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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, January 1-31, 1983

    SciTech Connect

    Not Available

    1983-03-01

    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.

  4. Pu-238 fuel form activities, January 1-31, 1981

    SciTech Connect

    Not Available

    1981-02-01

    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. 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.

  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 PAGESBeta

    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. Shippingport LWBR (Th/U Oxide) Fuel Characteristics for Disposal Criticality Analysis

    SciTech Connect

    L. L. Taylor; H. H. Loo

    1999-09-01

    Department of Energy (DOE)-owned spent nuclear fuels encompass many fuel types. In an effort to facilitate criticality analysis for these various fuel types, they were categorized into eight characteristic fuel groups with emphasis on fuel matrix composition. Out of each fuel group, a representative fuel type was chosen for analysis as a bounding case within that fuel group. Generally, burnup data, fissile enrichments, and total fuel and fissile mass govern the selection of the representative or candidate fuel within that group. The Shippingport Light Water Breeder Reactor (LWBR) fuels incorporate more of the conventional materials (zirconium cladding/heavy metal oxides) and fabrication details (rods and spacers) that make them comparable to a typical commercial fuel assembly. The LWBR seed/blanket configuration tested a light-water breeder concept with Th-232/U-233 binary fuel matrix. Reactor design used several assembly configurations at different locations within the same core . The seed assemblies contain the greatest fissile mass per (displaced) unit volume, but the blanket assemblies actually contain more fissile mass in a larger volume; the atom-densities are comparable.

  9. 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.

  10. Modeling of constituent redistribution in U Pu Zr metallic fuel

    NASA Astrophysics Data System (ADS)

    Kim, Yeon Soo; Hayes, S. L.; Hofman, G. L.; Yacout, A. M.

    2006-12-01

    A computer model was developed to analyze constituent redistribution in U-Pu-Zr metallic nuclear fuels. Diffusion and thermochemical properties were parametrically determined to fit the postirradiation data from a fuel test performed in the Experimental Breeder Reactor II (EBR-II). The computer model was used to estimate redistribution profiles of fuels proposed for the conceptual designs of small modular fast reactors. The model results showed that the level of redistribution of the fuel constituents of the designs was similar to the measured data from EBR-II.

  11. Method of removing Pu(IV) polymer from nuclear fuel reclaiming liquid

    DOEpatents

    Tallent, Othar K.; Mailen, James C.; Bell, Jimmy T.; Arwood, Phillip C.

    1982-01-01

    A Pu(IV) polymer not extractable from a nuclear fuel reclaiming solution by conventional processes is electrolytically converted to Pu.sup.3+ and PuO.sub.2.sup.2+ ions which are subsequently converted to Pu.sup.4+ ions extractable by the conventional processes.

  12. /sup 238/Pu fuel processes. Quarterly report, January-March 1981

    SciTech Connect

    Folger, R.L.

    1981-09-01

    Recent process development work indicates that the atmosphere (cover gas) in which /sup 238/PuO/sub 2/ granules are sintered is a critical parameter in the production of General-Purpose Heat Source (GPHS) fuel forms. An acceptable feed material for the direct fabrication of /sup 238/PuO/sub 2/ fuel was produced in the SRP HB-Line using a Pu(III) oxalate direct-strike precipitation technique that was developed at SRL.

  13. Gamma densitometer for measuring Pu density in fuel tubes

    SciTech Connect

    Winn, W.G.

    1982-01-01

    A fuel-gamma-densitometer (FGD) has been developed to examine nondestructively the uniformity of plutonium in aluminum-clad fuel tubes at the Savannah River Plant (SRP). The monitoring technique is ..gamma..-ray spectroscopy with a lead-collimated Ge(Li) detector. Plutonium density is correlated with the measured intensity of the 208 keV ..gamma..-ray from /sup 237/U (7d) of the /sup 241/Pu (15y) decay chain. The FGD measures the plutonium density within 0.125- or 0.25-inch-diameter areas of the 0.133- to 0.183-inch-thick tube walls. Each measurement yields a density ratio that relates the plutonium density of the measured area to the plutonium density in normal regions of the tube. The technique was used to appraise a series of fuel tubes to be irradated in an SRP reactor. High-density plutonium areas were initially identified by x-ray methods and then examined quantitatively with the FGD. The FGD reliably tested fuel tubes and yielded density ratios over a range of 0.0 to 2.5. FGD measurements examined (1) nonuniform plutonium densities or hot spots, (2) uniform high-density patches, and (3) plutonium density distribution in thin cladding regions. Measurements for tubes with known plutonium density agreed with predictions to within 2%. Attenuation measurements of the 208-keV ..gamma..-ray passage through the tube walls agreed to within 2 to 3% of calculated predictions. Collimator leakage measurements agreed with model calculations that predicted less than a 1.5% effect on plutonium density ratios. Finally, FGD measurements correlated well with x-ray transmission and fluoroscopic measurements. The data analysis for density ratios involved a small correction of about 10% for ..gamma..-shielding within the fuel tube. For hot spot examinations, limited information for this correction dictated a density ratio uncertainty of 3 to 5%.

  14. 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.

  15. New concept of designing Pu and MA containing fuel for fast reactors

    NASA Astrophysics Data System (ADS)

    Savchenko, A. M.; Konovalov, I. I.; Vatulin, A. V.; Glagovsky, E. M.

    2009-03-01

    New type of metal base fuel element is suggested for fast reactors. Basic approach to fuel element development - separated operations of fabricating uranium meat fuel element and introducing into it Pu or MA dioxides powder, that results in minimizing dust forming operations in fuel element fabrication. According to new fuel element design a framework fuel element having a porous uranium alloy meat is filled with standard PuO 2 powder of <50 μm fractions prepared by pyrochemical or other methods. In this way a high uranium content fuel meat metallurgically bonded to cladding forms a heat conducting framework, pores of which contain PuO 2 powder. Framework fuel element having porous meat is fabricated by capillary impregnation method with the use of Zr eutectic matrix alloys, which provides metallurgical bond between fuel and cladding and protects it from interaction. As compared to MOX fuel the new one features high thermal conductivity, higher uranium content, hence, high conversion ratio does not interact with fuel cladding and is more environmentally clean. Its principle advantage is a simple production process that is easily realized remotely, feasibility of involving high background Pu and MA isotopes into closed nuclear fuel cycle at the minimal influence on environment.

  16. TEM identification of subsurface phases in ternary U-Pu-Zr fuel

    NASA Astrophysics Data System (ADS)

    Aitkaliyeva, Assel; Madden, James W.; Papesch, Cynthia A.; Cole, James I.

    2016-05-01

    Phases and microstructure in as-cast, annealed at 850 °C, and subsequently cooled U-23Pu-9Zr fuel were characterized using scanning and transmission electron microscopy techniques. SEM examination shows formation of three phases in the alloy that were identified in TEM using selective area diffraction pattern analysis: α-Zr globular and elongated δ-UZr2 inclusions and a thick oxide layer formed on top of β-Pu phase, which has been initially assumed to be ζ-(U, Pu). However, further examination of the cross-sectional TEM specimens identified the matrix phases as δ-UZr2, β-Pu, and (U, Zr)ht. Two types of inclusions were observed in the immediate vicinity of the specimen surface and they were consistent with α-Zr and ζ-(U, Pu).

  17. Melting behavior of MgO-based inert matrix fuels containing (Pu,Am)O 2-x

    NASA Astrophysics Data System (ADS)

    Miwa, Shuhei; Sato, Isamu; Tanaka, Kosuke; Hirosawa, Takashi; Osaka, Masahiko

    2010-05-01

    The melting behavior of MgO-based inert matrix fuels containing (Pu,Am)O 2-x ((Pu,Am)O 2-x-MgO fuels) was experimentally investigated. Heat-treatment tests were carried out at 2173 K, 2373 K and 2573 K each. The fuel melted at about 2573 K in the eutectic reaction of the Pu-Am-Mg-O system. The (Pu,Am)O 2-x grains, MgO grains and pores grew with increasing temperature. In addition, Am-rich oxide phases were formed in the (Pu,Am)O 2-x phase by heat-treatment at high temperatures. The melting behavior was compared with behaviors of PuO 2-x-MgO and AmO 2-x-MgO fuels.

  18. /sup 238/Pu fuel form processes. Bimonthly report, November-December 1979

    SciTech Connect

    Folger, R. L.

    1980-11-01

    Progress in the Savannah River Laboratory's /sup 238/Pu Fuel Form Program is summarized. Full-scale fabrication tests continued in the Plutonium Experimental Facility (PEF) with the successful fabrication of seven additional GPHS pellets. Three pellets (GPHS Pellets 14, 15, and 16) were fabricated at off-centerline conditions to help define process limits for production of GPHS fuel pellets in the Plutonium Fuel Fabrication (PuFF) Facility. Two additional limit-test pellets (GPHS Pellets 12 and 13) previously hot pressed underwent final heat treatment. Two pellets (GPHS Pellets 17 and 18) were fabricated at centerline conditions as part of the effort to have Savannah River Laboratory (SRL) GPHS pellets impact tested at LASL. All seven pellets remained integral and demonstrated excellent dimensional stability during final heat treatment. However, the quality of those pellets fabricated at centerline conditions was superior to those that were fabricated as part of the limit tests.

  19. 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.

  20. 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

  1. 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. Between 2004 and 2006, four fuel segments were irradiated, with on-line recording of centerline temperature and rod pressure of the two instrumented rods and intermittent non-destructive hot-cell investigations of the other two non-instrumented rods. At the end of 2006, the instrumented rods were unloaded for hot-cell investigations. The hot-cell investigations reduced uncertainties in the power history to build a reliable and consistent irradiation history which can be used to assess and validate fuel performance codes. The on-line recorded temperatures of the instrumented rods are presented in this paper and are compared to corresponding calculations on the basis of the power history. One of the non-instrumented rods was re-inserted in the reactor in 2012 and attained a peak burnup level of 37 GWd/tHM by the end of 2014. The combined data set of on-line measurements and post irradiation examinations enables further code validation. In this context, the results of the in-house MACROS code of SCK·CEN have been compared with the experimental results. The code contains dedicated (Th,Pu)O2 models for the calculation of the thermal conductivity as a function of the burnup and models that determine the radial power profile within the pellet.

  2. 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.

  3. 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.

  4. 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.

  5. On the oxidation of (U, Pu)C fuel: Experimental and kinetic aspects, practical issues

    NASA Astrophysics Data System (ADS)

    Mazaudier, F.; Tamani, C.; Galerie, A.; Marc, Y.

    2010-11-01

    The oxidation of mixed (U, Pu) carbide fuel was studied to meet some of the general requirements applicable to the back- and front-end of the nuclear fuel cycle. Data are unfortunately scarce in this field. Based on an experimental study and a kinetic treatment, it was proved that the oxidation of solid or powdered mixed carbide fuel does not involve any unwanted kinetic transition and does not have the intrinsic ability to self-sustain. We never observed the formation of a protective oxide layer on the samples. The oxidation products were always low-density, finely-divided oxide powder expanding and tending to slow down the process. The low thermal activation observed demonstrates the key role of gas transport when using powders. Practical solutions have been derived from this work.

  6. High-silicon 238PuO2 fuel characterization study: Half module impact tests

    NASA Astrophysics Data System (ADS)

    Reimus, Mary Ann H.

    1997-01-01

    The General-Purpose Heat Source (GPHS) provides power for space missions by transmitting the heat of 238Pu 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.

  7. /sup 238/Pu fuel form processes bimonthly report, May-June 1979

    SciTech Connect

    Folger, R. L.

    1980-02-01

    Progress in the Savannah River /sup 238/Pu Fuel Form Program is summarized. Full-scale fabrication tests of General-Purpose Heat Source (GPHS) fuel forms continued in the SRL Plutonium Experimental Facility (PEF) as four additional pellets (GPHS Pellets 5-8) were hot pressed. GPHS pellets fabricated by the reference process were dimensionally and structurally stable during and after final heat treatment. Microstructural studies confirmed that centerline GPHS process conditions produce pellets with a homogeneous microstructure and a uniform density. Because of the potential for excessive metal creep in existing furnace racks, the racks were considered unacceptable for GPHS fuel production in the PuFF. To eliminate metal creep, racks containing some ceramic components were designed to operate at 1600/sup 0/C in an oxygen atmosphere for more than 100 h. The four-key variables previously identified (shard sintering temperature, hot press load, hot press temperature, and load ramp) were found to correlate with production sphere fracture tendency and bulk density.

  8. 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.

  9. Applicability of CeO 2 as a surrogate for PuO 2 in a MOX fuel development

    NASA Astrophysics Data System (ADS)

    Kim, Han Soo; Joung, Chang Yong; Lee, Byung Ho; Oh, Jae Yong; Koo, Yang Hyun; Heimgartner, Peter

    2008-08-01

    The applicability of cerium oxide, as a surrogate for plutonium oxide, was evaluated for the fabrication process of a MOX (mixed oxide) fuel pellet. Sintering behavior, pore former effect and thermal properties of the Ce-MOX were compared with those of Pu-MOX. Compacting parameters of the Pu-MOX powder were optimized by a simulation using Ce-MOX powder. Sintering behavior of Ce-MOX was very similar to that of Pu-MOX, in particular for the oxidative sintering process. The sintered density of both pellets was decreased with the same slope with an increasing DA (dicarbon amide) content. Both the Ce-MOX and Pu-MOX pellets which were fabricated by an admixing of 0.05 wt% DA and sintering in a CO 2 atmosphere had the same average grain size of 11 μm and a density of 95%T.D. The thermal conductivity of the Pu-MOX was a little higher than that of the Ce-MOX at a lower temperature but both conductivities became closer to each other above 900 K. Cerium oxide was found to be a useful surrogate to simulate the Pu behavior in the MOX fuel fabrication.

  10. /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.

  11. Thermochemical Analysis of Gas-Cooled Reactor Fuels Containing Am and Pu Oxides

    SciTech Connect

    Lindemer, T.B.

    2002-09-05

    Literature values and estimated data for the thermodynamics of the actinide oxides and fission products are applied to explain the chemical behavior in gas-cooled-reactor fuels. Emphasis is placed on the Am-O-C and Pu-O-C systems and the data are used to plot the oxygen chemical potential versus temperature of solid-solid and solid-gas equilibria. These results help explain observations of vaporization in Am oxides, nitrides, and carbides and provide guidance for the ceramic processing of the fuels. The thermodynamic analysis is then extended to the fission product systems and the Si-C-O system. Existing data on oxygen release (primarily as CO) as a function of burnup in the thoria-urania fuel system is reviewed and compared to values calculated from thermodynamic data. The calculations of oxygen release are then extended to the plutonia and americia fuels. Use of ZrC not only as a particle coating that may be more resistant to corrosion by Pd and other noble-metal fission products, but also as a means to getter oxygen released by fission is discussed.

  12. TRISO-fuel element thermo-mechanical performance modeling for the hybrid LIFE engine with Pu fuel blanket

    NASA Astrophysics Data System (ADS)

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

    2010-10-01

    A TRISO-coated fuel thermo-mechanical performance study is performed for the fusion-fission hybrid Laser Inertial Fusion Engine (LIFE) to test the viability of TRISO particles to achieve ultra-high burn-up of Pu or transuranic spent nuclear fuel blankets. Our methodology includes full elastic anisotropy, time and temperature varying material properties, and multilayer capabilities. In order to achieve fast fluences up to 30 × 10 25 n m -2 ( E > 0.18 MeV), judicious extrapolations across several orders of magnitude of existing material databases have been carried out. The results of our study indicate that failure of the pyrolytic carbon (PyC) layers occurs within the first 2 years of operation. The particles then behave as a single-SiC-layer particle and the SiC layer maintains reasonably-low tensile stresses until the end-of-life. It is also found that 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. Conversely, varying the geometry of the TRISO-coated fuel particles results in little differences in terms of fuel performance.

  13. 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.

  14. 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)

  15. 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

  16. 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.

  17. 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

  18. 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.

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

    DOE PAGESBeta

    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 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

  20. A new fabrication route for SFR fuel using (U, Pu)O2 powder obtained by oxalic co-conversion

    NASA Astrophysics Data System (ADS)

    Vaudez, Stéphane; Belin, Renaud C.; Aufore, Laurence; Sornay, Philippe; Grandjean, Stéphane

    2013-11-01

    The standard powder metallurgy preparation of SFR (Sodium Fast Reactor) oxide fuel involves UO2 and PuO2 co-milling. An alternative route, using a solid-solution of mixed oxide obtained by oxalic co-conversion as the starting material, is presented. It was used to manufacture nuclear fuels for the "COPIX" irradiation conducted in the Phenix SFR. Two processes using co-converted powders were tested to elaborate fuel pellets: (1) the Direct Process that consists in pressing and sintering the mixed oxide with the final Pu content and (2) the Dilution Process, which involves the dilution of a high Pu content mixed oxide with UO2. After studying the structural and microstructural evolution with temperature of these innovative raw materials, the elaboration parameters were adjusted to obtain final pellets in accordance with the Phenix fuel specifications. This study demonstrates the feasibility of such new fabrication route at laboratory scale and, from a more fundamental prospect, allows a better understanding of the underlying phenomena involved during sintering.

  1. 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.

  2. Burnup estimation of fuel sourcing radioactive material based on monitored Cs and Pu isotopic activity ratios in Fukushima N. P. S. accident

    SciTech Connect

    Yamamoto, T.; Suzuki, M.; Ando, Y.

    2012-07-01

    After the severe core damage of Fukushima Dai-Ichi Nuclear Power Station, radioactive material leaked from the reactor buildings. As part of monitoring of radioactivity in the site, measurements of radioactivity in soils at three fixed points have been performed for {sup 134}Cs and {sup 137}Cs with gamma-ray spectrometry and for Pu, Pu, and {sup 240}Pu with {alpha}-ray spectrometry. Correlations of radioactivity ratios of {sup 134}Cs to {sup 137}Cs, and {sup 238}Pu to the sum of {sup 239}Pu and {sup 240}Pu with fuel burnup were studied by using theoretical burnup calculations and measurements on isotopic inventories, and compared with the Cs and Pu radioactivity rations in the soils. The comparison indicated that the burnup of the fuel sourcing the radioactivity was from 18 to 38 GWd/t, which corresponded to that of the fuel in the highest power and, therefore, the highest decay heat in operating high-burnup fueled BWR cores. (authors)

  3. 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).

  4. 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.

  5. 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.

  6. U and Pu Gamma-Ray Measurements of Spent Fuel Using a Gamma-Ray Mirror Band-Pass Filter

    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.; Pivovaroff, M.J.

    2014-01-01

    Abstract. We report on the use of grazing incidence gamma-ray mirrors to serve as a narrow band-pass filter for advanced non-destructive analysis (NDA) of spent nuclear fuel. The purpose of the mirrors is to limit the radiation reaching a HPGe detector to narrow spectral bands around characteristic emission lines from fissile isotopes in the fuel. This overcomes the normal rate issues when performing gamma-ray NDA measurements. In a proof-of-concept experiment, a set of simple flat gamma-ray mirrors were used to directly observe the atomic florescence lines from U and Pu from spent fuel pins with the detector located in a shirt-sleeve environment. The mirrors, consisting of highly polished silicon substrates deposited with WC/SiC multilayer coatings, successfully deflected the lines of interest while the intense primary radiation beam from the fuel was blocked by a lead beam stop. The gamma-ray multilayer coatings that make the mirrors work at the gamma-ray energies used here (~ 100 keV) have been experimentally tested at energies as high as 645 keV, indicating that direct observation of nuclear emission lines from 239Pu should be possible with an appropriately designed optic and shielding configuration.

  7. 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.

  8. 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/.

  9. 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

  10. Effect of oxygen potential on the sintering behavior of MgO-based heterogeneous fuels containing (Pu, Am)O 2-x

    NASA Astrophysics Data System (ADS)

    Miwa, Shuhei; Ishi, Yohei; Osaka, Masahiko

    2009-06-01

    The effect of oxygen potential on the sintering behavior of MgO-based heterogeneous fuels containing (Pu, Am)O 2-x was experimentally investigated. Sintering tests in various atmospheres, i.e. air, moisturized 4%H 2-Ar, and 4%H 2-Ar atmosphere, were carried out. The sintering behavior was found to be significantly affected by the oxygen potential in the sintering atmosphere. The sintered density decreased with decreasing oxygen potential. The (Pu, Am)O 2-x phase sintered in a reductive atmosphere had hypostoichiometry. The aggregates of the (Pu, Am)O 2-x phase sintered in the reductive atmosphere grew, in comparison with those in the oxidizing one. The sintering mechanism was discussed in terms of the difference in sintering behavior of (Pu, Am)O 2-x and MgO.

  11. 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

  12. 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)

  13. /sup 238/Pu fuel form processes. Quarterly report, July-September 1982

    SciTech Connect

    Not Available

    1982-12-01

    Fracture tendency of pellets after final heat treatment or vacuum outgassing during production has been reviewed. A statistical analysis of fracture tendency has revealed a cyclical trend. The period of the cycle on average is about every 50 pellets. Phosphorus is considered detrimental to the impact behavior of iridium. Tests show that phosphorus is easily picked up by PuO/sub 2/ through a variety of pathways and is difficult to remove by heating techniques such as are possible in the PuFF Facility. High-temperature impact ductility of CVS welds may be related to grain structure in the weld centerline. Heating at 1500/sup 0/C causes finely structured thorium-bearing patches on grain surfaces in welds to agglomerate into particles. Heating at 2000/sup 0/C appears to heal grain boundary cavities and pores. High-temperature creep has been identified as another mechanism for producing grain boundary cavities that cause weld-quench cracking. 17 figures, 11 tables.

  14. 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.

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

    SciTech Connect

    Reimus, M.A.

    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. {copyright} {ital 1997 American Institute of Physics.}

  18. 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.

  19. 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)

  20. 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.

  1. 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.

  2. 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.

  3. 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.

  4. 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.

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

    SciTech Connect

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

    2012-07-18

    A key objective of the Next Generation Safeguards Initiative (NGSI) is to evaluate and develop non-destructive assay (NDA) techniques to determine the elemental plutonium content in a commercial-grade nuclear spent fuel assembly (SFA) [1]. Within this framework, we investigate by simulation a novel analytical approach based on combined information from passive measurement of the total neutron count rate of a SFA and its multiplication determined by the active interrogation using an instrument based on a Differential Die-Away technique (DDA). We use detailed MCNPX simulations across an extensive set of SFA characteristics to establish the approach and demonstrate its robustness. It is predicted that Pu content can be determined by the proposed method to a few %.

  6. 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}.

  7. 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.

  8. 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.

  9. Thermochemical Assessment of Oxygen Gettering by SiC or ZrC in PuO2-x TRISO Fuel

    SciTech Connect

    Besmann, Theodore M

    2010-01-01

    Particulate nuclear fuel in a modular helium reactor is being considered for the consumption of excess plutonium and related transuranics. In particular, efforts to largely consume transuranics in a single-pass will require the fuel to undergo very high burnup. This deep burn concept will thus make the proposed plutonia TRISO fuel particularly likely to suffer kernel migration where carbon in the buffer layer and inner pyrolytic carbon layer is transported from the high temperature side of the particle to the low temperature side. This phenomenon is oberved to cause particle failure and therefore must be mitigated. The addition of SiC or ZrC in the oxide kernel or in a layer in communication with the kernel will lower the oxygen potential and therefore prevent kernel migration, and this has been demonstrated with SiC. In this work a thermochemical analysis was performed to predict oxygen potential behavior in the plutonia TRISO fuel to burnups of 50% FIMA with and without the presence of oxygen gettering SiC and ZrC. Kernel migration is believed to be controlled by CO gas transporting carbon from the hot side to the cool side, and CO pressure is governed by the oxygen potential in the presence of carbon. The gettering phases significantly reduce the oxygen potential and thus CO pressure in an otherwise PuO2-x kernel, and prevent kernel migration by limiting CO gas diffusion through the buffer layer. The reduction in CO pressure can also reduce the peak pressure within the particles by ~50%, thus reducing the likelihood of pressure-induced particle failure. A model for kernel migration was used to semi-quantitatively assess the effect of controlling oxygen potential with SiC or ZrC and did demonstrated the dramatic effect of the addition of these phases on carbon transport.

  10. Next Generation Safeguards Initiative research to determine the Pu mass in spent fuel assemblies: Purpose, approach, constraints, implementation, and calibration

    NASA Astrophysics Data System (ADS)

    Tobin, S. J.; Menlove, H. O.; Swinhoe, M. T.; Schear, M. A.

    2011-10-01

    The Next Generation Safeguards Initiative (NGSI) of the U.S. Department of Energy has funded a multi-lab/multi-university collaboration to quantify the plutonium mass in spent nuclear fuel assemblies and to detect the diversion of pins from them. The goal of this research effort is to quantify the capability of various non-destructive assay (NDA) technologies as well as to train a future generation of safeguards practitioners. This research is "technology driven" in the sense that we will quantify the capabilities of a wide range of safeguards technologies of interest to regulators and policy makers; a key benefit to this approach is that the techniques are being tested in a unified manner. When the results of the Monte Carlo modeling are evaluated and integrated, practical constraints are part of defining the potential context in which a given technology might be applied. This paper organizes the commercial spent fuel safeguard needs into four facility types in order to identify any constraints on the NDA system design. These four facility types are the following: future reprocessing plants, current reprocessing plants, once-through spent fuel repositories, and any other sites that store individual spent fuel assemblies (reactor sites are the most common facility type in this category). Dry storage is not of interest since individual assemblies are not accessible. This paper will overview the purpose and approach of the NGSI spent fuel effort and describe the constraints inherent in commercial fuel facilities. It will conclude by discussing implementation and calibration of measurement systems. This report will also provide some motivation for considering a couple of other safeguards concepts (base measurement and fingerprinting) that might meet the safeguards need but not require the determination of plutonium mass.

  11. Fuel/cladding compatibility in high-burnup U-19Pu-10Zr/HT9-clad fuel at elevated temperatures

    SciTech Connect

    Cohen, A.B.; Tsai, H.; Neimark, L.A.

    1992-11-01

    This paper summarizes the most recent results of a continuing experimental effort to study compatibility issues of irradiated metallic fuel and cladding at elevated temperatures that may be encountered beyond those of nominal steady-state conditions.

  12. Disposition of weapon-grade plutonium with pebble bed type HTGRs using Pu burner balls and Th breeder balls

    SciTech Connect

    Yamashita, Kiyonobu; Tokuhara, Kazumi; Fujimoto, Nozomu; Kunitomi, Kazuhiko

    1996-08-01

    A concept of reactor system was developed with which weapons-grade plutonium could be made perfectly worthless in use for weapons. It is a pebble bed type HTGR using Pu burner ball fuels and Th breeder ball fuels. The residual amounts of {sup 239}Pu in spent Pu balls become less than 1% of the initial loading. Furthermore, a method was found that the power coefficient could be made negative by heavy Pu loading in the Pu burner ball fuels.

  13. 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 two-part manual describes and provides instructions for installing software for Lawrence Livermore National Laboratory's Pu-238 isotopic analysis system built for Westinghouse Hanford's Radioisotope Power Systems Facility. Part 1 contains descriptions of all the subroutines found in the main software program, WHC.ASY238. Also provided in this part are general instructions for modifying a subroutine and specific directions for relinking the WHC.ASY238 program, as well as information on the supporting program PU238.CHNG. Part 2 contains listings of the Pu-238 isotopic analysis system codes. The system uses a large (20% rel. efficiency), coaxial, n-type germanium detector (COAX). Parameter files for the detector have filenames with IS8 extensions. Spectral data files also have WH8 and I01, I02, etc. filename extensions.

  14. The crystal structure of ianthinite, [U 24+(UO 2) 4O 6(OH) 4(H 2O) 4](H 2O) 5: a possible phase for Pu 4+ incorporation during the oxidation of spent nuclear fuel

    NASA Astrophysics Data System (ADS)

    Burns, Peter C.; Finch, Robert J.; Hawthorne, Frank C.; Miller, Mark L.; Ewing, Rodney C.

    1997-10-01

    Ianthinite, [U 24+(UO 2) 4O 6(OH) 4(H 2O) 4](H 2O) 5, is the only known uranyl oxide hydrate mineral that contains U 4+, and it has been proposed that ianthinite may be an important Pu 4+-bearing phase during the oxidative dissolution of spent nuclear fuel. The crystal structure of ianthinite, orthorhombic, a = 0.7178(2), b = 1.1473(2), c = 3.039(1) nm, V = 2.5027 nm 3Z = 4, space group P2 1cn, has been solved by direct methods and refined by least-squares methods to an R index of 9.7% and a wR index of 12.6% using 888 unique observed [| F| ≥ 5 σ | F|] reflections. The structure contains both U 4+. The U 6+ cations are present as roughly linear (U 6+O 2) 2+ uranyl ion (Ur) that are in turn coordinated by five O 2- and OH - located at the equatorial positions of pentagonal bipyramids. The U 4+ cations are coordinated by O 2-, OH - and H 2O in a distorted octahedral arrangement. The Ur φ5and U 4+| 6 (φ: O 2-, OH -, H 2O) polyhedra l sharing edges to for two symmetrically distinct sheets at z ≈ 0.0 and z ≈ 0.25 that are parallel to (001). The sheets have the β-U 3O 8 sheet anion-topology. There are five symmetrically distinct H 2O groips located at z ≈ 0.125 between the sheets of U φn polyhedra, and the sheets of U φn polyhedra are linked together only by hydrogen bonding to the intersheet H 2O groups. The crystal-chemical requirements of U 4+ and Pu 4+ are very similar, suggesting that extensive Pu 4+ ↔ U 4+ substitution may occur within the sheets of U φn polyhedra in trh structure of ianthinine.

  15. 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.

  16. On the electrochemical formation of Pu-Al alloys in molten LiCl-KCl

    NASA Astrophysics Data System (ADS)

    Mendes, E.; Malmbeck, R.; Nourry, C.; Souček, P.; Glatz, J.-P.

    2012-01-01

    Properties of Pu-Al alloys were investigated in connection with development of pyrochemical methods for reprocessing of spent nuclear fuel. Electroseparation techniques in molten LiCl-KCl are being developed in ITU to group-selectively recover actinides from the mixture with fission products. In the process, actinides are electrochemically reduced on solid aluminium cathodes, forming solid actinide-aluminium alloys. This article is focused on electro-chemical characterisation of Pu-Al alloys in molten LiCl-KCl, on electrodeposition of Pu on solid Al electrodes and on determination of chemical composition and structure of the formed alloys. Cyclic voltammetry and chronopotentiometry were used to study Pu-Al alloys in the temperature range 400-550 °C. Pu is reduced to metal in one reduction step Pu 3+/Pu 0 on an inert W electrode. On a reactive Al electrode, the reduction of Pu 3+ to Pu 0 occurs at a more positive potential due to formation of Pu-Al alloys. The open circuit potential technique was used to identify the alloys formed. Stable deposits were obtained by potentiostatic electrolyses of LiCl-KCl-PuCl 3 melts on Al plates. XRD and SEM-EDX analyses were used to characterise the alloys, which were composed mainly of PuAl 4 with some PuAl 3. In addition, the preparation of PuCl 3 containing salt by carbochlorination of PuO 2 is described.

  17. 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

  18. 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

  19. Pu(V) and Pu(IV) sorption to montmorillonite.

    PubMed

    Begg, James D; Zavarin, Mavrik; Zhao, Pihong; Tumey, Scott J; Powell, Brian; Kersting, Annie B

    2013-05-21

    Plutonium (Pu) adsorption to and desorption from mineral phases plays a key role in controlling the environmental mobility of Pu. Here we assess whether the adsorption behavior of Pu at concentrations used in typical laboratory studies (≥10(-10) [Pu] ≤ 10(-6) M) are representative of adsorption behavior at concentrations measured in natural subsurface waters (generally <10(-12) M). Pu(V) sorption to Na-montmorillonite was examined over a wide range of initial Pu concentrations (10(-6)-10(-16) M). Pu(V) adsorption after 30 days was linear over the wide range of concentrations studied, indicating that Pu sorption behavior from laboratory studies at higher concentrations can be extrapolated to sorption behavior at low, environmentally relevant concentrations. Pu(IV) sorption to montmorillonite was studied at initial concentrations of 10(-6)-10(-11) M and was much faster than Pu(V) sorption over the 30 day equilibration period. However, after one year of equilibration, the extent of Pu(V) adsorption was similar to that observed for Pu(IV) after 30 days. The continued uptake of Pu(V) is attributed to a slow, surface-mediated reduction of Pu(V) to Pu(IV). Comparison between rates of adsorption of Pu(V) to montmorillonite and a range of other minerals (hematite, goethite, magnetite, groutite, corundum, diaspore, and quartz) found that minerals containing significant Fe and Mn (hematite, goethite, magnetite, and groutite) adsorbed Pu(V) faster than those which did not, highlighting the potential importance of minerals with redox couples in increasing the rate of Pu(V) removal from solution. PMID:23614502

  20. 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.

  1. 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.

  2. 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

  3. 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.

  4. 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

  5. Preliminary Simulations for Geometric Optimization of a High-Energy Delayed Gamma Spectrometer for Direct Assay of Pu in Spent Nuclear Fuel

    SciTech Connect

    Kulisek, Jonathan A.; Campbell, Luke W.; Rodriguez, Douglas C.

    2012-06-07

    High-energy, beta-delayed gamma-ray spectroscopy is under investigation as part of the Next Generation Safeguard Initiative effort to develop non-destructive assay instruments for plutonium mass quantification in spent nuclear fuel assemblies. Results obtained to date indicate that individual isotope-specific signatures contained in the delayed gamma-ray spectra can potentially be used to quantify the total fissile content and individual weight fractions of fissile and fertile nuclides present in spent fuel. Adequate assay precision for inventory analysis can be obtained using a neutron generator of sufficient strength and currently available detection technology. In an attempt to optimize the geometric configuration and material composition for a delayed gamma measurement on spent fuel, the current study applies MCNPX, a Monte Carlo radiation transport code, in order to obtain the best signal-to-noise ratio. Results are presented for optimizing the neutron spectrum tailoring material, geometries to maximize thermal or fast fissions from a given neutron source, and detector location to allow an acceptable delayed gamma-ray signal while achieving a reasonable detector lifetime while operating in a high-energy neutron field. This work is supported in part by the Next Generation Safeguards Initiative, Office of Nuclear Safeguards and Security, National Nuclear Security Administration.

  6. 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. PMID:22420016

  7. 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

  8. 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.

  9. Formation of Pu amorphous alloys or metastable structures in Pu-Fe, Pu-Ta, and Pu-Si alloys

    SciTech Connect

    Rizzo, H.F.; Echeverria, A.W.

    1985-08-20

    Sputter deposition technique was used to study the possible formation of amorphous structures in Pu-Fe, Pu-Ta, and Pu-Si systems. A triode sputtering system was used to prepare sputtered coatings: 13 to 59 at. % (a/o) Fe, 10 to 50 a/o Si, and 15 to 65 a/o Ta. Structure of the coatings was determined by x-ray diffraction techniques. The temperature stability of the obtained structures was determined by Differential Scanning Calorimetry (DSC) measurements. The Pu-Fe and Pu-Si binary systems showed strong evidence for the formation of amorphous phases in the sputtered coatings. X-ray analyses indicated the presence of Pu6Fe in the 13 to 20 a/o Fe range of Pu-Fe alloys and no apparent crystalline phases over the entire 10 to 50 a/o Si range of Pu-Si alloys. In the Pu-Ta system, the DSC data obtained for compositions below 50 a/o Ta did not show typical crystallization exotherms. At compositions above 50 a/o Ta, a metastable bcc alpha Ta structure was observed with an expanded lattice parameter. The calculated volume expansion (2.9%) corresponds to 29 a/o of Pu in solid solution if the lattice parameter is assumed to follow Vegards Law. After storage in a nitrogen glovebox atmosphere for over two years, the Pu-Si and Pu-Ta coatings have maintained a metallic luster and have shown no visible evidence of surface oxidation.

  10. 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. PMID:21911246

  11. Elastic properties of Pu metal and Pu-Ga alloys

    SciTech Connect

    Soderlind, P; Landa, A; Klepeis, J E; Suzuki, Y; Migliori, A

    2010-01-05

    We present elastic properties, theoretical and experimental, of Pu metal and Pu-Ga ({delta}) alloys together with ab initio equilibrium equation-of-state for these systems. For the theoretical treatment we employ density-functional theory in conjunction with spin-orbit coupling and orbital polarization for the metal and coherent-potential approximation for the alloys. Pu and Pu-Ga alloys are also investigated experimentally using resonant ultrasound spectroscopy. We show that orbital correlations become more important proceeding from {alpha} {yields} {beta} {yields} {gamma} plutonium, thus suggesting increasing f-electron correlation (localization). For the {delta}-Pu-Ga alloys we find a softening with larger Ga content, i.e., atomic volume, bulk modulus, and elastic constants, suggest a weakened chemical bonding with addition of Ga. Our measurements confirm qualitatively the theory but uncertainties remain when comparing the model with experiments.

  12. 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

  13. Designing Pu600 for Authentication

    SciTech Connect

    White, G

    2008-07-10

    Many recent Non-proliferation and Arms Control software projects include an authentication component. Demonstrating assurance that software and hardware performs as expected without hidden 'back-doors' is crucial to a project's success. In this context, 'authentication' is defined as determining that the system performs only its intended purpose and performs that purpose correctly and reliably over many years. Pu600 is a mature software solution for determining the presence of Pu and the ratio of Pu240 to Pu239 by analyzing the gamma ray spectra in the 600 KeV region. The project's goals are to explore hardware and software technologies which can by applied to Pu600 which ease the authentication of a complete, end-to-end solution. We will discuss alternatives and give the current status of our work.

  14. Magnetic Properties of Radiation Damage in Pu and Pu Alloys

    SciTech Connect

    McCall, S; Fluss, M J; Chung, B; Chapline, G; McElfresh, M; Jackson, D; Baclet, N; Jolly, L; Dormeval, M

    2005-03-31

    Among the many exceptional properties of Pu is its apparent lack of either local moments or cooperative magnetism. Lashley et al., have recently noted that little experimental evidence for the existence of local moments or collective magnetism has been found in over 50 years. Nevertheless the search for local moments in Pu and Pu-alloys continues, why? Plutonium's physical properties: resistance, magnetic susceptibility, and heat capacity, all support a system with an enhanced electron density of states. Pu sits on the edge of both magnetism and superconductivity and possesses one of the highest elemental Pauli susceptibilities, consistent with a highly correlated electron system. The low-density {delta}-Pu has eluded full first principles description and is both a challenge and an area of active investigation for theorists. The complex changes associated with the transition between the light and heavy actinides happen within the phase diagram of Pu, thus making Pu an intriguing and challenging solid-state system for continuing experimental and theoretical investigation. Recently, Griveau et al., observed the variations in the resistance and superconducting properties of Am metal as a function of pressure to 27GPa and T>0.4K. They postulate that the interesting features in the superconducting critical temperature, T{sub c}, vs. pressure, indicate a Mott-like, f-electron localization-delocalization transition as pressure drives Am towards a Pu and then a U-like structure. Hence, we posit that it would be reasonable to expect that dilating the Pu lattice will bring one to a similar transition. Experimental evidence supporting this point of view is given here.

  15. 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

  16. 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.

  17. 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

  18. 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.

  19. Overview of advanced technologies for stabilization of 238Pu-contaminated waste

    NASA Astrophysics Data System (ADS)

    Ramsey, Kevin B.; Foltyn, Elizabeth M.; Heslop, J. Mark

    1998-01-01

    This paper presents an overview of potential technologies for stabilization of 238Pu-contaminated waste. Los Alamos National Laboratory (LANL) has processed 238PuO2 fuel into heat sources for space and terrestrial uses for the past several decades. The 88-year half-life of 238Pu 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 238Pu attractive for heat source applications, the high Curie content (17 Ci/gram versus 0.06 Ci/gram for 239Pu), makes disposal of 238Pu-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 238Pu-contaminated glovebox waste. Use of advanced waste treatment technologies including Molten Salt Oxidation (MSO) and aqueous chemical separation will eliminate the combustible matrix from 238Pu-contaminated waste and recover kilogram quantities of 238PuO2 from the waste stream. A conceptual design of these advanced waste treatment technologies will be presented.

  20. Eleven-year field study of Pu migration from Pu III, IV, and VI sources.

    PubMed

    Kaplan, Daniel I; Demirkanli, Deniz I; Gumapas, Leo; Powell, Brian A; Fjeld, Robert A; Molz, Fred J; Serkiz, Steven M

    2006-01-15

    Understanding the processes controlling Pu mobility in the subsurface environment is important for estimating the amount of Pu waste that can be safely disposed in vadose zone burial sites. To study long-term Pu mobility, four 52-L lysimeters filled with sediment collected from the Savannah River Site near Aiken, South Carolina were amended with well-characterized solid Pu sources (PuIIICl3, PuIV(NO3)4, PuIV(C2O4)2, and PuVIO2(NO3)2) and left exposed to natural precipitation for 2-11 years. Pu oxidation state distribution in the Pu(III) and Pu(IV) lysimeters sediments (a red clayey sediment, pH = 6.3) were similar, consisting of 0% Pu(III), >92% Pu(IV), 1% Pu(V), 1% Pu(VI), and the remainder was a Pu polymer. These three lysimeters also had near identical sediment Pu concentration profiles, where >95% of the Pu remained within 1.25 cm of the source after 11 years; the other 5% of Pu moved at an overall rate of 0.9 cm yr(-1). As expected, Pu moved more rapidly through the Pu(VI) lysimeter, at an overall rate of 12.5 cm yr(-1). Solute transport modeling of the sediment Pu concentration profile data in the Pu(VI) lysimeter indicated that some transformation of Pu into a much less mobile form, presumably Pu(IV), had occurred during the course of the two-year study. This modeling also supported previous laboratory measurements showing that Pu(V) or Pu(VI) reduction was 5 orders of magnitude faster than corresponding Pu(III) or Pu(IV) oxidation. The slow oxidation rate (1 x 10(-8) hr(-1); t1/2 = 8000 yr) was not discernible from the Pu(VI) lysimeter data that reflected only two years of transport butwas readily discernible from the Pu(III) and Pu(IV) lysimeter data that reflected 11 years of transport. PMID:16468387

  1. 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. PMID:24401459

  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. Calculated k-effectives for light water reactor typical, U + Pu nitrate solution critical experiments

    SciTech Connect

    Primm, R.T. III; Mincey, J.F.

    1982-01-01

    The Department of Energy's Consolidated Fuel Reprocessing Program has as a goal the design of nuclear fuel reprocessing equipment. In order to validate computer codes used for criticality analyses in the design of such equipment, k-effectives have been calculated for several U + Pu nitrate solution critical experiments. As of January 1981, descriptions of 45 unpoisoned, U + Pu solution experiments were available in the open literature. Twelve of these experiments were performed with solutions which have physical characteristics typical of dissolved, light water reactor fuel. This paper contains a discussion of these twelve experiments, a review of the calculational procedure used to determine k-effectives, and the results of the calculations.

  4. 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.

  5. 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

    2012-11-01

    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. PMID:23016948

  6. 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.

  7. Distinguishing Pu Metal From Pu Oxide Using Fast Neutron Counting

    SciTech Connect

    Verbeke, J M; Chapline, G F; Nakae, L; Wurtz, R; Sheets, S

    2012-05-29

    We describe a method for simultaneously determining the {alpha}-ratio and k{sub eff} for fissile materials using fast neutrons. Our method is a generalization of the Hage-Cifarrelli method for determining k{sub eff} for fissile assemblies which utilizes the shape of the fast neutron spectrum. In this talk we illustrate the method using Monte Carlo simulations of the fast neutrons generated in PuO{sub 2} to calculate the fast neutron spectrum and Feynman correlations.

  8. 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).

  9. 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.

  10. 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

  11. Plutonium Immobilization Task 5.6 Metal Conversion: Milestone Report - Perform Feasibility Demonstrations on Pu-Al Alloys

    SciTech Connect

    Zundelevich, Y; Kerns, J; Bannochie, C

    2001-04-12

    The Plutonium Conversion Task within the Plutonium Immobilization Program (PIP) transforms incoming plutonium (Pu) feed materials into an oxide acceptable for blending with ceramic precursors. One of the feed materials originally planned for PIP was unirradiated fuel, which consisted mainly of the Zero Power Plutonium Reactor (ZPPR) fuel. Approximately 3.5 metric tons of Pu is in ZPPR fuel. The ZPPR fuel is currently stored at the Argonne National Laboratory-West as stainless steel clad metal plates and oxide pellets, with the vast majority of the Pu in the metal plates. The metal plates consist of a Pu-U-Mo alloy (containing 90% of the ZPPR plutonium metal) and a Pu-Al alloy (containing 10% of the ZPPR plutonium metal). The Department of Energy (DOE) decided that ZPPR fuel is a national asset and, therefore, not subject to disposition. This report documents work done prior to that decision. The Hydnde-Oxidation (HYDOX) Process was selected as the method for Metal Conversion in PIP because it provides a universal means for preparing oxide from all feed materials. HYDOX incorporates both the hydride process, originally developed to separate Pu from other pit materials, as well as the oxide formation step. Plutonium hydride is very reactive and is readily converted to either the nitride or the oxide. A previous feasibility study demonstrated that the Pu-U-Mo alloy could be successfully converted to oxide via the HYDOX Process. Another Metal Conversion milestone was to demonstrate the feasibility of the HYDOX Process for converting plutonium-aluminum (Pu-Al) alloy in ZPPR fuel plates to an acceptable oxide. This report documents the results of the latter feasibility study which was performed before the DOE decision to retain ZPPR fuel rather than immobilize it.

  12. Interception and retention of /sup 238/Pu deposition by orange trees

    SciTech Connect

    Pinder, J.E. III; Adriano, D.C.; Ciravolo, T.G.; Doswell, A.C.; Yehling, D.M.

    1987-06-01

    Radioisotope thermoelectric generators (RTG) transform the heat produced during the alpha decay of /sup 238/Pu into electrical energy for use by deep-space probes, such as the Voyager spacecraft, which have returned images and other data from Jupiter, Saturn and Uranus. Future missions involving RTGs may be launched aboard the space shuttle, and there is a remote possibility that an explosion of liquid-hydrogen and liquid-oxygen fuel could rupture the RTGs and disperse /sup 238/Pu into the atmosphere over central Florida. Research was performed to determine the potential transport to man of atmospherically dispersed Pu via contaminated orange fruits. The results indicate that the major contamination of oranges would result from the interception and retention of /sup 238/Pu deposition by fruits. The resulting surface contamination could enter human food chains through transfer to internal tissues during peeling or in the reconstituted juices and flavorings made from orange skins. The interception of /sup 238/Pu deposition by fruits is especially important because the results indicate no measurable loss of Pu from fruit surfaces through time or with washing. Approximately 1% of the /sup 238/Pu deposited onto an orange grove would be harvested in the year following deposition.

  13. 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.

  14. Characterization of Pu-238 heat source granule containment

    SciTech Connect

    Richardson Ii, P D; Thronas, D L; Romero, J P; Sandoval, F E; Neuman, A D; Duncan, W S

    2008-01-01

    The Milliwatt Radioisotopic Thermoelectric Generator (RTG) provides power for permissive-action links. These nuclear batteries convert thermal energy to electrical energy using a doped silicon-germanium thermopile. The thermal energy is provided by a heat source made of {sup 238}Pu, in the form of {sup 238}PuO{sub 2} granules. The granules are contained in 3 layers of encapsulation. A thin T-111 liner surrounds the {sup 238}PuO{sub 2} granules and protects the second layer (strength member) from exposure to the fuel granules. The T-111 strength member contains the fuel under impact condition. An outer clad of Hastelloy-C protects the T-111 from oxygen embrittlement. The T-111 strength member is considered the critical component in this {sup 238}PuO{sub 2} containment system. Any compromise in the strength member is something that needs to be characterized. Consequently, the T-111 strength member is characterized upon it's decommissioning through Scanning Electron Microscopy (SEM), and Metallography. SEM is used in 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 photomicrographs. SEM may further be used to examine polished Metallography mounts to characterize elements using the SEM mode of Energy Dispersive X-ray Spectroscopy (EDS). This paper describes the characterization of the metallurgical condition of decommissioned RTG heat sources.

  15. 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.

  16. 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.

  17. 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.

  18. Characterization of high-fired PuO/sub 2/ as a certified reference material

    SciTech Connect

    Legeled, M.A.; Cacic, C.G.; Crawford, D.W.; Spaletto, M.I.

    1984-07-01

    The New Brunswick Laboratory (NBL), U.S. Department of Energy, has certified a plutonium dioxide reference material, CRM 122, for plutonium assay and isotopic composition. The PuO/sub 2/ standard, one of several certified Pu reference materials currently being developed at NBL for use in instrumentation calibration and measurement control for safeguards, establishes traceability to the national measurement base. This plutonium reference material in the oxide form provides more directly demonstrable traceability than metal because it undergoes the same chemical treatment for dissolution as PuO/sub 2/ fuel materials. Various tests for achieving a constant weight and for dissolving CRM 122 high-fired PuO/sub 2/ were conducted. Results of these tests as well as the certification data generated by controlled-potential coulometry for plutonium assay and by thermal ionization mass spectrometry for isotopic composition will also be presented and discussed.

  19. 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.

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

    SciTech Connect

    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.

    2005-02-06

    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.

  1. 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.

  2. Probing the Pu4 + magnetic moment in PuF4 with 19F NMR spectroscopy

    NASA Astrophysics Data System (ADS)

    Capan, Cigdem; Dempsey, Richard J.; Sinkov, Sergey; McNamara, Bruce K.; Cho, Herman

    2016-06-01

    The magnetic fields produced by Pu4 + centers have been measured by 19F NMR spectroscopy to elucidate the Pu-F electronic interactions in polycrystalline PuF4. Spectra acquired at applied fields of 2.35 and 7.05 T reveal a linear scaling of the 19F line shape. A model is presented that treats the line broadening and shifts as due to dipolar fields produced by Pu valence electrons in localized noninteracting orbitals. Alternative explanations for the observed line shape involving covalent Pu-F bonding, superexchange interactions, and electronic configurations with enhanced magnetic moments are considered.

  3. MGA Analysis on Elevated 238 Pu Samples

    NASA Astrophysics Data System (ADS)

    Wang, T. F.; Moody, K. J.; Raschke, K. E.; Ruhter, W. D.

    2002-10-01

    Plutonium gamma-ray data analysis, in the 100-keV region, using MGA has been improved to overcome the original maximum limit of 2% 238Pu relative plutonium content in a sample in order to perform an analysis. MGA analysis results of elevated 238Pu samples are compared to the results from mass spectrometry.

  4. 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.

  5. Traits of bulk Pu phases in Pb-Pu superlattice phases from first principles

    NASA Astrophysics Data System (ADS)

    Rudin, Sven P.

    2007-11-01

    Density functional theory calculations allowing spin polarization predict two phases in Pb-Pu superlattices. One phase exhibits bond lengths similar to bulk α-Pu and a degree of localization of 5f electron states corresponding to bulk β-Pu , while for the other phase, these take on values like those found in bulk δ-Pu . The superlattice geometry localizes the 5f electron states mainly in planes perpendicular to the stacking direction. The disparate volumes between phases found in bulk Pu also emerge in Pb-Pu superlattices. The structures of the two phases differ in the presence of pairing between neighboring Pu planes. The paired and unpaired phases can coexist in special cases. The simple geometry of the pairing allows for detailed calculations to explore the transition along the complete path connecting the two phases; to date, the bulk phases have evaded such an examination. In Pb-Pu superlattices, the localization of 5f electron states smoothly parallels changes in geometry, in accordance with tendencies that emerge in bulk Pu calculations. Changing the layer thicknesses affects the ordering of the energies of the two phases for stacking along the (001) and (111) directions. For stacking in the (011) direction, only one phase appears with very weakly paired Pu planes. Compared to bulk Pb and Pu, the superlattices with single-monolayer thicknesses appear energetically favorable; pilot calculations suggest that thicker layers become energetically favorable with interface alloying.

  6. Characterization and testing of a {sup 238}Pu loaded ceramic waste form.

    SciTech Connect

    Johnson, S. G.

    1998-04-24

    This paper will describe the preparation and progress of the effort at Argonne National Laboratory-West to produce ceramic waste forms loaded with {sup 238}Pu. The purpose of this study is to determine the extent of damage, if any, that alpha decay events will play over time to the ceramic waste form under development at Argonne. The ceramic waste form is glass-bonded sodalite. The sodalite is utilized to encapsulate the fission products and transuranics which are present in a chloride salt matrix which results from a spent fuel conditioning process. {sup 238}Pu possesses approximately 250 times the specific activity of {sup 239}Pu and thus allows for a much shorter time frame to address the issue. In preparation for production of {sup 238}Pu loaded waste forms {sup 239}Pu loaded samples were produced. Data is presented for samples produced with typical reactor grade plutonium. X-ray diffraction, scanning electron micrographs and durability test results will be presented. The ramifications for the production of the {sup 238}Pu loaded samples will be discussed.

  7. Structural Investigation of (U0.7Pu0.3)O2-x Mixed Oxides.

    PubMed

    Vigier, Jean-François; Martin, Philippe M; Martel, Laura; Prieur, Damien; Scheinost, Andreas C; Somers, Joseph

    2015-06-01

    Uranium-plutonium mixed oxide containing 30% of plutonium is a candidate fuel for several fast neutron and accelerator driven reactor systems. In this work, a detailed structural investigation on sol-gel synthesized stoichiometric U0.7Pu0.3O2.00 and substoichiometric U0.7Pu0.3O2-x, using X-ray diffraction (XRD), oxygen 17 magic angle spinning nuclear magnetic resonance ((17)O MAS NMR) and X-ray absorption spectroscopy is described. As observed by XRD, the stoichiometric U0.7Pu0.3O2.00 is monophasic with a lattice parameter in good agreement with Vegard's law, while the substoichiometric U0.7Pu0.3O2-x material is biphasic. Solid solution ideality in terms of a random distribution of metal atoms is proven for U0.7Pu0.3O2.00 with (17)O MAS NMR. X-ray absorption near-edge structure (XANES) spectroscopy shows the presence of plutonium(III) in U0.7Pu0.3O2-x. Extended X-ray absorption fine-structure (EXAFS) spectroscopy indicates a similar local structure around both cations, and comparison with XRD indicates a close similarity between uranium and plutonium local structures and the long-range ordering. PMID:25984750

  8. 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.

  9. Preparation and characterization of (Pu, U, Np, Am, simulated FP) O2-X

    NASA Astrophysics Data System (ADS)

    Morimoto, K.; Kato, M.; Uno, H.; Hanari, A.; Tamura, T.; Sugata, H.; Sunaoshi, T.; Kono, S.

    2005-02-01

    The development of low decontaminated mixed oxide (MOX) fuel, which contains minor actinoides (MA) and fission products (FP), is in progress to established Advanced Fast Reactor (FR) Fuel Cycle system. This paper describes the study on the sintering characteristics and the physical properties of MOX fuel containing Am, Np, and simulated FP. MOX powder containing Am, Np and simulated FP were sintered at high temperature in various oxygen partial pressure. From the result of ceramography, it is found that the grain growth rate of the pellets sintered in high oxygen partial pressure is high. From the result of EPMA analysis (Pu, Am, Ln) oxide was observed in the pellets. The melting points of the pellets with oxygen to metal (O/M) ratio of 1.95 are higher than those with O/M ratio of 1.98. This tendency is similar to that of MOX fuel containing about 30% Pu.

  10. Room-temperature electron spectroscopy of 239Pu and 240Pu

    NASA Astrophysics Data System (ADS)

    Ahmad, I.; Kondev, F. G.; Greene, J. P.; Zhu, S.

    2015-06-01

    Passivated, implanted, planar silicon (PIPS) detectors have been used for the measurement of electron spectra. The commercially available PIPS detectors, available in thicknesses of 100 μm, 300 μm, and 500 μm, have an energy resolution (FWHM) of ~ 2.2 keV, which is essentially the same as that of PIN diodes. Alpha and electron spectra of mass-separated 239Pu and 240Pu sources have been measured with a 300-μm thick PIPS detector and the electron to alpha ratios for the conversion lines of the 51.62- and 45.24-keV transitions have been determined. A procedure has been developed to determine the amount of 239Pu and 240Pu in a mixed source. The α-particle emission rate of the mixed source is measured, which is the sum of individual rates. From the electron spectrum of the mixed source, measured with the same setup as the alpha spectrum, the rates of 239Pu electron lines are determined. Using the electron rate of the 239Pu line and the electron to alpha ratio measured for the pure source, the α-particle emission rate of 239Pu is determined. The difference from the total α-particle emission rate gives the α-particle emission rate of 240Pu. In addition, electron intensities and conversion coefficients of the 239Pu and 240Pu transitions have been measured.

  11. [Pu(IV) behavior in the serum].

    PubMed

    Surova, Z I

    1984-01-01

    This paper presents the results of studies of the hydrolysis and polymerization of Pu(IV) in blood serum. With nitrite Pu(IV) solutions incubated with blood serum 20-34% of the nuclide were precipitated as hydroxide and 11-36% converted into polymeric forms bound by high molecular weight proteins. For citrate solutions, these values were 3.8 and 3.0%, respectively. PMID:6505160

  12. 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.

  13. 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.

  14. 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.

  15. Chemically selective polymer substrate based direct isotope dilution alpha spectrometry of Pu.

    PubMed

    Paul, Sumana; Pandey, Ashok K; Shah, R V; Aggarwal, S K

    2015-06-01

    Quantification of actinides in the complex environmental, biological, process and waste streams samples requires multiple steps like selective preconcentration and matrix elimination, solid source preparations generally by evaporation or electrodeposition, and finally alpha spectrometry. To minimize the sample manipulation steps, a membrane based isotope dilution alpha spectrometry method was developed for the determination of plutonium concentrations in the complex aqueous solutions. The advantages of this method are that it is Pu(IV) selective at 3M HNO3, high preconcentration factor can be achieved, and obviates the need of solid source preparation. For this, a thin phosphate-sulfate bifunctional polymer layer was anchored on the surface of microporous poly(ethersulfone) membrane by UV induced surface grafting. The thickness of the bifunctional layer on one surface of the poly(ethersulfone) membrane was optimized. The thickness, physical and chemical structures of the bifunctional layer were studied by secondary ionization mass spectrometry (SIMS), scanning electron microscopy (SEM) and SEM-EDS (energy-dispersive spectroscopy). The optimized membrane was used for preconcentration of Pu(IV) from aqueous solutions having 3-4M HNO3, followed by direct quantification of the preconcentrated Pu(IV) by isotope dilution alpha spectrometry using (238)Pu spike. The chemical recovery efficiency of Pu(IV) was found to be 86±3% below Pu(IV) loading capacity (1.08 μg in 2×1 cm(2)) of the membrane sample. The experiments with single representative actinides indicated that Am(III) did not sorb to significant extent (7%) but U(VI) sorbed with 78±3% efficiency from the solutions having 3M HNO3 concentration. However, Pu(IV) chemical recovery in the membrane remained unaffected from the solution containing 1:1000 wt. proportion of Pu(IV) to U(VI). Pu concentrations in the (U, Pu)C samples and in the irradiated fuel dissolver solutions were determined. The results thus obtained

  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). PMID:27337652

  17. 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.

  18. Neutron-diffraction study of PuAs and PuSb

    NASA Astrophysics Data System (ADS)

    Burlet, P.; Quezel, S.; Rossat-Mignod, J.; Spirlet, J. C.; Rebizant, J.; Müller, W.; Vogt, O.

    1984-12-01

    The first neutron scattering experiments on PuAs and PuSb single crystals are reported. PuAs is found to be a ferromagnet below Tc=123+/-1 K. PuSb develops below TN=85+/-1 K an incommensurate ordering and undergoes, at TIC=67 K, a first-order transition to a commensurate phase, ferromagnetic in nature. In both compounds, moments are perpendicular to the ferromagnetic (001) planes, their low-temperature value is μ=(0.75+/-0.1)μB, indicating a Γ8-type ground state within the Russell-Saunders level scheme. The magnetic phase diagram of PuSb has been determined. The incommensurate phase is suppressed by a small field of 8.5 kOe.

  19. 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.

  20. Prompt fission γ -ray spectrum characteristics from 240Pu(sf ) and 242Pu(sf )

    NASA Astrophysics Data System (ADS)

    Oberstedt, S.; Oberstedt, A.; Gatera, A.; Göök, A.; Hambsch, F.-J.; Moens, A.; Sibbens, G.; Vanleeuw, D.; Vidali, M.

    2016-05-01

    In this paper we present first results for prompt fission γ -ray spectra (PFGS) characteristics from the spontaneous fission (sf) of 240Pu and 242Pu. For 242Pu(sf ) we obtained, after proper unfolding of the detector response, an average energy per photon ɛ¯γ=(0.843 ±0.012 ) MeV, an average multiplicity M¯γ=(6.72 ±0.07 ) , and an average total γ -ray energy release per fission E¯γ ,tot = (5.66 ± 0.06) MeV. The 240Pu(sf ) emission spectrum was obtained by applying a so-called detector-response transformation function determined from the 242Pu spectrum measured in exactly the same geometry. The results are an average energy per photon ɛ¯γ=(0.80 ±0.07 ) MeV, the average multiplicity M¯γ = (8.2 ± 0.4), and an average total γ -ray energy release per fission E¯γ ,tot = (6.6 ± 0.5) MeV. The PFGS characteristics for 242Pu(sf ) are in very good agreement with those from thermal-neutron-induced fission on 241Pu and scales well with the corresponding prompt neutron multiplicity. Our results in the case of 240Pu(sf ), although drawn from a limited number of events, show a significantly enhanced average multiplicity and average total energy, but may be understood from a different fragment yield distribution in 240Pu(sf ) compared to that of 242Pu(sf ).

  1. MCSNA: Experimental Benchmarking of Pu Electronic Structure

    SciTech Connect

    Tobin, J G

    2007-01-29

    The objective of this work is to develop and/or apply advanced diagnostics to the understanding of aging of Pu. Advanced characterization techniques such as photoelectron and x-ray absorption spectroscopy will provide fundamental data on the electronic structure of Pu phases. These data are crucial for the validation of the electronic structure methods. The fundamental goal of this project is to narrow the parameter space for the theoretical modeling of Pu aging. The short-term goal is to perform experiments to validate electronic structure calculations of Pu. The long-term goal is to determine the effects of aging upon the electronic structure of Pu. Many of the input parameters for aging models are not directly measurable. These parameters will need to be calculated or estimated. Thus a First Principles-Approach Theory is needed, but it is unclear what terms are important in the Hamiltonian. (H{Psi} = E{Psi}) Therefore, experimental data concerning the 5f electronic structure are needed, to determine which terms in the Hamiltonian are important. The data obtained in this task are crucial for reducing the uncertainty of Task LL-01-developed models and predictions. The data impact the validation of electronic structure methods, the calculation of defect properties, the evaluation of helium diffusion, and the validation of void nucleation models. The importance of these activities increases if difficulties develop with the accelerating aging alloy approach.

  2. 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)

  3. Spectroscopy of Neutron-rich Pu Nuclei

    SciTech Connect

    Chowdhury, P.; Hota, S.; Lakshmi, S.; Tandel, S. K.; Harrington, T.; Jackson, E.; Moran, K.; Shirwadkar, U.; Ahmad, I.; Carpenter, M. P.; Greene, J.; Hoffman, C. R.; Janssens, R. V. F.; Khoo, T. L.; Kondev, F. G.; Lauritsen, T.; Lister, C. J.; McCutchan, E. A.; Seweryniak, D.; Stefanescu, I.

    2011-10-28

    Spectroscopic studies of nuclei in the A{approx}250, Z{approx}100 region provide critical input to theoretical models that attempt to describe the structure and stability of the heaviest elements. We report here on new spectroscopic studies in the N = 150,151 nuclei {sup 244,245}Pu. (Z = 94). Excitations in these nuclei on the neutron-rich side of the valley of stability, accessed via inelastic and transfer reactions, complement fusion-evaporation studies of Z{>=}100 nuclei. States in {sup 244,245}Pu were populated using {sup 47}Ti and {sup 208}Pb beams incident on a {sup 244}Pu target, with delayed and prompt gamma rays detected by the Gammasphere array. The new results are discussed in the context of emerging systematics of one- and two-quasiparticle excitations in N{>=}150 nuclei.

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

    NASA Astrophysics Data System (ADS)

    Chamizo, E.; García-León, M.; Peruchena, J. I.; Cereceda, F.; Vidal, V.; Pinilla, E.; Miró, C.

    2011-12-01

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

  5. 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.

  6. 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.

  7. 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.

  8. Nitrate anion exchange in 238Pu aqueous scrap recovery operations

    NASA Astrophysics Data System (ADS)

    Pansoy-Hjelvik, M. E.; Silver, G. L.; Reimus, M. A. H.; Ramsey, K. B.

    1999-01-01

    Strong base, nitrate anion exchange (IX) is crucial to the purification of 238Pu solution feedstocks with gross levels of impurities. This paper discusses the work involved in bench scale experiments to optimize the nitrate anion exchange process. In particular, results are presented of experiments conducted to a) demonstrate that high levels of impurities can be separated from 238Pu solutions via nitrate anion exchange and, b) work out chemical pretreatment methodology to adjust and maintain 238Pu in the IV oxidation state to optimize the Pu(IV)-hexanitrato anionic complex sorption to Reillex-HPQ resin. Additional experiments performed to determine the best chemical treatment methodology to enhance recovery of sorbed Pu from the resin and VIS-NIR absorption studies to determine the steady state equilibrium of Pu(IV), Pu(III), and Pu(VI) in nitric acid are discussed.

  9. 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

  10. 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).

  11. 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.

  12. Investigation of single crystal zircon, (Zr,Pu)SiO4 doped with Pu

    NASA Astrophysics Data System (ADS)

    Hanchar, J. M.; Burakov, B. E.; Anderson, E. B.; Zamoryanskaya, M. V.

    2003-04-01

    Zircon-based ceramics are under consideration as durable waste forms for immobilization of weapons grade plutonium and other actinide elements. Samples of polycrystalline zircon doped with 238Pu and 239Pu have been obtained in previous studies. These materials, however, are difficult to use for precise measurement of the leach-rate of Pu, and to accurately determine the level of Pu doping that can be attained in zircon, (Zr,Pu)SiO_4. Single crystals of 238Pu doped zircon (ranging from 0.3 to 3.5 mm in size) were successfully grown for the first time ever using a Li-Mo flux synthesis method. The incorporation of Pu ranged from 1.9 to 4.7 wt. % el. (with approximately 81 wt.% of 238Pu isotope) based on electron microprobe analysis. The zircon crystals were pinkish-brown when they were crystallized, and then over a period of five months changed to a brown color. After fourteen months the crystals turned to a brown-gray color. The zircon crystals glow in the dark probably from alpha particle induced luminescence. The intensity of the cathodoluminescence (CL) emission in the Pu doped crystals is correlated with the Pu content, and the CL emission showed no change 141 days after the initial CL measurements were made. Single crystal X-ray diffraction results obtained 141 days after synthesis indicate unit cell parameters (in angstroms): a = 6.6267(15), c = 5.9992(10) and a cell volume of 263.41(10). When the zircon crystals were grown, they were free of cracks. Over the course of five months cracks appeared throughout the crystals, and after fourteen months the cracks became much more abundant. The zircon crystals were transparent upon crystallization, and even with numerous cracks throughout the crystals remain transparent. Radiation damage calculations indicate that after only a short period of time, six months, these zircon crystals had already accumulated significant alpha-induced radiation damage (˜2.5 x1014 alpha-decay events per milligram). After five years they

  13. 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.

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

    SciTech Connect

    Chung, B W; Schwartz, A J; Ebbinghaus, B B; Fluss, M J; Haslam, J J; Blobaum, K M; Tobin, J G

    2005-04-15

    Resonant Photoemission, a variant of Photoelectron Spectroscopy, has been demonstrated to have sensitivity to aging of Pu samples. The spectroscopic results are correlated with resistivity measurements and are shown to be the fingerprint of mesoscopic or nanoscale internal damage in the Pu physical structure. This means that a spectroscopic signature of internal damage due to aging in Pu has been established.

  15. Prediction of thermodynamic property of Pu-zircon and Pu-pyrochlore

    NASA Astrophysics Data System (ADS)

    Xu, Hulfang; Wang, Yifeng

    2000-07-01

    Due to its high durability, zircon is often present as a heavy mineral in natural environments and is the oldest mineral that has been dated on the earth. There are four zircon structure phases of M4+SiO4 occurring in nature: zircon (ZrSiO4), hafnon (HfSiO4), thorite (ThSiO4), and coffinite (USiO4). These phases may form solid solution. Recent interest in zircon minerals stems from the study of highly durable radioactive waste forms. Crystalline phases of M4+SiO4 with zircon structure have been proposed as a durable ceramic waste form for immobilizing actinides such as Pu, Np, and U. To predict the behavior of zircon-based waste forms in a geologic repository environment as well as to optimize the fabrication of those waste forms, the thermodynamic and kinetic properties for zircon mineral phases have to be determined. In this paper, we use a linear free energy relationship to predict the Gibbs free energies of formation of Pu-bearing phases (Xu et al., 1999). The calculated results show that the PuSiO4 phase with zircon structure is unstable with respect to oxides of PuO2 and quartz. However, the PuSiO4 phase will be stable with respect to oxides of PuO2 and silica glass at low temperature.

  16. 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.

  17. 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

  18. 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.

  19. Electrochemical behaviors of PuN and (U, Pu)N in LiCl KCl eutectic melts

    NASA Astrophysics Data System (ADS)

    Shirai, O.; Kato, T.; Iwai, T.; Arai, Y.; Yamashita, T.

    2005-02-01

    Electrochemical behaviors of PuN and (U, Pu)N in the LiCl KCl eutectic melts at 773 K were investigated by cyclic voltammetry. The electrochemical dissolution of PuN and (U, Pu)N began nearly at -0.90±0.05 and -0.95±0.05 V (vs. Ag+/Ag), respectively. The rest potentials of PuN and (U, Pu)N were observed at about 0.15 V more negative potential than that of UN, in the present experimental condition. The observed rest potentials of (U, Pu)N depended on the equilibrium potential of the Pu3+/PuN. In the cyclic voltammogram measured by use of (U, Pu)N as the working electrode, a steep rise of the positive current was observed at potentials more positive than -0.45 V in analogy with the cyclic voltammogram measured by use of UN as the working electrode. These indicate that UN and PuN in (U, Pu)N would be dissolved independently irrespective of forming the solid solution.

  20. Redox reactions of Pu(IV) and Pu(III) in the presence of acetohydroxamic acid in HNO(3) solutions.

    PubMed

    Tkac, Peter; Precek, Martin; Paulenova, Alena

    2009-12-21

    The reduction of Pu(IV) in the presence of acetohydroxamic acid (HAHA) was monitored by vis-NIR spectroscopy. All experiments were performed under low HAHA/Pu(IV) ratios, where only the Pu(IV)-monoacetohydroxamate complex and Pu uncomplexed with HAHA were present in relevant concentrations. Time dependent concentrations of all absorbing species were resolved using molar extinction coefficients for Pu(IV), Pu(III), and the Pu(AHA)(3+) complex by deconvolution of spectra. From fitting of the experimental data by rate equations integrated by a numeric method three reactions were proposed to describe a mechanism responsible for the reduction and oxidation of plutonium in the presence of HAHA and HNO(3). Decomposition of Pu(AHA)(3+) follows a second order reaction mechanism with respect to its own concentration and leads to the formation of Pu(III). At low HAHA concentrations, a two-electron reduction of uncomplexed Pu(IV) with HAHA also occurs. Formed Pu(III) is unstable and slowly reoxidizes back to Pu(IV), which, at the point when all HAHA is decomposed, can be catalyzed by the presence of nitrous acid. PMID:19904974

  1. 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.

  2. Preliminary studies of Pu measurement by AMS using PuF4-

    NASA Astrophysics Data System (ADS)

    Zhao, X.-L.; Kieser, W. E.; Dai, X.; Priest, N. D.; Kramer-Tremblay, S.; Eliades, J.; Litherland, A. E.

    2013-01-01

    Using targets made with PbF2 matrices, Cs+ sputter sources have been found to yield element-specific patterns of molecular fluoride anions that may be used to enhance the mass spectrometry of certain elements. While the patterns are found similar for all lanthanides and the heavier actinides, substantial differences are found for the lighter actinides. In the case of Pu and U, of all their fluoride anions, PuF4- and UF5- are produced with the highest yield. Mass spectrometry of Pu using PuF4- can provide a partial chemical separation in the ion source, as the yield of UF4- is two orders of magnitude lower than that of the UF5-. This, in turn, reduces scattering of U ions when measuring Pu in the high-energy components of the AMS system. This instrumental reduction of U is advantageous in cases that require rapid Pu analyses as it simplifies the chemistry of Pu/U separation and other steps in the sample processing. In this procedure, Pu can be co-precipitated with another element as a fluoride, which is then mixed with a sufficient amount of PbF2 powder to form a sputter target. A series of tests were carried out and NdF3 was identified as one such suitable carrier. Measurements of Pu+3 at ∼0.85 MV terminal voltage showed that the 239,240,241,242Pu isotopes can be detected with a manageably low background, high efficiency and a 1 fg detection limit. Preliminary tests were carried out using the existing IsoTrace AMS system, modified only by the addition of electronic controls to automatically adjust the terminal voltage and all high-energy electric analyzers, along with the injection magnet bouncer. However, both the injection and detection systems were not designed for this task, so considerable room is available for reducing the detection limit into the ag range with modern AMS systems - such as the one being commissioned at University of Ottawa.

  3. 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.

  4. Self-irradiation of Pu, its alloys and compounds

    NASA Astrophysics Data System (ADS)

    Timofeeva, L. F.

    2000-07-01

    Self-irradiation of Pu, its alloys and compounds by products of known α-decomposition is a continuous complicated process, which includes numerous different phenomena. The accumulation of Pu decomposition products causes material structure and properties change. This problem is the subject of many works, most of them concerned with the behavior of Pu and its alloys at low (liquid He and N) temperatures. The survey is given of the results of our experiments connected with radiogenic helium behavior, crystal structure and properties of Pu metallic compounds and Pu oxide ceramics in a self-irradiation process at room temperature under isochronal heat treatments.

  5. 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.

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

    DOEpatents

    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.

  7. Parametric Studies on Plutonium Transmutation Using Uranium-Free Fuels in Light Water Reactors

    SciTech Connect

    Shelley, Afroza; Akie, Hiroshi; Takano, Hideki; Sekimoto, Hiroshi

    2000-08-15

    To compare the once-through use of U-free fuels for plutonium burnup in light water reactors (LWRs), plutonium transmutation, minor actinide (MA) and long-life fission product (LLFP) buildup and radiotoxicity hazards were compared for PuO{sub 2} + ZrO{sub 2} (rock-like oxide: ROX) and PuO{sub 2} + ThO{sub 2} (thorium oxide: TOX) fuels, loaded in a soft-to-hard neutron spectrum LWR core (a moderator-to-fuel volume ratio V{sub m}/V{sub f} is from 0.5 to 3.0). For better understanding and proper improvement of the reactivity coefficient problem of ROX, the fuel temperature coefficient, the void coefficient, and the delayed neutron fraction were also studied. A mixed-oxide (MOX)-fueled LWR was considered for reference purposes.From the result of the cell burnup calculation, ROX fuel transmutes 90% of net initially loaded weapons-grade Pu, and 2.5% of initially loaded Pu is converted to MAs when V{sub m}/V{sub f} is 2.0 and discharge burnup in effective full-power days is equivalent to that of 33 GWd/t in MOX fuel. Reactor-grade Pu-based ROX fuel transmutes 80% of net initially loaded Pu, and 6.7% of initially loaded Pu converts to MAs with the same condition as the weapons-grade Pu ROX fuel. TOX fuel also has a good Pu transmutation capability, but the {sup 233}U production amount is approximately a half of the fissile Pu transmutation amount. The MA production amount in TOX fuel is lower than that in MOX and ROX fuels. The LLFP production amount in ROX fuel is lower than that in MOX and TOX fuels. The radiotoxicity hazard of ROX spent fuel is lower compared to that in TOX and MOX spent fuels.The thermal neutron energy region is important in ROX fuel for fuel temperature coefficient and void coefficient problems. From these calculations, 15 to 20% {sup 232}Th-added ROX fuel seems the best to use as a once-through Pu-burning fuel compared to TOX and MOX fuels in conventional LWRs, because of its higher Pu transmutation, lower radiotoxicity hazard.

  8. 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.

  9. Search for higher oxides of Pu: A photoemission study

    NASA Astrophysics Data System (ADS)

    Gouder, T.; Seibert, A.; Havela, L.; Rebizant, J.

    2007-07-01

    After decades of believing in a very stable PuO 2, suitable for final storage of nuclear waste, the existence of a higher oxide, PuO 2+ x, was recently claimed. This would have far reaching consequences on the strategies of storage of Pu-based waste. Its formation therefore has been discussed controversially for several years. In this work, existence and stability of the higher oxide, PuO 2+ x, has been probed by photoelectron spectroscopy study of PuO 2 exposed to atomic oxygen. The validity of this approach is first tested on UO 2, which oxidizes readily to UO 3. Under the same reaction conditions, PuO 2 is only covered by a chemisorbed layer of oxygen, which desorbs at elevated temperature. The study excludes the stability of any higher binary Pu oxide as a bulk species.

  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. PMID:16049580

  11. 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

  12. 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.

  13. 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. PMID:24601520

  14. Effect of cross-link density and hydrophilicity of PU on blood compatibility of hydrophobic PS/hydrophilic PU IPNs.

    PubMed

    Roh, H W; Song, M J; Han, D K; Lee, D S; Ahn, J H; Kim, S C

    1999-01-01

    To investigate the effect of the hydrophilic and hydrophobic microdomain structure on blood compatibility, a series of interpenetrating polymer networks (IPNs) composed of hydrophilic polyurethane (PU) and hydrophobic polystyrene (PS) was prepared. One series was prepared with varying cross-link densities of each network, the other with varying hydrophilicity of the PU component. All PU/PS IPNs exhibited microphase-separated structures that had dispersed PS domains in the continuous PU matrix. The domain size decreased with decreasing the hydrophilicity of the PU component and increasing the cross-link density of each network. As the cross-link density and hydrophobicity of the PU component was increased, an inward shift of Tgs was observed, which was due to the decrease in phase separation between the hydrophobic PS component and hydrophilic PU component. In the in vitro platelet adhesion test, as the microdomain size of PU/PS IPN surface decreased, the number of adhered platelets on the PU/PS IPN surface was reduced and deformation of the adhered platelets decreased. It could be concluded that blood compatibility of PU/PS IPN was mainly affected by the degree of mixing between PU and PS component, which was reflected by the domain size of PS rich phase. PMID:10091927

  15. Optical properties of PuO2 and α-Pu2O3 by GGA + U + QA studies

    NASA Astrophysics Data System (ADS)

    Yang, Yu; Lu, Yong; Zhang, Ping

    2014-09-01

    By performing first-principles calculations plus quasi-annealing simulations, we systematically study the ground-state electronic and optical properties for PuO2 and α-Pu2O3. We find that α-Pu2O3 has an energy band gap of 1.38 eV. Our obtained atomic and electronic structures for the two plutonium oxides are in agreement with available experimental as well as other theoretical results. Based on the ground-state electronic structures, we systematically calculate the frequency dependent dielectric functions, as well as the optical spectra for α-Pu2O3 and PuO2. It is found that at the visible light frequency range, the adsorption coefficient of α-Pu2O3 and PuO2 are similar, but their refractive indexes differ much. This difference can be used to detect or trace the oxidation products of the plutonium surfaces.

  16. Progress of nitride fuel cycle research for transmutation of minor actinides

    SciTech Connect

    Arai, Yasuo; Akabori, Mitsuo; Minato, Kazuo

    2007-07-01

    Recent progress of nitride fuel cycle research for transmutation of MA is summarized. Preparation of MA-bearing nitride pellets, such as (Np,Am)N, (Am,Pu)N and (Np,Pu,Am,Cm)N, was carried out. Irradiation behavior of U-free nitride fuel was investigated by the irradiation test of (Pu,Zr)N and PuN+TiN fuels, in which ZrN and TiN were added as a possible diluent material. Further, pyrochemical process of spent nitride fuel was developed by electrorefining in a molten chloride salt and subsequent re-nitridation of actinides in liquid Cd cathode electro-deposits. Nitride fuel cycle for transmutation of MA has been demonstrated in a laboratory scale by the experimental study with MA and Pu. (authors)

  17. Electronic Structure Calculations of delta-Pu Based Alloys

    SciTech Connect

    Landa, A; Soderlind, P; Ruban, A

    2003-11-13

    First-principles methods are employed to study the ground-state properties of {delta}-Pu-based alloys. The calculations show that an alloy component larger than {delta}-Pu has a stabilizing effect. Detailed calculations have been performed for the {delta}-Pu{sub 1-c}Am{sub c} system. Calculated density of Pu-Am alloys agrees well with the experimental data. The paramagnetic {yields} antiferromagnetic transition temperature (T{sub c}) of {delta}-Pu{sub 1-c}Am{sub c} alloys is calculated by a Monte-Carlo technique. By introducing Am into the system, one could lower T{sub c} from 548 K (pure Pu) to 372 K (Pu{sub 70}Am{sub 30}). We also found that, contrary to pure Pu where this transition destabilizes {delta}-phase, Pu{sub 3}Am compound remains stable in the antiferromagnetic phase that correlates with the recent discovery of a Curie-Weiss behavior of {delta}-Pu{sub 1-c}Am{sub c} at c {approx} 24 at. %.

  18. Speciation and unusual reactivity in PuO2+x.

    PubMed

    Conradson, Steven D; Begg, Bruce D; Clark, David L; Den Auwer, Christophe; Espinosa-Faller, Francisco J; Gordon, Pamela L; Hess, Nancy J; Hess, Ryan; Keogh, D Webster; Morales, Luis A; Neu, Mary P; Runde, Wolfgang; Tait, C Drew; Veirs, D Kirk; Villella, Phillip M

    2003-06-16

    Pu L(3) XAFS measurements show that the excess oxygen in single phase PuO(2+)(x)() occurs as oxo groups with Pu-O distances of 1.83-1.91 A. This distance and the energy of the edge (via comparison with a large number of related compounds) are more consistent with a Pu(IV/V) than a Pu(IV/VI) mixture. Analogous to Pu(IV) colloids, although the Pu-Pu pair distribution remains single site even when it shows substantial disorder, the Pu-O distribution can display a number of additional shells at specific distances up to 3.4 A even in high fired materials when no oxo groups are present, implying intrinsic H(+)/OH(-)(/H(2)O). The number of oxo atoms increases when samples are equilibrated with humid air at ambient temperature, indicating that the Pu reactivity in this solid system differs notably from that of isolated complexes and demonstrating the importance of nanoscale cooperative phenomena and total free energy in determining its chemical properties. PMID:12793805

  19. 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.

  20. 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.

  1. 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.

  2. 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)

  3. Materials compatibility for 238Pu-HNO3/HF solution containment: 238Pu aqueous processing

    NASA Astrophysics Data System (ADS)

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

    2000-07-01

    The Power Source Technologies Group at Los Alamos National Laboratory is building a 238Pu Aqueous Scrap Recovery Line at the Plutonium Facility. The process line incorporates several unit operations including dissolution, filtration, ion exchange, and precipitation. During 1997-1999, studies were carried out to determine the chemistry used in the full-scale process. Other studies focussed on the engineering design of the operation. Part of the engineering design was to determine, in compatibility studies, the materials for reaction and storage vessels which will contain corrosive 238Pu-HNO3/HF solutions. The full-scale line is to be operational by the end of year 2000.

  4. 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.

  5. 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. PMID:26656430

  6. Characterization of a Pu-bearing zirconolite-rich synroc

    SciTech Connect

    Buck, E.C.; Ebbinghaus, B.; Bakel, A.J.; Bates, J.K.

    1996-12-31

    A titanate-based ceramic waste form, rich in phases structurally related to zirconolite (CaZrTi{sub 2}O{sub 7}), is being developed as a possible method for immobilizing excess plutonium from dismantled nuclear weapons. As part of this program, Lawrence Livermore National Laboratory (LLNL) produced several ceramics that were then characterized at Argonne National Laboratory (ANL). The plutonium- loaded ceramic was found to contain a Pu-Gd zirconolite phase but also contained plutonium titanates, Gd-polymignyte, and a series of other phases. In addition, much of the Pu was remained as PuO{sub 2- x}. The Pu oxidation state in the zirconolite was determined to be mainly Pu{sup 4+}, although some Pu{sub 3+} was believed to be present.

  7. 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).

  8. 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)

  9. 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.

  10. Effect of equilibration time on Pu desorption from goethite

    DOE PAGESBeta

    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 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

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

    NASA Astrophysics Data System (ADS)

    Klimczuk, T.; Shick, A. B.; Kozub, A. L.; Griveau, J.-C.; Colineau, E.; Falmbigl, M.; Wastin, F.; 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 TN = 44 K, whereas ferromagnetic ordering was found for NpBC below TC = 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.

  12. 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.

  13. Free energy of formation of Cs 3PuCl 6 and CsPu 2Cl 7

    NASA Astrophysics Data System (ADS)

    Williamson, M. A.; Kleinschmidt, P. D.

    The free energy, enthalpy and entropy of formation of the compounds Cs 3PuCl 6 and CsPu 2Cl 7 have been determined by measuring the sublimation pressures for the reactions CsCl( s) / aiCsCl( g), {2}/{5}Cs 3PuCl 6(s) /ai {1}/{5}CsPu 2Cl 7(s) + CsCl(g) , and CsPu2Cl7( s) / ai 2 PuCl3( s) + CsCl( g). The pressures are measured using Knudsen effusion mass spectrometry over the temperature range 600 to 850 K. For the formation of Cs 3PuCl 6 from CsCl and PuCl 3, ΔG0298 = -77.3 ± 8.5 kJ/ mol, ΔH0298 = -82.1 ± 7.8 kJ/ mol, and ΔS0298 = -16.2 ± 10.9 J/ Kmol. For CsPu 2Cl 7, ΔG0298 = -39.4 ± 3.5 kJ/ mol, ΔH0298 = -40.8 ± 3.2 kJ/ mol, and ΔS0298 = -4.6 ± 4.2 J/ Kmol.

  14. STYPu fuel form activities, March 1-September 30, 1985

    SciTech Connect

    Not Available

    1986-01-01

    The SRP portion of this report summarizes production STYPuO2 fuel forms for use in radioisotopic thermoelectric generators (RTG's) in the Plutonium Fuel Form (PuFF) Facility at the Savannah River Plant. The PuFF Facility began producing iridium-encapsulated, 62.5-watt STYPuO2 right circular cylinders for GPHS (General Purpose Heat Source) RTG's in June 1980; this program was completed in December 1983. The PuFF Facility has been placed in a production readiness mode of operation pending funding of additional heat source programs.

  15. Is Octavalent Pu(VIII) Possible? Mapping the Plutonium Oxyfluoride Series PuO(n)F(8-2n) (n = 0-4).

    PubMed

    Huang, Wei; Pyykkö, Pekka; Li, Jun

    2015-09-01

    While the oxidation state Pu(VIII) is shown to be less stable than Pu(V) in the PuO4 molecule, it is not clear if the more electronegative fluorine can help to stabilize Pu(VIII). Our calculations on PuO(n)F(8-2n) (n = 0-4) molecules notably confirm that PuO2F4 has both (1)D(4h) and (5)C(2v) minima with the oxidation states Pu(VIII) and Pu(V), respectively, with the latter having lower energy. The hybrid-DFT, CCSD(T), and CASSCF methods all give the same result. The results conform to a superoxide ligand when n ≥ 2. PuF8 in a (1)O(h) state can decompose to PuF6 and F2, and PuOF6 in a (1)C(2v) state also can break down to PuF6 and 1/2 O2. The Pu(VIII) anion PuO2F5(-) does have a D(5h) minimum, which also lies above a (5)C(2v) Pu(V) peroxide structure. However, the energy differences between the different minima are not large, indicating that metastable species with oxidation states higher than Pu(V) cannot be completely excluded. PMID:26309065

  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. Pu-238 production at the Savannah River Plant

    SciTech Connect

    Roggenkamp, P.L.

    1987-11-01

    Pu-238 production capability at SRP is dependent on the availability of Np-237 feed material. With continuing operation of three production reactors at SRP, production of 46 kg Pu-238 per year can be sustained. Capacity of auxiliary facilities is adequate to support the production rates.

  18. 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

  19. 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.

  20. The environmental dependence of redox energetics of PuO2 and α-Pu2O3: A quantitative solution from DFT+U

    NASA Astrophysics Data System (ADS)

    Sun, Bo; Liu, Haifeng; Song, Haifeng; Zhang, Guangcai; Zheng, Hui; Zhao, Xiangeng; Zhang, Ping

    2012-08-01

    We report a comprehensive density functional theory (DFT)+U study of the energetics of charged and neutral oxygen defects in both PuO2 and α-Pu2O3, and present a quantitative determination of the equilibrium compositions of reduced PuO2 (PuO2 - x) as functions of environmental temperature and partial pressure of oxygen, which shows fairly agreement with corresponding high-temperature experiments. Under ambient conditions, the endothermic reduction of PuO2 to α-Pu2O3 is found to be facilitated by accompanying volume expansion of PuO2 - x and the possible migration of O-vacancy, whereas further reduction of α-Pu2O3 is predicted to be much more difficult. In contrast to the endothermic oxidation of PuO2, the oxidation of α-Pu2O3 is a stable exothermic process.

  1. 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.

  2. 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.

  3. 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.

  4. 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

  5. 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.

  6. 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.

  7. 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.

  8. 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.

  9. 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.

  10. 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. PMID:24274785

  11. Internal Corrosion Analysis of Model 9975 Packaging Containing Pu or PuO{sub 2} During Shipping and Storage

    SciTech Connect

    Vormelker, P.

    1999-03-23

    The Materials Consultation Group of SRTC has completed an internal corrosion analysis of the Model 9975 packaging assembly containing either Pu or PuO2 for storage in K Reactor under ambient conditions for a period of 12 years. The 12-year storage period includes two years for shipping and up to ten years for storage.

  12. 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.

  13. Fragment mass and kinetic energy distributions for /sup 242/Pu(sf), /sup 241/Pu(n/sub th/,f), and /sup 242/Pu(. gamma. ,f)

    SciTech Connect

    Thierens, H.; Jacobs, E.; D'hondt, P.; De Clercq, A.; Piessens, M.; De Frenne, D.

    1984-02-01

    Energy correlation measurements were performed for the spontaneous fission of /sup 242/Pu, the thermal-neutron-induced fission of /sup 241/Pu, and the photofission of /sup 242/Pu with 12-, 15-, 20-, and 30-MeV bremsstrahlung. The photofission cross section for /sup 242/Pu was determined up to 30 MeV. For /sup 242/Pu(sf) the overall kinetic energy distribution is strongly asymmetric and the overall mass distribution has a very high peak yield (9%). Important deviations of the average total kinetic energy release and the average light and heavy fragment masses and from the systematics of Unik et al. are also observed for this fissioning system. These effects can be explained in the framework of the static scission point model by the strong preferential formation of a shell-stabilized scission configuration with the neutron number of the heavy and light fragments in the vicinity of the spherical N = 82 neutron shell and the deformed N = 66 neutron shell, respectively. A decrease of with the average excitation energy , d/d = -0.30 +- 0.04, is observed in the photofission of /sup 242/Pu.

  14. 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. PMID:24531259

  15. Attempt to detect primordial 244Pu on Earth

    NASA Astrophysics Data System (ADS)

    Lachner, Johannes; Dillmann, Iris; Faestermann, Thomas; Korschinek, Gunther; Poutivtsev, Mikhail; Rugel, Georg; Lierse von Gostomski, Christoph; Türler, Andreas; Gerstmann, Udo

    2012-01-01

    With a half-life of 81.1Myr, 244Pu could be both the heaviest and the shortest-lived nuclide present on Earth as a relic of the last supernova(e) that occurred before the formation of the Solar System. Hoffman [Nature (London)NATUAS0028-083610.1038/234132a0 234, 132 (1971)] reported on the detection of this nuclide (1.0×10-18 g 244Pu/g) in the rare-earth mineral bastnäsite with the use of a mass spectrometer. Up to now these findings were never reassessed. We describe the search for primordial 244Pu in a sample of bastnäsite with the method of accelerator mass spectrometry (AMS). It was performed with a highly sensitive setup, identifying the ions by the determination of their time-of-flight and energy. Using AMS, the stripping to high charge states allows the suppression of any molecular interference. During our measurements we observed no event of 244Pu. Therefore, we can give an upper limit for the abundance of 244Pu in our sample of the mineral bastnäsite of 370 atoms per gram (1.5×10-19 g 244Pu/g). The concentration of 244Pu in our sample of bastnäsite is significantly lower than the previously determined value.

  16. Determination of alpha-emitting Pu isotopes in environmental samples.

    PubMed

    Vioque, I; Manjón, G; García-Tenorio, R; El-Daoushy, F

    2002-04-01

    This paper presents an improved radiochemical procedure for the determination of alpha-emitting Pu isotopes in environmental samples (soils, sediments, vegetation) by alpha-particle spectrometry. Quantitative Pu recovery yields were obtained (average 60%), 0.1 mBq being the average minimum detectable activity by the complete technique. Special efforts were made to ensure the removal of traces of different natural alpha-emitting radionuclides, which can interfere with the correct determination of 239+240Pu and 238Pu concentrations. The radiochemical procedure was validated by application to reference material and by participation in intercomparison exercises. This radiochemical procedure was applied to the different layers of a high-resolution sediment core taken from a lake in Sweden. The 239+240Pu and 238Pu/239+240Pu profiles obtained in the high-resolution sediment core correctly reproduced the expected evolution of these quantities as observed historically in the atmosphere, validating the procedure for this purpose and showing the power of these radionuclides for dating purposes. PMID:12022654

  17. Electronic structure and chemical bonding in PuO2

    NASA Astrophysics Data System (ADS)

    Teterin, Yu. A.; Maslakov, K. I.; Teterin, A. Yu.; Ivanov, K. E.; Ryzhkov, M. V.; Petrov, V. G.; Enina, D. A.; Kalmykov, St. N.

    2013-06-01

    Quantitative analysis of the x-ray photoelectron spectra structure in the binding energy (BE) range of 0 eV-˜35 eV for plutonium dioxide (PuO2) valence electrons was done. The BEs and structure of the core electronic shells (35 eV-1250 eV BE), as well as the relativistic discrete variation calculation results for the finite fragments of the PuO2 lattice and the data of other authors, were taken into account. The experimental data show that the many-body effects and the multiplet splitting contribute to the spectral structure much less than the outer (0 eV-˜15 eV) and the inner (˜15 eV-˜35 eV) valence molecular orbitals (OVMO and IVMO, respectively). The filled Pu 5f electronic states were shown to form in the PuO2 valence band. The Pu 6p electrons participate in the formation of both the IVMO and the OVMO (bands). The filled Pu 6p3/2 and the O 2s electronic shells were found to take maximum part in the IVMO formation. The MO composition and the sequence order in the BE range of 0 eV-˜35 eV in PuO2 were established. The experimental and theoretical data allowed a quantitative MO scheme for PuO2, which is fundamental for understanding both the chemical bond nature in plutonium dioxide and the interpretation of other x-ray spectra of PuO2.

  18. 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).

  19. Tissue, cellular, and subcellular distribution of /sup 241/Pu in the rat testes

    SciTech Connect

    Miller, S.C.; Bowman, B.M.

    1983-05-01

    The distribution and localization of /sup 241/Pu in rat testes were determined by quantitative autoradiography. Rats were given intravenous injection of /sup 241/Pu citrate and tissues were collected 1 week later. The tissue distribution of /sup 241/Pu was determined by light microscope autoradiography. Significant concentrations of /sup 241/Pu were observed in the interstitial tissue but not in seminiferous tubules. The cellular distribution and subcellular localization of /sup 241/Pu were determined by electron microscope autoradiography. Within the interstitial tissue, /sup 241/Pu was concentrated in microphages. There was no preferential localization of /sup 241/Pu in any other interstitial tissue components. Within interstitial tissue macrophages, /sup 241/Pu was concentrated in the lysosomal system of the cell. Other organellar compartments of the cell did not preferentially incorporate /sup 241/Pu. The association of /sup 241/Pu with the macrophage lysosomal system may explain the long retention times of Pu in testes as observed in experimental studies.

  20. 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.

  1. An Alternative Model for Electron Correlation in Pu

    SciTech Connect

    Yu, S; Tobin, J; Soderlind, P

    2007-10-23

    Using a density functional theory based approach that treats the 5f electrons relativistically, a Pu electronic structure with zero net magnetic moment is obtained, where the 5f orbital and 5f spin moments cancel each other. By combining the spin and orbital specific densities of states with state, spin and polarization specific transition moments, it is possible to reconstruct the experimentally observed photoemission spectra from Pu. Extrapolating to a spin-resolving Fano configuration, it is shown how this would resolve the extant controversy over Pu electronic structure.

  2. 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.

  3. 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

  4. 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.

  5. Cermet fuel for fast reactor - Fabrication and characterization

    NASA Astrophysics Data System (ADS)

    Mishra, Sudhir; Kutty, P. S.; Kutty, T. R. G.; Das, Shantanu; Dey, G. K.; Kumar, Arun

    2013-11-01

    (U, Pu)O2 ceramic fuel is the well-established fuel for the fast reactors and (U, Pu, Zr) metallic fuel is the future fuel. Both the fuels have their own merits and demerits. Optimal solution may lie in opting for a fuel which combines the favorable features of both fuel systems. The choice may be the use of cermet fuel which can be either (U, PuO2) or (Enriched U, UO2). In the present study, attempt has been made to fabricate (Natural U, UO2) cermet fuel by powder metallurgy route. Characterization of the fuel has been carried out using dilatometer, differential thermal analyzer, X-ray diffractometer, and Scanning Electron Microscope. The results show a high solidus temperature, high thermal expansion, presence of porosities, etc. in the fuel. The thermal conductivity of the fuel has also been measured. X-ray diffraction study on the fuel compact reveals presence of α U and UO2 phases in the matrix of the fuel.

  6. 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

  7. 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.

  8. Radiation damage effects in candidate titanates for Pu disposition: Pyrochlore

    NASA Astrophysics Data System (ADS)

    Strachan, D. M.; Scheele, R. D.; Buck, E. C.; Icenhower, J. P.; Kozelisky, A. E.; Sell, R. L.; Elovich, R. J.; Buchmiller, W. C.

    2005-10-01

    Laboratory experiments on titanate ceramics were performed to verify whether certain assumptions are valid regarding the swelling, chemical durability, and microcracking that might occur as 239Pu decays. Titanate ceramics are the material of choice for the immobilization of surplus weapons-grade Pu. The short-lived isotope 238Pu, was incorporated into the ceramic formulation to accelerate the effects of radiation-induced damage. We report on the effects of this damage on the density (volumetric swelling <6%), crystal structure of pyrochlore-bearing specimens (amorphous after about 2 × 1018 α/g), and dissolution (no change from the fully crystalline specimen). Even though the specimens became amorphous during the tests, there was no evidence for microcracking in the photomicrographs from the scanning electron microscope. Thus, although pyrochlore is susceptible to radiation-induced damage, the material remains chemically and physically viable as a material for immobilizing surplus weapons-grade Pu.

  9. Neutron Capture and Fission Measurement on ^238Pu at DANCE

    NASA Astrophysics Data System (ADS)

    Chyzh, Andrii; Wu, Ching-Yen; Kwan, Elaine; Henderson, Roger; Gostic, Jolie; Couture, Aaron; Young, Hye; Ullmann, John; O'Donnell, John; Jandel, Marian; Haight, Robert; Bredeweg, Todd

    2012-10-01

    Neutron capture and fission reactions on actinides are important in nuclear engineering and physics. DANCE (Detector for Advanced Neutron Capture Measurement, LANL) combined with PPAC (avalanche technique based fission tagging detector, LLNL) were used to study the neutron capture reactions in ^238Pu. Because of extreme spontaneous α-radioactivity in ^238Pu and associated safety issues, 3 separate experiments were performed in 2010-2012. The 1st measurement was done without fission tagging on a 396-μg thick target. The 2nd one was with PPAC on the same target. The 3rd final measurement was done on a thin target with a mass of 40 μg in order to reduce α-background load on PPAC. This was the first such measurement in a laboratory environment. The absolute ^238Pu(n,γ) cross section is presented together with the prompt γ-ray multiplicity in the ^238Pu(n,f) reaction.

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

    PubMed

    Karpova, V N

    1985-11-01

    Dogs of both sexes aged 2 to 4 were subjected to inhalation inoculation with polymer 239Pu or submicron 239PuO2 aerosols in amounts close to acute, subacute and chronically effective ones. ECG was recorded in standard, amplified and single leads (V3). All calculations were done by lead II. Signs of the right heart overburdening were noted in the presence of the P-pulmonale complex, deep S1 wave or cardiac electrical axis of SI-SII-SIII type. Signs of the right heart overburdening were revealed after inhalation of polimer 239Pu (70%). The absence of similar changes in damage caused by 239Pu could be attributed to its fast resorption from the lungs resulting in more moderate lesion of the respiratory organs. PMID:4068946

  11. On the electronic configuration in Pu: spectroscopy and theory

    SciTech Connect

    Tobin, J G; Soderlind, P; Landa, A; Moore, K T; Schwartz, A J; Chung, B W; Wall, M; Wills, J M; Eriksson, O; Haire, R; Kutepov, A L

    2006-10-11

    Photoelectron spectroscopy, synchrotron-radiation-based x-ray absorption, electron energy-loss spectroscopy, and density-functional calculations within the mixed-level and magnetic models, together with canonical band theory have been used to study the electron configuration in Pu. These methods suggest a 5f{sup n} configuration for Pu of 5 {le} n < 6, with n {ne} 6, contrary to what has recently been suggested in several publications. We show that the n = 6 picture is inconsistent with the usual interpretation of photoemission and x-ray absorption spectra. Instead, these spectra support the traditional conjecture of a 5f{sup 5} configuration in Pu as is obtained by density-functional theory. We further argue, based on 5f-band filling, that an n = 6 hypothesis is incompatible with the position of Pu in the actinide series and its monoclinic ground-state phase.

  12. Capabilities for Testing the Electronic Configuration in Pu

    SciTech Connect

    Tobin, J G; Soderlind, P; Landa, A; Moore, K T; Schwartz, A J; Chung, B W; Wall, M A

    2006-11-08

    The benchmarking of theoretical modeling is crucial to the ultimate determination of the nature of the electronic structure of Pu. Examples of experimental techniques used for cross checking state of the art calculations will be given.

  13. 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)

  14. Probing Actinide Electronic Structure through Pu Cluster Calculations

    DOE PAGESBeta

    Ryzhkov, Mickhail V.; Mirmelstein, Alexei; Yu, Sung-Woo; Chung, Brandon W.; Tobin, James G.

    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.

  15. 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. PMID:21890207

  16. Unsafe coulomb excitation of {sup 240-244}Pu.

    SciTech Connect

    Wiedenhoever, I.

    1998-12-01

    The high spin states of {sup 240}Pu and {sup 244}Pu have been investigated with GAMMASPHERE at ATLAS, using Coulomb excitation with a {sup 208}Pb beam at energies above the Coulomb barrier. Data on a transfer channel leading to {sup 242}Pu were obtained as well. In the case of {sup 244}Pu, the yrast band was extended to 34{h_bar}, revealing the completed {pi}i{sub 13/2} alignment, a ''first'' for actinide nuclei. The yrast sequence of {sup 242}Pu was also extended to higher spin and a similar backbend was delineated. In contrast, while the ground state band of {sup 240}Pu was measured up to the highest rotational frequencies ever reported in the actinide region ({approximately} 300 keV), no sign of particle alignment was observed. In this case, several observables such as the large B(E1)/B(E2) branching ratios in the negative parity band, and the vanishing energy staggering between the negative and positive parity bands suggest that the strength of octupole correlations increases with rotational frequency. These stronger correlations may well be responsible for delaying or suppressing the {pi}i{sub 13/2} particle alignment.

  17. Unusual behaviour of (Np,Pu)B2C

    NASA Astrophysics Data System (ADS)

    Klimczuk, Tomasz; Boulet, Pascal; Griveau, Jean-Christophe; Colineau, Eric; Bauer, Ernst; Falmbigl, Matthias; Rogl, Peter; Wastin, Franck

    2015-02-01

    Two transuranium metal boron carbides, NpB2C and PuB2C have been synthesized by argon arc melting. The crystal structures of the {Np,Pu}B2C compounds were determined from single-crystal X-ray data to be isotypic with the ThB2C-type (space group ?, a = 0.6532(2) nm; c = 1.0769(3) nm for NpB2C and a = 0.6509(2) nm; c = 1.0818(3) nm for PuB2C; Z = 9). Physical properties have been derived from polycrystalline bulk material in the temperature range from 2 to 300 K and in magnetic fields up to 9 T. Magnetic susceptibility and heat capacity data indicate the occurrence of antiferromagnetic ordering for NpB2C with a Neel temperature TN = 68 K. PuB2C is a Pauli paramagnet most likely due to a strong hybridization of s(p,d) electrons with the Pu-5f states. A pseudo-gap, as concluded from the Sommerfeld value and the electronic transport, is thought to be a consequence of the hybridization. The magnetic behaviour of {Np,Pu}B2C is consistent with the criterion of Hill.

  18. Accident tolerant fuels for LWRs: A perspective

    NASA Astrophysics Data System (ADS)

    Zinkle, S. J.; Terrani, K. A.; Gehin, J. C.; Ott, L. J.; Snead, L. L.

    2014-05-01

    The motivation for exploring the potential development of accident tolerant fuels in light water reactors to replace existing Zr alloy clad monolithic (U, Pu) oxide fuel is outlined. The evaluation includes a brief review of core degradation processes under design-basis and beyond-design-basis transient conditions. Three general strategies for accident tolerant fuels are being explored: modification of current state-of-the-art zirconium alloy cladding to further improve oxidation resistance (including use of coatings), replacement of Zr alloy cladding with an alternative oxidation-resistant high-performance cladding, and replacement of the monolithic ceramic oxide fuel with alternative fuel forms.

  19. Oxygen potential of a prototypic Mo-cermet fuel containing plutonium oxide

    NASA Astrophysics Data System (ADS)

    Miwa, Shuhei; Osaka, Masahiko; Nozaki, Takahiro; Arima, Tatsumi; Idemitsu, Kazuya

    2015-10-01

    Oxygen potential of a prototypic Mo-cermet fuel containing 50 vol.% PuO2-x were investigated by the thermogravimetric analysis in the temperature range from 1273 K to 1473 K. It was shown that the oxygen potential and oxidation rate of the Mo-cermet were the same as those of pure PuO2-x below the oxygen potential of Mo/MoO2 oxidation reaction. The same features of the Mo-cermet sample containing 50 vol.% PuO2-x with those of pure PuO2-x were discussed in terms of the microstructure.

  20. 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.

  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. 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. PMID:24374184

  3. 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.

  4. 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.

  5. 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

  6. 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.

  7. Determination of plutonium content in TRR spent fuel by nondestructive neutron counting

    NASA Astrophysics Data System (ADS)

    Chen, Yen-Fu; Sheu, Rong-Jiun; Chiao, Ling-Huan; Yuan, Ming-Chen; Jiang, Shiang-Huei

    2010-07-01

    For the nuclear safeguard purpose, this work aims to nondestructively determine the plutonium content in the Taiwan Research Reactor (TRR) spent fuel rods in the storage pool before the stabilization process, which transforms the metal spent fuel rods into oxide powder. A SPent-fuel-Neutron-Counter (SPNC) system was designed and constructed to carry out underwater scan measurements of neutrons emitting from the spent fuel rod, from which the 240Pu mass in the fuel rod will be determined. The SAS2 H control module of the SCALE 5.1 code package was applied to calculate the 240Pu-to-Pu mass ratio in the TRR spent fuel rod according to the given power history. This paper presents the methodology and design of our detector system as well as the measurements of four TRR spent fuel rods in the storage pool and the comparison of the measured results with the facility declared values.

  8. Investigation of the oxidation states of Pu isotopes in a hydrochloric acid solution.

    PubMed

    Lee, M H; Kim, J Y; Kim, W H; Jung, E C; Jee, K Y

    2008-12-01

    The characteristics of the oxidation states of Pu in a hydrochloric acid solution were investigated and the results were applied to a separating of Pu isotopes from IAEA reference soils. The oxidation states of Pu(III) and Pu(IV) were prepared by adding hydroxylamine hydrochloride and sodium nitrite to a Pu stock solution, respectively. Also, the oxidation state of Pu(VI) was adjusted with concentrated HNO(3) and HClO(4). The stability of the various oxidation states of plutonium in a HCl solution with elapsed time after preparation were found to be in the following order: Pu(III) approximately Pu(VI)>Pu(IV)>Pu(V). The chemical recoveries of Pu(IV) in a 9M HCl solution with an anion exchange resin were similar to those of Pu(VI). This method for the determination of Pu isotopes with an anion exchange resin in a 9M HCl medium was applied to IAEA reference soils where the activity concentrations of (239,240)Pu and (238)Pu in IAEA-375 and IAEA-326 were consistent with the reference values reported by the IAEA. PMID:18674920

  9. 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.

  10. The depth distribution of sup 90 Sr, sup 137 Cs, and sup 239,240 Pu in soil profile samples

    SciTech Connect

    Price, K.R.

    1989-04-01

    A special study was conducted at the Hanford Site and vicinity to investigate the depth distribution of {sup 90}Sr, {sup 137}Cs, and {sup 239,240}Pu in soil at two locations. Duplicate sets of samples were collected at each location from the soil surface to a depth of 30 cm in increments of 2.5 cm. Results from an onsite location near a retired nuclear fuel reprocessing facility were compared to results from a background location upwind and distant from the Site. The study showed that, regardless of location, the top 5 cm of soil contained 51 to 74% of the {sup 90}Sr, 99% of the {sup 137}Cs, and 96% of the {sup 239,240}Pu. Soil at the background location received radionuclides only from deposition of worldwide fallout, and averaged 1.6 pCi/cm{sup 2} of {sup 90}Sr, 3.0 pCi/cm{sup 2} of {sup 137}Cs, and 0.071 pCi/cm{sup 2} of {sup 239,240}Pu. Soil at the onsite location received radionuclides from deposition of both worldwide fallout and past operations of the retired fuel reprocessing facility and contained 4 times as much {sup 90}Sr, 5 times as much {sup 137}Cs, and 44 times as much {sup 239,240}Pu as the background location. (Pacific Northwest Laboratory is operated for the US Department of Energy by Battelle Memorial Institute under Contract AC06-76RLO1830.) 8 refs., 2 figs.

  11. Complexation Behavior of the Tri-n-butyl Phosphate Ligand with Pu(IV) and Zr(IV): A Computational Study.

    PubMed

    Gopakumar, Gopinadhanpillai; Sreenivasulu, B; Suresh, A; Brahmmananda Rao, C V S; Sivaraman, N; Joseph, M; Anoop, Anakuthil

    2016-06-23

    Tri-n-butyl phosphate (TBP), used as the extractant in nuclear fuel reprocessing, shows superior extraction abilities for Pu(IV) over a large number of fission products including Zr(IV). We have applied density functional theory (DFT) calculations to explain this selectivity by investigating differences in electronic structures of Pu(NO3)4·2TBP and Zr(NO3)4·2TBP complexes. On the basis of our quantum chemical calculations, we have established the lowest energy electronic states for both complexes; the quintet is the ground state for the former, whereas the latter exists in the singlet spin state. The calculated structural parameters for the optimized geometry of the plutonium complex are in agreement with the experimental results. Atoms in Molecules analysis revealed a considerable amount of ionic character to M-O{TBP} and M-O{NO3} bonds. Additionally, we have also investigated the extraction behavior of TBP for metal nitrates and have estimated the extraction energies to be -73.1 and -57.6 kcal/mol for Pu(IV) and Zr(IV), respectively. The large extraction energy of Pu(IV) system is in agreement with the observed selectivity in the extraction of Pu. PMID:27248966

  12. 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)

  13. 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.

  14. 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.

  15. Fuel flexible fuel injector

    SciTech Connect

    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.

  16. CONVERSION OF RUSSIAN WEAPON-GRADE PLUTONIUM INTO OXIDE FOR MIXED OXIDE (MOX) FUEL FABRICATION.

    SciTech Connect

    Glagovski, E.; Kolotilov, Y.; Glagolenko, Y.; Zygmunt, Stanley J.; Mason, C. F. V.; Hahn, W. K.; Durrer, R. E.; Thomas, S.; Sicard, B.; Herlet, N.; Fraize, G.; Villa, A.

    2001-01-01

    Progress has been made in the Russian Federation towards the conversion of weapons-grade plutonium (w-Pu) into plutonium oxide (PuO{sub 2}) suitable for further manufacture into mixed oxide (MOX) fuels. This program is funded both by French Commissariat x 1'Energie Atomique (CEA) and the US National Nuclear Security Administration (NNSA). The French program was started as a way to make available their expertise gained from manufacturing MOX fuel. The US program was started in 1998 in response to US proliferation concerns and the acknowledged international need to decrease available w-Pu. Russia has selected both the conversion process and the manufacturing site. This paper discusses the present state of development towards fulfilling this mission: the demonstration plant designed to process small amounts of Pu and validate all process stages and the industrial plant that will process up to 5 metric tons of Pu per year.

  17. 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).

  18. 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.

  19. Oxygen induced transformations of the δ-Pu(111) surface

    NASA Astrophysics Data System (ADS)

    Taylor, Christopher D.

    2013-12-01

    The oxides that form on metal surfaces are critical to the preservation of the material under oxidizing conditions. For the case of plutonium, oxide film properties may affect a variety of kinetic phenomena related to the corrosion of the material. To investigate the behavior of the metal-oxygen interactions critical to the formation of such passive films, electronic structure calculations were performed on the interactions between O and the δ-Pu(111) surface. By probing the relationship between structure (coordination), charge transfer (valence) and thermodynamics (reactivity), it was found that oxidation is initially a local phenomenon, but, at 1.0 ML oxygen coverage, significant reconstructions that alter the phase structure of the near-surface region are induced. At this high-surface coverage the surface metal atoms are disbonded and the Pusbnd O coordination becomes four-fold as opposed to three fold. Even at this high coverage, however, the charge state more closely resembles Pu2O3 rather than PuO2. The ability for surface Pu atoms to adapt to a variety of changes in charge state and coordination provides a fundamental basis for understanding the multilayer structure of passive films formed on clean Pu surfaces. An analysis using first-principles thermodynamics also suggests that these films should develop uniformly, and not via an island or columnar growth mechanism.

  20. 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.

  1. 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.

  2. 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.

  3. Monte Carlo simulations of differential die-away instrument for determination of fissile content in spent fuel assemblies

    NASA Astrophysics Data System (ADS)

    Lee, Tae-Hoon; Menlove, Howard O.; Swinhoe, Martyn T.; Tobin, Stephen J.

    2011-10-01

    The differential die-away (DDA) technique has been simulated by using the MCNPX code to quantify its capability of measuring the fissile content in spent fuel assemblies. For 64 different spent fuel cases of various initial enrichment, burnup and cooling time, the count rate and signal to background ratios of the DDA system were obtained, where neutron backgrounds are mainly coming from the 244Cm of the spent fuel. To quantify the total fissile mass of spent fuel, a concept of the effective 239Pu mass was introduced by weighing the relative contribution to the signal of 235U and 241Pu compared to 239Pu and the calibration curves of DDA count rate vs. 239Pu eff were obtained by using the MCNPX code. With a deuterium-tritium (DT) neutron generator of 10 9 n/s strength, signal to background ratios of sufficient magnitude are acquired for a DDA system with the spent fuel assembly in water.

  4. Electronic and thermodynamic properties of α-Pu2O3

    NASA Astrophysics Data System (ADS)

    Lu, Yong; Yang, Yu; Zheng, Fawei; Zhang, Ping

    2014-08-01

    Based on density functional theory+U calculations and the quasi-annealing simulation method, we obtain the ground electronic state for α-Pu2O3 and present its phonon dispersion curves as well as various thermodynamic properties, which have seldom been theoretically studied because of the huge unit cell. We find that the Pu-O chemical bonding is weaker in α-Pu2O3 than in fluorite PuO2, and subsequently a frequency gap appears between oxygen and plutonium vibration density of states. Based on the calculated Helmholtz free energies at different temperatures, we further study the reaction energies for Pu oxidation, PuO2 reduction, and transformation between PuO2 and α-Pu2O3. Our reaction energy results are in agreements with available experiment. And it is revealed that high temperature and insufficient oxygen environment are in favor of the formation of α-Pu2O3.

  5. 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.

  6. 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. PMID:21306104

  7. 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.

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

    PubMed

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

    2014-02-01

    Information on Pu in environmental samples is traditionally based on the determination of the (240+239)Pu activity via Alpha Spectrometry (AS). A large number of alpha spectrometry sources (planchettes) containing radiochemically separated Pu are therefore stored worldwide and are available for further analyses. These archive samples represent a resource from which valuable information on isotopic composition of alpha emitters including Pu can be obtained. The relative abundances of Pu isotopes can be used to trace specific Pu sources and characterize the relative contributions of different Pu sources in a sample. Thus, in addition to the total (239+240)Pu activity, determination of the (240)Pu/(239)Pu ratio can provide valuable information on the nature of the Pu emitting sources. The Pu isotopic ratios can be determined by mass spectrometry techniques such as Sector Field Inductively Coupled Plasma Mass Spectrometry (SF-ICPMS) or Accelerator Mass Spectrometry (AMS) that require dissolution and complete destruction of the material deposited on the planchettes. In this study Laser Ablation (LA)-quadrupole-ICP-MS has been employed for the analysis of (239)Pu/(240)Pu ratios from alpha-planchettes prepared from samples originating from the Mayak PA nuclear facility, Russia. The results are compared with data from AMS and show that the (240)Pu/(239)Pu ratios obtained by LA-ICP-MS can be utilized to distinguish weapons-grade Pu from civil reprocessing sources. Moreover, isotope ratio mapping can also be performed across the planchettes, allowing e.g. the visualization of possible inhomogeneities in the Pu-isotope distribution on their surface. Thus, this solid sample technique can be applied to extract additional information from existing archives of samples. PMID:24424783

  9. 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)

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

    PubMed

    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

  11. 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

  12. 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.

  13. Probing the Nature of Superconductivity in the Heavy Fermion PuMGa5 and PuMIn5 (M =Co, Rh) Compounds

    NASA Astrophysics Data System (ADS)

    Bauer, Eric; Tobash, Paul; Mitchell, Jeremy; Thompson, Joe

    2014-03-01

    The discovery of superconductivity in PuCoGa5 with a Tc = 18.5 K has generated renewed interest in Pu-based compounds. PuCoGa5, and its superconducting cousin PuRhGa5 (Tc = 8.7 K), have the same crystal structure as the tetragonal CeMIn5 (T =Co, Rh, Ir) heavy fermion superconductors, suggesting that the structure plays a key role in generating superconductivity in these materials. While a variety of measurements have firmly established that the CeTIn5 compounds are unconventional d-wave superconductors, most probably mediated by antiferromagnetic spin fluctuations, it is less clear what drives the high transition temperature in PuCoGa5, which is an order of magnitude larger than all other know Ce- or U-based heavy fermion superconductors. The physical properties of two new members of this ``115'' family of superconductors, PuRhIn5 and PuCoIn5, indicate that they reside close to an antiferromagnetic quantum critical point, while the smaller effective masses and much smaller unit cell volumes of PuCoGa5 and PuRhGa5 suggest that they may be near a T =0 valence instability or that the Pu 5f electrons couple to conduction electrons in multiple channels to form ``composite'' superconducting pairs. The nature of superconductivity in these four Pu115 materials will be discussed. Work at Los Alamos was performed under the auspices of the US DOE.

  14. 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.

  15. 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. PMID:18677996

  16. 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.

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

    NASA Astrophysics Data System (ADS)

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

    2014-09-01

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

  18. 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.

  19. Low temperature heat capacity of PuPO 4

    NASA Astrophysics Data System (ADS)

    Thiriet, C.; Konings, R. J. M.; Wastin, F.

    2005-09-01

    PuPO 4 was prepared successfully by coprecipitation and its heat capacity measured between 5 K and 300 K by a hybrid adiabatic relaxation calorimeter. The standard entropy S0 (298.15 K) of PuPO 4 was derived and a semi-empirical method was used to describe the total entropy as the sum of the lattice entropy Slat and the excess entropy Sexs as verified for the iso-electronic lanthanide orthophosphates. Thus the standard entropies of some actinide (III) orthophosphates were estimated.

  20. Constrained Density Functional Calculations of alpha and delta Pu

    NASA Astrophysics Data System (ADS)

    Eriksson, Olle

    2002-03-01

    The electronic structure of α and δ Pu are described using a modified density functional theory that incorporates localization effects of the 5f shell. It is argued that a Russel-Saunders coupled state involving a 5f^4 multiplet, together with one itinerant 5f electron explains most of the observed ground state properties of δ Pu (equilibrium volume, elastic constants, near degeneracy with the alpha phase). This 5f electrons in the α phase are argued to form itinerant states, that are well described in density functional theory. The two distinctly different electronic ground states give rise to different excitation spectra and a comparison with experimental data is made.

  1. 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).

  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. 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

    2007-02-01

    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. PMID:17257046

  4. 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

  5. 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

  6. 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.

  7. Reductive dissolution of Pu(IV) by Clostridium sp. under anaerobic conditions.

    PubMed

    Francis, Arokiasamy J; Dodge, Cleveland J; Gillow, Jeffrey B

    2008-04-01

    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 microm 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 suggestthat, 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. PMID:18504965

  8. 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

  9. Effects of cooling time on a closed LWR fuel cycle

    SciTech Connect

    Arnold, R. P.; Forsberg, C. W.; Shwageraus, E.

    2012-07-01

    In this study, the effects of cooling time prior to reprocessing spent LWR fuel has on the reactor physics characteristics of a PWR fully loaded with homogeneously mixed U-Pu or U-TRU oxide (MOX) fuel is examined. A reactor physics analysis was completed using the CASM04e code. A void reactivity feedback coefficient analysis was also completed for an infinite lattice of fresh fuel assemblies. Some useful conclusions can be made regarding the effect that cooling time prior to reprocessing spent LWR fuel has on a closed homogeneous MOX fuel cycle. The computational analysis shows that it is more neutronically efficient to reprocess cooled spent fuel into homogeneous MOX fuel rods earlier rather than later as the fissile fuel content decreases with time. Also, the number of spent fuel rods needed to fabricate one MOX fuel rod increases as cooling time increases. In the case of TRU MOX fuel, with time, there is an economic tradeoff between fuel handling difficulty and higher throughput of fuel to be reprocessed. The void coefficient analysis shows that the void coefficient becomes progressively more restrictive on fuel Pu content with increasing spent fuel cooling time before reprocessing. (authors)

  10. 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)

  11. 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)

  12. 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.

  13. 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.

  14. Inhalation deposition and retention patterns of a U-Pu chain aggregate aerosol.

    PubMed

    Briant, J K; Sanders, C L

    1987-10-01

    Chain aggregate aerosol particles are normally formed during many high-temperature combustion and vaporization processes. The shape of chain aggregate aerosol particles could have an effect on the pattern of inhalation deposition and retention of the particles in the respiratory tract. A chain aggregate aerosol of nuclear reactor fuel could be present as an inhalation hazard if it were released to the atmosphere after a meltdown, core-disruptive accident. Rats were exposed to a chain aggregate U-Pu aerosol made by laser vaporization of mixed-oxide, breeder reactor fuel (20% plutonium dioxide and 80% uranium dioxide), then sacrificed to measure the clearance and retention of the fuel aerosol particles. Deposition of the 0.7-micron (activity median aerodynamic equivalent diameter) aerosol particles resulted in an average initial lung burden of 4140 Bq alpha activity. The chain aggregate particle shape was not a major factor in the total deposition; however, it may have influenced the regional distribution of the activity deposited. Retention of the particles in the upper airways of the tracheobronchial tree was on the order of 1% of the concurrent lung burden, which is consistent with recent data of other investigations. This study indicates that insoluble chain aggregate particles are retained in the tracheobronchial airways to a degree similar to simple spherically shaped particles of equivalent volume diameter. PMID:3654224

  15. 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. PMID:17651874

  16. 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.

  17. 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.

  18. Microautoradiography in studies of Pu(V) sorption by trace and fracture minerals in tuff

    SciTech Connect

    Vaniman, D.; Furlano, A.; Chipera, S.; Thompson, J.; Triay, I.

    1996-08-01

    Microautoradiography was used to evaluate the mineralogic basis of Pu(V) retention by tufts from Yucca Mountain, Nevada. Altered orthopyroxenes and oxide minerals are associated with high Pu retention, but are limited to specific stratigraphic horizons. A weaker but more general association of Pu with smectite occurs in most samples. Thin-sections that cross fractures allow comparative studies of Pu retention by fracture-lining versus matrix minerals. Using Ag metal in emulsions as a measure of underlying Pu concentration, electron-microprobe (EMP) analysis can quantify Pu retention along fracture walls and provide mineral/mineral Pu retention factors. For smectite-lined microfractures in zeolitized tuff, the smectite/clinoptilolite Pu retention factor is > 80.

  19. Microautoradiography in studies of Pu(V) sorption by trace and fracture minerals in tuff

    SciTech Connect

    Vaniman, D.; Furlano, A.; Chipera, S.; Thompson, J.; Triay, I.

    1996-12-31

    Microautoradiography was used to evaluate the mineralogic basis of Pu(V) retention by tuffs from Yucca Mountain, Nevada. Altered orthopyroxenes and oxide minerals are associated with high Pu retention but are limited to specific stratigraphic horizons. A weaker but more general association of Pu with smectite occurs in most samples. Thin-sections that cross fractures allow comparative studies of Pu retention by fracture-lining versus matrix minerals. Using Ag metal in emulsions as a measure of underlying Pu concentration, electron-microprobe analysis can quantify Pu retention along fracture walls and provide mineral/mineral Pu retention factors. For smectite-lined microfractures in zeolitized tuff, the smectite/clinoptilolite Pu retention factor is >80.

  20. 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.

  1. 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.

  2. Quantum size effects in δ-Pu (110) films

    NASA Astrophysics Data System (ADS)

    Gong, H.; Ray, A. K.

    2005-12-01

    First-principles full-potential linearized-augmented-plane-wave (FP-LAPW) calculations have been carried out for δ-Pu (110) films up to seven layers. The layers have been studied at the non-spin-polarized-no-spin-orbit coupling (NSP-NSO), non-spin-polarized-spin-orbit coupling (NSP-SO), spin-polarized-no-spin-orbit coupling (SP-NSO), spin-polarized-spin-orbit coupling (SP-SO), antiferromagnetic-no-spin-orbit coupling (AFM-NSO), and antiferromagnetic-spin-orbit-coupling (AFM-SO) levels of theory. The ground state of δ-Pu (110) films is found to be at the AFM-SO level of theory and the surface energy is found to rapidly converge. The semi-infinite surface energy for δ-Pu (110) films is predicted to be 1.41 J/m2, while the magnetic moments show an oscillating behavior, gradually approaching the bulk value of zero with increase in the number of layers. Work functions indicate a strong quantum size effect up to and including seven layers. The work function of the seven-layer δ-Pu (110) film at the ground state is found to be 2.99 eV.

  3. 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. PMID:24631917

  4. 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.

  5. 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.

  6. 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. PMID:26736181

  7. 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.

  8. DENSITY-FUNCTIONAL STUDY OF Zr-BASED ACTINIDE ALLOYS: 2. U-Pu-Zr SYSTEM

    SciTech Connect

    Landa, A; Soderlind, P; Turchi, P; Vitos, L; Ruban, A

    2009-02-09

    Density-functional theory, previously used to describe phase equilibria in the U-Zr alloys [1], is applied to study ground state properties of the bcc U-Pu-Zr solid solutions. Calculated heats of formation of the Pu-U and Pu-Zr alloys are in a good agreement with CALPHAD assessments. We found that account for spin-orbit coupling is important for successful description of Pu-containing alloys.

  9. Minor Actinides Loading Optimization for Proliferation Resistant Fuel Design - BWR

    SciTech Connect

    G. S. Chang; Hongbin Zhang

    2009-09-01

    One approach to address the United States Nuclear Power (NP) 2010 program for the advanced light water reactor (LWR) (Gen-III+) intermediate-term spent fuel disposal need is to reduce spent fuel storage volume while enhancing proliferation resistance. One proposed solution includes increasing burnup of the discharged spent fuel and mixing minor actinide (MA) transuranic nuclides (237Np and 241Am) in the high burnup fuel. Thus, we can reduce the spent fuel volume while increasing the proliferation resistance by increasing the isotopic ratio of 238Pu/Pu. For future advanced nuclear systems, MAs 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 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. A typical boiling water reactor (BWR) fuel unit lattice cell model with UO2 fuel pins will be used to investigate the effectiveness of adding MAs (237Np and/or 241Am) to enhance proliferation resistance and improve fuel cycle performance for the intermediate-term goal of future nuclear energy systems. However, adding MAs will increase plutonium production in the discharged spent fuel. In this work, the Monte-Carlo coupling with ORIGEN-2.2 (MCWO) method was used to optimize the MA loading in the UO2 fuel such that the discharged spent fuel demonstrates enhanced proliferation resistance, while minimizing plutonium production. The axial averaged MA transmutation characteristics at different burnup were compared and their impact on neutronics criticality and the ratio of 238Pu/Pu discussed.

  10. A Blueprint for GNEP Advanced Burner Reactor Startup Fuel Fabrication Facility

    SciTech Connect

    S. Khericha

    2010-12-01

    The purpose of this article is to identify the requirements and issues associated with design of GNEP Advanced Burner Reactor Fuel Facility. The report was prepared in support of providing 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 was 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 was 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 was 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 was assumed to 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) was being considered for fabrication of WG Pu fuel for the ABR. It was estimated that the facility will provide the startup fuel for 10-15 years and would take 3 to 5 years to construct.

  11. 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.

  12. 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.

  13. Transcription factor PU.1 is expressed in white adipose and inhibits adipocyte differentiation

    Technology Transfer Automated Retrieval System (TEKTRAN)

    PU.1 transcription factor is a critical regulator of hematopoiesis and leukemogenesis. Because PU.1 interacts with transcription factors GATA-2 and C/EBPa, both of which are involved in the regulation of adipogenesis, we investigated whether PU.1 also plays a role in the regulation of adipocyte diff...

  14. An Internal LLNL Report: Spectroscopic Signature of Aging in (Delta)-Pu(Ga)

    SciTech Connect

    Chung, B W; Fluss, M J; Haslam, J J; Schwartz, A J; Tobin, J G

    2004-12-29

    Resonant Photoemission, a variant of Photoelectron Spectroscopy, has been demonstrated to have sensitivity to aging of Pu samples. The spectroscopic results are correlated with resistivity measurements and are shown to be the fingerprint of mesoscopic or nanoscale internal damage in the Pu physical structure. This means that a spectroscopic signature of internal damage due to aging in Pu has been established.

  15. The redox potential of Pu containing acidic solutions and the fate of "Pu(IV)-colloids": Direct measurement versus optical absorption spectroscopy

    NASA Astrophysics Data System (ADS)

    Icker, M.; Walther, C.; Neck, V.; Geckeis, H.

    2010-03-01

    Redox potentials were measured in acidic aqueous solutions (-log10[H+]=0.7) containing different fractions of tri- and tetravalent plutonium. Eh values measured directly by a Pt electrode vs Ag/AgCl reference electrode agree very well with the redox potential calculated from the oxidation state distribution Pu(III)/Pu(IV). By monitoring the solutions over 120 days the kinetics of redox state distribution and dissolution of initially present Pu(IV)-colloids were studied. In solutions of Eh>950mV colloids dissolve and form Pu(VI), whereas at lower Eh the dissolution of colloids leads to formation of Pu(III). These findings corroborate the assumption that colloids are an integral part of the aqueous Pu redox chemistry and that formation and dissolution can be fully understood by means of Eh / pH stability calculations.

  16. 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.

  17. 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.

  18. Radionuclide release from research reactor spent fuel

    NASA Astrophysics Data System (ADS)

    Curtius, H.; Kaiser, G.; Müller, E.; Bosbach, D.

    2011-09-01

    Numerous investigations with respect to LWR fuel under non oxidizing repository relevant conditions were performed. The results obtained indicate slow corrosion rates for the UO 2 fuel matrix. Special fuel-types (mostly dispersed fuels, high enriched in 235U, cladded with aluminium) are used in German research reactors, whereas in German nuclear power plants, UO 2-fuel (LWR fuel, enrichment in 235U up to 5%, zircaloy as cladding) is used. Irradiated research reactor fuels contribute less than 1% to the total waste volume. In Germany, the state is responsible for fuel operation and for fuel back-end options. The institute for energy research (IEF-6) at the Research Center Jülich performs investigation with irradiated research reactor spent fuels under repository relevant conditions. In the study, the corrosion of research reactor spent fuel has been investigated in MgCl 2-rich salt brine and the radionuclide release fractions have been determined. Leaching experiments in brine with two different research reactor fuel-types were performed in a hot cell facility in order to determine the corrosion behaviour and the radionuclide release fractions. The corrosion of two dispersed research reactor fuel-types (UAl x-Al and U 3Si 2-Al) was studied in 400 mL MgCl 2-rich salt brine in the presence of Fe 2+ under static and initially anoxic conditions. Within these experimental parameters, both fuel types corroded in the experimental time period of 3.5 years completely, and secondary alteration phases were formed. After complete corrosion of the used research reactor fuel samples, the inventories of Cs and Sr were quantitatively detected in solution. Solution concentrations of Am and Eu were lower than the solubility of Am(OH) 3(s) and Eu(OH) 3(s) solid phases respectively, and may be controlled by sorption processes. Pu concentrations may be controlled by Pu(IV) polymer species, but the presence of Pu(V) and Pu(IV) oxyhydroxides species due to radiolytic effects cannot

  19. 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.

  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. 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.

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

    DOE PAGESBeta

    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

  3. 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. PMID:25050458

  4. 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. PMID:25455816

  5. 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

  6. 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.

  7. 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.

  8. The Optimum Plutonium Fuel Form in Light Water Reactors

    NASA Astrophysics Data System (ADS)

    Tulenko, James S.; Savela, Michael; Gueorguiev, Gueorgui

    2003-07-01

    The University of Florida has underway a research program to validate the benefits of developing a Pu/ZrH/U matrix fuel for the irradiation of the U.S. weapons plutonium and European reprocessed plutonium from an economic, operational, and performance basis. Thermal reactors using plutonium as a fuel are inherently undermoderated because of the large absorption cross sections of plutonium and the presence of large absorption resonances for plutonium in the thermal and near-thermal energy ranges. The use of the proven TRIGA ZrHx-based fuel with plutonium has shown an extremely large (>20%) increase in reactivity over the conventional UO2/PuO2 fuel form currently being considered, with an additional major increase in the destruction of plutonium, rendering it an extremely attractive fuel form for plutonium disposition.

  9. 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. PMID:24266655

  10. PU.1 induces apoptosis in myeloma cells through direct transactivation of TRAIL

    PubMed Central

    Ueno, S; Tatetsu, H; Hata, H; Iino, T; Niiro, H; Akashi, K; Tenen, DG.; Mitsuya, H; Okuno, Y

    2010-01-01

    We previously reported that PU.1 was down-regulated in myeloma cell lines and myeloma cells in a subset of myeloma patients, and that conditional PU.1 expression in PU.1-negative myeloma cell lines, U266 and KMS12PE, induced growth arrest and apoptosis. To elucidate the molecular mechanisms of the growth arrest and apoptosis, we performed DNA microarray analyses to compare the difference in gene expression before and after PU.1 induction in U266 cells. Among cell cycle-related genes, cyclin A2, cyclin B1, CDK2 and CDK4 were down-regulated and p21 was up-regulated, while among apoptosis-related genes, TRAIL was found highly up-regulated. When TRAIL was knocked down by siRNAs, apoptosis of PU-1-expressing cells was inhibited, suggesting that TRAIL plays a critical role in PU.1-induced apoptosis in both U266 and KMS12PE myeloma cells. In both U266 and KMS12PE cells expressing PU.1, PU.1 directly bound to a region 30 bp downstream of the transcription start site of the TRAIL gene. Up-regulation of PU.1 induced transactivation of the TRAIL promoter in reporter assays, and disruption of the PU.1-binding site in the TRAIL promoter eliminated this transactivation. Therefore, we conclude that PU.1 is capable of inducing apoptosis in certain myeloma cells by direct transactivation of TRAIL. PMID:19749795

  11. Plutonium isotopes in settling particles: transport and scavenging of Pu in the western Northwest Pacific.

    PubMed

    Zheng, Jian; Yamada, Masatoshi

    2006-07-01

    We examined the vertical distributions of 239+240Pu activity and 240Pu/239Pu atom ratio in settling particles and quantified the particulate 239+240Pu fluxes in the water column in the western Northwest Pacific. Settling particle samples were collected using sediment traps. Plutonium isotopes were analyzed using a sector field high-resolution ICP-MS. To the best of our knowledge, this is the first time that both Pu activity and Pu isotope ratio data have been obtained for settling particles in the Pacific Ocean. The high (>0.18) 240Pu/239Pu atom ratios in settling particles indicate that plutonium from the Pacific Proving Grounds (PPG) source in the central Pacific is transported toward the western Northwest Pacific. Evidence indicates that Pu scavenging onto the settling particles is strongly dependent upon the bulk mass flux. The results suggest that advective lateral transport of dissolved Pu from the open ocean to the ocean margin and removal of Pu into the margin sediments by particle scavenging is a common phenomenon in the Pacific Ocean. Plutonium can be considered as a useful tracer to study the transport and fate of other contaminants that readily adsorb to particles in marine environments. PMID:16856723

  12. Helium Behavior in Oxide Nuclear Fuels: First Principles Modeling

    SciTech Connect

    Gryaznov, D.; Rashkeev, Sergey N.; Kotomin, E. A.; Heifets, Eugene; Zhukovskii, Yuri F.

    2010-10-01

    UO2 and (U, Pu)O2 solid solutions (the so-called MOX) nowadays are used as commercial nuclear fuels in many countries. One of the safety issues during the storage of these fuels is related to their self-irradiation that produces and accumulates point defects and helium therein. We present density functional theory (DFT) calculations for UO2, PuO2 and MOX containing He atoms in octahedral interstitial positions. In particular, we calculated basic MOX properties and He incorporation energies as functions of Pu concentration within the spin-polarized, generalized gradient approximation (GGA) DFT calculations. We also included the on-site electron correlation corrections using the Hubbard model (in the framework of the so-called DFT + U approach). We found that PuO2 remains semiconducting with He in the octahedral position while UO2 requires a specific lattice distortion. Both materials reveal a positive energy for He incorporation, which, therefore, is an exothermic process. The He incorporation energy increases with the Pu concentration in the MOX fuel.

  13. Electronic structure of α- and δ-Pu from photoelectron spectroscopy

    NASA Astrophysics Data System (ADS)

    Arko, A. J.; Joyce, J. J.; Morales, L.; Wills, J.; Lashley, J.; Wastin, F.; Rebizant, J.

    2000-07-01

    We report photoemission results on α- and δ-Pu using a laser plasma light source (LPLS) as well as He light as the exciting radiation. The LPLS is a pseudocontinuum tunable light source with intensities rivaling some second-generation synchrotrons. Both phases of Pu display a narrow, temperature-independent, 5f-related feature at the Fermi energy, which is narrower in δ-Pu than in α-Pu, suggestive of possible heavy-fermion-like behavior. In both α-Pu and δ-Pu the photon-energy dependence of this feature suggests some 6d admixture, albeit somewhat smaller in δ-Pu. In this respect it differs qualitatively from Ce and U heavy fermions.

  14. 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

  15. Design of a Pu-238 Waste Incineration Process

    SciTech Connect

    Charlesworth, D.L.

    2001-05-29

    Combustible Pu-238 waste is generated as a result of normal operation and decommissioning activity at the Savannah River Plant and is being retrievably stored there. As part of the long-term plan to process the stored waste and current waste in preparation for future disposition, a Pu-238 incineration process is being cold-tested at Savannah River Laboratory (SRL). The incineration process consists of a continuous-feed preparation system, a two-stage, electrically fired incinerator, and a filtration off-gas system. Process equipment has been designed, fabricated, and installed for nonradioactive testing and cold run-in. Design features to maximize the ability to remotely maintain the equipment were incorporated into the process. Interlock, alarm, and control functions are provided by a programmable controller. Cold testing is scheduled to be completed in 1986.

  16. 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.

  17. Quantum Size Effects in δ -- Pu (111) and (110) Films*

    NASA Astrophysics Data System (ADS)

    Gong, Haoran; Ray, Asok Kumar

    2006-03-01

    First-principles full-potential linearized-augmented-plane-wave (FP-LAPW) calculations have been carried out for δ-Pu (111) and (110) films up to seven layers. The layers have been studied at the non-spin-polarized-no-spin-orbit coupling (NSP-NSO), non-spin-polarized-spin-orbit coupling (NSP-SO), spin-polarized-no-spin-orbit coupling (SP-NSO), spin-polarized-spin-orbit coupling (SP-SO), anti-ferromagnetic-no-spin-orbit coupling (AFM-NSO), and anti-ferromagnetic-spin-orbit-coupling (AFM-SO) levels of theory. The ground state of both δ-Pu (111) and (110) films is found to be at the AFM-SO level of theory and the surface energy is found to rapidly converge. The semi-infinite surface energy for δ-Pu (111) and (110) films is predicted to be 1.18 and 1.42 J/m^2, while the magnetic moments show an oscillating behavior, gradually approaching the bulk value of zero with increase in the number of layers. Work functions indicate a strong quantum size effect up to and including five layers for the (111) surface and seven layers for the (110) surface, respectively. The work functions of δ-Pu (111) and (110) films at the ground state are predicted be 3.41 and 2.99eV, respectively. *This work is supported by the Chemical Sciences, Geosciences, and Biosciences Division, Office of Basic Energy Sciences, Office of Science, Department of Energy (Grant DE-FG02-03ER15409) and the Welch Foundation, Houston, Texas (Grant Y-1525).

  18. 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.

  19. Characterization of Pu concentration and its isotopic composition in soils of Gansu in northwestern China.

    PubMed

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

    2009-01-01

    The total 239+240Pu activities and 240Pu/239Pu atom ratios in surface soil samples (0-5cm) in the Kumtag Desert in western Gansu Province, and in a soil core sample in Lanzhou were investigated using a sector-field ICP-MS. In the surface soil samples, 239+240Pu activities in fine particles (<150microm) were 1.3-2.1 times of those in coarse particles (150microm-1mm) which ranged from 0.005 to 0.157mBq/g. Atom ratios of 240Pu/239Pu in the surface soils ranged from 0.168 to 0.192 with a mean of 0.182+/-0.008. The mean ratio was similar to the typical global fallout value although the Kumtag Desert was believed to have received close-in fallout derived from Chinese nuclear weapons tests mainly conducted in the 1970s. Furthermore, the mean 240Pu/239Pu atom ratio observed in the soil core sample in Lanzhou was similar to the typical global fallout value. In the soil core sample, 239+240Pu activities in the various layers ranged from 0.012 to 0.23mBq/g, and the inventory of 239+240Pu (32.4Bq/m2, 0-23cm) was slightly lower than that expected from global fallout (42Bq/m2) at the same latitude. Rapid downward migration of Pu isotopes was observed in Lanzhou soil core sample layers. The contribution of the 10-cm deep top layers of surface soils to total inventory was only 17%, while the contribution of deeper layers (10-23cm) was as high as 83%. The 239+240Pu activity levels and 240Pu/239Pu atom ratios in soils in Gansu Province, China are similar to those in atmospheric deposition samples collected in the spring in recent years in Japan. PMID:19058885

  20. The significance of low PU.1 expression in patients with acute promyelocytic leukemia

    PubMed Central

    2012-01-01

    Background Although the importance of the hematopoietic transcription factor PU.1 in acute myeloid leukemia (AML) has been demonstrated, the expression of PU.1 in acute promyelocytic leukemia (APL) patient samples awaits further investigation. The current study used APL patient samples to assess the expression pattern of PU.1 in the initiation and progression of APL. Findings We used real-time RT-PCR to compare PU.1 expression between de novo APL patient samples and normal blood specimens, and the results indicated that PU.1 expression was significantly lower in newly diagnosed APL patient samples as compared to normal hematopoietic cells. Further evidence showed a significant inverse correlation between the expression level of PML-RARα and that of PU.1. In addition, we analyzed the correlation between PML-RARα and PU.1 expression in a large population of AML patients retrieved from the expression profiles. The results showed that PU.1 expression was lower in patients with APL than other AML subtypes and there was also a trend towards increasing PU.1 expression from AML-M0 to AML-M5, with the exception of AML-M3 (APL). These observations suggested that PU.1 expression was reduced by PML-RARα in APL patients. Furthermore, we measured PU.1 expression in APL-initiating cells isolated from de novo APL patients by side population cell analysis and found that suppression of PU.1 expression occurred concurrently with PML-RARα expression, indicating the pivotal role of PU.1 in APL initiation. Conclusion Our findings provide evidence that low PU.1 expression in APL patients is required for disease initiation and progression. PMID:22569057

  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. 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.

  3. 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.

  4. 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

  5. Measurement of 240Pu/239Pu isotopic ratios in soils from the Marshall Islands using ICP-MS.

    PubMed

    Muramatsu, Y; Hamilton, T; Uchida, S; Tagami, K; Yoshida, S; Robison, W

    2001-10-20

    Nuclear weapons tests conducted by the United States in the Marshall Islands produced significant quantities of regional or tropospheric fallout contamination. Here we report on some preliminary inductively coupled plasma-mass spectrometry (ICP-MS) measurements of plutonium isolated from seven composite soil samples collected from Bikini, Enewetak and Rongelap Atolls in the northern Marshall Islands. These data show that 240Pu/239Pu isotopic signatures in surface soils from the Marshall Island vary significantly and could potentially be used to help quantify the range and extent of fallout deposition (and associated impacts) from specific weapons tests. 137Cs and 60Co were also determined on the same set of soil samples for comparative purposes. PMID:11669263

  6. 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

  7. 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.

  8. 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.

  9. 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.

  10. 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

    2016-06-01

    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. PMID:27145713

  11. Dissolution characteristics of Pu-contaminated soils and sediments in lung serum simulant solution.

    PubMed

    Lee, S Y; Bondietti, E A; Tamura, T

    1982-11-01

    Dissolution characteristics of Pu from contaminated Nevada Test Site (NTS) and Rocky Flats (RF) soils, and Mound Laboratory (ML) and Oak Ridge National Laboratory (ORNL) sediments in lung serum simulant solution at 37 degrees C were investigated. The dissolved Pu concentration had reached a maximum within a day of equilibration and the percent dissolved Pu at the maximum was 0.70 (RF), 0.43 (ML), 0.02 (ORNL), and 0.02 (NTS). The Pu concentrations of the RF, ML and ORNL samples in the successively extracted solutions decreased drastically but the concentration in the NTS soil extracts did not change significantly. The differences in Pu dissolution among the samples were caused by the differences in the total Pu concentration, particle size distribution, and chemical nature of Pu in contaminated soils and sediments. The higher solubility of the particulate Pu form in the RF soil relative to the ORNL sediment contaminated by dissolved Pu suggests that contamination source alone can not explain the observed differences. Variation of Pu solubility among the samples indicates that a single solubility class for dose assessment use may not be appropriate, particularly if one attempts to make comparative assessments among different sites. PMID:7152928

  12. 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.

  13. 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. PMID:24328266

  14. Neutronic Benchmarks for the Utilization of Mixed-Oxide Fuel: Joint U.S./Russian Progress Report for Fiscal Year 1997 - Volume 4, Part 2--Saxton Plutonium Program Critical Experiments

    SciTech Connect

    Abdurrahman, NM

    2000-10-12

    Critical experiments with water-moderated, single-region PuO{sub 2}-UO{sub 2} or UO{sub 2}, and multiple-region PuO{sub 2}-UO{sub 2}- and UO{sub 2}-fueled cores were performed at the CRX reactor critical facility at the Westinghouse Reactor Evaluation Center (WREC) at Waltz Mill, Pennsylvania in 1965 [1]. These critical experiments were part of the Saxton Plutonium Program. The mixed oxide (MOX) fuel used in these critical experiments and then loaded in the Saxton reactor contained 6.6 wt% PuO{sub 2} in a mixture of PuO{sub 2} and natural UO{sub 2}. The Pu metal had the following isotopic mass percentages: 90.50% {sup 239}Pu; 8.57% {sup 239}Pu; 0.89% {sup 240}Pu; and 0.04% {sup 241}Pu. The purpose of these critical experiments was to verify the nuclear design of Saxton partial plutonium cores while obtaining parameters of fundamental significance such as buckling, control rod worth, soluble poison worth, flux, power peaking, relative pin power, and power sharing factors of MOX and UO{sub 2} lattices. For comparison purposes, the core was also loaded with uranium dioxide fuel rods only. This series is covered by experiments beginning with the designation SX.

  15. Optimisation of composite metallic fuel for minor actinide transmutation in an accelerator-driven system

    NASA Astrophysics Data System (ADS)

    Uyttenhove, W.; Sobolev, V.; Maschek, W.

    2011-09-01

    A potential option for neutralization of minor actinides (MA) accumulated in spent nuclear fuel of light water reactors (LWRs) is their transmutation in dedicated accelerator-driven systems (ADS). A promising fuel candidate dedicated to MA transmutation is a CERMET composite with Mo metal matrix and (Pu, Np, Am, Cm)O 2-x fuel particles. Results of optimisation studies of the CERMET fuel targeting to increasing the MA transmutation efficiency of the EFIT (European Facility for Industrial Transmutation) core are presented. In the adopted strategy of MA burning the plutonium (Pu) balance of the core is minimized, allowing a reduction in the reactivity swing and the peak power form-factor deviation and an extension of the cycle duration. The MA/Pu ratio is used as a variable for the fuel optimisation studies. The efficiency of MA transmutation is close to the foreseen theoretical value of 42 kg TW -1 h -1 when level of Pu in the actinide mixture is about 40 wt.%. The obtained results are compared with the reference case of the EFIT core loaded with the composite CERCER fuel, where fuel particles are incorporated in a ceramic magnesia matrix. The results of this study offer additional information for the EFIT fuel selection.

  16. 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.

  17. 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.

  18. Characterization of ^{239,240}Pu Radionuclide Adsorption to Soil Particles and Mineral Dust Aerosols

    NASA Astrophysics Data System (ADS)

    Tatro, D. P.; Arimoto, R.; McMillan, N. J.; Barnes, M.

    2006-12-01

    The release of ^{239,240}Pu into the environment by nuclear weapons testing 50 years ago initiated the cyclic mobilization of Pu-contaminated soil particles via the resuspension of dust resulting in a widespread distribution of Pu and other radionuclides. It is unclear what enables the aeolian transport of Pu in the environment; plausible hypotheses of Pu binding to dust and soil particles include Pu adsorption to iron oxides/hydroxides, organic acids, or silicate minerals such as clays. To investigate the connections between surface soils, dust and radionuclides, samples of soil and/or dust were collected from the Project Gnome Site in Eddy County, NM, the Jemez Mountains near Los Alamos, NM, and two 50-year old attics and wind-blown dust in Big Spring, TX. This study tests the hypothesis that Pu is adsorbed onto Fe oxides and hydroxides that coat dust/soil particles. The samples are generally low in organic carbon (0.2 - 4.8%, except for the unburned Los Alamos sample at 9.4%), as measured by LOI (Loss On Ignition) at 360 °C. The citrate-bicarbonate-dithionite method (CDB) of Fe oxide removal, first proposed by Mehra and Jackson in 1960, was used to selectively extract Fe oxides from the samples while leaving silicate Fe intact. Chemical digestion of each sample creates two fractions, the extracted supernatant and a solid pellet residue. If the Pu were associated with Fe oxides, then Fe and Pu should both be selectively removed from the bulk sample during the CBD process, leaving the pellet depleted in Fe and Pu and the supernatant enriched. For Fe, this was confirmed by scanning electron microscope and petrographic analyses. Preliminary radiochemical analyses of Pu activity also verify this hypothesis. Pu activity is significantly lower in pellets than bulk samples (Pu activitypellet/Pu activitybulk average = 0.07, range 0.02-0.12); Pu activity in supernatants is significantly higher than in bulk samples (Pu activitysupernatant/Pu activitybulk average = 4

  19. Historical Review of U.S. Transient Fast Reactor Fuel Testing

    SciTech Connect

    Carmack, William J.; MacLean, Heather J.; Crawford, Douglas C.

    2007-07-01

    Development of fast spectrum nuclear fuels in the United States has been pursued over the course of approximately 30 years including the EBR-I and FERMI reactors and continuing through the early 1990's culminating with the FFTF and the EBR-II Integral Fast Reactor programs. These programs primarily focused on oxide and metallic fuels and the development process provided sufficient evidence for licensing of the 20%Pu-MOX oxide fuel and the ternary U-Pu-Zr metallic alloy. The development of a transuranic, actinide burning fuel system will require significant development including the investigation and testing of the behavior of candidate fuel systems under transient conditions. This paper will review the historical status of both metallic and oxide fuel transient testing completed under previous U.S. fast reactor fuel development programs. (authors)

  20. Final assessment of MOX fuel performance experiment with Japanese PWR specification fuel in the HBWR

    SciTech Connect

    Fujii, Hajime; Teshima, Hideyuki; Kanasugi, Katsumasa; Kosaka, Yuji; Arakawa, Yasushi

    2007-07-01

    In order to obtain high burn-up MOX fuel irradiation performance data, SBR and MIMAS MOX fuel rods with Pu-fissile enrichment of about 6 wt% had been irradiated in the HBWR from 1995 to 2006. The peak burn-up of MOX pellet achieved 72 GWd/tM. In this test, fuel centerline temperature, rod internal pressure, stack length and cladding length were measured for MOX fuel and UO{sub 2} fuel as reference. MOX fuel temperature is confirmed to have no significant difference in comparison with UO{sub 2}, taking into account of adequate thermal conductivity degradation due to PuO{sub 2} addition and burn-up development. And the measured fuel temperature agrees well with FINE code calculation up to high burn-up region. Fission gas release of MOX is possibly greater than UO{sub 2} based on temperature and pressure assessment. No significant difference is confirmed between SBR and MIMAS MOX on FGR behavior. MOX fuel swelling rate agrees well with solid swelling rate in the literature. Cladding elongation data shows onset of PCMI in high power region. (authors)

  1. 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

  2. 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.

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

    DOE PAGESBeta

    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

  4. 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.

  5. 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

  6. Bacterial Pu(V) reduction in the absence and presence of Fe(III)-NTA: modeling and experimental approach.

    PubMed

    Deo, Randhir P; Rittmann, Bruce E; Reed, Donald T

    2011-09-01

    Plutonium (Pu), a key contaminant at sites associated with the manufacture of nuclear weapons and with nuclear-energy wastes, can be precipitated to "immobilized" plutonium phases in systems that promote bioreduction. Ferric iron (Fe(3+)) is often present in contaminated sites, and its bioreduction to ferrous iron (Fe(2+)) may be involved in the reduction of Pu to forms that precipitate. Alternately, Pu can be reduced directly by the bacteria. Besides Fe, contaminated sites often contain strong complexing ligands, such as nitrilotriacetic acid (NTA). We used biogeochemical modeling to interpret the experimental fate of Pu in the absence and presence of ferric iron (Fe(3+)) and NTA under anaerobic conditions. In all cases, Shewanella alga BrY (S. alga) reduced Pu(V)(PuO(2) (+)) to Pu(III), and experimental evidence indicates that Pu(III) precipitated as PuPO(4(am).) In the absence of Fe(3+) and NTA, reduction of PuO(2) (+) was directly biotic, but modeling simulations support that PuO(2) (+) reduction in the presence of Fe(3+) and NTA was due to an abiotic stepwise reduction of PuO(2) (+) to Pu(4+), followed by reduction of Pu(4+) to Pu(3+), both through biogenically produced Fe(2+). This means that PuO(2) (+) reduction was slowed by first having Fe(3+) reduced to Fe(2+). Modeling results also show that the degree of PuPO(4(am)) precipitation depends on the NTA concentration. While precipitation out-competes complexation when NTA is present at the same or lower concentration than Pu, excess NTA can prevent precipitation of PuPO(4(am)). PMID:21234648

  7. 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.

  8. The transcription factor PU.1 promotes alternative macrophage polarization and asthmatic airway inflammation.

    PubMed

    Qian, Feng; Deng, Jing; Lee, Yong Gyu; Zhu, Jimmy; Karpurapu, Manjula; Chung, Sangwoon; Zheng, Jun-Nian; Xiao, Lei; Park, Gye Young; Christman, John W

    2015-12-01

    The transcription factor PU.1 is involved in regulation of macrophage differentiation and maturation. However, the role of PU.1 in alternatively activated macrophage (AAM) and asthmatic inflammation has yet been investigated. Here we report that PU.1 serves as a critical regulator of AAM polarization and promotes the pathological progress of asthmatic airway inflammation. In response to the challenge of DRA (dust mite, ragweed, and Aspergillus) allergens, conditional PU.1-deficient (PU/ER(T)(+/-)) mice displayed attenuated allergic airway inflammation, including decreased alveolar eosinophil infiltration and reduced production of IgE, which were associated with decreased mucous glands and goblet cell hyperplasia. The reduced asthmatic inflammation in PU/ER(T)(+/-) mice was restored by adoptive transfer of IL-4-induced wild-type (WT) macrophages. Moreover, after treating PU/ER(T)(+/-) mice with tamoxifen to rescue PU.1 function, the allergic asthmatic inflammation was significantly restored. In vitro studies demonstrate that treatment of PU.1-deficient macrophages with IL-4 attenuated the expression of chitinase 3-like 3 (Ym-1) and resistin-like molecule alpha 1 (Fizz-1), two specific markers of AAM polarization. In addition, PU.1 expression in macrophages was inducible in response to IL-4 challenge, which was associated with phosphorylation of signal transducer and activator of transcription 6 (STAT6). Furthermore, DRA challenge in sensitized mice almost abrogated gene expression of Ym-1 and Fizz-1 in lung tissues of PU/ER(T)(+/-) mice compared with WT mice. These data, all together, indicate that PU.1 plays a critical role in AAM polarization and asthmatic inflammation. PMID:26101328

  9. 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.

  10. Automated homogeneous oxalate precipitation of Pu(III)

    SciTech Connect

    Yarbro, S.L.; Schreiber, S.B.; Dunn, S.L.; Mills, C.W.

    1990-01-01

    Homogeneous oxalate precipitation using diethyl oxalate was compared to precipitating Pu(III) oxalate with solid oxalic acid. The diethyl oxalate technique at 75{degree}C is better because it gives 50% less plutonium in the filtrate with a reasonable filtering time. Also, the procedure for the homogeneous precipitation is easier to automate because the liquid diethyl oxalate is simpler to introduce into the precipitator than solid oxalic acid. It also provides flexibility because the hydrolysis rate and therefore the precipitation rate can be controlled by varying the temperature. 5 refs., 3 figs., 3 tabs.

  11. 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.

  12. Shubnikov-de Haas oscillation in PuIn3

    NASA Astrophysics Data System (ADS)

    Haga, Yoshinori; Bauer, Eric D.; Tobash, Paul H.; Mitchell, Jeremy N.; Ayala-Valenzuela, Oscar; McDonald, Ross D.; Mielke, Charles H.; Fisk, Zachary

    2013-08-01

    The Fermi surface of PuIn3 is investigated using flux-grown single crystals. Shubnikov-de Haas (SdH) oscillations were detected by means of the skin-depth measurement using a proximity-detector-oscillator circuit. Angular dependence of the SdH frequency which corresponds to the extremal cross-sectional area of Fermi surface agrees well with the previous magnetic susceptibility measurement using conventional field-modulation method. The SdH oscillation suddenly vanishes when the magnetic field is tilted from the cubic [111] direction.

  13. 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.

  14. 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.

  15. Normalization of the [sup 239]Pu fission cross section

    SciTech Connect

    Wagemans, C.; Van Uffelen, P.; Deruytter, A.; Barthelemy, R.; Van Gils, J. . Joint Research Centre)

    1993-10-01

    Measurements have been performed at the Geel Linear Accelerator from 0.01 eV up to 1,000 eV in order to investigate the normalization of [sup 239]Pu fission cross-section measurements. Two different experiments were performed using surface barrier detectors and a double ionization chamber, respectively. In both cases, the [sup 10]B(n, [alpha]) reaction was used as a flux monitor. The results indicate that the Weston and Todd data should be renormalized by [approximately]3%, resulting in a satisfactory agreement with ENDF/B-VI.

  16. First-principles elastic properties of (alpha)-Pu

    SciTech Connect

    Soderlind, P; Klepeis, J

    2009-02-18

    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 antiferromagnetic treatment with a generalized gradient approximation for the electron exchange and correlation functional. 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 recent resonant ultrasound spectroscopy for a cast sample is made.

  17. Activity ratios of 137Cs, 90Sr and 239+240Pu in environmental samples.

    PubMed

    Bossew, P; Lettner, H; Hubmer, A; Erlinger, C; Gastberger, M

    2007-01-01

    Both global and Chernobyl fallout have resulted in environmental contamination with radionuclides such as 137Cs, 90Sr and 239+240Pu. In environmental samples, 137Cs and 239+240Pu can be divided into the contributions of either source, if also the isotopes 134Cs and 238Pu are measurable, based on the known isotopic ratios in global and Chernobyl fallout. No analogous method is available for 90Sr. The activity ratios of Sr to Cs and Pu, respectively, are known for the actual fallout mainly from air filter measurements; but due to the high mobility of Sr in the environment, compared to Cs and Pu, these ratios generally do not hold for the inventory many years after deposition. In this paper we suggest a method to identify the mean contributions of global and Chernobyl fallout to total Sr in soil, sediment and cryoconite samples from Alpine and pre-Alpine regions of Austria, based on a statistical evaluation of Sr/Cs/Pu radionuclide activity ratios. Results are given for Sr:Cs, Sr:Pu and Cs:Pu ratios. Comparison with fallout data shows a strong depletion of Sr against Cs and Pu. PMID:17407799

  18. 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.

  19. Pharmacologic efficacy of PU.1 inhibition by heterocyclic dications: a mechanistic analysis.

    PubMed

    Stephens, Dominique C; Kim, Hye Mi; Kumar, Arvind; Farahat, Abdelbasset A; Boykin, David W; K Poon, Gregory M

    2016-05-19

    Heterocyclic dications are receiving increasing attention as targeted inhibitors of transcription factors. While many dications act as purely competitive inhibitors, some fail to displace protein efficiently at drug concentrations expected to saturate their DNA target. To achieve a mechanistic understanding of these non-competitive effects, we used a combination of dications, which are intrinsically fluorescent and spectrally-separated fluorescently labeled DNA to dissect complex interactions in multi-component drug/DNA/protein systems. Specifically, we interrogated site-specific binding by the transcription factor PU.1 and its perturbation by DB270, a furan-bisbenzimidazole-diamidine that strongly targets PU.1 binding sites yet poorly inhibits PU.1/DNA complexes. By titrating DB270 and/or cyanine-labeled DNA with protein or unlabeled DNA, and following the changes in their fluorescence polarization, we found direct evidence that DB270 bound protein independently of their mutual affinities for sequence-specific DNA. Each of the three species competed for the other two, and this interplay of mutually dependent equilibria abrogated DB270's inhibitory activity, which was substantively restored under conditions that attenuated DB270/PU.1 binding. PU.1 binding was consistent with DB270's poor inhibitory efficacy of PU.1 in vivo, while its isosteric selenophene analog (DB1976), which did not bind PU.1 and strongly inhibited the PU.1/DNA complex in vitro, fully antagonized PU.1-dependent transactivation in vivo. PMID:27079976

  20. 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

    2016-07-01

    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. PMID:27244483

  1. Pharmacologic efficacy of PU.1 inhibition by heterocyclic dications: a mechanistic analysis

    PubMed Central

    Stephens, Dominique C.; Kim, Hye Mi; Kumar, Arvind; Farahat, Abdelbasset A.; Boykin, David W.; K. Poon, Gregory M.

    2016-01-01

    Heterocyclic dications are receiving increasing attention as targeted inhibitors of transcription factors. While many dications act as purely competitive inhibitors, some fail to displace protein efficiently at drug concentrations expected to saturate their DNA target. To achieve a mechanistic understanding of these non-competitive effects, we used a combination of dications, which are intrinsically fluorescent and spectrally-separated fluorescently labeled DNA to dissect complex interactions in multi-component drug/DNA/protein systems. Specifically, we interrogated site-specific binding by the transcription factor PU.1 and its perturbation by DB270, a furan-bisbenzimidazole-diamidine that strongly targets PU.1 binding sites yet poorly inhibits PU.1/DNA complexes. By titrating DB270 and/or cyanine-labeled DNA with protein or unlabeled DNA, and following the changes in their fluorescence polarization, we found direct evidence that DB270 bound protein independently of their mutual affinities for sequence-specific DNA. Each of the three species competed for the other two, and this interplay of mutually dependent equilibria abrogated DB270's inhibitory activity, which was substantively restored under conditions that attenuated DB270/PU.1 binding. PU.1 binding was consistent with DB270's poor inhibitory efficacy of PU.1 in vivo, while its isosteric selenophene analog (DB1976), which did not bind PU.1 and strongly inhibited the PU.1/DNA complex in vitro, fully antagonized PU.1-dependent transactivation in vivo. PMID:27079976

  2. Adsorption of Pu(IV) Polymer onto 304L Stainless Steel

    SciTech Connect

    Bronikowski, M.G.

    1999-07-16

    'The report, Technical Basis for Safe Operations with Pu-239 Polymer in NMS&S Operating Facilities (F & H Areas), (WSRC-TR-99-00008) was issued in an effort to upgrade the Authorization Basis (AB) for H Area facilities relative to nuclear criticality. At the time, insufficient data were found in the literature to quantify the adsorption of Pu polymer onto the surfaces of stainless steel tanks. Additional experimental or literature information on the adsorption of Pu(IV) polymer and its removal was deemed necessary to support the H Area AB. The results obtained are also applicable to processing in F Area facilities.Additional literature sources suggest that adsorption on the tank walls should not be a safety concern. The sources show that the amount of Pu polymer that adsorbs from a solution comes to a limiting amount in 5 to 7 days after which no additional Pu is adsorbed. Adsorption increases with Pu concentration and decreases with acid concentration. The adsorbed amounts are small varying from 0.5 mg/cm2 for a 0.5 g/l Pu / 0.5M HNO3 solution to 11 mg/cm2 for a 1-3 g/l Pu / 0.1M HNO3 solution. Additionally, acid concentrations greater than 0.1M will remove a percentage of adsorbed Pu.The experimental results have generally confirmed much of what has been reported in the literature. Specifically, adsorption onto stainless steel was found to increase with increased Pu concentration, and decreased acid concentration. The amount adsorbed was found to come to a limiting amount after 5 to 7 days. Pu adsorbed as polymer was found to be harder to remove than if it was adsorbed as Pu(IV). The amount of Pu adsorbed as polymer was found to be almost an order of magnitude more than that from a similar concentration Pu(IV) solution. Unlike the literature, only a slight increase in adsorption values was found when the steel surface was removed, dried, and replaced in the Pu solution. The amount of Pu as polymer which would adsorb onto the surface of a 14,000L tank was

  3. Adsorption of Pu(IV) Polymer onto 304L Stainless Steel

    SciTech Connect

    Bronikowski, M.G.

    1999-07-16

    'The report, Technical Basis for Safe Operations with Pu-239 Polymer in NMS S Operating Facilities (F H Areas), (WSRC-TR-99-00008) was issued in an effort to upgrade the Authorization Basis (AB) for H Area facilities relative to nuclear criticality. At the time, insufficient data were found in the literature to quantify the adsorption of Pu polymer onto the surfaces of stainless steel tanks. Additional experimental or literature information on the adsorption of Pu(IV) polymer and its removal was deemed necessary to support the H Area AB. The results obtained are also applicable to processing in F Area facilities.Additional literature sources suggest that adsorption on the tank walls should not be a safety concern. The sources show that the amount of Pu polymer that adsorbs from a solution comes to a limiting amount in 5 to 7 days after which no additional Pu is adsorbed. Adsorption increases with Pu concentration and decreases with acid concentration. The adsorbed amounts are small varying from 0.5 mg/cm2 for a 0.5 g/l Pu / 0.5M HNO3 solution to 11 mg/cm2 for a 1-3 g/l Pu / 0.1M HNO3 solution. Additionally, acid concentrations greater than 0.1M will remove a percentage of adsorbed Pu.The experimental results have generally confirmed much of what has been reported in the literature. Specifically, adsorption onto stainless steel was found to increase with increased Pu concentration, and decreased acid concentration. The amount adsorbed was found to come to a limiting amount after 5 to 7 days. Pu adsorbed as polymer was found to be harder to remove than if it was adsorbed as Pu(IV). The amount of Pu adsorbed as polymer was found to be almost an order of magnitude more than that from a similar concentration Pu(IV) solution. Unlike the literature, only a slight increase in adsorption values was found when the steel surface was removed, dried, and replaced in the Pu solution. The amount of Pu as polymer which would adsorb onto the surface of a 14,000L tank was estimated

  4. 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.

  5. 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.

  6. 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

  7. Free energy of formation of Cs{sub 3}PuCl{sub 6} and CsPu{sub 2}Cl{sub 7}

    SciTech Connect

    Willamson, M.A.; Kleinschmidt, P.D.

    1992-09-01

    The free energy, enthalpy and entropy of formation of the compounds Cs{sub 3}PuCl{sub 6} and CsPu{sub 2}Cl{sub 7} have been determined by measuring the sublimation pressures for the reactions: CsCl(s) = CsCl(g), 2/5 Cs{sub 3}PuCl{sub 6}(s) = 1/5 CsPu{sub 2}Cl{sub 7}(s) + CsCl(g), and CsPu{sub 2}Cl{sub 7}(s) = 2 PuCl{sub 3}(s) + CsCl(g). The pressures are measured using Knudsen effusion mass spectrometry over the temperature range 600 to 850 K. For the formation of Cs{sub 3}PuCl{sub 6} from CsCl and PuCl{sub 3}, {Delta}G{sub 298}{sup 0} = {minus}77.3 +/{minus} 8.5 kJ/mole, {Delta}H{sub 298}{sup 0} = {minus}82.1 +/{minus} 7.8 kJ mole, and {Delta}S{sup 298}{sup 0} = {minus}16.2 +/{minus} 10.9 J/K mole. For CsPu{sub 2}Cl{sub 7}, {Delta}G{sub 298}{sup 0} = {minus}39.4 +/{minus} 3.5 kJ/mole, {Delta}H{sub 298}{sup 0} = {minus}40.8 +/{minus} 3.2 kJ/mole, and {Delta}S{sub 298}{sup 0} = {minus}4.6 +/{minus} 4.2 J/K mole.

  8. Free energy of formation of Cs sub 3 PuCl sub 6 and CsPu sub 2 Cl sub 7

    SciTech Connect

    Willamson, M.A.; Kleinschmidt, P.D.

    1992-01-01

    The free energy, enthalpy and entropy of formation of the compounds Cs{sub 3}PuCl{sub 6} and CsPu{sub 2}Cl{sub 7} have been determined by measuring the sublimation pressures for the reactions: CsCl(s) = CsCl(g), 2/5 Cs{sub 3}PuCl{sub 6}(s) = 1/5 CsPu{sub 2}Cl{sub 7}(s) + CsCl(g), and CsPu{sub 2}Cl{sub 7}(s) = 2 PuCl{sub 3}(s) + CsCl(g). The pressures are measured using Knudsen effusion mass spectrometry over the temperature range 600 to 850 K. For the formation of Cs{sub 3}PuCl{sub 6} from CsCl and PuCl{sub 3}, {Delta}G{sub 298}{sup 0} = {minus}77.3 +/{minus} 8.5 kJ/mole, {Delta}H{sub 298}{sup 0} = {minus}82.1 +/{minus} 7.8 kJ mole, and {Delta}S{sup 298}{sup 0} = {minus}16.2 +/{minus} 10.9 J/K mole. For CsPu{sub 2}Cl{sub 7}, {Delta}G{sub 298}{sup 0} = {minus}39.4 +/{minus} 3.5 kJ/mole, {Delta}H{sub 298}{sup 0} = {minus}40.8 +/{minus} 3.2 kJ/mole, and {Delta}S{sub 298}{sup 0} = {minus}4.6 +/{minus} 4.2 J/K mole.

  9. Transfer of aged 239+240Pu, 238Pu, 241Am, and 137Cs to cattle grazing a contaminated arid environment.

    PubMed

    Gilbert, R O; Engel, D W; Anspaugh, L R

    1989-09-01

    In this paper, estimates are obtained of the fraction of ingested 239+240Pu, 238Pu, 241Am and 137Cs transferred to blood, muscle, liver, kidney, femur, vertebra, and gonads of a reproducing herd of 17 beef cattle, individuals of which grazed within fenced enclosures for up to 1064 days under natural conditions with no supplemental feeding at an arid site contaminated 16 years previously with transuranic radionuclides. The estimated geometric mean (GM) GI-to-blood fractional transfer of 238Pu (0.0001) was about 20 times larger than the estimated transfer of 239+240Pu (0.000005), while the estimated transfer of 241Am (0.00001) was about 2 times larger than that of 239+240Pu. These GM GI-to-blood transfers were smaller than the GI-to-blood transfer value of 0.001 recommended by the International Commission on Radiological Protection (ICRP) for humans exposed via food chains or occupationally from unknown mixtures or compounds of plutonium and americium. Statistical tests indicated significantly (p less than 0.05) larger GI-to-tissue transfers of (1) 238Pu as compared to 239+240Pu for all tissues examined, (2) of 238Pu as compared to 241Am for muscle, liver, femur, and vertebra, and (3) of 241Am as compared to 239+240Pu for blood serum, femur, and kidney. The estimated GM fractional transfers of 137Cs from GI to muscle and liver were 0.03 (n = 8) and 0.001 (n = 3), respectively, assuming a 50-day biological half-time of 137Cs in cattle tissue. PMID:2814465

  10. Nitride fuels irradiation performance data base

    SciTech Connect

    Brozak, D.E.; Thomas, J.K.; Peddicord, K.L.

    1987-01-01

    An irradiation performance data base for nitride fuels has been developed from an extensive literature search and review that emphasized uranium nitride, but also included performance data for mixed nitrides ((U,Pu)N) and carbonitrides ((U,Pu)C,N) to increase the quantity and depth of pin data available. This work represents a very extensive effort to systematically collect and organize irradiation data for nitride-based fuels. The data base has many potential applications. First, it can facilitate parametric studies of nitride-based fuels to be performed using a wide range of pin designs and operating conditions. This should aid in the identification of important parameters and design requirements for multimegawatt and SP-100 fuel systems. Secondly, the data base can be used to evaluate fuel performance models. For detailed studies, it can serve as a guide to selecting a small group of pin specimens for extensive characterization. Finally, the data base will serve as an easily accessible and expandable source of irradiation performance information for nitride fuels.

  11. Indication of single-crystal PuO2 oxidation from O 1s x-ray absorption spectra

    NASA Astrophysics Data System (ADS)

    Modin, A.; Yun, Y.; Suzuki, M.-T.; Vegelius, J.; Werme, L.; Nordgren, J.; Oppeneer, P. M.; Butorin, S. M.

    2011-02-01

    The electronic structure of single-crystal PuO2 is studied using O 1s x-ray absorption (XA) and x-ray emission. Interpretation of the experimental data is supported by extensive first-principles calculations on the basis of the densityfunctionaltheory+U approach. The measured XA spectra show a significant difference in intensity for the first two peaks between different spots or areas on the single crystal. Our theoretical simulations show that the first peak, at ~531 eV, can be attributed to O 2p-Pu 5f hybridization, while the second peak, at ~533.4 eV, is due to hybridization of O 2p with Pu d states. The reasons for the observed differences in the O 1s XA spectra are explored by calculating a number of defect structures PuO2±x as well as by simulating the existence of Pu(V) sites. Our results indicate the presence of oxidation states higher than Pu(IV) in some areas of the single crystal. The findings also suggest that plutonium oxide with a Pu fraction in an oxidation state higher than Pu(IV) consists of inequivalent Pu sites with Pu(IV)O2 and Pu(V)O2 rather than representing a system where the Pu oxidation state is constantly fluctuating between Pu(IV) and Pu(V).

  12. Genome-scale definition of the transcriptional programme associated with compromised PU.1 activity in acute myeloid leukaemia.

    PubMed

    Sive, J I; Basilico, S; Hannah, R; Kinston, S J; Calero-Nieto, F J; Göttgens, B

    2016-01-01

    Transcriptional dysregulation is associated with haematological malignancy. Although mutations of the key haematopoietic transcription factor PU.1 are rare in human acute myeloid leukaemia (AML), they are common in murine models of radiation-induced AML, and PU.1 downregulation and/or dysfunction has been described in human AML patients carrying the fusion oncogenes RUNX1-ETO and PML-RARA. To study the transcriptional programmes associated with compromised PU.1 activity, we adapted a Pu.1-mutated murine AML cell line with an inducible wild-type PU.1. PU.1 induction caused transition from leukaemia phenotype to monocytic differentiation. Global binding maps for PU.1, CEBPA and the histone mark H3K27Ac with and without PU.1 induction showed that mutant PU.1 retains DNA-binding ability, but the induction of wild-type protein dramatically increases both the number and the height of PU.1-binding peaks. Correlating chromatin immunoprecipitation (ChIP) Seq with gene expression data, we found that PU.1 recruitment coupled with increased histone acetylation induces gene expression and activates a monocyte/macrophage transcriptional programme. PU.1 induction also caused the reorganisation of a subgroup of CEBPA binding peaks. Finally, we show that the PU.1 target gene set defined in our model allows the stratification of primary human AML samples, shedding light on both known and novel AML subtypes that may be driven by PU.1 dysfunction. PMID:26126967

  13. Reaction of plutonium with water kinetic and equilibrium behavior of binary and ternary phases in the Pu + O + H system

    SciTech Connect

    Haschke, J.M.; Hodges, A.E. III; Bixby, G.E.; Lucas, R.L.

    1983-02-03

    The kinetic and equilibrium behavior of the Pu + O + H system has been studied by measuring the production of hydrogen gas formed by a sequence of hydrolysis reactions. The kinetic dependence of the Pu + H/sub 2/O reaction on salt concentration and temperature has been defined. The metal is quantitatively converted to a fine black powder which has been identified as plutonium monoxide monohydride, PuOH. Other hydrolysis products formed in aqueous media include a second oxide hydride, Pu/sub 7/O/sub 9/H/sub 3/, and the oxides Pu/sub 2/O/sub 3/, Pu/sub 7/O/sub 12/, Pu/sub 9/O/sub 16/, Pu/sub 10/O/sub 18/, Pu/sub 12/O/sub 22/, and PuO/sub 2/. Thermal decomposition products of PuOH include Pu/sub 2/O/sub 2/H and PuO. A tentative phase diagram for Pu + O + H is presented and structural relationships of the oxide hydrides and oxides are discussed. 10 figures, 5 tables.

  14. 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. PMID:24144889

  15. Genome-scale definition of the transcriptional programme associated with compromised PU.1 activity in acute myeloid leukaemia

    PubMed Central

    Sive, J I; Basilico, S; Hannah, R; Kinston, S J; Calero-Nieto, F J; Göttgens, B

    2016-01-01

    Transcriptional dysregulation is associated with haematological malignancy. Although mutations of the key haematopoietic transcription factor PU.1 are rare in human acute myeloid leukaemia (AML), they are common in murine models of radiation-induced AML, and PU.1 downregulation and/or dysfunction has been described in human AML patients carrying the fusion oncogenes RUNX1-ETO and PML-RARA. To study the transcriptional programmes associated with compromised PU.1 activity, we adapted a Pu.1-mutated murine AML cell line with an inducible wild-type PU.1. PU.1 induction caused transition from leukaemia phenotype to monocytic differentiation. Global binding maps for PU.1, CEBPA and the histone mark H3K27Ac with and without PU.1 induction showed that mutant PU.1 retains DNA-binding ability, but the induction of wild-type protein dramatically increases both the number and the height of PU.1-binding peaks. Correlating chromatin immunoprecipitation (ChIP) Seq with gene expression data, we found that PU.1 recruitment coupled with increased histone acetylation induces gene expression and activates a monocyte/macrophage transcriptional programme. PU.1 induction also caused the reorganisation of a subgroup of CEBPA binding peaks. Finally, we show that the PU.1 target gene set defined in our model allows the stratification of primary human AML samples, shedding light on both known and novel AML subtypes that may be driven by PU.1 dysfunction. PMID:26126967

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

    PubMed

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

    1997-08-25

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

  17. 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.

  18. Radiation damage effects in candidate titanates for Pu disposition: Zirconolite

    NASA Astrophysics Data System (ADS)

    Strachan, D. M.; Scheele, R. D.; Buck, E. C.; Kozelisky, A. E.; Sell, R. L.; Elovich, R. J.; Buchmiller, W. C.

    2008-01-01

    Results from studies of radiation-induced damage from the alpha decay of 238Pu on the density and crystal structure of a nominally phase-pure zirconolite and two other zirconolite-bearing ceramics are discussed. Macro and micro swelling were found to be temperature independent, whereas the density determined with He gas pycnometry was temperature dependent. Approximately 2.6 × 10 18 α/g were needed to render the specimens X-ray amorphous- more to saturate the swelling. Unlike pyrochlore-based ceramics, we did not observe any phase changes associated with storage temperature and damage ingrowth. The forward dissolution rate at a pH value of 2 for material containing essentially all zirconolite is 1.7(4) × 10 -3 g/(m 2 d) with very little pH dependence and no dependence on the amount of radiation-induced damage. Even after the radiation-induced swelling saturated, the specimens remained physically intact with no evidence for microcracking. Thus, the material remains physically a viable material for the disposition of surplus weapons-grade Pu.

  19. 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.

  20. 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.

  1. Neutronics Benchmarks for the Utilization of Mixed-Oxide Fuel: Joint U.S./Russian Progress Report for Fiscal Year 1997

    SciTech Connect

    Akkurt, H

    2001-01-11

    In 1967, a series of critical experiments were conducted at the Westinghouse Reactor Evaluation Center (WREC) using mixed-oxide (MOX) PuO{sub 2}-UO{sub 2} and/or UO{sub 2} fuels in various lattices and configurations . These experiments were performed under the joint sponsorship of the Empire State Atomic Development Associates (ESADA) plutonium program and Westinghouse . The purpose of these experiments was to develop experimental data to validate analytical methods used in the design of a plutonium-bearing replacement fuel for water reactors. Three different fuels were used during the experimental program: two MOX fuels and a low-enriched UO{sub 2} fuel. The MOX fuels were distinguished by their {sup 240}Pu content: 8 wt% {sup 240}Pu and 24 wt% {sup 240}Pu. Both MOX fuels contained 2.0 wt % PuO{sub 2} in natural UO{sub 2} . The UO{sub 2} fuel with 2.72 wt % enrichment was used for comparison with the plutonium data and for use in multiregion experiments.

  2. 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. PMID:23770554

  3. Structure of mixed U(IV)-An(III) precursors synthesized by co-conversion methods (where An = Pu, Am or Cm)

    NASA Astrophysics Data System (ADS)

    Grandjean, S.; Arab-Chapelet, B.; Robisson, A. C.; Abraham, F.; Martin, Ph.; Dancausse, J.-Ph.; Herlet, N.; Léorier, C.

    2009-03-01

    Current concepts for future nuclear systems aim at improving the fuel cycle with the main following criteria: economy of resources, minimized volume and lower long-term potential radiotoxicity of ultimate wastes and proliferation risk reduction. Co-management of two (or more) actinides has recently been proposed for recycling reusable energy-producing actinides (mainly U and Pu) together, or for transmuting radiotoxic minor actinides within UO 2-based materials. Co-conversion processes play an important role by closing the actinide separation-purification operations and at the same time producing mixed actinide solid compounds for the fabrication of fresh fuel. Handling of actinides mixtures, from the initial solution up to the solid product, requires innovative synthesis methods and structures, particularly for the minor actinides such as americium and curium. Considering the different designs of future nuclear fuels, various uranium-actinide co-conversion routes are currently investigated in the CEA-ATALANTE facility.

  4. Opportunity fuels

    SciTech Connect

    Lutwen, R.C.

    1994-12-31

    Opportunity fuels - fuels that can be converted to other forms of energy at lower cost than standard fossil fuels - are discussed in outline form. The type and source of fuels, types of fuels, combustability, methods of combustion, refinery wastes, petroleum coke, garbage fuels, wood wastes, tires, and economics are discussed.

  5. 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.

  6. 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.

  7. 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.

  8. Critical experiments with mixed plutonium-uranium nitrate solutions having Pu:(Pu + U) ratios greater than 0.5

    SciTech Connect

    Primm, R.T. III; Lloyd, R.C.; Clayton, E.D.

    1986-04-01

    A series of critical experiments was conducted with mixed plutonium-uranium nitrate solutions having Pu:(Pu+U) ratios >0.5. Three geometries and four conditions of reflection were examined. The plutonium concentrations ranged from 170 to 350 g/L. The value of k-effective for each experiment was calculated using the KENO-IV code and 27-group cross sections derived from the Evaluated Nuclear Data File B--version IV (ENDF/B-IV). The mean value for the set of 26 experiments was 1.003, with a minimum value of 0.987 and a maximum of 1.022. The spread in the distribution of calculated k-effectives is believed to be the result of uncertainties in analytical chemistry measurements. No correlation between condition of reflection and calculated k-effective was found. An allowable multiplication factor to be used in the evaluation of reprocessing equipment at conditions that have been investigated was calculated to be 0.945.

  9. 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. PMID:16124281

  10. Antibacterial property and mechanism of a novel Pu-erh tea nanofibrous membrane.

    PubMed

    Su, Yajuan; Zhang, Chenlu; Wang, Yan; Li, Ping

    2012-02-01

    Pu-erh tea is made via a natural fermentation process. In this study, Pu-erh tea was used as a raw material for nanomaterials preparation and as an antibacterial agent. Antibacterial activities on Escherichia coli of Pu-erh tea, Pu-erh tea powder (PTP) of different sizes, and Pu-erh tea residual powder were firstly determined, respectively. With polyvinyl alcohol as the carrier, through an electrospinning technique, different kinds of nanofibrous membranes were obtained from the extract of Pu-erh tea and nano-PTP (NPTP), and their antibacterial properties and mechanism against E. coli were evaluated. The results showed better antibacterial activity with smaller PTP particles, the nano-sized particles had the best effects, and the MIC of NPTP was 13.5 mg/mL. When NPTP was in nanofibrous membranes, the antibacterial activity decreased slightly, but increased with modification by ZnO. Pu-erh tea in nanofibrous membranes damaged the E. coli cell membranes and caused leakage of K(+) and enzymes. What is more is that damage of the cell walls led to the leakage of fluorescent proteins from enhanced green fluorescence protein-expressing E. coli. These results indicate that the Pu-erh tea nanofibrous membranes had good antibacterial activities against E. coli, which may provide a promising application of novel antibacterial materials. PMID:21858494

  11. 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%).

  12. 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

  13. 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.

  14. Pu(V)O2+ adsorption and reduction by synthetic magnetite (Fe3O4).

    PubMed

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

    2004-11-15

    Changes in aqueous- and solid-phase Pu oxidation state were monitored over time in magnetite (Fe3O4) suspensions containing 239Pu(V)-amended 0.01 M NaCl. Oxidation state distribution was determined by leaching of Pu into an aqueous phase followed by an ultrafiltration/solvent extraction technique. The capability of the technique to measure Pu oxidation state distribution was verified using 230Th(IV), 237Np(V), and 233U(VI) as oxidation state analogues. Reduction of Pu(V) was observed at all pH values (pH 3 to 8) and magnetite concentrations (10 to 100 m2 L(-1)). In the pH range 5 to 8, adsorption was a rate-limiting step, and reduction was mediated by the solid phase; at pH 3 reduction occurred in the aqueous phase. The overall reaction (describing both adsorption and reduction of Pu(V)) was found to be approximately first order with respect to the magnetite concentration and of order -0.34+/-0.02 with respect to the hydrogen ion concentration. Assuming first order dependence with respect to Pu, the overall reaction rate constant was calculated as k(rxn) = 4.79+/-0.62 x 10(-8) (m(-2) L)0.99(mol(-1) L)-0.34(s(-1)). The Pu(IV) solid-phase species became more stable over time. PMID:15573601

  15. PU.1 can participate in an active enhancer complex without its transcriptional activation domain

    PubMed Central

    Pongubala, Jagan M. R.; Atchison, Michael L.

    1997-01-01

    The transcription factor PU.1 is necessary for the development of multiple hematopoietic lineages and contributes to the activity of the immunoglobulin κ 3′ enhancer. A variety of proteins bind to the 3′ enhancer (PU.1, PIP, ATF1, CREM, c-Fos, c-Jun, and E2A), but the mechanism of 3′-enhancer activity and the proteins necessary for its activity are presently unclear. We show here that PU.1 participates with other transcription factors in forming a higher-order complex with 3′-enhancer DNA sequences. Each protein is necessary for formation of this complex. Individually, transcription factors that bind to the 3′ enhancer do not appreciably stimulate transcription in a cell type in which the 3′ enhancer is normally silent (NIH 3T3). However, mixture of multiple transcription factors (PU.1, PIP, c-Fos, and c-Jun) can greatly activate the enhancer. PU.1 is necessary for maximal enhancer activity, but mutants of PU.1 that lack the transcriptional activation domain are nearly as efficient at stimulating enhancer activity as the wild-type PU.1 protein. PU.1 apparently can activate transcription by playing an architectural role in interactions with other transcription factors. PMID:8990172

  16. 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.

  17. Plutonium-239, /sup 240/Pu and /sup 210/Po contents of tobacco and cigarette smoke

    SciTech Connect

    Mussalo-Rauhamaa, H.; Jaakkola, T.

    1985-08-01

    The /sup 239/Pu and /sup 240/Pu found in the environment has mainly been produced by atmospheric nuclear tests. The accumulation of fallout Pu in man from inhalation and ingestion and its distribution in the body has previously been studied. Information about the accumulation is needed because of the expanding production of this highly radiotoxic substance. In the present work the Pu content of tobacco and cigarette smoke was determined to evaluate the contribution of smoking to total Pu intake by man. For comparison the /sup 210/Po content of tobacco and smoke were analyzed. The release of /sup 210/Po in tobacco smoke and the radiation dose for man have been widely studied because of the high incidence of lung cancer among smokers.

  18. Neutron-induced Fission Cross Section of 240242Pu up to En = 3 MeV

    NASA Astrophysics Data System (ADS)

    Salvador-Castiñeira, P.; Bryś, T.; Hambsch, F.-J.; Oberstedt, S.; Pretel, C.; Vidali, M.

    2014-05-01

    The neutron-induced fission cross sections of 240,242Pu have been measured at JRC-IRMM with incident neutron energy from 0.2 MeV up to 3 MeV. A Twin-Frisch Grid Ionization Chamber (TFGIC) has been used in a back-to-back geometry. The measurements have been performed using the secondary standards 237Np and 238U as a reference. The purity of the plutonium samples was 99.89% for 240Pu and 99.97% for 242Pu. The results obtained follow the ENDF/B-VII.1 evaluation for 240Pu, but some discrepancies are visible around E/n = 1 MeV for 242Pu. In addition, the spontaneous fission half-life has been measured for both isotopes.

  19. 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.

  20. Prompt Gamma Emission in Resonance Neutron Induced Fission of 239Pu

    NASA Astrophysics Data System (ADS)

    Ruskov, I.; Kopatch, Yu. N.; Panteleev, Ts.; Skoy, V. R.; Shvetsov, V. N.; Dermendjiev, E.; Janeva, N.; Pikelner, L. B.; Grigoriev, Yu. V.; Mezentseva, Zh. V.; Ivanov, I.

    The scientific interest in the resonance neutron induced capture and fission reactions on 239Pu is continuously rising during the last decade. From a practical point of view, this is because more precise data on capture and fission cross sections, fission fragment mass and kinetic energy distributions, variation of prompt fission neutron and gamma yields in the resonance neutron region, are needed for the modelling of new generation nuclear power plants and for nuclear spent fuel and waste transmutation. From a heuristic and fundamental point of view, such a research improves our knowledge and understanding of the fission phenomena itself. To achieve these goals more powerful neutron sources and more precise fission product detectors have to be used. At the Joint Institute for Nuclear Research (JINR) Frank Laboratory of Neutron Physics (FLNP), where already half a century the thermal and resonance neutron induced nuclear reactions are studied, a new electron accelerator driven white spectrum pulsed neutron source IREN has been built and successfully tested. The improved characteristics of this facility, in comparison with those of the former pulse neutron fast reactor IBR-30, will allow measuring some of the neutron-nuclear reaction data with better precision and accuracy. A new experimental setup for detecting gamma rays (and neutrons) has been designed and is under construction. It will consist of 2 rings (arrays) of 12 NaI(Tl) detectors each (or 1 array of 24 detectors) with variable ring diameter and distance between both rings. Such a setup will make possible not only to measure the multiplicity, energy and angular anisotropy of prompt fission gammas, but also to separate the contribution of prompt fission neutrons by their longer time-of-flight from the fissile target to the detectors. The signals from all the 24 detectors will be recorded simultaneously in digitized form and will be stored on the hard disk of the personal computer for further off

  1. 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

  2. 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.

  3. Gamma-ray Output Spectra from 239 Pu Fission

    DOE PAGESBeta

    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

  4. Gamma-ray Output Spectra from 239Pu Fission

    NASA Astrophysics Data System (ADS)

    Ullmann, John

    2015-05-01

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

  5. Nonmagnetic ground state of PuO2

    NASA Astrophysics Data System (ADS)

    Shick, A. B.; Kolorenč, J.; Havela, L.; Gouder, T.; Caciuffo, R.

    2014-01-01

    The correlated band theory implemented as a combination of the local density approximation with the exact diagonalization of the Anderson impurity model is applied to PuO2. We obtain an insulating electronic structure consistent with the experimental photoemission spectra. The calculations yield a band gap of 1.8 eV and a nonmagnetic singlet ground state that is characterized by a noninteger filling of the plutonium f shell (nf≈4.5). Due to sizable hybridization of the f shell with the p states of oxygen, the ground state is more complex than the four-electron Russell-Saunders 5I4 manifold split by the crystal field. The inclusion of hybridization improves the agreement between the theory and experiment for the magnetic susceptibility.

  6. 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. PMID:6643070

  7. 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.

  8. 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

  9. 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

  10. 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.

  11. /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.

  12. Research of water-base nano-PU paint for heat insulation

    NASA Astrophysics Data System (ADS)

    Jwo, Ching-Song; Jeng, Lung-Yue; Cheng, Ho; Chen, Sih-Li

    2008-12-01

    The purpose of this study is to research and produce water-base nano-PU paint with energy conservation, environmental consciousness and high efficiency of heat insulation, which can be enhance the traditional PU paint for performance improvement of heat insulation and range of application. In this study, research will be held on the two-stage synthesis method. The SiO2 nanoparticles are added into the water-base PU paint to improve the properties of traditional PU paint. Next, the fundamental properties of this paint, including water resistance, weather rsistance, weak acid solvent resistance, and heat insulation rate, will be measured and analyzed, and the performance of heat insulation will be evaluated in order to confirm the performance and practicability of the heat insulation of water-base nano-PU paint in this study. The experimental results show that for the SiO2/W-PU composite nanopaint prepared by two-stage synthesis method, the dispersion of SiO2 powder in the water-base PU (W-PU) paint is even. For the SiO2/W-PU nanocomposite paint prepared by adding SiO2 powder at 8% wt. to the marketed water-base PU, the water absorption of its experimental sample is enhanced by around 10.1 times, whereas its weak acid dissolve erosion rate is increased by 3.3 times. However, the average heat insulation rate in the thermal properties is also increased, increasing around 24.22% for the W-PU paint without SiO2 powder. Through the multilayered coating construction, the water-base nano-PU paint added with SiO2 powder can be used on any facility of heat insulation, including vehicle, safety helmet, umbrella, drapes, and outer wall of building. The newly developed water-base nano-PU paint with high thermal resistance is especially suitable for application to the shell coating of air conditioner and cooling tower,. Due to the better thermal resistance of this nanopaint, the problems of poor heat transfer and temperature rise of cooling water caused by direct sunlight can be

  13. Adipocyte expression of PU.1 transcription factor causes insulin resistance through upregulation of inflammatory cytokine gene expression and ROS production

    Technology Transfer Automated Retrieval System (TEKTRAN)

    We have reported previously that ETS family transcription factor PU.1 is expressed in mature adipocytes of white adipose tissue. PU.1 expression is increased greatly in mouse models of genetic or diet-induced obesity. Here, we show that PU.1 expression is increased only in visceral but not subcutane...

  14. Studies of vibrational properties in Ga stabilized delta-Pu by extended X-ray absorption fine structure

    SciTech Connect

    Allen, P.G.; Henderson, A.L.; Sylwester, E.R.; Turchi, P.E.A.; Shen, T.H.; Gallegos, G.F.; Booth, C.H.

    2002-02-14

    Temperature dependent extended x-ray absorption fine structure (EXAFS) spectra were measured for a 3.3 at. % Ga stabilized Pu alloy over the range T= 20 - 300 K. EXAFS data were acquired at both the Ga K-edge and the Pu L{sub III} edge. Curve-fits were performed to the first shell interactions to obtain pair-distance distribution widths, {sigma}, as a function of temperature. The temperature dependence of {sigma}(T) was accurately modeled using a correlated-Debye model for the lattice vibrational properties, suggesting Debye-like behavior in this material. Using this formalism, we obtain pair-specific correlated-Debye temperatures, {Theta}{sub cD}, of 110.7 {+-} 1.7 K and 202.6 {+-} 3.7 K, for the Pu-Pu and Ga-Pu pairs, respectively. The result for the Pu-{Theta}{sub cD} value compares well with previous vibrational studies on {delta}-Pu. In addition, our results represent the first unambiguous determination of Ga-specific vibrational properties in Pu-Ga alloys, i.e, {Theta}{sub cD} for the Ga-Pu pair. Because the Debye temperature can be related to a measure of the lattice stiffness, these results indicate the Ga-Pu bonds are significantly stronger than the Pu-Pu bonds. This effect has important implications for lattice stabilization mechanisms in these alloys.

  15. 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

  16. 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

  17. 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.

  18. Minimal PU.1 reduction induces a preleukemic state and promotes development of acute myeloid leukemia.

    PubMed

    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; Neriah, Daniela Ben; Roth, Michael; van Oers, Johanna; Schaetzlein, Sonja; McMahon, Christine; Edelmann, Winfried; Verma, Amit; Steidl, Ulrich

    2015-10-01

    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 reductions in 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 a 35% reduction of PU.1 expression, was sufficient to induce myeloid-biased preleukemic stem cells and their 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. Notably, we found marked molecular similarities between the disease in these mice and human myelodysplastic syndrome and AML. This study demonstrates that minimal reduction of a key lineage-specific transcription factor, which commonly occurs in human disease, is sufficient to initiate cancer development, and it provides mechanistic insight into the formation and progression of preleukemic stem cells in AML. PMID:26343801

  19. 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.

  20. 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.

  1. Safeguards Considerations for Thorium Fuel Cycles

    DOE PAGESBeta

    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 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

  2. 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.

  3. 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.

  4. 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.

  5. Sediment core record of global fallout and Bikini close-in fallout Pu in Sagami Bay, Western Northwest Pacific margin.

    PubMed

    Zheng, Jian; Yamada, Masatoshi

    2004-07-01

    The total 239-240Pu activity and 240Pu/239Pu atom ratio in the sediments in Sagami Bay of the western Northwest Pacific margin were investigated using ICP-MS with a shield torch system. 239+240Pu inventories in the examined sediment cores were found to be much higher than those predicted from atmospheric global fallout (42 MBq/km2) at the same latitude. In addition, elevated 240Pu/239Pu atom ratios ranging from 0.22 to 0.28 were observed in the sediment samples. On the basis of the vertical profiles of 239+240Pu and characterized 240Pu/239Pu atom ratios in a sediment core collected in the center of Sagami Bay, we identified two distinct sources of fallout Pu in the bay: the global stratospheric fallout with characteristic 240Pu/239Pu ratio of 0.18 and the transported close-in fallout derived from Bikini and Enewetak surface nuclear weapon test series in the 1950s. We propose that the Pu transportation was mainly due to oceanic processes (for example, through the North Equatorial Current and the Kuroshio Current). Using a two fallout end-member model, we find that the contribution of Bikini close-in fallout Pu ranged from 44 to 59% in Sagami Bay sediments. To the best of our knowledge, this is the first report that Pu contamination, which originated from Bikini and Enewetak nuclear weapon test series in the 1950s, has extended westwards as far as the Japanese coast. PMID:15296298

  6. 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.

  7. 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.

  8. Determination of Pu in urine at ultratrace level by sector field inductively coupled plasma mass spectrometry

    NASA Astrophysics Data System (ADS)

    Zoriy, M. V.; Pickhardt, C.; Ostapczuk, P.; Hille, R.; Becker, J. S.

    2004-04-01

    A new analytical procedure has been developed for the determination of Pu in urine at the low ag ml-1 concentration level by double-focusing sector field inductively coupled plasma mass spectrometry (ICP-SFMS). One liter of urine doped with 4 pg 242Pu was analyzed after co-precipitation with Ca3(PO4)2 followed by extraction chromatography on TEVA resin in order to enrich the Pu and remove uranium and matrix elements. Figures of merit of ICP-SFMS for the determination of Pu were studied using two nebulizers, PFA-100 and direct injection high-efficiency nebulizer (DIHEN), for solution introduction with uptake rates of 0.58 and 0.06 ml min-1, respectively. The sensitivity for Pu in ICP-SFMS was determined to be 2000 and 1380 MHz ppm-1 for the PFA-100 and DIHEN nebulizers, respectively. Due to the low solution uptake rate of DIHEN the absolute sensitivity was about seven times better and yielded 1380 counts fg-1 in comparison to 207 counts fg-1 measured with the PFA-100 nebulizer. Recovery using 242Pu tracer was about 70%. The limits of detection for 239Pu in 1 l of urine, based on an enrichment factor of 100 for PFA-100 nebulizer and 1000 for DIHEN, were 9×10-18 and 1.02×10-18 g ml-1, respectively. Measurements of 240Pu/239Pu isotopic ratio in synthetically prepared urine standard solution yielded a precision of 1.8 and 1.9% and accuracy of 1.5 and 1.8% for the PFA-100 and DIHEN nebulizers, respectively.

  9. Plutonium Residue Recovery (PuRR) project quarterly progress report, April--June 1989

    SciTech Connect

    Gregg, D.W.; Hickman, R.G.; Landrum, J.H. ); Johnson, G.K.; Johnson, I.; Mulcahey, T.P.; Pierce, R.D.; Poa, D.S. )

    1989-10-20

    A material-balance flowsheet for ash-heel processing has been prepared. The major process features are (1) reduction of Pu into a calcium-zinc alloy and selective electrolytic recovery of the Pu from the alloy, (2) removal of americium as a waste, (3) concentration of nontransuranic tramp elements in a zinc waste, (4) removal of oxygen and recovery of calcium by electrolysis of CaO, and (5) zinc recycle by evaporation. Based on this idealized flowsheet, the mass of solid waste is only 62% of that of the original residue. This is accomplished by recycling virtually all the reagents and discarding the oxygen as CO and CO{sub 2}. The pyrochemical recovery of Pu from incinerator ash heel from the Rocky Flats Plant was investigated. During this period, zinc-calcium alloys were used to reduce the PuC{sub 2} in the ash. Reduction of ash heel has been attempted with zinc-calcium alloys containing 2, 6, and 10 wt% calcium after the reduction. These resulted in extractions of 95%, 97%, and 99.5%, respectively, of the Pu from the salt. Following exposure of the reduction alloy to a ZnCl{sub 2}-bearing salt, the Pu was removed effectively from the alloy; however, the Pu recovered in the salt did not complete the material balance. Experiments were made to test a calcium-zinc reference electrode against a Zn-Ca-Mg-Al liquid alloy. The results agreed well with calculated potentials, and such electrodes are promising for application to process monitoring. Calculations were made that verify that most of the americium in the molten salt is present in the divalent state when distributed between liquid Pu and NaCl-KCl. The AmCl{sub 2} activity coefficient is about 10 times that of PuCl{sub 3} in the salt mixture.

  10. 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

  11. 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.

  12. 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.

  13. Systematic Investigation of the Superconducting Behavior in Aged PuCoGa{sub 5}

    SciTech Connect

    Jutier, Frederic; Colineau, Eric; Griveau, Jean-Christophe; Rebizant, Jean; Wastin, Franck

    2007-07-01

    In this work, we have undertaken to follow the evolution of the PuCoGa{sub 5} superconducting behavior as a function of the damages created by self-radiation effects induced from the Pu-decay. It is shown that the critical temperature is particularly sensitive with ageing. Ageing effects on fundamental parameters such as the lattice parameters of the PuCoGa{sub 5} and the electrical resistivity provide some new hints of the unconventional character of the superconductivity in this class of materials. (authors)

  14. 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.

  15. 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.

  16. 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.

  17. 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

  18. 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

  19. 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

  20. 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.

  1. 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.

  2. In vivo canine studies of a Sinkhole valve and vascular graft coated with biocompatible PU-PEO-SO3.

    PubMed

    Han, D K; Lee, K B; Park, K D; Kim, C S; Jeong, S Y; Kim, Y H; Kim, H M; Min, B G

    1993-01-01

    PU-PEO-SO3 was applied as a coating material over a newly designed Sinkhole bileaflet PU heart valve and a porous PU vascular graft. Performance and biocompatibility were evaluated using an in vivo canine shunt system between the right ventricle and pulmonary artery. The survival periods in three implantations were 14, 24, and 39 days, during which no mechanical failure occurred in any Sinkhole valve or vascular graft. Scanning electron microscopy (SEM) studies demonstrated much less platelet adhesion and thrombus formation on PU-PEO-SO3 grafts than on PU vascular grafts. Cracks in the valve leaflet were occasionally observed on PU surfaces, but not on PU-PEO-SO3. After a 39 day implantation, calcium deposition on vascular grafts was decreased as compared with valve leaflets, and calcification on PU-PEO-SO3 was much lower than on PU. These results suggest that Sinkhole valves and vascular grafts are promising, and PU-PEO-SO3 as a coating material is more blood compatible, biostable, and calcification resistant in vivo than in untreated PU. PMID:8268593

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

    NASA Astrophysics Data System (ADS)

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

    2005-05-01

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

  4. Experimental investigations of /sup 238/Pu behavior in soil columns

    SciTech Connect

    Nelson, G.B.; Herrera, B.; Stalnaker, N.D.; Coffelt, K.P.; Patterson, J.H.; Heaton, R.C.; Matlack, G.M.

    1984-05-01

    Two series of experiments were conducted to study the transport of plutonium through soils. The first series involved deposition of small quantities (2.0 to 3.5 mg) of particulate /sup 238/Pu oxide on soil columns containing silt loam soil. When deionized water was allowed to percolate through the columns, plutonium was released into the drainage at the rate of 8 to 15 pg/day. During the 6.8-y experiment, the total amount of plutonium released into the soil drainage amounted to less than 0.01% of the original source. Analysis of the soil as a function of depth at the end of the experiment revealed that more than 99% of the deposited source remained in the uppermost fraction (2.8 cm) of the column. The second series of experiments was performed by pumping water containing plutonium through columns of soil and comparing the amount of plutonium in the column effluents to that in the feed. For a loamy sand soil, the plutonium content of the effluent reached a steady state of 5% of the feed after 500 days. Analysis of the soil at the end of the experiment (1200 days) showed the columns to be approximately 50% saturated. Saturation of the soil with plutonium would require 13 ..mu..g/g and 6.6 y at the feed rate used (averaged of 1.2 ..mu..g/g into 300 g of soil).

  5. Spi-1/PU.1 transgenic mice develop multistep erythroleukemias.

    PubMed Central

    Moreau-Gachelin, F; Wendling, F; Molina, T; Denis, N; Titeux, M; Grimber, G; Briand, P; Vainchenker, W; Tavitian, A

    1996-01-01

    Insertional mutagenesis of the spi-1 gene is associated with the emergence of malignant proerythroblasts during Friend virus-induced acute erythroleukemia. To determine the role of spi-1/PU.1 in the genesis of leukemia, we generated spi-1 transgenic mice. In one founder line the transgene was overexpressed as an unexpected-size transcript in various mouse tissues. Homozygous transgenic animals gave rise to live-born offspring, but 50% of the animals developed a multistep erythroleukemia within 1.5 to 6 months of birth whereas the remainder survived without evidence of disease. At the onset of the disease, mice became severely anemic. Their hematopoietic tissues were massively invaded with nontumorigenic proerythroblasts that express a high level of Spi-1 protein. These transgenic proerythroblasts are partially blocked in differentiation and strictly dependent on erythropoietin for their proliferation both in vivo and in vitro. A complete but transient regression of the disease was observed after erythrocyte transfusion, suggesting that the constitutive expression of spi-1 is related to the block of the differentiation of erythroid precursors. At relapse, erythropoietin-independent malignant proerythroblasts arose. Growth factor autonomy could be partially explained by the autocrine secretion of erythropoietin; however, other genetic events appear to be necessary to confer the full malignant phenotype. These results reveal that overexpression of spi-1 is essential for malignant erythropoiesis and does not alter other hematopoietic lineages. PMID:8628313

  6. Osteosarcomas among beagles exposed to /sup 239/Pu

    SciTech Connect

    Whittemore, A.S.; McMillan, A.

    1982-04-01

    A Weibull distribution was fit to the osteosarcoma death times of beagles given single intravenous injections of /sup 239/Pu. For injected doses in the range 0-1..mu..Ci/kg the osteosarcoma incidence rate h(t) at t days after injection can be fit by a quadratic function of injected dose d: h(t) = 2.61 X 10/sup -18/ d/sup 2/t/sup 4.91/. The best-fitting linear function was rejected by the data (P < 0.001). A different formula for h(t), derived from a multistage theory for osteosarcoma induction, was also fit to these data. For this purpose microdosimetry calculations were used to estimate the dose to the cells at risk in the endosteal layer (endosteal dose). According to the best fit, h(t) is a quadratic function of endosteal dose at low doses. A linear dose-response relationship was again rejected. The absence of a linear component at low doses might be explained by the fact that 108 of the 185 animals injected at the lowest doses (<0.02 ..mu..Ci/kg) were still alive at the time these data were collected.

  7. Cluster approach to the structure of 240Pu

    NASA Astrophysics Data System (ADS)

    Shneidman, T. M.; Adamian, G. G.; Antonenko, N. V.; Jolos, R. V.; Zhou, Shan-Gui

    2015-09-01

    The cluster approach, which allows us to take into account both shape deformation parameters and cluster degrees of freedom, is developed to describe alternating-parity rotational bands. The important ingredient of the model is the dinuclear system concept in which the wave function of the nucleus is treated as a superposition of a mononucleus and two-cluster configurations. The model is applied to describe the multiple positive and negative parity rotational bands in 240Pu . The observed excitation spectrum and the angular momentum dependences of the parity splitting and of the electric E 1 and E 2 transition moments are explained. Special emphasis is made on the investigation of the recently measured positive parity 02+ rotational band of reflection-asymmetric nature. The results suggest that this band might be understood as being built on the lowest excited state in the mass asymmetry degree of freedom. The B (E 1 )/B (E 2 ) branching ratios between the reduced transition probabilities of decay from the states of the 02+ band to the first negative parity band and to the groundstate band, respectively, are calculated and compared with experimental data.

  8. 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.

  9. 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.

  10. Determination of {sup 230}Th, {sup 234}U, {sup 239}Pu, and {sup 240}Pu in soils by ICP-MS using flow-injection preconcentration

    SciTech Connect

    Hollenbach, M.; Grohs, J.; Mamich, S.; Kroft, M.

    1995-12-31

    The US Department of Energy needs improved analytical methods for alpha-emitting radionuclides to support environmental restoration and waste management projects. Inductively coupled plasma-mass spectrometry (ICP-MS) has been used successfully to measure radionuclides with relatively long half-lives; however, ICP-MS used with conventional sample introduction techniques lacks the sensitivity or selectivity to measure shorter-lived radionuclides at levels important for environmental monitoring. New methods were developed for measuring {sup 230}Th, {sup 234}U, {sup 239}Pu, and {sup 240}Pu in soils. Samples are dried, ground, and dissolved by fusion. A flow injection (FI) analysis system is used to separate and concentrate the analytes by solid-phase extraction. The FI eluent is pumped directly into the nebulizer of the ICP-MS. The use of FI resulted in greater sensitivity and freedom from interferences when compared with direct aspiration. Detection limits are improved by approximately a factor of 20. The detection limits are approximately 3 Bq/kg (4 ng/kg) for {sup 230}Th, 0.6 Bq/kg (3 ng/kg) for {sup 234}U, 0.4 Bq/kg (0.2 ng/kg) for {sup 239}Pu, and 2 Bq/kg (0.3 ng/kg) for {sup 240}Pu. The FI-ICP-MS methods are faster, less labor intensive, and generate less laboratory waste than traditional radiochemical methods. The FI-ICP-MS gives individual results for {sup 239}Pu and {sup 240}Pu which cannot be resolved by the usual radiochemical method. The accuracy of the methods was verified by analyzing reference soils.

  11. Synthesis and structures of plutonyl nitrate complexes: is plutonium heptavalent in PuO3(NO3)2(-) ?

    PubMed

    Maurice, Rémi; Renault, Eric; Gong, Yu; Rutkowski, Philip X; Gibson, John K

    2015-03-01

    Gas-phase plutonium nitrate anion complexes were produced by electrospray ionization (ESI) of a plutonium nitrate solution. The ESI mass spectrum included species with all four of the common oxidation states of plutonium: Pu(III), Pu(IV), Pu(V), and Pu(VI). Plutonium nitrate complexes were isolated in a quadrupole ion trap and subjected to collision-induced dissociation (CID). CID of complexes of the general formula PuOx(NO3)y(-) resulted in the elimination of NO2 to produce PuOx+1(NO3)y-1(-), which in most cases corresponds to an increase in the oxidation state of plutonium. Plutonyl species, Pu(V)O2(NO3)2(-) and Pu(VI)O2(NO3)3(-), were produced from Pu(III)(NO3)4(-) and Pu(IV)(NO3)5(-), respectively, by the elimination of two NO2 molecules. CID of Pu(VI)O2(NO3)3(-) resulted in NO2 elimination to yield PuO3(NO3)2(-), in which the oxidation state of plutonium could be VII, a known oxidation state in condensed phase but not yet in the gas phase. Density functional theory confirmed the nature of Pu(V)O2(NO3)2(-) and Pu(VI)O2(NO3)3(-) as plutonyl(V/VI) cores coordinated by bidentate equatorial nitrate ligands. The computed structure of PuO3(NO3)2(-) is essentially a plutonyl(VI) core, Pu(VI)O2(2+), coordinated in the equatorial plane by two nitrate ligands and one radical oxygen atom. The computations indicate that in the ground spin-orbit free state of PuO3(NO3)2(-), the unpaired electron of the oxygen atom is antiferromagnetically coupled to the spin-triplet state of the plutonyl core. The results indicate that Pu(VII) is not a readily accessible oxidation state in the gas phase, despite that it is stable in solution and solids, but rather that a Pu(VI)-O· bonding configuration is favored, in which an oxygen radical is involved. PMID:25695878

  12. Bacterial Pu(V) reduction in the absence and presence of Fe(III)-NTA: modeling and experimental approach

    SciTech Connect

    Deo, Randhir P; Rittmann, Bruce E; Reed, Donald T

    2013-01-10

    Plutonium (Pu), a key contaminant at sites associated with the manufacture of nuclear weapons and with nuclear-energy wastes, can be precipitated to 'immobilized' plutonium phases in systems that promote bioreduction. Ferric iron (Fe3+) is often present in contaminated sites, and its bioreduction to ferrous iron (Fe2+) may be involved in the reduction of Pu to forms that precipitate. Alternately, Pu can be reduced directly by the bacteria. Besides Fe, contaminated sites often contain strong complexing ligands, such as nitrilotriacetic acid (NTA). We used biogeochemical modeling to interpret the experimental fate of Pu in the absence and presence of ferric iron (Fe3+) and NTA under anaerobic conditions. In all cases, Shewanella alga BrY (S. alga) reduced Pu(V)(PuO2+) to Pu(III), and experimental evidence indicates that Pu(III) precipitated as PuPO4(am). In the absence of Fe3+ and NTA, reduction of PuO2+ was directly biotic, but modeling simulations support that PuO2+ reduction in the presence of Fe3+ and NTA was due to an abiotic stepwise reduction of PuO2+ to Pu4+, followed by reduction of Pu4+ to Pu3+, both through biogenically produced Fe2+. This means that PuO2+ reduction was slowed by first having Fe3+ reduced to Fe2+. Modeling results also show that the degree of PuPO4(am) precipitation depends on the NTA concentration. While precipitation out-competes complexation when NTA is present at the same or lower concentration than Pu, excess NTA can prevent precipitation of PuPO4(am).

  13. Thermophysical properties of α-Pu2O3: A new potential model

    NASA Astrophysics Data System (ADS)

    Günay, S. D.; Akgenç, B.; Akdere, Ü.; Taşseven, ć.

    2013-12-01

    α-Pu2O3 is an important material among plutonium based materials in nuclear industry. Pure plutonium surfaces quickly oxidizes into α-Pu2O3 and PuO2 which are in the form of layers one on another [1]. Here we have investigated thermal properties of α-Pu2O3 by molecular dynamics simulation by using a partially ionic semi-empirical rigid ion potential. Mechanical properties, thermal expansion, and heat capacity are calculated. Results were compared with available experimental data and quantum calculation [2]. Due to the experimental limitations such as toxicity and radiation effects, studying the physical properties of such materials from molecular dynamics simulations have vital importance.

  14. Direct high-precision mass measurements on Am241,243, Pu244, and Cf249

    NASA Astrophysics Data System (ADS)

    Eibach, M.; Beyer, T.; Blaum, K.; Block, M.; Düllmann, Ch. E.; Eberhardt, K.; Grund, J.; Nagy, Sz.; Nitsche, H.; Nörtershäuser, W.; Renisch, D.; Rykaczewski, K. P.; Schneider, F.; Smorra, C.; Vieten, J.; Wang, M.; Wendt, K.

    2014-06-01

    The absolute masses of four long-lived transuranium nuclides, Am241,243, Pu244, Pu244, and Cf249, in the vicinity of the deformed N =152 neutron shell closure have been measured directly with the Penning-trap mass spectrometer TRIGA-TRAP. Our measurements confirm the AME2012 mass values of Am241,243 and Pu244 within one standard deviation, which were indirectly determined, by decay spectroscopy studies. In the case of the Cf249 mass, a discrepancy of more than three standard deviations has been observed, affecting absolute masses even in the superheavy element region. The implementation of the mass values into the AME2012 network yields a reduced mass uncertainty for 84 nuclides, particularly for Pu244 and its strongly correlated α decay chains.

  15. Improved electrospinning processing of PU/PEDOT:PSS for electronic textile applications

    NASA Astrophysics Data System (ADS)

    Evke, Erin; Clippinger, Aaron; Spackman, Clayson; Samuel, Johnson; Ozisik, Rahmi

    Poly(3,4-ethylenedioxythiophene)/poly(4-styrenesulfonate), PEDOT:PSS, is an electrically conductive polymer used in electronic textile (e-textile) applications, such as eletrochromic textiles, strain sensors, and resistive heaters. In the current study, PEDOT:PSS is blended with varying concentrations of polyurethane (PU) to investigate the flexibility of PU/PEDOT:PSS fibers that are produced via a modified electrospinning process where the jet is collected close to the tip of the needle, thereby, enabling the collection of straight fibers by a rotating spool. The electrical conductivity and mechanical properties of PU/PEDOT:PSS fibers are characterized to understand the effect of PU concentration and the processing parameters. This material is based upon work supported by the National Science Foundation under Grant No. CMMI-1538730.

  16. Observation of Dynamical spin shielding in Ce: Why It Matters for Pu Electronic Structure

    SciTech Connect

    Tobin, J G; Yu, S W; Chung, B W; Morton, S A; Komesua, T; Waddill, G D

    2007-03-08

    In a series of experiments and linked theoretical modeling, the range of possible solutions for Pu electronic structure has been dramatically reduced. Nevertheless, the key issue of electron correlation remains.

  17. The influence of defects on magnetic properties of fcc-Pu

    SciTech Connect

    Shorikov, A. O.; Anisimov, V. I.; Korotin, M. A.; Dremov, V. V. Sapozhnikov, Ph. A.

    2013-10-15

    The influence of vacancies and interstitial atoms on magnetism in Pu is considered in the framework of the density functional theory. The crystal structure relaxation arising due to various types of defects is calculated using the molecular dynamics method with a modified embedded atom model. The local density approximation with explicit inclusion of Coulomb and spin-orbit interactions is applied in matrix invariant form to describe correlation effects in Pu with these types of defects. The calculations show that both vacancies and interstitials give rise to local moments in the f-shell of Pu in good agreement with experimental data for aged Pu. Magnetism appears due to the destruction of a delicate balance between spin-orbit and exchange interactions.

  18. Surprising Coordination Geometry Differences in Ce(IV)- and Pu(IV)-Maltol Complexes

    SciTech Connect

    Lawrence Berkeley National Laboratory; Raymond, Kenneth; Szigethy, Geza; Xu, Jide; Gorden, Anne E.V.; Teat, Simon J.; Shuh, David K.; Raymond, Kenneth N.

    2008-02-12

    As part of a study to characterize the detailed coordination behavior of Pu(IV), single crystal X-ray diffraction structures have been determined for Pu(IV) and Ce(IV) complexes with the naturally-occurring ligand maltol (3-hydroxy-2-methyl-pyran-4-one) and its derivative bromomaltol (5-bromo-3-hydroxy-2-methyl-pyran-4-one). Although Ce(IV) is generally accepted as a structural analog for Pu(IV), and the maltol complexes of these two metals are isostructural, the corresponding bromomaltol complexes are strikingly different with respect to ligand orientation about the metal ion: All complexes exhibit trigonal dodecahedral coordination geometry but the Ce(IV)-bromomaltol complex displays an uncommon ligand arrangement not mirrored in the Pu(IV) complex, although the two metal species are generally accepted to be structural analogs.

  19. Silver-catalyzed PuO sub 2 dissolution with persulfate

    SciTech Connect

    Fisher, F D; Barney, G S; Cooper, T D; Duchsherer, M J

    1991-06-01

    This report consists of 14 slides and associated narrative for a presentation to be given at the 15th Annual Actinide Separations Conference on silver-catalyzed PuO{sub 2} dissolution with persulfate. (JL)

  20. Role of PU.1 in MHC Class II Expression via CIITA Transcription in Plasmacytoid Dendritic Cells

    PubMed Central

    Miura, Ryosuke; Kasakura, Kazumi; Nakano, Nobuhiro; Hara, Mutsuko; Maeda, Keiko; Okumura, Ko; Ogawa, Hideoki; Yashiro, Takuya; Nishiyama, Chiharu

    2016-01-01

    The cofactor CIITA is a master regulator of MHC class II expression and several transcription factors regulating the cell type-specific expression of CIITA have been identified. Although the MHC class II expression in plasmacytoid dendritic cells (pDCs) is also mediated by CIITA, the transcription factors involved in the CIITA expression in pDCs are largely unknown. In the present study, we analyzed the role of a hematopoietic lineage-specific transcription factor, PU.1, in CIITA transcription in pDCs. The introduction of PU.1 siRNA into mouse pDCs and a human pDC cell line, CAL-1, reduced the mRNA levels of MHC class II and CIITA. When the binding of PU.1 to the 3rd promoter of CIITA (pIII) in CAL-1 and mouse pDCs was analyzed by a chromatin immunoprecipitation assay, a significant amount of PU.1 binding to the pIII was detected, which was definitely decreased in PU.1 siRNA-transfected cells. Reporter assays showed that PU.1 knockdown reduced the pIII promoter activity and that three Ets-motifs in the human pIII promoter were candidates of cis-enhancing elements. By electrophoretic mobility shift assays, it was confirmed that two Ets-motifs, GGAA (-181/-178) and AGAA (-114/-111), among three candidates, were directly bound with PU.1. When mouse pDCs and CAL-1 cells were stimulated by GM-CSF, mRNA levels of PU.1, pIII-driven CIITA, total CIITA, MHC class II, and the amount of PU.1 binding to pIII were significantly increased. The GM-CSF-mediated up-regulation of these mRNAs was canceled in PU.1 siRNA-introduced cells. Taking these results together, we conclude that PU.1 transactivates the pIII through direct binding to Ets-motifs in the promoter in pDCs. PMID:27105023

  1. Real time studies of Elastic Moduli Pu Aging using Resonant Ultrasound Spectroscopy

    NASA Astrophysics Data System (ADS)

    Maiorov, Boris

    Elastic moduli are fundamental thermodynamic susceptibilities that connect directly to thermodynamics, electronic structure and give important information about mechanical properties. To determine the time evolution of the elastic properties in 239Pu and it Ga alloys, is imperative to study its phase stability and self-irradiation damage process. The most-likely sources of these changes include a) ingrowth of radioactive decay products like He and U, b) the introduction of radiation damage, c) δ-phase instabilities towards α-Pu or to Pu3Ga. The measurement of mechanical resonance frequencies can be made with extreme precision and used to compute the elastic moduli without corrections giving important insight in this problem. Using Resonant Ultrasound Spectroscopy, we measured the time dependence of the mechanical resonance frequencies of fine-grained polycrystalline δ-phase 239Pu, from 300K up to 480K. At room temperature, the shear modulus shows an increase in time (stiffening), but the bulk modulus decreases (softening). These are the first real-time measurements of room temperature aging of the elastic moduli, and the changes are consistent with elastic moduli measurements performed on 44 year old δ-Pu. As the temperature is increased, the rate of change increases exponentially, with both moduli becoming stiffer with time. For T>420K an abrupt change in the time dependence is observed indicating that the bulk and shear moduli have opposite rates of change. Our measurements provide a basis for ruling out the decomposition of δ-Pu towards α-Pu or Pu3Ga, and indicate a complex defect-related scenario from which we are gathering important clues.

  2. Mass transport properties of Pu/DT mixtures from orbital free molecular dynamics simulations

    SciTech Connect

    Kress, Joel David; Ticknor, Christopher; Collins, Lee A.

    2015-09-16

    Mass transport properties (shear viscosity and diffusion coefficients) for Pu/DT mixtures were calculated with Orbital Free Molecular Dynamics (OFMD). The results were fitted to simple functions of mass density (for ρ=10.4 to 62.4 g/cm3) and temperature (for T=100 up to 3,000 eV) for Pu/DT mixtures consisting of 100/0, 25/75, 50/50, and 75/25 by number.

  3. Transcriptional Factor PU.1 Regulates Decidual C1q Expression in Early Pregnancy in Human.

    PubMed

    Madhukaran, Shanmuga Priyaa; Kishore, Uday; Jamil, Kaiser; Teo, Boon Heng Dennis; Choolani, Mahesh; Lu, Jinhua

    2015-01-01

    C1q is the first recognition subcomponent of the complement classical pathway, which in addition to being synthesized in the liver, is also expressed by macrophages and dendritic cells (DCs). Trophoblast invasion during early placentation results in accumulation of debris that triggers the complement system. Hence, both early and late components of the classical pathway are widely distributed in the placenta and decidua. In addition, C1q has recently been shown to significantly contribute to feto-maternal tolerance, trophoblast migration, and spiral artery remodeling, although the exact mechanism remains unknown. Pregnancy in mice, genetically deficient in C1q, mirrors symptoms similar to that of human preeclampsia. Thus, regulated complement activation has been proposed as an essential requirement for normal successful pregnancy. Little is known about the molecular pathways that regulate C1q expression in pregnancy. PU.1, an Ets-family transcription factor, is required for the development of hematopoietic myeloid lineage immune cells, and its expression is tissue-specific. Recently, PU.1 has been shown to regulate C1q gene expression in DCs and macrophages. Here, we have examined if PU.1 transcription factor regulates decidual C1q expression. We used immune-histochemical analysis, PCR, and immunostaining to localize and study the gene expression of PU.1 transcription factor in early human decidua. PU.1 was highly expressed at gene and protein level in early human decidual cells including trophoblast and stromal cells. Surprisingly, nuclear as well as cytoplasmic PU.1 expression was observed. Decidual cells with predominantly nuclear PU.1 expression had higher C1q expression. It is likely that nuclear and cytoplasmic PU.1 localization has a role to play in early pregnancy via regulating C1q expression in the decidua during implantation. PMID:25762996

  4. Absolute measurement of the 242Pu neutron-capture cross section

    NASA Astrophysics Data System (ADS)

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

    2016-04-01

    The absolute neutron-capture cross section of 242Pu was measured at the Los Alamos Neutron Science Center using the Detector for Advanced Neutron-Capture Experiments array along with a compact parallel-plate avalanche counter for fission-fragment detection. The first direct measurement of the 242Pu(n ,γ ) cross section was made over the incident neutron energy range from thermal to ≈6 keV, and the absolute scale of the (n ,γ ) cross section was set according to the known 239Pu(n ,f ) resonance at En ,R=7.83 eV. This was accomplished by adding a small quantity of 239Pu to the 242Pu sample. The relative scale of the cross section, with a range of four orders of magnitude, was determined for incident neutron energies from thermal to ≈40 keV. Our data, in general, are in agreement with previous measurements and those reported in ENDF/B-VII.1; the 242Pu(n ,γ ) cross section at the En ,R=2.68 eV resonance is within 2.4 % of the evaluated value. However, discrepancies exist at higher energies; our data are ≈30 % lower than the evaluated data at En≈1 keV and are approximately 2 σ away from the previous measurement at En≈20 keV.

  5. Application of a canine 238Pu biokinetics/dosimetry model to human bioassay data.

    PubMed

    Hickman, A W; Griffith, W C; Roessler, G S; Guilmette, R A

    1995-03-01

    Associated with the use of 238Pu in thermoelectric power sources for space probes is the potential for human exposure, primarily by inhalation and most likely as 238PuO2. Several models have been developed for assessing the level of intake and predicting the resulting radiation dose following human exposure to 239Pu. However, there are indications that existing models do not adequately describe the disposition and dosimetry of 238Pu following human exposure. In this study, a canine model that accounts for these differences has been adapted for use with human excretion data. The model is based on existing knowledge about organ retention of plutonium. An analysis of the sensitivity of the model to changes in aerosol-associated properties indicated that predictions of urinary excretion are most sensitive to changes in particle solubility and diameter and in the ratio of fragment:particle surface area. Application of the model to urinary excretion data from seven workers exposed to a 238Pu ceramic aerosol gave estimated intakes of 390-8,200 Bq and associated initial pulmonary burdens of 80-1,700 Bq. The resulting 50-y dose commitments to critical organs per Bq of 238Pu intake were estimated to be 0.5 mSv for the thoracic region, 0.2 mSv for the liver, and 1 mSv for the bone surfaces. PMID:7860307

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

    PubMed

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

    2016-03-01

    An electron spectrometry set-up was built at IRMM consisting of a vacuum chamber with a moveable source holder and windowless Peltier-cooled silicon drift detector (SDD). The SDD is well suited for measuring low-energy x rays and electrons emitted from thin radioactive sources with low self-absorption. The attainable energy resolution is better than 0.5keV for electrons of 30keV. It has been used to measure the conversion electron spectra of three plutonium isotopes, i.e. (238)Pu, (239)Pu, (240)Pu, as well as (241)Am (being a decay product of (241)Pu). The obtained mixed x-ray and electron spectra are compared with spectra obtained with a close-geometry set-up using another SDD in STUK and spectra measured with a Si(Li) detector at IRMM. The potential of conversion electron spectrometry for isotopic analysis of mixed plutonium samples is investigated. With respect to the (240)Pu/(239)Pu isotopic ratio, the conversion electron peaks of both isotopes are more clearly separated than their largely overlapping peaks in alpha spectra. PMID:26651177

  7. Measurement of Neutron Induced and Spontaneous Fission in Pu-242 at DANCE

    NASA Astrophysics Data System (ADS)

    Chyzh, Andrii; Wu, C. Y.; Henderson, R.; Couture, A.; Lee, H. Y.; Ullmann, J.; O'Donnell, J. M.; Jandel, M.; Haight, R. C.; Bredeweg, T. A.; Dance Collaboration

    2013-10-01

    Neutron capture and fission reactions are important in nuclear engineering and physics. DANCE (Detector for Advanced Neutron Capture Measurement, LANL) combined with PPAC (avalanche technique based fission tagging detector, LLNL) were used to study neutron induced and spontaneous fission in 242Pu. 2 measurements were performed in 2013. The first experiment was done without the incident neutron beam with the fission tagging ability to study γ-rays emitted in the spontaneous fission of 242Pu. The second one - with the neutron beam to measure both the neutron capture and fission reactions. This is the first direct measurement of prompt fission γ-rays in 242Pu. The γ-ray multiplicity, γ-ray energy, and total energy of γ-rays per fission in 242Pu will be presented. These distributions of the 242Pu spontaneous fission will be compared to those in the 241Pu neutron induced fission. This work was performed under the auspices of the US Department of Energy by Los Alamos National Laboratory under Contract DE-AC52-06NA25396 and Lawrence Livermore National Laboratory under Contract DE-AC52-07NA27344.

  8. Pip, a novel IRF family member, is a lymphoid-specific, PU.1-dependent transcriptional activator.

    PubMed

    Eisenbeis, C F; Singh, H; Storb, U

    1995-06-01

    The immunoglobulin light-chain gene enhancers E kappa 3', E lambda 2-4, and E lambda 3-1 contain a conserved cell type-specific composite element essential for their activities. This element binds a B cell-specific heterodimeric protein complex that consists of the Ets family member PU.1 and a second factor (NF-EM5), whose participation in the formation of the complex is dependent on the presence of DNA-bound PU.1. In this report we describe the cloning and characterization of Pip (PU.1 interaction partner), a lymphoid-specific protein that is most likely NF-EM5. As expected, the Pip protein binds the composite element only in the presence of PU.1; furthermore, the formation of this ternary complex is critically dependent on phosphorylation of PU.1 at serine-148. The Pip gene is expressed specifically in lymphoid tissues in both B- and T-cell lines. When coexpressed in NIH-3T3 cells, Pip and PU.1 function as mutually dependent transcription activators of the composite element. The amino-terminal DNA-binding domain of Pip exhibits a high degree of homology to the DNA-binding domains of members of the interferon regulatory factor (IRF) family, which includes IRF-1, IRF-2, ICSBP, and ISGF3 gamma. PMID:7797077

  9. Absolute measurement of the 242Pu neutron-capture cross section

    DOE PAGESBeta

    Buckner, M. Q.; Wu, C. Y.; Henderson, R. A.; Bucher, B.; Chyzh, A.; Bredeweg, T. A.; Baramsai, B.; Couture, A.; Jandel, M.; Mosby, S.; et al

    2016-04-21

    Here, the absolute neutron-capture cross section of 242Pu was measured at the Los Alamos Neutron Science Center using the Detector for Advanced Neutron-Capture Experiments array along with a compact parallel-plate avalanche counter for fission-fragment detection. The first direct measurement of the 242Pu(n,γ) cross section was made over the incident neutron energy range from thermal to ≈ 6 keV, and the absolute scale of the (n,γ) cross section was set according to the known 239Pu(n,f) resonance at En,R = 7.83 eV. This was accomplished by adding a small quantity of 239Pu to the 242Pu sample. The relative scale of the crossmore » section, with a range of four orders of magnitude, was determined for incident neutron energies from thermal to ≈ 40 keV. Our data, in general, are in agreement with previous measurements and those reported in ENDF/B-VII.1; the 242Pu(n,γ) cross section at the En,R = 2.68 eV resonance is within 2.4% of the evaluated value. However, discrepancies exist at higher energies; our data are ≈30% lower than the evaluated data at En ≈ 1 keV and are approximately 2σ away from the previous measurement at En ≈ 20 keV.« less

  10. COMPUTER SIMULATIONS TO ADDRESS PU-FE EUTECTICISSUE IN 3013 STORAGE VESSEL

    SciTech Connect

    Gupta, N; Allen Smith, A

    2007-03-06

    On November 22, 2005, the Manager of the Plutonium Finishing Plant (PFP) in Richland, WA issued an Occurrence Report involving a potential Pu-Fe eutectic failure mechanism for the stainless steel (SS) 3013 cans containing plutonium (Pu) metal. Four additional reports addressed nuclear safety concerns about the integrity of stainless steel containers holding plutonium during fire scenarios. The reports expressed a belief that the probability and consequences of container failure due to the formation of a plutonium-iron eutectic alloy had been overlooked. Simplified thermal model to address the Pu-Fe eutectic concerns using axisymmetric model similar to the models used in the 9975 SARP were performed. The model uses Rocky Flats configuration with 2 stacked Pu buttons inside a 3013 assembly. The assembly has an outer can, an inner can, and a convenience can, all stainless steel. The boundary conditions are similar to the regulatory 30 minutes HAC fire analyses. Computer simulations of the HAC fire transients lasting 4 hours of burn time show that the interface between the primary containment vessel and the Pu metal in the 9975 package will not reach Pu-Fe eutectic temperature of 400 C.

  11. PU/SS EUTECTIC ASSESSMENT IN 9975 PACKAGINGS IN A STORAGE FACILITY DURING EXTENDED FIRE

    SciTech Connect

    Gupta, N.

    2012-03-26

    In a radioactive material (RAM) packaging, the formation of eutectic at the Pu/SS (plutonium/stainless steel) interface is a serious concern and must be avoided to prevent of leakage of fissile material to the environment. The eutectic temperature for the Pu/SS is rather low (410 C) and could seriously impact the structural integrity of the containment vessel under accident conditions involving fire. The 9975 packaging is used for long term storage of Pu bearing materials in the DOE complex where the Pu comes in contact with the stainless steel containment vessel. Due to the serious consequences of the containment breach at the eutectic site, the Pu/SS interface temperature is kept well below the eutectic formation temperature of 410 C. This paper discusses the thermal models and the results for the extended fire conditions (1500 F for 86 minutes) that exist in a long term storage facility and concludes that the 9975 packaging Pu/SS interface temperature is well below the eutectic temperature.

  12. Determination of 240Pu/239Pu isotopic ratios in human tissues collected from areas around the Semipalatinsk Nuclear Test Site by sector-field high resolution ICP-MS.

    PubMed

    Yamamoto, M; Oikawa, S; Sakaguchi, A; Tomita, J; Hoshi, M; Apsalikov, K N

    2008-09-01

    Information on the 240Pu/239Pu isotope ratios in human tissues for people living around the Semipalatinsk Nuclear Test Site (SNTS) was deduced from 9 sets of soft tissues and bones, and 23 other bone samples obtained by autopsy. Plutonium was radiochemically separated and purified, and plutonium isotopes (239Pu and 240Pu) were determined by sector-field high resolution inductively coupled plasma-mass spectrometry. For most of the tissue samples from the former nine subjects, low 240Pu/239Pu isotope ratios were determined: bone, 0.125 +/- 0.018 (0.113-0.145, n = 4); lungs, 0.063 +/- 0.010 (0.051-0.078, n = 5); and liver, 0.148 +/- 0.026 (0.104-0.189, n = 9). Only 239Pu was detected in the kidney samples; the amount of 240Pu was too small to be measured, probably due to the small size of samples analyzed. The mean 240Pu/239Pu isotope ratio for bone samples from the latter 23 subjects was 0.152 +/- 0.034, ranging from 0.088 to 0.207. A significant difference (a two-tailed Student's t test; 95% significant level, alpha = 0.05) between mean 240Pu/239Pu isotope ratios for the tissue samples and for the global fallout value (0.178 +/- 0.014) indicated that weapons-grade plutonium from the atomic bombs has been incorporated into the human tissues, especially lungs, in the residents living around the SNTS. The present 239,240Pu concentrations in bone, lung, and liver samples were, however, not much different from ranges found for human tissues from other countries that were due solely to global fallout during the 1970's-1980's. PMID:18695410

  13. Recovery of Technetium and Iodine from Spent ATW TRISO Type Fuels.

    SciTech Connect

    Schroeder, N. C.; Attrep, Moses

    2001-01-01

    The Accelerator Transmutation of Waste (ATW) program is being developed to determine the feasibility of separating and transmutating the transactinides (Pu-Cm) and long-lived fission product (99Tc and 129I) from spent LWR fuel. Several types of ATW fuels have been suggested to transmutate the Pu-Cm fraction including TRISO type fuels. An ATW TRISO fuel would consist of a Pu-Cm oxide kernel surrounded by several layers of pyrolytic carbon, a layer of SiC, and an outer layer of pyrolytic carbon. Processing of the spent ATW fuel would involve the crush, burn, and leach approach used on normal TRISO fuels. This report describes experiments that determine the potential behavior of the two long-lived fission products, 99Tc and 129I, in this processing. Iodine can be removed and trapped during the burning of the carbon from the fuel. Some technetium may volatilize in the latter stages of the burn but the bulk of it will have to be recovered after dissolution of the oxide residue.

  14. PU.1 antisense lncRNA against its mRNA translation promotes adipogenesis in porcine preadipocytes.

    PubMed

    Wei, N; Wang, Y; Xu, R-X; Wang, G-Q; Xiong, Y; Yu, T-Y; Yang, G-S; Pang, W-J

    2015-04-01

    Antisense long non-coding RNAs (AS lncRNAs) play important roles in refined regulation of animal gene expression. However, their functions and molecular mechanisms for domestic animal adipogenesis are largely unknown. Here, we found a novel AS lncRNA transcribed from the porcine PU.1 gene (also known as SPI1) by strand-specific RT-PCR. Results showed that PU.1 AS lncRNA was expressed and generally lower than the level of PU.1 mRNA in porcine subcutaneous adipose, heart, liver, spleen, lympha, skeletal muscle and kidney tissues. We further found that the levels of PU.1 mRNA and PU.1 protein were significantly lower in subcutaneous and intermuscular adipose than in mesenteric and greater omentum adipose, whereas the levels of PU.1 AS lncRNA showed no difference in porcine adipose tissues from four different parts of the body. During porcine adipogenesis, levels of PU.1 mRNA increased at day 2 and then gradually decreased. Meanwhile, PU.1 AS lncRNA exhibited an expression trend similar to PU.1 mRNA but sharply decreased after day 2. Interestingly, PU.1 protein level rose during differentiation. In addition, at day 6 after differentiation, knockdown of endogenous PU.1 promoted adipogenesis, whereas knockdown of endogenous PU.1 AS lncRNA had the opposite effect. Moreover, peroxisome proliferator-activated receptor gamma (PPARG) and fatty acid synthase (FASN) were significantly upregulated in the PU.1 shRNA treatment group (P < 0.05), whereas they were downregulated in the PU.1 AS shRNA treatment group (P < 0.05). Adipose triglyceride lipase [ATGL; also known as patatin-like phospholipase domain containing 2 (PNPLA2)] and hormone-sensitive lipase [HSL; also known as lipase, hormone-sensitive (LIPE)] contrasted with PPARG and FASN. Finally, the PU.1 mRNA/PU.1 AS lncRNA duplex was detected by an endogenous ribonuclease protection assay combined with RT-PCR. Based on the above results, we suggest that PU.1 AS lncRNA (vs. its mRNA translation) promotes adipogenesis through

  15. 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

  16. Characterization of Actinides Complexed to Nuclear Fuel Constituents Using ESI-MS.

    PubMed

    McDonald, Luther W; Campbell, James A; Vercouter, Thomas; Clark, Sue B

    2016-03-01

    Electrospray ionization-mass spectrometry (ESI-MS) was tested for its use in monitoring spent nuclear fuel (SNF) constituents including U, Pu, dibutyl phosphate (DBP), and tributyl phosphate (TBP). Both positive and negative ion modes were used to evaluate the speciation of U and Pu with TBP and DBP. Furthermore, apparent stability constants were determined for U complexed to TBP and DBP. In positive ion mode, TBP produced a strong signal with and without complexation to U or Pu, but, in negative ion mode, no TBP, U-TBP, or Pu-TBP complexes were observed. Apparent stability constants were determined for [UO2(NO3)2(TBP)2], [UO2(NO3)2(H2O)(TBP)2], and [UO2(NO3)2(TBP)3]. In contrast DBP, U-DBP, and Pu-DBP complexes were observed in both positive and negative ion modes. Apparent stability constants were determined for the species [UO2(DBP)], [UO2(DBP)3], and [UO2(DBP)4]. Analyzing mixtures of U or Pu with TBP and DBP yielded the formation of ternary complexes whose stoichiometry was directly related to the ratio of TBP to DBP. The ESI-MS protocols used in this study will further demonstrate the utility of ESI-MS and its applicability to process control monitoring in SNF reprocessing facilities. PMID:26823002

  17. 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.

  18. 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.

  19. Chemical resolution of Pu+ from U+ and Am+ using a band-pass reaction cell inductively coupled plasma mass spectrometer.

    PubMed

    Tanner, Scott D; Li, Chunsheng; Vais, Vladimir; Baranov, Vladimir I; Bandura, Dmitry R

    2004-06-01

    Determination of the concentration and distribution of the Pu and Am isotopes is hindered by the isobaric overlaps between the elements themselves and U, generally requiring time-consuming chemical separation of the elements. A method is described in which chemical resolution of the elemental ions is obtained through ion-molecule reactions in a reaction cell of an ICPMS instrument. The reactions of "natural" U(+), (242)Pu(+), and (243)Am(+) with ethylene, carbon dioxide, and nitric oxide are reported. Since the net sensitivities to the isotopes of an element are similar, chemical resolution is inferred when one isobaric element reacts rapidly with a given gas and the isobar (or in this instance surrogate isotope) is unreactive or slowly reactive. Chemical resolution of the m/z 238 isotopes of U and Pu can be obtained using ethylene as a reaction gas, but little improvement in the resolution of the m/z 239 isobars is obtained. However, high efficiency of reaction of U(+) and UH(+) with CO(2), and nonreaction of Pu(+), allows the sub-ppt determination of (239)Pu, (240)Pu, and (242)Pu (single ppt for (238)Pu) in the presence of 7 orders of magnitude excess U matrix without prior chemical separation. Similarly, oxidation of Pu(+) by NO, and nonreaction of Am(+), permit chemical resolution of the isobars of Pu and Am over 2-3 orders of magnitude relative concentration. The method provides the potential for analysis of the actinides with reduced sample matrix separation. PMID:15167781

  20. Effectiveness of DTPA therapy when administered intragastrically or intraperitoneally to remove Pu from adult or neonatal rats

    SciTech Connect

    Sullivan, M.F.; Ruemmler, P.S.

    1986-11-01

    Adult and neonatal rats were given /sup 238/Pu by gavage or parenterally and treated with 0.5 mmoles/kg of calcium diethylenetriaminepentaacetate (DTPA), by gavage or parenterally, to determine its effectiveness for removing Pu. Parenteral administration of DTPA to adult rats 2 h after an intravenous /sup 238/Pu injection was much more effective than intragastric treatment, removing nearly 70% of the retained dose. When /sup 238/Pu was given to adults intragastrically (IG), followed by DTPA given either intraperitoneally (IP) or IG 2 h later, /sup 238/Pu absorption increased while retention remained either unchanged, or increased. When neonates were given /sup 238/Pu IG and treated 2 h later with intraperitoneal or intragastric DTPA, removal of /sup 238/Pu was better than in adults: more than 80% of the /sup 238/Pu that was absorbed and retained was removed by intragastric DTPA. When neonates were injected IP with /sup 238/Pu, treatment with intraperitoneal DTPA was more effective for /sup 238/Pu removal than intragastric treatment.