plutonium.

  5. Plutonium in the marine environment at Thule, NW-Greenland after a nuclear weapons accident

    DEFF Research Database (Denmark)

    Dahlgaard, H.; Eriksson, M.; Ilus, E.

    2001-01-01

    In January 1968, a B52 plane carrying 4 nuclear weapon!: crashed on the sea ice similar to 12 km from the Thule Air Base, in northwest Greenland. The benthic marine environment in the 180-230 m deep Bylot Sound was then contaminated with similar to1.4 TBq Pu-239,Pu-240 (similar to0.5 kg). The site...... than in sediments. Some biota groups show a somewhat higher uptake of americium than of plutonium. Sediment samples with weapons plutonium from the accident show a significant variation in Pu-240/Pu-239 atom ratios in the range 0.027-0.057. This supports the hypothesis that the Thule plutonium...

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

    Energy Technology Data Exchange (ETDEWEB)

    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)

  7. Uranium from German nuclear power projects of the 1940s - a nuclear forensic investigation

    Energy Technology Data Exchange (ETDEWEB)

    Mayer, Klaus; Wallenius, Maria; Luetzenkirchen, Klaus; Horta, Joan; Nicholl, Adrian; Rasmussen, Gert; Belle, Pieter van; Varga, Zsolt [European Commission, Joint Research Centre (JRC), Institute for Transuranium Elements (ITU), Karlsruhe (Germany); Buda, Razvan; Erdmann, Nicole [European Commission, Joint Research Centre (JRC), Institute for Transuranium Elements (ITU), Karlsruhe (Germany); Institut fuer Kernchemie, Universitaet Mainz (Germany); Kratz, Jens-Volker; Trautmann, Norbert [Institut fuer Kernchemie, Universitaet Mainz (Germany); Fifield, L. Keith; Tims, Stephen G. [Department of Nuclear Physics, Research School of Physics and Engineering, The Australian National University, Canberra, ACT (Australia); Froehlich, Michaela B. [Department of Nuclear Physics, Research School of Physics and Engineering, The Australian National University, Canberra, ACT (Australia); Universitaet Wien, Fakultaet fuer Chemie, Institut fuer Anorganische Chemie, Vienna (Austria); Steier, Peter [Universitaet Wien, Fakultaet fuer Physik, Isotopenforschung und Kernphysik, Vienna (Austria)

    2015-11-02

    Here we present a nuclear forensic study of uranium from German nuclear projects which used different geometries of metallic uranium fuel. Through measurement of the {sup 230}Th/{sup 234}U ratio, we could determine that the material had been produced in the period from 1940 to 1943. To determine the geographical origin of the uranium, the rare-earth-element content and the {sup 87}Sr/{sup 86}Sr ratio were measured. The results provide evidence that the uranium was mined in the Czech Republic. Trace amounts of {sup 236}U and {sup 239}Pu were detected at the level of their natural abundance, which indicates that the uranium fuel was not exposed to any major neutron fluence. (copyright 2015 WILEY-VCH Verlag GmbH and Co. KGaA, Weinheim)

  8. Tank 241-AX-103, cores 212 and 214 analytical results for the final report

    Energy Technology Data Exchange (ETDEWEB)

    Steen, F.H.

    1998-02-05

    This document is the analytical laboratory report for tank 241-AX-103 push mode core segments collected between July 30, 1997 and August 11, 1997. The segments were subsampled and analyzed in accordance with the Tank 241-AX-103 Push Mode Core Sampling and Analysis Plan (TSAP) (Comer, 1997), the Safety Screening Data Quality Objective (DQO) (Dukelow, et al., 1995) and the Data Quality Objective to Support Resolution of the Organic Complexant Safety Issue (Organic DQO) (Turner, et al., 1995). The analytical results are included in the data summary table (Table 1). None of the samples submitted for Differential Scanning Calorimetry (DSC), Total Alpha Activity (AT), plutonium 239 (Pu239), and Total Organic Carbon (TOC) exceeded notification limits as stated in the TSAP (Conner, 1997). The statistical results of the 95% confidence interval on the mean calculations are provided by the Tank Waste Remediation Systems Technical Basis Group in accordance with the Memorandum of Understanding (Schreiber, 1997) and not considered in this report.

  9. Precision spectroscopy with reactor anti-neutrinos

    CERN Document Server

    Huber, P; Huber, Patrick; Schwetz, Thomas

    2004-01-01

    In this work we present an accurate parameterization of the anti-neutrino flux produced by the isotopes 235U, 239Pu and 241Pu in nuclear reactors. We determine the coefficients of this parameterization, as well as their covariance matrix, by performing a fit to spectra inferred from experimentally measured beta spectra. Subsequently we show that flux shape uncertainties play only a minor role in the KamLAND experiment, however, we find that future reactor neutrino experiments to measure the mixing angle $\\theta_{13}$ are sensitive to the fine details of the reactor neutrino spectra. Finally, we investigate the possibility to determine the isotopic composition in nuclear reactors through an anti-neutrino measurement. We find that with a 3 month exposure of a one ton detector the isotope fractions and the thermal reactor power can be determined at a few percent accuracy, which may open the possibility of an application for safeguard or non-proliferation objectives.

  10. Characteristics of a lead slowing-down spectrometer coupled to the LANSCE accelerator

    Energy Technology Data Exchange (ETDEWEB)

    Rochman, D. [LANSCE-3, Los Alamos National Laboratory, MS H855, Los Alamos, NM 87545 (United States)]. E-mail: drochman@bnl.gov; Haight, R.C. [LANSCE-3, Los Alamos National Laboratory, MS H855, Los Alamos, NM 87545 (United States)]. E-mail: haight@lanl.gov; O' Donnell, J.M. [LANSCE-3, Los Alamos National Laboratory, MS H855, Los Alamos, NM 87545 (United States)]. E-mail: odonnell@lanl.gov; Michaudon, A. [LANSCE-3, Los Alamos National Laboratory, MS H855, Los Alamos, NM 87545 (United States)]. E-mail: michaudon@lanl.gov; Wender, S.A. [LANSCE-3, Los Alamos National Laboratory, MS H855, Los Alamos, NM 87545 (United States)]. E-mail: wender@lanl.gov; Vieira, D.J. [C-INC, Los Alamos National Laboratory, MS J514, Los Alamos, NM 87545 (United States)]. E-mail: vieira@lanl.gov; Bond, E.M. [C-INC, Los Alamos National Laboratory, MS J514, Los Alamos, NM 87545 (United States)]. E-mail: bond@lanl.gov; Bredeweg, T.A. [C-INC, Los Alamos National Laboratory, MS J514, Los Alamos, NM 87545 (United States)]. E-mail: toddb@lanl.gov; Kronenberg, A. [C-INC, Los Alamos National Laboratory, MS J514, Los Alamos, NM 87545 (United States)]. E-mail: kronenberga@mail.phy.ornl.gov; Wilhelmy, J.B. [C-INC, Los Alamos National Laboratory, MS J514, Los Alamos, NM 87545 (United States)]. E-mail: j_wilhelmy@lanl.gov; Ethvignot, T. [Commissariat a l' Energie Atomique, DIF/DPTA/Service de Physique Nucleaire, BP 12, 91680 Bruyeres-le-Cha-hat tel (France)]. E-mail: thierry.ethvignot@cea.fr; Granier, T. [Commissariat a l' Energie Atomique, DIF/DPTA/Service de Physique Nucleaire, BP 12, 91680 Bruyeres-le-Cha-hat tel (France)]. E-mail: thierry.granier@cea.fr; Petit, M. [Commissariat a l' Energie Atomique, DIF/DPTA/Service de Physique Nucleaire, BP 12, 91680 Bruyeres-le-Chatel (France)]. E-mail: michael.petit@cea.fr; Danon, Y. [Rensselaer Polytechnic Institute, Troy, New York, NY 12180 (United States)]. E-mail: danony@rpi.edu

    2005-09-11

    A description is given of a lead slowing-down spectrometer (LSDS) installed at the 800-MeV proton accelerator of the Los Alamos Neutron Science Center (LANSCE). The LSDS is designed to study neutron-induced fission on actinides that can only be obtained or used in small quantities. The characteristics of this LSDS (energy-time relation, energy resolution, neutron flux) are presented through simulations with MCNPX and measurements with several different methods. Results on neutron-induced fission of {sup 235}U and {sup 239}Pu with tens of micrograms and tens of nanograms, respectively, are presented. Finally, additional MCNPX calculations have been performed to simulate the measurement of the cross-section for U235m(n,f) using different target quantities and different initial isomer-to-ground state compositions.

  11. Prompt Fission Gamma-ray Studies at DANCE

    Science.gov (United States)

    Jandel, M.; Rusev, G.; Bond, E. M.; Bredeweg, T. A.; Chadwick, M. B.; Couture, A.; Fowler, M. M.; Haight, R. C.; Kawano, T.; Keksis, A. L.; Mosby, S. M.; O'Donnell, J. M.; Rundberg, R. S.; Stetcu, I.; Talou, P.; Ullmann, J. L.; Vieira, D. J.; Wilhelmy, J. B.; Stoyer, M. A.; Haslett, R. J.; Henderson, R. A.; Becker, J. A.; Wu, C. Y.

    Measurements of correlated data on prompt-fission γ-rays (PFG) have been carried out for various actinide isotopes in recent years using the Detector for Advanced Neutron Capture Experiments (DANCE) at Los Alamos National Laboratory (LANL). We have developed a model that conveniently parametrizes the correlated data of γ-ray multiplicity and energy. New results on two- dimensional prompt-fission γ-ray multiplicity versus energy distributions from spontaneous fission on 252Cf and neutron-induced fission on 242mAm are presented together with previously obtained results on 233,235U and 239Pu. Correlated PFG data from 252Cf are also compared to results of the detailed theoretical model developed at LANL, for different thresholds of PFG energies. Future plans to measure correlated data on fission fragments, prompt fission neutrons and γ-rays at DANCE are presented.

  12. Neutron-Induced Fission Measurements at the Dance and Lsds Facilities at Lanl

    Science.gov (United States)

    Jandel, M.; Bredeweg, T. A.; Bond, E. M.; Chadwick, M. B.; Couture, A.; O'Donnell, J. M.; Fowler, M. M.; Haight, R. C.; Hayes-Sterbenz, A. C.; Rundberg, R. S.; Rusev, G. Y.; Ullmann, J. L.; Vieira, D. J.; Wilhelmy, J. B.; Wu, C. Y.; Becker, J. A.; Alexander, C. W.; Belier, G.

    2014-09-01

    New results from neutron-induced fission measurements performed at the Detector for Advanced Neutron Capture Experiments (DANCE) and Lead Slowing Down Spectrometer (LSDS) are presented. New correlated data on promptfission γ-ray (PFG) distributions were measured using the DANCE array for resonant neutron-induced fission of 233U, 235U and 239Pu. The deduced properties of PFG emission are presented using a simple parametrization. An accurate knowledge of fission γ-ray spectra enables us to analyze the isomeric states of 236U created after neutron capture on 235U. We briefly discuss these new results. Finally, we review details and preliminary results of the challenging 237U(n,f) cross section measurement at the LSDS facility.

  13. Multi-collector Isotope Ratio Mass Spectrometer -- Operational Performance Report

    Energy Technology Data Exchange (ETDEWEB)

    Appelhans, Anthony D; Olson, John E; Watrous, Matthew G; Ward, Michael B.; Dahl, David A.

    2010-12-01

    This report describes the operational testing of a new magnetic sector mass spectrometer that utilizes seven full-sized discrete dynode electron multipliers operating simultaneously. The instrument includes a newly developed ion dispersion lens that enables the mass dispersed individual isotope beams to be separated sufficiently to allow a full-sized discrete dynode pulse counting multiplier to be used to measure each isotope beam. The performance of the instrument was measured using SRM 996 (244Pu spike) at loadings of 2.4 and 12 fg on resin beads and with SRM 4350B Columbia River Sediment samples. The measured limit of detection (3s) for 240Pu was 3.4 attograms for SRM 996. The limit of quantitation (LOQ), defined as 10 s, was 11.2 attograms. The measured concentration of 239Pu in the CRS standard was 152 ± 6 fg/g.

  14. Uncertainties analysis of fission fraction for reactor antineutrino experiments using DRAGON

    CERN Document Server

    Ma, X B; Chen, Y X; Zhong, W L; An, F P

    2014-01-01

    Rising interest in nuclear reactors as a source of antineutrinos for experiments motivates validated, fast, and accessible simulation to predict reactor rates. First, DRAGON was developed to calculate the fission rates of the four most important isotopes in fissions,235U,238U,239Pu and141Pu, and it was validated for PWRs using the Takahama benchmark. The fission fraction calculation function was validated through comparing our calculation results with MIT's results. we calculate the fission fraction of the Daya Bay reactor core, and compare its with those calculated by the commercial reactor simulation program SCIENCE, which is used by the Daya Bay nuclear power plant, and the results was consist with each other. The uncertainty of the antineutrino flux by the fission fraction was studied, and the uncertainty of the antineutrino flux by the fission fraction simulation is 0.6% per core for Daya Bay antineutrino experiment.

  15. Ternary particles with extreme N/Z ratios from neutron-induced fission

    Energy Technology Data Exchange (ETDEWEB)

    Koster, U.; Faust, H.; Friedrichs, T.; Oberstedt, S.; Fioni, G.; Grob, M.; Ahmad, I. J.; Devlin, M.; Heinz, A.; Kondev, F. G.; Lauritsen, T.; Sarantites, D. G.; Siem, S.; Sobotka, L. G.; Sonzogni, A.

    2000-05-16

    The existing ternary fission models can well reproduce the yields of the most abundant light charged particles. However, these models tend to significantly overestimate the yields of ternary particles with an extreme N/Z ratio: {sup 3}He, {sup 11}Li, {sup 14}Be, etc. The experimental yields of these isotopes were investigated with the recoil separator LOHENGRIN down to a level of 10{sup {minus}10} per fission. Results from the fissioning systems {sup 233}U (n{sub th}, f), {sup 235}U(n{sub th},f), {sup 239}Pu(n{sub th},f) {sup 241}Pu(n{sub th},f) and {sup 245}Cm(n{sub th},f) are presented and the implications for the ternary fission models are discussed.

  16. New Monte Carlo-based method to evaluate fission fraction uncertainties for the reactor antineutrino experiment

    Science.gov (United States)

    Ma, X. B.; Qiu, R. M.; Chen, Y. X.

    2017-02-01

    Uncertainties regarding fission fractions are essential in understanding antineutrino flux predictions in reactor antineutrino experiments. A new Monte Carlo-based method to evaluate the covariance coefficients between isotopes is proposed. The covariance coefficients are found to vary with reactor burnup and may change from positive to negative because of balance effects in fissioning. For example, between 235U and 239Pu, the covariance coefficient changes from 0.15 to -0.13. Using the equation relating fission fraction and atomic density, consistent uncertainties in the fission fraction and covariance matrix were obtained. The antineutrino flux uncertainty is 0.55%, which does not vary with reactor burnup. The new value is about 8.3% smaller.

  17. {sup 239,} {sup 240,} {sup 241}Pu fingerprinting of plutonium in western US soils using ICPMS: solution and laser ablation measurements

    Energy Technology Data Exchange (ETDEWEB)

    Cizdziel, James V. [University of Nevada - Las Vegas, Harry Reid Center for Environmental Studies, Las Vegas, NV (United States); Ketterer, Michael E. [Northern Arizona University, Department of Chemistry and Biochemistry, Box 5698, Flagstaff, AZ (United States); Farmer, Dennis [University of Nevada - Las Vegas, Department of Health Physics, Las Vegas, NV (United States); Faller, Scott H. [US Environmental Protection Agency, Radiation and Indoor Environments National Laboratory, Box 98517, Las Vegas, NV (United States); Hodge, Vernon F. [University of Nevada - Las Vegas, Department of Chemistry, Las Vegas, NV (United States)

    2008-01-15

    Sector field inductively coupled plasma mass spectrometry (SF-ICPMS) has been used with analysis of solution samples and laser ablation (LA) of electrodeposited alpha sources to characterize plutonium activities and atom ratios prevalent in the western USA. A large set of surface soils and attic dusts were previously collected from many locations in the states of Nevada, Utah, Arizona, and Colorado; specific samples were analyzed herein to characterize the relative contributions of stratospheric fallout vs. Nevada Test Site (NTS) plutonium. This study illustrates two different ICPMS-based analytical strategies that are successful in fingerprinting Pu in environmental soils and dusts. Two specific datasets have been generated: (1) soils are leached with HNO{sub 3}-HCl, converted into electrodeposited alpha sources, counted by alpha spectrometry, then re-analyzed using laser ablation SF-ICPMS; (2) samples are completely dissolved by treatment with HNO{sub 3}-HF-H{sub 3}BO{sub 3}, Pu fractions are prepared by extraction chromatography, and analyzed by SF-ICPMS. Optimal laser ablation and ICPMS conditions were determined for the re-analysis of archived alpha spectrometry ''planchette'' sources. The best ablation results were obtained using a large spot size (200 {mu}m), a defocused beam, full repetition rate (20 Hz) and scan rate (200 {mu}m s{sup -1}); LA-ICPMS data were collected with a rapid electrostatic sector scanning experiment. Less than 10% of the electroplated surface area is consumed in the LA-ICPMS analysis, which would allow for multiple re-analyses. Excellent agreement was found between {sup 239+240}Pu activities determined by LA-ICPMS vs. activity results obtained by alpha spectrometry for the same samples ten years earlier. LA-ICPMS atom ratios for {sup 240}Pu/{sup 239}Pu and {sup 241}Pu/{sup 239}Pu range from 0.038-0.132 and 0.00034-0.00168, respectively, and plot along a two-component mixing line ({sup 241}Pu/{sup 239}Pu = 0

  18. Fissile and Non-Fissile Material Detection using Nuclear Acoustic Resonance Signatures: Final Report

    Energy Technology Data Exchange (ETDEWEB)

    Herberg, J; Maxwell, R; Tittmann, B R; Lenahan, P M; Yerkes, S; Jayaraman, S B

    2006-11-02

    This is final report on NA-22 project LL251DP, where the goal was to develop a novel technique, Nuclear Acoustic Resonance (NAR), for remote, non-destructive, nonradiation-based detection of materials of interest to Nonproliferation Programs, including {sup 235}U and {sup 239}Pu. In short, we have developed a magnetic shield chamber and magnetic field, develop a digital lock-in amplifier computer to integrate both the ultrasound radiation with the detector, developed strain measurements, and begun to perform initial measurements to obtain a NAR signal from aluminum at room temperature and near the earth's magnetic field. Since our funding was cut in FY06, I will discuss where this project can go in the future with this technology.

  19. Fissile and Non-Fissile Material Detection using Nuclear Acoustic Resonance Signatures

    Energy Technology Data Exchange (ETDEWEB)

    Herberg, J; Maxwell, R; Tittmann, B R; Lenahan, P M; Yerkes, S; Jayaraman, S

    2005-10-04

    This report reviews progress made on NA22 project LL251DP to develop a novel technique, Nuclear Acoustic Resonance (NAR), for remote, non-destructive, nonradiation-based detection of materials of interest to Nonproliferation Programs, including {sup 235}U and {sup 239}Pu. We have met all milestones and deliverables for FY05, as shown in Table 1. In short, we have developed a magnetic shield chamber and magnetic field, develop a digital lock-in amplifier computer to integrate both the ultrasound radiation with the detector, developed strain measurements, and begin to perform initial measurements to obtain a NAR signal from aluminum at room temperature and near the earth's magnetic field. The results obtained in FY05 further support the feasibility of successful demonstration of an NAR experiment for remote, non-destructive, non-radiation-based detection of materials of interest to Nonproliferation Programs.

  20. Corrigendum to "Coupled thermochemical, isotopic evolution and heat transfer simulations in highly irradiated UO2 nuclear fuel"

    Science.gov (United States)

    Piro, M. H. A.; Banfield, J.; Clarno, K.; Simunovic, S.; Besmann, T. M.; Lewis, B. J.; Thompson, W. T.

    2016-09-01

    Figs. 7-9 in "Coupled thermochemical, isotopic evolution and heat transfer simulations in highly irradiated UO2 nuclear fuel" [1] have a consistent error corresponding to the relative proportions of iodine. Reported concentrations of iodine in the original manuscript are approximately ten times higher than expected, and are comparable in atomic proportions to cesium. One would expect that the amount of cesium would be about one order of magnitude greater than iodine based on the difference in fission yields of 235U and 239Pu. A practical consequence of this error would affect the predicted quantity and chemical composition of iodine on the fuel surface, which is related to iodine-induced stress corrosion cracking [2].

  1. Preparation of reference material for uranium and plutonium measurements using cellulose compound as a stabilizer

    Energy Technology Data Exchange (ETDEWEB)

    Surugaya, Naoki; Sato, Soichi; Hina, Tetsuro; Hiyama, Toshiaki [Japan Nuclear Cycle Development Inst., Tokai Works, Tokai, Ibaraki (Japan)

    2003-03-01

    Isotope dilution mass spectrometry, considered the most reliable analytical technique for input accountancy measurements of uranium and plutonium in spent fuel reprocessing plants, requires a well-characterized uranium/plutonium spike. Solid spikes containing {sup 235}U and {sup 239}Pu have been successfully utilized in safeguards inspections and in accountability analysis. They contain relatively large amounts of uranium and plutonium isotopically different to the uranium and plutonium of the sample, and are usually in the dried nitrate form. However, it is difficult to maintain and guarantee the integrity of the spike over long periods as they are in the dried nitrate form that can flake off the glass ampoule surface. Organic coatings were investigated using cellulose acetate butyrate as a stabilizer. The cellulose acetate butyrate had good characteristics, maintaining a thin film for a long time. (author)

  2. Study on the properties of saline HLLW in China

    Institute of Scientific and Technical Information of China (English)

    LiangJun-Fu; TianGuo-Xing; 等

    1997-01-01

    The properties and the component of HLLW(High Level Liquid Waste)were studied.The senuine saline HLLW is a blue-green liquid without any deposition.Its density and acidity are 1.399 g/ml(23±1℃) and 2.1 mol/L NHO3,respectively.The activities of 137Cs, 90Sr,99Tc,237Np,239Pu,241Am,total α,totalβ,totalγ are determined.The extractabilities of actinides in the genuine HLLW were examined with a five-stage cross extraction experiment.More than 98% of Pu is in Pu4+ species,and more than 70% of Np is in Np4+ species.More than 99.97% α-nuclides could be extracted by 30% TRPO-Kerosene in 1mol/L NHO3 from the HLLW.

  3. Three-dimensional SPECT imaging with LaBr{sub 3}:Ce scintillator for characterization of nuclear waste

    Energy Technology Data Exchange (ETDEWEB)

    Roy, Tushar, E-mail: tushar@barc.gov.in; Ratheesh, Jilju; Sinha, Amar

    2014-01-21

    Characterization of nuclear waste in terms of radioactivity distribution is important not only for their safe disposal but also for nuclear material accounting. Single Photon Emission Computed Tomography (SPECT) provides a non-invasive technique for the characterization and activity distribution of the gamma-emitting sources in a matrix. Sodium iodide scintillators, which are most commonly used, suffer from poor energy resolution and do not provide accurate peak discrimination for radioisotopes like {sup 239}Pu which have overlapping peaks. Cerium-activated lanthanum bromide (LaBr{sub 3}:Ce) scintillators have better energy resolution and provide better peak discrimination. In this paper, experimental studies using LaBr{sub 3}:Ce for 3D SPECT imaging of dummy waste drum has been discussed. The reconstruction has been done using the Filtered Backprojection scheme with attenuation compensation based on Novikov's inversion formula.

  4. Three-dimensional SPECT imaging with LaBr3:Ce scintillator for characterization of nuclear waste

    Science.gov (United States)

    Roy, Tushar; Ratheesh, Jilju; Sinha, Amar

    2014-01-01

    Characterization of nuclear waste in terms of radioactivity distribution is important not only for their safe disposal but also for nuclear material accounting. Single Photon Emission Computed Tomography (SPECT) provides a non-invasive technique for the characterization and activity distribution of the gamma-emitting sources in a matrix. Sodium iodide scintillators, which are most commonly used, suffer from poor energy resolution and do not provide accurate peak discrimination for radioisotopes like 239Pu which have overlapping peaks. Cerium-activated lanthanum bromide (LaBr3:Ce) scintillators have better energy resolution and provide better peak discrimination. In this paper, experimental studies using LaBr3:Ce for 3D SPECT imaging of dummy waste drum has been discussed. The reconstruction has been done using the Filtered Backprojection scheme with attenuation compensation based on Novikov's inversion formula.

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

    Science.gov (United States)

    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.

  6. Oxidation-state distribution of plutonium in surface and subsurface waters at Thule, northwest Greenland

    DEFF Research Database (Denmark)

    McMahon, C.A.; Vintró, L.L.; Mitchell, P.I.

    2000-01-01

    chemical form) is present as fully dissolved species. Most of this plutonium would seem to be of weapons fallout origin, as the mean Pu-238/Pu-239,Pu-240 activity ratio in the water column (dissolved phase) at Thule (0.06 +/- 0.02; n = 10) is similar to the global fallout ratio at this latitude......The speciation of plutonium in Arctic waters sampled on the northwest Greenland shelf in August 1997 is discussed in this paper. Specifically, we report the results of analyses carried out on seawater sampled (a) close to the Thule air base where, in 1968, a US military aircraft carrying four......(V, VI) (mean, 68 +/- 6%; n = 6), with little if any distinction apparent between surface and bottom waters. Further, the oxidation state distribution at stations close to the accident site is similar to that measured at Upernavik, remote from this site. It is also similar to the distribution observed...

  7. Plutonium, Mineralogy and Radiation Effects

    Science.gov (United States)

    Ewing, R. C.

    2006-05-01

    During the past fifty years, more than 1,800 metric tonnes of Pu and substantial quantities of other "minor" actinides, such as Np, Am and Cm, have been generated in nuclear reactors. Some of these transuranic elements can be a source of energy in fission reactions (e.g., 239Pu), a source of fissile material for nuclear weapons (e.g., 239Pu and 237Np), or are of environmental concern because of their long half- lives and radiotoxicity (e.g., 239Pu, t1/2 = 24,100 years, and 237Np, t1/2 = 2.1 million years). There are two basic strategies for the disposition of these elements: 1.) to "burn" or transmute the actinides using nuclear reactors or accelerators; 2.) to "sequester" the actinides in chemically durable, radiation-resistant materials that are suitable for geologic disposal. There has been substantial interest in the use of actinide-bearing minerals, such as zircon or isometric pyrochlore, A2B2O7 (A = rare earths; B = Ti, Zr, Sn, Hf; Fd3m; Z=8), for the immobilization of actinides, particularly plutonium. One of the principal concerns has been the accumulation of structural damage caused by alpha-decay events, particularly from the recoil nucleus. Systematic ion beam irradiation studies of rare-earth pyrochlores have led to the discovery that certain compositions (B = Zr, Hf) are stable to very high fluences of alpha-decay event damage. Some compositions, Gd2Ti2O7, are amorphized at relatively low doses (0.2 displacements per atom, dpa, at room temperature), while other compositions, Gd2Zr2O7, do not amorphize (even at doses of > 40 dpa at 25K), but instead disorder to a defect fluorite structure. By changing the composition of the A-site (e.g., substitution of different rare earth elements), the temperature above which the pyrochlore composition can no longer be amorphized, Tc, varies by >600 K (e.g., Lu2Ti2O7: Tc = 480 K; Gd2Ti2O7: Tc = 1120 K). The variation in response to irradiation as a function of composition can be used to model the long

  8. DEVELOPMENT OF AN IMPROVED SODIUM TITANATE FOR THE PRETREATMENT OF HIGH LEVEL NUCLEAR WASTE AT THE SAVANNAH RIVER SITE

    Energy Technology Data Exchange (ETDEWEB)

    Hobbs D. T.; Poirier, M. R.; Barnes, M. J.; Stallings, M. E.; Nyman, M. D.

    2005-11-22

    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 onsite as low level waste. Separation processes planned at SRS include caustic side solvent extraction, for {sup 137}Cs removal, and sorption of {sup 90}Sr and alpha-emitting radionuclides onto 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 describes recent results to produce an improved sodium titanate material that exhibits increased removal kinetics and capacity for {sup 90}Sr and alpha-emitting radionuclides compared to the baseline MST material.

  9. LITERATURE REVIEW ON MAXIMUM LOADING OF RADIONUCLIDES ON CRYSTALLINE SILICOTITANATE

    Energy Technology Data Exchange (ETDEWEB)

    Adu-Wusu, K.; Pennebaker, F.

    2010-10-13

    Plans are underway to use small column ion exchange (SCIX) units installed in high-level waste tanks to remove Cs-137 from highly alkaline salt solutions at Savannah River Site. The ion exchange material slated for the SCIX project is engineered or granular crystalline silicotitanate (CST). Information on the maximum loading of radionuclides on CST is needed by Savannah River Remediation for safety evaluations. A literature review has been conducted that culminated in the estimation of the maximum loading of all but one of the radionuclides of interest (Cs-137, Sr-90, Ba-137m, Pu-238, Pu-239, Pu-240, Pu-241, Am-241, and Cm-244). No data was found for Cm-244.

  10. Application of microdosimetric methods for the determination of energy deposition distributions by inhaled actinides

    Energy Technology Data Exchange (ETDEWEB)

    Aubineau-Laniece, I.; Castellan, G.; Caswell, R.S.; Guezingar, F.; Henge-Napoli, M.H.; Li, W.B.; Pihet, P

    1998-07-01

    The respiratory tract dosimetry model of ICRP Publication 66 takes into account the morphometry of lung tissues for the determination of average energy deposited by {alpha} emitters. However, it assumes a uniform distribution of radioactive material. The statistical fluctuations in frequency of cells hit and of energy deposited in individual target cells depends significantly on the real distribution of radioactive material, including possible high local concentrations. This paper is aimed at investigating the application of two established analytic methods, which have been combined to determine single and multi-event energy deposition distributions in epithelial cells of bronchiolar airway exposed to 5.15 MeV {alpha} particles ({sup 239}Pu). The relative importance of multi-event occurrence on the shape of the specific energy distributions is discussed. (author)

  11. Dating of a sediment core from Lake Biel (Switzerland) and source characterization of fallout Pu; {sup 210}Pb- und {sup 137}Cs-Datierung eines Sedimentbohrkerns aus dem Bieler See (CH) und Ursprungsbestimmung von Pu-Fallout

    Energy Technology Data Exchange (ETDEWEB)

    Pregler, Anja

    2016-08-01

    A sediment core from Lake Biel was dated by means of the naturally occurring radioactive isotope {sup 210}Pb as well as by the anthropogenic isotope {sup 137}Cs. The latter one can be detected as radioactive fallout of certain events in the sediment layers and accordingly be correlated with a distinct date. A verification of the correlated events is accomplished by particular isotope ratios of the anthropogenic isotopes {sup 238}Pu, {sup 239}Pu and {sup 240}Pu as well as {sup 241}Am as a decay product of the short-lived {sup 241}Pu. Furthermore, the percentage of the total {sup 137}Cs fallout was calculated corresponding to the specific events.

  12. Fusion energy and nuclear non-proliferation

    Energy Technology Data Exchange (ETDEWEB)

    Goldston, Rob [Princeton Plasma Physics Lab, Princeton (United States)

    2014-07-01

    Neutrons from DT fusion can be used to produce {sup 239}Pu or {sup 233}U. However since no fertile nor fissile material need be present in a pure fusion power plant, it would be relatively easy to detect significant covert transmutation in a declared facility. Clandestine fusion-based transmutation does not appear credible. Furthermore, no fissile materials are immediately available in a fusion breakout scenario. DT fusion systems produce and burn 400g of tritium per day, a small fraction of which, if diverted, could be used to enhance the efficiency, reliability and/or safety of a nuclear weapon. Very accurate T accountancy needs to be developed for fusion energy systems. Finally, the spread of inertial fusion energy R and D may result in dissemination of knowledge relevant to the design of nuclear weapons. International agreements to restrain information transfer are required. In summary, fusion is much safer from a proliferation standpoint than fission, but still requires verification and control.

  13. Safety and Environmental Protection Division. Progress report, January 1, 1974--December 31, 1975. [Radionuclides in Bikini foods during 1974 and 1975 and environmental monitoring data for BNL during 1975

    Energy Technology Data Exchange (ETDEWEB)

    None

    1977-01-01

    Progress is reported in the analysis of food chain samples collected during 1974 and 1975 at the Bikini Atoll in the Marshall Islands for /sup 90/Sr, /sup 137/Cs, /sup 239/Pu, /sup 240/Pu, and /sup 241/Am remaining in the environment from the 1946-1958 nuclear tests. Data on levels of radioactivity in environmental samples and SO/sub 2/ and NO/sub x/ in air samples collected in the vicinity of Brookhaven National Laboratory during 1975 are reported. Samples of surface air, surface waters, ground water, sediments and biota from streams, soils, grass, and milk were analyzed. Abstracts of papers published during 1974 and 1975 are included. (CH)

  14. Effect of compositional variation in plutonium on process shielding design

    Energy Technology Data Exchange (ETDEWEB)

    Brown, T.H.

    1997-11-01

    Radiation dose rate from plutonium with high {sup 239}Pu content varies with initial nuclidic content, radioactive decay time, and impurity elemental content. The two idealized states of old plutonium and clean plutonium, whose initial compositions are given, provide approximate upper and lower bounds on dose rate variation. Whole-body dose rates were calculated for the two composition states, using unshielded and shielded plutonium spheres of varying density. The dose rates from these variable density spheres are similar to those from expanded plutonium configurations encountered during processing. The dose location of 40 cm from the sphere center is representative of operator standoff for direct handling of plutonium inside a glove box. The results have shielding implications for glove boxes with only structurally inherent shielding, especially for processing of old plutonium in an expanded configuration. Further reduction in total dose rate by using lead to reduce photon dose rate is shown for two density cases representing compact and expanded plutonium configurations.

  15. Direct isotope ratio analysis of individual uranium-plutonium mixed particles with various U/Pu ratios by thermal ionization mass spectrometry.

    Science.gov (United States)

    Suzuki, Daisuke; Esaka, Fumitaka; Miyamoto, Yutaka; Magara, Masaaki

    2015-02-01

    Uranium and plutonium isotope ratios in individual uranium-plutonium (U-Pu) mixed particles with various U/Pu atomic ratios were analyzed without prior chemical separation by thermal ionization mass spectrometry (TIMS). Prior to measurement, micron-sized particles with U/Pu ratios of 1, 5, 10, 18, and 70 were produced from uranium and plutonium certified reference materials. In the TIMS analysis, the peaks of americium, plutonium, and uranium ion signals were successfully separated by continuously increasing the evaporation filament current. Consequently, the uranium and plutonium isotope ratios, except the (238)Pu/(239)Pu ratio, were successfully determined for the particles at all U/Pu ratios. This indicates that TIMS direct analysis allows for the measurement of individual U-Pu mixed particles without prior chemical separation.

  16. Distribution characteristics of ¹³⁷Cs, Pu isotopes and ²⁴¹Am in soil in Korea.

    Science.gov (United States)

    Lee, S H; Oh, J S; Lee, J M; Lee, K B; Park, T S; Lujaniene, G; Valiulis, D; Sakalys, J

    2013-11-01

    Cesium-137, Plutonium isotopes and (241)Am were studied in soil samples collected from Korea between 2006 and 2008 to provide information on the distribution and origin of Pu isotopes and (241)Am. The vertical profiles of radionuclides showed higher activity concentrations at the surface layer and then gradually decreased with depth. A good correlation between (137)Cs and (239,240)Pu was observed, whereas a poor relationship between (137)Cs and (241)Am was found. The (238)Pu/(239,240)Pu, (241)Am/(239,240)Pu and (239,240)Pu/(137)Cs activity ratios were concordant to those of the global fallout ratios. Furthermore, the atomic ratios of (240)Pu/(239)Pu in the samples provided the information of Pu depositional history and the origin of Pu isotopes in Korea.

  17. Analysis of the effects of inter-individual variation in the distribution of plutonium in skeleton and liver.

    Science.gov (United States)

    Klein, W; Breustedt, B

    2014-01-01

    One important parameter for biokinetic plutonium modelling is the ratio between the contents of plutonium in liver and skeleton. Autopsy data show a vast inter-individual variation in the partitioning between these organs. The capacity of recent biokinetic models for plutonium to reproduce these variations was studied. Autopsy data for plutonium amounts in liver and skeleton for both (238)Pu and (239)Pu isotopes can be merged into a single data set following several statistical tests. Simulations with different parameter values generate a mapping between the autopsy values and the model parameters. The observed partitioning distribution can be transformed into a distribution of transfer rates, which would result in the observed data. Besides, the variation in the partitioning between liver and skeleton leads via biliary pathway to a variation in the excretion ratio. This can be used to estimate an individual partitioning factor, which can be used in individual case assessments.

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

    Directory of Open Access Journals (Sweden)

    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.

  19. Ultra-sensitive detection of plutonium by accelerator mass spectrometry

    Energy Technology Data Exchange (ETDEWEB)

    Fifield, L.K.; Cresswell, R.G.; Ophel, T.R.; Ditada, M. [Australian National Univ., Canberra, ACT (Australia). Dept. of Nuclear Physics; Day, J.P.; Clacher, A. [Manchester Univ. (United Kingdom). Dept. of Chemistry; Priest, N.D. [AEA Technology, Harwell (United Kingdom)

    1996-12-31

    On the bases of the measurements performed to date, a sensitivity of 10{sup 6} atoms is achievable with accelerator mass spectroscopy (AMS) for each of the plutonium isotopes. Not only does this open the way to the sort of study outlined, but it also makes possible other novel applications, of which two examples are given: (i)the ration of {sup 240}Pu to {sup 239}Pu as a sensitive indicator of the source of the plutonium; (ii) the biochemistry of plutonium in humans. The ultra-sensitive atom counting capability of AMS will make it possible to use the very long-lived {sup 244}Pu (8x10{sup 7}a) in human volunteer studies without any significant increase in radiation body burden. This paper will describe the AMS technique as applied to plutonium using the ANU`s 14UD accelerator, will present the results obtained to date, and will discuss the prospects for the future.

  20. Advanced alpha spectrum analysis based on the fitting and covariance analysis of dependent variables

    Science.gov (United States)

    Ihantola, S.; Pelikan, A.; Pöllänen, R.; Toivonen, H.

    2011-11-01

    The correct handling of statistical uncertainties is crucial especially when unfolding alpha spectra that contain a low number of counts or overlapping peaks from different nuclides. For this purpose, we have developed a new spectrum analysis software package called ADAM, which performs a full covariance calculus for alpha-particle emitting radionuclides. By analyzing a large number of simulated and measured spectra, the program was proved to give unbiased peak areas and statistically correct uncertainty limits. This applies regardless of the peak areas and the number of unknown parameters during the fitting. In addition, ADAM performs reliable deconvolution for multiplets, which opens the way for the determination of isotope ratios, such as 239Pu/240Pu.

  1. Control of radioactive wastes and coupling of neutron/gamma measurements: use of radiative capture for the correction of matrix effects that penalize the fissile mass measurement by active neutron interrogation; Controle des dechets radioactifs et couplage de mesures neutron/gamma: exploitation de la capture radiative pour corriger les effets de matrice penalisant la mesure de la masse fissile par interrogation neutronique active

    Energy Technology Data Exchange (ETDEWEB)

    Loche, F

    2006-10-15

    In the framework of radioactive waste drums control, difficulties arise in the nondestructive measurement of fissile mass ({sup 235}U, {sup 239}Pu..) by Active Neutron Interrogation (ANI), when dealing with matrices containing materials (Cl, H...) influencing the neutron flux. The idea is to use the neutron capture reaction (n,{gamma}) to determine the matrix composition to adjust the ANI calibration coefficient value. This study, dealing with 118 litres, homogeneous drums of density less than 0,4 and composed of chlorinated and/or hydrogenated materials, leads to build abacus linking the {gamma} ray peak areas to the ANI calibration coefficient. Validation assays of these abacus show a very good agreement between the corrected and true fissile masses for hydrogenated matrices (max. relative standard deviation: 23 %) and quite good for chlorinated and hydrogenated matrices (58 %). The developed correction method improves the measured values. It may be extended to 0,45 density, heterogeneous drums. (author)

  2. Safety analysis, 200 Area, Savannah River Plant: Separations area operations. Building 221-H, B-Line, Scrap Recovery Facility (Supplement 2A): Revision 1

    Energy Technology Data Exchange (ETDEWEB)

    None

    1991-07-01

    The now HB-Line is located an top of the 221-H Building on the fifth and sixth levels and is designed to replace the aging existing HB-Line production facility. The new HB-Line consists of three separate facilities: the Scrap Recovery Facility, Neptunium Facility, and Plutonium Oxide Facility. The Scrap Recovery Facility is designed to routinely generate nitrate solutions of {sup 235}U{sup 239}Pu and Pu-238 fromscrap for purification by anion exchange or by solvent extraction in the canyon. The now facility incorporates improvements in: (1) engineered controls for nuclear criticality, (2) cabinet integrity and engineered barriers to contain contamination and minimize personnel exposure to airborne contamination, (3) shielding and remote operations to decrease radiation exposure, and (4) equipment and ventilation design to provide flexibility and improved process performance.

  3. RADIATION SAFETY JUSTIFICATION FOR THE LONG-TERM STORAGE OF GAS CONDENSATE IN THE UNDERGROUND RESERVOURS FORMED BY THE NUCLEAR EXPLOSION TECHNOLOGY

    Directory of Open Access Journals (Sweden)

    I. K. Romanovich

    2010-01-01

    Full Text Available The paper presents approaches to the safety justification of the gas condensate and brine long-term storage in the underground reservoirs formed by the nuclear explosion technology. Gas condensate and brine are the intermediate level liquid radioactive waste containing isotopes: 3Н, 137Cs and 90Sr, in traces - 239Pu, 235U, 241Am.Safety of the gas condensate and brine long-term storage in the underground reservoirs is assessed on the base of the multi-barrier principle implementation, used during radioactive waste disposal. It is shown that the gas condensate and brine long-term storage in the sealed underground reservoirs formed by nuclear explosion technologies in salt domes does not lead to the surface radioactive contamination and population exposure.

  4. Single-pass continuous-flow leach test of PNL 76-68 glass: some selected Bead Leach I results

    Energy Technology Data Exchange (ETDEWEB)

    Coles, D.G.

    1981-08-20

    A single-pass continuous-flow leach test of PNL 76-68 glass beads (7 mm dia) was concluded after 420 days of uninterrupted operation. Variables included in the experimental matrix were flow-rate, leachant composition, and temperature. Analysis was conducted on all leachate samples for /sup 237/Np and /sup 239/Pu as well as a number of nonradioactive elements. Results indicated that flow-rate and leachant systematically affected the leach rate, but only slightly. Temperature effects were significant. Plutonium leach rate was lower at higher temperature suggesting that Pu sorption onto the beads was enhanced at the higher temperature. The range of leach rates for all analyzed elements (except Pu), at both temperatures, at all three flow rates, and with all three leachant compositions varied over only three orders of magnitude. The range of variables used in this experiment covered those expected in many proposed repository environments.

  5. Future research program on prompt γ-ray emission in nuclear fission

    Energy Technology Data Exchange (ETDEWEB)

    Oberstedt, S.; Hambsch, F.J. [Joint Research Centre IRMM, European Commission, Geel (Belgium); Billnert, R. [Joint Research Centre IRMM, European Commission, Geel (Belgium); Chalmers Tekniska Hoegskola, Fundamental Fysik, Goeteborg (Sweden); Lebois, M.; Wilson, J.N. [Institut de Physique Nucleaire Orsay, Orsay (France); Oberstedt, A. [Chalmers Tekniska Hoegskola, Fundamental Fysik, Goeteborg (Sweden); Ossolution Consulting, Oerebro (Sweden)

    2015-12-15

    In recent years the measurement of prompt fission γ-ray spectra (PFGS) has gained renewed interest, after about forty years since the first comprehensive studies of the reactions {sup 235}U(n{sub th}, f), {sup 239}Pu(n{sub th},f) and {sup 252}Cf(sf). The renaissance was initiated by requests for new values especially for γ-ray multiplicity and average total energy release per fission in neutron-induced fission of {sup 235}U and {sup 239}Pu. Both isotopes are considered the most important ones with respect to the modeling of innovative cores required for the Generation-IV reactors, the majority working with fast neutrons. During the last 5 years we have conducted a systematic study of spectral data for thermal-neutron-induced fission on {sup 235}U and {sup 241}Pu as well as for the spontaneous fission of {sup 252}Cf with unprecedented accuracy. From the new data we conclude that those reactions do not considerably contribute to the observed heat excess and suspect other reactions playing a significant role. Possible contributions may originate from fast-neutron-induced reactions on {sup 238}U, which is largely present in the fuel, or from γ-induced fission from neutron capture in the construction material. A first experiment campaign on prompt γ-ray emission from fast-neutron-induced fission on {sup 235,238}U was successfully performed in order to test our assumptions. In the following we attempt to summarize, what has been done in the field to date, and to motivate future measurement campaigns exploiting dedicated neutron and photon beams as well as upcoming highly efficient detector assemblies. (orig.)

  6. Future research program on prompt γ-ray emission in nuclear fission

    Science.gov (United States)

    Oberstedt, S.; Billnert, R.; Hambsch, F.-J.; Lebois, M.; Oberstedt, A.; Wilson, J. N.

    2015-12-01

    In recent years the measurement of prompt fission γ-ray spectra (PFGS) has gained renewed interest, after about forty years since the first comprehensive studies of the reactions 235U(n th , f), 239Pu(n th ,f) and 252Cf(sf). The renaissance was initiated by requests for new values especially for γ-ray multiplicity and average total energy release per fission in neutron-induced fission of 235U and 239Pu. Both isotopes are considered the most important ones with respect to the modeling of innovative cores required for the Generation-IV reactors, the majority working with fast neutrons. During the last 5 years we have conducted a systematic study of spectral data for thermal-neutron-induced fission on 235U and 241Pu as well as for the spontaneous fission of 252Cf with unprecedented accuracy. From the new data we conclude that those reactions do not considerably contribute to the observed heat excess and suspect other reactions playing a significant role. Possible contributions may originate from fast-neutron-induced reactions on 238U, which is largely present in the fuel, or from γ-induced fission from neutron capture in the construction material. A first experiment campaign on prompt γ-ray emission from fast-neutron-induced fission on 235,238U was successfully performed in order to test our assumptions. In the following we attempt to summarize, what has been done in the field to date, and to motivate future measurement campaigns exploiting dedicated neutron and photon beams as well as upcoming highly efficient detector assemblies.

  7. Isotopic characterization and thermal neutron flux determination of a PuBe neutron source.

    Science.gov (United States)

    Purty, Ravi Ankit; Akanchha; Prasad, Shikha

    2017-07-01

    The Indian Institute of Technology Kanpur (IIT Kanpur) possesses a PuBe neutron source facility with an initial activity of 5 Ci, dated September 1966 (nearly 50 years ago). An understanding of the present activity and the rate of its change will allow implementation of proper radiological safety procedures and future radiological safety planning. Knowing the absolute neutron flux will help us in future neutron activation studies. These details are also important to ensure proper security precautions. In our work, we attempt to identify the isotopic composition to determine the rate of change of the source and the absolute thermal neutron flux of plutonium beryllium (PuBe) sample at IIT Kanpur. We have used gamma-ray spectroscopy for determining the isotopic composition of the PuBe neutron source. After utilizing gamma-ray spectroscopy it is found that the source is composed of (239)Pu and a small amount of (241)Am is present as an impurity. The mass ratio of (241)Am to (239)Pu is found to be approximately 18.1µg/g with an uncertainty of 1.39%. Delayed gamma neutron activation analysis (DGNAA) is used to determine the thermal neutron flux of the same PuBe neutron source using copper, cobalt, nickel and cadmium samples. The average thermal neutron flux as calculated from DGNAA is approximately 1.27×10(3)n/(cm(2)-s) at 1cm above the PuBe neutron source. Copyright © 2017 Elsevier Ltd. All rights reserved.

  8. Cumulative fission yields of short-lived isotopes under natural-abundance-boron-carbide-moderated neutron spectrum

    Energy Technology Data Exchange (ETDEWEB)

    Finn, Erin C.; Metz, Lori A.; Greenwood, Lawrence R.; Pierson, Bruce; Wittman, Richard S.; Friese, Judah I.; Kephart, Rosara F.

    2015-04-09

    The availability of gamma spectroscopy data on samples containing mixed fission products at short times after irradiation is limited. Due to this limitation, data interpretation methods for gamma spectra of mixed fission product samples, where the individual fission products have not been chemically isolated from interferences, are not well-developed. The limitation is particularly pronounced for fast pooled neutron spectra because of the lack of available fast reactors in the United States. Samples containing the actinide isotopes 233, 235, 238U, 237Np, and 239Pu individually were subjected to a 2$ pulse in the Washington State University 1 MW TRIGA reactor. To achieve a fission-energy neutron spectrum, the spectrum was tailored using a natural abundance boron carbide capsule to absorb neutrons in the thermal and epithermal region of the spectrum. Our tailored neutron spectrum is unique to the WSU reactor facility, consisting of a soft fission spectrum that contains some measurable flux in the resonance region. This results in a neutron spectrum at greater than 0.1 keV with an average energy of 70 keV, similar to fast reactor spectra and approaching that of 235U fission. Unique fission product gamma spectra were collected from 4 minutes to 1 week after fission using single-crystal high purity germanium detectors. Cumulative fission product yields measured in the current work generally agree with published fast pooled fission product yield values from ENDF/B-VII, though a bias was noted for 239Pu. The present work contributes to the compilation of energy-resolved fission product yield nuclear data for nuclear forensic purposes.

  9. Disaggregating measurement uncertainty from population variability and Bayesian treatment of uncensored results.

    Science.gov (United States)

    Strom, Daniel J; Joyce, Kevin E; MacLellan, Jay A; Watson, David J; Lynch, Timothy P; Antonio, Cheryl L; Birchall, Alan; Anderson, Kevin K; Zharov, Peter A

    2012-04-01

    In making low-level radioactivity measurements of populations, it is commonly observed that a substantial portion of net results is negative. Furthermore, the observed variance of the measurement results arises from a combination of measurement uncertainty and population variability. This paper presents a method for disaggregating measurement uncertainty from population variability to produce a probability density function (PDF) of possibly true results. To do this, simple, justifiable and reasonable assumptions are made about the relationship of the measurements to the measurands (the 'true values'). The measurements are assumed to be unbiased, that is, that their average value is the average of the measurands. Using traditional estimates of each measurement's uncertainty, a likelihood PDF for each individual's measurand is produced. Then using the same assumptions and all the data from the population of individuals, a prior PDF of measurands for the population is produced. The prior PDF is non-negative, and the average is equal to the average of the measurement results for the population. Using Bayes's theorem, posterior PDFs of each individual measurand are calculated. The uncertainty in these bayesian posterior PDFs appears to be all Berkson with no remaining classical component. The method is applied to baseline bioassay data from the Hanford site. The data include (90)Sr urinalysis measurements of 128 people, (137)Cs in vivo measurements of 5337 people and (239)Pu urinalysis measurements of 3270 people. The method produces excellent results for the (90)Sr and (137)Cs measurements, since there are non-zero concentrations of these global fallout radionuclides in people who have not been occupationally exposed. The method does not work for the (239)Pu measurements in non-occupationally exposed people because the population average is essentially zero relative to the sensitivity of the measurement technique. The method is shown to give results similar to

  10. Using radiosilver and plutonium isotopes to trace the dispersion of contaminated sediment in Fukushima coastal catchments

    Science.gov (United States)

    Evrard, O.; Ayrault, S.; Pointurier, F.; Onda, Y.; Laceby, J. P.; Lepage, H.; Chartin, C.; Cirella, M.; Pottin, A. C.; Hubert, A.; Lefèvre, I.

    2015-12-01

    The Fukushima Dai-ichi nuclear power plant (FDNPP) accident in March 2011 resulted in a 3000-km² radioactive pollution plume consisting predominantly of radiocesium (137Cs and 134Cs). This plume is drained by several rivers to the Pacific Ocean after flowing through less contaminated, but densely inhabited coastal plains. As the redistribution of radionuclide contaminated sediment could expose the local population to higher radiation rates, novel fingerprinting methods were developed to trace the downstream dispersion of contaminated sediment. First, the heterogeneous deposition of metastable silver-110 (110mAg) across these coastal catchments was used to investigate sediment migration. In particular, the 110mAg/137Cs activity ratio was measured in soils and river sediment demonstrating the occurrence of a seasonal cycle of soil erosion during typhoons and spring snowmelt in 2011 and 2012. However, due to the rapid decay of 110mAg (half-life of 250 days), alternative methods were required to continue tracking sediment from 2013 onwards. One promising method includes the analyses of plutonium isotopes to further understand sediment migration in the Fukushima region. For example, 241Pu/239Pu atom ratios measured in sediment collected in Fukushima coastal rivers shortly after the accident were shown to be significantly higher (0.0017 - 0.0884) than corresponding values attributed to the global fallout (0.00113 ± 0.00008). Additional analyses were conducted on sediment sampled in 2013 and 2014 after the start of decontamination works. These analyses show that the 241Pu/239Pu atom ratios decreased towards the global fallout values in rivers draining decontaminated paddy fields, demonstrating the effectiveness of remediation works.

  11. Reanalysis of the Gas-cooled fast reactor experiments at the zero power facility Proteus – Spectral indices

    Directory of Open Access Journals (Sweden)

    Girardin G.

    2013-03-01

    Full Text Available PROTEUS is a zero power reactor at the Paul Scherrer Institute which has been employed during the 1970’s to study experimentally the physics of the gas-cooled fast reactor. Reaction rate distributions, flux spectrum and reactivity effects have been measured in several configurations featuring PuO2/UO2 fuel, absorbers, large iron shields, and thorium oxide and thorium metal fuel either distributed quasihomogeneously in the reference PuO2/UO2 lattice or introduced in the form of radial and axial blanket zones. This papers focus on the spectral indices – including fission and capture in 232Th and 237Np - measured in the reference PuO2/UO2 lattices and their predictions with an MCNPX model specially developed for the PROTEUS-GCFR core. Predictions were obtained with JEFF-3.1 and -3.11, ENDF/B-VII.0 and VII.1, and JENDL-3.3 and -4.0. A general good agreement was demonstrated. The ratio of 232Th fission to 239Pu fission, however, was under-predicted by 8.7±2.1% and 6.5±2.1% using ENDF/B-VII.0 and VII.1, respectively. Finally, the capture rates in 237Np tended to be underpredicted by the JEFF and JENDL libraries, although the new cross section in JEFF-3.1.1 slightly improved the 237Np capture to 239Pu fission results (3.4±2.4%.

  12. Collective doses to man from dumping of radioactive waste in the Arctic Seas.

    Science.gov (United States)

    Nielsen, S P; Iosjpe, M; Strand, P

    1997-08-25

    A box model for the dispersion of radionuclides in the marine environment covering the Arctic Ocean and the North Atlantic Ocean has been constructed. Collective doses from ingestion pathways have been calculated from unit releases of the radionuclides 3H, 60Co, 63Ni, 90Sr, 129I, 137Cs, 239Pu and 241Am into a fjord on the east coast of NovayaZemlya. The results show that doses for the shorter-lived radionuclides (e.g. 137Cs) are derived mainly from seafood production in the Barents Sea. Doses from the longer-lived radionuclides (e.g. 239Pu) are delivered through marine produce further away from the Arctic Ocean. Collective doses were calculated for two release scenarios, both of which are based on information of the dumping of radioactive waste in the Barents and Kara Seas by the former Soviet Union and on preliminary information from the International Arctic Sea Assessment Programme. A worst-case scenario was assumed according to which all radionuclides in liquid and solid radioactive waste were available for dispersion in the marine environment at the time of dumping. Release of radionuclides from spent nuclear fuel was assumed to take place by direct corrosion of the fuel ignoring the barriers that prevent direct contact between the fuel and the seawater. The second scenario selected assumed that releases of radionuclides from spent nuclear fuel do not occur until after failure of the protective barriers. All other liquid and solid radioactive waste was assumed to be available for dispersion at the time of discharge in both scenarios. The estimated collective dose for the worst-case scenario was about 9 manSv and that for the second scenario was about 3 manSv. In both cases, 137Cs is the radionuclide predicted to dominate the collective doses as well as the peak collective dose rates.

  13. ENDF/B-VII.1 library - current and future trends in reaction data

    Science.gov (United States)

    Herman, Michal

    2011-10-01

    The ENDF/B-VII.0 library, made available in December 2006, has been the first major release of the US nuclear reaction data library in 16 years. Intensive validation proved generally good performance of the library but a number of deficiencies were discerned. In 2008 CSEWG decided to undertake multi-laboratory effort leading to VII.1 version, which is scheduled for release in December 2011. Highlights of the new library include (i) a consistent set of covariance data, for over 180 materials, targeting explicit needs of the Advanced Fuel Cycle Initiative, (ii) new R-matrix based evaluations for several light nuclei, (iii) evaluations for reactions on structural materials in both the fast neutron region and the resonance region, (iv) improvements of resonances regions and thermal cross sections for certain fission products and neutron absorber materials (Cd, Gd), (v) improvements in minor actinide evaluations for isotopes of U, Np, Pu, and Am, (vi) adoption of JENDL4.0 evaluations for the Cm, Bk, Cf, Es, Fm, and some other minor actinides, (vii) fission product yield advances for fission-spectrum neutrons and 14 MeV neutrons incident on 239Pu, and (viii) a new Decay Data sub-library. No significant changes are expected for the major actinides 235,8U and 239Pu, except reverting delayed neutron data to ENDF/B-VI.8 and adding covariances. Current update concerns only the most important neutron, fission yields, and decay data sub-libraries leaving the remaining 11 sub-libraries unchanged. Open issues and trends for the future releases of the ENDF/B will be discussed.

  14. Annual progress report on nuclear data 1992

    Energy Technology Data Exchange (ETDEWEB)

    Hansen, H.H. [ed.

    1993-06-01

    This is the 1992 annual report on nuclear data from the Central Bureau for Nuclear Measurements, Geel (Belgium). Work on standard neutron cross sections included {sup 235}U(n,f)/H(n,n) with Frisch gridded ionization chambers and using octacosanol samples. Mass, energy, and angular distribution of fission fragments for {sup 237}Np(n,f) from 0.5 to 5.5 MeV neutron energy. Alpha decay probabilities of {sup 239}Pu. In the area of nuclear data for fission technology, a measurement on the normalization of the {sup 239}Pu fission cross sections was performed. Parameters for 384 resonances in {sup 58}Ni and 350 resonances in {sup 60}Ni have been analyzed up to 1 MeV and 800 KeV, respectively. In the field of nuclear data for fusion technology, double differential neutron emission cross sections for {sup 9}Be(n,2n) for incident neutron energies between 0. 6 and 11.1 MeV have been reported. Extensive measurements of the neutron decay cross sections of {sup 207}Pb have been made. In the radionuclide metrology subproject contributions were made by the preparation of low energy x-ray standard sources, measurements of K- shell fluorescence yields, standardization of a {sup 152}Eu solution, evaluation of the second EUROMET intercomparison of {sup 192}Ir brachytherapy sources, and low level measurements on volcanic rock, archeological ceramics, soil and river sediments. Work was also reported in neutron metrology, major facilities upgrades, radiation physics, and support for a number of PhD projects.

  15. Processing Neutron Cross Section Covariances using NJOY-99 and PUFF-IV

    Energy Technology Data Exchange (ETDEWEB)

    Arcilla,R.; Kahler, A.C.; Oblozinsky, P.; Herman, M.

    2008-06-24

    With the growing demand for multigroup covariances, the National Nuclear Data Center (NNDC) has been experiencing an upsurge in its covariance data processing activities using the two US codes NJOY-99 (LANL) and PUFF-IV (ORNL). The code NJOY-99 was upgraded by incorporating the new module ERRORJ-2.3, while the NNDC served as the active user and provided feedback. The NNDC has been primarily processing neutron cross section covariances on its 64-bit Linux cluster in support of two DOE programs, the Global Nuclear Energy Partnership (GNEP) and the Nuclear Criticality Safety Program (NCSP). For GNEP, the NNDC used NJOY-99.259 to generate multigroup covariance matrices of {sup 56}Fe, {sup 23}Na, {sup 239}Pu, {sup 235}U and {sup 238}U from the JENDL-3.3 library using the 15-, 33-, and 230-energy group structures. These covariance matrices will be used to test a new collapsing algorithm which will subsequently be employed to calculate uncertainties on integral parameters in different fast neutron-based systems. For NCSP, we used PUFF-IV 1.0.4 to verify the processability of new evaluated covariance data of {sup 55}Mn, {sup 239}Pu, {sup 233}U, {sup 235}U and {sup 238}U generated by a collaboration of ORNL and LANL. For the data end-users at large, the NNDC has made available a Web site which provides a static visualization interface for all materials with covariance data in the four major data libraries: ENDF/B-VI.8 (47 materials), ENDF/B-VII.0 (26 materials), JEFF-3.1 (37 materials) and JENDL-3.3 (20 materials).

  16. The plutonium isotopic composition of marine biota on Enewetak Atoll: a preliminary assessment.

    Science.gov (United States)

    Hamilton, Terry F; Martinelli, Roger E; Kehl, Steven R; McAninch, Jeffrey E

    2008-10-01

    We have determined the level and distribution of gamma-emitting radionuclides, plutonium activity concentrations, and 240Pu/239Pu atom ratios in tissue samples of giant clam (Tridacna gigas and Hippopus hippopus), a top snail (Trochus nilaticas) and sea cucumber (Holothuria atra) collected from different locations around Enewetak Atoll. The plutonium isotopic measurements were performed using ultra-high sensitivity accelerator mass spectrometry (AMS). Elevated levels of plutonium were observed in the stomachs (includes the stomach lining) of Tridacna clam (0.62 to 2.98 Bq kg(-1), wet wt.), in the soft parts (edible portion) of top snails (0.25 to 1.7 Bq kg(-1)), wet wt.) and, to a lesser extent, in sea cucumber (0.015 to 0.22 Bq kg(-1), wet wt.) relative to muscle tissue concentrations in clam (0.006 to 0.021 Bq kg(-1), wet wt.) and in comparison with previous measurements of plutonium in fish. These data and information provide a basis for re-evaluating the relative significance of dietary intakes of plutonium from marine foods on Enewetak Atoll and, perhaps most importantly, demonstrate that discrete 240Pu239Pu isotope signatures might well provide a useful investigative tool to monitor source-term attribution and consequences on Enewetak Atoll. One potential application of immediate interest is to monitor and assess the health and ecological impacts of leakage of plutonium (as well as other radionuclides) from a low-level radioactive waste repository on Runit Island relative to background levels of fallout contamination in Enewetak Atoll lagoon.

  17. The mechanism of the hydrothermal alteration of cerium- and plutonium-doped zirconolite

    Science.gov (United States)

    Pöml, P.; Geisler, T.; Cobos-Sabaté, J.; Wiss, T.; Raison, P. E.; Schmid-Beurmann, P.; Deschanels, X.; Jégou, C.; Heimink, J.; Putnis, A.

    2011-03-01

    A comprehensive study on the aqueous stability of Ce- and Pu-doped zirconolite has been performed. Four series of hydrothermal experiments were carried out with Ce-doped zirconolite powders: (1) a solution series (1 M HCl, 2 M NaCl, 1 M NaOH, 1 M NH 3, pure H 2O), (2) a temperature series ( T = 100-300 °C), (3) a surface area-to-fluid volume ratio series, and (4) a series using different reactor materials (Teflon ©, Ni, and Ag). In addition, experiments on 238Pu- and 239Pu-doped zirconolite ceramics in a 1 M HCl solution have been performed. The 238Pu-doped zirconolite had already accumulated significant radiation damage and was X-ray amorphous, while the 239Pu-doped zirconolite was still well-crystalline. The results of the different experimental series can be summarized as follows: (1) After 14 days the degree of alteration is insignificant for all solutions other than 1 M HCl, which was therefore used for all other experimental series; (2) TiO 2 and m-ZrO 2 replaced the zirconolite grains to varying degrees in the 1 M HCl solution, i.e., zirconolite dissolution is incongruent; (3) the degree of alteration increases only slightly with increasing temperature; (4) the alteration rate is independent on the surface to volume ratio; (5) Ag dissolved from the silver reactors dramatically increases the reaction rate, while Ni from the Ni reactors reduces the solubility of Ti and Zr in the HCl solution, indicating that background electrolytes have a strong effect on the alteration rate. From the experiment with the Pu-doped samples at 200 °C in a 1 M HCl solution it was found that the amorphous 238Pu-doped zirconolite was altered to a significantly greater extent than the crystalline counterparts. The results suggest a coupled dissolution-reprecipitation mechanism, which is discussed in detail.

  18. MATERIAL PROPERTIES OF PLUTONIUM-BEARING OXIDES STORED IN STAINLESS STEEL CONTAINERS

    Energy Technology Data Exchange (ETDEWEB)

    Kessinger, G.; Almond, P.; Bridges, N.; Bronikowski, M.; Crowder, M.; Duffey, J.; Livingston, R.; Mcelwee, M.; Missimer, D.; Scogin, J.; Summer, M.; Jurgensen, A.

    2010-02-01

    The destructive examination (DE) of 3013 containers after storage is part of the Surveillance and Monitoring Program based on the Department of Energy's standard for long-term storage of Pu (DOE-STD-3013). The stored, Pu-bearing materials may contain alkali halide contamination that varies from trace amounts of salt to about 50 weight percent, with smaller fractions of other compounds and oxides. These materials were characterized prior to packaging, and surveillance characterizations are conducted to determine the behavior of the materials during long term storage. The surveillance characterization results are generally in agreement with the pre-surveillance data. The predominant phases identified by X-ray diffraction are in agreement with the expected phase assemblages of the as-received materials. The measured densities are in reasonable agreement with the expected densities of materials containing the fraction of salts and actinide oxide specified by the pre-surveillance data. The radiochemical results are generally in good agreement with the pre-surveillance data for mixtures containing 'weapons grade' Pu (nominally 94% {sup 239}Pu and 6% {sup 240}Pu); however, the ICP-MS results from the present investigation generally produce lower concentrations of Pu than the pre-surveillance analyses. For mixtures containing 'fuel grade' Pu (nominally 81-93% {sup 239}Pu and 7-19% {sup 240}Pu), the ICP-MS results from the present investigation appear to be in better agreement with the pre-surveillance data than the radiochemistry results.

  19. Measurement of fallout radionuclides, (239)(,240)Pu and (137)Cs, in soil and creek sediment: Sydney Basin, Australia.

    Science.gov (United States)

    Smith, B S; Child, D P; Fierro, D; Harrison, J J; Heijnis, H; Hotchkis, M A C; Johansen, M P; Marx, S; Payne, T E; Zawadzki, A

    2016-01-01

    Soil and sediment samples from the Sydney basin were measured to ascertain fallout radionuclide activity concentrations and atom ratios. Caesium-137 ((137)Cs) was measured using gamma spectroscopy, and plutonium isotopes ((239)Pu and (240)Pu) were quantified using accelerator mass spectrometry (AMS). Fallout radionuclide activity concentrations were variable ranging from 0.6 to 26.1 Bq/kg for (137)Cs and 0.02-0.52 Bq/kg for (239+240)Pu. Radionuclides in creek sediment samples were an order of magnitude lower than in soils. (137)Cs and (239+240)Pu activity concentration in soils were well correlated (r(2) = 0.80) although some deviation was observed in samples collected at higher elevations. Soil ratios of (137)Cs/(239+240)Pu (decay corrected to 1/1/2014) ranged from 11.5 to 52.1 (average = 37.0 ± 12.4) and showed more variability than previous studies. (240)Pu/(239)Pu atom ratios ranged from 0.117 to 0.165 with an average of 0.146 (±0.013) and an error weighted mean of 0.138 (±0.001). These ratios are lower than a previously reported ratio for Sydney, and lower than the global average. However, these ratios are similar to those reported for other sites within Australia that are located away from former weapons testing sites and indicate that atom ratio measurements from other parts of the world are unlikely to be applicable to the Australian context.

  20. Airborne Plutonium and non-natural Uranium from the Fukushima DNPP found at 120 km distance a few days after reactor hydrogen explosions.

    Science.gov (United States)

    Shinonaga, Taeko; Steier, Peter; Lagos, Markus; Ohkura, Takehisa

    2014-04-01

    Plutonium (Pu) and non-natural uranium (U) originating from the Fukushima Daiichi Nuclear Power Plant (FDNPP) were identified in the atmosphere at 120 km distance from the FDNPP analyzing the ratio of number of atoms, following written as n(isotope)/n(isotope), of Pu and U. The n((240)Pu)/n((239)Pu), n((241)Pu)/n((239)Pu), n((234)U)/n((238)U), n((235)U)/n((238)U) and n((236)U)/n((238)U) in aerosol samples collected before and after the FDNPP incident were analyzed by accelerator mass spectrometry (AMS) and inductively coupled plasma mass spectrometry (ICPMS). The activity concentrations of (137)Cs and (134)Cs in the same samples were also analyzed by gamma spectrometry before the destructive analysis. Comparing the time series of analytical data on Pu and U obtained in this study with previously reported data on Pu, U, and radioactive Cs, we concluded that Pu and non-natural U from the FDNPP were transported in the atmosphere directly over a 120 km distance by aerosol and wind within a few days after the reactor hydrogen explosions. Effective dose of Pu were calculated using the data of Pu: (130 ± 21) nBq/m(3), obtained in this study. We found that the airborne Pu contributes only negligibly to the total dose at the time of the incident. However the analytical results show that the amount of Pu and non-natural U certainly increased in the environment after the incident.

  1. Methodology using a portable X-ray fluorescence device for on-site and rapid evaluation of heavy-atom contamination in wounds: a model study for application to plutonium contamination.

    Directory of Open Access Journals (Sweden)

    Hiroshi Yoshii

    Full Text Available Workers decommissioning the Fukushima-Daiichi nuclear power plant damaged from the Great East Japan Earthquake and resulting tsunami are at risk of injury with possible contamination from radioactive heavy atoms including actinides, such as plutonium. We propose a new methodology for on-site and rapid evaluation of heavy-atom contamination in wounds using a portable X-ray fluorescence (XRF device. In the present study, stable lead was used as the model contaminant substitute for radioactive heavy atoms. First, the wound model was developed by placing a liquid blood phantom on an epoxy resin wound phantom contaminated with lead. Next, the correlation between the concentration of contaminant and the XRF peak intensity was formulated considering the thickness of blood exiting the wound. Methods to determine the minimum detection limit (MDL of contaminants at any maximal equivalent dose to the wound by XRF measurement were also established. For example, in this system, at a maximal equivalent dose of 16.5 mSv to the wound and blood thickness of 0.5 mm, the MDL value for lead was 1.2 ppm (3.1 nmol. The radioactivity of 239Pu corresponding to 3.1 nmol is 1.7 kBq, which is lower than the radioactivity of 239Pu contaminating puncture wounds in previous severe accidents. In conclusion, the established methodology could be beneficial for future development of a method to evaluate plutonium contamination in wounds. Highlights: Methodology for evaluation of heavy-atom contamination in a wound was established. A portable X-ray fluorescence device enables on-site, rapid and direct evaluation. This method is expected to be used for evaluation of plutonium contamination in wounds.

  2. Methodology using a portable X-ray fluorescence device for on-site and rapid evaluation of heavy-atom contamination in wounds: a model study for application to plutonium contamination.

    Science.gov (United States)

    Yoshii, Hiroshi; Yanagihara, Kouta; Imaseki, Hitoshi; Hamano, Tsuyoshi; Yamanishi, Hirokuni; Inagaki, Masayo; Sakai, Yasuhiro; Sugiura, Nobuyuki; Kurihara, Osamu; Sakai, Kazuo

    2014-01-01

    Workers decommissioning the Fukushima-Daiichi nuclear power plant damaged from the Great East Japan Earthquake and resulting tsunami are at risk of injury with possible contamination from radioactive heavy atoms including actinides, such as plutonium. We propose a new methodology for on-site and rapid evaluation of heavy-atom contamination in wounds using a portable X-ray fluorescence (XRF) device. In the present study, stable lead was used as the model contaminant substitute for radioactive heavy atoms. First, the wound model was developed by placing a liquid blood phantom on an epoxy resin wound phantom contaminated with lead. Next, the correlation between the concentration of contaminant and the XRF peak intensity was formulated considering the thickness of blood exiting the wound. Methods to determine the minimum detection limit (MDL) of contaminants at any maximal equivalent dose to the wound by XRF measurement were also established. For example, in this system, at a maximal equivalent dose of 16.5 mSv to the wound and blood thickness of 0.5 mm, the MDL value for lead was 1.2 ppm (3.1 nmol). The radioactivity of 239Pu corresponding to 3.1 nmol is 1.7 kBq, which is lower than the radioactivity of 239Pu contaminating puncture wounds in previous severe accidents. In conclusion, the established methodology could be beneficial for future development of a method to evaluate plutonium contamination in wounds. Highlights: Methodology for evaluation of heavy-atom contamination in a wound was established. A portable X-ray fluorescence device enables on-site, rapid and direct evaluation. This method is expected to be used for evaluation of plutonium contamination in wounds.

  3. Individual Radiological Protection Monitoring of Utrok Atoll Residents Based on Whole Body Counting of Cesium-137 (137Cs) and Plutonium Bioassay

    Energy Technology Data Exchange (ETDEWEB)

    Hamilton, T; Kehl, S; Brown, T; Martinelli, R; Hickman, D; Jue, T; Tumey, S; Langston, R

    2007-06-08

    group of people. In general, the results from the whole-body counting measurements of 137Cs are consistent with our knowledge that a key pathway for exposure to residual fallout contamination on Utrok Atoll is low-level chronic uptake of {sup 137}Cs from the consumption of locally grown produce (Robison et al., 1999). The error-weighted, average body burden of {sup 137}Cs measured in Group I and Group II volunteers was 0.31 kBq and 0.62 kBq, respectively. The associated average, annual committed effective dose equivalent (CEDE) delivered to Group I and Group II volunteers from {sup 137}Cs during the year of measurement was 2.1 and 4.0 mrem. For comparative purposes, the annual dose limit for members of the public as recommended by the National Council on Radiation Protection and Measurements (NCRP) and the International Commission on Radiological Protection (ICRP) is 100 mrem. Consequently, specific concerns about elevated levels of {sup 137}Cs uptake and higher risks from radiation exposure to Group I volunteers would be considered unfounded. Moreover, the urinary excretion of plutonium-239 ({sup 239}Pu) from Group I and Group II volunteers is statistically indistinguishable. In this case, the error-weighted, average urinary excretion of {sup 239}Pu from Group I volunteers of 0.10 {mu}Bq per 24-h void with a range between -0.01 and 0.23 {mu}Bq per 24-h void compares with an error-weighted average from Group II volunteers of 0.11 {mu}Bq per 24-h void with a range between -0.20 and 0.47 {mu}Bq per 24-h void. The range in urinary excretion of {sup 239}Pu from Utrok Atoll residents is very similar to that observed for other population groups in the Marshall Islands (Bogen et al., 2006; Hamilton et al., 2006a; 2006b; 2006c, 2007a; 2007b; 2007c) and is generally considered representative of worldwide background.

  4. The industrial development of atomic energy; Le developpement industriel de l'energie atomique

    Energy Technology Data Exchange (ETDEWEB)

    Kowarski, L. [Commissariat a l' Energie Atomique, Paris (France). Centre d' Etudes Nucleaires

    1955-07-01

    Countries with large stock of fissile material and producing large quantity of nuclear pure {sup 235}U and {sup 239}Pu are able to allocate part of the stock to non military research. For countries with low stock of fissile material, all the stock is allocated to military research. An economical and technical solution has to be find to dedicate a part of fissile material to non military research and develop the atomic energy industry. It stated the industrial and economical problems and in particular the choice between the use of enriched fuel with high refining cost or depleted fuel with low production cost. It discusses of four possible utilizations of the natural resources: reactors functioning with pure fissile material ({sup 235}U or {sup 239}Pu) or concentrated material ({sup 235}U mixed with small quantities of {sup 238}U after an incomplete isotopic separation), breeder reactors functioning with enriched material mixed with {sup 238}U or Thorium placed in an appropriate spatial distribution to allow neutrons beam to activate {sup 238}U or Thorium with the regeneration of fissile material in {sup 239}Pu, reactors using natural uranium or low enriched uranium can also produce Plutonium with less efficiency than breeder reactors and the last solution being the use of natural uranium with the only scope of energy production and no production of secondary fissile material. The first class using pure fissile material has a low energy efficiency and is used only by large fissile material stock countries to accumulate energy in small size fuel for nuclear engines researches for submarines and warships. The advantage of the second class of reactors, breeder reactors, is that they produce energy and plutonium. Two type of breeder reactor are considered: breeder reactor using pure fissile material and {sup 238}U or breeder reactor using the promising mixture of pure fissile material and Thorium. Different projects are in phase of development in United States, England

  5. Prompt Fission Neutron Spectra of Actinides

    Energy Technology Data Exchange (ETDEWEB)

    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

  6. Neutronic assessment of liquid-metal cooled fast reactors using thorium fuel

    Energy Technology Data Exchange (ETDEWEB)

    Pilarski, Stevan [Electricite de France R et D, 1 Avenue du General de Gaulle, 92141 Clamart (France); Institut de Physique Nucleaire d' Orsay, 15 rue Georges Clemenceau 91406 Orsay (France)

    2009-06-15

    The long-term sustainability of atomic fission energy will require the development of new types of reactors, able to exceed the limits of the existing ones in terms of optimal use of natural resources, which clearly necessitates breeding of fissile material. In this context, fast reactors using uranium-plutonium fuel are the most mature solution from an industrial viewpoint. In addition to the obvious interest in terms of fuel resources, there is a major incentive to consider the use of the {sup 232}Th- {sup 233}U fuel cycle as an alternative to the traditional {sup 238}U-{sup 239}Pu cycle for fast reactors: it is an effective way of addressing the safety issue of the highly positive void reactivity effect, which is a well-known problem for liquid-metal cooled fast reactors of commercial size [1]. This work investigates the performance of liquid-metal cooled fast reactors in {sup 232}Th-{sup 233}U fuel cycle and draws a comparison with the traditional {sup 238}U-{sup 239}Pu cycle. Four coolants have been considered: Na, Pb, Mg(17%at.)-Pb and Li(17%at.)-Pb; a simulation of their use in cores ranging from 700 MWth to 3600 MWth has been performed in two-dimensional diffusion theory using the European system of codes ERANOS [2,3] developed at CEA. The performance parameters such as the breeding ratio have been computed for each concept, alongside safety-related parameters: the delayed neutron fraction, the cycle reactivity swing, the Doppler constant and other thermal feedbacks. More specifically, the issue of void reactivity is studied in detail using perturbation theory. These calculations are performed at equilibrium fuel composition and are complemented by the study of the initial fuel loading at start-up which is a mixture of {sup 232}Th-{sup 239}Pu. The isotopic composition of the fissile corresponds to the plutonium available from French reactors in 2035. The conclusions of this work are that near-zero to large negative void reactivity effects can be achieved in

  7. Low-Level Plutonium Bioassay Measurements at the Lawrence Livermore National Laboratory

    Energy Technology Data Exchange (ETDEWEB)

    Hamilton, T; Brown, T; Hickman, D; Marchetti, A; Williams, R; Kehl, S

    2007-06-18

    Plutonium-239 ({sup 239}Pu) and plutonium-240 ({sup 240}Pu) are important alpha emitting radionuclides contained in radioactive debris from nuclear weapons testing. {sup 239}Pu and {sup 240}Pu are long-lived radionuclides with half-lives of 24,400 years and 6580 years, respectively. Concerns over human exposure to plutonium stem from knowledge about the persistence of plutonium isotopes in the environment and the high relative effectiveness of alpha-radiation to cause potential harm to cells once incorporated into the human body. In vitro bioassay tests have been developed to assess uptakes of plutonium based on measured urinary excretion patterns and modeled metabolic behaviors of the absorbed radionuclides. Systemic plutonium absorbed by the deep lung or from the gastrointestinal tract after ingestion is either excreted or distributed to other organs, primarily to the liver and skeleton, where it is retained for biological half-times of around 20 and 50 years, respectively. Dose assessment and atoll rehabilitation programs in the Marshall Islands have historically given special consideration to residual concentrations of plutonium in the environment even though the predicted dose from inhalation and/or ingestion of plutonium accounts for less than 5% of the annual effective dose from exposure to fallout contamination. Scientists from the Lawrence Livermore National Laboratory (LLNL) have developed a state-of-the-art bioassay test to assess urinary excretion rates of plutonium from Marshallese populations. This new heavy-isotope measurement system is based on Accelerator Mass Spectrometry (AMS). The AMS system at LLNL far exceeds the standard measurement requirements established under the latest United States Department of Energy (DOE) regulation, 10CFR 835, for occupational monitoring of plutonium, and offers several advantages over classical as well as competing new technologies for low-level detection and measurement of plutonium isotopes. The United States

  8. Elemental bio-imaging of thorium, uranium, and plutonium in tissues from occupationally exposed former nuclear workers.

    Science.gov (United States)

    Hare, Dominic; Tolmachev, Sergei; James, Anthony; Bishop, David; Austin, Christine; Fryer, Fred; Doble, Philip

    2010-04-15

    Internal exposure from naturally occurring radionuclides (including the inhaled long-lived actinides (232)Th and (238)U) is a component of the ubiquitous background radiation dose (National Council on Radiation Protection and Measurements. Ionizing radiation exposure of the population of the United States; NCRP Report No. 160; NCRP: Bethesda, MD, 2009). It is of interest to compare the concentration distribution of these natural alpha-emitters in the lungs and respiratory lymph nodes with those resulting from occupational exposure, including exposure to anthropogenic plutonium and depleted and enriched uranium. This study examines the application of laser ablation-inductively coupled plasma-mass spectrometry (LA-ICPMS) to quantifying and visualizing the mass distribution of uranium and thorium isotopes from both occupational and natural background exposure in human respiratory tissues and, for the first time, extends this application to the direct imaging of plutonium isotopes. Sections of lymphatic and lung tissues taken from deceased former nuclear workers with a known history of occupational exposure to specific actinide elements (uranium, plutonium, or americium) were analyzed by LA-ICPMS. Using a previously developed LA-ICPMS protocol for elemental bio-imaging of trace elements in human tissue and a new software tool, we generated images of thorium ((232)Th), uranium ((235)U and (238)U), and plutonium ((239)Pu and (240)Pu) mass distributions in sections of tissue. We used a laboratory-produced matrix-matched standard to quantify the (232)Th, (235)U, and (238)U concentrations. The plutonium isotopes (239)Pu and (240)Pu were detected by LA-ICPMS in 65 mum diameter localized regions of both a paratracheal lymph node and a sample of lung tissue from a person who was occupationally exposed to refractory plutonium (plutonium dioxide). The average (overall) (239)Pu concentration in the lymph node was 39.2 ng/g, measured by high purity germanium (HPGe) gamma

  9. Lead Slowing-Down Spectrometry for Spent Fuel Assay: FY12 Status Report

    Energy Technology Data Exchange (ETDEWEB)

    Warren, Glen A.; Anderson, Kevin K.; Casella, Andrew M.; Danon, Yaron; Devlin, M.; Gavron, A.; Haight, R. C.; Harris, Jason; Imel, G. R.; Kulisek, Jonathan A.; O' Donnell, J. M.; Stewart, T.; Weltz, Adam

    2012-10-01

    benchmarking measurements, we continue to improve our understanding of the experimental setup by studying issues such as the effect of room return and impurities in the lead. RPI performed a series of experiments with a fresh fuel pin and various 235U and 239Pu sources. A comparison between simulations and measurements shows significant deviations after 200 µs for both 235U and 239Pu samples, as well as significant deviations at earlier times for the 239Pu sample. The FY2013 effort will shift focus to planning for a Technical Readiness Level 5 demonstration. The primary deliverable for the year will be a plan on how to do this demonstration. The plan will include measurement design, sample acquisition, sample handling, cost estimate, schedule and assumptions. Research will continue on the 4He detector, algorithms development, thorium fission chambers and benchmarking measurements involving sub assemblies of fresh fuel.

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

    Energy Technology Data Exchange (ETDEWEB)

    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

  11. Measurements with the high flux lead slowing-down spectrometer at LANL

    Energy Technology Data Exchange (ETDEWEB)

    Danon, Y. [Rensselaer Polytechnic Intstitute, 110 8th Street, Troy, NY 12180 (United States)]. E-mail: danony@rpi.edu; Romano, C. [Rensselaer Polytechnic Intstitute, 110 8th Street, Troy, NY 12180 (United States); Thompson, J. [Rensselaer Polytechnic Intstitute, 110 8th Street, Troy, NY 12180 (United States); Watson, T. [Rensselaer Polytechnic Intstitute, 110 8th Street, Troy, NY 12180 (United States); Haight, R.C. [Los Alamos National Laboratory, Los Alamos, NM 87545 (United States); Wender, S.A. [Los Alamos National Laboratory, Los Alamos, NM 87545 (United States); Vieira, D.J. [Los Alamos National Laboratory, Los Alamos, NM 87545 (United States); Bond, E. [Los Alamos National Laboratory, Los Alamos, NM 87545 (United States); Wilhelmy, J.B. [Los Alamos National Laboratory, Los Alamos, NM 87545 (United States); O' Donnell, J.M. [Los Alamos National Laboratory, Los Alamos, NM 87545 (United States); Michaudon, A. [Los Alamos National Laboratory, Los Alamos, NM 87545 (United States); Bredeweg, T.A. [Los Alamos National Laboratory, Los Alamos, NM 87545 (United States); Schurman, T. [Los Alamos National Laboratory, Los Alamos, NM 87545 (United States); Rochman, D. [Brookhaven National Laboratory National Nuclear Data Center (NNDC), Upton, NY 11973-5000 (United States); Granier, T. [CEA-DAM, BP 12, 91680 Bruyeres-le-Chatel (France); Ethvignot, T. [CEA-DAM, BP 12, 91680 Bruyeres-le-Chatel (France); Taieb, J. [CEA-DAM, BP 12, 91680 Bruyeres-le-Chatel (France); Becker, J.A. [Lawrence Livermore National Laboratory, Livermore, CA 94550 (United States)

    2007-08-15

    A Lead Slowing-Down Spectrometer (LSDS) was recently installed at LANL [D. Rochman, R.C. Haight, J.M. O'Donnell, A. Michaudon, S.A. Wender, D.J. Vieira, E.M. Bond, T.A. Bredeweg, A. Kronenberg, J.B. Wilhelmy, T. Ethvignot, T. Granier, M. Petit, Y. Danon, Characteristics of a lead slowing-down spectrometer coupled to the LANSCE accelerator, Nucl. Instr. and Meth. A 550 (2005) 397]. The LSDS is comprised of a cube of pure lead 1.2 m on the side, with a spallation pulsed neutron source in its center. The LSDS is driven by 800 MeV protons with a time-averaged current of up to 1 {mu}A, pulse widths of 0.05-0.25 {mu}s and a repetition rate of 20-40 Hz. Spallation neutrons are created by directing the proton beam into an air-cooled tungsten target in the center of the lead cube. The neutrons slow down by scattering interactions with the lead and thus enable measurements of neutron-induced reaction rates as a function of the slowing-down time, which correlates to neutron energy. The advantage of an LSDS as a neutron spectrometer is that the neutron flux is 3-4 orders of magnitude higher than a standard time-of-flight experiment at the equivalent flight path, 5.6 m. The effective energy range is 0.1 eV to 100 keV with a typical energy resolution of 30% from 1 eV to 10 keV. The average neutron flux between 1 and 10 keV is about 1.7 x 10{sup 9} n/cm{sup 2}/s/{mu}A. This high flux makes the LSDS an important tool for neutron-induced cross section measurements of ultra-small samples (nanograms) or of samples with very low cross sections. The LSDS at LANL was initially built in order to measure the fission cross section of the short-lived metastable isotope of U-235, however it can also be used to measure (n, {alpha}) and (n, p) reactions. Fission cross section measurements were made with samples of {sup 235}U, {sup 236}U, {sup 238}U and {sup 239}Pu. The smallest sample measured was 10 ng of {sup 239}Pu. Measurement of (n, {alpha}) cross section with 760 ng of Li-6 was also

  12. Measurements with the high flux lead slowing-down spectrometer at LANL

    Science.gov (United States)

    Danon, Y.; Romano, C.; Thompson, J.; Watson, T.; Haight, R. C.; Wender, S. A.; Vieira, D. J.; Bond, E.; Wilhelmy, J. B.; O'Donnell, J. M.; Michaudon, A.; Bredeweg, T. A.; Schurman, T.; Rochman, D.; Granier, T.; Ethvignot, T.; Taieb, J.; Becker, J. A.

    2007-08-01

    A Lead Slowing-Down Spectrometer (LSDS) was recently installed at LANL [D. Rochman, R.C. Haight, J.M. O'Donnell, A. Michaudon, S.A. Wender, D.J. Vieira, E.M. Bond, T.A. Bredeweg, A. Kronenberg, J.B. Wilhelmy, T. Ethvignot, T. Granier, M. Petit, Y. Danon, Characteristics of a lead slowing-down spectrometer coupled to the LANSCE accelerator, Nucl. Instr. and Meth. A 550 (2005) 397]. The LSDS is comprised of a cube of pure lead 1.2 m on the side, with a spallation pulsed neutron source in its center. The LSDS is driven by 800 MeV protons with a time-averaged current of up to 1 μA, pulse widths of 0.05-0.25 μs and a repetition rate of 20-40 Hz. Spallation neutrons are created by directing the proton beam into an air-cooled tungsten target in the center of the lead cube. The neutrons slow down by scattering interactions with the lead and thus enable measurements of neutron-induced reaction rates as a function of the slowing-down time, which correlates to neutron energy. The advantage of an LSDS as a neutron spectrometer is that the neutron flux is 3-4 orders of magnitude higher than a standard time-of-flight experiment at the equivalent flight path, 5.6 m. The effective energy range is 0.1 eV to 100 keV with a typical energy resolution of 30% from 1 eV to 10 keV. The average neutron flux between 1 and 10 keV is about 1.7 × 109 n/cm2/s/μA. This high flux makes the LSDS an important tool for neutron-induced cross section measurements of ultra-small samples (nanograms) or of samples with very low cross sections. The LSDS at LANL was initially built in order to measure the fission cross section of the short-lived metastable isotope of U-235, however it can also be used to measure (n, α) and (n, p) reactions. Fission cross section measurements were made with samples of 235U, 236U, 238U and 239Pu. The smallest sample measured was 10 ng of 239Pu. Measurement of (n, α) cross section with 760 ng of Li-6 was also demonstrated. Possible future cross section measurements

  13. Plutonium and Uranium Atom Ratios and Activity Levels in Cochiti Lake Bottom Sediments Provided by Pueblo de Cochiti

    Energy Technology Data Exchange (ETDEWEB)

    Gallaher, B.M.; Efurd, D.W.; Rokop, D.J.; Benjamin, T.M.

    1999-05-01

    Historical operations at the Los Alamos National Laboratory have contaminated stream sediments with plutonium and other radionuclides. A small portion of these contaminated sediments has been carried by floods into the Rio Grande drainage system, eventually to be trapped by Cochiti Lake located on Pueblo de Cochiti lands approximately 8 km downstream of the Laboratory. In this study, lake bottom sediment samples provided by the Pueblo de Cochiti were analyzed by thermal ionization mass spectrometry to determine plutonium and uranium activity levels and isotopic atom ratios. This specialized analytical method allows us to take isotopic fingerprints of radionuclides found in the sediment and to determine how much plutonium and uranium came from the Laboratory and how much was deposited by worldwide fallout or is natural. Two distinct types of samples were processed: segments of a continuous vertical core of the entire accumulated sediment sequence and other samples from across the lake bottom at the water/sediment interface. Based on measurement of the {sup 240}Pu/{sup 239}Pu atom ratio, Laboratory-derived plutonium is present in eight of nine samples at the core site. On a depth-weighted basis, approximately one-half of the {sup 239}Pu and {sup 240}Pu came from early operations at the Laboratory; the remaining plutonium came from fallout dispersed by above-ground nuclear tests. In contrast to the core site, the samples from the other locations showed little or no evidence of Laboratory-derived plutonium, with more than 90 percent of the plutonium attributable to fallout. The overall amount of plutonium in all the samples is of the same magnitude as other reservoirs in the region. The net increase in plutonium over upstream reservoirs unaffected by Laboratory activities is a maximum of 0.014 pCi/g or 3.5 times. All of the samples reflect natural uranium compositions. Laboratory-derived uranium is not identifiable, presumably because the sediment contains abundant

  14. ENDF/B-VII.1 Nuclear Data for Science and Technology: Cross Sections, Covariances, Fission Product Yields and Decay Data

    Energy Technology Data Exchange (ETDEWEB)

    G. Palmiotti

    2011-12-01

    The ENDF/B-VII.1 library is our latest recommended evaluated nuclear data file for use in nuclear science and technology applications, and incorporates advances made in the five years since the release of ENDF/B-VII.0. These advances focus on neutron cross sections, covariances, fission product yields and decay data, and represent work by the US Cross Section Evaluation Working Group (CSEWG) in nuclear data evaluation that utilizes developments in nuclear theory, modeling, simulation, and experiment. The principal advances in the new library are: (1) An increase in the breadth of neutron reaction cross section coverage, extending from 393 nuclides to 418 nuclides; (2) Covariance uncertainty data for 185 of the most important nuclides, as documented in companion papers in this edition; (3) R-matrix analyses of neutron reactions on light nuclei, including isotopes of He, Li, and Be; (4) Resonance parameter analyses at lower energies and statistical high energy reactions at higher energies for isotopes of F, Cl, K, Ti, V, Mn, Cr, Ni, Zr and W; (5) Modifications to thermal neutron reactions on fission products (isotopes of Mo, Tc, Rh, Ag, Cs, Nd, Sm, Eu) and neutron absorber materials (Cd, Gd); (6) Improved minor actinide evaluations for isotopes of U, Np, Pu, and Am (we are not making changes to the major actinides 235,238U and 239Pu at this point, except for delayed neutron data, and instead we intend to update them after a further period of research in experiment and theory), and our adoption of JENDL-4.0 evaluations for isotopes of Cm, Bk, Cf, Es, Fm, and some other minor actinides; (7) Fission energy release evaluations; (8) Fission product yield advances for fission-spectrum neutrons and 14 MeV neutrons incident on 239Pu; and (9) A new Decay Data sublibrary. Integral validation testing of the ENDF/B-VII.1 library is provided for a variety of quantities: For nuclear criticality, the VII.1 library maintains the generally-good performance seen for VII.0 for a wide

  15. A multi-radionuclide approach to evaluate the suitability of (239+240)Pu as soil erosion tracer.

    Science.gov (United States)

    Meusburger, Katrin; Mabit, Lionel; Ketterer, Michael; Park, Ji-Hyung; Sandor, Tarjan; Porto, Paolo; Alewell, Christine

    2016-10-01

    Fallout radionuclides have been used successfully worldwide as tracers for soil erosion, but relatively few studies exploit the full potential of plutonium (Pu) isotopes. Hence, this study aims to explore the suitability of the plutonium isotopes (239)Pu and (240)Pu as a method to assess soil erosion magnitude by comparison to more established fallout radionuclides such as (137)Cs and (210)Pbex. As test area an erosion affected headwater catchment of the Lake Soyang (South Korea) was selected. All three fallout radionuclides confirmed high erosion rates for agricultural sites (>25tha(-1)yr(-1)). Pu isotopes further allowed determining the origin of the fallout. Both (240)Pu/(239)Pu atomic ratios and (239+240)Pu/(137)Cs activity ratios were close to the global fallout ratio. However, the depth profile of the (239+240)Pu/(137)Cs activity ratios in undisturbed sites showed lower ratios in the top soil increments, which might be due to higher migration rates of (239+240)Pu. The activity ratios further indicated preferential transport of (137)Cs from eroded sites (higher ratio compared to the global fallout) to the depositional sites (smaller ratio). As such the (239+240)Pu/(137)Cs activity ratio offered a new approach to parameterize a particle size correction factor that can be applied when both (137)Cs and (239+240)Pu have the same fallout source. Implementing this particle size correction factor in the conversion of (137)Cs inventories resulted in comparable estimates of soil loss for (137)Cs and (239+240)Pu. The comparison among the different fallout radionuclides highlights the suitability of (239+240)Pu through less preferential transport compared to (137)Cs and the possibility to gain information regarding the origin of the fallout. In conclusion, (239+240)Pu is a promising soil erosion tracer, however, since the behaviour i.e. vertical migration in the soil and lateral transport during water erosion was shown to differ from that of (137)Cs, there is a clear

  16. Lead Slowing-Down Spectrometry Time Spectral Analysis for Spent Fuel Assay: FY11 Status Report

    Energy Technology Data Exchange (ETDEWEB)

    Kulisek, Jonathan A.; Anderson, Kevin K.; Bowyer, Sonya M.; Casella, Andrew M.; Gesh, Christopher J.; Warren, Glen A.

    2011-09-30

    Developing a method for the accurate, direct, and independent assay of the fissile isotopes in bulk materials (such as used fuel) from next-generation domestic nuclear fuel cycles is a goal of the Office of Nuclear Energy, Fuel Cycle R&D, Material Protection and Control Technology (MPACT) Campaign. To meet this goal, MPACT supports a multi-institutional collaboration, of which PNNL is a part, to study the feasibility of Lead Slowing Down Spectroscopy (LSDS). This technique is an active nondestructive assay method that has the potential to provide independent, direct measurement of Pu and U isotopic masses in used fuel with an uncertainty considerably lower than the approximately 10% typical of today's confirmatory assay methods. This document is a progress report for FY2011 PNNL analysis and algorithm development. Progress made by PNNL in FY2011 continues to indicate the promise of LSDS analysis and algorithms applied to used fuel. PNNL developed an empirical model based on calibration of the LSDS to responses generated from well-characterized used fuel. The empirical model, which accounts for self-shielding effects using empirical basis vectors calculated from the singular value decomposition (SVD) of a matrix containing the true self-shielding functions of the used fuel assembly models. The potential for the direct and independent assay of the sum of the masses of 239Pu and 241Pu to within approximately 3% over a wide used fuel parameter space was demonstrated. Also, in FY2011, PNNL continued to develop an analytical model. Such efforts included the addition of six more non-fissile absorbers in the analytical shielding function and the non-uniformity of the neutron flux across the LSDS assay chamber. A hybrid analytical-empirical approach was developed to determine the mass of total Pu (sum of the masses of 239Pu, 240Pu, and 241Pu), which is an important quantity in safeguards. Results using this hybrid method were of approximately the same accuracy as the

  17. A Delayed Neutron Counting System for the Analysis of Special Nuclear Materials

    Science.gov (United States)

    Sellers, Madison Theresa

    Nuclear forensic analysis is a modem science that uses numerous analytical techniques to identify and attribute nuclear materials in the event of a nuclear explosion, radiological terrorist attack or the interception of illicit nuclear material smuggling. The Canadian Department of National Defence has participated in recent international exercises that have highlighted the Nation's requirement to develop nuclear forensics expertise, protocol and capabilities, specifically pertaining to the analysis of special nuclear materials (SNM). A delayed neutron counting (DNC) system has been designed and established at the Royal Military College of Canada (RMC) to enhance the Government's SNM analysis capabilities. This analytical technique complements those already at RMC by providing a rapid and non-destructive method for the analysis of the fissile isotopes of both uranium (U) and plutonium (Pu). The SLOWPOKE-2 reactor at RMC produces a predominately thermal neutron flux. These neutrons induce fission in the SNM isotopes 233U, 235U and 239Pu releasing prompt fast neutrons, energy and radioactive fission fragments. Some of these fission fragments undergo beta - decay and subsequently emit neutrons, which can be recorded by an array of sensitive 3He detectors. The significant time period between the fission process and the release of these neutrons results in their identification as 'delayed neutrons'. The recorded neutron spectrum varies with time and the count rate curve is unique to each fissile isotope. In-house software, developed by this project, can analyze this delayed neutron curve and provides the fissile mass in the sample. Extensive characterization of the DNC system has been performed with natural U samples with 235 U content ranging from 2--7 microg. The system efficiency and dead time behaviour determined by the natural uranium sample analyses were validated by depleted uranium samples with similar quantities of 235 U resulting in a typical relative error of

  18. Plutonium worker dosimetry.

    Science.gov (United States)

    Birchall, Alan; Puncher, M; Harrison, J; Riddell, A; Bailey, M R; Khokryakov, V; Romanov, S

    2010-05-01

    Epidemiological studies of the relationship between risk and internal exposure to plutonium are clearly reliant on the dose estimates used. The International Commission on Radiological Protection (ICRP) is currently reviewing the latest scientific information available on biokinetic models and dosimetry, and it is likely that a number of changes to the existing models will be recommended. The effect of certain changes, particularly to the ICRP model of the respiratory tract, has been investigated for inhaled forms of (239)Pu and uncertainties have also been assessed. Notable effects of possible changes to respiratory tract model assumptions are (1) a reduction in the absorbed dose to target cells in the airways, if changes under consideration are made to the slow clearing fraction and (2) a doubling of absorbed dose to the alveolar region for insoluble forms, if evidence of longer retention times is taken into account. An important factor influencing doses for moderately soluble forms of (239)Pu is the extent of binding of dissolved plutonium to lung tissues and assumptions regarding the extent of binding in the airways. Uncertainty analyses have been performed with prior distributions chosen for application in epidemiological studies. The resulting distributions for dose per unit intake were lognormal with geometric standard deviations of 2.3 and 2.6 for nitrates and oxides, respectively. The wide ranges were due largely to consideration of results for a range of experimental data for the solubility of different forms of nitrate and oxides. The medians of these distributions were a factor of three times higher than calculated using current default ICRP parameter values. For nitrates, this was due to the assumption of a bound fraction, and for oxides due mainly to the assumption of slower alveolar clearance. This study highlights areas where more research is needed to reduce biokinetic uncertainties, including more accurate determination of particle transport rates

  19. Studies on the Precise Measurement of Isotope of Trace Plutonium in Uranium by MC-ICP-MS%多接收电感耦合等离子体质谱法精确测量铀中痕量钚同位素方法研究

    Institute of Scientific and Technical Information of China (English)

    李力力; 李金英; 赵永刚; 常志远; 张继龙; 王同兴

    2009-01-01

    The infinitesimal plutonium impurity was contained in the uranium product obtained by reprocessing. The precise measurement of the isotope ratio of plutonium was beneficial to the identification of the corresponding source of uranium product. Basing on the separation of trace plutonium from uranium matrix, the operating parameters of MC-ICP-MS were studied and optimized for determining the isotope ratio of trace plutonium, such as the adjustment of resolution, selection of mode of ion extraction, elimination of background and interference, etc. The correction method of the mass discrimination was explored for MCICP-MS measuring isotope ratio. The isotope ratio of ~(239)pu/~(240)Pu in two selected uranium products obtained by reprocessing, which was measured and corrected by measuring plutonium reference material. The ratio of uranium and plutonium is more than 10~(10), and the sum of relative uncertainty for plutonium measurement is better than 5%. The measuring method of isotope ratiois establishes for ng · L~(-1) level of plutonium.%经过核燃料后处理得到的铀产品中含有极微量钚杂质,对其同位素组成进行分析有利于对应铀材料的溯源.本工作在铀钚化学分离的基础上,对影响MC-ICP-MS法精确测量痕量钚同位素丰度比值的仪器条件进行了优化,研究了仪器分辨率、离子提取模式的选择、"背景和干扰"等参数的影响,探索研究了MC-ICP-MS上质量偏倚的校正方法.对选择的两个后处理铀产品中痕量钚同位素比进行了测量,当铀钚比例达10~(10)时,测得的~(239)Pu/~(240)Pu相对不确定度优于5%.并且建立了在MC-ICP-MS上测量ng·L~(-1)量级钚同位素丰度比值的方法.

  20. Concentration of Plutonium in Desert Plants From Contaminated Area%钚在放射性污染区沙漠植物中的含量

    Institute of Scientific and Technical Information of China (English)

    徐辉; 金玉仁; 田梅; 李伟平; 王耀芹; 王煜; 曾可

    2012-01-01

    研究沙漠植物中钚的含量,对于评估沙漠植物受钚污染状况,寻找钚指示和超积累植物有重要意义.本文采集某放射性污染区内的植物并分析其中239 Pu的含量,获得7种沙漠植物受239Pu污染的数据,据此分析影响植物体内核素含量的因素.所研究沙漠植物体内239 Pu含量平均值为(1.8士4.9)Bq/kg(干重),明显受到钚的污染.再悬浮是造成植物表面污染严重的重要因素之一.植物体内钚的含量与植物种类、生长期、地表污染程度等密切相关.所研究沙漠植物中钚含量的大小顺序为:河西苣>芦苇>盐穗木>盐生草>黑果枸杞>刚毛柽柳>沙拐枣,其中草本植物中钚的含量均大于木本植物.%The investigation of plutonium in desert plants from contaminated sites contributes to the evaluation of its pollution situation and to the survey of plutonium hyperaccumulator. The concentration of 239Pu in desert plants collected from a contaminated site was determined, and the influence factors were studied. The concentration of 239Pu in plants was (1. 8 + 4. 9) Bq/kg in dry weight, and it means that the plants were contaminated, moreover, the resuspension results in dramatic plutonium pollution of plant surface. The concentration of plutonium in plants depends on species, live stages and the content of plutonium in the rhizosphere soil. The concentration of plutonium in herbage is higher than that in woody plant, and for the seven species of desert plants investigated, it decreases in the order of Hexinia polydichotoma, Phragmites austra-lis, Halostashys caspica, Halogeton arachnoideus, Lycium ruthenicum ,Tamarix hispida and Calligonum aphyllum.

  1. Investigation of environmental samples from Fukushima with respect to uranium and plutonium by AMS; Untersuchung von Umweltproben aus Fukushima in Bezug auf Plutonium und Uran mittels AMS

    Energy Technology Data Exchange (ETDEWEB)

    Schneider, Stephanie

    2017-02-01

    In March 2011, the nuclear power plant Fukushima Dai-ichi was seriously damaged by a tsunami caused by an earthquake. During the accident large quantities of radionuclides, mainly of the volatile elements cesium and iodine, were released to the environment. In small amounts refractory elements such as plutonium and uranium have also been released. Plutonium and the uraniumisotope {sup 236}U have primarily been delivered by human activities in the environment. Large amounts were released during the atmospheric nuclear weapons tests. Additional sources are accidents in nuclear facilities, like Chernobyl. Every source has its own characteristic isotopic composition. It is therefore possible to determine the origin of the contamination by measuring the isotopic ratios of {sup 240}Pu/{sup 239}Pu and {sup 236}U/{sup 238}U. These ratios can be determined by using accelerator mass spectrometry. Due to its high sensitivity, it is possible to measure even small amounts of plutonium and especially of {sup 236}U. These measurements were performed using the compact 500 kV facility ''TANDY'' of ETH Zurich. In 2013 and 2015 vegetation, litter and soil drill core samples were taken in the contaminated area in Fukushima prefecture. In 2015 samples were taken as close to the sampling locations of the 2013 campaign as possible. After isolation of plutonium and uranium by chemical extraction, separate targets were prepared for the measurement. The {sup 240}Pu/{sup 239}Pu ratios indicate global fallout as the plutonium source for most samples. The plutonium of the reactors of Fukushima Dai-ichi is located in the upper layers like in vegetation or litter. From the uranium ratios alone the reactors could not unambigously be identified as the source of {sup 236}U. However, this is plausible in the cases were reactor plutonium was detected. None of the samples contained higher plutonium activity concentrations than in the rest of Japan, caused by global fallout. This

  2. Plutonium in a grassland ecosystem. [Rocky Flats Plant

    Energy Technology Data Exchange (ETDEWEB)

    Little, C.A.

    1976-08-01

    A study was made of plutonium contamination of grassland at the Rocky Flats plant northwest of Denver, Colorado. Of interest were: the definition of major plutonium-containing ecosystem compartments; the relative amounts in those compartments; how those values related to studies done in other geographical areas; whether or not the predominant isotopes, /sup 238/Pu and /sup 239/Pu, behaved differently; and what mechanisms might have allowed for the observed patterns of contamination. Samples of soil, litter, vegetation, arthropods, and small mammals were collected for Pu analysis and mass determination from each of two macroplots. Small aliquots (5 g or less) were analyzed by a rapid liquid scintillation technique and by alpha spectrometry. Of the compartments sampled, greater than 99 percent of the total plutonium was contained in the soil and the concentrations were significantly inversely correlated with distance from the contamination source, depth of the sample, and particle size of the sieved soil samples. The soil data suggested that the distribution of contamination largely resulted from physical transport processes.

  3. SCALE Modeling of Selected Neutronics Test Problems within the OECD UAM LWR’s Benchmark

    Directory of Open Access Journals (Sweden)

    Luigi Mercatali

    2013-01-01

    Full Text Available The OECD UAM Benchmark was launched in 2005 with the objective of determining the uncertainty in the simulation of Light Water Reactors (LWRs system calculations at all the stages of the coupled reactor physics—thermal hydraulics modeling. Within the framework of the “Neutronics Phase” of the Benchmark the solutions of some selected test cases at the cell physics and lattice physics levels are presented. The SCALE 6.1 code package has been used for the neutronics modeling of the selected exercises. Sensitivity and Uncertainty analysis (S/U based on the generalized perturbation theory has been performed in order to assess the uncertainty of the computation of some selected reactor integral parameters due to the uncertainty in the basic nuclear data. As a general trend, it has been found that the main sources of uncertainty are the 238U (n, and the 239Pu nubar for the UOX- and the MOX-fuelled test cases, respectively. Moreover, the reference solutions for the test cases obtained using Monte Carlo methodologies together with a comparison between deterministic and stochastic solutions are presented.

  4. LWR decay heat calculations using a GRS improved ENDF/B-6 based ORIGEN data library

    Energy Technology Data Exchange (ETDEWEB)

    Hesse, U.; Hummelsheim, K.I.; Kilger, R.; Moser, F.E.; Langenbuch, S. [Gesellschaft fur Anlagen- und Reaktorsicherheit (GRS) mbH, Forschungsinstitute, Garching (Germany)

    2008-07-01

    The known ORNL ORIGEN code is widely spread over the world for inventory, activity and decay heat tasks and is used stand-alone or implemented in activation, shielding or burn-up systems. More than 1000 isotopes with more than six coupled neutron capture and radioactive decay channels are handled simultaneously by the code. The characteristics of the calculated inventories, e.g., masses, activities, neutron and photon source terms or the decay heat during short or long decay time steps are achieved by summing over all isotopes, characterized in the ORIGEN libraries. An extended nuclear GRS-ORIGENX data library is now developed for practical appliance. The library was checked for activation tasks of structure material isotopes and for actinide and fission product burn-up calculations compared with experiments and standard methods. The paper is directed to the LWR decay heat calculation features of the new library and shows the differences of dynamical and time integrated results of Endf/B-6 based and older Endf/B-5 based libraries for decay heat tasks compared to fission burst experiments, ANS curves and some other published data. A multi-group time exponential evaluation is given for the fission burst power of {sup 235}U, {sup 238}U, {sup 239}Pu and {sup 241}Pu, to be used in quick LWR reactor accident decay heat calculation tools. (authors)

  5. Determination of the neutron mass; Determinacion de la masa del neutron

    Energy Technology Data Exchange (ETDEWEB)

    Amador V, P.; Chacon R, A.; Arcos P, A.; Rodriguez N, S.; Pinedo S, A.; Vega C, H.R. [Unidad Academica de Estudios Nucleares, Cipres 10, Fracc. La Penuela, 98068 Zacatecas (Mexico)]. e-mail: paus2281@yahoo.com.mx

    2005-07-01

    The binding energy of the deuteron was measured and it was determined the neutron mass starting from the nuclear reaction, {sup 1}{sub 0} n + {sup 1}{sub 1} H {yields}{sup 2}{sub 1} D + {gamma}. The produced photon is soon a gamma ray that is emitted when the hydrogen captures a thermal neutron. The photon energy was measured using two spectrometric systems for gamma rays. A system with a detector of NaI(TI) of 3'' x 3'' and the other one with a High-purity Germanium detector. The first detector has a bigger efficiency and a smaller resolution in comparison with the second detector. The energy of the measured photon is the binding energy of the deuteron. With the measurement of the photon energy and the masses of the proton and of the deuterium it was determined the neutron mass. The value of the mass obtained with both systems it was compared with the value reported in the literature. The nuclear reaction was induced in a volume of paraffin that it was bombing with a source {sup 239} PuBe whose activity is of 3.7 x 10{sup 10} Bq. (Author)

  6. New antineutrino energy spectra predictions from the summation of beta decay branches of the fission products.

    Science.gov (United States)

    Fallot, M; Cormon, S; Estienne, M; Algora, A; Bui, V M; Cucoanes, A; Elnimr, M; Giot, L; Jordan, D; Martino, J; Onillon, A; Porta, A; Pronost, G; Remoto, A; Taín, J L; Yermia, F; Zakari-Issoufou, A-A

    2012-11-16

    In this Letter, we study the impact of the inclusion of the recently measured beta decay properties of the (102;104;105;106;107)Tc, (105)Mo, and (101)Nb nuclei in an updated calculation of the antineutrino energy spectra of the four fissible isotopes (235,238)U and (239,241)Pu. These actinides are the main contributors to the fission processes in pressurized water reactors. The beta feeding probabilities of the above-mentioned Tc, Mo, and Nb isotopes have been found to play a major role in the γ component of the decay heat of (239)Pu, solving a large part of the γ discrepancy in the 4-3000 s range. They have been measured by using the total absorption technique, insensitive to the pandemonium effect. The calculations are performed by using the information available nowadays in the nuclear databases, summing all the contributions of the beta decay branches of the fission products. Our results provide a new prediction of the antineutrino energy spectra of (235)U, (239,241)Pu, and, in particular, (238)U for which no measurement has been published yet. We conclude that new total absorption technique measurements are mandatory to improve the reliability of the predicted spectra.

  7. Characterization of a suspect nuclear fuel rod in a case of illegal international traffic of fissile material.

    Science.gov (United States)

    Capannesi, G; Vicini, C; Rosada, A; Avino, P

    2010-06-15

    This case study describes the characterization of a suspect rod of nuclear fuel seized in Italy: on request of the coroner, the characterization concerned the kind and the conditions of the rod, the amount and the specific characteristics of the species present in it, with particular attention to their possible use chemical and/or nuclear plants. The methodology used was based on radiochemical analyses (gammagraphic and gamma-spectrometry) whereas the comparison was performed by means of a fuel reference element working in the TRIGA nuclear reactor at Research Center of ENEA-Casaccia. The results show clearly how the exhibit was an element of nuclear fuel, how long it was irradiated, and the amount of (239)Pu produced and the (235)U consumed. Finally, even if the seized rod was briefly radiated at the "zero power" and traces of fission products and plutonium were found, it would be still usable as "fresh" fuel in a reactor type TRIGA if it had not been intercepted by Italian police authorities.

  8. Radiation portal monitor with {sup 10}B+ZnS(Ag) neutron detector performance for the detection of special nuclear materials

    Energy Technology Data Exchange (ETDEWEB)

    Guzman G, K. A.; Gallego, E.; Lorente, A.; Ibanez F, S. [Universidad Politecnica de Madrid, Departamento de Ingenieria Energetica, ETSI Industriales, C. Jose Gutierrez Abascal 2, 28006 Madrid (Spain); Vega C, H. R. [Universidad Autonoma de Zacatecas, Unidad Academica de Estudios Nucleares, Cipres No. 10, Fracc. La Penuela, 98068 Zacatecas, Zac. (Mexico); Gonzalez, J. A. [Universidad Politecnica de Madrid, Laboratorio de Ingenieria Nuclear, ETSI Caminos, Canales y Puertos, C. Prof. Aranguren 3, 28040 Madrid (Spain); Mendez, R., E-mail: ingkarenguzman@gmail.com [Centro de Investigaciones Energeticas, Medioambientales y Tecnologicas, Laboratorio de Patrones Neutronicos, Av. Complutense 40, 28040 Madrid (Spain)

    2016-10-15

    In homeland security, neutron detection is used to prevent the smuggling of special nuclear materials. Thermal neutrons are normally detected with {sup 3}He proportional counters, in the radiation portal monitors, Rpms, however due to the {sup 3}He shortage new procedures are being studied. In this work Monte Carlo methods, using the MCNP6 code, have been used to study the neutron detection features of a {sup 10}B+ZnS(Ag) under real conditions inside of a Rpm. The performance for neutron detection was carried out for {sup 252}Cf, {sup 238}U and {sup 239}Pu under different conditions. In order to mimic an actual situation occurring at border areas, a sample of SNM sited inside a vehicle was simulated and the Rpm with {sup 10}B+ZnS(Ag) response was calculated. At 200 cm the {sup 10}B+ZnS(Ag) on Rpm response is close to 2.5 cps-ng {sup 252}Cf, when the {sup 252}Cf neutron source is shielded with 0.5 cm-thick lead and 2.5 cm-thick polyethylene fulfilling the ANSI recommendations. Three different geometries of neutron detectors of {sup 10}B+ZnS(Ag) in a neutron detection system in Rpm were modeled. Therefore, the {sup 10}B+ZnS(Ag) detectors are an innovative and viable replacement for the {sup 3}He detectors in the Rpm. (Author)

  9. Main results of the 2012 joint Norwegian-Russian expedition to the dumping sites of the nuclear submarine K-27 and solid radioactive waste in Stepovogo Fjord, Novaya Zemlya.

    Science.gov (United States)

    Gwynn, Justin P; Nikitin, Aleksander; Shershakov, Viacheslav; Heldal, Hilde Elise; Lind, Bjørn; Teien, Hans-Christian; Lind, Ole Christian; Sidhu, Rajdeep Singh; Bakke, Gunnar; Kazennov, Alexey; Grishin, Denis; Fedorova, Anastasia; Blinova, Oxana; Sværen, Ingrid; Lee Liebig, Penny; Salbu, Brit; Wendell, Cato Christian; Strålberg, Elisabeth; Valetova, Nailja; Petrenko, Galina; Katrich, Ivan; Logoyda, Igor; Osvath, Iolanda; Levy, Isabelle; Bartocci, Jean; Pham, Mai Khanh; Sam, Adam; Nies, Hartmut; Rudjord, Anne Liv

    2016-01-01

    This paper reports the main results of the 2012 joint Norwegian-Russian expedition to investigate the radioecological situation of the Stepovogo Fjord on the eastern coast of Novaya Zemlya, where the nuclear submarine K-27 and solid radioactive waste was dumped. Based on in situ gamma measurements and the analysis of seawater and sediment samples taken around the submarine, there was no indication of any leakage from the reactor units of K-27. With regard to the radioecological status of Stepovogo Fjord, activity concentrations of all radionuclides in seawater, sediment and biota in 2012 were in general lower than reported from the previous investigations in the 1990s. However in 2012, the activity concentrations of (137)Cs and, to a lesser extent, those of (90)Sr remained elevated in bottom water from the inner part of Stepovogo Fjord compared with surface water and the outer part of Stepovogo Fjord. Deviations from expected (238)Pu/(239,240)Pu activity ratios and (240)Pu/(239)Pu atom ratios in some sediment samples from the inner part of Stepovogo Fjord observed in this study and earlier studies may indicate the possibility of leakages from dumped waste from different nuclear sources. Although the current environmental levels of radionuclides in Stepovogo Fjord are not of immediate cause for concern, further monitoring of the situation is warranted. Copyright © 2015 Elsevier Ltd. All rights reserved.

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

    Science.gov (United States)

    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. Copyright © 2015 Elsevier Ltd. All rights reserved.

  11. Mercuric iodide room-temperature array detectors for gamma-ray imaging

    Energy Technology Data Exchange (ETDEWEB)

    Patt, B. [Xsirius, Inc, Camarillo, CA (United States)

    1994-11-15

    Significant progress has been made recently in the development of mercuric iodide detector arrays for gamma-ray imaging, making real the possibility of constructing high-performance small, light-weight, portable gamma-ray imaging systems. New techniques have been applied in detector fabrication and then low noise electronics which have produced pixel arrays with high-energy resolution, high spatial resolution, high gamma stopping efficiency. Measurements of the energy resolution capability have been made on a 19-element protypical array. Pixel energy resolutions of 2.98% fwhm and 3.88% fwhm were obtained at 59 keV (241-Am) and 140-keV (99m-Tc), respectively. The pixel spectra for a 14-element section of the data is shown together with the composition of the overlapped individual pixel spectra. These techniques are now being applied to fabricate much larger arrays with thousands of pixels. Extension of these principles to imaging scenarios involving gamma-ray energies up to several hundred keV is also possible. This would enable imaging of the 208 keV and 375-414 keV 239-Pu and 240-Pu structures, as well as the 186 keV line of 235-U.

  12. Yields and spectroscopy of radioactive isotopes at LOHENGRIN and ISOLDE

    CERN Document Server

    Köster, U

    1999-01-01

    Yields of radioactive nuclei were measured at two facilities: the recoil separator LOHENGRIN at the Institut Laue Langevin in Grenoble and the on-line isotope separator ISOLDE at CERN in Geneva. At LOHENGRIN the yields of light charged particles were measured from thermal neutron induced ternary fission of several actinide targets: 233U, 235U, 239Pu, 241Pu and 245Cm. Thin targets are brought into a high neutron flux. The produced nuclei leave these with the recoil obtained in the fission reaction. They are measured at different energies and ionic charge states. After corrections for the experimental acceptance, the time behaviour of the fission rate and the ionic charge fraction, the yields are integrated over the kinetic energy distribution. Comparing these yields with the predictions of various ternary fission models shows that the most abundant nuclides are well reproduced. On the other hand the models overestimate significantly the production of more "exotic" nuclides with an extreme N/Z ratio. Therefore ...

  13. Uranium comparison by means of AMS and ICP-MS and Pu and 137Cs results around an Italian Nuclear Power Plant

    Directory of Open Access Journals (Sweden)

    De Cesare M.

    2015-01-01

    Full Text Available Italy built and commissioned 4 nuclear power plants between 1958-1978, which delivered a total of 1500 MW. All four were closed down after the Chernobyl accident following a referendum in 1987. One of the plants was Garigliano, commissioned in 1959. This plant used a 160 MW BWR1 (SEU of 2.3 % and was operational from 1964 to 1979, when it was switched off for maintenance. It was definitively stopped in 1982, and is presently being decommissioned. We report here details on the chemistry procedure and on the measurements for soil samples, collected up to 4.5 km from the Nuclear Plant. A comparison between uranium (238U concentration as determined by means of AMS (Accelerator Mass Spectrometry and by ICP-MS (Inductively Coupled Plasma-Mass Spectrometry techniques respectively at the ANU (Australian National University and at the Ecowise company in Canberra, Australia, is reported, as well as 236U and 239;240Pu concentration results detected by AMS. 236U/238U and 240Pu/239Pu isotopic ratios by means of AMS are also provided. A contamination from Chernobyl is visible in the 137Cs/239+240Pu activity ratio measurements.

  14. Measurement of Uranium Isotopes in Particles of U3O8 by Secondary Ion Mass Spectrometry-Single-Stage Accelerator Mass Spectrometry (SIMS-SSAMS).

    Science.gov (United States)

    Fahey, Albert J; Groopman, Evan E; Grabowski, Kenneth S; Fazel, Kamron C

    2016-07-19

    A commercial secondary ion mass spectrometer (SIMS) was coupled to a ± 300 kV single-stage accelerator mass spectrometer (SSAMS). Positive secondary ions generated with the SIMS were injected into the SSAMS for analysis. This combined instrument was used to measure the uranium isotopic ratios in particles of three certified reference materials (CRM) of uranium, CRM U030a, CRM U500, and CRM U850. The ability to inject positive ions into the SSAMS is unique for AMS systems and allows for simple analysis of nearly the entire periodic table because most elements will readily produce positive ions. Isotopic ratios were measured on samples of a few picograms to nanograms of total U. Destruction of UH(+) ions in the stripper tube of the SSAMS reduced hydride levels by a factor of ∼3 × 10(4) giving the UH(+)/U(+) ratio at the SSAMS detector of ∼1.4 × 10(-8). These hydride ion levels would allow the measurement of (239)Pu at the 10 ppb level in the presence of U and the equivalent of ∼10(-10 236)U concentration in natural uranium. SIMS-SSAMS analysis of solid nuclear materials, such as these, with signals nearly free of molecular interferences, could have a significant future impact on the way some measurements are made for nuclear nonproliferation.

  15. Standard test method for nondestructive assay of special nuclear material in low density scrap and waste by segmented passive gamma-Ray scanning

    CERN Document Server

    American Society for Testing and Materials. Philadelphia

    2010-01-01

    1.1 This test method covers the transmission-corrected nondestructive assay (NDA) of gamma-ray emitting special nuclear materials (SNMs), most commonly 235U, 239Pu, and 241Am, in low-density scrap or waste, packaged in cylindrical containers. The method can also be applied to NDA of other gamma-emitting nuclides including fission products. High-resolution gamma-ray spectroscopy is used to detect and measure the nuclides of interest and to measure and correct for gamma-ray attenuation in a series of horizontal segments (collimated gamma detector views) of the container. Corrections are also made for counting losses occasioned by signal processing limitations (1-3). 1.2 There are currently several systems in use or under development for determining the attenuation corrections for NDA of radioisotopic materials (4-8). A related technique, tomographic gamma-ray scanning (TGS), is not included in this test method (9, 10, 11). 1.2.1 This test method will cover two implementations of the Segmented Gamma Scanning ...

  16. Radionuclide migration at the Koongarra uranium deposit, Northern Australia Lessons from the Alligator Rivers analogue project

    Science.gov (United States)

    Payne, Timothy E.; Airey, Peter L.

    The Koongarra uranium deposit in Northern Australia provides a ‘natural analogue’ for processes that are of relevance for assessing the safety of radioactive waste disposal. In an international project extending over two decades, the Koongarra ore body was studied to increase the understanding of radionuclide migration and retention mechanisms that might occur in the vicinity of a geological repository. The research effort included extensive characterisation of the geological, hydrological and geochemical conditions at the site. Patterns of the distribution of radionuclides (predominantly members of the 238U decay chain, but also the rare isotopes 239Pu, 99Tc and 129I) were studied in both solid and groundwater phases. The project included detailed studies of uranium adsorption on mineral surfaces, and of subsequent processes that may lead to long-term uranium immobilisation. Numerous models for uranium migration were developed during the project. This paper provides a comprehensive review of the research at Koongarra, and assesses the value of the site for integrating the results of a complex series of laboratory, modelling and field studies. The insights gained from this review of the Koongarra project may assist in maximising the potential scientific benefit of future natural analogue studies.

  17. Anthropogenic plutonium-244 in the environment: Insights into plutonium's longest-lived isotope.

    Science.gov (United States)

    Armstrong, Christopher R; Brant, Heather A; Nuessle, Patterson R; Hall, Gregory; Cadieux, James R

    2016-02-22

    Owing to the rich history of heavy element production in the unique high flux reactors that operated at the Savannah River Site, USA (SRS) decades ago, trace quantities of plutonium with highly unique isotopic characteristics still persist today in the SRS terrestrial environment. Development of an effective sampling, processing, and analysis strategy enables detailed monitoring of the SRS environment, revealing plutonium isotopic compositions, e.g., (244)Pu, that reflect the unique legacy of plutonium production at SRS. This work describes the first long-term investigation of anthropogenic (244)Pu occurrence in the environment. Environmental samples, consisting of collected foot borne debris, were taken at SRS over an eleven year period, from 2003 to 2014. Separation and purification of trace plutonium was carried out followed by three stage thermal ionization mass spectrometry (3STIMS) measurements for plutonium isotopic content and isotopic ratios. Significant (244)Pu was measured in all of the years sampled with the highest amount observed in 2003. The (244)Pu content, in femtograms (fg = 10(-15) g) per gram, ranged from 0.31 fg/g to 44 fg/g in years 2006 and 2003 respectively. In all years, the (244)Pu/(239)Pu atom ratios were significantly higher than global fallout, ranging from 0.003 to 0.698 in years 2014 and 2003 respectively.

  18. New antineutrino energy spectra predictions from the summation of beta decay branches of the fission products

    CERN Document Server

    Fallot, M; Estienne, M; Algora, A; Bui, V M; Cucoanes, A; Elnimr, M; Giot, L; Jordan, D; Martino, J; Onillon, A; Porta, A; Pronost, G; Taín, J L; Yermia, F; Zakari-Issoufou, A -A

    2012-01-01

    In this paper, we study the impact of the inclusion of the recently measured beta decay properties of the $^{102;104;105;106;107}$Tc, $^{105}$Mo, and $^{101}$Nb nuclei in an updated calculation of the antineutrino energy spectra of the four fissible isotopes $^{235, 238}$U, and $^{239,241}$Pu. These actinides are the main contributors to the fission processes in Pressurized Water Reactors. The beta feeding probabilities of the above-mentioned Tc, Mo and Nb isotopes have been found to play a major role in the $\\gamma$ component of the decay heat of $^{239}$Pu, solving a large part of the $\\gamma$ discrepancy in the 4 to 3000\\,s range. They have been measured using the Total Absorption Technique (TAS), avoiding the Pandemonium effect. The calculations are performed using the information available nowadays in the nuclear databases, summing all the contributions of the beta decay branches of the fission products. Our results provide a new prediction of the antineutrino energy spectra of $^{235}$U, $^{239,241}$Pu ...

  19. Cancer risk at low doses of ionizing radiation: artificial neural networks inference from atomic bomb survivors.

    Science.gov (United States)

    Sasaki, Masao S; Tachibana, Akira; Takeda, Shunichi

    2014-05-01

    Cancer risk at low doses of ionizing radiation remains poorly defined because of ambiguity in the quantitative link to doses below 0.2 Sv in atomic bomb survivors in Hiroshima and Nagasaki arising from limitations in the statistical power and information available on overall radiation dose. To deal with these difficulties, a novel nonparametric statistics based on the 'integrate-and-fire' algorithm of artificial neural networks was developed and tested in cancer databases established by the Radiation Effects Research Foundation. The analysis revealed unique features at low doses that could not be accounted for by nominal exposure dose, including (i) the presence of a threshold that varied with organ, gender and age at exposure, and (ii) a small but significant bumping increase in cancer risk at low doses in Nagasaki that probably reflects internal exposure to (239)Pu. The threshold was distinct from the canonical definition of zero effect in that it was manifested as negative excess relative risk, or suppression of background cancer rates. Such a unique tissue response at low doses of radiation exposure has been implicated in the context of the molecular basis of radiation-environment interplay in favor of recently emerging experimental evidence on DNA double-strand break repair pathway choice and its epigenetic memory by histone marking.

  20. Plutonium partitioning in three-phase systems with water, granite grains, and different colloids.

    Science.gov (United States)

    Xie, Jinchuan; Lin, Jianfeng; Zhou, Xiaohua; Li, Mei; Zhou, Guoqing

    2014-01-01

    Low-solubility contaminants with high affinity for colloid surfaces may form colloid-associated species. The mobile characteristics of this species are, however, ignored by the traditional sorption/distribution experiments in which colloidal species contributed to the immobile fraction of the contaminants retained on the solids as a result of centrifugation or ultrafiltration procedures. The mobility of the contaminants in subsurface environments might be underestimated accordingly. Our results show that colloidal species of (239)Pu in three-phase systems remained the highest percentages in comparison to both the dissolved species and the immobile species retained on the granite grains (solid phase), although the relative fraction of these three species depended on the colloid types. The real solid/liquid distribution coefficients (K s/d) experimentally determined were generally smaller than the traditional K s/d (i.e., the K s+c/d in this study) by ~1,000 mL/g for the three-phase systems with the mineral colloids (granite particle, soil colloid, or kaolinite colloid). For the humic acid system, the traditional K s/d was 140 mL/g, whereas the real K s/d was approximately zero. The deviations from the real solid/liquid K s/d were caused by the artificially increased immobile fraction of Pu. One has to be cautious in using K s/d-based transport models to predict the fate and transport of Pu in the environment.

  1. Dating of sediments from four Swiss prealpine lakes with (210)Pb determined by gamma-spectrometry: progress and problems.

    Science.gov (United States)

    Putyrskaya, V; Klemt, E; Röllin, S; Astner, M; Sahli, H

    2015-07-01

    In this paper the most important problems in dating lake sediments with unsupported (210)Pb are summarized and the progress in gamma-spectrometry of the unsupported (210)Pb is discussed. The main topics of these studies concern sediment samples preparation for gamma-spectrometry, measurement techniques and data analysis, as well as understanding of accumulation and sedimentation processes in lakes. The vertical distributions of artificial ((137)Cs, (241)Am, (239)Pu) and natural radionuclides ((40)K, (210,214)Pb, (214)Bi) as well as stable trace elements (Fe, Mn, Pb) in sediment cores from four Swiss lakes were used as examples for the interpretation, inter-comparison and validation of depth-age relations established by three (210)Pb-based models (CF-CSR, CRS and SIT). The identification of turbidite layers and the influence of the turbidity flows on the accuracy of sediment dating is demonstrated. Time-dependent mass sedimentation rates in lakes Brienz, Thun, Biel and Lucerne are discussed and compared with published data.

  2. Distribution and source of (129)I, (239)(,240)Pu, (137)Cs in the environment of Lithuania.

    Science.gov (United States)

    Ežerinskis, Ž; Hou, X L; Druteikienė, R; Puzas, A; Šapolaitė, J; Gvozdaitė, R; Gudelis, A; Buivydas, Š; Remeikis, V

    2016-01-01

    Fifty five soil samples collected in the Lithuania teritory in 2011 and 2012 were analyzed for (129)I, (137)Cs and Pu isotopes in order to investigate the level and distribution of artificial radioactivity in Lithuania. The activity and atomic ratio of (238)Pu/((239,24)0)Pu, (129)I/(127)I and (131)I/(137)Cs were used to identify the origin of these radionuclides. The (238)Pu/(239+240)Pu and (240)Pu/(239)Pu ratios in the soil samples analyzed varied in the range of 0.02-0.18 and 0.18-0.24, respectively, suggesting the global fallout as the major source of Pu in Lithuania. The values of 10(-9) to 10(-6) for (129)I/(127)I atomic ratio revealed that the source of (129)I in Lithuania is global fallout in most cases though several sampling sites shows a possible impact of reprocessing releases. Estimated (129)I/(131)I ratio in soil samples from the southern part of Lithuania shows negligible input of the Chernobyl fallout. No correlation of the (137)Cs and Pu isotopes with (129)I was observed, indicating their different sources terms. Results demonstrate uneven distribution of these radionuclides in the Lithuanian territory and several sources of contamination i.e. Chernobyl accident, reprocessing releases and global fallout.

  3. Distribution and source of 129I, 239,240Pu, 137Cs in the environment of Lithuania

    DEFF Research Database (Denmark)

    Ezerinskis, Z.; Hou, Xiaolin; Druteikiene, R.;

    2016-01-01

    Fifty five soil samples collected in the Lithuania teritory in 2011 and 2012 were analyzed for 129I, 137Cs and Pu isotopes in order to investigate the level and distribution of artificial radioactivity in Lithuania. The activity and atomic ratio of 238Pu/239,240Pu, 129I/127I and 131I/137Cs were...... used to identify the origin of these radionuclides. The 238Pu/239þ240Pu and 240Pu/239Pu ratios in the soil samples analyzed varied in the range of 0.02e0.18 and 0.18e0.24, respectively, suggesting the global fallout as the major source of Pu in Lithuania. The values of 109 to 106 for 129I/127I atomic...... ratio revealed that the source of 129I in Lithuania is global fallout in most cases though several sampling sites shows a possible impact of reprocessing releases. Estimated 129I/131I ratio in soil samples from the southern part of Lithuania shows negligible input of the Chernobyl fallout...

  4. Assessment of sediment monitoring at LLNL

    Energy Technology Data Exchange (ETDEWEB)

    Gallegos, G.

    1994-03-17

    Three separate sediment monitoring studies have been conducted at the Lawrence Livermore National Laboratory (LLNL) Livermore site. ``Sediment`` is defined here as finely divided solid materials that have settled out of an active stream or standing water. Sediment samples from all three studies were analyzed for a number of contaminants including {sup 239}pu, {sup 3}H, gamma emitting radionuclides, heavy metals, volatile organic compounds and pesticides. The analytical results for metals and organic compounds were compared to limits for disposal of hazardous waste, the tritium values were compared to drinking water standards, and the other radionuclides were compared to soils monitoring values. No tritium values were above (or were greater than 55% of drinking water standards), and no other radionuclides in sediments were above soils values. In all of the studies, only two metals, lead and mercury, and six organic compounds, benzo(a)-pyrene, Dieldrin, p,p{prime}-DDT, Endosulfan L endosulfan sulfate, and vinyl chloride were above waste disposal limits. Three of the high contaminants, mercury, benzo(a)-pyrene, and vinyl chloride, were found at one sampling location; the others were not connected by drainage channels or physical proximity to each other. Overall, a total of 247 samples were analyzed, and the sporadic identification of materials over disposal limits demonstrates that there is negligible contamination of sediment.

  5. Sequestration of radioactive iodine in silver-palladium phases in commercial spent nuclear fuel

    Science.gov (United States)

    Buck, Edgar C.; Mausolf, Edward J.; McNamara, Bruce K.; Soderquist, Chuck Z.; Schwantes, Jon M.

    2016-12-01

    Radioactive iodine is the Achilles' heel in the design for the safe geological disposal of spent uranium oxide (UO2) nuclear fuel. Furthermore, iodine's high volatility and aqueous solubility were mainly responsible for the high early doses released during the accident at Fukushima Daiichi in 2011. Studies Kienzler et al., however, have indicated that the instant release fraction (IRF) of radioiodine (131/129I) does not correlate directly with increasing fuel burn-up. In fact, there is a peak in the release of iodine at around 50-60 MW d/kgU, and with increasing burn-up, the IRF of 131/129I decreases. The reasons for this decrease have not fully been understood. We have performed microscopic analysis of chemically processed high burn-up UO2 fuel (80 MW d/kgU) and have found recalcitrant nano-particles containing, Pd, Ag, I, and Br, possibly consistent with a high pressure phase of silver iodide in the undissolved residue. It is likely that increased levels of Ag and Pd from 239Pu fission in high burnup fuels leads to the formation of these metal halides. The occurrence of these phases in UO2 nuclear fuels may reduce the impact of long-lived 129I on the repository performance assessment calculations.

  6. Neutron imaging of radioactive sources

    Science.gov (United States)

    Hameed, F.; Karimzadeh, S.; Zawisky, M.

    2008-08-01

    Isotopic neutron sources have been available for more than six decades. At the Atomic Institute in Vienna, operating a 250 kW TRIGA reactor, different neutron sources are in use for instrument calibration and fast neutron applications but we have only little information about their construction and densities. The knowledge of source design is essential for a complete MCNP5 modeling of the experiments. Neutron radiography (NR) and neutron tomography (NT) are the best choices for the non-destructive inspection of the source geometry and homogeneity. From the transmission analysis we gain information about the shielding components and the densities of the radio-isotopes in the cores. Three neutron sources, based on (alpha, n) reaction, have been investigated, two 239PuBe sources and one 241AmBe source. In the NR images the internal structure was clearly revealed using high-resolving scintillation and imaging plate detectors. In one source tablet a crack was detected which causes asymmetric neutron emission. The tomography inspection of strong absorbing materials is more challenging due to the low beam intensity of 1.3x105 n/cm2s at our NT instrument, and due to the beam hardening effect which requires an extension of reconstruction software. The tomographic inspection of a PuBe neutron source and appropriate measures for background and beam hardening correction are presented.

  7. Feasibility of fissile mass assay of spent nuclear fuel using {sup 252}Cf-source-driven frequency-analysis

    Energy Technology Data Exchange (ETDEWEB)

    Mattingly, J.K.; Valentine, T.E.; Mihalczo, J.T.

    1996-10-01

    The feasibility was evaluated using MCNP-DSP, an analog Monte Carlo transport cod to simulate source-driven measurements. Models of an isolated Westinghouse 17x17 PWR fuel assembly in a 1500-ppM borated water storage pool were used. In the models, the fuel burnup profile was represented using seven axial burnup zones, each with isotopics estimated by the PDQ code. Four different fuel assemblies with average burnups from fresh to 32 GWd/MTU were modeled and analyzed. Analysis of the fuel assemblies was simulated by inducing fission in the fuel using a {sup 252}Cf source adjacent to the assembly and correlating source fissions with the response of a bank of {sup 3}He detectors adjacent to the assembly opposite the source. This analysis was performed at 7 different axial positions on each of the 4 assemblies, and the source-detector cross-spectrum signature was calculated for each of these 28 simulated measurements. The magnitude of the cross-spectrum signature follows a smooth upward trend with increasing fissile material ({sup 235}U and {sup 239}Pu) content, and the signature is independent of the concentration of spontaneously fissioning isotopes (e.g., {sup 244}Cm) and ({alpha},n) sources. Furthermore, the cross-spectrum signature is highly sensitive to changes in fissile material content. This feasibility study indicated that the signature would increase {similar_to}100% in response to an increase of only 0.1 g/cm{sup 3} of fissile material.

  8. Energy-Dependent Fission Q Values Generalized for All Actinides

    Energy Technology Data Exchange (ETDEWEB)

    Vogt, R

    2008-09-25

    We generalize Madland's parameterization of the energy release in fission to obtain the dependence of the fission Q values on incident neutron energy, E{sub n}, for all major and minor actinides. These Q(E{sub n}) parameterizations are included in the ENDL2008 release. This paper describes calculations of energy-dependent fission Q values based on parameterizations of the prompt energy release in fission [1], developed by Madland [1] to describe the prompt energy release in neutron-induced fission of {sup 235}U, {sup 238}U, and {sup 239}Pu. The energy release is then related to the energy deposited during fission so that experimentally measurable quantities can be used to obtain the Q values. A discussion of these specific parameterizations and their implementation in the processing code for Monte Carlo neutron transport, MCFGEN, [2] is described in Ref. [3]. We extend this model to describe Q(E) for all actinides, major and minor, in the Evaluated Nuclear Data Library (ENDL) 2008 release, ENDL2008.

  9. New prompt fission neutron spectra measurements in the 238U(n,f) reaction with a dedicated setup at LANSCE/WNR

    Science.gov (United States)

    Laurent, Benoit; Marini, Paola; Bélier, Gilbert; Bonnet, Thomas; Chatillon, Audrey; Taieb, Julien; Etasse, David; Devlin, Matthew; Haight, Robert

    2017-09-01

    A new prompt fission neutron spectra (PFNS) measurement in the 238U(n,f) reaction was performed at LANSCE/WNR facility. Evaluated data show discrepancies on the low (below 1 MeV) and high (above 5 MeV) energy parts in the PFNS for different major and minor actinides. The goal is to improve these measurements in a wide range of incident energy. The energy of the incoming neutron, inducing the fission, and the prompt neutron energies, are measured by time-of-flight method. A dedicated fission chamber was developed, in order to improve alpha-fission discrimination, timing resolution, actinide mass, and to reduce the amount of neutron scattering. To detect prompt neutrons, the 54 Chi-Nu scintillator cells array were surrounding the fission chamber. High statistics were recorded during this experiment, allowing a precise study of PFNS behavior as a function of incident neutron energy, from 1 MeV to 200 MeV. This experiment also showed that all the new tools developed to improve PFNS measurements are performing. Therefore, measurements of PFNS with others actinides such as 239Pu are planned.

  10. Determination of the Sensitivity of the Antineutrino Probe for Reactor Core Monitoring

    Science.gov (United States)

    Cormon, S.; Fallot, M.; Bui, V.-M.; Cucoanes, A.; Estienne, M.; Lenoir, M.; Onillon, A.; Shiba, T.; Yermia, F.; Zakari-Issoufou, A.-A.

    2014-06-01

    This paper presents a feasibility study of the use of the detection of reactor-antineutrinos (νbare) for non proliferation purpose. To proceed, we have started to study different reactor designs with our simulation tools. We use a package called MCNP Utility for Reactor Evolution (MURE), initially developed by CNRS/IN2P3 labs to study Generation IV reactors. The MURE package has been coupled to fission product beta decay nuclear databases for studying reactor antineutrino emission. This method is the only one able to predict the antineutrino emission from future reactor cores, which don't use the thermal fission of 235U, 239Pu and 241Pu. It is also the only way to include off-equilibrium effects, due to neutron captures and time evolution of the fission product concentrations during a reactor cycle. We will present here the first predictions of antineutrino energy spectra from innovative reactor designs (Generation IV reactors). We will then discuss a summary of our results of non-proliferation scenarios involving the latter reactor designs, taking into account reactor physics constraints.

  11. The feasibility of using Pu discharges from Sellafield to investigate the sediment dynamics of the Severn Estuary and the Welsh coast

    Energy Technology Data Exchange (ETDEWEB)

    Dunne, J.A.; Richards, D.A. [School of Geographical Sciences and Bristol Isotope Group, University of Bristol (United Kingdom)

    2014-07-01

    Decades of nuclear weapons testing and very low level radioactive waste discharges from civil nuclear sites have resulted in a global distribution of Pu isotopes. Given that the sources of these isotopes are spatially and temporally well-known, their distribution throughout the environment can provide insight into the processes that have governed their dispersal. Plutonium-239 and {sup 240}Pu have long half-lives and their atomic abundance ratio is indicative of the source, be it atmospheric fallout or releases from the nuclear industry. Plutonium is also strongly adsorbed on sediments. These characteristics make Pu an excellent tool for monitoring ocean currents, tracking sediment transport and examining the fate of the products of nuclear activities. We intend to exploit the discharges of Pu from Sellafield nuclear reprocessing plant to investigate transit times and sediment regime in inter-tidal sediments from proximal (Ravenglass Estuary, Cumbria) and distal (Portishead, North Somerset) sites. Continuing developments in analytical techniques (extraction chromatography and ion exchange) and inductively coupled plasma mass spectrometry (ICP-MS) permit isotopic analysis at low abundances (on the order of femto-grams), with reasonable efficiency and cost in comparison to traditional radiometric techniques. A major advantage of this technique is the ability to distinguish between {sup 239}Pu and {sup 240}Pu, which is not possible with alpha-spectrometry due to similar alpha energies. We present initial results using MC-ICP-MS, following methods in Lindahl et al. (2011). Document available in abstract form only. (authors)

  12. Concrete enclosure to shield a neutron source

    Energy Technology Data Exchange (ETDEWEB)

    Villagrana M, L. E.; Rivera P, E.; De Leon M, H. A.; Soto B, T. G.; Hernandez D, V. M.; Vega C, H. R., E-mail: emmanuelvillagrana@hotmail.com [Universidad Autonoma de Zacatecas, Unidad Academica de Estudios Nucleares, Apdo. Postal 336, 98000 Zacatecas (Mexico)

    2012-10-15

    In the aim to design a shielding for a {sup 239}PuBe isotopic neutron source several Monte Carlo calculations were carried out using MCNP5 code. First, a point-like source was modeled in vacuum and the neutron spectrum and the ambient dose equivalent were calculated at several distances ranging from 5 up to 150 cm, these calculations were repeated including air, and a 1 x 1 x 1 m{sup 3} enclosure that was shielded with 5, 15, 20, 25, 30, 50 and 80 cm-thick Portland type concrete walls. At all the points located inside the enclosure neutron spectra from 10{sup -8} up 0.5 MeV were the same regardless the distance from the source showing the room-return effect, for energies larger than 0.5 MeV neutron spectra are diminished as the distance increases. Outside the enclosure it was noticed that neutron spectra becomes -softer- as the concrete thickness increases due to reduction of mean neutron energy. With the ambient dose values the attenuation curve in terms of concrete thickness was calculated. (Author)

  13. Plutonium partitioning in three-phase systems with water, colloidal particles, and granites: new insights into distribution coefficients.

    Science.gov (United States)

    Xie, Jinchuan; Lin, Jianfeng; Zhou, Xiaohua; Li, Mei; Zhou, Guoqing

    2014-03-01

    The traditional sorption experiments commonly treated the colloid-associated species of low-solubility contaminants as immobile species resulted from the centrifugation or ultrafiltration, and then solid/liquid distribution coefficients (Ks/d) were determined. This may lead to significantly underestimated mobility of the actinides in subsurface environments. Accordingly, we defined a new distribution coefficient (Ks/d+c) to more adequately describe the mobile characteristics of colloidal species. The results show that under alkaline aqueous conditions the traditional Ks/d was 2-3 orders of magnitude larger than the Ks/d+c involving the colloidal species of (239)Pu. The colloid/liquid distribution coefficients Kc/d≫0 (∼10(6)mL/g) revealed strong competition of the colloidal granite particles with the granite grains for Pu. The distribution percentages of Pu in the three-phase systems, depending on various conditions such as particle concentrations, Na(+) concentrations, pH and time, were determined. Moreover, we developed the thermodynamic and kinetic complexation models to explore the interaction of Pu with the particle surfaces.

  14. Reference material manufacture and certification for the AVNG

    Energy Technology Data Exchange (ETDEWEB)

    Hauck, Danielle K [Los Alamos National Laboratory; Mac Arthur, Duncan [Los Alamos National Laboratory; Thron, Jonathan L [Los Alamos National Laboratory; Livke, Alexander [VNIIEF; Kondratov, Sergey [VNIIEF; Razinkov, Sergey [VNIIEF

    2010-01-01

    Testing and demonstration of any radiation measurement system requires the use of appropriate radioactive sources. The AVNG implementation that we describe is an attribute measurement system built by RFNC - VNIIEF in Sarov, Russia. The AVNG detects neutron and gamma radiation signatures and displays the three unclassified attributes of 'plutonium presence,' 'plutonium mass > 2 kg,' and 'plutonium isotopic ratio ({sup 240}Pu to {sup 239}Pu) < 0.1.' The AVNG was tested using a number of reference material (RM) sources with masses and isotopic ratios above and below these thresholds. The AVNG was demonstrated in June 2009 using several of these sources in addition to detector calibration sources. Since the AVNG was designed to measure multi-kg plutonium sources, the RM was manufactured specifically for use with this system. In addition, the RM was used to test the thresholds in the AVNG, so the size and composition of each RM was certified prior to use. In this presentation, we will describe the various steps in the manufacture and certification of these RM sources.

  15. Rapid determination of plutonium isotopes in environmental samples using sequential injection extraction chromatography and detection by inductively coupled plasma mass spectrometry.

    Science.gov (United States)

    Qiao, Jixin; Hou, Xiaolin; Roos, Per; Miró, Manuel

    2009-10-01

    This article presents an automated method for the rapid determination of 239Pu and 240Pu in various environmental samples. The analytical method involves the in-line separation of Pu isotopes using extraction chromatography (TEVA) implemented in a sequential injection (SI) network followed by detection of isolated analytes with inductively coupled plasma mass spectrometry (ICP-MS). The method has been devised for the determination of Pu isotopes at environmentally relevant concentrations, whereby it has been successfully applied to the analyses of large volumes/amounts of samples, for example, 100-200 g of soil and sediment, 20 g of seaweed, and 200 L of seawater following analyte preconcentration. The investigation of the separation capability of the assembled SI system revealed that up to 200 g of soil or sediment can be treated using a column containing about 0.70 g of TEVA resin. The analytical results of Pu isotopes in the reference materials showed good agreement with the certified or reference values at the 0.05 significance level. Chemical yields of Pu ranged from 80 to 105%, and the decontamination factors for uranium, thorium, mercury and lead were all above 10(4). The duration of the in-line extraction chromatographic run was determination of Pu isotopes in environmental risk assessment and emergency preparedness scenarios.

  16. Radiative capture on $^{242}$Pu for MOX fuel reactors

    CERN Multimedia

    The use of MOX fuel (mixed-oxide fuel made of UO$_{2}$ and PuO$_{2}$) in nuclear reactors allows substituting a large fraction of the enriched Uranium by Plutonium reprocessed from spent fuel. Indeed around 66% of the plutonium from spent fuel is made of $^{239}$Pu and $^{241}$Pu, which are fissile in thermal reactors. A typical reactor of this type uses a fuel with 7% reprocessed Pu and 93% depleted U, thus profiting from both the spent fuel and the remaining $^{238}$U following the $^{235}$U enrichment. With the use of such new fuel compositions rich in Pu the better knowledge of the capture and fission cross sections of the Pu isotopes becomes very important. This is clearly stated in the recent OECD NEA’s “High Priority Request List” and in the WPEC-26 “Uncertainty and target accuracy assessment for innovative systems using recent covariance data evaluations” report. In particular, a new series of cross section evaluations have been recently carried out jointly by the European (JEFF) and United ...

  17. Review and Assessment of Neutron Cross Section and Nubar Covariances for Advanced Reactor Systems

    Energy Technology Data Exchange (ETDEWEB)

    Maslov,V.M.; Oblozinsky, P.; Herman, M.

    2008-12-01

    In January 2007, the National Nuclear Data Center (NNDC) produced a set of preliminary neutron covariance data for the international project 'Nuclear Data Needs for Advanced Reactor Systems'. The project was sponsored by the OECD Nuclear Energy Agency (NEA), Paris, under the Subgroup 26 of the International Working Party on Evaluation Cooperation (WPEC). These preliminary covariances are described in two recent BNL reports. The NNDC used a simplified version of the method developed by BNL and LANL that combines the recent Atlas of Neutron Resonances, the nuclear reaction model code EMPIRE and the Bayesian code KALMAN with the experimental data used as guidance. There are numerous issues involved in these estimates of covariances and it was decided to perform an independent review and assessment of these results so that better covariances can be produced for the revised version in future. Reviewed and assessed are uncertainties for fission, capture, elastic scattering, inelastic scattering and (n,2n) cross sections as well as prompt nubars for 15 minor actinides ({sup 233,234,236}U, {sup 237}Np, {sup 238,240,241,242}Pu, {sup 241,242m,243}Am and {sup 242,243,244,245}Cm) and 4 major actinides ({sup 232}Th, {sup 235,238}U and {sup 239}Pu). We examined available evaluations, performed comparison with experimental data, taken into account uncertainties in model parameterization and made use state-of-the-art nuclear reaction theory to produce the uncertainty assessment.

  18. Deposition of fission and activation products after the Fukushima Dai-ichi nuclear power plant accident.

    Science.gov (United States)

    Shozugawa, Katsumi; Nogawa, Norio; Matsuo, Motoyuki

    2012-04-01

    The Great Eastern Japan Earthquake on March 11, 2011, damaged reactor cooling systems at Fukushima Dai-ichi nuclear power plant. The subsequent venting operation and hydrogen explosion resulted in a large radioactive nuclide emission from reactor containers into the environment. Here, we collected environmental samples such as soil, plant species, and water on April 10, 2011, in front of the power plant main gate as well as 35 km away in Iitate village, and observed gamma-rays with a Ge(Li) semiconductor detector. We observed activation products ((239)Np and (59)Fe) and fission products ((131)I, (134)Cs ((133)Cs), (137)Cs, (110m)Ag ((109)Ag), (132)Te, (132)I, (140)Ba, (140)La, (91)Sr, (91)Y, (95)Zr, and (95)Nb). (239)Np is the parent nuclide of (239)Pu; (59)Fe are presumably activation products of (58)Fe obtained by corrosion of cooling pipes. The results show that these activation and fission products, diffused within a month of the accident.

  19. The importance of recording physical and chemical variables simultaneously with remote radiological surveillance of aquatic systems: a perspective for environmental modelling.

    Science.gov (United States)

    Abril, J M; El-Mrabet, R; Barros, H

    2004-01-01

    Modern nuclear metrological tools allow the remote surveillance of the radiological status of the aquatic systems, providing an important advance in the protection of the environment. Nevertheless, the significance of the radiological data could be highly improved through simultaneous recording of physical and chemical variables that govern the behaviour and bioavailability of radionuclides in these aquatic systems. This work reviews some of these variables from the point of view of the environmental modelling. The amount, nature and dynamics of the suspended loads and bottom sediments strongly influence the behaviour of particle-reactive radionuclides. The kinetics of this process has a very fast component, as it is shown from our recent studies with 241Am, 239Pu and 133Ba in several aquatic systems from southern Spain. Changes in pH, temperature and in the electrical conductivity are influencing the uptake kinetics and the final partitioning of the radioactivity. Water currents govern the radionuclide transport and dispersion. These points are illustrated with modelling exercises in the scenarios of the Suez Canal (Egypt) and the Härsvatten Lake (Sweden).

  20. Measurements of reaction rate ratios as indexes of breeding performance in mock-up cores of FCA simulating metallic-fueled LMFBR and MOX-fueled LMFBR

    Energy Technology Data Exchange (ETDEWEB)

    Sakurai, Takeshi; Nemoto, Tatsuo [Japan Atomic Energy Research Inst., Tokai, Ibaraki (Japan). Tokai Research Establishment; Kobayashi, Keiji; Unesaki, Hironobu

    1999-08-01

    Measurements and analysis for reaction rate ratio of {sup 238}U capture to {sup 239}Pu fission (C8/F9) and that of {sup 238}U capture to {sup 235}U fission (C8/F5), which are important as indexes of breeding behavior of a fast breeder reactor, were made at Fast Critical Assembly (FCA) of Japan Atomic Energy Research Institute. The measurements were made by a foil activation technique at two assemblies simulating metallic-fueled liquid metal fast breeder reactor and an assembly simulating a MOX-fueled one. The analysis was made based on JENDL3.2 nuclear data file. Calculation to experiment ratios of C8/F9 and C8/F5 were 0.99-1.02 and 1.0-1.03 respectively. Furthermore, the {sup 238}U capture rate and the {sup 235}U fission rate were measured in a thermal neutron standard field in Heavy Water Facility of Kyoto University Research Reactor to verify accuracy of the present foil activation technique itself and to confirm these C/E values. (author)

  1. Certified reference material for radionuclides in fish flesh sample IAEA-414 (mixed fish from the Irish Sea and North Sea)

    Energy Technology Data Exchange (ETDEWEB)

    Pham, M.K. [International Atomic Energy Agency (IAEA), Marine Environment Laboratory (MEL), MC 98000 (Monaco)]. E-mail: m.pham@iaea.org; Sanchez-Cabeza, J.A.; Povinec, P.P.; Gastaud, J.; La Rosa, J.; Lee, S.-H.; Liong Wee Kwong, L.; Oregioni, B.; Wyse, E. [International Atomic Energy Agency (IAEA), Marine Environment Laboratory (MEL), MC 98000 (Monaco); Arnold, D. [Physikalisch-Technische Bundesanstalt, Braunschweig, 38116 Germany (Germany); Benmansour, M. [Centre National de l' Energie, des Sciences et des Techniques Nucleaires (CNESTEN), B.P. 1382, R.P.10001, Rabat (Morocco); Bojanowski, R. [Institute of Oceanology, Polish Academy of Sciences, PL-81-712 Sopot (Poland); Carvalho, F.P. [Instituto Tecnologico e Nuclear, Departamento de Proteccao Radiologica e Seguranca Nuclear, P-2685-953 Sacavem (Portugal); Kim, C.K. [Department of Radiological Environmental Assessment, Korea Institute of Nuclear Safety, Yo-song, Taejon 305-600, Korea (Korea); Esposito, M. [Laboratorio di Ingegneria Nucleare, Universita di Bologna, 40136 Bologna (Italy); Gasco, C.L. [CIEMAT-DIAE, Radioecologia del Medio Acuatico, 28040 Madrid (Spain); Ham, G.J. [National Radiological Protection Board, Chilton, Didcot, Oxon, OX11 0RA (United Kingdom); Hegde, A.G. [Environmental Survey Laboratory, Bhabha Atomic Research Center, Tarapur Atomic Power Station, Maharashtra 401 504 (India); Holm, E. [Department of Medical Radiation Physics, Lund University Hospital, 22185 Lund (Sweden); Jaskierowicz, D. [Lab. d' Analyses de Surveillance et d' Expertise de la Marine, Base Navale de Cherbourg, 50115 Cherbourg (France); Kanisch, G. [Federal Research Centre for Fisheries, Institute of Fisheries Ecology, 20539 Hamburg (Germany); Llaurado, M. [Lab. de Radiologia Ambiental, Dept. de Quimica Analitica, Facultat de Quimica, Universitat de Barcelona, 08028 Barcelona (Spain); Le Petit, G. [Commissariat a l' Energie Atomique, DASE/SRCE, 91680 Bruyeres-le-Chatel (France); Maruo, Y. [and others

    2006-10-15

    A certified reference material (CRM) for radionuclides in fish sample IAEA-414 (mixed fish from the Irish Sea and North Seas) is described and the results of the certification process are presented. Nine radionuclides ({sup 4}K, {sup 137}Cs, {sup 232}Th, {sup 234}U, {sup 235}U, {sup 238}U, {sup 238}Pu, {sup 239+24}Pu and {sup 241}Am) were certified for this material. Information on massic activities with 95% confidence intervals is given for six other radionuclides ({sup 9}Sr, {sup 21}Pb({sup 21}Po), {sup 226}Ra, {sup 239}Pu, {sup 24}Pu {sup 241}Pu). Less frequently reported radionuclides ({sup 99}Tc, {sup 129}I, {sup 228}Th, {sup 23}Th and {sup 237}Np) and information on some activity and mass ratios are also included. The CRM can be used for quality assurance/quality control of the analysis of radionuclides in fish sample, for the development and validation of analytical methods and for training purposes. The material is available from IAEA, Vienna, in 100 g units.

  2. Experimental investigation on radiation shielding of high performance concrete for nuclear and radiotherapy facilities

    Science.gov (United States)

    Domański, Szymon; Gryziński, Michał A.; Maciak, Maciej; Murawski, Łukasz; Tulik, Piotr; Tymińska, Katarzyna

    2016-06-01

    This paper presents the set of procedures developed in Radiation Protection Measurements Laboratory at National Centre for Nuclear Research for evaluation of shielding properties of high performance concrete. The purpose of such procedure is to characterize the material behaviour against gamma and neutron radiation. The range of the densities of the concrete specimens was from 2300 to 3900 kg/m3. The shielding properties against photons were evaluated using 137Cs and 60Co sources. The neutron radiation measurements have been performed by measuring the transmitted radiation from 239PuBe source. Scattered neutron radiation has been evaluated using the shadow cone technique. A set up of ionization chambers was used during all experiments. The gamma dose was measured using C-CO2 ionization chamber. The neutron dose was evaluated with recombination chamber of REM-2 type with appropriate recombination method applied. The method to distinguish gamma and neutron absorbed dose components in mixed radiation fields using twin detector method was presented. Also, recombination microdosimetric method was applied for the obtained results. Procedures to establish consecutive half value layers and tenth value layers (HVL and TVL) for gamma and neutron radiation were presented. Measured HVL and TVL values were linked with concrete density to highlight well known dependence. Also, influence of specific admixtures to concrete on neutron attenuation properties was studied. The results confirmed the feasibility of approach for the radiation shielding investigations.

  3. Resuspension and atmospheric transport of radionuclides due to wildfires near the Chernobyl Nuclear Power Plant in 2015: An impact assessment

    Science.gov (United States)

    Evangeliou, N.; Zibtsev, S.; Myroniuk, V.; Zhurba, M.; Hamburger, T.; Stohl, A.; Balkanski, Y.; Paugam, R.; Mousseau, T. A.; Møller, A. P.; Kireev, S. I.

    2016-05-01

    In April and August 2015, two major fires in the Chernobyl Exclusion Zone (CEZ) caused concerns about the secondary radioactive contamination that might have spread over Europe. The present paper assessed, for the first time, the impact of these fires over Europe. About 10.9 TBq of 137Cs, 1.5 TBq of 90Sr, 7.8 GBq of 238Pu, 6.3 GBq of 239Pu, 9.4 GBq of 240Pu and 29.7 GBq of 241Am were released from both fire events corresponding to a serious event. The more labile elements escaped easier from the CEZ, whereas the larger refractory particles were removed more efficiently from the atmosphere mainly affecting the CEZ and its vicinity. During the spring 2015 fires, about 93% of the labile and 97% of the refractory particles ended in Eastern European countries. Similarly, during the summer 2015 fires, about 75% of the labile and 59% of the refractory radionuclides were exported from the CEZ with the majority depositing in Belarus and Russia. Effective doses were above 1 mSv y-1 in the CEZ, but much lower in the rest of Europe contributing an additional dose to the Eastern European population, which is far below a dose from a medical X-ray.

  4. Design of a system for neutrons dosimetry; Diseno de un sistema para dosimetria de neutrones

    Energy Technology Data Exchange (ETDEWEB)

    Ceron, P.; Rivera, T. [IPN, Centro de Investigacion en Ciencia Aplicada y Tecnologia Avanzada, Legaria No. 694, Col. Irrigacion, 11500 Mexico D. F. (Mexico); Paredes G, L. [ININ, Carretera Mexico-Toluca s/n, 52750 Ocoyoacac, Estado de Mexico (Mexico); Azorin, J. [Universidad Autonoma Metropolitana, Unidad Iztapalapa, San Rafael Atlixco 186, Col. Vicentina, 09340 Mexico D. F. (Mexico); Sanchez, A. [IPN, Escuela Superior de Fisica y Matematicas, Av. Instituto Politecnico Nacional s/n, Col. San Pedro Zacatenco, 07738 Mexico D. F. (Mexico); Vega C, H. R., E-mail: victceronr@hotmail.com [Universidad Autonoma de Zacatecas, Unidad Academica de Estudios Nucleares, Cipres No. 10, Fracc. La Penuela, 98068 Zacatecas (Mexico)

    2014-08-15

    At the present time diverse systems of detection of neutrons exist, as proportional counters based on BF{sub 3}, He{sub 3} and spectrometers of Bonner spheres. However, the cost and the complexity of the implementation of these systems put them far from the reach for dosimetric purposes. For these reasons a system of neutrons detection composed by a medium paraffin moderator that forms a 4π (spheres) arrangement and of several couples of thermoluminescent dosimeters TLD 600/TLD 700. The response of the system presents a minor repeatability to 5% in several assays when being irradiated with a {sup 239}PuBe source and a deviation of 13.8% in the Tl readings of four different spheres. The calibration factor of the system with regard to the neutrons source which was of 56.2 p Sv/nc also was calculated. These detectors will be used as passive monitors of photoneutrons in a radiotherapy room with lineal accelerator of high energy. (Author)

  5. A comparative radiological assessment of five European biosphere systems in the context of potential contamination of well water from the hypothetical disposal of radioactive waste.

    Science.gov (United States)

    Olyslaegers, G; Zeevaert, T; Pinedo, P; Simon, I; Pröhl, G; Kowe, R; Chen, Q; Mobbs, S; Bergström, U; Hallberg, B; Katona, T; Eged, K; Kanyar, B

    2005-12-01

    In the framework of the BioMoSA project for the development of biosphere assessment models for radioactive waste disposal the Reference Biosphere Methodology developed in the IAEA programme BIOMASS was applied to five locations, situated in different European countries. Specific biosphere models were applied to assess the hypothetical contamination of a range of agricultural and environmental pathways and the dose to individuals, following contamination of well water. The results of these site-specific models developed by the different BioMoSA partners, and the individual normalised dose to the exposure groups were compared against each other. Ingestion of drinking water, fruit and vegetables were found to be among the most important pathways for almost all radionuclides. Stochastic calculations revealed that consumption habits, transfer factors, irrigation rates and distribution coefficients (Kd(s)) were the most important parameters that influence the end results. Variations in the confidence intervals were found to be higher for sorbing elements (e.g. (36)Cl, (237)Np, (99)Tc, (238)U, (129)I) than for mobile elements (e.g. (226)Ra, (79)Se, (135)Cs, (231)Pa, (239)Pu). The influence of daughter products, for which the distribution into the biosphere was calculated individually, was also shown to be important. This paper gives a brief overview of the deterministic and stochastic modelling results and the parameter sensitivity. A screening methodology was introduced to identify the most important pathways, simplify a generic biosphere tool and refine the existing models.

  6. Feasibility of Thorium Fuel Cycles in a Very High Temperature Pebble-Bed Hybrid System

    Directory of Open Access Journals (Sweden)

    L.P. Rodriguez

    2015-08-01

    Full Text Available Nuclear energy presents key challenges to be successful as a sustainable energy source. Currently, the viability of the use thorium-based fuel cycles in an innovative nuclear energy generation system is being investigated in order to solve these key challenges. In this work, the feasibility of three thorium-based fuel cycles (232Th-233U, 232Th-239Pu, and 232Th-U in a hybrid system formed by a Very High Temperature Pebble-Bed Reactor (VHTR and two Pebble-Bed Accelerator Driven Systems (ADSs was evaluated using parameters related to the neutronic behavior such as nuclear fuel breeding, minor actinide stockpile, the energetic contribution of each fissile isotope, and the radiotoxicity of the long lived wastes. These parameters were used to compare the fuel cycles using the well-known MCNPX ver. 2.6e computational code. The results obtained confirm that the 232Th-233U fuel cycle is the best cycle for minimizing the production of plutonium isotopes and minor actinides. Moreover, the inclusion of the second stage in the ADSs demonstrated the possibility of extending the burnup cycle duration and reducing the radiotoxicity of the discharged fuel from the VHTR.

  7. Vertical distribution and migration of global fallout Pu in forest soils in southwestern China.

    Science.gov (United States)

    Bu, Wenting; Zheng, Jian; Guo, Qiuju; Uchida, Shigeo

    2014-10-01

    Soil samples collected in southwestern China were analyzed for Pu isotopes. The (240)Pu/(239)Pu atom ratios were around 0.18, which indicated the dominant source of global fallout. Consistent sub-surface maximums followed by exponential decline of (239+240)Pu activities in the soil cores were observed. Most of the Pu has still remained in the 0-10 cm layers since its deposition. Convection velocities and dispersion coefficients for Pu migration in the soils were estimated by the convection-dispersion equation (CDE) model. The effective convection velocities and effective dispersion coefficients ranged from 0.05 to 0.11 cm/y and from 0.06 to 0.29 cm(2)/y, respectively. Other factors that control the vertical migratio