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Sample records for actinide isotope content

  1. Radiochemical studies of neutron deficient actinide isotopes

    Energy Technology Data Exchange (ETDEWEB)

    Williams, K.E.

    1978-04-01

    The production of neutron deficient actinide isotopes in heavy ion reactions was studied using alpha, gamma, x-ray, and spontaneous fission detection systems. A new isotope of berkelium, /sup 242/Bk, was produced with a cross-section of approximately 10 ..mu..b in reactions of boron on uranium and nitrogen on thorium. It decays by electron capture with a half-life of 7.0 +- 1.3 minutes. The alpha-branching ratio for this isotope is less than 1% and the spontaneous fission ratio is less than 0.03%. Studies of (Heavy Ion, pxn) and (Heavy Ion, ..cap alpha..xn) transfer reactions in comparison with (Heavy ion, xn) compound nucleus reactions revealed transfer reaction cross-sections equal to or greater than the compound nucleus yields. The data show that in some cases the yield of an isotope produced via a (H.I.,pxn) or (H.I.,..cap alpha..xn) reaction may be higher than its production via an xn compound nucleus reaction. These results have dire consequences for proponents of the ''Z/sub 1/ + Z/sub 2/ = Z/sub 1+2/'' philosophy. It is no longer acceptable to assume that (H.I.,pxn) and (H.I.,..cap alpha..xn) product yields are of no consequence when studying compound nucleus reactions. No evidence for spontaneous fission decay of /sup 228/Pu, /sup 230/Pu, /sup 232/Cm, or /sup 238/Cf was observed indicating that strictly empirical extrapolations of spontaneous fission half-life data is inadequate for predictions of half-lives for unknown neutron deficient actinide isotopes.

  2. Actinide Isotopes for the Synthesis of Superheavy Nuclei

    Science.gov (United States)

    Roberto, J. B.; Alexander, C. W.; Boll, R. A.; Dean, D. J.; Ezold, J. G.; Felker, L. K.; Rykaczewski, K. P.

    2014-09-01

    Recent research resulting in the synthesis of isotopes of new elements 113-118 has demonstrated the importance of actinide targets in superheavy element research. Oak Ridge National Laboratory (ORNL) has unique facilities for the production and processing of actinide target materials, including the High Flux Isotope Reactor (HFIR) and the Radiochemical Engineering Development Center (REDC). These facilities have provided actinide target materials that have been used for the synthesis of all superheavy (SHE) elements above Copernicium (element 112). In this paper, the use of actinide targets for SHE research and discovery is described, including recent results for element 117 using 249Bk target material from ORNL. ORNL actinide capabilities are reviewed, including production and separation/purification, availabilities of actinide materials, and future opportunities including novel target materials such as 251Cf.

  3. Microcalorimeter Q-spectroscopy for rapid isotopic analysis of trace actinide samples

    Energy Technology Data Exchange (ETDEWEB)

    Croce, M.P., E-mail: mpcroce@lanl.gov [Los Alamos National Laboratory, Los Alamos, NM (United States); Bond, E.M.; Hoover, A.S.; Kunde, G.J.; Mocko, V.; Rabin, M.W.; Weisse-Bernstein, N.R.; Wolfsberg, L.E. [Los Alamos National Laboratory, Los Alamos, NM (United States); Bennett, D.A.; Hays-Wehle, J.; Schmidt, D.R.; Ullom, J.N. [National Institute of Standards and Technology, Boulder, CO (United States)

    2015-06-01

    We are developing superconducting transition-edge sensor (TES) microcalorimeters that are optimized for rapid isotopic analysis of trace actinide samples by Q-spectroscopy. By designing mechanically robust TESs and simplified detector assembly methods, we have developed a detector for Q-spectroscopy of actinides that can be assembled in minutes. We have characterized the effects of each simplification and present the results. Finally, we show results of isotopic analysis of plutonium samples with Q-spectroscopy detectors and compare the results to mass spectrometry.

  4. The contrasting fission potential-energy structure of actinides and mercury isotopes

    CERN Document Server

    Ichikawa, Takatoshi; Möller, Peter; Sierk, Arnold J

    2012-01-01

    Fission-fragment mass distributions are asymmetric in fission of typical actinide nuclei for nucleon number $A$ in the range $228 \\lnsim A \\lnsim 258$ and proton number $Z$ in the range $90\\lnsim Z \\lnsim 100$. For somewhat lighter systems it has been observed that fission mass distributions are usually symmetric. However, a recent experiment showed that fission of $^{180}$Hg following electron capture on $^{180}$Tl is asymmetric. An earlier experiment has shown fission of $^{198}$Hg and nearby nuclei is symmetric, but with hints of asymmetric yield distributions up to about 10 MeV above the saddle-point energy. We calculate potential-energy surfaces for a typical actinide nucleus and for 12 even isotopes in the range $^{178}$Hg--$^{200}$Hg, demonstrating the radical differences between actinide and mercury potential surfaces. We discuss these differences and how the changing potential-energy structure along the mercury isotope chain affects the observed (a)symmetry of the fission fragments. We show that the ...

  5. Fast methods for determination of antropogenic actinides and U/Th-series isotopes in aqueous samples.

    Science.gov (United States)

    Eikenberg, J; Bajo, S; Beer, H; Hitz, J; Ruethi, M; Zumsteg, I; Letessier, P

    2004-01-01

    Rapid and simple methods are applied at the PSI radioanalytical laboratory for determining anthropogenic actinides in waste and nuclear reactor waters (U, Pu, Am, Cm) as well as for analysis of naturally occurring alpha-emitters in continental river and ground water. Anion exchange chromatography followed by alpha-spectrometry as well as alpha/beta-LSC is applied for the reactor coolant waters. To avoid alpha-spectrum interference between 238Pu and 241Am at 5.5 MeV, the Pu-fraction is purified using anion exchange resin. Prior to the separation of the Pu-fraction, all actinides (U, Pu, Am, Cm) are adsorbed batch-wise under stirring onto Actinide Resin and subsequent decomposition of the reagent. The residue is then re-dissolved in a sulfate buffer solution for electrolytic deposition. In tabular water samples isotopes of Ra and Po are analyzed additionally via sorption onto manganese coated discs (Ra) and deposition on silver discs (Po). For counting times of 1 day and use of 0.1-1l sample aliquots, detection limits of a few mBql(-1) can be obtained easily.

  6. A fast switching electrostatic deflector system for actinide isotopic ratio measurements

    Science.gov (United States)

    Zorko, Benjamin; Child, D. P.; Hotchkis, M. A. C.

    2010-04-01

    We have implemented a fast switching electrostatic system on the actinides beamline on the ANTARES accelerator at ANSTO, to improve the precision of analyses by accelerator mass spectrometry. This high-energy bouncing system is based on a pair of deflector plates, deflecting in the orbit plane, set at the entrance and exit of the analysing magnet. The design of deflector plates is unique, and it was modelled by SIMION in order to minimize field inhomogenity and fringe field effects. The pair of deflector plates are supplied by a high-voltage amplifier driven by an EPICS-enabled control unit, with two 4 W power supplies providing up to ±10 kV modulation. The high-energy bouncing system is synchronized with the existing low-energy bouncing system. To measure the isotopic ratio with the new system, the magnetic fields of the injector and analysing magnets are set to transmit selected isotopes along the beam line with zero voltage applied. The other isotopes of interest are transmitted by keeping the magnetic fields constant and modulating the voltages on the injector magnet chamber and on the high-energy deflector plates.

  7. AMS of actinides in groundwater: development of a new procedure for trace analysis of Np, Pu, Am and Cm isotopes

    Energy Technology Data Exchange (ETDEWEB)

    Quinto, Francesca; Lagos, Markus; Plaschke, Markus; Schaefer, Thorsten; Geckeis, Horst [Karlsruhe Institute of Technology, Institute for Nuclear Waste Disposal (KIT-INE), Hermann-von Helmholtz-Platz 1, D-76344 Eggenstein-Leopoldshafen (Germany); Steier, Peter [VERA Laboratory, Faculty of Physics, University of Vienna, Waehringer Strasse 17, A-1090 Vienna (Austria)

    2014-07-01

    In order to assess the actinides contamination in groundwater, their geochemistry is intensely studied in field and laboratory experiments focusing on speciation and ways of transport through the aquifers. A challenge lies in the analysis of actinides below ppq levels. We present a new analytical protocol suited to the measurement by accelerator mass spectrometry of Np, Pu, Am and Cm isotopes without previous chemical separation from each other. The actinides are quantitatively co-precipitated with Fe-hydroxide from the groundwater specimens. This procedure allows the pre-concentration of the actinides from the bulk elements and their incorporation into a sample matrix suited to the AMS measurements. The chemical yield of the co-precipitation is estimated measuring samples with suitable spikes by HR ICP-MS. At the AMS sytem: (a) the ionization yield of Np, Pu, Am and Cm in the given sample matrix, (b) the maximum number of nuclides per sample allowing detection limits below 0.01 ppq, and (c) the influence of the laboratory background on the results, are determined.

  8. Search for EC-decayed neutron-deficient actinide isotopes using gas-jet coupled JAERI-ISOL

    Energy Technology Data Exchange (ETDEWEB)

    Tsukada, Kazuaki [Japan Atomic Energy Research Inst., Tokai, Ibaraki (Japan). Tokai Research Establishment

    1997-07-01

    To study the nuclear properties of unknown neutron deficient actinide isotopes which decay mainly via orbital electron capture (EC), we have developed a composite system consisting of a gas-jet transport apparatus and a thermal ion-source at the JAERI-ISOL. With this system, search for {sup 236}Am produced in the {sup 235}U({sup 6}Li, 5n) reaction has been performed. Pu KX-rays associated with the EC decay of {sup 236}Am are observed at the mass-236 fraction. The half-life of {sup 236}Am is evaluated to be 4.4min. The outline of the gas-jet coupled JAERI-ISOL system and typical performance are given. (author)

  9. Dynamical approach to isotopic-distribution of fission fragments from actinide nuclei

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    Ishizuka Chikako

    2016-01-01

    Full Text Available Measurements of the isotope distribution of fission fragments, often denoted as the primary fission yield (pre-neutron yield or independent fission yield (post-neutron yield are still challenging at low excitation energies, so that it is important to investigate it within a theory. Such quantities are vital for applications as well. In this study, fragment distributions from the fission of U isotopes at low excitation energies are studied using a dynamical model. The potential energy surface is derived from the two center shell model including the shell and pairing corrections. In order to calculate the charge distribution of fission fragments, we introduce a new parameter ηZ as the charge asymmetry, in addition to three parameters describing a nuclear shape, z as the distance between two centers of mass, δ as fragment deformation, and ηA as the mass asymmetry. Using this model, we calculated the isotopic distribution of 236U for the n-induced process 235U + n → 236U at low excitation energies. As a result, we found that the current model can well reproduce isotopic fission-fragment distribution which can be compared favorably with major libraries.

  10. Dynamical approach to isotopic-distribution of fission fragments from actinide nuclei

    Science.gov (United States)

    Ishizuka, Chikako; Chiba, Satoshi; Karpov, Alexander V.; Aritomo, Yoshihiro

    2016-06-01

    Measurements of the isotope distribution of fission fragments, often denoted as the primary fission yield (pre-neutron yield) or independent fission yield (post-neutron yield) are still challenging at low excitation energies, so that it is important to investigate it within a theory. Such quantities are vital for applications as well. In this study, fragment distributions from the fission of U isotopes at low excitation energies are studied using a dynamical model. The potential energy surface is derived from the two center shell model including the shell and pairing corrections. In order to calculate the charge distribution of fission fragments, we introduce a new parameter ηZ as the charge asymmetry, in addition to three parameters describing a nuclear shape, z as the distance between two centers of mass, δ as fragment deformation, and ηA as the mass asymmetry. Using this model, we calculated the isotopic distribution of 236U for the n-induced process 235U + n → 236U at low excitation energies. As a result, we found that the current model can well reproduce isotopic fission-fragment distribution which can be compared favorably with major libraries.

  11. Accelerator Mass Spectrometry of Actinides in Ground- and Seawater: An Innovative Method Allowing for the Simultaneous Analysis of U, Np, Pu, Am, and Cm Isotopes below ppq Levels.

    Science.gov (United States)

    Quinto, Francesca; Golser, Robin; Lagos, Markus; Plaschke, Markus; Schäfer, Thorsten; Steier, Peter; Geckeis, Horst

    2015-06-02

    (236)U, (237)Np, and Pu isotopes and (243)Am were determined in ground- and seawater samples at levels below ppq (fg/g) with a maximum sample size of 250 g. Such high sensitivity was possible by using accelerator mass spectrometry (AMS) at the Vienna Environmental Research Accelerator (VERA) with extreme selectivity and recently improved efficiency and a significantly simplified separation chemistry. The use of nonisotopic tracers was investigated in order to allow for the determination of (237)Np and (243)Am, for which isotopic tracers either are rarely available or suffer from various isobaric mass interferences. In the present study, actinides were concentrated from the sample matrix via iron hydroxide coprecipitation and measured sequentially without previous chemical separation from each other. The analytical method was validated by the analysis of the Reference Material IAEA 443 and was applied to groundwater samples from the Colloid Formation and Migration (CFM) project at the deep underground rock laboratory of the Grimsel Test Site (GTS) and to natural water samples affected solely by global fallout. While the precision of the presented analytical method is somewhat limited by the use of nonisotopic spikes, the sensitivity allows for the determination of ∼10(5) atoms in a sample. This provides, e.g., the capability to study the long-term release and retention of actinide tracers in field experiments as well as the transport of actinides in a variety of environmental systems by tracing contamination from global fallout.

  12. Isotope Trace Studies of Diffusion in Silicates and of Geological Transport Processes Using Actinide Elements

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    Prof. G. J. Wasserburg

    2001-01-19

    Over the past year we have competed two studies of Os concentration and isotopic composition in rivers from the Himalayan uplift and in hydrothermal fluids from the Juan de Fuca Ridge. Both of these studies have been published. We have completed a study of paleo-climate in Soreq Cave, Israel, and have expanded our studies of the transport of U-Th through riverine and estuarine environments. We are completing two studies of weathering and transport in the vadose in two very different environments--one a tropical regime with a deep laterite profile and the other a northern arboreal forest with only a thin weathering zone. We have begun a new study of U-Th in aquifers with low water velocity.

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

    Energy Technology Data Exchange (ETDEWEB)

    G. Palmiottti; H. Hiruta; M. Salvatores

    2011-09-01

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

  14. Diets of introduced predators using stable isotopes and stomach contents

    Science.gov (United States)

    Meckstroth, A.M.; Miles, A.K.; Chandra, S.

    2007-01-01

    In a study of predation on ground-nesting birds at South San Francisco Bay (South Bay), California, USA, we analyzed stomach contents and stable isotopes of carbon and nitrogen to identify commonly consumed prey. We obtained the stomach contents from 206 nonnative red foxes (Vulpes vulpes regalis) collected in the South Bay area and Monterey County during 1995-2001 and from 68 feral cats (Felis silvestris) from the South Bay area during 2001-2002. We determined prey identity, biomass, and frequency, described seasonal diet trends, and derived an Index of Relative Importance. Avian species were the most frequent prey we found in the stomachs of red foxes from South Bay (61%), whereas small rodents were most frequent for red foxes from Monterey County (62%). Small rodents were the most frequent prey we found in feral cats (63%). Carbon and nitrogen isotopic signatures for foxes supported stomach content findings. However, isotope results indicated that cats received a majority of their energy from a source other than rodents and outside the natural system, which differed from the stomach content analysis. We demonstrated the utility of both stable isotope and stomach content analyses to establish a more complete understanding of predators' diets. This information aids natural resource managers in planning and evaluating future predator-removal programs and increases our understanding of the impacts of nonnative foxes and cats on native species.

  15. Actinides-1981

    Energy Technology Data Exchange (ETDEWEB)

    1981-09-01

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

  16. Isotope tracer studies of diffusion in silicates and of geological transport processes using actinide elements. Progress report

    Energy Technology Data Exchange (ETDEWEB)

    Wasserburg, G.J.

    1992-12-31

    The following are reported: high abundance sensitivity mass spectrometer for U-Th studies; {sup 238}U-{sup 230}Th disequilibrium in recent lavas from Iceland; water-rock interaction from U-Th studies; resonance ionization mass spectrometry of Os and Ti isotopes; and self-diffusion of Mg.

  17. Extending FEAST-METAL for analysis of low content minor actinide bearing and zirconium rich metallic fuels for sodium fast reactors

    Science.gov (United States)

    Karahan, Aydın

    2011-07-01

    Computational models in FEAST-METAL fuel behaviour code have been upgraded to simulate minor actinide bearing zirconium rich metallic fuels for use in sodium fast reactors. Increasing the zirconium content to 20-40 wt.% causes significant changes in fuel slug microstructure affecting thermal, mechanical, chemical, and fission gas behaviour. Inclusion of zirconium rich phase reduces the fission gas swelling rate significantly in early irradiation. Above the threshold fission gas swelling, formation of micro-cracks, and open pores increase material compliancy enhance diffusivity, leading to rapid fuel gas swelling, interconnected porosity development and release of the fission gases and helium. Production and release of helium was modelled empirically as a function of americium content and fission gas production, consistent with previous Idaho National Laboratory studies. Predicted fuel constituent redistribution is much smaller compared to typical U-Pu-10Zr fuel operated at EBR-II. Material properties such as fuel thermal conductivity, modulus of elasticity, and thermal expansion coefficient have been approximated using the available database. Creep rate and fission gas diffusivity of high zirconium fuel is lowered by an order of magnitude with respect to the reference low zirconium fuel based on limited database and in order to match experimental observations. The new code is benchmarked against the AFC-1F fuel assembly post irradiation examination results. Satisfactory match was obtained for fission gas release and swelling behaviour. Finally, the study considers a comparison of fuel behaviour between high zirconium content minor actinide bearing fuel and typical U-15Pu-6Zr fuel pins with 75% smear density. The new fuel has much higher fissile content, allowing for operating at lower neutron flux level compared to fuel with lower fissile density. This feature allows the designer to reach a much higher burnup before reaching the cladding dose limit. On the other

  18. Ventilation system of actinides handling facility in Oarai-branch of Tohoku University

    Energy Technology Data Exchange (ETDEWEB)

    Suzuki, Yoshimitsu; Watanabe, Makoto; Hara, Mituo; Shikama, Tatsuo; Kayano, Hideo; Mitsugashira, Toshiaki [Oarai Branch, Institute for Materials Research, Tohoku Univ., Oarai, Ibaraki (Japan)

    1999-09-01

    We have reported the development of the facility for handling actinides in Tohoku University at the second KAERI-JAERI joint seminar on PIE technology. Actinide isotopes have most hazurdous {alpha}-radioactivity. Therefore, a specially designed facility is necessary to carry out experimental study for actinide physics and chemistry. In this paper, we will describe the ventilation system and monitoring system for actinide handling facility. (author)

  19. Dietary interpretations for extinct megafauna using coprolites, intestinal contents and stable isotopes: Complimentary or contradictory?

    Science.gov (United States)

    Rawlence, Nicolas J.; Wood, Jamie R.; Bocherens, Herve; Rogers, Karyne M.

    2016-06-01

    For many extinct species, direct evidence of diet (e.g. coprolites, gizzard/intestinal contents) is not available, and indirect dietary evidence (e.g. stable isotopes) must be relied upon. The Late Holocene fossil record of New Zealand provides a unique opportunity to contrast palaeodietary reconstructions for the extinct moa (Aves: Dinornithiformes) using stable isotopes and coprolite/gizzard contents. Palaeodietary reconstructions from isotopes are found to contradict those based on direct dietary evidence. We discuss reasons for this and advocate, where possible, for the use of multiple lines of evidence in reconstructing the diets of extinct species.

  20. Post-depositional changes in snow isotope content: preliminary results of laboratory experiments

    Directory of Open Access Journals (Sweden)

    A. A. Ekaykin

    2009-10-01

    Full Text Available Isotopic content of the snow and firn thickness is assumed to be altered significantly due to the post-depositional (PD mass- and isotope exchange with the atmospheric water vapor. If so, these effects should be accounted for in the ice core-based isotope-temperature paleo-reconstructions. In order to study the intensity of the PD processes we set up a series of laboratory experiments. In this paper we describe in detail the experimental technique and briefly overview preliminary results. It is shown that the PD modifications in the upper layer of snow thickness are noticeably strong even under such a low temperature as −35°C (the value typical for the Central Antarctic summer. It is demonstrated that the PD isotopic changes in snow can be approximated as a linear function of the relative mass loss due to snow sublimation. Possible applications for improving the isotope-temperature paleo-reconstructions are shortly discussed.

  1. Possibilities of synthesis of unknown isotopes of superheavy nuclei with charge numbers Z > 108 in asymmetric actinide-based complete fusion reactions

    Energy Technology Data Exchange (ETDEWEB)

    Hong, Juhee [Institute for Basic Science, Rare Isotope Science Project, Daejeon (Korea, Republic of); Adamian, G.G. [Joint Institute for Nuclear Research, Dubna (Russian Federation); Antonenko, N.V. [Joint Institute for Nuclear Research, Dubna (Russian Federation); Tomsk Polytechnic University, Mathematical Physics Department, Tomsk (Russian Federation)

    2016-10-15

    The possibilities of production of new isotopes of superheavy nuclei with charge numbers Z = 109-114 in various asymmetric hot fusion reactions are studied for the first time. The excitation functions of the formation of these isotopes in the xn evaporation channels are predicted and the optimal conditions for the synthesis are proposed. The products of the suggested reactions can fill a gap of unknown isotopes between the isotopes of the heaviest nuclei obtained in cold and hot complete fusion reactions. (orig.)

  2. Possibilities of synthesis of unknown isotopes of superheavy nuclei with charge numbers Z > 108 in asymmetric actinide-based complete fusion reactions

    Science.gov (United States)

    Hong, Juhee; Adamian, G. G.; Antonenko, N. V.

    2016-10-01

    The possibilities of production of new isotopes of superheavy nuclei with charge numbers Z = 109-114 in various asymmetric hot fusion reactions are studied for the first time. The excitation functions of the formation of these isotopes in the xn evaporation channels are predicted and the optimal conditions for the synthesis are proposed. The products of the suggested reactions can fill a gap of unknown isotopes between the isotopes of the heaviest nuclei obtained in cold and hot complete fusion reactions.

  3. Nitrogen isotope and content record of Mesozoic orogenic gold deposits surrounding the North China craton

    Institute of Scientific and Technical Information of China (English)

    2003-01-01

    As an effective tracer, nitrogen isotopes have been used to determine the source of ore materials in recent years. In this study, the nitrogen isotopes and contents were measured on K- feldspar and sericite of gold deposits and some related granitic intrusions in Jiaodong, Xiaoqinling-Xiong'ershan, west Qinling, the west part of North Qilian and the Zhangjiakou-Xuanhua district around the North China craton (NCC). Although the gold deposits around the NCC are hosted in Precambrian metamorphic rocks, Phanerozoic sedimentary rocks, mafic volcanic rocks or granite, comparison of which with the nitrogen contents and isotope data of previous studies on mantle-derived rocks, granites, metamorphic rocks and gold deposits indicates that those deposits are closely related to granitic rocks. In addition, mantle-derived materials may have been involved in the ore-forming processes to a certain degree. This conclusion is consistent with the result of previous hydrogen, oxygen and carbon isotopic studies of those gold deposits.

  4. Integrating stomach content and stable isotope analyses to quantify the diets of pygoscelid penguins.

    Directory of Open Access Journals (Sweden)

    Michael J Polito

    Full Text Available Stomach content analysis (SCA and more recently stable isotope analysis (SIA integrated with isotopic mixing models have become common methods for dietary studies and provide insight into the foraging ecology of seabirds. However, both methods have drawbacks and biases that may result in difficulties in quantifying inter-annual and species-specific differences in diets. We used these two methods to simultaneously quantify the chick-rearing diet of Chinstrap (Pygoscelis antarctica and Gentoo (P. papua penguins and highlight methods of integrating SCA data to increase accuracy of diet composition estimates using SIA. SCA biomass estimates were highly variable and underestimated the importance of soft-bodied prey such as fish. Two-source, isotopic mixing model predictions were less variable and identified inter-annual and species-specific differences in the relative amounts of fish and krill in penguin diets not readily apparent using SCA. In contrast, multi-source isotopic mixing models had difficulty estimating the dietary contribution of fish species occupying similar trophic levels without refinement using SCA-derived otolith data. Overall, our ability to track inter-annual and species-specific differences in penguin diets using SIA was enhanced by integrating SCA data to isotopic mixing modes in three ways: 1 selecting appropriate prey sources, 2 weighting combinations of isotopically similar prey in two-source mixing models and 3 refining predicted contributions of isotopically similar prey in multi-source models.

  5. CORRESPONDENCE OF STABLE ISOTOPE AND GUT CONTENTS ANALYSES IN DETERMINING TROPHIC POSITION OF STREAM FISHES

    Science.gov (United States)

    It is generally accepted that both stable isotope analysis (SIA) and gut contents analysis (GCA) be used in food web studies; however, few researchers have analyzed these data in concert. We utilized SIA and GCA to determine if longitudinal and seasonal variation in diet affects...

  6. Comparing trophic position of stream fishes using stable isotope and gut contents analyses

    Science.gov (United States)

    Stable isotope analysis (SIA) and gut content analysis (GCA) are commonly used in food web studies, but few studies analyze these data in concert. We used SIA and GCA to identify diets and trophic position (TP) of six stream fishes and to compare TP estimates between methods. Ord...

  7. PREFACE: Actinides 2009

    Science.gov (United States)

    Rao, Linfeng; Tobin, James G.; Shuh, David K.

    2010-07-01

    This volume of IOP Conference Series: Materials Science and Engineering consists of 98 papers that were presented at Actinides 2009, the 8th International Conference on Actinide Science held on 12-17 July 2009 in San Francisco, California, USA. This conference was jointly organized by Lawrence Livermore National Laboratory and Lawrence Berkeley National Laboratory. The Actinides conference series started in Baden-Baden, Germany (1975) and this first conference was followed by meetings at Asilomar, CA, USA (1981), Aix-en-Provence, France (1985), Tashkent, USSR (1989), Santa Fe, NM, USA (1993), Baden-Baden, Germany (1997), Hayama, Japan (2001), and Manchester, UK (2005). The Actinides conference series provides a regular venue for the most recent research results on the chemistry, physics, and technology of the actinides and heaviest elements. Actinides 2009 provided a forum spanning a diverse range of scientific topics, including fundamental materials science, chemistry, physics, environmental science, and nuclear fuels. Of particular importance was a focus on the key roles that basic actinide chemistry and physics research play in advancing the worldwide renaissance of nuclear energy. Editors Linfeng Rao Lawrence Berkeley National Laboratory (lrao@lbl.gov) James G Tobin Lawrence Livermore National Laboratory (tobin1@llnl.gov) David K Shuh Lawrence Berkeley National Laboratory (dkshuh@lbl.gov)

  8. Chemistry of actinides; Chimie des actinides

    Energy Technology Data Exchange (ETDEWEB)

    Vitorge, P. [CEA/Saclay, Dept. d' Entreposage et de Stockage des Dechets (DESD), 91 - Gif-sur-Yvette (France)

    1999-07-01

    This article gives the basic data of the actinides chemistry, describes then qualitatively the main parts of the fuel cycle and concludes with quantitative data. The theoretical recalls give qualitative notions to explain the chemical reactivity of actinides and to understand thus the values of the thermodynamic data which allow quantitative anticipations at equilibrium. The Thermodynamic Data Base (TDB) of the NEA-OECD and the CEA in France have recently estimated some of them in using and developing methodologies whose some are presented here. Some current problems of actinides chemistry are described: analysis of the possibilities to (1)improve the reprocessing of long-lived actinides (2)anticipate their behaviour in the environment in order to compare the impact of the different options of the wastes management. The Pourbaix diagrams summarize the chemistry in solution; the author has added information on the solubility, the influence of the ionic strength and of the complexes formation in bicarbonate/carbonate (HCO{sub 3}{sup -}/CO{sub 3}{sup 2-}) media. The discussion on the choice of the equilibrium constants allows to point out the particular points, the dubiousness and the data which have to be proved. (O.M.)

  9. Design of unique pins for irradiation of higher actinides in a fast reactor

    Energy Technology Data Exchange (ETDEWEB)

    Basmajian, J.A.; Birney, K.R.; Weber, E.T.; Adair, H.L.; Quinby, T.C.; Raman, S.; Butler, J.K.; Bateman, B.C.; Swanson, K.M.

    1982-03-01

    The actinides produced by transmutation reactions in nuclear reactor fuels are a significant factor in nuclear fuel burnup, transportation and reprocessing. Irradiation testing is a primary source of data of this type. A segmented pin design was developed which provides for incorporation of multiple specimens of actinide oxides for irradiation in the UK's Prototype Fast Reactor (PFR) at Dounreay Scotland. Results from irradiation of these pins will extend the basic neutronic and material irradiation behavior data for key actinide isotopes.

  10. Influence of bacteria on lanthanide and actinide transfer from specific soil components (humus, soil minerals and vitrified municipal solid waste incinerator bottom ash) to corn plants: Sr-Nd isotope evidence

    Energy Technology Data Exchange (ETDEWEB)

    Aouad, Georges [Ecole et Observatoire des Sciences de la Terre, Centre de Geochimie de la Surface/CNRS UMR 7517, 1 rue Blessig, 67084 Strasbourg Cedex (France); Stille, Peter [Ecole et Observatoire des Sciences de la Terre, Centre de Geochimie de la Surface/CNRS UMR 7517, 1 rue Blessig, 67084 Strasbourg Cedex (France)]. E-mail: pstille@illite.u-strasbg.fr; Crovisier, Jean-Louis [Ecole et Observatoire des Sciences de la Terre, Centre de Geochimie de la Surface/CNRS UMR 7517, 1 rue Blessig, 67084 Strasbourg Cedex (France); Geoffroy, Valerie A. [UMR 7156 Universite Louis-Pasteur/CNRS, Genetique Moleculaire, Genomique Microbiologie, Departement Micro-organisme, Genomes, Environnement, 28 rue Goethe, 67083 Strasbourg Cedex (France); Meyer, Jean-Marie [UMR 7156 Universite Louis-Pasteur/CNRS, Genetique Moleculaire, Genomique Microbiologie, Departement Micro-organisme, Genomes, Environnement, 28 rue Goethe, 67083 Strasbourg Cedex (France); Lahd-Geagea, Majdi [Ecole et Observatoire des Sciences de la Terre, Centre de Geochimie de la Surface/CNRS UMR 7517, 1 rue Blessig, 67084 Strasbourg Cedex (France)

    2006-11-01

    Experiments have been performed to test the stability of vitrified municipal solid waste (MSW) incinerator bottom ash under the presence of bacteria (Pseudomonas aeruginosa) and plants (corn). The substratum used for the plant growth was a humus-rich soil mixed with vitrified waste. For the first time, information on the stability of waste glasses in the presence of bacteria and plants is given. Results show that inoculated plant samples contained always about two times higher lanthanide and actinide element concentrations. Bacteria support the element transfer since plants growing in inoculated environment developed a smaller root system but have higher trace element concentrations. Compared with the substratum, plants are light rare earth element (LREE) enriched. The vitrified bottom ash has to some extent been corroded by bacteria and plant activities as indicated by the presence of Nd (REE) and Sr from the vitrified waste in the plants. {sup 87}Sr/{sup 86}Sr and {sup 143}Nd/{sup 144}Nd isotope ratios of plants and soil components allow the identification of the corroded soil components and confirm that bacteria accelerate the assimilation of elements from the vitrified bottom ash. These findings are of importance for landfill disposal scenarios, and similar experiments should be performed in order to better constrain the processes of microbially mediated alteration of the MSW glasses in the biosphere.

  11. Subsurface Biogeochemistry of Actinides

    Energy Technology Data Exchange (ETDEWEB)

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

    2016-06-29

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

  12. Helium and fission gas behaviour in magnesium aluminate spinel and zirconia for actinide transmutation

    NARCIS (Netherlands)

    Damen, P.M.G.

    2003-01-01

    In order to reduce the long-term radiotoxicity of spent nuclear fuel, many studies are performed on partitioning and transmutation of actinides. In such a scenario, the long-lived radio-isotopes (mostly actinides) are partitioned from the nuclear waste, and subsequently transmuted or fissioned in a

  13. Production of heavy actinides in incomplete fusion reactions

    Science.gov (United States)

    Antonenko, N. V.; Cherepanov, E. A.; Iljinov, A. S.; Mebel, M. V.

    1994-10-01

    We present preliminary results of calculations by the phenomenological model of the estimated yield of some heavy actinide isotopes. It is assumed that these isotopes are produced as a result of multinucleon transfers followed by neutrons and charged particle emission A.S. Iljinov and E.A. Cherepanov (1980). The yield P(sub Z, N)(E*) of primary excited actinides is found using the model of N.V. Antonenko and R.V. Jolos (1991). Absolute cross-sections for different binary reaction channels are obtained by summing the cross-sections for all subchannels with an appreciable yield according to J. Wilczynski et al. (1980).

  14. Reconstruction of the isotope activity content of heterogeneous nuclear waste drums.

    Science.gov (United States)

    Krings, Thomas; Mauerhofer, Eric

    2012-07-01

    Radioactive waste must be characterized in order to verify its conformance with national regulations for intermediate storage or its disposal. Segmented gamma scanning (SGS) is a most widely applied non-destructive analytical technique for the characterization of radioactive waste drums. The isotope specific activity content is generally calculated assuming a homogeneous matrix and activity distribution for each measured drum segment. However, real radioactive waste drums exhibit non-uniform isotope and density distributions most affecting the reliability and accuracy of activities reconstruction in SGS. The presence of internal shielding structures in the waste drum contributes generally to a strong underestimation of the activity and this in particular for radioactive sources emitting low energy gamma-rays independently of their spatial distribution. In this work we present an improved method to quantify the activity of spatially concentrated gamma-emitting isotopes (point sources or hot spots) in heterogeneous waste drums with internal shielding structures. The isotope activity is reconstructed by numerical simulations and fits of the angular dependent count rate distribution recorded during the drum rotation in SGS using an analytical expression derived from a geometric model. First results of the improved method and enhancements of this method are shown and are compared to each other as well as to the conventional method which assumes a homogeneous matrix and activity distribution. It is shown that the new model improves the accuracy and the reliability of the activity reconstruction in SGS and that the presented algorithm is suitable with respect to the framework requirement of industrial application.

  15. Diet of invasive lionfish on hard bottom reefs of the Southeast USA: insights from stomach contents and stable isotopes

    Data.gov (United States)

    National Oceanic and Atmospheric Administration, Department of Commerce — Stomach contents and stable isotope analyses were used to determine the diet of lionfish in the warm-temperate hard bottom reef community in theSoutheast US Atlantic...

  16. Scenarios for the transmutation of actinides in CANDU reactors

    Energy Technology Data Exchange (ETDEWEB)

    Hyland, Bronwyn, E-mail: hylandb@aecl.ca [Atomic Energy of Canada Limited, Chalk River Laboratories, Chalk River, Ontario, K0J 1J0 (Canada); Gihm, Brian, E-mail: gihmb@aecl.ca [Atomic Energy of Canada Limited, 2251 Speakman Drive, Mississauga, Ontario, L5K 1B2 (Canada)

    2011-12-15

    With world stockpiles of used nuclear fuel increasing, the need to address the long-term utilization of this resource is being studied. Many of the transuranic (TRU) actinides in nuclear spent fuel produce decay heat for long durations, resulting in significant nuclear waste management challenges. These actinides can be transmuted to shorter-lived isotopes to reduce the decay heat period or consumed as fuel in a CANDU(R) reactor. Many of the design features of the CANDU reactor make it uniquely adaptable to actinide transmutation. The small, simple fuel bundle simplifies the fabrication and handling of active fuels. Online refuelling allows precise management of core reactivity and separate insertion of the actinides and fuel bundles into the core. The high neutron economy of the CANDU reactor results in high TRU destruction to fissile-loading ratio. This paper provides a summary of actinide transmutation schemes that have been studied in CANDU reactors at AECL, including the works performed in the past. The schemes studied include homogeneous scenarios in which actinides are uniformly distributed in all fuel bundles in the reactor, as well as heterogeneous scenarios in which dedicated channels in the reactor are loaded with actinide targets and the rest of the reactor is loaded with fuel. The transmutation schemes that are presented reflect several different partitioning schemes. Separation of americium, often with curium, from the other actinides enables targeted destruction of americium, which is a main contributor to the decay heat 100-1000 years after discharge from the reactor. Another scheme is group-extracted transuranic elements, in which all of the transuranic elements, plutonium (Pu), neptunium (Np), americium (Am), and curium (Cm) are extracted together and then transmuted. This paper also addresses ways of utilizing the recycled uranium, another stream from the separation of spent nuclear fuel, in order to drive the transmutation of other actinides.

  17. From carbon to actinides: A new universal 1MV accelerator mass spectrometer at ANSTO

    Science.gov (United States)

    Wilcken, K. M.; Hotchkis, M.; Levchenko, V.; Fink, D.; Hauser, T.; Kitchen, R.

    2015-10-01

    A new 1 MV NEC pelletron AMS system at ANSTO is presented. The spectrometer comprises large radius magnets for actinide measurements. A novel feature of the system is fast switching between isotopes both at low and high energy sections allowing measurements of up to 8 isotopes within a single sequence. Technical details and layout of the spectrometer is presented. Performance data for 14C, 10Be, 26Al and actinides demonstrate the system is ready for routine AMS measurements.

  18. From carbon to actinides: A new universal 1MV accelerator mass spectrometer at ANSTO

    Energy Technology Data Exchange (ETDEWEB)

    Wilcken, K.M., E-mail: klaus.wilcken@ansto.gov.au [Australian Nuclear Science & Technology Organisation, Sydney, New South Wales (Australia); Hotchkis, M.; Levchenko, V.; Fink, D. [Australian Nuclear Science & Technology Organisation, Sydney, New South Wales (Australia); Hauser, T.; Kitchen, R. [National Electrostatics Corporation, 7540 Graber Road, Middleton, WI 53562-0310 (United States)

    2015-10-15

    A new 1 MV NEC pelletron AMS system at ANSTO is presented. The spectrometer comprises large radius magnets for actinide measurements. A novel feature of the system is fast switching between isotopes both at low and high energy sections allowing measurements of up to 8 isotopes within a single sequence. Technical details and layout of the spectrometer is presented. Performance data for {sup 14}C, {sup 10}Be, {sup 26}Al and actinides demonstrate the system is ready for routine AMS measurements.

  19. The carbon isotopes ratio and trace metals content determinations in some Transylvanian fruit juices

    Science.gov (United States)

    Dehelean, A.; Magdas, D. A.; Cristea, G.

    2012-02-01

    This work presents a preliminary study on the carbon isotope signature and trace metal content investigated on the soil-plant-fruit pulp chain. The samples were collected from two Transylvanian areas namely Alba and Salaj. The average value of the δ13C at the soil surface was around δ13C ≈ -27%° and important differences of the δ13C values between the two studied areas were not observed. Meanwhile, differences between fruit pulp of grape juice and the pulp of pear juice relived a difference of about 1.5%° for δ13C values.

  20. A Summary of Actinide Enrichment Technologies and Capability Gaps

    Energy Technology Data Exchange (ETDEWEB)

    Patton, Bradley D. [Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); Robinson, Sharon M. [Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)

    2017-01-01

    The evaluation performed in this study indicates that a new program is needed to efficiently provide a national actinide radioisotope enrichment capability to produce milligram-to-gram quantities of unique materials for user communities as summarized in Table 1. This program xiv should leverage past actinide enrichment, the recent advances in stable isotope enrichment, and assessments of the future requirements to cost effectively develop this capability while establishing an experience base for a new generation of researchers in this vital area. Preliminary evaluations indicate that an EMIS device would have the capability to meet the future needs of the user community for enriched actinides. The EMIS technology could be potentially coupled with other enrichment technologies, such as irradiation, as pre-enrichment and/or post-enrichment systems to increase the throughput, reduce losses of material, and/or reduce operational costs of the base EMIS system. Past actinide enrichment experience and advances in the EMIS technology applied in stable isotope separations should be leveraged with this new evaluation information to assist in the establishment of a domestic actinide radioisotope enrichment capability.

  1. Metal Content and Stable Isotope Determination in Some Commercial Beers from Romanian Markets

    Directory of Open Access Journals (Sweden)

    Cezara Voica

    2015-01-01

    Full Text Available Characterization of beer samples is of interest because their compositions affect the taste and stability of beer and, also, consumer health. In this work, the characterizations of 20 Romanian beers were performed by mean of Inductively Coupled Plasma Mass Spectrometry (ICP-MS and Isotope Ratio Mass Spectrometry (IRMS in order to trace heavy metals and isotopic content of them. Major, minor, and trace metals are important in beer fermentation since they supply the appropriate environment for yeast growth and influence yeast metabolism. Beside this, the presence of the C4 plants in the brewing process was followed. Our study has shown that the analyzed beers indicated the presence of different plant types used in brewing: C3, C3-C4 mixtures, and also C4, depending on producers. Also the trace metal content of each sample is presented and discussed in this study. A comparison of the beers quality manufactured by the same producer but bottled in different type of packaging like glass, dose, or PET was made; our results show that no compositional differences among the same beer type exist.

  2. The Carbon Isotopic Content and Concentration of Ambient Formic and Acetic Acid

    Science.gov (United States)

    Johnson, Bryan Jay

    A direct method for source determination of atmospheric formic and acetic acid, through carbon isotopic analysis of the ambient acids and their potential sources, has been successfully developed and tested. These first carbon isotopic measurements of formic acid in the atmosphere were found to be fairly constant, regardless of location. This is consistent with a single dominating source of formic acid, with vegetation emissions being the most likely controlling source. Collection of relatively large quantities (0.3 -3.0 mg) of the organic acids, which was necessary for carbon isotopic measurements, was effectively accomplished by a new method using calcium hydroxide-treated filters with a high-volume sampler. Samples were collected on a regular basis at Mount Lemmon, Arizona (elevation = 9200 feet A.S.L.). Atmospheric concentrations showed a well-defined seasonal pattern, with the lowest concentrations (about 0.2 ppbv) occurring in the middle of the winter, which steadily increased to a maximum of nearly 2 ppbv in the summer. The ^{13}C content (delta ^{13}C) of HCOOH averaged -20.9 +/- 2.5 ^0/_{00 } during the growing season (April-September) and -23.2 +/- 3.5 ^0/_{00} during the non-growing season at Mount Lemmon. Isotopic measurements of formic acid from several other locations included two west coast marine sites ( delta ^{13} C range of -19.1 to -24.6 ^0/_{00} ), three Colorado Rocky Mountain samples averaging -23.2 +/- 1.0 ^0/_{00}, two from the prairie of North Dakota (-23.5 +/- 1.0 ^0/ _{00}) and three samples collected in the urban Tucson, Arizona area (- 20.8 +/- 3.4 ^0 /_{00}). Source measurements included HCOOH emissions from two species of formicine ants (-18.8 +/- 1.7 ^0/_ {00}), and HCOOH in automobile exhaust (-28 ^0/ _{00} from leaded gasoline, and -48.6 ^0/ _{00} from unleaded). Further support for a biogenic source of atmospheric HCOOH came from the carbon-14 analysis of six Mount Lemmon HCOOH samples (93-113% modern carbon), using accelerator

  3. Status of nuclear data for actinides

    Energy Technology Data Exchange (ETDEWEB)

    Guzhovskii, B.Y.; Gorelov, V.P.; Grebennikov, A.N. [Russia Federal Nuclear Centre, Arzamas (Russian Federation)] [and others

    1995-10-01

    Nuclear data required for transmutation problem include many actinide nuclei. In present paper the analysis of neutron fission, capture, (n,2n) and (n,3n) reaction cross sections at energy region from thermal point to 14 MeV was carried out for Th, Pa, U, Np, Pu, Am and Cm isotops using modern evaluated nuclear data libraries and handbooks of recommended nuclear data. Comparison of these data indicates on substantial discrepancies in different versions of files, that connect with quality and completeness of original experimental data.

  4. Device for Detecting Actinides, Method for Detecting Actinides

    Energy Technology Data Exchange (ETDEWEB)

    Stevens, Fred J.; Wilkins-Stevens, Priscilla

    1998-10-29

    A heavy metal detector is provided comprising a first molecule and a second molecule, whereby the first and second molecules interact in a predetermined manner; a first region on the first molecule adapted to interact with an actinide; and a second region on the second molecule adapted to interact with the actinide, whereby the interactions of the actinide with the regions effect the predetermined manner of interaction between the molecules.

  5. Physics studies of higher actinide consumption in an LMR

    Energy Technology Data Exchange (ETDEWEB)

    Hill, R.N.; Wade, D.C.; Fujita, E.K.; Khalil, H.S.

    1990-01-01

    The core physics aspects of the transuranic burning potential of the Integral Fast Reactor (IFR) are assessed. The actinide behavior in fissile self-sufficient IFR closed cycles of 1200 MWt size is characterized, and the transuranic isotopics and risk potential of the working inventory are compared to those from a once-through LWR. The core neutronic performance effects of rare-earth impurities present in the recycled fuel are addressed. Fuel cycle strategies for burning transuranics from an external source are discussed, and specialized actinide burner designs are described. 4 refs., 4 figs., 3 tabs.

  6. PF-4 actinide disposition strategy

    Energy Technology Data Exchange (ETDEWEB)

    Margevicius, Robert W [Los Alamos National Laboratory

    2010-05-28

    The dwindling amount of Security Category I processing and storage space across the DOE Complex has driven the need for more effective storage of nuclear materials at LANL's Plutonium Facility's (PF-4's) vault. An effort was begun in 2009 to create a strategy, a roadmap, to identify all accountable nuclear material and determine their disposition paths, the PF-4 Actinide Disposition Strategy (PADS). Approximately seventy bins of nuclear materials with similar characteristics - in terms of isotope, chemical form, impurities, disposition location, etc. - were established in a database. The ultimate disposition paths include the material to remain at LANL, disposition to other DOE sites, and disposition to waste. If all the actions described in the document were taken, over half of the containers currently in the PF-4 vault would been eliminated. The actual amount of projected vault space will depend on budget and competing mission requirements, however, clearly a significant portion of the current LANL inventory can be either dispositioned or consolidated.

  7. The Stable and Radio- Carbon Isotopic Content of Labile and Refractory Carbon in Atmospheric Particulate Matter

    Science.gov (United States)

    McNichol, A. P.; Rosenheim, B. E.; Gerlach, D. S.; Hayes, J. M.

    2006-12-01

    Studies of the isotopic content of atmospheric particulate matter are hampered by difficulties in chemically defining the pools of carbon and analytically isolating the different pools. We are conducting studies on reference materials and atmospheric aerosol samples to develop a method to measure stable and radio- carbon isotopes on the labile and refractory carbon. We are using a flow-through combustion system that allows us to combust, collect and measure the isotopic content of the gases produced at all stages of heating/oxidizing. We compare our results to those measured using a chemothermal oxidation method (CTO) (Gustafsson et al., 2001). In this method, refractory carbon is defined as the material remaining after pre- combusting a sample at 375°C in the presence of oxygen for 24 hours. The reference materials are diesel soot, apple leaves and a hybrid of the two (DiesApple), all from NIST. These provide carbon with two well-defined fractions -- the soot provides refractory carbon that is radiocarbon dead and the apple leaves provide organic carbon that is radiocarbon modern. Radiocarbon results from DiesApple indicate that the "refractory" carbon defined by the CTO method is actually a mixture of old and modern carbon that contains over 25% modern carbon. This suggests that charred material formed from the apples leaves during the pre-combustion step is contributing to the fraction we identify as refractory carbon. We are studying this by analyzing the individual materials and the mixture using our flow-through system. First results with this system indicate that the refractory fraction trapped from the DiesApple contains much less modern carbon than the CTO method, less than 7%. We will present detailed concentration and isotopic results of the generation of carbon dioxide during programmed combustion of each of the reference materials. We studied the radiocarbon content of both the total carbon (TC) and refractory carbon in the fine particulate matter (PM

  8. Gamma spectroscopy of neutron rich actinide nuclei

    Energy Technology Data Exchange (ETDEWEB)

    Birkenbach, Benedikt; Geibel, Kerstin; Vogt, Andreas; Hess, Herbert; Reiter, Peter; Steinbach, Tim; Schneiders, David [Koeln Univ. (Germany). IKP; Collaboration: AGATA-Collaboration

    2013-07-01

    Excited states in neutron-rich actinide Th and U nuclei were investigated after multi nucleon transfer reactions employing the AGATA demonstrator and PRISMA setup at LNL (INFN, Italy). A primary {sup 136}Xe beam of 1 GeV hitting a {sup 238}U target was used to produce the nuclei of interest. Beam-like reaction products of Xe- and Ba isotopes after neutron transfer were selected by the PRISMA spectrometer. The recoil like particles were registered by a MCP detector inside the scattering chamber. Coincident γ-rays from excited states in beam and target like particles were measured with the position sensitive AGATA HPGe detectors. Improved Doppler correction and quality of the γ-spectra is based on the novel γ-ray tracking technique which was successfully exploited. First results on the collective properties of various Th and U isotopes are discussed.

  9. Actinides in irradiated graphite of RBMK-1500 reactor

    Energy Technology Data Exchange (ETDEWEB)

    Plukienė, R., E-mail: rita@ar.fi.lt; Plukis, A.; Barkauskas, V.; Gudelis, A.; Gvozdaitė, R.; Duškesas, G.; Remeikis, V.

    2014-10-01

    Highlights: • Activation of actinides in the graphite of the RBMK-1500 reactor was analyzed. • Numerical modeling using SCALE 6.1 and MCNPX was used for actinide calculation. • Measurements of the irradiated graphite sample were used for model validation. • Results are important for further decommissioning process of the RBMK type reactors. - Abstract: The activation of graphite in the nuclear power plants is the problem of high importance related with later graphite reprocessing or disposal. The activation of actinide impurities in graphite due to their toxicity determines a particular long term risk to waste management. In this work the activation of actinides in the graphite constructions of the RBMK-1500 reactor is determined by nuclear spectrometry measurements of the irradiated graphite sample from the Ignalina NPP Unit I and by means of numerical modeling using two independent codes SCALE 6.1 (using TRITON-VI sequence) and MCNPX (v2.7 with CINDER). Both models take into account the 3D RBMK-1500 reactor core fragment with explicit graphite construction including a stack and a sleeve but with a different simplification level concerning surrounding graphite and construction of control roads. The verification of the model has been performed by comparing calculated and measured isotope ratios of actinides. Also good prediction capabilities of the actinide activation in the irradiated graphite have been found for both calculation approaches. The initial U impurity concentration in the graphite model has been adjusted taking into account the experimental results. The specific activities of actinides in the irradiated RBMK-1500 graphite constructions have been obtained and differences between numerical simulation results, different structural parts (sleeve and stack) as well as comparison with previous results (Ancius et al., 2005) have been discussed. The obtained results are important for further decommissioning process of the Ignalina NPP and other RBMK

  10. Recovery and chemical purification of actinides at JRC, Karlsruhe

    Science.gov (United States)

    Bokelund, H.; Apostolidis, C.; Glatz, J.-P.

    1989-07-01

    The application of actinide elements in research and in technology is many times subject to rather stringent purity requirements; often a nuclear grade quality is specified. The additional possible demand for a high isotopic purity is a special feature in the handling of these elements. The amount of actinide elements contained in or adhering to materials declared as waste should be low for safety reasons and out of economic considerations. The release of transuranium elements to the environment must be kept negligible. For these and for other reasons a keen interest in the separation of actinides from various materials exists, either for a re-use through recycling, or for their safe confinement in waste packages. This paper gives a short review of the separation methods used for recovery and purification of actinide elements over the past years in the European Institute for Transuranium Elements. The methods described here involve procedures based on precipitation, ion exchange or solvent extraction; often used in a combination. The extraction methods were preferably applied in a Chromatographie column mode. The actinide elements purified and/or separated from each other by the above methods include uranium, neptunium, plutonium, americium, curium, and californium. For the various elements the work was undertaken with different aims, ranging from reprocessing and fabrication of nuclear fuels on a kilogramme scale, over the procurement of alpha-free waste, to the preparation of neutron sources of milligramme size.

  11. Sulfur contents and sulfur-isotope compositions of thiotrophic symbioses in bivalve molluscs and vestimentiferan worms

    Science.gov (United States)

    Vetter, R.D.; Fry, B.

    1998-01-01

    Total sulfur (S(TOT)), elemental sulfur (S??) and sulfur-isotope compositions (??34S) of marine animals were analyzed to determine whether these chemical characteristics could help distinguish animals with a sulfur-based, thiotrophic nutrition from animals whose nutrition is based on methanotrophy or on more normal consumption of phytoplankton-derived organic matter. The presence of S??was almost entirely confined to the symbiont-containing tissues of thiotrophs, but was sometimes undetectable in thiotrophic species where sulfide availability was probably low. When S??contents were subtracted, the remaining tissue-sulfur concentrations were similar for all nutritional groups. ??34S values were typically lower for thiotrophs than for other groups, although there was overlap in methanotroph and thiotroph values at some sites. Field evidence supported the existence of small to moderate (1 to 10???)34S fractionations in the uptake of sulfides and metabolism of thiosulfate. In general, a total sulfur content of >3% dry weight, the presence of elemental sulfur, and ??34S values less than + 5??? can be used to infer a thiotrophic mode of nutrition.

  12. Effects of shock and Martian alteration on Tissint hydrogen isotope ratios and water content

    Science.gov (United States)

    Hallis, L. J.; Huss, G. R.; Nagashima, K.; Taylor, G. J.; Stöffler, D.; Smith, C. L.; Lee, M. R.

    2017-03-01

    The Tissint meteorite, a picritic shergottite, fell to Earth in Morocco on the 18th of July 2011, and is only the fifth Martian meteorite witnessed to fall. Hydrogen isotope ratios and water contents are variable within different minerals in Tissint. Ringwoodite and shock melt pockets contain elevated D/H ratios relative to terrestrial values (δD = 761-4224‰). These high ratios in recrystallized phases indicate significant implantation of hydrogen from the D-rich Martian atmosphere during shock. In contrast, although olivine has detectable water abundances (230-485 ppm), it exhibits much lower D/H ratios (δD = +88 to -150‰), suggesting this water was not implanted from the Martian atmosphere. The minimal terrestrial weathering experienced by Tissint gives confidence that the olivine-hosted water has a Martian origin, but its high concentration indicates direct inheritance from the parental melt is improbable, especially given the low pressure of olivine crystallisation. Incorporation of a low δD crustal fluid, or deuteric alteration during crystallisation, could explain the relatively high water contents and low D/H ratios in Tissint olivine.

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

    Science.gov (United States)

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

    2012-06-01

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

  14. Comparative feeding ecology of abyssal and hadal fishes through stomach content and amino acid isotope analysis

    Science.gov (United States)

    Gerringer, M. E.; Popp, B. N.; Linley, T. D.; Jamieson, A. J.; Drazen, J. C.

    2017-03-01

    The snailfishes, family Liparidae (Scorpaeniformes), have found notable success in the hadal zone from 6000-8200 m, comprising the dominant ichthyofauna in at least five trenches worldwide. Little is known about the biology of these deepest-living fishes, nor the factors that drive their success at hadal depths. Using recent collections from the Mariana Trench, Kermadec Trench, and neighboring abyssal plains, this study investigates the potential role of trophic ecology in structuring fish communities at the abyssal-hadal boundary. Stomach contents were analyzed from two species of hadal snailfishes, Notoliparis kermadecensis and a newly-discovered species from the Mariana Trench. Amphipods comprised the majority (Kermadec: 95.2%, Mariana: 97.4% index of relative importance) of stomach contents in both species. Decapod crustaceans, polychaetes (N. kermadecensis only), and remains of carrion (squid and fish) were minor dietary components. Diet analyses of abyssal species (families Macrouridae, Ophidiidae, Zoarcidae) collected from near the trenches and the literature are compared to those of the hadal liparids. Stomachs from abyssal fishes also contained amphipods, however macrourids had a higher trophic plasticity with a greater diversity of prey items, including larger proportions of carrion and fish remains; supporting previous findings. Suction-feeding predatory fishes like hadal liparids may find an advantage to descending into the trench - where amphipods are abundant. More generalist feeders and scavengers relying on carrion, such as macrourids, might not benefit from this nutritional advantage at hadal depths. Compound specific isotope analysis of amino acids was used to estimate trophic level of these species (5.3±0.2 Coryphaenoides armatus, 5.2±0.2 C. yaquinae, 4.6±0.2 Spectrunculus grandis, 4.2±0.2 N. kermadecensis, 4.4±0.2 Mariana snailfish). Source amino acid δ15N values were especially high in hadal liparids (8.0±0.3‰ Kermadec, 6.7±0.2

  15. Optimization of {sup 18}O measurement using NRA for studies of isotopic content in fossil meteorites

    Energy Technology Data Exchange (ETDEWEB)

    Borysiuk, M., E-mail: maciek.borysiuk@pixe.lth.se [Division of Nuclear Physics, Department of Physics, Lund University, Box 118, SE-221 00 Lund (Sweden); Kristiansson, P.; Arteaga-Marrero, N.; Elfman, M.; Golubev, P.; Nilsson, E.J.C.; Nilsson, C.; Pallon, J.; Salim, N. [Division of Nuclear Physics, Department of Physics, Lund University, Box 118, SE-221 00 Lund (Sweden)

    2011-10-15

    In this work, we discuss the possibility of a new approach to measuring oxygen isotope ratios in fossil meteorite samples, specifically one based on nuclear reaction analysis (NRA). Variations of oxygen ratios within meteoritic chromite grains can help to determine the type of meteorite to which the grains originally belonged. In this work, we have evaluated the possibility to use the reaction {sup 18}O(p, {alpha}){sup 15}N just above the 846 keV resonance to estimate the relative oxygen-18 content in a number of test samples. Another technique has to be employed for oxygen-16 measurements. A large area segmented silicon detector is used to detect the produced {alpha} particles. Results of the experimental {sup 18}O measurements for a number of samples including four extraterrestrial chromite grains are presented and compared with SIMNRA simulations. The advantage of a segmented silicon detector in the form of inherent pile-up suppression can be clearly seen in the current work.

  16. Actinides record, power calculations and activity for present isotopes in the spent fuel of a BWR; Historial de actinidos y calculos de potencia y actividad para isotopos presentes en el combustible gastado de un BWR

    Energy Technology Data Exchange (ETDEWEB)

    Enriquez C, P.; Ramirez S, J. R.; Lucatero, M. A., E-mail: pastor.enriquez@inin.gob.mx [ININ, Carretera Mexico-Toluca s/n, 52750 Ocoyoacac, Estado de Mexico (Mexico)

    2012-10-15

    The administration of spent fuel is one of the more important stages of the nuclear fuel cycle, and this has become a problem of supreme importance in countries that possess nuclear reactors. Due to this in this work, the study on the actinides record and present fission products to the discharge of the irradiated fuel in a light water reactor type BWR is shown, to quantify the power and activity that emit to the discharge and during the cooling time. The analysis was realized on a fuel assembly type 10 x 10 with an enrichment average of 3.69 wt % in U-235 and the assembly simulation assumes four cycles of operation of 18 months each one and presents an exposition of 47 G Wd/Tm to the discharge. The module OrigenArp of the Scale 6 code is the computation tool used for the assembly simulation and to obtain the results on the actinides record presents to the fuel discharge. The study covers the following points: a) Obtaining of the plutonium vector used in the fuel production of mixed oxides, and b) Power calculation and activity for present actinides to the discharge. The results presented in this work, correspond at the same time immediate of discharge (0 years) and to a cooling stage in the irradiated fuel pool (5 years). (Author)

  17. Actinide management with commercial fast reactors

    Science.gov (United States)

    Ohki, Shigeo

    2015-12-01

    The capability of plutonium-breeding and minor-actinide (MA) transmutation in the Japanese commercial sodium-cooled fast reactor offers one of practical solutions for obtaining sustainable energy resources as well as reducing radioactive toxicity and inventory. The reference core design meets the requirement of flexible breeding ratio from 1.03 to 1.2. The MA transmutation amount has been evaluated as 50-100 kg/GWey if the MA content in fresh fuel is 3-5 wt%, where about 30-40% of initial MA can be transmuted in the discharged fuel.

  18. Actinide management with commercial fast reactors

    Energy Technology Data Exchange (ETDEWEB)

    Ohki, Shigeo [Japan Atomic Energy Agency, 4002, Narita-cho, O-arai-machi, Higashi-Ibaraki-gun, Ibaraki 311-1393 (Japan)

    2015-12-31

    The capability of plutonium-breeding and minor-actinide (MA) transmutation in the Japanese commercial sodium-cooled fast reactor offers one of practical solutions for obtaining sustainable energy resources as well as reducing radioactive toxicity and inventory. The reference core design meets the requirement of flexible breeding ratio from 1.03 to 1.2. The MA transmutation amount has been evaluated as 50-100 kg/GW{sub e}y if the MA content in fresh fuel is 3-5 wt%, where about 30-40% of initial MA can be transmuted in the discharged fuel.

  19. Actinides, accelerators and erosion

    OpenAIRE

    Fifield L. K.; Tims S.G.

    2012-01-01

    Fallout isotopes can be used as artificial tracers of soil erosion and sediment accumulation. The most commonly used isotope to date has been 137Cs. Concentrations of 137Cs are, however, significantly lower in the Southern Hemisphere, and furthermore have now declined to 35% of original values due to radioactive decay. As a consequence the future utility of 137Cs is limited in Australia, with many erosion applications becoming untenable within the next 20 years, and there is a need to replace...

  20. Radionuclide content and state of isotopic disequilibrium in some utilized smoking pastes

    Energy Technology Data Exchange (ETDEWEB)

    Shabana, El-Said Ibrahim; Yahya, Ahmad Abu Bakre [King Abdulaziz Univ., Jeddah (Saudi Arabia). Faculty of Engineering, Radiation Protection and Training Centre; Kinsara, Abdulraheem Abdulrahman [King Abdulaziz Univ., Jeddah (Saudi Arabia). Faculty of Engineering, Nuclear Engineering Dept.

    2014-10-01

    {sup 238}U, {sup 234}U, {sup 226}Ra, {sup 210}Pb and {sup 210}Po were measured in some jurak and mehassel samples collected from the local market. Jurak is a paste mixture composed of 30% tobacco, 50% molasses and 20% spices and minced fruits. Mehassel is a local trade-name of a paste mixture of unknown ratios of tobacco to spices and minced fruits. Both jurak and mehassel are used for smoking by Shisha (a pipe used for smoking and has a water filter). Just for comparison, these radionuclides were measured in some cigarette tobacco samples. In cigarette tobacco samples, the average activity concentrations were 0.32 ± 0.10, 0.51 ± 0.11, 3.6 ± 1.0, 16.1 ± 2.4 and 15.8 ± 2.2 Bq/kg for {sup 238}U, {sup 234}U, {sup 226}Ra, {sup 210}Pb and {sup 210}Po, respectively. These values for the same isotopes were 1.01 ± 0.25, 1.04 ± 0.27, 1.2 ± 0.4, 4.4 ± 1.0 and 4.2 ± 0.9 Bq/kg in jurak samples and 0.17 ± 0.07, 0.24 ± 0.08, 1.8 ± 0.7, 7.5 ± 1.7 and 7.0 ± 1.6 Bq/kg in mehassel samples, respectively. Generally, the mean values of the results indicated that, except for uranium in jurak, the activity concentration for all the analyzed radionuclides in the different samples followed the sequence: {sup 210}Po ∼ {sup 210}Pb > {sup 226}Ra >> {sup 234}U > {sup 238}U, whereas for each radionuclide, its activity concentration followed the sequence: cigarette tobacco > mehassel > jurak. Molasses contributed to the enhanced uranium content in jurak samples. The obtained results are discussed in detail.

  1. Higher peroxidase activity, leaf nutrient contents and carbon isotope composition changes in Arabidopsis thaliana are related to rutin stress.

    Science.gov (United States)

    Hussain, M Iftikhar; Reigosa, Manuel J

    2014-09-15

    Rutin, a plant secondary metabolite that is used in cosmetics and food additive and has known medicinal properties, protects plants from UV-B radiation and diseases. Rutin has been suggested to have potential in weed management, but its mode of action at physiological level is unknown. Here, we report the biochemical, physiological and oxidative response of Arabidopsis thaliana to rutin at micromolar concentrations. It was found that fresh weight; leaf mineral contents (nitrogen, sodium, potassium, copper and aluminum) were decreased following 1 week exposure to rutin. Arabidopsis roots generate significant amounts of reactive oxygen species after rutin treatment, consequently increasing membrane lipid peroxidation, decreasing leaf Ca(2+), Mg(2+), Zn(2+), Fe(2+) contents and losing root viability. Carbon isotope composition in A. thaliana leaves was less negative after rutin application than the control. Carbon isotope discrimination values were decreased following rutin treatment, with the highest reduction compared to the control at 750μM rutin. Rutin also inhibited the ratio of CO2 from leaf to air (ci/ca) at all concentrations. Total protein contents in A. thaliana leaves were decreased following rutin treatment. It was concluded carbon isotope discrimination coincided with protein degradation, increase lipid peroxidation and a decrease in ci/ca values may be the primary action site of rutin. The present results suggest that rutin possesses allelopathic potential and could be used as a candidate to develop environment friendly natural herbicide.

  2. Chemostratigraphies of carbon, oxygen and strontium isotopes and oxygen contents across the Precambrian-Cambrian boundary

    Science.gov (United States)

    Komiya, T.; Sawaki, Y.; Ishikawa, T.

    2007-12-01

    The Precambrian-Cambrian (PC-C) boundary is one of the most important intervals for evolution of life. However, the scarcity of well-preserved outcrops through the boundary makes it ambiguous to decode change of the surface environment and biological evolution. In south China, strata through the PC-C boundary are continuously exposed and contain many fossils, suitable for study of environmental and biological change. In addition, we conducted excavations at four sites of Three Gorge area to obtain continuous and fresh samples. We measured the delta13C, delta18O and 87Sr/86Sr values of the drill core samples and REE compositions of fresh carbonate rocks, respectively. We identified two positive and two negative isotope excursions of delta13Ccarb within this interval: a moderate increase from 0 to +2 permil and a subsequent dramatic drop to -7 permil at the PC-C boundary, and a continuous increase to +5 permil at the upper part of the Nemakit-Daldynian (ND) stage and the subsequent sharp decrease to -9 permil just below the basal Tommotian unconformity, respectively. The continuous pattern of the delta13C shift is irrespective of lithotype and is comparable to fragmented records of other sections within and outside of the Yangtze Platform, indicating that the profile represents global change of seawater chemistry. A chemostratigraphy of 87Sr/86Sr ratios of the drilled samples also displays a smooth curve and its large positive anomaly just below the PC-C boundary. The estimate of oxygen content of seawater from REE composition of carbonate minerals shows significant decreases around PC-C and ND-Tommotian boundaries, respectively. The combination of chemostratigraphies of delta13C, 87Sr/86Sr and pO2 indicates that the 87Sr/86Sr excursions preceded the delta13C negative excursion at PC-C boundary, and suggests that global regression or formation of the Gondwana supercontinent, evident in increase of influx of continental materials, caused biological depression together

  3. Fluoride-conversion synthesis of homogeneous actinide oxide solid solutions

    Energy Technology Data Exchange (ETDEWEB)

    Silva, G W Chinthaka M [ORNL; Hunn, John D [ORNL; Yeamans, Charles B. [University of California, Berkeley; Cerefice, Gary S. [University of Nevada, Las Vegas; Czerwinski, Ken R. [University of Nevada, Las Vegas

    2011-01-01

    Here, a novel route to synthesize (U, Th)O2 solid solutions at a relatively low temperature of 1100 C is demonstrated. First, the separate actinide oxides reacted with ammonium bifluoride to form ammonium actinide fluorides at room temperature. Subsequently, this mixture was converted to the actinide oxide solid solution using a two-phased heat treatment, first at 610 C in static air, then at 1100 C in flowing argon. Solid solutions obeying Vegard s Law were synthesized for ThO2 content from 10 to 90 wt%. Microscopy showed that the (U, Th)O2 solid solutions synthesized with this method to have considerably high crystallinity and homogeneity, suggesting the suitability of material thus synthesized for sintering into nuclear fuel pellets at low temperatures.

  4. Oxygen and hydrogen stable isotope content in daily-collected precipitation samples at Dome C, East Antarctica

    Science.gov (United States)

    Dreossi, Giuliano; Stenni, Barbara; Del Guasta, Massimo; Bonazza, Mattia; Grigioni, Paolo; Karlicek, Daniele; Mognato, Riccardo; Scarchilli, Claudio; Turchetti, Filippo; Zannoni, Daniele

    2016-04-01

    Antarctic ice cores allow to obtain exceptional past climate records, thanks to their water stable isotope content, which provides integrated tracers of the atmospheric water cycle and local climate. Low accumulation sites of the East Antarctic plateau provide the oldest ice core records, with the record-breaking EPICA Dome C drilling covering the last eight climate cycles. However, the isotope-temperature relationship, commonly used to derive the temperature, may be characterized by significant geographical and temporal variations. Moreover, post-depositional effects may further complicate the climate interpretation. A continuous series of precipitation data is needed in order to gain a better understanding of the factors affecting the water stable isotopes in Antarctic precipitation at a specific site. In this study, we use the first and so-far only multi-year series of daily precipitation sampling and isotope measurements from the French-Italian Concordia Station, located at Dome C in East Antarctica (75°06'S 123°21'E; elevation: 3233 m a.s.l.; mean annual temperature: -54.5°C; snow accumulation rate: 25 kg m-2 yr-1), where the oldest deep Antarctic ice core has been retrieved. Surface air temperature data have been provided by the US automatic weather station (AWS), placed 1.5 km away from the base, while tropospheric temperature profiles are obtained by means of a radiosonde, launched once per day by the IPEV/Italian Antarctic Meteo-climatological Observatory. The new dataset also enables us for the first time to study the isotope-temperature relationship distinguishing between different types of precipitation, namely diamond dust, hoar frost and snowfall, identified by the observations carried out by the winter-over personnel collecting the snow samples. Here we present the complete data series of water stable isotopes in precipitation at Dome C spanning the time period from 2008 to 2014, in the framework of the PNRA PRE-REC project.

  5. Actinides, accelerators and erosion

    Science.gov (United States)

    Tims, S. G.; Fifield, L. K.

    2012-10-01

    Fallout isotopes can be used as artificial tracers of soil erosion and sediment accumulation. The most commonly used isotope to date has been 137Cs. Concentrations of 137Cs are, however, significantly lower in the Southern Hemisphere, and furthermore have now declined to 35% of original values due to radioactive decay. As a consequence the future utility of 137Cs is limited in Australia, with many erosion applications becoming untenable within the next 20 years, and there is a need to replace it with another tracer. Plutonium could fill this role, and has the advantages that there were six times as many atoms of Pu as of 137Cs in fallout, and any loss to decay has been negligible due to the long half-lives of the plutonium isotopes. Uranium-236 is another long-lived fallout isotope with significant potential for exploitation as a tracer of soil and sediment movement. Uranium is expected to be more mobile in soils than plutonium (or caesium), and hence the 236U/Pu ratio will vary with soil depth, and so could provide an independent measure of the amount of soil loss. In this paper we discuss accelerator based ultra-sensitive measurements of plutonium and 236U isotopes and their advantages over 137Cs as tracers of soil erosion and sediment movement.

  6. Actinides, accelerators and erosion

    Directory of Open Access Journals (Sweden)

    Fifield L.K.

    2012-10-01

    Full Text Available Fallout isotopes can be used as artificial tracers of soil erosion and sediment accumulation. The most commonly used isotope to date has been 137Cs. Concentrations of 137Cs are, however, significantly lower in the Southern Hemisphere, and furthermore have now declined to 35% of original values due to radioactive decay. As a consequence the future utility of 137Cs is limited in Australia, with many erosion applications becoming untenable within the next 20 years, and there is a need to replace it with another tracer. Plutonium could fill this role, and has the advantages that there were six times as many atoms of Pu as of 137Cs in fallout, and any loss to decay has been negligible due to the long half-lives of the plutonium isotopes. Uranium-236 is another long-lived fallout isotope with significant potential for exploitation as a tracer of soil and sediment movement. Uranium is expected to be more mobile in soils than plutonium (or caesium, and hence the 236U/Pu ratio will vary with soil depth, and so could provide an independent measure of the amount of soil loss. In this paper we discuss accelerator based ultra-sensitive measurements of plutonium and 236U isotopes and their advantages over 137Cs as tracers of soil erosion and sediment movement.

  7. Nuclear data uncertainty analysis on a minor actinide burner for transmuting spent fuel

    Energy Technology Data Exchange (ETDEWEB)

    Choi, Hangbok

    1998-08-01

    A comprehensive sensitivity and uncertainty analysis was performed on a 1200 MWt minor actinides burner designed for a low burnup reactivity swing, negative doppler coefficient, and low sodium void worth. Sensitivities of the performance parameters were generated using depletion perturbation methods for the constrained close fuel cycle of the reactor. The uncertainty analysis was performed using the sensitivity and covariance data taken from ENDF-B/V and other published sources. The uncertainty analysis of a liquid metal reactor for burning minor actinide has shown that uncertainties in the nuclear data of several key minor actinide isotopes can introduce large uncertainties in the predicted performance of the core. The relative uncertainties in the burnup swing, doppler coefficient, and void worth were conservatively estimated to be 180 %, 97 %, and 46 %, respectively. An analysis was performed to prioritize the minor actinide reactions for reducing the uncertainties. (author). 41 refs., 17 tabs., 1 fig.

  8. Winter diets of immature green turtles (Chelonia mydas) on a northern feeding ground: integrating stomach contents and stable isotope analyses

    Science.gov (United States)

    Williams, Natalie C.; Bjorndal, Karen A.; Lamont, Margaret M.; Carthy, Raymond R.

    2015-01-01

    The foraging ecology and diet of the green turtle, Chelonia mydas, remain understudied, particularly in peripheral areas of its distribution. We assessed the diet of an aggregation of juvenile green turtles at the northern edge of its range during winter months using two approaches. Stomach content analyses provide a single time sample, and stable isotope analyses integrate diet over a several-month period. We evaluated diet consistency in prey choice over time by comparing the results of these two approaches. We examined stomach contents from 43 juvenile green turtles that died during cold stunning events in St. Joseph Bay, Florida, in 2008 and 2011. Stomach contents were evaluated for volume, dry mass, percent frequency of occurrence, and index of relative importance of individual diet items. Juvenile green turtles were omnivorous, feeding primarily on seagrasses and tunicates. Diet characterizations from stomach contents differed from those based on stable isotope analyses, indicating the turtles are not feeding consistently during winter months. Evaluation of diets during warm months is needed.

  9. 33rd Actinide Separations Conference

    Energy Technology Data Exchange (ETDEWEB)

    McDonald, L M; Wilk, P A

    2009-05-04

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

  10. Stable isotope compositions and water contents of boninite series volcanic rocks from Chichi-jima, Bonin Islands, Japan

    Science.gov (United States)

    Dobson, P.F.; O'Neil, J.R.

    1987-01-01

    Measurements of stable isotope compositions and water contents of boninite series volcanic rocks from the island of Chichi-jima, Bonin Islands, Japan, confirm that a large amount (1.6-2.4 wt.%) of primary water was present in these unusual magmas. An enrichment of 0.6??? in 18O during differentiation is explained by crystallization of 18O-depleted mafic phases. Silicic glasses have elevated ??18O values and relatively low ??D values indicating that they were modified by low-temperature alteration and hydration processes. Mafic glasses, on the other hand, have for the most part retained their primary isotopic signatures since Eocene time. Primary ??D values of -53 for boninite glasses are higher than those of MORB and suggest that the water was derived from subducted oceanic lithosphere. ?? 1987.

  11. Calculation of cohesive energy of actinide metals

    Institute of Scientific and Technical Information of China (English)

    钱存富; 陈秀芳; 余瑞璜; 耿平; 段占强

    1997-01-01

    According to empirical electron theory of solids and molecules (EET), an equation for calculating the cohesive energy of actinide metals is given, the cohesive energy of 9 actinide metals with known crystal structure is calculated, which is identical with the experimental values on the whole, and the cohesive energy of 6 actinide metals with unknown crystal structure is forecast.

  12. Study of the behavior of actinides continuously recycled in a hard spectrum reactor

    Energy Technology Data Exchange (ETDEWEB)

    Schofield, P.E.

    1980-12-01

    The behavior of actinides continuously recycled through the central region of an EBR-II type reactor was studied. Such a reactor would convert long-lived nuclear wastes to short-lived isotopes, and simultaneously produce useful power. This process is proposed as an alternative to the geological isolation of long-lived actinide wastes. A driver region of 50% U-235 enriched fuel provided a nearly-constant spectrum and flux that was extremely hard compared to standard LMFBRs. This resulted in a high fission-to-capture ratio for most isotopes. The original actinide fuel was the discharge from a LWR, cooled for two years, with 99.9% of the uranium and plutonium removed by chemical processing. Comparison was made between removal of both Pu and U and removal of only U in subsequent cycles. The latter case resulted in substantial quantities of trans-plutonics burned per cycle.

  13. Recovery of minor actinides from irradiated superfact fuels

    Energy Technology Data Exchange (ETDEWEB)

    Apoltolidis, C.; Glatz, J.P.; Molinet, R.; Nicholl, A.; Pagliosa, G.; Romer, K.; Bokelund, H.; Koch, L. [European Commission, JRC, Institute fuer Transuranium Elements, Karlsruhe (Germany)

    1995-12-31

    It could be demonstrated that the reprocessing of fast reactor oxide fuels containing up to 45 % MA (Np and Am), irradiated in the PHENIX reactor in the frame of a transmutation study, is possible. The fuels were dissolved under PUREX type conditions in order to determine their behaviour in the head-end step of the reprocessing process. For one of the fuels containing 20 % Am and 20 % Np before irradiation, an almost complete partitioning of actinides from the dissolver solution could be achieved. Chromatographic extraction was used for the separation of the main bulk elements U, Pu and Np, whereas centrifugal extractors were used to separate the minor actinides from the remaining high level liquid wastes (HLLW). For the relevant radio-toxic isotopes a high recovery rate from the irradiation targets was reached. Those elements are thus available for new fuel fabrication. (authors) 12 refs.

  14. Actinide-specific sequestering agents and decontamination applications

    Energy Technology Data Exchange (ETDEWEB)

    Smith, William L. [Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Materials and Molecular Research Division; Univ. of California, Berkeley, CA (United States). Dept. of Chemistry; Raymond, Kenneth N. [Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Materials and Molecular Research Division; Univ. of California, Berkeley, CA (United States). Dept. of Chemistry

    1981-04-07

    With the commercial development of nuclear reactors, the actinides have become very important industrial elements. A major concern of the nuclear industry is the biological hazard associated with nuclear fuels and their wastes. The acute chemical toxicity of tetravalent actinides, as exemplified by Th(IV), is similar to Cr(III) or Al(III). However, the acute toxicity of 239Pu(IV) is similar to strychnine, which is much more toxic than any of the non-radioactive metals such as mercury. Although the more radioactive isotopes of the transuranium elements are more acutely toxic by weight than plutonium, the acute toxicities of 239Pu, 241Am, and 244Cm are nearly identical in radiation dose, ~100 μCi/kg in rodents. Finally and thus, the extreme acute toxicity of 239Pu is attributed to its high specific activity of alpha emission.

  15. Actinides and Life's Origins.

    Science.gov (United States)

    Adam, Zachary

    2007-12-01

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

  16. Sources of variability and comparability between salmonid stomach contents and isotopic analyses: study design lessons and recommendations

    Science.gov (United States)

    Vinson, M.R.; Budy, P.

    2011-01-01

    We compared sources of variability and cost in paired stomach content and stable isotope samples from three salmonid species collected in September 2001–2005 and describe the relative information provided by each method in terms of measuring diet overlap and food web study design. Based on diet analyses, diet overlap among brown trout, rainbow trout, and mountain whitefish was high, and we observed little variation in diets among years. In contrast, for sample sizes n ≥ 25, 95% confidence interval (CI) around mean δ15Ν and δ13C for the three target species did not overlap, and species, year, and fish size effects were significantly different, implying that these species likely consumed similar prey but in different proportions. Stable isotope processing costs were US$12 per sample, while stomach content analysis costs averaged US$25.49 ± $2.91 (95% CI) and ranged from US$1.50 for an empty stomach to US$291.50 for a sample with 2330 items. Precision in both δ15Ν and δ13C and mean diet overlap values based on stomach contents increased considerably up to a sample size of n = 10 and plateaued around n = 25, with little further increase in precision.

  17. Preliminary considerations concerning actinide solubilities

    Energy Technology Data Exchange (ETDEWEB)

    Newton, T.W.; Bayhurst, B.P.; Daniels, W.R.; Erdal, B.R.; Ogard, A.E.

    1980-01-01

    Work at the Los Alamos Scientific Laboratory on the fundamental solution chemistry of the actinides has thus far been confined to preliminary considerations of the problems involved in developing an understanding of the precipitation and dissolution behavior of actinide compounds under environmental conditions. Attempts have been made to calculate solubility as a function of Eh and pH using the appropriate thermodynamic data; results have been presented in terms of contour maps showing lines of constant solubility as a function of Eh and pH. Possible methods of control of the redox potential of rock-groundwater systems by the use of Eh buffers (redox couples) is presented.

  18. Improved Actinide Neutron Capture Cross Sections Using Accelerator Mass Spectrometry

    Science.gov (United States)

    Bauder, W.; Pardo, R. C.; Kondev, F. G.; Kondrashev, S.; Nair, C.; Nusair, O.; Palchan, T.; Scott, R.; Seweryniak, D.; Vondrasek, R.; Collon, P.; Paul, M.; Youinou, G.; Salvatores, M.; Palmotti, G.; Berg, J.; Maddock, T.; Imel, G.

    2014-09-01

    The MANTRA (Measurement of Actinide Neutron TRAnsmutations) project will improve energy-integrated neutron capture cross section data across the actinide region. These data are incorporated into nuclear reactor models and are an important piece in understanding Generation IV reactor designs. We will infer the capture cross sections by measuring isotopic ratios from actinide samples, irradiated in the Advanced Test Reactor at INL, with Accelerator Mass Spectrometry (AMS) at ATLAS (ANL). The superior sensitivity of AMS allows us to extract multiple cross sections from a single sample. In order to analyze the large number of samples needed for MANTRA and to meet the goal of extracting multiple cross sections per sample, we have made a number of modifications to the AMS setup at ATLAS. In particular, we are developing a technique to inject solid material into the ECR with laser ablation. With laser ablation, we can better control material injection and potentially increase efficiency in the ECR, thus creating less contamination in the source and reducing cross talk. I will present work on the laser ablation system and preliminary results from our AMS measurements. The MANTRA (Measurement of Actinide Neutron TRAnsmutations) project will improve energy-integrated neutron capture cross section data across the actinide region. These data are incorporated into nuclear reactor models and are an important piece in understanding Generation IV reactor designs. We will infer the capture cross sections by measuring isotopic ratios from actinide samples, irradiated in the Advanced Test Reactor at INL, with Accelerator Mass Spectrometry (AMS) at ATLAS (ANL). The superior sensitivity of AMS allows us to extract multiple cross sections from a single sample. In order to analyze the large number of samples needed for MANTRA and to meet the goal of extracting multiple cross sections per sample, we have made a number of modifications to the AMS setup at ATLAS. In particular, we are

  19. New cubic structure compounds as actinide host phases

    Energy Technology Data Exchange (ETDEWEB)

    Stefanovsky, S V [SIA Radon, 7th Rostovskii lane 2/14, Moscow 119121 (Russian Federation); Yudintsev, S V; Livshits, T S, E-mail: profstef@mtu-net.ru [Institute of Geology of Ore Deposits, Petrography, Mineralogy and Geochemistry RAS, Staromonetny lane 35, Moscow 119017 (Russian Federation)

    2010-03-15

    Various compounds with fluorite (cubic zirconia) and fluorite-derived (pyrochlore, zirconolite) structures are considered as promising actinide host phases at immobilization of actinide-bearing nuclear wastes. Recently some new cubic compounds - stannate and stannate-zirconate pyrochlores, murataite and related phases, and actinide-bearing garnet structure compounds were proposed as perspective matrices for complex actinide wastes. Zirconate pyrochlore (ideally Gd{sub 2}Zr{sub 2}O{sub 7}) has excellent radiation resistance and high chemical durability but requires high temperatures (at least 1500 deg. C) to be produced by hot-pressing from sol-gel derived precursor. Partial Sn{sup 4+} substitution for Zr{sup 4+} reduces production temperature and the compounds REE{sub 2}ZrSnO{sub 7} may be hot-pressed or cold pressed and sintered at {approx}1400 deg. C. Pyrochlore, A{sub 2}B{sub 2}O{sub 7-x} (two-fold elementary fluorite unit cell), and murataite, A{sub 3}B{sub 6}C{sub 2}O{sub 20-y} (three-fold fluorite unit cell), are end-members of the polysomatic series consisting of the phases whose structures are built from alternating pyrochlore and murataite blocks (nano-sized modules) with seven- (2C/3C/2C), five- (2C/3C), eight- (3C/2C/3C) and three-fold (3C - murataite) fluorite unit cells. Actinide content in this series reduces in the row: 2C (pyrochlore) > 7C > 5C > 8C > 3C (murataite). Due to congruent melting murataite-based ceramics may be produced by melting and the firstly segregated phase at melt crystallization is that with the highest fraction of the pyrochlore modules in its structure. The melts containing up to 10 wt. % AnO{sub 2} (An = Th, U, Np, Pu) or REE/An fraction of HLW form at crystallization zoned grains composed sequentially of the 5C {yields} 8C {yields} 3C phases with the highest actinide concentration in the core and the lowest - in the rim of the grains. Radiation resistance of the 'murataite' is comparable to titanate pyrochlores. One

  20. Adulteration Identification of Commercial Honey with the C-4 Sugar Content of Negative Values by an Elemental Analyzer and Liquid Chromatography Coupled to Isotope Ratio Mass Spectroscopy.

    Science.gov (United States)

    Dong, Hao; Luo, Donghui; Xian, Yanping; Luo, Haiying; Guo, Xindong; Li, Chao; Zhao, Mouming

    2016-04-27

    According to the AOAC 998.12 method, honey is considered to contain significant C-4 sugars with a C-4 sugar content of >7%, which are naturally identified as the adulteration. However, the authenticity of honey with a C-4 sugar content of sugars (sucrose, glucose, and fructose), δ(2)H and δ(18)O values, sucrose content, and reducing sugar content of honey using an elemental analyzer and liquid chromatography coupled to isotope ratio mass spectroscopy, was first developed to demonstrate the authenticity of honey with a C-4 sugar content of sugar content (%) sugar content (%) sugar content (%) sugars as well. A very strong correlation is also observed between δ(13)C honey values and δ(13)C protein values of both honey groups. For the δ(18)O value, the C-4 sugar content (%) sugar content (%) sugar content of sugar content of <0%.

  1. Environmental research on actinide elements

    Energy Technology Data Exchange (ETDEWEB)

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

    1987-08-01

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

  2. Innovative SANEX process for trivalent actinides separation from PUREX raffinate

    Energy Technology Data Exchange (ETDEWEB)

    Sypula, Michal

    2013-07-01

    Recycling of nuclear spent fuel and reduction of its radiotoxicity by separation of long-lived radionuclides would definitely help to close the nuclear fuel cycle ensuring sustainability of the nuclear energy. Partitioning of the main radiotoxicity contributors followed by their conversion into short-lived radioisotopes is known as partitioning and transmutation strategy. To ensure efficient transmutation of the separated elements (minor actinides) the content of lanthanides in the irradiation targets has to be minimised. This objective can be attained by solvent extraction using highly selective ligands that are able to separate these two groups of elements from each other. The objective of this study was to develop a novel process allowing co-separation of minor actinides and lanthanides from a high active acidic feed solution with subsequent actinide recovery using just one cycle, so-called innovative SANEX process. The conditions of each step of the process were optimised to ensure high actinide separation efficiency. Additionally, screening tests of several novel lipophilic and hydrophilic ligands provided by University of Twente were performed. These tests were aiming in better understanding the influence of the extractant structural modifications onto An(III)/Ln(III) selectivity and complexation properties. Optimal conditions for minor actinides separation were found and a flow-sheet of a new innovative SANEX process was proposed. Tests using a single centrifugal contactor confirmed high Eu(III)/Am(III) separation factor of 15 while the lowest SF{sub Ln/Am} obtained was 6,5 (for neodymium). In addition, a new masking agent for zirconium was found as a substitution for oxalic acid. This new masking agent (CDTA) was also able to mask palladium without any negative influence on An(III)/Ln(III). Additional tests showed no influence of CDTA on plutonium present in the feed solution unlike oxalic acid which causes Pu precipitation. Therefore, CDTA was proposed as

  3. Using trace element content and lead isotopic composition to assess sources of PM in Tijuana, Mexico

    Science.gov (United States)

    Salcedo, D.; Castro, T.; Bernal, J. P.; Almanza-Veloz, V.; Zavala, M.; González-Castillo, E.; Saavedra, M. I.; Perez-Arvízu, O.; Díaz-Trujillo, G. C.; Molina, L. T.

    2016-05-01

    PM2.5 samples were collected at two urban sites (Parque Morelos (PQM) and CECyTE (CEC)) in Tijuana during the Cal-Mex campaign from May 24 to June 5, 2010. Concentration of trace elements (Mg, Al, Ti, V, Mn, Fe, Co, Ni, Zn, Cu, Ga, As, Se, Rb, Sr, Mo, Cd, Sn, Sb, Ba, La, Ce, and Pb), and Pb isotopic composition were determined in order to study the sources of PM impacting each site. Other chemical analysis (gravimetric, elemental and organic carbon (EC/OC), and polycyclic aromatic hydrocarbons (PAHs)), were also performed. Finally, back-trajectories were calculated to facilitate the interpretation of the chemical data. Trace elements results show that CEC is a receptor site affected by mixed regional sources: sea salt, mineral, urban, and industrial. On the other hand, PQM seems to be impacted mainly by local sources. In particular, Pb at CEC is of anthropogenic, as well as crustal origin. This conclusion is supported by the lead isotopic composition, whose values are consistent with a combination of lead extracted from US mines, and lead from bedrocks in the Mexican Sierras. Some of the time variability observed can be explained using the back-trajectories.

  4. Behavior of actinides in the Integral Fast Reactor fuel cycle

    Energy Technology Data Exchange (ETDEWEB)

    Courtney, J.C. [Louisiana State Univ., Baton Rouge, LA (United States). Nuclear Science Center; Lineberry, M.J. [Argonne National Lab., Idaho Falls, ID (United States). Technology Development Div.

    1994-06-01

    The Integral Fast Reactor (IFR) under development by Argonne National Laboratory uses metallic fuels instead of ceramics. This allows electrorefining of spent fuels and presents opportunities for recycling minor actinide elements. Four minor actinides ({sup 237}Np, {sup 240}Pu, {sup 241}Am, and {sup 243}Am) determine the waste storage requirements of spent fuel from all types of fission reactors. These nuclides behave the same as uranium and other plutonium isotopes in electrorefining, so they can be recycled back to the reactor without elaborate chemical processing. An experiment has been designed to demonstrate the effectiveness of the high-energy neutron spectra of the IFR in consuming these four nuclides and plutonium. Eighteen sets of seven actinide and five light metal targets have been selected for ten day exposure in the Experimental Breeder Reactor-2 which serves as a prototype of the IFR. Post-irradiation analyses of the exposed targets by gamma, alpha, and mass spectroscopy are used to determine nuclear reaction-rates and neutron spectra. These experimental data increase the authors` confidence in their ability to predict reaction rates in candidate IFR designs using a variety of neutron transport and diffusion programs.

  5. Possibility of fusion power reactor to transmute minor actinides of spent nuclear fuel

    Energy Technology Data Exchange (ETDEWEB)

    Serikov, A. E-mail: serikov@nfi.kiae.ru; Shatalov, G.; Sheludjakov, S.; Shpansky, Yu.; Vasiliev, N

    2002-12-01

    A possibility to use fusion power reactor (FPR) is considered for burning long-life elements of spent nuclear fuel in parallel with energy production. In this study a principal design of FPR blanket was examined for transmutation of long-life minor actinides (Np, Am, Cm). A production of minor actinide isotopes is equal to 20-30 kg/1 GW{sub (e)} year for now operating fission reactors, and their amounts will rise with the expected growth of fission reactor power. These isotopes have long-life time and can be dangerous in big amounts in future. Plutonium isotopes are not included in an assumption that they will be used in fission reactors. The major goals of the study were to determine FPR blanket composition corresponding to fast transmutation rate of actinides and tritium self-supply simultaneously. Tritium breeding ratio (TBR) was obtained at level 1.11 for water cooling and reached up 1.56 in variant with helium-cooled assemblies with Np nitride. It was concluded that rows with actinides from processed waste fuel should be arranged near the plasma first wall. Advantages of helium above water cooling are observed in the twice-increased loading of waste fissionable materials and essential increase of achievable TBR. Burnout of Np, Am, Cm would remain at a level {approx}40-50% after 4 full power years.

  6. NMR studies of actinide dioxides

    Energy Technology Data Exchange (ETDEWEB)

    Tokunaga, Y. [Advanced Science Research Center, Japan Atomic Energy Agency, Tokai, Ibaraki 319-1195 (Japan)], E-mail: tokunaga.yo@jaea.go.jp; Sakai, H.; Fujimoto, T.; Kambe, S.; Walstedt, R.E.; Ikushima, K.; Yasuoka, H. [Advanced Science Research Center, Japan Atomic Energy Agency, Tokai, Ibaraki 319-1195 (Japan); Aoki, D.; Homma, Y. [Institute for Materials Research, Tohoku University, Oarai, Ibaraki 311-1313 (Japan); Haga, Y.; Matsuda, T.D.; Ikeda, S.; Yamamoto, E.; Nakamura, A. [Advanced Science Research Center, Japan Atomic Energy Agency, Tokai, Ibaraki 319-1195 (Japan); Shiokawa, Y. [Institute for Materials Research, Tohoku University, Oarai, Ibaraki 311-1313 (Japan); Nakajima, K.; Arai, Y. [Department of Nuclear Energy System, Japan Atomic Energy Agency, Tokai, Ibaraki 319-1195 (Japan); Onuki, Y. [Advanced Science Research Center, Japan Atomic Energy Agency, Tokai, Ibaraki 319-1195 (Japan); Department of Physics, Osaka University, Toyonaka, Osaka 560-0043 (Japan)

    2007-10-11

    {sup 17}O NMR measurements have been performed on a series of the actinide dioxides, UO{sub 2}, NpO{sub 2} and PuO{sub 2}. Although the {sup 17}O NMR spectra in these materials are similar at higher temperatures, the low-temperature spectra present are significantly different. In UO{sub 2} we have observed a wide spectrum, forming a rectangular shape below T{sub N}=30 K. In NpO{sub 2}, on the other hand, the spectra broaden rather gradually and exhibit a two-peak structure below T{sub 0}=26 K. In PuO{sub 2}, neither spectrum broadening nor splitting has been observed. We show that these NMR spectra clearly indicate the different nature of the low-temperature magnetic ground states in these actinide compounds.

  7. Actinides input to the dose in the irradiated graphite of RBMK-1500 reactor

    Energy Technology Data Exchange (ETDEWEB)

    Plukienė, R., E-mail: rita@ar.fi.lt [Institute of Physics, Center for Physical Sciences and Technology, Savanorių pr. 231, LT-02300 Vilnius (Lithuania); Plukis, A.; Puzas, A.; Gvozdaitė, R.; Barkauskas, V.; Duškesas, G. [Institute of Physics, Center for Physical Sciences and Technology, Savanorių pr. 231, LT-02300 Vilnius (Lithuania); Cizdziel, J.V.; Bussan, D. [University of Mississippi, Department of Chemistry and Biochemistry, 305 Coulter Hall, University, Oxford, MS 38677 (United States); Remeikis, V. [Institute of Physics, Center for Physical Sciences and Technology, Savanorių pr. 231, LT-02300 Vilnius (Lithuania)

    2016-04-15

    Highlights: • Actinides input to the dose in RBMK-1500 reactor graphite was estimated. • SCALE 6.1 and MCNPX models were used to calculate actinides specific activities. • ORIGEN-ARP was used for gamma power, neutron source and effective dose calculation. • Concentrations of Pu, Am and Cm isotopes in the RBMK graphite sample were measured. • {sup 244}Cm was found to be a critical contributor to effective dose of the personnel. - Abstract: The purpose of this work is to indicate the actinides input to the total radiation dose caused by the irradiated graphite of the RBMK-1500 reactor in comparison to the dose delivered by other nuclides. We used computer codes (SCALE 6.1 and MCNPX 2.7) to estimate the dose rate delivered by actinides giving special attention to the {sup 244}Cm isotope as a critical contributor to the total activity of actinides in the spent graphite for approximately up to 200 years. The concentrations of Pu, Am and Cm isotopes in the graphite sample from the Ignalina Nuclear Power Plant (NPP) Unit 1 have been measured with the inductively coupled plasma mass spectrometer and specific isotope ratios have been compared with alpha spectrometric results as well as with the values simulated by the computer codes. Good agreement of the experimental results and the simulated ratios serves as an additional confirmation of validity of the calculation models. The effective doses rates of inhalation and ingestion for personnel, gamma radiation power, and nuclides, which constitute the neutron source in the irradiated RBMK-1500 graphite constructions, have also been identified. The obtained results are important for decommissioning of the Ignalina NPP and other NPPs with graphite-moderated reactors.

  8. Diet of harbor porpoises along the Dutch coast: A combined stable isotope and stomach contents approach

    NARCIS (Netherlands)

    Jansen, O.E.; Michel, L.; Lepoint, G.; Das, K.; Couperus, A.S.; Reijnders, P.J.H.

    2013-01-01

    High stranding frequency of porpoises, Phocoena phocoena, along the Dutch coast since 2006 has led to increased interest in the ecology of porpoises in the North Sea. Stranded porpoises were collected along the Dutch coast (2006–2008) and their diet was assessed through stomach content and stable is

  9. The uncertainty analysis of a liquid metal reactor for burning minor actinides from light water reactors

    Energy Technology Data Exchange (ETDEWEB)

    Choi, Hang Bok [Korea Atomic Energy Research Institute, Taejon (Korea, Republic of)

    1998-12-31

    The neutronics analysis of a liquid metal reactor for burning minor actinides has shown that uncertainties in the nuclear data of several key minor actinide isotopes can introduce large uncertainties in the predicted performance of the core. A comprehensive sensitivity and uncertainty analysis was performed on a 1200 MWth actinide burner designed for a low burnup reactivity swing, negative doppler coefficient, and low sodium void worth. Sensitivities were generated using depletion perturbation methods for the equilibrium cycle of the reactor and covariance data was taken ENDF-B/V and other published sources. The relative uncertainties in the burnup swing, doppler coefficient, and void worth were conservatively estimated to be 180%, 97%, and 46%, respectively. 5 refs., 1 fig., 3 tabs. (Author)

  10. Standard practice for alternate actinide calibration for inductively coupled plasma-mass spectrometry

    CERN Document Server

    American Society for Testing and Materials. Philadelphia

    2004-01-01

    1.1 This practice provides guidance for an alternate linear calibration for the determination of selected actinide isotopes in appropriately prepared aqueous solutions by Inductively Coupled Plasma-Mass Spectrometry (ICP-MS). This alternate calibration is mass bias adjusted using thorium-232 (232Th) and uranium-238 (238U) standards. One of the benefits of this standard practice is the ability to calibrate for the analysis of highly radioactive actinides using calibration standards at much lower specific activities. Environmental laboratories may find this standard practice useful if facilities are not available to handle the highly radioactive standards of the individual actinides of interest. 1.2 The instrument response for a series of determinations of known concentration of 232Th and 238U defines the mass versus response relationship. For each standard concentration, the slope of the line defined by 232Th and 238U is used to derive linear calibration curves for each mass of interest using interference equ...

  11. Elemental partitioning and isotopic fractionation of Zn between metal and silicate and geochemical estimation of the S content of the Earth's core

    CERN Document Server

    Mahan, B; Pringle, E A; Moynier, F

    2016-01-01

    Zinc metal-silicate fractionation provides experimental access to the conditions of core formation and Zn has been used to estimate the S contents of the Earth's core and of the bulk Earth, assuming that they share similar volatility and that Zn was not partitioned into the Earth's core. We have conducted a suite of partitioning experiments to characterize Zn metal-silicate elemental and isotopic fractionation as a function of time, temperature, and composition. Experiments were conducted at temperatures from 1473-2273K, with run durations from 5-240 minutes for four starting materials. Chemical and isotopic equilibrium is achieved within 10 minutes. Zinc metal-silicate isotopic fractionation displays no resolvable dependence on temperature, composition, or oxygen fugacity. Thus, the Zn isotopic composition of silicate phases can be used as a proxy for bulk telluric bodies. Results from this study and literature data were used to parameterize Zn metal-silicate partitioning as a function of temperature, pressu...

  12. The importance of mangroves, mud and sand flats, and seagrass beds as feeding areas for juvenile fishes in Chwaka Bay, Zanzibar : gut content and stable isotope analyses

    NARCIS (Netherlands)

    Lugendo, B.; Nagelkerken, I.; Velde, G. van der; Mgaya, Y.D.

    2006-01-01

    The relative importance of bay habitats, consisting of mangrove creeks and channel, seagrass beds, and mud and sand flats, as feeding grounds for a number of fish species was studied in Chwaka Bay, Zanzibar, Tanzania, using gut content analysis and stable isotope analysis of carbon and nitrogen. Gut

  13. Prompt fission neutron spectrum of actinides

    Energy Technology Data Exchange (ETDEWEB)

    Capote, R. [International Atomic Energy Agency, Vienna (Austria); Chen, Y. -J. [China Institute of Atomic Energy, Beijing (China); Hambsch, F. J. [European Commission, Joint Research Centre - IRRM, Geel (Belgium); Jurado, B. [CENBG, CNRS/IN2P3, Gradignan (France); Kornilov, N. [Ohio Univ., Athens, OH (United States); Lestone, J. P. [Los Alamos National Lab. (LANL), Los Alamos, NM (United States); Litaize, O. [CEA, DEN, DER, SPRC, Saint-Paul-Lez-Durance (France); Morillon, B. [CEA, DAM, DIF, Arpajon (France); Neudecker, D. [Los Alamos National Lab. (LANL), Los Alamos, NM (United States); Oberstedt, S. [European Commission, Joint Research Centre - IRRM, Geel (Belgium); Ohsawa, T. [Kinki Univ., Osaka-fu (Japan); Otuka, N. [International Atomic Energy Agency, Vienna (Austria); Pronyaev, V. G. [Institute of Physics and Power Engineering, Obninsk (Russian Federation); Saxena, A. [Bhabha Atomic Research Centre, Mumbai (India); Schmidt, K. H. [CENBG, CNRS/IN2P3, Gradignan (France); Serot, O. [CEA, DEN, DER, SPRC, Saint-Paul-Lez-Durance (France); Shcherbakov, O. A. [Petersburg Nuclear Physics Institute of NRC " Kurchatov Institute" , Gatchina (Russian Federation); Shu, N. -C. [China Institute of Atomic Energy, Beijing (China); Smith, D. L. [Argonne National Lab. (ANL), Argonne, IL (United States); Talou, P. [Los Alamos National Lab. (LANL), Los Alamos, NM (United States); Trkov, A. [International Atomic Energy Agency, Vienna (Austria); Tudora, A. C. [Univ. of Bucharest, Magurele (Romania); Vogt, R. [Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States); Univ. of California, Davis, CA (United States); Vorobyev, A. S. [Petersburg Nuclear Physics Institute of NRC " Kurchatov Institute" , Gatchina (Russian Federation)

    2016-01-06

    Here, the energy spectrum of prompt neutron emitted in fission (PFNS) plays a very important role in nuclear science and technology. A Coordinated Research Project (CRP) "Evaluation of Prompt Fission Neutron Spectra of Actinides" was established by the IAEA Nuclear Data Section in 2009, with the major goal to produce new PFNS evaluations with uncertainties for actinide nuclei.

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

    Directory of Open Access Journals (Sweden)

    Oettingen Mikołaj

    2015-09-01

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

  15. Actinide ion sensor for pyroprocess monitoring

    Science.gov (United States)

    Jue, Jan-fong; Li, Shelly X.

    2014-06-03

    An apparatus for real-time, in-situ monitoring of actinide ion concentrations which comprises a working electrode, a reference electrode, a container, a working electrolyte, a separator, a reference electrolyte, and a voltmeter. The container holds the working electrolyte. The voltmeter is electrically connected to the working electrode and the reference electrode and measures the voltage between those electrodes. The working electrode contacts the working electrolyte. The working electrolyte comprises an actinide ion of interest. The reference electrode contacts the reference electrolyte. The reference electrolyte is separated from the working electrolyte by the separator. The separator contacts both the working electrolyte and the reference electrolyte. The separator is ionically conductive to the actinide ion of interest. The reference electrolyte comprises a known concentration of the actinide ion of interest. The separator comprises a beta double prime alumina exchanged with the actinide ion of interest.

  16. Catalytic Organic Transformations Mediated by Actinide Complexes

    Directory of Open Access Journals (Sweden)

    Isabell S. R. Karmel

    2015-10-01

    Full Text Available This review article presents the development of organoactinides and actinide coordination complexes as catalysts for homogeneous organic transformations. This chapter introduces the basic principles of actinide catalysis and deals with the historic development of actinide complexes in catalytic processes. The application of organoactinides in homogeneous catalysis is exemplified in the hydroelementation reactions, such as the hydroamination, hydrosilylation, hydroalkoxylation and hydrothiolation of alkynes. Additionally, the use of actinide coordination complexes for the catalytic polymerization of α-olefins and the ring opening polymerization of cyclic esters is presented. The last part of this review article highlights novel catalytic transformations mediated by actinide compounds and gives an outlook to the further potential of this field.

  17. Fission fragment angular distributions in pre-actinide nuclei

    Science.gov (United States)

    Banerjee, Tathagata; Nath, S.; Jhingan, A.; Kaur, Gurpreet; Dubey, R.; Yadav, Abhishek; Laveen, P. V.; Shamlath, A.; Shareef, M.; Gehlot, J.; Saneesh, N.; Prasad, E.; Sugathan, P.; Pal, Santanu

    2016-10-01

    Background: Complete fusion of two nuclei leading to formation of a heavy compound nucleus (CN) is known to be hindered by various fission-like processes, in which the composite system reseparates after capture of the target and the projectile inside the potential barrier. As a consequence of these non-CN fission (NCNF) processes, fusion probability (PCN) starts deviating from unity. Despite substantial progress in understanding, the onset and the experimental signatures of NCNF and the degree of its influence on fusion have not yet been unambiguously identified. Purpose: This work aims to investigate the presence of NCNF, if any, in pre-actinide nuclei by systematic study of fission angular anisotropies and fission cross sections (σfis) in a number of nuclear reactions carried out at and above the Coulomb barrier (VB) . Method: Fission fragment angular distributions were measured for six 28Si-induced reactions involving isotopically enriched targets of 169Tm,176Yb,175Lu,180Hf,181Ta, and 182W leading to probable formation of CN in the pre-actinide region, at a laboratory energy (Elab) range of 129-146 MeV. Measurements were performed with large angular coverage (θlab=41∘ -170∘) in which fission fragments (FFs) were detected by nine hybrid telescope (E -Δ E ) detectors. Extracted fission angular anisotropies and σfis were compared with statistical model (SM) predictions. Results: Barring two reactions involving targets with large non-zero ground state spin (J ) , viz., 175Lu(7/2+) and 181Ta(7/2+) , experimental fission angular anisotropies were found to be higher in comparison with predictions of the statistical saddle point model (SSPM), at Ec .m . near VB. Comparison of present results with those from neighboring systems revealed that experimental anisotropies increasingly deviated from SSPM predictions as one moved from pre-actinide to actinide nuclei. For reactions involving targets with large nonzero J , this deviation was subdued. Comparison between

  18. Actinides: How well do we know their stellar production?

    Science.gov (United States)

    Goriely, S.; Arnould, M.

    2001-12-01

    actinide content of meteorites. Both sets of constraints suffer from serious problems. The first set does not hold in the likely situation of the non-universality of the r-process. The definition of the second set is made difficult by the necessity of using intricate galactic evolution models in order to interpret the meteoritic data. Our calculations of the actinide production combined with future data on the galactic cosmic ray actinide composition should help confirming that galactic cosmic rays are not fresh supernova ejecta. They should also provide a tool to discriminate between two competing models for the cosmic ray acceleration, one calling for an isolated supernova exploding in the ordinary old interstellar medium, and one envisioning a superbubble instead.

  19. Isotopic composition of H2 from wood burning: Dependency on combustion efficiency, moisture content, and δD of local precipitation

    Science.gov (United States)

    RöCkmann, Thomas; Gómez ÁLvarez, Catalina X.; Walter, Sylvia; van der Veen, Carina; Wollny, Adam G.; Gunthe, Sachin S.; Helas, Günther; PöSchl, Ulrich; Keppler, Frank; Greule, Markus; Brand, Willi A.

    2010-09-01

    Differences in isotopic composition between the various sources of H2 are large, but only a few measurements have been carried out to constrain them. Two conflicting values have been published for H2 from biomass burning. Both rely on the assumption that the isotopic composition of H2 should scale with the isotopic composition of the precipitation at the location where the biomass grew. Here we test this hypothesis using 18 wood samples collected from various locations around the globe. The sample locations cover a range of δD content of H2 in precipitation, from below -120‰ in Siberia and Canada to -15‰ in Zimbabwe. The results confirm the predicted dependence of the H2 isotopic composition on the precipitation in the sampling region. The water content itself is found to at most slightly affect the results. Furthermore, δD of H2 depends strongly on combustion efficiency. Thus, the isotopic composition of H2 from biomass burning shows a strong variability around the globe and between different stages of a fire. It is suggested that, rather than a global bulk number, global models that attempt to reproduce the spatial and temporal distribution of δD in H2 should incorporate explicitly the variability of δD(H2) from biomass burning on δD in precipitation.

  20. Effect of different fertilizers on nitrogen isotope composition and nitrate content of Brassica campestris.

    Science.gov (United States)

    Yuan, Yuwei; Zhao, Ming; Zhang, Zhiheng; Chen, Tianjin; Yang, Guiling; Wang, Qiang

    2012-02-15

    The effect of different fertilizers on the δ(15)N value, nitrate concentration, and nitrate reductase activity of Brassica campestris and the δ(15)N value of soil has been investigated through a pot experiment. The δ(15)N mean value of B. campestris at the seedling stage observed in the composted chicken treatment (+8.65‰) was higher than that of chemical fertilizer treatment (+5.73‰), compost-chemical fertilizer (+7.53‰), and control check treatment (+7.86‰). There were significantly different δ(15)N values (p fertilizer treatment. The similar results were also found at the middle stage and the terminal stage. The variation of δ(15)N value in soil for different treatments was smaller than that of B. campestris, which was +6.71-+8.12‰, +6.83-+8.24‰, and +6.85-8.4‰, respectively, at seedling stage, middle stage, and terminal stage. With the growth of B. campestris, the nitrate content decreased in all treatments, and the nitrate reductase activity in B. campestris increased except for the CK. Results suggested that the δ(15)N values of B. campestris and soil were more effected by the fertilizer than by the dose level, and the δ(15)N value analysis could be used as a tool to discriminate the B. campestris cultivated with composted manure or chemical fertilizer.

  1. Ionic Interactions in Actinide Tetrahalides

    Science.gov (United States)

    Akdeniz, Z.; Karaman, A.; Tosi, M. P.

    2001-05-01

    We determine a model of the ionic interactions in AX 4 compounds (where A is an atom in the actinide series from Th to Am and X = F, Cl, Br or I) by an analysis of data on the static and dynamic structure of their molecular monomers. The potential energy function that we adopt is taken from earlier work on rare-earth trihalides [Z. Akdeniz, Z. Q q e k and M. P. Tosi, Z. Naturforsch. 55a, 861 (2000)] and in particular allows for the electronic polarizability of the actinide ion. This polarizability quantitatively determines the antisymmetric-bending vibrational mode, but its magnitude remains compatible with a symmetric tetrahedral shape of the molecule at equilibrium. The fluorides have an especially high degree of ionic character, and the interionic-force parameters for each halide of the U, Np, Pu and Am series show regular trends, suggesting that extrapolations to the other transuranic-element halides may usefully be made. The Th compounds show some deviations from these trends, and the interionic-force model that we determine for ThCl4 differs somewhat from that obtained in a previous study. We therefore return on the evaluation of the relative stability of charged oligomers of ThCl4 and ZrCl4 and find confirmation of our earlier results on this problem.

  2. The ALMR actinide burning system

    Energy Technology Data Exchange (ETDEWEB)

    Quinn, J.E. (General Electric Co., San Jose, CA (United States))

    1993-01-01

    The advanced liquid-metal reactor (ALMR) actinide burning system is being developed under the sponsorship of the US Department of Energy to bring its unique capabilities to fruition for deployment in the early 21st century. The system consists of four major parts: the reactor plant, the metal fuel and its recycle, the processing of light water reactor (LWR) spent fuel to extract the actinides, and the development of a residual waste package. This paper addresses the status and outlook for each of these four major elements. The ALMR is being developed by an industrial group under the leadership of General Electric (GE) in a cost-sharing arrangement with the US Department of Energy. This effort is nearing completion of the advanced conceptual design phase and will enter the preliminary design phase in 1994. The innovative modular reactor design stresses simplicity, economics, reliability, and availability. The design has evolved from GE's PRISM design initiative and has progressed to the final stages of a prelicensing review by the US Nuclear Regulatory Commission (NRC); a safety evaluation report is expected by the end of 1993. All the major issues identified during this review process have been technically resolved. The next design phases will focus on implementation of the basic safety philosophy of passive shutdown to a safe, stable condition, even without scram, and passive decay heat removal. Economic projections to date show that it will be competitive with non- nuclear and advanced LWR nuclear alternatives.

  3. Variations of Microbial Communities and the Contents and Isotopic Compositions of Total Organic Carbon and Total Nitrogen in Soil Samples during Their Preservation

    Institute of Scientific and Technical Information of China (English)

    TAO Qianye; LI Yumei; WANG Guo'an; QIAO Yuhui; LIU Tung-Sheng

    2009-01-01

    Semi-sealed preservation of soil samples at difierent moisture of 4%and 23%,respectively, was simulated to observe the variations of soil microbiaI communities and determine the contents and isotopic compositions of the total organic carbon and total nitrogen on the 7th and 30th day, respectively.The results show that during preservation,the quantity of microbial communities tended to increase first and then decrease,with a wider variation range at higher moisture(23%).At the moisture content of 23%,the microbial communities became more active on the 7th day.but less after 30 days,and their activity Was stable with little fluctuation at the moisture content of 4%.However. there were no significant changes in the contents and isotopic compositions of the total organic carbon and total nitrogen.During preservation.the responses of soil microbes to the environment are more sensitive to changes in the total nitrogen and organic carbon contents.It is thus suggested that the variations of microbial communities have not exerted remarkable impacts on the isotope compositions of the total nitrogen and total organic carbon.

  4. Content of the Alternaria mycotoxin tenuazonic acid in food commodities determined by a stable isotope dilution assay.

    Science.gov (United States)

    Asam, Stefan; Lichtenegger, Martina; Liu, Yang; Rychlik, Michael

    2012-02-01

    The Alternaria mycotoxin tenuazonic acid (TA) was quantified in fruit juices (n = 50), cereals (n = 12) and spices (n = 38) using a recently developed stable isotope dilution assay (SIDA). [(13) C6,(15) N]-TA was used as the internal standard. Method validation revealed low limits of detection (LODs) of 0.15 μg/kg (fruit juices), 1.0 μg/kg (cereals) and 17 μg/kg (spices). The respective limits of quantitation were about three times higher. Recovery was about 100% for all matrices. The precision (relative standard deviation of replicate analyses of naturally contaminated samples) was 4.2% (grape juice; 1.7 μg/kg), 3.5% (whole wheat flour; 36 μg/kg) and 0.9% (curry powder; 215 μg/kg). The median content of TA in the analyzed samples was 1.8 μg/kg (fruit juices), 16 μg/kg (cereals) and 500 μg/kg (spices). Positive samples amounted to 86% (fruit juices), 92% (cereals) and 87% (spices).

  5. Experimental studies of actinides in molten salts

    Energy Technology Data Exchange (ETDEWEB)

    Reavis, J.G.

    1985-06-01

    This review stresses techniques used in studies of molten salts containing multigram amounts of actinides exhibiting intense alpha activity but little or no penetrating gamma radiation. The preponderance of studies have used halides because oxygen-containing actinide compounds (other than oxides) are generally unstable at high temperatures. Topics discussed here include special enclosures, materials problems, preparation and purification of actinide elements and compounds, and measurements of various properties of the molten volts. Property measurements discussed are phase relationships, vapor pressure, density, viscosity, absorption spectra, electromotive force, and conductance. 188 refs., 17 figs., 6 tabs.

  6. Spin and orbital moments in actinide compounds

    DEFF Research Database (Denmark)

    Lebech, B.; Wulff, M.; Lander, G.H.

    1991-01-01

    experiments designed to determine the magnetic moments at the actinide and transition-metal sublattice sites in compounds such as UFe2, NpCo2, and PuFe2 and to separate the spin and orbital components at the actinide sites. The results show, indeed, that the ratio of the orbital to spin moment is reduced......The extended spatial distribution of both the transition-metal 3d electrons and the actinide 5f electrons results in a strong interaction between these electron states when the relevant elements are alloyed. A particular interesting feature of this hybridization, which is predicted by single...

  7. Recovery of actinides from actinide-aluminium alloys by chlorination: Part I

    OpenAIRE

    Cassayre, Laurent; Soucek, Pavel; Mendes, Eric; Malmbeck, Rikard; Nourry, Christophe; Eloirdi, Rachel; Glatz, Jean-Paul

    2011-01-01

    Pyrochemical processes in molten LiCl–KCl are being developed in ITU for recovery of actinides from spent nuclear fuel. The fuel is anodically dissolved to the molten salt electrolyte and actinides are electrochemically reduced on solid aluminium cathodes forming solid actinide–aluminium alloys. A chlorination route is being investigated for recovery of actinides from the alloys. This route consists in three steps: Vacuum distillation for removal of the salt adhered on the electrode, chlorina...

  8. Final Report on Actinide Glass Scintillators for Fast Neutron Detection

    Energy Technology Data Exchange (ETDEWEB)

    Bliss, Mary; Stave, Jean A.

    2012-10-01

    This is the final report of an experimental investigation of actinide glass scintillators for fast-neutron detection. It covers work performed during FY2012. This supplements a previous report, PNNL-20854 “Initial Characterization of Thorium-loaded Glasses for Fast Neutron Detection” (October 2011). The work in FY2012 was done with funding remaining from FY2011. As noted in PNNL-20854, the glasses tested prior to July 2011 were erroneously identified as scintillators. The decision was then made to start from “scratch” with a literature survey and some test melts with a non-radioactive glass composition that could later be fabricated with select actinides, most likely thorium. The normal stand-in for thorium in radioactive waste glasses is cerium in the same oxidation state. Since cerium in the 3+ state is used as the light emitter in many scintillating glasses, the next most common substitute was used: hafnium. Three hafnium glasses were melted. Two melts were colored amber and a third was clear. It barely scintillated when exposed to alpha particles. The uses and applications for a scintillating fast neutron detector are important enough that the search for such a material should not be totally abandoned. This current effort focused on actinides that have very high neutron capture energy releases but low neutron capture cross sections. This results in very long counting times and poor signal to noise when working with sealed sources. These materials are best for high flux applications and access to neutron generators or reactors would enable better test scenarios. The total energy of the neutron capture reaction is not the only factor to focus on in isotope selection. Many neutron capture reactions result in energetic gamma rays that require large volumes or high densities to detect. If the scintillator is to separate neutrons from gamma rays, the capture reactions should produce heavy particles and few gamma rays. This would improve the detection of a

  9. Subsurface interactions of actinide species and microorganisms : implications for the bioremediation of actinide-organic mixtures.

    Energy Technology Data Exchange (ETDEWEB)

    Banaszak, J.E.; Reed, D.T.; Rittmann, B.E.

    1999-02-12

    By reviewing how microorganisms interact with actinides in subsurface environments, we assess how bioremediation controls the fate of actinides. Actinides often are co-contaminants with strong organic chelators, chlorinated solvents, and fuel hydrocarbons. Bioremediation can immobilize the actinides, biodegrade the co-contaminants, or both. Actinides at the IV oxidation state are the least soluble, and microorganisms accelerate precipitation by altering the actinide's oxidation state or its speciation. We describe how microorganisms directly oxidize or reduce actinides and how microbiological reactions that biodegrade strong organic chelators, alter the pH, and consume or produce precipitating anions strongly affect actinide speciation and, therefore, mobility. We explain why inhibition caused by chemical or radiolytic toxicities uniquely affects microbial reactions. Due to the complex interactions of the microbiological and chemical phenomena, mathematical modeling is an essential tool for research on and application of bioremediation involving co-contamination with actinides. We describe the development of mathematical models that link microbiological and geochemical reactions. Throughout, we identify the key research needs.

  10. Overview of actinide chemistry in the WIPP

    Energy Technology Data Exchange (ETDEWEB)

    Borkowski, Marian [Los Alamos National Laboratory; Lucchini, Jean - Francois [Los Alamos National Laboratory; Richmann, Michael K [Los Alamos National Laboratory; Reed, Donald T [Los Alamos National Laboratory; Khaing, Hnin [Los Alamos National Laboratory; Swanson, Juliet [Los Alamos National Laboratory

    2009-01-01

    The year 2009 celebrates 10 years of safe operations at the Waste Isolation Pilot Plant (WIPP), the only nuclear waste repository designated to dispose defense-related transuranic (TRU) waste in the United States. Many elements contributed to the success of this one-of-the-kind facility. One of the most important of these is the chemistry of the actinides under WIPP repository conditions. A reliable understanding of the potential release of actinides from the site to the accessible environment is important to the WIPP performance assessment (PA). The environmental chemistry of the major actinides disposed at the WIPP continues to be investigated as part of the ongoing recertification efforts of the WIPP project. This presentation provides an overview of the actinide chemistry for the WIPP repository conditions. The WIPP is a salt-based repository; therefore, the inflow of brine into the repository is minimized, due to the natural tendency of excavated salt to re-seal. Reducing anoxic conditions are expected in WIPP because of microbial activity and metal corrosion processes that consume the oxygen initially present. Should brine be introduced through an intrusion scenario, these same processes will re-establish reducing conditions. In the case of an intrusion scenario involving brine, the solubilization of actinides in brine is considered as a potential source of release to the accessible environment. The following key factors establish the concentrations of dissolved actinides under subsurface conditions: (1) Redox chemistry - The solubility of reduced actinides (III and IV oxidation states) is known to be significantly lower than the oxidized forms (V and/or VI oxidation states). In this context, the reducing conditions in the WIPP and the strong coupling of the chemistry for reduced metals and microbiological processes with actinides are important. (2) Complexation - For the anoxic, reducing and mildly basic brine systems in the WIPP, the most important

  11. BWR Assembly Optimization for Minor Actinide Recycling

    Energy Technology Data Exchange (ETDEWEB)

    G. Ivan Maldonado; John M. Christenson; J.P. Renier; T.F. Marcille; J. Casal

    2010-03-22

    The Primary objective of the proposed project is to apply and extend the latest advancements in LWR fuel management optimization to the design of advanced boiling water reactor (BWR) fuel assemblies specifically for the recycling of minor actinides (MAs).

  12. Advanced Aqueous Separation Systems for Actinide Partitioning

    Energy Technology Data Exchange (ETDEWEB)

    Nash, Kenneth L.; Clark, Sue; Meier, G Patrick; Alexandratos, Spiro; Paine, Robert; Hancock, Robert; Ensor, Dale

    2012-03-21

    One of the most challenging aspects of advanced processing of spent nuclear fuel is the need to isolate transuranium elements from fission product lanthanides. This project expanded the scope of earlier investigations of americium (Am) partitioning from the lanthanides with the synthesis of new separations materials and a centralized focus on radiochemical characterization of the separation systems that could be developed based on these new materials. The primary objective of this program was to explore alternative materials for actinide separations and to link the design of new reagents for actinide separations to characterizations based on actinide chemistry. In the predominant trivalent oxidation state, the chemistry of lanthanides overlaps substantially with that of the trivalent actinides and their mutual separation is quite challenging.

  13. Actinides transmutation - a comparison of results for PWR benchmark

    Energy Technology Data Exchange (ETDEWEB)

    Claro, Luiz H. [Instituto de Estudos Avancados (IEAv/CTA), Sao Jose dos Campos, SP (Brazil)], e-mail: luizhenu@ieav.cta.br

    2009-07-01

    The physical aspects involved in the Partitioning and Transmutation (P and T) of minor actinides (MA) and fission products (FP) generated by reactors PWR are of great interest in the nuclear industry. Besides these the reduction in the storage of radioactive wastes are related with the acceptability of the nuclear electric power. From the several concepts for partitioning and transmutation suggested in literature, one of them involves PWR reactors to burn the fuel containing plutonium and minor actinides reprocessed of UO{sub 2} used in previous stages. In this work are presented the results of the calculations of a benchmark in P and T carried with WIMSD5B program using its new cross sections library generated from the ENDF-B-VII and the comparison with the results published in literature by other calculations. For comparison, was used the benchmark transmutation concept based in a typical PWR cell and the analyzed results were the k{infinity} and the atomic density of the isotopes Np-239, Pu-241, Pu-242 and Am-242m, as function of burnup considering discharge of 50 GWd/tHM. (author)

  14. Multi-nucleon transfer experiments in the actinide region

    Energy Technology Data Exchange (ETDEWEB)

    Geibel, Kerstin; Reiter, Peter; Birkenbach, Benedikt [Institut fuer Kernphysik, Universitaet zu Koeln (Germany); Valiente-Dobon, Jose Javier; Recchia, Francesco [Istituto Nazionale di Fisica Nucleare, Laboratori Nazionali di Legnaro (Italy); Gadea, Andres [IFIC, CSIC-Universidad de Valencia (Spain); Lenzi, Silvia [Dipartimento di Fisica, University of Padova (Italy)

    2012-07-01

    Two experiments at the PRISMA-CLARA-Setup at the LNL in Legnaro were analysed focussing on the target-like reaction products in the actinide region after multi-nucleon transfer reactions. Both experiments use {sup 238}U as target; a {sup 70}Zn-beam with 460 MeV and a {sup 136}Xe-beam with 926 MeV were employed. Kinematic correlations between the reaction partners are used to obtain information about the unobserved target-like reaction products by the analysis of the beam-like particles identified with the PRISMA-spectrometer. Clean {gamma}-spectra from neutron-rich actinide nuclei are obtained with the CLARA-array. An extension of the ground state rotational band in {sup 240}U and insights in neutron-rich Th-isotopes were achieved. Based on relative cross section distributions for various reaction channels the perspectives and limitations for in-beam {gamma}-spectroscopy with this experimental method in this mass region are discussed.

  15. The Actinide Transition Revisited by Gutzwiller Approximation

    Science.gov (United States)

    Xu, Wenhu; Lanata, Nicola; Yao, Yongxin; Kotliar, Gabriel

    2015-03-01

    We revisit the problem of the actinide transition using the Gutzwiller approximation (GA) in combination with the local density approximation (LDA). In particular, we compute the equilibrium volumes of the actinide series and reproduce the abrupt change of density found experimentally near plutonium as a function of the atomic number. We discuss how this behavior relates with the electron correlations in the 5 f states, the lattice structure, and the spin-orbit interaction. Our results are in good agreement with the experiments.

  16. Predictive Modeling in Actinide Chemistry and Catalysis

    Energy Technology Data Exchange (ETDEWEB)

    Yang, Ping [Los Alamos National Lab. (LANL), Los Alamos, NM (United States)

    2016-05-16

    These are slides from a presentation on predictive modeling in actinide chemistry and catalysis. The following topics are covered in these slides: Structures, bonding, and reactivity (bonding can be quantified by optical probes and theory, and electronic structures and reaction mechanisms of actinide complexes); Magnetic resonance properties (transition metal catalysts with multi-nuclear centers, and NMR/EPR parameters); Moving to more complex systems (surface chemistry of nanomaterials, and interactions of ligands with nanoparticles); Path forward and conclusions.

  17. Lattice effects in the light actinides

    Energy Technology Data Exchange (ETDEWEB)

    Lawson, A.C.; Cort, B.; Roberts, J.A.; Bennett, B.I.; Brun, T.O.; Dreele, R.B. von [Los Alamos National Lab., NM (United States); Richardson, J.W. Jr. [Argonne National Lab., IL (United States)

    1998-12-31

    The light actinides show a variety of lattice effects that do not normally appear in other regions of the periodic table. The article will cover the crystal structures of the light actinides, their atomic volumes, their thermal expansion behavior, and their elastic behavior as reflected in recent thermal vibration measurements made by neutron diffraction. A discussion of the melting points will be given in terms of the thermal vibration measurements. Pressure effects will be only briefly indicated.

  18. Transmutation of actinides in power reactors.

    Science.gov (United States)

    Bergelson, B R; Gerasimov, A S; Tikhomirov, G V

    2005-01-01

    Power reactors can be used for partial short-term transmutation of radwaste. This transmutation is beneficial in terms of subsequent storage conditions for spent fuel in long-term storage facilities. CANDU-type reactors can transmute the main minor actinides from two or three reactors of the VVER-1000 type. A VVER-1000-type reactor can operate in a self-service mode with transmutation of its own actinides.

  19. Advances in computational actinide chemistry in China

    Energy Technology Data Exchange (ETDEWEB)

    Wang, Dongqi; Wu, Jingyi; Chai, Zhifang [Chinese Academy of Sciences, Beijing (China). Multidisciplinary Initiative Center; Su, Jing [Chinese Academy of Sciences, Shanghai (China). Div. of Nuclear Materials Science and Engineering; Li, Jun [Tsinghua Univ., Beijing (China). Dept. of Chemistry and Laboratory of Organic Optoelectronics and Molecular Engineering

    2014-04-01

    The advances in computational actinide chemistry made in China are reviewed. Several areas relevant to chemistry of actinides in gas, liquid, and solid phases have been explored. However, we limit the scope to selected contributions in the chemistry of molecular actinide systems in gas and liquid phases. These studies may be classified into two categories: treatment of relativistic effects, which cover the development of two- and four-component Hamiltonians and the optimization of relativistic pseudopotentials, and the applications of theoretical methods in actinide chemistry. The applications include (1) the electronic structures of actinocene, noble gas complexes, An-C multiple bonding compounds, uranyl and its isoelectronic species, fluorides and oxides, molecular systems with metal-metal bonding in their isolated forms (U{sub 2}, Pu{sub 2}) and in fullerene (U{sub 2} rate at C{sub 60}), and the excited states of actinide complexes; (2) chemical reactions, including oxidation, hydrolysis of UF{sub 6}, ligand exchange, reactivities of thorium oxo and sulfido metallocenes, CO{sub 2}/CS{sub 2} functionalization promoted by trivalent uranium complex; and (3) migration of actinides in the environment. A future outlook is discussed. (orig.)

  20. Chemistry of tetravalent actinides phosphates. The thorium phosphate-diphosphate as immobilisation matrix of actinides; Chimie des phosphates d'actinides tetravalents. Le phosphate-diphosphate de thorium en tant que matrice d'imobilisation des actinides

    Energy Technology Data Exchange (ETDEWEB)

    Dacheux, N

    2002-07-01

    The author presents in this document its scientific works from 1992 to 2001, in order to obtain the enabling to manage scientific and chemical researches at the university Paris Sud Orsay. The first part gives an abstract of the thesis on the characterizations, lixiviation and synthesis of uranium and thorium based phosphate matrix in the framework of the search for a ceramic material usable in the radioactive waste storage. The second part presents briefly the researches realized at the CEA, devoted to a reliable, independent and accurate measure of some isotopes activity. The last part presents the abstracts of researches activities from 1996 to 2001 on the tetravalent actinides phosphates chemistry, the sintering of PDT and solid solutions of PDTU and the kinetic and thermodynamical studies of the PDT dissolution. Many references and some publication in full text are provided. (A.L.B.)

  1. Flammability Analysis For Actinide Oxides Packaged In 9975 Shipping Containers

    Energy Technology Data Exchange (ETDEWEB)

    Laurinat, James E.; Askew, Neal M.; Hensel, Steve J.

    2013-03-21

    Packaging options are evaluated for compliance with safety requirements for shipment of mixed actinide oxides packaged in a 9975 Primary Containment Vessel (PCV). Radiolytic gas generation rates, PCV internal gas pressures, and shipping windows (times to reach unacceptable gas compositions or pressures after closure of the PCV) are calculated for shipment of a 9975 PCV containing a plastic bottle filled with plutonium and uranium oxides with a selected isotopic composition. G-values for radiolytic hydrogen generation from adsorbed moisture are estimated from the results of gas generation tests for plutonium oxide and uranium oxide doped with curium-244. The radiolytic generation of hydrogen from the plastic bottle is calculated using a geometric model for alpha particle deposition in the bottle wall. The temperature of the PCV during shipment is estimated from the results of finite element heat transfer analyses.

  2. Elemental partitioning and isotopic fractionation of Zn between metal and silicate and geochemical estimation of the S content of the Earth's core

    Science.gov (United States)

    Mahan, Brandon; Siebert, Julien; Pringle, Emily A.; Moynier, Frédéric

    2017-01-01

    Zinc metal-silicate fractionation provides experimental access to the conditions of core formation and Zn has been used to estimate the S contents of the Earth's core and of the bulk Earth, assuming that they share similar volatility and that Zn was not partitioned into the Earth's core. Therefore, Zn provides both direct and indirect information into the origin and eventual fate of volatile and siderophile elements on Earth. However, the partitioning of Zn between metal and silicate - as well as the associated isotopic fractionation - is not well known. We have conducted a suite of partitioning experiments to characterize Zn elemental partitioning and isotopic fractionation between metal and silicate as a function of time, temperature, and composition. Experiments were conducted at 2 GPa and temperatures from 1473 K to 2273 K in a piston cylinder apparatus, with run durations from 5 to 240 min for four distinct starting materials. Chemical and isotopic equilibrium is achieved within 10 min of experimental outset. Zinc metal-silicate isotopic fractionation displays no resolvable dependence on temperature, composition, or oxygen fugacity within the data set. Therefore, the Zn isotopic composition of silicate phases can be used as a proxy for bulk telluric bodies. Partitioning results from this study and data from literature were used to robustly parameterize Zn metal-silicate partitioning as a function of temperature, pressure, and redox state. Using this parametric characterization and viable formation conditions, we have estimated a range of Zn contents in the cores of iron meteorite parent bodies (i.e. iron meteorites) of ∼0.1-150 ppm, in good agreement with natural observations. We have also calculated the first geochemical estimates for the Zn contents of the Earth's core and of the bulk Earth, at 242 ± 107 ppm and 114 ± 34 ppm (respectively), that consider the slightly siderophile behavior of Zn. These estimates of the Zn contents of the Earth's core and

  3. The isotopic composition of H2 from biomass burning - dependency on combustion efficiency, moisture content and dD of local precipitation

    Science.gov (United States)

    Röckmann, Thomas; Gómez Álvarez, Catalina; Walter, Sylvia; Wollny, Adam; Gunthe, Sachin; Helas, Günter; Pöschl, Ulrich; Keppler, Frank; Greule, Markus; Brand, Willi

    2010-05-01

    Differences in isotopic composition between the various sources of H2 are large, but only few measurements have been carried out to constrain them. For biomass burning, the values quoted in the literature are based on few combustion experiments, which were then extrapolated to the global scale based on a number of assumptions. One of these assumptions is that the isotopic composition of H2 should scale with the isotopic composition of the precipitation at the location where the biomass grew. Here we test this hypothesis using 18 wood samples collected from various locations around the globe. The sample locations cover a range in dD of precipitation from below -120 permil in Siberia and Canada to -15 permil in Zimbabwe. The results confirm the predicted linear relation with dD of the precipitation in the sampling region. The water content itself is found to at most slightly affect the results. Furthermore, dD of H2 depends on combustion efficiency. Thus, the isotopic composition of H2 from biomass burning shows a strong variability around the globe, and between different stages of a fire. It is suggested that this variability, rather than a global bulk number, should be incorporated explicitly in global models that attempt to reproduce the spatial and temporal distribution of dD in H2.

  4. FY2011 Annual Report for the Actinide Isomer Detection Project

    Energy Technology Data Exchange (ETDEWEB)

    Warren, Glen A.; Francy, Christopher J.; Ressler, Jennifer J.; Erikson, Luke E.; Tatishvili, Gocha; Hatarik, R.

    2011-10-01

    This project seeks to identify a new signature for actinide element detection in active interrogation. This technique works by exciting and identifying long-lived nuclear excited states (isomers) in the actinide isotopes and/or primary fission products. Observation of isomers in the fission products will provide a signature for fissile material. For the actinide isomers, the decay time and energy of the isomeric state is unique to a particular isotope, providing an unambiguous signature for SNM. This project entails isomer identification and characterization and neutron population studies. This document summarizes activities from its third year - completion of the isomer identification characterization experiments and initialization of the neutron population experiments. The population and decay of the isomeric state in 235U remain elusive, although a number of candidate gamma rays have been identified. In the course of the experiments, a number of fission fragment isomers were populated and measured [Ressler 2010]. The decays from these isomers may also provide a suitable signature for the presence of fissile material. Several measurements were conducted throughout this project. This report focuses on the results of an experiment conducted collaboratively by PNNL, LLNL and LBNL in December 2010 at LBNL. The measurement involved measuring the gamma-rays emitted from an HEU target when bombarded with 11 MeV neutrons. This report discussed the analysis and resulting conclusions from those measurements. There was one strong candidate, at 1204 keV, of an isomeric signature of 235U. The half-life of the state is estimated to be 9.3 {mu}s. The measured time dependence fits the decay time structure very well. Other possible explanations for the 1204-keV state were investigated, but they could not explain the gamma ray. Unfortunately, the relatively limited statistics of the measurement limit, and the lack of understanding of some of the systematic of the experiment, limit

  5. Content

    DEFF Research Database (Denmark)

    Keiding, Tina Bering

    Aim, content and methods are fundamental categories of both theoretical and practical general didactics. A quick glance in recent pedagogical literature on higher education, however, reveals a strong preoccupation with methods, i.e. how teaching should be organized socially (Biggs & Tang, 2007......; Race, 2001; Ramsden, 2003). This trend appears closely related to the ‘from-teaching-to-learning’ movement, which has had a strong influence on pedagogy since the early nineties (Keiding, 2007; Terhart, 2003). Another interpretation of the current interest in methodology can be derived from...... for selection of content (Klafki, 1985, 2000; Myhre, 1961; Nielsen, 2006). These attempts all share one feature, which is that criteria for selection of content appear very general and often, more or less explicitly, deal with teaching at the first Bologna-cycle; i.e. schooling at the primary and lower...

  6. Actinide transmutation in nuclear reactors

    Energy Technology Data Exchange (ETDEWEB)

    Bultman, J.H.

    1995-01-17

    An optimization method is developed to maximize the burning capability of the ALMR while complying with all constraints imposed on the design for reliability and safety. This method leads to a maximal transuranics enrichment, which is being limited by constraints on reactivity. The enrichment can be raised by using the neutrons less efficiently by increasing leakage from the fuel. With the developed optimization method, a metallic and an oxide fueled ALMR were optimized. Both reactors perform equally well considering the burning of transuranics. However, metallic fuel has a much higher heat conductivity coefficient, which in general leads to better safety characteristics. In search of a more effective waste transmuter, a modified Molten Salt Reactor was designed. A MSR operates on a liquid fuel salt which makes continuous refueling possible, eliminating the issue of the burnup reactivity loss. Also, a prompt negative reactivity feedback is possible for an overmoderated reactor design, even when the Doppler coefficient is positive, due to the fuel expansion with fuel temperature increase. Furthermore, the molten salt fuel can be reprocessed based on a reduction process which is not sensitive to the short-lived spontaneously fissioning actinides. (orig./HP).

  7. Actinide fission and capture cross section measurements at ILL: the Mini-INCA project

    Energy Technology Data Exchange (ETDEWEB)

    Letourneau, A.; Bringer, O.; Chabod, S.; Fioni, G.; Foucher, Y.; Marie, F.; Veyssiere, Ch. [CEA/Saclay/DSM/DAPNIA - Gif-sur-Yvette (France); Mahamid, I. Al. [Lawrence Berkeley National Laboratory, E.H. and S division, Berkeley CA (United States); Blandin, Ch. [CEA/Cadarache/DEN/DER/SPEX - Saint-Paul-lez-Durances (France); Chartier, F. [CEA/Saclay/DEN/DPC/SECR - Gif-sur-Yvette (France); Faust, H.; Mutti, P. [Institut Laue-Langevin, BP 156, F-38042 Grenoble Cedex 9 (France)

    2005-07-01

    Fission cross section of short-lived minor actinides is of prime importance for the incineration of minor actinides in high and thermal neutron fluxes. But due to the shortness of their half-lives, measurements are difficult to handle on these isotopes and the existing data present some large discrepancies. An original method has been developed, in the framework of the Mini-INCA project at ILL, to measure the fission and capture cross sections of minor actinides with low error bars associated even for short-lived isotopes. This method lies on a quasi on-line alpha- and gamma-spectroscopy of irradiated samples and on the use of fission micro-chambers. Coupled to a very powerful Monte-Carlo simulation, both microscopic information on nuclear reactions (total and partial cross sections for neutron capture and/or fission reactions) and macroscopic information on transmutation and incineration potentials could be gathered. In this paper, the method is explained in its originality and some recent results are given and compared with existing measurements and evaluated data libraries. (authors)

  8. TUCS/phosphate mineralization of actinides

    Energy Technology Data Exchange (ETDEWEB)

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

    1997-10-01

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

  9. Testing of an automated online EA-IRMS method for fast and simultaneous carbon content and stable isotope measurement of aerosol samples

    Science.gov (United States)

    Major, István; Gyökös, Brigitta; Túri, Marianna; Futó, István; Filep, Ágnes; Hoffer, András; Molnár, Mihály

    2016-04-01

    Comprehensive atmospheric studies have demonstrated that carbonaceous aerosol is one of the main components of atmospheric particulate matter over Europe. Various methods, considering optical or thermal properties, have been developed for quantification of the accurate amount of both organic and elemental carbon constituents of atmospheric aerosol. The aim of our work was to develop an alternative fast and easy method for determination of the total carbon content of individual aerosol samples collected on prebaked quartz filters whereby the mass and surface concentration becomes simply computable. We applied the conventional "elemental analyzer (EA) coupled online with an isotope ratio mass spectrometer (IRMS)" technique which is ubiquitously used in mass spectrometry. Using this technique we are able to measure simultaneously the carbon stable isotope ratio of the samples, as well. During the developing process, we compared the EA-IRMS technique with an off-line catalytic combustion method worked out previously at Hertelendi Laboratory of Environmental Studies (HEKAL). We tested the combined online total carbon content and stable isotope ratio measurement both on standard materials and real aerosol samples. Regarding the test results the novel method assures, on the one hand, at least 95% of carbon recovery yield in a broad total carbon mass range (between 100 and 3000 ug) and, on the other hand, a good reproducibility of stable isotope measurements with an uncertainty of ± 0.2 per mill. Comparing the total carbon results obtained by the EA-IRMS and the off-line catalytic combustion method we found a very good correlation (R2=0.94) that proves the applicability of both preparation method. Advantages of the novel method are the fast and simplified sample preparation steps and the fully automated, simultaneous carbon stable isotope ratio measurement processes. Furthermore stable isotope ratio results can effectively be applied in the source apportionment

  10. Monazite as a suitable actinide waste form

    Energy Technology Data Exchange (ETDEWEB)

    Schlenz, Hartmut; Heuser, Julia; Schmitz, Stephan; Bosbach, Dirk [Forschungszentrum Juelich GmbH (Germany). Inst. fuer Energie und Klimaforschung (IEK), Nukleare Entsorgung und Reaktorsicherheit (IEK-6); Neumann, Andreas [Forschungszentrum Juelich GmbH (Germany). Inst. fuer Energie und Klimaforschung (IEK), Nukleare Entsorgung und Reaktorsicherheit (IEK-6); RWTH Aachen Univ. (Germany). Inst. for Crystallography

    2013-03-01

    The conditioning of radioactive waste from nuclear power plants and in some countries even of weapons plutonium is an important issue for science and society. Therefore the research on appropriate matrices for the immobilization of fission products and actinides is of great interest. Beyond the widely used borosilicate glasses, ceramics are promising materials for the conditioning of actinides like U, Np, Pu, Am, and Cm. Monazite-type ceramics with general composition LnPO{sub 4} (Ln = La to Gd) and solid solutions of monazite with cheralite or huttonite represent important materials in this field. Monazite appears to be a promising candidate material, especially because of its outstanding properties regarding radiation resistance and chemical durability. This article summarizes the most recent results concerning the characterization of monazite and respective solid solutions and the study of their chemical, thermal, physical and structural properties. The aim is to demonstrate the suitability of monazite as a secure and reliable waste form for actinides. (orig.)

  11. Electronic Structure of the Actinide Metals

    DEFF Research Database (Denmark)

    Johansson, B.; Skriver, Hans Lomholt

    1982-01-01

    Some recent experimental photoelectron spectroscopic results for the actinide metals are reviewed and compared with the theoretical picture of the basic electronic structure that has been developed for the actinides during the last decade. In particular the experimental data confirm the change from...... itinerant to localized 5f electron behaviour calculated to take place between plutonium and americium. From experimental data it is shown that the screening of deep core-holes is due to 5f electrons for the lighter actinide elements and 6d electrons for the heavier elements. A simplified model for the full...... LMTO electronic structure calculations is introduced. In this model the spd and 5f electronic contributions are treated as separable entities. It is shown that the model reproduces quite well the results from the full treatment. The equilibrium volume, cohesive energy and bulk modulus are calculated...

  12. Fabrication and Pre-irradiation Characterization of a Minor Actinide and Rare Earth Containing Fast Reactor Fuel Experiment for Irradiation in the Advanced Test Reactor

    Energy Technology Data Exchange (ETDEWEB)

    Timothy A. Hyde

    2012-06-01

    The United States Department of Energy, seeks to develop and demonstrate the technologies needed to transmute the long-lived transuranic actinide isotopes contained in spent nuclear fuel into shorter lived fission products, thereby decreasing the volume of material requiring disposal and reducing the long-term radiotoxicity and heat load of high-level waste sent to a geologic repository. This transmutation of the long lived actinides plutonium, neptunium, americium and curium can be accomplished by first separating them from spent Light Water Reactor fuel using a pyro-metalurgical process, then reprocessing them into new fuel with fresh uranium additions, and then transmuted to short lived nuclides in a liquid metal cooled fast reactor. An important component of the technology is developing actinide-bearing fuel forms containing plutonium, neptunium, americium and curium isotopes that meet the stringent requirements of reactor fuels and materials.

  13. Assessment of SFR fuel pin performance codes under advanced fuel for minor actinide transmutation

    Energy Technology Data Exchange (ETDEWEB)

    Bouineau, V.; Lainet, M.; Chauvin, N.; Pelletier, M. [French Alternative Energies and Atomic Energy Commission - CEA, CEA Cadarache, DEN/DEC/SESC, 13108 Saint Paul lez Durance (France); Di Marcello, V.; Van Uffelen, P.; Walker, C. [European Commission, Joint Research Centre, Institute for Transuranium Elements, Hermann-von-Helmholtz-Platz 1, D- 76344 Eggenstein-Leopoldshafen (Germany)

    2013-07-01

    Americium is a strong contributor to the long term radiotoxicity of high activity nuclear waste. Transmutation by irradiation in nuclear reactors of long-lived nuclides like {sup 241}Am is, therefore, an option for the reduction of radiotoxicity and residual power packages as well as the repository area. In the SUPERFACT Experiment four different oxide fuels containing high and low concentrations of {sup 237}Np and {sup 241}Am, representing the homogeneous and heterogeneous in-pile recycling concepts, were irradiated in the PHENIX reactor. The behavior of advanced fuel materials with minor actinide needs to be fully characterized, understood and modeled in order to optimize the design of this kind of fuel elements and to evaluate its performances. This paper assesses the current predictability of fuel performance codes TRANSURANUS and GERMINAL V2 on the basis of post irradiation examinations of the SUPERFACT experiment for pins with low minor actinide content. Their predictions have been compared to measured data in terms of geometrical changes of fuel and cladding, fission gases behavior and actinide and fission product distributions. The results are in good agreement with the experimental results, although improvements are also pointed out for further studies, especially if larger content of minor actinide will be taken into account in the codes. (authors)

  14. Actinide and fission product separation and transmutation

    Energy Technology Data Exchange (ETDEWEB)

    NONE

    1993-07-01

    The second international information exchange meeting on actinide and fission product separation and transmutation, took place in Argonne National Laboratory in Illinois United States, on 11-13 November 1992. The proceedings are presented in four sessions: Current strategic system of actinide and fission product separation and transmutation, progress in R and D on partitioning processes wet and dry, progress in R and D on transmutation and refinements of neutronic and other data, development of the fuel cycle processes fuel types and targets. (A.L.B.)

  15. Spin–orbit coupling in actinide cations

    DEFF Research Database (Denmark)

    Bagus, Paul S.; Ilton, Eugene S.; Martin, Richard L.

    2012-01-01

    The limiting case of Russell–Saunders coupling, which leads to a maximum spin alignment for the open shell electrons, usually explains the properties of high spin ionic crystals with transition metals. For actinide compounds, the spin–orbit splitting is large enough to cause a significantly reduced...... spin alignment. Novel concepts are used to explain the dependence of the spin alignment on the 5f shell occupation. We present evidence that the XPS of ionic actinide materials may provide direct information about the angular momentum coupling within the 5f shell....

  16. CONTENTS

    Institute of Scientific and Technical Information of China (English)

    2012-01-01

    The Development and Evolution of the Idea of the Mandate of Heaven in the Zhou Dynasty The changes in the idea of Mandate of Heaven during the Shang and Zhou dynasties are of great significance in the course of the development of traditional Chinese culture. The quickening and awakening of the humanistic spirit was not the entire content of the Zhou idea of Mandate of Heaven. In the process of annihilating the Shang dynasty and setting up their state, the Zhou propagated the idea of the Mandate of Heaven out of practical needs. Their idea of the Mandate of Heaven was not very different from that of the Shang. From the Western Zhou on, the Zhou idea of Mandate of Heaven by no means developed in a linear way along a rational track. The intermingling of rationality and irrationality and of awakening and non-awakening remained the overall state of the Zhou intellectual superstructure after their "spiritual awakening".

  17. Build-up of actinides in irradiated fuel rods of the ET-RR-1 reactor

    Energy Technology Data Exchange (ETDEWEB)

    Adib, M.; Naguib, K.; Morcos, H.N

    2001-09-01

    The content concentrations of actinides are calculated as a function of operating reactor regime and cooling time at different percentage of fuel burn-up. The build-up transmutation equations of actinides content in an irradiated fuel are solved numerically .A computer code BAC was written to operate on a PC computer to provide the required calculations. The fuel element of 10% {sup 235}U enrichment of ET-RR-1 reactor was taken as an example for calculations using the BAC code. The results are compared with other calculations for the ET-RR-1 fuel rod. An estimation of fissile build-up content of a proposed new fuel of 20% {sup 235}U enrichment for ET-RR-1 reactor is given. The sensitivity coefficients of build-up plutonium concentrations as a function of cross-section data uncertainties are also calculated.

  18. Diet analysis of Alaska Arctic snow crabs (Chionoecetes opilio) using stomach contents and δ13C and δ15N stable isotopes

    Science.gov (United States)

    Divine, Lauren M.; Bluhm, Bodil A.; Mueter, Franz J.; Iken, Katrin

    2017-01-01

    We used stomach content and stable δ13C and δ15N isotope analyses to investigate male and female snow crab diets over a range of body sizes (30-130 mm carapace width) in five regions of the Pacific Arctic (southern and northern Chukchi Sea, western, central, and Canadian Beaufort Sea). Snow crab stomach contents from the southern Chukchi Sea were also compared to available prey biomass and abundance. Snow crabs consumed four main prey taxa: polychaetes, decapod crustaceans (crabs, amphipods), echinoderms (mainly ophiuroids), and mollusks (bivalves, gastropods). Both approaches revealed regional differences. Crab diets in the two Chukchi regions were similar to those in the western Beaufort (highest bivalve, amphipod, and crustacean consumption). The Canadian Beaufort region was most unique in prey composition and in stable isotope values. We also observed a trend of decreasing carbon stable isotopes in crabs from the Chukchi to those in the Canadian Beaufort, likely reflecting the increasing use of terrestrial carbon sources towards the eastern regions of the Beaufort Sea from Mackenzie River influx. Cannibalism on snow crabs was higher in the Chukchi regions relative to the Beaufort regions. We suggest that cannibalism may have an impact on recruitment in the Chukchi Sea via reduction of cohort strength after settlement to the benthos, as known from the Canadian Atlantic. Prey composition varied with crab size only in some size classes in the southern Chukchi and central Beaufort, while stable isotope results showed no size-dependent differences. Slightly although significantly higher mean carbon isotope values for males in the southern Chukchi may not be reflective of a gender-specific pattern but rather be driven by low sample size. Finally, the lack of prey selection relative to availability in crabs in the southern Chukchi suggests that crabs consume individual prey taxa in relative proportions to prey field abundances. The present study is the first to

  19. Isotopic evidence of TSR origin for natural gas bearing high H2S contents within the Feixianguan Formation of the northeastern Sichuan Basin, southwestern China

    Institute of Scientific and Technical Information of China (English)

    ZHU Guangyou; ZHANG Shuichang; LIANG Yingbo; DAI Jinxing; LI Jian

    2005-01-01

    The northeastern area of Sichuan Basin, southwestern China, is the area with the maximal reserve of natural gas containing higher hydrogen sulphide (H2S) that has been found among the petroliferous basins of China, with the proven and controlled gas reserve of more than 200 billion cubic meters. These gas pools, with higher H2S contents averaging 9%, some 17%, are mainly distributed on structural belts of Dukouhe, Tieshanpo, Luojiazhai, Puguang, etc., while the oolitic-shoal dolomite of the Triassic Feixianguan Fm. (T1f) is the reservoir. Although many scholars regard the plentiful accumulation of H2S within the deep carbonate reservoir as the result of Thermochemical Sulfate Reduction (TSR), however, the process of TSR as well as its residual geological and geochemical evidence is still not quite clear. Based on the carbon isotopic analysis of carbonate strata and secondary calcite, etc., together with the analysis of sulfur isotopes within H2S, sulphur, gypsum, iron pyrites, etc., as well as other aspects including the natural gas composition, carbon isotopes of hydrocarbons reservoir petrology, etc., it has been proved that the above natural gas is a product of TSR. The H2S, sulphur and calcite result from the participation of TSR reactions by hydrocarbon gas. During the process for hydrocarbons being consumed due to TSR, the carbons within the hydrocarbon gas participate in the reactions and finally are transferred into the secondary calcite, and become the carbon source of secondary calcite, consequently causing the carbon isotopes of the secondary calcite to be lower (-18.2‰). As for both the intermediate product of TSR, i.e. sulfur, and its final products, i.e. H2S and iron pyrites, their sulfur elements are all sourced from the sulfate within the Feixianguan Fm. During the fractional processes of sulfur isotopes, the bond energy leads to the 32S being released firstly, and the earlier it is released, the lower δ34S values for the generated sulphide (H2S

  20. Site-specific {sup 13}C content by quantitative isotopic {sup 13}C Nuclear Magnetic Resonance spectrometry: A pilot inter-laboratory study

    Energy Technology Data Exchange (ETDEWEB)

    Chaintreau, Alain; Fieber, Wolfgang; Sommer, Horst [Firmenich SA, Corporate R and D Division, P.O. Box 239, 1211 Geneva 8 (Switzerland); Gilbert, Alexis; Yamada, Keita [Department of Environmental Chemistry and Engineering, Tokyo Institute of Technology, 4259 Nagatsuta-cho, Midori-ku, Yokohama, Kanagawa 226-8503 (Japan); Yoshida, Naohiro [Department of Environmental Chemistry and Engineering, Tokyo Institute of Technology, 4259 Nagatsuta-cho, Midori-ku, Yokohama, Kanagawa 226-8503 (Japan); Earth-Life Science Institute, Tokyo Institute of Technology, Meguro, Tokyo 152-8551 (Japan); Pagelot, Alain [Bruker Biospin SAS, 34 rue de l‘Industrie, 67166 Wissembourg Cedex (France); Moskau, Detlef; Moreno, Aitor [Bruker Biospin AG, Industriestrasse 26, 8117 Fällanden (Switzerland); Schleucher, Jürgen [Department of Medical Biochemistry and Biophysics, Umeå University, S-90187 Umeå (Sweden); Reniero, Fabiano; Holland, Margaret; Guillou, Claude [European Commission, Joint Research Centre – Institute for Health and Consumer Protection, via E. Fermi 2749, I-21027 Ispra (Italy); Silvestre, Virginie; Akoka, Serge [EBSI team, Interdisciplinary Chemistry: Synthesis, Analysis, Modelling (CEISAM), University of Nantes-CNRS UMR 6230, 2 rue de la Houssinière, BP 92208, F-44322 Nantes cedex 3 (France); Remaud, Gérald S., E-mail: gerald.remaud@univ-nantes.fr [EBSI team, Interdisciplinary Chemistry: Synthesis, Analysis, Modelling (CEISAM), University of Nantes-CNRS UMR 6230, 2 rue de la Houssinière, BP 92208, F-44322 Nantes cedex 3 (France)

    2013-07-25

    Graphical abstract: -- Highlights: •First ring test on isotopic {sup 13}C NMR spectrometry. •Evaluation of the intra- and inter-variability of the NMR spectrometers used. •Definition of a protocol for qualification of the performance of the spectrometer. -- Abstract: Isotopic {sup 13}C NMR spectrometry, which is able to measure intra-molecular {sup 13}C composition, is of emerging demand because of the new information provided by the {sup 13}C site-specific content of a given molecule. A systematic evaluation of instrumental behaviour is of importance to envisage isotopic {sup 13}C NMR as a routine tool. This paper describes the first collaborative study of intra-molecular {sup 13}C composition by NMR. The main goals of the ring test were to establish intra- and inter-variability of the spectrometer response. Eight instruments with different configuration were retained for the exercise on the basis of a qualification test. Reproducibility at the natural abundance of isotopic {sup 13}C NMR was then assessed on vanillin from three different origins associated with specific δ{sup 13}C{sub i} profiles. The standard deviation was, on average, between 0.9 and 1.2‰ for intra-variability. The highest standard deviation for inter-variability was 2.1‰. This is significantly higher than the internal precision but could be considered good in respect of a first ring test on a new analytical method. The standard deviation of δ{sup 13}C{sub i} in vanillin was not homogeneous over the eight carbons, with no trend either for the carbon position or for the configuration of the spectrometer. However, since the repeatability for each instrument was satisfactory, correction factors for each carbon in vanillin could be calculated to harmonize the results.

  1. ENHANCING ADVANCED CANDU PROLIFERATION RESISTANCE FUEL WITH MINOR ACTINIDES

    Energy Technology Data Exchange (ETDEWEB)

    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.

  2. Scalar Static Polarizabilities of Lanthanides and Actinides

    CERN Document Server

    Dzuba, V A; Flambaum, V V

    2014-01-01

    We calculate scalar static polarizabilities for lanthanides and actinides, the atoms with open $4f$ or $5f$ subshell. We show that polarizabilities of the low states are approximately the same for all states of given configuration and present a way of calculating them reducing valence space to just two or three valence electrons occupying $6s$ and $5d$ states for lanthanides or $7s$ and $6d$ states for actinides while $4f$ and $5f$ states are considered to be in the core. Configuration interaction technique is used to calculate polarizabilities of lanthanides and actinides for all states of the $4f^n6s^2$ and $4f^{n-1}6s^25d$ configurations of lanthanides and all states of the $5f^{n}7s^2$ and $5f^{n-1}7s^26d$ configurations of actinides. Polarizability of the electron core (including f-orbitals) has been calculated in the RPA approximation.

  3. Actinide and fission product partitioning and transmutation

    Energy Technology Data Exchange (ETDEWEB)

    NONE

    1995-07-01

    The third international information exchange meeting on actinide and fission product partitioning and transmutation, took place in Cadarache France, on 12-14 December 1994. The proceedings are presented in six sessions : an introduction session, the major programmes and international cooperation, the systems studies, the reactors fuels and targets, the chemistry and a last discussions session. (A.L.B.)

  4. Actinide valences in xenotime and monazite

    Energy Technology Data Exchange (ETDEWEB)

    Vance, E.R. [Institute of Materials Engineering, Australian Nuclear Science and Technology Organisation, Locked Bag 2001 Kirrawee DC, NSW 2232 (Australia); Zhang, Y., E-mail: yzx@ansto.gov.au [Institute of Materials Engineering, Australian Nuclear Science and Technology Organisation, Locked Bag 2001 Kirrawee DC, NSW 2232 (Australia); McLeod, T.; Davis, J. [Institute of Materials Engineering, Australian Nuclear Science and Technology Organisation, Locked Bag 2001 Kirrawee DC, NSW 2232 (Australia)

    2011-02-28

    Tetravalent U, Np and Pu can be substituted by ceramic methods into the rare earth site of xenotime and monazite in air atmospheres using Ca ions as charge compensators, while no evidence of penta- or hexavalent actinide ions was found. Some Pu{sup 3+} and Np{sup 3+} can be incorporated in xenotime samples fired in a reducing atmosphere.

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

    Energy Technology Data Exchange (ETDEWEB)

    Maxwell, S.; Jones, V.

    2009-05-27

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

  6. Selective Separation of Trivalent Actinides from Lanthanides by Aqueous Processing with Introduction of Soft Donor Atoms

    Energy Technology Data Exchange (ETDEWEB)

    Kenneth L. Nash; Sue B. Clark; Gregg Lumetta

    2009-09-23

    With increased application of MOX fuels and longer burnup times for conventional fuels, higher concentrations of the transplutonium actinides Am and Cm (and even heavier species like Bk and Cf) will be produced. The half-lives of the Am isotopes are significantly longer than those of the most important long-lived, high specific activity lanthanides or the most common Cm, Bk and Cf isotopes, thus the greatest concern as regards long-term radiotoxicity. With the removal and transmutation of Am isotopes, radiation levels of high level wastes are reduced to near uranium mineral levels within less than 1000 years as opposed to the time-fram if they remain in the wastes.

  7. Contents

    Directory of Open Access Journals (Sweden)

    Editor IJRED

    2012-11-01

    Full Text Available International Journal of Renewable Energy Development www.ijred.com Volume 1             Number 3            October 2012                ISSN 2252- 4940   CONTENTS OF ARTICLES page Design and Economic Analysis of a Photovoltaic System: A Case Study 65-73 C.O.C. Oko , E.O. Diemuodeke, N.F. Omunakwe, and E. Nnamdi     Development of Formaldehyde Adsorption using Modified Activated Carbon – A Review 75-80 W.D.P Rengga , M. Sudibandriyo and M. Nasikin     Process Optimization for Ethyl Ester Production in Fixed Bed Reactor Using Calcium Oxide Impregnated Palm Shell Activated Carbon (CaO/PSAC 81-86 A. Buasri , B. Ksapabutr, M. Panapoy and N. Chaiyut     Wind Resource Assessment in Abadan Airport in Iran 87-97 Mojtaba Nedaei       The Energy Processing by Power Electronics and its Impact on Power Quality 99-105 J. E. Rocha and B. W. D. C. Sanchez       First Aspect of Conventional Power System Assessment for High Wind Power Plants Penetration 107-113 A. Merzic , M. Music, and M. Rascic   Experimental Study on the Production of Karanja Oil Methyl Ester and Its Effect on Diesel Engine 115-122 N. Shrivastava,  , S.N. Varma and M. Pandey  

  8. Strong linkage of polar cod (Boreogadus saida) to sea ice algae-produced carbon: Evidence from stomach content, fatty acid and stable isotope analyses

    Science.gov (United States)

    Kohlbach, Doreen; Schaafsma, Fokje L.; Graeve, Martin; Lebreton, Benoit; Lange, Benjamin Allen; David, Carmen; Vortkamp, Martina; Flores, Hauke

    2017-03-01

    The polar cod (Boreogadus saida) is considered an ecological key species, because it reaches high stock biomasses and constitutes an important carbon source for seabirds and marine mammals in high-Arctic ecosystems. Young polar cod (1-2 years) are often associated with the underside of sea ice. To evaluate the impact of changing Arctic sea ice habitats on polar cod, we examined the diet composition and quantified the contribution of ice algae-produced carbon (αIce) to the carbon budget of polar cod. Young polar cod were sampled in the ice-water interface layer in the central Arctic Ocean during late summer 2012. Diets and carbon sources of these fish were examined using 4 approaches: (1) stomach content analysis, (2) fatty acid (FA) analysis, (3) bulk nitrogen and carbon stable isotope analysis (BSIA) and (4) compound-specific stable isotope analysis (CSIA) of FAs. The ice-associated (sympagic) amphipod Apherusa glacialis dominated the stomach contents by mass, indicating a high importance of sympagic fauna in young polar cod diets. The biomass of food measured in stomachs implied constant feeding at daily rates of ∼1.2% body mass per fish, indicating the potential for positive growth. FA profiles of polar cod indicated that diatoms were the primary carbon source, indirectly obtained via amphipods and copepods. The αIce using bulk isotope data from muscle was estimated to be >90%. In comparison, αIce based on CSIA ranged from 34 to 65%, with the highest estimates from muscle and the lowest from liver tissue. Overall, our results indicate a strong dependency of polar cod on ice-algae produced carbon. This suggests that young polar cod may be particularly vulnerable to changes in the distribution and structure of sea ice habitats. Due to the ecological key role of polar cod, changes at the base of the sea ice-associated food web are likely to affect the higher trophic levels of high-Arctic ecosystems.

  9. Impact of feeding and short-term temperature stress on the content and isotopic signature of fatty acids, sterols, and alcohols in the scleractinian coral Turbinaria reniformis

    Science.gov (United States)

    Tolosa, I.; Treignier, C.; Grover, R.; Ferrier-Pagès, C.

    2011-09-01

    This study assesses the combined effect of feeding and short-term thermal stress on various physiological parameters and on the fatty acid, sterol, and alcohol composition of the scleractinian coral Turbinaria reniformis. The compound-specific carbon isotope composition of the lipids was also measured. Under control conditions (26°C), feeding with Artemia salina significantly increased the symbiont density and chlorophyll content and the growth rates of the corals. It also doubled the concentrations of almost all fatty acid (FA) compounds and increased the n-alcohol and sterol contents. δ13C results showed that the feeding enhancement of FA concentrations occurred either via a direct pathway, for one of the major polyunsaturated fatty acid (PUFA) compounds of the food (18:3n-3 FA), or via an enhancement of photosynthate transfer (indirect pathway), for the other coral FAs. Cholesterol (C27Δ5) was also directly acquired from the food. Thermal stress (31°C) affected corals, but differently according to their feeding status. Chlorophyll, protein content, and maximal photosynthetic efficiency of photosystem II (PSII) decreased to a greater extent in starved corals. In such corals, FA concentrations were reduced by 33%, (especially C16, C18 FAs, and n-3 PUFA) and the sterol content by 27% (especially the C28∆5,22 and C28∆5). The enrichment in the δ13C signature of the storage and structural FAs suggests that they were the main compounds respired during the stress to maintain the coral metabolism. Thermal stress had less effect on the lipid concentrations of fed corals, as only FA levels were reduced by 13%, with no major changes in their isotope carbon signatures. In conclusion, feeding plays an essential role in sustaining T. reniformis metabolism during the thermal stress.

  10. SRNL Development of Recovery Processes for Mark-18A Heavy Actinide Targets

    Energy Technology Data Exchange (ETDEWEB)

    Allender, Jeffrey S. [Savannah River Site (SRS), Aiken, SC (United States). Savannah River National Lab. (SRNL); Bridges, Nicholas J. [Savannah River Site (SRS), Aiken, SC (United States). Savannah River National Lab. (SRNL); Loftin, Bradley M. [Savannah River Site (SRS), Aiken, SC (United States). Savannah River National Lab. (SRNL); Dunsmuir, Michael D. [Savannah River Site (SRS), Aiken, SC (United States). Savannah River National Lab. (SRNL)

    2015-07-14

    Savannah River National Laboratory (SRNL) and Oak Ridge National Laboratory (ORNL) are developing plans for the recovery of rare and unique isotopes contained within heavy-actinide target assemblies, specifically the Mark-18A. Mark-18A assemblies were irradiated in Savannah River Site (SRS) reactors in the 1970s under extremely high neutron-flux conditions and produced, virtually, the world's supply of plutonium-244, an isotope of key importance to high-precision actinide measurement and other scientific and nonproliferation uses; and curium highly enriched in heavy isotopes (e.g., curium-246 and curium-248). In 2015 and 2016, SRNL is pursuing tasks that would reduce program risk and budget requirements, including further characterization of unprocessed targets; engineering studies for the use of the SRNL Shielded Cells Facility (SCF) for recovery; and development of onsite and offsite shipping methods including a replacement for the heavy (70 ton) cask previously used for onsite transfer of irradiated items at SRS. A status update is provided for the characterization, including modeling using the Monte Carlo N-Particle Transport Code (MCNP); direct non-destructive assay measurements; and cask design.

  11. Adventures in Actinide Chemistry: A Year of Exploring Uranium and Thorium in Los Alamos

    Energy Technology Data Exchange (ETDEWEB)

    Pagano, Justin [Los Alamos National Lab. (LANL), Los Alamos, NM (United States)

    2016-01-08

    The first part of this collection of slides is concerned with considerations when working with actinides. The topics discussed in the document as a whole are the following: Actinide chemistry vs. transition metal chemistry--tools we can use; New synthetic methods to obtain actinide hydrides; Actinide metallacycles: synthesis, structure, and properties; and Reactivity of actinide metallacycles.

  12. Synthesis of actinide nitrides, phosphides, sulfides and oxides

    Science.gov (United States)

    Van Der Sluys, William G.; Burns, Carol J.; Smith, David C.

    1992-01-01

    A process of preparing an actinide compound of the formula An.sub.x Z.sub.y wherein An is an actinide metal atom selected from the group consisting of thorium, uranium, plutonium, neptunium, and americium, x is selected from the group consisting of one, two or three, Z is a main group element atom selected from the group consisting of nitrogen, phosphorus, oxygen and sulfur and y is selected from the group consisting of one, two, three or four, by admixing an actinide organometallic precursor wherein said actinide is selected from the group consisting of thorium, uranium, plutonium, neptunium, and americium, a suitable solvent and a protic Lewis base selected from the group consisting of ammonia, phosphine, hydrogen sulfide and water, at temperatures and for time sufficient to form an intermediate actinide complex, heating said intermediate actinide complex at temperatures and for time sufficient to form the actinide compound, and a process of depositing a thin film of such an actinide compound, e.g., uranium mononitride, by subliming an actinide organometallic precursor, e.g., a uranium amide precursor, in the presence of an effectgive amount of a protic Lewis base, e.g., ammonia, within a reactor at temperatures and for time sufficient to form a thin film of the actinide compound, are disclosed.

  13. Measurement of electro-sprayed 238 and 239+240 plutonium isotopes using 4{pi}-alpha spectrometry. Application to environmental samples; Spectrometrie alpha 4{pi} de sources d'actinides realisees par electronebulisation. Developpement et optimisation d'un protocole applique au mesurage des isotopes 238 et 239+240 du plutonium dans l'environnement

    Energy Technology Data Exchange (ETDEWEB)

    Charmoille-Roblot, M. [CEA/Fontenay-aux-Roses, Dept. de Protection de l' Environnement (DPRE), 92 (France)]|[Paris-11 Univ., 91 - Orsay (France)

    1999-07-01

    A new protocol for plutonium deposition using the electro-spray technique coupled with 4{pi}-{alpha} spectrometry is proposed to improve the detection limit, shorten the counting time. In order to increase the detection efficiency, it was proposed to measure 238 and 239+240 plutonium isotopes electro-sprayed deposit simultaneously on both sides of the source support, that must be as transparent as possible to alpha-emissions, in a two-alpha detectors chamber. A radiochemical protocol was adapted to electro-spray constraints and a very thin carbon foil was selected for 4{pi} -alpha spectrometry. The method was applied to a batch of sediment samples and gave the same results as an electrodeposited source measured using conventional alpha spectrometry with a 25 % gain on counting time and 10 % on plutonium 238 detection limit. Validation and application of the technique have been made on reference samples. (author)

  14. Effect of spectral characterization of gaseous fuel reactors on transmutation and burning of actinides

    Energy Technology Data Exchange (ETDEWEB)

    Fung, C.; Anghaie, S. [Florida Univ., Wilmington, NC (United States)

    2007-07-01

    Gaseous Core Reactors (GCR) are fueled with stable uranium compounds in a reflected cavity. The spectral characteristics of neutrons in GCR systems could shift from one end of the spectrum to the other end by changing design parameters such as reflector material and thickness, uranium enrichment, and the average operational temperature and pressure. The rate of actinide generation, transmutation, and burnup is highly influenced by the average neutron energy in reactor core. In particular, the production rate and isotopic mix of plutonium are highly dependent on the neutron spectrum in the reactor. Other actinides of primary interest to this work are neptunium-237 and americium-241 due to their pivotal impact on high-level nuclear waste disposal. In all cavity reactors including GCR's, the reflector material and thickness are the most important design parameters in determining the core spectrum. The increase in the gaseous fuel pressure and enrichment results in relative shift of neutron population toward energies greater than 2 eV. Reflector materials considered in this study are beryllium oxide, lithium hydride, lithium deuteride, zirconium carbide, graphite, lead, and tungsten. Results of the study suggest that the beryllium oxide and tungsten reflected GCR systems set the lower (softest) and upper (hardest) limits of neutron spectra, respectively. The inventory of actinides with half-lives greater than 1000 years can be minimized by increasing neutron flux level in the reactor core. The higher the neutron flux, the lower the inventory of these actinides. The majority of the GCR designs maintained a flux level on the order of 10{sup 15} cm{sup -2}*s{sup -1} while the PWR flux is one order of magnitude lower. The inventory of the feeder isotopes to Np{sup 237} including U{sup 237}, Pu{sup 241}, and Am{sup 241} decreases with relative shift of neutron spectrum toward higher energies. This is due to increased resonance absorption in these isotopes due to higher

  15. Oxidative dissolution of actinide oxides in H 2O 2 containing aqueous solution - A preliminary study

    Science.gov (United States)

    Pehrman, Reijo; Amme, Marcus; Roth, Olivia; Ekeroth, Ella; Jonsson, Mats

    2010-02-01

    Oxidative dissolution of spent nuclear fuel is an important issue in the safety assessment of a future geological repository for spent nuclear fuel. Although UO 2 constitutes, in terms of mass, the majority of the spent fuel material, its main radiotoxicity is (after extended storage times) contained in actinides with half lives shorter than that of 238-uranium, such as isotopes of Np and Pu. Relatively little information is available on the dissolution behavior of Np and Pu in comparable environments. This work investigates the oxidative dissolution of NpO 2 and PuO 2 in non-complexing aqueous solutions containing H 2O 2 and compares their behavior with that of UO 2. We have found that oxidative dissolution takes place for all three actinides in the presence of H 2O 2. Based on the obtained dissolution rates, we would not expect the dissolution of the actinides to be congruent. Instead, in a system without complexing agent, the release rates of Np and Pu are expected to be lower than the U release rate.

  16. Electrorecovery of actinides at room temperature

    Energy Technology Data Exchange (ETDEWEB)

    Stoll, Michael E [Los Alamos National Laboratory; Oldham, Warren J [Los Alamos National Laboratory; Costa, David A [Los Alamos National Laboratory

    2008-01-01

    There are a large number of purification and processing operations involving actinide species that rely on high-temperature molten salts as the solvent medium. One such application is the electrorefining of impure actinide metals to provide high purity material for subsequent applications. There are some drawbacks to the electrodeposition of actinides in molten salts including relatively low yields, lack of accurate potential control, maintaining efficiency in a highly corrosive environment, and failed runs. With these issues in mind we have been investigating the electrodeposition of actinide metals, mainly uranium, from room temperature ionic liquids (RTILs) and relatively high-boiling organic solvents. The RTILs we have focused on are comprised of 1,3-dialkylimidazolium or quaternary ammonium cations and mainly the {sup -}N(SO{sub 2}CF{sub 3}){sub 2} anion [bis(trif1uoromethylsulfonyl)imide {equivalent_to} {sup -}NTf{sub 2}]. These materials represent a class of solvents that possess great potential for use in applications employing electrochemical procedures. In order to ascertain the feasibility of using RTILs for bulk electrodeposition of actinide metals our research team has been exploring the electron transfer behavior of simple coordination complexes of uranium dissolved in the RTIL solutions. More recently we have begun some fundamental electrochemical studies on the behavior of uranium and plutonium complexes in the organic solvents N-methylpyrrolidone (NMP) and dimethylsulfoxide (DMSO). Our most recent results concerning electrodeposition will be presented in this account. The electrochemical behavior of U(IV) and U(III) species in RTILs and the relatively low vapor pressure solvents NMP and DMSO is described. These studies have been ongoing in our laboratory to uncover conditions that will lead to the successful bulk electrodeposition of actinide metals at a working electrode surface at room temperature or slightly elevated temperatures. The RTILs we

  17. Recovery of actinides from actinide-aluminium alloys by chlorination: Part I

    Science.gov (United States)

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

    2011-07-01

    Pyrochemical processes in molten LiCl-KCl are being developed in ITU for recovery of actinides from spent nuclear fuel. The fuel is anodically dissolved to the molten salt electrolyte and actinides are electrochemically reduced on solid aluminium cathodes forming solid actinide-aluminium alloys. A chlorination route is being investigated for recovery of actinides from the alloys. This route consists in three steps: Vacuum distillation for removal of the salt adhered on the electrode, chlorination of the actinide-aluminium alloys by chlorine gas and sublimation of the formed AlCl 3. A thermochemical study showed thermodynamic feasibility of all three steps. On the basis of the conditions identified by the calculations, experiments using pure UAl 3 alloy were carried out to evaluate and optimise the chlorination step. The work was focused on determination of the optimal temperature and Cl 2/UAl 3 molar ratio, providing complete chlorination of the alloy without formation of volatile UCl 5 and UCl 6. The results showed high efficient chlorination at a temperature of 150 °C.

  18. Actinide and fission product separation and transmutation

    Energy Technology Data Exchange (ETDEWEB)

    NONE

    1991-07-01

    The first international information exchange meeting on actinide and fission product separation and transmutation, took place in Mito in Japan, on 6-8 November 1990. It starts with a number of general overview papers to give us some broad perspectives. Following that it takes a look at some basic facts about physics and about the quantities of materials it is talking about. Then it proceeds to some specific aspects of partitioning, starting with evolution from today commercially applied processes and going on to other possibilities. At the end of the third session it takes a look at the significance of partitioning and transmutation of actinides before it embarks on two sessions on transmutation, first in reactors and second in accelerators. The last session is designed to throw back into the discussion the main points which need to be looked at when considering future work in this area. (A.L.B.)

  19. Microbial Transformations of Actinides and Other Radionuclides

    Energy Technology Data Exchange (ETDEWEB)

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

    2009-01-07

    Microorganisms can affect the stability and mobility of the actinides and other radionuclides released from nuclear fuel cycle and from nuclear fuel reprocessing plants. Under appropriate conditions, microorganisms can alter the chemical speciation, solubility and sorption properties and thus could increase or decrease the concentrations of radionuclides in solution in the environment and the bioavailability. Dissolution or immobilization of radionuclides is brought about by direct enzymatic action or indirect non-enzymatic action of microorganisms. Although the physical, chemical, and geochemical processes affecting dissolution, precipitation, and mobilization of radionuclides have been extensively investigated, we have only limited information on the effects of microbial processes and biochemical mechanisms which affect the stability and mobility of radionuclides. The mechanisms of microbial transformations of the major and minor actinides U, Pu, Cm, Am, Np, the fission products and other radionuclides such as Ra, Tc, I, Cs, Sr, under aerobic and anaerobic conditions in the presence of electron donors and acceptors are reviewed.

  20. SPECIFIC SEQUESTERING AGENTS FOR THE ACTINIDES

    Energy Technology Data Exchange (ETDEWEB)

    Raymond, Kenneth N.; Smith, William L.; Weitl, Frederick L.; Durbin, Patricia W.; Jones, E.Sarah; Abu-Dari, Kamal; Sofen, Stephen R.; Cooper, Stephen R.

    1979-09-01

    This paper summarizes the current status of a continuing project directed toward the synthesis and characterization of chelating agents which are specific for actinide ions - especially Pu(IV) - using a biomimetic approach that relies on the observation that Pu(IV) and Fe(III) has marked similarities that include their biological transport and distribution in mammals. Since the naturally-occurring Fe(III) sequestering agents produced by microbes commonly contain hydroxamate and catecholate functional groups, these groups should complex the actinides very strongly and macrocyclic ligands incorporating these moieties are being prepared. We have reported the isolation and structure analysis of an isostructural series of tetrakis(catecholato) complexes with the general stoichiometry Na{sub 4}[M(C{sub 6}H{sub 4}O{sub 2}){sub 4}] • 21 H{sub 2}O (M = Th, U, Ce, Hf). These complexes are structural archetypes for the cavity that must be formed if an actinide-specific sequestering agent is to conform ideally to the coordination requirements of the central metal ion. The [M(cat){sub 4}]{sup 4-} complexes have the D{sub 2d} symmetry of the trigonal-faced dodecahedron.. The complexes Th [R'C(0)N(O)R]{sub 4} have been prepared where R = isopropyl and R' = t-butyl or neopentyl. The neopentyl derivative is also relatively close to an idealized D{sub 2d} dodecahedron, while the sterically more hindered t-butyl compound is distorted toward a cubic geometry. The synthesis of a series of 2, 3-dihydroxy-benzoyl amide derivatives of linear and cyclic tetraaza- and diazaalkanes is reported. Sulfonation of these compounds improves the metal complexation and in vivo removal of plutonium from test animals. These results substantially exceed the capabilities of compounds presently used for the therapeutic treatment of actinide contamination.

  1. Actinide and fission product partitioning and transmutation

    Energy Technology Data Exchange (ETDEWEB)

    NONE

    1997-07-01

    The fourth international information exchange meeting on actinide and fission product partitioning and transmutation, took place in Mito City in Japan, on 111-13 September 1996. The proceedings are presented in six sessions: the major programmes and international cooperation, the partitioning and transmutation programs, feasibility studies, particular separation processes, the accelerator driven transmutation, and the chemistry of the fuel cycle. (A.L.B.)

  2. Preparation, properties, and some recent studies of the actinide metals

    Energy Technology Data Exchange (ETDEWEB)

    Haire, R.G.

    1985-01-01

    The actinide elements form a unique series of metals. The variation in their physial properties combined with the varying availability of the different elements offers a challenge to the preparative scientist. This article provides a brief review of selected methods used for preparing ..mu..g to kg amounts of the actinide metals and the properties of these metals. In addition, some recent studies on selected actinide metals are discussed. 62 refs.

  3. Comparison of actinides and fission products recycling scheme with the normal plutonium recycling scheme in fast reactors

    Directory of Open Access Journals (Sweden)

    Salahuddin Asif

    2013-01-01

    Full Text Available Multiple recycling of actinides and non-volatile fission products in fast reactors through the dry re-fabrication/reprocessing atomics international reduction oxidation process has been studied as a possible way to reduce the long-term potential hazard of nuclear waste compared to that resulting from reprocessing in a wet PUREX process. Calculations have been made to compare the actinides and fission products recycling scheme with the normal plutonium recycling scheme in a fast reactor. For this purpose, the Karlsruhe version of isotope generation and depletion code, KORIGEN, has been modified accordingly. An entirely novel fission product yields library for fast reactors has been created which has replaced the old KORIGEN fission products library. For the purposes of this study, the standard 26 groups data set, KFKINR, developed at Forschungszentrum Karlsruhe, Germany, has been extended by the addition of the cross-sections of 13 important actinides and 68 most important fission products. It has been confirmed that these 68 fission products constitute about 95% of the total fission products yield and about 99.5% of the total absorption due to fission products in fast reactors. The amount of fissile material required to guarantee the criticality of the reactor during recycling schemes has also been investigated. Cumulative high active waste per ton of initial heavy metal is also calculated. Results show that the recycling of actinides and fission products in fast reactors through the atomics international reduction oxidation process results in a reduction of the potential hazard of radioactive waste.

  4. Actinide and lanthanide separation process (ALSEP)

    Science.gov (United States)

    Guelis, Artem V.

    2013-01-15

    The process of the invention is the separation of minor actinides from lanthanides in a fluid mixture comprising, fission products, lanthanides, minor actinides, rare earth elements, nitric acid and water by addition of an organic chelating aid to the fluid; extracting the fluid with a solvent comprising a first extractant, a second extractant and an organic diluent to form an organic extractant stream and an aqueous raffinate. Scrubbing the organic stream with a dicarboxylic acid and a chelating agent to form a scrubber discharge. The scrubber discharge is stripped with a simple buffering agent and a second chelating agent in the pH range of 2.5 to 6.1 to produce actinide and lanthanide streams and spent organic diluents. The first extractant is selected from bis(2-ethylhexyl)hydrogen phosphate (HDEHP) and mono(2-ethylhexyl)2-ethylhexyl phosphonate (HEH(EHP)) and the second extractant is selected from N,N,N,N-tetra-2-ethylhexyl diglycol amide (TEHDGA) and N,N,N',N'-tetraoctyl-3-oxapentanediamide (TODGA).

  5. Recovery of actinides from actinide-aluminium alloys by chlorination: Part II

    Science.gov (United States)

    Souček, P.; Cassayre, L.; Eloirdi, R.; Malmbeck, R.; Meier, R.; Nourry, C.; Claux, B.; Glatz, J.-P.

    2014-04-01

    A chlorination route is being investigated for recovery of actinides from actinide-aluminium alloys, which originate from pyrochemical recovery of actinides from spent metallic nuclear fuel by electrochemical methods in molten LiCl-KCl. In the present work, the most important steps of this route were experimentally tested using U-Pu-Al alloy prepared by electrodeposition of U and Pu on solid aluminium plate electrodes. The investigated processes were vacuum distillation for removal of the salt adhered on the electrode, chlorination of the alloy by chlorine gas and sublimation of the AlCl3 formed. The processes parameters were set on the base of a previous thermochemical study and an experimental work using pure UAl3 alloy. The present experimental results indicated high efficiency of salt distillation and chlorination steps, while the sublimation step should be further optimised.

  6. Hydrothermal decomposition of actinide(IV oxalates: a new aqueous route towards reactive actinide oxide nanocrystals

    Directory of Open Access Journals (Sweden)

    Walter Olaf

    2016-01-01

    Full Text Available The hydrothermal decomposition of actinide(IV oxalates (An= Th, U, Pu at temperatures between 95 and 250 °C is shown to lead to the production of highly crystalline, reactive actinide oxide nanocrystals (NCs. This aqueous process proved to be quantitative, reproducible and fast (depending on temperature. The NCs obtained were characterised by X-ray diffraction and TEM showing their size to be smaller than 15 nm. Attempts to extend this general approach towards transition metal or lanthanide oxalates failed in the 95–250 °C temperature range. The hydrothermal decomposition of actinide oxalates is therefore a clean, flexible and powerful approach towards NCs of AnO2 with possible scale-up potential.

  7. Distribution Coefficients of Elements on TODGA Resin in HNO3, HCl and HF: Application to Determination of Lu/Hf Ratio and Hf Isotopic Composition in Meteorites

    Science.gov (United States)

    Pourmand, A.; Dauphas, N.

    2008-03-01

    Distribution coefficients for 60 elements on TODGA resin are presented along with a robust single-column protocol for separation of HSFE, lanthanides and actinides in meteorites and terrestrial rocks for high-precision isotope analysis.

  8. An Analysis of Sulfur Content and Multiple Sulfur Isotope Fractionation of Tephra Deposits at Valles Caldera, New Mexico: Variations over the Course of Two Caldera-Forming Eruptions

    Science.gov (United States)

    Campbell, M. E.; Wing, B. A.; Stix, J.

    2010-12-01

    analyses for the LBT and UBT high-silica rhyolite ignimbrite samples are relatively moderate, varying from 3.5 to 4.3‰. Whole rock sulfur concentrations range from only 4 mg S/kg rock to 393 mg S/kg rock. Measured δ34S values and their corresponding whole rock sulfur concentrations are broadly inversely correlated, and are most simply interpreted as a series of degassing events that enriched the residual Valles magma in isotopically-heavy S. The S profiles of the LBT and UBT erupted products show similar trends: from the early plinian through to the late plinian units, S contents decrease and δ34S values increase, then plateau at the ignimbrite. Both profiles start out with δ34S values near 0‰, indicative of a relatively primitive, mafic source for the S in the Valles complex, and perhaps for the caldera-forming eruptions themselves.

  9. Oxygen isotopes and volatile contents of the Gorgona komatiites, Colombia: A confirmation of the deep mantle origin of H2O

    Science.gov (United States)

    Gurenko, Andrey A.; Kamenetsky, Vadim S.; Kerr, Andrew C.

    2016-11-01

    We report O isotopes in olivine grains (Fo89-93) and volatile contents (CO2, H2O, F, S, Cl) in olivine-hosted melt inclusions from one Gorgona picrite and five komatiites with the aim of constraining the origin of H2O in these magmas. These samples have previously been analysed for major and trace elements and volatile concentrations (H2O, S, Cl) and B isotopes in melt inclusions. A distinctive feature of the included melts is relatively high contents of volatile components and boron, which show positive anomalies in, otherwise depleted, primitive mantle normalised trace and rare earth element patterns and range in δ11 B from -11.5 to 15.6‰. In this study, the olivines were systematically analysed for O isotopes (1) in the centre of grains, (2) near the grain boundaries and, (3) as close as possible to the studied melt inclusions. The majority of olivines (∼66%) are "mantle"-like, 4.8 ‰ ≤δ18 O ≤ 5.5 ‰, with a subordinate but still significant number (∼33%) above, and only 2 grains below, this range. There is no systematic difference between the central and marginal parts of the grains. Higher than "mantle" δ18OOl values are ascribed to low-T (<300 °C) serpentinisation along inner fractures and grain boundaries of olivine phenocrysts. The measured concentrations of volatile components in the melt inclusions corrected for the effects of post-entrapment crystallisation and H2O-CO2 exsolution in inclusion shrinkage bubbles are: 286-1748 μg/g CO2, 0.2-0.86 wt.% H2O, 48-82 μg/g F, 398-699 μg/g S and 132-198 μg/g Cl. They correspond to a pressure of 86 ± 44MPa or ∼2.5-km crustal depth of olivine crystallisation. The correlations of S and, to a lesser extent, of H2O, with highly incompatible lithophile elements and the correlation of F with Cl, but no relationships of H2O with Cl, rule out shallow depth magma degassing and/or crustal contamination. Our new δ18 O olivine and volatile component data combined with the existing, highly variable δ11 B

  10. Advanced Aqueous Separation Systems for Actinide Partitioning

    Energy Technology Data Exchange (ETDEWEB)

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

    2015-04-02

    One of the most challenging aspects of advanced processing of used nuclear fuel is the separation of transplutonium actinides from fission product lanthanides. This separation is essential if actinide transmutation options are to be pursued in advanced fuel cycles, as lanthanides compete with actinides for neutrons in both thermal and fast reactors, thus limiting efficiency. The separation is difficult because the chemistry of Am3+ and Cm3+ is nearly identical to that of the trivalent lanthanides (Ln3+). The prior literature teaches that two approaches offer the greatest probability of devising a successful group separation process based on aqueous processes: 1) the application of complexing agents containing ligand donor atoms that are softer than oxygen (N, S, Cl-) or 2) changing the oxidation state of Am to the IV, V, or VI state to increase the essential differences between Am and lanthanide chemistry (an approach utilized in the PUREX process to selectively remove Pu4+ and UO22+ from fission products). The latter approach offers the additional benefit of enabling a separation of Am from Cm, as Cm(III) is resistant to oxidation and so can easily be made to follow the lanthanides. The fundamental limitations of these approaches are that 1) the soft(er) donor atoms that interact more strongly with actinide cations than lanthanides form substantially weaker bonds than oxygen atoms, thus necessitating modification of extraction conditions for adequate phase transfer efficiency, 2) soft donor reagents have been seen to suffer slow phase transfer kinetics and hydro-/radiolytic stability limitations and 3) the upper oxidation states of Am are all moderately strong oxidants, hence of only transient stability in media representative of conventional aqueous separations systems. There are examples in the literature of both approaches having been described. However, it is not clear at present that any extant process is sufficiently robust for application at the scale

  11. Estimating Change in Sedimentary Organic Carbon Content During Mangrove Restoration in Southern China Using Carbon Isotopic Measurements

    Institute of Scientific and Technical Information of China (English)

    ZHANG Jin-Ping; SHEN Cheng-De; REN Hai; WANG Jun; HAN Wei-Dong

    2012-01-01

    Based on total carbon (C) and C isotopes in sediment cores,sedimentary organic carbon (SOC) was quantified in three types of mangrove sites (barren fiat sites without mangroves,mangrove plantations,and natural mangrove forests),which were considered to represent a continuum from least restored to most restored sites in southern China.SOC densities in the barren sites,plantations,and natural forests were 90,170 and 288 Mg ha-1,respectively.We inferred that mangrove restoration increased SOC accumulation in coastal areas.At 0-70 cm depth,SOC δ13C values in both mangrove sites ranged from -27.37‰ to -23.07‰ and exhibited gradual enrichment with depth.In contrast,the values in the barren flat sites remained around -22.19‰ and fluctuated slightly with depth.At 0-60 cm,the 14C ages of the SOC in the barren flat site,the natural mangrove site,and the artificial mangrove site ranged from 1397 to 2 608,255 to 2 453,and 391 to 2512 years BP,respectively.In both types of mangrove sites but not in the barren flat sites,the enrichment of δ13C with depth was related to increases in SOC decay and SOC age with depth.According to analysis of 14C age,much of the mangrove-derived C was transported and stored at 0-60 cm depth under anaerobic conditions in both mangrove sites.The sediments of mangrove forests in southern China sequester large quantities of SOC during mangrove restoration.

  12. Diversity of trophic niches among herbivorous fishes on a Caribbean reef (Guadeloupe, Lesser Antilles), evidenced by stable isotope and gut content analyses

    Science.gov (United States)

    Dromard, Charlotte R.; Bouchon-Navaro, Yolande; Harmelin-Vivien, Mireille; Bouchon, Claude

    2015-01-01

    While herbivorous fishes have been widely studied due to the major ecological role they play on coral reefs, the description of their trophic niche remains challenging. In this study, we asked how 10 species of parrotfishes and surgeonfishes partition trophic resources on a Caribbean reef. The determination of trophic niches was conducted using gut and stomach content and stable isotope analyses (15N:14N and 13C:12C ratios). The contributions of food source to fish diet were calculated with concentration-dependent mixing models. Stomach content analyses distinguished two species of Acanthuridae from other fish species: Acanthurus coeruleus due to its high ingestion of fleshy macroalgae and Acanthurus chirurgus due to its high ingestion of calcified macroalgae. Acanthuridae and Sparisoma aurofrenatum presented similar diets in terms of assimilation of food resources with a high contribution of detritus and invertebrates to their diets. The diets of Sparisoma rubripinne and Sparisoma chrysopterum were more heterogeneous by comparison to the previous species. Scarus iseri, Scarus vetula, Scarus taeniopterus and Sparisoma viride appeared to share a similar trophic niche characterized by the contribution of live coral and fleshy macroalgae to their diet. The resource use among herbivorous fishes was partially related to the nutritional quality of food sources, but also to their physical structure and the capacity of fish to process them efficiently. These results showed that the ten species occupy distinct trophic niches, indicating a high functional diversity among the Caribbean herbivorous fishes.

  13. Chemistry of lower valent actinide halides

    Energy Technology Data Exchange (ETDEWEB)

    Lau, K.H.; Hildenbrand, D.L.

    1992-01-01

    This research effort was concerned almost entirely with the first two members of the actinide series, thorium and uranium, although the work was later extended to some aspects of the neptunium-fluorine system in a collaborative program with Los Alamos National Laboratory. Detailed information about the lighter actinides will be helpful in modeling the properties of the heavier actinide compounds, which will be much more difficult to study experimentally. In this program, thermochemical information was obtained from high temperature equilibrium measurements made by effusion-beam mass spectrometry and by effusion-pressure techniques. Data were derived primarily from second-law analysis so as to avoid potential errors in third-law calculations resulting from uncertainties in spectroscopic and molecular constants. This approach has the additional advantage of yielding reaction entropies that can be checked for consistency with various molecular constant assignments for the species involved. In the U-F, U-Cl, and U-Br systems, all of the gaseous species UX, UX{sub 2}, UX{sub 3}, UX{sub 4}, and UX{sub 5}, where X represents the halogen, were identified and characterized; the corresponding species ThX, ThX{sub 2}, ThX{sub 3}, and ThX{sub 4} were studied in the Th-F, Th-Cl, and Th-Br systems. A number of oxyhalide species in the systems U-0-F, U-0-Cl, Th-0-F, and Th-O-Cl were studied thermochemically. Additionally, the sublimation thermodynamics of NpF{sub 4}(s) and NpO{sub 2}F{sub 2}(s) were studied by mass spectrometry.

  14. Trace analysis of actinides in the environment using resonance ionization mass spectrometry; Spurenanalyse von Aktiniden in der Umwelt mittels Resonanzionisations-Massenspektrometrie

    Energy Technology Data Exchange (ETDEWEB)

    Raeder, Sebastian

    2011-04-12

    In this work the resonant ionization of neutral atoms using laser radiation was applied and optimized for ultra-trace analysis of the actinides thorium, uranium, neptunium and plutonium. The sensitive detection of these actinides is a challange for the monitoring and quantification of radioactive releases from nuclear facilities. Using resonance ionization spectroscopy combined with a newly developed quadrupole-mass-spectrometer, numerous energy levels in the atomic structure of these actinides could be identified. With this knowledge efficient excitation schemes for the mentioned actinides could be identified and characterised. The applied in-source-ionization ensures for a high detection efficiency due to the good overlap of laser radiation with the atomic beam and allows therefore for a low sample consumption which is required for the analysis of radio nuclides. The selective excitation processes in the resonant ionization method supresses unwanted contaminations and was optimized for analytical detection of ultra-trace amounts in environmental samples as well as for determination of isotopic compositions. The efficient in-source-ionization combined with high power pulsed laser radiation allows for detections efficiency up to 1%. For plutonium detection limits in the range of 10{sup 4}-10{sup 5} atoms could be demonstrated for synthetic samples as well as for first environmental samples. The usage of narrow bandwidth continuous wave lasers in combination with a transversal overlap of the laser radiation and the free propagating atomic beam enable for resolving individual isotopic shifts of the resonant transitions. This results in a high selectivity against dominant neighboring isotopes but with a significant loss in detection efficiency. For the ultra-trace isotope {sup 236}U a detection limit down to 10{sup -9} for the isotope ratio N ({sup 236}U)/N ({sup 238}U) could be determined.

  15. Electronic structure and magnetism in actinide compounds

    Energy Technology Data Exchange (ETDEWEB)

    Durakiewicz, T. [Los Alamos National Laboratory, Los Alamos, NM 87545 (United States)]. E-mail: tomasz@lanl.gov; Joyce, J.J. [Los Alamos National Laboratory, Los Alamos, NM 87545 (United States); Lander, G.H. [JRC, Institute of Transuranium Elements, Postfach 2340, 76125 Karlsruhe (Germany); Olson, C.G. [Ames Laboratory, Iowa State University, Ames, Iowa 5011 (United States); Butterfield, M.T. [Lawrence Livermoore National Laboratory, Livermoore, CA 94550 (United States); Guziewicz, E. [Institute of Physics, Polish Academy of Sciences, 02-668 Warsaw (Poland); Batista, C.D. [Los Alamos National Laboratory, Los Alamos, NM 87545 (United States); Arko, A.J. [Los Alamos National Laboratory, Los Alamos, NM 87545 (United States); Morales, L. [Los Alamos National Laboratory, Los Alamos, NM 87545 (United States); Mattenberger, K. [Laboratorium fur Festkorperphysik, ETH, CH-8093, Zurich (Switzerland); Vogt, O. [Laboratorium fur Festkorperphysik, ETH, CH-8093, Zurich (Switzerland)

    2006-05-01

    A close relationship between electronic structure and magnetic properties is observed in actinide compounds. The exact nature of this relationship is under investigation. We present examples of a direct link between electronic structure and ordered magnetic moment and/or magnetization. Specifically, results obtained for cubic U, Np and Pu compounds and quasi-2D U compounds are be presented. In the case of cubic compounds, a direct relationship between binding energy of valence band features and magnetic moment will be discussed. A Stoner-like mechanism and simple mean-field explanation is proposed for ferromagnetic UTe.

  16. Calculated Bulk Properties of the Actinide Metals

    DEFF Research Database (Denmark)

    Skriver, Hans Lomholt; Andersen, O. K.; Johansson, B.

    1978-01-01

    Self-consistent relativistic calculations of the electronic properties for seven actinides (Ac-Am) have been performed using the linear muffin-tin orbitals method within the atomic-sphere approximation. Exchange and correlation were included in the local spin-density scheme. The theory explains...... the variation of the atomic volume and the bulk modulus through the 5f series in terms of an increasing 5f binding up to plutonium followed by a sudden localisation (through complete spin polarisation) in americium...

  17. Fission cross section measurements for minor actinides

    Energy Technology Data Exchange (ETDEWEB)

    Fursov, B. [IPPE, Obninsk (Russian Federation)

    1997-03-01

    The main task of this work is the measurement of fast neutron induced fission cross section for minor actinides of {sup 238}Pu, {sup 242m}Am, {sup 243,244,245,246,247,248}Cm. The task of the work is to increase the accuracy of data in MeV energy region. Basic experimental method, fissile samples, fission detectors and electronics, track detectors, alpha counting, neutron generation, fission rate measurement, corrections to the data and error analysis are presented in this paper. (author)

  18. Potentiometric Sensor for Real-Time Remote Surveillance of Actinides in Molten Salts

    Energy Technology Data Exchange (ETDEWEB)

    Natalie J. Gese; Jan-Fong Jue; Brenda E. Serrano; Guy L. Fredrickson

    2012-07-01

    A potentiometric sensor is being developed at the Idaho National Laboratory for real-time remote surveillance of actinides during electrorefining of spent nuclear fuel. During electrorefining, fuel in metallic form is oxidized at the anode while refined uranium metal is reduced at the cathode in a high temperature electrochemical cell containing LiCl-KCl-UCl3 electrolyte. Actinides present in the fuel chemically react with UCl3 and form stable metal chlorides that accumulate in the electrolyte. This sensor will be used for process control and safeguarding of activities in the electrorefiner by monitoring the concentrations of actinides in the electrolyte. The work presented focuses on developing a solid-state cation conducting ceramic sensor for detecting varying concentrations of trivalent actinide metal cations in eutectic LiCl-KCl molten salt. To understand the basic mechanisms for actinide sensor applications in molten salts, gadolinium was used as a surrogate for actinides. The ß?-Al2O3 was selected as the solid-state electrolyte for sensor fabrication based on cationic conductivity and other factors. In the present work Gd3+-ß?-Al2O3 was prepared by ion exchange reactions between trivalent Gd3+ from GdCl3 and K+-, Na+-, and Sr2+-ß?-Al2O3 precursors. Scanning electron microscopy (SEM) was used for characterization of Gd3+-ß?-Al2O3 samples. Microfocus X-ray Diffraction (µ-XRD) was used in conjunction with SEM energy dispersive X-ray spectroscopy (EDS) to identify phase content and elemental composition. The Gd3+-ß?-Al2O3 materials were tested for mechanical and chemical stability by exposing them to molten LiCl-KCl based salts. The effect of annealing on the exchanged material was studied to determine improvements in material integrity post ion exchange. The stability of the ß?-Al2O3 phase after annealing was verified by µ-XRD. Preliminary sensor tests with different assembly designs will also be presented.

  19. Actinide Solubility and Speciation in the WIPP

    Energy Technology Data Exchange (ETDEWEB)

    Reed, Donald T. [Los Alamos National Laboratory

    2015-11-02

    The presentation begins with the role and need for nuclear repositories (overall concept, international updates (Sweden, Finland, France, China), US approach and current status), then moves on to the WIPP TRU repository concept (design, current status--safety incidents of February 5 and 14, 2014, path forward), and finally considers the WIPP safety case: dissolved actinide concentrations (overall approach, oxidation state distribution and redox control, solubility of actinides, colloidal contribution and microbial effects). The following conclusions are set forth: (1) International programs are moving forward, but at a very slow and somewhat sporadic pace. (2) In the United States, the Salt repository concept, from the perspective of the long-term safety case, remains a viable option for nuclear waste management despite the current operational issues/concerns. (3) Current model/PA prediction (WIPP example) are built on redundant conservatisms. These conservatisms are being addressed in the ongoing and future research to fill existing data gaps--redox control of plutonium by Fe(0, II), thorium (analog) solubility studies in simulated brine, contribution of intrinsic and biocolloids to the mobile concentration, and clarification of microbial ecology and effects.

  20. Thin extractive membrane for monitoring actinides in aqueous streams.

    Science.gov (United States)

    Chavan, Vivek; Paul, Sumana; Pandey, Ashok K; Kalsi, P C; Goswami, A

    2013-09-15

    Alpha spectrometry and solid state nuclear track detectors (SSNTDs) are used for monitoring ultra-trace amount of alpha emitting actinides in different aqueous streams. However, these techniques have limitations i.e. alpha spectrometry requires a preconcentration step and SSNTDs are not chemically selective. Therefore, a thin polymer inclusion membrane (PIM) supported on silanized glass was developed for preconcentraion and determination of ultra-trace concentration of actinides by α-spectrometry and SSNTDs. PIMs were formed by spin coating on hydrophobic glass slide or solvent casting to form thin and self-supported membranes, respectively. Sorption experiments indicated that uptakes of actinides in the PIM were highly dependent on acidity of solution i.e. Am(III) sorbed up to 0.1 molL(-1) HNO₃, U(VI) up to 0.5 molL(-1) HNO₃ and Pu(IV) from HNO₃ concentration as high as 4 molL(-1). A scheme was developed for selective sorption of target actinide in the PIM by adjusting acidity and oxidation state of actinide. The actinides sorbed in PIMs were quantified by alpha spectrometry and SSNTDs. For SSNTDs, neutron induced fission-fragment tracks and α-particle tracks were registered in Garware polyester and CR-39 for quantifications of natural uranium and α-emitting actinides ((241)Am/(239)Pu/(233)U), respectively. Finally, the membranes were tested to quantify Pu in 4 molL(-1) HNO3 solutions and synthetic urine samples.

  1. Separation of actinides from spent nuclear fuel: A review.

    Science.gov (United States)

    Veliscek-Carolan, Jessica

    2016-11-15

    This review summarises the methods currently available to extract radioactive actinide elements from solutions of spent nuclear fuel. This separation of actinides reduces the hazards associated with spent nuclear fuel, such as its radiotoxicity, volume and the amount of time required for its' radioactivity to return to naturally occurring levels. Separation of actinides from environmental water systems is also briefly discussed. The actinide elements typically found in spent nuclear fuel include uranium, plutonium and the minor actinides (americium, neptunium and curium). Separation methods for uranium and plutonium are reasonably well established. On the other hand separation of the minor actinides from lanthanide fission products also present in spent nuclear fuel is an ongoing challenge and an area of active research. Several separation methods for selective removal of these actinides from spent nuclear fuel will be described. These separation methods include solvent extraction, which is the most commonly used method for radiochemical separations, as well as the less developed but promising use of adsorption and ion-exchange materials.

  2. End point control of an actinide precipitation reactor

    Energy Technology Data Exchange (ETDEWEB)

    Muske, K.R. [Villanova Univ., PA (United States). Dept. of Chemical Engineering; Palmer, M.J. [Los Alamos National Lab., NM (United States)

    1997-10-01

    The actinide precipitation reactors in the nuclear materials processing facility at Los Alamos National Laboratory are used to remove actinides and other heavy metals from the effluent streams generated during the purification of plutonium. These effluent streams consist of hydrochloric acid solutions, ranging from one to five molar in concentration, in which actinides and other metals are dissolved. The actinides present are plutonium and americium. Typical actinide loadings range from one to five grams per liter. The most prevalent heavy metals are iron, chromium, and nickel that are due to stainless steel. Removal of these metals from solution is accomplished by hydroxide precipitation during the neutralization of the effluent. An end point control algorithm for the semi-batch actinide precipitation reactors at Los Alamos National Laboratory is described. The algorithm is based on an equilibrium solubility model of the chemical species in solution. This model is used to predict the amount of base hydroxide necessary to reach the end point of the actinide precipitation reaction. The model parameters are updated by on-line pH measurements.

  3. A systematic study of actinide production from the interactions of heavy ions with sup 248 Cm

    Energy Technology Data Exchange (ETDEWEB)

    Leyba, J.D.

    1990-09-07

    Production cross sections for heavy actinides produced from the interactions of {sup 12}C, {sup 31}P, {sup 40}Ar, and {sup 44}Ca ions with {sup 248}Cm were measured at energies ranging from 0.98 to 1.35 X Coulomb barrier. The recoiling reaction products were collected in copper or gold catcher foils located near the {sup 248}Cm target. Separate fractions of Bk, Cf, Es, Fm, and Md were obtained from a radiochemical separation procedure. For the {sup 12}C system, a He/KCl jet was used to transport the recoiling No activities of interest to a rotating wheel system. The isotopic distributions of the actinide products were found to be essentially symmetric about the maximum with full-widths-at-half-maximum of approximately 2.5 mass units. Isotopic distributions of the {sup 12}C, {sup 31}P, {sup 40}Ar, and {sup 44}Ca systems were found to be very similar to the {sup 40,48}Ca systems studied previously. The maxima of the isotopic distributions generally occurred for those reaction channels which involved the exchange of the fewest number of nucleons between the target and projectile for which the calculated excitation energy was a positive quantity. Additionally, the maxima of the excitation functions occurred at those projectile energies which were consistent with the calculated reaction barriers based upon a binary reaction mechanism. The experimental data from the four systems investigated were compared to several models of heavy ion interactions including a damped reaction mechanism, compound nucleus formation and subsequent particle evaporation, and classical partial wave calculations for binary systems.

  4. Separating the Minor Actinides Through Advances in Selective Coordination Chemistry

    Energy Technology Data Exchange (ETDEWEB)

    Lumetta, Gregg J.; Braley, Jenifer C.; Sinkov, Sergey I.; Carter, Jennifer C.

    2012-08-22

    This report describes work conducted at the Pacific Northwest National Laboratory (PNNL) in Fiscal Year (FY) 2012 under the auspices of the Sigma Team for Minor Actinide Separation, funded by the U.S. Department of Energy Office of Nuclear Energy. Researchers at PNNL and Argonne National Laboratory (ANL) are investigating a simplified solvent extraction system for providing a single-step process to separate the minor actinide elements from acidic high-level liquid waste (HLW), including separating the minor actinides from the lanthanide fission products.

  5. Distribution of actinides in SFR1; Aktinidfoerdelning i SFR1

    Energy Technology Data Exchange (ETDEWEB)

    Ingemansson, Tor [ALARA Engineering, Skultuna (Sweden)

    2000-02-01

    The amount of actinides in the Swedish repository for intermediate level radioactive wastes has been estimated. The sources for the actinides are mainly the purification filters of the reactors and the used fuel pools. Defect fuel elements are the originating source of the actinides. It is estimated that the 12 Swedish reactors, in total, have had 2.2 kg of fuel dissolved in their systems since start-up. About 880 g of this amount has been brought to the intermediate-level repository.

  6. Self-interaction corrected local spin density calculations of actinides

    DEFF Research Database (Denmark)

    Petit, Leon; Svane, Axel; Szotek, Z

    2010-01-01

    We use the self-interaction corrected local spin-density approximation in order to describe localization-delocalization phenomena in the strongly correlated actinide materials. Based on total energy considerations, the methodology enables us to predict the ground-state valency configuration...... of the actinide ions in these compounds from first principles. Here we review a number of applications, ranging from electronic structure calculations of actinide metals, nitrides and carbides to the behaviour under pressure of intermetallics, and O vacancies in PuO2....

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

    Energy Technology Data Exchange (ETDEWEB)

    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.

  8. Principle and Uncertainty Quantification of an Experiment Designed to Infer Actinide Neutron Capture Cross-Sections

    Energy Technology Data Exchange (ETDEWEB)

    G. Youinou; G. Palmiotti; M. Salvatorre; G. Imel; R. Pardo; F. Kondev; M. Paul

    2010-01-01

    An integral reactor physics experiment devoted to infer higher actinide (Am, Cm, Bk, Cf) neutron cross sections will take place in the US. This report presents the principle of the planned experiment as well as a first exercise aiming at quantifying the uncertainties related to the inferred quantities. It has been funded in part by the DOE Office of Science in the framework of the Recovery Act and has been given the name MANTRA for Measurement of Actinides Neutron TRAnsmutation. The principle is to irradiate different pure actinide samples in a test reactor like INL’s Advanced Test Reactor, and, after a given time, determine the amount of the different transmutation products. The precise characterization of the nuclide densities before and after neutron irradiation allows the energy integrated neutron cross-sections to be inferred since the relation between the two are the well-known neutron-induced transmutation equations. This approach has been used in the past and the principal novelty of this experiment is that the atom densities of the different transmutation products will be determined with the Accelerator Mass Spectroscopy (AMS) facility located at ANL. While AMS facilities traditionally have been limited to the assay of low-to-medium atomic mass materials, i.e., A < 100, there has been recent progress in extending AMS to heavier isotopes – even to A > 200. The detection limit of AMS being orders of magnitude lower than that of standard mass spectroscopy techniques, more transmutation products could be measured and, potentially, more cross-sections could be inferred from the irradiation of a single sample. Furthermore, measurements will be carried out at the INL using more standard methods in order to have another set of totally uncorrelated information.

  9. Stability of artificial ferrite garnets with actinides and lanthanoids in water solutions

    Science.gov (United States)

    Livshits, T. S.

    2008-12-01

    Extraction of the actinide-REE fraction and its subsequent incorporation into sparingly soluble crystalline phases (confinement matrices) is assumed in processing of spent nuclear fuel from high-level radioactive wastes (HLW). The chemical stability in the process of interaction with subsurface water governs the capability of a matrix phase to keep radionuclides from getting into the biosphere. In static experiments at 90 and 150°C, the chemical stability of ferrite garnets was investigated for three compositions with Th4+, Ce4+ and Gd3+ + serving as simulator components of the actinide fraction of HLW. Experiments were carried out in distilled water (pH 6.5), 0.01 M HCl solution (pH 2), and 0.01 M NaOH solution (pH 12). The behavior of ferrigarnet matrices depends on the acidity of the solution. In neutral and alkaline media, Th, Ce, and Gd are virtually not transferred into the liquid phase. Acid leaching promotes intense dissolution of garnet matrices. In this case, the leaching rate of Gd and Th from ceramics into the liquid phase is two orders of magnitude lower than the leaching rate of Ce because the Ce-doped phases contain less stable (relative to garnet) Ce-rich perovskite. Amorphization of the ferrigarnet structure due to 244Cm isotope decay leads to an increase in the leaching rate of Cm by no more than five times. In terms of radiation and chemical stability, ferrite garnets are not inferior to zirconolites and titanate pyrochlores. The experimental results suggest that garnet matrices can reliably immobilize actinides in subsurface repositories.

  10. Isotopic composition of H2 from wood burning: Dependency on combustion efficiency, moisture content, and δD of local precipitation

    NARCIS (Netherlands)

    Röckmann, T.; Gómez Álvarez, C.X.; Walter, S.; van der Veen, C.; Wollny, A.G.; Gunthe, S.S.; Helas, G.; Pöschl, U.; Keppler, F.; Greule, M.; Brand, W.A.

    2010-01-01

    Differences in isotopic composition between the various sources of H2 are large, but only a few measurements have been carried out to constrain them. Two conflicting values have been published for H2 from biomass burning. Both rely on the assumption that the isotopic composition of H2 should scale w

  11. Solidification of simulated actinides by natural zircon

    Institute of Scientific and Technical Information of China (English)

    YANG Jian-Wen; LUO Shang-Geng

    2004-01-01

    Natural zircon was used as precursor material to produce a zircon waste form bearing 20wt% simulated actinides (Nd2O3 and UO2) through a solid state reaction by a typical synroc fabrication process. The fabricated zircon waste form has relatively good physical properties (density 5.09g/cm3, open porosity 4.0%, Vickers hardness 715kg/mm2). The XRD, SEM/EDS and TEM/EDS analyses indicate that there are zircon phases containing waste elements formed through the reaction. The chemical durability and radiation stability are determined by the MCC-1method and heavy ion irradiation; the results show that the zircon waste form is highly leach resistance and relatively stable under irradiation (amorphous dose 0.7dpa). From this study, the method of using a natural mineral to solidify radioactive waste has proven to be feasible.

  12. Factors affecting the placental transfer of actinides

    Energy Technology Data Exchange (ETDEWEB)

    Sikov, M.R.; Kelman, B.J. (Pacific Northwest Laboratory, Richland, WA (USA))

    1989-01-01

    The primary goal of this paper is to consider factors that affect the availability and transport of actinides from maternal blood, through the placenta, to the conceptus. These factors, of particular importance in scaling results from animals to man, include the route and temporal pattern of administration, the mass and physicochemical state of material administered, metabolism of the pregnant animal and fetal organs or tissue, and species-specific changes in placental structure relative to stage of gestation at exposure. Preliminary concepts for descriptive and kinetic models are proposed to integrate these results, to identify additional information required for developing more comprehensive models, and to provide a basis for scaling to human pregnancies for purposes of radiation dosimetry.

  13. Pyrometallurgical processes for recovery of actinide elements

    Energy Technology Data Exchange (ETDEWEB)

    Battles, J.E.; Laidler, J.J.; McPheeters, C.C.; Miller, W.E.

    1994-01-01

    A metallic fuel alloy, nominally U-20-Pu-lOZr, is the key element of the Integral Fast Reactor (IFR) fuel cycle. Metallic fuel permits the use of an innovative, simple pyrometallurgical process, known as pyroprocessing, (the subject of this report), which features fused salt electrorefining of the spent fuel. Electrorefining separates the actinide elements from fission products, without producing a separate stream of plutonium. The plutonium-bearing product is contaminated with higher actinides and with a minor amount of rare earth fission products, making it diversion resistant while still suitable as a fuel material in the fast spectrum of the IFR core. The engineering-scale demonstration of this process will be conducted in the refurbished EBR-II Fuel Cycle Facility, which has entered the start-up phase. An additional pyrometallurgical process is under development for extracting transuranic (TRU) elements from Light Water Reactor (LWR) spent fuel in a form suitable for use as a feed to the IFR fuel cycle. Four candidate extraction processes have been investigated and shown to be chemically feasible. The main steps in each process are oxide reduction with calcium or lithium, regeneration of the reductant and recycle of the salt, and separation of the TRU product from the bulk uranium. Two processes, referred to as the lithium and salt transport (calcium reductant) processes, have been selected for engineering-scale demonstration, which is expected to start in late 1993. An integral part of pyroprocessing development is the treatment and packaging of high-level waste materials arising from the operations, along with the qualification of these waste forms for disposal in a geologic repository.

  14. Studies of actinides in a superanoxic fjord

    Energy Technology Data Exchange (ETDEWEB)

    Roos, P.

    1997-04-01

    Water column and sediment profiles of Pu, Am, Th and U have been obtained in the superanoxic Framvaren fjord, southern Norway. The concentration of bomb test fallout Pu, Am as well as `dissolved` Th in the bottom water are the highest recorded in the marine environment. The behaviour of the actinides in the anoxic water mass is to a large extent governed by the behaviour of the colloidal material. Ultrafiltration reveals that 40-60% of the actinides are associated to the large colloids, surprisingly this is valid also for U. The sediment acts as a source for Pu, Am, and Th to the water column but primarily as a sink for U. The remobilization of Pu, Am and Th is evident from the water column profiles which have similar diffusion shape profiles as other constituents originating from the sediments. The vertical eddy diffusion coefficient calculated from the Pu profile is in the same order of magnitude as reported from the H{sub 2}S profile. Decreased bottom water concentrations (but a constant water column inventory) between 1989 and 1995 as well as pore water Pu concentrations nearly identical to the overlaying bottom water indicates that the present Pu flux from the sediments are low. Contrary to Pu and Am, the water column Th inventory ({sup 232}Th and {sup 230}Th) continues to increase. The flux of {sup 232}Th from the sediments was determined from changes in water column inventory between 1989 and 1995 and from a pore water profile to be in the order of 2-8 Bq/m{sup 2}/y. 208 refs.

  15. Element Partitioning in Glass-Ceramic Designed for Actinides Immobilization

    Institute of Scientific and Technical Information of China (English)

    2008-01-01

    <正>Glass-ceramics were designed for immobilization of actinides. In order to immobilizing more wastes in the matrix and to develop the optimum formulation for the glass-ceramic, it is necessary to study the

  16. Advanced techniques for actinide spectroscopy (ATAS 2012). Abstract book

    Energy Technology Data Exchange (ETDEWEB)

    Foerstendorf, Harald; Mueller, Katharina; Steudtner, Robin (eds.)

    2012-07-01

    The abstract book of the International workshop on advanced techniques for actinide spectroscopy (ATAS 2012) include contributions concerning the following issues: environmental applications, NMR spectroscopy, vibrational spectroscopy, X-ray spectroscopy and theory, technical application: separation processes, emission spectroscopy.

  17. Lipid biomarkers for anaerobic oxidation of methane and sulphate reduction in cold seep sediments of Nyegga pockmarks (Norwegian margin): discrepancies in contents and carbon isotope signatures

    Science.gov (United States)

    Chevalier, Nicolas; Bouloubassi, Ioanna; Stadnitskaia, Alina; Taphanel, Marie-Hélène; Sinninghe Damsté, Jaap S.

    2014-06-01

    Distributions and carbon isotopic compositions of microbial lipid biomarkers were investigated in sediment cores from the G11 and G12 pockmarks in the Nyegga sector of the Storegga Slide on the mid-Norwegian margin to explore differences in depth zonation, type and carbon assimilation mode of anaerobic methane-oxidizing archaea (ANMEs) and associated sulphate-reducing bacteria responsible for anaerobic oxidation of methane (AOM) in these cold seep environments. While the G11 site is characterised by black reduced sediments colonized by gastropods and Siboglinidae tubeworms, the G12 site has black reduced sediments devoid of fauna but surrounded by a peripheral occurrence of gastropods and white filamentous microbial mats. At both sites, bulk sediments contained abundant archaeal and bacterial lipid biomarkers substantially depleted in 13C, consisting mainly of isoprenoidal hydrocarbons and dialkyl glycerol diethers, fatty acids and non-isoprenoidal monoalkylglycerol ethers. At the G11 site, down-core profiles revealed that lipid biomarkers were in maximum abundance from 10 cm depth to the core bottom at 16 cm depth, associated with δ13C values of -57 to -136‰. At the G12 site, by contrast, lipid biomarkers were in high abundance in the upper 5 cm sediment layer, associated with δ13C values of -43 to -133‰. This suggests that, as expected from the benthic fauna characteristics of the sites, AOM takes place mainly at depth in the G11 pockmark but just below the seafloor in the G12 pockmark. These patterns can be explained largely by variable fluid flow rates. Furthermore, at both sites, a dominance of ANME-2 archaea accompanied by their bacterial partners is inferred based on lipid biomarker distributions and carbon isotope signatures, which is in agreement with recently published DNA analyses for the G11 pockmark. However, the present data reveal high discrepancies in the contents and δ13C values for both archaeal and bacterial lipid profiles, implying the

  18. Radio-ecological researches in the Sea of Japan and northwestern part of the Pacific Ocean after accident on the Japanese nuclear power plant 'Fukushima-1': the content of plutonium isotopes and strontium-90 in sea water

    Energy Technology Data Exchange (ETDEWEB)

    Fedorova, A. [Research and Production Association - RPA Typhoon (Russian Federation)

    2014-07-01

    In April-May 2011 and in August-September 2012 'Roshydromet' has conducted radio ecological researches in the Sea of Japan and on the water area of northwestern part of the Pacific Ocean (Kuril-Kamchatka area and the area of the Kuroshio current), which had purpose to make assessment of contamination hazard that can be caused to the coast of Russian Far East because of emergency releases of radioactive materials on the nuclear power plant 'Fukushima-1'. During the research works was done the sampling and processing of sea water samples not only for detection of Cs{sup 134}, Cs{sup 137}, but also for such radio-ecological significant long-living radionuclides, as {sup 90}Sr, plutonium isotopes ({sup 239,240}Pu) and tritium. Information about radionuclides was required for correct assessment of nuclear power plant 'Fukushima-1' aftermath on the Far Eastern sea water areas, but was not available in the beginning of research. In the present report the radiochemical measuring results on content of plutonium isotopes and {sup 90}Sr in the sea water from researched areas are presented. Sampling was done from the various horizons. Surface and deep water samples were filtered via the compound filter which made it possible to filter particles bigger than 1 micron. Radiochemical testing of the {sup 90}Sr and plutonium isotopes content was done separately on a suspension and in a filtrate of sea water samples. The content of {sup 90}Sr in the filtrate of the sea water that had been selected in 2011, ranges 0,7-2,4 Bq/m{sup 3}, in suspensions the interval makes 0,0013-0,021 Bq/m3. The results received in researches in 2012 are in range of 0,5-2,6 Bq/m{sup 3} of the sea water filtrate. According to results of IAEA in 2000, the average content of {sup 90}Sr in surface water of the Sea of Japan made 1,6 Bq/m{sup 3}. Hereby, the data obtained in researches in 2011-2012 agrees with results which had been presented by IAEA before the accident. The

  19. Analysis of the Gas Core Actinide Transmutation Reactor (GCATR)

    Science.gov (United States)

    Clement, J. D.; Rust, J. H.

    1977-01-01

    Design power plant studies were carried out for two applications of the plasma core reactor: (1) As a breeder reactor, (2) As a reactor able to transmute actinides effectively. In addition to the above applications the reactor produced electrical power with a high efficiency. A reactor subsystem was designed for each of the two applications. For the breeder reactor, neutronics calculations were carried out for a U-233 plasma core with a molten salt breeding blanket. A reactor was designed with a low critical mass (less than a few hundred kilograms U-233) and a breeding ratio of 1.01. The plasma core actinide transmutation reactor was designed to transmute the nuclear waste from conventional LWR's. The spent fuel is reprocessed during which 100% of Np, Am, Cm, and higher actinides are separated from the other components. These actinides are then manufactured as oxides into zirconium clad fuel rods and charged as fuel assemblies in the reflector region of the plasma core actinide transmutation reactor. In the equilibrium cycle, about 7% of the actinides are directly fissioned away, while about 31% are removed by reprocessing.

  20. Isotope and Nuclear Chemistry Division annual report, FY 1983

    Energy Technology Data Exchange (ETDEWEB)

    Heiken, J.H.; Lindberg, H.A. (eds.)

    1984-05-01

    This report describes progress in the major research and development programs carried out in FY 1983 by the Isotope and Nuclear Chemistry Division. It covers radiochemical diagnostics of weapons tests; weapons radiochemical diagnostics research and development; other unclassified weapons research; stable and radioactive isotope production, separation, and applications (including biomedical applications); element and isotope transport and fixation; actinide and transition metal chemistry; structural chemistry, spectroscopy, and applications; nuclear structure and reactions; irradiation facilities; advanced analytical techniques; development and applications; atmospheric chemistry and transport; and earth and planetary processes.

  1. Hardening neutron spectrum for advanced actinide transmutation experiments in the ATR.

    Science.gov (United States)

    Chang, G S; Ambrosek, R G

    2005-01-01

    The most effective method for transmuting long-lived isotopes contained in spent nuclear fuel into shorter-lived fission products is in a fast neutron spectrum reactor. In the absence of a fast test reactor in the United States, initial irradiation testing of candidate fuels can be performed in a thermal test reactor that has been modified to produce a test region with a hardened neutron spectrum. Such a test facility, with a spectrum similar but somewhat softer than that of the liquid-metal fast breeder reactor (LMFBR), has been constructed in the INEEL's Advanced Test Reactor (ATR). The radial fission power distribution of the actinide fuel pin, which is an important parameter in fission gas release modelling, needs to be accurately predicted and the hardened neutron spectrum in the ATR and the LMFBR fast neutron spectrum is compared. The comparison analyses in this study are performed using MCWO, a well-developed tool that couples the Monte Carlo transport code MCNP with the isotope depletion and build-up code ORIGEN-2. MCWO analysis yields time-dependent and neutron-spectrum-dependent minor actinide and Pu concentrations and detailed radial fission power profile calculations for a typical fast reactor (LMFBR) neutron spectrum and the hardened neutron spectrum test region in the ATR. The MCWO-calculated results indicate that the cadmium basket used in the advanced fuel test assembly in the ATR can effectively depress the linear heat generation rate in the experimental fuels and harden the neutron spectrum in the test region.

  2. Radioactive Ion Beam Production by Fast-Neutron-Induced Fission in Actinide Targets at EURISOL

    CERN Document Server

    Herrera-Martínez, Adonai

    The European Isotope Separation On-Line Radioactive Ion Beam Facility (EURISOL) is set to be the 'next-generation' European Isotope Separation On-Line (ISOL) Radioactive Ion Beam (RIB) facility. It will extend and amplify current research on nuclear physics, nuclear astrophysics and fundamental interactions beyond the year 2010. In EURISOL, the production of high-intensity RIBs of specific neutron-rich isotopes is obtained by inducing fission in large-mass actinide targets. In our contribution, the use of uranium targets is shown to be advantageous to other materials, such as thorium. Therefore, in order to produce fissions in U-238 and reduce the plutonium inventory, a fast neutron energy spectrum is necessary. The large beam power required to achieve these RIB levels requires the use of a liquid proton-to-neutron converter. This article details the design parameters of the converter, with special attention to the coupled neutronics of the liquid converter and fission target. Calculations performed with the ...

  3. Measurement of fission cross-section of actinides at n_TOF for advanced nuclear reactors

    CERN Document Server

    Calviani, Marco; Montagnoli, G; Mastinu, P

    2009-01-01

    The subject of this thesis is the determination of high accuracy neutron-induced fission cross-sections of various isotopes - all of which radioactive - of interest for emerging nuclear technologies. The measurements had been performed at the CERN neutron time-of-flight facility n TOF. In particular, in this work, fission cross-sections on 233U, the main fissile isotope of the Th/U fuel cycle, and on the minor actinides 241Am, 243Am and 245Cm have been analyzed. Data on these isotopes are requested for the feasibility study of innovative nuclear systems (ADS and Generation IV reactors) currently being considered for energy production and radioactive waste transmutation. The measurements have been performed with a high performance Fast Ionization Chamber (FIC), in conjunction with an innovative data acquisition system based on Flash-ADCs. The first step in the analysis has been the reconstruction of the digitized signals, in order to extract the information required for the discrimination between fission fragm...

  4. Selective Separation of Trivalent Actinides from Lanthanides by Aqueous Processing with Introduction of Soft Donor Atoms

    Energy Technology Data Exchange (ETDEWEB)

    Kenneth L. Nash

    2009-09-22

    Implementation of a closed loop nuclear fuel cycle requires the utilization of Pu-containing MOX fuels with the important side effect of increased production of the transplutonium actinides, most importantly isotopes of Am and Cm. Because the presence of these isotopes significantly impacts the long-term radiotoxicity of high level waste, it is important that effective methods for their isolation and/or transmutation be developed. Furthermore, since transmutation is most efficiently done in the absence of lanthanide fission products (high yield species with large thermal neutron absorption cross sections) it is important to have efficient procedures for the mutual separation of Am and Cm from the lanthanides. The chemistries of these elements are nearly identical, differing only in the slightly stronger strength of interaction of trivalent actinides with ligand donor atoms softer than O (N, Cl-, S). Research being conducted around the world has led to the development of new reagents and processes with considerable potential for this task. However, pilot scale testing of these reagents and processes has demonstrated the susceptibility of the new classes of reagents to radiolytic and hydrolytic degradation. In this project, separations of trivalent actinides from fission product lanthanides have been investigated in studies of 1) the extraction and chemical stability properties of a class of soft-donor extractants that are adapted from water-soluble analogs, 2) the application of water soluble soft-donor complexing agents in tandem with conventional extractant molecules emphasizing fundamental studies of the TALSPEAK Process. This research was conducted principally in radiochemistry laboratories at Washington State University. Collaborators at the Radiological Processing Laboratory (RPL) at the Pacific Northwest National Laboratory (PNNL) have contributed their unique facilities and capabilities, and have supported student internships at PNNL to broaden their

  5. Reconstructions of the heliospheric modulation potential and Wolf numbers based on the content of the 14C isotope in tree rings during the Maunder and Spörer minimums

    Science.gov (United States)

    Kudryavtsev, I. V.; Dergachev, V. A.; Kuleshova, A. I.; Nagovitsyn, Yu. A.; Ogurtsov, M. G.

    2016-12-01

    Data on variations in the content of the 14C cosmogenic isotope in tree rings and the Earth's atmosphere (Δ14C) make it possible to study the behavior of solar activity (SA) in previous centuries and millenniums. The latter is related to the fact that SA temporal variations result in a change in the IMF (Interplanetary Magnetic Field) parameters and, as a consequence, in the galactic cosmic ray (GCR) flux, under the action of which the 14C isotope is produced in the Earth's atmosphere. This makes it possible to study SA history based on data on the 14C isotope content in tree rings. However, in this case we have several difficulties related to climate change. Climate changes result in carbon redistribution between natural reservoirs, which is reflected in radiocarbon data and results in solar signal distortion. The effect of variations in the global temperature and carbon dioxide concentration on the reconstruction of the heliospheric modulation potential and Wolf numbers from the late 14th century to the early 19th century is considered. It has been shown that the radiocarbon data do not make it possible to conclude that SA during the Maunder minimum was extremely low as compared to SA during the Dalton minimum.

  6. Electrochemical decontamination system for actinide processing gloveboxes

    Energy Technology Data Exchange (ETDEWEB)

    Wedman, D.E.; Lugo, J.L.; Ford, D.K.; Nelson, T.O.; Trujillo, V.L.; Martinez, H.E.

    1998-03-01

    An electrolytic decontamination technology has been developed and successfully demonstrated at Los Alamos National Laboratory (LANL) for the decontamination of actinide processing gloveboxes. The technique decontaminates the interior surfaces of stainless steel gloveboxes utilizing a process similar to electropolishing. The decontamination device is compact and transportable allowing it to be placed entirely within the glovebox line. In this way, decontamination does not require the operator to wear any additional personal protective equipment and there is no need for additional air handling or containment systems. Decontamination prior to glovebox decommissioning reduces the potential for worker exposure and environmental releases during the decommissioning, transport, and size reduction procedures which follow. The goal of this effort is to reduce contamination levels of alpha emitting nuclides for a resultant reduction in waste level category from High Level Transuranic (TRU) to low Specific Activity (LSA, less than or equal 100 nCi/g). This reduction in category results in a 95% reduction in disposal and disposition costs for the decontaminated gloveboxes. The resulting contamination levels following decontamination by this method are generally five orders of magnitude below the LSA specification. Additionally, the sodium sulfate based electrolyte utilized in the process is fully recyclable which results in the minimum of secondary waste. The process bas been implemented on seven gloveboxes within LANL`s Plutonium Facility at Technical Area 55. Of these gloveboxes, two have been discarded as low level waste items and the remaining five have been reused.

  7. Photofission of actinide and pre-actinide nuclei in the quasideuteron and delta energy regions

    CERN Document Server

    Berman, B L; Cole, P L; Dodge, W R; Feldman, G; Sanabria, J C; Kolb, N; Pywell, R E; Vogt, J; Nedorezov, V; Sudov, A; Kezerashvili, G Ya

    1999-01-01

    The photofission cross sections for the actinide nuclei sup 2 sup 3 sup 2 Th, sup 2 sup 3 sup 3 sup , sup 2 sup 3 sup 5 sup , sup 2 sup 3 sup 8 U, and sup 2 sup 3 sup 7 Np have been measured from 68 to 264 MeV and those for the pre-actinide nuclei sup 1 sup 9 sup 7 Au and sup N sup A sup T Pb from 122 to 222 MeV at the Saskatchewan Accelerator Laboratory, using monoenergetic tagged photons and novel parallel-plate avalanche detectors for the fission fragments. The aim of the experiment was to obtain a comprehensive and self-consistent data set and to investigate previous anomalous results in this energy region. The fission probability for transuranic nuclei is expected to be close to unity here. However, important discrepancies have been confirmed for sup 2 sup 3 sup 7 Np and sup 2 sup 3 sup 2 Th, compared with sup 2 sup 3 sup 8 U, which have serious implications for the inferred total photoabsorption strengths, and hence call into question the 'Universal Curve' for photon absorption at these energies. High-s...

  8. Studies on Neutron, Photon (Bremsstrahlung and Proton Induced Fission of Actinides and Pre-Actinides

    Directory of Open Access Journals (Sweden)

    H. Naik

    2015-08-01

    Full Text Available We present the yields of various fission products determined in the reactor neutron, 3.7-18.1 MeV quasi-mono energetic neutron, 8-80 MeV bremsstrahlung and 20-45 MeV proton induced fission of 232Th and 238U using radiochemical and off-line beta or gamma ray counting. The yields of the fission products in the bremsstrahlung induced fission natPb and 209Bi with 50- 70 MeV and 2.5 GeV based on off-line gamma ray spectrometric technique were also presented. From the yields of fission products, the mass chains yields were obtained using charge distribution correction. From the mass yield distribution, the peak-to-valley (P/V ratio was obtained. The role of excitation energy on the peak-to-valley ratio and fine structure such as effect of shell closure proximity and even-odd effect of mass yield distribution were examined. The higher yields of the fission products around A=133-134, 138-140 and 143-144 and their complementary products explained from the nuclear structure effect and role of standard I and II mode of asymmetric fission. In the neutron, photon (bremsstrahlung and proton induced fission, the asymmetric mass distribution for actinides (Th, U and symmetric distribution for pre-actinides (Pb, Bi were explained from different type of potential fission barrier

  9. Development of the Chalmers Grouped Actinide Extraction Process

    Directory of Open Access Journals (Sweden)

    Halleröd Jenny

    2015-12-01

    Full Text Available Several solvents for Grouped ActiNide EXtraction (GANEX processes have been investigated at Chalmers University of Technology in recent years. Four different GANEX solvents; cyclo-GANEX (CyMe4- -BTBP, 30 vol.% tri-butyl phosphate (TBP and cyclohexanone, DEHBA-GANEX (CyMe4-BTBP, 20 vol.% N,N-di-2(ethylhexyl butyramide (DEHBA and cyclohexanone, hexanol-GANEX (CyMe4-BTBP, 30 vol.% TBP and hexanol and FS-13-GANEX (CyMe4-BTBP, 30 vol.% TBP and phenyl trifluoromethyl sulfone (FS-13 have been studied and the results are discussed and compared in this work. The cyclohexanone based solvents show fast and high extraction of the actinides but a somewhat poor diluent stability in contact with the acidic aqueous phase. FS-13-GANEX display high separation factors between the actinides and lanthanides and a good radiolytic and hydrolytic stability. However, the distribution ratios of the actinides are lower, compared to the cyclohexanone based solvents. The hexanol-GANEX is a cheap solvent system using a rather stable diluent but the actinide extraction is, however, comparatively low.

  10. The actinides-a beautiful ending of the Periodic Table

    Energy Technology Data Exchange (ETDEWEB)

    Johansson, Boerje [Condensed Matter Theory Group, Department of Physics, Uppsala University, Box 530, S-751 21 Uppsala (Sweden); Applied Materials Physics, Department of Materials Science and Engineering, Royal Institute of Technology, Brinellvaegen 23, SE-100 44 Stockholm (Sweden)], E-mail: borje.johansson@fysik.uu.se; Li, Sa [Applied Materials Physics, Department of Materials Science and Engineering, Royal Institute of Technology, Brinellvaegen 23, SE-100 44 Stockholm (Sweden); Department of Physics, Virginia Commonwealth University, Richmond, VA 23284 (United States)

    2007-10-11

    The 5f elements, actinides, show many properties which have direct correspondence to the 4f transition metals, the lanthanides. The remarkable similarity between the solid state properties of compressed Ce and the actinide metals is pointed out in the present paper. The {alpha}-{gamma} transition in Ce is considered as a Mott transition, namely, from delocalized to localized 4f states. An analogous behavior is also found for the actinide series, where the sudden volume increase from Pu to Am can be viewed upon as a Mott transition within the 5f shell as a function of the atomic number Z. On the itinerant side of the Mott transition, the earlier actinides (Pa-Pu) show low symmetry structures at ambient conditions; while across the border, the heavier elements (Am-Cf) present the dhcp structure, an atomic arrangement typical for the trivalent lanthanide elements with localized 4f magnetic moments. The reason for an isostructural Mott transition of the f electron in Ce, as opposed to the much more complicated cases in the actinides, is identified. The strange appearance of the {delta}-phase (fcc) in the phase diagram of Pu is another consequence of the border line behavior of the 5f electrons. The path leading from {delta}-Pu to {alpha}-Pu is identified.

  11. Potential radiation dose from eating fish exposed to actinide contamination

    Energy Technology Data Exchange (ETDEWEB)

    Emery, R.M.; Klopfer, D.C.; Baker, D.A.; Soldat, J.K.

    1980-01-01

    The purpose of this work is to establish a maximum potential for transporting actinides to man via fish consumption. The study took place in U-Pond, a nuclear waste pond on the Hanford Site. It has concentrations of /sup 238/U, /sup 238/Pu, /sup 239,240/Pu and /sup 241/Am that are approximately three orders of magnitude greater than background levels. Fish living in the pond contain higher actinide concentrations than those observed in fish from any other location. Experiments were performed in U-pond to determine maximum quantities of actinides that could accumulate in fillets and whole bodies of two centrarchid fish species. Doses to hypothetical consumers were then estimated by assuming that actinide behavior in their bodies was similar to that defined for Standard Man by the International Commission on Radiological Protection. Results indicate that highest concentrations occurring in bluegill or bass muscle after more than a year's exposure to the pond would not be sufficient to produce a significant radiation dose to a human consumer, even if he ate 0.5 kg (approx.1 lb) of these fillets every day for 70 years. Natural predators (heron or coyote), having lifetime diets of whole fish from U-Pond, would receive less radiation dose from the ingested actinides than from natural background sources. 34 refs., 5 figs., 4 tabs.

  12. Hydrophilic actinide complexation studied by solvent extraction radiotracer technique

    Energy Technology Data Exchange (ETDEWEB)

    Rydberg, J. [Chalmers Univ. of Technology, Goeteborg (Sweden). Dept. of Nuclear Chemistry and Radiochemistry Consultant Group, Vaestra Froelunda (Sweden)

    1996-10-01

    Actinide migration in the ground water is enhanced by the formation of water soluble complexes. It is essential to the risk analysis of a wet repository to know the concentration of central atoms and the ligands in the ground water, and the stability of complexes formed between them. Because the chemical behavior at trace concentrations often differ from that at macro concentrations, it is important to know the chemical behavior of actinides at trace concentrations in ground water. One method used for such investigations is the solvent extraction radiotracer (SXRT) technique. This report describes the SXRT technique in some detail. A particular reason for this analysis is the claim that complex formation constants obtained by SXRT are less reliable than results obtained by other techniques. It is true that several difficulties are encountered in the application of SXRT technique to actinide solution, such as redox instability, hydrophilic complexation by side reactions and sorption, but it is also shown that a careful application of the SXRT technique yields results as reliable as by any other technique. The report contains a literature survey on solvent extraction studies of actinide complexes formed in aqueous solutions, particularly by using the organic reagent thenoyltrifluoroacetone (TTA) dissolved in benzene or chloroform. Hydrolysis constants obtained by solvent extraction are listed as well as all actinide complexes studied by SX with inorganic and organic ligands. 116 refs, 11 tabs.

  13. Isotopic signatures: An important tool in today`s world

    Energy Technology Data Exchange (ETDEWEB)

    Rokop, D.J.; Efurd, D.W.; Benjamin, T.M.; Cappis, J.H.; Chamberlin, J.W.; Poths, H.; Roensch, F.R.

    1995-12-01

    High-sensitivity/high-accuracy actinide measurement techniques developed to support weapons diagnostic capabilities at the Los Alamos National Laboratory are now being used for environmental monitoring. The measurement techniques used are Thermal Ionization Mass Spectrometry (TIMS), Alpha Spectrometry(AS), and High Resolution Gamma Spectrometry(HRGS). These techniques are used to address a wide variety of actinide inventory issues: Environmental surveillance, site characterizations, food chain member determination, sedimentary records of activities, and treaty compliance concerns. As little as 10 femtograms of plutonium can be detected in samples and isotopic signatures determined on samples containing sub-100 femtogram amounts. Uranium, present in all environmental samples, can generally yield isotopic signatures of anthropogenic origin when present at the 40 picogam/gram level. Solid samples (soils, sediments, fauna, and tissue) can range from a few particles to several kilograms in size. Water samples can range from a few milliliters to as much as 200 liters.

  14. Prompt Fission Neutron Spectra of Actinides

    Energy Technology Data Exchange (ETDEWEB)

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

    2016-01-01

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

  15. Actinide (III) solubility in WIPP Brine: data summary and recommendations

    Energy Technology Data Exchange (ETDEWEB)

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

    2009-09-01

    The solubility of actinides in the +3 oxidation state is an important input into the Waste Isolation Pilot Plant (WIPP) performance assessment (PA) models that calculate potential actinide release from the WIPP repository. In this context, the solubility of neodymium(III) was determined as a function of pH, carbonate concentration, and WIPP brine composition. Additionally, we conducted a literature review on the solubility of +3 actinides under WIPP-related conditions. Neodymium(III) was used as a redox-invariant analog for the +3 oxidation state of americium and plutonium, which is the oxidation state that accounts for over 90% of the potential release from the WIPP through the dissolved brine release (DBR) mechanism, based on current WIPP performance assessment assumptions. These solubility data extend past studies to brine compositions that are more WIPP-relevant and cover a broader range of experimental conditions than past studies.

  16. Lipid biomarkers for anaerobic oxidation of methane and sulphate reduction in cold seep sediments of Nyegga pockmarks (Norwegian margin): discrepancies in contents and carbon isotope signatures

    NARCIS (Netherlands)

    Chevalier, N.; Bouloubassi, I.; Stadnitskaia, A.; Taphanel, M.H.; Sinninghe Damsté, J.S.

    2014-01-01

    Distributions and carbon isotopic compositions of microbial lipid biomarkers were investigated in sediment cores from the G11 and G12 pockmarks in the Nyegga sector of the Storegga Slide on the mid-Norwegian margin to explore differences in depth zonation, type and carbon assimilation mode of anaero

  17. Comprehensive analysis for major, minor and trace element contents and Sr-Nd-Pb-Hf isotope ratios in sediment reference materials, JSd-1 and MAG-1

    Digital Repository Service at National Institute of Oceanography (India)

    Nath, B.N.; Makishima, A.; Noordmann, J.; Tanaka, R.; Nakamura, E.

    In view of the requirement of a well-characterized and easily available aquatic sediment reference material, a comprehensive analysis comprising of fifty major, minor and trace elements as well as Sr–Nd–Pb–Hf isotopes were carried out...

  18. Actinide consumption: Nuclear resource conservation without breeding

    Energy Technology Data Exchange (ETDEWEB)

    Hannum, W.H.; Battles, J.E.; Johnson, T.R.; McPheeters, C.C.

    1991-01-01

    A new approach to the nuclear power issue based on a metallic fast reactor fuel and pyrometallurgical processing of spent fuel is showing great potential and is approaching a critical demonstration phase. If successful, this approach will complement and validate the LWR reactor systems and the attendant infrastructure (including repository development) and will alleviate the dominant concerns over the acceptability of nuclear power. The Integral Fast Reactor (IFR) concept is a metal-fueled, sodium-cooled pool-type fast reactor supported by a pyrometallurgical reprocessing system. The concept of a sodium cooled fast reactor is broadly demonstrated by the EBR-II and FFTF in the US; DFR and PFR in the UK; Phenix and SuperPhenix in France; BOR-60, BN-350, BN-600 in the USSR; and JOYO in Japan. The metallic fuel is an evolution from early EBR-II fuels. This fuel, a ternary U-Pu-Zr alloy, has been demonstrated to be highly reliable and fault tolerant even at very high burnup (160-180,000 MWd/MT). The fuel, coupled with the pool type reactor configuration, has been shown to have outstanding safety characteristics: even with all active safety systems disabled, such a reactor can survive a loss of coolant flow, a loss of heat sink, or other major accidents. Design studies based on a small modular approach show not only its impressive safety characteristics, but are projected to be economically competitive. The program to explore the feasibility of actinide recovery from spent LWR fuel is in its initial phase, but it is expected that technical feasibility could be demonstrated by about 1995; DOE has not yet committed funds to achieve this objective. 27 refs.

  19. Static, Mixed-Array Total Evaporation for Improved Quantitation of Plutonium Minor Isotopes in Small Samples

    Science.gov (United States)

    Stanley, F. E.; Byerly, Benjamin L.; Thomas, Mariam R.; Spencer, Khalil J.

    2016-06-01

    Actinide isotope measurements are a critical signature capability in the modern nuclear forensics "toolbox", especially when interrogating anthropogenic constituents in real-world scenarios. Unfortunately, established methodologies, such as traditional total evaporation via thermal ionization mass spectrometry, struggle to confidently measure low abundance isotope ratios (plutonium minor isotope measurements, which have been resistant to enhancement in recent years because of elevated radiologic concerns. Results are presented for small sample (~20 ng) applications involving a well-known plutonium isotope reference material, CRM-126a, and compared with traditional total evaporation methods.

  20. Measurement of Actinides in Molybdenum-99 Solution Analytical Procedure

    Energy Technology Data Exchange (ETDEWEB)

    Soderquist, Chuck Z. [Pacific Northwest National Lab. (PNNL), Richland, WA (United States); Weaver, Jamie L. [Pacific Northwest National Lab. (PNNL), Richland, WA (United States)

    2015-11-01

    This document is a companion report to a previous report, PNNL 24519, Measurement of Actinides in Molybdenum-99 Solution, A Brief Review of the Literature, August 2015. In this companion report, we report a fast, accurate, newly developed analytical method for measurement of trace alpha-emitting actinide elements in commercial high-activity molybdenum-99 solution. Molybdenum-99 is widely used to produce 99mTc for medical imaging. Because it is used as a radiopharmaceutical, its purity must be proven to be extremely high, particularly for the alpha emitting actinides. The sample of 99Mo solution is measured into a vessel (such as a polyethylene centrifuge tube) and acidified with dilute nitric acid. A gadolinium carrier is added (50 µg). Tracers and spikes are added as necessary. Then the solution is made strongly basic with ammonium hydroxide, which causes the gadolinium carrier to precipitate as hydrous Gd(OH)3. The precipitate of Gd(OH)3 carries all of the actinide elements. The suspension of gadolinium hydroxide is then passed through a membrane filter to make a counting mount suitable for direct alpha spectrometry. The high-activity 99Mo and 99mTc pass through the membrane filter and are separated from the alpha emitters. The gadolinium hydroxide, carrying any trace actinide elements that might be present in the sample, forms a thin, uniform cake on the surface of the membrane filter. The filter cake is first washed with dilute ammonium hydroxide to push the last traces of molybdate through, then with water. The filter is then mounted on a stainless steel counting disk. Finally, the alpha emitting actinide elements are measured by alpha spectrometry.

  1. Electronic structure and ionicity of actinide oxides from first principles

    DEFF Research Database (Denmark)

    Petit, Leon; Svane, Axel; Szotek, Z.

    2010-01-01

    The ground-state electronic structures of the actinide oxides AO, A2O3, and AO2 (A=U, Np, Pu, Am, Cm, Bk, and Cf) are determined from first-principles calculations, using the self-interaction corrected local spin-density approximation. Emphasis is put on the degree of f-electron localization, whi...... lanthanide oxides. The ionic nature of the actinide oxides emerges from the fact that only those compounds will form where the calculated ground-state valency agrees with the nominal valency expected from a simple charge counting....

  2. SOLVENT EXTRACTION PROCESS FOR SEPARATING ACTINIDE AND LANTHANIDE METAL VALUES

    Science.gov (United States)

    Hildebrandt, R.A.; Hyman, H.H.; Vogler, S.

    1962-08-14

    A process of countercurrently extracting an aqueous mineral acid feed solution for the separation of actinides from lanthanides dissolved therern is described. The feed solution is made acid-defrcient with alkali metal hydroxide prior to.contact with acid extractant; during extraction, however, acid is transferred from organic to aqueous solution and the aqueous solution gradually becomes acid. The acid-deficient phase ' of the process promotes the extraction of the actinides, while the latter acid phase'' of the process improves retention of the lanthanides in the aqueous solution. This provides for an improved separation. (AEC)

  3. Thermally unstable complexants/phosphate mineralization of actinides

    Energy Technology Data Exchange (ETDEWEB)

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

    1996-10-01

    In situ immobilization is an approach to isolation of radionuclides from the hydrosphere that is receiving increasing attention. Rather than removing the actinides from contaminated soils, this approach transforms the actinides into intrinsically insoluble mineral phases resistant to leaching by groundwater. The principal advangates of this concept are the low cost and low risk of operator exposure and/or dispersion of the radionuclides to the wider environment. The challenge of this approach is toe accomplish the immobilization without causing collateral damage to the environment (the cure shouldn`t be worse than the disease) and verification of system performance.

  4. New molecules for the separation of actinides (III): the picolinamides

    Energy Technology Data Exchange (ETDEWEB)

    Cordier, P.Y.; Condamines, N.; Berthon, L.; Madic, C.

    1994-12-31

    Minor actinide partitioning from high level liquid wastes produced during the reprocessing of nuclear fuels by the Purex process, requires the design of new extracting molecules. These new extractants must be able to separate, for example, actinides from lanthanides. This separation is very difficult, due to the similar chemical properties of these metallic species, but it can possibly be reached by using extractants with soft donor atoms (N or S). Some new molecules : the picolinamides are investigated in this way. The general chemical formula and the behaviour of these compounds in acidic media are given. (O.L.). 3 refs.

  5. Minor actinides impact on basic safety parameters of medium-sized sodium-cooled fast reactor

    Directory of Open Access Journals (Sweden)

    Darnowski Piotr

    2015-03-01

    Full Text Available An analysis of the influence of addition of minor actinides (MA to the fast reactor fuel on the most important safety characteristics was performed. A special emphasis was given to the total control rods worth in order to describe qualitatively and quantitatively its change with MA content. All computations were performed with a homogeneous assembly model of modified BN-600 sodium-cooled fast reactor core with 0, 3 and 6% of MA. A model was prepared for the Monte Carlo neutron transport code MCNP5 for fresh fuel in the beginning-of-life (BOL state. Additionally, some other parameters, such as Doppler constant, sodium void reactivity, delayed neutron fraction, neutron fluxes and neutron spectra distribution, were computed and their change with MA content was investigated. Study indicates that the total control rods worth (CRW decreases with increasing MA inventory in the fuel and confirms that the addition of MA has a negative effect on the delayed neutron fraction.

  6. Non-compound nucleus fission in actinide and pre-actinide regions

    Indian Academy of Sciences (India)

    R Tripathi; S Sodaye; K Sudarshan

    2015-08-01

    In this article, some of our recent results on fission fragment/product angular distributions are discussed in the context of non-compound nucleus fission. Measurement of fission fragment angular distribution in 28Si+176Yb reaction did not show a large contribution from the non-compound nucleus fission. Data on the evaporation residue cross-sections, in addition to those on mass and angular distributions, are necessary for better understanding of the contribution from non-compound nucleus fission in the pre-actinide region. Measurement of mass-resolved angular distribution of fission products in 20Ne+232Th reaction showed an increase in angular anisotropy with decreasing asymmetry of mass division. This observation can be explained based on the contribution from pre-equilibrium fission. Results of these studies showed that the mass dependence of anisotropy may possibly be used to distinguish pre-equilibrium fission and quasifission.

  7. Topical Report on Actinide-Only Burnup Credit for PWR Spent Nuclear Fuel Packages. Revision 2

    Energy Technology Data Exchange (ETDEWEB)

    None, None

    1998-09-01

    The objective of this topical report is to present to the NRC for review and acceptance a methodology for using burnup credit in the design of criticality control systems for PWR spent fuel transportation packages, while maintaining the criticality safety margins and related requirements of 10 CFR Part 71 and 72. The proposed methodology consists of five major steps as summarized below: (1) Validate a computer code system to calculate isotopic concentrations in SNF created during burnup in the reactor core and subsequent decay. (2) Validate a computer code system to predict the subcritical multiplication factor, keff, of a spent nuclear fuel package. (3) Establish bounding conditions for the isotopic concentration and criticality calculations. (4) Use the validated codes and bounding conditions to generate package loading criteria (burnup credit loading curves). and (5) Verify that SNF assemblies meet the package loading criteria and confirm proper fuel assembly selection prior to loading. (This step is required but the details are outside the scope of this topical report.) When reviewed and accepted by the NRC, this topical report will serve as a criterion document for criticality control analysts and will provide steps for the use of actinide-only burnup credit in the design of criticality control systems. The NRC-accepted burnup credit methodology will be used by commercial SNF storage and transportation package designers. Design-specific burnup credit criticality analyses will be defined, developed, and documented in the Safety Analysis Report (SAR) for each specific storage or transportation package that uses burnup credit. These SARs will then be submitted to the NRC for review and approval. This topical report is expected to be referenced in a number of storage and transportation cask applications to be submitted by commercial cask and canister designers to the NRC. Therefore, NRC acceptance of this topical report will result in increased efficiency of the

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

    Energy Technology Data Exchange (ETDEWEB)

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

    2008-07-01

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

  9. Gamma ray spectroscopy of neutron-rich actinides after multi-nucleon transfer reactions

    Energy Technology Data Exchange (ETDEWEB)

    Vogt, Andreas; Birkenbach, Benedikt; Reiter, Peter; Hess, Herbert; Lewandowski, Lars; Steinbach, Tim [Institut fuer Kernphysik, Universitaet zu Koeln (Germany); Collaboration: LNL 11.22-Collaboration

    2014-07-01

    Excited states in neutron-rich Th and U nuclei were investigated after multi-nucleon transfer reactions employing the AGATA demonstrator and PRISMA setup at LNL (INFN, Italy). A primary {sup 136}Xe beam of 1 GeV hitting a {sup 238}U target was used to produce the nuclei of interest in the actinide region. Beam-like reaction products in the Xe-Ba-region were identified and selected by the PRISMA spectrometer. Kinematic coincidences between the binary reaction products of beam-like and target-like nuclei are detected with an additional MCP detector. Those coincidences allow clean conditions for in-beam γ-ray spectroscopy. Background contributions from excited fission fragments are successfully discriminated. γ-rays from excited states in beam- and target-like particles were measured with the position sensitive AGATA HPGe detectors. Improved energy resolution after Doppler correction is based on the novel γ-ray tracking technique which was successfully exploited to increase the quality of the γ-spectra. γ-ray spectra of the produced beam-like isotopes in the one-proton and two-proton transfer channels will be presented. Corresponding results from the hard-to-reach neutron-rich isotopes beyond {sup 232}Th will focus on their collective properties and cross section limits for their production.

  10. Solubility testing of actinides on breathing-zone and area air samples

    Energy Technology Data Exchange (ETDEWEB)

    Metzger, R.L.; Jessop, B.H.; McDowell, B.L. [Radiation Safety Engineering, Inc., Chandler, AZ (United States)

    1996-02-01

    A solubility testing method for several common actinides has been developed with sufficient sensitivity to allow profiles to be determined from routine breathing zone and area air samples in the workplace. Air samples are covered with a clean filter to form a filter-sample-filter sandwich which is immersed in an extracellular lung serum simulant solution. The sample is moved to a fresh beaker of the lung fluid simulant each day for one week, and then weekly until the end of the 28 day test period. The soak solutions are wet ashed with nitric acid and hydrogen peroxide to destroy the organic components of the lung simulant solution prior to extraction of the nuclides of interest directly into an extractive scintillator for subsequent counting on a Photon-Electron Rejecting Alpha Liquid Scintillation (PERALS{reg_sign}) spectrometer. Solvent extraction methods utilizing the extractive scintillators have been developed for the isotopes of uranium, plutonium, and curium. The procedures normally produce an isotopic recovery greater than 95% and have been used to develop solubility profiles from air samples with 40 pCi or less of U{sub 3}O{sub 8}. Profiles developed for U{sub 3}O{sub 8} samples show good agreement with in vitro and in vivo tests performed by other investigators on samples from the same uranium mills.

  11. New BRC neutron evaluations of actinides with the TALYS code: Modelization and first validation tests

    Directory of Open Access Journals (Sweden)

    Romain P.

    2010-10-01

    Full Text Available The reader may have a look on references [1–3,5] for more details. Over the last five years, new evaluations of plutonium and uranium have been performed at Bruyèeres-le-Châtel (BRC from the resolved resonance region up to 30MeV. Only nuclear reactions models have been used to build these evaluations. Total, shape elastic and direct inelastic cross sections are obtained from a coupled channel model using a dispersive optical potential (BRC, [13] devoted to actinides. All the other cross sections are calculated owing to the Hauser-Fesbach theory (TALYS code [4].We take particular care over the fission channel. For uranium isotopes, a triple-humped barrier [3] is required in order to reproduce accurately the variations of the experimental fission cross sections. As not commonly expected, we show [5] that the effect of the class II or class III states located in the wells of the aforementioned fission barrier provide sometimes an anti-resonant transmission rather than a resonant. With increasing neutron incident energy, a lot of residual nuclei produced by nucleon emission lead to fission also. All available experimental data assigned to the various fission mechanisms of the same nucleus are used to define its fission barrier parameters. As a result of this approach, we are now able to provide consistent evaluations for a large series of isotopes. Of course, our new evaluations have been tested against integral data.

  12. Molecular and electronic structure of actinide hexa-cyanoferrates; Structure moleculaire et electronique des hexacyanoferrates d'actinides

    Energy Technology Data Exchange (ETDEWEB)

    Bonhoure, I

    2001-07-01

    The goal of this work is to improve our knowledge on the actinide-ligand bond properties. To this end, the hexacyanoferrate entities have been used as pre-organized ligand. We have synthesized, using mild chemistry, the following series of complexes: An{sup IV}[Fe{sup II}(CN){sub 6}].xH{sub 2}O (An = Th, U, Np, Pu); Am{sup III}[Fe{sup III}(CN){sub 6}].xH{sub 2}O; Pu {sup III}[Co{sup III}(CN){sub 6}].xH{sub 2}O and K(H?)An{sup III}[Fe{sup II}(CN){sub 6}].xH{sub 2}O (An = Pu, Am). The metal oxidation states have been obtained thanks to the {nu}{sub CN}, stretching vibration and to the actinide L{sub III} absorption edge studies. As Prussian Blue, the An{sup IV}[Fe{sup II}(CN){sub 6}].xH{sub 2}O (An = Np, Pu) are class II of Robin and Day compounds. X-ray Diffraction has shown besides that these complexes crystallize in the P6{sub 3}/m space group, as the isomorphic LaKFe(CN){sub 6}.4H{sub 2}O complex used as structural model. The EXAFS oscillations at the iron K edge and at the An L{sub III} edge allowed to determine the An-N, An-O, Fe-C and Fe-N distances. The display of the multiple scattering paths for both edges explains the actinide contribution absence at the iron edge, whereas the iron signature is present at the actinide edge. We have shown that the actinide coordination sphere in actinides hexa-cyanoferrates is comparable to the one of lanthanides. However, the actinides typical behavior towards the lanthanides is brought to the fore by the An{sup IV} versus Ln{sup III} ions presence in this family of complexes. Contrarily to the 4f electrons, the 5f electrons influence the electronic properties of the compounds of this family. However, the gap between the An-N and Ln-N distances towards the corresponding metals ionic radii do not show any covalence bond evolution between the actinide and lanthanide series. (author)

  13. Effect of changes in the deuterium content of drinking water on the hydrogen isotope ratio of urinary steroids in the context of sports drug testing.

    Science.gov (United States)

    Piper, Thomas; Degenhardt, Karoline; Federherr, Eugen; Thomas, Andreas; Thevis, Mario; Saugy, Martial

    2013-03-01

    The hydrogen isotope ratio (HIR) of body water and, therefore, of all endogenously synthesized compounds in humans, is mainly affected by the HIR of ingested drinking water. As a consequence, the entire organism and all of its synthesized substrates will reflect alterations in the isotope ratio of drinking water, which depends on the duration of exposure. To investigate the effect of this change on endogenous urinary steroids relevant to doping-control analysis the hydrogen isotope composition of potable water was suddenly enriched from -50 to 200 ‰ and maintained at this level for two weeks for two individuals. The steroids under investigation were 5β-pregnane-3α,20α-diol, 5α-androst-16-en-3α-ol, 3α-hydroxy-5α-androstan-17-one (ANDRO), 3α-hydroxy-5β-androstan-17-one (ETIO), 5α-androstane-3α,17β-diol, and 5β-androstane-3α,17β-diol (excreted as glucuronides) and ETIO, ANDRO and 3β-hydroxyandrost-5-en-17-one (excreted as sulfates). The HIR of body water was estimated by determination of the HIR of total native urine, to trace the induced changes. The hydrogen in steroids is partly derived from the total amount of body water and cholesterol-enrichment could be calculated by use of these data. Although the sum of changes in the isotopic composition of body water was 150 ‰, shifts of approximately 30 ‰ were observed for urinary steroids. Parallel enrichment in their HIR was observed for most of the steroids, and none of the differences between the HIR of individual steroids was elevated beyond recently established thresholds. This finding is important to sports drug testing because it supports the intended use of this novel and complementary methodology even in cases where athletes have drunk water of different HIR, a plausible and, presumably, inevitable scenario while traveling.

  14. Multidimensionally constrained relativistic mean-field study of triple-humped barriers in actinides

    Science.gov (United States)

    Zhao, Jie; Lu, Bing-Nan; Vretenar, Dario; Zhao, En-Guang; Zhou, Shan-Gui

    2015-01-01

    Background: Potential energy surfaces (PES's) of actinide nuclei are characterized by a two-humped barrier structure. At large deformations beyond the second barrier, the occurrence of a third barrier was predicted by macroscopic-microscopic model calculations in the 1970s, but contradictory results were later reported by a number of studies that used different methods. Purpose: Triple-humped barriers in actinide nuclei are investigated in the framework of covariant density functional theory (CDFT). Methods: Calculations are performed using the multidimensionally constrained relativistic mean field (MDC-RMF) model, with the nonlinear point-coupling functional PC-PK1 and the density-dependent meson exchange functional DD-ME2 in the particle-hole channel. Pairing correlations are treated in the BCS approximation with a separable pairing force of finite range. Results: Two-dimensional PES's of 226,228,230,232Th and 232,235,236,238U are mapped and the third minima on these surfaces are located. Then one-dimensional potential energy curves along the fission path are analyzed in detail and the energies of the second barrier, the third minimum, and the third barrier are determined. The functional DD-ME2 predicts the occurrence of a third barrier in all Th nuclei and 238U . The third minima in 230 ,232Th are very shallow, whereas those in 226 ,228Th and 238U are quite prominent. With the functional PC-PK1 a third barrier is found only in 226 ,228 ,230Th . Single-nucleon levels around the Fermi surface are analyzed in 226Th, and it is found that the formation of the third minimum is mainly due to the Z =90 proton energy gap at β20≈1.5 and β30≈0.7 . Conclusions: The possible occurrence of a third barrier on the PES's of actinide nuclei depends on the effective interaction used in multidimensional CDFT calculations. More pronounced minima are predicted by the DD-ME2 functional, as compared to the functional PC-PK1. The depth of the third well in Th isotopes decreases

  15. Plant Mounds as Concentration and Stabilization Agents for Actinide Soil Contaminants in Nevada

    Energy Technology Data Exchange (ETDEWEB)

    D.S. Shafer; J. Gommes

    2009-02-03

    Plant mounds or blow-sand mounds are accumulations of soil particles and plant debris around the base of shrubs and are common features in deserts in the southwestern United States. An important factor in their formation is that shrubs create surface roughness that causes wind-suspended particles to be deposited and resist further suspension. Shrub mounds occur in some plant communities on the Nevada Test Site, the Nevada Test and Training Range (NTTR), and Tonopah Test Range (TTR), including areas of surface soil contamination from past nuclear testing. In the 1970s as part of early studies to understand properties of actinides in the environment, the Nevada Applied Ecology Group (NAEG) examined the accumulation of isotopes of Pu, 241Am, and U in plant mounds at safety experiment and storage-transportation test sites of nuclear devices. Although aerial concentrations of these contaminants were highest in the intershrub or desert pavement areas, the concentration in mounds were higher than in equal volumes of intershrub or desert pavement soil. The NAEG studies found the ratio of contaminant concentration of actinides in soil to be greater (1.6 to 2.0) in shrub mounds than in the surrounding areas of desert pavement. At Project 57 on the NTTR, 17 percent of the area was covered in mounds while at Clean Slate III on the TTR, 32 percent of the area was covered in mounds. If equivalent volumes of contaminated soil were compared between mounds and desert pavement areas at these sites, then the former might contain as much as 34 and 62 percent of the contaminant inventory, respectively. Not accounting for radionuclides associated with shrub mounds would cause the inventory of contaminants and potential exposure to be underestimated. In addition, preservation of shrub mounds could be important part of long-term stewardship if these sites are closed by fencing and posting with administrative controls.

  16. Preparation of actinide targets and sources using nonaqueous electrodeposition

    Energy Technology Data Exchange (ETDEWEB)

    Fowler, M.M.; Gursky, J.C.; Wilhelmy, J.B. (Los Alamos National Lab., NM (USA))

    1991-05-15

    Application of the method of 'molecular plating' to prepare actinide targets suitable for accelerator bombardment is presented. Two example applications involving {sup 229}Th and {sup 254}Es are discussed along with the merits and liabilities of the method. (orig.).

  17. Actinides How well do we know their stellar production?

    CERN Document Server

    Goriely, S

    2001-01-01

    The reliable evaluation of the r-process production of the actinides and careful estimates of the uncertainties affecting these predictions are key ingredients especially in nucleo-cosmochronology studies based on the analysis of very metal-poor stars or on the composition of meteorites. This type of information is also required in order to make the best possible use of future high precision data on the actinide composition of galactic cosmic rays, of the local interstellar medium, or of meteoritic grains of presumed circumstellar origin. This paper provides the practitioners in these various fields with the most detailed and careful analysis of the r-process actinide production available to-date. In total, thirty-two different multi-event canonical calculations using different nuclear ingredients or astrophysics conditions are presented, and are considered to give a fair picture of the level of reliability of the predictions of the actinide production, at least in the framework of a simple r-process model. T...

  18. Nuclear fuel cycle-oriented actinides separation in China

    Energy Technology Data Exchange (ETDEWEB)

    Chen, Jing; He, Xihong; Wang, Jianchen [Tsinghua Univ., Beijing (China). Inst. of Nuclear and New Energy Technology

    2014-04-01

    In the last decades, the separation of actinides was widely and continuously studied in China. A few kinds of salt-free reductants to adjust Pu and Np valences have been investigated. N,N-dimethylhydroxylamine is a good reductant with high reduction rate constants for the co-reduction of Pu(IV) and Np(VI), and monomethylhydrazine is a simple compound for the individual reduction of Np(VI). Advanced PUREX based on Organic Reductants (APOR) was proposed. Trialkylphosphine oxide (TRPO) with a single functional group was found to possess strong affinity to tri-, tetra- and hexa-valent actinides. TRPO process has been first explored in China for actinides partitioning from high level waste and the good partitioning performance was demonstrated by the hot test. High extraction selectivity for trivalent actinides over lanthanides by dialkyldithiophosphinic acids was originally found in China. A separation process based on purified Cyanex 301 for the separation of Am from lanthanides was presented and successfully tested in a battery of miniature centrifugal contactors. (orig.)

  19. RAPID SEPARATION OF ACTINIDES AND RADIOSTRONTIUM IN VEGETATION SAMPLES

    Energy Technology Data Exchange (ETDEWEB)

    Maxwell, S.

    2010-06-01

    A new rapid method for the determination of actinides and radiostrontium in vegetation samples has been developed at the Savannah River Site Environmental Lab (Aiken, SC, USA) that can be used in emergency response situations or for routine analysis. The actinides in vegetation method utilizes a rapid sodium hydroxide fusion method, a lanthanum fluoride matrix removal step, and a streamlined column separation process with stacked TEVA, TRU and DGA Resin cartridges. Lanthanum was separated rapidly and effectively from Am and Cm on DGA Resin. Alpha emitters are prepared using rare earth microprecipitation for counting by alpha spectrometry. The purified {sup 90}Sr fractions are mounted directly on planchets and counted by gas flow proportional counting. The method showed high chemical recoveries and effective removal of interferences. The actinide and {sup 90}Sr in vegetation sample analysis can be performed in less than 8 h with excellent quality for emergency samples. The rapid fusion technique is a rugged sample digestion method that ensures that any refractory actinide particles or vegetation residue after furnace heating is effectively digested.

  20. Functionalized pyrazines as ligands for minor actinide extraction and catalysis

    NARCIS (Netherlands)

    Nikishkin, N.

    2013-01-01

    The research presented in this thesis concerns the design of ligands for a wide range of applications, from nuclear waste treatment to catalysis. The strategies employed to design actinide-selective extractants, for instance, comprise the fine tuning of the ligand electronic properties as well as us

  1. Actinide biocolloid formation in brine by halophilic bacteria

    Energy Technology Data Exchange (ETDEWEB)

    Gillow, J.B.; Francis, A.J.; Dodge, C.J. [Brookhaven National Lab., Upton, NY (United States); Harris, R.; Beveridge, T.J. [Univ. of Guelph, Ontario (Canada); Brady, P.V.; Papenguth, H.W. [Sandia National Labs., Albuquerque, NM (United States)

    1998-12-31

    The authors examined the ability of a halophilic bacterium (WIPP 1A) isolated from the Waste Isolation Pilot Plant (WIPP) site to accumulate uranium in order to determine the potential for biocolloid facilitated actinide transport. The bacterial cell surface functional groups involved in the complexation of the actinide were determined by titration. Uranium, added as uranyl nitrate, was removed from solution at pH 5 by cells but at pH 7 and 9 very little uranium was removed due to its limited solubility. Although present as soluble species, uranyl citrate at pH 5, 7, and 9, and uranyl carbonate at pH 9 were not removed by the bacterium because they were not bioavailable due to their neutral or negative charge. Addition of uranyl EDTA to brine at pH 5, 7, and 9 resulted in the immediate precipitation of U. Transmission electron microscopy (TEM) and energy dispersive X-ray spectroscopy (EDS) analysis revealed that uranium was not only associated with the cell surface but also accumulated intracellularly as uranium-enriched granules. Extended X-ray absorption fine structure (EXAFS) analysis of the bacterial cells indicated the bulk sample contained more than one uranium phase. Nevertheless these results show the potential for the formation of actinide bearing bacterial biocolloids that are strictly regulated by the speciation and bioavailability of the actinide.

  2. ACTINIDE BIOCOLLOID FORMATION IN BRINE BY HALOPHILIC BACTERIA

    Energy Technology Data Exchange (ETDEWEB)

    GILLOW,J.B.; FRANCIS,A.J.; DODGE,C.J.; HARRIS,R.; BEVERIDGE,T.J.; BRADY,P.B.; PAPENGUTH,H.W.

    1998-11-09

    The authors examined the ability of a halophilic bacterium (WIPP 1A) isolated from the Waste Isolation Pilot Plant (WIPP) site to accumulate uranium in order to determine the potential for biocolloid facilitated actinide transport. The bacterial cell surface functional groups involved in the complexation of the actinide were determined by titration. Uranium, added as uranyl nitrate, was removed from solution at pH 5 by cells but at pH 7 and 9 very little uranium was removed due to its limited solubility. Although present as soluble species, uranyl citrate at pH 5, 7, and 9, and uranyl carbonate at pH 9 were not removed by the bacterium because they were not bioavailable due to their neutral or negative charge. Addition of uranyl EDTA to brine at pH 5, 7, and 9 resulted in the immediate precipitation of U. Transmission electron microscopy (TEM) and energy dispersive X-ray spectroscopy (EDS) analysis revealed that uranium was not only associated with the cell surface but also accumulated intracellularly as uranium-enriched granules. Extended X-ray absorption fine structure (EXAFS) analysis of the bacterial cells indicated the bulk sample contained more than one uranium phase. Nevertheless these results show the potential for the formation of actinide bearing bacterial biocolloids that are strictly regulated by the speciation and bioavailability of the actinide.

  3. Actinide Biocolloid Formation in Brine by Halophilic Bacteria

    Energy Technology Data Exchange (ETDEWEB)

    Gillow, J.B.; Francis, A.J.; Dodge, C.J.; Harris, R.; Beveridge, T.J.; Brady, P.V.; Papenguth, H.W.

    1999-07-28

    We examined the ability of a halophilic bacterium (WFP 1A) isolated from the Waste Isolation Pilot Plant (WIPP) site to accumulate uranium in order to determine the potential for biocolloid facilitated actinide transport. The bacterial cell Surface functional groups involved in the complexation of the actinide were determined by titration. Uranium, added as uranyl nitrate, was removed from solution at pH 5 by cells but at pH 7 and 9 very little uranium was removed due to its limited volubility. Although present as soluble species, uranyl citrate at pH 5, 7, and 9, and uranyl carbonate at pH 9 were not removed by the bacterium because they were not bioavailable due to their neutral or negative charge. Addition of uranyl EDTA to brine at pH 5, 7, and 9 resulted in the immediate precipitation of U. Transmission electron microscopy (TEM) and energy dispersive X-ray spectroscopy (EDS) analysis revealed that uranium was not only associated with the cell surface but also accumulated intracellulary as uranium-enriched granules. Extended X-ray absorption fine structure (EXAFS) analysis, of the bacterial cells indicated the bulk sample contained more than one uranium phase. Nevertheless these results show the potential for the formation of actinide bearing bacterial biocolloids that are strictly regulated by the speciation and bioavailability of the actinide.

  4. Experimental Evaluation of Actinide Transport in a Fractured Granodiorite

    Energy Technology Data Exchange (ETDEWEB)

    Dittrich, Timothy M. [Los Alamos National Laboratory; Reimus, Paul W. [Los Alamos National Laboratory

    2015-03-16

    The objective of this study was to demonstrate and evaluate new experimental methods for quantifying the potential for actinide transport in deep fractured crystalline rock formations. We selected a fractured granodiorite at the Grimsel Test Site (GTS) in Switzerland as a model system because field experiments have already been conducted with uranium and additional field experiments using other actinides are planned at the site. Thus, working on this system provides a unique opportunity to compare lab experiment results with fieldscale observations. Rock cores drilled from the GTS were shipped to Los Alamos National Laboratory, characterized by x-ray diffraction and microscopy, and used in batch sorption and column breakthrough experiments. Solutions with pH 6.8 and 8.8 were tested. Solutions were switched to radionuclide-free synthetic Grimsel groundwater after near-steady actinide/colloid breakthrough occurred in column experiments. We are currently evaluating actinide adsorption/desorption rates as a function of water chemistry (initial focus on pH), with future testing planned to evaluate the influence of carbonate concentrations, flow rates, and mineralogy in solutions and suspensions with bentonite colloids. (auth)

  5. Potential radiation dose from eating fish exposed to actinide contamination

    Energy Technology Data Exchange (ETDEWEB)

    Emery, R.M.; Klopfer, D.C.; Baker, D.A.; Soldat, J.K. (Battelle Pacific Northwest Labs., Richland, WA (USA))

    1981-04-01

    The purpose of this work is to establish a maximum potential for transporting actinides to man via fish consumption. The study took place in U-pond, a nuclear waste pond on the Hanford Site. It has concentrations of /sup 238/U, /sup 238/Pu, sup(239,240)Pu and /sup 241/Am that are approx. 3 orders of magnitude greater than background levels. Fish living in the pond contain higher actinide concentrations than those observed in fish from any other location. Experiments were performed in U-Pond to determine maximum quantities of actinides that could accumulate in fillets and whole bodies of two centrarchid fish species. Doses to hypothetical consumers were then estimated. Results indicate that highest concentrations occurring in bluegill or bass muscle after more than a year's exposure to the pond would not be sufficient to produce a significant radiation dose to a human consumer, even if he ate 0.5 kg (of the order of 1 lb) of these fillets every day for 70 yr. Natural predators (heron or coyote), having lifetime diets of whole fish from U-Pond, would receive less radiation dose from the ingested actinides than from natural background sources.

  6. Actinide partitioning-transmutation program final report. I. Overall assessment

    Energy Technology Data Exchange (ETDEWEB)

    Croff, A.G.; Blomeke, J.O.; Finney, B.C.

    1980-06-01

    This report is concerned with an overall assessment of the feasibility of and incentives for partitioning (recovering) long-lived nuclides from fuel reprocessing and fuel refabrication plant radioactive wastes and transmuting them to shorter-lived or stable nuclides by neutron irradiation. The principal class of nuclides considered is the actinides, although a brief analysis is given of the partitioning and transmutation (P-T) of /sup 99/Tc and /sup 129/I. The results obtained in this program permit us to make a comparison of the impacts of waste management with and without actinide recovery and transmutation. Three major conclusions concerning technical feasibility can be drawn from the assessment: (1) actinide P-T is feasible, subject to the acceptability of fuels containing recycle actinides; (2) technetium P-T is feasible if satisfactory partitioning processes can be developed and satisfactory fuels identified (no studies have been made in this area); and (3) iodine P-T is marginally feasible at best because of the low transmutation rates, the high volatility, and the corrosiveness of iodine and iodine compounds. It was concluded on the basis of a very conservative repository risk analysis that there are no safety or cost incentives for actinide P-T. In fact, if nonradiological risks are included, the short-term risks of P-T exceed the long-term benefits integrated over a period of 1 million years. Incentives for technetium and iodine P-T exist only if extremely conservative long-term risk analyses are used. Further RD and D in support of P-T is not warranted.

  7. Sequestering agents for the removal of actinides from waste streams

    Energy Technology Data Exchange (ETDEWEB)

    Raymond, K.N.; White, D.J.; Xu, Jide; Mohs, T.R. [Univ. of California, Berkeley, CA (United States)

    1997-10-01

    The goal of this project is to take a biomimetic approach toward developing new separation technologies for the removal of radioactive elements from contaminated DOE sites. To achieve this objective, the authors are investigating the fundamental chemistry of naturally occurring, highly specific metal ion sequestering agents and developing them into liquid/liquid and solid supported actinide extraction agents. Nature produces sideophores (e.g., Enterobactin and Desferrioxamine B) to selectivity sequester Lewis acidic metal ions, in particular Fe(III), from its surroundings. These chelating agents typically use multiple catechols or hydroxamic acids to form polydentate ligands that chelate the metal ion forming very stable complexes. The authors are investigating and developing analogous molecules into selective chelators targeting actinide(IV) ions, which display similar properties to Fe(III). By taking advantage of differences in charge, preferred coordination number, and pH stability range, the transition from nature to actinide sequestering agents has been applied to the development of new and highly selective actinide extraction technologies. Additionally, the authors have shown that these chelating ligands are versatile ligands for chelating U(VI). In particular, they have been studying their coordination chemistry and fundamental interactions with the uranyl ion [UO{sub 2}]{sup 2+}, the dominant form of uranium found in aqueous media. With an understanding of this chemistry, and results obtained from in vivo uranium sequestration studies, it should be possible to apply these actinide(IV) extraction technologies to the development of new extraction agents for the removal of uranium from waste streams.

  8. Measurements of the neutron capture cross sections and incineration potentials of minor-actinides in high thermal neutron fluxes: Impact on the transmutation of nuclear wastes; Mesures des sections efficaces de capture et potentiels d'incineration des actinides mineurs dans les hauts flux de neutrons: Impact sur la transmutation des dechets

    Energy Technology Data Exchange (ETDEWEB)

    Bringer, O

    2007-10-15

    This thesis comes within the framework of minor-actinide nuclear transmutation studies. First of all, we have evaluated the impact of minor actinide nuclear data uncertainties within the cases of {sup 241}Am and {sup 237}Np incineration in three different reactor spectra: EFR (fast), GT-MHR (epithermal) and HI-HWR (thermal). The nuclear parameters which give the highest uncertainties were thus highlighted. As a result of fact, we have tried to reduce data uncertainties, in the thermal energy region, for one part of them through experimental campaigns in the moderated high intensity neutron fluxes of ILL reactor (Grenoble). These measurements were focused onto the incineration and transmutation of the americium-241, the curium-244 and the californium-249 isotopes. Finally, the values of 12 different cross sections and the {sup 241}Am isomeric branching ratio were precisely measured at thermal energy point. (author)

  9. Sediment source detection by stable isotope analysis, carbon and nitrogen content and CSSI in a small river of the Swiss Plateau

    Science.gov (United States)

    SchindlerWildhaber, Yael; Alewell, Christine; Birkholz, Axel

    2014-05-01

    Suspended sediment (SS) and organic matter in rivers can harm the fauna by affecting health and fitness of free swimming fish and by causing siltation of the riverbed. The temporal and spatial dynamics of sediment, carbon (C) and nitrogen (N) during the brown trout spawning season in a small river of the Swiss Plateau were assessed and C isotopes as well as the C/N atomic ratio were used to distinguish autochthonous and allochthonous sources of organic matter in SS loads. The visual basic program IsoSource with 13Ctot and 15N as input isotopes was used to quantify the temporal and spatial sources of SS. We determined compound specific stable carbon isotopes (CSSI) in fatty acids of possible sediment source areas to the stream in addition and compared them to SS from selected high flow and low flow events. Organic matter concentrations in the infiltrated and suspended sediment were highest during low flow periods with small sediment loads and lowest during high flow periods with high sediment loads. Peak values in nitrate and dissolved organic C were measured during high flow and high rainfall, probably due to leaching from pasture and arable land. The organic matter was of allochthonous sources as indicated by the C/N atomic ratio and δ13Corg. Organic matter in SS increased from up- to downstream due to an increase in sediment delivery from pasture and arable land downstream of the river. While the major sources of SS are pasture and arable land during base flow conditions, SS from forest soils increased during heavy rain events and warmer winter periods most likely due to snow melt which triggered erosion. Preliminary results of CSSI analysis of sediment source areas and comparison to SS of selected events indicate that differences in d13C values of individual fatty acids are too small to differentiate unambiguously between sediment sources.

  10. Biomimetic Actinide Chelators: An Update on the Preclinical Development of the Orally Active Hydroxypyridonate Decorporation Agents 3,4,3-LI(1,2-HOPO) and 5-LIO(Me-3,2-HOPO)

    Energy Technology Data Exchange (ETDEWEB)

    Durbin, Patricia W.; Kullgren, Birgitta; Ebbe, Shirley N.; Xu, Jide; Chang, Polly Y.; Bunin, Deborah I.; Blakely, Eleanor A.; Bjornstad, Kathleen A.; Rosen, Chris J.; Shuh, David K.; Raymond, Kenneth N.

    2011-07-13

    The threat of a dirty bomb or other major radiological contamination presents a danger of large-scale radiation exposure of the population. Because major components of such contamination are likely to be actinides, actinide decorporation treatments that will reduce radiation exposure must be a priority. Current therapies for the treatment of radionuclide contamination are limited and extensive efforts must be dedicated to the development of therapeutic, orally bioavailable, actinide chelators for emergency medical use. Using a biomimetic approach based on the similar biochemical properties of plutonium(IV) and iron(III), siderophore-inspired multidentate hydroxypyridonate ligands have been designed and are unrivaled in terms of actinide-affinity, selectivity, and efficiency. A perspective on the preclinical development of two hydroxypyridonate actinide decorporation agents, 3,4,3-LI(1,2-HOPO) and 5-LIO(Me-3,2-HOPO), is presented. The chemical syntheses of both candidate compounds have been optimized for scale-up. Baseline preparation and analytical methods suitable for manufacturing large amounts have been established. Both ligands show much higher actinide-removal efficacy than the currently approved agent, diethylenetriaminepentaacetic acid (DTPA), with different selectivity for the tested isotopes of plutonium, americium, uranium and neptunium. No toxicity is observed in cells derived from three different human tissue sources treated in vitro up to ligand concentrations of 1 mM, and both ligands were well tolerated in rats when orally administered daily at high doses (>100 micromol kg d) over 28 d under good laboratory practice guidelines. Both compounds are on an accelerated development pathway towards clinical use.

  11. Internal contamination by actinides after wounding: a robust rodent model for assessment of local and distant actinide retention.

    Science.gov (United States)

    Griffiths, N M; Wilk, J C; Abram, M C; Renault, D; Chau, Q; Helfer, N; Guichet, C; Van der Meeren, A

    2012-08-01

    Internal contamination by actinides following wounding may occur in nuclear fuel industry workers or subsequent to terrorist activities, causing dissemination of radioactive elements. Contamination by alpha particle emitting actinides can result in pathological effects, either local or distant from the site of entry. The objective of the present study was to develop a robust experimental approach in the rat for short- and long- term actinide contamination following wounding by incision of the skin and muscles of the hind limb. Anesthetized rats were contaminated with Mixed OXide (MOX, uranium, plutonium oxides containing 7.1% plutonium) or plutonium nitrate (Pu nitrate) following wounding by deep incision of the hind leg. Actinide excretion and tissue levels were measured as well as histological changes from 2 h to 3 mo. Humid swabs were used for rapid evaluation of contamination levels and proved to be an initial guide for contamination levels. Although the activity transferred from wound to blood is higher after contamination with a moderately soluble form of plutonium (nitrate), at 7 d most of the MOX (98%) or Pu nitrate (87%) was retained at the wound site. Rapid actinide retention in liver and bone was observed within 24 h, which increased up to 3 mo. After MOX contamination, a more rapid initial urinary excretion of americium was observed compared with plutonium. At 3 mo, around 95% of activity remained at the wound site, and excretion of Pu and Am was extremely low. This experimental approach could be applied to other situations involving contamination following wounding including rupture of the dermal, vascular, and muscle barriers.

  12. MGA: A gamma-ray spectrum analysis code for determining plutonium isotopic abundances. Volume 3, FORTRAN listing of the GA code

    Energy Technology Data Exchange (ETDEWEB)

    Gunnink, R

    1991-09-01

    Nondestructive measurements of x-ray and gamma-ray emissions can be used to determine the abundances of various actinides in a sample. Volume 1 of this report describes the methods and algorithms we have developed to determine the relative isotopic abundances of actinides in a sample, by analyzing gamma-ray spectra obtained using germanium detector systems. Volume 2 is a guide to using the MGA (Multiple Group Analysis) computer program we have written to perform plutonium isotopic analyses. This report contains a listing of the FORTRAN instructions of the code.

  13. Solubility of actinides and surrogates in nuclear glasses; Solubilite des actinides et de leurs simulants dans les verres nucleaires. Limites d'incorporation et comprehension des mecanismes

    Energy Technology Data Exchange (ETDEWEB)

    Lopez, Ch

    2003-07-01

    The nuclear wastes are currently incorporated in borosilicate glass matrices. The resulting glass must be perfectly homogeneous. The work discussed here is a study of actinide (thorium and plutonium) solubility in borosilicate glass, undertaken to assess the extent of actinide solubility in the glass and to understand the mechanisms controlling actinide solubilization. Glass specimens containing; actinide surrogates were used to prepare and optimize the fabrication of radioactive glass samples. These preliminary studies revealed that actinide Surrogates solubility in the glass was enhanced by controlling the processing temperature, the dissolution kinetic of the surrogate precursors, the glass composition and the oxidizing versus reducing conditions. The actinide solubility was investigated in the borosilicate glass. The evolution of thorium solubility in borosilicate glass was determined for temperatures ranging from 1200 deg C to 1400 deg C.Borosilicate glass specimens containing plutonium were fabricated. The experimental result showed that the plutonium solubility limit ranged from 1 to 2.5 wt% PuO{sub 2} at 1200 deg C. A structural approach based on the determination of the local structure around actinides and their surrogates by EXAFS spectroscopy was used to determine their structural role in the glass and the nature of their bonding with the vitreous network. This approach revealed a correlation between the length of these bonds and the solubility of the actinides and their surrogates. (author)

  14. Theory of the crystal structures of the actinide metals; Theorie des structures cristallines des metaux actinides

    Energy Technology Data Exchange (ETDEWEB)

    Penicaud, M. [CEA Bruyeres-le-Chatel, 91 (France)

    2005-07-01

    We describe, by bands calculation methods, the delocalized-localized transition of 5f electrons in the series of actinide metals, at ambient conditions, which happens between {alpha}-Pu and Am, and which is characterized by the change from the open and complex monoclinic crystal structure to the double hexagonal close-packed structure, and by the density collapse from 19.86 g.cm{sup -3} to 13.67 g.cm{sup -3}. The case of the alloy stabilized Pu in the high temperature {delta} phase (face centered cubic) is treated. Its ambient experimental density (15.92 g.cm{sup -3}) is obtained with a localization of the only 5f5/2 electrons. We find a 5f5/2 density of states peak pinned at the Fermi level, in agreement with photoelectron spectroscopy, and the high value of the electronic specific heat coefficient. The crystalline stability under pressure of U, Np, Pu and Am is examined. We find theoretically, at high pressure in Am, the stability of the recently discovered experimentally Am IV structure which is primitive-orthorhombic with four atoms in the unit cell. We calculate this structure also stable for Pu, for which it is proposed that the sequence is: {alpha}-Pu {yields} Am IV {yields} body-centered cubic. (author)

  15. Monitoring the bio-stimulation of hydrocarbon-contaminated soils by measurements of soil electrical properties, and CO2 content and its 13C/12C isotopic signature

    Science.gov (United States)

    Noel, C.; Gourry, J.; Ignatiadis, I.; Colombano, S.; Dictor, M.; Guimbaud, C.; Chartier, M.; Dumestre, A.; Dehez, S.; Naudet, V.

    2013-12-01

    Hydrocarbon contaminated soils represent an environmental issue as it impacts on ecosystems and aquifers. Where significant subsurface heterogeneity exists, conventional intrusive investigations and groundwater sampling can be insufficient to obtain a robust monitoring of hydrocarbon contaminants, as the information they provide is restricted to vertical profiles at discrete locations, with no information between sampling points. In order to obtain wider information in space volume on subsurface modifications, complementary methods can be used like geophysics. Among geophysical methods, geoelectrical techniques such as electrical resistivity (ER) and induced polarization (IP) seem the more promising, especially to study the effects of biodegradation processes. Laboratory and field geoelectrical experiments to characterize soils contaminated by oil products have shown that mature hydrocarbon-contaminated soils are characterized by enhanced electrical conductivity although hydrocarbons are electrically resistive. This high bulk conductivity is due to bacterial impacts on geological media, resulting in changes in the chemical and physical properties and thus, to the geophysical properties of the ground. Moreover, microbial activity induced CO2 production and isotopic deviation of carbon. Indeed, produced CO2 will reflect the pollutant isotopic signature. Thus, the ratio δ13C(CO2) will come closer to δ13C(hydrocarbon). BIOPHY, project supported by the French National Research Agency (ANR), proposes to use electrical methods and gas analyses to develop an operational and non-destructive method for monitoring in situ biodegradation of hydrocarbons in order to optimize soil treatment. Demonstration field is located in the South of Paris (France), where liquid fuels (gasoline and diesel) leaked from some tanks in 1997. In order to stimulate biodegradation, a trench has been dug to supply oxygen to the water table and thus stimulate aerobic metabolic bioprocesses. ER and

  16. Actinide(IV) and actinide(VI) carbonate speciation studies by PAS and NMR spectroscopies; Yucca Mountain Project: Milestone report 3031-WBS 1.2.3.4.1.3.1

    Energy Technology Data Exchange (ETDEWEB)

    Clark, D.L.; Ekberg, S.A.; Morris, D.E.; Palmer, P.D.; Tait, C.D.

    1994-09-01

    Pulsed-laser photoacoustic spectroscopy (PAS) and Fourier-transform nuclear magnetic resonance (NMR) spectroscopy were used to study speciation of actinide(IV) and actinide(VI) ions (Np, Pu, Am) in aqueous carbonate solutions vs pH, carbonate content, actinide content, temperature. PAS focused on Pu(IV) speciation. Stability fields on a pH (8.4 to 12.0) versus total carbonate content (0.003 to 1.0 M) plot for dilute Pu(IV) carbonate species ([Pu]{sub tot} = 1 mM) were mapped. Four plutonium species, with absorption peaks at 486, 492, 500, and 512 nm were found. Loss of a single carbonate ligand does not account for the difference in speciation for the 486 and 492 nm absorption peaks, nor can any of the observed species be identified as colloidal Pu(IV). NMR data have been obtained for UO{sub 2}{sup 2+}, PuO{sub 2}{sup 2+} and AmO{sub 2}{sup 2+}. This report focuses on results for PuO{sub 2}{sup 2+}. The ligand exchange reaction between free and coordinated carbonate on the PuO{sub 2}(CO{sub 3}){sub 3}{sup 4{minus}} systems has been examined by variable temperature {sup 13}C NMR spectroscopy. In each of the six different PuO{sub 2}(CO{sub 3}){sub 3}{sup 4{minus}} samples, two NMR signals are present, one for the free carbonate ligand and one for the carbonate ligand coordinated to a paramagnetic plutonium metal center. The single{sup 13}C resonance line for coordinated carbonate is consistent with expectations of a monomeric PuO{sub 2}(CO{sub 3}){sub 3}{sup 4{minus}} species in solution. A modified Carr-Purcell-Meiboom-Gill NMR pulse sequence was used for determining ligand exchange parameters for paramagnetic actinide complexes. Eyring analysis at standard conditions provided activation parameters of {Delta}H = 38 KJ/M and {Delta}S = {minus}60 J/K for the plutonyl triscarbonate system, suggesting an associative transition state for the plutonyl(VI) carbonate complex self-exchange reaction.

  17. Isotope and Nuclear Chemistry Division annual report FY 1986, October 1985-September 1986

    Energy Technology Data Exchange (ETDEWEB)

    Heiken, J.H. (ed.)

    1987-06-01

    This report describes progress in the major research and development programs carried out in FY 1986 by the Isotope and Nuclear Chemistry Division. The report includes articles on radiochemical diagnostics and weapons tests; weapons radiochemical diagnostics research and development; other unclassified weapons research; stable and radioactive isotope production and separation; chemical biology and nuclear medicine; element and isotope transport and fixation; actinide and transition metal chemistry; structural chemistry, spectroscopy, and applications; nuclear structure and reactions; irradiation facilities; advanced concepts and technology; and atmospheric chemistry.

  18. Superabsorbing gel for actinide, lanthanide, and fission product decontamination

    Science.gov (United States)

    Kaminski, Michael D.; Mertz, Carol J.

    2016-06-07

    The present invention provides an aqueous gel composition for removing actinide ions, lanthanide ions, fission product ions, or a combination thereof from a porous surface contaminated therewith. The composition comprises a polymer mixture comprising a gel forming cross-linked polymer and a linear polymer. The linear polymer is present at a concentration that is less than the concentration of the cross-linked polymer. The polymer mixture is at least about 95% hydrated with an aqueous solution comprising about 0.1 to about 3 percent by weight (wt %) of a multi-dentate organic acid chelating agent, and about 0.02 to about 0.6 molar (M) carbonate salt, to form a gel. When applied to a porous surface contaminated with actinide ions, lanthanide ions, and/or other fission product ions, the aqueous gel absorbs contaminating ions from the surface.

  19. Radioanalytical determination of actinides and fission products in Belarus soils.

    Science.gov (United States)

    Michel, H; Gasparro, J; Barci-Funel, G; Dalmasso, J; Ardisson, G; Sharovarov, G

    1999-04-01

    Alpha emitting actinides such as plutonium, americium or curium were measured by alpha-spectrometry after radiochemical separation. The short range of alpha-particles within matter requires, after a pre-concentration process, a succession of isolation and purification steps based on the valence states modification of the researched elements. For counting, actinides were electrodeposited in view to obtain the mass-less source necessary to avoid self-absorption of the emitted radiations. Activity concentrations of gamma-emitting fission products were calculated after measurement with high purity germanium detectors (HPGe). These different methods were used to analyse soils sampled in the Republic of Belarus, not far from the Chernobyl nuclear plant.

  20. Accuracy Improvement of Neutron Nuclear Data on Minor Actinides

    Directory of Open Access Journals (Sweden)

    Harada Hideo

    2015-01-01

    Full Text Available Improvement of accuracy of neutron nuclear data for minor actinides (MAs and long-lived fission products (LLFPs is required for developing innovative nuclear system transmuting these nuclei. In order to meet the requirement, the project entitled as “Research and development for Accuracy Improvement of neutron nuclear data on Minor ACtinides (AIMAC” has been started as one of the “Innovative Nuclear Research and Development Program” in Japan at October 2013. The AIMAC project team is composed of researchers in four different fields: differential nuclear data measurement, integral nuclear data measurement, nuclear chemistry, and nuclear data evaluation. By integrating all of the forefront knowledge and techniques in these fields, the team aims at improving the accuracy of the data. The background and research plan of the AIMAC project are presented.

  1. Development of a remote bushing for actinide vitrification

    Energy Technology Data Exchange (ETDEWEB)

    Schumacher, R.F.; Ramsey, W.G.; Johnson, F.M. [and others

    1996-12-31

    The Savannah River Site (SRS) and the Savannah River Technology Center (SRTC) are combining their existing experience in handling highly radioactive, special nuclear materials with commercial glass fiberization technology in order to assemble a small vitrification system for radioactive actinide solutions. The vitrification system or {open_quotes}brushing{close_quotes}, is fabricated from platinum-rhodium alloy and is based on early marble remelt fiberization technology. Advantages of this unique system include its relatively small size, reliable operation, geometrical safety (nuclear criticality), and high temperature capability. The bushing design should be capable of vitrifying a number of the actinide nuclear materials, including solutions of americium/curium, neptunium, and possibly plutonium. State of the art, mathematical and oil model studies are being combined with basic engineering evaluations to verify and improve the thermal and mechanical design concepts.

  2. Status of measurements of fission neutron spectra of Minor Actinides

    Energy Technology Data Exchange (ETDEWEB)

    Drapchinsky, L.; Shiryaev, B. [V.G. Khlopin Radium Inst., Saint Petersburg (Russian Federation)

    1997-03-01

    The report considers experimental and theoretical works on studying the energy spectra of prompt neutrons emitted in spontaneous fission and neutron induced fission of Minor Actinides. It is noted that neutron spectra investigations were done for only a small number of such nuclei, most measurements, except those of Cf-252, having been carried out long ago by obsolete methods and imperfectapparatus. The works have no detailed description of experiments, analysis of errors, detailed numerical information about results of experiments. A conclusion is made that the available data do not come up to modern requirements. It is necessary to make new measurements of fission prompt neutron spectra of transuranium nuclides important for the objectives of working out a conception of minor actinides transmutation by means of special reactors. (author)

  3. Comparative Study of f-Element Electronic Structure across a Series of Multimetallic Actinide, Lanthanide-Actinide and Lanthanum-Actinide Complexes Possessing Redox-Active Bridging Ligands

    Energy Technology Data Exchange (ETDEWEB)

    Schelter, Eric J.; Wu, Ruilian; Veauthier, Jacqueline M.; Bauer, Eric D.; Booth, Corwin H.; Thomson, Robert K.; Graves, Christopher R.; John, Kevin D.; Scott, Brian L.; Thompson, Joe D.; Morris, David E.; Kiplinger, Jaqueline L.

    2010-02-24

    A comparative examination of the electronic interactions across a series of trimetallic actinide and mixed lanthanide-actinide and lanthanum-actinide complexes is presented. Using reduced, radical terpyridyl ligands as conduits in a bridging framework to promote intramolecular metal-metal communication, studies containing structural, electrochemical, and X-ray absorption spectroscopy are presented for (C{sub 5}Me{sub 5}){sub 2}An[-N=C(Bn)(tpy-M{l_brace}C{sub 5}Me4R{r_brace}{sub 2})]{sub 2} (where An = Th{sup IV}, U{sup IV}; Bn = CH{sub 2}C{sub 6}H{sub 5}; M = La{sup III}, Sm{sup III}, Yb{sup III}, U{sup III}; R = H, Me, Et) to reveal effects dependent on the identities of the metal ions and R-groups. The electrochemical results show differences in redox energetics at the peripheral 'M' site between complexes and significant wave splitting of the metal- and ligand-based processes indicating substantial electronic interactions between multiple redox sites across the actinide-containing bridge. Most striking is the appearance of strong electronic coupling for the trimetallic Yb{sup III}-U{sup IV}-Yb{sup III}, Sm{sup III}-U{sup IV}-Sm{sup III}, and La{sup III}-U{sup IV}-La{sup III} complexes, [8]{sup -}, [9b]{sup -} and [10b]{sup -}, respectively, whose calculated comproportionation constant K{sub c} is slightly larger than that reported for the benchmark Creutz-Taube ion. X-ray absorption studies for monometallic metallocene complexes of U{sup III}, U{sup IV}, and U{sup V} reveal small but detectable energy differences in the 'white-line' feature of the uranium L{sub III}-edges consistent with these variations in nominal oxidation state. The sum of this data provides evidence of 5f/6d-orbital participation in bonding and electronic delocalization in these multimetallic f-element complexes. An improved, high-yielding synthesis of 4{prime}-cyano-2,2{prime}:6{prime},2{double_prime}-terpyridine is also reported.

  4. A method for the determination of bacterial spore DNA content based on isotopic labelling, spore germination and diphenylamine assay; ploidy of spores of several Bacillus species.

    Science.gov (United States)

    Hauser, P M; Karamata, D

    1992-01-01

    A reliable method for measuring the spore DNA content, based on radioactive DNA labelling, spore germination in absence of DNA replication and diphenylamine assay, was developed. The accuracy of the method, within 10-15%, is adequate for determining the number of chromosomes per spore, provided that the genome size is known. B subtilis spores were shown to be invariably monogenomic, while those of larger bacilli Bacillus megaterium, Bacillus cereus and Bacillus thuringiensis, often, if not invariably, contain two genomes. Attempts to modify the spore DNA content of B subtilis by altering the richness of the sporulation medium, the sporulation conditions (liquid or solid medium), or by mutation, were apparently unsuccessful. An increase of spore size with medium richness, not accompanied by an increase in DNA content, was observed. The implication of the apparently species-specific spore ploidy and the influence of the sporulation conditions on spore size and shape are discussed.

  5. EXAFS studies of actinide ions in aqueous solution

    Energy Technology Data Exchange (ETDEWEB)

    Karim, D P; Georgopoulos, P; Knapp, G S

    1979-01-01

    The applicability of the EXAFS technique in the study of actinide systems is discussed. Uranium L/sub III/-edge spectra obtained on an in-lab rotating anode EXAFS facility are presented and analyzed for crystalline UO/sub 2/F/sub 2/ and aqueous solutions containing hexavalent uranium ions. Methods for the extension of the technique to more dilute systems are discussed.

  6. Future nuclear fuel cycles: Prospect and challenges for actinide recycling

    Science.gov (United States)

    Warin, Dominique

    2010-03-01

    The global energy context pleads in favour of a sustainable development of nuclear energy since the demand for energy will likely increase, whereas resources will tend to get scarcer and the prospect of global warming will drive down the consumption of fossil fuel. In this context, nuclear power has the worldwide potential to curtail the dependence on fossil fuels and thereby to reduce the amount of greenhouse gas emissions while promoting energy independence. How we deal with nuclear radioactive waste is crucial in this context. In France, the public's concern regarding the long-term waste management made the French Governments to prepare and pass the 1991 and 2006 Acts, requesting in particular the study of applicable solutions for still minimizing the quantity and the hazardousness of final waste. This necessitates High Active Long Life element (such as the Minor Actinides MA) recycling, since the results of fuel cycle R&D could significantly change the challenges for the storage of nuclear waste. HALL recycling can reduce the heat load and the half-life of most of the waste to be buried to a couple of hundred years, overcoming the concerns of the public related to the long-life of the waste and thus aiding the "burying approach" in securing a "broadly agreed political consensus" of waste disposal in a geological repository. This paper presents an overview of the recent R and D results obtained at the CEA Atalante facility on innovative actinide partitioning hydrometallurgical processes. For americium and curium partitioning, these results concern improvements and possible simplifications of the Diamex-Sanex process, whose technical feasibility was already demonstrated in 2005. Results on the first tests of the Ganex process (grouped actinide separation for homogeneous recycling) are also discussed. In the coming years, next steps will involve both better in-depth understanding of the basis of these actinide partitioning processes and, for the new promising

  7. Validation of minor actinides fission neutron cross-sections

    Directory of Open Access Journals (Sweden)

    Pešić Milan P.

    2015-01-01

    Full Text Available Verification of neutron fission cross-sections of minor actinides from some recently available evaluated nuclear data libraries was carried out by comparison of the reaction rates calculated by the MCNP6.1 computer code to the experimental values. The experimental samples, containing thin layers of 235U, 237Np, 238,239,240,241Pu, 242mAm, 243Cm, 245Cm, and 247Cm, deposited on metal support and foils of 235U (pseudo-alloy 27Al + 235U, 238U, natIn, 64Zn, 27Al, and multi-component sample alloy 27Al + 55Mn + natCu + natLu + 197Au, were irradiated in the channels of the tank containing fluorine salts 0.52NaF + 0.48ZrF4, labelled as the Micromodel Salt Blanket, inserted in the lattice centre of the MAKET heavy water critical assembly at the Institute for Theoretical and Experimental Physics, Moscow. This paper is a continuation of earlier initiated scientific-research activities carried out for validation of the evaluated fission cross-sections of actinides that were supposed to be used for the quality examination of the fuel design of the accelerator driven systems or fast reactors, and consequently, determination of transmutation rates of actinides, and therefore, determination of operation parameters of these reactor facilities. These scientific-research activities were carried out within a frame of scientific projects supported by the International Science and Technology Center and the International Atomic Energy Agency co-ordinated research activities, from 1999 to 2010. Obtained results confirm that further research is needed in evaluations in order to establish better neutron cross-section data for the minor actinides and selected nuclides which could be used in the accelerator driven systems or fast reactors.

  8. Chemical and Ceramic Methods Toward Safe Storage of Actinides

    Energy Technology Data Exchange (ETDEWEB)

    P.E.D. Morgan; R.M. Housley; J.B. Davis; M.L. DeHaan

    2005-08-19

    A very import, extremely-long-term, use for monazite as a radwaste encapsulant has been proposed. THe use of ceramic La-monazite for sequestering actinides (isolating them from the environment), especially plutonium and some other radioactive elements )e.g., fission-product rare earths), had been especially championed by Lynn Boatner of ORNL. Monazite may be used alone or, copying its compatibility with many other minerals in nature, may be used in diverse composite combinations.

  9. Chemical properties of the heavier actinides and transactinides

    Energy Technology Data Exchange (ETDEWEB)

    Hulet, E.K.

    1981-01-01

    The chemical properties of each of the elements 99 (Es) through 105 are reviewed and their properties correlated with the electronic structure expected for 5f and 6d elements. A major feature of the heavier actinides, which differentiates them from the comparable lanthanides, is the increasing stability of the divalent oxidation state with increasing atomic number. The divalent oxidation state first becomes observable in the anhydrous halides of californium and increases in stability through the series to nobelium, where this valency becomes predominant in aqueous solution. In comparison with the analogous 4f electrons, the 5f electrons in the latter part of the series are more tightly bound. Thus, there is a lowering of the 5f energy levels with respect to the Fermi level as the atomic number increases. The metallic state of the heavier actinides has not been investigated except from the viewpoint of the relative volatility among members of the series. In aqueous solutions, ions of these elements behave as a normal trivalent actinides and lanthanides (except for nobelium). Their ionic radii decrease with increasing nuclear charge which is moderated because of increased screening of the outer 6p electrons by the 5f electrons. The actinide series of elements is completed with the element lawrencium (Lr) in which the electronic configuration is 5f/sup 14/7s/sup 2/7p. From Mendeleev's periodicity and Dirac-Fock calculations, the next group of elements is expected to be a d-transition series corresponding to the elements Hf through Hg. The chemical properties of elements 104 and 105 only have been studied and they indeed appear to show the properties expected of eka-Hf and eka-Ta. However, their nuclear lifetimes are so short and so few atoms can be produced that a rich variety of chemical information is probably unobtainable.

  10. A literature review of actinide-carbonate mineral interactions

    Energy Technology Data Exchange (ETDEWEB)

    Stout, D.L. [Missouri Univ., Columbia, MO (United States). Dept. of Geological Sciences; Carroll, S.A. [Lawrence Livermore National Lab., CA (United States)

    1993-10-01

    Chemical retardation of actinides in groundwater systems is a potentially important mechanism for assessing the performance of the Waste Isolation Pilot Plant (WIPP), a facility intended to demonstrate safe disposal of transuranic waste. Rigorous estimation of chemical retardation during transport through the Culebra Dolomite, a water-bearing unit overlying the WIPP, requires a mechanistic understanding of chemical reactions between dissolved elements and mineral surfaces. This report represents a first step toward this goal by examining the literature for pertinent experimental studies of actinide-carbonate interactions. A summary of existing models is given, along with the types of experiments on which these models are based. Articles pertaining to research into actinide interactions with carbonate minerals are summarized. Select articles involving trace element-carbonate mineral interactions are also reviewed and may serve as templates for future research. A bibliography of related articles is included. Americium(III), and its nonradioactive analog neodymium(III), partition strongly from aqueous solutions into carbonate minerals. Recent thermodynamic, kinetic, and surface studies show that Nd is preferentially removed from solution, forming a Nd-Ca carbonate solid solution. Neptunium(V) is rapidly removed from solution by carbonates. Plutonium incorporation into carbonates is complicated by multiple oxidation states. Little research has been done on the radium(H) and thorium(IV) carbonate systems. Removal of uranyl ion from solution by calcite is limited to monolayer surface coverage.

  11. Crystalline matrices for the immobilization of plutonium and actinides

    Energy Technology Data Exchange (ETDEWEB)

    Anderson, E.B.; Burakov, E.E.; Galkin, Ya.B.; Starchenko, V.A.; Vasiliev, V.G. [V.G. Khlopin Radium Institute, St. Petersburg (Russian Federation)

    1996-05-01

    The management of weapon plutonium, disengaged as a result of conversion, is considered together with the problem of the actinide fraction of long-lived high level radioactive wastes. It is proposed to use polymineral ceramics based on crystalline host-phases: zircon ZrSiO{sub 4} and zirconium dioxide ZrO{sub 2}, for various variants of the management of plutonium and actinides (including the purposes of long-term safe storage or final disposal from the human activity sphere). It is shown that plutonium and actinides are able to form with these phases on ZrSiO{sub 4} and ZrO{sub 2} was done on laboratory level by the hot pressing method, using the plasmochemical calcination technology. To incorporate simulators of plutonium into the structure of ZrSiO{sub 4} and ZrO{sub 2} in the course of synthesis, an original method developed by the authors as a result of studying the high-uranium zircon (Zr,U) SiO{sub 4} form Chernobyl {open_quotes}lavas{close_quotes} was used.

  12. Actinides and lanthanides under pressure: the pseudopotential approach; Actinides et terres rares sous pression: approche pseudopotentiel

    Energy Technology Data Exchange (ETDEWEB)

    Richard, N

    2002-07-01

    In the Density Functional Theory Framework, the pseudopotential formalism offers a broader scope of study than other theoretical methods such as global relaxation of the parameters of the cell or ab initio molecular dynamics simulations. This method has been widely used to study light elements or transition metals but never to study f elements. We have generated two non local norm conserving Trouillier-Martins pseudopotentials (one in LDA and one in GGA) for the cerium. To check the validity of the pseudopotentials, we have calculated the equilibrium volume and the incompressibility modulus and compared our results to previous all-electron calculations. If the GGA and non linear core corrections are used, the equation of state is in a good agreement with the experimental equation of state. A static study of the previously proposed high pressure phases give a transitions fcc-a''(I)-bct. Using the pseudopotentials we have generated, an ab initio molecular dynamics simulation at constant pressure, in the region between 5 and 12 GPa where the stable phase of cerium is not well defined, lead us to predict that a centred monoclinic structure, as the a''(I) phase previously observed in some experiments, is the most stable phase. We have also generated pseudopotentials for the light actinides (Th, Pa, U and Np). We have study their phase transitions under pressure at zero temperature. We compared our results with all electron results. The structure parameters have always been relaxed in this study. And for the first time in pseudopotential calculation, the spin-orbit coupling has been taken into account. The curves describing the variation of the volume or the incompressibility modulus depending on the elements and the phase transitions are always in agreement with the one found in the all electron calculations. (author)

  13. Utilization of Minor Actinides (Np, Am, Cm) in Nuclear Power Reactor

    Science.gov (United States)

    Gerasimov, A.; Bergelson, B.; Tikhomirov, G.

    2014-06-01

    Calculation research of the utilization process of minor actinides (transmutation with use of power released) is performed for specialized power reactor of the VVER type operating on the level of electric power of 1000 MW. Five subsequent cycles are considered for the reactor with fuel elements containing minor actinides along with enriched uranium. It was shown that one specialized reactor for the one cycle (900 days) can utilize minor actinides from several VVER-1000 reactors without any technological and structural modifications. Power released because of minor actinide fission is about 4% with respect to the total power

  14. The low-energy dipole structure of 232Th , 236U and 238U actinide nuclei

    Science.gov (United States)

    Kuliev, A. A.; Guliyev, E.; Ertugral, F.; Özkan, S.

    2010-03-01

    In this study, ensuremath I^{π} = 1+ and ensuremath I^{π} = 1- dipole mode excitations are systematically investigated within the rotational and translational + Galilean invariant quasiparticle random-phase approximation for 232Th , 236U , and 238U actinide nuclei. It is shown that the investigated nuclei reach a B( M1) strength structure, which corresponds to the scissors mode. The calculated mean excitation energies as well as the summed B( M1) value of the scissors mode excitations are consistent with the available experimental data. The results of calculations indicate large differences to the rare-earth nuclei as is the case for the experiment: a doubling of the observed dipole strengths and a shift of the energy centroid to the lower energies by about 800keV. The calculations indicate the presence of a few prominent negative-parity ensuremath K^{π} = 1- states in the 2.0-4.0MeV energy interval. The occurrence of the negative-parity dipole states with the rather high B( E1) value less than 4MeV shows the necessity of explicit parity measurements for the correct determination of the scissors mode strength in 232Th , 236U , and 238U isotopes.

  15. Minimization of actinide waste by multi-recycling of thoriated fuels in the EPR reactor

    Science.gov (United States)

    Rose, S. J.; Wilson, J. N.; Capellan, N.; David, S.; Guillemin, P.; Ivanov, E.; Méplan, O.; Nuttin, A.; Siem, S.

    2012-02-01

    The multi-recycling of innovative uranium/thorium oxide fuels for use in the European Pressurized water Reactor (EPR) has been investigated. If increasing quantities of 238U, the fertile isotope in standard UO2 fuel, are replaced by 232Th, then a greater yield of new fissile material (233U) is produced during the cycle than would otherwise be the case. This leads to economies of natural uranium of around 45% if the uranium in the spent fuel is multi-recycled. In addition we show that minor actinide and plutonium waste inventories are reduced and hence waste radio-toxicities and decay heats are up to a factor of 20 lower after 103 years. Two innovative fuel types named S90 and S20, ThO2 mixed with 90% and 20% enriched UO2 respectively, are compared as an alternative to standard uranium oxide (UOX) and uranium/plutonium mixed oxide (MOX) fuels at the longest EPR fuel discharge burn-ups of 65 GWd/t. Fissile and waste inventories are examined, waste radio-toxicities and decay heats are extracted and safety feedback coefficients are calculated.

  16. Minimization of actinide waste by multi-recycling of thoriated fuels in the EPR reactor

    Directory of Open Access Journals (Sweden)

    Nuttin A.

    2012-02-01

    Full Text Available The multi-recycling of innovative uranium/thorium oxide fuels for use in the European Pressurized water Reactor (EPR has been investigated. If increasing quantities of 238U, the fertile isotope in standard UO2 fuel, are replaced by 232Th, then a greater yield of new fissile material (233U is produced during the cycle than would otherwise be the case. This leads to economies of natural uranium of around 45% if the uranium in the spent fuel is multi-recycled. In addition we show that minor actinide and plutonium waste inventories are reduced and hence waste radio-toxicities and decay heats are up to a factor of 20 lower after 103 years. Two innovative fuel types named S90 and S20, ThO2 mixed with 90% and 20% enriched UO2 respectively, are compared as an alternative to standard uranium oxide (UOX and uranium/plutonium mixed oxide (MOX fuels at the longest EPR fuel discharge burn-ups of 65 GWd/t. Fissile and waste inventories are examined, waste radio-toxicities and decay heats are extracted and safety feedback coefficients are calculated.

  17. Recycled oceanic crust and marine sediment in the source of alkali basalts in Shandong, eastern China: Evidence from magma water content and oxygen isotopes

    Science.gov (United States)

    Liu, Jia; Xia, Qun-Ke; Deloule, Etienne; Chen, Huan; Feng, Min

    2015-12-01

    The magma water contents and cpx δ18O values in alkali basalts from the Fuyanyshan (FYS) volcano in Shandong, eastern China, were investigated by an inverse calculation based on the water content of clinopyroxene (cpx) phenocrysts, the ivAlcpx-dependent water partitioning coefficient Dwatercpx>/melt, and secondary ion mass spectrometer, respectively. The calculated water content (H2O wt.) of magma ranges from 0.58% to 3.89%. It positively correlates with heavy rare earth element concentrations and bulk rock 87Sr/86Sr ratios, and it negatively correlates with Nb/U ratios. However, it is not correlated with bulk Mg# (Mg# = 100 × Mg / (Mg + Fe)) and (La/Yb)n (n represents primitive mantle normalization). Combined with the rather homogenous distribution of water content within cpx grains, these correlations indicate that the water variations among different samples represent the original magma signature, rather than results of a shallow process, such as degassing and diffusion. The δ18O of cpx phenocrysts varies from 3.6‰ to 6.3‰ (±0.5‰, 2SD), which may be best explained by the involvement of components from the lower and upper oceanic crust with marine sediments within the mantle source. The H2O/Ce ratios of the calculated melts range from 113 to 696 and form a positive trend with bulk rock 87Sr/86Sr, which cannot be explained by the recycled Sulu eclogite or by the metasomatized lithospheric mantle. Our modeling calculation shows that the decoupling of ɛHf and ɛNd could be caused by the involvement of marine sediments. Combing the high Ba/Th ratios, positive Sr spikes, and low Ce/Pb ratios for the Fuyanshan basalts, we suggest that the hydrous nature of the FYS basalts was derived from the hydrous mantle transition zone with ancient sediments.

  18. Gas Generation from Actinide Oxide Materials

    Energy Technology Data Exchange (ETDEWEB)

    George Bailey; Elizabeth Bluhm; John Lyman; Richard Mason; Mark Paffett; Gary Polansky; G. D. Roberson; Martin Sherman; Kirk Veirs; Laura Worl

    2000-12-01

    This document captures relevant work performed in support of stabilization, packaging, and long term storage of plutonium metals and oxides. It concentrates on the issue of gas generation with specific emphasis on gas pressure and composition. Even more specifically, it summarizes the basis for asserting that materials loaded into a 3013 container according to the requirements of the 3013 Standard (DOE-STD-3013-2000) cannot exceed the container design pressure within the time frames or environmental conditions of either storage or transportation. Presently, materials stabilized and packaged according to the 3013 Standard are to be transported in certified packages (the certification process for the 9975 and the SAFKEG has yet to be completed) that do not rely on the containment capabilities of the 3013 container. Even though no reliance is placed on that container, this document shows that it is highly likely that the containment function will be maintained not only in storage but also during transportation, including hypothetical accident conditions. Further, this document, by summarizing materials-related data on gas generation, can point those involved in preparing Safety Analysis Reports for Packages (SARPs) to additional information needed to assess the ability of the primary containment vessel to contain the contents and any reaction products that might reasonably be produced by the contents.

  19. Transmutation of minor actinides discharged from LMFBR spent fuel in a high power density fusion reactor

    Energy Technology Data Exchange (ETDEWEB)

    Uebeyli, Mustafa E-mail: mubeyli@gazi.edu.tr

    2004-12-01

    Significant amounts of nuclear wastes consisting of plutonium, minor actinides and long lived fission products are produced during the operation of commercial nuclear power plants. Therefore, the destruction of these wastes is very important with respect to public health, environment and also the future of nuclear energy. In this study, transmutation of minor actinides (MAs) discharged from LMFBR spent fuel in a high power density fusion reactor has been investigated under a neutron wall load of 10 MW/m{sup 2} for an operation period of 10 years. Also, the effect of MA percentage on the transmutation has been examined. The fuel zone, containing MAs as spheres cladded with W-5Re, has been located behind the first wall to utilize the high neutron flux for transmutation effectively. Helium at 40 atm has been used as an energy carrier. At the end of the operation period, the total burning and transmutation are greater than the total buildups in all investigated cases, and very high burnups (420-470 GWd/tHM) are reached, depending on the MA content. The total transmutation rate values are 906 and 979 kg/GW{sub th} year at startup and decrease to 140 and 178 kg/GW{sub th} year at the end of the operation for fuel with 10% and 20% MA, respectively. Over an operation period of 10 years, the effective half lives decrease from 2.38, 2.21 and 3.08 years to 1.95, 1.80 and 2.59 years for {sup 237}Np, {sup 241}Am and {sup 243}Am, respectively. Total atomic densities decrease exponentially during the operation period. The reductions in the total atomic densities with respect to the initial ones are 79%, 81%, 82%, 83%, 85% and 86% for 10%, 12%, 14%, 16%, 18% and 20% MAs, respectively.

  20. Isotopic Generation and Confirmation of the PWR Application Model 

    Energy Technology Data Exchange (ETDEWEB)

    L.B. Wimmer

    2003-11-10

    The objective of this calculation is to establish an isotopic database to represent commercial spent nuclear fuel (CSNF) from pressurized water reactors (PWRs) in criticality analyses performed for the proposed Monitored Geologic Repository at Yucca Mountain, Nevada. Confirmation of the conservatism with respect to criticality in the isotopic concentration values represented by this isotopic database is performed as described in Section 3.5.3.1.2 of the ''Disposal Criticality Analysis Methodology Topical Report'' (YMP 2000). The isotopic database consists of the set of 14 actinides and 15 fission products presented in Section 3.5.2.1.1 of YMP 2000 for use in CSNF burnup credit. This set of 29 isotopes is referred to as the principal isotopes. The oxygen isotope from the UO{sub 2} fuel is also included in the database. The isotopic database covers enrichments of {sup 235}U ranging from 1.5 to 5.5 weight percent (wt%) and burnups ranging from approximately zero to 75 GWd per metric ton of uranium (mtU). The choice of fuel assembly and operating history values used in generating the isotopic database are provided is Section 5. Tables of isotopic concentrations for the 29 principal isotopes (plus oxygen) as a function of enrichment and burnup are provided in Section 6.1. Results of the confirmation of the conservatism with respect to criticality in the isotopic concentration values are provided in Section 6.2.

  1. Actinide Foil Production for MPACT Research

    Energy Technology Data Exchange (ETDEWEB)

    Beller, Denis

    2012-10-30

    Sensitive fast-neutron detectors are required for use in lead slowing down spectrometry (LSDS), an active interrogation technique for used nuclear fuel assay for Materials Protection, Accounting, and Controls Technologies (MPACT). During the past several years UNLV sponsored a research project at RPI to investigate LSDS; began development of fission chamber detectors for use in LSDS experiments in collaboration with INL, LANL, and Oregon State U.; and participated in a LSDS experiment at LANL. In the LSDS technique, research has demonstrated that these fission chamber detectors must be sensitive to fission energy neutrons but insensitive to thermal-energy neutrons. Because most systems are highly sensitive to large thermal neutron populations due to the well-known large thermal cross section of 235U, even a miniscule amount of this isotope in a fission chamber will overwhelm the small population of higher-energy neutrons. Thus, fast-fission chamber detectors must be fabricated with highly depleted uranium (DU) or ultra-pure thorium (Th), which is about half as efficient as DU. Previous research conducted at RPI demonstrated that the required purity of DU for assay of used nuclear fuel using LSDS is less than 4 ppm 235U, material that until recently was not available in the U.S. In 2009 the PI purchased 3 grams of ultra-depleted uranium (uDU, 99.99998% 238U with just 0.2 ± 0.1 ppm 235U) from VNIIEF in Sarov, Russia. We received the material in the form of U3O8 powder in August of 2009, and verified its purity and depletion in a FY10 MPACT collaboration project. In addition, chemical processing for use in FC R&D was initiated, fission chamber detectors and a scanning alpha-particle spectrometer were developed, and foils were used in a preliminary LSDS experiment at a LANL/LANSCE in Sept. of 2010. The as-received U3O8 powder must be chemically processed to convert it to another chemical form while maintaining its purity, which then must be used to electro-deposit U

  2. Lichens as a useful mapping tool?--an approach to assess atmospheric N loads in Germany by total N content and stable isotope signature.

    Science.gov (United States)

    Boltersdorf, Stefanie H; Werner, Willy

    2014-08-01

    To assess whether nitrogen (N) content and δ(15)N ratios in nitrophytic lichen species (Xanthoria parietina (L.) Th. Fr. (1860) and Physcia spp. (Schreb.) Michaux (1803)) reflect the quantity and quality of atmospheric N loads, 348 lichen samples from 174 sampling grid cells were investigated in the western part of Germany. The analysed lichen N content ranged between 0.98 and 4.28 % and δ(15)N ratios between -15.2 and -1.3 ‰. Based on the N concentrations and the δ(15)N ratios of lichens, different landscape categories and coupled N deposition rates could be inferred for different regions of Germany. By analysing environmental variables like altitude, ammonia emission density, livestock unit and different defined deposition types, a direct relationship was found between lichen chemistry and N compounds produced from agricultural activity. The results support the development of a monitoring method which could be used nationally or even internationally to support current N deposition measurements, by providing reliable information on the quantity and quality of N deposition in high N environments.

  3. Leatherback Isotopes

    Data.gov (United States)

    National Oceanic and Atmospheric Administration, Department of Commerce — SWFSC is currently working on a project identifying global marine isotopes using leatherback turtles (Dermochelys coriacea) as the indicator species. We currently...

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

    Science.gov (United States)

    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

  5. Isotopic Paleoclimatology

    Science.gov (United States)

    Bowen, R.

    Paleotemperature scales were calculated by H. C. Urey and others in the 1950s to assess past temperatures, and later work using the stable isotopes of oxygen, hydrogen, and carbon employed standards such as Peedee belemnite (PDB) and Standard Mean Ocean Water (SMOW). Subsequently, subjects as diverse as ice volume and paleotemperatures, oceanic ice and sediment cores, Pleistocene/Holocene climatic changes, and isotope chronostratigraphy extending back to the Precambrian were investigated.

  6. Isotopic chirality

    Energy Technology Data Exchange (ETDEWEB)

    Floss, H.G. [Univ. of Washington, Seattle, WA (United States)

    1994-12-01

    This paper deals with compounds that are chiral-at least in part, due to isotope substitution-and their use in tracing the steric course of enzyme reaction in vitro and in vivo. There are other applications of isotopically chiral compounds (for example, in analyzing the steric course of nonenzymatic reactions and in probing the conformation of biomolecules) that are important but they will not be discussed in this context.

  7. Invisible structures in the X-ray absorption spectra of actinides

    NARCIS (Netherlands)

    Kvashnina, Kristina O.; De Groot, Frank M F

    2014-01-01

    The X-ray absorption spectra of actinides are discussed with an emphasis on the fundamental effects that influence their spectral shape, including atomic multiplet theory, charge transfer theory and crystal field theory. Many actinide spectra consist of a single peak and it is shown that the use of

  8. Actinide Partitioning and Transmutation Program. Progress report, April 1--June 30, 1977

    Energy Technology Data Exchange (ETDEWEB)

    Tedder, D. W.; Blomeke, J. O. [comps.

    1977-10-01

    Experimental work on the 16 tasks comprising the Actinide Partitioning and Transmutation Program was continued. Summaries of work are given on Purex Process modifications, actinide recovery, Am-Cm recovery, radiation effects on ion exchangers, LMFBR transmutation studies, thermal reactor transmutation studies, fuel cycle studies, and partitioning-transmutation evaluation. (JRD)

  9. Systematic Characteristics of Fast Neutron Fission Cross Sections for Actinide Nuclei

    Institute of Scientific and Technical Information of China (English)

    2011-01-01

    The neutron fission cross sections of actinide nuclei are important data for the design of nuclear reactor and nuclear engineering, and so on. So far, there has been a certain amount of experimental data for the fission cross sections of actinide nuclei. However,

  10. Fractionation behavior of chromium isotopes during coprecipitation with calcium carbonate

    DEFF Research Database (Denmark)

    Rodler, Alexandra; Sánchez-Pastor, Nuria; Fernández-Díaz, Lurdes;

    2015-01-01

    Interest in chromium (Cr) isotope incorporation into carbonates arises from the observation that Cr isotopic composition of carbonates could be used as a paleoclimate proxy to elucidate past fluctuations of oxygen contents in atmosphere and hydrosphere. The use of Cr isotopes to track paleoenviro......Interest in chromium (Cr) isotope incorporation into carbonates arises from the observation that Cr isotopic composition of carbonates could be used as a paleoclimate proxy to elucidate past fluctuations of oxygen contents in atmosphere and hydrosphere. The use of Cr isotopes to track...

  11. Impurities that cause difficulty in stripping actinides from commercial tetraalkylcarbamoylmethylphosphonates

    Energy Technology Data Exchange (ETDEWEB)

    Bahner, C. T.; Shoun, R. R.; McDowell, W. J.

    1977-09-01

    Dihexyl((diethylcarbamoyl)methyl)phosphonate (DHDECMP) in diethylbenzene extracts actinides well from 6 M nitric acid solution, but commercially available DHDECMP contains impurities which interfere with stripping the actinides from the organic extract. DHDECMP purified by molecular distillation does not contain these impurities, but the pot residue contains increased concentrations of them. Heating the purified DHDECMP causes the formation of products which interfere with stripping in the same way, suggesting that high temperatures employed in the manufacture of DHDECMP may produce the offending impurities. These impurities can be separated from the heat-decomposed material or the pot residues by dilution with a large volume of hexanes (causing part of the impurities to separate as a second liquid phase) followed by equilibration of the hexane solution with dilute alkali. After the treatment with hexane and dilute alkali, the DHDECMP is readily recovered and functions well in the actinide extraction process. Dibutyl((dibutylcarbamoyl)methyl)-phosphonate (DBDBCMP) and di(2-ethylhexyl)((diethylcarbamoyl)-methyl)phosphonate (DEHDECMP) are purified less effectively by these methods. Similar separation methods using diethylbenzene or CCl/sub 4/ as solvent do not remove impurities as completely as the hexane process. Impurities can also be removed from a benzene solution of the DHDECMP pot residue by passing it through a column packed with silica gel or diethylaminoethyl cellulose. These impurities have been separated into fractions for analytical examination by use of various solvents and by column chromatography. Hexyl hydrogen ((diethylcarbamoyl)methyl)-phosphonate has been identified tentatively as a principal objectionable impurity. Dihexyl phosphoric acid and possibly dihexylphosphonate have been identified in other fractions.

  12. MINOR ACTINIDE SEPARATIONS USING ION EXCHANGERS OR IONIC LIQUIDS

    Energy Technology Data Exchange (ETDEWEB)

    Hobbs, D.; Visser, A.; Bridges, N.

    2011-09-20

    This project seeks to determine if (1) inorganic-based ion exchange materials or (2) electrochemical methods in ionic liquids can be exploited to provide effective Am and Cm separations. Specifically, we seek to understand the fundamental structural and chemical factors responsible for the selectivity of inorganic-based ion-exchange materials for actinide and lanthanide ions. Furthermore, we seek to determine whether ionic liquids can serve as the electrolyte that would enable formation of higher oxidation states of Am and other actinides. Experiments indicated that pH, presence of complexants and Am oxidation state exhibit significant influence on the uptake of actinides and lanthanides by layered sodium titanate and hybrid zirconium and tin phosphonate ion exchangers. The affinity of the ion exchangers increased with increasing pH. Greater selectivity among Ln(III) ions with sodium titanate materials occurs at a pH close to the isoelectric potential of the ion exchanger. The addition of DTPA decreased uptake of Am and Ln, whereas the addition of TPEN generally increases uptake of Am and Ln ions by sodium titanate. Testing confirmed two different methods for producing Am(IV) by oxidation of Am(III) in ionic liquids (ILs). Experimental results suggest that the unique coordination environment of ionic liquids inhibits the direct electrochemical oxidation of Am(III). The non-coordinating environment increases the oxidation potential to a higher value, while making it difficult to remove the inner coordination of water. Both confirmed cases of Am(IV) were from the in-situ formation of strong chemical oxidizers.

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

    Energy Technology Data Exchange (ETDEWEB)

    Jarvinen, G.; Barrans, R.; Schroeder, N.; Wade, K.; Jones, M.; Smith, B.F. [Los Alamos National Lab., NM (United States); Mills, J.; Howard, G. [Texas Tech Univ., Lubbock, TX (United States); Freiser, H.; Muralidharan, S. [Arizona Univ., Tucson, AZ (United States)

    1995-01-01

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

  14. Studies on the properties of hard-spectrum, actinide fissioning reactors. Final report

    Energy Technology Data Exchange (ETDEWEB)

    Nelson, J.B.; Prichard, A.W.; Schofield, P.E.; Robinson, A.H.; Spinrad, B.I.

    1980-01-01

    It is technically feasible to construct an operable (e.g., safe and stable) reactor to burn waste actinides rapidly. The heart of the concept is a driver core of EBR-II type, with a central radial target zone in which fuel elements, made entirely of waste actinides are exposed. This target fuel undergoes fission, as a result of which actinides are rapidly destroyed. Although the same result could be achieved in more conventionally designed LWR or LMFBR systems, the fast spectrum reactor does a much more efficient job, by virtue of the fact that in both LWR and LMFBR reactors, actinide fission is preceded by several captures before a fissile nuclide is formed. In the fast spectrum reactor that is called ABR (actinide burning reactor), these neutron captures are short-circuited.

  15. Actinide collisions for QED and superheavy elements with the time-dependent Hartree-Fock theory and the Balian-Vénéroni variational principle

    Science.gov (United States)

    Simenel, Cédric; Golabek, Cédric; Kedziora, David J.

    2011-10-01

    nuclei (Z > 100) in the collision of prolate deformed actinides such as 232Th+250Cf. The collision of the tip of one nucleus with the side of the other results in a nucleon flux toward the latter. The probability distributions for transfermium production in such a collision are computed. The produced nuclei are more neutron-rich than those formed in fusion reactions, thus, leading to more stable isotopes closer to the predicted superheavy island of stability. In addition to mass and charge dispersion, the Balian-Veneroni variational principle is used to compute correlations between Z and N distributions, which are zero in standard TDHF calculations.

  16. Surface energy and work function of the light actinides

    DEFF Research Database (Denmark)

    Kollár, J.; Vitos, Levente; Skriver, Hans Lomholt

    1994-01-01

    We have calculated the surface energy and work function of the light actinides Fr, Ra, Ac, Th, Pa, U, Np, and Pu by means of a Green's-function technique based on the linear-muffin-tin-orbitals method within the tight-binding representation. In these calculations we apply an energy functional which...... combines the kinetic energy calculated within the atomic-sphere approximation with Coulomb- and exchange-correlation-energy terms calculated by means of the complete nonspherically symmetric charge density derived from the atomic-sphere potential within nonoverlapping and space-filling cells....... The calculated surface energies and work functions are in good agreement with the limited experimental data....

  17. Fission of actinides using a table-top laser

    CERN Document Server

    Schwoerer, H; Sauerbrey, R; Galy, J; Magill, J; Rondinella, V; Schenkel, R; Butz, T

    2003-01-01

    Powerful table-top lasers are now available in the laboratory and can be used to induce nuclear reactions. We report the first demonstration of nuclear fission using a high repetition rate table-top laser with intensities of 10 sup 2 sup 0 W/cm sup 2. Actinide photo-fission has been achieved in both sup 2 sup 3 sup 8 U and sup 2 sup 3 sup 2 Th from the high-energy Bremsstrahlung radiation produced by laser acceleration of electrons. The fission products were identified by time-resolved gamma-spectroscopy. (authors)

  18. Detection of Actinides via Nuclear Isomer De-Excitation

    Energy Technology Data Exchange (ETDEWEB)

    Francy, Christopher J. [Oregon State Univ., Corvallis, OR (United States)

    2009-07-01

    This dissertation discusses a data collection experiment within the Actinide Isomer Identification project (AID). The AID project is the investigation of an active interrogation technique that utilizes nuclear isomer production, with the goal of assisting in the interdiction of illicit nuclear materials. In an attempt to find and characterize isomers belonging to 235U and its fission fragments, a 232Th target was bombarded with a monoenergetic 6Li ion beam, operating at 45 MeV.

  19. Topical report on actinide-only burnup credit for PWR spent nuclear fuel packages. Revision 1

    Energy Technology Data Exchange (ETDEWEB)

    None, None

    1997-04-01

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

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

    Energy Technology Data Exchange (ETDEWEB)

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

    2010-02-18

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

  1. Normalization of oxygen and hydrogen isotope data

    Science.gov (United States)

    Coplen, T.B.

    1988-01-01

    To resolve confusion due to expression of isotopic data from different laboratories on non-corresponding scales, oxygen isotope analyses of all substances can be expressed relative to VSMOW or VPDB (Vienna Peedee belemnite) on scales normalized such that the ??18O of SLAP is -55.5% relative to VSMOW. H3+ contribution in hydrogen isotope ratio analysis can be easily determined using two gaseous reference samples that differ greatly in deuterium content. ?? 1988.

  2. Octupole correlations in excited 0{sup +} states of the actinides

    Energy Technology Data Exchange (ETDEWEB)

    Spieker, Mark; Endres, Janis; Zilges, Andreas [Institute for Nuclear Physics, University of Cologne (Germany); Bucurescu, Dorel; Pascu, Sorin; Zamfir, Nicolae-Victor [Horia Hulubei National Institute of Physics and Nuclear Engineering, Bucharest (Romania); Faestermann, Thomas [Physik Department, Technische Universitaet Muenchen, Munich (Germany); Hertenberger, Ralf; Wirth, Hans-Friedrich [Fakultaet fuer Physik, Ludwig-Maximilians-Universitaet Muenchen, Munich (Germany)

    2014-07-01

    New experimental data has once again shown the importance of the octupole degree of freedom in the actinides. To further study possible admixtures of double-octupole structures to the wave function of positive-parity states, a high-resolution (p,t) experiment on {sup 242}Pu has been recently performed at the Q3D magnetic spectrograph in Munich. Excited 0{sup +} states were populated in {sup 240}Pu up to an excitation energy of 3 MeV. The new data allowed for a stringent test of the predictions of the spdf interacting boson model. In order to find possible double-octupole 0{sup +} candidates in the actinides, the signature of close-lying first and second excited 0{sup +} states has been proposed. It is found that the observation of this signature coincides with an E1 γ-decay of the first excited 0{sup +} state, while this state is strongly populated in the (p,t) reaction.

  3. Actinide Solubility and Speciation in the WIPP [PowerPoint

    Energy Technology Data Exchange (ETDEWEB)

    Reed, Donald T. [Los Alamos National Lab. (LANL), Los Alamos, NM (United States)

    2015-11-02

    The presentation begins with the role and need for nuclear repositories (overall concept, international updates (Sweden, Finland, France, China), US approach and current status), then moves on to the WIPP TRU repository concept (design, current status--safety incidents of February 5 and 14, 2014, path forward), and finally considers the WIPP safety case: dissolved actinide concentrations (overall approach, oxidation state distribution and redox control, solubility of actinides, colloidal contribution and microbial effects). The following conclusions are set forth: (1) International programs are moving forward, but at a very slow and somewhat sporadic pace. (2) In the United States, the Salt repository concept, from the perspective of the long-term safety case, remains a viable option for nuclear waste management despite the current operational issues/concerns. (3) Current model/PA prediction (WIPP example) are built on redundant conservatisms. These conservatisms are being addressed in the ongoing and future research to fill existing data gaps--redox control of plutonium by Fe(0, II), thorium (analog) solubility studies in simulated brine, contribution of intrinsic and biocolloids to the mobile concentration, and clarification of microbial ecology and effects.

  4. Actinide production from xenon bombardments of curium-248

    Energy Technology Data Exchange (ETDEWEB)

    Welch, R.B.

    1985-01-01

    Production cross sections for many actinide nuclides formed in the reaction of /sup 129/Xe and /sup 132/Xe with /sup 248/Cm at bombarding energies slightly above the coulomb barrier were determined using radiochemical techniques to isolate these products. These results are compared with cross sections from a /sup 136/Xe + /sup 248/Cm reaction at a similar energy. When compared to the reaction with /sup 136/Xe, the maxima in the production cross section distributions from the more neutron deficient projectiles are shifted to smaller mass numbers, and the total cross section increases for the production of elements with atomic numbers greater than that of the target, and decreases for lighter elements. These results can be explained by use of a potential energy surface (PES) which illustrates the effect of the available energy on the transfer of nucleons and describes the evolution of the di-nuclear complex, an essential feature of deep-inelastic reactions (DIR), during the interaction. The other principal reaction mechanism is the quasi-elastic transfer (QE). Analysis of data from a similar set of reactions, /sup 129/Xe, /sup 132/Xe, and /sup 136/Xe with /sup 197/Au, aids in explaining the features of the Xe + Cm product distributions, which are additionally affected by the depletion of actinide product yields due to deexcitation by fission. The PES is shown to be a useful tool to predict the general features of product distributions from heavy ion reactions.

  5. Heat capacities of lanthanide and actinide monazite-type ceramics

    Science.gov (United States)

    Kowalski, Piotr M.; Beridze, George; Vinograd, Victor L.; Bosbach, Dirk

    2015-09-01

    (Ln, An)xPO4 monazite-type ceramics are considered as potential matrices for the disposal of nuclear waste. In this study we computed the heat capacities and the standard entropies of these compounds using density functional perturbation theory. The calculations of lanthanide monazites agree well with the existing experimental data and provide information on the variation of the standard heat capacities and entropies along the lanthanide series. The results for AnPO4 monazites are similar to those obtained for the isoelectronic lanthanide compounds. This suggests that the missing thermodynamic data on actinide monazites could be similarly computed or assessed based on the properties of their lanthanide analogs. However, the computed heat capacity of PuPO4 appear to be significantly lower than the measured data. We argue that this discrepancy might indicate potential problems with the existing experimental data or with their interpretation. This shows a need for further experimental studies of the heat capacities of actinide-bearing, monazite-type ceramics.

  6. The EBR-II X501 Minor Actinide Burning Experiment

    Energy Technology Data Exchange (ETDEWEB)

    W. J. Carmack; M. K. Meyer; S. L. Hayes; H. Tsai

    2008-01-01

    The X501 experiment was conducted in EBR II as part of the Integral Fast Reactor program to demonstrate minor actinide burning through the use of a homogeneous recycle scheme. The X501 subassembly contained two metallic fuel elements loaded with relatively small quantities of americium and neptunium. Interest in the behavior of minor actinides (MA) during fuel irradiation has prompted further examination of existing X501 data and generation of new data where needed in support of the U.S. waste transmutation effort. The X501 experiment is one of the few MA bearing fuel irradiation tests conducted worldwide, and knowledge can be gained by understanding the changes in fuel behavior due to addition of MAs. Of primary interest are the effect of the MAs on fuel cladding chemical interaction and the redistribution behavior of americium. The quantity of helium gas release from the fuel and any effects of helium on fuel performance are also of interest. It must be stressed that information presented at this time is based on the limited PIE conducted in 1995–1996 and, currently, represents a set of observations rather than a complete understanding of fuel behavior. This report provides a summary of the X501 fabrication, characterization, irradiation, and post irradiation examination.

  7. Stabilization of actinides and lanthanides in unusually high oxidation states

    Energy Technology Data Exchange (ETDEWEB)

    Eller, P.G.; Penneman, R.A.

    1986-01-01

    Chemical environments can be chosen which stabilize actinides and lanthanides in unusually high or low oxidation states and in unusual coordination. In many cases, one can rationalize the observed species as resulting from strong charge/size influences provided by specific sites in host lattices (e.g., Tb(IV) in BaTbO/sub 3/ or Am(IV) in polytungstate anions). In other cases, the unusual species can be considered from an acid-base viewpoint (e.g., U(III) in AsF/sub 5//HF solution or Pu(VII) in Li/sub 5/PuO/sub 6/). In still other cases, an interplay of steric and redox effects can lead to interesting comparisons (e.g., instability of double fluoride salts of Pu(V) and Pu(VI) relative to U, Np, and Am analogues). Generalized ways to rationalize compounds containing actinides and lanthanides in unusual valences (particularly high valences), including the above and numerous other examples, will form the focus of this paper. Recently developed methods for synthesizing high valent f-element fluorides using superoxidizers and superacids at low temperatures will also be described. 65 refs., 8 figs., 9 tabs.

  8. APPLICATION OF ABSORPTION SPECTROSCOPY TO ACTINIDE PROCESS ANALYSIS AND MONITORING

    Energy Technology Data Exchange (ETDEWEB)

    Lascola, R.; Sharma, V.

    2010-06-03

    The characteristic strong colors of aqueous actinide solutions form the basis of analytical techniques for actinides based on absorption spectroscopy. Colorimetric measurements of samples from processing activities have been used for at least half a century. This seemingly mature technology has been recently revitalized by developments in chemometric data analysis. Where reliable measurements could formerly only be obtained under well-defined conditions, modern methods are robust with respect to variations in acidity, concentration of complexants and spectral interferents, and temperature. This paper describes two examples of the use of process absorption spectroscopy for Pu analysis at the Savannah River Site, in Aiken, SC. In one example, custom optical filters allow accurate colorimetric measurements of Pu in a stream with rapid nitric acid variation. The second example demonstrates simultaneous measurement of Pu and U by chemometric treatment of absorption spectra. The paper concludes with a description of the use of these analyzers to supplement existing technologies in nuclear materials monitoring in processing, reprocessing, and storage facilities.

  9. Energy-Dependent Fission Q Values Generalized for All Actinides

    Energy Technology Data Exchange (ETDEWEB)

    Vogt, R

    2008-09-25

    We generalize Madland's parameterization of the energy release in fission to obtain the dependence of the fission Q values on incident neutron energy, E{sub n}, for all major and minor actinides. These Q(E{sub n}) parameterizations are included in the ENDL2008 release. This paper describes calculations of energy-dependent fission Q values based on parameterizations of the prompt energy release in fission [1], developed by Madland [1] to describe the prompt energy release in neutron-induced fission of {sup 235}U, {sup 238}U, and {sup 239}Pu. The energy release is then related to the energy deposited during fission so that experimentally measurable quantities can be used to obtain the Q values. A discussion of these specific parameterizations and their implementation in the processing code for Monte Carlo neutron transport, MCFGEN, [2] is described in Ref. [3]. We extend this model to describe Q(E) for all actinides, major and minor, in the Evaluated Nuclear Data Library (ENDL) 2008 release, ENDL2008.

  10. MCNPX Monte Carlo burnup simulations of the isotope correlation experiments in the NPP Obrigheim

    Energy Technology Data Exchange (ETDEWEB)

    Cao Yan, E-mail: ycao@anl.go [Nuclear Engineering Division, Argonne National Laboratory, 9700 South Cass Avenue, Argonne, IL 60439 (United States); Gohar, Yousry [Nuclear Engineering Division, Argonne National Laboratory, 9700 South Cass Avenue, Argonne, IL 60439 (United States); Broeders, Cornelis H.M. [Forschungszentrum Karlsruhe, Institute for Neutron Physics and Reactor Technology, P.O. Box 3640, 76021 Karlsruhe (Germany)

    2010-10-15

    This paper describes the simulation work of the Isotope Correlation Experiment (ICE) using the MCNPX Monte Carlo computer code package. The Monte Carlo simulation results are compared with the ICE-Experimental measurements for burnup up to 30 GWD/t. The comparison shows the good capabilities of the MCNPX computer code package for predicting the depletion of the uranium fuel and the buildup of the plutonium isotopes in a PWR thermal reactor. The Monte Carlo simulation results show also good agreements with the experimental data for calculating several long-lived and stable fission products. However, for the americium and curium actinides, it is difficult to judge the predication capabilities for these actinides due to the large uncertainties in the ICE-Experimental data. In the MCNPX numerical simulations, a pin cell model is utilized to simulate the fuel lattice of the nuclear power reactor. Temperature dependent libraries based on JEFF3.1 nuclear data files are utilized for the calculations. In addition, temperature dependent libraries based ENDF/B-VII nuclear data files are utilized and the obtained results are very close to the JEFF3.1 results, except for {approx}10% differences in the prediction of the minor actinide isotopes buildup.

  11. Advanced techniques in actinide spectroscopy (ATAS 2014). Abstract book

    Energy Technology Data Exchange (ETDEWEB)

    Foerstendorf, Harald; Mueller, Katharina; Steudtner, Robin (eds.)

    2014-07-01

    In 2012, The Institute of Resource Ecology at the Helmholtz-Zentrum Dresden Rossendorf organized the first international workshop of Advanced Techniques in Actinide Spectroscopy (ATAS). A very positive feedback and the wish for a continuation of the workshop were communicated from several participants to the scientific committee during the workshop and beyond. Today, the ATAS workshop has been obviously established as an international forum for the exchange of progress and new experiences on advanced spectroscopic techniques for international actinide and lanthanide research. In comparison to already established workshops and conferences on the field of radioecology, one main focus of ATAS is to generate synergistic effects and to improve the scientific discussion between spectroscopic experimentalists and theoreticians. The exchange of ideas in particular between experimental and theoretical applications in spectroscopy and the presentation of new analytical techniques are of special interest for many research institutions working on the improvement of transport models of toxic elements in the environment and the food chain as well as on reprocessing technologies of nuclear and non-nuclear waste. Spectroscopic studies in combination with theoretical modelling comprise the exploration of molecular mechanisms of complexation processes in aqueous or organic phases and of sorption reactions of the contaminants on mineral surfaces to obtain better process understanding on a molecular level. As a consequence, predictions of contaminant's migration behaviour will become more reliable and precise. This can improve the monitoring and removal of hazardous elements from the environment and hence, will assist strategies for remediation technologies and risk assessment. Particular emphasis is placed on the results of the first inter-laboratory Round-Robin test on actinide spectroscopy (RRT). The main goal of RRT is the comprehensive molecular analysis of the actinide

  12. TAILORING INORGANIC SORBENTS FOR SRS STRONTIUM AND ACTINIDE SEPARATIONS: MODIFIED MONOSODIUM TITANATE PHASE III FINAL REPORT

    Energy Technology Data Exchange (ETDEWEB)

    Taylor-Pashow, K.; Hobbs, D.

    2010-09-01

    This document provides a final report of Phase III testing activities for the development of modified monosodium titanate (mMST), which exhibits improved strontium and actinide removal characteristics compared to the baseline MST material. The activities included characterization of the crystalline phases present at varying temperatures, solids settling characteristics, quantification of the peroxide content; evaluation of the post-synthesis gas release under different conditions; the extent of desorption of {sup 85}Sr, Np, and Pu under washing conditions; and the effects of age and radiation on the performance of the mMST. Key findings and conclusions include the following. The peroxide content of several mMST samples was determined using iodometric titration. The peroxide content was found to decrease with age or upon extended exposure to elevated temperature. A loss of peroxide was also measured after exposure of the material to an alkaline salt solution similar in composition to the simulated waste solution. To determine if the loss of peroxide with age affects the performance of the material, Sr and actinide removal tests were conducted with samples of varying age. The oldest sample (4 years and 8 months) did show lower Sr and Pu removal performance. When compared to the youngest sample tested (1 month), the oldest sample retained only 15% of the DF for Pu. Previous testing with this sample indicated no decrease in Pu removal performance up to an age of 30 months. No loss in Np removal performance was observed for any of the aged samples, and no uptake of uranium occurred at the typical sorbent loading of 0.2 g/L. Additional testing with a uranium only simulant and higher mMST loading (3.0 g/L) indicated a 10% increase of uranium uptake for a sample aged 3 years and 8 months when compared to the results of the same sample measured at an age of 1 year and 5 months. Performance testing with both baseline-MST and mMST that had been irradiated in a gamma source to

  13. Phytosiderophore Effects on Subsurface Actinide Contaminants: Potential for Phytostabilization and Phytoextraction

    Energy Technology Data Exchange (ETDEWEB)

    Ruggiero, Christy

    2005-06-01

    This project seeks to understand the influence of phytosiderophore-producing plants (grasses, including crops such as wheat and barley) on the biogeochemistry of actinide and other metal contaminants in the subsurface environment, and to determine the potential of phytosiderophore-producing plants for phytostabilization and phytoextraction of actinides and some metal soil contaminants. Phytosiderophores are secreted by graminaceous plants such as barley and wheat for the solubilization, mobilization and uptake of Fe and other essential nutrients from soils. The ability for these phytosiderophores to chelate and absorb actinides using the same uptake system as for Fe is being investigated though characterization of actinide-phytosiderophore complexes (independently of plants), and characterization of plant uptake of such complexes. We may also show possible harm caused by these plants through increased chelation of actinides that increase in actinide mobilization & migration in the subsurface environment. This information can then be directly applied by either removal of harmful plants, or can be used to develop plant-based soil stabilization/remediation technologies. Such technologies could be the low-cost, low risk solution to many DOE actinide contamination problems.

  14. Production Pathways and Separation Procedures for High-Diagnostic-Value Activation Species, Fission Products, and Actinides Required for Preparation of Realistic Synthetic Post-Detonation Nuclear Debris: Status Report and FY16 Project Plan

    Energy Technology Data Exchange (ETDEWEB)

    Faye, S. A. [Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States); Shaughnessy, D. A. [Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States)

    2015-08-19

    The objective of this project is to provide a comprehensive study on the production routes and chemical separation requirements for activation products, fission products, and actinides required for the creation of realistic post-detonation surrogate debris. Isotopes that have been prioritized by debris diagnosticians will be examined for their ability to be produced at existing irradiation sources, production rates, and availability of target materials, and chemical separation procedures required to rapidly remove the products from the bulk target matrix for subsequent addition into synthetic debris samples. The characteristics and implications of the irradiation facilities on the isotopes of interest will be addressed in addition to a summary of the isotopes that are already regularly produced. This is a planning document only.

  15. Octupole collectivity in the Sm isotopes

    Energy Technology Data Exchange (ETDEWEB)

    Babilon, M. [Yale Univ., New Haven, CT (United States). Wright Nuclear Structure Lab.]|[Technische Univ. Darmstadt (Germany). Inst. fuer Kernphysik; Zamfir, N.V. [Yale Univ., New Haven, CT (United States). Wright Nuclear Structure Lab.]|[National Inst. for Physics and Nuclear Engineering, Bucharest (Romania); Kusnezov, D. [Yale Univ., New Haven, CT (United States). Sloane Physics Lab.; McCutchan, E.A. [Yale Univ., New Haven, CT (United States). Wright Nuclear Structure Lab.; Zilges, A. [Technische Univ. Darmstadt (Germany). Inst. fuer Kernphysik

    2005-08-27

    Microscopic models suggest the occurrence of strong octupole correlations in nuclei with N{approx}88. To examine the signatures of octupole correlations in this region, the spdf Interacting Boson Approximation (IBA) Model is applied to the Sm isotopes with N = 86 - 92. The effects of including multiple negative parity bosons in the basis are compared to more standard one negative parity boson calculations and are analyzed in terms of signatures for strong octupole correlations. It is found that multiple negative parity bosons are needed to describe properties at medium spin. Bands with strong octupole correlations (multiple negative parity bosons) become yrast at medium spin in {sup 148,150}Sm. This region shares some similarities with the light actinides, where strong octupole correlations were also found at medium spin. (orig.)

  16. Interaction of actinides with amino acids: from peptides to proteins; Interaction des actinides avec les acides amines: du peptide a la proteine

    Energy Technology Data Exchange (ETDEWEB)

    Jeanson, A

    2008-09-15

    Structural information on complexes of actinides with molecules of biological interest is required to better understand the mechanisms of actinides transport in living organisms, and can contribute to develop new decorporation treatments. Our study is about Th(IV), Np(IV), Pu(IV) and uranyl(VI) cations, which have a high affinity for some protein domains, and Fe(III), which is the natural cation of these biological systems. In this work, chelation of actinides has been brought to light with UV-visible-Near Infra Red spectroscopy, NMR, EPR, and ultrafiltration. Determination of the structure of the complexation site has been undertaken with Exafs measurements, and of the tertiary structure of the protein with SANS measurements. The first approach was to describe the interaction modes between actinides and essential chemical functions of proteins. Thus, the Ac-AspAspProAspAsp-NH{sub 2} peptide was studied as a possible chelate of actinides. Polynuclear species with {mu}-oxo or {mu}-hydroxo bridges were identified. The iron complex is binuclear, and the actinide ones have a higher nuclearity. The second approach was to study a real case of complexation of actinide with a protein: transferrin. Results show that around physiological ph a mononuclear complex is formed with Np(IV) and Pu(IV), while transferrin does not complex Th(IV) in the same conditions. Characteristic distances of M-transferrin complexes (M = Fe, Np, Pu) were determined. Moreover, the protein seems to be in its close conformation with Pu(IV), and in its open form with Np(IV) and UO{sub 2}{sup 2+}. (author)

  17. Advanced Extraction Methods for Actinide/Lanthanide Separations

    Energy Technology Data Exchange (ETDEWEB)

    Scott, M.J.

    2005-12-01

    The separation of An(III) ions from chemically similar Ln(III) ions is perhaps one of the most difficult problems encountered during the processing of nuclear waste. In the 3+ oxidation states, the metal ions have an identical charge and roughly the same ionic radius. They differ strictly in the relative energies of their f- and d-orbitals, and to separate these metal ions, ligands will need to be developed that take advantage of this small but important distinction. The extraction of uranium and plutonium from nitric acid solution can be performed quantitatively by the extraction with the TBP (tributyl phosphate). Commercially, this process has found wide use in the PUREX (plutonium uranium extraction) reprocessing method. The TRUEX (transuranium extraction) process is further used to coextract the trivalent lanthanides and actinides ions from HLLW generated during PUREX extraction. This method uses CMPO [(N, N-diisobutylcarbamoylmethyl) octylphenylphosphineoxide] intermixed with TBP as a synergistic agent. However, the final separation of trivalent actinides from trivalent lanthanides still remains a challenging task. In TRUEX nitric acid solution, the Am(III) ion is coordinated by three CMPO molecules and three nitrate anions. Taking inspiration from this data and previous work with calix[4]arene systems, researchers on this project have developed a C3-symmetric tris-CMPO ligand system using a triphenoxymethane platform as a base. The triphenoxymethane ligand systems have many advantages for the preparation of complex ligand systems. The compounds are very easy to prepare. The steric and solubility properties can be tuned through an extreme range by the inclusion of different alkoxy and alkyl groups such as methyoxy, ethoxy, t-butoxy, methyl, octyl, t-pentyl, or even t-pentyl at the ortho- and para-positions of the aryl rings. The triphenoxymethane ligand system shows promise as an improved extractant for both tetravalent and trivalent actinide recoveries form

  18. Thermodynamics of actinide complexation in solution at elevated temperatures: application of variable-temperature titration calorimetry.

    Science.gov (United States)

    Rao, Linfeng

    2007-06-01

    Studies of actinide complexation in solution at elevated temperatures provide insight into the effect of solvation and the energetics of complexation, and help to predict the chemical behavior of actinides in nuclear waste processing and disposal where temperatures are high. This tutorial review summarizes the data on the complexation of actinides at elevated temperatures and describes the methodology for thermodynamic measurements, with the emphasis on variable-temperature titration calorimetry, a highly valuable technique to determine the enthalpy and, under appropriate conditions, the equilibrium constants of complexation as well.

  19. AMS of the Minor Plutonium Isotopes.

    Science.gov (United States)

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

    2013-01-01

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

  20. Surrogate Measurements of Actinide (n,2n) Cross Sections with NeutronSTARS

    Energy Technology Data Exchange (ETDEWEB)

    Casperson, R. J. [Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States); Burke, J. T. [Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States); Hughes, R. O. [Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States); Akindele, O. A. [Univ. of California, Berkeley, CA (United States); Koglin, J. D. [Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States); Wang, B. [Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States); Tamashiro, A. [Oregon State Univ., Corvallis, OR (United States)

    2016-09-27

    Directly measuring (n,2n) cross sections on short-lived actinides presents a number of experimental challenges. The surrogate reaction technique is an experimental method for measuring cross sections on short-­lived isotopes, and it provides a unique solution for measuring (n,2n) cross sections. This technique involves measuring a charged-­particle reaction cross section, where the reaction populates the same compound nucleus as the reaction of interest. To perform these surrogate (n,2n) cross section measurements, a silicon telescope array has been placed along a beam line at the Texas A&M University Cyclotron Institute, which is surrounded by a large tank of gadolinium-doped liquid scintillator, which acts as a neutron detector. The combination of the charge-particle and neutron-detector arrays is referred to as NeutronSTARS. In the analysis procedure for calculating the (n,2n) cross section, the neutron detection efficiency and time structure plays an important role. Due to the lack of availability of isotropic, mono-energetic neutron sources, modeling is an important component in establishing this efficiency and time structure. This report describes the NeutronSTARS array, which was designed and commissioned during this project. It also describes the surrogate reaction technique, specifically referencing a 235U(n,2n) commissioning measurement that was fielded during the past year. Advanced multiplicity analysis techniques have been developed for this work, which should allow for efficient analysis of 241Pu(n,2n) and 239Pu(n,2n) cross section measurements

  1. Bruyères-le-Châtel Neutron Evaluations of Actinides with the TALYS Code: The Fission Channel

    Science.gov (United States)

    Romain, P.; Morillon, B.; Duarte, H.

    2016-01-01

    For several years, various neutron evaluations of plutonium and uranium isotopes have been performed at Bruyères-le-Châtel (BRC), from 1 keV up to 30 MeV. Since only nuclear reaction models have been used to produce these evaluations, our approach was named the "Full Model" approach. Total, shape elastic and direct inelastic cross sections were obtained from the coupled channels model using a dispersive optical potential developed for actinides, with a large enough coupling scheme including the lowest octupolar band. All other cross sections were calculated using the Hauser-Feshbach theory (TALYS code) with a pre-equilibrium component above 8-10 MeV. In this paper, we focus our attention on the fission channel. More precisely, we will present the BRC contribution to fission modeling and the philosophy adopted in our "Full Model" approach. Performing evaluations with the "Full Model" approach implies the optimization of a large number of model parameters. With increasing neutron incident energy, many residual nuclei produced by nucleon emission also lead to fission. All available experimental data assigned to various fission mechanisms of the same nucleus were used to determine fission barrier parameters. For uranium isotopes, triple-humped fission barriers were required in order to reproduce accurately variations of the experimental fission cross sections. Our BRC fission modeling has shown that the effects of the class II or class III states located in the wells of the fission barrier sometimes provide an anti-resonant transmission rather than a resonant one. Consistent evaluations were produced for a large series of U and Pu isotopes. Resulting files were tested against integral data.

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

    Energy Technology Data Exchange (ETDEWEB)

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

    2011-02-15

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

  3. First ionization potential of the heaviest actinide lawrencium, element 103

    Science.gov (United States)

    Sato, Tetsuya K.; Asai, Masato; Borschevsky, Anastasia; Stora, Thierry; Sato, Nozomi; Kaneya, Yusuke; Tsukada, Kazuaki; Düllmann, Christoph E.; Eberhardt, Klaus; Eliav, Ephraim; Ichikawa, Shinichi; Kaldor, Uzi; Kratz, Jens V.; Miyashita, Sunao; Nagame, Yuichiro; Ooe, Kazuhiro; Osa, Akihiko; Renisch, Dennis; Runke, Jörg; Schädel, Matthias; Thörle-Pospiech, Petra; Toyoshima, Atsushi; Trautmann, Norbert

    2016-12-01

    The first ionization potential (IP1) of element 103, lawrencium (Lr), has been successfully determined for the first time by using a newly developed method based on a surface ionization process. The measured IP1 value is 4.963 eV. This value is the smallest among those of actinide elements and is in excellent agreement with the value of 4.963(15) eV predicted by state-of-the-art relativistic calculations also performed in this work. Our results strongly support that the Lr atom has an electronic configuration of [Rn]7s25f147p, which is influenced by strong relativistic effects. The present work provides a reliable benchmark for theoretical calculations and also opens the way for studies on atomic properties of heavy elements with atomic number Z > 100. Moreover, the present achievement has triggered a controversy on the position of lutetium (Lu) and Lr in the Periodic Table of Elements.

  4. Facilities for preparing actinide or fission product-based targets

    CERN Document Server

    Sors, M

    1999-01-01

    Research and development work is currently in progress in France on the feasibility of transmutation of very long-lived radionuclides such as americium, blended with an inert medium such as magnesium oxide and pelletized for irradiation in a fast neutron reactor. The process is primarily designed to produce ceramics for nuclear reactors, but could also be used to produce targets for accelerators. The Actinide Development Laboratory is part of the ATALANTE complex at Marcoule, where the CEA investigates reprocessing, liquid and solid waste treatment and vitrification processes. The laboratory produces radioactive sources; after use, their constituents are recycled, notably through R and D programs requiring such materials. Recovered americium is purified, characterized and transformed for an experiment known as ECRIX, designed to demonstrate the feasibility of fabricating americium-based ceramics and to determine the reactor transmutation coefficients.

  5. Pillared metal(IV) phosphate-phosphonate extraction of actinides

    Energy Technology Data Exchange (ETDEWEB)

    Burns, J.D.; Clearfield, A. [Texas A and M Univ., College Station, TX (United States). Dept. of Chemistry; Borkowski, M.; Reed, D.T. [Los Alamos National Laboratory, Carlsbad, NM (United States). Earth and Environmental Sciences Div.

    2012-07-01

    Four pillared metal(IV) phosphate-phosphonate ion exchange materials were synthesized and characterized. Studies were conducted to determine their affinity for the lanthanides (Ln's) and actinides (An's). It was determined that by simply manipulating the metal source (Zr or Sn) and the phosphate source (H{sub 3}PO{sub 4} or Na{sub 3}PO{sub 4}) large differences were seen in the extraction of the Ln and An species. K{sub d} values higher than 4 x 10{sup 5} were observed for the AnO{sub 2}{sup 2+} species in nitric acid at pH 2. These basic uptake experiments are important, as the data they provide may indicate the possibility of a separation of Ln's from An's or even more notably americium from curium and Ln's. (orig.)

  6. Angular distributions in the neutron-induced fission of actinides

    CERN Multimedia

    In 2003 the n_TOF Collaboration performed the fission cross section measurement of several actinides ($^{232}$Th, $^{233}$U, $^{234}$U, $^{237}$Np) at the n_TOF facility using an experImental setup made of Parallel Plate Avalanche Counters (PPAC). The method based on the detection of the 2 fragments in coincidence allowed to clearly disentangle the fission reactions among other types of reactions occurring in the spallation domain. We have been therefore able to cover the very broad neutron energy range 1eV-1GeV, taking full benefit of the unique characteristics of the n_TOF facility. Figure 1 shows an example obtained in the case of $^{237}$Np where the n_ TOF measurement showed that the cross section was underestimated by a large factor in the resonance region.

  7. Review and needs in actinide chemistry in relation with biological purposes

    Energy Technology Data Exchange (ETDEWEB)

    Ansoborlo, E.; Moulin, V.; Bion, L.; Doizi, D.; Moulin, C.; Cote, G.; Madic, C.; Van der Lee, J

    2004-07-01

    In case of accidental release of radionuclides in the environment, actinides could occur and may present an healthy risk for human beings. In order to study their behavior in human organism (metabolism, retention, excretion), it is of prime importance to know solution actinide chemistry, and more particularly thermodynamic constants, which will allow to determine their speciation: speciation governs biological availability and toxicity of elements and is also of great interest for decorporation purposes. In this framework, a CEA working group on speciation has been created in order to share data both on thermodynamic constants and on speciation analytical methods, interesting chemists, environmentalists and biologists. It has been focused, in a first time, on actinides. The purpose of this paper is to present the state of the art on actinide speciation within biological media and to focus on the lack of information in order to orientate future research. (authors)

  8. Organophosphorus reagents in actinide separations: Unique tools for production, cleanup and disposal

    Energy Technology Data Exchange (ETDEWEB)

    Nash, K. L.

    2000-01-12

    Interactions of actinide ions with phosphate and organophosphorus reagents have figured prominently in nuclear science and technology, particularly in the hydrometallurgical processing of irradiated nuclear fuel. Actinide interactions with phosphorus-containing species impact all aspects from the stability of naturally occurring actinides in phosphate mineral phases through the application of the bismuth phosphate and PUREX processes for large-scale production of transuranic elements to the development of analytical separation and environment restoration processes based on new organophosphorus reagents. In this report, an overview of the unique role of organophosphorus compounds in actinide production, disposal, and environment restoration is presented. The broad utility of these reagents and their unique chemical properties is emphasized.

  9. SACSESS – the EURATOM FP7 project on actinide separation from spent nuclear fuels

    Directory of Open Access Journals (Sweden)

    Bourg Stéphane

    2015-12-01

    Full Text Available Recycling of actinides by their separation from spent nuclear fuel, followed by transmutation in fast neutron reactors of Generation IV, is considered the most promising strategy for nuclear waste management. Closing the fuel cycle and burning long-lived actinides allows optimizing the use of natural resources and minimizing the long-term hazard of high-level nuclear waste. Moreover, improving the safety and sustainability of nuclear power worldwide. This paper presents the activities striving to meet these challenges, carried out under the Euratom FP7 collaborative project SACSESS (Safety of Actinide Separation Processes. Emphasis is put on the safety issues of fuel reprocessing and waste storage. Two types of actinide separation processes, hydrometallurgical and pyrometallurgical, are considered, as well as related aspects of material studies, process modeling and the radiolytic stability of solvent extraction systems. Education and training of young researchers in nuclear chemistry is of particular importance for further development of this field.

  10. Special Form Testing of Sealed Source Encapsulation for High-Alpha-Activity Actinide Materials

    Energy Technology Data Exchange (ETDEWEB)

    Martinez, Oscar A [ORNL

    2016-01-01

    In the United States all transportation of radioactive material is regulated by the U.S. Department of Transportation (DOT). Beginning in 2008 a new type of sealed-source encapsulation package was developed and tested by Oak Ridge National Laboratory (ORNL). These packages contain high-alpha-activity actinides and are regulated and transported in accordance with the requirements for DOT Class 7 hazardous material. The DOT provides specific regulations pertaining to special form encapsulation designs. The special form designation indicates that the encapsulated radioactive contents have a very low probability of dispersion even when subjected to significant structural events. The special form designs have been shown to simplify the delivery, transport, acceptance, and receipt processes. It is intended for these sealed-source encapsulations to be shipped to various facilities making it very advantageous for them to be certified as special form. To this end, DOT Certificates of Competent Authority (CoCAs) have been sought for the design suitable for containing high-alpha-activity actinide materials. This design consists of the high-alpha-activity material encapsulated within a triangular zirconia canister, referred to as a ZipCan, tile that is then enclosed by a spherical shell. The spherical shell design, with ZipCan tile inside, was tested for compliance with the special form regulations found in 49 CFR 173.469. The spherical enclosure was subjected to 9-m impact, 1 m percussion, and 10-minute thermal tests at the Packaging Evaluation Facility located at the National Transportation Research Center in Knoxville, TN USA and operated by ORNL. Before and after each test, the test units were subjected to a helium leak check and a bubble test. The ZipCan tiles and core were also subjected to the tests required for ISO 2919:2012(E), including a Class IV impact test and heat test and subsequently subjected to helium leakage rate tests [49 CFR 173.469(a)(4)(i)]. The impact

  11. Radiochemical separation of actinides for their determination in environmental samples and waste products

    Energy Technology Data Exchange (ETDEWEB)

    Gleisberg, B. [Nuclear Engineering and Analytics Rossendorf, Inc. (VKTA), Dresden (Germany)

    1997-03-01

    The determination of low level activities of actinides in environmental samples and waste products makes high demands on radiochemical separation methods. Artificial and natural actinides were analyzed in samples form the surrounding areas of NPP and of uranium mines, incorporation samples, solutions containing radioactive fuel, solutions and solids resutling from the process, and in wastes. The activities are measured by {alpha}-spectrometry and {gamma}-spectrometry. (DG)

  12. Actinides in molecules: exotic properties probed by X-ray Absorption Spectroscopy

    Energy Technology Data Exchange (ETDEWEB)

    Den Auwer, C.; Moisy, P.; Guilbaud, P.; Guillaumont, D.; Simoni, E.; Conradson, S.D

    2004-07-01

    Dealing with actinide elements in molecular chemistry may result in particularly attractive and exotic physico-chemical properties. In solution, one of the spectroscopic tools able to selectively probe the structural or electronic properties of these molecules is the X-ray absorption process. Different aspects of absorption edge or EXAFS analysis related to actinide studies are presented, including phenomenological and semi-quantitative approaches. (authors)

  13. Static, Mixed-Array Total Evaporation for Improved Quantitation of Plutonium Minor Isotopes in Small Samples.

    Science.gov (United States)

    Stanley, F E; Byerly, Benjamin L; Thomas, Mariam R; Spencer, Khalil J

    2016-06-01

    Actinide isotope measurements are a critical signature capability in the modern nuclear forensics "toolbox", especially when interrogating anthropogenic constituents in real-world scenarios. Unfortunately, established methodologies, such as traditional total evaporation via thermal ionization mass spectrometry, struggle to confidently measure low abundance isotope ratios (<10(-6)) within already limited quantities of sample. Herein, we investigate the application of static, mixed array total evaporation techniques as a straightforward means of improving plutonium minor isotope measurements, which have been resistant to enhancement in recent years because of elevated radiologic concerns. Results are presented for small sample (~20 ng) applications involving a well-known plutonium isotope reference material, CRM-126a, and compared with traditional total evaporation methods. Graphical Abstract ᅟ.

  14. Isotopic Yield Distributions of Transfer- and Fusion-Induced Fission from 238U+12C Reactions in Inverse Kinematics

    CERN Document Server

    Caamaño, M; Farget, F; Derkx, X; Schmidt, K -H; Audouin, L; Bacri, C -O; Barreau, G; Benlliure, J; Casarejos, E; Chbihi, A; Fernandez-Dominguez, B; Gaudefroy, L; Golabek, C; Jurado, B; Lemasson, A; Navin, A; Rejmund, M; Roger, T; Shrivastava, A; Schmitt, C

    2013-01-01

    A novel method to access the complete identification in atomic number Z and mass A of fragments produced in low-energy fission of actinides is presented. This method, based on the use of multi- nucleon transfer and fusion reactions in inverse kinematics, is applied in this work to reactions between a 238U beam and a 12C target to produce and induce fission of moderately excited actinides. The fission fragments are detected and fully identified with the VAMOS spectrometer of GANIL, allowing the measurement of fragment yields of several hundreds of isotopes in a range between A ~ 80 and ~ 160, and from Z ~ 30 to ~ 64. For the first time, complete isotopic yield distributions of fragments from well-defined fissioning systems are available. Together with the precise measurement of the fragment emission angles and velocities, this technique gives further insight into the nuclear-fission process.

  15. CHARACTERIZATION OF ACTINIDES IN SIMULATED ALKALINE TANK WASTE SLUDGES AND LEACHATES

    Energy Technology Data Exchange (ETDEWEB)

    Nash, Kenneth L.

    2008-11-20

    In this project, both the fundamental chemistry of actinides in alkaline solutions (relevant to those present in Hanford-style waste storage tanks), and their dissolution from sludge simulants (and interactions with supernatants) have been investigated under representative sludge leaching procedures. The leaching protocols were designed to go beyond conventional alkaline sludge leaching limits, including the application of acidic leachants, oxidants and complexing agents. The simulant leaching studies confirm in most cases the basic premise that actinides will remain in the sludge during leaching with 2-3 M NaOH caustic leach solutions. However, they also confirm significant chances for increased mobility of actinides under oxidative leaching conditions. Thermodynamic data generated improves the general level of experiemental information available to predict actinide speciation in leach solutions. Additional information indicates that improved Al removal can be achieved with even dilute acid leaching and that acidic Al(NO3)3 solutions can be decontaminated of co-mobilized actinides using conventional separations methods. Both complexing agents and acidic leaching solutions have significant potential to improve the effectiveness of conventional alkaline leaching protocols. The prime objective of this program was to provide adequate insight into actinide behavior under these conditions to enable prudent decision making as tank waste treatment protocols develop.

  16. Reactor Fuel Isotopics and Code Validation for Nuclear Applications

    Energy Technology Data Exchange (ETDEWEB)

    Francis, Matthew W. [Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); Weber, Charles F. [Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); Pigni, Marco T. [Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); Gauld, Ian C. [Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)

    2015-02-01

    Experimentally measured isotopic concentrations of well characterized spent nuclear fuel (SNF) samples have been collected and analyzed by previous researchers. These sets of experimental data have been used extensively to validate the accuracy of depletion code predictions for given sets of burnups, initial enrichments, and varying power histories for different reactor types. The purpose of this report is to present the diversity of data in a concise manner and summarize the current accuracy of depletion modeling. All calculations performed for this report were done using the Oak Ridge Isotope GENeration (ORIGEN) code, an internationally used irradiation and decay code solver within the SCALE comprehensive modeling and simulation code. The diversity of data given in this report includes key actinides, stable fission products, and radioactive fission products. In general, when using the current ENDF/B-VII.0 nuclear data libraries in SCALE, the major actinides are predicted to within 5% of the measured values. Large improvements were seen for several of the curium isotopes when using improved cross section data found in evaluated nuclear data file ENDF/B-VII.0 as compared to ENDF/B-V-based results. The impact of the flux spectrum on the plutonium isotope concentrations as a function of burnup was also shown. The general accuracy noted for the actinide samples for reactor types with burnups greater than 5,000 MWd/MTU was not observed for the low-burnup Hanford B samples. More work is needed in understanding these large discrepancies. The stable neodymium and samarium isotopes were predicted to within a few percent of the measured values. Large improvements were seen in prediction for a few of the samarium isotopes when using the ENDF/B-VII.0 libraries compared to results obtained with ENDF/B-V libraries. Very accurate predictions were obtained for 133Cs and 153Eu. However, the predicted values for the stable ruthenium and rhodium isotopes varied

  17. Simultaneous Evaluation of Fission Cross Sections for Cm Isotopes

    Directory of Open Access Journals (Sweden)

    Lee Y.-O.

    2010-03-01

    Full Text Available Fission Cross Sections for a complete set of Cm-isotopes, 240-250Cm, have been calculated in the incident energy range from above resonance region to 20 MeV. This work aims at providing the fission cross sections with consistent set of model parameters for Cm isotopes, as a part of a complete evaluation including covariance files for several minor actinides which play a great role in the Advanced Fuel Cycle (AFC design and applications as well as the design of new generation of nuclear reactors (GEN-IV. This was accomplished by means of computational analyses carried out with the nuclear model code EMPIRE-2.19 which is the modular system of nuclear reaction codes. A Fission model of this work took into account transmission derived in the WKB approximation within an optical model through a double-humped fission barrier.

  18. Simultaneous Evaluation of Fission Cross Sections for Cm Isotopes

    Science.gov (United States)

    Kim, H. I.; Gil, C.-S.; Lee, Y.-O.

    2010-03-01

    Fission Cross Sections for a complete set of Cm-isotopes, 240-250Cm, have been calculated in the incident energy range from above resonance region to 20 MeV. This work aims at providing the fission cross sections with consistent set of model parameters for Cm isotopes, as a part of a complete evaluation including covariance files for several minor actinides which play a great role in the Advanced Fuel Cycle (AFC) design and applications as well as the design of new generation of nuclear reactors (GEN-IV). This was accomplished by means of computational analyses carried out with the nuclear model code EMPIRE-2.19 which is the modular system of nuclear reaction codes. A Fission model of this work took into account transmission derived in the WKB approximation within an optical model through a double-humped fission barrier.

  19. Stable isotope separation in calutrons: Forty years of production and distribution

    Energy Technology Data Exchange (ETDEWEB)

    Bell, W.A.; Tracy, J.G.

    1987-11-01

    The stable isotope separation program, established in 1945, has operated continually to provide enriched stable isotopes and selected radioactive isotopes, including the actinides, for use in research, medicine, and industrial applications. This report summarizes the first forty years of effort in the production and distribution of stable isotopes. Evolution of the program along with the research and development, chemical processing, and production efforts are highlighted. A total of 3.86 million separator hours has been utilized to separate 235 isotopes of 56 elements. Relative effort expended toward processing each of these elements is shown. Collection rates (mg/separator h), which vary by a factor of 20,000 from the highest to the lowest (/sup 205/Tl to /sup 46/Ca), and the attainable isotopic purity for each isotope are presented. Policies related to isotope pricing, isotope distribution, and support for the enrichment program are discussed. Changes in government funding, coupled with large variations in sales revenue, have resulted in 7-fold perturbations in production levels.

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

    Science.gov (United States)

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

    2015-02-01

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

  1. Actinides reduction by recycling in a thermal reactor; Reduccion de actinidos por reciclado en un reactor termico

    Energy Technology Data Exchange (ETDEWEB)

    Ramirez S, J. R.; Martinez C, E.; Balboa L, H., E-mail: ramon.ramirez@inin.gob.mx [ININ, Carretera Mexico-Toluca s/n, 52750 Ocoyoacac, Estado de Mexico (Mexico)

    2014-10-15

    This work is directed towards the evaluation of an advanced nuclear fuel cycle in which radioactive actinides could be recycled to remove most of the radioactive material; firstly a production reference of actinides in standard nuclear fuel of uranium at the end of its burning in a BWR reactor is established, after a fuel containing plutonium is modeled to also calculate the actinides production in MOX fuel type. Also it proposes a design of fuel rod containing 6% of actinides in a matrix of uranium from the tails of enrichment, then four standard uranium fuel rods are replaced by actinides rods to evaluate the production and transmutation thereof, the same procedure was performed in the fuel type MOX and the end actinide reduction in the fuel was evaluated. (Author)

  2. The procedure and results of calculations of the equilibrium isotopic composition of a demonstration subcritical molten salt reactor

    Energy Technology Data Exchange (ETDEWEB)

    Nevinitsa, V. A., E-mail: Neviniza-VA@nrcki.ru; Dudnikov, A. A.; Blandinskiy, V. Yu.; Balanin, A. L.; Alekseev, P. N. [National Research Centre Kurchatov Institute (Russian Federation); Titarenko, Yu. E.; Batyaev, V. F.; Pavlov, K. V.; Titarenko, A. Yu., E-mail: yuri.titarenko@itep.ru [Institute for Theoretical and Experimental Physics (Russian Federation)

    2015-12-15

    A subcritical molten salt reactor with an external neutron source is studied computationally as a facility for incineration and transmutation of minor actinides from spent nuclear fuel of reactors of VVER-1000 type and for producing {sup 233}U from {sup 232}Th. The reactor configuration is chosen, the requirements to be imposed on the external neutron source are formulated, and the equilibrium isotopic composition of heavy nuclides and the key parameters of the fuel cycle are calculated.

  3. The procedure and results of calculations of the equilibrium isotopic composition of a demonstration subcritical molten salt reactor

    Science.gov (United States)

    Nevinitsa, V. A.; Dudnikov, A. A.; Blandinskiy, V. Yu.; Balanin, A. L.; Alekseev, P. N.; Titarenko, Yu. E.; Batyaev, V. F.; Pavlov, K. V.; Titarenko, A. Yu.

    2015-12-01

    A subcritical molten salt reactor with an external neutron source is studied computationally as a facility for incineration and transmutation of minor actinides from spent nuclear fuel of reactors of VVER-1000 type and for producing 233U from 232Th. The reactor configuration is chosen, the requirements to be imposed on the external neutron source are formulated, and the equilibrium isotopic composition of heavy nuclides and the key parameters of the fuel cycle are calculated.

  4. Sensitivity analysis of minor actinides transmutation to physical and technological parameters

    Directory of Open Access Journals (Sweden)

    Kooyman Timothée

    2015-01-01

    Full Text Available Minor actinides transmutation is one of the three main axis defined by the 2006 French law for management of nuclear waste, along with long-term storage and use of a deep geological repository. Transmutation options for critical systems can be divided in two different approaches: (a homogeneous transmutation, in which minor actinides are mixed with the fuel. This exhibits the drawback of “polluting” the entire fuel cycle with minor actinides and also has an important impact on core reactivity coefficients such as Doppler Effect or sodium void worth for fast reactors when the minor actinides fraction increases above 3 to 5% depending on the core; (b heterogeneous transmutation, in which minor actinides are inserted into transmutation targets which can be located in the center or in the periphery of the core. This presents the advantage of decoupling the management of the minor actinides from the conventional fuel and not impacting the core reactivity coefficients. In both cases, the design and analyses of potential transmutation systems have been carried out in the frame of Gen IV fast reactor using a “perturbation” approach in which nominal power reactor parameters are modified to accommodate the loading of minor actinides. However, when designing such a transmutation strategy, parameters from all steps of the fuel cycle must be taken into account, such as spent fuel heat load, gamma or neutron sources or fabrication feasibility. Considering a multi-recycling strategy of minor actinides, an analysis of relevant estimators necessary to fully analyze a transmutation strategy has been performed in this work and a sensitivity analysis of these estimators to a broad choice of reactors and fuel cycle parameters has been carried out. No threshold or percolation effects were observed. Saturation of transmutation rate with regards to several parameters has been observed, namely the minor actinides volume fraction and the irradiation time

  5. Quantum Mechanical Studies of the Early Actinide Compounds

    Science.gov (United States)

    Obodo, Kingsley Onyebuchi

    This study involves the investigation of the early actinide systems using ab initio techniques based on density functional theory (DFT). It was motivated by: (i) the incomplete description of these systems using conventional DFT because they are strongly correlated, (ii) the usefulness of these systems in nuclear energy generation, (iii) the complexity that arises in experimentally studying these systems due to their inherent radioactive nature and (iv) their limited availability. The results obtained from this study are divided into two broad sections. The first comprises chapters 3 and 4 while the second comprises chapters 5 and 6. Thorium based compounds are studied in chapters 3 and 4. In the first section, the Hubbard U parameter is not necessary to accurately describe the electronic, elastic and mechanical properties of these systems. In the second, the inclusion of the Hubbard U parameter is shown to be paramount for the accurate description of most compounds considered. Chapter 3 presents the electronic, structural and bonding character of thorium based nitrides. We obtained the result that Th2N2 NH, which is crystallographically equivalent to metallic Th2N 3, is insulating. Chapter 4 demonstrates that the formation of a meta-stable thorium-titanium based alloy is plausible and also further information on bonding, electronic and elastic properties of the determined meta-stable alloy is provided. This has provided important new knowledge about these bulk systems. In Chapter 5 the DFT + U based study on Pa and its oxides is presented. The electronic, structural and bonding character of these systems was studied. We found that PaO2 is a Mott-Hubbard insulator with an indirect band gap of 3.48 eV within the generalized gradient approximation GGA + U. Chapter 6 discusses various actinide nitrides. We explored the electronic properties, elastic properties, lattice dynamics and the energetics of the various compounds using GGA + U. Also, we investigated the effect

  6. Silicon isotope fractionation during magmatic differentiation

    Science.gov (United States)

    Savage, Paul S.; Georg, R. Bastian; Williams, Helen M.; Burton, Kevin W.; Halliday, Alex N.

    2011-10-01

    The Si isotopic composition of Earth's mantle is thought to be homogeneous (δ 30Si = -0.29 ± 0.08‰, 2 s.d.) and not greatly affected by partial melting and recycling. Previous analyses of evolved igneous material indicate that such rocks are isotopically heavy relative to the mantle. To understand this variation, it is necessary to investigate the degree of Si isotopic fractionation that takes place during magmatic differentiation. Here we report Si isotopic compositions of lavas from Hekla volcano, Iceland, which has formed in a region devoid of old, geochemically diverse crust. We show that Si isotopic composition varies linearly as a function of silica content, with more differentiated rocks possessing heavier isotopic compositions. Data for samples from the Afar Rift Zone, as well as various igneous USGS standards are collinear with the Hekla trend, providing evidence of a fundamental relationship between magmatic differentiation and Si isotopes. The effect of fractionation has been tested by studying cumulates from the Skaergaard Complex, which show that olivine and pyroxene are isotopically light, and plagioclase heavy, relative to the Si isotopic composition of the Earth's mantle. Therefore, Si isotopes can be utilised to model the competing effects of mafic and felsic mineral fractionation in evolving silicate liquids and cumulates. At an average SiO 2 content of ˜60 wt.%, the predicted δ 30Si value of the continental crust that should result from magmatic fractionation alone is -0.23 ± 0.05‰ (2 s.e.), barely heavier than the mantle. This is, at most, a maximum estimate, as this does not take into account weathered material whose formation drives the products toward lighter δ 30Si values. Mass balance calculations suggest that removal of continental crust of this composition from the upper mantle will not affect the Si isotopic composition of the mantle.

  7. Paving the way for the synthesis of a series of divalent actinide complexes: a theoretical perspective.

    Science.gov (United States)

    Wu, Q-Y; Lan, J-H; Wang, C-Z; Cheng, Z-P; Chai, Z-F; Gibson, J K; Shi, W-Q

    2016-02-21

    Recently, the +2 formal oxidation state in soluble molecular complexes for lanthanides (La-Nd, Sm-Lu) and actinides (Th and U) has been discovered [W. J. Evans, et al., J. Am. Chem. Soc., 2011, 133, 15914; J. Am. Chem. Soc., 2012, 134, 8420; J. Am. Chem. Soc., 2013, 135, 13310; Chem. Sci., 2015, 6, 517]. To explore the nature of the bonding and stabilities of the low-valent actinide complexes, a series of divalent actinide species, [AnCp'3](-) (An[double bond, length as m-dash]Th-Am, Cp' = [η(5)-C5H4(SiMe3)](-)) have been investigated in THF solution using scalar relativistic density functional theory. The electronic structures and electron affinity properties were systematically studied to identify the interactions between the +2 actinide ions and Cp' ligands. The ground state electron configurations for the [AnCp'3](-) species are [ThCp'3](-) 6d(2), [PaCp'3](-) 5f(2)6d(1), [UCp'3](-) 5f(3)6d(1), [NpCp'3](-) 5f(5), [PuCp'3](-) 5f(6), and [AmCp'3](-) 5f(7), respectively, according to the MO analysis. The total bonding energy decreases from the Th- to the Am-complex and the electrostatic interactions mainly dominate the bonding between the actinide atom and ligands. The electron affinity analysis suggests that the reduction reaction of AnCp'3→ [AnCp'3](-) should become increasingly facile across the actinide series from Th to Am, in accord with the known An(iii/ii) reduction potentials. This work expands the knowledge on the low oxidation state chemistry of actinides, and further motivates and guides the synthesis of related low oxidation state compounds of 5f elements.

  8. Reversible optical sensor for the analysis of actinides in solution; Capteur optique reversible pour l'analyse des actinides en solution

    Energy Technology Data Exchange (ETDEWEB)

    Lesage, B.; Picard, S. [CEA Marcoule, Dept. de Radiochimie et Procedes, Service de Chimie des Procedes de Separation, Lab. de Chimie des Actinides, 30 (France); Serein-Spirau, F.; Lereporte, J.P. [Ecole Nationale Superieure de Chimie de Montpellier (ENSCM), CNRS UMR 5076, Lab. Heterochimie Moleculaire et Macromoleculaire, 34 - Montpellier (France)

    2007-07-01

    In this work is presented a concept of reversible optical sensor for actinides. It is composed of a p doped conducing polymer support and of an anion complexing the actinides. The chosen conducing polymer is the thiophene-2,5-di-alkoxy-benzene whose solubility and conductivity are perfectly known. The actinides selective ligand is a lacunar poly-oxo-metallate such as P{sub 2}W{sub 17}O{sub 61}{sup 10-} or SiW{sub 11}O{sub 39}{sup 8-} which are strong anionic complexing agents of actinides at the oxidation state (IV) even in a very acid medium. The sensor is prepared by spin coating of the composite mixture 'polymer + ligand' on a conducing glass electrode and then tested towards its optical and electrochemical answer in presence of uranium (IV). The absorption change due to the formation of cations complexes by poly-oxo-metallate reveals the presence of uranium (IV). After the measurement, the sensor is regenerated by anodic polarization of the support and oxidation of the uranium (IV) into uranium (VI) which weakly interacts with the poly-oxo-metallate and is then released in solution. (O.M.)

  9. 15N Isotope Techniques for Estimating Effects of Urea-N Fertilizer Application Rate on Yieids and Nutrient Contents of Pakchoi Cabbage and Asparagus Lettuce and Nitrogen Utilization Efficiency

    Institute of Scientific and Technical Information of China (English)

    LIAO Yu-Iin; ZHENG Sheng-xian; RONG Xiang-min; LIU Qiang; FAN Mei-rong

    2010-01-01

    A pot experiment combined with15 N isotope techniques was conducted to evaluate effects of the varying rates of urea.N fertilizer application on yields,quailty,and nitrogen use efficiency(NUE)of pakchoi cabbage(Brassica chinensis L.)and asparagus lettuce(Lactuca saiva L.).15 N-labbled urea(5.35 15 N atom%)was added to pots with 6.5kg soil of 0.14,0.18,0.21,0.25,and 0.29 g N/kg soil.and applied in two splits:60 percenl as basel dressing in the mixture and 40 percent as toodressing.The fresh yields of two vegetable species increased with the increasing input of urea-N,but there was a significant quadratic relationship between the dose of urea-N fertilizer application and the fresh yields.Whan the dosage of urea-N fertilizer reached a certain value,nitrate readily accumulated in the two kinds of plants due to the decrease in NR activity;furthermore,there was a linear nagative correlation between nitrate content and NR activity.With the increasing input of urea-N.ascorbic acid and soluble sugar initially increased,declined after a while,and crude fiber rapidly decreased too.Total absorbed N(TAN).N derived from fertilizer(Ndff),and N derived from soil(Ndfs)increased,and the ratio of Ndff and TAN also increased.but the ratio of Ndfs and TAN as well as NUE of urea-N fertilizer decreased with the increasing input of urea-N.These results suggested that the increasing application of labeled N fertilizer led lo the increase in unlabeled N(namely,Ndfs)presumably due to"added nitrogen interaction"(ANI),the decease in NUE of urea-N fertilizer may be due to excess fertilization beyond the levels of plant requirements and the ANI.and the decrease jn the two vege table yields with the increasing addition of urea-N possibly because the excess accumulation of nitrate reached a toxic level.

  10. On the valence fluctuation in the early actinide metals

    Energy Technology Data Exchange (ETDEWEB)

    Söderlind, P., E-mail: soderlind@llnl.gov [Lawrence Livermore National Laboratory, Livermore, CA 94550 (United States); Landa, A.; Tobin, J.G.; Allen, P. [Lawrence Livermore National Laboratory, Livermore, CA 94550 (United States); Medling, S.; Booth, C.H. [Lawrence Berkeley National Laboratory, Berkeley, CA 94720 (United States); Bauer, E.D.; Cooley, J.C. [Los Alamos National Laboratory, Los Alamos, NM 87545 (United States); Sokaras, D.; Weng, T.-C.; Nordlund, D. [Stanford Synchrotron Radiation Lightsource, SLAC National Laboratory, Menlo Park, CA 94025 (United States)

    2016-02-15

    Highlights: • We make a connection between experimentally observed valence fluctuations and density functional theory. • We present a new model for valence fluctuations. • We present new experimental data for uranium and valence fluctuations. - Abstract: Recent X-ray measurements suggest a degree of valence fluctuation in plutonium and uranium intermetallics. We are applying a novel scheme, in conjunction with density functional theory, to predict 5f configuration fractions of states with valence fluctuations for the early actinide metals. For this purpose we perform constrained integer f-occupation calculations for the α phases of uranium, neptunium, and plutonium metals. For plutonium we also investigate the δ phase. The model predicts uranium and neptunium to be dominated by the f{sup 3} and f{sup 4} configurations, respectively, with only minor contributions from other configurations. For plutonium (both α and δ phase) the scenario is dramatically different. Here, the calculations predict a relatively even distribution between three valence configurations. The δ phase has a greater configuration fraction of f{sup 6} compared to that of the α phase. The theory is consistent with the interpretations of modern X-ray experiments and we present resonant X-ray emission spectroscopy results for α-uranium.

  11. First ionization potential of the heaviest actinide lawrencium, element 103

    Directory of Open Access Journals (Sweden)

    Sato Tetsuya K.

    2016-01-01

    Full Text Available The first ionization potential (IP1 of element 103, lawrencium (Lr, has been successfully determined for the first time by using a newly developed method based on a surface ionization process. The measured IP1 value is 4.9630.080.07 eV. This value is the smallest among those of actinide elements and is in excellent agreement with the value of 4.963(15 eV predicted by state-of-the-art relativistic calculations also performed in this work. Our results strongly support that the Lr atom has an electronic configuration of [Rn]7s25f147p11/2, which is influenced by strong relativistic effects. The present work provides a reliable benchmark for theoretical calculations and also opens the way for studies on atomic properties of heavy elements with atomic number Z > 100. Moreover, the present achievement has triggered a controversy on the position of lutetium (Lu and Lr in the Periodic Table of Elements.

  12. Functionalization of mesoporous materials for lanthanide and actinide extraction.

    Science.gov (United States)

    Florek, Justyna; Giret, Simon; Juère, Estelle; Larivière, Dominic; Kleitz, Freddy

    2016-10-14

    Among the energy sources currently available that could address our insatiable appetite for energy and minimize our CO2 emission, solar, wind, and nuclear energy currently occupy an increasing portion of our energy portfolio. The energy associated with these sources can however only be harnessed after mineral resources containing valuable constituents such as actinides (Ac) and rare earth elements (REEs) are extracted, purified and transformed into components necessary for the conversion of energy into electricity. Unfortunately, the environmental impacts resulting from their manufacture including the generation of undesirable and, sometimes, radioactive wastes and the non-renewable nature of the mineral resources, to name a few, have emerged as challenges that should be addressed by the scientific community. In this perspective, the recent development of functionalized solid materials dedicated to selective elemental separation/pre-concentration could provide answers to several of the above-mentioned challenges. This review focuses on recent advances in the field of mesoporous solid-phase (SP) sorbents designed for REEs and Ac liquid-solid extraction. Particular attention will be devoted to silica and carbon sorbents functionalized with commonly known ligands, such as phosphorus or amide-containing functionalities. The extraction performances of these new systems are discussed in terms of sorption capacity and selectivity. In order to support potential industrial applications of the silica and carbon-based sorbents, their main drawbacks and advantages are highlighted and discussed.

  13. Iron (III) Matrix Effects on Mineralization and Immobilization of Actinides

    Energy Technology Data Exchange (ETDEWEB)

    Cynthia-May S. Gong; Tyler A. Sullens; Kenneth R. Czerwinski

    2006-01-01

    Abstract - A number of models for the Yucca Mountain Project nuclear waste repository use studies of actinide sorption onto well-defined iron hydroxide materials. In the case of a waste containment leak, however, a complex interaction between dissolved waste forms and failed containment vessel components can lead to immediate precipitation of migratory iron and uranyl in the silicate rich near-field environment. Use of the Fe(III) and UO22+ complexing agent acetohydroxamic acid (AHA) as a colorimetric agent for visible spectrophotometry is well-known. Using the second derivative of these spectra a distinct shift in iron complexation in the presence of silicate is seen that is not seen with uranyl or alone. Silica also decreases the ability of uranyl and ferric solutions to absorb hydroxide, hastening precipitation. These ferric silicate precipitates are highly amorphous and soluble. Precipitates formed in the presence of uranyl below ~1 mol% exhibit lower solubility than precipitates from up to 50 mol % and of uranyl silicates alone.

  14. Actinide-specific complexing agents: their structural and solution chemistry

    Energy Technology Data Exchange (ETDEWEB)

    Raymond, K.N.; Freeman, G.E.; Kappel, M.J.

    1983-07-01

    The synthesis of a series of tetracatecholate ligands designed to be specific for Pu(IV) and other actinide(IV) ions has been achieved. Although these compounds are very effective as in vivo plutonium removal agents, potentiometric and voltammetric data indicate that at neutral pH full complexation of the Pu(IV) ion by all four catecholate groups does not occur. Spectroscopic results indicate that the tetracatecholates, 3,4,3-LICAMS and 3,4,3-LICAMC, complex Am(III). The Am(IV)/(III)-catecholate couple (where catecholate = 3,4,3-LICAMS or 3,4,3-LICAMC) is not observed, but may not be observable due to the large currents associated with ligand oxidation. However, within the potential range where ligand oxidation does not occur, these experiments indicate that the reduction potential of free Am(IV)/(III) is probably greater than or equal to + 2.6 V vs NHE or higher. Proof of the complexation of americium in the trivalent oxidation state by 3,4,3-LICAMS and 3,4,3-LICAMC elimates the possibility of tetracatholates stabilizing Am(IV) in vivo.

  15. Structural organization and spectroscopy of peptide-actinide(IV) complexes; Organisation structurale et spectroscopie de peptides susceptibles de complexer les actinides(IV)

    Energy Technology Data Exchange (ETDEWEB)

    Dahou, S.

    2010-11-05

    The contamination of living organisms by actinide elements is at the origin of both radiological and chemical toxicity that may lead to severe dysfunction. Most of the data available on the actinide interaction with biological systems are macroscopic physiological measurements and are lacking a molecular description of the systems. Because of the intricacy of these systems, classical biochemical methods are difficult to implement. Our strategy consisted in designing simplified biomimetic peptides, and describing the corresponding intramolecular interactions with actinides. A carboxylic pentapeptide of the form DDPDD has been at the starting point of this work in order to further assess the influence of the peptide sequence on the topology of the complexes.To do so, various linear (Asp/Ala permutations, peptoids) and cyclic analogues have been synthesized. Furthermore, in order to include the hydroxamic function (with a high affinity for Fe(III)) in the peptide, both desferrioxamine and acetohydroxamic acid have been investigated. However because of difficulties in synthesis, we have not been able to test these peptides. Three actinide cations have been considered at oxidation state +IV (Th, Np, Pu) and compared to Fe(III), often considered as a biological surrogate of Pu(IV). The spatial arrangement of the peptide around the cation has been probed by spectrophotometry and X-ray Absorption Spectroscopy. The spectroscopic data and EXAFS data adjustment lead us to rationalize the topology of the complexes as a function of the peptide sequence: mix hydroxy polynuclear species for linear and cyclic peptides, mononuclear for the desferrioxamine complexes. Furthermore, significant differences have appeared between Fe(III) and actinide(IV), related to differences of reactivity in aqueous medium. (author)

  16. Synthesis and Evaluation of new Polyfunctional Molecules for Group Actinide Extraction; Synthese et evaluation de Nouvelles Molecules Polyfonctionnelles pour la Separation Groupee des Actinides

    Energy Technology Data Exchange (ETDEWEB)

    Marie, C.

    2009-10-15

    The aim of this project is to design new extracting molecules for spent nuclear fuel reprocessing. In order to minimize the long-term residual radiotoxicity of the waste, the GANEX process is an option based on homogeneous recycling of actinides. All actinides (U, Np, Pu, Am, Cm), present in a highly acidic aqueous solution, would be extracted together and separated from fission products (especially from lanthanides) using liquid-liquid extraction. In this context, twenty new bi-topic ligands constituted of a nitrogen poly-aromatic unit functionalized by amide groups were synthesized. Liquid-liquid extraction tests with these ligands dissolved alone in the organic phase show that N, N, N', N'-tetra-alkyl-6, 6''(2, 2':6', 2''-terpyridine)-diamides are able to selectively extract actinides at different oxidation states (Np(V et VI), U(VI), Pu(IV), Am(III), Cm(III)) from an aqueous solution 3M HNO{sub 3}. Nevertheless, actinides(III) are poorly extracted. According to crystallographic structures of complexes with Nd(III) and U(VI) determined by X-rays diffraction, these ligands are penta-dentate. In solution (methanol), complexes stoichiometries (1:1) of Nd(III), U(VI) and Pu(IV) were determined by electro-spray ionization mass spectrometry. Stability constants, evaluated by UV-visible spectrophotometry in MeOH/H{sub 2}O solutions, confirm the selectivity of ligands toward actinides(III) with respect to lanthanides(III). Associate to nuclear magnetic resonance experiments and DFT calculations (Density Functional Theory), a better knowledge of their coordination mode was achieved. (author)

  17. MOLECULAR SPECTROSCPY AND REACTIONS OF ACTINIDES IN THE GAS PHASE AND CRYOGENIC MATRICES

    Energy Technology Data Exchange (ETDEWEB)

    Heaven, Michael C.; Gibson, John K.; Marcalo, Joaquim

    2009-02-01

    In this chapter we review the spectroscopic data for actinide molecules and the reaction dynamics for atomic and molecular actinides that have been examined in the gas phase or in inert cryogenic matrices. The motivation for this type of investigation is that physical properties and reactions can be studied in the absence of external perturbations (gas phase) or under minimally perturbing conditions (cryogenic matrices). This information can be compared directly with the results from high-level theoretical models. The interplay between experiment and theory is critically important for advancing our understanding of actinide chemistry. For example, elucidation of the role of the 5f electrons in bonding and reactivity can only be achieved through the application of experimentally verified theoretical models. Theoretical calculations for the actinides are challenging due the large numbers of electrons that must be treated explicitly and the presence of strong relativistic effects. This topic has been reviewed in depth in Chapter 17 of this series. One of the goals of the experimental work described in this chapter has been to provide benchmark data that can be used to evaluate both empirical and ab initio theoretical models. While gas-phase data are the most suitable for comparison with theoretical calculations, there are technical difficulties entailed in generating workable densities of gas-phase actinide molecules that have limited the range of species that have been characterized. Many of the compounds of interest are refractory, and problems associated with the use of high temperature vapors have complicated measurements of spectra, ionization energies, and reactions. One approach that has proved to be especially valuable in overcoming this difficulty has been the use of pulsed laser ablation to generate plumes of vapor from refractory actinide-containing materials. The vapor is entrained in an inert gas, which can be used to cool the actinide species to room

  18. Minor actinide fission induced by multi-nucleon transfer reaction in inverse kinematics

    Directory of Open Access Journals (Sweden)

    Taieb J.

    2010-03-01

    Full Text Available In the framework of nuclear waste incineration and design of new generation nuclear reactors, experimental data on fission probabilities and on fission fragment yields of minor actinides are crucial to design prototypes. Transfer-induced fission has proven to be an efficient method to study fission probabilities of actinides which cannot be investigated with standard techniques due to their high radioactivity. We report on the preliminary results of an experiment performed at GANIL that investigates fission probabilities with multi-nucleon transfer reactions in inverse kinematics between a 238U beam on a 12C target. Actinides from U to Cm were produced with an excitation energy range from 0 to 30 MeV. In addition, inverse kinematics allowed to characterize the fission fragments in mass and charge. A key point of the analysis resides in the identification of the actinides produced in the different transfer channels. The new annular telescope SPIDER was used to tag the target-like recoil nucleus of the transfer reaction and to determine the excitation energy of the actinide. The fission probability for each transfer channel is accessible and the preliminary results for 238U are promising.

  19. Application of chemical structure and bonding of actinide oxide materials for forensic science

    Energy Technology Data Exchange (ETDEWEB)

    Wilkerson, Marianne Perry [Los Alamos National Laboratory

    2010-01-01

    We are interested in applying our understanding of actinide chemical structure and bonding to broaden the suite of analytical tools available for nuclear forensic analyses. Uranium- and plutonium-oxide systems form under a variety of conditions, and these chemical species exhibit some of the most complex behavior of metal oxide systems known. No less intriguing is the ability of AnO{sub 2} (An: U, Pu) to form non-stoichiometric species described as AnO{sub 2+x}. Environmental studies have shown the value of utilizing the chemical signatures of these actinide oxide materials to understand transport following release into the environment. Chemical speciation of actinide-oxide samples may also provide clues as to the age, source, or process history of the material. The scientific challenge is to identify, measure and understand those aspects of speciation of actinide analytes that carry information about material origin and history most relevant to forensics. Here, we will describe our efforts in material synthesis and analytical methods development that we will use to provide the fundamental science to characterize actinide oxide molecular structures for forensic science. Structural properties and initial results to measure structural variability of uranium oxide samples using synchrotron-based X-ray Absorption Fine Structure will be discussed.

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

    Science.gov (United States)

    Ewing, Rodney C.

    2011-02-01

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

  1. Technical requirements for the actinide source-term waste test program

    Energy Technology Data Exchange (ETDEWEB)

    Phillips, M.L.F.; Molecke, M.A.

    1993-10-01

    This document defines the technical requirements for a test program designed to measure time-dependent concentrations of actinide elements from contact-handled transuranic (CH TRU) waste immersed in brines similar to those found in the underground workings of the Waste Isolation Pilot Plant (WIPP). This test program wig determine the influences of TRU waste constituents on the concentrations of dissolved and suspended actinides relevant to the performance of the WIPP. These influences (which include pH, Eh, complexing agents, sorbent phases, and colloidal particles) can affect solubilities and colloidal mobilization of actinides. The test concept involves fully inundating several TRU waste types with simulated WIPP brines in sealed containers and monitoring the concentrations of actinide species in the leachate as a function of time. The results from this program will be used to test numeric models of actinide concentrations derived from laboratory studies. The model is required for WIPP performance assessment with respect to the Environmental Protection Agency`s 40 CFR Part 191B.

  2. Thermally unstable complexants: Stability of lanthanide/actinide complexes, thermal instability of the ligands, and applications in actinide separations

    Energy Technology Data Exchange (ETDEWEB)

    Nash, K.L.; Rickert, P.G.

    1991-01-01

    Water soluble complexing agents are commonly used in separations to enhance the selectivity of both ion exchange and solvent extraction processes. Applications of this type in the treatment of nuclear wastes using conventional complexing agents have found mixed success due to the nature of the complexants. In addition, the residual solutions containing these species have led to potentially serious complications in waste storage. To overcome some of the limitations of carboxylic acid and aminopolycarboxylate ligands, we have initiated a program to investigate the complexing ability, thermal/oxidative instability, and separation potential of a group of water soluble organophosphorus compounds which we call Thermally Unstable Complexants, or simply TUCS. Complexants of this type appear to be superior to conventional analogues in a number of respects. In this report, we will summarize our research to date on the actinide/lanthanide complexes with a series of substituted methanediphosphonic acids, the kinetics of their oxidative decomposition, and a few applications which have been developed for their use. 17 refs., 5 figs., 3 tab.

  3. Stable isotope studies

    Energy Technology Data Exchange (ETDEWEB)

    Ishida, T.

    1992-01-01

    The research has been in four general areas: (1) correlation of isotope effects with molecular forces and molecular structures, (2) correlation of zero-point energy and its isotope effects with molecular structure and molecular forces, (3) vapor pressure isotope effects, and (4) fractionation of stable isotopes. 73 refs, 38 figs, 29 tabs.

  4. Phosphonates as alternative to tributyl phosphate for the separation of actinides from fission products

    Energy Technology Data Exchange (ETDEWEB)

    Vyas, Chirag K.; Joshirao, Pranav M.; Manchanda, Vijay K. [Sungkyunkwan Univ., Suwon (Korea, Republic of). Dept. of Energy Science; Rao, C.V.S. Brahmmananda; Jayalakshmi, S. [Indira Gandhi Centre for Atomic Research, Kalpakkam (India). Fuel Chemistry Div.

    2015-06-01

    The present work investigates the role of increase in the basicity of organophosphorus extractant (dialkylalkyl phosphonates) on the uptake of actinides and fission products vis-a-vis tributyl phosphate (TBP), currently employed as a universal extractant. Two dialkylalkyl phosphonates viz. dibutylpropyl phosphonate (DBPrP) and dibutylpentyl phosphonate (DBPeP) were synthesized, characterized and evaluated for their solvent extraction behavior towards U(VI), Th(IV), Eu(III) and Tc(VII) in nitric acid medium ranging from 0.01-6 M. It was observed that increasing the basicity of the phosphoryl oxygen enhanced the uptake of the actinides and the distribution coefficient values were significantly larger as compared to TBP. The limiting organic concentration (LOC) value was estimated for Th(IV) for these extractants and compared with the TBP system. The separation factors of actinides with phosphonates over Tc(VII) are distinctly better than that with TBP.

  5. Research in actinide chemistry. Progress report, March 1, 1980-February 28, 1981

    Energy Technology Data Exchange (ETDEWEB)

    Choppin, G.R.

    1981-01-01

    Visible spectroscopy, NMR (/sup 1/H/sub 1/, /sup 6/C/sub 13/, /sup 57/La/sub 139/) spectroscopy, potentiometry, and calorimetry were used in lanthanide studies which have allowed much more thorough interpretation of actinide tracer studies. In the last several years, the studies were expanded to include actinides in the IV, V and VI oxidation states. Part of the research during this time was directed to investigation of actinide interaction with naturally occurring polyelectrolytes such as humic and fulvic acids. Since redox reactions seemingly occur in some of these interactions, a study of plutonium and neptunium redox behavior in the presence of organic complexing agents was started. Preliminary data are given for reduction of Np(VI) by various organic acids.

  6. Studies on fluoride complexing of hexavalent actinides using a fluoride ion selective electrode

    Energy Technology Data Exchange (ETDEWEB)

    Sawant, R.M.; Chaudhuri, N.K.; Rizvi, G.H.; Patil, S.K.

    1985-08-01

    Complex formation between actinide(VI) and fluoride ions in aqueous solutions was investigated using a fluoride ion selective electrode (F-ISE). As fairly high acidity used to suppress hydrolysis of the actinide(VI) ions, significant liquid junction potentials (Esub(j)) existed in the system. An iterative procedure was developed for computing free hydrogen ion concentration (Hsup(+)) as it could not be measured directly, using data obtained with F-ISE. Esub(j) values were estimated from known (Hsup(+)) and the stability constants of fluoride complexes of actinide(VI) ions were calculated following King and Gallagher's method using a computer program. The stability constants were found to follow the order U(VI) > Np(VI) > Pu(VI). (author). 18 refs.; 3 figs.; 9 tables.

  7. ACTINIDE REMOVAL PROCESS SAMPLE ANALYSIS, CHEMICAL MODELING, AND FILTRATION EVALUATION

    Energy Technology Data Exchange (ETDEWEB)

    Martino, C.; Herman, D.; Pike, J.; Peters, T.

    2014-06-05

    Filtration within the Actinide Removal Process (ARP) currently limits the throughput in interim salt processing at the Savannah River Site. In this process, batches of salt solution with Monosodium Titanate (MST) sorbent are concentrated by crossflow filtration. The filtrate is subsequently processed to remove cesium in the Modular Caustic Side Solvent Extraction Unit (MCU) followed by disposal in saltstone grout. The concentrated MST slurry is washed and sent to the Defense Waste Processing Facility (DWPF) for vitrification. During recent ARP processing, there has been a degradation of filter performance manifested as the inability to maintain high filtrate flux throughout a multi-batch cycle. The objectives of this effort were to characterize the feed streams, to determine if solids (in addition to MST) are precipitating and causing the degraded performance of the filters, and to assess the particle size and rheological data to address potential filtration impacts. Equilibrium modelling with OLI Analyzer{sup TM} and OLI ESP{sup TM} was performed to determine chemical components at risk of precipitation and to simulate the ARP process. The performance of ARP filtration was evaluated to review potential causes of the observed filter behavior. Task activities for this study included extensive physical and chemical analysis of samples from the Late Wash Pump Tank (LWPT) and the Late Wash Hold Tank (LWHT) within ARP as well as samples of the tank farm feed from Tank 49H. The samples from the LWPT and LWHT were obtained from several stages of processing of Salt Batch 6D, Cycle 6, Batch 16.

  8. New unsymmetrical digycolamide ligands for trivalent actinide separation

    Energy Technology Data Exchange (ETDEWEB)

    Ravi, Jammu; Venkatesan, K.A.; Antony, M.P.; Srinivasan, T.G.; Rao, P.R. Vasudeva [Indira Gandhi Centre for Atomic Research, Kalpakkam (India). Fuel Chemistry Div.

    2014-10-01

    New unsymmetrical diglycolamides (UDGAs), N,N-di-butyl-N',N'-di-dodecyl-3-oxapentane-1,5-diamide (C{sub 12}-C{sub 4}), N,N-di-dodecyl-N',N'-di-hexyl-3-oxapentane-1,5-diamide (C{sub 12}-C{sub 6}), N,N-di-decyl-N',N'-di-dodecyl-3-oxapentane-1,5-diamide (C{sub 12}-C{sub 10}) have been synthesized, and evaluated for the separation of americium(III) and europium(III) from nitric acid medium. The extraction behavior of Am(III), Eu(III), and Sr(II) in a solution of these UDGAs in n-dodecane was studied as a function of concentration of nitric acid in the aqueous phase. The distribution ratio of Am(III) and Eu(III) increased with increase in the concentration of nitric acid. The third phase formation behavior of nitric acid and neodymium(III) in 0.1 M UDGA/n-dodecane was studied. The third phase formation was not observed in all these UDGAs in n-dodecane (0.1 M), when the concentration of Nd(III) was ∝ 500 mM in 3-4M nitric acid. The stoichiometry of Am(III)-UDGA was determined from the slope analysis of the extraction data, which indicated the formation of 1:3 complex in all cases. Our studies revealed that the UDGA ligands with dodecyl group attached to one amidic nitrogen atom is inevitable for preventing third phase formation and the alkyl group at the other amidic nitrogen can be varied from butyl to decyl group for obtaining efficient extraction of trivalent actinides from high-level nuclear waste. (orig.)

  9. Pyrochlore as nuclear waste form. Actinide uptake and chemical stability

    Energy Technology Data Exchange (ETDEWEB)

    Finkeldei, Sarah Charlotte

    2015-07-01

    Radioactive waste is generated by many different technical and scientific applications. For the past decades, different waste disposal strategies have been considered. Several questions on the waste disposal strategy remain unanswered, particularly regarding the long-term radiotoxicity of minor actinides (Am, Cm, Np), plutonium and uranium. These radionuclides mainly arise from high level nuclear waste (HLW), specific waste streams or dismantled nuclear weapons. Although many countries have opted for the direct disposal of spent fuel, from a scientific and technical point of view it is imperative to pursue alternative waste management strategies. Apart from the vitrification, especially for trivalent actinides and Pu, crystalline ceramic waste forms are considered. In contrast to glasses, crystalline waste forms, which are chemically and physically highly stable, allow the retention of radionuclides on well-defined lattice positions within the crystal structure. Besides polyphase ceramics such as SYNROC, single phase ceramics are considered as tailor made host phases to embed a specific radionuclide or a specific group. Among oxidic single phase ceramics pyrochlores are known to have a high potential for this application. This work examines ZrO{sub 2} based pyrochlores as potential nuclear waste forms, which are known to show a high aqueous stability and a high tolerance towards radiation damage. This work contributes to (1) understand the phase stability field of pyrochlore and consequences of non-stoichiometry which leads to pyrochlores with mixed cationic sites. Mixed cationic occupancies are likely to occur in actinide-bearing pyrochlores. (2) The structural uptake of radionuclides themselves was studied. (3) The chemical stability and the effect of phase transition from pyrochlore to defect fluorite were probed. This phase transition is important, as it is the result of radiation damage in ZrO{sub 2} based pyrochlores. ZrO{sub 2} - Nd{sub 2}O{sub 3} pellets

  10. Magnesium isotope geochemistry in arc volcanism

    Science.gov (United States)

    Teng, Fang-Zhen; Hu, Yan; Chauvel, Catherine

    2016-06-01

    Incorporation of subducted slab in arc volcanism plays an important role in producing the geochemical and isotopic variations in arc lavas. The mechanism and process by which the slab materials are incorporated, however, are still uncertain. Here, we report, to our knowledge, the first set of Mg isotopic data for a suite of arc lava samples from Martinique Island in the Lesser Antilles arc, which displays one of the most extreme geochemical and isotopic ranges, although the origin of this variability is still highly debated. We find the δ26Mg of the Martinique Island lavas varies from -0.25 to -0.10, in contrast to the narrow range that characterizes the mantle (-0.25 ± 0.04, 2 SD). These high δ26Mg values suggest the incorporation of isotopically heavy Mg from the subducted slab. The large contrast in MgO content between peridotite, basalt, and sediment makes direct mixing between sediment and peridotite, or assimilation by arc crust sediment, unlikely to be the main mechanism to modify Mg isotopes. Instead, the heavy Mg isotopic signature of the Martinique arc lavas requires that the overall composition of the mantle wedge is buffered and modified by the preferential addition of heavy Mg isotopes from fluids released from the altered subducted slab during fluid-mantle interaction. This, in turn, suggests transfer of a large amount of fluid-mobile elements from the subducting slab to the mantle wedge and makes Mg isotopes an excellent tracer of deep fluid migration.

  11. Magnesium isotope geochemistry in arc volcanism.

    Science.gov (United States)

    Teng, Fang-Zhen; Hu, Yan; Chauvel, Catherine

    2016-06-28

    Incorporation of subducted slab in arc volcanism plays an important role in producing the geochemical and isotopic variations in arc lavas. The mechanism and process by which the slab materials are incorporated, however, are still uncertain. Here, we report, to our knowledge, the first set of Mg isotopic data for a suite of arc lava samples from Martinique Island in the Lesser Antilles arc, which displays one of the most extreme geochemical and isotopic ranges, although the origin of this variability is still highly debated. We find the δ(26)Mg of the Martinique Island lavas varies from -0.25 to -0.10, in contrast to the narrow range that characterizes the mantle (-0.25 ± 0.04, 2 SD). These high δ(26)Mg values suggest the incorporation of isotopically heavy Mg from the subducted slab. The large contrast in MgO content between peridotite, basalt, and sediment makes direct mixing between sediment and peridotite, or assimilation by arc crust sediment, unlikely to be the main mechanism to modify Mg isotopes. Instead, the heavy Mg isotopic signature of the Martinique arc lavas requires that the overall composition of the mantle wedge is buffered and modified by the preferential addition of heavy Mg isotopes from fluids released from the altered subducted slab during fluid-mantle interaction. This, in turn, suggests transfer of a large amount of fluid-mobile elements from the subducting slab to the mantle wedge and makes Mg isotopes an excellent tracer of deep fluid migration.

  12. Functionalized ionic liquids: new agents for the extraction of actinides/lanthanides

    Energy Technology Data Exchange (ETDEWEB)

    Ouadi, A.; Hesemann, P.; Billard, I.; Gaillard, C.; Gadenne, B.; Moreau, Joel J.E; Moutiers, G.; Mariet, C.; Labet, A

    2004-07-01

    The potentialities of hydrophobic ionic liquids BumimPF{sub 6} and BumimTf{sub 2}N for their use in the nuclear fuel cycle were investigated, in particular for the liquid liquid extraction. We demonstrate that the use of RTILs in replacement of the organic diluents for actinides partitioning is promising. In our contribution, we present the synthesis of several task-specific ionic liquids. Our results show that grafting metal complexing groups increases the affinity of metals to the IL phase and gives rise to suitable media for the liquid-liquid extraction of actinides. (authors)

  13. Equilibrium distribution of actinides including Cm between molten LiCl-KCl eutectic and liquid cadmium

    Energy Technology Data Exchange (ETDEWEB)

    Koyama, T.; Kinoshita, K.; Inoue, T. [Central Research Inst. of Electric Power Industry, Tokyo (Japan); Ougier, M.; Malmbeck, R.; Glatz, J.P. [Joint Research Centre, Karlsruhe (Germany). Inst. for Transuranium Elements

    2008-07-01

    Equilibrium distribution of actinides both in molten LiCl-KCl eutectic and liquid cadmium were measured from the concentration data obtained in electrorefining tests and reductive extraction tests. Separation factors for U, Np, Am, Cm against Pu were derived in the practical temperature range of 700 K to 783 K. The derived separation factors are consistent with the reported values measured at 773 K and 723 K. The temperature dependence for Cm is different compared to the other actinides (U, Np and Am). This behavior remains unclear and additional experimental measurements of distribution coefficient of Cm are required before ruling on the real behavior. (orig.)

  14. Oxyhydroxy Silicate Colloids: A New Type of Waterborne Actinide(IV) Colloids

    OpenAIRE

    Zänker, Harald; Weiss, Stephan; Hennig, Christoph; Brendler, Vinzenz; Ikeda‐Ohno, Atsushi

    2016-01-01

    Abstract At the near‐neutral and reducing aquatic conditions expected in undisturbed ore deposits or in closed nuclear waste repositories, the actinides Th, U, Np, and Pu are primarily tetravalent. These tetravalent actinides (AnIV) are sparingly soluble in aquatic systems and, hence, are often assumed to be immobile. However, AnIV could become mobile if they occur as colloids. This review focuses on a new type of AnIV colloids, oxyhydroxy silicate colloids. We herein discuss the chemical cha...

  15. Accurate labeling of the light-actinide O4,5 ionization edges

    Energy Technology Data Exchange (ETDEWEB)

    Moore, K; der Laan, G v

    2006-08-23

    In this short article the accurate labeling of the O4,5 edges of the light actinides is addressed. The O4 and O5 edges are both contained in what is termed the ''giant resonance'' and the smaller ''pre-peak'' that is observed is a consequence of first-order perturbation by the 5d spin-orbit interaction. Thus, the small prepeak in the actinide 5d {yields} 5f transition should not be labeled the O5 peak, but rather the {Delta}S=1 peak.

  16. A comparison of new reagents and processes for hydrometallurgical processing of actinides

    Energy Technology Data Exchange (ETDEWEB)

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

    2001-07-01

    The future viability of nuclear power as an electricity generation technology depends greatly on addressing all aspects of radioactive waste disposal. A closed fuel cycle with recycle and burnup of actinides is one important option for solving long-term waste sequestration issues. The 50 years of accumulated experience in application of solvent extraction to the processing of spent nuclear fuels uniquely qualifies this technology for actinide partitioning. However, employment of new reagents and development of new processes must be reconciled with century 21 expectations for environment protection. The interrelationship between the separations potential and waste disposal aspects of new reagents and processes are discussed in this report. (author)

  17. Methods for the determination of low-level actinide concentrations and their behaviour in the aquatic environment

    Energy Technology Data Exchange (ETDEWEB)

    Pilvioe, R

    1998-12-31

    Intentional and accidental releases have contaminated the environment with radionuclides, posing a potential health hazard to populations of the polluted regions. Low concentrations of the actinides in the environment and complex sample matrices have made their determination a time consuming and complicated task. Separation methods based on anion exchange and extraction chromatography were developed, and subsequently modified, for analysis of different sample matrices in this work. These methods were used for the investigations of the behaviour of actinides in the environment. Chemical properties play an important role in the phenomena affecting the migration of radionuclides. The method based on anion exchange was used to study the behaviour of U in a small U-Th deposit and also the behaviour of Pu, Am and Cm in a lake system after the Chernobyl accident. The speciation of U and Pu in natural waters has also been investigated. A trend of higher {sup 234}U/{sup 238}U activity ratios with lower {sup 238}U concentrations was seen in the ground waters in the Palmottu analogue study site in southern Finland. This indicates chemical leaching of U(VI) in oxidising conditions and preferable dissolution of {sup 234}U due to the recoil effects of the alpha decay in reducing conditions. The factors affecting the distribution of U concentrations and the {sup 234}U/{sup 238}U activity ratios in filtered ground water and the particulate fraction in the Palmottu are also discussed. The concentrations of Pu, Am and Cm in filtered water, particulate and surface sediment samples in Lake Paeijaenne in southern Finland have been determined. Pu, Am and Cm fallout from the Chernobyl accident was minor compared to global fallout from atmospheric nuclear weapon tests. Based on the {sup 238}Pu/{sup 239,240}Pu isotopic ratio, only 10 % of the Pu in the surface layer of the bottom sediment derived from the Chernobyl accident. Three months after the accident, 73 % of the total {sup 239

  18. Actinide collisions for QED and superheavy elements with the time-dependent Hartree-Fock theory and the Balian-Vénéroni variational principle

    Directory of Open Access Journals (Sweden)

    Kedziora David J.

    2011-10-01

    produce transfermium nuclei (Z > 100 in the collision of prolate deformed actinides such as 232Th+250Cf. The collision of the tip of one nucleus with the side of the other results in a nucleon flux toward the latter. The probability distributions for transfermium production in such a collision are computed. The produced nuclei are more neutron-rich than those formed in fusion reactions, thus, leading to more stable isotopes closer to the predicted superheavy island of stability. In addition to mass and charge dispersion, the Balian-Veneroni variational principle is used to compute correlations between Z and N distributions, which are zero in standard TDHF calculations.

  19. Chemical and ceramic methods toward safe storage of actinides using monazite. 1998 annual progress report

    Energy Technology Data Exchange (ETDEWEB)

    Morgan, P.E.D. [Rockwell International Corp., Thousand, Oaks, CA (US); Boatner, L.A. [Oak Ridge National Lab., TN (US)

    1998-06-01

    'The use of ceramic monazite, (La,Ce)PO{sub 4}, for sequestering actinides, especially plutonium, and some other radioactive waste elements (rare earths e.g.) and thus isolating them from the environment has been championed by Lynn Boatner of ORNL. It may be used alone or, as it is compatible with many other minerals in nature, can be used in composite combinations. Natural monazite, which almost invariably contains Th and U, is often formed in hydrothermal pegmatites and is extremely water resistant--examples are known where the mineral has been washed out of rocks (becoming a placer mineral as on the beach sands of India, Australia, Brazil etc.) then reincorporated into new rocks with new crystal overgrowths and then washed out again--being 2.5--3 billion years old. During this demanding water treatment it has retained Th and U. Where very low levels of water attack have been seen (in more siliceous waters), the Th is tied up as new ThSiO{sub 4} and remains immobile. Lest it be thought that rare-earths are rare or expensive, this is not so. In fact, the less common lanthanides such as gadolinium, samarium, europium, and terbium, are necessarily extracted and much used by, e.g., the electronics industry, leaving La and Ce as not-sufficiently-used by-products. The recent development of large scale use of Nd in Nd-B-Fe magnets has further exaggerated this. Large deposits of the parent mineral bastnaesite are present in the USA and in China. (Mineral monazite itself is not preferred due to its thorium content.) In the last 5 years it has become apparent show that monazite (more specifically La-monazite) is an unrecognized/becoming-interesting ceramic material. PuPO4 itself has the monazite structure; the PO{sub 4} 3-unit strongly stabilizes actinides and rare earths in their trivalent state. Monazite melts without decomposition (in a closed system) at 2,074 C and, being compatible with common ceramic oxides such as alumina, mullite, zirconia and YAG, is useful

  20. Neutron-Induced Fission Cross Section Measurements for Full Suite of Uranium Isotopes

    Science.gov (United States)

    Laptev, Alexander; Tovesson, Fredrik; Hill, Tony

    2010-11-01

    A well established program of neutron-induced fission cross section measurement at Los Alamos Neutron Science Center (LANSCE) is supporting the Fuel Cycle Research program (FC R&D). The incident neutron energy range spans energies from sub-thermal energies up to 200 MeV by measuring both the Lujan Center and the Weapons Neutron Research center (WNR). Conventional parallel-plate fission ionization chambers with actinide deposited foils are used as a fission detector. The time-of-flight method is implemented to measure neutron energy. Counting rate ratio from investigated and standard U-235 foils is translated into fission cross section ratio. Different methods of normalization for measured ratio are employed, namely, using of actinide deposit thicknesses, normalization to evaluated data, etc. Finally, ratios are converted to cross sections based on the standard U-235 fission cross section data file. Preliminary data for newly investigated isotopes U-236 and U-234 will be reported. Those new data complete a full suite of Uranium isotopes, which were investigated with presented experimental approach. When analysis of the new measured data will is completed, data will be delivered to evaluators. Having data for full set of Uranium isotopes will increase theoretical modeling capabilities and make new data evaluations much more reliable.

  1. Radionuclide content of selected root vegetables as influenced by culinary preparation

    Energy Technology Data Exchange (ETDEWEB)

    Adriano, D.C.; Doswell, A.C.; Ciravolo, T.G.; Pinder, J.E. III; McLeod, K.W

    2000-07-01

    A greenhouse study involving root vegetables (carrot, red beet, and turnips) was conducted primarily to evaluate the effect of culinary processing (light washing, scrubbing, and peeling) on the radionuclide content of the edible portions. In terms of concentration ratio of the radionuclides left in roots after peeling, the trend follows: {sup 90}Sr>{sup 137}Cs>>{sup 234}U congruent with {sup 238}U{>=}{sup 238}Pu. The actinide contents in the roots were apparently due to surface adherence of the contaminated soil particulates as indicated by the diminution of the contents upon brushing the surface, which were further decreased by peeling the skin. Rigorous culinary processing of roots, such as scrubbing or peeling, could substantially diminish the contents of the actinides, but not of the more mobile {sup 90}Sr and {sup 137}Cs.

  2. Method of loading organic materials with group III plus lanthanide and actinide elements

    Science.gov (United States)

    Bell, Zane W.; Huei-Ho, Chuen; Brown, Gilbert M.; Hurlbut, Charles

    2003-04-08

    Disclosed is a composition of matter comprising a tributyl phosphate complex of a group 3, lanthanide, actinide, or group 13 salt in an organic carrier and a method of making the complex. These materials are suitable for use in solid or liquid organic scintillators, as in x-ray absorption standards, x-ray fluorescence standards, and neutron detector calibration standards.

  3. Sorption Speciation of Lanthanides/Actinides on Minerals by TRLFS, EXAFS and DFT Studies: A Review

    Directory of Open Access Journals (Sweden)

    Xiaoli Tan

    2010-11-01

    Full Text Available Lanthanides/actinides sorption speciation on minerals and oxides by means of time resolved laser fluorescence spectroscopy (TRLFS, extended X-ray absorption fine structure spectroscopy (EXAFS and density functional theory (DFT is reviewed in the field of nuclear disposal safety research. The theoretical aspects of the methods are concisely presented. Examples of recent research results of lanthanide/actinide speciation and local atomic structures using TRLFS, EXAFS and DFT are discussed. The interaction of lanthanides/actinides with oxides and minerals as well as their uptake are also of common interest in radionuclide chemistry. Especially the sorption and inclusion of radionuclides into several minerals lead to an improvement in knowledge of minor components in solids. In the solid-liquid interface, the speciation and local atomic structures of Eu(III, Cm(III, U(VI, and Np(IV/VI in several natural and synthetic minerals and oxides are also reviewed and discussed. The review is important to understand the physicochemical behavior of lanthanides/actinides at a molecular level in the natural environment.

  4. A calculation for radial expectation values of helium like actinide ions (Z=89-93)

    Science.gov (United States)

    Ürer, G.; Arslan, M.; Balkaya, E.; Keçeli, A.

    2016-03-01

    Radial expectation values, , for helium like actinides (ZAc=89, ZTh=90, ZPa=91, ZU=92, and ZNp=93) are reported using the Multiconfiguration Hartree-Fock (MCHF) within the framework Breit-Pauli corrections. Atomic data as energy levels, wavelengths, weighted oscillator strengths, and transition probabilities for allowed and forbidden transitions need these calculations. The obtained results are compared available works.

  5. Rapid radiochemical method for determination of actinides in emergency concrete and brick samples.

    Science.gov (United States)

    Maxwell, Sherrod L; Culligan, Brian K; Kelsey-Wall, Angel; Shaw, Patrick J

    2011-09-02

    A new rapid method for the determination of actinides in emergency concrete and brick samples has been developed at the Savannah River Site Environmental Lab (Aiken, SC, USA) that can be used in emergency response situations or for routine analysis. If a radiological dispersive device (RDD), Improvised Nuclear Device (IND) or nuclear accident occurs, there will be a urgent need for rapid analyses of many different environmental matrices, including building materials such as concrete and brick, to support dose mitigation and environmental clean-up. The new method for actinides in concrete and brick method utilizes a rapid sodium hydroxide fusion method, a lanthanum fluoride matrix removal step, and a column separation process with stacked TEVA, TRU and DGA Resin cartridges. Alpha emitters are prepared using rare earth microprecipitation for counting by alpha spectrometry. The method showed high chemical recoveries and effective removal of interferences. The determination of actinides in concrete and brick sample analysis can be performed in less than 8h with excellent quality for emergency samples. The rapid fusion technique is a rugged sample digestion method that ensures that any refractory actinide particles are effectively digested.

  6. Mechanical behaviour and diffusion of gas during neutron irradiation of actinides in ceramic inert matrices

    NARCIS (Netherlands)

    Neeft, E.A.C.

    2004-01-01

    Fission of actinides from nuclear waste in inert matrices (materials without uranium) can reduce the period in time that nuclear waste is more radiotoxic than uranium ore that is the rock from which ordinary reactor fuel is made. A pioneering study is performed with the inert matrices: MgO, MgAl2O4,

  7. New limit of $^{244}$Pu on Earth points to rarity of actinide nucleosynthesis

    CERN Document Server

    Wallner, A; Feige, J; Feldstein, C; Knie, K; Korschinek, G; Kutschera, W; Ofan, A; Paul, M; Quinto, F; Rugel, G; Steier, P

    2015-01-01

    Half of the heavy elements including all actinides are produced in r-process nucleosynthesis whose sites and history still remain a mystery. If continuously produced, the Interstellar Medium (ISM) is expected to build up a quasi-steady state of abundances of short-lived nuclides (with half-lives <100My), including actinides produced in r-process nucleosynthesis. Their existence in today's ISM would serve as a radioactive clock and would establish that their production was recent. In particular $^{244}$Pu, a radioactive actinide nuclide (81 My half-life), can place strong constraints on recent r-process frequency and production yield. Here we report on the detection of live interstellar $^{244}$Pu, archived in Earth's deep-sea floor during the last 25 My, at abundances lower by about two orders of magnitude than expected from continuous production in the Galaxy. This large discrepancy may signal a rarity of actinide r-process nucleosynthesis sites, compatible with neutron-star mergers or with a small subset...

  8. A Screened Hybrid DFT Study of Actinide Oxides, Nitrides, and Carbides

    Energy Technology Data Exchange (ETDEWEB)

    Wen, Xiaodong; Martin, Richard L.; Scuseria, Gustavo E.; Rudin, Sven P.; Batista, Enrique R.

    2013-06-27

    A systematic study of the structural, electronic, and magnetic properties of actinide oxides, nitrides, and carbides (AnX1–2 with X = C, N, O) is performed using the Heyd–Scuseria–Ernzerhof (HSE) hybrid functional. Our computed results show that the screened hybrid HSE functional gives a good description of the electronic and structural properties of actinide dioxides (strongly correlated insulators) when compared with available experimental data. However, there are still some problems reproducing the electronic properties of actinide nitrides and carbides (strongly correlated metals). In addition, in order to compare with the results by HSE, the structures, electronic, and magnetic properties of these actinide compounds are also investigated in the PBE and PBE+U approximation. Interestingly, the density of states of UN obtained with PBE compares well with the experimental photoemission spectra, in contrast to the hybrid approximation. This is presumably related to the need of additional screening in the Hartree–Fock exchange term of the metallic phases.

  9. Comparison of experimental and theoretical binding and transition energies in the actinide region. [Review

    Energy Technology Data Exchange (ETDEWEB)

    Krause, M.O.; Nestor, C.W. Jr.

    1977-01-01

    The status of experimental and theoretical binding and transition energy determinations is reviewed extending the comparison between experiment and theory to encompass representative series of data for all actinides. This comprehensive comparison reveals areas where improvements may be indicated, showing whether theoretical treatments including all known contributions to the lowest order would be adequate in all instances. 45 references. (JFP)

  10. Sigma Team for Advanced Actinide Recycle FY2015 Accomplishments and Directions

    Energy Technology Data Exchange (ETDEWEB)

    Moyer, Bruce A. [Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)

    2015-09-30

    The Sigma Team for Minor Actinide Recycle (STAAR) has made notable progress in FY 2015 toward the overarching goal to develop more efficient separation methods for actinides in support of the United States Department of Energy (USDOE) objective of sustainable fuel cycles. Research in STAAR has been emphasizing the separation of americium and other minor actinides (MAs) to enable closed nuclear fuel recycle options, mainly within the paradigm of aqueous reprocessing of used oxide nuclear fuel dissolved in nitric acid. Its major scientific challenge concerns achieving selectivity for trivalent actinides vs lanthanides. Not only is this challenge yielding to research advances, but technology concepts such as ALSEP (Actinide Lanthanide Separation) are maturing toward demonstration readiness. Efforts are organized in five task areas: 1) combining bifunctional neutral extractants with an acidic extractant to form a single process solvent, developing a process flowsheet, and demonstrating it at bench scale; 2) oxidation of Am(III) to Am(VI) and subsequent separation with other multivalent actinides; 3) developing an effective soft-donor solvent system for An(III) selective extraction using mixed N,O-donor or all-N donor extractants such as triazinyl pyridine compounds; 4) testing of inorganic and hybrid-type ion exchange materials for MA separations; and 5) computer-aided molecular design to identify altogether new extractants and complexants and theory-based experimental data interpretation. Within these tasks, two strategies are employed, one involving oxidation of americium to its pentavalent or hexavalent state and one that seeks to selectively complex trivalent americium either in the aqueous phase or the solvent phase. Solvent extraction represents the primary separation method employed, though ion exchange and crystallization play an important role. Highlights of accomplishments include: Confirmation of the first-ever electrolytic oxidation of Am(III) in a

  11. Benchmark of SCALE (SAS2H) isotopic predictions of depletion analyses for San Onofre PWR MOX fuel

    Energy Technology Data Exchange (ETDEWEB)

    Hermann, O.W.

    2000-02-01

    The isotopic composition of mixed-oxide (MOX) fuel, fabricated with both uranium and plutonium, after discharge from reactors is of significant interest to the Fissile Materials Disposition Program. The validation of the SCALE (SAS2H) depletion code for use in the prediction of isotopic compositions of MOX fuel, similar to previous validation studies on uranium-only fueled reactors, has corresponding significance. The EEI-Westinghouse Plutonium Recycle Demonstration Program examined the use of MOX fuel in the San Onofre PWR, Unit 1, during cycles 2 and 3. Isotopic analyses of the MOX spent fuel were conducted on 13 actinides and {sup 148}Nd by either mass or alpha spectrometry. Six fuel pellet samples were taken from four different fuel pins of an irradiated MOX assembly. The measured actinide inventories from those samples has been used to benchmark SAS2H for MOX fuel applications. The average percentage differences in the code results compared with the measurement were {minus}0.9% for {sup 235}U and 5.2% for {sup 239}Pu. The differences for most of the isotopes were significantly larger than in the cases for uranium-only fueled reactors. In general, comparisons of code results with alpha spectrometer data had extreme differences, although the differences in the calculations compared with mass spectrometer analyses were not extremely larger than that of uranium-only fueled reactors. This benchmark study should be useful in estimating uncertainties of inventory, criticality and dose calculations of MOX spent fuel.

  12. The role of actinide burning and the Integral Fast Reactor in the future of nuclear power

    Energy Technology Data Exchange (ETDEWEB)

    Hollaway, W.R.; Lidsky, L.M.; Miller, M.M.

    1990-12-01

    A preliminary assessment is made of the potential role of actinide burning and the Integral Fast Reactor (IFR) in the future of nuclear power. The development of a usable actinide burning strategy could be an important factor in the acceptance and implementation of a next generation of nuclear power. First, the need for nuclear generating capacity is established through the analysis of energy and electricity demand forecasting models which cover the spectrum of bias from anti-nuclear to pro-nuclear. The analyses take into account the issues of global warming and the potential for technological advances in energy efficiency. We conclude, as do many others, that there will almost certainly be a need for substantial nuclear power capacity in the 2000--2030 time frame. We point out also that any reprocessing scheme will open up proliferation-related questions which can only be assessed in very specific contexts. The focus of this report is on the fuel cycle impacts of actinide burning. Scenarios are developed for the deployment of future nuclear generating capacity which exploit the advantages of actinide partitioning and actinide burning. Three alternative reactor designs are utilized in these future scenarios: The Light Water Reactor (LWR); the Modular Gas-Cooled Reactor (MGR); and the Integral Fast Reactor (FR). Each of these alternative reactor designs is described in some detail, with specific emphasis on their spent fuel streams and the back-end of the nuclear fuel cycle. Four separation and partitioning processes are utilized in building the future nuclear power scenarios: Thermal reactor spent fuel preprocessing to reduce the ceramic oxide spent fuel to metallic form, the conventional PUREX process, the TRUEX process, and pyrometallurgical reprocessing.

  13. ENHANCED CHEMICAL CLEANING OF SRS WASTE TANKS TO IMPROVE ACTINIDE SOLUBILITY

    Energy Technology Data Exchange (ETDEWEB)

    Rudisill, T.; Thompson, M.

    2011-09-20

    Processes for the removal of residual sludge from SRS waste tanks have historically used solutions containing up to 0.9 M oxalic acid to dissolve the remaining material following sludge removal. The selection of this process was based on a comparison of a number of studies performed to evaluate the dissolution of residual sludge. In contrast, the dissolution of the actinide mass, which represents a very small fraction of the waste, has not been extensively studied. The Pu, Np, and Am in the sludge is reported to be present as hydrated and crystalline oxides. To identify aqueous solutions which have the potential to increase the solubility of the actinides, the alkaline and mildly acidic test solutions shown below were selected as candidates for use in a series of solubility experiments. The efficiency of the solutions in solubilizing the actinides was evaluated using a simulated sludge prepared by neutralizing a HNO{sub 3} solution containing Pu, Np, and Am. The hydroxide concentration was adjusted to a 1.2 M excess and the solids were allowed to age for several weeks prior to starting the experiments. The sludge was washed with 0.01 M NaOH to prepare the solids for use. Following the addition of an equal portion of the solids to each test solution, the concentrations of Pu, Np, and Am were measured as a function of time over a 792 h (33 day) period to provide a direct comparison of the efficiency of each solution in solubilizing the actinide elements. Although the composition of the sludge was limited to the hydrated actinide oxides (and did not contain other components of demonstrated importance), the results of the study provides guidance for the selection of solutions which should be evaluated in subsequent tests with a more realistic surrogate sludge and actual tank waste.

  14. Correlation of retention of lanthanide and actinide complexes with stability constants and their speciation

    Energy Technology Data Exchange (ETDEWEB)

    Datta, A.; Sivaraman, N.; Viswanathan, K.S.; Ghosh, Suddhasattwa; Srinivasan, T.G.; Vasudeva Rao, P.R. [Indira Gandhi Centre for Atomic Research, Kalpakkam (India). Chemistry Group

    2013-03-01

    The present study describes a correlation that is developed from retention of lanthanide and actinide complexes with the stability constant. In these studies, an ion-pairing reagent, camphor-10-sulphonic acid (CSA) was used as the modifier and organic acids such as {alpha}-hydroxy isobutyric acid ({alpha}-HIBA), mandelic acid, lactic acid and tartaric acid were used as complexing reagent for elution. From these studies, a correlation has been established between capacity factor of a metal ion, concentration of ion-pairing reagent and complexing agent with the stability constant of metal complex. Based on these studies, it has been shown that the stability constant of lanthanide and actinide complexes can be estimated using a single lanthanide calibrant. Validation of the method was carried out with the complexing agents such as {alpha}-HIBA and lactic acid. It was also demonstrated that data from a single chromatogram can be used for estimation of stability constant at various ionic strengths. These studies also demonstrated that the method can be applied for estimation of stability constant of actinides with a ligand whose value is not reported yet, e.g., ligands of importance in the lanthanide-actinide separations, chelation therapy etc. The chromatographic separation method is fast and the estimation of stability constant can be done in a very short time, which is a significant advantage especially in dealing with radioactive elements. The stability constant data was used to derive speciation data of plutonium in different oxidation states as well as that of americium with {alpha}-HIBA. The elution behavior of actinides such as Pu and Am from reversed phase chromatographic technique could be explained based on these studies. (orig.)

  15. Actinide ion extraction using room temperature ionic liquids: opportunities and challenges for nuclear fuel cycle applications.

    Science.gov (United States)

    Mohapatra, Prasanta Kumar

    2017-02-14

    Studies on the extraction of actinide ions from radioactive feeds have great relevance in nuclear fuel cycle activities, mainly in the back end processes focused on reprocessing and waste management. Room temperature ionic liquid (RTIL) based diluents are becoming increasingly popular due to factors such as more efficient extraction vis-à-vis molecular diluents, higher metal loading, higher radiation resistance, etc. The fascinating chemistry of the actinide ions in RTIL based solvent systems due to complex extraction mechanisms makes it a challenging area of research. By the suitable tuning of the cationic and anionic parts of the ionic liquids, their physical properties such as density, dielectric constant and viscosity can be changed which are considered key parameters in metal ion extraction. Aqueous solubility of the RTILs, which can lead to significant loss in the solvent inventory, can be avoided by appending the extractant moieties onto the ionic liquid. While the low vapour pressure and non-flammability of the ionic liquids make them appear as 'green' diluents, their aqueous solubility raises concerns of environmental hazards. The present article gives a summary of studies carried out on actinide ion extraction and presents perspectives of its applications in the nuclear fuel cycle. The article discusses various extractants used for actinide ion extraction and at many places, comparison is made vis-à-vis molecular diluents which includes the nature of the extracted species and the mechanism of extraction. Results of studies on rare earth elements are also included in view of their similarities with the trivalent minor actinides.

  16. Statistical clumped isotope signatures

    NARCIS (Netherlands)

    Röckmann, T.; Popa, M. E.; Krol, M. C.; Hofmann, M. E. G.

    2016-01-01

    High precision measurements of molecules containing more than one heavy isotope may provide novel constraints on element cycles in nature. These so-called clumped isotope signatures are reported relative to the random (stochastic) distribution of heavy isotopes over all available isotopocules of a m

  17. Calcium isotopes in wine

    Science.gov (United States)

    Holmden, C. E.

    2011-12-01

    The δ 44/40Ca values of bottled wine vary between -0.76% to -1.55% on the seawater scale and correlate weakly with inverse Ca concentration and Mg/Ca ratio, such that the lowest δ 44/40Ca values have the highest Ca concentrations and lowest Mg/Ca ratios. The correlation is notable in the sense that the measured wines include both whites and reds sampled from different wine growing regions of the world, and cover a wide range of quality. Trends among the data yield clues regarding the cause of the observed isotopic fractionation. White wines, and wines generally perceived to be of lower quality, have lower δ 44/40Ca values compared to red wines and wines of generally perceived higher quality. Quality was assessed qualitatively through sensory evaluation, price, and scores assigned by critics. The relationship between δ 44/40Ca and wine quality was most apparent when comparing wines of one varietal from one producer from the same growing region. In the vineyard, wine quality is related to factors such as the tonnage of the crop and the ripeness of the grapes at the time of harvesting, the thickness of the skins for reds, the age of the vines, as well as the place where the grapes were grown (terroir). Quality is also influenced by winemaking practices such as fermentation temperature, duration of skin contact, and barrel ageing. Accordingly, the relationship between δ 44/40Ca and wine quality may originate during grape ripening in the vineyard or during winemaking in the cellar. We tested the grape ripening hypothesis using Merlot grapes sampled from a vineyard in the Okanagan, British Columbia, using sugar content (degrees Brix) as an indicator of ripeness. The grapes were separated into pulp, skin, and pip fractions and were analyzed separately. Thus far, there is no clear evidence for a systematic change in δ 44/40Ca values associated with progressive ripening of grapes in the vineyard. On the day of harvesting, the δ 44/40Ca value of juice squeezed from

  18. Isotopes in heterogeneous catalysis

    CERN Document Server

    Hargreaves, Justin SJ

    2006-01-01

    The purpose of this book is to review the current, state-of-the-art application of isotopic methods to the field of heterogeneous catalysis. Isotopic studies are arguably the ultimate technique in in situ methods for heterogeneous catalysis. In this review volume, chapters have been contributed by experts in the field and the coverage includes both the application of specific isotopes - Deuterium, Tritium, Carbon-14, Sulfur-35 and Oxygen-18 - as well as isotopic techniques - determination of surface mobility, steady state transient isotope kinetic analysis, and positron emission profiling.

  19. Generation of Radixenon Isotopes

    Energy Technology Data Exchange (ETDEWEB)

    McIntyre, Justin I.; Bowyer, Ted W.; Hayes, James C.; Heimbigner, Tom R.; Morris, Scott J.; Panisko, Mark E.; Pitts, W. K.; Pratt, Sharon L.; Reeder, Paul L.; Thomas, Charles W.

    2003-06-30

    Pacific Northwest National Laboratory has developed an automated system for separating Xe from air and can detect the following radioxenon isotopes, 131mXe, 133mXe, 133Xe, and 135Xe. This report details the techniques used to generate the various radioxenon isotopes that are used for the calibration of the detector as well as other isotopes that have the potential to interfere with the fission produced radioxenon isotopes. Fission production is covered first using highly enriched uranium followed by a description and results from an experiment to produce radioxenon isotopes from neutron activation of ambient xenon.

  20. Isotopic modeling of the sub-cloud evaporation effect in precipitation.

    Science.gov (United States)

    Salamalikis, V; Argiriou, A A; Dotsika, E

    2016-02-15

    In dry and warm environments sub-cloud evaporation influences the falling raindrops modifying their final stable isotopic content. During their descent from the cloud base towards the ground surface, through the unsaturated atmosphere, hydrometeors are subjected to evaporation whereas the kinetic fractionation results to less depleted or enriched isotopic signatures compared to the initial isotopic composition of the raindrops at cloud base. Nowadays the development of Generalized Climate Models (GCMs) that include isotopic content calculation modules are of great interest for the isotopic tracing of the global hydrological cycle. Therefore the accurate description of the underlying processes affecting stable isotopic content can improve the performance of iso-GCMs. The aim of this study is to model the sub-cloud evaporation effect using a) mixing and b) numerical isotope evaporation models. The isotope-mixing evaporation model simulates the isotopic enrichment (difference between the ground and the cloud base isotopic composition of raindrops) in terms of raindrop size, ambient temperature and relative humidity (RH) at ground level. The isotopic enrichment (Δδ) varies linearly with the evaporated raindrops mass fraction of the raindrop resulting to higher values at drier atmospheres and for smaller raindrops. The relationship between Δδ and RH is described by a 'heat capacity' model providing high correlation coefficients for both isotopes (R(2)>80%) indicating that RH is an ideal indicator of the sub-cloud evaporation effect. Vertical distribution of stable isotopes in falling raindrops is also investigated using a numerical isotope-evaporation model. Temperature and humidity dependence of the vertical isotopic variation is clearly described by the numerical isotopic model showing an increase in the isotopic values with increasing temperature and decreasing RH. At an almost saturated atmosphere (RH=95%) sub-cloud evaporation is negligible and the isotopic

  1. Production of actinide nuclei by multi-nucleon transfer

    Energy Technology Data Exchange (ETDEWEB)

    Lauritsen, T.; Ahmad, I.; Carpenter, M.P. [and others

    1995-08-01

    Multi-nucleon transfers have increasingly allowed us to reach parts of the nuclear chart where regular compound nuclear reactions are prohibited. The interesting region of Ra and Rn, where a rich tapestry of nuclear structure manifests itself, is now accessible using this technique of deep inelastic scattering. In particular, these nuclei are predicted to lie at the onset of octupole deformation and the region is rich in examples of shape coexistence. There are several theoretical predictions of nuclear structure of these nuclei that have not been experimentally tested. Moreover, there is serious disagreement among these theories. We used a beam of {sup 136}Xe at 720 MeV from ATLAS on a target of {sup 232}Th to produce a range of Rn isotopes, with a mass from 220 to 224, and Ra isotopes with masses greater than 222. The beam energy, target and beam were selected carefully to enhance the cross-section for production of these nuclei and reduce the Doppler broadening of the gamma rays that were observed in the Argonne Notre Dame gamma-ray facility. The 12 germanium detectors of this array allowed the observation of gamma-gamma coincidences. The inner ball of 50 BGO detectors allowed us to record the multiplicity and sum-energy information for each event. The latter should permit us to determine the entry region in the products of the transfer reaction. We had four successful days of beam-time, when we collected in excess of 8 x 10{sup 7} events. Data analysis is in progress at the University of Liverpool. A complete set of spectroscopic information on the yrast structure of the many nuclei produced in this reaction is being extracted.

  2. Improved Fission Neutron Data Base for Active Interrogation of Actinides

    Energy Technology Data Exchange (ETDEWEB)

    Pozzi, Sara; Czirr, J. Bart; Haight, Robert; Kovash, Michael; Tsvetkov, Pavel

    2013-11-06

    This project will develop an innovative neutron detection system for active interrogation measurements. Many active interrogation methods to detect fissionable material are based on the detection of neutrons from fission induced by fast neutrons or high-energy gamma rays. The energy spectrum of the fission neutrons provides data to identify the fissionable isotopes and materials such as shielding between the fissionable material and the detector. The proposed path for the project is as follows. First, the team will develop new neutron detection systems and algorithms by Monte Carlo simulations and bench-top experiments. Next, They will characterize and calibrate detection systems both with monoenergetic and white neutron sources. Finally, high-fidelity measurements of neutron emission from fissions induced by fast neutrons will be performed. Several existing fission chambers containing U-235, Pu-239, U-238, or Th-232 will be used to measure the neutron-induced fission neutron emission spectra. The challenge for making confident measurements is the detection of neutrons in the energy ranges of 0.01 – 1 MeV and above 8 MeV, regions where the basic data on the neutron energy spectrum emitted from fission is least well known. In addition, improvements in the specificity of neutron detectors are required throughout the complete energy range: they must be able to clearly distinguish neutrons from other radiations, in particular gamma rays and cosmic rays. The team believes that all of these challenges can be addressed successfully with emerging technologies under development by this collaboration. In particular, the collaboration will address the area of fission neutron emission spectra for isotopes of interest in the advanced fuel cycle initiative (AFCI).

  3. MOLECULAR SPECTROSCPY AND REACTIONS OF ACTINIDES IN THE GAS PHASE AND CRYOGENIC MATRICES

    Energy Technology Data Exchange (ETDEWEB)

    Heaven, Michael C.; Gibson, John K.; Marcalo, Joaquim

    2009-02-01

    In this chapter we review the spectroscopic data for actinide molecules and the reaction dynamics for atomic and molecular actinides that have been examined in the gas phase or in inert cryogenic matrices. The motivation for this type of investigation is that physical properties and reactions can be studied in the absence of external perturbations (gas phase) or under minimally perturbing conditions (cryogenic matrices). This information can be compared directly with the results from high-level theoretical models. The interplay between experiment and theory is critically important for advancing our understanding of actinide chemistry. For example, elucidation of the role of the 5f electrons in bonding and reactivity can only be achieved through the application of experimentally verified theoretical models. Theoretical calculations for the actinides are challenging due the large numbers of electrons that must be treated explicitly and the presence of strong relativistic effects. This topic has been reviewed in depth in Chapter 17 of this series. One of the goals of the experimental work described in this chapter has been to provide benchmark data that can be used to evaluate both empirical and ab initio theoretical models. While gas-phase data are the most suitable for comparison with theoretical calculations, there are technical difficulties entailed in generating workable densities of gas-phase actinide molecules that have limited the range of species that have been characterized. Many of the compounds of interest are refractory, and problems associated with the use of high temperature vapors have complicated measurements of spectra, ionization energies, and reactions. One approach that has proved to be especially valuable in overcoming this difficulty has been the use of pulsed laser ablation to generate plumes of vapor from refractory actinide-containing materials. The vapor is entrained in an inert gas, which can be used to cool the actinide species to room

  4. Sulfur Isotopic Characteristics of Coal in China and Sulfur Isotopic Fractionation during Coal—burning Process

    Institute of Scientific and Technical Information of China (English)

    洪业汤; 张鸿斌; 等

    1993-01-01

    The determined results of the sulfur contents and isotopic composition of coal samples from major coal mines in 15 provinces and regions of China show that the coal mined in the north of China is characterized by higher 34S and lower sulfur content, but that in the south of China has lower 34S and higher sulfur content.During the coal-burning process in both indrstrial and daily use of coal as fuel the released sulfur dioxide is always enriched in lighter sulfur isotope relative to the corresponding coal;the particles are always enriched in heavier sulfur isotope.The discussion on the environmental geochemical significance of the above-mentioned results also has been made.

  5. Calculations of the actinide transmutation with HELIOS for fuels of light water reactors; Calculos de la transmutacion de actinidos con HELIOS para combustibles de reactores de agua ligera

    Energy Technology Data Exchange (ETDEWEB)

    Francois L, J.L.; Guzman A, J.R. [UNAM-FI, Laboratorio de Analisis en Ingenieria de Reactores Nucleares, Paseo Cuauhnahuac 8532, Jiutepec, Morelos (Mexico)]. e-mail: jlfl@fi-b.unam.mx

    2006-07-01

    In this work a comparison of the obtained results with the HELIOS code is made and those obtained by other similar codes, used in the international community, respect to the transmutation of smaller actinides. For this the one it is analyzed the international benchmark: 'Calculations of Different Transmutation Concepts', of the Nuclear Energy Agency. In this benchmark two cell types are analyzed: one small corresponding to a PWR standard, and another big one corresponding to a PWR highly moderated. Its are considered two types of burnt of discharge: 33 GWd/tHM and 50 GWd/tHM. The following types of results are approached: the k{sub eff} like a function of the burnt one, the atomic densities of the main isotopes of the actinides, the radioactivities in the moment in that the reactor it is off and in the times of cooling from 7 up to 50000 years, the reactivity by holes and the Doppler reactivity. The results are compared with those obtained by the following institutions: FZK (Germany), JAERI (Japan), ITEP (Russia) and IPPE (Russian Federation). In the case of the eigenvalue, the obtained results with HELIOS showed a discrepancy around 3% {delta}k/k, which was also among other participants. For the isotopic concentrations: {sup 241}Pu, {sup 242} Pu and {sup 242m} Am the results of all the institutions present a discrepancy bigger every time, as the burnt one increases. Regarding the activities, the discrepancy of results is acceptable, except in the case of the {sup 241} Pu. In the case of the Doppler coefficients the discrepancy of results is acceptable, except for the cells with high moderation; in the case of the holes coefficients, the discrepancy of results increases in agreement with the holes fraction increases, being quite high to 95% of holes. In general, the results are consistent and in good agreement with those obtained by all the participants in the benchmark. The results are inside of the established limits by the work group on Plutonium Fuels

  6. Development of non-lethal methods for investigation of actinide uptake by wildlife

    Energy Technology Data Exchange (ETDEWEB)

    Johansen, M.; Child, D.; Davis, E.; Harrison, J.; Hotchkis, M.; Payne, T.; Thiruvoth, S. [Australian Nuclear Science and Technology Org. (Australia); Wood, M. [University of Salford (United Kingdom)

    2014-07-01

    There is growing interest in the use of non-lethal methods in radioecology and an International Union of Radioecology Task Group has been established to facilitate international cooperation in this field (http://iur-uir.org/en/task-groups/id-19-non-lethal-methods-in-radioecology). In this paper, we evaluate the use of lethally-, and non-lethally obtained samples (various body tissues, excreta and blood withdrawals as well as parasites and found bones) as indicators of contamination. Samples of mammals and reptiles were collected from the semi-arid former weapons test site at Maralinga, Australia and analysed for thorium, plutonium, and uranium isotopes by accelerator mass spectrometry and alpha-spectrometry. Most samples were of low mass and presented analytical challenges as a result. The plutonium concentrations in blood withdrawn from the marginal ear veins of Oryctolagus cuniculus (European rabbit) were successfully analysed using small samples (0.2 -7.9 ml, below the ∼10 ml threshold for safe extraction of blood from these rabbits). The results demonstrate that small-volume blood samples can serve as indicators of the presence of plutonium absorbed within other tissues (e.g., muscle, bone). However, the magnitude of the blood plutonium masses were poorly correlated with those in muscle and bone due to the presence of a small number of outliers (without the outliers, correlations improved to r = +0.66 and r = +0.51 for muscle and bone respectively). The activity concentrations in parasitic ticks were relatively high compared with those of their hosts Pseudomys hermannsburgensis (sandy inland mouse) and Ctenophorus cristatus (crested dragon lizard). Successful measurement of tick samples indicates a potential for use of parasites as general indicators of contamination within host organisms. The concentrations of actinides in found bones of Macropus rufus (red kangaroo) and O. cuniculus demonstrated potential for their use as indicators of the areal extent of

  7. Neutron capture measuremetns on minor actinides at the n_TOF facility at CERN: past, present and future

    OpenAIRE

    Cano Ott, Daniel; Colonna, Nicola; Tagliente, G.; Belloni, Fabio; Calviño Tavares, Francisco; Cortés Rossell, Guillem Pere; Poch Parés, Agustí; Pretel Sánchez, Carme

    2011-01-01

    The successful development of advanced nuclear systems for sustainable energy production and nuclear waste management depends on high quality nuclear data libraries. Recent sensitivity stud- ies and reports [1-3] have identi ed the need for substantially improving the accuracy of neutron cross-section data for minor actinides. The n TOF collaboration has initiated an ambitious exper- imental program for the measurement of neutron capture cross sections of minor actinides. Two e...

  8. Lanthanides and actinides extraction by calixarenes containing CMPO groups; Extraction des lanthanides et des actinides au moyen de calixarenes portant des groupements CMPO

    Energy Technology Data Exchange (ETDEWEB)

    Garcia Carrera, A

    2001-07-01

    In the framework of the French program SPIN concerning the radioactive waste management, researches are performed to develop processes allowing the separation of long-lived radioisotopes in order to their transmutation or their specific conditioning. These studies deal with the extraction and the separation of trivalent lanthanides and actinides in acid solution. Many systems ''calixarene-diluent-aqueous phase'' are examined by extraction liquid-liquid and membrane transport. The extraction efficiency and the selectivity of the synthesized calixarene-CMPO and of the CMPO are compared with these cations, as the nitric acid extraction by these molecules. (A.L.B.)

  9. Iron isotopic fractionation during continental weathering

    Energy Technology Data Exchange (ETDEWEB)

    Fantle, Matthew S.; DePaolo, Donald J.

    2003-10-01

    The biological activity on continents and the oxygen content of the atmosphere determine the chemical pathways through which Fe is processed at the Earth's surface. Experiments have shown that the relevant chemical pathways fractionate Fe isotopes. Measurements of soils, streams, and deep-sea clay indicate that the {sup 56}Fe/{sup 54}Fe ratio ({delta}{sup 56}Fe relative to igneous rocks) varies from +1{per_thousand} for weathering residues like soils and clays, to -3{per_thousand} for dissolved Fe in streams. These measurements confirm that weathering processes produce substantial fractionation of Fe isotopes in the modern oxidizing Earth surface environment. The results imply that biologically-mediated processes, which preferentially mobilize light Fe isotopes, are critical to Fe chemistry in weathering environments, and that the {delta}{sup 56}Fe of marine dissolved Fe should be variable and negative. Diagenetic reduction of Fe in marine sediments may also be a significant component of the global Fe isotope cycle. Iron isotopes provide a tracer for the influence of biological activity and oxygen in weathering processes through Earth history. Iron isotopic fractionation during weathering may have been smaller or absent in an oxygen-poor environment such as that of the early Precambrian Earth.

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

    Science.gov (United States)

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

    2016-03-01

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

  11. Alpha decay and cluster decay of some neutron-rich actinide nuclei

    Indian Academy of Sciences (India)

    G M CARMEL VIGILA BAI; R NITHYA AGNES

    2017-03-01

    Nuclei in the actinide region are good in exhibiting cluster radioactivity. In the present work, the half-lives of $\\alpha$-decay and heavy cluster emission from certain actinide nuclei have been calculated using cubic plus Yukawa plus exponential model ($\\bf{CYEM}$). Our model has a cubic potential for the overlapping region which is smoothly connected by a Yukawa plus exponential potential for the region after separation. The computed half-lives are compared with those of other theoretical models and are found to be in good agreement with each other. In this work, we have also studied the deformation effects on half-lives of cluster decay. These deformation effects lower the half-life values and it is also found that the neutron-rich parent nuclei slow down the cluster decay process. Geiger–Nuttal plots for various clusters are found to be linear and most of the emitted clusters are $\\alpha$-like nuclei.

  12. Actinides sorption onto hematite. Experimental data, surface complexation modeling and linear free energy relationship

    Energy Technology Data Exchange (ETDEWEB)

    Romanchuk, Anna Y.; Kalmykov, Stephan N. [Lomonosov Moscow State Univ., Moscow (Russian Federation). Dept. of Chemistry

    2014-07-01

    The sorption of actinides in different valence states - Am(III), Th(IV), Np(V) and U(VI) onto hematite have been revisited with the special emphasis on the equilibrium constants of formation of surface species. The experimental sorption data have been treated using surface complexation modeling from which the set of new values of equilibrium constants were obtained. Formation of inner sphere monodentate surface species adequately describes the pH-sorption edges for actinide ions indicative the ionic electrostatic nature of bonding with small or no covalency contribution. The linear free energy relationship representing the correlation between the hydrolysis constants and surface complexation constants has been developed for various cations including K(I), Li(I), Na(I), Ag(I), Tl(I), Sr(II), Cu(II), Co(II), La(III), Eu(III), Ga(III), Am(III), Th(IV), Np(V), U(VI). (orig.)

  13. Selective Media for Actinide Collection and Pre-Concentration: Results of FY 2006 Studies

    Energy Technology Data Exchange (ETDEWEB)

    Lumetta, Gregg J.; Addleman, Raymond S.; Hay, Benjamin P.; Hubler, Timothy L.; Levitskaia, Tatiana G.; Sinkov, Sergey I.; Snow, Lanee A.; Warner, Marvin G.; Latesky, Stanley L.

    2006-11-17

    In this work, we have investigated new materials for potential use in automated radiochemical separations. The work can be divided into three primary tasks: (1) synthesis of new ligands with high affinity for actinide ions, (2) evaluation of new materials for actinide ion affinity, and (3) computational design of advanced ligand architectures for highly selective binding of actinide ions. Ligand Synthesis Work was conducted on synthesizing Kl?ui ligand derivatives containing functionalized pendant groups on the cyclopentadienyl ring. The functionalized pendent groups would allow these ligands to be attached to organic and inorganic solid supports. This work focused on synthesizing the compound Na[Cp?Co(PO(OC2H5)2)3], where Cp?= C5H4C(O)OCH3. Synthesizing this compound is feasible, but the method used in FY 2006 produced an impure material. A modified synthetic scheme has been developed and will be pursued in FY 2007. Work was also initiated on synthesizing bicyclic diamides functionalized for binding to polymeric resins or other surfaces. Researchers at the University of Oregon are collaborators in this work. To date, this effort has focused on synthesizing and characterizing a symmetrically substituted bicyclic diamide ligand with the ?COOH functionality. Again, this synthetic effort will continue into FY 2007. Separations Material Evaluation Work was conducted in FY 2006 to provide a more extensive set of data on the selectivity and affinity of extraction chromatography resins prepared by sorption of Kl?ui ligand onto an inert macroreticular polymeric support. Consistent with previous observations, it was found that these materials strongly bind tetravalent actinides. These materials also adsorb trivalent actinides at low nitric acid concentrations, but the affinity for the trivalent actinides decreases with increasing nitric acid concentration. These materials have relatively low affinity for U(VI), but they do sorb U(VI) to a greater extent than Am(III) at [HNO

  14. Detailed studies of Minor Actinide transmutation-incineration in high-intensity neutron fluxes

    Energy Technology Data Exchange (ETDEWEB)

    Bringer, O. [CEA/Saclay/DSM/DAPNIA, Gif-sur-Yvette (France); Al Mahamid, I. [Lawrence Berkeley National Laboratory, E.H. and S. Div., CA (United States); Blandin, C. [CEA/Cadarache/DEN/DER/SPEX, Saint-Paul-lez-Durances (France); Chabod, S. [CEA/Saclay/DSM/DAPNIA, Gif-sur-Yvette (France); Chartier, F. [CEA/Cadarache/DEN/DPC/SECR, Gif-sur-Yvette (France); Dupont, E.; Fioni, G. [CEA/Saclay/DSM/DAPNIA, Gif-sur-Yvette (France); Isnard, H. [CEA/Cadarache/DEN/DPC/SECR, Gif-sur-Yvette (France); Letourneau, A.; Marie, F. [CEA/Saclay/DSM/DAPNIA, Gif-sur-Yvette (France); Mutti, P. [Institut Laue-Langevin, Grenoble (France); Oriol, L. [CEA/Cadarache/DEN/DER/SPEX, Saint-Paul-lez-Durances (France); Panebianco, S.; Veyssiere, C. [CEA/Saclay/DSM/DAPNIA, Gif-sur-Yvette (France)

    2006-07-01

    The Mini-INCA project is dedicated to the measurement of incineration-transmutation chains and potentials of minor actinides in high-intensity thermal neutron fluxes. In this context, new types of detectors and methods of analysis have been developed. The {sup 241}Am and {sup 232}Th transmutation-incineration chains have been studied and several capture and fission cross sections measured very precisely, showing some discrepancies with existing data or evaluated data. An impact study was made on different based-like GEN-IV reactors. It underlines the necessity to proceed to precise measurements for a large number of minor-actinides that contribute to these future incineration scenarios. (authors)

  15. Engineering test plan for US/UK higher actinides irradiations tests

    Energy Technology Data Exchange (ETDEWEB)

    Basmajian, J A

    1981-03-01

    The objective of the Higher Actinides Irradiations Program is to verify the neutronic and irradiation performance of americium and curium oxides in a fast reactor. The data obtained from the irradiation will be used to assess the basic neutronics parameters for actinide elements and determine the irradiation potential of the oxides of {sup 241}Am and {sup 244}Cm. This information has application in breeder reactor physics, fuel cycle analysis and assessment of waste management options. The irradiation test program is a cooperative effort wherein the US is supplying the completed irradiation test pins, while the UK will perform the irradiation in their Prototype Fast Reactor (PFR). Postirradiation examination and data analyses will be conducted on a cooperative basis, with some examinations performed in the UK and others in the US. 5 figs., 5 tabs.

  16. Neutron nuclear data evaluation of actinide nuclei for CENDL-3.1

    Institute of Scientific and Technical Information of China (English)

    CHEN Guo-Chang; CAO Wen-Tian; YU Bao-Sheng; TANG Guo-You; SHI Zhao-Min; TAO Xi

    2012-01-01

    New evaluations for several actinide nuclei of the third version of Chinese Evaluated Nuclear Data Library for Neutron Reaction Data (CENDL-3.1) have been completed and released.The evaluation is for all neutron induced reactions with uranium,neptunium,plutonium and americium in the mass range A=232-241,236-239,236-246 and 240-244,respectively,and cover the incident neutron energy up to 20 MeV.In the present evaluation,much more effort was devoted to improving the reliability of the evaluated nuclear data for available new measured data,especially scarce or absent experimental data.A general description for the evaluation of several actinides' data is presented.

  17. Simulation of alpha decay of actinides in iron phosphate glasses by ion irradiation

    Energy Technology Data Exchange (ETDEWEB)

    Dube, Charu L., E-mail: dubecharu@gmail.com; Stennett, Martin C.; Gandy, Amy S.; Hyatt, Neil C.

    2016-03-15

    Highlights: • Alpha decay of actinides in iron phosphate glasses is simulated by employing ion irradiation technique. • FTIR and Raman spectroscopic measurements confirm modification of glass network. • The depolymerisation of glass network after irradiation is attributed to synergetic effect of nuclear and electronic losses. - Abstract: A surrogate approach of ion beam irradiation is employed to simulate alpha decay of actinides in iron phosphate nuclear waste glasses. Bismuth and helium ions of different energies have been selected for simulating glass matrix modification owing to radiolysis and ballistic damage due to recoil atoms. Structural modification and change in coordination number of network former were probed by employing Reflectance Fourier-Transform Infrared (FT-IR), and Raman spectroscopies as a consequence of ion irradiation. Depolymerisation is observed in glass sample irradiated at intermediate energy of 2 MeV. Helium blisters of micron size are seen in glass sample irradiated at low helium ion energy of 30 keV.

  18. Odd–even effect in fragment angular momentum in low-energy fission of actinides

    Indian Academy of Sciences (India)

    B S Tomar; R Tripathi; A Goswami

    2007-01-01

    Quantitative explanation for the odd–even effect on fragment angular momenta in the low-energy fission of actinides have been provided by taking into account the single particle spin of the odd proton at the fragment's scission point deformation in the case of odd- fragments along with the contribution from the population of angular momentum bearing collective vibrations of the fissioning nucleus at scission point. The calculated fragment angular momenta have been found to be in very good agreement with the experimental data for fragments in the mass number region of 130–140. The odd–even effect observed in the fragment angular momenta in the low-energy fission of actinides has been explained quantitatively for the first time.

  19. Advancing Chemistry with the Lanthanide and Actinide Elements: Final Report, September 2013

    Energy Technology Data Exchange (ETDEWEB)

    Evans, William John [Univ. of California, Irvine, CA (United States). Dept. of Chemistry

    2013-09-11

    The objective of this research is to use the unique chemistry available from complexes of the lanthanides and actinides, as well as related heavy metals such as scandium, yttrium, and bismuth to advance chemistry in energy-related areas. The lanthanides and actinides have a combination of properties in terms of size, charge, electropositive character, and f valence orbitals that provides special opportunities to probe reactivity and catalysis in ways not possible with the other metals in the periodic table. We seek to discover reaction pathways and structural types that reveal new options in reaction chemistry related to energy. Identification of new paradigms in structure and reactivity should stimulate efforts to develop new types of catalytic processes that at present are not under consideration because either the transformation or the necessary intermediates are unknown.

  20. Actinide neutron induced cross section measurements using the oscillation technique in the Minerve reactor

    Energy Technology Data Exchange (ETDEWEB)

    Bernard, B.; Leconte, P.; Gruel, A.; Antony, M.; Di-Salvo, J.; Hudelot, J.P.; Pepino, A.; Lecluze, A. [CEA Cadarache, DEN/CAD/DER/SPRC/LEPh, 13 - Saint-Paul-lez-Durance (France)

    2009-07-01

    CEA is deeply involved research programs concerning nuclear fuel advanced studies (actinides, plutonium), waste management, the scientific and technical support of French PWR reactors and EPR reactor, and innovative systems. In this framework, specific neutron integral experiments have been carried out in the critical ZPR (zero power reactor) facilities of the CEA at Cadarache such as MINERVE, EOLE and MASURCA. This paper deals with MINERVE Pool Reactor experiments. MINERVE is mainly devoted to neutronics studies of different reactor core types. The aim is to improve the knowledge of the integral absorption cross sections of actinides (OSMOSE program), of new absorbers (OCEAN program) and also for fission Products (CBU program) in thermal, epithermal and fast neutron spectra. (authors)

  1. Evaluation and testing of sequestering agents for the removal of actinides from waste streams

    Energy Technology Data Exchange (ETDEWEB)

    Hoffman, D.C.; Romanovski, V.V.; Veeck, A.C. [Lawrence Livermore National Lab., CA (United States)] [and others

    1997-10-01

    The purpose of this project is to evaluate and test the complexing ability of a variety of promising new complexing agents synthesized by Professor Kenneth Raymond`s group at the University of California, Berkeley (ESP-CP TTP Number SF16C311). Some of these derivatives have already shown the potential for selectivity binding Pu(IV) in a wide range of solutions in the presence of other metals. Professor Raymond`s group uses molecular modeling to design and synthesize ligands based on modification of natural siderophores, or their analogs, for chelation of actinides. The ligands are then modified for use as liquid/liquid and solid/liquid extractants. The authors` group at the Glenn T. Seaborg Institute for Transactinium Science (ITS) at Lawrence Livermore National Laboratory determines the complex formation constants between the ligands and actinide ions, the capacity and time dependence for uptake on the resins, and the effect of other metal ions and pH.

  2. A many-body potential approach to modelling the thermomechanical properties of actinide oxides.

    Science.gov (United States)

    Cooper, M W D; Rushton, M J D; Grimes, R W

    2014-03-12

    A many-body potential model for the description of actinide oxide systems, which is robust at high temperatures, is reported for the first time. The embedded atom method is used to describe many-body interactions ensuring good reproduction of a range of thermophysical properties (lattice parameter, bulk modulus, enthalpy and specific heat) between 300 and 3000 K for AmO2, CeO2, CmO2, NpO2, ThO2, PuO2 and UO2. Additionally, the model predicts a melting point for UO2 between 3000 and 3100 K, in close agreement with experiment. Oxygen-oxygen interactions are fixed across the actinide oxide series because it facilitates the modelling of oxide solid solutions. The new potential is also used to predict the energies of Schottky and Frenkel pair disorder processes.

  3. Design of an Actinide Burning, Lead-Bismuth Cooled Reactor That Produces Low Cost Electricity

    Energy Technology Data Exchange (ETDEWEB)

    C. Davis; S. Herring; P. MacDonald; K. McCarthy; V. Shah; K. Weaver (INEEL); J. Buongiorno; R. Ballinger; K. Doyoung; M. Driscoll; P. Hejzler; M. Kazimi; N. Todreas (MIT)

    1999-07-01

    The purpose of this project is to investigate the suitability of lead-bismuth cooled fast reactors for producing low-cost electricity as well as for actinide burning. The goal is to identify and analyze the key technical issues in core neutronics, materials, thermal-hydraulics, fuels, and economics associated with the development of this reactor concept. The choice of lead-bismuth for the reactor coolant is an actinide burning fast reactor offers enhanced safety and reliability. The advantages of lead-bismuth over sodium as a coolant are related to the following material characteristics: chemical inertness with air and water; higher atomic number; lower vapor pressure at operating temperatures; and higher boiling temperature. Given the status of the field, it was agreed that the focus of this investigation in the first two years will be on the assessment of approaches to optimize core and plant arrangements in order to provide maximum safety and economic potential in this type of reactor.

  4. f-state luminescence of lanthanide and actinide ions in solution

    Energy Technology Data Exchange (ETDEWEB)

    Beitz, J.V.

    1993-09-01

    Detailed studies of the luminescence of aquated Am{sup 3+} are presented in the context of prior lanthanide and actinide ion work. The luminescing state of aquated Am{sup 3+} is confirmed to be {sup 5}D{sub l} based on observed emission and excitation spectra. The luminescence lifetime of Am{sup 3+} in H{sub 2}O solution is (22 {plus_minus} 3) ns and (155 {plus_minus} 4) ns in D{sub 2}O solution at 295 K. Judd-Ofelt transition intensity theory qualitatively describes the observed Am{sup 3+} relative integrated fluorescence intensities. Recent luminescence studies on complexed trivalent f-element ions in solution are reviewed as to the similarities and differences between lanthanide ion 4f state and actinide ion 5f state properties.

  5. Angular distribution in the neutron-induced fission of actinides

    Directory of Open Access Journals (Sweden)

    Leong L.S.

    2013-12-01

    Full Text Available Above 1 MeV of incident neutron energy the fission fragment angular distribution (FFAD has generally a strong anisotropic behavior due to the combination of the incident orbital momentum and the intrinsic spin of the fissioning nucleus. This effect has to be taken into account for the efficiency estimation of devices used for fission cross section measurements. In addition it bears information on the spin deposition mechanism and on the structure of transitional states. We designed and constructed a detection device, based on Parallel Plate Avalanche Counters (PPAC, for measuring the fission fragment angular distributions of several isotopes, in particular 232Th. The measurement has been performed at n_TOF at CERN taking advantage of the very broad energy spectrum of the neutron beam. Fission events were recognized by back to back detection in coincidence in two position-sensitive detectors surrounding the targets. The detection efficiency, depending mostly on the stopping of fission fragments in backings and electrodes, has been computed with a Geant4 simulation and validated by the comparison to the measured case of 235U below 3 keV where the emission is isotropic. In the case of 232Th, the result is in good agreement with previous data below 10 MeV, with a good reproduction of the structures associated to vibrational states and the opening of second chance fission. In the 14 MeV region our data are much more accurate than previous ones which are broadly scattered.

  6. Strategic Design and Optimization of Inorganic Sorbents For Cesium, Strontium and Actinides

    Energy Technology Data Exchange (ETDEWEB)

    Hobbs, D.; Nyman, M.; Clearfield, A.; Maginn, E.

    2006-06-01

    The basic science goal in this project identifies structure/affinity relationships for selected radionuclides and existing sorbents. The task will apply this knowledge to the design and synthesis of new sorbents that will exhibit increased affinity for cesium, strontium and actinide separations. The target problem focuses on the treatment of high-level nuclear wastes. The general approach can likewise be applied to nonradioactive separations.

  7. Synthesis and Characterization of Templated Ion Exchange Resins for the Selective Complexation of Actinide Ions

    Energy Technology Data Exchange (ETDEWEB)

    Uy, O. Manual

    2001-03-01

    The purpose of this research is to develop a polymeric extractant for the selective complexation of uranyl ions (and subsequently other actinyl and actinide ions) from aqueous solutions (lakes, streams, waste tanks and even body fluids). Chemical insights into what makes a good complexation site will be used to synthesize reagents tailor-made for the complexation of uranyl and other actinide ions. These insights, derived from studies of molecular recognition include ion coordination number and geometry, ionic size and ionic shape, as well as ion to ligand thermodynamic affinity. Selectivity for a specific actinide ion will be obtained by providing the polymers with cavities lined with complexing ligands so arranged as to match the charge, coordination number, coordination geometry, and size of the actinide metal ion. These cavity-containing polymers will be produced by using a specific ion (or surrogate) as a template around which monomeric complexing ligands will be polymerized. The complexing ligands will be ones containing functional groups known to form stable complexes with a specific ion and less stable complexes with other cations. Prior investigator's approaches for making templated resins for metal ions have had marginal success. We have extended and amended these methodologies in our work with Pb(II) and uranyl ion, by changing the order of the steps, by the inclusion of sonication, by using higher complex loading, and the selection of functional groups with better complexation constants. This has resulted in significant improvements to selectivity. The unusual shape of the uranyl ion suggests that this approach will result in even greater selectivities than already observed for Pb(II). Preliminary data obtained for uranyl templated polymers shows unprecedented selectivity and has resulted in the first ion selective electrode for uranyl ion.

  8. Measurement of actinides in environmental samples by Photo-Electron Rejecting Alpha Liquid Scintillation

    Energy Technology Data Exchange (ETDEWEB)

    Cadieux, J.R. [Westinghouse Savannah River Co., Aiken, SC (United States); Clark, S. [Savannah River Ecology Lab., Univ. of Georgia (United States); Fjeld, R.A.; Reboul, S.; Sowder, A. [Clemson Univ., SC (United States). Dept. of Environmental Systems Engineering

    1994-05-01

    This work describes the adaptation of extractive scintillation with a Photo-Electron Rejecting Alpha Liquid Scintillation (PERALS) (ORDELA, Inc.) spectrometer to the analysis of actinides in environmental samples from the Savannah River Site (SRS). Environmental quality assurance standards and actual water samples were treated by one of two methods; either a two step direct extraction, or for more complex samples, pretreatment by an extraction chromatographic separation prior to measurement of the alpha activity by PERALS.

  9. Influence of microorganisms on the oxidation state distribution of multivalent actinides under anoxic conditions

    Energy Technology Data Exchange (ETDEWEB)

    Reed, Donald Timothy [Los Alamos National Laboratory; Borkowski, Marian [Los Alamos National Laboratory; Lucchini, Jean - Francois [Los Alamos National Laboratory; Ams, David [Los Alamos National Laboratory; Richmann, M. K. [Los Alamos National Laboratory; Khaing, H. [Los Alamos National Laboratory; Swanson, J. S. [Los Alamos National Laboratory

    2010-12-10

    The fate and potential mobility of multivalent actinides in the subsurface is receiving increased attention as the DOE looks to cleanup the many legacy nuclear waste sites and associated subsurface contamination. Plutonium, uranium and neptunium are the near-surface multivalent contaminants of concern and are also key contaminants for the deep geologic disposal of nuclear waste. Their mobility is highly dependent on their redox distribution at their contamination source as well as along their potential migration pathways. This redox distribution is often controlled, especially in the near-surface where organic/inorganic contaminants often coexist, by the direct and indirect effects of microbial activity. Under anoxic conditions, indirect and direct bioreduction mechanisms exist that promote the prevalence of lower-valent species for multivalent actinides. Oxidation-state-specific biosorption is also an important consideration for long-term migration and can influence oxidation state distribution. Results of ongoing studies to explore and establish the oxidation-state specific interactions of soil bacteria (metal reducers and sulfate reducers) as well as halo-tolerant bacteria and Archaea for uranium, neptunium and plutonium will be presented. Enzymatic reduction is a key process in the bioreduction of plutonium and uranium, but co-enzymatic processes predominate in neptunium systems. Strong sorptive interactions can occur for most actinide oxidation states but are likely a factor in the stabilization of lower-valent species when more than one oxidation state can persist under anaerobic microbiologically-active conditions. These results for microbiologically active systems are interpreted in the context of their overall importance in defining the potential migration of multivalent actinides in the subsurface.

  10. Actinide partitioning and transmutation program. Progress report, July 1--September 30, 1977

    Energy Technology Data Exchange (ETDEWEB)

    Tedder, D.W.; Blomeke, J.O. (comps.)

    1978-02-01

    In Purex process modifications, two cold runs with mixer-settlers were made on the extraction and stripping of ruthenium and zirconium without the presence of uranium. Efforts in actinide recovery from solids were directed toward the determination of dissolution parameters in various reagents for /sup 241/Am and /sup 239/Pu oxide mixtures, /sup 233/U oxide, /sup 237/Np oxide, /sup 244/Cm oxide, /sup 232/Th oxide, and PuO/sub 2/. Studies in americium-curium recovery with OPIX (oxalate precipitation and ion exchange), Talspeak, and cation exchange chromatography focused on the feasibility of forming oxalate precipitates in continuous systems, the effects of zirconium on Talspeak, and methods for removing solvent degradation products of the Talspeak system. In studies of americium-curium recovery using bidentate extractants, additional distribution coefficients for actinides and other key elements between reduced synthetic LWR waste solution and 30 percent dihexyl-N, N-diethyl-carbamylmethylene phosphonate in diisopropylbenzene were measured. Studies in the americium-curium recovery using inorganic ion exchange media to determine the pH dependence of lanthanide ion affinity for niobate, titanate, and zirconate ion exchange materials have been completed. A modified flowsheet for the extraction of uranium, neptunium, plutonium, americium, and curium from high-level liquid waste is presented. Evaluation of methods for measuring actinides from incinerator ash is continuing. A preliminary evaluation of methods for treatment of salt waste and waste waters was completed. In thermal reactor transmutation studies, waste actinides from an LWR lattice containing mixed uranium-plutonium assemblies were recycled in separate target assemblies. (LK)

  11. Optimization of moderated targets loading in LMFBR for minor actinides incineration

    Energy Technology Data Exchange (ETDEWEB)

    Wu Hongchun; Takeda, Toshikazu [Osaka Univ., Suita (Japan). Dept. of Nuclear Engineering

    1999-04-01

    Optimization of moderated targets loading in LMFBR for minor actinides (MAs) incineration has been performed in this paper. Results of many different composition ratios of moderated target mixture were compared. An optimum case was proposed which can offer good core performance and transmute MAs by about 73 percent (386 kg) and incinerate MAs by about 34 percent (181 kg) through 3 years of reactor operation. (author)

  12. Mono(imidazolin-2-iminato) actinide complexes: synthesis and application in the catalytic dimerization of aldehydes.

    Science.gov (United States)

    Karmel, Isabell S R; Fridman, Natalia; Tamm, Matthias; Eisen, Moris S

    2014-12-10

    The synthesis of the mono(imidazolin-2-iminato) actinide(IV) complexes [(Im(R)N)An(N{SiMe3)2}3] (3-8) was accomplished by the protonolysis reaction between the respective imidazolin-2-imine (Im(R)NH, R = tBu, Mes, Dipp) and the actinide metallacycles [{(Me3Si)N}2An{κ(2)C,N-CH2SiMe2N(SiMe3)}] (1, An = U; 2, M = Th). The thorium and uranium complexes were obtained in high yields, and their structures were established by single-crystal X-ray diffraction analysis. The mono(imidazolin-2-iminato) actinide complexes 3-8 display short An-N bonds together with large An-N-C angles, indicating strong electron donation from the imidazolin-2-iminato moiety to the metal, corroborating a substantial π-character to the An-N bond. The reactivity of complexes 3-8 toward benzaldehyde was studied in the catalytic dimerization of aldehydes (Tishchenko reaction), displaying low to moderate catalytic activities for the uranium complexes 3-5 and moderate to high catalytic activities for the thorium analogues 6-8, among which 8 exhibited the highest catalytic activity. In addition, actinide coordination compounds showed unprecedented reactivity toward cyclic and branched aliphatic aldehydes in the catalytic Tishchenko reaction mediated by the thorium complex [(Im(Dipp)N)Th{N(SiMe3)2}3] (8), exhibiting high activity even at room temperature. Moreover, complex 8 was successfully applied in the crossed Tishchenko reaction between an aromatic or polyaromatic and an aliphatic cyclic and branched aldehyde, yielding selectively the asymmetrically substituted ester in high yields (80-100%).

  13. Soft X-ray scanning transmission X-ray microscopy (STXM) of actinide particles.

    Science.gov (United States)

    Nilsson, Hans J; Tyliszczak, Tolek; Wilson, Richard E; Werme, Lars; Shuh, David K

    2005-09-01

    A descriptive account is given of our most recent research on the actinide dioxides with the Advanced Light Source Molecular Environmental Science (ALS-MES) Beamline 11.0.2 soft X-ray scanning transmission X-ray microscope (STXM) at the Lawrence Berkeley National Laboratory (LBNL). The ALS-MES STXM permits near-edge X-ray absorption fine structure (NEXAFS) and imaging with 30-nm spatial resolution. The first STXM spectromicroscopy NEXAFS spectra at the actinide 4d5/2 edges of the imaged transuranic particles, NpO2 and PuO2, have been obtained. Radiation damage induced by the STXM was observed in the investigation of a mixed oxidation state particle (Np(V,VI)) and was minimized during collection of the actual spectra at the 4d5/2 edge of the Np(V,VI) solid. A plutonium elemental map was obtained from an irregular PuO2 particle with the dimensions of 650 x 650 nm. The Pu 4d5/2 NEXAFS spectra were collected at several different locations from the PuO2 particle and were identical. A representative oxygen K-edge spectrum from UO2 was collected and resembles the oxygen K-edge from the bulk material. The unique and current performance of the ALS-MES STXM at extremely low energies (ca. 100 eV) that may permit the successful measurement of the actinide 5d edge is documented. Finally, the potential of STXM as a tool for actinide investigations is briefly discussed.

  14. Magnesium isotope geochemistry in arc volcanism

    Science.gov (United States)

    Teng, Fang-Zhen; Hu, Yan

    2016-01-01

    Incorporation of subducted slab in arc volcanism plays an important role in producing the geochemical and isotopic variations in arc lavas. The mechanism and process by which the slab materials are incorporated, however, are still uncertain. Here, we report, to our knowledge, the first set of Mg isotopic data for a suite of arc lava samples from Martinique Island in the Lesser Antilles arc, which displays one of the most extreme geochemical and isotopic ranges, although the origin of this variability is still highly debated. We find the δ26Mg of the Martinique Island lavas varies from −0.25 to −0.10, in contrast to the narrow range that characterizes the mantle (−0.25 ± 0.04, 2 SD). These high δ26Mg values suggest the incorporation of isotopically heavy Mg from the subducted slab. The large contrast in MgO content between peridotite, basalt, and sediment makes direct mixing between sediment and peridotite, or assimilation by arc crust sediment, unlikely to be the main mechanism to modify Mg isotopes. Instead, the heavy Mg isotopic signature of the Martinique arc lavas requires that the overall composition of the mantle wedge is buffered and modified by the preferential addition of heavy Mg isotopes from fluids released from the altered subducted slab during fluid−mantle interaction. This, in turn, suggests transfer of a large amount of fluid-mobile elements from the subducting slab to the mantle wedge and makes Mg isotopes an excellent tracer of deep fluid migration. PMID:27303032

  15. DISSOLUTION OF METAL OXIDES AND SEPARATION OF URANIUM FROM LANTHANIDES AND ACTINIDES IN SUPERCRITICAL CARBON DIOXIDE

    Energy Technology Data Exchange (ETDEWEB)

    Donna L. Quach; Bruce J. Mincher; Chien M. Wai

    2013-10-01

    This paper investigates the feasibility of extracting and separating uranium from lanthanides and other actinides by using supercritical fluid carbon dioxide (sc-CO2) as a solvent modified with tri-n-butylphosphate (TBP) for the development of a counter current stripping technique, which would be a more efficient and environmentally benign technology for spent nuclear fuel reprocessing compared to traditional solvent extraction. Several actinides (U, Pu, and Np) and europium were extracted in sc-CO2 modified with TBP over a range of nitric acid concentrations and then the actinides were exposed to reducing and complexing agents to suppress their extractability. According to this study, uranium/europium and uranium/plutonium extraction and separation in sc-CO2 modified with TBP is successful at nitric acid concentrations of less than 6 M and at nitric acid concentrations of less than 3 M with acetohydroxamic acid or oxalic acid, respectively. A scheme for recycling uranium from spent nuclear fuel by using sc-CO2 and counter current stripping columns is presented.

  16. JOWOG 22/2 - Actinide Chemical Technology (July 9-13, 2012)

    Energy Technology Data Exchange (ETDEWEB)

    Jackson, Jay M. [Los Alamos National Laboratory; Lopez, Jacquelyn C. [Los Alamos National Laboratory; Wayne, David M. [Los Alamos National Laboratory; Schulte, Louis D. [Los Alamos National Laboratory; Finstad, Casey C. [Los Alamos National Laboratory; Stroud, Mary Ann [Los Alamos National Laboratory; Mulford, Roberta Nancy [Los Alamos National Laboratory; MacDonald, John M. [Los Alamos National Laboratory; Turner, Cameron J. [Los Alamos National Laboratory; Lee, Sonya M. [Los Alamos National Laboratory

    2012-07-05

    The Plutonium Science and Manufacturing Directorate provides world-class, safe, secure, and reliable special nuclear material research, process development, technology demonstration, and manufacturing capabilities that support the nation's defense, energy, and environmental needs. We safely and efficiently process plutonium, uranium, and other actinide materials to meet national program requirements, while expanding the scientific and engineering basis of nuclear weapons-based manufacturing, and while producing the next generation of nuclear engineers and scientists. Actinide Process Chemistry (NCO-2) safely and efficiently processes plutonium and other actinide compounds to meet the nation's nuclear defense program needs. All of our processing activities are done in a world class and highly regulated nuclear facility. NCO-2's plutonium processing activities consist of direct oxide reduction, metal chlorination, americium extraction, and electrorefining. In addition, NCO-2 uses hydrochloric and nitric acid dissolutions for both plutonium processing and reduction of hazardous components in the waste streams. Finally, NCO-2 is a key team member in the processing of plutonium oxide from disassembled pits and the subsequent stabilization of plutonium oxide for safe and stable long-term storage.

  17. Lanthanide and actinide chemistry at high C/O ratios in the solar nebula

    Science.gov (United States)

    Lodders, Katharina; Fegley, Bruce, Jr.

    1993-01-01

    Chemical equilibrium calculations were performed to study the condensation chemistry of the REE and actinides under the highly reducing conditions which are necessary for the formation of the enstatite chondrites. Our calculations confirm that the REE and actinides condensed into oldhamite (CaS), the major REE and actinide host phase in enstatite chondrites, at a carbon-oxygen (C/O) ratio not less than 1 in an otherwise solar gas. Five basic types of REE abundance patterns, several of which are analogous to REE abundance patterns observed in the Ca, Al-rich inclusions in carbonaceous chondrites, are predicted to occur in meteoritic oldhamites. All of the reported REE patterns in oldhamites in enstatite chondrites can be interpreted in terms of our condensation calculations. The observed patterns fall into three of the five predicted categories. The reported Th and U enrichments and ratios in meteoritic oldhamites are also consistent with predictions of the condensation calculations. Pure REE sulfides are predicted to condense in the 10 exp -6 to 10 exp -9 bar range and may be found in enstatite chondrites if they formed in this pressure range.

  18. Fundamental thermodynamics of actinide-bearing mineral waste forms. 1998 annual progress report

    Energy Technology Data Exchange (ETDEWEB)

    Williamson, M.A. [Los Alamos National Lab., NM (US); Ebbinghaus, B.B.

    1998-06-01

    'The end of the Cold War raised the need for the technical community to be concerned with the disposition of excess nuclear weapon material. The plutonium will either be converted into mixed-oxide fuel for use in nuclear reactors or immobilized in glass or ceramic waste forms and placed in a repository. The stability and behavior of plutonium in the ceramic materials as well as the phase behavior and stability of the ceramic material in the environment is not well established. In order to provide technically sound solutions to these issues, thermodynamic data are essential in developing an understanding of the chemistry and phase equilibria of the actinide-bearing mineral waste form materials proposed as immobilization matrices. Mineral materials of interest include zircon, zirconolite, and pyrochlore. High temperature solution calorimetry is one of the most powerful techniques, sometimes the only technique, for providing the fundamental thermodynamic data needed to establish optimum material fabrication parameters, and more importantly, understand and predict the behavior of the mineral materials in the environment. The purpose of this project is to experimentally determine the enthalpy of formation of actinide orthosilicates, the enthalpy of formation of actinide substituted zircon, zirconolite and pyrochlore, and develop an understanding of the bonding characteristics and stability of these materials. This report summarizes work after eight months of a three year project.'

  19. Extraction studies of actinides and lanthanides by bifunctional H-phosphonates

    Energy Technology Data Exchange (ETDEWEB)

    Brahmmananda Rao, C.V.S.; Jayalakshmi, S.; Subramaniam, S.; Sivaraman, N.; Vasudeva Rao, P.R. [Indira Gandhi Centre for Atomic Research, Kalpakkam (India). Fuel Chemistry Div.

    2015-07-01

    The extraction behavior of actinides and lanthanides was investigated by three homologues of H-phosphonates viz. diamylhydrogen phosphonate (DAHP), dihexylhydrogen phosphonate (DHeHP) and dioctylhydrogen phosphonate (DOHP). These compounds were synthesized, characterized by using elemental analysis, IR, NMR ({sup 1}H, {sup 13}C and {sup 31}P) and mass spectroscopy. The extraction behavior of these ligands was compared with a member of dialkylalkyl phosphonate viz. diamylamyl phosphonate (DAAP). The present study has been taken up to understand the influence of phosphorus bonded hydrogen and alkyl groups in H-phosphonates on the extraction behavior of actinides and lanthanides. The important physicochemical properties such as density, viscosity, phase disengagement time, dispersion number and solubility are also reported for the first time. These compounds extract actinides through the P-OH group which is present in tautomeric equilibrium with the P-H bond at lower acidities, and through the phosphoryl group at higher acidities thus exhibiting a dual behaviour. The physical properties can be modified by suitably designing the extractant based on the requirement for a given purpose. The H-phosphonates have potential applications in pre-concentration of large quantities of dilute solutions of uranium and plutonium.

  20. An Ion Exchange Study of Possible Hydridized 5f Bonding in theActinides

    Energy Technology Data Exchange (ETDEWEB)

    Diamond, R.M.; Street, Jr., K.; Seaborg, G.T.

    1951-08-28

    A study has been made of the elution behavior of curium(III), americium(III), plutonium(III), actinium(III), plutonium(IV), neptunium(IV), uraniuM(IV), thorium(IV), neptunium(V), plutonium (VI), uranium (VI), lanthanum(III), cerium(III), europium(III), ytterbium(III), ytterium(III), strontium(II), barium(II), radium(II), cesium(I) with 3.2 M, 6.2 M, 9.3 M, and 12.2 M HCl solutions from Dowex-50 cation exchange resin columns. These elutions show that in high concentrations of hydrochloric acid the actinides form complex ions with chloride ion to a much greater extent than the lanthanides. The strengths of the tripositive actinide complex ions apparently go in the order plutonium > americium> curium, although their ionic radii also decrease in this same order. To explain these results, a partial covalent character may be ascribed to the bonding in the transuranium complex ions. It is shown that a reasonable structure for such covalent bonding involves hybridization of the 5f orbitals in the actinide elements.

  1. Study on separation of minor actinides from HLLW with new extractant of TODGA-DHOA/Kerosene

    Energy Technology Data Exchange (ETDEWEB)

    Ye, Guo-an; Zhu, Wen-bin; Li, Feng-feng; Lin, Ru-shan; Li, Hui-rong [China Institute of Atomic Energy, P.O.Box 275-26, Beijing 102413 (China)

    2013-07-01

    The extraction behavior of U, Np, Pu, Am, rare earth elements and Sr from nitric acid solutions by TODGA/dodecan, DHOA/dodecane and TODGA-DHOA/dodecane were investigated, respectively. Based on experimental results, a separation process was proposed for minor actinide isolation from high level liquid waste (HLLW): the TODGA-DHOA/kerosene system. The multi-stage counter-current cascade experiments were carried out for the purpose by 0.1 mol/l TODGA-1.0 mol/l DHOA/kerosene with miniature mixer- settler contactor rigs (8 stages for extraction, 6 stages for scrubbing, 8 stages for first stripping, 8 stages for second stripping). The results show that the recovery efficiencies of the actinides and lanthanides are more than 99.9%, whereas less than 1% Sr was extracted by 0.1 mol/l TODGA - 1.0 mol/l DHOA/kerosene. The stripping efficiencies of U, Np and Pu are more than 95% in the first stripping step by 0.5 mol/l HNO{sub 3} + 0.5 mol/l AHA(aceto-hydroxamic acid), all of the remained actinides and lanthanides can be stripped by 0.01 mol/l HNO{sub 3} in the second stripping step. 99% Sr was extracted by 0.1 mol/l TODGA/kerosene, so Sr can be recovered efficiently directly from the raffinate by 0.1 mol/l TODGA/kerosene. (authors)

  2. Hydroxypyri(mi)dine-based chelators as antidotes of toxicity due to aluminum and actinides.

    Science.gov (United States)

    Santos, M A; Esteves, M A; Chaves, S

    2012-01-01

    This review is focused on recent developments on hydroxypyri(mi)dines, as aluminum and actinide chelating agents to combat the toxicity due to accumulations of these metal ions in human body resulting from excessive metal exposure. After a brief update revision of the most common processes of aluminum (Al) exposure, as well as the associated toxicities and pathologies, we will focus on the current available Al chelators and future perspective as potential antidotes of Al toxicity. Due to the similarity between Al and Fe, a major emphasis is given to the hydroxypyridinone and hydroxypyrimidinone chelators, since they are analogues of the current iron chelators in clinical use (DFP and DFO). This review includes issues such as molecular design strategies and corresponding effects on the associated physico-chemical properties, lipo-hydrophilic balance, toxicity, in vivo bioassays and current clinical applications. The hydroxypyri(mi)dine chelators are also suitable for other hard metal ions, such as the radiotoxic actinides, and so a brief review is included on the applications of these chelators in actinides scavenging.

  3. Fundamental Thermodynamics of Actinide-Bearing Mineral Waste Forms - Final Report

    Energy Technology Data Exchange (ETDEWEB)

    Williamson, Mark A.; Ebbinghaus, Bartley B.; Navrotsky, Alexandra

    2001-03-01

    The end of the Cold War raised the need for the technical community to be concerned with the disposition of excess nuclear weapon material. The plutonium will either be converted into mixed-oxide fuel for use in nuclear reactors or immobilized in glass or ceramic waste forms and placed in a repository. The stability and behavior of plutonium in the ceramic materials as well as the phase behavior and stability of the ceramic material in the environment is not well established. In order to provide technically sound solutions to these issues, thermodynamic data are essential in developing an understanding of the chemistry and phase equilibria of the actinide-bearing mineral waste form materials proposed as immobilization matrices. Mineral materials of interest include zircon, zirconolite, and pyrochlore. High temperature solution calorimetry is one of the most powerful techniques, sometimes the only technique, for providing the fundamental thermodynamic data needed to establish optimum material fabrication parameters, and more importantly understand and predict the behavior of the mineral materials in the environment. The purpose of this project is to experimentally determine the enthalpy of formation of actinide orthosilicates, the enthalpies of formation of actinide substituted zirconolite and pyrochlore, and develop an understanding of the bonding characteristics and stabilities of these materials.

  4. Conjugates of Magnetic Nanoparticle -- Actinide Specific Chelator for Radioactive Waste Separation

    Energy Technology Data Exchange (ETDEWEB)

    Maninder Kaur; Huijin Zhang; Leigh Martin; Terry Todd; You Qiang

    2013-11-01

    A novel nanotechnology for the separation of radioactive waste that uses magnetic nanoparticles (MNPs) conjugated with actinide specific chelators (MNP-Che) is reviewed with a focus on design and process development. The MNP-Che separation process is an effective way of separating heat generating minor actinides (Np, Am, Cm) from spent nuclear fuel solution to reduce the radiological hazard. It utilizes coated MNPs to selectively adsorb the contaminants onto their surfaces, after which the loaded particles are collected using a magnetic field. The MNP-Che conjugates can be recycled by stripping contaminates into a separate, smaller volume of solution, and then become the final waste form for disposal after reusing number of times. Due to the highly selective chelators, this remediation method could be both simple and versatile while allowing the valuable actinides to be recovered and recycled. Key issues standing in the way of large-scale application are stability of the conjugates and their dispersion in solution to maintain their unique properties, especially large surface area, of MNPs. With substantial research progress made on MNPs and their surface functionalization, as well as development of environmentally benign chelators, this method could become very flexible and cost-effective for recycling used fuel. Finally, the development of this nanotechnology is summarized and its future direction is discussed.

  5. Isotopic modeling of the sub-cloud evaporation effect in precipitation

    Energy Technology Data Exchange (ETDEWEB)

    Salamalikis, V., E-mail: vsalamalik@upatras.gr [Laboratory of Atmospheric Physics, Department of Physics, University of Patras, GR 26500 Patras (Greece); Argiriou, A.A. [Laboratory of Atmospheric Physics, Department of Physics, University of Patras, GR 26500 Patras (Greece); Dotsika, E. [Stable Isotope Unit, Institute of Nanoscience and Nanotechnology, National Center of Scientific Research ‘Demokritos’, Ag. Paraskevi Attikis, 15310 Athens (Greece)

    2016-02-15

    In dry and warm environments sub-cloud evaporation influences the falling raindrops modifying their final stable isotopic content. During their descent from the cloud base towards the ground surface, through the unsaturated atmosphere, hydrometeors are subjected to evaporation whereas the kinetic fractionation results to less depleted or enriched isotopic signatures compared to the initial isotopic composition of the raindrops at cloud base. Nowadays the development of Generalized Climate Models (GCMs) that include isotopic content calculation modules are of great interest for the isotopic tracing of the global hydrological cycle. Therefore the accurate description of the underlying processes affecting stable isotopic content can improve the performance of iso-GCMs. The aim of this study is to model the sub-cloud evaporation effect using a) mixing and b) numerical isotope evaporation models. The isotope-mixing evaporation model simulates the isotopic enrichment (difference between the ground and the cloud base isotopic composition of raindrops) in terms of raindrop size, ambient temperature and relative humidity (RH) at ground level. The isotopic enrichment (Δδ) varies linearly with the evaporated raindrops mass fraction of the raindrop resulting to higher values at drier atmospheres and for smaller raindrops. The relationship between Δδ and RH is described by a ‘heat capacity’ model providing high correlation coefficients for both isotopes (R{sup 2} > 80%) indicating that RH is an ideal indicator of the sub-cloud evaporation effect. Vertical distribution of stable isotopes in falling raindrops is also investigated using a numerical isotope-evaporation model. Temperature and humidity dependence of the vertical isotopic variation is clearly described by the numerical isotopic model showing an increase in the isotopic values with increasing temperature and decreasing RH. At an almost saturated atmosphere (RH = 95%) sub-cloud evaporation is negligible and the

  6. Partnew - New solvent extraction processes for minor actinides - final report; Partnew - Nouveaux procedes d'extraction par solvant pour les actinides mineurs - rapport final

    Energy Technology Data Exchange (ETDEWEB)

    Madic, C.; Testard, F.; Hudson, M.J.; Liljenzin, J.O.; Christiansen, B.; Ferrando, M.; Facchini, A.; Geist, A.; Modolo, G.; Gonzalez-Espartero, A.; Mendoza, J. de

    2004-07-01

    The objectives of the European project PARTNEW were to define solvent extraction processes for the partitioning of the minor actinides, Am and Cm, from the aqueous high active raffinate or high active concentrate issuing the reprocessing of nuclear spent fuels by the PUREX process. Eleven laboratories participated to the research: 1/ CEA-DEN (Marcoule), 2/ CEA-DSM (Saclay), 3/ UREAD (U.K.), 4/ CTU (Sweden), 5/ ITU (Germany), 6/ ENEA (Italy), 7/ PoliMi (Italy), 8/ FZK-INE (Germany), 9/ FZJ-ISR (Germany), 10/ CIEMAT (Spain) and 11/ UAM (Spain). The research was organised into eight work packages (WP): Basic and applied DIAMEX studies, using diamide extractants for the co-extraction of actinides(III) (An(III)) and lanthanides(III) (Ln(III)) nitrates (WP1 and WP2), Basic and applied SANEX studies based on the use of polydentate N-ligands for the An(III)/Ln(III) separation (WP3 and WP4), Basic and applied SANEX studies based on the use of synergistic mixtures made of bis-(chloro-phenyl)-di-thio-phosphinic acid + neutral O-bearing ligand, (WP5 and WP6), Basic SANEX studies for the An(III)/Ln(III) separation, based on the use of new S-bearing ligands, Basic and applied studies for the Am(III)/Cm(III) separation. The work done in the fundamental and applied domains was very fruitful. Several processes have been successfully tested with genuine high active raffinates and concentrate. (authors)

  7. Actinides(3)/lanthanides(3) separation by nano-filtration assisted by complexation; Separation actinides(3)lanthanides(3) par nanofiltration assistee par complexation

    Energy Technology Data Exchange (ETDEWEB)

    Sorin, A

    2006-07-01

    In France, one of the research trend concerning the reprocessing of spent nuclear fuel consists to separate selectively the very radio-toxic elements with a long life to be recycled (Pu) or transmuted (Am, Cm, Np). The aim of this thesis concerns the last theme about actinides(III)/lanthanides(III) separation by a process of nano-filtration assisted by complexation. Thus, a pilot of tangential membrane filtration was designed and established in a glove box at the ATALANTE place of CEA-Marcoule. Physico-chemical characterisation of the Desal GH membrane (OSMONICS), selected to carry out actinides(III)/lanthanides(III) separation, was realized to determine the zeta potential of the active layer and its resistance to ionizing radiations. Moreover, a parametric study was also carried out to optimize the selectivity of complexation, and the operating conditions of complex retention (influences of the transmembrane pressure, solute concentration, tangential velocity and temperature). Finally, the separation of traces of Am(III) contained in a mixture of lanthanides(III), simulating the real load coming from a reprocessing cycle, was evaluated with several chelating agents such as poly-amino-carboxylic acids according to the solution acidity and the [Ligand]/[Cation(III)] ratio. (author)

  8. Selective Gaseous Extraction: Research, Development and Training for Isotope Production, Final Technical Report

    Energy Technology Data Exchange (ETDEWEB)

    Bertch, Timothy C, [General Atomics

    2014-03-31

    General Atomics and the University of Missouri Research Reactor (MURR) completed research and development of selective gaseous extraction of fission products from irradiated fuel, which included training and education of MURR students. The process used porous fuel and after irradiation flowed product gases through the fuel to selectively removed desired fission products with the primary goal of demonstrating the removal of rhodium 105. High removal rates for the ruthenium/rhodium (Ru/Rh), tellurium/iodine (Te/I) and molybdenum/technetium (Mo/Tc) series were demonstrated. The success of this research provides for the reuse of the target for further production, significantly reducing the production of actinide wastes relative to processes that dissolve the target. This effort was conducted under DOE funding (DE-SC0007772). General Atomics objective of the project was to conduct R&D on alternative methods to produce a number of radioactive isotopes currently needed for medical and industry applications to include rhodium-105 and other useful isotopes. Selective gaseous extraction was shown to be effective at removing radioisotopes of the ruthenium/rhodium, tellurium/iodine and molybdenum/technetium decay chains while having trace to no quantities of other fission products or actinides. This adds a new, credible method to the area of certain commercial isotope production beyond current techniques, while providing significant potential reduction of process wastes. Waste reduction, along with reduced processing time/cost provides for superior economic feasibility which may allow domestic production under full cost recovery practices. This provides the potential for improved access to domestically produced isotopes for medical diagnostics and treatment at reduced cost, providing for the public good.

  9. Design of an Actinide-Burning, Lead or Lead-Bismuth Cooled Reactor that Produces Low-Cost Electricity

    Energy Technology Data Exchange (ETDEWEB)

    Mac Donald, Philip Elsworth; Weaver, Kevan Dean; Davis, Cliff Bybee; MIT folks

    2000-07-01

    The purpose of this Idaho National Engineering and Environmental Laboratory (INEEL) and Massachusetts Institute of Technology (MIT) University Research Consortium (URC) project is to investigate the suitability of lead or lead-bismuth cooled fast reactors for producing low-cost electricity as well as for actinide burning. The goal is to identify and analyze the key technical issues in core neutronics, materials, thermal-hydraulics, fuels, and economics associated with the development of this reactor concept. Work has been accomplished in four major areas of research: core neutronic design, material compatibility, plant engineering, and coolant activation. In the area of core neutronic design, the reactivity vs. burnup and discharge isotopics of both non-fertile and fertile fuels were evaluated. An innovative core for pure actinide burning that uses streaming, fertile-free fuel assemblies was studied in depth. This particular core exhibits excellent reactivity performance upon coolant voiding, even for voids that occur in the core center, and has a transuranic (TRU) destruction rate that is comparable to the proposed accelerator transmutation of waste (ATW) facility. These studies suggest that a core can be designed to achieve a long life while maintaining safety and minimizing waste. In the area of material compatibility studies, an experimental apparatus for the investigation of the flow-assisted dissolution and precipitation (corrosion) of potential fuel cladding and structural materials has been designed and built at the INEEL. The INEEL forced-convection corrosion cell consists of a small heated vessel with a shroud and gas flow system. The corrosion cell is being used to test steel that is commercially available in the United States to temperatures above 650°C. Progress in plant engineering was made for two reactor concepts, one utilizing an indirect cycle with heat exchangers and the other utilizing a direct-contact steam cycle. The evaluation of the

  10. Discovery of the Cobalt Isotopes

    OpenAIRE

    Szymanski, T.; Thoennessen, M.

    2009-01-01

    Twenty-six cobalt isotopes have so far been observed; the discovery of these isotopes is discussed. For each isotope a brief summary of the first refereed publication, including the production and identification method, is presented.

  11. Discovery of the Arsenic Isotopes

    CERN Document Server

    Shore, A; Heim, M; Schuh, A; Thoennessen, M

    2009-01-01

    Twenty-nine arsenic isotopes have so far been observed; the discovery of these isotopes is discussed. For each isotope a brief summary of the first refereed publication, including the production and identification method, is presented.

  12. Intracellular Cadmium Isotope Fractionation

    Science.gov (United States)

    Horner, T. J.; Lee, R. B.; Henderson, G. M.; Rickaby, R. E.

    2011-12-01

    Recent stable isotope studies into the biological utilization of transition metals (e.g. Cu, Fe, Zn, Cd) suggest several stepwise cellular processes can fractionate isotopes in both culture and nature. However, the determination of fractionation factors is often unsatisfactory, as significant variability can exist - even between different organisms with the same cellular functions. Thus, it has not been possible to adequately understand the source and mechanisms of metal isotopic fractionation. In order to address this problem, we investigated the biological fractionation of Cd isotopes within genetically-modified bacteria (E. coli). There is currently only one known biological use or requirement of Cd, a Cd/Zn carbonic anhydrase (CdCA, from the marine diatom T. weissfloggii), which we introduce into the E. coli genome. We have also developed a cleaning procedure that allows for the treating of bacteria so as to study the isotopic composition of different cellular components. We find that whole cells always exhibit a preference for uptake of the lighter isotopes of Cd. Notably, whole cells appear to have a similar Cd isotopic composition regardless of the expression of CdCA within the E. coli. However, isotopic fractionation can occur within the genetically modified E. coli during Cd use, such that Cd bound in CdCA can display a distinct isotopic composition compared to the cell as a whole. Thus, the externally observed fractionation is independent of the internal uses of Cd, with the largest Cd isotope fractionation occurring during cross-membrane transport. A general implication of these experiments is that trace metal isotopic fractionation most likely reflects metal transport into biological cells (either actively or passively), rather than relating to expression of specific physiological function and genetic expression of different metalloenzymes.

  13. Hitting the moving target: modelling ontogenetic shifts with stable isotopes reveals the importance of isotopic turnover.

    Science.gov (United States)

    Hertz, Eric; Trudel, Marc; El-Sabaawi, Rana; Tucker, Strahan; Dower, John F; Beacham, Terry D; Edwards, Andrew M; Mazumder, Asit

    2016-05-01

    Ontogenetic niche shifts are widely prevalent in nature and are important in shaping the structure and dynamics of ecosystems. Stable isotope analysis is a powerful tool to assess these shifts, with δ(15) N providing a measure of trophic level and δ(13) C a measure of energy source. Previous applications of stable isotopes to study ontogenetic niche shifts have not considered the appreciable time lag between diet and consumer tissue associated with isotopic turnover. These time lags introduce significant complexity into field studies of ontogenetic niche shifts. Juvenile Chinook salmon (Oncorhynchus tshawytscha) migrate from freshwater to marine ecosystems and shift their diet from feeding primarily on invertebrates to feeding primarily on fish. This dual ontogenetic habitat and diet shift, in addition to the long time lag associated with isotopic turnover, suggests that there is potential for a disconnect between the prey sources that juvenile salmon are consuming, and the inferred prey sources from stable isotopes. We developed a model that considered ontogenetic niche shifts and time lags associated with isotopic turnover, and compared this 'ontogeny' model to one that considered only isotopic turnover. We used a Bayesian framework to explicitly account for parameter uncertainty. Data showed overwhelming support for the ontogeny model relative to the isotopic turnover model. Estimated variables from best model fits indicate that the ontogeny model predicts a much greater reliance on fish prey than does the stomach content data. Overall, we found that this method of quantifying ontogenetic niche shifts effectively accounted for both isotopic turnover and ontogenetic diet shifts; a finding that could be widely applicable to a variety of systems.

  14. Characterization of partitioning relevant lanthanide and actinide complexes by NMR spectroscopy; Charakterisierung von partitioningrelevanten Lanthaniden- und Actinidenkomplexen mittels NMR-Spektroskopie

    Energy Technology Data Exchange (ETDEWEB)

    Adam, Christian

    2016-01-15

    In the present work the interaction of N-donor ligands, such as 2,6-Bis(5,6-dipropyl-1,2,4-triazin-3-yl)pyridine (nPrBTP) and 2,6-Bis(5-(2,2-dimethylpropyl)1H-pyrazol)-3-yl-pyridine (C5-BPP), with trivalent lanthanide and actinide ions was studied. Ligands of this type show a high selectivity for the separation of trivalent actinide ions over lanthanides from nitric acid solutions. However, the reason for this selectivity, which is crucial for future partitioning and transmutation strategies for radioactive wastes, is still unknown. So far, the selectivity of some N-donor ligands is supposed to be an effect of an increased covalency in the actinide-ligand bond, compared to the lanthanide compounds. NMR spectroscopy on paramagnetic metal complexes is an excellent tool for the elucidation of bonding modes. The overall paramagnetic chemical shift consists of two contributions, the Fermi Contact Shift (FCS), due to electron spin delocalisation through covalent bonds, and the Pseudo Contact Shift (PCS), which describes the dipolar coupling of the electron magnetic moment and the nuclear spin. By assessing the FCS share in the paramagnetic shift, the degree of covalency in the metal-ligand bond can be gauged. Several methods to discriminate FCS and PCS have been used on the data of the nPrBTP- and C5-BPP-complexes and were evaluated regarding their applicability on lanthanide and actinide complexes with N-donor ligands. The study comprised the synthesis of all Ln(III) complexes with the exceptions of Pm(III) and Gd(III) as well as the Am(III) complex as a representative of the actinide series with both ligands. All complexes were fully characterised ({sup 1}H, {sup 13}C and {sup 15}N spectra) using NMR spectroscopy. By isotope enrichment with the NMR-active {sup 15}N in positions 8 and 9 in both ligands, resonance signals of these nitrogen atoms were detected for all complexes. The Bleaneymethod relies on different temperature dependencies for FCS (T{sup -1}) and PCS (T

  15. Accurate determination of Curium and Californium isotopic ratios by inductively coupled plasma quadrupole mass spectrometry (ICP-QMS) in 248Cm samples for transmutation studies

    Energy Technology Data Exchange (ETDEWEB)

    Gourgiotis, A.; Isnard, H.; Aubert, M.; Dupont, E.; AlMahamid, I.; Cassette, P.; Panebianco, S.; Letourneau, A.; Chartier, F.; Tian, G.; Rao, L.; Lukens, W.

    2011-02-01

    The French Atomic Energy Commission has carried out several experiments including the mini-INCA (INcineration of Actinides) project for the study of minor-actinide transmutation processes in high intensity thermal neutron fluxes, in view of proposing solutions to reduce the radiotoxicity of long-lived nuclear wastes. In this context, a Cm sample enriched in {sup 248}Cm ({approx}97 %) was irradiated in thermal neutron flux at the High Flux Reactor (HFR) of the Laue-Langevin Institute (ILL). This work describes a quadrupole ICP-MS (ICP-QMS) analytical procedure for precise and accurate isotopic composition determination of Cm before sample irradiation and of Cm and Cf after sample irradiation. The factors that affect the accuracy and reproducibility of isotopic ratio measurements by ICP-QMS, such as peak centre correction, detector dead time, mass bias, abundance sensitivity and hydrides formation, instrumental background, and memory blank were carefully evaluated and corrected. Uncertainties of the isotopic ratios, taking into account internal precision of isotope ratio measurements, peak tailing, and hydrides formations ranged from 0.3% to 1.3%. This uncertainties range is quite acceptable for the nuclear data to be used in transmutation studies.

  16. Determination of Atto- to Femtogram Levels of Americium and Curium Isotopes in Large-Volume Urine Samples by Compact Accelerator Mass Spectrometry.

    Science.gov (United States)

    Dai, Xiongxin; Christl, Marcus; Kramer-Tremblay, Sheila; Synal, Hans-Arno

    2016-03-01

    Ultralow level analysis of actinides in urine samples may be required for dose assessment in the event of internal exposures to these radionuclides at nuclear facilities and nuclear power plants. A new bioassay method for analysis of sub-femtogram levels of Am and Cm in large-volume urine samples was developed. Americium and curium were co-precipitated with hydrous titanium oxide from the urine matrix and purified by column chromatography separation. After target preparation using mixed titanium/iron oxides, the final sample was measured by compact accelerator mass spectrometry. Urine samples spiked with known quantities of Am and Cm isotopes in the range of attogram to femtogram levels were measured for method evaluation. The results are in good agreement with the expected values, demonstrating the feasibility of compact accelerator mass spectrometry (AMS) for the determination of minor actinides at the levels of attogram/liter in urine samples to meet stringent sensitivity requirements for internal dosimetry assessment.

  17. Chromium isotope variations

    DEFF Research Database (Denmark)

    D'Arcy, Joan Mary

    is incorporated into carbonates. Hence, ancient carbonates can potentially record the Cr isotopic composition (δ53Cr ‰) of seawater in the geological past. Reliable application and interpretation of this proxy requires a detailed knowledge about processes that fractionate Cr on the Earth’s surface...... deposited during the Early Ordovician — a time of known redox instability in ancient oceans – exhibit a significant positive Cr isotope excursion of +0.5‰. This excursion is interpreted as the reductive drawn down of dissolved Cr in seawater in response to the development of a proximal anoxic sink......, and the quantification the Cr isotope composition of major Cr fluxes into and out of ocean. This thesis adds to the current knowledge of the Cr isotope system and is divided into two studies. The focus of the first study was to determine what processes control the Cr isotopic compositionof river water and to quantify...

  18. Isotopic composition and neutronics of the Okelobondo natural reactor

    Science.gov (United States)

    Palenik, Christopher Samuel

    The Oklo-Okelobondo and Bangombe uranium deposits, in Gabon, Africa host Earth's only known natural nuclear fission reactors. These 2 billion year old reactors represent a unique opportunity to study used nuclear fuel over geologic periods of time. The reactors in these deposits have been studied as a means by which to constrain the source term of fission product concentrations produced during reactor operation. The source term depends on the neutronic parameters, which include reactor operation duration, neutron flux and the neutron energy spectrum. Reactor operation has been modeled using a point-source computer simulation (Oak Ridge Isotope Generation and Depletion, ORIGEN, code) for a light water reactor. Model results have been constrained using secondary ionization mass spectroscopy (SIMS) isotopic measurements of the fission products Nd and Te, as well as U in uraninite from samples collected in the Okelobondo reactor zone. Based upon the constraints on the operating conditions, the pre-reactor concentrations of Nd (150 ppm +/- 75 ppm) and Te (<1 ppm) in uraninite were estimated. Related to the burnup measured in Okelobondo samples (0.7 to 13.8 GWd/MTU), the final fission product inventories of Nd (90 to 1200 ppm) and Te (10 to 110 ppm) were calculated. By the same means, the ranges of all other fission products and actinides produced during reactor operation were calculated as a function of burnup. These results provide a source term against which the present elemental and decay abundances at the fission reactor can be compared. Furthermore, they provide new insights into the extent to which a "fossil" nuclear reactor can be characterized on the basis of its isotopic signatures. In addition, results from the study of two other natural systems related to the radionuclide and fission product transport are included. A detailed mineralogical characterization of the uranyl mineralogy at the Bangombe uranium deposit in Gabon, Africa was completed to improve

  19. Utilization of Minor Actinides as a Fuel Component for Ultra-Long Life Bhr Configurations: Designs, Advantages and Limitations

    Energy Technology Data Exchange (ETDEWEB)

    Dr. Pavel V. Tsvetkov

    2009-05-20

    This project assessed the advantages and limitations of using minor actinides as a fuel component to achieve ultra-long life Very High Temperature Reactor (VHTR) configurations. Researchers considered and compared the capabilities of pebble-bed and prismatic core designs with advanced actinide fuels to achieve ultra-long operation without refueling. Since both core designs permit flexibility in component configuration, fuel utilization, and fuel management, it is possible to improve fissile properties of minor actinides by neutron spectrum shifting through configuration adjustments. The project studied advanced actinide fuels, which could reduce the long-term radio-toxicity and heat load of high-level waste sent to a geologic repository and enable recovery of the energy contained in spent fuel. The ultra-long core life autonomous approach may reduce the technical need for additional repositories and is capable to improve marketability of the Generation IV VHTR by allowing worldwide deployment, including remote regions and regions with limited industrial resources. Utilization of minor actinides in nuclear reactors facilitates developments of new fuel cycles towards sustainable nuclear energy scenarios.

  20. Particular features of ternary fission induced by polarized neutrons in the major actinides U,235233 and Pu,241239

    Science.gov (United States)

    Gagarski, A.; Gönnenwein, F.; Guseva, I.; Jesinger, P.; Kopatch, Yu.; Kuzmina, T.; Lelièvre-Berna, E.; Mutterer, M.; Nesvizhevsky, V.; Petrov, G.; Soldner, T.; Tiourine, G.; Trzaska, W. H.; Zavarukhina, T.

    2016-05-01

    Ternary fission in (n ,f ) reactions was studied with polarized neutrons for the isotopes U,235233 and Pu,241239. A cold longitudinally polarized neutron beam was available at the High Flux Reactor of the Institut Laue-Langevin in Grenoble, France. The beam was hitting the fissile targets mounted at the center of a reaction chamber. Detectors for fission fragments and ternary particles were installed in a plane perpendicular to the beam. In earlier work it was discovered that the angular correlations between neutron spin and the momenta of fragments and ternary particles were very different for 233U or 235U. These correlations could now be shown to be simultaneously present in all of the above major actinides though with different weights. For one of the correlations it was observed that up to scission the compound nucleus is rotating with the axis of rotation parallel to the neutron beam polarization. Entrained by the fragments also the trajectories of ternary particles are turned away albeit by a smaller angle. The difference in turning angles becomes observable upon reversing the sense of rotation by flipping neutron spin. All turning angles are smaller than 1∘. The phenomenon was called the ROT effect. As a distinct second phenomenon it was found that for fission induced by polarized neutrons an asymmetry in the emission probability of ternary particles relative to a plane formed by fragment momentum and neutron spin appears. The asymmetry is attributed to the Coriolis force present in the nucleus while it is rotating up to scission. The size of the asymmetry is typically 10-3. This asymmetry was termed the TRI effect. The interpretation of both effects is based on the transition state model. Both effects are shown to be steered by the properties of the collective (J ,K ) transition states which are specific for any of the reactions studied. The study of asymmetries of ternary particle emission in fission induced by slow polarized neutrons provides a new

  1. Actinide Sorption in Rainier Mesa Tunnel Waters from the Nevada Test Site

    Energy Technology Data Exchange (ETDEWEB)

    Zhao, P; Zavarin, M; Leif, R; Powell, B; Singleton, M; Lindvall, R; Kersting, A

    2007-12-17

    The sorption behavior of americium (Am), plutonium (Pu), neptunium (Np), and uranium (U) in perched Rainier Mesa tunnel water was investigated. Both volcanic zeolitized tuff samples and groundwater samples were collected from Rainier Mesa, Nevada Test Site, NV for a series of batch sorption experiments. Sorption in groundwater with and without the presence of dissolved organic matter (DOM) was investigated. Am(III) and Pu(IV) are more soluble in groundwater that has high concentrations of DOM. The sorption K{sub d} for Am(III) and Pu(IV) on volcanic zeolitized tuff was up to two orders of magnitude lower in samples with high DOM (15 to 19 mg C/L) compared to samples with DOM removed (< 0.4 mg C/L) or samples with naturally low DOM (0.2 mg C/L). In contrast, Np(V) and U(VI) sorption to zeolitized tuff was much less affected by the presence of DOM. The Np(V) and U(VI) sorption Kds were low under all conditions. Importantly, the DOM was not found to significantly sorb to the zeolitized tuff during these experiment. The concentration of DOM in groundwater affects the transport behavior of actinides in the subsurface. The mobility of Am(III) and Pu(IV) is significantly higher in groundwater with elevated levels of DOM resulting in potentially enhanced transport. To accurately model the transport behavior of actinides in groundwater at Rainier Mesa, the low actinide Kd values measured in groundwater with high DOM concentrations must be incorporated in predictive transport models.

  2. Actinide(IV) Deposits on Bone: Potential Role of the Osteopontin-Thorium Complex.

    Science.gov (United States)

    Creff, Gaëlle; Safi, Samir; Roques, Jérôme; Michel, Hervé; Jeanson, Aurélie; Solari, Pier-Lorenzo; Basset, Christian; Simoni, Eric; Vidaud, Claude; Den Auwer, Christophe

    2016-01-04

    In case of a nuclear event, contamination (broad or limited) of the population or of specific workers might occur. In such a senario, the fate of actinide contaminants may be of first concern, in particular with regard to human target organs like the skeleton. To improve our understanding of the toxicological processes that might take place, a mechanistic approach is necessary. For instance, ∼50% of Pu(IV) is known from biokinetic data to accumulate in bone, but the underlining mechanisms are almost unknown. In this context, and to obtain a better description of the toxicological mechanisms associated with actinides(IV), we have undertaken the investigation, on a molecular scale, of the interaction of thorium(IV) with osteopontin (OPN) a hyperphosphorylated protein involved in bone turnover. Thorium is taken here as a simple model for actinide(IV) chemistry. In addition, we have selected a phosphorylated hexapeptide (His-pSer-Asp-Glu-pSer-Asp-Glu-Val) that is representative of the peptidic sequence involved in the bone interaction. For both the protein and the biomimetic peptide, we have determined the local environment of Th(IV) within the bioactinidic complex, combining isothermal titration calorimetry, attenuated total reflectance Fourier transform infrared spectroscopy, theoretical calculations with density functional theory, and extended X-ray absorption fine structure spectroscopy at the Th LIII edge. The results demonstrate a predominance of interaction of metal with the phosphate groups and confirmed the previous physiological studies that have highlighted a high affinity of Th(IV) for the bone matrix. Data are further compared with those of the uranyl case, representing the actinyl(V) and actinyl(VI) species. Last, our approach shows the importance of developing simplified systems [Th(IV)-peptide] that can serve as models for more biologically relevant systems.

  3. Analysis methodology and development of a statistical tool for biodistribution data from internal contamination with actinides.

    Science.gov (United States)

    Lamart, Stephanie; Griffiths, Nina M; Tchitchek, Nicolas; Angulo, Jaime F; Van der Meeren, Anne

    2017-03-01

    The aim of this work was to develop a computational tool that integrates several statistical analysis features for biodistribution data from internal contamination experiments. These data represent actinide levels in biological compartments as a function of time and are derived from activity measurements in tissues and excreta. These experiments aim at assessing the influence of different contamination conditions (e.g. intake route or radioelement) on the biological behavior of the contaminant. The ever increasing number of datasets and diversity of experimental conditions make the handling and analysis of biodistribution data difficult. This work sought to facilitate the statistical analysis of a large number of datasets and the comparison of results from diverse experimental conditions. Functional modules were developed using the open-source programming language R to facilitate specific operations: descriptive statistics, visual comparison, curve fitting, and implementation of biokinetic models. In addition, the structure of the datasets was harmonized using the same table format. Analysis outputs can be written in text files and updated data can be written in the consistent table format. Hence, a data repository is built progressively, which is essential for the optimal use of animal data. Graphical representations can be automatically generated and saved as image files. The resulting computational tool was applied using data derived from wound contamination experiments conducted under different conditions. In facilitating biodistribution data handling and statistical analyses, this computational tool ensures faster analyses and a better reproducibility compared with the use of multiple office software applications. Furthermore, re-analysis of archival data and comparison of data from different sources is made much easier. Hence this tool will help to understand better the influence of contamination characteristics on actinide biokinetics. Our approach can aid

  4. Actinide Production in the Reaction of Heavy Ions withCurium-248

    Energy Technology Data Exchange (ETDEWEB)

    Moody, K.J.

    1983-07-01

    Chemical experiments were performed to examine the usefulness of heavy ion transfer reactions in producing new, neutron-rich actinide nuclides. A general quasi-elastic to deep-inelastic mechanism is proposed, and the utility of this method as opposed to other methods (e.g. complete fusion) is discussed. The relative merits of various techniques of actinide target synthesis are discussed. A description is given of a target system designed to remove the large amounts of heat generated by the passage of a heavy ion beam through matter, thereby maximizing the beam intensity which can be safely used in an experiment. Also described is a general separation scheme for the actinide elements from protactinium (Z = 91) to mendelevium (Z = 101), and fast specific procedures for plutonium, americium and berkelium. The cross sections for the production of several nuclides from the bombardment of {sup 248}Cm with {sup 18}O, {sup 86}Kr and {sup 136}Xe projectiles at several energies near and below the Coulomb barrier were determined. The results are compared with yields from {sup 48}Ca and {sup 238}U bombardments of {sup 248}Cm. Simple extrapolation of the product yields into unknown regions of charge and mass indicates that the use of heavy ion transfer reactions to produce new, neutron-rich above-target species is limited. The substantial production of neutron-rich below-target species, however, indicates that with very heavy ions like {sup 136}Xe and {sup 238}U the new species {sup 248}Am, {sup 249}Am and {sup 247}Pu should be produced with large cross sections from a {sup 248}Cm target. A preliminary, unsuccessful attempt to isolate {sup 247}Pu is outlined. The failure is probably due to the half life of the decay, which is calculated to be less than 3 minutes. The absolute gamma ray intensities from {sup 251}Bk decay, necessary for calculating the {sup 251}Bk cross section, are also determined.

  5. Isotopic and elemental composition of plutonium/americium oxides influence pulmonary and extra-pulmonary distribution after inhalation in rats.

    Science.gov (United States)

    Van der Meeren, A; Grémy, O

    2010-09-01

    The biodistribution of plutonium and americium has been studied in a rat model after inhalation of two PuO(2) powders in lungs and extra-pulmonary organs from 3 d to 3 mo. The main difference between the two powders was the content of americium (approximately 46% and 4.5% of total alpha activity). The PuO(2) with a higher proportion of americium shows an accelerated transfer of activity from lungs to blood as compared to PuO(2) with the lower americium content, illustrated by increased urinary excretion and higher bone and liver actinide retention. The total alpha activity measured reflects mostly the americium biological behavior. The activity contained in epithelial lining fluid, recovered in the acellular phase of broncho-alveolar lavages, mainly contains americium, whereas plutonium remains trapped in macrophages. Epithelial lining fluid could represent a transitional pulmonary compartment prior to translocation of actinides to the blood and subsequent deposition in extra-pulmonary retention organs. In addition, differential behaviors of plutonium and americium are also observed between the PuO(2) powders with a higher dissolution rate for both plutonium and americium being obtained for the PuO(2) with the highest americium content. Our results indicate that the biological behavior of plutonium and americium after translocation into blood differ two-fold: (1) for the two actinides for the same PuO(2) aerosol, and (2) for the same actinide from the two different aerosols. These results highlight the importance of considering the specific behavior of each contaminant after accidental pulmonary intake when assessing extra-pulmonary deposits from the level of activity excreted in urine or for therapeutic strategy decisions.

  6. High-spin states in boson models with applications to actinide nuclei

    CERN Document Server

    Kuyucak, S

    1995-01-01

    We use the 1/N expansion formalism in a systematic study of high-spin states in the sd and sdg boson models with emphasis on spin dependence of moment of inertia and E2 transitions. The results are applied to the high-spin states in the actinide nuclei ^{232}Th, ^{234-238}U, where the need for g bosons is especially acute but until now, no realistic calculation existed. We find that the d-boson energy plays a crucial role in description of the high-spin data.

  7. ORNL actinide materials and a new detection system for superheavy nuclei

    Directory of Open Access Journals (Sweden)

    Rykaczewski Krzysztof P.

    2016-01-01

    Full Text Available The actinide resources and production capabilities at Oak Ridge National Laboratory (ORNL are reviewed, including potential electromagnetic separation of rare radioactive materials. The first experiments at the Dubna Gas Filled Recoil Separator (DGFRS with a new digital detection system developed at ORNL and University of Tennessee Knoxville (UTK are presented. These studies used 240Pu material provided by ORNL and mixed-Cf targets made at ORNL. The proposal to use an enriched 251Cf target and a large dose of 58Fe beam to reach the N = 184 shell closure and to observe new elements with Z = 124, 122 and 120 is discussed.

  8. MICROBIAL TRANSFORMATIONS OF TRU AND MIXED WASTES: ACTINIDE SPECIATION AND WASTE VOLUME REDUCTION

    Energy Technology Data Exchange (ETDEWEB)

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

    2006-06-01

    The overall goals of this research project are to determine the mechanism of microbial dissolution and stabilization of actinides in Department of Energy’s (DOE) TRU wastes, contaminated sludges, soils, and sediments. This includes (i) investigations on the fundamental aspects of microbially catalyzed radionuclide and metal transformations (oxidation/reduction reactions, dissolution, precipitation, chelation); (ii) understanding of the microbiological processes that control speciation and alter the chemical forms of complex inorganic/organic contaminant mixtures; and (iii) development of new and improved microbially catalyzed processes resulting in immobilization of metals and radionuclides in the waste with concomitant waste volume reduction.

  9. MICROBIAL TRANSFORMATIONS OF TRU AND MIXED WASTES: ACTINIDE SPECIATION AND WASTE VOLUME REDUCTION.

    Energy Technology Data Exchange (ETDEWEB)

    FRANCIS, A.J.; DODGE, C.J.

    2006-11-16

    The overall goals of this research project are to determine the mechanism of microbial dissolution and stabilization of actinides in Department of Energy's (DOE) TRU wastes, contaminated sludges, soils, and sediments. This includes (1) investigations on the fundamental aspects of microbially catalyzed radionuclide and metal transformations (oxidation/reduction reactions, dissolution, precipitation, chelation); (2) understanding of the microbiological processes that control speciation and alter the chemical forms of complex inorganic/organic contaminant mixtures; and (3) development of new and improved microbially catalyzed processes resulting in immobilization of metals and radionuclides in the waste with concomitant waste volume reduction.

  10. MICROBIAL TRANSFORMATIONS OF TRU AND MIXED WASTES: ACTINIDE SPECIATION AND WASTE VOLUME REDUCTION

    Energy Technology Data Exchange (ETDEWEB)

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

    2006-06-01

    The overall goals of this research project are to determine the mechanism of microbial dissolution and stabilization of actinides in Department of Energy's (DOE) TRU wastes, contaminated sludges, soils, and sediments. This includes (1) investigations on the fundamental aspects of microbially catalyzed radionuclide and metal transformations (oxidation/reduction reactions, dissolution, precipitation, chelation); (2) understanding of the microbiological processes that control speciation and alter the chemical forms of complex inorganic/organic contaminant mixtures; and (3) development of new and improved microbially catalyzed processes resulting in immobilization of metals and radionuclides in the waste with concomitant waste volume reduction.

  11. Bidentate organophosphorus extractants: purification, properties and applications to removal of actinides from acidic waste solutions

    Energy Technology Data Exchange (ETDEWEB)

    Schulz, W.W.; McIsaac, L.D.

    1977-05-01

    At both Hanford and Idaho, DHDECMP (dihexyl-N, N-diethylcarbamylmethylene phosphonate) continuous counter-current solvent extraction processes are being developed for removal of americium, plutonium, and, in some cases, other actinides from acidic wastes generated at these locations. Bench and, eventually, pilot and plant-scale testing and application of these processes have been substantially enhanced by the discovery of suitable chemical and physical methods of removing deleterious impurities from technical-grade DHDECMP. Flowsheet details, as well as various properties of purified DHDECMP extractants, are enumerated.

  12. Detection limits for actinides in a monochromatic, wavelength-dispersive x-ray fluorescence instrument

    Energy Technology Data Exchange (ETDEWEB)

    Collins, Michael L [Los Alamos National Laboratory; Havrilla, George J [Los Alamos National Laboratory

    2009-01-01

    Recent developments in x-ray optics have made it possible to examine the L x-rays of actinides using doubly-curved crystals in a bench-top device. A doubly-curved crystal (DCC) acts as a focusing monochromatic filter for polychromatic x-rays. A Monochromatic, Wavelength-Dispersive X-Ray Fluorescence (MWDXRF) instrument that uses DCCs to measure Cm and Pu in reprocessing plant liquors was proposed in 2007 by the authors at Los Alamos National Laboratory. A prototype design of this MWDXRF instrument was developed in collaboration with X-ray Optical Systems Inc. (XOS), of East Greenbush, New York. In the MWDXRF instrument, x-rays from a Rhodium-anode x-ray tube are passed through a primary DCC to produce a monochromatic beam of 20.2-keV photons. This beam is focused on a specimen that may contain actinides. The 20.2-keV interrogating beam is just above the L3 edge of Californium; each actinide (with Z = 90 to 98) present in the specimen emits characteristic L x-rays as the result of L3-shell vacancies. In the LANL-XOS prototype MWDXRf, these x-rays enter a secondary DCC optic that preferentially passes 14.961-keV photons, corresponding to the L-alpha-1 x-ray peak of Curium. In the present stage of experimentation, Curium-bearing specimens have not been analyzed with the prototype MWDXRF instrument. Surrogate materials for Curium include Rubidium, which has a K-beta-l x-ray at 14.961 keV, and Yttrium, which has a K-alpha-1 x-ray at 14.958 keV. In this paper, the lower limit of detection for Curium in the LANL-XOS prototype MWDXRF instrument is estimated. The basis for this estimate is described, including a description of computational models and benchmarking techniques used. Detection limits for other actinides are considered, as well as future safeguards applications for MWDXRF instrumentation.

  13. Micro-Analysis of Actinide Minerals for Nuclear Forensics and Treaty Verification

    Energy Technology Data Exchange (ETDEWEB)

    M. Morey, M. Manard, R. Russo, G. Havrilla

    2012-03-22

    Micro-Raman spectroscopy has been demonstrated to be a viable tool for nondestructive determination of the crystal phase of relevant minerals. Collecting spectra on particles down to 5 microns in size was completed. Some minerals studied were weak scatterers and were better studied with the other techniques. A decent graphical software package should easily be able to compare collected spectra to a spectral library as well as subtract out matrix vibration peaks. Due to the success and unequivocal determination of the most common mineral false positive (zircon), it is clear that Raman has a future for complementary, rapid determination of unknown particulate samples containing actinides.

  14. Simulation of alpha decay of actinides in iron phosphate glasses by ion irradiation

    Science.gov (United States)

    Dube, Charu L.; Stennett, Martin C.; Gandy, Amy S.; Hyatt, Neil C.

    2016-03-01

    A surrogate approach of ion beam irradiation is employed to simulate alpha decay of actinides in iron phosphate nuclear waste glasses. Bismuth and helium ions of different energies have been selected for simulating glass matrix modification owing to radiolysis and ballistic damage due to recoil atoms. Structural modification and change in coordination number of network former were probed by employing Reflectance Fourier-Transform Infrared (FT-IR), and Raman spectroscopies as a consequence of ion irradiation. Depolymerisation is observed in glass sample irradiated at intermediate energy of 2 MeV. Helium blisters of micron size are seen in glass sample irradiated at low helium ion energy of 30 keV.

  15. Nucleon scattering on actinides using a dispersive optical model with extended couplings

    Science.gov (United States)

    Soukhovitskiĩ, E. Sh.; Capote, R.; Quesada, J. M.; Chiba, S.; Martyanov, D. S.

    2016-12-01

    The Tamura coupling model [Rev. Mod. Phys. 37, 679 (1965), 10.1103/RevModPhys.37.679] has been extended to consider the coupling of additional low-lying rotational bands to the ground-state band. Rotational bands are built on vibrational bandheads (even-even targets) or single-particle bandheads (odd-A targets) including both axial and nonaxial deformations. These additional excitations are introduced as a perturbation to the underlying axially symmetric rigid-rotor structure of the ground-state rotational band. Coupling matrix elements of the generalized optical model are derived for extended multiband transitions in even-even and odd-A nuclei. Isospin symmetric formulation of the optical model is employed. A coupled-channels optical-model potential (OMP) containing a dispersive contribution is used to fit simultaneously all available optical experimental databases including neutron strength functions for nucleon scattering on 232Th,233,235,238U, and 239Pu nuclei. Quasielastic (p ,n ) scattering data on 232Th and 238U to the isobaric analog states of the target nucleus are also used to constrain the isovector part of the optical potential. Lane consistent OMP is derived for all actinides if corresponding multiband coupling schemes are defined. For even-even (odd-A ) actinides almost all low-lying collective levels below 1 MeV (0.5 MeV) of excitation energy are coupled. OMP parameters show a smooth energy dependence and energy-independent geometry. A phenomenological optical-model potential that couples multiple bands in odd-A actinides is published for a first time. Calculations using the derived OMP potential reproduce measured total cross-section differences between several actinide pairs within experimental uncertainty for incident neutron energies from 50 keV up to 150 MeV. The importance of extended coupling is studied. Multiband coupling is stronger in even-even targets owing to the collective nature of the coupling; the impact of extended coupling on

  16. Sigma Team for Minor Actinide Separation: PNNL FY 2011 Status Report

    Energy Technology Data Exchange (ETDEWEB)

    Lumetta, Gregg J.; Braley, Jenifer C.; Sinkov, Sergey I.; Levitskaia, Tatiana G.; Carter, Jennifer C.; Warner, Marvin G.; Pittman, Jonathan W.

    2011-08-13

    This report summarizes work conducted in FY 2011 at PNNL to investigate new methods of separating the minor actinide elements (Am and Cm) from the trivalent lanthanide elements, and separation of Am from Cm. For the former, work focused on a solvent extraction system combining an acidic extractant (HDEHP) with a neutral extractant (CMPO) to form a hybrid solvent extraction system referred to as TRUSPEAK (combining the TRUEX and TALSPEAK processes). For the latter, ligands that strongly bing uranyl ion were investigated for stabilizing corresponding americyl ion.

  17. Measurement of boron isotopes by negative thermal ionization mass spectrometry

    Institute of Scientific and Technical Information of China (English)

    2000-01-01

    The isobaric interference for boron isotopic measurement by negative thermal ionization mass spectrometry (NTIMS) has been studied. The result shows that the CNO- is not only from the organic material, but also from nitrate in loading reagent in NTIMS. Monitoring the mass 43 ion intensity and 43/42 ratio of blank are also necessary for the boron isotopic measurement by NTIMS, other than is only boron content.

  18. Isotope Ratio Monitoring Gas Chromatography Mass Spectrometry (IRM-GCMS)

    Science.gov (United States)

    Freeman, K. H.; Ricci, S. A.; Studley, A.; Hayes, J. M.

    1989-01-01

    On Earth, the C-13 content of organic compounds is depleted by roughly 13 to 23 permil from atmospheric carbon dioxide. This difference is largely due to isotope effects associated with the fixation of inorganic carbon by photosynthetic organisms. If life once existed on Mars, then it is reasonable to expect to observe a similar fractionation. Although the strongly oxidizing conditions on the surface of Mars make preservation of ancient organic material unlikely, carbon-isotope evidence for the existence of life on Mars may still be preserved. Carbon depleted in C-13 could be preserved either in organic compounds within buried sediments, or in carbonate minerals produced by the oxidation of organic material. A technique is introduced for rapid and precise measurement of the C-13 contents of individual organic compounds. A gas chromatograph is coupled to an isotope-ratio mass spectrometer through a combustion interface, enabling on-line isotopic analysis of isolated compounds. The isotope ratios are determined by integration of ion currents over the course of each chromatographic peak. Software incorporates automatic peak determination, corrections for background, and deconvolution of overlapped peaks. Overall performance of the instrument was evaluated by the analysis of a mixture of high purity n-alkanes of know isotopic composition. Isotopic values measured via IRM-GCMS averaged withing 0.55 permil of their conventionally measured values.

  19. Perchlorate isotope forensics

    Science.gov (United States)

    Böhlke, J.K.; Sturchio, N.C.; Gu, B.; Horita, J.; Brown, G.M.; Jackson, W.A.; Batista, J.; Hatzinger, P.B.

    2005-01-01

    Perchlorate has been detected recently in a variety of soils, waters, plants, and food products at levels that may be detrimental to human health. These discoveries have generated considerable interest in perchlorate source identification. In this study, comprehensive stable isotope analyses ( 37Cl/35Cl and 18O/17O/ 16O) of perchlorate from known synthetic and natural sources reveal systematic differences in isotopic characteristics that are related to the formation mechanisms. In addition, isotopic analyses of perchlorate extracted from groundwater and surface water demonstrate the feasibility of identifying perchlorate sources in contaminated environments on the basis of this technique. Both natural and synthetic sources of perchlorate have been identified in water samples from some perchlorate occurrences in the United States by the isotopic method. ?? 2005 American Chemical Society.

  20. Isotope Production Facility (IPF)

    Data.gov (United States)

    Federal Laboratory Consortium — The Los Alamos National Laboratory has produced radioactive isotopes for medicine and research since the mid 1970s, when targets were first irradiated using the 800...

  1. Calcium stable isotope geochemistry

    Energy Technology Data Exchange (ETDEWEB)

    Gausonne, Nikolaus [Muenster Univ. (Germany). Inst. fuer Mineralogie; Schmitt, Anne-Desiree [Strasbourg Univ. (France). LHyGeS/EOST; Heuser, Alexander [Bonn Univ. (Germany). Steinmann-Inst. fuer Geologie, Mineralogie und Palaeontologie; Wombacher, Frank [Koeln Univ. (Germany). Inst. fuer Geologie und Mineralogie; Dietzel, Martin [Technische Univ. Graz (Austria). Inst. fuer Angewandte Geowissenschaften; Tipper, Edward [Cambridge Univ. (United Kingdom). Dept. of Earth Sciences; Schiller, Martin [Copenhagen Univ. (Denmark). Natural History Museum of Denmark

    2016-08-01

    This book provides an overview of the fundamentals and reference values for Ca stable isotope research, as well as current analytical methodologies including detailed instructions for sample preparation and isotope analysis. As such, it introduces readers to the different fields of application, including low-temperature mineral precipitation and biomineralisation, Earth surface processes and global cycling, high-temperature processes and cosmochemistry, and lastly human studies and biomedical applications. The current state of the art in these major areas is discussed, and open questions and possible future directions are identified. In terms of its depth and coverage, the current work extends and complements the previous reviews of Ca stable isotope geochemistry, addressing the needs of graduate students and advanced researchers who want to familiarize themselves with Ca stable isotope research.

  2. Isotopes in Greenland Precipitation

    DEFF Research Database (Denmark)

    Faber, Anne-Katrine

    the Arctic Ocean. A comprehensive database is created based on ice core and weather station data from Greenland within the period 1890-2014. Present day annual and seasonal mean values are computed for 326 locations in Greenland. Parameterization of the spatial distribution of temperature and δ18O are used...... of model and data can be used to improve the understanding of climate changes. This is done through analysis of isotope modelling, observations and ice core measurements. This dissertation comprises three projects: (1) Modelling the isotopic response to changes in Arctic sea surface conditions, (2......) Constructing a new Greenland database of observations and present-day ice core measurements, and (3) Performance test of isotope-enabled CAM5 for Greenland. The recent decades of rapid Arctic sea ice decline are used as a basis for an observational-based model experiment using the isotope-enabled CAM model 3...

  3. Isotopically controlled semiconductors

    Energy Technology Data Exchange (ETDEWEB)

    Haller, E.E.

    2004-11-15

    A review of recent research involving isotopically controlled semiconductors is presented. Studies with isotopically enriched semiconductor structures experienced a dramatic expansion at the end of the Cold War when significant quantities of enriched isotopes of elements forming semiconductors became available for worldwide collaborations. Isotopes of an element differ in nuclear mass, may have different nuclear spins and undergo different nuclear reactions. Among the latter, the capture of thermal neutrons which can lead to neutron transmutation doping, can be considered the most important one for semiconductors. Experimental and theoretical research exploiting the differences in all the properties has been conducted and will be illustrated with selected examples. Manuel Cardona, the longtime editor-in-chief of Solid State Communications has been and continues to be one of the major contributors to this field of solid state physics and it is a great pleasure to dedicate this review to him.

  4. Assessment of sensitivity of neutron-physical parameters of fast neutron reactor to purification of reprocessed fuel from minor actinides

    Science.gov (United States)

    Cherny, V. A.; Kochetkov, L. A.; Nevinitsa, A. I.

    2013-12-01

    The work is devoted to computational investigation of the dependence of basic physical parameters of fast neutron reactors on the degree of purification of plutonium from minor actinides obtained as a result of pyroelectrochemical reprocessing of spent nuclear fuel and used for manufacturing MOX fuel to be reloaded into the reactors mentioned. The investigations have shown that, in order to preserve such important parameters of a BN-800 type reactor as the criticality, the sodium void reactivity effect, the Doppler effect, and the efficiency of safety rods, it is possible to use the reprocessed fuel without separation of minor actinides for refueling (recharging) the core.

  5. Isotopes through the looking glass

    Science.gov (United States)

    Mårtensson Pendrill, Ann Marie

    2000-08-01

    Nuclear distributions affect many aspects of atomic spectra. As an example, recent experimental results for the hyperfine anomaly in Fr isotopes are considered. These depend on nuclear charge and magnetization distributions. The variations in charge radii for these isotopes were studied earlier by measuring optical isotope shifts. The hyperfine anomalies for the odd-odd isotopes involve the neutron distributions, of interest for studies of parity nonconserving effects along a chain of isotopes.

  6. Methods of isotopic geochronology

    Science.gov (United States)

    Gorokhov, I. M.; Levchenkov, O. A.

    Papers are presented on such topics as the age of the chemical elements; the age of meteorites, the moon, and the earth; isotopic ages of the most ancient terrestrial formations; and the Archean evolution of Enderby Land in the Antarctic as evidenced by isotopic dating. Consideration is also given to a uranium-lead geochronology technique for investigating Precambrian ore deposits, a Pb-Pb technique of zircon dating, and the potentials and limitations of Sm-Nd geochronology.

  7. Standard test method for analysis of total and isotopic uranium and total thorium in soils by inductively coupled plasma-mass spectrometry

    CERN Document Server

    American Society for Testing and Materials. Philadelphia

    2008-01-01

    1.1 This test method covers the measurement of total uranium (U) and thorium (Th) concentrations in soils, as well as the determination of the isotopic weight percentages of 234U, 235U, 236U, and 238U, thereby allowing for the calculation of individual isotopic uranium activity or total uranium activity. This inductively coupled plasma-mass spectroscopy (ICP-MS) method is intended as an alternative analysis to methods such as alpha spectroscopy or thermal ionization mass spectroscopy (TIMS). Also, while this test method covers only those isotopes listed above, the instrumental technique may be expanded to cover other long-lived radioisotopes since the preparation technique includes the preconcentration of the actinide series of elements. The resultant sample volume can be further reduced for introduction into the ICP-MS via an electrothermal vaporization (ETV) unit or other sample introduction device, even though the standard peristaltic pump introduction is applied for this test method. The sample preparatio...

  8. Mass-dependent fractionation of nickel isotopes in meteoritic metal

    Science.gov (United States)

    Cook, David L.; Wadhwa, Meenakshi; Clayton, Robert N.; Dauphas, Nicolas; Janney, Philip E.; Davis, Andrew M.

    We measured nickel isotopes via multicollector inductively coupled plasma mass spectrometry (MC-ICPMS) in the bulk metal from 36 meteorites, including chondrites, pallasites, and irons (magmatic and non-magmatic). The Ni isotopes in these meteorites are mass fractionated; the fractionation spans an overall range of ≈0.4‰ amu-1. The ranges of Ni isotopic compositions (relative to the SRM 986 Ni isotopic standard) in metal from iron meteorites (≈0.0 to ≈0.3‰ amu-1) and chondrites (≈0.0 to ≈0.2‰ amu-1) are similar, whereas the range in pallasite metal (≈-0.1 to 0.0‰ amu-1) appears distinct. The fractionation of Ni isotopes within a suite of fourteen IIIAB irons (≈0.0 to ≈0.3‰ amu-1) spans the entire range measured in all magmatic irons. However, the degree of Ni isotopic fractionation in these samples does not correlate with their Ni content, suggesting that core crystallization did not fractionate Ni isotopes in a systematic way. We also measured the Ni and Fe isotopes in adjacent kamacite and taenite from the Toluca IAB iron meteorite. Nickel isotopes show clearly resolvable fractionation between these two phases; kamacite is heavier relative to taenite by ≈0.4‰ amu-1. In contrast, the Fe isotopes do not show a resolvable fractionation between kamacite and taenite. The observed isotopic compositions of kamacite and taenite can be understood in terms of kinetic fractionation due to diffusion of Ni during cooling of the Fe-Ni alloy and the development of the Widmanstätten pattern.

  9. Oxygen Isotopes in Meteorites

    Science.gov (United States)

    Clayton, R. N.

    2003-12-01

    Oxygen isotope abundance variations in meteorites are very useful in elucidating chemical and physical processes that occurred during the formation of the solar system (Clayton, 1993). On Earth, the mean abundances of the three stable isotopes are 16O: 99.76%, 17O: 0.039%, and 18O: 0.202%. It is conventional to express variations in abundances of the isotopes in terms of isotopic ratios, relative to an arbitrary standard, called SMOW (for standard mean ocean water), as follows:The isotopic composition of any sample can then be represented by one point on a "three-isotope plot," a graph of δ17O versus δ18O. It will be seen that such plots are invaluable in interpreting meteoritic data. Figure 1 shows schematically the effect of various processes on an initial composition at the center of the diagram. Almost all terrestrial materials lie along a "fractionation" trend; most meteoritic materials lie near a line of "16O addition" (or subtraction). (4K)Figure 1. Schematic representation of various isotopic processes shown on an oxygen three-isotope plot. Almost all terrestrial materials plot along a line of "fractionation"; most primitive meteoritic materials plot near a line of "16O addition." The three isotopes of oxygen are produced by nucleosynthesis in stars, but by different nuclear processes in different stellar environments. The principal isotope, 16O, is a primary isotope (capable of being produced from hydrogen and helium alone), formed in massive stars (>10 solar masses), and ejected by supernova explosions. The two rare isotopes are secondary nuclei (produced in stars from nuclei formed in an earlier generation of stars), with 17O coming primarily from low- and intermediate-mass stars (shielding in the UV photodissociation of CO (van Dishoeck and Black, 1988). This process results from the large differences in abundance between C16O, on the one hand, and C17O and C18O on the other. Photolysis of CO occurs by absorption of stellar UV radiation in the

  10. Fission decay properties of ultra neutron-rich uranium isotopes

    Indian Academy of Sciences (India)

    L Satpathy; S K Patra; R K Choudhury

    2008-01-01

    The fission decay of highly neutron-rich uranium isotopes is investigated which shows interesting new features in the barrier properties and neutron emission characteristics in the fission process. 233U and 235U are the nuclei in the actinide region in the beta stability valley which are thermally fissile and have been mainly used in reactors for power generation. The possibility of occurrence of thermally fissile members in the chain of neutron-rich uranium isotopes is examined here. The neutron number = 162 or 164 has been predicted to be magic in numerous theoretical studies carried out over the years. The series of uranium isotopes around it with = 154-172 are identified to be thermally fissile on the basis of the fission barrier and neutron separation energy systematics; a manifestation of the close shell nature of = 162 (or 164). We consider here the thermal neutron fission of a typical representative 249U nucleus in the highly neutron-rich region. Semiempirical study of fission barrier height and width shows that 250U nucleus is stable against spontaneous fission due to increase in barrier width arising out of excess neutrons. On the basis of the calculation of the probability of fragment mass yields and the microscopic study in relativistic mean field theory, this nucleus is shown to undergo exotic decay mode of thermal neutron fission (multi-fragmentation fission) whereby a number of prompt scission neutrons are expected to be simultaneously released along with the two heavy fission fragments. Such properties will have important implications in stellar evolution involving -process nucleosynthesis.

  11. Characterization of partitioning relevant lanthanide and actinide complexes by NMR spectroscopy; Charakterisierung von partitioningrelevanten Lanthaniden- und Actinidenkomplexen mittels NMR-Spektroskopie

    Energy Technology Data Exchange (ETDEWEB)

    Adam, Christian

    2016-01-15

    In the present work the interaction of N-donor ligands, such as 2,6-Bis(5,6-dipropyl-1,2,4-triazin-3-yl)pyridine (nPrBTP) and 2,6-Bis(5-(2,2-dimethylpropyl)1H-pyrazol)-3-yl-pyridine (C5-BPP), with trivalent lanthanide and actinide ions was studied. Ligands of this type show a high selectivity for the separation of trivalent actinide ions over lanthanides from nitric acid solutions. However, the reason for this selectivity, which is crucial for future partitioning and transmutation strategies for radioactive wastes, is still unknown. So far, the selectivity of some N-donor ligands is supposed to be an effect of an increased covalency in the actinide-ligand bond, compared to the lanthanide compounds. NMR spectroscopy on paramagnetic metal complexes is an excellent tool for the elucidation of bonding modes. The overall paramagnetic chemical shift consists of two contributions, the Fermi Contact Shift (FCS), due to electron spin delocalisation through covalent bonds, and the Pseudo Contact Shift (PCS), which describes the dipolar coupling of the electron magnetic moment and the nuclear spin. By assessing the FCS share in the paramagnetic shift, the degree of covalency in the metal-ligand bond can be gauged. Several methods to discriminate FCS and PCS have been used on the data of the nPrBTP- and C5-BPP-complexes and were evaluated regarding their applicability on lanthanide and actinide complexes with N-donor ligands. The study comprised the synthesis of all Ln(III) complexes with the exceptions of Pm(III) and Gd(III) as well as the Am(III) complex as a representative of the actinide series with both ligands. All complexes were fully characterised ({sup 1}H, {sup 13}C and {sup 15}N spectra) using NMR spectroscopy. By isotope enrichment with the NMR-active {sup 15}N in positions 8 and 9 in both ligands, resonance signals of these nitrogen atoms were detected for all complexes. The Bleaneymethod relies on different temperature dependencies for FCS (T{sup -1}) and PCS (T

  12. Synthesis, phase structure and microstructure of monazite-type Ce1-xPrxPO4 solid solutions for immobilization of minor actinide neptunium

    Science.gov (United States)

    Zeng, Pan; Teng, Yuancheng; Huang, Yi; Wu, Lang; Wang, Xiaohuan

    2014-09-01

    Praseodymium was used as the surrogate for trivalent minor actinide neptunium, and a complete series of pure monazite-type Ce1-xPrxPO4 (x = 0-1) solid solutions were successfully prepared by the solid state reaction. The effects of calcining temperature, holding time and Pr content on the structure of Ce1-xPrxPO4 solid solutions were investigated. The results show that although Pr6O11 (Pr23+Pr44+O11) exists two stabilized oxidation states, there has been no tetravalent praseodymium phosphate during the synthesis process. The optimized temperature for the synthesis of Ce0.8Pr0.2PO4 solid solution is more than 1100 °C, and a hypothetical reaction mechanism is also proposed. Besides, the crystalline grains coarsen as the increasing of holding time. The linear variation of unit cell parameters and a gradual hypsochromic shift in the Raman spectra are observed with the increase of Pr content, indicating that cerium is progressively replaced by praseodymium and Ce1-xPrxPO4 solid solutions were prepared.

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

    Science.gov (United States)

    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.

  14. Supercritical Carbon Dioxide-Soluble Ligands for Extracting Actinide Metal Ions from Porous Solids

    Energy Technology Data Exchange (ETDEWEB)

    Joan Brennecke; Mark Dietz; Richard Barrans; Alabert Herlinger

    2003-07-03

    Numerous types of actinide-bearing waste materials are found throughout the DOE complex. Most of these wastes consist of large volumes of non-hazardous materials contaminated with relatively small quantities of actinide elements. Separation of these wastes into their inert and radioactive components would dramatically reduce the costs of stabilization and disposal. For example, the DOE is responsible for decontaminating concrete within 7000 surplus contaminated buildings. The best technology now available for removing surface contamination from concrete involves removing the surface layer by grit blasting, which produces a large volume of blasting residue containing a small amount of radioactive material. Disposal of this residue is expensive because of its large volume and fine particulate nature. Considerable cost savings would result from separation of the radioactive constituents and stabilization of the concrete dust. Similarly, gas diffusion plants for uranium enrichment contain valuable high-purity nickel in the form of diffusion barriers. Decontamination is complicated by the extremely fine pores in these barriers, which are not readily accessible by most cleaning techniques. A cost-effect method for the removal of radioactive contaminants would release this valuable material for salvage.

  15. The inverse-trans-influence in tetravalent lanthanide and actinide bis(carbene) complexes

    Science.gov (United States)

    Gregson, Matthew; Lu, Erli; Mills, David P.; Tuna, Floriana; McInnes, Eric J. L.; Hennig, Christoph; Scheinost, Andreas C.; McMaster, Jonathan; Lewis, William; Blake, Alexander J.; Kerridge, Andrew; Liddle, Stephen T.

    2017-02-01

    Across the periodic table the trans-influence operates, whereby tightly bonded ligands selectively lengthen mutually trans metal-ligand bonds. Conversely, in high oxidation state actinide complexes the inverse-trans-influence operates, where normally cis strongly donating ligands instead reside trans and actually reinforce each other. However, because the inverse-trans-influence is restricted to high-valent actinyls and a few uranium(V/VI) complexes, it has had limited scope in an area with few unifying rules. Here we report tetravalent cerium, uranium and thorium bis(carbene) complexes with trans C=M=C cores where experimental and theoretical data suggest the presence of an inverse-trans-influence. Studies of hypothetical praseodymium(IV) and terbium(IV) analogues suggest the inverse-trans-influence may extend to these ions but it also diminishes significantly as the 4f orbitals are populated. This work suggests that the inverse-trans-influence may occur beyond high oxidation state 5f metals and hence could encompass mid-range oxidation state actinides and lanthanides. Thus, the inverse-trans-influence might be a more general f-block principle.

  16. Studies into new solvent extraction reagents for the separation of trivalent minor actinides from trivalent lanthanides

    CERN Document Server

    Russell, M L

    2000-01-01

    Ligands, suitable for the separation of minor actinide(lll) cations from lanthanide(lll) cations from acidic aqueous media, have been synthesised. Two oligopyridine ligands, 4', 4''-(bis (4-tolyl))-2, 2': 6', 2'': 6'', 2'''-quaterpyridine and 4',4'''-(bis(4-heptyloxyphenyl))-2,2':6',2'':6'',2''':6''',2'''' -quinquepyridi= ne, have been synthesised and tested by solvent extraction experiments. The ability of the ligands to separate minor actinide from lanthanide has been attributed to the number of pyridyl rings present. A series of terpyridine analogues based on sym-triazine have been prepared, via the cyclisation of aromatic carbonitriles with guanidine. New lipophilic derivatives of 2-amino-bis(4,6(2-pyridyl))-1,3,5-triazine, 2-amino-bis(4,6(2-pyrazinyl)-1,3,5-triazine, 2-amino-bis(4,6(2-isoquinolinyl)-1,3,5-triazine, 2-amino-bis(4,6(2-(4-methyl)pyridyl)-1,3,5-triazine, 2-amino-bis(4,6(4-pyridyl)-1,3,5-triazine, 2-amino-bis(4,6(2-thiophenyl)-1,3,5-triazine and 2-amino-bis(4,6(2-quinolinyl)-1,3,5-triazine ha...

  17. Comparative evaluation of actinide ion uptake by polymer inclusion membranes containing TODGA as the carrier extractant.

    Science.gov (United States)

    Mahanty, B N; Raut, D R; Mohapatra, P K; Das, D K; Behere, P G; Afzal, Md

    2014-06-30

    Polymer inclusion membranes (PIM) containing TODGA (N,N,N',N'-tetra-n-octyl diglycolamide) were evaluated for the separation of actinide ions such as Am(3+), Pu(4+), UO2(2+) and Th(4+) from acidic feeds. The PIMs were prepared using cellulose triacetate (CTA) as the polymer matrix and 2-nitrophenyloctyl ether (NPOE) as the plasticizer along with the diglycolamide carrier extractants and were characterized by conventional techniques such as XRD, thermal analysis and AFM. The PIM composition was optimized by a series of studies which involved variation in the CTA, NPOE and carrier concentration which suggested 58% TODGA, 30% NPOE and 12% CTA to be optimum. The uptake studies were carried out using feed solutions containing varying concentrations of nitric acid and showed the trend: Am(3+)>Pu(4+)>Th(4+)>UO2(2+). Transport studies were carried out in a two-compartment cell where nitric acid concentration the feed was varied (1-3M) while the receiver compartment contained alpha-hydroxy-iso-butyric acid (AHIBA). The actinide ion transport efficiencies with TODGA containing PIMs followed the same trend as seen in the uptake studies. The AFM patterns of the PIMs changed when loaded with Eu(3+) carrier (used as a surrogate for Am(3+)) while the regenerated membranes have displayed comparable morphologies. Diffusion coefficient values were experimentally obtained from the transport studies and were found to be 8.89×10(-8) cm(2)/s for Am(3+) transport.

  18. A comparative study of actinide complexation in three ligand systems with increasing complexity

    Energy Technology Data Exchange (ETDEWEB)

    Jeanson, A; Dahou, S; Guillaumont, D; Moisy, P; Auwer, C Den [CEA Marcoule, DEN/DRCP/SCPS, 30207 Bagnols sur Ceze (France); Scheinost, A; Hennig, C [Forschungszentrum Dresden-Rossendorf, 01314 Dresden (Germany); Vidaud, C [CEA Marcoule DSV/iBEB/SBTN, 30207 Bagnols sur Ceze (France); Subra, G [Institut des Biomolecules Max Mousseron, CNRS UMR-5247, Universite Montpellier I-II, 34093 Montpellier (France); Solari, P L, E-mail: Christophe.denauwer@cea.f [Synchrotron SOLEIL, MARS beam line, 91192 Gif sur Yvette (France)

    2009-11-15

    The complexation of thorium, neptunium and plutonium at oxidation state +IV with three ligands of increasing complexity has been investigated. These ligands are relevant for bio inorganic systems. The first ligand is the small nitrilotriacetic acid that often play the role of protecting ligands against hydrolysis. EXAFS results for the Th to Pu series have been correlated to quantum chemical calculations and show an homogeneous behavior of the actinide at oxidation state +IV. For larger ligands, steric effects may become significant and one can ask how the ligand may accommodate the large actinide cation coordination sphere. Model pentapeptides have been synthesized and tested as complexing agents. Comparison with NTA shows that the molecular arrangements are radically different. The third ligand system is transferrin, a diferric metalloptrotein that is well known to coordinate a large variety of cations from transition metals of f-elements. Metalloproteins bear primary, secondary and tertiary structures that all play a crucial role in bonding. At a given oxidation state (+IV), but for various atomic numbers (Th, Np, Pu) EXAFS data at the cation L{sub III} edge exhibit significant coordination discrepancies that are related to a changes in protein geometry. In that sense, the metalloprotein may be viewed as a complex system.

  19. Thorium Phosphate - Diphosphate / Monazite based ceramics for the immobilization of actinides

    Energy Technology Data Exchange (ETDEWEB)

    Clavier, N.; Dacheux, N.; Podor, R.; Le Coustumer, P

    2004-07-01

    The elaboration of {beta}-TUPD/monazite based materials was performed in order to immobilize simultaneously tri- and tetravalent actinides and a neutron absorber. Both phases were initially prepared via the precipitation of crystallized precursors. The transformation of these solids into high-temperature phases was extensively studied. Two different processes were then considered to prepare composite materials either in the powder or in the pellet form. A good chemical compatibility was found between f{beta}-TUPD and monazite and the properties of both phases were kept in these composites. The relative density of the pellets reached 90 - 95 % of the value calculated from XRD data. The normalized dissolution rates determined in acidic media did not exceed 5.10{sup -4} g.m{sup -2}.day{sup -1} which confirms the very good durability of such materials during leaching tests. Moreover, the rapid precipitation of phosphate-based neo formed phases at the saturation of the leachate should delay significantly the release of actinides. (authors)

  20. Preparation of actinide targets by molecular plating for coulomb excitation studies at ATLAS

    CERN Document Server

    Greene, J P; Ahmad, I

    1999-01-01

    Molecular plating is now routinely used to prepare sources and targets of actinide elements. Although the technique is simple and fairly reproducible, because of the radioactive nature of the targets, it is very useful to record various parameters in the preparation process. At Argonne, approx 200 mu g/cm sup 2 thick targets of Pu and Cm were required for Coulomb Excitation (COULEX) studies with the Argonne-Notre Dame boron germanate (BGO) gamma-ray facility and later with the GAMMASPHERE. These targets were plated on 50 mg/cm sup 2 Au backings and were covered with 150 mu g/cm sup 2 Au foil. Targets of sup 2 sup 3 sup 9 Pu, sup 2 sup 4 sup 0 Pu, sup 2 sup 4 sup 2 Pu, sup 2 sup 4 sup 4 Pu and sup 2 sup 4 sup 8 Cm were prepared by dissolving the material in isopropyl alcohol and electroplating the actinide ions by applying 600 V. The amount of these materials on the target was determined by alpha particle counting and gamma-ray counting. Details of the molecular plating and counting will be discussed.