WorldWideScience

Sample records for actinide alloys

  1. 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...

  2. 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.

  3. 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.

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

    Energy Technology Data Exchange (ETDEWEB)

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

    2009-02-09

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

  5. Electronic structure and magnetic properties of selected lanthanide and actinide intermetallic Laves-phase alloys

    DEFF Research Database (Denmark)

    Eriksson, Olle; Johansson, Börje; Brooks, M. S. S.

    1989-01-01

    The electronic structure and magnetic properties of some yttrium and uranium Laves-phase pseudobinary alloys with 3d elements have been calculated. The calculations were done by simulating the electronic structure of the alloy by that of an ordered compound with the same stoichiometry. In general...

  6. 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.

  7. 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...

  8. 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)

  9. 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.)

  10. 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).

  11. 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.

  12. Alloy

    Science.gov (United States)

    Cabeza, Sandra; Garcés, Gerardo; Pérez, Pablo; Adeva, Paloma

    2014-07-01

    The Mg98.5Gd1Zn0.5 alloy produced by a powder metallurgy route was studied and compared with the same alloy produced by extrusion of ingots. Atomized powders were cold compacted and extruded at 623 K and 673 K (350 °C and 400 °C). The microstructure of extruded materials was characterized by α-Mg grains, and Mg3Gd and 14H-LPSO particles located at grain boundaries. Grain size decreased from 6.8 μm in the extruded ingot, down to 1.6 μm for powders extruded at 623 K (350 °C). Grain refinement resulted in an increase in mechanical properties at room and high temperatures. Moreover, at high temperatures the PM alloy showed superplasticity at high strain rates, with elongations to failure up to 700 pct.

  13. 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.

  14. 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.

  15. 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.

  16. 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.

  17. 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

  18. 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.

  19. 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.

  20. 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)

  1. 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.

  2. 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.

  3. 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.

  4. 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.

  5. 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.

  6. 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.

  7. 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.

  8. 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.

  9. 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)

  10. 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.

  11. 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

  12. 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).

  13. 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.

  14. 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.

  15. 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.

  16. 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.

  17. 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.

  18. 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.)

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

    Energy Technology Data Exchange (ETDEWEB)

    Morgan, Dane [Univ. of Wisconsin, Madison, WI (United States); Yang, Yong Austin [Univ. of Wisconsin, Madison, WI (United States)

    2013-10-28

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

  20. 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).

  1. 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.

  2. 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.

  3. 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.)

  4. 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...

  5. 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.)

  6. 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....

  7. 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.

  8. 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.)

  9. 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.

  10. 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

  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. 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

  14. 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.

  15. 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.)

  16. 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.

  17. 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.

  18. 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.)

  19. 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.

  20. 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).

  1. 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.

  2. 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

  3. 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.

  4. 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.

  5. 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.

  6. 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.

  7. 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...

  8. 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.

  9. 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)

  10. 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.

  11. Separation of actinides from irradiated An–Zr based fuel by electrorefining on solid aluminium cathodes in molten LiCl–KCl

    Energy Technology Data Exchange (ETDEWEB)

    Souček, P., E-mail: Pavel.Soucek@ec.europa.eu [European Commission, Joint Research Centre (JRC), Institute for Transuranium Elements (ITU), Postfach 2340, 76125 Karlsruhe (Germany); Murakami, T. [Central Research Institute of Electric Power Industry (CRIEPI), Komae-shi, Tokyo 201-8511 (Japan); Claux, B.; Meier, R.; Malmbeck, R. [European Commission, Joint Research Centre (JRC), Institute for Transuranium Elements (ITU), Postfach 2340, 76125 Karlsruhe (Germany); Tsukada, T. [Central Research Institute of Electric Power Industry (CRIEPI), Komae-shi, Tokyo 201-8511 (Japan); Glatz, J.-P. [European Commission, Joint Research Centre (JRC), Institute for Transuranium Elements (ITU), Postfach 2340, 76125 Karlsruhe (Germany)

    2015-04-15

    Highlights: • Electrorefining process in molten LiCl-KCl using solid Al electrodes was demonstrated. • High separation factors of actinides over lanthanides were achieved. • Efficient recovery of actinides from irradiated nuclear fuel was achieved. • Uniform, dense and well adhered deposits were obtained and characterised. • Kinetic parameters of actinide–aluminium alloy formation were evaluated. - Abstract: An electrorefining process for metallic spent nuclear fuel treatment is being investigated in ITU. Solid aluminium cathodes are used for homogeneous recovery of all actinides within the process carried out in molten LiCl–KCl eutectic salt at a temperature of 500 °C. As the selectivity, efficiency and performance of solid Al has been already shown using un-irradiated An–Zr alloy based test fuels, the present work was focused on laboratory-scale demonstration of the process using irradiated METAPHIX-1 fuel composed of U{sub 67}–Pu{sub 19}–Zr{sub 10}–MA{sub 2}–RE{sub 2} (wt.%, MA = Np, Am, Cm, RE = Nd, Ce, Gd, Y). Different electrorefining techniques, conditions and cathode geometries were used during the experiment yielding evaluation of separation factors, kinetic parameters of actinide–aluminium alloy formation, process efficiency and macro-structure characterisation of the deposits. The results confirmed an excellent separation and very high efficiency of the electrorefining process using solid Al cathodes.

  12. 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.

  13. 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.

  14. 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.

  15. 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.

  16. 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.

  17. 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.

  18. 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....

  19. 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.

  20. 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.

  1. 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.

  2. 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.

  3. 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.

  4. 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

  5. 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.

  6. A comparison of radioactive waste from first generation fusion reactors and fast fission reactors with actinide recycling

    Energy Technology Data Exchange (ETDEWEB)

    Koch, M.; Kazimi, M.S.

    1991-04-01

    Limitations of the fission fuel resources will presumably mandate the replacement of thermal fission reactors by fast fission reactors that operate on a self-sufficient closed fuel cycle. This replacement might take place within the next one hundred years, so the direct competitors of fusion reactors will be fission reactors of the latter rather than the former type. Also, fast fission reactors, in contrast to thermal fission reactors, have the potential for transmuting long-lived actinides into short-lived fission products. The associated reduction of the long-term activation of radioactive waste due to actinides makes the comparison of radioactive waste from fast fission reactors to that from fusion reactors more rewarding than the comparison of radioactive waste from thermal fission reactors to that from fusion reactors. Radioactive waste from an experimental and a commercial fast fission reactor and an experimental and a commercial fusion reactor has been characterized. The fast fission reactors chosen for this study were the Experimental Breeder Reactor 2 and the Integral Fast Reactor. The fusion reactors chosen for this study were the International Thermonuclear Experimental Reactor and a Reduced Activation Ferrite Helium Tokamak. The comparison of radioactive waste parameters shows that radioactive waste from the experimental fast fission reactor may be less hazardous than that from the experimental fusion reactor. Inclusion of the actinides would reverse this conclusion only in the long-term. Radioactive waste from the commercial fusion reactor may always be less hazardous than that from the commercial fast fission reactor, irrespective of the inclusion or exclusion of the actinides. The fusion waste would even be far less hazardous, if advanced structural materials, like silicon carbide or vanadium alloy, were employed.

  7. 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.

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

    Science.gov (United States)

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

    2012-01-01

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

  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. 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.

  11. 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...

  12. 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

  13. 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.

  14. 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.

  15. 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.

  16. 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.

  17. 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.

  18. 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.

  19. 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)

  20. 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

  1. 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.

  2. 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.

  3. 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.

  4. 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....

  5. 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)

  6. 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.

  7. 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

  8. 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.

  9. 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.

  10. 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).

  11. 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.

  12. Nuclear fuel alloys or mixtures and method of making thereof

    Science.gov (United States)

    Mariani, Robert Dominick; Porter, Douglas Lloyd

    2016-04-05

    Nuclear fuel alloys or mixtures and methods of making nuclear fuel mixtures are provided. Pseudo-binary actinide-M fuel mixtures form alloys and exhibit: body-centered cubic solid phases at low temperatures; high solidus temperatures; and/or minimal or no reaction or inter-diffusion with steel and other cladding materials. Methods described herein through metallurgical and thermodynamics advancements guide the selection of amounts of fuel mixture components by use of phase diagrams. Weight percentages for components of a metallic additive to an actinide fuel are selected in a solid phase region of an isothermal phase diagram taken at a temperature below an upper temperature limit for the resulting fuel mixture in reactor use. Fuel mixtures include uranium-molybdenum-tungsten, uranium-molybdenum-tantalum, molybdenum-titanium-zirconium, and uranium-molybdenum-titanium systems.

  13. 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)

  14. Actinides-lanthanides (neodymium) separation by electrolytic extraction in molten fluoride media; Separation actinides-lanthanides (neodyne) par extraction electrolytique en milieux fluorures fondus

    Energy Technology Data Exchange (ETDEWEB)

    Hamel, C

    2005-02-15

    The aim of this thesis is to assess the potentialities of pyrochemical processes for future nuclear fuels and Generation IV reactors (more particularly molten salt reactors). This study concerns the Actinides-Lanthanides and Lanthanides-Solvent separation by electrolytic extraction in molten fluoride media at high temperature. Three elements are selected for this study: neodymium (NdF{sub 3}), uranium (UF{sub 4}) and plutonium (PuF{sub 3}). Firstly, the electrochemical study of these three compounds in molten fluoride media is performed to evaluate the separations. Electrodeposition processes are studied and the values of formal potentials of U(III)/U(0), Pu(III)/Pu(0) and Nd(III)/Nd(0) are obtained in LiF-CaF{sub 2} eutectic mixture. Thermodynamically, the values of potentials differences are enough to separate U-Nd and Pu-Nd with a yield of extraction of 99.99%; this value is just sufficient for the Pu-Nd separation. Concerning the Nd-solvent separation this potential difference is too small. Next, the electrodeposition of solid metals on inert electrodes is performed. This study showed that the uranium and neodymium deposits are unstable in several fluoride media. In addition, the presence of salts in the dendritic metal is observed for the U solid deposits. Finally, a reactive cathode is used to improve these separation results and the shape of the deposits. The experimental results on nickel electrodes showed an improvement of the Pu-Nd separation and the Nd-solvent separation with the depolarization phenomenon of the metal deposit on the nickel. Moreover, U and Nd metal are stabilized in the alloy which allows the elimination of reactions with the solvent as observed for the solid deposit. The formation of liquids alloys makes also easier the recovery of these three. (author)

  15. Actinides-lanthanides (neodymium) separation by electrolytical extraction in molten fluoride media; Separation actinides-lanthanides (neodyne) par extraction electrolytique en milieux fluorures fondus

    Energy Technology Data Exchange (ETDEWEB)

    Hamel, C

    2005-02-15

    The aim of this thesis is to assess the potentialities of pyrochemical processes for futur nuclear fuels and Generation IV reactors (more particularly molten salt reactors). This study concerns the Actinides-Lanthanides and Lanthanides-Solvent separation by electrolytical extraction in molten fluoride media at high temperature. Three elements are selected for this study: neodymium (NdF{sub 3}), uranium (UF{sub 4}) and plutonium (PuF{sub 3}). Firstly, the electrochemical study of these three compounds in molten fluoride media is performed to evaluate the separations. Electrodeposition processes are studied and the values of formal potentials of U(III)/U(0), Pu(III)/Pu(0) and Nd(III)/Nd(0) are obtained in LiF-CaF{sub 2} eutectic mixture. Thermodynamically, the values of potentials differences are enough to separate U-Nd and Pu-Nd with a yield of extraction of 99.99%; this value is just sufficient for the Pu-Nd separation. Concerning the Nd-solvent separation this potential difference is too small. Next, the electrodeposition of solid metals on inert electrodes is performed. This study showed that the uranium and neodymium deposits are unstable in several fluoride media. In addition, the presence of salts in the dendritic metal is observed for the U solid deposits. Finally, a reactive cathode is used to improve these separation results and the shape of the deposits. The experimental results on nickel electrodes showed an improvement of the Pu-Nd separation and the Nd-solvent separation with the depolarisation phenomenon of the metal deposit on the nickel. Moreover, U and Nd metal are stabilized in the alloy which allows the elimination of reactions with the solvent as observed for the solid deposit. The formation of liquids alloys makes also easier the recovery of these three. (author)

  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. 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

  7. 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.

  8. 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.

  9. 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.

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

    Science.gov (United States)

    Goriely, S.; Arnould, M.

    2001-12-01

    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. This study is based on a version of the multi-event canonical model of the r-process which discards the largely used waiting point approximation. It considers also different combinations of models for the calculation of nuclear masses, beta -decay and fission rates. Two variants of the model used to predict nuclear reaction rates are adopted. In addition, the influence of the level of Pb and Bi production by the r-process on the estimated actinide production is evaluated by relying on the solar abundances of these two elements. In total, thirty-two different cases 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. This simplicity is imposed by our inability to identify the proper astrophysical sites for the r-process. As a guide to the practitioners, constraints on the actinide yield predictions and associated uncertainties are suggested on grounds of the measured abundances of r-nuclides, including Th and U, in the star CS 31082-001, and under the critical and questionable assumption of the ``universality'' of the r-process. We also define alternative constraints based on the nucleo-cosmochronological results derived from the present

  11. 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)

  12. 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

  13. Spectral properties of actinide materials: Charge density self-consistent LDA+Hubbard I method in FP-LAPW basis

    Energy Technology Data Exchange (ETDEWEB)

    Kolorenc, Jindrich [Institute of Physics ASCR, Prague (Czech Republic); University of Hamburg, Hamburg (Germany); Shick, Alexander B. [Institute of Physics ASCR, Prague (Czech Republic); Havela, Ladislav [Charles University, Prague (Czech Republic); Lichtenstein, Alexander I. [University of Hamburg, Hamburg (Germany)

    2010-07-01

    We provide a numerically efficient procedure to perform LDA+Hubbard I calculations including self-consistency over the charge density in the FP-LAPW basis. The method is applied to Pu, Am, and PuAm and PuCe alloys. Our results for valence photoemission spectra (PES) agree with experimental data and with previous LDA+DMFT calculations. Analysis of the J=5/2 and J=7/2 contributions to the f-occupation supports the intermediate-coupling picture of f-states in heavy actinides. The electronic specific heat coefficient is calculated for PuAm and PuCe alloys in reasonable agreement with recent experiments. We show that Pu atoms keep their mixed-valence character in these alloys. Next, we study electronic and spectral properties of Pu-based superconductor PuCoGa{sub 5} and obtain good agreement with experimental PES. Finally, we analyze surface effects. In Pu monolayer, we find substantial modification of PES due to 5f-electron localization consistent with experimental observations.

  14. 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.

  15. 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.

  16. 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.

  17. 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.

  18. 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.

  19. 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)

  20. 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.

  1. 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.

  2. 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

  3. 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.

  4. 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.

  5. 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.

  6. 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.

  7. 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.

  8. 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.

  9. 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)

  10. 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

  11. 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

  12. Study of thermodynamic properties of Np-Al alloys in molten LiCl-KCl eutectic

    Science.gov (United States)

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

    2009-10-01

    Pyrochemical methods are investigated worldwide within the framework of Partitioning and Transmutation concepts for spent nuclear fuel reprocessing. Electroseparation techniques in a molten LiCl-KCl are being developed in ITU to recover all actinides from a mixture with fission products. During the process, actinides are selectively electrochemically reduced on a solid aluminium cathode, forming solid actinide-aluminium alloys. This work is focused on the thermodynamic properties of Np-Al alloys in a temperature range of 400-550 °C and on the characterisation of the structure and chemical composition of deposits obtained by electrodeposition of Np on solid Al electrodes in a LiCl-KCl-NpCl 3 melt. Cyclic voltammetry and open circuit chronopotentiometry have been used to examine the electrochemical behaviour of Np on inert W and reactive Al electrodes. Gibbs energies, enthalpy and entropy of formation and standard electrode potentials of Np-Al alloys were evaluated and compared with ab initio calculations. Galvanostatic electrolyses at 450 °C were carried out to recover Np onto Al plates and the solid surface deposits were characterised by XRD and SEM-EDX analyses. Stable and dense deposits consisting of NpAl 3 and NpAl 4 alloys were identified. In addition, the conversion of NpO 2 to NpCl 3 is described, using chlorination of the oxide in a molten salt media by pure chlorine gas.

  13. 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

  14. 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

  15. 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)

  16. 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,

  17. 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

  18. 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.

  19. 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.

  20. 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.

  1. 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.

  2. 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....

  3. 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)

  4. 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.

  5. 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.

  6. 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.

  7. 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.

  8. 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.

  9. 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)

  10. 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.

  11. 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.

  12. 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.

  13. 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.

  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. 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

  16. 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.

  17. 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)

  18. 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

  19. 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.

  20. 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

  1. 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)

  2. 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.

  3. 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.)

  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. 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.

  8. 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.

  9. Aluminum alloy

    Science.gov (United States)

    Blackburn, Linda B. (Inventor); Starke, Edgar A., Jr. (Inventor)

    1989-01-01

    This invention relates to aluminum alloys, particularly to aluminum-copper-lithium alloys containing at least about 0.1 percent by weight of indium as an essential component, which are suitable for applications in aircraft and aerospace vehicles. At least about 0.1 percent by weight of indium is added as an essential component to an alloy which precipitates a T1 phase (Al2CuLi). This addition enhances the nucleation of the precipitate T1 phase, producing a microstructure which provides excellent strength as indicated by Rockwell hardness values and confirmed by standard tensile tests.

  10. 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.

  11. 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)

  12. 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.

  13. 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.

  14. 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)

  15. 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)

  16. 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.

  17. 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.

  18. 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.

  19. 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)

  20. Electrical Resistance Alloys and Low-Expansion Alloys

    DEFF Research Database (Denmark)

    Kjer, Torben

    1996-01-01

    The article gives an overview of electrical resistance alloys and alloys with low thermal expansion. The electrical resistance alloys comprise resistance alloys, heating alloys and thermostat alloys. The low expansion alloys comprise alloys with very low expansion coefficients, alloys with very low...

  1. 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

  2. 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.

  3. 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.)

  4. 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.

  5. 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.

  6. 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.

  7. 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.

  8. 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.

  9. 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)

  10. 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)

  11. 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

  12. 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.

  13. 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.

  14. 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.

  15. 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.

  16. 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.

  17. 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.

  18. 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)

  19. 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.

  20. 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.

  1. 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.

  2. 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...

  3. 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.

  4. 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.

  5. 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.)

  6. 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

  7. 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)

  8. 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.)

  9. 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...

  10. 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.

  11. 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.

  12. 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)

  13. Atomic Structure and Phase Transformations in Pu Alloys

    Energy Technology Data Exchange (ETDEWEB)

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

    2008-04-28

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

  14. THERMODYNAMICS AND KINETICS OF PHASE TRANSFORMATIONS IN PLUTONIUM ALLOYS - PART I

    Energy Technology Data Exchange (ETDEWEB)

    Turchi, P A; Kaufman, L; Liu, Z; Zhou, S

    2004-08-18

    In this report we investigate order, stability, and phase transformations for a series of actinide-based alloys. The statics and kinetics of precipitation and ordering in this class of alloys are modeled with a scheme that couples fundamental information on the alloy energetics obtained from experimental and assessed thermo-chemical data to the CALPHAD approach commonly used in industry for designing alloys with engineering specificity with the help of the Thermo-Calc software application. The CALPHAD approach is applied to the study of the equilibrium thermodynamic properties of Pu-based alloys, Pu-X, where X=Al, Fe, Ga. The assessment of the equilibrium phase diagrams in the whole range of alloy composition has been performed with the PARROT module of the Thermo-Calc application software. Predictions are made on the low temperature and Pu-rich side of the phase diagrams of Pu-Ga and Pu-Al for which controversy has been noted in the past. The validity of the assessed thermo-chemical database will be discussed by comparing predicted heats of transformation for pure Pu with measured values from differential scanning calorimetry analysis. An overall picture for the stability properties of Pu-Ga and Pu-Al that reconciles the results of past studies carried out on these alloys is proposed. Results on phase stability in the ternary Fe-Ga-Pu and Al-Fe-Pu alloys are discussed. The information collected in this study is then used to model metastability, long-term stability and aging for this class of alloys by coupling Thermo-Calc with DICTRA, a series of modules that allow the analysis of DIffusion Controlled TRAnsformations. Kinetics information is then summarized in so-called TTT (temperature-time-transformations) diagrams for the most relevant phases of actinide alloys. Specifically, results are presented on kinetics of phase transformations associated with the eutectoid-phase decomposition reaction occurring at low temperature, and with the martensitic transformation

  15. 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)

  16. 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.

  17. 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.

  18. 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.

  19. 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.

  20. 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,

  1. 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...

  2. 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.

  3. 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.

  4. 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)

  5. 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

  6. 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.

  7. 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.

  8. 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.

  9. 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.)

  10. 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.

  11. 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

  12. 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.

  13. 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...

  14. 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.)

  15. Electrodeposition of alloys or compounds in molten salts and applications

    Directory of Open Access Journals (Sweden)

    Taxil P.

    2003-01-01

    Full Text Available This article deals with the different modes of preparation of alloys or intermetallic compounds using the electrodeposition in molten salts, more particularly molten alkali fluorides. The interest in this process is to obtain new materials for high technology, particularly the compounds of reactive components such as actinides, rare earth and refractory metals. Two ways of preparation are considered: (i electrocoating of the more reactive metal on a cathode made of the noble one and reaction between the two metals in contact, and (ii electrocoating on an inert cathode of the intermetallic compound by coreduction of the ions of each elements. The kinetic is controlled by the reaction at the electrolyte interface. A wide bibliographic survey on the preparation of various compounds (intermetallic compounds, borides, carbides… is given and a special attention is paid to the own experience of the authors in the preparation of these compounds and interpretation of their results.

  16. Translating VDM to Alloy

    DEFF Research Database (Denmark)

    Lausdahl, Kenneth

    2013-01-01

    . Traditionally, theorem provers are used to prove that specifications are correct but this process is highly dependent on expert users. Alternatively, model finding has proved to be useful for validation of specifications. The Alloy Analyzer is an automated model finder for checking and visualising Alloy...... specifications. However, to take advantage of the automated analysis of Alloy, the model-oriented VDM specifications must be translated into a constraint-based Alloy specifications. We describe how a sub- set of VDM can be translated into Alloy and how assertions can be expressed in VDM and checked by the Alloy...

  17. 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.

  18. 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.

  19. 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.)

  20. 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

  1. 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)

  2. 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.

  3. 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.

  4. 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.

  5. 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.

  6. 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.

  7. 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)

  8. 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.

  9. 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.

  10. 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.

  11. 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.

  12. 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.

  13. 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.

  14. 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.

  15. 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.

  16. 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.

  17. 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)

  18. 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)

  19. 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%).

  20. 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.

  1. 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.

  2. 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.

  3. 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.

  4. 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.'

  5. 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)

  6. 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.

  7. 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.

  8. 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.

  9. 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)

  10. 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.

  11. 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.

  12. 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 ...

  13. 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.

  14. 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.

  15. 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)

  16. 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)

  17. Alloy Fabrication Laboratory

    Data.gov (United States)

    Federal Laboratory Consortium — At NETL’s Alloy Fabrication Facility in Albany, OR, researchers conduct DOE research projects to produce new alloys suited to a variety of applications, from gas...

  18. F-Alloy: An Alloy Based Model Transformation Language

    OpenAIRE

    Gammaitoni, Loïc; Kelsen, Pierre

    2015-01-01

    Model transformations are one of the core artifacts of a model-driven engineering approach. The relational logic language Alloy has been used in the past to verify properties of model transformations. In this paper we introduce the concept of functional Alloy modules. In essence a functional Alloy module can be viewed as an Alloy module representing a model transformation. We describe a sublanguage of Alloy called F-Alloy that allows the specification of functional Alloy modules. Module...

  19. PLUTONIUM-THORIUM ALLOYS

    Science.gov (United States)

    Schonfeld, F.W.

    1959-09-15

    New plutonium-base binary alloys useful as liquid reactor fuel are described. The alloys consist of 50 to 98 at.% thorium with the remainder plutonium. The stated advantages of these alloys over unalloyed plutonium for reactor fuel use are easy fabrication, phase stability, and the accompanying advantuge of providing a means for converting Th/sup 232/ into U/sup 233/.

  20. High strength alloys

    Energy Technology Data Exchange (ETDEWEB)

    Maziasz, Phillip James [Oak Ridge, TN; Shingledecker, John Paul [Knoxville, TN; Santella, Michael Leonard [Knoxville, TN; Schneibel, Joachim Hugo [Knoxville, TN; Sikka, Vinod Kumar [Oak Ridge, TN; Vinegar, Harold J [Bellaire, TX; John, Randy Carl [Houston, TX; Kim, Dong Sub [Sugar Land, TX

    2010-08-31

    High strength metal alloys are described herein. At least one composition of a metal alloy includes chromium, nickel, copper, manganese, silicon, niobium, tungsten and iron. System, methods, and heaters that include the high strength metal alloys are described herein. At least one heater system may include a canister at least partially made from material containing at least one of the metal alloys. At least one system for heating a subterranean formation may include a tubular that is at least partially made from a material containing at least one of the metal alloys.

  1. High strength alloys

    Science.gov (United States)

    Maziasz, Phillip James; Shingledecker, John Paul; Santella, Michael Leonard; Schneibel, Joachim Hugo; Sikka, Vinod Kumar; Vinegar, Harold J.; John, Randy Carl; Kim, Dong Sub

    2012-06-05

    High strength metal alloys are described herein. At least one composition of a metal alloy includes chromium, nickel, copper, manganese, silicon, niobium, tungsten and iron. System, methods, and heaters that include the high strength metal alloys are described herein. At least one heater system may include a canister at least partially made from material containing at least one of the metal alloys. At least one system for heating a subterranean formation may include a tublar that is at least partially made from a material containing at least one of the metal alloys.

  2. Creep Resistant Zinc Alloy

    Energy Technology Data Exchange (ETDEWEB)

    Frank E. Goodwin

    2002-12-31

    This report covers the development of Hot Chamber Die Castable Zinc Alloys with High Creep Strengths. This project commenced in 2000, with the primary objective of developing a hot chamber zinc die-casting alloy, capable of satisfactory service at 140 C. The core objectives of the development program were to: (1) fill in missing alloy data areas and develop a more complete empirical model of the influence of alloy composition on creep strength and other selected properties, and (2) based on the results from this model, examine promising alloy composition areas, for further development and for meeting the property combination targets, with the view to designing an optimized alloy composition. The target properties identified by ILZRO for an improved creep resistant zinc die-casting alloy were identified as follows: (1) temperature capability of 1470 C; (2) creep stress of 31 MPa (4500 psi); (3) exposure time of 1000 hours; and (4) maximum creep elongation under these conditions of 1%. The project was broadly divided into three tasks: (1) Task 1--General and Modeling, covering Experimental design of a first batch of alloys, alloy preparation and characterization. (2) Task 2--Refinement and Optimization, covering Experimental design of a second batch of alloys. (3) Task 3--Creep Testing and Technology transfer, covering the finalization of testing and the transfer of technology to the Zinc industry should have at least one improved alloy result from this work.

  3. Biocompatibility of dental alloys

    Energy Technology Data Exchange (ETDEWEB)

    Braemer, W. [Heraeus Kulzer GmbH and Co. KG, Hanau (Germany)

    2001-10-01

    Modern dental alloys have been used for 50 years to produce prosthetic dental restorations. Generally, the crowns and frames of a prosthesis are prepared in dental alloys, and then veneered by feldspar ceramics or composites. In use, the alloys are exposed to the corrosive influence of saliva and bacteria. Metallic dental materials can be classified as precious and non-precious alloys. Precious alloys consist of gold, platinum, and small amounts of non-precious components such as copper, tin, or zinc. The non-precious alloys are based on either nickel or cobalt, alloyed with chrome, molybdenum, manganese, etc. Titanium is used as Grade 2 quality for dental purposes. As well as the dental casting alloys, high purity electroplated gold (99.8 wt.-%) is used in dental technology. This review discusses the corrosion behavior of metallic dental materials with saliva in ''in vitro'' tests and the influence of alloy components on bacteria (Lactobacillus casei and Streptococcus mutans). The test results show that alloys with high gold content, cobalt-based alloys, titanium, and electroplated gold are suitable for use as dental materials. (orig.)

  4. 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.

  5. 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.

  6. 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.

  7. 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.

  8. 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

  9. 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.

  10. 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.

  11. 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.

  12. 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.

  13. 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.

  14. 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.

  15. 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.

  16. 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.

  17. 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.

  18. 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

  19. 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.

  20. 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.

  1. 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.

  2. 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

  3. 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.

  4. Catalyst Alloys Processing

    Science.gov (United States)

    Tan, Xincai

    2014-10-01

    Catalysts are one of the key materials used for diamond formation at high pressures. Several such catalyst products have been developed and applied in China and around the world. The catalyst alloy most widely used in China is Ni70Mn25Co5 developed at Changsha Research Institute of Mining and Metallurgy. In this article, detailed techniques for manufacturing such a typical catalyst alloy will be reviewed. The characteristics of the alloy will be described. Detailed processing of the alloy will be presented, including remelting and casting, hot rolling, annealing, surface treatment, cold rolling, blanking, finishing, packaging, and waste treatment. An example use of the catalyst alloy will also be given. Industrial experience shows that for the catalyst alloy products, a vacuum induction remelt furnace can be used for remelting, a metal mold can be used for casting, hot and cold rolling can be used for forming, and acid pickling can be used for metal surface cleaning.

  5. 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.

  6. PLUTONIUM-ZIRCONIUM ALLOYS

    Science.gov (United States)

    Schonfeld, F.W.; Waber, J.T.

    1960-08-30

    A series of nuclear reactor fuel alloys consisting of from about 5 to about 50 at.% zirconium (or higher zirconium alloys such as Zircaloy), balance plutonium, and having the structural composition of a plutonium are described. Zirconium is a satisfactory diluent because it alloys readily with plutonium and has desirable nuclear properties. Additional advantages are corrosion resistance, excellent fabrication propenties, an isotropie structure, and initial softness.

  7. NICKEL-BASE ALLOY

    Science.gov (United States)

    Inouye, H.; Manly, W.D.; Roche, T.K.

    1960-01-19

    A nickel-base alloy was developed which is particularly useful for the containment of molten fluoride salts in reactors. The alloy is resistant to both salt corrosion and oxidation and may be used at temperatures as high as 1800 deg F. Basically, the alloy consists of 15 to 22 wt.% molybdenum, a small amount of carbon, and 6 to 8 wt.% chromium, the balance being nickel. Up to 4 wt.% of tungsten, tantalum, vanadium, or niobium may be added to strengthen the alloy.

  8. 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.

  9. 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.

  10. 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.

  11. 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.

  12. 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...

  13. 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.

  14. 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.

  15. 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)

  16. 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.

  17. Multi-dimensional constraint relativistic mean field model and applications in actinide and transfermium nuclei

    CERN Document Server

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

    2013-01-01

    In this contribution we present some results of potential energy surfaces of actinide and transfermium nuclei from multi-dimensional constrained relativistic mean field (MDC-RMF) models. Recently we developed multi-dimensional constrained covariant density functional theories (MDC-CDFT) in which all shape degrees of freedom $\\beta_{\\lambda\\mu}$ with even $\\mu$ are allowed and the functional can be one of the following four forms: the meson exchange or point-coupling nucleon interactions combined with the non-linear or density-dependent couplings. In MDC-RMF models, the pairing correlations are treated with the BCS method. With MDC-RMF models, the potential energy surfaces of even-even actinide nuclei were investigated and the effect of triaxiality on the fission barriers in these nuclei was discussed. The non-axial reflection-asymmetric $\\beta_{32}$ shape in some transfermium nuclei with $N=150$, namely $^{246}$Cm, $^{248}$Cf, $^{250}$Fm, and $^{252}$No were also studied.

  18. A comparative study of actinide complexation in three ligand systems with increasing complexity

    Science.gov (United States)

    Jeanson, A.; Dahou, S.; Guillaumont, D.; Moisy, P.; Den Auwer, C.; Scheinost, A.; Hennig, C.; Vidaud, C.; Subra, G.; Solari, P. L.

    2009-11-01

    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 LIII 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. Developing an in-situ Detector of Neutron-Induced Fission for Actinide Sputtering Characterization

    Science.gov (United States)

    Fellers, Deion

    2016-09-01

    The physical mechanism describing the transfer of large amounts of energy due to fission in a material is not well understood and represents one of the modern challenges facing nuclear scientists, with applications including nuclear energy and national defense. Fission fragments cause damage to the material from sputtering of matter as they pass through or near the material's surface. We have developed a new technique at the Los Alamos Neutron Science Center for characterizing the ejecta by using ultracold neutrons (neutrons with kinetic energy less than 300 neV) to induce fission at finely controlled depths in an actinide. This program will ultimately provide a detailed description of the properties of the sputtered particles as a function of the depth of the fission in the material. A key component of this project is accurately quantifying the number of neutron induced fissions in the sample. This poster depicts the development of an in-situ detector of neutron-induced fission for the AShES (Actinide Sputtering from ultracold neutron Exposure at the Surface) experiment.

  20. Leaching of actinides and technetium from simulated high-level waste glass

    Energy Technology Data Exchange (ETDEWEB)

    Bradley, D.J.; Harvey, C.O.; Turcotte, R.P.

    1979-08-01

    Leach tests were conducted using a modified version of the IAEA procedure to study the behavior of glass waste-solution interactions. Release rates were determined for Tc, U, Np, Pu, Am, Cm, and Si in the following solutions: WIPP B salt brine, NaCl (287 g/l), NaCl (1.76 g/1), CaCl/sub 2/ (1.66 g/l), NaHCO/sub 3/ (2.52 g/l), and deionized water. The leach rates for all elements decreased an order of magnitude from their initial values during the first 20 to 30 days leaching time. The sodium bicarbonate solution produced the highest elemental release rates, while the saturated salt brine and deionized water in general gave the lowest release. Technetium has the highest initial release of all elements studied. The technetium release rates, however, decreased by over four orders of magnitude in 150 days of leaching time. In the prepared glass, technetium was phase separated, concentrating on internal pore surfaces. Neptunium, in all cases except CaCl/sub 2/ solution, shows the highest actinide release rate. In general, curium and uranium have the lowest release rates. The range of actinide release rates is from 10/sup -5/ to 10/sup -8/ g/cm/sup 2//day. 25 figures, 7 tables.

  1. Plutonium and Minor Actinides Recycling in Standard BWR using Equilibrium Burnup Model

    Directory of Open Access Journals (Sweden)

    Abdul Waris

    2008-03-01

    Full Text Available Plutonium (Pu and minor actinides (MA recycling in standard BWR with equilibrium burnup model has been studied. We considered the equilibrium burnup model as a simple time independent burnup method, which can manage all possible produced nuclides in any nuclear system. The equilibrium burnup code was bundled with a SRAC cell-calculation code to become a coupled cell-burnup calculation code system. The results show that the uranium enrichment for the criticality of the reactor, the amount of loaded fuel and the required natural uranium supply per year decrease for the Pu recycling and even much lower for the Pu & MA recycling case compared to those of the standard once-through BWR case. The neutron spectra become harder with the increasing number of recycled heavy nuclides in the reactor core. The total fissile rises from 4.77% of the total nuclides number density in the reactor core for the standard once-through BWR case to 6.64% and 6.72% for the Plutonium recycling case and the Pu & MA recycling case, respectively. The two later data may become the main basis why the required uranium enrichment declines and consequently diminishes the annual loaded fuel and the required natural uranium supply. All these facts demonstrate the advantage of plutonium and minor actinides recycling in BWR.

  2. 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)

    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. This project is one half of my laboratory’s DOE research which was split 50:50 between Catalysis and Heavy Element Chemistry programs in 2010. Hence, this report is for a half-project.

  3. Conceptual design of minor actinides burner with an accelerator-driven subcritical system.

    Energy Technology Data Exchange (ETDEWEB)

    Cao, Y.; Gohar, Y. (Nuclear Engineering Division)

    2011-11-04

    In the environmental impact study of the Yucca Mountain nuclear waste repository, the limit of spent nuclear fuel (SNF) for disposal is assessed at 70,000 metric tons of heavy metal (MTHM), among which 63,000 MTHM are the projected SNF discharge from U.S. commercial nuclear power plants though 2011. Within the 70,000 MTHM of SNF in storage, approximately 115 tons would be minor actinides (MAs) and 585 tons would be plutonium. This study describes the conceptual design of an accelerator-driven subcritical (ADS) system intended to utilize (burn) the 115 tons of MAs. The ADS system consists of a subcritical fission blanket where the MAs fuel will be burned, a spallation neutron source to drive the fission blanket, and a radiation shield to reduce the radiation dose to an acceptable level. The spallation neutrons are generated from the interaction of a 1 GeV proton beam with a lead-bismuth eutectic (LBE) or liquid lead target. In this concept, the fission blanket consists of a liquid mobile fuel and the fuel carrier can be LBE, liquid lead, or molten salt. The actinide fuel materials are dissolved, mixed, or suspended in the liquid fuel carrier. Therefore, fresh fuel can be fed into the fission blanket to adjust its reactivity and to control system power during operation. Monte Carlo analyses were performed to determine the overall parameters of an ADS system utilizing LBE as an example. Steady-state Monte Carlo simulations were studied for three fission blanket configurations that are similar except that the loaded amount of actinide fuel in the LBE is either 5, 7, or 10% of the total volume of the blanket, respectively. The neutron multiplication factor values of the three configurations are all approximately 0.98 and the MA initial inventories are each approximately 10 tons. Monte Carlo burnup simulations using the MCB5 code were performed to analyze the performance of the three conceptual ADS systems. Preliminary burnup analysis shows that all three conceptual ADS

  4. Predictions of Actinide Solubilities under Near-Field Conditions Expected in the WIPP

    Science.gov (United States)

    Brush, L. H.; Xiong, Y.

    2009-12-01

    The Waste Isolation Pilot Plant (WIPP) is a U.S. Department of Energy (DOE) repository in southeast New Mexico for defense-related transuranic (TRU) waste. The repository, which opened in March 1999, is located at a subsurface depth of 655 m (2150 ft) in the Salado Fm., a Permian bedded-salt formation. The repository will eventually contain the equivalent of 844,000 208 L (55 gal) drums of TRU waste. After filling the rooms and access drifts and installing panel closures, creep closure of the salt will crush the steel waste containers in most cases and encapsulate the waste. The WIPP actinide source term model used for long-term performance assessment (PA) of the repository comprises dissolved and suspended submodels (solubilities and colloids). This presentation will describe the solubilities. From the standpoint of long-term PA, the order of importance of the radioelements in the TRU waste to be emplaced in the WIPP is Pu ~ Am >> U > Th >> Np ~ Cm and fission products. The DOE has included all of these actinides, but not fission products, in the WIPP Actinide Source Term Program (ASTP). Anoxic corrosion of Fe- and Al-base metals and microbial consumption of cellulosic, plastic, and rubber materials will produce gas and create strongly reducing conditions in the WIPP after closure. The use of MgO as an engineered barrier to consume microbially produced CO2 will result in low fCO2 and basic pH. Under these conditions, Th, U, Np, Pu, and Am will speciate essentially entirely as Th(IV), U(IV), Np(IV), Pu(III), and Am(III); or Th(IV), U(VI), Np(V), Pu(IV), and Am(III). The DOE has developed thermodynamic speciation-and-solubility models for +III, +IV, and +V actinides in brines. Experimental data for Nd, Am, and Cm species were used to parameterize the +III Pitzer activity-coefficient model; data for Th species were used for the +IV model; and data for Np(V) species were used for the +V model. These models include the effects of the organic ligands acetate, citrate

  5. Ductile transplutonium metal alloys

    Science.gov (United States)

    Conner, William V.

    1983-01-01

    Alloys of Ce with transplutonium metals such as Am, Cm, Bk and Cf have properties making them highly suitable as sources of the transplutonium element, e.g., for use in radiation detector technology or as radiation sources. The alloys are ductile, homogeneous, easy to prepare and have a fairly high density.

  6. Revisiting the melting temperature of NpO2 and the challenges associated with high temperature actinide compound measurements

    NARCIS (Netherlands)

    Böhler, R.; Welland, M.J.; De Bruycker, F.; Boboridis, K.; Janssen, A.; Eloirdi, R.; Konings, R.J.M.; Manara, D.

    2012-01-01

    This work revisits the melting behaviour of neptunium dioxide, an actinide compound which can be produced in the nuclear fuel during operation, and which has an important impact on the nuclear fuel and waste radioactivity especially on the very long term. The present experimental approach employs re

  7. 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.

  8. 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.

  9. DEVELOPMENT OF PROTOTYPE TITANATE ION EXCHANGE LOADED MEMBRANES FOR STRONTIUM, CESIUM AND ACTINIDE DECONTAMINATION FROM AQUEOUS MEDIA

    Energy Technology Data Exchange (ETDEWEB)

    Oji, L; Keisha Martin, K; David Hobbs, D

    2008-05-30

    We have successfully incorporated high surface area particles of titanate ion exchange materials (monosodium titanate and crystalline silicotitanate) with acceptable particle size distribution into porous and inert support membrane fibrils consisting of polytetrafluoroethylene (Teflon{reg_sign}), polyethylene and cellulose materials. The resulting membrane sheets, under laboratory conditions, were used to evaluate the removal of surrogate radioactive materials for cesium-137 and strontium-90 from high caustic nuclear waste simulants. These membrane supports met the nominal requirement for nonchemical interaction with the embedded ion exchange materials and were porous enough to allow sufficient liquid flow. Some of this 47-mm size stamped out prototype titanium impregnated ion exchange membrane discs was found to remove more than 96% of dissolved cesium-133 and strontium-88 from a caustic nuclear waste salt simulants. Since in traditional ion exchange based column technology monosodium titanate (MST) is known to have great affinity for the sorbing of other actinides like plutonium, neptunium and even uranium, we expect that the MST-based membranes developed here, although not directly evaluated for uptake of these three actinides because of costs associated with working with actinides which do not have 'true' experimental surrogates, would also show significant affinity for these actinides in aqueous media. It was also observed that crystalline silicotitanate impregnated polytetrafluoroethylene or polyethylene membranes became less selective and sorbed both cesium and strontium from the caustic aqueous salt simulants.

  10. Actinide Corroles: Synthesis and Characterization of Thorium(IV) and Uranium(IV) bis(-chloride) Dimers

    Energy Technology Data Exchange (ETDEWEB)

    Ward, Ashleigh L.; Buckley, Heather L.; Gryko, Daniel T.; Lukens, Wayne W.; Arnold, John

    2013-12-01

    The first synthesis and structural characterization of actinide corroles is presented. Thorium(IV) and uranium(IV) macrocycles of Mes2(p-OMePh)corrole were synthesised and characterized by single-crystal X-ray diffraction, UV-Visible spectroscopy, variable-temperature 1H NMR, ESI mass spectrometry and cyclic voltammetry.

  11. Ultrahigh temperature intermetallic alloys

    Energy Technology Data Exchange (ETDEWEB)

    Brady, M.P.; Zhu, J.H.; Liu, C.T.; Tortorelli, P.F.; Wright, J.L.; Carmichael, C.A.; Walker, L.R. [Oak Ridge National Lab., TN (United States). Metals and Ceramics Div.

    1997-12-01

    A new family of Cr-Cr{sub 2}X based alloys with fabricability, mechanical properties, and oxidation resistance superior to previously developed Cr-Cr{sub 2}Nb and Cr-Cr{sub 2}Zr based alloys has been identified. The new alloys can be arc-melted/cast without cracking, and exhibit excellent room temperature and high-temperature tensile strengths. Preliminary evaluation of oxidation behavior at 1100 C in air indicates that the new Cr-Cr{sub 2}X based alloys form an adherent chromia-based scale. Under similar conditions, Cr-Cr{sub 2}Nb and Cr-Cr{sub 2}Zr based alloys suffer from extensive scale spallation.

  12. New density functional theory approaches for enabling prediction of chemical and physical properties of plutonium and other actinides.

    Energy Technology Data Exchange (ETDEWEB)

    Mattsson, Ann Elisabet

    2012-01-01

    Density Functional Theory (DFT) based Equation of State (EOS) construction is a prominent part of Sandia's capabilities to support engineering sciences. This capability is based on amending experimental data with information gained from computational investigations, in parts of the phase space where experimental data is hard, dangerous, or expensive to obtain. A prominent materials area where such computational investigations are hard to perform today because of limited accuracy is actinide and lanthanide materials. The Science of Extreme Environment Lab Directed Research and Development project described in this Report has had the aim to cure this accuracy problem. We have focused on the two major factors which would allow for accurate computational investigations of actinide and lanthanide materials: (1) The fully relativistic treatment needed for materials containing heavy atoms, and (2) the needed improved performance of DFT exchange-correlation functionals. We have implemented a fully relativistic treatment based on the Dirac Equation into the LANL code RSPt and we have shown that such a treatment is imperative when calculating properties of materials containing actinides and/or lanthanides. The present standard treatment that only includes some of the relativistic terms is not accurate enough and can even give misleading results. Compared to calculations previously considered state of the art, the Dirac treatment gives a substantial change in equilibrium volume predictions for materials with large spin-orbit coupling. For actinide and lanthanide materials, a Dirac treatment is thus a fundamental requirement in any computational investigation, including those for DFT-based EOS construction. For a full capability, a DFT functional capable of describing strongly correlated systems such as actinide materials need to be developed. Using the previously successful subsystem functional scheme developed by Mattsson et.al., we have created such a functional. In

  13. 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

  14. Mg based alloys obtained by mechanical alloying

    Energy Technology Data Exchange (ETDEWEB)

    Ordonez, S. [Univ. de Santiago de Chile (Chile). Fac. de Ingenieria; Garcia, G.; Serafini, D.; San Martin, A.

    1999-07-01

    In the present work, we studied the production of magnesium alloys, of stoichiometry 2Mg + Ni, by mechanical alloying (MA) and the behavior of the alloys under hydrogen in a Sievert`s type apparatus. The elemental powders were milled under argon atmosphere in a Spex 8000 high energy ball mill. The milled materials were characterized by X-ray diffraction (XRD) and scanning electron microscopy (SEM). Only minimum amounts of the Mg{sub 2}Ni intermetallic compound was obtained after 22 h of milling time. Most of the material was sticked to the inner surface of the container as well as to the milling balls. Powders milled only for 12 hours transforms to the intermetallic at around 433 K. Effects of the MA on the hydrogen absorption kinetics were also studied. (orig.) 10 refs.

  15. DISTRIBUTION OF ACTINIDES BETWEEN THE AQUEOUS AND ORGANIC PHASES IN THE TALSPEAK PROCESS

    Energy Technology Data Exchange (ETDEWEB)

    Rudisill, T.; Kyser, E.

    2010-09-02

    One objective of the US Department of Energy's Office of Nuclear Energy (DOE-NE) is the development of sustainable nuclear fuel cycles which improve uranium resource utilization, maximize energy generation, minimize waste generation, improve safety, and complement institutional measures limiting proliferation risks. Activities in progress which support this objective include the development of advanced separation technologies to recover the actinides from used nuclear fuels. With the increased interest in the development of technology to allow closure of the nuclear fuel cycle, the TALSPEAK process is being considered for the separation of Am and Cm from the lanthanide fission products in a next generation reprocessing plant. However, at this time, the level of understanding associated with the chemistry and the control of the process variables is not acceptable for deployment of the process on an industrial scale. To address this issue, DOE-NE is supporting basic scientific studies focused on the TALSPEAK process through its Fuel Cycle Research and Development (R&D) program. One aspect of these studies is an experimental program at the Savannah River National Laboratory (SRNL) in which temperature-dependent distribution coefficients for the extraction of actinide elements in the TALSPEAK process were measured. The data were subsequently used to calculate conditional enthalpies and entropies of extraction by van't Hoff analysis to better understand the thermodynamic driving forces for the TALSPEAK process. In the SRNL studies, the distribution of Pu(III) in the TALSPEAK process was of particular interest. A small amount of Pu(III) would be present in the feed due to process losses and valence adjustment in prior recovery operations. Actinide elements such as Np and Pu have multiple stable oxidation states in aqueous solutions; therefore the oxidation state for these elements must be controlled in the TALSPEAK process, as the extraction chemistry is

  16. LIBS Spectral Data for a Mixed Actinide Fuel Pellet Containing Uranium, Plutonium, Neptunium and Americium

    Energy Technology Data Exchange (ETDEWEB)

    Judge, Elizabeth J. [Los Alamos National Laboratory; Berg, John M. [Los Alamos National Laboratory; Le, Loan A. [Los Alamos National Laboratory; Lopez, Leon N. [Los Alamos National Laboratory; Barefield, James E. [Los Alamos National Laboratory

    2012-06-18

    Laser-induced breakdown spectroscopy (LIBS) was used to analyze a mixed actinide fuel pellet containing 75% UO{sub 2}/20% PuO{sub 2}/3% AmO{sub 2}/2% NpO{sub 2}. The preliminary data shown here is the first report of LIBS analysis of a mixed actinide fuel pellet, to the authors knowledge. The LIBS spectral data was acquired in a plutonium facility at Los Alamos National Laboratory where the sample was contained within a glove box. The initial installation of the glove box was not intended for complete ultraviolet (UV), visible (VIS) and near infrared (NIR) transmission, therefore the LIBS spectrum is truncated in the UV and NIR regions due to the optical transmission of the window port and filters that were installed. The optical collection of the emission from the LIBS plasma will be optimized in the future. However, the preliminary LIBS data acquired is worth reporting due to the uniqueness of the sample and spectral data. The analysis of several actinides in the presence of each other is an important feature of this analysis since traditional methods must chemically separate uranium, plutonium, neptunium, and americium prior to analysis. Due to the historic nature of the sample fuel pellet analyzed, the provided sample composition of 75% UO{sub 2}/20% PuO{sub 2}/3% AmO{sub 2}/2% NpO{sub 2} cannot be confirm without further analytical processing. Uranium, plutonium, and americium emission lines were abundant and easily assigned while neptunium was more difficult to identify. There may be several reasons for this observation, other than knowing the exact sample composition of the fuel pellet. First, the atomic emission wavelength resources for neptunium are limited and such techniques as hollow cathode discharge lamp have different dynamics than the plasma used in LIBS which results in different emission spectra. Secondly, due to the complex sample of four actinide elements, which all have very dense electronic energy levels, there may be reactions and

  17. The interaction of human serum albumin with selected lanthanide and actinide ions: Binding affinities, protein unfolding and conformational changes.

    Science.gov (United States)

    Ali, Manjoor; Kumar, Amit; Kumar, Mukesh; Pandey, Badri N

    2016-04-01

    Human serum albumin (HSA), the most abundant soluble protein in blood plays critical roles in transportation of biomolecules and maintenance of osmotic pressure. In view of increasing applications of lanthanides- and actinides-based materials in nuclear energy, space, industries and medical applications, the risk of exposure with these metal ions is a growing concern for human health. In present study, binding interaction of actinides/lanthanides [thorium: Th(IV), uranium: U(VI), lanthanum: La(III), cerium: Ce(III) and (IV)] with HSA and its structural consequences have been investigated. Ultraviolet-visible, Fourier transform-infrared, Raman, Fluorescence and Circular dichroism spectroscopic techniques were applied to study the site of metal ions interaction, binding affinity determination and the effect of metal ions on protein unfolding and HSA conformation. Results showed that these metal ions interacted with carbonyl (CO..:)/amide(N..-H) groups and induced exposure of aromatic residues of HSA. The fluorescence analysis indicated that the actinide binding altered the microenvironment around Trp214 in the subdomain IIA. Binding affinity of U(VI) to HSA was slightly higher than that of Th(IV). Actinides and Ce(IV) altered the secondary conformation of HSA with a significant decrease of α-helix and an increase of β-sheet, turn and random coil structures, indicating a partial unfolding of HSA. A correlation was observed between metal ion's ability to alter HSA conformation and protein unfolding. Both cationic effects and coordination ability of metal ions seemed to determine the consequences of their interaction with HSA. Present study improves our understanding about the protein interaction of these heavy ions and their impact on its secondary structure. In addition, binding characteristics may have important implications for the development of rational antidote for the medical management of health effects of actinides and lanthanides.

  18. Criticality investigations for the fixed bed nuclear reactor using thorium fuel mixed with plutonium or minor actinides

    Energy Technology Data Exchange (ETDEWEB)

    Sahin, Suemer [Beykoz Lojistik Meslek Yueksekokulu, Beykoz, Istanbul (Turkey)], E-mail: sumer@gazi.edu.tr; Sahin, Haci Mehmet; Acir, Adem [Beykoz Lojistik Meslek Yueksekokulu, Istanbul (Turkey); Al-Kusayer, Tawfik Ahmed [King Saud University, College of Engineering, P.O. Box 800, Riyadh 11421 (Saudi Arabia)

    2009-08-15

    Prospective fuels for a new reactor type, the so called fixed bed nuclear reactor (FBNR) are investigated with respect to reactor criticality. These are (1) low enriched uranium (LEU); (2) weapon grade plutonium + ThO{sub 2}; (3) reactor grade plutonium + ThO{sub 2}; and (4) minor actinides in the spent fuel of light water reactors (LWRs) + ThO{sub 2}. Reactor grade plutonium and minor actinides are considered as highly radio-active and radio-toxic nuclear waste products so that one can expect that they will have negative fuel costs. The criticality calculations are conducted with SCALE5.1 using S{sub 8}-P{sub 3} approximation in 238 neutron energy groups with 90 groups in thermal energy region. The study has shown that the reactor criticality has lower values with uranium fuel and increases passing to minor actinides, reactor grade plutonium and weapon grade plutonium. Using LEU, an enrichment grade of 9% has resulted with k{sub eff} = 1.2744. Mixed fuel with weapon grade plutonium made of 20% PuO{sub 2} + 80% ThO{sub 2} yields k{sub eff} = 1.2864. Whereas a mixed fuel with reactor grade plutonium made of 35% PuO{sub 2} + 65% ThO{sub 2} brings it to k{sub eff} = 1.267. Even the very hazardous nuclear waste of LWRs, namely minor actinides turn out to be high quality nuclear fuel due to the excellent neutron economy of FBNR. A relatively high reactor criticality of k{sub eff} = 1.2673 is achieved by 50% MAO{sub 2} + 50% ThO{sub 2}. The hazardous actinide nuclear waste products can be transmuted and utilized as fuel in situ. A further output of the study is the possibility of using thorium as breeding material in combination with these new alternative fuels.

  19. Selective extraction of actinides by calixarenes: application to bioassay analysis; Extraction selective des actinides par les calixarenes: application a l'analyse radiotoxicologique

    Energy Technology Data Exchange (ETDEWEB)

    Boulet, B

    2006-01-15

    In the context of nuclear workers monitoring, the aim of this PhD was to selectively isolate U, Pu, and Am from urine to propose a new analytical procedure to the Medical and Biology Analysis Laboratories. The 1,3,5-OCH{sub 3}-2,4,6-OCH{sub 2}CONHOH-p-tert-butyl-calix[6]arene molecule has been selected as a promising extractant for U, Pu, and Am. Its physico-chemical properties and its affinity for UO{sub 2}{sup 2+} have been studied through two approaches, one theoretical (molecular modelling at DFT level), and one experimental. The extractions of the three actinides by the hydroxamic calix[6]arene were quantitative in liquid-liquid and solid-liquid systems. Their separation has also been shown possible and efficient. After optimization, the proposed procedure should allow the laboratories to carry out the chemical treatment of urine, before the measurement, in one day instead of the three days needed nowadays. (author)

  20. 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

  1. 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

  2. TUNGSTEN BASE ALLOYS

    Science.gov (United States)

    Schell, D.H.; Sheinberg, H.

    1959-12-15

    A high-density quaternary tungsten-base alloy having high mechanical strength and good machinability composed of about 2 wt.% Ni, 3 wt.% Cu, 5 wt.% Pb, and 90wt.% W is described. This alloy can be formed by the powder metallurgy technique of hot pressing in a graphite die without causing a reaction between charge and the die and without formation of a carbide case on the final compact, thereby enabling re-use of the graphite die. The alloy is formable at hot- pressing temperatures of from about 1200 to about 1350 deg C. In addition, there is little component shrinkage, thereby eliminating the necessity of subsequent extensive surface machining.

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

    CERN Document Server

    Garza, Alejandro J; Scuseria, Gustavo E

    2015-01-01

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

  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; 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.

  5. Strategic Design and Optimization of Inorganic Sorbents for Cesium, Strontium and Actinides

    Energy Technology Data Exchange (ETDEWEB)

    Edward J. Maginn

    2009-11-09

    The primary objective of the Notre Dame component of the project was computational in nature. The goal was to provide a design tool for the synthesis of optimized sorbents for the removal of cesium, strontium and actinides from nuclear waste solutions. Molecular modeling enables us to observe and better understand the molecular level interactions that govern the selectivity of specific radionuclides in a particular sorbent. The research focused on the development and validation of a suitable and transferable model for all the cations and ion exchangers of interest, nd then subsequent simulations which determined the siting and mobility of water and cations. Speciic accomplishments include: (1) improving existing intermolecular force fields to accurately model the sorbents of interest; (2) utilizing energy-minimizations and molecular dynamics simulations for structural prediction of CST and niobium-substituted CST materials; (3) determining Na+/water positions in polyoxoniobate materials using molecular dynamics simulations; and (4) developing Hybrid Monte Carlo methods for improved structural prediction.

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

    Energy Technology Data Exchange (ETDEWEB)

    Greenspan, Ehud; Todreas, Neil; Taiwo, Temitope

    2009-03-10

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

  7. 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.

  8. A practical fabrication method for the advanced heterogeneous fuel with magnesia containing minor actinides

    Energy Technology Data Exchange (ETDEWEB)

    Miwa, Shuhei [Oarai Research and Development Center, Japan Atomic Energy Agency, 4002 Narita-cho, Oarai-machi, Higashi-ibaraki-gun, Ibaraki 311-1393 (Japan)], E-mail: miwa.shuhei@jaea.go.jp; Osaka, Masahiko [Oarai Research and Development Center, Japan Atomic Energy Agency, 4002 Narita-cho, Oarai-machi, Higashi-ibaraki-gun, Ibaraki 311-1393 (Japan)

    2009-03-15

    Fabrication tests on advanced heterogeneous fuel with MgO were carried out for the purpose of establishing a practical fabrication method. Advanced heterogeneous fuel consists of spheres (diameter greater than 100 {mu}m) of a minor actinide oxide and MgO inert matrix (macro-dispersed type fuel). Macro-dispersed type fuel pellets with a high density above 90% T.D. were successfully fabricated. In addition, the fabricated pellets showed a homogeneous dispersion of near spherical host phase granules. These were attained by optimization of the fabrication process and conditions; i.e. a preliminary heat treatment of raw powders of host phase, an adjustment of pressure at the granulation process, deployment of a spray-dry process for MgO sphere preparation and sintering in a He atmosphere. From these results, a practical fabrication method for MgO-based macro-dispersed type fuel based on a simple powder metallurgical technique was established.

  9. TAILORING INORGANIC SORBENTS FOR SRS STRONTIUM AND ACTINIDE SEPARATIONS: OPTIMIZED MONOSODIUM TITANATE PHASE II FINAL REPORT

    Energy Technology Data Exchange (ETDEWEB)

    Hobbs, D; Thomas Peters, T; Michael Poirier, M; Mark Barnes, M; Major Thompson, M; Samuel Fink, S

    2007-06-29

    This document provides a final report of Phase II testing activities for the development of a modified monosodium titanate (MST) that exhibits improved strontium and actinide removal characteristics compared to the baseline MST material. The activities included determining the key synthesis conditions for preparation of the modified MST, preparation of the modified MST at a larger scale by a commercial vendor, demonstration of the strontium and actinide removal characteristics with actual tank waste supernate and measurement of filtration characteristics. Key findings and conclusions include the following. Testing evaluated three synthetic methods and eleven process parameters for the optimum synthesis conditions for the preparation on an improved form of MST. We selected the post synthesis method (Method 3) for continued development based on overall sorbate removal performance. We successfully prepared three batches of the modified MST using Method 3 procedure at a 25-gram scale. The laboratory prepared modified MST exhibited increased sorption kinetics with simulated and actual waste solutions and similar filtration characteristics to the baseline MST. Characterization of the modified MST indicated that the post synthesis treatment did not significantly alter the particle size distribution, but did significantly increase the surface area and porosity compared to the original MST. Testing indicated that the modified MST exhibits reduced affinity for uranium compared to the baseline MST, reducing risk of fissile loading. Shelf-life testing indicated no change in strontium and actinide performance removal after storing the modified MST for 12-months at ambient laboratory temperature. The material releases oxygen during the synthesis and continues to offgas after the synthesis at a rapidly diminishing rate until below a measurable rate after 4 months. Optima Chemical Group LLC prepared a 15-kilogram batch of the modified MST using the post synthesis procedure (Method

  10. CHARACTERIZATION OF MODIFIED MONOSODIUM TITANATE - AN IMPROVED SORBENT FOR STRONTIUM AND ACTINIDE SEPARATIONS

    Energy Technology Data Exchange (ETDEWEB)

    Hobbs, D.; Taylor-Pashow, K.; Missimer, D.

    2010-12-21

    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. An inorganic sorbent, monosodium titanate (MST), is currently used to remove {sup 90}Sr and alpha-emitting radionuclides, while a caustic-side solvent extraction process is used for removing {sup 134,137}Cs. A new peroxotitanate material, modified MST, or mMST, has recently been developed and has shown increased removal kinetics and capacity for {sup 90}Sr and alpha-emitting radionuclides compared to the current baseline material, MST. This paper describes recent results focused on further characterization of this material.

  11. Low-temperature synthesis of actinide tetraborides by solid-state metathesis reactions

    Science.gov (United States)

    Lupinetti, Anthony J.; Garcia, Eduardo; Abney, Kent D.

    2004-12-14

    The synthesis of actinide tetraborides including uranium tetraboride (UB.sub.4), plutonium tetraboride (PuB.sub.4) and thorium tetraboride (ThB.sub.4) by a solid-state metathesis reaction are demonstrated. The present method significantly lowers the temperature required to .ltoreq.850.degree. C. As an example, when UCl.sub.4 is reacted with an excess of MgB.sub.2, at 850.degree. C., crystalline UB.sub.4 is formed. Powder X-ray diffraction and ICP-AES data support the reduction of UCl.sub.3 as the initial step in the reaction. The UB.sub.4 product is purified by washing water and drying.

  12. Chromatographic generator systems for the actinides and natural decay series elements

    Energy Technology Data Exchange (ETDEWEB)

    McAlister, D.R.; Horwitz, E.P. [PG Research Foundation, Lisle, IL (United States)

    2011-07-01

    This work describes chromatographic radionuclide generator systems for the production of actinides and natural decay series elements. The generator systems begin with alpha emitting parent radioisotopes with half-lives (T{sub 1/2}) of greater than one year and produce alpha or beta emitting radioisotopes with half-lives of hours to days. Chromatographic systems were chosen to minimize radiolytic damage to chromatographic supports, preserve the parent activity for repeated use, provide high purity daughter radionuclide tracers, and to minimize or eliminate the need for evaporation of solutions of the parent or daughter nuclides. Useful secondary separations involving the daughters of the initial parent radionuclide are also described. Separation systems for {sup 210}Bi, {sup 210}Po, {sup 211}Pb, {sup 212}Pb, {sup 223}Ra, {sup 224}Ra, {sup 225}Ra, {sup 225}Ac, {sup 227}Th, {sup 228}Th, {sup 231}Th, {sup 234}Th, and {sup 239}Np are outlined in detail. (orig.)

  13. Standard Specification for Copper-Aluminum-Silicon-Cobalt Alloy, Copper-Nickel-Silicon-Magnesium Alloy, Copper-Nickel-Silicon Alloy, Copper-Nickel-Aluminum-Magnesium Alloy, and Copper-Nickel-Tin Alloy Sheet and Strip

    CERN Document Server

    American Society for Testing and Materials. Philadelphia

    2015-01-01

    Standard Specification for Copper-Aluminum-Silicon-Cobalt Alloy, Copper-Nickel-Silicon-Magnesium Alloy, Copper-Nickel-Silicon Alloy, Copper-Nickel-Aluminum-Magnesium Alloy, and Copper-Nickel-Tin Alloy Sheet and Strip

  14. 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.

  15. 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.

  16. Probing the chemistry, electronic structure and redox energetics in pentavalent organometallic actinide complexes

    Energy Technology Data Exchange (ETDEWEB)

    Graves, Christopher R [Los Alamos National Laboratory; Vaughn, Anthony E [Los Alamos National Laboratory; Morris, David E [Los Alamos National Laboratory; Kiplinger, Jaqueline L [Los Alamos National Laboratory

    2008-01-01

    Complexes of the early actinides (Th-Pu) have gained considerable prominence in organometallic chemistry as they have been shown to undergo chemistries not observed with their transition- or lanthanide metal counterparts. Further, while bonding in f-element complexes has historically been considered to be ionic, the issue of covalence remains a subject of debate in the area of actinide science, and studies aimed at elucidating key bonding interactions with 5f-orbitals continue to garner attention. Towards this end, our interests have focused on the role that metal oxidation state plays in the structure, reactivity and spectral properties of organouranium complexes. We report our progress in the synthesis of substituted U{sup V}-imido complexes using various routes: (1) Direct oxidation of U{sup IV}-imido complexes with copper(I) salts; (2) Salt metathesis with U{sup V}-imido halides; (3) Protonolysis and insertion of an U{sup V}-imido alkyl or aryl complex with H-N{double_bond}CPh{sub 2} or N{triple_bond}C-Ph, respectively, to form a U{sup V}-imido ketimide complex. Further, we report and compare the crystallographic, electrochemical, spectroscopic and magnetic characterization of the pentavalent uranium (C{sub 5}Me{sub 5}){sub 2}U({double_bond}N-Ar)(Y) series (Y = OTf, SPh, C{triple_bond}C-Ph, NPh{sub 2}, OPh, N{double_bond}CPh{sub 2}) to further interrogate the molecular, electronic, and magnetic structures of this new class of uranium complexes.

  17. 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.

  18. Preliminary studies of a new accelerator-driven minor actinide burner in industrial scale

    Energy Technology Data Exchange (ETDEWEB)

    Li, Xunzhao; Zhou, Shengcheng [School of Nuclear Science and Technology, Xi’an Jiaotong University, Xi’an 710049, Shaanxi (China); Zheng, Youqi, E-mail: yqzheng@mail.xjtu.edu.cn [School of Nuclear Science and Technology, Xi’an Jiaotong University, Xi’an 710049, Shaanxi (China); Wang, Kunpeng [Nuclear and Radiation Safety Center, PO Box 8088, No. 54, Beijing 100082 (China); Wu, Hongchun [School of Nuclear Science and Technology, Xi’an Jiaotong University, Xi’an 710049, Shaanxi (China)

    2015-10-15

    Highlights: • A new accelerator-driven minor actinide (MA) burner was proposed. • Comprehensive design of spallation target, fuel assembly and subcritical core was performed. • Preliminary safety analyses indicate the inherent safety of the core in the reactivity insertion (500 pcm) and beam overpower (50% increase) transients. - Abstract: Pursuing high transmutation rate of minor actinide (MA), a preliminary conceptual design of a lead-bismuth (LBE) cooled accelerator-driven system (ADS) is proposed in this study. Parametric studies are performed to optimize the neutronics and thermal–hydraulics performances. The proton energy and axial position of the proton beam impact is investigated to obtain high neutron source efficiency and spallation neutron yield. The influences of MA/Pu mixing ratio and the ratio of pin pitch to diameter (P/D) are also optimized to control the burnup reactivity swing and the minimum coolant velocity for adequate cooling. To reduce the power peak, three kinds of power flattening techniques are adopted and compared. The results show that the inert matrix ratio zone loading method seems more versatile. Based on the analyses, an optimized three zone loading pattern is proposed for the 800 MWth subcritical core. The total transmutation rate of MA is 328.8 kg per effective full power year. Preliminary safety analyses based on the balance of power method (BOP) are performed and the results show that in the reactivity insertion and beam overpower transients, the core shows inherent safety, but the scram is necessary by cutting off the beam current to protect the core from possible damages caused by the loss of flow.

  19. Discrete fragment model for apparent formation constants of actinide ions with humic substances

    Energy Technology Data Exchange (ETDEWEB)

    Sasaki, Takayuki; Yoshida, Hatsumi; Aoyama, Shunsuke; Kobayashi, Taishi; Takagi, Ikuji [Kyoto Univ. (Japan). Dept. of Nuclear Engineering; Moriyama, Hirotake [Kyoto Univ., Osaka (Japan). Research Reactor Inst.

    2015-09-01

    A semi-empirical thermodynamic model was applied to estimate the apparent formation constants of actinide ions, i.e., Th(IV), Pu(IV) and Np(V), with humic substances (HSs), including humic and fulvic acids, over a wide range of solution conditions, i.e., pH, ionic strength, and HS and metal concentrations. The hypothetical HSs consist of humic and fulvic acids with nine types of simple organic ligands, which include aromatic and aliphatic carboxyl groups and phenol groups, as binding sites. The abundance of each binding site in the hypothetical HSs was determined via a fitting analysis using an acid-dissociation dataset for several HSs. To determine the apparent formation constant of a given metal ion with HSs, 54 specific binding sites were considered, including nine monodentate sites (1:1 metal/ligand complexes) and 45 bidentate sites (1:2 metal/ligand complexes). The formation constant of each monodentate binding was determined from the experimental data, while those of the bidentate bindings were determined by considering two monodentate bindings and the chelating effect, for which one of the adjustable parameters was introduced in the model. Introduction of the other parameter, which is related to the fraction of monodentate to bidentate sites (i.e., the heterogeneity), afforded the parameter values with good correlation with the apparent formation constant data. The present model with adjusted parameter values well reproduced the experimental apparent complex formation constants for actinide ion interaction with HSs in a wide range of solution conditions except for those obtained at trace concentrations.

  20. Solar r-process-constrained actinide production in neutrino-driven winds of supernovae

    Science.gov (United States)

    Goriely, S.; Janka, H.-Th.

    2016-07-01

    Long-lived radioactive nuclei play an important role as nucleo-cosmochronometers and as cosmic tracers of nucleosynthetic source activity. In particular, nuclei in the actinide region like thorium, uranium, and plutonium can testify to the enrichment of an environment by the still enigmatic astrophysical sources that are responsible for the production of neutron-rich nuclei by the rapid neutron-capture process (r-process). Supernovae and merging neutron-star (NS) or NS-black hole binaries are considered as most likely sources of the r-nuclei. But arguments in favour of one or the other or both are indirect and make use of assumptions; they are based on theoretical models with remaining simplifications and shortcomings. An unambiguous observational determination of a production event is still missing. In order to facilitate searches in this direction, e.g. by looking for radioactive tracers in stellar envelopes, the interstellar medium or terrestrial reservoirs, we provide improved theoretical estimates and corresponding uncertainty ranges for the actinide production (232Th, 235, 236, 238U, 237Np, 244Pu, and 247Cm) in neutrino-driven winds of core-collapse supernovae. Since state-of-the-art supernova models do not yield r-process viable conditions - but still lack, for example, the effects of strong magnetic fields - we base our investigation on a simple analytical, Newtonian, adiabatic and steady-state wind model and consider the superposition of a large number of contributing components, whose nucleosynthesis-relevant parameters (mass weight, entropy, expansion time-scale, and neutron excess) are constrained by the assumption that the integrated wind nucleosynthesis closely reproduces the Solar system distribution of r-process elements. We also test the influence of uncertain nuclear physics.

  1. 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.

  2. Strength of Hard Alloys,

    Science.gov (United States)

    Partial replacement of titanium carbide by tantalum carbide in three-phase WC-TiC-Co alloys tends to have a favorable effect on mechanical properties such as fatigue strength under bending and impact durability.

  3. Alloy Selection System

    Energy Technology Data Exchange (ETDEWEB)

    None

    2001-02-01

    Software will Predict Corrosion Rates to Improve Productivity in the Chemical Industry. Many aspects of equipment design and operation are influenced by the choice of the alloys used to fabricate process equipment.

  4. First Everlasting Alloy

    Institute of Scientific and Technical Information of China (English)

    杨仲言

    1994-01-01

    There′s new alloy that apparently just won′t give up. When a pin was scraped along it the equivalent of one million times, the alloy-made of zirconium, palladium, and ruthenium—displayed no net loss of surface material. When astonished researchers at the National Institute of Standards and Technology(NIST) persevered with a five-million-cycle wear test, they got the same result.

  5. Machining of titanium alloys

    CERN Document Server

    2014-01-01

    This book presents a collection of examples illustrating the resent research advances in the machining of titanium alloys. These materials have excellent strength and fracture toughness as well as low density and good corrosion resistance; however, machinability is still poor due to their low thermal conductivity and high chemical reactivity with cutting tool materials. This book presents solutions to enhance machinability in titanium-based alloys and serves as a useful reference to professionals and researchers in aerospace, automotive and biomedical fields.

  6. Dissolution of britholites and monazite / brabantite solid solutions doped with actinides; Etude de la dissolution de britholites et de solutions solides monazite / brabantite dopees avec des actinides

    Energy Technology Data Exchange (ETDEWEB)

    Du Fou De Kerdaniel, E

    2007-12-15

    In the field of the radwaste storage in underground repository, several matrices were considered as promising ceramics for the specific immobilization of actinides. Two of them, britholites and monazite/ brabantite solid solution, have been considered during this work. In order to examine the dissolution mechanisms occurring at the solid liquid interface, several leaching experiments have been conducted on (Ln{sup III}PO{sub 4} ), brabantite (Ca{sup II}An{sup IV}(PO{sub 4}){sub 2}: An = Th, U) and britholites (Ca{sub 9}Nd{sub 0.5}An{sub 0.5}{sup IV} (PO{sub 4}){sub 4.5}(SiO{sub 4}){sub 1.5}F{sub 2}: An = Th, U). Some steady experiments, performed in under saturation conditions for various pH and temperature conditions allowed to evaluate the long term behaviour of such matrices through their chemical durability. On the contrary, the thermodynamic equilibria were examined through the leaching experiments performed near the saturation conditions. By the way, various secondary phases, precipitated onto the surface of altered samples have been identified and characterized. Among them, the (Nd, Ca, Th) - rhabdophane, novelly prepared in over- saturation experiments for a thorium weight loading lower than 11 % appeared to be metastable. Indeed, it turns into TPHPH (Th{sub 2}(PO{sub 4}){sub 2}HPO{sub 4}.H{sub 2}O) and Nd - rhabdophane (NdPO{sub 4}.1/2H{sub 2}O) when increasing leaching time. (author)

  7. Delta phase plutonium and its alloys with III B elements: a microscopic study; Etude du plutonium en phase {delta} et de ses alliages avec les elements de la colonne IIIB

    Energy Technology Data Exchange (ETDEWEB)

    Bouchet, J

    2001-07-01

    The plutonium belongs to the actinides where it occupies a crucial place. In the actinide series the competition between the itinerant and local character of the f-electrons is responsible of its unique properties. The series can be divided into two sub-series: the light ({sub 90}Th-{sub 94}Pu) and the heavy ({sub 95}Am and beyond) actinides with very different characteristics. The volume behavior of the light actinides is very similar to the one found for the transitions metals with a parabolic decrease of the volume as a function of atomic number. This trend can be explained by the itinerant character of the 5 f electrons which participate to the chemical bonding, and thus the light actinides are considered to form a 5 f transition series. The density functional theory in the local-density approximation (LDA) gives a good description of the ground state of the light actinides in agreement with experiment and a simple Friedel model can explain the parabolic decrease of the volumes. As for heavy actinides, the pattern is reversed: 5 f electrons are localized. This picture places plutonium as the link between the two series, at the transition from delocalized to localized states. The density functional theory within the local density approximation is a very crude approximation for these systems where the on-site interaction between f electrons is strong enough to overcome the kinetic energy. Equilibrium properties for the {delta}-phase of Pu have been calculated. Taking into account strong electron correlations in the 5 f shell, we show how the equilibrium volume and the bulk modulus are improved in comparison to previous results using the local density approximation (LDA) or the generalized gradient approximation (GGA). In addition, an augmentation of the orbital moment is observed due to the respect of Hund's rules, reducing the total magnetic moment. The stability of the {delta}-phase is explored and for the first time a positive value for the tetragonal

  8. Reduction of minor actinides for recycling in a light water reactor; Reduccion de actinidos menores por reciclado en un reactor de agua ligera

    Energy Technology Data Exchange (ETDEWEB)

    Martinez C, E.; Ramirez S, J. R.; Alonso V, G., E-mail: eduardo.martinez@inin.gob.mx [ININ, Carretera Mexico-Toluca s/n, 52750 Ocoyoacac, Estado de Mexico (Mexico)

    2015-09-15

    The aim of actinide transmutation from spent nuclear fuel is the reduction in mass of high-level waste which must be stored in geological repositories and the lifetime of high-level waste; these two achievements will reduce the number of repositories needed, as well as the duration of storage. The present work is directed towards the evaluation of an advanced nuclear fuel cycle in which the minor actinides (Np, Am and Cm) could be recycled to remove most of the radioactive material; a reference of actinides production in standard nuclear fuel of uranium at the end of its burning in a BWR is first established, after a design of fuel rod containing 6% of minor actinides in a matrix of uranium from the enrichment lines is proposed, then 4 fuel rods of standard uranium are replaced by 4 actinides bars to evaluate the production and transmutation of them and finally the minor actinides reduction in the fuel is evaluated. In the development of this work the calculation tool are the codes: Intrepin-3, Casmo-4 and Simulate-3. (Author)

  9. Complexation parameters for the actinides(IV)-humic acid system: a search for consistency and application to laboratory and field observations

    Energy Technology Data Exchange (ETDEWEB)

    Reiller, P.E. [Commissariat a l' Energie Atomique, CE Saclay, Gif-sur Yvette (France). Nuclear Energy Div./DPC/SECR/Lab. de Speciation des Radionucleides et des Molecules; Evans, N.D.M. [Loughborough Univ., Leics (United Kingdom). Dept. of Chemistry; Szabo, G. [' Frederic Joliot-Curie' National Research Inst. for Radiobiology and Radiohygiene, Budapest (Hungary)

    2008-07-01

    The coherence of actinide(IV) complexation by humic substances (HS) is reviewed and new data are proposed. In a first attempt, the values of independent data from literature on Th(IV), U(IV), and Pu(IV) are collected, selected, and compiled. The data obtained follow the 'classical' trend of increasing conditional formation 'constants' with pH, led both by the increasing ionisation of HS and by the extensive hydrolysis of the tetravalent actinides. Even though a fair agreement is evident, the experimental uncertainties do not permit a full analogy between the actinides(IV) to be ascertained. In a second attempt, the experiments from which the original data are available were reinterpreted using only one hydrolysis constant set for U(IV) as an example, considering that all actinides(IV) have analogous humic complexation behaviour. Hence, the obtained evolution of conditional formation 'constants' is much more coherent and the uncertainties do not permit to distinguish an actinide(IV) from one another. The obtained data are then applied to independent laboratory and in situ experiments in order to delimit the domain of possible applicability. This exercise demonstrates the treatment of data through analogy in the case of actinides(IV) and would permit to limit and orientate the number of necessary, but difficult, experiment with redox sensitive elements like U, Np, or Pu. It also demonstrates that complexation-only mechanisms may not be sufficient to understand field observations. (orig.)

  10. Study of the actinide-lanthanide separation from nuclear waste by a new pyrochemical process; Etude de la separation actinides-lanthanides des dechets nucleaires par un procede pyrochimique nouveau

    Energy Technology Data Exchange (ETDEWEB)

    Lemort, F. [CEA Marcoule, Departement de Retraitement, des Dechets et du Demantelement, 30 - Bagnols-sur-Ceze (France)]|[Institut National Polytechnique, 38 - Grenoble (France)

    1997-01-01

    The theoretical extraction and separation of platinoids, actinides and lanthanides is allowed by thermodynamic using two adapted reducing agents: zinc and magnesium. Thereby, a pyrochemical method for the nuclear waste processing has been devised. The high temperature handling of the elements in fluoride forms and their processing by a reactive metallic phase required special precautions. The study of the behavior of matter in exploratory systems allowed the development of an experimental technology for the treatment and contacting of phases. The thermodynamical analysis of the experimental results shows the feasibility of the process. A model was developed to predict the distribution coefficients of zirconium, uranium and lanthanum as a function of the system composition. An estimation method was proposed in order to evaluate the distribution coefficients in diluted solution of all the actinides and lanthanides existing in the fission products between LiF CaF{sub 2} and Zn-Mg at 720 deg C. Coupled with the experimental results, the estimates results may be extrapolated to concentrated solutions allowing predictions of the separation of all actinides and lanthanides. The rapidity of element transfer is induced by a thermal effect caused by the high exothermicity of the reduction by magnesium. The kinetic coefficients have been linked with the reduction enthalpy of each element. Moreover, the kinetics seem limited by chemical reaction and not by mass transfer. (author) 66 refs.

  11. Study of irradiation effects in perovskite: use of this matrix for actinides conditioning; Effets de l'irradiation dans une perovskite: utilisation de cette matrice pour un conditionnement des actinides

    Energy Technology Data Exchange (ETDEWEB)

    Sabathier, C

    2003-07-01

    The aim of this work is to study a specific conditioning matrix (ceramics) for actinides: the strontium titanate. At first, the choice of strontium titanate is discussed as well as its structure and its ability to incorporate actinides. The different studies carried out on the irradiation effects on the strontium titanate are reviewed. The main ion-matter interactions considered in the energy range used during our experiments are given. The different devices and techniques used with ion beams to carry out our experiments according to the type of sample: monocrystal or polycrystal are described. The experimental results on the behaviour of strontium titanate in terms of irradiation, temperature and ion flux used to damage the matrix are presented. The experimental results on the different steps of strontium titanate annealing are given as well as the identifying of the defects by different analyses techniques (Rutherford backscattering spectroscopy, transmission electron spectroscopy and x-rays spectroscopy). At last, a model of the behaviour of the strontium titanate in the case of an actinide conditioning is proposed and the evolving of the strontium titanate disorder during the storage is discussed. (O.M.)

  12. 3 and 4 oxidation state element solubilities in borosilicate glasses. Implement to actinides in nuclear glasses; Solubilite des elements aux degres d'oxydation (3) et (4) dans les verres de borosilicate. Application aux actinides dans les verres nucleaires

    Energy Technology Data Exchange (ETDEWEB)

    Cachia, J.N

    2005-12-15

    In order to ensure optimal radionuclides containment, the knowledge of the actinide loading limits in nuclear waste glasses and also the comprehension of the solubilization mechanisms of these elements are essential. A first part of this manuscript deals with the study of the differences in solubility of the tri and tetravalent elements (actinides and surrogates) particularly in function of the melting temperature. The results obtained indicate that trivalent elements (La, Gd, Nd, Am, Cm) exhibit a higher solubility than tetravalent elements (Hf, Th, Pu). Consequently, it was planned to reduce plutonium at the oxidation state (III), the later being essentially tetravalent in borosilicate glasses. An innovating reduction process of multi-valent elements (cerium, plutonium) using silicon nitride has been developed in a second part of this work. Reduced plutonium-bearing glasses synthesized by Si{sub 3}N{sub 4} addition made it possible to double the plutonium solubility from 2 to 4 wt% at 1200 deg C. A structural approach to investigate the differences between tri and tetravalent elements was finally undertaken. These investigations were carried out by X-rays Absorption Spectroscopy (EXAFS) and NMR. Trivalent rare earth and actinide elements seem to behave as network modifiers while tetravalent elements rather present true intermediaries' behaviour. (author)

  13. Neutron Capture Measuremetns on Minor Actinides at the n_TOF Facility at CERN: Past, Present and Future

    CERN Document Server

    Cano-Ott, D; Eleftheriadis, C; Leeb, H; Calvino, F; Herrera-Martinez, A; Savvidis, I; Vlachoudis, V; Haas, B; Abbondanno, U; Vannini, G; Oshima, M; Gramegna, F; Wiescher, M; Pigni, M T; Wiendler, H; Mengoni, A; Quesada, J; Becvar, F; Rosetti, M; Cennini, P; Mosconi, M; Duran, I; Rauscher, T; Ketlerov, V; Couture, A; Capote, R; Sarchiapone, L; Vlastou, R; Domingo-Pardo, C; Pavlopoulos, P; Karamanis, D; Krticka, M; Griesmayer, E; Jericha, E; Ferrari, A; Martinez, T; Oberhummer, H; Karadimos, D; Plompen, A; Mendoza, E; Terlizzi, R; Cortes, G; Cox, J; Voss, F; Pretel, C; Colonna, N; Berthoumieux, E; Dolfini, R; Vaz, P; Heil, M; Lopes, I; Lampoudis, C; Walter, S; Calviani, M; Gonzalez-Romero, E; Stephan, C; Tain, J L; Belloni, F; Igashira, M; Papachristodoulou, C; Aerts, G; Tavora, L; Milazzo, P M; Rudolf, G; Andrzejewski, J; Villamarin, D; Ferreira-Marques, R; Meaze, M H; O'Brien, S; Gunsing, F; Reifarth, R; Perrot, L; Lindote, A; Neves, F; Poch, A; Konovalov, V; Kerveno, M; Marques, L; Rubbia, C; Koehler, P; Dahlfors, M; Wisshak, K; Fujii, K; De Albornoz, A C; Salgado, J; Dridi, W; Ventura, A; Andriamonje, S; Dillman, I; Assimakopoulos, P; Ferrant, L; Lozano, M; Patronis, N; Chiaveri, E; Guerrero, C; Kadi, Y; Vicente, M C; Praena, J; Baumann, P; Moreau, C; Kappeler, F; Rullhusen, P; Furman, W; David, S; Marrone, S; Paradela, C; Audouin, L; Tassan-Got, L; Alvarez-Velarde, F; Massimi, C; Mastinu, P; Isaev, S; Pancin, J; Papadopoulos, C; Tagliente, G; Alvarez, H; Haight, R; Goverdovski, A; Chepel, V; Plag, R; Kossionides, E; Badurek, G; Marganiec, J; Lukic, S; Frais-Koelbl, H; Pavlik, A; Goncalves, I

    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 studies and reports {[}1-3] have identified the need for substantially improving the accuracy of neutron cross-section data for minor actinides. The n\\_TOF collaboration has initiated an ambitious experimental program for the measurement of neutron capture cross sections of minor actinides. Two experimental setups have been constructed for this purpose: a Total Absorption Calorimeter (TAC) {[}4] for measuring neutron capture cross-sections of low-mass and/or radioactive samples and a set of two low neutron sensitivity C(6)D(6) detectors for the less radioactive materials.

  14. The 'granite encapsulation' route to the safe disposal of Pu and other actinides

    Energy Technology Data Exchange (ETDEWEB)

    Gibb, F.G.F. [Immobilisation Science Laboratory, Department of Engineering Materials, University of Sheffield, Sheffield S1 3JD (United Kingdom)], E-mail: f.gibb@sheffield.ac.uk; Taylor, K.J. [Department of Geography, University of Sheffield, Sheffield S10 2TN (United Kingdom); Burakov, B.E. [Laboratory of Applied Mineralogy and Radiogeochemistry, V.G. Khlopin Radium Institute, St. Petersburg 194021 (Russian Federation)

    2008-03-15

    Waste actinides, including plutonium, present a long-term management problem and a serious security issue. Immobilisation in mineral or ceramic waste forms for interim storage is a widely proposed first step. The safest, most secure geological disposal for Pu is in very deep boreholes and we propose that the key step to combination of these immobilisation and disposal concepts is encapsulation of the waste form in cylinders of recrystallized granite. We discuss the underpinning science, focusing on experimental work, and consider implementation. Finally, we present and discuss analyses of zircon, UO{sub 2} and Ce-doped cubic zirconia from high pressure and temperature experiments in granitic melts that demonstrate the viability of this solution and that actinides can be isolated from the environment for millions, maybe hundreds of millions, of years.

  15. Correlation between diffusion barriers and alloying energy in binary alloys

    DEFF Research Database (Denmark)

    Vej-Hansen, Ulrik Grønbjerg; Rossmeisl, Jan; Stephens, Ifan;

    2016-01-01

    In this paper, we explore the notion that a negative alloying energy may act as a descriptor for long term stability of Pt-alloys as cathode catalysts in low temperature fuel cells.......In this paper, we explore the notion that a negative alloying energy may act as a descriptor for long term stability of Pt-alloys as cathode catalysts in low temperature fuel cells....

  16. 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

  17. Gas-phase energies of actinide oxides -- an assessment of neutral and cationic monoxides and dioxides from thorium to curium

    Energy Technology Data Exchange (ETDEWEB)

    Marcalo, Joaquim; Gibson, John K.

    2009-08-10

    An assessment of the gas-phase energetics of neutral and singly and doubly charged cationic actinide monoxides and dioxides of thorium, protactinium, uranium, neptunium, plutonium, americium, and curium is presented. A consistent set of metal-oxygen bond dissociation enthalpies, ionization energies, and enthalpies of formation, including new or revised values, is proposed, mainly based on recent experimental data and on correlations with the electronic energetics of the atoms or cations and with condensed-phase thermochemistry.

  18. INVESTIGATION OF MAGNESIUM ALLOYS MACHINABILITY

    Directory of Open Access Journals (Sweden)

    Berat Barıs BULDUM

    2013-01-01

    Full Text Available Magnesium is the lightest structural metal. Magnesium alloys have a hexagonal lattice structure, which affects the fundamental properties of these alloys. Plastic deformation of the hexagonal lattice is more complicated than in cubic latticed metals like aluminum, copper and steel. Magnesium alloy developments have traditionally been driven by industry requirements for lightweight materials to operate under increasingly demanding conditions. Magnesium alloys have always been attractive to designers due to their low density, only two thirds that of aluminium and its alloys [1]. The element and its alloys take a big part of modern industry needs. Especially nowadays magnesium alloys are used in automotive and mechanical (trains and wagons manufacture, because of its lightness and other features. Magnesium and magnesium alloys are the easiest of all metals to machine, allowing machining operations at extremely high speed. All standard machining operations such as turning, drilling, milling, are commonly performed on magnesium parts.

  19. Level Densities in the actinide region and indirect n,y cross section measurements using the surrogate method

    Directory of Open Access Journals (Sweden)

    Wiedeking M.

    2012-02-01

    Full Text Available Results from a program of measurements of level densities and gamma ray strength functions in the actinide region are presented. Experiments at the Oslo cyclotron involving the Cactus/Siri detectors and 232Th(d,x and 232Th(3He,x reactions were carried out to help answer the question of which level density model is the most appropriate for actinide nuclei, since it will have an impact on cross section calculations important for reactor physics simulations. A new technique for extracting level densities and gamma ray strength functions from particle-gamma coincidence data is proposed and results from the development of this technique are presented. In addition, simultaneous measurements of compound nuclear gamma decay probabilities have been performed for the key thorium cycle nuclei 233Th, 231Th and 232Pa up to around 1MeV above the neutron binding energy and have enabled extraction of indirect neutron induced capture cross sections for the 232Th, 231Pa and 230Th nuclei using the surrogate reaction method. Since the neutron capture cross section for 232Th is already well known from direct measurements a comparison provides a stringent test of the applicability of the surrogate technique in the actinide region.

  20. Measurements of actinide-fission product yields in Caliban and Prospero metallic core reactor fission neutron fields

    Energy Technology Data Exchange (ETDEWEB)

    Casoli, P.; Authier, N. [CEA, Centre de Valduc, 21120 Is-sur-Tille (France); Laurec, J.; Bauge, E.; Granier, T. [CEA, Centre DIF, 91297 Arpajon (France)

    2011-07-01

    In the 1970's and early 1980's, an experimental program was performed on the facilities of the CEA Valduc Research Center to measure several actinide-fission product yields. Experiments were, in particular, completed on the Caliban and Prospero metallic core reactors to study fission-neutron-induced reactions on {sup 233}U, {sup 235}U, and {sup 239}Pu. Thick actinide samples were irradiated and the number of nuclei of each fission product was determined by gamma spectrometry. Fission chambers were irradiated simultaneously to measure the numbers of fissions in thin deposits of the same actinides. The masses of the thick samples and the thin deposits were determined by mass spectrometry and alpha spectrometry. The results of these experiments will be fully presented in this paper for the first time. A description of the Caliban and Prospero reactors, their characteristics and performances, and explanations about the experimental approach will also be given in the article. A recent work has been completed to analyze and reinterpret these measurements and particularly to evaluate the associated uncertainties. In this context, calculations have also been carried out with the Monte Carlo transport code Tripoli-4, using the published benchmarked Caliban description and a three-dimensional model of Prospero, to determine the average neutron energy causing fission. Simulation results will be discussed in this paper. Finally, new fission yield measurements will be proposed on Caliban and Prospero reactors to strengthen the results of the first experiments. (authors)

  1. Investigation of the complexation and the migration of actinides and non-radioactive substances with humic acids under geogenic conditions. Complexation of humic acids with actinides in the ocidation state IV Th, U, Np

    Energy Technology Data Exchange (ETDEWEB)

    Sachs, S.; Schmeide, K.; Brendler, V.; Krepelova, A.; Mibus, J.; Geipel, G.; Heise, K.H.; Bernhard, G.

    2004-03-01

    Objective of this project was the study of basic interaction and migration processes of actinides in the environment in presence of humic acids (HA). To obtain more basic knowledge on these interaction processes synthetic HA with specific functional properties as well as {sup 14}C-labeled HA were synthesized and applied in comparison to the natural HA Aldrich. One focus of the work was on the synthesis of HA with distinct redox functionalities. The obtained synthetic products that are characterized by significantly higher Fe(III) redox capacities than Aldrich HA were applied to study the redox properties of HA and the redox stability of U(VI) humate complexes. It was confirmed that phenolic OH groups play an important role for the redox properties of HA. However, the results indicate that there are also other processes than the single oxidation of phenolic OH groups and/or other functional groups contributing to the redox behavior of HA. A first direct-spectroscopic proof for the reduction of U(VI) by synthetic HA with distinct redox functionality was obtained. The complexation behavior of synthetic and natural HA with actinides (Th, Np, Pu) was studied. Structural parameters of Pu(III), Th(IV), Np(IV) and Np(V) humates were determined by X-ray absorption spectroscopy (XAS). The results show that carboxylate groups dominate the interaction between HA and actinide ions. These are predominant monodentately bound. The influence of phenolic OH groups on the Np(V) complexation by HA was studied with modified HA (blocked phenolic OH groups). The blocking of phenolic OH groups induces a decrease of the number of maximal available complexing sites of HA, whereas complex stability constant and Np(V) near-neighbor surrounding are not affected. The effects of HA on the sorption and migration behavior of actinides was studied in batch and column experiments. Th(IV) sorption onto quartz and Np(V) sorption onto granite and its mineral constituents are affected by the pH value

  2. Selective dissolution in binary alloys

    Science.gov (United States)

    McCall, Carol Rene

    Corrosion is an important issue in the design of engineering alloys. De-alloying is an aspect of alloy corrosion related to the selective dissolution of one or more of the components in an alloy. The work reported herein focuses on the topic of de-alloying specific to single-phase binary noble metal alloy systems. The alloy systems investigated were gold-silver and gold-copper. The onset of a bulk selective dissolution process is typically marked by a critical potential whereby the more reactive component in the alloy begins dissolving from the bulk, leading to the formation of a bi-continuous solid-void morphology. The critical potential was investigated for the entire composition range of gold-silver alloys. The results presented herein include the formulation of an expression for critical potential as a function of both alloy and electrolyte composition. Results of the first investigation of underpotential deposition (UPD) on alloys are also presented herein. These results were implemented as an analytical tool to provide quantitative measurements of the surface evolution of gold during de-alloying. The region below the critical potential was investigated in terms of the compositional evolution of the alloy surface. Below the critical potential, there is a competition between the dissolution of the more reactive alloying constituent (either silver or copper) and surface diffusion of gold that serves to cover dissolution sites and prevent bulk dissolution. By holding the potential at a prescribed value below the critical potential, a time-dependent gold enrichment occurs on the alloy surface leading to passivation. A theoretical model was developed to predict the surface enrichment of gold based on the assumption of layer-by-layer dissolution of the more reactive alloy constituent. The UPD measurements were used to measure the time-dependent surface gold concentration and the results agreed with the predictions of the theoretical model.

  3. Structural thermodynamics of alloys

    CERN Document Server

    Manenc, Jack

    1973-01-01

    Technical progress has for a very long time been directly dependent on progress in metallurgy, which is itself connected with improvements in the technology of alloys. Metals are most frequently used in the form of alloys for several reasons: the quantity of pure metal in its native state in the earth's crust is very limited; pure metals must be extracted from ores which are themselves impure. Finally, the methods of treatment used lead more easily to alloys than to pure metals. The most typical case is that of iron, where a pure ore may be found, but which is the starting point for cast iron or steel, alloys of iron and carbon. In addition, the properties of alloys are in general superior to those of pure metals and modem metallurgy consists of controlling these properties so as to make them conform to the requirements of the design office. Whilst the engineer was formerly compelled to adapt his designs and constructions to the materials available, such as wood, stone, bronze, iron, cast iron and ordinary st...

  4. 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

  5. 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

  6. 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

  7. De-alloyed platinum nanoparticles

    Science.gov (United States)

    Strasser, Peter; Koh, Shirlaine; Mani, Prasanna; Ratndeep, Srivastava

    2011-08-09

    A method of producing de-alloyed nanoparticles. In an embodiment, the method comprises admixing metal precursors, freeze-drying, annealing, and de-alloying the nanoparticles in situ. Further, in an embodiment de-alloyed nanoparticle formed by the method, wherein the nanoparticle further comprises a core-shell arrangement. The nanoparticle is suitable for electrocatalytic processes and devices.

  8. Neutron absorbing alloy

    Energy Technology Data Exchange (ETDEWEB)

    Hayashi, Masayuki

    1998-12-04

    The neutron absorbing alloy of the present invention comprises Ti or an alloy thereof as a mother material, to which from 2 to 40% by weight of Hf and Gd within a range of from 4 to 50% by weight in total are added respectively. Ti is excellent in specific strength, corrosion resistance and workability, and produces no noxious intermetallic compound with Hf and Gd. In addition, since the alloy can incorporate a great quantity of Hf and Gd, a neutron absorbing material having excellent neutron absorbing performance than usual and excellent in specific strength, corrosion resistance and workability can be manufactured conveniently and economically not by a special manufacturing method. (T.M.)

  9. Shape Memory Alloys

    Directory of Open Access Journals (Sweden)

    Deexith Reddy

    2016-07-01

    Full Text Available Shape memory alloys (SMAs are metals that "remember" their original shapes. SMAs are useful for such things as actuators which are materials that "change shape, stiffness, position, natural frequency, and other mechanical characteristics in response to temperature or electromagnetic fields" The potential uses for SMAs especially as actuators have broadened the spectrum of many scientific fields. The study of the history and development of SMAs can provide an insight into a material involved in cutting-edge technology. The diverse applications for these metals have made them increasingly important and visible to the world. This paper presents the working of shape memory alloys , the phenomenon of super-elasticity and applications of these alloys.

  10. Double Glow Plasma Surface Alloyed Burn-resistant Titanium Alloy

    Institute of Scientific and Technical Information of China (English)

    ZHANG Ping-ze; XU Zhong; HE Zhi-yong; ZHANG Gao-hui

    2004-01-01

    Conventional titanium alloy may be ignited and burnt under high temperature, high pressure and high gas flow velocity condition. In order to avoid this problem, we have developed a new kind of burn-resistant titanium alloy-double glow plasma surface alloying burn-resistant titanium alloy. Alloying element Cr, Mo, Cu are induced into the Ti-6Al-4V and Ti-6.5Al-0.3Mo-l.5Zr-0.25Si substrates according to double glow discharge phenomenon, Ti-Cr ,Ti-Mo, Ti-Cu binary burn-resistant alloy layers are formed on the surface of Ti-6Al-4V and Ti-6.5Al-0.3Mo-l.5Zr-0.25Si alloys. The depth of the surface burn-resistant alloy layer can reach to above 200 microns and alloying element concentration can reach 90%.Burn-resistant property experiments reveal that if Cr concentration reach to 14%, Cu concentration reach to 12%, Mo concentration reach to 10% in the alloying layers, ignition and burn of titanium alloy can be effectively avoided.

  11. Double Glow Plasma Surface Alloyed Burn-resistant Titanium Alloy

    Institute of Scientific and Technical Information of China (English)

    ZHANGPing-ze; XUZhong; HEZhi-yong; ZHANGGao-hui

    2004-01-01

    Conventional titanium alloy may be ignited and burnt under high temperature, high pressure and high gas flow velocity condition. In order to avoid this problem, we have developed a new kind of burn-resistant titanium alloy-double glow plasma surface alloying burn-resistant titanium alloy. Alloying element Cr, Mo, Cu are induced into the Ti-6A1-4V and Ti-6.5Al-0.3Mo-1.5Zr-0.25Si substrates according to double glow discharge phenomenon, Ti-Cr ,Ti-Mo, Ti-Cu binary burn-resistant alloy layers are formed on the surface of Ti-6A1-4V and Ti-6.5Al-0.3Mo-1.5Zr-0.25Si alloys. The depth of the surface burn-resistant alloy layer can reach to above 200 microns and alloying element concentration can reach 90%. Burn-resistant property experiments reveal that if Cr concentration reach to 14%, Cu concentration reach to 12%, Mo concentration reach to 10% in the alloying layers, ignition and burn of titanium alloy can be effectively avoided.

  12. Strip Casting of High Performance Structural Alloys

    Institute of Scientific and Technical Information of China (English)

    S S Park; J G Lee; Nack J Kim

    2004-01-01

    There exists a great need for the development of high performance alloys due to increasing demands for energy conservation and environmental protection. Application of strip casting shows a strong potential for the improvement of properties of existing alloys and also for the development of novel alloy systems with superior properties. The present paper reviews our Center's activities in the development of high performance alloys by strip casting. Examples include (1) Al alloys, (2) wrought Mg alloys, and (3) bulk metallic glass (BMG) alloys.

  13. Pemilihan Bahan Alloy Untuk Konstruksi Gigitiruan

    OpenAIRE

    Medila Dahlan

    2008-01-01

    Pada kedokteran gigi bahan alloy sangat banyak digunakan dalam segala bidang. Dalam pembuatan konstruksi gigitiman biasanya digunakan alloy emas, alloy kobalt kromium, alloy nikei kromium dan alloy stainless steel sebagai komponen gigitiman kerangka logam serta pembuatan mahkota dan jembatan. Pemilihan bahan alloy dapat dilakukan berdasarkan sifat yang dimiiiki oleh masing-masing bahan alloy sehingga akan didapat hasil konstmksi gigitiruan yang memuaskan. Pada pemakaiannya didaiam mulut...

  14. Tungsten Alloy Outgassing Measurements

    CERN Document Server

    Rutherfoord, John P; Shaver, L

    1999-01-01

    Tungsten alloys have not seen extensive use in liquid argon calorimeters so far. Because the manufacturing process for tungsten is different from the more common metals used in liquid argon there is concern that tungsten could poison the argon thereby creating difficulties for precision calorimetry. In this paper we report measurements of outgassing from the tungsten alloy slugs proposed for use in the ATLAS FCal module and estimate limits on potential poisoning with reasonable assumptions. This estimate gives an upper limit poisoning rate of

  15. Charged defects during alpha-irradiation of actinide oxides as revealed by Raman and luminescence spectroscopy

    Energy Technology Data Exchange (ETDEWEB)

    Mohun, R.; Desgranges, L.; Léchelle, J. [CEA/DEN/DEC/SESC, Centre de Cadarache, 13108 Saint-Paul-lez-Durance (France); Simon, P.; Guimbretière, G.; Canizarès, A.; Duval, F. [CNRS, UPR 3079 CEMHTI, et Université d’Orléans, 1D avenue de la Recherche Scientifique, 45071 Orléans (France); Jegou, C.; Magnin, M. [CEA/DEN/DTCD, Centre de Marcoule, BP 17171, 30207 Bagnols sur Cèze (France); Clavier, N.; Dacheux, N. [ICSM, UMR 5257 CEA/CNRS/UM2/ENSCM, Site de Marcoule, BP 17171, 30207 Bagnols sur Cèze (France); Valot, C. [CEA/DEN/DTEC/SECA/LCC, BP 17171, 30207 Bagnols sur Cèze (France); Vauchy, R. [CEA/DEN/DEC/SPUA, Centre de Cadarache, 13108 Saint-Paul-lez-Durance (France)

    2016-05-01

    We have recently evidenced an original Raman signature of alpha irradiation-induced defects in UO{sub 2}. In this study, we aim to determine whether the same signature also exists in different actinide oxides, namely ThO{sub 2} and PuO{sub 2}. Sintered UO{sub 2} and ThO{sub 2} were initially irradiated with 21 MeV He{sup 2+} ions using a cyclotron device and were subjected to an in situ luminescence experiment followed by Raman analysis. In addition, a PuO{sub 2} sample which had accumulated self-irradiation damage due to alpha particles was investigated only by Raman measurement. Results obtained for the initially white ThO{sub 2} showed that a blue color appeared in the irradiated areas as well as luminescence signals during irradiation. However, Raman spectroscopic analysis showed the absence of Raman signature in ThO{sub 2}. In contrast, the irradiated UO{sub 2} and PuO{sub 2} confirmed the presence of the Raman signature but no luminescence peaks were observed. The proposed mechanism involves electronic defects in ThO{sub 2}, while a coupling between electronic defects and phonons is required to explain the Raman spectra for UO{sub 2} and PuO{sub 2}.

  16. Feasibility Study of Supercritical Light Water Cooled Fast Reactors for Actinide Burning and Electric Power Production

    Energy Technology Data Exchange (ETDEWEB)

    Mac Donald, Philip Elsworth; Buongiorno, Jacopo; Davis, Cliff Bybee; Weaver, Kevan Dean

    2002-01-01

    The use of supercritical temperature and pressure light water as the coolant in a direct-cycle nuclear reactor offers potential for considerable plant simplification and consequent capital and O&M cost reduction compared with current light water reactor (LWR) designs. Also, given the thermodynamic conditions of the coolant at the core outlet (i.e. temperature and pressure beyond the water critical point), very high thermal efficiencies of the power conversion cycle are possible (i.e. up to 46%). Because no change of phase occurs in the core, the need for steam separators and dryers as well as for BWR-type recirculation pumps is eliminated, which, for a given reactor power, results in a substantially shorter reactor vessel than the current BWRs. Furthermore, in a direct cycle the steam generators are not needed. If a tight fuel rod lattice is adopted, it is possible to significantly reduce the neutron moderation and attain fast neutron energy spectrum conditions. In this project a supercritical water reactor concept with a simple, blanket-free, pancake-shaped core will be developed. This type of core can make use of either fertile or fertile-free fuel and retain the hard spectrum to effectively burn plutonium and minor actinides from LWR spent fuel while efficiently generating electricity.

  17. 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.

  18. Relativistic Multireference Quantum Chemical Study of the Electronic Structure of Actinide Trioxide Molecules.

    Science.gov (United States)

    Kovács, Attila

    2017-03-17

    Actinide trioxide (AnO3, An = U, Np, Pu, Am, Cm) molecules have been investigated by relativistic multireference quantum chemical calculations with the goal to elucidate their electronic structures. The molecular geometries of the ground and selected excited electronic states have been optimized at the spin-orbit-free complete active space second-order perturbation theory (SF-CASPT2) level. The low-lying vertical excitation states have been computed and characterized by CASPT2 calculations taking into account spin-orbit coupling. The reason for the considerable lengthening of the equatorial An-O bond in AmO3 and CmO3 with respect to the other trioxides has been analyzed on the basis of valence molecular orbitals of the SF ground electronic states. For the bond in question a singly occupied π orbital has been identified, this orbital is doubly occupied in the other (An = U, Np, Pu) trioxides. The clarified electronic structures of the investigated AnO3 molecules confirmed the pentavalent character of Am and Cm in their trioxides in contrast to the hexavalent character of U, Np, and Pu.

  19. 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.

  20. Solar r-process-constrained actinide production in neutrino-driven winds of supernovae

    CERN Document Server

    Goriely, S

    2016-01-01

    Long-lived radioactive nuclei play an important role as nucleo-cosmochronometers and as cosmic tracers of nucleosynthetic source activity. In particular nuclei in the actinide region like thorium, uranium, and plutonium can testify to the enrichment of an environment by the still enigmatic astrophysical sources that are responsible for the production of neutron-rich nuclei by the rapid neutron-capture process (r-process). Supernovae and merging neutron-star (NS) or NS-black hole binaries are considered as most likely sources of the r-nuclei. But arguments in favour of one or the other or both are indirect and make use of assumptions; they are based on theoretical models with remaining simplifications and shortcomings. An unambiguous observational determination of a production event is still missing. In order to facilitate searches in this direction, e.g.\\ by looking for radioactive tracers in stellar envelopes, the interstellar medium or terrestrial reservoirs, we provide improved theoretical estimates and co...

  1. 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.

  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. Characterization of actinide targets by low solid-angle alpha particle counting

    CERN Document Server

    Denecke, B; Pauwels, J; Robouch, P; Gilliam, D M; Hodge, P; Hutchinson, J M R; Nico, J S

    1999-01-01

    Actinide samples were characterized in an interlaboratory comparison between IRMM and NIST, including alpha-particle counting at defined low solid angle and counting in a 2 pi proportional gas counter. For this comparison, nine sup 2 sup 3 sup 3 UF sub 4 samples with high uniformity in the layer thickness were prepared at IRMM by deposition under vacuum. Polished silicon wafers were used as source substrates, and these were rotated during the deposition using a planetary rotation system. The estimated uncertainties for the defined low solid-angle methods were about 0.1% at both NIST and IRMM. The agreement of reported alpha-particle emission rates in the energy range 2.5-5.09 MeV was better than or equal to 0.02% for the defined solid-angle methods. When comparing total alpha-particle emission rates over the larger energy range 0-9 MeV (which includes all emissions from the daughter nuclides and the impurities), the agreement of the defined solid-angle methods was better than or equal to 0.05%. The 2 pi propo...

  4. 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...

  5. 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.

  6. Detailed investigation of neutron emitters in the transmutation of Minor Actinides

    Energy Technology Data Exchange (ETDEWEB)

    Letourneau, A.; Bringer, O.; Dupont, E.; Panebianco, S.; Veyssiere, Ch. [CEA/Saclay/DSM/IRFU - Gif-sur-Yvette (France); Al Mahamid, I. [Wadsworth Center, New York State Department of Health, Albany, NY 12201 (United States); Chartier, F. [CEA/Saclay/DEN/DPC/SECR - Gif-sur-Yvette (France); Mutti, P. [Institut Laue-Langevin, Grenoble (France); Oriol, L. [CEA/Cadarache/DEN/DER/SPEX - Saint-Paul-lez-Durances (France)

    2008-07-01

    The production of neutron emitters during the incineration process of minor actinides could be very penalizing for the reprocessing of the targets when transmuted in heterogeneous mode, either in dedicated systems (ADS) or in generation IV reactors. Therefore their production has to be carefully evaluated. The reliability of such evaluation really depends on nuclear data (capture and fission cross sections) and their accuracy. In this paper we present a work we have done to investigate the production of neutron emitters in the incineration of {sup 237}Np and {sup 241}Am targets in fast and thermal nuclear reactor concepts. The impact of nuclear data uncertainties on the production of those neutron-emitters was evaluated by sensitivity calculations. The reduction for some of these uncertainties in the thermal energy region was done by measuring more precisely the {sup 244}Cm(n,gamma){sup 245}Cm, {sup 245}Cm(n,f) and {sup 249}Cf(n,gamma){sup 250}Cf capture cross sections at the Laue-Langevin Institute (ILL). It amounts to (15.6+-2.4) b for the first one, (1923+-49) b for the second and (389+-10) b for the third one. (authors)

  7. A moving target: responding to magnetic and structural disorder in lanthanide- and actinide-based superconductors

    Energy Technology Data Exchange (ETDEWEB)

    Bauer, Eric D [Los Alamos National Laboratory; Mitchell, Jeremy N [Los Alamos National Laboratory; Booth, C H [LBNL

    2009-01-01

    The effects of various chemical substitutions and induced lattice disorder in the Ce- and Pu-based 115 superconductors are reviewed, with particular emphasis on results from x-ray absorption fine structure (XAFS) measurements. The competition between spin, charge, and lattice interactions is at the heart of many of the strongly-correlated ground states in materials of current interest, such as in colossal magnetoresistors and high-temperature superconductors. This relationship is particularly strong in the CeTIn{sub 5} and PuTGa{sub 5} series (T = Co, Rh, Ir) of heavy-fermion superconductors. In these systems (figure 1), competition between bulk magnetic and non-magnetic ground states, as well as between superconducting and normal states, are directly related to local properties around the lanthanide or actinide ion, such as the nearest-neighbor bond lengths and the local density of states at the Fermi level. Tiny changes in the latter values can easily tip the balance from one ground state to another. This paper reviews recent work by the authors exploring the relationship between local crystal and electronic structure and ground state magnetic and conducting properties in the Ce- and Pu-based 115 materials.

  8. REVIEW OF EXPERIMENTAL STUDIES INVESTIGATING THE RATE OF STRONTIUM AND ACTINIDE ADSORPTION BY MONOSODIUM TITANATE

    Energy Technology Data Exchange (ETDEWEB)

    Hobbs, D.

    2010-10-01

    A number of laboratory studies have been conducted to determine the influence of mixing and mixing intensity, solution ionic strength, initial sorbate concentrations, temperature, and monosodium titanate (MST) concentration on the rates of sorbate removal by MST in high-level nuclear waste solutions. Of these parameters, initial sorbate concentrations, ionic strength, and MST concentration have the greater impact on sorbate removal rates. The lack of a significant influence of mixing and mixing intensity on sorbate removal rates indicates that bulk solution transport is not the rate controlling step in the removal of strontium and actinides over the range of conditions and laboratory-scales investigated. However, bulk solution transport may be a significant parameter upon use of MST in a 1.3 million-gallon waste tank such as that planned for the Small Column Ion Exchange (SCIX) program. Thus, Savannah River National Laboratory (SRNL) recommends completing the experiments in progress to determine if mixing intensity influences sorption rates under conditions appropriate for this program. Adsorption models have been developed from these experimental studies that allow prediction of strontium (Sr), plutonium (Pu), neptunium (Np) and uranium (U) concentrations as a function of contact time with MST. Fairly good agreement has been observed between the predicted and measured sorbate concentrations in the laboratory-scale experiments.

  9. Fission barriers and half-lives of actinides in the quasimolecular shape valley

    Science.gov (United States)

    Royer, G.; Jaffré, M.; Moreau, D.

    2012-10-01

    The energy of actinide nuclei in the fusionlike deformation valley has been determined from a liquid-drop model, taking into account the proximity energy, the mass and charge asymmetries, and the shell and pairing energies. Double-humped potential barriers appear. The saddle point corresponds to the second maximum and to the transition from compact one-body shapes with a deep neck to two touching ellipsoids. The scission point, where the effects of the nuclear attractive forces between the fragments vanish, lies at the end of an energy plateau below the saddle point and corresponds to two well-separated fragments. The kinetic and excitation energies of the fragments come from the energy on this plateau. The shell and pairing effects play a main role to decide the most probable decay path. The heights of the potential barriers roughly agree with the experimental data and the calculated half-lives follow the trend of the experimental values. A shallow third minimum and a third peak appear in specific asymmetric exit channels where one fragment is close to a double magic quasispherical nucleus, while the other one evolves from oblate to prolate shapes.

  10. Monte Carlo Modeling of Minor Actinide Burning in Fissile Spallation Targets

    Science.gov (United States)

    Malyshkin, Yury; Pshenichnov, Igor; Mishustin, Igor; Greiner, Walter

    2014-06-01

    Minor actinides (MA) present a harmful part of spent nuclear fuel due to their long half-lives and high radio-toxicity. Neutrons produced in spallation targets of Accelerator Driven Systems (ADS) can be used to transmute and burn MA. Non-fissile targets are commonly considered in ADS design. However, additional neutrons from fission reactions can be used in targets made of fissile materials. We developed a Geant4-based code MCADS (Monte Carlo model for Accelerator Driven Systems) for simulating neutron production and transport in different spallation targets. MCADS is suitable for calculating spatial distributions of neutron flux and energy deposition, neutron multiplication factors and other characteristics of produced neutrons and residual nuclei. Several modifications of the Geant4 source code described in this work were made in order to simulate targets containing MA. Results of MCADS simulations are reported for several cylindrical targets made of U+Am, Am or Am2O3 including more complicated design options with a neutron booster and a reflector. Estimations of Am burning rates are given for the considered cases.

  11. 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.

  12. Potential incursion of marine sediment inland during storms: the radiological importance of actinides

    Energy Technology Data Exchange (ETDEWEB)

    Wilkins, B.T.; Green, N.; Haslam, I.K. [National Radiological Protection Board, Chilton, Didcot, Oxon (United Kingdom); Huntley, D.A.; Dyer, K.R.; Cavrot, D.; Tooley, M.J. [Institute for Marine Studies, University of Plymouth, Drake Circus, Plymouth PL44 8AA, Devon (United Kingdom); Zong, Y. [Environmental Research Centre, University of Durham, Science Laboratories, Parks Road, Durham (United Kingdom)

    1999-08-01

    An assessment of the possible future incursion of marine sediment inland in Cumbria and Lancashire has been carried out. The assessment indicated that material from the patch of clay and silt offshore from Sellafield would not be readily mobilised and would not be brought ashore during a single-storm event. Several low-lying areas are potentially at risk of flooding as a result of severe storms, but any marine sediment deposited inland would have come from the nearshore zone. The original assessment, published in 1996, was made using measurement data for 1988. The results indicated that, in many cases, external irradiation was the most important contributor to the doses to those involved in clean-up operations and to residents, {sup 137}Cs being the radionuclide of importance. The predicted doses were a small fraction of the principal limit recommended by ICRP for members of the public. In this paper, the dose estimates have been refined using newly available data for 1995. Since 1988, activity concentrations of {sup 137}Cs have declined markedly because of remobilisation from the sediment, but changes in the values of {sup 241}Am and Pu are much less. As a result, the predicted overall doses to the various population groups are lower than those estimated previously, and in many cases actinides have become the radionuclides of importance. (Copyright (c) 1999 Elsevier Science B.V., Amsterdam. All rights reserved.)

  13. 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.

  14. Interplay of fission modes in mass distribution of light actinide nuclei 225,227Pa

    Directory of Open Access Journals (Sweden)

    R. Dubey

    2016-01-01

    Full Text Available Fission-fragment mass distributions were measured for 225,227Pa nuclei formed in fusion reactions of 19F+206,208Pb around fusion barrier energies. Mass-angle correlations do not indicate any quasi-fission like events in this bombarding energy range. Mass distributions were fitted by Gaussian distribution and mass variance extracted. At below-barrier energies, the mass variance was found to increase with decrease in energy for both nuclei. Results from present work were compared with existing data for induced fission of 224,226Th and 228U around barrier energies. Enhancement in mass variance of 225,227Pa nuclei at below-barrier energies shows evidence for presence of asymmetric fission events mixed with symmetric fission events. This is in agreement with the results of mass distributions of nearby nuclei 224,226Th and 228U where two-mode fission process was observed. Two-mode feature of fission arises due to the shell effects changing the landscape of the potential-energy surfaces at low excitation energies. The excitation-energy dependence of the mass variance gives strong evidence for survival of microscopic shell effects in fission of light actinide nuclei 225,227Pa with initial excitation energy ∼30–50 MeV.

  15. Rapid determination of actinides and {sup 90}Sr in river water

    Energy Technology Data Exchange (ETDEWEB)

    Habibi, A., E-mail: azza.habibi@irsn.fr [IRSN/PRP-ENV/STEME/LMRE, Rue du belvédère, Bâtiment 501, Bois des rames, 91400 Orsay (France); Boulet, B. [IRSN/PRP-ENV/STEME/LMRE, Rue du belvédère, Bâtiment 501, Bois des rames, 91400 Orsay (France); Gleizes, M. [IRSN/PRP-ENV/STEME, 31 rue de l' écluse, 78116 Le Vésinet (France); Larivière, D. [Laboratoire de radioécologie, Département de chimie, Université Laval, 1045 Avenue de la médecine, G1V 0A6 Québec (Canada); Cote, G. [PSL Research University, Chimie ParisTech CNRS, Institut de Recherche de Chimie Paris, 11 rue Pierre et Marie Curie, 75005 Paris (France)

    2015-07-09

    Highlights: • A new method to separate six actinides and {sup 90}Sr was developed. • The method was applied successfully to river water samples. • The separation and the measure take about seven hours. • The method permits to reach high yields. - Abstract: Nuclear accidents occurred in latest years highlighted the difficulty to achieve, in a short time, the quantification of alpha and beta emitters. Indeed, most of the existing methods, though displaying excellent performances, can be very long, taking up to several weeks for some radioisotopes, such as {sup 90}Sr. This study focuses on alpha and beta radioisotopes which could be accidentally released from nuclear installations and which could be measured by inductively coupled plasma mass spectrometer (ICP-MS). Indeed, a new and rapid separation method was developed for {sup 234,235,236,238}U, {sup 230,232}Th, {sup 239,240}Pu, {sup 237}Np, {sup 241}Am and {sup 90}Sr. The main objective was to minimize the duration of the separation protocol by the development of a unique radiochemical procedure with elution media compatible with ICP-MS measurements. Excellent performances were obtained with spiked river water samples. These performances are characterized by total yields exceeding 80% for all monitored radionuclides, as well as good reproducibility (RSD ≤ 10%, n = 12). The proposed radiochemical separation (including counting time) required less than 7 h for a batch of 8 samples.

  16. 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.

  17. Actinide incineration in fusion-fission hybrid-A model nuclear synergy

    Science.gov (United States)

    Taczanowski, Stefan

    2012-06-01

    The alliance of fusion with fission is a cause worthy of great efforts, as being able to ease (if not even to solve) serious problems that both these forms of nuclear energy are facing. Very high investment costs caused by tokamak enormous size, material consumption and difficult technology put in doubt whether alone the minute demand for fuel raw material (Li) and lack of danger of uncontrolled supercriticality prove sufficient for making it competitive. Preliminary evaluations demonstrated that a radical shift of energy production i.e. the energy gain from plasma to fission blanket is feasible [1]. A reduction in the fusion component to about 2% at given system power allows for a radical drop in plasma Q down to the values of ˜0.2-0.3 achievable in small systems [2] (e.g. mirrors) of sizes comparable to fission reactors. As a result in a Fusion-Driven Actinide Incinerator (FDI) both radiations from the plasma: corpuscular (i.e. neutrons and ions) and photons are drastically reduced. Thus are too, first of all - the neutron induced radiation damage: DPA and gas production, then plasma-wall interactions. The fundamental safety of the system has been proved by simulation of its collapse that has shown preservation its subcriticality. Summarizing, all the above problems may be solved with synergic union of fusion with fission embodied in the concept of FDI - small and less expensive.

  18. GCFR Coupled Neutronic and Thermal-Fluid-Dynamics Analyses for a Core Containing Minor Actinides

    Directory of Open Access Journals (Sweden)

    Diego Castelliti

    2009-01-01

    Full Text Available Problems about future energy availability, climate changes, and air quality seem to play an important role in energy production. While current reactor generations provide a guaranteed and economical energy production, new nuclear power plant generation would increase the ways and purposes in which nuclear energy can be used. To explore these new technological applications, several governments, industries, and research communities decided to contribute to the next reactor generation, called “Generation IV.” Among the six Gen-IV reactor designs, the Gas Cooled Fast Reactor (GCFR uses a direct-cycle helium turbine for electricity generation and for a CO2-free thermochemical production of hydrogen. Additionally, the use of a fast spectrum allows actinides transmutation, minimizing the production of long-lived radioactive waste in an integrated fuel cycle. This paper presents an analysis of GCFR fuel cycle optimization and of a thermal-hydraulic of a GCFR-prototype under steady-state and transient conditions. The fuel cycle optimization was performed to assess the capability of the GCFR to transmute MAs, while the thermal-hydraulic analysis was performed to investigate the reactor and the safety systems behavior during a LOFA. Preliminary results show that limited quantities of MA are not affecting significantly the thermal-fluid-dynamics behavior of a GCFR core.

  19. Electronic Structure of Transition Metal Clusters, Actinide Complexes and Their Reactivities

    Energy Technology Data Exchange (ETDEWEB)

    Krishnan Balasubramanian

    2009-07-18

    This is a continuing DOE-BES funded project on transition metal and actinide containing species, aimed at the electronic structure and spectroscopy of transition metal and actinide containing species. While a long term connection of these species is to catalysis and environmental management of high-level nuclear wastes, the immediate relevance is directly to other DOE-BES funded experimental projects at DOE-National labs and universities. There are a number of ongoing gas-phase spectroscopic studies of these species at various places, and our computational work has been inspired by these experimental studies and we have also inspired other experimental and theoretical studies. Thus our studies have varied from spectroscopy of diatomic transition metal carbides to large complexes containing transition metals, and actinide complexes that are critical to the environment. In addition, we are continuing to make code enhancements and modernization of ALCHEMY II set of codes and its interface with relativistic configuration interaction (RCI). At present these codes can carry out multi-reference computations that included up to 60 million configurations and multiple states from each such CI expansion. ALCHEMY II codes have been modernized and converted to a variety of platforms such as Windows XP, and Linux. We have revamped the symbolic CI code to automate the MRSDCI technique so that the references are automatically chosen with a given cutoff from the CASSCF and thus we are doing accurate MRSDCI computations with 10,000 or larger reference space of configurations. The RCI code can also handle a large number of reference configurations, which include up to 10,000 reference configurations. Another major progress is in routinely including larger basis sets up to 5g functions in thee computations. Of course higher angular momenta functions can also be handled using Gaussian and other codes with other methods such as DFT, MP2, CCSD(T), etc. We have also calibrated our RECP

  20. Microbial Transformation of TRU and Mixed Waste: Actinide Speciation and Waste Volume

    Energy Technology Data Exchange (ETDEWEB)

    Halada, Gary P

    2008-04-10

    In order to understand the susceptibility of transuranic and mixed waste to microbial degradation (as well as any mechanism which depends upon either complexation and/or redox of metal ions), it is essential to understand the association of metal ions with organic ligands present in mixed wastes. These ligands have been found in our previous EMSP study to limit electron transfer reactions and strongly affect transport and the eventual fate of radionuclides in the environment. As transuranic waste (and especially mixed waste) will be retained in burial sites and in legacy containment for (potentially) many years while awaiting treatment and removal (or remaining in place under stewardship agreements at government subsurface waste sites), it is also essential to understand the aging of mixed wastes and its implications for remediation and fate of radionuclides. Mixed waste containing actinides and organic materials are especially complex and require extensive study. The EMSP program described in this report is part of a joint program with the Environmental Sciences Department at Brookhaven National Laboratory. The Stony Brook University portion of this award has focused on the association of uranium (U(VI)) and transuranic analogs (Ce(III) and Eu(III)) with cellulosic materials and related compounds, with development of implications for microbial transformation of mixed wastes. The elucidation of the chemical nature of mixed waste is essential for the formulation of remediation and encapsulation technologies, for understanding the fate of contaminant exposed to the environment, and for development of meaningful models for contaminant storage and recovery.

  1. Effect of organic compounds for the advection of actinide elements in the environments

    Energy Technology Data Exchange (ETDEWEB)

    Muraoka, Susumu; Nagao, Seiya; Tanaka, Tadao [Japan Atomic Energy Research Inst., Tokai, Ibaraki (Japan). Tokai Research Establishment; Hiraki, Keizo; Nakaguchi, Yuzuru; Suzuki, Yasuhiro

    1998-01-01

    The aim of this studies is understood the effects of humic substances for the advection of actinide elements in the environments. These substances are a major role of dissolved organic matter in natural waters. In order to obtain the informations on the structure of metal-humic substances complexes, these substances were studied by fluorescence spectroscopy. Observation the spectrum forms, peak positions of maximum intensity are related to these informations on the chemical structures and functional groups in organic compounds. Using three-dimensional excitation emission matrix (3-D EEM) spectroscopy, the characteristics of metal-humic substances complexes were studied. Observation the wavelengths and fluorescence intensity of the peaks were varied between humic substances before the complex to the metal and these substances after ones. Understanding the fluorescence properties of metal-humic substances complexes, working program of the 3-D EEM spectroscopy was studied to obtaining detailed data collection. New program was applied to copper-humic acid complex, the peak positions which different with before the complex and after ones were recorded. This program is supported by the interpreation of fluorescence properties in the metal-humic substances by the 3-D EEM spectroscopy. (author)

  2. 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.

  3. Alloy catalyst material

    DEFF Research Database (Denmark)

    2014-01-01

    The present invention relates to a novel alloy catalyst material for use in the synthesis of hydrogen peroxide from oxygen and hydrogen, or from oxygen and water. The present invention also relates to a cathode and an electrochemical cell comprising the novel catalyst material, and the process use...

  4. Shape Memory Alloy Actuator

    Science.gov (United States)

    Baumbick, Robert J. (Inventor)

    2002-01-01

    The present invention discloses and teaches a unique, remote optically controlled micro actuator particularly suitable for aerospace vehicle applications wherein hot gas, or in the alternative optical energy, is employed as the medium by which shape memory alloy elements are activated. In gas turbine powered aircraft the source of the hot gas may be the turbine engine compressor or turbine sections.

  5. Pareto-optimal alloys

    DEFF Research Database (Denmark)

    Bligaard, Thomas; Johannesson, Gisli Holmar; Ruban, Andrei;

    2003-01-01

    and the cost. In this letter we present a database consisting of the lattice parameters, bulk moduli, and heats of formation for over 64 000 ordered metallic alloys, which has been established by direct first-principles density-functional-theory calculations. Furthermore, we use a concept from economic theory...

  6. Thermodynamic study on the complexation of Trivalent actinide and lanthanide cation by N-donor ligands in homogeneous conditions; Etude thermodynamique de la complexation des ions actinide (III) et lanthanide (III) par des ligands polyazotes en milieu homogene

    Energy Technology Data Exchange (ETDEWEB)

    Miguirditchian, M

    2004-07-01

    Polydentate N-donor ligands, alone or combined with a synergic acid, may selectively extract minor actinides(III) from lanthanide(III) ions, allowing to develop separation processes of long-live radioelements. The aim of the researches carried out during this thesis was to better understand the chemical mechanisms of the complexation of f-elements by Adptz, a tridentate N-donor ligand, in homogeneous conditions. A thermodynamic approach was retained in order to estimate, from an energetic point of view, the influence of the different contributions to the reaction, and to acquire a complete set of thermodynamic data on this reaction. First, the influence of the nature of the cation on the thermodynamics was considered. The stability constants of the 1/1 complexes were systematically determined by UV-visible spectrophotometry for every lanthanide ion (except promethium) and for yttrium in a mixed solvent methanol/water in volume proportions 75/25%. The thermodynamic parameters ({delta}H{sup 0} {delta}{sup S}) of complexation were estimated by the van't Hoff method and by micro-calorimetry. The trends of the variations across the lanthanide series are compared with similar studies. The same methods were applied to the study of three actinide(III) cations: plutonium, americium and curium. The comparison of these values with those obtained for the lanthanides highlights the increase of stability of these complexes by a factor of 20 in favor of the actinide cations. This gap is explained by a more exothermic reaction and is associated, in the data interpretation, to a higher covalency of the actinide(III)-nitrogen bond. Then, the influence of the change of solvent composition on the thermodynamic of complexation was studied. The thermodynamic parameters of the complexation of europium(III) by Adptz were determined for several fractions of methanol. The stability of the complex formed increases with the percentage of methanol in the mixed solvent, owing to an

  7. 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.

  8. Advanced ordered intermetallic alloy deployment

    Energy Technology Data Exchange (ETDEWEB)

    Liu, C.T.; Maziasz, P.J.; Easton, D.S. [Oak Ridge National Lab., TN (United States)

    1997-04-01

    The need for high-strength, high-temperature, and light-weight materials for structural applications has generated a great deal of interest in ordered intermetallic alloys, particularly in {gamma}-based titanium aluminides {gamma}-based TiAl alloys offer an attractive mix of low density ({approximately}4g/cm{sup 3}), good creep resistance, and high-temperature strength and oxidation resistance. For rotating or high-speed components. TiAl also has a high damping coefficient which minimizes vibrations and noise. These alloys generally contain two phases. {alpha}{sub 2} (DO{sub 19} structure) and {gamma} (L 1{sub 0}), at temperatures below 1120{degrees}C, the euticoid temperature. The mechanical properties of TiAl-based alloys are sensitive to both alloy compositions and microstructure. Depending on heat-treatment and thermomechanical processing, microstructures with near equiaxed {gamma}, a duplex structure (a mix of the {gamma} and {alpha}{sub 2} phases) can be developed in TiAl alloys containing 45 to 50 at. % Al. The major concern for structural use of TiAl alloys is their low ductility and poor fracture resistance at ambient temperatures. The purpose of this project is to improve the fracture toughness of TiAl-based alloys by controlling alloy composition, microstructure and thermomechanical treatment. This work is expected to lead to the development of TiAl alloys with significantly improved fracture toughness and tensile ductility for structural use.

  9. 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

  10. 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.

  11. Separation of lanthanides and actinides(III) using tridentate benzimidazole, benzoxazole and benzothiazole ligands

    Energy Technology Data Exchange (ETDEWEB)

    Drew, M.G.B.; Hudson, M.J.; Iveson, P.B.; Vaillant, L.; Youngs, T.G.A. [Reading Univ. (United Kingdom). Dept. of Chemistry; Hill, C.; Madic, Ch. [CEA Valrho, Dir. de l' Energie Nucleaire, Departement RadioChimie et Procedes, Service de Chimie des Procedes de Separation (DEN/DRCP/SCPS/LCSE), 30 - Marcoule (France)

    2004-04-01

    The ability of new hydrophobic tridentate ligands based on 2,6-bis(benzimidazole-2-yl)pyridine, 2,6-bis(benzoxazole-2-yl)pyridine and 2,6-bis(benzothiazole-2-yl)pyridine to selectively extract americium(III) from europium(III) was measured. The most promising ligand - 2,6-bis(benzoxazole-2-yl)-4-(2-decyl-1-tetra-decyl-oxy)pyridine L{sup 9} was found to give separation factors (SF{sub Am/Eu}) of up to 70 when used to extract cations from 0.02-0.10 M HNO{sub 3} into TPH in synergy with 2-bromo-decanoic acid. Six structures of lanthanide complexes with 2,6-bis(benzoxazole-2-yl)pyridine L{sup 6} were then determined to evaluate the types of species that are likely to be involved in the separation process. Three structural types were observed, namely [LnL{sup 6}(NO{sub 3}){sub 3}(H{sub 2}O){sub 2}), 11-coordinate only for La, [LnL{sup 6}(NO{sub 3})3 (CH{sub 3}CN)], 10-coordinate for Pr, Nd and Eu and [LnL{sup 6}(NO{sub 3}){sub 3}(H{sub 2}O)], L 10-coordinate for Eu and Gd. Quantum Mechanics calculations were carried out on the tridentate ligands to elucidate the conformational preferences of the ligands in the free state and protonated and di-protonated forms and to assess the electronic properties of the ligands for comparison with other ter-dentate ligands used in lanthanide/actinide separation processes. (authors)

  12. 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

  13. Wavelength Dispersive X-ray Fluorescence Analysis of Actinides in Dissolved Nuclear Fuels

    Energy Technology Data Exchange (ETDEWEB)

    O' Hara, David [Parallax Research, Inc., Tallahassee, FL (United States)

    2015-10-15

    There is an urgent need for an instrument that can quickly measure the concentration of Plutonium and other Actinides mixed with Uranium in liquids containing dissolved spent fuel rods. Parallax Research, Inc. proposes to develop an x-ray spectrometer capable of measuring U, Np and Pu in dissolved nuclear fuel rod material to less than 10 ppm levels to aid in material process control for these nuclear materials. Due to system noise produced by high radioactivity, previous x-ray spectrometers were not capable of low level measurements but the system Parallax proposed has no direct path for undesired radiation to get to the detector and the detector in the proposed device is well shielded from scatter and has very low dark current. In addition, the proposed spectrometer could measure these three elements simultaneously, also measuring background positions with an energy resolution of roughly 100 eV making it possible to see a small amount of Pu that would be hidden under the tail of the U peak in energy dispersive spectrometers. Another nearly identical spectrometer could be used to target Am and Cm if necessary. The proposed spectrometer needs only a tiny sample of roughly 1 micro-liter (1 mm3) and the measurement can be done with the liquid flowing in a radiation and chemical immune quartz capillary protected by a stainless steel rod making it possible to continuously monitor the liquid or to use a capillary manifold to measure other liquid streams. Unlike other methods such as mass spectroscopy where the sample must be taken to a remote facility and might take days for turn-around, the proposed measurement should take less than an hour. This spectrometer could enable near real-time measurement of U, Pu and Np in dilute dissolved spent nuclear fuel rod streams.

  14. Microbial diversity in opalinus clay and interaction of dominant microbial strains with actinides

    Energy Technology Data Exchange (ETDEWEB)

    Moll, Henry; Luetke, Laura; Bachvarova, Velina; Steudtner, Robin; Geissler, Andrea; Krawczyk-Baersch, Evelyn; Selenska-Pobell, Sonja; Bernhardt, Gert

    2013-07-01

    For the first time microbial tDNA could be isolated from 50 g unperturbed Mont Terri Opalinus Clay. Based on the analysis of the tDNA the bacterial diversity of the unperturbed clay is dominated by representatives of Firmicutes, Betaproteobacteria, and Bacteriodetes. Firmicutes also dominate after treatment of the clay with R2A medium. Bacteria isolated from Mont Terri Opalinus Clay on R2A medium were related to Sporomusa spp., Paenibacillus spp., and Clostridium spp. All further investigations are concentrated on the unique isolates Sporomusa sp. MT-2 and Paenibacillus sp. MT-2. Cells of the type Sporomusa sp. MT-2 and Paenibacillus sp. MT-2 were comprehensively analyzed in terms of growing, morphology, functional groups of the cell envelope, and cell membrane structure. Strong actinide(An)/lanthanide(Ln)-interactions with the Opalinus Clay isolates and the Aespoe-strain Pseudomonas fluorescens (CCUG 32456) could be determined within a broad pH range (2-8). The metals bind as a function of pH on protonated phosphoryl, carboxyl and deprotonated phosphoryl sites of the respective cell membrane. The thermodynamic surface complexation constants of bacterial An/Ln-species were determined and can be used in modeling programs. Depending on the used An different interaction mechanisms were found (U(VI): biosorption, partly biomineralisation; Cm(III): biosorption, indications for embedded Cm(III); Pu: biosorption, bioreduction and indications for embedded Pu). Different strategies of coping with U(VI) were observed comparing P. fluorescens planktonic cells and biofilms under the chosen experimental conditions. An enhanced capability of the biofilm to form meta-autunite in comparison to the planktonic cells was proven. Conclusively, the P. fluorescens biofilm is more efficient in U(VI) detoxification. In conclusion, Mont Terri Opalinus Clay contains bacterial communities, that may influence the speciation and hence the migration behavior of selected An/Ln under

  15. Analyses in Support of Z-Pinch IFE and Actinide Transmutation - LLNL Progress Report for FY-06

    Energy Technology Data Exchange (ETDEWEB)

    Meier, W R; Moir, R W; Abbott, R

    2006-09-19

    This report documents results of LLNL's work in support of two studies being conducted by Sandia National Laboratories (SNL): the development of the Z-pinch driven inertial fusion energy (Z-IFE), and the use of Z-pinch driven inertial fusion as a neutron source to destroy actinides from fission reactor spent fuel. LLNL's efforts in FY06 included: (1) Development of a systems code for Z-IFE and use of the code to examine the operating parameter space in terms of design variables such as the Z-pinch driver energy, the chamber pulse repetition rate, the number of chambers making up the power plant, and the total net electric power of the plant. This is covered in Section 3 with full documentation of the model in Appendix A. (2) Continued development of innovative concepts for the design and operation of the recyclable transmission line (RTL) and chamber for Z-IFE. The work, which builds on our FY04 and FY05 contributions, emphasizes design features that are likely to lead to a more attractive power plant including: liquid jets to protect all structures from direct exposure to neutrons, rapid insertion of the RTL to maximize the potential chamber rep-rate, and use of cast flibe for the RTL to reduce recycling and remanufacturing costs and power needs. See Section 4 and Appendix B. (3) Description of potential figures of merit (FOMs) for actinide transmutation technologies and a discussion of how these FOMs apply and can be used in the ongoing evaluation of the Z-pinch actinide burner, referred to as the In-Zinerator. See Section 5. (4) A critique of, and suggested improvements to, the In-Zinerator chamber design in response to the SNL design team's request for feedback on its preliminary design. This is covered in Section 6.

  16. High-Pressure Synthesis and Characterization of New Actinide Borates, AnB4O8 (An=Th, U)

    Science.gov (United States)

    Hinteregger, Ernst; Hofer, Thomas S; Heymann, Gunter; Perfler, Lukas; Kraus, Florian; Huppertz, Hubert

    2013-01-01

    New actinide borates ThB4O8 and UB4O8 were synthesized under high-pressure, high-temperature conditions (5.5 GPa/1100 °C for thorium borate, 10.5 GPa/1100 °C for the isotypic uranium borate) in a Walker-type multianvil apparatus from their corresponding actinide oxide and boron oxide. The crystal structure was determined on basis of single-crystal X-ray diffraction data that were collected at room temperature. Both compounds crystallized in the monoclinic space group C2/c (Z=4). Lattice parameters for ThB4O8: a=1611.3(3), b=419.86(8), c=730.6(2) pm; β=114.70(3)°; V=449.0(2) Å3; R1=0.0255, wR2=0.0653 (all data). Lattice parameters for UB4O8: a=1589.7(3), b=422.14(8), c=723.4(2) pm; β=114.13(3)°; V=443.1(2) Å3; R1=0.0227, wR2=0.0372 (all data). The new AnB4O8 (An=Th, U) structure type is constructed from corner-sharing BO4 tetrahedra, which form layers in the bc plane. One of the four independent oxygen atoms is threefold-coordinated. The actinide cations are located between the boron–oxygen layers. In addition to Raman spectroscopic investigations, DFT calculations were performed to support the assignment of the vibrational bands. PMID:24123698

  17. High-pressure synthesis and characterization of new actinide borates, AnB4O8 (An=Th, U).

    Science.gov (United States)

    Hinteregger, Ernst; Hofer, Thomas S; Heymann, Gunter; Perfler, Lukas; Kraus, Florian; Huppertz, Hubert

    2013-11-18

    New actinide borates ThB4O8 and UB4O8 were synthesized under high-pressure, high-temperature conditions (5.5 GPa/1100 °C for thorium borate, 10.5 GPa/1100 °C for the isotypic uranium borate) in a Walker-type multianvil apparatus from their corresponding actinide oxide and boron oxide. The crystal structure was determined on basis of single-crystal X-ray diffraction data that were collected at room temperature. Both compounds crystallized in the monoclinic space group C2/c (Z=4). Lattice parameters for ThB4O8: a=1611.3(3), b=419.86(8), c=730.6(2) pm; β=114.70(3)°; V=449.0(2) Å(3); R1=0.0255, wR2=0.0653 (all data). Lattice parameters for UB4O8: a=1589.7(3), b=422.14(8), c=723.4(2) pm; β=114.13(3)°; V=443.1(2) Å(3); R1=0.0227, wR2=0.0372 (all data). The new AnB4O8 (An=Th, U) structure type is constructed from corner-sharing BO4 tetrahedra, which form layers in the bc plane. One of the four independent oxygen atoms is threefold-coordinated. The actinide cations are located between the boron-oxygen layers. In addition to Raman spectroscopic investigations, DFT calculations were performed to support the assignment of the vibrational bands.

  18. Monazite-type ceramics for conditioning of minor actinides. Structural characterization and properties

    Energy Technology Data Exchange (ETDEWEB)

    Babelot, Carole

    2013-07-01

    The minor actinides (MA) neptunium, americium, and curium are mainly responsible for the long-term radiotoxicity of the High Active Waste (HAW) generated during the nuclear power operation. If these long-lived radionuclides are removed from the HAW by partitioning and converted by neutron fission (transmutation) into shorter-lived or stable elements, the remaining waste loses most of its long-term radiotoxicity. Thus, partitioning and transmutation (P and T) are considered as attractive options for reducing the burden on geological disposals. As an alternative, these separated MA can also be conditioned (P and C strategy) in specifically adapted ceramics to ensure their safe final disposal over long periods. At the moment, spent fuel elements are foreseen either for direct disposal in deep geological repositories or for reprocessing. The highly active liquid waste that is produced during reprocessing is conditioned industrially using a vitrification process before final disposal. Although the widely used borosilicate glasses meet most of the specifications needed, ceramic host matrices appear to be even more suitable in terms of resistance to corrosion. The development of new materials based on tailor-made highly specific ceramics with extremely stable behavior would make it possible to improve the final storage of long-lived high-level radiotoxic waste. In the framework of this PhD research project, monazite-type ceramics were chosen as promising host matrices for the conditioning of trivalent actinides. The focus on the monazite-type ceramics is justified by their properties such as high chemical durability. REPO{sub 4} ceramics are named monazite for RE = La - Gd (monoclinic symmetry) and xenotime for RE = Tb - Lu and Y (tetragonal symmetry). The objective of this study is to contribute to the understanding of the alteration behavior of such ceramics under the repository conditions. REPO{sub 4} (with RE = La, Eu) is prepared by hydrothermal synthesis at 200 C

  19. Tungsten carbide laser alloying of a low alloyed steel

    Science.gov (United States)

    Cojocaru, Mihai; Taca, Mihaela

    1996-10-01

    Laser alloying is a way to change the composition of metal surfaces in order to improve their corrosion-resistance, high-temperature strength and hardness. The results of a structural and phase analysis of a tungsten carbide based surface layer prepared by laser alloying of a low carbon steel substrate are presented. Structure, phase composition and microhardness of surface alloyed layers have been investigated. The surface of the samples exhibited a thin layer with a different chemical and phase composition. An increase in alloyed surface hardness and wear-resistance was observed.

  20. Filler metal alloy for welding cast nickel aluminide alloys

    Science.gov (United States)

    Santella, M.L.; Sikka, V.K.

    1998-03-10

    A filler metal alloy used as a filler for welding cast nickel aluminide alloys contains from about 15 to about 17 wt. % chromium, from about 4 to about 5 wt. % aluminum, equal to or less than about 1.5 wt. % molybdenum, from about 1 to about 4.5 wt. % zirconium, equal to or less than about 0.01 wt. % yttrium, equal to or less than about 0.01 wt. % boron and the balance nickel. The filler metal alloy is made by melting and casting techniques such as are melting the components of the filler metal alloy and cast in copper chill molds. 3 figs.

  1. Filler metal alloy for welding cast nickel aluminide alloys

    Energy Technology Data Exchange (ETDEWEB)

    Santella, Michael L. (Knoxville, TN); Sikka, Vinod K. (Oak Ridge, TN)

    1998-01-01

    A filler metal alloy used as a filler for welding east nickel aluminide alloys contains from about 15 to about 17 wt. % chromium, from about 4 to about 5 wt. % aluminum, equal to or less than about 1.5 wt. % molybdenum, from about 1 to about 4.5 wt. % zirconium, equal to or less than about 0.01 wt. % yttrium, equal to or less than about 0.01 wt. % boron and the balance nickel. The filler metal alloy is made by melting and casting techniques such as are melting the components of the filler metal alloy and east in copper chill molds.

  2. Materials data handbook, Inconel alloy 718

    Science.gov (United States)

    Sessler, J.; Weiss, V.

    1967-01-01

    Materials data handbook on Inconel alloy 718 includes data on the properties of the alloy at cryogenic, ambient, and elevated temperatures and other pertinent engineering information required for the design and fabrication of components and equipment utilizing this alloy.

  3. SINTERED REFRACTORY TUNGSTEN ALLOYS. Gesinterte hochschmelzende wolframlegierungen

    Energy Technology Data Exchange (ETDEWEB)

    Kieffer, R.; Sedlatschek, K.; Braun, H.

    1971-12-15

    Dependence of the melting point of the refractory metals on their positions in the periodic system - alloys of tungsten with other refractory metals - sintering of the alloys - processing of the alloys - technological properties.

  4. Hydration Gibbs free energies of open and closed shell trivalent lanthanide and actinide cations from polarizable molecular dynamics.

    Science.gov (United States)

    Marjolin, Aude; Gourlaouen, Christophe; Clavaguéra, Carine; Ren, Pengyu Y; Piquemal, Jean-Philip; Dognon, Jean-Pierre

    2014-10-01

    The hydration free energies, structures, and dynamics of open- and closed-shell trivalent lanthanide and actinide metal cations are studied using molecular dynamics simulations (MD) based on a polarizable force field. Parameters for the metal cations are derived from an ab initio bottom-up strategy. MD simulations of six cations solvated in bulk water are subsequently performed with the AMOEBA polarizable force field. The calculated first-and second shell hydration numbers, water residence times, and free energies of hydration are consistent with experimental/theoretical values leading to a predictive modeling of f-elements compounds.

  5. Spectroscopy of neutron rich nuclei using cold neutron induced fission of actinide targets at the ILL: The EXILL campaign

    Directory of Open Access Journals (Sweden)

    Blanc A.

    2013-12-01

    Full Text Available One way to explore exotic nuclei is to study their structure by performing γ-ray spectroscopy. At the ILL, we exploit a high neutron flux reactor to induce the cold fission of actinide targets. In this process, fission products that cannot be accessed using standard spontaneous fission sources are produced with a yield allowing their detailed study using high resolution γ-ray spectroscopy. This is what was pursued at the ILL with the EXILL (for EXOGAM at the ILL campaign. In the present work, the EXILL setup and performance will be presented.

  6. Atomistic Calculations of the Effect of Minor Actinides on Thermodynamic and Kinetic Properties of UO{sub 2{+-}x}

    Energy Technology Data Exchange (ETDEWEB)

    Deo, Chaitanya; Adnersson, Davis; Battaile, Corbett; uberuaga, Blas

    2012-10-30

    The team will examine how the incorporation of actinide species important for mixed oxide (MOX) and other advanced fuel designs impacts thermodynamic quantities of the host UO{sub 2} nuclear fuel and how Pu, Np, Cm and Am influence oxygen mobility. In many cases, the experimental data is either insufficient or missing. For example, in the case of pure NpO2, there is essentially no experimental data on the hyperstoichiometric form it is not even known if hyperstoichiometry NpO{sub 2{+-}x} is stable. The team will employ atomistic modeling tools to calculate these quantities

  7. Determination of Uncertainties for +III and +IV Actinide Solubilities in the WIPP Geochemistry Model for the 2009 Compliance Recertification Application

    Science.gov (United States)

    Ismail, A. E.; Xiong, Y.; Nowak, E. J.; Brush, L. H.

    2009-12-01

    The Waste Isolation Pilot Plant (WIPP) is a U.S. Department of Energy (DOE) repository in southeast New Mexico for defense-related transuranic (TRU) waste. Every five years, the DOE is required to submit an application to the Environmental Protection Agency (EPA) demonstrating the WIPP’s continuing compliance with the applicable EPA regulations governing the repository. Part of this recertification effort involves a performance assessment—a probabilistic evaluation of the repository performance with respect to regulatory limits on the amount of releases from the repository to the accessible environment. One of the models used as part of the performance assessment process is a geochemistry model, which predicts solubilities of the radionuclides in the brines that may enter the repository in the different scenarios considered by the performance assessment. The dissolved actinide source term comprises actinide solubilities, which are input parameters for modeling the transport of radionuclides as a result of brine flow through and from the repository. During a performance assessment, the solubilities are modeled as the product of a “base” solubility determined from calculations based on the chemical conditions expected in the repository, and an uncertainty factor that describes the potential deviations of the model from expected behavior. We will focus here on a discussion of the uncertainties. To compute a cumulative distribution function (CDF) for the uncertainties, we compare published, experimentally measured solubility data to predictions made using the established WIPP geochemistry model. The differences between the solubilities observed for a given experiment and the calculated solubilities from the model are used to form the overall CDF, which is then sampled as part of the performance assessment. We will discuss the methodology used to update the CDF’s for the +III actinides, obtained from data for Nd, Am, and Cm, and the +IV actinides, obtained

  8. High-temperature Titanium Alloys

    Directory of Open Access Journals (Sweden)

    A.K. Gogia

    2005-04-01

    Full Text Available The development of high-temperature titanium alloys has contributed significantly to the spectacular progress in thrust-to-weight ratio of the aero gas turbines. This paper presents anoverview on the development of high-temperature titanium alloys used in aero engines and potential futuristic materials based on titanium aluminides and composites. The role of alloychemistry, processing, and microstructure, in determining the mechanical properties of titanium alloys is discussed. While phase equilibria and microstructural stability consideration haverestricted the use of conventional titanium alloys up to about 600 "C, alloys based on TiPl (or,, E,AINb (0, TiAl (y, and titaniumltitanium aluminides-based composites offer a possibility ofquantum jump in the temperature capability of titanium alloys.

  9. Aqueous complexation of trivalent lanthanide and actinide cations by N,N,N'{sub 2},N'-tetrakis(2-pyridylmethyl)ethylenediamine.

    Energy Technology Data Exchange (ETDEWEB)

    Beitz, J. V.; Ensor, D. D.; Jensen, M. P.; Morss, L. R.

    1999-06-16

    The aqueous complexation reactions of trivalent lanthanide and actinide cations with the hexadentate ligand N,N,N{prime},N{prime}-tetrakis(2-pyridylmethyl)ethylenediamine (TPEN), have been characterized using potentiometric and spectroscopic techniques in 0.1 M NaClO{sub 4} At 25 C, the stability constant of Am(TPEN){sup 3+} is two orders of magnitude larger than that of Sm(TPEN){sup 3+}, reflecting the stronger interactions of the trivalent actinide cations with softer ligands as compared to lanthanide cations.

  10. Numerical analysis on reduction of radioactive actinides by recycling of nuclear fuel; Analisis numerico sobre reduccion de actinidos radiactivos por reciclado de combustible nuclear

    Energy Technology Data Exchange (ETDEWEB)

    Balboa L, H. E.

    2014-07-01

    Worldwide, human growth has reached unparalleled levels historically, this implies a need for more energy, and just in 2007 was consumed in the USA 4157 x 10{sup 9} kWh of electricity and there were 6 x 10{sup 9} metric tons of carbon dioxide, which causes a devastating effect on our environment. To this problem, a solution to the demand for non-fossil energy is nuclear energy, which is one of the least polluting and the cheapest among non-fossil energy; however, a problem remains unresolved the waste generation of nuclear fuels. In this work the option of a possible transmutation of actinides in a nuclear reactor of BWR was analyzed, an example of this are the nuclear reactors at the Laguna Verde nuclear power plant, which have generated spent fuel stored in pools awaiting a decision for final disposal or any other existing alternative. Assuming that the spent fuel was reprocessed to separate useful materials and actinides such as plutonium and uranium remaining, could take these actinides and to recycle them inside the same reactor that produced them, so il will be reduced the radiotoxicity of spent fuel. The main idea of this paper is to evaluate by means of numeric simulation (using the Core Management System (CMS)) the reduction of minor actinides in the case of being recycled in fresh fuel of the type BWR. The actinides were introduced hypothetically in the fuel pellets to 6% by weight, and then use a burned in the range of 0-65 G Wd/Tm, in order to have a better panorama of their behavior and thus know which it is the best choice for maximum reduction of actinides. Several cases were studied, that is to say were used as fuels; the UO{sub 2} and MOX. Six different cases were also studied to see the behavior of actinides in different situations. The CMS platform calculation was used for the analysis of the cases presented. Favorable results were obtained, having decreased from a range of 35% to 65% of minor actinides initially introduced in the fuel rods

  11. Effect of oxidation state and ionic strength on sorption of actinides (Th, U, Np, Am) to geologic media [Abstract and References Only

    Energy Technology Data Exchange (ETDEWEB)

    Dittrich, Timothy M. [Los Alamos National Lab. (LANL), Los Alamos, NM (United States); Richmann, Michael K. [Los Alamos National Lab. (LANL), Los Alamos, NM (United States); Reed, Donald T. [Los Alamos National Lab. (LANL), Los Alamos, NM (United States)

    2015-10-30

    The degree of conservatism in the estimated sorption partition coefficients (Kds) used in a performance assessment model is being evaluated based on a complementary batch and column method. The main focus of this work is to investigate the role of ionic strength, solution chemistry, and oxidation state (III-VI) in actinide sorption to dolomite rock. Based on redox conditions and solution chemistry expected at the WIPP, possible actinide species include Pu(III), Pu(IV), U(IV), U(VI), Np(IV), Np(V), Am(III), and Th(IV).

  12. Multicomponent and High Entropy Alloys

    Directory of Open Access Journals (Sweden)

    Brian Cantor

    2014-08-01

    Full Text Available This paper describes some underlying principles of multicomponent and high entropy alloys, and gives some examples of these materials. Different types of multicomponent alloy and different methods of accessing multicomponent phase space are discussed. The alloys were manufactured by conventional and high speed solidification techniques, and their macroscopic, microscopic and nanoscale structures were studied by optical, X-ray and electron microscope methods. They exhibit a variety of amorphous, quasicrystalline, dendritic and eutectic structures.

  13. Porosity of porous Al alloys

    Institute of Scientific and Technical Information of China (English)

    2001-01-01

    Two porosity models of porous Al alloys with different pore types (ball and polygon shape) were established. The experimental results coincide well with theoretical computations. The porosity of Al alloys (Prc) consists of three parts, porosity caused by preform particles (Prp), additional porosity (Pra), and porosity caused by solidification shrinkage (Prs). Prp is the main part of Prc while Pra is the key for fabricating porous Al alloys successfully in spite of its little contribution to Prc.

  14. Duct and cladding alloy

    Science.gov (United States)

    Korenko, Michael K.

    1983-01-01

    An austenitic alloy having good thermal stability and resistance to sodium corrosion at 700.degree. C. consists essentially of 35-45% nickel 7.5-14% chromium 0.8-3.2% molybdenum 0.3-1.0% silicon 0.2-1.0% manganese 0-0.1% zirconium 2.0-3.5% titanium 1.0-2.0% aluminum 0.02-0.1% carbon 0-0.01% boron and the balance iron.

  15. Analysis of laser alloyed surfaces

    Energy Technology Data Exchange (ETDEWEB)

    Jacobson, D.C.; Augustyniak, W.M.; Buene, L.; Draper, C.W.; Poate, J.M.

    1981-04-01

    Surface alloys of precious metals have many advantages over bulk alloys, the most obvious of which is cost reduction due to the reduced consumption of precious metal. There are several techniques for producing surface alloys. In this paper the laser irradiation technique is presented. The following lasers: CW CO/sub 2/, Q-switched Nd-YAG, frequency double Q-switched Nd-YAG, and pulsed ruby were used to irradiate and melt thin solid films of precious metals on metal substrates. This causes the surfaces to melt to a depth of approximately 10,000A. Alloying then takes place in the liquid phase where most metals are miscible. The high quench rates obtainable by this method of melting can result in the forming of metastable alloys. This melting and regrowth process is well understood and has been discussed in the literature over the last few years. This paper deals with two binary alloy systems, Au-Ni and Pd-Ti. Surface alloys of Au-Ni with a wide range of concentrations have been produced by laser irradiation of thin Au films on Ni. These films have been analyzed using Rutherford backscattering (RBS) and channeling. Many thin film metals other than Au have also been successfully alloyed using these methods. An example of a potential application is the laser surface alloying of Pd to Ti for corrosion passivation.

  16. Hybrid conducting polymer materials incorporating poly-oxo-metalates for extraction of actinides; Materiaux polymeres conducteurs hybrides incorporant des polyoxometallates pour l'extraction d'actinides

    Energy Technology Data Exchange (ETDEWEB)

    Racimor, D

    2003-09-15

    The preparation and characterization of hybrid conducting polymers incorporating poly-oxo-metalates for extracting actinides is discussed. A study of the coordination of various lanthanide cations (Ce(III), Ce(IV), Nd(III)) by the mono-vacant poly-oxo-metalate {alpha}{sub 2}-[P{sub 2}W{sub 17}O{sub 61}]{sup 10-} showed significant differences according to the cation.. Various {alpha}-A-[PW{sub 9}O{sub 34}(RPO){sub 2}]{sup 5-} hybrids were synthesized and their affinity for actinides or lanthanides was demonstrated through complexation. The first hybrid poly-oxo-metallic lanthanide complexes were then synthesized, as was the first hybrid functionalized with a pyrrole group. The electro-polymerization conditions of this pyrrole remain still to be optimized. Poly-pyrrole materials incorporating {alpha}{sub 2}-[P{sub 2}W{sub 17}O{sub 61}]{sup 10-} or its neodymium or cerium complexes as doping agents proved to be the first conducting polymer incorporating poly-oxo-metalates capable of extracting plutonium from nitric acid. (author)

  17. Elaboration of extracting, incinerable and/or conducting resins, for the grouped conversion of actinides; Conception de resines extractantes, incinerables et/ou conductrices, pour la conversion groupee d'actinides

    Energy Technology Data Exchange (ETDEWEB)

    Mokhtari, H. [Paris-11 Univ., 91 - Orsay (France)]|[CEA Valrho, Lab. de Chimie des Actinides (LCA), 30 - Marcoule (France)

    2006-07-01

    The first results obtained in the framework of the study called PEACE (Process for the Elaboration of Actinide Carbide from ion Exchange resin) concern the fixation of neodymium(III) (simulating trivalent actinides) on two carboxylic resins: the first one is of gel type and the second one of macroporous type. A kinetic study of the exchange NH{sub 4}{sup +}/Nd{sup 3+} has shown that: 1)neodymium is fixed under the form of a complexed or hydrolyzed specie of neodymium of charge 2+ 2)a high charge rate is reached (40% in mass for the dried resin which corresponds to an exchange capacity of 11 meq/g dry of introduced resin) 3)the exchange kinetics is better for the macroporous resin than for the gel resin. A heat treatment of the macroporous resin charged in neodymium has been carried out until the carbonization by the mean of thermal gravimetric analyses carried out under air and argon. A carbon/neodymium ratio of about 5 is obtained after carbonization under argon. Scanning electron microscopy analyses carried out on the macroporous resin charged in neodymium have revealed a conservation of the sphericity and a consequent reduction of the resin balls diameter after heat treatment and an homogeneous distribution of neodymium inside the sphere. (O.M.)

  18. Intergranular tellurium cracking of nickel-based alloys in molten Li, Be, Th, U/F salt mixture

    Energy Technology Data Exchange (ETDEWEB)

    Ignatiev, Victor, E-mail: ignatiev@vver.kiae.ru; Surenkov, Alexander; Gnidoy, Ivan; Kulakov, Alexander; Uglov, Vadim; Vasiliev, Alexander; Presniakov, Mikhail

    2013-09-15

    In Russia, R and D on Molten Salt Reactor (MSR) are concentrated now on fast/intermediate spectrum concepts which were recognized as long term alternative to solid fueled fast reactors due to their attractive features: strong negative feedback coefficients, easy in-service inspection, and simplified fuel cycle. For high-temperature MSR corrosion of the metallic container alloy in primary circuit is the primary concern. Key problem receiving current attention include surface fissures in Ni-based alloys probably arising from fission product tellurium attack. This paper summarizes results of corrosion tests conducted recently to study effect of oxidation state in selected fuel salt on tellurium attack and to develop means of controlling tellurium cracking in the special Ni-based alloys recently developed for molten salt actinide recycler and tranforming (MOSART) system. Tellurium corrosion of Ni-based alloys was tested at temperatures up to 750 °C in stressed and unloaded conditions in molten LiF–BeF{sub 2} salt mixture fueled by about 20 mol% of ThF{sub 4} and 2 mol% of UF{sub 4} at different [U(IV)]/[U(III)] ratios: 0.7, 4, 20, 100 and 500. Following Ni-based alloys (in mass%): HN80M-VI (Mo—12, Cr—7.6, Nb—1.5), HN80MTY (Mo—13, Cr—6.8, Al—1.1, Ti—0.9), HN80MTW (Mo—9.4, Cr—7.0, Ti—1.7, W—5.5) and EM-721 (W—25.2, Cr—5.7, Ti—0.17) were used for the study in the corrosion facility.

  19. Oligocrystalline shape memory alloys

    Energy Technology Data Exchange (ETDEWEB)

    Ueland, Stian M.; Chen, Ying; Schuh, Christopher A. [Department of Materials Science and Engineering, Massachusetts Institute of Technology, 77 Massachusetts Avenue, Cambridge, MA 02139 (United States)

    2012-05-23

    Copper-based shape memory alloys (SMAs) exhibit excellent shape memory properties in single crystalline form. However, when they are polycrystalline, their shape memory properties are severely compromised by brittle fracture arising from transformation strain incompatibility at grain boundaries and triple junctions. Oligocrystalline shape memory alloys (oSMAs) are microstructurally designed SMA structures in which the total surface area exceeds the total grain boundary area, and triple junctions can even be completely absent. Here it is shown how an oligocrystalline structure provides a means of achieving single crystal-like SMA properties without being limited by constraints of single crystal processing. Additionally, the formation of oSMAs typically involves the reduction of the size scale of specimens, and sample size effects begin to emerge. Recent findings on a size effect on the martensitic transformation in oSMAs are compared and a new regime of heat transfer associated with the transformation heat evolution in these alloys is discussed. New results on unassisted two-way shape memory and the effect of loading rate in oSMAs are also reported. (Copyright copyright 2012 WILEY-VCH Verlag GmbH and Co. KGaA, Weinheim)

  20. Aluminum alloy impact sparkling

    Directory of Open Access Journals (Sweden)

    M. Dudyk

    2008-08-01

    Full Text Available The cast machine parts are widely used in many branches of industry. A very important issue is gaining the appropriate knowledge relating to the application of castings in places of explosion risks including but not limited to mining, chemical industry and rescue works. A possibility of explosion risks occurrence following the impact sparkling of the cast metal parts is still not solved problem in scientific research. In relation to this issue, in this article, the results of the study are presented, and relating to the tendency to impact sparkling of the aluminium alloys used in machine building. On the grounds of the results obtained, it was demonstrated that the registered impact sparkles bunches of feathers from the analyzed alloys: AlSi7Mg, (AK7; AlSi9Mg, (AK9; AlSi6Cu4, (AK64 and AlSi11, (AK11 show significant differences between each other. The quantitative analysis of the temperature distribution and nuclei surface area performed on the example of the alloy AK9 (subjected to defined period of corrosion allows for the statement that they are dangerous in conditions of explosion risk. Following this fact, designers and users of machine parts made from these materials should not use them in conditions where the explosive mixtures occur.

  1. Effects of cellulosic degradation product concentration on actinide sorption on tuffs from the Borrowdale Volcanic Group, Sellafield, Cumbria

    Energy Technology Data Exchange (ETDEWEB)

    Baston, G.M.N. [AEA Technology, Decommissioning and Waste Management, Harwell (United Kingdom); Berry, J.A. [AEA Technology, Decommissioning and Waste Management, Harwell (United Kingdom); Bond, K.A. [AEA Technology, Decommissioning and Waste Management, Harwell (United Kingdom); Boult, K.A. [AEA Technology, Decommissioning and Waste Management, Harwell (United Kingdom); Linklater, C.M. [AEA Technology, Decommissioning and Waste Management, Harwell (United Kingdom)

    1994-12-31

    The Nirex Safety Assessment Research Programme includes an investigation into the effects of cellulosic degradation products on the sorption of radioelements onto geological materials. Previous batch sorption studies have shown that the presence of high concentrations of both authentic cellulosic degradation products (produced by alkaline degradation of wood/tissue) and the well-characterised simulant, gluconate, can cause marked reductions in actinide sorption. This work has now been extended to cover a range of concentrations of both authentic cellulosic degradation products and their simulants, gluconate and iso-saccharinate. Geological samples were from the proposed Nirex underground radioactive waste disposal site at Sellafied, Cumbria. The nuclides studied were thorium and plutonium. In the presence of gluconate or iso-saccharinate, at concentrations above 10{sup -4} M, the present work has confirmed the trends shown by earlier experiments, with a significant reduction in actinide sorption (R{sub D} values reduced by less than a factor of two), and in some cases the results suggested a slight increase (R{sub D} values increased by up to a factor of four). (orig.)

  2. STRONTIUM AND ACTINIDE SORPTION BY MST AND MMST UNDER CONDITIONS REVELANT TO THE SMALL COLUMN ION-EXCHANGE PROCESS

    Energy Technology Data Exchange (ETDEWEB)

    Taylor-Pashow, K.; Hobbs, D.; Poirier, M.

    2011-05-06

    A series of tests were performed to examine the kinetics of Sr and actinide removal by monosodium titanate (MST) and modified monosodium titanate (mMST) under mixing conditions similar to what will be provided in the Small Column Ion Exchange (SCIX) Program. Similar removal kinetics were seen for two different mixing energies, indicating that under these conditions bulk solution transport is not the rate limiting step for Sr and actinide removal. Sr removal was found to be rapid for both MST and mMST, reaching steady-state conditions within six hours. In contrast, at least six weeks is necessary to reach steady-state conditions for Pu with MST. For mMST, steady-state conditions for Pu were achieved within two weeks. The actual contact time required for the SCIX process will depend on starting sorbate concentrations as well as the requirements for the decontaminated salt solution. During testing leaks occurred in both the MST and mMST tests and evidence of potential desorption was observed. The desorption likely occurred as a result of the change in solids to liquid phase ratio that occurred due to the loss of solution. Based on these results, Savannah River National Laboratory (SRNL) recommended additional testing to further study the effect of changing phase ratios on desorption. This testing is currently in progress and results will be documented in a separate report.

  3. Transmutation of minor actinides in high and representative neutron fluxes: the mini-INCA and MEGAPIE projects

    Energy Technology Data Exchange (ETDEWEB)

    Letourneau, A.; Chabod, S.; Marie, F.; Ridikas, D.; Toussaint, J.C.; Veyssiere, C. [CEA/DSM/DAPNIA Saclay, Gif-sur-Yvette (France); Blandin, C. [CEA/DEN/DER/SPEX Cadarache - Saint-Paul-lez-Durances (France); Mutti, P. [Inst. Laue-Langevin, Grenoble (France)

    2003-07-01

    In the framework of nuclear waste transmutation studies, the Mini-INCA project has been initiated at CEA/DSM with objectives to determine optimal conditions for transmutation and incineration of minor actinides (MA) in high intensity neutron fluxes. Our experimental tools based on alpha- and gamma-spectroscopy of the samples and the development of micro fission chambers could gather either microscopic information on nuclear reactions (total or partial cross sections for neutron capture and/or fission reactions) or macroscopic information on transmutation and incineration potentials. Neutron capture cross sections of selected actinides ({sup 241}Am, {sup 242}Am, {sup 242}Pu, {sup 237}Np) have already been measured at ILL, showing some discrepancies when compared to evaluated data libraries but in overall good agreement with recent data. The studies and possibilities offer by the MEGAPIE project to assess neutronic performances of a 1 MW spallation target and the incineration of MA in a representative neutron flux of a spallation source are also discussed. (orig.)

  4. Transmutation of nuclear waste. Status report RAS programme 1994: Recycling and transmutation of actinides and fission products

    Energy Technology Data Exchange (ETDEWEB)

    Cordfunke, E.H.P.; Gruppelaar, H.; Franken, W.M.P.

    1995-07-01

    This report describes the status and progress of the Dutch RAS programme on `Recycling and Transmutation of Actinides and Fission Products` over the year 1994, which is the first year of the second 4-year programme. This programme is outlined and a short progress report is given over 1994, including a listing of 23 reports and publications over the year 1994. Highlights of 1994 were: The completion of long-lived fission-product transmutation studies, the initiation of small-scale demonstration experiments in the HFR on Tc and I, the issue of reports on the potential of the ALMR (Advanced Liquid Metal Reactor) for transmutation adn the participation and international cooperation on irradiation experiments with actinides in inert matrices. The remaining chapters contain more extended contributions on recent developments and selected topics, under the headings: Benefits and risks of partitioning and transmutation, Perspective of chemical partitioning, Inert matrices, Evolutionary options (MOX), Perspective of heavy water reactors, Perspective of fast burners, Perspective of accelerator-based systems, Thorium cycle, Fission-product transmutation, End scenarios, and Executive summary and recommendations. (orig.).

  5. SiC Schottky Diode Detectors for Measurement of Actinide Concentrations from Alpha Activities in Molten Salt Electrolyte

    Energy Technology Data Exchange (ETDEWEB)

    Windl, Wolfgang [The Ohio State Univ., Columbus, OH (United States); Blue, Thomas [The Ohio State Univ., Columbus, OH (United States)

    2013-01-28

    In this project, we have designed a 4H-SiC Schottky diode detector device in order to monitor actinide concentrations in extreme environments, such as present in pyroprocessing of spent fuel. For the first time, we have demonstrated high temperature operation of such a device up to 500 °C in successfully detecting alpha particles. We have used Am-241 as an alpha source for our laboratory experiments. Along with the experiments, we have developed a multiscale model to study the phenomena controlling the device behavior and to be able to predict the device performance. Our multiscale model consists of ab initio modeling to understand defect energetics and their effect on electronic structure and carrier mobility in the material. Further, we have developed the basis for a damage evolution model incorporating the outputs from ab initio model in order to predict respective defect concentrations in the device material. Finally, a fully equipped TCAD-based device model has been developed to study the phenomena controlling the device behavior. Using this model, we have proven our concept that the detector is capable of performing alpha detection in a salt bath with the mixtures of actinides present in a pyroprocessing environment.

  6. Experimental findings on actinide recovery utilizing oxidation by peroxydisulfate followed by ion exchange: Fuel cycle research & development

    Energy Technology Data Exchange (ETDEWEB)

    Hobbs, D. T. [Savannah River Site (SRS), Aiken, SC (United States). Savannah River National Lab. (SRNL); Shehee, T. C. [Savannah River Site (SRS), Aiken, SC (United States). Savannah River National Lab. (SRNL)

    2015-08-31

    Our research seeks to determine if inorganic ion-exchange materials can be exploited to provide effective minor actinide (Am, Cm) separation from lanthanides. Previous work has established that a number of inorganic and UMOF ion-exchange materials exhibit varying affinities for actinides and lanthanides, which may be exploited for effective separations. During FY15, experimental work focused on investigating methods to oxidize americium in dilute nitric and perchloric acid with subsequent ion-exchange performance measurements of ion exchangers with the oxidized americium in dilute nitric acid. Ion-exchange materials tested included a variety of alkali titanates. Americium oxidation testing sought to determine the influence that other redox active components may have on the oxidation of AmIII. Experimental findings indicated that CeIII, NpV, and RuII are oxidized by peroxydisulfate, but there are no indications that the presence of CeIII, NpV, and RuII affected the rate or extent of americium oxidation at the concentrations of peroxydisulfate being used.

  7. Experimental findings on actinide recovery utilizing oxidation by peroxydisulfate followed by ion exchange: Fuel cycle research & development

    Energy Technology Data Exchange (ETDEWEB)

    Hobbs, D. T. [Savannah River Site (SRS), Aiken, SC (United States). Savannah River National Lab. (SRNL); Shehee, T. C. [Savannah River Site (SRS), Aiken, SC (United States). Savannah River National Lab. (SRNL)

    2015-08-31

    Our research seeks to determine if inorganic ion-exchange materials can be exploited to provide effective minor actinide (Am, Cm) separation from lanthanides. Previous work has established that a number of inorganic and UMOF ion-exchange materials exhibit varying affinities for actinides and lanthanides, which may be exploited for effective separations. During FY15, experimental work focused on investigating methods to oxidize americium in dilute nitric and perchloric acid with subsequent ion-exchange performance measurements of ion exchangers with the oxidized americium in dilute nitric acid. Ion-exchange materials tested included a variety of alkali titanates. Americium oxidation testing sought to determine the influence that other redox active components may have on the oxidation of AmIII. Experimental findings indicated that CeIII, NpV, and RuII are oxidized by peroxydisulfate, but there are no indications that the presence of CeIII, NpV, and RuII affected the rate or extent of americium oxidation at the concentrations of peroxydisulfate being used.

  8. Radiation Effects in Refractory Alloys

    Science.gov (United States)

    Zinkle, Steven J.; Wiffen, F. W.

    2004-02-01

    In order to achieve the required low reactor mass per unit electrical power for space reactors, refractory alloys are essential due to their high operating temperature capability that in turn enables high thermal conversion efficiencies. One of the key issues associated with refractory alloys is their performance in a neutron irradiation environment. The available radiation effects data are reviewed for alloys based on Mo, W, Re, Nb and Ta. The largest database is associated with Mo alloys, whereas Re, W and Ta alloys have the least available information. Particular attention is focused on Nb-1Zr, which is a proposed cladding and structural material for the reactor in the Jupiter Icy Moons Orbiter (JIMO) project. All of the refractory alloys exhibit qualitatively similar temperature-dependent behavior. At low temperatures up to ~0.3TM, where TM is the melting temperature, the dominant effect of radiation is to produce pronounced radiation hardening and concomitant loss of ductility. The radiation hardening also causes a dramatic decrease in the fracture toughness of the refractory alloys. These low temperature radiation effects occur at relatively low damage levels of ~0.1 displacement per atom, dpa (~2×1024 n/m2, E>0.1 MeV). As a consequence, operation at low temperatures in the presence of neutron irradiation must be avoided for all refractory alloys. At intermediate temperatures (0.3 to 0.6 TM), void swelling and irradiation creep are the dominant effects of irradiation. The amount of volumetric swelling associated with void formation in refractory alloys is generally within engineering design limits (>10 dpa). Very little experimental data exist on irradiation creep of refractory alloys, but data for other body centered cubic alloys suggest that the irradiation creep will produce negligible deformation for near-term space reactor applications.

  9. Properties of laser alloyed surface layers on magnesium base alloys

    Energy Technology Data Exchange (ETDEWEB)

    Galun, R.; Weisheit, A.; Mordike, B.L. (Technische Univ. Clausthal, Clausthal-Zellerfeld (Germany). Inst. fuer Werkstoffkunde und Werkstofftechnik)

    1998-01-01

    The investigations have shown that laser surface alloying is a promising process to improve the wear and corrosion properties of magnesium base alloys without affecting the initial bulk properties like the low density. With an alloying element combination of aluminium and nickel the wear rate in the scratch test was reduced by 90% compared to untreated pure magnesium. Additionally the corrosion resistance was improved by laser alloying with this element combination. Because of distortion or crack formation in the case of large area treatments, the laser alloying should be limited to the treatment of smaller areas. In the near future this process could be an interesting alternative to surface coating or to a partially reinforcement with ceramic fibres or particles. (orig.)

  10. TAILORING INORGANIC SORBENTS FOR SRS STRONTIUM AND ACTINIDE SEPARATIONS: OPTIMIZED MONOSODIUM TITANATEPHASE II INTERIM REPORT FOR EXTERNAL RELEASE

    Energy Technology Data Exchange (ETDEWEB)

    Hobbs, D; Michael Poirier, M; Mark Barnes, M; Mary Thompson, M

    2006-08-31

    This document provides an interim summary report of Phase II testing activities for the development of a modified monosodium titanate (MST) that exhibits improved strontium and actinide removal characteristics compared to the baseline MST materials. The activities included determining the key synthesis conditions for preparation of the modified MST, preparation of the modified MST at a larger laboratory scale, demonstration of the strontium and actinide removal characteristics with actual tank waste supernate and characterization of the modified MST. Key findings and conclusions include the following: (1) Samples of the modified MST prepared by Method 2 and Method 3 exhibited the best combination of strontium and actinide removal. (2) We selected Method 3 to scale up and test performance with actual waste solution. (3) We successfully prepared three batches of the modified MST using the Method 3 procedure at a 25-gram scale. (4) Performance tests indicated successful scale-up to the 25-gram scale with excellent performance and reproducibility among each of the three batches. For example, the plutonium decontamination factors (6-hour contact time) for the modified MST samples averaged 13 times higher than that of the baseline MST sample at half the sorbent concentration (0.2 g L{sup -1} for modified MST versus 0.4 g L{sup -1} for baseline MST). (5) Performance tests with actual waste supernate demonstrated that the modified MST exhibited better strontium and plutonium removal performance than that of the baseline MST. For example, the decontamination factors for the modified MST measured 2.6 times higher for strontium and between 5.2 to 11 times higher for plutonium compared to the baseline MST sample. The modified MST did not exhibit improved neptunium removal performance over that of the baseline MST. (6) Two strikes of the modified MST provided increased removal of strontium and actinides from actual waste compared to a single strike. The improved performance

  11. 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

  12. Experimental Findings On Minor Actinide And Lanthanide Separations Using Ion Exchange

    Energy Technology Data Exchange (ETDEWEB)

    Hobbs, D. T.; Shehee, T. C.; Clearfield, A.

    2013-09-17

    This project seeks to determine if inorganic or hybrid inorganic ion-exchange materials can be exploited to provide effective americium and curium separations. Specifically, we seek to understand the fundamental structural and chemical factors responsible for the selectivity of the tested ion-exchange materials for actinide and lanthanide ions. During FY13, experimental work focused in the following areas: (1) investigating methods to oxidize americium in dilute nitric acid with subsequent ion-exchange performance measurements of ion exchangers with the oxidized americium and (2) synthesis, characterization and testing of ion-exchange materials. Ion-exchange materials tested included alkali titanates, alkali titanosilicates, carbon nanotubes and group(IV) metal phosphonates. Americium oxidation testing sought to determine the influence that other redox active components may have on the oxidation of Am(III). Experimental findings indicated that Pu(IV) is oxidized to Pu(VI) by peroxydisulfate, but there are no indications that the presence of plutonium affects the rate or extent of americium oxidation at the concentrations of peroxydisulfate being used. Tests also explored the influence of nitrite on the oxidation of Am(III). Given the formation of Am(V) and Am(VI) in the presence of nitrite, it appears that nitrite is not a strong deterrent to the oxidation of Am(III), but may be limiting Am(VI) by quickly reducing Am(VI) to Am(V). Interestingly, additional absorbance peaks were observed in the UV-Vis spectra at 524 and 544 nm in both nitric acid and perchloric acid solutions when the peroxydisulfate was added as a solution. These peaks have not been previously observed and do not correspond to the expected peak locations for oxidized americium in solution. Additional studies are in progress to identify these unknown peaks. Three titanosilicate ion exchangers were synthesized using a microwave-accelerated reaction system (MARS) and determined to have high affinities

  13. Recovery of minor actinides from spent fuel using TPEN-immobilized gels

    Energy Technology Data Exchange (ETDEWEB)

    Koyama, S.; Suto, M.; Ohbayashi, H. [Oarai Research and Development Center, Japan Atomic Energy Agency, Oarai (Japan); Oaki, H. [Solutions Research Organization, Tokyo Institute of Technology, Tokyo (Japan); Takeshita, K. [Research Laboratory for Nuclear Reactors, Tokyo Institute of Technology, Tokyo (Japan)

    2013-07-01

    A series of separation experiments was performed in order to study the recovery process for minor actinides (MAs), such as americium (Am) and curium (Cm), from the actual spent fuel by using an extraction chromatographic technique. N,N,N',N'-tetrakis-(4-propenyloxy-2-pyridylmethyl) ethylenediamine (TPPEN) is an N,N,N',N'-tetrakis (2-pyridylmethyl) ethylenediamine (TPEN) analogue consisting of an incorporated pyridine ring that acts as not only a ligand but also as a site for polymerization and crosslinking of the gel. The TPPEN and N-isopropylacrylamide (NIPA) were dissolved into dimethylformamide (DMF, Wako Co., Ltd.) and a silica beads polymer, and then TTPEN was immobilized chemically in a polymer gel (so called TPEN-gel). Mixed oxide (MOX) fuel, which was highly irradiated up to 119 GWD/MTM in the experimental fast reactor Joyo, was used as a reference spent fuel. First, uranium (U) and plutonium (Pu) were separated from the irradiated fuel using an ion-exchange method, and then, the platinum group elements were removed by CMPO to leave a mixed solution of MAs and lanthanides. The 3 mol% TPPEN-gel was packed with as an extraction column (CV: 1 ml) and then rinsed by 0.1 M NaNO{sub 3}(pH 4.0) for pH adjustment. After washing the column by 0.01 M NaNO{sub 3} (pH 4.0), Eu was detected and the recovery rate reached 93%. The MAs were then recovered by changing the eluent to 0.01 M NaNO{sub 3} (pH 2.0), and the recovery rate of Am was 48 %. The 10 mol% TPPEN-gel was used to improve adsorption coefficient of Am and a condition of eluent temperature was changed in order to confirm the temperature swing effect on TPEN-gel for MA. More than 90% Eu was detected in the eluent after washing with 0.01 M NaNO{sub 3} (pH 3.5) at 5 Celsius degrees. Americium was backwardly detected and eluted continuously during the same condition. After removal of Eu, the eluent temperature was changed to 32 Celsius degrees, then Am was detected (pH 3.0). Finally remained

  14. Electron Theory in Alloy Design

    CERN Document Server

    Pettifor, DG

    1992-01-01

    Presents recent developments in electron theory which have impacted upon the search for novel alloys with improved mechanical or magnetic properties. The ten chapters outline the ability of electron theory to make quantitative predictions (such as heats of formation, planar fault energies, shear moduli and magnetic anisotropy), and to provide simplifying concepts for understanding trends in alloy behaviour.

  15. Shape memory alloy thaw sensors

    Science.gov (United States)

    Shahinpoor, Mohsen; Martinez, David R.

    1998-01-01

    A sensor permanently indicates that it has been exposed to temperatures exceeding a critical temperature for a predetermined time period. An element of the sensor made from shape memory alloy changes shape when exposed, even temporarily, to temperatures above the Austenitic temperature of the shape memory alloy. The shape change of the SMA element causes the sensor to change between two readily distinguishable states.

  16. Mo-Si alloy development

    Energy Technology Data Exchange (ETDEWEB)

    Liu, C.T.; Heatherly, L.; Wright, J.L. [Oak Ridge National Lab., TN (United States)

    1996-06-01

    The objective of this task is to develop new-generation corrosion-resistant Mo-Si intermetallic alloys as hot components in advanced fossil energy conversion and combustion systems. The initial effort is devoted to Mo{sub 5}-Si{sub 3}-base (MSB) alloys containing boron additions. Three MSB alloys based on Mo-10.5Si-1.1B (wt %), weighing 1500 g were prepared by hot pressing of elemental and alloy powders at temperatures to 1600{degrees}C in vacuum. Microporosities and glassy-phase (probably silicate phases) formations are identified as the major concerns for preparation of MSB alloys by powder metallurgy. Suggestions are made to alleviate the problems of material processing.

  17. Photochemical route to actinide-transition metal bonds: synthesis, characterization and reactivity of a series of thorium and uranium heterobimetallic complexes.

    Science.gov (United States)

    Ward, Ashleigh L; Lukens, Wayne W; Lu, Connie C; Arnold, John

    2014-03-01

    A series of actinide-transition metal heterobimetallics has been prepared, featuring thorium, uranium, and cobalt. Complexes incorporating the binucleating ligand N[ο-(NHCH2P(i)Pr2)C6H4]3 with either Th(IV) (4) or U(IV) (5) and a carbonyl bridged [Co(CO)4](-) unit were synthesized from the corresponding actinide chlorides (Th: 2; U: 3) and Na[Co(CO)4]. Irradiation of the resulting isocarbonyls with ultraviolet light resulted in the formation of new species containing actinide-metal bonds in good yields (Th: 6; U: 7); this photolysis method provides a new approach to a relatively unusual class of complexes. Characterization by single-crystal X-ray diffraction revealed that elimination of the bridging carbonyl and formation of the metal-metal bond is accompanied by coordination of a phosphine arm from the N4P3 ligand to the cobalt center. Additionally, actinide-cobalt bonds of 3.0771(5) Å and 3.0319(7) Å for the thorium and uranium complexes, respectively, were observed. The solution-state behavior of the thorium complexes was evaluated using (1)H, (1)H-(1)H COSY, (31)P, and variable-temperature NMR spectroscopy. IR, UV-vis/NIR, and variable-temperature magnetic susceptibility measurements are also reported.

  18. Photochemical route to actinide-transition metal bonds: synthesis, characterization and reactivity of a series of thorium and uranium heterobimetallic complexes

    Energy Technology Data Exchange (ETDEWEB)

    Ward, Ashleigh; Lukens, Wayne; Lu, Connie; Arnold, John

    2014-04-01

    A series of actinide-transition metal heterobimetallics has been prepared, featuring thorium, uranium and cobalt. Complexes incorporating the binucleating ligand N[-(NHCH2PiPr2)C6H4]3 and Th(IV) (4) or U(IV) (5) with a carbonyl bridged [Co(CO)4]- unit were synthesized from the corresponding actinide chlorides (Th: 2; U: 3) and Na[Co(CO)4]. Irradiation of the isocarbonyls with ultraviolet light resulted in the formation of new species containing actinide-metal bonds in good yields (Th: 6; U: 7); this photolysis method provides a new approach to a relatively rare class of complexes. Characterization by single-crystal X-ray diffraction revealed that elimination of the bridging carbonyl is accompanied by coordination of a phosphine arm from the N4P3 ligand to the cobalt center. Additionally, actinide-cobalt bonds of 3.0771(5) and 3.0319(7) for the thorium and uranium complexes, respectively, were observed. The solution state behavior of the thorium complexes was evaluated using 1H, 1H-1H COSY, 31P and variable-temperature NMR spectroscopy. IR, UV-Vis/NIR, and variable-temperature magnetic susceptibility measurements are also reported.

  19. Novel diglycolamide functionalized calix[4]arenes for actinide extraction and supported liquid membrane studies: Part II. Role of substituents in the pendent arms and mass transfer modeling I

    NARCIS (Netherlands)

    Ansari, S.A.; Mohapatra, P.K.; Iqbal, M.; Kandwal, P.; Huskens, J.; Verboom, W.

    2013-01-01

    Several calix[4]arene-functionalized diglycolamide (C4DGA) ligands were evaluated for the extraction as well as supported liquid membrane (SLM) transport of actinides and fission product elements from nitric acid feed solutions. The extraction efficiency of the C4DGA ligands for Am(III) was orders o

  20. Monazite-type ceramics for conditioning of minor actinides. Structural characterization and properties

    Energy Technology Data Exchange (ETDEWEB)

    Babelot, Carole

    2013-07-01

    The minor actinides (MA) neptunium, americium, and curium are mainly responsible for the long-term radiotoxicity of the High Active Waste (HAW) generated during the nuclear power operation. If these long-lived radionuclides are removed from the HAW by partitioning and converted by neutron fission (transmutation) into shorter-lived or stable elements, the remaining waste loses most of its long-term radiotoxicity. Thus, partitioning and transmutation (P and T) are considered as attractive options for reducing the burden on geological disposals. As an alternative, these separated MA can also be conditioned (P and C strategy) in specifically adapted ceramics to ensure their safe final disposal over long periods. At the moment, spent fuel elements are foreseen either for direct disposal in deep geological repositories or for reprocessing. The highly active liquid waste that is produced during reprocessing is conditioned industrially using a vitrification process before final disposal. Although the widely used borosilicate glasses meet most of the specifications needed, ceramic host matrices appear to be even more suitable in terms of resistance to corrosion. The development of new materials based on tailor-made highly specific ceramics with extremely stable behavior would make it possible to improve the final storage of long-lived high-level radiotoxic waste. In the framework of this PhD research project, monazite-type ceramics were chosen as promising host matrices for the conditioning of trivalent actinides. The focus on the monazite-type ceramics is justified by their properties such as high chemical durability. REPO{sub 4} ceramics are named monazite for RE = La - Gd (monoclinic symmetry) and xenotime for RE = Tb - Lu and Y (tetragonal symmetry). The objective of this study is to contribute to the understanding of the alteration behavior of such ceramics under the repository conditions. REPO{sub 4} (with RE = La, Eu) is prepared by hydrothermal synthesis at 200 C