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Sample records for pu u-oxide fuel

  1. ZPR-6 assembly 7 high {sup 240} PU core : a cylindrical assemby with mixed (PU, U)-oxide fuel and a central high {sup 240} PU zone.

    SciTech Connect

    Lell, R. M.; Schaefer, R. W.; McKnight, R. D.; Tsiboulia, A.; Rozhikhin, Y.; Nuclear Engineering Division; Inst. of Physics and Power Engineering

    2007-10-01

    Over a period of 30 years more than a hundred Zero Power Reactor (ZPR) critical assemblies were constructed at Argonne National Laboratory. The ZPR facilities, ZPR-3, ZPR-6, ZPR-9 and ZPPR, were all fast critical assembly facilities. The ZPR critical assemblies were constructed to support fast reactor development, but data from some of these assemblies are also well suited to form the basis for criticality safety benchmarks. Of the three classes of ZPR assemblies, engineering mockups, engineering benchmarks and physics benchmarks, the last group tends to be most useful for criticality safety. Because physics benchmarks were designed to test fast reactor physics data and methods, they were as simple as possible in geometry and composition. The principal fissile species was {sup 235}U or {sup 239}Pu. Fuel enrichments ranged from 9% to 95%. Often there were only one or two main core diluent materials, such as aluminum, graphite, iron, sodium or stainless steel. The cores were reflected (and insulated from room return effects) by one or two layers of materials such as depleted uranium, lead or stainless steel. Despite their more complex nature, a small number of assemblies from the other two classes would make useful criticality safety benchmarks because they have features related to criticality safety issues, such as reflection by soil-like material. The term 'benchmark' in a ZPR program connotes a particularly simple loading aimed at gaining basic reactor physics insight, as opposed to studying a reactor design. In fact, the ZPR-6/7 Benchmark Assembly (Reference 1) had a very simple core unit cell assembled from plates of depleted uranium, sodium, iron oxide, U3O8, and plutonium. The ZPR-6/7 core cell-average composition is typical of the interior region of liquid-metal fast breeder reactors (LMFBRs) of the era. It was one part of the Demonstration Reactor Benchmark Program,a which provided integral experiments characterizing the important features of demonstration

  2. ZPR-6 assembly 7 high {sup 240}Pu core experiments : a fast reactor core with mixed (Pu,U)-oxide fuel and a centeral high{sup 240}Pu zone.

    SciTech Connect

    Lell, R. M.; Morman, J. A.; Schaefer, R.W.; McKnight, R.D.; Nuclear Engineering Division

    2009-02-23

    ZPR-6 Assembly 7 (ZPR-6/7) encompasses a series of experiments performed at the ZPR-6 facility at Argonne National Laboratory in 1970 and 1971 as part of the Demonstration Reactor Benchmark Program (Reference 1). Assembly 7 simulated a large sodium-cooled LMFBR with mixed oxide fuel, depleted uranium radial and axial blankets, and a core H/D near unity. ZPR-6/7 was designed to test fast reactor physics data and methods, so configurations in the Assembly 7 program were as simple as possible in terms of geometry and composition. ZPR-6/7 had a very uniform core assembled from small plates of depleted uranium, sodium, iron oxide, U{sub 3}O{sub 8} and Pu-U-Mo alloy loaded into stainless steel drawers. The steel drawers were placed in square stainless steel tubes in the two halves of a split table machine. ZPR-6/7 had a simple, symmetric core unit cell whose neutronic characteristics were dominated by plutonium and {sup 238}U. The core was surrounded by thick radial and axial regions of depleted uranium to simulate radial and axial blankets and to isolate the core from the surrounding room. The ZPR-6/7 program encompassed 139 separate core loadings which include the initial approach to critical and all subsequent core loading changes required to perform specific experiments and measurements. In this context a loading refers to a particular configuration of fueled drawers, radial blanket drawers and experimental equipment (if present) in the matrix of steel tubes. Two principal core configurations were established. The uniform core (Loadings 1-84) had a relatively uniform core composition. The high {sup 240}Pu core (Loadings 85-139) was a variant on the uniform core. The plutonium in the Pu-U-Mo fuel plates in the uniform core contains 11% {sup 240}Pu. In the high {sup 240}Pu core, all Pu-U-Mo plates in the inner core region (central 61 matrix locations per half of the split table machine) were replaced by Pu-U-Mo plates containing 27% {sup 240}Pu in the plutonium

  3. Pu-238 fuel form activities, June 1-30, 1980

    SciTech Connect

    Not Available

    1980-07-18

    This monthly report for Pu-238 Fuel Form Activities has two main sections: SRP-PuFF Pu-238 Fuel Form Production Processes and SRL Pu-238 Fuel Form Research and Development. The program status, budget information, and milestone information are discussed in each main section. The Work Breakdown Structures (WBS) for this program is outlined. Only one monthly report per year is processed for EDB.

  4. Pu-238 fuel form activities, January 1-31, 1982

    SciTech Connect

    Not Available

    1982-03-01

    This monthly report for /sup 238/Pu fuel form activities has two main sections: SRP-PuFF facility and SRL fuel form activities. The program status, budget information, and milestone schedules are discussed in each main section. The Work Breakdown Structure (WBS) for this program is shown. Only one monthly report per year is processed for EDB.

  5. Improved MOX fuel calculations using new Pu-239, Am-241 and Pu-240 evaluations

    NASA Astrophysics Data System (ADS)

    Noguere, G.; Bouland, O.; Bernard, D.; Leconte, P.; Blaise, P.; Peneliau, Y.; Vidal, J. F.; De Saint Jean, C.; Leal, L.; Schillebeeckx, P.; Kopecky, S.; Lampoudis, C.

    2013-03-01

    Several studies based on the JEFF-3.1.1 nuclear data library show a systematic overestimation of the critical keff for core configurations of MOX fuel assemblies. The present work investigates possible improvements of the C/E results by using new evaluations for Am-241, Pu-239 and Pu-240.

  6. Performance of Cladding on MOX Fuel with Low 240Pu/239Pu Ratio

    SciTech Connect

    McCoy, Kevin; Blanpain, Patrick; Morris, Robert Noel

    2014-01-01

    The U.S. Department of Energy has decided to dispose of a portion of its surplus plutonium by reconstituting it into mixed oxide (MOX) fuel and irradiating it in commercial power reactors. As part of fuel qualification, four lead assemblies were manufactured and irradiated to a maximum fuel rod average burnup of 47.3 MWd/kg heavy metal. This was the world s first commercial irradiation of MOX fuel with a 240Pu/239Pu ratio less than 0.10. Five fuel rods with varying burnups and plutonium contents were selected from one of the assemblies and shipped to Oak Ridge National Laboratory for hot cell examination. This paper discusses the results of those examinations with emphasis on cladding performance. Exams relevant to the cladding included visual and eddy current exams, profilometry, microscopy, hydrogen analysis, gallium analysis, and mechanical testing. There was no discernible effect of the type of MOX fuel on the performance of the cladding.

  7. Thermal Analysis of ZPPR High Pu Content Stored Fuel

    DOE PAGES

    Solbrig, Charles W.; Pope, Chad L.; Andrus, Jason P.

    2014-01-01

    The Zero Power Physics Reactor (ZPPR) operated from April 18, 1969, until 1990. ZPPR operated at low power for testing nuclear reactor designs. This paper examines the temperature of Pu content ZPPR fuel while it is in storage. Heat is generated in the fuel due to Pu and Am decay and is a concern for possible cladding damage. Damage to the cladding could lead to fuel hydriding and oxidizing. A series of computer simulations were made to determine the range of temperatures potentially occuring in the ZPPR fuel. The maximum calculated fuel temperature is 292°C (558°F). Conservative assumptions in themore » model intentionally overestimate temperatures. The stored fuel temperatures are dependent on the distribution of fuel in the surrounding storage compartments, the heat generation rate of the fuel, and the orientation of fuel. Direct fuel temperatures could not be measured but storage bin doors, storage sleeve doors, and storage canister temperatures were measured. Comparison of these three temperatures to the calculations indicates that the temperatures calculated with conservative assumptions are, as expected, higher than the actual temperatures. The maximum calculated fuel temperature with the most conservative assumptions is significantly below the fuel failure criterion of 600°C (1,112°F).« less

  8. Bulk characterization of (U, Pu) mixed carbide fuel for distribution of plutonium

    SciTech Connect

    Devi, K. V. Vrinda Khan, K. B.; Biju, K.; Kumar, Arun

    2015-06-24

    Homogeneous distribution of plutonium in (U, Pu) mixed fuels is important from fuel performance as well as reprocessing point of view. Radiation imaging and assay techniques are employed for the detection of Pu rich agglomerates in the fuel. A simulation study of radiation transport was carried out to analyse the technique of autoradiography so as to estimate the minimum detectability of Pu agglomerates in MC fuel with nominal PuC content of 70% using Monte Carlo simulations.

  9. Cracking mechanism of PuO/sub 2/ fuel hot pressed in graphite dies

    SciTech Connect

    Taylor, D.H.

    1981-01-01

    Internal cracking in PuO/sub 2/ fuel is caused by gas pressure during hot pressing. Surface cracks are caused by tensile stresses arising from the phase change of ..cap alpha..-PuO/sub 2/ to ..gamma..-PuO/sub 2/ on reoxidation. To control cracking, process variables were chosen to minimize fuel reduction and to give large intergranular porosity. 19 figures.

  10. Irradiation performance of (Th,Pu)O2 fuel under Pressurized Water Reactor conditions

    NASA Astrophysics Data System (ADS)

    Boer, B.; Lemehov, S.; Wéber, M.; Parthoens, Y.; Gysemans, M.; McGinley, J.; Somers, J.; Verwerft, M.

    2016-04-01

    This paper examines the in-pile safety performance of (Th,Pu)O2 fuel pins under simulated Pressurized Water Reactor (PWR) conditions. Both sol-gel and SOLMAS produced (Th,Pu)O2 fuels at enrichments of 7.9% and 12.8% in Pu/HM have been irradiated at SCK·CEN. The irradiation has been performed under PWR conditions (155 bar, 300 °C) in a dedicated loop of the BR-2 reactor. The loop is instrumented with flow and temperature monitors at inlet and outlet, which allow for an accurate measurement of the deposited enthalpy.

  11. Oxidation and reduction behaviors of a prototypic MgO-PuO2-x inert matrix fuel

    NASA Astrophysics Data System (ADS)

    Miwa, Shuhei; Osaka, Masahiko

    2017-04-01

    Oxidation and reduction behaviors of prototypic MgO-based inert matrix fuels (IMFs) containing PuO2-x were experimentally investigated by means of thermogravimetry. The oxidation and reduction kinetics of the MgO-PuO2-x specimen were determined. The oxidation and reduction rates of the MgO-PuO2-x were found to be low compared with those of PuO2-x. It is note that the changes in O/Pu ratios of MgO-PuO2-x from stoichiometry were smaller than those of PuO2-x at high oxygen partial pressure.

  12. Stress and Diffusion in Stored Pu ZPPR Fuel from Alpha Generation

    SciTech Connect

    Charles W. Solbrig; Chad L. Pope; Jason P. Andrus

    2014-07-01

    ZPPR (Zero Power Physics Reactor) is a research reactor that has been used to investigate breeder reactor fuel designs. The reactor has been dismantled but its fuel is still stored there. Of concern are its plutonium containing metal fuel elements which are enclosed in stainless steel cladding with gas space filled with helium–argon gas and welded air tight. The fuel elements which are 5.08 cm by 0.508 cm up to 20.32 cm long (2 in × 0.2 in × 8 in) were manufactured in 1968. A few of these fuel elements have failed releasing contamination raising concern about the general state of the large number of other fuel elements. Inspection of the large number of fuel elements could lead to contamination release so analytical studies have been conducted to estimate the probability of failed fuel elements. This paper investigates the possible fuel failures due to generation of helium in the metal fuel from the decay of Pu and its possible damage to the fuel cladding from metal fuel expansion or from diffusion of helium into the fuel gas space. This paper (1) calculates the initial gas loading in a fuel element and its internal free volume after it has been brought into the atmosphere at ZPPR, (2) shows that the amount of helium generated by decay of Pu over 46 years since manufacture is significantly greater than this initial loading, (3) determines the amount of fuel swelling if the helium stays fixed in the fuel plate and estimates the amount of helium which diffuses out of the fuel plate into the fuel plenum assuming the helium does not remain fixed in the fuel plate but can diffuse to the plenum and possibly through the cladding. Since the literature is not clear as to which possibility occurs, as with Schroedinger’s cat, both possibilities are analyzed. The paper concludes that (1) if the gas generated is fixed in the fuel, then the fuel swelling it can cause would not cause any fuel failure and (2) if the helium does diffuse out of the fuel (in accordance

  13. TRISO-Fuel Element Performance Modeling for the Hybrid LIFE Engine with Pu Fuel Blanket

    SciTech Connect

    DeMange, P; Marian, J; Caro, M; Caro, A

    2010-02-18

    A TRISO-coated fuel thermo-mechanical performance study is performed for the hybrid LIFE engine to test the viability of TRISO particles to achieve ultra-high burnup of a weapons-grade Pu blanket. Our methodology includes full elastic anisotropy, time and temperature varying material properties for all TRISO layers, and a procedure to remap the elastic solutions in order to achieve fast fluences up to 30 x 10{sup 25} n {center_dot} m{sup -2} (E > 0.18 MeV). In order to model fast fluences in the range of {approx} 7 {approx} 30 x 10{sup 25} n {center_dot} m{sup -2}, for which no data exist, careful scalings and extrapolations of the known TRISO material properties are carried out under a number of potential scenarios. A number of findings can be extracted from our study. First, failure of the internal pyrolytic carbon (PyC) layer occurs within the first two months of operation. Then, the particles behave as BISO-coated particles, with the internal pressure being withstood directly by the SiC layer. Later, after 1.6 years, the remaining PyC crumbles due to void swelling and the fuel particle becomes a single-SiC-layer particle. Unrestrained by the PyC layers, and at the temperatures and fluences in the LIFE engine, the SiC layer maintains reasonably-low tensile stresses until the end-of-life. Second, the PyC creep constant, K, has a striking influence on the fuel performance of TRISO-coated particles, whose stresses scale almost inversely proportional to K. Obtaining more reliable measurements, especially at higher fluences, is an imperative for the fidelity of our models. Finally, varying the geometry of the TRISO-coated fuel particles results in little differences in the scope of fuel performance. The mechanical integrity of 2-cm graphite pebbles that act as fuel matrix has also been studied and it is concluded that they can reliable serve the entire LIFE burnup cycle without failure.

  14. The prospect of uranium nitride (UN) and mixed nitride fuel (UN-PuN) for pressurized water reactor

    SciTech Connect

    Syarifah, Ratna Dewi Suud, Zaki

    2015-09-30

    Design study of small Pressurized Water Reactors (PWRs) core loaded with uranium nitride fuel (UN) and mixed nitride fuel (UN-PuN), Pa-231 as burnable poison, and Americium has been performed. Pa-231 known as actinide material, have large capture cross section and can be converted into fissile material that can be utilized to reduce excess reactivity. Americium is one of minor actinides with long half life. The objective of adding americium is to decrease nuclear spent fuel in the world. The neutronic analysis results show that mixed nitride fuel have k-inf greater than uranium nitride fuel. It is caused by the addition of Pu-239 in mixed nitride fuel. In fuel fraction analysis, for uranium nitride fuel, the optimum volume fractions are 45% fuel fraction, 10% cladding and 45% moderator. In case of UN-PuN fuel, the optimum volume fractions are 30% fuel fraction, 10% cladding and 60% coolant/ moderator. The addition of Pa-231 as burnable poison for UN fuel, enrichment U-235 5%, with Pa-231 1.6% has k-inf more than one and excess reactivity of 14.45%. And for mixed nitride fuel, the lowest value of reactivity swing is when enrichment (U-235+Pu) 8% with Pa-231 0.4%, the excess reactivity value 13,76%. The fuel pin analyze for the addition of Americium, the excess reactivity value is lower than before, because Americium absorb the neutron. For UN fuel, enrichment U-235 8%, Pa-231 1.6% and Am 0.5%, the excess reactivity is 4.86%. And for mixed nitride fuel, when enrichment (U-235+Pu) 13%, Pa-231 0.4% and Am 0.1%, the excess reactivity is 11.94%. For core configuration, it is better to use heterogeneous than homogeneous core configuration, because the radial power distribution is better.

  15. The prospect of uranium nitride (UN) and mixed nitride fuel (UN-PuN) for pressurized water reactor

    NASA Astrophysics Data System (ADS)

    Syarifah, Ratna Dewi; Suud, Zaki

    2015-09-01

    Design study of small Pressurized Water Reactors (PWRs) core loaded with uranium nitride fuel (UN) and mixed nitride fuel (UN-PuN), Pa-231 as burnable poison, and Americium has been performed. Pa-231 known as actinide material, have large capture cross section and can be converted into fissile material that can be utilized to reduce excess reactivity. Americium is one of minor actinides with long half life. The objective of adding americium is to decrease nuclear spent fuel in the world. The neutronic analysis results show that mixed nitride fuel have k-inf greater than uranium nitride fuel. It is caused by the addition of Pu-239 in mixed nitride fuel. In fuel fraction analysis, for uranium nitride fuel, the optimum volume fractions are 45% fuel fraction, 10% cladding and 45% moderator. In case of UN-PuN fuel, the optimum volume fractions are 30% fuel fraction, 10% cladding and 60% coolant/ moderator. The addition of Pa-231 as burnable poison for UN fuel, enrichment U-235 5%, with Pa-231 1.6% has k-inf more than one and excess reactivity of 14.45%. And for mixed nitride fuel, the lowest value of reactivity swing is when enrichment (U-235+Pu) 8% with Pa-231 0.4%, the excess reactivity value 13,76%. The fuel pin analyze for the addition of Americium, the excess reactivity value is lower than before, because Americium absorb the neutron. For UN fuel, enrichment U-235 8%, Pa-231 1.6% and Am 0.5%, the excess reactivity is 4.86%. And for mixed nitride fuel, when enrichment (U-235+Pu) 13%, Pa-231 0.4% and Am 0.1%, the excess reactivity is 11.94%. For core configuration, it is better to use heterogeneous than homogeneous core configuration, because the radial power distribution is better.

  16. Compatibility of U-Pu-Zr alloy fuel with stainless steel cladding

    SciTech Connect

    Leibowitz, L.; Hins, A. G.; Strain, R. V.; Tsai, H.; Hofman, G. L.

    1989-07-01

    An important issue in the development of the Integral Fast Reactor is the chemical interaction between fuel and cladding. With a U--Pu--Zr ternary alloy fuel clad in stainless steel, the existence of low-melting eutectics in the U--Fe and Pu--Fe systems must be taken into account. There is at least the possibility that cladding integrity could be compromised by formation of liquid phases during irradiation. Data from a variety of sources have been brought to bear on this issue, and our current state of understanding is summarized in this report. The phase behavior of the relevant systems has been studied to provide a framework for understanding fuel/cladding interactions. Several experimental methods have been used. Differential thermal analysis experiments were performed, and the results compared with those of the phase studies. In addition, experiments were performed in which unirradiated fuel was heated in contact with cladding alloys. The results of these tests were strongly dependent on the state of the contacting surfaces. Other tests were performed in which sections of irradiated fuel with cladding were subjected to carefully controlled heating cycles. In general, there were no inconsistencies in these experimental and analytical studies although the data are still fragmentary. Differences that were observed may be reflections of kinetic factors. 9 refs., 12 figs., 6 tabs.

  17. Characterization of self-damaged (U,Pu)N fuel used in the NIMPHE program

    NASA Astrophysics Data System (ADS)

    Carvajal-Nunez, Ursula; Prieur, Damien; Janssen, Arne; Wiss, Thierry; Cambriani, Andrea; Vermorel, Emmanuel; Scheinost, Andreas; Somers, Joseph

    2013-11-01

    During in-pile, irradiation-induced damage occurs in nuclear fuel and results in a deterioration of its properties, which can affect the margin to melt of the fuel. Damage also occurs in fresh fuel through the self-irradiation process, and thus provides a convenient means to investigate changes in the material. A uranium-plutonium mixed nitride fuel made over 25 years ago, and stored in the ITU archives has been retrieved. Coupling EXAFS and TEM has shown that this material was still well-crystallized. However, an increase of 0.3% of the lattice parameter was found. As shown by the EXAFS, the U-N and Pu-N as well as the metal-metal distances are similarly affected. However, no significant modification of both anion and cation sublattice was found. Although no defect clustering was found by EXAFS, the presence of nanometric helium bubbles was demonstrated by TEM as well as nanometric disordered domains.

  18. EQ6 Calculation for Chemical Degradation of Shippingport LWBR (TH/U Oxide) Spent Nuclear Fuel Waste Packages

    SciTech Connect

    S. Arthur

    2000-09-14

    The Monitored Geologic Repository (MGR) Waste Package Department of the Civilian Radioactive Waste Management System Management & Operating contractor (CRWMS M&O) performed calculations to provide input for disposal of spent nuclear fuel (SNF) from the Shippingport Light Water Breeder Reactor (LWBR) (Ref. 1). The Shippingport LWBR SNF has been considered for disposal at the potential Yucca Mountain site. Because of the high content of fissile material in the SNF, the waste package (WP) design requires special consideration of the amount and placement of neutron absorbers and the possible loss of absorbers and SNF materials over geologic time. For some WPs, the outer shell corrosion-resistant material (CRM) and the corrosion-allowance inner shell may breach (Refs. 2 and 3), allowing the influx of water. Water in the WP will moderate neutrons, increasing the likelihood of a criticality event within the WP; and the water may, in time, gradually leach the fissile components and neutron absorbers from the WP, further affecting the neutronics of the system. This study presents calculations of the long-term geochemical behavior of WPs containing a Shippingport LWBR SNF seed assembly, and high-level waste (HLW) glass canisters arranged according to the codisposal concept (Ref. 4). The specific study objectives were to determine: (1) The extent to which criticality control material, suggested for this WP design, will remain in the WP after corrosion/dissolution of the initial WP configuration (such that it can be effective in preventing criticality); (2) The extent to which fissile uranium and fertile thorium will be carried out of the degraded WP by infiltrating water (such that internal criticality is no longer possible, but the possibility of external criticality may be enhanced); and (3) The nominal chemical composition for the criticality evaluations of the WP design, and to suggest the range of parametric variations for additional evaluations. The scope of this

  19. Preparation, characterisation and out-of-pile property evaluation of (U,Pu)N fuel pellets

    NASA Astrophysics Data System (ADS)

    Ganguly, C.; Hegde, P. V.; Sengupta, A. K.

    1991-02-01

    (U 0.45Pu 0.55)N and (U 0.8Pu 0.2)N are being considered in India as advanced alternative fuels for the operating fast breeder test reactor (FBTR) and the forthcoming prototype fast breeder reactor (PFBR). Mixed nitride fuel pellets containing <0.1 wt% each of oxygen and carbon impurities were fabricated by the conventional "powder-pellet" (POP) and the advanced "sol-gel microsphere pelletisation" (SGMP) processes, involving two major steps. First, carbothermic reduction of an oxide-graphite powder mixture (in the form of tablets) or gel-microspheres at 1773-1823 K in N 2 followed by N2 + H2 and Ar+ H2 atmospheres. The nitride microspheres could be directly pelletised and sintered to pellets of relatively low density (≤ 85% TD) with an "open" pore structure desirable for LMFBR application. Thermal conductivity and hot hardness of nitride pellets were evaluated up to 1800 and 1500 K respectively. The out-of-pile chemical compatibility experiments of mixed nitride fuel pellets for FBTR with SS 316 cladding at 973 K for 1000 h did not reveal any significant fuel-cladding chemical interaction.

  20. Performance of U-Pu-Zr fuel cast into zirconium molds

    SciTech Connect

    Crawford, D.C.; Lahm, C.E. ); Tsai, H. )

    1992-10-01

    U-3Zr and U-20.5Pu-3Zr were injection cast into Zr tubes, or sheaths, rather than into quartz molds and clad in 316SS. These elements and standard-cast U-l0Zr and U-IgPu-l0Zr elements were irradiated in EBR-II to 2 at.% and removed for interim examination. Measurements of axial growth at indicate that the Zr-sheathed elements exhibited significantly less axial elongation than the standard-cast elements (1.3 to 1.8% versus 4.9 to 8.1%). Fuel material extruded through the ends of the Zr sheaths. allowing the low-Zr fuel to contact the cladding in some cases. Transverse metallographic sections reveal cracks in the Zr sheath through which fuel extruded and contacted cladding. The sheath is not a sufficient barrier between fuel and cladding to reduce FCCI. and any adverse effects due to increased FCCI will be evident as the elements attain higher burnup.

  1. Postirradiation examinations of U-Pu-Zr fuel elements from subassemblies X419 and X419A

    SciTech Connect

    Pahl, R G; Beck, W N; Hofman, G L; Lahm, C E; Villarreal, R

    1986-10-01

    Initial postirradiation examination of IFR type U-Pu-Zr fuel elements from X419 and X419A are reported. Characterization of the fuel at three levels of burnup, 0.8 at.%, 1.9 at.%, and 2.7 at.% is presented. Fuel swelling, microstructure, chemical redistribution, and fission gas behavior is discussed. No evidence was found for any performance-limiting damage to the fuel elements at these burnups.

  2. Validation studies based on critical experiments performed with fuel pin arrays moderated by Pu + U solutions

    SciTech Connect

    Smolen, G.R.; Matsumoto, T. )

    1989-01-01

    This paper outlines the results of a calculational study that was performed to validate the SCALE computer code system using data from critical experiments performed with fuel pin arrays moderated by mixed Pu + U aqueous solutions. A companion paper describes the experiments and discusses the criticality data that were obtained. These experimental activities are part of a joint exchange program between the US Department of Energy (DOE) and the Power Reactor and Nuclear Fuel Development Corporation of Japan in the area of criticality data development. The Consolidated fuel Reprocessing Program (CFRP) at Oak Ridge National Laboratory (ORNL) manages the program for the DOE. The experiments were conducted at the Battelle Pacific Northwest Laboratories-Critical Mass Laboratory (PNL-CML).

  3. Analysis of Pu Isotopes in Melted Fuel by Neutron Resonance Transmission: Examination by Linear Absorption Model

    NASA Astrophysics Data System (ADS)

    Kitatani, F.; Harada, H.; Takamine, J.; Kureta, M.; Seya, M.

    2014-04-01

    We have been studying the feasibility of neutron resonance transmission analysis (NRTA) for quantifying nuclear materials (Pu/U isotopes) in particle-like debris of melted fuel for nuclear material accountability and safeguards. The achievable measurement accuracy of NRTA was examined using a linear absorption model for the sample which contain substances other than nuclear fuel materials, such as boron and iron. The impurities (boron and iron etc.) in melted fuel are from the support structure and criticality control materials of the reactor core, and should be included to study the feasibility of NRTA for actual application. Neutron transmission spectra were calculated using the total neutron cross-sections in JENDL-4.0. The transmission spectra together with their uncertainties were evaluated. The study showed quantitatively that the statistical uncertainty in the determination of atomic number density of each isotope depends on the impurity density in the sample. The optimal thickness of the sample was determined for various impurity densities.

  4. Assessing the oxygen stoichiometry during the sintering of (U, Pu)O2 fuel

    NASA Astrophysics Data System (ADS)

    Vaudez, Stéphane; Léchelle, Jacques; Berzati, Ségolène; Heintz, Jean-Marc

    2015-05-01

    Diffusion phenomena occurring in ceramics such as (U, Pu)O2 during sintering are affected by the oxygen content in the atmosphere. The latter sets the nature and the concentration of point defects which govern diffusion mechanisms in the bulk of the material. The oxygen partial pressure, pO2, of the sintering gas in equilibrium with mixed oxide (MOX) pellets needs to be precisely controlled; otherwise it may induce a large dispersion in the critical parameters for fuel manufacturing (Gauche, 2013; Matzke, 1987). It is crucial to understand the relation between the sintering atmosphere and the fuel throughout the thermal cycle. In this study, the oxygen potential of the sintering gas was monitored by measuring the oxygen partial pressure (pO2) at the outlet of a dilatometer by means of a zirconia probe. Coupling the thermal cycle with an outlet gas pO2 measurement makes it possible to identify different redox phenomena. Variations in the oxygen stoichiometry can be determined during the sintering of (U, Pu)O2, as well as can its final O/M. Our results make it possible to recommend a sintering atmosphere and sintering thermal cycle in order to obtain an O/M ratio that is as close as possible to the target value.

  5. Moisture content of PuO/sub 2/ fuel used for the milliwatt generator heat source

    SciTech Connect

    Zanotelli, W.A.

    1980-01-31

    The determination of the moisture content of /sup 238/Pu dioxide fuel for use in Milliwatt Generator heat sources was studied in an attempt to more clearly define the production fuel preloading procedures. The study indicated that water was not present or being adsorbed at various steps of the process (or during storage) that could lead to compatibility problems during pretreatment or long-term storage. The moisture content of the plutonium dioxide was analyzed by a commercial moisture analyzer. The moisture content at all steps of the process including storage averaged from 0.002% to 0.005%. The moisture content of the plutonium dioxide exposed to moist atmosphere for 7 days was 0.001%. These values indicated that no significant amount of moisture was adsorbed by the plutonium dioxide fuel charges. The only significant moisture content found was an average of 3.47%, after self-calcination. This was expected since no additional steps, other than self-heating of the fuel, are taken to remove the water.

  6. /sup 238/Pu fuel form processes. Quarterly report, April-June 1982

    SciTech Connect

    j

    1982-11-01

    Progress in studies of /sup 238/Pu fuel form processes is reported. Analytical studies of weld-quench cracking in DOP-26 iridium alloy-clad vent sets in General Purpose Heat Sources (GPHS) showed that weld-quench cracking is much more severe in MER alloy than in LR and NR alloys. Spark source mass spectrometry indicated that areas in DOP-26 alloy with severe weld-quench cracking have high thorium inhomogeneity. Secondary ion mass spectrometry revealed differences in LR and MR alloys that may be related to their dissimilar susceptibilities for weld-quench cracking. Impact ductility tests showed that welds in DOP-26 alloy clad vent sets made using parameters similar to PuFF production welding had high elongations. Decontamination of encapsulated GPHS pellets in PuFF was demonstrated using a solution of 3.5 M HNO/sub 3/ + 6.4 M HF which is capable of reducing transferable contamination below the specified 10/sup 3/ dpm upper limit in <30 minutes at a bath temperature of 80/sup 0/C using ultrasonic cleaning. Decontamination vessels were constructed to trap and condense acid vapors during decontamination. Impact and metallographic data showed that although the micro and macrostructures between LANL and SRL pellets have large differences, the difference in impact response between these two types of pellets is not correspondingly large. Both types of pellets have impacted successfully. The micro and macrostructures of SRP pellets made with either low fired shards sintered in Ar/5%O/sub 2/ or Ar are intermediate between those of the LANL and SRL pellets. Therefore, either type of SRP pellet should impact successfully.

  7. Improving the Assay of 239Pu in Spent and Melted Fuel Using the Nuclear Resonance Fluorescence Integral Resonance Transmission Method

    NASA Astrophysics Data System (ADS)

    Angell, C. T.; Hayakawa, T.; Shizuma, T.; Hajima, R.; Quiter, B. J.; Ludewigt, B. A.; Karwowski, H.; Rich, G.

    2015-10-01

    Non-destructive assay (NDA) of 239Pu in spent nuclear fuel is possible using the isotope-specific nuclear resonance fluorescence (NRF) integral resonance transmission (IRT) method. The IRT method measures the absorption of photons from a quasi-monoenergetic γ-ray beam due to all resonances in the energy width of the beam. According to calculations the IRT method could greatly improve assay times for 239Pu in nuclear fuel. To demonstrate and verify the IRT method, the IRT signature was first measured in 181Ta, whose nuclear resonant properties are similar to those of 239Pu, and then measured in 239Pu. These measurements were done using the quasi-monoenergetic beam at the High Intensity γ-ray Source (HIγS) in Durham, NC, USA. The IRT signature was observed as a decrease in scattering strength when the same isotope material was placed upstream of the scattering target. The results confirm the validity of the IRT method in both 181Ta and 239Pu.

  8. Full-length U-xPu-10Zr (x=0, 8, 19 wt%) Fast Reactor Fuel Test in FFTF

    SciTech Connect

    D. L. Porter; H.C. Tsai

    2012-08-01

    The Integral Fast Reactor-1 (IFR-1) experiment performed in the Fast Flux Test Facility (FFTF) was the only U-Pu-10Zr (Pu-0, 8 and 19 wt%) metallic fast reactor test with commercial-length (91.4 cm active fuel column length) conducted to date. With few remaining test reactors there is little opportunity for performing another test with a long active fuel column. The assembly was irradiated to the goal burnup of 10 at.%. The beginning of life (BOL) peak cladding temperature of the hottest pin was 608?C, cooling to 522?C at end of life (EOL). Selected fuel pins were examined non destructively using neutron radiography, precision axial gamma scanning, and both laser and spiral contact cladding profilometry. Destructive exams included plenum gas pressure, volume, and gas composition determinations on a number of pins followed by optical metallography, electron probe microanalysis (EPMA), and alpha and beta gamma autoradiography on a single U-19Pu-10Zr pin. The post-irradiation examinations (PIEs) showed very few differences compared to the short-pin (34.3 cm fuel column) testing performed on fuels of similar composition in Experimental Breeder Reactor-II (EBR-II). The fuel column grew axially slightly less than observed in the short pins, but with the same pattern of decreasing growth with increasing Pu content. There was a difference in the fuel-cladding chemical interaction (FCCI) in that the maximum cladding penetration by interdiffusion with fuel/fission products did not occur at the top of the fuel column where the cladding temperature is highest, as observed in EBR-II tests. Instead, the more exaggerated fission-rate profile of the FFTF pins resulted in a peak FCCI at ~0.7 X/L axial location along the fuel column. This resulted from a lower production of rare earth fission products higher in the fuel column as well as a much smaller delta-T between fuel center and cladding, and therefore less FCCI, despite the higher cladding temperature. This behavior could

  9. Phase Characteristics of a Number of U-Pu-Am-Np-Zr Metallic Alloys for Use as Fast Reactor Fuels

    SciTech Connect

    Douglas E. Burkes; J. Rory Kennedy; Thomas Hartmann; Cynthia A. Papesch; Denis D. Keiser, Jr.

    2010-01-01

    Metallic fuel alloys consisting of uranium, plutonium, and zirconium with minor additions of americium and neptunium are under evaluation for potential use to transmute long-lived transuranic actinide isotopes in fast reactors. A series of test designs for the Advanced Fuel Cycle Initiative (AFCI) have been irradiated in the Advanced Test Reactor (ATR), designated as the AFC-1 and AFC-2 designs. Metal fuel compositions in these designs have included varying amounts of U, Pu, Zr, and minor actinides (Am, Np). Investigations into the phase behavior and relationships based on the alloy constituents have been conducted using x-ray diffraction and differential thermal analysis. Results of these investigations, along with proposed relationships between observed behavior and alloy composition, are provided. In general, observed behaviors can be predicted by a ternary U-Pu-Zr phase diagram, with transition temperatures being most dependent on U content. Furthermore, the enthalpy associated with transitions is strongly dependent on the as-cast microstructural characteristics.

  10. Full-length U-xPu-10Zr (x = 0, 8, 19 wt.%) fast reactor fuel test in FFTF

    NASA Astrophysics Data System (ADS)

    Porter, D. L.; Tsai, Hanchung

    2012-08-01

    The Integral Fast Reactor-1 (IFR-1) experiment performed in the Fast Flux Test Facility (FFTF) was the only U-Pu-10Zr (Pu-0, 8 and 19 wt.%) metallic fast reactor test with commercial-length (91.4-cm active fuel-column length) conducted to date. With few remaining test reactors, there is little opportunity for performing another test with a long active fuel column. The assembly was irradiated to the goal burnup of 10 at.%. The beginning-of-life (BOL) peak cladding temperature of the hottest pin was 608 °C, cooling to 522 °C at end-of-life (EOL). Selected fuel pins were examined non-destructively using neutron radiography, precision axial gamma scanning, and both laser and spiral contact cladding profilometry. Destructive exams included plenum gas pressure, volume, and gas composition determinations on a number of pins followed by optical metallography, electron probe microanalysis (EPMA), and alpha and beta-gamma autoradiography on a single U-19Pu-10Zr pin. The post-irradiation examinations (PIEs) showed very few differences compared to the short-pin (34.3-cm fuel column) testing performed on fuels of similar composition in Experimental Breeder Reactor-II (EBR-II). The fuel column grew axially slightly less than observed in the short pins, but with the same pattern of decreasing growth with increasing Pu content. There was a difference in the fuel-cladding chemical interaction (FCCI) in that the maximum cladding penetration by interdiffusion with fuel/fission products did not occur at the top of the fuel column where the cladding temperature is highest, as observed in EBR-II tests. Instead, the more exaggerated fission-rate profile of the FFTF pins resulted in a peak FCCI at ˜0.7 X/L axial location along the fuel column. This resulted from a higher production of rare-earth fission products at this location and a higher ΔT between fuel center and cladding than at core center, together providing more rare earths at the cladding and more FCCI. This behavior could

  11. Space and Time Distribution of Pu Isotopes inside The First Experimental Fuel Pin Designed for PWR and Manufactured in Indonesia

    NASA Astrophysics Data System (ADS)

    Suwardi; Setiawan, J.; Susilo, J.

    2017-01-01

    The first short fuel pin containing natural UO2 pellet in Zry4 cladding has been prepared and planned to be tested in power ramp irradiation. An irradiation test should be designed to allow an experiment can be performed safely and giving maximum results of many performance aspects of design and manufacturing. Performance analysis to the fuel specimen shows that the specimen is not match to be used for power ramp testing. Enlargement by 0.20 mm of pellet diameter has been proposed. The present work is evaluation of modified design for important aspect of isotopic Pu distribution during irradiation test, because generated Pu isotopes in natural UO2 fuel, contribute more power relative to the contribution by enriched UO2 fuel. The axial profile of neutrons flux have been chosen from both experimental measurement and model calculation. The parameters of ramp power has been obtained from statistical experiment data. A simplified and typical base-load commercial PHWR profile of LHR history has been chosen, to determine the minimum irradiation time before ramp test can be performed. The data design and Mat pro XI materials properties models have been chosen. The axial profile of neutrons flux has been accommodated by 5 slices of discrete pin. The Pu distribution of slice-4 with highest power rate has been chosen to be evaluated. The radial discretion of pellet and cladding and numerical parameter have been used the default best practice of TU. The results shows that Pu 239 increased rapidly. The maximum burn up of slice 4 at upper the median slice, it reached nearly 90% of maximum value at about 6000 h with peak of 0.8%a Pu/HM at 22000 h, which is higher than initial U 235. Each 240, 241 and 240 Pu grows slower and ends up to 0.4, 0.2 and 0.18 % respectively. This results can be used for verification of other aspect of fuel behavior in the modeling results and also can be used as guide and comparison to the future post irradiation examination for Pu isotopes distribution.

  12. Modeling of Selected Ceramic Processing Parameters Employed in the Fabrication of 238PuO 2 Fuel Pellets

    NASA Astrophysics Data System (ADS)

    Brockman, R. A.; Kramer, D. P.; Barklay, C. D.; Cairns-Gallimore, D.; Brown, J. L.; Huling, J. C.; Van Pelt, C. E.

    Recent deep space missions utilize the thermal output of the radioisotope plutonium-238 as the fuel in the thermal to electrical power system. Since the application of plutonium in its elemental state has several disadvantages, the fuel employed in these deep space power systems is typically in the oxide form such as plutonium-238 dioxide (238PuO2). As an oxide, the processing of the plutonium dioxide into fuel pellets is performed via "classical" ceramic processing unit operations such as sieving of the powder, pressing, sintering, etc. Modeling of these unit operations can be beneficial in the understanding and control of processing parameters with the goal of further enhancing the desired characteristics of the 238PuO2 fuel pellets. A finite element model has been used to help identify the time-temperature-stress profile within a pellet during a furnace operation taking into account that 238PuO2 itself has a significant thermal output. Results of the modeling efforts will be discussed.

  13. Modeling of selected ceramic processing parameters employed in the fabrication of 238PuO2 fuel pellets

    DOE PAGES

    Brockman, R. A.; Kramer, D. P.; Barklay, C. D.; ...

    2011-10-01

    Recent deep space missions utilize the thermal output of the radioisotope plutonium-238 as the fuel in the thermal to electrical power system. Since the application of plutonium in its elemental state has several disadvantages, the fuel employed in these deep space power systems is typically in the oxide form such as plutonium-238 dioxide (238PuO2). As an oxide, the processing of the plutonium dioxide into fuel pellets is performed via ''classical'' ceramic processing unit operations such as sieving of the powder, pressing, sintering, etc. Modeling of these unit operations can be beneficial in the understanding and control of processing parameters withmore » the goal of further enhancing the desired characteristics of the 238PuO2 fuel pellets. A finite element model has been used to help identify the time-temperature-stress profile within a pellet during a furnace operation taking into account that 238PuO2 itself has a significant thermal output. The results of the modeling efforts will be discussed.« less

  14. Analysis of Pu-Only Partitioning Strategies in LMFBR Fuel Cycles

    SciTech Connect

    Samuel Bays; Gilles Youinou

    2013-02-01

    sold to the MOX LWRs. The third scenario considered a LMFBR fuel cycle in an expansionary mode where excess bred transuranic material is accumulated for spinning off additional LMFBR cores. In this latter scenario, no plutonium partitioning was considered. After every cycle, transuranic from both driver and blankets is sold to the MOX LWRs. The MA production from LMFBR operated in a Pu-only fuel cycle is roughly only 1% that of the transuranic production rate. This is in contrast to LWR fuel cycles where the MA content in TRU is closer to 10% or more. If such a LMFBR were operated to provide fissile material to a fleet of MOX reactors, then 1 GWe of LMFBR could support between approximately 0.11 and 0.43 GWe of LWR-MOX reactors for a LMFBR conversion ratio between 1.1 and 1.5, if the MOX reactors were operated in a once-through-then out mode. If the plutonium is continuously recycled in the MOX reactors then the support ratio is approximately 1 GWe of LMFBR for between 0.13 and 0.65 GWe of LWR-MOX reactors depending on the LMFBR conversion ratio. Also, it was found that if the LMFBR fleet were operated in a purely expansionary mode, the smallest doubling time achievable would be seven years.

  15. Physical characteristics of LWRs and SCLWRs loaded by ({sup 233}U-Th-{sup 238}U) oxide fuel with small additions of {sup 231}Pa

    SciTech Connect

    Kulikov, E.G.; Shmelev, A.N.; Apse, V.A.; Kulikov, G.G.

    2007-07-01

    The paper investigates the possibility and attractiveness of using (U-Th) fuel in light-water reactors (LWRs) and in light-water reactors with super-critical coolant parameters (SCLWRs). It is proposed to dilute {sup 233}U with {sup 238}U to enhance the proliferation resistance of this fissionable isotope. If is noteworthy that she idea was put forward for the first time by she well known American physicist and participant of the Manhattan Project Dr. T. Taylor. Various fuel compositions are analyzed and compared on fuel breeding, achievable values of fuel burn-up and cross-sections of parasitic neutron absorption. It is also demonstrated that small {sup 231}Pa additions (several percent) into the fuel allows: to increase fuel burn-up, to achieve more negative temperature reactivity coefficient of coolant and to enhance nonproliferation of the fuel. (authors)

  16. Results of irradiation of (U0.55Pu0.45)N and (U0.4Pu0.6)N fuels in BOR-60 up to ˜12 at.% burn-up

    NASA Astrophysics Data System (ADS)

    Rogozkin, B. D.; Stepennova, N. M.; Fedorov, Yu. Ye.; Shishkov, M. G.; Kryukov, F. N.; Kuzmin, S. V.; Nikitin, O. N.; Belyaeva, A. V.; Zabudko, L. M.

    2013-09-01

    In the article presented are the results of post-irradiation tests of helium bonded fuel pins with mixed mononitride fuel (U0.55Pu0.45)N and (U0.4Pu0.6)N having 85% density irradiated in BOR-60 reactor. Achieved maximum burn-up was, respectively, equal to 9.4 and 12.1 at.% with max linear heat rates 41.9 and 54.5 kW/m. Maximum irradiation dose was 43 dpa. No damage of claddings made of ChS-68 steel (20% cold worked) was observed, and ductility margin existed. Maximum depth of cladding corrosion was within 15 μm. Swelling rates of (U0.4Pu0.6)N and (U0.55Pu0.45)N were, respectively, ˜1.1% and ˜0.68% per 1 at.%. Gas release rate did not exceed 19.3% and 19%. Pattern of porosity distribution in the fuel influenced fuel swelling and gas release rates. Plutonium and uranium are uniformly distributed in the fuel, local minimum values of their content being caused by pores and cracks in the pellets. The observable peaks in content distribution are probably connected with the local formation of isolated phases (e.g. Mo, Pd) while the minimum values refer to fuel pores and cracks. Xenon and cesium tend to migrate from the hot sections of fuel, and therefore their min content is observed in the central section of the fuel pellets. Phase composition of the fuel was determined with X-ray diffractometer. The X-ray patterns of metallographic specimens were obtained by the scanning method (the step was 0.02°, the step exposition was equal to 2 s). From the X-ray diffraction analysis data, it follows that the nitrides of both fuel types have the single-phase structure with an FCC lattice (see Table 6).

  17. Development of spent fuel reprocessing process based on selective sulfurization: Study on the Pu, Np and Am sulfurization

    NASA Astrophysics Data System (ADS)

    Kirishima, Akira; Amano, Yuuki; Nihei, Toshifumi; Mitsugashira, Toshiaki; Sato, Nobuaki

    2010-03-01

    For the recovery of fissile materials from spent nuclear fuel, we have proposed a novel reprocessing process based on selective sulfurization of fission products (FPs). The key concept of this process is utilization of unique chemical property of carbon disulfide (CS2), i.e., it works as a reductant for U3O8 but works as a sulfurizing agent for minor actinides and lanthanides. Sulfurized FPs and minor actinides (MA) are highly soluble to dilute nitric acid while UO2 and PuO2 are hardly soluble, therefore, FPs and MA can be removed from Uranium and Plutonium matrix by selective dissolution. As a feasibility study of this new concept, the sulfurization behaviours of U, Pu, Np, Am and Eu are investigated in this paper by the thermodynamical calculation, phase analysis of chemical analogue elements and tracer experiments.

  18. Evaluation of Aqueous and Powder Processing Techniques for Production of Pu-238-Fueled General Purpose Heat Sources

    SciTech Connect

    Not Available

    2008-06-01

    This report evaluates alternative processes that could be used to produce Pu-238 fueled General Purpose Heat Sources (GPHS) for radioisotope thermoelectric generators (RTG). Fabricating GPHSs with the current process has remained essentially unchanged since its development in the 1970s. Meanwhile, 30 years of technological advancements have been made in the fields of chemistry, manufacturing, ceramics, and control systems. At the Department of Energy’s request, alternate manufacturing methods were compared to current methods to determine if alternative fabrication processes could reduce the hazards, especially the production of respirable fines, while producing an equivalent GPHS product. An expert committee performed the evaluation with input from four national laboratories experienced in Pu-238 handling.

  19. Feedback components of a U20Pu10Zr-fueled compared to a U10Zr-fueled EBR-II

    SciTech Connect

    Meneghetti, D.; Kucera, D.A.

    1988-12-31

    Calculated feedback components of the regional contributions of the power reactivity decrements (PRDs) and of the temperature coefficients of reactivity of a U20Pu10Zr-fueled and of a U10Zr-fueled Experimental Breeder Reactor II (EBR-II) are compared. The PRD components are also separated into power-to-flow dependent and solely power dependent parts. The effects of these values upon quantities useful for indicating the comparative potential inherent safety characteristics of these EBR-II loadings are presented.

  20. Feedback components of a U20Pu10Zr-fueled compared to a U10Zr-fueled EBR-II

    SciTech Connect

    Meneghetti, D.; Kucera, D.A.

    1988-01-01

    Calculated feedback components of the regional contributions of the power reactivity decrements (PRDs) and of the temperature coefficients of reactivity of a U20Pu10Zr-fueled and of a U10Zr-fueled Experimental Breeder Reactor II (EBR-II) are compared. The PRD components are also separated into power-to-flow dependent and solely power dependent parts. The effects of these values upon quantities useful for indicating the comparative potential inherent safety characteristics of these EBR-II loadings are presented.

  1. Experimental studies of U-Pu-Zr fast reactor fuel pins in EBR-II (Experimental Breeder Reactor)

    SciTech Connect

    Pahl, R.G.; Porter, D.L.; Lahm, C.E.; Hofman, G.L.

    1988-01-01

    The Integral Fast Reactor (IFR) is a generic reactor concept under development by Argonne National Laboratory. Much of the technology for the IFR is being demonstrated at the Experimental Breeder Reactor II (EBR-II) on the Department of Energy site near Idaho Falls, Idaho. The IFR concept relies on four technical features to achieve breakthroughs in nuclear power economics and safety: (1) a pool-type reactor configuration, (2) liquid sodium cooling, (3) metallic fuel, and (4) an integral fuel cycle with on-site reprocessing. The purpose of this paper will be to summarize our latest results of irradiation testing uranium-plutonium-zirconium (U-Pu-Zr) fuel in the EBR-II. 10 refs., 13 figs., 2 tabs.

  2. High-silicon {sup 238}PuO{sub 2} fuel characterization study: Half module impact tests

    SciTech Connect

    Reimus, M.A.H.

    1997-01-01

    The General-Purpose Heat Source (GPHS) provides power for space missions by transmitting the heat of [sup 238]Pu decay to an array of thermoelectric elements. The modular GPHS design was developed to address both survivability during launch abort and return from orbit. Previous testing conducted in support of the Galileo and Ulysses missions documented the response of GPHSs to a variety of fragment- impact, aging, atmospheric reentry, and Earth-impact conditions. The evaluations documented in this report are part of an ongoing program to determine the effect of fuel impurities on the response of the heat source to conditions baselined during the Galileo/Ulysses test program. In the first two tests in this series, encapsulated GPHS fuel pellets containing high levels of silicon were aged, loaded into GPHS module halves, and impacted against steel plates. The results show no significant differences between the response of these capsules and the behavior of relatively low-silicon fuel pellets tested previously.

  3. Conceptual design for a receiving station for the nondestructive assay of PuO/sub 2/ at the fuels and materials examination facility

    SciTech Connect

    Sampson, T.E.; Speir, L.G.; Ensslin, N.; Hsue, S.T.; Johnson, S.S.; Bourret, S.; Parker, J.L.

    1981-11-01

    We propose a conceptual design for a receiving station for input accountability measurements on PuO/sub 2/ received at the Fuels and Materials Examination Facility at the Hanford Engineering Development Laboratory. Nondestructive assay techniques are proposed, including neutron coincidence counting, calorimetry, and isotopic determination by gamma-ray spectroscopy, in a versatile data acquisition system to perform input accountability measurements with precisions better than 1% at throughputs of up to 2 M.T./yr of PuO/sub 2/.

  4. 238PuO2 Fuel and Dosimetry

    SciTech Connect

    Mayo, Douglas R.; Rawool-Sullivan, Mohini; Garner, Scott Edward; Wenz, Tracy R.; Karpius, Peter Joseph

    2016-06-01

    238Pu is an ideal material for use as a heat source with its half-life of 87.7 years and copious particle emissions. 238Pu radioisotope thermoelectric generators (RTGs) have found use for pacemakers, Apollo Space missions, Mars rovers, and Voyager spacecraft. In evaluating the dose to personnel and components near a 238Pu-based RTG, a number of additional nuclides and their daughter products must be considered to get an accurate estimate for γ-dose, and the amount of 17O and 18O for the neutron-dose must be considered. This paper looks at the contributing nuclides and their daughter products that add the most to the dose rates.

  5. Direct Measurement of U235 and Pu239 in Spent Fuel Rods with Gamma-Ray Mirrors

    SciTech Connect

    Ziock, Klaus-Peter; Alameda, J. B.; Brejnholt, N. F.; Decker, T. A.; Descalle, M. A.; Fernandez-Perea, M.; Hill, R. M.; Kisner, R. A.; Melin, A. M.; Patton, B. W.; Ruz, J.; Soufli, R.

    2013-09-30

    The amounts of fissile Pu and U in spent nuclear fuel are of primary concern to the safeguards community. In particular, there are issues when safeguards transitions from an item accountancy basis (such as fuel bundles) to a fissile material mass basis as occurs when spent fuel enters a reprocessing plant. Discrepancies occur because item accountancy requires estimating the content of fissile material using indirect techniques such as the fuel burn-up and item-level measurements of radiation emissions from fission by-products. Direct measurement of the fissile content by monitoring line emissions from fissile species themselves is impossible because the lines are much weaker than those emitted by shorter-lived isotopes in the fuel. The goal of this project is to develop a technique to directly measure these weaker lines despite the presence of overwhelming radiation from other isotopes. This is achieved by using gamma-ray mirrors as a narrow band-pass filter. The mirrors reflect only energies of interest toward a HPGe detector that is shielded from direct view of the spent fuel and its fierce emissions. This can significantly improve the reliability with which the mass of fissile material is tracked.

  6. Oxidative dissolution of unirradiated Mimas MOX fuel (U/Pu oxides) in carbonated water under oxic and anoxic conditions

    NASA Astrophysics Data System (ADS)

    Odorowski, Mélina; Jégou, Christophe; De Windt, Laurent; Broudic, Véronique; Peuget, Sylvain; Magnin, Magali; Tribet, Magaly; Martin, Christelle

    2016-01-01

    Few studies exist concerning the alteration of Mimas Mixed-OXide (MOX) fuel, a mixed plutonium and uranium oxide, and data is needed to better understand its behavior under leaching, especially for radioactive waste disposal. In this study, two leaching experiments were conducted on unirradiated MOX fuel with a strong alpha activity (1.3 × 109 Bq.gMOX-1 reproducing the alpha activity of spent MOX fuel with a burnup of 47 GWd·tHM-1 after 60 years of decay), one under air (oxic conditions) for 5 months and the other under argon (anoxic conditions with [O2] < 1 ppm) for one year in carbonated water (10-2 mol L-1). For each experiment, solution samples were taken over time and Eh and pH were monitored. The uranium in solution was assayed using a kinetic phosphorescence analyzer (KPA), plutonium and americium were analyzed by a radiochemical route, and H2O2 generated by the water radiolysis was quantified by chemiluminescence. Surface characterizations were performed before and after leaching using Scanning Electron Microscopy (SEM), Electron Probe Microanalyzer (EPMA) and Raman spectroscopy. Solubility diagrams were calculated to support data discussion. The uranium releases from MOX pellets under both oxic and anoxic conditions were similar, demonstrating the predominant effect of alpha radiolysis on the oxidative dissolution of the pellets. The uranium released was found to be mostly in solution as carbonate species according to modeling, whereas the Am and Pu released were significantly sorbed or precipitated onto the TiO2 reactor. An intermediate fraction of Am (12%) was also present as colloids. SEM and EPMA results indicated a preferential dissolution of the UO2 matrix compared to the Pu-enriched agglomerates, and Raman spectroscopy showed the Pu-enriched agglomerates were slightly oxidized during leaching. Unlike Pu-enriched zones, the UO2 grains were much more sensitive to oxidative dissolution, but the presence of carbonates did not enable observation of an

  7. Microwave based oxidation process for recycling the off-specification (U,Pu)O2 fuel pellets

    NASA Astrophysics Data System (ADS)

    Singh, G.; Khot, P. M.; Kumar, Pradeep; Bhatt, R. B.; Behere, P. G.; Afzal, Mohd

    2017-02-01

    This paper reports development of a process named MicroWave Direct Oxidation (MWDO) for recycling the off-specification (U,Pu)O2 mixed oxide (MOX) fuel pellets generated during fabrication of typical fast reactor fuels. MWDO is a two-stage, single-cycle process based on oxidative pulverisation of pellets using 2450 MHz microwave. The powder sinterability was evaluated by bulk density and BET specific surface area. The oxidised powders were analyzed for phases using XRD and stoichiometry by thermogravimetry. The sinterability was significantly enhanced by carrying out oxidation in higher oxygen partial pressure and by subjecting MOX to multiple micronisation-oxidation cycles. After three cycles, the recycled powder from (U,28%Pu)O2 resulted surface area >3 m2/g and 100% re-used for MOX fabrication. The flow sheet was developed for maximum utilization of recycled powder describable by a parameter called Scrap Recycling Ratio (SRR). The process demonstrates smaller processing cycle, better powder properties and higher oxidative pulverisation over conventional method.

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

    PubMed

    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.

  9. Fully Coupled Modeling of Burnup-Dependent (U1- y , Pu y )O2- x Mixed Oxide Fast Reactor Fuel Performance

    NASA Astrophysics Data System (ADS)

    Liu, Rong; Zhou, Wenzhong; Zhou, Wei

    2016-03-01

    During the fast reactor nuclear fuel fission reaction, fission gases accumulate and form pores with the increase of fuel burnup, which decreases the fuel thermal conductivity, leading to overheating of the fuel element. The diffusion of plutonium and oxygen with high temperature gradient is also one of the important fuel performance concerns as it will affect the fuel material properties, power distribution, and overall performance of the fuel pin. In order to investigate these important issues, the (U1- y Pu y )O2- x fuel pellet is studied by fully coupling thermal transport, deformation, oxygen diffusion, fission gas release and swelling, and plutonium redistribution to evaluate the effects on each other with burnup-dependent models, accounting for the evolution of fuel porosity. The approach was developed using self-defined multiphysics models based on the framework of COMSOL Multiphysics to manage the nonlinearities associated with fast reactor mixed oxide fuel performance analysis. The modeling results showed a consistent fuel performance comparable with the previous results. Burnup degrades the fuel thermal conductivity, resulting in a significant fuel temperature increase. The fission gas release increased rapidly first and then steadily with the burnup increase. The fuel porosity increased dramatically at the beginning of the burnup and then kept constant as the fission gas released to the fuel free volume, causing the fuel temperature to increase. Another important finding is that the deviation from stoichiometry of oxygen affects greatly not only the fuel properties, for example, thermal conductivity, but also the fuel performance, for example, temperature distribution, porosity evolution, grain size growth, fission gas release, deformation, and plutonium redistribution. Special attention needs to be paid to the deviation from stoichiometry of oxygen in fuel fabrication. Plutonium content will also affect the fuel material properties and performance

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

    SciTech Connect

    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.

  11. Modeling Constituent Redistribution in U-Pu-Zr Metallic Fuel Using the Advanced Fuel Performance Code BISON

    SciTech Connect

    Douglas Porter; Steve Hayes; Various

    2014-06-01

    The Advanced Fuels Campaign (AFC) metallic fuels currently being tested have higher zirconium and plutonium concentrations than those tested in the past in EBR reactors. Current metal fuel performance codes have limitations and deficiencies in predicting AFC fuel performance, particularly in the modeling of constituent distribution. No fully validated code exists due to sparse data and unknown modeling parameters. Our primary objective is to develop an initial analysis tool by incorporating state-of-the-art knowledge, constitutive models and properties of AFC metal fuels into the MOOSE/BISON (1) framework in order to analyze AFC metallic fuel tests.

  12. Steady-state irradiation testing of U-Pu-Zr fuel to >18% burnup

    SciTech Connect

    Pahl, R.G.; Wisner, R.S. ); Billone, M.C.; Hofman, G.L. )

    1990-01-01

    Tests of austenitic stainless steel clad U-xP-10Zr fuel (x=o, 8, 19 wt. %) to peak burnups as high as 18.4 at. % have been completed in the EBR-II. Fuel swelling and fractional fission gas release are slowly increasing functions of burnup beyond 2 at. % burnup. Increasing plutonium content in the fuel reduces swelling and decreases the amount of fission gas which diffuses from fuel to plenum. LIFE-METAL code modelling of cladding strains is consistent with creep by fission gas loading and irradiation-induced swelling mechanisms. Fuel/cladding chemical interaction involves the ingress of rare-earth fission products. Constituent redistribution in the fuel had not limited steady-state performance. Cladding breach behavior at closure welds, in the gas plenum, and in the fuel column region have been benign events. 3 refs., 5 figs.

  13. Imminent: Irradiation Testing of (Th,Pu)O{sub 2} Fuel - 13560

    SciTech Connect

    Kelly, Julian F.; Franceschini, Fausto

    2013-07-01

    Commercial-prototype thorium-plutonium oxide (Th-MOX) fuel pellets have been loaded into the material test reactor in Halden, Norway. The fuel is being operated at full power - with instrumentation - in simulated LWR / PHWR conditions and its behaviour is measured 'on-line' as it operates to high burn-up. This is a vital test on the commercialization pathway for this robust new thoria-based fuel. The performance data that is collected will support a fuel modeling effort to support its safety qualification. Several different samples of Th-MOX fuel will be tested, thereby collecting information on ceramic behaviours and their microstructure dependency. The fuel-cycle reasoning underpinning the test campaign is that commercial Th- MOX fuels are an achievable intermediate / near-term SNF management strategy that integrates well with a fast reactor future. (authors)

  14. Chemical states of fission products in irradiated (U 0.3Pu 0.7)C 1+ x fuel at high burn-ups

    NASA Astrophysics Data System (ADS)

    Agarwal, Renu; Venugopal, V.

    2006-12-01

    The chemical states of fission products have been theoretically determined for the irradiated carbide fuel of Fast Breeder Test Reactor (FBTR) at Kalpakkam, India, at different burn-ups. The SOLGASMIX-PV computer code was used to determine the equilibrium chemical composition of the fuel. The system was assumed to be composed of a gaseous phase at one atmosphere pressure, and various solid phases. The distribution of elements in these phases and their chemical states at different temperatures were calculated as a function of burn-up. The FBTR fuel, (U 0.3Pu 0.7)C 1+ x, was loaded with C/M values in the range, 1.03-1.06. The present calculations indicated that even for the lowest starting C/M of 1.03 in the FBTR fuel, the liquid metal phase of (U, Pu), should not appear at a burn-up as high as 150 GWd/t.

  15. Coprocessed nuclear fuels containing (U, Pu) values as oxides, carbides or carbonitrides

    DOEpatents

    Lloyd, Milton H.

    1983-01-01

    Method for direct coprocessing of nuclear fuels derived from a product stream of a fuels reprocessing facility containing uranium, plutonium, and fission product values comprising nitrate stabilization of said stream vacuum concentration to remove water and nitrates, neutralization to form an acid deficient feed solution for the internal gelation mode of sol-gel technology, green spherule formation, recovery and treatment for loading into a fuel element by vibra packed or pellet formation technologies.

  16. Coprocessed nuclear fuels containing (U, Pu) values as oxides, carbides or carbonitrides

    DOEpatents

    Lloyd, M.H.

    1981-01-09

    Method for direct coprocessing of nuclear fuels derived from a product stream of fuels reprocessing facility containing uranium, plutonium, and fission product values comprising nitrate stabilization of said stream vacuum concentration to remove water and nitrates, neutralization to form an acid deficient feed solution for the internal gelation mode of sol-gel technology, green spherule formation, recovery and treatment for loading into a fuel element by vibra packed or pellet formation technologies.

  17. The thermal conductivity of mixed fuel UxPu1-xO2: molecular dynamics simulations

    SciTech Connect

    Liu, Xiang-Yang; Cooper, Michael William Donald; Stanek, Christopher Richard; Andersson, Anders David Ragnar

    2015-10-16

    Mixed oxides (MOX), in the context of nuclear fuels, are a mixture of the oxides of heavy actinide elements such as uranium, plutonium and thorium. The interest in the UO2-PuO2 system arises from the fact that these oxides are used both in fast breeder reactors (FBRs) as well as in pressurized water reactors (PWRs). The thermal conductivity of UO2 fuel is an important material property that affects fuel performance since it is the key parameter determining the temperature distribution in the fuel, thus governing, e.g., dimensional changes due to thermal expansion, fission gas release rates, etc. For this reason it is important to understand the thermal conductivity of MOX fuel and how it differs from UO2. Here, molecular dynamics (MD) simulations are carried out to determine quantitatively, the effect of mixing on the thermal conductivity of UxPu1-xO2, as a function of PuO2 concentrations, for a range of temperatures, 300 – 1500 K. The results will be used to develop enhanced continuum thermal conductivity models for MARMOT and BISON by INL. These models express the thermal conductivity as a function of microstructure state-variables, thus enabling thermal conductivity models with closer connection to the physical state of the fuel.

  18. LWR spent fuel reduction by the removal of U and the compact storage of Pu with FP for long-term nuclear sustainability

    SciTech Connect

    Fukasawa, T.; Hoshino, K.; Takano, M.; Sato, S.; Shimazu, Y.

    2013-07-01

    Fast breeder reactors (FBR) nuclear fuel cycle is needed for long-term nuclear sustainability while preventing global warming and maximum utilizing the limited uranium (U) resources. The 'Framework for Nuclear Energy Policy' by the Japanese government on October 2005 stated that commercial FBR deployment will start around 2050 under its suitable conditions by the successive replacement of light water reactors (LWR) to FBR. Even after Fukushima Daiichi Nuclear Power Plant accident which made Japanese tendency slow down the nuclear power generation activities, Japan should have various options for energy resources including nuclear, and also consider the delay of FBR deployment and increase of LWR spent fuel (LWR-SF) storage amounts. As plutonium (Pu) for FBR deployment will be supplied from LWR-SF reprocessing and Japan will not possess surplus Pu, the authors have developed the flexible fuel cycle initiative (FFCI) for the transition from LWR to FBR. The FFCI system is based on the possibility to stored recycled materials (U, Pu)temporarily for a suitable period according to the FBR deployment rate to control the Pu demand/supply balance. This FFCI system is also effective after the Fukushima accident for the reduction of LWR-SF and future LWR-to-FBR transition. (authors)

  19. Quantification of Uncertainties due to 235,238U, 239,240,241Pu and Fission Products Nuclear Data Uncertainties for a PWR Fuel Assembly

    NASA Astrophysics Data System (ADS)

    da Cruz, D. F.; Rochman, D.; Koning, A. J.

    2014-04-01

    Uncertainty analysis on reactivity and discharged inventory for a typical PWR fuel element as a result of uncertainties in 235,238U, 239,240,241Pu, and fission products nuclear data was performed. The Total Monte-Carlo (TMC) method was applied using the deterministic transport code DRAGON. The nuclear data used in this study is from the JEFF-3.1 evaluations, with the exception of the nuclear data files for U, Pu and fission products isotopes, which are taken from the nuclear data library TENDL-2012. Results show that the calculated total uncertainty in keff (as result of uncertainties in nuclear data of the considered isotopes) is virtually independent on fuel burnp and amounts to 700 pcm. The uncertainties in inventory of the discharged fuel is dependent on the element considered and lies in the range 1-15% for most fission products, and is below 5% for the most important actinides.

  20. Fuel Fraction Analysis of 500 MWth Gas Cooled Fast Reactor with Nitride (UN-PuN) Fuel without Refueling

    NASA Astrophysics Data System (ADS)

    Dewi Syarifah, Ratna; Su’ud, Zaki; Basar, Khairul; Irwanto, Dwi

    2017-01-01

    Nuclear Power Plant (NPP) is one of candidates which can support electricity demand in the world. The Generation IV NPP has fourth main objective, i.e. sustainability, economics competitiveness, safety and reliability, and proliferation and physical protection. One of Gen-IV reactor type is Gas Cooled Fast Reactor (GFR). In this study, the analysis of fuel fraction in small GFR with nitride fuel has been done. The calculation was performed by SRAC code, both Pij and CITATION calculation. SRAC2002 system is a code system applicable to analyze the neutronics of variety reactor type. And for the data library used JENDL-3.2. The step of SRAC calculation is fuel pin calculated by Pij calculation until the data homogenized, after it homogenized we calculate core reactor. The variation of fuel fraction is 40% up to 65%. The optimum design of 500MWth GFR without refueling with 10 years burn up time reach when radius F1:F2:F3 = 50cm:30cm:30cm and height F1:F2:F3 = 50cm:40cm:30cm, variation percentage Plutonium in F1:F2:F3 = 7%:10%:13%. The optimum fuel fraction is 41% with addition 2% Plutonium weapon grade mix in the fuel. The excess reactivity value in this case 1.848% and the k-eff value is 1.01883. The high burn up reached when the fuel fraction is low. In this study 41% fuel fraction produce faster fissile fuel, so it has highest burn-up level than the other fuel fraction.

  1. Pu-Zr alloy for high-temperature foil-type fuel

    DOEpatents

    McCuaig, Franklin D.

    1977-01-01

    A nuclear reactor fuel alloy consists essentially of from slightly greater than 7 to about 4 w/o zirconium, balance plutonium, and is characterized in that the alloy is castable and is rollable to thin foils. A preferred embodiment of about 7 w/o zirconium, balance plutonium, has a melting point substantially above the melting point of plutonium, is rollable to foils as thin as 0.0005 inch thick, and is compatible with cladding material when repeatedly cycled to temperatures above 650.degree. C. Neutron reflux densities across a reactor core can be determined with a high-temperature activation-measurement foil which consists of a fuel alloy foil core sandwiched and sealed between two cladding material jackets, the fuel alloy foil core being a 7 w/o zirconium, plutonium foil which is from 0.005 to 0.0005 inch thick.

  2. Atmospheric deposition, resuspension, and root uptake of Pu in corn and other grain-producing agroecosystems near a nuclear fuel facility.

    PubMed

    Pinder, J E; McLeod, K W; Adriano, D C; Corey, J C; Boni, A L

    1990-12-01

    Plutonium released to the environment may contribute to dose to humans through inhalation or ingestion of contaminated foodstuffs. Plutonium contamination of agricultural plants may result from interception and retention of atmospheric deposition, resuspension of Pu-bearing soil particles to plant surfaces, and root uptake. Plutonium on vegetation surfaces may be transferred to grain surfaces during mechanical harvesting. Data obtained from corn grown near the U.S. Department of Energy's H-Area nuclear fuel chemical separations facility on the Savannah River Site were used to estimate parameters of a simple model of Pu transport in agroecosystems. The parameter estimates for corn were compared to those previously obtained for wheat and soybeans. Despite some differences in parameter estimates among crops, the relative importances of atmospheric deposition, resuspension, and root uptake were similar among crops. For even small deposition rates, the relative importances of processes for Pu contamination of corn grain should be: transfer of atmospheric deposition from vegetation surfaces to grain surfaces during combining greater than resuspension of soil to grain surfaces greater than root uptake. Approximately 3.9 X 10(-5) of a year's atmospheric deposition is transferred to grain. Approximately 6.2 X 10(-9) of the Pu inventory in the soil is resuspended to corn grain, and a further 7.3 X 10(-10) of the soil Pu inventory is absorbed and translocated to grains.

  3. Modeling of selected ceramic processing parameters employed in the fabrication of 238PuO2 fuel pellets

    SciTech Connect

    Brockman, R. A.; Kramer, D. P.; Barklay, C. D.; Cairns-Gallimore, D.; Brown, J. L.; Huling, J. C.; Van Pelt, C. E.

    2011-10-01

    Recent deep space missions utilize the thermal output of the radioisotope plutonium-238 as the fuel in the thermal to electrical power system. Since the application of plutonium in its elemental state has several disadvantages, the fuel employed in these deep space power systems is typically in the oxide form such as plutonium-238 dioxide (238PuO2). As an oxide, the processing of the plutonium dioxide into fuel pellets is performed via ''classical'' ceramic processing unit operations such as sieving of the powder, pressing, sintering, etc. Modeling of these unit operations can be beneficial in the understanding and control of processing parameters with the goal of further enhancing the desired characteristics of the 238PuO2 fuel pellets. A finite element model has been used to help identify the time-temperature-stress profile within a pellet during a furnace operation taking into account that 238PuO2 itself has a significant thermal output. The results of the modeling efforts will be discussed.

  4. Fabrication experience of Al- sup 233 U and Al-Pu plate fuel for the Purnima III and Kamini research reactors

    SciTech Connect

    Ganguly, C.; Prasad, G.J.; Mahule, N.; Ghosh, J.K.; Assari, K.V.J.; Chandrasekharan, K.N.P.; Muralidhar, S.; Balan, T.S.; Roy, P.R. )

    1991-10-01

    This paper reports on aluminum-clad Al-20 wt% {sup 233}U and Al-23 wt% Pu plate fuel subassemblies that have been fabricated for the Purnima III critical facility and the Kamini research reactor. The fabrication flow sheet consists of preparing the master alloy using aluminum and uranium or plutonium metals as feed materials, remelting and casting the fuel alloy ingots, rolling, picture framing and sandwiching the fuel alloy between aluminum sheets, roll bonding, locating the fuel alloy core outline by x-ray radiography, and trimming and machining to final dimensions. Metallic molds produce better ingots than graphite ones. The addition of zirconium during melting improves the microstructure of the Al-U and Al-Pu castings and facilitates hot rolling of the ingots. In the subassembly the fuel plates are finally locked in aluminum spacer grooves by a novel roll-swaging technique. High-resolution x-ray radiographs and microdensitometric scans are utilized to confirm the homogeneous distribution of the fissile material in the fuel plates. Nonbond areas are detected by blister testing and immersion ultrasonic testing of the roll-bonded fuel plates.

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

    SciTech Connect

    Lafleur, Adrienne M; Charlton, William S; Menlove, Howard O; Swinhoe, Martyn T

    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.

  6. An initial assessment of a mechanistic model, GRASS-SST, in U-Pu-Zr metallic alloy fuel fission-gas behavior simulations

    NASA Astrophysics Data System (ADS)

    Yun, Di; Rest, Jeffrey; Hofman, Gerard L.; Yacout, Abdellatif M.

    2013-04-01

    A mechanistic kinetic rate theory model originally developed for the prediction of fission gas behavior in oxide nuclear fuels under steady-state and transient conditions has been assessed to investigate its applicability to model fission gas behavior in U-Pu-Zr metallic alloy fuel. In order to capture and validate the underlying physics for irradiated U-Pu-Zr fuels, the mechanistic model was applied to evaluate fission gas release, fission gas and fission product induced swelling, and detailed gas bubble size distributions in three different fuel zones: the outer α-U, the intermediate, and the inner γ-U zones. Due to its special microstructural features, the α-U zone in U-Pu-Zr fuels is believed to contribute the largest fraction of fission gas release among the different fuel zones. It is shown that with the use of small effective grain sizes, the mechanistic model can predict fission gas release that is in reasonable consistence with (though slightly lower than) experimentally measured data. These simulation results are comparable to the experimentally measured fission gas release since the mechanism of fission gas transport through the densely distributed laminar porosity in the α-U zone is analogous to the mechanism of fission gas transport through the interconnected gas bubble porosity utilized in the mechanistic model. Detailed gas bubble size distributions predicted with the mechanistic model in both the intermediate zone and the high temperature γ-U zone of U-Pu-Zr fuel are also compared to experimental measurements from available SEM micrographs. These comparisons show good agreement between the simulation results and experimental measurements, and therefore provide crucial guidelines for the selection of key physical parameters required for modeling these two zones. Material properties such as fuel grain size and thermal diffusivity of gas and model parameters such as di-atom nucleation probability and gas bubble re-solution constant are predicted

  7. Preliminary Study on LiF4-ThF4-PuF4 Utilization as Fuel Salt of miniFUJI Molten Salt Reactor

    NASA Astrophysics Data System (ADS)

    Waris, Abdul; Aji, Indarta K.; Pramuditya, Syeilendra; Widayani; Irwanto, Dwi

    2016-08-01

    miniFUJI reactor is molten salt reactor (MSR) which is one type of the Generation IV nuclear energy systems. The original miniFUJI reactor design uses LiF-BeF2-ThF4-233UF4 as a fuel salt. In the present study, the use of LiF4-ThF4-PuF4 as fuel salt instead of LiF-BeF2-ThF4-UF4 will be discussed. The neutronics cell calculation has been performed by using PIJ (collision probability method code) routine of SRAC 2006 code, with the nuclear data library is JENDL-4.0. The results reveal that the reactor can attain the criticality condition with the plutonium concentration in the fuel salt is equal to 9.16% or more. The conversion ratio diminishes with the enlarging of plutonium concentration in the fuel. The neutron spectrum of miniFUJI MSR with plutonium fuel becomes harder compared to that of the 233U fuel.

  8. Application of density functional theory in assessing properties of thoria and recycled fuels

    NASA Astrophysics Data System (ADS)

    Szpunar, B.; Szpunar, J. A.

    2013-08-01

    The application of the Density Functional Theory (DFT) approximation to assess the mechanical and structural properties of recycled urania and thoria fuel is presented. The total energy technique based on the local density approximation plus Hubbard U as implemented in the CASTEP code is used. The calculated values of the lattice constants and mechanical moduli of ThO2 and UO2 agree with the experimental data. However only non-local hybrid functional (B3LYP) leads to a larger band gap (6.9 eV) of thoria, in better agreement with experiment (6 eV) than value (4.7 eV) calculated using the LDA + U (6 eV) scheme. The calculations are further expanded to study lattice constants of (Pu, U) oxides and U3O8 for which we currently do not have experimental data. The elastic moduli of ThO2, UO2 and (Pu, U) oxides are compared.

  9. The prospect of uranium nitride (UN-PuN) fuel for 25- 100MWe gas cooled fast reactor long life without refuelling

    NASA Astrophysics Data System (ADS)

    Syarifah, R. D.; Su'ud, Z.; Basar, K.; Irwanto, D.

    2016-11-01

    The prospect of uranium nitride (UN-PuN) fuel for 25-100MWe Gas Cooled Fast Reactor has been done. This research use helium coolant which has low neutron moderation, chemical inert and single phase. This study use natural uranium and plutonium. Plutonium taken from spent fuel of LWR (Light Water Reactor). So, it can reduced spent fuel in the world. The calculation use SRAC2006 and JENDL 4.0 for the data libraries. First, we calculate PIJ for fuel pin cell calculation and CITATION for core calculation. The reflector radial-axial width is 50 cm. The variation of fuel fraction is 40% until 65%, cladding 10%, and moderator 25% up to 50%. The variation of the power is 75-300 MWth (25-100 MWe). The calculation of survey parameter has been done. The variation of percentage plutonium is 7% up to 13%. We have optimum k-eff value in percentage of plutonium 11%. The high powers cause k-eff value high too. Second, the core configuration divided by three variation fuel (F1, F2, and F3). F1 is located in the central core, F2 middle core and F3 outer core. The variation percentage Plutonium for fuel F1:F2:F3 = 8%:10%:12%. The increasing power level make the burn up level increase. All case can reach burn up time plus than 20 years. The thermal powers increase cause the peak power density increase. The power 150 MWth, 225 MWth, and 300 MWth have excess reactivity (%Ak/k) less than 2%.

  10. Microstructural Changes In Thermally Cycled U-Pu-Zr-Am-Np Metallic Transmutation Fuel With 1.5% Lanthanides

    SciTech Connect

    Dawn E. Janney; J. Rory Kennedy

    2008-06-01

    The United States Department of Energy (DOE) Global Nuclear Energy Partnership (GNEP) is developing metallic actinide-zirconium alloy fuels for the transmutation of minor actinides as part of a closed fuel cycle. The molten salt electrochemical process to be used for fuel recycle has the potential to carry over up to 2% fission product lanthanide content into the fuel fabrication process. Within the scope of the fuel irradiation testing program at Idaho National Laboratory (INL), candidate metal alloy transmutation fuels containing quantities of lanthanide elements have been fabricated, characterized, and delivered to the Advanced Test Reactor for irradiation testing.

  11. Large area quantitative X-ray mapping of (U,Pu)O 2 nuclear fuel pellets using wavelength dispersive electron probe microanalysis

    NASA Astrophysics Data System (ADS)

    Brémier, S.; Haas, D.; Somers, J.; Walker, C. T.

    2003-04-01

    The work presented is an example of how large area compositional mapping (≥1 mm 2) can be used to provide quantitative information on element distribution and specimen homogeneity. High-resolution was accomplished by producing a collage of X-ray maps acquired using classical conditions; magnification ×400, spatial resolution 256×256 pixels. The individual images, each measuring roughly 250×250 μm, were converted to quantitative maps using the HIMAX® software package and the XMAS® matrix correction from SAMx. The quantitative gray-level large area X-ray picture was pieced together using the 'Multiple Image Alignment' function of the ANALYSIS® image processing software. This software was also used to convert the gray-level pictures to false color images. The specimens investigated were transverse sections of MOX fuel pellets. Results are presented for the distribution of Pu by area fraction and cumulative area fraction, the size distribution of regions of high Pu concentration and average separation of these regions.

  12. Thermodynamic assessment of the LiF-CeF3-ThF4 system: Prediction of PuF3 concentration in a molten salt reactor fuel

    NASA Astrophysics Data System (ADS)

    Beneš, O.; Konings, R. J. M.

    2013-04-01

    A thermodynamic description of the LiF-CeF3-ThF4 system is made in this study using a two-sublattice model for the description of the solid solution and a quasi-chemical model based on quadruplet approximation for the liquid phase. New calorimetric experimental data of the binary LiF-CeF3, CeF3-ThF4 and ternary LiF-CeF3-ThF4 systems have been obtained in this work justifying the calculated phase diagrams. Using the obtained thermodynamic assessment the concentration of PuF3 in the LiF-ThF4 melt was estimated based on the similarities with CeF3 and the melting behaviour of the initial molten salt fast reactor fuel was discussed.

  13. A Deterministic Study of the Deficiency of the Wigner-Seitz Approximation for Pu/MOX Fuel Pins

    SciTech Connect

    DeHart, M.D.

    1999-09-27

    The Wigner-Seitz pin-cell approximation has long been applied as a modeling approximation in analysis of UO2 lattice fuel cells. In the past, this approximation has been appropriate for such fuel. However, with increasing attention drawn to mixed-oxide (MOX) fuels with significant plutonium content, it is important to understand the implications of the approximation in a uranium-plutonium matrix. The special geometric capabilities of the deterministic NEWT computer code have been used to assess the adequacy of the Wigner-Seitz cell in such an environment, as part of a larger study of computational aspects of MOX fuel modeling. Results of calculations using various approximations and boundary conditions are presented, and are validated by comparison to results obtained using KENO V.a and XSDRNPM.

  14. Pyrochemical processes for the recovery of weapons grade plutonium either as a metal or as PuO{sub 2} for use in mixed oxide reactor fuel pellets

    SciTech Connect

    Colmenares, C.A.; Ebbinghaus, B.B.; Bronson, M.C.

    1995-11-03

    The authors have developed two processes for the recovery of weapons grade Pu, as either Pu metal or PuO{sub 2}, that are strictly pyrochemical and do not produce any liquid waste. Large amounts of Pu metal (up to 4 kg.), in various geometric shapes, have been recovered by a hydride/dehydride/casting process (HYDEC) to produce metal ingots of any desired shape. The three processing steps are carried out in a single compact apparatus. The experimental technique and results obtained will be described. The authors have prepared PuO{sub 2} powders from weapons grade Pu by a process that hydrides the Pu metal followed by the oxidation of the hydride (HYDOX process). Experimental details of the best way to carry out this process will be presented, as well as the characterization of both hydride and oxide powders produced.

  15. Numerical Tests for the Problem of U-Pu Fuel Burnup in Fuel Rod and Polycell Models Using the MCNP Code

    NASA Astrophysics Data System (ADS)

    Muratov, V. G.; Lopatkin, A. V.

    An important aspect in the verification of the engineering techniques used in the safety analysis of MOX-fuelled reactors, is the preparation of test calculations to determine nuclide composition variations under irradiation and analysis of burnup problem errors resulting from various factors, such as, for instance, the effect of nuclear data uncertainties on nuclide concentration calculations. So far, no universally recognized tests have been devised. A calculation technique has been developed for solving the problem using the up-to-date calculation tools and the latest versions of nuclear libraries. Initially, in 1997, a code was drawn up in an effort under ISTC Project No. 116 to calculate the burnup in one VVER-1000 fuel rod, using the MCNP Code. Later on, the authors developed a computation technique which allows calculating fuel burnup in models of a fuel rod, or a fuel assembly, or the whole reactor. It became possible to apply it to fuel burnup in all types of nuclear reactors and subcritical blankets.

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

    SciTech Connect

    Henzl, Vladimir; Croft, Stephen; Swinhoe, Martyn T.; Tobin, Stephen J.

    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.

  17. Photoelectron Spectroscopy of U Oxide at LLNL

    SciTech Connect

    Tobin, J G; Yu, S; Chung, B W; Waddill, G D

    2010-03-02

    In our laboratory at LLNL, an effort is underway to investigate the underlying complexity of 5f electronic structure with spin-resolved photoelectron spectroscopy using chiral photonic excitation, i.e. Fano Spectroscopy. Our previous Fano measurements with Ce indicate the efficacy of this approach and theoretical calculations and spectral simulations suggest that Fano Spectroscopy may resolve the controversy concerning Pu electronic structure and electron correlation. To this end, we have constructed and commissioned a new Fano Spectrometer, testing it with the relativistic 5d system Pt. Here, our preliminary photoelectron spectra of the UO{sub 2} system are presented. X-ray photoelectron spectroscopy has been used to characterize a sample of UO{sub 2} grown on an underlying substrate of Uranium. Both AlK{alpha} (1487 eV) and MgK{alpha} (1254 eV) emission were utilized as the excitation. Using XPS and comparing to reference spectra, it has been shown that our sample is clearly UO{sub 2}.

  18. Inventories of 239+240Pu, 137Cs, and excess 210Pb in sediments from freshwater and brackish lakes in Rokkasho, Japan, adjacent to a spent nuclear fuel reprocessing plant.

    PubMed

    Ueda, Shinji; Ohtsuka, Yoshihito; Kondo, Kunio; Hisamatsu, Shun'ichi

    2009-10-01

    We investigated the vertical profiles of (239+240)Pu, (137)Cs, and excess (210)Pb ((210)Pb(ex)) in sediment core samples obtained from two freshwater lakes and two brackish lakes situated near the first commercial spent nuclear fuel reprocessing plant in Rokkasho, Japan, before the final test of the plant using actual spent nuclear fuel. The inventory of (239+240)Pu in those lakes was larger than that in soil in Rokkasho, which indicated the inflow of (239+240)Pu from the catchment area in addition to direct deposition on the lake surfaces. The (137)Cs inventory in sediments of the brackish lakes was lower than that in the soil, which showed that part of the (137)Cs was removed from the sediments by the brackish water or that it was not deposited into the sediments, because of the high solubility of Cs in brackish water. The (137)Cs inventory in sediments of the freshwater lakes was higher than that of the brackish lakes, and comparable with that in soil except for one core sample out of four. The (239+240)Pu/(137)Cs ratio in freshwater lake sediments was higher than that in soil, and that indicated that part of the (137)Cs was lost from the sediments. The low inventory of (137)Cs may be attributable to competition for absorption sites in sediments with ammonium ions formed in the reducing environment which occurs from summer to fall in the sediments. Those data will be used as background data on the artificial radionuclides in the lakes to assess the effect of released radionuclides on their concentrations.

  19. Determination of 240Pu/239Pu atom ratio in coastal surface seawaters from the western North Pacific Ocean and Japan Sea.

    PubMed

    Yamada, Masatoshi; Zheng, Jian

    2008-01-01

    Surface seawater samples were collected from a site in the vicinity of the nuclear fuel reprocessing facility at Rokkasho, Japan and sites along the Japan Sea coast. (239+240)Pu activities and (240)Pu/(239)Pu atom ratios were determined by alpha-spectrometry and isotope-dilution sector-field ICP-MS. The (240)Pu/(239)Pu atom ratio with the mean value of 0.227 +/- 0.006 was significantly higher than the mean global fallout ratio of 0.18. The contribution of the Pacific Proving Grounds close-in fallout was estimated to be 33% of the (239+240)Pu.

  20. Purification of 238Pu Oxide using the Pu Oxalate Process

    SciTech Connect

    Mew, D A; Krikorian, O H; Dodson, K E; Schmitz, J A

    2001-11-28

    The Pu oxalate process is used to remove {sup 234}U from aged {sup 238}Pu-enriched PuO{sub 2} ({sup 234}U grows into the PuO{sub 2} material with time from a-decay of {sup 238}Pu). The Pu oxalate process was first used on a mixture of weapons grade PuO{sub 2} with UO{sub 2} to work out the processing parameters. It was then applied to aged {sup 238}Pu-enriched PuO{sub 2} ({sup 238}PuO{sub 2}). The {sup 234}U content of the {sup 238}PuO{sub 2} was reduced from 13.2 wt% to 0.0254 wt%, and the Pu recovery yield was 78.5%. The process is complex and is complicated by radiolysis problems when working with {sup 238}Pu. Details of the experiments are described.

  1. Sintering and characterization of (Pu,Zr)N

    NASA Astrophysics Data System (ADS)

    Pukari, Merja; Takano, Masahide; Nishi, Tsuyoshi

    2014-01-01

    Nitride fuel, with the composition of (Pu0.4Zr0.6)N, is fabricated for studying the sinterability of nitride fuel as a function of oxygen concentration in the material. Oxygen concentration of up to 0.6 wt% evidently enhances the densification of the material. Increasing the sintering temperature from 1923 to 1973 K improves the sintered pellet densities by up to 3.8%TD. In addition, the measured thermophysical and electrical properties of (Pu0.4Zr0.6)N reveal that the values are close to those of PuN. Elevated oxygen concentration in the material decreases its thermal conductivity. Oxygen concentration of 0.34 wt% in (Pu,Zr)N is a consequence of the fabrication process, considering the relatively pure ZrN (0.03 wt% O) and PuN (0.08 wt% O) powders initially fabricated.

  2. Adsorption behaviour of PuF6 on UO2F2 by the use of 236Pu

    NASA Astrophysics Data System (ADS)

    Sato, Nobuaki; Matsuda, Minoru; Mitsugashira, Toshiaki; Kirishima, Akira

    2010-03-01

    To know the behavior of plutonium in the fluoride volatility process (FLUOREX PROCESS) for the spent nuclear fuel, both UO2 and PuO2 are fluorinated by fluorine forming volatile UF6 and PuF6, respectively. Then PuF6 is separated and recovered from UF6 by using adsorption materials such as uranyl fluoride UO2F2. In this paper, adsorption behavior of PuF6on UO2F2 was examined by the use of 236Pu tracer. First, the stability of UO2F2 in F2atmosphere was analyzed by TG-DTA method showing that uranium volatilized completely over 350 °C by the formation of UF6 and the adsorption of plutonium by UO2F2 should be done at temperatures lower than 250 °C. The behavior of PtF6 as a chemical analogue of PuF6 was also conducted for comparison and it showed that the deposition of PtF4 on UO2F2 at 200 °C. When the 236Pu doped U3O8 was reacted with 10%F2-He gas, the PuF6 vaporized at ca. 600 °C. Then adsorption of 236Pu on UO2F2 was observed by α ray measurement. The adsorption mechanism of Pu on UO2F2 was discussed with experimental data and thermodynamic consideration.

  3. Anaerobic Biotransformation and Mobility of Pu and Pu-EDTA

    SciTech Connect

    Bolton, H., Jr.; Bailey, V.L.; Plymale, A.E.; Rai, D.; Xun, L.

    2006-04-05

    The complexation of radionuclides (e.g., plutonium (Pu) and {sup 60}Co) by co-disposed ethylenediaminetetraacetate (EDTA) has enhanced their transport in sediments at DOE sites. Pu(IV)-EDTA is not stable in the presence of relatively soluble Fe(III) compounds. Since most DOE sites have Fe(III) containing sediments, Pu(IV) is likely not the mobile form of Pu-EDTA. The only other Pu-EDTA complex stable in groundwater relevant to DOE sites would be Pu(III)-EDTA, which only forms under anaerobic conditions. Research is therefore needed to investigate the biotransformation of Pu and Pu-EDTA under anaerobic conditions and the anaerobic biodegradation of Pu-EDTA. The biotransformation of Pu and Pu-EDTA under various anaerobic regimes is poorly understood including the reduction kinetics of Pu(IV) to Pu(III) from soluble (Pu(IV)-EDTA) and insoluble Pu(IV), the redox conditions required for this reduction, the strength of the Pu(III)-EDTA, how the Pu(III)-EDTA competes with other dominant anoxic soluble metals (e.g., Fe(II)), and the oxidation kinetics of Pu(III)-EDTA. Finally, soluble Pu(III)-EDTA under anaerobic conditions would require anaerobic degradation of the EDTA to limit Pu(III) transport. Anaerobic EDTA degrading microorganisms have never been isolated. Recent results have shown that Shewanella oneidensis MR-1, a dissimilatory metal reducing bacterium, can reduce Pu(IV) to Pu(III). The Pu(IV) was provided as insoluble PuO2. The highest rate of Pu(IV) reduction was with the addition of AQDS, an electron shuttle. Of the total amount of Pu solubilized (i.e., soluble through a 0.36 nm filter), approximately 70% was Pu(III). The amount of soluble Pu was between 4.8 and 3.2 micromolar at day 1 and 6, respectively, indicating rapid reduction. The micromolar Pu is significant since the drinking water limit for Pu is 10{sup -12} M. On-going experiments are investigating the influence of EDTA on the rate of Pu reduction and the stability of the formed Pu(III). We have also

  4. Plutonium isotopic analysis system for plutonium samples enriched in sup 238 Pu in EP 60/61 and fuel-clad containers

    SciTech Connect

    Ruhter, W.D.

    1991-07-01

    This user's manual is addressed to the Hanford Site personnel (routine operators and supervisors) who perform measurements with the Pu-238 isotopic analysis system. Each chapter begins with a table of contents that lists the section titles, illustrations, and tabular data presented in that chapter. The first chapter in this manual is an introduction to the system. Chapter 2 lists required settings for the system's commercial nuclear instrument modules. System operating procedures are given in Chapter 3. Chapter 4 contains routine and supervisorial operator interactions. Chapter 5 describes the system's short- and long-printout output formats. Chapter 6 gives instructions for changing system parameters. Error messages are listed and described in Chapter 7. Chapter 8 contains reference articles on measuring relative plutonium isotopics in solid samples.

  5. AC-3-irradiation test of sphere-pac and pellet (U,Pu)C fuel in the US Fast Flux Test Facility

    NASA Astrophysics Data System (ADS)

    Bart, G.; Botta, F. B.; Hoth, C. W.; Ledergerber, G.; Mason, R. E.; Stratton, R. W.

    2008-05-01

    The objective of the AC-3 bundle experiment in the Fast Flux Test Facility (FFTF) was to evaluate a fuel fabrication method by 'direct conversion' of nitrate solutions into spherical uranium-plutonium carbide particles and to compare the irradiation performance of 'sphere-pac' fuel pins prepared at Paul Scherrer Institute (PSI) with standard pellet fuel pins fabricated at Los Alamos National Laboratory (LANL). The irradiation and post test examination results show that mixed carbide pellet fuel produced by powder methods and sphere-pac particle fuel developed by internal gelation techniques are both valuable advanced fuel candidates for liquid metal reactors. The PSI fabrication process with direct conversion of actinide nitrate solutions into various sizes of fuel spheres by internal gelation and direct filling of spheres into cladding tubes is seen as more easily transferable to remote operation, showing a significant reduction of process steps. The process is also adaptable for the fabrication of carbonitrides and nitrides (still based on a uranium matrix), as well as for actinides diluted in a (uranium-free) yttrium stabilized zirconium oxide matrix. The AC-3 fuel bundle was irradiated in the Fast Flux Test Facility (FFTF) during the years 1986-1988 for 630 full power days to a peak burn up of ˜8 at.% fissile material. All of the pins, irradiated at linear powers of up to 84 kW/m, with cladding outer temperatures of 465 °C appeared to be in good condition when removed from the assembly. The rebirth of interest for fast reactor systems motivated the earlier teams to report about the excellent, still perfectly relevant results reached; this paper focusing on the sphere-pac fuel behaviour.

  6. Anaerobic Biotransformation and Mobility of Pu and Pu-EDTA

    SciTech Connect

    Bolton, H., Jr.; Rai, D.; Xun, L.

    2005-04-18

    The complexation of radionuclides (e.g., plutonium (Pu) and {sup 60}Co) by codisposed ethylenediaminetetraacetate (EDTA) has enhanced their transport in sediments at DOE sites. Our previous NABIR research investigated the aerobic biodegradation and biogeochemistry of Pu(IV)-EDTA. Plutonium(IV) forms stable complexes with EDTA under aerobic conditions and an aerobic EDTA degrading bacterium can degrade EDTA in the presence of Pu and decrease Pu mobility. However, our recent studies indicate that while Pu(IV)-EDTA is stable in simple aqueous systems, it is not stable in the presence of relatively soluble Fe(III) compounds (i.e., Fe(OH){sub 3}(s)--2-line ferrihydrite). Since most DOE sites have Fe(III) containing sediments, Pu(IV) in likely not the mobile form of Pu-EDTA in groundwater. The only other Pu-EDTA complex stable in groundwater relevant to DOE sites would be Pu(III)-EDTA, which only forms under anaerobic conditions. Research is therefore needed in this brand new project to investigate the biotransformation of Pu and Pu-EDTA under anaerobic conditions. The biotransformation of Pu and Pu-EDTA under various anaerobic regimes is poorly understood including the reduction kinetics of Pu(IV) to Pu(III) from soluble (Pu(IV)-EDTA) and insoluble Pu(IV) as PuO2(am) by metal reducing bacteria, the redox conditions required for this reduction, the strength of the Pu(III)-EDTA complex, how the Pu(III)-EDTA complex competes with other dominant anoxic soluble metals (e.g., Fe(II)), and the oxidation kinetics of Pu(III)-EDTA. Finally, the formation of a stable soluble Pu(III)-EDTA complex under anaerobic conditions would require degradation of the EDTA complex to limit Pu(III) transport in geologic environments. Anaerobic EDTA degrading microorganisms have not been isolated. These knowledge gaps preclude the development of a mechanistic understanding of how anaerobic conditions will influence Pu and Pu-EDTA fate and transport to assess, model, and design approaches to stop

  7. Biotransformation of PuEDTA: Implications to Pu Immobilization

    SciTech Connect

    Bolton, Harvey, Jr.

    2006-06-01

    This project integrates three distinct goals to develop a fundamental understanding of the potential fate and disposition of plutonium in sediments that are co-contaminated with EDTA. The three objectives are: (1) Develop thermodynamic data for Pu-EDTA species and determine the dominant mobile form of Pu under anaerobic conditions. (2) Elucidate the mechanism and rates of Pu(IV) and Pu(IV)-EDTA reduction by metal-reducing bacteria and determine where the Pu is located (in solution, biosorbed, bioaccumulated). (3) Enrich and isolate anaerobic EDTA-degrading microorganisms to investigate the anaerobic biodegradation of Pu-EDTA.

  8. Control of Urania Crystallite Size by HMTA-Urea Reactions in the Internal Gelation Process for Preparing (U, Pu)O2Fuel Kernels

    SciTech Connect

    Collins, J.L.

    2005-04-26

    In the development of (U,Pu)O{sub 2} kernels by the internal gelation process for the Direct Press Spheroidized process at Oak Ridge National Laboratory, a novel crystal growth step was discovered that made it possible to prepare calcined porous kernels that could be used as direct-press feed for Fast Breeder Reactor pellet fabrication. High-quality pellets were prepared that were near theoretical density and that (upon examination) revealed no evidence of sphere remnants. The controlled crystal growth step involved using hexamethylenetetramine (HMTA)-urea stock solutions that were boiled for 60 min or less. Before this discovery, all the other crystal growth steps (when utilized) could reduce the tap density to only {approx}1.3 g/cm{sup 3}, which was not sufficiently low for use in ideal pellet pressing. The use of the boiled HMTA-urea solution allowed the tap density to be lowered to 0.93 g/cm{sup 3}, with the ideal density being about 1.0 g/cm{sup 3}. This report describes the development of this technology and its scaleup.

  9. A Brief Review of Past INL Work Assessing Radionuclide Content in TMI-2 Melted Fuel Debris: The Use of 144Ce as a Surrogate for Pu Accountancy

    SciTech Connect

    D. L. Chichester; S. J. Thompson

    2013-09-01

    This report serves as a literature review of prior work performed at Idaho National Laboratory, and its predecessor organizations Idaho National Engineering Laboratory (INEL) and Idaho National Engineering and Environmental Laboratory (INEEL), studying radionuclide partitioning within the melted fuel debris of the reactor of the Three Mile Island 2 (TMI-2) nuclear power plant. The purpose of this review is to document prior published work that provides supporting evidence of the utility of using 144Ce as a surrogate for plutonium within melted fuel debris. When the TMI-2 accident occurred no quantitative nondestructive analysis (NDA) techniques existed that could assay plutonium in the unconventional wastes from the reactor. However, unpublished work performed at INL by D. W. Akers in the late 1980s through the 1990s demonstrated that passive gamma-ray spectrometry of 144Ce could potentially be used to develop a semi-quantitative correlation for estimating plutonium content in these materials. The fate and transport of radioisotopes in fuel from different regions of the core, including uranium, fission products, and actinides, appear to be well characterized based on the maximum temperature reached by fuel in different parts of the core and the melting point, boiling point, and volatility of those radioisotopes. Also, the chemical interactions between fuel, fuel cladding, control elements, and core structural components appears to have played a large role in determining when and how fuel relocation occurred in the core; perhaps the most important of these reaction appears to be related to the formation of mixed-material alloys, eutectics, in the fuel cladding. Because of its high melting point, low volatility, and similar chemical behavior to plutonium, the element cerium appears to have behaved similarly to plutonium during the evolution of the TMI-2 accident. Anecdotal evidence extrapolated from open-source literature strengthens this logical feasibility for

  10. Pu-239 and Pu-240 inventories and Pu-240/ Pu-239 atom ratios in the water column off Sanriku, Japan.

    NASA Astrophysics Data System (ADS)

    Yamada, Masatoshi; Zheng, Jian; Aono, Tatsuo

    2013-04-01

    A magnitude 9.0 earthquake and subsequent tsunami occurred in the Pacific Ocean off northern Honshu, Japan, on 11 March 2011 which caused severe damage to the Fukushima Dai-ichi Nuclear Power Plant. This accident has resulted in a substantial release of radioactive materials to the atmosphere and ocean, and has caused extensive contamination of the environment. However, no information is available on the amounts of radionuclides such as Pu isotopes released into the ocean at this time. Investigating the background baseline concentration and atom ratio of Pu isotopes in seawater is important for assessment of the possible contamination in the marine environment. Pu-239 (half-life: 24,100 years), Pu-240 (half-life: 6,560 years) and Pu-241 (half-life: 14.325 years) mainly have been released into the environment as the result of atmospheric nuclear weapons testing. The atom ratio of Pu-240/Pu-239 is a powerful fingerprint to identify the sources of Pu in the ocean. The Pu-239 and Pu-240 inventories and Pu-240/Pu-239 atom ratios in seawater samples collected in the western North Pacific off Sanriku before the accident at Fukushima Dai-ichi Nuclear Power Plant will provide useful background baseline data for understanding the process controlling Pu transport and for distinguishing additional Pu sources. Seawater samples were collected with acoustically triggered quadruple PVC sampling bottles during the KH-98-3 cruise of the R/V Hakuho-Maru. The Pu-240/Pu-239 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. The Pu-239 and Pu-240 concentrations were 2.07 and 1.67 mBq/m3 in the surface water, respectively, and increased with depth; a subsurface maximum was identified at 750 m depth, and the concentrations decreased with depth, then increased at the bottom layer. The total Pu-239+240 inventory in the entire water column (depth interval 0

  11. 238Pu: accumulation, tissue distribution, and excretion in Mayak workers after exposure to plutonium aerosols.

    PubMed

    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.

  12. Report of an investigation into deterioration of the Plutonium Fuel Form Fabrication Facility (PuFF) at the DOE Savannah River Site

    SciTech Connect

    Not Available

    1991-10-01

    This investigations of the Savannah River Site's Plutonium Fuel Form fabrication facility located in Building 235-F was initiated in April 1991. The purpose of the investigation was to determine whether, as has been alleged, operation of the facility's argon inert gas system was terminated with the knowledge that continued inoperability of the argon system would cause accelerated corrosion damage to the equipment in the plutonium 238 processing cells. The investigation quickly established that the decision to discontinue operation of the argon system, by not repairing it, was merely one of the measures, and not the most important one, which led to the current deteriorated state of the facility. As a result, the scope of the investigation was broadened to more identify and assess those factors which contributed to the facility's current condition. This document discusses the backgrounds, results, and recommendations of this investigation.

  13. Pu(V) transport through Savannah River Site soils - an evaluation of a conceptual model of surface- mediated reduction to Pu (IV).

    PubMed

    Powell, Brian A; Kaplan, Daniel I; Serkiz, Steven M; Coates, John T; Fjeld, Robert A

    2014-05-01

    Over the last fifteen years the Savannah River Site (SRS) in South Carolina, USA, was selected as the site of three new plutonium facilities: the Mixed Oxide Fuel Fabrication Facility, Pit Disassembly and Conversion Facility, and the Pu Immobilization Plant. In order to assess the potential human and environmental risk associated with these recent initiatives, improved understanding of the fate and transport of Pu in the SRS subsurface environment is necessary. The hypothesis of this study was that the more mobile forms of Pu, Pu(V) and Pu(VI), would be reduced to the less mobile Pu(III/IV) oxidation states under ambient SRS subsurface conditions. Laboratory-scale dynamic flow experiments (i.e., column studies) indicated that Pu(V) was very mobile in SRS sediments. At higher pH values the mobility of Pu decreased and the fraction of Pu that became irreversibly sorbed to the sediment increased, albeit, only slightly. Conversely, these column experiments showed that Pu(IV) was essentially immobile and was largely irreversibly sorbed to the sediment. More than 100 batch sorption experiments were also conducted with four end-member sediments, i.e., sediments that include the chemical, textural, and mineralogical properties likely to exist in the SRS. These tests were conducted as a function of initial Pu oxidation state, pH, and contact time and consistently demonstrated that although Pu(V) sorbed initially quite weakly to sediments, it slowly, over the course of <33 days, sorbed very strongly to sediments, to approximately the same degree as Pu(IV). This is consistent with our hypothesis that Pu(V) is reduced to the more strongly sorbing form of Pu, Pu(IV). These studies provide important experimental support for a conceptual geochemical model for dissolved Pu in a highly weathered subsurface environment. That is that, irrespective of the initial oxidation state of the dissolved Pu introduced into a SRS sediment system, Pu(IV) controls the environmental transport

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

    PubMed

    Lindahl, Patric; Worsfold, Paul; Keith-Roach, Miranda; Andersen, Morten B; Kershaw, Peter; Leonard, Kins; Choi, Min-Seok; Boust, Dominique; Lesueur, Patrick

    2011-11-01

    A depth profile of (239)Pu and (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 ~10 k Bq kg(-1) was observed for (239+240)Pu, corresponding to the peak in Pu discharge from Sellafield in 1973, with a decreasing trend with depth down to ~0.04 k Bq kg(-1) in the deeper layers. The depth profile of (239+240)Pu specific activities together with results from gamma-ray spectrometry for (137)Cs and (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 (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 (240)Pu/(239)Pu atom ratios ranged from ~0.03 in the deepest layers to >0.20 in the sub-surface layers with an activity-weighted average of 0.181. The decreasing (240)Pu/(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 (240)Pu/(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.

  15. Biodegradation of PuEDTA and Impacts on Pu Mobility

    SciTech Connect

    Bolton, H., Jr.; Rai, D.; Xun, L.

    2004-03-17

    The contamination of many DOE sites by Pu presents a long-term problem because of its long half-life (240,000 yrs) and the low drinking water standard (<10{sup -12} M). EDTA was co-disposed with radionuclides (e.g., Pu, {sup 60}Co), formed strong complexes, and enhanced radionuclide transport at several DOE sites. Biodegradation of EDTA should decrease Pu mobility. One objective of this project was to determine the biodegradation of EDTA in the presence of PuEDTA complexes. The aqueous system investigated at pH 7 (10{sup -4} M EDTA and 10{sup -6} M Pu) contained predominantly Pu(OH){sub 2}EDTA{sup 2-}. The EDTA was degraded at a faster rate in the presence of Pu. As the total concentration of both EDTA and PuEDTA decreased (i.e., 10{sup -5} M EDTA and 10{sup -7} M PuEDTA), the presence of Pu decreased the biodegradation rate of the EDTA. It is currently unclear why the concentration of Pu directly affects the increase/decrease in rate of EDTA biodegradation. The soluble Pu concentration decreased, in agreement with thermodynamic predictions, as the EDTA was biodegraded, indicating that biodegradation of EDTA will decrease Pu mobility when the Pu is initially present as Pu(IV)EDTA. A second objective was to investigate how the presence of competing metals, commonly encountered in geologic media, will influence the speciation and biodegradation of Pu(IV)-EDTA. Studies on the solubilities of Fe(OH){sub 3}(s) and of Fe(OH){sub 3}(s) plus PuO{sub 2}(am) in the presence of EDTA and as a function of pH showed that Fe(III) out competes the Pu(IV) for the EDTA complex, thereby showing that Pu(IV) will not form stable complexes with EDTA for enhanced transport of Pu in Fe(III) dominated subsurface systems. A third objective is to investigate the genes and enzymes involved in EDTA biodegradation. BNC1 can use EDTA and another synthetic chelating agent nitrilotriacetate (NTA) as sole carbon and nitrogen sources. The same catabolic enzymes are responsible for both EDTA and NTA

  16. Pu Workshop Letter

    SciTech Connect

    Tobin, J G; Schwartz, A J; Fluss, M

    2006-03-06

    In preparation for the upcoming Pu Workshop in Livermore, CA, USA, during July 14 and 15, 2006, we have begun to give some thought as to how the meeting will be structured and what will be discussed. Below, you will find our first proposal as to the agenda and contents of the meeting. From you, we need your feedback and suggestions concerning the desirability of each aspect of our proposal. Hopefully, we will be able to converge to a format that is acceptable to all parties. First, it now appears that we will be limited to three main sessions, Friday morning (July 14), Friday afternoon (July 14) and Saturday morning (July 15). The Pu Futures Meeting will conclude on Thursday, July 13. Following a social excursion, the Russian participants will be transported from Monterey Bay to their hotel in Livermore. We anticipate that the hotel will be the Residence Inn at 1000 Airway Blvd in Livermore. However, the hotel arrangements still need to be confirmed. We expect that many of our participants will begin their travels homeward in the afternoon of Saturday, July 15 and the morning of Sunday, July 16. Associated with the three main sessions, we propose that there be three main topics. Each session will have an individual focus. Because of the limited time available, we will need to make some judicious choices concerning the focus and the speakers for each session. We will also have a poster session associated with each session, to facilitate discussions, and a rotating set of Lab Tours, to maximize participation in the tour and minimize the disruption of the speaking schedule. Presently, we are planning a tour of the Dynamical Transmission Electron Microscope (DTEM) facilities, but this is still in a preliminary stage. We estimate that for each session and topic, there will be time for five (5) speakers. We propose that, typically, there be three (3) Russian and two (2) American speakers per session. We also propose that each session have a chair (or two chairs), who

  17. Characterization of insoluble residues from the dissolution of irradiated (U,Pu)O{sub 2}

    SciTech Connect

    Goode, J.H.; Arwood, P.C.

    1983-05-01

    Hot-cell tests were conducted using (U,Pu)O{sub 2} fuels that had been irradiated to about 5.2 TJ/kg (U + Pu) [60 MWd/kg (U + Pu)] in an effort to characterize the insoluble residues that remained after the fuel pellets had been dissolved in HNO{sub 3} and in HNO{sub 3}-KF. The composition, particle size range, and density of the material were determined by newer analytical techniques, including spark-source mass spectrometry, neutron activation, scanning electron microscopy, and x-ray fluorescence, combined with older methods such as sedimentation and powder density by water displacement.

  18. Fabrication of a 238Pu target

    SciTech Connect

    Wu, C Y; Chyzh, A; Kwan, E; Henderson, R; Gostic, J; Carter, D

    2010-11-16

    Precision neutron-induced reaction data are important for modeling the network of isotope production and destruction within a given diagnostic chain. This network modeling has many applications such as the design of advanced fuel cycle for reactors and the interpretation of radiochemical data related to the stockpile stewardship and nuclear forensics projects. Our current funded effort is to improve the neutron-induced reaction data on the short-lived actinides and the specific goal is to improve the neutron capture data on {sup 238}Pu with a half-life of 87.7 years. In this report, the fabrication of a {sup 238}Pu target for the proposed measurement using the DANCE array at LANL is described. The {sup 238}Pu target was fabricated from a sample enriched to 99.35%, acquired from ORNL. A total of 395 {micro}g was electroplated onto both sides of a 3 {micro}m thick Ti foil using a custom-made plating cell, shown in Fig 1. The target-material loaded Ti foil is sandwiched between two double-side aluminized mylar foils with a thickness of 1.4 {micro}m. The mylar foil is glued to a polyimide ring. This arrangement is shown partially in Fig. 2. The assembled target is then inserted into an aluminum container with a wall thickness of 0.76 mm, shown in Fig. 3. A derlin ring is used to keep the target assembly in place. The ends of this cylindrical container are vacuum-sealed by two covers with thin Kapton foils as windows for the beam entrance and exit. Shown in Fig. 4 is details of the arrangement. This target is used for phase I of the proposed measurement on {sup 238}Pu scheduled for Nov 2010 together with the DANCE array to address the safety issues raised by LANL. Shown in Fig. 5 is the preliminary results on the yield spectrum as a function of neutron incident energy with a gate on the total {gamma}-ray energy of equivalent Q value. Since no fission PPAC is employed, the distinction between the capture and fission events cannot be made, which is important for the

  19. Pu Anion Exchange Process Intensification

    SciTech Connect

    Taylor-Pashow, K.

    2015-10-08

    This project seeks to improve the efficiency of the plutonium anion-exchange process for purifying Pu through the development of alternate ion-exchange media. The objective of the project in FY15 was to develop and test a porous foam monolith material that could serve as a replacement for the current anion-exchange resin, Reillex® HPQ, used at the Savannah River Site (SRS) for purifying Pu. The new material provides advantages in efficiency over the current resin by the elimination of diffusive mass transport through large granular resin beads. By replacing the large resin beads with a porous foam there is much more efficient contact between the Pu solution and the anion-exchange sites present on the material. Several samples of a polystyrene based foam grafted with poly(4-vinylpyridine) were prepared and the Pu sorption was tested in batch contact tests.

  20. Overview of advanced technologies for stabilization of {sup 238}Pu-contaminated waste

    SciTech Connect

    Ramsey, K.B.; Foltyn, E.M.; Heslop, J.M.

    1998-02-01

    This paper presents an overview of potential technologies for stabilization of {sup 238}Pu-contaminated waste. Los Alamos National Laboratory (LANL) has processed {sup 238}PuO{sub 2} fuel into heat sources for space and terrestrial uses for the past several decades. The 88-year half-life of {sup 238}Pu and thermal power of approximately 0.6 watts/gram make this isotope ideal for missions requiring many years of dependable service in inaccessible locations. However, the same characteristic which makes {sup 238}Pu attractive for heat source applications, the high Curie content (17 Ci/gram versus 0.06 Ci/gram for 239{sup Pu}), makes disposal of {sup 238}Pu-contaminated waste difficult. Specifically, the thermal load limit on drums destined for transport to the Waste Isolation Pilot Plant (WIPP), 0.23 gram per drum for combustible waste, is impossible to meet for nearly all {sup 238}Pu-contaminated glovebox waste. Use of advanced waste treatment technologies including Molten Salt Oxidation (MSO) and aqueous chemical separation will eliminate the combustible matrix from {sup 238}Pu-contaminated waste and recover kilogram quantities of {sup 238}PuO{sub 2} from the waste stream. A conceptual design of these advanced waste treatment technologies will be presented.

  1. Program Pu Futures 2006

    SciTech Connect

    Fluss, M

    2006-06-12

    The coordination chemistry of plutonium remains relatively unexplored. Thus, the fundamental coordination chemistry of plutonium is being studied using simple multi-dentate ligands with the intention that the information gleaned from these studies may be used in the future to develop plutonium-specific sequestering agents. Towards this goal, hard Lewis-base donors are used as model ligands. Maltol, an inexpensive natural product used in the commercial food industry, is an ideal ligand because it is an all-oxygen bidentate donor, has a rigid structure, and is of small enough size to impose little steric strain, allowing the coordination preferences of plutonium to be the deciding geometric factor. Additionally, maltol is the synthetic precursor of 3,4-HOPO, a siderophore-inspired bidentate moiety tested by us previously as a possible sequestering agent for plutonium under acidic conditions. As comparisons to the plutonium structure, Ce(IV) complexes of the same and related ligands were examined as well. Cerium(IV) complexes serve as good models for plutonium(IV) structures because Ce(IV) has the same ionic radius as Pu(IV) (0.94 {angstrom}). Plutonium(IV) maltol crystals were grown out of a methanol/water solution by slow evaporation to afford red crystals that were evaluated at the Advanced Light Source at Lawrence Berkeley National Laboratory using single crystal X-ray diffraction. Cerium(IV) complexes with maltol and bromomaltol were crystallized via slow evaporation of the mother liquor to afford tetragonal, black crystals. All three complexes crystallize in space group I4{sub 1}/a. The Ce(IV) complex is isostructural with the Pu(IV) complex, in which donating oxygens adopt a trigonal dodecahedral geometry around the metal with the maltol rings parallel to the crystallographic S{sub 4} axis and lying in a non-crystallographic mirror plane of D{sub 2d} molecular symmetry (Fig 1). The metal-oxygen bonds in both maltol complexes are equal to within 0.04 {angstrom

  2. In situ high temperature X-Ray diffraction study of the phase equilibria in the UO2-PuO2-Pu2O3 system

    NASA Astrophysics Data System (ADS)

    Belin, Renaud C.; Strach, Michal; Truphémus, Thibaut; Guéneau, Christine; Richaud, Jean-Christophe; Rogez, Jacques

    2015-10-01

    The region of the U-Pu-O phase diagram delimited by the compounds UO2-PuO2-Pu2O3 is known to exhibit a miscibility gap at low temperature. Consequently, MOX fuels with a composition entering this region could decompose into two fluorite phases and thus exhibit chemical heterogeneities. The experimental data on this domain found in the literature are scarce and usually provided using DTA that is not suitable for the investigation of such decomposition phenomena. In the present work, new experimental data, i.e. crystallographic phases, lattice parameters, phase fractions and temperature of phase separation, were measured in the composition range 0.14 < Pu/(U + Pu) < 0.62 and 1.85 < O/(U + Pu) < 2 from 298 to 1750 K using a novel in situ high temperature X-ray diffraction apparatus. A very good agreement is found between the temperature of phase separation determined from our results and using the thermodynamic model of the U-Pu-O system based on the CALPHAD method. Also, the combined use of thermodynamic calculations and XRD results refinement proved helpful in the determination of the O/M ratio of the samples during cooling. The methodology used in the current work might be useful to investigate other oxides systems exhibiting a miscibility gap.

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

    PubMed

    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.

  4. Hematological responses after inhaling {sup 238}PuO{sub 2}: An extrapolation from beagle dogs to humans

    SciTech Connect

    Scott, B.R.; Muggenburg, B.A.; Welsh, C.A.; Angerstein, D.A.

    1994-11-01

    The alpha emitter plutonium-238 ({sup 238}Pu), which is produced in uranium-fueled, light-water reactors, is used as a thermoelectric power source for space applications. Inhalation of a mixed oxide form of Pu is the most likely mode of exposure of workers and the general public. Occupational exposures to {sup 238}PuO{sub 2} have occurred in association with the fabrication of radioisotope thermoelectric generators. Organs and tissue at risk for deterministic and stochastic effects of {sup 238}Pu-alpha irradiation include the lung, liver, skeleton, and lymphatic tissue. Little has been reported about the effects of inhaled {sup 238}PuO{sub 2} on peripheral blood cell counts in humans. The purpose of this study was to investigate hematological responses after a single inhalation exposure of Beagle dogs to alpha-emitting {sup 238}PuO{sub 2} particles and to extrapolate results to humans.

  5. Characterization of Pu-238 Heat Source Granule Containment

    SciTech Connect

    Richardson, Paul Dean II; Sanchez, Joey Leo; Wall, Angelique Dinorah; Chavarria, Rene

    2015-02-11

    The Milliwatt Radioisotopic Themoelectric Generator (RTG) provides power for permissive-action links. Essentially these are nuclear batteries that convert thermal energy to electrical energy using a doped silicon-germanium thermopile. The thermal energy is provided by a heat source made of 238Pu, in the form of 238PuO2 granules. The granules are contained by 3 layers of encapsulation. A thin T-111 liner surrounds the 238PuO2 granules and protects the second layer (strength member) from exposure to the fuel granules. An outer layer of Hastalloy-C protects the T-111 from oxygen embrittlement. The T-111 strength member is considered the critical component in this 238PuO2 containment system. Any compromise in the strength member seen during destructive testing required by the RTG surveillance program is characterized. The T-111 strength member is characterized through Scanning Electron Microscopy (SEM), and Metallography. SEM is used in the Secondary Electron mode to reveal possible grain boundary deformation and/or cracking in the region of the strength member weld. Deformation and cracking uncovered by SEM are further characterized by Metallography. Metallography sections are mounted and polished, observed using optical microscopy, then documented in the form of microphotographs. SEM mat further be used to examine polished Metallography mounts to characterize elements using the SEM mode of Energy Dispersive X-ray spectroscopy (EDS).

  6. Economical Production of Pu-238

    SciTech Connect

    Steven D. Howe; Douglas Crawford; Jorge Navarro; Terry Ring

    2013-02-01

    All space exploration missions traveling beyond Jupiter must use radioisotopic power sources for electrical power. The best isotope to power these sources is plutonium-238. The US supply of Pu-238 is almost exhausted and will be gone within the next decade. The Department of Energy has initiated a production program with a $10M allocation from NASA but the cost is estimated at over $100 M to get to production levels. The Center for Space Nuclear Research has conceived of a potentially better process to produce Pu-238 earlier and for significantly less cost. The new process will also produce dramatically less waste. Potentially, the front end costs could be provided by private industry such that the government only had to pay for the product produced. Under a NASA Phase I NIAC grant, the CSNR has evaluated the feasibility of using a low power, commercially available nuclear reactor to produce at least 1.5 kg of Pu-238 per year. The impact on the neutronics of the reactor have been assessed, the amount of Neptunium target material estimated, and the production rates calculated. In addition, the size of the post-irradiation processing facility has been established. In addition, a new method for fabricating the Pu-238 product into the form used for power sources has been identified to reduce the cost of the final product. In short, the concept appears to be viable, can produce the amount of Pu-238 needed to support the NASA missions, can be available within a few years, and will cost significantly less than the current DOE program.

  7. Controls on soluble Pu concentrations in PuO2/magnetite suspensions.

    PubMed

    Felmy, Andrew R; Moore, Dean A; Pearce, Carolyn I; Conradson, Steven D; Qafoku, Odeta; Buck, Edgar C; Rosso, Kevin M; Ilton, Eugene S

    2012-11-06

    Time-dependent reduction of PuO(2)(am) was studied over a range of pH values in the presence of aqueous Fe(II) and magnetite (Fe(3)O(4)) nanoparticles. At early time frames (up to 56 days) very little aqueous Pu was mobilized from PuO(2)(am), even though measured pH and redox potentials, coupled to equilibrium thermodynamic modeling, indicated the potential for significant reduction of PuO(2)(am) to relatively soluble Pu(III). Introduction of Eu(III) or Nd(III) to the suspensions as competitive cations to displace possible sorbed Pu(III) resulted in the release of significant concentrations of aqueous Pu. However, the similarity of aqueous Pu concentrations that resulted from the introduction of Eu(III)/Nd(III) to suspensions with and without magnetite indicated that the Pu was solubilized from PuO(2)(am), not from magnetite.

  8. Oxygen diffusion model of the mixed (U,Pu)O2 ± x: Assessment and application

    NASA Astrophysics Data System (ADS)

    Moore, Emily; Guéneau, Christine; Crocombette, Jean-Paul

    2017-03-01

    The uranium-plutonium (U,Pu)O2 ± x mixed oxide (MOX) is used as a nuclear fuel in some light water reactors and considered for future reactor generations. To gain insight into fuel restructuring, which occurs during the fuel lifetime as well as possible accident scenarios understanding of the thermodynamic and kinetic behavior is crucial. A comprehensive evaluation of thermo-kinetic properties is incorporated in a computational CALPHAD type model. The present DICTRA based model describes oxygen diffusion across the whole range of plutonium, uranium and oxygen compositions and temperatures by incorporating vacancy and interstitial migration pathways for oxygen. The self and chemical diffusion coefficients are assessed for the binary UO2 ± x and PuO2 - x systems and the description is extended to the ternary mixed oxide (U,Pu)O2 ± x by extrapolation. A simulation to validate the applicability of this model is considered.

  9. Pu isotopes in the western North Pacific Ocean before the accident at Fukushima Dai-ichi Nuclear Power Station

    NASA Astrophysics Data System (ADS)

    Yamada, M.; Zheng, J.; Aono, T.

    2011-12-01

    Anthropogenic radionuclides such as Pu-239 (half-life: 24100 yr), Pu-240 (half-life: 6560 yr) and Pu-241 (half-life: 14.325 yr) mainly have been released into the environment as the result of atmospheric nuclear weapons testing. In the North Pacific Ocean, two distinct sources of Pu isotopes can be identified; i.e., the global stratospheric fallout and close-in tropospheric fallout from nuclear weapons testing at the Pacific Proving Grounds in the Marshall Islands. The atom ratio of Pu-240/Pu-239 is a powerful fingerprint to identify the sources of Pu in the ocean. The Pu-240/Pu-239 atom ratios in seawater and marine sediment samples collected in the western North Pacific before the accident at Fukushima Dai-ichi Nuclear Power Station will provide useful background data for understanding the process controlling Pu transport and for distinguishing future Pu sources. The atom ratios of Pu-240/Pu-239 in water columns from the Yamato and Tsushima Basins in the Japan Sea were significantly higher than the mean global fallout ratio of 0.18; however, there were no temporal variation of atom ratios during the period from 1984 to 1993 in the Japan Sea. The total Pu-239+240 inventories in the whole water columns were approximately doubled during the period from 1984 to 1993 in the two basins. The atom ratio of Pu-240/Pu-239 in surface water from Sagami Bay, western North Pacific Ocean, was 0.224 and showed no notable variation from the surface to the bottom with the mean atom ratio being 0.234. The atom ratios for the Pacific coast, near the Rokkasho nuclear fuel reprocessing plant, were approximately the same as the 0.224 ratio obtained from Sagami Bay, western North Pacific margin. The atom ratios in the surficial sediments from Sagami Bay ranged from 0.229 to 0.247. The mean atom ratio in the sediment columns in the East China Sea ranged from 0.248 for the Changjiang estuary to 0.268 for the shelf edge. The observed atom ratios were significantly higher than the mean

  10. Oxidation of Pu-bearing solids: A process for Pu recovery from Rocky Flats incinerator ash

    SciTech Connect

    Karraker, D.G.

    1997-07-18

    High-fired PuO{sub 2}, RFP ash heels, and synthetic RFP incinerator ash were easily soluble after oxidation of Pu(IV) to Pu(VI) by heating with Na{sub 2}O{sub 2} or KO{sub 2} to 450{degrees} for two hours. This offers a route to the recovery of Pu from these and similar PuO{sub 2}-bearing solids that can be carried out in present equipment. Evidence for new compounds K{sub 2}PuO{sub 4}, K{sub 4}PuO{sub 5} and K{sub 6}PuO{sub 6} is presented. A process for recovery of Pu from RFP incinerator ash is presented.

  11. Characterization and property evaluation of U-15 wt%Pu alloy for fast reactor

    NASA Astrophysics Data System (ADS)

    Kaity, Santu; Banerjee, Joydipta; Ravi, K.; Keswani, R.; Kutty, T. R. G.; Kumar, Arun; Prasad, G. J.

    2013-02-01

    The characterization and high temperature behaviour of U-15 wt%Pu alloy has been investigated in this study for the first time. U-15 wt%Pu alloy sample for this study was prepared by following melting and casting route. Microstructural characterization of the alloy was carried out by XRD and optical microscopy. The thermophysical properties like phase transition temperatures, coefficient of thermal expansion and hot hardness of the above alloy were determined. Eutectic temperature between T91 and U-15 wt%Pu was established. Apart from that, the fuel-cladding chemical compatibility of U-15 wt%Pu alloy with T91 grade steel was studied by diffusion couple experiment.

  12. Controls on Soluble Pu Concentrations in PuO2/Magnetite Suspensions

    SciTech Connect

    Felmy, Andrew R.; Moore, Dean A.; Pearce, Carolyn I.; Conradson, Steven D.; Qafoku, Odeta; Buck, Edgar C.; Rosso, Kevin M.; Ilton, Eugene S.

    2012-11-06

    Time-dependent reduction of PuO2(am) was studied over a range of pH values in the presence of aqueous Fe(II) and magnetite (Fe3O4) nanoparticles. At early time frames (up to 56 days) very little aqueous Pu was mobilized from PuO2(am), even though measured pH and redox potentials, coupled to equilibrium thermodynamic modeling indicated the potential for significant reduction of PuO2(am) to relatively soluble Pu(III). Introduction of Eu(III) or Nd(III) to the suspensions as competitive cations to displace possible sorbed Pu(III) resulted in the release of significant concentrations of aqueous Pu. However, the similarity of aqueous Pu concentrations that resulted from the introduction of Eu(III)/Nd(III) to suspensions with and without magnetite indicated that the Pu was displaced from the PuO2(am), not from magnetite. The fact that soluble forms of Pu can be displaced from the surface of PuO2(am) represents a potential, but previously unidentified, source of Pu to aqueous solution or subsurface groundwaters.

  13. Adsorption of Atmospheric Gases on Pu Surfaces

    SciTech Connect

    Nelson, A J; Holliday, K S; Stanford, J A; Grant, W K; Erler, R G; Allen, P G; McLean, W; Roussel, P

    2012-03-29

    Surface adsorption represents a competition between collision and scattering processes that depend on surface energy, surface structure and temperature. The surface reactivity of the actinides can add additional complexity due to radiological dissociation of the gas and electronic structure. Here we elucidate the chemical bonding of gas molecules adsorbed on Pu metal and oxide surfaces. Atmospheric gas reactions were studied at 190 and 300 K using x-ray photoelectron spectroscopy. Evolution of the Pu 4f and O 1s core-level states were studied as a function of gas dose rates to generate a set of Langmuir isotherms. Results show that the initial gas dose forms Pu{sub 2}O{sub 3} on the Pu metal surface followed by the formation of PuO{sub 2} resulting in a layered oxide structure. This work represents the first steps in determining the activation energy for adsorption of various atmospheric gases on Pu.

  14. Pu electronic structure and photoelectron spectroscopy

    SciTech Connect

    Joyce, John J; Durakiewicz, Tomasz; Graham, Kevin S; Bauer, Eric D; Moore, David P; Mitchell, Jeremy N; Kennison, John A; Martin, Richard L; Roy, Lindsay E; Scuseria, G. E.

    2010-01-01

    The electronic structure of PuCoGa{sub 5}, Pu metal, and PuO{sub 2} is explored using photoelectron spectroscopy. Ground state electronic properties are inferred from temperature dependent photoemission near the Fermi energy for Pu metal. Angle-resolved photoemission details the energy vs. crystaJ momentum landscape near the Fermi energy for PuCoGa{sub 5} which shows significant dispersion in the quasiparticle peak near the Fermi energy. For the Mott insulators AnO{sub 2}(An = U, Pu) the photoemission results are compared against hybrid functional calculations and the model prediction of a cross over from ionic to covalent bonding is found to be reasonable.

  15. Pu, 137Cs and excess 210Pb in Russian Arctic sediments

    NASA Astrophysics Data System (ADS)

    Baskaran, M.; Asbill, Shaunna; Santschi, Peter; Brooks, James; Champ, Michael; Adkinson, Dan; Colmer, Matthew R.; Makeyev, Vyacheslav

    1996-05-01

    The activity ratios of Pu and radiocesium isotopes have been used to delineate the major sources (such as global and close-in (debris) fallout, nuclear fuel reprocessing and fabrication plant effluents) in the environment. We have measured 238Pu, 239,240Pu, 137Cs, and excess 210Pb concentrations in 107 surficial sediments as well as in 5 sediment cores collected in the summer months of 1993 and 1994 from the Ob and Yenisey Rivers (Russia) and the Kara sea. A comparison of the sediment core inventories of 239,240Pu and 137Cs, along with the 238Pu/ 239,240Pu activity ratios, with those expected from global fallout allows us to estimate the relative amounts, if any, of reactor-derived 238Pu and 239,240Pu from the dumped reactor sites in the study area. In surficial sediment samples collected in 1993 and 1994, the 239,240Pu concentrations varied between 4.2 and 856 mBq kg -1, with a mean of 239 mBq kg -1. In samples with a measurable 238Pu, the 238Pu/ 239,240Pu activity ratios varied between 0.010 and 0.069, with an average value of 0.035 ± 0.014. This range can be compared to the average 238Pu/ 239,240Pu activity ratio of 0.030 for the year 1993 from nuclear weapons testing and SNAP fallout obtained from soil studies, indicating very little (≤ 5%) additional sources of 238Pu to the sediments in the study area. The inventories of Pu in the 5 sediment cores from the study area varied between 2.67 ± 0.67 and 24.5 ± 2.2 Bq m -2 with a mean value of 8.83 Bq m -2. The 137Cs concentrations in the upper 3 cm of the sediments varied between below detection limit to 71.4 Bq kg -1, with a mean of 14.9 Bq kg -1. The 137Cs inventories in the 5 sediment cores varied between 156.7 ± 28.3 and 1600 ± 153.3 Bq m -2, with a mean value of 583.3 Bq m -2. The mean ratio of inventories of Pu to that of 137Cs, 0.015, is comparable to the values in other places in the Arctic region. There is a significant correlation between total organic carbon and concentrations of 137Cs, 239,240Pu

  16. Recovery of 238PuO2 by Molten Salt Oxidation Processing of 238PuO2 Contaminated Combustibles (Part II)

    NASA Astrophysics Data System (ADS)

    Remerowski, Mary Lynn; Dozhier, C.; Krenek, K.; VanPelt, C. E.; Reimus, M. A.; Spengler, D.; Matonic, J.; Garcia, L.; Rios, E.; Sandoval, F.; Herman, D.; Hart, R.; Ewing, B.; Lovato, M.; Romero, J. P.

    2005-02-01

    Pu-238 heat sources are used to fuel radioisotope thermoelectric generators (RTG) used in space missions. The demand for this fuel is increasing, yet there are currently no domestic sources of this material. Much of the fuel is material reprocessed from other sources. One rich source of Pu-238 residual material is that from contaminated combustible materials, such as cheesecloth, ion exchange resins and plastics. From both waste minimization and production efficiency standpoints, the best solution is to recover this material. One way to accomplish separation of the organic component from these residues is a flameless oxidation process using molten salt as the matrix for the breakdown of the organic to carbon dioxide and water. The plutonium is retained in the salt, and can be recovered by dissolution of the carbonate salt in an aqueous solution, leaving the insoluble oxide behind. Further aqueous scrap recovery processing is used to purify the plutonium oxide. Recovery of the plutonium from contaminated combustibles achieves two important goals. First, it increases the inventory of Pu-238 available for heat source fabrication. Second, it is a significant waste minimization process. Because of its thermal activity (0.567 W per gram), combustibles must be packaged for disposition with much lower amounts of Pu-238 per drum than other waste types. Specifically, cheesecloth residues in the form of pyrolyzed ash (for stabilization) are being stored for eventual recovery of the plutonium.

  17. Extinct 244Pu in ancient zircons.

    PubMed

    Turner, Grenville; Harrison, T Mark; Holland, Greg; Mojzsis, Stephen J; Gilmour, Jamie

    2004-10-01

    We have found evidence, in the form of fissiogenic xenon isotopes, for in situ decay of 244Pu in individual 4.1- to 4.2-billion-year-old zircons from the Jack Hills region of Western Australia. Because of its short half-life, 82 million years, 244Pu was extinct within 600 million years of Earth's formation. Detrital zircons are the only known relics to have survived from this period, and a study of their Pu geochemistry will allow us to date ancient metamorphic events and determine the terrestrial Pu/U ratio for comparison with the solar ratio.

  18. Design Studies of ``100% Pu'' Mox Lead Test Assembly

    SciTech Connect

    Pavlovichev, A.M.

    2001-01-11

    In this document the results of neutronics studies of <<100%Pu>> MOX LTA design are presented. The parametric studies of infinite MOX-UOX grids, MOX-UOX core fragments and of VVER-1000 core with 3 MOX LTAs are performed. The neutronics parameters of MOX fueled core have been performed for the chosen design MOX LTA using the Russian 3D code BIPR-7A and 2D code PERMAK-A with the constants prepared by the cell spectrum code TVS-M.

  19. New measurement of the 242Pu(n,γ) cross section at n_TOF

    NASA Astrophysics Data System (ADS)

    Lerendegui-Marco, J.; Guerrero, C.; Cortés-Giraldo, M. A.; Quesada, J. M.; Mendoza, E.; Cano-Ott, D.; Eberhardt, K.; Junghans, A.

    2016-03-01

    The use of MOX fuel (mixed-oxide fuel made of UO2 and PuO2) in nuclear reactors allows substituting a large fraction of the enriched Uranium by Plutonium reprocessed from spent fuel. With the use of such new fuel composition rich in Pu, a better knowledge of the capture and fission cross sections of the Pu isotopes becomes very important. In particular, a new series of cross section evaluations have been recently carried out jointly by the European (JEFF) and United States (ENDF) nuclear data agencies. For the case of 242Pu, the two only neutron capture time-of-flight measurements available, from 1973 and 1976, are not consistent with each other, which calls for a new time-of flight capture cross section measurement. In order to contribute to a new evaluation, we have perfomed a neutron capture cross section measurement at the n_TOF-EAR1 facility at CERN using four C6D6 detectors, using a high purity target of 95 mg. The preliminary results assessing the quality and limitations (background, statistics and γ-flash effects) of this new experimental data are presented and discussed, taking into account that the aimed accuracy of the measurement ranges between 7% and 12% depending on the neutron energy region.

  20. 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.

    PubMed

    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.

  1. Use of plutonium isotope activity ratios in dating recent sediments. [/sup 238/Pu//sup 239/Pu + /sup 240/Pu

    SciTech Connect

    Beasley, T. M.

    1982-01-01

    The majority of plutonium presently in the biosphere has come from the testing of nuclear devices. In the early 1950s, the Pu-238/239+240 activity ratio of fallout debris was > 0.04; in the more extensive test series of 1961 to 1962, the Pu-238/239+240 activity ratios were quite consistent at 0.02 to 0.03 and maximum fallout delivery occurred in mid-1963. A significant perturbation in Pu isotope activity ratios occurred in mid-1966 with the deposition of Pu-238 from the SNAP-9A reentry and burn-up. Recently deposited sediments have recorded these events and where accumulation rates are rapid (> 1 cm/y), changes in Pu isotope activity ratios can be used as a geochronological tool.

  2. Biodegradation of PuEDTA and Impacts on Pu Mobility

    SciTech Connect

    Xun, Luying; Bolton, Jr., Harvey

    2001-06-01

    Ethylenediaminetetraacetate (EDTA) and nitrilotriacetate (NTA) are synthetic chelating agents, which can form strong water-soluble complexes with radionuclides and metals and has been used to decontaminate and process nuclear materials. Synthetic chelating agents were co-disposed with radionuclides (e.g., 60Co, Pu) and heavy metals enhancing their transport in the subsurface. An understanding of EDTA biodegradation is essential to help mitigate enhanced radionuclide transport by EDTA. The objective of this research is to develop fundamental data on factors that govern the biodegradation of radionuclide-EDTA. These factors include the dominant EDTA aqueous species, the biodegradation of various metal-EDTA complexes, the uptake of various metal-EDTA complexes into the cell, the distribution and mobility of the radionuclide during and after EDTA biodegradation, and the enzymology and genetics of EDTA biodegradation.

  3. Determination of the 240Pu/ 239Pu atomic ratio in soils from Palomares (Spain) by low-energy accelerator mass spectrometry

    NASA Astrophysics Data System (ADS)

    Chamizo, E.; García-León, M.; Synal, H.-A.; Suter, M.; Wacker, L.

    2006-08-01

    In 1966, the nuclear fuel of two thermonuclear bombs was released over the Spanish region of Palomares, due to a B52 bomber accident during a refuelling operation. Since then, much effort has been made to assess its impact to the different environmental compartments of this area in South-East Spain, mostly by measuring the 239+240Pu activity concentration and the 238Pu/239+240Pu activity ratio. Nevertheless, these measurements do not give enough information on the problem. In order to recognize unambiguously small traces of the weapon-grade plutonium released in the accident, the ratio of the two major isotopes of plutonium, 240Pu/239Pu, has to be determined. In this work, this ratio has been measured in low- and high-activity samples from Palomares by means of low-energy accelerator mass spectrometry (AMS). That way, we will show the potential of the new generation of compact AMS facilities in terms of plutonium characterization at ultra-trace levels.

  4. Software Aspects of PuMa-II

    NASA Astrophysics Data System (ADS)

    Karuppusamy, R.; Stappers, B.; Stappers, B.

    2006-08-01

    The Pulsar Machine II (PuMa-II) is a state of the art pulsar machine-installed at the Westerbork Synthesis Radio Telescope (WSRT), in December 2005. PuMa-II is a flexible instrument and is designed around an ensemble of 44 high-performance computers running the Linux operating system. Much of the flexibility of PuMa-II comes from the software that is being developed for this instrument. The radio signals reaching the telescope undergo several stages of electronic and software processing before a scientifically useful data product is generated. The electronic processing of signals includes the usual RF to IF conversion, analogue to digital conversion and telescope dependent electronic digital delay compensation that happen in the signal chain of WSRT. Within PuMa-II, this data is acquired, stored and suitably processed. In this poster we present various aspects of PuMa-II software and illustrate its pulsar signal processing capabilities.

  5. Distribution of nuclear bomb Pu in Nishiyama area, Nagasaki, estimated by accurate and precise determination of 240Pu/239Pu ratio in soils.

    PubMed

    Yoshida, S; Muramatsu, Y; Yamazaki, S; Ban-Nai, T

    2007-01-01

    Plutonium isotopes in forest soils collected in Nishiyama area, Nagasaki, were successfully determined by high resolution inductively coupled plasma mass spectrometry after the treatment with a microwave decomposition system. The (240)Pu/(239)Pu atom ratios observed in the samples in the Nishiyama area were obviously lower than the range of the global fallout. The low ratios (minimum 0.032) observed in Nishiyama area indicated the influence of detonation of the Pu nuclear weapon in 1945. Since the area is contaminated also by global fallout, the (240)Pu/(239)Pu atom ratio can be more sensitive indicator of bomb-derived Pu than Pu activity concentration.

  6. Flowsheet Analysis of U-Pu Co-Crystallization Process as a New Reprocessing System

    SciTech Connect

    Shunji Homma; Jun-ichi Ishii; Jiro Koga; Shiro Matsumoto; Toshiaki Kikuchi; Takahiro Chikazawa; Atsuhiro Shibata

    2006-07-01

    A new fuel reprocessing system by U-Pu co-crystallization process is proposed and examined by flowsheet analysis. This reprocessing system is based on the fact that hexavalent plutonium in nitric acid solution is co-crystallized with uranyl nitrate, whereas it is not crystallized when uranyl nitrate does not exist in the solution. The system consists of five steps: dissolution of spent fuel, plutonium oxidation, U-Pu co-crystallization as a co-decontamination, re-dissolution of the crystals, and U re-crystallization as a U-Pu separation. The system requires a recycling of the mother liquor from the U-Pu co-crystallization step and the appropriate recycle ratio is determined by flowsheet analysis such that the satisfactory decontamination is achieved. Further flowsheet study using four different compositions of LWR spent fuels demonstrates that the constant ratio of plutonium to uranium in mother liquor from the re-crystallization step is achieved for every composition by controlling the temperature. It is also demonstrated by comparing to the Purex process that the size of the plant based on the proposed system is significantly reduced. (authors)

  7. Analysis on fuel breeding capability of FBR core region based on minor actinide recycling doping

    NASA Astrophysics Data System (ADS)

    Permana, Sidik; Novitrian, Waris, Abdul; Ismail, Suzuki, Mitsutoshi; Saito, Masaki

    2014-09-01

    Nuclear fuel breeding based on the capability of fuel conversion capability can be achieved by convertion rasio of some fertile materials into fissile materials during nuclear reaction processes such as main fissile materials of U-233, U-235, Pu-239 and Pu-241 and for fertile materials of Th-232, U-238, and Pu-240 as well as Pu-238. Minor actinide (MA) loading option which consists of neptunium, americium and curium will gives some additional contribution from converted MA into plutonium such as conversion Np-237 into Pu-238 and it's produced Pu-238 converts to Pu-239 via neutron capture. Increasing composition of Pu-238 can be used to produce fissile material of Pu-239 as additional contribution. Trans-uranium (TRU) fuel (Mixed fuel loading of MOX (U-Pu) and MA composition) and mixed oxide (MOX) fuel compositions are analyzed for comparative analysis in order to show the effect of MA to the plutonium productions in core in term of reactor criticality condition and fuel breeding capability. In the present study, neptunium (Np) nuclide is used as a representative of MAin trans-uranium (TRU) fuel composition as Np-MOX fuel type. It was loaded into the core region gives significant contribution to reduce the excess reactivity in comparing to mixed oxide (MOX) fuel and in the same time it contributes to increase nuclear fuel breeding capability of the reactor. Neptunium fuel loding scheme in FBR core region gives significant production of Pu-238 as fertile material to absorp neutrons for reducing excess reactivity and additional contribution for fuel breeding.

  8. Analysis on fuel breeding capability of FBR core region based on minor actinide recycling doping

    SciTech Connect

    Permana, Sidik; Novitrian,; Waris, Abdul; Ismail; Suzuki, Mitsutoshi; Saito, Masaki

    2014-09-30

    Nuclear fuel breeding based on the capability of fuel conversion capability can be achieved by conversion ratio of some fertile materials into fissile materials during nuclear reaction processes such as main fissile materials of U-233, U-235, Pu-239 and Pu-241 and for fertile materials of Th-232, U-238, and Pu-240 as well as Pu-238. Minor actinide (MA) loading option which consists of neptunium, americium and curium will gives some additional contribution from converted MA into plutonium such as conversion Np-237 into Pu-238 and it's produced Pu-238 converts to Pu-239 via neutron capture. Increasing composition of Pu-238 can be used to produce fissile material of Pu-239 as additional contribution. Trans-uranium (TRU) fuel (Mixed fuel loading of MOX (U-Pu) and MA composition) and mixed oxide (MOX) fuel compositions are analyzed for comparative analysis in order to show the effect of MA to the plutonium productions in core in term of reactor criticality condition and fuel breeding capability. In the present study, neptunium (Np) nuclide is used as a representative of MAin trans-uranium (TRU) fuel composition as Np-MOX fuel type. It was loaded into the core region gives significant contribution to reduce the excess reactivity in comparing to mixed oxide (MOX) fuel and in the same time it contributes to increase nuclear fuel breeding capability of the reactor. Neptunium fuel loading scheme in FBR core region gives significant production of Pu-238 as fertile material to absorp neutrons for reducing excess reactivity and additional contribution for fuel breeding.

  9. NEUTRONIC REACTOR FUEL ELEMENT

    DOEpatents

    Shackleford, M.H.

    1958-12-16

    A fuel element possessing good stability and heat conducting properties is described. The fuel element comprises an outer tube formed of material selected from the group consisting of stainhess steel, V, Ti. Mo. or Zr, a fuel tube concentrically fitting within the outer tube and containing an oxide of an isotope selected from the group consisting of U/sup 235/, U/sup 233/, and Pu/sup 239/, and a hollow, porous core concentrically fitting within the fuel tube and formed of an oxide of an element selected from the group consisting of Mg, Be, and Zr.

  10. Neutronics Simulations of 237Np Targets to Support Safety-Basis and 238Pu Production Assessment Efforts at the High Flux Isotope Reactor

    SciTech Connect

    Chandler, David; Ellis, Ronald James

    2015-01-01

    Fueled by two highly enriched uranium-bearing fuel elements surrounded by a large concentric ring of beryllium reflector, the High Flux Isotope Reactor (HFIR) provides one of the highest neutron fluxes in the world and is used to produce unique isotopes like plutonium-238. The National Aeronautics and Space Administration use radioisotope thermoelectric generators powered by 238Pu for deep-space missions. As part of the US Department of Energy s task to reestablish the domestic production of 238Pu, a technology demonstration sub-project has been initiated to establish a new 238Pu supply chain. HFIR safety-basis neutronics calculations are being performed to ensure the target irradiations have no adverse impacts on reactor performance and to calculate data required as input to follow-on thermal-structural, thermal-hydraulic and radionuclide/dose analyses. Plutonium-238 production assessments are being performed to estimate the amount of 238Pu that can be produced in HFIR s permanent beryllium reflector. It is estimated that a total of 0.96 1.12 kg 238Pu (~1.28 1.49 kg PuO2 at 85% 238Pu/Pu purity) could be produced per year in HFIR s permanent beryllium reflector irradiation facilities if they are all utilized.

  11. Thermodynamic assessment of the LiF-ThF4-PuF3-UF4 system

    NASA Astrophysics Data System (ADS)

    Capelli, E.; Beneš, O.; Konings, R. J. M.

    2015-07-01

    The LiF-ThF4-PuF3-UF4 system is the reference salt mixture considered for the Molten Salt Fast Reactor (MSFR) concept started with PuF3. In order to obtain the complete thermodynamic description of this quaternary system, two binary systems (ThF4-PuF3 and UF4-PuF3) and two ternary systems (LiF-ThF4-PuF3 and LiF-UF4-PuF3) have been assessed for the first time. The similarities between CeF3/PuF3 and ThF4/UF4 compounds have been taken into account for the presented optimization as well as in the experimental measurements performed, which have confirmed the temperatures predicted by the model. Moreover, the experimental results and the thermodynamic database developed have been used to identify potential compositions for the MSFR fuel and to evaluate the influence of partial substitution of ThF4 by UF4 in the salt.

  12. Resonant photoemission in f-electron systems: Pu and Gd

    NASA Astrophysics Data System (ADS)

    Tobin, J. G.; Chung, B. W.; Schulze, R. K.; Terry, J.; Farr, J. D.; Shuh, D. K.; Heinzelman, K.; Rotenberg, E.; Waddill, G. D.; van der Laan, G.

    2003-10-01

    Resonant photoemission in the Pu 5f and Pu 6p states is compared to that in the Gd 4f and Gd 5p states. Spectral simulations, based upon an atomic model with angular momentum coupling, are compared to the Gd and Pu results. Additional spectroscopic measurements of Pu, including core level photoemission and x-ray absorption, are also presented.

  13. Resonant Photoemission in f Electron Systems: Pu& Gd

    SciTech Connect

    Tobin, J G; Chung, B W; Schulze, R K; Terry, J; Farr, J D; Shuh, D K; Heinzelman, K; Rotenberg, E; Waddill, G D; van der Laan, G

    2003-03-07

    Resonant photoemission in the Pu5f and Pu6p states is compared to that in the Gd4f and Gd5p states. Spectral simulations, based upon and atomic model with angular momentum coupling, are compared to the Gd and Pu results. Additional spectroscopic measurements of Pu, including core level photoemission and x-ray absorption are also presented.

  14. Resonant photoemission in f electron systems: Pu and Gd

    SciTech Connect

    Tobin, J.G.; Chung, B.W.; Waddill, G.D.; Schulze, R.K.; Terry,J.; Farr, J.D.; Zocco, T.; Shuh, D.K.; Heinzelman, K.; Rotenberg, E.; Vander Laan, G.

    2003-10-14

    Resonant photoemission in the Pu 5f and Pu 6p states is compared to that in the Gd 4f and Gd 5p states. Spectral simulations, based upon an atomic model with angular momentum coupling, are compared to the Gd and Pu results. Additional spectroscopic measurements of Pu, including core level photoemission and x-ray absorption, are also presented.

  15. PuMa, a digital Pulsar Machine

    NASA Astrophysics Data System (ADS)

    Voûte, J. L. L.; Kouwenhoven, M. L. A.; van Haren, P. C.; Langerak, J. J.; Stappers, B. W.; Driesens, D.; Ramachandran, R.; Beijaard, Th. D.

    2002-04-01

    We have designed and constructed PuMa, a pulsar machine that has both a baseband recording and a digital filterbank mode. Its design is based on the use of digital signal processors (DSPs). Their operation is controlled by software, which makes PuMa reconfigurable, flexible and easy to operate. The maximum number of channels in the digital filterbank mode is 32 768 over a bandwidth of 80 MHz. This makes PuMa suitable for pulsar observations at low sky frequencies. The maximum bandwidth in baseband recording mode is two times 10 MHz. The machine was installed at the Westerbork Synthesis Radio Telescope in The Netherlands in 1998. We discuss in some detail PuMa's technical properties and capabilities. Recent observations, a sample of which are presented here, demonstrate its capabilities and that it is performing up to its specifications.

  16. Development of prototype induced-fission-based Pu accountancy instrument for safeguards applications.

    PubMed

    Seo, Hee; Lee, Seung Kyu; An, Su Jung; Park, Se-Hwan; Ku, Jeong-Hoe; Menlove, Howard O; Rael, Carlos D; LaFleur, Adrienne M; Browne, Michael C

    2016-09-01

    Prototype safeguards instrument for nuclear material accountancy (NMA) of uranium/transuranic (U/TRU) products that could be produced in a future advanced PWR fuel processing facility has been developed and characterized. This is a new, hybrid neutron measurement system based on fast neutron energy multiplication (FNEM) and passive neutron albedo reactivity (PNAR) methods. The FNEM method is sensitive to the induced fission rate by fast neutrons, while the PNAR method is sensitive to the induced fission rate by thermal neutrons in the sample to be measured. The induced fission rate is proportional to the total amount of fissile material, especially plutonium (Pu), in the U/TRU product; hence, the Pu amount can be calibrated as a function of the induced fission rate, which can be measured using either the FNEM or PNAR method. In the present study, the prototype system was built using six (3)He tubes, and its performance was evaluated for various detector parameters including high-voltage (HV) plateau, efficiency profiles, dead time, and stability. The system's capability to measure the difference in the average neutron energy for the FNEM signature also was evaluated, using AmLi, PuBe, (252)Cf, as well as four Pu-oxide sources each with a different impurity (Al, F, Mg, and B) and producing (α,n) neutrons with different average energies. Future work will measure the hybrid signature (i.e., FNEM×PNAR) for a Pu source with an external interrogating neutron source after enlarging the cavity size of the prototype system to accommodate a large-size Pu source (~600g Pu).

  17. Synthesis of Pu-Doped Ceramic

    SciTech Connect

    Anderson, E. B

    1998-09-02

    Plutonium-doped zircon containing about 10 wt% Pu was synthesized in this cooperative project between Russia and the United States conducted at the V. G. Khlopin Radium Institute. The sol-gel method was used for starting precursor preparation to provide complete mixing of initial components and to avoid dust formation inside the glove-box. The sol-gel process also gives interim Pu stabilization in the form of amorphous zirconium hydrosilicate (AZHS), which is a result of gel solidification. AZHS is a solid and relatively durable material that can be easy converted into crystalline zircon by pressureless sintering, thus avoiding significant radioactive contamination of laboratory equipment. A methanol-aqueous solution of tetraethoxysilane Si(OC2H5)4, Pu-nitrate, and zirconil oxynitrate was prepared in final stoichiometry of zircon (Zr,Pu)SiO4 80 wt% + zirconia (Zr,Pu)O2 20 wt%. Gelation occurred after 90 hours at room temperature. AZHS with excess of zirconia 20 wt% was obtained as an interim calcine product and then it was converted into zircon/zirconia ceramic by sintering at 1490 to 1500°C in air for different time periods. The samples obtained were studied by SRD and ESEM methods. It was found that both zircon yield and zircon cell parameters that are correlated with Pu incorporation depend on sintering time.

  18. A Neutronic Analysis of TRU Recycling in PWRs Loaded with MOX-UE Fuel (MOX with U-235 Enriched U Support)

    SciTech Connect

    G. Youinou; S. Bays

    2009-05-01

    This report presents the results of a study dealing with the homogeneous recycling of either Pu or Pu+Np or Pu+Np+Am or Pu+Np+Am+Cm in PWRs using MOX-UE fuel, i.e. standard MOX fuel with a U235 enriched uranium support instead of the standard tail uranium (0.25%) for standard MOX fuel. This approach allows to multirecycle Pu or TRU (Pu+MA) as long as U235 is available, by keeping the Pu or TRU content in the fuel constant and at a value ensuring a negative moderator void coefficient (i.e. the loss of the coolant brings imperatively the reactor to a subcritical state). Once this value is determined, the U235 enrichment of the MOX-UE fuel is adjusted in order to reach the target burnup (51 GWd/t in this study).

  19. The Spectroscopic Signature of Aging in (delta)-Pu(Ga)

    SciTech Connect

    Tobin, J G; Yu, S; Chung, B W

    2009-04-29

    The electronic structure of Pu is briefly discussed, with emphasis upon Aging effects. Photoelectron Spectroscopy and X-ray Absorption Spectroscopy have contributed greatly to our improved understanding of Pu electronic structure. (See Figure 1.) From these and related measurements, the following has been determined: (1) The Pu 5f spin-orbit splitting is large; (2) The number of Pu5f electrons is 5; and (3) The Pu 5f spin-orbit splitting effect dominates 5f itineracy.

  20. Prevention of Pu(IV) polymerization in a PUREX-based process

    SciTech Connect

    Paviet-Hartmann, Patricia; Senentz, Gerald

    2007-07-01

    The US Mixed Oxide (MOX) Fuel Fabrication Facility (MFFF) is being designed to produce MOX fuel assemblies for use in domestic, commercial nuclear power reactors, as part of the U.S. DOE efforts to dispose of surplus weapon-grade plutonium. The feed material is plutonium dioxide from surplus weapon grade plutonium. PuO{sub 2}, issued from a pit disassembly and conversion facility (PDCF), will be processed using a flowsheet derived from the La Hague reprocessing plant to remove impurities. The purified PuO{sub 2} will be blended with UO{sub 2} to form mixed oxide pellets, and loaded into fuel rods, to create MOX fuel assemblies based on the process and technology of the MELOX plant in France,. Safety studies are necessary to support the development of the design basis per regulation 10 CFR Part 70 to complete an integrated safety analysis for the MFFF facility. The formation of tetravalent plutonium polymers in certain process vessels of the aqueous polishing (AP) process has been identified as a potential hazard. Based on scientific literature, the following paper demonstrates that within the AP process units, the polymerization of Pu(IV) will not occur and/or will not create a criticality issue even where the acidity may drop below 0.5 N HNO{sub 3}. We will identify and control the conditions under which plutonium (IV) will not polymerize. (authors)

  1. Fuel element design for the enhanced destruction of plutonium in a nuclear reactor

    DOEpatents

    Crawford, Douglas C.; Porter, Douglas L.; Hayes, Steven L.; Hill, Robert N.

    1999-01-01

    A uranium-free fuel for a fast nuclear reactor comprising an alloy of Pu, Zr and Hf, wherein Hf is present in an amount less than about 10% by weight of the alloy. The fuel may be in the form of a Pu alloy surrounded by a Zr--Hf alloy or an alloy of Pu--Zr--Hf or a combination of both.

  2. Fuel element design for the enhanced destruction of plutonium in a nuclear reactor

    SciTech Connect

    Crawford, D.C.; Porter, D.L.; Hayes, S.L.; Hill, R.N.

    1999-03-23

    A uranium-free fuel for a fast nuclear reactor comprising an alloy of Pu, Zr and Hf, wherein Hf is present in an amount less than about 10% by weight of the alloy. The fuel may be in the form of a Pu alloy surrounded by a Zr--Hf alloy or an alloy of Pu--Zr--Hf or a combination of both. 7 figs.

  3. Fuel element design for the enhanced destruction of plutonium in a nuclear reactor

    SciTech Connect

    Crawford, Douglas C.; Porter, Douglas L.; Hayes, Steven L.; Hill, Robert N.

    1997-12-01

    A uranium-free fuel for a fast nuclear reactor comprising an alloy of Pu, Zr and Hf, wherein Hf is present in an amount less than about 10% by weight of the alloy. The fuel may be in the form of a Pu alloy surrounded by a Zr-Hf alloy or an alloy of Pu-Zr-Hf or a combination of both.

  4. Chemical potential of oxygen in (U, Pu) mixed oxide with Pu/(U+Pu) = 0.46

    NASA Astrophysics Data System (ADS)

    Dawar, Rimpi; Chandramouli, V.; Anthonysamy, S.

    2016-05-01

    Chemical potential of oxygen in (U,Pu) mixed oxide with Pu/(U + Pu) = 0.46 was measured for the first time using H2/H2O gas equilibration combined with solid electrolyte EMF technique at 1073, 1273 and 1473 K covering an oxygen potential range of -525 to -325 kJ mol-1. The effect of oxygen potential on the oxygen to metal ratio was determined. Increase in oxygen potential increases the O/M. In this study the minimum O/M obtained was 1.985 below which reduction was not possible. Partial molar enthalpy ΔHbar O2 and entropy ΔSbar O2 of oxygen were calculated from the oxygen potential data. The values of -752.36 kJ mol-1 and 0.25 kJ mol-1 were obtained for ΔHbar O2 and ΔSbar O2 respectively.

  5. An analysis of plutonium immobilization versus the "spent fuel" standard

    SciTech Connect

    Gray, W L; McKibben, J M

    1998-06-16

    Safe Pu management is an important and urgent task with profound environmental, national, and international security implications. Presidential Policy Directive 13 and analyses by scientific, technical, and international policy organizations brought about a focused effort within the Department of Energy (DOE) to identify and implement long-term disposition paths for surplus Pu. The principal goal is to render surplus Pu as inaccessible and unattractive for reuse in nuclear weapons as Pu in spent reactor fuel. In the Programmatic Environmental Impact Statement and Record of Decision for the Storage and Disposition of Weapons- Usable Fissile Materials (1997), DOE announced pursuit of two disposition technologies: (1) irradiation of Pu as MOX fuel in existing reactors and (2) immobilization of Pu into solid forms containing fission products as a radiation barrier. DOE chose an immobilization approach that includes "use of the can-in-canister option.. . for a portion of the surplus, non-pit Pu material." In the can-in-canister approach, cans of glass or ceramic forms containing Pu are encapsulated within canisters of HLW glass. In support of the selection process, a technical evaluation of retrievability and recoverability of Pu from glass and ceramic forms by a host nation and by rogue nations or subnational groups was completed. The evaluation involved determining processes and flowsheets for Pu recovery, comparing these processes against criteria and metrics established by the Fissile Materials Disposition Program and then comparing the recovery processes against each other and against SNF processes.

  6. First positron annihilation lifetime measurement of Pu

    SciTech Connect

    Colmenares, C.; Howell, R.H.; Ancheta, D.; Cowan, T.; Hanafee, J.; Sterne, P.

    1996-11-21

    We have made the first measurement of defects in an aged sample of {delta} phase, Ga stabilized Pu, using positron annihilation lifetime spectroscopy. This measurement validates the procedure necessary to perform measurements on this highly toxic material and obtain data representative of sample conditions. Comparison of the positron annihilation lifetime analysis of the data with calculated values suggests that He filled vacancies or vacancy clusters dominate the defect population. Such defects are the necessary precursor to void growth and swelling. The evolution of defects resulting from the radioactive decay of Pu during its life in the stockpile is one of the unknown quantities affecting our confidence in predictions of the limit on stockpile components. Radiation damage leads to changes in the size and strength of metals studied for reactor and accelerator use and similar effects may be expected in Pu. The evolution of radiation produced vacancies into larger void structures and accompanying macroscopic swelling may occur in Pu at some age. A detailed understanding of the defects in self irradiated Pu is required to predict the time scale of void swelling and related radiation effects. 1 fig.

  7. Localized 5f electrons in superconducting PuCoIn₅: consequences for superconductivity in PuCoGa₅.

    PubMed

    Bauer, E D; Altarawneh, M M; Tobash, P H; Gofryk, K; Ayala-Valenzuela, O E; Mitchell, J N; McDonald, R D; Mielke, C H; Ronning, F; Griveau, J-C; Colineau, E; Eloirdi, R; Caciuffo, R; Scott, B L; Janka, O; Kauzlarich, S M; Thompson, J D

    2012-02-08

    The physical properties of the first In analog of the PuMGa(5) (M = Co, Rh) family of superconductors, PuCoIn(5), are reported. With its unit cell volume being 28% larger than that of PuCoGa(5), the characteristic spin-fluctuation energy scale of PuCoIn(5) is three to four times smaller than that of PuCoGa(5), which suggests that the Pu 5f electrons are in a more localized state relative to PuCoGa(5). This raises the possibility that the high superconducting transition temperature T(c) = 18.5 K of PuCoGa(5) stems from the proximity to a valence instability, while the superconductivity at T(c) = 2.5 K of PuCoIn(5) is mediated by antiferromagnetic spin fluctuations associated with a quantum critical point.

  8. The geochemistry of fallout plutonium in the North Atlantic: II. 240Pu /239Pu ratios and their significance

    NASA Astrophysics Data System (ADS)

    Buesseler, Ken O.; Sholkovitz, Edward R.

    1987-10-01

    A systematic decrease in the 240Pu /239Pu ratio in marine sediments is found with increasing water depth along a transect of cores between Woods Hole and Bermuda. The 240Pu /239Pu atom ratios range from ≅O.18 on the shelf to ≅O.10 at 5000 m but do not change with depth in individual cores. A model is presented which can account for the range of 240Pu /239Pu ratios found in this and other similar studies ( NOSHKIN and GATROUSIS, 1974; SCOTTet al., 1983). We propose that there have been at least two distinct sources of fallout Pu to this region. The major source of Pu is global stratospheric fallout, characterized by a 240Pu /239Pu ratio of 0.18 and a relatively long residence time in seawater. The second source is characterized by a much lower 240Pu /239Pu ratio, and relative to global fallout it must have been much more efficiently removed from the water column to deep-sea sediments. We suggest that surface-based low yield testing at the Nevada Test Site is the only source of low ratio fallout Pu which could account for the timing, inventories, and refractory characteristics of this second component of fallout Pu inputs to the North Atlantic.

  9. Microstructural Characterization of Cast Metallic Transmutation Fuels

    SciTech Connect

    J. I. Cole; D. D. Keiser; J. R. Kennedy

    2007-09-01

    As part of the Global Nuclear Energy Partnership (GNEP) and the Advanced Fuel Cycle Initiative (AFCI), the US Department of Energy (DOE) is participating in an international collaboration to irradiate prototypic actinide-bearing transmutation fuels in the French Phenix fast reactor (FUTURIX-FTA experiment). The INL has contributed to this experiment by fabricating and characterizing two compositions of metallic fuel; a non-fertile 48Pu-12Am-40Zr fuel and a low-fertile 35U-29Pu-4Am-2Np-30Zr fuel for insertion into the reactor. This paper highlights results of the microstructural analysis of these cast fuels, which were reasonably homogeneous in nature, but had several distinct phase constituents. Spatial variations in composition appeared to be more pronounced in the low-fertile fuel when compared to the non-fertile fuel.

  10. The basic features of a closed fuel cycle without fast reactors

    NASA Astrophysics Data System (ADS)

    Bobrov, E. A.; Alekseev, P. N.; Teplov, P. S.

    2017-01-01

    In this paper the basic features of a closed fuel cycle with thermal reactors are considered. The three variants of multiple Pu and U recycling in VVER reactors was investigated. The comparison of MOX and REMIX fuel approaches for closed fuel cycle with thermal reactors is presented. All variants make possible to recycle several times the total amount of Pu and U obtained from spent fuel. The reported study was funded by RFBR according to the research project № 16-38-00021

  11. Effect of polyurethane (PU) - bioactive glass (BG) ratio on the development of BG reinforced PU scaffold

    NASA Astrophysics Data System (ADS)

    Lip, Lim Weng; Abdullah, Tuti Katrina; Zubir, Syazana Ahmad

    2016-12-01

    Nowadays, variety of biomaterials may be used to produce implanted scaffolds such as metal-based, ceramic-based and polymer-based materials. In this study, porous bioactive glass (BG) reinforced polyurethane (PU) composite scaffolds with different PU:BG mass ratio (10 to 40 wt%) were fabricated as a potential candidate for synthetic bone graft. The PU-BG scaffolds were prepared using solvent casting combined with salt leaching (SCPL) method and were subjected to several characterizations including fourier transform infra-red (FTIR) spectroscopy, scanning electron microscopy (SEM) and energy dispersive x-ray spectroscopy (EDX). FTIR spectrum showed the trace of BG particles in the PU-BG scaffolds with high concentration of BG (30 and 40 wt%). EDX confirmed that the white particles in the PU-BG scaffold as observed via SEM micrograph were BG particles. A slightly round and irregular pore structures were observed for the PU-BG scaffolds prepared in this study. More homogeneous pore structures were observed as the amount of BG in the PU-BG scaffold is increased. The overall pore size for all scaffolds was in the range of 130 to 400 µm which is suitable for the growth of bone tissue.

  12. Oxidation behaviour of plutonium rich (U, Pu)C and (U, Pu)O2

    NASA Astrophysics Data System (ADS)

    Sali, S. K.; Kulkarni, N. K.; Phatak, Rohan; Agarwal, Renu

    2016-10-01

    Oxidation behaviour of (U0.3Pu0.7)C1.06 was investigated in air by heating samples up to 1073 K and 1273 K. Thermogravimetry (TG) of the samples and X-ray powder diffraction (XRD) of the intermediate products were used to understand the phenomenon taking place during this process. Theoretical calculations were carried out to understand the multiple phase changes taking place during oxidation of carbide. Theoretical results were validated by XRD analysis of the products obtained at different stages of oxidation. The final oxidized products were found to be a single FCC phase with O/M = 2.15 (M = U + Pu). Oxidation kinetic studies of (U0.3Pu0.7)O2 and (U0.47Pu0.53)O2 were carried out in dry air, using thermogravimetry, under non-isothermal conditions. The activation energy of oxidation was found to be 49 and 70 kJ/mol, respectively. Lattice parameter dependence on Pu/M and O/M of plutonium rich mixed oxide (MOX) was established using combined results of XRD and TG analysis of (U0.3Pu0.7)O2+x and (U0.47Pu0.53)O2+x.

  13. [Acupuncture messenger--Pu Xiang-cheng].

    PubMed

    Du, Huai-bin; Liang, Fan-rong

    2011-06-01

    PU Xiang-cheng is the eminent acupuncture master in modern history of China. He studied diligently in early years and devoted his life to the cause of acupuncture practice and education in Chinese medicine. Combination of acupuncture and herbal medicine, coordination of acupuncture and moxibustion, unique application of acupoints, flexible combination of acupoints and focusing on needling techniques are the essence of his academic thoughts. The life of PU Xiang-cheng, the acupuncture master, and his major academic thoughts are described in this paper, so as to commemorate his contributions to acupuncture theory, practice and promotions.

  14. Neutron Capture Cross Section of 239Pu

    NASA Astrophysics Data System (ADS)

    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.

  15. Polymeric Species of Pu in Low Ionic Strength Media

    SciTech Connect

    Romanovski, V V; Palmer, C E; Shaw, H F; Bourcier, W L; Jardine, L J

    2000-01-27

    The US Government has declared that approximately 50 tons of plutonium is surplus to US needs and should be set aside for eventual disposition. The US is currently following a dual path for the disposition of this plutonium: immobilization and irradiation of mixed-oxide fuel. Some fraction of this plutonium material that is undesirable for use in mixed-oxide fuel will be immobilized in a titanate ceramic and disposed of in a geologic repository for high level waste. The reminder of Pu will be fabricated into mixed-oxide fuel and irradiated in domestic light-water reactors. The resulting spent fuel would also be disposed of in a geologic repository for high level waste. The proposed US repository would be at the Yucca Mountain site in Nevada. Plutonium present in the disposal forms, either ceramics or spent fuel, must remain isolated from the biosphere over the geologic repository regulatory performance period, which is currently 10,000 years. Contamination of the biosphere could result from slow dissolution of the disposal forms followed by transport of the dissolution products into the biosphere by flowing ground water. Measurable amounts of apparently soluble plutonium can be released if plutonium dioxide is exposed to water under some conditions. Furthermore, recent studies in Nevada near the Yucca Mountain Site revealed that plutonium, associated with the colloidal fraction of the groundwater, was detected over a kilometer from its source within 30 years after it was placed underground for a nuclear weapons testing. It was not clear whether plutonium was transported as an intrinsic plutonium colloid or as plutonium sorbed onto colloidal clay or zeolite particles.

  16. A practical strategy for reducing the future security risk of United States spent nuclear fuel

    SciTech Connect

    Chodak, P. III; Buksa, J.J.

    1997-06-01

    Depletion calculations show that advanced oxide (AOX) fuels can be used in existing light water reactors (LWRs) to achieve and maintain virtually any desired level of US (US) reactor-grade plutonium (R-Pu) inventory. AOX fuels are composed of a neutronically inert matrix loaded with R-Pu and erbium. A 1/2 core load of 100% nonfertile, 7w% R-Pu AOX and 3.9 w% UO{sub 2} has a net total plutonium ({sup TOT}Pu) destruction rate of 310 kg/yr. The 20% residual {sup TOT}Pu in discharged AOX contains > 55% {sup 242}Pu making it unattractive for nuclear explosive use. A three-phase fuel-cycle development program sequentially loading 60 LWRs with 100% mixed oxide, 50% AOX with a nonfertile component displacing only some of the {sup 238}U, and 50% AOX, which is 100% nonfertile, could reduce the US plutonium inventory to near zero by 2050.

  17. Transport of 137Cs and 239,240Pu with ice-rafted debris in the Arctic Ocean

    USGS Publications Warehouse

    Landa, E.R.; Reimnitz, E.; Beals, D.M.; Pochkowski, J.M.; Winn, W.G.; Rigor, I.

    1998-01-01

    Ice rafting is the dominant mechanism responsible for the transport of fine-grained sediments from coastal zones to the deep Arctic Basin. Therefore, the drift of ice-rafted debris (IRD) could be a significant transport mechanism from the shelf to the deep basin for radionuclides originating from nuclear fuel cycle activities and released to coastal Arctic regions of the former Soviet Union. In this study, 28 samples of IRD collected from the Arctic ice pack during expeditions in 1989-95 were analyzed for 137Cs by gamma spectrometry and for 239Pu and 240Pu by thermal ionization mass spectrometry. 137Cs concentrations in the IRD ranged from less than 0.2 to 78 Bq??kg-1 (dry weight basis). The two samples with the highest 137Cs concentrations were collected in the vicinity of Franz Josef Land, and their backward trajectories suggest origins in the Kara Sea. Among the lowest 137Cs values are seven measured on sediments entrained on the North American shelf in 1989 and 1995, and sampled on the shelf less than six months later. Concentrations of 239Pu + 240Pu ranged from about 0.02 to 1.8 Bq??kg-1. The two highest values came from samples collected in the central Canada Basin and near Spitsbergen; calculated backward trajectories suggest at least 14 years of circulation in the Canada Basin in the former case, and an origin near Severnaya Zemlya (at the Kara Sea/Laptev Sea boundary) in the latter case. While most of the IRD samples showed 240Pu/239Pu ratios near the mean global fallout value of 0.185, five of the samples had lower ratios, in the 0.119 to 0.166 range, indicative of mixtures of Pu from fallout and from the reprocessing of weapons-grade Pu. The backward trajectories of these five samples suggest origins in the Kara Sea or near Severnaya Zemlya.

  18. THERMOSTATICS AND KINETICS OF TRANSFORMATIONS IN PU-BASED ALLOYS

    SciTech Connect

    Turchi, P; Kaufman, L; Liu, Z

    2006-06-30

    CALPHAD assessment of the thermodynamic properties of a series of Pu-based alloys is briefly presented together with some results on the kinetics of phase formation and transformations in Pu-Ga alloys.

  19. First-principles calculations of PuO(2+/-x).

    PubMed

    Petit, L; Svane, A; Szotek, Z; Temmerman, W M

    2003-07-25

    The electronic structure of PuO(2+/-x) was studied using first-principles quantum mechanics, realized with the self-interaction corrected local spin density method. In the stoichiometric PuO2 compound, Pu occurs in the Pu(IV) oxidation state, corresponding to a localized f4 shell. If oxygen is introduced onto the octahedral interstitial site, the nearby Pu atoms turn into Pu(V) (f3) by transferring electrons to the oxygen. Oxygen vacancies cause Pu(III) (f5) to form by taking up electrons released by oxygen. At T = 0, the PuO2 compound is stable with respect to free oxygen, but the delicate energy balance suggests the possible deterioration of the material during long-term storage.

  20. Pb-Pu superlattices: an example of nanostructured actinide materials.

    PubMed

    Rudin, Sven P

    2007-03-16

    Density functional theory applied to Pb-Pu superlattices reveals two competing phases separated by a Mott transition between itinerant and localized 5f electrons. One phase, corresponding to Pu's bulk alpha phase, exhibits paired up Pu planes, thereby broadening the 5f bandwidth. Allowing spin polarization to emulate the energetics of electron correlation leads to another phase with larger volume, narrow 5f bandwidth, and more uniform local crystal structure, similar to bulk fcc Pu.

  1. Experimental Benchmarking of Pu Electronic Structure

    SciTech Connect

    Tobin, J.G.; Moore, K.T.; Chung, B.W.; Wall, M.A.; Schwartz, A.J.; Ebbinghaus, B.B.; Butterfield, M.T.; Teslich, Jr., N.E.; Bliss, R.A.; Morton, S.A.; Yu, S.W.; Komesu, T.; Waddill, G.D.; van der Laan, G.; Kutepov, A.L.

    2008-10-30

    The standard method to determine the band structure of a condensed phase material is to (1) obtain a single crystal with a well defined surface and (2) map the bands with angle resolved photoelectron spectroscopy (occupied or valence bands) and inverse photoelectron spectroscopy (unoccupied or conduction bands). Unfortunately, in the case of Pu, the single crystals of Pu are either nonexistent, very small and/or having poorly defined surfaces. Furthermore, effects such as electron correlation and a large spin-orbit splitting in the 5f states have further complicated the situation. Thus, we have embarked upon the utilization of unorthodox electron spectroscopies, to circumvent the problems caused by the absence of large single crystals of Pu with well-defined surfaces. Our approach includes the techniques of resonant photoelectron spectroscopy, x-ray absorption spectroscopy, electron energy loss spectroscopy, Fano Effect measurements, and Bremstrahlung Isochromat Spectroscopy, including the utilization of micro-focused beams to probe single-crystallite regions of polycrystalline Pu samples.

  2. Experimental Benchmarking of Pu Electronic Structure

    SciTech Connect

    Tobin, J G; Moore, K T; Chung, B W; Wall, M A; Schwartz, A J; Ebbinghaus, B B; Butterfield, M T; Teslich, Jr., N E; Bliss, R A; Morton, S A; Yu, S W; Komesu, T; Waddill, G D; der Laan, G v; Kutepov, A L

    2005-10-13

    The standard method to determine the band structure of a condensed phase material is to (1) obtain a single crystal with a well defined surface and (2) map the bands with angle resolved photoelectron spectroscopy (occupied or valence bands) and inverse photoelectron spectroscopy (unoccupied or conduction bands). Unfortunately, in the case of Pu, the single crystals of Pu are either nonexistent, very small and/or having poorly defined surfaces. Furthermore, effects such as electron correlation and a large spin-orbit splitting in the 5f states have further complicated the situation. Thus, we have embarked upon the utilization of unorthodox electron spectroscopies, to circumvent the problems caused by the absence of large single crystals of Pu with well-defined surfaces. Our approach includes the techniques of resonant photoelectron spectroscopy [1], x-ray absorption spectroscopy [1,2,3,4], electron energy loss spectroscopy [2,3,4], Fano Effect measurements [5], and Bremstrahlung Isochromat Spectroscopy [6], including the utilization of micro-focused beams to probe single-crystallite regions of polycrystalline Pu samples. [2,3,6

  3. Statistical properties of 243Pu, and 242Pu(n ,γ ) cross section calculation

    NASA Astrophysics Data System (ADS)

    Laplace, T. A.; Zeiser, F.; Guttormsen, M.; Larsen, A. C.; Bleuel, D. L.; Bernstein, L. A.; Goldblum, B. L.; Siem, S.; Garotte, F. L. Bello; Brown, J. A.; Campo, L. Crespo; Eriksen, T. K.; Giacoppo, F.; Görgen, A.; Hadyńska-KlÈ©k, K.; Henderson, R. A.; Klintefjord, M.; Lebois, M.; Renstrøm, T.; Rose, S. J.; Sahin, E.; Tornyi, T. G.; Tveten, G. M.; Voinov, A.; Wiedeking, M.; Wilson, J. N.; Younes, W.

    2016-01-01

    The level density and γ -ray strength function (γ SF ) of 243Pu have been measured in the quasicontinuum using the Oslo method. Excited states in 243Pu were populated using the 242Pu(d ,p ) reaction. The level density closely follows the constant-temperature level density formula for excitation energies above the pairing gap. The γ SF displays a double-humped resonance at low energy as also seen in previous investigations of actinide isotopes. The structure is interpreted as the scissors resonance and has a centroid of ωSR=2.42 (5 ) MeV and a total strength of BSR=10.1 (15 ) μN2 , which is in excellent agreement with sum-rule estimates. The measured level density and γ SF were used to calculate the 242Pu(n ,γ ) cross section in a neutron energy range for which there were previously no measured data.

  4. [Dialectic research on "shu pu" (referring a symptom) and "shu pu" (referring a place)].

    PubMed

    Wang, Z

    2001-01-01

    The name of "shu pu" come from Shen shi fang (Prescriptions of Master Shen), which was quoted by Wai tai mi yao (Medical Secrets of an Official), compiled by Wang Tao of the Tang dynasty. In the successive processes of Zheng lei ben cao (Classified Materia Medica) and Ben cao gang mu (Compendium of Materia Medica), it was mixed up with "shu pu", a symptom, in Su wen ci jin lun (On Banning of Acupuncture in Plain Questions), and "shu pu", a place, in Zhen jiu jia yi jing (A -- B Classin of Acupuncture and Moxibustion). In fact, "shu pu" was the meat of rats with no processing, which can be used externally or administered orally to treat injury due to metallic tools and abscess.

  5. Metallic fuel development

    SciTech Connect

    Walters, L.C.

    1987-01-01

    Metallic fuels are capable of achieving high burnup as a result of design modifications instituted in the late 1960's. The gap between the fuel slug and the cladding is fixed such that by the time the fuel swells to the cladding the fission gas bubbles interconnect and release the fission gas to an appropriately sized plenum volume. Interconnected porosity thus provides room for the fuel to deform from further swelling rather than stress the cladding. In addition, the interconnected porosity allows the fuel pin to be tolerant to transient events because as stresses are generated during a transient event the fuel flows rather than applying significant stress to the cladding. Until 1969 a number of metallic fuel alloys were under development in the US. At that time the metallic fuel development program in the US was discontinued in favor of ceramic fuels. However, development had proceeded to the point where it was clear that the zirconium addition to uranium-plutonium fuel would yield a ternary fuel with an adequately high solidus temperature and good compatibility with austenitic stainless steel cladding. Furthermore, several U-Pu-Zr fuel pins had achieved about 6 at.% bu by the late 1960's, without failure, and thus the prospect for high burnup was promising.

  6. Electronic structure of delta-Pu and PuCoGa[sub 3] from photoemission and the mixed level model

    SciTech Connect

    Joyce, J. J.; Wills, J. M.; Durakiewicz, T.; Butterfield, M. T.; Guziewicz, E.; Sarrao, John L.,; Arko, A. J.; Moore, D. P.; Morales, L. A.; Eriksson, O.

    2004-01-01

    The electronic structure of {delta}-phase Pu metal and the Pu-based superconductor PuCoGa{sub 5} is explored using photoelectron spectroscopy and a novel theoretical scheme. Excellent agreement between calculation and experiment defines a path forward for understanding electronic structure aspects of Pu-based materials. The photoemission results show two separate regions of 5f electron spectral intensity, one at the Fermi energy and another centered 1.2 eV below the Fermi level. A comparison is made between the photoemission data and five computational schemes for {delta}-Pu. The results for {delta}-Pu and PuCoGa{sub 5} indicate 5f electron behavior on the threshold between localized and itinerant and a broader framework for understanding the fundamental electronic properties of the Pu 5f levels in general within two configurations, one localized and one itinerant.

  7. Melting behavior of mixed U-Pu oxides under oxidizing conditions

    NASA Astrophysics Data System (ADS)

    Strach, Michal; Manara, Dario; Belin, Renaud C.; Rogez, Jacques

    2016-05-01

    In order to use mixed U-Pu oxide ceramics in present and future nuclear reactors, their physical and chemical properties need to be well determined. The behavior of stoichiometric (U,Pu)O2 compounds is relatively well understood, but the effects of oxygen stoichiometry on the fuel performance and stability are often still obscure. In the present work, a series of laser melting experiments were carried out to determine the impact of an oxidizing atmosphere, and in consequence the departure from a stoichiometric composition on the melting behavior of six mixed uranium plutonium oxides with Pu content ranging from 14 to 62 wt%. The starting materials were disks cut from sintered stoichiometric pellets. For each composition we have performed two laser melting experiments in pressurized air, each consisting of four shots of different duration and intensity. During the experiments we recorded the temperature at the surface of the sample with a pyrometer. Phase transitions were qualitatively identified with the help of a reflected blue laser. The observed phase transitions occur at a systematically lower temperature, the lower the Pu content of the studied sample. It is consistent with the fact that uranium dioxide is easily oxidized at elevated temperatures, forming chemical species rich in oxygen, which melt at a lower temperature and are more volatile. To our knowledge this campaign is a first attempt to quantitatively determine the effect of O/M on the melting temperature of MOX.

  8. PROPERTIES AND BEHAVIOR OF 238PU RELEVANT TO DECONTAMINATION OF BUILDING 235-F

    SciTech Connect

    Duncan, A.; Kane, M.

    2009-11-24

    This report was prepared to document the physical, chemical and radiological properties of plutonium oxide materials that were processed in the Plutonium Fuel Form Facility (PuFF) in building 235-F at the Savannah River Plant (now known as the Savannah River Site) in the late 1970s and early 1980s. An understanding of these properties is needed to support current project planning for the safe and effective decontamination and deactivation (D&D) of PuFF. The PuFF mission was production of heat sources to power Radioisotope Thermoelectric Generators (RTGs) used in space craft. The specification for the PuO{sub 2} used to fabricate the heat sources required that the isotopic content of the plutonium be 83 {+-} 1% Pu-238 due to its high decay heat of 0.57 W/g. The high specific activity of Pu-238 (17.1 Ci/g) due to alpha decay makes this material very difficult to manage. The production process produced micron-sized particles which proved difficult to contain during operations, creating personnel contamination concerns and resulting in the expenditure of significant resources to decontaminate spaces after loss of material containment. This report examines high {sup 238}Pu-content material properties relevant to the D&D of PuFF. These relevant properties are those that contribute to the mobility of the material. Physical properties which produce or maintain small particle size work to increase particle mobility. Early workers with {sup 238}PuO{sub 2} felt that, unlike most small particles, Pu-238 oxide particles would not naturally agglomerate to form larger, less mobile particles. It was thought that the heat generated by the particles would prevent water molecules from binding to the particle surface. Particles covered with bound water tend to agglomerate more easily. However, it is now understood that the self-heating effect is not sufficient to prevent adsorption of water on particle surfaces and thus would not prevent agglomeration of particles. Operational

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

    PubMed

    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.

  10. Investigating Pu and U isotopic compositions in sediments: a case study in Lake Obuchi, Rokkasho Village, Japan using sector-field ICP-MS and ICP-QMS.

    PubMed

    Zheng, Jian; Yamada, Masatoshi

    2005-08-01

    The objectives of the present work were to study isotope ratios and the inventory of plutonium and uranium isotope compositions in sediments from Lake Obuchi, which is in the vicinity of several nuclear fuel facilities in Rokkasho, Japan. Pu and its isotopes were determined using sector-field ICP-MS and U and its isotopes were determined with ICP-QMS after separation and purification with a combination of ion-exchange and extraction chromatography. The observed (240)Pu/(239)Pu atom ratio (0.186 +/- 0.016) was similar to that of global fallout, indicating that the possible early tropospheric fallout Pu did not deliver Pu from the Pacific Proving Ground to areas above 40 degrees N. The previously reported higher Pu inventory in the deep water area of Lake Obuchi could be attributed to the lateral transportation of Pu deposited in the shallow area which resulted from the migration of deposited global fallout Pu from the land into the lake by river runoff and from the Pacific Ocean by tide movement and sea water scavenging, as well as from direct soil input by winds. The (235)U/(238)U atom ratios ranged from 0.00723 to 0.00732, indicating the natural origin of U in the sediments. The average (234)U/(238)U activity ratio of 1.11 in a sediment core indicated a significant sea water U contribution. No evidence was found for the release of U containing wastes from the nearby nuclear facilities. These results will serve as a reference baseline on the levels of Pu and U in the studied site so that any further contamination from the spent nuclear fuel reprocessing plants, the radioactive waste disposal and storage facilities, and the uranium enrichment plant can be identified, and the impact of future release can be rapidly assessed.

  11. Determination of (239)Pu, (240)Pu, (241)Pu and (242)Pu at femtogram and attogram levels - evidence for the migration of fallout plutonium in an ombrotrophic peat bog profile.

    PubMed

    Quinto, Francesca; Hrnecek, Erich; Krachler, Michael; Shotyk, William; Steier, Peter; Winkler, Stephan R

    2013-04-01

    The isotopic composition of plutonium ((239)Pu, (240)Pu, (241)Pu and (242)Pu) was investigated in a ∼0.5 m long peat core from an ombrotrophic bog (Black Forest, Germany) using clean room procedures and accelerator mass spectrometry (AMS). This sophisticated analytical approach was ultimately needed to detect reliably the Pu concentrations present in the peat samples at femtogram (fg) and attogram (ag) levels. The mean (240)Pu/(239)Pu isotopic ratio of 0.19 ± 0.02 (N = 32) in the peat layers, representing approximately the last 80 years, was in good agreement with the accepted value of 0.18 for the global fallout in the Northern Hemisphere. This finding is largely supported by the corresponding and rather constant (241)Pu/(239)Pu (0.0012 ± 0.0005) and (242)Pu/(239)Pu (0.004 ± 0.001) ratios. Since the Pu isotopic composition characteristic of the global fallout was also identified in peat samples pre-dating the period of atmospheric atom bomb testing (AD 1956-AD 1980), migration of Pu within the peat profile is clearly indicated. These results highlight, for the first time, the mobility of Pu in a peat bog with implications for the migration of Pu in other acidic, organic rich environments such as forest soils and other wetland types. These findings constitute a direct observation of the behaviour of Pu at fg and ag levels in the environment. The AMS measurements of Pu concentrations (referring to a corresponding activity of (240+239)Pu from 0.07 mBq g(-1) to 5 mBq g(-1)) essentially confirm our a priori estimates based on existing (241)Am and (137)Cs data in the investigated peat core and agree well with the global fallout levels from the literature. Exclusively employing the Pu isotope ratios established for the peat samples, the date of the Pu irradiation (AD 1956, correctable to AD 1964) was calculated and subsequently compared to the (210)Pb age of the peat layers; this comparison provided an additional hint that global fallout derived Pu is not fixed in

  12. Isotopic compositions of (236)U and Pu isotopes in "black substances" collected from roadsides in Fukushima prefecture: fallout from the Fukushima Dai-ichi nuclear power plant accident.

    PubMed

    Sakaguchi, Aya; Steier, Peter; Takahashi, Yoshio; Yamamoto, Masayoshi

    2014-04-01

    Black-colored road dusts were collected in high-radiation areas in Fukushima Prefecture. Measurement of (236)U and Pu isotopes and (134,137)Cs in samples was performed to confirm whether refractory elements, such as U and Pu, from the fuel core were discharged and to ascertain the extent of fractionation between volatile and refractory elements. The concentrations of (134,137)Cs in all samples were exceptionally high, ranging from 0.43 to 17.7 MBq/kg, respectively. (239+240)Pu was detected at low levels, ranging from 0.15 to 1.14 Bq/kg, and with high (238)Pu/(239+240)Pu activity ratios of 1.64-2.64. (236)U was successfully determined in the range of (0.28 to 6.74) × 10(-4) Bq/kg. The observed activity ratios for (236)U/(239+240)Pu were in reasonable agreement with those calculated for the fuel core inventories, indicating that trace amounts of U from the fuel cores were released together with Pu isotopes but without large fractionation. The quantities of U and (239+240)Pu emitted to the atmosphere were estimated as 3.9 × 10(6) Bq (150 g) and 2.3 × 10(9) Bq (580 mg), respectively. With regard to U, this is the first report to give a quantitative estimation of the amount discharged. Appreciable fractionation between volatile and refractory radionuclides associated with the dispersal/deposition processes with distance from the Fukushima Dai-ichi Nuclear Power Plant was found.

  13. Biokinetics of sup 237 Pu citrate and nitrate in the rat: Implications for Pu studies in man

    SciTech Connect

    Talbot, R.J.; Knight, D.A.; Morgan, A. )

    1990-08-01

    Plutonium-237 decays mainly by electron capture with a half-life of 45 d. Alpha particles are emitted in only 5 x 10(-3)% of its disintegrations. This nuclide can now be produced with relatively small amounts of alpha-emitting contaminants so that, in principle, {sup 237}Pu can be used for studies of Pu biokinetics in man. However, because of its high specific activity, there was some doubt that its metabolism would be the same as that of the alpha- and beta-emitting isotopes of Pu normally encountered in the nuclear industry. In this study, the biokinetics of nearly pure, high specific activity {sup 237}Pu are compared with those of lower specific activity, impure {sup 237}Pu containing significant amounts of alpha-emitting Pu, following administration to rats by intravenous injection as the citrate. Both the distribution and excretion of the pure and impure {sup 237}Pu used in the two studies were similar and also in good agreement with the results of previously reported studies using {sup 239}Pu and {sup 241}Pu citrate, thus validating the use of {sup 237}Pu for studies of Pu metabolism in man. Data on the biokinetics of {sup 237}Pu nitrate are also included.

  14. Pu speciation in actual and simulated aged wastes

    SciTech Connect

    Lezama-pacheco, Juan S; Conradson, Steven D

    2008-01-01

    X-ray Absorption Fine Structure Spectroscopy (XAFS) at the Pu L{sub II/III} edge was used to determine the speciation of this element in (1) Hanford Z-9 Pu crib samples, (2) deteriorated waste resins from a chloride process ion-exchange purification line, and (3) the sediments from two Waste Isolation Pilot Plant Liter Scale simulant brine systems. The Pu speciation in all of these samples except one is within the range previously displayed by PuO{sub 2+x-2y}(OH){sub y}{center_dot}zH{sub 2}O compounds, which is expected based on the putative thermodynamic stability of this system for Pu equilibrated with excess H{sub 2}O and O{sub 2} under environmental conditions. The primary exception was a near neutral brine experiment that displayed evidence for partial substitution of the normal O-based ligands with Cl{sup -} and a concomitant expansion of the Pu-Pu distance relative to the much more highly ordered Pu near neighbor shell in PuO{sub 2}. However, although the Pu speciation was not necessarily unusual, the Pu chemistry identified via the history of these samples did exhibit unexpected patterns, the most significant of which may be that the presence of the Pu(V)-oxo species may decrease rather than increase the overall solubility of these compounds. Several additional aspects of the Pu speciation have also not been previously observed in laboratory-based samples. The molecular environmental chemistry of Pu is therefore likely to be more complicated than would be predicted based solely on the behavior of PuO{sub 2} under laboratory conditions.

  15. Complementary Pu Resuspension Study at Palomares, Spain

    SciTech Connect

    Shinn, J

    2002-10-01

    Soil in an area near Palomares, Spain, was contaminated with plutonium as a result of a mid-air collision of U.S. military aircraft in January 1966. The assessment for potential inhalation dose can be found in Iranzo et al., (1987). Long-term monitoring has been used to evaluate remedial actions (Iranzo et al., 1988) and there are many supporting studies of the Pu contamination at Palomares that have been carried out by the Centro de Investigaciones Energeticas, Medioambientales y Tecnologicas (CIEMAT) in Madrid. The purpose of this study is to evaluate the resuspension of Pu from the soil in terms of Pu-concentrations in air and resuspension rates in a complementary investigation to those of CIEMAT but in an intensive short-term field effort. This study complements the resuspension studies of CIEMAT at Palomares with additional information, and with confirmation of their previous studies. Observed mass loadings (M) were an average of 70 mg/m{sup 3} with peaks in the daytime of 130 mg/m{sup 3} and low values at night below 30 {micro}g/m{sup 3}. The Pu-activity of aerosols (A) downwind of plot 2-1 was 0.12 Bq/g and the enhancement factor (E{sub f}) had a value of 0.3, which is low but similar to a typical value of 0.7 for other undisturbed sites. This E{sub f} value may increase further away from ground zero. The particle size distribution of the Pu in air measured by cascade impactors was approximately lognormal with a median aerodynamic diameter of 3.7 {micro}m and a geometric standard deviation of 3.5 in the respirable range. This peak midway between 1 ? m and 10 {micro}m in the respirable range is commonly observed. Daily fluctuations in the Pu concentration in air (C) detected by the UHV were lognormally distributed with a geometric standard deviation of 4.9 indicating that the 98th percentile would be 24 times as high as the median. Downwind of plot 2-1 the mean Pu concentration in air, C, was 8.5 {micro}Bq/m{sup 3}. The resuspension factor (Sf) was 2.4 x 10

  16. Formation and stability of metastable structures and amorphous phases in PU-V, PU-TA, and PU-YB systems with positive heats of mixing

    NASA Astrophysics Data System (ADS)

    Rizzo, H. F.; Zocco, T.; Massalski, T. B.; Nastasi, M.; Echeverria, A.

    1994-08-01

    The triode sputtering technique with a “split-target” arrangement was used to obtain metastable crystalline and amorphous phases in the Pu-V, Pu-Ta, and Pu-Yb systems. The proposed phase diagrams for these systems all exhibit liquid immiscibility. The heats of mixing are estimated to be highly positive, and the atomic radii of the component atoms differ by at least 10 pct. Extended amorphous and body-centered cubic (bcc) solid-solution regions were observed in the Pu-V and Pu-Ta systems. The corresponding lattice parameters appear to follow in each case an assumed Vegard’s Law extension. In the Pu-Yb system, no amorphous phase was obtained, but an extended face-centered cubic (fcc) solid-solution region (24 to 78 at. pct Yb) was observed with a large positive deviation of the lattice parameter (˜9 pct at 40 at. pct Yb) from a linear Vegard’s Law between the pure fcc components. The observed ranges of amorphous and metastable solid-solution phases have been interpreted in terms of predicated heats of formation for these phases using Miedema’s thermodynamic approximations that include chemical, elastic, and structural contributions. The effect of the high deposition rates on the formation of amorphous and metastable phases has also been considered. Thermal annealing of Pu-Ta amorphous alloys brings about a rapid diffusion of Pu to the free surface of the amorphous phase without crystallization of the remaining Ta-rich amorphous phase. Microhardness measurements indicate that amorphous Pu-V and Pu-Ta alloys are softer than the crystalline bcc solid-solution alloys in the same composition range. Several similarities in the formation of mixed phase regions (amorphous and solid solutions), microhardness, and resistance to decomposition on heating were noted between the Pu-Ta and Pu-V systems and the Cu-W system studied previously.

  17. Pu and Am determination in the environment—method development

    NASA Astrophysics Data System (ADS)

    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. Plutonium partitioning in uranium and plutonium co-recovery system for fast reactor fuel recycling with enhanced nuclear proliferation resistance

    SciTech Connect

    Nakahara, Masaumi; Koma, Yoshikazu; Nakajima, Yasuo

    2013-07-01

    For enhancement of nuclear proliferation resistance, a 'co-processing' method for U and Pu co-recovery was studied. Two concepts, no U scrubbing and no Pu reduction partitioning, were employed to formulate two types of flow sheets by using a calculation code. Their process performance was demonstrated using radioactive solutions derived from an irradiated fast reactor fuel. These experimental results indicated that U and Pu were co-recovered in the U/Pu product, and the Pu content in the U/Pu product increased approximately 2.3 times regardless of using reductant. The proposed no U scrubbing and no Pu reductant flow sheet is applicable to fast reactor fuel reprocessing and enhances its resistance to nuclear proliferation. (authors)

  19. PuPO4(cr, hyd.) Solubility Product and Pu3+ Complexes With Phosphate and Ethylenediaminetetraacetic Acid

    SciTech Connect

    Rai, Dhanpat; Moore, Dean A.; Felmy, Andrew R.; Rosso, Kevin M.; Bolton, Harvey

    2010-06-15

    To determine the solubility product of PuPO4(cr, hyd.) and the complexation constants of Pu(III) with phosphate and EDTA, the solubility of PuPO4(cr, hyd.) was investigated as a function of: 1) time and pH varying from 1.0 to 12.0 and at a fixed 0.00032 M phosphate concentration; 2) NaH2PO4 concentrations varying from 0.0001 M to 1.0 M and at a fixed pH value of 2.5; 3) time and pH varying from 1.3 to 13.0 at fixed concentrations of 0.00032 M phosphate and 0.0004 M or 0.002 M Na2H2EDTA; and 4) Na2H2EDTA concentrations varying from 0.00005 M to 0.0256 M at a fixed 0.00032 M phosphate concentration and at pH values of approximately 3.5, 10.6, and 12.6. A combination of solvent extraction and spectrophotometric techniques confirmed that the use of hydroquinone and Na2S2O4 helped maintain Pu as Pu(III). The solubility data were interpreted using Pitzer and SIT models, and both provided similar values for the solubility product of PuPO4(cr, hyd.) and for the formation constant of PuEDTA-. The log10 of the solubility product of PuPO4(cr, hyd.) (PuPO4(cr, hyd.) = Pu3+ + PO4 ) was determined to be –(24.42 ± 0.38). Pitzer modeling showed that phosphate interactions with Pu3+ were extremely weak and did not require any phosphate complexes (e.g., PuPO4(aq), PuH2PO42+, Pu(H2PO4)2+, Pu(H2PO4)3(aq), and Pu(H2PO4)4-), as proposed in existing literature, to explain the experimental data. SIT modeling, however, required the inclusion of PuH2PO42+ to explain the data in high NaH2PO4 concentrations; this illustrates the differences one can expect when using these two chemical models to interpret the data. As the Pu(III)-EDTA species, only PuEDTA- was needed to interpret the experimental data in a large range in pH values (1.3–12.9) and EDTA concentrations (0.00005–0.256 M). Calculations based on density functional theory support the existence of PuEDTA- (with prospective stoichiometry as Pu(OH2)3EDTA-) as the chemically and structurally stable species. The log10 of the

  20. Irradiation performance of full-length metallic IFR fuels

    SciTech Connect

    Tsai, H.; Neimark, L.A.

    1992-07-01

    An assembly irradiation of 169 full-length U-Pu-Zr metallic fuel pins was successfully completed in FFTF to a goal burnup of 10 at.%. All test fuel pins maintained their cladding integrity during the irradiation. Postirradiation examination showed minimal fuel/cladding mechanical interaction and excellent stability of the fuel column. Fission-gas release was normal and consistent with the existing data base from irradiation testing of shorter metallic fuel pins in EBR-II.

  1. ²³⁹Pu and ²⁴⁰Pu inventories and ²⁴⁰Pu/²³⁹Pu atom ratios in the equatorial Pacific Ocean water column.

    PubMed

    Yamada, Masatoshi; Zheng, Jian

    2012-07-15

    The (239+240)Pu concentrations and (240)Pu/(239)Pu atom ratios were determined by alpha spectrometry and inductively coupled plasma mass spectrometry for seawater samples from two stations, one at the equator and the other in the equatorial South Pacific. To better understand the fate of Pu isotopes, this study dealt with the contribution of the close-in fallout Pu from the Pacific Proving Grounds (PPG) in water columns of the Pacific Ocean. The (239)Pu, (240)Pu and (239+240)Pu inventories over the depth interval 0-3000 m at the equator station were 10.4, 8.9 and 19.3 Bq m(-2), respectively. Further, no noticeable difference was observed in (239)Pu, (240)Pu and (239+240)Pu inventories over the depth interval 0-3000 m between the two stations. The total (239+240)Pu inventories were significantly higher than the expected cumulative deposition density of global fallout. Water column (239+240)Pu inventories measured in this study were lower than those reported for comparable stations in the Geochemical Ocean Sections Study, indicating that these inventories have been decreasing at average rates of 0.89 ± 0.07 and 0.16 ± 0.07 Bq m(-2)yr(-1) at the equator and equatorial South Pacific stations, respectively, from 1973 to 1990. The obtained (240)Pu/(239)Pu atom ratios were higher than the mean global fallout ratio of 0.18. These high atom ratios proved the existence of close-in tropospheric fallout Pu from the PPG in the Marshall Islands. The (239+240)Pu inventories originating from the close-in fallout in the entire water column were estimated to be 11.1 Bq m(-2) at the equator station and 7.1 Bq m(-2) at the equatorial South Pacific Ocean station, and the relative percentages of close-in fallout Pu were 40% at the former and 34% at the latter. A significant amount of close-in fallout Pu originating from the PPG has been transported to deep layers below the 1000 m depth in the equatorial Pacific Ocean.

  2. FCRD Transmutation Fuels Handbook 2015

    SciTech Connect

    Janney, Dawn Elizabeth; Papesch, Cynthia Ann

    2015-09-01

    Transmutation of minor actinides such as Np, Am, and Cm in spent nuclear fuel is of international interest because of its potential for reducing the long-term health and safety hazards caused by the radioactivity of the spent fuel. One important approach to transmutation (currently being pursued by the DOE Fuel Cycle Research & Development Advanced Fuels Campaign) involves incorporating the minor actinides into U-Pu-Zr alloys, which can be used as fuel in fast reactors. It is, therefore, important to understand the properties of U-Pu-Zr alloys, both with and without minor actinide additions. In addition to requiring extensive safety precautions, alloys containing U and Pu are difficult to study for numerous reasons, including their complex phase transformations, characteristically sluggish phase-transformation kinetics, tendency to produce experimental results that vary depending on the histories of individual samples, and sensitivity to contaminants such as oxygen in concentrations below a hundred parts per million. Many of the experimental measurements were made before 1980, and the level of documentation for experimental methods and results varies widely. It is, therefore, not surprising that little is known with certainty about U-Pu-Zr alloys, and that general acceptance of results sometimes indicates that there is only a single measurement for a particular property. This handbook summarizes currently available information about U, Pu, Zr, and alloys of two or three of these elements. It contains information about phase diagrams and related information (including phases and phase transformations); heat capacity, entropy, and enthalpy; thermal expansion; and thermal conductivity and diffusivity. In addition to presenting information about materials properties, it attempts to provide information about how well the property is known and how much variation exists between measurements. Although the handbook includes some references to publications about modeling

  3. Nevada test site fallout atom ratios: /sup 240/Pu//sup 239/Pu and /sup 241/Pu//sup 239/Pu

    SciTech Connect

    Hicks, H.G.; Barr, D.W.

    1984-02-01

    The exposure of the population in Utah to external gamma radiation from the fallout from nuclear weapons tests carried out between 1951 and 1958 at the Nevada Test Site (NTS) has been reconstructed from recent measurements of /sup 137/Cs and plutonium in soil. The fraction of /sup 137/Cs in the fallout from NTS events was calculated from the total plutonium and the /sup 240/Pu//sup 239/Pu ratios measured in the soil, using the values of 0.180 +- 0.006 and 0.032 +- 0.003 for that ratio in global fallout and NTS fallout, respectively. The total population exposure from NTS events was then calculated on the basis of exposure rates resulting from short-lived radionuclides associated with the /sup 137/Cs at the time of deposition. While the /sup 240/Pu//sup 239/Pu ratio is constant in global fallout, this ratio varies greatly in the fallout from individual events. While the composition of fallout on Utah from NTS events is rather uniform, the Off-Site Radiation Exposure Review Project is currently reconstructing radiation exposures for locations close to NTS where the fallout may be predominantly from one event. Therefore, the authors compiled the pertinent ratios in order to provide information concerning the exposure resulting from any individual event. The plutonium ratios measured at 30 days postshot were compiled from unpublished values in the archives of the Nuclear Chemistry Division of LLNL and INC-11 of LANL. These ratios are pertinent to fallout data. Dates for each event were taken from a publication by the Nevada Operations Office of the Department of Energy. 3 references.

  4. Pu-content verification by calorimetry

    SciTech Connect

    Beets, C.; Carchon, R.; Fettweis, P.; Corbellini, M.; D'Adama, D.; Guardini, S.; Rodenburg, W.W.; Strohm, W.W.; Fiarman, S.; Keddar, A.

    1984-05-01

    The aim of this paper is to present calorimetric assay measurements that were performed on a set of high burnup plutonium samples using the Mound No. 150 twin resistance bridge calorimeter. The samples and the calorimeter are described in the first part of the paper and the experimental results are discussed in a second part. The isotopic composition, obtained by destructive analysis, was combined with the measured power values for the Pu-assay.

  5. Magnetic Properties of Radiation Damage in Pu

    SciTech Connect

    McCall, S; Fluss, M J; Chung, B W; McElfresh, M; Chapline, G; Jackson, D

    2004-10-27

    First, we review earlier studies reporting possible magnetic characteristics for radiation defects in Pu. We then report, for {alpha}-Pu, two studies of the excess magnetic susceptibility (EMS) due to radiation damage, as a function of time and temperature. We have observed several annealing stages associated with the EMS of the accumulated self-damage and we report that annealing begins at {approx}31K, while below that temperature the displacement damage from self-irradiation of the Pu alpha particle emission and the U recoil are immobile. A detailed investigation was made of this EMS well below the first annealing stage as a function of temperature (2K < T < 15K) and time in a magnetic field of 2T. A linear increase in magnetic susceptibility is seen as a function of time for all isotherms. The excess susceptibility per alpha decay, determined from a linear fit of the slope of the time dependent EMS, is reasonably described with a Curie-Weiss law exhibiting a small negative Weiss temperature. We conclude by describing some future experiments in light of the present results.

  6. Recent advances in the study of the UO2-PuO2 phase diagram at high temperatures

    NASA Astrophysics Data System (ADS)

    Böhler, R.; Welland, M. J.; Prieur, D.; Cakir, P.; Vitova, T.; Pruessmann, T.; Pidchenko, I.; Hennig, C.; Guéneau, C.; Konings, R. J. M.; Manara, D.

    2014-05-01

    Recently, novel container-less laser heating experimental data have been published on the melting behaviour of pure PuO2 and PuO2-rich compositions in the uranium dioxide-plutonium dioxide system. Such data showed that previous data obtained by more traditional furnace heating techniques were affected by extensive interaction between the sample and its containment. It is therefore paramount to check whether data so far used by nuclear engineers for the uranium-rich side of the pseudo-binary dioxide system can be confirmed or not. In the present work, new data are presented both in the UO2-rich part of the phase diagram, most interesting for the uranium-plutonium dioxide based nuclear fuel safety, and in the PuO2 side. The new results confirm earlier furnace heating data in the uranium-dioxide rich part of the phase diagram, and more recent laser-heating data in the plutonium-dioxide side of the system. As a consequence, it is also confirmed that a minimum melting point must exist in the UO2-PuO2 system, at a composition between x(PuO2) = 0.4 and x(PuO2) = 0.7 and 2900 K ⩽ T ⩽ 3000 K. Taking into account that, especially at high temperature, oxygen chemistry has an effect on the reported phase boundary uncertainties, the current results should be projected in the ternary U-Pu-O system. This aspect has been extensively studied here by X-ray diffraction and X-ray absorption spectroscopy. The current results suggest that uncertainty bands related to oxygen behaviour in the equilibria between condensed phases and gas should not significantly affect the qualitative trend of the current solid-liquid phase boundaries.

  7. 240Pu/239Pu isotopic ratios and 239 + 240Pu total measurements in surface and deep waters around Mururoa and Fangataufa atolls compared with Rangiroa atoll (French Polynesia).

    PubMed

    Chiappini, R; Pointurier, F; Millies-Lacroix, J C; Lepetit, G; Hemet, P

    1999-09-30

    The average values of 240Pu/239Pu mass isotopic ratios of plutonium deposited in Mururoa and Fangataufa atoll sediments by French atmospheric nuclear tests range from 3.5 to 5%. In order to assess the near field and far field influence of those deposits in the open ocean, two water profiles were measured for 239 + 240Pu and 240Pu/239Pu using, for the first time, an Inductively Coupled Plasma Mass Spectrometer which was developed to achieve femtogram detection limits. One site was located at the limit of the French territorial waters, which is 22 km distant from Mururoa. The second site was located close to Rangiroa atoll, at a distance of approximately 1200-km from French nuclear test sites. The sample volumes were approximately 500 litres and plutonium was purified prior to mass spectrometry and alpha spectrometry measurements. In Rangiroa, the 239 + 240Pu profile is comparable with those already determined in world open oceans but the maximum detected activity, 9 mBq/m3 at 500-600 m is a lot lower than those measured in the northern hemisphere. 240Pu/239Pu ratios were measured between 500 and 1000 m and were not statistically different from the typical 0.18 +/- 0.01 ratio which characterises the global fallout. Consequently, any influence of plutonium from the tests in Mururoa and Fangataufa is not apparent at Rangiroa. The vertical distribution of 239 + 240Pu near Mururoa shows similar changes with depth but with a slight increase in concentration. 240Pu/239Pu mass ratios vary with depth, from 7 to 10% in the upper 500 m and in the deep waters (below 1000 m) to 15-16% between 600 and 1000 m. A contribution from plutonium deposited in the sediments at Mururoa and Fangataufa is observed at the limit of territorial waters, especially in surface and deep waters.

  8. Optimization of hybrid-type instrumentation for Pu accountancy of U/TRU ingot in pyroprocessing.

    PubMed

    Seo, Hee; Won, Byung-Hee; Ahn, Seong-Kyu; Lee, Seung Kyu; Park, Se-Hwan; Park, Geun-Il; Menlove, Spencer H

    2016-02-01

    One of the final products of pyroprocessing for spent nuclear fuel recycling is a U/TRU ingot consisting of rare earth (RE), uranium (U), and transuranic (TRU) elements. The amounts of nuclear materials in a U/TRU ingot must be measured as precisely as possible in order to secure the safeguardability of a pyroprocessing facility, as it contains the most amount of Pu among spent nuclear fuels. In this paper, we propose a new nuclear material accountancy method for measurement of Pu mass in a U/TRU ingot. This is a hybrid system combining two techniques, based on measurement of neutrons from both (1) fast- and (2) thermal-neutron-induced fission events. In technique #1, the change in the average neutron energy is a signature that is determined using the so-called ring ratio method, according to which two detector rings are positioned close to and far from the sample, respectively, to measure the increase of the average neutron energy due to the increased number of fast-neutron-induced fission events and, in turn, the Pu mass in the ingot. We call this technique, fast-neutron energy multiplication (FNEM). In technique #2, which is well known as Passive Neutron Albedo Reactivity (PNAR), a neutron population's changes resulting from thermal-neutron-induced fission events due to the presence or absence of a cadmium (Cd) liner in the sample's cavity wall, and reflected in the Cd ratio, is the signature that is measured. In the present study, it was considered that the use of a hybrid, FNEM×PNAR technique would significantly enhance the signature of a Pu mass. Therefore, the performance of such a system was investigated for different detector parameters in order to determine the optimal geometry. The performance was additionally evaluated by MCNP6 Monte Carlo simulations for different U/TRU compositions reflecting different burnups (BU), initial enrichments (IE), and cooling times (CT) to estimate its performance in real situations.

  9. Optimization of burnable poison design for Pu incineration in fully fertile free PWR core

    SciTech Connect

    Fridman, E.; Shwageraus, E.; Galperin, A.

    2006-07-01

    The design challenges of the fertile-free based fuel (FFF) can be addressed by careful and elaborate use of burnable poisons (BP). Practical fully FFF core design for PWR reactor has been reported in the past [1]. However, the burnable poison option used in the design resulted in significant end of cycle reactivity penalty due to incomplete BP depletion. Consequently, excessive Pu loading were required to maintain the target fuel cycle length, which in turn decreased the Pu burning efficiency. A systematic evaluation of commercially available BP materials in all configurations currently used in PWRs is the main objective of this work. The BP materials considered are Boron, Gd, Er, and Hf. The BP geometries were based on Wet Annular Burnable Absorber (WABA), Integral Fuel Burnable Absorber (IFBA), and Homogeneous poison/fuel mixtures. Several most promising combinations of BP designs were selected for the full core 3D simulation. All major core performance parameters for the analyzed cases are very close to those of a standard PWR with conventional UO{sub 2} fuel including possibility of reactivity control, power peaking factors, and cycle length. The MTC of all FFF cores was found at the full power conditions at all times and very close to that of the UO{sub 2} core. The Doppler coefficient of the FFF cores is also negative but somewhat lower in magnitude compared to UO{sub 2} core. The soluble boron worth of the FFF cores was calculated to be lower than that of the UO{sub 2} core by about a factor of two, which still allows the core reactivity control with acceptable soluble boron concentrations. The main conclusion of this work is that judicial application of burnable poisons for fertile free fuel has a potential to produce a core design with performance characteristics close to those of the reference PWR core with conventional UO{sub 2} fuel. (authors)

  10. X-ray excited Auger transitions of Pu compounds

    SciTech Connect

    Nelson, Art J. Grant, William K.; Stanford, Jeff A.; Siekhaus, Wigbert J.; Allen, Patrick G.; McLean, William

    2015-05-15

    X-ray excited Pu core–valence–valence and core–core–valence Auger line-shapes were used in combination with the Pu 4f photoelectron peaks to characterize differences in the oxidation state and local electronic structure for Pu compounds. The evolution of the Pu 4f core-level chemical shift as a function of sputtering depth profiling and hydrogen exposure at ambient temperature was quantified. The combination of the core–valence–valence Auger peak energies with the associated chemical shift of the Pu 4f photoelectron line defines the Auger parameter and results in a reliable method for definitively determining oxidation states independent of binding energy calibration. Results show that PuO{sub 2}, Pu{sub 2}O{sub 3}, PuH{sub 2.7}, and Pu have definitive Auger line-shapes. These data were used to produce a chemical state (Wagner) plot for select plutonium oxides. This Wagner plot allowed us to distinguish between the trivalent hydride and the trivalent oxide, which cannot be differentiated by the Pu 4f binding energy alone.

  11. Comparative Analysis on Nuclear Fuel Sustainability Aspect of FBR

    NASA Astrophysics Data System (ADS)

    Permana, Sidik; Irwanto, Dwi; Suzuki, Mitsutoshi; Saito, Masaki

    2017-01-01

    Recycle program of spent nuclear fuel (SNF) will have some challanges in term of fuel cycle capability and its facilities as well as nuclear non-proliferation concern of special nuclear materials. A different analysis approach as a comparative study have been analyzed based on breeding ratio and heavy metal inventory ratio concepts in fast breeder reactor (FBR) type. Breeding ratio and heavy metal inventory obtain higher than unity which shows breeding gain or surplus inventory of heavy metals are obtained. Breeding ratio indicates the fuel conversion capability from conversion process of fertile materials into fissile material such as fertile materials of U-238, Pu-238, Pu-240 and fissile materials of Pu-239 and Pu-241. Inventory ratio approaches are appropriate to estimate some selected actinide as a mass inventory production such as plutonium inventory ratio which estimate the surplus mass inventory from the ratio of produced plutonium at the net of operation to the initial inventory ratio.

  12. Sintering of compacts of UN, (U,Pu)N, and PuN

    DOEpatents

    Tennery, V.J.; Godfrey, T.G.; Bomar, E.S.

    1973-10-16

    >A method is provided for preparing a densified compact of a metal nitride selected from the group consisting of UN, (U,Pu)N, and PuN which comprises heating a green compact of at least one selected nitride in the mononitride single-phase region, as displayed by a phase diagram of the mononitride of said compact, in a nitrogen atmosphere at a pressure of nitrogen less than 760 torr. At a given temperature, this process produces a singlephase structure and a maximal sintered density as measured by mercury displacement. (Official Gazette)

  13. FEASIBILITY OF RECYCLING PLUTONIUM AND MINOR ACTINIDES IN LIGHT WATER REACTORS USING HYDRIDE FUEL

    SciTech Connect

    Greenspan, Ehud; Todreas, Neil; Taiwo, Temitope

    2009-03-10

    The objective of this DOE NERI program sponsored project was to assess the feasibility of improving the plutonium (Pu) and minor actinide (MA) recycling capabilities of pressurized water reactors (PWRs) by using hydride instead of oxide fuels. There are four general parts to this assessment: 1) Identifying promising hydride fuel assembly designs for recycling Pu and MAs in PWRs 2) Performing a comprehensive systems analysis that compares the fuel cycle characteristics of Pu and MA recycling in PWRs using the promising hydride fuel assembly designs identified in Part 1 versus using oxide fuel assembly designs 3) Conducting a safety analysis to assess the likelihood of licensing hydride fuel assembly designs 4) Assessing the compatibility of hydride fuel with cladding materials and water under typical PWR operating conditions Hydride fuel was found to offer promising transmutation characteristics and is recommended for further examination as a possible preferred option for recycling plutonium in PWRs.

  14. Iron Corrosion Observations: Pu(VI)-Fe Reduction Studies

    SciTech Connect

    Reed, Donald T.; Swanson, Juliet S.; Richmann, Michael K.; Lucchini, Jean-Francois; Borkowski, Marian

    2012-09-11

    Iron and Pu Reduction: (1) Very different appearances in iron reaction products were noted depending on pH, brine and initial iron phase; (2) Plutonium was associated with the Fe phases; (3) Green rust was often noted at the higher pH; (4) XANES established the green rust to be an Fe2/3 phase with a bromide center; and (5) This green rust phase was linked to Pu as Pu(IV).

  15. The optimization of an AP1000 fuel assembly for the transmutation of plutonium and minor actinides

    NASA Astrophysics Data System (ADS)

    Washington, Jeremy A.

    The average nuclear power plant produces twenty metric tons of used nuclear fuel per year, containing approximately 95 wt% uranium, 1 wt% plutonium, and 4 wt% fission products and transuranic elements. Fast reactors are a preferred option for the transmutation of plutonium and minor actinides; however, an optimistic deployment time of at least 20 years indicates a need for a near-term solution. The goal of this thesis is to examine the potential of light water reactors for plutonium and minor actinides transmutation as a near-term solution. This thesis screens the available nuclear isotope database to identify potential absorbers as coatings on a transmutation fuel in a light water reactor. A spectral shift absorber coating tunes the neutron energy spectrum experienced by the underlying target fuel. Eleven different spectral shift absorbers (B4C, CdO, Dy2O3, Er 2O3, Eu2O3, Gd2O3, HfO2, In2O3, Lu2O3, Sm2O3, and TaC) have been selected for further evaluation. A model developed using the NEWT module of SCALE 6.1 code provided performance data for the burnup of the target fuel rods. Irradiation of the target fuels occurs in a Westinghouse 17x17 XL Robust Fuel Assembly over a 1400 Effective Full Power Days (EFPD) interval. The fuels evaluated in this thesis include PuO2, Pu3Si2, PuN, MOX, PuZrH, PuZrHTh, PuZrO 2, and PuUZrH. MOX (5 wt% PuO2), Pu0.31ZrH 1.6Th1.08, and PuZrO2MgO (8 wt%) are selected for detailed analysis in a multi-pin transmutation assembly. A coupled model optimized the resulting transmutation fuel elements. The optimization considered three stages of fuel assemblies containing target fuel pins. The first stage optimized four target fuel pins adjacent to the central instrumentation channel. The second stage evaluated a variety of assemblies with multiple target fuel pins and the third stage re-optimized target fuel pins in the second-stage assembly. A PuZrO2MgO (8 wt%) target fuel with a coating of Lu 2O3 resulted in the greatest reduction in curium-244

  16. Effect of equilibration time on Pu desorption from goethite

    SciTech Connect

    Wong, Jennifer C.; Zavarin, Mavrik; Begg, James D.; Kersting, Annie B.; Powell, Brian A.

    2015-01-28

    Strongly sorbing ions such as plutonium may become irreversibly bound to mineral surfaces over time implicates near- and far-field transport of Pu. Batch adsorption–desorption data were collected as a function of time and pH to study the surface stability of Pu on goethite. Pu(IV) was adsorbed to goethite over the pH range 4.2 to 6.6 for different periods of time (1, 6, 15, 34 and 116 d). Moreover, following adsorption, Pu was leached from the mineral surface with desferrioxamine B (DFOB), a complexant capable of effectively competing with the goethite surface for Pu. The amount of Pu desorbed from the goethite was found to vary as a function of the adsorption equilibration time, with less Pu removed from the goethite following longer adsorption periods. This effect was most pronounced at low pH. Logarithmic desorption distribution ratios for each adsorption equilibration time were fit to a pH-dependent model. Model slopes decreased between 1 and 116 d adsorption time, indicating that overall Pu(IV) surface stability on goethite surfaces becomes less dependent on pH with greater adsorption equilibration time. The combination of adsorption and desorption kinetic data suggest that non-redox aging processes affect Pu sorption behavior on goethite.

  17. Effect of equilibration time on Pu desorption from goethite

    DOE PAGES

    Wong, Jennifer C.; Zavarin, Mavrik; Begg, James D.; ...

    2015-01-28

    Strongly sorbing ions such as plutonium may become irreversibly bound to mineral surfaces over time implicates near- and far-field transport of Pu. Batch adsorption–desorption data were collected as a function of time and pH to study the surface stability of Pu on goethite. Pu(IV) was adsorbed to goethite over the pH range 4.2 to 6.6 for different periods of time (1, 6, 15, 34 and 116 d). Moreover, following adsorption, Pu was leached from the mineral surface with desferrioxamine B (DFOB), a complexant capable of effectively competing with the goethite surface for Pu. The amount of Pu desorbed from the goethitemore » was found to vary as a function of the adsorption equilibration time, with less Pu removed from the goethite following longer adsorption periods. This effect was most pronounced at low pH. Logarithmic desorption distribution ratios for each adsorption equilibration time were fit to a pH-dependent model. Model slopes decreased between 1 and 116 d adsorption time, indicating that overall Pu(IV) surface stability on goethite surfaces becomes less dependent on pH with greater adsorption equilibration time. The combination of adsorption and desorption kinetic data suggest that non-redox aging processes affect Pu sorption behavior on goethite.« less

  18. Size and density of a /sup 242/Pu colloid

    SciTech Connect

    Rundberg, R.S.; Mitchell, A.J.; Torstenfelt, N.B.

    1987-01-01

    The size and density of a /sup 242/Pu colloid has been measured by autocorrelation photon spectrometry. The density of the colloid was determined by ultraspeed centrifugation. From the concentration profiles of /sup 242/Pu in the centrifuged test tubes, a standard sedimentation formula was used to calculate the density; the size of the colloid was known from the light scattering experiments. The determined density of the /sup 242/Pu colloid was unexpectedly low compared to the density of crystalline PuO/sub 2/. 5 refs., 1 tab.

  19. Neutron Capture Cross Section of 239Pu

    NASA Astrophysics Data System (ADS)

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

    2014-05-01

    The Detector for Advanced Neutron Capture Experiments (DANCE) has been used to measure the 239Pu(n,γ) cross section from 10 eV to the keV region. Three experimental run conditions were used to characterize the prompt fission γ-ray spectrum across the entire energy regime, measure the cross section in the resolved resonance region, and obtain necessary count rate well into the keV region. The preliminary cross sections are in good agreement with current evaluations from 10 eV to 80 keV.

  20. Statistical properties of Pu243 , and Pu242(n,γ) cross section calculation

    DOE PAGES

    Laplace, T. A.; Zeiser, F.; Guttormsen, M.; ...

    2016-01-29

    The level density and γ-ray strength function (γSF) of 243Pu have been measured in the quasicontinuum using the Oslo method. Excited states in 243Pu were populated using the 242Pu(d,p) reaction. The level density closely follows the constant-temperature level density formula for excitation energies above the pairing gap. The γSF displays a double-humped resonance at low energy as also seen in previous investigations of actinide isotopes. The structure is interpreted as the scissors resonance and has a centroid of ωSR = 2.42(5) MeV and a total strength of BSR = 10.1(15) μ2N, which is in excellent agreement with sum-rule estimates. Lastly,more » the measured level density and γSF were used to calculate the 242Pu(n,γ) cross section in a neutron energy range for which there were previously no measured data.« less

  1. Simulation of radiation driven fission gas diffusion in UO2, ThO2 and PuO2

    NASA Astrophysics Data System (ADS)

    Cooper, M. W. D.; Stanek, C. R.; Turnbull, J. A.; Uberuaga, B. P.; Andersson, D. A.

    2016-12-01

    Below 1000 K it is thought that fission gas diffusion in nuclear fuel during irradiation occurs through atomic mixing due to radiation damage. Here we present a molecular dynamics (MD) study of Xe, Kr, Th, U, Pu and O diffusion due to irradiation. It is concluded that the ballistic phase does not sufficiently account for the experimentally observed diffusion. Thermal spike simulations are used to confirm that electronic stopping remedies the discrepancy with experiment and the predicted diffusivities lie within the scatter of the experimental data. Our results predict that the diffusion coefficients are ordered such that DO* > DKr* > DXe* > DU*. For all species >98.5% of diffusivity is accounted for by electronic stopping. Fission gas diffusivity was not predicted to vary significantly between ThO2, UO2 and PuO2, indicating that this process would not change greatly for mixed oxide fuels.

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

    SciTech Connect

    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.

  3. DOE plutonium disposition study: Pu consumption in ALWRs. Volume 2, Final report

    SciTech Connect

    Not Available

    1993-05-15

    The Department of Energy (DOE) has contracted with Asea Brown Boveri-Combustion Engineering (ABB-CE) to provide information on the capability of ABB-CE`s System 80 + Advanced Light Water Reactor (ALWR) to transform, through reactor burnup, 100 metric tonnes (MT) of weapons grade plutonium (Pu) into a form which is not readily useable in weapons. This information is being developed as part of DOE`s Plutonium Disposition Study, initiated by DOE in response to Congressional action. This document Volume 2, provides a discussion of: Plutonium Fuel Cycle; Technology Needs; Regulatory Considerations; Cost and Schedule Estimates; and Deployment Strategy.

  4. On the multi-reference nature of plutonium oxides: PuO22+, PuO2, PuO3 and PuO2(OH)2

    NASA Astrophysics Data System (ADS)

    Boguslawski, Katharina; Réal, Florent; Tecmer, Paweł; Duperrouzel, Corinne; Gomes, André Severo Pereira; Legeza, Örs; Ayers, Paul W.; Vallet, Valérie

    Actinide-containing complexes present formidable challenges for electronic structure methods due to the large number of degenerate or quasi-degenerate electronic states arising from partially occupied 5f and 6d shells. Conventional multi-reference methods can treat active spaces that are often at the upper limit of what is required for a proper treatment of species with complex electronic structures, leaving no room for verifying their suitability. In this work we address the issue of properly defining the active spaces in such calculations, and introduce a protocol to determine optimal active spaces based on the use of the Density Matrix Renormalization Group algorithm and concepts of quantum information theory. We apply the protocol to elucidate the electronic structure and bonding mechanism of volatile plutonium oxides (PuO$_3$ and PuO$_2$(OH)$_2$), species associated with nuclear safety issues for which little is known about the electronic structure and energetics. We show how, within a scalar relativistic framework, orbital-pair correlations can be used to guide the definition of optimal active spaces which provide an accurate description of static/non-dynamic electron correlation, as well as to analyse the chemical bonding beyond a simple orbital model. From this bonding analysis we are able to show that the addition of oxo- or hydroxo-groups to the plutonium dioxide species considerably changes the pi-bonding mechanism with respect to the bare triatomics, resulting in bent structures with considerable multi-reference character.

  5. 239Pu Prompt Fission Neutron Spectra Impact on a Set of Criticality and Experimental Reactor Benchmarks

    NASA Astrophysics Data System (ADS)

    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

  6. Fuel flexible fuel injector

    DOEpatents

    Tuthill, Richard S; Davis, Dustin W; Dai, Zhongtao

    2015-02-03

    A disclosed fuel injector provides mixing of fuel with airflow by surrounding a swirled fuel flow with first and second swirled airflows that ensures mixing prior to or upon entering the combustion chamber. Fuel tubes produce a central fuel flow along with a central airflow through a plurality of openings to generate the high velocity fuel/air mixture along the axis of the fuel injector in addition to the swirled fuel/air mixture.

  7. Incorporation of excess weapons material into the IFR fuel cycle

    SciTech Connect

    Hannum, W.H.; Wade, D.C.

    1993-09-01

    The Integral Fast Reactor (IFR) provides both a diversion resistant closed fuel cycle for commercial power generation and a means of addressing safeguards concerns related to excess nuclear weapons material. Little head-end processing and handling of dismantled warhead materials is required to convert excess weapons plutonium (Pu) to IFR fuel and a modest degree of proliferation protection is available immediately by alloying weapons Pu to an IFR fuel composition. Denaturing similar to that of spent fuel is obtained by short cycle (e.g. 45 day) use in an IFR reactor, by mixing which IFR recycle fuel, or by alloying with other spent fuel constituents. Any of these permanent denaturings could be implemented as soon as an operating IFR and/or an IFR recycle capability of reasonable scale is available. The initial Pu charge generated from weapons excess Pu can then be used as a permanent denatured catalyst, enabling the IFR to efficiently and economically generate power with only a natural or depleted uranium feed. The Pu is thereafter permanently safeguarded until consumed, with essentially none going to a waste repository.

  8. Further evaluations of the toxicity of irradiated advanced heavy water reactor fuels.

    PubMed

    Edwards, Geoffrey W R; Priest, Nicholas D

    2014-11-01

    The neutron economy and online refueling capability of heavy water moderated reactors enable them to use many different fuel types, such as low enriched uranium, plutonium mixed with uranium, or plutonium and/or U mixed with thorium, in addition to their traditional natural uranium fuel. However, the toxicity and radiological protection methods for fuels other than natural uranium are not well established. A previous paper by the current authors compared the composition and toxicity of irradiated natural uranium to that of three potential advanced heavy water fuels not containing plutonium, and this work uses the same method to compare irradiated natural uranium to three other fuels that do contain plutonium in their initial composition. All three of the new fuels are assumed to incorporate plutonium isotopes characteristic of those that would be recovered from light water reactor fuel via reprocessing. The first fuel investigated is a homogeneous thorium-plutonium fuel designed for a once-through fuel cycle without reprocessing. The second fuel is a heterogeneous thorium-plutonium-U bundle, with graded enrichments of U in different parts of a single fuel assembly. This fuel is assumed to be part of a recycling scenario in which U from previously irradiated fuel is recovered. The third fuel is one in which plutonium and Am are mixed with natural uranium. Each of these fuels, because of the presence of plutonium in the initial composition, is determined to be considerably more radiotoxic than is standard natural uranium. Canadian nuclear safety regulations require that techniques be available for the measurement of 1 mSv of committed effective dose after exposure to irradiated fuel. For natural uranium fuel, the isotope Pu is a significant contributor to the committed effective dose after exposure, and thermal ionization mass spectrometry is sensitive enough that the amount of Pu excreted in urine is sufficient to estimate internal doses, from all isotopes, as low

  9. A comparative study of nitride purity and Am fabrication losses in PuN materials by the powder and internal gelation production routes

    NASA Astrophysics Data System (ADS)

    Hedberg, Marcus; Ekberg, Christian

    2016-12-01

    Fabrication of plutonium containing fuels through the internal gelation method has mostly been studied in mixed metal systems such as U, Pu or Zr,Pu. In this work production of undiluted PuN has been performed by carbothermal reduction on both oxide powder and Pu microspheres produced by the internal gelation method. Nitride purities reached using the different methods have been studied together with final densities achieved during pellet fabrication as well as losses of ingrown Am during the different production steps. Formation of Pu microspheres was successfully performed using the internal gelation method, although extensive microsphere fracturing occurred during thermal treatment. Final densities of PuN pellets produced by cold pressing and sintering reached 70-80% of theoretical density. Am losses during the carbothermal reduction step was on average about 3.7%. After sintering about 11% of Am was lost in total through the entire production process if sintering in N2 + 5% H2 atmosphere while about 50% of the Am in total was lost when using Ar as sintering atmosphere.

  10. Isotopic Pu, Am and Cm signatures in environmental samples contaminated by the Fukushima Dai-ichi Nuclear Power Plant accident.

    PubMed

    Yamamoto, M; Sakaguchi, A; Ochiai, S; Takada, T; Hamataka, K; Murakami, T; Nagao, S

    2014-06-01

    Dust samples from the sides of roads (black substances) have been collected together with litter and soil samples at more than 100 sites contaminated heavily in the 20-km exclusion zones around Fukushima Dai-ichi Nuclear Power Plant (FDNPP) (Minamisoma City, and Namie, Futaba and Okuma Towns), in Iitate Village located from 25 to 45 km northwest of the plant and in southern areas from the plant. Isotopes of Pu, Am and Cm have been measured in the samples to evaluate their total releases into the environment from the FDNPP and to get the isotopic compositions among these nuclides. For black substances and litter samples, in addition to Pu isotopes, (241)Am, (242)Cm and (243,244)Cm were determined for most of samples examined, while for soil samples, only Pu isotopes were determined. The results provided a coherent data set on (239,240)Pu inventories and isotopic composition among these transuranic nuclides. When these activity ratios were compared with those for fuel core inventories in the FDNPP accident estimated by a group at JAEA, except (239,240)Pu/(137)Cs activity ratios, fairly good agreements were found, indicating that transuranic nuclides, probably in the forms of fine particles, were released into the environment without their large fractionations. The obtained data may lead to more accurate information about the on-site situation (e.g., burn-up, conditions of fuel during the release phase, etc.), which would be difficult to get otherwise, and more detailed information on the dispersion and deposition processes of transuranic nuclides and the behavior of these nuclides in the environment.

  11. Ostwald Ripening and Its Effect on PuO2 Particle Size in Hanford Tank Waste

    SciTech Connect

    Delegard, Calvin H.

    2011-09-29

    Between 1944 and 1989, the Hanford Site produced 60 percent (54.5 metric tons) of the United States weapons plutonium and produced an additional 12.9 metric tons of fuels-grade plutonium. High activity wastes, including plutonium lost from the separations processes used to isolate the plutonium, were discharged to underground storage tanks during these operations. Plutonium in the Hanford tank farms is estimated to be {approx}700 kg but may be up to {approx}1000 kg. Despite these apparent large quantities, the average plutonium concentration in the {approx}200 million liter tank waste volume is only about 0.003 grams per liter ({approx}0.0002 wt%). The plutonium is largely associated with low solubility metal hydroxide/oxide sludges where its low concentration and intimate mixture with neutron-absorbing elements (e.g., iron) are credited in nuclear criticality safety. However, concerns have been expressed that plutonium, in the form of plutonium hydrous oxide, PuO{sub 2} {center_dot} xH{sub 2}O, could undergo sufficient crystal growth through Ostwald ripening in the alkaline tank waste to potentially be separable from neutron absorbing constituents by settling or sedimentation. It was found that plutonium that entered the alkaline tank waste by precipitation through neutralization from acid solution is initially present as 2- to 3-nm (0.002- to 0.003-{mu}m) scale PuO{sub 2} {center_dot} xH{sub 2}O crystallite particles and grows from that point at exceedingly slow rates, posing no risk to physical segregation. These conclusions are reached by both general considerations of Ostwald ripening and specific observations of the behaviors of PuO{sub 2} and PuO{sub 2} {center_dot} xH{sub 2}O upon aging in alkaline solution.

  12. Ab Initio Enhanced calphad Modeling of Actinide-Rich Nuclear Fuels

    SciTech Connect

    Morgan, Dane; Yang, Yong Austin

    2013-10-28

    The process of fuel recycling is central to the Advanced Fuel Cycle Initiative (AFCI), where plutonium and the minor actinides (MA) Am, Np, and Cm are extracted from spent fuel and fabricated into new fuel for a fast reactor. Metallic alloys of U-Pu-Zr-MA are leading candidates for fast reactor fuels and are the current basis for fast spectrum metal fuels in a fully recycled closed fuel cycle. Safe and optimal use of these fuels will require knowledge of their multicomponent phase stability and thermodynamics (Gibbs free energies). In additional to their use as nuclear fuels, U-Pu-Zr-MA contain elements and alloy phases that pose fundamental questions about electronic structure and energetics at the forefront of modern many-body electron theory. This project will validate state-of-the-art electronic structure approaches for these alloys and use the resulting energetics to model U-Pu-Zr-MA phase stability. In order to keep the work scope practical, researchers will focus on only U-Pu-Zr-{Np,Am}, leaving Cm for later study. The overall objectives of this project are to: Provide a thermodynamic model for U-Pu-Zr-MA for improving and controlling reactor fuels; and, Develop and validate an ab initio approach for predicting actinide alloy energetics for thermodynamic modeling.

  13. Procedure for plutonium determination using Pu(VI) spectra

    SciTech Connect

    Walker, L.F.; Temer, D.J.; Jackson, D.D.

    1996-09-01

    This document describes a simple spectrophotometric method for determining total plutonium in nitric acid solutions based on the spectrum of Pu(VI). Plutonium samples in nitric acid are oxidized to Pu(VI) with Ce(IV) and the net absorbance at the 830 nm peak is measured.

  14. Global distribution of Pu isotopes and 237Np.

    PubMed

    Kelley, J M; Bond, L A; Beasley, T M

    1999-09-30

    Inventories and compositions of Pu isotopes and 237Np in archived soil samples collected in the 1970s from 54 locations around the world were determined to provide regional baselines for recognizing possible future environmental inputs of non-fallout Pu and Np. As sample sizes used in this work were small (typically 1 g), inhomogeneities in Pu and Np concentrations were easily recognizable and, as a result, we were able to determine that atypical debris in South America, from French testing in the South Pacific, is more widely and uniformly distributed than previously supposed. From our results we conclude that fallout 237Np/239Pu atom ratios are generally lower in the Southern Hemisphere (approximately 0.35) than in the Northern Hemisphere (approximately 0.47.) Moreover, 237Np/239Pu atom ratios are more device-dependent, hence more variable, than counterpart 240Pu/239Pu atom ratios. Given predictable trends caused by sample inhomogeneities, with only two exceptions, the Pu results of this work are entirely consistent with (and in several instances improve on) results previously reported for these same samples. However, unlike earlier interpretations used to explain these results, we recommend that fallout isotopic signatures be represented by mixing lines, rather than averages, to better reflect regional variations of stratospheric fallout inventories relative to tropospheric fallout inventories, and provide the theoretical basis for doing so. Finally, the Np results of this work constitute one of the largest single compilations of such data reported to date.

  15. Synchrotron-Radiation-based Investigationsof the Electronic Structure of Pu

    SciTech Connect

    Tobin, J; Chung, B; Terry, J; Schulze, R; Farr, J; Heinzelman, K; Rotenberg, E; Shuh, D

    2004-09-27

    Synchrotron radiation from the Advanced Light Source has been used to investigate the electronic structure of {alpha}-Pu and {delta}-Pu. Measurements include core level and valence band photoelectron spectroscopy, Resonant Photoelectron Spectroscopy (REPES), and X-ray Absorption Spectroscopy (XAS).

  16. PU.1 silencing leads to terminal differentiation of erythroleukemia cells

    SciTech Connect

    Atar, Orna; Levi, Ben-Zion . E-mail: blevi@technion.ac.il

    2005-04-22

    The transcription factor PU.1 plays a central role in development and differentiation of hematopoietic cells. Evidence from PU.1 knockout mice indicates a pivotal role for PU.1 in myeloid lineage and B-lymphocyte development. In addition, PU.1 is a key player in the development of Friend erythroleukemia disease, which is characterized by proliferation and differentiation arrest of proerythrocytes. To study the role of PU.1 in erythroleukemia, we have used murine erythroleukemia cells, isolated from Friend virus-infected mice. Expression of PU.1 small interfering RNA in these cells led to significant inhibition of PU.1 levels. This was accompanied by inhibition of proliferation and restoration in the ability of the proerythroblastic cells to produce hemoglobin, i.e., reversion of the leukemic phenotype. The data suggest that overexpression of PU.1 gene is the immediate cause for maintaining the leukemic phenotype of the disease by retaining the self-renewal capacity of transformed erythroblastic cells and by blocking the terminal differentiation program towards erythrocytes.

  17. Resolving global versus local/regional Pu sources in the environment using sector ICP-MS

    USGS Publications Warehouse

    Ketterer, M.E.; Hafer, K.M.; Link, C.L.; Kolwaite, D.; Wilson, Jim; Mietelski, J.W.

    2004-01-01

    Sector inductively coupled plasma mass spectrometry is a versatile method for the determination of plutonium activities and isotopic compositions in samples containing this element at fallout levels. Typical detection limits for 239+240Pu are 0.1, 0.02 and 0.002 Bq kg -1Pu for samples sizes of 0.5 g, 3 g, and 50 g of soil, respectively. The application of sector ICP-MS-based Pu determinations is demonstrated in studies in sediment chronology, soil Pu inventory and depth distribution, and the provenance of global fallout versus local or regional Pu sources. A sediment core collected from Sloans Lake (Denver, Colorado, USA) exhibits very similar 137Cs and 239+240Pu activity profiles; 240Pu/239Pu atom ratios indicate possible small influences from the Nevada Test Site and/or the Rocky Flats Environmental Technology Site. An undisturbed soil profile from Lockett Meadow (Flagstaff, Arizona, USA) exhibits an exponential decrease in 239+240Pu activity versus depth; 240Pu/239Pu in the top 3 cm is slightly lower than the global fallout range of 0.180 ?? 0.014 due to possible regional influence of Nevada Test Site fallout. The 239??240Pu inventory at Lockett Meadow is 56 ?? 4 Bq m-2, consistent with Northern Hemisphere mid-latitude fallout. Archived NdF3 sources, prepared from Polish soils, demonstrate that substantial 239+240Pu from the 1986 Chernobyl disaster has been deposited in north eastern regions of Poland; compared to global fallout, Chernobyl Pu exhibits higher abundances of 240Pu and 241Pu. The ratios 240Pu/239pu and 241Pu/239Pu co-vary and range from 0.186-0.348 and 0.0029-0.0412, respectively, in forest soils (241Pu/239Pu = 0.2407??[240Pu/239Pu] - 0.0413; r2 = 0.9924). ?? The Royal Society of Chemistry 2004.

  18. Fission xenon from extinct Pu-244 in 14,301.

    NASA Technical Reports Server (NTRS)

    Drozd, R.; Hohenberg, C. M.; Ragan, D.

    1972-01-01

    Xenon extracted in step-wise heating of lunar breccia 14,301 contains a fission-like component in excess of that attributable to uranium decay during the age of the solar system. There seems to be no adequate source for this component other than Pu-244. Verification that this component is in fact due to the spontaneous fission of extinct Pu-244 comes from the derived spectrum which is similar to that observed from artificially produced Pu-244. It thus appears that Pu-244 was extant at the time lunar crustal material cooled sufficiently to arrest the thermal diffusion of xenon. Subsequent history has apparently maintained the isotopic integrity of plutonium fission xenon. Of major importance are details of the storage itself. Either the fission component is the result of in situ fission of Pu-244 and subsequent storage in 14,301 material, or the fission xenon was stored in an intermediate reservoir before incorporation into 14,301.

  19. Sputtering yield of Pu bombarded by fission Fragments from Cf

    SciTech Connect

    Danagoulian, Areg; Klein, Andreas; Mcneil, Wendy V; Yuan, Vincent W

    2008-01-01

    We present results on the yield of sputtering of Pu atoms from a Pu foil, bombarded by fission fragments from a {sup 252}Cf source in transmission geometry. We have found the number of Pu atoms/incoming fission fragments ejected to be 63 {+-} 1. In addition, we show measurements of the sputtering yield as a function of distance from the central axis, which can be understood as an angular distribution of the yield. The results are quite surprising in light of the fact that the Pu foil is several times the thickness of the range of fission fragment particles in Pu. This indicates that models like the binary collision model are not sufficient to explain this behavior.

  20. Laboratory studies of actinide partitioning relevant to 244Pu chronometry

    NASA Technical Reports Server (NTRS)

    Benjamin, T.; Heuser, W. R.; Burnett, D. S.

    1978-01-01

    Actinide partitioning and light lanthanide fractionation have been studied to gain an understanding of Pu chemistry under meteoritic and lunar conditions. The goal of the study was to identify conditions and samples from which chronological information can be retrieved. The laboratory investigations involved particle track radiography of the crystal/liquid partitioning of Th, U and Pu among diopsidic clinopyroxene, whitlockite and liquid. It is found that trivalent Pu plays an important role in partitioning for lunar and most meteoritic conditions. The use of Pu/Nd for relative age assessments is supported to some extent by the investigations; samples with unfractionated U, Th and Nd abundances (relative to average solar system values) may be suitable for Pu chronometry.

  1. Impact of Fission Products Impurity on the Plutonium Content of Metal- and Oxide- Fuels in Sodium Cooled Fast Reactors

    SciTech Connect

    Hikaru Hiruta; Gilles Youinou

    2013-09-01

    This short report presents the neutronic analysis to evaluate the impact of fission product impurity on the Pu content of Sodium-cooled Fast Reactor (SFR) metal- and oxide- fuel fabrication. The similar work has been previously done for PWR MOX fuel [1]. The analysis will be performed based on the assumption that the separation of the fission products (FP) during the reprocessing of UOX spent nuclear fuel assemblies is not perfect and that, consequently, a certain amount of FP goes into the Pu stream used to fabricate SFR fuels. Only non-gaseous FPs have been considered (see the list of 176 isotopes considered in the calculations in Appendix 1 of Reference 1). Throughout of this report, we define the mixture of Pu and FPs as PuFP. The main objective of this analysis is to quantify the increase of the Pu content of SFR fuels necessary to maintain the same average burnup at discharge independently of the amount of FP in the Pu stream, i.e. independently of the PuFP composition. The FP losses are considered element-independent, i.e., for example, 1% of FP losses mean that 1% of all non-gaseous FP leak into the Pu stream.

  2. Performance and design considerations in metal fueled cores. [LMFBR

    SciTech Connect

    Orechwa, Y.; Khalil, H.; Turski, R.B.

    1984-01-01

    To focus future metal fuel development requirements a study was performed to quantify the relationship between some critical core design parameters. The fuel studied was U-Pu-Zr alloy. Of interest are performance parameters, such as peak Pu enrichment, burnup swing, fast fluence, breeding ratio, and their relation to core parameters such as reactor size, degree of core heterogeneity, pin diameter, and linear heat rating. These performance parameters, while numericaly different from those of ceramic fuels, were found to exhibit the same qualitative dependence on the key design variables.

  3. Technical overview: CANDU MOX fuel dual irradiation experiment

    SciTech Connect

    Dimayuga, F.C.; M.R. Floyd, M.R.; Schankula, M.H.; Sullivan, J.D.

    1996-02-01

    This Technical Overview describes: the technical objectives and rational for the choice of MOX fuel fabrication parameters that are to be investigated; the pre-irradiation fuel characterization plan; the NRU irradiation plan; the post-irradiation examination plan; and a summary of the evaluations that can be extracted from the Parallex data. This Technical Overview is based on the 37-element reference CANDU MOX fuel design established in the 1994 Pu Dispositioning Study. An extension to this study is currently underway, aimed at increasing the Pu disposition rates of the mission. The results of this new study will likely specify a higher Pu loading for the CANDU MOX fuel. If confirmed, this Technical Overview document will be revised and the Parallex test matrix could be modified accordingly.

  4. Thermodynamic evaluation of the NaCl-MgCl 2-UCl 3-PuCl 3 system

    NASA Astrophysics Data System (ADS)

    Beneš, O.; Konings, R. J. M.

    2008-04-01

    A full thermodynamic description of the quaternary NaCl-MgCl 2-UCl 3-PuCl 3 system, a Molten Salt Fast Breeder Fuel, is presented. The binary phase diagrams have been assessed in this study and the data were used to extrapolate the higher order systems. To optimize the excess parameters of the liquid phase the modified quasi chemical model has been used, while for the solid solution the classical polynomial model has been applied. From the obtained results a possible fuel composition for the Molten Salt Reactor has been evaluated.

  5. Oxidation states, geometries, and electronic structures of plutonium tetroxide PuO4 isomers: is octavalent Pu viable?

    PubMed

    Huang, Wei; Xu, Wen-Hua; Su, Jing; Schwarz, W H E; Li, Jun

    2013-12-16

    In neutral chemical compounds, the highest known oxidation state of all elements in the Periodic Table is +VIII. While PuO4 is viewed as an exotic Pu(+VIII) complex, we have shown here that no stable electronic homologue of octavalent RuO4 and OsO4 exists for PuO4, even though Pu has the same number of eight valence electrons as Ru and Os. Using quantum chemical approaches at the levels of quasi-relativistic DFT, MP2, CCSD(T), and CASPT2, we find the ground state of PuO4 as a quintet (5)C2v-(PuO2)(+)(O2)(-) complex with the leading valence configuration of an (f(3))plutonyl(V) unit, loosely coupled to a superoxido (π*(3))O2(-) ligand. This stable isomer is likely detectable as a transient species, while the previously suggested planar (1)D4h-Pu(VIII)O4 isomer is only metastable. Through electronic structure analyses, the bonding and the oxidation states are explained and rationalized. We have predicted the characteristics of the electronic and vibrational spectra to assist future experimental identification of (PuO2)(+)(O2)(-) by IR, UV-vis, and ionization spectroscopy.

  6. ANALYSIS AND EXAMINATION OF MOX FUEL FROM NONPROLIFERATION PROGRAMS

    SciTech Connect

    McCoy, Kevin; Machut, Dr McLean; Morris, Robert Noel; Blanpain, Patrick; Hemrick, James Gordon

    2013-01-01

    The U.S. Department of Energy has decided to dispose of a portion of the nation s surplus plutonium by reconstituting it into mixed oxide (MOX) fuel and irradiating it in commercial power reactors. Four lead assemblies were manufactured and irradiated to a maximum fuel rod burnup of 47.3 MWd/kg heavy metal. This was the first commercial irradiation of MOX fuel with a 240Pu/239Pu ratio of less than 0.10. Five fuel rods with varying burnups and plutonium contents were selected from one of the assemblies and shipped to Oak Ridge National Laboratory for hot cell examination. The performance of the rods was analyzed with AREVA s next-generation GALILEO code. The results of the analysis confirmed that the fuel rods had performed safely and predictably, and that GALILEO is applicable to MOX fuel with a low 240Pu/239Pu ratio as well as to standard MOX. The results are presented and compared to the GALILEO database. In addition, the fuel cladding was tested to confirm that traces of gallium in the fuel pellets had not affected the mechanical properties of the cladding. The irradiated cladding was found to remain ductile at both room temperature and 350 C for both the axial and circumferential directions.

  7. Distinguishing Pu Metal from Pu Oxide and Determining alpha-ratio using Fast Neutron Counting

    SciTech Connect

    Verbeke, J. M.; Chapline, G. F.; Nakae, L. F.; Prasad, M. K.; Sheets, S. A.; Snyderman, N. J.

    2015-01-07

    We describe a new method for determining the ratio of the rate of (α, n) source neutrons to the rate of spontaneous fission neutrons, the so called α-ratio. This method is made possible by fast neutron counting with liquid scintillator detectors, which can determine the shape of the fast neutron spectrum. The method utilizes the spectral difference between fission spectrum neutrons from Pu metal and the spectrum of (α, n) neutrons from PuO2. Our method is a generalization of the Cifarelli-Hage method for determining keff for fissile assemblies, and also simultaneously determines keff along with the α-ratio.

  8. Criticality safety evaluation report for FFTF 42% fuel assemblies

    SciTech Connect

    Richard, R.F.

    1997-10-28

    An FFTF tritium/isotope production mission will require a new fuel supply. The reference design core will use a mixed oxide fuel nominally enriched to 40 wt% Pu. This enrichment is significantly higher than that of the standard Driver Fuel Assemblies used in past operations. Consequently, criticality safety for handling and storage of this fuel must be addressed. The purpose of this document is to begin the process by determining the minimum critical number for these new fuel assemblies in water, sodium and air. This analysis is preliminary and further work can be done to refine the results reported here. Analysis was initially done using 45 wt 5 PuO. Additionally, a preliminary assessment is done concerning storage of these fuel assemblies in Interim Decay Storage (IDS), Fuel Storage Facility (FSF), and Core Component Containers/Interim Storage Casks (CCC/ISC).

  9. Microscopic Calculations of 240Pu Fission

    SciTech Connect

    Younes, W; Gogny, D

    2007-09-11

    Hartree-Fock-Bogoliubov calculations have been performed with the Gogny finite-range effective interaction for {sup 240}Pu out to scission, using a new code developed at LLNL. A first set of calculations was performed with constrained quadrupole moment along the path of most probable fission, assuming axial symmetry but allowing for the spontaneous breaking of reflection symmetry of the nucleus. At a quadrupole moment of 345 b, the nucleus was found to spontaneously scission into two fragments. A second set of calculations, with all nuclear moments up to hexadecapole constrained, was performed to approach the scission configuration in a controlled manner. Calculated energies, moments, and representative plots of the total nuclear density are shown. The present calculations serve as a proof-of-principle, a blueprint, and starting-point solutions for a planned series of more comprehensive calculations to map out a large set of scission configurations, and the associated fission-fragment properties.

  10. Preparation of Pu{sup 239} sources

    SciTech Connect

    Holcomb, H.P.

    1988-08-05

    The Separations Technology Laboratory has prepared four sources to be used for calibrating a waste assay system (Passive/Active Neutron Assay) in Building 724-8G (Burial Ground). The four sources contain 0.5, 0.1, 0.05, and 0.01 grams Pu{sup 239}, respectively. The sources were prepared using aliquots from a single solution provided by the Quality Control (QC) group of Laboratories Department. The solution contained weapons-grade plutonium dissolved in nitric acid. Final solution acidity was 3M. Coulometry had been used to obtain a total plutonium content per unit volume. The weight percent of the plutonium isotopes present was obtained via mass spectrometry.

  11. LLNL Workshop on TEM of Pu

    SciTech Connect

    King, W.E.

    1996-09-10

    On Sept. 10, 1996, LLNL hosted a workshop aimed at answering the question: Is it possible to carry out transmission electron microscopy (TEM) on plutonium metal in an electron microscope located outside the LLNL plutonium facility. The workshop focused on evaluation of a proposed plan for Pu microscopy both from a technical and environment, health, and safety point of view. After review and modification of the plan, workshop participants unanimously concluded that: (1) the technical plan is sound, (2) this technical plan, including a proposal for a new TEM, provides significant improvements and unique capabilities compared with the effort at LANL and is therefore complementary, (3) there is no significant environment, health, and safety obstacle to this plan.

  12. Americium and plutonium release behavior from irradiated mixed oxide fuel during heating

    NASA Astrophysics Data System (ADS)

    Sato, I.; Suto, M.; Miwa, S.; Hirosawa, T.; Koyama, S.

    2013-06-01

    The release behavior of Pu and Am was investigated under the reducing atmosphere expected in sodium cooled fast reactor severe accidents. Irradiated Pu and U mixed oxide fuels were heated at maximum temperatures of 2773 K and 3273 K. EPMA, γ-ray spectrometry and α-ray spectrometry for released and residual materials revealed that Pu and Am can be released more easily than U under the reducing atmosphere. The respective release rate coefficients for Pu and Am were obtained as 3.11 × 10-4 min-1 and 1.60 × 10-4 min-1 at 2773 K under the reducing atmosphere with oxygen partial pressure less than 0.02 Pa. Results of thermochemical calculations indicated that the main released chemical forms would likely be PuO for Pu and Am for Am under quite low oxygen partial pressure.

  13. Multirecycling of Plutonium from LMFBR Blanket in Standard PWRs Loaded with MOX Fuel

    SciTech Connect

    Sonat Sen; Gilles Youinou

    2013-02-01

    It is now well-known that, from a physics standpoint, Pu, or even TRU (i.e. Pu+M.A.), originating from LEU fuel irradiated in PWRs can be multirecycled also in PWRs using MOX fuel. However, the degradation of the isotopic composition during irradiation necessitates using enriched U in conjunction with the MOX fuel either homogeneously or heterogeneously to maintain the Pu (or TRU) content at a level allowing safe operation of the reactor, i.e. below about 10%. The study is related to another possible utilization of the excess Pu produced in the blanket of a LMFBR, namely in a PWR(MOX). In this case the more Pu is bred in the LMFBR, the more PWR(MOX) it can sustain. The important difference between the Pu coming from the blanket of a LMFBR and that coming from a PWR(LEU) is its isotopic composition. The first one contains about 95% of fissile isotopes whereas the second one contains only about 65% of fissile isotopes. As it will be shown later, this difference allows the PWR fed by Pu from the LMFBR blanket to operate with natural U instead of enriched U when it is fed by Pu from PWR(LEU)

  14. Some neutron and gamma radiation characteristics of plutonium cermet fuel for isotopic power sources

    NASA Technical Reports Server (NTRS)

    Neff, R. A.; Anderson, M. E.; Campbell, A. R.; Haas, F. X.

    1972-01-01

    Gamma and neutron measurements on various types of plutonium sources are presented in order to show the effects of O-17, O-18 F-19, Pu-236, age of the fuel, and size of the source on the gamma and neutron spectra. Analysis of the radiation measurements shows that fluorine is the main contributor to the neutron yields from present plutonium-molybdenum cermet fuel, while both fluorine and Pu-236 daughters contribute significantly to the gamma ray intensities.

  15. Next-generation purex flowsheets with acetohydroxamic acid as complexant for FBR and thermal-fuel reprocessing

    SciTech Connect

    Kumar, Shekhar; Koganti, S.B.

    2008-07-01

    Acetohydroxamic acid (AHA) is a novel complexant for recycle of nuclear-fuel materials. It can be used in ordinary centrifugal extractors, eliminating the need for electro-redox equipment or complex maintenance requirements in a remotely maintained hot cell. In this work, the effect of AHA on Pu(IV) distribution ratios in 30% TBP system was quantified, modeled, and integrated in SIMPSEX code. Two sets of batch experiments involving macro Pu concentrations (conducted at IGCAR) and one high-Pu flowsheet (literature) were simulated for AHA based U-Pu separation. Based on the simulation and validation results, AHA based next-generation reprocessing flowsheets are proposed for co-processing based FBR and thermal-fuel reprocessing as well as evaporator-less macro-level Pu concentration process required for MOX fuel fabrication. Utilization of AHA results in significant simplification in plant design and simpler technology implementations with significant cost savings. (authors)

  16. Properties measurements of (U{sub 0.7}Pu{sub 0.3})O{sub 2-x} in PO{sub 2}-controlled atmosphere

    SciTech Connect

    Kato, M.; Murakami, T.; Sunaoshi, T.; Nelson, A.T.; McClellan, K.J.

    2013-07-01

    The investigation of physical properties of uranium and plutonium mixed oxide (MOX) fuels is important for the development of fast reactor fuels. It is well known that MOX is a nonstoichiometric oxide, and the physical properties change drastically with the Oxygen-to-Metal (O/M) ratio. A control technique for O/M ratio was established for measurements of high temperature properties of uranium and plutonium mixed oxide fuels. Sintering behavior, thermal expansion and O/M change of (U{sub 0.7}Pu{sub 0.3})O{sub 2.00} and (U{sub 0.7}Pu{sub 0.3})O{sub 1.99} were investigated in PO{sub 2}-controlled atmosphere which was controlled by H{sub 2}/H{sub 2}O gas system. Sintering behavior changed drastically with O/M ratio, and shrinkage of (U{sub 0.7}Pu{sub 0.3})O{sub 2.00} was faster and more advanced at lower temperatures as compared with (U{sub 0.7}Pu{sub 0.3})O{sub 1.99}. Thermal expansion was observed to be slightly increased with decreasing O/M ratio. (authors)

  17. Postirradiation examination of the HT9 clad fuel test X425 at 2.9% burnup

    SciTech Connect

    Pahl, R G; Beck, W N; Sanecki, J E

    1987-11-01

    The X425 experiment was the first EBR-II subassembly to be irradiated with U-Pu-Zr metallic fuel clad in the HT9 alloy. This report summarizes our initial postirradiation examination of selected elements from X425 at 2.9% peak burnup. Fuel microstructure, swelling behavior, fission gas release, and fuel/clad chemical interaction are discussed.

  18. An Investigation of the Use of Fully Ceramic Microencapsulated Fuel for Transuranic Waste Recycling in Pressurized Water Reactors

    SciTech Connect

    Gentry, Cole A; Godfrey, Andrew T; Terrani, Kurt A; Gehin, Jess C; Powers, Jeffrey J; Maldonado, G Ivan

    2014-01-01

    An investigation of the utilization of TRistructural- ISOtropic (TRISO)-coated fuel particles for the burning of plutonium/neptunium (Pu/Np) isotopes in typical Westinghouse four-loop pressurized water reactors is presented. Though numerous studies have evaluated the burning of transuranic isotopes in light water reactors (LWRs), this work differentiates itself by employing Pu/Np-loaded TRISO particles embedded within a silicon carbide (SiC) matrix and formed into pellets, constituting the fully ceramic microencapsulated (FCM) fuel concept that can be loaded into standard LWR fuel element cladding. This approach provides the capability of Pu/Np burning and, by virtue of the multibarrier TRISO particle design and SiC matrix properties, will allow for greater burnup of Pu/Np material, plus improved fuel reliability and thermal performance. In this study, a variety of heterogeneous assembly layouts, which utilize a mix of FCM rods and typical UO2 rods, and core loading patterns were analyzed to demonstrate the neutronic feasibility of Pu/Np-loaded TRISO fuel. The assembly and core designs herein reported are not fully optimized and require fine-tuning to flatten power peaks; however, the progress achieved thus far strongly supports the conclusion that with further rod/assembly/core loading and placement optimization, Pu/Np-loaded TRISO fuel and core designs that are capable of balancing Pu/Np production and destruction can be designed within the standard constraints for thermal and reactivity performance in pressurized water reactors.

  19. Measurement of the 242Pu neutron capture cross section

    NASA Astrophysics Data System (ADS)

    Buckner, M. Q.; Wu, C. Y.; Henderson, R. A.; Bucher, B.; Bredeweg, T. A.; Baramsai, B.; Couture, A.; Jandel, M.; Mosby, S.; O'Donnell, J. M.; Ullmann, J. L.; Chyzh, A.; Dance Collaboration

    2015-10-01

    Precision (n,f) and (n, γ) cross sections are important for the network calculations of the radiochemical diagnostic chain for the U.S. DOE's Stockpile Stewardship Program. 242Pu(n, γ) cross section is relevant to the network calculations of Pu and Am. Additionally, new reactor concepts have catalyzed considerable interest in the measurement of improved cross sections for neutron-induced reactions on key actinides. To date, little or no experimental data has been reported on 242Pu(n, γ) for incident neutron energy below 50 keV. A new measurement of the 242Pu(n, γ) reaction was performed with the DANCE together with an improved PPAC for fission-fragment detection at LANSCE during FY14. The relative scale of the 242Pu(n, γ) cross section spans four orders of magnitude for incident neutron energies from thermal to ~ 30 keV. The absolute scale of the 242Pu(n, γ) cross section is set according to the measured 239Pu(n,f) resonance at 7.8 eV; the target was spiked with 239Pu for this measurement. The absolute 242Pu(n, γ) neutron capture cross section is ~ 30% higher than the cross section reported in ENDF for the 2.7 eV resonance. Latest results to be reported. Funded by U.S. DOE Contract No. DE-AC52-07NA27344 (LLNL) and DE-AC52-06NA25396 (LANL). U.S. DOE/NNSA Office of Defense Nuclear Nonproliferation Research and Development. Isotopes (ORNL).

  20. An alternative structure of Pu{sub 4}O{sub 9} (''PuO{sub 2.25}'') incorporating interstitial hydroxyl rather than oxide

    SciTech Connect

    Penneman, R.A.; Paffett, M.T. . E-mail: mtp@lanl.gov

    2005-02-15

    Bond length/bond strength relationships are applied to the Pu{sub 4}O{sub 9} ('PuO{sub 2.25}') structure proposed by others and support one Pu(V) with a central hydroxyl ion but not a central oxide ion nor formation of Pu(VI). Bond distances and bond strengths are normal for a central ion of unit charge, and reconcile the finding that cell dimensions are so minimally changed from those of PuO{sub 2}. Substitution of hydroxyl for oxide accounts for the 'excess' oxygen content of PuO{sub 2.265,} yielding PuO{sub 2}(OH){sub 0.249.} The short range, local order (structure) of the 'Pu{sub 4}O{sub 9}' entity is alternatively formulated as Pu{sub 4}O{sub 8}OH.

  1. Study of Pu consumption in light water reactors: Evaluation of GE advanced boiling water reactor plants, compilation of Phase 1C task reports

    SciTech Connect

    Not Available

    1994-01-15

    This report summarizes the evaluations conducted during Phase 1C of the Pu Disposition Study have provided further results which reinforce the conclusions reached during Phase 1A & 1B: These conclusions clearly establish the benefits of the fission option and the use of the ABWR as a reliable, proven, well-defined and cost-effective means available to disposition the weapons Pu. This project could be implemented in the near-term at a cost and on a schedule being validated by reactor plants currently under construction in Japan and by cost and schedule history and validated plans for MOX plants in Europe. Evaluations conducted during this phase have established that (1) the MOX fuel is licensable based on existing criteria for new fuel with limited lead fuel rod testing, (2) that the applicable requirements for transport, handling and repository storage can be met, and (3) that all the applicable safeguards criteria can be met.

  2. 239Pu Resonance Evaluation for Thermal Benchmark System Calculations

    SciTech Connect

    Leal, Luiz C; Noguere, G; De Saint Jean, C; Kahler, A.

    2013-01-01

    Analyses of thermal plutonium solution critical benchmark systems have indicated a deciency in the 239Pu resonance evaluation. To investigate possible solutions to this issue, the Organisation for Economic Co-operation and Development (OECD) Nuclear Energy Agency (NEA) Working Party for Evaluation Cooperation (WPEC) established Subgroup 34 to focus on the reevaluation of the 239Pu resolved resonance parameters. In addition, the impacts of the prompt neutron multiplication (nubar) and the prompt neutron ssion spectrum (PFNS) have been investigated. The objective of this paper is to present the results of the 239Pu resolved resonance evaluation eort.

  3. 239Pu Resonance Evaluation for Thermal Benchmark System Calculations

    NASA Astrophysics Data System (ADS)

    Leal, L. C.; Noguere, G.; de Saint Jean, C.; Kahler, A. C.

    2014-04-01

    Analyses of thermal plutonium solution critical benchmark systems have indicated a deficiency in the 239Pu resonance evaluation. To investigate possible solutions to this issue, the Organisation for Economic Co-operation and Development (OECD) Nuclear Energy Agency (NEA) Working Party for Evaluation Cooperation (WPEC) established Subgroup 34 to focus on the reevaluation of the 239Pu resolved resonance parameters. In addition, the impacts of the prompt neutron multiplicity (νbar) and the prompt neutron fission spectrum (PFNS) have been investigated. The objective of this paper is to present the results of the 239Pu resolved resonance evaluation effort.

  4. Elastic properties of gamma-Pu by resonant ultrasound spectroscopy

    SciTech Connect

    Migliori, Albert; Betts, J; Trugman, A; Mielke, C H; Mitchell, J N; Ramos, M; Stroe, I

    2009-01-01

    Despite intense experimental and theoretical work on Pu, there is still little understanding of the strange properties of this metal. We used resonant ultrasound spectroscopy method to investigate the elastic properties of pure polycrystalline Pu at high temperatures. Shear and longitudinal elastic moduli of the {gamma}-phase of Pu were determined simultaneously and the bulk modulus was computed from them. A smooth linear and large decrease of all elastic moduli with increasing temperature was observed. We calculated the Poisson ratio and found that it increases from 0.242 at 519K to 0.252 at 571K.

  5. Process parameters optimization in ion exchange 238Pu aqueous processing

    NASA Astrophysics Data System (ADS)

    Pansoy-Hjelvik, M. E.; Nixon, J.; Laurinat, J.; Brock, J.; Silver, G.; Reimus, M.; Ramsey, K. B.

    2000-07-01

    This paper describes bench-scale efforts (5-7 grams of 238Pu) to optimize the ion exchange process for 234U separation with minimal 238Pu losses to the effluent and wash liquids. The bench-scale experiments also determine the methodology to be used for the full-scale process: 5 kg238Pu annual throughput. Heat transfer calculations used to determine the thermal gradients expected during ion exchange processing are also described. The calculations were performed in collaboration with Westinghouse Savannah River Technology Center (WSRTC) and provide information for the design of the full-scale ion exchange equipment.

  6. Heavy metal inventory and fuel sustainability of recycling TRU in FBR design

    NASA Astrophysics Data System (ADS)

    Permana, Sidik; Suzuki, Mitsutoshi; Su'ud, Zaki

    2012-06-01

    Nuclear fuel materials from spent fuel of light water reactors have a potential to be used for destructive devices with very huge energy release or in the same time, it can be utilized as a peaceful energy or civil applications, for generating electricity, desalination of water, medical application and others applications. Several research activities showed some recycled spent fuel can be used as additional fuel loading for increasing fuel breeding capability as well as improving intrinsic aspect of nuclear non-proliferation. The present investigation intends to evaluate the composition of heavy metals inventories and fuel breeding capability in the FBR design based on the loaded fuel of light water reactor (LWR) spent fuel (SF) of 33 GWd/t with 5 years cooling time by adopting depletion code of ORIGEN. Whole core analysis of FBR design is performed by adopting and coupling codes such as SLAROM code, JOINT and CITATION codes. Nuclear data library, JFS-3-J-3.2R which is based on the JENDL 3.2 has been used for nuclear data analysis. JSFR design is the basis design reference which basically adopted 800 days cycle length for 4 batches system. Higher inventories of plutonium of MOX fuel and TRU fuel types at equilibrium composition than initial composition have been shown. Minor actinide (MA) inventory compositions obtain a different inventory trends at equilibrium composition for both fuel types. Higher Inventory of MA is obtained by MOX fuel and less MA inventory for TRU fuel at equilibrium composition than initial composition. Some different MA inventories can be estimated from the different inventory trend of americium (Am). Higher americium inventory for MOX fuel and less americium inventory for TRU fuel at equilibrium condition. Breeding ratio of TRU fuel is relatively higher compared with MOX fuel type. It can be estimated from relatively higher production of Pu-238 (through converted MA) in TRU fuel, and Pu-238 converts through neutron capture to produce Pu-239

  7. Heavy metal inventory and fuel sustainability of recycling TRU in FBR design

    SciTech Connect

    Permana, Sidik; Suzuki, Mitsutoshi; Su'ud, Zaki

    2012-06-06

    Nuclear fuel materials from spent fuel of light water reactors have a potential to be used for destructive devices with very huge energy release or in the same time, it can be utilized as a peaceful energy or civil applications, for generating electricity, desalination of water, medical application and others applications. Several research activities showed some recycled spent fuel can be used as additional fuel loading for increasing fuel breeding capability as well as improving intrinsic aspect of nuclear non-proliferation. The present investigation intends to evaluate the composition of heavy metals inventories and fuel breeding capability in the FBR design based on the loaded fuel of light water reactor (LWR) spent fuel (SF) of 33 GWd/t with 5 years cooling time by adopting depletion code of ORIGEN. Whole core analysis of FBR design is performed by adopting and coupling codes such as SLAROM code, JOINT and CITATION codes. Nuclear data library, JFS-3-J-3.2R which is based on the JENDL 3.2 has been used for nuclear data analysis. JSFR design is the basis design reference which basically adopted 800 days cycle length for 4 batches system. Higher inventories of plutonium of MOX fuel and TRU fuel types at equilibrium composition than initial composition have been shown. Minor actinide (MA) inventory compositions obtain a different inventory trends at equilibrium composition for both fuel types. Higher Inventory of MA is obtained by MOX fuel and less MA inventory for TRU fuel at equilibrium composition than initial composition. Some different MA inventories can be estimated from the different inventory trend of americium (Am). Higher americium inventory for MOX fuel and less americium inventory for TRU fuel at equilibrium condition. Breeding ratio of TRU fuel is relatively higher compared with MOX fuel type. It can be estimated from relatively higher production of Pu-238 (through converted MA) in TRU fuel, and Pu-238 converts through neutron capture to produce Pu-239

  8. Implications of Plutonium isotopic separation on closed fuel cycles and repository design

    SciTech Connect

    Forsberg, C.

    2013-07-01

    Advances in laser enrichment may enable relatively low-cost plutonium isotopic separation. This would have large impacts on LWR closed fuel cycles and waste management. If Pu-240 is removed before recycling plutonium as mixed oxide (MOX) fuel, it would dramatically reduce the buildup of higher plutonium isotopes, Americium, and Curium. Pu-240 is a fertile material and thus can be replaced by U-238. Eliminating the higher plutonium isotopes in MOX fuel increases the Doppler feedback, simplifies reactor control, and allows infinite recycle of MOX plutonium in LWRs. Eliminating fertile Pu-240 and Pu-242 reduces the plutonium content in MOX fuel and simplifies fabrication. Reducing production of Pu-241 reduces production of Am-241 - the primary heat generator in spent nuclear fuels after several decades. Reducing heat generating Am-241 would reduce repository cost and waste toxicity. Avoiding Am- 241 avoids its decay product Np-237, a nuclide that partly controls long-term oxidizing repository performance. Most of these benefits also apply to LWR plutonium recycled into fast reactors. There are benefits for plutonium isotopic separation in fast reactor fuel cycles (particularly removal of Pu-242) but the benefits are less. (author)

  9. Studies on preparation of (U0.47,Pu0.53)O2 microspheres by internal gelation process

    NASA Astrophysics Data System (ADS)

    Kumar, Ashok; Radhakrishna, J.; Kumar, N.; Pai, Rajesh V.; Dehadrai, J. V.; Deb, A. C.; Mukerjee, S. K.

    2013-03-01

    It is proposed to irradiate experimental fuel pins containing 750 μm (U0.47,Pu0.53)O2 microspheres (coarse fraction) and 110 μm UO2 microspheres (fine fraction) in the Fast Breeder Test Reactor at Kalpakkam, with a view to develop sphere-pac fuel for Fast Breeder Reactors in India. This communication describes optimization of the internal gelation process to produce dense sintered (U0.47,Pu0.53)O2 microspheres. Major modifications were incorporated in the feed preparation and the calcination and sintering steps. Use of pre-heated HMTA and urea and plutonium nitrate solution with optimum nitrate to plutonium ratio led to desired gelation kinetics and growth of crystallites which is necessary to obtain good gel microspheres. The calcination process was optimised to remove residual organics without cracking of microspheres. The studies showed that dense crack free sintered (U0.47,Pu0.53)O2 microspheres of about 98% theoretical density (TD) can be prepared using the internal gelation method.

  10. PU IMMOBILIZATION - INDUCTION MELTING ND OFFGAS TESTING

    SciTech Connect

    Marra, J

    2006-11-28

    The Cylindrical Induction Melter (CIM) at the Aiken County Technology Laboratory (ACTL) has been operated by the Savannah River National Laboratory (SRNL) to support the Pu Disposition Conceptual Design (CD-0) development effort. The primary purpose of this report is to summarize the offgas sampling tests conducted in the CIM to capture and analyze the particulate and vapors emitted from lanthanide borosilicate (LaBS) Frit X with HfO{sub 2} as a surrogate for PuO{sub 2} and added impurities. In addition, this report describes several initial tests of the CIM for the vitrification of LaBS Frit X with HfO{sub 2}. The activities required to produce Frit X from batch chemical oxides for subsequent milling to yield glass frit of nominally 20 micron particle size are also discussed. The tests with impurities added showed that alkali salts such as NaCl and KCl were substantially emitted into the offgas system as the salt particulate, HCl, or Cl{sub 2}. Retention of Na and K in the glass were about 80 and 55%, respectively. Chloride retention was about 35%; chloride remaining in the glass was 0.29-0.37 wt%. Based on a material balance, approximately 83% of F fed was retained in the glass at about 0.09 wt % (F could not be measured directly at this concentration). Transition metals (Ni, Cu, Fe, Mo, Cr) were also volatilized to varying extents. A very small amount (<0.1 g) of nickel compounds and KCl were found in crystals deposited on the melter offgas line. Overall, about 58-72% of the impurities added were volatilized. Virtually all of the particulate species were collected on the nominal 0.3 {micro}m filter. The particulate evolution rate ranged from 2-8 g/kg glass/h. The particulate was found to be as small as 0.2 {micro}m and have an approximate median size of 0.5 {micro}m. The particulate salt was also found to stick together by forming bridges between particles. Further runs without washable salts are recommended. Measurements of particle size distribution for use in

  11. PU Vulpeculae: an eclipsing symbiotic nova.

    NASA Astrophysics Data System (ADS)

    Nussbaumer, H.; Vogel, M.

    1996-03-01

    A series of IUE observation from 1992 to 1995 has definitely established PU Vul as an eclipsing binary. The outburst of this symbiotic nova began in 1977. An extended fading in 1980 gave rise to various interpretations, the eclipse scenario being one of them, dust formation being another. From AFOEV and AAVSO observations we find a period of 4900+/-100days, or 13.42+/-0.27years. An eclipsing object of such a long period signifies that we see the binary system at an orbital inclination close to 90deg. ESO observations in the near infrared give an orbital velocity of 4.7km/s and a mass function of m_f_=~0.05. Assuming a white dwarf mass between 0.4Msun_ and 0.5Msun_ gives for the red giant 0.7<=M/Msun_<=1.1. From the length of the eclipse the radius of the red giant is determined as R_giant_>=82Rsun_. We discuss IUE, HST and ground based observations of PU Vulpeculae before and during its second observed eclipse of the hot component by the cool giant which lasted from 1993 to 1995, mid-eclipse was in April 1994. Line profiles, particularly those taken by HST, allow a neat distinction between narrow nebular lines and broader wind lines which prove the existence of a fast wind from the hot star in the binary system of v=~1000km/s. That wind has relatively high densities (N_e_>10^12^cm^-3^) and is optically thick to radiation at λ<228A. Nebular lines have half widths corresponding to v=~70km/s. During the 1994 eclipse the more highly ionized lines were strongly eclipsed, whereas the lowly ionized nebular lines were hardly affected. This proves that the lowly ionized nebular lines are emitted in a very extended region, and not only close to the cool giant. From 1990 to 1994 relative C/N/O abundances of the nebular and wind emission regions have not changed beyond observational uncertainties.

  12. (239)Pu, (240)Pu, and (241)Am determination in hot particles by low level gamma-spectrometry.

    PubMed

    Jiménez-Ramos, M C; Hurtado, S; Chamizo, E; García-Tenorio, R; León-Vintró, L; Mitchell, P I

    2010-06-01

    A nondestructive method based on low-energy, high-resolution photon spectrometry is presented which allows accurate determination of (239)Pu, (240)Pu, and (241)Am (as a daughter of (241)Pu) activities in radioactive particles containing relatively high levels of plutonium isotopes. The proposed method requires only one measurement for the establishment of an absolute efficiency curve. Since the density and composition of the radioactive particles of interest may vary, a self-absorption correction is required for the accurate determination of isotopic activities and ratios. This correction is carried out for each individual particle using the convenient gamma-ray emissions of (241)Am.

  13. Proliferation resistant fuel for pebble bed modular reactors

    SciTech Connect

    Ronen, Y.; Aboudy, M.; Regev, D.; Gilad, E.

    2012-07-01

    We show that it is possible to denature the Plutonium produced in Pebble Bed Modular Reactors (PBMR) by doping the nuclear fuel with either 3050 ppm of {sup 237}Np or 2100 ppm of Am vector. A correct choice of these isotopes concentration yields denatured Plutonium with isotopic ratio {sup 238}Pu/Pu {>=} 6%, for the entire fuel burnup cycle. The penalty for introducing these isotopes into the nuclear fuel is a subsequent shortening of the fuel burnup cycle, with respect to a non-doped reference fuel, by 41.2 Full Power Days (FPDs) and 19.9 FPDs, respectively, which correspond to 4070 MWd/ton and 1965 MWd/ton reduction in fuel discharge burnup. (authors)

  14. Spatial and temporal distribution of Pu in the Northwest Pacific Ocean using modern coral archives.

    PubMed

    Lindahl, Patric; Andersen, Morten B; Keith-Roach, Miranda; Worsfold, Paul; Hyeong, Kiseong; Choi, Min-Seok; Lee, Sang-Hoon

    2012-04-01

    Historical (239)Pu activity concentrations and (240)Pu/(239)Pu atom ratios were determined in skeletons of dated modern corals collected from three locations (Chuuk Lagoon, Ishigaki Island and Iki Island) to identify spatial and temporal variations in Pu inputs to the Northwest Pacific Ocean. The main Pu source in the Northwest Pacific is fallout from atmospheric nuclear weapons testing which consists of global fallout and close-in fallout from the former US Pacific Proving Grounds (PPG) in the Marshall Islands. PPG close-in fallout dominated the Pu input in the 1950s, as was observed with higher (240)Pu/(239)Pu atom ratios (>0.30) at the Ishigaki site. Specific fallout Pu contamination from the Nagasaki atomic bomb and the Ivy Mike thermonuclear detonation at the PPG were identified at Ishigaki Island from the (240)Pu/(239)Pu atom ratios of 0.07 and 0.46, respectively. During the 1960s and 1970s, global fallout was the major Pu source to the Northwest Pacific with over 60% contribution to the total Pu. After the cessation of the atmospheric nuclear tests, the PPG again dominated the Pu input due to the continuous transport of remobilised Pu from the Marshall Islands along the North Equatorial Current and the subsequent Kuroshio Current. The Pu contributions from the PPG in recent coral bands (1984 onwards) varied over time with average estimated PPG contributions between 54% and 72% depending on location.

  15. Suitability of 239+240Pu and 137Cs as tracers for soil erosion assessment in mountain grasslands.

    PubMed

    Alewell, Christine; Meusburger, Katrin; Juretzko, Gregor; Mabit, Lionel; Ketterer, Michael E

    2014-05-01

    Anthropogenic radionuclides have been distributed globally due to nuclear weapons testing, nuclear accidents, nuclear weapons fabrication, and nuclear fuel reprocessing. While the negative consequences of this radioactive contamination are self-evident, the ubiquitous fallout radionuclides (FRNs) distribution form the basis for the use as tracers in ecological studies, namely for soil erosion assessment. Soil erosion is a major threat to mountain ecosystems worldwide. We compare the suitability of the anthropogenic FRNs, 137Cs and 239+240Pu as soil erosion tracers in two alpine valleys of Switzerland (Urseren Valley, Canton Uri, Central Swiss Alps and Val Piora, Ticino, Southern Alps). We sampled reference and potentially erosive sites in transects along both valleys. 137Cs measurements of soil samples were performed with a Li-drifted Germanium detector and 239+240Pu with ICP-MS. Our data indicates a heterogeneous deposition of the 137Cs, since most of the fallout origins from the Chernobyl April/May 1986 accident, when large parts of the European Alps were still snow-covered. In contrast, 239+240Pu fallout originated mainly from 1950s to 1960s atmospheric nuclear weapons tests, resulting in a more homogenous distribution and thus seems to be a more suitable tracer in mountainous grasslands. Soil erosion assessment using 239+240Pu as a tracer pointed to a huge dynamic and high heterogeneity of erosive processes (between sedimentation of 1.9 and 7 t ha(-1) yr(-1) and erosion of 0.2-16.4 t ha(-1) yr(-1) in the Urseren Valley and sedimentation of 0.4-20.3 t ha(-1) yr(-1) and erosion of 0.1-16.4 t ha(-1) yr(-1) at Val Piora). Our study represents a novel and successful application of 239+240Pu as a tracer of soil erosion in a mountain environment.

  16. Experimental Bench-marking of Pu Electronic Structure

    SciTech Connect

    Lawrence Livermore National Laboratory

    2007-07-31

    Our plan is to do Ce (as a Pu surrogate) this year and be ready to do Pu next year. The Fano (Spin-resolved Photoelectron Spectroscopy) measurements are essential to testing electron correlation in the occupied 5f states. BIS (Bremstrahlung Isochromat Spectroscopy or high energy Inverse Photoelectron Spectroscopy) experiments are crucial to a quantitative determination of the 5f unoccupied density of states (5f-UDOS). The 5f UDOS is the key to differentiation between a myriad of models of 5f electronic structure. During this time, we will work to converge to a solution for the Pu safety issues, with the plan to implement these in the next FY. Acceleration of this schedule and implementation of the safety plan in this FY will require a very significant increase in funding. Ultimately, results from the Pu experiments will be fed into calculations performed by P. Soderlind, A. Landa, and others.

  17. [239Pu and chromosomal aberrations in human peripheral blood lymphocytes].

    PubMed

    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).

  18. Ferro- and antiferro-magnetism in (Np, Pu)BC

    SciTech Connect

    Klimczuk, T.; Kozub, A. L.; Griveau, J.-C.; Colineau, E.; Wastin, F.; Falmbigl, M.; Rogl, P.

    2015-04-01

    Two new transuranium metal boron carbides, NpBC and PuBC, have been synthesized. Rietveld refinements of powder XRD patterns of (Np,Pu)BC confirmed in both cases isotypism with the structure type of UBC. Temperature dependent magnetic susceptibility data reveal antiferromagnetic ordering for PuBC below T{sub N} = 44 K, whereas ferromagnetic ordering was found for NpBC below T{sub C} = 61 K. Heat capacity measurements prove the bulk character of the observed magnetic transition for both compounds. The total energy electronic band structure calculations support formation of the ferromagnetic ground state for NpBC and the antiferromagnetic ground state for PuBC.

  19. Phase Characteristics of a U-20Pu-3Am-2Np-15Zr Metallic Alloy Containing Rare Earths

    SciTech Connect

    Douglas E. Burkes; J. Rory Kennedy; Thomas Hartmann; Cynthia A. Papesch

    2009-12-01

    Metallic fuel alloys consisting of uranium, plutonium, and zirconium with minor additions of americium and neptunium are under evaluation for potential use to transmute long-lived transuranic actinide isotopes in fast reactors. The current irradiation test series design, designated AFC2, includes minor additions of rare earth elements to simulate expected fission product carry-over from the electrochemical molten salt reprocessing technique. The metal fuel alloys have been fabricated by an arc casting technique. The as-cast fuel alloys have been investigated for phase and thermal properties, specifically, enthalpies of transition, transition temperatures, and room temperature phase characteristics. Results and observations related to these characteristics for the “fresh” fuel alloys are provided. The alloy compositions are based on a U-20Pu-3Am-2Np-15Zr alloy, along with additions of 1 and 1.5 wt% RE (at the expense of U) where RE denotes rare earth alloy of cerium, lanthanum, praseodymium and neodymium). Phase behavior and associated transitions have been compared to available U-Pu-Zr ternary diagrams with acceptable agreement. Enthalpies of transition were deconvoluted from heating and cooling thermal traces for relatively reliable values. The rare earth additions to the base alloy have a minimal influence on the room temperature phases present, but the room temperature phases present slightly impacted the enthalpies of transition and transition temperatures.

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

    NASA Astrophysics Data System (ADS)

    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.

  1. Probing Actinide Electronic Structure through Pu Cluster Calculations

    DOE PAGES

    Ryzhkov, Mickhail V.; Mirmelstein, Alexei; Yu, Sung-Woo; ...

    2013-02-26

    The calculations for the electronic structure of clusters of plutonium have been performed, within the framework of the relativistic discrete-variational method. Moreover, these theoretical results and those calculated earlier for related systems have been compared to spectroscopic data produced in the experimental investigations of bulk systems, including photoelectron spectroscopy. Observation of the changes in the Pu electronic structure as a function of size provides powerful insight for aspects of bulk Pu electronic structure.

  2. FUEL CYCLE POTENTIAL WASTE FOR DISPOSITION

    SciTech Connect

    Carter, J.

    2011-01-03

    The United States (U.S.) currently utilizes a once-through fuel cycle where used nuclear fuel (UNF) is stored on-site in either wet pools or in dry storage systems with ultimate disposal in a deep mined geologic repository envisioned. Within the Department of Energy's (DOE) Office of Nuclear Energy (DOE-NE), the Fuel Cycle Research and Development Program (FCR&D) develops options to the current commercial fuel cycle management strategy to enable the safe, secure, economic, and sustainable expansion of nuclear energy while minimizing proliferation risks by conducting research and development of advanced fuel cycles, including modified open and closed cycles. The safe management and disposition of used nuclear fuel and/or nuclear waste is a fundamental aspect of any nuclear fuel cycle. Yet, the routine disposal of used nuclear fuel and radioactive waste remains problematic. Advanced fuel cycles will generate different quantities and forms of waste than the current LWR fleet. This study analyzes the quantities and characteristics of potential waste forms including differing waste matrices, as a function of a variety of potential fuel cycle alternatives including: (1) Commercial UNF generated by uranium fuel light water reactors (LWR). Four once through fuel cycles analyzed in this study differ by varying the assumed expansion/contraction of nuclear power in the U.S. (2) Four alternative LWR used fuel recycling processes analyzed differ in the reprocessing method (aqueous vs. electro-chemical), complexity (Pu only or full transuranic (TRU) recovery) and waste forms generated. (3) Used Mixed Oxide (MOX) fuel derived from the recovered Pu utilizing a single reactor pass. (4) Potential waste forms generated by the reprocessing of fuels derived from recovered TRU utilizing multiple reactor passes.

  3. FUEL CYCLE POTENTIAL WASTE FOR DISPOSITION

    SciTech Connect

    Jones, R.; Carter, J.

    2010-10-13

    The United States (U.S.) currently utilizes a once-through fuel cycle where used nuclear fuel (UNF) is stored on-site in either wet pools or in dry storage systems with ultimate disposal in a deep mined geologic repository envisioned. Within the Department of Energy's (DOE) Office of Nuclear Energy (DOE-NE), the Fuel Cycle Research and Development Program (FCR&D) develops options to the current commercial fuel cycle management strategy to enable the safe, secure, economic, and sustainable expansion of nuclear energy while minimizing proliferation risks by conducting research and development of advanced fuel cycles, including modified open and closed cycles. The safe management and disposition of used nuclear fuel and/or nuclear waste is a fundamental aspect of any nuclear fuel cycle. Yet, the routine disposal of used nuclear fuel and radioactive waste remains problematic. Advanced fuel cycles will generate different quantities and forms of waste than the current LWR fleet. This study analyzes the quantities and characteristics of potential waste forms including differing waste matrices, as a function of a variety of potential fuel cycle alternatives including: (1) Commercial UNF generated by uranium fuel light water reactors (LWR). Four once through fuel cycles analyzed in this study differ by varying the assumed expansion/contraction of nuclear power in the U.S; (2) Four alternative LWR used fuel recycling processes analyzed differ in the reprocessing method (aqueous vs. electro-chemical), complexity (Pu only or full transuranic (TRU) recovery) and waste forms generated; (3) Used Mixed Oxide (MOX) fuel derived from the recovered Pu utilizing a single reactor pass; and (4) Potential waste forms generated by the reprocessing of fuels derived from recovered TRU utilizing multiple reactor passes.

  4. Neutronic double heterogeneity effect in particle dispersed type inert matrix fuels

    NASA Astrophysics Data System (ADS)

    Akie, H.; Takano, H.

    2006-06-01

    Rock-like oxide (ROX) fuel concept is studied in Japan for effective plutonium burning in light water reactors (LWRs). ROX is a heterogeneous fuel, where Pu containing yttria stabilized zirconia (YSZ) particles are dispersed in spinel matrix, and similar to the high temperature gas cooled reactor (HTR) fuel. The effect of such a 'double' heterogeneity (fuel, structure and coolant heterogeneity in reactor core, plus fuel heterogeneity) on HTR neutronic characteristics is important, while the effect was not taken into account in the ROX fueled LWR neutronics calculations. Here, this double heterogeneity effect is estimated for ROX fueled LWR, and compared with the Pu containing YSZ particle fueled HTR. As a result, the heterogeneity effect was negligible in the ROX-LWR system, while it is notable in YSZ-HTR system. The volume fraction of YSZ particle in the fuel region is one of the important parameter to cause the difference.

  5. METHOD OF PREPARING A CERAMIC FUEL ELEMENT

    DOEpatents

    Ross, W.T.; Bloomster, C.H.; Bardsley, R.E.

    1963-09-01

    A method is described for preparing a fuel element from -325 mesh PuO/ sub 2/ and -20 mesh UO/sub 2/, and the steps of screening --325 mesh UO/sub 2/ from the -20 mesh UO/sub 2/, mixing PuO/sub 2/ with the --325 mesh UO/sub 2/, blending this mixture with sufficient --20 mesh UO/sub 2/ to obtain the desired composition, introducing the blend into a metal tube, repeating the procedure until the tube is full, and vibrating the tube to compact the powder are included. (AEC)

  6. IMPACT OF FISSION PRODUCTS IMPURITY ON THE PLUTONIUM CONTENT IN PWR MOX FUELS

    SciTech Connect

    Gilles Youinou; Andrea Alfonsi

    2012-03-01

    This report presents the results of a neutronics analysis done in response to the charter IFCA-SAT-2 entitled 'Fuel impurity physics calculations'. This charter specifies that the separation of the fission products (FP) during the reprocessing of UOX spent nuclear fuel assemblies (UOX SNF) is not perfect and that, consequently, a certain amount of FP goes into the Pu stream used to fabricate PWR MOX fuel assemblies. Only non-gaseous FP have been considered (see the list of 176 isotopes considered in the calculations in Appendix 1). This mixture of Pu and FP is called PuFP. Note that, in this preliminary analysis, the FP losses are considered element-independent, i.e., for example, 1% of FP losses mean that 1% of all non-gaseous FP leak into the Pu stream.

  7. PRELIMINARY DATA CALL REPORT ADVANCED BURNER REACTOR START UP FUEL FABRICATION FACILITY

    SciTech Connect

    S. T. Khericha

    2007-04-01

    The purpose of this report is to provide data for preparation of a NEPA Environmental Impact Statement in support the U. S. Department of Energy (DOE) Global Nuclear Energy Partnership (GNEP). One of the GNEP objectives is to reduce the inventory of long lived actinide from the light water reactor (LWR) spent fuel. The LWR spent fuel contains Plutonium (Pu) -239 and other transuranics (TRU) such as Americium-241. One of the options is to transmute or burn these actinides in fast neutron spectra as well as generate the electricity. A sodium-cooled Advanced Recycling Reactor (ARR) concept has been proposed to achieve this goal. However, fuel with relatively high TRU content has not been used in the fast reactor. To demonstrate the utilization of TRU fuel in a fast reactor, an Advanced Burner Reactor (ABR) prototype of ARR is proposed, which would necessarily be started up using weapons grade (WG) Pu fuel. The WG Pu is distinguished by relatively highest proportions of Pu-239 and lesser amount of other actinides. The WG Pu will be used as the startup fuel along with TRU fuel in lead test assemblies. Because such fuel is not currently being produced in the US, a new facility (or new capability in an existing facility) is being considered for fabrication of WG Pu fuel for the ABR. This report is provided in response to ‘Data Call’ for the construction of startup fuel fabrication facility. It is anticipated that the facility will provide the startup fuel for 10-15 years and will take to 3 to 5 years to construct.

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

    NASA Astrophysics Data System (ADS)

    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.

  9. Method for photochemical reduction of uranyl nitrate by tri-N-butyl phosphate and application of this method to nuclear fuel reprocessing

    DOEpatents

    De Poorter, Gerald L.; Rofer-De Poorter, Cheryl K.

    1978-01-01

    Uranyl ion in solution in tri-n-butyl phosphate is readily photochemically reduced to U(IV). The product U(IV) may effectively be used in the Purex process for treating spent nuclear fuels to reduce Pu(IV) to Pu(III). The Pu(III) is readily separated from uranium in solution in the tri-n-butyl phosphate by an aqueous strip.

  10. Nuclear Fuel Reprocessing

    SciTech Connect

    Harold F. McFarlane; Terry Todd

    2013-11-01

    Reprocessing is essential to closing nuclear fuel cycle. Natural uranium contains only 0.7 percent 235U, the fissile (see glossary for technical terms) isotope that produces most of the fission energy in a nuclear power plant. Prior to being used in commercial nuclear fuel, uranium is typically enriched to 3–5% in 235U. If the enrichment process discards depleted uranium at 0.2 percent 235U, it takes more than seven tonnes of uranium feed to produce one tonne of 4%-enriched uranium. Nuclear fuel discharged at the end of its economic lifetime contains less one percent 235U, but still more than the natural ore. Less than one percent of the uranium that enters the fuel cycle is actually used in a single pass through the reactor. The other naturally occurring isotope, 238U, directly contributes in a minor way to power generation. However, its main role is to transmute into plutoniumby neutron capture and subsequent radioactive decay of unstable uraniumand neptuniumisotopes. 239Pu and 241Pu are fissile isotopes that produce more than 40% of the fission energy in commercially deployed reactors. It is recovery of the plutonium (and to a lesser extent the uranium) for use in recycled nuclear fuel that has been the primary focus of commercial reprocessing. Uraniumtargets irradiated in special purpose reactors are also reprocessed to obtain the fission product 99Mo, the parent isotope of technetium, which is widely used inmedical procedures. Among the fission products, recovery of such expensive metals as platinum and rhodium is technically achievable, but not economically viable in current market and regulatory conditions. During the past 60 years, many different techniques for reprocessing used nuclear fuel have been proposed and tested in the laboratory. However, commercial reprocessing has been implemented along a single line of aqueous solvent extraction technology called plutonium uranium reduction extraction process (PUREX). Similarly, hundreds of types of reactor

  11. UO2 and PuO2 utilization in high temperature engineering test reactor with helium coolant

    NASA Astrophysics Data System (ADS)

    Waris, Abdul; Aji, Indarta K.; Novitrian, Pramuditya, Syeilendra; Su'ud, Zaki

    2016-03-01

    High temperature engineering test reactor (HTTR) is one of high temperature gas cooled reactor (HTGR) types which has been developed by Japanese Atomic Energy Research Institute (JAERI). The HTTR is a graphite moderator, helium gas coolant, 30 MW thermal output and 950 °C outlet coolant temperature for high temperature test operation. Original HTTR uses UO2 fuel. In this study, we have evaluated the use of UO2 and PuO2 in form of mixed oxide (MOX) fuel in HTTR. The reactor cell calculation was performed by using SRAC 2002 code, with nuclear data library was derived from JENDL3.2. The result shows that HTTR can obtain its criticality condition if the enrichment of 235U in loaded fuel is 18.0% or above.

  12. A study of accelerated radiation damage effects in PuO2 and gadolinia-stabilized cubic zirconia, Zr0.79Gd0.14Pu0.07O1.93, doped with 238Pu

    NASA Astrophysics Data System (ADS)

    Burakov, B. E.; Yagovkina, M. A.

    2015-12-01

    Polycrystalline samples of cubic zirconia, Zr0.79Gd0.14Pu0.07O1.93, doped with approximately 9.9 wt.% 238Pu, and PuO2 containing 11.0 wt. % 238Pu (and main isotope is 239Pu) have been repeatedly studied during many years by X-ray diffraction analysis. At a temperature of 25 °C the unit-cell parameter of PuO2 increases depending on accumulated dose, and is accompanied by decrease of coherent scattering region (CSR). Self-irradiation of Zr0.79Gd0.14Pu0.07O1.93 is accompanied with repeated change of unit-cell parameter and CSR.

  13. Static Electric Dipole Polarizabilities of Tri- and Tetravalent U, Np, and Pu Ions

    SciTech Connect

    Parmar, Payal; Peterson, Kirk A.; Clark, Aurora E.

    2013-11-21

    High-quality static electric dipole polarizabilities have been determined for the ground states of the hard-sphere cations of U, Np, and Pu in the III and IV oxidation states. The polarizabilities have been calculated using the numerical finite field technique in a four-component relativistic framework. Methods including Fock-space coupled cluster (FSCC) and Kramers-restricted configuration interaction (KRCI) have been performed in order to account for electron correlation effects. Comparisons between polarizabilities calculated using Dirac-Hartree-Fock (DHF), FSCC, and KRCI methods have been made using both triple- and quadruple-ζ basis sets for U⁴⁺. In addition to the ground state, this study also reports the polarizability data for the first two excited states of U3+/4+, Np3+/4+, and Pu3+/4+ ions at different levels of theory. The values reported in this work are the most accurate to date calculations for the dipole polarizabilities of the hard-sphere tri- and tetravalent actinide ions and may serve as reference values, aiding in the calculation of various electronic and response properties (for example, intermolecular forces, optical properties, etc.) relevant to the nuclear fuel cycle and material science applications.

  14. Static electric dipole polarizabilities of tri- and tetravalent U, Np, and Pu ions.

    PubMed

    Parmar, Payal; Peterson, Kirk A; Clark, Aurora E

    2013-11-21

    High-quality static electric dipole polarizabilities have been determined for the ground states of the hard-sphere cations of U, Np, and Pu in the III and IV oxidation states. The polarizabilities have been calculated using the numerical finite field technique in a four-component relativistic framework. Methods including Fock-space coupled cluster (FSCC) and Kramers-restricted configuration interaction (KRCI) have been performed in order to account for electron correlation effects. Comparisons between polarizabilities calculated using Dirac-Hartree-Fock (DHF), FSCC, and KRCI methods have been made using both triple- and quadruple-ζ basis sets for U(4+). In addition to the ground state, this study also reports the polarizability data for the first two excited states of U(3+/4+), Np(3+/4+), and Pu(3+/4+) ions at different levels of theory. The values reported in this work are the most accurate to date calculations for the dipole polarizabilities of the hard-sphere tri- and tetravalent actinide ions and may serve as reference values, aiding in the calculation of various electronic and response properties (for example, intermolecular forces, optical properties, etc.) relevant to the nuclear fuel cycle and material science applications.

  15. Characterization of Nuclear Fuel using Multivariate Statistical Analysis

    SciTech Connect

    Robel, M; Robel, M; Robel, M; Kristo, M J; Kristo, M J

    2007-11-27

    Various combinations of reactor type and fuel composition have been characterized using principle components analysis (PCA) of the concentrations of 9 U and Pu isotopes in the 10 fuel as a function of burnup. The use of PCA allows the reduction of the 9-dimensional data (isotopic concentrations) into a 3-dimensional approximation, giving a visual representation of the changes in nuclear fuel composition with burnup. Real-world variation in the concentrations of {sup 234}U and {sup 236}U in the fresh (unirradiated) fuel was accounted for. The effects of reprocessing were also simulated. The results suggest that, 15 even after reprocessing, Pu isotopes can be used to determine both the type of reactor and the initial fuel composition with good discrimination. Finally, partial least squares discriminant analysis (PSLDA) was investigated as a substitute for PCA. Our results suggest that PLSDA is a better tool for this application where separation between known classes is most important.

  16. Pu and 137Cs in the Yangtze River estuary sediments: distribution and source identification.

    PubMed

    Liu, Zhiyong; Zheng, Jian; Pan, Shaoming; Dong, Wei; Yamada, Masatoshi; Aono, Tatsuo; Guo, Qiuju

    2011-03-01

    Pu isotopes and (137)Cs were analyzed using sector field ICP-MS and γ spectrometry, respectively, in surface sediment and core sediment samples from the Yangtze River estuary. (239+240)Pu activity and (240)Pu/(239)Pu atom ratios (>0.18) shows a generally increasing trend from land to sea and from north to south in the estuary. This spatial distribution pattern indicates that the Pacific Proving Grounds (PPG) source Pu transported by ocean currents was intensively scavenged into the suspended sediment under favorable conditions, and mixed with riverine sediment as the water circulated in the estuary. This process is the main control for the distribution of Pu in the estuary. Moreover, Pu is also an important indicator for monitoring the changes of environmental radioactivity in the estuary as the river basin is currently the site of extensive human activities and the sea level is rising because of global climate changes. For core sediment samples the maximum peak of (239+240)Pu activity was observed at a depth of 172 cm. The sedimentation rate was estimated on the basis of the Pu maximum deposition peak in 1963-1964 to be 4.1 cm/a. The contributions of the PPG close-in fallout Pu (44%) and the riverine Pu (45%) in Yangtze River estuary sediments are equally important for the total Pu deposition in the estuary, which challenges the current hypothesis that the riverine Pu input was the major source of Pu budget in this area.

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

    PubMed

    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.

  18. Soft tissue tumors induced by monomeric {sup 239}Pu

    SciTech Connect

    Lloyd, R.D.; Angus, W.; Taylor, G.N.; Miller, S.C.

    1995-10-01

    Individual records of soft tissue tumor occurrence (lifetime incidence) among 236 beagles injected with {sup 239}Pu citrate as young adults and 131 comparable control beagles given no radioactivity enabled us to analyze the possible effects on soft tissue tumor induction resulting from internal exposure to {sup 239}Pu. A significant trend was identified in the proportion of animals having malignant liver tumors with increasing radiation dose from {sup 239}. There was also a significant difference in the relative numbers of both malignant liver tumors (18.1 expected, 66 observed). Malignant tumors of the mouth, pancreas, and skin were more frequent among controls than among the dogs given {sup 239}Pu as well as tumors (malignant plus benign) of the mouth, pancreas, testis, and vagina. For all other tumor sites or types, there was no significant difference for both malignant and all (malignant plus benign) tumors. Mammary tumor occurrence appeared not to be associated with {sup 239}Pu incorporation. We conclude that the only soft-tissue neoplasia induced by the intake of {sup 239}Pu directly into blood is probably a liver tumor. 20 refs., 6 tabs.

  19. Measurements Conducted on an Unknown Object Labeled Pu-239

    SciTech Connect

    Hoteling, Nathan

    2013-11-18

    Measurements were carried out on 12 November 2013 to determine whether Pu-239 was present on an object discovered in a plastic bag with label “Pu-­239 6 uCi.” Following initial survey measurements to verify that the object was not leaking or contaminated, spectra were collected with a High Purity Germanium (HPGe) detector with object positioned in two different configurations. Analysis of the spectra did not yield any direct evidence of Pu-­239. From the measured spectra, minimum detectable activity (MDA) was determined to be approximately 2 uCi for the gamma-­ray measurements. Although there was no direct evidence of Pu-239, a peak at 60 keV characteristic of Am-­241 decay was observed. Since it is very likely that Am-­241 would be present in aged plutonium samples, this was interpreted as indirect evidence for the presence of plutonium on the object. Analysis of this peak led to an estimated Pu-­239 activity of 0.02–0.04 uCi, or <1x10-6 grams.

  20. Neutron Capture Cross Section Measurement on $^{238}$Pu at DANCE

    SciTech Connect

    Chyzh, A; Wu, C Y

    2011-02-14

    The proposed neutron capture measurement for {sup 238}Pu was carried out in Nov-Dec, 2010, using the DANCE array at LANSCE, LANL. The total beam-on-target time is about 14 days plus additional 5 days for the background measurement. The target was prepared at LLNL with the new electrplating cell capable of plating the {sup 238}Pu isotope simultaneously on both sides of the 3-{micro}m thick Ti backing foil. A total mass of 395 {micro}g with an activity of 6.8 mCi was deposited onto the area of 7 mm in diameter. The {sup 238}Pu sample was enriched to 99.35%. The target was covered by 1.4 {micro}m double-side aluminized mylar and then inserted into a specially designed vacuum-tight container, shown in Fig. 1, for the {sup 238}Pu containment. The container was tested for leaks in the vacuum chamber at LLNL. An identical container without {sup 238}Pu was made as well and used as a blank for the background measurement.

  1. Pulmonary Function in Flight (PuFF) Experiment

    NASA Technical Reports Server (NTRS)

    2003-01-01

    In this International Space Station (ISS) onboard photo, Expedition Six Science Officer Donald R. Pettit works to set up the Pulmonary Function in Flight (PuFF) experiment hardware in the Destiny Laboratory. Expedition Six is the fourth and final crew to perform the PuFF experiment. The PuFF experiment was developed to better understand what effects long term exposure to microgravity may have on the lungs. The focus is on measuring changes in the everness of gas exchange in the lungs, and on detecting changes in respiratory muscle strength. It allows astronauts to measure blood flow through the lungs, the ability of the lung to take up oxygen, and lung volumes. Each PuFF session includes five lung function tests, which involve breathing only cabin air. For each planned extravehicular (EVA) activity, a crew member performs a PuFF test within one week prior to the EVA. Following the EVA, those crew members perform another test to document the effect of exposure of the lungs to the low-pressure environment of the space suits. This experiment utilizes the Gas Analyzer System for Metabolic Analysis Physiology, or GASMAP, located in the Human Research Facility (HRF), along with a variety of other Puff equipment including a manual breathing valve, flow meter, pressure-flow module, pressure and volume calibration syringes, and disposable mouth pieces.

  2. Combined effects of Fe(II) and oxidizing radiolysis products on UO2 and PuO2 dissolution in a system containing solid UO2 and PuO2

    NASA Astrophysics Data System (ADS)

    Amme, Marcus; Pehrman, Reijo; Deutsch, Rudolf; Roth, Olivia; Jonsson, Mats

    2012-11-01

    The stability of UO2 spent nuclear fuel in an oxygen-free geological repository depends on the absence of oxidizing reaction partners in the near field. This work investigates the reactions between the products of water radiolysis by alpha radiation and Fe(II) an the effect on UO2 dissolution. Solid 238PuO2 powder and UO2 pellet were allowed to react in Fe(II) solution in oxygen-free batch reactor tests and kinetics of the subsequent redox reactions were measured. Depending on the concentration of Fe(II) (tests with 10-5 and 10-4 mol L-1 were made), the induced redox reactions took place between 20 and 400 h. Dissolved uranium concentrations went first through a minimum caused by reduction, followed by a maximum caused by radiolytic oxidation, and eventually reached another minimum, probably due to sorption on precipitated Fe(III). Plutonium concentrations were decreasing steadily after going through a maximum about 70 h from the start of the experiments. The results show that in the presence of the strong alpha-radiolytic field induced by the presence of solid 238Pu, the behavior of the system is largely governed by Fe(II) as it controls the H2O2 concentration, reduces U(VI) in solution and drives the Fenton reaction leading to the oxidation of Pu(IV).

  3. Out-of-pile chemical compatibility of hyperstoichiometric (Pu 0.7U 0.3)C with stainless steel cladding and sodium coolant

    NASA Astrophysics Data System (ADS)

    Ganguly, C.; Sengupta, A. K.

    1988-09-01

    Chemical compatibility experiments of the hitherto unknown fuel (Pu 0.7U 0.3)C 1+xwith sodium coolant and SS 316 (20% cold-worked) cladding were carried out at 973 K for 1000 h for its out-of-pile 'proof testing'. Any possible chemical interaction was assessed by metallographic examination and microhardness measurements of SS 316 cladding specimens. Hyperstoichiometric (Pu 0.7U 0.3)C containing upto 0.7% oxygen and 20% mixed sesquicarbide (M 2C 3) did not interact at all with sodium and caused insignificant carburization of the SS 316 cladding. Mixed carbide pellets containing high 'O' (~ 1%) and high M 2C 3(~ 60%) caused clad carburization to a depth of around 90 μm. These experiments generated valuable informations in support of choosing plutonium rich mixed carbide as the driver fuel for the fast breeder test reactor (FBTR).

  4. The inflow of 238Pu and (239+240)Pu from the Odra and Pomeranian rivers catchments area to the Baltic Sea.

    PubMed

    Strumińska-Parulska, Dagmara I; Skwarzec, Bogdan; Tuszkowska, Agnieszka

    2012-11-01

    The aim of the work was to estimate plutonium inflow from the Odra River catchments area to the Baltic Sea. The highest activities of (238)Pu and (239+240)Pu were observed in a winter and a spring season. The highest annual surface inflow of (239+240)Pu from the Odra River watershed was observed for a mountain tributary the Bóbr (1230 Bq km(-2) year(-1)). The annual inflow of (238)Pu and (239+240)Pu to the Baltic Sea was estimated at 9.51 MBq and 45.86 MBq respectively and the highest plutonium surface runoff was observed for the Bóbr drainage.

  5. Characterization of Pu concentration and its isotopic composition in a reference fallout material.

    PubMed

    Zhang, Yongsan; Zheng, Jian; Yamada, Masatoshi; Wu, Fengchang; Igarashi, Yasuhito; Hirose, Katsumi

    2010-02-01

    Because there is no reference material for fallout plutonium isotope monitoring, preparation of such a material is necessary for quality control of fallout radionuclides analysis for atmospheric environmental studies. In this work, we report the characterization of Pu activity and its isotopic composition in a reference fallout material prepared by the Meteorological Research Institute (MRI), Japan. This material was prepared from samples collected at 14 stations throughout Japan in 1963-1979, with reference values of (137)Cs, (90)Sr and (239)(+)(240)Pu activities. We analyzed the activities of (239)(+)(240)Pu and (241)Pu, and the atom ratios of (240)Pu/(239)Pu and (241)Pu/(239)Pu using an isotope dilution sector-field inductively coupled plasma mass spectrometry (SF-ICP-MS). The (239)(+)(240)Pu activities in this fallout material using acid leaching and total digestion were 6.56+/-0.20 mBq/g and 6.79+/-0.16 mBq/g, respectively. Atom ratios of (240)Pu/(239)Pu were 0.1915+/-0.0030 and 0.1922+/-0.0044, respectively. Both (240)Pu/(239)Pu and (241)Pu/(239)Pu atom ratios were slightly higher than those of global fallout, which could be attributed to the deposition of fallout radionuclides resulting from the Chinese nuclear weapons tests conducted in the 1970s. The dominant host phases of (239)(+)(240)Pu were found to be organic matter-sulfides (70%) with a relative high (240)Pu/(239)Pu atom ratio, and Fe-Mn oxides (19%) using a sequential extraction method.

  6. Spent fuel temperature and age determination from the analysis of uranium and plutonium isotopics

    SciTech Connect

    Scott, Mark R; Eccleston, George W; Bedell, Jeffrey J; Lockard, Chanelle M

    2009-01-01

    The capability to determine the age (time since irradiation) of spent fuel can be useful for verification and safeguards. While the age of spent fuel can be determined based on measurements of short-lived fission products, these measurements are not routinely done nor generally reported. As an alternative, age can also be determined if the uranium (U) and plutonium (Pu) isotopic values are available. Uranium isotopics are not strongly affected by fuel temperature, and bumup is determined from the {sup 235}U and {sup 236}U isotopic values. Age is calculated after estimating the {sup 241}Pu at the end of irradiation while accounting for the fuel temperature, which is determined from {sup 239}Pu or {sup 240}Pu. Burnup and age determinations are calibrated to reactor models that provide uranium and plutonium isotopics over the range of fuel irradiation. The reactor model must contain sufficient fidelity on details of the reactor type, fuel burnup, irradiation history, initial fuel enrichment and fuel temperature to obtain accurate isotopic calculations. If the latter four are unknown, they can be derived from the uranium and plutonium isotopics. Fuel temperature has a significant affect on the production of plutonium isotopics; therefore, one group cross section reactor models, such as ORIGEN, cannot be used for these calculations. Multi-group cross section set codes, such as Oak Ridge National Laboratory's TRITON code, must be used.

  7. Thorium-Based Transmuter Fuels for Light Water Reactors

    SciTech Connect

    J. Stephen Herring; P. E. MacDonald; K. Weaver

    2004-04-01

    A light water reactor (LWR) fuel cycle is proposed where the reactor core mainly consists of standard uranium-dioxide (UO2) fuel rods with typical 235U enrichment, along with thoria-urania (ThO2-UO2) or yttria-stablized zirconia fertile-free fuel rods containing the plutonium and minor actinides typical of 30-yr old UO2 fuel in 1/9 to 1/3 of the positions. The goals of this mono-recycling strategy or "twice through fuel cycle" are to transmute the great majority of the long lived actinides in existing LWRs and to discharge a fuel form that is a very robust waste form and whose isotopic content is very proliferation resistant. The incorporation of plutonium into a ThO2 or yttria-stablized zirconia fertile-free matrix results in the consumption of already-separated plutonium without breeding significant additional 239Pu. The minor actinides (i.e., neptunium, americium, curium, berkelium, californium, etc.) are also included in the ThO2 or fertile-free transmuter fuel rods to further reduce the overall long-term radiotoxicity of the fuel cycle. Our analyses have shown that thorium-based or fertile-free fuels can reduce the amount of 239Pu needing further transmutation or going to a repository by ~90%. Also, thorium-based fuels produce a mixture of plutonium isotopes high in 238Pu. Because of the high decay heat and spontaneous neutron generation of 238Pu, this isotope provides intrinsic proliferation resistance.

  8. Thorium-Based Transmuter Fuels for Light Water Reactors

    SciTech Connect

    Herring, J. Stephen; MacDonald, Philip E.; Weaver, Kevan D.

    2004-07-15

    A light water reactor (LWR) fuel cycle is proposed where the reactor core mainly consists of standard uranium-dioxide (UO{sub 2}) fuel rods with typical {sup 235}U enrichment, along with thoria-urania (ThO{sub 2}-UO{sub 2}) or yttria-stablized zirconia fertile-free fuel rods containing the plutonium and minor actinides typical of 30-yr old UO{sub 2} fuel in 1/9 to 1/3 of the positions. The goals of this mono-recycling strategy or 'twice through fuel cycle' are to transmute the great majority of the long lived actinides in existing LWRs and to discharge a fuel form that is a very robust waste form and whose isotopic content is very proliferation resistant. The incorporation of plutonium into a ThO{sub 2} or yttria-stablized zirconia fertile-free matrix results in the consumption of already-separated plutonium without breeding significant additional {sup 239}Pu. The minor actinides (i.e., neptunium, americium, curium, berkelium, californium, etc.) are also included in the ThO{sub 2} or fertile-free transmuter fuel rods to further reduce the overall long-term radiotoxicity of the fuel cycle. Our analyses have shown that thorium-based or fertile-free fuels can reduce the amount of {sup 239}Pu needing further transmutation or going to a repository by {approx}90%. Also, thorium-based fuels produce a mixture of plutonium isotopes high in {sup 238}Pu. Because of the high decay heat and spontaneous neutron generation of {sup 238}Pu, this isotope provides intrinsic proliferation resistance.

  9. An evaluation of alternate production methods for Pu-238 general purpose heat source pellets

    SciTech Connect

    Mark Borland; Steve Frank

    2009-06-01

    For the past half century, the National Aeronautics and Space Administration (NASA) has used Radioisotope Thermoelectric Generators (RTG) to power deep space satellites. Fabricating heat sources for RTGs, specifically General Purpose Heat Sources (GPHSs), has remained essentially unchanged since their development in the 1970s. Meanwhile, 30 years of technological advancements have been made in the applicable fields of chemistry, manufacturing and control systems. This paper evaluates alternative processes that could be used to produce Pu 238 fueled heat sources. Specifically, this paper discusses the production of the plutonium-oxide granules, which are the input stream to the ceramic pressing and sintering processes. Alternate chemical processes are compared to current methods to determine if alternative fabrication processes could reduce the hazards, especially the production of respirable fines, while producing an equivalent GPHS product.

  10. ICE1 of Pyrus ussuriensis functions in cold tolerance by enhancing PuDREBa transcriptional levels through interacting with PuHHP1

    NASA Astrophysics Data System (ADS)

    Huang, Xiaosan; Li, Kongqing; Jin, Cong; Zhang, Shaoling

    2015-12-01

    ICE1 transcription factor plays an important role in plant cold stress via regulating the expression of stress-responsive genes. In this study, a PuICE1 gene isolated from Pyrus ussuriensis was characterized for its function in cold tolerance. The expression levels of the PuICE1 were induced by cold, dehydration and salt, with the greatest induction under cold conditions. PuICE1 was localized in the nucleus and could bind specifically to the MYC element in the PuDREBa promoter. The PuICE1 fused to the GAL4 DNA-binding domain to have transcriptional activation activity. Ectopic expression of the PuICE1 in tomato conferred enhanced tolerance to cold stress at cold temperatures, less electrolyte leakage, less MDA content, higher chlorophyll content, higher survival rate, higher proline content, higher activities of enzymes. In additon, steady-state mRNA levels of six stress-responsive genes coding for either functional or regulatory genes were induced to higher levels in the transgenic lines by cold stress. Yeast two-hybrid, transient assay, split luciferase complementation and BiFC assays all revealed that PuHHP1 protein can physically interact with PuICE1. Taken together, these results demonstrated that PuICE1 plays a positive role in cold tolerance, which may be due to enhancement of PuDREBa transcriptional levels through interacting with the PuHHP1.

  11. Formation of crystalline PuO2+x·nH2O nanoparticles upon sorption of Pu(V,VI) onto hematite

    NASA Astrophysics Data System (ADS)

    Romanchuk, Anna Yu.; Kalmykov, Stepan N.; Egorov, Alexander V.; Zubavichus, Yan V.; Shiryaev, Andrey A.; Batuk, Olga N.; Conradson, Steven D.; Pankratov, Denis A.; Presnyakov, Igor A.

    2013-11-01

    It has been recognized that natural aquatic colloids can readily sorb actinide elements, including plutonium, whose behavior is complicated by its multiple valence states and the possibility of redox reactions under environmental conditions. In this paper, the sorption and surface-mediated redox transformations of hexavalent plutonium on synthetic well-characterized hematite colloids are studied in a series of batch sorption experiments. The variation in the kinetics of the Pu-hematite interactions, Pu-L3-XAFS, and HRTEM over a broad range of total concentrations of Pu have been studied in an attempt to define the molecular-level speciation of Pu. The surface-mediated slow reduction of Pu(V/VI) results in the formation of crystalline nanoparticles of PuO2+x·nH2O approximately 1.5 nm in size at [Pu]tot ⩾ 10-9 M. This result is confirmed independently by HRTEM images of Pu-containing particles and through the identification in the EXAFS of a Pu neighbor shell at 3.8 Å. The formation of such nanoparticles potentially influences the colloid-mediated transport of Pu in the subsurface environment because of the very slow leaching of Pu from the hematite colloids.

  12. ICE1 of Pyrus ussuriensis functions in cold tolerance by enhancing PuDREBa transcriptional levels through interacting with PuHHP1

    PubMed Central

    Huang, Xiaosan; Li, Kongqing; Jin, Cong; Zhang, Shaoling

    2015-01-01

    ICE1 transcription factor plays an important role in plant cold stress via regulating the expression of stress-responsive genes. In this study, a PuICE1 gene isolated from Pyrus ussuriensis was characterized for its function in cold tolerance. The expression levels of the PuICE1 were induced by cold, dehydration and salt, with the greatest induction under cold conditions. PuICE1 was localized in the nucleus and could bind specifically to the MYC element in the PuDREBa promoter. The PuICE1 fused to the GAL4 DNA-binding domain to have transcriptional activation activity. Ectopic expression of the PuICE1 in tomato conferred enhanced tolerance to cold stress at cold temperatures, less electrolyte leakage, less MDA content, higher chlorophyll content, higher survival rate, higher proline content, higher activities of enzymes. In additon, steady-state mRNA levels of six stress-responsive genes coding for either functional or regulatory genes were induced to higher levels in the transgenic lines by cold stress. Yeast two-hybrid, transient assay, split luciferase complementation and BiFC assays all revealed that PuHHP1 protein can physically interact with PuICE1. Taken together, these results demonstrated that PuICE1 plays a positive role in cold tolerance, which may be due to enhancement of PuDREBa transcriptional levels through interacting with the PuHHP1. PMID:26626798

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

    PubMed

    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.

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

    DTIC Science & Technology

    2008-01-20

    reprocessing is currently conducted in France, Britain, and Russia. The 239Pu they produce is blended with uranium to make mixed- oxide ( MOX ) fuel, in which...Association, Mixed Oxide Fuel ( MOX ), November 2006, at [http://www.world-nuclear.org/info/inf29.html]. 53 World Nuclear Association, Uranium Markets, March...older plants to reprocess gas-cooled reactor fuel, and India has a 275-ton plant.51 About 200 metric tons of MOX fuel is used annually, about 2% of

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

    SciTech Connect

    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.

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

    NASA Astrophysics Data System (ADS)

    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).

  17. Determination of Plutonium Activity Concentrations and 240Pu/239Pu Atom Ratios in Brown Algae (Fucus distichus) Collected from Amchitka Island, Alaska.

    SciTech Connect

    Hamilton, T F; Brown, T A; Marchetti, A A; Martinelli, R E; Kehl, S R

    2005-05-02

    Plutonium-239 ({sup 239}Pu) and plutonium-240 ({sup 240}Pu) activity concentrations and {sup 240}Pu/{sup 239}Pu atom ratios are reported for Brown Algae (Fucus distichus) collected from the littoral zone of Amchitka Island (Alaska) and at a control site on the Alaskan peninsula. Plutonium isotope measurements were performed in replicate using Accelerator Mass Spectrometry (AMS). The average {sup 240}Pu/{sup 239}Pu atom ratio observed in dried Fucus d. collected from Amchitka Island was 0.227 {+-} 0.007 (n=5) and compares with the expected {sup 240}Pu/{sup 239}Pu atom ratio in integrated worldwide fallout deposition in the Northern Hemisphere of 0.1805 {+-} 0.0057 (Cooper et al., 2000). In general, the characteristically high {sup 240}Pu/{sup 239}Pu content of Fucus d. analyzed in this study appear to indicate the presence of a discernible basin-wide secondary source of plutonium entering the marine environment. Of interest to the study of plutonium source terms within the Pacific basin are reports of elevated {sup 240}Pu/{sup 239}Pu atom ratios in fallout debris from high-yield atmospheric nuclear tests conducted in the Marshall Islands during the 1950s (Diamond et al., 1960), the wide range of {sup 240}Pu/{sup 239}Pu atom ratio values (0.19 to 0.34) observed in sea water, sediments, coral and other environmental media from the North Pacific Ocean (Hirose et al., 1992; Buesseler, 1997) and updated estimates of the relative contributions of close-in and intermediate fallout deposition on oceanic inventories of radionuclidies, especially in the Northern Pacific Ocean (Hamilton, 2004).

  18. Economical Production of Pu-238: NIAC Phase I Final Report

    NASA Technical Reports Server (NTRS)

    Howe, Steven D.; Crawford, Douglas; Navarro, Jorge; O'Brien, Robert C.; Katalenich, Jeff; Ring, Terry

    2016-01-01

    All space exploration missions traveling beyond Jupiter must use radioisotopic power sources for electrical power. The best isotope to power these sources is plutonium-238 (Pu-238). The US supply of Pu-238 is almost exhausted and will be gone within the next decade. The Department of Energy has initiated a production program with a $10M allocation from NASA but the cost is estimated at over $100M to get to production levels. The Center for Space Nuclear Research (CSNR) has conceived of a potentially better process to produce Pu-238 earlier and for significantly less cost. Potentially, the front end capital costs could be provided by private industry such that the government only had to pay for the product produced. In the Phase I NIAC (NASA Innovative Advanced Concepts) grant, the CSNR has evaluated the feasibility of using a low power, commercially available nuclear reactor to produce 1.5 kg of Pu-238 per year. The impact on the neutronics of the reactor have been assessed, the amount of Neptunium target material estimated, and the production rates calculated. In addition, the size of the post-irradiation processing facility has been established. Finally, as the study progressed, a new method for fabricating the Pu-238 product into the form used for power sources has been identified to reduce the cost of the final product. In short, the concept appears to be viable, can produce the amount of Pu-238 needed to support the NASA missions, can be available within a few years, and will cost significantly less than the current DOE program.

  19. Neutron radiation characteristics of plutonium dioxide fuel

    NASA Technical Reports Server (NTRS)

    Taherzadeh, M.

    1972-01-01

    The major sources of neutrons from plutonium dioxide nuclear fuel are considered in detail. These sources include spontaneous fission of several of the Pu isotopes, (alpha, n) reactions with low Z impurities in the fuel, and (alpha, n) reactions with O-18. For spontaneous fission neutrons a value of (1.95 + or - 0.07) X 1,000 n/s/g PuO2 is obtained. The neutron yield from (alpha, n) reactions with oxygen is calculated by integrating the reaction rate equation over all alpha-particle energies and all center-of-mass angles. The results indicate a neutron emission rate of (1.14 + or - 0.26) X 10,000 n/s/g PuO2. The neutron yield from (alpha, n) reactions with low Z impurities in the fuel is presented in tabular form for one part part per million of each impurity. The total neutron yield due to the combined effects of all the impurities depends upon the fractional weight concentration of each impurity. The total neutron flux emitted from a particular fuel geometry is estimated by adding the neutron yield due to the induced fission to the other neutron sources.

  20. Complexation of Pu(IV) with the natural siderophore desferrioxamine B and the redox properties of Pu(IV)(siderophore) complexes.

    PubMed

    Boukhalfa, Hakim; Reilly, Sean D; Neu, Mary P

    2007-02-05

    The bioavailability and mobility of Pu species can be profoundly affected by siderophores and other oxygen-rich organic ligands. Pu(IV)(siderophore) complexes are generally soluble and may constitute with other soluble organo-Pu(IV) complexes the main fraction of soluble Pu(IV) in the environment. In order to understand the impact of siderophores on the behavior of Pu species, it is important to characterize the formation and redox behavior of Pu(siderophore) complexes. In this work, desferrioxamine B (DFO-B) was investigated for its capacity to bind Pu(IV) as a model siderophore and the properties of the complexes formed were characterized by optical spectroscopy measurements. In a 1:1 Pu(IV)/DFO-B ratio, the complexes Pu(IV)(H2DFO-B)4+, Pu(IV)(H1DFO-B)3+, Pu(IV)(DFO-B)2+, and Pu(IV)(DFO-B)(OH)+ form with corresponding thermodynamic stability constants log beta1,1,2 = 35.48, log beta1,1,1 = 34.87, log beta1,1,0 = 33.98, and log beta1,1,-1 = 27.33, respectively. In the presence of excess DFO-B, the complex Pu(IV)H2(DFO-B)22+ forms with the formation constant log beta2,1,2 = 62.30. The redox potential of the complex Pu(IV)H2(DFO-B)22+ was determined by cyclic voltammetry to be E1/2 = -0.509 V, and the redox potential of the complex Pu(IV)(DFO-B)2+ was estimated to be E1/2 = -0.269 V. The redox properties of Pu(IV)(DFO-B)2+ complexes indicate that Pu(III)(siderophore) complexes are more than 20 orders of magnitude less stable than their Pu(IV) analogues. This indicates that under reducing conditions, stable Pu(siderophore) complexes are unlikely to persist.

  1. Radiation dose aspects in the handling of emerging nuclear fuels.

    PubMed

    Nicolaou, G

    2014-12-01

    The occupational annual dose levels, encountered at fabrication of emerging nuclear fuels, have been studied. Emerging fuels for the single and multiple recycling of Pu and MA have resulted in considerably higher gamma and neutron doses in comparison with commercial fuels. The occupational dose limit is exceeded at fabrication by a single fuel rod in all fuel cases with (241)Am and Cm isotopes present in their composition. In the absence of these isotopes, 2-4 adjacent fuel rods are sufficient to exceed the limit. Self-shielding within the fuel reduces significantly only the gamma dose that would have been delivered otherwise. Hence, only the first row of fuel rods in an assembly contributes to the dose, whereas in the case of neutrons, all fuel rods contribute.

  2. Reductive Disslocation of Pu(IV) by Clostridium sp. Under Anaerobic Conditions

    SciTech Connect

    Francis,A.; Dodge, C.; Gillow, J.

    2008-01-01

    An anaerobic, gram positive, spore-forming bacterium Clostridium sp., common in soils and wastes, capable of reduction of Fe(III) to Fe(II), Mn(IV) to Mn(II), Tc(VII) to Tc(IV), and U(VI) to U(IV), reduced Pu(IV) to Pu(III). Addition of 242Pu (IV)-nitrate to the bacterial growth medium at pH 6.4 resulted in the precipitation of Pu as amorphous Pu(OH)4 due to hydrolysis and polymerization reactions. The Pu (1 x 10-5 M) had no effect upon growth of the bacterium as evidenced by glucose consumption; carbon dioxide and hydrogen production; a decrease in pH of the medium from 6.4 to 3.0 due to production of acetic and butyric acids from glucose fermentation; and a change in the Eh of the culture medium from +50 to -180 mV. Commensurate with bacterial growth, Pu was rapidly solubilized as evidenced by an increase in Pu concentration in solution which passed through a 0.03 {mu}m filtration. Selective solvent extraction of the culture by thenoyltrifluoroacetone (TTA) indicated the presence of a reduced Pu species in the soluble fraction. X-ray absorption near edge spectroscopic (XANES) analysis of Pu in the culture sample at the Pu LIII absorption edge (18.054 keV) showed a shift of -3 eV compared to a Pu(IV) standard indicating reduction of Pu(IV) to Pu(III). These results suggest that, although Pu generally exists as insoluble Pu(IV) in the environment, under appropriate conditions, anaerobic microbial activity could affect the long-term stability and mobility of Pu by its reductive dissolution.

  3. Thermal conductivity of (Np0.20Pu0.50Am0.25Cm0.05)O2-x solid solutions

    NASA Astrophysics Data System (ADS)

    Nishi, Tsuyoshi; Takano, Masahide; Akabori, Mitsuo; Arai, Yasuo

    2013-09-01

    recovery behavior by annealing. The thermal conductivity of (Np0.20Pu0.50Am0.25Cm0.05)O2-x was smaller than those of PuO2 and (Pu0.91Cm0.09)O2 mainly because of the oxygen vacancies as is seen other actinide dioxide, such as mixed oxide (MOX) fuels.

  4. PLUTONIUM METALLIC FUELS FOR FAST REACTORS

    SciTech Connect

    STAN, MARIUS; HECKER, SIEGFRIED S.

    2007-02-07

    Early interest in metallic plutonium fuels for fast reactors led to much research on plutonium alloy systems including binary solid solutions with the addition of aluminum, gallium, or zirconium and low-melting eutectic alloys with iron and nickel or cobalt. There was also interest in ternaries of these elements with plutonium and cerium. The solid solution and eutectic alloys have most unusual properties, including negative thermal expansion in some solid-solution alloys and the highest viscosity known for liquid metals in the Pu-Fe system. Although metallic fuels have many potential advantages over ceramic fuels, the early attempts were unsuccessful because these fuels suffered from high swelling rates during burn up and high smearing densities. The liquid metal fuels experienced excessive corrosion. Subsequent work on higher-melting U-PuZr metallic fuels was much more promising. In light of the recent rebirth of interest in fast reactors, we review some of the key properties of the early fuels and discuss the challenges presented by the ternary alloys.

  5. Evidence of extinct 244Pu in ancient terrestrial zircons

    NASA Astrophysics Data System (ADS)

    Harrison, T. M.; Turner, G.; Holland, G.; Gilmour, J. D.; Mojzsis, S. J.

    2003-04-01

    The Pu/U ratio of the early Earth is an important parameter in models of mantle evolution based on noble gas isotopes. Current estimates assume the Earth accreted with a chondritic Pu/U and are based on analyses of the chondrite St Severin and the achondrite Angra dos Reis. These estimates are poorly constrained, ranging from 0.004 to 0.008. On account of its short, 82 Ma, half-life, 244Pu was essentially extinct 3,900 Ma ago, and consequently there exists no reliable measurement of Pu/U for the Earth. The discovery of zircons dating from the period when 244Pu was "live" offers the first opportunity to measure the former terrestrial abundance of 244Pu directly. Xenon isotopes are produced by spontaneous fission and, in principle, are readily distinguishable from those produced by 238U-fission (e.g. 131Xe/136Xe = 0.24 and 0.08 respectively). However the expected levels of fission xenon in individual zircons, weighing 1 - 2 μg and containing 100 - 200 ppm U, are below, or at best comparable to, the Xe blank levels (˜10-15 ccSTP) typical of conventional noble gas mass spectrometers. In order to analyse these minute amounts of xenon we have made use of a uniquely sensitive instrument, developed in Manchester, based on the principle of laser resonance ionisation. RELAX (Refrigerator Enhanced Laser Analyser for Xenon) is capable of analysing samples of only a few thousand atoms, some two orders of magnitude smaller than conventional mass spectrometers. We have carried out preliminary analyses of 4 individual 4,150 Ma zircons and one 3,600 Ma zircon from Jack Hills, Western Australia, and obtained five clear fission spectra. All but one were essentially free from significant atmospheric blank (the average 130Xe blank was 3× 10-18 ccSTP, i.e. 80 atoms). The spectra of the older zircons clearly demonstrated the presence of varying amounts of 244Pu fission xenon. The highest 131Xe/136Xe, 0.136 ± 0.003, corresponds to an initial Pu/U ratio of 0.0057. The lower ratios

  6. Biogeochemical Cycling and Environmental Stability of Pu Relevant to Long-Term Stewardship of DOE Sites

    SciTech Connect

    Santschi, Peter H.

    2006-06-01

    The overall objective of this proposed research is to understand the biogeochemical cycling of Pu in environments of interest to long-term DOE stewardship issues. Central to Pu cycling (transport initiation to immobilization) is the role of microorganisms. The hypothesis underlying this proposal is that microbial activity is the causative agent in initiating the mobilization of Pu in near-surface environments: through the transformation of Pu associated with solid phases, production of extracellular polymeric substances (EPS) carrier phases, and the creation of microenvironments. Also, microbial processes are central to the immobilization of Pu species, through the metabolism of organically complexed Pu species and Pu associated with extracellular carrier phases and the creation of environments favorable for Pu transport retardation.

  7. Global fallout Pu recorded in lacustrine sediments in Lake Hongfeng, SW China.

    PubMed

    Zheng, Jian; Wu, Fengchang; Yamada, Masatoshi; Liao, Haiqing; Liu, Congqiang; Wan, Guojiang

    2008-03-01

    Studies on the distribution and isotope compositions of fallout Pu are important for source characterization of possible future non-fallout Pu contamination in aquatic environments, and useful for dating of recent sediments to understand the pollution history of environmental contaminants. We present the historical record of atmospheric Pu fallout reconstructed from a sediment core from Lake Hongfeng, China. The Pu activity profile was in agreement with the 137Cs profile. Inventories were 50.7 Bq m(-2) for 239+240Pu and 1586 Bq m(-2) for 137Cs. The average 240Pu/239Pu atom ratio was 0.185+/-0.009, indicating that Pu originated from global stratospheric fallout rather than from direct tropospheric or close-in fallout from the Chinese nuclear testing conducted in the 1970s. Our data suggested that Lake Hongfeng would be an ideal setting for monitoring atmospheric fallout and environmental changes in this region.

  8. Biogeochemical Cycling and Environmental Stability of Pu Relevant to Long-Term Stewardship of DOE Sites

    SciTech Connect

    Honeyman, Bruce D.; Francis, A.J.; Gillow, Jeffrey B.; Dodge, Cleveland J.; Santschi, Peter H.; Chin-Chang Hung; Diaz, Angelique; Tinnacher, Ruth; Roberts, Kimberly; Schwehr, Kathy

    2006-04-05

    The overall objective of this research is to understand the biogeochemical cycling of Pu in environments of interest to long-term DOE stewardship issues. Central to Pu cycling (transport initiation and immobilization) is the role of microorganisms. The hypothesis underlying this work is that microbial activity is the causative agent in initiating the mobilization of Pu in near-surface environments: through the transformation of Pu associated with solid phases, production of extracellular polymeric substances (EPS) carrier phases and the creation of microenvironments. Also, microbial processes are central to the immobilization of Pu species, through the metabolism of organically complexed Pu species and Pu associated with extracellular carrier phases and the creation of environments favorable for Pu transport retardation.

  9. Biogeochemical Cycling and Environmental Stability of Pu Relevant to Long-Term Stewardship of DOE Sites

    SciTech Connect

    Francis, Arokiasamy J.; Santschi, Peter H.; Honeyman, Bruce D.

    2005-06-01

    The overall objective of this proposed research is to understand the biogeochemical cycling of Pu in environments of interest to long-term DOE stewardship issues. Central to Pu cycling (transport initiation to immobilization) is the role of microorganisms. The hypothesis underlying this proposal is that microbial activity is the causative agent in initiating the mobilization of Pu in near-surface environments: through the transformation of Pu associated with solid phases, production of extracellular polymeric substances (EPS) carrier phases, and the creation of microenvironments. Also, microbial processes are central to the immobilization of Pu species, through the metabolism of organically complexed Pu species and Pu associated with extracellular carrier phases and the creation of environments favorable for Pu transport retardation.

  10. XAFS and LIBD Investigation of the Formation and Structure of Pu(IV) Hydrolysis Products

    SciTech Connect

    Rothe, J.; Walther, C.; Denecke, M.A.; Fanghänel, Th.

    2010-11-16

    Pu(IV) oxyhydroxide colloid growth is investigated with XAFS and LIBD. From combined results a model of colloid formation is proposed, which leads to a face-centered cubic Pu sublattice having cation defects, as observed with EXAFS, and a linear dependency of log [Pu(IV)] on -log [H{sup +}] with slope -2, in accord with LIBD. The solubility for Pu(IV) measured with LIBD is close to the lower limit of the solubility curve from previously reported data.

  11. Analysis of thorium-salted fuels to improve uranium utilization in the once-through fuel cycle

    SciTech Connect

    Eschbach, E.A.; Merrill, E.T.; Prichard, A.W.

    1981-09-01

    Calculations and analyses indicate that no improvement can be achieved in uranium utilization for the once-through LWR fuel cycle over use of slightly enriched uranium by employing thorium distributed with uranium. The study included thorium additions: (1) slight amounts, (2) larger amounts, in either intimately mixed or in duplex pellets, (3) in spectrally shifted or not spectrally shifted reactors, and (4) in three- or five-year reactivity limited exposures. While thorium-uranium combinations improves the initial conversion ratio, the reactivity lifetime was not extended enough to override the additional uranium required. The effective fission cross-section of the bred /sup 233/U relative to /sup 239/Pu's in typical LWR neutron spectra is not large enough for /sup 233/U to make as great a contribution to end-of-life reactivity as /sup 239/Pu in a slightly enriched uranium fuel element. /sup 233/U's reactivity contribution relative to /sup 239/Pu's is lower in fuel configurations such as slightly enriched uranium LWR fuel loads. On the other hand, /sup 233/U's reactivity contribution appears more positive for reactors that involve lower average concentrations of thermal neutron absorbers. If /sup 238/U-thorium fuels reprocessed, the recovered /sup 233/U would increase uranium utilization, but may not reduce fuel cycle costs. The thorium-salted fuels exhibit substantially flatter reactivity characteristics with exposure time. Spectral shift helped the utilization of uranium and thorium.

  12. Fuel clad chemical interactions in fast reactor MOX fuels

    NASA Astrophysics Data System (ADS)

    Viswanathan, R.

    2014-01-01

    Clad corrosion being one of the factors limiting the life of a mixed-oxide fast reactor fuel element pin at high burn-up, some aspects known about the key elements (oxygen, cesium, tellurium, iodine) in the clad-attack are discussed and many Fuel-Clad-Chemical-Interaction (FCCI) models available in the literature are also discussed. Based on its relatively superior predictive ability, the HEDL (Hanford Engineering Development Laboratory) relation is recommended: d/μm = ({0.507 ṡ [B/(at.% fission)] ṡ (T/K-705) ṡ [(O/M)i-1.935]} + 20.5) for (O/M)i ⩽ 1.98. A new model is proposed for (O/M)i ⩾ 1.98: d/μm = [B/(at.% fission)] ṡ (T/K-800)0.5 ṡ [(O/M)i-1.94] ṡ [P/(W cm-1)]0.5. Here, d is the maximum depth of clad attack, B is the burn-up, T is the clad inner surface temperature, (O/M)i is the initial oxygen-to-(uranium + plutonium) ratio, and P is the linear power rating. For fuels with [n(Pu)/n(M = U + Pu)] > 0.25, multiplication factors f are recommended to consider the potential increase in the depth of clad-attack.

  13. 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.

    PubMed

    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.

  14. Selection and Evaluation of a new Pu Density Measurement Fluid

    SciTech Connect

    Dziewinska, Krystyna; Peters, Michael A; Martinez, Patrick P; Dziewinski, Jacek J; Pugmire, David L; Trujillo, Stephen M; La Verne, Jake A; Rajesh, P

    2009-01-01

    This paper summarizes efforts leading to selection of a new fluid for the determination of the density of large Pu parts. Based on an extended literature search, perfluorotributylamine (FC-43) was chosen for an experimental study. Plutonium coupon corrosion studies were performed by exposing Pu to deaerated and aerated solutions and measuring corrosion gravimetrically. Corrosion rates were determined. Samples of deaerated and aerated perfuluorotributylamine (FC-43) were also irradiated with {sup 60}Co gamma rays (96 Gy/min) to various doses. The samples were extracted with NaOH and analyzed by IC and showed the presence of F and Cl{sup -}. The G-values were established. In surface study experiments Pu coupons were exposed to deaerated and aerated solutions of FC-43 and analyzed by X-ray photoelectron spectroscopy (XPS). The XPS data indicate that there is no detectable surface effect caused by the new fluid. In conclusion the FC-43 was determined to be a very effective and practical fluid for Pu density measurements.

  15. Fractionation of (137)Cs and Pu in natural peatland.

    PubMed

    Mihalík, Ján; Bartusková, Miluše; Hölgye, Zoltán; Ježková, Tereza; Henych, Ondřej

    2014-08-01

    High Cs-137 concentrations in plants growing on peatland inspired us to investigate the quantity of its bioavailable fraction in natural peat. Our investigation aims to: a) estimate the quantity of bioavailable Cs-137 and Pu present in peat, b) verify the similarity of Cs-137 and K-40 behaviours, and c) perform a quantification of Cs-137 and Pu transfer from peat to plants. We analysed the vertical distribution of Cs-137 and Pu isotopes in the peat and their concentrations in plants growing on these places. Bioavailability of radionuclides was investigated by sequential extraction. Sequential analyses revealed that it was the upper layer which contained the majority of Cs-137 in an available form while deeper layers retained Cs-137 in immobile fractions. We can conclude that 18% of all Cs-137 in the peat is still bioavailable. Despite of the low quantity of bioavailable fraction of Cs-137 its transfer factor reached extremely high values. In the case of Pu, 64% of its total amount was associated with fulvic/humic acids which resulted in the high transfer factor from peat to plants. 27 years after the Chernobyl nuclear accident, the significant part of radionuclides deposited in peatland is still bioavailable.

  16. PU Vulpeculae - The outburst of a symbiotic nova

    NASA Astrophysics Data System (ADS)

    Vogel, M.; Nussbaumer, H.

    1992-06-01

    We report the full history of PU Vulpeculae from outburst to 1991 as seen in its ultraviolet emission. We show that PU Vul is a symbiotic nova, which went into outburst in 1977 after a nova-like thermonuclear event. The outbursting object went first into an F supergiant phase. The spectrum evolved between 1979 and 1989 from F-type into that of Ao. In 1990 PU Vul entered the nebular phase, showing a rich emission line spectrum in the UV and in the optical. Between 1979 and 1983-1985 the luminosity of the outbursting object increased by approximately a factor of 2 against 2600 solar luminosities in 1979. It subsequently decreased to reach in 1989 approximately the same value as in 1979. During 1980 the lightcurve went through a minimum and the spectral appearance changed. We interpret this as an eclipse of the outbursting star by the M giant companion. Based on IUE observations we discuss the early nebular phase of PU Vul, and we show that the UV is still dominated by the outbursting component, which in 1991 has reached a temperature of 40,000 K.

  17. Atomic Structure and Phase Transformations in Pu Alloys

    SciTech Connect

    Schwartz, A J; Cynn, H; Blobaum, K M; Wall, M A; Moore, K T; Evans, W J; Farber, D L; Jeffries, J R; Massalski, T B

    2008-04-28

    Plutonium and plutonium-based alloys containing Al or Ga exhibit numerous phases with crystal structures ranging from simple monoclinic to face-centered cubic. Only recently, however, has there been increased convergence in the actinides community on the details of the equilibrium form of the phase diagrams. Practically speaking, while the phase diagrams that represent the stability of the fcc {delta}-phase field at room temperature are generally applicable, it is also recognized that Pu and its alloys are never truly in thermodynamic equilibrium because of self-irradiation effects, primarily from the alpha decay of Pu isotopes. This article covers past and current research on several properties of Pu and Pu-(Al or Ga) alloys and their connections to the crystal structure and the microstructure. We review the consequences of radioactive decay, the recent advances in understanding the electronic structure, the current research on phase transformations and their relations to phase diagrams and phase stability, the nature of the isothermal martensitic {delta} {yields} {alpha}{prime} transformation, and the pressure-induced transformations in the {delta}-phase alloys. New data are also presented on the structures and phase transformations observed in these materials following the application of pressure, including the formation of transition phases.

  18. Polymerization of Pu(IV) in aqueous nitric acid solutions

    SciTech Connect

    Toth, L.M.; Friedman, H.A.; Osborne, M.M.

    1980-10-01

    The polymerization of Pu(IV) in aqueous nitric acid solutions has been studied spectrophotometrically both to establish the influence of large UO{sub 2}(NO{sub 3}){sub 2} concentrations on the polymerization rates and, more generally, to review the influence of the major parameters on the polymer reaction. Typically, experiments have been performed at 50{sup 0}C and with 0.05 M Pu in nitric acid solutions that vary in acidity from 0.07 to 0.4 M. An induction period usually precedes the polymer growth stage during which time nucleation of primary hydrolysis products occurs. Uranyl nitrate retards the polymerization reaction by approximately 35% in spite of the counteracting influence of the nitrate ions associated with this solute. The rate of polymer formation, expressed as d(percent polymer)/dt, has been shown to depend on the total plutonium concentration in reactions where the Pu(IV) concentration remained constant; and it is therefore suggested that the polymer reaction rate is not first order with respect to the concentration of plutonium as was previously thought. It has been shown further that accurate acid determinations on stock reagents are essential in order to obtain reliable polymerization experiments. Satisfactory procedures for these analyses did not exist, so appropriate modifications to the iodate precipitation methods were developed. The most ideal plutonium reagent material has been shown to be crystalline Pu(IV) nitrate because it can be added directly to acid solutions without the occurrence of unintentional hydrolysis reactions.

  19. Evaluation of the neutron cross sections for Pu-240

    SciTech Connect

    Weston, L.W.; Arthur, E.D.

    1987-04-01

    The present evaluation is proposed to supersede the ENDF/B-V, Revision 2 file for /sup 240/Pu. In this work, resonance parameters, cross sections, energy distributions, and angular distributions have been modified. These changes are outlined in detail and appropriate references included. 37 refs., 21 figs., 2 tabs.

  20. Enhancing VVER Annular Proliferation Resistance Fuel with Minor Actinides

    SciTech Connect

    G. S. Chang

    2007-06-01

    Key aspects of the Global Nuclear Energy Partnership (GNEP) are to significantly advance the science and technology of nuclear energy systems and the Advanced Fuel Cycle (AFC) program. The merits of nuclear energy are the high-density energy, and low environmental impacts i.e. almost zero greenhouse gas emission. Planned efforts involve near-term and intermediate-term improvements in fuel utilization and recycling in current LWR as well as the longer-term development of new nuclear energy systems that offer much improved fuel utilization and proliferation resistance, along with continued advances in operational safety. The challenges are solving the energy needs of the world, protection against nuclear proliferation, the problem of nuclear waste, and the global environmental problem. To reduce the spent fuel for storage and enhance the proliferation resistance for the intermediate-term, there are two major approaches (a) increase the discharged spent fuel burnup in the advanced LWR (Gen-III Plus), which not only can reduce the spent fuel for storage, but also increase the 238Pu and 240Pu isotopes ratio to enhance the proliferation resistance, (b) use of transuranic nuclides (237Np and 241Am) in the high burnup fuel, which can drastically increase the proliferation resistance isotope 238Pu /Pu ratio. For future advanced nuclear systems, the minor actinides are viewed more as a resource to be recycled, or transmuted to less hazardous and possibly more useful forms, rather than simply as a waste stream to be disposed of in expensive repository facilities. In this paper, a typical pressurized water reactor (PWR) VVER-1000 annular fuel unit lattice cell model with UO2 fuel pins will be used to investigate the effectiveness of minor actinide reduction approach (MARA) for enhancing proliferation resistance and improving the fuel cycle performance. We concluded that the concept of MARA, involves the use of transuranic nuclides (237Np and/or 241Am), can not only drastically

  1. Development program to recycle and purify plutonium-238 oxide fuel from scrap

    NASA Astrophysics Data System (ADS)

    Schulte, Louis D.; Silver, Gary L.; Avens, Larry R.; Jarvinen, Gordon D.; Espinoza, Jacob; Foltyn, Elizabeth M.; Rinehart, Gary H.

    1997-01-01

    Nuclear Materials Technology (NMT) Division of Los Alamos National Laboratory (LANL) has initiated a development program to recover & purify plutonium-238 oxide from impure sources. A glove box line has been designed and a process flowsheet developed to perform this task on a large scale. Our initial effort has focused on purification of 238PuO2 fuel that fails to meet General Purpose Heat Source (GPHS) specifications because of impurities. The most notable non-actinide impurity was silicon, but aluminum, chromium, iron and nickel were also near or in excess of limits specified by GPHS fuel powder specifications. 234U was by far the largest actinide impurity observed in the feed material because it is the daughter product of 238Pu by alpha decay. An aqueous method based on nitric acid was selected for purification of the 238PuO2 fuel. All aqueous processing used high purity reagents, and was performed in PTFE apparatus to minimize introduction of new contaminants. Impure 238PuO2 was finely milled, then dissolved in refluxing HNO3/HF and the solution filtered. The dissolved 238Pu was adjusted to the trivalent state by an excess of reducing reagents to compensate for radiolytic effects, precipitated as plutonium(III) oxalate, and recovered by filtration. The plutonium(III) oxalate was subsequently calcined to convert the plutonium to the oxide. Decontamination factors for silicon, phosphorus and uranium were excellent. Decontamination factors for aluminum, chromium, iron and nickel were very good. The purity of the 238PuO2 recovered from this operation was significantly better than specifications. Efforts continue to develop the capability for efficient, safe, cost-effective, and environmentally acceptable methods to recover and purify 238PuO2 fuel in a glove box environment. Plutonium-238 materials targeted for recovery includes impure oxide and scrap items that are lean in 238Pu values.

  2. Lead Slowing-Down Spectrometry Time Spectral Analysis for Spent Fuel Assay: FY11 Status Report

    SciTech Connect

    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 pure

  3. Modelling the thermal conductivity of (UxTh1-x)O2 and (UxPu1-x)O2

    DOE PAGES

    Cooper, M. W. D.; Middleburgh, S. C.; Grimes, R. W.

    2015-07-15

    The degradation of thermal conductivity due to the non-uniform cation lattice of (UxTh1-x)O2 and (UxPu1-x)O2 solid solutions has been investigated by molecular dynamics, using the non-equilibrium method, from 300 to 2000 K. Degradation of thermal conductivity is predicted in (UxTh1-x)O2 and (UxPu1-x)O2 as compositions deviate from the pure end members: UO2, PuO2 and ThO2. The reduction in thermal conductivity is most apparent at low temperatures where phonon-defect scattering dominates over phonon-phonon interactions. The effect is greater for (UxTh1-x)O2 than UxPu1-x)O2 due to the greater mismatch in cation size. Parameters for an analytical expressions have been developed that describe the predictedmore » thermal conductivities over the full temperature and compositional ranges. Finally, these expressions may be used in higher level fuel performance codes.« less

  4. Determination of plutonium in spent nuclear fuel using high resolution X-ray

    DOE PAGES

    McIntosh, Kathryn G.; Reilly, Sean D.; Havrilla, George J.

    2015-05-30

    Characterization of Pu is an essential aspect of safeguards operations at nuclear fuel reprocessing facilities. A novel analysis technique called hiRX (high resolution X-ray) has been developed for the direct measurement of Pu in spent nuclear fuel dissolver solutions. hiRX is based on monochromatic wavelength dispersive X-ray fluorescence (MWDXRF), which provides enhanced sensitivity and specificity compared with conventional XRF techniques. A breadboard setup of the hiRX instrument was calibrated using spiked surrogate spent fuel (SSF) standards prepared as dried residues. Samples of actual spent fuel were utilized to evaluate the performance of the hiRX. The direct detection of just 39more » ng of Pu is demonstrated. Initial quantitative results, with error of 4–27% and precision of 2% relative standard deviation (RSD), were obtained for spent fuel samples. The limit of detection for Pu (100 s) within an excitation spot of 200 μm diameter was 375 pg. This study demonstrates the potential for the hiRX technique to be utilized for the rapid, accurate, and precise determination of Pu. Moreover, the results highlight the analytical capability of hiRX for other applications requiring sensitive and selective nondestructive analyses.« less

  5. Determination of plutonium in spent nuclear fuel using high resolution X-ray

    SciTech Connect

    McIntosh, Kathryn G.; Reilly, Sean D.; Havrilla, George J.

    2015-05-30

    Characterization of Pu is an essential aspect of safeguards operations at nuclear fuel reprocessing facilities. A novel analysis technique called hiRX (high resolution X-ray) has been developed for the direct measurement of Pu in spent nuclear fuel dissolver solutions. hiRX is based on monochromatic wavelength dispersive X-ray fluorescence (MWDXRF), which provides enhanced sensitivity and specificity compared with conventional XRF techniques. A breadboard setup of the hiRX instrument was calibrated using spiked surrogate spent fuel (SSF) standards prepared as dried residues. Samples of actual spent fuel were utilized to evaluate the performance of the hiRX. The direct detection of just 39 ng of Pu is demonstrated. Initial quantitative results, with error of 4–27% and precision of 2% relative standard deviation (RSD), were obtained for spent fuel samples. The limit of detection for Pu (100 s) within an excitation spot of 200 μm diameter was 375 pg. This study demonstrates the potential for the hiRX technique to be utilized for the rapid, accurate, and precise determination of Pu. Moreover, the results highlight the analytical capability of hiRX for other applications requiring sensitive and selective nondestructive analyses.

  6. Fossil fuels -- future fuels

    SciTech Connect

    1998-03-01

    Fossil fuels -- coal, oil, and natural gas -- built America`s historic economic strength. Today, coal supplies more than 55% of the electricity, oil more than 97% of the transportation needs, and natural gas 24% of the primary energy used in the US. Even taking into account increased use of renewable fuels and vastly improved powerplant efficiencies, 90% of national energy needs will still be met by fossil fuels in 2020. If advanced technologies that boost efficiency and environmental performance can be successfully developed and deployed, the US can continue to depend upon its rich resources of fossil fuels.

  7. Post irradiation examination of thermal reactor fuels

    NASA Astrophysics Data System (ADS)

    Sah, D. N.; Viswanathan, U. K.; Ramadasan, E.; Unnikrishnan, K.; Anantharaman, S.

    2008-12-01

    The post irradiation examination (PIE) facility at the Bhabha Atomic Research Centre (BARC) has been in operation for more than three decades. Over these years this facility has been utilized for examination of experimental fuel pins and fuels from commercial power reactors operating in India. In a program to assess the performance of (U,Pu)O 2 MOX fuel prior to its introduction in commercial reactors, three experimental MOX fuel clusters irradiated in the pressurized water loop (PWL) of CIRUS up to burnup of 16 000 MWd/tU were examined. Fission gas release from these pins was measured by puncture test. Some of these fuel pins in the cluster contained controlled porosity pellets, low temperature sintered (LTS) pellets, large grain size pellets and annular pellets. PIE has also been carried out on natural UO 2 fuel bundles from Indian PHWRs, which included two high burnup (˜15 000 MWd/tU) bundles. Salient investigations carried out consisted of visual examination, leak testing, axial gamma scanning, fission gas analysis, microstructural examination of fuel and cladding, β, γ autoradiography of the fuel cross-section and fuel central temperature estimation from restructuring. A ThO 2 fuel bundle irradiated in Kakrapar Atomic Power Station (KAPS) up to a nominal fuel burnup of ˜11 000 MWd/tTh was also examined to evaluate its in-pile performance. The performance of the BWR fuel pins of Tarapur Atomic Power Stations (TAPS) was earlier assessed by carrying out PIE on 18 fuel elements selected from eight fuel assemblies irradiated in the two reactors. The burnup of these fuel elements varied from 5000 to 29 000 MWd/tU. This paper provides a brief review of some of the fuels examined and the results obtained on the performance of natural UO 2, enriched UO 2, MOX, and ThO 2 fuels.

  8. A theoretical study of the ground state and lowest excited states of PuO0/+/+2 and PuO20/+/+2

    SciTech Connect

    Gibson, John K.; La Macchia, Giovanni; Infante, Ivan; Gagliardi, Laura; Raab, Juraj

    2008-12-08

    The ground and excited states of neutral and cationic PuO and PuO2 have been studied with multiconfigurational quantum chemical methods followed by second order perturbation theory, the CASSCF/CASPT2 method. Scalar relativistic effects and spin-orbit coupling have been included in the treatment. As literature values for the ionization energy of PuO2 are in the wide range of ~;;6.6 eV to ~;;10.1 eV, a central goal of the computations was to resolve these discrepancies; the theoretical results indicate that the ionization energy is near the lower end of this range. The calculated ionization energies for PuO, PuO+ and PuO2+ are in good agreement with the experimental values.

  9. Determination of (235)U, (239)Pu, (240)Pu, and (241)Am in a nuclear bomb particle using a position-sensitive α-γ coincidence technique.

    PubMed

    Peräjärvi, Kari A; Ihantola, Sakari; Pöllänen, Roy C; Toivonen, Harri I; Turunen, Jani A

    2011-02-15

    A nuclear bomb particle containing 1.6 ng of Pu was investigated nondestructively with a position-sensitive α detector and a broad-energy HPGe γ-ray detector. An event-mode data acquisition system was used to record the data. α-γ coincidence counting was shown to be well suited to nondestructive isotope ratio determination. Because of the very small background, the 51.6 keV γ rays of (239)Pu and the 45.2 keV γ rays of (240)Pu were identified, which enabled isotopic ratio calculations. In the present work, the (239)Pu/((239)Pu+(240)Pu) atom ratio was determined to be 0.950 ± 0.010. The uncertainties were much smaller than in the previous more conventional nondestructive studies on this particle. Obtained results are also in good agreement with the data from the destructive mass spectrometric studies obtained previously by other investigators.

  10. Effects of Aging on PuO2∙xH2O Particle Size in Alkaline Solution

    SciTech Connect

    Delegard, Calvin H.

    2013-05-01

    Between 1944 and 1989, 54.5 metric tons of the United States’ weapons-grade plutonium and an additional 12.9 metric tons of fuel-grade plutonium were produced and separated from irradiated fuel at the Hanford Site. Acidic high-activity wastes containing around 600 kg of plutonium were made alkaline and discharged to underground storage tanks from separations, isolation, and recycle processes to yield average plutonium concentration of about 0.003 grams per liter (or ~0.0002 wt%) in the ~200 million liter tank waste volume. The plutonium is largely associated with low-solubility metal hydroxide/oxide sludges where its low concentration and intimate mixture with neutron-absorbing elements (e.g., iron) are credited in nuclear criticality safety. However, concerns have been expressed that plutonium, in the form of plutonium hydrous oxide, PuO2∙xH2O, could undergo sufficient crystal growth through dissolution and reprecipitation in the alkaline tank waste to potentially become separable from neutron absorbing constituents by settling or sedimentation. Thermodynamic considerations and laboratory studies of systems chemically analogous to tank waste show that the plutonium formed in the alkaline tank waste by precipitation through neutralization from acid solution probably entered as 2–4-nm PuO2∙xH2O crystallite particles that, because of their low solubility and opposition from radiolytic processes, grow from that point at exceedingly slow rates, thus posing no risk of physical segregation.

  11. Simulation of radiation driven fission gas diffusion in UO2, ThO2 and PuO2

    DOE PAGES

    Cooper, Michael William D.; Stanek, Christopher Richard; Turnbull, James Anthony; ...

    2016-12-01

    Below 1000 K it is thought that fission gas diffusion in nuclear fuel during irradiation occurs through atomic mixing due to radiation damage. Here we present a molecular dynamics (MD) study of Xe, Kr, Th, U, Pu and O diffusion due to irradiation. It is concluded that the ballistic phase does not sufficiently account for the experimentally observed diffusion. Thermal spike simulations are used to confirm that electronic stopping remedies the discrepancy with experiment and the predicted diffusivities lie within the scatter of the experimental data. Here, our results predict that the diffusion coefficients are ordered such that D*0 >more » D*Kr > D*Xe > D*U. For all species >98.5% of diffusivity is accounted for by electronic stopping. Fission gas diffusivity was not predicted to vary significantly between ThO2, UO2 and PuO2, indicating that this process would not change greatly for mixed oxide fuels.« less

  12. Irradiated Nuclear Fuel Management: Resource Versus Waste

    SciTech Connect

    Nash, Kenneth L.; Lumetta, Gregg J.; Vienna, John D.

    2013-01-01

    Management of irradiated fuel is an important component of commercial nuclear power production. Although it is broadly agreed that the disposition of some fraction of the fuel in geological repositories will be necessary, there is a range of options that can be considered that affect exactly what fraction of material will be disposed in that manner. Furthermore, until geological repositories are available to accept commercial irradiated fuel, these materials must be safely stored. Temporary storage of irradiated fuel has traditionally been conducted in storage pools, and this is still true for freshly discharged fuel. Criticality control technologies have led to greater efficiencies in packing of irradiated fuel into storage pools. With continued delays in establishing permanent repositories, utilities have begun to move some of the irradiated fuel inventory into dry storage. Fuel cycle options being considered worldwide include the once-through fuel cycle, limited recycle in which U and Pu are recycled back to power reactors as mixed oxide fuel, and advance partitioning and transmutation schemes designed to reduce the long term hazards associated with geological disposal from millions of years to a few hundred years. Each of these options introduces specific challenges in terms of the waste forms required to safely immobilize the hazardous components of irradiated fuel.

  13. FUEL ELEMENTS FOR THERMAL-FISSION NUCLEAR REACTORS

    DOEpatents

    Flint, O.

    1961-01-10

    Fuel elements for thermal-fission nuclear reactors are described. The fuel element is comprised of a core of alumina, a film of a metal of the class consisting of copper, silver, and nickel on the outer face of the core, and a coating of an oxide of a metal isotope of the class consisting of Un/sup 235/, U/ sup 233/, and Pu/sup 239/ on the metal f ilm.

  14. ENHANCING ADVANCED CANDU PROLIFERATION RESISTANCE FUEL WITH MINOR ACTINIDES

    SciTech Connect

    Gray S. Chang

    2010-05-01

    The advanced nuclear system will significantly advance the science and technology of nuclear energy systems and to enhance the spent fuel proliferation resistance. Minor actinides (MA) are viewed more as a resource to be recycled, and transmuted to less hazardous and possibly more useful forms, rather than simply disposed of as a waste stream in an expensive repository facility. MAs can play a much larger part in the design of advanced systems and fuel cycles, not only as additional sources of useful energy, but also as direct contributors to the reactivity control of the systems into which they are incorporated. In this work, an Advanced CANDU Reactor (ACR) fuel unit lattice cell model with 43 UO2 fuel rods will be used to investigate the effectiveness of a Minor Actinide Reduction Approach (MARA) for enhancing proliferation resistance and improving the fuel cycle performance. The main MARA objective is to increase the 238Pu / Pu isotope ratio by using the transuranic nuclides (237Np and 241Am) in the high burnup fuel and thereby increase the proliferation resistance even for a very low fuel burnup. As a result, MARA is a very effective approach to enhance the proliferation resistance for the on power refueling ACR system nuclear fuel. The MA transmutation characteristics at different MA loadings were compared and their impact on neutronics criticality assessed. The concept of MARA, significantly increases the 238Pu/Pu ratio for proliferation resistance, as well as serves as a burnable absorber to hold-down the initial excess reactivity. It is believed that MARA can play an important role in atoms for peace and the intermediate term of nuclear energy reconnaissance.

  15. Fuel Cycle System Analysis Handbook

    SciTech Connect

    Steven J. Piet; Brent W. Dixon; Dirk Gombert; Edward A. Hoffman; Gretchen E. Matthern; Kent A. Williams

    2009-06-01

    This Handbook aims to improve understanding and communication regarding nuclear fuel cycle options. It is intended to assist DOE, Campaign Managers, and other presenters prepare presentations and reports. When looking for information, check here. The Handbook generally includes few details of how calculations were performed, which can be found by consulting references provided to the reader. The Handbook emphasizes results in the form of graphics and diagrams, with only enough text to explain the graphic, to ensure that the messages associated with the graphic is clear, and to explain key assumptions and methods that cause the graphed results. Some of the material is new and is not found in previous reports, for example: (1) Section 3 has system-level mass flow diagrams for 0-tier (once-through), 1-tier (UOX to CR=0.50 fast reactor), and 2-tier (UOX to MOX-Pu to CR=0.50 fast reactor) scenarios - at both static and dynamic equilibrium. (2) To help inform fast reactor transuranic (TRU) conversion ratio and uranium supply behavior, section 5 provides the sustainable fast reactor growth rate as a function of TRU conversion ratio. (3) To help clarify the difference in recycling Pu, NpPu, NpPuAm, and all-TRU, section 5 provides mass fraction, gamma, and neutron emission for those four cases for MOX, heterogeneous LWR IMF (assemblies mixing IMF and UOX pins), and a CR=0.50 fast reactor. There are data for the first 10 LWR recycle passes and equilibrium. (4) Section 6 provides information on the cycle length, planned and unplanned outages, and TRU enrichment as a function of fast reactor TRU conversion ratio, as well as the dilution of TRU feedstock by uranium in making fast reactor fuel. (The recovered uranium is considered to be more pure than recovered TRU.) The latter parameter impacts the required TRU impurity limits specified by the Fuels Campaign. (5) Section 7 provides flows for an 800-tonne UOX separation plant. (6) To complement 'tornado' economic uncertainty

  16. Spent nuclear fuel recycling with plasma reduction and etching

    DOEpatents

    Kim, Yong Ho

    2012-06-05

    A method of extracting uranium from spent nuclear fuel (SNF) particles is disclosed. Spent nuclear fuel (SNF) (containing oxides of uranium, oxides of fission products (FP) and oxides of transuranic (TRU) elements (including plutonium)) are subjected to a hydrogen plasma and a fluorine plasma. The hydrogen plasma reduces the uranium and plutonium oxides from their oxide state. The fluorine plasma etches the SNF metals to form UF6 and PuF4. During subjection of the SNF particles to the fluorine plasma, the temperature is maintained in the range of 1200-2000 deg K to: a) allow any PuF6 (gas) that is formed to decompose back to PuF4 (solid), and b) to maintain stability of the UF6. Uranium (in the form of gaseous UF6) is easily extracted and separated from the plutonium (in the form of solid PuF4). The use of plasmas instead of high temperature reactors or flames mitigates the high temperature corrosive atmosphere and the production of PuF6 (as a final product). Use of plasmas provide faster reaction rates, greater control over the individual electron and ion temperatures, and allow the use of CF4 or NF3 as the fluorine sources instead of F2 or HF.

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

    PubMed

    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.

  18. Synthesis, structural and thermal studies of Pu(VO3)4: A new vanadate in PuO2-V2O5 system

    NASA Astrophysics Data System (ADS)

    Dahale, N. D.; Achary, S. N.; Sali, S. K.; Keskar, Meera; Phatak, R.; Kannan, S.

    2012-08-01

    A new phase Pu(VO3)4 in PuO2-V2O5 system was prepared by heating an appropriate amount of pre-dried PuO2 and V2O5 at 640 °C. The structural and thermal properties of Pu(VO3)4 were investigated by powder X-ray diffraction and thermogravimetry (TG). Structural analyses revealed that Pu(VO3)4 crystallizes in tetragonal (space group: I41/a) lattice with unit cell parameters, a = 8.4528(2) Å and c = 28.6644(9) Å and is isostructural to metavanadates of thorium and neptunium. Structure shows crystallographically two distinct vanadium atoms V(1) and V(2), one plutonium atom (Pu1) and seven oxygen atoms in the unit cell of Pu(VO3)4. Vanadium atoms form VO4 tetrahedra while plutonium forms PuO8 polyhedra with oxygen atoms. The VO4 units are linked together by sharing apex oxygen atoms and form infinite spiral chains of (VO3)n. Along c-axis, the plutonium atoms are sandwiched between the two layers of (VO3)n chains. TG of Pu(VO3)4 showed thermal stability of the compound up to 700 °C.

  19. Structural, magnetic, electronic and optical properties of PuC and PuC0.75: A hybrid density functional study

    NASA Astrophysics Data System (ADS)

    Yang, Rong; Tang, Bin; Gao, Tao; Ao, BingYun

    2016-05-01

    We perform first principles calculations to investigate the structural, magnetic, electronic and optical properties of PuC and PuC0.75. Furthermore, we examine the influence of carbon non-stoichiometry on plutonium monocarbide. For the treatment of strongly correlated electrons, the hybrid density functionals like PBE0, Fock-0.25 are used and we compare the results with the generalized gradient approximation (GGA), local density approximation (LDA), LDA + U and experimental ones. The optimized lattice constant a0 = 4.961 Å for PuC in the Fock-0.25 scheme is the most close to the experimental data. The ground states of PuC and PuC0.75 are found to be anti-ferromagnetic. Our results indicate that additional removal of a C atom make lattice contract and new DOS peak appear in the near-Fermi region. We also compute and compare the optical properties of PuC and PuC0.75. The difference in optical properties between PuC and PuC0.75 should also be the influence of carbon vacancies.

  20. Accelerator Mass Spectrometric (AMS) Measurements of Plutonium Activity Concentrations and 240Pu/239Pu Atom Ratios In Soil Extracts Supplied by the Carlsbad Environmental Monitoring & Research Center

    SciTech Connect

    Hamilton, T F; Brown, T A; Marchetti, A A; Martinelli, R E; Kehl, S R

    2005-02-28

    Plutonium-239 ({sup 239}Pu) and plutonium-239+240 ({sup 239+240}Pu) activities concentrations and {sup 240}Pu/{sup 239}Pu atom ratios are reported for a series of chemically purified soil extracts received from the Carlsbad Environmental Monitoring & Research Center (CEMRC) in New Mexico. Samples were analyzed without further purification at the Lawrence Livermore National Laboratory (LLNL) using accelerator mass spectrometry (AMS). This report also includes a brief description of the AMS system and internal laboratory procedures used to ensure the quality and reliability of the measurement data.

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

    NASA Astrophysics Data System (ADS)

    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.

  2. AFS-2 FLOWSHEET MODIFICATIONS TO ADDRESS THE INGROWTH OF PU(VI) DURING METAL DISSOLUTION

    SciTech Connect

    Crapse, K.; Rudisill, T.; O'Rourke, P.; Kyser, E.

    2014-07-02

    In support of the Alternate Feed Stock Two (AFS-2) PuO{sub 2} production campaign, Savannah River National Laboratory (SRNL) conducted a series of experiments concluding that dissolving Pu metal at 95°C using a 6–10 M HNO{sub 3} solution containing 0.05–0.2 M KF and 0–2 g/L B could reduce the oxidation of Pu(IV) to Pu(VI) as compared to dissolving Pu metal under the same conditions but at or near the boiling temperature. This flowsheet was demonstrated by conducting Pu metal dissolutions at 95°C to ensure that PuO{sub 2} solids were not formed during the dissolution. These dissolution parameters can be used for dissolving both Aqueous Polishing (AP) and MOX Process (MP) specification materials. Preceding the studies reported herein, two batches of Pu metal were dissolved in the H-Canyon 6.1D dissolver to prepare feed solution for the AFS-2 PuO{sub 2} production campaign. While in storage, UV-visible spectra obtained from an at-line spectrophotometer indicated the presence of Pu(VI). Analysis of the solutions also showed the presence of Fe, Ni, and Cr. Oxidation of Pu(IV) produced during metal dissolution to Pu(VI) is a concern for anion exchange purification. Anion exchange requires Pu in the +4 oxidation state for formation of the anionic plutonium(IV) hexanitrato complex which absorbs onto the resin. The presence of Pu(VI) in the anion feed solution would require a valence adjustment step to prevent losses. In addition, the presence of Cr(VI) would result in absorption of chromate ion onto the resin and could limit the purification of Pu from Cr which may challenge the purity specification of the final PuO{sub 2} product. Initial experiments were performed to quantify the rate of oxidation of Pu(IV) to Pu(VI) (presumed to be facilitated by Cr(VI)) as functions of the HNO{sub 3} concentration and temperature in simulated dissolution solutions containing Cr, Fe, and Ni. In these simulated Pu dissolutions studies, lowering the temperature from near boiling

  3. Vertical distribution of (241)Pu in the southern Baltic Sea sediments.

    PubMed

    Strumińska-Parulska, Dagmara I

    2014-12-15

    The vertical distribution of plutonium (241)Pu in marine sediments can assist in determining the deposition history and sedimentation process of analyzed regions. In addition, (241)Pu/(239+240)Pu activity ratio could be used as a sensitive fingerprint for radioactive source identification. The present preliminary studies on vertical distribution of (241)Pu in sediments from four regions of the southern Baltic Sea are presented. The distribution of (241)Pu was not uniform and depended on sediment geomorphology and depth as well as location. The highest concentrations of plutonium were found in the surface layers of all analyzed sediments and originated from the Chernobyl accident.

  4. Anaerobic Biotransformation and Mobility of Pu and of Pu-EDTA

    SciTech Connect

    Xun, Luying

    2009-11-20

    The enhanced mobility of radionuclides by co-disposed chelating agent, ethylenediaminetetraacetate (EDTA), is likely to occur only under anaerobic conditions. Our extensive effort to enrich and isolate anaerobic EDTA-degrading bacteria has failed. Others has tried and also failed. To explain the lack of anaerobic biodegradation of EDTA, we proposed that EDTA has to be transported into the cells for metabolism. A failure of uptake may contribute to the lack of EDTA degradation under anaerobic conditions. We demonstrated that an aerobic EDTA-degrading bacterium strain BNC1 uses an ABC-type transporter system to uptake EDTA. The system has a periplasmic binding protein that bind EDTA and then interacts with membrane proteins to transport EDTA into the cell at the expense of ATP. The bind protein EppA binds only free EDTA with a Kd of 25 nM. The low Kd value indicates high affinity. However, the Kd value of Ni-EDTA is 2.4 x 10^(-10) nM, indicating much stronger stability. Since Ni and other trace metals are essential for anaerobic respiration, we conclude that the added EDTA sequestrates all trace metals and making anaerobic respiration impossible. Thus, the data explain the lack of anaerobic enrichment cultures for EDTA degradation. Although we did not obtain an EDTA degrading culture under anaerobic conditions, our finding may promote the use of certain metals that forms more stable metal-EDTA complexes than Pu(III)-EDTA to prevent the enhanced mobility. Further, our data explain why EDTA is the most dominant organic pollutant in surface waters, due to the lack of degradation of certain metal-EDTA complexes.

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

    DTIC Science & Technology

    2009-07-01

    uranium to make mixed-oxide ( MOX ) fuel, in which the 239Pu largely substitutes for 235U. Two French reprocessing plants at La Hague can each...Managing the Nuclear Fuel Cycle Congressional Research Service 17 plant.54 About 200 metric tons of MOX fuel is used annually, about 2% of new nuclear...fuel,55 equivalent to about 2,000 metric tons of mined uranium.56 However, the benefits of reprocessing spent fuel to make MOX fuel for today’s

  6. Production of {sup 238}PuO{sub 2} heat sources for the Cassini mission

    SciTech Connect

    George, T.G.; Foltyn, E.M.

    1998-01-01

    NASA{close_quote}s Cassini mission to Saturn, scheduled to launch in October, 1997, is perhaps the most ambitious interplanetary explorer ever constructed. Electric power for the spacecraft{close_quote}s science instruments and on-board computers will be provided by three radioisotope thermoelectric generators (RTGs) powered by 216 {sup 238}PuO{sub 2}-fueled General-Purpose Heat Source (GPHS) capsules. In addition, critical equipment and instruments on the spacecraft and Huygens probe will be warmed by 128 Light-Weight Radioisotope Heater Units (LWRHUs). Fabrication and assembly of the GPHS capsules and LWRHU heat sources was performed at Los Alamos National Laboratory (LANL) between January 1994 and September 1996. During this production campaign, LANL pressed and sintered 315 GPHS fuel pellets and 181 LWRHU pellets. By October 1996, NMT-9 had delivered a total of 235 GPHS capsules to EG&G Mound Applied Technologies (EG&G MAT) in Miamisburg, Ohio. EG&G MAT conditioned the capsules for use, loaded the capsules into the Cassini RTGs, tested the RTGs, and coordinated transportation to Kennedy Space Center (KSC). LANL also fabricated and assembled a total of 180 LWRHUs. The LWRHUs required for the Cassini spacecraft were shipped to KSC in mid-1997. {copyright} {ital 1998 American Institute of Physics.}

  7. Surface-mediated formation of Pu(IV) nanoparticles at the muscovite-electrolyte interface.

    PubMed

    Schmidt, Moritz; Lee, Sang Soo; Wilson, Richard E; Knope, Karah E; Bellucci, Francesco; Eng, Peter J; Stubbs, Joanne E; Soderholm, L; Fenter, P

    2013-12-17

    The formation of Pu(IV)-oxo-nanoparticles from Pu(III) solutions by a surface-enhanced redox/polymerization reaction at the muscovite (001) basal plane is reported, with a continuous increase in plutonium coverage observed in situ over several hours. The sorbed Pu extends >70 Å from the surface with a maximum concentration at 10.5 Å and a total coverage of >9 Pu atoms per unit cell area of muscovite (0.77 μg Pu/cm(2)) (determined independently by in situ resonant anomalous X-ray reflectivity and by ex-situ alpha-spectrometry). The presence of discrete nanoparticles is confirmed by high resolution atomic force microscopy. We propose that the formation of these Pu(IV) nanoparticles from an otherwise stable Pu(III) solution can be explained by the combination of a highly concentrated interfacial Pu-ion species, the Pu(III)-Pu(IV) redox equilibrium, and the strong proclivity of tetravalent Pu to hydrolyze and form polymeric species. These results are the first direct observation of such behavior of plutonium on a naturally occurring mineral, providing insights into understanding the environmental transport of plutonium and other contaminants capable of similar redox/polymerization reactions.

  8. PU.1 is a potent tumor suppressor in classical Hodgkin lymphoma cells.

    PubMed

    Yuki, Hiromichi; Ueno, Shikiko; Tatetsu, Hiro; Niiro, Hiroaki; Iino, Tadafumi; Endo, Shinya; Kawano, Yawara; Komohara, Yoshihiro; Takeya, Motohiro; Hata, Hiroyuki; Okada, Seiji; Watanabe, Toshiki; Akashi, Koichi; Mitsuya, Hiroaki; Okuno, Yutaka

    2013-02-07

    PU.1 has previously been shown to be down-regulated in classical Hodgkin lymphoma (cHL) cells via promoter methylation. We performed bisulfite sequencing and proved that the promoter region and the -17 kb upstream regulatory element of the PU.1 gene were highly methylated. To evaluate whether down-regulation of PU.1 is essential for the growth of cHL cells, we conditionally expressed PU.1 in 2 cHL cell lines, L428 and KM-H2. Overexpression of PU.1 induced complete growth arrest and apoptosis in both cell lines. Furthermore, in a Hodgkin lymphoma tumor xenograft model using L428 and KM-H2 cell lines, overexpression of PU.1 led to tumor regression or stable disease. Lentiviral transduction of PU.1 into primary cHL cells also induced apoptosis. DNA microarray analysis revealed that among genes related to cell cycle and apoptosis, p21 (CDKN1A) was highly up-regulated in L428 cells after PU.1 induction. Stable knockdown of p21 rescued PU.1-induced growth arrest in L428 cells, suggesting that the growth arrest and apoptosis observed are at least partially dependent on p21 up-regulation. These data strongly suggest that PU.1 is a potent tumor suppressor in cHL and that induction of PU.1 with demethylation agents and/or histone deacetylase inhibitors is worth exploring as a possible therapeutic option for patients with cHL.

  9. PLANTS AS BIO-MONITORS FOR 137CS, 238PU, 239, 240PU AND 40K AT THE SAVANNAH RIVER SITE

    SciTech Connect

    Caldwell, E.; Duff, M.; Ferguson, C.

    2010-12-16

    The nuclear fuel cycle generates a considerable amount of radioactive waste, which often includes nuclear fission products, such as strontium-90 ({sup 90}Sr) and cesium-137 ({sup 137}Cs), and actinides such as uranium (U) and plutonium (Pu). When released into the environment, large quantities of these radionuclides can present considerable problems to man and biota due to their radioactive nature and, in some cases as with the actinides, their chemical toxicity. Radionuclides are expected to decay at a known rate. Yet, research has shown the rate of elimination from an ecosystem to differ from the decay rate due to physical, chemical and biological processes that remove the contaminant or reduce its biological availability. Knowledge regarding the rate by which a contaminant is eliminated from an ecosystem (ecological half-life) is important for evaluating the duration and potential severity of risk. To better understand a contaminants impact on an environment, consideration should be given to plants. As primary producers, they represent an important mode of contamination transfer from sediments and soils into the food chain. Contaminants that are chemically and/or physically sequestered in a media are less likely to be bio-available to plants and therefore an ecosystem.

  10. Redox state of plutonium in irradiated mixed oxide fuels

    NASA Astrophysics Data System (ADS)

    Degueldre, C.; Pin, S.; Poonoosamy, J.; Kulik, D. A.

    2014-03-01

    Nowadays, MOX fuels are used in about 20 nuclear power plants around the world. After irradiation, plutonium co-exists with uranium oxide. Due to the redox sensitive nature of UO2 other plutonium oxides than PuO2 potentially present in the fuel may interact with the matrix. The aim of this study is to determine which plutonium species are present in heterogeneous and homogeneous MOX. The results provided by X-ray Absorption Near Edge Spectroscopy (XANES) for non-irradiated as well as irradiated (center and periphery) homogeneous MOX fuel were published earlier and are completed by Extended X-ray Fine Structure (EXAFS) analysis in this work. The EXAFS signals have been extracted using the ATHENA code and the analyses were carried using EXCURE98 as performed earlier for an analogous element. EXAFS shows that plutonium redox state remains tetravalent in the solid solution and that the minor fraction of trivalent Pu must be below 10%. Independently, the study of homogeneous MOX was also approached by thermodynamics of solid solution of (U,Pu)O2. Such solid solutions were modeled using the Gibbs Energy Minimisation (GEM)-Selektor code (developed at LES, NES, PSI) supported by the literature data on such solid solutions. A comparative study was performed showing which plutonium oxides in their respective mole fractions are more likely to occur in (U,Pu)O2. In the modeling, these oxides were set as ideal and non-ideal solid solutions, as well as separate pure phases. Pu exists mainly as PuO2 in the case of separate phases, but can exist under its reduced forms, PuO1.61 and PuO1.5 in minor fraction i.e. ~15% in ideal solid solution (unlikely) and ~10% in non-ideal solid solution (likely) and at temperature around 1300 K. This combined thermodynamic and EXAFS studies confirm independently the results obtained so far by Pu XANES for the same MOX samples.

  11. Np and Pu Sorption to Manganese Oxide Minerals

    SciTech Connect

    Zhao, P; Johnson, M R; Roberts, S K; Zavarin, M

    2005-08-30

    Manganese oxide minerals are a significant component of the fracture lining mineralogy at Yucca Mountain (Carlos et al., 1993) and within the tuff-confining unit at Yucca Flat (Prothro, 1998), Pahute Mesa (Drellack et al., 1997), and other locations at the Nevada Test Site (NTS). Radionuclide sorption to manganese oxide minerals was not included in recent Lawrence Livermore National Laboratory (LLNL) hydrologic source term (HST) models which attempt to predict the migration behavior of radionuclides away from underground nuclear tests. However, experiments performed for the Yucca Mountain Program suggest that these minerals may control much of the retardation of certain radionuclides, particularly Np and Pu (Triay et al., 1991; Duff et al., 1999). As a result, recent HST model results may significantly overpredict radionuclide transport away from underground nuclear tests. The sorption model used in HST calculations performed at LLNL includes sorption to iron oxide, calcite, zeolite, smectite, and mica minerals (Zavarin and Bruton 2004a; 2004b). For the majority of radiologic source term (RST) radionuclides, we believe that this accounts for the dominant sorption processes controlling transport. However, for the case of Np, sorption is rather weak to all but the iron and manganese oxides (Figure 1). Thus, we can expect to significantly reduce predicted Np transport by accounting for Np sorption to manganese oxides. Similarly, Pu has been shown to be predominantly associated with manganese oxides in Yucca Mountain fractured tuffs (Duff et al., 1999). Recent results on colloid-facilitated Pu transport (Kersting and Reimus, 2003) also suggest that manganese oxide coatings on fracture surfaces may compete with colloids for Pu, thus reducing the effects of colloid-facilitated Pu transport (Figure 1b). The available data suggest that it is important to incorporate Np and Pu sorption to manganese oxides in reactive transport models. However, few data are available for

  12. First results from PuMa: The Dutch Pulsar machine

    NASA Astrophysics Data System (ADS)

    Stappers, B. W.; Ramachandran, R.; Kouwenhoven, M.; Voute, L.

    1998-12-01

    A new pulsar machine, called PuMa, has been developed in the Netherlands and has recently been installed at the Westerbork Synthesis Radio Telescope. PuMa takes advantage of high speed DSPs to carry out FFTs of the incoming data rather than the traditional filter approach to sampling the bandpass. This enables the formation of very fine frequency channels thus greatly improving the ability to correct for dispersion across the bandpass. The system is also very versatile allowing the approriate number channels to be chosen for a particular experiment. As the data are sampled at 20 MHz very high time resolution can also be acheived. It is also possible to record 10 MHz of raw bandwidth which can be coherently dedispersed off-line. I will present the initial results from a number of projects which we are undertaking, including a globular cluster survey, high resolution pulse studies and polarimetry.

  13. Irradiation experiment on fast reactor metal fuels containing minor actinides up to 7 at.% burnup

    SciTech Connect

    Ohta, H.; Yokoo, T.; Ogata, T.; Inoue, T.; Ougier, M.; Glatz, J.P.; Fontaine, B.; Breton, L.

    2007-07-01

    Fast reactor metal fuels containing minor actinides (MAs: Np, Am, Cm) and rare earths (REs) have been irradiated in the fast reactor PHENIX. In this experiment, four types of fuel alloys, U-19Pu-10Zr, U-19Pu-10Zr-2MA-2RE, U-19Pu-10Zr-5MA-5RE and U-19Pu-10Zr-5MA (wt.%), are loaded into part of standard metal fuel stacks. The postirradiation examinations will be conducted at {approx}2.4, {approx}7 and {approx}11 at.% burnup. As for the low-burnup fuel pins, nondestructive postirradiation tests have already been performed and the fuel integrity was confirmed. Furthermore, the irradiation experiment for the intermediate burnup goal of {approx}7 at.% was completed in July 2006. For the irradiation period of 356.63 equivalent full-power days, the neutron flux level remained in the range of 3.5-3.6 x 10{sup 15} n/cm{sup 2}/s at the axial peak position. On the other hand, the maximum linear power of fuel alloys decreased gradually from 305-315 W/cm (beginning of irradiation) to 250-260 W/cm (end of irradiation). The discharged peak burnup was estimated to be 6.59-7.23 at.%. The irradiation behavior of MA-containing metal fuels up to 7 at.% burnup was predicted using the ALFUS code, which was developed for U-Pu-Zr ternary fuel performance analysis. As a result, it was evaluated that the fuel temperature is distributed between {approx}410 deg. C and {approx}645 deg. C at the end of the irradiation experiment. From the stress-strain analysis based on the preliminarily employed cladding irradiation properties and the FCMI stress distribution history, it was predicted that a cladding strain of not more than 0.9% would appear. (authors)

  14. Ultrasound-assisted reductive dissolution of CeO2 and PuO2 in the presence of Ti particles.

    PubMed

    Beaudoux, Xavier; Virot, Matthieu; Chave, Tony; Leturcq, Gilles; Jouan, Gauthier; Venault, Laurent; Moisy, Philippe; Nikitenko, Sergey I

    2016-06-07

    PuO2 is considered an important material for current and future nuclear fuel; however it is a very refractive compound towards dissolution. Among other techniques, its reprocessing can be performed via complexing dissolution in concentrated and boiling nitric acid containing hydrofluoric acid, or via oxidant dissolution in the presence of reagents with redox couples having high potentials such as Ce(iv)/Ce(iii), or Ag(ii)/Ag(i). Reductive dissolution can be performed under softer conditions and is considered an alternative to these methods which may suffer from several drawbacks (corrosion, effluent management, compatibility with nuclear waste disposal, etc.). In this study, a sonochemical and reductive approach is investigated for PuO2 dissolution under relatively mild conditions. At the first stage, the experiments are performed with CeO2 as an inactive surrogate for PuO2. The quantitative dissolution of both oxides can be achieved under ultrasound (20 kHz, 0.35-0.70 W mL(-1)) in 0.5 M HNO3/0.1 M [N2H5NO3]/2 M HCOOH sparged with Ar at 33-35 °C in the presence of Ti particles as a generating source of reductive species. Ultrasound enables the depassivation of the Ti surface (usually strongly passivated in nitric solutions) through acoustic cavitation which then allows further generation of the intermediate Ti(iii) reductive species. Dissolution rates and yields can be further increased with the injection of dilute fluoride aliquots (NH4F or HF) in the sonicated solution to favor Ti chemical depassivation. The rapid and complete dissolution of PuO2 under selected conditions is accompanied by Pu(iii) accumulation in solution.

  15. High temperature investigation of the solid/liquid transition in the PuO2-UO2-ZrO2 system

    NASA Astrophysics Data System (ADS)

    Quaini, A.; Guéneau, C.; Gossé, S.; Sundman, B.; Manara, D.; Smith, A. L.; Bottomley, D.; Lajarge, P.; Ernstberger, M.; Hodaj, F.

    2015-12-01

    The solid/liquid transitions in the quaternary U-Pu-Zr-O system are of great interest for the analysis of core meltdown accidents in Pressurised Water Reactors (PWR) fuelled with uranium-dioxide and MOX. During a severe accident the Zr-based cladding can become completely oxidised due to the interaction with the oxide fuel and the water coolant. In this framework, the present analysis is focused on the pseudo-ternary system UO2-PuO2-ZrO2. The melting/solidification behaviour of five pseudo-ternary and one pseudo-binary ((PuO2)0.50(ZrO2)0.50) compositions have been investigated experimentally by a laser heating method under pre-set atmospheres. The effects of an oxidising or reducing atmosphere on the observed melting/freezing temperatures, as well as the amount of UO2 in the sample, have been clearly identified for the different compositions. The oxygen-to-metal ratio is a key parameter affecting the melting/freezing temperature because of incongruent vaporisation effects. In parallel, a detailed thermodynamic model for the UO2-PuO2-ZrO2 system has been developed using the CALPHAD method, and thermodynamic calculations have been performed to interpret the present laser heating results, as well as the high temperature behaviour of the cubic (Pu,U,Zr)O2±x-c mixed oxide phase. A good agreement was obtained between the calculated and experimental data points. This work enables an improved understanding of the major factors relevant to severe accident in nuclear reactors.

  16. Slow Neutron Velocity Spectrometer Transmission Studies Of Pu

    DOE R&D Accomplishments Database

    Havens, W. W. Jr.; Melkonian, E.; Rainwater, L. J.; Levin, M.

    1951-05-28

    The slow neutron transmission of several samples of Pu has been investigated with the Columbia Neutron Velocity Spectrometer. Data are presented in two groups, those covering the energy region from 0 to 6 ev, and those covering the region above 6 ev. Below 6 ev the resolution was relatively good, and a detailed study of the cross section variation was made. Work above 6 ev consisted of merely locating levels and obtaining a rough idea of their strengths.

  17. Imitators of plutonium and americium in a mixed uranium- plutonium nitride fuel

    NASA Astrophysics Data System (ADS)

    Nikitin, S. N.; Shornikov, D. P.; Tarasov, B. A.; Baranov, V. G.; Burlakova, M. A.

    2016-04-01

    Uranium nitride and mix uranium nitride (U-Pu)N is most popular nuclear fuel for Russian Fast Breeder Reactor. The works in hot cells associated with the radiation exposure of personnel and methodological difficulties. To know the main physical-chemical properties of uranium-plutonium nitride it necessary research to hot cells. In this paper, based on an assessment of physicochemical and thermodynamic properties of selected simulators Pu and Am. Analogues of Pu is are Ce and Y, and analogues Am - Dy. The technique of obtaining a model nitride fuel based on lanthanides nitrides and UN. Hydrogenation-dehydrogenation- nitration method of derived powders nitrides uranium, cerium, yttrium and dysprosium, held their mixing, pressing and sintering, the samples obtained model nitride fuel with plutonium and americium imitation. According to the results of structural studies have shown that all the samples are solid solution nitrides rare earth (REE) elements in UN.

  18. Environmental and radiological safety studies: interaction of /sup 238/PuO/sub 2/ heat sources with terrestrial and aquatic environments. Progress report, April 1-June 30, 1981

    SciTech Connect

    Matlack, G.M.; Patterson, J.H.

    1981-09-01

    The containers for /sup 238/PuO/sub 2/ heat sources in radioisotope thermoelectric generators are designed with large safety factors to ensure they will withstand reentry from orbit and impact with the earth and safely contain the nuclear fuel until it is recovered. Existing designs have proved more than adequately safe, but the Space and Terrestrial Division of the Department of Energy Office of Advanced Nuclear Systems and Projects continually seeks more information about the heat sources to improve their safety. The work discussed here includes studies of the effects on the heat source of terrestrial and aquatic environments to obtain data for design of even safer systems. This report includes data from environmental chamber experiments that simulate terrestrial conditions, experiments to measure PuO/sub 2/ dissolution rates, soil column experiments to measure sorption of plutonium by soils, and several aquatic experiments.

  19. Differential die-away technique for determination of the fissile contents in spent fuel assembly

    SciTech Connect

    Lee, Tachoon; Menlove, Howard O; Swinhoe, Nartyn T; Tobin, Stephen J

    2010-01-01

    Monte Carlo simulations were performed for the differential die-away (DDA) technique to quantify its capability to measure the fissile contents in spent fuel assemblies of 64 different cases in terms of initial enrichment, burnup, and cooling time. The DDA count rate varies according to the contents of fissile isotopes such as {sup 235}U, {sup 239}Pu, and {sup 241}Pu contained in the spent fuel assembly. The effective {sup 239}Pu concept was introduced to quantify the total fissile mass of spent fuel by weighting the relative signal contributions of {sup 235}U and {sup 241}Pu compared to that of {sup 239}Pu. The Monte Carlo simulation results show that the count rate of the DDA instrument for a spent fuel assembly of 4% initial enrichment, 45 GWD/MTU burnup, and 5 year cooling time is {approx} 9.8 x 10{sup 4} counts per second (c/s) with the 100-Hz repeated interrogation pattern of 0 to 10 {micro}s interrogation, 0.2 ms to 1 ms counting time, and 1 x 10{sup 9} n/s neutron source. The {sup 244}Cm neutron background count rate for this counting time scheme is {approx} 1 x 10{sup 4} c/s, and thus the signal to background ratio is {approx}10.

  20. PuMa, the first fully digital pulsar machine.

    NASA Astrophysics Data System (ADS)

    van Haren, P. C.; Voute, J. L. L.; Beijaard, T. D.; Driesens, D.; Kouwenhoven, M. L. A.; Langerak, J. J.

    2000-04-01

    Pulsars are neutron stars, rapidly rotating remains of supernova explosions, emitting bundles of broadband electromagnetic radiation. To carry out pulsar observations, two hurdles have to be overcome. Typically, the signal-to-noise ratio is poor, requiring long observations and large bandwidths. Next there is dispersion, causing the pulsating signals to smear out and calls for narrow signal bands. PuMa, the first Dutch pulsar machine, uses digital signal processing to split the incoming signal in up to thousands of narrow bands. The processor based design also increases flexibility as it allows different observational modes by loading the appropriate software into the signal processors. In total 192 SHARC processors (ADSP 21062) deliver the processing capacity. For PuMa a general purpose 6-processor SHARC board was developed, optimized for concurrent use of data busses. Other parts are commercially available components and all is joined in a VME environment. Mid 1998 PuMa was installed at the Westerbork Synthesis Radio Telescope in the Netherlands and its commissioning is completed.

  1. Pu-238 assay performance with the Canberra IQ3 system

    SciTech Connect

    Booth, L.; Gillespie, B.; Seaman, G.

    1997-11-01

    Canberra Industries has recently completed a demonstration project at the Westinghouse Savannah River Site (WSRC) to characterize 55-gallon drums containing Pu-238 contaminated waste. The goal of this project was to detect and quantify Pu-238 contaminated waste. The goal of this project was to detect and quantify Pu-238 waste to detection limits of less than 50 nCi/g using gamma assay techniques. This would permit reclassification of these drums from transuranic (TRU) waste to low-level waste (LLW). The instrument used for this assay was a Canberra IQ3 high sensitivity gamma assay system, mounted in a trailer. The results of the measurements demonstrate achievement of detection levels as low as 1 nCi/g for low density waste drums, and good correlation with known concentrations in several test drums. In addition, the data demonstrates significant advantages for using large area low-energy germanium detectors for achieving the lowest possible MDAs for gamma rays in the 80-250 keV range. 1 fig., 2 tabs.

  2. Thermal conductivity of heterogeneous LWR MOX fuels

    NASA Astrophysics Data System (ADS)

    Staicu, D.; Barker, M.

    2013-11-01

    It is generally observed that the thermal conductivity of LWR MOX fuel is lower than that of pure UO2. For MOX, the degradation is usually only interpreted as an effect of the substitution of U atoms by Pu. This hypothesis is however in contradiction with the observations of Duriez and Philiponneau showing that the thermal conductivity of MOX is independent of the Pu content in the ranges 3-15 and 15-30 wt.% PuO2 respectively. Attributing this degradation to Pu only implies that stoichiometric heterogeneous MOX can be obtained, while we show that any heterogeneity in the plutonium distribution in the sample introduces a variation in the local stoichiometry which in turn has a strong impact on the thermal conductivity. A model quantifying this effect is obtained and a new set of experimental results for homogeneous and heterogeneous MOX fuels is presented and used to validate the proposed model. In irradiated fuels, this effect is predicted to disappear early during irradiation. The 3, 6 and 10 wt.% Pu samples have a similar thermal conductivity. Comparison of the results for this homogeneous microstructure with MIMAS (heterogeneous) fuel of the same composition showed no difference for the Pu contents of 3, 5.9, 6, 7.87 and 10 wt.%. A small increase of the thermal conductivity was obtained for 15 wt.% Pu. This increase is of about 6% when compared to the average of the values obtained for 3, 6 and 10 wt.% Pu. For comparison purposes, Duriez also measured the thermal conductivity of FBR MOX with 21.4 wt.% Pu with O/M = 1.982 and a density close to 95% TD and found a value in good agreement with the estimation obtained using the formula of Philipponneau [8] for FBR MOX, and significantly lower than his results corresponding to the range 3-15 wt.% Pu. This difference in thermal conductivity is of about 20%, i.e. higher than the measurement uncertainties.Thus, a significant difference was observed between FBR and PWR MOX fuels, but was not explained. This difference

  3. Fabrication of high exposure nuclear fuel pellets

    DOEpatents

    Frederickson, James R.

    1987-01-01

    A method is disclosed for making a fuel pellet for a nuclear reactor. A mixture is prepared of PuO.sub.2 and UO.sub.2 powders, where the mixture contains at least about 30% PuO.sub.2, and where at least about 12% of the Pu is the Pu.sup.240 isotope. To this mixture is added about 0.3 to about 5% of a binder having a melting point of at least about 250.degree. F. The mixture is pressed to form a slug and the slug is granulated. Up to about 4.7% of a lubricant having a melting point of at least about 330.degree. F. is added to the granulated slug. Both the binder and the lubricant are selected from a group consisting of polyvinyl carboxylate, polyvinyl alcohol, naturally occurring high molecular weight cellulosic polymers, chemically modified high molecular weight cellulosic polymers, and mixtures thereof. The mixture is pressed to form a pellet and the pellet is sintered.

  4. Determination of Pu isotopes and 241Am in a reference fallout material using SF-ICP-MS.

    PubMed

    Zheng, Jian; Zhang, Yongsan; Yamada, Masatoshi; Wu, Fengchang; Igarashi, Yasuhito; Hirose, Katsumi

    2011-07-01

    This paper reports on the characterisation of activities of Pu and (241)Am, and Pu isotopic composition in a reference fallout material prepared by the Meteorological Research Institute (MRI), Japan, from samples collected at 14 stations throughout Japan in 1963-1979. The acid leaching and total digestion were used to compare whether there is difference in Pu and (241)Am activities and Pu isotopic composition between these two methods. The results of activities of (239+240)Pu and (241)Pu, and Pu isotopic composition have been reported in the previous work (Sci. Total Environ. 2010, 408, 1139-1144). In this study, the (241)Am activity and (241)Am/(239+240)Pu activity ratio in the reference fallout material are reported, and the usefulness of Pu atom ratios and (241)Am/(239+240)Pu activity ratio for source identification is discussed.

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

    SciTech Connect

    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

  6. Steady-state fuel behavior modeling of nitride fuels in FRAPCON-EP

    NASA Astrophysics Data System (ADS)

    Feng, Bo; Karahan, Aydın; Kazimi, Mujid S.

    2012-08-01

    Fuel material properties and mechanistic fission gas models in FRAPCON-EP were updated to model the steady-state behavior of high-porosity nitride fuel operating at temperatures below half of the melting point. The fuel thermal conductivity and fuel thermal expansion models were updated with correlations for UN and (U,Pu)N fuels. Hot-pressing of the as-fabricated porosity was modeled as a function of the hydrostatic pressure and creep rate. The solid fission product swelling was assumed to increase linearly with burnup. Fission gas swelling constitutive models were updated to appropriately capture the intragranular gas bubble evolution in nitride fuel. Intergranular gas swelling was neglected due to the assumed high porosity of the fuel. The fission gas release behavior was modeled by fitting the fission gas diffusion coefficient in UN to FRAPCON's default fission gas release model. This fitted gas diffusion coefficient reflects the effects of porosity, burnup, operating temperature, fission rate, and bubble sink strength. Fission gas release and fuel swelling benchmarks against irradiation data were performed. The updated code was applied to UN fuel in typical PWR geometry and operating conditions, with an extended cycle length of 24 months. The results show that swelling of the nitride fuel up to 60 MWd/kg burnup did not lead to excessive straining of the cladding. Furthermore, this study showed that a porous (>15% porosity) nitride fuel pellet could achieve a much higher margin to failure from the cladding collapse and grid-to-rod fretting.

  7. Vertical distribution and migration of global fallout Pu in forest soils in southwestern China.

    PubMed

    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 migration of Pu in soil besides precipitation, soil particle size distribution and organic matter were suggested. Long-term migration behaviors of Pu in the soils were simulated. The results provide the Pu background baseline for further environmental monitoring and source identification of non-global fallout Pu inputs in the future.

  8. The hematopoietic transcription factor PU.1 regulates RANK gene expression in myeloid progenitors

    SciTech Connect

    Kwon, Oh Hyung; Lee, Chong-Kil; Lee, Young Ik; Paik, Sang-Gi; Lee, Hyun-Jun . E-mail: hjlee7@kribb.re.kr

    2005-09-23

    Osteoclasts are bone resorbing cells of hematopoietic origin. The hematopoietic transcription factor PU.1 is critical for osteoclastogenesis; however, the molecular mechanisms of PU.1-regulated osteoclastogenesis have not been explored. Here, we present evidence that the receptor activator of nuclear factor {kappa}B (RANK) gene that has been shown to be crucial for osteoclastogenesis is a transcriptional target of PU.1. The PU.1 {sup -/-} progenitor cells failed to express the RANK gene and reconstitution of PU.1 in these cells induced RANK expression. Treatment of the PU.1 reconstituted cells with M-CSF and RANKL further augmented the RANK gene expression. To explore the regulatory mechanism of the RANK gene expression by PU.1, we have cloned the human RANK promoter. Transient transfection assays have revealed that the 2.2-kb RANK promoter was functional in a monocyte line RAW264.7, whereas co-transfection of PU.1 transactivated the RANK promoter in HeLa cells. Taken together, these results suggest that PU.1 regulates the RANK gene transcription and this may represent one of the key roles of PU.1 in osteoclast differentiation.

  9. Pu-erh Tea Inhibits Tumor Cell Growth by Down-Regulating Mutant p53

    PubMed Central

    Zhao, Lanjun; Jia, Shuting; Tang, Wenru; Sheng, Jun; Luo, Ying

    2011-01-01

    Pu-erh tea is a kind of fermented tea with the incorporation of microorganisms’ metabolites. Unlike green tea, the chemical characteristics and bioactivities of Pu-erh tea are still not well understood. Using water extracts of Pu-erh tea, we analyzed the tumor cell growth inhibition activities on several genetically engineered mouse tumor cell lines. We found that at the concentration that did not affect wild type mouse embryo fibroblasts (MEFs) growth, Pu-erh tea extracts could inhibit tumor cell growth by down-regulated S phase and cause G1 or G2 arrest. Further study showed that Pu-erh tea extracts down-regulated the expression of mutant p53 in tumor cells at the protein level as well as mRNA level. The same concentration of Pu-erh tea solution did not cause p53 stabilization or activation of its downstream pathways in wild type cells. We also found that Pu-erh tea treatment could slightly down-regulate both HSP70 and HSP90 protein levels in tumor cells. These data revealed the action of Pu-erh tea on tumor cells and provided the possible mechanism for Pu-erh tea action, which explained its selectivity in inhibiting tumor cells without affecting wild type cells. Our data sheds light on the application of Pu-erh tea as an anti-tumor agent with low side effects. PMID:22174618

  10. Pu-erh tea inhibits tumor cell growth by down-regulating mutant p53.

    PubMed

    Zhao, Lanjun; Jia, Shuting; Tang, Wenru; Sheng, Jun; Luo, Ying

    2011-01-01

    Pu-erh tea is a kind of fermented tea with the incorporation of microorganisms' metabolites. Unlike green tea, the chemical characteristics and bioactivities of Pu-erh tea are still not well understood. Using water extracts of Pu-erh tea, we analyzed the tumor cell growth inhibition activities on several genetically engineered mouse tumor cell lines. We found that at the concentration that did not affect wild type mouse embryo fibroblasts (MEFs) growth, Pu-erh tea extracts could inhibit tumor cell growth by down-regulated S phase and cause G1 or G2 arrest. Further study showed that Pu-erh tea extracts down-regulated the expression of mutant p53 in tumor cells at the protein level as well as mRNA level. The same concentration of Pu-erh tea solution did not cause p53 stabilization or activation of its downstream pathways in wild type cells. We also found that Pu-erh tea treatment could slightly down-regulate both HSP70 and HSP90 protein levels in tumor cells. These data revealed the action of Pu-erh tea on tumor cells and provided the possible mechanism for Pu-erh tea action, which explained its selectivity in inhibiting tumor cells without affecting wild type cells. Our data sheds light on the application of Pu-erh tea as an anti-tumor agent with low side effects.

  11. Ab-Initio Study on Plutonium Compounds Pu3M (M=Al, Ga, In), PuNp and Elemental Neptunium

    SciTech Connect

    Kutepov, A L

    2005-09-07

    Using spin-polarized relativistic density functional theory the electronic and magnetic structures for the plutonium compounds Pu{sub 3}M(M = Al; Ga; In) and PuNp have been investigated. For the first group of compounds the enhanced hybridization between Pu 5f and p-states of alloying element, as it has been found in spin-polarized calculations, is believed to be the main reason for the higher formation energies obtained in such kind of studies in comparison with the non-spin-polarized case. Also, comparative analysis of the actinides U, Np, Pu, Am, and Cm has been performed based on their electronic and magnetic structure. Some noticeable difference in the calculated magnetic structure was discovered between the actinide with local magnetic moments (Cm) and the actinides (Pu, Am) in which magnetic moments were found only in the calculations.

  12. Alternative Fuels

    EPA Pesticide Factsheets

    Alternative fuels include gaseous fuels such as hydrogen, natural gas, and propane; alcohols such as ethanol, methanol, and butanol; vegetable and waste-derived oils; and electricity. Overview of alternative fuels is here.

  13. Safety Report - Experiments 999 and 891 Muon Spin Relaxation in Pu and Pu-based Heavy Fermion Materials

    SciTech Connect

    Fluss, M; Heffner, R; Morris, G

    2004-04-23

    Experiment E999 proposes to carry out conventional muon spin relaxation ({mu}SR) measurements on solid samples of plutonium and plutonium alloys. Experiment 891 will be involved with {mu}SR experiments on PuCoGa{sub 5} and related Pu-based superconductors. Other than a dedicated cryostat to be provided by Los Alamos and a pumping station provided by Livermore, the experiments will use existing {mu}SR User Facility spectrometers and associated equipment such as detectors and electronics. The main topics of this report are therefore (1) the passivation of the samples with a polymer coating, (2) the design, fabrication and testing of a sealed titanium sample secondary encapsulation cell, (3) the transport of samples to and from TRIUMF and (4) the related on-site procedures for the safe handling of the encapsulated samples. Because both E999 and E891 share the same equipment and Pu-safety related issues, we are submitting a single safety report for both experiments.

  14. 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.

    PubMed

    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.

  15. Fuel pin

    DOEpatents

    Christiansen, David W.; Karnesky, Richard A.; Leggett, Robert D.; Baker, Ronald B.

    1989-01-01

    A fuel pin for a liquid metal nuclear reactor is provided. The fuel pin includes a generally cylindrical cladding member with metallic fuel material disposed therein. At least a portion of the fuel material extends radially outwardly to the inner diameter of the cladding member to promote efficient transfer of heat to the reactor coolant system. The fuel material defines at least one void space therein to facilitate swelling of the fuel material during fission.

  16. Fuel pin

    DOEpatents

    Christiansen, D.W.; Karnesky, R.A.; Leggett, R.D.; Baker, R.B.

    1987-11-24

    A fuel pin for a liquid metal nuclear reactor is provided. The fuel pin includes a generally cylindrical cladding member with metallic fuel material disposed therein. At least a portion of the fuel material extends radially outwardly to the inner diameter of the cladding member to promote efficient transfer of heat to the reactor coolant system. The fuel material defines at least one void space therein to facilitate swelling of the fuel material during fission.

  17. Fuel pin

    DOEpatents

    Christiansen, David W.; Karnesky, Richard A.; Leggett, Robert D.; Baker, Ronald B.

    1989-10-03

    A fuel pin for a liquid metal nuclear reactor is provided. The fuel pin includes a generally cylindrical cladding member with metallic fuel material disposed therein. At least a portion of the fuel material extends radially outwardly to the inner diameter of the cladding member to promote efficient transfer of heat to the reactor coolant system. The fuel material defines at least one void space therein to facilitate swelling of the fuel material during fission.

  18. Safeguards Considerations for Thorium Fuel Cycles

    DOE PAGES

    Worrall, Louise G.; Worrall, Andrew; Flanagan, George F.; ...

    2016-04-21

    We report that by around 2025, thorium-based fuel cycles are likely to be deployed internationally. States such as China and India are pursuing research, development, and deployment pathways toward a number of commercial-scale thorium fuel cycles, and they are already building test reactors and the associated fuel cycle infrastructure. In the future, the potential exists for these emerging programs to sell, export, and deploy thorium fuel cycle technology in other states. Without technically adequate international safeguards protocols and measures in place, any future potential clandestine misuse of these fuel cycles could go undetected, compromising the deterrent value of these protocolsmore » and measures. The development of safeguards approaches for thorium-based fuel cycles is therefore a matter of some urgency. Yet, the focus of the international safeguards community remains mainly on safeguarding conventional 235U- and 239Pu-based fuel cycles while the safeguards challenges of thorium-uranium fuel cycles remain largely uninvestigated. This raises the following question: Is the International Atomic Energy Agency and international safeguards system ready for thorium fuel cycles? Furthermore, is the safeguards technology of today sufficiently mature to meet the verification challenges posed by thorium-based fuel cycles? In defining these and other related research questions, the objectives of this paper are to identify key safeguards considerations for thorium-based fuel cycles and to call for an early dialogue between the international safeguards and the nuclear fuel cycle communities to prepare for the potential safeguards challenges associated with these fuel cycles. In this paper, it is concluded that directed research and development programs are required to meet the identified safeguards challenges and to take timely action in preparation for the international deployment of thorium fuel cycles.« less

  19. Safeguards Considerations for Thorium Fuel Cycles

    SciTech Connect

    Worrall, Louise G.; Worrall, Andrew; Flanagan, George F.; Croft, Steven

    2016-04-21

    We report that by around 2025, thorium-based fuel cycles are likely to be deployed internationally. States such as China and India are pursuing research, development, and deployment pathways toward a number of commercial-scale thorium fuel cycles, and they are already building test reactors and the associated fuel cycle infrastructure. In the future, the potential exists for these emerging programs to sell, export, and deploy thorium fuel cycle technology in other states. Without technically adequate international safeguards protocols and measures in place, any future potential clandestine misuse of these fuel cycles could go undetected, compromising the deterrent value of these protocols and measures. The development of safeguards approaches for thorium-based fuel cycles is therefore a matter of some urgency. Yet, the focus of the international safeguards community remains mainly on safeguarding conventional 235U- and 239Pu-based fuel cycles while the safeguards challenges of thorium-uranium fuel cycles remain largely uninvestigated. This raises the following question: Is the International Atomic Energy Agency and international safeguards system ready for thorium fuel cycles? Furthermore, is the safeguards technology of today sufficiently mature to meet the verification challenges posed by thorium-based fuel cycles? In defining these and other related research questions, the objectives of this paper are to identify key safeguards considerations for thorium-based fuel cycles and to call for an early dialogue between the international safeguards and the nuclear fuel cycle communities to prepare for the potential safeguards challenges associated with these fuel cycles. In this paper, it is concluded that directed research and development programs are required to meet the identified safeguards challenges and to take timely action in preparation for the international deployment of thorium fuel cycles.

  20. In vitro dissolution of respirable aerosols of industrial uranium and plutonium mixed-oxide nuclear fuels.

    PubMed

    Eidson, A F; Mewhinney, J A

    1983-12-01

    Dissolution characteristics of mixed-oxide nuclear fuels are important considerations for prediction of biological behavior of inhaled particles. Four representative industrial mixed-oxide powders were obtained from fuel fabrication enclosures. Studies of the dissolution of Pu, Am and U from aerosol particles of these materials in a serum simulant solution and in 0.1M HCl showed: (1) dissolution occurred at a rapid rate initially and slowed at longer times, (2) greater percentages of U dissolved than Pu or Am: with the dissolution rates of U and Pu generally reflecting the physical nature of the UO2-PuO2 matrix, (3) the temperature history of industrial mixed-oxides could not be reliably related to Pu dissolution except for a 3-5% increase when incorporated into a solid solution by sintering at 1750 degrees C, and (4) dissolution in the serum simulant agreed with the in vivo UO2 dissolution rate and suggested the dominant role of mechanical processes in PuO2 clearance from the lung. The rapid initial dissolution rate was shown to be related, in part, to an altered surface layer. The advantages and uses of in vitro solubility data for estimation of biological behavior of inhaled industrial mixed oxides, such as assessing the use of chelation therapy and interpretation of urinary excretion data, are discussed. It was concluded that in vitro solubility tests were useful, simple and easily applied to individual materials potentially inhaled by humans.

  1. Molecular Dynamics study of the mixed oxide fuel thermal conductivity

    NASA Astrophysics Data System (ADS)

    Nichenko, S.; Staicu, D.

    2013-08-01

    There is still no clear understanding of the plutonium content influence on the thermal conductivity behaviour of the (U,Pu) O2 MOX fuels. In this work Classical Molecular Dynamics (MD) was used to investigate the (U,Pu) O2 thermal conductivity in the whole concentration range and in the temperature range from 400 K to 1600 K. The Green-Kubo approach was used for the thermal conductivity calculation and an algorithm was proposed to improve the accuracy of the calculation. The obtained results are in good agreement with the literature experimental data and results of modelling of other authors. On the basis of the obtained results we give recommendations for the MOX thermal conductivity evaluation in the concentration range from pure UO2 up to pure PuO2.

  2. Roles of PU.1 in monocyte- and mast cell-specific gene regulation: PU.1 transactivates CIITA pIV in cooperation with IFN-gamma.

    PubMed

    Ito, Tomonobu; Nishiyama, Chiharu; Nakano, Nobuhiro; Nishiyama, Makoto; Usui, Yoshihiko; Takeda, Kazuyoshi; Kanada, Shunsuke; Fukuyama, Kanako; Akiba, Hisaya; Tokura, Tomoko; Hara, Mutsuko; Tsuboi, Ryoji; Ogawa, Hideoki; Okumura, Ko

    2009-07-01

    Over-expression of PU.1, a myeloid- and lymphoid-specific transcription factor belonging to the Ets family, induces monocyte-specific gene expression in mast cells. However, the effects of PU.1 on each target gene and the involvement of cytokine signaling in PU.1-mediated gene expression are largely unknown. In the present study, PU.1 was over-expressed in two different types of bone marrow-derived cultured mast cells (BMMCs): BMMCs cultured with IL-3 plus stem cell factor (SCF) and BMMCs cultured with pokeweed mitogen-stimulated spleen-conditioned medium (PWM-SCM). PU.1 over-expression induced expression of MHC class II, CD11b, CD11c and F4/80 on PWM-SCM-cultured BMMCs, whereas IL-3/SCF-cultured BMMCs expressed CD11b and F4/80, but not MHC class II or CD11c. When IFN-gamma was added to the IL-3/SCF-based medium, PU.1 transfectant acquired MHC class II expression, which was abolished by antibody neutralization or in Ifngr(-/-) BMMCs, through the induction of expression of the MHC class II transactivator, CIITA. Real-time PCR detected CIITA mRNA driven by the fourth promoter, pIV, and chromatin immunoprecipitation indicated direct binding of PU.1 to pIV in PU.1-over-expressing BMMCs. PU.1-over-expressing cells showed a marked increase in IL-6 production in response to LPS stimulation in both IL-3/SCF and PWM-SCM cultures. These results suggest that PU.1 overproduction alone is sufficient for both expression of CD11b and F4/80 and for amplification of LPS-induced IL-6 production. However, IFN-gamma stimulation is essential for PU.1-mediated transactivation of CIITA pIV. Reduced expression of mast cell-related molecules and transcription factors GATA-1/2 and up-regulation of C/EBPalpha in PU.1 transfectants indicate that enforced PU.1 suppresses mast cell-specific gene expression through these transcription factors.

  3. Soft X-ray Studies of Pu Electronic Structure: Past Lessons and Future Directions

    SciTech Connect

    Tobin, J G; Yu, S W

    2008-02-07

    Photoelectron Spectroscopy (PES) and X-ray Absorption Spectroscopy (XAS, Figure 1) have contributed greatly to our improved understanding of Pu electronic structure. From these and related measurements, the following has been determined: (1) The Pu 5f spin-orbit splitting is large; (2) The number of Pu5f electrons is near 5; and (3) The Pu 5f spin-orbit splitting effect dominates 5f itineracy. Significant questions remain concerning the nature of Pu electronic structure. Perhaps the missing piece of the puzzle is the direct experimental determination of the unoccupied electronic structure using high energy inverse photoelectron spectroscopy or Bremstrahlung Isochromat Spectroscopy (BIS). Past BIS studies of Th and U indicate the feasibility and utility of Pu studies.

  4. Microstructure changes caused by annealing of U-Pu-Zr alloys

    NASA Astrophysics Data System (ADS)

    Janney, Dawn E.; Sencer, Bulent H.

    2017-04-01

    Thermally induced microstructural changes in five uranium-plutonium-zirconium alloys (38U-22Pu-40Zr, 49U-19Pu-32Zr, 33U-27Pu-40Zr, 19U-41Pu-40Zr, and 20U-12Pu-68Zr, compositions in at%) were examined by comparing as-cast alloys with alloys that had been annealed at 500 °C for 168 h using scanning electron microscopy. All of the as-cast and annealed alloys had high-Zr inclusions not predicted from currently available phase diagrams. Microstructures in all alloys except U-12Pu-68Zr demonstrate increasing development of irregularly shaped polygons with high-actinide, low-Zr boundaries as a result of annealing.

  5. Fuel pump

    SciTech Connect

    Bellis, P.D.; Nesselrode, F.

    1991-04-16

    This patent describes a fuel pump. It includes: a fuel reservoir member, the fuel reservoir member being formed with fuel chambers, the chambers comprising an inlet chamber and an outlet chamber, means to supply fuel to the inlet chamber, means to deliver fuel from the outlet chamber to a point of use, the fuel reservoir member chambers also including a bypass chamber, means interconnecting the bypass chamber with the outlet chamber; the fuel pump also comprising pump means interconnecting the inlet chamber and the outlet chamber and adapted to suck fuel from the fuel supply means into the inlet chamber, through the pump means, out the outlet chamber, and to the fuel delivery means; the bypass chamber and the pump means providing two substantially separate paths of fuel flow in the fuel reservoir member, bypass plunger means normally closing off the flow of fuel through the bypass chamber one of the substantially separate paths including the fuel supply means and the fuel delivery means when the bypass plunger means is closed, the second of the substantially separate paths including the bypass chamber when the bypass plunger means is open, and all of the chambers and the interconnecting means therebetween being configured so as to create turbulence in the flow of any fuel supplied to the outlet chamber by the pump means and bypassed through the bypass chamber and the interconnecting means.

  6. Enhancing BWR proliferation resistance fuel with minor actinides

    NASA Astrophysics Data System (ADS)

    Chang, Gray S.

    2009-03-01

    To reduce spent fuel for storage and enhance the proliferation resistance for the intermediate-term, there are two major approaches (a) increase the discharged spent fuel burnup in the advanced light water reactor- LWR (Gen-III Plus), which not only can reduce the spent fuel for storage, but also increase the 238Pu isotopes ratio to enhance the proliferation resistance, and (b) use of transuranic nuclides ( 237Np and 241Am) in the high burnup fuel, which can drastically increase the proliferation resistance isotope ratio of 238Pu/Pu. For future advanced nuclear systems, minor actinides (MA) are viewed more as a resource to be recycled, and transmuted to less hazardous and possibly more useful forms, rather than simply disposed of as a waste stream in an expensive repository facility. As a result, MAs play a much larger part in the design of advanced systems and fuel cycles, not only as additional sources of useful energy, but also as direct contributors to the reactivity control of the systems into which they are incorporated. In the study, a typical boiling water reactor (BWR) fuel unit lattice cell model with UO 2 fuel pins will be used to investigate the effectiveness of minor actinide reduction approach (MARA) for enhancing proliferation resistance and improving the fuel cycle performance in the intermediate-term goal for future nuclear energy systems. To account for the water coolant density variation from the bottom (0.76 g/cm 3) to the top (0.35 g/cm 3) of the core, the axial coolant channel and fuel pin were divided to 24 nodes. The MA transmutation characteristics at different elevations were compared and their impact on neutronics criticality discussed. The concept of MARA, which involves the use of transuranic nuclides ( 237Np and/or 241Am), significantly increases the 238Pu/Pu ratio for proliferation resistance, as well as serves as a burnable absorber to hold-down the initial excess reactivity. It is believed that MARA can play an important role in

  7. Enhancing BWR Proliferation Resistance Fuel with Minor Actinides

    SciTech Connect

    Gray S. Chang

    2009-03-01

    To reduce spent fuel for storage and enhance the proliferation resistance for the intermediate-term, there are two major approaches (a) increase the discharged spent fuel burnup in the advanced light water reactor- LWR (Gen-III Plus), which not only can reduce the spent fuel for storage, but also increase the 238Pu isotopes ratio to enhance the proliferation resistance, and (b) use of transuranic nuclides (237Np and 241Am) in the high burnup fuel, which can drastically increase the proliferation resistance isotope ratio of 238Pu/Pu. For future advanced nuclear systems, minor actinides (MA) are viewed more as a resource to be recycled, and transmuted to less hazardous and possibly more useful forms, rather than simply disposed of as a waste stream in an expensive repository facility. As a result, MAs play a much larger part in the design of advanced systems and fuel cycles, not only as additional sources of useful energy, but also as direct contributors to the reactivity control of the systems into which they are incorporated. In the study, a typical boiling water reactor (BWR) fuel unit lattice cell model with UO2 fuel pins will be used to investigate the effectiveness of minor actinide reduction approach (MARA) for enhancing proliferation resistance and improving the fuel cycle performance in the intermediate-term goal for future nuclear energy systems. To account for the water coolant density variation from the bottom (0.76 g/cm3) to the top (0.35 g/cm3) of the core, the axial coolant channel and fuel pin were divided to 24 nodes. The MA transmutation characteristics at different elevations were compared and their impact on neutronics criticality discussed. The concept of MARA, which involves the use of transuranic nuclides (237Np and/or 241Am), significantly increases the 238Pu/Pu ratio for proliferation resistance, as well as serves as a burnable absorber to hold-down the initial excess reactivity. It is believed that MARA can play an important role in atoms

  8. Analysis of spent fuel assay with a lead slowing down spectrometer

    SciTech Connect

    Gavron, Victor I; Smith, L Eric; Ressler, Jennifer J

    2008-01-01

    Assay of fissile materials in spent fuel that are produced or depleted during the operation of a reactor, is of paramount importance to nuclear materials accounting, verification of the reactor operation history, as well as for criticality considerations for storage. In order to prevent future proliferation following the spread of nuclear energy, we must develop accurate methods to assay large quantities of nuclear fuels. We analyze the potential of using a Lead Slowing Down Spectrometer for assaying spent fuel. We conclude that it is possible to design a system that will provide around 1% statistical precision in the determination of the {sup 239}Pu, {sup 241}Pu and {sup 235}U concentrations in a PWR spent-fuel assembly, for intermediate-to-high burnup levels, using commercial neutron sources, and a system of {sup 238}U threshold fission detectors. Pending further analysis of systematic errors, it is possible that missing pins can be detected, as can asymmetry in the fuel bundle.

  9. Analysis of spent fuel assay with a lead slowing down spectrometer

    SciTech Connect

    Gavron, Victor I; Smith, L. Eric; Ressler, Jennifer J

    2010-10-29

    Assay of fissile materials in spent fuel that are produced or depleted during the operation of a reactor, is of paramount importance to nuclear materials accounting, verification of the reactor operation history, as well as for criticality considerations for storage. In order to prevent future proliferation following the spread of nuclear energy, we must develop accurate methods to assay large quantities of nuclear fuels. We analyze the potential of using a Lead Slowing Down Spectrometer for assaying spent fuel. We conclude that it is possible to design a system that will provide around 1% statistical precision in the determination of the {sup 239}Pu, {sup 241}Pu and {sup 235}U concentrations in a PWR spent-fuel assembly, for intermediate-to-high burnup levels, using commercial neutron sources, and a system of {sup 238}U threshold fission detectors. Pending further analysis of systematic errors, it is possible that missing pins can be detected, as can asymmetry in the fuel bundle.

  10. Removal of Pu238 from Neptunium Solution by Anion Exchange

    SciTech Connect

    KYSER, EDWARD

    2003-12-01

    A new anion flowsheet for use in HB-Line was tested in the lab with Reillex{trademark} HPQ for removal of Pu{sup 238} contamination from Np. Significant rejection of Pu{sup 238} was observed by washing with 6 to 12 bed volumes (BV) of reductive wash containing reduced nitric acid concentration along with both ferrous sulfamate (FS) and hydrazine. A shortened-height column was utilized in these tests to match changes in the plant equipment. Lab experiments scaled to plant batch sizes of 1500 to 2200 g Np were observed with modest losses for up-flow washing. Down-flow washing was observed to have high losses. The following are recommended conditions for removing Pu{sup 238} from Np solutions by anion exchange in HB-Line: (1) Feed conditions: Up-flow 6.4-8 M HNO{sub 3}, 0.02 M hydrazine, 0.05 M excess FS, less than 5 days storage of solution after FS addition. (2) Reductive Wash conditions: Up-flow 6-12 BV of 6.4 M HNO{sub 3}, 0.05 M FS, 0.05 M hydrazine. 1.8 mL/min/cm{sup 2} flowrate. (3) Decontamination Wash conditions: Up-flow 1-2 BV of 6.4-8 M HNO{sub 3}, no FS, no hydrazine. (4) Elution conditions: Down-flow 0.17 M HNO{sub 3}, 0.05 M hydrazine, no FS.

  11. Testing New Inert Matrix and Thoria Fuels for Plutonium Incineration

    SciTech Connect

    Vettraino, F.; Padovan, E.; Tverberg, T.

    2002-07-01

    One major issue for nuclear power continues to be the public concern about rad-waste and proliferation risk induced by large plutonium stockpiles accumulated worldwide. In this context, nuclear fuels which exhibit no-plutonium production, and possibly allow for an efficient utilization of the plutonium to get rid of, are of great interest. This is the basic reason for the efforts that many international institutions are devoting to R and D on such new U-free fuel concepts as Inert Matrix (IMF) and Thorium fuels. At the moment the major merit of such innovative fuels is primarily related to the safe closure of the nuclear fuel cycle as especially expected from those new concepts like ADS (Accelerated Driven System) for the transmutation of plutonium, minor actinides and LLFP. Both ceramic inert matrix (IM) and thoria (T) fuels have been identified as suitable to the scope of burning weapon and civilian plutonium and to act also as possible carrier for transmutation of minor actinides. For testing the irradiation behaviour of these new materials, three kinds of fuels have been selected: inert matrix (IM) fuel, inert matrix thoria-doped (IMT) fuel, and thoria (T) fuel. A first experiment, IFA-652, 40 MWD/kg burnup target, including high enriched uranium (HEU) as fissile phase, instead of plutonium, is currently underway in the Halden HWBR. The reason for this choice was that manufacturing of Pu containing fuels is more complex and there was no fabrication facility available at the needed time for the Pu fuel. It is expected, however, that the relative behaviour of the different kind of matrices would be only slightly dependent on the adopted fissile material. So, the comparison of the in-pile performance of the three fuels will constitute a significant common database also for plutonium bearing fuels. The primary aim for the IFA-652 experiment is the measurement of basic characteristics under LWR irradiation conditions over a period of 4-5 years. The design of a

  12. Final Report on Two-Stage Fast Spectrum Fuel Cycle Options

    SciTech Connect

    Yang, Won Sik; Lin, C. S.; Hader, J. S.; Park, T. K.; Deng, P.; Yang, G.; Jung, Y. S.; Kim, T. K.; Stauff, N. E.

    2016-01-30

    This report presents the performance characteristics of two “two-stage” fast spectrum fuel cycle options proposed to enhance uranium resource utilization and to reduce nuclear waste generation. One is a two-stage fast spectrum fuel cycle option of continuous recycle of plutonium (Pu) in a fast reactor (FR) and subsequent burning of minor actinides (MAs) in an accelerator-driven system (ADS). The first stage is a sodium-cooled FR fuel cycle starting with low-enriched uranium (LEU) fuel; at the equilibrium cycle, the FR is operated using the recovered Pu and natural uranium without supporting LEU. Pu and uranium (U) are co-extracted from the discharged fuel and recycled in the first stage, and the recovered MAs are sent to the second stage. The second stage is a sodium-cooled ADS in which MAs are burned in an inert matrix fuel form. The discharged fuel of ADS is reprocessed, and all the recovered heavy metals (HMs) are recycled into the ADS. The other is a two-stage FR/ADS fuel cycle option with MA targets loaded in the FR. The recovered MAs are not directly sent to ADS, but partially incinerated in the FR in order to reduce the amount of MAs to be sent to the ADS. This is a heterogeneous recycling option of transuranic (TRU) elements

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

    PubMed

    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.

  14. Experimental geochemistry of Pu and Sm and the thermodynamics of trace element partitioning

    NASA Technical Reports Server (NTRS)

    Jones, John H.; Burnett, Donald S.

    1987-01-01

    An experimental study of the partitioning of Pu and Sm between diopside/liquid and whitlockite/liquid supports the hypothesis that Pu behaves as a light rare earth element during igneous processes in reducing environments. D-Pu/D-Sm is found to be about 2 for both diopsidic pyroxene and whitlockite, and the amount of fractionation would be decreased further if Pu were compared to Ce or Nd. Data indicate that temperature, rather than melt composition, is the most important control on elemental partitioning, and that P2O5 in aluminosilicate melts serves as a complexing agent for the actinides and lanthanides.

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

    PubMed

    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.

  16. Neutron producing reactions in PuBe neutron sources

    NASA Astrophysics Data System (ADS)

    Bagi, János; Lakosi, László; Nguyen, Cong Tam

    2016-01-01

    There are a plenty of out-of-use plutonium-beryllium neutron sources in Eastern Europe presenting both nuclear safeguards and security issues. Typically, their actual Pu content is not known. In the last couple of years different non-destructive methods were developed for their characterization. For such methods detailed knowledge of the nuclear reactions taking place within the source is necessary. In this paper we investigate the role of the neutron producing reactions, their contribution to the neutron yield and their dependence on the properties of the source.

  17. Neutron Resonance Parameters and Covariance Matrix of 239Pu

    SciTech Connect

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

    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.

  18. First-principles elastic properties of (alpha)-Pu

    SciTech Connect

    Soderlind, P; Klepeis, J E

    2008-11-04

    Density-functional electronic structure calculations have been used to investigate the ambient pressure and low temperature elastic properties of the ground-state {alpha} phase of plutonium metal. The electronic structure and correlation effects are modeled within a fully relativistic anti-ferromagnetic treatment with a generalized gradient approximation for the electron exchange and correlation functionals. The 13 independent elastic constants, for the monoclinic {alpha}-Pu system, are calculated for the observed geometry. A comparison of the results with measured data from resonant ultrasound spectroscopy for a cast sample is made.

  19. The alpha-decay of Pu-236 to U-232

    NASA Astrophysics Data System (ADS)

    Ardisson, G.; Bosschot, J. M.; Hussonnois, M.; Le Du, J. F.; Trubert, D.; Lederer, C. M.

    1994-10-01

    The gamma-spectrum following the alpha-decay of Pu-236 was reinvestigated using a high resolution HPGe detector. The energy and intensity of 26 gamma-transitions were measured accurately; 21 of these were observed for the first time. All gamma-rays were placed in a U-232 level scheme accounting for 13 levels of which 8 are reported for the first time. The ground state rotational band was found to be fed up to spin I (sup pi) = 8(sup +) and the K(sup pi) = 0(sup-) octupole band to be fed up to I = 5.

  20. Status of the Norwegian thorium light water reactor (LWR) fuel development and irradiation test program

    SciTech Connect

    Drera, S.S.; Bjork, K.I.; Kelly, J.F.; Asphjell, O.

    2013-07-01

    Thorium based fuels offer several benefits compared to uranium based fuels and should thus be an attractive alternative to conventional fuel types. In order for thorium based fuel to be licensed for use in current LWRs, material properties must be well known for fresh as well as irradiated fuel, and accurate prediction of fuel behavior must be possible to make for both normal operation and transient scenarios. Important parameters are known for fresh material but the behaviour of the fuel under irradiation is unknown particularly for low Th content. The irradiation campaign aims to widen the experience base to irradiated (Th,Pu)O{sub 2} fuel and (Th,U)O{sub 2} with low Th content and to confirm existing data for fresh fuel. The assumptions with respect to improved in-core fuel performance are confirmed by our preliminary irradiation test results, and our fuel manufacture trials so far indicate that both (Th,U)O{sub 2} and (Th,Pu)O{sub 2} fuels can be fabricated with existing technologies, which are possible to upscale to commercial volumes.

  1. Recycle of scrap plutonium-238 oxide fuel to support future radioisotope applications

    NASA Astrophysics Data System (ADS)

    Schulte, Louis D.; Purdy, Geraldine M.; Jarvinen, Gordon D.; Ramsey, Kevin; Silver, Gary L.; Espinoza, Jacob; Rinehart, Gary H.

    1998-01-01

    The Nuclear Materials Technology (NMT) Division of Los Alamos National Laboratory has initiated a development program to recover & purify plutonium-238 oxide from impure feed sources in a glove box environment. A glove box line has been designed and a chemistry flowsheet developed to perform this recovery task at large scale. The initial demonstration effort focused on purification of 238PuO2 fuel by HNO3/HF dissolution, followed by plutonium(III) oxalate precipitation and calcination to an oxide. Decontamination factors for most impurities of concern in the fuel were very good, producing 238PuO2 fuel significantly better in purity than specified by General Purpose Heat Source (GPHS) fuel powder specifications. A sufficient quantity of purified 238PuO2 fuel was recovered from the process to allow fabrication of a GPHS unit for testing. The results are encouraging for recycle of relatively impure plutonium-238 oxide and scrap residue items into fuel for useful applications. The high specific activity of plutonium-238 magnifies the consequences and concerns of radioactive waste generation. This work places an emphasis on development of waste minimization technologies to complement the aqueous processing operation. Results from experiments on neutralized solutions of plutonium-238 resulted in decontamination to about 1 millicurie/L. Combining ultrafiltration treatment with addition of a water-soluble polymer designed to coordinate Pu, allowed solutions to be decontaminated to about 1 microcurie/L. Efforts continue to develop a capability for efficient, safe, cost-effective, and environmentally acceptable methods to recover and purify 238PuO2 fuel.

  2. Analysis of IFR driver fuel hot channel factors

    SciTech Connect

    Ku, J.Y.; Chang, L.K.; Mohr, D.

    1994-03-01

    Thermal-hydraulic uncertainty factors for Integral Fast Reactor (IFR) driver fuels have been determined based primarily on the database obtained from the predecessor fuels used in the IFR prototype, Experimental Breeder Reactor II. The uncertainty factors were applied to the channel factors (HCFs) analyses to obtain separate overall HCFs for fuel and cladding for steady-state analyses. A ``semistatistical horizontal method`` was used in the HCFs analyses. The uncertainty factor of the fuel thermal conductivity dominates the effects considered in the HCFs analysis; the uncertainty in fuel thermal conductivity will be reduced as more data are obtained to expand the currently limited database for the IFR ternary metal fuel (U-20Pu-10Zr). A set of uncertainty factors to be used for transient analyses has also been derived.

  3. Estimate of the Sources of Plutonium-Containing Wastes Generated from MOX Fuel Production in Russia

    SciTech Connect

    Kudinov, K. G.; Tretyakov, A. A.; Sorokin, Yu. P.; Bondin, V. V.; Manakova, L. F.; Jardine, L. J.

    2002-02-26

    In Russia, mixed oxide (MOX) fuel is produced in a pilot facility ''Paket'' at ''MAYAK'' Production Association. The Mining-Chemical Combine (MCC) has developed plans to design and build a dedicated industrial-scale plant to produce MOX fuel and fuel assemblies (FA) for VVER-1000 water reactors and the BN-600 fast-breeder reactor, which is pending an official Russian Federation (RF) site-selection decision. The design output of the plant is based on a production capacity of 2.75 tons of weapons plutonium per year to produce the resulting fuel assemblies: 1.25 tons for the BN-600 reactor FAs and the remaining 1.5 tons for VVER-1000 FAs. It is likely the quantity of BN-600 FAs will be reduced in actual practice. The process of nuclear disarmament frees a significant amount of weapons plutonium for other uses, which, if unutilized, represents a constant general threat. In France, Great Britain, Belgium, Russia, and Japan, reactor-grade plutonium is used in MOX-fuel production. Making MOX-fuel for CANDU (Canada) and pressurized water reactors (PWR) (Europe) is under consideration in Russia. If this latter production is added, as many as 5 tons of Pu per year might be processed into new FAs in Russia. Many years of work and experience are represented in the estimates of MOX fuel production wastes derived in this report. Prior engineering studies and sludge treatment investigations and comparisons have determined how best to treat Pu sludges and MOX fuel wastes. Based upon analyses of the production processes established by these efforts, we can estimate that there will be approximately 1200 kg of residual wastes subject to immobilization per MT of plutonium processed, of which approximately 6 to 7 kg is Pu in the residuals per MT of Pu processed. The wastes are various and complicated in composition. Because organic wastes constitute both the major portion of total waste and of the Pu to be immobilized, the recommended treatment of MOX-fuel production waste is

  4. Decreased solubilization of Pu(IV) polymers by humic acids under anoxic conditions

    NASA Astrophysics Data System (ADS)

    Xie, Jinchuan; Lin, Jianfeng; Liang, Wei; Li, Mei; Zhou, Xiaohua

    2016-11-01

    Pu(IV) polymer has a very low solubility (log[Pu(IV)aq]total = -10.4 at pH 7.2 and I = 0). However, some aspects of their environmental fate remain unclear. Humic acids are able to complex with Pu4+ ions and their dissolved species (<10 kD) in the groundwater (neutral to alkaline pH) may cause solubilization of the polymers. Also, humic acids have the native reducing capacity and potentially reduce the polymeric Pu(IV) to Pu(III)aq (log[Pu(III)aq]total = -5.3 at pH 7.2 and I = 0). Solubilization and reduction of the polymers can enhance their mobility in subsurface environments. Nevertheless, humic acids readily coat the surfaces of metal oxides via electrostatic interaction and ligand exchange mechanisms. The humic coatings are expected to prevent both solubilization and reduction of the polymers. Experiments were conducted under anoxic and slightly alkaline (pH 7.2) conditions in order to study whether humic acids have effects on stability of the polymers. The results show that the polymeric Pu(IV) was almost completely transformed into aqueous Pu(IV) in the presence of EDTA ligands. In contrast, the dissolved humic acids did not solubilize the polymers but in fact decreased their solubility by one order of magnitude. The humic coatings were responsible for the decreased solubilization. Such coatings limited the contact between the polymers and EDTA ligands, especially at the relatively high concentrations of humic acids (>0.57 mg/L). Solubilization of the humic-coated polymers was thus inhibited to a significant extent although EDTA, having the great complexation ability, was present in the humic solutions. Reduction of Pu(IV) polymers by the humic acids was also not observed in the absence of EDTA. In the presence of EDTA, the polymers were partially reduced to Pu(III)aq by the humic acids of 0.57 mg/L and the percentage of Pu(III)aq accounted for 51.7% of the total aqueous Pu. This demonstrates that the humic acids were able to reduce the aqueous Pu

  5. Unconventional superconductivity in PuCoGa5.

    PubMed

    Curro, N J; Caldwell, T; Bauer, E D; Morales, L A; Graf, M J; Bang, Y; Balatsky, A V; Thompson, J D; Sarrao, J L

    2005-03-31

    In the Bardeen-Cooper-Schrieffer theory of superconductivity, electrons form (Cooper) pairs through an interaction mediated by vibrations in the underlying crystal structure. Like lattice vibrations, antiferromagnetic fluctuations can also produce an attractive interaction creating Cooper pairs, though with spin and angular momentum properties different from those of conventional superconductors. Such interactions have been implicated for two disparate classes of materials--the copper oxides and a set of Ce- and U-based compounds. But because their transition temperatures differ by nearly two orders of magnitude, this raises the question of whether a common pairing mechanism applies. PuCoGa5 has a transition temperature intermediate between those classes and therefore may bridge these extremes. Here we report measurements of the nuclear spin-lattice relaxation rate and Knight shift in PuCoGa5, which demonstrate that it is an unconventional superconductor with properties as expected for antiferromagnetically mediated superconductivity. Scaling of the relaxation rates among all of these materials (a feature not exhibited by their Knight shifts) establishes antiferromagnetic fluctuations as a likely mechanism for their unconventional superconductivity and suggests that related classes of exotic superconductors may yet be discovered.

  6. On the multi-reference nature of plutonium oxides: PuO2(2+), PuO2, PuO3 and PuO2(OH)2.

    PubMed

    Boguslawski, Katharina; Réal, Florent; Tecmer, Paweł; Duperrouzel, Corinne; Gomes, André Severo Pereira; Legeza, Örs; Ayers, Paul W; Vallet, Valérie

    2017-02-08

    Actinide-containing complexes present formidable challenges for electronic structure methods due to the large number of degenerate or quasi-degenerate electronic states arising from partially occupied 5f and 6d shells. Conventional multi-reference methods can treat active spaces that are often at the upper limit of what is required for a proper treatment of species with complex electronic structures, leaving no room for verifying their suitability. In this work we address the issue of properly defining the active spaces in such calculations, and introduce a protocol to determine optimal active spaces based on the use of the Density Matrix Renormalization Group algorithm and concepts of quantum information theory. We apply the protocol to elucidate the electronic structure and bonding mechanism of volatile plutonium oxides (PuO3 and PuO2(OH)2), species associated with nuclear safety issues for which little is known about the electronic structure and energetics. We show how, within a scalar relativistic framework, orbital-pair correlations can be used to guide the definition of optimal active spaces which provide an accurate description of static/non-dynamic electron correlation, as well as to analyse the chemical bonding beyond a simple orbital model. From this bonding analysis we are able to show that the addition of oxo- or hydroxo-groups to the plutonium dioxide species considerably changes the π-bonding mechanism with respect to the bare triatomics, resulting in bent structures with a considerable multi-reference character.

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

    PubMed

    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.

  8. PU.1 regulates both cytokine-dependent proliferation and differentiation of granulocyte/macrophage progenitors.

    PubMed Central

    DeKoter, R P; Walsh, J C; Singh, H

    1998-01-01

    PU.1 is a unique regulatory protein required for the generation of both the innate and the adaptive immune system. It functions exclusively in a cell-intrinsic manner to control the development of granulocytes, macrophages, and B and T lymphocytes. We demonstrate that mutation of the PU.1 gene causes a severe reduction in myeloid (granulocyte/macrophage) progenitors. PU.1 -/- myeloid progenitors can proliferate in vitro in response to the multilineage cytokines interleukin-3 (IL-3), IL-6 and stem cell factor but are unresponsive to the myeloid-specific cytokines granulocyte-macrophage colony-stimulating factor (GM-CSF), G-CSF and M-CSF. The failure of PU.1 -/- progenitors to respond to G-CSF is bypassed by transient signaling with IL-3. In the presence of IL-3 and G-CSF, PU.1 -/- progenitors can differentiate into granulocytic precursors containing myeloperoxidase-positive granules. Thus PU.1 is not essential for specification of granulocytic precursors, but is required for their further differentiation. The failure of PU.1 -/- progenitors to respond to M-CSF is due to lack of c-fms gene transcription. Transduction of c-fms into PU.1 -/- myeloid progenitors bypasses the block to M-CSF-dependent proliferation but does not induce detectable macrophage differentiation. Therefore, PU. 1 appears to be essential for specification of monocytic precursors. Importantly, retroviral transduction of PU.1 into mutant progenitors restores responsiveness to myeloid-specific cytokines and development of mature granulocytes and macrophages. Thus PU.1 controls myelopoiesis by regulating both proliferation and differentiation pathways. PMID:9687512

  9. Progress in the development of metallic fuel in fast reactors

    SciTech Connect

    Seidel, B.R.; Walters, L.C.

    1988-01-01

    Renewed interest has developed in metallic fuel for fast reactors as a result of Argonne National Laboratory's integral fast reactor (IFR) concept. This concept involves a novel approach to fuel-cycle closure that is based on metal reprocessing and injection-casting fabrication. This paper delves into recent developments associated with the performance of metallic fuels. In February of 1985, three full assemblies of advanced metallic fuel were placed in the core of the Experimental Breeder Reactor II (EBR-II). The 61-pin assemblies each contained an identical complement of metallic fuel of three compositions: U-10 Zr, U-8 Pu-10 Zr, and U-19 Pu-10 Zr. The pins were clad with the austenitic D9, had linear power rating of 15 kW/ft, and achieved peak cladding temperatures of 600{degree}C. The burnup achieved to date on these pins is 14 at.% burnup without any failures, and the irradiation continues. These lead assemblies have demonstrated that metallic fuels have the potential of being competitive with any existing fuel type in terms of steady-state performance.

  10. Constituent Redistribution in U-Zr Metallic Fuel Using the Advanced Fuel Performance Code BISON

    SciTech Connect

    Galloway, Jack D.; Unal, Cetin; Matthews, Christopher

    2016-09-30

    Previous work done by Galloway, et. al. on EBR-II ternary (U-Pu-Zr) fuel constituent redistribution yielded accurate simulation data for the limited data sets of Zr redistribution. The data sets included EPMA scans of two different irradiated rods. First, T179, which was irradiated to 1.9 at% burnup, was analyzed. Second, DP16, which was irradiated to 11 at% burnup, was analyzed. One set of parameters that most accurately represented the zirconium profiles for both experiments was determined. Since the binary fuel (U-Zr) has previously been used as the driver fuel for sodium fast reactors (SFR) as well as being the likely driver fuel if a new SFR is constructed, this same process has been initiated on the binary fuel form. From limited binary EPMA scans as well as other fuel characterization techniques, it has been observed that zirconium redistribution also occurs in the binary fuel, albeit at a reduced rate compared to observation in the ternary fuel, as noted by Kim et. al. While the rate of redistribution has been observed to be slower, numerous metallographs of U-Zr fuel show distinct zone formations.

  11. Activities of Pu and Am isotopes and isotopic ratios in a soil contaminated by weapons-grade plutonium.

    PubMed

    Lee, M H; Clark, S B

    2005-08-01

    An accident and fire at the former McGuire Air Force Base and Boeing Michigan Aeronautical Research Center (BOMARC) site in New Jersey resulted in dispersion of weapons-grade plutonium in particulate form to the local environment. Soil samples collected at the BOMARC site were measured for their activities and isotopic ratios of Pu and Am isotopes by radioanalytical techniques. The activities of the Pu and Am isotopes in the BOMARC soil were markedly higher than fallout levels, and they decreased nearly exponentially with increasing particle size of the soil. The measured (241)Am activity was compared to calculated values based on decay of (241)Pu. The activity ratios of (238)Pu/(239,240)Pu, (241)Pu/(239,240)Pu, and (241)Am/(239,240)Pu observed in the BOMARC soil were much lower than those attributed to nuclear reprocessing plants and Chernobyl fallout. From the activity ratios of (241)Pu/(239,240)Pu and (241)Am/(239,240)Pu, the origin of the Pu isotopes was identified as weapons-grade and the time since production of the material was estimated. Furthermore, the atomic ratio of (240)Pu/(239)Pu in the BOMARC soil was remarkably lower than the fallout value influenced by nuclear weapons testing and the Chernobyl accident. The atomic ratio of (240)Pu/(239)Pu was very close to the value of the weapons-grade Pu detected from the Thule accident in Greenland. This work demonstrates the utility of radioanalytical measurements and decay calculations for defining characteristics of the source term and discriminating multiple processes that contribute to a source. Such an approach would also be needed to respond to a terrorist event involving an improvised nuclear device or radiological dispersal device.

  12. Heterogeneous reduction of PuO₂ with Fe(II): importance of the Fe(III) reaction product.

    PubMed

    Felmy, Andrew R; Moore, Dean A; Rosso, Kevin M; Qafoku, Odeta; Rai, Dhanpat; Buck, Edgar C; Ilton, Eugene S

    2011-05-01

    Heterogeneous reduction of actinides in higher, more soluble oxidation states to lower, more insoluble oxidation states by reductants such as Fe(II) has been the subject of intensive study for more than two decades. However, Fe(II)-induced reduction of sparingly soluble Pu(IV) to the more soluble lower oxidation state Pu(III) has been much less studied, even though such reactions can potentially increase the mobility of Pu in the subsurface. Thermodynamic calculations are presented that show how differences in the free energy of various possible solid-phase Fe(III) reaction products can greatly influence aqueous Pu(III) concentrations resulting from reduction of PuO₂(am) by Fe(II). We present the first experimental evidence that reduction of PuO₂(am) to Pu(III) by Fe(II) was enhanced when the Fe(III) mineral goethite was spiked into the reaction. The effect of goethite on reduction of Pu(IV) was demonstrated by measuring the time dependence of total aqueous Pu concentration, its oxidation state, and system pe/pH. We also re-evaluated established protocols for determining Pu(III) {[Pu(III) + Pu(IV)] - Pu(IV)} by using thenoyltrifluoroacetone (TTA) in toluene extractions; the study showed that it is important to eliminate dissolved oxygen from the TTA solutions for accurate determinations. More broadly, this study highlights the importance of the Fe(III) reaction product in actinide reduction rate and extent by Fe(II).

  13. Discrimination of source reactor type by multivariate statistical analysis of uranium and plutonium isotopic concentrations in unknown irradiated nuclear fuel material.

    PubMed

    Robel, Martin; Kristo, Michael J

    2008-11-01

    The problem of identifying the provenance of unknown nuclear material in the environment by multivariate statistical analysis of its uranium and/or plutonium isotopic composition is considered. Such material can be introduced into the environment as a result of nuclear accidents, inadvertent processing losses, illegal dumping of waste, or deliberate trafficking in nuclear materials. Various combinations of reactor type and fuel composition were analyzed using Principal Components Analysis (PCA) and Partial Least Squares Discriminant Analysis (PLSDA) of the concentrations of nine U and Pu isotopes in fuel as a function of burnup. Real-world variation in the concentrations of (234)U and (236)U in the fresh (unirradiated) fuel was incorporated. The U and Pu were also analyzed separately, with results that suggest that, even after reprocessing or environmental fractionation, Pu isotopes can be used to determine both the source reactor type and the initial fuel composition with good discrimination.

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

    PubMed

    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 < 0.001); lichen and moss averaged 0.184 ± 0.007, similar to the integrated global fallout ratio, whereas kelp and mussel (soft tissue) averaged 0.226 ± 0.003. These observations provide supporting evidence that a large input of isotopically heavier 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

  15. Temporal evolution of (137)Cs, (237)Np, and (239+240)Pu and estimated vertical (239+240)Pu export in the northwestern Mediterranean Sea.

    PubMed

    Bressac, M; Levy, I; Chamizo, E; La Rosa, J J; Povinec, P P; Gastaud, J; Oregioni, B

    2017-04-03

    The evolution of (137)Cs, (237)Np and (239+240)Pu at the DYFAMED station (NW Mediterranean) is discussed in relation to physical processes, downward fluxes of particles, and changes in the main input sources. The data set presented in this study represents the first complete (237)Np vertical profiles (0.12-0.27μBqL(-1)), and constitutes a baseline measurement to assess future changes. A similar behavior of Cs and Np has been evidenced, confirming that Np behaves conservatively. While the (137)Cs decrease has been driven by its radioactive decay, the vertical distribution of (237)Np has not substantially changed over the last decade. In the absence of recent major inputs, a homogenization of their vertical distribution occurred, partly due to deep convection events that became more intense during the last decade. In contrast, (239+240)Pu surface levels in the NW Mediterranean waters have fallen in the past four decades by a factor of 5. This decrease in surface has been balanced by higher concentrations in the deep-water layers. A first estimate of the downward (239+240)Pu fluxes in the NW Mediterranean Sea is proposed over more than two decades. This estimation, based on the DYFAMED sediment trap time-series data and published (239+240)Pu flux measurements, suggests that sinking particles have accounted for 60-90% of the upper layer (0-200m) Pu inventory loss over the period 1989-2013. The upper layer residence time of Pu is estimated to be ~28years, twice as long as the residence time estimated for the whole western Mediterranean (~15years). This difference highlights the slow removal of Pu in the open waters of the NW Mediterranean and confirms that most of the Pu removal occurs along the coastal margin where sedimentation rates are high.

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

    NASA Astrophysics Data System (ADS)

    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. Pu isotopes in soils collected downwind from Lop Nor: regional fallout vs. global fallout

    NASA Astrophysics Data System (ADS)

    Bu, Wenting; Ni, Youyi; Guo, Qiuju; Zheng, Jian; Uchida, Shigeo

    2015-07-01

    For the first time, soil core samples from the Jiuquan region have been analyzed for Pu isotopes for radioactive source identification and radiological assessment. The Jiuquan region is in downwind from the Lop Nor Chinese nuclear test (CNT) site. The high Pu inventories (13 to 546 Bq/m2) in most of the sampling locations revealed that this region was heterogeneously contaminated by the regional fallout Pu from the CNTs. The contributions of the CNTs to the total Pu in soils were estimated to be more than 40% in most cases. The 240Pu/239Pu atom ratios in the soils ranged from 0.059 to 0.186 with an inventory-weighted average of 0.158, slightly lower than that of global fallout. This atom ratio could be considered as a mixed fingerprint of Pu from the CNTs. In addition, Pu in soils of Jiuquan region had a faster downward migration rate compared with other investigated places in China.

  18. Pu isotopes in soils collected downwind from Lop Nor: regional fallout vs. global fallout.

    PubMed

    Bu, Wenting; Ni, Youyi; Guo, Qiuju; Zheng, Jian; Uchida, Shigeo

    2015-07-17

    For the first time, soil core samples from the Jiuquan region have been analyzed for Pu isotopes for radioactive source identification and radiological assessment. The Jiuquan region is in downwind from the Lop Nor Chinese nuclear test (CNT) site. The high Pu inventories (13 to 546 Bq/m(2)) in most of the sampling locations revealed that this region was heterogeneously contaminated by the regional fallout Pu from the CNTs. The contributions of the CNTs to the total Pu in soils were estimated to be more than 40% in most cases. The (240)Pu/(239)Pu atom ratios in the soils ranged from 0.059 to 0.186 with an inventory-weighted average of 0.158, slightly lower than that of global fallout. This atom ratio could be considered as a mixed fingerprint of Pu from the CNTs. In addition, Pu in soils of Jiuquan region had a faster downward migration rate compared with other investigated places in China.

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

    SciTech Connect

    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.

  20. Pu isotopes in soils collected downwind from Lop Nor: regional fallout vs. global fallout

    PubMed Central

    Bu, Wenting; Ni, Youyi; Guo, Qiuju; Zheng, Jian; Uchida, Shigeo

    2015-01-01

    For the first time, soil core samples from the Jiuquan region have been analyzed for Pu isotopes for radioactive source identification and radiological assessment. The Jiuquan region is in downwind from the Lop Nor Chinese nuclear test (CNT) site. The high Pu inventories (13 to 546 Bq/m2) in most of the sampling locations revealed that this region was heterogeneously contaminated by the regional fallout Pu from the CNTs. The contributions of the CNTs to the total Pu in soils were estimated to be more than 40% in most cases. The 240Pu/239Pu atom ratios in the soils ranged from 0.059 to 0.186 with an inventory-weighted average of 0.158, slightly lower than that of global fallout. This atom ratio could be considered as a mixed fingerprint of Pu from the CNTs. In addition, Pu in soils of Jiuquan region had a faster downward migration rate compared with other investigated places in China. PMID:26184740

  1. Essential role of Jun family transcription factors in PU.1 knockdown-induced leukemic stem cells.

    PubMed

    Steidl, Ulrich; Rosenbauer, Frank; Verhaak, Roel G W; Gu, Xuesong; Ebralidze, Alexander; Otu, Hasan H; Klippel, Steffen; Steidl, Christian; Bruns, Ingmar; Costa, Daniel B; Wagner, Katharina; Aivado, Manuel; Kobbe, Guido; Valk, Peter J M; Passegué, Emmanuelle; Libermann, Towia A; Delwel, Ruud; Tenen, Daniel G

    2006-11-01

    Knockdown of the transcription factor PU.1 (encoded by Sfpi1) leads to acute myeloid leukemia (AML) in mice. We examined the transcriptome of preleukemic hematopoietic stem cells (HSCs) in which PU.1 was knocked down (referred to as 'PU.1-knockdown HSCs') to identify transcriptional changes preceding malignant transformation. Transcription factors c-Jun and JunB were among the top-downregulated targets. Restoration of c-Jun expression in preleukemic cells rescued the PU.1 knockdown-initiated myelomonocytic differentiation block. Lentiviral restoration of JunB at the leukemic stage led to loss of leukemic self-renewal capacity and prevented leukemia in NOD-SCID mice into which leukemic PU.1-knockdown cells were transplanted. Examination of human individuals with AML confirmed the correlation between PU.1 and JunB downregulation. These results delineate a transcriptional pattern that precedes leukemic transformation in PU.1-knockdown HSCs and demonstrate that decreased levels of c-Jun and JunB contribute to the development of PU.1 knockdown-induced AML by blocking differentiation and increasing self-renewal. Therefore, examination of disturbed gene expression in HSCs can identify genes whose dysregulation is essential for leukemic stem cell function and that are targets for therapeutic interventions.

  2. Highly accurate measurements of the spontaneous fission half-life of 240,242Pu

    NASA Astrophysics Data System (ADS)

    Salvador-Castiñeira, P.; Bryś, T.; Eykens, R.; Hambsch, F.-J.; Moens, A.; Oberstedt, S.; Sibbens, G.; Vanleeuw, D.; Vidali, M.; Pretel, C.

    2013-12-01

    Fast spectrum neutron-induced fission cross-section data for transuranic isotopes are of special demand from the nuclear data community. In particular highly accurate data are needed for the new generation IV nuclear applications. The aim is to obtain precise neutron-induced fission cross sections for 240Pu and 242Pu. To do so, accurate data on spontaneous fission half-lives must be available. Also, minimizing uncertainties in the detector efficiency is a key point. We studied both isotopes by means of a twin Frisch-grid ionization chamber with the goal of improving the present data on the neutron-induced fission cross section. For the two plutonium isotopes the high α-particle decay rates pose a particular problem to experiments due to piling-up events in the counting gas. Argon methane and methane were employed as counting gases, the latter showed considerable improvement in signal generation due to its higher drift velocity. The detection efficiency for both samples was determined, and improved spontaneous fission half-lives were obtained with very low statistical uncertainty (0.13% for 240Pu and 0.04% for 242Pu): for 240Pu, T1/2,SF=1.165×1011 yr (1.1%), and for 242Pu, T1/2,SF=6.74×1010 yr (1.3%). Systematic uncertainties are due to sample mass (0.4% for 240Pu and 0.9% for 242Pu) and efficiency (1%).

  3. Determination of /sup 239,240/Pu in bottom sediments of the Baltic Sea

    SciTech Connect

    Kuznetsov, Yu.V.; Legin, V.K.; Pospelov, Yu.N.; Simonyak, Z.N.

    1988-11-01

    We present a technique for determining the /sup 239,240/Pu content, using /sup 236/Pu as the monitor of chemical yield, in samples of soils and bottom sediments - objects of the external environment. Plutonium is extracted from the matrix material by leaching with a mixture of concentrated acids HCl-HNO/sub 3/, after which it is separated by ion-exchange methods. After electrodeposition onto stainless steel discs the activity of the nuclides of plutonium is measured by the method of alpha-spectrometry. The average chemical yields during the analysis of the samples was 40-60%, the relative standard deviation was 10%, and the lower limit of detectability was 0.3 Bq. We present results of the determination of the /sup 239,240/Pu content in surface samples of bottom sediments from the Gulf of Finland and that past of the Baltic Sea which adjoins the territory of the USSR. It is found that the unit activity of /sup 239,240/Pu in the bottom sediments varies within the limits of 0.4-1.2 Bq/kg and lies at the global level. Global genesis of /sup 239,240/Pu in the bottom sediments of the Gulf of Finland and the open parts of the Baltic Sea is also confirmed by the values which are found for the ratios /sup 238/Pu//sup 239,240/Pu and /sup 239,240/Pu//sup 137/Cs.

  4. /sup 238/Pu fuel form processes. Quarterly report, April-June 1981

    SciTech Connect

    Folger, R.L.

    1981-12-01

    An analytical program has been started to determine the cause of cracking in DOP-26 iridium alloy during welding of GPHS clad vent sets. Analyses revealed that (1) intergranular cracking in the interior weld bead occurs in the heat-affected zone adjacent to the arc quench taper and at weld edges, (2) grain surfaces exposed by cracking exhibit a characteristic ridge network topography, and (3) no elements that could cause hot shortness were detected in the ridge networks.

  5. Electrolysis cell for reprocessing plutonium reactor fuel

    DOEpatents

    Miller, William E.; Steindler, Martin J.; Burris, Leslie

    1986-01-01

    An electrolytic cell for refining a mixture of metals including spent fuel containing U and Pu contaminated with other metals, the cell including a metallic pot containing a metallic pool as one anode at a lower level, a fused salt as the electrolyte at an intermediate level and a cathode and an anode basket in spaced-apart positions in the electrolyte with the cathode and anode being retractable to positions above the electrolyte during which spent fuel may be added to the anode basket and the anode basket being extendable into the lower pool to dissolve at least some metallic contaminants, the anode basket containing the spent fuel acting as a second anode when in the electrolyte.

  6. Electrolysis cell for reprocessing plutonium reactor fuel

    DOEpatents

    Miller, W.E.; Steindler, M.J.; Burris, L.

    1985-01-04

    An electrolytic cell for refining a mixture of metals including spent fuel containing U and Pu contaminated with other metals is claimed. The cell includes a metallic pot containing a metallic pool as one anode at a lower level, a fused salt as the electrolyte at an intermediate level and a cathode and an anode basket in spaced-apart positions in the electrolyte with the cathode and anode being retractable to positions above the electrolyte during which spent fuel may be added to the anode basket. The anode basket is extendable into the lower pool to dissolve at least some metallic contaminants; the anode basket contains the spent fuel acting as a second anode when in the electrolyte.

  7. Proliferation Resistance Evaluation of ACR-1000 Fuel with Minor Actinides

    SciTech Connect

    Gray S. Chang

    2008-09-01

    The Global Nuclear Energy Partnership (GNEP) program is to significantly advance the science and technology of nuclear energy systems and to enhance the spent fuel proliferation resistance. It consists of both innovative nuclear reactors and innovative research in separation and transmutation. The merits of nuclear energy are high-density energy, with low environmental impacts (i.e. almost zero greenhouse gas emission). Planned efforts involve near-term and intermediate-term improvements in fuel utilization and recycling in current light water reactors (LWRs) as well as the longer-term development of new nuclear energy systems that offer much improved fuel utilization and proliferation resistance, along with continued advances in operational safety. For future advanced nuclear systems, minor actinides (MA) are viewed more as a resource to be recycled, and transmuted to less hazardous and possibly more useful forms, rather than simply disposed of as a waste stream in an expensive repository facility. MAs can play a much larger part in the design of advanced systems and fuel cycles, not only as additional sources of useful energy, but also as direct contributors to the reactivity control of the systems into which they are incorporated. In this work, an Advanced CANDU Reactor (ACR) fuel unit lattice cell model with 43 UO2 fuel rods will be used to investigate the effectiveness of a Minor Actinide Reduction Approach (MARA) for enhancing proliferation resistance and improving the fuel cycle performance. The main MARA objective is to increase the 238Pu / Pu isotope ratio by using the transuranic nuclides (237Np and 241Am) in the high burnup fuel and thereby increase the proliferation resistance even for a very low fuel burnup. As a result, MARA is a very effective approach to enhance the proliferation resistance for the on power refueling ACR system nuclear fuel. The MA transmutation characteristics at different MA loadings were compared and their impact on neutronics

  8. Comparative skeletal distribution of Am and Pu in man, monkey, and baboon

    SciTech Connect

    Lynch, T.P.; Kathren, R.L.; Dagle, G.E.; McInroy, J.F. )

    1989-01-01

    The skeletal distribution of Am and Pu in four human cases was compared with the skeletal distributions of these radioelements in baboons and monkeys. Excellent agreement was noted among the four human cases; data were available for Am in all four and Pu in three. A statistically significant correlation was found between the {sup 241}Am and {sup 239}Pu + {sup 240}Pu skeletal distributions in the humans and those in nonhuman primates. Trabecular bone had the highest concentrations of {sup 241}Am and {sup 239+240}Pu in humans, baboons, and monkeys. Scaling factors are proposed to convert the percentages of skeletal activity in animal bones to the corresponding percentages in the bones of the human skeleton.

  9. Characterization of pu-erh tea using chemical and metabolic profiling approaches.

    PubMed

    Xie, Guoxiang; Ye, Mao; Wang, Yungang; Ni, Yan; Su, Mingming; Huang, Hua; Qiu, Mingfeng; Zhao, Aihua; Zheng, Xiaojiao; Chen, Tianlu; Jia, Wei

    2009-04-22

    In this study, the chemical constituents of pu-erh tea, black tea, and green tea, as well as those of pu-erh tea products of different ages, were analyzed and compared using a chemical profiling approach. Differences in tea processing resulted in differences in the chemical constituents and the color of tea infusions. Human biological responses to pu-erh tea ingestion were also studied by using ultraperformance liquid chromatography-quadrupole time-of-flight mass spectrometry (UPLC-QTOFMS) in conjunction with multivariate statistical techniques. Metabolic alterations during and after pu-erh tea ingestion were characterized by increased urinary excretion of 5-hydroxytryptophan, inositol, and 4-methoxyphenylacetic acid, along with reduced excretion of 3-chlorotyrosine and creatinine. This study highlights the potential for metabonomic technology to assess nutritional interventions and is an important step toward a full understanding of pu-erh tea and its influence on human metabolism.

  10. Induction of the autophagy-associated gene MAP1S via PU.1 supports APL differentiation.

    PubMed

    Haimovici, Aladin; Brigger, Daniel; Torbett, Bruce E; Fey, Martin F; Tschan, Mario P

    2014-09-01

    The PU.1 transcription factor is essential for myeloid development. We investigated if the microtubule-associated protein 1S (MAP1S) is a novel PU.1 target with a link to autophagy, a cellular recycling pathway. Comparable to PU.1, MAP1S expression was significantly repressed in primary AML blasts as compared to mature neutrophils. Accordingly, MAP1S expression was induced during neutrophil differentiation of CD34(+) progenitor and APL cells. Moreover, PU.1 bound to the MAP1S promoter and induced MAP1S expression during APL differentiation. Inhibiting MAP1S resulted in aberrant neutrophil differentiation and autophagy. Taken together, our findings implicate the PU.1-regulated MAP1S gene in neutrophil differentiation and autophagy control.

  11. The Pu-U-Am system: An ab initio informed CALPHAD thermodynamic study

    NASA Astrophysics Data System (ADS)

    Perron, A.; Turchi, P. E. A.; Landa, A.; Söderlind, P.; Ravat, B.; Oudot, B.; Delaunay, F.

    2015-03-01

    Phase diagram and thermodynamic properties of the Am-U system, that are experimentally unknown, are calculated using the CALPHAD method with input from ab initio electronic-structure calculations for the fcc and bcc phases. A strong tendency toward phase separation across the whole composition range is predicted. In addition, ab initio informed Pu-U and Am-Pu thermodynamic assessments are combined to build a Pu-U-Am thermodynamic database. Regarding the Pu-rich corner of the ternary system, predictions indicate that Am acts as a powerful δ-Pu (fcc) stabilizer. In the U-rich corner, similar predictions are made but to a lesser extent. In both cases, the bcc phase is destabilized and the fcc phase is enhanced. Finally, results and methodology are discussed and compared with previous assessments and guidelines are provided for further experimental studies.

  12. U.S.-Russian experts NATO collaborative research grant exchange visit meeting on excess Pu ceramics formulations and characterizations

    SciTech Connect

    Jardine, L.J., LLNL

    1998-11-24

    This document contains the agenda and meeting notes. Topics of discussion included US Pu disposition ceramics activities, Russian experience and proposals in Pu ceramics, and development of possible Russian ceramic proposals or collaborations.

  13. Preparation and characterization of {sup 238}Pu-ceramics for radiation damage experiments

    SciTech Connect

    DM Strachan; RD Scheele; WC Buchmiller; JD Vienna; RL Sell; RJ Elovich

    2000-06-15

    As a result of treaty agreements between Russia and the US, portions of their respective plutonium and nuclear weapons stockpiles have been declared excess. In support of the US Department of Energy's 1998 decision to pursue immobilization of a portion of the remaining Pu in a titanate-based ceramic, the authors prepared nearly 200 radiation-damage test specimens of five Pu- and {sup 238}Pu-ceramics containing 10 mass% Pu to determine the effects of irradiation from the contained Pu and U on the ceramic. The five Pu-ceramics were (1) phase-pure pyrochlore [ideally, Ca(U, Pu)Ti{sub 2}O{sub 7}], (2) pyrochlore-rich baseline, (3) pyrochlore-rich baseline with impurities, (4) phase-pure zirconolite [ideally Ca(U, Pu)Ti{sub 2}O{sub 7}], and (5) a zirconolite-rich baseline. These ceramics were prepared with either normal weapons-grade Pu, which is predominantly {sup 239}Pu, or {sup 238}Pu. The {sup 238}Pu accelerates the radiation damage relative to the {sup 239}Pu because of its much higher specific activity. The authors were unsuccessful in preparing phase-pure (Pu, U) brannerite, which is the third crystalline phase present in the baseline immobilization form. Since these materials will contain {approximately}10 mass% Pu and about 20 mass% U, radiation damage to the crystalline structure of these materials will occur overtime. As the material becomes damaged from the decay of the Pu and U, it is possible for the material to swell as both the alpha particles and recoiling atoms rupture chemical bonds within the solid. As the material changes density, cracking, perhaps in the form of microcracks, may occur. If cracking occurs in ceramic that has been placed in a repository, the calculated rate of radionuclide release if the can has corroded would increase proportionately to the increase in surface area. To investigate the effects of radiation damage on the five ceramics prepared, the authors are storing the specimens at 20, 125, and 250 C until the {sup 238}Pu specimens

  14. Synthetic Fuel

    ScienceCinema

    Idaho National Laboratory - Steve Herring, Jim O'Brien, Carl Stoots

    2016-07-12

    Two global energy priorities today are finding environmentally friendly alternatives to fossil fuels, and reducing greenhouse gass Two global energy priorities today are finding environmentally friendly alternatives to fossil fuels, and reducing greenhous

  15. Synthetic Fuel

    SciTech Connect

    Idaho National Laboratory - Steve Herring, Jim O'Brien, Carl Stoots

    2008-03-26

    Two global energy priorities today are finding environmentally friendly alternatives to fossil fuels, and reducing greenhouse gass Two global energy priorities today are finding environmentally friendly alternatives to fossil fuels, and reducing greenhous

  16. Fuel cells

    NASA Astrophysics Data System (ADS)

    1984-12-01

    The US Department of Energy (DOE), Office of Fossil Energy, has supported and managed a fuel cell research and development (R and D) program since 1976. Responsibility for implementing DOE's fuel cell program, which includes activities related to both fuel cells and fuel cell systems, has been assigned to the Morgantown Energy Technology Center (METC) in Morgantown, West Virginia. The total United States effort of the private and public sectors in developing fuel cell technology is referred to as the National Fuel Cell Program (NFCP). The goal of the NFCP is to develop fuel cell power plants for base-load and dispersed electric utility systems, industrial cogeneration, and on-site applications. To achieve this goal, the fuel cell developers, electric and gas utilities, research institutes, and Government agencies are working together. Four organized groups are coordinating the diversified activities of the NFCP. The status of the overall program is reviewed in detail.

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

    PubMed

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

    2004-01-01

    The activity concentrations of (237)Np and the two Pu isotopes, (239)Pu and (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 (238)Pu/(239+240)Pu and (134)Cs/(137)Cs measured previously were also included in this study for comparison. The (237)Np activity concentration ranged from 0.08 +/- 0.01 to 2.08 +/- 0.17 MBq kg(-1), depending on the location of the sampling site and time of collection. The (239+240)Pu activity concentration ranged from 0.09 +/- 0.01 to 4.09 +/- 0.15 Bq kg(-1), with the (240)Pu/(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 (237)Np/(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 degrees N, 12.38 degrees 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.

  18. Direct high-resolution alpha spectrometry from nuclear fuel particles in an outdoor air sample.

    PubMed

    Pöllänen, R; Siiskonen, T

    2008-01-01

    The potential use of direct high-resolution alpha spectrometry to identify the presence of transactinium elements in air samples is illustrated in the case when alpha-particle-emitting radionuclides are incorporated in nuclear fuel particles. Alpha particle energy spectra are generated through Monte Carlo simulations assuming a nuclide composition similar to RBMK (Chernobyl) nuclear fuel. The major alpha-particle-emitting radionuclides, in terms of activity, are 242Cm, 239Pu and 240Pu. The characteristics of the alpha peaks are determined by fuel particle properties as well as the type of the air filter. It is shown that direct alpha spectrometry can be readily applied to membrane filter samples containing nuclear fuel particles when rapid nuclide identification is of relevance. However, the development of a novel spectrum analysis code is a prerequisite for unfolding complex alpha spectra.

  19. Lead Slowing Down Spectrometry Analysis of Data from Measurements on Nuclear Fuel

    SciTech Connect

    Warren, Glen A.; Anderson, Kevin K.; Kulisek, Jonathan A.; Danon, Yaron; Weltz, Adam; Gavron, Victor A.; Harris, Jason; Stewart, Trevor N.

    2015-01-12

    Improved non-destructive assay of isotopic masses in used nuclear fuel would be valuable for nuclear safeguards operations associated with the transport, storage and reprocessing of used nuclear fuel. Our collaboration is examining the feasibility of using lead slowing down spectrometry techniques to assay the isotopic fissile masses in used nuclear fuel assemblies. We present the application of our analysis algorithms on measurements conducted with a lead spectrometer. The measurements involved a single fresh fuel pin and discrete 239Pu and 235U samples. We are able to describe the isotopic fissile masses with root mean square errors over seven different configurations to 6.35% for 239Pu and 2.7% for 235U over seven different configurations. Funding Source(s):

  20. Isotopic Details of the Spent Catawba-1 MOX Fuel Rods at ORNL

    SciTech Connect

    Ellis, Ronald James

    2015-04-01

    The United States Department of Energy funded Shaw/AREVA MOX Services LLC to fabricate four MOX Lead Test Assemblies (LTA) from weapons-grade plutonium. A total of four MOX LTAs (including MX03) were irradiated in the Catawba Nuclear Station (Unit 1) Catawba-1 PWR which operated at a total thermal power of 3411 MWt and had a core with 193 total fuel assemblies. The MOX LTAs were irradiated along with Duke Energy s irradiation of eight Westinghouse Next Generation Fuel (NGF) LEU LTAs (ref.1) and the remaining 181 LEU fuel assemblies. The MX03 LTA was irradiated in the Catawba-1 PWR core (refs.2,3) during cycles C-16 and C-17. C-16 began on June 5, 2005, and ended on November 11, 2006, after 499 effective full power days (EFPDs). C-17 started on December 29, 2006, (after a shutdown of 48 days) and continued for 485 EFPDs. The MX03 and three other MOX LTAs (and other fuel assemblies) were discharged at the end of C-17 on May 3, 2008. The design of the MOX LTAs was based on the (Framatome ANP, Inc.) Mark-BW/MOX1 17 17 fuel assembly design (refs. 4,5,6) for use in Westinghouse PWRs, but with MOX fuel rods with three Pu loading ranges: the nominal Pu loadings are 4.94 wt%, 3.30 wt%, and 2.40 wt%, respectively, for high, medium, and low Pu content. The Mark-BW/MOX1 (MOX LTA) fuel assembly design is the same as the Advanced Mark-BW fuel assembly design but with the LEU fuel rods replaced by MOX fuel rods (ref. 5). The fabrication of the fuel pellets and fuel rods for the MOX LTAs was performed at the Cadarache facility in France, with the fabrication of the LTAs performed at the MELOX facility, also in France.

  1. Future Fuels

    DTIC Science & Technology

    2005-10-04

    tactical ground mobility and increasing operational reach • Identify, review, and assess – Technologies for reducing fuel consumption, including...T I O N S A C T I O N S TOR Focus - Tactical ground mobility - Operational reach - Not A/C, Ships, or troops Hybrid Electric Vehicle Fuel Management...Fuel Management During Combat Operations Energy Fundamentals • Energy Density • Tactical Mobility • Petroleum Use • Fuel Usage (TWV) • TWV OP TEMPO TOR

  2. The FUTURIX-FTA experiment in Phenix: status of oxides fuels fabrication

    SciTech Connect

    Jorion, F.; Donnet, L.

    2007-07-01

    Eliminating long-lived radionuclides by transmuting them into nonradioactive or short-lived nuclei is a reference approach in nuclear waste management. FUTURIX/FTA (FUels for Transmutation of transuranium elements in Phenix / Fortes Teneurs en Actinides [high actinide content]) is an international program intended to demonstrate the technical feasibility, primarily with regard to fuel behavior, of transmuting minor actinides in fast neutron reactors. This research is carried out in collaboration with the US Department of Energy (DOE), the Japan Atomic Energy Research Institute (JAERI), the Institute for Transuranium Elements (ITU) in Germany, and the Commissariat a l'Energie Atomique (CEA) in France. In this context, the CEA investigated four ceramic/ceramic (cercer) compositions ((Pu{sub 0.5}Am{sub 0.5})O{sub 2-x} + 80 vol% MgO), (Pu{sub 0.5}Am{sub 0.5})O{sub 2-x} + 70 vol% MgO), (Pu{sub 0.2}Am{sub 0.8})O{sub 2-x} + 75 vol% MgO), (Pu{sub 0.2}Am{sub 0.8})O{sub 2-x} + 65 vol% MgO) and fabricated two fuel pins. The mixed actinide oxides were synthesized by oxalate co-conversion and incorporated into a magnesia matrix by classical powder metallurgy. The resulting fuel pellets were subjected to chemical, dimensional, structural and microstructural characterization. The results for each composition were interpreted and compared. (authors)

  3. Pyroprocess for processing spent nuclear fuel

    DOEpatents

    Miller, William E.; Tomczuk, Zygmunt

    2002-01-01

    This is a pyroprocess for processing spent nuclear fuel. The spent nuclear fuel is chopped into pieces and placed in a basket which is lowered in to a liquid salt solution. The salt is rich in ZrF.sub.4 and containing alkali or alkaline earth fluorides, and in particular, the salt chosen was LiF-50 mol % ZrF.sub.4 with a eutectic melting point of 500.degree. C. Prior to lowering the basket, the salt is heated to a temperature of between 550.degree. C. and 700.degree. C. in order to obtain a molten solution. After dissolution the oxides of U, Th, rare earth and other like oxides, the salt bath solution is subject to hydro-fluorination to remove the oxygen and then to a fluorination step to remove U as gaseous UF.sub.6. In addition, after dissolution, the basket contains PuO.sub.2 and undissolved parts of the fuel rods, and the basket and its contents are processed to remove the Pu.

  4. 137Cs, 239+240Pu and 240Pu/239Pu atom ratios in the surface waters of the western North Pacific Ocean, eastern Indian Ocean and their adjacent seas.

    PubMed

    Yamada, Masatoshi; Zheng, Jian; Wang, Zhong-Liang

    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 (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 (137)Cs activities showed a wide variation with values ranging from 1.1 Bq m(-3) in the Antarctic Circumpolar Region of the Southern Ocean to 3 Bq m(-3) in the western North Pacific Ocean and the South China Sea. The latitudinal distributions of (137)Cs activity were not reflective of that of the integrated deposition density of atmospheric global fallout. The removal rates of (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 (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(-1) in the Sulu and Indonesian Seas, 0.033 yr(-1) in the Bay of Bengal and Andaman Sea, and 0.029 yr(-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. (239+240)Pu activities and (240)Pu/(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 (240)Pu/(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 the two end-member mixing model. The higher (240)Pu/(239)Pu

  5. Gamma-ray Output Spectra from 239 Pu Fission

    DOE PAGES

    Ullmann, John

    2015-05-25

    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-raymore » 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.« less

  6. Electronic structure of nitrides PuN and UN

    NASA Astrophysics Data System (ADS)

    Lukoyanov, A. V.; Anisimov, V. I.

    2016-11-01

    The electronic structure of uranium and plutonium nitrides in ambient conditions and under pressure is investigated using the LDA + U + SO band method taking into account the spin-orbit coupling and the strong correlations of 5 f electrons of actinoid ions. The parameters of these interactions for the equilibrium cubic structure are calculated additionally. The application of pressure reduces the magnetic moment in PuN due to predominance of the f 6 configuration and the jj-type coupling. An increase in the occupancy of the 5 f state in UN leads to a decrease in the magnetic moment, which is also detected in the trigonal structure of the UN x β phase (La2O3-type structure). The theoretical results are in good agreement with the available experimental data.

  7. Developing the Pulsed Fission-Fusion (PuFF) Engine

    NASA Technical Reports Server (NTRS)

    Adams, Robert B.; Cassibry, Jason; Bradley, David; Fabisinski, Leo; Statham, Geoffrey

    2014-01-01

    In September 2013 the NASA Innovative Advanced Concept (NIAC) organization awarded a phase I contract to the PuFF team. Our phase 1 proposal researched a pulsed fission-fusion propulsion system that compressed a target of deuterium (D) and tritium (T) as a mixture in a column, surrounded concentrically by Uranium. The target is surrounded by liquid lithium. A high power current would flow down the liquid lithium and the resulting Lorentz force would compress the column by roughly a factor of 10. The compressed column would reach criticality and a combination of fission and fusion reactions would occur. Our Phase I results, summarized herein, review our estimates of engine and vehicle performance, our work to date to model the fission-fusion reaction, and our initial efforts in experimental analysis.

  8. Fossil Fuels.

    ERIC Educational Resources Information Center

    Crank, Ron

    This instructional unit is one of 10 developed by students on various energy-related areas that deals specifically with fossil fuels. Some topics covered are historic facts, development of fuels, history of oil production, current and future trends of the oil industry, refining fossil fuels, and environmental problems. Material in each unit may…

  9. Chronic cigarette smoke exposure increases the pulmonary retention and radiation dose of {sup 239}Pu inhaled as {sup 239}PuO{sub 2} by F344 rats

    SciTech Connect

    Finch, G.L.; Lundgren, D.L.; Barr, E.B.; Chen, B.T.; Griffith, W.C.; Hobbs, C.H.; Hoover, M.D.; Nikula, K.J.; Mauderly, J.L.

    1998-12-01

    As a portion of a study to examine how chronic cigarette smoke exposure might alter the risk of lung tumors from inhaled {sup 239}PuO{sub 2} in rats, the effects of smoke exposure on alpha-particle lung dosimetry over the life-span of exposed rats were determined. Male and female rats were exposed to inhaled {sup 239}PuO{sub 2} alone or in combination with cigarette smoke. Animals exposed to filtered air along served as controls for the smoke exposure. Whole-body exposure to mainstream smoke diluted to concentrations of either 100 or 250 mg total particulate matter m{sup {minus}3} began at 6 wk of age and continued for 6 h d{sup {minus}1}, 5 d wk{sup {minus}1}, for 30 mo. A single, pernasal, acute exposure to {sup 239}PuO{sub 2} was given to all rats at 12 wk of age. Exposure to cigarette smoke caused decreased body weight gains in a concentration dependent manner. Lung-to-body weight ratios were increased in smoke-exposed rats. Rats exposed to cigarette smoke before the {sup 239}PuO{sub 2} exposure deposited less {sup 239}Pu in the lung than did controls. Except for male rats exposed to LCS, exposure to smoke retarded the clearance of {sup 239}Pu from the lung compared to control rats through study termination at 870 d after {sup 239}PuO{sub 2} exposure. Radiation doses to lungs were calculated by sex and by exposure group for rats on study for at least 360 d using modeled body weight changes, lung-to-body weight ratios, and standard dosimetric calculations. For both sexes, estimated lifetime radiation doses from the time of {sup 239}PuO{sub 2} exposure to death were 3.8 Gy, 4.4 Gy, or 6.7 Gy for the control, LCS, or HCS exposure groups, respectively. Assuming an approximately linear dose-response relationship between radiation dose and lung neoplasm incidence, approximate increases of 20% or 80% in tumor incidence over controls would be expected in rats exposed to {sup 239}PuO{sub 2} and LCS or {sup 239}PuO{sub 2} and HCS, respectively.

  10. Consistent Data Assimilation of Isotopes: 242Pu and 105Pd

    SciTech Connect

    G. Palmiotti; H. Hiruta; M. Salvatores

    2012-09-01

    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 are analyzed using the EMPIRE evaluated files for 242Pu and 105Pd. In particular irradiation experiments (PROFIL-1 and -2, TRAPU-1, -2 and -3) provide information about capture cross sections, and a critical configuration, COSMO, where fission spectral indexes were measured, provides information about fission cross section. The observed discrepancies between calculated and experimental results are used in conjunction with the computed sensitivity coefficients and covariance matrix for nuclear parameters in a consistent data assimilation. The results obtained by the consistent data assimilation indicate that not so large modifications on some key identified nuclear parameters allow to obtain reasonable C/E. However, for some parameters such variations are outside the range of 1 s of their initial standard deviation. This can indicate a possible conflict between differential measurements (used to calculate the initial standard deviations) and the integral measurements used in the statistical data adjustment. Moreover, an inconsistency between the C/E of two sets of irradiation experiments (PROFIL and TRAPU) is observed for 242Pu. This is the end of this project funded by the Nuclear Physics Program of the DOE Office of Science. We can indicate that a proof of principle has been demonstrated for a few isotopes for this innovative methodology. However, we are still far from having explored all the possibilities and made this methodology to be considered proved and robust. In particular many issues are worth further investigation: • Non-linear effects • Flexibility of nuclear parameters in describing cross sections • Multi-isotope consistent assimilation • Consistency between differential and integral

  11. IFR fuel cycle process equipment design environment and objectives

    SciTech Connect

    Rigg, R.H.

    1993-03-01

    Argonne National laboratory (ANL) is refurbishing the hot cell facility originally constructed with the EBR-II reactor. When refurbishment is complete, the facility win demonstrate the complete fuel cycle for current generation high burnup metallic fuel elements. These are sodium bonded, stainless steel clad fuel pins of U-Zr or U-Pu-Zr composition typical of the fuel type proposed for a future Integral Fast Reactor (IFR) design. To the extent possible, the process equipment is being built at full commercial scale, and the facility is being modified to incorporate current DOE facility design requirements and modem remote maintenance principles. The current regulatory and safety environment has affected the design of the fuel fabrication equipment, most of which will be described in greater detail in subsequent papers in this session.

  12. IFR fuel cycle process equipment design environment and objectives

    SciTech Connect

    Rigg, R.H.

    1993-01-01

    Argonne National laboratory (ANL) is refurbishing the hot cell facility originally constructed with the EBR-II reactor. When refurbishment is complete, the facility win demonstrate the complete fuel cycle for current generation high burnup metallic fuel elements. These are sodium bonded, stainless steel clad fuel pins of U-Zr or U-Pu-Zr composition typical of the fuel type proposed for a future Integral Fast Reactor (IFR) design. To the extent possible, the process equipment is being built at full commercial scale, and the facility is being modified to incorporate current DOE facility design requirements and modem remote maintenance principles. The current regulatory and safety environment has affected the design of the fuel fabrication equipment, most of which will be described in greater detail in subsequent papers in this session.

  13. Modelling the thermal conductivity of (UxTh1-x)O2 and (UxPu1-x)O2

    SciTech Connect

    Cooper, M. W. D.; Middleburgh, S. C.; Grimes, R. W.

    2015-07-15

    The degradation of thermal conductivity due to the non-uniform cation lattice of (UxTh1-x)O2 and (UxPu1-x)O2 solid solutions has been investigated by molecular dynamics, using the non-equilibrium method, from 300 to 2000 K. Degradation of thermal conductivity is predicted in (UxTh1-x)O2 and (UxPu1-x)O2 as compositions deviate from the pure end members: UO2, PuO2 and ThO2. The reduction in thermal conductivity is most apparent at low temperatures where phonon-defect scattering dominates over phonon-phonon interactions. The effect is greater for (UxTh1-x)O2 than UxPu1-x)O2 due to the greater mismatch in cation size. Parameters for an analytical expressions have been developed that describe the predicted thermal conductivities over the full temperature and compositional ranges. Finally, these expressions may be used in higher level fuel performance codes.

  14. Assessment of Startup Fuel Options for the GNEP Advanced Burner Reactor (ABR)

    SciTech Connect

    Jon Carmack; Kemal O. Pasamehmetoglu; David Alberstein

    2008-02-01

    The Global Nuclear Energy Program (GNEP) includes a program element for the development and construction of an advanced sodium cooled fast reactor to demonstrate the burning (transmutation) of significant quantities of minor actinides obtained from a separations process and fabricated into a transuranic bearing fuel assembly. To demonstrate and qualify transuranic (TRU) fuel in a fast reactor, an Advanced Burner Reactor (ABR) prototype is needed. The ABR would necessarily be started up using conventional metal alloy or oxide (U or U, Pu) fuel. Startup fuel is needed for the ABR for the first 2 to 4 core loads of fuel in the ABR. Following start up, a series of advanced TRU bearing fuel assemblies will be irradiated in qualification lead test assemblies in the ABR. There are multiple options for this startup fuel. This report provides a description of the possible startup fuel options as well as possible fabrication alternatives available to the program in the current domestic and international facilities and infrastructure.

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

    PubMed

    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.

  16. Experience in PWR and BWR mixed-oxide fuel management

    SciTech Connect

    Schlosser, G.J.; Krebs, W.; Urban, P. )

    1993-04-01

    Germany has adopted the strategy of a closed fuel cycle using reprocessing and recycling. The central issue today is plutonium recycling by the use of U-Pu mixed oxide (MOX) in pressurized water reactors (PWRs) and boiling water reactors (BWRs). The design of MOX fuel assemblies and fuel management in MOX-containing cores are strongly influenced by the nuclear properties of the plutonium isotopes. Optimized MOX fuel assembly designs for PWRs currently use up to three types of MOX fuel rods having different plutonium contents with natural uranium or uranium tailings as carrier material but without burnable absorbers. The MOX fuel assembly designs for BWRs use four to six rod types with different plutonium contents and Gd[sub 2]O[sub 3]/UO[sub 2] burnable absorber rods. Both the PWR and the BWR designs attain good burnup equivalence and compatibility with uranium fuel assemblies. High flexibility exists in the loading schemes relative to the position and number of MOX fuel assemblies in the reloads and in the core as a whole. The Siemens experience with MOX fuel assemblies is based on the insertion of 318 MOX fuel assemblies in eight PWRs and 168 in BWRs and pressurized heavy water reactors so far. The primary operating results include information on the cycle length, power distribution, reactivity coefficients, and control rod worth of cores containing MOX fuel assemblies.

  17. ZPPR FUEL ELEMENT THERMAL STRESS-STRAIN ANALYSIS

    SciTech Connect

    Charles W. Solbrig; Jason Andrus; Chad Pope

    2014-04-01

    The design temperature of high plutonium concentration ZPPR fuel assemblies is 600 degrees C. Cladding integrity of the 304L stainless steel cladding is a significant concern with this fuel since even small holes can lead to substantial fuel degradation. Since the fuel has a higher coefficient of thermal expansion than the cladding, an investigation of the stress induced in the cladding due to the differential thermal expansion of fuel and cladding up to the design temperature was conducted. Small holes in the cladding envelope would be expected to lead to the fuel hydriding and oxidizing into a powder over a long period of time. This is the same type of chemical reaction chain that exists in the degradion of the high uranium concentration ZPPR fuel. Unfortunately, the uranium fuel was designed with vents which allowed this degradation to occur. The Pu cladding is sealed so only fuel with damaged cladding would be subject to this damage. The thermal stresses that can be developed in the fuel cladding have been calculated in in this paper and compared to the ultimate tensile stress of the cladding. The conclusion is drawn that thermal stresses cannot induce holes in the cladding even for the highest storage temperatures predicted in calculations (292°C). In fact, thermal stress can not cause cladding failure as long as the fuel temperatures are below the design limit of 600 degrees C (1,112 degrees F).

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

    DTIC Science & Technology

    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

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

    DTIC Science & Technology

    2008-09-03

    http://www.world-nuclear.org/info/inf69.html]. 53 World Nuclear Association, Mixed Oxide Fuel ( MOX ), November 2006, at [http://www.world-nuclear.org...oxide ( MOX ) fuel, in which the 239Pu largely substitutes for 235U. Two French reprocessing plants at La Hague can each reprocess up to 800 metric tons of...to reprocess gas-cooled reactor fuel, and India has a 275-ton plant.52 About 200 metric tons of MOX fuel is used annually, about 2% of new nuclear

  20. Alternative fuels

    NASA Technical Reports Server (NTRS)

    Grobman, J. S.; Butze, H. F.; Friedman, R.; Antoine, A. C.; Reynolds, T. W.

    1977-01-01

    Potential problems related to the use of alternative aviation turbine fuels are discussed and both ongoing and required research into these fuels is described. This discussion is limited to aviation turbine fuels composed of liquid hydrocarbons. The advantages and disadvantages of the various solutions to the problems are summarized. The first solution is to continue to develop the necessary technology at the refinery to produce specification jet fuels regardless of the crude source. The second solution is to minimize energy consumption at the refinery and keep fuel costs down by relaxing specifications.

  1. Validation of the SCALE code system using criticality data from experiments performed with Pu + U solutions in cylindrical and slab geometry

    SciTech Connect

    Smolen, G.R.; Funabashi, H.

    1988-01-01

    This paper outlines the results of a calculational study that was performed to validate two versions of the SCALE computer code system using data from critical experiments performed with mixed Pu + U aqueous solutions. The critical experiments were conducted in a 35-cm-diam cylinder and variable thickness slab tank. A companion paper reports on the criticality data that was obtained. These experimental activities are part of a joint exchange program between the US Department of Energy (USDOE) and the Power Reactor and Nuclear Fuel Development Corporation (PNC) of Japan in the area of criticality data development. The Consolidated Fuel Reprocessing Program (CFRP) at Oak Ridge National Laboratory (ORNL) manages the program for the USDOE. The experiments were conducted at the Battelle Pacific Northwest Laboratories-Critical Mass Laboratory (PNL-CML). 5 refs., 1 fig., 1 tab.

  2. Enhancing BWR Proliferation Resistance Fuel with Minor Actinides

    SciTech Connect

    Gray S. Chang

    2008-07-01

    Key aspects of the Global Nuclear Energy Partnership (GNEP) are to significantly advance the science and technology of nuclear energy systems and the Advanced Fuel Cycle (AFC) program. It consists of both innovative nuclear reactors and innovative research in separation and transmutation. To accomplish these goals, international cooperation is very important and public acceptance is crucial. The merits of nuclear energy are high-density energy, with low environmental impacts (i.e. almost zero greenhouse gas emission). Planned efforts involve near-term and intermediate-term improvements in fuel utilization and recycling in current light water reactors (LWRs) as well as the longer-term development of new nuclear energy systems that offer much improved fuel utilization and proliferation resistance, along with continued advances in operational safety. The challenges are solving the energy needs of the world, protection against nuclear proliferation, the problem of nuclear waste, and the global environmental problem. To reduce spent fuel for storage and enhance the proliferation resistance for the intermediate-term, there are two major approaches (a) increase the discharged spent fuel burnup in the advanced LWR (Gen-III Plus), which not only can reduce the spent fuel for storage, but also increase the 238Pu and 240Pu isotopes ratio to enhance the proliferation resistance, and (b) use of transuranic nuclides (237Np and 241Am) in the high burnup fuel, which can drastically increase the proliferation resistance isotope ratio of 238Pu /Pu. For future advanced nuclear systems, the minor actinides (MA) are viewed more as a resource to be recycled, or transmuted to less hazardous and possibly more useful forms, rather than simply as a waste stream to be disposed of in expensive repository facilities. As a result, MAs play a much larger part in the design of advanced systems and fuel cycles, not only as additional sources of useful energy, but also as direct contributors to the

  3. Simulation of radiation driven fission gas diffusion in UO2, ThO2 and PuO2

    SciTech Connect

    Cooper, Michael William D.; Stanek, Christopher Richard; Turnbull, James Anthony; Uberuaga, Blas P.; Andersson, David Anders

    2016-12-01

    Below 1000 K it is thought that fission gas diffusion in nuclear fuel during irradiation occurs through atomic mixing due to radiation damage. Here we present a molecular dynamics (MD) study of Xe, Kr, Th, U, Pu and O diffusion due to irradiation. It is concluded that the ballistic phase does not sufficiently account for the experimentally observed diffusion. Thermal spike simulations are used to confirm that electronic stopping remedies the discrepancy with experiment and the predicted diffusivities lie within the scatter of the experimental data. Here, our results predict that the diffusion coefficients are ordered such that D*0 > D*Kr > D*Xe > D*U. For all species >98.5% of diffusivity is accounted for by electronic stopping. Fission gas diffusivity was not predicted to vary significantly between ThO2, UO2 and PuO2, indicating that this process would not change greatly for mixed oxide fuels.

  4. Experimental Determination of Metal Fuel Point Defect Parameters

    SciTech Connect

    Fluss, M J; McCall, S

    2008-06-03

    Nuclear metallic fuels are one of many options for advanced nuclear fuel cycles because they provide dimensional stability, mechanical integrity, thermal efficiency, and irradiation resistance while the associated pyro-processing is technically relevant to concerns about proliferation and diversion of special nuclear materials. In this presentation we will discuss recent success that we have had in studying isochronal annealing of damage cascades in Pu and Pu(Ga) arising from the self-decay of Pu as well as the annealing characteristics of noninteracting point defect populations produced by ion accelerator irradiation. Comparisons of the annealing properties of these two populations of defects arising from very different source terms are enlightening and point to complex defect and mass transport properties in the plutonium specimens which we are only now starting to understand as a result of many follow-on studies. More importantly however, the success of these measurements points the way to obtaining important mass transport parameters for comparison with theoretical predictions or to use directly in existing and future materials modeling of radiation effects in nuclear metallic fuels. The way forward on such measurements and the requisite theory and modeling will be discussed.

  5. Estimate of the Sources of Plutonium-Containing Wastes Generated from MOX Fuel Production in Russia

    SciTech Connect

    Kudinov, K.G.; Tretyakov, A.A.; Sorokin, Y.P.; Bondin, V.V.; Manakova, L.F.; Jardine, L.J.

    2001-12-01

    In Russia, mixed oxide (MOX) fuel is produced in a pilot facility ''Paket'' at ''MAYAK'' Production Association. The Mining-Chemical Combine (MCC) has developed plans to design and build a dedicated industrial-scale plant to produce MOX fuel and fuel assemblies (FA) for VVER-1000 water reactors and the BN-600 fast-breeder reactor, which is pending an official Russian Federation (RF) site-selection decision. The design output of the plant is based on production capacity of 2.75 tons of weapons plutonium per year to produce the resulting fuel assemblies: 1.25 tons for the BN-600 reactor FAs and the remaining 1.5 tons for VVER-1000 FAs. It is likely the quantity of BN-600 FAs will be reduced in actual practice. The process of nuclear disarmament frees a significant amount of weapons plutonium for other uses, which, if unutilized, represents a constant general threat. In France, Great Britain, Belgium, Russia, and Japan, reactor-grade plutonium is used in MOX-fuel production. Making MOX-fuel for CANDU (Canada) and pressurized water reactors (PWR) (Europe) is under consideration Russia. If this latter production is added, as many as 5 tons of Pu per year might be processed into new FAs in Russia. Many years of work and experience are represented in the estimates of MOX fuel production wastes derived in this report. Prior engineering studies and sludge treatment investigations and comparisons have determined how best to treat Pu sludges and MOX fuel wastes. Based upon analyses of the production processes established by these efforts, we can estimate that there will be approximately 1200 kg of residual wastes subject to immobilization per MT of plutonium processed, of which approximately 6 to 7 kg is Pu in the residuals per MT of Pu processed. The wastes are various and complicated in composition. Because organic wastes constitute both the major portion of total waste and of the Pu to be immobilized, the recommended treatment of MOX-fuel production waste is incineration

  6. Toxicity of irradiated advanced heavy water reactor fuels.

    PubMed

    Priest, N D; Richardson, R B; Edwards, G W R

    2013-02-01

    The good neutron economy and online refueling capability of the CANDU® heavy water moderated reactor (HWR) enable it to use many different fuels such as low enriched uranium (LEU), plutonium, or thorium, in addition to its traditional natural uranium (NU) fuel. The toxicity and radiological protection methods for these proposed fuels, unlike those for NU, are not well established. This study uses software to compare the fuel composition and toxicity of irradiated NU fuel against those of two irradiated advanced HWR fuel bundles as a function of post-irradiation time. The first bundle investigated is a CANFLEX® low void reactor fuel (LVRF), of which only the dysprosium-poisoned central element, and not the outer 42 LEU elements, is specifically analyzed. The second bundle investigated is a heterogeneous high-burnup (LEU,Th)O(2) fuelled bundle, whose two components (LEU in the outer 35 elements and thorium in the central eight elements) are analyzed separately. The LVRF central element was estimated to have a much lower toxicity than that of NU at all times after shutdown. Both the high burnup LEU and the thorium fuel had similar toxicity to NU at shutdown, but due to the creation of such inhalation hazards as (238)Pu, (240)Pu, (242)Am, (242)Cm, and (244)Cm (in high burnup LEU), and (232)U and (228)Th (in irradiated thorium), the toxicity of these fuels was almost double that of irradiated NU after 2,700 d of cooling. New urine bioassay methods for higher actinoids and the analysis of thorium in fecal samples are recommended to assess the internal dose from these two fuels.

  7. Assessment of Nuclear Resonance Fluorescence for Spent Nuclear Fuel Assay

    SciTech Connect

    Quiter, Brian; Ludewigt, Bernhard; Ambers, Scott

    2011-06-30

    In nuclear resonance fluorescence (NRF) measurements, resonances are excited by an external photon beam leading to the emission of gamma rays with specific energies that are characteristic of the emitting isotope. NRF promises the unique capability of directly quantifying a specific isotope without the need for unfolding the combined responses of several fissile isotopes as is required in other measurement techniques. We have analyzed the potential of NRF as a non-destructive analysis technique for quantitative measurements of Pu isotopes in spent nuclear fuel (SNF). Given the low concentrations of 239Pu in SNF and its small integrated NRF cross sections, the main challenge in achieving precise and accurate measurements lies in accruing sufficient counting statistics in a reasonable measurement time. Using analytical modeling, and simulations with the radiation transport code MCNPX that has been experimentally tested recently, the backscatter and transmission methods were quantitatively studied for differing photon sources and radiation detector types. Resonant photon count rates and measurement times were estimated for a range of photon source and detection parameters, which were used to determine photon source and gamma-ray detector requirements. The results indicate that systems based on a bremsstrahlung source and present detector technology are not practical for high-precision measurements of 239Pu in SNF. Measurements that achieve the desired uncertainties within hour-long measurements will either require stronger resonances, which may be expressed by other Pu isotopes, or require quasi-monoenergetic photon sources with intensities that are approximately two orders of magnitude higher than those currently being designed or proposed.This work is part of a larger effort sponsored by the Next Generation Safeguards Initiative to develop an integrated instrument, comprised of individual NDA techniques with complementary features, that is fully capable of

  8. Thermodynamic assessments and inter-relationships between systems involving Al, Am, Ga, Pu, and U

    NASA Astrophysics Data System (ADS)

    Perron, A.; Turchi, P. E. A.; Landa, A.; Oudot, B.; Ravat, B.; Delaunay, F.

    2016-12-01

    A newly developed self-consistent CALPHAD thermodynamic database involving Al, Am, Ga, Pu, and U is presented. A first optimization of the slightly characterized Am-Al and completely unknown Am-Ga phase diagrams is proposed. To this end, phase diagram features as crystal structures, stoichiometric compounds, solubility limits, and melting temperatures have been studied along the U-Al → Pu-Al → Am-Al, and U-Ga → Pu-Ga → Am-Ga series, and the thermodynamic assessments involving Al and Ga alloying are compared. In addition, two distinct optimizations of the Pu-Al phase diagram are proposed to account for the low temperature and Pu-rich region controversy. The previously assessed thermodynamics of the other binary systems (Am-Pu, Am-U, Pu-U, and Al-Ga) is also included in the database and is briefly described in the present work. Finally, predictions on phase stability of ternary and quaternary systems of interest are reported to check the consistency of the database.

  9. Change Spectroscopic, thermal and mechanical studies of PU/PVC blends

    NASA Astrophysics Data System (ADS)

    Hezma, A. M.; Elashmawi, I. S.; Rajeh, A.; Kamal, Mustafa

    2016-08-01

    Blends of polyurethane (PU) and polyvinyl chloride (PVC) with different concentrations were prepared by casting method. The effects of PU on PVC blends was examined by Fourier transform-infrared (FTIR), Ultra-violet visible studies (UV/VIS.), X-ray diffraction (XRD), Thermogravimetric (TGA), Differential scanning calorimetry (DSC), and mechanical properties (stress-strain curve). The interaction between PU and PVC was examined by FT-IR through the absorbance of the N-H groups and was correlated to mechanical/thermal properties. Ultra-violet visible said that optical energy gap decrease with increasing concentration of PU. Differential scanning calorimetry results was observed a single glass transition temperature (Tg) for blends this confirming existence miscibility within the blends. The causes for best thermal stability of some blends may be described by measurements of interactions between C=O groups of PU and the α-hydrogen of PVC or a dipole-dipole -C=O..Cl-C- interactions. Significant alterations in FTIR, X-ray and DSC examination shows an interactions between blends had good miscibility. X-ray shows some alterations in the intensity with additional PU. PU change the mechanical behavior of PVC through of the blends. When polyurethane content increase causes polyvinyl chloride tensile strength decreases and elongation at break increase.

  10. Minimum pickup velocity ( U pu) of nanoparticles in gas-solid pneumatic conveying

    NASA Astrophysics Data System (ADS)

    Anantharaman, Aditya; van Ommen, J. Ruud; Chew, Jia Wei

    2015-12-01

    This paper is the first systematic study of the pneumatic conveying of nanoparticles. The minimum pickup velocity, U pu, of six nanoparticle species of different materials [i.e., silicon dioxide (SiO2), aluminum oxide (Al2O3), and titanium dioxide (TiO2)] and surfaces (i.e., apolar and polar) was determined by the weight loss method. Results show that (1) due to relative lack of hydrogen bonding, apolar nanoparticles had higher mass loss values at the same velocities, mass loss curves with accentuated S-shaped profiles, and lower U pu values, (2) among the three species, SiO2, which has the lowest Hamaker coefficient, exhibited the greatest discrepancy between apolar and polar surfaces with respect to both mass loss curves and U pu values, (3) U mf,polar/ U mf,apolar was between 1 and 3.5 times that of U pu,polar/ U pu,apolar due to greater extents of hydrogen bonding associated with U mf, (4) U pu values were at least an order-of-magnitude lower than that expected from the well-acknowledged U pu correlation (Kalman et al., Powder Technol 160:103-113, 2005) due to agglomeration, (5) although nanoparticles should be categorized as Zone III (Kalman et al. 2005) (or Geldart group C, Powder Technol 7:285-292, 1973), the nanoparticles, and primary and complex agglomerates agreed more with the Zone I (or Geldart group B) correlation.

  11. Langerhans cells are generated by two distinct PU.1-dependent transcriptional networks.

    PubMed

    Chopin, Michaël; Seillet, Cyril; Chevrier, Stéphane; Wu, Li; Wang, Hongsheng; Morse, Herbert C; Belz, Gabrielle T; Nutt, Stephen L

    2013-12-16

    Langerhans cells (LCs) are the unique dendritic cells found in the epidermis. While a great deal of attention has focused on defining the developmental origins of LCs, reports addressing the transcriptional network ruling their differentiation remain sparse. We addressed the function of a group of key DC transcription factors-PU.1, ID2, IRF4, and IRF8-in the establishment of the LC network. We show that although steady-state LC homeostasis depends on PU.1 and ID2, the latter is dispensable for bone marrow-derived LCs. PU.1 controls LC differentiation by regulating the expression of the critical TGF-β responsive transcription factor RUNX3. PU.1 directly binds to the Runx3 regulatory elements in a TGF-β-dependent manner, whereas ectopic expression of RUNX3 rescued LC differentiation in the absence of PU.1 and promoted LC differentiation from PU.1-sufficient progenitors. These findings highlight the dual molecular network underlying LC differentiation, and show the central role of PU.1 in these processes.

  12. Thermodynamic assessments and inter-relationships between systems involving Al, Am, Ga, Pu, and U

    SciTech Connect

    Perron, A.; Turchi, P. E. A.; Landa, A.; Oudot, B.; Ravat, B.; Delaunay, F.

    2016-12-01

    We present a newly developed self-consistent CALPHAD thermodynamic database involving Al, Am, Ga, Pu, and U. A first optimization of the slightly characterized Am-Al and completely unknown Am-Ga phase diagrams is proposed. To this end, phase diagram features as crystal structures, stoichiometric compounds, solubility limits, and melting temperatures have been studied along the U-Al → Pu-Al → Am-Al, and U-Ga → Pu-Ga → Am-Ga series, and the thermodynamic assessments involving Al and Ga alloying are compared. In addition, two distinct optimizations of the Pu-Al phase diagram are proposed to account for the low temperature and Pu-rich region controversy. We included the previously assessed thermodynamics of the other binary systems (Am-Pu, Am-U, Pu-U, and Al-Ga) in the database and is briefly described in the present work. In conclusion, predictions on phase stability of ternary and quaternary systems of interest are reported to check the consistency of the database.

  13. The coprecipitation of Pu and other radionuclides with CaCO[sub 3

    SciTech Connect

    Meece, D.E.; Benninger, L.K. )

    1993-04-01

    The record of fallout plutonium concentrations in annual bands of corals is strikingly similar to the record of atmospheric deposition of [sup 90]Sr. This similarity implies that corals may incorporate Pu from seawater with a constant partition coefficient (constant discrimination). To investigate physicochemical aspects of Pu incorporation, the following have been coprecipitated with CaCO[sub 3] (calcite and aragonite): oxidized and reduced Pu; americium, thorium, and uranium as analogs to Pu oxidation states (III, IV, VI), respectively; and [sup 210]Pb as a particle-reactive nuclide which may be incorporated by corals with constant discrimination. Americium, thorium, and lead adsorb onto both calcite and aragonite, with more than 99% of the recovered activity found associated with the solids. Uranium exhibits a behavior consistent with lattice substitution. Partition coefficients for U in aragonite range from 1.8 to 9.8 and vary inversely with pH and/or rate of precipitation. The partition coefficient for U in calcite is less than 0.2 and may be as low as 0.046. Reduced Pu sorbs with 3 to 4% remaining in solution. Oxidized Pu may both sorb and coprecipitate. The coral record for Pb and U results primarily from biological, rather than physicochemical, effects; it is likely that the PU coral record also reflects biological discrimination. 50 refs., 4 figs., 5 tabs.

  14. Criticality Safety Controls for 55-Gallon Drums with a Mass Limit of 200 grams Pu-239

    SciTech Connect

    Chou, P

    2011-12-14

    The following 200-gram Pu drum criticality safety controls are applicable to RHWM drum storage operations: (1) Mass (Fissile/Pu) - each 55-gallon drum or its equivalent shall be limited to 200 gram Pu or Pu equivalent; (2) Moderation - Hydrogen materials with a hydrogen density greater than that (0.133 g H/cc) of polyethylene and paraffin are not allowed and hydrogen materials with a hydrogen density no greater than that of polyethylene and paraffin are allowed with unlimited amounts; (3) Interaction - a spacing of 30-inches (76 cm) is required between arrays and 200-gram Pu drums shall be placed in arrays for 200-gram Pu drums only (no mingling of 200-gram Pu drums with other drums not meeting the drum controls associated with the 200-gram limit); (4) Reflection - no beryllium and carbon/graphite (other than the 50-gram waiver amount) is allowed, (note that Nat-U exceeding the waiver amount is allowed when its U-235 content is included in the fissile mass limit of 200 grams); and (5) Geometry - drum geometry, only 55-gallon drum or its equivalent shall be used and array geometry, 55-gallon drums are allowed for 2-high stacking. Steel waste boxes may be stacked 3-high if constraint.

  15. Melting behavior of (Th,U)O2 and (Th,Pu)O2 mixed oxides

    NASA Astrophysics Data System (ADS)

    Ghosh, P. S.; Kuganathan, N.; Galvin, C. O. T.; Arya, A.; Dey, G. K.; Dutta, B. K.; Grimes, R. W.

    2016-10-01

    The melting behaviors of pure ThO2, UO2 and PuO2 as well as (Th,U)O2 and (Th,Pu)O2 mixed oxides (MOX) have been studied using molecular dynamics (MD) simulations. The MD calculated melting temperatures (MT) of ThO2, UO2 and PuO2 using two-phase simulations, lie between 3650-3675 K, 3050-3075 K and 2800-2825 K, respectively, which match well with experiments. Variation of enthalpy increments and density with temperature, for solid and liquid phases of ThO2, PuO2 as well as the ThO2 rich part of (Th,U)O2 and (Th,Pu)O2 MOX are also reported. The MD calculated MT of (Th,U)O2 and (Th,Pu)O2 MOX show good agreement with the ideal solidus line in the high thoria section of the phase diagram, and evidence for a minima is identified around 5 atom% of ThO2 in the phase diagram of (Th,Pu)O2 MOX.

  16. Thermodynamic assessments and inter-relationships between systems involving Al, Am, Ga, Pu, and U

    DOE PAGES

    Perron, A.; Turchi, P. E. A.; Landa, A.; ...

    2016-12-01

    We present a newly developed self-consistent CALPHAD thermodynamic database involving Al, Am, Ga, Pu, and U. A first optimization of the slightly characterized Am-Al and completely unknown Am-Ga phase diagrams is proposed. To this end, phase diagram features as crystal structures, stoichiometric compounds, solubility limits, and melting temperatures have been studied along the U-Al → Pu-Al → Am-Al, and U-Ga → Pu-Ga → Am-Ga series, and the thermodynamic assessments involving Al and Ga alloying are compared. In addition, two distinct optimizations of the Pu-Al phase diagram are proposed to account for the low temperature and Pu-rich region controversy. We includedmore » the previously assessed thermodynamics of the other binary systems (Am-Pu, Am-U, Pu-U, and Al-Ga) in the database and is briefly described in the present work. In conclusion, predictions on phase stability of ternary and quaternary systems of interest are reported to check the consistency of the database.« less

  17. Minimal PU.1 reduction induces a preleukemic state and promotes development of acute myeloid leukemia

    PubMed Central

    Will, Britta; Vogler, Thomas O.; Narayanagari, Swathi; Bartholdy, Boris; Todorova, Tihomira I.; da Silva Ferreira, Mariana; Chen, Jiahao; Yu, Yiting; Mayer, Jillian; Barreyro, Laura; Carvajal, Luis; Ben Neriah, Daniela; Roth, Michael; van Oers, Johanna; Schaetzlein, Sonja; McMahon, Christine; Edelmann, Winfried; Verma, Amit; Steidl, Ulrich

    2016-01-01

    Modest transcriptional changes caused by genetic or epigenetic mechanisms are frequent in human cancer. Although loss or near-complete loss of the hematopoietic transcription factor PU.1 induces acute myeloid leukemia (AML) in mice, a similar degree of PU.1 impairment is exceedingly rare in human AML; yet moderate PU.1 inhibition is common in AML patients. We assessed functional consequences of modest reduction of PU.1 expression on leukemia development in mice harboring DNA lesions resembling those acquired during human stem cell aging. Heterozygous deletion of an enhancer of PU.1, which resulted in 35% reduction of PU.1 expression, was sufficient to induce myeloid biased preleukemic stem cells and subsequent transformation to AML in a DNA mismatch repair-deficient background. AML progression was mediated by inhibition of expression of a PU.1 cooperating transcription factor, Irf8. Strikingly, we found significant molecular similarities with human myelodysplastic syndrome and AML. This study demonstrates that minimal reduction of a key lineage-specific transcription factor that commonly occurs in human disease is sufficient to initiate cancer development and provides mechanistic insight into the formation and progression of preleukemic stem cells in AML. PMID:26343801

  18. EnEnvironmental Mobility of Pu(IV) in the Presence of Ethylenediaminetetraacetic Acid: Myth or Reality

    SciTech Connect

    Rai, Dhanpat; Moore, Dean A.; Rosso, Kevin M.; Felmy, Andrew R.; Bolton, Harvey

    2008-07-01

    Ethylenediaminetetracetic acid (EDTA), which was co-disposed with Pu at several U. S. Department of Energy sites, has been reported to enhance the solubility and transport of Pu. It is generally assumed that this enhanced transport of Pu in geologic environments is a result of complexation of Pu(IV) with EDTA. However, the fundamental bases for this assumption have never been fully explored. Whether EDTA can mobilize Pu(IV) in geologic environments is dependent on many factors, chief among them are not only the complexation constants of Pu with EDTA and dominant oxidation state and the nature of Pu solids, but also 1) the complexation constants of environmentally important metal ions (e.g. Fe, Al, Ca, Mg) that compete with Pu for EDTA and 2) EDTA interactions with geomedia (e.g., adsorption, biodegradation) that reduce effective EDTA concentrations available for complexation. Extensive studies over a large range of pH values (1 to 14) and EDTA concentrations (0.0001 to 0.01 M) as a function of time were conducted on the solubility of 2-line ferrihydrite (Fe(OH)3(s)), PuO2(am) in the presence of different concentrations of Ca ions, and mixtures of PuO2(am) and Fe(OH)3(s). The solubility data were interpreted using Pitzer’s ion-interaction approach to determine/validate the solubility product of Fe(OH)3(s), the complexation constants of Pu(IV)-EDTA and Fe(III)-EDTA, and to determine the affect of EDTA in solubilizing Pu(IV) from PuO2(am) in the presence of Fe(III) compounds and aqueous Ca concentrations. Predictions based on these extensive fundamental data show that environmental mobility of Pu as a result of Pu(IV)-EDTA complexation as reported/implied in the literature is a myth rather than the reality.

  19. High-Energy Delayed Gamma Spectroscopy for Spent Nuclear Fuel Assay

    SciTech Connect

    Campbell, Luke W.; Smith, Leon E.; Misner, Alex C.; Ressler, Jennifer J.

    2009-10-07

    High-accuracy, direct, nondestructive measurement of fissile and fissionable isotopes in spent fuel, particularly the Pu isotopes, is a well-documented, but still unmet challenge in international safeguards. As nuclear fuel cycles propagate around the globe, the need for improved materials accountancy techniques for irradiated light-water reactor fuel will only increase (e.g. for shipper-receiver verification at interim or permanent storage, or at the head end of a reprocessing plant). This modeling study investigates the use of delayed gamma rays from fission-product nuclei to directly measure the relative concentrations of U-235, Pu-239, and Pu-241 in spent fuel assemblies. The method is based on the unique distribution of fission-product nuclei produced from fission in each of these fissile isotopes. Fission is stimulated in the assembly with a beam of interrogating neutrons and the measured distributions of the short-lived fission products from the unknown sample are then fit with a linear combination of the known fission-product yield curves from pure U-235, Pu-239, and Pu-241 to determine the original proportions of these fissile isotopes. Modeling approaches for the intense gamma-ray background promulgated by the long-lived fission-product inventory, and the high-energy gamma-ray signatures emitted by short-lived fission products from induced fission are described. Results for the simulated assay of simplified individual fuel elements ranging from fresh to 60 GWd/MTU burnup are used to demonstrate the utility of the modeling methods and provide preliminary viability data for the technique. A limited set of benchmarking measurements, and additional work needed to more realistically assess the potential of the High-Energy Delayed Gamma Spectroscopy (HEDGS) technique are described.

  20. High-Energy Delayed Gamma Spectroscopy for Spent Nuclear Fuel Assay

    SciTech Connect

    Campbell, Luke W.; Smith, Leon E.; Misner, Alex C.

    2011-02-01

    High-accuracy, direct, nondestructive measurement of fissile and fissionable isotopes in spent fuel, particularly the Pu isotopes, is a well-documented, but still unmet challenge in international safeguards. As nuclear fuel cycles propagate around the globe, the need for improved materials accountancy techniques for irradiated light-water reactor fuel will increase. This modeling study investigates the use of delayed gamma rays from fission-product nuclei to directly measure the relative concentrations of U-235, Pu-239, and Pu-241 in spent fuel assemblies. The method is based on the unique distribution of fission-product nuclei produced from fission in each of these fissile isotopes. Fission is stimulated in the assembly with a pulse-capable source of interrogating neutrons. The measured distributions of the short-lived fission products from the unknown sample are then fit with a linear combination of the known fission-product yield curves from pure U-235, Pu-239, and Pu-241 to determine the original proportions of these fissile isotopes. Modeling approaches for the intense gamma-ray background promulgated by the long-lived fission-product inventory and for the high-energy gamma-ray signatures emitted by short-lived fission products from induced fission are described. Benchmarking measurements are presented and compare favorably with the results of these models. Results for the simulated assay of simplified individual fuel elements ranging from fresh to 60 GWd/MTU burnup demonstrate the utility of the modeling methods for viability studies, although additional work is needed to more realistically assess the potential of High-Energy Delayed Gamma Spectroscopy (HEDGS).

  1. Restructuring and redistribution of actinides in Am-MOX fuel during the first 24 h of irradiation

    NASA Astrophysics Data System (ADS)

    Tanaka, Kosuke; Miwa, Shuhei; Sekine, Shin-ichi; Yoshimochi, Hiroshi; Obayashi, Hiroshi; Koyama, Shin-ichi

    2013-09-01

    In order to confirm the effect of minor actinide additions on the irradiation behavior of MOX fuel pellets, 3 wt.% and 5 wt.% americium-containing MOX (Am-MOX) fuels were irradiated for 10 min at 43 kW/m and for 24 h at 45 kW/m in the experimental fast reactor Joyo. Two nominal values of the fuel pellet oxygen-to-metal ratio (O/M), 1.95 and 1.98, were used as a test parameter. Emphasis was placed on the behavior of restructuring and redistribution of actinides which directly affect the fuel performance and the fuel design for fast reactors. Microstructural evolutions in the fuels were observed by optical microscopy and the redistribution of constituent elements was determined by EPMA using false color X-ray mapping and quantitative point analyses. The ceramography results showed that structural changes occurred quickly in the initial stage of irradiation. Restructuring of the fuel from middle to upper axial positions developed and was almost completed after the 24-h irradiation. No sign of fuel melting was found in any of the specimens. The EPMA results revealed that Am as well as Pu migrated radially up the temperature gradient to the center of the fuel pellet. The increase in Am concentration on approaching the edge of the central void and its maximum value were higher than those of Pu after the 10-min irradiation and the difference was more pronounced after the 24-h irradiation. The increment of the Am and Pu concentrations due to redistribution increased with increasing central void size. In all of the specimens examined, the extent of redistribution of Am and Pu was higher in the fuel of O/M ratio of 1.98 than in that of 1.95.

  2. Transmutation, Burn-Up and Fuel Fabrication Trade-Offs in Reduced-Moderation Water Reactor Thorium Fuel Cycles - 13502

    SciTech Connect

    Lindley, Benjamin A.; Parks, Geoffrey T.; Franceschini, Fausto

    2013-07-01

    Multiple recycle of long-lived actinides has the potential to greatly reduce the required storage time for spent nuclear fuel or high level nuclear waste. This is generally thought to require fast reactors as most transuranic (TRU) isotopes have low fission probabilities in thermal reactors. Reduced-moderation LWRs are a potential alternative to fast reactors with reduced time to deployment as they are based on commercially mature LWR technology. Thorium (Th) fuel is neutronically advantageous for TRU multiple recycle in LWRs due to a large improvement in the void coefficient. If Th fuel is used in reduced-moderation LWRs, it appears neutronically feasible to achieve full actinide recycle while burning an external supply of TRU, with related potential improvements in waste management and fuel utilization. In this paper, the fuel cycle of TRU-bearing Th fuel is analysed for reduced-moderation PWRs and BWRs (RMPWRs and RBWRs). RMPWRs have the advantage of relatively rapid implementation and intrinsically low conversion ratios. However, it is challenging to simultaneously satisfy operational and fuel cycle constraints. An RBWR may potentially take longer to implement than an RMPWR due to more extensive changes from current BWR technology. However, the harder neutron spectrum can lead to favourable fuel cycle performance. A two-stage fuel cycle, where the first pass is Th-Pu MOX, is a technically reasonable implementation of either concept. The first stage of the fuel cycle can therefore be implemented at relatively low cost as a Pu disposal option, with a further policy option of full recycle in the medium term. (authors)

  3. Determining site-specific drum loading criteria for storing combustible {sup 238}Pu waste

    SciTech Connect

    Marshall, R.S.; Callis, E.L.; Cappis, J.H.; Espinoza, J.M.; Foltyn, E.M.; Reich, B.T.; Smith, M.C.

    1994-02-01

    Waste containing hydrogenous-combustible material contaminated with {sup 238}Pu can generate hydrogen gas at appreciable rates through alpha radiolysis. To ensure safe transportation of WIPP drums, the limit for {sup 238}Pu-combustible waste published in the WIPP TRUPACT-11 CONTENT (TRUCON) CODES is 21 milliwafts per 55 gallon drum. This corresponds to about 45 milligrams of {sup 238}PuO{sub 2} used for satellite heat source-electrical generators. The Los Alamos waste storage site adopted a {sup 238}Pu waste storage criteria based on these TRCUCON codes. However, reviews of the content in drums of combustible waste generated during heat source assembly at Los Alamos showed the amount of {sup 238}Pu is typically much greater than 45 milligrams. It is not feasible to appreciably reduce Los Alamos {sup 238}Pu waste drum loadings without significantly increasing waste volumes or introducing unsafe practices. To address this concern, a series of studies were implemented to evaluate the applicability of the TRUCON limits for storage of this specific waste. Addressed in these evaluations were determination of the hydrogen generation rate, hydrogen diffusion rates through confinement layers and vent filters, and packaging requirements specific to Los Alamos generated {sup 238}Pu contaminated combustible waste. These studies also showed that the multiple-layer packaging practices in use at Los Alamos could be relaxed without significantly increasing the risk of contamination. Based on a model developed to predict H{sub 2} concentrations in packages and drum headspace, the site specific effective hydrogen generation rate, and hydrogen-diffusion values, and revising the waste packaging practices, we were able to raise the safe loading limit for {sup 238}Pu waste drums for on site storage to the gram levels typical of currently generated {sup 238}Pu waste.

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

    SciTech Connect

    Hickman, A.W. Jr.

    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.

  5. Investigation of the Performance of D2O-Cooled High-Conversion Reactors for Fuel Cycle Calculations

    SciTech Connect

    Hikaru Hiruta; Gilles Youinou

    2013-09-01

    This report presents FY13 activities for the analysis of D2O cooled tight-pitch High-Conversion PWRs (HCPWRs) with U-Pu and Th-U fueled cores aiming at break-even or near breeder conditions while retaining the negative void reactivity. The analyses are carried out from several aspects which could not be covered in FY12 activities. SCALE 6.1 code system is utilized, and a series of simple 3D fuel pin-cell models are developed in order to perform Monte Carlo based criticality and burnup calculations. The performance of U-Pu fueled cores with axial and internal blankets is analyzed in terms of their impact on the relative fissile Pu mass balance, initial Pu enrichment, and void coefficient. In FY12, Pu conversion performances of D2O-cooled HCPWRs fueled with MOX were evaluated with small sized axial/internal DU blankets (approximately 4cm of axial length) in order to ensure the negative void reactivity, which evidently limits the conversion performance of HCPWRs. In this fiscal year report, the axial sizes of DU blankets are extended up to 30 cm in order to evaluate the amount of DU necessary to reach break-even and/or breeding conditions. Several attempts are made in order to attain the milestone of the HCPWR designs (i.e., break-even condition and negative void reactivity) by modeling of HCPWRs under different conditions such as boiling of D2O coolant, MOX with different 235U enrichment, and different target burnups. A similar set of analyses are performed for Th-U fueled cores. Several promising characteristics of 233U over other fissile like 239Pu and 235U, most notably its higher fission neutrons per absorption in thermal and epithermal ranges combined with lower ___ in the fast range than 239Pu allows Th-U cores to be taller than MOX ones. Such an advantage results in 4% higher relative fissile mass balance than that of U-Pu fueled cores while retaining the negative void reactivity until the target burnup of 51 GWd/t. Several other distinctions between U-Pu and

  6. Plants as bio-monitors for Cs-137, Pu-238, Pu-239,240 and K-40 at the Savannah River Site.

    PubMed

    Caldwell, Eric Frank; Duff, Martine C; Ferguson, Caitlin E; Coughlin, Daniel P

    2011-05-01

    The Savannah River Site was constructed in South Carolina to produce plutonium (Pu) in the 1950s. Discharges associated with these now-ceased operations have contaminated large areas within the site, particularly streams associated with reactor cooling basins. Evaluating the exposure risk of contamination to an ecosystem requires methodologies that can assess the bioavailability of contaminants. Plants, as primary producers, represent an important mode of transfer of contaminants from soils and sediments into the food chain. The objective of this study was to identify local area plants for their ability to act as bio-monitors of radionuclides. The concentrations of cesium-137 ((137)Cs), potassium-40 ((40)K), (238)Pu and (239,240)Pu in plants and their associated soils were determined using γ and α spectrometry. The ratio of contamination concentration found in the plant relative to the soil was calculated to assess a concentration ratio (CR). The highest CR for (137)Cs was found in Pinus palustris needles (CR of 2.18). The correlation of soil and plant (137)Cs concentration was strong (0.76) and the R(2) (0.58) from the regression was significant (p = 0.006). This suggests the ability to predict the degree of (137)Cs contamination of a soil through analysis of the pine needles. The (238)Pu and (239,240)Pu concentrations were most elevated within the plant roots. Extremely high CR values were found in Sparganium americanum (bur-reed) roots with a value of 5.86 for (238)Pu and 5.66 for (239,240)Pu. The concentration of (40)K was measured as a known congener of (137)C. Comparing (40)K and (137)C concentrations in each plant revealed an inverse relationship for these radioisotopes. Correlating (40)K and (137)Cs was most effective in identifying plants that have a high affinity for (137)Cs uptake. The P. palustris and S. americanum proved to be particularly strong accumulators of all K congeners from the soil. Some species that were measured, warrant further

  7. Topological analysis of void space in phosphate frameworks: Assessing storage properties for the environmentally important guest molecules and ions: CO2, H2O, UO2, PuO2, U, Pu, Sr2+, Cs+, CH4, and H2

    DOE PAGES

    Cramer, Alisha J.; Cole, Jacqueline M.

    2016-06-27

    The entrapment of environmentally important materials to enable containment of polluting wastes from industry or energy production, storage of alternative fuels, or water sanitation, is of vital and immediate importance. Many of these materials are small molecules or ions that can be encapsulated via their adsorption into framework structures to create a host-guest complex. This is an ever-growing field of study and, as such, the search for more suitable porous materials for environmental applications is fundamental to progress. However, many industrial areas that require the use of adsorbents are fraught with practical challenges such as high temperatures, rapid gas expansion,more » radioactivity, or repetitive gas cycling, that the host material must withstand. Inorganic phosphates have a proven history of rigid structures, thermal stability, and are suspected to possess good resistance to radiation over geologic time scales. Furthermore, various experimental studies have established their ability to adsorb small molecules, such as water. In light of this, all known crystal structures of phosphate frameworks with meta- (P3O9) or ultra- (P5O14) stoichiometries are combined in a data-mining survey together with all theoretically possible structures of LnaPbOc (where a, b, c are any integer, and Ln = La, Ce, Pr, Nd, Sm, Eu, Gd, Tb, Dy, Ho, Er, or Tm) that are statistically likely to form. Topological patterns within these framework structures are used to assess their suitability for hosting a variety of small guest molecules or ions that are important for environmental applications: CO2, H2O, UO2, PuO2, U, Pu, Sr2+, Cs+, CH4 and H2. A range of viable phosphate-based host-guest complexes are identified from this data-mining and pattern-based structural analysis. Moreover, distinct topological preferences for hosting such guests are found, and metaphosphate stoichiometries are generally preferred over ultraphosphate configurations.« less

  8. I-Pu-Xe dating and the relative ages of the earth and moon

    NASA Technical Reports Server (NTRS)

    Swindle, T. D.; Caffee, M. W.; Hohenberg, C. M.; Taylor, S. R.

    1986-01-01

    The ages of the earth and moon as determined by various chronometric systems are discussed with primary emphasis placed on the development of an I-Pu-Xe chronometer. Data on excess fission xenon are reviewed with attention given to the strengths and weaknesses of the assumptions required for lunar I-Pu-Xe chronometry. Using I-Pu-Xe dating, it is estimated that the retention of excess fission xenon in lunar samples began no more than 63 + or - 42 m.y. after the time of primitive meteorite formation.

  9. Operation of the Oxide Washer for Water-Washing Solubles out of Impure Pu Oxide

    SciTech Connect

    Dodson, K E; Close, W L; Krikorian, O H; Summers III, H V

    2006-01-30

    An evaluation has been made for using the Oxide Washer to wash water-soluble materials out of impure Pu oxide. It is found that multiple washes are needed to reduce the water-soluble materials to very low levels in the impure Pu oxides. The removal of the wash water from the Oxide Washer is accompanied by particulates of the impure Pu oxide, which subsequently need to be filtered out. In spite of the additional filtration needed, the overall level of manpower required for processing is still only about one third of that for an all-manual operation.

  10. Isochronal annealing of radiation damage in (alpha)- and (delta)-Pu alloys

    SciTech Connect

    McCall, S K; Fluss, M J; Chung, B W; Haire, R G

    2009-06-22

    Magnetic isochronal annealing curves were measured on specimens of self damaged {alpha}-Pu and several {delta}-Pu alloys stabilized by Ga and Am. These results are compared to one another and to isochronal resistivity annealing curves, where distinct differences are observed between the magnetic and resistive annealing for the case of {delta}-Pu. The first stage of annealing observed in the resistivity measurements is largely missing from the magnetic measurements, indicating that interstitials contribute little if any signal to the magnetization, while the onset of vacancy migration is strongly reflected in the magnetization signal.

  11. Reaction of Np(VI) and Pu(IV) with heteroblues in aqueous solutions

    SciTech Connect

    Shilov, V.P.; Astafurova, L.N.; Krot, N.N.

    1995-01-01

    Reactions of heteroblues SiMo{sub 12}, PMo{sub 12}, PV{sub 2}Mo{sub 10}, PV{sub 6}Mo{sub 6}, and P{sub 2}W{sub 18} with Np(VI) and Pu(IV) in HCl and HNO{sub 3} solutions are studied by spectrophotometry. The species Np(VI) is quickly reduced by all five blues. The species Pu(IV) is reduced by the first four blues if the solution of heteroblue is added to the Pu solution and is not reduced by any blues if they contain HNO{sub 3}.

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

    NASA Astrophysics Data System (ADS)

    Hain, K.; Faestermann, T.; Famulok, N.; Fimiani, L.; Gómez-Guzmán, J. M.; Korschinek, G.; Kortmann, F.; Lierse v. Gostomski, Ch.; Ludwig, P.; Shinonaga, T.

    2015-10-01

    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. 241Am, which causes isobaric background to 241Pu in mass spectrometric measurements, was successfully separated from the Pu fraction by this method. Water samples which were spiked with 242Pu and 237Np or 239Np, 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 240Pu, 241Pu and 237Np obtained in this study are in agreement with the certified and literature values within the uncertainties. Due to strong isotopic interference of 239Pu with 238U, it was not possible to analyze the concentration of 239Pu. 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.

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

    SciTech Connect

    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.

  14. Regulation of early T-lineage gene expression and developmental progression by the progenitor cell transcription factor PU.1

    PubMed Central

    Champhekar, Ameya; Damle, Sagar S.; Freedman, George; Carotta, Sebastian; Nutt, Stephen L.

    2015-01-01

    The ETS family transcription factor PU.1 is essential for the development of several blood lineages, including T cells, but its function in intrathymic T-cell precursors has been poorly defined. In the thymus, high PU.1 expression persists through multiple cell divisions in early stages but then falls sharply during T-cell lineage commitment. PU.1 silencing is critical for T-cell commitment, but it has remained unknown how PU.1 activities could contribute positively to T-cell development. Here we employed conditional knockout and modified antagonist PU.1 constructs to perturb PU.1 function stage-specifically in early T cells. We show that PU.1 is needed for full proliferation, restricting access to some non-T fates, and controlling the timing of T-cell developmental progression such that removal or antagonism of endogenous PU.1 allows precocious access to T-cell differentiation. Dominant-negative effects reveal that this repression by PU.1 is mediated indirectly. Genome-wide transcriptome analysis identifies novel targets of PU.1 positive and negative regulation affecting progenitor cell signaling and cell biology and indicating distinct regulatory effects on different subsets of progenitor cell transcription factors. Thus, in addition to supporting early T-cell proliferation, PU.1 regulates the timing of activation of the core T-lineage developmental program. PMID:25846797

  15. Building flexibility into the design of a pilot plant for the immobilisation of Pu containing residues and wastes

    SciTech Connect

    Scales, C R; Maddrell, E R; Hobbs, J; Stephen, R; Moricca, S; Stewart, M W A

    2013-07-01

    NNL and ANSTO on behalf of Sellafield Ltd have developed a process for the immobilisation of a range of Pu containing wastes and residues. Following the inactive demonstration of the technology the project is now focusing on the design of an active pilot plant capable of validating the technology and ultimately immobilising a waste inventory containing around 100 kg plutonium. The diverse wastes from which it is uneconomic to recover Pu, require a flexible process with a wide product envelope capable of producing a wasteform suitable for disposal in a UK repository. Ceramics, glass ceramics and metal encapsulated waste-forms can be delivered by the process line which incorporates size reduction and heat treatment techniques with the aim of feeding a hot isostatic pressing process designed to deliver the highly durable waste-forms. Following a demonstration of feasibility, flowsheet development is progressing to support the design which has the aim of a fully flexible facility based in NNL's Central Laboratory on the Sellafield site. Optimisation of the size reduction, mixing and blending operations is being carried out using UO{sub 2} as a surrogate for PuO{sub 2}. This work is supporting the potential of using an enhanced glass ceramic formulation in place of the full ceramic with the aim of simplifying glove box operations. Heat treatment and subsequent HIPing strategies are being explored in order to eliminate any carbon from the feeds without increasing the valence state of the uranium present in some of the inventory which can result in an unwanted increase in wasteform volumes. The HIP and ancillary systems are being specifically designed to meet the requirements of the Sellafield site and within the constraints of the NNL Central Laboratory. The HIP is being configured to produce consolidated product cans consistent with the requirements of ongoing storage and disposal. With the aim of one cycle per day, the facility will deliver its mission of immobilising

  16. Comparison of REMIX vs. MOX fuel characteristics in multiple recycling in VVER reactor

    SciTech Connect

    Dekusar, V.M.; Kalashnikov, A.G.; Kapranova, E.N.; Korobitsyn, V.E.; Puzakov, A.Y.

    2013-07-01

    Multiple recycling of regenerated uranium-plutonium fuel in thermal reactors of VVER-1000 type with high enriched uranium feeding (REMIX-fuel) gives a possibility to terminate the accumulation of spent nuclear fuels (SNF) and Pu and decrease the accumulation of irradiated uranium by an order of magnitude. Results of comparison of VVER-1000 nuclear fuel cycle characteristics vs different fuel types such as UOX, MOX and REMIX-fuel have been presented. REMIX fuel (Regenerated Mixture of U-, Pu oxides) is the mixture of plutonium and uranium extracted from SNF and refined from other actinides and fission products with the addition of enriched uranium to provide the power pot